WO2011126097A1 - 有機led素子、透光性基板、および有機led素子の製造方法 - Google Patents
有機led素子、透光性基板、および有機led素子の製造方法 Download PDFInfo
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- WO2011126097A1 WO2011126097A1 PCT/JP2011/058853 JP2011058853W WO2011126097A1 WO 2011126097 A1 WO2011126097 A1 WO 2011126097A1 JP 2011058853 W JP2011058853 W JP 2011058853W WO 2011126097 A1 WO2011126097 A1 WO 2011126097A1
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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
- H10K50/85—Arrangements for extracting light from the devices
- H10K50/854—Arrangements for extracting light from the devices comprising scattering means
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/12—Silica-free oxide glass compositions
- C03C3/16—Silica-free oxide glass compositions containing phosphorus
- C03C3/21—Silica-free oxide glass compositions containing phosphorus containing titanium, zirconium, vanadium, tungsten or molybdenum
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C8/00—Enamels; Glazes; Fusion seal compositions being frit compositions having non-frit additions
- C03C8/02—Frit compositions, i.e. in a powdered or comminuted form
- C03C8/08—Frit compositions, i.e. in a powdered or comminuted form containing phosphorus
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C8/00—Enamels; Glazes; Fusion seal compositions being frit compositions having non-frit additions
- C03C8/14—Glass frit mixtures having non-frit additions, e.g. opacifiers, colorants, mill-additions
- C03C8/16—Glass frit mixtures having non-frit additions, e.g. opacifiers, colorants, mill-additions with vehicle or suspending agents, e.g. slip
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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
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K2102/00—Constructional details relating to the organic devices covered by this subclass
- H10K2102/301—Details of OLEDs
- H10K2102/351—Thickness
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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
- 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
- H10K50/81—Anodes
- H10K50/813—Anodes characterised by their shape
Definitions
- the present invention relates to an organic LED element, a translucent substrate, and a method for manufacturing the organic LED element.
- Organic LED (Light Emitting Diode) elements are widely used for displays, backlights, lighting applications, and the like.
- a general organic LED element has a first electrode (anode) placed on a substrate, a second electrode (cathode), and an organic layer placed between these electrodes.
- a voltage is applied between the electrodes, holes and electrons are injected from each electrode into the organic layer.
- binding energy is generated, and the organic light emitting material in the organic layer is excited by the binding energy. Since light is emitted when the excited light emitting material returns to the ground state, a light emitting (LED) element can be obtained by utilizing this.
- a transparent thin film such as ITO (Indium Tin Oxide) is used for the first electrode, that is, the anode, and a metal thin film such as aluminum and silver is used for the second electrode, that is, the cathode.
- ITO Indium Tin Oxide
- the light scattering layer is made of resin
- Patent Document 1 since the configuration of the invention is disclosed in a partial sectional view as shown in FIG. 4 of the document, the positional relationship between the substrate, the light scattering layer, and the transparent electrode is unclear. .
- the organic LED element is often configured as shown in FIG. Therefore, when the light scattering layer of Patent Document 1 is applied to Patent Document 2, the light scattering layer is provided between the anode 12 and the glass substrate 11 of FIG.
- the difference in level of the stepped portion is larger by adding the thickness of the light scattering layer to the thickness of the anode 12.
- the side surface of the resin layer is often substantially perpendicular to the upper surface.
- the anode 12 In such a state, it becomes extremely difficult to form the anode 12 at the stepped portion. Alternatively, even if the anode 12 can be formed on the stepped portion, there may arise a problem that the anode 12 cannot have a desired state (for example, thickness, uniformity, adhesion). Further, in this case, since the thickness of the anode 12 is locally reduced and current is concentrated there, there is a possibility that the anode 12 is deteriorated or further broken.
- a desired state for example, thickness, uniformity, adhesion
- the resin-made light scattering layer is likely to undergo heat shrinkage, and even if the entire light scattering layer can be covered with the thin film of the anode 12, in such a configuration, the light scattering layer is subjected to heat shrinkage.
- the anode 12 may be peeled or cracked.
- the present invention has been made in view of such a problem, and an object of the present invention is to provide an organic LED element having higher reliability than conventional ones.
- the present invention provides the following organic LED element, translucent substrate, and organic LED element manufacturing method.
- an organic LED element having a second electrode formed on the organic light emitting layer has a base material made of glass, and a plurality of scattering materials dispersed in the base material,
- the light scattering layer has a bottom surface on the transparent substrate side, a top surface on the first electrode side, and a side surface, and the side surface of the light scattering layer is directed from the top surface to the bottom surface, Having a surface inclined at a gentler angle than a right angle;
- the organic LED element, wherein the first electrode is disposed so as to continuously cover the side surface of the light scattering layer.
- the first electrode terminal includes a first barrier layer disposed on the transparent substrate, and a first conductive layer disposed on the first barrier layer and electrically connected to the first electrode.
- the second electrode terminal includes a second barrier layer disposed on the transparent substrate, and a second conductive layer disposed on the second barrier layer and electrically connected to the second electrode.
- the organic LED element according to (1) comprising: a layer.
- the first conductive layer is made of the same material as the first electrode, and / or the second conductive layer is made of the same material as the first electrode, The organic LED element according to (2) or (3).
- the organic LED element according to any one of (1) to (7), wherein the light scattering layer has a thickness in a range of 5 ⁇ m to 50 ⁇ m.
- a translucent substrate having a transparent substrate, a light scattering layer formed on the transparent substrate, and a transparent electrode formed on the light scattering layer,
- the light scattering layer has a base material made of glass, and a plurality of scattering materials dispersed in the base material,
- the light scattering layer has a bottom surface on the transparent substrate side, a top surface on the transparent electrode side, and a side surface, and the side surface of the light scattering layer is perpendicular to the bottom surface from the top surface.
- the transparent electrode wherein the transparent electrode is installed so as to continuously cover the side surface of the light scattering layer.
- (11) A method of manufacturing an organic LED element having a transparent substrate, a light scattering layer, a first electrode, an organic light emitting layer, and a second electrode, (A) forming a light scattering layer on the transparent substrate,
- the light scattering layer has a base material made of glass and a plurality of scattering materials dispersed in the base material, and the light scattering layer has a bottom surface, an upper surface, and a side surface on the transparent substrate side.
- the side surface of the light scattering layer has a surface inclined at a gentler angle than a right angle from the top surface toward the bottom surface; (B) installing a transparent first electrode on the light scattering layer, The first electrode is disposed so as to continuously cover the side surface of the light scattering layer; and (C) installing an organic light emitting layer on the first electrode; (D) installing a second electrode on the organic light emitting layer; The manufacturing method of the organic LED element which has this. (12) The step (a) (A1) a step of placing a paste containing glass powder on a transparent substrate; and (a2) a step of firing the transparent substrate on which the paste is placed in a temperature range of the softening temperature of the glass powder ⁇ 30 ° C.
- An organic LED element comprising a transparent substrate, a light scattering layer, a first electrode, an organic light emitting layer, a second electrode, and a sealing substrate,
- the transparent substrate has a first region, a second region, and a third region on an upper surface, the second region is adjacent to the first region, and the first region is adjacent to the third region.
- the light scattering layer includes a base material made of glass and a plurality of scattering materials dispersed in the base material, and is disposed over the first region, the second region, and the third region on the transparent substrate.
- the first electrode is installed on the light scattering layer so as to extend to the first region and the second region
- the organic light emitting layer is disposed in the first region on the upper surface of the transparent substrate so as to be in contact with the first electrode and the light scattering layer
- the second electrode is disposed so as to extend to the first region and the third region so as to be in contact with at least a part of the organic light emitting layer and a part of the light scattering layer
- the organic LED element wherein the sealing substrate is disposed in the first region so as to cover a portion of the second electrode disposed in the first region.
- FIG. 5 is a schematic cross-sectional view along the line BB ′ of the organic LED element shown in FIG. 4.
- FIG. 5 is a schematic cross-sectional view of the organic LED element shown in FIG. 4 taken along the line CC ′. It is the flowchart which showed roughly an example of the manufacturing method of the organic LED element by this invention.
- 1 is a conceptual cross-sectional view of an organic LED element according to the present invention.
- FIG. 1 shows a simplified cross-sectional view of a conventional organic LED element.
- the conventional organic LED element 1 includes a transparent substrate 10, a light scattering layer 20, a transparent electrode (anode) 30, an organic light emitting layer 40, and a counter electrode (cathode) 50 in this order. It is configured by stacking.
- the lower surface of the organic LED element 1 (that is, the exposed surface of the transparent substrate 10) is the light extraction surface 60.
- the organic light emitting layer 40 includes a plurality of layers such as an electron transport layer, an electron injection layer, a hole transport layer, and a hole injection layer in addition to the light emitting layer. The configuration of such an organic light emitting layer 40 is well known to those skilled in the art and will not be described further here.
- the light scattering layer 20 has a characteristic of scattering incident light in a plurality of directions.
- the light scattering layer 20 is configured by dispersing a scattering material (for example, bubbles, particles, etc.) having a refractive index different from that of a transparent material in a matrix of a transparent material such as resin.
- the particle size of the scattering material reaches a maximum of about 10 ⁇ m, and therefore the light scattering layer 20 has a thickness on the order of at least about 20 ⁇ m to 30 ⁇ m.
- the light scattering layer 20 can scatter incident light and reduce reflection of light at the interface with a layer adjacent to the light scattering layer 20. For this reason, the amount of light totally reflected in the organic LED element 1 is reduced. Therefore, in the organic LED element 1 having the configuration shown in FIG. 1, the amount of light emitted from the light extraction surface 60 can be improved as compared with the configuration without the light scattering layer 20.
- the light emitting area of the element is determined by the width L1 of the organic light emitting layer 40 in the X direction. Further, in order to increase the light emitting area of the element 1, the transparent electrode 30 covers the entire surface including the side surface 22 of the light scattering layer 20 so that the effective light emitting region of the organic light emitting layer 40 in the X direction is expanded. It is necessary to install the organic light emitting layer 40 so as to cover the entire transparent electrode 30.
- the light scattering layer 20 is composed of a relatively thick resin layer as described above, the entire light scattering layer 20 including the side surface 22 of the light scattering layer 20 is transparent with a thickness of only about 100 nm. It is extremely difficult to cover with a thin film such as the electrode 30. For example, in a film forming method such as a general sputtering method, it is impossible to continuously install the transparent electrode 30 on the side surface 22 of the light scattering layer 20.
- the resin has a characteristic that heat shrinkage is relatively likely to occur. Therefore, when the light scattering layer 20 is made of a resin, even if the entire light scattering layer 20 can be covered with the transparent electrode 30, the light scattering layer 20 is particularly at the time of thermal contraction of the light scattering layer 20. In the vicinity of the side surface 22, the possibility that peeling or cracking occurs in the transparent electrode 30 becomes extremely high. Further, when such peeling or cracking occurs in the transparent electrode 30, there is a problem that the organic LED element 1 cannot perform a proper light emitting operation.
- the conventional organic LED element 1 has a configuration in which it is difficult to increase the light emitting area of the element.
- the light scattering layer has a base material made of glass, and a plurality of scattering materials dispersed in the base material,
- the light scattering layer has a bottom surface on the transparent substrate side, a top surface on the first electrode side, and a side surface, and the side surface of the light scattering layer is directed from the top surface to the bottom surface, Having a surface inclined at a gentler angle than a right angle;
- the first electrode is provided so as to continuously cover the side surface of the light scattering layer.
- An organic LED element is provided.
- the side surface of the light scattering layer has a gentle inclination, even if the first electrode is a thin film, a continuous film is formed on the side surface of the light scattering layer by the first electrode. Can be formed. Therefore, in the organic LED element according to the present invention, the light emitting area of the organic LED element can be significantly increased.
- that the side surface of the light scattering layer has a gentle slope means that the maximum value of the inner angle formed by the tangent and the bottom surface at each part of the side surface of the light scattering layer is less than 90 °.
- the interior angle means an angle formed on the light scattering layer side among the angles formed by the tangent and the bottom surface.
- FIG. 2 schematically shows an example of a top view of the organic LED element according to the present invention.
- FIG. 3 schematically shows an AA ′ cross section of the organic LED element according to the present invention shown in FIG.
- the organic LED element 100 includes a transparent substrate 110, a light scattering layer 120, a first electrode (anode) 130, an organic light emitting layer 140, and a second electrode. (Cathode) 150 is laminated in this order.
- the first electrode 130 has an exposed portion extending in a horizontal direction (X direction) from a part of one side, and this exposed portion constitutes the first electrode terminal 170.
- the second electrode 150 has a portion extending in the horizontal direction (X direction) from a part of one side, and this portion constitutes the second electrode terminal 180.
- the light scattering layer 120 includes a glass base material 121 having a first refractive index, and a plurality of scattering materials 124 having a second refractive index different from the base material 121 and dispersed in the base material 121. It consists of.
- the thickness of the light scattering layer 120 is, for example, in the range of 5 ⁇ m to 50 ⁇ m. The thickness of the light scattering layer 120 means the thickness of the thickest part in the light scattering layer.
- the first electrode 130 is made of a transparent metal oxide thin film such as ITO (Indium Tin Oxide), and has a thickness of about 50 nm to 1.0 ⁇ m.
- the second electrode 150 is made of a metal such as aluminum or silver.
- the light scattering layer 120 has a side surface 122.
- the side surface 122 is not a surface substantially parallel to the Z direction, but has a surface shape gently inclined along the X direction.
- the entire side surface 122 of the light scattering layer 120 can be covered with the first electrode 130. Therefore, the light scattering layer 120 can be entirely covered with the first electrode 130 except the bottom surface.
- the first electrode 130 is entirely covered with the organic light emitting layer 140 except for the bottom surface and the first electrode terminal 170.
- Each exposed portion except the end face of the organic light emitting layer 140 is covered with the second electrode 150.
- the width in the X direction contributing to light emission (that is, the width of the first electrode 130 covered with the organic light emitting layer 140) is L2, which is shown in FIG.
- the light emitting area can be significantly improved.
- the side surface 122 of the light scattering layer 120 can be covered with the first electrode 130. Therefore, in the present invention, it is possible to avoid or suppress the problem that the light scattering layer 120 is eroded from the side surface 122 side by the etching agent in the step of patterning the first electrode 130.
- indium and bismuth can be recovered by the following procedure.
- the entire organic LED element 100 is immersed in a solvent such as an organic solvent.
- a solvent such as an organic solvent.
- the organic layer 140 is dissolved, and the second electrode 150 is peeled off from the transparent substrate 110 along with this.
- the light scattering layer 120 is entirely covered with the first electrode 130, including the side surface 122, it does not change during this process.
- the light scattering layer 120 is also dissolved at the same time. Thereafter, indium and bismuth can be recovered through substitution deposition and electrolytic scouring.
- FIG. 4 schematically shows an example of a top view of another organic LED element according to the present invention.
- FIG. 5 schematically shows a BB ′ cross section of the organic LED element shown in FIG.
- FIG. 6 schematically shows a CC ′ cross section of the organic LED element shown in FIG.
- the organic LED element 200 has substantially the same configuration as the organic LED element 100 described above. Accordingly, in FIGS. 4 to 6, the same members as those in FIGS. 2 and 3 are denoted by the same reference numerals as those in FIGS.
- the structure of the two electrode terminals is different from that of the organic LED element 100 described above.
- the organic LED element 200 has a first electrode terminal 270.
- the first electrode terminal 270 has a barrier layer 220 and a conductive layer disposed on the barrier layer 220 as shown in FIG. Layer 230.
- the organic LED element 200 has a second electrode terminal 280.
- the second electrode terminal 280 has a barrier layer 240 and a conductive layer disposed on the barrier layer 240 as shown in FIG. Layer 250.
- the conductive layer 230 of the first electrode terminal 270 is electrically connected to the first electrode 130.
- the conductive layer 230 is configured by an extended portion of the first electrode 130.
- the barrier layer 220 may be the same layer as the light scattering layer 120.
- the conductive layer 250 of the second electrode terminal 280 is electrically connected to the second electrode 150.
- the conductive layer 250 is electrically connected to the second electrode 150 at the position P.
- the conductive layer 250 may be formed using the same material as the first electrode 130.
- the barrier layer 240 may be made of the same material as the light scattering layer 120.
- the barrier layer 220 and the barrier layer 240 have a role of suppressing migration of so-called alkali metal ions that may occur during operation of the organic LED element.
- the migration of alkali metal ions refers to, for example, the first electrode 130 and the second electrode via the first and second electrode terminals 170 and 180 in the organic LED element 100 shown in FIGS.
- This refers to a phenomenon in which alkali metal ions contained in the transparent substrate 110 move toward the first and second electrode terminals 170 and 180 when energization is performed between the electrodes 150.
- an alkali metal salt precipitates at the interface between the transparent substrate 110 and the electrode terminals 170 and 180, thereby causing the electrode terminals 170 and 180 to deteriorate or break. There is a case.
- the first electrode terminal 270 since the first electrode terminal 270 has the barrier layer 220 between the conductive layer 230 and the transparent substrate 110, the migration phenomenon of alkali metal ions as described above is suppressed.
- the second electrode terminal 280 since the second electrode terminal 280 includes the barrier layer 240 between the conductive layer 250 and the transparent substrate 110, the migration phenomenon of alkali metal ions as described above is suppressed.
- the organic LED element 200 can maintain stable light emission characteristics over a long period of time.
- FIG. 8 schematically shows a cross section of another organic LED element 300 according to the present invention.
- members similar to those in FIGS. 2 to 5 are given the same reference numerals.
- the organic LED element 300 includes a transparent substrate 110, a light scattering layer 310, a first electrode (anode) 130, an organic light emitting layer 140, a second electrode (cathode) 150, A sealing substrate 320, a resin seal 330, and a connection wiring 340 are provided.
- the transparent substrate 110 of the organic LED element 300 has an upper surface having a first region 350A, a second region 350B, and a third region 350C.
- the first region 350 ⁇ / b> A is located in a region above the transparent substrate 110 where the organic light emitting layer 140 is installed.
- the second region 350B is located in the region where the organic light emitting layer 140 and the second electrode 150 are not provided and at least a part of the first electrode 130 is provided above the transparent substrate 110.
- the third region 350C is located in a region where the organic light emitting layer 140 and the first electrode 130 are not installed, and at least a part of the second electrode 150 is installed, above the transparent substrate 110. .
- the light scattering layer 310 is formed on the upper surface of the transparent substrate 110 over the entire first region to third region.
- the first electrode 130 is disposed on the light scattering layer 310 so as to extend to the first region (light emitting region) 350A and the second region 350B.
- the organic light emitting layer 140 is disposed in the first region 350A on the transparent substrate 110 so as to be in contact with the first electrode 130 and the light scattering layer 310.
- the second electrode 150 is disposed so as to extend in the first region 350A and the third region 350C so as to be in contact with a part of the organic light emitting layer 140 and a part of the light scattering layer 310.
- the sealing substrate 320 is installed in the first region 350A through the resin seal 330 so as to surround a portion of the second electrode 150 installed in the first region 350A.
- connection wiring 340 is formed on the third region 350B so as to be electrically connected to the first electrode 130.
- Such a configuration of the organic LED element 300 includes the light scattering layer 310 extending over a wide range of the first region to the third region, so that the light extraction efficiency can be expected to be greatly improved.
- the transparent substrate 110 is made of a material having a high transmittance for visible light.
- the transparent substrate 110 may be a glass substrate or a plastic substrate, for example.
- the material of the glass substrate includes inorganic glass such as alkali glass, non-alkali glass or quartz glass.
- the plastic substrate material include polyester, polycarbonate, polyether, polysulfone, polyethersulfone, polyvinyl alcohol, and fluorine-containing polymers such as polyvinylidene fluoride and polyvinyl fluoride.
- the thickness of the transparent substrate 110 is not particularly limited, but may be in the range of 0.1 mm to 2.0 mm, for example. Considering strength and weight, the thickness of the transparent substrate 110 is preferably 0.5 mm to 1.4 mm.
- the light scattering layer 120 includes a base material 121 and a plurality of scattering materials 124 dispersed in the base material 121.
- the base material 121 has a first refractive index
- the scattering material 124 has a second refractive index different from that of the base material.
- the content of the scattering material 124 in the light scattering layer 120 is preferably 1 vol% or more.
- the amount of the scattering material 124 in the light scattering layer 120 is preferably small from the inside to the outside of the light scattering layer 120. In this case, highly efficient light extraction can be realized.
- the base material 121 is made of glass, and as the material of the glass, inorganic glass such as soda lime glass, borosilicate glass, alkali-free glass, and quartz glass is used.
- inorganic glass such as soda lime glass, borosilicate glass, alkali-free glass, and quartz glass is used.
- the scattering material 124 includes, for example, bubbles, precipitated crystals (such as precipitated crystals of glass constituting the base material), material particles different from the base material, phase separation glass, and the like.
- a phase-separated glass refers to a glass composed of two or more types of glass phases.
- the scattering material 124 is preferably a precipitated crystal of glass constituting bubbles and / or a base material.
- the difference between the refractive index of the base material 121 and the refractive index of the scattering material 124 should be large.
- one or more components of P 2 O 5 , SiO 2 , B 2 O 3 , GeO 2 , and TeO 2 are selected as the network former.
- high refractive index components TiO 2 , Nb 2 O 5 , WO 3 , Bi 2 O 3 , La 2 O 3 , Gd 2 O 3 , Y 2 O 3 , ZrO 2 , ZnO, BaO, PbO, and Sb 2
- alkali oxides, alkaline earth oxides, fluorides, and the like may be added within a range that does not affect the refractive index.
- examples of the glass system constituting the base material 121 include B 2 O 3 —ZnO—La 2 O 3 system, P 2 O 5 —B 2 O 3 —R ′ 2 O—R ′′ O—TiO 2 — Nb 2 O 5 —WO 3 —Bi 2 O 3 system, TeO 2 —ZnO system, B 2 O 3 —Bi 2 O 3 system, SiO 2 —Bi 2 O 3 system, SiO 2 —ZnO system, B 2 O 3 -ZnO-based, P 2 O 5 -ZnO-based, etc.
- R ′ represents an alkali metal element
- R ′′ represents an alkaline-earth metal element.
- the above material system is only an example, and if it is the structure which satisfy
- the refractive index of the base material 121 is preferably equal to or higher than the refractive index of the first electrode 130. This is because when the refractive index of the base material 121 is lower than the refractive index of the first electrode 130, there is a possibility that a loss due to total reflection may occur at the interface between the light scattering layer 120 and the first electrode 130.
- the color of light emission can be changed by adding a colorant to the base material 121.
- a colorant for example, transition metal oxides, rare earth metal oxides, metal colloids, and the like can be used alone or in combination.
- a fluorescent material can be used for the base material 121 or the scattering material 124.
- the emission color of the organic LED element can be reduced, and the emitted light is scattered and emitted, so that the angle dependency of the color and / or the color change with time can be suppressed. it can.
- Such a configuration is suitable for backlight and lighting applications that require white light emission.
- the first electrode 130 is preferably 80% or more translucent in order to extract light generated in the organic light emitting layer 140 to the outside. In addition, since many holes are injected, it is preferable that the work function is high.
- Examples of the first electrode 130 include ITO, SnO 2 , ZnO, IZO (Indium Zinc Oxide), AZO (ZnO—Al 2 O 3 : zinc oxide doped with aluminum), and GZO (ZnO—Ga 2 O). 3 : zinc oxide doped with gallium), Nb-doped TiO 2 , and Ta-doped TiO 2 .
- the thickness of the first electrode 130 is preferably 50 nm (more preferably 100 nm) or more and 1.0 ⁇ m or less.
- the refractive index of the first electrode 130 is, for example, in the range of 1.9 to 2.2.
- the refractive index of the first electrode 130 can be reduced by increasing the carrier concentration.
- Commercially available ITO contains 10 wt% SnO 2 as standard, but the refractive index of ITO can be lowered by further increasing the Sn concentration.
- the carrier concentration increases, but the mobility and transmittance decrease. Therefore, it is necessary to determine the Sn amount in consideration of the overall balance.
- the refractive index of the first electrode 130 is preferably determined in consideration of the refractive index of the base material 121 constituting the light scattering layer 120 and the refractive index of the second electrode 150. In consideration of waveguide calculation, the reflectance of the second electrode 150, and the like, the difference in refractive index between the first electrode 130 and the base material 121 is preferably 0.2 or less.
- the organic light emitting layer 140 is a layer having a light emitting function, and is generally composed of a hole injection layer, a hole transport layer, a light emitting layer, an electron transport layer, and an electron injection layer. However, it is obvious to those skilled in the art that the organic light emitting layer 140 does not necessarily have all of the other layers as long as it has a light emitting layer. In general, the refractive index of the organic light emitting layer 140 is in the range of 1.7 to 1.8.
- the hole injection layer preferably has a small difference in ionization potential in order to lower the hole injection barrier from the first electrode 130.
- the material of the hole injection layer a high molecular material or a low molecular material is used.
- polymer materials polyethylene dioxythiophene (PEDOT: PSS) doped with polystyrene sulfonic acid (PSS) is often used, and among low molecular materials, phthalocyanine-based copper phthalocyanine (CuPc) is widely used.
- the hole transport layer serves to transport holes injected from the hole injection layer to the light emitting layer.
- Examples of the hole transport layer include triphenylamine derivatives, N, N′-bis (1-naphthyl) -N, N′-diphenyl-1,1′-biphenyl-4,4′-diamine (NPD), N , N′-Diphenyl-N, N′-bis [N-phenyl-N- (2-naphthyl) -4′-aminobiphenyl-4-yl] -1,1′-biphenyl-4,4′-diamine ( NPTE), 1,1′-bis [(di-4-tolylamino) phenyl] cyclohexane (HTM2), and N, N′-diphenyl-N, N′-bis (3-methylphenyl) -1,1′- Diphenyl-4,4′-diamine (TPD) or the like is used.
- NPD triphenylamine derivatives
- the thickness of the hole transport layer is, for example, in the range of 10 nm to 150 nm.
- the light emitting layer has a role of providing a field where the injected electrons and holes are recombined.
- the organic light emitting material a low molecular weight or high molecular weight material is used.
- Examples of the light emitting layer include tris (8-quinolinolato) aluminum complex (Alq3), bis (8-hydroxy) quinaldine aluminum phenoxide (Alq′2OPh), bis (8-hydroxy) quinaldine aluminum-2,5- Dimethylphenoxide (BAlq), mono (2,2,6,6-tetramethyl-3,5-heptanedionate) lithium complex (Liq), mono (8-quinolinolato) sodium complex (Naq), mono (2, 2,6,6-tetramethyl-3,5-heptanedionate) lithium complex, mono (2,2,6,6-tetramethyl-3,5-heptanedionate) sodium complex and bis (8-quinolinolate) Metal complexes of quinoline derivatives such as calcium complexes (Caq2), tetraphenylbutadiene, phenyl Nakudorin (QD), anthracene, perylene, as well as fluorescent substance such as coronene.
- a quinolinolate complex may be used, and in particular, an aluminum complex having 8-quinolinol and a derivative thereof as a ligand may be used.
- the electron transport layer serves to transport electrons injected from the electrode.
- the electron transport layer include quinolinol aluminum complex (Alq3), oxadiazole derivatives (for example, 2,5-bis (1-naphthyl) -1,3,4-oxadiazole (END), and 2- ( 4-t-butylphenyl) -5- (4-biphenyl))-1,3,4-oxadiazole (PBD) etc.), triazole derivatives, bathophenanthroline derivatives, silole derivatives and the like.
- the electron injection layer is configured, for example, by providing a layer doped with an alkali metal such as lithium (Li) or cesium (Cs) at the interface with the second electrode 150.
- the second electrode 150 a metal having a small work function or an alloy thereof is used.
- the second electrode 150 may be, for example, an alkali metal, an alkaline earth metal, a metal belonging to Group 3 of the periodic table, or the like.
- aluminum (Al), magnesium (Mg), or an alloy thereof is used for the second electrode 150.
- a laminated electrode in which aluminum (Al) is deposited on a thin film of aluminum (Al), magnesium silver (MgAg), lithium fluoride (LiF), or lithium oxide (Li 2 O) may be used. good.
- a laminated film of calcium (Ca) or barium (Ba) and aluminum (Al) may be used.
- barrier layers 220 and 240 are not limited to this, but the same material as that of the light scattering layer 120 described above may be used.
- the thickness of the barrier layers 220 and 240 is, for example, in the range of 0.5 ⁇ m to 50 ⁇ m.
- FIG. 7 shows a schematic flow chart when manufacturing the organic LED element according to the present invention.
- a step of forming a light scattering layer on a transparent substrate (step S110), and a transparent first electrode is installed on the light scattering layer.
- Step S120 installing an organic light emitting layer on the first electrode
- Step S140 installing a second electrode on the organic light emitting layer
- a transparent substrate is prepared. As described above, a glass substrate or a plastic substrate is usually used as the transparent substrate.
- a light scattering layer in which scattering materials are dispersed in a glass base material is formed on the transparent substrate.
- the method for forming the light scattering layer is not particularly limited, but here, a method for forming the light scattering layer by the “frit paste method” will be particularly described. However, it will be apparent to those skilled in the art that the light scattering layer may be formed by other methods.
- frit paste method a paste containing a glass material called a frit paste is prepared (preparation process), this frit paste is applied to the surface of the substrate to be installed, patterned (pattern formation process), and the frit paste is then baked.
- This is a method of forming a desired glass film on the surface of the substrate to be installed by performing (firing process).
- a glass powder is comprised with the material which finally forms the base material of a light-scattering layer.
- the composition of the glass powder is not particularly limited as long as desired scattering characteristics can be obtained, and the glass powder can be frit pasted and fired.
- the composition of the glass powder is, for example, 20-30 mol% of P 2 O 5 , 3-14 mol% of B 2 O 3 , 10-20 mol% of Bi 2 O 3 , 3-15 mol% of TiO 2 , Nb 2 O 5 10 to 20 mol%, WO 3 to 5 to 15 mol%, the total amount of Li 2 O, Na 2 O and K 2 O is 10 to 20 mol%, and the total amount of the above components is 90 mol% or more. May be.
- the particle size of the glass powder is, for example, in the range of 1 ⁇ m to 100 ⁇ m.
- a predetermined amount of filler may be added to the glass powder.
- the filler for example, particles such as zircon, silica, or alumina are used, and the particle size is usually in the range of 0.1 ⁇ m to 20 ⁇ m.
- the resin examples include ethyl cellulose, nitrocellulose, acrylic resin, vinyl acetate, butyral resin, melamine resin, alkyd resin, and rosin resin.
- ethyl cellulose and nitrocellulose may be used. Note that the addition of butyral resin, melamine resin, alkyd resin, and rosin resin improves the strength of the frit paste coating film.
- the solvent has a role of dissolving the resin and adjusting the viscosity.
- the solvent include ether solvents (butyl carbitol (BC), butyl carbitol acetate (BCA), diethylene glycol di-n-butyl ether, dipropylene glycol butyl ether, tripropylene glycol butyl ether, butyl cellosolve), alcohol solvents ( ⁇ -terpineol, pine oil, dawanol), ester solvent (2,2,4-trimethyl-1,3-pentanediol monoisobutyrate), phthalate ester solvent (DBP (dibutyl phthalate), DMP (dimethyl phthalate) ), DOP (dioctyl phthalate)).
- BC butyl carbitol
- BCA butyl carbitol acetate
- diethylene glycol di-n-butyl ether dipropylene glycol butyl ether
- DBP dibutyl phthalate
- DMP dimethyl phthalate
- DOP dioctyl phthalate
- a surfactant may be added to the frit paste to adjust the viscosity and promote frit dispersion.
- you may use a silane coupling agent for surface modification.
- these raw materials are mixed to prepare a frit paste in which glass raw materials are uniformly dispersed.
- the frit paste prepared by the above-described method is applied on a transparent substrate and patterned.
- the application method and the patterning method are not particularly limited.
- a frit paste may be pattern-printed on a transparent substrate using a screen printer.
- a doctor blade printing method or a die coat printing method may be used.
- the frit paste film is baked. Usually, firing is performed in two steps. In the first step, the resin in the frit paste film is decomposed and lost, and in the second step, the glass powder is sintered and softened.
- the first step is performed by maintaining the frit paste film in a temperature range of 200 ° C. to 400 ° C. in an air atmosphere.
- the processing temperature varies depending on the resin material contained in the frit paste.
- the treatment temperature may be about 350 ° C. to 470 ° C.
- the resin is nitrocellulose
- the treatment temperature may be about 200 ° C. to 300 ° C.
- the processing time is usually about 30 minutes to 10 hours.
- the second step is performed by maintaining the frit paste film in the temperature range of the softening temperature ⁇ 30 ° C. of the contained glass powder in an air atmosphere.
- the processing temperature is, for example, in the range of 450 ° C. to 600 ° C.
- the processing time is not particularly limited, but is, for example, 30 minutes to 1 hour.
- the glass powder is sintered and softened to form a base material for the light scattering layer. Further, the scattering material uniformly dispersed in the base material can be obtained by the bubbles present in the frit paste film.
- a light scattering layer having a surface whose side surface portion is inclined at a gentler angle than a right angle from the upper surface toward the bottom surface is formed.
- the thickness of the finally obtained light scattering layer may be in the range of 5 ⁇ m to 50 ⁇ m.
- a transparent first electrode (anode) is placed on the light scattering layer obtained in the above step.
- the first electrode is formed so as to continuously cover the side surface of the light scattering layer in addition to the upper portion of the light scattering layer.
- the side surface of the light scattering layer has a surface inclined at a gentler angle than a right angle from the upper surface toward the bottom surface. Therefore, even if the thickness of the first electrode is thin, the continuous layer of the first electrode can be easily installed on the side surface of the light scattering layer.
- the method for installing the first electrode is not particularly limited, and for example, a film forming method such as a sputtering method, a vapor deposition method, and a vapor phase film forming method may be used. Further, the first electrode may be patterned.
- the material of the first electrode may be ITO or the like.
- the thickness of the first electrode is not particularly limited, and the thickness of the first electrode may be, for example, in the range of 50 nm to 1.0 ⁇ m.
- the laminate having the transparent substrate, the light scattering layer, and the first electrode obtained in the steps so far is referred to as a “translucent substrate”.
- the specification of the organic light emitting layer to be installed in the next process varies depending on the application application of the finally obtained organic LED element. Therefore, conventionally, the “translucent substrate” is often distributed in the market as an intermediate product in this state, and the subsequent steps are often omitted.
- Step S130 When manufacturing an organic LED element, next, an organic light emitting layer is installed so that a 1st electrode may be covered.
- the installation method of the organic light emitting layer is not particularly limited, and for example, a vapor deposition method and / or a coating method may be used.
- Step S140 a second electrode is placed on the organic light emitting layer.
- the method for installing the second electrode is not particularly limited, and for example, a vapor deposition method, a sputtering method, a vapor deposition method, or the like may be used.
- the organic LED element 100 as shown in FIGS. 2 and 3 is manufactured. It is obvious to those skilled in the art that the organic LED element 200 as shown in FIGS. 4 to 6 can be manufactured by the same method.
- a substrate was prepared by forming a silica film of 40 nm on a soda lime substrate having a thickness of 0.55 mm and 50 mm ⁇ by sputtering.
- a scattering layer glass material is prepared. Glasses shown in Table 1 were prepared and dissolved as the glass material for the scattering layer. Melting was performed at 1050 ° C., and then allowed to stand at 950 ° C. for 30 minutes, and then cast into twin rolls to obtain flakes.
- the glass had a glass transition temperature of 475 ° C. and a thermal expansion coefficient of 72 ⁇ 10 ⁇ 7 (1 / ° C.).
- the refractive index nd at the d line (587.56 nm) was 1.98.
- the glass transition point was measured by a thermal analysis method (manufactured by Bruker, trade name: TD5000SA) by a thermal expansion method at a heating rate of 5 ° C./min.
- the refractive index was measured with a refractometer (trade name: KRP-2, manufactured by Kalnew Optical Industry Co., Ltd.).
- the above-mentioned flakes were dry-ground for 2 hours with a planetary ball mill made of zirconia to produce a glass powder having an average particle size (d50, particle size of 50% integrated value, unit ⁇ m) of 1 to 3 ⁇ m. Then, 75 g of the obtained glass powder was kneaded with 25 g of an organic vehicle (about 10% by mass of ethyl cellulose dissolved in ⁇ -terpineol or the like) to prepare a paste ink (glass paste). This glass paste was printed using a screen printer to form a square pattern. After screen printing, drying was performed at 120 ° C. for 10 minutes, and then printing and drying were repeated. The substrate is heated to 450 ° C.
- a glass layer (scattering layer) 902 was formed on a glass substrate 901.
- the film thickness of the scattering layer 902 was 42 ⁇ m.
- the total light transmittance and haze value of the scattering layer 902 formed on the glass substrate 901 were measured.
- Suga Test Instruments Haze Meter HGM-2 was used as a measuring device.
- the above-mentioned soda lime substrate was measured.
- the total light transmittance was 69%, and the haze value was 73%.
- the surface waviness was measured using SURFCOM 1400D manufactured by Tokyo Seimitsu.
- the average arithmetic roughness (Ra) was 0.95 ⁇ m.
- an ITO layer 1001 having a film thickness of 150 nm was formed by DC pulse sputtering with an input power of 300 W using an ITO target. Thereafter, the substrate heater was turned off, the sputtering apparatus was opened to the atmosphere, and the glass substrate with the scattering layer after film formation was taken out.
- FIG. 11 is a top view showing the positional relationship between a glass substrate with a scattering layer on which an ITO pattern is formed, an organic layer, and a reflective electrode.
- reference numeral 1101 denotes an organic layer
- 1102 denotes a reflective electrode.
- the sealing substrate and this substrate were bonded together with a UV curable resin, bonded by UV irradiation to obtain an organic EL element.
- the AA ′ cross-sectional shape in FIG. 11 is the same as that shown in FIG.
- FIG. 12 is a photograph showing a state in which the scattering layer upper part 1201 and the scattering layer pattern edge part 1202 emit light.
- the device is formed with three regions of the scattering layer upper portion 1201, the scattering layer pattern edge portion 1202, and the glass substrate upper portion 1203. Good light emission is confirmed in any region. It can be seen that in the scattering layer upper part 1201, a large amount of light is extracted by the scattering layer, which is brighter than the glass substrate upper part 1203.
- the scattering layer edge 1202 is gentle, the coverage of ITO, organic film, LiF, and Al is good, and the ITO and Al electrodes are not short-circuited or disconnected. It was confirmed that the element on the glass substrate upper part 1203 can be lit with a pair of electrode patterns.
- the present invention can be applied to organic LED elements used for light-emitting devices and the like.
Abstract
Description
(1)透明基板と、該透明基板上に形成された光散乱層と、該光散乱層上に形成された透明な第1の電極と、該第1の電極上に形成された有機発光層と、該有機発光層上に形成された第2の電極とを有する有機LED素子であって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、
前記光散乱層は、前記透明基板の側にある底面、前記第1の電極の側にある上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有し、
前記第1の電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されていることを特徴とする有機LED素子。
(2)さらに、第1の電極端子および第2の電極端子を有し、
前記第1の電極端子は、前記透明基板上に設置された第1のバリア層と、該第1のバリア層上に設置され、前記第1の電極と電気的に接続された第1の導電層とで構成され、
前記第2の電極端子は、前記透明基板上に設置された第2のバリア層と、該第2のバリア層上に設置され、前記第2の電極と電気的に接続された第2の導電層とで構成されることを特徴とする(1)に記載の有機LED素子。
(3)前記第1のバリア層は、前記光散乱層で構成され、および/または
前記第2のバリア層は、前記光散乱層で構成されることを特徴とする(2)に記載の有機LED素子。
(4)前記第1の導電層は、前記第1の電極と同じ材料で構成され、および/または
前記第2の導電層は、前記第1の電極と同じ材料で構成されることを特徴とする(2)または(3)に記載の有機LED素子。
(5)前記散乱物質は、気泡および/または前記ベース材を構成するガラスの析出結晶であることを特徴とする(1)乃至(4)のいずれか一つに記載の有機LED素子。
(6)前記光散乱層中における前記散乱物質の含有率は、1vol%以上であることを特徴とする(1)乃至(5)のいずれか一つに記載の有機LED素子。
(7)前記第1の電極は、厚さが50nm~1.0μmの範囲であることを特徴とする(1)乃至(6)のいずれか一つに記載の有機LED素子。
(8)前記光散乱層は、厚さが5μm~50μmの範囲であることを特徴とする(1)乃至(7)のいずれか一つに記載の有機LED素子。
(9)透明基板と、該透明基板上に形成された光散乱層と、該光散乱層上に形成された透明電極と、を有する透光性基板であって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、
前記光散乱層は、前記透明基板の側にある底面、前記透明電極の側にある上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有し、
前記透明電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されていることを特徴とする透光性基板。
(10)前記散乱物質は、気泡および/または前記ベース材を構成するガラスの析出結晶であることを特徴とする(9)に記載の透光性基板。
(11)透明基板と、光散乱層と、第1の電極と、有機発光層と、第2の電極とを有する有機LED素子を製造する方法であって、
(a)透明基板上に光散乱層を形成するステップであって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、前記光散乱層は、前記透明基板の側にある底面、上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有するステップと、
(b)前記光散乱層上に、透明な第1の電極を設置するステップであって、
前記第1の電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されるステップと、
(c)前記第1の電極上に、有機発光層を設置するステップと、
(d)前記有機発光層上に、第2の電極を設置するステップと、
を有する有機LED素子の製造方法。
(12)前記ステップ(a)は、
(a1)透明基板上に、ガラス粉末を含むペーストを設置するステップ、および
(a2)前記ペーストが設置された前記透明基板を、前記ガラス粉末の軟化温度±30℃の温度範囲で焼成するステップであって、これにより前記ベース材と、該ベース材中に分散された複数の散乱物質が形成されるステップ
を有することを特徴とする(11)に記載の有機LED素子の製造方法。
(13)透明基板、光散乱層、第1の電極、有機発光層、第2の電極、および封止基板を備える有機LED素子であって、
前記透明基板は、上面に、第1領域、第2領域および第3領域を有し、前記第2領域は、前記第1領域と隣接し、該第1領域は、前記第3領域と隣接しており、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、前記透明基板上に、前記第1領域、第2領域および第3領域にわたって設置され、
前記第1の電極は、前記光散乱層上に、前記第1領域と前記第2領域に延在するように設置され、
前記有機発光層は、前記第1の電極および前記光散乱層と接するようにして、前記透明基板上面の前記第1領域内に設置され、
前記第2の電極は、前記有機発光層の少なくとも一部および前記光散乱層の一部と接するようにして、前記第1領域と前記第3領域に延在するように設置され、
前記封止基板は、前記第2の電極の前記第1領域に設置されている部分を覆うようにして、前記第1領域に設置されることを特徴とする有機LED素子。
透明基板と、該透明基板上に形成された光散乱層と、該光散乱層上に形成された透明な第1の電極と、該第1の電極上に形成された有機発光層と、該有機発光層上に形成された第2の電極とを有する有機LED素子であって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、
前記光散乱層は、前記透明基板の側にある底面、前記第1の電極の側にある上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有し、
前記第1の電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されていることを特徴とする有機LED素子が提供される。
ここで、光散乱層の側面が緩やかな斜面を有するとは、光散乱層側面の各部位における接線と底面とで形成される内角の最大値が90°未満であることを意味する。ここで、内角とは前記接線と底面とで形成される角度のうち、光散乱層の側に形成される角度を意味する。
以下、図2および図3を参照して、本発明の構成についてより詳しく説明する。
次に、図4~図6を参照して、本発明による有機LED素子の別の構成について説明する。
次に、図8を参照して、本発明による有機LED素子の別の構成について説明する。
透明基板110は、可視光に対する透過率が高い材料で構成される。透明基板110は、例えば、ガラス基板またはプラスチック基板であっても良い。
光散乱層120は、ベース材121と、該ベース材121中に分散された複数の散乱物質124とを有する。ベース材121は、第1の屈折率を有し、散乱物質124は、ベース材とは異なる第2の屈折率を有する。
光散乱層120中の散乱物質124の存在量は、光散乱層120の内部から外側に向かって小さくなっていることが好ましく、この場合、高効率の光取り出しを実現することができる。
第1の電極130には、有機発光層140で生じた光を外部に取り出すため、80%以上の透光性であることが好ましい。また、多くの正孔を注入するため、仕事関数が高いことが好ましい。
有機発光層140は、発光機能を有する層であり、通常の場合、ホール注入層と、ホール輸送層と、発光層と、電子輸送層と、電子注入層とにより構成される。ただし、有機発光層140は、発光層を有していれば、必ずしも他の層の全てを有する必要はないことは、当業者には明らかである。なお、通常の場合、有機発光層140の屈折率は、1.7~1.8の範囲である。
ホール輸送層は、前述のホール注入層から注入されたホールを発光層に輸送する役割をする。ホール輸送層には、例えば、トリフェニルアミン誘導体、N,N'-ビス(1-ナフチル)-N,N'-ジフェニル-1,1'-ビフェニル-4,4'-ジアミン(NPD)、N,N'-ジフェニル-N,N'-ビス[N-フェニル-N-(2-ナフチル)-4'-アミノビフェニル-4-イル] -1,1'-ビフェニル-4,4'-ジアミン(NPTE)、1,1'-ビス[(ジ-4-トリルアミノ)フェニル]シクロヘキサン(HTM2)、およびN,N'-ジフェニル-N,N'-ビス(3-メチルフェニル)-1,1'-ジフェニル-4,4'-ジアミン(TPD)などが用いられる。
発光層は、注入された電子とホールが再結合する場を提供する役割を有する。有機発光材料としては、低分子系または高分子系のものが使用される。
電子輸送層は、電極から注入された電子を輸送する役割をする。電子輸送層には、例えば、キノリノールアルミニウム錯体(Alq3)、オキサジアゾール誘導体(例えば、2,5-ビス(1-ナフチル)-1,3,4-オキサジアゾール(END)、および2-(4-t-ブチルフェニル) -5-(4-ビフェニル))-1,3,4-オキサジアゾール(PBD)など)、トリアゾール誘導体、バソフェナントロリン誘導体、およびシロール誘導体などが用いられる。
電子注入層は、例えば、第2の電極150との界面に、リチウム(Li)、セシウム(Cs)等のアルカリ金属をドープした層を設けることにより構成される。
第2の電極150には、仕事関数の小さな金属またはその合金が用いられる。第2の電極150は、例えば、アルカリ金属、アルカリ土類金属、および周期表第3属の金属などであっても良い。第2の電極150には、例えば、アルミニウム(Al)、マグネシウム(Mg)、またはこれらの合金などが用いられる。
バリア層220、240には、これに限られるものではないが、前述の光散乱層120と同様の材料を使用しても良い。
次に、図7を参照して、本発明による有機LED素子の製造方法の一例について説明する。図7には、本発明による有機LED素子を製造する際の概略的なフロー図を示す。
まず、透明基板が準備される。前述のように、通常、透明基板には、ガラス基板やプラスチック基板が用いられる。
まず、ガラス粉末、樹脂、および溶剤等を含むフリットペーストが調製される。
次に、前述の方法で調製したフリットペーストを、透明基板上に塗布し、パターン化する。塗布の方法およびパターン化の方法は、特に限られない。例えば、スクリーン印刷機を用いて、透明基板上にフリットペーストをパターン印刷しても良い。あるいは、ドクターブレード印刷法またはダイコート印刷法を利用しても良い。
次に、フリットペースト膜が焼成される。通常、焼成は、2段階のステップで行われる。第1のステップでは、フリットペースト膜中の樹脂が分解、消失され、第2のステップでは、ガラス粉末が焼結、軟化される。
次に、前記工程で得られた光散乱層上に、透明な第1の電極(陽極)が設置される。第1の電極は、光散乱層の上部の他、光散乱層の側面を連続的に覆うようにして形成される。前述のように、光散乱層の側面は、上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有する。従って、第1の電極の厚さが薄い場合であっても、光散乱層の側面に、第1の電極の連続層を容易に設置することができる。
有機LED素子を製造する場合は、次に、第1の電極を覆うように、有機発光層が設置される。有機発光層の設置方法は、特に限られず、例えば、蒸着法および/または塗布法を使用しても良い。
次に、有機発光層上に第2の電極が設置される。第2の電極の設置方法は、特に限られず、例えば、蒸着法、スパッタ法、気相成膜法等を使用しても良い。
厚さ0.55mm、50mm□のソーダライム基板にスパッタ法でシリカ膜を40nm成膜した基板を用意した。次いで散乱層用ガラス材料を用意する。散乱層用ガラス材料として表1に示すガラスを調合、溶解した。溶解は、1050℃で溶解し、その後950℃30分放置した後、双ロールにキャストしてフレークを得た。
バッチ式マグネトロンスパッタリング装置のそれぞれのカソードに、直径6インチのITOターゲットを設置した。次に、スパッタリング装置の基板ホルダーに、図9の散乱層付きガラス基板上に、図10に示すような1辺の長さが3cmとなる矩形のITOパターン1001が得られるように金属製マスクを設置した。スパッタリング装置を1×10-3Pa以下まで排気した後、基板加熱ヒーターを250℃に設定した。散乱層付きガラス基板が加熱されたところで、雰囲気ガスとして、アルゴンガス98sccmと酸素ガス2sccmを導入した。ここで、ITOターゲットを用い、投入電力300WのDCパルススパッタリングにより、膜厚150nmのITO層1001を形成した。その後、基板加熱ヒーターをOFFにし、スパッタリング装置を大気開放して、成膜を終えた散乱層付きガラス基板を取り出した。
上述の基板を用いて有機EL素子を作製した。まず、純水およびIPAを用いた超音波洗浄を行った後、酸素プラズマを照射して、表面を清浄化した。次に、真空蒸着装置を用いて、α-NPD(N,N’-diphenyl-N,N’-bis(l-naphthyl)-l,l’biphenyl-4,4’’diamine)を100nm、Alq3(tris8-hydroxyquinoline aluminum)を60nm、LiFを0.5nm、Alを80nmを連続成膜した。このとき、α-NPD、Alq3、LiF及びAlはマスクを用いて図11に示すようなパターンを得た。図11は、ITOパターンが形成された散乱層付きガラス基板と、有機層及び反射電極の位置関係を示す上面図である。図11中、1101は有機層を示し、1102は反射電極を示す。その後封止用基板と本基板をUV硬化樹脂で張り合わせ、UV照射を行い接着して、有機EL素子を得た。
図11のA-A’断面形状は、前述の図3に示すものと同様の形状となっている。
作製した有機ELパネルに5Vを印加して、発光状態を確認した。図12は、散乱層上部1201や散乱層パターンエッジ部1202が発光している状態を示す写真である。このように、素子は散乱層上部1201、散乱層パターンエッジ部1202、ガラス基板上部1203の3領域形成されているが、いずれの領域でも良好な発光が確認される。散乱層上部1201では、散乱層により光が多く取り出されており、ガラス基板上部1203と比較して、明るくなっていることが分かる。また散乱層エッジ部1202では、その形状がなだらかなため、ITO、有機膜、LiF、Alの被覆性が良く、ITOとAl電極の短絡や、これらの断線が発生せず、散乱層上部1201とガラス基板上部1203の素子を1対の電極パターンで点灯できることを確認した。
本出願は、2010年4月8日出願の日本特許出願2010-089596に基づくものであり、その内容はここに参照として取り込まれる。
10 透明基板
20 光散乱層
22 側面
30 透明電極(陽極)
40 有機発光層
50 対向電極(陰極)
60 光取り出し面
100 本発明による有機LED素子
110 透明基板
120 光散乱層
121 ベース材
122 側面
124 散乱物質
130 第1の電極(陽極)
140 有機発光層
150 第2の電極(陰極)
170 第1の電極端子
180 第2の電極端子
200 別の有機LED素子
220 バリア層
230 導電層
240 バリア層
250 導電層
270 第1の電極端子
280 第2の電極端子
300 別の有機LED素子
310 光散乱層
320 封止基板
330 樹脂シール
340 接続配線
350A、350B、350C 領域。
Claims (13)
- 透明基板と、該透明基板上に形成された光散乱層と、該光散乱層上に形成された透明な第1の電極と、該第1の電極上に形成された有機発光層と、該有機発光層上に形成された第2の電極とを有する有機LED素子であって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、
前記光散乱層は、前記透明基板の側にある底面、前記第1の電極の側にある上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有し、
前記第1の電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されていることを特徴とする有機LED素子。 - さらに、第1の電極端子および第2の電極端子を有し、
前記第1の電極端子は、前記透明基板上に設置された第1のバリア層と、該第1のバリア層上に設置され、前記第1の電極と電気的に接続された第1の導電層とで構成され、
前記第2の電極端子は、前記透明基板上に設置された第2のバリア層と、該第2のバリア層上に設置され、前記第2の電極と電気的に接続された第2の導電層とで構成されることを特徴とする請求項1に記載の有機LED素子。 - 前記第1のバリア層は、前記光散乱層で構成され、および/または
前記第2のバリア層は、前記光散乱層で構成されることを特徴とする請求項2に記載の有機LED素子。 - 前記第1の導電層は、前記第1の電極と同じ材料で構成され、および/または
前記第2の導電層は、前記第1の電極と同じ材料で構成されることを特徴とする請求項2または3に記載の有機LED素子。 - 前記散乱物質は、気泡および/または前記ベース材を構成するガラスの析出結晶であることを特徴とする請求項1乃至4のいずれか一つに記載の有機LED素子。
- 前記光散乱層中における前記散乱物質の含有率は、1vol%以上であることを特徴とする請求項1乃至5のいずれか一つに記載の有機LED素子。
- 前記第1の電極は、厚さが50nm~1.0μmの範囲であることを特徴とする請求項1乃至6のいずれか一つに記載の有機LED素子。
- 前記光散乱層は、厚さが5μm~50μmの範囲であることを特徴とする請求項1乃至7のいずれか一つに記載の有機LED素子。
- 透明基板と、該透明基板上に形成された光散乱層と、該光散乱層上に形成された透明電極と、を有する透光性基板であって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、
前記光散乱層は、前記透明基板の側にある底面、前記透明電極の側にある上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有し、
前記透明電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されていることを特徴とする透光性基板。 - 前記散乱物質は、気泡および/または前記ベース材を構成するガラスの析出結晶であることを特徴とする請求項9に記載の透光性基板。
- 透明基板と、光散乱層と、第1の電極と、有機発光層と、第2の電極とを有する有機LED素子を製造する方法であって、
(a)透明基板上に光散乱層を形成するステップであって、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、前記光散乱層は、前記透明基板の側にある底面、上面、および側面を有し、前記光散乱層の前記側面は、前記上面から前記底面に向かって、直角よりも緩やかな角度で傾斜した表面を有するステップと、
(b)前記光散乱層上に、透明な第1の電極を設置するステップであって、
前記第1の電極は、前記光散乱層の前記側面を連続的に覆うようにして設置されるステップと、
(c)前記第1の電極上に、有機発光層を設置するステップと、
(d)前記有機発光層上に、第2の電極を設置するステップと、
を有する有機LED素子の製造方法。 - 前記ステップ(a)は、
(a1)透明基板上に、ガラス粉末を含むペーストを設置するステップ、および
(a2)前記ペーストが設置された前記透明基板を、前記ガラス粉末の軟化温度±30℃の温度範囲で焼成するステップであって、これにより前記ベース材と、該ベース材中に分散された複数の散乱物質が形成されるステップ
を有することを特徴とする請求項11に記載の有機LED素子の製造方法。 - 透明基板、光散乱層、第1の電極、有機発光層、第2の電極、および封止基板を備える有機LED素子であって、
前記透明基板は、上面に、第1領域、第2領域および第3領域を有し、前記第2領域は、前記第1領域と隣接し、該第1領域は、前記第3領域と隣接しており、
前記光散乱層は、ガラスからなるベース材と、該ベース材中に分散された複数の散乱物質とを有し、前記透明基板上に、前記第1領域、第2領域および第3領域にわたって設置され、
前記第1の電極は、前記光散乱層上に、前記第1領域と前記第2領域に延在するように設置され、
前記有機発光層は、前記第1の電極および前記光散乱層と接するようにして、前記透明基板上面の前記第1領域内に設置され、
前記第2の電極は、前記有機発光層の少なくとも一部および前記光散乱層の一部と接するようにして、前記第1領域と前記第3領域に延在するように設置され、
前記封止基板は、前記第2の電極の前記第1領域に設置されている部分を覆うようにして、前記第1領域に設置されることを特徴とする有機LED素子。
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Also Published As
Publication number | Publication date |
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CN102845130A (zh) | 2012-12-26 |
TW201203649A (en) | 2012-01-16 |
EP2557896A4 (en) | 2016-07-27 |
US20130026461A1 (en) | 2013-01-31 |
JP5742838B2 (ja) | 2015-07-01 |
EP2557896B1 (en) | 2019-10-30 |
EP3608984B1 (en) | 2020-11-11 |
US20140353656A1 (en) | 2014-12-04 |
KR20130044227A (ko) | 2013-05-02 |
US8835960B2 (en) | 2014-09-16 |
CN102845130B (zh) | 2015-12-09 |
EP3608984A1 (en) | 2020-02-12 |
US9419248B2 (en) | 2016-08-16 |
JPWO2011126097A1 (ja) | 2013-07-11 |
EP2557896A1 (en) | 2013-02-13 |
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