CN111697090B - Amorphous Ga2O3Photoelectric detector, manufacturing method thereof and performance improving method - Google Patents
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Images
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
- H01L31/0296—Inorganic materials including, apart from doping material or other impurities, only AIIBVI compounds, e.g. CdS, ZnS, HgCdTe
- H01L31/02963—Inorganic materials including, apart from doping material or other impurities, only AIIBVI compounds, e.g. CdS, ZnS, HgCdTe characterised by the doping material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
- H01L31/1828—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof the active layers comprising only AIIBVI compounds, e.g. CdS, ZnS, CdTe
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
- H01L31/1876—Particular processes or apparatus for batch treatment of the devices
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Condensed Matter Physics & Semiconductors (AREA)
- Electromagnetism (AREA)
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- Microelectronics & Electronic Packaging (AREA)
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- Inorganic Chemistry (AREA)
- Light Receiving Elements (AREA)
Abstract
The invention discloses amorphous Ga2O3Photoelectric detector, preparation method and performance improvement method thereof, and amorphous Ga2O3The photodetector includes: substrate, hydrogen-doped amorphous Ga deposited on surface of substrate2O3A thin film active layer and an amorphous Ga doped with hydrogen2O3An electrode on the thin film active layer; wherein the hydrogen-doped amorphous Ga2O3The film active layer is an amorphous film prepared by a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere; the vacuum deposition method comprises any one of magnetron sputtering, pulsed laser deposition, electron beam deposition and chemical vapor deposition.
Description
Technical Field
The invention relates to the technical field of photoelectric detection, in particular to amorphous Ga2O3A photoelectric detector, a manufacturing method thereof and a performance improving method.
Background
Because the background radiation of the solar blind (200-280 nm) wave band in the atmosphere is close to zero, the solar blind ultraviolet detector working in the wave band has the advantages of low background noise, high sensitivity and the like, so the solar blind ultraviolet detector has very wide application prospects in the fields of space communication, flame monitoring, biomedicine, missile guidance, ozone monitoring and the like; similarly, X-ray detectors are also important in medical inspection, military weapons, space communications, satellite navigation, and other fields. Ga2O3The material has the characteristics of 4.5-5.0 electron voltage wide band gap, low noise current, strong irradiation resistance and the like, so that the material is more and more widely concerned in the solar blind deep ultraviolet detection field and the X-ray detection field.
At present, Ga is involved2O3In the report of the photodetector, high-quality single-crystal-phase Ga is mostly adopted2O3As an active layer. And single crystal phase Ga2O3The preparation needs complex processes of single crystal substrate, high temperature growth, high temperature annealing and the like: for example, high vacuum equipment such as molecular beam epitaxy, pulsed laser deposition, metal organic chemical vapor deposition and the like are used, the doped film grows under a high temperature condition, and high temperature annealing is needed to activate donors, acceptors and the like, so that the film has high preparation cost and large volume and mass, is not beneficial to large-area industrial application, and cannot be integrated with flexible equipment. In contrast to the single-crystal phase, the amorphous phase Ga2O3The film has the advantages of simple preparation process, low cost, low-temperature growth, realization of flexibility and the like, thereby having great market application potential.
However, amorphous Ga grown at room temperature is currently used2O3The defect density in the film is high, which causes large dark current and unstable performance, so that the problems of high energy consumption, low light-dark ratio, poor stability and the like can occur in practical application. To realize the amorphous Ga2O3The organic regulation and control of the defect density in the film has invented a micro-oxygen flow regulation and control method in the industry, which effectively inhibits the oxygen vacancy point defect concentration in the film, reduces the dark current, and respectively increases the light-dark ratio of solar blind ultraviolet and X-ray irradiation to 107And 104Magnitude.
However, we find that although the accurate regulation of the oxygen flow greatly reduces the dark current and greatly improves the response speed, the responsiveness of the device is also greatly reduced, and the actual application effect of the device is seriously affected.
Disclosure of Invention
The invention aims to provide amorphous Ga aiming at the defects of the prior art2O3Photoelectric detector and preparation method thereofAnd a performance enhancing method.
In view of the above, in a first aspect, embodiments of the present invention provide an amorphous Ga2O3A photodetector, comprising:
substrate, hydrogen-doped amorphous Ga deposited on surface of substrate2O3A thin film active layer and an amorphous Ga doped with hydrogen2O3An electrode on the thin film active layer;
wherein the hydrogen-doped amorphous Ga2O3The film active layer is an amorphous film prepared by a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere; the vacuum deposition method comprises any one of magnetron sputtering, pulsed laser deposition, electron beam deposition and chemical vapor deposition.
Preferably, the substrate comprises one or more of mica, polyimide, polyethylene terephthalate, polyethylene naphthalate, polyvinyl chloride, polycarbonate, polystyrene, polyethylene, polypropylene, sapphire, silicon carbide, quartz glass, polymethyl methacrylate, plexiglass or gallium arsenide;
the electrode comprises one or more of Indium Tin Oxide (ITO), Aluminum Zinc Oxide (AZO), Gallium Zinc Oxide (GZO), Fluorine Tin Oxide (FTO), chromium, copper, silver, gold, nickel, titanium gold, aluminum or platinum.
Preferably, the amorphous Ga2O3The structure of the photoelectric detector is one of a metal-semiconductor-metal MSM structure, a PN junction structure, a PIN junction structure or a Schottky diode structure.
In a second aspect, embodiments of the present invention provide an amorphous Ga according to the first aspect2O3A method of making a photodetector comprising:
preprocessing a substrate;
putting the pretreated substrate into a cavity of vacuum deposition equipment, starting a vacuum pump, and preparing the hydrogen-doped amorphous Ga by adopting a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere2O3A thin film active layer;
in the hydrogen-doped amorphous Ga2O3On the thin film active layerAnd preparing an electrode.
Preferably, the pre-treating the substrate specifically includes: and ultrasonically cleaning the substrate by using a chemical reagent and drying the substrate by blowing.
Preferably, the hydrogen-doped amorphous Ga2O3The preparation of the electrode on the thin film active layer specifically comprises the following steps:
by ultraviolet exposure and development and fixation, the hydrogen-doped amorphous Ga is added2O3Photoetching an electrode structure on the thin film active layer;
depositing an electrode medium;
and stripping and removing the photoresist and the electrode medium on the photoresist.
Preferably, after the vacuum pump is started, the method specifically includes:
after the cavity of the vacuum deposition equipment is pumped to the background vacuum, hydrogen-containing gas is introduced in advance, and after the vacuum degree is stable, hydrogen-doped amorphous Ga is carried out in the hydrogen-containing atmosphere2O3And depositing a thin film active layer.
Preferably, the hydrogen-containing gas comprises hydrogen or ammonia; the hydrogen comprises protium, deuterium, tritium.
In a third aspect, embodiments of the present invention provide an amorphous Ga2O3The performance improvement method of the photoelectric detector comprises the following steps:
amorphous Ga prepared in hydrogen-containing atmosphere2O3Amorphous Ga for photodetector2O3Thin film active layer of amorphous Ga2O3Oxygen vacancy defects in the thin film active layer are occupied by hydrogen incorporation and bond with gallium metal dangling bonds.
Amorphous Ga provided by the invention2O3Photodetector by applying amorphous Ga2O3Introducing hydrogen doping during the growth of the thin film active layer so as to carry out amorphous Ga2O3Oxygen vacancy defects in the material are taken up and combined with gallium metal dangling bonds, thereby reducing or eliminating amorphous Ga2O3Defects in the material such that amorphous Ga2O3The photodetector maintains high responsivity, i.e. photocurrent remains unchangedIn the case of (2), the dark current can be effectively inhibited and reduced, so that the photocurrent-dark current ratio (light-dark ratio) is greatly improved and can reach as high as nearly 108。
Drawings
The technical solutions of the embodiments of the present invention are further described in detail with reference to the accompanying drawings and embodiments.
FIG. 1 shows an embodiment of the present invention for reducing or eliminating amorphous Ga by hydrogen doping2O3Schematic diagram of the defect;
FIG. 2 shows amorphous Ga deposited at different hydrogen flow rates according to an embodiment of the present invention2O3An optical transmittance profile of the film;
FIG. 3 shows amorphous Ga deposited at different hydrogen flow rates according to an embodiment of the present invention2O3XRD pattern of the film;
FIG. 4 shows amorphous Ga deposited at different hydrogen flow rates according to an embodiment of the present invention2O3A graph of dark current of a photoelectric detector corresponding to the film under 254nm solar blind ultraviolet illumination along with voltage change;
FIG. 5 shows amorphous Ga deposited at different hydrogen flow rates according to an embodiment of the present invention2O3A graph of photocurrent of a photoelectric detector corresponding to the film under 254nm solar blind ultraviolet illumination along with voltage change;
FIG. 6 shows amorphous Ga deposited under the condition of introducing 0.5sccm hydrogen gas according to an embodiment of the present invention2O3Film and amorphous Ga deposited without introducing hydrogen2O3A curve comparison graph of the change of the photocurrent of the photoelectric detector corresponding to the film along with the time under the irradiation of the X-ray;
FIG. 7 shows amorphous Ga deposited under the condition of a medium hydrogen flow of 1.0sccm according to an embodiment of the present invention2O3And (3) a stability test curve graph of dark current and photocurrent of the photoelectric detector corresponding to the thin film under 254nm solar blind ultraviolet illumination along with time change.
Detailed Description
The embodiment of the invention provides amorphous Ga2O3The photodetector includes: substrate, depositionHydrogen-doped amorphous Ga on the surface of a substrate2O3Thin film active layer and amorphous Ga doped with hydrogen2O3An electrode on the thin film active layer;
wherein, the hydrogen-doped amorphous Ga2O3The film active layer is an amorphous film prepared by a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere. The vacuum deposition method includes any one of magnetron sputtering, pulsed laser deposition, electron beam deposition, chemical vapor deposition, and the like.
The substrate may comprise one or more of mica, polyimide, polyethylene terephthalate, polyethylene naphthalate, polyvinyl chloride, polycarbonate, polystyrene, polyethylene, polypropylene, sapphire, silicon carbide, quartz glass, polymethylmethacrylate, plexiglass or gallium arsenide;
the electrode comprises one or more materials of Indium Tin Oxide (ITO), Aluminum Zinc Oxide (AZO), Gallium Zinc Oxide (GZO), Fluorine Tin Oxide (FTO), chromium, copper, silver, gold, nickel, titanium gold, aluminum or platinum.
Amorphous Ga2O3The structure of the photodetector is one of a metal-semiconductor-metal (MSM) structure, a PN junction structure, a PIN junction structure, or a Schottky diode structure.
FIG. 1 shows the reduction or elimination of amorphous Ga by hydrogen doping2O3Schematic view of defect, wherein the upper diagram is amorphous Ga without hydrogen doping2O3According to the schematic diagram of the thin film, a plurality of defects such as oxygen vacancies, gallium dangling bonds and the like can be seen, so that the dark current of the device is higher, and therefore, the light-dark ratio of the detector is lower, and the power consumption is higher. The lower figure is amorphous Ga prepared by a vacuum deposition method at the temperature of 20-400 ℃ in hydrogen-containing atmosphere2O3The film has a molecular structure schematic diagram, wherein hydrogen and gallium dangling bonds form Ga-H bonds, and the defect concentration of oxygen vacancies in the film is reduced by occupying the lattice positions of the oxygen vacancies by hydrogen, so that the dark current is effectively reduced, and the light-dark ratio is improved.
Hydrogen-doped amorphous Ga2O3The photoelectric detector can greatly improve the light-dark ratio on the premise of maintaining high responsivity, and the main reason is derived fromTwo aspects are as follows: 1. amorphous Ga2O3The film has a plurality of oxygen vacancy defects and gallium metal dangling bonds, and hydrogen is doped into the film to occupy the positions of the oxygen vacancies to be combined with the gallium metal dangling bonds, so that the oxygen vacancy defects and the metal dangling bonds can be effectively passivated, the defect concentration is greatly reduced, and the dark current of the photoelectric detector is greatly reduced; 2. the doping of hydrogen will be in amorphous Ga2O3Bonds such as-OH, Ga-H and the like are formed in the film, the density of interband states is increased, and the concentration of carriers excited under illumination is increased, so that the hydrogen is doped to maintain large response of the device, and the light-dark ratio of the device is improved.
Accordingly, embodiments of the present invention provide amorphous Ga2O3The preparation method of the photoelectric detector comprises the following main processes:
pretreating the substrate: and ultrasonically cleaning the substrate by using a chemical reagent and drying the substrate by blowing.
Putting the pretreated substrate into a cavity of vacuum deposition equipment, starting a vacuum pump, and preparing the hydrogen-doped amorphous Ga by adopting a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere2O3Thin film active layer: specifically, after the vacuum pump is started, the cavity of the vacuum deposition equipment is pumped to the background vacuum, the hydrogen-containing gas is introduced into the ultrahigh-precision gas flowmeter, the vacuum numerical value in the cavity after the hydrogen-containing gas is introduced is recorded, the hydrogen-containing gas is uniformly distributed in the cavity after the flow rate of the hydrogen-containing gas and the vacuum in the cavity are stable for a period of time, and then amorphous Ga is started2O3And (4) coating or depositing the film.
In the preparation of the obtained hydrogen-doped amorphous Ga2O3Preparing an electrode on the thin film active layer: by ultraviolet exposure and development and fixation, the hydrogen-doped amorphous Ga is added2O3And photoetching an electrode structure on the thin film active layer, then depositing an electrode medium, and stripping and removing the photoresist and the electrode medium on the photoresist.
In this embodiment, hydrogen-containing gases that may be specifically used include hydrogen or ammonia; wherein the hydrogen comprises protium, deuterium, tritium.
The invention adopts the method that the hydrogen-containing atmosphere is adoptedPrepared amorphous Ga2O3Amorphous Ga for photodetector2O3Thin film active layer of amorphous Ga2O3Oxygen vacancy defects in the active layer of the film are occupied by doping of hydrogen and combined with gallium metal dangling bonds to promote amorphous Ga2O3Performance of the photodetector.
The preparation method of the invention has the following advantages:
1. the invention is in amorphous Ga2O3The flow of the hydrogen-containing gas is regulated and controlled by a high-precision gas flow controller in the film growth process, so that the defects in the film can be effectively reduced or eliminated, and the dark current is greatly reduced under the condition that the photocurrent is kept unchanged, thereby greatly improving the light-dark ratio of the device.
2. The hydrogen-doped amorphous Ga prepared by the invention2O3The solar blind photoelectric detector is sensitive in response to the solar blind area, the light-dark ratio is improved under the condition of maintaining the response constant, and the hydrogen-containing gas flow in the film growth process is regulated and controlled to achieve the light-dark ratio of more than 107Light-to-dark ratio of order of magnitude.
3. The hydrogen-doped amorphous Ga prepared by the invention2O3The photoelectric detector can realize high-sensitivity X-ray detection, and has the advantages of small dark current, high light-dark ratio, good repeatability and stable performance.
4. The whole process of film deposition and device preparation can be completed at room temperature and low temperature, and the preparation method has the advantages of low preparation cost and simple process, and is suitable for large-area industrial research.
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention will be further described in detail by embodiments with reference to the accompanying drawings.
Example 1
This example provides a high light-to-dark ratio amorphous Ga2O3The structure of the photoelectric detector is a metal-semiconductor-metal (MSM) structure. The specific preparation method of the photodetector of this embodiment is as follows:
step 1: a piece of a 15mm by 0.5mm size deep ultra-violet ultra-pure quartz substrate was cleaned by ultrasonic cleaning and blow-dried with dry high purity nitrogen gas, and placed on a sample holder of the same size. After the substrate is fixed, the substrate is placed into a growth chamber of a magnetron sputtering apparatus provided with a gallium oxide ceramic target (the purity of the gallium oxide ceramic target used in the example is 99.999%), a sample table is lifted to the highest position (the distance between the target and the substrate is about 8mm), a baffle plate below the sample is closed, and finally a quick-release opening of the chamber is screwed down.
Step 2: starting a vacuum pumping system of the cavity, introducing 0.5sccm high-purity hydrogen into the vacuum chamber through a high-precision gas flowmeter after the background vacuum in the cavity is lower than 4.5E-4Pa, waiting for about 10min to uniformly distribute the hydrogen in the cavity, continuing introducing 10sccm high-purity argon as sputtering gas if the hydrogen flow and the vacuum in the cavity are kept unchanged, wherein the vacuum in the cavity is 1.6E-1Pa, gradually closing a molecular pump to connect a gate valve of the cavity, and increasing the pressure of a 300V plate to start brightness when the vacuum in the cavity rises to 2-3 Pa. After the normal glow starting, the sputtering power is adjusted to be 60W, the sputtering pressure is adjusted to be 0.4Pa, the baffle plate below the sample is opened to start formal sputtering after the pre-sputtering is carried out for 5min, when the total sputtering time is 15min (the thickness of the gallium oxide layer is about 83nm), the sputtering is completely stopped, and the pump is stopped to take out the sample.
And step 3: and (3) coating a 1-micron thick S6487 positive photoresist on the hydrogen-doped gallium oxide film obtained in the step (2) by a spin coating method. The photoresist coated samples were placed on a hot plate stable at 115 ℃ for a pre-bake of 65 seconds.
And 4, step 4: the electrode structures were exposed on the sample film using a well-known uv lithography machine MA6, using a mask plate structure of 5 μm wide, 5 μm pitch, 300 μm long, for a total of 75 pairs of interdigitated structures. And developing and fixing the exposed sample by adopting MF-319 as a developing solution and deionized water as a fixing solution.
And 5: and (4) depositing an Indium Tin Oxide (ITO) electrode with the thickness of 80nm on the sample obtained in the step (4) by utilizing a magnetron sputtering process. The specific parameters of magnetron sputtering are as follows: the sputtering power is 50W, the sputtering pressure is 0.4Pa, the sputtering gas is high-purity argon of 10sccm, the sample table is kept at the highest position during sputtering, and the total sputtering time is 8 min.
Step 6: for the sample obtained in step 5Stripping acetone to remove the redundant photoresist and the ITO electrode thereon, thereby forming an interdigital electrode and finally obtaining amorphous Ga2O3A photodetector. Denoted sample 1.
Two parts of the ITO electrodes were wired to the ketely 6487 source meter with conductive silver paste, the voltage was held constant and uv response testing was performed using a 254nm uv hand lamp.
Example 2
The present embodiment is substantially the same as embodiment 1, except that in step 2, after the background vacuum is pumped to be lower than 4.5E-4Pa, 1.0sccm of high-purity hydrogen is introduced, after the gas flow is stable, the process waits for 10min, if the hydrogen flow and the vacuum in the chamber are stable, 10sccm of high-purity argon is introduced, the vacuum in the chamber reaches 1.6E-1Pa, and Ga is sputtered to initiate glow2O3And the thickness of the film is about 84 nm. Amorphous Ga obtained finally2O3The photodetector is denoted sample 2.
Example 3
This example is substantially the same as example 1, except that: in the step 2, after the background vacuum is pumped to be lower than 4.5E-4Pa, 1.5sccm of high-purity hydrogen is introduced, after the gas flow is stable, the waiting time is 10min, if the hydrogen flow and the vacuum in the cavity are stable, 10sccm of high-purity argon is introduced, the vacuum in the cavity reaches 1.6E-1Pa, and the Ga is sputtered under glow2O3And the thickness of the film is about 85 nm. Amorphous Ga obtained finally2O3The photodetector is denoted as sample 3.
Example 4
This example is substantially the same as example 1, except that: in the step 2, after the background vacuum is pumped to be lower than 4.5E-4Pa, introducing high-purity hydrogen of 2.0sccm, the vacuum in the cavity reaches 1.6E-3Pa, waiting for 10min after the gas flow is stable, introducing high-purity argon of 10sccm if the oxygen flow and the vacuum in the cavity are stable, the vacuum in the cavity reaches 1.6E-1Pa, and starting to sputter Ga2O3And the thickness of the film is about 93 nm. Amorphous Ga obtained finally2O3The photodetector is denoted as sample 4.
For the above examples 1-4, we also designed comparative example 1 for comparative illustration.
Comparative example 1
A photodetector of the present invention was fabricated by substantially the same procedure as in example 1, except that in step 2, after the background vacuum was evacuated to less than 4.5E-4Pa, high-purity hydrogen gas (hydrogen flow: 0sccm) was not introduced, high-purity argon gas of 10sccm was directly introduced, the vacuum in the chamber reached 1.6E-1Pa, and Ga was sputtered under glow2O3And the thickness of the film is about 84 nm. Amorphous Ga obtained finally2O3The photodetector is denoted as comparative sample 1.
In FIGS. 2 to 5, the flow rates of the sputtering hydrogen gas corresponding to comparative sample 1 and samples 1 to 4 are shown to be 0sccm, 0.5sccm, 1.0sccm, 1.5sccm and 2.0sccm, respectively.
Fig. 2 shows the optical transmittance maps of the magnetron sputtering samples under different hydrogen flow rates. As can be seen from the graph, the hydrogen flow rate was determined for Ga before and after doping2O3The transmittance of the film has little effect. All amorphous Ga2O3The absorption edge of the film is about 250nm, and the film has a transmittance of more than 85% for light with a wavelength of 300nm or more.
Fig. 3 gives XRD patterns of the magnetron sputtered samples at different hydrogen flow rates. No diffraction peak was observed except for an amorphous diffraction peak around 21.5 ° of the quartz substrate. From this, it can be seen that all of the hydrogen-doped Ga2O3Are all amorphous films.
FIG. 4 shows the magnetron sputter deposited amorphous Ga in different hydrogen flow rates2O3Graph of dark current versus voltage for a thin film corresponding photodetector under 254nm solar blind uv illumination. The flow rates of the sputter hydrogen gas for the samples were 0sccm, 0.5sccm, 1.0sccm, 1.5sccm, and 2.0sccm, respectively, and it can be seen that the dark current of the comparative sample 1 without hydrogen doping was about 1X 10 at the same applied voltage-6Ampere, while dark current for samples 1-4 with hydrogen doping is about 1X 10-9～1×10-11Ampere, dark current is greatly reduced.
FIG. 5 shows the magnetron sputter deposited amorphous Ga in different hydrogen flow rates2O3And (3) a graph of photocurrent of a photoelectric detector corresponding to the thin film under 254nm solar blind ultraviolet illumination along with voltage change. The flow rates of the sputter hydrogen gas for the samples were 0sccm, 0.5sccm, 1.0sccm, 1.5sccm, and 2.0sccm, respectively, and it can be seen that the photocurrent for all the samples was about 1X 10 at the same applied voltage-3Amperometric indicates that hydrogen incorporation did not result in a decrease in photocurrent. The light-to-dark ratio of comparative sample 1 without hydrogen doping was only 103And the light-to-dark ratio of samples 1-4 exceeds 107. This shows that the light-dark ratio of the device is effectively improved by the hydrogen doping on the premise of ensuring that the responsivity of the device is not changed.
Example 5
This example provides a high light-to-dark ratio amorphous Ga2O3The structure of the thin film ultraviolet photoelectric detector is an MSM structure, wherein the substrate is quartz glass, and the electrode is an ITO electrode.
The ultraviolet photodetector of this embodiment is substantially the same as that of embodiment 1, except that in step 2, after the background vacuum is pumped to a pressure lower than 4.5E-4Pa, ammonia gas with a flow rate of 5sccm is introduced through the high-precision flow meter, and after the gas pressure is stabilized, amorphous Ga deposition is started2O3A film. The substrate temperature was room temperature. Amorphous Ga obtained finally2O3The photodetector is denoted as sample 5.
Two parts of the ITO electrodes were wired to the ketely 6487 source meter with conductive silver paste, the voltage was held constant and uv response testing was performed using a 254nm uv hand lamp. Amorphous Ga deposited under the same applied voltage and the condition of introducing ammonia2O3Compared with amorphous Ga deposited under the condition of not introducing ammonia gas, the film ultraviolet photoelectric detector2O3For a thin film ultraviolet photodetector, the optical dark ratio can be improved by 1 order of magnitude.
Example 6
This example provides a high light-to-dark ratio amorphous Ga2O3The structure of the thin film ultraviolet photoelectric detector is a Schottky diode structure, wherein the substrate is quartz glass, and the electrode is an ITO electrode.
This exampleThe method is basically the same as the embodiment 1, except that different masks are adopted to prepare the schottky diode structure by the ultraviolet exposure technology after the film preparation is finished in the steps 3 and 4. Amorphous Ga obtained finally2O3The photodetector is denoted sample 6.
Two parts of the ITO electrodes were wired to the ketely 6487 source meter with conductive silver paste, the voltage was held constant and uv response testing was performed using a 254nm uv hand lamp. Schottky diode type amorphous Ga deposited under the condition of 0.5sccm hydrogen under the same applied voltage2O3The film ultraviolet photoelectric detector is compared with Schottky diode type amorphous Ga deposited under the condition of no hydrogen2O3For thin film UV photodetectors, the optical-to-dark ratio is from about 104To about 105It can be shown that the incorporation of hydrogen effectively increases the light-dark ratio of the ultraviolet photodetector.
Example 7
This example provides a high optical-dark ratio hydrogen-doped amorphous Ga2O3The thin film X-ray detector is of an MSM structure, wherein the substrate is quartz glass, and the electrode is an ITO electrode.
The detector of this embodiment is substantially the same as embodiment 1, except that the active layer in steps 1 and 2 is prepared by plasma enhanced atomic layer deposition, and hydrogen is introduced in a pulse form during deposition at a growth temperature of 100 ℃ after the background vacuum is stabilized, wherein the amount of introduced hydrogen is 0.5sccm, and the thickness of the film is 80 nm. Amorphous Ga obtained finally2O3The photodetector is denoted as sample 7.
And connecting the two parts of ITO electrodes to a Kethely 6487 source meter by using conductive silver adhesive through a wire, keeping the voltage constant, and performing an X-ray response test by using an X-ray light source.
For example 7 above, we also designed comparative example 2 for comparative illustration.
Comparative example 2
This comparative example provides a high light-to-dark ratio hydrogen-doped amorphous Ga2O3A method for preparing a film X-ray detector. Book (I)The X-ray detector of the comparative example is substantially the same as example 7 except that no hydrogen gas is introduced after the background vacuum has stabilized in step 2.
The structure is MSM structure, wherein the substrate is quartz glass, and the electrode is ITO electrode. And connecting the two parts of ITO electrodes to a Kethely 6487 source meter by using conductive silver adhesive through a wire, keeping the voltage constant, and performing an X-ray response test by using an X-ray light source.
FIG. 6 shows amorphous Ga prepared in example 7 deposited under 0.5sccm hydrogen2O3Thin film and amorphous Ga deposited in comparative example 2 without passing through hydrogen2O3And (3) a graph of the change of the photocurrent of the corresponding photoelectric detector of the thin film under the irradiation of X-rays along with the time. Sample 7 corresponds to the X-ray detector prepared from the sample film having a hydrogen flow rate of 0.5sccm in example 7, and comparative sample 2 corresponds to the X-ray detector prepared from the sample film not passing hydrogen in comparative example 2. At the same applied voltage, it can be seen that the photocurrent of sample 7 was about 1 × 10-4Ampere, the photocurrent of comparative sample 2 was about 1X 10-7The ampere indicates that the photoelectric current of the photoelectric detector is greatly increased by introducing hydrogen, thereby ensuring high responsivity. While the dark current of sample 7 was about 1X 10-10Ampere, dark current of about 1X 10 for comparative sample 2-11The amperes indicated that the introduction of hydrogen did not cause a significant increase in dark current in the sample. Amorphous Ga deposited under the same applied voltage and without hydrogen2O3The light-to-dark ratio of the thin film X-ray detector is about 104Amorphous Ga deposited under the condition of introducing 0.5sccm hydrogen2O3The light-dark ratio of the film X-ray detector is about 106. It can be shown that the incorporation of hydrogen effectively improves the optical dark ratio of the X-ray detector.
Example 8
This example provides a high light-to-dark ratio amorphous Ga2O3The structure of the thin film ultraviolet photoelectric detector is an MSM structure, wherein the substrate is quartz glass, and the electrode is an ITO electrode.
The detector of this embodiment is substantially the same as that of embodiment 1 except thatThe active layer in the steps 1 and 2 is prepared by adopting a plasma enhanced chemical vapor deposition method, and the amount of introduced hydrogen is 1.0sccm at the growth temperature of 200 ℃ after the background vacuum is stable. Amorphous Ga obtained finally2O3The photodetector is denoted as sample 8.
Two parts of the ITO electrodes were wired to the ketely 6487 source meter with conductive silver paste, the voltage was held constant and uv response testing was performed using a 254nm uv hand lamp.
FIG. 7 shows amorphous Ga deposited at a hydrogen flow rate of 1.0sccm, prepared in this example2O3And (3) a stability test curve of dark current and photocurrent of the photoelectric detector corresponding to the thin film under 254nm solar blind ultraviolet illumination along with time change. In more than 2 months of continuous observation, the photocurrent is almost kept unchanged, the dark current has a trend of decreasing, the light-dark ratio is increased, the hydrogen can stably exist in the film, the instability caused by the defects of the film is effectively improved by the passivation effect of the hydrogen, and the method has important significance in industrial application.
Although the electrode material in each of the above embodiments is an Indium Tin Oxide (ITO) thin film as an example, the material of the electrode of the present invention is not limited to the Indium Tin Oxide (ITO) thin film, and may be titanium gold, metal chromium, metal nickel, Aluminum Zinc Oxide (AZO), Gallium Zinc Oxide (GZO), Fluorine Tin Oxide (FTO), or the like.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are merely exemplary embodiments of the present invention, and are not intended to limit the scope of the present invention, and any modifications, equivalent substitutions, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (9)
1. Amorphous Ga2O3Photodetector characterized in that said amorphous Ga2O3The photodetector includes: substrate, hydrogen-doped amorphous Ga deposited on surface of substrate2O3A thin film active layer and a hydrogen-doped amorphous layer arranged on the active layerGa2O3An electrode on the thin film active layer;
wherein the hydrogen-doped amorphous Ga2O3The film active layer is an amorphous film prepared by a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere; the vacuum deposition method comprises any one of magnetron sputtering, pulsed laser deposition, electron beam deposition and chemical vapor deposition;
amorphous Ga prepared in hydrogen-containing atmosphere2O3Amorphous Ga for photodetector2O3Thin film active layer of amorphous Ga2O3The oxygen vacancy defects in the active layer of the film are occupied by hydrogen incorporation and combine with gallium metal dangling bonds, thereby reducing or eliminating the amorphous Ga2O3Defects in thin film active layers.
2. Amorphous Ga according to claim 12O3A photodetector, wherein the substrate comprises one or more of mica, polyimide, polyethylene terephthalate, polyethylene naphthalate, polyvinyl chloride, polycarbonate, polystyrene, polyethylene, polypropylene, sapphire, silicon carbide, quartz glass, polymethyl methacrylate, plexiglass, or gallium arsenide;
the electrode comprises one or more of Indium Tin Oxide (ITO), Aluminum Zinc Oxide (AZO), Gallium Zinc Oxide (GZO), Fluorine Tin Oxide (FTO), chromium, copper, silver, gold, nickel, titanium gold, aluminum or platinum.
3. Amorphous Ga according to claim 12O3Photodetector characterized in that said amorphous Ga2O3The structure of the photoelectric detector is one of a metal-semiconductor-metal MSM structure, a PN junction structure, a PIN junction structure or a Schottky diode structure.
4. Amorphous Ga as claimed in claim 12O3A method of fabricating a photodetector, the method comprising:
preprocessing a substrate;
putting the pretreated substrate into a cavity of vacuum deposition equipment, starting a vacuum pump, and preparing the hydrogen-doped amorphous Ga by adopting a vacuum deposition method at the temperature of 20-400 ℃ in a hydrogen-containing atmosphere2O3A thin film active layer;
in the hydrogen-doped amorphous Ga2O3And preparing an electrode on the thin film active layer.
5. The method according to claim 4, wherein the pre-treating the substrate specifically comprises: and ultrasonically cleaning the substrate by using a chemical reagent and drying the substrate by blowing.
6. The method according to claim 4, wherein the hydrogen-doped amorphous Ga is2O3The preparation of the electrode on the thin film active layer specifically comprises the following steps:
by ultraviolet exposure and development and fixation, the hydrogen-doped amorphous Ga is added2O3Photoetching an electrode structure on the thin film active layer;
depositing an electrode medium;
and stripping and removing the photoresist and the electrode medium on the photoresist.
7. The method according to claim 4, wherein after the starting of the vacuum pump, the method specifically comprises:
after the cavity of the vacuum deposition equipment is pumped to the background vacuum, hydrogen-containing gas is introduced in advance, and after the vacuum degree is stable, hydrogen-doped amorphous Ga is carried out in the hydrogen-containing atmosphere2O3And depositing a thin film active layer.
8. The production method according to claim 7, wherein the hydrogen-containing gas includes hydrogen gas or ammonia gas; the hydrogen comprises protium, deuterium, tritium.
9. Amorphous Ga as claimed in any one of claims 1 to 32O3Method for improving performance of photoelectric detectorCharacterized in that the method comprises:
amorphous Ga prepared in hydrogen-containing atmosphere2O3Amorphous Ga for photodetector2O3Thin film active layer of amorphous Ga2O3Oxygen vacancy defects in the thin film active layer are occupied by hydrogen incorporation and bond with gallium metal dangling bonds.
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