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• W2993841089 abstract "Abstract The complex choreography of electronic, vibrational, and vibronic couplings used by photoexcited molecules to transfer energy efficiently is remarkable, but an unambiguous description of the temporally evolving vibronic states governing these processes has proven experimentally elusive. We use multidimensional electronic-vibrational spectroscopy to identify specific time-dependent excited state vibronic couplings involving multiple electronic states, high-frequency vibrations, and low-frequency vibrations which participate in ultrafast intersystem crossing and subsequent relaxation of a photoexcited transition metal complex. We discover an excited state vibronic mechanism driving long-lived charge separation consisting of an initial electronically-localized vibrational wavepacket which triggers delocalization onto two charge transfer states after propagating for ~600 femtoseconds. Electronic delocalization consequently occurs through nonadiabatic internal conversion driven by a 50 cm −1 coupling resulting in vibronic coherence transfer lasting for ~1 picosecond. This study showcases the power of multidimensional electronic-vibrational spectroscopy to elucidate complex, non-equilibrium energy and charge transfer mechanisms involving multiple molecular coordinates." @default.
• W2993841089 created "2019-12-13" @default.
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• W2993841089 date "2019-12-09" @default.
• W2993841089 modified "2023-10-17" @default.
• W2993841089 title "Vibronic coherence evolution in multidimensional ultrafast photochemical processes" @default.
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• W2993841089 doi "https://doi.org/10.1038/s41467-019-13503-9" @default.
• W2993841089 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/6901526" @default.
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• W2993841089 hasPublicationYear "2019" @default.
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