WO2016152792A1

WO2016152792A1 - Organic electroluminescence panel module

Info

Publication number: WO2016152792A1
Application number: PCT/JP2016/058756
Authority: WO
Inventors: 進竹川
Original assignee: コニカミノルタ株式会社
Priority date: 2015-03-23
Filing date: 2016-03-18
Publication date: 2016-09-29
Also published as: JPWO2016152792A1

Abstract

The present invention addresses the problem of providing an organic electroluminescence panel module having a high surface reflectivity and capable of displaying clear patterns which differ depending on the presence or absence of light emission from an organic electroluminescence element. The organic electroluminescence panel module according to the present invention is configured by disposing, from the viewing side, a surface protection sheet, a decorative sheet, an organic electroluminescence element, and a rear surface protection member, and is characterized in that the organic electroluminescence panel module displays patterns that differ when the organic electroluminescence element is emitting light and is not emitting light, and has an average reflectivity of 50% or more with respect to external light with a wavelength of 550 nm when the organic electroluminescence element is not emitting light.

Description

Organic electroluminescence panel module

The present invention relates to an organic electroluminescence panel module that has a high surface reflectivity and can display different clear patterns depending on whether or not the organic electroluminescence element emits light.

¡Various display methods are used to display various information. For example, many sign boards are used for providing product information using a board on which a design or the like is printed on a decorative board such as an acrylic resin or for displaying an escape route.

In recent years, in these various information display boards (hereinafter also referred to as sign boards), a light-emitting display device that incorporates a light-emitting light source and displays a message by light emission has been widely used.

A general light-emitting sign board has an illuminating device (light-emitting device) on the back side (back side) of a display board on which display information is displayed as viewed from an observer. As a lighting device, a box-shaped structure in which a reflector (reflector), a light source such as a fluorescent lamp, and a scattering plate are arranged in this order from the back side to the front side is common, and the inner surface of the box-shaped structure is particularly light. The white color is used to ensure the extraction efficiency. Various display information produced by printing, coating, labeling or sticking is arranged on the front side of the box-shaped lighting device.

2. Description of the Related Art In recent years, surface-emitting bodies that use electroluminescence elements (EL elements) as light sources have been actively developed as electroluminescent elements in box-type lighting devices. A surface light emitter of this type is a surface light source that emits light almost uniformly in a plane, and has excellent characteristics such as low heat generation and thinness. Therefore, it is expected as a next-generation illumination that replaces conventional incandescent lamps and fluorescent lamps.

For example, a decorative luminous body having a decorative layer formed of a curable ink on a substrate surface on the light extraction side of a surface light emitting element (organic electroluminescence element) is disclosed (for example, see Patent Document 1). Moreover, a light-emitting pattern board, a pattern light emitting display device including an organic electroluminescence element plate on the back side of the pattern board and a light-transmissive back plate is disclosed (for example, see Patent Document 2). .)

However, in the methods disclosed in Patent Document 1 and Patent Document 2, the organic electroluminescence element or the like is simply used as a surface-emitting illumination member, and information to be displayed is displayed on the surface of the pattern or This is a method expressed by printed matter, and only displays one message. In addition, the organic electroluminescence element has high energy consumption efficiency, high brightness, no heat generation, and excellent visibility, while the organic electroluminescence element is placed inside a storage box etc. and is thin and flexible It is difficult to say that the characteristics of the organic electroluminescence device having the characteristics are fully utilized.

Further, in Patent Document 3, an electroluminescent lamp composed of a transparent electrode drawn with an electrode, a light emitting layer, and a conductive ink on a base material, and the drawn transparent electrode is not caused to emit light when no power is supplied. A method is disclosed in which a transparent electrode emits light when energized and a pattern drawn with conductive ink can be visually recognized. However, the method disclosed in Patent Document 3 is a method of displaying only a single printed symbol as described above, and does not have a function of displaying a plurality of symbols.

On the other hand, on the electroluminescence light emitting sheet, a sheet-like exhibit having translucency is arranged through an adhesive layer, and when the electroluminescence light emitting sheet is in a non-light emitting state, the surface pattern of the exhibit is observed, A method is disclosed in which when the electroluminescent light emitting sheet emits light, the light emission pattern of the electroluminescent light emitting sheet emerges from the back of the exhibit through the exhibit (see, for example, Patent Document 4).

However, in the method described in Patent Document 4, the display pattern at the time of light emission and non-light emission of the electroluminescence light emitting sheet is the same and lacks diversity, and between the electroluminescence light emitting sheet and the exhibit, Only the adhesive layer is present, and when the electroluminescent light emitting sheet is not emitting light, when observed from the surface, the pattern of the electroluminescent light emitting sheet and the light emitting pattern formed by the transparent electrode are visible, At the time of non-light-emission, there is a problem that the clarity of the display pattern is deteriorated because the pattern of the transparent electrode located on the lower surface is also visually recognized as the pattern of the surface of the exhibit having translucency.

International Publication No. 2011/048956 JP 2013-221379 A JP 2004-273349 A JP 2009-129823 A

The present invention has been made in view of the above problems, and its solution is to provide an organic electroluminescence panel module that has a high surface reflectance and can display a clear pattern that varies depending on whether or not the organic electroluminescence element emits light. Is to provide.

As a result of intensive studies in view of the above problems, the present inventor has arranged a surface protection sheet, a decorative sheet, an organic electroluminescence element and a back surface protection member from the viewing side, and when the organic electroluminescence element is not emitting light, To provide an organic electroluminescence panel module capable of displaying a plurality of appropriate clear patterns according to the situation by an organic electroluminescence panel module having an average reflectance of external light having a wavelength of 550 nm of 50% or more. We found out what we can do and arrived at the present invention.

That is, the above-mentioned problem of the present invention is solved by the following means.

1. From the viewing side, it is a planar organic electroluminescence panel module configured by disposing a surface protection sheet, a decorative sheet, an organic electroluminescence element and a back surface protection member,
Display different patterns at the time of light emission and non-light emission of the organic electroluminescence element,
An organic electroluminescence panel module, wherein an average reflectance of external light having a wavelength of 550 nm is 50% or more when the organic electroluminescence element is not emitting light.

2. The organic electroluminescence panel module according to claim 1, further comprising a half mirror between the decorative sheet and the organic electroluminescence element.

3. 3. The organic electroluminescence panel module according to

item

1 or 2, further comprising a color difference forming layer whose color tone changes depending on a viewing angle on the organic electroluminescence element.

4. The organic electroluminescence panel module according to any one of claims 1 to 3, further comprising a mask member between the decorative sheet and the organic electroluminescence element.

5. The organic electroluminescence panel module according to any one of items 1 to 4, wherein the surface protective sheet, the decorative sheet, the organic electroluminescence element, and the back surface protection member all have flexibility. .

6. 6. The organic electroluminescence panel module according to any one of items 1 to 5, wherein the total film thickness is in a range of 0.3 to 3.0 mm.

By the above means of the present invention, it is possible to provide an organic electroluminescence panel module which has a high surface reflectance and can display clear symbols of two or more designs depending on whether or not the organic electroluminescence element emits light. it can.

The technical features of the multi-symbol display device having the configuration defined in the present invention and the mechanism of its effects are as follows.

Conventionally, in the electroluminescence light emitting device proposed in, for example, Patent Document 4 and the like, as described above, an adhesive is bonded between an electroluminescence light emitting sheet (hereinafter referred to as an EL light emitting sheet) and an exhibit displayed during surface observation. It is a structure in which only the layer exists, and when the EL light emitting sheet is not emitting light, the transparent electrode pattern that forms the light emitting pattern of the EL light emitting sheet is visually recognized when observed from the surface. Simultaneously with the surface design of the exhibited display, the pattern of the transparent electrode located on the lower surface was also observed and the display design was blurred and a clear design could not be obtained. In addition, in the method described in Patent Document 4, since an inorganic electroluminescent element is used as an EL light emitting sheet, the light emission luminance and the element life are low. In particular, in the configuration in which the above exhibits are stacked, It also had the problem of the luminous pattern becoming dark.

The organic electroluminescence panel module of the present invention (hereinafter also referred to as an organic EL panel module) has been made in view of the above-described problems of the prior art. Using an electroluminescence element (hereinafter referred to as an organic EL element), a surface protective sheet, a decorative sheet, an organic EL element, and a back surface protective member are arranged from the observation side surface, and the wavelength of the organic electroluminescence element when not emitting light is 550 nm. By setting the average reflectance of outside light to 50% or more, when not emitting light, a half mirror is provided between the decorative sheet and the organic EL element to increase the surface reflectance. The EL element design pattern is shielded so that it cannot be seen. When the organic EL element emits light, By sure, at any time of non-emission time and light emission of the organic EL element can also be stably display a clear different pattern.

Schematic diagram showing an example of the display pattern of the organic EL panel module when not emitting light and when emitting light Schematic diagram showing another example of the display pattern of the organic EL panel module when not emitting light and when emitting light Schematic perspective view showing an example of the configuration (embodiment 1) of the organic EL panel module Schematic perspective view showing another example of the configuration (embodiment 1) of the organic EL panel module Schematic perspective view showing an example of the configuration (embodiment 2) of the organic EL panel module Schematic perspective view showing another example of the configuration (embodiment 3) of the organic EL panel module Schematic sectional view showing an example of the configuration (embodiment 3) of the organic EL panel module Schematic showing an example of the state of observation light at the time of non-light emission and light emission of the organic EL panel module Schematic showing another example of the state of observation light when the organic EL panel module is not emitting light and when emitting light Schematic sectional view showing Embodiment 4 having a color difference forming layer in the configuration of the organic EL panel module Schematic sectional view showing an example of an organic EL element applicable to an organic EL panel module FIG. 8 is a schematic cross-sectional view showing an example in which a color difference forming layer unit is provided in the organic EL element having the configuration shown in FIG. Schematic sectional view showing another example (tandem configuration) of an organic EL element applicable to an organic EL panel module Schematic sectional view showing an example of a sealed configuration of an organic EL panel module Schematic sectional view showing another example of the sealed structure of the organic EL panel module

The organic electroluminescence panel module of the present invention is a planar organic electroluminescence panel module configured by disposing a surface protection sheet, a decorative sheet, an organic electroluminescence element, and a back surface protection member from the viewing side. Different patterns are displayed when the electroluminescence element emits light and when it does not emit light, and the average reflectance of external light having a wavelength of 550 nm when the organic electroluminescence element does not emit light is 50% or more. This feature is a technical feature common to the inventions according to claims 1 to 6.

As an embodiment of the present invention, a decorative sheet and an organic electroluminescence device are used as means for setting the average reflectance of external light having a wavelength of 550 nm to 50% or more from the viewpoint of further achieving the effect of the present invention. It is preferable to provide a half mirror between the two from the viewpoint of displaying clear symbols of two or more designs.

Also, by providing a color difference forming layer that changes the color tone depending on the viewing angle on the organic electroluminescence element, it is possible to easily realize light-emitting patterns with different color tones depending on the viewing angle, which is rich in diversity. You can get a luminous pattern.

In addition, having a mask member for controlling the light emitting pattern between the half mirror and the organic electroluminescent element easily obtains a desired pattern to be expressed without controlling the light emitting region of the organic EL element itself. From the viewpoint of being able to do so.

Moreover, the surface protection sheet, the decorative sheet, the half mirror, the organic electroluminescence element, and the back surface protection member constituting the organic EL panel module are all made of a material having flexibility, thereby having high flexibility and various shapes. It is possible to provide an organic EL panel module that can cope with the above.

In addition, by making the total thickness of the organic EL panel module into a thin film sheet within the range of 0.3 to 3.0 mm, such as concert tickets, signboards and postings attached to walls, advertising media, message boards, business cards, etc. It can be applied to a wide range of fields such as cards.

Hereinafter, the present invention, its components, and modes and modes for carrying out the present invention will be described in detail with reference to the drawings. In the following description, “˜” is used to mean that the numerical values described before and after it are included as a lower limit value and an upper limit value. Moreover, in the following description, the number described in parentheses after each component represents the reference numeral of each component described in each figure.

<Overview of overall configuration of organic EL panel module>
The organic EL panel module of the present invention is configured by disposing a surface protection sheet, a decorative sheet, an organic electroluminescence element, and a back surface protection member from the viewing side, and is different depending on whether the organic electroluminescence element emits light or not. And a planar organic EL panel module in which the average reflectance of external light having a wavelength of 550 nm is 50% or more when the organic electroluminescence element is not emitting light. The average reflectance of external light having a wavelength of 550 nm is characterized by being 50% or more, preferably 50 to 95%, more preferably 65 to 95%. More preferably, it is in the range of 75 to 95%.

First, an example of symbol display by the organic EL panel module of the present invention will be described with reference to the drawings. In the following description, the symbol displayed on the decorative sheet is referred to as symbol A, and the symbol displayed on the organic EL element or the organic EL element and the mask member is referred to as symbol B.

FIG. 1A and FIG. 1B are schematic diagrams showing examples of typical display symbols when the organic EL panel module is not emitting light and when emitting light.

An organic EL panel module (1) shown in FIG. 1A is an example of a pattern observed from the surface side in a state where an organic EL element (not shown) is not emitting light, and is formed by a decorative sheet (5). Shows the state of being appreciated. In this state, since the half mirror (not shown) is provided in the lower part, the symbol B displayed by the organic EL element is not recognized.

On the other hand, FIG. 1B shows a state in which the organic EL element emits light, and together with the pattern A formed by the decorative sheet (5), the pattern B that emits light formed by the organic EL element and the mask member. it's shown.

<< Specific configuration of organic EL panel module >>
Next, the basic configuration of the organic EL panel module of the present invention will be described with reference to the drawings.

(Embodiment 1)
2A and 2B are schematic perspective views showing Embodiment 1 which is an example of the configuration of the organic EL panel module according to the present invention.

The organic EL panel module (1) shown in FIG. 2A is composed of the following members. At the uppermost part on the observation surface side (upper part of the paper surface), there is a transparent surface protection sheet (6) for protecting internal components from external impacts and scratches, and at the lower part is an organic EL For the purpose of displaying the pattern A when the element is not emitting light, a decorative sheet (5) on which various patterns are printed is provided. The pattern A printed on the decorative sheet (5) is also recognized when the organic EL element (3) emits light.

Next, on the lower surface side of the decorative sheet (5), an organic EL element (3) in which the pattern B is patterned is arranged as a surface emitting panel. 2A, for example, when a pattern B as shown in FIG. 1B is formed, for example, the organic EL element is irradiated with an electron beam or the like so as to have a desired pattern B, and the organic EL element The pattern B can be patterned by partially deactivating the light-emitting function, forming a non-light-emitting portion and a light-emitting portion.

A back surface protection member (2) is disposed in the lowermost layer, and functions as a member for ensuring the self-supporting property of the organic EL panel module having high flexibility, for example, when protecting the above-described constituent members and during installation. You can also.

In the organic EL panel module (1) shown in FIG. 2B, a mask member (4) is further provided between the decorative sheet (5) and the organic EL element (3) with respect to the configuration shown in FIG. 2A. It is a configuration. In such a configuration, the pattern B can be formed by a combination of the organic EL element (3) and the mask member (4). By using such a configuration, the pattern is formed on the organic EL element (3) itself. There is no need to pattern B, and an organic EL element (3) having uniform light emission characteristics can be used.

In the configuration shown in FIGS. 2A and 2B, when the organic EL element defined in the present invention does not emit light, the average reflectance of external light having a wavelength of 550 nm is 50% or more. Examples thereof include a method of imparting a function, for example, a method of forming a sheet having a half mirror effect.

(Embodiment 2)
FIG. 3 is a schematic perspective view showing Embodiment 2 which is an example of the configuration of the organic EL panel module according to the present invention.

In FIG. 3, the organic EL panel module (1) is composed of the following members. At the uppermost part on the observation surface side (upper part of the paper surface), there is a transparent surface protection sheet (6) for protecting internal components from external impacts and scratches, and at the lower part is an organic EL For the purpose of displaying the pattern A when the element is not emitting light, a decorative sheet (5) on which various patterns are printed is provided. The pattern A printed on the decorative sheet (5) is also recognized when the organic EL element (3) emits light.

Next, a half mirror (HM) is arranged on the lower surface side of the decorative sheet (5). This half mirror (HM) is an organic EL located in the lower part when the organic EL element (3) is not emitting light, and the symbol A is printed only with the symbol A printed on the decorative sheet (5). It has a function of preventing the pattern B formed by the element (3) from being displayed as noise.

The organic EL element (3) in which the pattern B is patterned is arranged as a surface emitting panel at the lower part of the half mirror. For example, in the case of forming the pattern B as shown in FIG. 1B with the configuration shown in FIG. 3, for example, the organic EL element is irradiated with an electron beam or the like so as to have the desired pattern B, thereby forming the organic EL element. The method of patterning the pattern B composed of the non-light emitting portion and the light emitting portion can be taken by partially deactivating the light emitting function.

(Embodiment 3)
FIG. 4 is a schematic perspective view showing Embodiment 3 which is another example of the configuration of the organic EL panel module.

3 is an example in which a mask member (4) is further disposed between the half mirror (HM) and the organic EL element (3), and the organic EL element (3) and the mask member ( The pattern B can be formed by the combination of 4). By using such a configuration, it is not necessary to pattern the pattern B on the organic EL element (3) itself, and the organic EL element (3) having uniform light emission characteristics can be used. In the mask member (4), the light transmission part (the formation part of the light emission pattern B) may be formed as a transparent area, or the area may be colored with color ink or the like to function as a color display pattern.

Next, a specific configuration of the organic EL panel module of the present invention will be described.

FIG. 5 is a schematic cross-sectional view showing the configuration of the above-described embodiment 3 of the organic EL panel module of the present invention.

FIG. 5 shows the configuration of the organic EL panel module (1) described in FIG.

The upper side of the paper surface is the viewing surface side, and the organic EL panel module (1) has a surface protection sheet (6), a decorative sheet (5), a half mirror (HM), a mask member (4), It has the structure which laminated | stacked the organic EL element (3) and the back surface protection member (2).

In the configuration shown in FIG. 5, the decorative sheet (5) has been described as an independent member. However, even if the decorative sheet (5) is integrated with the surface protective sheet (6), the decorative sheet (5) is integrated with the half mirror (HM). Also good. Moreover, although FIG. 5 demonstrated as one decoration sheet (5), even if it is the structure which laminated | stacked several decoration sheets (5) from which a pattern differs as the pattern A, for example, or a pattern differs A configuration in which the pattern A is formed by arranging a plurality of decorative sheets (5) in parallel in the horizontal direction may be employed.

Similarly, the mask member (4) may have a configuration in which a plurality of mask members (4) having different mask patterns are stacked, or a plurality of mask members (4) having different mask patterns may be horizontally aligned. It may be a configuration arranged in parallel.

Moreover, in FIG. 5, although only the organic EL element (3) is described as a surface emitting member, it is natural that a power supply unit (not shown) for supplying power to the organic EL element (3), light emission However, the description is omitted here. Moreover, although the organic EL element (3) has shown the single organic EL element in FIG. 5, it is good also as a structure which arranged the some organic EL element (3) in parallel according to the condition.

FIG. 6A and FIG. 6B are schematic diagrams for explaining the state of observation light during non-light emission and during light emission in the organic EL panel module (1) of the present invention.

In the organic EL panel module (1) having the configuration of the embodiment 3 described with reference to FIGS. 4 and 5 above, FIG. 6A shows the state of an appreciation pattern when the organic EL element (3) is not emitting light. In the state where the organic EL element (3) is not emitting light, the symbol that the viewer can see is the symbol A formed by the decorative sheet (5) by illumination light (L1) such as room lighting in the observation environment. Observe.

The illumination light (L1) enters from the outside, is reflected by the half mirror (HM), and the observer can visually recognize the information of the pattern A formed by the decorative sheet (5). At this time, the pattern of the mask member (4) disposed under the half mirror (HM) is hidden by the half mirror (HM) and is not recognized. As a result, it is possible to observe a clear pattern A of only the decorative sheet (5) with less noise such as the lower pattern pattern.

FIG. 6B shows symbol information observed when the organic EL element (3) emits light. Similarly to the above, together with the symbol A displayed by the decorative sheet (5), the organic EL element (3) The pattern B formed by the mask member (4) can be observed through the half mirror (HM) as emitted light (L2).

At this time, since the half mirror itself has a function of lowering the transmittance to some extent, it is important to set the emission luminance of the surface light emitter high. Therefore, in the present invention, it is an important condition for forming a clear pattern to apply a high-luminance organic EL element rather than an inorganic EL element having a relatively low emission luminance.

(Embodiment 4)
FIG. 7 is a schematic cross-sectional view showing an organic EL panel module having a configuration in which a color difference forming layer is provided on an organic EL element as a fourth embodiment.

The organic EL panel module (1) shown in FIG. 7 has a color difference forming layer further between the organic EL element (3) and the mask member (4) with respect to the organic EL panel module of Embodiment 3 shown in FIG. (8) is provided.

The color difference forming layer (8) uses at least one of the effects of thin film interference, multilayer film interference, diffraction interference, microgroove interference, microprotrusion interference, and scattering by microparticles, and the viewing angle. The layer functions so that different color tones are observed depending on the thickness. Specifically, it can be formed on the organic EL element (3) via a light diffusion layer. Details will be described later.

<Components of organic EL panel module>
Next, details of a surface protective sheet, a decorative sheet, a half mirror, a mask member, an organic EL element, a color difference forming layer, a back surface protective sheet, and the like will be described as components constituting the organic EL panel module of the present invention.

[Surface protection sheet]
The surface protective sheet according to the present invention is not particularly limited as long as it is made of a sheet-like material that transmits light, but a resin sheet is preferable from the viewpoint of durability, transparency, and the like. Examples of the resin sheet applicable to the present invention include a cellulose ester sheet, a polyester sheet, a polycarbonate sheet, a polyarylate sheet, a polysulfone (including polyethersulfone) sheet, polyethylene terephthalate, and polyethylene naphthalate. Polyester sheet, polyethylene sheet, polypropylene sheet, cellulose diacetate sheet, cellulose triacetate sheet, cellulose acetate propionate sheet, cellulose acetate butyrate sheet, polyvinylidene chloride sheet, polyvinyl chloride sheet, polyvinyl alcohol sheet, ethylene vinyl alcohol sheet, Syndiotactic polystyrene sheet, polycarbonate sheet, norbornene resin sheet, polymethyl Pentene sheet, polyether ketone sheet, polyether ketone imide sheet, polyamide sheet, polyamide imide sheet, fluororesin sheet, nylon sheet, polymethyl methacrylate sheet, acrylic sheet, Teflon (registered trademark) PTFE sheet, Teflon (registered trademark) TFE A sheet etc. can be mentioned.

Further, the thickness of the surface protective sheet is preferably selected within the range of 50 μm to 5 mm. When the total film thickness, which is a preferred embodiment of the organic EL panel module of the present invention, satisfies the range of 0.3 to 3.0 mm and importance is attached to flexibility, it may be in the range of 50 to 500 μm. preferable. On the other hand, in order to ensure the self-supporting property as the organic EL panel module, a material in the range of 0.5 to 5 mm can be selected.

[Decoration sheet]
The decorative sheet is, for example, a method of printing using a printing ink on the viewing surface side surface or the back surface side of a film of the same material as the surface protection sheet, or a method of forming a pattern by infiltrating the ink into the film It may be.

The printing method is not particularly limited. For example, letterpress: letterpress printing method, flexographic printing method, dry offset printing method, intaglio: gravure printing method, gravure offset printing method, pad printing method, planographic: offset printing method, Stencil: A screen printing method or an ink jet recording method can be applied. Moreover, the method by which a person draws directly on a base material sheet using the printing ink depending on a condition may be sufficient.

Examples of printing inks include oil-based letterpress ink, flexographic ink, dry offset ink, gravure ink, gravure offset ink, pad ink, offset ink, and screen ink.

As a method for fixing the pattern A after the printing ink is transferred from the plate onto the base sheet, the method shown below can be used.

(1) Evaporative drying type: Method of forming pattern A by evaporating volatile solvent in ink (resin component: vinyl resin, acrylic resin, polyester resin)
(2) Oxidative polymerization type: A method in which oxygen in the atmosphere is absorbed on the pattern A surface formed by ink mainly composed of drying oil, and vehicle molecules are bonded and polymerized to form a three-dimensional structure (resin component: alkyd) Resin)
(3) Two-component reaction type: one of two types of ink mixture using a resin having a reactive group (for example, epoxy resin or urethane resin) as a vehicle, and the other as a composition of a curing agent. Method of curing by combining liquids (4) Ultraviolet curing type: A method of forming a printing ink film on a substrate sheet and then irradiating it with ultraviolet rays to cause reaction curing. In particular, a method (resin component: acrylate resin, epoxy resin, oxetane resin, etc.) that can stably form a high-definition pattern A by applying it as an ink for an ink jet recording system.

The coloring material for ink is roughly classified into pigment-based ink and dye-based ink, but considering that the multi-pattern display device of the present invention is used outdoors and exposed to the environment such as ultraviolet rays and water, It is preferable to use a pigment-based ink having excellent weather resistance. The pigment can be appropriately selected from inorganic pigments and organic pigments according to the use and color to be expressed.

Also, a method of transferring a cutting sheet or the like prepared in advance as the decorative sheet may be used. For example, there is a method in which a pattern A is cut with a plotter or the like on each color sheet of a thin film, for example, each sheet made of vinyl chloride, a transfer sheet is applied, and then the cut pattern A is transferred onto a base sheet. be able to.

Further, in the decorative sheet used in Embodiment 1, it is preferable that the sheet is made of a material having a half mirror property.

[Half mirror]
In this invention, it is a preferable aspect that it is the structure which arrange | positions a half mirror between a decoration sheet and an organic EL device.

The organic EL panel module of the present invention is characterized in that the average reflectance of external light having a wavelength of 550 nm is 50% or more when the organic EL device is not emitting light. As one means for achieving this condition, by arranging a half mirror, when the organic EL device is not emitting light, the pattern A of the decorative sheet can be displayed by reflection of the half mirror, and when the organic EL device emits light. The duality of the symbol display of transmitting the emitted light and displaying the luminescent symbol B formed by the organic EL device and the mask member can be achieved more reliably.

The surface reflectance referred to in the present invention is a spectrophotometer (manufactured by JASCO Corporation), which is prepared by rubbing the back surface of an organic EL panel module with sandpaper and applying black magic so that reflection on the back surface does not occur. Was used to determine the surface reflectance of regular reflection at an incident light of 5 ° in the wavelength region of 550 nm. The present first branch is characterized in that the average reflectance of external light having a wavelength of 550 nm is 50% or more when the organic EL device is not emitting light, but preferably in the range of 50 to 95%. More preferably, it is in the range of 65 to 95%, and still more preferably in the range of 75 to 95%.

“Half mirror” refers to a translucent mirror that does not reflect all of the light that hits the mirror, but has the property of transmitting some percent of the light. Also in the half mirror according to the present invention, the average reflectance of external light having a wavelength of 550 nm is preferably 50% or more, more preferably in the range of 50 to 95%, still more preferably 65 to 95%. And particularly preferably in the range of 75 to 95%. In addition, the light transmittance of 350 to 850 nm is preferably 50% or less from the viewpoint of achieving the effects described in the present invention. Here, the half mirror means that the intensity of reflected light and transmitted light is approximately 1: 1.

The half mirror according to the present invention is preferably a mirror having flexibility on the film, and is a mirror having flexibility both of a property of specularly reflecting and transmitting the light irradiated on the mirror surface. In addition, the half mirror has a different refractive index of titanium oxide, silicon oxide, etc., as in the case of a semi-transparent metal film formed on a smooth surface of a mirror substrate such as a transparent film, and the multilayer mirror. Examples thereof include a material obtained by forming a multilayer film in which a high refractive index film and a low refractive index film are alternately laminated on a smooth surface of a mirror base material. Here, the semi-transmissive metal film is a film of a metal such as chromium or titanium that is thin enough to transmit a part of the irradiated light. The semipermeable metal film or multilayer film may be formed on the surface of the mirror substrate or on the back surface. When a semi-permeable metal film or multilayer film is formed on the surface, a transparent protective film such as a synthetic resin or a thin layer of silicon oxide or titanium oxide for protecting the film is formed on the film. When it is formed on the back surface, an antireflection film or the like can be formed on the surface of the mirror substrate.

[Mask member]
Next, the mask member according to the present invention will be described.

In the present invention, as a method of forming a mask pattern on the mask member (4), a light shielding part and a light transmitting part are formed on the surface side of the light transmissive resin base material by, for example, a screen printing method, A mask member provided with a pattern can be produced.

The ink used for the production of the mask member is not particularly limited as long as it is an ink that exhibits a light shielding effect and can form a film having excellent abrasion resistance. For example, a light-shielding ink containing a light-shielding pigment (for example, a black pigment) and an ultraviolet curable resin component is used, and after applying the ink to the light shielding part (12A) by screen printing, The pattern B can be formed by irradiating and curing.

Also, from the viewpoint of imparting color to the light emitting pattern, a method of coloring the light transmitting portion with color ink or the like can also be used.

[Organic EL device]
[Basic components of organic EL elements]
Next, details of the organic EL element according to the present invention will be described.

The organic EL element constituting the flexible surface light emitter according to the present invention can form various constituent layers on the resin substrate and the transparent anode. For example, the following layers (i) to (v) You may have a structure. Further, the following light emitting layer is preferably composed of a blue light emitting layer, a green light emitting layer and a red light emitting layer.

(I) A configuration in which a transparent anode / organic functional layer unit (light emitting layer / electron transport layer) / cathode / sealing adhesive / sealing member are laminated on a resin substrate,
(Ii) A configuration in which a transparent anode / organic functional layer unit (hole transport layer / light emitting layer / electron transport layer) / cathode / sealing adhesive / sealing member are laminated on a resin base material,
(Iii) A transparent anode / organic functional layer unit (hole transport layer / light emitting layer / hole blocking layer / electron transport layer) / cathode / sealing adhesive / sealing member was laminated on the resin substrate. Constitution,
(Iv) On the resin substrate, transparent anode / organic functional layer unit (hole transport layer / light emitting layer / hole blocking layer / electron transport layer / cathode buffer layer) / cathode / sealing adhesive / sealing member A stacked structure,
(V) On the resin substrate, transparent anode / organic functional layer unit (anode buffer layer / hole transport layer / light emitting layer / hole blocking layer / electron transport layer / cathode buffer layer) / cathode / sealing adhesive / Configuration in which sealing members are laminated,
Etc.

Next, each component of the organic EL element will be described.

(Resin base material)
The resin base material applied to the organic EL element according to the present invention is preferably a flexible resin base material having flexibility.

Examples of the resin base material applicable to the present invention include polyesters such as polyethylene terephthalate (abbreviation: PET) and polyethylene naphthalate (abbreviation: PEN), polyethylene, polypropylene, cellophane, cellulose diacetate, and cellulose triacetate (abbreviation: TAC). ), Cellulose acetate butyrate, cellulose acetate propionate (abbreviation: CAP), cellulose esters such as cellulose acetate phthalate, cellulose nitrate and their derivatives, polyvinylidene chloride, polyvinyl alcohol, polyethylene vinyl alcohol, syndiotactic polystyrene , Polycarbonate (abbreviation: PC), norbornene resin, polymethylpentene, polyetherketone, polyimide, polyethersulfone Abbreviation: PES), polyphenylene sulfide, polysulfones, polyetherimide, polyetherketoneimide, polyamide, fluororesin, nylon, polymethylmethacrylate, acrylic and polyarylates, Arton (trade name, manufactured by JSR) and Appel (trade name) The base material currently formed with resin materials, such as cycloolefin resin, such as Mitsui Chemicals, Inc. can be mentioned.

Among these resin substrates, films such as polyethylene terephthalate (abbreviation: PET), polybutylene terephthalate, polyethylene naphthalate (abbreviation: PEN), and polycarbonate (abbreviation: PC) are flexible in terms of cost and availability. It is preferably used as a resin base material.

In the present invention, the thickness of the resin substrate can be in the range of 3 to 200 μm, preferably in the range of 10 to 100 μm, and more preferably in the range of 20 to 50 μm.

The resin substrate according to the present invention can also be suitably used as a sealing member (transparent substrate) for organic EL elements. The resin base material may be an unstretched film or a stretched film.

The resin base material applicable to the present invention can be manufactured by a conventionally known general film forming method. For example, an unstretched resin base material that is substantially amorphous and not oriented can be produced by melting a resin as a material with an extruder, extruding it with an annular die or a T-die, and quenching. In addition, the unstretched resin base material is transported in the direction of the resin base material (vertical axis direction) by a known method such as uniaxial stretching, tenter sequential biaxial stretching, tenter simultaneous biaxial stretching, tubular simultaneous biaxial stretching, or the like. , MD direction), or a stretched resin substrate can be produced by stretching in a direction perpendicular to the conveying direction of the resin substrate (horizontal axis direction, TD direction). The draw ratio in this case can be appropriately selected according to the resin as the raw material of the resin base material, but is preferably in the range of 2 to 10 times in each of the vertical axis direction and the horizontal axis direction.

(Anode: Transparent anode)
As the anode constituting the organic EL device according to the present invention, a metal such as Ag or Au or an alloy containing a metal as a main component, CuI or indium-tin composite oxide (abbreviation: ITO), SnO _2, ZnO, or the like The metal oxide is preferably a metal or an alloy containing a metal as a main component, more preferably silver or an alloy containing silver as a main component.

When the transparent anode is composed mainly of silver, the purity of silver is preferably 99% or more. Further, palladium (Pd), copper (Cu), gold (Au), or the like may be added to ensure the stability of silver.

The transparent anode is a layer composed mainly of silver. Specifically, the transparent anode may be formed of silver alone or may be composed of an alloy containing silver (Ag). Examples of such alloys include silver-magnesium (Ag-Mg), silver-copper (Ag-Cu), silver-palladium (Ag-Pd), silver-palladium-copper (Ag-Pd-Cu), silver -Indium (Ag-In) and the like.

Among the constituent materials constituting the anode, the anode constituting the organic EL device according to the present invention is a transparent anode composed mainly of silver and having a thickness in the range of 2 to 20 nm. The thickness is preferably in the range of 4 to 12 nm. A thickness of 20 nm or less is preferable because the absorption component and reflection component of the transparent anode can be kept low and high light transmittance can be maintained.

The “layer composed of silver as a main component” in the present invention means that the silver content in the transparent anode is 60% by mass or more, preferably the silver content is 80% by mass or more. More preferably, the silver content is 90% by mass or more, and particularly preferably the silver content is 98% by mass or more. The term “transparent” in the transparent anode according to the present invention means that the light transmittance at a wavelength of 550 nm is 50% or more.

The transparent anode according to the present invention may have a configuration in which a layer composed mainly of silver is divided into a plurality of layers as necessary.

Further, in the present invention, when the anode is a transparent anode composed mainly of silver, a base layer may be provided at the lower portion from the viewpoint of improving the uniformity of the silver film of the transparent anode to be formed. preferable. Although there is no restriction | limiting in particular as a base layer, It is preferable that it is a layer containing the organic compound which has a nitrogen atom or a sulfur atom, and the method of forming a transparent anode on the said base layer is a preferable aspect.

In general, as a method of forming a transparent conductive film, for example, a method using a wet process such as a coating method, an ink jet method, a coating method, a dip method, a vapor deposition method (resistance heating, EB method, etc.), a sputtering method, a CVD method, etc. The method using the dry process is a method of manufacturing an organic EL device of the present invention, wherein the transparent anode according to the present invention is formed by vapor deposition.

As a vapor deposition method, a vacuum vapor deposition method is mainly used, and a resistance heating boat for vapor deposition in a vacuum vapor deposition apparatus is filled with silver, which is a constituent material of the transparent anode, and, if necessary, other alloys. The resistance heating boat for vapor deposition is made of molybdenum or tungsten. When forming the transparent anode, the vacuum degree in the vacuum deposition apparatus is reduced to, for example, a range of 1 × 10 ⁻² to 1 × 10 ⁻⁶ Pa, and then the above-described deposition material containing a transparent anode forming material such as silver is used. The resistance heating boat is energized and heated, and a silver thin film is vapor-deposited on the resin substrate or the underlayer at a predetermined vapor deposition rate (nm / second), and the thickness is in the range of 2 to 20 nm. An anode is formed.

(Organic functional layer unit)
Next, each layer constituting the organic functional layer unit will be described in the order of a charge injection layer, a light emitting layer, a hole transport layer, an electron transport layer, and a blocking layer.

<Charge injection layer>
The charge injection layer according to the present invention is a layer provided between the electrode and the light-emitting layer in order to lower the driving voltage and improve the light emission luminance. “The organic EL element and its industrialization front line (November 30, 1998) The details are described in Chapter 2, “Electrode Materials” (pages 123 to 166) of the second edition of “NTS Co., Ltd.”, and there are a hole injection layer and an electron injection layer.

In general, the charge injection layer is present between the anode and the light emitting layer or the hole transport layer in the case of a hole injection layer, and between the cathode and the light emitting layer or the electron transport layer in the case of an electron injection layer. However, the present invention is characterized in that the charge injection layer is disposed adjacent to the transparent electrode. When used in an intermediate electrode, it is sufficient that at least one of the adjacent electron injection layer and hole injection layer satisfies the requirements of the present invention.

The hole injection layer according to the present invention is a layer disposed adjacent to the anode, which is a transparent electrode, in order to lower the drive voltage and improve the light emission luminance. The details are described in Volume 2, Chapter 2, “Electrode Materials” (pages 123-166) of “Month 30th, NTS Corporation”.

The details of the hole injection layer are described in JP-A-9-45479, JP-A-9-260062, JP-A-8-288069, etc. Examples of materials used for the hole injection layer include: , Porphyrin derivatives, phthalocyanine derivatives, oxazole derivatives, oxadiazole derivatives, triazole derivatives, imidazole derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, hydrazone derivatives, stilbene derivatives, polyarylalkane derivatives, triarylamine derivatives, carbazole derivatives, Indolocarbazole derivatives, isoindole derivatives, acene derivatives such as anthracene and naphthalene, fluorene derivatives, fluorenone derivatives, polyvinylcarbazole, aromatic amines introduced into the main chain or side chain Child material or oligomer, polysilane, a conductive polymer or oligomer (e.g., PEDOT (polyethylene dioxythiophene): PSS (polystyrene sulfonic acid), aniline copolymers, polyaniline, polythiophene, etc.) and the like can be mentioned.

Examples of the triarylamine derivative include benzidine type represented by α-NPD (4,4′-bis [N- (1-naphthyl) -N-phenylamino] biphenyl), and MTDATA (4,4 ′, 4 ″). Examples include a starburst type represented by -tris [N- (3-methylphenyl) -N-phenylamino] triphenylamine), a compound having fluorene or anthracene in the triarylamine-linked core.

In addition, hexaazatriphenylene derivatives such as those described in JP-T-2003-519432 and JP-A-2006-135145 can also be used as a hole transport material.

The electron injection layer is a layer provided between the cathode and the light emitting layer for lowering the driving voltage and improving the light emission luminance. When the cathode is composed of the transparent electrode according to the present invention, Chapter 2 “Electrode materials” (pages 123 to 166) of the second edition of “Organic EL devices and their industrialization front line (issued by NTS, November 30, 1998)” ) Is described in detail.

Details of the electron injection layer are also described in JP-A-6-325871, JP-A-9-17574, JP-A-10-74586, and the like. Specific examples of materials preferably used for the electron injection layer are as follows. Metals represented by strontium and aluminum, alkali metal compounds represented by lithium fluoride, sodium fluoride, potassium fluoride, etc., alkali metal halide layers represented by magnesium fluoride, calcium fluoride, etc. Examples thereof include an alkaline earth metal compound layer typified by magnesium, a metal oxide typified by molybdenum oxide and aluminum oxide, and a metal complex typified by lithium 8-hydroxyquinolate (Liq). Moreover, when the transparent electrode in this invention is a cathode, organic materials, such as a metal complex, are used especially suitably. The electron injection layer is preferably a very thin film, and depending on the constituent material, the layer thickness is preferably in the range of 1 nm to 10 μm.

<Light emitting layer>
The light emitting layer constituting the organic functional layer unit of the organic EL device according to the present invention preferably has a structure containing a phosphorescent light emitting compound as a light emitting material.

This light emitting layer is a layer that emits light by recombination of electrons injected from the electrode or the electron transport layer and holes injected from the hole transport layer, and the light emitting portion is in the layer of the light emitting layer. Alternatively, it may be the interface between the light emitting layer and the adjacent layer.

Such a light emitting layer is not particularly limited in its configuration as long as the light emitting material contained satisfies the light emission requirements. Moreover, there may be a plurality of layers having the same emission spectrum and emission maximum wavelength. In this case, it is preferable to have a non-light emitting intermediate layer between the light emitting layers.

The total thickness of the light emitting layers is preferably in the range of 1 to 100 nm, and more preferably in the range of 1 to 30 nm because a lower driving voltage can be obtained. In addition, the sum total of the thickness of a light emitting layer is the thickness also including the said intermediate | middle layer, when a nonluminous intermediate | middle layer exists between light emitting layers.

In the present invention, one of the characteristics is a structure in which two or more light emitting layer units are laminated. The thickness of each light emitting layer is preferably adjusted within a range of 1 to 50 nm. More preferably, it is more preferable to adjust within the range of 1 to 20 nm. When the plurality of stacked light emitting layers correspond to the respective emission colors of blue, green, and red, there is no particular limitation on the relationship between the thicknesses of the blue, green, and red light emitting layers.

The light emitting layer as described above is prepared by using a known method such as a vacuum evaporation method, a spin coating method, a casting method, an LB method (Langmuir-Blodget, Langmuir Blodgett method) and an ink jet method. Can be formed.

In the light emitting layer, a plurality of light emitting materials may be mixed, and a phosphorescent light emitting material and a fluorescent light emitting material (also referred to as a fluorescent dopant or a fluorescent compound) may be mixed and used in the same light emitting layer. The structure of the light-emitting layer preferably includes a host compound (also referred to as a light-emitting host) and a light-emitting material (also referred to as a light-emitting dopant compound), and emits light from the light-emitting material.

<Host compound>
As the host compound contained in the light emitting layer, a compound having a phosphorescence quantum yield of phosphorescence emission at room temperature (25 ° C.) of less than 0.1 is preferable. Further, the phosphorescence quantum yield is preferably less than 0.01. Moreover, it is preferable that the volume ratio in the layer is 50% or more among the compounds contained in a light emitting layer.

As the host compound, a known host compound may be used alone, or a plurality of types of host compounds may be used. By using a plurality of types of host compounds, it is possible to adjust the movement of charges, and the efficiency of the organic electroluminescent device can be improved. In addition, by using a plurality of kinds of light emitting materials described later, it is possible to mix different light emission, thereby obtaining an arbitrary light emission color.

The host compound used in the light emitting layer may be a conventionally known low molecular compound or a high molecular compound having a repeating unit, and a low molecular compound having a polymerizable group such as a vinyl group or an epoxy group (evaporation polymerizable light emitting host). )

Examples of host compounds applicable to the present invention include, for example, JP-A Nos. 2001-257076, 2002-308855, 2001-313179, 2002-319491, 2001-357777, 2002-334786, 2002-8860, 2002-334787, 2002-15871, 2002-334788, 2002-43056, 2002-334789, 2002 -75645, 2002-338579, 2002-105445, 2002-343568, 2002-141173, 2002-352957, 2002-203683, 2002 36 No. 227, No. 2002-231453, No. 2003-3165, No. 2002-234888, No. 2003-27048, No. 2002-255934, No. 2002-260861, No. 2002-280183. No. 2002, No. 2002-299060, No. 2002-302516, No. 2002-305083, No. 2002-305084, No. 2002-308837, US Patent Publication No. 2003/0175553, US Patent Publication No. 2006/0280965, United States Patent Publication No. 2005/0112407, United States Patent Publication No. 2009/0017330, United States Patent Publication No. 2009/0030202, United States Patent Publication No. 2005/2389. No. 9, International Publication No. 2001/039234, International Publication No. 2009/021126, International Publication No. 2008/056746, International Publication No. 2004/093207, International Publication No. 2005/089025, International Publication No. 2007 / No. 063796, International Publication No. 2007/063754, International Publication No. 2004/107822, International Publication No. 2005/030900, International Publication No. 2006/114966, International Publication No. 2009/086028, International Publication No. 2009/003898 And compounds described in International Publication No. 2012/023947, JP 2008-074939 A, JP 2007-254297 A, European Patent No. 2034538, and the like.

<Light emitting material>
As the light-emitting material that can be used in the present invention, a phosphorescent compound (also referred to as a phosphorescent compound, a phosphorescent material, or a phosphorescent dopant) and a fluorescent compound (both a fluorescent compound or a fluorescent material) are used. Say).

<Phosphorescent compound>
A phosphorescent compound is a compound in which light emission from an excited triplet is observed. Specifically, it is a compound that emits phosphorescence at room temperature (25 ° C.), and the phosphorescence quantum yield is 0 at 25 ° C. A preferred phosphorescence quantum yield is 0.1 or more, although it is defined as 0.01 or more compounds.

The phosphorescent quantum yield can be measured by the method described in Spectroscopic II, page 398 (1992 edition, Maruzen) of the Fourth Edition Experimental Chemistry Course 7. The phosphorescence quantum yield in the solution can be measured using various solvents, but when using a phosphorescent compound in the present invention, the phosphorescence quantum yield is 0.01 or more in any solvent. Should be achieved.

The phosphorescent compound can be appropriately selected from known compounds used for the light-emitting layer of a general organic EL device, but preferably contains a group 8 to 10 metal in the periodic table of elements. More preferred are iridium compounds, more preferred are iridium compounds, osmium compounds, platinum compounds (platinum complex compounds) or rare earth complexes, and most preferred are iridium compounds.

In the present invention, at least one light emitting layer may contain two or more phosphorescent compounds, and the concentration ratio of the phosphorescent compound in the light emitting layer varies in the thickness direction of the light emitting layer. It may be an embodiment.

Specific examples of known phosphorescent compounds that can be used in the present invention include compounds described in the following documents.

Nature 395, 151 (1998), Appl. Phys. Lett. 78, 1622 (2001), Adv. Mater. 19, 739 (2007), Chem. Mater. 17, 3532 (2005), Adv. Mater. 17, 1059 (2005), International Publication No. 2009/100991, International Publication No. 2008/101842, International Publication No. 2003/040257, US Patent Publication No. 2006/835469, US Patent Publication No. 2006/020202194. The compounds described in the specification, US Patent Publication No. 2007/0087321, US Patent Publication No. 2005/0244673, and the like can be mentioned.

Also, Inorg. Chem. 40, 1704 (2001), Chem. Mater. 16, 2480 (2004), Adv. Mater. 16, 2003 (2004), Angew. Chem. lnt. Ed. 2006, 45, 7800, Appl. Phys. Lett. 86, 153505 (2005), Chem. Lett. 34, 592 (2005), Chem. Commun. 2906 (2005), Inorg. Chem. 42, 1248 (2003), International Publication No. 2009/050290, International Publication No. 2002/015645, International Publication No. 2009/000673, US Patent Publication No. 2002/0034656, US Pat. No. 7,332,232, US Patent Publication No. 2009/0108737, US Patent Publication No. 2009/0039776, US Patent No. 6921915, US Patent No. 6,687,266, US Patent Publication No. 2007/0190359, US Patent Publication No. 2006 No./0008670, U.S. Patent Publication No. 2009/0165846, U.S. Patent Publication No. 2008/0015355, U.S. Pat. No. 7,250,226, U.S. Pat. No. 7,396,598, U.S. Patent Publication No. 2006 / 026363 Pat, U.S. Patent Publication No. 2003/0138657, U.S. Patent Publication No. 2003/0152802, may be mentioned compounds described in U.S. Patent No. 7,090,928 Pat like.

In the present invention, preferred phosphorescent compounds include organometallic complexes having Ir as a central metal. More preferably, a complex containing at least one coordination mode of metal-carbon bond, metal-nitrogen bond, metal-oxygen bond, and metal-sulfur bond is preferable.

The phosphorescent compound described above (also referred to as a phosphorescent metal complex) is described in, for example, Organic Letter, vol. 16, 2579-2581 (2001), Inorganic Chemistry, Vol. 30, No. 8, pp. 1685-1687 (1991), J. Am. Am. Chem. Soc. , 123, 4304 (2001), Inorganic Chemistry, Vol. 40, No. 7, pages 1704-1711 (2001), Inorganic Chemistry, Vol. 41, No. 12, pages 3055-3066 (2002) , New Journal of Chemistry. 26, 1171 (2002), European Journal of Organic Chemistry, Vol. 4, pages 695-709 (2004), and methods disclosed in the references and the like described in these documents Can be synthesized.

<Fluorescent compound>
Fluorescent compounds include coumarin dyes, pyran dyes, cyanine dyes, croconium dyes, squalium dyes, oxobenzanthracene dyes, fluorescein dyes, rhodamine dyes, pyrylium dyes, perylene dyes, stilbene dyes. And dyes, polythiophene dyes, and rare earth complex phosphors.

<Hole transport layer>
The hole transport layer is made of a hole transport material having a function of transporting holes. In a broad sense, the hole injection layer and the electron blocking layer also have the function of a hole transport layer. The hole transport layer can be provided as a single layer or a plurality of layers.

The hole transport material has any of hole injection or transport and electron barrier properties, and may be either organic or inorganic. For example, triazole derivatives, oxadiazole derivatives, imidazole derivatives, polyarylalkane derivatives, pyrazoline derivatives, pyrazolone derivatives, phenylenediamine derivatives, arylamine derivatives, amino-substituted chalcone derivatives, oxazole derivatives, styrylanthracene derivatives, fluorenone derivatives, hydrazone derivatives, Examples include stilbene derivatives, silazane derivatives, aniline copolymers, conductive polymer oligomers, and thiophene oligomers.

As the hole transport material, those described above can be used, but porphyrin compounds, aromatic tertiary amine compounds and styrylamine compounds can be used, and in particular, aromatic tertiary amine compounds can be used. preferable.

For the hole transport layer, the hole transport material may be formed by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an ink jet method, and an LB method (Langmuir Brodget, Langmuir Brodgett method). Thus, it can be formed by thinning. The layer thickness of the hole transport layer is not particularly limited, but is usually about 5 nm to 5 μm, preferably 5 to 200 nm. The hole transport layer may have a single layer structure composed of one or more of the above materials.

Also, the p property can be increased by doping impurities into the material of the hole transport layer. Examples thereof include JP-A-4-297076, JP-A-2000-196140, 2001-102175 and J.P. Appl. Phys. 95, 5773 (2004), and the like.

Thus, it is preferable to increase the p property of the hole transport layer because an element with lower power consumption can be manufactured.

<Electron transport layer>
The electron transport layer is made of a material having a function of transporting electrons, and in a broad sense, an electron injection layer and a hole blocking layer are also included in the electron transport layer. The electron transport layer can be provided as a single layer structure or a stacked structure of a plurality of layers.

In the electron transport layer having a single-layer structure and the electron transport layer having a multilayer structure, an electron transport material (also serving as a hole blocking material) constituting a layer portion adjacent to the light emitting layer is used as an electron transporting material. What is necessary is just to have the function to transmit. As such a material, any one of conventionally known compounds can be selected and used. Examples include nitro-substituted fluorene derivatives, diphenylquinone derivatives, thiopyran dioxide derivatives, carbodiimides, fluorenylidenemethane derivatives, anthraquinodimethane, anthrone derivatives, and oxadiazole derivatives.

The electron transport layer can be formed by thinning the above material by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an inkjet method, and an LB method. The thickness of the electron transport layer is not particularly limited, but is usually about 5 nm to 5 μm, preferably 5 to 200 nm. The electron transport layer may have a single structure composed of one or more of the above materials.

<Blocking layer>
The blocking layer includes a hole blocking layer and an electron blocking layer, and is a layer provided as necessary in addition to the constituent layers of the organic functional layer unit 3 described above. For example, it is described in JP-A Nos. 11-204258 and 11-204359, and “Organic EL elements and the forefront of industrialization (published by NTT Corporation on November 30, 1998)” on page 237. Hole blocking (hole block) layer and the like.

The hole blocking layer has a function of an electron transport layer in a broad sense. The hole blocking layer is made of a hole blocking material that has a function of transporting electrons but has a very small ability to transport holes, and recombines electrons and holes by blocking holes while transporting electrons. Probability can be improved. Moreover, the structure of an electron carrying layer can be used as a hole-blocking layer as needed. The hole blocking layer is preferably provided adjacent to the light emitting layer.

On the other hand, the electron blocking layer has a function of a hole transport layer in a broad sense. The electron blocking layer is made of a material that has the ability to transport holes and has a very small ability to transport electrons. By blocking holes while transporting holes, the probability of recombination of electrons and holes is improved. Can be made. Moreover, the structure of a positive hole transport layer can be used as an electron blocking layer as needed. The layer thickness of the hole blocking layer applied to the present invention is preferably in the range of 3 to 100 nm, more preferably in the range of 5 to 30 nm.

(Cathode: Second electrode)
The cathode (second electrode) is an electrode film that functions to supply holes to the second organic functional layer unit or the third organic functional layer unit, and is a metal, alloy, organic or inorganic conductive compound, or these A mixture is used. Specifically, gold, aluminum, silver, magnesium, lithium, magnesium / copper mixture, magnesium / silver mixture, magnesium / aluminum mixture, magnesium / indium mixture, indium, lithium / aluminum mixture, rare earth metal, ITO, ZnO, TiO Oxide semiconductors such as ₂ and SnO ₂ .

The second electrode can be produced by forming a thin film of these conductive materials by a method such as vapor deposition or sputtering. The sheet resistance as the second electrode is several hundred Ω / sq. The film thickness is usually selected from the range of 5 nm to 5 μm, preferably 5 to 200 nm.

In the case where the organic EL element is a double-sided light emitting type in which the emitted light L is also taken out from the second electrode, the second electrode having good light transmittance may be selected and configured.

(Sealing member)
Examples of the sealing means used for sealing the organic EL element according to the present invention include a method of adhering the sealing member, the second electrode 6 and the transparent substrate 1 with an adhesive.

The sealing member may be disposed so as to cover the display area of the organic EL element, and may be concave or flat. Further, transparency and electrical insulation are not particularly limited.

Specifically, a material having flexibility can be used, and examples thereof include polycarbonate, acrylic, polyethylene terephthalate, polyether sulfide, polysulfone, and the like.

The polymer film that can be used as the sealing member further has a water vapor transmission rate of 1 at a temperature of 25 ± 0.5 ° C. and a relative humidity of 90 ± 2% RH measured by a method according to JIS K 7129-1992. is preferably ^{^{× 10 -3 g / m 2 ·}} 24h or less, more, oxygen permeability measured by the method based on JIS K 7126-1987 ^{^{is, 1 × 10 -3 ml / m}} 2 · 24h · Atm (1 atm is 1.01325 × 10 ⁵ Pa) or less, and the water vapor permeability at a temperature of 25 ± 0.5 ° C. and a relative humidity of 90 ± 2% RH is 1 × 10 ⁻³ g / m ² -It is preferable that it is 24 hours or less.

In addition, an organic functional layer unit is sandwiched between the second electrode and the organic functional layer unit on the outer side of the second electrode facing the transparent substrate, and an inorganic or organic layer is formed in contact with the transparent substrate. A sealing film can also be suitably used. In this case, the material for forming the sealing film may be any material that has a function of suppressing intrusion of moisture, oxygen, or the like that degrades the organic EL element. For example, silicon oxide, silicon dioxide, silicon nitride, or the like is used. be able to. Furthermore, in order to improve the brittleness of the sealing film, it is preferable to have a laminated structure of these inorganic layers and organic layers made of organic materials. The method for forming these films is not particularly limited. For example, vacuum deposition method, sputtering method, reactive sputtering method, molecular beam epitaxy method, cluster ion beam method, ion plating method, plasma polymerization method, atmospheric pressure plasma A polymerization method, a plasma CVD method, a laser CVD method, a thermal CVD method, a coating method, or the like can be used.

In the gap between the sealing member and the display area of the organic EL element, it is preferable to inject an inert gas such as nitrogen or argon, or an inert liquid such as fluorinated hydrocarbon or silicon oil in the gas phase and the liquid phase. . Further, the gap between the sealing member and the display area of the organic EL element can be evacuated, or a hygroscopic compound can be sealed in the gap.

[Color difference forming layer unit]
In the organic EL device according to the present invention, light from the light diffusion layer is observed on the light emitting surface side of the organic EL device so that different colors are observed on the light diffusion layer according to the viewing angle. It is a preferable aspect to provide a color difference forming layer unit composed of a color difference forming layer that changes colors and emits them.

By providing the color difference forming layer unit on the light emitting surface side of the organic EL element, the light emission pattern B formed by the organic EL element and the mask member varies depending on the angle (hereinafter also referred to as viewing angle) observed by the observer. It is possible to obtain a light emitting pattern B having a characteristic that changes to a proper color tone.

The color difference forming layer uses at least one of the interference of a thin film, the interference of a multilayer film, the interference of diffraction, the interference of a fine groove, the interference of a fine protrusion, and the scattering by a fine particle, depending on the viewing angle. The color of light from the light diffusion layer is changed so that different colors are observed. In a preferred embodiment, the color difference forming layer is formed from a hologram sheet or a dielectric multilayer film.

(Light diffusion layer)
The light diffusion layer is provided on the light emitting surface of the organic EL element. The light diffusion layer has a function of diffusing light that passes through the light diffusion layer. When comparing the light before passing through the light diffusing layer with the light after passing through the light diffusing layer, the light distribution characteristic of the light after passing through the light diffusing layer is the difference in light intensity for each angle of the light distribution characteristics. It changes so that becomes small.

The organic EL element emits light inside a layer having a refractive index higher than that of air (within a refractive index of about 1.6 to 2.1), and is about 15% to 20% of the light generated in the light emitting layer. It is generally said that it can only be taken out. This is because light incident on the interface (interface between the resin substrate and the air) at an angle θ greater than the critical angle causes total reflection and cannot be extracted outside the device, or between the transparent electrode or the light emitting layer and the resin substrate. This is because light is totally reflected between the light and the light is guided through the transparent electrode or the light emitting layer, and as a result, the light escapes in the direction of the side surface of the device.

As a means for improving the light extraction efficiency, in the organic EL element according to the present invention, a light diffusion layer is provided on the organic EL element. The film having the light diffusion layer is also referred to as a light extraction film, and the light extraction film is also referred to as an outcoupling film (OCF).

As a light extraction method, for example, a method of forming irregularities on the surface of the film substrate to prevent total reflection at the resin substrate and the air interface (for example, US Pat. No. 4,774,435), concentrating the substrate. (For example, Japanese Patent Application Laid-Open No. 63-314795), a method for forming a reflection surface on the side surface of the element (for example, Japanese Patent Application Laid-Open No. 1-220394), an intermediate between the substrate and the light emitter. A method of forming an antireflection film by introducing a flat layer having a refractive index (for example, Japanese Patent Laid-Open No. 62-172691), and introducing a flat layer having a lower refractive index than the substrate between the substrate and the light emitter. (For example, Japanese Patent Laid-Open No. 2001-202827), a method of forming a diffraction grating between any one of the substrate, the transparent electrode layer and the light emitting layer (including between the substrate and the outside) (Japanese Patent Laid-Open No. 11-283951) And a method of providing an organic layer or a scattering layer having a high refractive index than the substrate between the substrate and the light emitting element and the like.

In the organic EL device according to the present invention, as the OCF (out coupling film), for example, a microlens film, a lenticular film, and a light scattering property provided with many microlens-like structures on the light extraction side on the film. Examples thereof include a light scattering film containing fine particles, a diffusion film whose surface has been processed into random irregularities, an internal refractive index distribution type film, and a light diffusion film containing a diffraction grating layer. For example, Japanese Patent No. 2822983, JP JP 2001-33783 A, JP 2001-56461 A, JP 6-18706 A, JP 10-20103 A, JP 11-160505 A, JP 11-305010 A, and JP 11-11 A. No. 326608, JP-A No. 2000-121809, JP-A No. 2000-18 A film according to 611 and JP 2000-338310 JP, and the like. In particular, it is preferable to use a light-scattering film mixed with fine particles that are inexpensive and can be mass-produced.

(Color difference forming layer)
The color difference forming layer is provided on the light diffusion layer. A light diffusion layer is located between the color difference forming layer and the organic EL element. The color difference forming layer includes a color difference forming layer unit and an adhesive provided so as to cover the surface of one side of the color difference forming layer unit. The pressure-sensitive adhesive bonds the color difference forming layer unit and the light diffusion layer. Since the adhesive is not an essential component, it may be used as necessary.

The color difference forming layer (color difference forming layer unit) emits light from the surface by changing the color of light from the light diffusion layer so that different colors are observed according to the viewing angle. Such a function of the color difference forming layer can be realized by the principle of structural color, for example. Illustratively, by utilizing at least one action of interference by a thin film, interference by a multilayer film, interference by diffraction, interference by fine grooves, interference by fine protrusions, and scattering by fine particles, the color difference forming layer described above is used. Functions can be realized.

In the color difference forming layer, a dielectric multilayer film may be used instead of a so-called hologram sheet such as a color difference forming layer unit. When a dielectric multilayer film is used, the way of interference of light can be changed by a combination of film thicknesses for each of a plurality of layers or a combination of film qualities for each of a plurality of layers. That is, the dielectric multilayer film uses the interference effect of the multilayer film to change the color of the light from the light diffusion layer so that different colors are observed according to the viewing angle, and emits them from the surface. Can do.

In the above description, the color difference forming layer unit is described as being installed on the light emitting surface side of the organic EL element, but if necessary, for example, the surface side of the surface protective sheet (6) or the decorative sheet (5). Or on the back side.

[Configuration of organic EL element]
(Organic EL device composed of a single organic functional layer unit)
FIG. 8 is a schematic cross-sectional view showing an example of the configuration of an organic EL element having a single organic functional layer unit.

The organic EL element (200) shown in FIG. 8 has a first electrode (102, anode) as a transparent electrode, a single organic functional layer unit (103), and a second electrode as a counter electrode on a transparent substrate (101). (106, cathode) are sequentially laminated.

The single organic functional layer unit (103) is composed of, for example, a hole transport layer / a light emitting layer / a hole blocking layer / an electron transport layer, and a blue light emitting phosphorescent compound and a green light emitting phosphorescent compound are included in the light emitting layer. A red light-emitting phosphorescent compound and a host compound, and emits white light by applying a voltage between the first electrode (102, anode) and the second electrode (106, cathode).

In the organic EL element (201) shown in FIG. 9, the light emission color tone is changed on the light extraction side (L direction) surface of the organic EL element (201) due to the difference in viewing angle, as described in FIG. It has a color difference forming layer unit composed of a light diffusion layer (107) having a function for changing and a color difference forming layer (108).

[Tandem type organic EL device]
FIG. 10 is a schematic cross-sectional view showing an example of the configuration of a tandem organic EL element.

The organic EL element (400) shown in FIG. 10 has a first electrode (102, anode), a first organic functional layer unit (103A), and a second organic functional layer unit (103B) as transparent electrodes on a transparent substrate (101). ), A third organic functional layer unit (103C), and a second electrode (106, cathode) as a counter electrode are sequentially stacked. For example, when the first organic functional layer unit (103A) emits red light, the second organic functional layer unit (103B) emits green light, and the third organic functional layer unit (103C) emits blue light, the first electrode (102, By applying a voltage between the anode) and the second electrode (106, cathode), white light is emitted.

In the organic EL element (400) shown in FIG. 10 as well, the light diffusion layer (107) having a function for changing the color tone of the emission color by the difference in the viewing angle and the color difference formation as described in FIG. A color difference forming layer unit composed of the layer (108) can be provided.

[Method of forming light emission pattern]
In the organic EL device according to the present invention, as a method of forming the light emission pattern as the pattern B, in addition to the method using the mask member described above, a light emitting portion and a non-light emitting portion are formed on the organic EL device, A method of forming the pattern B which is a light emission pattern can also be used.

Hereinafter, a method for forming a non-light emitting region and a light emitting region in the organic EL element will be described.

The light irradiation treatment method for the organic EL element is not particularly limited. For example, a method of performing light irradiation after forming a hole injection layer, a hole transport layer, an electron injection layer, or an electron transport layer, or the above Any of the methods of patterning the light emitting area by irradiating light to the organic EL element subjected to the sealing treatment may be used, but the latter method is in a state where the sealed organic EL element is exposed to the atmosphere. Since light irradiation can be performed, it is preferable from the viewpoint of simplifying the light irradiation process and reducing the manufacturing cost.

In the present invention, the light irradiation method may be a specific pattern forming method as long as the irradiation portion can be a non-light emitting region by irradiating a predetermined pattern region of the organic functional layer unit. Although not limited, Preferably, the method of forming the pattern B which forms a light emission area | region and a non-light emission area | region by irradiating light through the photomask member which consists of desired light emission shapes is preferable.

The light to be irradiated in the light irradiation step contains at least ultraviolet light, and may further have visible light or infrared light. As a light source applicable to the present invention, a high pressure mercury lamp, a low pressure mercury lamp, a hydrogen (deuterium) lamp, a rare gas (xenon, argon, helium, neon, etc.) discharge lamp, a nitrogen laser, an excimer laser (XeCl, XeF, KrF, KrCl, etc.), hydrogen laser, halogen laser, harmonics of various visible (LD) -infrared lasers (THG (Third Harmonic Generation) light of YAG laser) and the like.

[Back protection sheet]
Examples of the back surface protective sheet applicable to the present invention include a sheet-like base material made of the same material as the above-described surface protective sheet. However, the back surface protection sheet is not necessarily light transmissive.

Further, the thickness of the back surface protection sheet is preferably selected within the range of 50 μm to 5 mm. When the total film thickness, which is a preferred embodiment of the organic EL panel module of the present invention, satisfies the range of 0.3 to 3.0 mm and importance is attached to flexibility, it may be in the range of 50 to 500 μm. preferable. On the other hand, in order to ensure the self-supporting property as the organic EL panel module, a material in the range of 0.5 to 5 mm can be selected.

<< Formation of sealing structure >>
Finally, the formation method of the sealing body of the organic EL panel module comprised from said each structural member is demonstrated.

FIG. 11A and FIG. 11B are schematic cross-sectional views showing an example of a sealed configuration of an organic EL panel module.

11A shows a state where both ends of the organic EL panel module (1) having the configuration of the above-described embodiment 2 (FIG. 4) are sealed. As such a sealing method, a relatively thin surface protective sheet (6) and a back surface protective sheet (2) are used for sealing from a laminate or via an adhesive layer. Such a sealing method is applied to sealing a thin and highly flexible organic EL panel module.

In FIG. 11B, in order to ensure the self-supporting property of the organic EL panel module, for example, the back surface protection sheet (2) is formed of a thick film substrate, and the surface of the thin film is formed on the flat back surface protection sheet (2) surface. A method of bonding and sealing the protective sheet (6) through a laminating method or an adhesive layer can also be used.

ADVANTAGE OF THE INVENTION According to this invention, the organic electroluminescent panel module which has a high surface reflectivity and can display a clear pattern which changes with the presence or absence of light emission of an organic electroluminescent element can be provided, and the cards by which flexibility is requested | required The present invention provides a multi-organic electroluminescence panel module capable of displaying a plurality of appropriate symbols in accordance with various situations such as tickets, indoor or outdoor exhibits, decoration of wall surfaces and vehicle body surfaces, and the like.

DESCRIPTION OF SYMBOLS 1 Organic EL panel module 2 Back

surface protection member

3, 200, 201, 400 Organic EL element 4 Mask member 5 Decoration sheet 6 Surface protection sheet 8 Color difference formation layer 101 Transparent substrate 102 1st electrode 103 Organic functional layer unit 103A 1st organic function Layer unit 103B Second organic functional layer unit 103C Third organic functional layer unit 106 Second electrode 107 Light diffusion layer 108 Color difference forming layer HM Half mirror h Luminescent point L Luminous light L1 Illuminating light L2 Luminous pattern

Claims

From the viewing side, it is a planar organic electroluminescence panel module configured by disposing a surface protection sheet, a decorative sheet, an organic electroluminescence element and a back surface protection member,
Display different patterns at the time of light emission and non-light emission of the organic electroluminescence element,
An organic electroluminescence panel module, wherein an average reflectance of external light having a wavelength of 550 nm is 50% or more when the organic electroluminescence element is not emitting light.
The organic electroluminescence panel module according to claim 1, further comprising a half mirror between the decorative sheet and the organic electroluminescence element.
3. The organic electroluminescence panel module according to claim 1, further comprising a color difference forming layer whose color tone changes depending on a viewing angle on the organic electroluminescence element.
The organic electroluminescence panel module according to any one of claims 1 to 3, further comprising a mask member between the decorative sheet and the organic electroluminescence element.
5. The organic electroluminescence panel module according to claim 1, wherein the surface protection sheet, the decorative sheet, the organic electroluminescence element, and the back surface protection member all have flexibility. .
The organic electroluminescence panel module according to any one of claims 1 to 5, wherein the total film thickness is in a range of 0.3 to 3.0 mm.