Generalized (quantum) master equations: Exact memory kernel and high order perturbative approximation
Qiang Shi, Chinese Academy of Sciences
In this talk, I will summarize some recent progresses in our group in combining the generalized master equations (GMEs) and the hierarchical equation of motion (HEOM) to study quantum dynamics in condensed phases. (1) The HEOM and extended HEOM methods are used to calculate the exact time non-local (TNL)and time-local (TL) memory kernels and their high order perturbative expansions. By applying the new methods to the spin-Boson model, we are able to investigate the convergence of high order electron transfer reactions rates. (2) The method is applied to a one-dimensional Holstein type of model to understand the charge carrier mobility in organic semiconductors. It is shown that the long-range hopping beyond nearest neighbor plays an important rule if the intermolecular coupling is large. (3) Similar ideas are applied to a model of electron transport in molecular junctions, where we derive a new expression to calculate the transport current based on populations.
References
[1] M. Xu, Y.-M. Yan, Y.-Y. Liu, and Q. Shi, J. Chem. Phys. 148, 174102 (2018).
[2] Y.-M. Yan, M. Xu, Y.-Y. Liu, and Q. Shi, J. Chem. Phys. 150, 234101 (2019).
[3] Y.-Y. Liu, Y.-M. Yan, M. Xu, and Q. Shi, Chin. J. Chem. Phys. 31, 575 (2018).
[4] X.-H Dan, M. Xu, Y.-M. Yan, and Q. Shi, J. Chem. Phys., in press.