The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large ...The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large open-circuit voltage deficit(V_(oc,deficit)) and significantly limit kesterite photovoltaics performance,primarily arising from the generated more recombination centers and insufficient p to n conversion at p-n junction. Herein, we establish a surface defects ordering structure in CZTSSe system via local substitution of Cu by Ag to suppress disordered Cu_(Zn) defects and generate benign n-type Zn_(Ag) donors. Taking advantage of the decreased annealing temperature of Ag F post deposition treatment(PDT), the high concentration of Ag incorporated into surface absorber facilitates the formation of surface ordered defect environment similar to that of efficient CIGS PV. The manipulation of highly doped surface structure could effectively reduce recombination centers, increase depletion region width and enlarge the band bending near p-n junction. As a result, the Ag F-PDT device finally achieves maximum efficiency of 12.34% with enhanced V_(oc) of 0.496 V. These results offer a new solution route in surface defects and energy-level engineering, and open the way to build up high quality p-n junction for future development of kesterite technology.展开更多
Cadmium sulfide(CdS)is an n-type semiconductor with excellent electrical conductivity that is widely used as an electron transport material(ETM)in solar cells.At present,numerous methods for preparing CdS thin films h...Cadmium sulfide(CdS)is an n-type semiconductor with excellent electrical conductivity that is widely used as an electron transport material(ETM)in solar cells.At present,numerous methods for preparing CdS thin films have emerged,among which magnetron sputtering(MS)is one of the most commonly used vacuum techniques.For this type of technique,the substrate temperature is one of the key deposition parameters that affects the interfacial properties between the target film and substrate,determining the specific growth habits of the films.Herein,the effect of substrate temperature on the microstructure and electrical properties of magnetron-sputtered CdS(MS-CdS)films was studied and applied for the first time in hydrothermally deposited antimony selenosulfide(Sb_(2)(S,Se)_(3))solar cells.Adjusting the substrate temperature not only results in the design of the flat and dense film with enhanced crystallinity but also leads to the formation of an energy level arrangement with a Sb_(2)(S,Se)_(3)layer that is more favorable for electron transfer.In addition,we developed an oxygen plasma treatment for CdS,reducing the parasitic absorption of the device and resulting in an increase in the short-circuit current density of the solar cell.This study demonstrates the feasibility of MS-CdS in the fabrication of hydrothermal Sb_(2)(S,Se)_(3)solar cells and provides interface optimization strategies to improve device performance.展开更多
Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)has attracted considerable attention as a non-toxic and earthabundant solar cell material.During selenization of CZTSSe film at high temperature,the reaction between CZTSSe and Mo...Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)has attracted considerable attention as a non-toxic and earthabundant solar cell material.During selenization of CZTSSe film at high temperature,the reaction between CZTSSe and Mo is one of the main reasons that result in unfavorable absorber and interface quality,which leads to large open circuit voltage deficit(VOC-def)and low fill factor(FF).Herein,a WO_(3)intermediate layer introduced at the back interface can effectually inhibit the unfavorable interface reaction between absorber and back electrode in the preliminary selenization progress;thus high-quality crystals are obtained.Through this back interface engineering,the traditional problems of phase segregation,voids in the absorber and over thick Mo(S,Se)_(2)at the back interface can be well solved,which greatly lessens the recombination in the bulk and at the interface.The increased minority carrier diffusion length,decreased barrier height at back interface contact and reduced deep acceptor defects give rise to systematic improvement in VOCand FF,finally a 12.66%conversion efficiency for CZTSSe solar cell has been achieved.This work provides a simple way to fabricate highly efficient solar cells and promotes a deeper understanding of the function of intermediate layer at back interface in kesterite-based solar cells.展开更多
Antimony chalcogenide Sb_(2)(S, Se)_(3) is attracting a lot of attention as photovoltaic absorber owing to its rewarding photoelectric properties, low toxicity, and earth abundance. However, its device efficiency is s...Antimony chalcogenide Sb_(2)(S, Se)_(3) is attracting a lot of attention as photovoltaic absorber owing to its rewarding photoelectric properties, low toxicity, and earth abundance. However, its device efficiency is still limited by the absorber material quality and device interface recombination. In this work, a fluorinedoped tin oxide(FTO) substrate with ultra-thin SnO_(2) layer and a low-cost stabilized carbon paste are introduced as a front and back contact layer respectively in Sb_(2)(S, Se)_(3) based planar solar cells. Over 5.2% efficiency is demonstrated in the structure of FTO/SnO_(2)/Cd S/Sb_(2)(S, Se)_3/Carbon/Ag, where the Sb_(2)(S, Se)_(3) is prepared by hydrothermal technique. The complementary device physics characterizations reveal that the interfacial recombination between TCO and Cd S is significantly suppressed by the introduction of ultra-thin SnO_(2) layer, which is profited from the leakage protection and bandgap offset engineering by its high resistivity and suitable conduction band minimum. Meanwhile, the successful adoption of the lowcost stabilized carbon as a back contact here shows an enormous potential to replace the conventional organic hole transport materials and noble metal. We hope this work can provide positive guidance to optimize Sb_(2)(S, Se)_(3) based planar solar cells in the future.展开更多
The use of organic hole transport layer(HTL)Spiro-OMeTAD in various solar cells imposes serious stabil-ity and cost problems,and thus calls for inorganic substitute materials.In this work,a novel inorganic MnS film pr...The use of organic hole transport layer(HTL)Spiro-OMeTAD in various solar cells imposes serious stabil-ity and cost problems,and thus calls for inorganic substitute materials.In this work,a novel inorganic MnS film prepared by thermal evaporation has been demonstrated to serve as a decent HTL in high-performance Sb_(2)(S,Se)_(3)solar cells,providing a cost-effective all-inorganic solution.A low-temperature air-annealing process for the evaporated MnS layer was found to result in a significant positive effect on the power conversion efficiency(PCE)of Sb_(2)(S,Se)_(3)solar cells,due to its better-matched energy band alignment after partial oxidation.Impressively,the device with the optimized MnS HTL has achieved an excellent PCE of about 9.24%,which is the highest efficiency among all-inorganic Sb_(2)(S,Se)_(3)solar cells.Our result has revealed that MnS is a feasible substitute for organic HTL in Sb-based solar cells to achieve high PCE,low cost,and high stability.展开更多
Hydrothermal deposition of antimony selenosulfide(Sb_(2)(S,Se_(3)))has enabled solar cell applications to surpass the 10%efficiency threshold.This deposition process involves the reaction of three precursor materials:...Hydrothermal deposition of antimony selenosulfide(Sb_(2)(S,Se_(3)))has enabled solar cell applications to surpass the 10%efficiency threshold.This deposition process involves the reaction of three precursor materials:Sb,S,and Se.However,this process generates an unfavourable gradient of Se and S anions in the Sb_(2)(S,Se)_(3)film,which limits further efficiency improvements.Herein,we demonstrate how NH_(4)F can be used as an additive to regulate the band gradient of the Sb_(2)(S,Se)_(3)and modify the surface of the CdS electron-transporting layer.On the one hand,NH_(4)F inhibits the decomposition of Na_(2)S_(2)O_(3)and selenourea,which optimizes the deposition process and allows for adjustment of the Se/S ratio and their distribution in the Sb_(2)(S,Se)_(3)film.On the other hand,hydrolysis of NH_(4)F induces dissolution and redeposition of CdS,thereby effectively improving the morphology and crystallinity of the CdS substrate.Finally,the dual effect of NH_(4)F enables improved surface morphology and energy alignment of the Sb_(2)(S,Se)_(3)film,thus yielding a maximum efficiency of 10.28%,a 12%improvement over the control device.This study demonstrates an effective strategy for simultaneously modifying a sulfide-based substrate and regulating the element distribution during the deposition of a metal chalcogenide film for optoelectronic device applications.展开更多
Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)thin film solar cells have been regarded as one of the most promising thin film photovoltaic technologies,offering a low-cost and environmentally friendly solar energy option.Alth...Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)thin film solar cells have been regarded as one of the most promising thin film photovoltaic technologies,offering a low-cost and environmentally friendly solar energy option.Although remarkable advances have been achieved in kesterite solar cells,the performance gap relative to mature thin film photovoltaic technologies such as CIGSe and Cd Te remains large.Significant open-circuit voltage(V_(OC))deficit has been recognized as the main limiting factor to performance improvement,with undesirable intrinsic defects being a key culprit contributing to the low V_(OC).To realize the promise inherent in kesterite CZTS to become an earth-abundant alternative to existing thin film photovoltaic technologies with comparable performance,significant research effort has been invested to tackle the challenging defect issues.In this review,recent progress and achievements relevant to engineering improvements to the defect properties of the semiconductor have been examined and summarized.Promising strategies include:(i)manipulating the synthesis process to obtain a desirable reaction pathway and chemical environment;(ii)introducing cation substitution to increase the ionic size difference and supress the related band tailing deep-level defects;(iii)applying post deposition treatment(PDT)with alkaline elements to passivate the detrimental defects.These advances obtained from work on kesterite solar cells may lead to future high performance from this material and may be further extended to other earth-abundant chalcogenide photovoltaic technologies.展开更多
基金supported by the National Natural Science Foundation of China(61874159,62074052,61974173,52072327,51702085 and 51802081)the Joint Talent Cultivation Funds of NSFC-HN(U1704151 and U1904192)+1 种基金the Zhongyuan Thousand Talents(Zhongyuan Scholars)Program of Henan Province(202101510004)the Science and Technology Innovation Talents in Universities of Henan Province(21HASTIT023)。
文摘The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large open-circuit voltage deficit(V_(oc,deficit)) and significantly limit kesterite photovoltaics performance,primarily arising from the generated more recombination centers and insufficient p to n conversion at p-n junction. Herein, we establish a surface defects ordering structure in CZTSSe system via local substitution of Cu by Ag to suppress disordered Cu_(Zn) defects and generate benign n-type Zn_(Ag) donors. Taking advantage of the decreased annealing temperature of Ag F post deposition treatment(PDT), the high concentration of Ag incorporated into surface absorber facilitates the formation of surface ordered defect environment similar to that of efficient CIGS PV. The manipulation of highly doped surface structure could effectively reduce recombination centers, increase depletion region width and enlarge the band bending near p-n junction. As a result, the Ag F-PDT device finally achieves maximum efficiency of 12.34% with enhanced V_(oc) of 0.496 V. These results offer a new solution route in surface defects and energy-level engineering, and open the way to build up high quality p-n junction for future development of kesterite technology.
基金supported by the National Natural Science Foundation of China(22275180)the National Key Research and Development Program of China(2019YFA0405600)the Collaborative Innovation Program of Hefei Science Center,CAS,and the University Synergy Innovation Program of Anhui Province(GXXT-2023-031).
文摘Cadmium sulfide(CdS)is an n-type semiconductor with excellent electrical conductivity that is widely used as an electron transport material(ETM)in solar cells.At present,numerous methods for preparing CdS thin films have emerged,among which magnetron sputtering(MS)is one of the most commonly used vacuum techniques.For this type of technique,the substrate temperature is one of the key deposition parameters that affects the interfacial properties between the target film and substrate,determining the specific growth habits of the films.Herein,the effect of substrate temperature on the microstructure and electrical properties of magnetron-sputtered CdS(MS-CdS)films was studied and applied for the first time in hydrothermally deposited antimony selenosulfide(Sb_(2)(S,Se)_(3))solar cells.Adjusting the substrate temperature not only results in the design of the flat and dense film with enhanced crystallinity but also leads to the formation of an energy level arrangement with a Sb_(2)(S,Se)_(3)layer that is more favorable for electron transfer.In addition,we developed an oxygen plasma treatment for CdS,reducing the parasitic absorption of the device and resulting in an increase in the short-circuit current density of the solar cell.This study demonstrates the feasibility of MS-CdS in the fabrication of hydrothermal Sb_(2)(S,Se)_(3)solar cells and provides interface optimization strategies to improve device performance.
基金supported by the National Natural Science Foundation of China (22005293, U19A2092 and 22275180)the National Key Research and Development Program of China (2019YFA0405600)+1 种基金the Institute of Energy, Hefei Comprehensive National Science Center (21KZS212)the Collaborative Innovation Program of Hefei Science Center, CAS。
基金supported by the National Key R&D Program of China(no.2018YFE0203400)the National Natural Science Foundation of China(no.62074102)+1 种基金the Guangdong Basic and Applied Basic Research Foundation(no.2022A1515010979)the Science and Technology plan project of Shenzhen(nos.JCYJ20190808120001755 and 20220808165025003)。
文摘Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)has attracted considerable attention as a non-toxic and earthabundant solar cell material.During selenization of CZTSSe film at high temperature,the reaction between CZTSSe and Mo is one of the main reasons that result in unfavorable absorber and interface quality,which leads to large open circuit voltage deficit(VOC-def)and low fill factor(FF).Herein,a WO_(3)intermediate layer introduced at the back interface can effectually inhibit the unfavorable interface reaction between absorber and back electrode in the preliminary selenization progress;thus high-quality crystals are obtained.Through this back interface engineering,the traditional problems of phase segregation,voids in the absorber and over thick Mo(S,Se)_(2)at the back interface can be well solved,which greatly lessens the recombination in the bulk and at the interface.The increased minority carrier diffusion length,decreased barrier height at back interface contact and reduced deep acceptor defects give rise to systematic improvement in VOCand FF,finally a 12.66%conversion efficiency for CZTSSe solar cell has been achieved.This work provides a simple way to fabricate highly efficient solar cells and promotes a deeper understanding of the function of intermediate layer at back interface in kesterite-based solar cells.
基金supported by National Natural Science Foundation of China (Grant No. 61974028)Fujian Normal University(FNU) Training Program of Innovation and Enterpreneurship for Undergraduates (cxxl-2019135+2 种基金20191402019143)the support from Huai An Yaoke Optoelectronics Co.Ltd。
文摘Antimony chalcogenide Sb_(2)(S, Se)_(3) is attracting a lot of attention as photovoltaic absorber owing to its rewarding photoelectric properties, low toxicity, and earth abundance. However, its device efficiency is still limited by the absorber material quality and device interface recombination. In this work, a fluorinedoped tin oxide(FTO) substrate with ultra-thin SnO_(2) layer and a low-cost stabilized carbon paste are introduced as a front and back contact layer respectively in Sb_(2)(S, Se)_(3) based planar solar cells. Over 5.2% efficiency is demonstrated in the structure of FTO/SnO_(2)/Cd S/Sb_(2)(S, Se)_3/Carbon/Ag, where the Sb_(2)(S, Se)_(3) is prepared by hydrothermal technique. The complementary device physics characterizations reveal that the interfacial recombination between TCO and Cd S is significantly suppressed by the introduction of ultra-thin SnO_(2) layer, which is profited from the leakage protection and bandgap offset engineering by its high resistivity and suitable conduction band minimum. Meanwhile, the successful adoption of the lowcost stabilized carbon as a back contact here shows an enormous potential to replace the conventional organic hole transport materials and noble metal. We hope this work can provide positive guidance to optimize Sb_(2)(S, Se)_(3) based planar solar cells in the future.
基金the Science and Technology Department of Hubei Province(2019AAA020)Wuhan Science and Technology Project of China(2019010701011420)+1 种基金Fundamental Research Funds for the Central University(2042021kf0069)the National Natural Science Foundation of China(61974028)。
文摘The use of organic hole transport layer(HTL)Spiro-OMeTAD in various solar cells imposes serious stabil-ity and cost problems,and thus calls for inorganic substitute materials.In this work,a novel inorganic MnS film prepared by thermal evaporation has been demonstrated to serve as a decent HTL in high-performance Sb_(2)(S,Se)_(3)solar cells,providing a cost-effective all-inorganic solution.A low-temperature air-annealing process for the evaporated MnS layer was found to result in a significant positive effect on the power conversion efficiency(PCE)of Sb_(2)(S,Se)_(3)solar cells,due to its better-matched energy band alignment after partial oxidation.Impressively,the device with the optimized MnS HTL has achieved an excellent PCE of about 9.24%,which is the highest efficiency among all-inorganic Sb_(2)(S,Se)_(3)solar cells.Our result has revealed that MnS is a feasible substitute for organic HTL in Sb-based solar cells to achieve high PCE,low cost,and high stability.
基金the National Natural Science Foundation of China(22005293 and U19A2092)the National Key Research and Development Program of China(2019YFA0405600).
文摘Hydrothermal deposition of antimony selenosulfide(Sb_(2)(S,Se_(3)))has enabled solar cell applications to surpass the 10%efficiency threshold.This deposition process involves the reaction of three precursor materials:Sb,S,and Se.However,this process generates an unfavourable gradient of Se and S anions in the Sb_(2)(S,Se)_(3)film,which limits further efficiency improvements.Herein,we demonstrate how NH_(4)F can be used as an additive to regulate the band gradient of the Sb_(2)(S,Se)_(3)and modify the surface of the CdS electron-transporting layer.On the one hand,NH_(4)F inhibits the decomposition of Na_(2)S_(2)O_(3)and selenourea,which optimizes the deposition process and allows for adjustment of the Se/S ratio and their distribution in the Sb_(2)(S,Se)_(3)film.On the other hand,hydrolysis of NH_(4)F induces dissolution and redeposition of CdS,thereby effectively improving the morphology and crystallinity of the CdS substrate.Finally,the dual effect of NH_(4)F enables improved surface morphology and energy alignment of the Sb_(2)(S,Se)_(3)film,thus yielding a maximum efficiency of 10.28%,a 12%improvement over the control device.This study demonstrates an effective strategy for simultaneously modifying a sulfide-based substrate and regulating the element distribution during the deposition of a metal chalcogenide film for optoelectronic device applications.
基金supported by the Australian Renewable Energy Agency(Grant Nos.1-USO028,and 2017/RND006)the Australian Research Council(ARC)Future Fellowship Programme(Grant No.FT190100756)the ACAP Postdoctoral Fellowship Supported by Australian Centre for Advanced Photovoltaics(Grant No.1-SRI001)。
文摘Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)thin film solar cells have been regarded as one of the most promising thin film photovoltaic technologies,offering a low-cost and environmentally friendly solar energy option.Although remarkable advances have been achieved in kesterite solar cells,the performance gap relative to mature thin film photovoltaic technologies such as CIGSe and Cd Te remains large.Significant open-circuit voltage(V_(OC))deficit has been recognized as the main limiting factor to performance improvement,with undesirable intrinsic defects being a key culprit contributing to the low V_(OC).To realize the promise inherent in kesterite CZTS to become an earth-abundant alternative to existing thin film photovoltaic technologies with comparable performance,significant research effort has been invested to tackle the challenging defect issues.In this review,recent progress and achievements relevant to engineering improvements to the defect properties of the semiconductor have been examined and summarized.Promising strategies include:(i)manipulating the synthesis process to obtain a desirable reaction pathway and chemical environment;(ii)introducing cation substitution to increase the ionic size difference and supress the related band tailing deep-level defects;(iii)applying post deposition treatment(PDT)with alkaline elements to passivate the detrimental defects.These advances obtained from work on kesterite solar cells may lead to future high performance from this material and may be further extended to other earth-abundant chalcogenide photovoltaic technologies.
