Path-integral simulations with fermionic and bosonic reservoirs: Transport and dissipation in molecular electronic junctions

Abstract: We expand iterative numerically-exact influence functional path-integral tools and present a method capable of following the nonequilibrium time evolution of subsystems coupled to multiple bosonic and fermionic reservoirs simultaneously. Using this method, we study the real-time dynamics of charge transfer and vibrational mode excitation in an electron conducting molecular junction. We focus on nonequilibrium vibrational effects, particularly, the development of vibrational instability in a current-rectifying junction. Our simulations are performed by assuming large molecular vibrational anharmonicity (or low temperature). This allows us to truncate the molecular vibrational mode to include only a two-state system. Exact numerical results are compared to perturbative Master equation calculations demonstrating an excellent agreement in the weak electron-phonon coupling regime. Significant deviations take place only at strong coupling. Our simulations allow us to quantify the contribution of different transport mechanisms, coherent dynamics and inelastic transport, in the overall charge current. This is done by studying two model variants: The first admits inelastic electron transmission only, while the second one allows for both coherent and incoherent pathways.