Theory of coherent resonance energy transfer for coherent initial condition.
A theory of coherent resonance energy transfer [Jang et al., J. Chem. Phys. 129, 101104 (2008)] is extended for coherent initial condition. For the situation where the initial excitation is an arbitrary linear combination of donor and acceptor excitations, a second order time local quantum master equation combined with polaron transformation is derived. Inhomogeneous terms in the resulting equation have contributions not only from initial donor and acceptor populations but also from their coherence terms. Numerical tests are performed for general super Ohmic spectral density where the bath degrees of freedom coupled to donor and acceptor can be correlated with each other. Calculation results demonstrate sensitivity of early nonstationary population dynamics on the relative sign of initial donor and acceptor excitation states. It is shown that contribution of inhomogeneous terms is more significant for coherent initial condition than for localized one. The overall model calculations provide details of the interplay between quantum coherence and nonequilibrium/non-Markovian effects in the time dependent donor population dynamics.
Jang
Seogjoo
S
Department of Chemistry and Biochemistry, Queens College, City University of New York, 65-30 Kissena Boulevard, Flushing, New York 11367, USA. seogjoo.jang@qc.cuny.edu