Stochastic Liouville Equation Model for Nonperiodic Systems and Finite Temperatures

Abstract

Abstract Theoretical background leading to the recently proposed generalization of the stochastic Liouville equation model of the excitation transfer to nonperiodic systems and finite temperatures is reformulated here using the time‐convolutionless generalized master equations. In the lowest order and for linear coupling to phonons, the Haken‐Strobl‐Reineker parametrization becomes acceptable after a short initial time‐interval following the creation of the excitation, but with time‐dependent parametrization, the theory applies to arbitrarily short time‐intervals. For separable initial conditions, the time development of the excitation is calculated numerically for onedimensional models describing the dynamics of the excitation near traps, trap‐luminescence etc. provided that the time‐development in the initial time interval is negligible. The equations correctly provide non‐equal asymptotic site‐occupation probabilities for non‐equal sites if the excitation lifetime is infinite.