| 2 | Engineering Exciton-Phonon Interactions for Suppressing Nonradiative Energy Loss in Energy-Transfer-Initiated Photocatalysis显示文摘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-dimensional systems lead to robust nonradiative energy loss,which inevitably impedes photocatalytic performance of energy-transfer-initiated reactions.Herein,we highlight the crucial role of engineering exciton-phonon interactions in suppressing nonradiative energy losses in low-dimensional semiconductor-based photocatalysts.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 investigations,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,nonradiative decay of excitons in defective BiOBr is significantly suppressed,thereby facilitating exciton accumulation and hence energy-transfer-initiated photocatalysis. | Hui Wang Sen Jin Aolei Wang Xiang Jiang Wenxiu Liu Xiaodong Zhang Wensheng Yan Kuai Yu Jin Zhao Yi Xie | 2023 | CCS Chemistry2023，5，1： | 0 |
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