CN103579419A - Grapheme/MoS2/Si heterojunction thin-film solar cell and manufacturing method thereof - Google Patents
Grapheme/MoS2/Si heterojunction thin-film solar cell and manufacturing method thereof Download PDFInfo
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- 239000010409 thin film Substances 0.000 title claims abstract description 8
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical compound S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 title abstract description 15
- 229910052961 molybdenite Inorganic materials 0.000 title abstract description 6
- 229910052982 molybdenum disulfide Inorganic materials 0.000 title abstract description 6
- 238000004519 manufacturing process Methods 0.000 title abstract description 3
- 239000010408 film Substances 0.000 claims abstract description 54
- 230000000694 effects Effects 0.000 claims abstract description 20
- 239000007789 gas Substances 0.000 claims abstract description 15
- 238000000034 method Methods 0.000 claims abstract description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 59
- 229910021389 graphene Inorganic materials 0.000 claims description 57
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 27
- 235000012239 silicon dioxide Nutrition 0.000 claims description 24
- 239000003708 ampul Substances 0.000 claims description 21
- 239000010453 quartz Substances 0.000 claims description 21
- 229910052710 silicon Inorganic materials 0.000 claims description 20
- 239000010703 silicon Substances 0.000 claims description 20
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 19
- 239000000758 substrate Substances 0.000 claims description 14
- 229910052799 carbon Inorganic materials 0.000 claims description 13
- 150000001721 carbon Chemical group 0.000 claims description 13
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 12
- 239000000126 substance Substances 0.000 claims description 12
- 238000002360 preparation method Methods 0.000 claims description 11
- 230000008569 process Effects 0.000 claims description 11
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 8
- 238000000137 annealing Methods 0.000 claims description 7
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 6
- 229910052786 argon Inorganic materials 0.000 claims description 6
- 230000006911 nucleation Effects 0.000 claims description 6
- 238000010899 nucleation Methods 0.000 claims description 6
- 230000015572 biosynthetic process Effects 0.000 claims description 4
- 239000002253 acid Substances 0.000 claims description 3
- 238000000637 aluminium metallisation Methods 0.000 claims description 3
- 239000008367 deionised water Substances 0.000 claims description 3
- 229910021641 deionized water Inorganic materials 0.000 claims description 3
- 239000002019 doping agent Substances 0.000 claims description 3
- 229910052739 hydrogen Inorganic materials 0.000 claims description 3
- 239000001257 hydrogen Substances 0.000 claims description 3
- 230000005012 migration Effects 0.000 claims description 3
- 238000013508 migration Methods 0.000 claims description 3
- 229910052757 nitrogen Inorganic materials 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 239000002904 solvent Substances 0.000 claims description 3
- 238000004506 ultrasonic cleaning Methods 0.000 claims description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 3
- 238000000354 decomposition reaction Methods 0.000 claims description 2
- 238000005137 deposition process Methods 0.000 claims description 2
- 125000004435 hydrogen atom Chemical class [H]* 0.000 claims description 2
- 238000006243 chemical reaction Methods 0.000 abstract description 15
- 238000005286 illumination Methods 0.000 abstract description 6
- 238000005229 chemical vapour deposition Methods 0.000 abstract description 5
- 230000004044 response Effects 0.000 abstract description 4
- 239000007791 liquid phase Substances 0.000 abstract description 2
- 239000010410 layer Substances 0.000 description 29
- 238000000151 deposition Methods 0.000 description 11
- 238000010521 absorption reaction Methods 0.000 description 8
- 239000007792 gaseous phase Substances 0.000 description 7
- 238000010586 diagram Methods 0.000 description 5
- 239000004065 semiconductor Substances 0.000 description 5
- 230000005355 Hall effect Effects 0.000 description 4
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 4
- 238000001237 Raman spectrum Methods 0.000 description 4
- 238000000862 absorption spectrum Methods 0.000 description 4
- 238000009825 accumulation Methods 0.000 description 4
- 230000005540 biological transmission Effects 0.000 description 4
- 239000013078 crystal Substances 0.000 description 4
- 230000008021 deposition Effects 0.000 description 4
- 239000012528 membrane Substances 0.000 description 4
- 229910052750 molybdenum Inorganic materials 0.000 description 4
- 239000011733 molybdenum Substances 0.000 description 4
- 230000005855 radiation Effects 0.000 description 4
- 238000001069 Raman spectroscopy Methods 0.000 description 3
- 230000005684 electric field Effects 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 230000031700 light absorption Effects 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000001228 spectrum Methods 0.000 description 3
- 238000012876 topography Methods 0.000 description 3
- 238000000411 transmission spectrum Methods 0.000 description 3
- 101100069231 Caenorhabditis elegans gkow-1 gene Proteins 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 125000004429 atom Chemical group 0.000 description 2
- 238000004630 atomic force microscopy Methods 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 230000001413 cellular effect Effects 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 230000003287 optical effect Effects 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 230000005622 photoelectricity Effects 0.000 description 2
- 230000000630 rising effect Effects 0.000 description 2
- 230000009466 transformation Effects 0.000 description 2
- 230000007704 transition Effects 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- 239000011358 absorbing material Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 229910021417 amorphous silicon Inorganic materials 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
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- 238000011065 in-situ storage Methods 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 239000011229 interlayer Substances 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 239000002932 luster Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910021421 monocrystalline silicon Inorganic materials 0.000 description 1
- 230000005693 optoelectronics Effects 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
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- 238000005424 photoluminescence Methods 0.000 description 1
- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 1
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Images
Classifications
-
- 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
-
- 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
- C23C16/305—Sulfides, selenides, or tellurides
-
- 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
- C23C16/44—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
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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
- H01L31/04—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 adapted as photovoltaic [PV] conversion devices
- H01L31/06—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 adapted as photovoltaic [PV] conversion devices characterised by at least one potential-jump barrier or surface barrier
- H01L31/072—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 adapted as photovoltaic [PV] conversion devices characterised by at least one potential-jump barrier or surface barrier the potential barriers being only of the PN heterojunction type
- H01L31/074—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 adapted as photovoltaic [PV] conversion devices characterised by at least one potential-jump barrier or surface barrier the potential barriers being only of the PN heterojunction type comprising a heterojunction with an element of Group IV of the Periodic System, e.g. ITO/Si, GaAs/Si or CdTe/Si solar cells
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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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
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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
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- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The invention relates to a grapheme/MoS2/Si heterojunction thin-film solar cell and a manufacturing method thereof. A chemical vapor deposition method that gases carry liquid phase MoS2 molecules is adopted, the flow and the response speed can be well controlled, and an MoS2 thin film which is ultra-thin, even in large area, smooth in surface and small in roughness is obtained. Interface special shapes of a p-MoS2/n-Si heterojunction are effectively reduced, leak currents are reduced, and the photoelectric conversion efficiency of the solar cell is improved. The grapheme film which is even in large area and good in transparency and electric conductivity and obtained with the chemical vapor deposition method is used as a transparent electric conduction electrode. The MoS2-Si heterojunction has strong collecting function on photoproduction electrons and holes, and the photovoltaic effect and the conversion efficiency of the solar cell are improved. The solar cell has the open-circuit voltage of 0.98V, the short-circuit currents of 4.6mA and the light energy conversion efficiency of 4.5% under 100mW white light illumination.
Description
Technical field
The present invention relates to a kind of solar cell, particularly a kind of Graphene/MoS
2/ Si heterojunction solar battery and preparation method thereof.
Background technology
MoS
2, being called again brightness molybdenum, the black solid material of metal luster under normal temperature, has excellent chemical stability, thermal stability (1185 ℃ of fusing points) and lubrification, is generally used for face coat or the lubricant of machinery, cutting tools.In structure, brightness molybdenum is the graphite laminate structure of hexagonal closs packing, and layer combines with the van der waals force of interlayer by weak interaction.Easily peel off as the Graphene of monoatomic layer similarly to graphite, by micromechanics, peeling off brightness molybdenum also easily becomes individual layer MoS
2film [S. Bertolazzi, J. Brivio, A. Kis, Stretching and Breaking of Ultrathin MoS
2, ACS Nano, V. 5 (12): 9703-9709,2011.].Individual layer MoS2 is the regular hexagon planar structure that S-Mo-S tri-atom covalence bonds are closed, and thickness is only 0.65nm.
Block MoS
2for indirect band gap (1.2eV) semiconductor, due to quantum confined effect, individual layer MoS
2change direct band gap (1.8eV) [K. F. Mak, C.Lee, J. Hone, J. Shan, T. F. Heinz, Atomically thin MoS into
2: a new direct-gap semiconductor. Phys. Rev. Lett. V.105:136805-08,2010].By indirect band gap transitions, be direct band gap, photon transition gain can improve~and 10
4, make individual layer MoS
2visible ray (300-700 nm) is had to catch light absorptivity and light emission effciency [G. Eda, H. Yamaguchi, D. Voiry, T. Fujita, M. Chen, M. Chhowalla, Correction to Photoluminescence from Chemically Exfoliated MoS
2, Nano Lett.V. 12 (1), 526 – 526,2012.].
Silicon solar cell (monocrystalline silicon, polysilicon, amorphous silicon) occupies more than 90% market share with advantages such as mature preparation process, life-span length always.But Si is indirect gap semiconductor, efficiency of light absorption is very low, makes the conversion efficiency of commercialization silicon solar cell generally lower than 20%.Lower conversion efficiency and higher cost have become the bottleneck of solar cell, have seriously limited the development of photovoltaic industry.We know, the conversion efficiency of solar cell is determined by semi-conductive photovoltaic effect.Therefore, find and there is remarkable photovoltaic effect, low-cost solar battery material, realize the main direction that high conversion efficiency has become current solar cell research field.
Si is indirect gap semiconductor, and efficiency of light absorption is very low, and in addition, the absorption peak wavelength of silicon is 930 nm, and the radiation of near infrared band has good absorption, and to the visible absorption of 300-700 nanometer relatively a little less than.Make the conversion efficiency of silicon solar cell lower.Individual layer MoS
2at 400~700nm visible light wave range, have very strong absorption, its absorption spectra has just in time formed mutual supplement with each other's advantages with Si absorption spectra, has covered whole visible ray and near infrared band.If by individual layer MoS
2contact with Si, form MoS
2/ Si heterojunction greatly enhance device, in the absorption of visible light-wave band, significantly improves device photovoltaic effect and photoelectric conversion efficiency, prepares high efficiency MoS
2/ Si heterojunction solar battery.
Graphene is that a kind of by carbon atom, to take thickness that the tight storehouse of hexagon cellular forms be only individual layer two dimension (2D) cellular crystal of 0.35 nm.Graphene is to be known as in the world the material the thinnest, the hardest, conduction electron is fastest.Its carrier mobility is up to 2 * 10
5cm
2/ v is higher 100 times than electron mobility in silicon.Graphene also has good optical property, and transmission of visible light, up to 98.5%, can be used for nesa coating and solar cell.Therefore, at MoS
2in/Si heterojunction solar battery, Graphene can be used as transparent conductive film.
Summary of the invention
The object of the invention is to overcome the deficiency that prior art exists, a kind of Graphene/MoS that can effectively improve photoelectric conversion efficiency is provided
2/ Si heterojunction solar battery and preparation method thereof.
The technical scheme that realizes the object of the invention is to provide a kind of Graphene/MoS
2the preparation method of/Si hetero-junction thin-film solar cell, comprises the steps:
(1) substrate cleans: with
n-Si (111) sheet is substrate, removes the silicon dioxide on Si surface, then use successively acetone, ethanol, deionized water Ultrasonic Cleaning by rare HF acid soak, removes the organic substance on silicon chip, with nitrogen, dries up, and puts into quartz ampoule and carries out deposition processes; The vacuum degree of quartz ampoule is 10
-2pa, is heated to 300 ℃ and maintains 10 minutes, to remove the steam of silicon chip surface;
(2) MoS
2film preparation: quartz ampoule is heated to 500~600 ℃, take as carrying gas, passing into the MoS that dilute sulfuric acid is solvent with argon gas
2solution, at described MoS
2in solution, add Al (NO
3)
3solution, with Al (NO
3)
3as Al dopant to MoS
2carry out p-type doping, in mass ratio, MoS
2:al (NO
3)
3for 1:20~1:50; Gas carries MoS
2and Al (NO
3)
3entering quartz ampoule exists
n-Si (111) sheet adsorbs, nucleation and growth be after 5~10 minutes, quartz ampoule is warmed up to 950 ℃ and carries out annealing in process, and annealing time is 20~40 minutes, obtains MoS
2/ Si pn knot;
(3) quartz ampoule temperature is maintained to 950 ℃, methane decomposition is carbon atom and hydrogen, and under the vapor transportation effect of argon gas 10~30 sccm flows, carbon atom arrives established MoS
2the MoS of/Si pn knot
2surface is also adsorbed to surface, in substrate surface nucleation, then attracts other carbon atom by Van der Waals attraction, and form the cancellated graphene film of hexagonal with the carbon atom of Cheng Jian after substrate surface migration;
(4) right
nthe lower surface AM aluminum metallization electrode of-Si (111) sheet, the negative electrode of formation solar cell, obtains a kind of Graphene/MoS
2/ Si heterojunction solar battery.
Technical solution of the present invention also comprises the Graphene/MoS preparing as stated above
2/ Si hetero-junction thin-film solar cell.
The beneficial effect of technical solution of the present invention: owing to having adopted gas to carry liquid phase MoS
2the chemical gaseous phase depositing process of molecule, can better control flow and reaction speed, obtains ultra-thin, Large-Area-Uniform, MoS that surfacing roughness is very little
2film, thus can effectively reduce p-MoS
2the interface special type of/n-Si heterojunction, reduces leakage current, improves the photoelectric conversion efficiency of solar cell.Meanwhile, utilize chemical gaseous phase depositing process can obtain the good graphene film of Large-Area-Uniform, the transparency and conductivity.
Accompanying drawing explanation
Fig. 1 is Graphene/p-MoS that the embodiment of the present invention provides
2the structural representation of/n-Si heterojunction solar battery;
Fig. 2 is Graphene/MoS that the embodiment of the present invention provides
2the band structure schematic diagram of/Si heterojunction solar battery;
Fig. 3 is Graphene/MoS that the embodiment of the present invention provides
2the operation principle of/Si heterojunction solar battery;
Fig. 4 is the MoS that the embodiment of the present invention provides
2film adopts the structural representation of chemical gas-phase deposition system device;
Fig. 5, Fig. 6 and Fig. 7 are respectively the MoS that the embodiment of the present invention utilizes chemical gaseous phase depositing process to prepare
2the surface topography of film, x-ray diffraction pattern and Raman spectrogram;
Fig. 8 is the MoS that the embodiment of the present invention utilizes chemical gaseous phase depositing process to prepare
2the light absorption spectrogram of film;
Fig. 9 is the MoS that the embodiment of the present invention provides
2moS in/Si heterojunction
2the current-voltage characteristic curve diagram of film surface;
Figure 10, Figure 11 and Figure 12 are respectively surface atom force microscope photo, Raman spectrum and the ultraviolet-visible light transmission spectrums of the graphene film that provides of the embodiment of the present invention;
Figure 13 is Graphene/MoS that the embodiment of the present invention provides
2dark current-voltage characteristic curve chart of the unglazed photograph of/Si heterojunction solar battery;
Figure 14 is Graphene/MoS that the embodiment of the present invention provides under 100mW white light
2the voltage-to-current characteristic curve diagram of/Si solar cell;
Figure 15 is Graphene/MoS that the embodiment of the present invention provides under 100mW white light
2the response curve of/Si solar cell;
In figure, 1, Graphene electrodes; 2, p-MoS
2thin layer; 3, n-Si conductive layer; 4, Al electrode.
Embodiment
Below in conjunction with drawings and Examples, technical solution of the present invention is further elaborated.
Referring to accompanying drawing 1, it is Graphene/MoS that the present embodiment provides
2the structural representation of/Si heterojunction solar battery, it comprises Graphene electrodes 1, p-MoS
2 thin layer 2, n-Si layer 3 and Al electrode 4; In Fig. 1, the anode that Graphene electrodes is this solar cell, p-MoS
2the pn forming with n-Si layer becomes the core cell that this solar cell photoelectric is changed, the negative electrode that Al electrode is this solar cell.
Utilize chemical gaseous phase depositing process at the upper grow ultra-thin MoS of n-type silicon chip (111)
2film (several atomic layer), and in its growth course, utilize Al atom to adulterate to make its conduction type become P type, contact with n-type silicon chip substrate and form p-n junction.At p-type MoS
2the graphene film of 10~20 atomic layers thick of film surface recycling chemical gaseous phase depositing process growth, this layer graphene film and MoS
2the common formation of/Si pn knot Graphene/p-MoS
2/ n-Si heterojunction solar battery.
Referring to accompanying drawing 2, it is MoS
2the band structure schematic diagram of/Si pn joint solar cell; Fig. 2 (a) the right and left is respectively MoS
2band structure before contacting with Si.Wherein,
e 0 for vacuum level,
w m for MoS
2work function,
f fm for MoS
2fermi level,
e cm ,
e vm , E
gmrespectively MoS
2conduction band, valence-band level and band gap, χ
m for MoS
2electron affinity.
w s for the work function of Si,
e cs ,
e vs ,
e gs respectively conduction band, valence-band level and the band gap of Si, χ
s for the electron affinity of Si,
f fs fermi level for Si.Δ E
c, Δ E
vrespectively MoS
2with the conduction band of Si and the energy level difference of valence band.
MoS
2work function
w m =
e 0-
e fm =4.6 eV, silicon chip work function
w s =
e 0-
e fs =χ+[
e c -
e fs ], for Si, χ=4.05 eV.
e c -
e fs depend on carrier concentration and doping type in silicon chip.The band gap of Si
e g be 1.12 eV, therefore,
n-Si,
w m >
w s . due to MoS
2work function be greater than the work function of Si,
w m >
w s , after the two contact, as shown in Fig. 2 (b), the hole on Si sheet surface will be to MoS
2one side flow, Si sheet surface leaves Immobile anion (positive center), forms space charge layer.Because the electronics of n side moves to MoS
2one side, makes
n-Si sheet surface forms electronics and piles up, and forms positive potential, makes conduction band
e cs , valence band
e vs end points is bent upwards, as Fig. 2 (b).
qV d for MoS
2the barrier height of-Si heterojunction.MoS
2with
p-type silicon face forms p-n junction, forms MoS
2/ Si heterojunction solar battery.
Graphene/MoS that the present embodiment provides
2the photoelectricity transformation principle of/Si heterojunction solar battery is referring to accompanying drawing 3.Shown in figure, graphene layer, MoS
2film, p-MoS
2space charge region and n-Si substrate that/n-Si interface forms, its photoelectricity transformation principle is as follows:
The transmissivity of Graphene is very high, and the light transmission Graphene under illumination more than 85% is irradiated to MoS
2film, at MoS
2surface produces electron hole pair, when the diffusion length of light induced electron is greater than MoS
2the thickness of film and be diffused into MoS
2during/Si heterojunction edge, at heterojunction space charge region internal electric field
e mS effect under light induced electron swept to rapidly
n-Si district, forms electronics accumulation on n-Si surface; MoS
2the photohole of middle generation is swept to MoS
2surface, forms hole accumulation layer.Therefore the hole that, illumination produces, electronics are respectively at MoS
2surface and
n-Si forms accumulation, makes MoS
2/ Si knot both sides form voltage difference, and this voltage difference is the voltage difference that illumination produces under without extraneous bias effect, so has photovoltaic effect.
Due to ultra-thin MoS
2only have after several atomic layers, some light can also see through MoS
2layer and enter
n-Si layer is absorbed again (special for being near the near infrared light radiation of 900nm) by Si layer, produce electron hole pair, when hole is diffused into MoS
2during/Si heterojunction border, under the effect of pn heterojunction internal electric field, swept to
p-moS
2, light induced electron exists
nthe accumulation of-Si face.MoS
2/ Si heterojunction both sides further produce voltage difference, and produce photovoltaic effect.This photovoltaic effect superposes the photovoltaic effect in above.
In the process forming at heterojunction solar battery photovoltaic effect, MoS
2internal electric field in/Si
e mS play the effect of accelerating electron motion.Compare with traditional silicon pn joint solar cell, this heterojunction solar battery has biabsorption effect, MoS
2the main light radiation that absorbs 300~700nm, Si mainly absorbs the radiation of near infrared band, has increased absorptivity and the internal quantum efficiency of solar cell, has enlarged markedly photovoltaic effect, thereby has greatly improved conversion efficiency.By measuring the open circuit voltage of this device
v oc and short-circuit current density
j sc , just can calculate the energy conversion efficiency of double-junction solar battery.
Referring to accompanying drawing 4, it is that the present embodiment adopts chemical vapor deposition (CVD) legal system for MoS
2the apparatus structure schematic diagram of film.This device consists of four parts: reactive deposition chamber, vacuum-pumping system, mass-flow gas meter and temperature control system that quartz ampoule forms.Backing material employing resistivity is 3~5 Ω cm, crystal orientation (111)
ntype silicon (Si) sheet, is of a size of 12 * 12 mm
2* 500 μ m.
Preparation method comprises the steps:
Substrate cleans: first by rare HF acid soak, within 15 minutes, remove the silicon dioxide on Si surface, then use successively acetone, ethanol, deionized water Ultrasonic Cleaning, remove the organic substance on silicon chip, finally with nitrogen, dry up, then put into quartz ampoule.Before deposition, quartz ampoule vacuum is evacuated to 10
-2pa, is heated to 300 ℃ and maintains 10 minutes, to remove the steam of silicon chip surface.
MoS
2film preparation: quartz ampoule is heated to 500 ℃,, passes into and analyze pure MoS as carrying gas with Ar gas
2solution (dilute sulfuric acid is solvent).And to analyze pure Al (NO
3)
3as Al dopant to MoS
2carry out p-type doping.For at MoS
2in the time of film growth, adulterate, at MoS
2solution adds Al (NO with the mass ratio of 1:20
3)
3solution.Argon gas carries MoS
2and Al (NO
3)
3entering quartz ampoule exists
n-Si (111) sheet adsorbs, nucleation and growth 10 minutes, then quartz ampoule is raised to 950 ℃ and carries out annealing in process, annealing time 30 minutes.
Electrode fabrication: Graphene is the nesa coating that a kind of conductivity is fabulous, has fabulous conductivity, can be used as in solar cell as anode.The growth of Graphene: quartz ampoule temperature still maintains 950 ℃, methane is decomposed into carbon atom and hydrogen under 800~950 ℃ of high temperature, and under the vapor transportation effect of argon gas 10 sccm (10~30 sccm) flow, carbon atom arrives established MoS
2the MoS of/Si pn knot
2surface is also adsorbed to surface, finally in substrate surface nucleation, then attracts other carbon atom by Van der Waals attraction, and become with it key to form the cancellated graphene film of hexagonal after substrate surface migration.Generally, the in the situation that of reactant abundance, the speed of the deposition film of CVD is very fast.In the present embodiment, the methane flow of employing is very little, only has a small amount of carbon atom to arrive silicon chip surface in the unit interval, by controlling the reaction time at 5~10 minutes, just can obtain ultra-thin graphene film.After having reacted, quartz ampoule temperature is raised to 950~1000 ℃, by sample annealing 10 minutes.After having annealed, take out sample after waiting quartz ampoule to naturally cool to room temperature.
Lower surface AM aluminum metallization electrode to n-silicon chip, the negative electrode of formation solar cell.Complete Graphene/MoS
2the preparation of/Si heterojunction solar battery.
By the Graphene/MoS preparing
2/ Si heterojunction solar battery carries out surface topography and photovoltaic effect is measured, and utilizes atomic force microscope, current/voltage testing apparatus and Hall effect to analyze surface topography and the photocurrent characteristics of this device.Membrane structure application Raman spectrum is observed, and with the transmitance of ultraviolet-visible light (UV-vis) spectrophotometer (Shimadzu UV-3600) analytic sample, finally Graphene/MoS
2photocurrent characteristics application Keithley 4200 SCS of/Si heterojunction solar battery measure.
Referring to accompanying drawing 5~7, Fig. 5 is one
nthe multilayer MoS preparing on Si sheet
2the typical atomic force microscopy of film.Can find out many MoS
2small pieces are evenly distributed in Si sheet surface.This layer of MoS
2about 5~10 nm of thickness of film, are equivalent to tens atomic layers thick.Fig. 6 is prepared MoS
2the x-ray diffraction pattern of film.Discovery has 6 very strong diffraction to meet at 13.482 °, 32.997 °, 47.786 °, 14.460 °, 33.212 °, 47.898 ° 2 θ angle place, with MoS
2the XRD standard card contrast of crystal, above diffraction maximum is corresponding MoS respectively
2(002), the diffraction peak of (104), (100), (105) (106), (110) crystal face matches substantially, and the MoS of growth is described
2film is the MoS of polycrystalline
2film.Fig. 7 is prepared MoS
2the Raman spectrum of film.In figure, there are 2 very strong Raman vibration peak, are positioned at 385.5 cm
1the corresponding E of vibration peak
1 2gplane internal vibration pattern, and be positioned at 408.1cm
-1corresponding (A
1g) the outer vibration mode of plane. E
1 2gand A
1gfor MoS
2typical vibration mode, has further confirmed MoS
2the existence of structure. in addition, A
1gand E
1 2gthe alternate position spike of pattern (Δ) can be for rough estimate MoS
2the thickness of film, Δ is larger, MoS
2the film number of plies is more.Common individual layer MoS
2the alternate position spike Δ of two patterns of this of film is 18.In our sample, these two pattern Δs are 22.6, and the MoS of the present embodiment growth has been described
2film is multilayer film.
Referring to accompanying drawing 8, it is prepared MoS
2the visible absorption spectrum of film.The prepared MoS that utilized UV-3600 spectrophotometer measurement
2film sample absorption spectra.Can find out, molybdenum sulfide has very strong absorption to the visible ray between 300 ~ 700 nm wavelength, and this shows that molybdenum sulfide can be used as good light absorbing material.While surpassing 732 nm, absorption intensity reduces rapidly.732nm is the absorption limit of molybdenum sulfide film, according to the relation between semi-conducting material band gap width and wavelength: E
gthe band gap width that=1.24/ λ (eV) can obtain prepared molybdenum sulfide film is 1.69 eV.The band gap width of individual layer molybdenum bisuphide (1.8eV), because the band gap width of molybdenum sulfide can reduce with the increase of the number of plies, so the band gap width drawing in experiment is less.
Referring to accompanying drawing 9, it is the surperficial I-V characteristic of prepared molybdenum sulfide film, has measured the surperficial conductive characteristic of molybdenum sulfide film with HMS-3000 Hall effect tester.Voltage V
ab, V
bc, V
cd, V
dabe respectively the voltage between molybdenum sulfide film surface a, b, c, tetra-symmetry electrodes of d.Can find out, these four interelectrode voltages and added electric current I are approximated to linear relationship, have embodied molybdenum sulfide film and have had good surface conductance characteristic.Because sample surfaces exists some fluctuatings or interelectrode asymmetry to cause straight line to produce a little fluctuation.The Hall coefficient R that Hall effect is measured
hpositive negative value can infer the conduction type of sample, the R of sample provided by the invention
hbe 1.830 * 10
7, illustrate that molybdenum sulfide film is in-situ doped by Al, present P type characteristic.
Referring to accompanying drawing 10~12, Figure 10 is MoS
2the atomic force microscopy of the graphene membrane electrode of preparing on film.Can find out, many Graphene small pieces are evenly distributed on substrate.About 3~5 nm of thickness of graphene film, are equivalent to tens atomic layers thick.Figure 11 is the Raman spectrum of graphene membrane electrode.In this spectrum, have 2 significant Raman vibration peak, one is G peak, is positioned at 1590 cm
-1wave number place, the eigen vibration peak that this peak is graphite; Another is that 2D peak position is in 2690 cm
-1wave number place, according to document announcement, the eigen vibration peak that this peak position is Graphene.The strength ratio at these two peaks is
i 2D:
i g=2.8, this ratio is larger, illustrates that Graphene contained in film is larger mutually, and graphite-phase seldom; Also illustrate that the present invention utilizes the quality of graphene film prepared by the chemical gaseous phase depositing process of low pressure, low discharge good.Figure 12 is the visible transmission spectrum spectrum of graphene membrane electrode, the light transmission spectrum of the graphene film that it provides for the present embodiment.The light transmission rate of its visible region reaches more than 80%.In addition, its light transmission rate is with wavelength change also certain variation.To longer wavelength 600 – 800 nm wave bands, transmitance surpasses 85%, and the high permeability of this spectrum segment can effectively improve the conversion efficiency of solar cell.And carrier concentration and the electron mobility on Graphene surface of having utilized Hall effect apparatus measures.The carrier concentration on the graphene film surface that we are prepared is 10
10cm
-2, electron mobility is 9.5 * 10
4cm
2v
-1s
-1, the ideal value 2 * 10 of this value and Graphene
5cm
2v
-1s
-1very approaching, the good conductivity of graphene film prepared by the present invention is described.
Referring to accompanying drawing 13, Graphene/MoS that it provides for embodiment
2the dark current characteristic of/Si heterojunction solar battery (without light characteristics) curve chart; Result demonstration, this device has good rectification characteristic, and with the rising of applied voltage, electric current is exponential increase.And under reverse biased, its reverse drain saturation current is very little, almost nil.
Referring to accompanying drawing 14, it is at 100 mW cm
-2graphene/MoS that under white light, the present embodiment provides
2the photocurrent characteristics curve chart of/Si heterojunction solar battery.Can find out the open circuit voltage of this solar cell
v ocfor 0.89V, short-circuit current density
j scbe 4.6 mA cm
-2. can calculate this Graphene/MoS
2the energy conversion efficiency of/Si heterojunction solar cell is 4.5%.
Referring to accompanying drawing 15, it is figure time response of the solar cell that provides of the present embodiment.Can find out, under illumination, this device has steep rising edge; While removing illumination, there is vertical trailing edge, and repeatability is fine.Current on/off ratio
i on/
i offsurpass 10
3.Show that this response device speed of light is fast, repeatability is high, can be used as high performance optical detection and opto-electronic device.
Claims (2)
1. a Graphene/MoS
2the preparation method of/Si hetero-junction thin-film solar cell, is characterized in that comprising the steps:
(1) substrate cleans: with
n-Si (111) sheet is substrate, removes the silicon dioxide on Si surface, then use successively acetone, ethanol, deionized water Ultrasonic Cleaning by rare HF acid soak, removes the organic substance on silicon chip, with nitrogen, dries up, and puts into quartz ampoule and carries out deposition processes; The vacuum degree of quartz ampoule is 10
-2pa, is heated to 300 ℃ and maintains 10 minutes, to remove the steam of silicon chip surface;
(2) MoS
2film preparation: quartz ampoule is heated to 500~600 ℃, take as carrying gas, passing into the MoS that dilute sulfuric acid is solvent with argon gas
2solution, at described MoS
2in solution, add Al (NO
3)
3solution, with Al (NO
3)
3as Al dopant to MoS
2carry out p-type doping, in mass ratio, MoS
2:al (NO
3)
3for 1:20~1:50; Gas carries MoS
2and Al (NO
3)
3entering quartz ampoule exists
n-Si (111) sheet adsorbs, nucleation and growth be after 5~10 minutes, quartz ampoule is warmed up to 950 ℃ and carries out annealing in process, and annealing time is 20~40 minutes, obtains MoS
2/ Si pn knot;
(3) quartz ampoule temperature is maintained to 950 ℃, methane decomposition is carbon atom and hydrogen, and under the vapor transportation effect of argon gas 10~30 sccm flows, carbon atom arrives established MoS
2the MoS of/Si pn knot
2surface is also adsorbed to surface, in substrate surface nucleation, then attracts other carbon atom by Van der Waals attraction, and form the cancellated graphene film of hexagonal with the carbon atom of Cheng Jian after substrate surface migration;
(4) right
nthe lower surface AM aluminum metallization electrode of-Si (111) sheet, the negative electrode of formation solar cell, obtains a kind of Graphene/MoS
2/ Si heterojunction solar battery.
2. a Graphene/MoS who prepares by claim 1
2/ Si hetero-junction thin-film solar cell.
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CN109935654A (en) * | 2019-03-21 | 2019-06-25 | 电子科技大学 | A kind of silicon substrate molybdenum disulfide heterojunction photovoltaic sensor and preparation method |
CN112635620A (en) * | 2020-12-21 | 2021-04-09 | 昆明理工大学 | Gr/MX2Preparation method of/Si solar cell |
CN112993075A (en) * | 2021-02-07 | 2021-06-18 | 西安交通大学 | Intercalated graphene/silicon Schottky junction photoelectric detector and preparation process thereof |
CN112993075B (en) * | 2021-02-07 | 2022-08-16 | 西安交通大学 | Intercalated graphene/silicon Schottky junction photoelectric detector and preparation process thereof |
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