Curing the Divergence in Time-Dependent Density Functional Quadratic Response Theory

This is the authors' abstract. We don't add key points for this paper.

The adiabatic approximation in time-dependent density functional theory 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.