CN113130794B - Quantum dot light-emitting diode and preparation method thereof - Google Patents
Quantum dot light-emitting diode and preparation method thereof Download PDFInfo
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- CN113130794B CN113130794B CN201911425210.4A CN201911425210A CN113130794B CN 113130794 B CN113130794 B CN 113130794B CN 201911425210 A CN201911425210 A CN 201911425210A CN 113130794 B CN113130794 B CN 113130794B
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
- H10K50/115—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising active inorganic nanostructures, e.g. luminescent quantum dots
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
- H10K50/125—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light
- H10K50/13—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light comprising stacked EL layers within one EL unit
- H10K50/131—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light comprising stacked EL layers within one EL unit with spacer layers between the electroluminescent layers
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
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Abstract
The invention discloses a quantum dot light-emitting diode and a preparation method thereof. The quantum dot light emitting diode includes: anode, negative pole, set up in stromatolite between anode and the negative pole, the stromatolite includes first quantum dot luminescent layer, spacer layer and second quantum dot luminescent layer, the spacer layer set up in first quantum dot luminescent layer and between the second quantum dot luminescent layer, the spacer layer includes a plurality of ZnS quantum dot. The invention adopts the technical scheme that the quantum dot light emitting layer which is originally one layer thick is set as two relatively thin quantum dot light emitting layers, a spacing layer is added between the two quantum dot light emitting layers, and the high band gap of ZnS is utilized to penetrate between the two relatively thin quantum dot light emitting layers as a barrier, so that the problem of fluorescence resonance energy transfer is avoided, and the final device brightness, quantum efficiency and service life are ensured. Meanwhile, the spacer layer can also serve as a charge injection layer to transfer certain charges into the QDs, so that the efficiency is further improved.
Description
Technical Field
The invention relates to the technical field of quantum dot light-emitting diodes, in particular to a quantum dot light-emitting diode and a preparation method thereof.
Background
The quantum dot electroluminescence is a novel solid-state lighting technology, has the advantages of low cost, light weight, high response speed, high color saturation and the like, has wide development prospect, and becomes one of important research directions of new generation LED lighting.
The main structures of the existing quantum dot light emitting diode (QLED) are a cathode, an anode, a hole/electron transport layer and a quantum dot light emitting layer, but the brightness, the quantum efficiency and the service life of the existing quantum dot light emitting diode (QLED) cannot reach an ideal value, mainly because the selection of a thin film material and the optimization of a preparation process are not perfect.
Accordingly, there is a need for improvements and developments in the art.
Disclosure of Invention
In view of the above-mentioned deficiencies of the prior art, the present invention aims to provide a quantum dot light emitting diode and a method for manufacturing the same, which aims to solve the problem of the prior quantum dot light emitting diode that the brightness, the quantum efficiency and the lifetime are not ideal to a certain extent.
The technical scheme of the invention is as follows:
a quantum dot light emitting diode, comprising: the laminated quantum dot light-emitting diode comprises an anode, a cathode and a laminated layer arranged between the anode and the cathode, wherein the laminated layer comprises a first quantum dot light-emitting layer, a spacing layer and a second quantum dot light-emitting layer, the spacing layer is arranged between the first quantum dot light-emitting layer and the second quantum dot light-emitting layer, and the spacing layer comprises a plurality of ZnS quantum dots.
A preparation method of a quantum dot light-emitting diode comprises the following steps:
providing an anode;
forming a first quantum dot light emitting layer on the anode;
forming a spacer layer on the first quantum dot light emitting layer, the spacer layer comprising a plurality of ZnS quantum dots; (ii) a
Forming a second quantum dot light emitting layer on the spacer layer;
forming a cathode on the second quantum dot light-emitting layer to obtain a quantum dot light-emitting diode;
or,
providing a cathode;
forming a second quantum dot light emitting layer on the cathode;
forming a spacer layer on the second quantum dot light emitting layer, the spacer layer comprising a plurality of ZnS quantum dots;
forming a first quantum dot light emitting layer on the spacer layer;
and forming an anode on the first quantum dot light-emitting layer to obtain the quantum dot light-emitting diode.
Has the advantages that: in the invention, the original one-layer thick quantum dot light-emitting layer is arranged into two relatively thin quantum dot light-emitting layers (a first quantum dot light-emitting layer and a second quantum dot light-emitting layer), a spacing layer (the spacing layer comprises a plurality of ZnS quantum dots) is added between the two quantum dot light-emitting layers, and the high band gap (about 3.65 eV) of ZnS is utilized to be inserted between the two relatively thin quantum dot light-emitting layers as a barrier, so that the problem of Fluorescence Resonance Energy Transfer (FRET) caused by the original arrangement of the one-layer thick quantum dot light-emitting layer is avoided, and the final brightness, quantum efficiency and service life of the device are ensured. According to the invention, the spacing layer enables a certain distance to be reserved between the two layers of quantum dots, and finally, the radiative exciton recombination is generated in the quantum dot light-emitting layer, so that the brightness and the quantum efficiency of the device are improved. Meanwhile, the spacer layer can also serve as a charge injection layer to transfer certain charges into the QDs, so that the efficiency is further improved.
Drawings
Fig. 1 is a schematic structural diagram of a quantum dot light emitting diode with a front-mounted structure according to an embodiment of the present invention.
Fig. 2 is a schematic structural diagram of a quantum dot light emitting diode with an inverted structure according to an embodiment of the present invention.
Fig. 3 is a schematic flow chart of a method for manufacturing a quantum dot light emitting diode with a front-mounted structure according to an embodiment of the present invention.
Fig. 4 is a schematic flow chart of a method for manufacturing an inverted quantum dot light emitting diode according to an embodiment of the present invention.
Detailed Description
The invention provides a quantum dot light-emitting diode and a preparation method thereof, and the invention is further described in detail below in order to make the purpose, technical scheme and effect of the invention clearer and clearer. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The embodiment of the invention provides a quantum dot light-emitting diode, which comprises: the laminated quantum dot light-emitting diode comprises an anode, a cathode and a laminated layer arranged between the anode and the cathode, wherein the laminated layer comprises a first quantum dot light-emitting layer, a spacing layer and a second quantum dot light-emitting layer, the spacing layer is arranged between the first quantum dot light-emitting layer and the second quantum dot light-emitting layer, and the spacing layer comprises a plurality of ZnS quantum dots.
Fluorescence Resonance Energy Transfer (FRET) refers to a strong resonance transfer by the strength of the point-to-point coupling as the distance between the donor and acceptor becomes closer and the spectral overlap between the donor emission and acceptor absorption becomes larger. If the quantum dot light-emitting layer is too thick, the resonance transfer phenomenon caused by complete overlapping of spectrums can be approximately seen to occur in the quantum dot light-emitting layer, but the lost energy cannot cause radiation, so that the final device brightness, quantum efficiency and service life are reduced. That is, the FRET is a non-radiative energy transfer that affects device brightness, quantum efficiency, and lifetime of the overall device. In this embodiment, a mode that an originally thick quantum dot light emitting layer is set as two relatively thin quantum dot light emitting layers (a first quantum dot light emitting layer and a second quantum dot light emitting layer) is adopted, a spacer layer (the spacer layer includes a plurality of ZnS quantum dots) is added between the two quantum dot light emitting layers, and a high band gap (about 3.65 eV) of ZnS is utilized to interpose between the two relatively thin quantum dot light emitting layers as a barrier, so that a Fluorescence Resonance Energy Transfer (FRET) problem caused by the originally set thick quantum dot light emitting layer is avoided, and final device brightness, quantum efficiency and service life are ensured. In this embodiment, the spacer layer provides a certain distance between the two quantum dots, and finally allows radiative exciton recombination to occur in the quantum dot light-emitting layer, thereby improving device brightness and quantum efficiency. Meanwhile, the spacer layer can also serve as a charge injection layer to transfer certain charges into the QDs, so that the efficiency is further improved.
In one embodiment, the spacer layer is comprised of ZnS quantum dots.
In one embodiment, the first quantum dot light-emitting layer and the second quantum dot light-emitting layer are each composed of quantum dots, a ratio of an average particle diameter of the quantum dots of the first quantum dot light-emitting layer to an average particle diameter of the ZnS quantum dots is less than or equal to 1.5 and greater than or equal to 0.5, and a ratio of an average particle diameter of the quantum dots of the second quantum dot light-emitting layer to an average particle diameter of the ZnS quantum dots is less than or equal to 1.5 and greater than or equal to 0.5. For example, the average particle size of the quantum dots of the first quantum dot light-emitting layer is 15nm, the average particle size of the zns quantum dots is 10nm, and the ratio is 1.5; or the average grain diameter of the quantum dots of the first quantum dot light-emitting layer is 15nm, the average grain diameter of the ZnS quantum dots is 15nm, and the ratio is 1; the ratio of the average particle size of the quantum dots of the first quantum dot light-emitting layer to the average particle size of the ZnS quantum dots may be 0.8, 0.9, 1, 1.1, 1.2, 1.3, 1.4, 1.5, or the like. For example, the average particle size of the quantum dots of the second quantum dot light-emitting layer is 15nm, the average particle size of the zns quantum dots is 10nm, and the ratio is 1.5; or the average grain diameter of the quantum dots of the second quantum dot light-emitting layer is 15nm, the average grain diameter of the ZnS quantum dots is 15nm, and the ratio is 1; the ratio of the average particle size of the quantum dots of the second quantum dot light-emitting layer to the average particle size of the ZnS quantum dots may be 0.8, 0.9, 1, 1.1, 1.2, 1.3, 1.4, 1.5, or the like.
Note that the actual particle size distribution of the quantum dots is in one interval. The average particle size of the quantum dots in this embodiment can be obtained by combining with a method for measuring particle size commonly known in the art, for example, by combining with a characterization method of a Transmission Electron Microscope (TEM) (digitalmiograph software or imageJ software can be used to directly count electron microscope pictures), or by combining with an X-ray diffraction method (XRD) (for example, by combining with a commonly used Scherrel formula — Scherrel formula), or by combining with a characterization method of a particle size analyzer or Zeta potential meter, or by combining with other methods for characterizing particle size commonly known in the field of nanomaterials. Since the average particle size of the quantum dots in this embodiment can be obtained statistically by combining methods for measuring particle sizes that are common in the art, detailed description is omitted here, and reference may be made to the prior art.
In one embodiment, the thickness of the spacer layer is less than or equal to the thickness of the first quantum dot light emitting layer, and/or the thickness of the spacer layer is less than or equal to the thickness of the second quantum dot light emitting layer. Thus, the spacer layer thickness is moderate. Since the electroluminescent capability is much weaker than that of the quantum dot light emitting layer, the brightness and efficiency at the same voltage may be lowered if the thickness is too thick.
In some examples, the thickness of the spacer layer is less than or equal to the thickness of the first quantum dot light emitting layer and the thickness of the spacer layer is less than or equal to the thickness of the second quantum dot light emitting layer. In other examples, the thickness of the spacer layer is less than or equal to the thickness of the first quantum dot light emitting layer. In still other examples, the thickness of the spacer layer is less than or equal to the thickness of the second quantum dot light emitting layer.
In one embodiment, the spacer layer has a thickness of 10 to 16nm. When the thickness of the spacing layer is gradually increased, the distance between the two layers of quantum dots is large enough, and the radiative exciton recombination occurs in the quantum dot light-emitting layer, so that the brightness of the device is improved. Certainly, the spacer layer itself cannot be too thick, because the electroluminescent capability of the spacer layer is far weaker than that of the quantum dot light-emitting layer itself, and thus, if the spacer layer is too thick, the brightness and efficiency at the same voltage become low.
In one embodiment, the thickness of the first quantum dot light emitting layer is 15 to 25nm, and the thickness of the second quantum dot light emitting layer is 15 to 25nm. The thickness of the first quantum dot light emitting layer and the thickness of the second quantum dot light emitting layer may be the same or different.
In one embodiment, the material forming the first quantum dot light emitting layer is the same as the material forming the second quantum dot light emitting layer. Because the present embodiment mainly aims to enhance the luminance of the quantum dot light emitting diode, the quantum dot light emitting diode has the advantage of narrow half-peak width of the material, and if the first quantum dot light emitting layer and the second quantum dot light emitting layer use different kinds of quantum dot materials, the light emitting peak position may be changed or the half-peak width may be increased, so that the uniformity of the material is maintained, and the luminance is improved while the original color purity of the light emitted is ensured.
In one embodiment, the spacer layer covers the first quantum dot light-emitting layer at an orthographic area of the first quantum dot light-emitting layer, and the spacer layer covers the second quantum dot light-emitting layer at an orthographic area of the second quantum dot light-emitting layer. The problem of fluorescence resonance energy transfer caused by the fact that a quantum dot light-emitting layer with one layer thickness is originally arranged is avoided to the maximum extent, and the brightness, quantum efficiency and service life of a final device are guaranteed.
In one embodiment, the quantum dot light emitting diode further comprises: a hole injection layer and a hole transport layer disposed between the anode and the stack, and an electron transport layer disposed between the cathode and the stack. The hole injection layer is provided on the side close to the anode, and the hole transport layer is provided on the side close to the stack.
In this embodiment, the quantum dot light emitting diode has various forms, and the quantum dot light emitting diode may be an upright structure or an inverted structure, where the quantum dot light emitting diode with the upright structure will be described mainly by taking the structure shown in fig. 1 as an example. Specifically, as shown in fig. 1, the quantum dot light emitting diode with the front-facing structure includes an anode 10, a hole injection layer 11, a hole transport layer 12, a first quantum dot light emitting layer 13, a spacer layer 14, a second quantum dot light emitting layer 15, an electron transport layer 16, and a cathode 17, which are sequentially arranged from bottom to top, and the spacer layer 14 includes a plurality of ZnS quantum dots.
In one embodiment, the substrate may be a rigid substrate, such as glass, or a flexible substrate, such as one of PET or PI.
In one embodiment, the anode may be selected from one or more of indium doped tin oxide (ITO), fluorine doped tin oxide (FTO), antimony doped tin oxide (ATO), aluminum doped zinc oxide (AZO), and the like. Further, the anode is indium-doped tin oxide (ITO).
In one embodiment, the material of the hole injection layer may be poly (3,4-ethylenedioxythiophene) -poly (styrenesulfonic acid) (PEDOT: PSS) and its doped s-MoO 3 (PEDOT: PSS: s-MoO) 3 ) And the like.
In one embodiment, the material of the hole transport layer is an organic material having good hole transport ability, and may include, for example, but not limited to, one or more of 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), poly (9,9-dioctylfluorene-CO-bis-N, N-phenyl-1,4-Phenylenediamine) (PFB), 5725 zxf5725 ',4 ″ -tris (carbazol-9-yl) triphenylamine (TCTA), 4,4' -bis (9-Carbazole) Biphenyl (CBP), N '-diphenyl-N, N' -bis (3-methylphenyl) -1,1 '-biphenyl-4,4' -diamine (TPD), N '-diphenyl-N' -biphenyl-4234 '-naphthalene-4264' -C-b, and graphene (N-4264).
In one embodiment, the hole transport layer may also be an inorganic material with hole transport capability, such as may include but is not limited to NiO x 、MoO x 、WO x 、CrO x 、CuO、MoS x 、MoSe x 、WS x 、WSe x And CuS.
In one embodiment, the quantum dots forming the first quantum dot light emitting layer are the same as the quantum dots forming the second quantum dot light emitting layer. In one embodiment, the quantum dots may be selected from one of the three common red, green and blue quantum dots, and may also be yellow quantum dots. Specifically, the quantum dots are binary phase quantum dots, ternary phase quantum dots, quaternary phase quantum dots, or the like, but are not limited thereto. Wherein the binary phase quantum dots include but are not limited to at least one of CdS, cdSe, cdTe, inP, agS, pbS, pbSe, hgS; the ternary phase quantum dots include but are not limited to Zn X Cd 1-X S、Cu X In 1-X S、Zn X Cd 1-X Se、Zn X Se 1-X S、Zn X Cd 1-X Te、PbSe X S 1-X At least one of (a); the quaternary phase quantum dots include, but are not limited to, zn X Cd 1-X S/ZnSe、Cu X In 1-X S/ZnS、Zn X Cd 1-X Se/ZnS、CuInSeS、Zn X Cd 1-X Te/ZnS、PbSe X S 1-X At least one of/ZnS wherein 0<X<1。
In one embodiment, the material of the electron transport layer may be selected from N-type semiconductor oxides having good electron transport properties, such as, but not limited to, znO, tiO, which may be N-type 2 、Fe 2 O 3 、SnO 2 、Ta 2 O 3 One or more of AlZnO, znSnO, inSnO, N-type doping of these oxides, and the like.
In one embodiment, the cathode may be selected from one of an aluminum (Al) electrode, a silver (Ag) electrode, a gold (Au) electrode, and the like, and may also be selected from one of a nano aluminum wire, a nano silver wire, a nano gold wire, and the like.
In this embodiment, the quantum dot light emitting diode has various forms, and the quantum dot light emitting diode may be in an upright structure or an inverted structure, where the quantum dot light emitting diode in the inverted structure will be described mainly by taking the structure shown in fig. 2 as an example. Specifically, as shown in fig. 2, the quantum dot light emitting diode with the inverted structure includes a cathode 20, an electron transport layer 21, a second quantum dot light emitting layer 22, a spacer layer 23, a first quantum dot light emitting layer 24, a hole transport layer 25, a hole injection layer 26, and an anode 27, which are sequentially arranged from bottom to top, where the spacer layer includes a plurality of ZnS quantum dots.
In one embodiment, the cathode may be selected from one or more of indium doped tin oxide (ITO), fluorine doped tin oxide (FTO), antimony doped tin oxide (ATO), aluminum doped zinc oxide (AZO), and the like. Further, the cathode is indium-doped tin oxide (ITO).
In one embodiment, the anode may be selected from one of an aluminum (Al) electrode, a silver (Ag) electrode, a gold (Au) electrode, and the like, and may also be selected from one of a nano aluminum wire, a nano silver wire, a nano gold wire, and the like.
In the above device, the material selection of the remaining layers is described above and will not be described herein.
Referring to fig. 3, fig. 3 is a schematic flow chart of a method for manufacturing a quantum dot light emitting diode with a front-mounted structure according to an embodiment of the present invention, as shown in fig. 3, including the steps of:
s10, providing an anode;
s11, forming a first quantum dot light-emitting layer on the anode;
s12, forming a spacing layer on the first quantum dot light-emitting layer, wherein the spacing layer comprises a plurality of ZnS quantum dots;
s13, forming a second quantum dot light-emitting layer on the spacing layer;
and S14, forming a cathode on the second quantum dot light-emitting layer to obtain the quantum dot light-emitting diode.
Referring to fig. 4, fig. 4 is a schematic flow chart of a method for manufacturing an inverted quantum dot light emitting diode according to an embodiment of the present invention, as shown in fig. 4, including the steps of:
s20, providing a cathode;
s21, forming a second quantum dot light-emitting layer on the cathode;
s22, forming a spacing layer on the second quantum dot light-emitting layer, wherein the spacing layer comprises a plurality of ZnS quantum dots;
s23, forming a first quantum dot light-emitting layer on the spacing layer;
and S24, forming an anode on the first quantum dot light-emitting layer to obtain the quantum dot light-emitting diode.
In this embodiment, a mode that a quantum dot light emitting layer originally having a thick layer is set as two relatively thin quantum dot light emitting layers (a first quantum dot light emitting layer and a second quantum dot light emitting layer) is adopted, a spacer layer (the spacer layer includes a plurality of ZnS quantum dots) is added between the two quantum dot light emitting layers, and a high band gap (about 3.65 eV) of ZnS is utilized to interpose the two relatively thin quantum dot light emitting layers as a barrier, so that a problem of Fluorescence Resonance Energy Transfer (FRET) caused by the originally set thick quantum dot light emitting layer is avoided, and final device brightness, quantum efficiency and service life are ensured. In this embodiment, the spacer layer makes a certain distance between two layers of quantum dots, and finally makes radiative exciton recombination occur in the quantum dot light-emitting layer, so that the device brightness and quantum efficiency are improved. Meanwhile, the spacer layer can also serve as a charge injection layer to transfer certain charges into the QDs, so that the efficiency is further improved.
In one embodiment, the spacer layer is comprised of ZnS quantum dots.
In one embodiment, the first quantum dot light-emitting layer and the second quantum dot light-emitting layer are each composed of quantum dots, a ratio of an average particle diameter of the quantum dots of the first quantum dot light-emitting layer to an average particle diameter of the ZnS quantum dots is less than or equal to 1.5 and greater than or equal to 0.5, and a ratio of an average particle diameter of the quantum dots of the second quantum dot light-emitting layer to an average particle diameter of the ZnS quantum dots is less than or equal to 1.5 and greater than or equal to 0.5. For example, the average particle size of the quantum dots of the first quantum dot light-emitting layer is 15nm, the average particle size of the zns quantum dots is 10nm, and the ratio is 1.5; or the average grain diameter of the quantum dots of the first quantum dot light-emitting layer is 15nm, the average grain diameter of the ZnS quantum dots is 15nm, and the ratio is 1; the ratio of the average particle size of the quantum dots of the first quantum dot light-emitting layer to the average particle size of the ZnS quantum dots may be 0.8, 0.9, 1, 1.1, 1.2, 1.3, 1.4, 1.5, or the like. For example, the average particle size of the quantum dots of the second quantum dot light-emitting layer is 15nm, the average particle size of the zns quantum dots is 10nm, and the ratio is 1.5; or the average grain diameter of the quantum dots of the second quantum dot light-emitting layer is 15nm, the average grain diameter of the ZnS quantum dots is 15nm, and the ratio is 1; the ratio of the average particle size of the quantum dots of the second quantum dot light-emitting layer to the average particle size of the ZnS quantum dots may be 0.8, 0.9, 1, 1.1, 1.2, 1.3, 1.4, 1.5, or the like.
Note that the actual particle size distribution of the quantum dots is in one interval. The average particle size of the quantum dots in this embodiment can be obtained by combining with a method for measuring particle size commonly known in the art, for example, by combining with a characterization method of a Transmission Electron Microscope (TEM) (digitalmiograph software or imageJ software can be used to directly count electron microscope pictures), or by combining with an X-ray diffraction method (XRD) (for example, by combining with a commonly used Scherrel formula — Scherrel formula), or by combining with a characterization method of a particle size analyzer or Zeta potential meter, or by combining with other methods for characterizing particle size commonly known in the field of nanomaterials. Since the average particle size of the quantum dots in this embodiment can be obtained statistically by combining methods for measuring particle sizes that are common in the art, detailed description is omitted here, and reference may be made to the prior art.
In one embodiment, the thickness of the spacer layer is less than or equal to the thickness of the first quantum dot light emitting layer, and/or the thickness of the spacer layer is less than or equal to the thickness of the second quantum dot light emitting layer. Thus, the spacer layer thickness is moderate. Since the electroluminescent capability is much weaker than that of the quantum dot light emitting layer, the brightness and efficiency at the same voltage may be lowered if the thickness is too thick.
In some examples, the thickness of the spacer layer is less than or equal to the thickness of the first quantum dot light emitting layer and the thickness of the spacer layer is less than or equal to the thickness of the second quantum dot light emitting layer. In other examples, the thickness of the spacer layer is less than or equal to the thickness of the first quantum dot light emitting layer. In still other examples, the thickness of the spacer layer is less than or equal to the thickness of the second quantum dot light emitting layer.
In one embodiment, the spacer layer has a thickness of 10 to 16nm. When the thickness of the spacing layer is gradually increased, the distance between the two layers of quantum dots is large enough, and the radiative exciton recombination occurs in the quantum dot light-emitting layer, so that the brightness of the device is improved. Certainly, the spacer layer itself cannot be too thick, because the electroluminescent capability is much weaker than that of the quantum dot light-emitting layer itself, so that the brightness and efficiency at the same voltage are lowered if the spacer layer is too thick.
In one embodiment, the thickness of the first quantum dot light emitting layer is 15 to 25nm, and the thickness of the second quantum dot light emitting layer is 15 to 25nm. The thickness of the first quantum dot light-emitting layer and the thickness of the second quantum dot light-emitting layer may be the same or different.
In one embodiment, the material forming the first quantum dot light emitting layer is the same as the material forming the second quantum dot light emitting layer. Because the present embodiment mainly aims to enhance the luminance of the quantum dot light emitting diode, the quantum dot light emitting diode has the advantage of narrow half-peak width of the material, and if the first quantum dot light emitting layer and the second quantum dot light emitting layer use different kinds of quantum dot materials, the light emitting peak position may be changed or the half-peak width may be increased, so that the uniformity of the material is maintained, and the luminance is improved while the original color purity of the light emitted is ensured.
In this embodiment, the quantum dot light emitting diode has various forms, and a method for manufacturing the quantum dot light emitting diode with the front-facing structure will be described below by taking the structure shown in fig. 1 as an example. The preparation method of the quantum dot light-emitting diode with the positive structure shown in fig. 1 comprises the following steps:
s101, forming a hole injection layer 11 on the anode 10;
s102, forming a hole transport layer 12 on the hole injection layer 11;
s103, forming a first quantum dot light-emitting layer 13 on the hole transport layer 12;
s104, forming a spacer layer 14 on the first quantum dot light emitting layer 13, where the spacer layer 14 includes a plurality of ZnS quantum dots;
s105, forming a second quantum dot light emitting layer 15 on the spacing layer 14;
s106, forming an electron transport layer 16 on the second quantum dot light emitting layer 15;
and S107, manufacturing a cathode 17 to obtain the quantum dot light-emitting diode with the positive structure.
In this embodiment, the quantum dot light emitting diode has various forms, and a method for manufacturing the quantum dot light emitting diode with an inverted structure will be described below by taking the structure shown in fig. 2 as an example. The preparation method of the quantum dot light-emitting diode with the inverted structure shown in fig. 2 comprises the following steps:
s201, forming an electron transport layer 21 on the cathode 20;
s202, forming a second quantum dot light-emitting layer 22 on the electron transport layer 21;
s203, forming a spacer layer 23 on the second quantum dot light-emitting layer 22, where the spacer layer 23 includes a plurality of ZnS quantum dots;
s204, forming a first quantum dot light-emitting layer 24 on the spacing layer 23;
s205, forming a hole transport layer 25 on the first quantum dot light-emitting layer 24;
s205, forming a hole injection layer 26 on the hole transport layer 25;
and S206, manufacturing an anode 27 to obtain the quantum dot light-emitting diode with the inverted structure.
In one embodiment, the obtained quantum dot light emitting diode is subjected to an encapsulation process. The packaging process can adopt common machine packaging or manual packaging. Preferably, the oxygen content and the water content in the packaging treatment environment are both lower than 0.1ppm so as to ensure the stability of the device.
In this embodiment, the preparation method of each layer may be a chemical method or a physical method, wherein the chemical method includes, but is not limited to, one or more of a chemical vapor deposition method, a continuous ion layer adsorption and reaction method, an anodic oxidation method, an electrolytic deposition method, and a coprecipitation method; the physical method includes, but is not limited to, one or more of solution method (such as spin coating, printing, knife coating, dip-coating, dipping, spraying, roll coating, casting, slit coating, or bar coating), evaporation method (such as thermal evaporation, electron beam evaporation, magnetron sputtering, or multi-arc ion plating), deposition method (such as physical vapor deposition, atomic layer deposition, pulsed laser deposition, etc.).
The invention is further illustrated by the following specific examples.
Example 1
Preparing a QLED device with a positive structure:
s11, spin-coating a layer of PEDOT (PSS: S-MoO) on the ITO substrate 3 A hole injection layer, and annealing at 150 ℃ in the air;
s12, in a nitrogen atmosphere, spin-coating a 20nm PVK hole transport layer on the hole injection layer, and annealing at 150 ℃;
s13, spin-coating a 20nm CdSe/ZnS first quantum dot light-emitting layer on the hole transport layer, placing the hole transport layer in the air for 1min, and taking the hole transport layer back to the nitrogen glove box;
s14, a 15nm ZnS spacing layer is spin-coated on the first quantum dot light-emitting layer, placed in the air for 1min and then taken back to the nitrogen glove box;
s15, spin-coating a 20nm CdSe/ZnS second quantum dot light-emitting layer on the ZnS spacing layer, and annealing at 80 ℃;
s16, plating a 30nm AZO electronic transmission layer on the second quantum dot light-emitting layer by a magnetron sputtering method;
s17, evaporating and plating an 80nm Al electrode on the electron transport layer;
and S18, packaging to obtain the QLED device with the positive structure.
Example 2
Preparing an inverted structure QLED device:
s21, depositing a 50nm ZnO electron transmission layer on the ITO substrate in a nitrogen atmosphere;
s22, spin-coating a 15nm CdZnSeS/ZnS second quantum dot light-emitting layer on the electron transmission layer, placing the electron transmission layer in the air for 1min, and taking the electron transmission layer back to the nitrogen glove box;
s23, a ZnS spacing layer with the thickness of 10nm is spin-coated on the second quantum dot light-emitting layer, and the ZnS spacing layer is placed in the air for 1min and then taken back to the nitrogen glove box;
s24, spin-coating a 15nm CdZnSeS/ZnS first quantum dot light-emitting layer on the ZnS spacing layer, and annealing at 100 ℃;
s25, spin-coating a 25nm NPB hole transport layer on the first quantum dot light-emitting layer, and annealing at 80 ℃;
s26, spraying a PEDOT (PSS) hole injection layer on the hole transport layer in a spraying mode;
s27, evaporating and plating a 90nm Ag electrode on the hole injection layer;
and S28, packaging to obtain the QLED device with the inverted structure.
In summary, according to the quantum dot light emitting diode and the method for manufacturing the same provided by the invention, the quantum dot light emitting layer originally having the one layer thickness is set to be the two relatively thin quantum dot light emitting layers (the first quantum dot light emitting layer and the second quantum dot light emitting layer), the ZnS spacing layer is added between the two quantum dot light emitting layers, and the ZnS high band gap (about 3.65 eV) is utilized to penetrate between the two relatively thin quantum dot light emitting layers as a barrier, so that the problem of Fluorescence Resonance Energy Transfer (FRET) caused by the quantum dot light emitting layer originally having the one layer thickness is avoided, and the final device brightness, quantum efficiency and service life are ensured. According to the invention, the ZnS spacer layer enables a certain distance to be reserved between the two layers of quantum dots, and finally, the radiative exciton recombination is generated in the quantum dot light-emitting layer, so that the brightness and the quantum efficiency of the device are improved. Meanwhile, the ZnS spacer layer can also serve as a charge injection layer to transfer certain charges into the QDs, so that the efficiency is further improved.
It is to be understood that the invention is not limited to the examples described above, but that modifications and variations may be effected thereto by those of ordinary skill in the art in light of the foregoing description, and that all such modifications and variations are intended to be within the scope of the invention as defined by the appended claims.
Claims (7)
1. A quantum dot light emitting diode, comprising: the laminated layer comprises a first quantum dot light-emitting layer, a spacing layer and a second quantum dot light-emitting layer, the spacing layer is arranged between the first quantum dot light-emitting layer and the second quantum dot light-emitting layer, and the spacing layer comprises a plurality of ZnS quantum dots; the thickness of the spacing layer is 10-16 nm; the material for forming the first quantum dot light-emitting layer and the material for forming the second quantum dot light-emitting layer are binary phase quantum dots, ternary phase quantum dots or quaternary phase quantum dots respectively;
wherein,
the binary phase quantum dots comprise at least one of CdS, cdSe, cdTe, inP, agS, pbS, pbSe and HgS;
the ternary phase quantum dots comprise Zn X Cd 1-X S、Cu X In 1-X S、Zn X Cd 1-X Se、Zn X Se 1-X S、Zn X Cd 1-X Te、PbSe X S 1-X At least one of (b), wherein 0<X<1;
The quaternary phase quantum dots comprise Zn X Cd 1-X S/ZnSe、Cu X In 1-X S/ZnS、Zn X Cd 1-X Se/ZnS、CuInSeS、Zn X Cd 1-X Te/ZnS、PbSe X S 1-X At least one of/ZnS, wherein 0<X<1;
The thickness of the spacing layer is less than or equal to that of the first quantum dot light-emitting layer, and/or the thickness of the spacing layer is less than or equal to that of the second quantum dot light-emitting layer;
the spacing layer covers the first quantum dot light-emitting layer in the orthographic projection area of the first quantum dot light-emitting layer, and/or the spacing layer covers the second quantum dot light-emitting layer in the orthographic projection area of the second quantum dot light-emitting layer.
2. The quantum dot light-emitting diode of claim 1, wherein the material forming the first quantum dot light-emitting layer is the same as the material forming the second quantum dot light-emitting layer.
3. The quantum dot light-emitting diode of claim 1, wherein the first quantum dot light-emitting layer and the second quantum dot light-emitting layer are each composed of quantum dots, a ratio of an average particle diameter of the quantum dots of the first quantum dot light-emitting layer to an average particle diameter of the ZnS quantum dots is less than or equal to 1.5 and greater than or equal to 0.5, and a ratio of an average particle diameter of the quantum dots of the second quantum dot light-emitting layer to an average particle diameter of the ZnS quantum dots is less than or equal to 1.5 and greater than or equal to 0.5.
4. The quantum dot light-emitting diode of claim 1, wherein the first quantum dot light-emitting layer has a thickness of 15 to 25nm, and the second quantum dot light-emitting layer has a thickness of 15 to 25nm.
5. A preparation method of a quantum dot light-emitting diode is characterized by comprising the following steps:
providing an anode;
forming a first quantum dot light emitting layer on the anode;
forming a spacer layer on the first quantum dot light emitting layer, the spacer layer comprising a plurality of ZnS quantum dots; the thickness of the spacing layer is 10-16 nm;
forming a second quantum dot light emitting layer on the spacer layer;
forming a cathode on the second quantum dot light-emitting layer to obtain a quantum dot light-emitting diode; the thickness of the spacing layer is less than or equal to that of the first quantum dot light-emitting layer, and/or the thickness of the spacing layer is less than or equal to that of the second quantum dot light-emitting layer;
the spacing layer covers the first quantum dot light-emitting layer in the orthographic projection area of the first quantum dot light-emitting layer, and/or the spacing layer covers the second quantum dot light-emitting layer in the orthographic projection area of the second quantum dot light-emitting layer;
the material for forming the first quantum dot light-emitting layer and the material for forming the second quantum dot light-emitting layer are binary phase quantum dots, ternary phase quantum dots or quaternary phase quantum dots respectively;
wherein,
the binary phase quantum dots comprise at least one of CdS, cdSe, cdTe, inP, agS, pbS, pbSe and HgS;
the ternary phase quantum dots comprise Zn X Cd 1-X S、Cu X In 1-X S、Zn X Cd 1-X Se、Zn X Se 1-X S、Zn X Cd 1-X Te、PbSe X S 1-X At least one of (1), wherein 0<X<1;
The quaternary phase quantum dots comprise Zn X Cd 1-X S/ZnSe、Cu X In 1-X S/ZnS、Zn X Cd 1-X Se/ZnS、CuInSeS、Zn X Cd 1-X Te/ZnS、PbSe X S 1-X At least one of/ZnS wherein 0<X<1
Or,
providing a cathode;
forming a second quantum dot light emitting layer on the cathode;
forming a spacer layer on the second quantum dot light emitting layer, the spacer layer comprising a plurality of ZnS quantum dots; the thickness of the spacing layer is 10-16 nm;
forming a first quantum dot light emitting layer on the spacer layer;
forming an anode on the first quantum dot light-emitting layer to obtain a quantum dot light-emitting diode;
the thickness of the spacing layer is less than or equal to that of the first quantum dot light-emitting layer, and/or the thickness of the spacing layer is less than or equal to that of the second quantum dot light-emitting layer;
the spacing layer covers the first quantum dot light-emitting layer in the orthographic projection area of the first quantum dot light-emitting layer, and/or the spacing layer covers the second quantum dot light-emitting layer in the orthographic projection area of the second quantum dot light-emitting layer;
the material for forming the first quantum dot light-emitting layer and the material for forming the second quantum dot light-emitting layer are binary phase quantum dots, ternary phase quantum dots or quaternary phase quantum dots respectively;
wherein,
the binary phase quantum dots comprise at least one of CdS, cdSe, cdTe, inP, agS, pbS, pbSe and HgS;
the ternary phase quantum dots comprise Zn X Cd 1-X S、Cu X In 1-X S、Zn X Cd 1-X Se、Zn X Se 1-X S、Zn X Cd 1-X Te、PbSe X S 1-X At least one of (1), wherein 0<X<1;
The quaternary phase quantum dots comprise Zn X Cd 1-X S/ZnSe、Cu X In 1-X S/ZnS、Zn X Cd 1-X Se/ZnS、CuInSeS、Zn X Cd 1-X Te/ZnS、PbSe X S 1-X At least one of/ZnS, wherein 0<X<1。
6. The method of claim 5, wherein the first quantum dot light emitting layer has a thickness of 15 to 25nm, and the second quantum dot light emitting layer has a thickness of 15 to 25nm.
7. The method of claim 5, wherein the first quantum dot light emitting layer is formed of the same material as the second quantum dot light emitting layer.
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CN105098084A (en) * | 2015-06-16 | 2015-11-25 | 武汉华星光电技术有限公司 | Quantum dot-based light-emitting diode and display device |
CN106206967A (en) * | 2016-08-10 | 2016-12-07 | 京东方科技集团股份有限公司 | Quantum dot light emitting device and preparation method thereof, display device |
KR20180047820A (en) * | 2016-11-01 | 2018-05-10 | 엘지디스플레이 주식회사 | Quantum dot emitting diode and Quantum dot display device including the same |
CN107093673A (en) * | 2017-05-17 | 2017-08-25 | 南昌航空大学 | Multi-layer quantum white point luminescent device |
CN109935725A (en) * | 2017-12-15 | 2019-06-25 | Tcl集团股份有限公司 | Light emitting diode with quantum dots and its preparation method and application |
CN109980105A (en) * | 2017-12-28 | 2019-07-05 | Tcl集团股份有限公司 | A kind of QLED device |
CN110212105A (en) * | 2019-06-26 | 2019-09-06 | 苏州星烁纳米科技有限公司 | Quantum dot light emitting device and preparation method thereof, lighting device |
CN110611033A (en) * | 2019-08-29 | 2019-12-24 | 深圳市华星光电半导体显示技术有限公司 | White light quantum dot light-emitting diode device and preparation method thereof |
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