Trajectory surface hopping in the time-dependent Kohn-Sham approach for electron-nuclear dynamics

Phys Rev Lett. 2005 Oct 14;95(16):163001. doi: 10.1103/PhysRevLett.95.163001. Epub 2005 Oct 10.


The mean-field treatment of electron-nuclear interaction results in many qualitative breakdowns in the time-dependent Kohn-Sham (TDKS) density functional theory. Examples include current-induced heating in nanoelectronics, charge dynamics in quantum dots and carbon nanotubes, and relaxation of biological chromophores. The problem is resolved by the trajectory surface-hopping TDKS approach, which is illustrated by the photoinduced electron injection from a molecular chromophore into TiO2, and the excited-state relaxation of the green fluorescent protein chromophore.