The description of complex time-dependent processes in molecular junctions from quantum mechanical principles can be very challenging. This challenge takes a particular form when this complexity originates in the coupling of the electronic levels in the molecule to molecular vibrations. In this case, a natural assumption that permits efficient descriptions is that classical mechanics accurately describes the nuclear motion. In this spirit, we present a practical quantum-classical formalism for electron transport that integrates Nonequilibrium Green Functions (NEGF) and classical stochastic equations of motion. This formalism is perturbative in the electron-vibration strength and can be efficiently used to propagate the system at room temperature. We implement our formalism in model systems and investigate the current statistic and the effect of environmental noise in the transient regime induced by mechanical and optical stimuli. We also illustrate the advantages of our method by studying the impact of classical vibrational coherence in the electronic transport. Our approach provides an alternative to assess the performance of molecular junctions at room temperature, their response to mechanical perturbations, and coherent molecular motion.

Semiclassical theory of transient transport in molecular junctions with electron-vibration couplings

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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