Vibronic coherence evolution in multidimensional ultrafast photochemical processes.

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 tri

SUBMITTER: Gaynor JD 

PROVIDER: S-EPMC6901526 | biostudies-literature | 2019 Dec

REPOSITORIES: biostudies-literature