Classifications

• • G—PHYSICS
  • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
  • G03G—ELECTROGRAPHY; ELECTROPHOTOGRAPHY; MAGNETOGRAPHY
  • G03G15/00—Apparatus for electrographic processes using a charge pattern
  • G03G15/04—Apparatus for electrographic processes using a charge pattern for exposing, i.e. imagewise exposure by optically projecting the original image on a photoconductive recording material
  • G03G15/04036—Details of illuminating systems, e.g. lamps, reflectors
  • G03G15/04045—Details of illuminating systems, e.g. lamps, reflectors for exposing image information provided otherwise than by directly projecting the original image onto the photoconductive recording material, e.g. digital copiers
• • G—PHYSICS
  • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
  • G03B—APPARATUS OR ARRANGEMENTS FOR TAKING PHOTOGRAPHS OR FOR PROJECTING OR VIEWING THEM; APPARATUS OR ARRANGEMENTS EMPLOYING ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ACCESSORIES THEREFOR
  • G03B17/00—Details of cameras or camera bodies; Accessories therefor
  • G03B17/18—Signals indicating condition of a camera member or suitability of light
• • G—PHYSICS
  • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
  • G03G—ELECTROGRAPHY; ELECTROPHOTOGRAPHY; MAGNETOGRAPHY
  • G03G15/00—Apparatus for electrographic processes using a charge pattern
  • G03G15/04—Apparatus for electrographic processes using a charge pattern for exposing, i.e. imagewise exposure by optically projecting the original image on a photoconductive recording material
  • G03G15/04036—Details of illuminating systems, e.g. lamps, reflectors
• • H—ELECTRICITY
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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K50/00—Organic light-emitting devices
  • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
  • H10K50/14—Carrier transporting layers
  • H10K50/15—Hole transporting layers
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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K50/00—Organic light-emitting devices
  • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
  • H10K50/14—Carrier transporting layers
  • H10K50/16—Electron transporting layers
• • 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
  • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
  • H10K50/17—Carrier injection layers
  • H10K50/171—Electron injection layers
• • 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
  • H10K50/818—Reflective anodes, e.g. ITO combined with thick metallic layers
• • 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
  • H10K50/858—Arrangements for extracting light from the devices comprising refractive means, e.g. lenses
• • H—ELECTRICITY
  • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
  • H10K59/80—Constructional details
  • H10K59/805—Electrodes
  • H10K59/8051—Anodes
  • H10K59/80518—Reflective anodes, e.g. ITO combined with thick metallic layers
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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
  • H10K59/80—Constructional details
  • H10K59/875—Arrangements for extracting light from the devices
  • H10K59/879—Arrangements for extracting light from the devices comprising refractive means, e.g. lenses
• • 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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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K2101/00—Properties of the organic materials covered by group H10K85/00
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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
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  • H10K2101/27—Combination of fluorescent and phosphorescent emission
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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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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K50/00—Organic light-emitting devices
  • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
  • H10K50/17—Carrier injection layers
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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
  • H10K85/60—Organic compounds having low molecular weight
  • H10K85/615—Polycyclic condensed aromatic hydrocarbons, e.g. anthracene
  • H10K85/622—Polycyclic condensed aromatic hydrocarbons, e.g. anthracene containing four rings, e.g. pyrene
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  • H10K85/60—Organic compounds having low molecular weight
  • H10K85/631—Amine compounds having at least two aryl rest on at least one amine-nitrogen atom, e.g. triphenylamine
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  • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
  • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
  • H10K85/60—Organic compounds having low molecular weight
  • H10K85/649—Aromatic compounds comprising a hetero atom
  • H10K85/657—Polycyclic condensed heteroaromatic hydrocarbons
  • H10K85/6572—Polycyclic condensed heteroaromatic hydrocarbons comprising only nitrogen in the heteroaromatic polycondensed ring system, e.g. phenanthroline or carbazole

Definitions

• the present invention relates to an organic compound
• electroluminescence (EL) element an electroluminescence (EL) element, and an image-forming apparatus, a display apparatus, and an imaging
• the organic EL element has excellent features such as surface emitting characteristics, a light weight, and visibility. Accordingly, the element has been used as a thin display, lighting equipment, or a head-mounted display in order that those excellent features may be exploited.
• an organic EL element constituting a pixel in an organic EL display apparatus is of a structure in which a pair of electrodes and a functionally separated organic compound layer each having a thickness of several tens of nanometers to several hundreds of nanometers are laminated.
• the thickness of each layer constituting the organic EL element is comparable to the wavelength of light and hence the organic EL element has the following property. Its emission efficiency largely changes owing to an
• an improvement in emission efficiency can reduce the power consumption of an apparatus using the organic EL element (such as a display) .
• the emission efficiency of the organic EL element is strongly affected by the optical interference, and hence the emission efficiency of the organic EL element largely fluctuates depending on the refractive index and thickness of the organic compound layer.
• no specific technology or approach for the optimization of the emission efficiency of the organic EL element through the utilization of the thickness and refractive index of the organic compound layer provided between the pair of electrodes has been established.
• the behavior of light in an organic EL element can be calculated by an optical simulation introduced in, for example, Non Patent Literature 1. Calculation methods for the reflectance, transmittance, phase shift, and the like of an optical multilayer thin film have also been known.
• Patent Literature 1 proposes, for example, the following approach for the purpose of improving the emission efficiency of an organic EL element.
• An organic compound layer is placed between a hole injection layer and a hole transport layer, the organic compound layer having a refractive index smaller than that of each adjacent layer.
• Patent Literature 2 discloses that when a hole
• transport layer constituting a blue-light-emitting element is of. a construction formed of two layers having different refractive indices, the emission efficiency of the element changes depending on a thickness ratio between the two hole transport layers.
• NPL 1 S. Nowy et . al., Journal of Applied Physics 104, 123109 (2008)
• he present invention has been accomplished to solve the problems and is directed to providing an organic EL element improved in emission efficiency.
• a reflective electrode includes: a reflective electrode; a light exiting side electrode; an emission layer provided between the reflective electrode and the light exiting side
• the reflective electrode and at least one low-refractive index layer provided between the reflective electrode and the emission layer, the low-refractive index layer having a refractive index lower than a refractive index of the emission layer, in which: an optical path Li between a maximum emission surface of the emission layer and a reflection surface of the reflective electrode
• ⁇ represents a maximum peak wavelength of an emission spectrum
• ⁇ represents a phase shift [deg] on the reflection surface of the reflective electrode
• m represents a positive integer
• an optical path L 2 between an interface on an emission layer side of the low-refractive index layer closest to the emission layer and the maximum emission surface of the emission layer satisfies the following expression (2 ) :
• FIG. 1 is a schematic sectional view illustrating a
• FIG. 2 is a view illustrating a phase shift when light entering a reflective electrode from an organic
• FIG. 3 is a view illustrating the wavelength dependence of the refractive index of each of an emission layer and an HTL1.
• FIG. 4 is a graph showing a relationship between: the refractive index and thickness of an HTL2; and emission efficiency .
• FIG. 5 is a graph showing a relationship between: the refractive index of the HTL1 and the thickness of the HTL2; and the emission efficiency.
• FIG. 6 is a schematic sectional view illustrating a second embodiment in the organic EL element of the present invention.
• FIG. 7 is a schematic sectional view illustrating a third embodiment in the organic EL element of the present invention.
• FIG. 8 is a schematic sectional view illustrating an example of an image-forming apparatus including the organic EL element of the present invention.
• FIG. 9 is a schematic sectional view illustrating an example of a display apparatus including the organic EL element of the present invention.
• FIG. 10 is a schematic sectional view illustrating an example of an imaging apparatus including the organic EL element of the present invention.
• An organic EL element of the present invention includes: a reflective electrode; a light exiting side electrode; an emission layer provided between the reflective electrode and the light exiting side
• the electrode and at least one low-refractive index layer provided between the reflective electrode and the emission layer, the low-refractive index layer having a refractive index lower than the refractive index of the emission layer.
• the low-refractive index layer having a refractive index lower than the refractive index of the emission layer.
• refractive index of the low-refractive index layer is lower than the refractive index of the emission layer by preferably 0.1 or more, more preferably 0.2 or more.
• the layer has a function as a charge injection/transport layer, but the number of low-refractive index layers to be provided between the emission layer and the
• the reflective electrode is not particularly limited.
• the low-refractive index layer to be provided between the emission layer and the reflective electrode may be one layer, or may be two or more layers.
• a high-refractive index layer having a refractive index equal to or higher than the refractive index of the emission layer may be disposed between the multiple low-refractive index layers so as to be in contact with the respective low- refractive index layers.
• the refractive index of the high-refractive index layer is higher than the
• each low-refractive index layer by preferably 0.1 or more, more preferably 0.2 or more.
• the low-refractive index layer closest to the emission layer relative to any other low-refractive index layer is defined as the low-refractive index layer closest to the emission layer.
• the low-refractive index layer is the low- refractive index layer closest to the emission layer.
• the low-refractive index layer is a layer provided between the emission layer and the reflective electrode, and hence has two interfaces, i.e., an interface on an emission layer side and an interface on a reflective electrode side.
• refractive index higher than that of the low-refractive index layer on the surface of the low-refractive index layer on the emission layer side and the surface thereof on the reflective electrode side are each sometimes referred to as "reflection interface".
• an optical path Li between the maximum emission surface of the emission layer and the reflection surface of the reflective electrode satisfies the following expression (1) . It is to be noted that the definition of the reflection surface of the reflective electrode is described later.
• ⁇ represents the maximum peak
• ⁇ a phase shift [deg] on the reflection surface of the reflective electrode
• m a positive integer.
• the optical path Li more preferably satisfies the following expression ( ⁇ ').
• the maximum emission surface of the emission layer means a. region having the highest emission intensity out of the emission layer.
• the maximum emission surface of the emission layer which is ideally a surface region having a thickness of zero, is typically a three-dimensional region having some degree of thickness.
• the thickness as used herein can be neglected upon consideration of, for example, the optical interference condition of the expression (1) . It is to be noted that the position of the
• maximum emission surface of the emission layer can be appropriately set depending on, for example, a charge balance in the emission layer.
• the thickness of a layer between the reflective electrode and the light exiting side electrode can be set to a thickness sufficient for the suppression of the occurrence of a short circuit or an emission point.
• an optical path L 2 between the interface on the emission layer side of the low-refractive index layer closest to the emission layer and the maximum emission surface of the emission layer satisfies the following expression (2), and p in the expression (2) equals 0.
• ⁇ represents the maximum peak wavelength of the emission spectrum and p represents 0 or a positive integer. It is to be noted that for the low-refractive index layer provided between the
• p in the expression (2) represents 0 or a positive integer.
• p in the expression (2) is determined based on the number of low-refractive index layers provided between the reflective electrode and the emission layer, and their placement positions.
• the optical path L 2 is an optical path between the interface on the emission layer side of the low-refractive index layer closest to the emission layer and the maximum emission surface of the emission layer
• p in the expression (2) equals 0.
• p for the low-refractive index layer closest to the emission layer out of the low-refractive index layers, p equals 0. Accordingly, a requirement concerning the L 2 for the low-refractive index layer closest to the emission layer can be represented by the following expression (2').
• the expression (2) may also hold in the optical path (L 2 ) between the interface on an emission layer side of the low-refractive index layer, which differs from the low-refractive index layer closest to the emission layer, and the maximum emission surface of the emission layer.
• p in the expression (2) represents an integer of 1 or more (p ⁇ l) .
• the optical path L 2 itself means an optical path between the interface on the emission layer side of at least one low-refractive index layer, which is provided between the emission layer and the reflective electrode, and the maximum emission surface of the emission layer. Accordingly, the expression (2) itself is never a requirement imposed only on the low-refractive index layer closest to the emission layer.
• the thickness of the low- refractive index layer is preferably more than 1/8 ⁇ and less than 3/8 ⁇ in terms of an optical path length.
• an organic EL element including a low-refractive index layer that is a layer having a refractive index lower than that of an emission layer.
• the inventors have found that the element has efficiency higher than the conventional one when the interference conditions of the expression (1) and the expression (2) are satisfied.
• an organic EL element according to an embodiment of the present invention is described with reference to the drawings. It is to be noted that a widely known technology or publicly known technology in the art is applicable to a portion that is neither particularly shown in the drawings nor particularly described in the following description.
• the embodiment to be described below is merely one embodiment of the present invention and the present invention is not limited to the embodiment.
• FIG. 1 is a schematic sectional view illustrating an organic EL element according to a first embodiment of the present invention.
• the organic EL element 1 of FIG. 1 is an electronic element obtained by laminating, on a substrate 10, a lower electrode 21, a first charge injection/transport layer 22, a second charge
• an optical adjustment layer 30 may be provided on the upper electrode 26 as illustrated in FIG. 1.
• electrode 21 functions as a reflective electrode.
• the organic EL element 1 of FIG. 1 is a top emission-type organic EL element in which light is extracted from a side opposite to the substrate 10. It should be appreciated that the present invention is not limited to the aspect, and a bottom emission type in which the upper electrode 26 is a reflective electrode and light is extracted from a substrate 10 side is also included in the present invention.
• Examples of the substrate 10 include various glass substrates and silicon substrates.
• a substrate having a drive circuit such as a thin-film transistor (TFT) , which is formed of a semiconductor such as poly-Si or amorphous silicon (a- Si), formed on a base material is used in some cases.
• TFT thin-film transistor
• the lower electrode 21 as a reflective electrode is an electrode layer mainly having a metal reflective film for the purpose of improving the emission efficiency of the organic EL element.
• a metal material constituting the metal reflective film is preferably a metal
• the lower electrode 21 may be one metal reflective film alone, or may be a laminate of the metal reflective film and a material having a large work function that also serves as a barrier layer for barriering the metal reflective film. In this case, a constituent material for the barrier layer is
• a transparent conductive layer made of an indium tin oxide, an indium zinc oxide, or the like, a metal material such as Ti, Mo, or W, or a metal oxide such as Mo0 3 .
• the reflection surface of the reflective electrode is an interface between the metal reflective film and an organic compound layer to be described later.
• reflective electrode is constituted of the metal
• the reflection surface of the reflective electrode is an interface between the metal reflective film and the barrier layer. In other words, the reflection surface of the
• reflective electrode can be defined as the interface of the metal reflective film on an emission layer side.
• the charge injection/transport layers (22, 23, and 25) provided between the electrodes (the lower electrode 21 and the upper electrode 26) and the emission layer 24 are classified into two kinds, i.e., a hole
• the hole injection/transport layer is a concept comprehending a hole injection layer, a hole transport layer, an
• the electron injection/transport layer is a concept comprehending an electron injection layer, an electron transport layer, a hole-blocking layer, and the like, and it should be appreciated that a laminate obtained by laminating multiple electron injection layers, multiple electron transport layers, or multiple hole-blocking layers is also included in the concept.
• the lower electrode 21 and upper electrode 26 in the organic EL element 1 of FIG. 1 are an anode and a cathode, respectively, the first charge
• the third charge injection/transport layer 25 provided between the emission layer 24 and the upper electrode 26 is an electron injection/transport layer.
• injection/transport layer 23 (hole injection/transport layer) in the organic EL element 1 of FIG. 1 has a refractive index lower than that of the adjacent layers (the first charge injection/transport layer 22 and the emission layer 24) and hence functions as a low- refractive index layer.
• the second charge injection/transport layer 23 functions as a low- refractive index layer and hence the first charge injection/transport layer 22 functions as a charge injection/transport layer having a refractive index higher than that of the low-refractive index layer. It is to be noted that a function of the low-refractive index layer is described later.
• injection/transport layer are not particularly limited, and a publicly known charge injection material or charge transport material can be used.
• a light-emitting material as a constituent material for the emission layer 24 may be a fluorescent material or may be a phosphorescent material.
• the luminescent color of the emission layer 24 is not particularly limited, and examples thereof include a red color, a green color, and a blue color.
• the emission layer 24 depends on the luminescent color of the emission layer 24, i.e., the wavelength bandwidth of light output from the emission layer 24.
• the wavelength bandwidth of the light output from the emission layer 24 is around 460 nm as a . blue wavelength bandwidth
• the refractive index of the emission layer 24 is about 1.8 to 1.9.
• the wavelength bandwidth of the light output from the emission layer 24 is around 600 nm as a red wavelength bandwidth
• the refractive index of the emission layer 24 is about 1.7 to 1.8.
• the upper electrode 26 as a light exiting side
• the electrode functions as a light transmissive electrode.
• the light transmissive electrode is specifically, for example, a transparent conductive layer formed of a transparent conductive material or a semi-transmissive metal film obtained by forming a metal material into a film having a predetermined thickness.
• a constituent material for the upper electrode 26 is, for example, a transparent electrode material such as an indium zinc oxide or an indium tin oxide.
• a transparent electrode material such as an indium zinc oxide or an indium tin oxide.
• the upper electrode 26 is a semi-transmissive metal film, examples of the
• constituent material for the upper electrode 26 include a metal material such as Ag or Mg, and an alloy
• the thickness of the upper electrode 26 is preferably 10 nm or more and 40 nm or less from the viewpoints of its film characteristics and light transmission property.
• an electron injection layer containing an alkali metal is preferably provided between the third charge injection/transport layer 25 (electron
• an alkali metal is preferably added into the upper electrode 26.
• the optical adjustment layer 30 provided on the upper electrode 26 is provided for the purpose of protecting the upper electrode 26. It is to be noted that when the thickness of the optical adjustment layer 30 corresponds to 650 nm or less as the wavelength range of visible light, the optical adjustment layer 30 becomes a member that may be involved in optical interference, and hence the layer affects a reflectance in a direction from the emission layer 24 to the upper electrode 26.
• the optical adjustment layer 30, which is preferably formed of a material having a high refractive index from the viewpoint of the adjustment of the reflectance, may be formed of an organic material or may be formed of an inorganic material as long as a requirement for the refractive index is satisfied.
• an intervening layer may be provided between the emission layer 24 and the second charge injection/transport layer 23 (low- refractive index layer) .
• the layer is desirably provided after its thickness has been
• the refractive index of the intervening layer is equal to or more than the refractive index of the intervening layer
• optical interference condition required of the organic EL element of FIG. 1 is described. It is to be noted that the optical interference condition required in the present invention is an optical interference condition resulting from a member formed between the emission layer 24 and the lower electrode 21.
• the intensity in a front direction of light having a wavelength ⁇ which one wishes to extract can be strengthened when the optical path Li from a maximum emission surface 24a of the emission layer 24 to the surface (reflective metal film surface) of the lower electrode 21 satisfies the following expression ( I ) .
• ⁇ represents a phase shift [deg] at the time of reflection and its sign is negative in a phase delay direction.
• m represents a constant called the order of interference.
• the optical path Li takes the positive minimum (- ⁇ /720) satisfying the expression (I).
• the refractive index of a layer positioned on the surface of the metal species is generally about -100° to -160°.
• FIG. 2 is a graph showing a phase shift when light
• FIG. 2 is also a graph showing the dependence of a phase shift on the wavelength of the light entering the reflective electrode.
• the optical path Li in the expression (I) is determined by summing the product of the refractive index (n) and thickness (d) of each layer provided between the maximum emission surface 24a of the
• laminated can be determined by general calculation for . an optical multilayer thin film.
• the optical path does not necessarily need to be caused to strictly coincide with a thickness determined from the optical path Li determined through calculation with the
• the optical path may have an error of up to + ⁇ /8 from the optical path Li
• the optical path Li preferably satisfies the following expression (1') ⁇
• At least one low-refractive index layer having a refractive index at the maximum peak wavelength of the emission spectrum of light output from the emission layer 24 lower than that of the emission layer 24 by 0.1 or more is placed between the emission layer 24 and the lower electrode 21
• the second charge in ection/transport layer 23 is a layer (low- refractive index layer) having a refractive index lower than that of the emission layer 24 by 0.1 or more and the first charge injection/transport layer 22 is a layer having a refractive index higher than that of the second charge injection/transport layer 23 by 0.1 or more.
• a refractive index difference arises at each of an interface between the first charge
• injection/transport layers (an HTL1 on a reflective electrode side and an HTL2 on an emission layer side) are provided between an anode as a reflective electrode and an emission layer.
• HTL1 corresponds to the first charge injection/transport layer 22 of FIG. 1
• HTL2 corresponds to the second charge in ection/transport layer 23 of FIG. 1.
• the following description is also applicable to an organic EL element in which two electron
• injection/transport layers are provided between a cathode as a reflective electrode and an emission layer.
• Lower electrode 21 A reflective electrode formed of an Ag film
• each of the two interfaces of the HTL2 can be viewed as a reflection interface.
• a phase shift when light entering a layer having a low refractive index from a layer having a high refractive index is reflected at a reflection interface is 0. Therefore, a phase matching condition in the optical path L 2 between a reflection interface directed from the layer having a high refractive index to the layer having a low refractive index when viewed from the maximum emission surface of the emission layer, specifically, the interface of the HTL2 on the emission layer side and the maximum emission surface of the emission layer is as represented by the following expression ( II ) .
• the optical path L 2 is allowed to have an error of about ⁇ /8 from a theoretical value (thickness value determined from the expression (II) through calculation) as in the Li . Therefore, the optical path L 2 is required to satisfy the following expression ( 2 ) .
• the optical path L 2 preferably satisfies the following expression (2a) .
• expression (2) is substantially the expression (2') and the expression (2a) is substantially the expression
• a phase shift when light entering a layer having a high refractive index from a layer having a low refractive index is reflected at a reflection interface is 180°. Therefore, a suitable phase
• the optical path L 3 is allowed to have an error of about ⁇ /8 as in the Li and the L 2 . Therefore, the optical path L 3 preferably satisfies the following expression (3).
• the error range is preferably up to ⁇ /16 from the thickness value
• the optical path L 3 preferably satisfies the following numerical expression (3').
• the low-refractive index layer to be utilized upon determination of the optical path L 2 from the expression (2) and the low-refractive index layer to be utilized upon determination of the optical path L 3 from the expression (3) may be identical to or different from each other.
• an emission region in the emission layer localizes toward the hole injection/transport layer (HTL2) and the maximum emission surface of the emission layer is positioned at 2 nm from the interface of the emission layer on the reflective electrode side.
• reflection interface of the HTL2 (the reflection interface on the emission layer side or the reflection interface on the HTL1 side) is discussed based on those conditions .
• FIG. 3 is a graph showing the wavelength dependence of the refractive index of each of the emission layer and the HTLl. As shown in FIG. 3, the refractive index of each of the emission layer and the HTLl at a wavelength of 460 nm is about 1.85. It is to be noted that in the following simulation, the optimization of the optical path Li is performed in the case where m in the expression (1) represents 1 unless otherwise stated.
• the emission region in the emission layer is assumed to localize toward the hole injection/transport layer (HTL2) and the maximum emission surface in the emission layer is assumed to be positioned at 2 nm from the interface of the emission layer on the hole injection/transport layer (HTL2) side.
• the simulation was performed by the same approach as that of Non Patent Literature 1, and with regard to internal quantum efficiency, exciton
• FIG. 4 is a graph showing a relationship between: the refractive index and thickness of the HTL2 ; and the emission efficiency. It is to be noted that the graph of FIG. 4 was determined by a simulation. In addition, the case where a value indicated by the axis of
• abscissa in the graph of FIG. 4 is 0 states that the thickness of the HTL2 is 0 nm, which means that the HTL2 is absent as a constituent member for the organic EL element. That is, the case where the value
• 0 represents an aspect in which only the HTLl is provided between the reflective electrode (anode) and the emission layer.
• the refractive indices of 1.6 and 1.75 apply to the definition of the low-refractive index layer as used in the present invention.
• an effect occurring when the refractive index of the HTL2 is set to 1.6 is described.
• the value is always constant irrespective of the state of the HTL2.
• a range in terms of the thickness of the HTL2 obtained by dividing the numerical range by the refractive index (1.6) of the HTL2 is from 33.6 nm or more to 105.5 nm or less.
• the emission efficiency takes a local maximum when its thickness is in the vicinity of 60 nm.
• the efficiency is found to be higher than that in the case where the HTL2 is absent (the case where the thickness of the HTL2 is 0) .
• the emission efficiency improves according to the thickness of the HTL2. Then, the emission efficiency takes a second local maximum when the thickness of the HTL2 is 177 nm or more.
• the electrode is specified by the expression (1), and hence there is an upper limit for the sum of the thicknesses of the two kinds of hole transport layers (the HTL1 and the HTL2) positioned between the emission layer and the reflective electrode.
• the thickness of the HTL1 is 0 nm
• the only reflection interface that differs in refractive index from an adjacent layer by 0.1 or more in the two interfaces of the low-refractive index layer (HTL2) is the reflection interface on the emission layer side.
• the emission is specified by the expression (1), and hence there is an upper limit for the sum of the thicknesses of the two kinds of hole transport layers (the HTL1 and the HTL2) positioned between the emission layer and the reflective electrode.
• the thickness of the HTL1 is 0 nm
• the emission is specified by the expression (1), and hence there is
• interference of light at the reflection interface of the HTL2 on the emission layer side can be utilized.
• the refractive index of the HTL2 is in the following state: the refractive index is lower than that of each of the emission layer and the HTL1 by 0.1.
• reflection interface of the HTL2 on the HTL1 side is 57.5 nm or more and 172.5 nm or less under the
• a range in terms of the thickness of the HTL2 obtained by dividing the numerical range by the refractive index (1.75) of the HTL2 is from 30.8 nm or more to 96.4 nm or less. Meanwhile, as shown in FIG. 4, the emission efficiency takes a local maximum when the thickness of the HTL2 is in the vicinity of 50 nm. In addition, even in the range of from 30.8 nm or more to 96.4 nm or less, the efficiency is found to be higher than that in the case where the HTL2 is absent (the case where the thickness of the HTL2 is 0 nm) .
• the refractive index of the HTL2 is 1.95 is described below.
• the emission efficiency is lower than that in the case where the HTL2 is absent (the case where the thickness of the HTL2 is 0 nm) no matter how the thickness of the HTL2 is set.
• the foregoing results from a reduction in emission efficiency due to the fact that the reflection interface of the HTL2 needed for defining the optical path L 3 is not set at a proper position.
• interface needed for defining the optical path L 3 out of the two interfaces of the HTL2 is the interface of the HTL2 on the emission layer side. This is because the interface needed for defining the optical path L 3 is based on an interface (reflection interface) when light traveling from the emission layer to the
• reflective electrode travels from a low-refractive index medium to a high-refractive index medium.
• the optical path L 3 i.e., the optical path from the interface between the emission layer and the HTL2 to the maximum emission surface of the
• FIG. 5 is a graph showing a relationship between: the refractive index of the HTL1 and the thickness of the HTL2; and the emission efficiency. It is to be noted that the graph of FIG. 5 was determined by a simulation. In addition, the case where a value indicated by the axis of abscissa in the graph of FIG. 5 is 0 states that the thickness of the HTL2 is 0 nm, which means that the HTL2 is absent as a constituent member for the organic EL element. That is, the case where the value indicated by the axis of abscissa is 0 represents an aspect in which only the HTL1 is provided between the reflective electrode (anode) and the emission layer.
• HTL1 is 1.6
• the thickness of the HTL2 to 29 nm or less provides good emission efficiency.
• the graph shown in FIG. 5 also shows that the emission efficiency is improved by bringing the low-refractive index layer (HTL1) and the emission layer close to each other. This is because of the following reason: a phase shift at wide angles enlarges and hence energy from excitons to be distributed in a vertical direction becomes relatively large. In the case where the refractive index of the HTLl is 1.75 as well, the efficiency becomes highest when the thickness of the HTL2 is in the vicinity of 0 nm.
• the refractive index of the HTL1 is 1.6 or 1.75 and the thickness of the HTL2 is in the vicinity of 0 nm shows that the emission efficiency is low when the refractive index of the HTL1 is higher than that of the emission layer.
• a hole transport material (HTL) having a low refractive index is, for example, Compound 2 shown below.
• Compound 2 is a compound in which a tert-butyl group as a bulky functional group is introduced to a terminal of a triarylamine-based skeleton having hole transport property.
• a bulky tert-butyl group is introduced, the film density of a formed film reduces and hence the refractive index of the film itself can be reduced.
• the refractive index-reducing effect can be expected from, for example, the introduction of a long- chain alkyl group to the terminal or the introduction of a functional group containing fluorine thereto. It is to be noted that the method is applicable even when a charge injection/transport layer provided between the reflective electrode (the lower electrode 21) and the emission layer 24 is an electron injection/transport layer.
• the low-refractive index material may be an organic material or may be an inorganic material.
• a film obtained by mixing, into Compound 1 (hole transportable material) shown below, Compound 2 or lithium fluoride as the low-refractive index material is described as an example.
• the refractive index of Compound 1 at a wavelength of 460 nm is 1.90. However, the refractive index is quantitatively changed (reduced) by doping with the low-refractive index material (Compound 2 or LiF) as shown in Table 3 and Table 4. [0104]Table 3
• the charge inj ectable/transportable material with the low- refractive index material can quantitatively change the refractive index, and hence the refractive index of the charge injection/transport layer can be quantitatively reduced.
• the method for the doping with the low-refractive index material can be appropriately selected depending on a method of forming a layer of interest. Specifically, when the layer is formed by a dry film-forming method such as a vapor deposition method, the formation can be performed by an ordinary codeposition method. On the other hand, when the layer is formed by a wet film-forming method such as an application method, a solution obtained by mixing a constituent material for the layer at a predetermined ratio with a solvent has only to be formed into a film by the application method or the like.
• a fluorine-based -polymer such -as - - polytetrafluoroethylene .
• the layer formed of the fluorine-based polymer is formed by the wet film- forming method such as the application method and a low-refractive index film having a refractive index around 1.30 can be formed from the polymer. It is to be noted that a substantial lower limit for the
• refractive index of the low-refractive index layer may be about 1.3 because there may be no solid material having a refractive index lower than that of the fluorine-based polymer. It is to be noted that in the present invention, an upper limit for the refractive index of the low-refractive index layer is a value lower than the refractive index of the emission layer by 0.1. In addition, the thickness of the low- refractive index layer is an odd number multiple of 1/4 ⁇ in terms of an optical path length in order that both target values for the expression (2) and the expression (3) may be satisfied at both interfaces of the low-refractive index layer.
• the charge mobility of the low-refractive index layer is generally low and hence a target value for the thickness of the low-refractive index layer is most preferably 1/4 ⁇ that is thinnest in terms of an optical path length. It is to be noted that the target value is allowed to have an error of about ⁇ 1/8 ⁇ . Accordingly, the thickness of the low-refractive index layer is preferably more than 1/8 ⁇ and less than 3/8 ⁇ in terms of an optical path length. The thickness of the low-refractive index layer is more preferably 3/1 ⁇ or more and 5/16X or less in terms of an optical path length.
• FIG. 6 is a schematic sectional view illustrating a second embodiment in the organic EL element of the present invention.
• An organic EL element 2 of FIG. 6 is of the same construction as that of the organic EL element 1 of FIG. 1 with the exception that a fourth charge injection/transport layer 27 is further provided between the lower electrode 21 and the first charge injection/transport layer in the organic EL element 1 of FIG. 1.
• charge injection/transport layer 27 is a hole
• the layer is provided between the lower electrode 21, which serves as an anode and as a reflective electrode, and the emission layer 24.
• the following organic EL element was used: three kinds of hole injection/transport layers, i.e., the HTL1, the HTL2, and an HTL3 were placed between the anode as the reflective electrode and the emission layer so that the HTL1 was on a reflective electrode side and the HTL3 was on a
• the HTL1 corresponds to the fourth charge injection/transport layer 27 of FIG. 6, the HTL2 corresponds to the first charge
• the fourth charge injection/transport layer 27 (HTL1) is a layer in contact with the first charge injection/transport layer 22 (HTL2) on the reflective electrode side, and is a layer (low-refractive index layer) having a refractive index lower than those of the emission layer 24 and the first charge injection/transport layer 22 (HTL2) .
• the construction in this embodiment is such that two low-refractive index layers (the second charge injection/transport layer 23 (HTL3) and the fourth charge injection/transport layer 27 (HTL1) ) are provided between the emission layer 24 and the
• the following simulation is performed on the premise that the optical path Li in this embodiment satisfies the expression (1).
• an emission region present in the emission layer is assumed to localize toward the hole injection/transport layer (HTL3) , and the maximum emission surface in the
• emission layer is assumed to be positioned at 2 nm frdm an interface between the emission layer and the HTL3.
• the simulation was performed by the same approach as that of each of Non Patent Literature 1 and Non Patent Literature 2, and with regard to internal quantum efficiency, exciton production efficiency was set to 25% and an emission yield was set to 80%.
• the organic EL element used in the simulation is such that the refractive index of each of the HTL1 and the HTL3 is different from (a refractive index lower than) those of the HTL2 and the emission layer. Accordingly, two interfaces of the HTL3 (an interface on the
• reflection interface to satisfy the requirement of the present invention is ( 115-3.7 ) /n H TL3 where n H TL3
• each of the embodiment 2A and embodiment 2B in Table 6 the expression (2) or the expression (3) is satisfied at all three reflection interfaces shown in Table 5, and as can be seen from Table 6 above, each of the embodiments has efficiency higher than that of the conventional form.
• the emission layer/HTL3 interface and the HTL2/HTL1 interface satisfy the expression (2) shown in Table 5, but the HTL3/HTL2 interface does not satisfy the expression (3) shown in Table 5. Therefore, it is found that the embodiment 2C has efficiency higher than that of the conventional form, though the efficiency is not as high as that of the embodiment 2B similarly formed of two low-refractive index layers.
• FIG. 7 is a schematic sectional view illustrating a third embodiment in the organic EL element of the present invention.
• An organic EL element 3 of FIG. 7 is of the same construction as that of the organic EL element 1 of FIG. 1 with the exception that only the second charge in ection/transport layer 23 is provided between the lower electrode 21 and the emission layer 24 (the first charge in ection/transport layer 22 in FIG. -1-is -not provided " between the lower electrode 21 and the emission layer 24) in the organic EL element 1 of FIG . 1.
• the organic EL element of the present invention is applicable to a light-emitting apparatus.
• the light- emitting apparatus is applicable to various combinations
• the printer head has a construction in which the multiple organic EL elements of the present invention are arrayed in a substantially one- dimensional direction.
• FIG. 8 is a schematic sectional view illustrating an example of an image-forming apparatus including the organic EL element of the present invention.
• the image-forming apparatus of FIG. 8 can selectively perform: a color mode in which toners of four colors, i.e., yellow (Y) , magenta (M) , cyan (C) , and black (K) toners are
• FIG. 8 is a sectional view of a main portion in a sub- scanning direction.
• code data Dc is input from an external device such as a personal computer to a print controller (not shown)
• the code data Dc is converted into image data (dot data) Di .
• the image data Di is input to each of exposure units 70Y, 70M, 70C, and 70K built in the image-forming apparatus. Then, the exposure units 70Y, 70M, 70C, and 70K are each controlled based on the image data Di .
• the exposure unit 70Y includes: a light-emitting
• exposure unit 70Y may include a light-absorbing member so that a position except a predetermined position on the surface of the photosensitive drum 85Y may not be irradiated with the light.
• the print controller In addition to the exposure units (70Y, 70M, 70C, and 70K) , the print controller, a transfer belt 81, a sheet-feeding unit 82, a fixing roller 83, and a pressure roller 84 are placed in a casing 80 of the image-forming apparatus. Further, photosensitive drums (85Y, 85M, 85C, and 85K) , charging rollers (86Y, 86 , 86C, and 86K) , developing devices (87Y, 87 , 87C, and 87K) , and transfer rollers (88Y, 88M, 88C, and 88K) are placed in the casing 80. In the image-forming
• the sheet-feeding unit 82 is removably mounted.
• respective magenta (M) , cyan (C) , and black (K) images are sequentially formed in the same manner as in the formation of the yellow (Y) image upon conveyance of paper by the transfer belt 81.
• the photosensitive drum 85Y as an electrostatic latent image-bearing member is rotated clockwise by a motor (not shown) based on a signal from the print controller. Then, in association with the rotation, each photosensitive surface of the photosensitive drum 85Y rotates with respect to each exposure light.
• the charging roller 86Y for charging the surface of the photosensitive drum 85Y according to a desired pattern is provided below the photosensitive drum 85Y so as to abut on the surface. Then, the surface of the
• photosensitive drum 85Y uniformly charged by the charging roller 86Y is irradiated with exposure light by the exposure unit 70Y.
• irradiation time, irradiation intensity, and the like of the exposure light emitted from the exposure unit 70Y are adjusted based on the image data Di, and then an electrostatic latent image is formed on the surface of the photosensitive drum 85Y by the exposure light.
• the electrostatic latent image is developed as a toner image by the developing device 87Y provided on a downstream side in the rotation direction of the photosensitive drum 85Y relative to the irradiation position of the exposure light so as to abut on the photosensitive drum 85Y.
• the toner image developed by the developing device 87Y is transferred onto the paper as a transfer material by the transfer roller 88Y provided below the
• the paper which is stored in a paper cassette in the sheet-feeding unit 82, can also be fed with a manual bypass tray.
• a sheet-feeding roller is provided at an end portion of the paper cassette and feeds the paper in the paper cassette into a conveyance path.
• the paper onto which the toner image has been transferred is conveyed to a fixing device by the transfer belt 81.
• the fixing device is constituted of the fixing roller 83 including a fixing heater (not shown) in itself and the pressure roller 84 provided so as to be in pressure contact with the fixing roller 83, and the device fixes the toner image on the conveyed paper by heating the paper while pressurizing the paper with the fixing roller 83 and the pressure roller 84.
• the image-forming apparatus includes the organic EL element of the present
• a photosensitive member on the surface of which a latent image is formed by the organic EL element and a charging unit for charging the
• FIG. 9 is a schematic sectional view illustrating an example of a display apparatus including the organic EL element of the present invention.
• the organic EL element of the present invention can be used as a constituent member for a pixel 4 in the display apparatus.
• the display apparatus includes multiple organic EL elements and a drive circuit for driving the organic EL elements.
• the multiple organic EL elements are preferably placed in a two- dimensional manner.
• each pixel unit is constituted of multiple pixels having different luminescent colors such as a red-light-emitting pixel, a green-light- emitting pixel, and a blue-light-emitting pixel.
• the red-light-emitting pixel includes an organic EL element that emits red light.
• pixel refers to the minimum unit whose light emission can be independently controlled.
• pixel unit refers to the minimum unit that: is constituted of multiple pixels having different luminescent colors; and can emit light having a desired color through the color mixing of the
• all pixels may each be the organic EL element of the present invention or only part of the pixels may each be the organic EL element of the present invention. That is, a construction in which both the organic EL element of the present invention and the conventional organic EL element are present is permitted. In this case, the emission characteristics of the display apparatus can be adjusted by adjusting a ratio between both the elements.
• the organic EL element of the present invention and the conventional organic EL element may be regularly arrayed.
• the organic EL elements of the present invention may be irregularly placed in a scattered manner.
• a pixel may be provided with a unit for improving light extraction efficiency.
• the unit may be provided in each of the pixels or may be provided only in a specific pixel.
• Examples of the display apparatus include a television set, the display of a personal computer, the back- surface display portion of an imaging apparatus, the display portion of a portable telephone, and the display portion of a portable game machine. Further examples thereof include the display portion of a portable music-reproducing apparatus, the display portion of a personal digital assistant (PDA) , and the display portion of a car navigation system.
• PDA personal digital assistant
• FIG. 10 is a schematic sectional, view illustrating an example of an imaging apparatus including the organic EL element of the present invention.
• the imaging apparatus of FIG. 10 includes a display apparatus 94 including the organic EL element, and includes, in a casing 90, a low-pass filter 91, an infrared cut filter 92, and an imaging element 93 such as a CMOS sensor.
• the display apparatus 94 is placed in the casing 90 of the imaging apparatus, and can display an image
• a lens 95 is provided outside the casing 90 of the imaging apparatus, and the lens 95 is removably mounted onto the casing 90. It is to be noted that the display apparatus according to this embodiment is also
• An organic EL element (blue organic EL element) of FIG. 1 was produced by the following method. It is to be noted that part of the materials used in this example are shown below.
• a TFT drive circuit (not shown) formed of low- temperature polysilicon was formed on a glass base material.
• an acrylic resin was formed into a film on the TFT drive circuit to form a planarizing film (not shown) .
• the substrate 10 by a sputtering method to form an Ag alloy film.
• the thickness of the Ag alloy film was set to 150 nm.
• an iridium tin oxide (ITO) was formed into a film on the Ag alloy film by the sputtering method to form an ITO film.
• the thickness of the ITO film was set to 5 nm.
• a laminated electrode film formed of the Ag alloy film and the ITO film was subjected to patterning according to an emission region.
• the lower electrode 21 (reflective electrode) having a predetermined pattern shape was formed.
• a polyimide-based resin was formed into a film by a spin coating method to form an insulating layer.
• the insulating layer was subjected to patterning by a photolithography method so that an opening was formed in a region where an organic EL element was to be provided, whereby an element isolation film was formed.
• Compound 1 was formed into a film on the lower electrode 21 by a vacuum deposition method to form a first hole injection/transport layer (the first charge injection/transport layer 22).
• injection/transport layer 23 functions as a low- refractive index layer having a refractive index lower than that of an adjacent layer by 0.1 or more.
• Compound 4 (host) and Compound 5 (guest) were codeposited from the vapor onto the electron-blocking layer to form the emission layer 24.
• the emission layer 24 had a thickness of 15 nm
• Compound 6 was formed into a film on the emission layer 24 by a vacuum deposition method to form an electron injection/transport layer (the third charge injection/transport layer 25) .
• the thickness of the electron injection/transport layer (third charge injection/transport layer 25) was set to 20 nm.
• Compound 6 and Cs were codeposited from the vapor onto the electron injection/transport layer (third charge injection/transport layer 25) to form an electron injection layer, (not shown). At this time, the thickness of the electron injection layer was set to 20 nm.
• Ag was formed into a film on the electron
• the thickness of the upper electrode 26 was set to 12 nm.
• Alq 3 was formed into a film on the upper electrode 26 to form the optical adjustment layer 30.
• the thickness of the optical adjustment layer 30 was set to 70 nm.
• the organic EL element was obtained.
• the electron-blocking layer is provided between the
• the electron-blocking layer does not affect an
• each of p in the expression (2) and q in the expression (3) equals 0.
• Compound 1 was formed into a film having a thickness of 135 nm to serve as the first charge
• injection/transport layer 22 and Compound 7 was formed into a film having a thickness of 10 nm to serve as the second charge in ection/transport layer 23.
• the organic EL element 2 (blue organic EL element) of FIG. 6 was produced by a method described below.
• the substrate 10 was produced by the same method as Example 1.
• the substrate 10 by a sputtering method to form an Ag alloy film.
• the thickness of the Ag alloy film was set to 150 nm.
• the Ag alloy film was
• the lower electrode 21 (reflective electrode) having a predetermined pattern shape was formed.
• a polyimide-based resin was formed into a film by a spin coating method to form an insulating layer.
• the insulating layer was subjected to patterning by a photolithography method so that an opening was formed in a region where an organic EL element was to be provided, whereby an element isolation film was formed.
• the emission layer 24 was formed by the same method as that of Example 1.
• the electron in ection/transport layer (third charge injection/transport layer) 25 and an electron transport layer to be formed on the electron in ection/transport layer were formed by the same method as that of Example 1.
• the upper electrode 26 and the optical adjustment layer 30 were sequentially formed by the same method as that of Example 1. After that, the same sealing treatment as that of Example 1 was performed to provide the organic EL element .
• the emission efficiency of the resultant organic EL element was 5.2 cd/A in the same chromaticity
• An organic EL element blue organic EL element in which each organic layer between a reflective electrode and an emission layer was formed of a low-refractive index layer was produced by a method described below.
• the substrate 10 was produced by the same method as Example 2.
• a lower electrode was produced by the same method as Example 2.
• the emission layer 24 was formed by the same method as that of Example 1.
• the electron injection/transport layer (third charge injection/transport layer) 25 and an electron transport layer to be formed on the electron injection/transport layer were formed by the same method as that of Example 1.
• the upper electrode 26 and the optical adjustment layer 30 were sequentially formed by the same method as that of Example 1. After that, the same sealing treatment as that of Example 1 was performed to provide the organic EL element.
• Patent Application No. 2013-084661 filed April 15, 2013, which is hereby incorporated by reference herein in its entirety.

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