CN105609651A - High-efficiency quantum dot light emitting diode with self-assembly polymer hole transmission layer structure - Google Patents
High-efficiency quantum dot light emitting diode with self-assembly polymer hole transmission layer structure Download PDFInfo
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- CN105609651A CN105609651A CN201610008669.4A CN201610008669A CN105609651A CN 105609651 A CN105609651 A CN 105609651A CN 201610008669 A CN201610008669 A CN 201610008669A CN 105609651 A CN105609651 A CN 105609651A
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—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
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/14—Carrier transporting layers
- H10K50/15—Hole transporting layers
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/14—Carrier transporting layers
- H10K50/16—Electron transporting layers
Abstract
The invention discloses and proposes a high-efficiency quantum dot light emitting diode with a self-assembly polymer hole transmission layer structure. Except a positive electrode and a negative electrode, the high-efficiency quantum dot light emitting diode comprises a three-layer structure: a hole transmission layer, a quantum dot light emitting layer and an electron transmission layer, wherein one end of the quantum dot light emitting layer is connected with the hole transmission layer, the other end of the quantum dot light emitting layer is connected with the electron transmission layer, the electron transmission layer is organic nanoparticles after doped, the hole transmission layer is formed by doping a monomer, a polymer, small-molecule, inorganic oxidized metal nanoparticles or a two-dimensional nanometer material into poly(3,4- ethylenedioxythiophene monomer), a quantum dot is quantum dots of zinc sulfide, zinc selenide, cadmium sulfide, cadmium selenide, cadmium telluride, mercury sulfide, mercury selenide, mercury telluride or core-shell nanometer structured cadmium selenide-zinc sulfide, cadmium sulfide-zinc sulfide, cadmium sulfide-zinc selenide and graphene thereof and the like, and the negative electrode is glass or polyethylene terephthalate (PET) with a layer of indium tin oxide (ITO) or fluorine-doped tin oxide (FTO) or graphene.
Description
Technical field
The invention belongs to light emitting diode with quantum dots devices field, be specifically related to a kind of self-assembling polymers hole buffering transmission layer three-decker highly effective quantum point luminescent diode.
Background technology
The colloid inorganic-quantum-dot of accurately controlling form and composition has unique chemical physical property and is applied to the devices such as luminescent device, solar cell, photo-detector. Although quantum dot is synthetic and the improvement of device architecture, operational version processing type colloid is piled up to make high performance solid-state devices and is still had difficulties.
Individual layer and double-deck light emitting diode with quantum dots (QLEDs) in many reports, are mentioned. Utilize the actual performance of the individual layer light emitting diode with quantum dots of the function monofilm that has simultaneously mixed transmission and transmitting to can not show a candle to theoretical calculated value. Double-deck light emitting diode with quantum dots performance is better than the light emitting diode with quantum dots of individual layer, but Double Quantum Dots light emitting diode will be brought into play quantum dot layer the function of utilizing emitted light sublayer and electron transfer layer simultaneously. The adjacent efficiency that hinders photo emissions of quantum dot layer and electronics. Not long ago, researchers have invented three layers of light emitting diode with quantum dots device that have independent hole transmission layer and electron transfer layer. Although the luminous efficiency of the light emitting diode with quantum dots that the luminous efficiency of three layers of light emitting diode with quantum dots is mentioned before comparing has improved 25 times, show color saturation and the external quantum efficiency aspect of three layers of light emitting diode with quantum dots still cannot reach basic requirement. Chief reason be hole transmission layer inject the low and quantum dot light emitting layer of the efficiency of quantum dot layer and and hole transmission layer between huge energy offset. Multilayer device is suggested and overcomes the obstruction that hole is injected. Most of multi-layer quantum point LED device is at hole injection efficiency, external quantum efficiency, and the performance of low driving voltage and high brightness aspect is very remarkable.
It is worth mentioning that, the external quantum efficiency that multi-layer quantum point luminescent diode glows the recently limiting value 21% of approximation theory reaches 19%, and the low driving voltage of these devices and high brightness are given the credit to the injection balance of carrier. But from thermodynamics, the transport layer of these multilayers can affect life-span and the bearing power of device at device.
Summary of the invention
Goal of the invention: the highly effective quantum point luminescent diode that the object of this invention is to provide a kind of self-assembling polymers hole transmission layer three-decker that can improve light emitting diode with quantum dots efficiency.
Technical scheme: to achieve these goals, the technical solution used in the present invention is:
A kind of highly effective quantum point luminescent diode of self-assembling polymers hole transmission layer structure, except anode and negative electrode, only need trilaminate material, respectively hole transmission layer, quantum dot light emitting layer and electron transfer layer, described quantum dot light emitting layer one end joins with the hole transmission layer that is being connected anode, the other end is connected with the electron transfer layer that is being connected negative electrode, and the material of described hole transmission layer is single polymers or polymer material.
As preferably, described electric transmission layer material is the inorganic nanoparticles after doping.
As preferably, described hole transport layer material is material doped poly-(3,4-ethylene dioxythiophene monomer) composition that enters of single polymers, polymer, little molecule, inorganic oxide metal nanoparticle or two-dimensional nano, and both part by weight that adulterates are 0 ~ 20%.
As preferably, the quantum dot of described quantum dot layer is the quantum dot being made up of II-VI family element, or it forms core-shell nano structure quantum point, or graphene quantum dot, or the combination of calcium halide titanium ore organic metal quantum dot or above material; The described quantum dot being made up of II-VI family element comprises zinc sulphide, zinc selenide, zinc telluridse, cadmium sulfide, cadmium selenide, cadmium telluride, mercuric sulphide, mercury selenide, tellurium mercury, one or more in vulcanized lead or lead selenide; The quantum dot of described core-shell nano structure, comprises cadmium selenide-zinc sulphide, one or more in cadmium sulfide-zinc sulphide or zinc selenide-cadmium sulfide.
As preferably, the diameter of the inorganic nanoparticles after the doping of described electron transfer layer and the quanta point material of quantum dot light emitting layer is less than 10 nanometers.
As preferably, described hole transport bed thickness 10-30nm, quantum dot light emitting bed thickness 20-40nm, electric transmission bed thickness 30-70nm.
In concrete embodiment, the material of described electron transfer layer is the titanium dioxide not mixing, zinc oxide or combined dopants comprise calcium, cadmium, gadolinium, germanium, caesium, copper, nickel, silver, aluminium, lithium, gold, indium, three oxidation two tantalums, tin oxide, tungsten oxide, zinc selenide, cadmium sulfide or zinc sulphide are at interior metal or nonmetallic nano particle.
In concrete embodiment, the dopant material in described electric transmission layer material is rare metal terbium, dysprosium, thulium, erbium, europium or its combination.
In concrete embodiment, described inorganic oxide metal nanoparticle is made up of P type zinc oxide, and the material of doping is P type gallium nitride, nickel oxide, chrome green, molybdenum bisuphide, manganese trioxide, bismuth oxide or its combination; Described single polymers or polymer material are: poly-(3,4-ethylene dioxythiophene monomer) (PEDOT:PSS), gathers (N-VCz) (PVK), poly-(N, N'-diphenyl-N, N'-bis-(tolyl) benzidine) (poly-TPD), 4-azido-2,3,5,6-tetrafluorobenzoic aid N-succinimide ester (TFB), gathers (to phenylene vinylidene) (PPV), perfluor ionomer (PFIs), or its combination; Described little molecule is: 4,4 '-N, N '-carbazole) biphenyl (CBP), N, N'-is (1-naphthyl partially; )-N, N'-biphenyl-1,1'-biphenyl-4,4'-diamine (α-NPD), 4,40,400-tri-(N-carbazyl) triphenylamine (TCTA) or its combination; Described two-dimensional nano material is: pure Graphene (G), graphene oxide (GO), redox Graphene (RGO), cobalt sulfide (CoS) or its combination.
The preparation method of above-mentioned light emitting diode with quantum dots: adopt spin coating, revolve film, drop-coating, ink-jet method or its are used in combination prepares hole transmission layer, quantum dot light emitting layer and electron transfer layer.
Beneficial effect: compared with prior art, tool of the present invention has the following advantages:
(1) be applied in light emitting diode with quantum dots by self-assembling polymers hole transmission layer, between hole transmission layer and quantum dot layer, produce the strong injected hole of efficient electrical potential difference and control the injection of equilbrium carrier, make light emitting diode with quantum dots obtain higher efficiency. Meanwhile, select the compound of two kinds of cavitation layer materials, not only can improve hole mobility, and two kinds of energy bands formation energy level ladders, contribute to accelerate the transfer rate of hole in hole transmission layer, improve the efficiency of light emitting diode with quantum dots.
(2) production method can adopt spin coating, the method for printing or sputter, and preparation method is simple, has superiority especially in the time preparing the film of large-area high-quality.
Brief description of the drawings
Fig. 1 is forward bias self-assembling polymers hole transmission layer structure high-efficiency quantum dot light emitting diode construction schematic diagram, wherein: 1-negative electrode, 2-hole transmission layer, 3-quantum dot light emitting layer, 4-electron transfer layer, 5-anode.
Fig. 2 is reverse biased self-assembling polymers hole transmission layer structure high-efficiency quantum dot light emitting diode construction schematic diagram, wherein: 1-negative electrode, 2-electron transfer layer, 3-quantum dot light emitting layer, 4-hole transmission layer, 5-anode.
Detailed description of the invention
Below in conjunction with the drawings and specific embodiments, further illustrate the present invention. Should understand these embodiment and only be not used in and limit the scope of the invention for the present invention is described, after having read the present invention, those skilled in the art all fall within the application's claims limited range to the amendment of the various equivalent form of values of the present invention.
Embodiment 1:
The highly effective quantum point luminescent diode of forward formula self-assembling polymers cavitation layer, as shown in Figure 1, comprise the negative electrode 1, the hole transmission layer 2 that in substrate, form, quantum dot light emitting layer 3, electron transfer layer 4 and anode electrode 5, negative electrode is placed in bottom, is respectively hole transmission layer from the bottom to top, quantum dot light emitting layer, electron transfer layer and anode, wherein hole transport bed thickness 10nm, quantum dot light emitting bed thickness 20nm, electric transmission bed thickness 30nm.
The preparation method of the highly effective quantum point luminescent diode of above-mentioned forward formula self-assembling polymers cavitation layer, comprises the steps:
(1) on transparent conducting glass substrate, adopt ink-jet method to prepare hole transmission layer perfluor ionomer PFIs doping poly-3,4-ethylenedioxy thiophene monomer PEDOT:PSS, perfluor ionomer PFIs mass fraction is 10%, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(2) preparation of quantum dot: adopt and revolve quantum dot layer prepared by embrane method, core is cadmium selenide, and shell is zinc sulphide, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(3) the ZnO nano stratum granulosum of indium doping is prepared on quantum dot layer, by inorganic nanoparticles luminescent layer sintering 20 minutes in oxygen, 200 DEG C of sintering temperatures.
(4) finally prepare anode electrode, electrode material is aluminium.
Embodiment 2
The highly effective quantum point luminescent diode of inverse type self-assembling polymers cavitation layer, as shown in Figure 2, comprise the anode 1, the electron transfer layer 2 that in substrate, form, quantum dot light emitting layer 3, hole transmission layer 4 and cathode electrode 5, anode is placed in bottom, is respectively electron transfer layer from the bottom to top, quantum dot light emitting layer, hole transmission layer and negative electrode, wherein electric transmission bed thickness 50nm, quantum dot light emitting bed thickness 30nm, hole transport bed thickness 20nm.
The preparation method of the highly effective quantum point luminescent diode of above-mentioned inverse type self-assembling polymers cavitation layer, comprises the steps:
(1) by the TiO of calcium doping2Nano-particle layer is prepared on anode electrode Al, by inorganic nanoparticles luminescent layer sintering 20 minutes in oxygen, 200 DEG C of sintering temperatures.
(2) preparation of quantum dot: adopt the quantum dot layer prepared of ink-jet method, core is cadmium selenide, and shell is zinc sulphide, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(3) on quantum dot layer, adopt ink-jet method to prepare the poly-3,4-ethylene dioxythiophene monomer PEDOT:PSS of hole transmission layer perfluor ionomer PFIs doping, perfluor ionomer PFIs mass fraction is 5%, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(4) finally prepare cathode electrode, electrode material is ITO.
Embodiment 3
The highly effective quantum point luminescent diode of forward formula self-assembling polymers cavitation layer, as shown in Figure 1, comprise the negative electrode 1, the hole transmission layer 2 that in substrate, form, quantum dot light emitting layer 3, electron transfer layer 4 and anode electrode 5, negative electrode is placed in bottom, is respectively hole transmission layer from the bottom to top, quantum dot light emitting layer, electron transfer layer and anode, wherein hole transport bed thickness 30nm, quantum dot light emitting bed thickness 40nm, electric transmission bed thickness 70nm.
The preparation method of the highly effective quantum point luminescent diode of above-mentioned forward formula self-assembling polymers cavitation layer, comprises the steps:
(1) on transparent conducting glass substrate, adopt ink-jet method to prepare hole transmission layer poly (phenylenevinylene) PPV doping poly-3,4-ethylenedioxy thiophene monomer PEDOT:PSS, be 5% to phenylene vinylidene PPV mass fraction, prepare hole transmission layer, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(2) preparation of quantum dot: adopt spin-coating method to prepare quantum dot layer, it consists of calcium halide titanium ore organic metal quantum dot particle, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent. .
(3) by the TiO of gadolinium doping2Nano-particle layer is prepared on quantum dot layer, by inorganic nanoparticles luminescent layer sintering 20 minutes in oxygen, 200 DEG C of sintering temperatures.
(4) finally prepare anode electrode, electrode material is gold, aluminium, silver etc.
Embodiment 4
The highly effective quantum point luminescent diode of inverse type self-assembling polymers cavitation layer, as shown in Figure 2, comprise the anode 1, the electron transfer layer 2 that in substrate, form, quantum dot light emitting layer 3, hole transmission layer 4 and cathode electrode 5, anode is placed in bottom, is respectively electron transfer layer from the bottom to top, quantum dot light emitting layer, hole transmission layer and negative electrode, wherein electric transmission bed thickness 50nm, quantum dot light emitting bed thickness 30nm, hole transport bed thickness 20nm.
The preparation method of the highly effective quantum point luminescent diode of above-mentioned inverse type self-assembling polymers cavitation layer, comprises the steps:
(1) by the TiO of nickel doping2Nano-particle layer is prepared on anode electrode gold, by inorganic nanoparticles luminescent layer sintering 20 minutes in oxygen, 200 DEG C of sintering temperatures.
(2) preparation of quantum dot: adopt spin-coating method to prepare graphene quantum dot layer, its composition particle size is less than 10 nanometers, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(3) on graphene quantum dot layer, prepare hole transmission layer, it consists of the poly-3,4-ethylene dioxythiophene monomer PEDOT:PSS of P type manganese trioxide doping, and P type manganese trioxide mass fraction is 8%, and under nitrogen environment sintering 20 minutes, sintering temperature 150 is spent.
(4) finally prepare cathode electrode, electrode material is glass or the PET of ITO or FTO or Graphene.
The material that some typical hole transmission layers, quantum dot light emitting layer and electron transfer layer use of just having given an example in the three-decker of the highly effective quantum point luminescent diode in above-described embodiment, other material that its structure and preparation method are equally applicable to mention in technical solution of the present invention, does not enumerate at this.
Claims (10)
1. the highly effective quantum point luminescent diode of a self-assembling polymers hole transmission layer structure, it is characterized in that: described diode is except anode and negative electrode, only need trilaminate material, respectively hole transmission layer, quantum dot light emitting layer and electron transfer layer, described quantum dot light emitting layer one end joins with the hole transmission layer that is being connected anode, the other end is connected with the electron transfer layer that is being connected negative electrode, and the material of described hole transmission layer is single polymers or polymer material.
2. light emitting diode with quantum dots according to claim 1, is characterized in that, described electric transmission layer material is the inorganic nanoparticles after doping.
3. light emitting diode with quantum dots according to claim 1; it is characterized in that; to be that single polymers, polymer, little molecule, inorganic oxide metal nanoparticle or two-dimensional nano are material doped enter poly-(3 to described hole transport layer material; 4-ethylenedioxy thiophene monomer) composition, both part by weight that adulterates are 0 ~ 20%.
4. light emitting diode with quantum dots according to claim 1, it is characterized in that, the quantum dot of described quantum dot layer is the quantum dot being made up of II-VI family element, or it forms core-shell nano structure quantum point, or graphene quantum dot, or the combination of calcium halide titanium ore organic metal quantum dot or above material; The described quantum dot being made up of II-VI family element comprises zinc sulphide, zinc selenide, zinc telluridse, cadmium sulfide, cadmium selenide, cadmium telluride, mercuric sulphide, one or more in mercury selenide or tellurium mercury; The quantum dot of described core-shell nano structure, comprises cadmium selenide-zinc sulphide, one or more in cadmium sulfide-zinc sulphide or zinc selenide-cadmium sulfide.
5. light emitting diode with quantum dots according to claim 2, is characterized in that, the material of described electron transfer layer is the titanium dioxide not mixing, zinc oxide or combined dopants comprise calcium, cadmium, gadolinium, germanium, caesium, copper, nickel, silver, aluminium, lithium, gold, indium, three oxidation two tantalums, tin oxide, tungsten oxide, zinc selenide, cadmium sulfide or zinc sulphide are at interior metal or nonmetallic nano particle.
6. light emitting diode with quantum dots according to claim 2, is characterized in that, the dopant material in described electric transmission layer material is rare metal terbium, dysprosium, thulium, erbium, europium or its combination.
7. light emitting diode with quantum dots according to claim 2, is characterized in that, the diameter of the inorganic nanoparticles after the doping of described electron transfer layer and the quanta point material of quantum dot light emitting layer is less than 10 nanometers.
8. light emitting diode with quantum dots according to claim 3, is characterized in that, described inorganic oxide metal nanoparticle is made up of P type zinc oxide, the material of doping is P type gallium nitride, nickel oxide, chrome green, molybdenum bisuphide, manganese trioxide, bismuth oxide or its combination; Described single polymers or polymer material are: poly-3,4-ethylene dioxythiophene monomer PEDOT:PSS, poly N-vinyl carbazole PVK, poly-N, N'-diphenyl-N, bis-tolyl benzidine poly-TPD of N'-, 4-azido-2,3,5,6-tetrafluorobenzoic aid N-succinimide ester TFB, poly (phenylenevinylene) PPV, perfluor ionomer PFIs, or its combination; Described little molecule is: 4,4 '-N, N '-carbazole biphenyl CBP, N, the inclined to one side 1-naphthyl of N'-;-N, N'-biphenyl-1,1'-biphenyl-4,4'-diamine α-NPD, three N-carbazyl triphenylamine TCTA or its combinations; Described two-dimensional nano material is: pure Graphene, graphene oxide GO, redox Graphene RGO, cobalt sulfide CoS or its combination.
9. according to the light emitting diode with quantum dots described in claim 1-8 any one, it is characterized in that described hole transport bed thickness 10-30nm, quantum dot light emitting bed thickness 20-40nm, electric transmission bed thickness 30-70nm.
10. according to the preparation method of the light emitting diode with quantum dots described in claim 1-8 any one, it is characterized in that, adopt spin coating, revolve film, drop-coating, ink-jet method or its are used in combination prepares hole transmission layer, quantum dot light emitting layer and electron transfer layer.
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