CN110880558A - Alternating current driving perovskite LED device with charge generation layer - Google Patents
Alternating current driving perovskite LED device with charge generation layer Download PDFInfo
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- CN110880558A CN110880558A CN201911200107.XA CN201911200107A CN110880558A CN 110880558 A CN110880558 A CN 110880558A CN 201911200107 A CN201911200107 A CN 201911200107A CN 110880558 A CN110880558 A CN 110880558A
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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
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
- H10K71/15—Deposition of organic active material using liquid deposition, e.g. spin coating characterised by the solvent used
Abstract
The invention relates to an AC driven perovskite LED device with a charge generation layer. The light-emitting diode comprises an anode layer, a first dielectric layer, a first p-n junction type charge generation layer, a light-emitting layer, a second p-n junction type charge generation layer, a second dielectric layer and a cathode layer which are sequentially stacked on a substrate from bottom to top. The luminescent layer is prepared by a solution method, is simple to operate, is suitable for large-scale production, and can greatly reduce the production cost. And the brightness of the perovskite LED can be adjusted by adjusting the frequency under a defined voltage or power; multicolor emission of the device can also be achieved by varying the composition of the perovskite material.
Description
Technical Field
The invention relates to an AC driven perovskite LED device with a charge generation layer.
Background
Perovskite LED is regarded as one of the potential application technologies of next generation display and lighting technology because of its advantages such as narrow light-emitting spectrum, wide color gamut, low preparation cost and high efficiency. Although the External Quantum Efficiency (EQE) of the current near-infrared, red-light and green-light perovskite LEDs exceeds 20%, the EQE of the blue-light perovskite LEDs has also been greatly improved, from the perspective of the device structure, the perovskite LEDs belong to dc-driven devices, and the devices can emit light only when a dc voltage is applied across the devices. However, the power source used in real life is usually 220V, 50Hz alternating current, and in order to make the perovskite LED emit light normally, an ac-dc conversion device is further provided to the device, thereby resulting in complexity of the system. The alternating current driven perovskite LED provided by the invention can directly work in the environment of 220V and 50Hz, and the problems can be effectively solved.
Disclosure of Invention
The invention aims to provide an alternating current driving perovskite LED device with a charge generation layer, and aims to solve the problem that the existing direct current driving perovskite LED cannot directly work in an environment of 220V and 50Hz, and an alternating current-direct current conversion device is required to be configured, so that the complexity of a system is increased.
In order to achieve the purpose, the technical scheme of the invention is as follows: an alternating current driving perovskite LED device with a charge generation layer comprises an anode layer, a first dielectric layer, a first p-n junction type charge generation layer, a light emitting layer, a second p-n junction type charge generation layer, a second dielectric layer and a cathode layer which are sequentially stacked on a substrate from bottom to top.
In one embodiment of the invention, the luminescent layer material is a perovskite quantum dot, a perovskite thin film or a mixed structure of the two; the perovskite quantum dot and the perovskite thin film comprise an ABX3, A4BX6 or AB2X5 structural system, wherein A is an inorganic metal ion, an amine organic group or a mixture of the inorganic metal ion and the amine organic group; b is lead, antimony, manganese, tellurium or tin; the halogen X is any one or more of F, Br, I and Cl.
In an embodiment of the present invention, the light emitting layer is prepared by a solution method or a vacuum evaporation method, and the solution method includes one of a spin coating method, a dip coating method, a blade coating method, a casting method, a screen printing method, a spray coating method, and an inkjet printing method.
In an embodiment of the present invention, the first dielectric layer and the second dielectric layer are made of an insulator or a semiconductor material, and include an inorganic insulator or a semiconductor material and/or an organic insulator or a semiconductor material.
In one embodiment of the present invention, the inorganic insulator or semiconductor material is: a compound of groups IV-IV; III-V compound composed of III elements Al, Ga, In and V elements P, As, Sb; II-VI compound composed of II elements Zn, Cd, Hg and VI elements S, Se and Te; the I-VII compound consists of I group elements Cu, Ag and Au and VII group elements Cl, Br and I; the group V-VI compound consists of group V elements of As, Sb and Bi, and group VI elements of S, Se and Te; oxides of group B and transition elements Cu, Zn, Sc, Ti, V, Cr, Mn, Fe, Co, Ni in the fourth period; one or more compounds formed by rare earth elements Sc, Y, Sm, Eu, Yb and Tm and group V element N, As or group VI element S, Se and Te; the organic insulator or semiconductor material is one or more of naphthalene, anthracene, pentacene type, triphenylamine, fullerene, perylene derivative, polyacetylene type, polyaryl ring type and copolymer type.
In an embodiment of the present invention, a method for depositing the first dielectric layer and the second dielectric layer includes one of chemical vapor deposition, pulsed laser deposition, atomic layer deposition, magnetron sputtering, and anodic oxidation.
In an embodiment of the invention, each of the first p-n junction type charge generation layer and the second p-n junction type charge generation layer includes a p-type charge generation layer and an n-type charge generation layer, wherein the p-type or n-type charge generation layer and the n-type or p-type charge generation layer are stacked on the upper surface and the lower surface of the light emitting layer, respectively.
In an embodiment of the invention, a method for depositing the first p-n junction type charge generation layer and the second p-n junction type charge generation layer includes one of a vacuum evaporation method and a solution method.
In an embodiment of the present invention, the substrate is a rigid substrate or a flexible substrate.
In an embodiment of the present invention, the frequency range of the ac power source is between 1Hz and 20MHz, and the waveform of the ac power source includes one of a sine wave, a triangular wave, a square wave, and a pulse.
Compared with the prior art, the invention has the following beneficial effects:
the luminescent layer is prepared by a solution method, is simple to operate, is suitable for large-scale production, and can greatly reduce the production cost. And the brightness of the perovskite LED can be adjusted by adjusting the frequency at a defined voltage or power. The alternating current driven perovskite LED provided by the invention can directly work in the environments of 220V and 50Hz, and can effectively solve the problem that the existing direct current driven perovskite LED can not directly work in the environments of 220V and 50Hz, and needs to be provided with an alternating current-direct current conversion device, so that the complexity of a system is increased.
Drawings
Fig. 1 is a schematic structural view of an ac-driven perovskite LED provided by an embodiment of the present invention, in which a second n-type charge generation layer and a first p-type charge generation layer are respectively stacked on the upper and lower surfaces of the light emitting layer;
fig. 2 is a schematic structural view of an ac-driven perovskite LED provided in an embodiment of the present invention, in which a second p-type charge generation layer and a first n-type charge generation layer are respectively stacked on the upper and lower surfaces of the light emitting layer.
Detailed Description
The technical scheme of the invention is specifically explained below with reference to the accompanying drawings.
The invention discloses an alternating current driving perovskite LED device with a charge generation layer, which comprises an anode layer, a first dielectric layer, a first p-n junction type charge generation layer, a light emitting layer, a second p-n junction type charge generation layer, a second dielectric layer and a cathode layer which are sequentially stacked on a substrate from bottom to top.
The following is a specific implementation of the present invention.
Referring to fig. 1 and 2, which are cross-sectional views illustrating an embodiment of an ac-driven perovskite LED device having a charge generation layer according to the present invention, the embodiment provides a perovskite LED device including an anode layer 101, a first dielectric layer 102, a first p-n junction type charge generation layer 13, a light emitting layer 104, a second p-n junction type charge generation layer 15, a second dielectric layer 112, and a cathode layer 106, and the functional layers are sequentially stacked in the stated order on a substrate. The following detailed description of the embodiments will be made with reference to the accompanying drawings. The example provides a deposition sequence for such a perovskite LED device of depositing a transparent conductive anode 101 on a glass substrate 100, depositing a first dielectric layer 102 on the transparent conductive anode 101, depositing a first p-n junction type charge generation layer 13 on the first dielectric layer 102, depositing a light emitting layer 104 on the first p-n junction type charge generation layer 13, depositing a second p-n junction type charge generation layer 15 on the light emitting layer 104, and then depositing a second dielectric layer 112 and a cathode layer 106 on the second p-n junction type charge generation layer 15.
Wherein the first p-n junction type charge generation layer 13 and the second p-n junction type charge generation layer 15 each comprise a p-type charge generation layer 113/115 and an n-type charge generation layer 103/105 which are stacked, and the p (or n) -type charge generation layer and the n (or p) -type charge generation layer are stacked on the upper and lower surfaces of the quantum dot light emitting layer 104, respectively.
The preparation method of the alternating current driven perovskite LED device specifically comprises the following steps:
firstly, an anode substrate is provided, the anode material adopts an ITO conductive film prepared by magnetron sputtering, and the substrate needs to be cleaned before a first dielectric layer 102 is deposited on the anode substrate, and the specific process comprises the following steps: and respectively putting the substrate into a glass cleaning agent, deionized water, acetone and ethanol in sequence for ultrasonic treatment, wherein the ultrasonic time of each step is 15min, and putting the substrate into an oven for drying after ultrasonic cleaning.
Secondly, a first dielectric layer 102 is deposited on the cleaned anode substrate by adopting a magnetron sputtering method, the dielectric layer 102 is a metal oxide hafnium oxide prepared by adopting a magnetron sputtering method, the dielectric layer belongs to an insulating material, the dielectric constant is 25, the light transmittance and the film forming property are good, and the thickness is 30-50 nm.
Then, the first p-n junction type charge generation layer 13 is deposited on the first dielectric layer 102 using a solution method including, but not limited to, spin coating, dip coating, doctor blading, casting, spray coating, screen printing, inkjet printing, or vacuum evaporation. The p-n junction type charge generation layer 13/15 includes a p-type charge generation layer 113/115 and an n-type charge generation layer 103/105 stacked one on another, and the p-type charge generation layer may use a p-type doped hole transport material, that is, a p-type dopant and a hole transport material are mixed. PEDOT was chosen as the p-type charge generation layer material in this example. The n-type charge generation layer material is a doped n-type electron transport material. TPBi is selected as the n-type charge generation layer material in this example. The thickness of the p-type charge generation layer and the thickness of the n-type charge generation layer are both in the range of 30-50 nm. Depending on the specific location of the p-n junction type charge generation layer, two cases can be distinguished: the first is to laminate a second n-type charge generation layer 105 and a first p-type charge generation layer 113 on the upper and lower surfaces of the light-emitting layer 104; a second p-type charge generation layer 115 and a first n-type charge generation layer 103 are deposited on the upper surface of the second n-type charge generation layer 105 and the lower surface of the first p-type charge generation layer 113, respectively, as shown in fig. 1. The second is to laminate a second p-type charge generation layer 115 and a first n-type charge generation layer 103 on the upper and lower surfaces of the light emitting layer 104; a second n-type charge generation layer 105 and a first p-type charge generation layer 113 are deposited on the upper surface of the second p-type charge generation layer 115 and the lower surface of the first n-type charge generation layer 103, respectively, as shown in fig. 2.
Then, a layer of perovskite quantum dot solution synthesized by a high-temperature injection method is deposited on the first p-n junction type charge generation layer 13 by a solution method or a vacuum evaporation method, the perovskite quantum dot has the specific structural formula of CsPbBr3, and the concentration is 20mg/ml, so that the perovskite LED device manufactured in the embodiment can emit bright green light under the driving of alternating voltage.
The preparation method of the perovskite quantum dot solution comprises the following steps: a precursor solution was first synthesized by charging Cs2CO3 (0.814 g) into a 100mL four-necked flask along with octadecene (ODE, 40 mL) and oleic acid (2.5 mL, OA). Dried at 120 ℃ for 1 hour and then heated to 150 ℃ under N2 until all Cs2CO3 reacted with OA. ODE (5 mL), PbBr2 (0.188 mmol), oleylamine (0.5 mL, OLA) and OA (0.5 mL) were then charged into a 100mL four-necked flask and dried under vacuum at 120 ℃ for 1 hour. After complete dissolution of the PbX2 salt, the temperature was raised to 160 ℃ and the precursor solution (0.4 mL) was injected rapidly, after 5s, the reaction mixture was cooled with an ice-water bath. Finally, the crude solution was cooled in a water bath, and then centrifuged after adding ethyl acetate at a volume ratio of 1: 3. The supernatant was discarded, and the precipitate was dispersed in hexane, followed by addition of ethyl acetate at a volume ratio of 1:3, centrifugation, and dissolution of the precipitate in octane to form a stable colloidal solution.
Next, a second p-n junction type charge generation layer 15 is deposited on the light emitting layer 104.
Next, a second dielectric layer 112 is deposited over the second p-n junction charge generation layer 15. Finally, a cathode layer 106 is deposited on the second dielectric layer 112, wherein the cathode layer 106 is made of Al/LiF prepared by vacuum evaporation, the thickness of Al is 150nm, the thickness of LiF is 1nm, and the vacuum vapor pressure is 1.8 × 10-6 torr.
Due to the existence of the dielectric layer, the charge injection of the electrode is blocked, and the device does not use the carriers injected by an external circuit to compound and emit light, so a p-n junction type charge generation layer is needed to provide new carriers. If the voltage connected with the cathode is positive and the voltage connected with the anode is negative, the first p-n junction type charge generation layer and the second p-n junction type charge generation layer can generate a large number of electrons and holes under the action of an electric field, the electrons generated by the second p-n junction type charge generation layer move to the cathode under the action of the electric field, the movement process is hindered by the second dielectric layer, the electrons are remained between the second dielectric layer and the second n-type charge generation layer, and the holes generated by the electrons move to the anode along the direction of the electric field and finally reach the valence band of the perovskite quantum dots in the light emitting layer. In a similar way, holes generated by the first P-n junction type charge generation layer move to the anode under the action of an electric field, the movement process is hindered by the first dielectric layer and finally stays between the first dielectric layer and the first P-type charge generation layer, and electrons generated by the holes move to the cathode under the action of the electric field and reach a conduction band of perovskite quantum dots in the light emitting layer. So that the holes reaching the valence band and the electrons reaching the conduction band emit light by radiative recombination. According to the above analysis, a similar phenomenon can be obtained when the voltage applied to the cathode is negative and the voltage applied to the anode is positive.
The luminescent layer is prepared by a solution method, is simple to operate, is suitable for large-scale production, and can reduce the production cost to a certain extent. By varying the composition of the perovskite material, multiple colors of light emission from the device can be achieved. And under a certain voltage or power, the brightness of the perovskite LED can be adjusted by adjusting the frequency. Due to the continuous change of the direction of the external electric field, the alternating current driven perovskite LED device can effectively avoid the charge accumulation phenomenon. And the dielectric layer can effectively avoid electrochemical reaction between the organic layer and the cathode and the anode, thereby protecting the perovskite LED device from the influence of moisture and oxygen in the atmosphere.
The above are preferred embodiments of the present invention, and all changes made according to the technical scheme of the present invention that produce functional effects do not exceed the scope of the technical scheme of the present invention belong to the protection scope of the present invention.
Claims (10)
1. An alternating current driving perovskite LED device with a charge generation layer is characterized by comprising an anode layer, a first dielectric layer, a first p-n junction type charge generation layer, a light emitting layer, a second p-n junction type charge generation layer, a second dielectric layer and a cathode layer which are sequentially stacked on a substrate from bottom to top.
2. An ac driven perovskite LED device with a charge generation layer as claimed in claim 1 wherein the light emitting layer material is a hybrid structure of one or both of perovskite quantum dots, perovskite thin films; the perovskite quantum dot and the perovskite thin film comprise an ABX3, A4BX6 or AB2X5 structural system, wherein A is an inorganic metal ion, an amine organic group or a mixture of the inorganic metal ion and the amine organic group; b is lead, antimony, manganese, tellurium or tin; the halogen X is any one or more of F, Br, I and Cl.
3. The ac-driven perovskite LED device with the charge generation layer as claimed in claim 1, wherein the light emitting layer is prepared by a solution method or a vacuum evaporation method, the solution method comprising one of spin coating, dip coating, doctor blading, casting, screen printing, spray coating, and inkjet printing.
4. An ac driven perovskite LED device with a charge generation layer according to claim 1, wherein the first dielectric layer, the second dielectric layer is made of an insulator or a semiconductor material, including an inorganic insulator or semiconductor material and/or an organic insulator or semiconductor material.
5. An ac driven perovskite LED device with a charge generation layer according to claim 4 wherein the inorganic insulator or semiconductor material is: a compound of groups IV-IV; III-V compound composed of III elements Al, Ga, In and V elements P, As, Sb; II-VI compound composed of II elements Zn, Cd, Hg and VI elements S, Se and Te; the I-VII compound consists of I group elements Cu, Ag and Au and VII group elements Cl, Br and I; the group V-VI compound consists of group V elements of As, Sb and Bi, and group VI elements of S, Se and Te; oxides of group B and transition elements Cu, Zn, Sc, Ti, V, Cr, Mn, Fe, Co, Ni in the fourth period; one or more compounds formed by rare earth elements Sc, Y, Sm, Eu, Yb and Tm and group V element N, As or group VI element S, Se and Te; the organic insulator or semiconductor material is one or more of naphthalene, anthracene, pentacene type, triphenylamine, fullerene, perylene derivative, polyacetylene type, polyaryl ring type and copolymer type.
6. An ac driven perovskite LED device with a charge generation layer as claimed in claim 1 wherein the method of depositing the first and second dielectric layers is one of chemical vapor deposition, pulsed laser deposition, atomic layer deposition, magnetron sputtering, anodic oxidation.
7. An ac-driven perovskite LED device with a charge generation layer as set forth in claim 1, wherein the first p-n junction type charge generation layer and the second p-n junction type charge generation layer each comprise a p-type charge generation layer and an n-type charge generation layer, and wherein the p-type or n-type charge generation layer and the n-type or p-type charge generation layer are respectively stacked on the upper and lower surfaces of the light emitting layer.
8. An ac driven perovskite LED device with a charge generation layer as claimed in claim 1 wherein the method of depositing the first and second p-n junction type charge generation layers is one of vacuum evaporation and solution.
9. An ac driven perovskite LED device with a charge generation layer as claimed in claim 1 wherein the substrate base is a rigid substrate base or a flexible substrate base.
10. An ac driven perovskite LED device with a charge generation layer as claimed in claim 1 wherein the frequency of the ac power source is in the range of 1Hz-20MHz and the waveform of the ac power source is one of a sine wave, a triangular wave, a square wave, and a pulse.
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| CN105161629A (en) * | 2015-08-18 | 2015-12-16 | Tcl集团股份有限公司 | Alternating-current drive quantum dot light-emitting diode (QLED) and preparation method thereof |
| CN105244450A (en) * | 2015-10-09 | 2016-01-13 | 北京大学深圳研究生院 | Organic light-emitting device driven by alternating electric field and preparation method for organic light-emitting device |
| CN107768527A (en) * | 2017-08-02 | 2018-03-06 | 武汉华美晨曦光电有限责任公司 | A kind of small molecule OLED surface luminescent device of AC power driving |
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- 2019-11-29 CN CN201911200107.XA patent/CN110880558A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105161629A (en) * | 2015-08-18 | 2015-12-16 | Tcl集团股份有限公司 | Alternating-current drive quantum dot light-emitting diode (QLED) and preparation method thereof |
| CN105244450A (en) * | 2015-10-09 | 2016-01-13 | 北京大学深圳研究生院 | Organic light-emitting device driven by alternating electric field and preparation method for organic light-emitting device |
| CN107768527A (en) * | 2017-08-02 | 2018-03-06 | 武汉华美晨曦光电有限责任公司 | A kind of small molecule OLED surface luminescent device of AC power driving |
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