Undoing static correlation: Long-range charge transfer in time-dependent density functional theory
Chemical Physics
2009-11-11 v1 Materials Science
Abstract
Long-range charge transfer excited states are notoriously badly underestimated in time-dependent density functional theory (TDDFT). We resolve how {\it exact} TDDFT captures charge transfer between open-shell species: in particular the role of the step in the ground-state potential, and the severe frequency-dependence of the exchange-correlation kernel. An expression for the latter is derived, that becomes exact in the limit that the charge-transfer excitations are well-separated from other excitations. The exchange-correlation kernel has the task of undoing the static correlation in the ground state introduced by the step, in order to accurately recover the physical charge-transfer states.
Cite
@article{arxiv.physics/0502147,
title = {Undoing static correlation: Long-range charge transfer in time-dependent density functional theory},
author = {Neepa T. Maitra},
journal= {arXiv preprint arXiv:physics/0502147},
year = {2009}
}
Comments
2 figures