Inelastic effects in molecular transport junctions: The probe technique at high bias

TL;DR

This paper extends the Landauer-Büttiker probe formalism to high bias regimes in molecular junctions, revealing how inelastic scattering induces rectification and affects current-voltage characteristics.

Contribution

It introduces a phenomenological probe technique for modeling inelastic effects at high bias, highlighting the emergence of diode-like behavior due to incoherent scattering.

Findings

Inelastic scattering causes asymmetry and rectification in molecular junctions.

Dephasing and voltage probes behave similarly at low bias but differ significantly at high bias.

Inelastic effects are crucial for accurate modeling of molecular electronic transport far from equilibrium.

Abstract

We extend the Landauer-B\"uttiker probe formalism for conductances to the high bias regime, and study the effects of environmentally-induced elastic and inelastic scattering on charge current in single molecule junctions, focusing on high-bias effects. The probe technique phenomenologically incorporates incoherent elastic and inelastic effects to the fully coherent case, mimicking a rich physical environment at trivial cost. We further identify environmentally-induced mechanisms which generate an asymmetry in the current, manifested as a weak diode behavior. This rectifying behavior, found in two types of molecular junction models, is absent in the coherent-elastic limit, and is only active in the case with incoherent-inelastic scattering. Our work illustrates that in the low bias - linear response regime, the commonly used "dephasing probe" (mimicking only elastic decoherence effects) operates nearly indistinguishably from a "voltage probe" (admitting inelastic-dissipative effects). However, these probes realize fundamentally distinct $I$-$V$ characteristics at high biases, reflecting the central roles of dissipation and inelastic scattering processes on molecular electronic transport far-from-equilibrium.