Transport through molecular junctions with a nonequilibrium phonon population

TL;DR

This paper investigates how nonequilibrium phonon populations influence the nonlinear conductance in single-molecule junctions, revealing significant differences from equilibrium cases especially at high transmission and long electron dwell times.

Contribution

It introduces a detailed analysis of the impact of bias-voltage-dependent phonon populations on the conductance, highlighting the role of electron-phonon interactions at low temperatures.

Findings

Logarithmic singularities and discontinuities in self energy at inelastic thresholds.

Differences in differential conductance are more pronounced with higher transmission.

Nonequilibrium phonon populations significantly alter conductance compared to equilibrium cases.

Abstract

The calculation of the nonlinear conductance of a single-molecule junction is revisited. The self energy on the junction resulting from the electron-phonon interaction has at low temperatures logarithmic singularities (in the real part) and discontinuities (in the imaginary one) at the frequencies corresponding to the opening of the inelastic channels. These singularities generate discontinuities and logarithmic divergences (as a function of the bias voltage) in the low-temperature differential conductance around the inelastic thresholds. The self energy also depends on the population of the vibrational modes. The case of a vibrating free junction (not coupled to a thermal bath), where the phonon population is determined by the bias voltage is examined. We compare the resulting zero-temperature differential conductance with the one obtained for equilibrated phonons, and find that the difference is larger the larger is the bare transmission of the junction and the product of the electron dwell time on the junction with the phonon frequency.