Nonequilibrium heat transport in a molecular junction: A mixed quantum-classical approach.

Abstract

In a recent study [J. Liu et al., J. Chem. Phys. 149, 224104 (2018)], we developed a general mixed quantum-classical framework for studying heat transport through molecular junctions, in which the junction molecule is treated quantum mechanically and the thermal reservoirs to which the molecule is coupled are treated classically. This framework yields expressions for the transferred heat and steady-state heat current, which could be calculated using a variety of mixed quantum-classical dynamics methods. In this work, we use the recently developed "Deterministic Evolution of Coordinates with Initial Decoupled Equations" (DECIDE) method for calculating the steady-state heat current in the nonequilibrium spin-boson model in a variety of parameter regimes. Our results are compared and contrasted with those obtained using the numerically exact multilayer multiconfiguration time-dependent Hartree approach, and using approximate methods, including mean field theory, Redfield theory, and adiabatic mixed quantum-classical dynamics. Despite some quantitative differences, the DECIDE method performs quite well, is capable of capturing the expected trends in the steady-state heat current, and, overall, outperforms the approximate methods. These results hold promise for DECIDE simulations of nonequilibrium heat transport in realistic models of nanoscale systems.