CN113809252B - Up-conversion device and manufacturing method thereof - Google Patents
Up-conversion device and manufacturing method thereof Download PDFInfo
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- CN113809252B CN113809252B CN202110893394.8A CN202110893394A CN113809252B CN 113809252 B CN113809252 B CN 113809252B CN 202110893394 A CN202110893394 A CN 202110893394A CN 113809252 B CN113809252 B CN 113809252B
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Classifications
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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
-
- 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
-
- 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
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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- Physics & Mathematics (AREA)
- Optics & Photonics (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Crystallography & Structural Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Nanotechnology (AREA)
- Led Devices (AREA)
Abstract
The invention discloses an up-conversion device and a manufacturing method thereof, comprising the following steps: the light-emitting diode comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generating layer, a hole transporting layer, a light-emitting layer, an electron transporting 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 regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer. The up-conversion device is of a three-terminal non-vertical structure, can enrich photo-generated carriers, improves the photo-conversion efficiency, reduces the starting voltage of the device, enables the device to be kept in a closed state in a dark state by the carrier regulating layer, improves the transportation efficiency of the photo-generated carriers, facilitates the absorption of long-wavelength infrared light by a window between the second electrode and the third electrode, and avoids the scattering and absorption of infrared light by the electrodes of the vertical structure device.
Description
Technical Field
The invention relates to the technical field of photoelectrons, 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 the infrared light extends from 760nm to 1mm, and the infrared technology has wide application in the aspects of night vision devices, area detection, national defense safety, semiconductor wafer detection and the like. However, conventional CCD and CMOS sensing devices cannot detect infrared bands greater than 1 μm, and in the industrial process, the existing infrared imaging device is formed by connecting an infrared detector with a silicon-based readout circuit based on an indium bonding technology, which is a one-at-a-time process, many factors of which limit its yield and size expansibility. In addition, in order to manufacture a larger-sized pixel array, the size of each pixel must be reduced, which puts stringent process requirements on the device.
Based on the drawbacks of conventional infrared imaging devices, light up-conversion devices are proposed that can up-convert low-energy incident radiation of photons into high-energy output radiation. The infrared up-conversion light-emitting 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 emission capability, infrared light is absorbed by the PD unit, photocurrent is generated and directly injected into the LED, and the LED is driven to generate visible light. However, the existing infrared up-conversion luminescent device has the problems of low light-light conversion efficiency, overlarge starting voltage, overlarge infrared detection wavelength and the like.
Accordingly, there is a need for improvement and development in the art.
Disclosure of Invention
The invention aims to solve the technical problems of low light-light conversion efficiency, overlarge starting voltage and overlarge infrared detection wavelength of the traditional infrared up-conversion luminescent 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 device comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generating layer, a hole transporting layer, a light emitting layer, an electron transporting 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 regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer.
The up-conversion device, wherein the up-conversion device further comprises: and 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, transparent conductive film and heavily doped silicon.
The up-conversion device is characterized in that 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 is characterized in that 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 regulating 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 nanotubes, carbon quantum dots, black scales, graphene and graphene oxide.
The up-conversion device is characterized in that the dielectric layer is at least one of silicon dioxide, silicon nitride, polyvinylpyrrolidone, polymethyl methacrylate and poly (vinylidene fluoride-trifluoroethylene).
The up-conversion device is characterized in that the light-emitting layer is at least one of quantum dots, perovskite, organic polymers and organic small molecules.
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.
The up-conversion device is characterized in that 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 preparation method of each layer in the up-conversion device 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 the up-conversion device, including:
pretreating a first electrode deposited on a 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 generating layer on the first intermediate layer; the first intermediate layer and the second intermediate layer are respectively a carrier regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer;
and forming a hole transport layer, a light emitting layer, an electron transport layer and a third electrode on the carrier generating layer in sequence.
The beneficial effects are that: the up-conversion device provided by the embodiment of the invention is a three-terminal non-vertical structure device, can enrich photogenerated carriers, improves the photo-photo conversion efficiency, reduces the starting voltage of the device, can be used as a buffer layer to reduce exciton annihilation in a carrier generation layer, can block electric injection carriers from being injected into a light-emitting layer and generate photogenerated carriers, so that the device keeps a closed state in a dark state, improves the transportation efficiency and the photo-photo conversion efficiency of the photogenerated carriers, and a window between a second electrode and a third electrode in a three-terminal electrode structure is favorable for absorbing long-wavelength infrared light, thereby avoiding scattering and absorption of infrared light by electrodes of the vertical structure device.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings that are required to be used in the embodiments or the description of the prior art will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments described in the present invention, and other drawings may be obtained according to the drawings without inventive effort to those skilled in the art.
Fig. 1 is a schematic structural diagram of an up-conversion device according to an embodiment of the present invention;
FIG. 2 is a schematic diagram of the operation of the up-conversion device according to the embodiment of the present invention when not irradiated by infrared light;
fig. 3 is a schematic diagram of the operation of the up-conversion device according to the embodiment of the present invention when irradiated by infrared light.
The marks in the drawings are as follows: 0. a substrate; 1. a first electrode; 2. a dielectric layer; 3. a first intermediate layer; 4. a second intermediate layer; 5. a carrier generating 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 more clear and clear, the present invention will be further described in detail below with reference to the accompanying drawings and examples. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the scope of the invention.
It should be noted that, if directional indications (such as up, down, left, right, front, and rear … …) are included in the embodiments of the present invention, the directional indications are merely used to explain the relative positional relationship, movement conditions, etc. between the components in a specific posture (as shown in the drawings), and if the specific posture is changed, the directional indications are correspondingly changed.
Infrared light is an electromagnetic wave between visible light waves and microwaves, the wavelength range of the infrared light extends from 760nm to 1mm, and the infrared technology has wide application in the aspects of night vision devices, area detection, national defense safety, semiconductor wafer detection and the like. However, common CCD and CMOS sensing devices cannot detect infrared bands greater than 1 μm, and in the industrialization process, the existing infrared imaging devices are formed by connecting an infrared detector with a silicon-based readout circuit based on an indium bonding technology, which is currently becoming an industry standard program. In this system structure, each pixel point of the silicon-based readout integrated circuit is connected to the infrared detection unit in a one-to-one correspondence manner, and the indium bonding technology is a one-at-a-time process, and many factors limit the yield and the size expansibility of the silicon-based readout integrated circuit. In addition, in order to manufacture a larger-sized pixel array, the size of each pixel must be reduced, which places stringent process requirements on the device.
Based on the drawbacks of conventional infrared imaging devices, light up-conversion devices are proposed that can up-convert low-energy incident radiation of photons into high-energy output radiation. Optical up-conversion devices mainly have two up-conversion mechanisms, a nonlinear optical process and a linear optical process, the nonlinear up-conversion optical process needs to have two or more metastable energy states to store the absorbed pump photon energy, and the energy accumulation of the pump photon can lead to photon emission with higher energy, but the nonlinear up-conversion mechanism is generally low in efficiency and is not suitable for being applied to the specific infrared imaging field. The infrared up-conversion light-emitting 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 emission capability, infrared light is absorbed by the PD unit, photocurrent is generated and directly injected into the LED, and the LED is driven to generate visible light. This structure requires the infrared light detector to have a high light response, while the LED is required to have a low turn-on voltage and high luminous efficiency. The up-conversion light emitting device developed in the prior art has the following main problems: (1) The up-conversion luminescence integrated by PD and LED back-to-back reverse series connection has natural carrier potential barrier and larger series resistance in the device, and the carrier potential barrier is further increased by a barrier layer introduced for setting an optical switch; the interaction and the recombination mechanism between the photo-generated carriers and the electric injection carriers are not clear, which leads to the difficulty in obtaining devices with high conversion efficiency and low starting voltage at present; (2) At present, a transparent electrode in a 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 a middle-far infrared band is very low, and the detection of the device on long-wavelength infrared light is seriously influenced; (3) It is difficult to balance the relationship between conversion efficiency and the on-luminance voltage, resulting in an excessive on-luminance voltage of the device.
In order to solve the problems in the prior art, the present invention provides an up-conversion device, as shown in fig. 1, where the up-conversion device provided in the embodiment of the present invention includes: 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; wherein the first intermediate layer 3 and the second intermediate layer 4 are a carrier regulating 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 regulating layer, respectively. The up-conversion device provided by the embodiment of the invention is a three-terminal non-vertical structure device, can enrich photogenerated carriers, improves the photo-photo conversion efficiency, reduces the starting voltage of the device, can be used as a buffer layer to reduce exciton annihilation in a carrier generation layer, can block electric injection carriers from being injected into a light-emitting layer and generate photogenerated carriers, so that the device keeps a closed state in a dark state, improves the transportation efficiency and the photo-photo conversion efficiency of the photogenerated carriers, and a window between a second electrode and a third electrode in a three-terminal electrode structure is favorable for absorbing long-wavelength infrared light, thereby avoiding scattering and absorption of infrared light by electrodes of the vertical structure device.
Specifically, the up-conversion device provided by the embodiment of the invention can realize conversion from 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, the first power supply is used for applying grid bias voltage, so that the first electrode 1 and the dielectric layer 2 form a capacitor-like structure and are used for enriching photo-generated carriers; the second power supply is connected between the second electrode and the third electrode 9 to generate an electric field effect, so that photo-generated carriers enriched in the carrier regulating layer and the carrier generating layer are driven to be injected into the light emitting layer 7, and the photo-generated carriers and the carriers injected by the third electrode 9 are combined to emit light, so that the conversion from infrared light to visible light can be realized.
As shown in fig. 2 and fig. 3, which are schematic diagrams illustrating the operation of the up-conversion device according to the embodiment of the present invention, holes are induced by the first electrode 1 through the dielectric layer 2 without irradiation of infrared light, and the holes concentrated in the second electrode are difficult to inject into the light emitting layer 7 due to the blocking of the carrier regulating layer, so that the device does not emit light. Under the irradiation of infrared light, the carrier regulating and controlling and carrier generating layer 5 can absorb infrared light to generate photo-generated electrons and holes, the carriers generate the enrichment and amplification phenomena of the carriers in the layer under the induction of an electric field under the combined action of the first electrode 1 and the dielectric layer 2, the carriers are injected into the light emitting layer 7 under the action of bias voltage, and are combined with the carriers injected by the third electrode 9 to emit visible light, so that the up-conversion process from infrared light to visible light is realized. The up-conversion device provided by the embodiment can realize conversion from infrared light to visible light, and has the advantages of high conversion efficiency, low starting voltage and wide detection bandwidth.
In a specific implementation manner, the projection surfaces of the substrate 0, the first electrode 1, the dielectric layer 2 and the first intermediate layer 3 on a horizontal plane are completely coincident, the second intermediate layer 4 and the carrier generating layer 5 are arranged on the first intermediate layer 3 side by side, a preset distance is reserved between the second intermediate layer 4 and the carrier generating layer 5, the projection surfaces of the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 on a horizontal plane are completely coincident, and the area of the projection surfaces of the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 on a horizontal plane is smaller than the area of the projection surface of the carrier generating layer 5 on a horizontal plane.
When the first intermediate layer 3 is a carrier regulating layer and the second intermediate layer 4 is a second electrode, the projection surfaces of the substrate 0, the first electrode 1, the dielectric layer 2 and the carrier regulating layer on the horizontal plane are completely overlapped, the second electrode and the carrier generating layer 5 are arranged on the carrier regulating layer side by side, a preset distance is reserved between the second electrode and the carrier generating layer 5, the projection surfaces of the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 on the horizontal plane are completely overlapped, and the area of the projection surfaces of the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 on the horizontal plane is smaller than the area of the projection surface of the carrier generating layer 5 on the horizontal plane. The first electrode 1 and the dielectric layer 2 are used for biasing the device, so that photo-generated carriers are enriched in the carrier regulating layer and the carrier generating layer 5, and the carrier regulating layer can prevent the second electrode 4 from being in direct contact with the carrier generating layer 5 to generate an exciton annihilation effect, and can prevent electric injection holes from being injected from the second electrode and generate photo-generated holes to be injected into the light emitting layer, and a window between the second electrode and the third electrode is beneficial to absorption of long-wavelength infrared light, so that scattering and absorption of infrared light by the electrodes of the vertical structure device are avoided.
In a specific implementation manner, the position order of the carrier regulating layer and the second electrode may be changed, that is, the first intermediate layer 3 is the second electrode, the second intermediate layer 4 is the carrier regulating layer, and the up-conversion device includes: the light-emitting diode comprises a substrate 0, a first electrode 1, a dielectric layer 2 and a second electrode which are sequentially arranged from bottom to top, a carrier regulating layer and a carrier generating layer 5 which are arranged on the second electrode, 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 generating layer 5 from bottom to top. The working principle of the up-conversion device in this case is similar to that of the former case, the carrier regulating layer and the carrier generating layer 5 generate photo-generated carriers after absorbing infrared light, the carriers generate enrichment and amplification phenomena of the carriers in the layer under the induction of an electric field through the combined action of the first electrode 1 and the dielectric layer 2, the carriers are injected into the light emitting layer 7 under the action of bias voltage, and the carriers injected by the third electrode 9 are combined to emit visible light, so that the up-conversion process from infrared light to visible light is realized. The up-conversion device provided by the embodiment can also realize conversion from infrared light to visible light, and has the advantages of high conversion efficiency, low starting voltage and wide detection bandwidth.
When the positions of the carrier regulating layer and the second electrode are sequentially exchanged, 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 carrier regulating layer and the carrier generating layer 5 are arranged on the second electrode side by side, a preset distance is reserved between the carrier regulating layer and the carrier generating layer 5, the projection surfaces of the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 on the horizontal plane are completely overlapped, and the area of the projection surfaces of the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 on the horizontal plane is smaller than the area of the projection surface of the carrier generating layer 5 on the horizontal plane. The first electrode 1 and the dielectric layer 2 are used for biasing the device, so that photo-generated carriers are enriched in the carrier regulating layer and the carrier generating layer 5, and the carrier regulating layer can block electric injection holes from being injected from the second electrode and generate photo-generated holes to be injected into the light emitting layer 7, so that the window between the second electrode and the third electrode 9 is favorable for absorbing long-wavelength infrared light, and scattering and absorption of infrared light by the electrodes of the vertical structure device are avoided.
In a specific implementation manner, the carrier regulating layer and the carrier generating layer 5 can both absorb infrared light and generate photo-generated carriers, and the carrier regulating layer and the carrier generating layer 5 are made of two semiconductor materials with different conductive types. For example, the carrier regulating layer is an N-type semiconductor, the carrier generating layer 5 is a P-type semiconductor, and the carrier regulating layer can block holes injected from the second electrode on one hand and absorb infrared light to generate photo-generated holes on the other hand, and transport the photo-generated holes together with the photo-generated holes generated in the P-type carrier generating layer to the light emitting layer 7.
In a specific implementation manner, the carrier regulating layer and the carrier generating layer 5 are 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 scales, graphene and graphene oxide, respectively. For example, the carrier regulating layer is a PbS quantum dot, the carrier generating layer 5 is a PbSe quantum dot, or the carrier regulating layer is a carbon nanotube, and the carrier generating layer 5 is Ag 2 S quantum dots or Ag as the carrier regulating layer 2 And Se quantum dots, wherein the carrier generation layer 5 is black scales 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, 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 manner, the light emitting layer 7 is at least one of quantum dots, perovskite, organic polymers and small organic molecules. For example, the light emitting layer 7 is CdSe/ZnS quantum dot, 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, znSnO 2 Nanoparticles, and the like.
In a specific implementation manner, other functional layers may be added to the device, for example, the device further includes a hole injection layer and an electron injection layer, where 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 methods of each layer, namely the base, 0, the first electrode 1, the dielectric layer 2, the carrier regulating layer, the second electrode, the carrier generating layer 5, the hole transporting layer 6, the light emitting layer 7, the electron transporting layer 8 and the third electrode 9 in the up-conversion device include 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.
Based on the up-conversion device, an embodiment of the present invention provides a method for manufacturing an up-conversion device, including:
s1, preprocessing a first electrode deposited on a 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 generating layer on the first intermediate layer; the first intermediate layer and the second intermediate layer are respectively a carrier regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer;
and S4, sequentially forming a hole transmission layer, a light emitting layer, an electron transmission layer and a third electrode on the carrier generation layer.
Specifically, the first electrode deposited on the substrate can be selected from an ITO substrate with a charge pattern, an ITO sheet with a sheet resistance of 15 Ω/sq, an ITO sheet with a sheet resistance of 20 Ω/sq, and the like, and the first electrode is pretreated before a dielectric layer is formed on the first electrode.
After the pretreated first electrode is obtained, a dielectric layer is formed on the pretreated first electrode, a first intermediate layer is formed on the dielectric layer, a second intermediate layer and a carrier generating layer are formed on the first intermediate layer, and finally a hole transport layer, a light emitting layer, an electron transport layer and a third electrode are sequentially formed on the carrier generating layer, so that an up-conversion device is obtained; the first intermediate layer and the second intermediate layer are respectively a carrier regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer. The formation 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 conversion from 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 examples.
Example 1:
(1) And sequentially carrying out ultrasonic treatment on the ITO substrate with the electrode pattern by using acetone, isopropyl alcohol and deionized water for 8 minutes, and taking out and drying for later use. Carrying out ultraviolet ozone treatment on the dried ITO substrate for 10 minutes, sequentially spin-coating PVP and PbS quantum dots on an electrode pattern of the ITO substrate, and sequentially forming a dielectric layer and a carrier regulating layer on the ITO substrate with the electrode pattern, wherein spin-coating of PVP and PbS quantum dots is carried out in a glove box filled with nitrogen, PVP concentration is 100mg/ml, the ITO substrate spin-coated with PVP is baked for 10 minutes in a baking oven at 100 ℃, the concentration of PbS quantum dots is 50mg/ml, the rotating speed of the PbS quantum dots is 1500r/min, the spin-coating time of the PbS quantum dots is 30s, and the ITO substrate spin-coated with the PbS quantum dots is baked for 10 minutes in the baking oven at 90 ℃ after the spin-coating of the PbS quantum dots is finished;
(2) And depositing an ITO transparent conductive electrode with the thickness of 70nm on the PbS quantum dot 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 carrier regulating layer. Simultaneously, spin-coating a PbSe quantum dot layer on the PbS quantum dot to obtain a carrier generation layer deposited on the carrier regulation layer, wherein the concentration of the PbSe quantum dot is 550mg/mL, repeatedly spin-coating 5 layers, and cleaning the PbSe quantum dot layer by using methanol after each spin-coating is finished;
(3) Sequentially spin-coating PVK (in chlorobenzene, 9 mg/mL), cdSe/ZnS quantum dots (in n-hexane, 10 mg/mL) and ZnO nanoparticles on a PbSe quantum dot layer to obtain a hole transmission layer, a luminescent layer and an electron transmission 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 rotation speed of the spin-coating PVK is 3500r/min, the spin-coating process is baked at 90 ℃ for 30min, the rotation speed of the spin-coating CdSe/ZnS quantum dots is 2500r/min, the spin-coating process is baked at 90 ℃ for 10min, the rotation speed of the spin-coating ZnO nanoparticles is 2000r/min, and the spin-coating process is baked at 90 ℃ for 10min;
(4) Transferring the ITO substrate coated with the ZnO nano particles into high-vacuum magnetron sputtering equipment, depositing an ITO transparent conductive electrode with the thickness of 70nm on the ZnO nano particles through magnetron sputtering, and then patterning the ITO transparent conductive electrode by adopting a negative photoresist photoetching mode to obtain the up-conversion device.
Example 2:
(1) Sequentially performing ultrasonic treatment on an ITO sheet with a sheet resistance of 15 omega/sq by using deionized water, acetone and isopropyl alcohol for 15min, drying in a vacuum drying oven, performing plasma treatment on the dried ITO substrate for 1min, and depositing 200nm SiO on the ITO substrate by adopting PECVD 2 Then, spin-coating a silver nanowire with a wavelength of 100nm, and forming a second electrode pattern on the silver nanowire by adopting plasma etching, so as to sequentially form a dielectric layer and a second electrode on the ITO substrate;
(2) And spin-coating the carbon nano tube on the silver nano wire, wherein 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 at 100 ℃ for 10min after the spin-coating is finished, so that the carrier regulating layer deposited on the second electrode is obtained. Simultaneously, ag is spin-coated on silver nanowires 2 S quantum dot layer, repeatedly spin coating 5 layers, and using methanol to carry out Ag after each spin coating 2 The S quantum dot layer is cleaned to obtain a carrier generating layer deposited on the second electrode;
(3) In Ag 2 Spin-coating TFB (10 mg/mL in chlorobenzene), cdSe/ZnS quantum dots (10 mg/mL in n-hexane) and ZnO nanoparticles sequentially on the S quantum dot layer to obtain a hole transport layer, a light emitting layer and an electron transport layer sequentially arranged on the carrier generation layer from bottom to top, wherein the spin-coating process is thatThe spin coating is carried out in a glove box filled with nitrogen, the rotating speed is 3000r/min when the spin coating is carried out on TFB, the spin coating is carried out at 90 ℃ for 15min, the rotating speed is 2500r/min when the spin coating is carried out on CdSe/ZnS quantum dots, the spin coating is carried out at 90 ℃ for 10min after the spin coating is carried out, the rotating speed is 2000r/min when the spin coating is carried out on ZnO nano particles, and the spin coating is carried out at 90 ℃ for 10min after the spin coating is carried out;
(4) Transferring the ITO substrate coated with the ZnO nano particles into high-vacuum magnetron sputtering equipment, depositing an ITO transparent conductive electrode with the thickness of 70nm on the ZnO nano particles through magnetron sputtering, and then patterning the ITO transparent conductive electrode by adopting a negative photoresist photoetching mode to obtain the up-conversion device.
Example 3:
(1) Ultrasonically cleaning an ITO sheet with a sheet resistance of 20 omega/sq sequentially by adopting a detergent, deionized water, acetone and isopropyl alcohol, drying by using nitrogen, treating for 15min by using ultraviolet ozone, and depositing and sequentially spin-coating PMMA and Ag on an ITO substrate 2 Se, thereby sequentially forming a dielectric layer and a carrier regulating layer on the ITO substrate, wherein the concentration of PMMA is 60mg/mL, the rotating speed of spin-coating PMMA is 3000r/min, the spin-coating PMMA time is 45s, the spin-coating PMMA is baked for 20min at 100 ℃ after the end, and Ag 2 Se concentration is 60mg/mL, spin coating Ag 2 The rotating speed of Se is 3000r/min, and Ag is coated by spin coating 2 Se time is 45s, spin coating Ag 2 Roasting at 100 ℃ for 10min after Se is over;
(2) Ag by thermal vacuum coating method 2 And 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 regulating layer. Meanwhile, adopting a chemical vapor deposition method to deposit Ag 2 And depositing 200nm black phosphorus on Se to obtain a carrier generating layer deposited on the carrier regulating layer.
(3) Spin-coating TFB (9 mg/mL in chlorobenzene), cdZnSeS/ZnS quantum dots (12 mg/mL in n-hexane) on black phosphorus in this order 2 The nano particles are used for obtaining a hole transmission layer, a light-emitting layer and an electron transmission 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 the spin coating TFB is 3500r/min, the spin coating process is carried out after the spin coating is finished, the baking is carried out at 90 ℃ for 30min, and the spin coating is carried outThe rotating speed of CdSe/ZnS quantum dots is 2500r/min, the ZnO nano particles are baked for 10min at 90 ℃ after spin coating, the rotating speed of ZnO nano particles are 2000r/min, and the ZnO nano particles are baked for 10min at 90 ℃ after spin coating;
(4) In ZnSnO 2 And spin-coating 100nm silver nanowires on the nano particles, 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 manufacturing method thereof, including: the device comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generating layer, a hole transporting layer, a light emitting layer, an electron transporting 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 regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer. The up-conversion device provided by the embodiment of the invention is a three-terminal non-vertical structure device, can enrich photogenerated carriers, improves the photo-photo conversion efficiency, reduces the starting voltage of the device, can be used as a buffer layer to reduce exciton annihilation in a carrier generation layer, can block electric injection carriers from being injected into a light-emitting layer and generate photogenerated carriers, so that the device keeps a closed state in a dark state, improves the transportation efficiency and the photo-photo conversion efficiency of the photogenerated carriers, and a window between a second electrode and a third electrode in a three-terminal electrode structure is favorable for absorbing long-wavelength infrared light, thereby avoiding scattering and absorption of infrared light by electrodes of the vertical structure device.
It is to be understood that the invention is not limited in its application to the examples described above, but is capable of modification and variation in light of the above teachings by those skilled in the art, and that all such modifications and variations are intended to be included within the scope of the appended claims.
Claims (13)
1. An up-conversion device, comprising: the device comprises a substrate, a first electrode, a dielectric layer, a first intermediate layer, a second intermediate layer, a carrier generating layer, a hole transporting layer, a light emitting layer, an electron transporting 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 regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer;
the substrate, the first electrode, the dielectric layer and the projection surface of the first intermediate layer on the horizontal plane are completely overlapped, the second intermediate layer and the carrier generation layer are arranged on the first intermediate layer side by side, a preset distance is reserved between the second intermediate layer and the carrier generation layer, the projection surfaces of the hole transmission layer, the light-emitting layer, the electron transmission layer and the third electrode on the horizontal plane are completely overlapped, and the area of the projection surfaces of the hole transmission layer, the light-emitting layer, the electron transmission layer and the third electrode on the horizontal plane is smaller than the area of the projection surface of the carrier generation layer on the horizontal plane.
2. The up-conversion device of claim 1, wherein the up-conversion device further comprises: and 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 according to claim 1, wherein the first electrode, the second electrode, and the third electrode are each one of a metal, a transparent conductive film, and heavily doped silicon.
4. The up-conversion device according to 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 upconverter 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 according to claim 1, wherein the carrier regulating layer and the carrier generating 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 upconverter device of claim 1, wherein the dielectric layer is at least one of silicon dioxide, silicon nitride, polyvinylpyrrolidone, polymethyl methacrylate, and poly (vinylidene fluoride-trifluoroethylene).
8. The up-conversion device according to claim 1, wherein the light emitting layer is at least one of quantum dots, perovskite, organic polymers, and small organic molecules.
9. The upconverter 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 according to 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 according to 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 according to claim 1, wherein the preparation method of each layer in the up-conversion device 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 pulsed laser epitaxial deposition method, and an atomic layer epitaxial deposition method.
13. A method of manufacturing an up-conversion device according to claim 1, comprising:
pretreating a first electrode deposited on a 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 generating layer on the first intermediate layer; the first intermediate layer and the second intermediate layer are respectively a carrier regulating layer and a second electrode, or the first intermediate layer and the second intermediate layer are respectively a second electrode and a carrier regulating layer;
and forming a hole transport layer, a light emitting layer, an electron transport layer and a third electrode on the carrier generating layer in sequence.
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