CN110463349B - Electrode for organic electroluminescent element, organic electroluminescent display device, and method for producing electrode for organic electroluminescent element - Google Patents
Electrode for organic electroluminescent element, organic electroluminescent display device, and method for producing electrode for organic electroluminescent element Download PDFInfo
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- CN110463349B CN110463349B CN201880020886.2A CN201880020886A CN110463349B CN 110463349 B CN110463349 B CN 110463349B CN 201880020886 A CN201880020886 A CN 201880020886A CN 110463349 B CN110463349 B CN 110463349B
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/80—Constructional details
- H10K50/805—Electrodes
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/02—Details
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/10—Apparatus or processes specially adapted to the manufacture of electroluminescent light sources
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/12—Light sources with substantially two-dimensional radiating surfaces
- H05B33/22—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of auxiliary dielectric or reflective layers
- H05B33/24—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of auxiliary dielectric or reflective layers of metallic reflective layers
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/12—Light sources with substantially two-dimensional radiating surfaces
- H05B33/26—Light sources with substantially two-dimensional radiating surfaces characterised by the composition or arrangement of the conductive material used as an electrode
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- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/12—Light sources with substantially two-dimensional radiating surfaces
- H05B33/26—Light sources with substantially two-dimensional radiating surfaces characterised by the composition or arrangement of the conductive material used as an electrode
- H05B33/28—Light sources with substantially two-dimensional radiating surfaces characterised by the composition or arrangement of the conductive material used as an electrode of translucent electrodes
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K2102/00—Constructional details relating to the organic devices covered by this subclass
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- Devices For Indicating Variable Information By Combining Individual Elements (AREA)
Abstract
The present invention provides: an organic EL element electrode which suppresses external reflection by reducing the reflectance in the visible light region, can adjust the work function as desired, and can be used for either the anode or the cathode of an organic EL element; and a method for manufacturing an electrode for an organic EL element. The organic EL element electrode (20) is provided, and the organic EL element electrode (20) includes: the organic electroluminescence element electrode comprises a conductive layer (1) mainly composed of a metal or an alloy, a blackened layer (2) provided on the conductive layer and having a reflectance in the visible light region of 40% or less, and a work function adjusting layer (3) provided on the blackened layer and composed of a transparent conductive oxide having a predetermined work function, wherein the reflectance in the visible light region of the organic electroluminescence element electrode is 10% or less, and the sheet resistance is 1 Ω/sq or less.
Description
Technical Field
The present invention relates to an electrode for an organic electroluminescent element, an organic electroluminescent display device, and a method for manufacturing an electrode for an organic electroluminescent element.
Background
In recent years, organic electroluminescent elements (hereinafter referred to as organic EL elements) have been used in various fields, particularly in applications such as displays of smart phones, display devices of thin televisions and the like, and lighting fixtures.
Organic EL panels used in display devices and illumination devices using organic EL elements are roughly classified into two types, top emission type and bottom emission type, depending on the direction of light extraction.
In the top emission type, a TFT (Thin Film Transistor) layer is formed on a substrate, and layers such as an electrode and an organic EL layer are stacked thereon. The top emission type is a type in which light is extracted from the opposite side of the substrate, that is, the opposite side of the TFT circuit. On the other hand, the bottom emission type is a type of extracting light from the substrate side, i.e., a region other than the TFT circuit.
The top emission type organic EL device is suitable for high luminance and high definition because it is free from the restriction of light-shielding materials such as TFTs and wirings and can secure a high aperture ratio as compared with the bottom emission type organic EL device.
In the top emission type organic EL panel, it has been conventionally necessary to provide a circularly polarizing plate on the panel surface to prevent external light reflection between the TFT and the electrode for the organic EL element, and it has been difficult to produce a flexible organic EL panel because several circularly polarizing films must be stacked.
To omit the circularly polarizing plate, it is necessary to prevent external light reflection of the TFT and the organic EL element. Although external light reflection from the TFT array can be prevented by the black matrix, the anode of the organic EL element needs to have a material which has low reflectance of an electrode, conductivity, and a large work function. When the reflective electrode side is used as a cathode, a material having a small work function is required.
Patent document 1 relates to a technique for preventing the formation of a mirror surface in an EL light-emitting device without using a circular polarizing film, and describes: an EL light-emitting element is provided with an anode or a cathode made of an oxide conductive film and a light-shielding film.
Documents of the prior art
Patent document
Patent document 1 Japanese laid-open patent publication No. 2002-033185
Disclosure of Invention
Problems to be solved by the invention
Patent documents 1 to 4 disclose that a light-shielding film and an antireflection layer are provided in an organic EL element to prevent external reflection, but the organic EL element does not have an electrode structure having a low reflectance in the visible light region, good conductivity, and an adjustable work function.
Further, an electrode structure which has a low reflectance in the visible light region, has good conductivity, has an adjustable work function, and can be etched at once has not been realized.
The present invention has been made in view of the above problems, and an object of the present invention is to provide: an organic EL element electrode which suppresses external reflection by reducing the reflectance in the visible light region, can adjust the work function as desired, and can be applied to either the anode or the cathode of an organic EL element; and a method for manufacturing an electrode for an organic EL element.
Another object of the present invention is to provide: an electrode for an organic EL element, which has a low reflectance in the visible light region, has good conductivity, has an adjustable work function, and can be etched at once; and a method for manufacturing an electrode for an organic EL element.
Means for solving the problems
The above object can be achieved by an electrode for an organic electroluminescent element according to the present invention, the electrode for an organic electroluminescent element comprising: the organic electroluminescence element electrode comprises a conductive layer mainly composed of a metal or an alloy, a blackened layer provided on the conductive layer and having a reflectance in a visible light region of 40% or less, and a work function adjusting layer provided on the blackened layer and composed of a transparent conductive oxide having a predetermined work function, wherein the reflectance in the visible light region of the organic electroluminescence element electrode is 10% or less, and the sheet resistance is 1 Ω/sq or less.
According to the above configuration, since the conductive layer is provided with the blackening layer and the work function adjustment layer, it is possible to provide an electrode for an organic EL element which suppresses external reflection by reducing the reflectance in the visible light region, has a small sheet resistance value, and can arbitrarily adjust the work function. Thus, a flexible organic EL panel without a polarizing plate can be formed.
In this case, the electrode for an organic electroluminescence element preferably includes 3 layers including the conductive layer, the black layer, and the work function adjusting layer.
This has the advantage of having a low reflectance in the visible light region and sufficient conductivity, and being usable as an anode and a cathode, and is easy to manufacture and thin because it is composed of a small number of layers of 3.
In this case, the conductive layer is preferably a metal or an alloy containing, as a main component, one or more metals selected from the group consisting of Al, Cu, Ag, Mo, and Cr.
By using these metals or alloys, a low sheet resistance can be achieved by stacking conductive layers by a simple process such as sputtering.
In this case, the blackened layer is preferably made of a lower oxide, a lower nitride, or a lower oxynitride containing Mo or Zn as a main component.
Thus, by using a conductive substance having a high absorbance in the visible light region as the blackening layer, a low reflectance in the visible light region and a good conductivity can be achieved.
In this case, the work function adjusting layer is formed of In2O3Or ZnO as a base, preferably In2O3Is added with a catalyst selected from Ga, Ce,The transparent conductive oxide film is composed of one or more transparent conductive oxides selected from the group consisting of Zn, Sn, Si, W and Ti, or is composed of ZnO to which one or more transparent conductive oxides selected from the group consisting of Al and Ga are added.
Thus, by using a transparent conductive oxide which can be doped with various metals and whose work function can be adjusted depending on the amount of the dopant added as a work function adjusting layer, an electrode which can be used as an anode or a cathode and has a low reflectance in the visible light region can be provided.
In this case, it is preferable that the work function adjusting layer has a work function of 4.6eV or less and the organic electroluminescence element electrode is used as a cathode of the organic electroluminescence element, or the work function adjusting layer has a work function of 4.7eV or more and the organic electroluminescence element electrode is used as an anode of the organic electroluminescence element.
Thus, the work function of the work function adjusting layer is adjusted according to the kind and the addition amount of the dopant added to the transparent conductive oxide serving as the base, and therefore the work function adjusting layer can be used as an anode of the organic EL element and also as a cathode.
The above problems can be solved by an organic electroluminescent element including the electrode for an organic electroluminescent element of the present invention, and an organic electroluminescent display device including the organic electroluminescent element and not including a polarizing plate.
Accordingly, the electrode for an organic electroluminescent element of the present invention has a reduced reflectance in the visible light region, and therefore, when used as an electrode for an organic EL element or an organic EL display device, external reflection can be suppressed, and an organic EL display device without a polarizing plate can be provided.
The above object can be achieved by a method for manufacturing an electrode for an organic electroluminescent element according to the present invention, which comprises the steps of: a conductive layer laminating step of laminating a conductive layer containing, as a main component, one or more metals selected from the group consisting of Al, Cu, Ag, Mo, and Cr on a base material; a step of laminating a blackened layer, in which Mo or Zn is mainly laminated on the conductive layer A black layer which is composed of a lower oxide, a lower nitride, or a lower oxynitride as an essential component and has a reflectance in a visible light region of 40% or less; a work function adjusting layer laminating step of laminating In on the blackened layer2O3Or a work function adjusting layer made of a transparent conductive oxide with ZnO as a base and having a predetermined work function; and an etching step of collectively etching the stacked conductive layer, blackened layer, and work function adjustment layer.
Thus, since the conductive layer, the blackening layer, and the work function adjustment layer are formed using appropriate materials, they can be collectively etched by wet etching using a nitrohydrochloric acid etching solution (a mixed solution of phosphoric acid, nitric acid, and acetic acid), and thus, the electrode can be easily manufactured.
Further, since the conductive layer is provided with the blackening layer and the work function adjusting layer, it is possible to provide an electrode for an organic EL element which suppresses external reflection by reducing the reflectance in the visible light region, has a small sheet resistance, and can arbitrarily adjust the work function.
The above object can be achieved by an electrode for electronic equipment according to the present invention, the electrode for electronic equipment comprising: the electrode for electronic equipment comprises a conductive layer mainly composed of a metal or an alloy, a blackened layer provided on the conductive layer and having a reflectance in a visible light region of 40% or less, and a work function adjusting layer provided on the blackened layer and comprising a transparent conductive oxide having a predetermined work function, wherein the electrode for electronic equipment has a reflectance in a visible light region of 10% or less and a sheet resistance of 1 Ω/sq or less
According to the above configuration, since the conductive layer is provided with the blackening layer and the work function adjustment layer, the reflectance in the visible light region is reduced to suppress external reflection, and the sheet resistance value is small, so that the electrode for electronic equipment, which reduces power consumption of electronic equipment, can be provided.
Effects of the invention
In the electrode for an organic EL element of the present invention, the blackened layer is formed of a lower oxide, a lower nitride, or a lower oxynitride containing Mo or Zn as a main component, which has high conductivity and high absorbance in the visible light region, and therefore, the reflectance can be reduced while maintaining a low sheet resistance value. In addition, since a transparent conductive oxide having an appropriate work function is used as the work function adjusting layer, the electrode can be used as either an anode or a cathode. Further, by combining the blackening layer and the work function adjusting layer, the reflectance in the visible light region can be reduced to 10% or less. Therefore, a flexible organic EL panel without a polarizing plate can be formed.
Further, the conductive layer, the blackening layer, and the work function adjusting layer are selected from materials that can be collectively etched, and therefore, the electrode can be easily manufactured.
Drawings
Fig. 1 is a schematic cross-sectional view showing an electrode for an organic EL element according to an embodiment of the present invention.
Fig. 2 is a flowchart of a method for manufacturing an electrode for an organic EL element according to an embodiment of the present invention.
Fig. 3 is a schematic cross-sectional view showing an organic EL element according to an embodiment of the present invention.
Fig. 4 is a schematic cross-sectional view showing an organic EL element according to a modification of the embodiment of the present invention.
Fig. 5A is a graph showing the measurement results of optical constants of the blackened layers in reference example 1 and reference example 2 of the present invention, and shows refractive indices.
Fig. 5B is a graph showing the results of measuring optical constants of the blackened layers in reference example 1 and reference example 2 of the present invention, and showing extinction coefficients.
Fig. 6 is a graph showing the results of measuring the reflectance of the blackened layers in reference examples 1 to 3 of the present invention.
Fig. 7 is a graph showing the results of measuring the reflectance of the work function adjusting layers of reference examples 4 to 8 of the present invention.
Fig. 8 is a graph showing the results of measuring the reflectance of the electrodes for organic EL elements of example 1 and comparative example 1 of the present invention.
Fig. 9 is a graph showing the results of measuring the reflectance of the electrodes for organic EL elements of examples 2 to 6 of the present invention and comparative example 2.
Fig. 10 is an SEM cross-sectional photograph of a sample obtained by etching the electrode for an organic EL element of example 2.
Fig. 11 is a graph showing the results of measuring the reflectance of the conductive film of example 7 of the present invention.
Detailed Description
An organic EL element electrode, a method for manufacturing the organic EL element electrode, an organic EL element including the organic EL element electrode, and an organic EL display device using the organic EL element according to an embodiment of the present invention will be described below.
< electrode for organic EL element >
As shown in fig. 1, the electrode 20 for an organic EL element according to the present embodiment is formed by laminating a conductive layer 1, a blackened layer 2 formed on the conductive layer 1, and a work function adjusting layer 3 formed on the blackened layer 2. The layers constituting the organic EL element electrode 20 will be described in detail below.
(conductive layer)
The conductive layer 1 is a metal mainly containing one or more selected from the group consisting of Al, Cu, Ag, and Mo, or an alloy selected from the group consisting of APC (an alloy of silver, palladium, and copper), AlNd, AlSi, AlCu, and AlSiCu.
Here, the main components are: the conductive layer may contain 50% by weight or more in terms of a weight ratio.
The metal constituting the conductive layer 1 may be any metal that has sufficient conductivity and can be used for an organic EL element. Examples thereof include, but are not limited to, Al, Cu, Ag, Mo, etc.
The alloy constituting the conductive layer 1 may be any alloy that has sufficient conductivity and can be used for an organic EL element. Examples thereof include: alloys containing Al, Cu, Ag, Mo, etc. as main components; alternatively, an alloy selected from the group consisting of APC (alloy of silver, palladium, copper), AlNd, AlSi, AlCu, AlSiCu, but is not limited thereto.
The thickness of the conductive layer 1 is preferably 10nm or more and 1000nm or less, more preferably 20nm or more and 800nm or less, more preferably 30nm or more and 700nm or less, further preferably 40nm or more and 600nm or less, and further preferably 50nm or more and 500nm or less. When the thickness of the conductive layer 1 is too thin, the conductivity is lowered. On the other hand, when the conductive layer 1 is too thick, the thickness of the organic EL element increases, and the etching processability and manufacturability deteriorate.
(blackened layer)
The blackened layer 2 is a layer composed of a lower oxide, a lower nitride, or a lower oxynitride containing Mo or Zn as a main component, and has a reflectance in the visible light region of 40% or less.
Here, the main components are: mo or Zn contained in the blackened layer may be contained by 50 atomic% or more in terms of an atomic ratio of metal atoms.
The lower oxide, lower nitride, or lower oxynitride constituting the black layer 2 may be any that can sufficiently absorb light in the visible light region and have sufficient conductivity. Examples thereof include, but are not limited to, lower oxides, lower nitrides, and lower oxynitrides containing Mo or Zn as a main component.
The lower oxide containing Mo as main component is MoO x(x is a stoichiometric ratio, 2. ltoreq. x < 3), and the lower nitride containing Mo as a main component means MoNy(y is a stoichiometric ratio), and the lower oxynitride containing Mo as a main component means MoOxNy(x, y are stoichiometric ratios).
The lower oxide containing Zn as main component refers to ZnOx(x is the stoichiometric ratio) and the lower nitride containing Zn as the main component means ZnNy(y is a stoichiometric ratio) and the lower oxynitride containing Zn as a main component means ZnOxNy(x, y ═ stoichiometric).
In addition to the metal other than Mo or Zn as the main component, a dopant metal may be added to the blackening layer 2.
The dopant metal is preferably a transition metal, such as Nb, W, Al, Ni, Cu, Cr, Ti, Ag, Ga, Zn, In, Ta, but is not limited thereto.
The content ratio of the dopant metal to the lower oxide, lower nitride or lower oxynitride containing Mo or Zn as a main component is preferably 20 atomic% or less. When the content ratio of the dopant metal (Nb, Ta, or the like) is within the above range, good conductivity and light absorption in the visible light region can be achieved.
The reflectance of the blackened layer 2 in the visible light region is preferably 50% or less, and more preferably 40% or less. The lower limit of the wavelength of the electromagnetic wave corresponding to visible light is about 360 to 400nm and the upper limit is about 760 to 830nm according to the definition of JIS Z8120, and in the present embodiment, the visible light region is a wavelength region of 400 to 700 nm.
When the black layer 2 has a low visible light transmittance, the visible light reflected by the organic EL element electrode 20 decreases, and thus the organic EL display device can be suitably used for a flexible organic EL display device without a polarizing plate.
The thickness of the blackened layer 2 is preferably 5nm or more and 200nm or less, more preferably 10nm or more and 150nm or less, more preferably 20nm or more and 100nm or less, further preferably 30nm or more and 75nm or less, further preferably 40nm or more and 60nm or less. If the thickness of blackened layer 2 is too small, absorption of light in the visible light region becomes insufficient or film formation becomes difficult. On the other hand, if the blackened layer 2 is too thick, the etching processability and the manufacturability are deteriorated.
(work function adjusting layer)
The work function adjusting layer 3 is a layer made of a transparent conductive oxide having a predetermined work function.
The transparent conductive oxide constituting the work function adjusting layer 3 may be any transparent conductive oxide that has sufficient conductivity and can adjust the work function by adding various metals. Examples of such transparent conductive oxides include In2O3、ZnO、Ga2O3、SnO2、TiO2CdO, and composite oxides thereof, and the like, but are not limited thereto.
In this embodiment, In is preferably used as a material constituting the work function adjusting layer 3 2O3Or ZnO is transparent conductive oxide of the matrix.
As In2O3The transparent conductive oxide as the matrix can be used In the main component In2O3In which at least one selected from the group consisting of Ga, Ce, Zn, Sn, Si, W and Ti is addedA transparent conductive oxide of a metal element.
In this class2O3Among the transparent conductive oxides as the matrix, there can be preferably used: IGO (gallium-doped indium oxide) to which Ga is added, IZO (indium zinc oxide) to which Zn is added, ITO (indium tin oxide) to which Sn is added, ICO (indium cerium oxide) to which Ce, Sn, and Ti are added, and IWZO (tungsten-zinc-doped indium oxide) to which W and Zn are added.
In addition, In2O3The content ratio of the metal element added in (a) is preferably 50% by weight or less. When the content exceeds the above range, the resistance becomes high, which is not preferable.
In is used In2O3The transparent conductive oxide as the base may contain other elements in addition to Ga, Ce, Zn, Sn, Si, W, and Ti within a range that does not impair the performance of the electrode for an organic EL element of the present embodiment.
As the transparent conductive oxide based on ZnO, a transparent conductive oxide in which one or more metal elements selected from the group consisting of Al and Ga are added to ZnO as a main component can be used.
As such transparent conductive oxides based on ZnO, there can be preferably used: AZO (aluminum-doped zinc oxide) to which Al is added, GZO (gallium-doped zinc oxide) to which Ga is added, GAZO (gallium/aluminum-doped zinc oxide) to which Al and Ga are added.
The content ratio of the metal element added to ZnO is preferably 10 wt% or less in terms of weight ratio. When the content exceeds the above range, the resistance becomes high, which is not preferable.
In addition to Al or Ga, the transparent conductive oxide based on ZnO may contain other elements within a range that does not impair the performance of the electrode for an organic EL element according to the present embodiment.
When the organic EL element electrode 20 is used as a cathode, for example, the transparent conductive oxide may be selected so that the work function of the work function adjusting layer 3 is 4.6eV or less.
On the other hand, when the electrode 20 for an organic EL element is used as an anode, for example, the transparent conductive oxide may be selected so that the work function of the work function adjusting layer is 4.7eV or more.
In the present embodiment, various metals are added to the work function adjustment layer 3 to adjust the work function to a predetermined work function, and the addition of various metals causes In to be a base 2O3Or a decrease in crystallinity of ZnO. Therefore, the work function adjusting layer 3 is lowered in crystallinity and amorphized by the addition of the metal, and thus can be etched with a predetermined etchant.
The thickness of the work function adjusting layer 3 is preferably 5nm or more and 150nm or less, more preferably 10nm or more and 100nm or less, more preferably 20nm or more and 80nm or less, further preferably 30nm or more and 60nm or less, and further preferably 40nm or more and 50nm or less. When the thickness of the work function adjusting layer 3 is too thin, absorption of light in the visible light region becomes insufficient, the work function becomes unstable, or film formation becomes difficult. On the other hand, if the work function adjusting layer 3 is too thick, the etching workability and the manufacturing property are deteriorated.
(physical Properties of electrode for organic EL element)
The electrode 20 for an organic EL element of the present embodiment is characterized by having a low reflectance in the visible light region and sufficient conductivity, which can be used in an organic EL display device without a polarizing plate, by adopting the above-described configuration.
The reflectance of the organic EL element electrode 20 in the visible light region (400nm to 700nm) is 10% or less.
The sheet resistance of the electrode 20 for organic EL element is 1 Ω/sq or less, more preferably 0.75 Ω/sq or less, still more preferably 0.5 Ω/sq or less, and particularly preferably 0.25 Ω/sq or less.
The work function of the organic EL element electrode 20 is determined by the work function of the work function adjusting layer 3, and is 4.6eV or less when the organic EL element electrode 20 is used as a cathode, and 4.7eV or more when the organic EL element electrode 20 is used as an anode.
The organic EL element electrode 20 is composed of a small number of 3 layers, including the conductive layer 1, the blackening layer 2, and the work function adjusting layer 3, and the organic EL element electrode 20 has the following advantages: has a low reflectance in the visible light region and sufficient conductivity, and can be used as both an anode and a cathode of an organic EL element by appropriately selecting a material for the work function adjusting layer.
The thickness of the electrode 20 for an organic EL element is preferably 20nm to 1500nm, more preferably 100nm to 1000nm, even more preferably 200nm to 800nm, even more preferably 300nm to 600nm, even more preferably 350nm to 500 nm. When the organic EL element electrode 20 is too thick, the etching workability and the manufacturability are deteriorated.
< method for producing electrode for organic EL element >
The organic EL element electrode 20 of the present embodiment is manufactured by a method for manufacturing an organic EL element electrode, and as shown in fig. 2, the method for manufacturing an organic EL element electrode is characterized by performing the following steps: a conductive layer laminating step of laminating a conductive layer containing, as a main component, one or more metals selected from the group consisting of Al, Cu, Ag, Mo, and Cr on a base material; a blackened layer laminating step of laminating a blackened layer, which is composed of a lower oxide, a lower nitride, or a lower oxynitride containing Mo or Zn as a main component and has a reflectance in a visible light region of 40% or less, on the conductive layer; a work function adjusting layer laminating step of laminating In on the blackened layer 2O3Or a work function adjusting layer made of a transparent conductive oxide with ZnO as a base and having a predetermined work function; and an etching step of collectively etching the stacked conductive layer, the blackening layer, and the work function adjustment layer.
The respective steps will be described in detail below with reference to fig. 2.
(conductive layer lamination Process)
In the conductive layer laminating step (step S1), the conductive layer 1 containing, as a main component, one or more metals selected from the group consisting of Al, Cu, Ag, Mo, and Cr is laminated on the substrate 10. The method of forming the conductive layer 1 on the substrate 10 may be physical vapor deposition such as sputtering, vacuum vapor deposition, or ion plating, but is not limited thereto.
(blackened layer lamination step)
In the blackening layer laminating step (step S2), a blackening layer 2 composed of a lower oxide, a lower nitride, or a lower oxynitride containing Mo or Zn as a main component and having a reflectance in the visible light region of 40% or less is laminated on the conductive layer 1 laminated on the base material 10 in the conductive layer laminating step. As a method for forming blackened layer 2 on conductive layer 1, physical vapor deposition methods such as sputtering, vacuum vapor deposition, and ion plating can be used, but the method is not limited thereto.
In the step of laminating the blackened layers, Mo and ZnO are used as targets and the flow rate of oxygen is set to be 5 to 50sccm in order to obtain a lower oxide, a lower nitride or a lower oxynitride containing Mo or Zn as a main component.
(work function adjusting layer laminating step)
In the work function adjusting layer laminating step (step S3), In is laminated on the blackened layer 2 laminated on the conductive layer 1 In the blackened layer laminating step2O3Or a work function adjusting layer 3 made of a transparent conductive oxide with ZnO as a base and having a predetermined work function. As a method for forming the work function adjusting layer 3 on the blackened layer 2, a physical vapor deposition method such as a sputtering method, a vacuum vapor deposition method, or an ion plating method can be used, but the method is not limited thereto.
In the work function adjusting layer laminating step, In is obtained2O3Or ZnO as a base, and ITO or GZO as a target and an oxygen flow rate of 5sccm were used.
If the conductive layer 1, the blackening layer 2, and the work function adjusting layer 3 are formed by, for example, a vacuum deposition method and/or a sputtering method, the electrode 20 for an organic EL element can be continuously formed on the substrate 10 by a dry process.
(etching Process)
In the etching step (step S4), the conductive layer 1, the blackened layer 2, and the work function adjusting layer 3 stacked on the substrate 10 are collectively etched. For example, a photoresist is applied to the conductive layer 1, the blackening layer 2, and the work function adjusting layer 3 stacked on the base material 10 by a photolithography technique, exposure and development are sequentially performed to transfer a mask pattern to the resist, and portions other than portions to be left as electrodes are removed by etching. Then, the resist was removed to obtain a remaining portion as the electrode 20 for organic EL element.
As for the etching method, it is possible to utilize: wet etching using an etching solution, or dry etching such as reactive gas etching, reactive ion beam etching, or reactive laser beam etching.
In the present embodiment, since the conductive layer 1, the blackened layer 2, and the work function adjusting layer 3 are formed using the above-described materials, they can be etched at once by wet etching using a nitrohydrochloric acid etching solution (a mixed solution of phosphoric acid, nitric acid, and acetic acid).
< organic light emitting element >
As shown in fig. 3, a top emission type organic EL device 100 including the organic EL device electrode 20 of the present embodiment as an Anode (Anode) includes a substrate 10, the organic EL device electrode 20, a hole transport layer 30, an organic light emitting layer 40, an electron transport layer 50, and a transparent electrode 60, which are stacked in this order, and light emission L is extracted from the opposite side of the substrate 10.
The organic EL element electrode 20 of the present embodiment has an advantage that the reflectance in the visible light region is 10% or less, and the reflection of external light is suppressed, so that the use of a polarizing plate is not required.
The respective constituent elements of the organic EL element 100 will be described in detail below.
(substrate)
The substrate 10 constituting the organic EL device 100 of the present invention may be any substrate as long as it does not change when forming the electrode and the organic layer, and for example, glass, plastic, a polymer film, a silicon substrate, a substrate obtained by laminating these materials, or the like may be used.
(hole transport layer)
As materials constituting the hole transport layer 30, there can be mentioned: polyvinylcarbazole or a derivative thereof, polysilane or a derivative thereof, a polysiloxane derivative having an aromatic amine in a side chain or a main chain, a pyrazoline derivative, an arylamine derivative, a stilbene derivative, a triphenyldiamine derivative, polyaniline or a derivative thereof, polythiophene or a derivative thereof, polyarylamine or a derivative thereof, polypyrrole or a derivative thereof, poly (phenylene vinylene) or a derivative thereof, or poly (2, 5-thiophenylene) or a derivative thereof, and the like.
The method for forming the hole transport layer 30 is not particularly limited, and in the case of a low molecular weight hole transport material, a method of forming a film from a mixed solution with a polymer binder is exemplified, and in the case of a high molecular weight hole transport material, a method of forming a film from a solution is exemplified.
The film thickness of the hole transport layer 30 may be selected to have an optimum value depending on the material so that the driving voltage and the light emission efficiency are appropriate values, but it is necessary to have a thickness at least not causing pinholes. When the film thickness is too large, the driving voltage of the organic EL element 100 increases, and therefore, the film thickness of the hole transport layer 30 is, for example, 1nm to 1 μm, preferably 2nm to 500nm, and more preferably 5nm to 200 nm.
(organic light-emitting layer)
The organic light-emitting layer 40 contains an organic substance (low molecular compound or high molecular compound) that emits fluorescence or phosphorescence. It is noted that a dopant material may be further included. Examples of the material for forming the organic light-emitting layer 40 that can be used in this embodiment include, but are not limited to, dye-based materials, metal complex-based materials, and polymer-based materials.
In addition, a dopant may be added to the organic light emitting layer 40 in order to improve light emitting efficiency, change light emitting wavelength, and the like.
The method for forming the organic light-emitting layer 40 is not particularly limited, and a method of applying a solution containing a light-emitting material onto or over a substrate, a vacuum evaporation method, a transfer method, or the like can be used.
The thickness of the organic light emitting layer 40 is generally
(Electron transport layer)
As the material constituting the electron transport layer 50, known materials can be used, and examples thereof include: oxadiazole derivatives, anthraquinone dimethane or derivatives thereof, benzoquinone or derivatives thereof, naphthoquinone or derivatives thereof, anthraquinone or derivatives thereof, tetracyanoanthraquinone dimethane or derivatives thereof, fluorenone derivatives, diphenyldicyanoethylene or derivatives thereof, diphenoquinone derivatives, or metal complexes of 8-hydroxyquinoline or derivatives thereof, polyquinoline or derivatives thereof, polyquinoxaline or derivatives thereof, polyfluorene or derivatives thereof, and the like.
The method for forming the electron transport layer 50 is not particularly limited, and in the case of a low molecular electron transport material, a vacuum vapor deposition method using a powder or a method for forming a film from a solution or a molten state may be used, and in the case of a high molecular electron transport material, a method for forming a film from a solution or a molten state may be used.
The film thickness of the electron transport layer 50 may be selected to have an optimum value depending on the material so that the driving voltage and the light emission efficiency can be appropriately set, but it is necessary to have a thickness at least not causing pinholes. If the film thickness is too large, the driving voltage of the organic EL element 100 increases, and therefore, the film thickness of the electron transport layer 50 is, for example, 1nm to 1 μm, preferably 2nm to 500nm, and more preferably 5nm to 200 nm.
(transparent electrode)
Since the organic EL element 100 of the present embodiment emits light by penetrating the transparent electrode 60, the transparent electrode 60 needs to be a transparent or translucent electrode.
In the organic EL element 100 of the present embodiment, when the electrode 20 for an organic EL element is used as an anode, a material having a small work function and easily injecting electrons into the electron transport layer 50 and the organic light emitting layer 40 is preferable as a material constituting the transparent electrode 60 as a cathode. For example, a conductive metal oxide, a conductive organic substance, or the like can be used. Specifically, as the conductive metal oxide, indium oxide, zinc oxide, tin oxide, and ITO and IZO which are a composite of these can be used, but the present invention is not limited thereto. As the conductive organic material, an organic transparent conductive film such as polyaniline or a derivative thereof, polythiophene or a derivative thereof, or the like can be used, but not limited thereto.
(modification of organic light-emitting device)
Fig. 3 shows a top emission type organic EL element 100 including the organic EL element electrode 20 of the present embodiment as an Anode (Anode), but the organic EL element electrode 20 of the present embodiment can also be used as a Cathode (Cathode).
Fig. 4 shows an organic EL element 100 'using an organic EL element electrode 20' as a cathode, as a modification of the present embodiment. In the organic EL element 100 ', the substrate 10, the organic EL element electrode 20', the electron transport layer 50, the organic light-emitting layer 40, the hole transport layer 30, and the transparent electrode 60 'are sequentially stacked and formed, and the position of the electron transport layer 50 and the position of the hole transport layer 30 are different because the organic EL element electrode 20' is used as a cathode.
Here, in the organic EL element 100 ' according to the modification of the present embodiment, the organic EL element electrode 20 ' is used as a cathode, and a material having a large work function and easily injecting holes into the hole transport layer 30 and the organic light emitting layer 40 is preferable as a material constituting the transparent electrode 60 ' as an anode. As the transparent electrode or the translucent electrode, a thin film of a metal oxide, a metal sulfide, or a metal having high electrical conductivity can be used. As the transparent electrode, indium oxide, zinc oxide, tin oxide, and ITO and IZO which are a composite of these are preferable, but not limited thereto.
(organic light emitting device)
Since the organic EL elements 100 and 100' of the present embodiment have low reflectance in the visible light region and suppress external reflection, an organic EL display device without a polarizing plate can be manufactured without using a polarizing plate.
Examples of the organic EL display device include, but are not limited to, displays of portable terminals such as smart phones and tablet terminals, displays of thin-type televisions, and the like.
If a flexible substrate such as a plastic film is selected as the substrate 10, a flexible organic EL display device can be obtained.
In this embodiment, the electrode for an organic EL element, the organic EL display device, and the method for manufacturing the electrode for an organic EL element according to the present invention are mainly described.
However, the above-described embodiments are merely examples for facilitating understanding of the present invention, and do not limit the present invention. The present invention can be modified and improved without departing from the gist thereof, and it is needless to say that the present invention also includes equivalent inventions.
Examples
Hereinafter, specific examples of the electrode for an organic EL element of the present invention will be described, but the present invention is not limited thereto.
< A. formation of electrodes for organic EL elements of examples and comparative examples >
(A-1. Process for Forming conductive layer)
The conductive layers of examples 1 to 6 and comparative examples 1 and 2 were stacked on a substrate under the following conditions.
A sputtering device: rotary disk type intermittent sputtering device
Target: 5 'X25', thickness 6mm, aluminum (Al) 100%
A sputtering mode: DC magnetron sputtering
An exhaust device: turbo molecular pump
Reaching the vacuum degree: 5X 10－4Pa
Base material temperature: 25 ℃ (room temperature)
Sputtering power: 6kW
Film thickness of conductive layer: 300 +/-10 nm
Ar flow rate: 250sccm
Using a substrate: glass substrate (1.1mm thick)
(A-2. procedure for laminating blackened layer)
On the conductive layers of example 1 and comparative example 1, MoNbO as a blackened layer was laminated under the following conditionsx(x is a stoichiometric ratio), MoO as a black layer was stacked on the conductive layers of examples 2 to 6 and comparative example 2x(x is the stoichiometric ratio).
A sputtering device: rotary disk type intermittent sputtering device
Target:
example 1. 5 ". times.25", thickness 6mm, Mo 90 atom%, Nb 10 atom%
Comparative example 1)5 ". times.25", thickness 6mm, Mo 90 atom%, Nb 10 atom%
(examples 2 to 6)5 '. times.25', 6mm thick, Mo 100 atom%
Comparative example 25 ". times.25", thickness 6mm, Mo 100 atom%
A sputtering mode: DC magnetron sputtering
An exhaust device: turbo molecular pump
Reaching the vacuum degree: 5X 10－4Pa
Base material temperature: 25 ℃ (room temperature)
Sputtering power: 3kW
Film thickness of blackened layer: 50 +/-5 nm
Ar flow rate: 250sccm
Oxygen flow rate: 50sccm
(A-3. work function adjusting layer laminating step)
IGO (gallium-doped indium oxide) as a work function adjusting layer was stacked on the blackened layers of examples 1 to 6 under the following conditions. On the other hand, the work function adjusting layer was not laminated on the blackening layer of comparative examples 1 and 2.
A sputtering device: rotary disk type intermittent sputtering device
Target:
example 1 In 5 ". times.25", thickness 6mm2O360% by weight Ga2O340% by weight
Example 2 In 5 ". times.25", thickness 6mm2O360% by weight Ga2O340% by weight
Example 3 In 5 ". times.25", thickness 6mm2O390% by weight of Sn2O310% by weight
Example 4 In 5 ". times.25", thickness 6mm2O390% by weight, ZnO 10% by weight
Example 5 ". times.25", thickness 6mm, In2O386.5 wt.% of CeO 210% by weight SnO23.2 wt.% TiO20.3% by weight
Example 6 In 5 ". times.25", thickness 6mm2O396.5 weight portionsAmount% WO33.0% by weight, ZnO 0.5% by weight
A sputtering mode: DC magnetron sputtering
An exhaust device: turbo molecular pump
Reaching the vacuum degree: 5X 10－4Pa
Base material temperature: 25 ℃ (room temperature)
Sputtering power: 2kW
Film thickness of work function adjusting layer: 35 +/-5 nm
Ar flow rate: 100sccm
Oxygen flow rate: 5sccm
Reference example blackening layer or work function adjusting layer formation
(B-1. procedure for laminating blackened layer)
The blackened layers of reference examples 1 to 3 were laminated on a base material under the following conditions.
A sputtering device: rotary disk type intermittent sputtering device
Target:
(reference example 1)5 ". times.25", thickness 6mm, Mo 100 atom%
(reference example 2)5 ". times.25", thickness 6mm, Mo 90 atom%, Nb 10 atom%
(reference example 3)5 "X25", thickness 6mm, Mo 90 atom%, Nb 7 atom%, Ta3 atom%
A sputtering mode: DC magnetron sputtering
An exhaust device: turbo molecular pump
Reaching the vacuum degree: 5X 10－4Pa
Base material temperature: 25 ℃ (room temperature)
Sputtering power: 3kW
Film thickness of blackened layer: 50 +/-5 nm
Ar flow rate: 250sccm
Oxygen flow rate: 50sccm
(B-2. working procedure for laminating work function adjusting layer)
The work function adjusting layers of reference examples 4 to 8 were stacked on a base material under the following conditions.
A sputtering device: rotary disk type intermittent sputtering device
Target:
reference example 4 In 5 ". times.25" thickness 6mm2O360% by weight Ga2O340% by weight
Reference example 5 In 5 ". times.25", thickness 6mm2O390% by weight of Sn2O310% by weight
(reference example 6)5 '. times.25', 6mm In thickness2O390% by weight, ZnO 10% by weight
(reference example 7)5 ". times.25", thickness 6mm, In2O386.5 wt.% of CeO 210% by weight SnO23.2 wt.% TiO20.3% by weight
(reference example 8)5 ". times.25", thickness 6mm, In2O396.5 wt.%, WO33.0% by weight, ZnO 0.5% by weight
A sputtering mode: DC magnetron sputtering
An exhaust device: turbo molecular pump
Reaching the vacuum degree: 5X 10－4Pa
Base material temperature: 25 ℃ (room temperature)
Sputtering power: 2kW
Film thickness of work function adjusting layer: 35 +/-5 nm
Ar flow rate: 100sccm
Oxygen flow rate: 5sccm
< C. various experiments
(reference test 1: measurement of optical constant of blackened layer)
The optical constants of the blackened layers of reference examples 1 and 2 were measured. The optical constants were measured by using a spectroscopic ellipsometer (M-220, manufactured by Nippon spectral Co., Ltd.).
The results are shown in FIGS. 5A and 5B. Fig. 5A is a graph showing the refractive index, and fig. 5B is a graph showing the extinction coefficient.
The refractive index n and the extinction coefficient k at 550nm are shown in Table 1.
[ Table 1]
(reference test 2: measurement of reflectance of blackened layer)
The reflectance of the blackened layers of reference examples 1 to 3 was measured. The reflectance was measured in a wavelength region of 350nm to 800nm using a spectrophotometer (manufactured by Hitachi High-Technologies, U-4100, Ltd.).
The results are shown in FIG. 6.
The reflectance of the black layer in reference examples 1 to 3 was about 25% or more and 40% or less, and it was found that the reflectance in the visible light region could not be reduced to 10% or less in the case where only the black layer was laminated.
(reference test 3: measurement of reflectance of work function adjusting layer)
The reflectance of the work function adjusting layers of reference examples 4 to 8 was measured. The reflectance was measured in a wavelength region of 350nm to 800nm using a spectrophotometer (manufactured by Hitachi High-Technologies, U-4100, Ltd.).
The results are shown in FIG. 7.
It is understood that the reflectance of the work function adjusting layers in reference examples 4 to 8 is greater than 10%, and that the reflectance in the visible light region cannot be reduced to 10% or less when only the work function adjusting layers are stacked.
(reference test 4: work function measurement of work function adjusting layer)
The work functions of the work function adjusting layers of reference examples 4 to 8 were measured.
Work function was calculated using an atmospheric photoelectron spectroscopy apparatus (equipment name AC-2, manufactured by Rigaku corporation).
The results are shown in table 2 below.
[ Table 2]
(test 1: measurement of reflectance of electrode for organic EL element)
The reflectance of the electrodes of examples (examples 1 to 6) and comparative examples (comparative example 1 and comparative example 2) was measured. The reflectance was measured in a wavelength region of 350nm to 800nm using a spectrophotometer (manufactured by Hitachi High-Technologies, U-4100, Ltd.).
The results are shown in fig. 8 and 9.
In fig. 8, the reflectance of comparative example 1 shown by a broken line is 10% or more. On the other hand, the reflectance of example 1 shown by the solid line was only 7.4% (535nm) at the maximum, and showed a low value of 10% or less over the entire visible light region of 400nm to 700 nm.
In fig. 9, the reflectance of comparative example 2 shown by a dotted line is 10% or more. On the other hand, the reflectance of examples 2 to 6 was as low as 10% or less over the entire visible light region of 400nm to 700 nm.
From these results, it was found that when only the black layer was laminated on the conductive layer, the reflectance in the visible light region could not be reduced to 10% or less, and the reflectance in the visible light region could be reduced to 10% or less by configuring the conductive layer, the black layer, and the work function adjusting layer as 3 layers.
(test 2: measurement of sheet resistance and work function of electrode for organic EL element)
The sheet resistance of the electrodes of example 1 and comparative example 1 was measured by a four-terminal method using a resistivity meter (MCP-T610, product of Analytech, Mitsubishi chemical corporation).
The work functions of the electrodes of examples 1 to 6 and comparative examples 1 and 2 were calculated using an atmospheric photoelectron spectroscopy apparatus (equipment name AC-2, manufactured by seikagaku corporation).
The results are shown in table 3 below.
[ Table 3]
As is clear from the above, the electrode of example 1 exhibited a sufficiently small value of 0.11 Ω/sq in sheet resistance, and was usable as an electrode for an organic EL element. The electrode of example 1 showed the same value as the sheet resistance value of comparative example 1 having no work function adjusting layer, and it was found that the work function adjusting layer did not affect the sheet resistance value and the reflectance in the visible light region could be made 10% or less.
Further, the work function of the work function adjusting layer can be set to an arbitrary value depending on the kind of the dopant added to the transparent conductive oxide which becomes the base, and therefore, it is known that the work function adjusting layer can be used as both an anode and a cathode of the organic EL element.
(test 3: evaluation of etching)
The electrode of example 2 was evaluated for etching.
A photoresist (OFPR-800 LB, tokyo chemical) was coated on the conductive film of example 2, and a patterned reticle was used to irradiate an ultraviolet ray, thereby leaving a pattern on the photoresist. The uncured photoresist is removed using a developer (TMAH (tetramethylammonium hydroxide) aqueous solution), the pattern of the original plate is developed, and unnecessary portions of the conductive film from which the photoresist has been removed are etched and removed using an etchant (phosphoric acid, nitric acid, acetic acid mixed solution). Then, the photoresist remaining on the conductive film was stripped and washed, and the etching sample of example 2 was obtained.
Then, SEM cross-sectional analysis was performed on the etching sample of example 2 (S-4300 manufactured by Hitachi High-Tech field).
An SEM cross-sectional photograph of the etching sample of example 2 is shown in fig. 10. As shown in fig. 10, an etched surface was observed as a clear boundary, and it was found that favorable etching was performed.
Example 7 Al-Nd/nitrided Mo-Nb/IGO conductive film
An Al-Nd alloy layer (330 nm thick), a Mo-Nb alloy nitride layer (40 nm thick), and an IGO layer (30 nm thick) were formed on a glass substrate as the conductive film of example 7 by the following steps.
An Al-Nd alloy layer was formed on a glass substrate to a film thickness of 330nm by a DC magnetron sputtering method.
Then, a Mo-Nb alloy nitride layer was formed on the Al-Nd alloy layer by changing the target, film thickness, sputtering power, and introduced gas as described below.
Target: Mo-Nb target with thickness of 9mm
Sputtering power：1.5W/cm2
Film thickness: 40nm
Ar flow rate: 500sccm
·N2Flow rate: 88sccm
Then, the target, film thickness, sputtering power, and introduced gas were changed as described below to form an IGO layer on the nitrided layer of the Mo — Nb alloy.
Target: IGO 6t 5 "X62" target
Sputtering power: 2.5W/cm2
Film thickness: 30nm
Ar flow rate: 500sccm
·O2Flow rate: 12sccm
By the above operation, the conductive film of example 7 was obtained.
Characteristics of good conductive film
The characteristics of the conductive film of example 7 formed as described above were measured.
Resistance value and reflectance of conductive film of example 7
The reflectance of the conductive film of example 7 in the visible light region with a wavelength of 400nm to 700nm was measured using a spectrophotometer (U-4100, manufactured by Hitachi Ltd.). The resistance value was measured using a resistivity meter (Loresta GP, manufactured by mitsubishi chemical corporation), and the reflectance was measured using a film thickness meter (DEKTAKXT, manufactured by ULVAC). The measurement results of the reflectance are shown in fig. 11, and the measurement results of the resistance value and the film thickness are shown in table 4.
[ Table 4]
In fig. 11, the reflectance of the conductive film of example 7 shown by a solid line is low at 10% or less over the entire visible light region of 400nm to 700 nm.
It is also understood that the conductive film of example 7 has a sufficiently small sheet resistance value of 0.16 Ω/sq, and can be used as a conductive film.
Although the electrode of the present invention has been described as an example of an electrode for an organic EL element as a specific example, the electrode of the present invention has low resistance and low reflectance of about 10% or less in the visible light region, and therefore, the application thereof is not limited to the electrode for an organic EL element, and the electrode can be used as an electrode for an electronic device and an electrode for an optical device.
As such an electronic device, a capacitive input device of a touch panel is exemplified. Here, the touch panel refers to a touch sensor-integrated display device integrally including a touch sensor and a display device. As the touch panel, there are the following types: a touch panel manufactured by bonding a touch sensor substrate, which has a pattern formed of a transparent conductive film on a transparent substrate as a detection electrode, to a viewing side of a display device such as a liquid crystal device; a touch panel of a touch sensor integrated display device is manufactured by forming a touch sensor electrode pattern on a substrate of the display device.
In electronic devices such as touch panels in which a substrate with electrodes is disposed in front of a display element, it is a necessary condition that visibility of display is not impaired, and therefore shielding, scattering, diffusion, reflection, and the like of the electrodes are required to be as small as possible.
According to the electrode of the present invention, since the reflectance in the visible light region is 10% or less, glare can be suppressed even when the electrode is used for an electrode of a capacitive touch panel input device, a decrease in the contrast of a display can be suppressed, and the sheet resistance is as low as 1 Ω/sq or less, so that power consumption of an electronic device such as a capacitive input device can be reduced.
Description of the symbols
1 conductive layer
2 blackened layer
3 work function adjusting layer
10 base material
20. Electrode for 20' organic EL element
30 hole transport layer
40 organic light emitting layer
50 electron transport layer
60. 60' transparent electrode
100. 100' organic EL element
L luminescence
Claims (13)
1. An electrode for an organic electroluminescent element, comprising:
a conductive layer containing a metal or an alloy as a main component,
A black layer having a reflectance of 40% or less in a visible light region provided on the conductive layer, and
a work function adjusting layer made of a transparent conductive oxide provided on the blackened layer and having a predetermined work function,
the conductive layer is a metal or alloy containing one or more metals selected from the group consisting of Al, Cu, Ag, Mo and Cr as a main component,
the blackened layer is a physically deposited film of a lower oxide, a lower nitride or a lower oxynitride containing Mo or Zn as a main component,
the work function adjusting layer is formed of In2O3Or ZnO is used as the transparent conductive oxide of the matrix,
the electrode for an organic electroluminescent element has a reflectance of 10% or less in the visible light region,
the sheet resistance is 1 omega/sq or less.
2. The electrode for an organic electroluminescent element according to claim 1, wherein the electrode for an organic electroluminescent element is composed of 3 layers, and the 3 layers include the conductive layer, the blackening layer, and the work function adjusting layer.
3. The electrode for an organic electroluminescent element according to claim 1, wherein the electrode can be collectively etched by wet etching using a phosphorus, nitric and acetic acid etching solution which is a mixed solution of phosphoric acid, nitric acid and acetic acid.
4. The electrode for organic electroluminescent element according to claim 1, wherein the black layer is formed of a lower oxide, a lower nitride, or a lower oxynitride containing Mo as a main component.
5. The electrode according to claim 1, wherein the work function adjusting layer is formed of In2O3A transparent conductive oxide which is a base.
6. The electrode according to claim 1, wherein the work function adjusting layer is composed of In2O3The transparent conductive oxide is added with more than one selected from the group consisting of Ga, Ce, Zn, Sn, Si, W and Ti.
7. The electrode according to claim 1, wherein the work function adjustment layer is formed of a transparent conductive oxide in which at least one selected from the group consisting of Al and Ga is added to ZnO.
8. The electrode for an organic electroluminescent element according to claim 1, wherein the work function of the work function adjusting layer is 4.6eV or less, and the electrode for an organic electroluminescent element is used as a cathode of an organic electroluminescent element.
9. The electrode for an organic electroluminescent element according to claim 1, wherein a work function of the work function adjusting layer is 4.7eV or more, and the electrode for an organic electroluminescent element is used as an anode of an organic electroluminescent element.
10. An organic electroluminescent element comprising the electrode for an organic electroluminescent element according to any one of claims 1 to 9.
11. An organic electroluminescent display device comprising the organic electroluminescent element according to claim 10 and not comprising a polarizing plate.
12. A method for manufacturing an electrode for an organic electroluminescent element, characterized by performing the following steps:
a conductive layer laminating step of laminating a conductive layer mainly containing at least one metal selected from the group consisting of Al, Cu, Ag, Mo, and Cr on a base material;
a blackened layer laminating step of laminating a blackened layer, which is composed of a lower oxide, a lower nitride, or a lower oxynitride containing Mo or Zn as a main component and has a reflectance in a visible light region of 40% or less, on the conductive layer by a physical vapor deposition method;
a work function adjusting layer laminating step of laminating In on the blackened layer2O3Or a work function adjusting layer made of a transparent conductive oxide with ZnO as a base and having a predetermined work function; and
And an etching step of collectively etching the stacked conductive layer, the blackened layer, and the work function adjusting layer by wet etching using a phosphorus-nitro-acetic acid etching solution which is a mixed solution of phosphoric acid, nitric acid, and acetic acid.
13. An electrode for an electronic device, comprising:
a conductive layer containing a metal or an alloy as a main component,
A black layer having a reflectance in a visible light region of 40% or less, provided on the conductive layer, and
a work function adjusting layer made of a transparent conductive oxide and provided on the blackened layer and having a predetermined work function,
the conductive layer is a metal or alloy containing at least one metal selected from the group consisting of Al, Cu, Ag, Mo and Cr as a main component,
the blackened layer is a physically deposited film of a lower oxide, a lower nitride or a lower oxynitride containing Mo or Zn as a main component,
the work function adjusting layer is formed of In2O3Or ZnO is used as the transparent conductive oxide of the matrix,
the electrode for electronic equipment has a reflectance of 10% or less in the visible light region,
the sheet resistance is 1 omega/sq or less.
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| JP2017-065598 | 2017-03-29 | ||
| JP2017065598A JP6975543B2 (en) | 2017-03-29 | 2017-03-29 | A method for manufacturing an electrode for an organic electroluminescence element, an organic electroluminescence element, an organic electroluminescence display device, and an electrode for an organic electroluminescence element. |
| PCT/JP2018/012968 WO2018181573A1 (en) | 2017-03-29 | 2018-03-28 | Electrode for organic electroluminescence element, organic electroluminescence element, organic electroluminescence display device, and method for manufacturing electrode for organic electroluminescence element |
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| CN109917968A (en) * | 2019-03-28 | 2019-06-21 | 京东方科技集团股份有限公司 | A kind of conductive structure, touch-control structure and touch control display apparatus |
| WO2020202284A1 (en) * | 2019-03-29 | 2020-10-08 | シャープ株式会社 | Display device |
| KR20210018641A (en) | 2019-08-07 | 2021-02-18 | 삼성디스플레이 주식회사 | Conductive pattern, display device including conductive pattern, and method of manufacturing conductive pattern |
| CN111244114B (en) | 2020-02-10 | 2023-10-17 | Tcl华星光电技术有限公司 | display panel |
| US20220115468A1 (en) * | 2020-03-27 | 2022-04-14 | Boe Technology Group Co., Ltd. | Display Panel and Manufacturing Method thereof, and Electronic Device |
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| JP2002033185A (en) | 2000-05-06 | 2002-01-31 | Semiconductor Energy Lab Co Ltd | Light emitting device and electric apparatus |
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| JP2003115389A (en) * | 2001-10-02 | 2003-04-18 | Hitachi Ltd | Organic electric field light emitting element |
| KR100472502B1 (en) * | 2001-12-26 | 2005-03-08 | 삼성에스디아이 주식회사 | Organic electro luminescence display device |
| JP2004303481A (en) | 2003-03-28 | 2004-10-28 | Sanyo Electric Co Ltd | Light-emitting element and emission display device |
| GB2404284B (en) * | 2003-07-10 | 2007-02-21 | Dainippon Printing Co Ltd | Organic electroluminescent element |
| JP2005222724A (en) * | 2004-02-03 | 2005-08-18 | Seiko Epson Corp | Electro-optical device, its manufacturing method and electronic equipment |
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| CN1333924A (en) * | 1998-12-08 | 2002-01-30 | 剑桥显示技术有限公司 | Display devices |
| JP2001176674A (en) * | 1999-12-14 | 2001-06-29 | Tdk Corp | Organic electroluminescent element |
| JP2007329363A (en) * | 2006-06-09 | 2007-12-20 | Canon Inc | Organic el device and manufacturing method thereof |
| CN103378312A (en) * | 2012-04-19 | 2013-10-30 | 株式会社东芝 | Display device |
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| CN110463349A (en) | 2019-11-15 |
| KR20190132378A (en) | 2019-11-27 |
| JP6975543B2 (en) | 2021-12-01 |
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| WO2018181573A1 (en) | 2018-10-04 |
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