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Reformulation of thermally assisted-occupation density functional theory in the Kohn-Sham framework.

Publication ,  Journal Article
Yeh, S-H; Yang, W; Hsu, C-P
Published in: The Journal of chemical physics
May 2022

We reformulate the thermally assisted-occupation density functional theory (TAO-DFT) into the Kohn-Sham single-determinant framework and construct two new post-self-consistent field (post-SCF) static correlation correction schemes, named rTAO and rTAO-1. In contrast to the original TAO-DFT with the density in an ensemble form, in which each orbital density is weighted with a fractional occupation number, the ground-state density is given by a single-determinant wavefunction, a regular Kohn-Sham (KS) density, and total ground state energy is expressed in the normal KS form with a static correlation energy formulated in terms of the KS orbitals. In post-SCF calculations with rTAO functionals, an efficient energy scanning to quantitatively determine θ is also proposed. The rTAOs provide a promising method to simulate systems with strong static correlation as original TAO, but simpler and more efficient. We show that both rTAO and rTAO-1 is capable of reproducing most results from TAO-DFT without the additional functional Eθ used in TAO-DFT. Furthermore, our numerical results support that, without the functional Eθ, both rTAO and rTAO-1 can capture correct static correlation profiles in various systems.

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Published In

The Journal of chemical physics

DOI

EISSN

1089-7690

ISSN

0021-9606

Publication Date

May 2022

Volume

156

Issue

17

Start / End Page

174108

Related Subject Headings

  • Chemical Physics
  • 51 Physical sciences
  • 40 Engineering
  • 34 Chemical sciences
  • 09 Engineering
  • 03 Chemical Sciences
  • 02 Physical Sciences
 

Citation

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Yeh, S.-H., Yang, W., & Hsu, C.-P. (2022). Reformulation of thermally assisted-occupation density functional theory in the Kohn-Sham framework. The Journal of Chemical Physics, 156(17), 174108. https://doi.org/10.1063/5.0087012
Yeh, Shu-Hao, Weitao Yang, and Chao-Ping Hsu. “Reformulation of thermally assisted-occupation density functional theory in the Kohn-Sham framework.The Journal of Chemical Physics 156, no. 17 (May 2022): 174108. https://doi.org/10.1063/5.0087012.
Yeh S-H, Yang W, Hsu C-P. Reformulation of thermally assisted-occupation density functional theory in the Kohn-Sham framework. The Journal of chemical physics. 2022 May;156(17):174108.
Yeh, Shu-Hao, et al. “Reformulation of thermally assisted-occupation density functional theory in the Kohn-Sham framework.The Journal of Chemical Physics, vol. 156, no. 17, May 2022, p. 174108. Epmc, doi:10.1063/5.0087012.
Yeh S-H, Yang W, Hsu C-P. Reformulation of thermally assisted-occupation density functional theory in the Kohn-Sham framework. The Journal of chemical physics. 2022 May;156(17):174108.

Published In

The Journal of chemical physics

DOI

EISSN

1089-7690

ISSN

0021-9606

Publication Date

May 2022

Volume

156

Issue

17

Start / End Page

174108

Related Subject Headings

  • Chemical Physics
  • 51 Physical sciences
  • 40 Engineering
  • 34 Chemical sciences
  • 09 Engineering
  • 03 Chemical Sciences
  • 02 Physical Sciences