文摘
To determine the dynamics of a molecular aggregate under the influence of a strongly time-dependent perturbation within a dissipative environment is still, in general, a challenge. The time-dependent perturbation might be, for example, due to external fields or explicitly treated fluctuations within the environment. Methods to calculate the dynamics in these cases do exist though some of these approaches assume that the corresponding correlation functions can be written as a weighted sum of exponentials. One such theory is the hierarchical equations of motion approach. If the environment, however, is described by a complex spectral density or if its temperature is low, these approaches become very inefficient. Therefore, we propose a scheme based on a Chebyshev decomposition of the bath correlation functions and detail the respective quantum master equations within second-order perturbation theory in the environmental coupling. Similar approaches have recently been proposed for systems coupled to Fermionic reservoirs. The proposed scheme is tested for a simple two-level system and compared to existing results. Furthermore, the advantages and disadvantages of the present Chebyshev approach are discussed.