Interplay of exciton or electron transfer and relaxation: Time-convolution generalized master equation approach

Abstract

Generalized Master Equation theory of the time-convolution type for exciton or electron interacting with harmonic phonons is suggested yielding the full single-carrier density matrix. A new form of the projection superoperator used makes the initial condition term zero for a broad class of initial conditions with a partially formed polaron cloud around carrier. Specification to a particle in a symmetric dimer and comparison with standard Haken-Strobl-Reineker model is performed. The theory is shown to yield that, surprisingly, in the resulting memory functions, apart of information about initial polaron cloud survives even after a short redressing time-interval following each individual (and not only initial) carrier hop.