Excited-State Densities from Time-Dependent Density Functional Response Theory
Anna Baranova, Neepa T. Maitra
TL;DR
This paper introduces a new method to calculate excited-state densities using time-dependent density functional theory, focusing on double-excitation states.
Contribution
The paper derives a real-space expression for excited-state densities that includes nonadiabatic kernels, enabling accurate double-excitation density calculations.
Findings
The derived method successfully yields densities for states with double-excitation character.
The local-density and exact-exchange approximations show distinct performance on local and charge-transfer excitations.
The dressed TDDFT approach provides good results for double-excitation densities under certain simplifications.
Abstract
While the variational principle for excited-state energies leads to a route to obtaining excited-state densities from time-dependent density functional theory, relatively little attention has been paid to the quality of the resulting densities in real space obtained with different exchange-correlation functional approximations or how nonadiabatic approximations developed for energies of states of double-excitation character perform for their densities. Here we derive an expression directly in real space for the excited-state density, which includes the case of nonadiabatic kernels and consequently is able, for the first time, to yield densities of states of double-excitation character. Under some well-defined simplifications, we compare the performance of the local-density approximation and exact-exchange approximation, which are in a sense at the opposite extremes of the fundamental…
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Taxonomy
TopicsSpectroscopy and Quantum Chemical Studies · Photochemistry and Electron Transfer Studies · Advanced Chemical Physics Studies