Curing the Divergence in Time-Dependent Density Functional Quadratic Response Theory
Chemical Physics
2023-05-01 v3
Abstract
The adiabatic approximation in time-dependent density functional theory (TDDFT) is known to give an incorrect pole structure in the quadratic response function, leading to unphysical divergences in excited state-to-state transition probabilities and hyperpolarizabilties. We find the form of the exact quadratic response kernel and derive a practical and accurate approximation that cures the divergence. We demonstrate our results on excited state-to-state transition probabilities of a model system and of the LiH molecule.
Keywords
Cite
@article{arxiv.2211.09885,
title = {Curing the Divergence in Time-Dependent Density Functional Quadratic Response Theory},
author = {Davood Dar and Saswata Roy and Neepa T. Maitra},
journal= {arXiv preprint arXiv:2211.09885},
year = {2023}
}