The time-convolutionless （TCL） quantum master equation provides a powerful tool to simulate reduced dynanfics of a quantum system coupled to a bath. The key quantity ill the TCL master equation is the so-called kern...The time-convolutionless （TCL） quantum master equation provides a powerful tool to simulate reduced dynanfics of a quantum system coupled to a bath. The key quantity ill the TCL master equation is the so-called kernel or generator, which describes eflhcts of the bath degrees of freedom. Since the exact TCL generators are usually hard to calculate analytically, most applications of the TCL generalized master equation have relied on approximate generators using second and fourth order perturbative expansions. By using the hierarchical equation of motion （HEOM） and extended HEOM methods, we present a new approach to calculating the exact TCL generator and its high order perturbative expansions. The new approach is applied to the spin-boson model with diflhrent sets of parameters, to investigate the convergence of the high order expansiolls of the TCL generator. We also discuss circumstances where the exact TCL generator becomes singular for the spin-boson model, and a model of excitation energy transfer in the Fenna-Matthews-Olson complex.展开更多
基金supported by the National Natural Science Foundation of China(No.21673246)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB12020300)
文摘The time-convolutionless （TCL） quantum master equation provides a powerful tool to simulate reduced dynanfics of a quantum system coupled to a bath. The key quantity ill the TCL master equation is the so-called kernel or generator, which describes eflhcts of the bath degrees of freedom. Since the exact TCL generators are usually hard to calculate analytically, most applications of the TCL generalized master equation have relied on approximate generators using second and fourth order perturbative expansions. By using the hierarchical equation of motion （HEOM） and extended HEOM methods, we present a new approach to calculating the exact TCL generator and its high order perturbative expansions. The new approach is applied to the spin-boson model with diflhrent sets of parameters, to investigate the convergence of the high order expansiolls of the TCL generator. We also discuss circumstances where the exact TCL generator becomes singular for the spin-boson model, and a model of excitation energy transfer in the Fenna-Matthews-Olson complex.
