CN116437687A - Photoelectric device, preparation method thereof and photoelectric device - Google Patents

Photoelectric device, preparation method thereof and photoelectric device Download PDF

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CN116437687A
CN116437687A CN202111675725.7A CN202111675725A CN116437687A CN 116437687 A CN116437687 A CN 116437687A CN 202111675725 A CN202111675725 A CN 202111675725A CN 116437687 A CN116437687 A CN 116437687A
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hole transport
transport layer
layer
hexafluoropropylene
anode
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田鹍飞
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TCL Technology Group Co Ltd
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Abstract

The application discloses a photoelectric device and a preparation method thereof, and a photoelectric device, wherein the photoelectric device comprises a cathode, an anode, a light-emitting layer and a hole transport layer, wherein the light-emitting layer and the hole transport layer are arranged between the cathode and the anode, the hole transport layer contains polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane, and the dielectric constant of the hole transport layer is improved by adding polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane into the hole transport layer, so that the efficiency and the service life of the device are improved, and the performance of the device is improved; on the other hand, the film forming property of the electron transport layer is better and more uniform, and the film layer is more compact, so that the problem of leakage current is solved; in addition, the concentration of holes can be effectively improved, and the conductivity of the device is improved.

Description

Photoelectric device, preparation method thereof and photoelectric device
Technical Field
The application relates to the technical field of photoelectricity, in particular to a photoelectric device, a preparation method thereof and a photoelectric device.
Background
A quantum dot light Emitting diode (QLED) is a photoelectric device that uses quantum dots as a light Emitting source. The general basic structure is a multi-layer structure composed of a hole transport layer, a light emitting layer and an electron transport layer, and the light emitting principle is as follows: under the drive of an external electric field, holes and electrons respectively enter the valence band energy level and the conduction band energy level of the light-emitting layer to overcome interface barriers, and when the light-emitting layer returns to a stable ground state from an excited state, photons are released to emit light. The method has the advantages of good material stability, continuous and adjustable luminescence wavelength along with the size of the quantum dot, narrow luminescence spectrum, high fluorescence quantum yield, capability of being constructed by a full solution method and the like, and is paid attention to more and more scientific researchers.
At present, through years of development, photoelectric device technologies represented by quantum dot light emitting diodes have been greatly broken through and developed, however, many problems to be solved still exist, especially unbalance of electron and hole injection, and the influence on device life and luminous efficiency is significant.
Disclosure of Invention
In view of the above, the present application provides an optoelectronic device, a method for manufacturing the same, and an optoelectronic apparatus, which aim to improve the performance of the device.
In a first aspect, an embodiment of the present application provides an optoelectronic device, including a cathode, an anode, and a light emitting layer and a hole transporting layer disposed between the cathode and the anode, where the hole transporting layer is disposed near the anode, the light emitting layer is disposed near the cathode, and the hole transporting layer contains polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane.
Optionally, the hole transport layer contains polyvinylidene fluoride co-hexafluoropropylene and 2-cyanoethyl trimethoxysilane, and the mass ratio of the polyvinylidene fluoride co-hexafluoropropylene to the 2-cyanoethyl trimethoxysilane is (1-3): (1-2).
Optionally, the mass ratio of the polyvinylidene fluoride co-hexafluoropropylene to the 2-cyanoethyl trimethoxysilane is (2-3): 1.
Optionally, in the hole transport layer, the total mass ratio of the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyl trimethoxysilane is 17% -29%.
Optionally, in the hole transport layer, the total mass ratio of the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyl trimethoxysilane is 17% -20%.
Optionally, the hole transport layer has a thickness of 22nm to 28nm.
Optionally, the hole transport layer has a thickness of 22nm to 25nm.
Optionally, the hole transport layer is composed of a first hole transport material, and polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxysilane.
Optionally, the material of the light emitting layer includes quantum dots, the quantum dots are selected from at least one of single-structure quantum dots and core-shell structure quantum dots, the single-structure quantum dots are selected from at least one of II-VI group compounds, III-V group compounds and I-III-VI group compounds, the II-VI group compounds are selected from at least one of CdSe, cdS, cdTe, znO, znSe, znS, cdTe, znTe, hgS, hgSe, hgTe, cdZnS, cdZnSe, cdZnTe, znSeS, znSeTe, znTeS, cdSeS, cdSeTe, cdTeS, cdZnSeS, cdZnSeTe and CdZnSTe, and the III-V group compounds are selected from at least one of InP, inAs, gaP, gaAs, gaSb, inSb, alAs, alN, alP, inAsP, inNP, inNSb, gaAlNP and InAlNP; the I-III-VI compound is selected from CuInS 2 、CuInSe 2 AgInS 2 The core of the quantum dot with the core-shell structure is selected from any one of the quantum dots with the single structure, and the shell material of the quantum dot with the core-shell structure is selected from at least one of CdS, cdTe, cdSeTe, cdZnSe, cdZnS, cdSeS, znSe, znSeS and ZnS; and/or the number of the groups of groups,
the first hole transport material is selected from: at least one of N, N '-dinaphthyl-N, N' -diphenyl benzidine, N '-bis- (3-methylphenyl) -N, N' -bis- (phenyl) -benzidine), 4',4 "-tris (N-3-methylphenyl-N-phenyl-amino) -triphenylamine, poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine), polyvinylcarbazole, poly (N, N' -bis (4-butylphenyl) -N, N '-bis (phenyl) benzidine) or 4,4',4" -tris (carbazol-9-yl) triphenylamine; and/or the number of the groups of groups,
the cathode material is selected from: at least one of an Ag electrode, an Al electrode, an Au electrode, a Pt electrode, or an alloy electrode; and/or the anode material is selected from a metal oxide electrode or a composite electrode, the metal being oxidizedThe object electrode is at least one selected from ITO, FTO, ATO, AZO, GZO, 1ZO, MZO and AMO, and the composite electrode is AZO/Ag/AZO, AZO/Al/AZO, ITO/Ag/ITO, ITO/Al/ITO, znO/Ag/ZnO, znO/Al/ZnO, tiO 2 /Ag/TiO 2 、TiO 2 /Al/TiO 2 At least one of ZnS/Ag/ZnS or ZnS/Al/ZnS.
Optionally, a hole injection layer is further disposed between the anode and the hole transport layer, and a material of the hole injection layer is selected from the group consisting of: poly (ethylenedioxythiophene): polystyrene sulfonate, poly (9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine), polyarylamine, poly (N-vinylcarbazole), polyaniline, polypyrrole, N, N, N ', N' -tetra (4-methoxyphenyl) -benzidine, 4-bis [ N- (1-naphthyl) -N-phenyl-amino ] biphenyl, 4 '-tris [ phenyl (m-tolyl) amino ] triphenylamine, 4', at least one of 4 "-tris (N-carbazolyl) -triphenylamine, 1-bis [ (di-4-tolylamino) phenylcyclohexane, 4',4" -tris (diphenylamino) triphenylamine doped with tetrafluoro-tetracyano-quinone dimethane, p-doped phthalocyanine, F4-TCNQ doped N, N' -diphenyl-N, N '-bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine or hexaazabenzophenanthrene-hexanenitrile.
In a second aspect, the present application provides a method for preparing an optoelectronic device, comprising the steps of:
preparing a hole transport layer on the anode;
preparing a light emitting layer on the hole transport layer; and
preparing a cathode on the light-emitting layer to obtain the photoelectric device; or alternatively, the process may be performed,
Preparing a light emitting layer on a cathode;
preparing a hole transport layer on the light emitting layer; and
preparing an anode on the hole transport layer to obtain the photoelectric device;
wherein the hole transport layer contains polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxysilane.
Optionally, the hole transport layer is prepared by the following method: mixing polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxy silane, a first hole transport material and an organic solvent to obtain a mixed solution; and
and forming a film on the light-emitting layer or the anode by the mixed solution, and drying to obtain the hole transport layer.
Optionally, in the mixed solution, the concentration ratio of the polyvinylidene fluoride co-hexafluoropropylene and the 2-cyanoethyl trimethoxysilane is (1-3): (1-2); and/or the ratio of the total concentration of the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyl trimethoxysilane to the concentration of the first hole transport material is 1: (2.5-5); and/or the concentration of the first hole transport material is 6mg/mL to 10mg/mL; and/or the organic solvent is chlorobenzene.
The application also provides an optoelectronic device comprising the optoelectronic device of the first aspect or comprising the optoelectronic device prepared by the preparation method of the second aspect.
The beneficial effects are that:
the application provides a photoelectric device, comprising a cathode, an anode, a light-emitting layer and a hole-transporting layer, wherein the light-emitting layer and the hole-transporting layer are arranged between the cathode and the anode, the hole-transporting layer contains polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxysilane, the dielectric constant of the hole-transporting layer is improved by adding the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyl trimethoxysilane into the hole-transporting layer, so that the improvement of the hole injection level is realized, the balance of carriers is realized, the efficiency and the service life of the device are improved, and the performance of the device is improved; on the other hand, the addition of the two materials can also lead the film forming property of the electron transport layer to be better and more uniform and the film layer to be more compact, thereby improving the problem of leakage current; in addition, the fluorine-containing group in the polyvinylidene fluoride co-hexafluoropropylene and the cyano group in the 2-cyanoethyl trimethoxy silane have better electron-withdrawing effect, so that electrons on a semiconductor can be sucked away, holes are left, the concentration of the holes can be effectively improved, and the conductivity of the device is improved.
Drawings
In order to more clearly illustrate the technical solutions in the embodiments of the present application, the drawings that are required to be used in the description of the embodiments will be briefly described below.
Fig. 1 is a schematic structural diagram of a positive photoelectric device according to an embodiment of the present application;
fig. 2 is a schematic structural diagram of an inversion photoelectric device according to an embodiment of the present application;
fig. 3 is a flowchart of a preparation of a positive photoelectric device according to an embodiment of the present application;
fig. 4 is a flowchart of a preparation of an inversion photoelectric device according to an embodiment of the present application;
fig. 5 to 9 are schematic diagrams of test results of current density-voltage curves of examples and comparative examples provided in examples of the present application.
Detailed Description
The following description of the embodiments of the present application will be made clearly and fully with reference to the accompanying drawings, in which it is evident that the embodiments described are only some, but not all, of the embodiments of the present application. All other embodiments, which can be made by those skilled in the art based on the embodiments herein without making any inventive effort, are intended to be within the scope of the present application.
The embodiment of the application provides an optoelectronic device, a preparation method thereof and an optoelectronic device. The following will describe in detail. The following description of the embodiments is not intended to limit the preferred embodiments. In addition, in the description of the present application, the term "comprising" means "including but not limited to". Various embodiments of the present application may exist in a range of forms; it should be understood that the description in a range format is merely for convenience and brevity and should not be construed as a rigid limitation on the scope of the application; it is therefore to be understood that the range description has specifically disclosed all possible sub-ranges and individual values within that range. Whenever a numerical range is referred to herein, it is meant to include any reference number (fractional or integer) within the range referred to.
First, as shown in fig. 1 and 2, an embodiment of the present application provides an optoelectronic device, including a cathode 70, an anode 20, and a light emitting layer 50 and a hole transporting layer 40 disposed between the cathode 70 and the anode 20, wherein the hole transporting layer 40 is disposed near the anode 20, the light emitting layer 50 is disposed near the cathode 70, and the hole transporting layer 40 contains polyvinylidene fluoride co-hexafluoropropylene (P (VDF-HFP) with a structural formula shown in formula 1 and/or 2-cyanoethyl trimethoxysilane (3- (trimethoysilyl) with a structural formula shown in formula 2). Namely: the hole transport layer 40 contains P (VDF-HFP); or the hole transport layer 40 contains NETMS; still alternatively, the hole transport layer 40 contains P (VDF-HFP) and (NETMS).
Figure BDA0003451905160000051
The inventors found that: adjusting the dielectric constant of the hole transport layer 40 is an effective means of adjusting the level of carrier injection, and by increasing the dielectric constant of the hole transport layer 40, an increase in the level of hole injection can be achieved, thereby improving the efficiency and lifetime of the device. According to the embodiment of the application, the P (VDF-HFP) and/or NETMS are added into the hole transport layer 40 to improve the dielectric constant of the hole transport layer 40, so that the improvement of the hole injection level is realized, the balance of carriers is realized, the efficiency and the service life of the device are improved, and the performance of the device is improved.
On the other hand, it has been found that the efficiency and lifetime of the photovoltaic device are affected by the thickness of the hole transport layer 40, and that, within a certain thickness range, the thinner the hole transport layer 40, the higher the level of hole injection, and thus the higher the device efficiency and lifetime, and appropriate reduction of the thickness of the hole transport layer 40 can have higher efficiency and lifetime. However, when the thickness of the hole transport layer 40 is reduced to a certain extent, other problems such as increased instability of film formation, and high leakage current easily occur in the device, and the turn-on voltage of the device increases, which results in a significant decrease in the light emitting efficiency and lifetime of the device. The P (VDF-HFP) and/or NETMS material in the present application has good chemical stability in the solution in the preparation process of the hole transport layer 40, is not easy to volatilize and aggregate, and the addition of P (VDF-HFP) can also reduce the surface energy of the solution, so that the spreadability of the solution is improved, the film forming property of the hole transport layer 40 can be better and more uniform, and the compactness of the film layer can be improved, thereby preventing the problem of higher leakage current caused by a thinner hole transport layer 40. Therefore, the embodiment of the application not only can improve the service life and efficiency of the device under the condition that the thickness of the hole transport layer 40 is unchanged, but also can prevent the problem of high leakage current under the condition that the thickness of the hole transport layer 40 is thinned, thereby further improving the service life and efficiency of the device and breaking through the barrier of the leakage current problem caused by the improvement of the service life and the efficiency in the prior art.
In addition, the fluorine-containing group in P (VDF-HFP) and the cyano group in NETMS have better electron-withdrawing effect, and the strong electron-withdrawing group can suck electrons on a semiconductor, so that holes are left, the concentration of the holes can be effectively improved, and the conductivity of the device is improved. The polyvinylidene fluoride co-hexafluoropropylene material can simultaneously reduce the injection barrier of carriers through the interface dipole effect, thereby improving the hole transmission efficiency and the hole transmission performance of the semiconductor material.
In some embodiments, a hole injection layer 30 is further disposed between the anode 20 and the hole transport layer 40.
Since the hole injection layer 30 material, poly (3, 4-ethylenedioxythiophene) -polystyrene sulfonic acid (PEDOT: PSS), exhibits weak acidity in a solution at the time of film preparation, and the PSS unit absorbs water more easily, degradation of the hole transport layer 40, which is an organic semiconductor material, which is subsequently deposited, is accelerated, and eventually the light emitting efficiency, uniformity, lifetime, and stability of the device are affected. In the application, substances with high dielectric constants such as P (VDF-HFP) and/or NETMS are added, so that the dielectric constants of the film layer can be effectively regulated, meanwhile, the two materials are both lipophilic substances, moisture can be effectively prevented from entering the hole transport layer 40 and even the luminescent layer 50, a good protection effect can be achieved, and the device is more stable.
In some embodiments, when the first hole transport material contains P (VDF-HFP) and NETMS, the lifetime and efficiency of the device can be further improved, and the performance improvement effect is further improved. In some embodiments, the mass ratio of P (VDF-HFP) to NETMS is (1-3): (1-2). In particular, in some embodiments, the mass ratio is 2.5:1. When the ratio of the two is (2-3): 1, in particular 2.5:1, the injection level of the hole transport layer 40 is better; the P (VDF-HFP) material can effectively regulate hole injection, and reduce the injection barrier of carriers through the interface dipole effect, but introducing too much P (VDF-HFP) material can cause leakage current problem of the device. The introduction of NETMS can also adjust the dielectric constant of the hole transport layer 40 while effectively avoiding the moisture absorption problem of the device and protecting the stability of the device, but too much introduction can affect the conductivity of the device. It is understood that the mass ratio of P (VDF-HFP) to NETMS may be (1-3): any value within the range of (1-2), for example: 3: 1. 2: 1. 1: 1. 1:2, or (1 to 3): other values not listed in the range of (1-2).
In some embodiments, the mass ratio of the total mass of P (VDF-HFP) and/or NETMS to the first hole transport material is 1: (2.5-5), namely, in the hole transport layer, the total mass ratio of the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyl trimethoxysilane is 17-29%. When the mass ratio of the total mass of the P (VDF-HFP) and/or NETMS to the first hole transport material is 1: (4 to 5), in particular 1:4, that is, in the hole transport layer, the effect of improving the device performance is better when the total mass ratio of the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyltrimethoxysilane is 17% -20%, particularly 20%. If the content of P (VDF-HFP) and/or NETMS is too high, the conductivity of the hole transport layer 40 is affected, so that the device turn-on voltage is easily increased, and the adjustment of the dielectric constant of the solution is not achieved. It is understood that the mass ratio of the total mass of P (VDF-HFP) and/or NETMS to the first hole transport material may be 1: any value within the range of (2.5 to 5), for example: 1:2.5, 1:3. 1:3.5, 1:4. 1:4.5, 1:5, etc., or 1: other values not listed in the range of (2.5-5).
The optoelectronic device in the embodiments of the present application may be a positive type structure or an inverse type structure. In an optoelectronic device, the cathode 70 or the anode 20 further comprises a substrate 10 on the side facing away from the light-emitting layer 50, the anode 20 being arranged on the substrate 10 in a positive configuration and the cathode 70 being arranged on the substrate 10 in an negative configuration. A hole-injecting layer 30, an electron-blocking layer, and other hole-functional layers may be provided between the anode 20 and the light-emitting layer 50, and an electron-injecting layer, an electron-transporting layer 60, an electron-blocking layer, and other electron-functional layers may be provided between the cathode 70 and the light-emitting layer 50, regardless of the positive type structure or the negative type structure.
Fig. 1 shows a schematic diagram of a positive structure of an optoelectronic device according to an embodiment of the present application, as shown in fig. 1, where the positive structure optoelectronic device includes a substrate 10, an anode 20 disposed on a surface of the substrate 10, a hole injection layer 30 disposed on a surface of the anode 20, a hole transport layer 40 disposed on a surface of the hole injection layer 30, a light emitting layer 50 disposed on a surface of the hole transport layer 40, an electron transport layer 60 disposed on a surface of the light emitting layer 50, and a cathode 70 disposed on a surface of the electron transport layer 60, where the hole transport layer 40 contains a first hole transport material, P (VDF-HFP), and NETMS.
Fig. 2 is a schematic diagram of an inversion structure of the optoelectronic device according to the embodiment of the present application, as shown in fig. 2, where the inversion structure optoelectronic device includes a substrate 10, a cathode 70 disposed on a surface of the substrate 10, an electron transport layer 60 disposed on a surface of the cathode 70, a light emitting layer 50 disposed on a surface of the electron transport layer 60, a hole transport layer 40 disposed on a surface of the light emitting layer 50, and a hole injection layer 30 disposed on a surface of the hole transport layer 40, and an anode 20, and the hole transport layer 40 contains a first hole transport material, P (VDF-HFP) and NETMS.
In the embodiments of the present application, the materials of the respective functional layers are common materials in the art, for example:
the substrate 10 may be a rigid substrate or a flexible substrate. Specific materials may include at least one of glass, silicon wafer, polycarbonate, polymethyl methacrylate, polyethylene terephthalate, polyethylene naphthalate, polyamide, polyethersulfone.
The hole injection layer 30 material may be selected from, but is not limited to: poly (ethylenedioxythiophene): polystyrene sulfonate (PEDOT: PSS), poly (9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine) (TFB), polyarylamines, poly (N-vinylcarbazole), polyaniline, polypyrrole, N, N, N ', N' -tetrakis (4-methoxyphenyl) -benzidine (TPD), 4-bis [ N- (1-naphthyl) -N-phenyl-amino ] biphenyl (. Alpha. -NPD), 4 '-tris [ phenyl (m-tolyl) amino ] triphenylamine (m-MTDATA), 4',4 '-tris (N-carbazolyl) -triphenylamine (TCTA), 1-bis [ (di-4-tolylamino) phenylcyclohexane (TAPC), 4' -tris (diphenylamino) triphenylamine (TDATA) doped with tetrafluoro-tetracyano-quinone dimethane (F4-TCNQ), p-doped phthalocyanines (e.g., F4-TCNQ-doped zinc phthalocyanine (ZnPc)), F4-TCNQ doped N, N '-diphenyl-N, N' -bis (1-naphthyl) -1,1 '-biphenyl-4, 4' -diamine (alpha-NPD), hexaazabenzophenanthrene-hexanitrile (HAT-CN); or a combination of any one or more of the above.
The hole transport layer is composed of a first hole transport material, polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxysilane. In some embodiments, the first hole transport material may be selected from, but is not limited to: at least one of N, N '-dinaphthyl-N, N' -diphenyl benzidine (NPD), N '-bis- (3-methylphenyl) -N, N' -bis- (phenyl) -benzidine) (TPD), and 4,4',4 "-tris (N-3-methylphenyl-N-phenyl-amino) -triphenylamine (MTDATA), poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine) (TFB), polyvinylcarbazole (PVK), poly (N, N' -bis (4-butylphenyl) -N, N '-bis (phenyl) benzidine (poly-TPD), 4',4" -tris (carbazol-9-yl) triphenylamine (TCTA). However, it is not limited thereto, and it is understood that the first hole transport material may be selected from any other known materials in the art, as long as the first hole transport material can be used in the hole transport layer, and materials other than P (VDF-HFP) and NETMS are not particularly limited thereto.
The material of the light emitting layer 50 includes quantum dots selected from, but not limited to, at least one of single structure quantum dots and core-shell structure quantum dots. The single structure quantum dot may be selected from but not limited to group II-VI At least one of a compound, a III-V compound, and a I-III-VI compound. By way of example, the group II-VI compound may be selected from, but not limited to, at least one of CdSe, cdS, cdTe, znSe, znS, cdTe, znTe, cdZnS, cdZnSe, cdZnTe, znSeS, znSeTe, znTeS, cdSeS, cdSeTe, cdTeS, cdZnSeS, cdZnSeTe and CdZnSTe; the III-V compounds may be selected from, but are not limited to, at least one of InP, inAs, gaP, gaAs, gaSb, alN, alP, inAsP, inNP, inNSb, gaAlNP and InAlNP; the I-III-VI compound may be selected from, but is not limited to, cuInS 2 、CuInSe 2 AgInS 2 At least one of them. The core of the quantum dot of the core-shell structure can be selected from any one of the quantum dots of the single structure, and the shell material of the quantum dot of the core-shell structure can be selected from at least one of CdS, cdTe, cdSeTe, cdZnSe, cdZnS, cdSeS, znSe, znSeS and ZnS, but not limited to. As an example, the quantum dot of the core-shell structure may be selected from, but not limited to, at least one of CdZnSe/CdZnS/ZnS, cdZnSe/ZnSe/ZnS, cdSe/ZnS, znSe/ZnS, znSeTe/ZnS, cdSe/CdZnSeS/ZnS, inP/ZnSe/ZnS, and InP/ZnSeS/ZnS.
The material of the electron transport layer 60 may be composed of an inorganic material and/or an organic material. When inorganic, it may be: metal/non-metal oxides (e.g., tiO) undoped or doped with aluminum (Al), magnesium (Mg), indium (In), lithium (Li), gallium (Ga), cadmium (Cd), cesium (Cs), or copper (Cu) 2 、ZnO、ZrO、SnO 2 、WO 3 、Ta 2 O 3 、HfO 3 、Al 2 O 3 、ZrSiO 4 、BaTiO 3 And BaZrO 3 ) The method comprises the steps of carrying out a first treatment on the surface of the Semiconductor particles undoped or doped with Al, mg, in, li, ga, cd, cs or Cu (e.g., cdS, znSe, and ZnS); nitrides, e.g. Si 3 N 4 The method comprises the steps of carrying out a first treatment on the surface of the And combinations thereof. In the case of an organic material, the organic material may be formed of an organic material such as an oxazole compound, an isoxazole compound, a triazole compound, an isothiazole compound, an oxadiazole compound, a thiadiazole compound, a perylene compound, or an aluminum complex.
The cathode 70 material is selected from, but not limited to: at least one of an Ag electrode, an Al electrode, an Au electrode, a Pt electrode, or an alloy electrode.
The anode 20 material is selected from, but not limited to, a metal oxide electrode selected from at least one of ITO, FTO, ATO, AZO, GZO, 1ZO, MZO and AMO, or a composite electrode of AZO/Ag/AZO, AZO/Al/AZO, ITO/Ag/ITO, ITO/Al/ITO, znO/Ag/ZnO, znO/Al/ZnO, tiO 2 /Ag/TiO 2 、TiO 2 /Al/TiO 2 At least one of ZnS/Ag/ZnS or ZnS/Al/ZnS.
The thickness of the anode 20 is 20nm to 200nm (nanometers); the thickness of the hole injection layer 30 is 20nm to 200nm; the thickness of the light emitting layer 50 is 15nm to 180nm. The thickness of the electron transport layer 60 is 10nm to 180nm; the thickness of the cathode 70 is 40nm to 190nm.
The thickness of the hole transport layer 40 is 30nm to 180nm, and in order to obtain better device performance, the thickness of the hole transport layer 40 may be 22nm to 28nm in some embodiments, because the lifetime and efficiency of the device are affected by the thickness of the hole transport layer 40. It is understood that the thickness of the hole transport layer 40 may be any value in the range of 22nm to 28nm, such as 22nm, 23nm, 24nm, 25nm, 26nm, 27nm, 28nm, etc., or any other value not listed in the range of 22nm to 28nm. In other embodiments, the thickness of the hole transport layer 40 may be below 25nm, such as 22nm to 25nm, for further achieving better device performance. In a common device, the hole transport layer 40 with the thickness in the range is thinner, so that the service life and the efficiency are higher, but the phenomenon of high leakage current of the device is easier to cause, and the addition of P (VDF-HFP) and/or NETMS in the hole transport layer 40 can improve the phenomenon of high leakage current and further improve the service life and the efficiency, so that compared with other thicknesses, the hole transport layer 40 with the thickness can realize higher service life and efficiency, improve the phenomenon of high leakage current, and realize better device performance.
In some embodiments, the hole transport layer is comprised of a first hole transport material, and polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane. However, the hole transport layer is not limited thereto, and may include other materials as long as they can be used in the hole transport layer, and the specific examples thereof are not limited thereto.
Based on the same conception, the present application also provides a method for preparing an optoelectronic device, fig. 3 shows a method for preparing a positive structure of the optoelectronic device according to the embodiment of the present application, and as shown in fig. 3, the method for preparing an optoelectronic device with a positive structure includes the following steps:
s10, preparing a hole transport layer on an anode, wherein the hole transport layer contains P (VDF-HFP) and/or NETMS;
s20, preparing a light-emitting layer on the hole transport layer; and
s30, preparing a cathode on the light-emitting layer to obtain the photoelectric device.
Fig. 4 shows a method for preparing an inversion structure of an optoelectronic device according to an embodiment of the present application, where, as shown in fig. 4, the method for preparing an inversion structure of an optoelectronic device includes the following steps:
s100, preparing a light-emitting layer on a cathode;
s200, preparing a hole transport layer on the light-emitting layer, wherein the hole transport layer contains P (VDF-HFP) and/or NETMS; and
S300, preparing an anode on the hole transport layer to obtain the photoelectric device.
In the embodiment of the present invention, the preparation method of the hole transport layer may be implemented by a method known in the art, and as an exemplary embodiment, the preparation method may be implemented by a solution method, which may greatly reduce the production cost, for mass production, and the solution method may include a spin coating method, a printing method, an inkjet printing method, a doctor blade method, a printing method, a dip-coating method, a dipping method, a spraying method, a roll coating method, a casting method, a slit coating method, and a bar coating method. In a specific embodiment, when the preparation method of the hole transport layer is spin coating, the rotation speed in the spin coating process is not limited additionally, but the thickness of the film layer is affected by the rotation speed and the solution concentration, and the thickness of the film layer can be controlled by controlling the rotation speed and the concentration. In a specific embodiment, the spin-coating is performed at a speed of 2500r/min (revolutions/min) for 30 seconds, the solvent is chlorobenzene, and the thickness of the hole-transporting layer is 28nm when the concentration of the mixed solution is 10mg/mL, the thickness of the layer is 25nm when the concentration is 8mg/mL, and the thickness of the layer is 22nm when the concentration is 6 mg/mL.
In some embodiments, the hole transport layer is prepared by:
(1) Mixing polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxy silane, a first hole transport material and an organic solvent to obtain a mixed solution; and
(2) And forming a film on the light-emitting layer or the anode by the mixed solution, and drying to obtain the hole transport layer.
Because the concentration of the solution affects the thickness of the device, in order to obtain better device performance, in some embodiments, the concentration of the first hole transporting material in the mixed solution ranges from 6mg/mL to 10mg/mL. In other embodiments, the first hole transport material concentration may be below 8mg/mL, for example 6mg/mL to 8mg/mL, for further achieving better device performance. In a common device, when the concentration of the hole transport layer is reduced to below 8mg/mL, the device has a larger leakage current problem, and after a certain proportion of P (VDF-HFP) and/or NETMS is added, the concentration of the hole transport layer is reduced to 6mg/mL under the same conditions, so that the device performance can be kept better.
In some embodiments, the concentration ratio of P (VDF-HFP) and NETMS in the mixed solution is (1-3): (1-2), the specific concentration ratio is (2-3): 1, e.g., 2.5:1, p (VDF-HFP) and NETMS may both achieve adjustment of the dielectric constants of the mixed solution, but in some embodiments, when the ratio of the two is (2-3): 1, the injection level of the hole transport layer is better; the P (VDF-HFP) material can effectively regulate hole injection, and reduce the injection barrier of carriers through the interface dipole effect, but introducing too much P (VDF-HFP) material can cause leakage current problem of the device. The dielectric constant of the hole transport layer can be adjusted by introducing NETMS, the moisture absorption problem of the device can be effectively avoided, the stability of the device is protected, and the conductivity of the device can be influenced by introducing too much NETMS. It is understood that the concentration ratio of P (VDF-HFP) to NETMS may be (1-3): any value within the range of (1-2), for example: 3: 1. 2: 1. 1: 1. 1:2, or (1 to 3): other values not listed in the range of (1-2).
In some embodiments, the ratio of the total concentration of P (VDF-HFP) and/or NETMS to the concentration of the first hole transport material in the mixed solution is 1: (2.5 to 5), in particular, the mass ratio is 1: (4-5), for example 1:4. if the total concentration of P (VDF-HFP) and/or NETMS is too high, the conductivity of the hole transport layer is affected, so that the device turn-on voltage is easily increased dramatically, and the dielectric constant of the solution cannot be adjusted too low. It is understood that the ratio of the total concentration of P (VDF-HFP) and/or NETMS to the concentration of the first hole transport material may be 1: any value within the range of (2.5 to 5), for example: 1:2.5, 1:3. 1:3.5, 1:4. 1:4.5, 1:5, etc., or 1: other values not listed in the range of (2.5-5).
In some embodiments, the organic solvent is chlorobenzene.
Based on the same conception, the application also provides an optoelectronic device, which comprises any one of the optoelectronic devices or the optoelectronic device prepared by the preparation method, and the structure, the implementation principle and the effect of the optoelectronic device are similar, and are not repeated herein. In a specific embodiment, the optoelectronic device is a QLED.
Alternatively, the optoelectronic device may be: the lighting lamp and the backlight source are any products or components with display functions, such as mobile phones, tablet computers, televisions, displays, notebook computers, digital photo frames, navigator and the like.
It should be noted that, the drawings relate to only the structures related to the embodiments of the present application, and other structures may refer to the general designs.
In addition, for a better understanding of the present application, the present application also provides the following specific examples.
Example 1:
embodiment 1 provides an optoelectronic device, the method of making the optoelectronic device comprising the steps of:
(1) Placing the ITO glass sheet into a glass dish filled with ethanol solution, sequentially carrying out ultrasonic treatment on the ITO glass sheet by using acetone, deionized water and ethanol for 20 minutes, and drying by using a nitrogen gun; finally, placing the cleaned ITO glass sheet in oxygen plasma for further cleaning for 10 minutes; the surface of the ITO substrate was treated with ultraviolet-ozone for 15 minutes.
(2) The cleaned ITO glass sheet is spin-coated with PEDOT PSS in air at 4000r/min. Spin coating time was 30 seconds; after spin coating, placing in air for annealing at 150 ℃ for 30 minutes; after the annealing was completed, the tablets were quickly transferred to a glove box under nitrogen atmosphere.
(3) Continuously spin-coating the glass/ITO/PEDOT PSS chip with the mixed solution to form a hole transport layer, wherein the rotation speed is 2500r/min, and the spin-coating time is 30 seconds; annealing in a glove box after spin coating is completed, wherein the annealing temperature is 180 ℃ and the annealing time is 25 minutes.
(4) Spin-coating a quantum dot solution after finishing annealing the sheet of the glass/ITO/PEDOT/PSS/TFB, wherein the spin-coating rotating speed is 2000r/min, and the spin-coating time is 30 seconds; annealing in a glove box after spin coating is finished, wherein the annealing temperature is 60 ℃ and the annealing time is 10 minutes; the blue quantum dot material structure used in the examples is: cd (cadmium sulfide) 0.10 Zn 0.9 Se/Cd 0.05 Zn 0.95 Se/CdZnS/CdS。
(5) The glass/ITO/PEDOT PSS/TFB/QDs chips were spin coated with the electron transport layer solution at 3000r/min for 30 seconds.
(6) Placing the prepared sample slice into a vacuum cavity, and evaporating a top silver electrode; the thickness of the silver electrode was 100nm.
Wherein, the mixed solution in this example was added with a solution containing P (VDF-HFP) and NETMS at appropriate concentrations. The preparation method of the P (VDF-HFP) and NETMS solution comprises the following steps: an amount of P (VDF-HFP) was dispersed in chlorobenzene, stirred at 60℃to give 5mg/mL of a solution of P (VDF-HFP), and an amount of NETMS was dispersed in the solution of P (VDF-HFP), and the solutions of P (VDF-HFP) and NETMS were vigorously stirred. The first hole transport material was TFB, and the concentration of TFB in the mixed solution was 8mg/mL. The mass ratio of P (VDF-HFP) to NETMS is: the mass ratio of the total mass of P (VDF-HFP) and NETMS to the first hole transport material was 1:4.
Example 2:
this example is substantially identical to example 1, except that the mass ratio of P (VDF-HFP) to NETMS in this example is 2.5:1.
Example 3:
this example is substantially identical to example 1, except that the mass ratio of P (VDF-HFP) to NETMS in this example is 2:1.
Example 4:
this example is substantially identical to example 1, except that the mass ratio of P (VDF-HFP) to NETMS in this example is 1:1.
Example 5:
this example is substantially identical to example 1, except that the mass ratio of P (VDF-HFP) to NETMS in this example is 1:2.
Example 6:
this example is substantially the same as example 1, except that the TFB concentration in this example is 10mg/mL and the mass ratio of P (VDF-HFP) to NETMS is 2.5:1.
Example 7
This example is substantially the same as example 1, except that the TFB concentration in this example is 6mg/mL and the mass ratio of P (VDF-HFP) to NETMS is 2.5:1.
Comparative example 1:
this comparative example differs from example 1 in that no P (VDF-HFP) and NETMS were added, providing a total of three photovoltaic devices with TFB concentrations of 10mg/mL, 8mg/mL, 6mg/mL, respectively.
Comparative example 2
This comparative example differs from example 1 in that only P (VDF-HFP) was added in the comparative example.
Comparative example 3
This comparative example differs from example 1 in that only NETMS was added to the comparative example.
Comparative example 4:
this comparative example provides two optoelectronic devices that differ from example 1 in that the mass ratio of P (VDF-HFP) to NETMS is 2.5:1, and the mass ratio of P (VDF-HFP) and NETMS to the first hole transport material is 1:2 and 1:5.
performance test:
the results of the test are shown in Table 1, FIGS. 5-9, wherein:
(1) External Quantum Efficiency (EQE): measured using an EQE optical test instrument.
(2) Life span: to a constant current density (2 mA/cm) 2 ) The time taken for the lower device brightness to drop to 95% of its original brightness (converted to 1000 nit brightness).
(3) Dielectric constant test: and (3) measuring by adopting a QS87 dielectric loss and dielectric constant measuring system.
(4) Comparison of electron injection size: the current density-voltage curve of a single carrier transport thin film device (HOD/EOD), which is anode/light emitting layer/electron transport layer/cathode (electron injection size), was tested and the current density at the operating voltage (8V) of the device was compared, and HOD, which is anode/hole transport layer/light emitting layer/cathode (hole injection size).
The devices used for external quantum efficiency testing and lifetime testing were complete devices, namely: anode/hole function layer/light emitting layer/electron function layer/cathode.
TABLE 1
Figure BDA0003451905160000161
TABLE 2
Figure BDA0003451905160000162
As can be seen from the experimental data of examples 1 to 7 and comparative examples 1 to 3 in Table 1, the dielectric constant of the hole transport layer was increased by adding different proportions of P (VDF-HFP) and NETMS, the hole injection of the device was increased (HOD device current density-summarized in Table 1), which is also demonstrated in FIGS. 5 to 8, and the measured EOD device current density was 249.89mA cm -2 It is shown that the electron injection is more similar to that in example 7, so that the carrier injection in the scheme of example 7 is more balanced, and the luminous efficiency and the service life of the device are more excellent.
As can be seen from examples 1 and 5, the external quantum efficiency and lifetime of the device of example 2 are better, indicating that when the mass ratio of P (VDF-HFP) and NETMS is (2-3): 1, especially 2.5:1, the device performance is better, the content of P (VDF-HFP) or NETMS in example 1, example 3-example 5 is more than that in example 2, the device performance begins to decrease although the dielectric constant is further increased, which indicates that adding too much P (VDF-HFP) or NETMS can lead to decrease in device conductivity, decrease in device carrier injection and decrease in device luminous efficiency.
From comparison of comparative example 1 with comparative example 2 and comparative example 3, it can be seen that the performance of the device is improved by adding either P (VDF-HFP) or NETMS alone in the first hole transport material, but the efficiency and lifetime are inferior to those of examples 1 to 7, for example, comparative example 2 and example 1 are compared, and although the total mass ratio of P (VDF-HFP) and/or NETMS to the first hole transport material is 1:4 in comparative example 2 and example 1, only P (VDF-HFP) is added in comparative example 2, the efficiency and lifetime are 12.1% and 125h, respectively, whereas example 1 improves to 13.6% and 143h after P (VDF-HFP) and NETMS are added, indicating that both are used together with a synergistic effect, which can further improve the device performance.
It can be seen from examples 2, 6, 7 and comparative example 1 that the concentration of TFB was too high or too low without adding the materials of this protocol, and the device performance was reduced, but the optimal concentration of TFB could be further reduced to 6mg/mL after adding the materials of this protocol.
Further, as can be confirmed from table 2 and fig. 9, when the mass ratio of the total mass of P (VDF-HFP) and NETMS to the first hole transport material is 1: (2.5 to 5), for example, 1: in the range of (4 to 5), in particular 1:4, the performance of the device is better, because excessive content of P (VDF-HFP) and NETMS can cause the conductivity of the device to be greatly reduced, thereby severely limiting the hole injection performance of the device; too low is unfavorable for controlling hole injection of the device, and the hole injection is still low, so that the unbalance of carrier injection of the device is caused, and the performance of the device is influenced.
The above describes in detail an optoelectronic device, a method for manufacturing the same, and an optoelectronic device provided in the embodiments of the present application, and specific examples are applied herein to illustrate the principles and embodiments of the present application, where the above description of the embodiments is only for helping to understand the method and core ideas of the present application; meanwhile, those skilled in the art will have variations in the specific embodiments and application scope in light of the ideas of the present application, and the present description should not be construed as limiting the present application in view of the above.

Claims (14)

1. An optoelectronic device comprising a cathode, an anode, and a light-emitting layer and a hole-transporting layer arranged between the cathode and the anode, wherein the hole-transporting layer is arranged close to the anode, and the light-emitting layer is arranged close to the cathode.
2. The photovoltaic device according to claim 1, wherein the hole transport layer contains polyvinylidene fluoride co-hexafluoropropylene and 2-cyanoethyltrimethoxysilane in a mass ratio of (1 to 3): (1-2).
3. The optoelectronic device according to claim 2, wherein the mass ratio of the polyvinylidene fluoride co-hexafluoropropylene and the 2-cyanoethyltrimethoxysilane is (2-3): 1.
4. An optoelectronic device according to claim 1, wherein the total mass ratio of polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane in the hole transport layer is 17% to 29%.
5. The photovoltaic device according to claim 4, wherein the total mass ratio of polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane in the hole transport layer is 17% to 20%.
6. The optoelectronic device of claim 1, wherein the hole transport layer has a thickness of 22nm to 28nm.
7. The optoelectronic device of claim 6, wherein the hole transport layer has a thickness of 22nm to 25nm.
8. An optoelectronic device according to claim 1, wherein the hole transport layer is composed of the first hole transport material, and polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyltrimethoxysilane.
9. The optoelectronic device of claim 8, wherein the material of the light emitting layer comprises quantum dots selected from at least one of single structure quantum dots selected from at least one of group II-VI compounds, group III-V compounds, and group I-III-VI compounds selected from at least one of CdSe, cdS, cdTe, znO, znSe, znS, cdTe, znTe, hgS, hgSe, hgTe, cdZnS, cdZnSe, cdZnTe, znSeS, znSeTe, znTeS, cdSeS, cdSeTe, cdTeS, cdZnSeS, cdZnSeTe and CdZnSTe, and core-shell structure quantum dots selected from at least one of InP, inAs, gaP, gaAs, gaSb, inSb, alAs, alN, alP, inAsP, inNP, inNSb, gaAlNP and InAlNP; the I-III-VI compound is selected from CuInS 2 、CuInSe 2 AgInS 2 The core of the quantum dot with the core-shell structure is selected from any one of the quantum dots with the single structure, and the shell material of the quantum dot with the core-shell structure is selected from at least one of CdS, cdTe, cdSeTe, cdZnSe, cdZnS, cdSeS, znSe, znSeS and ZnS; andand/or,
the first hole transport material is selected from: at least one of N, N '-dinaphthyl-N, N' -diphenyl benzidine, N '-bis- (3-methylphenyl) -N, N' -bis- (phenyl) -benzidine), 4',4 "-tris (N-3-methylphenyl-N-phenyl-amino) -triphenylamine, poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine), polyvinylcarbazole, poly (N, N' -bis (4-butylphenyl) -N, N '-bis (phenyl) benzidine) or 4,4',4" -tris (carbazol-9-yl) triphenylamine; and/or the number of the groups of groups,
the cathode material is selected from: at least one of an Ag electrode, an Al electrode, an Au electrode, a Pt electrode, or an alloy electrode; and/or the anode material is selected from a metal oxide electrode or a composite electrode, wherein the metal oxide electrode is selected from at least one of ITO, FTO, ATO, AZO, GZO, 1ZO, MZO and AMO, and the composite electrode is AZO/Ag/AZO, AZO/Al/AZO, ITO/Ag/ITO, ITO/Al/ITO, znO/Ag/ZnO, znO/Al/ZnO, tiO 2 /Ag/TiO 2 、TiO 2 /Al/TiO 2 At least one of ZnS/Ag/ZnS or ZnS/Al/ZnS.
10. The optoelectronic device according to claim 1, wherein a hole injection layer is further provided between the anode and the hole transport layer, and wherein a material of the hole injection layer is selected from the group consisting of: poly (ethylenedioxythiophene): polystyrene sulfonate, poly (9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine), polyarylamine, poly (N-vinylcarbazole), polyaniline, polypyrrole, N, N, N ', N' -tetra (4-methoxyphenyl) -benzidine, 4-bis [ N- (1-naphthyl) -N-phenyl-amino ] biphenyl, 4 '-tris [ phenyl (m-tolyl) amino ] triphenylamine, 4', at least one of 4 "-tris (N-carbazolyl) -triphenylamine, 1-bis [ (di-4-tolylamino) phenylcyclohexane, 4',4" -tris (diphenylamino) triphenylamine doped with tetrafluoro-tetracyano-quinone dimethane, p-doped phthalocyanine, F4-TCNQ doped N, N' -diphenyl-N, N '-bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine or hexaazabenzophenanthrene-hexanenitrile.
11. A method of fabricating an optoelectronic device comprising the steps of:
preparing a hole transport layer on the anode;
preparing a light emitting layer on the hole transport layer; and
Preparing a cathode on the light-emitting layer to obtain the photoelectric device; or alternatively, the process may be performed,
preparing a light emitting layer on a cathode;
preparing a hole transport layer on the light emitting layer; and
preparing an anode on the hole transport layer to obtain the photoelectric device;
wherein the hole transport layer contains polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxysilane.
12. The method of manufacturing according to claim 11, wherein the hole transport layer is manufactured by: mixing polyvinylidene fluoride co-hexafluoropropylene and/or 2-cyanoethyl trimethoxy silane, a first hole transport material and an organic solvent to obtain a mixed solution; and
and forming a film on the light-emitting layer or the anode by the mixed solution, and drying to obtain the hole transport layer.
13. The production method according to claim 12, wherein the concentration ratio of the polyvinylidene fluoride co-hexafluoropropylene and the 2-cyanoethyltrimethoxysilane in the mixed solution is (1 to 3): (1-2); and/or the ratio of the total concentration of the polyvinylidene fluoride co-hexafluoropropylene and/or the 2-cyanoethyl trimethoxysilane to the concentration of the first hole transport material is 1: (2.5-5); and/or the concentration of the first hole transport material is 6mg/mL to 10mg/mL; and/or the organic solvent is chlorobenzene.
14. An optoelectronic apparatus comprising an optoelectronic device according to any one of claims 1 to 10, or an optoelectronic device prepared by the preparation method according to any one of claims 11 to 13.
CN202111675725.7A 2021-12-31 2021-12-31 Photoelectric device, preparation method thereof and photoelectric device Pending CN116437687A (en)

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