CN111139449A - Zinc oxide based transparent electrode photoelectric detector and preparation method thereof - Google Patents
Zinc oxide based transparent electrode photoelectric detector and preparation method thereof Download PDFInfo
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- CN111139449A CN111139449A CN201911423521.7A CN201911423521A CN111139449A CN 111139449 A CN111139449 A CN 111139449A CN 201911423521 A CN201911423521 A CN 201911423521A CN 111139449 A CN111139449 A CN 111139449A
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- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 title claims abstract description 310
- 239000011787 zinc oxide Substances 0.000 title claims abstract description 155
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 229910052751 metal Inorganic materials 0.000 claims abstract description 48
- 239000002184 metal Substances 0.000 claims abstract description 46
- 229910052725 zinc Inorganic materials 0.000 claims abstract description 35
- 239000011701 zinc Substances 0.000 claims abstract description 35
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims abstract description 34
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 34
- 239000000758 substrate Substances 0.000 claims abstract description 33
- 238000000151 deposition Methods 0.000 claims abstract description 30
- 238000000034 method Methods 0.000 claims abstract description 17
- 239000007789 gas Substances 0.000 claims description 68
- 239000004065 semiconductor Substances 0.000 claims description 57
- 239000001257 hydrogen Substances 0.000 claims description 16
- 229910052739 hydrogen Inorganic materials 0.000 claims description 16
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 15
- 230000004888 barrier function Effects 0.000 claims description 15
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N titanium dioxide Inorganic materials O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 15
- 230000008021 deposition Effects 0.000 claims description 12
- 239000002019 doping agent Substances 0.000 claims description 11
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 11
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 claims description 10
- 229910052782 aluminium Inorganic materials 0.000 claims description 10
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 10
- 230000000903 blocking effect Effects 0.000 claims description 10
- 229910052733 gallium Inorganic materials 0.000 claims description 10
- 229910052738 indium Inorganic materials 0.000 claims description 10
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims description 10
- HQWPLXHWEZZGKY-UHFFFAOYSA-N diethylzinc Chemical compound CC[Zn]CC HQWPLXHWEZZGKY-UHFFFAOYSA-N 0.000 claims description 5
- JLTRXTDYQLMHGR-UHFFFAOYSA-N trimethylaluminium Chemical compound C[Al](C)C JLTRXTDYQLMHGR-UHFFFAOYSA-N 0.000 claims description 5
- 238000004519 manufacturing process Methods 0.000 claims description 4
- HBCLZMGPTDXADD-UHFFFAOYSA-N C[Zn](C)C Chemical compound C[Zn](C)C HBCLZMGPTDXADD-UHFFFAOYSA-N 0.000 claims description 3
- RGGPNXQUMRMPRA-UHFFFAOYSA-N triethylgallium Chemical group CC[Ga](CC)CC RGGPNXQUMRMPRA-UHFFFAOYSA-N 0.000 claims description 3
- IBEFSUTVZWZJEL-UHFFFAOYSA-N trimethylindium Chemical group C[In](C)C IBEFSUTVZWZJEL-UHFFFAOYSA-N 0.000 claims description 3
- 229910052760 oxygen Inorganic materials 0.000 abstract description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 10
- 239000001301 oxygen Substances 0.000 abstract description 10
- 238000000605 extraction Methods 0.000 abstract description 5
- 238000012360 testing method Methods 0.000 description 13
- 238000006243 chemical reaction Methods 0.000 description 11
- 238000002834 transmittance Methods 0.000 description 8
- 238000001514 detection method Methods 0.000 description 7
- 230000000694 effects Effects 0.000 description 7
- 239000010408 film Substances 0.000 description 7
- 230000004044 response Effects 0.000 description 7
- FMRLDPWIRHBCCC-UHFFFAOYSA-L Zinc carbonate Chemical compound [Zn+2].[O-]C([O-])=O FMRLDPWIRHBCCC-UHFFFAOYSA-L 0.000 description 6
- 239000000969 carrier Substances 0.000 description 6
- 239000000386 donor Substances 0.000 description 6
- 238000002425 crystallisation Methods 0.000 description 4
- 230000008025 crystallization Effects 0.000 description 4
- 239000000852 hydrogen donor Substances 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 239000011521 glass Substances 0.000 description 3
- 238000012545 processing Methods 0.000 description 3
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 239000002585 base Substances 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 239000012535 impurity Substances 0.000 description 2
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 2
- 230000031700 light absorption Effects 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 230000003287 optical effect Effects 0.000 description 2
- 230000006798 recombination Effects 0.000 description 2
- 238000005215 recombination Methods 0.000 description 2
- 230000007480 spreading Effects 0.000 description 2
- 238000003892 spreading Methods 0.000 description 2
- 230000004913 activation Effects 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000005229 chemical vapour deposition Methods 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- -1 hydrogen ions Chemical class 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 238000005459 micromachining Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000003071 parasitic effect Effects 0.000 description 1
- 238000001259 photo etching Methods 0.000 description 1
- 238000009832 plasma treatment Methods 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000004043 responsiveness Effects 0.000 description 1
- 229910052594 sapphire Inorganic materials 0.000 description 1
- 239000010980 sapphire Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
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- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/02—Pretreatment of the material to be coated
- C23C16/0272—Deposition of sub-layers, e.g. to promote the adhesion of the main coating
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/40—Oxides
- C23C16/407—Oxides of zinc, germanium, cadmium, indium, tin, thallium or bismuth
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- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/44—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating
- C23C16/455—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating characterised by the method used for introducing gases into reaction chamber or for modifying gas flows in reaction chamber
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- 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
- H01L31/02—Details
- H01L31/0224—Electrodes
- H01L31/022466—Electrodes made of transparent conductive layers, e.g. TCO, ITO layers
- H01L31/022483—Electrodes made of transparent conductive layers, e.g. TCO, ITO layers composed of zinc oxide [ZnO]
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Abstract
The invention belongs to the technical field of photoelectric detectors, and particularly relates to a preparation method of a zinc oxide-based transparent electrode photoelectric detector, which comprises the following steps: obtaining a substrate on which a photodetector is formed; and providing a zinc source, a doped metal source and water, and depositing on the surface of one side of the photoelectric detector far away from the substrate at the temperature of 300-450 ℃ to form a zinc oxide-based transparent electrode layer to obtain the zinc oxide-based transparent electrode photoelectric detector. The method for preparing the zinc oxide based transparent electrode photoelectric detector takes water as an oxygen source, so that the prepared zinc oxide based transparent electrode photoelectric detector has the characteristics of high reliability, low forward working voltage, high light extraction efficiency and the like.
Description
Technical Field
The invention belongs to the technical field of photoelectric detectors, and particularly relates to a zinc oxide-based transparent electrode photoelectric detector and a preparation method thereof.
Background
CdS/TiO2When the semiconductor photoelectric detection chip is in the visible light wave bandThe performance is superior, and the method has wide application prospect in the aspects of photoelectric detection, image recognition and the like. The transparent conductive glass substrate solves the light absorption problem of the substrate, but the high-quality top transparent electrode needs breakthrough of materials and technology, the ITO transparent electrode is the mainstream technology of the current transparent electrode, but the ITO is expensive, the resources are scarce, the micro-processing is difficult, and the yield is difficult to ensure. The ZnO-based transparent electrode (ZnO-TCL) not only has high transmittance and low resistivity comparable to ITO, but also has the advantages of abundant resources, low price, no need of strong acid and strong alkali for micromachining, environmental friendliness and the like, and represents a development trend of future LED transparent electrodes as a third-generation transparent electrode material. ZnO-TCL (indium tin oxide) instead of ITO (indium tin oxide) applied to CdS/TiO2The photoelectric detection chip is an effective way for realizing the high-efficiency photoelectric chip.
At present, the preparation of zinc oxide-based transparent conductive film mostly adopts sputtering technology, but the compactness and the crystallization quality of the film prepared by the method are poor, and the film is similar to TiO2The contact interface is not controllable, ohmic contact is difficult to form, contact resistance is high, and the method is not applied to the photoelectric chip industry. The Metal Organic Chemical Vapor Deposition (MOCVD) is an effective means for preparing high-quality zinc oxide-based transparent conductive films due to the advantages of mass production, high crystallization quality of epitaxially grown semiconductor films, controllable growth mode and interface, compatibility with the existing photoelectric chip process and the like.
However, the ZnO-based transparent electrode prepared by the MOCVD method mostly utilizes high-purity oxygen as an oxygen source, the growth temperature is 500-550 ℃, and the zinc oxide-based transparent conductive film and TiO are added due to the high growth temperature2The interdiffusion and reaction of elements such as Ti, Zn, O and the like between interfaces lead to easy formation of high-resistance oxides between the interfaces, which causes overhigh contact resistance, and simultaneously, the high-temperature growth improves the requirements on equipment and increases the process cost. In addition, due to TiO2The doping concentration of the heavily doped contact layer on the surface is difficult to achieve 1020/cm3,TiO2Ohmic contact to the oxide transparent electrode is difficult to form.
Disclosure of Invention
The invention aims to provide a preparation method of a zinc oxide-based transparent electrode photoelectric detector, and aims to solve the technical problems that the existing zinc oxide-based transparent electrode is high in preparation temperature, too high in resistance of an electrode and a semiconductor interface, difficult to form ohmic contact and the like.
Another object of the present invention is to provide a zinc oxide-based transparent electrode photodetector.
In order to achieve the purpose of the invention, the technical scheme adopted by the invention is as follows:
a preparation method of a zinc oxide based transparent electrode photoelectric detector comprises the following steps:
obtaining a substrate on which a photodetector is formed;
and providing a zinc source, a doped metal source and water, and depositing on the surface of one side of the photoelectric detector far away from the substrate at the temperature of 300-450 ℃ to form a zinc oxide-based transparent electrode layer to obtain the zinc oxide-based transparent electrode photoelectric detector.
Preferably, the step of providing a zinc source, a doped metal source and water comprises: at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~4×10-3Providing water at a flow rate of moles/minute; and/or the presence of a gas in the gas,
the pressure for forming the zinc oxide-based transparent electrode layer by deposition is 6-12 Torr; and/or the presence of a gas in the gas,
the photodetector includes a photosensitive semiconductor layer and a blocking semiconductor layer.
Preferably, the step of depositing a zinc oxide-based transparent electrode layer on the surface of the photodetector far away from the substrate comprises:
at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 1X 10 mol/min-3~4×10-3Providing water at a flow rate of mol/min, and depositing on the surface of one side of the photoelectric detector, which is far away from the substrate, to form a first zinc oxide-based transparent electrode layer under the conditions that the temperature is 300-400 ℃ and the pressure is 6-12 Torr;
at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~1×10-3Providing water at a flow rate of mol/min, and depositing on the surface of the first zinc oxide-based transparent electrode layer to form a second zinc oxide-based transparent electrode layer under the conditions that the temperature is 400-450 ℃ and the pressure is 6-12 Torr.
Preferably, the barrier semiconductor layer includes: TiO 22Doped TiO 22At least one of NiO, CuO and SnSe; and/or the presence of a gas in the gas,
the photosensitive semiconductor layer includes: at least one of CdS, ZnO and doped ZnO; and/or the presence of a gas in the gas,
the thickness of the barrier semiconductor layer is 50-500 nm; and/or the presence of a gas in the gas,
the thickness of the photosensitive semiconductor layer is 20-500 nm.
Preferably, the zinc source is selected from: at least one of diethyl zinc and trimethyl zinc; and/or the presence of a gas in the gas,
the doped metal source is selected from: at least one of aluminum source, indium source and gallium source.
Preferably, the aluminium source is selected from trimethylaluminium; and/or the presence of a gas in the gas,
the indium source is selected from trimethyl indium; and/or the presence of a gas in the gas,
the gallium source is selected from triethyl gallium.
Preferably, in the zinc oxide-based transparent electrode layer, the mass ratio of the doped metal element to the zinc element is 1-10%; and/or the presence of a gas in the gas,
the thickness of the first zinc oxide-based transparent electrode layer is 10-50 nm; and/or the presence of a gas in the gas,
the thickness of the second zinc oxide-based transparent electrode layer is 90-450 nm; and/or the presence of a gas in the gas,
the thickness of the zinc oxide-based transparent electrode layer is 100-500 nm.
Correspondingly, the invention also provides a zinc oxide based transparent electrode photoelectric detector, which comprises a photoelectric detector and a zinc oxide based transparent electrode layer, wherein a hydrogen-rich layer is formed between the photoelectric detector and the zinc oxide based transparent electrode layer, and the zinc oxide based transparent electrode layer contains metal doped elements
Preferably, the photodetector includes a photosensitive semiconductor layer and a blocking semiconductor layer; and/or the presence of a gas in the gas,
in the zinc oxide-based transparent electrode layer, the mass ratio of the metal doping element to the zinc element is 1-10%; and/or the presence of a gas in the gas,
the thickness of the zinc oxide-based transparent electrode layer is 100-500 nm; and/or the presence of a gas in the gas,
the metal doping element is selected from: at least one of aluminum, indium and gallium.
Preferably, the barrier semiconductor layer comprises TiO2Doped TiO2At least one of NiO, CuO and SnSe; and/or the presence of a gas in the gas,
the photosensitive semiconductor layer comprises at least one of CdS, ZnO and doped ZnO; and/or the presence of a gas in the gas,
the thickness of the barrier semiconductor layer is 50-500 nm; and/or the presence of a gas in the gas,
the thickness of the photosensitive semiconductor layer is 20-500 nm.
According to the preparation method of the zinc oxide-based transparent electrode photoelectric detector, provided by the invention, a zinc source, a doped metal source and water are provided, and a zinc oxide-based transparent electrode layer is deposited on the surface of one side of the photoelectric detector, which is far away from the substrate, at the temperature of 300-450 ℃, so that the zinc oxide-based transparent electrode photoelectric detector can be prepared on the substrate. On one hand, water is used as an oxygen source, a hydrogen-rich layer is formed at the interface between the photoelectric detector and the zinc oxide transparent electrode, so that the interface is prevented from being oxidized, the interface carrier concentration is increased, and the ohmic contact is improved. Furthermore, the deposition temperature of the zinc oxide-based electrode layer is reduced by taking water as an oxygen source, the deposition of the zinc oxide-based electrode layer can be completed at a lower epitaxial temperature of 300-450 ℃, the mutual diffusion and interface reaction between the zinc oxide-based transparent electrode and a semiconductor layer of a photoelectric detector are greatly reduced, the formation of high-resistance oxides between interfaces is avoided, and the contact resistance and non-radiative recombination are reduced. On the other hand, the metal source is doped in the zinc oxide-based electrode layer, so that the concentration of donor carriers is improved, and the resistance is reduced, thereby improving the photoelectric response and the current spreading effect of the photoelectric detector. The zinc oxide-based transparent electrode photoelectric detector prepared by the invention has the characteristics of high reliability, low forward working voltage, high light extraction efficiency and the like.
The zinc oxide based transparent electrode photoelectric detector provided by the invention can be prepared by the method, and comprises a photoelectric detector, a zinc oxide based transparent electrode layer arranged on the surface of one side of the photoelectric detector, and a hydrogen-rich layer formed between the photoelectric detector and the zinc oxide based transparent electrode layer, wherein more hydrogen donors are introduced between the photoelectric detector and the zinc oxide layer by the hydrogen-rich layer, the hydrogen-rich layer has higher carrier concentration on the basis of doping conduction, and the zinc oxide based transparent electrode layer contains metal doping elements, so that the donor carriers of devices are further improved, the resistance is reduced, and the zinc oxide based transparent electrode photoelectric detector has high reliability, low forward working voltage and high light extraction efficiency.
Drawings
Fig. 1 is a schematic structural diagram of a photodetection chip according to embodiment 1 of the present invention.
FIG. 2 is an optical transmittance test chart of a zinc oxide-based transparent electrode layer according to example 1 of the present invention.
FIG. 3 is an XRD diffractogram of the zinc oxide-based transparent electrode layer of example 1 of the present invention.
FIG. 4 is a scanning electron microscope image of the surface structure of the zinc oxide-based transparent electrode layer in example 1 of the present invention.
Fig. 5 is a photo-response diagram of the photo-detection chip in embodiment 1 of the present invention.
Detailed Description
In order to make the purpose, technical solution and technical effect of the embodiments of the present invention clearer, the technical solution in the embodiments of the present invention is clearly and completely described, and it is obvious that the described embodiments are a part of the embodiments of the present invention, but not all embodiments. All other embodiments obtained by a person of ordinary skill in the art without any inventive step in connection with the embodiments of the present invention shall fall within the scope of protection of the present invention.
In the description of the present invention, it is to be understood that the terms "first", "second" and the like are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implying any number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
The weight of the related components mentioned in the description of the embodiments of the present invention may not only refer to the specific content of each component, but also represent the proportional relationship of the weight among the components, and therefore, the content of the related components is scaled up or down within the scope disclosed in the description of the embodiments of the present invention as long as it is in accordance with the description of the embodiments of the present invention. Specifically, the weight described in the description of the embodiment of the present invention may be a unit of mass known in the chemical industry field, such as μ g, mg, g, and kg.
The embodiment of the invention provides a preparation method of a zinc oxide based transparent electrode photoelectric detector, which comprises the following steps:
s10, obtaining a substrate with a photoelectric detector;
s20, providing a zinc source, a doped metal source and water, and depositing on the surface of one side, far away from the substrate, of the photoelectric detector to form a zinc oxide-based transparent electrode layer at the temperature of 300-450 ℃ to obtain the zinc oxide-based transparent electrode photoelectric detector.
According to the preparation method of the zinc oxide-based transparent electrode photoelectric detector provided by the embodiment of the invention, a zinc source, a doped metal source and water are provided, and a zinc oxide-based transparent electrode layer is deposited on the surface of one side of the photoelectric detector, which is far away from the substrate, at the temperature of 300-450 ℃, so that the zinc oxide-based transparent electrode photoelectric detector can be prepared on the substrate. On one hand, water is used as an oxygen source, a hydrogen-rich layer is formed at the interface between the photoelectric detector and the zinc oxide transparent electrode, so that the interface is prevented from being oxidized, the interface carrier concentration is increased, and the ohmic contact is improved. Furthermore, the deposition temperature of the zinc oxide-based electrode layer is reduced by taking water as an oxygen source, the deposition of the zinc oxide-based electrode layer can be completed at a lower epitaxial temperature of 300-450 ℃, the mutual diffusion and interface reaction between the zinc oxide-based transparent electrode and a semiconductor layer of a photoelectric detector are greatly reduced, the formation of high-resistance oxides between interfaces is avoided, and the contact resistance and non-radiative recombination are reduced. On the other hand, the metal source is doped in the zinc oxide-based electrode layer, so that the concentration of donor carriers is improved, and the resistance is reduced, thereby improving the photoelectric response and the current spreading effect of the photoelectric detector. The zinc oxide-based transparent electrode photoelectric detector prepared by the embodiment of the invention has the characteristics of high reliability, low forward working voltage, high light extraction efficiency and the like.
Specifically, in the above step S10, the substrate on which the photodetector is formed is acquired. In some embodiments, the photodetector includes a photosensitive semiconductor layer and a blocking semiconductor layer. In some embodiments, the barrier semiconductor layer includes: TiO 22Doped TiO 22NiO, CuO and SnSe. In some embodiments, the photosensitive semiconductor layer includes: at least one of CdS, ZnO and doped ZnO. In some embodiments, the photodetector uses CdS as the photosensitive semiconductor and TiO as the photosensitive semiconductor2As a barrier semiconductor, the CdS semiconductor material has good photosensitive characteristic, the photoelectric leakage current of a single CdS layer is large, and TiO is applied2The layer and CdS form a semiconductor junction photoelectric detector, which can reduce leakage current, improve photoelectric response effect and has excellent performance in visible light wave band.
In some embodiments, the substrate includes, but is not limited to, a transparent conductive glass substrate, although other transparent conductive substrates may also be employed.
In some embodiments, after the substrate on which the photodetector is formed is obtained, the surface of the photodetector is cleaned by ozone light treatment, acid washing, plasma treatment, or the like, so as to remove impurities on the surface of the device.
In some embodiments, the thickness of the barrier semiconductor layer is 50 to 500 nm. In some embodiments, the photosensitive semiconductor layer has a thickness of 20 to 500 nm. In some embodiments, the photodetector comprises TiO with a thickness of 50-500 nm2The layer and thickness is 20-50The photoelectric detector with the structural characteristic has better photoelectric response and other performances in a visible light wave band in a 0nm CdS layer.
Specifically, in step S20, a zinc source, a doped metal source, and water are provided, and a zinc oxide-based transparent electrode layer is deposited on a surface of the photodetector, which is away from the substrate, at a temperature of 300 to 450 ℃, so as to obtain the zinc oxide-based transparent electrode photodetector. According to the embodiment of the invention, water is used as an oxygen source, so that a zinc source and a doped metal source can be deposited at a lower temperature of 300-450 ℃ to form a zinc oxide-based transparent electrode layer, element interdiffusion and interface reaction between a semiconductor layer of a photoelectric detector and the zinc oxide-based transparent electrode are avoided, and the stability of a device is improved; and water is used as an oxygen source, a hydrogen-rich high carrier concentration layer can be formed at the interface, ohmic contact is improved and improved, the carrier concentration of the interface is improved, photoelectric response and current expansion effects are further improved, and forward voltage is reduced. If the reaction temperature is too low, the crystallization quality is poor, doping activation is insufficient, the conductivity is low, the carrier mobility is low, and the photoelectric conversion efficiency is low; if the reaction temperature is too high, the parasitic reaction is more in the growth process of the zinc oxide-based electrode layer, and the deposition rate is slow.
In some embodiments, the step of providing a zinc source, a doped metal source, and water comprises: at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~4×10-3The flow of moles/minute provides water. The temperature and pressure conditions in the embodiment of the invention ensure that all raw materials are fully reacted and deposited to form a zinc oxide-based transparent electrode layer; wherein, the zinc source, the doped metal source and the water source are provided under the conditions, which is beneficial to the uniform and stable deposition of the zinc oxide-based electrode layer, and the flow rate is 7 multiplied by 10-4~4×10-3The water is provided in mol/min, so that not only is a sufficient oxygen source provided for the deposition of zinc oxide, but also a hydrogen-rich layer can be formed on the interface between the semiconductor layer of the photoelectric detector and the zinc oxide electrode layer, the interface resistance is reduced, the optical signal conversion efficiency is improved, and the photoelectric responsiveness of the device is improvedCan be used.
In some embodiments, the zinc source is selected from: at least one of diethyl zinc and trimethyl zinc. In some embodiments, the doped metal source is selected from: at least one of aluminum source, indium source and gallium source. In some embodiments, the aluminum source is selected from trimethylaluminum. In some embodiments, the indium source is selected from trimethylindium. In some embodiments, the gallium source is selected from triethyl gallium.
In some embodiments, the pressure for depositing the zinc oxide-based transparent electrode layer is 6 to 12 Torr. The zinc sources, the aluminum sources, the indium sources, the gallium sources and other doped metal sources adopted in the embodiment of the invention have high reaction activity under the conditions that the temperature is 300-450 ℃ and the pressure is 6-12 Torr, and can be fully reacted and deposited to form the zinc oxide transparent electrode layer.
In some embodiments, the zinc oxide-based transparent electrode layer has a mass ratio of doped metal element to zinc element of 1% to 10%. The mass ratio of the metal element doped in the zinc oxide-based transparent electrode layer to the zinc element is 1-10%, the concentration of donor carriers is improved, the resistance is reduced, and if the content of the doped metal element is too low, the concentration of the carriers is too low, so that the resistance is increased; if the content of the doped metal elements is too high, the doped metal elements cannot be completely activated to form a scattering center, the carrier mobility is reduced, the resistance is also increased, and the photoelectric conversion of the detector is not facilitated.
In some embodiments, the zinc oxide-based transparent electrode layer has a thickness of 100 to 500 nm. The thickness of the zinc oxide-based electrode is 100-500 nanometers, the balance between the square resistance and the transmittance is effectively balanced by the zinc oxide-based electrode, if the zinc oxide-based transparent electrode layer is too thick, the square resistance is small, the light absorption is increased, the transmittance is reduced, the deposition time of the electrode layer is long, and the cost is high.
In some embodiments, the step of depositing a zinc oxide-based transparent electrode layer on a surface of the photodetector away from the substrate comprises:
at 8X 10-5~4×10-4The flow rate of mol/min provides a zinc sourceAt 7X 10-6~4×10-5The dopant metal source was supplied at a flow rate of 1X 10 mol/min-3~4×10-3Providing water at a flow rate of mol/min, and depositing on the surface of one side of the photoelectric detector, which is far away from the substrate, to form a first zinc oxide-based transparent electrode layer under the conditions that the temperature is 300-400 ℃ and the pressure is 6-12 Torr;
at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~1×10-3Providing water at a flow rate of mol/min, and depositing on the surface of the first zinc oxide-based transparent electrode layer to form a second zinc oxide-based transparent electrode layer under the conditions that the temperature is 400-450 ℃ and the pressure is 6-12 Torr.
The embodiment of the invention provides a preparation method of a zinc oxide-based transparent electrode photoelectric detector, wherein the zinc oxide-based transparent electrode layer is prepared in two steps, a first zinc oxide transparent electrode layer is prepared under the condition of large water flow rate to form a contact layer, more hydrogen donors can be introduced between the surface of one side of the photoelectric detector, which is far away from a substrate, and the zinc oxide layer, and the zinc oxide-based transparent electrode layer has higher carrier concentration on the basis of doping and conduction and is used as a donor to increase the carrier concentration at an interface and reduce the contact resistance. But this layer is only introduced at the interface, since too many hydrogen ions cause instability of the film. Then, the deposition temperature is increased, the water flow is reduced, the hydrogen content in the subsequently deposited zinc oxide layer is reduced, and the stability of the prepared second zinc oxide-based transparent electrode layer is better.
In some embodiments, a method of fabricating a zinc oxide-based transparent electrode photodetector includes the steps of:
s10, obtaining a substrate with a photoelectric detector, wherein the photoelectric detector comprises a blocking semiconductor layer TiO2And a photosensitive semiconductor layer CdS, wherein the barrier semiconductor layer is arranged on one side far away from the substrate;
s20, 8 is multiplied by 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 1X 10 mol/min-3~4×10-3Providing water at a flow rate of mol/min, and depositing on the surface of the barrier semiconductor layer to form a first zinc oxide-based transparent electrode layer under the conditions that the temperature is 300-400 ℃ and the pressure is 6-12 Torr;
s30. with 8 multiplied by 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~1×10-3Providing water at a flow rate of mol/min, and depositing on the surface of the first zinc oxide-based transparent electrode layer to form a second zinc oxide-based transparent electrode layer under the conditions that the temperature is 400-450 ℃ and the pressure is 6-12 Torr.
In some embodiments, the first zinc oxide-based transparent electrode layer has a thickness of 10 to 50 nm. In some embodiments, the second zinc oxide-based transparent electrode layer has a thickness of 90 to 450 nm. According to the embodiment of the invention, the first zinc oxide transparent electrode layer with the thickness of 10-50 nm and the second zinc oxide transparent electrode with the thickness of 90-450 nm can form a hydrogen-rich layer between the semiconductor layer of the photoelectric detector and the zinc oxide layer, so that a hydrogen donor is introduced, the carrier concentration is improved, and the stability of the zinc oxide electrode formed by deposition is ensured.
Correspondingly, the embodiment of the invention also provides a zinc oxide-based transparent electrode photoelectric detector which comprises a photoelectric detector and a zinc oxide-based transparent electrode layer, wherein a hydrogen-rich layer is formed between the photoelectric detector and the zinc oxide-based transparent electrode layer, and the zinc oxide-based transparent electrode layer contains metal doping elements.
The zinc oxide based transparent electrode photoelectric detector provided by the embodiment of the invention can be prepared by the method, and comprises a photoelectric detector, a zinc oxide based transparent electrode layer arranged on one side surface of the photoelectric detector, and a hydrogen-rich layer formed between the photoelectric detector and the zinc oxide based transparent electrode layer, wherein more hydrogen donors are introduced between the photoelectric detector and the zinc oxide layer by the hydrogen-rich layer, and the hydrogen-rich layer has higher carrier concentration on the basis of doping conduction, and the zinc oxide based transparent electrode layer contains metal doping elements, so that the donor carriers of devices are further improved, the resistance is reduced, and the zinc oxide based transparent electrode photoelectric detector has high reliability, low forward working voltage and high light extraction efficiency.
In some embodiments, the photodetector includes a photosensitive semiconductor layer and a blocking semiconductor layer.
In some embodiments, in the zinc oxide-based transparent electrode layer, the mass ratio of the metal doping element to the zinc element is 1% to 10%; and/or,.
In some embodiments, the zinc oxide-based transparent electrode layer has a thickness of 100 to 500 nm.
In some embodiments, the metal doping element is selected from: at least one of aluminum, indium and gallium.
In some embodiments, the barrier semiconductor layer comprises TiO2Doped TiO2NiO, CuO and SnSe.
In some embodiments, the photosensitive semiconductor layer comprises at least one of CdS, ZnO, doped ZnO.
In some embodiments, the thickness of the barrier semiconductor layer is 50 to 500 nm.
In some embodiments, the photosensitive semiconductor layer has a thickness of 20 to 500 nm.
The technical effects of the above embodiments of the present invention are discussed in detail in the foregoing, and are not described herein again.
In order to make the above implementation details and operations of the present invention clearly understood by those skilled in the art, and to make the progress of the zinc oxide-based transparent electrode photodetector and the manufacturing method thereof obviously apparent, the above technical solutions are illustrated by a plurality of examples below.
Example 1
A zinc oxide based transparent electrode photoelectric detector comprises the following preparation steps:
s10, obtaining a transparent conductive glass substrate layer with a photoelectric detector, wherein the photoelectric detector comprises a blocking semiconductor layer TiO2And a photosensitive semiconductor layer CdSThe barrier semiconductor layer is arranged on one side far away from the substrate; carrying out ozone light treatment on the photoelectric detector so as to remove impurities on the surface of the device unit;
s20, flow rate is 8 multiplied by 10-5The diethyl zinc is provided in mol/min at a flow rate of 7X 10-6Supply of trimethylaluminum in a molar/min flow of 1X 10-3Providing deionized water at a temperature of 300 ℃ and a pressure of 6.0Torr in mol/min, and depositing a first zinc oxide-based transparent electrode layer with a thickness of 10 nanometers on the surface of the barrier semiconductor layer;
s30, flow rate is 8 multiplied by 10-5The diethyl zinc is provided in mol/min at a flow rate of 7X 10-6Supply of trimethylaluminum in moles/minute at a flow rate of 7X 10-4Providing deionized water at a mol/min ratio, and depositing on the surface of the first zinc oxide-based transparent electrode layer to form a second zinc oxide-based transparent electrode layer with a thickness of 290 nanometers under the conditions that the temperature is 400 ℃ and the pressure is 6.0 Torr; and obtaining the zinc oxide-based photoelectric detector.
S40, carrying out photoetching process mask on the zinc oxide-based photoelectric detector, and processing the zinc oxide-based photoelectric detector into a size of 2mm multiplied by 2mm to obtain the required photoelectric detection chip.
Further, in order to verify the advancement of the zinc oxide-based transparent electrode photodetector in the embodiment of the invention, the embodiment of the invention performs related tests.
Test example 1
In the test example, a Hall55 measuring instrument is adopted to respectively test the resistivity, the carrier concentration and the carrier mobility of the zinc oxide-based transparent electrode layer prepared in the example 1, wherein the resistivity is 5.5 multiplied by 10-4Omega cm, carrier concentration of 3.26X 1020cm-3Mobility of 28cm2.V-1S-1。
Test example 2
As shown in fig. 2 (wavelength on abscissa and transmittance on ordinate), the transmittance of the zinc oxide-based transparent electrode layer prepared in example 1 on a quartz substrate was tested by the test, and the transmittance was greater than 90% in the visible light range.
Test example 3
As shown in fig. 3 (abscissa 2 θ, ordinate intensity), the XRD diffractogram of the zinc oxide-based transparent electrode layer prepared in example 1 on the sapphire substrate of this test example shows that the photovoltaic chip prepared in example 1 is a polycrystalline thin film with preferred c-axis orientation.
Test example 4
As shown in fig. 4, in the test example, the surface morphology of the zinc oxide-based transparent electrode layer prepared in example 1 is tested by a scanning electron microscope, and it can be seen from fig. 4 that the grain size is 50 to 100 nm.
From the test results, the zinc oxide-based transparent electrode layer prepared in the embodiment 1 of the invention has high transmittance, high conductivity and high crystallization quality.
Test example 5
Further, the present invention tested the photoelectric response of the photodetection chip prepared in example 1.
Under the illumination condition of 100 μ W and 500nm wave band incident light, current under illumination was tested, as shown in FIG. 5 (time on abscissa and current on ordinate), photocurrent was close to 1 μ A, on-off ratio was 103The photoelectric chip prepared by the invention has excellent conductive and transparent characteristics and is also combined with CdS/TiO2TiO of base photoelectric detection chip2Good ohmic contact is formed to promote CdS/TiO2The low-cost application and sustainable development of the base photoelectric detection chip in the field of detectors and image processing.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (10)
1. A preparation method of a zinc oxide based transparent electrode photoelectric detector is characterized by comprising the following steps:
obtaining a substrate on which a photodetector is formed;
and providing a zinc source, a doped metal source and water, and depositing on the surface of one side of the photoelectric detector far away from the substrate at the temperature of 300-450 ℃ to form a zinc oxide-based transparent electrode layer to obtain the zinc oxide-based transparent electrode photoelectric detector.
2. The method of claim 1, wherein the step of providing a zinc source, a doped metal source, and water comprises: at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~4×10-3Providing water at a flow rate of moles/minute; and/or the presence of a gas in the gas,
the pressure for forming the zinc oxide-based transparent electrode layer by deposition is 6-12 Torr; and/or the presence of a gas in the gas,
the photodetector includes a photosensitive semiconductor layer and a blocking semiconductor layer.
3. The method for preparing a zinc oxide-based transparent electrode photodetector according to claim 2, wherein the step of depositing a zinc oxide-based transparent electrode layer on a surface of the photodetector away from the substrate comprises:
at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 1X 10 mol/min-3~4×10-3Providing water at a flow rate of mol/min, and depositing on the surface of one side of the photoelectric detector, which is far away from the substrate, to form a first zinc oxide-based transparent electrode layer under the conditions that the temperature is 300-400 ℃ and the pressure is 6-12 Torr;
at 8X 10-5~4×10-4The zinc source was supplied at a flow rate of 7X 10 mol/min-6~4×10-5The dopant metal source was supplied at a flow rate of 7X 10 mol/min-4~1×10-3Providing water at a flow rate of mol/min, and depositing on the surface of the first zinc oxide-based transparent electrode layer to form a second zinc oxide-based transparent electrode layer under the conditions that the temperature is 400-450 ℃ and the pressure is 6-12 Torr.
4. The method of claim 3, wherein the blocking semiconductor layer comprises: TiO 22Doped TiO 22At least one of NiO, CuO and SnSe; and/or the presence of a gas in the gas,
the photosensitive semiconductor layer includes: at least one of CdS, ZnO and doped ZnO; and/or the presence of a gas in the gas,
the thickness of the barrier semiconductor layer is 50-500 nm; and/or the presence of a gas in the gas,
the thickness of the photosensitive semiconductor layer is 20-500 nm.
5. The method of claim 4, wherein the zinc source is selected from the group consisting of: at least one of diethyl zinc and trimethyl zinc; and/or the presence of a gas in the gas,
the doped metal source is selected from: at least one of aluminum source, indium source and gallium source.
6. The method of claim 5, wherein the aluminum source is selected from the group consisting of trimethylaluminum; and/or the presence of a gas in the gas,
the indium source is selected from trimethyl indium; and/or the presence of a gas in the gas,
the gallium source is selected from triethyl gallium.
7. The method for manufacturing a zinc oxide-based transparent electrode photodetector as claimed in any one of claims 3 to 6, wherein the mass ratio of the doped metal element to the zinc element in the zinc oxide-based transparent electrode layer is 1% to 10%; and/or the presence of a gas in the gas,
the thickness of the first zinc oxide-based transparent electrode layer is 10-50 nm; and/or the presence of a gas in the gas,
the thickness of the second zinc oxide-based transparent electrode layer is 90-450 nm; and/or the presence of a gas in the gas,
the thickness of the zinc oxide-based transparent electrode layer is 100-500 nm.
8. The photoelectric detector is characterized by comprising a photoelectric detector and a zinc oxide-based transparent electrode layer, wherein a hydrogen-rich layer is formed between the photoelectric detector and the zinc oxide-based transparent electrode layer, and the zinc oxide-based transparent electrode layer contains metal doping elements.
9. The zinc oxide-based transparent electrode photodetector of claim 8, wherein the photodetector comprises a photosensitive semiconductor layer and a blocking semiconductor layer; and/or the presence of a gas in the gas,
in the zinc oxide-based transparent electrode layer, the mass ratio of the metal doping element to the zinc element is 1-10%; and/or the presence of a gas in the gas,
the thickness of the zinc oxide-based transparent electrode layer is 100-500 nm; and/or the presence of a gas in the gas,
the metal doping element is selected from: at least one of aluminum, indium and gallium.
10. The zinc oxide-based transparent electrode photodetector of claim 9, wherein the blocking semiconductor layer comprises TiO2Doped TiO2At least one of NiO, CuO and SnSe; and/or the presence of a gas in the gas,
the photosensitive semiconductor layer comprises at least one of CdS, ZnO and doped ZnO; and/or the presence of a gas in the gas,
the thickness of the barrier semiconductor layer is 50-500 nm; and/or the presence of a gas in the gas,
the thickness of the photosensitive semiconductor layer is 20-500 nm.
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