TW202142663A - Adhesive and use thereof - Google Patents

Abstract

Provided is an adhesive that contains an acrylic polymer (F) containing a fluorine-containing acrylic monomer (M1) as a monomer unit. The adhesive has a refractive index of at most 1.46 and a storage elastic modulus G' at 25 DEG C of at most 400 kPa.

Description

Adhesives and their use

The present invention relates to an adhesive, and in detail, it relates to an acrylic polymer containing a fluorine-containing acrylic monomer as a monomer unit and its use. The claim of this application is based on Japanese Patent Application No. 2020-052408 filed on March 24, 2020, Japanese Patent Application No. 2020-166428 filed on September 30, 2020, and Japanese Patent Application No. 2020-166428 filed on September 30, 2020. Priority is given to Japanese Patent Application No. 2021-049062 filed on March 23, and the entire contents of these applications are incorporated into this specification for reference.

Generally speaking, adhesives (also known as pressure-sensitive adhesives, the same hereinafter) present a soft solid (viscoelastic) state in a temperature region near room temperature, and have the ability to be easily adhered to the adherend by pressure nature. Utilizing this property, adhesives are widely used for bonding, fixing, and protecting purposes in various industrial fields ranging from home appliances to automobiles, various machinery, electrical equipment, and electronic equipment. Regarding the technical literature of the adhesive, patent literatures 1 to 4 can be cited. Prior art literature Patent literature

Patent Document 1: Japanese Patent No. 6014781 Patent Document 2: Japanese Patent Application Publication No. 2020-111740 Patent Document 3: Japanese Patent Application Publication No. 2019-210343 Patent Document 4: Japanese Patent Application Publication No. 2018-193553

The problem to be solved by the invention Patent Documents 1 to 4 propose an adhesive which contains a (meth)acrylate copolymer, and the (meth)acrylate copolymer contains a structural unit derived from a fluorine-containing acrylic monomer. These are all adhesives that focus on sebum resistance and/or chemical resistance, and do not take into account the refractive index.

The purpose of the present invention is to provide a low refractive index and flexible adhesive. Related other objects are to provide a laminated sheet including an adhesive layer composed of the adhesive and a light-emitting device including the laminated sheet.

Means for Solving the Problem According to this specification, an adhesive is provided, which contains an acrylic polymer (F), and the acrylic polymer (F) contains a fluorine-containing acrylic monomer (M1) as a monomer unit. The refractive index of the above-mentioned adhesive is 1.46 or less. The storage elastic modulus G'of the above-mentioned adhesive at 25°C (the following is indicated as "storage elastic modulus _G'V2 (25)") should be 400 kPa or less (for example, 1.0 kPa or more and 400 kPa or less). The adhesive can be suitably used for the purpose of controlling the behavior of light in the form of being laminated on a layer with a higher refractive index (which may be an adhesive layer), for example. The storage elastic modulus _G'V2 (25) of the above-mentioned adhesive is limited to the predetermined value, so it is easy to stick or adhere to the adherend, followability to the surface shape of the adherend, and It is advantageous from the viewpoint of the followability of body deformation.

In the monomer components constituting the acrylic polymer (F), the content of the fluorine-containing acrylic monomer (M1) is preferably 25% by weight or more. By including the acrylic polymer (F) composed of monomer components of this composition, an adhesive having a refractive index of 1.46 or less can be suitably realized. The above-mentioned fluorine-containing acrylic monomer (M1) preferably contains a fluorine atom-containing alkyl (meth)acrylate from the viewpoint of ease of polymerization and low refractive index effect.

In several aspects, the above-mentioned acrylic polymer (F) contains a hydroxyl group-containing monomer as a monomer unit. The monomer unit derived from the hydroxyl-containing monomer helps to realize an adhesive that has the desired flexibility and moderate agglutinating properties.

According to this specification, a laminated sheet is provided, which includes: a low-refractive-index adhesive layer formed by any of the adhesives disclosed herein; and a high-refractive-index adhesive layer laminated on the low-refractive adhesive layer. According to the laminated sheet included in the form of laminating adhesive layers with different refractive indexes as described above, the difference in refractive index between the high refractive index adhesive layer and the low refractive index adhesive layer can be used to control the light transmitted through the laminated sheet the behavior of. The ratio (n ₁ /n ₂ ) of the refractive index n ₁ of the high refractive index adhesive layer to the refractive index n ₂ of the low refractive index adhesive layer may be 1.02 or more, for example.

In several aspects, the refractive index n _{1 of} the high refractive index adhesive layer may be greater than 1.570. The laminated sheet provided with the high-refractive-index adhesive layer has a large refractive index difference with the low-refractive-index adhesive layer, so that the behavior of light transmitted through the laminated sheet can be better controlled.

In several aspects, the storage elastic modulus G'of the high-refractive index adhesive layer at 25° C. (hereinafter referred to as "storage elastic modulus _G'V1 (25)") is 700 kPa or less. As described above, a laminate sheet having a high refractive index adhesive layer whose storage elastic modulus _G'V1 (25) is limited to a predetermined value or less is ideal from the viewpoint of ease of attachment or flexibility.

In several aspects, the total light transmittance of the above-mentioned laminated sheet is 86% or more, and the haze value is 3.0% or less. As described above, the transparent laminated sheet can be suitably used for bonding optical members or controlling the behavior of light transmitted through the laminated sheet.

The laminated sheet disclosed here is suitable as, for example, a constituent element of a light-emitting device. Therefore, according to this specification, a light-emitting device including any of the laminated sheets disclosed herein and a self-luminous element is provided.

In addition, the appropriate combination of the various elements described in this specification may also be included in the scope of the invention for which patent protection is sought through this patent application.

The preferred embodiment of the present invention will be described below. Matters not specifically mentioned in this specification are matters that are required for the implementation of the present invention, and those who are familiar with the art can understand them based on the teachings on the implementation of the invention contained in this specification and common technical knowledge at the time of application. The present invention can be implemented based on the content disclosed in this specification and common technical knowledge in the field. In addition, in the following drawings, members and parts that perform the same function are given the same symbols for description, and repeated descriptions may be omitted or simplified. In addition, the embodiments described in the drawings are schematic in order to clearly explain the present invention, and do not completely accurately represent the dimensions or scales of the products actually provided.

In this specification, the self-luminous element means a light-emitting element that can control the luminance of light emitted by the value of the current flowing through it. The self-luminous element may be composed of a single body, or may be composed of an assembly. Specific examples of self-luminous elements include light-emitting diodes (LED) and organic EL, but are not limited to these. The light-emitting device disclosed herein includes the self-luminous element as a constituent element. In the example of the above-mentioned light-emitting device, it also includes a light-source module device used as lighting (for example, a planar light-emitting body module) or a display device formed with pixels, but it is not limited thereto.

The technology disclosed by this specification includes: a low refractive index adhesive and an adhesive composition for forming it, a high refractive index adhesive layer and an adhesive composition for forming it, a high refractive index adhesive layer and a low A laminated sheet (adhesive sheet) with a refractive index adhesive layer, a laminated sheet with a release liner in which the adhesive surface of the laminated sheet is protected by a release liner, and a light-emitting device containing a high-refractive-index adhesive layer and a low-refractive-index adhesive layer Wait. The technology disclosed in this specification may further include: an interlayer sheet including a high-refractive-index adhesive layer and a low-refractive-index adhesive layer and arranged between the layers of the optical laminate.

＜Example of the composition of the adhesive sheet＞ The adhesive disclosed here can be used, for example, in the form of an adhesive sheet including a layer (adhesive layer) formed by the adhesive, and is preferably used in the form of an adhesive sheet having an adhesive surface formed by the adhesive layer . The above-mentioned adhesive sheet may be a substrate-attached adhesive sheet having an adhesive layer on one or both sides of a non-releasable substrate (supporting substrate), or a form in which the above-mentioned adhesive layer is held on a release liner, etc. Adhesive sheets without a substrate (ie, an adhesive sheet without a non-peelable substrate, typically an adhesive sheet composed of an adhesive layer). The concept of the adhesive sheet mentioned here can include those called adhesive tape, adhesive label, adhesive film, etc. The adhesive sheet disclosed here can be rolled or flake-shaped. Or it can also be an adhesive sheet that is further processed into various shapes.

An example of the configuration of an adhesive sheet including an adhesive layer formed of the adhesive disclosed herein is shown in FIG. 1. The adhesive sheet 1 is configured as a single-sided adhesive sheet (single-sided adhesive sheet), which includes: an adhesive layer 10, the first surface 10A of which becomes an adhesive surface (adhesive surface) attached to an adherend者; And a supporting substrate 20, which is laminated on the second surface 10B of the adhesive layer 10. The second surface 10B of the adhesive layer 10 is bonded to the first surface (non-peelable surface) 20A of the support base 20. As the support base 20, a plastic film such as a polyester film can be used. The supporting substrate 20 may also be an optical film such as a polarizing plate. The adhesive sheet 1 before use (before being attached to the adherend) can be, for example, as shown in FIG. 30 is the one where at least this adhesive layer side becomes a peelable surface (peelable surface). Alternatively, the following form may be adopted: the second surface 20B (the surface on the opposite side to the first surface 20A, also referred to as the back surface) of the support base 20 becomes a peeling surface, and the adhesive surface 10A abuts the second surface 20B The method is wound or laminated to protect the adhesive surface 10A.

The adhesive layer 10 may be a single-layer structure, or may be a laminated structure in which two or more sub-adhesive layers with different compositions are in direct contact (that is, not separated by layers of non-adhesive materials). The refractive index of the sub-adhesive layer constituting the above-mentioned laminated structure may be the same or different. In the adhesive layer of the laminated structure including two or more sub-adhesive layers with different refractive indexes, it is preferable that at least one sub-adhesive layer meets the refractive index of 1.46 or less (preferably further meets the storage elastic modulus G'(25 ) 400kPa or less) low refractive index adhesive layer. The refractive index and storage elastic modulus G'(25) of other sub-adhesive layers are not particularly limited. For example, the refractive index can be less than 1.46 or greater than 1.46, and the storage elastic modulus G'(25) can be 400kPa Below, it can also be greater than 400kPa.

The adhesive sheet disclosed here may also be in the form of a substrate-free double-sided adhesive sheet composed of an adhesive layer. The adhesive layer constituting the double-sided adhesive sheet without base material can be a single-layer structure like the adhesive layer 10 in the adhesive sheet 1 shown in FIG. Layered structure made up of layers. 2 shows an example of the structure of a double-sided adhesive sheet 2 without a base material composed of an adhesive layer 10 including a laminated structure of a first adhesive layer 11 and a second adhesive layer 12 with different compositions. The second adhesive layer 12 is a low-refractive-index adhesive layer that satisfies the refractive index of 1.46 or less, and can be a layer that further satisfies the storage elastic modulus G'(25) of 400 kPa or less. In relation to the second adhesive layer 12, the first adhesive layer 11 may be an adhesive layer with a relatively high refractive index (high refractive index adhesive layer). The adhesive sheet 2 of the aforementioned structure can be regarded as a laminated sheet having a laminated structure of a high-refractive-index adhesive layer/low-refractive-index adhesive layer.

The double-sided adhesive sheet 2 without a base material can be in the following form before use: As shown in FIG. 2, the first surface (first adhesive surface) 10A and the second surface (second adhesive surface) 10B of the adhesive layer 10 are covered At least the adhesive layer side is protected by the release liners 31 and 32 that serve as a release surface (release surface). Alternatively, it may be a form in which the back surface of the release liner 31 (the surface on the side opposite to the adhesive side) becomes the release surface, and the adhesive surface 10B is wound or laminated so that the adhesive surface 10B abuts against the back surface of the release liner 31, In order to protect the adhesive surfaces 10A, 10B. The double-sided adhesive sheet without a substrate, for example, can be bonded to a substrate (preferably a light-transmitting substrate, such as an optical member such as an optical film) on at least one of the first adhesive surface and the second adhesive surface. use.

The low-refractive-index adhesives (adhesives with a refractive index below 1.46) disclosed herein can be used, for example, in the form of being incorporated into a light-emitting device. An example of the configuration of the light-emitting device is shown in FIG. 3. The light-emitting device 100 shown in FIG. 3 includes: a self-luminous element 70; a low-refractive-index adhesive layer 12, which is arranged on the side closer to the view than the self-luminous element 70; and a high-refractive-index adhesive layer 11, which is in direct contact with the low-refraction The adhesive layer 12 is laminated at a higher rate. The light emitting device 100 may further include a cover window member 80 disposed on the viewing side of the high refractive index adhesive layer 11. In the light-emitting device 100 shown in FIG. 3, a laminated sheet 10 composed of a high-refractive-index adhesive layer 11 and a low-refractive-index adhesive layer 12 is arranged between the self-luminous element 70 and the cover window member 80. Between the self-luminous element 70 and the low-refractive-index adhesive layer 12, between the high-refractive-index adhesive layer 12 and the cover window member 80, and the cover window member 80 closer to the visibility side, 1 or 2 can be independently interposed respectively The above layers are not shown in the figure, and the layer body may not be interposed. In addition, contrary to FIG. 3, the high-refractive-index adhesive layer 11 may be arranged on the side of the self-luminous element, and the low-refractive-index adhesive layer 12 may be arranged on the side of the cover window member. Alternatively, the low-refractive-index adhesive disclosed herein can also be used in a light-emitting device in which the high-refractive-index adhesive layer 11 in FIG. 3 is omitted or replaced with a non-adhesive high-refractive-index layer (hard resin layer, etc.).

The adhesive sheet disclosed herein may be a constituent element of an optical member of an adhesive sheet with an optical member bonded to at least one surface of an adhesive layer. For example, the adhesive sheet 1 shown in FIG. 1 may be a constituent element of an optical member of an adhesive sheet in which an optical member is bonded to the first surface 10A of the adhesive layer 10. The above-mentioned optical member may be, for example, a glass plate, a resin film, a metal plate, or the like. In addition, in the adhesive sheet 1 shown in FIG. 1, when the supporting substrate 20 is an optical member such as an optical film, the adhesive sheet 1 can be regarded as an adhesive sheet with an optical member bonded to the second surface 10B of the adhesive layer 10的optical components.

In addition, although there is no special illustration, the adhesive sheet disclosed here can also be in the form of the following double-sided adhesive sheet with a substrate (double-sided adhesive sheet with a substrate): One side and the second side of the supporting base material, the first adhesive layer is fixedly laminated on the first side, and the second adhesive layer is fixedly laminated on the second side. Examples of the configuration of the double-sided adhesive sheet with a substrate include the following: In the single-sided adhesive sheet 1 shown in FIG. 1, the second surface 20B of the supporting substrate 20 is a non-releasable surface and the A second adhesive layer is provided on the 2 surface 20B, the second surface of the second adhesive layer is joined to the second surface 20B of the support base 20, and the first surface (and the second surface of the second adhesive layer) The surface on the opposite side) becomes the second adhesive surface of the double-sided adhesive sheet with base material. The composition of the adhesive constituting the second adhesive layer may be the same as or different from the composition of the adhesive constituting the first adhesive layer. The double-sided adhesive sheet with a base material before use is the same as the above-mentioned double-sided adhesive sheet without a base material. The first adhesive surface and the second adhesive surface can be protected by the release liner.

In addition, for the convenience of explanation, the following descriptions of adhesives with refractive index below 1.46 (low refractive index adhesives) are described for comparison with higher refractive index layers, but it is not intended to limit the low refractive index adhesives disclosed here. The state of use of the agent.

<Low refractive index adhesive> According to this specification, an adhesive with a refractive index of 1.46 or less is provided. The adhesive having the refractive index may be suitably used for the purpose of controlling the behavior of light in the form of being laminated on a layer with a higher refractive index (which may be an adhesive layer), for example. In several aspects, from _{the viewpoint of increasing the refractive index difference with the refractive index n 1} of the high refractive index layer to easily improve the positive brightness improvement effect described later, the refractive index n _{2 of the} low refractive index adhesive layer is, for example, It is preferably 1.45 or less, and preferably 1.44 or less, can be 1.43 or less, can be 1.41 or less, can be 1.40 or less, or can be less than 1.40 (for example, less than 1.39, and further less than 1.38). In addition, from the viewpoint of easy availability of materials or ease of compatibility with adhesive properties, in several aspects, the refractive index n _{2 of the} low refractive index adhesive can be, for example, 1.35 or more, or 1.36 or more, and It is 1.38 or more, may be 1.40 or more, or may be 1.42 or more. The technique disclosed herein can be suitably implemented in a state where the refractive index n ₂ of the low refractive index adhesive is 1.35 or more and 1.46 or less (preferably 1.36 or more and 1.45 or less).

In addition, in this specification, the refractive index of the adhesive means the refractive index of the surface (adhesive surface) of the adhesive. The refractive index of the adhesive can be measured using a commercially available refractive index measuring device (Abbe refractometer) under the conditions of a measurement wavelength of 589 nm and a measurement temperature of 25°C. The Abbe refractometer can use, for example, the type "DR-M4" manufactured by ATAGO or its equivalent. The measurement sample may use an adhesive layer composed of the adhesive of the evaluation object. Specifically, the refractive index of the adhesive can be measured by the method described in the following examples. The refractive index of the adhesive can be adjusted by, for example, the composition of the adhesive (e.g., the composition of the monomer components constituting the base polymer, the additives that can be used as needed, etc.).

From the viewpoints of ease of attachment or adhesion to the adherend, surface shape followability, deformation followability, etc., the storage elastic modulus _G'V2 (25) of the low refractive index adhesive disclosed here is Below 400kPa is appropriate. In several aspects, the storage elastic modulus _G'V2 (25) should be less than 300kPa, more preferably less than 200kPa (for example, less than 180kPa or 150kPa), can be less than 120kPa, can be less than 90kPa, or less than 70kPa the following. The storage elastic modulus _G'V2 (25) is low, for example, in the use state of the layer on the high refractive index layer, the effect of increasing the low refractive index adhesive layer to impart flexibility or improve the followability to deformation, etc. It's also beneficial to look at. The lower limit of the storage elastic modulus _G'V2 (25) is not particularly limited, and may be 1.0 kPa or more, for example. In several aspects, which is easy to impart a low refractive index adhesive layer moderately aggregated perspective view of the storage elastic modulus G _'V2 (25) e.g. 5.0kPa above are suitable for, and is suitably 10kPa or more, It is 15 kPa or more, it can be 25 kPa or more, it can be 35 kPa or more, it can be 60 kPa or more, and it can also be 80 kPa or more. Which is easy to achieve higher cohesive force or adhesive properties of the view perspective, in several aspects, the storage elastic modulus G _'V2 (25) can be more than 95kPa, more can be 110kPa, 140kPa may also be more.

In several ideal situations, the storage elastic modulus G'(that is, the storage elastic modulus _G'V2 (25)) of the low refractive index adhesive layer at 25°C should be lower than that which can be adjacent to the low refractive index adhesive The storage elastic modulus G'of the high refractive index layer of the layer configuration at 25°C (there are cases in which it is expressed as "storage elastic modulus _G'V1 (25)"). That is, it should be _G'V2 (25)<G' _V1 (25). According to the above configuration, the storage elastic modulus G'tends to increase due to the high refractive index layer (such as a high-refractive-index adhesive layer) as a compensation for higher refractive index. The high-speed adhesive layer can impart adhesion or flexibility, improve the followability of height difference or followability to curved surfaces, etc., so as to realize a laminated sheet (adhesive sheet) that can be suitably applied to a variety of device designs.

The low refractive index adhesive disclosed here contains an acrylic polymer (F), and the acrylic polymer (F) contains a fluorine-containing acrylic monomer (M1) as a monomer unit. The low refractive index adhesive is preferably an acrylic adhesive containing the acrylic polymer (F) as a base polymer.

In addition, in this specification, the "base polymer" of the adhesive means the main component of the rubber-like polymer contained in the adhesive, and other than that, no limited interpretation is made. The above-mentioned rubbery polymer refers to a polymer that exhibits rubber elasticity in a temperature region around room temperature. In addition, in this specification, the "main component" means that it contains more than 50% by weight of a component when it is not specifically noted. In addition, in this specification, "acrylic polymer" means a polymer containing the following monomer unit as a monomer unit constituting the polymer: the monomer unit is derived from having at least one (former) in one molecule Base) Monomers based on acrylic acid. Hereinafter, a monomer having at least one (meth)acrylic acid group in one molecule is also referred to as an "acrylic monomer". Therefore, the acrylic polymer in this specification is defined as a polymer containing monomer units derived from acrylic monomers. A typical example of the acrylic polymer can be a polymer with an acrylic monomer ratio of more than 50% by weight (preferably more than 70% by weight, for example, more than 90% by weight) in the total monomers that can be used in the synthesis of the acrylic polymer. In addition, in this specification, "(meth)acryloyl group" means an allyl group and methacryloyl group. Similarly, "(meth)acrylate" means acrylate and methacrylate collectively, and "(meth)acrylic acid" means acrylic and methacrylic acid collectively. Therefore, the concept of acrylic monomers mentioned herein may include both monomers having acrylic groups (acrylic monomers) and monomers having methacrylic groups (methacrylic monomers).

(Acrylic polymer (F)) The acrylic polymer (F) in the technology disclosed here contains a fluorine-containing acrylic monomer (M1) as a monomer component constituting the polymer. That is, the acrylic polymer (F) contains a fluorine-containing acrylic monomer (M1) as a monomer unit. By appropriately using the fluorine-containing acrylic monomer (M1), the acrylic polymer (F) can be lowered in refractive index.

Here, the "monomer components constituting the acrylic polymer" in this specification means whether it is contained in the adhesive composition in the form of a preformed polymer (which may be an oligomer), or whether it is contained in the adhesive composition. The form of the polymerized monomer is included in the adhesive composition, and all monomers constitute the repeating unit of the acrylic polymer in the adhesive formed by the adhesive composition. That is, the monomer components constituting the acrylic polymer may be included in the above-mentioned adhesive composition in any form of polymer, unpolymerized, and partial polymer. From the viewpoint of ease of preparation of the adhesive composition, among several aspects, it is preferable to include substantially all of the monomer components (for example, 95% by weight or more, preferably 99% by weight or more) in the form of a polymer The adhesive composition. An adhesive composition containing substantially all of the monomer components in the form of a polymer is also preferable from the viewpoint of easily forming an adhesive sheet with little strain or warpage.

The acrylic polymer (F) may be a polymer of the following monomer raw materials: at least containing a fluorine-containing acrylic monomer (M1) (hereinafter referred to as "monomer (M1)"), and may further contain and This monomer (M1) has other copolymerizable monomers (copolymerizable monomers). The monomer (M1) is not particularly limited as long as it is an acrylic monomer having at least one fluorine atom in the molecule. For example, fluorine-containing (meth)acrylate can be suitably used. Suitable examples of the fluorine-containing (meth)acrylate include those having a fluorinated hydrocarbon group at the end of the ester. Examples of the fluorinated hydrocarbon group include a fluorinated aliphatic hydrocarbon group, a fluorinated alicyclic hydrocarbon group, and a fluorinated aromatic hydrocarbon group. The fluorinated hydrocarbon group is preferably a fluorinated aliphatic hydrocarbon group. Examples of fluorinated aliphatic hydrocarbon groups include fluorinated alkyl groups. In the fluorinated aliphatic hydrocarbon group, the aliphatic hydrocarbon portion may be linear or branched. In addition, in the fluorinated aliphatic hydrocarbon group, a fluorine atom may be bonded to any carbon atom in the aliphatic hydrocarbon group. The fluorine atom bonded to a carbon atom may be singular or plural. The number of carbon atoms to which fluorine atoms are bonded is not particularly limited.

In the fluorinated aliphatic hydrocarbon group (which is also a fluorinated alkyl group), the number of carbon atoms in the hydrocarbon group portion is not particularly limited. In several aspects, considering the compatibility with other comonomers, a fluorinated aliphatic hydrocarbon group with a carbon number of, for example, about 1 to 18 (preferably 1 to 12) is preferred. Specific examples of fluorinated aliphatic hydrocarbon groups include fluorinated methyl groups such as trifluoromethyl, difluoromethyl, and monofluoromethyl; pentafluoroethyl, 1,1,2,2-tetrafluoroethyl, 1, 2,2,2-tetrafluoroethyl, 1,1,2-trifluoroethyl, 1,2,2-trifluoroethyl, 2,2,2-trifluoroethyl, 1,1-difluoro Fluorinated ethyl groups such as ethyl, 1,2-difluoroethyl, 2,2-difluoroethyl, 1-monofluoroethyl, 2-monofluoroethyl, etc. The fluorinated alkyl group with 3 or more carbon atoms can be exemplified in the same way as the fluorinated methyl group or fluorinated ethyl group in the above-mentioned examples. Any one or more of the carbon atoms in the alkyl group has a singular or plural fluorine atom bonded to it. Of various fluorinated alkyl groups.

Examples of the fluorinated alicyclic hydrocarbon group include a fluorinated cycloalkyl group and the like. Similar to the above-mentioned fluorinated aliphatic hydrocarbon group, in the fluorinated alicyclic hydrocarbon group, the fluorine atom can be bonded to any carbon atom of the alicyclic hydrocarbon group, and the fluorine atom bonded to 1 carbon atom can be Either singular or plural. In addition, the number of carbon atoms to which fluorine atoms are bonded is not particularly limited. Fluorinated alicyclic hydrocarbon groups include, for example: 2-fluorocyclohexyl, 3-fluorocyclohexyl, 4-fluorocyclohexyl and other cyclohexyl groups with one fluorine atom; 2,4-difluorocyclohexyl, 2,6-difluorocyclohexyl, etc. Cyclohexyl having 2 fluorine atoms such as fluorocyclohexyl; cyclohexyl having 3 fluorine atoms such as 2,4,6-trifluorocyclohexyl, etc.

The fluorinated hydrocarbon group may not have a substituent or may have a substituent. The substituent is not particularly limited, and examples thereof include hydrocarbon groups such as alkyl groups, alkoxy groups, hydroxyl groups, carboxyl groups, amino groups, nitro groups, cyano groups, halogen atoms, and the like. A substituent can be used individually by 1 type or in combination of 2 or more types.

(Meth)acrylates containing fluorine atoms [fluorinated (meth)acrylates] include, for example, alkyl (meth)acrylates containing fluorine atoms [fluorinated alkyl (meth)acrylates], fluorine-containing Cycloalkyl (meth)acrylates of atoms [fluorinated cycloalkyl (meth)acrylates], aryl (meth)acrylates containing fluorine atoms [fluorinated aryl (meth)acrylates], etc. .

The (meth)acrylate containing a fluorine atom is preferably a fluorinated alkyl (meth)acrylate (especially a fluorinated alkyl acrylate). Examples of fluorinated alkyl (meth)acrylates include 2,2,2-trifluoroethyl acrylate (trade name "Viscoat 3F" manufactured by Osaka Organic Chemical Industry Co., Ltd.), 2,2,3,3 -Tetrafluoropropyl acrylate (trade name "Viscoat 4F" manufactured by Osaka Organic Chemical Industry Co., Ltd.), 1H,1H,5H-octafluoropentyl acrylate (trade name "Viscoat 4F" manufactured by Osaka Organic Chemical Industry Co., Ltd.) 8F'' etc.), 1H, 1H, 5H-octafluoropentyl methacrylate (trade name "Viscoat 8FM", etc. manufactured by Osaka Organic Chemical Industry Co., Ltd.), 2-(heptafluorononyl) ethyl acrylate (Trade name "FA-108" manufactured by Kyoeisha Chemical Co., Ltd.), 1H, 1H, 2H, 2H-Tridecafluorooctyl acrylate (trade name "Viscoat 13F" manufactured by Osaka Organic Chemical Industry Co., Ltd., etc.) )Wait.

From the viewpoint of low refractive index effect and flexibility, the number of carbon atoms of the fluorinated alkyl group in the fluorinated alkyl (meth)acrylate is 3 or more, preferably 4 or more, and 5 or more is more advantageous. Good, more preferably 6 or more, more preferably 8 or more. From the standpoint of adhesive performance and the like, it is advantageous that the number of carbon atoms of the above-mentioned fluorinated alkyl group is 18 or less, and is preferably 14 or less, preferably 12 or less, and may be 10 or less or 9 or less. In several aspects, the number of carbon atoms of the above-mentioned fluorinated alkyl group may be 7 or less, or may be 5 or less. In addition, in several aspects, the fluorine atom-containing (meth)acrylate is preferably a fluorinated alkyl (meth)acrylate whose carbon at the 1-position of the alkyl group is not bonded to fluorine. For example, 1H ,1H,2H,2H-Tridecafluorooctyl acrylate is a fluorinated alkyl (meth)acrylate that is not bonded to any one of the carbon at the 1 position and the carbon at the 2 position of the alkyl group.

The content of the monomer (M1) in the monomer raw material used to prepare the acrylic polymer (F) may be, for example, 10% by weight or more, 25% by weight or more is appropriate, and it may also be 35% by weight or more. From the viewpoint of easily achieving a lower refractive index adhesive, the content of the above-mentioned monomer (M1) is preferably 40% by weight or more, preferably 45% by weight or more, more preferably 55% by weight or more, and can be 60% by weight or more , Can be 75% by weight or more, can be 85% by weight or more, can be 90% by weight or more, or can be 95% by weight or more. The upper limit of the content of the monomer (M1) in the monomer raw material is not particularly limited, and it may be 100% by weight. In several aspects, from the viewpoint of the cohesiveness of the adhesive, etc., the content of the above-mentioned monomer (M1) is appropriate to be 99.9% by weight or less, and is preferably 99.5 or less, may be 99% by weight or less, and may be 97% by weight or less, and 92% by weight or less. A monomer (M1) can be used individually by 1 type or in combination of 2 or more types.

The monomer raw material used to prepare the acrylic polymer (F) may be a composition containing a copolymerizable monomer in addition to the monomer (M1). The copolymerizable monomer contributes to the introduction of crosslinking points into the acrylic polymer or to increase the cohesive force of the acrylic polymer. The above-mentioned copolymerizable monomers can be used, for example, carboxyl group-containing monomers, hydroxyl group-containing monomers, acid anhydride group-containing monomers, amine group-containing monomers, amine group-containing monomers, monomers having nitrogen atom-containing rings (e.g., N-ethylene One or two or more of functional group-containing monomers such as N-vinyl cyclic amides such as 2-pyrrolidone), sulfonic acid group-containing monomers, and phosphoric acid group-containing monomers. Other examples of copolymerizable monomers include: (meth)acrylic acid containing non-aromatic ring such as alkyl (meth)acrylate, cycloalkyl (meth)acrylate, isobornyl (meth)acrylate, etc. Vinyl ester-based monomers such as esters and vinyl acetate, aromatic vinyl compounds such as styrene, alkoxy-containing monomers, and the like. Specific examples of the copolymerizable monomer include the same monomers that can be used for the preparation of the acrylic polymer (A) described below, but are not limited thereto.

Among several aspects, from the viewpoint of enhancing the cohesive force, etc., it is preferable to use one or more monomers selected from the group consisting of hydroxyl-containing monomers and carboxyl-containing monomers (hereinafter also referred to as "Monomer (M2)") is an acrylic polymer (F) as the above-mentioned copolymerizable monomer. Examples of the hydroxyl-containing monomer are the same as the hydroxyl-containing monomers exemplified for the monomer (m2) described later. Suitable examples of the hydroxyl-containing monomer include 2-hydroxyethyl acrylate or 4-hydroxybutyl acrylate. From the viewpoint of flexibility, 4-hydroxybutyl acrylate is more preferable. The carboxyl group-containing monomer may be the same as the carboxyl group-containing monomer exemplified for the monomer (m2) described later. Suitable examples of the carboxyl group-containing monomer include acrylic acid and methacrylic acid.

The content of the monomer (M2) in the monomer raw material used to prepare the acrylic polymer (F) is not particularly limited, and can be appropriately set so that the desired use effect can be exerted. The content of the monomer (M2) can be, for example, 0.01% by weight or more (preferably 0.1% by weight or more, more preferably 0.5% by weight or more). In several aspects, the content of the aforementioned monomer (M2) can be 0.7% by weight or more of the monomer raw material, can be 0.9% by weight or more, or can be 1.5% by weight or more. The upper limit of the content of the monomer (M2) is not particularly limited, and it can be appropriately set so that the sum of the content of the other monomers does not exceed 100% by weight. From the viewpoint of making the content of the monomer (M1) relatively large and easy to lower the refractive index, the content of the monomer (M2) is appropriately set to 15% by weight or less or 10% by weight, and preferably less than 10 The weight% is preferably less than 5% by weight, can be less than 3% by weight, can be less than 2.5% by weight, or less than 1.5% by weight. The monomer (M2) may not be used.

In several ideal aspects, the monomer raw material used to prepare the acrylic polymer (F) may be a composition containing a hydroxyl-containing monomer as the monomer (M2). The hydroxyl-containing monomer helps to increase the cohesive force or introduce cross-linking points. Suitable examples of the hydroxyl group-containing monomer include hydroxyalkyl (meth)acrylates such as 2-hydroxyethyl acrylate or 4-hydroxybutyl acrylate. From the viewpoint of improving the flexibility in the room temperature region, 4-hydroxybutyl acrylate may be more suitably used. The content of the hydroxyl-containing monomer in the monomer raw material is not particularly limited. For example, it can be 0.01% by weight or more (preferably 0.1% by weight or more, more preferably 0.5% by weight or more). In several aspects, the content of the hydroxyl-containing monomer may be 0.7% by weight or more of the monomer raw material, may be 0.9% by weight or more, or may be 1.5% by weight or more. The upper limit of the content of the hydroxyl group-containing monomer is not particularly limited. For example, it may be 15% by weight or less or 10% by weight or less. In several aspects, from the viewpoint of low refractive index, it is appropriate that the content of the hydroxyl-containing monomer in the monomer raw material is less than 10% by weight, and is preferably less than 5% by weight, and can be less than 3% by weight. , Can be less than 2.5% by weight, or less than 1.5% by weight.

In several aspects, the monomer raw materials used to prepare the acrylic polymer (F) may include copolymerizable monomers other than monomer (M2) (that is, copolymerizable monomers that do not have hydroxyl group-containing and carboxyl group-containing monomers). body). Hereinafter, the copolymerizable monomer may be referred to as "monomer (M3)". As the monomer (M3), those that are not equivalent to the monomer (M2) among the aforementioned various copolymerizable monomers can be used.

The content of the monomer (M3) in the monomer raw material used to prepare the acrylic polymer (F) is not particularly limited, and can be appropriately set so that the desired use effect can be exerted. The content of the monomer (M3) can be, for example, 0.1% by weight or more (preferably 1% by weight or more, more preferably 5% by weight or more). In several aspects, the content of the aforementioned monomer (M2) may be 7% by weight or more of the monomer raw material, may be 10% by weight or more, or may be 15% by weight or more. From the viewpoint of improving flexibility, among several aspects, the content of the above-mentioned monomer (M2) can be 10% by weight or more, 25% by weight or more, 35% by weight or more, or 45% by weight. Above, it can be more than 55% by weight, or more than 60% by weight. The upper limit of the content of the monomer (M3) is not particularly limited, and it can be appropriately set so that the sum of the content of the other monomers does not exceed 100% by weight. The content of the monomer (M3) may be, for example, 90% by weight or less, or 85% by weight or less. From the viewpoint of making the content of the monomer (M1) relatively large and easy to lower the refractive index, the content of the monomer (M3) is preferably 80% by weight or less, and more preferably 70% by weight or less. In several aspects, from the viewpoint of low refractive index, it is appropriate that the content of monomer (M3) in the monomer raw material is less than 60% by weight, preferably less than 50% by weight, and can be less than 45% by weight. , Can be less than 35% by weight, can be less than 20% by weight, can be less than 10% by weight, or less than 5% by weight. The monomer (M3) may not be used.

Suitable examples of monomers that can be used as the monomer (M3) include: (meth)acrylic acid alkyl esters, monomers having a ring containing nitrogen atoms (for example, N-vinyl-2-pyrrolidone and other N-vinyl groups). Non-aromatic ring-containing (meth)acrylates such as cyclic amide), cycloalkyl (meth)acrylate, or isobornyl (meth)acrylate. A monomer (M3) may be used individually by 1 type, and may be used in combination of 2 or more types. For example, the following aspects can be suitably adopted: the aspect in which one type of alkyl (meth)acrylate is used alone, the aspect in which two or more kinds of alkyl (meth)acrylate are used in combination, and the aspect in which alkyl (meth)acrylate is used in combination The use of the base ester and N-vinyl cyclic amide, the combination of the alkyl (meth)acrylate and the non-aromatic ring-containing (meth)acrylate.

For the alkyl (meth)acrylate, for example, a compound represented by the following formula (1) can be suitably used. ^{_{CH 2 = C (R 1)}} COOR 2 (1) Here, in the above-described formula ⁽¹⁾ R 1 is a hydrogen atom or a methyl group. In addition, R ² is a chain alkyl group having 1 to 20 carbon atoms (hereinafter, the range of the number of carbon atoms may be expressed as "C _1-20 "). From the viewpoint of the storage elastic modulus of the adhesive, the alkyl (meth)acrylate ^{of which R 2} is a _{chain alkyl group of C 1-12} (for example, C _2-10 , typically C _4-8) Better. The ^{alkyl (meth)acrylate in which R 2} is a C _1-20 chain alkyl group can be used alone or in combination of two or more kinds. Preferred alkyl (meth)acrylates include n-butyl acrylate and 2-ethylhexyl acrylate.

In several aspects, from the viewpoint of inhibiting the coloration or discoloration (for example, yellowing) of the adhesive, the content of the carboxyl group-containing monomer in the monomer raw material used to prepare the acrylic polymer (F) should be limited. The content of the carboxyl group-containing monomer in the aforementioned monomer raw materials can be, for example, less than 1% by weight, preferably less than 0.5% by weight, more preferably less than 0.3% by weight, and more preferably less than 0.1% by weight (for example, less than 0.05% by weight). As the content of the carboxyl group-containing monomer is limited, the corrosion of metal materials (such as metal wiring or metal film that may be present on the adherend) that can be in contact with or disposed adjacent to the adhesive disclosed herein is suppressed. The point of view is also favorable. The technology disclosed herein can be suitably implemented in the state where the aforementioned monomer raw materials do not contain a carboxyl group-containing monomer. For the same reason, in several aspects, the monomer raw material used to prepare the acrylic polymer (F) contains the content of monomers with acidic functional groups (in addition to carboxyl groups, sulfonic acid groups, phosphoric acid groups, etc.) It is suitable to be restricted. The content of the acidic functional group-containing monomer in the monomer raw material of the above aspect can be applied to the ideal content of the above-mentioned carboxyl group-containing monomer. The technology disclosed here can be suitably implemented in a state where the above-mentioned monomer raw materials do not contain acidic group-containing monomers (that is, the acrylic polymer (F) is in an acid-free state).

The acrylic polymer (F) can be prepared by appropriately employing a known polymerization method in the same manner as the acrylic polymer (A) described later. The weight average molecular weight (Mw) of the acrylic polymer (F) is not particularly limited, and may be, for example, in the range of about 10×10 ⁴ to 500×10 ⁴ , or may be in the range of about 20×10 ⁴ to 200×10 ⁴ . In several aspects, from the viewpoint of adhesion to the adherend or the adjacent layer (which may be a high refractive index layer such as a high refractive index adhesive layer), the Mw of the acrylic polymer (F) is 150×10 ⁴ or less is appropriate, and preferably 120×10 ⁴ or less (for example, 95×10 ⁴ or less), 75×10 ⁴ or less, 68×10 ⁴ or less, or 60×10 ⁴ or less . In addition, in several aspects, from the viewpoint of the cohesiveness of the adhesive, the Mw of the acrylic polymer (F) may be, for example, 30×10 ⁴ or more, 40×10 ⁴ or more, or 50 ×10 ⁴ or more. In order to prepare Mw, conventionally known chain transfer agents can be used according to needs.

Although not particularly limited, from the viewpoint of adhesiveness, it is advantageous that the Tg of the acrylic polymer (F) is about 0°C or less, and preferably about -5°C or less (for example, about -15°C or less or -25°C). ℃ below). In addition, from the viewpoint of the cohesive force of the adhesive layer, the Tg of the acrylic polymer (F) is approximately -75°C or higher, and preferably approximately -70°C or higher (for example, -50°C or higher, further -30°C) above). The Tg of the acrylic polymer (F) can be adjusted by appropriately changing the monomer composition (that is, the type of monomer or the ratio of the amount used when synthesizing the polymer).

When an alkyl (meth)acrylate is used as the monomer (M3), from the viewpoint of easy reduction of the Tg of the acrylic polymer (F), in several aspects, only the above-mentioned alkyl (meth)acrylate is used. It is advantageous for the usage amount of the base ester to be lower than -50°C calculated by the Fox formula, and preferably lower than -55°C, may be lower than -60°C, or lower than -65°C.

(Preparation method of acrylic polymer (F)) In the technique disclosed herein, the method for obtaining the acrylic polymer (F) composed of the above-mentioned monomer components is not particularly limited, and the solution polymerization method, emulsion polymerization method, bulk polymerization method, suspension polymerization method, Known polymerization methods such as photopolymerization method. Among several aspects, the solution polymerization method can be suitably used. The polymerization temperature during solution polymerization can be appropriately selected according to the types of monomers and solvents used, and the types of polymerization initiators. For example, it can be set at around 20°C to 170°C (typically around 40°C to 140°C).

The solvent (polymerization solvent) used in the solution polymerization can be appropriately selected from conventionally known organic solvents. For example, any one solvent or a mixed solvent of two or more selected from the following can be used: aromatic compounds such as toluene (typically aromatic hydrocarbons); acetates such as ethyl acetate; hexane or cyclic Aliphatic or alicyclic hydrocarbons such as hexane; haloalkanes such as 1,2-dichloroethane; lower alcohols such as isopropanol (for example, monohydric alcohols with 1 to 4 carbon atoms); tertiary butyl methyl Ethers such as ethers; ketones such as methyl ethyl ketone, etc.

The initiator used for the polymerization can be appropriately selected from known polymerization initiators according to the type of polymerization method. For example, one kind or two or more kinds of azo polymerization initiators such as 2,2'-azobisisobutyronitrile (AIBN) can be suitably used. Other examples of polymerization initiators include persulfates such as potassium persulfate; peroxide-based initiators such as benzyl peroxide and hydrogen peroxide; substituted ethane-based initiators such as phenyl substituted ethane; Aromatic carbonyl compounds, etc. As yet another example of the polymerization initiator, an oxygen-reducing initiator in which a peroxide and a reducing agent are combined can be cited. A polymerization initiator can be used individually by 1 type or in combination of 2 or more types. The usage amount of the polymerization initiator may be a usual usage amount, for example, it can be selected within the range of about 0.005 to 1 part by weight (typically about 0.01 to 1 part by weight) relative to 100 parts by weight of the monomer component.

In the above polymerization, various chain transfer agents known in the past can be used as needed. For example, mercaptans such as n-dodecyl mercaptan, tertiary dodecyl mercaptan, thioglycolic acid, and α-thioglycerin can be used. Alternatively, a chain transfer agent containing no sulfur atom (non-sulfur tethered chain transfer agent) can also be used. Examples of non-sulfur chain transfer agents include anilines such as N,N-dimethylaniline and N,N-diethylaniline; terpenoids such as α-pinene and terpinolene; α-methylbenzene Styrenes such as ethylene, α-methylstyrene dimer, etc. A chain transfer agent can be used individually by 1 type or in combination of 2 or more types. The usage amount when using a chain transfer agent can be set to about 0.01 to 1 part by weight with respect to 100 parts by weight of the monomer raw material, for example.

The weight average molecular weight (Mw) of the base polymer is not particularly limited, and may be, for example, in the range of about 10×10 ⁴ to 500×10 ⁴ . From the point of view of adhesion performance, the Mw of the base polymer should be about 20×10 ⁴ to 400×10 ⁴ (preferably about 30×10 ⁴ to 150×10 ⁴ , for example, about 50×10 ⁴ to 130×10 ⁴ ).

Here, the Mw of the polymer can be obtained by converting into polystyrene by gel permeation chromatography (GPC). Specifically, it can be obtained by using the brand name "HLC-8220GPC" (manufactured by Tosoh Corporation) as a GPC measuring device and measuring under the following conditions. [GPC measurement conditions] Sample concentration: 0.2% by weight (tetrahydrofuran solution) Sample injection volume: 10µL Eluent: Tetrahydrofuran (THF) Flow (velocity): 0.6mL/min Column temperature (measurement temperature): 40℃ String: Sample column: 1 piece of product name "TSKguardcolumn SuperHZ-H" + 2 pieces of product name "TSKgel SuperHZM-H" (manufactured by Tosoh) Reference column: trade name "TSKgel SuperH-RC" 1 (manufactured by Tosoh) Detector: Differential Refractometer (RI) Standard sample: polystyrene

(Crosslinking agent) In the technique disclosed herein, the adhesive composition used to form the low-refractive-index adhesive layer may contain a cross-linking agent as needed in order to adjust the cohesive force of the adhesive. As the crosslinking agent, isocyanate-based crosslinking agents, epoxy-based crosslinking agents, aziridine-based crosslinking agents, azoline-based crosslinking agents, melamine-based resins, metal chelate-based crosslinking agents, etc. can be used in the adhesive. A well-known crosslinking agent in the field. Among them, an isocyanate-based crosslinking agent can be suitably used. As another example of the crosslinking agent, a monomer having two or more ethylenically unsaturated groups in one molecule, that is, a polyfunctional monomer, can be cited. A crosslinking agent can be used individually by 1 type or in combination of 2 or more types. Regarding the specific examples or usage amount of the crosslinking agent, the description of the crosslinking agent that can be used for the adhesive composition used to form the high refractive index adhesive layer can also be applied to the description of the crosslinking agent used to form the low refractive index adhesive layer. Adhesive composition.

In the case where the adhesive composition for forming the low-refractive-index adhesive layer includes a crosslinking agent, the above-mentioned crosslinking agent can be suitably used, for example, an isocyanate-based crosslinking agent. In several aspects, from the viewpoint of adhesion to the adherend or adjacent layers, the amount of the isocyanate-based crosslinking agent used can be less than 0.5, for example, relative to 100 parts by weight of the acrylic polymer (F). Parts by weight can be less than 0.3 parts by weight, can be less than 0.2 parts by weight, or less than 0.15 parts by weight. In addition, from the viewpoint of properly exerting the effect of the crosslinking agent, in several aspects, the amount of the isocyanate-based crosslinking agent used can be, for example, 0.005 parts by weight relative to 100 parts by weight of the acrylic polymer (F). The above may be 0.01 parts by weight or more, 0.05 parts by weight or more, or 0.08 parts by weight or more.

(Other additives) The low refractive index adhesive may contain plasticizing materials, leveling agents, tackifiers, inorganic particles, and other additives as optional components. Optional components such as these can be appropriately selected from the same ones that can be used for the high-refractive-index adhesive layer, and an appropriate amount can be used.

<High refractive index adhesive> The adhesive (low refractive index adhesive) disclosed here can be laminated with an adhesive with a relatively high refractive index (high refractive index adhesive) in relation to the adhesive Use it in its form. In the use aspect, the adhesive is a high refractive index n ₁ and the refractive index of the low refractive index layer ₂ of the adhesive ratio (n ₁ / n _2), for example, may be greater than 1.00 n, may be about 1.01 or more, is About 1.02 or more is appropriate, and it may also be about 1.03 or more. In several aspects, it is advantageous for the ratio (n ₁ /n ₂ ) to be about 1.05 or higher, and is preferably about 1.07 or higher, preferably about 1.10 or higher, and may also be about 1.11 or higher. The upper limit of the ratio (n ₁ /n ₂ ) is not particularly limited. Among several aspects, the adhesive properties of the adhesive surface formed by the high refractive index adhesive and/or the adhesive surface formed by the low refractive index adhesive, or the transparency of each adhesive layer, further include From the viewpoint of the transparency of the laminated sheet of the high-refractive index adhesive and the low-refractive index adhesive, the ratio (n ₁ /n ₂ ) can be, for example, about 1.20 or less, about 1.18 or less, or about 1.16 or less. It is about 1.14 or less, and may also be about 1.12 or less.

In several aspects, the difference between the refractive index n ₁ of the high refractive index adhesive and the refractive index n ₂ of the low refractive index adhesive, that is, the refractive index difference (n ₁ -n ₂ ), may be greater than 0.00, for example, It can be 0.01 or more, it can be 0.02 or more, it can be 0.03 or more, it can be 0.05 or more, it can be 0.10 or more, it can be 0.15 or more, it can be 0.20 or more, or it can be 0.25 or more. The upper limit of the refractive index difference (n ₁ -n ₂ ) is not particularly limited. Among several aspects, the adhesive properties of the adhesive surface formed by the high refractive index adhesive and/or the adhesive surface formed by the low refractive index adhesive, or the transparency of each adhesive layer, further include From the viewpoint of the transparency of the laminated sheet of the high refractive index adhesive and the low refractive index adhesive, the refractive index difference (n ₁ -n ₂ ) may be 0.30 or less, 0.26 or less, 0.21 or less, or 0.18 or less, but also 0.16 or less.

The ideal lower limit of the refractive index of the high refractive index adhesive can be different in relation to the refractive index of the low refractive index adhesive, so it is not limited by a specific range. For example, the refractive index of the high refractive index adhesive may be 1.45 or higher, 1.47 or higher, 1.50 or higher, 1.53 or higher, 1.55 or higher, or 1.56 or higher. The use of a high refractive index adhesive with a higher refractive index is ideal from the viewpoint of increasing the refractive index difference with the low refractive index adhesive, and from the viewpoint of increasing the design freedom of the low refractive index adhesive Also beneficial.

In several aspects, the refractive index of the high refractive index adhesive can be, for example, 1.570 or higher. It is advantageous to be higher than 1.570, and is preferably 1.580 or higher, more preferably 1.585 or higher, and more preferably 1.590 or higher (for example, 1.595 or higher). With the high refractive index adhesive layer having the refractive index, the relationship between the relative refractive index of the high refractive index adhesive layer and the low refractive index adhesive layer as described above can be used to effectively control the transmission of low refractive index adhesives The light behavior of the agent layer and/or the high refractive index adhesive layer. In several aspects of the technology disclosed herein, the refractive index of the high refractive index adhesive can be, for example, 1.600 or greater or greater than 1.600, 1.605 or greater or greater than 1.605, or 1.610 or greater or greater than 1.610. The ideal upper limit of the refractive index of the high refractive index adhesive may vary depending on the refractive index of adjacent layers, etc., so it is not limited by a specific range. In several aspects, considering the balance with adhesive properties or transparency, the refractive index of the high refractive index adhesive can be, for example, 1.700 or less, 1.670 or less, or 1.650 or less.

(Storage elastic modulus G') In the technology disclosed here, the storage elastic modulus G'(hereinafter also referred to as "storage elastic modulus _G'V1 (25)") of the high refractive index adhesive at 25°C can be adapted to Appropriate settings such as the purpose of use or the state of use are not limited by the specific range. The storage elastic modulus _G'V1 (25) may be about 700 kPa or less, for example. In several aspects, from the viewpoint of ease of attachment to the _{adherend, it is advantageous for the storage elastic modulus G'V1} (25) to be approximately 600kPa or less, preferably 500kPa or less, more preferably 400kPa or less (For example, 350kPa or less). _{In several aspects, the storage elastic modulus G'V1} (25) is to improve the flexibility of the high refractive index adhesive at room temperature (for example, 25°C) so as to easily adhere to the adherend. It is advantageous to be approximately 330 kPa or less, and preferably 300 kPa or less. In more attention or attachment flexibility at room temperature of several aspects of the region, the storage elastic modulus G _'V1 (25), for example, may be less than 270kPa 250kPa or less, and less than 200kPa is advantageous and should be less than 180kPa, preferably less than 160kPa (for example, less than 140kPa). In several aspects, the storage elastic modulus _G'V1 (25) can be less than 100kPa or less than 90kPa. The lower limit of the storage elastic modulus _G'V1 (25) is not particularly limited, but from the viewpoint of workability or handling properties, for example, it may be 30 kPa or more, 50 kPa or more, or 70 kPa or more. In several aspects, considering the high refractive index, the storage elastic modulus _G'V1 (25) can be 100kPa or more, 150kPa or more, 200kPa or more, 250kPa or more, or 300kPa or more.

In the technology disclosed herein, the storage elastic modulus G'(hereinafter also referred to as "storage elastic modulus _G'V1 (50)") of the high refractive index adhesive layer at 50° C. is not particularly limited, and may be less than 100 kPa, for example. In several aspects, the storage elastic modulus G _'V1 (50) is less than 60kPa is suitable, and should be less than 40kPa, more should be less than 38 kPa (e.g. less than 36kPa). For the high refractive index adhesive with limited storage elastic modulus _G'V1 (50), moderate heating can be used to easily improve the adhesion to the adherend according to requirements, thereby improving the adhesion to the adherend. Body adhesion. The lower limit of the storage elastic modulus _G'V1 (50) is not particularly limited. In several aspects, a perspective view of the heat resistance and the like, the storage elastic modulus G _'V1 (50) can be, for example, more than 10kPa, more can be 15kPa, 20kPa or more may be, may also be more than 23kPa.

In the several aspects of the technology disclosed herein, the high refractive index adhesive layer should satisfy at least one of the following conditions: (a) The storage elastic modulus _G'V1 (25) is 350kPa or less (preferably less than 200kPa _, such as 180kPa) or less); and (b) the storage elastic modulus G _'V1 (50) is less than 60kPa (should be less than 50kPa, more should be less than 40kPa, for example less than 38kPa). The high-refractive-index adhesive layer that satisfies at least the above-mentioned condition (a) is ideal from the viewpoint of adhesion or flexibility to the adherend in a room temperature region (for example, 25°C). The high-refractive-index adhesive layer that satisfies at least the above condition (b) is preferred because it can easily improve the adhesion (adhesion) to the adherend by heating to a temperature slightly higher than room temperature. Adhesive sheets with a high refractive index adhesive layer that does not satisfy the above condition (a) and satisfy the above (b) can be used as a heat-activated adhesive sheet, and its initial reworkability (re-attachment) when attached at room temperature Good adhesion), by heating to a temperature slightly higher than room temperature, the peel strength from the adherend can be effectively improved. The above-mentioned thermal activation can also be performed by heating the adhesive sheet to a temperature slightly higher than room temperature when it is attached to the adherend. The above-mentioned so-called temperature slightly higher than room temperature is, for example, about 60°C or lower, and preferably about 55°C or lower (for example, about 50°C or lower).

Among the several aspects of the technology disclosed here, the ratio of the storage elastic modulus _G'V1 (50) [kPa] to the storage elastic modulus _G'V1 (25) [kPa], that is, the storage elastic modulus ratio _G'V1 (50)/G' _V1 (25) is, for example, 70% or less, 40% or less, 30% or less, or 20% or less. _{Adhesive sheets with a small G'V1} (50)/G' _V1 (25) high refractive index adhesive layer are suitable for use as the above-mentioned thermally activated adhesive sheets. _{The lower limit of G'V1} (50)/G' _V1 (25) is not particularly limited. _G'V1 (50)/G' _V1 (25) is, for example, 5% or more, and from the viewpoint of heat resistance, it is preferably 10% or more, may be 12% or more, or may be 15% or more.

The storage elastic modulus _G'V1 (25)およびG' _V1 (50) can be obtained by dynamic viscoelasticity measurement, and _G'V1 (50)/G' _V1 (25) can be calculated from the result. The dynamic viscoelasticity measurement can be performed by a conventional method using a commercially available dynamic viscoelasticity measurement device. For example, ARES manufactured by TA Instruments or its equivalent can be used under the following measurement conditions. The sample for measurement is to use the adhesive layer of the evaluation object to be laminated according to the needs and adjusted to a thickness of approximately 1.5mm. [Measurement conditions] Deformation mode: Torsion measurement frequency: 1Hz Heating rate: 5°C/min Shape: Parallel plate 7.9mmφ

The storage elastic modulus _G'V1 (25), _G'V1 (50) and the storage elastic modulus ratio (G' _V1 (50)/G' _V1 (25)) can be selected by selecting the base polymer that constitutes the adhesive The composition of the monomer components (for example, select the type and content of the monomer (m1) described below), whether to use a crosslinking agent and select the type and amount of use, whether to use the refractive index enhancer or plasticizing material described below, and select the type and use The amount and so on to adjust. For example, as the monomer (m1), in addition to the first monomer which is the main component of the monomer (m1), a smaller amount of a second monomer having a different chemical structure from the first monomer can also be used. _{Combining the above-mentioned first monomer to use, in addition to reducing G'V1} (50) when the first monomer is used alone as the monomer (m1), it can _{also make G'V1} (50)/G' _V1 (25) )reduce.

The type of adhesive constituting the high refractive index adhesive layer is not particularly limited. The above-mentioned adhesives may include acrylic polymers, rubber-based polymers (natural rubber, synthetic rubber, mixtures of these, etc.), polyester-based polymers, and urethane-based polymers that can be used in the field of adhesives. , Polyether polymer, silicone polymer, polyamide polymer, fluorine polymer It is a structural polymer that is shaped by an agent, hereinafter also referred to as "base polymer"). From the viewpoints of adhesive performance and cost, an adhesive containing an acrylic polymer or a rubber polymer as the base polymer can be suitably used. Among them, acrylic polymer is suitable as the adhesive of the base polymer (acrylic adhesive). The technique disclosed here is suitable to be implemented in a state where an acrylic adhesive is used.

Hereinafter, the high-refractive-index adhesive layer composed of acrylic adhesive is mainly described, but it is not intended to limit the high-refractive-index adhesive layer in the technology disclosed here to the acrylic adhesive layer.

(Acrylic polymer (A)) The high refractive index adhesive layer disclosed here can be an acrylic adhesive layer. The acrylic polymer, which is the base polymer of the acrylic adhesive layer, preferably contains an aromatic ring-containing monomer (m1) as a monomer component constituting the acrylic polymer. That is, it is preferably an acrylic polymer containing an aromatic ring-containing monomer (m1) as a monomer unit. Hereinafter, the acrylic polymer is also referred to as "acrylic polymer (A)".

(Single (m1)) As the monomer (m1), a compound containing at least one aromatic ring and at least one ethylenically unsaturated group in one molecule can be used. The monomer (m1) can be used singly or in combination of two or more.

Examples of the above-mentioned ethylenically unsaturated groups include (meth)acryloyl groups, vinyl groups, and (meth)allyl groups. From the viewpoint of polymerization reactivity, it is preferably a (meth)acryloyl group, and from the viewpoint of flexibility or adhesiveness, an acryloyl group is more preferable. From the viewpoint of suppressing the decrease in the flexibility of the adhesive, as the monomer (m1), a compound (ie, a monofunctional monomer) containing one ethylenically unsaturated group in one molecule can be suitably used.

The number of aromatic rings contained in 1 molecule of the compound that can be used as the monomer (m1) may be 1, or may be 2 or more. The upper limit of the number of aromatic rings contained in the monomer (m1) is not particularly limited. For example, it may be 16 or less. In several aspects, from the viewpoint of the ease of preparation of the acrylic polymer (A) or the transparency of the adhesive, the number of the above-mentioned aromatic rings can be, for example, 12 or less, preferably 8 or less, and more preferably 6 Below, it may be 5 or less, 4 or less, 3 or less, or 2 or less.

The aromatic ring of the compound that can be used as the monomer (m1) can be, for example, a benzene ring (which can be a part of a biphenyl structure or a benzene ring); naphthalene ring, indene ring, azulene ring, anthracene ring, phenanthrene ring The carbocyclic ring such as the condensed ring; can also be, for example, pyridine ring, pyrimidine ring, pyridine ring, pyrrolidine ring, tripyridine ring, pyrrole ring, pyrazole ring, imidazole ring, triazole ring, azole ring, iso-㗁Heterocycles such as azole ring, thiazole ring and thiophene ring. The heteroatoms contained as ring constituent atoms in the heterocyclic ring may be, for example, one or two or more selected from the group consisting of nitrogen, sulfur, and oxygen. In several aspects, the heteroatom constituting the heterocyclic ring may be one or both of nitrogen and sulfur. The monomer (m1) may also have a structure in which 1 or 2 or more carbocyclic rings and 1 or 2 or more heterocyclic rings have been condensed like the dinaphthothiophene structure, for example.

The above-mentioned aromatic ring (preferably a carbocyclic ring) may have 1 or 2 or more substituents on the ring constituent atoms, or may not have a substituent. When it has a substituent, the substituent can be exemplified by an alkyl group, an alkoxy group, an aryloxy group, a hydroxyl group, a halogen atom (a fluorine atom, a chlorine atom, a bromine atom, etc.), a hydroxyalkyl group, a hydroxyalkoxy group, and a glycidoxy group. Base, etc., but not subject to such restrictions. In the substituents containing carbon atoms, the number of carbon atoms contained in the substituents is preferably 1 to 4, more preferably 1 to 3, and may be 1 or 2, for example. In several aspects, the above-mentioned aromatic ring may be an aromatic ring having no substituents on the constituent atoms of the ring, or may have a constituent selected from the group consisting of an alkyl group, an alkoxy group, and a halogen atom (such as bromine). Atom) constitutes an aromatic ring of 1 or more substituents in the group. In addition, the aromatic ring of the monomer (m1) has a substituent on the ring constituent atoms, which means that the aromatic ring has a substituent other than the substituent having an ethylenically unsaturated group.

The aromatic ring and the ethylenically unsaturated group may be directly bonded, or may be bonded via a linking group. The above-mentioned linking group may include, for example, 1 or 2 selected from the group consisting of alkylene, oxyalkylene, poly(oxyalkylene), phenyl, alkylphenyl, alkoxyphenyl, and these groups Groups with the above hydrogen atoms substituted by hydroxy groups (for example, hydroxyalkylene groups), oxy groups (-O- groups), thiooxy groups (-S- groups), etc., groups with more than one or two structures . In several aspects, an aromatic ring-containing monomer having a structure in which an aromatic ring is directly bonded to an ethylenic A group consisting of a linking group in the group constitutes an aromatic ring-containing monomer with a structure that is bonded. The number of carbon atoms of the above-mentioned alkylene group and the above-mentioned oxyalkylene group is preferably 1 to 4, more preferably 1 to 3, and may be 1 or 2, for example. The repeating number of the oxyalkylene unit in the above-mentioned poly(oxyalkylene) group may be 2 to 3, for example.

Examples of compounds that can be suitably used as the monomer (m1) include aromatic ring-containing (meth)acrylates and aromatic ring-containing vinyl compounds. The aromatic ring-containing (meth)acrylate and the aromatic ring-containing vinyl compound can be used individually by 1 type or in combination of 2 or more types. One or more types of aromatic ring-containing (meth)acrylates and one or more types of aromatic ring-containing vinyl compounds can also be used in combination.

The content of the monomer (m1) in the monomer component constituting the acrylic polymer (A) is not particularly limited, and can be set to achieve the desired refractive index and adhesion characteristics (such as peel strength, flexibility, etc.) and/ Or an adhesive layer with optical properties (such as total light transmittance, haze value, etc.). In several aspects, the content of the monomer (m1) in the above-mentioned monomer component may be, for example, 30% by weight or more, preferably 50% by weight or more, 60% by weight or more, or 70% by weight or more. . From the viewpoint of the ease of obtaining a higher refractive index, in several ideal situations, the content of the above monomer (m1) can be, for example, greater than 70% by weight, 75% by weight or more, 80% by weight or more, It is 85% by weight or more, may be 90% by weight or more, or may be 95% by weight or more. The upper limit of the content of the monomer (m1) in the monomer component is 100% by weight. From the viewpoint of balancing high refractive index and adhesion properties and/or optical properties, it is advantageous to set the content of the above monomer (m1) to be less than 100% by weight, for example, preferably about 99% by weight or less, more preferably 98 The weight% or less may be 97 weight% or less, or 96 weight% or less. In several aspects, the content of the aforementioned monomer (m1) may be 93% by weight or less, 90% by weight or less, 80% by weight or less, or 75% by weight or less. In several aspects where more emphasis is placed on adhesion properties and/or optical properties, the content of the monomer (m1) in the monomer component may be 70% by weight or less, 60% by weight or less, or 45% by weight %the following.

Among the several aspects of the technology disclosed here, in view of the ease of obtaining a higher refractive index effect, a monomer having two or more aromatic rings (preferably carbocyclic) per molecule can be suitably used as the monomer (m1). Examples of monomers having two or more aromatic rings in one molecule (hereinafter also referred to as "monomers containing multiple aromatic rings") include: monomers having a structure in which two or more non-condensed aromatic rings are bonded via a linking group Monomers, monomers with a structure where two or more non-condensed aromatic rings are directly chemically bonded (that is, without intervening other atoms), monomers with a condensed aromatic ring structure, monomers with a turbid structure, and a dinaphthothiophene structure Monomers, monomers with dibenzothiophene structure, etc. The monomer containing a plurality of aromatic rings can be used alone or in combination of two or more kinds.

The above-mentioned linking group may be, for example, an oxy group (-O-), a thiooxy group (-S-), an oxyalkylene group (for example, -O-(CH ₂ ) _n -group, where n is 1 to 3, and Preferably 1), thiooxyalkylene (for example -S-(CH ₂ ) _n -group, where n is 1~3, and preferably 1), straight-chain alkylene (ie -(CH ₂₎ ) _n -group, where n is 1 to 6, and preferably 1 to 3), the alkylene group in the above-mentioned oxyalkylene group, the above-mentioned thiooxyalkylene group and the above-mentioned linear alkylene group has been partially halogenated or Fully halogenated groups, etc. From the viewpoint of the flexibility of the adhesive, etc., suitable examples of the above-mentioned linking group include an oxy group, a thiooxy group, an oxyalkylene group, and a linear alkylene group. Specific examples of monomers having a structure in which two or more non-condensed aromatic rings are bonded via a linking group include phenoxybenzyl (meth)acrylate (e.g., m-phenoxybenzyl (meth)acrylate) , Thiophenoxy benzyl (meth)acrylate, benzyl benzyl (meth)acrylate, etc.

The monomers of the above-mentioned two or more non-condensed aromatic rings directly chemically bonded structure can be, for example, (meth)acrylate containing biphenyl structure, (meth)acrylate containing triphenyl structure, and biphenyl containing vinyl group. Wait. Specific examples include o-phenylphenol (meth)acrylate, biphenylmethyl (meth)acrylate, and the like.

Examples of the monomer having a condensed aromatic ring structure include naphthalene ring-containing (meth)acrylate, anthracene ring-containing (meth)acrylate, vinyl-containing naphthalene, and vinyl-containing anthracene. Specific examples include: 1-naphthyl methyl (meth) acrylate (alias: 1-naphthyl methyl (meth) acrylate), hydroxyethylated β-naphthol acrylate, 2-naphthyl ethyl ( Meth)acrylate, 2-naphthoxyethyl acrylate, 2-(4-methoxy-1-naphthoxy)ethyl (meth)acrylate, and the like.

Specific examples of the above-mentioned monomers having a chlorophyll structure include 9,9-bis(4-hydroxyphenyl) chlorophyll (meth)acrylate, 9,9-bis[4-(2-hydroxyethoxy)phenyl ] 茀(meth)acrylate etc. In addition, a monomer having a fluorine structure includes a structural part in which two benzene rings are directly chemically bonded, so it is included in the concept of a monomer having a structure in which two or more non-condensed aromatic rings are directly chemically bonded.

The monomer having a dinaphthothiophene structure may include (meth)acryloyl-containing dinaphthothiophene, vinyl-containing dinaphthothiophene, (meth)allyl-containing dinaphthothiophene, and the like. Specific examples include: (meth)acryloyloxymethyl dinaphthothiophene (for example, CH ₂ CH(R ¹ )C(O)OCH _2- The structure of the compound; where R ¹ is a hydrogen atom or a methyl group), (meth)acryloyloxyethyl dinaphthothiophene (for example, a CH ₂ CH(R ¹ )C(O)OCH(CH ₃ )- or CH ₂ CH(R ¹ )C(O)OCH ₂ CH ₂ -A compound of the structure; here, R ¹ is a hydrogen atom or a methyl group) , Vinyl dinaphthothiophene (for example, a compound with a vinyl bond at position 5 or 6 of the naphthothiophene ring), (meth)allyloxy dinaphthothiophene, etc. In addition, a single system with a dinaphthothiophene structure includes a naphthalene structure and a structure in which a thiophene ring and two naphthalene structures have been condensed, and it is also included in the above-mentioned concept of a monomer with a condensed aromatic ring structure. .

The above-mentioned monomers having a dibenzothiophene structure include (meth)acrylic acid group-containing dibenzothiophene, vinyl group-containing dibenzothiophene, and the like. In addition, the monomer having a dibenzothiophene structure is included in the above-mentioned concept of a monomer having a condensed aromatic ring structure because it has a structure in which a thiophene ring and two benzene rings have been condensed. In addition, the dinaphthothiophene structure and the dibenzothiophene structure do not belong to the structure in which two or more non-condensed aromatic rings are directly chemically bonded.

As the monomer (m1) of the technology disclosed here, a monomer having one aromatic ring (preferably a carbocyclic ring) in one molecule can also be used. Monomers with one aromatic ring in one molecule, for example, help improve the flexibility of the adhesive, adjust the adhesive properties, and improve transparency. In several aspects, from the viewpoint of increasing the refractive index of the adhesive, a monomer having one aromatic ring in one molecule is preferably used in combination with a monomer containing multiple aromatic rings.

Examples of monomers having one aromatic ring in one molecule include: benzyl (meth)acrylate, methoxybenzyl (meth)acrylate, phenyl (meth)acrylate, ethoxylated phenol (formaldehyde) Base) acrylate, phenoxypropyl (meth)acrylate, phenoxybutyl (meth)acrylate, cresyl (meth)acrylate, 2-hydroxy-3-phenoxypropyl (meth)acrylate, Carbon-containing aromatic ring (meth)acrylate such as chlorobenzyl (meth)acrylate; 2-(4,6-dibromo-2-second-butylphenoxy)ethyl (meth)acrylate, 2-(4,6-Dibromo-2-isopropylphenoxy)ethyl(meth)acrylate, 6-(4,6-dibromo-2-dibutylphenoxy)hexyl( Meth) acrylate, 6-(4,6-dibromo-2-isopropylphenoxy)hexyl (meth)acrylate, 2,6-dibromo-4-nonylphenyl acrylate, 2 ,6-Dibromo-4-dodecylphenyl acrylate and other bromine-containing substituted aromatic ring (meth)acrylates; styrene, α-methylstyrene, vinyl toluene, tertiary butyl styrene, etc. Carbon aromatic ring vinyl compounds; N-vinylpyridine, N-vinylpyrimidine, N-vinylpyridine, N-vinylpyrrole, N-vinylimidazole, N-vinyl azole and other heteroaromatic rings have vinyl substituents The compound and so on.

The monomer (m1) can also be a monomer having a structure in which an oxyethylene chain is sandwiched between the ethylenically unsaturated group and the aromatic ring in the above-mentioned various aromatic ring-containing monomers. As mentioned above, the monomer in which the oxyethylene chain is sandwiched between the ethylenic unsaturated group and the aromatic ring can be regarded as the ethoxylate of the original monomer. The repeating number of the oxyethylene unit (-CH ₂ CH ₂ O-) in the above oxyethylene chain is typically 1 to 4, preferably 1 to 3, more preferably 1 to 2, and for example, 1. Specific examples of ethoxylated aromatic ring-containing monomers include: ethoxylated ortho-phenylphenol (meth)acrylate, ethoxylated nonphenol (meth)acrylate, ethoxylated methyl acrylate Phenol (meth)acrylate, phenoxyethyl (meth)acrylate, phenoxydiethylene glycol di(meth)acrylate, etc.

The content of the monomer containing multiple aromatic rings in the monomer (m1) is not particularly limited. For example, it may be 5% by weight or more, 25% by weight or more, or 40% by weight or more. In several aspects, from the viewpoint of easy realization of an adhesive with a higher refractive index, the content of the monomer containing a plurality of aromatic rings in the monomer (m1) may be, for example, 50% by weight or more, and preferably It is 70% by weight or more, it may be 85% by weight or more, it may be 90% by weight or more, or it may be 95% by weight or more. The monomer (m1) may be substantially 100% by weight of a monomer containing a plurality of aromatic rings. That is, as the monomer (m1), only one type or two or more types of monomers containing a plurality of aromatic rings may be used. In addition, in several aspects, for example, considering the balance of high refractive index and adhesive properties and/or optical properties, the content of the monomer containing multiple aromatic rings in the monomer (m1) can be less than 100% by weight, which can be It is 98% by weight or less, may be 90% by weight or less, may be 80% by weight or less, or may be 65% by weight or less. In several aspects, considering the adhesive properties and/or optical properties, the content of the monomer containing multiple aromatic rings in the monomer (m1) may be 70% by weight or less, 50% by weight or less, or 25% by weight or less may also be 10% by weight or less. The technique disclosed here can be implemented even when the content of the monomer containing a plurality of aromatic rings in the monomer (m1) is less than 5% by weight. It is also possible not to use monomers containing multiple aromatic rings.

The content of monomers containing multiple aromatic rings in the monomer components constituting the acrylic polymer is not particularly limited, and can be set to achieve the desired refractive index and adhesion characteristics (such as peel strength, flexibility, etc.) and/ Or an adhesive layer with optical properties (such as total light transmittance, haze value, etc.). The content of the monomer containing a plurality of aromatic rings in the above-mentioned monomer component may be, for example, 3% by weight or more, 10% by weight or more, or 25% by weight or more. In several aspects, from the viewpoint of easy realization of an adhesive with a higher refractive index, the content of the monomer containing multiple aromatic rings in the above-mentioned monomer component can be, for example, greater than 35% by weight, preferably greater than 50% by weight %, can be more than 70% by weight, can be more than 75% by weight, can be more than 85% by weight, can be more than 90% by weight, or more than 95% by weight. The content of the monomer containing multiple aromatic rings in the above monomer components can be 100% by weight, but from the viewpoint of balancing high refractive index and adhesive properties and/or optical properties, it is advantageous to set it to less than 100% by weight , It should be about 99% by weight or less, preferably 98% by weight or less, 96% by weight or less, 93% by weight or less, 90% by weight or less, 85% by weight or less, and 80% by weight or less. The weight% or less may also be 75 weight% or less. In several aspects, considering the adhesive properties and/or optical properties, the content of the monomers containing multiple aromatic rings in the above-mentioned monomer components may be 70% by weight or less, 50% by weight or less, or 25% by weight. The weight% or less may be 15 weight% or less, or may be 5 weight% or less. The technology disclosed here can be implemented even when the content of the monomer containing multiple aromatic rings in the above-mentioned monomer component is less than 3% by weight.

Among several aspects of the technology disclosed herein, a high refractive index monomer can be preferably used as at least a part of the monomer (m1). Here, "high refractive index monomer" means a monomer whose refractive index is, for example, about 1.510 or more, preferably about 1.530 or more, and more preferably about 1.550 or more. The upper limit of the refractive index of the high refractive index monomer is not particularly limited, but from the viewpoint of ease of preparation of the adhesive composition or ease of compatibility with flexibility suitable as an adhesive, for example, it is 3.000 or less, and can be 2.500 Below, it may be 2.000 or less, 1.900 or less, 1.800 or less, or 1.700 or less. A high refractive index monomer can be used individually by 1 type or in combination of 2 or more types. In addition, the refractive index of the monomer was measured using an Abbe refractometer under the conditions of a measurement wavelength of 589 nm and a measurement temperature of 25°C. The Abbe refractometer can use the type "DR-M4" made by ATAGO or its equivalent. When the manufacturer provides a nominal value of the refractive index at 25°C, the nominal value can be used.

The above-mentioned high-refractive-index monomer can suitably adopt the one having the refractive index from the compounds contained in the concept of the aromatic ring-containing monomer (m1) disclosed herein (for example, the compounds and compound groups exemplified above). Specific examples include: m-phenoxybenzyl acrylate (refractive index: 1.566, homopolymer Tg: -35°C), 1-naphthalene methacrylate (refractive index: 1.595, homopolymer Tg: 31 °C), ethoxylated ortho-phenylphenol acrylate (repetition number of oxyethylene unit: 1, refractive index: 1.578), benzyl acrylate (refractive index (nD20): 1.519, homopolymer Tg: 6 ℃), phenoxyethyl acrylate (refractive index (nD20): 1.517, Tg of homopolymer: 2℃), phenoxy diethylene glycol acrylate (refractive index: 1.510, Tg of homopolymer: -35 ℃), 6-acryloyloxymethyl dinaphthothiophene (6MDNTA, refractive index: 1.75), 6-methacryloyloxymethyl dinaphthothiophene (6MDNTMA, refractive index: 1.726), 5-propylene Acrylic oxyethyl dinaphthothiophene (5EDNTA, refractive index: 1.786), 6-propenyl oxyethyl dinaphthothiophene (6EDNTA, refractive index: 1.722), 6-vinyl dinaphthothiophene (6VDNT, Refractive index: 1.802), 5-vinyl dinaphthothiophene (abbreviation: 5VDNT, refractive index: 1.793), etc., but not limited by these.

The content of the high refractive index monomer (that is, the aromatic ring-containing monomer having a refractive index of about 1.510 or more, preferably about 1.530 or more, and more preferably about 1.550 or more) in the monomer (m1) is not particularly limited, and may be, for example, 5% by weight or more, 25% by weight or more, 35% by weight or more, or 40% by weight or more. In several aspects, from the viewpoint of easily obtaining a higher refractive index, the content of the high refractive index monomer in the monomer (m1) can be, for example, 50% by weight or more, and preferably 70% by weight or more. It is 85% by weight or more, may be 90% by weight or more, or may be 95% by weight or more. The monomer (m1) may be substantially 100% by weight as a high refractive index monomer. In addition, in several aspects, for example, from the viewpoint of balancing high refractive index and adhesive properties and/or optical properties, the content of the high refractive index monomer in the monomer (m1) can be less than 100% by weight, It is 98% by weight or less, may be 90% by weight or less, may be 80% by weight or less, or may be 65% by weight or less. In several aspects, considering the adhesive properties and/or optical properties, the content of the high refractive index monomer in the monomer (m1) can be 70% by weight or less, 50% by weight or less, or 25% by weight Below, it may be 15% by weight or less, or 10% by weight or less. The technology disclosed here can be implemented even when the content of the high refractive index monomer in the monomer component (m1) is less than 5% by weight. The high refractive index monomer may not be used.

The content of the high refractive index monomer in the monomer component of the acrylic polymer is not particularly limited, and it can be set to achieve the desired refractive index and adhesive properties (such as peel strength, flexibility, etc.) and/or optical properties. (Such as total light transmittance, haze value, etc.) of the adhesive layer. The content of the high refractive index monomer in the above monomer component may be, for example, 3% by weight or more, 10% by weight or more, or 25% by weight or more. In several aspects, from the viewpoint of easy realization of an adhesive with a higher refractive index, the content of the high refractive index monomer in the above-mentioned monomer component can be, for example, greater than 35% by weight, preferably greater than 50% by weight. More than 70% by weight, may be 75% by weight or more, 85% by weight or more, 90% by weight or more, or 95% by weight or more. The content of the high refractive index monomer in the above monomer components can be 100% by weight, but from the viewpoint of balancing high refractive index and adhesive properties and/or optical properties, it is advantageous to set it to less than 100% by weight. It is set to 99% by weight or less, preferably 98% by weight or less, can be 96% by weight or less, can be 93% by weight or less, can be 90% by weight or less, can be 85% by weight or less, can be 80% by weight or less, It may be 75% by weight or less. In several aspects, considering the adhesive properties and/or optical properties, the content of the high refractive index monomer in the above monomer components may be 70% by weight or less, 50% by weight or less, or 25% by weight or less , May be 15% by weight or less, or 5% by weight or less. The technology disclosed here can be implemented even when the content of the high refractive index monomer in the above-mentioned monomer component is less than 3% by weight.

In several ideal aspects of the technology disclosed herein, at least a part of the monomer (m1) is a homopolymer whose Tg is below 10°C (preferably below 5°C or below 0°C, more preferably -10°C) Hereinafter, it is more preferably -20°C or less, for example, -25°C or less) aromatic ring-containing monomer (hereinafter, it is expressed as "monomer L"). When increasing the aromatic ring-containing monomer (m1) in the monomer component (especially the aromatic ring-containing monomer (m1) equivalent to one or both of the above-mentioned monomers containing multiple aromatic rings and high refractive index monomers )), there is a tendency for the storage elastic modulus G'of the adhesive to increase roughly, but by using the monomer L as part or all of the monomer (m1), the storage elastic modulus G'can be suppressed rise. Thereby, the flexibility suitable as an adhesive can be maintained better, and the refractive index can be improved. The lower limit of the Tg of the monomer L is not particularly limited. In consideration of the balance with the refractive index improvement effect, in several aspects, the Tg of the monomer L may be, for example, -70°C or higher, -55°C or higher, or -45°C or higher. Monomer L can be used individually by 1 type or in combination of 2 or more types.

As the monomer L, one having the Tg can be appropriately adopted from the compounds contained in the concept of the aromatic ring-containing monomer (m1) disclosed herein (for example, the compounds and compound groups exemplified above). A suitable example of an aromatic ring-containing monomer that can be used as the monomer L includes m-phenoxybenzyl acrylate (Tg of homopolymer: -35°C). Another suitable example can be phenoxy diethylene glycol acrylate (Tg of homopolymer: -35°C).

The content of the monomer L in the monomer (m1) is not particularly limited. For example, it may be 5% by weight or more, 25% by weight or more, or 40% by weight or more. In several aspects, from the standpoint of easily obtaining a higher-level adhesive that combines high refractive index and flexibility, the content of monomer L in the monomer (m1) can be, for example, 50% by weight or more. It may be 60% by weight or more, 70% by weight or more, 75% by weight or more, 85% by weight or more, 90% by weight or more, or 95% by weight or more. The monomer (A1) may be substantially 100% by weight as the monomer L. In addition, in several aspects, for example, from the viewpoint of balancing flexibility and high refractive index suitable for use as an adhesive, the content of monomer L in the monomer (m1) can be less than 100% by weight, which can be 98 The weight% or less may be 90 weight% or less, 80 weight% or less, 70 weight% or less, 50 weight% or less, 25 weight% or less, or 10 weight% or less. The technique disclosed here can be implemented even when the content of the monomer L in the monomer (m1) is less than 5% by weight. The monomer L may not be used.

The content of the monomer L in the monomer components constituting the acrylic polymer may be, for example, 3% by weight or more, 10% by weight or more, or 25% by weight or more. In several aspects, from the standpoint of easily obtaining an adhesive with a higher level of compatibility between high refractive index and flexibility, the content of monomer L in the monomer component can be, for example, greater than 35% by weight, or greater than 50% by weight. %, can be more than 70% by weight, can be more than 75% by weight, can be more than 85% by weight, can be more than 90% by weight, or more than 95% by weight. The content of the monomer L in the above monomer components can be 100% by weight, but considering the balance of high refractive index and adhesive properties and/or optical properties, it is advantageous to set it to less than 100% by weight, and it is preferably about 99% by weight. % Or less, preferably 98% by weight or less, can be 96% by weight or less, 95% by weight or less, 93% by weight or less, 90% by weight or less, 85% by weight or less, or 80% by weight % Or less, and may be 75% by weight or less. In several aspects, the content of the monomer L in the above-mentioned monomer component may be 70% by weight or less, 50% by weight or less, 25% by weight or less, 15% by weight or less, or 5 Weight% or less. The technique disclosed here can be implemented even when the content of the monomer L in the above-mentioned monomer component is less than 3% by weight.

In several aspects, from the viewpoint of the flexibility of the adhesive, it _{is advantageous for the glass transition temperature Tg m1} of the composition of the monomer (m1) to be approximately 20°C or less, preferably 10°C or less (for example, 5°C). Below), preferably below 0°C, more preferably below -10°C, may be below -20°C, or below -25°C. The lower limit of the glass transition temperature Tg _{m1 is not particularly limited.} In consideration of the balance with the refractive index improvement effect, in several aspects, the glass transition temperature Tg _m1 may be, for example, -70°C or higher, -55°C or higher, or -45°C or higher. The technique disclosed here can be suitably implemented even when the glass transition temperature Tg _m1 is, for example, -40°C or higher, -35°C or higher, -33°C or higher, -30°C or higher, or -25°C or higher.

Here, the glass transition temperature Tg _m1 based on the composition of the monomer (m1) means the Tg obtained by the Fox formula described below based only on the composition of the monomer (m1) in the monomer components constituting the acrylic polymer. The glass transition temperature Tg _m1 can be applied only to the monomer (m1) of the monomer components constituting the acrylic polymer to apply the Fox formula described later, and from the total of the aromatic ring-containing monomers used as the monomer (m1) Calculate the weight fraction of each aromatic ring-containing monomer in the total amount of the glass transition temperature of the polymer and the monomer (m1). In the case where only one monomer is used as the monomer (m1), the Tg of the homopolymer of the monomer is consistent _{with the glass transition temperature Tg m1.}

In several aspects, the aromatic ring-containing monomer (m1) can be combined with the monomer L (that is, the Tg of the homopolymer is below 10℃, and preferably below 5℃ or below 0℃, more preferably -10 ℃ or less, more preferably -20 ℃ or less, for example, -25 ℃ or less aromatic ring-containing monomers) and Tg higher than 10 ℃ monomer H to use. The Tg of monomer H may be higher than 10°C, higher than 15°C, or higher than 20°C, for example. By combining the monomer L and the monomer H to use, for example, in the composition where the content of the aromatic ring-containing monomer (m1) in the monomer component is large, the high refractive index and flexibility of the adhesive can be taken into account at a higher level . The usage amount ratio of the monomer L to the monomer H can be set to appropriately exhibit the effect, and is not particularly limited. For example, it is advisable to set the usage ratio of monomer L to monomer H to satisfy any of the above-mentioned glass transition temperatures Tg _m1 .

In several aspects, the aromatic ring-containing monomer (m1) can be suitably selected from compounds that do not contain a structure in which two or more non-condensed aromatic rings are directly chemically bonded (for example, a biphenyl structure). For example, it is preferably an acrylic polymer composed of monomer components of the following composition: the content of a compound containing two or more non-condensed aromatic rings directly chemically bonded to a structure is less than 5% by weight (preferably less than 3% by weight, It may also be 0% by weight). As mentioned above, the limitation on the amount of the compound containing two or more non-condensed aromatic rings directly chemically bonded is advantageous from the viewpoint of achieving a balance between flexibility or adhesiveness and a high refractive index adhesive.

(Single (m2)) In the several aspects of the technology disclosed herein, the monomer component constituting the acrylic polymer may further contain a monomer (m2) in addition to the above-mentioned monomer (m1). The above-mentioned monomer (m2) is a monomer corresponding to at least one of a monomer having a hydroxyl group (a hydroxyl group-containing monomer) and a monomer having a carboxyl group (a carboxyl group-containing monomer). The compound having at least one hydroxyl group and at least one ethylenically unsaturated group in one molecule of the above-mentioned hydroxyl group-containing single system. The compound containing at least one carboxyl group and at least one ethylenically unsaturated group in one molecule of the above-mentioned carboxyl group-containing single system. The monomer (m2) is useful for introducing crosslinking points into the acrylic polymer, or for imparting appropriate cohesiveness to the adhesive. A monomer (m2) can be used individually by 1 type or in combination of 2 or more types. The monomer (m2) is typically a monomer without an aromatic ring.

Examples of the ethylenically unsaturated group possessed by the monomer (m2) include a (meth)acrylic group, a vinyl group, and a (meth)allyl group. From the viewpoint of polymerization reactivity, it is preferably a (meth)acryloyl group, and from the viewpoint of flexibility or adhesiveness, an acryloyl group is more preferable. From the viewpoint of suppressing the decrease in the flexibility of the adhesive, the monomer (m2) can suitably use a compound (ie, a monofunctional monomer) in which the number of ethylenically unsaturated groups contained in one molecule is one.

Examples of hydroxyl-containing monomers include: 2-hydroxyethyl (meth)acrylate, 2-hydroxypropyl (meth)acrylate, 4-hydroxybutyl (meth)acrylate, 6-hydroxyethyl (meth)acrylate Hexyl ester, 8-hydroxyoctyl (meth)acrylate, 10-hydroxydecyl (meth)acrylate, 12-hydroxylauryl (meth)acrylate, (4-hydroxymethylcyclohexyl) methyl (methyl) ) Hydroxyalkyl (meth)acrylates such as acrylates, but not limited to these. Examples of hydroxyl-containing monomers that can be suitably used include 4-hydroxybutyl acrylate (Tg: -40°C) and 2-hydroxyethyl acrylate (Tg: -15°C). From the viewpoint of improving the flexibility in the room temperature region, 4-hydroxybutyl acrylate having a lower Tg is preferred. In an ideal aspect, more than 50% by weight (for example, more than 50% by weight, more than 70% by weight, or more than 85% by weight) of the monomer (m2) may be 4-hydroxybutyl acrylate. A hydroxyl group-containing monomer can be used individually by 1 type or in combination of 2 or more types.

Among the several aspects in which a hydroxyl-containing monomer is used as the monomer (m2), the above-mentioned hydroxyl-containing monomer may be one or two or more selected from compounds having no methacrylic acid group. Suitable examples of the hydroxyl-containing monomer having no methacrylic acid group include the various hydroxyalkyl acrylates described above. For example, more than 50% by weight, more than 70% by weight, or more than 85% by weight of the hydroxyl-containing monomer used as the monomer (m2) is preferably a hydroxyalkyl acrylate. By using hydroxyalkyl acrylates, hydroxyl groups that help provide crosslinking points or impart moderate agglutinating properties can be introduced into acrylic polymers, and it is easier to obtain than when only the corresponding hydroxyalkyl methacrylates are used. An adhesive with good flexibility or adhesion in the room temperature area.

Examples of carboxyl group-containing monomers include acrylic monomers such as (meth)acrylic acid, carboxyethyl (meth)acrylate, and carboxypentyl (meth)acrylate, as well as itaconic acid, maleic acid, fumaric acid, But crotonic acid and isocrotonic acid are not limited by these. Examples of suitable carboxyl group-containing monomers include acrylic acid and methacrylic acid. A carboxyl group-containing monomer can be used individually by 1 type or in combination of 2 or more types. A hydroxyl group-containing monomer and a carboxyl group-containing monomer can also be used in combination.

The content of the monomer (m2) in the monomer components constituting the acrylic polymer is not particularly limited, and can be set according to the purpose. In several aspects, the content of the aforementioned monomer (m2) can be, for example, 0.01% by weight or more, 0.1% by weight or more, or 0.5% by weight or more. From the viewpoint of obtaining a higher use effect, in several aspects, the content of the above-mentioned monomer (A2) is preferably set to 1% by weight or more, can be set to 2% by weight or more, or can be set to 4% by weight above. The upper limit of the content of the monomer (m2) in the monomer component is set so that the sum of the content of other monomers does not exceed 100% by weight. In several aspects, the content of the above-mentioned monomer (m2) is appropriate, for example, 30% by weight or less or 25% by weight or less, and the relatively high content of the monomer (m1) makes it easy to increase the refractive index. From a standpoint, it is preferably 20% by weight or less, more preferably 15% by weight or less, can be less than 12% by weight, can be less than 10% by weight, or less than 7% by weight.

In the case of using a hydroxyl-containing monomer as the monomer (m2), the content of the hydroxyl-containing monomer in the monomer component is not particularly limited. For example, it can be 0.01% by weight or more (preferably 0.1% by weight or more, more preferably 0.5% by weight or more). In several aspects, the content of the hydroxyl group-containing monomer is preferably set to 1% by weight or more of the monomer component, may be 2% by weight or more, or may be set to 4% by weight or more. The upper limit of the content of the hydroxyl-containing monomer in the monomer component is set so that the sum of the content of the other monomers does not exceed 100% by weight. For example, it is appropriate to set it to 30% by weight or less or 25% by weight. From the viewpoint that the content of the body (m1) is relatively large and easy to increase the refractive index, it is preferably set to 20% by weight or less, more preferably to 15% by weight or less, may be less than 12% by weight, may be less than 10% by weight, or It can be less than 7% by weight.

In the case of using a carboxyl group-containing monomer as the monomer (m2), the content of the carboxyl group-containing monomer in the monomer component is not particularly limited. For example, it can be 0.01% by weight or more (preferably 0.1% by weight or more, more preferably 0.3% by weight or more). In several aspects, the content of the above-mentioned carboxyl group-containing monomer may be 1% by weight or more, 2% by weight or more, or 4% by weight or more. The upper limit of the content of the carboxyl group-containing monomer in the monomer component is set so that the total amount of other monomers used does not exceed 100% by weight. For example, it is appropriate to set it to 30% by weight or less or 25% by weight. From the viewpoint that the content of the monomer (m1) is relatively large and easy to increase the refractive index, it is preferably 20% by weight or less, more preferably 15% by weight or less, may be less than 12% by weight, or less than 10% by weight . In several aspects, from the viewpoint of improving the flexibility of the adhesive, it is advantageous to set the content of the above-mentioned carboxyl group-containing monomer to be less than 7% by weight, preferably less than 5% by weight, and can be set to less than 3% by weight. % May be less than 1% by weight, or less than 0.5% by weight. The technique disclosed herein can be suitably implemented in a state where only a hydroxyl group-containing monomer is used as the monomer (m2), that is, a state where a carboxyl group-containing monomer is not used.

The total content of the monomer (m1) and the monomer (m2) in the monomer components constituting the acrylic polymer may be, for example, 31% by weight or more, preferably 51% by weight or more, may be 61% by weight or more, or It is 71% by weight or more. In several aspects, the total content of the monomer (m1) and the monomer (m2) in the monomer components constituting the acrylic polymer can be, for example, 76% by weight or more, preferably 81% by weight or more, 86% by weight or more, 91% by weight or more, 96% by weight or more, 99% by weight or more, or substantially 100% by weight.

(Single m3) The monomer components constituting the acrylic polymer may optionally include the above-mentioned monomer (m1) and monomers other than the above-mentioned monomer (m2). As an example of the said arbitrary component, the alkyl (meth)acrylate (hereinafter also referred to as "monomer (m3)") is mentioned. The monomer (m3) helps to adjust the softness of the adhesive or improve the compatibility in the adhesive.

The monomer (m3) can be suitably used for _{alkyl (meth)acrylates having a C 1-20} (ie C 1-20) linear or branched alkyl group at the end of the ester. _{Specific examples of C 1-20} alkyl (meth)acrylate include: methyl (meth)acrylate, ethyl (meth)acrylate, propyl (meth)acrylate, and isopropyl (meth)acrylate , N-butyl (meth)acrylate, isobutyl (meth)acrylate, secondary butyl (meth)acrylate, tertiary butyl (meth)acrylate, amyl (meth)acrylate, (meth) ) Isoamyl acrylate, hexyl (meth)acrylate, heptyl (meth)acrylate, octyl (meth)acrylate, 2-ethylhexyl (meth)acrylate, isooctyl (meth)acrylate , Nonyl (meth)acrylate, isononyl (meth)acrylate, decyl (meth)acrylate, isodecyl (meth)acrylate, undecyl (meth)acrylate, ten (meth)acrylate Diester, tridecyl (meth)acrylate, tetradecyl (meth)acrylate, pentadecyl (meth)acrylate, hexadecyl (meth)acrylate, heptadecyl (meth)acrylate, (meth)acrylate Octadecyl acrylate, isooctadecyl (meth)acrylate, nonadecyl (meth)acrylate, eicosanyl (meth)acrylate, etc., but are not limited thereto.

In several aspects, at least a part of the monomer (m3) can suitably be a homopolymer with a Tg of -20°C or less (preferably -40°C or less, for example, -50°C or less) (meth)acrylic acid alkane Base ester. The low Tg alkyl (meth)acrylate helps to improve the flexibility of the adhesive. The lower limit of the Tg of the above-mentioned alkyl (meth)acrylate is not particularly limited. For example, it may be -85°C or higher, -75°C or higher, -65°C or higher, or -60°C or higher. Specific examples of the aforementioned low Tg (meth)acrylic acid alkyl esters include n-butyl acrylate (BA), 2-ethylhexyl acrylate (2EHA), isononyl acrylate (iNA), and the like.

Among the several aspects in which the monomer (m3) is used, it is preferable that at least a part of the above-mentioned monomer (m3) is an alkyl acrylate from the viewpoint of flexibility or adhesiveness. For example, it is preferable that 50% by weight or more (more preferably 75% by weight or more, more preferably 90% by weight or more) of the monomer (m3) is alkyl acrylate. It is also possible to use only one type or two or more types of alkyl acrylates and not use alkyl methacrylates as the monomer (m3).

In the case where the monomer component contains the alkyl (meth)acrylate, the content of the alkyl (meth)acrylate in the monomer component can be set to appropriately exert its use effect. In several aspects, the content of the alkyl (meth)acrylate may be, for example, 1% by weight or more, 3% by weight or more, 5% by weight or more, or 8% by weight or more. In several aspects, the content of the alkyl (meth)acrylate may be 15% by weight or more, 30% by weight or more, or 45% by weight or more. The upper limit of the content of the monomer (m3) in the monomer component is set so that the sum of the content of other monomers does not exceed 100% by weight, and may be less than 50% by weight, for example. In several aspects, the content of the aforementioned monomer (m3) may be less than 35% by weight, for example. Generally speaking, the refractive index of alkyl (meth)acrylate is low. Therefore, in order to increase the refractive index, the content of monomer (m3) in the monomer component is limited, and the content of monomer (m1) is relatively large. Is advantageous. From the said point of view, it is advantageous that the content of monomer (m3) is 24% by weight or less of the monomer components, preferably less than 23% by weight, more preferably less than 20% by weight, can be less than 17% by weight, and can be less than 12% by weight %, can be less than 7% by weight, can be less than 3% by weight, or less than 1% by weight. The monomer (m3) may not be used substantially.

(Other monomers) The monomer components constituting the acrylic polymer may optionally include monomers other than the above-mentioned monomers (m1), (m2), and (m3) (hereinafter referred to as "other monomers"). The above-mentioned other monomers can be used, for example, to adjust the Tg of the acrylic polymer, adjust the adhesive performance, and improve the compatibility in the adhesive layer. The above-mentioned other monomers can be used individually by 1 type or in combination of 2 or more types.

Examples of the above-mentioned other monomers include monomers having functional groups other than a hydroxyl group and a carboxyl group (functional group-containing monomers). For example, other monomers that can improve the cohesive force or heat resistance of the adhesive include sulfonic acid group-containing monomers, phosphoric acid group-containing monomers, and cyano group-containing monomers. In addition, as a monomer that can introduce functional groups that can become cross-linking points into the acrylic polymer, or can help increase the peel strength or improve the compatibility in the adhesive layer, examples include monomers containing amide groups. Body (for example (meth)acrylamide, N-methylol (meth)acrylamide, etc.), amine group-containing monomers (for example, aminoethyl (meth)acrylate, N,N-dimethyl Aminoethyl (meth)acrylate, etc.), monomers with a ring containing nitrogen atoms (such as N-vinyl-2-pyrrolidone, N-(meth)acryloyl mopholin, etc.), containing Imine group monomers, epoxy group-containing monomers, ketone group-containing monomers, isocyanate group-containing monomers, alkoxysilyl group-containing monomers, etc. In addition, among the monomers having a ring containing nitrogen atoms, for example, N-vinyl-2-pyrrolidone is also equivalent to an amine group-containing monomer. The relationship between the above-mentioned monomer having a nitrogen atom-containing ring and an amine group-containing monomer is also the same.

Other monomers that can be used in addition to the functional group-containing monomers include: vinyl acetate-based monomers such as vinyl acetate; non-aromatic ring-containing monomers such as cyclohexyl (meth)acrylate and isobornyl (meth)acrylate (Meth)acrylates; olefin monomers such as ethylene, butadiene, isobutylene, etc.; chlorine-containing monomers such as vinyl chloride; methoxyethyl (meth)acrylate, ethoxyethyl (meth)acrylic acid Alkoxy group-containing monomers such as esters and ethoxyethoxyethyl (meth)acrylate; vinyl ether-based monomers such as methyl vinyl ether, etc. A suitable example of other monomers used for the purpose of improving the flexibility of the adhesive can be ethoxy ethoxy ethyl acrylate (alias: ethyl carbitol acrylate, Tg of homopolymer: -67 ℃).

When the above-mentioned other monomers are used, the amount used is not particularly limited, and can be appropriately set within a range where the total amount of monomer components does not exceed 100% by weight. In several aspects, from the viewpoint of easily exhibiting the refractive index improvement effect obtained by using the monomer (m1), the content of the above-mentioned other monomers in the monomer component can be set to, for example, about 35% by weight or less, which is about 25% by weight or less (for example, 0 to 25% by weight) is appropriate, may be about 20% by weight or less (for example, 0-20% by weight), may be about 10% by weight or less, may be about 5% by weight or less, or may be, for example, about 1 Weight% or less. The technology disclosed herein can be suitably implemented in a state where the monomer component does not substantially contain the above-mentioned other monomers.

In several aspects, the monomer component constituting the acrylic polymer may be a composition in which the usage amount of the methacrylic acid group-containing monomer is suppressed below a predetermined level. The usage amount of the methacryl group-containing monomer in the monomer component can be, for example, less than 5% by weight, less than 3% by weight, less than 1% by weight, or less than 0.5% by weight. As mentioned above, the limitation on the amount of methacrylic acid group-containing monomer is advantageous from the viewpoint of achieving a balance between flexibility or adhesion and a high refractive index adhesive. The monomer component constituting the acrylic polymer may also be a composition that does not contain a methacryl group-containing monomer (for example, a composition composed only of an acryl group-containing monomer).

In several aspects, the monomer component of the base polymer (for example, acrylic polymer) constituting the high refractive index adhesive layer contains The amount of carboxyl monomer used should be limited. The usage amount of the carboxyl group-containing monomer in the monomer component can be, for example, less than 1% by weight, preferably less than 0.5% by weight, more preferably less than 0.3% by weight, can be less than 0.1% by weight, or less than 0.05% by weight. As the usage amount of the carboxyl group-containing monomer is limited, the corrosion of metal materials (such as metal wiring or metal film that may be present on the adherend) that can contact or be arranged adjacent to the high refractive index adhesive layer is suppressed The point of view is also favorable. The technique disclosed here can be suitably implemented in the state where the above-mentioned monomer components do not contain a carboxyl group-containing monomer. For the same reason, in several aspects, the monomer components of the base polymer constituting the high refractive index adhesive layer are among the monomers having acidic functional groups (in addition to carboxyl groups, sulfonic acid groups, phosphoric acid groups, etc.) The amount of use should be restricted. The usage amount of the acidic functional group-containing monomer in the monomer component of the above aspect can be applied to the ideal usage amount of the above-mentioned carboxyl group-containing monomer. The technology disclosed here can be suitably implemented in a state where the above-mentioned monomer components do not contain an acidic group-containing monomer (that is, a state where the base polymer of the high refractive index adhesive layer is acid-free).

(Glass transition temperature Tg _{T of the} base polymer) In several aspects, in the base polymer (such as acrylic polymer) of the adhesive layer, the glass transition temperature Tg is based on the composition of the monomer components constituting the polymer _{It is appropriate for T to} be below about 20°C, preferably below 10°C, more preferably below 0°C, may be below -10°C, may be below -20°C, may be below -25°C, and may be below -28°C It can also be below -30°C. From the viewpoint of improving the flexibility of the adhesive, a _{low glass transition temperature Tg T} is advantageous. In addition, the glass transition temperature Tg _T may be, for example, -60°C or higher, and from the viewpoint of facilitating the high refractive index of the adhesive, it is preferably -50°C or higher, more preferably higher than -45°C, and may be higher than- 40°C, can be higher than -35°C, can be higher than -25°C, can be higher than -15°C, or can be higher than -5°C.

Here, the glass transition temperature Tg _T of the polymer means the glass transition temperature obtained by the Fox formula based on the composition of the monomer components constituting the polymer, unless otherwise specified. The Fox formula is shown below, which is the relational formula between the Tg of the copolymer and the glass transition temperature Tgi of the homopolymer after the monomers constituting the copolymer are each homopolymerized. 1/Tg=Σ(Wi/Tgi) In the above Fox formula, Tg represents the glass transition temperature of the copolymer (unit: K), and Wi represents the weight fraction of monomer i in the copolymer (copolymerization ratio on a weight basis) ), Tgi represents the glass transition temperature of the homopolymer of monomer i (unit: K). Regarding the glass transition temperature of the homopolymer used in the calculation of Tg, the value described in known materials such as "Polymer Handbook" (3rd edition, John Wiley & Sons, Inc., 1989) is used. Regarding the monomer with multiple values described in the above-mentioned Polymer Handbook, the highest value is used. When the Tg of the homopolymer is not described in the known materials, the value obtained by the measurement method described in Japanese Patent Application Publication No. 2007-51271 is used.

(Preparation method of base polymer) In the technique disclosed herein, the method of obtaining the base polymer of the high refractive index adhesive layer (for example, the acrylic polymer (A) composed of the above-mentioned monomer components) is not particularly limited. For example, the above description regarding the preparation method of the acrylic polymer (F) can also be applied to the preparation method of the base polymer of the high refractive index adhesive layer.

(Refractive index enhancer) In several aspects of the technology disclosed herein, in addition to the base polymer, the high refractive index adhesive layer (for example, the acrylic adhesive layer) may also contain a refractive index enhancer if necessary. Here, the refractive index enhancer in this specification means a material that can increase the refractive index of the adhesive layer by using it. The refractive index enhancer can suitably use a material with a refractive index higher than that of the adhesive layer containing the refractive index enhancer. In addition, the refractive index enhancer can suitably use a material with a higher refractive index than the base polymer (for example, acrylic polymer (A)) of the adhesive layer containing the refractive index enhancer. By appropriately using the refractive index enhancer, it can be suitable to take into account a higher refractive index and practical adhesive performance. In several aspects, the refractive index enhancer is preferably an organic material. The organic material that can be used as a refractive index enhancer can be a polymer or a non-polymer. Moreover, it may have a polymerizable functional group, and may not have a polymerizable functional group. A refractive index improver can be used individually by 1 type or in combination of 2 or more types.

The refractive index of the refractive index enhancer (for example, the additive ((H _RO ) described later)) can be set to an appropriate range under the relative relationship with the refractive index of the base polymer, so it is not limited by the specific range. The refractive index enhancer The refractive index is, for example, greater than 1.55, greater than 1.56, or greater than 1.57, and can be selected from a range higher than the refractive index of the base polymer. From the viewpoint of the higher refractive index of the adhesive, in several aspects, the refractive index It is advantageous for the refractive index of the rate enhancer to be 1.58 or higher, and preferably 1.60 or higher, more preferably 1.63 or higher, may be 1.65 or higher, may be 1.70 or higher, or may be 1.75 or higher. By virtue of the higher refractive index of the refractive index The lifter can achieve the target refractive index even by using a smaller amount of the refractive index lifter. This is ideal from the viewpoint of suppressing the decrease in adhesion properties or optical properties. The upper limit of the refractive index of the refractive index lifter is not particularly limited. However, from the viewpoint of compatibility in the adhesive, high refractive index and ease of compatibility with flexibility suitable as an adhesive, for example, it is 3.000 or less, 2.500 or less, 2.000 or less, or 1.950 or less, can be 1.900 or less, or 1.850 or less.

In several aspects, the refractive index improvers (e.g., later-described additives (H _RO)) of the refractive index n _B of the polymer substrate and the refractive index n of _a difference, i.e. n _b -n _a (hereinafter known as "Δn _A ") is set to be greater than 0. In several aspects, Δn _{A is,} for example, 0.02 or greater, may be 0.05 or greater, may be 0.07 or greater, may be 0.10 or greater, may be 0.15 or greater, or may be 0.20 or greater or 0.25 or greater. By selecting the base polymer and the refractive index enhancer in such a way that Δn _{A is} changed large, the effect of using the refractive index enhancer to increase the refractive index tends to be higher. In addition, from the viewpoint of compatibility in the adhesive layer or transparency of the adhesive layer, in several aspects, Δn _A may be 0.70 or less, 0.60 or less, 0.50 or less, or It is 0.40 or less or 0.35 or less.

In several aspects, the difference between the refractive index n _b of the refractive index enhancer (such as the additive (H _{RO ) described later) and the refractive index n T} of the adhesive layer containing the refractive index enhancer, that is, n _b -n _T (hereinafter also referred to as "Δn _B ") is set to be greater than 0. In several aspects, Δn _{B is,} for example, 0.02 or greater, may be 0.05 or greater, may be 0.07 or greater, may be 0.10 or greater, may be 0.15 or greater, or may be 0.20 or greater or 0.25 or greater. By selecting the composition of the adhesive layer and the refractive index enhancer in such a way that Δn _{B is} changed large, the effect of using the refractive index enhancer to increase the refractive index tends to be higher. In addition, from the viewpoints of compatibility in the adhesive layer or transparency of the adhesive layer, in several aspects, Δn _B can be, for example, 0.70 or less, 0.60 or less, 0.50 or less, or It is 0.40 or less or 0.35 or less.

The usage amount of the refractive index enhancer relative to 100 parts by weight of the base polymer (the total amount of the refractive index enhancer when a plurality of types of refractive index enhancers are used) is not particularly limited, and can be set according to the purpose. From the viewpoint of increasing the refractive index of the adhesive, the amount of the refractive index enhancer relative to 100 parts by weight of the base polymer can be set to, for example, 1 part by weight or more, and it is advantageous to set it as 3 parts by weight or more. 5 parts by weight or more, may be 7 parts by weight or more, may be 10 parts by weight or more, may be 15 parts by weight or more, or may be 20 parts by weight or more. In addition, in several aspects, the usage amount of the refractive index enhancer relative to 100 parts by weight of the base polymer can be set to be 80 parts by weight or less, and the high refractive index of the adhesive is balanced with the suppression of adhesion characteristics or optical properties. From the viewpoint of property degradation, it is advantageous to set it to 60 parts by weight or less, and it is preferable to set it to 45 parts by weight or less. In several aspects where more emphasis is placed on adhesion properties or optical properties, the use amount of the refractive index enhancer relative to 100 parts by weight of the base polymer can be, for example, 30 parts by weight or less, 20 parts by weight or less, or 15 parts by weight. Below, it may be 10 parts by weight or less, 5 parts by weight or less, or 3 parts by weight or less. The technology disclosed here can be suitably implemented even when the usage amount of the refractive index enhancer relative to 100 parts by weight of the base polymer in the adhesive layer is less than 1 part by weight, or the refractive index enhancer is not used substantially. Here, substantially non-use means at least unintentional use.

(Additives (H _RO )) In several aspects, the refractive index enhancer can suitably be an organic material with a higher refractive index than the base polymer. Hereinafter, there are cases where the organic material is listed as "additive (H _RO )". Here, the above-mentioned "H _RO "means an organic material with a high refractive index (High Refractive index). By combining the base polymer (for example, acrylic polymer, preferably acrylic polymer (A)) and additive (H _RO ), it is possible to achieve a better balance between refractive index and adhesive properties (peel strength, flexibility, etc.) ) And/or optical properties (total light transmittance, haze value, etc.) adhesives. The organic materials that can be used as additives (H _RO ) can be polymers or non-polymers. Moreover, it may have a polymerizable functional group, and may not have a polymerizable functional group. The additive (H _RO ) can be used alone or in combination of two or more.

The refractive index of the additive (H _RO ) is the same as the refractive index of the monomer, and it is measured using an Abbe refractometer under the conditions of a measurement wavelength of 589 nm and a measurement temperature of 25°C. When the manufacturer provides a nominal value of the refractive index at 25°C, the nominal value can be used.

The molecular weight of the organic material used as the additive (H _RO ) is not particularly limited, and can be selected according to the purpose. The molecular weight of the additive (H _RO ) can be selected from the range of 30,000 or less, for example. In addition, the additive (H _RO ) is preferably a polymer or non-polymer with a lower molecular weight than the base polymer. From the viewpoint of balancing the effect of high refractive index and other properties (for example, optical properties such as softness and haze suitable for adhesives), in several aspects, the molecular weight of the _{additive (H RO) is approximately less than} 10,000 is appropriate, preferably less than 5,000, more preferably less than 3,000 (for example, less than 1,000), can be less than 800, can be less than 600, can be less than 500, or less than 400. The fact that _{the molecular weight of the additive (H RO} ) is not too large is advantageous from the viewpoint of enhancing the compatibility in the adhesive layer. In addition, _{the molecular weight of the additive (H RO} ) may be 130 or more, or 150 or more, for example. In several aspects, from the viewpoint of high refractive index of the additive (H _RO) of view, the additive (H _RO) of the appropriate molecular weight of 170 or more, 200 or more is more appropriate, can be 230 or more, 250 The above may be 270 or more, 500 or more, 1000 or more, or 2000 or more. In several aspects, a polymer with a molecular weight of about 1,000 to 10,000 (for example, more than 1,000 and less than 5,000) can be used as an additive (H _RO ). The molecular weight of the additive (H _RO ) can be calculated based on the chemical structure of a polymer with a non-polymer or low polymerization degree (for example, about 2 to 5 polymers). When the additive (H _RO ) is a polymer with a higher degree of polymerization, the weight average molecular weight (Mw) according to GPC performed under appropriate conditions can be used. When a nominal value of molecular weight is provided from the manufacturer, etc., the nominal value can be used.

Examples of organic materials that can be an _{option for additives (H RO} ) include organic compounds with aromatic rings, organic compounds with heterocycles (may be aromatic or non-aromatic heterocycles), etc., but are not affected by the And other qualifications.

The aromatic ring of the above-mentioned organic compound with aromatic ring (hereinafter also referred to as "aromatic ring-containing compound") that can be used as an additive (H _{RO) can be free from the aromatic ring of the compound that can be used as a monomer (m1)} Choose from the same thing as the ring.

The above-mentioned aromatic ring may have 1 or 2 or more substituents on the ring constituent atoms, or may not have a substituent. When it has a substituent, the substituent can be exemplified by an alkyl group, an alkoxy group, an aryloxy group, a hydroxyl group, a halogen atom (a fluorine atom, a chlorine atom, a bromine atom, etc.), a hydroxyalkyl group, a hydroxyalkoxy group, and a glycidoxy group. Base, etc., but not subject to such restrictions. Among the substituents containing carbon atoms, the number of carbon atoms contained in the substituent is, for example, 1-10, and 1-6 is advantageous, preferably 1-4, more preferably 1-3, and may be 1 or 2, for example. In several aspects, the above-mentioned aromatic ring may be an aromatic ring having no substituents on the constituent atoms of the ring, or may have a constituent selected from the group consisting of an alkyl group, an alkoxy group, and a halogen atom (such as bromine). Atom) constitutes an aromatic ring of 1 or more substituents in the group.

Examples of aromatic ring-containing compounds that can be used as additives (H _RO ) include: compounds that can be used as monomers (m1); oligomers containing compounds that can be used as monomers (m1) as monomer units ; Remove the ethylenically unsaturated group from the compound that can be used as the monomer (m1) (may be a substituent bonded to the ring constituent atoms) or the part of the group that constitutes the ethylenically unsaturated group and Substituted into a structure of a hydrogen atom or a group that does not have an ethylenically unsaturated group (such as a hydroxyl group, an amino group, a halogen atom, an alkyl group, an alkoxy group, a hydroxyalkyl group, a hydroxyalkoxy group, a glycidoxy group, etc.) Compounds, etc., but are not subject to such restrictions. Non-limiting specific examples of aromatic ring-containing compounds that can be used as additives (H _RO ) may include: benzyl acrylate, m-phenoxybenzyl acrylate, 2-(o-phenylphenoxy)ethyl acrylate, Phenoxy ethyl acrylate, phenoxy diethylene glycol acrylate, phenoxy polyethylene glycol acrylate, 2-hydroxy-3-phenoxy propyl acrylate, the above-mentioned monomers with a chrysanthemum structure, have two Monomers with naphthothiophene structure, monomers with dibenzothiophene structure, and other aromatic ring-containing monomers; 3-phenoxybenzyl alcohol, dinaphthothiophene and their derivatives (for example, the bond on the dinaphthothiophene ring Compounds with one or more substituents selected from the group consisting of hydroxyl, methanol, diethanol and glycidyl groups) and other aromatic ring-containing compounds that do not have ethylenically unsaturated groups Wait. In addition, the aromatic ring-containing compound may be an oligomer containing the aromatic ring-containing monomer as a monomer unit (preferably an oligomer with a molecular weight of about 5000 or less, more preferably about 1000 or less; for example, 2 to 5 polymers) Low polymer around). The above-mentioned oligomers may be, for example, homopolymers containing aromatic ring monomers; copolymers of one or more aromatic ring-containing monomers; copolymerization of one or more aromatic ring-containing monomers with other monomers Things etc. One type or two or more types of monomers that do not have an aromatic ring can be used for the above-mentioned other monomers.

Among several aspects, in view of the ease of obtaining a higher refractive index effect, organic compounds with more than two aromatic rings per molecule (hereinafter also referred to as "compounds containing multiple aromatic rings") can be suitably used. As an additive (H _RO ). The compound containing a plurality of aromatic rings may or may not have polymerizable functional groups such as ethylenically unsaturated groups. In addition, the compound containing a plurality of aromatic rings may be a polymer or a non-polymer. In addition, the above-mentioned polymer may be an oligomer containing a plurality of aromatic ring-containing monomers as monomer units (preferably an oligomer with a molecular weight of about 5000 or less, more preferably about 1000 or less; for example, 2 to 5 polymers). Low polymer around). The above-mentioned oligomers may be, for example, homopolymers of monomers containing multiple aromatic rings; copolymers of one or more monomers containing multiple aromatic rings; one or more monomers containing multiple aromatic rings The monomer and other monomer copolymers, etc. The above-mentioned other monomers may be aromatic ring-containing monomers that are not monomers containing multiple aromatic rings, may be monomers without aromatic rings, or a combination of these.

Non-limiting examples of compounds containing multiple aromatic rings include: compounds with a structure in which two or more non-condensed aromatic rings are bonded via a linking group, and two or more non-condensed aromatic rings directly (that is, without other atoms) ) Compounds with a chemically bonded structure, compounds with a condensed aromatic ring structure, compounds with a sulphur structure, compounds with a dinaphthothiophene structure, compounds with a dibenzothiophene structure, etc. The compound containing a plurality of aromatic rings can be used singly or in combination of two or more kinds.

In addition to the above-mentioned monomers having the fluorescein structure, or the oligomers of the homopolymers or copolymers of the above-mentioned monomers, specific examples of the compounds having the fluorescein structure may also include 9,9-bis(4-hydroxybenzene) Group) 茀 (refractive index: 1.68), 9,9-bis(4-aminophenyl) 茀 (refractive index: 1.73), 9,9-bis(4-hydroxy-3-methylphenyl) 茀 ( Refractive index: 1.68), 9,9-bis[4-(2-hydroxyethoxy)phenyl] pyrene (refractive index: 1.65) and 9,9-bisphenyl pyrene and its derivatives.

Specific examples of the compound having a dinaphthothiophene structure, in addition to the monomers having a dinaphthothiophene structure, or the oligomers of homopolymers or copolymers of the monomers, can also include: Thiophene (refractive index: 1.808); hydroxyalkyl dinaphthothiophene such as 6-hydroxymethyl dinaphthothiophene (refractive index: 1.766); 2,12-dihydroxy dinaphthothiophene (refractive index: 1.750), etc. Dihydroxy dinaphthothiophene; 2,12-dihydroxyethyloxy dinaphthothiophene (refractive index: 1.677) and other dihydroxyalkyloxy dinaphthothiophene; 2,12-diepoxypropyl Diglycidyloxy dinaphthothiophene (refractive index: 1.723), etc.; 2,12-diallyloxy dinaphthothiophene (abbreviation: 2,12-DAODNT, refractive index 1.729) Dinaphthothiophene and its derivatives such as dinaphthothiophene having two or more ethylenically unsaturated groups.

Specific examples of the above-mentioned compound having a dibenzothiophene structure, in addition to the above-mentioned monomer having a dibenzothiophene structure, or an oligomer of a homopolymer or copolymer of the monomer, can also include dibenzothiophene (Refractive index: 1.607), 4-dimethyldibenzothiophene (refractive index: 1.617), 4,6-dimethyldibenzothiophene (refractive index: 1.617), etc.

Examples of organic compounds having a heterocyclic ring (hereinafter also referred to as heterocyclic-containing organic compounds) that can be an option of the additive (H _{RO) include thioepoxy compounds, compounds having tricyclic rings, and the like.} Examples of the thioepoxy compound include bis(2,3-epithiopropyl) disulfide and its polymer (refractive index: 1.74) described in Japanese Patent No. 3712653. Examples of compounds with tricyclic rings include compounds having at least one (for example, 3-40, preferably 5-20)) tricyclic rings in one molecule. In addition, tricyclic rings are aromatic, so compounds with tricyclic rings are also included in the above-mentioned concept of aromatic ring-containing compounds, and compounds with plural tricyclic rings are also included in the above-mentioned compounds containing plural aromatic rings In the concept.

In several aspects, compounds without ethylenic unsaturated groups can be suitably used as additives (H _RO ). Thereby, deterioration of the adhesive composition due to heat or light (decrease in leveling due to progress of gelation or increase in viscosity) can be suppressed, and storage stability can be improved. _{The use of an additive (H RO} ) that does not have an ethylenically unsaturated group prevents ethylenic unsaturation in an adhesive layer containing the additive (H _RO ) or a laminate (such as a laminate sheet) containing the adhesive layer. It is also preferable from the viewpoints of dimensional change or deformation (warpage, undulation, etc.) caused by radical reaction, generation of optical strain, etc.

In the aspect of using an oligomer as an additive (H _RO ), the oligomer can be obtained by polymerizing the corresponding monomer component by a known method. When the oligomer is produced by radical polymerization, a polymerization initiator, a chain transfer agent, an emulsifier, etc., which can be used for radical polymerization, can be appropriately added to the monomer component to perform polymerization. The above-mentioned polymerization initiators, chain transfer agents, emulsifiers, etc. that can be used for radical polymerization are not particularly limited, and can be appropriately selected and used. In addition, the weight average molecular weight of the oligomer can be controlled by the usage amount of the polymerization initiator and the chain transfer agent, and the reaction conditions, and the usage amount can be appropriately adjusted according to the type of the oligomer. The chain transfer agent may include, for example, lauryl mercaptan, glycidyl mercaptan, thioacetic acid, 2-mercaptoethanol, α-thioglycerol, thioglycolic acid, 2-ethylhexyl thioglycolic acid, 2, 3-Dimercapto-1-propanol and the like. A chain transfer agent may be used individually by 1 type, and 2 or more types may be mixed and used for it. The amount of the chain transfer agent used can be set to obtain the oligomer with the desired weight average molecular weight in accordance with the composition of the monomer components that can be used in the synthesis of the oligomer or the type of the chain transfer agent. In several aspects, it is appropriate for the chain transfer agent to be used in an amount of about 15 parts by weight or less with respect to 100 parts by weight of the total amount of monomers that can be used in the synthesis of oligomers, and may be 10 parts by weight or less, or It may be about 5 parts by weight or less. The lower limit of the use amount of the chain transfer agent relative to 100 parts by weight of the total amount of monomers that can be used in the synthesis of oligomers is not particularly limited. For example, it may be 0.01 parts by weight or more, 0.1 parts by weight or more, or 0.5 parts by weight. The above may be 1 part by weight or more.

In the aspect of using the additive (H _RO ) as the refractive index enhancer, _{the usage amount of the additive (H RO} ) relative to 100 parts by weight of the base polymer (the total amount of the same when using multiple compounds) is not particularly limited. It can be set according to purpose. From the viewpoint of increasing the refractive index of the adhesive, the amount of the additive (H _RO ) relative to 100 parts by weight of the base polymer can be set to, for example, 1 part by weight or more, and it is advantageous to set it to 3 parts by weight or more. It is 5 parts by weight or more, may be 7 parts by weight or more, may be 10 parts by weight or more, may be 15 parts by weight or more, or may be 20 parts by weight or more. In several aspects, the usage amount of the additive (H _RO ) relative to 100 parts by weight of the base polymer can be set to be less than 80 parts by weight, for example, to balance the high refractive index of the adhesive and suppress the adhesion or optical properties. From the viewpoint of reduction, it is advantageous to set it to 60 parts by weight or less, and it is preferable to set it to 45 parts by weight or less. In several aspects where more emphasis is placed on adhesion properties or optical properties, the amount of the additive (H _RO ) relative to 100 parts by weight of the base polymer can be, for example, 30 parts by weight or less, 20 parts by weight or less, or 15 parts by weight. Below, it may be 10 parts by weight or less.

(Plasticized material) In several aspects, the high refractive index adhesive layer may include a plasticized material with a lower molecular weight than the base polymer of the adhesive layer. By using plasticized materials, the flexibility of the high refractive index adhesive layer can be improved, thereby improving the adhesion to the adherend, or the flexibility as a whole, and the followability to deformation. From the viewpoint of compatibility or transparency in the adhesive layer, an organic material can be suitably used for the plasticizing material. The plasticized material can also be a material that can be used as the above-mentioned refractive index enhancer (for example, the above-mentioned additive (H _RO )).

The molecular weight of the plasticized material is lower than that of the base polymer, and it is not particularly limited. In several aspects, from the standpoint of easily exhibiting the plasticizing effect, the molecular weight of the plasticized material can be less than 30,000, can be less than 25,000, can be less than 10,000, preferably less than 5,000, more preferably less than 3,000 (for example, less than 1,000) , Can be less than 800, can be less than 600, can be less than 500, can also be less than 400. The fact that the molecular weight of the plasticized material is not too large is advantageous from the viewpoint of improving the compatibility in the adhesive layer. In addition, in several aspects, from the viewpoint of easily exerting a sufficient plasticizing effect, the molecular weight of the plasticized material is appropriately 130 or more, and preferably 150 or more, more preferably 170 or more, and may be 200 or more , Can be 250 or more, or 300 or more. In several aspects, the molecular weight of the plasticized material can be 500 or more, 1000 or more, or 2000 or more. The fact that the molecular weight of the plasticized material is not too low is also preferable from the viewpoint of the heat resistance of the adhesive layer or the prevention of contamination by the adherend.

Non-limiting examples of compounds that can be an option for plasticizing materials include: compounds that can be used as monomers (m1) (for example, aromatic ring (meth)acrylates such as benzyl, phenoxy, naphthyl, etc.), Structure monomers, monomers with dinaphthothiophene structure, monomers with dibenzothiophene structure, etc.); oligomers containing compounds that can be used as monomers (m1) as monomer units; from The compound used in the monomer (m1) is a compound (for example, 3-phenoxybenzyl alcohol) having a structure in which a part having an ethylenically unsaturated group is removed and substituted with a hydrogen atom or a group without an ethylenically unsaturated group. From the viewpoint of improving flexibility, low Tg monomers such as n-butyl acrylate or 2-ethylhexyl acrylate can also be used in oligomers containing compounds that can be used as monomers (m1) as monomer units. Copolymerization. As the plasticizing material, well-known plasticizers (such as phthalate, terephthalate, adipate, adipic acid polyester, ethylene benzoate, etc.) can also be used. Etc.) 1 or more.

In several aspects, the plasticized material can suitably be an organic material with a refractive index above about 1.50 (preferably above 1.53). Specific examples of compounds that can be an option for plasticizing materials include: diethylene glycol dibenzoate (refractive index 1.55), dipropylene glycol dibenzoate (refractive index 1.54), 3-phenoxytoluene ( Refractive index 1.57), 3-ethylbiphenyl (refractive index 1.59), 3-methoxybiphenyl (refractive index 1.61), 4-methoxybiphenyl (refractive index 1.57), polyethylene glycol diphenylmethyl Ester, 3-phenoxybenzyl alcohol (refractive index 1.59), triphenyl phosphate (refractive index 1.56), benzyl benzoate (refractive index 1.57), 4-(tertiary butyl) phenyl diphenyl Phosphate (refractive index 1.56), trimethylphenyl phosphate (refractive index 1.55), butyl benzyl phthalate (refractive index 1.54), rosin methyl ester (refractive index 1.53), alkyl benzyl phthalate Ester (refractive index 1.53), butyl (phenylsulfonyl) amine (refractive index 1.53), trimethyl trimellitate (refractive index 1.52), benzyl phthalate (refractive index 1.52), 2- Ethylhexyl diphenyl phosphate (refractive index 1.51), ginseng phosphite (2,4-di-tertiary butyl phenyl) ester, etc., but not limited thereto. From the viewpoint of refractive index and compatibility, for example, diethylene glycol dibenzoate can be suitably used. The upper limit of the refractive index of the plasticized material is not particularly limited, and may be 3.00 or less, for example. In several aspects, from the viewpoint of the ease of preparation of the adhesive composition or the compatibility in the adhesive, etc., it is appropriate that the refractive index of the plasticized material is 2.50 or less, and it is advantageous to be 2.00 or less. It is 1.90 or less, may be 1.80 or less, or may be 1.70 or less. In addition, the refractive index of the plasticized material is the same as the refractive index of the monomer, and it is measured using an Abbe refractometer under the conditions of a measurement wavelength of 589 nm and a measurement temperature of 25°C. When the manufacturer provides a nominal value of the refractive index at 25°C, the nominal value can be used.

In the aspect of using the plasticized material, the usage amount of the plasticized material relative to 100 parts by weight of the base polymer is not particularly limited, and can be set according to the purpose. From the point of view of improving the plasticizing effect, the amount of plasticizing material used relative to 100 parts by weight of the base polymer can be, for example, 0.1 parts by weight or more, or 0.5 parts by weight or more, and a higher plasticizing effect can be obtained. From a viewpoint, it is preferably 1 part by weight or more, preferably 3 parts by weight or more, and may be 5 parts by weight or more, 7 parts by weight or more, 10 parts by weight or more, 15 parts by weight or more, or It can be 20 parts by weight or more. In addition, from the viewpoint of balancing the high refractive index of the adhesive with transparency and plasticizing effect, it is appropriate that the usage amount of the plasticizing material relative to 100 parts by weight of the base polymer is about 100 parts by weight or less. It is 80 parts by weight or less, preferably 60 parts by weight or less, and may be 45 parts by weight or less, 35 parts by weight or less, or 25 parts by weight or less. In several aspects where more emphasis is placed on adhesion properties or optical properties, the amount of plasticizing material used relative to 100 parts by weight of the base polymer can be, for example, 15 parts by weight or less, 10 parts by weight or less, or 5 parts by weight. the following.

(Leveling agent) In several aspects, the adhesive composition used to form the adhesive layer can be used to improve the appearance of the adhesive layer formed by the composition (for example, to improve the uniformity of thickness) or to improve the adhesive composition. For coating properties, etc., a leveling agent is included as required. Non-limiting examples of the leveling agent include acrylic leveling agents, fluorine leveling agents, silicone leveling agents, and the like. As the leveling agent, for example, a suitable one can be selected from commercially available leveling agents and used in a conventional manner.

In several aspects, the above-mentioned leveling agent can suitably use the following polymer (hereinafter also referred to as "polymer (B)"), which is a monomer containing a polyorganosiloxane skeleton (hereinafter also referred to as "monomer") S1") is a polymer of acrylic monomer raw material (hereinafter also referred to as "monomer raw material B"). The polymer (B) can be referred to as a copolymer of monomer S1 and acrylic monomer. The polymer (B) can be used alone or in combination of two or more.

The monomer S1 is not particularly limited, and any monomer containing a polyorganosiloxane skeleton can be used. The monomer S1 can be suitably used for a structure having a polymerizable reactive group at one end. Among them, a base polymer (for example, an acrylic polymer) that has a polymerizable reactive group at one end and does not have a base polymer (for example, an acrylic polymer) that has a cross-linking reaction with the adhesive composition blended with the leveling agent at the other end can be suitably used. The monomer S1 of the base structure. Commercially available products include, for example, a terminally reactive silicone oil manufactured by Shin-Etsu Chemical Co., Ltd. (for example, models such as X-22-174ASX, X-22-2426, X-22-2475, KF-2012, etc.). The monomer S1 can be used alone or in combination of two or more.

The functional group equivalent of the monomer S1 can be, for example, about 100 g/mol to 30000 g/mol. In several ideal aspects, the functional group equivalent is, for example, 500 g/mol or more, may be 800 g/mol or more, may be 1500 g/mol or more, or may be 2000 g/mol or more. In addition, the functional group equivalent may be, for example, 20,000 g/mol or less, may be less than 10,000 g/mol, may be 7000 g/mol or less, or may be 5500 g/mol or less. If the functional group equivalent of monomer S1 is within the above range, it is easy to exert a good leveling effect. In addition, when two or more monomers with different functional group equivalents are used as the monomer S1, the functional group equivalent of the monomer S1 can be the sum of the product of the functional group equivalents of various monomers and the weight fraction of the monomer.

Here, "functional group equivalent" means the weight of the main skeleton (for example, polydimethylsiloxane) bonded to each functional group. The relevant labeling unit g/mol is converted to 1 mol of the functional group. The functional group equivalent of the monomer S1 can be ^{calculated from, for example, 1} H-NMR (proton NMR) spectral intensity based on nuclear magnetic resonance (NMR). The calculation of the functional group equivalent (g/mol) of monomer S1 based on ^{1 H-NMR spectrum intensity can be based on the general structure analysis method related to 1} H-NMR spectrum analysis, and if necessary, refer to Japanese Patent No. 5951153 No. Bulletin of the record. In the functional group equivalent of the monomer S1, the above-mentioned functional group means a polymerizable functional group (for example, an ethylenically unsaturated group such as a (meth)acryloyl group, a vinyl group, and an allyl group).

The content of the monomer S1 in the monomer raw material B can be an appropriate value within the range where the monomer S1 can exert the desired effect, and is not limited by the specific range. In several aspects, the content of the monomer S1 in the monomer raw material B can be, for example, 5-60% by weight, 10-50% by weight, or 15-40% by weight.

In addition to monomer S1, monomer raw material B also contains acrylic monomers that can be copolymerized with monomer S1. Thereby, the compatibility of the polymer (B) in the adhesive layer can be improved. The acrylic monomer that can be used for the monomer raw material B includes, for example, alkyl acrylate. The "alkyl" mentioned here refers to a chain (including linear and branched) alkyl (group), and does not include the alicyclic hydrocarbon group described later. In several aspects, the monomer raw material B may contain (meth)acrylate C _4-12 alkyl ester (preferably (meth)acrylate C _4-10 alkyl ester, for example (meth)acrylate C _{6- 10} alkyl esters) at least one kind. In several other aspects, the monomer raw material B may contain C _1-18 alkyl methacrylate (preferably C _1-14 alkyl methacrylate, for example, C _1-10 alkyl (meth)acrylate). At least one of ester). The monomer raw material B may include, for example, one or two or more selected from methyl methacrylate (MMA), n-butyl methacrylate (BMA), and 2-ethylhexyl methacrylate (2EHMA) as acrylic monomer.

Other examples of the aforementioned acrylic monomers include (meth)acrylates having an alicyclic hydrocarbon group. For example, cyclopentyl (meth)acrylate, cyclohexyl (meth)acrylate, isobornyl (meth)acrylate, dicyclopentyl (meth)acrylate, 1-adamantyl (meth)acrylate can be used Ester etc. The (meth)acrylate having an alicyclic hydrocarbon group may not be used.

The content of the (meth)acrylate having the above-mentioned alkyl (meth)acrylate and the above-mentioned alicyclic hydrocarbon group in the monomer raw material B may be, for example, 10% by weight or more and 95% by weight or less, and may be 20% by weight or more and 95% by weight or less, 30% by weight or more and 90% by weight or less, 40% by weight or more and 90% by weight or less, or 50% by weight or more and 85% by weight or less.

Other examples of the monomers that can be included in the monomer raw material B together with the monomer S1 include: carboxyl group-containing monomers, acid anhydride group-containing monomers, hydroxyl group-containing monomers, Epoxy group-containing monomers, cyano group-containing monomers, isocyanate group-containing monomers, amine group-containing monomers, monomers with nitrogen atom-containing rings, (meth)acrylic acid aminoalkyl esters, vinyl esters , Vinyl ethers, olefins, (meth)acrylates with aromatic hydrocarbon groups, (meth)acrylates with halogen atoms, etc.

The Mw of the polymer (B) may be, for example, 5,000 or more, preferably 10,000 or more, or 15,000 or more. In addition, the Mw of the polymer (B) may be 200,000 or less, preferably 100,000 or less, 50,000 or less, or 30,000 or less, for example. By setting the Mw of the polymer (B) in an appropriate range, good compatibility and leveling properties can be exerted.

The polymer (B) can be produced by polymerizing the above-mentioned monomers by a known method such as a solution polymerization method, an emulsion polymerization method, a bulk polymerization method, a suspension polymerization method, and a photopolymerization method. In order to adjust the molecular weight of the polymer (B), a chain transfer agent can be used according to the needs. Examples of chain transfer agents used include: compounds with mercapto groups such as tertiary dodecyl mercaptan, mercaptoethanol, and α-thioglycerol; thioglycolic acid esters such as thioglycolic acid and methyl thioglycolate ; Α-Methylstyrene dimer and so on. The amount of the chain transfer agent used is not particularly limited, and it can be appropriately set so that a polymer (B) having a desired molecular weight can be obtained. In several aspects, the usage amount of the chain transfer agent relative to 100 parts by weight of the monomer can be, for example, 0.1-5 parts by weight, 0.2-3 parts by weight, or 0.5-2 parts by weight.

The usage amount of the polymer (B) relative to 100 parts by weight of the base polymer (for example, acrylic polymer) can be set to, for example, 0.001 parts by weight or more, and from the viewpoint of obtaining higher usage effects, it can be set to 0.01 parts by weight Part or more, but also 0.03 part by weight or more. In addition, the amount of the polymer (B) used may be, for example, 3 parts by weight or less, and from the viewpoint of reducing the influence on the refractive index, 1 part by weight or less is appropriate, and it may be 0.5 parts by weight or less. It may be 0.1 parts by weight or less.

(Inorganic Particles) The technique disclosed here can also be suitably implemented in a state where inorganic particles as a refractive index enhancer are not used substantially. In particular, in several aspects, as long as the application effect of the technology disclosed herein is not significantly impaired, the use of inorganic particles as a refractive index enhancer can be allowed. Examples of inorganic particles that can be used as a refractive index enhancer include titanium oxide (titania, TiO ₂ ), zirconia (zirconia, ZrO ₂ ), aluminum oxide, zinc oxide, tin oxide, copper oxide, barium titanate, Inorganic particles composed of niobium oxide (Nb ₂ O _5, etc.) and other inorganic oxides (specifically, metal oxides). The average particle size of the above-mentioned inorganic particles (referring to the 50% volume average particle size obtained by the laser scattering diffraction method) can be selected from, for example, the range of about 10 nm to 100 nm. In addition, the refractive index of the inorganic particles is based on the single-layer film of the material constituting the inorganic particles (using a film thickness that can be used for refractive index measurement), using a commercially available spectroscopic ellipsometer, at a measurement wavelength of 589nm and a measurement temperature of 23°C. Measure under the conditions. For the spectroscopic ellipsometer, for example, the product name "EC-400" (manufactured by JA.Woolam) or its equivalent can be used. The usage amount when using inorganic particles as the refractive index enhancer is preferably less than 5 parts by weight, more preferably less than 1 part by weight, relative to 100 parts by weight of the base polymer. In the aspect of using the additive (H _RO ), the usage amount of the above-mentioned inorganic particles should be set to _{less than 2 times the usage amount of the above-mentioned additive (H RO} ) on a weight basis, and set to 1 time or less or 0.5 times or less. good.

(Crosslinking agent) In the technique disclosed herein, the adhesive composition used to form the adhesive layer may contain a cross-linking agent as needed in order to adjust the cohesive force of the adhesive. As the crosslinking agent, isocyanate-based crosslinking agents, epoxy-based crosslinking agents, aziridine-based crosslinking agents, azoline-based crosslinking agents, melamine-based resins, metal chelate-based crosslinking agents, etc. can be used in the adhesive. A well-known crosslinking agent in the field. Among them, an isocyanate-based crosslinking agent can be suitably used. As another example of the crosslinking agent, a monomer having two or more ethylenically unsaturated groups in one molecule, that is, a polyfunctional monomer, can be cited. A crosslinking agent can be used individually by 1 type or in combination of 2 or more types.

The isocyanate-based crosslinking agent can use isocyanate compounds with more than two functions, such as trimethylene diisocyanate, butylene diisocyanate, hexamethylene diisocyanate (HDI), and aliphatic polyisocyanate such as diisocyanate. Class; cyclopentyl diisocyanate, cyclohexyl diisocyanate, isophorone diisocyanate (IPDI), 1,3-bis(isocyanatomethyl)cyclohexane and other alicyclic isocyanates; 2,4 -Aromatic isocyanates such as toluene diisocyanate, 4,4'-diphenylmethane diisocyanate, XDI Bonds, uretdione bonds, urea bonds, carbodiimide bonds, uretonimine bonds, polyisocyanate modified materials such as modified polyisocyanate bonds, etc. Examples of commercially available products include: trade names TAKENATE 300S, TAKENATE 500, TAKENATE 600, TAKENATE D165N, TAKENATE D178N (above, manufactured by Takeda Pharmaceutical Co., Ltd.), Sumidur T80, Sumidur L, Desmodur N3400 (above, Sumika Bayer Urethane Co., Ltd.) System), Millionate MR, Millionate MT, Coronate L, Coronate HL, Coronate HX (above, manufactured by Tosoh), etc. An isocyanate compound can be used individually by 1 type or in combination of 2 or more types. A bifunctional isocyanate compound and a trifunctional or higher isocyanate compound can also be used in combination.

Examples of epoxy crosslinking agents include bisphenol A, epichlorohydrin type epoxy resins, ethyleneglycidyl ether, polyethylene glycol diglycidyl ether, and glycerin diglycidyl ether. , Glycerol triglycidyl ether, 1,6-hexanediol glycidyl ether, trimethylolpropane triglycidyl ether, diglycidyl aniline, diaminoglycidylamine, N ,N,N',N'-tetraglycidyl-diamine and 1,3-bis(N,N-diglycidylaminomethyl)cyclohexane, etc. These can be used individually by 1 type or in combination of 2 or more types.

Examples of multifunctional monomers include ethylene glycol di(meth)acrylate, propylene glycol di(meth)acrylate, polyethylene glycol di(meth)acrylate, polypropylene glycol di(meth)acrylate , Neopentyl glycol di(meth)acrylate, neopentyl erythritol di(meth)acrylate, neopentyl erythritol tri(meth)acrylate, dineopentyl erythritol hexa(meth)acrylate, Ethylene glycol di(meth)acrylate, 1,6-hexanediol di(meth)acrylate, 1,12-dodecanediol di(meth)acrylate, trimethylolpropane tri(meth)acrylate Base) acrylate, tetramethylolmethane tri(meth)acrylate, allyl (meth)acrylate, vinyl (meth)acrylate, divinylbenzene, diphenoxyethanol and bis(meth)acrylic acid Ester, bisphenol A di(meth)acrylate, epoxy acrylate, polyester acrylate, urethane acrylate, butyl glycol di(meth)acrylate, hexyl glycol di(meth) Acrylic etc. A polyfunctional monomer can be used individually by 1 type or in combination of 2 or more types.

The amount of the crosslinking agent (which may be a polyfunctional monomer) is not particularly limited, and for example, it may be in the range of about 0.001 parts by weight to 5.0 parts by weight relative to 100 parts by weight of the base polymer. From the viewpoint of improving the flexibility of the adhesive, in several aspects, the amount of crosslinking agent used relative to 100 parts by weight of the base polymer is preferably 3.0 parts by weight or less, more preferably 2.0 parts by weight or less, which can be 1.0 parts by weight or less, may be 0.5 parts by weight or less, or 0.2 parts by weight or less. In addition, from the viewpoint of properly exerting the effect of the cross-linking agent, in several aspects, the amount of the cross-linking agent used relative to 100 parts by weight of the base polymer may be, for example, 0.005 parts by weight or more, or 0.01 parts by weight. The above may be 0.05 parts by weight or more, or 0.08 parts by weight or more.

In order to make the crosslinking reaction proceed more efficiently, a crosslinking catalyst may also be used. Examples of crosslinking catalysts include metal crosslinking catalysts such as tetra-n-butyl titanate, tetraisopropyl titanate, iron (III) acetone acetone, butyl tin oxide, and dioctyl tin dilaurate. Among them, tin-based crosslinking catalysts such as dioctyl tin dilaurate are preferred. The amount of crosslinking catalyst used is not particularly limited. Taking into account the balance between the speed of the cross-linking reaction and the life span of the adhesive composition, the usage amount of the cross-linking catalyst relative to 100 parts by weight of the base polymer can be set to, for example, about 0.0001 part by weight or more and 1 part by weight or less The range is preferably 0.001 part by weight or more and 0.5 part by weight or less.

The adhesive composition may contain a compound capable of producing keto-enol tautomerism as a crosslinking retarder. Thereby, the effect of extending the service life of the adhesive composition can be achieved. For example, in an adhesive composition containing an isocyanate-based crosslinking agent, a compound capable of producing keto-enol tautomerism can be suitably used. Various β-dicarbonyl compounds can be used as compounds capable of producing keto-enol tautomerism. For example, β-diketones (acetone, 2,4-hexanedione, etc.) or acetyl acetates (methyl acetylacetate, ethyl acetylacetate, etc.) can be suitably used. The compound capable of producing keto-enol tautomerism can be used singly or in combination of two or more kinds. The amount of the compound that can produce keto-enol tautomerism can be set to, for example, 0.1 part by weight or more and 20 parts by weight, or 0.5 part by weight or more and 10 parts by weight relative to 100 parts by weight of the base polymer. Hereinafter, it may be 1 part by weight or more and 5 parts by weight or less.

(Tackifier) The adhesive layer in the technology disclosed herein may also contain a tackifier. Tackifiers can use rosin-based tackifying resins, terpene-based tackifying resins, phenol-based tackifying resins, hydrocarbon-based tackifying resins, ketone-based tackifying resins, polyamide-based tackifying resins, epoxy-based tackifying resins, Well-known tackifying resins such as elastic system tackifying resins. These can be used individually by 1 type or in combination of 2 or more types. The amount of the tackifying resin used is not particularly limited, and it can be set according to the purpose and application so that it can exert an appropriate adhesive performance. In several aspects, from the viewpoint of refractive index or transparency, it is appropriate to set the amount of tackifier to be 30 parts by weight or less relative to 100 parts by weight of the base polymer of the adhesive layer, and it is suitable to be 10 Parts by weight or less, preferably 5 parts by weight or less. The technique disclosed here can be suitably implemented without using a tackifier.

(Other additives) In the technology disclosed herein, the adhesive composition used to form the adhesive layer can also optionally include plasticizers, softeners, colorants, antistatic agents, and anti-aging agents within the range that does not significantly hinder the effects of the present invention. Well-known additives such as additives, ultraviolet absorbers, antioxidants, light stabilizers, preservatives, etc. can be used for the adhesive composition. Regarding the various additives, conventionally known additives can be used in accordance with conventional methods, without particularly imparting any characteristics to the present invention, so detailed descriptions are omitted.

＜Production of Adhesive Layer＞ In the technology disclosed herein, the adhesive forming the adhesive layer (which can be a high-refractive-index adhesive layer and/or a low-refractive-index adhesive layer; the same applies hereinafter) can be dried, cross-linked, polymerized, cooled, etc. The adhesive formed by curing the adhesive composition of solvent type, active energy ray curing type, water dispersion type, hot melt type, etc., can also be the cured product of the above-mentioned adhesive composition. The hardening means (such as drying, cross-linking, polymerization, cooling, etc.) of the adhesive composition can be applied only one type, or two or more types can be applied simultaneously or in multiple stages. In the case of a solvent-based adhesive composition, the composition can typically be dried (preferably further cross-linked) to form an adhesive. Regarding the active energy ray-curable adhesive composition, the adhesive is typically formed by irradiating active energy rays to cause the polymerization reaction and/or the crosslinking reaction to proceed. When the active energy ray hardening adhesive composition must be used for drying, the active energy ray can be irradiated after drying.

The adhesive layer of the adhesive sheet in the technology disclosed herein can be formed by applying (for example, coating) an adhesive composition to a suitable surface and then hardening the composition. For coating the adhesive composition, for example, a gravure roll coater, a reverse roll coater, a touch roll coater, a dip roll coater, a bar coater, a knife coater, a sprayer, etc. can be used. Fabric machine to implement.

The adhesive layer in the technology disclosed herein may be an adhesive layer with post-curing properties, or an adhesive layer without post-curing properties. Here, the post-curable adhesive layer refers to an adhesive layer that can be further cured by irradiation of heat or active energy rays (for example, ultraviolet rays). Examples of the adhesive layer having post-curing properties include an adhesive layer having an unreacted ethylenically unsaturated group in the side chain of the base polymer, or an adhesive layer containing an unreacted polyfunctional monomer. In several aspects, the adhesive layer should not have post-curing properties. The adhesive layer without post-curing property does not undergo dimensional changes accompanying the post-curing reaction (that is, the dimensional stability is good), so it is easy to suppress the warpage of the adhesive layer or the adherend to which the adhesive layer is attached. It is also advantageous from the viewpoint of suppressing the optical strain of the adhesive layer that dimensional changes (such as curing shrinkage) caused by post-curing will not occur.

The thickness of the adhesive layer is not particularly limited, and it can be set to, for example, 3 µm or more, and preferably 5 µm or more. With an adhesive layer with a thickness of 5µm or more, good adhesive properties can be easily obtained. In addition, the thickness of the adhesive layer absorbs the unevenness that may exist on the surface of the adherend, and is easily bonded to the adherend with good adhesion. From the viewpoint of preventing coloration or color unevenness caused by light interference, the thickness of the adhesive layer (for example, the thickness of the high refractive index adhesive layer) is preferably 5 µm or more. In several aspects, the thickness of the adhesive layer can be 10 μm or more, 20 μm or more, 30 μm or more, 50 μm or more, or 70 μm or more or 85 μm or more. Moreover, in several aspects, the thickness of the adhesive layer may be, for example, 300 µm or less, 250 µm or less, 200 µm or less, 150 µm or less, or 120 µm or less. The thickness of the adhesive layer is not too large, which is advantageous from the viewpoint of thinning of the laminate sheet or the light-emitting device including the adhesive layer. The technique disclosed here is suitable to be implemented when the thickness of the adhesive layer is in the range of 3 μm to 200 μm (preferably 5 μm to 100 μm). In several aspects, the thickness of the aforementioned adhesive layer can be at least applied to the thickness T _{1 of the} high-refractive-index adhesive layer. _{The thickness T 2 of the} low refractive index adhesive layer can also be selected from the same range. The thickness of the high refractive index layer of the adhesive agent T ₁ and the thickness of the low refractive index layer of the adhesive agent T ₂ may be the same level, or different. The ratio of the thickness T ₁ of the high refractive index adhesive layer to the thickness T ₂ of the _{low refractive index adhesive layer (T 1} /T ₂ ) can be, for example, 0.1 or more, 0.3 or more, 0.5 or more, or 0.8 or more , Can be 1.2 or more, or 1.5 or more. In addition, the aforementioned ratio (T ₁ /T ₂ ) may be, for example, 20 or less, 10 or less, 5 or less, or 3 or less. In several aspects, the aforementioned ratio (T ₁ /T ₂ ) can be less than 2, can be less than 1.5, or less than 1.

The method of obtaining a structure (laminated sheet) composed of a low-refractive-index adhesive layer and a high-refractive-index layer (typically a high-refractive A method of forming a high-refractive-index adhesive layer and a low-refractive-index adhesive layer on the surface) respectively, and bonding them; bonding the low-refractive-index adhesive layer formed on the peelable surface to the non-adhesive high The method of the refractive index layer; the method of coating the adhesive composition used to form the low refractive index adhesive layer on the high refractive index layer and hardening, or vice versa, coating the composition used to form the high refractive index layer The method of laying on the low-refractive-index adhesive layer and hardening, etc. are not limited by these. When bonding the high-refractive index layer and the low-refractive-index adhesive layer, processing to promote the adhesion of the other layers can also be performed as required. For example, autoclave treatment, roll pressing treatment, etc. can be carried out, but it is not limited by these.

(Peel strength) In several aspects, it is appropriate that the peel strength of the adhesive layer to the glass plate disclosed here is about 1.0N/25mm or more (for example, 1.5N/25mm or more), preferably 2N/25mm or more, more preferably 3N /25mm or more, can be 4N/25mm or more, can be 6N/25mm or more, can be 8N/25mm or more, can be 10N/25mm or more, or can be 12N/25mm or more. The upper limit of the peel strength is not particularly limited. For example, it may be 30N/25mm or less, 25N/25mm or less, or 20N/25mm or less.

Here, the above-mentioned peeling strength is grasped by the following method: crimping on an alkali glass plate as the adherend and placing it in an environment of 23°C and 50% RH for 30 minutes, and then putting it into a pressurized deaeration device ( Autoclave) in an autoclave at a temperature of 50°C and a pressure of 0.5MPa for 30 minutes, and then placed in a gas environment of 23°C and 50%RH for 24 hours, at a peeling angle of 180° and a stretching speed of 300mm/ Peel off at 180° under the condition of minutes, and measure the adhesive force. During the measurement, a suitable backing material (for example, a polyethylene terephthalate (PET) film with a thickness of about 25 µm ~ 50 µm) can be attached to the measurement object as required to reinforce it. More specifically, the peel strength can be measured according to the method described in the examples described later. When the low-refractive-index adhesive layer and the high-refractive-index adhesive layer disclosed herein are laminated to form a laminated sheet in the form of a double-sided adhesive sheet having a first adhesive surface and a second adhesive surface, among several aspects, the above The peel strength should be applied to at least the second adhesive surface (adhesive surface composed of a low refractive index adhesive layer), and more preferably applied to both the first adhesive surface and the second adhesive surface. The peel strength of the glass plate on the first adhesive surface and the peel strength of the glass on the second adhesive surface may be the same or different.

＜Support base material＞ The low-refractive-index adhesive disclosed herein can be used in the form of an adhesive sheet with a substrate including an adhesive layer formed of the adhesive and a supporting substrate.

The material of the supporting base material is not particularly limited, and can be appropriately selected according to the purpose of use or the state of use. Non-limiting examples of substrates that can be used include: polyolefin films mainly composed of polypropylene (PP) or polyolefins such as ethylene-propylene copolymers, polyethylene terephthalate (PET), polyolefin films, etc. Polyethylene terephthalate (PBT), polyethylene naphthalate (PEN) and other polyester films as main components, polyvinyl chloride films with polyvinyl chloride as the main component, and other plastic films; Polyurethane foam, polyethylene (PE) foam, polychloroprene foam and other foams consist of foam sheets; various fibrous materials (can be natural fibers such as hemp and cotton) , Polyester, vinylon and other synthetic fibers, acetate and other semi-synthetic fibers, etc.) woven and non-woven fabrics individually or blended; Japanese paper, Dolin paper, kraft paper, crepe paper and other papers; aluminum foil, copper foil And other metal foils. It can also be a base material composed of these composites. Examples of the composite substrate include, for example, a substrate with a structure formed by laminating a metal foil and the above-mentioned plastic film, a plastic substrate reinforced with inorganic fibers such as glass cloth, and the like.

In several aspects, various film substrates can be suitably used. The above-mentioned film substrate may be a porous substrate such as a foamed film or a non-woven sheet, a non-porous substrate, or a laminated structure of a porous layer and a non-porous layer. Substrate. In several aspects, the above-mentioned film substrate can be suitably used as a base film including an independent and shape-maintainable (free-standing or non-dependent) resin film. Here, "resin film" refers to a non-porous structure and is typically a resin film that contains substantially no bubbles (no pores). Therefore, the above-mentioned resin film is a concept that can be distinguished from a foam film or a non-woven fabric. The above-mentioned resin film can be suitably used independently and capable of maintaining its shape (independent or non-dependent). The above-mentioned resin film may have a single-layer structure or a multilayer structure of two or more layers (for example, a three-layer structure).

Examples of materials constituting the resin film include polyesters such as polyethylene terephthalate (PET), polybutylene terephthalate (PBT), and polyethylene naphthalate (PEN) as the main component. Polyester resins, polyolefin resins based on polyolefins such as polyethylene (PE), polypropylene (PP), ethylene-propylene copolymers, ethylene-butene copolymers, and cellulose triacetate Polyamide (PA) resins such as resins, acetate-based resins, polyether-based resins, polyether-based resins, polycarbonate-based resins, nylon 6, nylon 66, and partially aromatic polyamides, etc. Amine (PI) resin, transparent polyimide resin, polyamide imide (PAI), polyether ether ketone (PEEK), polyether agglomerate (PES), norbornene resin and other cyclic polyolefin resins , (Meth) acrylic resin, polyvinyl chloride resin, polyvinylidene chloride resin, polystyrene resin, polyvinyl alcohol resin, ethylene-vinyl acetate copolymer resin, ethylene-vinyl alcohol copolymer Resin, polyarylate resin, polyphenylene sulfide (PPS) resin, polyurethane (PU), ethylene-vinyl acetate copolymer (EVA), polytetrafluoroethylene (PTFE) or fluorinated poly Fluorine resins such as imines.

The above-mentioned resin film may be formed using a resin material containing one type of the resin alone, or may be formed using a resin material in which two or more types are blended. The above-mentioned resin film may be non-stretched or stretched (for example, uniaxially stretched or biaxially stretched). For example, PET film, PBT film, PEN film, non-stretched polypropylene (CPP) film, biaxially stretched polypropylene (OPP) film, low-density polyethylene (LDPE) film, linear low-density polyethylene ( LLDPE) film, PP/PE blend film, etc. From the standpoint of strength or dimensional stability, examples of ideal resin films include PET film, PEN film, PPS film, and PEEK film. From the viewpoint of ease of acquisition, PET film and PPS film are particularly suitable, and among them, PET film is preferred.

In the resin film, light stabilizers, antioxidants, antistatic agents, colorants (dyes, pigments, etc.), fillers, slipping agents, Anti-blocking agents and other well-known additives. The blending amount of additives is not particularly limited, and can be appropriately set according to the application of the adhesive sheet.

The manufacturing method of the resin film is not specifically limited. For example, conventionally known general resin film forming methods such as extrusion molding, inflation molding, T-die casting molding, and calender roll molding can be suitably used.

The above-mentioned substrate may be substantially constituted by the above-mentioned base film. Alternatively, the above-mentioned substrate may also include an auxiliary layer in addition to the above-mentioned base film. Examples of the aforementioned auxiliary layers include optical property adjustment layers (for example, coloring layers, anti-reflection layers), printed layers or laminated layers for imparting a desired appearance to the substrate, antistatic layers, and primer layers. , Surface treatment layer such as peeling layer.

In several aspects, a light-transmitting substrate (hereinafter also referred to as a light-transmitting substrate) can be suitably used as the supporting substrate. In this way, an adhesive sheet with a light-transmitting substrate can be constructed. The total light transmittance of the light-transmitting substrate can be, for example, greater than 50%, or more than 70%. In several ideal situations, the total light transmittance of the supporting substrate is more than 80%, preferably more than 90%, or more than 95% (for example, 95-100%). The above-mentioned total light transmittance is measured in accordance with JIS K 7136:2000 using a commercially available transmittance meter. The transmittance meter can use the product name "HAZEMETER HM-150" manufactured by Murakami Color Technology Research Institute or its equivalent. Suitable examples of the above-mentioned light-transmitting substrate include a resin film having light-transmitting properties. The above-mentioned light-transmitting substrate may also be an optical film.

The thickness of the substrate is not particularly limited, and it can be selected according to the purpose of use or the state of use. The thickness of the substrate can be, for example, 500 µm or less, and from the viewpoint of handleability or processability, it is preferably 300 µm or less, and can be 150 µm or less, 100 µm or less, 50 µm or less, 25 µm or less, or It is less than 10µm. If the thickness of the substrate becomes smaller, the followability to the surface shape of the adherend tends to increase. In addition, from the viewpoint of handleability or processability, the thickness of the substrate may be, for example, 2 μm or more, 10 μm or more, or 25 μm or more.

The surface of the substrate on the side where the adhesive layer is to be laminated can also be subjected to corona discharge treatment, plasma treatment, ultraviolet radiation treatment, acid treatment, alkali treatment, and primer formation by coating a primer (primer). Conventionally known surface treatment such as coating. The surface treatment may be a treatment for improving the anchoring property of the adhesive layer to the substrate. The composition of the primer used to form the primer layer is not particularly limited, and can be appropriately selected from known materials. The thickness of the primer layer is not particularly limited. Usually, about 0.01µm~1µm is appropriate, and about 0.1µm~1µm is better. Other treatments that can be performed on the substrate according to needs include antistatic layer formation treatment, colored layer formation treatment, printing treatment, and the like. These treatments can be applied individually or in combination.

In the technology disclosed herein, when the low-refractive-index adhesive layer constitutes an adhesive sheet with a substrate, the thickness of the adhesive sheet can be, for example, 1000 µm or less, 350 µm or less, 200 µm or less, 120 µm or less, or Below 75µm, it can also be below 50µm. In addition, from the viewpoint of handling properties and the like, the thickness of the adhesive sheet may be, for example, 10 μm or more, 25 μm or more, 80 μm or more, or 130 μm or more. In addition, the thickness of the adhesive sheet means the thickness of the part attached to the adherend. For example, in the double-sided adhesive sheet 2 without a substrate in the structure shown in FIG. 2, the thickness from the first surface (first adhesive surface) 10A of the adhesive layer to the second surface (second adhesive surface) 10B , Excluding the thickness of the release liner 31, 32.

＜Adhesive sheet＞ The low-refractive-index adhesive disclosed here can be used in the form of an adhesive sheet that includes an adhesive layer (low-refractive-index adhesive layer) formed by the adhesive, and may further include other layers ( High refractive index adhesive layer, supporting substrate, etc.).

(Total light transmittance) In the technology disclosed herein, the total light transmittance of the low refractive index adhesive layer is suitably 86% or more, preferably 88% or more, more preferably 90% or more (for example, more than 90.0%), and can be 90.5% or more , Can be more than 93%, or more than 95%. The upper limit of total light transmittance is theoretically a value obtained by excluding 100% of the light loss (Fresnel loss) caused by reflection at the air interface. In practice, it can be about 98% or less, which can be About 96% or less, or about 95% or less. In several aspects, considering the refractive index or adhesive properties, the total light transmittance of the low refractive index adhesive layer can be about 94% or less, about 93% or less, or about 92% or less. The total light transmittance is measured in accordance with JIS K 7136:2000 using a commercially available transmittance meter. The transmittance meter can use the product name "HAZEMETER HM-150" manufactured by Murakami Color Technology Research Institute or its equivalent. More specifically, for example, the total light transmittance of the low-refractive-index adhesive layer can be measured according to the following examples. The total light transmittance of the low refractive index adhesive layer can be adjusted by, for example, selecting the composition or thickness of the low refractive index adhesive layer. The above description of the total light transmittance of the low refractive index adhesive layer can also be applied to: the total light transmittance of the adhesive sheet comprising the low refractive index adhesive layer and the supporting substrate, or the total light transmittance of the high refractive index layer , The total light transmittance of the laminated sheet (adhesive sheet) containing a low-refractive-index adhesive layer and a high-refractive-index layer (typically a high-refractive-index adhesive layer).

(Haze value) It is appropriate that the haze value of the low refractive index adhesive layer is below 3.0%, and is preferably below 2.0%, more preferably below 1.0%, and more preferably below 0.9%. The low haze value of the low-refractive-index adhesive layer is beneficial for applications that require high light transmittance (such as optical applications), or applications that require good visibility of the performance of the adherend through the low-refractive-index adhesive layer . In several aspects, the haze value of the low refractive index adhesive layer can be 0.8% or less, 0.5% or less, or 0.3% or less. The lower limit of the haze value of the low refractive index adhesive layer is not particularly limited. From the viewpoint of improving transparency, the smaller the haze value, the better. On the other hand, in several aspects, considering the refractive index or adhesive properties, the haze value of the low refractive index adhesive layer can be, for example, 0.05% or more, 0.1% or more, 0.2% or more, or 0.3% or more, but also 0.4% or more. The above description of the haze value of the low-refractive-index adhesive layer can also be applied to: the haze value of the adhesive sheet containing the low-refractive The haze value of the laminated sheet (adhesive sheet) of the refractive index adhesive layer and the high refractive index layer (typically a high refractive index adhesive layer).

Here, "haze value" refers to the ratio of diffuse transmitted light to total transmitted light when the object to be measured is irradiated with visible light. Also known as Haze Value. The haze value can be expressed by the following formula. Th(%)=Td/Tt×100 In the above formula, Th is the haze value (%), Td is the scattered light transmittance, and Tt is the total light transmittance. The measurement of the haze value can be carried out in accordance with the method described in the following examples. The haze value of the adhesive layer can be adjusted by, for example, selecting the composition or thickness of the adhesive layer.

(Surface smoothness of adhesive surface) In several aspects, the surface (adhesive surface) of the adhesive layer preferably has high surface smoothness.

For example, the arithmetic average roughness Ra of the above-mentioned adhesive surface should be limited below a predetermined value. From the viewpoint of optical homogeneity, it is preferable to have a structure with an adhesive surface designed so that the arithmetic average roughness Ra becomes low. By limiting the arithmetic average thickness Ra, for example, in the use of the above-mentioned adhesion surface to capture light (the light-emitting device is arranged on the adhesive sheet on the side of the viewpoint than the self-luminous element, etc.), it is possible to suppress the adhesion due to The surface state of the agent layer has the effect of uneven brightness. The fact that the arithmetic average roughness Ra of the adhesive surface is low is also beneficial to suppress the optical strain, and the suppression of the optical strain also helps to improve the optical homogeneity. When the adhesive sheet disclosed here is in the form of a double-sided adhesive sheet having a first adhesive surface and a second adhesive surface (for example, the form of a laminated sheet including a high-refractive-index adhesive layer and a low-refractive-index adhesive layer), preferably at least The arithmetic average roughness Ra of the first adhesive surface is limited to a predetermined value or less, and it is preferable that the arithmetic average roughness Ra of both adhesive surfaces is limited to a predetermined value or less. With the high surface smoothness of each adhesive surface of the double-sided adhesive sheet, it is suitable to realize bonding with excellent optical homogeneity.

In several aspects, the arithmetic average roughness Ra of the adhesive surface is preferably about 70 nm or less, more preferably about 65 nm or less, more preferably about 55 nm or less, and may be less than 50 nm, less than 45 nm, or less than 40 nm. From the viewpoint of production efficiency and the like, in several aspects, the arithmetic average roughness Ra of the adhesive surface may be, for example, about 10 nm or more, about 20 nm or more, or about 30 nm or more (for example, about 40 nm or more). In the case where the adhesive sheet has a first adhesive surface and a second adhesive surface, the arithmetic average thickness Ra of the first adhesive surface and the arithmetic average thickness Ra of the second adhesive surface may be the same or different.

Also, for example, the maximum height Rz of the above-mentioned adhesive surface should be limited to a predetermined value or less. From the viewpoint of optical homogeneity, it is preferable to have a structure with an adhesive surface designed to reduce the maximum height Rz. By limiting the maximum height Rz, for example, in the above-mentioned use mode of capturing light through the above-mentioned adhesive surface, the effect of suppressing uneven brightness due to the surface state of the adhesive layer can be exerted. The fact that the maximum height of the adhesive surface Rz is low is also beneficial to suppress the optical strain. When the adhesive sheet disclosed here is in the form of a double-sided adhesive sheet with a first adhesive surface and a second adhesive surface, it is preferable that at least the maximum height Rz of the first adhesive surface is limited to a predetermined value or less, preferably one of the two adhesive surfaces The maximum height Rz is restricted below a predetermined value. With the high surface smoothness of each adhesive surface of the double-sided adhesive sheet, it is suitable to realize bonding with excellent optical homogeneity.

In several aspects, the maximum height Rz of the adhesive surface is preferably about 600nm or less, more preferably about 500nm or less, more preferably about 450nm or less, particularly preferably about 400nm or less, may be less than 350nm, may be less than 300nm, or Less than 250nm. From the viewpoint of production efficiency, among several aspects, the maximum height Rz of the adhesive surface may be, for example, about 10 nm or more, about 50 nm or more, about 100 nm or more, or about 200 nm or more. In the aspect having the first adhesive surface and the second adhesive surface, the maximum height Rz of the first adhesive surface and the maximum height Rz of the second adhesive surface may be the same or different.

The arithmetic average roughness Ra and maximum height Rz of the adhesive surface are measured using a non-contact surface roughness measuring device. The non-contact surface roughness measuring device can be an optical interference surface roughness measuring device, for example, a three-dimensional optical profiler (trade name "NewView 7300", manufactured by ZYGO) or its equivalent can be used. Specifically, for example, the arithmetic average roughness Ra and the maximum height Rz can be measured by the following measurement method or by setting the measurement operation or measurement conditions such that the result equivalent or corresponding to the case of using the measurement method can be obtained.

That is, using a three-dimensional optical profiler (trade name "NewView7300", manufactured by ZYGO), the surface shape of the measurement sample was measured under the following conditions in an environment of 23° C. and 50% RH. From the measured data, the arithmetic surface roughness Ra is calculated in accordance with JIS B 0601-2001. The maximum height Rz is based on the data (roughness curve) obtained by the above measurement, the height Rp from the average line of the roughness curve to the highest top on the upper side and the depth Rv from the average line to the deepest valley on the lower side are obtained的和。 The sum. Perform 5 measurements (that is, N=5), and use the average value of these. The sample for measurement can be prepared by cutting, for example, the adhesive layer of the object to be measured or the adhesive sheet containing the adhesive layer into a size of approximately 150 mm in length and 50 mm in width. When the adhesive surface is protected by the release liner, peel off the release liner smoothly (for example, at a stretching speed of 300 mm/min and a peeling angle of 180°) to expose the adhesive surface. It is advisable to make the measurement after allowing the adhesive surface to stand for about 30 minutes. [Measurement conditions] Measuring area: 5.62mm×4.22mm (Objective lens: 2.5 times, internal lens: 0.5 times) Analysis mode: Remove: Cylinder Data Fill: ON (Max: 25) Remove Spikes: ON (xRMS: 1) Filter: OFF

The arithmetic average roughness Ra and maximum height Rz of the adhesive surface can be determined by the composition or properties (viscosity, leveling, etc.) of the adhesive composition used to form the adhesive layer, and the surface of the release liner that protects the adhesive surface (peeling Noodles) traits and so on.

(Water absorption) Among the several aspects in which the low refractive index adhesive can be used together with the high refractive index adhesive layer disclosed herein, the water absorption rate of the high refractive index adhesive layer should be limited below a predetermined value. By limiting the water absorption of the high refractive index adhesive layer, it is possible to suppress the change in the amount of moisture in the high refractive index adhesive layer (such as the absorption and release of moisture in the environment) resulting in the high refractive index adhesive layer The tendency of size changes. As a result, the high refractive index adhesion caused by the inconsistency of the dimensional changes between the high refractive index adhesive layer and the adjacent layer (which can be a low refractive index adhesive layer, support substrate, release liner, adherend, etc.) can be suppressed Warpage of the agent layer or the optical laminate containing the high refractive index adhesive layer. It is also preferable from the viewpoint that the flatness, transparency, and refractive index of the high-refractive-index adhesive layer can be fixed and maintained because the fluctuation of the moisture content in the high-refractive-index adhesive layer can be suppressed. In addition, the high-refractive-index adhesive layer with low water absorption is not easy to absorb moisture, so it is suitable as a component of a member or product containing an element that does not like moisture, such as an organic EL element.

In several aspects, the water absorption rate of the high refractive index adhesive layer is approximately 1.0% or less, preferably 0.7% or less, more preferably 0.5% or less (for example, less than 0.5%), and can be 0.4% or less, It can be 0.3% or less, or 0.2% or less. The lower limit of the water absorption of the high refractive index adhesive layer is not particularly limited. From a practical point of view such as compatibility with adhesive properties, for example, it can be 0.01% or more, 0.05% or more, 0.1% or more, or 0.15 % Or more, but also 0.25% or more. The water absorption rate of the low refractive index adhesive layer may be the same as or different from the water absorption rate of the high refractive index adhesive layer. From the viewpoint of obtaining a higher effect, the water absorption of the high-refractive-index adhesive layer and the low-refractive-index adhesive layer should both be restricted below a predetermined value.

In addition, the water absorption (also referred to as moisture content) of the high refractive index adhesive layer was measured by the following method. The water absorption of the low refractive index adhesive layer is also measured by the same method. [Measurement of moisture content] Cut the adhesive layer of the evaluation object and two release liners arranged on one side and the other side into a size of 4cm×5cm (area: 20cm ² ), and remove the peeling on one side After padding, attach it to the pre-weighed aluminum foil. Next, remove the release liner on the other side of the adhesive layer, put it into a constant temperature and humidity bath at a temperature of 60°C and a relative humidity of 90%, and take it out 72 hours later. After weighing the test piece laminated with the adhesive layer and aluminum foil, use a moisture meter (Mitsubishi Chemical Analytech CA-200) equipped with a heating vaporization device (Mitsubishi Chemical Analytech VA-200) by Karl Fischer (Karl Fischer) Coulometric titration measures the moisture content under the following conditions. Anolyte: AQUAMICRON AKX (manufactured by Mitsubishi Chemical) Catholyte: AQUAMICRON CXU (manufactured by Mitsubishi Chemical) Heating and vaporization temperature: 150°C

(Gel fraction) The gel fraction of the adhesive layer disclosed here can be appropriately set according to the purpose of use or usage, and is not limited by a specific range. The above-mentioned gel fraction is, for example, approximately 99% or less, and approximately 97% or less is suitable. From the viewpoint of easy and suitable compatibility between low refractive index and adhesive properties, in several ideal situations, the above-mentioned gel fraction is about 95% or less, preferably about 92% or less (for example, about 90% or less). The reason that the gel fraction is not too high can appropriately follow the unevenness that exists on the surface of the adherend (for example, the uneven structure provided in the light-emitting device to improve the light extraction efficiency, etc.) so as to achieve good adhesion. In several aspects, the gel fraction may be about 88% or less, may be about 75% or less, or may be about 65% or less. In addition, from the viewpoint of imparting moderate agglutinating properties to the adhesive and exhibiting adequate adhesive properties, the gel fraction is, for example, about 10% or more, and it is appropriate to set it to about 20% or more, and it may also be about 30% or more. . From the point of view of the resistance to deformation of the adhesive layer (preventing overflow caused by pressure or bubbles caused by the inclusion of foreign objects, etc.), the above-mentioned gel fraction should be about 30% or more, more preferably about 40% or more, It may be about 45% or more, it may be about 50% or more, it may be about 65% or more, or it may be about 75% or more. Adhesive sheet comprising a high-refractive-index adhesive layer and a low-refractive-index adhesive layer (e.g., a laminated sheet in the form of a double-sided adhesive sheet without a substrate composed of a high-refractive-index adhesive layer and a low-refractive-index adhesive layer) The gel fraction should also be set to the range exemplified above. The gel fraction can be adjusted by the molecular weight or molecular structure, concentration, and degree of crosslinking of the base polymer. The gel fraction is measured by the following method.

[Determination of Gel Fraction] A predetermined amount of adhesive sample (weight Wg _{1 ) is wrapped into a small bag with a porous polytetrafluoroethylene membrane (weight Wg 2} ) with an average pore diameter of 0.2 µm, and used kite string (weight Wg) ₃ ) Tie the opening. The above-mentioned porous polytetrafluoroethylene (PTFE) film uses the trade name "Nitoflon (registered trademark) NTF1122" (average pore diameter 0.2 µm, porosity 75%, thickness 85 µm) available from Nitto Denko Corporation or its equivalent. The package is immersed in a sufficient amount of ethyl acetate and kept at room temperature (typically 23°C) for 7 days. After only the sol in the adhesive is dissolved out of the film, the package is taken out and the adhesion is wiped. Apply ethyl acetate on the outer surface, dry the package at 130°C for 2 hours, and measure the weight (Wg ₄ ) of the package. The gel fraction of the adhesive layer can be obtained by substituting each value into the following formula. Gel fraction (%)=[(Wg ₄ -Wg ₂ -Wg ₃ )/Wg ₁ ]×100

The gel fraction of the high refractive index adhesive layer and the gel fraction of the low refractive index adhesive layer may be the same or different. In several aspects, the gel fraction of the low refractive index adhesive layer can be made higher. The gel fraction of the refractive index adhesive layer can be lower. According to this structure, it is easy to improve the overall flexibility due to the contribution of the low-refractive-index adhesive layer with a relatively low gel fraction. In this way, high refractive index and flexibility can be balanced.

In several aspects of the technology disclosed herein, the peak temperature of tanδ of the adhesive constituting the high refractive index adhesive layer is preferably about -50°C or more, and preferably about 50°C or less. Here, the tanδ (loss tangent) of the adhesive means the ratio of the loss elastic modulus G" to the storage elastic modulus G'of the adhesive. That is, tanδ=G"/G'. The tanδ of the adhesive can sandwich a disk-shaped adhesive sample with a thickness of about 2mm and a diameter of 7.9mm in parallel plates, while using a viscoelastic test device to give a shear strain of 1 Hz, while measuring the temperature range of -60 ℃ Under the condition of ~60℃ and heating rate of 5℃/min, conduct the temperature dispersion test of the adhesive in shear mode, and from this time the storage elastic modulus G'(Pa) and loss elastic modulus G"(Pa) It can be obtained by the following formula: tanδ=G”/G'. The peak temperature of tan δ of the adhesive can be obtained from the transition of tan δ in the above temperature range (there are cases where it is expressed as Tpeak below). The viscoelasticity test device can use ARES manufactured by TA Instruments or its equivalent.

In several aspects, it is advantageous for the Tpeak of the high refractive index adhesive layer to be below 45°C or below 35°C, and preferably below 30°C (for example, below 25°C), may be below 20°C, or 15 Below ℃. With lower Tpeak adhesives, there is a tendency to easily obtain good initial adhesion or adhesion at room temperature. On the other hand, the Tpeak of the adhesive is not too low from the viewpoint of imparting moderate agglutinating properties to the adhesive, and it has a tendency to be suitable for taking into account the high refractive index. From the above point of view, in several aspects, the Tpeak of the adhesive can be, for example, -40°C or higher, -30°C or higher, -20°C or higher, -5°C or higher, or 5 The temperature is higher than 15°C, and it may be higher than 25°C. When the adhesive with higher Tpeak is attached to the adherend, it can be used in a state where one or both of the adhesive and the adherend are heated to a temperature slightly higher than room temperature as required. . The Tpeak of the adhesive can be adjusted by selecting the composition of the adhesive (for example, the composition of the monomer components constituting the base polymer, whether to use a refractive index enhancer or plasticizing material, and the type and amount of use). The Tpeak of the above-mentioned adhesive is preferably applied to at least the high-refractive-index adhesive layer, and is more preferably applied to both the high-refractive-index adhesive layer and the low-refractive-index adhesive layer. The Tpeak of the high refractive index adhesive layer and the Tpeak of the low refractive index adhesive layer may be the same or different.

＜Laminated sheet with release liner＞ The high-refractive-index adhesive layer and the low-refractive-index adhesive layer disclosed herein can be brought into contact with and peeled off the adhesive surface of the laminated sheet including the high-refractive-index adhesive layer and the low-refractive-index adhesive layer before being incorporated into the light-emitting device. The form of the release surface of the liner is the form of an adhesive product (laminated sheet with release liner). Therefore, according to this specification, a laminated sheet (adhesive product) with a release liner is provided, which includes a laminated sheet of a high-refractive-index adhesive layer and a low-refractive-index adhesive layer, and a peeling sheet having an adhesive surface that abuts the laminated sheet The surface of the release liner.

The release liner is not particularly limited. For example, a release liner with a release treatment layer on a release liner substrate such as a resin film or paper (paper laminated with resin such as polyethylene) can be used, or by Fluorine-based polymers (polytetrafluoroethylene, etc.) or polyolefin-based resins (polyethylene, polypropylene, etc.) and other low-adhesion materials composed of resin films composed of release liners, etc. The above-mentioned release treatment layer may be formed by subjecting a release liner base material to a surface treatment with a release treatment agent. The release treatment agent may be a known release treatment agent such as a silicone-based release treatment agent, a long-chain alkyl-based release treatment agent, a fluorine-based release treatment agent, and molybdenum (IV) sulfide. Among several aspects, a release liner having a release treatment layer obtained with a silicone release treatment agent can be suitably used. The thickness or formation method of the release treatment layer is not particularly limited, and it can be set so that it can exhibit appropriate release properties on the adhesive surface side surface of the release liner.

Among several aspects, from the viewpoint of smoothness of the adhesive surface, etc., a release liner having a release treatment layer on a resin film as a release liner substrate (hereinafter also referred to as a release film substrate) can be suitably used (Hereinafter also referred to as release film). Various plastic films can be used for the release film substrate. In this specification, the so-called plastic film is typically a non-porous sheet, which is, for example, a concept that can be distinguished from non-woven fabric (that is, non-woven fabric is not included).

The material of the above-mentioned plastic film may include, for example, polyester resins such as polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), and polyethylene (PE), polypropylene (PP), polyolefin resins such as ethylene-propylene copolymers, ethylene-butene copolymers, cellulose resins such as cellulose triacetate, acetate-based resins, polytene-based resins, and polyethers Cyclic polyolefin resins such as chrysene resins, polycarbonate resins, polyamide resins, polyimide resins, norbornene resins, (meth)acrylic resins, polyvinyl chloride resins, polyamide resins, etc. Dichlorovinylidene resins, polystyrene resins, polyvinyl alcohol resins, ethylene-vinyl acetate copolymer resins, ethylene-vinyl alcohol copolymer resins, polyarylate resins, polyphenylene sulfide resins, etc. . It is also possible to use a release film substrate formed of any one or a mixture of two or more of these resins. Among them, a preferred release film substrate includes a polyester resin film formed of a polyester resin (for example, a PET film).

The plastic film that can be used as the base material of the release film can be any one of non-stretched film, uniaxially stretched film, and biaxially stretched film. In addition, the above-mentioned plastic film may have a single-layer structure or a multi-layer structure including two or more sub-layers. The above plastic film can also be mixed with antioxidants, anti-aging agents, heat-resistant stabilizers, light stabilizers, ultraviolet absorbers, pigments or dyes, such as coloring agents, lubricants, fillers, antistatic agents, nucleating agents, etc. A well-known additive that can be used for the release film substrate of the adhesive sheet. In the multi-layer plastic film, the additives can be blended in all sublayers or only part of the sublayers.

In several ideal aspects, the above-mentioned release film substrate (typically a plastic film) can be suitably used in the layer on the release surface side of inorganic particles and other particles (for example, pigments, lubricants, fillers, etc.) Those whose content has been restricted, or those that do not substantially contain the particles. The term "substantially not included" here means that the amount of particles (for example, inorganic particles) in the layer is less than 1% by weight, and it means that it is preferably less than 0.1% by weight (for example, 0 to 0.01% by weight). The release film provided with the release film base material tends to have a lower arithmetic mean roughness Ra or maximum height Rz of the release surface. When the above-mentioned release film substrate (typically a plastic film) has a multilayer structure, the particle content in the layer on the release surface side may be less than 1/10 (for example, 1/50) of the particle content in the layer other than the release surface side layer. the following).

In the laminated sheet with release liner in the form of a release liner on the first adhesive surface and the second adhesive surface, respectively, the release liner arranged on one of the adhesive surfaces (hereinafter, also referred to as one of the release liners) ) And the release liner (hereinafter, also referred to as another release liner) disposed on the other adhesive surface may have the same material and composition, or may have different materials and composition.

The thickness of the release liner (preferably a release film) is not particularly limited, and may be, for example, about 10 μm to 500 μm. From the standpoint of the strength or dimensional stability of the release liner, it is appropriate that the thickness of the release liner is 20 μm or more, preferably 30 μm or more, can be 35 μm or more, can be 40 μm or more, or can be 45 μm or more. In addition, from the viewpoint of the rationality of the release liner (for example, ease of winding), etc., the thickness of the release liner is appropriately 300 µm or less, and preferably 250 µm or less, 200 µm or less, 150 µm or less, or It can be below 130µm. In several ideal situations, the thickness of the release liner is about 125 µm or less, can be about 115 µm or less, can be about 105 µm or less, can be about 90 µm or less, or can be about 70 µm or less. By setting the thickness of the release liner below a predetermined value, it is not easy to form the winding marks when it is made into a roll shape, and can be smoothly removed from the adhesive sheet, so that the adhesive surface after the release liner is removed is easy to obtain a high surface smoothness sex.

In the laminated sheet with release liner provided with one release liner and the other release liner, the thickness of the release liners may be the same or different from each other. In several aspects, from the viewpoint of release workability, one release liner and the other release liner should have different thicknesses. For example, the thickness of a thicker release liner is preferably a thinner release liner. The thickness is about 1.1 times or more (for example, about 1.25 times or more; the upper limit is not particularly limited, for example, 5 times or less).

(Arithmetic average roughness of the side surface of the adhesive surface Ra) In several aspects, the release liner (preferably a release film), from the viewpoint of achieving an adhesive surface with high surface smoothness, the arithmetic average roughness Ra of the adhesive surface side surface should be limited to a predetermined value or less (for example, About 100nm or less, and further less than 50nm). In several aspects, the arithmetic average roughness Ra of the adhesive surface side surface of the release liner is preferably about 30 nm or less, more preferably about 25 nm or less, may be about 20 nm or less, or may be about 18 nm or less. In addition, from the viewpoints of ease of manufacture and handling of the release liner, in several aspects, the arithmetic average roughness Ra may be, for example, about 5 nm or more, about 10 nm or more, or about 15 nm or more. . In the laminated sheet with release liner in the form of a release liner arranged on the first adhesive surface and the second adhesive surface, the adhesive surface side surfaces of the two release liners should satisfy any of the above-mentioned arithmetic average roughness Ra. The arithmetic average roughness Ra of the adhesive surface side surface of the two release liners may be the same or different.

(Maximum height Rz of the adhesive surface side surface) In several aspects, the release liner (preferably a release film), from the viewpoint of achieving an adhesive surface with high surface smoothness, the maximum height Rz of the adhesive surface side surface is preferably 700 nm or less. In several aspects, the maximum height Rz of the adhesive surface side surface of the release liner is preferably about 600 nm or less, may be about 500 nm or less, may be about 400 nm or less, or may be about 300 nm or less. In addition, from the viewpoints of ease of manufacture or handling of the release liner, among several aspects, the maximum height Rz may be, for example, about 50 nm or more, about 80 nm or more, about 100 nm or more, or It is about 200 nm or more, and it can also be about 300 nm or more. In the laminated sheet with a release liner in the form of a release liner arranged on the first adhesive surface and the second adhesive surface, the adhesive surface side surfaces of the two release liners should satisfy any one of the above-mentioned maximum heights Rz. The maximum height Rz of the side surfaces of the adhesive surfaces of the two release liners may be the same or different.

(Surface properties on the back) The arithmetic average roughness Ra or the maximum height Rz of the back surface (the side opposite to the adhesive layer side) of the release liner (preferably a release film) is not particularly limited. From the viewpoint of productivity and the like, the arithmetic average roughness Ra of the back surface of the release liner may be greater than 30 nm (for example, greater than 35 nm, and further greater than about 50 nm). From the viewpoint of productivity and the like, the maximum height Rz of the back surface of the release liner may be greater than 400 nm (for example, about 500 nm or more), or may be greater than 800 nm (for example, 1000 nm or more).

The arithmetic average roughness Ra and the maximum height Rz of the peeling film surface can be adjusted by the selection of the film material, the forming method, and the surface treatment such as peeling treatment. For example, it is possible to adjust the smoothness of the layer (anti-adhesive layer, hard coat layer, oligomer prevention layer, etc.) constituting the peelable surface, so that the filler particles in the surface layer or the peeling film base material are reduced or not used (no particle化), there are also adjustments to extension conditions and so on.

The arithmetic average roughness Ra and the maximum height Rz of the surface of the release liner (preferably a release film) are measured using a non-contact surface roughness measuring device. The non-contact surface roughness measuring device can be an optical interference surface roughness measuring device, for example, a three-dimensional optical profiler (trade name "NewView 7300", manufactured by ZYGO) or its equivalent can be used. For example, a glass plate (a soda lime glass plate made by Matsunami, thickness 1.3mm) can be attached to the surface of the release liner on the opposite side of the measurement surface with an adhesive and fixed, using a 3D optical profiler (trade name " "NewView7300", manufactured by ZYGO Corporation) The surface shape was measured under an environment of 23°C and 50%RH.

<Use> The adhesive disclosed here (for example, a low-refractive-index adhesive) can be attached to various adherends for use. The constituent material of the above-mentioned adherend (adherent material) is not particularly limited, and examples include copper, silver, gold, iron, tin, palladium, aluminum, nickel, titanium, chromium, indium, zinc, etc., or include them Metal materials such as two or more alloys, or, for example, polyimide resins, acrylic resins, polyether nitrile resins, polyether nitrile resins, polyester resins (PET resins, polyethylene naphthalate resins) Diester resins, etc.), polyvinyl chloride resins, polyphenylene sulfide resins, polyether ether ketone resins, polyamide resins (so-called aramid resins, etc.), polyarylate resins, fluorine Resins, polycarbonate resins, cellulose polymers such as cellulose diacetate or cellulose triacetate, vinyl butyral polymers, liquid crystal polymers, carbon materials such as graphene and other resin materials (typically For plastic materials), aluminum oxide, zirconium oxide, titanium oxide, SiO ₂ , ITO (indium tin oxide), ATO (antimony doped tin oxide) and other metal oxides and their mixtures, aluminum nitride, silicon nitride, nitride Titanium, gallium nitride, indium nitride and other nitrides and their composites, alkali glass, alkali-free glass, quartz glass, borosilicate glass, sapphire glass carbon and other inorganic materials. The adhesive disclosed herein can be used by being attached to a member (such as an optical member) whose surface is at least composed of the above-mentioned materials.

The adhesive disclosed here can be used in the following attachment mode: After being attached to the adherend, it does not need to be heated to a higher temperature than the room temperature range (for example, 20°C~35°C) The attached state. In addition, as permitted by the type of the adherend, etc., the heat treatment may be performed at least at any point after the adherend, the time of the adherence, and before the adherence. The heat treatment can be carried out for the purpose of improving the adhesion of the adhesive to the adherend or promoting adhesion. The heat treatment temperature can be set within the allowable range according to the material of the adhesive sheet or the type of the adherend, and the surface condition of the adherend can be considered to obtain the desired effect. For example, it can be about 100°C or so Below, it may be 80°C or less, 60°C or less, or 50°C or less.

The member or material that is the object of the adhesive can be light transmissive. For the adherend, it is easy to obtain the advantage that the adhesive disclosed here can be of high transparency. The total light transmittance of the adherend can be greater than 50%, or more than 70%, for example. In several ideal situations, the total light transmittance of the adherend is more than 80%, more preferably more than 90%, and more preferably more than 95% (for example, 95-100%). The adhesive disclosed here is suitable for use in a state of being attached to an adherend (for example, an optical member) whose total light transmittance is above a predetermined value. The above-mentioned total light transmittance is measured in accordance with JIS K 7136:2000 using a commercially available transmittance meter. The transmittance meter can use the product name "HAZEMETER HM-150" manufactured by Murakami Color Technology Research Institute or its equivalent.

The refractive index of the adherend and the adhesive layer arranged in contact with the adherend (typically a low-refractive-index adhesive layer, but can also be a high-refractive-index adhesive in the form of a high-refractive-index adhesive layer The refractive index of the layers can be the same or different. For example, by making the refractive index of the adhesive layer relatively high relative to the refractive index of the adherend, the light incident on the adhesive layer from the adherend side at an angle below the critical angle can be refracted on the front side, improving Front brightness. At this time, the refractive index of the adherend can be, for example, 1.55 or less, 1.50 or less, 1.48 or less, or 1.45 or less, or less than 1.45, and for example, it can be 1.10 or more, 1.20 or more, 1.30 or more, or 1.35 or more. In addition, with the adherend having a relatively high refractive index with respect to the adhesive layer, the light incident on the adherend from the adhesive layer side can be refracted on the front side, and the front brightness is improved. At this time, the refractive index of the adherend may be 1.60 or higher, 1.65 or higher, or 1.70 or higher, for example, 3.00 or lower, and 2.50 or lower or 2.00 or lower. On the other hand, by reducing the refractive index difference between the adhesive layer and the adherend, light reflection at the interface can be suppressed. At this time, the refractive index of the adherend can be around 1.55~1.80, around 1.55~1.75, or around 1.60~1.70. The refractive index of the adherend can be measured by the same method as the refractive index of the adhesive.

In several ideal aspects, the adherend may have any of the above refractive indices and any of the above total light transmittances. In optical products (such as light-emitting devices) in which the adherend is attached or laminated with a high-refractive-index adhesive layer and/or a low-refractive-index adhesive layer, it is particularly suitable to take advantage of the technology disclosed here Effect.

The low-refractive-index adhesive layer and the high-refractive-index adhesive layer disclosed herein can be used by attaching them to various adherends in the form of a laminate including them. An example of a preferable application can be an optical application. More specifically, for example, the laminated sheet disclosed herein can be suitably used for optical applications such as applications that can be used for bonding optical members (for optical member bonding) or for manufacturing products (optical products) using the above-mentioned optical members. Adhesive sheet to use. The laminated sheet used in this manner can also be regarded as an interlayer sheet arranged between the layers of the optical laminated body.

The above-mentioned optical member refers to a member having optical properties (for example, polarization, light refraction, light scattering, light reflectivity, light transmittance, light absorption, light diffraction, optical rotation, visibility, etc.). The above-mentioned optical member is not particularly limited as long as it is a member having optical properties. Examples include members constituting devices (optical devices) such as display devices (image display devices) and input devices, or members used in such devices, such as polarized light. Plate, wave plate, phase difference plate, optical compensation film, brightness enhancement film, light guide plate, reflective film, anti-reflection film, hard coating (HC) film, impact absorption film, antifouling film, photochromic film, dimming film , Transparent conductive film (ITO film), design film, decorative film, surface protection board, 稜鏡, lens, color filter, transparent substrate, or further laminated components (these are sometimes collectively referred to as " Functional film") etc. In addition, the above-mentioned "plate" and "film" are set to include plate, film, sheet, etc., respectively. For example, "polarizing film" is set to include "polarizing plate" or "polarizer", etc., and " The “light guide plate” is set to include “light guide film” or “light guide sheet”. In addition, the above-mentioned "polarizing plate" includes a circular polarizing plate.

The above-mentioned display device may include, for example, a liquid crystal display device, an organic EL (electroluminescence) display device, micro LED (µLED), mini LED (mini LED), PDP (plasma display panel), electronic paper, and the like. In addition, the above-mentioned input device may include a touch panel or the like.

The said optical member is not specifically limited, For example, a member (for example, a sheet-shaped, film-shaped, plate-shaped member) etc. which consist of glass, acrylic resin, polycarbonate, polyethylene terephthalate, a metal film, etc. are mentioned. In addition, the "optical member" in this specification is also set to include a member (design film, decorative film, or surface protection film, etc.) that maintains the visibility of the display device or input device while serving as a decoration or protection function.

The low-refractive-index adhesive layer disclosed here (which can be in the form of a laminated sheet with a high- and low-refractive layer), for example, can be configured to have one or more types of light transmission, reflection, diffusion, waveguide, light collection, diffraction, etc. It can be used between functional films or optical films such as fluorescent films and other optical members (which may be other optical films), and can be suitably used for bonding the above-mentioned optical film and the above-mentioned other optical members. Among them, in the bonding of optical films with at least one kind of optical waveguide, condensing, and diffracting functions, the entire bonding layer should preferably have a high refractive index, and the technology that will be disclosed here includes a high refractive index. It is an ideal application object when implemented in the form of a layer (typically a high-refractive-index adhesive layer).

The adhesive layer disclosed here can be suitably used for bonding optical films such as light guide films, diffuser films, fluorescent films, toner films, lenticular films, lenticular films, and microlens array films, for example. Among these applications, from the viewpoint of the trend of miniaturization or higher performance of optical components, thinning or improvement of light extraction efficiency is required. The adhesive layer disclosed here can be suitably used as an adhesive layer that can meet the requirements. In more detail, for example, when bonding a light guide film or a diffusion film, adjusting the refractive index (for example, a higher refractive index) of the adhesive layer as the bonding layer can contribute to thinning. The bonding of the fluorescent film can improve the light extraction efficiency (which can also be regarded as the luminous efficiency) by appropriately adjusting the refractive index difference between the fluorescent light-emitting body and the adhesive. Regarding the bonding of the toning film, by appropriately adjusting the refractive index of the adhesive to reduce the difference in refractive index with the coloring pigment, the scattering component can be reduced and the light transmittance can be improved. In the joining of prisms, lenticular films, microlens array films, etc., by appropriately adjusting the refractive index of the adhesive to control the diffraction of light, it can help improve brightness and/or viewing angle.

The high-refractive-index adhesive layer disclosed herein can be suitably used in the form of a laminated sheet with a low-refractive adhesive layer in the state of being attached to a high-refractive-index adherend (which can be a high-refractive-index layer or member, etc.) It can be used in the same way, and it can suppress the interface reflection with the above-mentioned adherend. The high-refractive-index adhesive layer that can be used in the above-mentioned aspect preferably has a small difference in refractive index from the adherend with a high refractive index and high adhesion at the interface with the adherend. In addition, from the viewpoint of improving the uniformity of appearance, the uniformity of the thickness of the adhesive layer should be high, for example, the surface smoothness of the adhesive surface should be high. When the thickness of the adherend with high refractive index is small (for example, 5µm or less, 4µm or less, or 2µm or less), from the viewpoint of suppressing the coloration or uneven color caused by the interference of reflected light, the reflection at the interface is suppressed One thing is particularly meaningful. As an example of the usage aspect, the following aspect may be mentioned: it can be used in the polarizer with the polarizer, the first retardation layer and the second retardation layer in the polarizing plate with retardation layer in this order. The bonding of the first retardation layer and/or the bonding of the first retardation layer and the second retardation layer.

In addition, the high-refractive-index adhesive layer disclosed herein can be suitably used in the form of being attached to a light-emitting layer such as an optical semiconductor (for example, a high-refractive light-emitting layer mainly composed of an inorganic material). By reducing the refractive index difference between the light-emitting layer and the high-refractive-index adhesive layer, the reflection at these interfaces can be suppressed, and the light extraction efficiency can be improved. In addition, from the viewpoint of preventing the deterioration of the self-luminous element caused by moisture in advance, the water absorption rate of the high-refractive-index adhesive layer is preferably low. From the viewpoint of improving brightness, the high-refractive-index adhesive layer is preferably low-colored. It is also advantageous from the viewpoint of suppressing inadvertent coloration caused by the high refractive index adhesive layer.

The high-refractive-index adhesive layer disclosed here is suitable for use in microlenses and other lens components (such as microlenses constituting a microlens array film or microlenses for cameras) used as constituent components such as cameras or light-emitting devices. As a coating layer covering the lens surface, a bonding layer of a member facing the lens surface (e.g., a member having a surface shape corresponding to the lens surface), a filling layer filled between the lens surface and the member, etc. use. Even if the high refractive index adhesive layer disclosed here is placed against a high refractive index lens (for example, a lens made of a high refractive index resin, or a lens with a surface layer made of a high refractive index resin), it can still reduce and The refractive index difference of the lens. This is advantageous from the viewpoint of the thickness reduction of the above-mentioned lens and the product provided with the lens, and can also help suppress aberrations or increase the Abbe number. In the technique disclosed herein, the adhesive (viscoelastic material) constituting the high-refractive-index adhesive layer can also be used as a lens resin in the form of filling the recesses or voids of an appropriate transparent member, for example.

Use the adhesive layer disclosed here (a high refractive index adhesive layer and/or a low refractive index adhesive layer, and preferably a low refractive index adhesive layer that can also be laminated on a high refractive index layer) to bond optical components The aspect is not particularly limited. For example, it may be the following aspects: (1) the aspect in which the optical members are bonded to each other through the adhesive layer disclosed here; or (2) the optical member is bonded through the adhesive layer disclosed here The state of bonding to a member other than the optical member; (3) The adhesive layer disclosed here is in the form of an adhesive sheet including an optical member, and the adhesive sheet is bonded to the optical member or a member other than the optical member The state. In addition, in the aspect (3) above, the adhesive sheet in the form of the optical member may be, for example, an adhesive sheet in which the support is an optical member (for example, an optical film). As described above, the adhesive sheet including the optical member as a support can also be regarded as an adhesive optical member (for example, an adhesive optical film). In addition, when the adhesive layer disclosed here constitutes an adhesive sheet of the type with a support and the functional film is used as the support, the adhesive sheet can also be regarded as having the one disclosed here on at least one side of the functional film The "adhesive functional film" of the adhesive layer.

From the foregoing, according to the technology disclosed herein, an optical laminate including the adhesive layer disclosed herein and a member to which the adhesive sheet is attached (for example, a resin film such as an optical film) is provided. The member to which the adhesive layer can be attached may have the refractive index of the above-mentioned adherend material. In addition, the difference between the refractive index of the adhesive layer and the refractive index of the member (refractive index difference) may be the refractive index difference between the adherend and the adhesive layer. Regarding the members constituting the laminated body, the above-mentioned members, materials, and adherends are described, so the description will not be repeated.

As can be understood from the above description and the following examples, the following matters are included in the matters disclosed in this specification.

[101] An adhesive containing acrylic polymer (F), and the acrylic polymer (F) contains a fluorine-containing acrylic monomer (M1) as a monomer unit; the refractive index of the adhesive is 1.46 Below, and its storage elastic modulus G'at 25° C. is 1.0 kPa or more and 400 kPa or less. [102] The adhesive of the above-mentioned [101], wherein the content of the fluorine-containing acrylic monomer (M1) in the monomer components constituting the acrylic polymer (F) is 25% by weight or more. [103] The adhesive of [101] or [102] above, wherein the fluorine-containing acrylic monomer (M1) contains a fluorine atom-containing alkyl (meth)acrylate. [104] The adhesive according to any one of [101] to [103] above, wherein the acrylic polymer (F) contains a hydroxyl-containing monomer as a monomer unit. [105] A laminated sheet, comprising: a low-refractive-index adhesive layer formed by the adhesive of any one of the aforementioned [101] to [104]; and a high-refractive-index adhesive layer laminated on the aforementioned low-refractive adhesive layer Agent layer. [106] The laminated sheet of the above-mentioned [105], wherein the ratio of the refractive index n ₁ of the high refractive index adhesive layer to the refractive index n ₂ of the low refractive index adhesive layer (n ₁ /n ₂ ) is 1.02 or more . [107] The laminated sheet of [105] or [106] above, wherein the refractive index n _{1 of} the high refractive index adhesive layer is greater than 1.570. [108] The laminated sheet according to any one of the above [105] to [107], wherein the storage elastic modulus G'of the high refractive index adhesive layer at 25° C. is 700 kPa or less. [109] The laminated sheet of any one of [105] to [108] above has a total light transmittance of 86% or more, and a haze value of 3.0% or less. [110] A light-emitting device comprising: a self-luminous element and the laminated sheet as described in any one of [105] to [109] above; and the laminated sheet is arranged on a side that is more visible than the self-luminous element.

[1] An adhesive sheet comprising an adhesive layer; and It has an adhesive surface formed by the above-mentioned adhesive layer; The above-mentioned adhesive layer has a refractive index greater than 1.570, a total light transmittance of 86% or more, and a haze value of 3.0% or less. [2] The adhesive sheet of [1] above, wherein the thickness of the adhesive layer is 5 µm or more. [3] The adhesive sheet of [1] or [2] above, the peeling strength (adhesion) to the glass plate is 3N/25mm or more. [4] The adhesive sheet according to any one of [1] to [3] above, wherein the arithmetic average roughness Ra of the adhesive surface is 100 nm or less. [5] The adhesive sheet according to any one of [1] to [4] above, wherein the water absorption rate of the adhesive layer is 1.0% or less. [6] The adhesive sheet according to any one of [1] to [5] above, which is constituted in the form of a laminate including the adhesive layer and the light-transmitting substrate. [7] The adhesive sheet of the above [6], wherein the light-transmitting substrate is a resin film. [8] The adhesive sheet according to any one of [1] to [5] above, which is a double-sided adhesive adhesive sheet composed of the above-mentioned adhesive layer. [9] An adhesive sheet with a release liner, including: Adhesive sheets as in any one of [1]~[8] above; and A release liner arranged on the adhesive surface of the above-mentioned adhesive sheet. [10] An adhesive composition used to form the adhesive layer of the adhesive sheet of any one of [1] to [8] above.

[11] An adhesive composition comprising: an acrylic polymer (A), which contains an aromatic ring-containing monomer (m1) as a monomer unit; and an additive (H _RO ) whose refractive index is higher than that of the acrylic polymer (A) Higher organic materials. [12] The adhesive composition of the above [11], wherein _{the refractive index of the additive (H RO} ) is 1.60 or more. [13] The adhesive composition of the above [11] or [12], wherein the content of the additive (H _RO ) relative to 100 parts by weight of the acrylic polymer (A) is greater than 0 parts by weight and less than 60 parts by weight . [14] The adhesive composition according to any one of the above [11] to [13], wherein the additive (H _RO ) comprises at least one selected from the group consisting of aromatic ring-containing compounds and heterocyclic-containing compounds 1 kind of compound. [15] The adhesive composition according to any one of [11] to [14] above, wherein the additive (H _RO ) comprises a compound having two or more aromatic rings in one molecule. [16] The adhesive composition of the above-mentioned [15], wherein the additive (H _RO ) contains a compound satisfying at least one of the following as the compound having two or more aromatic rings in one molecule: (i) contains two A structure in which non-condensed aromatic rings are directly chemically bonded; and (ii) a structure in which two aromatic rings have been condensed. [17] The adhesive composition according to any one of the above [11] to [16], wherein in the monomer components constituting the acrylic polymer (A), the content of the aromatic ring-containing monomer (m1) is More than 50% by weight. [18] The adhesive composition of any one of the above [11] to [17], wherein in the monomer components constituting the acrylic polymer (A), the content of the aromatic ring-containing monomer (m1) is greater than 70% by weight and less than 100% by weight, and more than 50% by weight of the above-mentioned aromatic ring-containing monomer (m1) is a monomer whose homopolymer has a glass transition temperature below 10°C. [19] The adhesive composition of any one of [11] to [18] above, wherein the monomer component constituting the acrylic polymer (A) further contains a monomer (m2), and the monomer (m2) It has at least one of a hydroxyl group and a carboxyl group. [20] The adhesive composition according to any one of [11] to [18] above is used to form the adhesive layer of the adhesive sheet according to any one of [1] to [8] above. [21] An adhesive, which is formed of the adhesive composition of any one of [11] to [20] above, and has a refractive index higher than 1.570. [22] An adhesive sheet comprising an adhesive layer composed of an adhesive, and the adhesive is formed of the adhesive composition of any one of [11] to [20] above. [23] The adhesive sheet of [22] above, wherein the haze value of the adhesive layer is 1.0% or less.

[24] An interlayer sheet, which is arranged between the layers of the laminate for optical purposes; and includes a _{viscoelastic layer V 1 with a refractive index n 1} of 1.570 or more, and satisfies: the total light transmittance is 86% or more ; The haze value is below 1.0%; and the storage elastic modulus G'at 25℃ is 30kPa~700kPa. [25] The interlayer sheet as in [24] above has a thickness of 5 µm or more. [26] The interlayer sheet of the above [24] or [25], wherein the viscoelastic layer V ₁ comprises a main polymer and a plasticized material with a lower molecular weight than the main polymer. [27] The interlayer sheet of the above [26], wherein the weight average molecular weight of the plasticized material is 30,000 or less. [28] The interlayer sheet according to any one of [24] to [27] above, which further comprises a viscoelastic layer V _{2 laminated on the viscoelastic layer V 1} , and the viscoelastic layer V _{2 is} at 25° C. storage elastic modulus G _'V2 viscoelastic layer is less than the V ₁ stored at 25 deg.] C of the elastic modulus G' _V1. [29] As the inter [28] of the plies, wherein the refractive index of the viscoelastic layer of V ₂ n ₂ is less than the refractive index of the viscoelastic layer V ₁ n _1. [30] The interlayer sheet of any one of [24] to [29] above, wherein the viscoelastic layer V ₁ is a layer formed of the adhesive composition of any one of [11] to [18] above . [31] The interlayer sheet of any one of [24] to [29] above, wherein the viscoelastic layer V ₁ is the adhesive layer in the adhesive sheet of any one of [1] to [5]. [32] An optical laminate, comprising: an interlayer sheet as described in any one of [24] to [31] above, and a resin film laminated on the interlayer sheet. [33] An interlayer sheet with a release liner, comprising: the interlayer sheet of any one of [24] to [31] above, and a release liner covering at least one surface of the interlayer sheet.

[34] A light-emitting device, comprising: a self-luminous element; a low-refractive-index layer disposed on the side of the visible side of the self-luminous element; and a high-refractive-index adhesive layer which is laminated in direct contact with the low-refractive index layer _{; The refractive index n 1 of} the high refractive index adhesive layer is greater than 1.570, the total light transmittance is 86% or more, and the haze value is 3.0% or less. [35] As the above-mentioned [34] The light-emitting device, wherein the refractive index of the high refractive index layer of the adhesive agent and said refractive index n ₁ of the low refractive index layer ₂ ratio (n ₁ / n ₂₎ is 1.05 or more n. [36] The light-emitting device of [35] or [36], wherein the arithmetic average roughness Ra of the surface of the high refractive index adhesive layer is 100 nm or less. [37] As the above-mentioned [34] - [36] the light emitting device of any one of, wherein the thickness of the high refractive index layer of _an adhesive agent with a thickness ratio of the low refractive index layer is a T T ₂ (T ₁ / T ₂ ) Is 0.5~5. [38] The light-emitting device according to any one of [34] to [37], wherein the thickness T ₁ of the high refractive index adhesive layer is 5 μm or more. [39] The light-emitting device according to any one of the above [34] to [38], wherein the total light transmittance of the laminated sheet composed of the high refractive index adhesive layer and the low refractive index layer is 86% or more, and The haze value is 3.0% or less. [40] The light-emitting device according to any one of the above [34] to [39], wherein the high refractive index adhesive layer is formed of the adhesive composition according to any one of the above [11] to [18]的层。 The layer. [41] The light-emitting device according to any one of [34] to [40], wherein the high refractive index adhesive layer is the adhesive layer in the adhesive sheet of any one of [1] to [5] . [42] The light-emitting device according to any one of the above [34] to [41], wherein the low refractive index layer is a layer composed of the adhesive according to any one of the above [101] to [104]. [43] The interlayer sheet according to any one of the above [24] to [31], wherein the viscoelastic layer V ₂ is a layer composed of the adhesive of any one of the above [101] to [104] .

Example Hereinafter, several experiments related to the present invention will be explained. In addition, in the following description, "parts" and "%" indicating the amount or content of use are based on weight unless otherwise specified.

＜Preparation of adhesive composition C1＞ In a four-necked flask equipped with a stirring blade, a thermometer, a nitrogen introduction tube, and a cooler, 1H, 1H, 2H, 2H-tridecafluorooctyl acrylate (manufactured by Osaka Organic Chemical Industry Co., Ltd., Trade name "Viscoat 13F") 99.0 parts, 4-hydroxybutyl acrylate (4HBA) 1.0 part, 2,2'-azobisisobutyronitrile (AIBN) as a polymerization initiator 0.2 part, and ethyl acetate as a polymerization solvent 200 parts of ester, nitrogen was introduced while slowly stirring, and the liquid temperature in the flask was maintained at around 60° C. to perform polymerization reaction for 9 hours to prepare a solution (33%) of acrylic polymer P1. The polymerization average molecular weight (Mw) of the acrylic polymer P1 was 800,000. The solution (33%) of the above acrylic polymer P1 was diluted to 30% with ethyl acetate, and the trimerization of hexamethylene diisocyanate as a crosslinking agent was added to 100 parts of non-volatile components (solid content) An isocyanate body (manufactured by Tosoh, brand name "Coronate HX", trifunctional isocyanate compound) in 10 parts of 1% ethyl acetate solution (0.1 part of non-volatile components) was stirred and mixed to prepare an adhesive composition C1.

＜Preparation of adhesive composition C2~C10＞ Except that the composition of the monomer components was changed as shown in Table 1, the acrylic polymer P2 to P10 solution was prepared in the same manner as the preparation of the acrylic polymer P1 solution. Except that the solutions of acrylic polymers P2 to P10 were used instead of the solutions of acrylic polymer P1, the adhesive compositions C2 to C10 were prepared in the same manner as the preparation of the adhesive composition C1.

In addition, in the composition of the monomer components shown in Table 1, "V13F" means 1H, 1H, 2H, 2H-tridecafluorooctyl acrylate (manufactured by Osaka Organic Chemical Industry Co., Ltd., trade name "Viscoat 13F"), " "V8F" means 1H,1H,5H-octafluoropentyl acrylate (manufactured by Osaka Organic Chemical Industry Co., Ltd., trade name "Viscoat 8F"), "V3F" means 2,2,2-trifluoroethyl acrylate (Osaka The brand name "Viscoat 3F" manufactured by Organic Chemical Industry Co., Ltd.). In addition, 2EHA represents 2-ethylhexyl acrylate, NVP represents N-vinyl-2-pyrrolidone, IBXA represents isobornyl acrylate, and CHA represents cyclohexyl acrylate.

＜Making of Adhesive Sheet (1)＞ (example 1) Coat the adhesive composition C1 prepared above on the silicone-treated surface of a polyethylene terephthalate (PET) film R1 (thickness 50µm) treated with silicone on one side, at 130°C Heat for 2 minutes to form an adhesive layer with a thickness of 25 µm. A silicone-treated surface of PET film R2 (thickness: 38µm) treated with silicone on one side was attached to the surface of the above-mentioned adhesive layer. In the above manner, an adhesive layer (a double-sided adhesive sheet without a substrate) in a form where both sides are protected by the PET film (release liner) R1 and R2 is obtained. In addition, compared with the release liner R1, the release liner R2 is relatively lightly peelable.

(Example 2~10) Except that the adhesive compositions C2 to C10 were used instead of the adhesive composition C1, the adhesive layers of Examples 2 to 10 (double-sided adhesive sheets without substrate) were produced in the same manner as in Example 1.

After fully adapting the obtained adhesive sheet to an environment of 23°C and 50%RH, it is used for the following measurement and evaluation.

＜Measurement and evaluation (1)＞ (Refractive index) For each adhesive layer, the refractive index was measured using an Abbe refractometer (manufactured by ATAGO CO., LTD., model "DR-M4") under the conditions of a measurement wavelength of 589 nm and a measurement temperature of 25°C. The results are listed in Table 1.

(Storage elastic modulus G') The laminated layers of each adhesive were made to have a thickness of approximately 1.5 mm, which was used as a sample for measurement. Using ARES manufactured by TA Instruments, the dynamic viscoelasticity measurement was performed under the following conditions. Read the storage elastic modulus G'at 25°C from the measurement result. The results are listed in Table 1. [Measurement conditions] Deformation mode: twist Measurement frequency: 1Hz Heating rate: 5°C/min Shape: parallel plate 7.9mmφ

(Total light transmittance and haze value) Use the test piece in which the adhesive sheets of each example are pasted on alkali-free glass (thickness 0.8~1.0mm, total light transmittance 92%, haze 0.4%), with a haze meter (manufactured by Murakami Color Research Institute, The product name is "HAZEMETER HM-150"), and the total light transmittance and haze of the above test piece are measured under a measurement environment at 23°C. The value obtained by subtracting the total light transmittance and haze of the above-mentioned alkali-free glass from the measured value is used as the total light transmittance and haze value of the adhesive sheet. The results are listed in Table 1.

(Peel strength to glass plate) Under a measurement environment of 23°C and 50%RH, peel off the release liner from one side of the adhesive sheet of each example, and laminate a PET film with a thickness of 50μm to make the substrate, and then cut it into a size of 25mm in width and 100mm in length. Test piece. The release liner on the other side was peeled off from the test piece, and a 2 kg roller was applied to the surface of an alkali glass plate (manufactured by Matsunami Glass Industry Co., Ltd., thickness 1.35 mm, green plate frosted product) as a to-be-adhered body to perform 1 reciprocating pressure bonding. Place it in this environment for 30 minutes, then put it into a pressure degassing device (autoclave), perform autoclave treatment at a temperature of 50°C and a pressure of 0.5MPa for 30 minutes, and then heat it at 23°C and 50%RH. After being placed in a gas environment for 24 hours, use a universal tensile and compression testing machine, in accordance with JIS Z 0237: 2000, and measure the peel strength (adhesion) at a tensile speed of 300 mm/min and a peeling angle of 180 degrees [N/25mm] . The universal tensile and compression testing machine uses Minebea's "Tensile and Compression Testing Machine, TG-1kN".

[Table 1]

As shown in Table 1, the adhesive sheets of Examples 1-9 all have a refractive index of 1.46 or less, and a storage elastic modulus G'(25) of 400kPa. These adhesive sheets exhibit high transparency and exhibit practical peel strength suitable for the bonding of optical components.

＜Preparation of adhesive composition C11＞ In a four-necked flask equipped with a stirring blade, a thermometer, a nitrogen introduction tube, and a cooler, 65 parts of 2EHA, 1H,1H,5H-octafluoropentyl acrylate (manufactured by Osaka Organic Chemical Industry Co., Ltd. , Trade name: Viscoat 8F) 30 parts, N-vinyl-2-pyrrolidone (NVP, manufactured by Nippon Shokubai) 3 parts and 4HBA 2 parts, AIBN 0.2 parts as polymerization initiator and ethyl acetate as polymerization solvent 200 parts of ester, nitrogen was introduced while slowly stirring, and the liquid temperature in the flask was kept at around 60°C for 9 hours to perform polymerization reaction to prepare a solution (33%) of acrylic polymer P11. The polymerization average molecular weight (Mw) of the acrylic polymer P11 was 550,000. The solution (33%) of the above acrylic polymer P11 is diluted to 30% with ethyl acetate, and the trimerization of hexamethylene diisocyanate as a crosslinking agent is added to 100 parts of non-volatile components (solid content) 10 parts of 1% ethyl acetate solution (0.1 part of non-volatile component) of isocyanate body (manufactured by Tosoh, trade name "Coronate HX", trifunctional isocyanate compound) was stirred and mixed to prepare adhesive composition C11.

<Preparation of adhesive composition C12> In a four-necked flask equipped with a stirring blade, a thermometer, a nitrogen introduction tube, and a cooler, feed the phenoxybenzyl acrylate between the monomer components (Kyoeisha Chemical Co., Ltd.) Manufacture, trade name "LIGHT ACRYLATE POB-A", refractive index: 1.566, homopolymer Tg: -35°C; hereinafter referred to as "POB-A") 95 parts and 4HBA 5 parts, AIBN 0.2 as a polymerization initiator Part and 100 parts of toluene as a polymerization solvent, introduce nitrogen while slowly stirring, and keep the liquid temperature in the flask at around 60°C for 6 hours to perform polymerization reaction to prepare a solution of acrylic polymer P12 (50%) . The polymerization average molecular weight (Mw) of the acrylic polymer P12 was 500,000. In the acrylic polymer P12, the Tg (that is, Tg _T ) based on the composition of the monomer components is -35°C, and the Tg (that is, Tg _m1 ) based on the composition of the aromatic ring-containing monomer is -35°C. Dilute the above acrylic polymer P12 solution (50%) with ethyl acetate to 30%, and add hexamethylene diisocyanate as a crosslinking agent to 334 parts of the solution (100 parts of non-volatile components). 10 parts of 1% ethyl acetate solution of polyisocyanate (manufactured by Tosoh, trade name "Coronate HX", trifunctional isocyanate compound) (0.1 part of non-volatile content), 2 parts of acetone as a crosslinking retarder, as 1 part of 1% ethyl acetate solution of acetone iron (III) of crosslinking catalyst (0.01 part of non-volatile content) was stirred and mixed to prepare adhesive composition C12.

＜Preparation of adhesive composition C13＞ Into a four-necked flask equipped with a stirring blade, a thermometer, a nitrogen introduction tube, and a cooler, 72 parts of POB-A as a monomer component, 1-naphthyl methacrylate (manufactured by Kyoeisha Chemical Co., Ltd., product Name "LIGHT ACRYLATE NMT-A", refractive index: 1.595, homopolymer Tg: 31°C; hereinafter referred to as "NMT-A") 23 parts and 4HBA 5 parts, AIBN 0.2 parts as polymerization initiator, and as For 100 parts of toluene as the polymerization solvent, nitrogen was introduced while stirring slowly, and the liquid temperature in the flask was maintained at around 60°C for 6 hours of polymerization to prepare a solution (50%) of acrylic polymer P13. The polymerization average molecular weight (Mw) of the acrylic polymer P13 was 500,000. Put 20 parts of POB-A as monomer components, 80 parts of NMT-A and 0.2 parts of AIBN as polymerization initiator in a separable flask equipped with a thermometer, agitator, reflux cooling tube and nitrogen introduction tube, as a chain transfer After 3.5 parts of α-thioglycerin and 67 parts of methyl ethyl ketone of the agent, nitrogen was introduced, and nitrogen substitution was performed for about 1 hour while stirring. Then, the flask was heated to 70°C and allowed to react for 12 hours, and then an acrylic oligomer (oligomer B) having a weight average molecular weight (Mw) of 4000 and a refractive index of 1.63 was obtained. Dilute the solution (50%) of the above acrylic polymer C13 with ethyl acetate to 30%, and add 20 parts of the oligomer B prepared above to 334 parts of the solution (100 parts of non-volatile components) as a crossover The linking agent is a trimeric isocyanate body of hexamethylene diisocyanate (manufactured by Tosoh, trade name "Coronate HX", trifunctional isocyanate compound) in 1% ethyl acetate solution 10 parts (non-volatile component 0.1 part), as a cross-linking agent 2 parts of acetone acetone as a linking retarder, 1 part of 1% ethyl acetate solution of iron (III) acetone as a cross-linking catalyst (0.01 parts of non-volatile components) and mixed to prepare the adhesive composition C13 .

＜Making of Adhesive Sheet (2)＞ (Example 11) The adhesive composition C11 prepared above was coated on the silicone-treated surface of the release liner R1 (thickness 50µm), and heated at 130°C for 2 minutes to form an adhesive layer with a thickness of 10µm. Paste the silicone-treated surface of the release liner R2 (thickness 38µm) on the surface of the above-mentioned adhesive layer. In the above manner, an adhesive layer (a double-sided adhesive sheet without a substrate) formed of the adhesive composition C11 with both sides protected by the PET film (release liner) R1 and R2 is obtained.

(Example 12) The adhesive composition C12 prepared above was coated on the silicone-treated surface of the release liner R1 and heated at 130°C for 2 minutes to form an adhesive layer with a thickness of 25 µm. Paste the silicone-treated surface of the release liner R2 on the surface of the adhesive layer. In the above manner, an adhesive layer (a double-sided adhesive sheet without a substrate) formed of the adhesive composition C12 with both sides protected by the PET film (release liner) R1 and R2 is obtained. The release liner R2 was peeled off from the obtained adhesive layer and the adhesive layer produced in Example 11, and the adhesive surfaces were attached to each other, and they were crimped with a hand ink roller. The laminate was subjected to autoclave treatment under conditions of 50°C and 0.60 MPa for 30 minutes, and then aged in an environment of 50°C for 48 hours. In the above manner, a two-layer structure of adhesive layer (high refractive index adhesive layer) formed by adhesive composition C12/adhesive layer (low refractive index adhesive layer) formed by adhesive composition C11 is obtained The laminated sheet (double-sided adhesive sheet without base material) is constructed. The surface of the adhesive sheet is protected by two release liners R1.

(Example 13) Except that the type of adhesive composition used to form each adhesive layer and the thickness of each adhesive layer were changed as shown in Table 2, the same method as in Example 12 was used to obtain a high-refractive-index adhesive layer/low-refractive index A laminated sheet composed of a two-layer structure of the adhesive layer (a double-sided adhesive sheet without a substrate).

(Examples 14, 15) In the same manner as in Example 13, an adhesive layer composed of adhesive compositions C12 and C13 and having a single-layer structure having the thickness shown in Table 2 was produced as the adhesive sheets of Examples 14 and 15.

＜Measurement and evaluation (2)＞ After fully adapting the adhesive sheets obtained in Examples 11 to 15 to an environment of 23°C and 50% RH, the measurement and evaluation of each item were performed in the same manner as in the above-mentioned "Measurement and Evaluation (1)". In a double-sided adhesive sheet without a substrate composed of a two-layer structure of a high-refractive-index adhesive layer/low-refractive-index adhesive layer, the peel strength of the high-refractive-index adhesive layer side was measured. The results are listed in Table 2.

[Table 2]

As shown in Table 2, the adhesive sheets of Examples 11 to 13 include an adhesive layer with a refractive index of 1.46 or less, and exhibit high transparency in the adhesive sheet. These adhesive sheets exhibit practical peel strength suitable for the bonding of optical components.

＜Evaluation of the effect of improving the front brightness＞ Attach the adhesive sheets of each of Examples 11 to 15 on the white LED light source. After the light source is turned on for more than 30 minutes to stabilize in a darkroom environment, use the spectroradiometer SR-UL1R (manufactured by TOPCON TECHNOHOUSE Co., Ltd.) Measure the front brightness of the part where the adhesive sheet is attached. Using the average value of the brightness measured 3 times, the brightness improvement effect of the light source without the adhesive sheet is evaluated as G (good), and the brightness improvement less than 10% is evaluated as P (poor) ). The results are listed in Table 3.

[table 3]

As shown in Table 3, it is based on a laminated structure formed by combining an adhesive layer with a low refractive index formed by an adhesive composition C11 and an adhesive layer with a high refractive index formed by an adhesive composition C12 or C13 For the adhesive sheets (laminated sheets) of Examples 12 and 13 of the adhesive layer, compared with the case where the adhesive sheet was not used, it was confirmed that more than 10% of the frontal brightness improvement effect was confirmed. In the adhesive sheets of Examples 11, 14, and 15 where the adhesive layer has a single-layer structure, the frontal brightness enhancement effect brought by the adhesive sheet alone was not confirmed.

＜Preparation of adhesive composition C14＞ Into a four-necked flask equipped with a stirring blade, thermometer, nitrogen introduction tube and cooler, feed 79 parts of POB-A as monomer components, 20 parts of n-butyl acrylate, 1 part of 4HBA, and AIBN 0.2 as polymerization initiator Part and 100 parts of toluene as a polymerization solvent. While slowly stirring, nitrogen was introduced, and the liquid temperature in the flask was kept at around 60°C for 6 hours polymerization reaction to prepare a solution of acrylic polymer P14 (50%) . The Mw of the acrylic polymer P14 was 520,000. Dilute the above acrylic polymer P14 solution (50%) with ethyl acetate to 30%, and add 1% ethyl acetate of Coronate HX as a crosslinking agent to 334 parts of the solution (100 parts of non-volatile components) 10 parts of solution (0.1 part of non-volatile content), 2 parts of acetone as a crosslinking retarder, 1 part of 1% ethyl acetate solution of acetone iron (III) as a crosslinking catalyst (non-volatile content of 0.01 Parts) and stirred and mixed to prepare adhesive composition C14.

＜Preparation of adhesive composition C15＞ Except that the composition (weight ratio) of the monomer components is changed to POB-A/ethyl carbitol acrylate (CBA)/4HBA=79/20/1, it is the same as the preparation of the acrylic polymer P14 solution Method to prepare a solution (50%) of acrylic polymer P15. The Mw of the acrylic polymer P15 was 460,000. Except that the solution of acrylic polymer P15 was used instead of the solution of acrylic polymer P14, the adhesive composition C15 was prepared in the same manner as the preparation of the adhesive composition C14.

<Preparation of adhesive composition C16> Except that the composition (weight ratio) of the monomer components was changed to P2H-A/4HBA=99/1, it was prepared in the same manner as the preparation of the acrylic polymer P14 solution Acrylic polymer P16 solution (50%). "P2H-A" in the composition of the above monomer components means phenoxy diethylene glycol acrylate (manufactured by Kyoeisha Chemical Co., Ltd., trade name "LIGHT ACRYLATE P2H-A", refractive index: 1.510, homopolymer Tg: -35°C). The Mw of the acrylic polymer P16 was 1 million. Dilute the acrylic polymer P16 solution (50%) with ethyl acetate to 30%, and add 6-ethyl acrylate _{as an additive (H RO) to 334 parts of the solution (100 parts of non-volatile components)} Dinaphtho[2,1-b:1',2'-d]thiophene (6-propenoxyethyl dinaphthothiophene manufactured by SUGAI Chemical Industry Co., Ltd., code name: 6EDNTA, refractive index: 1.722) 20 10 parts of 1% ethyl acetate solution of Coronaate HX as a crosslinking agent (0.1 part of non-volatile content), 2 parts of acetone as a crosslinking retarder, iron (III) acetone as a crosslinking catalyst 1 part of 1% ethyl acetate solution (0.01 part of non-volatile content) of) and stir and mix to prepare adhesive composition C16.

＜Making of Adhesive Sheet＞ (Example 16~18) Except that the type of adhesive composition used to form each adhesive layer and the thickness of each adhesive layer are shown in Table 4, a high-refractive-index adhesive layer/low-refractive-index adhesive was obtained in the same manner as in Example 12 A laminated sheet composed of a two-layer structure of the agent layer (a double-sided adhesive sheet without a substrate). In addition, the Mw of the acrylic polymer P4 of the base polymer of the adhesive composition C4 was 550,000.

＜Measurement and evaluation (3)＞ After fully adapting the adhesive sheets obtained in Examples 16 to 18 to an environment of 23°C and 50% RH, the measurement and evaluation of each item were carried out in the same manner as the above-mentioned "Measurement and Evaluation (2)". The results are listed in Table 4.

[Table 4]

As shown in Table 4, an adhesive layer with a low refractive index formed by the adhesive composition C4 and an adhesive layer with a refractive index higher than the low refractive index adhesive layer by 0.01 or more (more specifically, 0.10 or more) The laminated sheets of Examples 16 to 18 of the laminated structure all showed high transparency. These adhesive sheets exhibit practical peel strength suitable for the bonding of optical components.

The specific examples of the present invention have been described in detail above, but these are only examples and do not limit the scope of the patent application. The technology described in the scope of the patent application includes various modifications and changes to the specific examples illustrated above.

1: Adhesive sheet 2: Adhesive sheet (laminated sheet) 10: Adhesive layer 10A: The first surface (the first adhesive surface) 10B: The second surface (the second adhesive surface) 11: The first adhesive layer (high refractive index adhesive layer) 12: The second adhesive layer (low refractive index adhesive layer) 20: Support substrate 20A: Surface 1 (non-peelable surface) 20B: Side 2 30: Peel off the liner 31, 32: Release the liner 50: Adhesive sheet with release liner 70: Self-luminous element 80: Covering window components 100: Light-emitting device

Fig. 1 is a cross-sectional view schematically showing the structure of an adhesive sheet according to an embodiment. Fig. 2 is a cross-sectional view schematically showing the structure of a laminated sheet according to an embodiment. Fig. 3 is a cross-sectional view schematically showing the structure of a light-emitting device according to an embodiment.

1: Adhesive sheet

10: Adhesive layer

10A: The first surface (the first adhesive surface)

10B: The second surface (the second adhesive surface)

20: Support substrate

20A: Surface 1 (non-peelable surface)

20B: Side 2

30: Peel off the liner

50: Adhesive sheet with release liner

Claims (10)

An adhesive containing acrylic polymer (F), and the acrylic polymer (F) contains fluorine-containing acrylic monomer (M1) as a monomer unit; The refractive index of the adhesive is below 1.46, and Its storage elastic modulus G'at 25°C is above 1.0 kPa and below 400 kPa. The adhesive of claim 1, wherein, in the monomer components constituting the acrylic polymer (F), the content of the fluorine-containing acrylic monomer (M1) is 25% by weight or more. The adhesive of claim 1 or 2, wherein the aforementioned fluorine-containing acrylic monomer (M1) contains a fluorine atom-containing alkyl (meth)acrylate. The adhesive according to any one of claims 1 to 3, wherein the aforementioned acrylic polymer (F) contains a hydroxyl-containing monomer as a monomer unit. A multi-layered piece that contains: A low refractive index adhesive layer formed by the adhesive according to any one of claims 1 to 4; and The high-refractive-index adhesive layer laminated on the aforementioned low-refractive adhesive layer. The laminated sheet according to claim 5, wherein the ratio of the refractive index n ₁ of the high refractive index adhesive layer to the refractive index n ₂ of the _{low refractive index adhesive layer (n 1} /n ₂ ) is 1.02 or more. The laminated sheet according to claim 5 or 6, wherein the refractive index n _{1 of the} aforementioned high refractive index adhesive layer is greater than 1.570. The laminated sheet according to any one of claims 5 to 7, wherein the storage elastic modulus G'of the aforementioned high refractive index adhesive layer at 25° C. is 700 kPa or less. For example, the laminated sheet of any one of Claims 5 to 8 has a total light transmittance of 86% or more, and a haze value of 3.0% or less. A light-emitting device comprising: a self-luminous element and a laminated sheet as claimed in any one of claims 5 to 9; and, The above-mentioned laminated sheet is arranged on the visual side more than the above-mentioned self-luminous element.

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