In recent years,solution-processible semiconductors with perovskite or perovskite-inspired structures have been extensively investigated for optoelectronic applications.In particular,silver-bismuth-halides have been i...In recent years,solution-processible semiconductors with perovskite or perovskite-inspired structures have been extensively investigated for optoelectronic applications.In particular,silver-bismuth-halides have been identified as especially promising because of their bulk properties and lack of heavily toxic elements.This study investigates the potential of Ag2BiI5 for near-infrared(NIR)-blind visible light photodetection,which is critical to emerging applications(e.g.,wearable optoelectronics and the Internet of Things).Self-powered photodetectors were realized and provided a near-constant≈100 mA W−1 responsivity through the visible,a NIR rejection ratio of>250,a long-wavelength responsivity onset matching standard colorimetric functions,and a linear photoresponse of>5 orders of magnitude.The optoelectronic characterization of Ag2BiI5 photodetectors additionally revealed consistency with one-center models and the role of the carrier collection distance in self-powered mode.This study provides a positive outlook of Ag2BiI5 toward emerging applications on low-cost and low-power NIR-blind visible light photodetector.展开更多
All-inorganic perovskite solar cells(PVSCs)have drawn widespread attention for its superior thermal stability.Carbon-based devices are promising to demonstrate excellent long-term operational stability due to the hydr...All-inorganic perovskite solar cells(PVSCs)have drawn widespread attention for its superior thermal stability.Carbon-based devices are promising to demonstrate excellent long-term operational stability due to the hydrophobicity of carbon materials and the abandon of organic holetransporting materials(HTMs).However,the difficulty to control the crystallinity process and the poor morphology leads to serious non-radiative recombination,resulting in low V_(OC)and power conversion efficiency(PCE).In this article,the crystal formation process of all-inorganic perovskites is controlled with a facile composition engineering strategy.By bromide incorporation,high-quality perovskite films with large grain and fewer grain boundaries are achieved.As-prepared perovskite films demonstrate longer carrier lifetime,contributing to lower energy loss and better device performance.Fabricated carbon-based HTM-free PVSCs with CsPbI_(2.33)Br_(0.67) perovskite realized champion PCE of 12.40%,superior to 8.80%of CsPbI_(3)-based devices,which is one of the highest efficiencies reported for the carbon-based all-inorganic PVSCs to date.The high V_(OC) of 1.01 V and FF of 70.98% indicate the significance of this composition engineering method.Moreover,fabricated carbon-based devices exhibit excellent stability,and unencapsulated device retains over 90%of its initial efficiency under continuous one sun illumination for 250 h in N_(2) atmosphere and keeps~84%of its original value after stored in ambient environment with RH 15–20% for 200 h.This work provides a facile way to fabricate high-performance and stable carbon-based all-inorganic PVSCs.展开更多
The precisely customizable attributes of self-assembled monolayers(SAMs)molecules at the atomic level hold the potential to facilitate efficient hole selection and interface passivation simultaneously.However,the corr...The precisely customizable attributes of self-assembled monolayers(SAMs)molecules at the atomic level hold the potential to facilitate efficient hole selection and interface passivation simultaneously.However,the correlation between the exposure of passivating groups on the surface and device performance remains unexplored.Herein,we introduce two newly designed SAM molecules,Cbz2S and Cbz2SMe,incorporating cyclic disulfide or two flanking thiomethyls by modifying the 4,5-position of carbazole to adjust the Lewis basicity of the SAM-modified surface.Despite possessing suitable energetic alignment,Cbz2S with more-exposed sulfur atoms exhibited inferior device performance due to excessive reactivity,leading to an overpopulation of PbI2 crystallites at the buried perovskite interface.In contrast,the screening effect from the methyl groups of Cbz2SMe optimized SAM reactivity,exquisitely integrating buried interface passivation and hole selection together.Consequently,the champion inverted perovskite solar cell(PSC)employing Cbz2SMe achieved an impressive power conversion efficiency of 24.42%,accompanied by prolonged stability.This work demonstrates the feasibility of incorporating Lewis-basic passivation groups into SAM molecules and elucidates the relationship between the reactivity of SAM passivation groups and device performance.These findings provide valuable insights for the design of novel multifunctional SAM molecules,further advancing the performance of PSCs.展开更多
CONSPECTUS:Along with the rapid industrialization of human society over the past century,incessant energy consumption and endless damage to the environment have aroused growing attention for seeking clean and renewabl...CONSPECTUS:Along with the rapid industrialization of human society over the past century,incessant energy consumption and endless damage to the environment have aroused growing attention for seeking clean and renewable energy sources.Photovoltaics(PV)that can directly harvest and transform sunlight into electricity have shown great potential in achieving this goal.Especially for solution-processed thin-film solar cells,their extremely cost-effective and facile processing methods compatible with different substrates at large scales exhibit unique advantages over conventional PVs based on crystalline silicon.Various types of solutionprocessed thin-film PVs have been achieving or already exceeded 15%power conversion efficiency(PCE)through the numerous efforts of researchers.Organic solar cells(OSCs)and organic−inorganic hybrid perovskite solar cells(PVSCs)are the most well-known emerging solution-processed thin-film solar cells that have attracted great interest recently(the PCE of PVSCs soared form 3.8%to over 25%in the past decade).Usually,photogenerated excitons will form as a response to illumination in the active layer,then dissociate into charge carriers,travel in between layers,and finally get collected by electrodes of the device.Besides the broad exploration of active layer materials,suitably matched charge-transporting layers and electrodes also play a vital role in achieving high PCE and stability in PV devices.Furthermore,interfaces between different functional layers created during solution processing need to be carefully addressed to ensure efficient charge transport and prevent degradation.The utilization of proper interfacial materials to modify the chemical and electrical properties at interfaces has become an effective strategy to enhance the performance of PV.Therefore,it is important to develop a comprehensive understanding into the correlation between interfacial properties and charge carrier dynamics and establish molecular design principles for interfacial materials to realize commercialization of emerging PVs.展开更多
基金financial support from the National Natural Science Foundation of China (61750110517 and 61805166)the Jiangsu Province Natural Science Foundation (BK20170345)+3 种基金supported by the Collaborative Innovation Center of Suzhou Nano Science & Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the 111 Projectthe Joint International Research Laboratory of Carbon-Based Functional Materials and Devices
文摘In recent years,solution-processible semiconductors with perovskite or perovskite-inspired structures have been extensively investigated for optoelectronic applications.In particular,silver-bismuth-halides have been identified as especially promising because of their bulk properties and lack of heavily toxic elements.This study investigates the potential of Ag2BiI5 for near-infrared(NIR)-blind visible light photodetection,which is critical to emerging applications(e.g.,wearable optoelectronics and the Internet of Things).Self-powered photodetectors were realized and provided a near-constant≈100 mA W−1 responsivity through the visible,a NIR rejection ratio of>250,a long-wavelength responsivity onset matching standard colorimetric functions,and a linear photoresponse of>5 orders of magnitude.The optoelectronic characterization of Ag2BiI5 photodetectors additionally revealed consistency with one-center models and the role of the carrier collection distance in self-powered mode.This study provides a positive outlook of Ag2BiI5 toward emerging applications on low-cost and low-power NIR-blind visible light photodetector.
基金supported by the New Faculty Start-up Grant of the City University of Hong Kong(9610421)the ECS grant(City U 21301319)from the Research Grants Council of Hong Kong+4 种基金the Office of Naval Research(N00014-17-1-2201)Innovation and Technology Fund(ITS/497/18FP,GHP/021/18SZ)Natural Science Foundation of Guangdong Province(2019A1515010761)Guangdong Major Project of Basic and Applied Basic Research(No.2019B030302007)Guangdong-Hong Kong-Macao joint laboratory of optoelectronic and magnetic functional materials(No.2019B121205002)
文摘All-inorganic perovskite solar cells(PVSCs)have drawn widespread attention for its superior thermal stability.Carbon-based devices are promising to demonstrate excellent long-term operational stability due to the hydrophobicity of carbon materials and the abandon of organic holetransporting materials(HTMs).However,the difficulty to control the crystallinity process and the poor morphology leads to serious non-radiative recombination,resulting in low V_(OC)and power conversion efficiency(PCE).In this article,the crystal formation process of all-inorganic perovskites is controlled with a facile composition engineering strategy.By bromide incorporation,high-quality perovskite films with large grain and fewer grain boundaries are achieved.As-prepared perovskite films demonstrate longer carrier lifetime,contributing to lower energy loss and better device performance.Fabricated carbon-based HTM-free PVSCs with CsPbI_(2.33)Br_(0.67) perovskite realized champion PCE of 12.40%,superior to 8.80%of CsPbI_(3)-based devices,which is one of the highest efficiencies reported for the carbon-based all-inorganic PVSCs to date.The high V_(OC) of 1.01 V and FF of 70.98% indicate the significance of this composition engineering method.Moreover,fabricated carbon-based devices exhibit excellent stability,and unencapsulated device retains over 90%of its initial efficiency under continuous one sun illumination for 250 h in N_(2) atmosphere and keeps~84%of its original value after stored in ambient environment with RH 15–20% for 200 h.This work provides a facile way to fabricate high-performance and stable carbon-based all-inorganic PVSCs.
基金support from the CityU Infrastructure Support from Central (APRCgrant nos.9380086,9610419,9610492,and 9610508)of the City University of Hong Kong+5 种基金the Guangdong-Hong Kong Technology Cooperation Funding Scheme (TCFS,grant no.GHP/018/20SZ)Midstream Research Programme for Universities (MRP)Grant (grant no.MRP/040/21X)from the Innovation and Technology Commission of Hong Kongthe Green Tech Fund (grant no.202020164)from the Environment and Ecology Bureau of Hong Kongthe General Research Fund (GRF,grant nos.11307621 and 11316422)from the Research Grants Council of Hong KongShenzhen Science and Technology Program (grant no.SGDX20201103095412040)Guangdong Major Project of Basic and Applied Basic Research (grant no.2019B030302007).
文摘The precisely customizable attributes of self-assembled monolayers(SAMs)molecules at the atomic level hold the potential to facilitate efficient hole selection and interface passivation simultaneously.However,the correlation between the exposure of passivating groups on the surface and device performance remains unexplored.Herein,we introduce two newly designed SAM molecules,Cbz2S and Cbz2SMe,incorporating cyclic disulfide or two flanking thiomethyls by modifying the 4,5-position of carbazole to adjust the Lewis basicity of the SAM-modified surface.Despite possessing suitable energetic alignment,Cbz2S with more-exposed sulfur atoms exhibited inferior device performance due to excessive reactivity,leading to an overpopulation of PbI2 crystallites at the buried perovskite interface.In contrast,the screening effect from the methyl groups of Cbz2SMe optimized SAM reactivity,exquisitely integrating buried interface passivation and hole selection together.Consequently,the champion inverted perovskite solar cell(PSC)employing Cbz2SMe achieved an impressive power conversion efficiency of 24.42%,accompanied by prolonged stability.This work demonstrates the feasibility of incorporating Lewis-basic passivation groups into SAM molecules and elucidates the relationship between the reactivity of SAM passivation groups and device performance.These findings provide valuable insights for the design of novel multifunctional SAM molecules,further advancing the performance of PSCs.
基金A.K.Y.J.thanks the sponsorship of the Lee Shau-Kee Chair Professor(Materials Science)the support from the APRC Grant of the City University of Hong Kong(9380086)+3 种基金Innovation and Technology Fund(ITS/497/18FP,GHP/021/18SZ)the US Office of Naval Research(N00014-20-1-2191)the GRF grant(11307621)from the Research Grants Council of Hong Kong,Guangdong Major Project of Basic and Applied Basic Research(2019B030302007)the Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(2019B121205002).
文摘CONSPECTUS:Along with the rapid industrialization of human society over the past century,incessant energy consumption and endless damage to the environment have aroused growing attention for seeking clean and renewable energy sources.Photovoltaics(PV)that can directly harvest and transform sunlight into electricity have shown great potential in achieving this goal.Especially for solution-processed thin-film solar cells,their extremely cost-effective and facile processing methods compatible with different substrates at large scales exhibit unique advantages over conventional PVs based on crystalline silicon.Various types of solutionprocessed thin-film PVs have been achieving or already exceeded 15%power conversion efficiency(PCE)through the numerous efforts of researchers.Organic solar cells(OSCs)and organic−inorganic hybrid perovskite solar cells(PVSCs)are the most well-known emerging solution-processed thin-film solar cells that have attracted great interest recently(the PCE of PVSCs soared form 3.8%to over 25%in the past decade).Usually,photogenerated excitons will form as a response to illumination in the active layer,then dissociate into charge carriers,travel in between layers,and finally get collected by electrodes of the device.Besides the broad exploration of active layer materials,suitably matched charge-transporting layers and electrodes also play a vital role in achieving high PCE and stability in PV devices.Furthermore,interfaces between different functional layers created during solution processing need to be carefully addressed to ensure efficient charge transport and prevent degradation.The utilization of proper interfacial materials to modify the chemical and electrical properties at interfaces has become an effective strategy to enhance the performance of PV.Therefore,it is important to develop a comprehensive understanding into the correlation between interfacial properties and charge carrier dynamics and establish molecular design principles for interfacial materials to realize commercialization of emerging PVs.
