Daniel J. Sharpe
Approximating the Shifted Hartree-Exchange-Correlation Potential in Direct Energy Kohn–Sham Theory
Sharpe, Daniel J.; Levy, Mel; Tozer, David J.
Professor David Tozer email@example.com
Levy and Zahariev [Phys. Rev. Lett. 113 113002 (2014)] have proposed a new approach for performing density functional theory calculations, termed direct energy Kohn–Sham (DEKS) theory. In this approach, the electronic energy equals the sum of orbital energies, obtained from Kohn–Sham-like orbital equations involving a shifted Hartree-exchange-correlation potential, which must be approximated. In the present study, density scaling homogeneity considerations are used to facilitate DEKS calculations on a series of atoms and molecules, leading to three nonlocal approximations to the shifted potential. The first two rely on preliminary Kohn–Sham calculations using a standard generalized gradient approximation (GGA) exchange-correlation functional and the results illustrate the benefit of describing the dominant Hartree component of the shift exactly. A uniform electron gas analysis is used to eliminate the need for these preliminary Kohn–Sham calculations, leading to a potential with an unconventional form that yields encouraging results, providing strong motivation for further research in DEKS theory.
Sharpe, D. J., Levy, M., & Tozer, D. J. (2018). Approximating the Shifted Hartree-Exchange-Correlation Potential in Direct Energy Kohn–Sham Theory. Journal of Chemical Theory and Computation, 14(2), 684-692. https://doi.org/10.1021/acs.jctc.7b01060
|Journal Article Type||Article|
|Acceptance Date||Jan 3, 2018|
|Online Publication Date||Jan 3, 2018|
|Publication Date||Mar 1, 2018|
|Deposit Date||Jan 24, 2018|
|Publicly Available Date||Jan 3, 2019|
|Journal||Journal of Chemical Theory and Computation|
|Publisher||American Chemical Society|
|Peer Reviewed||Peer Reviewed|
Accepted Journal Article
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Chemical Theory and Computation, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jctc.7b01060.
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