Regularized and Opposite Spin-Scaled Functionals from Møller-Plesset Adiabatic Connection─Higher Accuracy at Lower Cost

Kimberly J. Daas; Derk P. Kooi; Nina C. Peters; Eduardo Fabiano; Fabio Della Sala; Paola Gori-Giorgi; Stefan Vuckovic

doi:10.1021/acs.jpclett.3c01832

Regularized and Opposite Spin-Scaled Functionals from Møller-Plesset Adiabatic Connection─Higher Accuracy at Lower Cost

Kimberly J. Daas, Derk P. Kooi, Nina C. Peters, Eduardo Fabiano, Fabio Della Sala, Paola Gori-Giorgi, Stefan Vuckovic^*

^*Corresponding author for this work

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Abstract

Noncovalent interactions (NCIs) play a crucial role in biology, chemistry, material science, and everything in between. To improve pure quantum-chemical simulations of NCIs, we propose a methodology for constructing approximate correlation energies by combining an interpolation along the Møller-Plesset adiabatic connection (MP AC) with a regularization and spin-scaling strategy applied to MP2 correlation energies. This combination yields c_osκ_os-SPL2, which exhibits superior accuracy for NCIs compared to any of the individual strategies. With the N⁴ formal scaling, c_osκ_os-SPL2 is competitive or often outperforms more expensive dispersion-corrected double hybrids for NCIs. The accuracy of c_osκ_os-SPL2 particularly shines for anionic halogen bonded complexes, where it surpasses standard dispersion-corrected DFT by a factor of 3 to 5.

Original language	English
Pages (from-to)	8448-8459
Number of pages	12
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	38
Early online date	18 Sept 2023
DOIs	https://doi.org/10.1021/acs.jpclett.3c01832
Publication status	Published - 28 Sept 2023

Bibliographical note

Funding Information:
SV acknowledges funding from the SNSF Starting Grant project (TMSGI2_211246). KJD, DPK, and PG-G acknowledge financial support from The Netherlands Organisation for Scientific Research under Vici grant 724.017.001. FDS is grateful for the financial support from ICSC – Centro Nazionale di Ricerca in High Performance Computing, Big Data and Quantum Computing, funded by European Union – NextGenerationEU – PNRR. We want to thank Arno Förster for calculating the aug-QZ6P B2PLYP-D3 data for X40 and for fruitful discussions regarding this work. We also want to thank Suhwan Song for providing his MP2 data for the B30 data set and Lucas de Azevedo Santos and Klaas Giesbertz for insightful discussions.

Publisher Copyright:
© 2023 American Chemical Society

Funding

SV acknowledges funding from the SNSF Starting Grant project (TMSGI2_211246). KJD, DPK, and PG-G acknowledge financial support from The Netherlands Organisation for Scientific Research under Vici grant 724.017.001. FDS is grateful for the financial support from ICSC – Centro Nazionale di Ricerca in High Performance Computing, Big Data and Quantum Computing, funded by European Union – NextGenerationEU – PNRR. We want to thank Arno Förster for calculating the aug-QZ6P B2PLYP-D3 data for X40 and for fruitful discussions regarding this work. We also want to thank Suhwan Song for providing his MP2 data for the B30 data set and Lucas de Azevedo Santos and Klaas Giesbertz for insightful discussions.

Funders	Funder number
Centro Nazionale di Ricerca
International Council of Shopping Centers
European Commission
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	TMSGI2_211246
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	724.017.001
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

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10.1021/acs.jpclett.3c01832

Daas-et-al-2023_Regularized-and-opposite-spin-scaled-functionals-from-møller-plesset-adiabatic-connection-higherFinal published version, 3.89 MBLicence: Article 25fa Dutch Copyright Act

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abstract = "Noncovalent interactions (NCIs) play a crucial role in biology, chemistry, material science, and everything in between. To improve pure quantum-chemical simulations of NCIs, we propose a methodology for constructing approximate correlation energies by combining an interpolation along the M{\o}ller-Plesset adiabatic connection (MP AC) with a regularization and spin-scaling strategy applied to MP2 correlation energies. This combination yields cosκos-SPL2, which exhibits superior accuracy for NCIs compared to any of the individual strategies. With the N4 formal scaling, cosκos-SPL2 is competitive or often outperforms more expensive dispersion-corrected double hybrids for NCIs. The accuracy of cosκos-SPL2 particularly shines for anionic halogen bonded complexes, where it surpasses standard dispersion-corrected DFT by a factor of 3 to 5.",

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note = "Funding Information: SV acknowledges funding from the SNSF Starting Grant project (TMSGI2_211246). KJD, DPK, and PG-G acknowledge financial support from The Netherlands Organisation for Scientific Research under Vici grant 724.017.001. FDS is grateful for the financial support from ICSC – Centro Nazionale di Ricerca in High Performance Computing, Big Data and Quantum Computing, funded by European Union – NextGenerationEU – PNRR. We want to thank Arno F{\"o}rster for calculating the aug-QZ6P B2PLYP-D3 data for X40 and for fruitful discussions regarding this work. We also want to thank Suhwan Song for providing his MP2 data for the B30 data set and Lucas de Azevedo Santos and Klaas Giesbertz for insightful discussions. Publisher Copyright: {\textcopyright} 2023 American Chemical Society",

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Regularized and Opposite Spin-Scaled Functionals from Møller-Plesset Adiabatic Connection─Higher Accuracy at Lower Cost

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