Excited State Densities from Time-Dependent Density Functional Response Theory
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arXiv
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| Format: | Preprint |
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2025
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| _version_ | 1866915489636155392 |
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| author | Baranova, Anna Maitra, Neepa T. |
| author_facet | Baranova, Anna Maitra, Neepa T. |
| contents | 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, nor how non-adiabatic 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, that includes the case of non-adiabatic 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 opposite extremes of the fundamental functional approximations, on local and charge-transfer excitations in one-dimensional model systems, and show that the dressed TDDFT approach gives good densities of double-excitations. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2506_05082 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Excited State Densities from Time-Dependent Density Functional Response Theory Baranova, Anna Maitra, Neepa T. Chemical Physics 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, nor how non-adiabatic 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, that includes the case of non-adiabatic 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 opposite extremes of the fundamental functional approximations, on local and charge-transfer excitations in one-dimensional model systems, and show that the dressed TDDFT approach gives good densities of double-excitations. |
| title | Excited State Densities from Time-Dependent Density Functional Response Theory |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2506.05082 |