A. Okada et al., SOLVENT REORGANIZATION IN LONG-RANGE ELECTRON-TRANSFER - DENSITY-MATRIX APPROACH, The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 102(8), 1998, pp. 1241-1251
The dynamics of charge transfer from a photoexcited donor to an accept
or coupled through a bridge is investigated by using a correlation-fun
ction approach in Liouville space that takes into account solvent dyna
mics with an arbitrary distribution of time scales. The time- and freq
uency-resolved fluorescence spectrum from the acceptor is used to prob
e the scaling of the ET rate with bridge size. The crossover between t
he coherent tunneling (transfer) and the incoherent sequential (transp
ort) regimes and its implications on the nature of ET processes in DNA
are discussed.