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Universal Framework for Multiconfigurational DFT

Delcey, Mickael G. LU orcid (2025) In Journal of Chemical Theory and Computation 21(6). p.2952-2960
Abstract

Strong correlation remains a significant challenge for DFT with no satisfying solutions found yet within the standard Kohn-Sham framework. Instead, for decades, a number of different approaches have been suggested to combine the accuracy of multiconfigurational methods with the efficiency of DFT. In this article, we demonstrate that many of these methods are or would be significantly improved by being reformulated as variants of multiconfigurational pair-density functional theory (MC-PDFT). This work presents the first implementation of these methods within the recently proposed variational formulation of MC-PDFT. It also provides for the first time a systematic comparison of their accuracy across representative examples of strongly... (More)

Strong correlation remains a significant challenge for DFT with no satisfying solutions found yet within the standard Kohn-Sham framework. Instead, for decades, a number of different approaches have been suggested to combine the accuracy of multiconfigurational methods with the efficiency of DFT. In this article, we demonstrate that many of these methods are or would be significantly improved by being reformulated as variants of multiconfigurational pair-density functional theory (MC-PDFT). This work presents the first implementation of these methods within the recently proposed variational formulation of MC-PDFT. It also provides for the first time a systematic comparison of their accuracy across representative examples of strongly correlated systems. By analyzing their accuracy and formal properties, we provide design guidelines to inform the development of future functionals.

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Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Chemical Theory and Computation
volume
21
issue
6
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:40053889
  • scopus:105001083003
ISSN
1549-9618
DOI
10.1021/acs.jctc.4c01687
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2025 The Author. Published by American Chemical Society.
id
6f5959c2-5844-4a1c-bb9f-4362a654a516
date added to LUP
2025-08-22 15:07:59
date last changed
2025-08-22 15:08:41
@article{6f5959c2-5844-4a1c-bb9f-4362a654a516,
  abstract     = {{<p>Strong correlation remains a significant challenge for DFT with no satisfying solutions found yet within the standard Kohn-Sham framework. Instead, for decades, a number of different approaches have been suggested to combine the accuracy of multiconfigurational methods with the efficiency of DFT. In this article, we demonstrate that many of these methods are or would be significantly improved by being reformulated as variants of multiconfigurational pair-density functional theory (MC-PDFT). This work presents the first implementation of these methods within the recently proposed variational formulation of MC-PDFT. It also provides for the first time a systematic comparison of their accuracy across representative examples of strongly correlated systems. By analyzing their accuracy and formal properties, we provide design guidelines to inform the development of future functionals.</p>}},
  author       = {{Delcey, Mickael G.}},
  issn         = {{1549-9618}},
  language     = {{eng}},
  month        = {{03}},
  number       = {{6}},
  pages        = {{2952--2960}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Journal of Chemical Theory and Computation}},
  title        = {{Universal Framework for Multiconfigurational DFT}},
  url          = {{http://dx.doi.org/10.1021/acs.jctc.4c01687}},
  doi          = {{10.1021/acs.jctc.4c01687}},
  volume       = {{21}},
  year         = {{2025}},
}