期刊
NATURE CHEMISTRY
卷 12, 期 9, 页码 795-+出版社
NATURE PORTFOLIO
DOI: 10.1038/s41557-020-0507-3
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资金
- National Science Foundation (NSF) [PHYS-1753324]
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy (DOE) [DE-FG02-86ER13491]
- LaserLab Europe
- Engineering and Physical Sciences Research Council (EPSRC) [EP/L005913/1]
- EPSRC [EP/R513039/1]
- Australian Research Council (ARC) [DE200100549]
- European Union Horizon 2020 research and innovation programme [803718]
- Science and Technology Facilities Council, UK
- Swedish Research Council
- Knut and Alice Wallenberg Foundation, Sweden
- Faculty of Natural Science of the University of Gothenburg
- Australian Research Council [DE200100549] Funding Source: Australian Research Council
- EPSRC [2202831, EP/L005913/1] Funding Source: UKRI
Photoinduced isomerization reactions lie at the heart of many chemical processes in nature. The mechanisms of such reactions are determined by a delicate interplay of coupled electronic and nuclear dynamics occurring on the femtosecond scale, followed by the slower redistribution of energy into different vibrational degrees of freedom. Here we apply time-resolved photoelectron spectroscopy with a seeded extreme ultraviolet free-electron laser to trace the ultrafast ring opening of gas-phase thiophenone molecules following ultraviolet photoexcitation. When combined with ab initio electronic structure and molecular dynamics calculations of the excited- and ground-state molecules, the results provide insights into both the electronic and nuclear dynamics of this fundamental class of reactions. The initial ring opening and non-adiabatic coupling to the electronic ground state are shown to be driven by ballistic S-C bond extension and to be complete within 350 fs. Theory and experiment also enable visualization of the rich ground-state dynamics that involve the formation of, and interconversion between, ring-opened isomers and the cyclic structure, as well as fragmentation over much longer timescales.
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