Simulation of optical response functions in molecular junctions

TL;DR

This paper develops theoretical methods for simulating nonlinear optical responses in molecular junctions, enabling detailed analysis of their optical properties considering intra-molecular interactions and contact effects.

Contribution

It introduces a Green function-based framework for calculating optical response functions in molecular junctions, including pseudoparticle nonequilibrium Green functions.

Findings

Derived expressions suitable for Green function techniques

Accounted for intra-molecular interactions and hybridization effects

Applied to two-dimensional optical spectroscopy in junctions

Abstract

We discuss theoretical approaches to nonlinear optical spectroscopy of molecular junctions. Optical response functions are derived in the form convenient for implementation of Green function techniques, and their expressions in terms of pseudoparticle nonequilibrium Green functions are proposed. The formulation allows to account for both intra-molecular interactions and hybridization of molecular states due to coupling to contacts. Two-dimensional optical spectroscopy in junctions is considered as an example.