Lead-halide perovskites exhibit outstanding performance in X-ray detection due to their intrinsic features such as high charge carrier mobility,large atomic number,and long carrier lifetime,but the toxicity of lead is...Lead-halide perovskites exhibit outstanding performance in X-ray detection due to their intrinsic features such as high charge carrier mobility,large atomic number,and long carrier lifetime,but the toxicity of lead is regarded as the major factor hindering their development.Here,we introduce organic molecule(R)-(-)-2-methylpiperazine(R-MPz)into the bismuth-based structure to synthesize lead-free(R)-(H_(2)MPz)BiI_(5)(R-MBI).The high-quality centimeter-sized single crystals have been obtained,which show a low dark current and superior environmental stability.Particularly,the single-crystal device of R-MBI exhibits a highμτproduct up to 1.88×10^(-4)cm^(2)/V and a low trap density of 1.21×10^(10)cm^(-3).Further,the detector displays excellent detection sensitivity of 263.58μC Gy_(air)^(-1)cm^(-2)and a favorable low detection limit of 4.35μGyair/s,both of which meet the requirement for medical diagnostics.These findings shed light on the exploration of innovative bismuth-based hybrid perovskites for high-performance X-ray detection.展开更多
Metal halide perovskites have made significant progress in X-ray detection owing to their exceptional optoelec-tronic properties.However,most of these materials suffer from toxic element lead and require for high oper...Metal halide perovskites have made significant progress in X-ray detection owing to their exceptional optoelec-tronic properties.However,most of these materials suffer from toxic element lead and require for high operating voltages.Hence,it is imperative to explore environmentally friendly perovskite crystals without external bias for X-ray detection.Herein,we strategically introduce chiral cations to synthesize a pair of lead-free chiral-polar hybrid perovskites(S-MPz)_(6)Bi_(3)I_(21)·6H_(2)O and(R-MPz)_(6)Bi_(3)I_(21)·6H_(2)O(1S and 1R,S/R-MPz=S/R-2-methylpipera-zinium),which exhibit strong circular dichroism(CD)signals with an anisotropic g-factor reaching approximately 0.017.Significantly,the chiral-polar feature gives rise to distinctive spontaneous polarization,which leads to a photovoltage of 1.1 V under X-ray illumination,endowing self-powered detection capabilities for X-ray.Further exploration of X-ray devices based on 1R single crystal(SC)demonstrates a high sensitivity of 5.2 pC Gy_(air)^(-1)cm^(-2)at zero bias.This study realizes passive X-ray detection depending on the intrinsic spontaneous polarization induced built-in electric field of chiral-polar perovskite,providing an effective approach to the chemical design of desired materials for high-performance"green"self-powered radiation detection.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22175177,21971238,22193042,21833010,22125110,22122507,21921001,and U21A2069)the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(No.ZDBS-LY-SLH024)+1 种基金The National Postdoctoral Program for Innovative Talents(No.BX2021315)the National Key Research and Development Program of China(No.2019YFA0210402)。
文摘Lead-halide perovskites exhibit outstanding performance in X-ray detection due to their intrinsic features such as high charge carrier mobility,large atomic number,and long carrier lifetime,but the toxicity of lead is regarded as the major factor hindering their development.Here,we introduce organic molecule(R)-(-)-2-methylpiperazine(R-MPz)into the bismuth-based structure to synthesize lead-free(R)-(H_(2)MPz)BiI_(5)(R-MBI).The high-quality centimeter-sized single crystals have been obtained,which show a low dark current and superior environmental stability.Particularly,the single-crystal device of R-MBI exhibits a highμτproduct up to 1.88×10^(-4)cm^(2)/V and a low trap density of 1.21×10^(10)cm^(-3).Further,the detector displays excellent detection sensitivity of 263.58μC Gy_(air)^(-1)cm^(-2)and a favorable low detection limit of 4.35μGyair/s,both of which meet the requirement for medical diagnostics.These findings shed light on the exploration of innovative bismuth-based hybrid perovskites for high-performance X-ray detection.
基金supported by the National Natural Science Foundation of China(22322506,22175177,22193042,22125110,22122507,21921001 and U21A2069)the Natural Science Foundation of Fujian Province(2023J06052)the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(ZDBS-LY-SLH024).
文摘Metal halide perovskites have made significant progress in X-ray detection owing to their exceptional optoelec-tronic properties.However,most of these materials suffer from toxic element lead and require for high operating voltages.Hence,it is imperative to explore environmentally friendly perovskite crystals without external bias for X-ray detection.Herein,we strategically introduce chiral cations to synthesize a pair of lead-free chiral-polar hybrid perovskites(S-MPz)_(6)Bi_(3)I_(21)·6H_(2)O and(R-MPz)_(6)Bi_(3)I_(21)·6H_(2)O(1S and 1R,S/R-MPz=S/R-2-methylpipera-zinium),which exhibit strong circular dichroism(CD)signals with an anisotropic g-factor reaching approximately 0.017.Significantly,the chiral-polar feature gives rise to distinctive spontaneous polarization,which leads to a photovoltage of 1.1 V under X-ray illumination,endowing self-powered detection capabilities for X-ray.Further exploration of X-ray devices based on 1R single crystal(SC)demonstrates a high sensitivity of 5.2 pC Gy_(air)^(-1)cm^(-2)at zero bias.This study realizes passive X-ray detection depending on the intrinsic spontaneous polarization induced built-in electric field of chiral-polar perovskite,providing an effective approach to the chemical design of desired materials for high-performance"green"self-powered radiation detection.