Engineering Exciton-Phonon Interactions for Suppressing Nonradiative Energy Loss in Energy-Transfer-lnitiated Photocatalysis

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外文摘要：The prevalent excitonic effects in low-dimensional semiconductors enable energy-transfer-initiated photocatalytic solar-to-chemical energy conversion.However,the generally strong interactions between excitons and lattice vibrations in these low-dimension-al systems lead to robust nonradiative energy loss,which inevitably impedes photocatalytic performance of energy-transfer-initiated reactions.Herein,we high-light the crucial role of engineering exciton-phonon interactions in suppressing nonradiative energy losses in low-dimensional semiconductor-based photocata-lysts.By taking bismuth oxybromide(BiOBr)as an example,we demonstrate that phonon engineering could be effectively implemented by introducing Bi-Br vacancy clusters.Based on nonadiabatic molecular dynamics simulations and spectroscopic investiga-tions,we demonstrate that the defective structure can promote exciton-low-frequency phonon coupling and reduce exciton-high-frequency optical phonon coupling.Benefiting from the tailored couplings,non-radiative decay of excitons in defective BiOBr is sig-nificantly suppressed,thereby facilitating exciton accumulation and hence energy-transfer-initiated photocatalvsis.

外文关键词：

photocatalysisexciton-phonon interac-tionnonradiative decaysenergy transfer

作者：

Hui Wang、Sen Jin、Aolei Wang、Xiang Jiang、Wenxiu Liu、Xiaodong Zhang、Wensheng Yan、Kuai Yu、Jin Zhao、Yi Xie

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作者单位：

Hefei National Laboratory for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei,Anhui 230026

Institute of Energy,Hefei Comprehensive National Science Center,Hefei,Anhui230031

Department of Physics,CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics,International Center for Quantum Design of Functional Materials,University of Science and Technology of China,Hefei,Anhui 230026

National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei,Anhui 230029

Institute of Microscale Optoelectronics,Shenzhen University,Shenzhen,Guangdong 518060

Department of Physics and Astronomy,Univer-sity of Pittsburgh,Pittsburgh,PA 15260

CAS Center for Excellence in Quantum Information and Quantum Physics,University of Science and Technology of China,Hefei,Anhui 230031

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基金：

国家重点研发计划中国科学院战略规划重点项目国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金安徽省自然科学基金University Synergy Innovation Program of Anhui ProvinceUniversity Synergy Innovation Program of Anhui Province深圳市科技计划

项目编号：

2019YFA0210004XDB36000000219225092190526221890754T212200492163105 120742661162010100311974322U2032212U20321602108085J07GXXT-2020-005GXXT-2021-02020200802180159001

出版年：

2023

DOI：

10.31635/ccschem.022.202101748

中国化学会会刊(英文)

CSCD

ISSN：

年,卷(期)：2023.5(1)

参考文献量39