Antimony selenosulfide(Sb2(S,Se)3)is a promising photovoltaic absorber material for both outdoor and indoor application scenarios.Nevertheless,the performance of Sb2(S,Se)3 solar cells remains constrained ...Antimony selenosulfide(Sb2(S,Se)3)is a promising photovoltaic absorber material for both outdoor and indoor application scenarios.Nevertheless,the performance of Sb2(S,Se)3 solar cells remains constrained by the severe interface trap-induced nonradiative recombination.Interface engineering has been recognized as an effective approach to suppress recombination and boost charge transport.In this work,we introduce an organic modifier(O-BDT)between Sb2(S,Se)3 absorber and hole transport layer.The theoretical and experimental results evidence that O-BDT can simultaneously passivates interface defects and optimizes the energy-level alignment,leading to a significantly reduced voltage loss.Finally,the O-BDT modified solar cell achieves a power conversion efficiency(PCE)of 8.01%under AM 1.5G illumination.Moreover,the device delivers a PCE of 19.04% under 1000 lux,3312 K LED lighting,among the best list of IPVs based on antimony chalcogenide compounds.展开更多
Antimony selenosulfide(Sb2(S,Se)3)has recently emerged as an attractive thin-film photovoltaic absorber because of its tunable bandgap,excellent optoelectronic properties,and long-term stability.Hydrothermal syn...Antimony selenosulfide(Sb2(S,Se)3)has recently emerged as an attractive thin-film photovoltaic absorber because of its tunable bandgap,excellent optoelectronic properties,and long-term stability.Hydrothermal synthesis using separate Sb,Se,and S precursors enables the direct preparation of ternary Sb2(S,Se)3thin films,and photovoltaic devices with efficiencies above 10%have been reported.However,due to the higher chemical reactivity of selenium compared to sulfur,the incorporation of Se occurs much faster,leading to compositional inhomogeneity with selenide enrichment near the electron transport interface.This reaction characteristic produces a reverse bandgap gradient that is detrimental to charge extraction.In this study,we unveil a kinetic modulation strategy by employing thiourea(TU)as a multifunctional additive to precisely regulate precursor reaction pathways during hydrothermal growth.TU coordinating with SSeO32-intermediates generate stable complexes,thereby suppressing uncontrolled selenide release and achieving a balanced Se/S incorporation.This manipulation engenders Sb2(S,Se)3films with homogenized bandgap distributions,well-aligned interfacial energetics,and substantially reduced defect densities.Consequently,the optimized devices attain a power conversion efficiency of 10.83%,representing the state-of-the-art performance for Sb2(S,Se)3photovoltaics.This study establishes a novel method for in situ bandgap homogenization and deepens the synthetic mechanism regarding mixed-anion chalcogenide thin films.展开更多
Hydrothermal deposition of antimony selenosulfide(Sb2(S,Se3))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(Sb2(S,Se3))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 Sb2(S,Se)3film,which limits further efficiency improvements.Herein,we demonstrate how NH4F can be used as an additive to regulate the band gradient of the Sb2(S,Se)3and modify the surface of the CdS electron-transporting layer.On the one hand,NH4F inhibits the decomposition of Na2S2O3and selenourea,which optimizes the deposition process and allows for adjustment of the Se/S ratio and their distribution in the Sb2(S,Se)3film.On the other hand,hydrolysis of NH4F induces dissolution and redeposition of CdS,thereby effectively improving the morphology and crystallinity of the CdS substrate.Finally,the dual effect of NH4F enables improved surface morphology and energy alignment of the Sb2(S,Se)3film,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
Carrier separation in a solar cell usually relies on the p–n junction. Here we show that an n–n type inorganic semiconductor heterojunction is also able to separate the exciton for efficient solar cell applications....Carrier separation in a solar cell usually relies on the p–n junction. Here we show that an n–n type inorganic semiconductor heterojunction is also able to separate the exciton for efficient solar cell applications. The n–n type heterojunction was formed by hydrothermal deposition of Sb2(S,Se)3 and thermal evaporation of Sb2Se3. We found that the n–n junction is able to enhance the carrier separation by the formation of an electric field, reduce the interfacial recombination and generate optimized band alignment. The device based on this n–n junction shows 2.89% net efficiency improvement to 7.75%when compared with the device consisted of semiconductor absorber–metal contact. The study in the n–n type solar cell is expected to bring about more versatile materials utility, new interfacial engineering strategy and fundamental findings in the photovoltaic energy conversion process.展开更多
基金the support from National Natural Science Foundation of China(52002105,51972091,51602089 and 52102231)Natural Science Foundation of Anhui Province(2408085MF166,1908085QB56 and 2008085QB89)Xuancheng&Xuancheng Economic Development Zone Joint Science and Technology Project(JZ2024AHDS0322)。
摘要Antimony selenosulfide(Sb2(S,Se)3)is a promising photovoltaic absorber material for both outdoor and indoor application scenarios.Nevertheless,the performance of Sb2(S,Se)3 solar cells remains constrained by the severe interface trap-induced nonradiative recombination.Interface engineering has been recognized as an effective approach to suppress recombination and boost charge transport.In this work,we introduce an organic modifier(O-BDT)between Sb2(S,Se)3 absorber and hole transport layer.The theoretical and experimental results evidence that O-BDT can simultaneously passivates interface defects and optimizes the energy-level alignment,leading to a significantly reduced voltage loss.Finally,the O-BDT modified solar cell achieves a power conversion efficiency(PCE)of 8.01%under AM 1.5G illumination.Moreover,the device delivers a PCE of 19.04% under 1000 lux,3312 K LED lighting,among the best list of IPVs based on antimony chalcogenide compounds.
基金National Natural Science Foundation of China(Grant No.22275180 and 52572274)Major Science and Technology Projects of Anhui Province(AHZDCYCXLSDT2023-10)+2 种基金Collaborative Innovation Program of Hefei Science Center,CASUniversity Synergy Innovation Program of Anhui Province(GXXT-2023-031)Fundamental Research Funds for the Central Universities(No.WK2490000002)。
摘要Antimony selenosulfide(Sb2(S,Se)3)has recently emerged as an attractive thin-film photovoltaic absorber because of its tunable bandgap,excellent optoelectronic properties,and long-term stability.Hydrothermal synthesis using separate Sb,Se,and S precursors enables the direct preparation of ternary Sb2(S,Se)3thin films,and photovoltaic devices with efficiencies above 10%have been reported.However,due to the higher chemical reactivity of selenium compared to sulfur,the incorporation of Se occurs much faster,leading to compositional inhomogeneity with selenide enrichment near the electron transport interface.This reaction characteristic produces a reverse bandgap gradient that is detrimental to charge extraction.In this study,we unveil a kinetic modulation strategy by employing thiourea(TU)as a multifunctional additive to precisely regulate precursor reaction pathways during hydrothermal growth.TU coordinating with SSeO32-intermediates generate stable complexes,thereby suppressing uncontrolled selenide release and achieving a balanced Se/S incorporation.This manipulation engenders Sb2(S,Se)3films with homogenized bandgap distributions,well-aligned interfacial energetics,and substantially reduced defect densities.Consequently,the optimized devices attain a power conversion efficiency of 10.83%,representing the state-of-the-art performance for Sb2(S,Se)3photovoltaics.This study establishes a novel method for in situ bandgap homogenization and deepens the synthetic mechanism regarding mixed-anion chalcogenide thin films.
基金the National Natural Science Foundation of China(22005293 and U19A2092)the National Key Research and Development Program of China(2019YFA0405600).
摘要Hydrothermal deposition of antimony selenosulfide(Sb2(S,Se3))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 Sb2(S,Se)3film,which limits further efficiency improvements.Herein,we demonstrate how NH4F can be used as an additive to regulate the band gradient of the Sb2(S,Se)3and modify the surface of the CdS electron-transporting layer.On the one hand,NH4F inhibits the decomposition of Na2S2O3and selenourea,which optimizes the deposition process and allows for adjustment of the Se/S ratio and their distribution in the Sb2(S,Se)3film.On the other hand,hydrolysis of NH4F induces dissolution and redeposition of CdS,thereby effectively improving the morphology and crystallinity of the CdS substrate.Finally,the dual effect of NH4F enables improved surface morphology and energy alignment of the Sb2(S,Se)3film,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Project supported by Institute of Energy, Hefei Comprehensive National Science Center (Grant No. 21KZS212)the National Key Research and Development Program of China (Grant No. 2019YFA0405600)+2 种基金the National Natural Science Foundation of China (Grant Nos. U19A2092 and 22005293)the China Postdoctoral Science Foundation (Grant No. 2021M693045)Collaborative Innovation Program of Hefei Science Center, Chinese Academy of Sciences。
摘要Carrier separation in a solar cell usually relies on the p–n junction. Here we show that an n–n type inorganic semiconductor heterojunction is also able to separate the exciton for efficient solar cell applications. The n–n type heterojunction was formed by hydrothermal deposition of Sb2(S,Se)3 and thermal evaporation of Sb2Se3. We found that the n–n junction is able to enhance the carrier separation by the formation of an electric field, reduce the interfacial recombination and generate optimized band alignment. The device based on this n–n junction shows 2.89% net efficiency improvement to 7.75%when compared with the device consisted of semiconductor absorber–metal contact. The study in the n–n type solar cell is expected to bring about more versatile materials utility, new interfacial engineering strategy and fundamental findings in the photovoltaic energy conversion process.