Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microsco...Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.展开更多
Thanks to the excellent optoelectronic properties,lead halide perovskites(LHPs)have been widely employed in highperformance optoelectronic devices such as solar cells and lightemitting diodes.However,overcoming their ...Thanks to the excellent optoelectronic properties,lead halide perovskites(LHPs)have been widely employed in highperformance optoelectronic devices such as solar cells and lightemitting diodes.However,overcoming their poor stability against water has been one of the biggest challenges for most applications.Herein,we report a novel hot-injection method in a Pb-poor environment combined with a well-designed purification process to synthesize water-dispersible CsPbBr_(3) nanocrystals(NCs).The as-prepared NCs sustain their superior photoluminescence(91%quantum yield in water)for more than 200 days in an aqueous environment,which is attributed to a passivation effect induced by excess CsBr salts.Thanks to the ultra-stability of these LHP NCs,for the first time,we report a new application of LHP NCs,in which they are applied to electrocatalysis of CO_(2) reduction reaction.Noticeably,they show significant electrocatalytic activity(faradaic yield:32%for CH4,40%for CO)and operation stability(>350 h).展开更多
基金Project supported by the National Natural Science Foundation of China (Grant No. 62174079)the Fund from the Science, Technology, and Innovation Commission of Shenzhen Municipality (Grant Nos. JCYJ20220530113015035, JCYJ20210324120204011, JCYJ20190808121211510, and KQTD2015071710313656)。
文摘Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.
基金This research was supported by the National Natural Science Foundation of China(Nos.11674258,51602305,51702219,61975134,11904250)Guangdong Basic and Applied Basic Research Foundation(2020B1515020051)+2 种基金the Science and Technology Innovation Commission of Shenzhen(JCYJ20180305125345378)Shenzhen Nanshan District Pilotage Team Program(LHTD20170006)Partial support from The Institute For Lasers,Photonics and Biophotonics at The University at Buffalo is also acknowledged.T.Z.and I.Z.were supported by the U.S.DOE,Office of Science BES,Award No.DE-SC0004890.
文摘Thanks to the excellent optoelectronic properties,lead halide perovskites(LHPs)have been widely employed in highperformance optoelectronic devices such as solar cells and lightemitting diodes.However,overcoming their poor stability against water has been one of the biggest challenges for most applications.Herein,we report a novel hot-injection method in a Pb-poor environment combined with a well-designed purification process to synthesize water-dispersible CsPbBr_(3) nanocrystals(NCs).The as-prepared NCs sustain their superior photoluminescence(91%quantum yield in water)for more than 200 days in an aqueous environment,which is attributed to a passivation effect induced by excess CsBr salts.Thanks to the ultra-stability of these LHP NCs,for the first time,we report a new application of LHP NCs,in which they are applied to electrocatalysis of CO_(2) reduction reaction.Noticeably,they show significant electrocatalytic activity(faradaic yield:32%for CH4,40%for CO)and operation stability(>350 h).