Density-functional theory of nonequilibrium tunneling

TL;DR

This paper develops a comprehensive density functional theory framework for modeling nonequilibrium tunneling in nanoscale systems, incorporating full electron-electron interactions and providing a variational principle for steady-state transport.

Contribution

It introduces a Lippmann-Schwinger collision DFT that explicitly accounts for many-body interactions in tunneling, extending beyond standard ground-state DFT methods.

Findings

Formulates a variational principle for nonequilibrium density.

Expresses many-body scattering matrices via universal density functionals.

Provides an exact reformulation using quantum-kinetic equations.

Abstract

Nanoscale optoelectronics and molecular-electronics systems operate with current injection and nonequilibrium tunneling, phenomena that challenge consistent descriptions of the steady-state transport. The current affects the electron-density variation and hence the inter- and intra-molecular bonding which in turn determines the transport magnitude. The standard approach for efficient characterization of steady-state tunneling combines ground-state density functional theory (DFT) calculations (of an effective scattering potential) with a Landauer-type formalism and ignores all actual many-body scattering. The standard method also lacks a formal variational basis. This paper formulates a Lippmann-Schwinger collision density functional theory (LSC-DFT) for tunneling transport with full electron-electron interactions. Quantum-kinetic (Dyson) equations are used for an exact reformulation that expresses the variational noninteracting and interacting many-body scattering T-matrices in terms of universal density functionals. The many-body Lippmann-Schwinger (LS) variational principle defines an implicit equation for the exact nonequilibrium density.