CN111384197B - Defect-state graphene/semiconductor heterojunction photoelectric detector - Google Patents
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- 238000006722 reduction reaction Methods 0.000 claims description 6
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 5
- XMBWDFGMSWQBCA-UHFFFAOYSA-N hydrogen iodide Chemical compound I XMBWDFGMSWQBCA-UHFFFAOYSA-N 0.000 claims description 4
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- 229910052732 germanium Inorganic materials 0.000 claims description 3
- YBNMDCCMCLUHBL-UHFFFAOYSA-N (2,5-dioxopyrrolidin-1-yl) 4-pyren-1-ylbutanoate Chemical compound C=1C=C(C2=C34)C=CC3=CC=CC4=CC=C2C=1CCCC(=O)ON1C(=O)CCC1=O YBNMDCCMCLUHBL-UHFFFAOYSA-N 0.000 claims description 2
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- 229910001218 Gallium arsenide Inorganic materials 0.000 claims description 2
- -1 HgSe Inorganic materials 0.000 claims description 2
- 229910004262 HgTe Inorganic materials 0.000 claims description 2
- 229910000673 Indium arsenide Inorganic materials 0.000 claims description 2
- GPXJNWSHGFTCBW-UHFFFAOYSA-N Indium phosphide Chemical compound [In]#P GPXJNWSHGFTCBW-UHFFFAOYSA-N 0.000 claims description 2
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- UHYPYGJEEGLRJD-UHFFFAOYSA-N cadmium(2+);selenium(2-) Chemical compound [Se-2].[Cd+2] UHYPYGJEEGLRJD-UHFFFAOYSA-N 0.000 claims description 2
- 239000003638 chemical reducing agent Substances 0.000 claims description 2
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- SBIBMFFZSBJNJF-UHFFFAOYSA-N selenium;zinc Chemical compound [Se]=[Zn] SBIBMFFZSBJNJF-UHFFFAOYSA-N 0.000 claims description 2
- OCGWQDWYSQAFTO-UHFFFAOYSA-N tellanylidenelead Chemical compound [Pb]=[Te] OCGWQDWYSQAFTO-UHFFFAOYSA-N 0.000 claims description 2
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- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 13
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- 229910010271 silicon carbide Inorganic materials 0.000 description 1
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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
- H01L31/08—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 in which radiation controls flow of current through the device, e.g. photoresistors
- H01L31/10—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 in which radiation controls flow of current through the device, e.g. photoresistors characterised by at least one potential-jump barrier or surface barrier, e.g. phototransistors
- H01L31/101—Devices sensitive to infrared, visible or ultraviolet radiation
- H01L31/102—Devices sensitive to infrared, visible or ultraviolet radiation characterised by only one potential barrier or surface barrier
- H01L31/109—Devices sensitive to infrared, visible or ultraviolet radiation characterised by only one potential barrier or surface barrier the potential barrier being of the PN heterojunction type
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/184—Preparation
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
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- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/194—After-treatment
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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
- H01L31/0328—Inorganic materials including, apart from doping materials or other impurities, semiconductor materials provided for in two or more of groups H01L31/0272 - H01L31/032
- H01L31/0336—Inorganic materials including, apart from doping materials or other impurities, semiconductor materials provided for in two or more of groups H01L31/0272 - H01L31/032 in different semiconductor regions, e.g. Cu2X/CdX hetero-junctions, X being an element of Group VI of the Periodic System
Abstract
The invention discloses a defect state graphene/semiconductor heterojunction photoelectric detector which has a two-layer structure, wherein one layer is a semiconductor layer, the other layer is a defect state graphene layer, and the defect state graphene layer is attached to the semiconductor layer; the thickness of the defect state graphene layer is 10-100nm, and the defect state graphene layer contains defect state sp3/sp2The carbon content ratio is 1-40%. According to the invention, the film is prepared by adopting a suction filtration method, so that the uniformity of the film and the stability of a device are ensured; by controlling the sintering process, the defect state graphene film is prepared, the defect state is introduced into the heterojunction, electrons are scattered to phonons, the heat effect is caused, and the photoresponse is further improved. Compared with a non-defect-state graphene/semiconductor heterojunction photoelectric detector, the defect state is introduced, and the external quantum efficiency magnitude is improved.
Description
Technical Field
The invention belongs to the technical field of photoelectric detectors, and particularly relates to a defect-state graphene/semiconductor heterojunction photoelectric detector.
Background
With the development of the technology, the photoelectric detection range is widened from visible light to ultraviolet, infrared and X rays, even terahertz wave bands, and the photoelectric detection device plays a vital role in national economy and even national defense and military. However, in the development process of the observation photoelectric detector, the search for the high-response, room-temperature wide-band photoelectric detector is still an important research direction. The defect state graphene/semiconductor heterojunction photoelectric detector is one of the defects, a heterojunction is constructed by applying different work functions of graphene (4.5eV) and a semiconductor, when light irradiates the heterojunction, the defect state graphene absorbs the light, photon energy jumps to generate a photon-generated carrier, and the photon-generated carrier is transmitted to a heterojunction interface under the action of an external bias voltage to realize photoelectric conversion.
However, the conventional graphene/semiconductor heterojunction photoelectric detector uses single-layer graphene or few-layer mechanically-exfoliated graphene as a metal material, and has the following problems that firstly, the graphene is low in thickness and too low in light absorption rate; secondly, the area of the few-layer graphene is too small, so that the few-layer graphene is not suitable for mass preparation.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a defect-state graphene/semiconductor heterojunction photoelectric detector. By designing the nano-scale graphene film, the light absorption is increased, and the various problems of the conventional graphene are solved. And sintering to obtain nano-scale graphene films with different defect state contents, and introducing defect states to increase electron scattering to phonons, so as to cause a thermal effect and improve photoresponse.
The purpose of the invention is realized by the following technical scheme: a defect state graphene/semiconductor heterojunction photoelectric detector is provided, and the photoelectric detector has a two-layer structure, wherein one layer is a semiconductor layer, the other layer is a defect state graphene layer, and the defect state graphene layer is attached to the semiconductor layer; the thickness of the defect state graphene layer is 10-100nm, and the defect state graphene layer contains defect state sp3/sp2The carbon content ratio is 1-40%. The defect-state graphene layer is prepared by the following method:
(1) carrying out suction filtration on an AAO substrate to obtain a graphene oxide film with a nano thickness, wherein the graphene oxide film is loaded on the AAO substrate;
(2) chemically reducing the AAO substrate loaded with the graphene oxide film at 60-120 ℃ for 6-12h to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate carrying the reduced graphene oxide film through camphor at the temperature of 120-200 ℃, and removing the camphor at the temperature of 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at the temperature of 1600-2000 ℃ for 1min-8h to prepare the defect-state nano-thickness graphene film.
Further, the chemical reduction method in step 2 is hydroiodic acid reduction.
Further, the semiconductor may be Si, Ge, SiC, AlN, AlP, AlAs, AlSb, GaN, GaP, GaAs, GaSb, InN, InP, InAs, InSb, ZnO, ZnS, ZnSe, ZnTe, CdS, CdSe, CdTe, HgSe, HgTe, PbS, PbSe, PbTe, or the like.
The invention has the beneficial effects that: according to the invention, the graphene oxide film is prepared by a suction filtration method, so that the uniformity of the graphene oxide film and the stability of a device are ensured; by controlling the sintering process, the defect state graphene film is prepared, the defect state is introduced into the heterojunction, electrons are scattered to phonons, the heat effect is caused, and the photoresponse is further improved. Compared with a non-defect-state graphene/semiconductor heterojunction photoelectric detector, the defect state is introduced, and the external quantum efficiency is improved in magnitude. In addition, compared with few-layer graphene, the thin film prepared by the method is large in size and higher in operability.
Drawings
Fig. 1 is a current-voltage curve of a graphene/silicon heterojunction photodetector prepared in example 1 for 1600-1 min (defect 40%).
Fig. 2 is a current-voltage curve of a graphene/silicon heterojunction photodetector prepared in example 2 for 1600-30 min (defect 20%).
Fig. 3 is a current-voltage curve of a graphene/silicon heterojunction photodetector manufactured in example 3 for 1600-8 h (defect 10%).
FIG. 4 is a graph of current-voltage curves for the 2800-2h (defect free) graphene/silicon heterojunction photodetector made in example 4.
Detailed Description
The objects and effects of the present invention will become more apparent by describing the contents of the present invention in further detail with reference to the accompanying drawings. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
Example 1
(1) Diluting a graphene oxide solution, and performing suction filtration on an AAO substrate to obtain a graphene oxide film, wherein the graphene oxide film is loaded on the AAO substrate;
(2) carrying out hydriodic acid reduction on the AAO substrate loaded with the graphene oxide film at 60 ℃ for 12h to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate supporting the reduced graphene oxide film through camphor at 120 ℃ and removing the camphor at 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 1600 ℃ for 1min to prepare the defect-state graphene film with the thickness of 40 nm.
XPS detects and calculates that the defect state graphene film contains defect state sp3/sp2The carbon content ratio was 40%.
The defect-state graphene film is attached to a silicon wafer to prepare a photoelectric device, and a current-voltage curve at a wavelength of 4um is measured, as shown in fig. 1. Calculating the responsivity and the external quantum efficiency according to the measurement result to obtain the responsivity of 7.41 multiplied by 10 when the 4um laser power is 71mw-5A/W, external quantum efficiency of 2.30X 10-5。
Example 2:
(1) diluting a graphene oxide solution, and performing suction filtration on an AAO substrate to obtain a graphene oxide film, wherein the graphene oxide film is loaded on the AAO substrate;
(2) carrying out hydriodic acid reduction on the AAO substrate loaded with the graphene oxide film at 120 ℃ for 8h to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate supporting the reduced graphene oxide film through camphor at 200 ℃ and removing the camphor at 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 1600 ℃ for 30min to prepare the defect-state graphene film with the thickness of 40 nm.
XPS detection is carried out to calculate that the defect state graphene film contains defect state sp3/sp2The carbon content ratio was 20%.
Attaching the defect state graphene film and a silicon wafer to prepare a photoelectric device, and measuring current-electricity at a wavelength of 4umPressure curve, as shown in fig. 2. And calculating the responsivity and the external quantum efficiency according to the measurement result. The responsivity is 5.01 multiplied by 10 when the laser power of 4um is 71mw-5A/W, external quantum efficiency of 1.57X 10-6。
Example 3:
(1) diluting a graphene oxide solution, and performing suction filtration on an AAO substrate to obtain a graphene oxide film, wherein the graphene oxide film is loaded on the AAO substrate;
(2) chemically reducing the AAO substrate loaded with the graphene oxide film at 120 ℃ for 12h to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate supporting the reduced graphene oxide film through camphor at 200 ℃ and removing the camphor at 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 1600 ℃ for 8h to prepare the defect-state graphene film with the thickness of 40 nm.
XPS detection is carried out to calculate that the defect state graphene film contains defect state sp3/sp2The carbon content ratio was 10%.
And (3) attaching the defect state graphene film and a silicon wafer to prepare a photoelectric device, and measuring a current-voltage curve under the wavelength of 4um, as shown in figure 3. Calculating the responsivity and the external quantum efficiency according to the measurement result to obtain the responsivity of 7.79 multiplied by 10 when the laser power of 4um is 71mw-5A/W, external quantum efficiency of 2.42X 10-5。
Comparative example
(1) Diluting a graphene oxide solution, and performing suction filtration on an AAO substrate to obtain a graphene oxide film, wherein the graphene oxide film is loaded on the AAO substrate;
(2) chemically reducing the AAO substrate loaded with the graphene oxide film at 120 ℃ for 12h to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate supporting the reduced graphene oxide film through camphor at 200 ℃ and removing the camphor at 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 2800 ℃ for 2h to prepare the 40nm graphene film.
XPS detection is carried out, and defect sp state contained in the graphene film is calculated3/sp2The carbon content ratio was 0.
And (3) attaching the defect state graphene film and a silicon wafer to prepare a photoelectric device, and measuring a current-voltage curve under the wavelength of 4um, as shown in figure 4. Calculating the responsivity and the external quantum efficiency according to the measurement result to obtain the responsivity of 2.60 multiplied by 10 when the laser power of 4um is 71mw-6A/W, external quantum efficiency of 8.06X 10-7。
The current-voltage curve of the defect-state graphene/silicon heterojunction photodetector determined in the examples 1 to 3 and the current-voltage curve of the comparative defect-free graphene/silicon heterojunction photodetector are calculated and compared with corresponding external quantum efficiencies, and the results are as follows: table 1 shows that as the laser power decreases, the external quantum efficiency of the graphene/silicon heterojunction photodetector decreases; for the laser power under the same power, the external quantum efficiency of the defective graphene/silicon heterojunction photoelectric detector is higher than that of the defect-free graphene/silicon heterojunction photoelectric detector. Therefore, the external quantum efficiency of the photoelectric device prepared by taking the defect-state graphene film as the two-dimensional material is higher than that of the photoelectric device prepared by taking the defect-state graphene film as the two-dimensional material.
TABLE 1 external Quantum efficiency of optoelectronic devices at different powers (different defect states graphene films)
Example 4
(1) Diluting a graphene oxide solution, and performing suction filtration on an AAO substrate to obtain a graphene oxide film, wherein the graphene oxide film is loaded on the AAO substrate;
(2) chemically reducing the AAO substrate loaded with the graphene oxide film at 120 ℃ for 10 hours to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate supporting the reduced graphene oxide film through camphor at 200 ℃ and removing the camphor at 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 2000 ℃ for 8h to prepare the 10nm defect state graphene film.
XPS detection is carried out, and defect sp state contained in the defect state graphene film is calculated3/sp2The carbon content ratio was 1%.
And attaching the defect state graphene film and a germanium sheet to prepare a photoelectric device, measuring a current-voltage curve under the wavelength of 4um, and calculating the responsivity and the external quantum efficiency according to the measurement result to obtain the responsivity of 0.0037A/W when the laser power of 4um is 5 mw.
Example 5
(1) Diluting a graphene oxide solution, and performing suction filtration on an AAO substrate to obtain a graphene oxide film, wherein the graphene oxide film is loaded on the AAO substrate;
(2) chemically reducing the AAO substrate loaded with the graphene oxide film at 120 ℃ for 6 hours to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate supporting the reduced graphene oxide film through camphor at 200 ℃ and removing the camphor at 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 1600 ℃ for 8h to prepare the 100nm defect state graphene film.
XPS detection is carried out, and defect sp state contained in the defect state graphene film is calculated3/sp2The carbon content ratio was 10%.
And (3) attaching the defect state graphene film and zinc oxide to prepare a photoelectric device, measuring a current-voltage curve under the wavelength of 4um, and calculating the responsivity and the external quantum efficiency according to the measurement result to obtain the responsivity of 0.00499A/W when the laser power of 4um is 20 mw.
Claims (3)
1. Defect-state graphene/semiconductor heterojunction photoelectric detectorThe photoelectric detector is characterized by having a two-layer structure, wherein one layer is a semiconductor layer, the other layer is a defect state graphene layer, and the defect state graphene layer is attached to the semiconductor layer; the thickness of the defect state graphene layer is 10-100nm, and the defect state graphene layer contains defect state sp3/sp2The carbon content ratio is 1-40%; the defect-state graphene layer is prepared by the following method:
(1) carrying out suction filtration on an AAO substrate to obtain a graphene oxide film with a nano thickness, wherein the graphene oxide film is loaded on the AAO substrate;
(2) chemically reducing the AAO substrate loaded with the graphene oxide film at 60-120 ℃ for 6-12h to obtain the AAO substrate loaded with the reduced graphene oxide film;
(3) peeling the AAO substrate carrying the reduced graphene oxide film through camphor at the temperature of 120-200 ℃, and removing the camphor at the temperature of 60 ℃; obtaining a reduced graphene oxide film;
(4) and (4) sintering the reduced graphene oxide film obtained in the step (3) at 1600-2000 ℃ for 1min-8h to prepare the defect-state nano-thickness graphene film.
2. The defect-state graphene/semiconductor heterojunction photodetector of claim 1, wherein the chemical reduction method in the step (2) is hydroiodic acid reduction.
3. The defective graphene/semiconductor heterojunction photodetector of claim 1, wherein the semiconductor is Si, Ge, SiC, AlN, AlP, AlAs, AlSb, GaN, GaP, GaAs, GaSb, InN, InP, InAs, InSb, ZnO, ZnS, ZnSe, ZnTe, CdS, CdSe, CdTe, HgSe, HgTe, PbS, PbSe, or PbTe.
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