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Approximately self-consistent ensemble density functional theory: toward inclusion of all correlations
preprintrevised on 22.10.2020, 19:39 and posted on 23.10.2020, 06:49 by Tim Gould
Recent theory developments in ensemble density functional theory (EDFT) promise to bring decades of work for ground-states to the practical resolution of excited-states - provided newly-discovered "density-driven correlations" can be dealt with and adequate effective potentials can be found. This Letter introduces simple theories for both; and shows that EDFT using these theories outperforms ΔSCF DFT and time-dependent DFT for low-lying gaps in most of the small atoms and molecules tested, even when all use the same density functional approximations. It thus establishes EDFT as a promising tool for low-cost studies of excited states; and provides a clear route to practical EDFT implementation of arbitrary functional approximations.
Read the published paper
in The Journal of Physical Chemistry Letters