First-Principles Method for Open Electronic Systems

We prove the existence of the exact density-functional theory formalism for open electronic systems, and develop subsequently an exact time-dependent density-functional theory (TDDFT) formulation for the dynamic response. The TDDFT formulation depends in principle only on the electron density of the reduced system. Based on the nonequilibrium Green's function technique, it is expressed in the form of the equation of motion for the reduced single-electron density matrix, and this provides thus an efficient numerical approach to calculate the dynamic properties of open electronic systems. In the steady-state limit, the conventional first-principles nonequilibrium Green's function formulation for the current is recovered.