N.N. Lathiotakis
Local reduced-density-matrix-functional theory: Incorporating static correlation effects in Kohn-Sham equations
Lathiotakis, N.N.; Helbig, N.; Rubio, A.; Gidopoulos, N.I.
Authors
Abstract
We propose a scheme to bring reduced-density-matrix-functional theory into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately static and left-right correlation effects in molecules and keeping the good computational performance of DFT-based schemes. The key ingredient is to relax the requirement that the local potential is the functional derivative of the energy with respect to the density. Instead, we propose to restrict the search for the approximate natural orbitals within a domain where these orbitals are eigenfunctions of a single-particle Hamiltonian with a local effective potential. In this way, fractional natural occupation numbers are accommodated into Kohn-Sham equations allowing for the description of molecular dissociation without breaking spin symmetry. Additionally, our scheme provides a natural way to connect an energy eigenvalue spectrum to the approximate natural orbitals and this spectrum is found to represent accurately the ionization potentials of atoms and small molecules.
Citation
Lathiotakis, N., Helbig, N., Rubio, A., & Gidopoulos, N. (2014). Local reduced-density-matrix-functional theory: Incorporating static correlation effects in Kohn-Sham equations. Physical Review A, 90(3), Article 032511. https://doi.org/10.1103/physreva.90.032511
Journal Article Type | Article |
---|---|
Acceptance Date | Apr 28, 2014 |
Online Publication Date | Sep 24, 2014 |
Publication Date | Sep 24, 2014 |
Deposit Date | Sep 26, 2014 |
Publicly Available Date | Oct 2, 2014 |
Journal | Physical Review A |
Print ISSN | 1050-2947 |
Electronic ISSN | 1094-1622 |
Publisher | American Physical Society |
Peer Reviewed | Peer Reviewed |
Volume | 90 |
Issue | 3 |
Article Number | 032511 |
DOI | https://doi.org/10.1103/physreva.90.032511 |
Public URL | https://durham-repository.worktribe.com/output/1453568 |
Related Public URLs | http://arxiv.org/abs/1407.7128 |
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Copyright Statement
Reprinted with permission from the American Physical Society: Physical Review A 90, 032511 © 2014 by the American Physical Society. Readers may view, browse, and/or download material for temporary copying purposes only, provided these uses are for noncommercial personal purposes. Except as provided by law, this material may not be further reproduced, distributed, transmitted, modified, adapted, performed, displayed, published, or sold in whole or part, without prior written permission from the American Physical Society.
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