A multilayer multiconfigurational time-dependent Hartree study of vibrationally coupled electron transport using the scattering state representation

TL;DR

This paper presents an efficient computational approach using a multilayer multiconfiguration time-dependent Hartree method combined with scattering state representation to study vibrationally coupled electron transport in single molecule junctions, enabling accurate steady-state current simulations.

Contribution

It introduces a scattering state-based Hamiltonian representation that reduces artificial electron correlation, improving simulation efficiency for vibrationally coupled charge transport.

Findings

Reduced artificial electron correlation with scattering state representation

Efficient simulation of steady-state currents across various parameters

Numerical examples demonstrating method effectiveness

Abstract

The multilayer multiconfiguration time-dependent Hartree method is employed to study vibrationally coupled charge transport in models of single molecule junctions. To increase the efficiency of the simulation method, a representation of the Hamiltonian in terms of the scattering states of the underlying electronic Hamiltonian is used. It is found that with an appropriate choice of the scattering states the artificial electron correlation present in the original representation of the model is greatly reduced. This allows efficient simulation of the steady-state currents in a wide physical parameter space, which is demonstrated by several numerical examples.