WO2022270556A1 - 光学積層体の製造方法および光学積層体 - Google Patents

光学積層体の製造方法および光学積層体 Download PDF

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Publication number
WO2022270556A1
WO2022270556A1 PCT/JP2022/024974 JP2022024974W WO2022270556A1 WO 2022270556 A1 WO2022270556 A1 WO 2022270556A1 JP 2022024974 W JP2022024974 W JP 2022024974W WO 2022270556 A1 WO2022270556 A1 WO 2022270556A1
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Prior art keywords
adhesive layer
adhesive
less
optical sheet
main surface
Prior art date
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Ceased
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PCT/JP2022/024974
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English (en)
French (fr)
Japanese (ja)
Inventor
峻哉 若山
繁嘉 桐部
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Nitto Denko Corp
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Nitto Denko Corp
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Priority to KR1020237036893A priority Critical patent/KR20240024042A/ko
Priority to JP2023530103A priority patent/JPWO2022270556A1/ja
Priority to CN202280031935.9A priority patent/CN117242150A/zh
Publication of WO2022270556A1 publication Critical patent/WO2022270556A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/12—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by using adhesives
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B3/00—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form
    • B32B3/26—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by a particular shape of the outline of the cross-section of a continuous layer; characterised by a layer with cavities or internal voids ; characterised by an apertured layer
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B3/00—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form
    • B32B3/26—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by a particular shape of the outline of the cross-section of a continuous layer; characterised by a layer with cavities or internal voids ; characterised by an apertured layer
    • B32B3/30—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by a particular shape of the outline of the cross-section of a continuous layer; characterised by a layer with cavities or internal voids ; characterised by an apertured layer characterised by a layer formed with recesses or projections, e.g. hollows, grooves, protuberances, ribs
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/10—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the pressing technique, e.g. using action of vacuum or fluid pressure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/06—Non-macromolecular additives organic
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J133/00—Adhesives based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by only one carboxyl radical, or of salts, anhydrides, esters, amides, imides, or nitriles thereof; Adhesives based on derivatives of such polymers
    • C09J133/04—Homopolymers or copolymers of esters
    • C09J133/14—Homopolymers or copolymers of esters of esters containing halogen, nitrogen, sulfur or oxygen atoms in addition to the carboxy oxygen
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J167/00—Adhesives based on polyesters obtained by reactions forming a carboxylic ester link in the main chain; Adhesives based on derivatives of such polymers
    • C09J167/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J201/00—Adhesives based on unspecified macromolecular compounds
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J5/00—Adhesive processes in general; Adhesive processes not provided for elsewhere, e.g. relating to primers
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00—Adhesives in the form of films or foils
    • C09J7/30—Adhesives in the form of films or foils characterised by the adhesive composition
    • C09J7/38—Pressure-sensitive adhesives [PSA]
    • G—PHYSICS
    • G02—OPTICS
    • G02B—OPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B5/00—Optical elements other than lenses
    • G—PHYSICS
    • G02—OPTICS
    • G02B—OPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B5/00—Optical elements other than lenses
    • G02B5/02—Diffusing elements; Afocal elements
    • G—PHYSICS
    • G02—OPTICS
    • G02B—OPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B7/00—Mountings, adjusting means, or light-tight connections, for optical elements
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/12—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by using adhesives
    • B32B2037/1253—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by using adhesives curable adhesive

Definitions

  • the present invention relates to an optical layered body manufacturing method and an optical layered body.
  • Optical sheets e.g., microlens sheets, prism sheets, brightness enhancement films (e.g., 3M Brightness Enhancement Film: BEF, (registered trademark)) are used in various optical devices (e.g., display devices and lighting devices).
  • the term "optical sheet” is not limited to the above examples, but broadly includes sheet-like optical members, and further includes, for example, diffusion plates and light guide plates.
  • Optical sheets are attached to other optical sheets or optical devices using, for example, an adhesive layer.
  • the term “optical laminate” refers to a configuration including an optical sheet and an adhesive layer or a configuration including a plurality of optical sheets.
  • the term “adhesive” is used to include pressure-sensitive adhesives (also referred to as "pressure-sensitive adhesives").
  • Patent Document 1 discloses in Patent Document 1 an optical laminate (referred to as an "optical laminate sheet” in Patent Document 1) that can be used in display devices and lighting devices.
  • the optical laminate of Patent Document 1 has an optical sheet (for example, a microlens sheet) having an uneven structure on its surface, and an adhesive layer provided on the surface having an uneven structure. 5% to 90% of the height of the projections of the uneven structure is filled with the adhesive layer.
  • the adhesive layer is formed from an adhesive composition containing a graft polymer obtained by graft-polymerizing a chain containing a cyclic ether group-containing monomer to a (meth)acrylic polymer and a photocationic polymerization initiator or a thermosetting catalyst.
  • Patent Documents 2 and 3 disclose a light distribution structure that utilizes total reflection at interfaces of a plurality of air cavities and that can be used in display devices and lighting devices. By using the light distribution structures disclosed in Patent Documents 2 and 3, the degree of freedom and accuracy of light distribution control can be improved.
  • the extent to which the adhesive layer penetrates into (fills in) the recesses of the uneven structure affects the function of the optical sheet. Therefore, the extent to which the adhesive layer penetrates into the recesses of the uneven structure (the ratio of the volume of the adhesive layer existing in the space to the volume of the space defined by the recesses of the uneven structure) is required to be suppressed. .
  • Patent Documents 2 and 3 We considered forming a plurality of air cavities (internal spaces) that constitute a light distribution control structure.
  • Patent Documents 2 and 3 do not describe that a plurality of air cavities (internal spaces) forming a light distribution structure are formed by the surface having the uneven structure of the optical sheet and the surface of the adhesive layer.
  • the present invention has been made to solve the above-mentioned problems, and provides a method for manufacturing an optical laminate having an adhesive layer whose degree of penetration into concave portions of an uneven structure of an optical sheet is suppressed, and such an optical laminate.
  • the purpose is to provide the body.
  • Pl is the pressure when the adhesive layer is attached to the first main surface of the first optical sheet, and
  • Pf be the pressure applied to the flat portion when the adhesive layer is attached to the first main surface of the first optical sheet, When Sp ⁇ sin ⁇ a ⁇ Pf
  • [Item 2] A manufacturing method according to item 1, wherein Dd is 0.5 ⁇ m or less.
  • [Item 3] 3. The manufacturing method according to item 1 or 2, wherein the pressure Pl in the step C is 0.1 MPa or more and 0.5 MPa or less.
  • [Item 4] 4. The manufacturing method according to any one of items 1 to 3, wherein the adhesive layer has a thickness Dt of 3 ⁇ m or more and 10 ⁇ m or less.
  • the adhesive layer is An adhesive containing a polyester resin that is a copolymer of a polyhydric carboxylic acid and a polyhydric alcohol, a cross-linking agent, and at least one cross-linking catalyst selected from the group consisting of an organic zirconium compound, an organic iron compound and an organic aluminum compound. formed by cross-linking the composition, The gel fraction after holding for 300 hours at a temperature of 85 ° C. and a relative humidity of 85% is 40% or more, 11.
  • [Item 12] 11 The manufacturing method according to any one of items 1 to 10, wherein the adhesive layer is the following adhesive layer Aa or adhesive layer Ab: In a creep test using a rotational rheometer, the creep deformation rate is 10% or less when a stress of 10000 Pa is applied at 50°C for 1 second, and the creep deformation is obtained when a stress of 10000 Pa is applied at 50°C for 30 minutes. rate is 16% or less, Adhesive layer Aa having a 180° peel adhesive strength to a PMMA film of 10 mN/20 mm or more; formed by curing the curable resin of an adhesive composition containing a polymer and a curable resin, The initial tensile elastic modulus at 23° C.
  • each of the plurality of recesses has another inclined surface opposite to the inclined surface; 14. The manufacturing method according to any one of items 1 to 13, wherein the inclination angle ⁇ a of the inclined surface is smaller than the inclination angle ⁇ b of the other inclined surface.
  • the step B is An adhesive composition solution containing a (meth)acrylic polymer and/or polyester polymer, a cross-linking agent, and a solvent is applied onto the release-treated main surface of a substrate having a release-treated main surface. to form an adhesive composition solution layer; Step Bb of removing the solvent from the adhesive composition solution layer to form an adhesive composition layer; Another base material having a release-treated main surface is placed on the main surface of the adhesive composition layer opposite to the base material so that the release-treated main surface is in contact with the adhesive composition layer.
  • the step C is step Ca of bonding the first main surface of the first optical sheet to one main surface of the base material or the other base material of the adhesive layer; 15.
  • the manufacturing method according to item 15, wherein the one main surface of the base material or the other base material subjected to the release treatment has an arithmetic mean roughness Ra of less than 0.05 ⁇ m. [Item 17] 17.
  • a first optical sheet comprising a flat portion between the recesses; an adhesive layer disposed on the first main surface side of the first optical sheet and in contact with the flat portion; the surface of the adhesive layer and the first major surface of the first optical sheet define an internal space within each of the plurality of recesses; each of the plurality of recesses has an inclined surface with an inclination angle ⁇ a,
  • the adhesive layer is attached to the first main surface of the first optical sheet with pressure Pl, Pf is the pressure applied to the flat portion when the adhesive layer is attached to the first main surface of the first optical sheet; Sp is the stress obtained by dividing the 180° peel adhesive strength of the adhesive layer to the first main surface of the first optical sheet by the cross-sectional area of the film, which was obtained by a 180° peel test;
  • the adhesive layer is An adhesive comprising a polyester resin that is a copolymer of a polyhydric carboxylic acid and a polyhydric alcohol, a cross-linking agent, and at least one cross-linking catalyst selected from the group consisting of an organic zirconium compound, an organic iron compound and an organic aluminum compound. formed by cross-linking the composition,
  • the gel fraction after holding for 300 hours at a temperature of 85 ° C. and a relative humidity of 85% is 40% or more, 21.
  • the optical laminate according to item 20 which has a 180° peel adhesive strength to a PMMA film of 100 mN/20 mm or more. [Item 22] 21.
  • the creep deformation rate is 10% or less when a stress of 10000 Pa is applied at 50°C for 1 second, and the creep deformation is obtained when a stress of 10000 Pa is applied at 50°C for 30 minutes. rate is 16% or less
  • Adhesive layer Aa having a 180° peel adhesive strength to a PMMA film of 10 mN/20 mm or more; formed by curing the curable resin of an adhesive composition containing a polymer and a curable resin, The initial tensile elastic modulus at 23° C.
  • the adhesive layer Ab wherein the initial tensile elastic modulus at 23° C. after curing the curable resin of the adhesive composition is 1.00 MPa or more.
  • an optical layered body having an adhesive layer whose degree of penetration into the concave portions of the concave-convex structure of the optical sheet is suppressed, and such an optical layered body.
  • FIG. 1 is a schematic cross-sectional view of an optical layered body 100A according to an embodiment of the present invention
  • FIG. FIG. 10 is a schematic cross-sectional view of an optical layered body 101A according to another embodiment of the present invention
  • It is a typical sectional view of 100 A of optical laminated bodies.
  • FIG. 4 is a schematic perspective view of a first optical sheet 10a included in the optical layered body 100A.
  • FIG. 3 is a schematic cross-sectional view of a lighting device 200A including an optical layered body 100A;
  • FIG. 3 is a schematic cross-sectional view of a lighting device 200B including an optical layered body 100A; It is a figure which shows typically the process which manufactures 100 A of optical laminated bodies by a roll-to-roll method.
  • FIG. 10 is a schematic diagram for explaining a problem when manufacturing an optical layered body of a reference example by a roll-to-roll method
  • FIG. 10 is a schematic diagram for explaining a problem when manufacturing an optical layered body of a reference example by a roll-to-roll method
  • FIG. 3 is a schematic plan view of a concave-convex shaping film 70 included in the optical layered body according to the embodiment of the present invention.
  • FIG. 3 is a schematic cross-sectional view of a film for forming concavities and convexities 70; 5 is a graph showing evaluation results of the area ratio (%) of air bubbles and the height ( ⁇ m) of an adhesive layer present in recesses in optical laminates of Examples.
  • FIG. 5 is a schematic diagram for explaining a method of evaluating a change in the degree of penetration of an adhesive layer into recesses using an optical layered body;
  • FIG. 10 is a schematic cross-sectional view for explaining a method of evaluating a change in the degree of penetration of the adhesive layer into the concave portion using the optical layered body;
  • Optical images of the sample 1000A having the optical laminate 100S of Example A the upper is the optical image of the sample 1000A before applying force, the middle is the optical image of the sample 1000A when the force is applied, and the lower is the optical image of the sample 1000A.
  • an optical image of sample 1000A after the force has been removed.
  • Fig. 10 is an optical image of a sample having the optical stack of Example B, the top optical image of the sample before force is applied, the middle optical image of the sample when the force is applied, and the bottom is the optical image of the sample after the force is removed;
  • FIG. 10 shows an optical image of the sample after it has been exposed;
  • FIG. 3 is a schematic plan view of an unevenness-shaping film 52 included in the optical layered body according to the embodiment of the present invention.
  • FIG. 5 is a schematic cross-sectional view of an uneven-shaped film 52.
  • FIG. FIG. 3 is a schematic plan view of an uneven shaped film 82 included in the optical layered body according to the embodiment of the present invention.
  • FIG. 4 is a schematic cross-sectional view of recesses 84 included in the unevenness-forming film 82.
  • FIG. FIG. 3 is a schematic plan view of recesses 84 included in the unevenness-forming film 82.
  • FIG. 5 is a schematic diagram for explaining a method of calculating a calculated embedding amount Dd of an adhesive layer
  • FIG. 5 is a schematic diagram for explaining a method of calculating a calculated embedding amount Dd of an adhesive layer
  • FIG. 5 is a schematic diagram for explaining a method of calculating a calculated embedding amount Dd of an adhesive layer
  • 4 is a graph showing the correlation between the measured value ( ⁇ m) of the height of the adhesive layer present in the recess and the calculated embedding amount Dd ( ⁇ m).
  • FIG. 4 is a schematic perspective view for explaining a method of measuring a compressive stress-strain curve of an adhesive layer.
  • FIG. 4 is a schematic cross-sectional view for explaining a method for measuring the 180° peel adhesive strength of the adhesive layer to the optical sheet.
  • FIG. 4 is a schematic top view for explaining a method of measuring the 180° peel adhesive strength of the adhesive layer to the optical sheet.
  • FIG. 4 is a schematic cross-sectional view for explaining a method for measuring the 180° peel adhesive strength of the adhesive layer to the optical sheet.
  • An optical laminate according to an embodiment of the present invention includes an optical sheet having a first main surface having an uneven structure and a second main surface opposite to the first main surface; and an adhesive layer.
  • the adhesive layer attached to the surface (first main surface) having the uneven structure of the optical sheet has the uneven structure. An example that does not intrude into the concave portion of is described.
  • FIG. 1A shows a schematic cross-sectional view of an optical layered body 100A according to an embodiment of the present invention.
  • FIG. 1B shows a schematic cross-sectional view of an optical laminate 101A according to an embodiment of the invention.
  • FIG. 2 is a schematic cross-sectional view showing an enlarged part of the optical layered body 100A.
  • FIG. 3 is a schematic perspective view of an optical sheet 10a included in the optical laminate 100A.
  • FIG. 4A is a schematic cross-sectional view of a lighting device 200A including the optical layered body 100A.
  • the optical layered body 100A includes a first optical sheet 10a having a first principal surface 12s having an uneven structure and a second principal surface 18s opposite to the first principal surface 12s; and an adhesive layer 20a disposed on the first main surface 12s side of 10a.
  • the uneven structure of the first main surface 12 s includes a plurality of recesses 14 and flat portions 10 s between adjacent recesses 14 among the plurality of recesses 14 .
  • the adhesive layer 20a is in contact with the flat portion 10s.
  • the surface of the adhesive layer 20a and the first major surface 12s of the first optical sheet 10a define an internal space 14a within each of the plurality of recesses 14. As shown in FIG.
  • the optical layered body 101A has an optical layered body 100A and a second optical sheet 30 arranged on the opposite side of the adhesive layer 20a from the first optical sheet 10a side.
  • the description of the optical layered body 100A also applies to the optical layered body 101A, so the description may be omitted to avoid duplication.
  • the second optical sheet 30 included in the optical laminate 101A has a main surface 38s on the side of the adhesive layer 20a and a main surface 32s opposite to the main surface 38s. 38 s of main surfaces are flat surfaces. At least one other optical member (or optical sheet) may be arranged on the opposite side of the adhesive layer 20a of the second optical sheet 30 of the optical laminate 101A (that is, on the main surface 32s).
  • Other optical members include, for example, a diffuser plate, a light guide plate, etc., and are adhered onto the main surface 32s of the optical sheet 30 via an adhesive layer.
  • the adhesive layer 20a does not enter the recess 14. That is, the adhesive layer 20a does not exist within the space defined by the recess 14 .
  • the space defined by the recess 14 refers to the space defined by the recess 14 and the sheet surface (parallel to the XY plane) including the flat portion 10s adjacent to the recess 14 . Therefore, the internal space 14a defined by the first optical sheet 10a side surface 28s of the adhesive layer 20a and the first main surface 12s of the first optical sheet 10a is the space defined by the concave portion 14 in this example. match.
  • the internal space 14a is sometimes called an air cavity or an optical cavity.
  • the internal space 14a is typically a void filled with air.
  • the internal space 14a may be filled with a material having a lower refractive index than the first optical sheet 10a and the adhesive layer 20a.
  • the plurality of internal spaces are continuous in the X direction (for example, triangular prismatic spaces extending in the X direction), as shown in the example of FIG.
  • the grooves may be provided discretely in the Y direction, or may be discretely provided in the form of islands in both the X direction and the Y direction as in the example of FIG. 9A. As shown in FIGS.
  • the light guiding direction of the light guide layer 80 is the -Y direction.
  • the -Y direction is referred to as the light guide direction, and light having a component in the -Y direction (not zero) propagates in the -Y direction. Let's say there is.
  • the optical laminate 100A functions as a light distribution structure described in Patent Documents 2 and 3.
  • the optical laminate 100A has a plurality of internal spaces 14a that form an interface that directs light in the Z direction (downward in the figure) by total internal reflection.
  • the internal space 14a is defined by a surface 16s and a surface 17s, which are part of the first main surface 12s of the first optical sheet 10a, and a surface 28s of the adhesive layer 20a on the side of the first optical sheet 10a.
  • the cross-sectional shape of the internal space 14a (the cross-sectional shape perpendicular to the X direction and parallel to the YZ plane) is triangular.
  • the interface formed by the inclined surface 16s functions as an interface that directs light in the Z direction (downward in the drawing) by total internal reflection.
  • the inclination angle ⁇ a of the inclined surface 16s is, for example, 10° or more and 70° or less.
  • the lower limit is preferably 30° or more, more preferably 45° or more.
  • the angle of inclination ⁇ a is less than 10°, the controllability of the light distribution may deteriorate, and the light extraction efficiency may also deteriorate.
  • the inclination angle ⁇ a exceeds 70°, it may become difficult to process the irregular shaped film, for example.
  • the inclination angle ⁇ b of the inclined surface 17s is, for example, 50° or more and 100° or less. The lower limit is preferably 70° or more. If the tilt angle ⁇ b is less than 50°, stray light may occur in an unintended direction. On the other hand, if the angle of inclination ⁇ b exceeds 100°, it may become difficult to process the irregular shaped film, for example.
  • the inclination angle ⁇ a of the inclined surface 16s and the inclination angle ⁇ b of the inclined surface 17s are angles with respect to the direction parallel to the Y direction in the cross section of the recess 14 (the cross section perpendicular to the X direction and parallel to the YZ plane).
  • the inclination angle ⁇ a of the inclined surface 16s is smaller than the inclination angle ⁇ b of the inclined surface 17s.
  • the inclined surface 16s is arranged closer to the light source 60 than the inclined surface 17s.
  • the shape of the cross section of the internal space 14a (the cross section perpendicular to the X direction and parallel to the YZ plane) is defined by the inclination angle ⁇ a of the inclined surface 16s, the inclination angle ⁇ b of the inclined surface 17s, the width Wy, and the depth C. .
  • the shape of the internal space 14a (recess 14) is not limited to the illustrated one, and can be modified in various ways. By adjusting the shape, size, arrangement density, etc. of the internal space 14a (recesses 14), it is possible to adjust the distribution of light rays (light distribution) emitted from the optical laminate 100A (for example, Patent Document 2 and 3).
  • An optical laminate that functions as a light distribution control structure can constitute a light guide layer and/or a direction conversion layer having a plurality of internal spaces.
  • the optical laminate 100A is used in a lighting device 200A.
  • the illumination device 200A includes an optical laminate 102A and a light source 60.
  • the optical layered body 102A has an optical layered body 100A and a light guide layer 80 provided on the side of the adhesive layer 20a of the optical layered body 100A opposite to the first optical sheet 10a side.
  • the light guide layer 80 is, for example, adhered to the surface 22s of the adhesive layer 20a on the opposite side of the first optical sheet 10a.
  • the light guide layer 80 has a first principal surface 80 a , a second principal surface 80 b opposite to the first principal surface 80 a , and a light receiving portion 80 c that receives light emitted from the light source 60 .
  • the light source 60 is, for example, an LED device, and may be used by arranging a plurality of LED devices.
  • TIR total internal reflection
  • Part of the light guided into the light guide layer 80 undergoes total internal reflection (TIR) at the interfaces 16s and 14s formed by the internal space 14a, as indicated by arrows in FIG. 4A.
  • TIR total internal reflection
  • Light totally internally reflected at the interface 14s (surface 28s of the adhesive layer 20a on the first optical sheet side) propagates through the light guide layer 80 and the adhesive layer 20a, and is totally internally reflected at the inclined surface 16s. is emitted to the outside of the optical laminate 102A from the second main surface 18s side of the first optical sheet 10a.
  • the light guide layer 80, the adhesive layer 20a and the first optical sheet 10a have approximately the same refractive index.
  • the difference (absolute value) in refractive index between the light guide layer 80 and the adhesive layer 20a and the difference (absolute value) in refractive index between the adhesive layer 20a and the first optical sheet 10a are each independently, for example, 0.20.
  • the thickness of the adhesive layer 20a is, for example, 2.0 ⁇ m or more and 15.0 ⁇ m or less.
  • the lower limit is preferably 4.0 ⁇ m or more.
  • the upper limit is preferably 11.0 ⁇ m or less, more preferably 9.0 ⁇ m or less.
  • the thickness of the adhesive layer 20a refers to the thickness on the flat portion 10s of the first main surface 12s of the first optical sheet 10a.
  • the haze value of the optical laminate 100A is, for example, 5.0% or less.
  • the haze value can be measured with D65 light, for example, using a haze meter (apparatus name “HZ-1”, manufactured by Suga Test Instruments Co., Ltd.).
  • the light guide layer 80 is provided on the first optical sheet 10a side of the optical laminate 100A (closer to the first optical sheet 10a than the adhesive layer 20a) as in the illumination device 200B shown in FIG. 4B, good.
  • the light guide layer 80 and the first optical sheet 10a may be attached via an adhesive layer.
  • the light totally internally reflected at the interface 14s (the surface 28s of the adhesive layer 20b on the side of the first optical sheet) propagates through the adhesive layer 20a and is totally internally reflected at the inclined surface 16s. The light is emitted to the outside of the optical laminate 102B from the second main surface 18s side of the first optical sheet 10a.
  • a substrate layer may be provided on the side of the lighting device 200A opposite to the light guide layer 80 of the optical laminate 100A.
  • an antireflection layer may be provided, and instead of the substrate layer, a hard coat layer (for example, having a pencil hardness of H or higher) may be provided.
  • An antireflection layer and/or a hard coat layer may be provided on the substrate layer.
  • an antireflection layer and/or a hard coat layer may be provided on the opposite side of the light guide layer 80 to the exit surface (upper side in the figure).
  • the antireflection layer and the hard coat layer can be formed by known methods using known materials.
  • a low refractive index layer may be provided between the optical laminate 102A and the substrate layer (or antireflection layer and/or hard coat layer).
  • a base material layer may be provided on the side opposite to the light guide layer 80 of the optical laminate 100A.
  • An antireflection layer and/or a hard coat layer (for example, a pencil hardness of H or higher) may be provided instead of the base layer, and an antireflection layer and/or a hard coat layer may be provided on the base layer.
  • an antireflection layer and/or a hard coat layer may be provided on the exit surface side (lower side in the figure) of the light guide layer 80 .
  • a low refractive index layer may be provided between the optical laminate 102B and the substrate layer (or antireflection layer and/or hard coat layer).
  • each of the plurality of recesses 14 extends in the X direction and is continuous in the X direction.
  • the plurality of recesses 14 are arranged discretely in the Y direction, and flat portions 10 s are provided between the recesses 14 .
  • the concave portions 14 are preferably arranged periodically with a pitch Py of, for example, 6 ⁇ m or more and 120 ⁇ m or less.
  • the width Wy of the recess 14 is, for example, 3 ⁇ m or more and 20 ⁇ m or less
  • the width Dy of the flat portion 10s is, for example, 3 ⁇ m or more and 100 ⁇ m or less.
  • a ratio Wy/Dy between the width Wy of the recess 14 and the width Dy of the flat portion 10s is, for example, 0.3 or more and 7 or less.
  • the depth C (depth in the Z direction) of the concave portion 14 is, for example, 1 ⁇ m or more and 100 ⁇ m or less.
  • the depth C of the concave portion 14 is preferably 20 ⁇ m or less, more preferably 12 ⁇ m or less.
  • the depth C of the concave portion 14 is preferably 4 ⁇ m or more, more preferably 6 ⁇ m or more, and even more preferably 8 ⁇ m or more.
  • the density of the plurality of recesses 14 is the ratio of the area of the plurality of recesses 14 to the area of the first optical sheet 10a (occupied area ratio) is preferably 0.3% or more from the viewpoint of obtaining good luminance.
  • the occupied area ratio of the plurality of concave portions 14 is appropriately selected depending on the application in which it is used. % or less. It is preferably 30% or more and 80% or less for applications requiring higher luminance. Note that the occupied area ratios of the plurality of recesses 14 may be uniform, or may be increased with increasing distance from the light source (e.g., light source 60 in FIG. 4A or FIG. 4B) so that luminance does not decrease as the distance increases. The occupied area ratio may be increased as the time increases.
  • a concavo-convex shaping film 70 (optical sheet) shown in FIGS. 9A and 9B may be used.
  • the concave-convex shaped film 70 has a main surface having a concave-convex structure, and the concave-convex structure has a plurality of concave portions 74 and flat portions 72 s between adjacent concave portions 74 .
  • the plurality of concave portions 74 are discretely arranged in an island shape in both the X direction and the Y direction.
  • the recesses 74 have a size (length L, width W: see FIGS. 9A and 9B), for example, the length L is preferably 10 ⁇ m or more and 500 ⁇ m or less, and the width W is 1 ⁇ m or more and 100 ⁇ m. The following are preferable.
  • the depth H is preferably 1 ⁇ m or more and 100 ⁇ m or less.
  • the depth H of the concave portion 74 is preferably 20 ⁇ m or less, more preferably 12 ⁇ m or less.
  • the depth H of the concave portion 74 is preferably 4 ⁇ m or more, more preferably 6 ⁇ m or more, and more preferably 8 ⁇ m or more.
  • the pitch Px is preferably, for example, 10 ⁇ m or more and 500 ⁇ m or less
  • the pitch Py is, for example, preferably 10 ⁇ m or more and 500 ⁇ m or less.
  • the recesses are not limited to the example of FIG. 9A, and when used in a lighting device, the plurality of recesses are discretely arranged in the light guiding direction of the light guide layer and in a direction intersecting the light guiding direction of the light guide layer. good too.
  • the density of the plurality of concave portions 74 is the ratio of the area of the plurality of concave portions 74 to the area of the concave-convex formed film 70 (occupied area ratio) is preferably 0.3% or more from the viewpoint of obtaining good luminance.
  • the occupied area ratio of the plurality of concave portions 74 is appropriately selected depending on the application, and for example, in applications requiring transparency, it is preferably 30% or less in order to obtain good visible light transmittance and haze value. It is preferably 1% or more from the viewpoint of obtaining good luminance.
  • the upper limit is more preferably 25% or less, preferably 10% or less, more preferably 5% or less in order to obtain a high visible light transmittance.
  • the occupied area ratio of the plurality of recesses 74 may be uniform, or may be increased with increasing distance from the light source (e.g., light source 60 in FIG. 4A or 4B) so that brightness does not decrease.
  • the occupied area ratio may be increased as the time increases.
  • the cross-sectional shape of the concave portion 14 is not limited to this. (eg trapezoidal). Also, the shape is not limited to a polygon, and may be a shape including at least a part of a curved line. Shapes at least partially curved include, for example, a portion of the circumference of a circle or an ellipse, or a shape including a combination of multiple curves with different curvatures.
  • a concavo-convex shaping film 82 (optical sheet) shown in FIG. 15A may be used.
  • the light source 60 is also shown in FIG. 15A.
  • the concave-convex shaped film 82 has a main surface having a concave-convex structure, and the concave-convex structure has a plurality of concave portions 84 and flat portions 82s between adjacent concave portions 84 .
  • Each of the plurality of recesses 84 has a first inclined surface 86s that directs part of the light propagating in the optical stack in the Z direction by total internal reflection, and a second inclined surface 87s opposite to the first inclined surface 86s. have As shown in FIG.
  • the first inclined surface 86s of the concave portion 84 forms a curved surface that is convex toward the light source 60 side.
  • the light emitted from each LED device spreads in the Y direction. Having a curved surface causes the first inclined surface 86s to act more uniformly on the light.
  • the first inclined surface 86s may be parallel to the X direction.
  • Preferable ranges of the size (length L, width W: see FIGS. 15B and 15C) and depth H (see FIG. 15C) of the recesses 84 and the pitches Px and Py are, for example, the same as those of the recesses 74 of the unevenness-shaping film 70. can be the same.
  • the optical layered body 100A can be produced by attaching the adhesive layer 20a to the uneven surface 12s of the first optical sheet 10a using, for example, a roll-to-roll method. From the viewpoint of mass productivity, it is preferable to manufacture the optical layered body 100A by a roll-to-roll method as shown in FIG.
  • the first optical sheet 10a and the adhesive layer 20a are bonded together by rolls Ra and Rb rotating in the directions of the arrows.
  • one of the rolls Ra and Rb is the driving roll and the other is the driven roll.
  • the pressure (nip pressure, bonding pressure, lamination pressure) applied to the first optical sheet 10a and the adhesive layer 20a between the roll Ra and the roll Rb is the TD (Transverse Direction) direction (roll can vary depending on the position in the direction parallel to the axes of Ra and Rb).
  • the pressure applied to the first optical sheet 10a and the adhesive layer 20a is greater at both end portions Ae in the TD direction than at the center portion Ad in the TD direction.
  • the size of the white arrow schematically indicates the size of the pressure applied to the first optical sheet 10a and the adhesive layer 20a between the rolls Ra and Rb.
  • the optical layered body of the reference example is manufactured by the roll-to-roll method using the adhesive layer 90 and the first optical sheet 10a of the reference example, the following problems occur. may occur.
  • the adhesive layer 90 of the reference example is used to produce the optical layered body by the roll-to-roll method. .
  • the optical sheet 10a and the adhesive layer 90 are applied with an appropriate pressure at the central portion Ad in the TD direction, that is, the adhesive layer 90 is on the uneven surface of the optical sheet 10a.
  • the pressure is adjusted so as to suppress the penetration of the adhesive layer 90 into the concave portion 14 while maintaining good adhesiveness to 12s, a larger pressure is applied to both ends Ae in the TD direction. 1 optical sheet 10a and adhesive layer 90, the adhesive layer 90 may excessively penetrate into the recesses 14 at both ends Ae.
  • FIG. 7A the optical sheet 10a and the adhesive layer 90 are applied with an appropriate pressure at the central portion Ad in the TD direction, that is, the adhesive layer 90 is on the uneven surface of the optical sheet 10a.
  • the length in the TD direction of the optical layered body produced by the roll-to-roll method is, for example, several meters. Such a problem is more likely to occur as the length of the optical layered body in the TD direction increases.
  • the inventors have found that using a predetermined adhesive layer 20a, as shown in FIG. 8A, can solve the above problems described with reference to FIGS. 7A and 7B.
  • the left arrow in FIG. 8A indicates the time series.
  • the first optical sheet 10a and the adhesive layer 20a are prepared (upper part of FIG. 8A), and when the surface having the concave-convex structure of the first optical sheet 10a and the adhesive layer 20a are bonded together, the flat portion 10s of the concave-convex structure and the adhesive layer 20a are adhered to each other. Sufficient pressure is applied so as not to excessively generate air bubbles at the interface with the agent layer 20a.
  • the adhesive layer 20a may temporarily and excessively enter the concave portion 14 during lamination (middle of FIG. 8A). This is because when the pressure applied during lamination is removed, the degree of penetration (embedding) of the adhesive layer 20a into the recesses 14 decreases (lower part of FIG. 8A).
  • An example of such an adhesive layer 20a will be shown in Experimental Examples below. In the obtained optical layered body 100A, the penetration of the adhesive layer 20a into the concave portion 14 is suppressed, and air bubbles present at the interface between the flat portion 10s of the concave-convex structure and the adhesive layer 20a are suppressed. .
  • the flat portion 10s and the adhesive layer 20a when viewed in plan from the normal direction of the first main surface of the first optical sheet, the flat portion 10s and the adhesive layer 20a occupy the area of the first optical sheet.
  • the area ratio of air bubbles existing at the interface is 3% or less, and the height of the adhesive layer 20a existing in the plurality of recesses 14 is 2 ⁇ m or less.
  • the height of the adhesive layer 20a present in the recess 14 is the height of the adhesive layer 20b in the Z direction in the cross section of the recess 14 (the cross section perpendicular to the X direction and parallel to the YZ plane in FIG. 1A), It is obtained using the flat portion 10s as a reference.
  • the height of the adhesive layer 20a present in the recess 14 can be determined from a cross-sectional SEM image of an arbitrarily selected recess 14, for example, as in the examples described later. It can be obtained by measuring the maximum height.
  • the area ratio of air bubbles can be measured, for example, by the method described in Examples below.
  • the area ratio of air bubbles is preferably 2.5% or less, more preferably 1.5% or less, and still more preferably 0.1% or less.
  • the height of the adhesive layer present in the plurality of recesses is preferably 1 ⁇ m or less, more preferably 0.6 ⁇ m or less. Note that the optical layered body according to the embodiment of the present invention is not limited to one manufactured by the roll-to-roll method. Even in an optical layered body produced by a manufacturing method other than the roll-to-roll method, the penetration of the adhesive layer into the recessed portions is suppressed, and air bubbles existing at the interface between the flat portion and the adhesive layer are suppressed. be.
  • the area ratio of air bubbles depends on the surface roughness of the adhesive layer. can also change. If the surface of the adhesive layer (the surface on the side of the first optical sheet) has a large surface roughness, air bubbles are likely to occur.
  • the adhesive layer is formed, for example, by the following method. First, an adhesive composition solution containing a (meth)acrylic polymer and/or polyester polymer, a cross-linking agent, and a solvent is applied to a substrate (first separator) having a release-treated main surface. An adhesive composition solution layer is formed by applying it onto the release-treated main surface. Then, the solvent of the adhesive composition solution layer is removed to form an adhesive composition layer. Subsequently, on the main surface of the adhesive composition layer opposite to the first separator side, another base material (second separator) having a release-treated main surface is placed on the release-treated main surface.
  • an adhesive composition solution containing a (meth)acrylic polymer and/or polyester polymer, a cross-linking agent, and a solvent is applied to a substrate (first separator) having a release-treated main surface.
  • An adhesive composition solution layer is formed by applying it onto the release-treated main surface.
  • the solvent of the adhesive composition solution layer is removed to form an adhesive composition layer.
  • the adhesive layer is obtained by cross-linking the (meth)acrylic polymer and/or the polyester-based polymer of the adhesive composition layer with a cross-linking agent. That is, a laminate having a laminated structure of base material (first separator)/adhesive layer/another base material (second separator) is obtained here.
  • a laminate including a substrate having a release-treated main surface and an adhesive layer is sometimes called an adhesive sheet. Either the principal surface of the first separator side or the principal surface of the second separator side of the adhesive layer thus obtained is the surface having the uneven structure of the first optical sheet (unevenness-imparting film).
  • the optical layered body according to the embodiment of the present invention can be obtained by laminating them together.
  • the peel-treated main surface of the second separator is, for example, preferably less than 0.05 ⁇ m, more preferably less than 0.03 ⁇ m.
  • the lower limit of the arithmetic mean roughness Ra is not particularly limited, it is, for example, 0.001 ⁇ m.
  • the maximum height Rz of the peel-treated main surface (surface on the adhesive layer side) of the second separator is, for example, less than 0.5 ⁇ m, preferably less than 0.3 ⁇ m.
  • the lower limit of the maximum height Rz is not particularly limited, it is, for example, 0.005 ⁇ m.
  • the y-direction or -y-direction of the first optical sheet 10a can be the MD (Machine Direction) direction.
  • the inclined surface 16s having the smaller inclination angle ⁇ a of the recess 14 is closer to the nip portion between the rolls Ra and Rb than the inclined surface 17s having the larger inclination angle ⁇ b.
  • the extent to which the adhesive layer 20a penetrates into the concave portion 14 does not change greatly depending on the bonding direction.
  • the present inventor evaluated the embedding amount of the adhesive layer in the concave portion (the degree of penetration of the adhesive layer into the concave portion) using the value of "calculated embedding amount Dd" calculated by the following method. I found what I can do. By using the calculated embedding amount Dd, it is possible to evaluate the degree of embedding of the adhesive layer into the concave portions without actually attaching the adhesive layer to the optical sheet having the concave portions on the surface.
  • the method of manufacturing the optical layered body 100A includes a step of preparing the first optical sheet 10a (sometimes referred to as “step A”), and preparing an adhesive layer 20a. It includes a step (sometimes referred to as “step B”) and a step of bonding the adhesive layer 20a to the first main surface 12s of the first optical sheet 10a (sometimes referred to as “step C”). At this time, in step C, the pressure (laminating pressure) when bonding the adhesive layer 20a to the first main surface 12s of the first optical sheet 10a is defined as Pl.
  • the embedding amount of the adhesive layer 20a in the recess 14 (here, the maximum value of the height of the adhesive layer in the recess 14) becomes the largest (middle of FIG. 8A). After that, when the pressure Pl is removed, the embedding amount of the adhesive layer 20a in the concave portion 14 decreases (lower stage in FIG. 8A).
  • dmax be the embedding amount of the adhesive layer 20a in the concave portion 14 when the pressure Pl is applied.
  • the lower part of FIG. 8A shows a state in which the adhesive layer 20a is not embedded in the recess 14 at all, the present invention is not limited to this, and the amount of embedding may be smaller than that in the middle part of FIG. 8A.
  • FIG. 8B is a diagram schematically showing another example of the process of manufacturing the optical layered body 100A.
  • the type of the adhesive layer 20a as shown in the lower part of FIG. 8B, even if the pressure Pl is removed, the embedding amount of the adhesive layer 20a in the concave portion 14 does not decrease (or the degree of decrease is small). It is possible.
  • the compressive elastic modulus of the adhesive layer 20a is smaller than that in the example of FIG. 8A.
  • the embedding amount of the adhesive layer 20a in the concave portion 14 is It is considered to be determined by the relationship between the restoring force F1 due to the compressive elasticity of the adhesive layer 20a when the loading amount is dmax and the stress F2 obtained from the peel adhesive strength of the adhesive layer 20a to the first optical sheet 10a.
  • the pressure applied to the flat portion 10s of the first main surface 12s of the first optical sheet 10a is Pf.
  • the lamination pressure Pl is given below.
  • the occupied area ratio Rr of the concave portions 14 is the ratio of the area of the plurality of concave portions 14 to the area of the first optical sheet 10a when the first optical sheet 10a is viewed from the normal direction of the first main surface 12s.
  • the area of the plurality of recesses 14 when the first optical sheet 10a is viewed from the normal direction of the first main surface 12s is the area of the first optical sheet 10a when viewed from the normal direction of the first main surface 12s. is obtained by subtracting the area of the flat portion 10s from the area of .
  • the restoring force F1 due to compressive elasticity is evaluated using the stress Sm corresponding to the ratio (dmax/Dt) of the embedded amount dmax to the thickness Dt of the adhesive layer 20a in the compressive stress-strain curve of the adhesive layer 20a.
  • the thickness Dt of the adhesive layer 20a is the thickness of the adhesive layer 20a on the flat portion 10s of the first main surface 12s of the first optical sheet 10a. is the thickness of the adhesive layer 20a before it is applied.
  • the ratio of the embedded amount dmax to the thickness Dt of the adhesive layer 20a (dmax/Dt) is the compressive stress-strain curve of the adhesive layer 20a with the lamination pressure Pl added.
  • the stress F2 caused by the peel adhesive force is obtained by dividing the 180° peel adhesive force of the adhesive layer 20a to the first optical sheet 10a by the cross-sectional area of the film, which is obtained by the 180° peel test, and sin ⁇ a is added to the stress Sp. Evaluation is performed using the multiplied value (Sp ⁇ sin ⁇ a). It is the component of the stress Sp that is parallel to the direction in which the lamination pressure Pl is applied.
  • the cases are classified according to the magnitude relationship between the restoring force F1 due to compressive elasticity and the stress F2 due to the peel adhesive force.
  • the pressure Pl is removed, it is considered that the embedding amount of the adhesive layer 20a in the concave portion 14 does not change.
  • the calculated embedding amount Dd can be used to represent an optical layered body in which the penetration of the adhesive layer 20a into the concave portion 14 is suppressed. Specifically, when the height (measured value) of the adhesive layer present in the recess 14 is 2 ⁇ m or less, the calculated embedding amount Dd can be expressed as 1.3 ⁇ m or less.
  • optical laminate 100A As described above, the optical laminate 100A according to this embodiment can be expressed as follows.
  • the optical layered body 100A includes a first optical sheet 10a having a first principal surface 12s having an uneven structure and a second principal surface 18s opposite to the first principal surface 12s, and the first principal surface 12s of the first optical sheet 10a. and an adhesive layer 20a disposed on the side.
  • the uneven structure of the first main surface 12 s includes a plurality of recesses 14 and flat portions 10 s between adjacent recesses 14 among the plurality of recesses 14 .
  • the adhesive layer 20a is in contact with the flat portion 10s.
  • the surface of the adhesive layer 20a and the first major surface 12s of the first optical sheet 10a define an internal space 14a within each of the plurality of recesses 14. As shown in FIG.
  • Each of the plurality of recesses 14 has an inclined surface with an inclination angle ⁇ a.
  • the adhesive layer 20a is adhered to the first main surface 12s of the first optical sheet 10a with pressure Pl.
  • Pf is the pressure applied to the flat portion 10s when the adhesive layer 20a is attached to the first main surface 12s of the first optical sheet 10a.
  • Sp is the stress obtained by dividing the 180° peel adhesive strength of the adhesive layer 20a to the first main surface 12s of the first optical sheet 10a, which was obtained by the 180° peel test, by the cross-sectional area of the film.
  • Dd is the value obtained by multiplying the strain corresponding to Pf in the compressive stress-strain curve of the adhesive layer 20a by the thickness Dt of the adhesive layer 20a.
  • Dd is a value obtained by multiplying the strain corresponding to Sp ⁇ sin ⁇ a in the compressive stress-strain curve of the adhesive layer 20a by the thickness Dt of the adhesive layer 20a, Dd is 1.3 ⁇ m or less.
  • the method for manufacturing the optical layered body 100A comprises a step A of preparing the first optical sheet 10a, a step B of preparing the adhesive layer 20a, and forming the adhesive layer 20a as the first main layer of the first optical sheet 10a. and a step C of bonding to the surface 12s.
  • Each of the plurality of recesses 14 has an inclined surface with an inclination angle ⁇ a.
  • the pressure when the adhesive layer 20a is attached to the first main surface 12s of the first optical sheet 10a is Pl.
  • Pf is the pressure applied to the flat portion 10s when the adhesive layer 20a is attached to the first main surface 12s of the first optical sheet 10a.
  • Sp is the stress obtained by dividing the 180° peel adhesive strength of the adhesive layer 20a to the first main surface 12s of the first optical sheet 10a, which was obtained by the 180° peel test, by the cross-sectional area of the film.
  • Dd is the value obtained by multiplying the strain corresponding to Pf in the compressive stress-strain curve of the adhesive layer 20a by the thickness Dt of the adhesive layer 20a.
  • Dd is a value obtained by multiplying the strain corresponding to Sp ⁇ sin ⁇ a in the compressive stress-strain curve of the adhesive layer 20a by the thickness Dt of the adhesive layer 20a
  • Dd is 1.3 ⁇ m or less.
  • the compressive stress-strain curve of the adhesive layer 20a can be obtained, for example, by the method described in Examples.
  • y the compressive stress
  • x the strain
  • Dd multiplication
  • the 180° peel adhesive strength of the adhesive layer 20a to the first main surface 12s of the first optical sheet 10a obtained by the 180° peel test and the stress Sp obtained by dividing it by the cross-sectional area of the film are, for example, It can be determined by the method described in Examples.
  • the inclined surface having the inclination angle ⁇ a here partially reflects the light propagating in the adhesive layer 20a to the second main surface of the first optical sheet 10a by total internal reflection. Turn to the 18s side.
  • Each of the plurality of recesses 14 has another inclined surface (inclined angle ⁇ b) opposite to the inclined surface having the inclined angle ⁇ a, and the inclined angle ⁇ a is smaller than the inclined angle ⁇ b.
  • the adhesive layer included in the optical layered body according to the embodiment of the invention is not limited to the following examples.
  • Adhesive layer Aa International Publication No. 2021/167090 by the present applicant describes that in a creep test using a rotational rheometer, the creep deformation rate when a stress of 10000 Pa is applied at 50 ° C. for 1 second is 10% or less, and 50 An adhesive layer having a creep deformation rate of 16% or less when a stress of 10000 Pa is applied for 30 minutes at ° C. and a 180 ° peel adhesive strength to the PMMA film of 10 mN / 20 mm or more (hereinafter, "adhesive layer Aa" ) is described.
  • the degree of penetration into the concave portions when the adhesive layer is attached to the surface having the concave-convex structure of the optical sheet and its change over time are correlated with the creep deformation rate of the adhesive layer.
  • an adhesive layer having a creep deformation rate of 10% or less when a stress of 10,000 Pa was applied at 50° C. for 1 second was found to have a surface with an uneven structure.
  • the degree of penetration into the recesses of the uneven structure is suppressed
  • the creep deformation rate is 16 when a stress of 10,000 Pa is applied at 50 ° C. for 30 minutes (1800 seconds). % or less, the degree of penetration into the recesses of the uneven structure is suppressed from changing with time.
  • the entire disclosure content of WO2021/167090 is incorporated herein by reference.
  • Adhesive layer Ab Applicant's WO2021/167091 discloses at least one (meth)acrylate monomer selected from the group consisting of hydroxyl group-containing copolymerizable monomers, carboxyl group-containing copolymerizable monomers and nitrogen-containing vinyl monomers.
  • an adhesive layer formed by curing a curable resin of an adhesive composition comprising a polymer containing a copolymer with at least one copolymerizable functional group-containing monomer, and a curable resin.
  • the initial tensile elastic modulus at 23° C. before curing the curable resin of the adhesive composition is 0.35 MPa or more and 8.00 MPa or less, and 23 after curing the curable resin of the adhesive composition.
  • an adhesive layer (hereinafter sometimes referred to as "adhesive layer Ab") having an initial tensile modulus at °C of 1.00 MPa or more is described.
  • the initial tensile elastic modulus at 23° C. before curing the curable resin of the adhesive composition is 0.35 MPa or more, so that when the adhesive layer 20a is formed, that is, the adhesive composition layer is attached to the optical sheet 10a.
  • the adhesive composition layer has an initial tensile elastic modulus of 8.00 MPa or less at 23° C. before the curable resin of the adhesive composition is cured, so that the adhesive composition layer is formed on the first main surface of the optical sheet 10a.
  • the polymer contained in the adhesive composition is, for example, a copolymer comprising at least one (meth)acrylate monomer (e.g. alkyl (meth)acrylate), a hydroxyl group-containing copolymerizable monomer, a carboxyl group-containing copolymer, including copolymers with at least one copolymerizable functional group-containing monomer selected from the group consisting of polymerizable monomers and nitrogen-containing vinyl monomers.
  • the at least one copolymerizable functional group-containing monomer comprises a nitrogen-containing vinyl monomer
  • the weight ratio of (meth)acrylate monomer to nitrogen-containing vinyl monomer is, for example, between 95:5 and 50:50, 95:5.
  • the adhesive layer Ab is formed by curing a curable resin of an adhesive composition containing a polymer and a curable resin.
  • an adhesive composition layer formed from an adhesive composition is provided on the first main surface 12s of the optical sheet 10a.
  • the adhesive composition is cured by applying heat or irradiating the adhesive composition layer with active energy rays. harden the adhesive resin.
  • the curable resin for example, ultraviolet curable resin
  • the initial tensile elastic modulus at 23° C. before curing the curable resin of the adhesive composition is, for example, 0.35 MPa or higher, 0.40 MPa or higher, 0.45 MPa or higher, or 0.50 MPa or higher, and 8.00 MPa or less, 7.70 MPa or less, 7.50 MPa or less, 7.00 MPa or less, 6.50 MPa or less, 6.00 MPa or less, 5.50 MPa or less, 5.00 MPa or less, 4.50 MPa or less, 4.00 MPa or less, 3.50 MPa or less or 3.00 MPa or less.
  • the upper limit of the initial tensile modulus at 23° C. after curing the curable resin of the adhesive composition is not particularly limited, but is, for example, 1000 MPa or less, 800 MPa or less, 600 MPa or less, 400 MPa or less, or 200 MPa or less.
  • the tensile modulus is 3.00 MPa or more.
  • the gel fraction before curing the curable resin of the adhesive composition is, for example, 75% or more, and the gel fraction after curing the curable resin of the adhesive composition is, for example, 90% or more.
  • the upper limit of these gel fractions is not particularly limited, it is, for example, 100%.
  • Adhesive layer Ac International application PCT/JP2022/004554 by the present applicant describes a group consisting of a polyester resin which is a copolymer of a polyhydric carboxylic acid and a polyhydric alcohol, a cross-linking agent, an organic zirconium compound, an organic iron compound and an organic aluminum compound. It is formed by cross-linking an adhesive composition containing at least one cross-linking catalyst selected from and has a gel fraction of 40% or more after holding for 300 hours at a temperature of 85 ° C. and a relative humidity of 85% , an adhesive layer (hereinafter sometimes referred to as "adhesive layer Ac") having a 180° peel adhesive strength to a PMMA film of 100 mN/20 mm or more. The adhesive layer Ac can also suppress changes over time under high temperature and high humidity conditions.
  • the entire disclosure of International Application PCT/JP2022/004554 is incorporated herein by reference.
  • the following adhesives can be suitably used for the adhesives forming the adhesive layer Aa or the adhesive layer Ab.
  • the adhesive contains, for example, a (meth)acrylic polymer
  • the (meth)acrylic polymer is, for example, a copolymer of a nitrogen-containing (meth)acrylic monomer and at least one other monomer.
  • Nitrogen-containing (meth)acrylic monomers have, for example, a nitrogen-containing cyclic structure.
  • a (meth)acrylic polymer is prepared using a nitrogen-containing (meth)acrylic monomer, especially when the nitrogen-containing (meth)acrylic monomer has a nitrogen-containing cyclic structure, the (meth)acrylic polymer is elastically elastic. An effect of improving the characteristics can be obtained.
  • the (meth)acrylic polymer is preferably crosslinked.
  • the adhesive may further include an active energy ray-curable resin (e.g., ultraviolet-curable resin) and a curing agent (e.g., photopolymerization initiator).
  • an active energy ray-curable resin e.g., ultraviolet-curable resin
  • a curing agent e.g., photopolymerization initiator
  • it may further contain a cured product of an active energy ray-curable resin. Active energy rays are visible light and ultraviolet rays, for example.
  • the deformation of the adhesive layer 20a over time can be suppressed. It is possible to prevent the adhesive layer 20a from changing over time to the extent that the adhesive layer 20a intrudes into the concave portion.
  • the adhesive layer 20a is hardened. If the adhesive layer 20a is too hard, it may become difficult to bond the adhesive layer 20a to the optical sheet 10a by a roll-to-roll method. This problem can be avoided by curing the active energy ray-curable resin at .
  • the adhesive layer 20a containing the cured product of the active energy ray-curable resin is formed, for example, by the following method.
  • an adhesive composition solution layer is formed from an adhesive composition solution containing a (meth)acrylic polymer, a cross-linking agent, an active energy ray-curable resin, a polymerization initiator, and a solvent.
  • the adhesive composition solution layer is formed, for example, on the release-treated major surface of the substrate.
  • the solvent in the adhesive composition solution layer is removed, and the (meth)acrylic polymer in the adhesive composition solution layer is crosslinked (for example, by heating) with a crosslinking agent, thereby forming an adhesive having a crosslinked structure.
  • a composition layer is obtained.
  • the adhesive composition solution layer is formed on the release-treated main surface of the substrate
  • the adhesive composition layer is formed on the release-treated main surface of the substrate, and the substrate and the adhesive composition A laminate having a layer is obtained.
  • the cross-linked structure formed by the (meth)acrylic polymer and the cross-linking agent is referred to as the first cross-linked structure. It is distinguished from a crosslinked structure (second crosslinked structure) formed by curing an active energy ray-curable resin, which will be described later.
  • the polymer of the adhesive composition solution layer may be crosslinked, or after the step of removing the solvent of the adhesive composition solution layer, the adhesive composition solution Aside from the step of removing the solvent from the layer, a step of cross-linking the polymer of the adhesive composition solution layer may be further performed.
  • the adhesive composition layer is attached onto the first main surface 12s of the optical sheet 10a, and the adhesive composition layer is placed on the first main surface 12s of the optical sheet 10a.
  • the adhesive layer 20a having the second crosslinked structure in addition to the first crosslinked structure can be formed.
  • the first crosslinked structure and the second crosslinked structure of the adhesive layer 20a are considered to form a so-called interpenetrating network structure (IPN).
  • IPN interpenetrating network structure
  • the adhesive layer 20a that does not contain the cured product of the active energy ray-curable resin is formed, for example, by the following method.
  • an adhesive composition solution layer is formed from an adhesive composition solution containing a polymer, a cross-linking agent and a solvent.
  • This adhesive composition solution does not contain an active energy ray-curable resin and a polymerization initiator.
  • the adhesive composition solution layer is formed, for example, on the release-treated major surface of the substrate.
  • the solvent in the adhesive composition solution layer is removed, and the polymer in the adhesive composition solution layer is crosslinked (for example, by heating) with a crosslinking agent to obtain an adhesive layer 20a having a crosslinked structure.
  • the adhesive layer is formed on the release-treated main surface of the substrate, the adhesive layer is formed on the release-treated main surface of the substrate, and has the substrate and the adhesive layer. A laminate is obtained.
  • the step of removing the solvent of the adhesive composition solution layer the polymer of the adhesive composition solution layer may be crosslinked, or after the step of removing the solvent of the adhesive composition solution layer, the adhesive composition solution Aside from the step of removing the solvent from the layer, a step of cross-linking the polymer of the adhesive composition solution layer may be further performed.
  • the adhesive preferably does not contain a graft polymer. If the adhesive layer is formed from an adhesive composition containing a graft polymer, as in the adhesive layer described in Patent Document 1, the number of design factors and control factors for the material increases, and mass productivity may be poor. Adhesives that do not contain a graft polymer can be adjusted in creep property by various factors (eg, type and amount of cross-linking agent, type and amount of actinic ray-curable resin).
  • the adhesive contains, for example, a (meth)acrylic polymer.
  • Any (meth)acrylate can be used as the monomer used for producing the (meth)acrylic polymer, and is not particularly limited.
  • an alkyl (meth)acrylate having an alkyl group with 4 or more carbon atoms can be used.
  • the ratio of the alkyl (meth)acrylate having an alkyl group with 4 or more carbon atoms to the total amount of monomers used for producing the (meth)acrylic polymer is, for example, 50% by mass or more.
  • Alkyl (meth)acrylate refers to a (meth)acrylate having a linear or branched alkyl group.
  • the number of carbon atoms in the alkyl group of the alkyl (meth)acrylate is preferably 4 or more, more preferably 4 or more and 9 or less.
  • (Meth)acrylate refers to acrylate and/or methacrylate.
  • alkyl (meth)acrylates include n-butyl (meth)acrylate, s-butyl (meth)acrylate, t-butyl (meth)acrylate, isobutyl (meth)acrylate, n-pentyl (meth)acrylate, isopentyl (meth) acrylate, hexyl (meth) acrylate, heptyl (meth) acrylate, isoamyl (meth) acrylate, 2-ethylhexyl (meth) acrylate, n-octyl (meth) acrylate, isooctyl (meth) acrylate, n-nonyl ( meth) acrylate, isononyl (meth) acrylate, n-decyl (meth) acrylate, isodecyl (meth) acrylate, n-dodecyl (meth) acrylate, isomy
  • the adhesive may contain a (meth)acrylic polymer that is a copolymer of a nitrogen-containing (meth)acrylic monomer and at least one other monomer.
  • the (meth)acrylic polymer is a copolymer obtained by copolymerizing the following monomers in the following amounts when the total amount of the monomers used in the copolymerization is 100 parts by mass. is preferred.
  • Nitrogen-containing (meth) acrylic monomer 10.0 parts by mass or more, 15.0 parts by mass or more, 20.0 parts by mass or more, 25.0 parts by mass or more, 30.0 parts by mass or more, or 35.0 parts by mass or more Yes, and 40.0 parts by mass or less, 35.0 parts by mass or less, 30.0 parts by mass or less, 25.0 parts by mass or less, 20.0 parts by mass or less, or 15.0 parts by mass or less.
  • hydroxyl group-containing acrylic monomer 0.05 parts by mass or more, 0.75 parts by mass or more, 1.0 parts by mass or more, 2.0 parts by mass or more, 3.0 parts by mass or more, 4.0 parts by mass or more; 0 parts by mass or more, 6.0 parts by mass or more, 7.0 parts by mass or more, 8.0 parts by mass or more, or 9.0 parts by mass or more, and 10.0 parts by mass or less and 9.0 parts by mass or less , 8.0 parts by mass or less, 7.0 parts by mass or less, 6.0 parts by mass or less, 5.0 parts by mass or less, 4.0 parts by mass or less, 3.0 parts by mass or less, 2.0 parts by mass or less, or 1.0 parts by mass or less.
  • Carboxyl group-containing acrylic monomer 1.0 parts by mass or more, 2.0 parts by mass or more, 3.0 parts by mass or more, 4.0 parts by mass or more, 5.0 parts by mass or more, 6.0 parts by mass or more;7. 0 parts by mass or more, 8.0 parts by mass or more, or 9.0 parts by mass or more, and 10.0 parts by mass or less, 9.0 parts by mass or less, 8.0 parts by mass or less, and 7.0 parts by mass or less , 6.0 parts by mass or less, 5.0 parts by mass or less, 4.0 parts by mass or less, 3.0 parts by mass or less, or 2.0 parts by mass or less.
  • Alkyl (meth)acrylate monomer (100 parts by mass) - (total amount of monomers other than alkyl (meth)acrylate monomer used for copolymerization)
  • the "nitrogen-containing (meth)acrylic monomer” includes, without particular limitation, a monomer having a polymerizable functional group having an unsaturated double bond of a (meth)acryloyl group and having a nitrogen atom.
  • a "nitrogen-containing (meth)acrylic monomer” has, for example, a nitrogen-containing cyclic structure.
  • nitrogen-containing (meth)acrylic monomers having a nitrogen-containing cyclic structure include, for example, N-vinyl-2-pyrrolidone (NVP), N-vinyl- ⁇ -caprolactam (NVC), 4-acryloylmorpholine (ACMO). be done. These can be used alone or in combination.
  • the "hydroxyl group-containing acrylic monomer” includes, without particular limitation, a monomer having a polymerizable functional group having an unsaturated double bond of a (meth)acryloyl group and having a hydroxyl group.
  • a monomer having a polymerizable functional group having an unsaturated double bond of a (meth)acryloyl group and having a hydroxyl group For example, 2-hydroxybutyl (meth)acrylate, 2-hydroxypropyl (meth)acrylate, 3-hydroxypropyl (meth)acrylate, 4-hydroxybutyl (meth)acrylate, 6-hydroxyhexyl (meth)acrylate, 8-hydroxy Hydroxyalkyl (meth)acrylates such as octyl (meth)acrylate, 10-hydroxydecyl (meth)acrylate, 12-hydroxylauryl (meth)acrylate; 4-hydroxymethylcyclohexyl (meth)acrylate, 4-hydroxybutyl vinyl ether, etc. be done.
  • carboxyl group-containing acrylic monomer refers to a monomer having a polymerizable functional group having an unsaturated double bond such as a (meth)acryloyl group or a vinyl group, and having a carboxyl group, without particular limitation.
  • unsaturated carboxylic acid-containing monomers include (meth)acrylic acid, carboxyethyl (meth)acrylate, carboxypentyl (meth)acrylate, itaconic acid, maleic acid, fumaric acid, and crotonic acid. These can be used alone or in combination.
  • the adhesive may contain a (meth)acrylic polymer that is a copolymer of a carboxyl group-containing acrylic monomer and at least one other monomer (excluding nitrogen-containing (meth)acrylic monomers).
  • the (meth)acrylic polymer is a copolymer obtained by copolymerizing the following monomers in the following amounts when the total amount of the monomers used in the copolymerization is 100 parts by mass. is preferred.
  • Carboxyl group-containing acrylic monomer 1.0 parts by mass or more, 2.0 parts by mass or more, 3.0 parts by mass or more, 4.0 parts by mass or more, 5.0 parts by mass or more, 6.0 parts by mass or more;7. 0 parts by mass or more, 8.0 parts by mass or more, or 9.0 parts by mass or more, and 10.0 parts by mass or less, 9.0 parts by mass or less, 8.0 parts by mass or less, and 7.0 parts by mass or less , 6.0 parts by mass or less, 5.0 parts by mass or less, 4.0 parts by mass or less, 3.0 parts by mass or less, or 2.0 parts by mass or less.
  • Alkyl (meth)acrylate monomer 90.0 parts by mass or more, 91.0 parts by mass or more, 92.0 parts by mass or more, 93.0 parts by mass or more, 94.0 parts by mass or more, 95.0 parts by mass or more, 96 .0 parts by mass or more, 97.0 parts by mass or more, or 98.0 parts by mass or more, and 99.0 parts by mass or less, 98.0 parts by mass or less, 97.0 parts by mass or less, and 96.0 parts by mass or less , 95.0 parts by mass or less, 94.0 parts by mass or less, 93.0 parts by mass or less, 92.0 parts by mass or less, or 91.0 parts by mass or less.
  • Crosslinking agents that introduce a crosslinked structure into (meth)acrylic polymers include isocyanate crosslinkers, epoxy crosslinkers, silicone crosslinkers, oxazoline crosslinkers, aziridine crosslinkers, silane crosslinkers, and alkyl ethers.
  • cross-linking agents such as melamine-based cross-linking agents, metal chelate-based cross-linking agents, and peroxides.
  • the cross-linking agents can be used singly or in combination of two or more.
  • An isocyanate-based cross-linking agent refers to a compound having two or more isocyanate groups (including isocyanate-regenerative functional groups in which isocyanate groups are temporarily protected by blocking agents or quantization) in one molecule.
  • isocyanate-based cross-linking agents examples include aromatic isocyanates such as tolylene diisocyanate and xylene diisocyanate, alicyclic isocyanates such as isophorone diisocyanate, and aliphatic isocyanates such as hexamethylene diisocyanate.
  • lower aliphatic polyisocyanates such as butylene diisocyanate and hexamethylene diisocyanate
  • alicyclic isocyanates such as cyclopentylene diisocyanate, cyclohexylene diisocyanate and isophorone diisocyanate
  • 2,4-tolylene diisocyanate Aromatic diisocyanates such as 4,4′-diphenylmethane diisocyanate, xylylene diisocyanate, polymethylene polyphenyl isocyanate, trimethylolpropane/tolylene diisocyanate trimer adduct (manufactured by Tosoh Corporation, trade name Coronate L), trimethylol Propane/hexamethylene diisocyanate trimer adduct (manufactured by Tosoh Corporation, trade name Coronate HL), isocyanate adducts such as hexamethylene diisocyanate isocyanur
  • the isocyanate-based cross-linking agents may be used singly or in combination of two or more.
  • the amount of the isocyanate-based crosslinking agent is, for example, 0.01 parts by mass or more, 0.02 parts by mass or more, 0.05 parts by mass or more, or 0.1 parts by mass or more with respect to 100 parts by mass of the (meth)acrylic polymer. and 10 parts by mass or less, 9 parts by mass or less, 8 parts by mass or less, 7 parts by mass or less, 6 parts by mass or less, or 5 parts by mass or less, preferably 0.01 parts by mass or more and 10 parts by mass or less , 0.02 to 9 parts by mass, and 0.05 to 8 parts by mass.
  • the blending amount may be appropriately adjusted in consideration of cohesive strength, prevention of peeling in a durability test, and the like.
  • Epoxy-based cross-linking agents are polyfunctional epoxy compounds that have two or more epoxy groups in one molecule.
  • Epoxy crosslinking agents include, for example, bisphenol A, epichlorohydrin type epoxy resin, ethylene glycidyl ether, N,N,N',N'-tetraglycidyl-m-xylenediamine, diglycidylaniline, diamineglycidylamine, 1 ,3-bis(N,N-diglycidylaminomethyl)cyclohexane, 1,6-hexanediol diglycidyl ether, neopentyl glycol diglycidyl ether, ethylene glycol diglycidyl ether, propylene glycol diglycidyl ether, polyethylene glycol diglycidyl ether , polypropylene glycol diglycidyl ether, sorbitol polyglycidyl ether, glycerol polyglycidyl ether, penta
  • Epoxy-based cross-linking agents may be used singly or in combination of two or more.
  • the amount of the epoxy crosslinking agent is, for example, 0.01 parts by mass or more, 0.02 parts by mass or more, 0.05 parts by mass or more, or 0.1 parts by mass or more with respect to 100 parts by mass of the (meth)acrylic polymer. and 10 parts by mass or less, 9 parts by mass or less, 8 parts by mass or less, 7 parts by mass or less, 6 parts by mass or less, or 5 parts by mass or less, preferably 0.01 parts by mass or more and 10 parts by mass or less , 0.02 to 9 parts by mass, and 0.05 to 8 parts by mass.
  • the blending amount may be appropriately adjusted in consideration of cohesive strength, prevention of peeling in a durability test, and the like.
  • Any peroxide cross-linking agent that generates radical active species upon heating and promotes cross-linking of the base polymer of the pressure-sensitive adhesive can be used as appropriate. It is preferable to use a peroxide having a 1-minute half-life temperature of 80° C. or higher and 160° C. or lower, more preferably 90° C. or higher and 140° C. or lower.
  • Peroxides include, for example, di(2-ethylhexyl) peroxydicarbonate (1 minute half-life temperature: 90.6° C.), di(4-t-butylcyclohexyl) peroxydicarbonate (1 minute half-life temperature : 92.1°C), di-sec-butyl peroxydicarbonate (1-minute half-life temperature: 92.4°C), t-butyl peroxyneodecanoate (1-minute half-life temperature: 103.5°C) , t-hexyl peroxypivalate (1 minute half-life temperature: 109.1 ° C.), t-butyl peroxypivalate (1 minute half-life temperature: 110.3 ° C.), dilauroyl peroxide (1 minute half-life temperature: 116.4 ° C.), di-n-octanoyl peroxide (1 minute half-life temperature: 117.4 ° C.), 1,1,3,3-tetramethylbutylperoxy-2-e
  • di(4-t-butylcyclohexyl)peroxydicarbonate (1-minute half-life temperature: 92.1° C.) and dilauroyl peroxide (1-minute half-life temperature: 116.0° C.) are particularly effective in cross-linking reaction efficiency. 4° C.), dibenzoyl peroxide (1-minute half-life temperature: 130.0° C.), and the like are preferably used.
  • the half-life of peroxide is an index that expresses the decomposition rate of peroxide, and refers to the time until the remaining amount of peroxide is halved.
  • the decomposition temperature for obtaining a half-life at an arbitrary time and the half-life time at an arbitrary temperature are described in manufacturer catalogs. For example, NOF Corporation's "Organic Peroxide Catalog 9th Edition ( May 2003)”.
  • Peroxides may be used singly or in combination of two or more.
  • the amount of the peroxide compounded is 0.02 parts by mass or more and 2 parts by mass or less, preferably 0.05 parts by mass or more and 1 part by mass or less, relative to 100 parts by mass of the (meth)acrylic polymer. In order to adjust workability, reworkability, crosslink stability, peelability, etc., it is appropriately adjusted within this range.
  • the residual peroxide decomposition amount after the reaction treatment for example, it can be measured by HPLC (high performance liquid chromatography).
  • an organic cross-linking agent or a polyfunctional metal chelate may be used in combination.
  • Polyfunctional metal chelates are those in which polyvalent metals are covalently or coordinately bonded to organic compounds.
  • Polyvalent metal atoms include Al, Cr, Zr, Co, Cu, Fe, Ni, V, Zn, In, Ca, Mg, Mn, Y, Ce, Sr, Ba, Mo, La, Sn, and Ti. mentioned.
  • Atoms in organic compounds that form covalent bonds or coordinate bonds include oxygen atoms, and examples of organic compounds include alkyl esters, alcohol compounds, carboxylic acid compounds, ether compounds, and ketone compounds.
  • the blending amount of the active energy ray-curable resin is, for example, 3 parts by mass or more and 60 parts by mass or less with respect to 100 parts by mass of the (meth)acrylic polymer.
  • the weight average molecular weight (Mw) before curing is 4000 or more and 50000 or less.
  • the active energy ray-curable resin for example, an acrylate-based, epoxy-based, urethane-based, or en-thiol-based UV-curable resin can be preferably used.
  • active energy ray-curable resin monomers and/or oligomers that undergo radical polymerization or cationic polymerization by active energy rays are used.
  • Monomers that are radically polymerized by active energy rays include monomers having unsaturated double bonds such as (meth)acryloyl groups and vinyl groups. Monomers having (meth)acryloyl groups are particularly preferred because of their excellent reactivity. be done.
  • monomers having a (meth)acryloyl group include allyl (meth)acrylate, caprolactone (meth)acrylate, cyclohexyl (meth)acrylate, N,N-diethylaminoethyl (meth)acrylate, 2-ethylhexyl (Meth)acrylate, heptadecafluorodecyl (meth)acrylate, glycidyl (meth)acrylate, caprolactone-modified 2-hydroxylethyl (meth)acrylate, isobornyl (meth)acrylate, morpholine (meth)acrylate, phenoxyethyl (meth)acrylate - tripropylene glycol di (meth) acrylate, bisphenol A diglycidyl ether di (meth) acrylate, neopentyl hydroxypivalate glycol di (meth) acrylate, trimethylolpropane tri (meth) acrylate, tri
  • Oligomers that are radically polymerized by active energy rays include polyesters ( Meth)acrylate, epoxy (meth)acrylate, urethane (meth)acrylate and the like are used.
  • Polyester (meth) acrylate is obtained by reacting (meth) acrylic acid with a polyester having a terminal hydroxyl group obtained from a polyhydric alcohol and a polycarboxylic acid, and a specific example is Aronix M- 6000, 7000, 8000, 9000 series and the like.
  • Epoxy (meth)acrylate is obtained by reacting (meth)acrylic acid with epoxy resin, and specific examples include Lipoxy SP and VR series manufactured by Showa Polymer Co., Ltd. and epoxy ester manufactured by Kyoeisha Chemical Co., Ltd. series and the like.
  • Urethane (meth)acrylate is obtained by reacting polyol, isocyanate, and hydroxy (meth)acrylate.
  • Specific examples include the Artresin UN series manufactured by Neagari Kogyo Co., Ltd., and NK manufactured by Shin-Nakamura Chemical Co., Ltd. Oligo U series, Mitsubishi Chemical Corporation Shikou UV series, and the like can be mentioned.
  • the photopolymerization initiator has the effect of generating radicals by being excited and activated by irradiation with ultraviolet rays, and curing the polyfunctional oligomer through radical polymerization.
  • the polymerization initiator is preferably added in an amount of 0.5 to 30 parts by mass, more preferably 1 to 20 parts by mass, per 100 parts by mass of the active energy ray-curable resin. If the amount is less than 0.5 parts by mass, the polymerization does not proceed sufficiently, resulting in a slow curing rate. If the amount exceeds 30 parts by mass, the hardness of the cured sheet may decrease.
  • the active energy ray is not particularly limited, ultraviolet rays, visible light, and electron beams are preferred.
  • the cross-linking treatment by ultraviolet irradiation can be performed using an appropriate ultraviolet light source such as a high-pressure mercury lamp, a low-pressure mercury lamp, an excimer laser, a metal halide lamp, and an LED lamp.
  • the irradiation dose of ultraviolet rays can be appropriately selected according to the required degree of cross - linking. It is desirable to
  • the temperature during irradiation is not particularly limited, but is preferably up to about 140° C. in consideration of the heat resistance of the support.
  • the adhesive contains a polyester polymer in place of the (meth)acrylic polymer or together with the (meth)acrylic polymer, a polyester polymer having the following characteristics, for example, is preferable.
  • Type of carboxylic acid component (or characteristics of skeleton, etc.): containing at least dicarboxylic acid containing two carboxyl groups, specifically dicarboxylic acid.
  • dicarboxylic acid include, but are not limited to, dimer acids derived from sebacic acid, oleic acid and erucic acid.
  • Other examples include glutaric acid, suberic acid, adipic acid, azelaic acid, 1,4-cyclohexanedicarboxylic acid, 4-methyl-1,2-cyclohexanedicarboxylic acid, dodecenyl succinic anhydride, fumaric acid, succinic acid, dodecane.
  • Aliphatic or alicyclic dicarboxylic acids such as diacids, hexahydrophthalic anhydride, tetrahydrophthalic anhydride, maleic acid, maleic anhydride, itaconic acid, citraconic acid, terephthalic acid, isophthalic acid, orthophthalic acid, 1,5- naphthalenedicarboxylic acid, 2,6-naphthalenedicarboxylic acid, 4,4'-diphenyldicarboxylic acid, 2,2'-diphenyldicarboxylic acid and 4,4'-diphenyletherdicarboxylic acid.
  • dicarboxylic acids tricarboxylic acids containing 3 or more carboxyl groups can also be used.
  • Type of diol component (or skeleton characteristics, etc.): containing at least two hydroxyl groups in the molecule, specifically diol.
  • Others include aliphatic glycols such as ethylene glycol and 1,2-propylene glycol, ethylene oxide adducts and propylene oxide adducts of bisphenol A, and ethylene oxide additions of hydrogenated bisphenol A as non-aliphatic glycols. and propylene oxide adducts.
  • an isocyanate-based cross-linking agent As the cross-linking agent for introducing a cross-linked structure into the polyester polymer, an isocyanate-based cross-linking agent, an oxazoline-based cross-linking agent, an aziridine-based cross-linking agent, a silane-based cross-linking agent, an alkyl-etherified melamine-based cross-linking agent, and a metal chelate-based cross-linking agent are used. be able to.
  • the blending amount is, for example, 2.0 parts by mass or more and 10.0 parts by mass or less with respect to 100 parts by mass of the polyester polymer.
  • composition of the adhesive layer Ac will be described below.
  • polyvalent carboxylic acids include aromatic dicarboxylic acids such as terephthalic acid, isophthalic acid, benzylmalonic acid, diphenic acid, 4,4'-oxydibenzoic acid, and naphthalene dicarboxylic acid; Malonic acid, dimethylmalonic acid, succinic acid, glutaric acid, adipic acid, trimethyladipic acid, pimelic acid, 2,2-dimethylglutaric acid, azelaic acid, sebacic acid, fumaric acid, maleic acid, itaconic acid, thiodipropionic acid , aliphatic dicarboxylic acids such as diglycolic acid; Alicyclic groups such as 1,3-cyclopentanedicarboxylic acid, 1,2-cyclohexanedicarboxylic acid, 1,3-cyclopentanedicarboxylic acid, 1,4-cyclohexanedicarboxylic acid, 2,5-n
  • an aromatic dicarboxylic acid from the viewpoint of imparting cohesive force, it is preferable to contain an aromatic dicarboxylic acid, and it is particularly preferable to contain terephthalic acid or isophthalic acid.
  • polyhydric alcohols include Ethylene glycol, diethylene glycol, triethylene glycol, propylene glycol, dipropylene glycol, 1,3-propanediol, 2,4-dimethyl-2-ethylhexane-1,3-diol, 2-methyl-1,3-propanediol , 2,2-dimethyl-1,3-propanediol (neopentyl glycol), 2-ethyl-2-butyl-1,3-propanediol, 2-ethyl-2-isobutyl-1,3-propanediol, 1 ,3-butanediol, 1,4-butanediol, 1,5-pentanediol, 1,6-hexanediol, 3-methyl-1,5-pentanediol, 2,2,4-trimethyl-1,6- Aliphatic diols such as hexane
  • it preferably contains an aliphatic diol or an alicyclic diol, and more preferably contains polytetramethylene glycol, neopentyl glycol or cyclohexanedimethanol.
  • the cross-linking agent is not particularly limited, and known ones can be used. Oxazoline compounds, polyfunctional aziridine compounds, metal chelate compounds, and the like can be used. In particular, it is preferable to use an isocyanate-based cross-linking agent from the viewpoint of obtaining the transparency of the adhesive layer to be obtained and the elastic modulus suitable for the adhesive layer.
  • An isocyanate-based cross-linking agent refers to a compound having two or more isocyanate groups (including isocyanate-regenerative functional groups in which isocyanate groups are temporarily protected by blocking agents or quantization) in one molecule.
  • isocyanate-based cross-linking agents examples include aromatic isocyanates such as tolylene diisocyanate and xylene diisocyanate, alicyclic isocyanates such as isophorone diisocyanate, and aliphatic isocyanates such as hexamethylene diisocyanate.
  • lower aliphatic polyisocyanates such as butylene diisocyanate and hexamethylene diisocyanate
  • alicyclic isocyanates such as cyclopentylene diisocyanate, cyclohexylene diisocyanate and isophorone diisocyanate
  • 2,4-tolylene diisocyanate Aromatic diisocyanates such as 4,4′-diphenylmethane diisocyanate, xylylene diisocyanate, polymethylene polyphenyl isocyanate, trimethylolpropane/tolylene diisocyanate trimer adduct (manufactured by Tosoh Corporation, trade name Coronate L), trimethylol Propane/hexamethylene diisocyanate trimer adduct (manufactured by Tosoh Corporation, trade name Coronate HL), isocyanate adducts such as hexamethylene diisocyanate isocyanur
  • the isocyanate-based cross-linking agents may be used singly or in combination of two or more.
  • the lower limit of the amount of the isocyanate-based cross-linking agent is 6 parts by mass or more, preferably 7 parts by mass or more, 8 parts by mass or more, 9 parts by mass or more, or 10 parts by mass or more with respect to 100 parts by mass of the polyester resin.
  • the upper limit of the amount of the system crosslinking agent is 20 parts by mass or less, preferably 15 parts by mass or less. Within this range, it is possible to prevent the adhesive layer from penetrating into the recesses of the uneven structure over time while maintaining good adhesion to the surface having the uneven structure.
  • Organic aluminum compounds include aluminum trisacetylacetonate, aluminum trisethylacetoacetate, diisopropoxyaluminumethylacetoacetate and the like.
  • organic iron compounds examples include acetylacetone-iron complexes.
  • organic zirconium compounds examples include zirconium tetraacetylacetonate.
  • the cross-linking speed can be increased and the production lead time can be shortened.
  • an adhesive composition layer is formed by applying (coating) an adhesive composition (or a solution containing the adhesive composition) onto a support (substrate) and drying if necessary.
  • an adhesive composition solution layer is formed on a substrate by applying an adhesive composition solution containing a polyester resin, a cross-linking agent, a cross-linking catalyst, and a solvent onto the substrate, and the adhesive composition is An adhesive composition layer is obtained by removing the solvent of the product solution layer.
  • the adhesive composition layer is subjected to cross-linking treatment (for example, heat treatment) to cross-link the polyester resin of the adhesive composition layer with a cross-linking agent, thereby forming an adhesive layer having a cross-linked structure.
  • cross-linking treatment for example, heat treatment
  • an adhesive layer is formed on the substrate, and a laminate having the substrate and the adhesive layer is obtained.
  • a substrate a substrate having a release-treated major surface, such as a release liner, may be used.
  • the adhesive layer formed on the release liner by the above method may be transferred (transferred) onto a support (or another release liner).
  • a known method can be employed as a method for applying the adhesive composition (adhesive composition solution) onto the substrate. Examples thereof include roll coating, gravure coating, reverse roll coating, roll brush coating, air knife coating, spray coating, and extrusion coating using a die coater.
  • the light guide layer 80 can be made of a known material with high visible light transmittance.
  • the light guide layer 80 is made of, for example, acrylic resin such as polymethyl methacrylate (PMMA), polycarbonate (PC) resin, cycloolefin resin, or glass (for example, quartz glass, alkali-free glass, or borosilicate glass). be.
  • the refractive index n GP of the light guide layer 80 is, for example, 1.40 or more and 1.80 or less. Unless otherwise specified, the refractive index refers to the refractive index measured with an ellipsometer at a wavelength of 550 nm.
  • the thickness of the light guide layer 80 can be appropriately set according to the application.
  • the thickness of the light guide layer 80 is, for example, 0.05 mm or more and 50 mm or less.
  • the first optical sheet 10a can be produced, for example, by the method described in JP-T-2013-524288. Specifically, for example, the surface of a polymethyl methacrylate (PMMA) film is coated with a lacquer (for example, Fine Cure RM-64 manufactured by Sanyo Chemical Industries, Ltd.: an acrylate-based photocurable resin), and the film surface containing the lacquer
  • a lacquer for example, Fine Cure RM-64 manufactured by Sanyo Chemical Industries, Ltd.: an acrylate-based photocurable resin
  • the first optical sheet 10a can be made by embossing an optical pattern thereon and then curing the lacquer (for example, UV irradiation conditions: D bulb, 1000 mJ/cm 2 , 320 mW/cm 2 ).
  • Materials for the second optical sheet 30 include, for example, thermoplastic resins having optical transparency, and more specifically, for example, (meth)acrylic resins such as polymethyl methacrylate (PMMA), or polycarbonates.
  • PMMA polymethyl methacrylate
  • a film formed of a (PC)-based resin or the like can be mentioned. Any appropriate material can be adopted for the second optical sheet 30 depending on the purpose.
  • the thickness of the base material layer is, for example, 1 ⁇ m or more and 1000 ⁇ m or less, preferably 10 ⁇ m or more and 100 ⁇ m or less, and more preferably 20 ⁇ m or more and 80 ⁇ m or less.
  • the refractive index of the substrate layer is preferably 1.40 or more and 1.70 or less, more preferably 1.43 or more and 1.65 or less.
  • the refractive index n L1 of each of the low refractive index layers is, for example, preferably 1.30 or less, more preferably 1.20 or less, and even more preferably 1.15 or less.
  • the low refractive index layer is preferably solid, and preferably has a refractive index of, for example, 1.05 or more.
  • the difference between the refractive index of the light guide layer 80 and the refractive index layer of the low refractive index layer is preferably 0.20 or more, more preferably 0.23 or more, and still more preferably 0.25 or more.
  • a low refractive index layer having a refractive index of 1.30 or less can be formed using, for example, a porous material.
  • the thickness of each low refractive index layer is, for example, 0.3 ⁇ m or more and 5 ⁇ m or less.
  • the porosity is preferably 35% by volume or more, more preferably 38% by volume or more, and particularly preferably 40% by volume or more. . Within such a range, a low refractive index layer having a particularly low refractive index can be formed.
  • the upper limit of the porosity of the low refractive index layer is, for example, 90% by volume or less, preferably 75% by volume or less. Within such a range, a low refractive index layer having excellent strength can be formed.
  • the porosity is a value calculated from the value of the refractive index measured by an ellipsometer using the Lorentz-Lorenz's formula.
  • the low refractive index layer for example, a voided low refractive index layer disclosed in International Publication No. 2019/146628 can be used.
  • the entire disclosure of WO2019/146628 is incorporated herein by reference.
  • the low refractive index layer having voids includes substantially spherical particles such as silica particles, silica particles having micropores, and hollow silica nanoparticles; fibrous particles such as cellulose nanofibers, alumina nanofibers, and silica nanofibers; It includes tabular particles such as nanoclays composed of bentonite.
  • the low refractive index layer having voids is a porous body formed by directly chemically bonding particles (for example, microporous particles) to each other.
  • the particles constituting the low refractive index layer having voids may be bonded together via a small amount (for example, the mass of the particles or less) of one component of the binder.
  • the porosity and refractive index of the low refractive index layer can be adjusted by the particle size, particle size distribution, etc. of the particles forming the low refractive index layer.
  • Methods for obtaining a low refractive index layer having voids include, for example, JP-A-2010-189212, JP-A-2008-040171, JP-A-2006-011175, International Publication No. 2004/113966, and their Methods described in ref. All of the disclosures of JP-A-2010-189212, JP-A-2008-040171, JP-A-2006-011175, and International Publication No. 2004/113966 are incorporated herein by reference.
  • a silica porous material can be preferably used as the low refractive index layer having voids.
  • a silica porous body is produced, for example, by the following method. a silicon compound; hydrolyzable silanes and/or silsesquioxane, and a method of hydrolyzing and polycondensing at least one of its partial hydrolyzate and dehydration condensate; porous particles and/or hollow fine particles; method, method of generating an airgel layer using the springback phenomenon, pulverizing the gel-like silicon compound obtained by the sol-gel method, and chemically pulverizing the resulting pulverized microporous particles with a catalyst or the like. and a method using a combined pulverized gel.
  • the low refractive index layer is not limited to the porous silica material, nor is the manufacturing method limited to the exemplified manufacturing method, and may be manufactured by any manufacturing method.
  • the porous layer is not limited to the silica porous body, and the manufacturing method is not limited to the exemplified manufacturing method, and may be manufactured by any manufacturing method.
  • Silsesquioxane is a silicon compound having (RSiO 1.5 , R is a hydrocarbon group) as a basic structural unit, and is strictly different from silica having SiO 2 as a basic structural unit.
  • a porous material containing silsesquioxane as a basic structural unit is also referred to herein as a silica porous material or a silica-based porous material, since it has a network structure crosslinked with silica in common.
  • the silica porous body can be composed of microporous particles of a gel-like silicon compound bonded together.
  • pulverized bodies of the gelled silicon compound can be mentioned.
  • the silica porous body can be formed, for example, by coating a base material with a coating liquid containing a pulverized gel-like silicon compound.
  • the pulverized gel-like silicon compound can be chemically bonded (for example, siloxane bond) by the action of a catalyst, light irradiation, heating, or the like.
  • Example 1 (1) Preparation of polyester resin A A four-necked separable flask was equipped with a stirrer, a thermometer, a nitrogen inlet tube, and a cooling tube with a trap. 45 g of isophthalic acid (molecular weight: 166), and as alcohol components, 115 g of polytetramethylene glycol (molecular weight: 566), 4 g of ethylene glycol (molecular weight: 62), 16 g of neopentyl glycol (molecular weight: 104) and 23 g of cyclohexanedimethanol (molecular weight: 104). : 144), 0.1 g of tetrabutyl titanate was added as a catalyst, and the temperature was raised to 240°C while stirring while filling the flask with nitrogen gas, and the temperature was maintained at 240°C for 4 hours.
  • polyester resin A was obtained. Polyester resin A was obtained by polymerizing the above monomers without using a solvent. The mass average molecular weight (Mw) of polyester resin A measured by GPC was 59,200. The prepared polyester resin A was dissolved in ethyl acetate and removed from the flask to prepare a polyester resin A solution having a solid content concentration of 50% by mass.
  • Adhesive Sheet The adhesive composition solution was applied to one side of the base material (first separator) subjected to silicone release treatment to form an adhesive composition solution layer.
  • a polyethylene terephthalate (PET) film with a thickness of 38 ⁇ m (trade name “MRF38”, manufactured by Mitsubishi Chemical Corporation) was used as the first separator.
  • the thickness of the adhesive composition solution layer was such that the thickness of the adhesive layer after the following step of treatment at 40° C. for 3 days was 10 ⁇ m.
  • the solvent in the adhesive composition solution layer was removed to obtain an adhesive composition layer.
  • the adhesive composition layer was attached to the release-treated surface of another substrate (second separator) that had been subjected to silicone release treatment, and left at 40° C. for 3 days.
  • second separator a 75 ⁇ m-thick biaxially oriented polyethylene terephthalate film (manufactured by Mitsubishi Chemical Corporation, trade name: Diafoil T302, hereinafter sometimes referred to as “T302”) was used.
  • the adhesive composition layer was treated at 40° C. for 3 days to crosslink the polyester resin A of the adhesive composition layer with a crosslinking agent to form an adhesive layer.
  • an adhesive sheet (laminate) having a laminated structure of first separator (PET film)/adhesive layer/second separator (PET film) was produced.
  • the cross-linking reaction of the polyester resin A may partially occur even in the step of treating the adhesive composition solution layer at 150° C. for 1 minute, but most of the cross-linking reaction occurs in the subsequent step of heat treatment at 40° C. for 3 days.
  • unevenness-shaped film A was produced according to the method described in JP-T-2013-524288. Specifically, the surface of a polymethyl methacrylate (PMMA) film is coated with a lacquer (manufactured by Sanyo Chemical Industries, Ltd., Fine Cure RM-64), and an optical pattern is embossed on the film surface containing the lacquer, After that, the lacquer was cured to produce the intended irregular shaped film.
  • the unevenness-shaped film A had a total thickness of 130 ⁇ m and a haze value of 0.8%.
  • FIG. 9B shows a 9B-9B′ cross-sectional view of the irregular shaped film 70 of FIG. 9A.
  • a plurality of concave portions 74 having a triangular cross section and having a length L of 86 ⁇ m, a width W of 9.2 ⁇ m, and a depth H of 10 ⁇ m were arranged at intervals of a width E (155 ⁇ m) in the X-axis direction. Furthermore, such a pattern of recesses 74 was arranged at intervals of width D (100 ⁇ m) in the Y-axis direction.
  • the density of the concave portions 74 on the concave-convex shaped film surface was 3612/cm 2 .
  • the inclination angle ⁇ a in FIG. 9B was 49°, the inclination angle ⁇ b was 85°, and the occupied area ratio Rr of the concave portions 74 when the film was viewed from the uneven surface side was 4.05%.
  • the adhesive sheet obtained in (3) above that is, the laminate having a laminated structure of the first separator/adhesive layer/second separator
  • one main surface of the adhesive layer is covered with the first separator
  • the other main surface of the adhesive layer is bonded to the release-treated surface of the second separator.
  • the first separator was peeled off from the adhesive sheet obtained in (3) above, and the surface (one main surface) of the exposed adhesive layer was driven into an acrylic resin film (thickness: 30 ⁇ m).
  • a laminate having a laminate structure of acrylic resin film/adhesive layer/second separator was obtained by laminating between a nip roller including a roll and a driven roll.
  • the second separator is peeled off from the obtained laminate, and the surface of the exposed adhesive layer (the other main surface) is applied to the surface having the uneven structure of the uneven structure-imparted film A of (4). , and laminated between nip rollers including a drive roll and a driven roll to obtain an optical laminate having a laminated structure of acrylic resin film/adhesive layer/concavo-convex shaping film A.
  • the nip pressure between the nip rollers including the drive roll and the driven roll was as shown in Tables 1A to 1C. As a result, a long optical laminate with a width of 300 mm having a laminate structure of acrylic resin film/adhesive layer/concavo-convex shaping film A was obtained.
  • the main surface of the adhesive layer which had been bonded to the release-treated surface of the second separator, is bonded to the surface of the concave-convex shaped film A having the concave-convex structure.
  • the release-treated surface of T302 used as the second separator had an arithmetic mean roughness Ra of 0.02 ⁇ m and a maximum height Rz of 0.15 ⁇ m.
  • Example 2 An optical laminate was produced in the same manner as in Example 1, except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 3 Optical laminates were produced in the same manner as in Example 2, except that the nip pressure between the nip rollers and the type of the second separator were changed as shown in Tables 1A to 1C.
  • the second separator PET film
  • the separator to be bonded to the main surface of the adhesive layer to be bonded to the irregular shaped film A was a commercially available ultra-high 38 ⁇ m thick separator.
  • a retardation polyethylene terephthalate film manufactured by Mitsubishi Chemical Corporation, trade name: Diafoil MRF38CK
  • 38CK Diafoil MRF38CK
  • the release-treated surface of 38CK used as the second separator had an arithmetic mean roughness Ra of 0.01 ⁇ m and a maximum height Rz of 0.10 ⁇ m.
  • Example 4 An optical layered body was produced in the same manner as in Example 3, except that the unevenness-shaping film B was used instead of the unevenness-shaping film A.
  • FIG. 14A shows a plan view of a part of the unevenness-forming film B used as an unevenness-forming film 52 as viewed from the uneven surface side.
  • 14B shows a cross-sectional view taken along line 14B-14B' in FIG. 14A.
  • the concave portions 54 of the concave-convex shaped film 52 are continuous in the X direction (grooves extending in the X direction) and arranged at predetermined intervals in the Y direction.
  • the cross-sectional shape of the concave portion 54 is a triangle with a depth H of 6.78 ⁇ m, a maximum width of 6.5 ⁇ m, an inclination angle ⁇ a of 50°, and an inclination angle ⁇ b of 85°.
  • the width of the concave portion 54 changes at a period of 17 ⁇ m.
  • the concave portions 54 are arranged so as to protrude toward the light source in plan view.
  • Example 5 An optical laminate was produced in the same manner as in Example 4, except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 6 An optical laminate was produced in the same manner as in Example 2, except that the following adhesive layer was used.
  • the adhesive layer was produced as follows.
  • the liquid temperature in the flask was maintained at around 58°C and the polymerization reaction was carried out for 8 hours.
  • a system polymer was obtained.
  • ethyl acetate was added dropwise over 3 hours so that the solid content reached 35% by mass. That is, the acrylic polymer was obtained as an acrylic polymer solution having a solid content of 35% by mass.
  • UV curable urethane acrylate resin A (mass average molecular weight Mw: 5,500) was added to the obtained acrylic polymer solution with respect to 100 parts by mass of the polymer. 10 parts by mass of solid content, 1.0 parts by mass of 4-(2-hydroxyethoxy)phenyl (2-hydroxy-2-propyl) ketone (trade name “Omnirad2959”, manufactured by IGM Japan LLC) as a photopolymerization initiator.
  • Adhesive Sheet Acrylic adhesive composition solution A was applied to one side of a polyethylene terephthalate (PET) film (trade name “MRF38”, manufactured by Mitsubishi Chemical Corporation) having a thickness of 38 ⁇ m that had been subjected to silicone release treatment. to form an adhesive composition solution layer.
  • PET polyethylene terephthalate
  • MRF38 manufactured by Mitsubishi Chemical Corporation
  • the adhesive composition solution layer was applied so that the thickness after drying (that is, the thickness of the adhesive composition layer) was 5 ⁇ m.
  • the solvent in the adhesive composition solution layer is removed and the acrylic polymer is crosslinked with the cross-linking agent to form the acrylic polymer and the cross-linking agent.
  • An adhesive layer having a crosslinked structure was obtained.
  • the adhesive layer was obtained without curing the ultraviolet curable resin of the adhesive composition solution.
  • the obtained adhesive layer does not have a crosslinked structure formed by curing the ultraviolet curable resin.
  • the adhesive composition layer was laminated to the release-treated surface of a 38 ⁇ m-thick polyethylene terephthalate (PET) film (trade name “MRE38”, manufactured by Mitsubishi Chemical Corporation) that had been subjected to silicone release treatment, thereby forming a PET film/adhesive layer.
  • PET polyethylene terephthalate
  • An optical laminate was produced in the same manner as in Example 2 using the adhesive sheet obtained in (3) above.
  • Example 7 An optical laminate was produced in the same manner as in Example 6 except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 8 An optical laminate was produced in the same manner as in Example 7 except that the nip pressure between the nip rollers was changed as shown in Tables 1A to 1C.
  • Example 9 Optical laminates were produced in the same manner as in Example 6, except that the nip pressure between the nip rollers was changed as shown in Tables 1A to 1C.
  • Example 10 An optical laminate was produced in the same manner as in Example 9, except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 11 An optical laminate was produced in the same manner as in Example 9, except that the unevenness-forming film B was used instead of the unevenness-forming film A.
  • Example 12 An optical laminate was produced in the same manner as in Example 11 except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 13 (1) Preparation of Acrylic Polymer Solution First, an acrylic polymer was prepared. 90.7 parts by mass of n-butyl acrylate (BA), 6.3 parts by mass of 4-acryloylmorpholine (ACMO), acrylic acid, and (AA) 2.7 parts by mass, 0.3 parts by mass of 4-hydroxybutyl acrylate (4HBA), 0.1 parts by mass of 2,2'-azobisisobutyronitrile as a polymerization initiator, and the total amount of monomers is 50 parts by mass. %, and nitrogen gas was introduced while gently stirring to replace nitrogen gas for 1 hour. Then, the liquid temperature in the flask was maintained at around 58°C and the polymerization reaction was carried out for 8 hours. A system polymer was obtained.
  • BA n-butyl acrylate
  • ACMO 4-acryloylmorpholine
  • acrylic acid acrylic acid
  • AA 2.7 parts by mass
  • 4HBA 4-hydroxybutyl acrylate
  • 4HBA 4-hydroxybutyl acrylate
  • the acrylic polymer was obtained as an acrylic polymer solution having a solid content of 35% by mass.
  • Adhesive Composition Solution To the obtained acrylic polymer solution, 1,3-bis(N,N-diglycidylaminomethyl) as a cross-linking agent is added to 100 parts by mass of the solid content (polymer).
  • an adhesive composition solution (sometimes referred to as “acrylic adhesive composition solution B”) containing 0.1 part by mass of cyclohexane (trade name “TETRAD-C”, manufactured by Mitsubishi Gas Chemical Co., Ltd.) did.
  • Adhesive Sheet Acrylic adhesive composition solution B was applied to one side of a polyethylene terephthalate (PET) film (trade name “MRF38”, manufactured by Mitsubishi Chemical Corporation) having a thickness of 38 ⁇ m that had been subjected to silicone release treatment. to form an adhesive composition solution layer.
  • PET polyethylene terephthalate
  • MRF38 manufactured by Mitsubishi Chemical Corporation
  • the adhesive composition solution layer was applied so that the thickness after drying (that is, the thickness of the adhesive composition layer) was 5 ⁇ m.
  • the solvent in the adhesive composition solution layer is removed and the acrylic polymer is crosslinked with the cross-linking agent to form the acrylic polymer and the cross-linking agent.
  • An adhesive layer having a crosslinked structure was obtained.
  • the adhesive composition layer was laminated to the release-treated surface of a 38 ⁇ m-thick polyethylene terephthalate (PET) film (trade name “MRE38”, manufactured by Mitsubishi Chemical Corporation) that had been subjected to silicone release treatment, thereby forming a PET film/adhesive layer. / An adhesive sheet having a laminated structure of PET films was produced.
  • PET polyethylene terephthalate
  • Example 14 (1) Preparation of Acrylic Polymer Solution The same procedure as in Example 13 was carried out.
  • Adhesive Composition Solution 0.25 parts by mass of dibenzoyl peroxide (1-minute half-life: 130° C.) as a cross-linking agent is added to 100 parts by mass of solid content in the resulting acrylic polymer solution.
  • a polyisocyanate-based cross-linking agent consisting of a trimethylolpropane adduct of tolylene diisocyanate (Coronate L, manufactured by Nippon Polyurethane Industry Co., Ltd.) 0.15 parts by mass, and a silane coupling agent (3-glycidoxypropyltrimethoxysilane;
  • An adhesive composition solution (sometimes referred to as “acrylic adhesive composition solution C”) containing 0.075 part by mass of Shin-Etsu Chemical Co., Ltd., product name “KBM-403”) was prepared.
  • Example 18 An optical laminate was produced in the same manner as in Example 14, except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 15 Optical laminates were produced in the same manner as in Example 14, except that the nip pressure between the nip rollers was changed as shown in Tables 1A to 1C.
  • Example 16 An optical laminate was produced in the same manner as in Example 15, except that the thickness of the adhesive layer was changed as shown in Tables 1A to 1C.
  • Example 17 In the same manner as in Example 13, except that the thickness of the adhesive layer and the nip pressure between the nip rollers were changed as shown in Tables 1A to 1C, and the concave-convex-shaped film B was used instead of the concave-convex-shaped film A. A laminate was produced.
  • Adhesive Composition Solution To the obtained acrylic polymer solution, trimethylolpropane/tolylene diisocyanate trimer adduct (manufactured by Tosoh Corporation) is added as a cross-linking agent to 100 parts by mass of polymer.
  • Product name Coronate L) and 0.075 parts by mass of dibenzoyl peroxide (manufactured by NOF Co., Ltd.: Nyper BMT40 (SV)) are blended to form an adhesive composition solution (“acrylic adhesive composition”).
  • Solution D was prepared.
  • An optical laminate was produced in the same manner as in Example 13, except that the nip pressure between the nip rollers was changed as shown in Tables 1A to 1C.
  • FIB processing Helios G4 UX DualBeam System manufactured by FEI
  • nip pressure laminate pressure
  • a pressure-sensitive paper manufactured by Fuji Film Co., Ltd., Prescale 3LW
  • the pressure (Mpa) was measured.
  • the average value over the entire nipped width is described as "nip pressure (laminate pressure) Pl".
  • the pressure Pf applied to the flat part is the value of the nip pressure between the rolls measured as described above, assuming that no pressure is applied to the recessed part of the surface of the unevenness-shaped film. , and converted by subtracting the area of the concave portion as shown in the following formula.
  • the occupied area ratio Rr of the concave portions the numerical value for designing the concave-convex shaped film was used.
  • FIG. 18 is a schematic perspective view for explaining a method of measuring the compressive stress-strain curve of the adhesive layer.
  • Each adhesive layer 20a (thickness 20 ⁇ m) of the example was cut into a size of approximately 10 mm ⁇ 10 mm (10 mm square), placed on the acrylic film 41, and Pt—Pd vapor deposition was performed for 30 seconds, followed by a predetermined was fixed to the support of , nanoindentation measurements were performed, and compressive stress-strain curves were obtained.
  • the measurement result is output as a load (N) for a displacement (mm).
  • 19A, 19B, and 19C are schematic cross-sectional views, top views, and cross-sectional views for explaining a method for measuring the 180° peel adhesive strength of the adhesive layer to the optical sheet.
  • an acrylic adhesive layer 49A (thickness: 100 ⁇ m) is placed on the unevenness-shaping film 70 (the unevenness-shaping film A) (thickness: 130 ⁇ m).
  • the adhesive layer 20a (thickness 15 ⁇ m) of each example were arranged in this order.
  • a PET film (thickness: 38 ⁇ m) was inserted between the adhesive layer 20a and the ruggedness-forming film 70 (arrow in FIG. 19A) so that peeling occurred at the interface between the adhesive layer 20a and the ruggedness-forming film 70.
  • the concave-convex shaping film 70 is arranged so that the inclined surface having the inclination angle ⁇ a (49°) of the concave portion 74 is farther from the bent portion of the film laminate 40f than the inclined surface having the inclination angle ⁇ b (85°). did.
  • the acrylic adhesive layers 49A and 49B are known general-purpose glues. (Apparatus/measurement conditions) Apparatus: Autograph AGT-5N (manufactured by Shimadzu Corporation) Peeling speed: 150 mm/min Measurement temperature: Room temperature
  • the range of 20 mm to 40 mm from the end was measured at 1640 points at equal intervals, A 180° peel adhesive strength (N/25 mm) was obtained by calculating the average value.
  • a peel adhesion force was obtained.
  • the stress Sp was obtained by dividing the obtained 180° peel adhesive strength (N/25 mm) by the cross-sectional area of the film (that is, the cross-sectional area of the film laminate 40f, 25 mm ⁇ 195 ⁇ m).
  • ⁇ Calculated embedding amount Dd> The calculated embedding amount Dd of the adhesive layer in each example was calculated.
  • the embedding amount dmax shown in Tables 1A to 1C is a value obtained by multiplying the strain with respect to the pressure Pf applied to the flat portion in the compressive stress-strain curve of the adhesive layer 20a by the thickness Dt of the adhesive layer 20a. dmax.
  • FIG. 10 is a graph showing evaluation results of the area ratio (%) of air bubbles and the height ( ⁇ m) of the adhesive layer present in the recesses in the optical laminates of Examples 1 to 18.
  • Examples 1 to 5 using the polyester adhesive composition solution A are hatched circles or triangles, and Examples 6 to 12 using the acrylic adhesive composition solution A are black.
  • the circles or triangles indicate the results of Examples 13 to 18 using the acrylic adhesive composition solution B or C, the white circles or triangles indicate the results.
  • Triangles indicate the results for the case where the film B for forming irregularities was used.
  • FIG. 17 shows the correlation between the measured value ( ⁇ m) of the height of the adhesive layer present in the recess and the calculated embedding amount Dd(1) ( ⁇ m) in the optical laminates of Examples 1 to 18. graph.
  • the results of Examples 1 to 18 are indicated by the same symbols as in FIG.
  • the present inventors tried to measure the adhesion to a surface as flat as possible made of the same material as the slanted surface of the recess 14.
  • the 180° peel adhesive strength of the adhesive layer 20a is measured, and the result is used to calculate the calculated embedding amount Dd regardless of the density of the concave portions of the optical sheet (concavo-convex shaped film) to be bonded to the adhesive layer 20a.
  • the area ratio of air bubbles existing at the interface between the flat portion and the adhesive layer was 3% or less, and the adhesive layer existing in the plurality of recesses had a high density. is 2 ⁇ m or less.
  • the area ratio of air bubbles present at the interface between the flat portion and the adhesive layer is more than 3% and/or air bubbles exist in a plurality of concave portions.
  • the height of the adhesive layer is greater than 2 ⁇ m.
  • the optical layered body of Example 14 and the optical layered body of Example 18 were produced by changing only the thickness Dt of the adhesive layer on the flat portion.
  • the area ratio of the optical layered body of Example 14 is suppressed to 3% or less, while that of the optical layered body of Example 18 exceeds 3%. From these results, it is preferable that the thickness Dt of the adhesive layer on the flat portion is, for example, 2 ⁇ m or more.
  • the thickness Dt of the adhesive layer may be, for example, 3 ⁇ m or more.
  • the upper limit of the thickness Dt of the adhesive layer is not particularly limited, and is, for example, 10 ⁇ m or less.
  • the area ratio of air bubbles existing at the interface between the flat portion and the adhesive layer depends not only on the thickness of the adhesive layer on the flat portion, but also on the thickness of the adhesive layer and the thickness of the adhesive layer when the adhesive layer and the optical sheet are bonded together.
  • the pressure applied to the optical sheet, the surface roughness of the surface of the separator used when producing the adhesive layer (specifically, the surface of the adhesive layer that is bonded to the uneven surface of the optical sheet) It may also change due to the surface roughness of the separator surface, the gel fraction of the adhesive layer, and the like.
  • the degree of penetration of the adhesive layer into the recesses of the uneven structure can also vary depending on the conditions for preparing the adhesive layer and the physical properties of the adhesive layer. For example, even if the same adhesive composition solution is used, if the thickness of the adhesive layer (thickness of the adhesive layer on the flat portion) is different, the crosslink density of the adhesive layer may be different.
  • the degree of penetration of the adhesive layer into the can vary. Therefore, the optical layered body according to the embodiment of the present invention can be obtained by appropriately adjusting the preparation conditions of the adhesive layer and the physical properties of the adhesive layer, without being limited to the examples described above.
  • the adhesive layer was produced without curing the ultraviolet curable resin contained in the acrylic adhesive composition solution A as described above.
  • the adhesive layer is not limited to this, and may contain a cured product of an ultraviolet curable resin. That is, an adhesive layer obtained by curing an ultraviolet curable resin using an acrylic adhesive composition solution containing an ultraviolet curable resin may be used. Whether or not the UV-curable resin is cured does not significantly change the surface roughness of the adhesive layer obtained, and does not significantly change the area ratio of the air bubbles in the optical layered body.
  • the calculated embedding amount Dd can be used to represent an optical layered body in which the penetration of the adhesive layer 20a into the concave portion 14 is suppressed. Specifically, when the height (measured value) of the adhesive layer present in the recess 14 is 2 ⁇ m or less, the calculated embedding amount Dd can be said to be 1.3 ⁇ m or less.
  • the calculation The embedded amount Dd is 1.3 ⁇ m or less.
  • the calculated embedding amount Dd is 1.3 ⁇ m or less in both calculation methods (1) and (2) (that is, both when the approximation formula of the compressive stress-strain curve of the adhesive layer is used or not). It can also be seen that Dd is 0.5 ⁇ m or less.
  • the lamination pressure Pl is 0.1 MPa or more. Although the upper limit of the lamination pressure Pl is not limited, it is, for example, 0.5 MPa or less.
  • the acrylic adhesive composition solutions B and C differ only in the type of cross-linking agent. Differences in crosslinkers did not affect the compressive stress-strain curves of the formed adhesive layers.
  • the adhesive layer formed from the polyester adhesive composition solution A has the largest coefficient a, and the adhesive layer formed from the acrylic adhesive composition solution A, The coefficient a becomes smaller in the order of the adhesive layer formed from the acrylic adhesive composition solution B or C.
  • the stress F2 caused by the peel adhesive strength was greater than or equal to the restoring force F1 due to compressive elasticity.
  • F2 ⁇ F1 that is, Sp ⁇ sin ⁇ a ⁇ Pf is satisfied
  • the calculated embedding amount Dd is equal to the embedding amount dmax.
  • the embedding amount dmax is a value obtained by multiplying the strain corresponding to Pf in the compressive stress-strain curve of the adhesive layer by the thickness Dt of the adhesive layer.
  • the peel adhesive strength The applied stress F2 is smaller than the restoring force F1 due to compression elasticity (F2 ⁇ F1), that is, satisfies Sp x sin ⁇ a ⁇ Pf, and the calculated embedding amount Dd is the compressive stress of the adhesive layer - Sp x sin ⁇ a in the strain curve , multiplied by the thickness Dt of the adhesive layer.
  • the stress Sp obtained from the peel adhesive strength is, for example, 0.5 MPa or less.
  • the adhesive layer can be used without being limited by the magnitude of the compression elastic modulus.
  • the stress Sp obtained from the peel adhesive strength is, for example, 1.0 MPa or more.
  • the adhesive layer formed from the polyester-based adhesive composition solution A is an example of the adhesive layer Ac described in International Application PCT/JP2022/004554 by the present applicant mentioned above. and a polyhydric alcohol copolymer, a cross-linking agent, and at least one cross-linking catalyst selected from the group consisting of an organic zirconium compound, an organic iron compound and an organic aluminum compound. It has a gel fraction of 40% or more after being held at a temperature of 85° C. and a relative humidity of 85% for 300 hours, and a 180° peel adhesive force to a PMMA film of 100 mN/20 mm or more.
  • the adhesive layer formed from the acrylic adhesive composition solution A is an example of the adhesive layer Aa described in International Publication No. WO 2021/167090 by the applicant mentioned above.
  • the creep deformation rate is 10% or less when a stress of 10,000 Pa is applied at 50 ° C. for 1 second, and the creep deformation rate is 16% when a stress of 10,000 Pa is applied at 50 ° C. for 30 minutes. and the 180° peel adhesive strength to the PMMA film is 10 mN/20 mm or more.
  • the optical layered body of Example A was prepared in the same manner as the optical layered body of Example 1, except that the thickness of the adhesive layer was 300 ⁇ m.
  • An optical layered body having a layered structure of The optical laminate of Example B was prepared in the same manner as in Example 18, except that the laminate structure of acrylic resin film/adhesive layer/concavo-convex shaping film B was formed so that the thickness of the adhesive layer was 160 ⁇ m.
  • An optical laminate having Here, the adhesive layer was made thick so that the penetration (embedding) of the adhesive layer into the concave portion could be easily observed.
  • FIG. 11A a transparent plate 150A is arranged on one main surface side of an optical layered body 100S of Example A, and a transparent plate 150B is arranged on the other main surface side to obtain a sample 1000A.
  • FIG. 11B is a diagram schematically showing a cross section of sample 1000A.
  • the transparent plate 150B is shorter than the optical laminate 100S so that the optical laminate 100S of Example A hits the corner of the transparent plate 150B.
  • the optical layered body 100S of Example A is pressed against the corner of the transparent plate 150B, and a force is manually applied to the optical layered body 100S of Example A through the transparent plate 150A (arrow in the figure).
  • the optical layered body 100S (broken line ellipse portion in the figure) was observed while applying the force and after the force was removed.
  • FIG. 12 shows optical images of the sample 1000A before applying the force (top), the sample 1000A with the force applied (middle), and the sample 1000A after the force was removed (bottom).
  • FIG. 13 shows the results of similar evaluation using the optical layered body of Example B in place of the optical layered body of Example A. As shown in FIG. FIG. 13 shows a sample with the optical stack of Example B before the force was applied (top), a sample with the optical stack of Example B while the force was applied (middle), and the force removed. The optical image of the sample (bottom row) having the optical layered body of Example B below is shown.
  • the adhesive layer was made thick and evaluated so that the penetration (embedding) of the adhesive layer into the concave portion was easy to observe, this evaluation result is based on the optical laminate according to the embodiment of the present invention. is not limited to the adhesive layer possessed by As described above, in the optical laminates of Examples 14 to 16 using the adhesive layer having the same composition as that of the optical laminate of Example B, the area ratio of the air bubbles present at the interface between the flat portion and the adhesive layer was 3% or less, and the height of the adhesive layer present in the plurality of recesses is 2 ⁇ m or less.
  • optical laminate of the present invention is widely used in optical devices such as display devices and lighting devices.
  • first optical sheet 12s 10a first optical sheet 12s, 18s main surface (surface) 20a adhesive layer 60 light source 80 light guide layer 100A, 102A, 102B optical laminate 200A, 200B lighting device

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  • General Physics & Mathematics (AREA)
  • Optics & Photonics (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Fluid Mechanics (AREA)
  • Laminated Bodies (AREA)
PCT/JP2022/024974 2021-06-22 2022-06-22 光学積層体の製造方法および光学積層体 Ceased WO2022270556A1 (ja)

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