Linear optical response of current-carrying molecular junction: A nonequilibrium Green’s function–time-dependent density functional theory approach

Abstract

We propose a scheme for calculation of linear optical response of current-carrying molecular junctions for the case when electronic tunneling through the junction is much faster than characteristic time of external laser field. We discuss relationships between nonequilibrium Green's function (NEGF) and time-dependent density functional theory (TDDFT) approaches and derive expressions for optical response and linear polarizability within NEGF-TDDFT scheme. Corresponding results for isolated molecule, derived within TDDFT approach previously, are reproduced when coupling to contacts is neglected.