WO2012161179A1 - Dispositif électroluminescent - Google Patents

Dispositif électroluminescent Download PDF

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Publication number
WO2012161179A1
WO2012161179A1 PCT/JP2012/063019 JP2012063019W WO2012161179A1 WO 2012161179 A1 WO2012161179 A1 WO 2012161179A1 JP 2012063019 W JP2012063019 W JP 2012063019W WO 2012161179 A1 WO2012161179 A1 WO 2012161179A1
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light emitting
transport layer
layer
emitting layer
quantum dots
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Japanese (ja)
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晴哉 宮田
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株式会社 村田製作所
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y20/00—Nanooptics, e.g. quantum optics or photonic crystals
    • 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
    • H05B33/14—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of the electroluminescent material, or by the simultaneous addition of the electroluminescent material in or onto the light source
    • 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]
    • H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] 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]
    • H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
    • H10K50/115—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising active inorganic nanostructures, e.g. luminescent quantum dots
    • 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]
    • H10K50/14—Carrier transporting layers
    • H10K50/15—Hole 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]
    • H10K50/14—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
    • H10K2101/00—Properties of the organic materials covered by group H10K85/00
    • H10K2101/30—Highest occupied molecular orbital [HOMO], lowest unoccupied molecular orbital [LUMO] or Fermi energy values
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2101/00—Properties of the organic materials covered by group H10K85/00
    • H10K2101/40—Interrelation of parameters between multiple constituent active layers or sublayers, e.g. HOMO values in adjacent layers
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
    • H10K2102/301—Details of OLEDs
    • H10K2102/331—Nanoparticles used in non-emissive layers, e.g. in packaging layer

Definitions

  • the present invention relates to a light emitting device, and more particularly to a light emitting device having a light emitting layer formed of quantum dots.
  • Quantum dots which are nanoparticles with a particle size of 10 nm or less, have excellent carrier (electron, hole) confinement properties, and can easily generate excitons by electron-hole recombination. Therefore, light emission from free excitons can be expected, and it is possible to realize sharp light emission with high emission efficiency and a narrow half-value width. Further, since quantum dots can be controlled in a wide wavelength range using the quantum size effect, their application to light emitting devices such as light emitting diodes (LEDs) and semiconductor lasers has attracted attention.
  • LEDs light emitting diodes
  • Non-Patent Document 1 reports improved characteristics of multilayer quantum dot light-emitting diodes by heat treatment of quantum dot layers.
  • Non-Patent Document 1 the hole transport layer 103 and the electron transport layer 105 (hereinafter, these may be collectively referred to as “carrier transport layer”) are formed of an organic semiconductor, and these hole transport layers 103 are formed.
  • a light emitting layer 104 made of an inorganic semiconductor quantum dot 104 a is provided between the electron transport layer 105 and the electron transport layer 105. Then, by applying a voltage between the anode 101 and the cathode 106, holes are injected into the quantum dots 104 a through the hole injection layer 102 and the hole transport layer 103, while electrons pass through the electron transport layer 105. Then, it is injected into the quantum dot 104a, and holes and electrons are recombined in the quantum dot 104 to emit excitons.
  • the light emitting diode which uses the quantum dot produced by the liquid phase method as the light emitting layer 104 has a structure in which the light emitting layer in the organic EL (electroluminescence) element is formed with an inorganic semiconductor quantum dot instead of an organic semiconductor.
  • the carrier transport layers 103 and 105 are usually formed of an organic semiconductor.
  • the molecular orbitals are in an empty state not occupied by electrons, but the lowest molecular orbital among these molecular orbitals not occupied by electrons (Lowest ⁇ Unoccupied Molecular Orbital;
  • the energy level corresponding to this LUMO is the LUMO level.
  • electrons move in the LUMO level (conduction band), and holes move in the HOMO level (valence band).
  • FIG. 10 is an energy state diagram of Non-Patent Document 1.
  • the HOMO level h 1 of BiVB-MeTPD forming the hole transport layer 103 is 5.3 eV
  • the HOMO level h 2 of TPBI forming the electron transport layer 105 is 6.3 eV
  • Non-Patent Document 1 lacks consistency in the energy level, and therefore, carriers cannot be efficiently injected into the quantum dot core portion 104a ′, and the injected carriers are not allowed to flow into the quantum dot core portion. It is difficult to confine effectively in 104a '. As a result, electrons and holes cannot be efficiently recombined in the quantum dot core portion 104a ′, resulting in a decrease in light emission efficiency.
  • the carrier transport layers 103 and 105 As the characteristics of the carrier transport layers 103 and 105, it is desired that the carrier mobility is high and the transportability is good. In organic semiconductors having high carrier mobility, the ⁇ bond system often carries carrier transport.
  • ⁇ -bonded electrons absorb ultraviolet light and have a weaker binding force than ⁇ bonds.
  • an organic semiconductor having a high carrier mobility in which the ⁇ bond system is responsible for carrier transport may be decomposed by absorption of ultraviolet light, and thus has a problem of low durability against ultraviolet light.
  • the present invention has been made in view of such circumstances, and an object of the present invention is to provide a light emitting device capable of improving the injection efficiency and confinement efficiency of carriers into quantum dots and obtaining good light emission efficiency. To do.
  • the hole transport layer is required to have a function of efficiently injecting holes into the light emitting layer and confining electrons injected from the electron transport layer into the light emitting layer.
  • the electron transport layer is required to have a function of efficiently injecting electrons into the light emitting layer and confining holes injected from the hole transport layer into the light emitting layer. Therefore, in order to increase the efficiency of injecting carriers into the light emitting layer and effectively confine the carriers in the light emitting layer, the hole transport layer and the electron transport layer need to have appropriate energy levels.
  • the carrier transport layer (hole transport layer and electron transport layer) with quantum dots of an inorganic semiconductor instead of an organic semiconductor
  • the energy level of the carrier transport layer can be simply changed by changing the particle size of these quantum dots. The position can be adjusted.
  • the present invention has been made based on such knowledge, and the light-emitting device according to the present invention has a light-emitting layer formed of first quantum dots interposed between a hole transport layer and an electron transport layer.
  • the hole transport layer and the electron transport layer are formed of second and third quantum dots made of an inorganic material different from the first quantum dots, respectively. It is said.
  • the hole transport layer and the electron transport layer can obtain appropriate energy levels only by changing the particle diameters of the second and third quantum dots.
  • the injection efficiency can be increased, and the carriers can be effectively confined in the light emitting layer.
  • the light emitting layer and the hole transport are made so that the LUMO level of the hole transporting layer is sufficiently smaller than the LUMO level of the light emitting layer.
  • a large electron transport barrier needs to be formed between the layers.
  • the energy level of the hole transport layer so that the hole transport barrier from the hole transport layer to the light-emitting layer is small and the electron transport barrier from the light-emitting layer to the hole transport layer is large.
  • the light emitting layer and the electron transport layer are formed so that the HOMO level of the electron transport layer is sufficiently larger than the HOMO level of the light emitting layer. It is necessary to form a large hole transport barrier between them.
  • the energy level of the electron transport layer so that the electron transport barrier from the electron transport layer to the light emitting layer is small and the hole transport barrier from the light emitting layer to the electron transport layer is large.
  • the light emitting device of the present invention has a small hole and electron transport barrier transported from the hole transport layer and the electron transport layer to the light emitting layer, and the electron transport layer and the hole transport from the light emitting layer.
  • the particle size of the second and third quantum dots is controlled so that a hole and electron transport barrier transported to the layer is increased, and each energy level of the hole transport layer and the electron transport layer is controlled. Is preferably adjusted.
  • the second and third quantum dots are formed of an inorganic material having a larger band gap energy than the light emitting layer so as not to absorb the light emitted from the light emitting layer, thereby effectively improving the light emission efficiency. It becomes possible.
  • the carrier transport layer does not absorb the light emitted from the light emitting layer, and a light emitting device having better light emission efficiency can be obtained.
  • the hole transport layer is formed on the surface of the first electrode, and the HOMO level of the hole transport layer is determined by the work function of the first electrode and the light emitting layer. It is preferable that the average particle diameter of the second quantum dots is set so as to be in the middle value of the HOMO level or in the vicinity of the middle value.
  • the transport barriers between the first electrode, the hole transport layer, and the light emitting layer are made uniform or substantially uniform, and the holes injected into the anode can be smoothly injected into the light emitting layer.
  • the LUMO level of the hole transport layer has an energy level smaller than the LUMO level of the light emitting layer.
  • This increases the electron transport barrier from the light emitting layer to the hole transport layer, and enables electrons to be effectively confined in the light emitting layer.
  • the second electrode is formed on the surface of the electron transport layer, and the LUMO level of the electron transport layer is determined by the work function of the second electrode and the LUMO level of the light emitting layer. It is preferable that the average particle diameter of the third quantum dots is set so as to be an intermediate value from the level or near the intermediate value.
  • the transport barriers between the second electrode, the electron transport layer, and the light emitting layer are made uniform or substantially uniform, and the electrons injected into the cathode can be smoothly injected into the light emitting layer.
  • the HOMO level of the electron transport layer has an energy level larger than the HOMO level of the light emitting layer.
  • the first to third quantum dots are any one of an oxide semiconductor, a compound semiconductor, and a single semiconductor.
  • the hole transport layer and the electron transport layer are respectively formed of the second and third quantum dots made of an inorganic material different from the first quantum dot forming the light emitting layer. Therefore, the energy level of the carrier transport layer (the hole transport layer and the electron transport layer) can be changed by the quantum size effect only by changing the particle diameters of the second and third quantum dots, and thus the carrier It becomes possible to easily adjust the energy level of the transport layer. That is, only by changing the particle size of the second and third quantum dots, the hole transport layer and the electron transport layer can obtain appropriate energy levels, and the injection efficiency of carriers into the light emitting layer is improved. The carriers can be effectively confined in the light emitting layer.
  • the inorganic material constituting the second and third quantum dots has high mobility compared to conventional organic materials, excellent carrier transportability, and is excellent in that it is not decomposed by ultraviolet light. Has excellent durability.
  • the hole transport layer and the electron transport layer are formed of the second and third quantum dots as described above, the first quantum dot and the third quantum dot that form the second quantum dot and the light emitting layer are formed.
  • the dots and the first quantum dots are in sphere contact with each other. Therefore, the contact area between the hole transport layer and the electron transport layer and the light emitting layer is increased compared to the case where the surface and the sphere are in contact with each other as in the conventional organic material, and the probability of carrier injection into the light emitting layer is increased. This can be further improved.
  • FIG. 6 is an energy state diagram of sample number 5; It is sectional drawing which shows the conventional light-emitting device described in the nonpatent literature 1 typically. It is an energy state figure of the conventional light emitting device described in the nonpatent literature 1.
  • an anode (first electrode) 2 made of a conductive transparent material such as ITO is formed on a glass substrate (transparent substrate) 1, and a positive electrode made of a second quantum dot 3 a is formed on the surface of the anode 2.
  • a hole transport layer 3 is formed, and a light emitting layer 4 composed of the first quantum dots 4 a is formed on the surface of the hole transport layer 3.
  • an electron transport layer 5 composed of third quantum dots 5a is formed on the surface of the light emitting layer 4, and a cathode (second electrode) 6 containing a metal conductive material such as Al is formed on the surface of the electron transport layer 5. Is formed.
  • the hole transport layer 3 and the electron transport layer 5 are the second and third quantum dots 3 a and 5 a made of an inorganic material different from the first quantum dot 4 a forming the light emitting layer 4. Each is formed.
  • the light emitting diode has a small hole and electron transport barrier transported from the hole transport layer 3 and the electron transport layer 5 to the light emitting layer 4, and the light emitting layer 4 is changed from the light emitting layer 4 to the electron transport layer 3 and the hole transport layer 5.
  • the energy levels of the hole transport layer 3 and the electron transport layer 5 are adjusted by the second and third quantum dots 3a and 5a so that the transport barriers of the transported holes and electrons are increased.
  • carriers can be efficiently injected into the first quantum dots 4a, and these carriers can be effectively confined in the first quantum dots 4a, thereby improving the recombination probability.
  • the carrier injection efficiency and the recombination probability can be improved, the driving voltage of the light emitting diode is lowered, and the light emission efficiency can be improved.
  • the function of the hole transport layer 3 is to efficiently inject holes injected from the anode 2 into the first quantum dots 4a of the light emitting layer 4, while from the electron transport layer 5 to the first quantum dots 4a.
  • the injected electrons are prevented from flowing out into the hole transport layer 3 without being recombined with holes in the first quantum dots 4a, and the electrons are effectively confined in the first quantum dots 4a. It is in.
  • the function of the electron transport layer 5 is that the electrons injected from the cathode 6 are efficiently injected into the first quantum dots 4a, while the electrons are injected from the hole transport layer 3 into the first quantum dots 4a.
  • the purpose is to prevent holes from flowing out into the electron transport layer 5 without recombining with electrons in the first quantum dots 4a, and to effectively confine holes in the first quantum dots 4a.
  • the hole transport layer 3 and the electron transport layer 5 have appropriate values of the HOMO level and the LUMO level. By forming, carrier injection efficiency and confinement efficiency can be improved.
  • the hole transport layer 3 when the HOMO level of the hole transport layer 3 is larger than the HOMO level of the light-emitting layer 4, there is no hole transport barrier from the hole transport layer 3 to the light-emitting layer 4, and the holes are emitted from the light-emitting layer. 4 is easily injected.
  • the HOMO level of the hole transport layer 3 when the HOMO level of the hole transport layer 3 is smaller than the HOMO level of the light emitting layer 4, a hole transport barrier is formed between the hole transport layer 3 and the light emitting layer 4, and the hole transport barrier is formed. Is small, holes are injected into the light emitting layer 4 relatively easily. However, when the hole transport barrier is large, holes are hardly injected into the light emitting layer 4.
  • the difference between the LUMO level of the hole transport layer 3 and the LUMO level of the light emitting layer 4 is small, electrons injected into the light emitting layer 4 easily flow out to the hole transport layer 3 and transport holes.
  • the LUMO level of the layer 3 is sufficiently smaller than the LUMO level of the light emitting layer 4, a large electron transport barrier is formed, and electrons can be effectively confined in the light emitting layer 4.
  • the HOMO of the hole transport layer is set so as to be in the middle value of the work function of the anode 2 and the HOMO level of the light emitting layer 4 or in the vicinity of the intermediate value.
  • the hole transport barrier can be made as small as possible, and holes can be efficiently injected into the light emitting layer 4.
  • the LUMO level of the electron transport layer 5 is smaller than the LUMO level of the light-emitting layer 4, there is no electron transport barrier from the electron transport layer 5 to the light-emitting layer 4, and electrons are easily in the light-emitting layer 4. Injected into.
  • the LUMO level of the electron transport layer 5 is larger than the LUMO level of the light emitting layer 4, an electron transport barrier is formed between the electron transport layer 3 and the light emitting layer 4, and when the electron transport barrier is small, Can be injected into the light emitting layer 4 relatively easily.
  • the electron transport barrier is increased, electrons are hardly injected into the light emitting layer 4.
  • the electron transport having a LUMO level that is an intermediate value between the work function of the cathode 6 and the LUMO level of the light emitting layer 4 or near the intermediate value.
  • the electron transport barrier can be made as small as possible, and electrons can be efficiently injected into the light emitting layer 4.
  • the light emitting layer is formed of an inorganic semiconductor material, but the hole transport layer and the electron transport layer are formed of an organic semiconductor. Therefore, it has been difficult to obtain sufficiently good injection efficiency and confinement efficiency.
  • the transport barrier between the carrier transport layers 3 and 5 changes, but the carrier transport layer 3
  • an organic semiconductor material corresponding to the energy structure must be selected in order to optimize the energy structure, resulting in a complicated structure design of the device.
  • quantum dots (second and third quantum dots 3a and 5a) made of an inorganic material that can easily control the energy level by adjusting the particle size without depending on the material type.
  • the hole transport layer 3 and the electron transport layer 5 are formed, thereby matching the energy levels between the respective layers (between the anode 2, the hole transport layer 3, the light emitting layer 4, the electron transport layer 5 and the cathode 6), Carrier injection efficiency and confinement efficiency are improved.
  • the inorganic material has higher carrier mobility than the organic material, is excellent in carrier transportability, and can obtain good durability without being decomposed by ultraviolet light.
  • the hole transport layer 3 and the electron transport layer 5 are formed by the second and third quantum dots 3a and 5a as described above, the first quantum that forms the light emitting layer 4 with the second quantum dots 3a.
  • the dots 4a and the third quantum dots 5a and the first quantum dots 4a come into contact with each other in spheres, and the light emitting layer 4 is compared with the case where the surface and the sphere are in contact with each other as in the case of a conventional organic material.
  • the first quantum dots 4a forming the sphere are in contact with each other. Therefore, the contact area between the hole transport layer 3 and the electron transport layer 5 and the light emitting layer 4 is increased as compared with the case where the surface and the sphere are in contact with each other as in the case of a conventional organic material.
  • the injection probability of can be further improved.
  • the HOMO level H 0 and the LUMO level L 0 of the light emitting layer 4 according to the average particle diameter are determined.
  • the quantum dot HOMO level (hereinafter referred to as “quantum dot HOMO level”) E Hd (eV) and the quantum dot LUMO level (hereinafter referred to as “quantum dot LUMO level”).
  • E Ld (eV) can be expressed by Equations (1) and (2).
  • the quantum dot HOMO level E Hd and the quantum dot LUMO level E Ld corresponding to the average particle diameter are calculated by substituting the average particle diameter and other known numerical values into the formulas (1) and (2), and the light emitting layer 4
  • the HOMO level H 0 and the LUMO level L 0 of the (first quantum dot 4a) are determined.
  • an inorganic material larger than the band gap energy Eg of the light emitting layer 4 is selected so that the light emitted from the light emitting layer 4 is not absorbed.
  • the HOMO level H 1 of the hole transport layer 3 is determined.
  • the difference between the HOMO level H 1 of the hole transport layer 3 and the HOMO level H 0 of the light-emitting layer 4 is small Is preferred.
  • the difference between the work function W 1 of the anode 2 and the HOMO level H 1 of the hole transport layer 3 is small. Is preferred.
  • the particle size d is substituted into the formula (2) to obtain the quantum dot LUMO level E Ld, thereby determining the LUMO level L 1 of the hole transport layer 3.
  • an inorganic material used for the electron transport layer 5 is selected.
  • an inorganic material larger than the band gap energy Eg of the light emitting layer 4 is selected so that the light emitted from the light emitting layer 4 is not absorbed.
  • the LUMO level L 2 and the HOMO level H 2 of the electron transport layer 5 are determined as follows.
  • the cathode 6 ⁇ the electron
  • the electron transport barrier in the transport layer 5 ⁇ the light emitting layer 4 can be optimized.
  • the second quantum dots 3a forming the hole transport layer 3 are not particularly limited as long as they are inorganic semiconductor materials larger than the band gap energy Eg of the first quantum dots 4a.
  • An inorganic semiconductor material having a high hole mobility in the transport layer 3 is preferably used.
  • an oxide semiconductor such as NiO or MoO 3 or a compound semiconductor such as ZnTe or CdTe can be used.
  • the third quantum dot 5a forming the electron transport layer 5 is not particularly limited as long as it is an inorganic semiconductor material larger than the band gap energy of the first quantum dot 4a. It is preferable to use an inorganic semiconductor material having a high electron mobility therein.
  • an oxide semiconductor such as ZnO or TiO 2 or a compound semiconductor such as ZnS, ZnSe, or GaN can be used.
  • FIG. 3 is a manufacturing process diagram showing a manufacturing method of the light emitting diode.
  • a transparent film such as ITO is formed on a glass substrate 1 by sputtering or the like, and UV ozone treatment is performed to form an anode 2 having a thickness of 100 nm to 150 nm.
  • the second quantum dot dispersion solution is applied onto the anode 2 to form the hole transport layer 3 having a thickness of 50 to 100 nm composed of the second quantum dots 3a.
  • a first quantum dot dispersion solution in which the first quantum dots 4a are dispersed in a dispersion solvent is prepared.
  • the first quantum dot dispersion solution is applied onto the hole transport layer 3, and as shown in FIG. A 20 nm light emitting layer 4 is formed.
  • the third quantum dot dispersion solution is applied onto the light emitting layer 4, and as shown in FIG. 3C, the film thickness of 50 to 100 nm made of the third quantum dots 5a is formed.
  • the electron transport layer 5 is formed.
  • LiF, Al, or the like is used to form a cathode 6 having a film thickness of 100 nm to 300 nm by a vacuum deposition method, whereby a light emitting diode is manufactured.
  • the hole transport layer 3 is directly formed on the surface of the anode 2.
  • a hole injection layer may be interposed between the anode 2 and the hole transport layer 3. It is also preferred to optimize the energy structure by multilayering the transport layer 3 to reduce the interlayer barrier.
  • an organic material such as PEDOT: PSS or an inorganic material may be used as the material of the hole injection layer.
  • an organic material such as PEDOT: PSS or an inorganic material may be used as the material of the hole injection layer.
  • an organic material it is possible to contribute to planarization of the electrode surface.
  • the first to third quantum dots 3a to 5a have only a core portion and no shell portion, but have a core-shell structure or a core-shell-shell structure in which the shell portion has a two-layer structure. The same applies to the above.
  • Example No. 1 [Design of energy structure] ITO having a work function of 4.9 eV was used as the anode material, and Al having a work function of 4.3 eV was used as the cathode material.
  • InP quantum dots were used as the light emitting layer, and the average particle size was set to 6.8 nm (band gap energy Eg: 1.8 eV).
  • the quantum dot HOMO level E Hd and the quantum dot LUMO level E Ld are calculated from the mathematical formulas (1) and (2) described in [Description of Embodiments], and the HOMO level of the InP quantum dot is calculated. H 0 and LUMO level L 0 were obtained.
  • the bulk HOMO level E Hb of InP is 5.8 eV
  • bulk LUMO level E Lb is 4.5 eV
  • holes and electrons effective mass m h in InP from the following non-patent document 2
  • NiO quantum dots having a band gap energy Eg sufficiently larger than the band gap energy Eg of the InP quantum dots were selected as the hole transport layer material.
  • the average particle size of NiO quantum dots was determined.
  • the HOMO of NiO quantum dots is obtained from Equation (1).
  • the average particle diameter d corresponding to the level H Hd : 5.4 eV was determined to be 9.0 nm.
  • the quantum LUMO level E Lb of NiO is 1 .6 eV. J. Mater. Chem., 2007, 17, 127
  • ZnO quantum dots having band gap energy Eg sufficiently larger than the band gap energy Eg of InP quantum dots were selected as the electron transport layer material.
  • the average particle diameter of ZnO quantum dots was determined.
  • the LUMO level of ZnO quantum dots is obtained from Equation (2).
  • the average particle diameter d corresponding to the position L 2 : 4.2 eV was determined to be 7.7 nm.
  • Example preparation First, an InP quantum dot dispersion solution in which InP quantum dots (first quantum dots) were dispersed in toluene (dispersion solvent) was prepared.
  • indium acetate (In (CH 3 COO) 3 ) and myristic acid (C 13 H 27 COOH) were dissolved in octadecene (C 18 H 36 ) to prepare an In raw material solution.
  • trismethylsilylphosphine ((CH 3 ) 3 Si) 3 P) and octylamine (C 8 H 17 NH 2 ) were dissolved in octadecene to prepare a P raw material solution.
  • the In raw material solution was heated to 200 ° C.
  • the P raw material solution was dropped into the heated In raw material solution, and held for 2 hours to obtain InP quantum dots having an average particle diameter of 6.8 nm.
  • NiO quantum dot dispersion solution in which NiO quantum dots (second quantum dots) were dispersed in 2-propanol (dispersion solvent) was prepared.
  • Ni (CH 3 COO) nickel acetate
  • ethanol C 2 H 5 OH
  • sodium hydroxide NaOH
  • a sodium hydroxide / ethanol solution was added dropwise to the nickel acetate / ethanol solution and held for 2 hours to obtain NiO quantum dots having an average particle size of 9.0 nm.
  • a centrifuge is used to separate the precipitate from the unreacted material, and the precipitate is redispersed in 2-propanol (CH 3 CH (OH) CH 3 ), thereby producing a NiO quantum dot dispersion solution. did.
  • ZnO quantum dot dispersion solution in which ZnO quantum dots (third quantum dots) were dispersed in 2-propanol (dispersion solvent) was prepared.
  • zinc acetate Zn (CH 3 COO)
  • sodium hydroxide was dissolved in ethanol to prepare a sodium hydroxide / ethanol solution.
  • a sodium hydroxide / ethanol solution was dropped into the zinc acetate / ethanol solution and held for 2 hours to obtain ZnO quantum dots having an average particle size of 7.7 nm.
  • the precipitate and the unreacted material were separated using a centrifuge, and the precipitate was redispersed in 2-propanol, thereby preparing a ZnO quantum dot dispersion solution.
  • an ITO film was formed on the glass substrate by a sputtering method, UV ozone treatment was performed, and an anode with a film thickness of 120 nm was produced.
  • a NiO quantum dot dispersion solution was applied on the anode to form a hole transport layer having a thickness of 50 nm.
  • an InP quantum dot dispersion solution was applied onto the hole transport layer to form a light emitting layer having a thickness of 20 nm.
  • a ZnO quantum dot dispersion solution was applied onto the light emitting layer to form an electron transport layer having a thickness of 50 nm.
  • a cathode having a film thickness of 100 nm was formed by a vacuum deposition method, and thereby a sample of sample number 1 was produced.
  • Table 1 shows the average particle diameter, HOMO level, LUMO level, and band gap energy Eg of the first to third quantum dots of sample number 1.
  • Example No. 2 [Design of energy structure] Similar to Sample No. 1, ITO was used as the anode, NiO quantum dots with an average particle size of 9.0 nm were used as the hole transport layer, and Al was used as the cathode.
  • the HOMO level H 2 of ZnO was found to be 7.9 eV.
  • Example preparation An InP quantum dot dispersion solution having an average particle size of 4.7 nm was prepared by dripping the P raw material solution into the In raw material solution and holding it for 1 hour in the same manner as in Sample No. 1.
  • a ZnO quantum dot dispersion solution having an average particle size of 4.4 nm was prepared by dripping a sodium hydroxide / ethanol solution into a zinc acetate / ethanol solution and holding it for 1 hour in the same manner as in Sample No. 1. .
  • sample of sample number 2 was prepared in the same manner and procedure as sample number 1.
  • Table 2 shows the average particle diameter, HOMO level, LUMO level, and band gap energy Eg of each quantum dot of sample number 2.
  • Example No. 3 [Design of energy structure] Similar to Sample No. 1, ITO was used as the anode and Al was used as the cathode.
  • This InP quantum dot was used as a light emitting layer, and the average particle diameter was set to 3.7 nm (band gap energy Eg: 2.9 eV).
  • This InP quantum dot has a HOMO level H 0 of 6.0 eV and a LUMO level L 0 of 3.1 eV according to equations (1) and (2).
  • NiO was used as the hole transport layer material.
  • the average particle diameter was determined from Equation (1), it was 5.8 nm.
  • the average particle size was determined from 2), it was 3.3 nm.
  • Example preparation An InP quantum dot dispersion solution having an average particle diameter of 3.7 nm was prepared by dripping the P raw material solution into the In raw material solution and holding it for 30 minutes in the same manner as in Sample No. 1.
  • a ZnO quantum dot dispersion solution having an average particle diameter of 3.3 nm was prepared by dropping a sodium hydroxide / ethanol solution into a zinc acetate / ethanol solution and maintaining it for 30 minutes in the same manner as in Sample No. 1.
  • sample No. 3 was prepared in the same manner and procedure as the sample No. 1.
  • Example No. 4 [Design of energy structure] Similar to Sample No. 1, ITO was used as the anode and Al was used as the cathode.
  • CdSe quantum dots were used as the light emitting layer, and the average particle size was set to 5.5 nm (band gap energy Eg: 2.2 eV).
  • NiO having an average particle diameter of 2.0 nm was selected for the hole transport layer.
  • the HOMO level H 1 and LUMO level L 1 of NiO corresponding to an average particle diameter of 2.0 nm were found to be 5.9 eV and 1.5 eV from the equations (1) and (2), respectively.
  • ZnO having an average particle diameter of 7.8 nm was selected for the electron transport layer.
  • the HOMO level H 2 and LUMO level L 2 of ZnO corresponding to an average particle diameter of 7.8 nm were found to be 7.8 eV and 4.2 eV from Equations (1) and (2), respectively.
  • Example preparation First, a CdSe quantum dot dispersion solution in which CdSe quantum dots (first quantum dots) were dispersed in toluene (dispersion solvent) was prepared.
  • CdO cadmium oxide
  • octadecylamine C 13 H 37 NH 2
  • selenium Se
  • tributylphosphine (C 4 H 9 ) 3 P) were dissolved in octadecene to prepare a Se raw material solution.
  • the Cd raw material solution is heated to 280 ° C.
  • the Se raw material solution is dropped into the heated Cd raw material solution, and held at a temperature of 250 ° C. for 1 hour to obtain CdSe quantum dots having an average particle size of 5.5 nm. Produced.
  • unreacted substances and CdSe quantum dots were separated using methanol, and the precipitated CdSe quantum dots were redispersed in toluene, thereby preparing a CdSe quantum dot dispersion solution.
  • a NiO quantum dot dispersion solution having an average particle diameter of 2.0 nm was prepared by dropping a sodium hydroxide / ethanol solution into a nickel acetate / ethanol solution and maintaining it for 30 minutes in the same manner as in sample number 1.
  • a ZnO quantum dot dispersion solution having an average particle diameter of 7.8 nm was prepared by dripping a sodium hydroxide / ethanol solution into a zinc acetate / ethanol solution and keeping it for 2 hours in the same manner as in Sample No. 1.
  • a sample No. 4 was prepared in the same manner and procedure as Sample No. 1 except that the above CdSe quantum dot dispersion solution, NiO quantum dot dispersion solution, and ZnO quantum dot dispersion solution were used.
  • Table 4 shows the average particle diameter, HOMO level, LUMO level, and band gap energy Eg of each quantum dot of sample number 4.
  • Sample No. 5 [Design of energy structure] Similar to Sample No. 1, ITO was used as the anode, Al was used as the cathode, and ZnO having an average particle diameter of 7.8 nm was used as the Sample No. 4 as the electron transport layer.
  • This CdSe quantum dot has a HOMO level H 0 of 6.7 eV and a LUMO level L 0 of 4.9 eV according to equations (1) and (2).
  • NiO having an average particle diameter of 2.3 nm was selected for the hole transport layer.
  • the HOMO level H 1 and LUMO level L 1 of NiO corresponding to an average particle diameter of 2.0 nm were determined to be 5.8 eV and 1.5 eV from the equations (1) and (2), respectively.
  • a NiO quantum dot dispersion solution having an average particle size of 2.3 nm was prepared by dropping a sodium hydroxide / ethanol solution into a nickel acetate / ethanol solution and holding it for 30 minutes in the same manner as in sample number 1.
  • Table 5 shows the average particle diameter, HOMO level, LUMO level, and band gap energy Eg of each quantum dot of sample number 5.
  • FIG. 4 to 8 are energy state diagrams showing the energy states of the samples of sample numbers 1 to 5.
  • FIG. 4 to 8 are energy state diagrams showing the energy states of the samples of sample numbers 1 to 5.
  • Table 6 shows hole or electron transport barriers.
  • Table 6 shows hole or electron transport barriers in Non-Patent Document 1 as comparative examples.
  • the hole transport barrier from the hole transport layer to the light emitting layer is 1.5 eV, the hole transport barrier is high, and the carrier injection efficiency is poor.
  • the electron transport barrier from the light-emitting layer to the hole transport layer is relatively high at 2.1 eV
  • the hole transport barrier from the light-emitting layer to the electron transport layer is as low as ⁇ 0.5 eV. Holes injected into the InP quantum dots of the layer easily flow out to the electron transport layer, and it is difficult to effectively confine electrons in the InP quantum dots.
  • Sample No. 1 has a hole transport barrier of 0.5 eV from the hole transport layer to the light emitting layer, and electron transport from the electron transport layer to the light emitting layer.
  • the barrier is also 0.1 eV, and both have low carrier transport barriers, and carriers can be easily injected from the carrier transport layer into the light emitting layer.
  • the hole transport barrier from the light-emitting layer to the electron transport layer is 1.9 eV, and the electron transport barrier from the light-emitting layer to the hole transport layer is 2.5 eV. It was found that the transport barrier is high and the carrier confinement property is excellent.
  • Sample No. 2 has a hole transport barrier from the hole transport layer to the light-emitting layer of 0.5 eV, and also has an electron transport barrier from the electron transport layer to the light-emitting layer of 0 eV. .3 eV, both of which have a low carrier transport barrier, and carriers can be easily injected from the carrier transport layer into the light-emitting layer.
  • the hole transport barrier from the light-emitting layer to the electron transport layer is 2.0 eV
  • the electron transport barrier from the light-emitting layer to the hole transport layer is 2.1 eV. It was found that the transport barrier is high and the carrier confinement property is excellent.
  • Sample No. 3 has a hole transport barrier from the hole transport layer to the light-emitting layer of 0.5 eV, and also has an electron transport barrier from the electron transport layer to the light-emitting layer of 0.
  • the carrier transport barrier is low, and carriers can be easily injected from the carrier transport layer into the light emitting layer.
  • the hole transport barrier from the light emitting layer to the electron transport layer is 2.1 eV, and the electron transport barrier from the light emitting layer to the hole transport layer is 1.5 eV. It was found that the transport barrier is high and the carrier confinement property is excellent.
  • Sample No. 4 has a hole transport barrier of 0.9 eV from the hole transport layer to the light emitting layer, and also has an electron transport barrier from the electron transport layer to the light emitting layer ⁇ Each of them is 0.4 eV, and the carrier transport barrier is low. Carriers can be easily injected from the carrier transport layer into the light emitting layer.
  • the electron transport barrier from the light emitting layer to the hole transport layer is as high as 3.1 eV, and the hole transport barrier from the light emitting layer to the electron transport layer is 1.0 eV. It was found to have a sufficiently high barrier to confine holes in CdSe quantum dots, although it is low compared to 1-3.
  • the hole transport barrier from the hole transport layer to the light emitting layer is 0.9 eV, and the electron transport barrier from the electron transport layer to the light emitting layer is ⁇
  • the carrier transport barrier is low, and the carrier can be easily injected from the carrier transport layer into the light emitting layer.
  • the electron transport barrier from the light emitting layer to the hole transport layer is as high as 3.4 eV, and the hole transport barrier from the light emitting layer to the electron transport layer is 1.1 eV. It was found to have a sufficiently high barrier to confine holes in CdSe quantum dots, although it is low compared to 1-3.
  • the electron mobility of TPBI used in the electron transport layer is 10 ⁇ 5 cm 2 / V as described in Non-Patent Document 6. -S.
  • the electron mobility of ZnO used for the electron transport layer in the examples of the present invention is 100 cm 2 / V ⁇ s as described in Non-Patent Document 7.
  • the inorganic semiconductor material of the embodiment of the present invention has a higher electron mobility than the organic semiconductor material, and thus has excellent carrier transportability, and is improved in durability without being absorbed and decomposed by ultraviolet light. You can plan. Chemical Physics Letters, 2001, 334, 61 Appl.Phys.Lett. 2005, 87, 152101

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Abstract

Selon l'invention, une couche de transport de trous positifs (3) et une couche de transport d'électrons (5) sont formées respectivement par des deuxièmes et troisièmes points quantiques (3a, 5a) faits d'un matériau inorganique différent de celui de premiers points quantiques (4a) qui forment une couche électroluminescente (4). Les niveaux d'énergie de la couche de transport de trous positifs (3) et de la couche de transport d'électrons (5) sont ajustés par les deuxièmes et troisièmes points quantiques (3a, 5a), si bien que la barrière s'opposant au transport des trous positifs et des électrons provenant de la couche de transport de trous positifs (3) et de la couche de transport d'électrons (5) vers la couche électroluminescente (4) est faible et que la barrière s'opposant au transport des trous positifs et des électrons provenant de la couche électroluminescente (4) vers la couche de transport d'électrons (5) et la couche de transport de trous positifs (3) est élevée. De cette manière, il est possible de réaliser un dispositif électroluminescent dans lequel l'efficacité de l'injection et l'efficacité du confinement des porteurs dans les points quantiques sont améliorées, ce qui permet d'obtenir une excellente efficacité de la production de lumière.
PCT/JP2012/063019 2011-05-26 2012-05-22 Dispositif électroluminescent WO2012161179A1 (fr)

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