CN112750959A - Composite electrode, preparation method thereof and electroluminescent device - Google Patents
Composite electrode, preparation method thereof and electroluminescent device Download PDFInfo
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- CN112750959A CN112750959A CN202010216578.6A CN202010216578A CN112750959A CN 112750959 A CN112750959 A CN 112750959A CN 202010216578 A CN202010216578 A CN 202010216578A CN 112750959 A CN112750959 A CN 112750959A
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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
- H10K50/80—Constructional details
- H10K50/805—Electrodes
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/80—Constructional details
- H10K50/85—Arrangements for extracting light from the devices
- H10K50/852—Arrangements for extracting light from the devices comprising a resonant cavity structure, e.g. Bragg reflector pair
-
- 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
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- Physics & Mathematics (AREA)
- Optics & Photonics (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Electroluminescent Light Sources (AREA)
Abstract
The invention relates to a composite electrode, a preparation method thereof and an electroluminescent device. The composite electrode comprises a laminated metal layer and a graphene layer, wherein the metal layer is transparent and has a micro-nano structure on the surface. According to the composite electrode adopting the technical scheme, the micro-nano structure is arranged on the surface of the metal layer, so that plasma exists, when light emitted by the electroluminescent device passes through the metal layer, surface plasma resonance is easy to occur, and the emergent light is enhanced. And electron transfer can occur between the metal layer and the graphene layer, the free electron concentration on the surface of the metal can be changed, and the free electron concentration can influence the frequency of surface plasma resonance, so that the light-emitting peak position of the light-emitting device can be finely adjusted. In general, the free electron concentration of the metal surface is increased, and the resonance peak position of surface plasma is blue-shifted; the free electron concentration of the metal surface is reduced, and the resonance peak position of the surface plasma is red-shifted.
Description
Technical Field
The invention relates to the technical field of devices, in particular to a composite electrode, a preparation method of the composite electrode and an electroluminescent device.
Background
The emergence and development of new light emitting devices, represented by Organic Light Emitting Diodes (OLEDs) and quantum dot light emitting diodes (QLEDs), has brought tremendous innovation in display and lighting technologies. The OLED and QLED devices have similar structures and similar light emitting principles, and simply require electrons and holes to move from the cathode and anode to the light emitting layer respectively and to undergo radiative recombination to emit photons. Therefore, different luminescent materials are required to obtain different luminescent colors. Although the light-emitting wavelength of the material can be regulated by synthesis, the regulation cannot be fine; on the other hand, although the emission of the material is tunable, it does not mean that the material of any emission wavelength has equally excellent stability and emission efficiency. Therefore, from the viewpoint of product and application scenarios, it is very valuable to fine-tune the color of the light emitting device to achieve better results.
Disclosure of Invention
In view of the above, it is necessary to provide a composite electrode capable of achieving color trimming of a light emitting device, a method for manufacturing the composite electrode, and an electroluminescent device, in order to solve the problem of how to achieve color trimming of the light emitting device.
A composite electrode comprises a metal layer and a graphene layer which are laminated, wherein the metal layer is transparent, and the surface of the metal layer is provided with a micro-nano structure.
According to the composite electrode adopting the technical scheme, the micro-nano structure is arranged on the surface of the metal layer, so that plasma exists, when light emitted by the electroluminescent device passes through the metal layer, surface plasma resonance is easy to occur, and the emergent light is enhanced. And electron transfer can occur between the metal layer and the graphene layer, the free electron concentration on the surface of the metal layer can be changed, and the free electron concentration can influence the frequency of surface plasma resonance, so that the light-emitting peak position of the light-emitting device can be finely adjusted. In general, the free electron concentration of the metal surface is increased, and the resonance peak position of surface plasma is blue-shifted; the free electron concentration of the metal surface is reduced, and the resonance peak position of the surface plasma is red-shifted.
In one embodiment, the material of the metal layer is at least one selected from Al, Ga, Ag, Cu and Au, and the thickness of the metal layer is 5nm to 20 nm.
In one embodiment, the composite electrode further comprises a metal oxide layer between the metal layer and the graphene layer.
In one embodiment, the material of the metal oxide layer is selected from Al2O3、Ga2O3、Ag2At least one of O and CuO, and the thickness of the metal oxide layer is 0.5nm to 5 nm.
In one embodiment, the thickness of the graphene layer is 0.1nm to 10 nm.
A preparation method of a composite electrode comprises the following steps:
providing a substrate;
forming a metal layer on the substrate; and
forming a graphene layer on the metal layer.
The preparation method of the composite electrode, which is provided by the technical scheme of the invention, has a simple and convenient process and can realize the color fine adjustment of the light-emitting device.
In one embodiment, the composite electrode further includes a metal oxide layer between the metal layer and the graphene layer, and the method for preparing the composite electrode includes the following steps: :
providing a substrate;
forming a metal layer on the substrate;
forming a metal oxide layer on the metal layer; and
forming a graphene layer on the metal oxide layer.
An electroluminescent device comprising an anode, a cathode and a light-emitting layer between the cathode and the anode, the cathode and the anode being oppositely disposed;
at least one of the anode and the cathode is the composite electrode, and the metal layer of the composite electrode is arranged close to the light-emitting layer.
According to the electroluminescent device adopting the technical scheme, the composite electrode comprises the metal layer, the surface of the metal layer is provided with the micro-nano structure, so that plasma exists, when light emitted by the electroluminescent device passes through the metal layer, surface plasma resonance is easy to occur, and the light emission is enhanced. And electron transfer can occur between the metal layer and the graphene layer, the free electron concentration on the surface of the metal can be changed, and the free electron concentration can influence the frequency of surface plasma resonance, so that the light-emitting peak position of the light-emitting device can be finely adjusted. In general, the free electron concentration of the metal surface is increased, and the resonance peak position of surface plasma is blue-shifted; the free electron concentration of the metal surface is reduced, and the resonance peak position of the surface plasma is red-shifted.
In one embodiment, the electroluminescent device is an organic light emitting diode or a quantum dot light emitting diode.
In one embodiment, the electroluminescent device further comprises a hole functional layer between the anode and the light-emitting layer, and an electron functional layer between the cathode and the light-emitting layer.
Drawings
FIG. 1 is a schematic view of a composite electrode according to an embodiment of the present invention;
fig. 2 is a schematic view of an electroluminescent device according to an embodiment of the present invention.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention comprehensible, embodiments accompanied with figures are described in detail below. In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.
Referring to fig. 1, a composite electrode according to an embodiment of the present invention includes a metal layer 101, a metal oxide layer 102, and a graphene layer 103, which are sequentially stacked, wherein the metal layer 101 is transparent and has a micro-nano structure on a surface thereof.
The metal layer 101 is transparent, that is, when the composite electrode is used as a light emitting electrode, the metal layer 101 has a certain transparency and does not block the transmission of light.
The metal oxide layer 102 serves to adjust the work function of the surface of the metal layer 101, and the work function is generally linearly related to the thickness of the metal oxide.
The micro-nano structure refers to a functional structure which is artificially designed, has a characteristic dimension of micron or nanometer scale and is arranged according to a specific mode, such as a nano island. Since the metal layer 101 has a micro-nano structure on the surface thereof, plasma (also referred to as free electron gas) exists, and when light emitted from the electroluminescent device passes through the metal layer 101, surface plasmon resonance is likely to occur, thereby enhancing light emission.
After the metal oxide layer 102 and the graphene layer 103 are deposited on the surface of the metal layer 101, electron transfer may occur between the metal layer 101 and the graphene layer 103. Since the metal oxide layer 102 can adjust the work function of the surface of the metal layer 101, and the adjusting effect is related to the thickness of the metal oxide layer 102 (in a linear relationship), the metal oxide layer 102 can adjust the electron transfer between the metal layer 101 and the graphene layer 103.
The electron transfer between the metal layer 101 and the graphene layer 103 changes the free electron concentration on the surface of the metal layer 101, the free electron concentration affects the resonance frequency of the surface plasmon of the metal layer 101, and when the frequency range of the light emitted by the device includes the resonance frequency of the surface plasmon of the metal, the emergent light intensity of the device is enhanced at the resonance frequency point, and meanwhile, the light-emitting peak position of the light-emitting device can be finely adjusted. In general, the free electron concentration on the surface of the metal layer 101 increases, and the surface plasmon resonance peak position is blue shifted; the free electron concentration on the surface of the metal layer 101 is reduced, and the surface plasmon resonance peak position is red-shifted.
Specifically, the work function of graphene is determined to be about 4.0 eV. When the work function of the metal in the metal layer 101 is greater than that of graphene, electrons may be transferred from the graphene layer 103 to the metal layer 101, so that the electrons on the surface of the metal layer 101 increase, the work function of the metal decreases, and the surface plasmon resonance peak position is blue-shifted. On the contrary, when the work function of the metal in the metal layer 101 is smaller than that of the graphene, electrons may be transferred from the metal layer 101 to the graphene layer 103, so that the electrons on the surface of the metal layer 101 are reduced, the work function of the metal is increased, and the surface plasmon resonance peak position is red-shifted.
In addition, the metal oxide in the metal oxide layer 102 has a function of fine-tuning the work function of the metal, so that the work function of the metal surface is increased or decreased, and thus the charge transfer between the metal and the graphene is finally affected. Compared with a binary metal/graphene system, charge transfer between ternary metal/metal oxide/graphene is more dynamic, and the adjustment of the wavelength is more subtle and wider as a result.
Further, the effect of the metal oxide layer 102 in adjusting the work function of the surface of the metal layer 101 is linear with the thickness of the metal oxide layer 102. Specifically, when the work function of the surface of the metal layer 101 is reduced, the reduction of the work function of the surface of the metal layer 101 is more obvious as the thickness of the metal oxide layer 102 is increased; conversely, when the work function of the surface of the metal layer 101 is increased, the increase in the work function of the surface of the metal layer 101 becomes more significant as the thickness of the metal oxide layer 102 is increased. Of course, the metal oxide layer 102 has a limit to adjust the work function of the surface of the metal layer 101, the thickness of the metal oxide layer 102 has a significant adjusting effect on the work function of the surface of the metal layer 101 within a range of several nanometers, and the work function of the surface of the metal layer 101 tends to be unchanged after the thickness of the metal oxide layer 102 exceeds a critical value.
Preferably, the material of the metal layer 101 is at least one selected from Al, Ga, Ag, Cu and Au. That is, the material of the metal layer 101 may be any one of the metals or an alloy of any at least two of the metals.
Preferably, the material of the metal oxide layer 102 is selected from Al2O3、Ga2O3、Ag2At least one of O and CuO. That is, the material of the metal oxide layer 102 may be selected from any one of the above metal oxides or a mixture of any at least two of the metal oxides. These kinds of metal oxide layers 102 can adjust the work function of the surface of the metal layer 101.
The metal type in the metal oxide layer 102 may be the same as or different from that of the metal layer 101. When the metal species in the metal oxide layer 102 is the same as the metal species of the metal layer 101, the metal oxide layer 102 is produced by oxidizing the surface of the metal layer, and thus the production process is simple.
Preferably, the thickness of the metal layer 101 is 5nm to 20 nm. At this time, on the one hand, the metal layer 101 has sufficient light transmittance; on the other hand, the surface of the metal film with the thickness generally has a micro-nano structure regardless of the preparation process. Therefore, when the thickness of the metal layer 101 is 5nm to 20nm, the light transmittance can be ensured, and the surface plasmon resonance can be easily generated, which is advantageous for enhancing the emission of light.
Preferably, the thickness of the metal oxide layer 102 is 0.5nm to 5 nm. At this time, the thickness of the metal oxide layer 102 is moderate, and electron transfer between the barrier metal layer 101 and the graphene layer 103 can be avoided.
Preferably, the thickness of the graphene layer 103 is 0.1nm to 10 nm. In this case, both the electrical performance and the optical performance can be achieved.
The composite electrode according to the present invention may not include the metal oxide layer. At this time, the composite electrode includes a metal layer and a graphene layer which are laminated, the metal layer is transparent, and the surface of the metal layer has a micro-nano structure.
According to the composite electrode adopting the technical scheme, the micro-nano structure is arranged on the surface of the metal layer, so that plasma exists, when light emitted by the electroluminescent device passes through the metal layer, surface plasma resonance is easy to occur, and the emergent light is enhanced. And electron transfer can take place between metal level and the graphite alkene layer, can change the free electron concentration on metal surface, and this free electron concentration can influence the resonant frequency of surface plasma, and when the frequency range of the light that the device emitted contains the resonant frequency of metal surface plasma, at resonant frequency point, the emergent light intensity of device can be strengthened, and meanwhile, the luminous peak position of luminescent device can obtain the fine setting. In general, the free electron concentration of the metal surface is increased, and the resonance peak position of surface plasma is blue-shifted; the free electron concentration of the metal surface is reduced, and the resonance peak position of the surface plasma is red-shifted.
The preparation method of the composite electrode of one embodiment of the invention comprises the following steps:
and S10, providing a substrate.
Wherein the substrate functions as a carrier metal layer, the substrate herein is not limited to the substrate of an OLED or a QLED in the conventional sense.
And S20, forming a metal layer on the substrate.
The metal layer may be formed on the substrate by atomic layer deposition, evaporation, magnetron sputtering, or MOCVD, among other processes.
Preferably, the material of the metal layer 101 is at least one selected from Al, Ga, Ag, Cu and Au.
And S30, forming a graphene layer on the metal layer.
The graphene layer may be formed on the metal oxide layer using a chemical vapor deposition process or the like.
The preparation method of the composite electrode, which is provided by the technical scheme of the invention, has a simple and convenient process and can realize the color fine adjustment of the light-emitting device.
Preferably, the composite electrode according to an embodiment of the present invention further includes a metal oxide layer between the metal layer and the graphene layer, and the method for preparing the composite electrode includes the steps of:
s100, providing a substrate.
Wherein the substrate functions as a carrier metal layer, the substrate herein is not limited to the substrate of an OLED or a QLED in the conventional sense.
And S200, forming a metal layer on the substrate.
The metal layer may be formed on the substrate by atomic layer deposition, evaporation, magnetron sputtering, or MOCVD, among other processes.
Preferably, the material of the metal layer 101 is at least one selected from Al, Ga, Ag, Cu and Au.
And S300, forming a metal oxide layer on the metal layer.
The Metal oxide layer may be formed on the Metal layer by atomic layer Deposition, magnetron sputtering, or MOCVD (Metal-organic Chemical Vapor Deposition).
Preferably, the material of the metal oxide layer 102 is selected from Al2O3、Ga2O3、Ag2At least one of O and CuO.
And S400, forming a graphene layer on the metal oxide layer.
The graphene layer may be formed on the metal oxide layer using a chemical vapor deposition process or the like.
The preparation method of the composite electrode, which is provided by the technical scheme of the invention, has a simple and convenient process and can realize the color fine adjustment of the light-emitting device.
In an embodiment of the present invention, there is also provided an electroluminescent device including an anode, a cathode, and a light-emitting layer between the cathode and the anode, the cathode and the anode being disposed opposite to each other.
At least one of the anode and the cathode is the composite electrode, and the metal layer of the composite electrode is arranged close to the light-emitting layer.
The electroluminescent device may be an upright device or an inverted device.
Illustratively, referring to fig. 2, an electroluminescent device according to an embodiment of the present invention comprises a substrate 201, an anode 202, a hole-functional layer 203, a light-emitting layer 204, an electron-functional layer 205, and a cathode 206. At least one of the anode 202 and the cathode 206 is the composite electrode, and the metal layer of the composite electrode is disposed near the light-emitting layer 204. It will of course be appreciated that the substrate 201 of the electroluminescent device described above may also be provided on the cathode 206 side.
The hole functional layer 203 is at least one of a hole transport layer and a hole injection layer, and when the hole functional layer 203 is two layers, the hole injection layer is located between the hole transport layer and the anode 202.
The material of the hole transport layer can be Poly-TPD, Cu2O, CuSCN, NiO, TFB, NPB, alpha-NPD, TAPC, 4P-NPD, PVK, TCTA, mCP, CBP, mCBP, CDBP, and the like.
Cavities of the waferThe material of the injection layer may be a conductive polymer, for example: PEDOT: PSS; it may also be a high work function n-type semiconductor, such as: HAT-CN, MoO3、WO3、V2O5、Rb2O, and the like.
The electron functional layer 205 is at least one of an electron transport layer and an electron injection layer, and when the electron functional layer 205 is two layers, the electron injection layer is located between the electron transport layer and the cathode 206.
The material of the electron transport layer may be an n-type organic semiconductor or an n-type metal oxide. Among them, the n-type organic semiconductor includes, but is not limited to, TPBi, TAZ, TmPyPb, BCP, Bphen, TmPyTz, B3PYMPM, 3TPYMB and PO-T2T. n-type metal oxides include, but are not limited to, ZnO, ZnMgO, ZnAlO, TiO2And SnO2。
The material of the electron injection layer may be an alkali metal salt or a low work function metal. Among them, alkali metal salts include, but are not limited to, LiF, NaF, CsF, and Cs2CO3. Low work function metals include, but are not limited to Yb, Ba, and Mg.
Of course, the hole function layer 203 and the electron function layer 205 may not be provided. In this case, the light-emitting layer is located on the anode, and the cathode is located on the light-emitting layer.
The light emitting material of the light emitting layer 204 may be organic or inorganic quantum dots. Organic substances such as: BCzVBi, Firpic, Cz-2pbb, Bepp2、POTA、DSA-Ph、Ir(ppy)3、Ir(ppy)2(acac)、Ir(ppy)2(bpmp)、DIcTRz、MEH-PPV、Ir(dmpq)2(acac)、Ir(piq)3、Ir(piq)2(acac)、Ir(btpy)3And the like. Inorganic quantum dots, for example: ZnCdSeS, CdSe/ZnSe, CdSeS/CdS, CdSe/CdS/ZnS, ZnCdS/ZnS, ZnCdSeS/ZnS, InP/ZnS, CuInS, AgInS, CuInS/ZnS, AnInS/ZnS, CsPbX3(X ═ Cl, Br, I), and the like. Of course, combinations of the above materials are also possible.
Preferably, the electroluminescent device is an Organic Light Emitting Diode (OLED) or a quantum dot light emitting diode (QLED).
According to the electroluminescent device adopting the technical scheme, the composite electrode comprises the metal layer, the surface of the metal layer is provided with the micro-nano structure, so that plasma exists, when light emitted by the electroluminescent device passes through the metal layer, surface plasma resonance is easy to occur, and the light emission is enhanced. And electron transfer can occur between the metal layer and the graphene layer, the free electron concentration on the surface of the metal can be changed, and the free electron concentration can influence the frequency of surface plasma resonance, so that the light-emitting peak position of the light-emitting device can be finely adjusted. In general, the free electron concentration of the metal surface is increased, and the resonance peak position of surface plasma is blue-shifted; the free electron concentration of the metal surface is reduced, and the resonance peak position of the surface plasma is red-shifted.
The application fields of the invention include flat panel display, solid state lighting and other photoelectric application fields.
In order to make the objects and advantages of the present application more apparent, the present application is further described in detail with reference to the following examples. It should be understood that the specific embodiments described herein are merely illustrative of the present application and are not intended to limit the present application.
Example 1
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TAPC on the hole injection layer by a solution method to form a hole transport layer 1 with the thickness of 30 nm;
depositing TCTA on the hole transport layer 1 by an evaporation method to form a hole transport layer 2 with the thickness of 10 nm;
co-evaporating TCTA Firpic (2%) as a light-emitting layer on the hole transport layer 2 by evaporation method, wherein the thickness is 20 nm;
TPBi is deposited on the luminous layer by an evaporation method to be used as an electron transport layer, and the thickness is 40 nm;
depositing LiF on the electron transport layer by using an evaporation method to form an electron injection layer with the thickness of 1 nm;
depositing Al on the electron injection layer by an evaporation method to serve as a cathode layer 1, wherein the thickness of the cathode layer is 15 nm;
and depositing graphene on the cathode layer 1 by using a chemical vapor deposition method to serve as a cathode layer 3, wherein the thickness is 3 nm.
Example 2
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TAPC on the hole injection layer by a solution method to form a hole transport layer 1 with the thickness of 30 nm;
depositing TCTA on the hole transport layer 1 by an evaporation method to form a hole transport layer 2 with the thickness of 10 nm;
co-evaporating TCTA Firpic (2%) as a light-emitting layer on the hole transport layer 2 by evaporation method, wherein the thickness is 20 nm;
TPBi is deposited on the luminous layer by an evaporation method to be used as an electron transport layer, and the thickness is 40 nm;
depositing LiF on the electron transport layer by using an evaporation method to form an electron injection layer with the thickness of 1 nm;
depositing Al on the electron injection layer by an evaporation method to serve as a cathode layer 1, wherein the thickness of the cathode layer is 15 nm;
depositing Al on the cathode layer 1 by atomic layer deposition2O3As the cathode layer 2, the thickness is 1 nm;
and depositing graphene on the cathode layer 2 by using a chemical vapor deposition method to serve as a cathode layer 3, wherein the thickness is 3 nm.
Example 3
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TAPC on the hole injection layer by a solution method to form a hole transport layer 1 with the thickness of 30 nm;
depositing TCTA on the hole transport layer 1 by an evaporation method to form a hole transport layer 2 with the thickness of 10 nm;
co-evaporating TCTA Firpic (2%) as a light-emitting layer on the hole transport layer 2 by evaporation method, wherein the thickness is 20 nm;
TPBi is deposited on the luminous layer by an evaporation method to be used as an electron transport layer, and the thickness is 40 nm;
depositing LiF on the electron transport layer by using an evaporation method to form an electron injection layer with the thickness of 1 nm;
depositing Al on the electron injection layer by an evaporation method to serve as a cathode layer 1, wherein the thickness of the cathode layer is 15 nm;
depositing Al on the cathode layer 1 by atomic layer deposition2O3As the cathode layer 2, the thickness is 2 nm;
and depositing graphene on the cathode layer 2 by using a chemical vapor deposition method to serve as a cathode layer 3, wherein the thickness is 3 nm.
Example 4
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TAPC on the hole injection layer by a solution method to form a hole transport layer 1 with the thickness of 30 nm;
depositing TCTA on the hole transport layer 1 by an evaporation method to form a hole transport layer 2 with the thickness of 10 nm;
co-evaporating TCTA Firpic (2%) as a light-emitting layer on the hole transport layer 2 by evaporation method, wherein the thickness is 20 nm;
TPBi is deposited on the luminous layer by an evaporation method to be used as an electron transport layer, and the thickness is 40 nm;
depositing LiF on the electron transport layer by using an evaporation method to form an electron injection layer with the thickness of 1 nm;
depositing Al on the electron injection layer by an evaporation method to serve as a cathode layer 1, wherein the thickness of the cathode layer is 15 nm;
depositing Al on the cathode layer 1 by atomic layer deposition2O3As the cathode layer 2, the thickness is 3 nm;
and depositing graphene on the cathode layer 2 by using a chemical vapor deposition method to serve as a cathode layer 3, wherein the thickness is 3 nm.
Example 5
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TFB on the hole injection layer by a solution method to serve as a hole transport layer, wherein the thickness of the TFB is 30 nm;
depositing ZnCdS/ZnS quantum dots on the hole transport layer by a solution method to be used as a light-emitting layer, wherein the thickness of the ZnCdS/ZnS quantum dots is 20 nm;
ZnMgO is deposited on the luminous layer by a solution method to be used as an electron transport layer, and the thickness is 50 nm;
depositing Ag on the electron transmission layer by using an evaporation method to serve as a cathode layer 1, wherein the thickness of the Ag is 15 nm;
depositing Ag on the cathode layer 1 by atomic layer deposition2O is used as a cathode layer 2, and the thickness is 2 nm;
and depositing graphene on the cathode layer 2 by using a chemical vapor deposition method to serve as a cathode layer 3, wherein the thickness is 3 nm.
Example 6
Using ITO/Ag/ITO as a cathode, wherein the thickness is 50/100/30nm respectively;
depositing ZnO as an electron transport layer on the cathode by a solution method, wherein the thickness of the ZnO is 60 nm;
depositing CdSe/CdS quantum dots on the electron transport layer by a solution method to be used as a light emitting layer, wherein the thickness of the CdSe/CdS quantum dots is 20 nm;
depositing TCTA as a hole transport layer on the luminescent layer by an evaporation method, wherein the thickness of the TCTA is 40 nm;
deposition of MoO on hole transport layer by evaporation3As a hole injection layer, 10 a 10nnm a thick;
depositing Au on the hole injection layer by an evaporation method to be used as an anode layer 1, wherein the thickness of the Au is 15 nm;
deposition of Al on the anode layer 1 by atomic layer deposition2O3As the anode layer 2, the thickness was 2 nm;
graphene was deposited as an anode layer 3 on the anode layer 2 by chemical vapor deposition to a thickness of 3 nm.
Comparative example 1
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TAPC on the hole injection layer by a solution method to form a hole transport layer 1 with the thickness of 30 nm;
depositing TCTA on the hole transport layer 1 by an evaporation method to form a hole transport layer 2 with the thickness of 10 nm;
co-evaporating TCTA Firpic (2%) as a light-emitting layer on the hole transport layer 2 by evaporation method, wherein the thickness is 20 nm;
TPBi is deposited on the luminous layer by an evaporation method to be used as an electron transport layer, and the thickness is 40 nm;
depositing LiF on the electron transport layer by using an evaporation method to form an electron injection layer with the thickness of 1 nm;
al is deposited as a cathode on the electron injection layer by evaporation to a thickness of 20 nm.
Comparative example 2
Taking ITO/Ag/ITO as an anode, wherein the thickness is 50/100/30nm respectively;
PSS is used as a hole injection layer, and the thickness is 30 nm;
depositing TFB on the hole injection layer by a solution method to serve as a hole transport layer, wherein the thickness of the TFB is 30 nm;
depositing ZnCdS/ZnS quantum dots on the hole transport layer by a solution method to be used as a light-emitting layer, wherein the thickness of the ZnCdS/ZnS quantum dots is 20 nm;
ZnMgO is deposited on the luminous layer by a solution method to be used as an electron transport layer, and the thickness is 50 nm;
ag was deposited as a cathode on the electron transport layer by evaporation to a thickness of 20 nm.
Comparative example 3
Using ITO/Ag/ITO as a cathode, wherein the thickness is 50/100/30nm respectively;
depositing ZnO as an electron transport layer on the cathode by a solution method, wherein the thickness of the ZnO is 60 nm;
depositing CdSe/CdS quantum dots on the electron transport layer by a solution method to be used as a light emitting layer, wherein the thickness of the CdSe/CdS quantum dots is 20 nm;
depositing TCTA as a hole transport layer on the luminescent layer by an evaporation method, wherein the thickness of the TCTA is 40 nm;
deposition of MoO on hole transport layer by evaporation3As a hole injection layer, 10 a 10nnm a thick;
au was deposited as an anode on the hole injection layer by evaporation to a thickness of 20 nm.
And (3) testing:
the electroluminescent peak positions and the maximum external quantum efficiencies of the electroluminescent devices of examples 1 to 6 and comparative examples 1 to 3 were examined to obtain the data of table 1:
TABLE 1
| Examples | Peak position of electroluminescence | Maximum external quantum efficiency (%) |
| Example 1 | 467 | 13.5 |
| Example 2 | 471 | 13.2 |
| Example 3 | 475 | 13.7 |
| Example 4 | 478 | 13.5 |
| Example 5 | 450 | 12.8 |
| Examples6 | 625 | 16.2 |
| Comparative example 1 | 475 | 13.8 |
| Comparative example 2 | 460 | 12.5 |
| Comparative example 3 | 630 | 16.7 |
As can be seen from the data in table 1:
(1) compared with the example 1 and the comparative example 1, the differences of the examples 2 to 4 are that: different from the cathodes, the composite cathodes of examples 2 to 4 were made of Al (work function of 4.3eV)/Al2O3(Fermi level of 2.5 eV)/graphene (work function of 4.0eV), and Al in the composite cathodes of examples 2 to 42O3Gradually increases in thickness. The test result shows that: the external quantum efficiency was not substantially affected, but the emission peak positions of examples 2 to 4 were changed from those of example 1 and comparative example 1.
Specifically, the electroluminescence peak position of the electroluminescent device of example 1 was reduced compared to that of comparative example 1, which is presumed to be because electrons would be transferred from the graphene layer to the Al surface due to the work function of Al being larger than that of graphene, resulting in an increase in electrons at the Al surface and a reduction in the work function of Al, thereby blue-shifting the surface plasmon resonance peak position.
The electroluminescent peak positions of the electroluminescent devices of examples 2 to 4 are gradually increased compared to example 1. This is presumably because Al is attached to the Al surface2O3The work function of Al is gradually reduced due to the increase of the thickness, so that the charge between Al and graphene is transferredThe shift changes from graphene to Al gradually, and the electron concentration on the Al surface gradually changes from high to low, so that the emission peak positions of the electroluminescent devices of examples 2 to 4 are gradually red-shifted relative to the emission peak position of the electroluminescent device of example 1.
(2) Example 5 differs from comparative example 2 in that: the cathode of example 5 was different from the cathode in Ag (work function 4.3eV)/Ag2O (work function greater than Ag)/graphene (work function of 4.0 eV). The test result shows that: the external quantum efficiency has substantially no effect, but the surface plasmon resonance peak position is reduced (blue-shifted). This indicates that the use of the composite electrode of example 5 allows fine adjustment of the emission peak position; this is presumably due to Ag2The presence of O further increases the work function of Ag, so that more electrons are transferred from the graphene layer to the Ag surface, the electrons on the Ag surface are increased, the work function of Ag is reduced, and the resonance peak position of surface plasma is blue shifted.
(3) Example 6 differs from comparative example 3 in that: the anode of example 6 was different from the other, and was Au (work function: 5.1eV)/Al2O3(Fermi level of 2.5 eV)/graphene (work function of 4.0 eV). The test result shows that: the external quantum efficiency has substantially no effect, but the surface plasmon resonance peak position is reduced (blue-shifted). This indicates that the use of the composite electrode of example 6 allows fine adjustment of the emission peak position. This is presumed to be because the work function of Au is larger than that of graphene, and electrons are transferred from the graphene layer to the Au surface, so that the number of electrons on the Au surface increases, the work function of Au decreases, and the surface plasmon resonance peak position is blue-shifted.
The above whole shows that the composite electrode of the present invention has no influence on the external quantum efficiency of the electroluminescent device, but can be used for micro-adjusting the luminescence peak position, and the adjusting effect is irrelevant to the composite electrode as an anode or a cathode.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (10)
1. The composite electrode is characterized by comprising a laminated metal layer and a graphene layer, wherein the metal layer is transparent and the surface of the metal layer is provided with a micro-nano structure.
2. The composite electrode according to claim 1, wherein the metal layer is made of at least one material selected from the group consisting of Al, Ga, Ag, Cu, and Au, and has a thickness of 5nm to 20 nm.
3. The composite electrode of claim 1, further comprising a metal oxide layer between the metal layer and the graphene layer.
4. The composite electrode of claim 3, wherein the metal oxide layer is made of a material selected from Al2O3、Ga2O3、Ag2At least one of O and CuO, and the thickness of the metal oxide layer is 0.5nm to 5 nm.
5. A composite electrode according to any one of claims 1 to 4, wherein the graphene layer has a thickness of from 0.1nm to 10 nm.
6. The preparation method of the composite electrode is characterized by comprising the following steps of:
providing a substrate;
forming a metal layer on the substrate; and
forming a graphene layer on the metal layer.
7. The method of manufacturing a composite electrode according to claim 6, further comprising a metal oxide layer between the metal layer and the graphene layer, the method comprising the steps of:
providing a substrate;
forming a metal layer on the substrate;
forming a metal oxide layer on the metal layer; and
forming a graphene layer on the metal oxide layer.
8. An electroluminescent device comprising an anode, a cathode and a light-emitting layer between the cathode and the anode, the cathode and the anode being disposed opposite to each other;
wherein at least one of the anode and the cathode is the composite electrode according to any one of claims 1 to 5, and the metal layer of the composite electrode is disposed adjacent to the light-emitting layer.
9. An electroluminescent device as claimed in claim 8, characterized in that the electroluminescent device is an organic light-emitting diode or a quantum dot light-emitting diode.
10. The device of claim 8, further comprising a hole functional layer between the anode and the light-emitting layer and an electron functional layer between the cathode and the light-emitting layer.
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