Open AccessUltrafast dynamics of multi-exciton state coupled to coherent vibration in zinc chlorin aggregates for artificial photosynthesis
Author(s) -
Tongchao Shi,
Zhengzheng Liu,
Tomohiro Miyatake,
Hitoshi Tamiaki,
Takayoshi Kobayashi,
Zeyu Zhang,
Juan Du,
Yuxin Leng
Publication year - 2017
Publication title -
optics express
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.394
H-Index - 271
ISSN - 1094-4087
DOI - 10.1364/oe.25.029667
Subject(s) - exciton , transition dipole moment , relaxation (psychology) , spectroscopy , ultrafast laser spectroscopy , molecular physics , dipole , absorption spectroscopy , ultrashort pulse , materials science , biexciton , vibrational energy relaxation , atomic physics , physics , optics , condensed matter physics , laser , psychology , social psychology , quantum mechanics , excited state
Ultrafast vibronic dynamics induced by the interaction of the Frenkel exciton with the coherent molecular vibrations in a layer-structured zinc chlorin aggregates prepared for artificial photosynthesis have been studied by 7.1 fs real-time vibrational spectroscopy with multi-spectrum detection. The fast decay of 100 ± 5fs is ascribed to the relaxation from the higher multi-exciton state (MES) to the one-exciton state, and the slow one of 863 ± 70fs is assigned to the relaxation from Q-exciton state to the dark nonfluorescent charge-transfer (CT) state, respectively. In addition, the wavelength dependences of the exciton-vibration coupling strength are found to follow the zeroth derivative of the transient absorption spectra of the exciton. It could be explained in term of the transition dipole moment modulated by dynamic intensity borrowing between the B transition and the Q transition through the vibronic interactions.