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Engineering Exciton-Phonon Interactions for Suppressing nonradiative Energy Loss in Energy-Transfer-Initiated Photocatalysis

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CCS Chemistry 2023年第1期5卷 234-244页

作者： Hui Wang Sen Jin Aolei Wang Xiang Jiang Wenxiu Liu Xiaodong Zhang Wensheng Yan Kuai Yu Jin Zhao Yi Xie Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefeiAnhui 230026 Institute of Energy Hefei Comprehensive National Science CenterHefeiAnhui 230031 Department of Physics CAS Key Laboratory of Strongly-Coupled Quantum Matter PhysicsInternational Center for Quantum Design of Functional MaterialsUniversity of Science and Technology of ChinaHefeiAnhui 230026 National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefeiAnhui 230029 Institute of Microscale Optoelectronics Shenzhen UniversityShenzhenGuangdong 518060 Department of Physics and Astronomy University of PittsburghPittsburghPA 15260 CAS Center for Excellence in Quantum Information and Quantum Physics University of Science and Technology of ChinaHefeiAnhui 230031

The prevalent excitonic effects in low-dimensional semiconductors enable energy-transfer-initiated photocatalytic solar-to-chemical energy ***,the generally strong interactions between excitons and lattice vibrations in these low-dimensional systems lead to robust nonradiative energy loss,which inevitably impedes photocatalytic performance of energy-transfer-initiated ***,we highlight the crucial role of engineering exciton-phonon interactions in suppressing nonradiative energy losses in low-dimensional semiconductor-based *** taking bismuth oxybromide(BiOBr)as an example,we demonstrate that phonon engineering could be effectively implemented by introducing Bi-Br vacancy *** on nonadiabatic molecular dynamics simulations and spectroscopic investigations,we demonstrate that the defective structure can promote exciton-low-frequency phonon coupling and reduce exciton-high-frequency optical phonon *** from the tailored couplings,nonradiative decay of excitons in defective BiOBr is significantly suppressed,thereby facilitating exciton accumulation and hence energy-transfer-initiated photocatalysis.

关键词： photocatalysis exciton-phonon interaction nonradiative decays energy transfer

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