CN118265334A - Electroluminescent device, preparation method thereof and display device - Google Patents
Electroluminescent device, preparation method thereof and display device Download PDFInfo
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- CN118265334A CN118265334A CN202211700515.3A CN202211700515A CN118265334A CN 118265334 A CN118265334 A CN 118265334A CN 202211700515 A CN202211700515 A CN 202211700515A CN 118265334 A CN118265334 A CN 118265334A
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- 238000002360 preparation method Methods 0.000 title claims abstract description 16
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 124
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 124
- 239000000463 material Substances 0.000 claims abstract description 68
- 239000010410 layer Substances 0.000 claims description 196
- 239000002096 quantum dot Substances 0.000 claims description 53
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 38
- 150000001875 compounds Chemical class 0.000 claims description 34
- 239000002346 layers by function Substances 0.000 claims description 34
- 229910052950 sphalerite Inorganic materials 0.000 claims description 29
- 229910052984 zinc sulfide Inorganic materials 0.000 claims description 29
- 238000002347 injection Methods 0.000 claims description 28
- 239000007924 injection Substances 0.000 claims description 28
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims description 24
- -1 4-butylphenyl Chemical group 0.000 claims description 23
- 239000004065 semiconductor Substances 0.000 claims description 18
- 239000002245 particle Substances 0.000 claims description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 15
- 229920003227 poly(N-vinyl carbazole) Polymers 0.000 claims description 15
- 239000002131 composite material Substances 0.000 claims description 12
- 229910052751 metal Inorganic materials 0.000 claims description 12
- 239000002184 metal Substances 0.000 claims description 12
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- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 claims description 10
- 239000007772 electrode material Substances 0.000 claims description 10
- 229920000553 poly(phenylenevinylene) Polymers 0.000 claims description 10
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- 239000011258 core-shell material Substances 0.000 claims description 9
- 229920001467 poly(styrenesulfonates) Polymers 0.000 claims description 9
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- 229920000128 polypyrrole Polymers 0.000 claims description 9
- SBIBMFFZSBJNJF-UHFFFAOYSA-N selenium;zinc Chemical compound [Se]=[Zn] SBIBMFFZSBJNJF-UHFFFAOYSA-N 0.000 claims description 9
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims description 8
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 8
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 8
- 229910001632 barium fluoride Inorganic materials 0.000 claims description 8
- 229910052737 gold Inorganic materials 0.000 claims description 8
- 150000004767 nitrides Chemical class 0.000 claims description 8
- 229910052710 silicon Inorganic materials 0.000 claims description 8
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- 125000001637 1-naphthyl group Chemical group [H]C1=C([H])C([H])=C2C(*)=C([H])C([H])=C([H])C2=C1[H] 0.000 claims description 5
- IXHWGNYCZPISET-UHFFFAOYSA-N 2-[4-(dicyanomethylidene)-2,3,5,6-tetrafluorocyclohexa-2,5-dien-1-ylidene]propanedinitrile Chemical compound FC1=C(F)C(=C(C#N)C#N)C(F)=C(F)C1=C(C#N)C#N IXHWGNYCZPISET-UHFFFAOYSA-N 0.000 claims description 5
- AWXGSYPUMWKTBR-UHFFFAOYSA-N 4-carbazol-9-yl-n,n-bis(4-carbazol-9-ylphenyl)aniline Chemical compound C12=CC=CC=C2C2=CC=CC=C2N1C1=CC=C(N(C=2C=CC(=CC=2)N2C3=CC=CC=C3C3=CC=CC=C32)C=2C=CC(=CC=2)N2C3=CC=CC=C3C3=CC=CC=C32)C=C1 AWXGSYPUMWKTBR-UHFFFAOYSA-N 0.000 claims description 5
- ZOKIJILZFXPFTO-UHFFFAOYSA-N 4-methyl-n-[4-[1-[4-(4-methyl-n-(4-methylphenyl)anilino)phenyl]cyclohexyl]phenyl]-n-(4-methylphenyl)aniline Chemical compound C1=CC(C)=CC=C1N(C=1C=CC(=CC=1)C1(CCCCC1)C=1C=CC(=CC=1)N(C=1C=CC(C)=CC=1)C=1C=CC(C)=CC=1)C1=CC=C(C)C=C1 ZOKIJILZFXPFTO-UHFFFAOYSA-N 0.000 claims description 5
- DIVZFUBWFAOMCW-UHFFFAOYSA-N 4-n-(3-methylphenyl)-1-n,1-n-bis[4-(n-(3-methylphenyl)anilino)phenyl]-4-n-phenylbenzene-1,4-diamine Chemical compound CC1=CC=CC(N(C=2C=CC=CC=2)C=2C=CC(=CC=2)N(C=2C=CC(=CC=2)N(C=2C=CC=CC=2)C=2C=C(C)C=CC=2)C=2C=CC(=CC=2)N(C=2C=CC=CC=2)C=2C=C(C)C=CC=2)=C1 DIVZFUBWFAOMCW-UHFFFAOYSA-N 0.000 claims description 5
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 5
- 229910004613 CdTe Inorganic materials 0.000 claims description 5
- 101000837344 Homo sapiens T-cell leukemia translocation-altered gene protein Proteins 0.000 claims description 5
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- 229920002098 polyfluorene Polymers 0.000 claims description 5
- 229910021649 silver-doped titanium dioxide Inorganic materials 0.000 claims description 5
- SPDPTFAJSFKAMT-UHFFFAOYSA-N 1-n-[4-[4-(n-[4-(3-methyl-n-(3-methylphenyl)anilino)phenyl]anilino)phenyl]phenyl]-4-n,4-n-bis(3-methylphenyl)-1-n-phenylbenzene-1,4-diamine Chemical compound CC1=CC=CC(N(C=2C=CC(=CC=2)N(C=2C=CC=CC=2)C=2C=CC(=CC=2)C=2C=CC(=CC=2)N(C=2C=CC=CC=2)C=2C=CC(=CC=2)N(C=2C=C(C)C=CC=2)C=2C=C(C)C=CC=2)C=2C=C(C)C=CC=2)=C1 SPDPTFAJSFKAMT-UHFFFAOYSA-N 0.000 claims description 4
- QZTQQBIGSZWRGI-UHFFFAOYSA-N 2-n',7-n'-bis(3-methylphenyl)-2-n',7-n'-diphenyl-9,9'-spirobi[fluorene]-2',7'-diamine Chemical compound CC1=CC=CC(N(C=2C=CC=CC=2)C=2C=C3C4(C5=CC=CC=C5C5=CC=CC=C54)C4=CC(=CC=C4C3=CC=2)N(C=2C=CC=CC=2)C=2C=C(C)C=CC=2)=C1 QZTQQBIGSZWRGI-UHFFFAOYSA-N 0.000 claims description 4
- HONWGFNQCPRRFM-UHFFFAOYSA-N 2-n-(3-methylphenyl)-1-n,1-n,2-n-triphenylbenzene-1,2-diamine Chemical compound CC1=CC=CC(N(C=2C=CC=CC=2)C=2C(=CC=CC=2)N(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 HONWGFNQCPRRFM-UHFFFAOYSA-N 0.000 claims description 4
- WPUSEOSICYGUEW-UHFFFAOYSA-N 4-[4-(4-methoxy-n-(4-methoxyphenyl)anilino)phenyl]-n,n-bis(4-methoxyphenyl)aniline Chemical compound C1=CC(OC)=CC=C1N(C=1C=CC(=CC=1)C=1C=CC(=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC=C(OC)C=C1 WPUSEOSICYGUEW-UHFFFAOYSA-N 0.000 claims description 4
- NHCDCRWRKBUWEC-UHFFFAOYSA-N 4-methyl-n-(4-methylphenyl)-n-(1-phenylcyclohexyl)aniline Chemical compound C1=CC(C)=CC=C1N(C1(CCCCC1)C=1C=CC=CC=1)C1=CC=C(C)C=C1 NHCDCRWRKBUWEC-UHFFFAOYSA-N 0.000 claims description 4
- LZSJBLXYNYSKPJ-UHFFFAOYSA-N 9-octyl-9h-fluorene Chemical compound C1=CC=C2C(CCCCCCCC)C3=CC=CC=C3C2=C1 LZSJBLXYNYSKPJ-UHFFFAOYSA-N 0.000 claims description 4
- 229910017676 MgTiO3 Inorganic materials 0.000 claims description 4
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 4
- 229910002113 barium titanate Inorganic materials 0.000 claims description 4
- 229910021523 barium zirconate Inorganic materials 0.000 claims description 4
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- 229910052593 corundum Inorganic materials 0.000 claims description 4
- CJNBYAVZURUTKZ-UHFFFAOYSA-N hafnium(IV) oxide Inorganic materials O=[Hf]=O CJNBYAVZURUTKZ-UHFFFAOYSA-N 0.000 claims description 4
- RBTKNAXYKSUFRK-UHFFFAOYSA-N heliogen blue Chemical compound [Cu].[N-]1C2=C(C=CC=C3)C3=C1N=C([N-]1)C3=CC=CC=C3C1=NC([N-]1)=C(C=CC=C3)C3=C1N=C([N-]1)C3=CC=CC=C3C1=N2 RBTKNAXYKSUFRK-UHFFFAOYSA-N 0.000 claims description 4
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 claims description 4
- 229910052750 molybdenum Inorganic materials 0.000 claims description 4
- IBHBKWKFFTZAHE-UHFFFAOYSA-N n-[4-[4-(n-naphthalen-1-ylanilino)phenyl]phenyl]-n-phenylnaphthalen-1-amine Chemical compound C1=CC=CC=C1N(C=1C2=CC=CC=C2C=CC=1)C1=CC=C(C=2C=CC(=CC=2)N(C=2C=CC=CC=2)C=2C3=CC=CC=C3C=CC=2)C=C1 IBHBKWKFFTZAHE-UHFFFAOYSA-N 0.000 claims description 4
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- YBNMDCCMCLUHBL-UHFFFAOYSA-N (2,5-dioxopyrrolidin-1-yl) 4-pyren-1-ylbutanoate Chemical compound C=1C=C(C2=C34)C=CC3=CC=CC4=CC=C2C=1CCCC(=O)ON1C(=O)CCC1=O YBNMDCCMCLUHBL-UHFFFAOYSA-N 0.000 claims description 3
- ZMEAEUNNMHQAJK-UHFFFAOYSA-N 2-[3-[3-[2,2-diphenylethyl-[(4-methoxyphenyl)methyl]amino]propoxy]phenyl]acetamide Chemical compound C1=CC(OC)=CC=C1CN(CC(C=1C=CC=CC=1)C=1C=CC=CC=1)CCCOC1=CC=CC(CC(N)=O)=C1 ZMEAEUNNMHQAJK-UHFFFAOYSA-N 0.000 claims description 3
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- WLKLBMLIJRMZJS-UHFFFAOYSA-N 6-(3,4,5,16,17,18-hexazatetracyclo[12.4.0.02,7.08,13]octadeca-1(18),2,4,6,8,10,12,14,16-nonaen-6-yl)hexanenitrile Chemical compound C1(=NN=NC=2C3=NN=NC=C3C3=CC=CC=C3C1=2)CCCCCC#N WLKLBMLIJRMZJS-UHFFFAOYSA-N 0.000 claims description 3
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Abstract
The invention provides an electroluminescent device, a preparation method thereof and a display device, and relates to the technical field of display. The electroluminescent device includes: a first electrode and a second electrode disposed opposite to each other; at least two light emitting units, which are sequentially stacked between the first electrode and the second electrode; and at least one charge generation layer, each charge generation layer is respectively arranged between two adjacent light emitting units, the material of the charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV. The charge generation layer in the electroluminescent device provided by the invention has high charge generation efficiency and good device performance.
Description
Technical Field
The invention relates to the technical field of display, in particular to an electroluminescent device, a preparation method thereof and a display device.
Background
The stacked structure in which light emitting cells including a light emitting layer are connected in series using a Charge Generation Layer (CGL) has advantages of high current efficiency and long operation life, and thus is widely used in the field of display technology. However, the charge generation efficiency of the charge generation layer in the existing stacked device is low, which greatly limits the development of the stacking technology.
Disclosure of Invention
The invention aims to provide an electroluminescent device, wherein the charge generation efficiency of a charge generation layer in the electroluminescent device is high, and the device performance is good.
Another object of the present invention is to provide a method for manufacturing an electroluminescent device.
It is still another object of the present invention to provide a display device.
The invention solves the technical problems by adopting the following technical scheme:
An electroluminescent device comprising:
A first electrode and a second electrode disposed opposite to each other;
At least two light emitting units, which are sequentially stacked between the first electrode and the second electrode; and
And at least one charge generation layer, each charge generation layer is respectively arranged between two adjacent light emitting units, the material of the charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV.
Alternatively, in some embodiments of the invention, the conduction band energy level of-5.0 eV.ltoreq.first metal oxide is.ltoreq.4.5 eV; and/or
-5.0EV < 4.5eV of conduction band energy level of the second metal oxide; and/or
-5.5EV is less than or equal to-4.5 eV of the valence band energy level of the third metal oxide; and/or
The first metal oxide is an n-type semiconductor; and/or
The third metal oxide is a p-type semiconductor.
Optionally, in some embodiments of the invention, the first metal oxide is selected from one or more of ZnO、Znx1Mgy1O、Znx1Aly1O、Znx2Mgy2Liz2O、SnO2、Znx1Sny1O, wherein x1+y1=1 or x2+y2+z2=1; and/or
The second metal oxide is selected from one or more of MnO 3、WO3; and/or
The third metal oxide is selected from one or more of NiO, snO, cuO.
Alternatively, in some embodiments of the invention, the first metal oxide is present in the charge generating layer material at a ratio of 10 to 40wt%; and/or
The second metal oxide accounts for 30-50wt% of the material of the charge generation layer; and/or
The third metal oxide accounts for 30-50wt% of the material of the charge generation layer.
Alternatively, in some embodiments of the invention, the charge generating layer has a thickness of 5 to 30nm; and/or
The average particle size of the first metal oxide, the second metal oxide and the third metal oxide is 3-15 nm respectively.
Alternatively, in some embodiments of the present invention, each light emitting unit independently includes: a light emitting layer; the material of the luminescent layer is selected from one or more of single-structure quantum dots, core-shell structure quantum dots, doped or undoped inorganic perovskite type quantum dots and organic-inorganic hybrid perovskite type quantum dots; Wherein the single-structure quantum dot is selected from one or more of II-VI compound, III-V compound, II-V compound, III-VI compound, IV-VI compound, I-III-VI compound, II-IV-VI compound and IV simple substance, the II-VI compound is selected from one or more of CdSe、CdS、CdTe、ZnSe、ZnS、CdTe、ZnTe、CdZnS、CdZnSe、CdZnTe、ZnSeS、ZnSeTe、ZnTeS、CdSeS、CdSeTe、CdTeS、CdZnSeS、CdZnSeTe、CdZnSTe, the III-V compound is selected from InP, inAs, gaP, gaAs, gaN, gaSb, AlN, alP, inAsP, inNP, inNSb, gaAlNP, inAlNP, wherein the IV-VI compound is selected from one or more of PbS and PbSe; The I-III-VI compound is selected from one or more of CuInS 2、CuInSe2、AgInS2; the IV group simple substance is selected from one or more of silicon and germanium; the core of the quantum dot with the core-shell structure is selected from any one of quantum dots with single structures, and the shell material of the quantum dot with the core-shell structure is selected from one or more of CdS, cdTe, cdSe, cdSeTe, cdZnSe, cdZnS, cdSeS, znSe, znTe, znSeS, znS; The structural general formula of the inorganic perovskite type quantum dot is AMX 3, wherein A is Cs +, M is one or more of Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+, and X is one or more of Cl -、Br-、I-; The organic-inorganic hybrid perovskite quantum dot has a structural general formula of BMX 3, wherein B is selected from one or more of CH 3(CH2)n-2NH3+、NH3(CH2)nNH3 2+, n is more than or equal to 2, M is selected from one or more of Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2 +、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+, and X is selected from one or more of Cl -、Br-、I-.
Optionally, in some embodiments of the present invention, each light emitting unit independently further includes:
the first charge functional layer is arranged on one side of the light-emitting layer, which is close to the first electrode; and
The second charge functional layer is arranged on one side of the light-emitting layer, which is close to the second electrode;
the first charge functional layer and the second charge functional layer respectively and independently comprise a charge injection layer and/or a charge transmission layer, and each charge generation layer is respectively arranged between the second charge functional layer of one light-emitting unit and the first charge functional layer of the other light-emitting unit.
Optionally, in some embodiments of the present invention, the material of the first electrode and the material of the second electrode are each independently selected from one or more of doped or undoped metal, carbon silicon material, doped or undoped metal oxide, and composite electrode material; wherein the doped or undoped metal is selected from one or more of Al、Ag、Cu、Mo、Au、Ba、Ca、Mg、Ni、Pt、Ir、Ca:Al、LiF:Ca、LiF:Al、BaF2:Al、CsF:Al、CaCO3:Al、BaF2:Ca:Al、Au:Mg、Ag:Mg; the carbon-silicon material is selected from one or more of silicon, graphite, carbon nano tube, graphene and carbon fiber; the doped or undoped metal oxide is selected from one or more of ITO, FTO, ATO, AZO, GZO, IZO, MZO, AMO, ITZO, ICO, snO 2、In2O3、Cd:ZnO、Ga:SnO2; the composite electrode material is selected from one or more of AZO/Ag/AZO、AZO/Al/AZO、ITO/Ag/ITO、ITO/Al/ITO、ZnO/Ag/ZnO、ZnO/Al/ZnO、TiO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS; and/or
The material of the charge injection layer is selected from Ca, ba, csF, csCO 3, PEIE, PEI, liF, naF, poly (ethylenedioxythiophene): polystyrene sulfonate, poly [9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine ], polyarylamine, poly (N-vinylcarbazole), polyaniline, polythiophene, polypyrrole, N, N, N ', N' -tetrakis (4-methoxyphenyl) -benzidine, 4-bis [ N- (1-naphthyl) -N-phenyl-amino ] biphenyl, 4 '-tris [ phenyl (m-tolyl) amino ] triphenylamine, 4', one or more of 4 "-tris (N-carbazolyl) -triphenylamine, 1-bis [ (di-4-tolylamino) phenylcyclohexane, tetrafluoro-tetracyano-quinone dimethane doped 4,4',4" -tris (diphenylamino) triphenylamine, p-doped phthalocyanine, F4-TCNQ doped N, N' -diphenyl-N, N '-bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine, hexaazabenzophenanthrene-hexanenitrile, metal oxides; and/or
The material of the charge transport layer is selected from one or more of doped or undoped oxides, doped or undoped semiconductor particles, nitrides, alq3, almq3, DVPBi, TAZ, OXD, PBD, BND, PV, CBP, alpha-NPD, TPD, spiro-TPD, DNTPD, TCTA, m-MTDATA, TAPC, TFB, poly-TPD, polyaniline, polyfluorene, polypyrrole, PPV, MEH-PPV, MOMO-PPV, copper phthalocyanine, aromatic tertiary amine, polynuclear aromatic tertiary amine, 4' -bis (p-carbazolyl) -1,1' -biphenyl compound, N ' -tetraarylbenzidine, PEDOT: PSS and derivatives thereof, PVK and derivatives thereof, polymethacrylate and derivatives thereof, poly (9, 9-octylfluorene) and derivatives thereof, poly (spirofluorene) and derivatives thereof, NPB, spironpb, HATCN; wherein the oxide is selected from one or more of TiO2、ZnO、ZrO2、SnO2、WO3、NiO、Ta2O3、HfO2、Al2O3、ZrSiO4、BaTiO3、BaZrO3、SrTiO3、MgTiO3、TiLiO、ZnAlO、ZnSnO、ZnLiO、InSnO, the semiconductor particles are selected from one or more of CdS, znSe, znS, the nitride is selected from Si 3N4, and the doping elements of the oxide and semiconductor particles are selected from one or more of Al, mg, in, li, ga, cd, cs, cu.
In addition, the preparation method of the electroluminescent device comprises the following steps:
Providing a first electrode;
Forming at least two light emitting cells and at least one charge generating layer on the first electrode; each charge generation layer is respectively arranged between two adjacent light emitting units, the material of each charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV; and
A second electrode is formed on the light emitting unit.
In addition, the display device comprises the electroluminescent device or the electroluminescent device prepared by the preparation method.
Compared with the prior art, the invention has the following beneficial effects: in the invention, the materials of the charge generation layer of the device comprise the first metal oxide, the second metal oxide and the third metal oxide, and the three metal oxides are properly matched based on the energy level of a conduction band/a valence band, so that the formed charge generation layer has higher charge generation efficiency, and the device comprising the charge generation layer has low starting voltage and high current efficiency.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings that are needed in the description of the embodiments will be briefly described below, it being obvious that the drawings in the following description are only some embodiments of the present invention, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
Fig. 1 is a schematic structural diagram of a quantum dot light emitting diode according to embodiment 1 of the present invention.
Wherein the reference numerals are summarized as follows:
a first electrode 101; a first hole injection layer 102; a first hole transport layer 103; a first light emitting layer 104; a first electron transport layer 105;
A charge generation layer 201;
a second hole transport layer 301; a second light emitting layer 302; a second electron transport layer 303; a second electrode 304.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to fall within the scope of the invention.
The technical scheme provided by the invention will be described in detail below. The following description of the embodiments is not intended to limit the preferred embodiments. In addition, in the description of the present invention, the term "comprising" means "including but not limited to". The terms "first," "second," "third," and the like are used merely as labels, and do not impose numerical requirements or on order of establishment. Various embodiments of the invention 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 invention; it is therefore to be understood that the range description has specifically disclosed all possible sub-ranges and individual values within that range.
The invention provides an electroluminescent device comprising:
A first electrode and a second electrode disposed opposite to each other;
At least two light emitting units, which are sequentially stacked between the first electrode and the second electrode; and
And at least one charge generation layer, each charge generation layer is respectively arranged between two adjacent light emitting units, the material of the charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV.
It should be noted that "between … …" includes the case where the boundary value is equal. Further, -5.0eV is less than or equal to-4.5 eV of conduction band energy level of the first metal oxide; -5.0eV < 4.5eV of conduction band energy level of the second metal oxide; -5.5eV is less than or equal to-4.5 eV of the valence band energy level of the third metal oxide.
At least two light emitting units are stacked light emitting units connected in series, and the at least two light emitting units are connected through a charge generating layer. The light emitting unit and the charge generating layer may be stacked. The average particle size of the first metal oxide, the second metal oxide, and the third metal oxide may be nano-scale.
The second metal oxide has a deep conduction band energy level, the third metal oxide has a shallow valence band energy level, and the charge generation layer comprises a plurality of metal oxides based on energy level matching, so that the charge generation layer has higher charge generation efficiency.
In some embodiments, the first metal oxide may be selected to have an electron transporting capability, and further, the first metal oxide is an n-type semiconductor. The first metal oxide having an electron transporting ability can rapidly transport electrons.
In some embodiments, the third metal oxide is a p-type semiconductor.
Further, the first metal oxide is selected from one or more of ZnO、Znx1Mgy1O、Znx1Aly1O、Znx2Mgy2Liz2O、SnO2、Znx1Sny1O, wherein x1+y1=1 or x2+y2+z2=1; the second metal oxide is selected from one or more of MnO 3、WO3; the third metal oxide is selected from one or more of NiO, snO, cuO.
In some embodiments, the first metal oxide is present in the charge generating layer material at a ratio of 10 to 40wt%, e.g., 10 to 20%, 15 to 30%, 30 to 40%; the proportion of the second metal oxide in the material of the charge generation layer is 30 to 50wt%, for example, 30 to 35%, 35 to 45%, 42 to 50%; the proportion of the third metal oxide in the material of the charge generation layer is 30 to 50wt%, for example, 30 to 35%, 35 to 45%, 42 to 50%.
In some embodiments, the charge generation layer has a thickness of 5 to 30nm, and may also be 10 to 15nm, 15 to 25nm, 22 to 30nm.
In some embodiments, the average particle size of the first metal oxide, the second metal oxide, and the third metal oxide is 3 to 15nm, respectively, and may be 5 to 9nm, 10 to 15nm.
The device types of the electroluminescent device provided by the invention are not limited to double-layer devices, three-layer devices, multi-layer devices, top emitter devices, bottom emitter devices, double-sided emitting devices, rigid devices, flexible devices, upright structure devices, inverted structure devices and the like. The electroluminescent device may be one of a quantum dot light emitting diode (QLED), an Organic Light Emitting Diode (OLED), a sub-millimeter light emitting diode (Mini LED), a Micro light emitting diode (Micro LED).
In some embodiments, each light emitting unit independently includes: and a light emitting layer. In the case of an electroluminescent device being a quantum dot light emitting diode, the light emitting layer may be a quantum dot light emitting layer. The material of the quantum dot luminescent layer can be one or more of red quantum dots, green quantum dots and blue quantum dots. The PL wavelength of the red quantum dot, the green quantum dot and the blue quantum dot material is 615-635 nm, 535-555 nm and 465-480 nm respectively. Further, the material of the light-emitting layer can be selected from one or more of single-structure quantum dots, core-shell structure quantum dots, doped or undoped inorganic perovskite type quantum dots and organic-inorganic hybrid perovskite type quantum dots; Wherein the single-structure quantum dot is selected from one or more of II-VI compound, III-V compound, II-V compound, III-VI compound, IV-VI compound, I-III-VI compound, II-IV-VI compound and IV simple substance, the II-VI compound is selected from one or more of CdSe、CdS、CdTe、ZnSe、ZnS、ZnTe、CdZnS、CdZnSe、CdZnTe、ZnSeS、ZnSeTe、ZnTeS、CdSeS、CdSeTe、CdTeS、CdZnSeS、CdZnSeTe、CdZnSTe, the III-V compound is selected from InP, inAs, gaP, gaAs, gaN, gaSb, AlN, alP, inAsP, inNP, inNSb, gaAlNP, inAlNP, wherein the IV-VI compound is selected from one or more of PbS and PbSe; The I-III-VI compound is selected from one or more of CuInS 2、CuInSe2、AgInS2; the IV group simple substance is selected from one or more of silicon and germanium; the core of the quantum dot with the core-shell structure is selected from any one of quantum dots with single structures, and the shell material of the quantum dot with the core-shell structure is selected from one or more of CdS, cdTe, cdSe, cdSeTe, cdZnSe, cdZnS, cdSeS, znSe, znTe, znSeS, znS; The structural general formula of the inorganic perovskite type quantum dot is AMX 3, wherein A is Cs +, M is one or more of Pb2+、Sn2+、Cu2+、Ni2 +、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+, and X is one or more of Cl -、Br-、I-; the organic-inorganic hybrid perovskite quantum dot has a structural general formula of BMX 3, wherein B is selected from one or more of CH 3(CH2)n-2NH3+、NH3(CH2)nNH3 2+, n is more than or equal to 2, M is selected from one or more of Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+, and X is selected from one or more of Cl -、Br-、I-. the light emitting layer may have a thickness of 10 to 50 nm.
In some embodiments, each light emitting unit independently further comprises:
the first charge functional layer is arranged on one side of the light-emitting layer, which is close to the first electrode; and
The second charge functional layer is arranged on one side of the light-emitting layer, which is close to the second electrode;
the first charge functional layer and the second charge functional layer respectively and independently comprise a charge injection layer and/or a charge transmission layer, and each charge generation layer is respectively arranged between the second charge functional layer of one light-emitting unit and the first charge functional layer of the other light-emitting unit.
In some embodiments, the first electrode is an anode, the first charge functional layer is a hole functional layer, the second charge functional layer is an electron functional layer, and the second electrode is a cathode. In other embodiments, the first electrode may be a cathode, and the first charge functional layer is an electron functional layer, the second charge functional layer is a hole functional layer, and the second electrode is an anode.
Further, since the first charge functional layer and the second charge functional layer respectively and independently include the charge injection layer and/or the charge transport layer, for example, if the first charge functional layer is a hole functional layer, the first charge functional layer may include the hole injection layer and/or the hole transport layer; if the second charge functional layer is an electron functional layer, the second charge functional layer may include an electron injection layer and/or an electron transport layer.
In some embodiments, the material of the first electrode and the material of the second electrode are each independently selected from one or more of doped or undoped metal, carbon silicon material, doped or undoped metal oxide, and composite electrode material; wherein the doped or undoped metal is selected from one or more of Al、Ag、Cu、Mo、Au、Ba、Ca、Mg、Ni、Pt、Ir、Ca:Al、LiF:Ca、LiF:Al、BaF2:Al、CsF:Al、CaCO3:Al、BaF2:Ca:Al、Au:Mg、Ag:Mg; the carbon-silicon material is selected from one or more of silicon, graphite, carbon nano tube, graphene and carbon fiber; the doped or undoped metal oxide is selected from one or more of ITO, FTO, ATO, AZO, GZO, IZO, MZO, AMO, ITZO, ICO, snO 2、In2O3、Cd:ZnO、Ga:SnO2; the composite electrode material is selected from one or more of AZO/Ag/AZO、AZO/Al/AZO、ITO/Ag/ITO、ITO/Al/ITO、ZnO/Ag/ZnO、ZnO/Al/ZnO、TiO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS.
Further, in the case that the first electrode or the second electrode is an anode, the material of the anode may be selected from one or more of doped or undoped metal oxide, carbon silicon material, metal, and composite electrode material; wherein the doped or undoped metal oxide is selected from one or more of ITO, FTO, ATO, IZO, ITZO, ICO, snO 2、In2O3、Cd:ZnO、Ga:SnO2, AZO, GZO, MZO, AMO; the carbon-silicon material is selected from one or more of silicon, graphite, carbon nano tube, graphene and carbon fiber; the metal is selected from one or more of Al, ag, cu, mo, au, ba, ca, mg; the composite electrode material is selected from one or more of AZO/Ag/AZO、AZO/Al/AZO、ITO/Ag/ITO、ITO/Al/ITO、ZnO/Ag/ZnO、ZnO/Al/ZnO、TiO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS, i.e., the anode may be a composite electrode with metal sandwiched between doped or undoped metal oxides.
In the case that the first electrode or the second electrode is a cathode, the material of the cathode may be selected from one or more of doped or undoped metal, carbon silicon material, doped or undoped metal oxide, and composite electrode material; wherein the doped or undoped metal is selected from one or more of Al、Ag、Cu、Mo、Au、Ba、Ca、Mg、Pt、Ca:Al、LiF:Ca、LiF:Al、BaF2:Al、CsF:Al、CaCO3:Al、BaF2:Ca:Al、Au:Mg、Ag:Mg, and the doped metal electrode is an alloy electrode; the carbon-silicon material is selected from one or more of silicon, graphite, carbon nano tube, graphene and carbon fiber; the doped or undoped metal oxide is selected from one or more of ITO, FTO, ATO, AZO, GZO, IZO, MZO, AMO; the composite electrode material is selected from one or more of AZO/Ag/AZO、AZO/Al/AZO、ITO/Ag/ITO、ITO/Al/ITO、ZnO/Ag/ZnO、ZnO/Al/ZnO、TiO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS, i.e. the cathode may be a composite electrode of AZO/Ag/AZO, AZO/Al/AZO, for example. The thickness of the cathode may be 80 to 500nm.
The material of the charge injection layer is selected from Ca, ba, csF, csCO 3, PEIE, PEI, liF, naF, poly (ethylenedioxythiophene): polystyrene sulfonate, poly [9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine ], polyarylamine, poly (N-vinylcarbazole), polyaniline, polythiophene, polypyrrole, N, N, N ', N' -tetrakis (4-methoxyphenyl) -benzidine, 4-bis [ N- (1-naphthyl) -N-phenyl-amino ] biphenyl, 4 '-tris [ phenyl (m-tolyl) amino ] triphenylamine, 4', one or more of 4 "-tris (N-carbazolyl) -triphenylamine, 1-bis [ (di-4-tolylamino) phenylcyclohexane, tetrafluoro-tetracyano-quinone dimethane doped 4,4',4" -tris (diphenylamino) triphenylamine, p-doped phthalocyanine, F4-TCNQ doped N, N' -diphenyl-N, N '-bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine, hexaazabenzophenanthrene-hexanenitrile, metal oxides.
Further, in the case where the charge injection layer is a hole injection layer, the material of the hole injection layer may be selected from poly (ethylenedioxythiophene): polystyrene sulfonate (PEDOT: PSS), poly [9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine ] (TFB), polyarylamine, poly (N-vinylcarbazole) (PVK), polyaniline (Pan), polythiophene, polypyrrole (PPY), 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, one or more of N '-bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine (α -NPD), hexaazabenzophenanthrene-hexa-nitrile (HAT-CN), metal oxides; wherein the metal oxide may be selected from one or more of MnO 3、WO3. The thickness of the hole injection layer may be 10 to 50nm.
The material of the charge transport layer is selected from one or more of doped or undoped oxides, doped or undoped semiconductor particles, nitrides, alq3, almq3, DVPBi, TAZ, OXD, PBD, BND, PV, CBP, alpha-NPD, TPD, spiro-TPD, DNTPD, TCTA, m-MTDATA, TAPC, TFB, poly-TPD, polyaniline, polyfluorene, polypyrrole, PPV, MEH-PPV, MOMO-PPV, copper phthalocyanine, aromatic tertiary amine, polynuclear aromatic tertiary amine, 4' -bis (p-carbazolyl) -1,1' -biphenyl compound, N ' -tetraarylbenzidine, PEDOT: PSS and derivatives thereof, PVK and derivatives thereof, polymethacrylate and derivatives thereof, poly (9, 9-octylfluorene) and derivatives thereof, poly (spirofluorene) and derivatives thereof, NPB, spironpb, HATCN; wherein the oxide is selected from one or more of TiO2、ZnO、ZrO2、SnO2、WO3、NiO、Ta2O3、HfO2、Al2O3、ZrSiO4、BaTiO3、BaZrO3、SrTiO3、MgTiO3、TiLiO、ZnAlO、ZnSnO、ZnLiO、InSnO, the semiconductor particles are selected from one or more of CdS, znSe, znS, the nitride is selected from Si 3N4, and the doping elements of the oxide and semiconductor particles are selected from one or more of Al, mg, in, li, ga, cd, cs, cu.
Further, in the case where the charge transport layer is an electron transport layer, the material of the electron transport layer may be selected from one or more of an inorganic material and an organic material. Wherein the inorganic material may be selected from one or more of doped or undoped oxides, doped or undoped semiconductor particles, nitrides. Further, the oxide may be selected from, but not limited to TiO2、ZnO、ZrO2、SnO2、WO3、NiO、Ta2O3、HfO2、Al2O3、ZrSiO4、BaTiO3、BaZrO3、SrTiO3、MgTiO3、TiLiO、ZnAlO、ZnSnO、ZnLiO、InSnO; semiconductor particles may be selected from, but not limited to CdS, znSe, znS; the nitride may be Si 3N4; the doping elements of the oxide and semiconductor particles may be selected from, but are not limited to Al, mg, in, li, ga, cd, cs, cu, respectively. The organic material of the electron transport layer may be selected from one or more of an oxazole compound, an isoxazole compound, a triazole compound, an isothiazole compound, an oxadiazole compound, a thiadiazole compound, a perylene compound, and an aluminum complex, and further, may be selected from one or more of, but not limited to, alq3, almq3, DVPBi, TAZ, OXD, PBD, BND, PV. The thickness of the electron transport layer may be 20 to 60nm.
In the case where the charge transport layer is a hole transport layer, the material of the hole transport layer may be selected from arylamines such as 4,4' -N, N ' -dicarbazolyl-biphenyl (CBP), N ' -diphenyl-N, N ' -bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine (a-NPD), N ' -diphenyl-N, N ' -bis (3-methylphenyl) - (1, 1' -biphenyl) -4,4' -diamine (TPD), N ' -bis (3-methylphenyl) -N, N ' -bis (phenyl) -spiro (spiro-TPD), N, N ' -bis (4- (N, N ' -diphenyl-amino) phenyl) -N, N ' -diphenyl benzidine (DNTPD), 4' -tris (N-carbazolyl) -triphenylamine (TCTA), tris (3-methylphenyl-phenylamino) -triphenylamine (m-MTDATA), TAPC, poly [ (9, 9' -dioctylfluorene-2, 7-diyl) -co- (4, 4' - (N- (4-sec-butylphenyl) diphenylamine)) ] (TFB) and poly (4-butylphenyl-diphenylamine) (poly-TPD); polyaniline; polyfluorene; polypyrrole; poly (p) phenylenevinylenes and derivatives thereof, such as poly (phenylenevinylene) (PPV), poly [ 2-methoxy-5- (2-ethylhexyloxy) -1, 4-phenylenevinylene ] (MEH-PPV) and poly [ 2-methoxy-5- (3 ',7' -dimethyloctyloxy) -1, 4-phenylenevinylene ] (MOMO-PPV); copper phthalocyanine; aromatic tertiary amines or polynuclear aromatic tertiary amines; 4,4 '-bis (p-carbazolyl) -1,1' -biphenyl compounds; n, N' -tetraarylbenzidine; PEDOT PSS and its derivatives; poly (N-vinylcarbazole) (PVK) and derivatives thereof; polymethacrylate and derivatives thereof; poly (9, 9-octylfluorene) and derivatives thereof; poly (spirofluorene) and derivatives thereof; n, N '-bis (naphthalen-1-yl) -N, N' -diphenyl benzidine (NPB); spiro NPB; HATCN; p-NiO; or a combination of the foregoing compounds. The thickness of the hole transport layer may be 15 to 40nm.
For example, in some embodiments, the light emitting unit may include a first light emitting unit and a second light emitting unit, and the electroluminescent device preferably includes an anode, a first light emitting unit (first hole injection layer, first hole transport layer, first light emitting layer, first electron transport layer), a charge generating layer, a second light emitting unit (second hole transport layer, second light emitting layer, second electron transport layer) and a cathode, which are stacked.
Wherein the first metal oxide in the charge generation layer material may have an electron transport capability to rapidly transport electrons to the first electron transport layer. The conduction band energy level of the first metal oxide may be less than the conduction band energy level of the first electron transport layer material.
The first hole transport layer is preferably a high molecular conductive polymer such as polyaniline, polyfluorene, TFB, PVK, poly-TPD, or the like. The first electron transport layer is preferably an N-type metal oxide, such as ZnO、Znx1Mgy1O、Znx1Aly1O、Znx2Mgy2Liz2O、SnO2、Znx1Sny1O, wherein x1+y1=1 or x2+y2+z2=1. The second hole transport layer is preferably a p-type metal oxide such as p-NiO, or a p-type organic material such as HATCN. The second electron transport layer is preferably a metal oxide such as ZnO, zn x1Mgy1O、Znx1Aly1O、Znx2Mgy2Liz2 O, or the like.
In addition, the invention also provides a preparation method of the electroluminescent device, which comprises the following steps:
Providing a first electrode;
Forming at least two light emitting cells and at least one charge generating layer on the first electrode; each charge generation layer is respectively arranged between two adjacent light emitting units, the material of each charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV; and
A second electrode is formed on the light emitting unit.
It should be noted that, in the preparation method, reference to "forming another structural layer/unit on" a certain structural layer/unit is a broad concept, including "on" having a contact or adjacent relationship, and also including "above" having a spaced relationship, which may mean that the formed another structural layer/unit is adjacent to the certain structural layer/unit, and may also mean that a spacer layer/unit exists between the another structural layer/unit and the certain structural layer/unit.
The deposition/preparation of the structural layers of the electroluminescent device may be achieved by means well known in the art, including by chemical or physical means. The chemical method is, for example, chemical vapor deposition, continuous ion layer adsorption and reaction, anodic oxidation, electrolytic deposition, or coprecipitation. The physical method may be a physical plating method or a solution processing method. Specifically, the physical plating method is, for example, a thermal evaporation plating method, an electron beam evaporation plating method, a magnetron sputtering method, a multi-arc ion plating method, a physical vapor deposition method, an atomic layer deposition method, a pulse laser deposition method; examples of the solution processing method include spin coating, printing, inkjet printing, knife coating, printing, dip-coating, dipping, spraying, roll coating, casting, slit coating, and bar coating. Specific treatment methods and treatment conditions can be referred to as common methods in the art, and will not be described herein.
In addition, the invention also provides a display device comprising the electroluminescent device or the electroluminescent device prepared by the preparation method.
Example 1
The embodiment provides a quantum dot light emitting diode and a preparation method thereof, wherein the quantum dot light emitting diode comprises:
S1, preparing a first hole injection layer 102 on a first electrode 101 made of ITO (indium tin oxide), wherein the material is PEDOT PSS, and the thickness is 15nm;
S2, preparing a first hole transport layer 103 on the first hole injection layer 102, wherein the material is PVK, and the thickness is 25nm;
s3, preparing a first luminescent layer 104 of red quantum dots on the first hole transport layer 103, wherein the material of the first luminescent layer 104 is CdZnSe/ZnSe/ZnS (the luminescent wavelength is 630 nm), and the thickness is 15nm;
S4, preparing a first electron transport layer 105 on the first light-emitting layer 104, wherein the material is Zn 0.95Mg0.05 O (conduction band energy level is-3.75 eV), and the thickness is 40nm;
s5, preparing a charge generation layer 201 on the first electron transport layer 105, wherein the charge generation layer 201 comprises ZnO, mnO 3 and NiO with the mass ratio of 1:2:2, and the thickness is 15nm;
s6, preparing a second hole transport layer 301, which is made of NiO and has a thickness of 25nm, on the charge generation layer 201;
S7, preparing a second luminescent layer 302 of red quantum dots on the second hole transport layer 301, wherein the material of the second luminescent layer 302 is CdZnSe/ZnSe/ZnS (the luminescent wavelength is 630 nm), and the thickness is 15nm;
s8, preparing a second electron transport layer 303 on the second light-emitting layer 302, wherein the material is Zn 0.95Mg0.05 O, and the thickness is 40nm;
s9, preparing a second electrode 304 by a vacuum evaporation process, wherein the material is silver, and the thickness is 100nm.
Example 2
The quantum dot light emitting diode and the preparation method thereof provided in this embodiment are basically the same as those in embodiment 1, except that: in step S5 of this embodiment, the material of the charge generation layer includes SnO 2、MnO3 and CuO in a mass ratio of 2:5:3, and the thickness is 25nm.
Example 3
The quantum dot light emitting diode and the preparation method thereof provided in this embodiment are basically the same as those in embodiment 1, except that: in step S5 of the present embodiment, the material of the charge generation layer includes Zn 0.9Mg0.1O、WO3 and NiO in a mass ratio of 1:4:5, and the thickness is 20nm.
Comparative example 1
The quantum dot light emitting diode and the preparation method thereof provided by the comparative example comprise the following steps:
S1, preparing a first hole injection layer on a first electrode made of ITO (indium tin oxide), wherein the material is PEDOT PSS, and the thickness is 15nm;
s2, preparing a first hole transport layer on the first hole injection layer, wherein the material is PVK, and the thickness is 25nm;
S3, preparing a first luminescent layer of the red quantum dot on the first hole transport layer, wherein the material of the first luminescent layer is CdZnSe/ZnSe/ZnS (the luminescent wavelength is 630 nm), and the thickness is 15nm;
s4, preparing a first electron transport layer on the first light-emitting layer, wherein the material of the first electron transport layer is Zn 0.95Mg0.05 O (conduction band energy level is-3.75 eV), and the thickness of the first electron transport layer is 40nm;
s5, preparing a second hole injection layer on the first electron transport layer, wherein the material is PEDOT PSS, and the thickness is 15nm;
S6, preparing a second hole transport layer on the second hole injection layer, wherein the material is PVK, and the thickness is 25nm;
s7, preparing a second luminescent layer of the red quantum dot on the second hole transport layer, wherein the material of the second luminescent layer is CdZnSe/ZnSe/ZnS (the luminescent wavelength is 630 nm), and the thickness is 15nm;
s8, preparing a second electron transport layer on the second luminescent layer, wherein the material is Zn 0.95Mg0.05 O, and the thickness is 40nm;
s9, preparing a second electrode by a vacuum evaporation process, wherein the material of the second electrode is silver, and the thickness of the second electrode is 100nm.
In this comparative example, the charge generation layer of the device was constituted by the first electron transport layer and the second hole injection layer.
Comparative example 2
The quantum dot light emitting diode and the preparation method thereof provided by the comparative example comprise the following steps:
S1, preparing a first hole injection layer on a first electrode made of ITO (indium tin oxide), wherein the material is PEDOT PSS, and the thickness is 15nm;
s2, preparing a first hole transport layer on the first hole injection layer, wherein the material is PVK, and the thickness is 25nm;
S3, preparing a first luminescent layer of the red quantum dot on the first hole transport layer, wherein the material of the first luminescent layer is CdZnSe/ZnSe/ZnS (the luminescent wavelength is 630 nm), and the thickness is 15nm;
s4, preparing a1 st-1 st electron transport layer on the first luminescent layer, wherein the material is Zn 0.95Mg0.05 O (conduction band energy level is-3.75 eV), and the thickness is 25nm; preparing a 1-2 electron transport layer on the 1-1 electron transport layer, wherein the conduction band energy level of the 1-2 electron transport layer is lower than that of the 1-1 electron transport layer, the 1-2 electron transport layer is made of ZnO, and the thickness of the 1-2 electron transport layer is 15nm;
S5, preparing a second hole injection layer on the 1 st-2 nd electron transport layer, wherein the material is MoO 3, and the thickness is 10nm;
s6, preparing a second hole transport layer on the second hole injection layer, wherein the material is NiO, and the thickness is 25nm.
S7, preparing a second luminescent layer of the red quantum dot on the second hole transport layer, wherein the material of the second luminescent layer is CdZnSe/ZnSe/ZnS (the luminescent wavelength is 630 nm), and the thickness is 15nm;
s8, preparing a second electron transport layer on the second luminescent layer, wherein the material is Zn 0.95Mg0.05 O, and the thickness is 40nm;
s9, preparing a second electrode by a vacuum evaporation process, wherein the material of the second electrode is silver, and the thickness of the second electrode is 100nm.
In this comparative example, the charge generation layer of the device was constituted by the second hole injection layer and the second hole transport layer.
The devices provided in examples 1 to 3 and comparative examples 1 to 2 were tested, and the test results are shown in table 1:
TABLE 1
As can be seen from table 1, since the difference between the conduction band energy level of the first electron transport layer and the HOMO energy level of the second hole injection layer is large in the device provided in comparative example 1, the device has a high turn-on voltage and low current efficiency, and the device provided in comparative example 2 is slightly improved but still in a poor level, whereas the electroluminescent device provided in the present invention has a lower turn-on voltage and higher current efficiency, and the device has excellent performance.
The foregoing has outlined the detailed description of the embodiments of the present invention, and the detailed description of the principles and embodiments of the present invention is provided herein by way of example only to facilitate the understanding of the method and core concepts of the present invention; meanwhile, as those skilled in the art will have variations in the specific embodiments and application scope in light of the ideas of the present invention, the present description should not be construed as limiting the present invention.
Claims (10)
1. An electroluminescent device, comprising:
A first electrode and a second electrode disposed opposite to each other;
at least two light emitting units, wherein the at least two light emitting units are sequentially stacked between the first electrode and the second electrode; and
And at least one charge generation layer, each charge generation layer is respectively arranged between two adjacent light emitting units, the material of the charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV.
2. An electroluminescent device according to claim 1, characterized in that-5.0 eV +.4.5 eV +.conduction band level of the first metal oxide; and/or
-5.0EV +.conduction band level of the second metal oxide < -4.5eV; and/or
-5.5EV < ltoreq.4.5 eV of the valence band energy level of the third metal oxide; and/or
The first metal oxide is an n-type semiconductor; and/or
The third metal oxide is a p-type semiconductor.
3. The electroluminescent device of claim 2, wherein the first metal oxide is selected from one or more of ZnO、Znx1Mgy1O、Znx1Aly1O、Znx2Mgy2Liz2O、SnO2、Znx1Sny1O, wherein x1+y1=1 or x2+y2+z2=1; and/or
The second metal oxide is selected from one or more of MnO 3、WO3; and/or
The third metal oxide is selected from one or more of NiO, snO, cuO.
4. An electroluminescent device according to claim 1, characterized in that the first metal oxide is present in the charge generating layer material in a proportion of 10 to 40wt%; and/or
The second metal oxide accounts for 30-50wt% of the material of the charge generation layer; and/or
The third metal oxide accounts for 30-50wt% of the material of the charge generation layer.
5. The electroluminescent device of claim 1, wherein the charge generation layer has a thickness of 5 to 30nm; and/or
The average particle diameters of the first metal oxide, the second metal oxide and the third metal oxide are respectively 3-15 nm.
6. An electroluminescent device as claimed in any one of claims 1 to 5, wherein each of the light emitting units independently comprises: a light emitting layer; the material of the luminescent layer is one or more selected from single-structure quantum dots, core-shell structure quantum dots, doped or undoped inorganic perovskite type quantum dots and organic-inorganic hybrid perovskite type quantum dots; Wherein the single-structure quantum dot is selected from one or more of II-VI compound, III-V compound, II-V compound, III-VI compound, IV-VI compound, I-III-VI compound, II-IV-VI compound and IV simple substance, the II-VI compound is selected from one or more of CdSe、CdS、CdTe、ZnSe、ZnS、CdTe、ZnTe、CdZnS、CdZnSe、CdZnTe、ZnSeS、ZnSeTe、ZnTeS、CdSeS、CdSeTe、CdTeS、CdZnSeS、CdZnSeTe、CdZnSTe, the III-V compound is selected from InP, inAs, gaP, gaAs, gaN, GaSb, alN, alP, inAsP, inNP, inNSb, gaAlNP, inAlNP, wherein the IV-VI compound is selected from one or more of PbS and PbSe; The I-III-VI compound is selected from one or more of CuInS 2、CuInSe2、AgInS2; the IV group simple substance is selected from one or more of silicon and germanium; 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 one or more of CdS, cdTe, cdSe, cdSeTe, cdZnSe, cdZnS, cdSeS, znSe, znTe, znSeS, znS; the structural general formula of the inorganic perovskite type quantum dot is AMX 3, wherein A is Cs +, M is one or more of Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+, and X is one or more of Cl -、Br-、I-; The organic-inorganic hybrid perovskite quantum dot has a structural general formula of BMX 3, wherein B is selected from one or more of CH 3(CH2)n-2NH3+、NH3(CH2)nNH3 2+, n is more than or equal to 2, M is selected from one or more of Pb2+、Sn2+、Cu2+、Ni2+、Cd2+、Cr2+、Mn2+、Co2+、Fe2+、Ge2+、Yb2+、Eu2+, and X is selected from one or more of Cl -、Br-、I-.
7. The electroluminescent device of claim 6, wherein each of the light emitting units is independent further comprising:
A first charge functional layer disposed on a side of the light emitting layer near the first electrode; and
A second charge functional layer disposed on a side of the light emitting layer near the second electrode;
The first charge functional layer and the second charge functional layer respectively and independently comprise a charge injection layer and/or a charge transmission layer, and each charge generation layer is respectively arranged between the second charge functional layer of one light-emitting unit and the first charge functional layer of the other light-emitting unit.
8. The electroluminescent device of claim 7, wherein the material of the first electrode and the material of the second electrode are each independently selected from one or more of doped or undoped metals, carbon silicon materials, doped or undoped metal oxides, and composite electrode materials; wherein the doped or undoped metal is selected from one or more of Al、Ag、Cu、Mo、Au、Ba、Ca、Mg、Ni、Pt、Ir、Ca:Al、LiF:Ca、LiF:Al、BaF2:Al、CsF:Al、CaCO3:Al、BaF2:Ca:Al、Au:Mg、Ag:Mg; the carbon-silicon material is selected from one or more of silicon, graphite, carbon nano tubes, graphene and carbon fibers; the doped or undoped metal oxide is selected from one or more of ITO, FTO, ATO, AZO, GZO, IZO, MZO, AMO, ITZO, ICO, snO 2、In2O3、Cd:ZnO、Ga:SnO2; the composite electrode material is selected from one or more of AZO/Ag/AZO、AZO/Al/AZO、ITO/Ag/ITO、ITO/Al/ITO、ZnO/Ag/ZnO、ZnO/Al/ZnO、TiO2/Ag/TiO2、TiO2/Al/TiO2、ZnS/Ag/ZnS、ZnS/Al/ZnS; and/or
The material of the charge injection layer is selected from Ca, ba, csF, csCO 3, PEIE, PEI, liF, naF and poly (ethylenedioxythiophene): polystyrene sulfonate, poly [9, 9-dioctyl-fluorene-co-N- (4-butylphenyl) -diphenylamine ], polyarylamine, poly (N-vinylcarbazole), polyaniline, polythiophene, polypyrrole, N, N, N ', N' -tetrakis (4-methoxyphenyl) -benzidine, 4-bis [ N- (1-naphthyl) -N-phenyl-amino ] biphenyl, 4 '-tris [ phenyl (m-tolyl) amino ] triphenylamine, 4', one or more of 4 "-tris (N-carbazolyl) -triphenylamine, 1-bis [ (di-4-tolylamino) phenylcyclohexane, tetrafluoro-tetracyano-quinone dimethane doped 4,4',4" -tris (diphenylamino) triphenylamine, p-doped phthalocyanine, F4-TCNQ doped N, N' -diphenyl-N, N '-bis (1-naphthyl) -1,1' -biphenyl-4, 4 "-diamine, hexaazabenzophenanthrene-hexanenitrile, metal oxides; and/or
The material of the charge transport layer is selected from one or more of doped or undoped oxide, doped or undoped semiconductor particles, nitride, alq3, almq3, DVPBi, TAZ, OXD, PBD, BND, PV, CBP, alpha-NPD, TPD, spiro-TPD, DNTPD, TCTA, m-MTDATA, TAPC, TFB, poly-TPD, polyaniline, polyfluorene, polypyrrole, PPV, MEH-PPV, MOMO-PPV, copper phthalocyanine, aromatic tertiary amine, polynuclear aromatic tertiary amine, 4 '-bis (p-carbazolyl) -1,1' -biphenyl compound, N, N, N ', N' -tetraarylbenzidine, PEDOT: PSS and derivatives thereof, PVK and derivatives thereof, polymethacrylate and derivatives thereof, poly (9, 9-octylfluorene) and derivatives thereof, poly (spirofluorene) and derivatives thereof, NPB, spiroNPB, HATCN; wherein the oxide is selected from one or more of TiO2、ZnO、ZrO2、SnO2、WO3、NiO、Ta2O3、HfO2、Al2O3、ZrSiO4、BaTiO3、BaZrO3、SrTiO3、MgTiO3、TiLiO、ZnAlO、ZnSnO、ZnLiO、InSnO, the semiconductor particles are selected from one or more of CdS, znSe, znS, the nitride is selected from Si 3N4, and the oxide and doping elements of the semiconductor particles are selected from one or more of Al, mg, in, li, ga, cd, cs, cu.
9. The preparation method of the electroluminescent device is characterized by comprising the following steps:
Providing a first electrode;
Forming at least two light emitting cells and at least one charge generating layer on the first electrode; each charge generation layer is respectively arranged between two adjacent light emitting units, and the material of each charge generation layer comprises a first metal oxide, a second metal oxide and a third metal oxide, wherein the conduction band energy level of the first metal oxide is between the conduction band energy level of the second metal oxide and-4.5 eV, and the valence band energy level of the third metal oxide is between the conduction band energy level of the first metal oxide and-5.5 eV; and
A second electrode is formed on the light emitting unit.
10. Display device, characterized in that it comprises an electroluminescent device according to any one of claims 1 to 8 or an electroluminescent device produced by the production method according to claim 9.
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