Time-dependent density functional theory for open quantum systems with unitary propagation.
We extend the Runge-Gross theorem for a very general class of open quantum systems under weak assumptions about the nature of the bath and its coupling to the system. We show that for Kohn-Sham (KS) time-dependent density functional theory, it is possible to rigorously include the effects of the environment within a bath functional in the KS potential. A Markovian bath functional inspired by the theory of nonlinear Schrödinger equations is suggested, which can be readily implemented in currently existing real-time codes. Finally, calculations on a helium model system are presented.
Yuen-Zhou
Joel
J
Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street, 02138, Cambridge, Massachusetts, USA.
Tempel
David G
DG
Rodríguez-Rosario
César A
CA
Aspuru-Guzik
Alán
A