CN113809252A - Up-conversion device and manufacturing method thereof - Google Patents
Up-conversion device and manufacturing method thereof Download PDFInfo
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- CN113809252A CN113809252A CN202110893394.8A CN202110893394A CN113809252A CN 113809252 A CN113809252 A CN 113809252A CN 202110893394 A CN202110893394 A CN 202110893394A CN 113809252 A CN113809252 A CN 113809252A
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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]
- H10K50/17—Carrier injection layers
-
- 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
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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]
- H10K50/17—Carrier injection layers
- H10K50/171—Electron injection 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
Abstract
The invention discloses an up-conversion device and a manufacturing method thereof, wherein the up-conversion device comprises: the light-emitting diode comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generation layer, a hole transport layer, a light-emitting layer, an electron transport layer and a third electrode, wherein the substrate, the first electrode, the dielectric layer and the first intermediate layer are sequentially arranged from bottom to top; the first intermediate layer and the second intermediate layer are respectively a carrier control layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier control layer. The up-conversion device is of a three-end non-vertical structure, can enrich photo-generated carriers, improve the light conversion efficiency and reduce the starting voltage of the device, the carrier regulation and control layer enables the device to be kept in a closed state in a dark state, the transport efficiency of the photo-generated carriers is improved, a window between the second electrode and the third electrode is beneficial to absorption of long wavelength infrared light, and scattering and absorption of the electrode of the vertical structure device to the infrared light are avoided.
Description
Technical Field
The invention relates to the technical field of photoelectron, in particular to an up-conversion device and a manufacturing method thereof.
Background
Infrared light is an electromagnetic wave between visible light waves and microwaves, the wavelength range of which extends from 760nm to 1mm, and infrared technology has wide application in night vision devices, area detection, national defense security, semiconductor wafer detection and the like. However, the conventional CCD and CMOS sensor devices cannot detect the infrared band larger than 1 μm, and in the industrial process, the conventional infrared imaging device is formed by connecting an infrared detector and a silicon-based readout circuit based on an indium bonding technology, which is a one-chip process, and many factors of which limit the yield and the size expansibility thereof. Furthermore, in order to manufacture a larger size pixel array, the size of each pixel must therefore be reduced, which places stringent process requirements on the device.
Based on the disadvantages of conventional infrared imaging devices, photo-upconversion devices are proposed that can convert low-energy incident radiation of photons into high-energy output radiation. The infrared up-conversion luminescent device is formed by directly integrating a Photoelectric Detector (PD) with a near-infrared absorption semiconductor material and a Light Emitting Diode (LED) with visible light emitting capability, absorbs infrared light through a PD unit, generates photocurrent and directly injects the photocurrent into the LED, and drives the LED to generate visible light. However, the existing infrared up-conversion luminescent device has the problems of low light-light conversion efficiency, overlarge starting voltage, too short infrared detection wavelength and the like.
Thus, there is still a need for improvement and development of the prior art.
Disclosure of Invention
The present invention is directed to an up-conversion device and a method for manufacturing the same, which are provided to solve the above-mentioned problems of low light-light conversion efficiency, excessive on-voltage, and short infrared detection wavelength of the existing infrared up-conversion light emitting device.
The technical scheme adopted by the invention for solving the problems is as follows:
in a first aspect, an embodiment of the present invention provides an up-conversion device, including: the light-emitting diode comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generation layer, a hole transport layer, a light-emitting layer, an electron transport layer and a third electrode, wherein the substrate, the first electrode, the dielectric layer and the first intermediate layer are sequentially arranged from bottom to top; the first intermediate layer and the second intermediate layer are respectively a carrier control layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier control layer.
The up-conversion device, wherein the up-conversion device further comprises: a hole injection layer disposed between the carrier generation layer and the hole transport layer, and an electron injection layer disposed between the electron transport layer and the third electrode.
The up-conversion device, wherein the first electrode, the second electrode and the third electrode are respectively one of metal, a transparent conductive film and heavily doped silicon.
The up-conversion device, wherein the transparent conductive film is at least one of an indium tin oxide semiconductor transparent conductive film, an aluminum-doped zinc oxide transparent conductive film, a silver nanowire, a carbon nanotube, graphene, or a metal grid.
The up-conversion device, wherein the metal is at least one of barium, calcium, aluminum, magnesium, tin, copper, silver, gold, and platinum.
The up-conversion device is characterized in that the carrier regulation and control layer and the carrier transmission layer are respectively at least one of silicon, silicon carbide, gallium antimonide, gallium arsenide, indium gallium arsenide, lead sulfide, lead selenide, silver sulfide, vanadium oxide, carbon nano tubes, carbon quantum dots, black scales, graphene and graphene oxide.
The upper conversion device, wherein the dielectric layer is at least one of silicon dioxide, silicon nitride, polyvinylpyrrolidone, polymethyl methacrylate, and poly (vinylidene fluoride-trifluoroethylene).
The up-conversion device, wherein the light emitting layer is at least one of quantum dots, perovskite, organic polymer and organic small molecule.
The up-conversion device, wherein the electron transport layer is at least one of zinc oxide, magnesium zinc oxide, indium tin oxide, titanium niobium oxide, tin oxide, and tin oxyfluoride.
In the up-conversion device, the hole injection layer is at least one of poly (3, 4-ethylenedioxythiophene) -polystyrene sulfonic acid, nickel oxide, molybdenum oxide, tin oxide, magnesium oxide, nickel magnesium oxide and nickel tin oxide.
The up-conversion device, wherein the electron injection layer is at least one of 8-hydroxyquinoline-lithium, lithium fluoride and aluminum oxide.
The upper converter part is characterized in that the preparation method of each layer in the upper converter part comprises at least one of a solution spin coating method, a vacuum thermal evaporation coating method, a vacuum electron beam thermal evaporation method, a magnetron sputtering method, a plasma enhanced chemical vapor deposition method, a pulse laser epitaxial deposition method and an atomic layer epitaxial deposition method.
In a second aspect, an embodiment of the present invention provides a method for manufacturing an up-conversion device, where the method includes:
pretreating the first electrode deposited on the substrate, and forming a dielectric layer on the pretreated first electrode;
forming an up-conversion on the dielectric layer;
forming a second intermediate layer and a carrier generation layer on the first intermediate layer; the first intermediate layer and the second intermediate layer are respectively a carrier regulation layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulation layer;
and sequentially forming a hole transport layer, a light emitting layer, an electron transport layer and a third electrode on the carrier generation layer.
Has the advantages that: the up-conversion device provided by the embodiment of the invention is a three-terminal non-vertical structure device, can enrich photo-generated carriers, improve the light-light conversion efficiency and reduce the starting voltage of the device, the carrier regulation and control layer can be used as a buffer layer to reduce exciton annihilation in a carrier generation layer, and can also prevent the electrically injected carriers from being injected into a light emitting layer and generating the photo-generated carriers, so that the device is kept in a closed state in a dark state, the transport efficiency and the light-light conversion efficiency of the photo-generated carriers are improved, a window between a second electrode and a third electrode in a three-terminal electrode structure is favorable for absorbing long-wavelength infrared light, and the scattering and absorption of the electrode of the vertical structure device to the infrared light are avoided.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, it is obvious that the drawings in the following description are only some embodiments described in the present invention, and for those skilled in the art, other drawings can be obtained according to the drawings without creative efforts.
Fig. 1 is a schematic structural diagram of an up-conversion device provided in an embodiment of the present invention;
FIG. 2 is a schematic diagram of the operation of the up-conversion device provided by the embodiment of the present invention when not being exposed to infrared light;
fig. 3 is a schematic diagram of the operation of the up-conversion device provided by the embodiment of the present invention when the up-conversion device is irradiated by infrared light.
The various symbols in the drawings: 0. a substrate; 1. a first electrode; 2. a dielectric layer; 3. a first intermediate layer; 4. a second intermediate layer; 5. a carrier generation layer; 6. a hole transport layer; 7. a light emitting layer; 8. an electron transport layer; 9. and a third electrode.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention clearer and clearer, the present invention is further described in detail below with reference to the accompanying drawings and examples. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
It should be noted that, if directional indications (such as up, down, left, right, front, and back … …) are involved in the embodiment of the present invention, the directional indications are only used to explain the relative positional relationship between the components, the movement situation, and the like in a specific posture (as shown in the drawing), and if the specific posture is changed, the directional indications are changed accordingly.
Infrared light is an electromagnetic wave between visible light waves and microwaves, the wavelength range of which extends from 760nm to 1mm, and infrared technology has wide application in night vision devices, area detection, national defense security, semiconductor wafer detection and the like. However, the conventional CCD and CMOS sensor devices cannot detect the infrared band greater than 1 μm, and in the industrial process, the conventional infrared imaging device is formed by connecting an infrared detector and a silicon-based readout circuit based on an indium bonding technology, and has become an industry standard program at present. In this system structure, each pixel point of the silicon-based readout integrated circuit is connected with the infrared detection unit in a one-to-one correspondence manner at the corresponding position, and the indium bonding technology is a one-at-a-time process, wherein a plurality of factors limit the yield and the size expansibility of the silicon-based readout integrated circuit. Furthermore, in order to manufacture a larger size pixel array, the size of each pixel must be reduced, which imposes strict process requirements on the device.
Based on the disadvantages of conventional infrared imaging devices, photo-upconversion devices are proposed that can convert low-energy incident radiation of photons into high-energy output radiation. The optical upconversion device mainly has two upconversion mechanisms, namely a nonlinear optical process and a linear optical process, wherein the nonlinear upconversion optical process needs two or more metastable energy states to store absorbed pump photon energy, and the energy accumulation of the pump photons can cause photon emission with higher energy. The infrared up-conversion luminescent device is formed by directly integrating a Photoelectric Detector (PD) with a near-infrared absorption semiconductor material and a Light Emitting Diode (LED) with visible light emitting capability, absorbs infrared light through a PD unit, generates photocurrent and directly injects the photocurrent into the LED, and drives the LED to generate visible light. This structure requires the infrared light detector to have a high optical response, while requiring the LED to have a low turn-on voltage and a high luminous efficiency. The existing developed up-conversion light-emitting device has the following main problems: (1) the up-conversion luminescence integrated by back-to-back reverse series connection of PD and LED, the device has natural carrier potential barrier and larger series resistance, the 'barrier layer' introduced for setting the 'optical switch' also makes the carrier potential barrier further increase; the interaction and recombination mechanism between the photon-generated carriers and the electrical injection carriers are not clear, which leads to the difficulty in obtaining devices with high conversion efficiency and low turn-on voltage at present; (2) the transparent electrode in the existing device is Indium Tin Oxide (ITO), and the material is difficult to realize effective balance among infrared transmittance, carrier concentration and mobility, so that the transmittance of the material in middle and far infrared bands is low, and the detection of the device on long-wavelength infrared light is seriously influenced; (3) it is difficult to balance the relationship between the conversion efficiency and the turn-on voltage, resulting in an excessive turn-on voltage of the device.
In order to solve the problems of the prior art, the present invention provides an up-conversion device, as shown in fig. 1, an up-conversion device provided in an embodiment of the present invention includes: the light-emitting diode comprises a substrate 0, a first electrode 1, a dielectric layer 2 and a first intermediate layer 3 which are sequentially arranged from bottom to top, a second intermediate layer 4 and a carrier generation layer 5 which are arranged on the first intermediate layer 3, and a hole transport layer 6, a light-emitting layer 7, an electron transport layer 8 and a third electrode 9 which are sequentially arranged on the carrier generation layer 5 from bottom to top; the first intermediate layer 3 and the second intermediate layer 4 are a carrier control layer and a second electrode, respectively, or the first intermediate layer 3 and the second intermediate layer 4 are a second electrode and a carrier control layer, respectively. The up-conversion device provided by the embodiment of the invention is a three-terminal non-vertical structure device, can enrich photo-generated carriers, improve the light-light conversion efficiency and reduce the starting voltage of the device, the carrier regulation and control layer can be used as a buffer layer to reduce exciton annihilation in a carrier generation layer, and can also prevent the electrically injected carriers from being injected into a light emitting layer and generating the photo-generated carriers, so that the device is kept in a closed state in a dark state, the transport efficiency and the light-light conversion efficiency of the photo-generated carriers are improved, a window between a second electrode and a third electrode in a three-terminal electrode structure is favorable for absorbing long-wavelength infrared light, and the scattering and absorption of the electrode of the vertical structure device to the infrared light are avoided.
Specifically, the up-conversion device provided by the embodiment of the invention can realize the conversion of infrared light to visible light under the action of bias voltage. For example, a first power supply is arranged on the first electrode 1, a second power supply is arranged between the second electrode and the third electrode 9, and the first power supply is used for applying a gate bias voltage, so that the first electrode 1 and the dielectric layer 2 form a capacitor-like structure for enriching a photon-generated carrier; the second power supply is connected between the second electrode and the third electrode 9, generates an electric field effect, drives the photon-generated carriers enriched in the carrier regulation layer and the carrier generation layer to be injected into the light-emitting layer 7, and is combined with the carriers injected by the third electrode 9 to emit light, so that the conversion of infrared light to visible light can be realized.
As shown in fig. 2 and fig. 3, which are schematic diagrams of the operation of the up-conversion device provided by the embodiment of the present invention, under no infrared light irradiation, holes are induced from the first electrode 1 through the dielectric layer 2, and holes enriched at the second electrode are difficult to inject into the light-emitting layer 7 due to the blocking of the carrier control layer, so that the device does not emit light. Under the irradiation of infrared light, the carrier regulation and control and carrier generation layer 5 absorbs the infrared light to generate photo-generated electrons and holes, the carriers generate the phenomena of carrier enrichment and amplification in the layer under the induction of an electric field through the combined action of the first electrode 1 and the dielectric layer 2, are injected into the light emitting layer 7 under the action of bias voltage, are compounded with the carriers injected by the third electrode 9 to emit visible light, and therefore the up-conversion process from the infrared light to the visible light is achieved. The up-conversion device provided by the embodiment can realize the conversion of infrared light to visible light, and has the advantages of high conversion efficiency, low lighting voltage and wide detection bandwidth.
In a specific implementation manner, projection surfaces of the substrate 0, the first electrode 1, the dielectric layer 2, and the first intermediate layer 3 on a horizontal plane completely coincide, the second intermediate layer 4 and the carrier generation layer 5 are arranged side by side on the first intermediate layer 3, a preset distance is provided between the second intermediate layer 4 and the carrier generation layer 5, projection surfaces of the hole transport layer 6, the light emitting layer 7, the electron transport layer 8, and the third electrode 9 on the horizontal plane completely coincide, and areas of the projection surfaces of the hole transport layer 6, the light emitting layer 7, the electron transport layer 8, and the third electrode 9 on the horizontal plane are smaller than areas of the projection surfaces of the carrier generation layer 5 on the horizontal plane.
When the first intermediate layer 3 is a carrier control layer and the second intermediate layer 4 is a second electrode, the substrate 0, the first electrode 1, the dielectric layer 2 and the projection plane of the carrier control layer on the horizontal plane completely coincide with each other, the second electrode and the carrier generation layer 5 are arranged side by side on the carrier control layer, a preset distance is arranged between the second electrode and the carrier generation layer 5, the projection planes of the hole transport layer 6, the light emitting layer 7, the electron transport layer 8 and the third electrode 9 on the horizontal plane completely coincide with each other, and the areas of the projection planes of the hole transport layer 6, the light emitting layer 7, the electron transport layer 8 and the third electrode 9 on the horizontal plane are smaller than the area of the projection plane of the carrier generation layer 5 on the horizontal plane. The first electrode 1 and the dielectric layer 2 are used for biasing the device to enable photon-generated carriers to be enriched in the carrier regulation layer and the carrier generation layer 5, the carrier regulation layer can prevent exciton annihilation effect caused by direct contact of the second electrode 4 and the carrier generation layer 5, electric injection holes can be blocked from being injected from the second electrode and can generate photon-generated holes to be injected into the light emitting layer, a window between the second electrode and the third electrode is favorable for absorption of long-wavelength infrared light, and scattering and absorption of infrared light by the electrode of the vertical structure device are avoided.
In a specific implementation manner, the position order of the carrier control layer and the second electrode may be switched, that is, the first intermediate layer 3 is the second electrode, the second intermediate layer 4 is the carrier control layer, and the up-conversion device includes: the organic electroluminescent device comprises a substrate 0, a first electrode 1, a dielectric layer 2, a second electrode, a carrier regulation layer and a carrier generation layer 5, wherein the substrate 0, the first electrode 1, the dielectric layer 2 and the second electrode are sequentially arranged from bottom to top, and the hole transport layer 6, a light emitting layer 7, an electron transport layer 8 and a third electrode 9 are sequentially arranged on the carrier generation layer 5 from bottom to top. The working principle of the up-conversion device under the condition is similar to that of the former condition, the carrier regulation layer and the carrier generation layer 5 generate photon-generated carriers after absorbing infrared light, the carriers generate the phenomena of carrier enrichment and amplification under the induction of an electric field through the combined action of the first electrode 1 and the dielectric layer 2, are injected into the light-emitting layer 7 under the action of bias voltage, are compounded with the carriers injected by the third electrode 9, and emit visible light, so that the up-conversion process from the infrared light to the visible light is realized. The up-conversion device provided by the embodiment can also realize the conversion of infrared light to visible light, and has the advantages of high conversion efficiency, low lighting voltage and wide detection bandwidth.
When the positions of the current carrier regulation layer and the second electrode are sequentially changed, the projection surfaces of the substrate 0, the first electrode 1, the dielectric layer 2 and the second electrode on the horizontal plane are completely overlapped, the current carrier regulation layer and the current carrier generation layer 5 are arranged on the second electrode side by side, a preset distance is arranged between the current carrier regulation layer and the current carrier generation layer 5 at intervals, the projection surfaces of the hole transmission layer 6, the light emitting layer 7, the electron transmission layer 8 and the third electrode 9 on the horizontal plane are completely overlapped, and the area of the projection surfaces of the hole transmission layer 6, the light emitting layer 7, the electron transmission layer 8 and the third electrode 9 on the horizontal plane is smaller than the area of the projection surface of the current carrier generation layer 5 on the horizontal plane. The first electrode 1 and the dielectric layer 2 are used for biasing the device to enable photogenerated carriers to be enriched in the carrier regulation layer and the carrier generation layer 5, the carrier regulation layer is arranged to prevent electric injection holes from being injected from the second electrode and can also generate photogenerated holes to be injected into the light emitting layer 7, a window between the second electrode and the third electrode 9 is beneficial to absorption of long-wavelength infrared light, and scattering and absorption of infrared light by the electrode of the vertical structure device are avoided.
In a specific implementation manner, the carrier control layer and the carrier generation layer 5 may both absorb infrared light and generate a photon-generated carrier, and the carrier control layer and the carrier generation layer 5 are two semiconductor materials with different conduction types. For example, the carrier control layer is an N-type semiconductor, the carrier generation layer 5 is a P-type semiconductor, and the carrier control layer can block holes injected from the second electrode on the one hand, and can absorb infrared light to generate photo-generated holes on the other hand, and the photo-generated holes generated in the P-type carrier generation layer are transported to the light emitting layer 7 together.
In a specific implementation, the carrier control layer and the carrier generationThe layer 5 is at least one of silicon, silicon carbide, gallium antimonide, gallium arsenide, indium gallium arsenide, lead sulfide, lead selenide, silver sulfide, vanadium oxide, carbon nanotube, carbon quantum dot, black scale, graphene and graphene oxide. For example, the carrier control layer is PbS quantum dots, the carrier generation layer 5 is PbSe quantum dots, or the carrier control layer is carbon nanotubes, the carrier generation layer 5 is Ag2S quantum dot or the carrier regulation layer is Ag2Se quantum dots, and the carrier generation layer 5 is black scale and the like.
In a specific implementation manner, the first electrode 1, the second electrode, and the third electrode 9 are respectively one of metal, a transparent conductive film, and heavily doped silicon. The transparent conductive film is at least one of an indium tin oxide semiconductor transparent conductive film, an aluminum-doped zinc oxide transparent conductive film, a silver nanowire, a carbon nanotube, graphene or a metal grid, and the metal is at least one of barium, calcium, aluminum, magnesium, tin, copper, silver, gold and platinum. For example, the first electrode 1 is an ITO transparent conductive electrode, the second electrode is a silver nanowire, and the third electrode 9 is an ITO transparent conductive electrode.
In a specific implementation manner, the dielectric layer 2 is at least one of silicon dioxide, silicon nitride, polyvinylpyrrolidone, polymethyl methacrylate and poly (vinylidene fluoride-trifluoroethylene), and the hole transport layer 6 is at least one of Polyvinylcarbazole (PVK) and poly (9, 9-dioctylfluorene-CO-N- (4-butylphenyl) diphenylamine).
In a specific implementation, the light emitting layer 7 is at least one of quantum dots, perovskites, organic polymers, and organic small molecules. For example, the light-emitting layer 7 is a CdSe/ZnS quantum dot, a CdZnSeS/ZnS quantum dot, or the like.
In a specific implementation, the electron transport layer 8 is at least one of zinc oxide, magnesium zinc oxide, indium tin oxide, titanium niobium oxide, tin oxide, and tin oxyfluoride. For example, the electron transport layer 8 is ZnO nanoparticles, ZnSnO2Nanoparticles, and the like.
In a specific implementation manner, the device may further include other functional layers, for example, the device further includes a hole injection layer and an electron injection layer, the electron injection layer is disposed between the carrier generation layer 5 and the hole transport layer 6, and the electron injection layer is disposed between the electron transport layer 8 and the third electrode 9. The hole injection layer is at least one of poly (3, 4-ethylenedioxythiophene) -polystyrene sulfonic acid, nickel oxide, molybdenum oxide, tin oxide, magnesium oxide, nickel magnesium oxide and nickel tin oxide, and the electron injection layer is at least one of 8-hydroxyquinoline-lithium, lithium fluoride and aluminum oxide.
In a specific implementation manner, the preparation method of each layer, i.e. the base, 0 in the up-conversion device, the first electrode 1, the dielectric layer 2, the carrier control layer, the second electrode, the carrier generation layer 5, the hole transport layer 6, the luminescent layer 7, the electron transport layer 8 and the third electrode 9 includes at least one of a solution spin coating method, a vacuum thermal evaporation coating method, a vacuum electron beam thermal evaporation method, a magnetron sputtering method, a plasma enhanced chemical vapor deposition method, a pulsed laser epitaxial deposition method and an atomic layer epitaxial deposition method.
Based on the above up-conversion device, an embodiment of the present invention provides a method for manufacturing an up-conversion device, including:
s1, preprocessing the first electrode deposited on the substrate, and forming a dielectric layer on the preprocessed first electrode;
s2, forming a first intermediate layer on the dielectric layer;
s3, forming a second intermediate layer and a carrier generation layer on the first intermediate layer; the first intermediate layer and the second intermediate layer are respectively a carrier regulation layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulation layer;
and S4, sequentially forming a hole transport layer, a light emitting layer, an electron transport layer and a third electrode on the carrier generation layer.
Specifically, the first electrode deposited on the substrate can be an ITO substrate with an electrode pattern, an ITO sheet with a sheet resistance of 15 Ω/sq, an ITO sheet with a sheet resistance of 20 Ω/sq, or the like, and before a dielectric layer is formed on the first electrode, the first electrode is pretreated, wherein the pretreatment method comprises the steps of sequentially carrying out ultrasonic cleaning by using one or more reagents selected from a detergent, deionized water, acetone and isopropanol, and carrying out ultraviolet ozone treatment or plasma treatment after drying to obtain the pretreated first electrode.
After the pretreated first electrode is obtained, forming a dielectric layer on the pretreated first electrode, then forming a first intermediate layer on the dielectric layer, then forming a second intermediate layer and a current carrier generation layer on the first intermediate layer, and finally sequentially forming a hole transmission layer, a light emitting layer, an electron transmission layer and a third electrode on the current carrier generation layer, thereby obtaining the up-conversion device; the first intermediate layer and the second intermediate layer are respectively a carrier control layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier control layer. The forming method of each layer comprises at least one of a solution spin coating method, a vacuum thermal evaporation coating method, a vacuum electron beam thermal evaporation method, a magnetron sputtering method, a plasma enhanced chemical vapor deposition method, a pulse laser epitaxial deposition method and an atomic layer epitaxial deposition method, and the obtained up-conversion device can realize the conversion of infrared light to visible light and has the advantages of high conversion efficiency, low starting voltage and wide detection bandwidth.
The invention is further illustrated by the following specific examples.
Example 1:
(1) and (3) sequentially carrying out ultrasonic treatment on the ITO substrate with the electrode pattern for 8 minutes by using acetone, isopropyl acetone and deionized water, and taking out and drying for later use. Carrying out ultraviolet ozone treatment on the dried ITO substrate for 10 minutes, and then sequentially carrying out spin coating on PVP and PbS quantum dots on an electrode pattern of the ITO substrate, so as to sequentially form a dielectric layer and a carrier regulation and control layer on the ITO substrate with the electrode pattern, wherein the spin coating of the PVP and PbS quantum dots is carried out in a glove box filled with nitrogen, the concentration of PVP is 100mg/ml, after the spin coating of PVP is finished, the ITO substrate spin-coated with PVP is baked in a baking oven at 100 ℃ for 10 minutes, the concentration of PbS quantum dots is 50mg/ml, the rotating speed of the PbS quantum dots during spin coating is 1500r/min, the spin coating time of PbS quantum dots is 30s, and after the spin coating of PbS quantum dots is finished, the ITO substrate spin-coated with PbS quantum dots is baked in a baking oven at 90 ℃ for 10 minutes;
(2) and depositing a 70nm ITO transparent conductive electrode on the PbS quantum dots by adopting a magnetron sputtering vacuum coating method, and then forming a second electrode pattern by adopting negative photoresist photoetching to obtain a second electrode layer deposited on the current carrier regulation layer. Meanwhile, a PbSe quantum dot layer is spin-coated on the PbS quantum dots to obtain a carrier generation layer deposited on the carrier regulation layer, wherein the concentration of the PbSe quantum dots is 550mg/mL, 5 layers are spin-coated repeatedly, and the PbSe quantum dot layer is cleaned by using methanol after each spin-coating;
(3) spin-coating PVK (9 mg/mL in chlorobenzene), CdSe/ZnS quantum dots (10 mg/mL in n-hexane) and ZnO nanoparticles on the PbSe quantum dot layer in sequence to obtain a hole transport layer, a light emitting layer and an electron transport layer which are arranged on the carrier generation layer in sequence from bottom to top, wherein the spin-coating process is carried out in a glove box filled with nitrogen, the rotation speed during spin-coating the PVK is 3500r/min, baking is carried out at 90 ℃ for 30min after the spin-coating is finished, the rotation speed during spin-coating the CdSe/ZnS quantum dots is 2500r/min, baking is carried out at 90 ℃ for 10min after the spin-coating is finished, the rotation speed during spin-coating the ZnO nanoparticles is 2000r/min, and baking is carried out at 90 ℃ for 10min after the spin-coating is finished;
(4) transferring the ITO substrate spin-coated with the ZnO nanoparticles into high-vacuum magnetron sputtering equipment, depositing 70nm of ITO transparent conductive electrodes on the ZnO nanoparticles through magnetron sputtering, and patterning the ITO transparent conductive electrodes in a negative photoresist photoetching mode to obtain the up-conversion device.
Example 2:
(1) sequentially subjecting an ITO sheet with sheet resistance of 15 omega/sq to ultrasonic treatment for 15min by using deionized water, acetone and isopropyl ketone respectively, drying in a vacuum drying oven, carrying out plasma treatment on the dried ITO substrate for 1min, and depositing 200nm SiO on the ITO substrate by adopting PECVD2Then, spinning 100nm silver nanowires, and forming a second electrode pattern on the silver nanowires by adopting plasma etching, thereby sequentially forming a dielectric layer and a second electrode on the ITO substrate;
(2) spin coating of carbon nanotubes on silver nanowires, whichAnd the concentration of the carbon nano tube is 70mg/mL, the rotating speed during spin coating is 2000r/min, the spin coating time is 30s, and the carbon nano tube is baked for 10min at 100 ℃ after the spin coating is finished, so that the carrier regulation and control layer deposited on the second electrode is obtained. Meanwhile, Ag is spin-coated on the silver nanowire2Repeatedly spin-coating 5S quantum dot layers on Ag layer with methanol2Cleaning the S quantum dot layer to obtain a carrier generation layer deposited on the second electrode;
(3) in Ag2Sequentially spin-coating TFB (in chlorobenzene, 10mg/mL), CdSe/ZnS quantum dots (in n-hexane, 10mg/mL) and ZnO nanoparticles on the S quantum dot layer to obtain a hole transport layer, a light emitting layer and an electron transport layer which are sequentially arranged on the carrier generation layer from bottom to top, wherein the spin-coating process is carried out in a glove box filled with nitrogen, the rotating speed of the spin-coating TFB is 3000r/min, the baking is carried out at 90 ℃ for 15min after the spin-coating is finished, the rotating speed of the spin-coating CdSe/ZnS quantum dots is 2500r/min, the baking is carried out at 90 ℃ for 10min after the spin-coating is finished, the rotating speed of the spin-coating ZnO nanoparticles is 2000r/min, and the baking is carried out at 90 ℃ for 10min after the spin-coating is finished;
(4) transferring the ITO substrate spin-coated with the ZnO nanoparticles into high-vacuum magnetron sputtering equipment, depositing 70nm of ITO transparent conductive electrodes on the ZnO nanoparticles through magnetron sputtering, and patterning the ITO transparent conductive electrodes in a negative photoresist photoetching mode to obtain the up-conversion device.
Example 3:
(1) sequentially carrying out ultrasonic cleaning on an ITO sheet with the sheet resistance of 20 omega/sq in a detergent, deionized water, acetone and isopropyl acetone, blow-drying by nitrogen, treating for 15min by using ultraviolet ozone, and depositing and sequentially spin-coating PMMA and Ag on an ITO substrate2Se, thereby sequentially forming a dielectric layer and a carrier regulation and control layer on the ITO substrate, wherein the concentration of PMMA is 60mg/mL, the rotating speed when PMMA is coated in a spinning mode is 3000r/min, the time for coating PMMA is 45s, after the PMMA is coated in a spinning mode, the ITO substrate is baked for 20min at the temperature of 100 ℃, and Ag is formed2Se concentration is 60mg/mL, Ag is spin-coated2The rotation speed of Se is 3000r/min, Ag is coated by spin coating2Se time is 45s, Ag is coated by spin coating2Baking at 100 deg.C for 10min after Se is finished;
(2) by thermal vacuum coating method on Ag2And depositing a 100nm metal aluminum layer on Se, and patterning the metal aluminum layer through a mask plate to obtain a second electrode layer deposited on the carrier regulation layer. Simultaneously, chemical vapor deposition is adopted to deposit on Ag2And depositing black phosphorus with the thickness of 200nm on Se to obtain a carrier generation layer deposited on the carrier regulation layer.
(3) Spin-coating TFB (9 mg/mL in chlorobenzene), CdZnSeS/ZnS quantum dots (12 mg/mL in n-hexane) and ZnSnO on black phosphorus in sequence2The method comprises the following steps of (1) obtaining nanoparticles to obtain a hole transport layer, a light emitting layer and an electron transport layer which are sequentially arranged on a carrier generation layer from bottom to top, wherein the spin coating process is carried out in a glove box filled with nitrogen, the rotating speed of TFB is 3500r/min, baking is carried out at 90 ℃ for 30min after the spin coating is finished, the rotating speed of CdSe/ZnS quantum dots is 2500r/min, baking is carried out at 90 ℃ for 10min after the spin coating is finished, the rotating speed of ZnO nanoparticles is 2000r/min, and baking is carried out at 90 ℃ for 10min after the spin coating is finished;
(4) in ZnSnO2And spin-coating 100nm silver nanowires on the nanoparticles, and forming a third electrode pattern by photoetching to obtain the up-conversion device.
In summary, the present invention discloses an up-conversion device and a method for manufacturing the same, including: the light-emitting diode comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generation layer, a hole transport layer, a light-emitting layer, an electron transport layer and a third electrode, wherein the substrate, the first electrode, the dielectric layer and the first intermediate layer are sequentially arranged from bottom to top; the first intermediate layer and the second intermediate layer are respectively a carrier control layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier control layer. The up-conversion device provided by the embodiment of the invention is a three-terminal non-vertical structure device, can enrich photo-generated carriers, improve the light-light conversion efficiency and reduce the starting voltage of the device, the carrier regulation and control layer can be used as a buffer layer to reduce exciton annihilation in a carrier generation layer, and can also prevent the electrically injected carriers from being injected into a light emitting layer and generating the photo-generated carriers, so that the device is kept in a closed state in a dark state, the transport efficiency and the light-light conversion efficiency of the photo-generated carriers are improved, a window between a second electrode and a third electrode in a three-terminal electrode structure is favorable for absorbing long-wavelength infrared light, and the scattering and absorption of the electrode of the vertical structure device to the infrared light are avoided.
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 (13)
1. An up-conversion device, comprising: the light-emitting diode comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generation layer, a hole transport layer, a light-emitting layer, an electron transport layer and a third electrode, wherein the substrate, the first electrode, the dielectric layer and the first intermediate layer are sequentially arranged from bottom to top; the first intermediate layer and the second intermediate layer are respectively a carrier control layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier control layer.
2. The up-conversion device of claim 1, further comprising: a hole injection layer disposed between the carrier generation layer and the hole transport layer, and an electron injection layer disposed between the electron transport layer and the third electrode.
3. The up-conversion device of claim 1, wherein the first, second, and third electrodes are each one of a metal, a transparent conductive film, and heavily doped silicon.
4. The up-conversion device of claim 3, wherein the transparent conductive film is at least one of an indium tin oxide semiconductor transparent conductive film, an aluminum doped zinc oxide transparent conductive film, silver nanowires, carbon nanotubes, graphene, or a metal mesh.
5. The up-conversion device of claim 4, wherein the metal is at least one of barium, calcium, aluminum, magnesium, tin, copper, silver, gold, and platinum.
6. The up-conversion device of claim 1, wherein the carrier-conditioning layer and the carrier transport layer are each at least one of silicon, silicon carbide, gallium antimonide, gallium arsenide, indium gallium arsenide, lead sulfide, lead selenide, silver sulfide, vanadium oxide, carbon nanotubes, carbon quantum dots, black scale, graphene, and graphene oxide.
7. The up-conversion device of claim 1, wherein the dielectric layer is at least one of silicon dioxide, silicon nitride, polyvinylpyrrolidone, polymethylmethacrylate, and poly (vinylidene fluoride-trifluoroethylene).
8. The up-conversion device of claim 1, wherein the light emitting layer is at least one of a quantum dot, a perovskite, an organic polymer, and a small organic molecule.
9. The up-conversion device of claim 1, wherein the electron transport layer is at least one of zinc oxide, magnesium zinc oxide, indium tin oxide, titanium niobium oxide, tin oxide, and tin oxyfluoride.
10. The up-conversion device of claim 2, wherein the hole injection layer is at least one of poly (3, 4-ethylenedioxythiophene) -polystyrene sulfonic acid, nickel oxide, molybdenum oxide, tin oxide, magnesium oxide, nickel magnesium oxide, and nickel tin oxide.
11. The up-conversion device of claim 2, wherein the electron injection layer is at least one of 8-hydroxyquinoline-lithium, lithium fluoride, and aluminum oxide.
12. The up-conversion device of claim 1, wherein the layers of the up-conversion device are formed by a process comprising at least one of solution spin coating, vacuum thermal evaporation coating, vacuum electron beam thermal evaporation, magnetron sputtering, plasma enhanced chemical vapor deposition, pulsed laser epitaxial deposition, and atomic layer epitaxial deposition.
13. A method of manufacturing an up-conversion device as claimed in claim 1, comprising:
pretreating the first electrode deposited on the substrate, and forming a dielectric layer on the pretreated first electrode;
forming a first intermediate layer on the dielectric layer;
forming a second intermediate layer and a carrier generation layer on the first intermediate layer; the first intermediate layer and the second intermediate layer are respectively a carrier regulation layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulation layer;
and sequentially forming a hole transport layer, a light emitting layer, an electron transport layer and a third electrode on the carrier generation layer.
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