Quantum coherent dynamics in single molecule systems: generalized stochastic Liouville equation

Abstract: We propose the generalized stochastic Liouville equation to investigate the coherent dynamics in single molecule systems coupled to environments which exhibit both nonstationary and non-Markovian features. The generalized stochastic Liouville equation contains a generalized memory kernel associated with both the intrinsic system Hamiltonian and the non-Markovian features of the environmental noise, which returns to the well-known framework established by Kubo in the limit case that the environmental noise is stationary and memoryless. The coherence of the quantum system can be derived by means of the generalized stochastic Liouville equation in two separated averages with no need to consider the statistical characteristics of the environmental noise. We express the exact analytical expressions of the coherence of the single molecule systems induced by the nonstationary and non-Markovian RTN, and the analytical results of the system coherence are in well consistent with that derived by means of some other theoretical approaches.