Time-dependent density-functional theory for open systems

Abstract

With our proof of the holographic electron density theorem for time-dependent systems, a first-principles method for any open electronic system is established. By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the Kohn-Sham reduced single-electron density matrix of the reduced system. Two approximate schemes are proposed for the dissipative interactions, the complete second-order approximation and the wide-band limit approximation. A numerical method based on the wide-band limit approximation is subsequently developed and implemented to simulate the steady and transient current through various realistic molecular devices. Simulation results are presented and discussed.