On correlated electron-nuclear dynamics using time-dependent density functional theory

摘要

We discuss possibilities and challenges for describing correlated electron and nuclear dynamics within a surface-hopping framework using time-dependent density functional theory (TDDFT) for the electron dynamics.We discuss the recent surface-hopping method proposed by Craig et al.[Phys.Rev.Lett.95,163001 (2005)] that is based on Kohn-Sham potential energy surfaces.Limitations of this approach arise due to the Kohn-Sham surfaces generally having different gradients than the true TDDFT-corrected ones.Two mechanisms of the linear response procedure cause this effect:we illustrate these with examples.