Metal halide perovskite nanostructures have emerged as low-dimensional semiconductors of great significance in many fields such as photovoltaics,photonics,and optoelectronics.Extensive efforts on the controlled synthe...Metal halide perovskite nanostructures have emerged as low-dimensional semiconductors of great significance in many fields such as photovoltaics,photonics,and optoelectronics.Extensive efforts on the controlled synthesis of perovskite nanostructures have been made towards potential device applications.The engineering of their band structures holds great promise in the rational tuning of the electronic and optical properties of perovskite nanostructures,which is one of the keys to achieving efficient and multifunctional optoelectronic devices.In this article,we summarize recent advances in band structure engineering of perovskite nanostructures.A survey of bandgap engineering of nanostructured perovskites is firstly presented from the aspects of dimensionality tailoring,compositional substitution,phase segregation and transition,as well as strain and pressure stimuli.The strategies of electronic doping are then reviewed,including defect-induced self-doping,inorganic or organic molecules-based chemical doping,and modification by metal ions or nanostructures.Based on the bandgap engineering and electronic doping,discussions on engineering energy band alignments in perovskite nanostructures are provided for building high-performance perovskite p-n junctions and heterostructures.At last,we provide our perspectives in engineering band structures of perovskite nanostructures towards future low-energy optoelectronics technologies.展开更多
Two-dimensional Dion-Jacobson(DJ)perovskite has garnered significant attention due to its superior responsivity and operation stability.However,efforts are predominantly focused on discovering new organic spacer to sy...Two-dimensional Dion-Jacobson(DJ)perovskite has garnered significant attention due to its superior responsivity and operation stability.However,efforts are predominantly focused on discovering new organic spacer to synthesize novel perovskites,while material-form-associated light management,which is crucial for enhancing the photodetector’s efficiency,is largely overlooked.Herein,we introduced surface light management strategy into DJ-type perovskite system by synthesizing surface-patterned BDAPbBr4(BPB,BDA=NH_(3)(CH_(2))_(4)NH_(3))microplates(MPs)using template-assisted space-confined method,which was further elucidated by theoretical optical simulation.By leveraging surface-patterned MPs to enhance light absorption,the BPB-based photodetectors(PDs)achieved remarkable photoresponse in ultraviolet region,marked by a high on/off ratio(~5000),superior responsivity(2.24 A W^(-1)),along with large detectivity(~10^(13) Jones)and low detection limit(68.7 nW cm^(-2)).Additionally,the PDs showcased superior light communication and imaging capabilities even under weak-light illumination.Notably,the anisotropic nature of the surface-patterned MPs conferred excellent polarization sensitivity to the PD.These results represented the first demonstration of BPB perovskite in weak-light communication and imaging,as well as in polarized light detection.Our findings offer valuable insights into enhancing photodetector performance and optoelectronic applications through surface light management strategies.展开更多
Two-dimensional(2D) layered perovskites have emerged as potential alternates to traditional three-dimensional(3D)analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been ...Two-dimensional(2D) layered perovskites have emerged as potential alternates to traditional three-dimensional(3D)analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been spent on manipulating the interlayer organic spacing cation to improve the photovoltaic properties of Dion–Jacobson(DJ) perovskites. In this work, a serious of cycloalkane(CA) molecules were selected as the organic spacing cation in 2D DJ perovskites, which can widely manipulate the optoelectronic properties of the DJ perovskites. The underlying relationship between the CA interlayer molecules and the crystal structures, thermodynamic stabilities, and electronic properties of 58 DJ perovskites has been investigated by using automatic high-throughput workflow cooperated with density-functional(DFT) calculations.We found that these CA-based DJ perovskites are all thermodynamic stable. The sizes of the cycloalkane molecules can influence the degree of inorganic framework distortion and further tune the bandgaps with a wide range of 0.9–2.1 eV.These findings indicate the cycloalkane molecules are suitable as spacing cation in 2D DJ perovskites and provide a useful guidance in designing novel 2D DJ perovskites for optoelectronic applications.展开更多
基金support from Australian Research Council (ARC, FT150100450, IH150100006 and CE170100039)support from the MCATM and the FLEET+1 种基金the support from Shenzhen Nanshan District Pilotage Team Program (LHTD20170006)support from Guangzhou Science and Technology Program (Grant No. 201804010322)
文摘Metal halide perovskite nanostructures have emerged as low-dimensional semiconductors of great significance in many fields such as photovoltaics,photonics,and optoelectronics.Extensive efforts on the controlled synthesis of perovskite nanostructures have been made towards potential device applications.The engineering of their band structures holds great promise in the rational tuning of the electronic and optical properties of perovskite nanostructures,which is one of the keys to achieving efficient and multifunctional optoelectronic devices.In this article,we summarize recent advances in band structure engineering of perovskite nanostructures.A survey of bandgap engineering of nanostructured perovskites is firstly presented from the aspects of dimensionality tailoring,compositional substitution,phase segregation and transition,as well as strain and pressure stimuli.The strategies of electronic doping are then reviewed,including defect-induced self-doping,inorganic or organic molecules-based chemical doping,and modification by metal ions or nanostructures.Based on the bandgap engineering and electronic doping,discussions on engineering energy band alignments in perovskite nanostructures are provided for building high-performance perovskite p-n junctions and heterostructures.At last,we provide our perspectives in engineering band structures of perovskite nanostructures towards future low-energy optoelectronics technologies.
基金the Key Research and Development Program sponsored by the Ministry of Science and Technology of China(2024YFE0201800)the National Natural Science Foundation of China(Nos.12134010,12174290)the Natural Science Foundation of Hubei Province,China(Grant Nos.2023BAB102 and 2021CFB039).
文摘Two-dimensional Dion-Jacobson(DJ)perovskite has garnered significant attention due to its superior responsivity and operation stability.However,efforts are predominantly focused on discovering new organic spacer to synthesize novel perovskites,while material-form-associated light management,which is crucial for enhancing the photodetector’s efficiency,is largely overlooked.Herein,we introduced surface light management strategy into DJ-type perovskite system by synthesizing surface-patterned BDAPbBr4(BPB,BDA=NH_(3)(CH_(2))_(4)NH_(3))microplates(MPs)using template-assisted space-confined method,which was further elucidated by theoretical optical simulation.By leveraging surface-patterned MPs to enhance light absorption,the BPB-based photodetectors(PDs)achieved remarkable photoresponse in ultraviolet region,marked by a high on/off ratio(~5000),superior responsivity(2.24 A W^(-1)),along with large detectivity(~10^(13) Jones)and low detection limit(68.7 nW cm^(-2)).Additionally,the PDs showcased superior light communication and imaging capabilities even under weak-light illumination.Notably,the anisotropic nature of the surface-patterned MPs conferred excellent polarization sensitivity to the PD.These results represented the first demonstration of BPB perovskite in weak-light communication and imaging,as well as in polarized light detection.Our findings offer valuable insights into enhancing photodetector performance and optoelectronic applications through surface light management strategies.
基金supported by the National Natural Science Foundation of China (Grant No. 62004080)the Postdoctoral Innovative Talents Supporting Program (Grant No. BX20190143)the China Postdoctoral Science Foundation (Grant No. 2020M670834)。
文摘Two-dimensional(2D) layered perovskites have emerged as potential alternates to traditional three-dimensional(3D)analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been spent on manipulating the interlayer organic spacing cation to improve the photovoltaic properties of Dion–Jacobson(DJ) perovskites. In this work, a serious of cycloalkane(CA) molecules were selected as the organic spacing cation in 2D DJ perovskites, which can widely manipulate the optoelectronic properties of the DJ perovskites. The underlying relationship between the CA interlayer molecules and the crystal structures, thermodynamic stabilities, and electronic properties of 58 DJ perovskites has been investigated by using automatic high-throughput workflow cooperated with density-functional(DFT) calculations.We found that these CA-based DJ perovskites are all thermodynamic stable. The sizes of the cycloalkane molecules can influence the degree of inorganic framework distortion and further tune the bandgaps with a wide range of 0.9–2.1 eV.These findings indicate the cycloalkane molecules are suitable as spacing cation in 2D DJ perovskites and provide a useful guidance in designing novel 2D DJ perovskites for optoelectronic applications.
