CN110416420B - Quantum dot light-emitting diode and preparation method thereof - Google Patents
Quantum dot light-emitting diode and preparation method thereof Download PDFInfo
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- CN110416420B CN110416420B CN201810403828.XA CN201810403828A CN110416420B CN 110416420 B CN110416420 B CN 110416420B CN 201810403828 A CN201810403828 A CN 201810403828A CN 110416420 B CN110416420 B CN 110416420B
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- 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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Abstract
The invention provides a quantum dot light-emitting diode which comprises an anode and a cathode which are oppositely arranged, wherein a quantum dot light-emitting layer is arranged between the anode and the cathode, a first functional layer is arranged between the cathode and the quantum dot light-emitting layer, the first functional layer is an electron transmission layer, and the electron transmission layer is made of silicon-doped zinc oxide.
Description
Technical Field
The invention belongs to the technical field of panel display, and particularly relates to a quantum dot light-emitting diode and a preparation method thereof.
Background
Semiconductor quantum dots have size-tunable optoelectronic properties and have been widely used in light emitting diodes, solar cells, and bioluminescent labels. Through the development of quantum dot synthesis technology for more than twenty years, people can synthesize various high-quality nano materials, and the photoluminescence efficiency of the nano materials can reach more than 85%. Because quantum dots have the characteristics of adjustable light emitting size, narrow light emitting line width, high photoluminescence efficiency, thermal stability and the like, quantum dot light emitting diodes (QD-LEDs) taking the quantum dots as light emitting layers are potential next generation display and solid state lighting light sources. Quantum dot light emitting diodes (QLEDs) have gained much attention and research in the field of illumination and display in recent years due to their advantages of high brightness, low power consumption, wide color gamut, and easy processing. Through years of development, the QLED technology has been greatly developed. From the publicly reported literature, the external quantum efficiency of the currently highest red and green QLEDs has exceeded or approached 20%, indicating that the internal quantum efficiency of the red and green QLEDs has actually approached the 100% limit. However, the blue QLED, which is indispensable for high-performance full-color display, is currently much lower than the red-green QLED in both the electro-optical conversion efficiency and the lifetime, thereby limiting the application of the QLED in full-color display.
For the conventional QLED device, the device efficiency has reached the requirement of display technology, but its stability is an important technical defect that restricts its application. Therefore, it is extremely important to improve the stability of the QLED device. One important reason for the stability of QLEDs is short circuit current, which increases the thermal power of the device and affects the stability and efficiency of the device. The main factors causing the large short-circuit current of the device include impurity particles, uneven thin film, uneven ITO electrode and the like.
Disclosure of Invention
The invention aims to provide a quantum dot light-emitting diode and a preparation method thereof, and aims to solve the problem that the existing quantum dot light-emitting diode is poor in stability.
In order to achieve the purpose, the invention adopts the following technical scheme:
the utility model provides a quantum dot emitting diode, includes relative positive pole and the negative pole that sets up, and the positive pole with be provided with quantum dot luminescent layer between the negative pole, the negative pole with be provided with first functional layer between the quantum dot luminescent layer, just first functional layer is electron transport layer, just the material of electron transport layer is silicon-doped zinc oxide.
And, a method for preparing quantum dot light emitting diode, comprising the steps of:
providing a cathode;
preparing a first functional layer on the cathode, wherein the first functional layer is an electron transport layer made of silicon-doped zinc oxide material;
preparing a quantum dot light-emitting layer on the surface of the electron transport layer;
and preparing an anode on the quantum dot light-emitting layer.
According to the quantum dot light-emitting diode provided by the invention, the electron transmission layer made of the silicon-doped zinc oxide material, namely the first functional layer, is arranged between the cathode and the quantum dot light-emitting layer, so that the stability of the device can be improved on the premise of increasing the efficiency and color purity of the device.
Firstly, the first functional layer is introduced, and because the silicon-doped zinc oxide material has lower electron mobility compared with pure ZnO, but for the quantum dot light-emitting diode with the hole transport layer material being organic material, because the hole transport capability of the common organic material is greatly lower than the electron transport capability of the inorganic material, the silicon-doped zinc oxide material with lower electron transport capability can better balance carriers, reduce non-radiative transition, reduce the temperature of the device and improve the stability of the device.
And secondly, the work function of the silicon-doped zinc oxide material is smaller than that of a pure ZnO material, so that the first functional layer can form ohmic contact with an ITO cathode, and the open-circuit voltage is reduced. In addition, by increasing the thickness of the electron transport layer of the silicon-doped zinc oxide material, the short-circuit current caused by the uneven surface of the cathode can be reduced as much as possible, and the stability of the device is further improved.
The preparation method of the quantum dot light-emitting diode provided by the invention only needs to prepare the electron transport layer of the silicon-doped zinc oxide material on the cathode, and then sequentially prepare the quantum dot light-emitting diode and the anode. The method is relatively mature in process, simple and controllable, and beneficial to large-scale production.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present invention more clearly apparent, the present invention is further described in detail below with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
In the description of the present invention, it is to be understood that the terms "first", "second" and the like are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implying any number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
The embodiment of the invention provides a quantum dot light-emitting diode which comprises an anode and a cathode which are oppositely arranged, wherein a quantum dot light-emitting layer is arranged between the anode and the cathode, a first functional layer is arranged between the cathode and the quantum dot light-emitting layer, the first functional layer is an electron transmission layer, and the electron transmission layer is made of silicon-doped zinc oxide.
According to the quantum dot light-emitting diode provided by the embodiment of the invention, the electron transmission layer made of the silicon-doped zinc oxide material, namely the first functional layer, is arranged between the cathode and the quantum dot light-emitting layer, so that the stability of the device can be improved on the premise of increasing the efficiency and the color purity of the device.
Firstly, the first functional layer is introduced, and because the silicon-doped zinc oxide material has lower electron mobility compared with pure ZnO, but for the quantum dot light-emitting diode with the hole transport layer material being organic material, because the hole transport capability of the common organic material is greatly lower than the electron transport capability of the inorganic material, the silicon-doped zinc oxide material with lower electron transport capability can better balance carriers, reduce non-radiative transition, reduce the temperature of the device and improve the stability of the device.
And secondly, the work function of the silicon-doped zinc oxide material is smaller than that of a pure ZnO material, so that the first functional layer can form ohmic contact with an ITO cathode, and the open-circuit voltage is reduced. In addition, by increasing the thickness of the electron transport layer of the silicon-doped zinc oxide material, the short-circuit current caused by the uneven surface of the cathode can be reduced as much as possible, and the stability of the device is further improved.
In the embodiment of the invention, the material of the first functional layer is amorphous ZnmSinThe values of m and n in the O material have large influence on charge transmission. The value range of m is 0.8-0.95, the work function of the formed compound is close to that of ITO when the value range of n is 0.05-0.2, ohmic contact is formed, and the electron mobility which can be in the same order of magnitude as that of the hole injection layer is achieved. When the zinc salt is excessive and the silicon is small, the Zn content in the system is highmSinThe electron mobility of O is high, but the work function of O is also high, so that ohmic contact with ITO is not favorably formed, and the injection barrier is reduced. Conversely, ZnmSinThe resistivity of O is too large to facilitate electron transport.
Preferably, the silicon-doped zinc oxide is ZnmSinAnd O, wherein the value range of m is 0.8-0.95, and the value range of n is 0.05-0.2. Preference is given toThe silicon-doped zinc oxide can better improve the stability of the device.
Further preferably, the thickness of the electron transport layer is 130-280 nm. The embodiment of the invention adds amorphous Zn with the thickness of 130-280nmmSinThe electronic transmission layer of the O material can form an optical microcavity in the quantum dot light-emitting diode, and the optical microcavity structure can increase the luminous intensity of the resonant wavelength, narrow the luminous spectrum, improve the color purity and improve the luminous efficiency of the device.
In the embodiment of the present invention, the thickness of the first functional layer may be further optimized according to a difference in light emission color of the quantum dot light emitting diode, where d is equal to n λ (d is an optical path difference, and λ is an emission wavelength). As an implementation case, the quantum dot light emitting diode is a green quantum dot light emitting diode, and the (Zn)mSinO material) electron transport layer with thickness of 170-250nm can effectively enhance resonance and increase light extraction efficiency. As; in another embodiment, the quantum dot light emitting diode is a blue quantum dot light emitting diode, and the (Zn)mSinO material) electron transport layer with a thickness of 130-220nm can effectively enhance resonance and increase light extraction efficiency. In yet another embodiment, the quantum dot light emitting diode is a red quantum dot light emitting diode, and the (Zn)mSinO material) electron transport layer with thickness of 210-280nm can effectively enhance resonance and increase light extraction efficiency.
In the embodiment of the present invention, in order to better promote hole transport, it is preferable that a second functional layer is disposed between the anode and the quantum dot light emitting layer, and the second functional layer is a hole transport layer. The hole transport layer may be selected from poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine), polyvinylcarbazole, poly (N, N 'bis (4-butylphenyl) -N, N' -bis (phenyl) benzidine), poly (9, 9-dioctylfluorene-CO-bis-N, N-phenyl-1, 4-phenylenediamine), 4', 4 ″ -tris (carbazol-9-yl) triphenylamine, 4' -bis (9-carbazole) biphenyl, but is not limited thereto.
The thickness of the second functional layer is 0-100 nm. Further preferably, the thickness of the second functional layer is 40 to 50 nm. If it is too thin, the conductivity is weaker and a hole-electron imbalance results, the light emitting region may be in the electron transport layer and not in the quantum dot layer; too thick is not conducive to implantation.
In the embodiment of the present invention, the anode may be, but is not limited to, a metal anode, and the cathode may be, but is not limited to, an ITO cathode.
The quantum dots in the quantum dot layer can be at least one of II-VI compound, III-V compound, II-V compound, III-VI compound, IV-VI compound, I-III-VI compound, II-IV-VI compound or IV group single crystal semiconductor compound, at least one of II-VI compound, III-V compound, II-V compound, III-VI compound, IV-VI compound, I-III-VI compound, II-IV-VI compound or IV group binary or multi-element core-shell structure semiconductor compound, or a mixture of single crystal semiconductor compound and core-shell structure semiconductor compound. In the embodiment of the invention, the thickness of the quantum dot light-emitting layer is 10-100 nm.
The quantum dot light-emitting diode provided by the embodiment of the invention can be prepared by the following method.
The embodiment of the invention also provides a preparation method of the quantum dot light-emitting diode, which is characterized by comprising the following steps of:
s01, providing a cathode;
s02, preparing a first functional layer on the cathode, wherein the first functional layer is an electron transport layer made of silicon-doped zinc oxide materials;
s03, sequentially preparing quantum dot light-emitting layers on the surface of the electron transport layer;
and S04, preparing an anode on the quantum dot light-emitting layer.
According to the preparation method of the quantum dot light-emitting diode provided by the embodiment of the invention, only the electron transmission layer made of the silicon-doped zinc oxide material is prepared on the cathode, and then the quantum dot light-emitting diode and the anode are sequentially prepared. The method is relatively mature in process, simple and controllable, and beneficial to large-scale production.
Specifically, in step S01, the cathode is preferably subjected to a cleaning process. As a specific preferred embodiment, the method of the cleaning treatment is: the patterned cathode substrate is subjected to ultrasonic cleaning in sequence in acetone, a washing solution, deionized water and isopropanol, each step of ultrasonic cleaning lasting 10-25m minutes, more preferably 15 minutes. And after the ultrasonic treatment is finished, the cathode is placed in a clean oven to be dried for later use.
In the step S02, a first functional layer is formed on the cathode, and preferably, the silicon-doped zinc oxide is ZnmSinAnd O, wherein the value range of m is 0.8-0.95, and the value range of n is 0.05-0.2. Particularly preferably, the preparation method of the first functional layer comprises the following steps:
providing zinc salt and silicate, mixing the zinc salt and the silicate to form a mixed raw material, taking argon as protective gas and oxygen as working gas, and preparing amorphous Zn through magnetron sputteringmSinAn electron transport layer of O material. The zinc salt and the silicate raw material are sputtered by introducing Ar and O2Depositing on the ITO cathode substrate under the condition of the mixed gas. Wherein, O2And after the mixed raw materials are provided, taking argon as protective gas and oxygen as working gas, and preparing the O element in the silicon-doped zinc oxide mixture by magnetron sputtering. By magnetron sputtering, amorphous Zn can be obtainedmSinAnd (3) O material.
Wherein the zinc salt is at least one selected from zinc sulfate, zinc chloride and zinc nitrate. The molar ratio of the zinc salt to the silicate is m: n is the same as the formula (I).
In step S03, a quantum dot light emitting layer is prepared on the surface of the electron transport layer, and further preferably, after the quantum dot light emitting layer is prepared, a second functional layer is prepared on the quantum dot light emitting layer, where the second functional layer is a hole transport layer.
In step S04, an anode is prepared on the quantum dot light emitting layer by a conventional method.
In the embodiment of the invention, the preparation methods of the quantum dot light-emitting layer and the second functional layer comprise a chemical method and a physical method, wherein the physical method comprises a physical coating method and a solution processing method. Specifically, the chemical method comprises: chemical vapor deposition, continuous ionic layer adsorption and reaction, anodic oxidation, electrolytic deposition, and coprecipitation. The physical coating method comprises the following steps: thermal evaporation coating, electron beam evaporation coating, magnetron sputtering, multi-arc ion coating, physical vapor deposition, atomic layer deposition, pulsed laser deposition, and the like. The solution processing method comprises a spin coating method, a printing method, a dip-coating method, a soaking method, a spraying method, a rolling coating method, a casting method, a slit coating method and a strip coating method. In the embodiment of the invention, a solution processing method is preferably adopted to prepare the uniform and compact interface modification layer.
The following description will be given with reference to specific examples.
Example 1
A preparation method of a quantum dot light-emitting diode comprises the following steps:
s11, placing the patterned ITO substrate in acetone, washing liquor, deionized water and isopropanol in sequence for ultrasonic cleaning, wherein the ultrasonic cleaning of each step lasts for about 15 minutes. And after the ultrasonic treatment is finished, drying the ITO in a clean oven for later use.
S12, after the ITO substrate is dried, depositing a layer of Zn on the ITO substrate by a sputtering methodmSinAn O electron transport layer.
S13, after the upper sheet is cooled to room temperature, QD is deposited on the upper sheet, and the thickness of the layer is 20-40nm without heating. After that, a hole transport layer TFB was deposited with a thickness of 40 nm. After the deposition in this step was completed, the wafer was placed on a heating stage at 100 ℃ and heated for 30 minutes to remove the residual solvent. And finally, placing the sheet on which the functional layers are deposited in an evaporation bin, and thermally evaporating a layer of 100nm metal silver as an anode through a mask plate. And completing the preparation of the device.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (10)
1. The quantum dot light-emitting diode is characterized by comprising an anode and a cathode which are oppositely arranged, wherein a quantum dot light-emitting layer is arranged between the anode and the cathode, a first functional layer is arranged between the cathode and the quantum dot light-emitting layer, the first functional layer is an electron transmission layer, and the electron transmission layer is made of ZnmSinO, wherein the value range of m is 0.8-0.95, the value range of n is 0.05-0.2, the cathode is ITO, and the thickness of the electron transmission layer is 130-280 nm.
2. The quantum dot light-emitting diode of claim 1, wherein the quantum dot light-emitting diode is a green light quantum dot light-emitting diode, and the thickness of the electron transport layer is 170-250 nm.
3. The quantum dot light-emitting diode of claim 1, wherein the quantum dot light-emitting diode is a blue quantum dot light-emitting diode, and the thickness of the electron transport layer is 130-220 nm.
4. The quantum dot light-emitting diode of claim 1, wherein the quantum dot light-emitting diode is a red quantum dot light-emitting diode, and the thickness of the electron transport layer is 210-280 nm.
5. The qd-led of any one of claims 1 to 4, wherein a second functional layer is disposed between the anode and the qd-light emitting layer, and the second functional layer is a hole transport layer.
6. The quantum dot light-emitting diode of claim 5, wherein the thickness of the second functional layer is 0 to 100 nm.
7. The quantum dot light-emitting diode of claim 6, wherein the thickness of the second functional layer is 40-50 nm.
8. A preparation method of a quantum dot light-emitting diode is characterized by comprising the following steps:
providing a cathode, wherein the cathode is ITO;
preparing a first functional layer on the cathode, wherein the first functional layer is an electron transport layer, and the material of the electron transport layer is ZnmSinO, wherein the value range of m is 0.8-0.95, the value range of n is 0.05-0.2, and the thickness of the electron transport layer is 130-280 nm;
preparing a quantum dot light-emitting layer on the surface of the electron transport layer;
and preparing an anode on the quantum dot light-emitting layer.
9. The method of manufacturing a quantum dot light emitting diode according to claim 8, wherein the method of manufacturing the first functional layer comprises:
and (2) providing zinc salt and silicate, mixing the zinc salt and the silicate to form a mixed raw material, taking argon as protective gas and oxygen as working gas, and preparing the electron transport layer of the silicon-doped zinc oxide material by magnetron sputtering.
10. The method of claim 9, wherein the zinc salt is at least one selected from the group consisting of zinc sulfate, zinc chloride, and zinc nitrate.
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| CN114079027B (en) * | 2020-12-31 | 2023-10-31 | 广东聚华印刷显示技术有限公司 | Light emitting device and method of manufacturing the same |
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Non-Patent Citations (3)
| Title |
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| "Electronic transport in highly conducting Si-doped ZnO thin films prepared by pulsed laser deposition";Vladimir L. Kuznetsov, et al;《APPLIED PHYSICS LETTERS》;20151231;第232103-1-232103-5页 * |
| "Enhancing the Performance of Quantum Dot Light-Emitting Diodes Using Room-Temperature-Processed Ga-Doped ZnO Nanoparticles as the Electron Transport Layer";Sheng Cao, et al;《ACS Appl. Mater. Interfaces》;20170419;第15605-15614页 * |
| "Zn1-xMgxO作为电子传输层在量子点发光二极管中的应用";冯丹丹;《中国优秀硕士学位论文全文数据库》;20170315;第31-50页 * |
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