Unraveling the Mechanism of Photoinduced Charge Transfer in Carotenoid-Porphyrin-C-60 Molecular Triad

作者：Manna Arun K; Balamurugan D; Cheung Margaret S^*; Dunietz Barry D

来源：Journal of Physical Chemistry Letters, 2015, 6(7): 1231-1237.

DOI：10.1021/acs.jpclett.5b00074

Photoinduced charge transfer (CT) plays a central role in biologically significant systems and in applications that harvest solar energy. We investigate the relationship of CT kinetics and conformation in a molecular triad. The triad, consisting of carotenoid, porphyrin, and fullerene is structurally and able to acquire significantly varied conformations under ambient conditions With an in approach of quantum calculations and molecular dynamics simulations, we compute the rate of CT at two distinctive conformations. The linearly extended conformation, in which the donor (carotenoid) and the acceptor (fullerene) are separated by nearly 50 angstrom, enables charge separation through a sequential CT process. A representative bent conformation that is entropically dominant, however, attenuates the CT, although the donor and the acceptor are spatially closer. Our computed rate of CT at the linear conformation is in good agreement with measured values. Our work provides unique fundamental understanding of the photoinduced CT process in the molecular triad.

• 出版日期2015-4-2