Universal Framework for Multiconfigurational DFT
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| Title: | Universal Framework for Multiconfigurational DFT |
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| Authors: | Delcey, Mickael G. |
| Contributors: | Lund University, Faculty of Science, Department of Chemistry, Physical and theoretical chemistry, Computational Chemistry, Lunds universitet, Naturvetenskapliga fakulteten, Kemiska institutionen, Enheten för fysikalisk och teoretisk kemi, Beräkningskemi, Originator |
| Source: | Journal of Chemical Theory and Computation. 21(6):2952-2960 |
| Subject Terms: | Natural Sciences, Chemical Sciences, Theoretical Chemistry (including Computational Chemistry), Naturvetenskap, Kemi, Teoretisk kemi (Här ingår: Beräkningskemi), Mathematical Sciences, Computational Mathematics, Matematik, Beräkningsmatematik |
| Description: | 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. |
| Access URL: | https://doi.org/10.1021/acs.jctc.4c01687 |
| Database: | SwePub |
Nájsť tento článok vo Web of Science | 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 correlated systems. By analyzing their accuracy and formal properties, we provide design guidelines to inform the development of future functionals. |
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| ISSN: | 15499618 15499626 |
| DOI: | 10.1021/acs.jctc.4c01687 |