CN111384257A - Quantum dot electroluminescent device and display - Google Patents
Quantum dot electroluminescent device and display Download PDFInfo
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- CN111384257A CN111384257A CN201811625837.XA CN201811625837A CN111384257A CN 111384257 A CN111384257 A CN 111384257A CN 201811625837 A CN201811625837 A CN 201811625837A CN 111384257 A CN111384257 A CN 111384257A
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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]
- H10K50/14—Carrier transporting layers
- H10K50/16—Electron transporting layers
- H10K50/166—Electron transporting layers comprising a multilayered structure
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/80—Constructional details
- H10K50/805—Electrodes
- H10K50/82—Cathodes
-
- 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
- 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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- Physics & Mathematics (AREA)
- Optics & Photonics (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Electroluminescent Light Sources (AREA)
Abstract
The invention relates to a quantum dot electroluminescent device with long service life and a display. According to the quantum dot electroluminescent device and the display comprising the same, the electron transmission layer and the inert metal layer are arranged on the quantum dot light emitting layer, wherein the electron transmission layer comprises the inorganic electron transmission layer and the organic electron transmission layer which are arranged in a stacked mode, the inert metal layer contains the inert metal with metal activity arranged behind hydrogen, and therefore the inert metal layer is matched with the electron transmission layer and the quantum dot light emitting layer, the service life of the whole quantum dot electroluminescent device can be prolonged remarkably, and the light emitting stability is improved.
Description
Technical Field
The invention relates to the technical field of electroluminescence, in particular to a quantum dot electroluminescent device and a display.
Background
Nanocrystalline semiconductor materials, also known as nanocrystals, are composed of a finite number of atoms, at least two dimensions are on the order of nanometers, the appearance is like a tiny dot or rod/wire, the internal electron motion is limited in two-dimensional space, and the quantum confinement effect is particularly remarkable. The nano-crystal semiconductor material can emit a spectrum with narrow half-peak width (usually, the half-peak width is less than 40nm) under the excitation of light or electricity, the luminescent color is mainly determined by the particle size, and the luminescent material has the characteristics of high luminescent color purity, high luminescent quantum efficiency, stable performance and the like. The nanocrystalline semiconductor material has great application potential in next generation display technology due to the advantages. The excitation mode generally includes both photoluminescence and electroluminescence. The photoluminescence mode mainly uses a blue light LED as an excitation light source and is applied to the illumination field, a backlight module of LCD display and the like. The electroluminescent device can be applied to the fields of illumination and display, and particularly has wider display application prospect.
An electroluminescent device made of a nanocrystal semiconductor material has recently received much attention as a new light-emitting device. Because of the characteristics of quantum confinement effects, electroluminescent diodes made with nanocrystalline semiconductor materials, also known as QLEDs (Q stands for the meaning of quantum, and a particular luminescent material may include materials in the form of dots, rods, or wires).
Compared with the traditional Organic Light Emitting Diode (OLED), the QLED has the characteristics of more excellent color purity, brightness, visual angle and the like. The nano-crystal semiconductor material can be dispersed in a solvent to prepare printing materials such as ink and the like, is suitable for preparation by a solution method, and can be used for manufacturing a luminescent film by methods such as printing, pad printing, spin coating, blade coating and the like to realize large-area solution processing. If a Drop on Demand (Drop) technology similar to ink jet Printing is adopted, the luminescent material can be accurately deposited at the set position according to the required quantity, and a precise pixel thin film structure is deposited to manufacture the large-size color QLED display screen. Due to the characteristics, the QLED taking the nano-crystal semiconductor material as the light emitting layer has wide application prospects in the fields of solid-state lighting, flat panel display and the like, and is widely concerned by academia and industry.
Through the improvement of the nano-crystal semiconductor material and the continuous optimization of the structure of the QLED device, the luminous performance of the existing QLED device is greatly improved, but certain performances can not meet the requirements, and especially the long-term service life of the device has a certain gap with the requirements of industrialized production.
Disclosure of Invention
Accordingly, there is a need for a long lifetime quantum dot electroluminescent device and display.
A quantum dot electroluminescent device comprises a substrate, an anode layer, a luminescent layer, an electron transport layer and an inert metal layer, wherein the anode layer is arranged on the substrate, the luminescent layer is arranged on the anode layer, the electron transport layer is arranged on the luminescent layer, and the inert metal layer is arranged on the electron transport layer; the light-emitting layer is a quantum dot light-emitting layer; the electron transport layer comprises an inorganic electron transport layer and an organic electron transport layer which are arranged in a stacked mode; the inert metal layer contains an inert metal that has metal activity arranged behind hydrogen.
In one embodiment, the inert metal layer comprises a cathode layer; or
The inert metal layer forms an electron injection layer, the quantum dot electroluminescent device further comprises a cathode layer arranged on the inert metal layer, and the material of the cathode layer is different from that of the inert metal layer.
In one embodiment, the inert metal is selected from at least one of copper, silver, platinum, and gold.
In one embodiment, the inert metal layer contains, in addition to the inert metal, other metals having a metal activity that is more active than the inert metal.
In one embodiment, the other metal is selected from at least one of magnesium, calcium, aluminum, and ytterbium.
In one embodiment, the volume ratio of the inert metal to other metals in the inert metal layer is 99: 1-50: 50.
In one embodiment, the inorganic electron transport layer is made of a material selected from ZnO and/or TiO doped with at least one of Mg, Y and Sc2(ii) a And/or
The material of the organic electron transport layer is selected from anthracene, fluorene, triazine, naphthalene, phenanthrene, fluorine, triazine, fluorine, and fluorine, which contain or do not contain substituent groups,
At least one of pyrene, quinoline, fluoranthene, benzanthracene, phenanthroline, triphenylene, pyridine, pyrimidine, imidazole, oxadiazole, and derivatives of the above compounds; and/or
The material of the quantum dot light-emitting layer is at least one of quantum dots taking CdSe, CdS, CdTe, PbS, PbTe, ZnSe, InP, CuZnS, CuZnSe, CuZnCdS, CuZnInSe and CuInP as cores.
In one embodiment, the inorganic electron transport layer is made of ZnO, the organic electron transport layer is made of Alq3, and the inert metal layer is made of Ag; or
The inorganic electron transport layer is made of ZnO, the organic electron transport layer is made of Alq3, and the inert metal layer is made of AgMg alloy; or
The inorganic electron transport layer is made of ZnMgO, the organic electron transport layer is made of Alq3, and the inert metal layer is made of Ag; or
The inorganic electron transport layer is made of ZnMgO, the organic electron transport layer is made of N-164, and the inert metal layer is made of Ag; or
The inorganic electron transport layer is made of ZnMgO, the organic electron transport layer is made of a mixed material of N-164 and LiQ, and the inert metal layer is made of Ag.
In one embodiment, the thickness of the inorganic electron transport layer is 15nm to 30 nm; the thickness of the organic electron transmission layer is 10 nm-20 nm; the thickness of the inert metal layer is 8 nm-20 nm or 150 nm-200 nm.
In one embodiment, the material of the light-emitting layer is CdSe core/ZnS shell quantum dots, and the thickness is 15 nm-25 nm.
A display comprising a quantum dot electroluminescent device as described in any one of the above embodiments.
According to the quantum dot electroluminescent device and the display comprising the same, the electron transmission layer and the inert metal layer are arranged on the quantum dot light emitting layer, wherein the electron transmission layer comprises the inorganic electron transmission layer and the organic electron transmission layer which are arranged in a stacked mode, the inert metal layer contains the inert metal with metal activity arranged behind hydrogen, and therefore the inert metal layer is matched with the electron transmission layer and the quantum dot light emitting layer, the service life of the whole quantum dot electroluminescent device can be prolonged remarkably, and the light emitting stability is improved.
Drawings
Fig. 1 is a schematic structural diagram of a quantum dot electroluminescent device according to an embodiment of the present invention.
Detailed Description
To facilitate an understanding of the invention, the invention will now be described more fully with reference to the accompanying drawings. Preferred embodiments of the present invention are shown in the drawings. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
It will be understood that when an element is referred to as being "on" another element, it can be directly on the other element or intervening elements may also be present. When an element is referred to as being "connected" to another element, it can be directly connected to the other element or intervening elements may also be present.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.
As shown in fig. 1, the present invention provides a quantum dot electroluminescent device 10 including a substrate 100, an anode layer 200, a light emitting layer 300, an electron transport layer 400, and an inert metal layer 500. The anode layer 200 is disposed on the substrate 100, the light emitting layer 300 is disposed on the anode layer 200, the electron transport layer 400 is disposed on the light emitting layer 300, and the inert metal layer 500 is disposed on the electron transport layer 400. The light emitting layer 300 is a quantum dot light emitting layer. The electron transport layer 400 includes an inorganic electron transport layer 410 and an organic electron transport layer 420, which are stacked. The inert metal layer 500 contains an inert metal that has metal activity that is driven off after hydrogen.
The inert metal layer 500 may directly form a cathode layer, and the thickness may be in a range of 10nm to 200nm, specifically, when the device is a top emission device structure, the inert metal layer is thinner, generally 8nm to 20 nm; when the device is a bottom emission device structure, the inert metal layer is thicker, generally 150nm to 200 nm. Alternatively, the inert metal layer 500 constitutes an electron injection layer and may have a thickness ranging from 1nm to 20 nm. When the inert metal layer 500 serves as an electron injection layer, the quantum dot electroluminescent device 10 further includes a cathode layer (not shown) disposed on the inert metal layer, and the material of the cathode layer is different from that of the inert metal layer.
In one specific example, the inert metal is selected from at least one of copper, silver, platinum, and gold.
Further, in some specific examples, the inert metal layer 500 may contain other metals in addition to the inert metal. The other metal is preferably a metal having metal activity more active than the inert metal, and may be at least one selected from magnesium, calcium, aluminum, and ytterbium. More specifically, the volume ratio of the inert metal to the other metals in the inert metal layer 500 is 99:1 to 50:50, and may be, for example, 99:1, 95:5, 90:10, 80:20, 70:30, 60:40, or 50: 50. The inorganic electron transport layer 410 of the electron transport layer 400 is closer to the light emitting layer 300 than the organic electron transport layer 420, and the organic electron transport layer 420 is closer to the inert metal layer 500.
In one specific example, the inorganic electron transport layer 410 is selected from ZnO and/or TiO2 that is undoped or doped with at least one metal selected from magnesium, yttrium, and scandium, and may have a thickness in a range of 10nm to 40 nm.
The organic electron transport layer 420 is made of a material selected from the group consisting of substituted or unsubstituted anthracene, fluorene, triazine, naphthalene, phenanthrene, anthracene,
At least one of pyrene, quinoline, fluoranthene, benzanthracene, phenanthroline, triphenylene, pyridine, pyrimidine, imidazole, oxadiazole, and derivatives of the above compounds (e.g., Alq3, LiQ, etc.), and the thickness thereof may be in the range of 5nm to 40 nm.
The material of the light emitting layer 300 is at least one selected from quantum dots with CdSe, CdS, CdTe, PbS, PbTe, ZnSe, InP, CuZnS, CuZnSe, CuZnCdS, CuZnInSe and CuInP as cores, and the thickness of the quantum dots can be within the range of 10nm to 50 nm.
In some preferred embodiments, the inorganic electron transport layer 410 is ZnO, the organic electron transport layer 420 is Alq3, and the inert metal layer 500 is Ag; or the inorganic electron transport layer 410 is made of ZnO, the organic electron transport layer 420 is made of Alq3, and the inert metal layer 500 is made of AgMg alloy, such as AgMg alloy with the volume ratio of Ag to Mg being 9: 1; or the inorganic electron transport layer 410 is ZnMgO, the organic electron transport layer 420 is Alq3, and the inert metal layer 500 is Ag; or the inorganic electron transport layer 410 is ZnMgO (Mg-doped ZnO), the organic electron transport layer 420 is N-164, and the inert metal layer 500 is Ag; or the inorganic electron transport layer 410 is ZnMgO, the organic electron transport layer 420 is a mixture of N-164 and LiQ, for example, the volume ratio of N-164 to LiQ is 2:8, and the inert metal layer 500 is Ag.
Further preferably, the thickness of the inorganic electron transporting layer 410 is 15nm to 30nm, such as 25 nm; the thickness of the organic electron transport layer 420 is 10nm to 20nm, and may be 15nm, for example; the thickness of the inert metal layer 500 is 8nm to 20nm (corresponding to a top emission type device, preferably, a transparent cathode layer is further provided on the inert metal layer 500) or 150nm to 200nm (corresponding to a bottom emission type device).
Further, the material of the light emitting layer 300, which is combined with the preferable materials of the inorganic electron transport layer 410, the organic electron transport layer 420, and the inert metal layer 500, may be CdSe core/ZnS shell quantum dots, and the thickness may be 15nm to 25 nm.
Still further, the quantum dot electroluminescent device 10 may further include at least one of a hole injection layer and a hole transport layer between the anode layer 200 and the light emitting layer 300.
According to the quantum dot electroluminescent device and the display comprising the same, the electron transmission layer and the inert metal layer are arranged on the quantum dot light emitting layer, wherein the electron transmission layer comprises the inorganic electron transmission layer and the organic electron transmission layer which are arranged in a stacked mode, the inert metal layer contains the inert metal with metal activity arranged behind hydrogen, and therefore the inert metal layer is matched with the electron transmission layer and the quantum dot light emitting layer, the service life of the whole quantum dot electroluminescent device can be prolonged remarkably, and the light emitting stability is improved.
The quantum dot electroluminescent device 10 can be used as a backlight module or a display module in a display, such as various flat panel displays.
The structure and performance of the quantum dot electroluminescent device according to the present invention will be described in further detail with reference to specific examples and comparative examples.
Example 1
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/Alq 3 organic electron transport layer/inert metal Ag layer as cathode, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the ZnO layer by vacuum thermal deposition to a thickness of 15 nm.
(6) Preparing a metal cathode: an inert metal silver (Ag, which is behind "hydrogen" in the metal reactive sequence, i.e., less active than "hydrogen") is evaporated in a thickness of 150nm over the organic electron transport layer by vacuum thermal evaporation to form the cathode of the electroluminescent device.
Example 2
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/Alq 3 organic electron transport layer/alloy layer of inert metal Ag and active metal Mg as cathode, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the ZnO layer by vacuum thermal deposition to a thickness of 15 nm.
(6) Preparing a metal cathode: and (3) evaporating a magnesium-silver alloy (the ratio of magnesium to silver is 1:9) with the thickness of 150nm on the organic electron transport layer by a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
Example 3
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/Alq 3 organic electron transport layer/inert metal Ag layer as electron injection layer/Al cathode layer, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the ZnO layer by vacuum thermal deposition to a thickness of 15 nm.
(6) Preparing an electron injection layer: firstly, inert metal silver with the thickness of 10nm is evaporated on the organic electron transport layer by a vacuum thermal evaporation mode to be used as an electron injection layer.
(7) Preparing a metal cathode: aluminum was deposited on the electron injection layer by vacuum thermal deposition to a thickness of 150nm to form a cathode of the electroluminescent device.
Example 4
The structure of the device is as follows: the glass-ITO/PEDOT comprises a PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/Alq 3 organic electron transport layer/an alloy layer of inert metal Ag and active metal Mg, which is used as an electron injection layer/Al cathode layer, and the preparation method comprises the following steps:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the ZnO layer by vacuum thermal deposition to a thickness of 15 nm.
(6) Preparing an electron injection layer: a magnesium-silver alloy (the volume ratio of magnesium to silver is 1:9) with the thickness of 10nm is evaporated on the organic electron transport layer by a vacuum thermal evaporation method to be used as an electron injection layer.
(7) Preparing a metal cathode: aluminum was deposited on the electron injection layer by vacuum thermal deposition to a thickness of 150nm to form a cathode of the electroluminescent device.
Comparative example 1
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/Al cathode layer, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing a metal cathode: aluminum (Al, which precedes "hydrogen" in the metal reactive sequence, i.e., is more active than "hydrogen") was evaporated in a thickness of 150nm over the electron transport layer by vacuum thermal evaporation to form the cathode of the electroluminescent device.
Comparative example 2
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/Alq 3 organic electron transport layer/Al cathode layer, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the ZnO layer by vacuum thermal deposition to a thickness of 15 nm.
(6) Preparing a metal cathode: aluminum (Al, which precedes "hydrogen" in the metal reactivity sequence, i.e., is more active than "hydrogen") was evaporated in a thickness of 150nm by vacuum thermal evaporation over the organic electron transport layer to form the cathode of the electroluminescent device.
Comparative example 3
The structure of the device is as follows: the glass-ITO/PEDOT comprises a PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnO inorganic electron transport layer/inert metal Ag layer as a cathode, and the preparation method comprises the following steps:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) is spin-coated at the rotating speed of 3000rpm/min for 30 seconds, and then is baked at 120 ℃ for 10 minutes to obtain a ZnO layer film with the thickness of 25 nm.
(5) Preparing a metal cathode: and (3) evaporating an Ag layer with the thickness of 150nm on the electron transport layer by a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
Comparative example 4
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/Alq 3 organic electron transport layer/inert metal Ag layer as cathode, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparing an organic electron transport layer: an Alq3 thin film with a thickness of 15nm was deposited on the quantum dot light emitting layer by vacuum thermal deposition.
(5) Preparing a metal cathode: and (3) evaporating an Ag layer with the thickness of 150nm on the electron transport layer by a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
The luminous performance of the above examples 1 to 4 and comparative examples 1 to 4 was tested, the time for the luminance of the device to decay to 50% was tested in a 1000 nit initial luminance, constant current mode, and the decay time of comparative example 1 was normalized to 100%, to obtain the corresponding decay times of examples 1 to 4 and comparative examples 2 to 4, and the results are shown in table 1 below.
TABLE 1
| Comparative example 1 | Comparative example 2 | Comparative example 3 | Comparative example 4 | Example 1 | Example 2 | Example 3 | Example 4 |
| 100％ | 150％ | 120％ | 65％ | 720％ | 320％ | 710％ | 300％ |
It can be seen from table 1 that the lifetime of the device can be improved to a certain extent by adding the organic electron transport layer between the relatively active metal aluminum and the ZnO layer, and the lifetime of the QLED device is significantly improved by using the combination of the organic electron transport layer and the inert metal silver on the ZnO layer.
Further, based on example 1, the present invention further performed performance studies on QLED devices with different material and thickness parameters, and the device structures were as in examples 5, 6, 7, and 8 below.
Example 5
The structure of the device is as follows: PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnMgO inorganic electron transport layer/Alq 3 organic electron transport layer/inert metal Ag layer as cathode, and the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparation of ZnMgO layer: the nano ZnMgO ink (60mg/ml) is spin-coated at a rotating speed of 3000rpm/min for 30 seconds, and then baked at 120 ℃ for 10 minutes to obtain a ZnMgO layer film with a thickness of 25 nm.
(5) Preparing an organic electron transport layer: a film of Alq3 was deposited on the ZnMgO layer by vacuum thermal deposition to a thickness of 15 nm.
(6) Preparing a metal cathode: an inert metal silver (Ag, which is behind "hydrogen" in the metal reactive sequence, i.e., less active than "hydrogen") is evaporated in a thickness of 150nm over the organic electron transport layer by vacuum thermal evaporation to form the cathode of the electroluminescent device.
Example 6
The structure of the device is as follows: the glass-ITO/PEDOT comprises a PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnMgO inorganic electron transport layer/N-164 organic electron transport layer/inert metal Ag layer as a cathode, and the preparation method comprises the following steps:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparation of ZnMgO layer: the nano ZnMgO ink (60mg/ml) is spin-coated at a rotating speed of 3000rpm/min for 30 seconds, and then baked at 120 ℃ for 10 minutes to obtain a ZnMgO layer film with a thickness of 25 nm.
(5) Preparing an organic electron transport layer: a film of an electron transport layer material (Novaled) having a designation N-164 was deposited on the ZnMgO layer in a thickness of 15nm by vacuum thermal deposition.
(6) Preparing a metal cathode: and (3) evaporating inert metal silver with the thickness of 150nm on the organic electron transport layer in a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
Example 7
The structure of the device is as follows: glass-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnMgO inorganic electron transport layer/N-164 LiQ co-evaporation organic electron transport layer/inert metal Ag layer as cathode, the preparation method is as follows:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparation of ZnMgO layer: the nano ZnMgO ink (60mg/ml) is spin-coated at a rotating speed of 3000rpm/min for 30 seconds, and then baked at 120 ℃ for 10 minutes to obtain a ZnMgO layer film with a thickness of 25 nm.
(5) Preparing an organic electron transport layer: a15 nm thick N-164: LiQ (volume ratio of N-164 to LiQ of 2:8) film was co-evaporated over the ZnMgO layer.
(6) Preparing a metal cathode: and (3) evaporating inert metal silver with the thickness of 150nm on the organic electron transport layer in a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
Example 8
The structure of the device is a top emitting device: ITO-Ag-ITO/PEDOT, PSS hole injection layer/TFB hole transport layer/CdSe/ZnS quantum dot luminescent layer/ZnMgO inorganic electron transport layer/N-164 LiQ co-evaporation organic electron transport layer/Ag electron injection layer/IZO cathode, and the preparation method is as follows:
(1) preparing a hole injection layer: on the glass-ITO substrate, PEDOT: PSS ink (40mg/ml) was spin-coated at a rotation speed of 1200rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (40mg/ml) was spin-coated at 1000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing a luminescent layer: CdSe/ZnS quantum dot ink (20mg/ml) was spin-coated at a rotation speed of 1500rpm/min for 30 seconds, and then baked at 100 ℃ for 10 minutes to obtain a light-emitting layer thin film with a thickness of 18 nm.
(4) Preparation of ZnMgO layer: the nano ZnMgO ink (60mg/ml) is spin-coated at a rotating speed of 3000rpm/min for 30 seconds, and then baked at 120 ℃ for 10 minutes to obtain a ZnMgO layer film with a thickness of 25 nm.
(5) Preparing an organic electron transport layer: a25 nm thick N-164: LiQ (volume ratio of N-164 to LiQ of 2:8) film was co-evaporated over the ZnMgO layer.
(6) Preparing an Ag electron injection layer: and evaporating metal silver with the thickness of 8nm on the organic electron transport layer by a vacuum thermal evaporation mode to form an electron injection layer.
(7) Preparing a transparent cathode: IZO (transparent conductive oxide containing In and Zn elements) of 70nm was deposited on the Ag electron injection layer by sputtering.
The luminous performance of the above examples 5 to 8 was studied, the time for the luminance of the device to decay to 50% was tested in a 1000 nit initial luminance, constant current mode, and the decay time of comparative example 1 was normalized to 100%, to obtain the corresponding decay times of examples 5 to 8, and the results are shown in table 2 below.
TABLE 2
| Comparative example 1 | Example 1 | Example 5 | Example 6 | Example 7 | Example 8 |
| 100％ | 720％ | 780％ | 850％ | 1200％ | 1120％ |
As can be seen from Table 2, the devices of examples 5 to 8 have better device lifetime, wherein examples 5 to 7 are bottom emission devices, and example 8 is a top emission device.
The present invention further investigated the effect of inert metals on the performance of OLED devices, as shown in comparative example 5 and comparative example 6 below.
Comparative example 5
The structure of the device is as follows: glass-ITO/PEDOT PSS hole injection layer/TFB hole transport layer/CBP Ir (ppy)3The organic light-emitting layer/Alq 3 organic electron transport layer/metal Al electrode is prepared by the following steps:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing an organic light-emitting layer: co-evaporation of CBP Ir (ppy)3Organic light emitting layer film (CBP and Ir (ppy)3The volume ratio of (1) is 90% to 10%).
(4) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the organic light-emitting layer by vacuum thermal deposition to a thickness of 35 nm.
(5) Preparing a metal cathode: and evaporating metal Al with the thickness of 150nm on the organic electron transport layer by a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
Comparative example 6
The structure of the device is as follows: glass-ITO/PEDOT PSS hole injection layer/TFB hole transport layer/CBP: ir (ppy)3The organic light-emitting layer/Alq 3 organic electron transport layer/inert metal Ag layer is prepared by the following steps:
(1) preparing a hole injection layer: on a glass-ITO substrate, PEDOT: PSS ink (20mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 110 ℃ for 15 minutes to obtain a hole injection layer film.
(2) Preparing a hole transport layer: the TFB ink (20mg/ml) was spin-coated at 2000rpm/min for 30 seconds, and then baked at 150 ℃ for 30 minutes to obtain a hole transport layer thin film.
(3) Preparing an organic light-emitting layer: co-evaporation of CBP Ir (ppy)3Organic light emitting layer film (CBP and Ir (ppy)3The volume ratio of (1) is 90% to 10%).
(4) Preparing a ZnO layer: the nano ZnO ink (60mg/ml) was spin-coated at a rotation speed of 3000rpm/min for 30 seconds, and then baked at 120 ℃ for 10 minutes to obtain a ZnO layer thin film.
(5) Preparing an organic electron transport layer: a thin film of Alq3 was deposited on the organic light-emitting layer by vacuum thermal deposition to a thickness of 35 nm.
(6) Preparing a metal cathode: and (3) evaporating inert metal silver with the thickness of 150nm on the organic electron transport layer in a vacuum thermal evaporation mode to form a cathode of the electroluminescent device.
The luminescent properties of comparative examples 5 to 6 were investigated, and the device life of comparative example 5 was 100%, and the device result of comparative example 6 was 20%. In view of the fact that an inorganic electron transport layer is not generally used in an OLED device, the results of comparative examples 5 to 6 show that the device structure of "inorganic electron transport layer + organic electron transport layer + inert metal" for a quantum dot light emitting device (QLED) according to the present invention is not suitable for an OLED device including an organic light emitting layer in terms of increasing the lifetime of the device.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (11)
1. A quantum dot electroluminescent device is characterized by comprising a substrate, an anode layer, a luminescent layer, an electron transmission layer and an inert metal layer, wherein the anode layer is arranged on the substrate, the luminescent layer is arranged on the anode layer, the electron transmission layer is arranged on the luminescent layer, and the inert metal layer is arranged on the electron transmission layer; the light-emitting layer is a quantum dot light-emitting layer; the electron transport layer comprises an inorganic electron transport layer and an organic electron transport layer which are arranged in a stacked mode; the inert metal layer contains an inert metal that has metal activity arranged behind hydrogen.
2. A quantum dot electroluminescent device as claimed in claim 1, wherein the inert metal layer constitutes a cathode layer; or
The inert metal layer forms an electron injection layer, the quantum dot electroluminescent device further comprises a cathode layer arranged on the inert metal layer, and the material of the cathode layer is different from that of the inert metal layer.
3. The quantum dot electroluminescent device of claim 2, wherein the inert metal is selected from at least one of copper, silver, platinum, and gold.
4. The quantum dot electroluminescent device according to claim 2, wherein the inert metal layer contains, in addition to the inert metal, another metal having a metal activity more active than the inert metal.
5. The quantum dot electroluminescent device according to claim 4, wherein the other metal is selected from at least one of magnesium, calcium, aluminum, and ytterbium.
6. The quantum dot electroluminescent device according to claim 4, wherein the volume ratio of the inert metal to the other metals in the inert metal layer is 99:1 to 50: 50.
7. The quantum dot electroluminescent device according to any one of claims 1 to 6, wherein the inorganic electron transport layer is made of a material selected from ZnO and/or TiO that is undoped or doped with at least one metal selected from magnesium, yttrium, and scandium2(ii) a And/or
The material of the organic electron transport layer is selected from anthracene, fluorene, triazine, naphthalene, phenanthrene, fluorine, triazine, fluorine, and fluorine, which contain or do not contain substituent groups,
At least one of pyrene, quinoline, fluoranthene, benzanthracene, phenanthroline, triphenylene, pyridine, pyrimidine, imidazole, oxadiazole, and derivatives of the above compounds; and/or
The material of the quantum dot light-emitting layer is at least one of quantum dots taking CdSe, CdS, CdTe, PbS, PbTe, ZnSe, InP, CuZnS, CuZnSe, CuZnCdS, CuZnInSe and CuInP as cores.
8. The quantum dot electroluminescent device according to any one of claims 1 to 6, wherein the inorganic electron transport layer is made of ZnO, the organic electron transport layer is made of Alq3, and the inert metal layer is made of Ag; or
The inorganic electron transport layer is made of ZnO, the organic electron transport layer is made of Alq3, and the inert metal layer is made of AgMg alloy; or
The inorganic electron transport layer is made of ZnMgO, the organic electron transport layer is made of Alq3, and the inert metal layer is made of Ag; or
The inorganic electron transport layer is made of ZnMgO, the organic electron transport layer is made of N-164, and the inert metal layer is made of Ag; or
The inorganic electron transport layer is made of ZnMgO, the organic electron transport layer is made of a mixed material of N-164 and LiQ, and the inert metal layer is made of Ag.
9. The quantum dot electroluminescent device of claim 8, wherein the inorganic electron transport layer has a thickness of 15nm to 30 nm; the thickness of the organic electron transmission layer is 10 nm-20 nm; the thickness of the inert metal layer is 8 nm-20 nm or 150 nm-200 nm.
10. The quantum dot electroluminescent device according to claim 9, wherein the material of the light emitting layer is CdSe core/ZnS shell quantum dots, and the thickness is 15nm to 25 nm.
11. A display comprising the quantum dot electroluminescent device according to any one of claims 1 to 10.
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| WO2022143820A1 (en) * | 2020-12-31 | 2022-07-07 | Tcl科技集团股份有限公司 | Light-emitting device and preparation method therefor |
| WO2023125072A1 (en) * | 2021-12-29 | 2023-07-06 | Tcl科技集团股份有限公司 | Light-emitting diode and preparation method therefor |
| WO2023206228A1 (en) * | 2022-04-28 | 2023-11-02 | 京东方科技集团股份有限公司 | Light-emitting device, manufacturing method therefor, display substrate and display apparatus |
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| WO2023125072A1 (en) * | 2021-12-29 | 2023-07-06 | Tcl科技集团股份有限公司 | Light-emitting diode and preparation method therefor |
| WO2023206228A1 (en) * | 2022-04-28 | 2023-11-02 | 京东方科技集团股份有限公司 | Light-emitting device, manufacturing method therefor, display substrate and display apparatus |
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