Extending density functional theory with near chemical accuracy beyond pure water

Suhwan Song; Stefan Vuckovic; Youngsam Kim; Hayoung Yu; Eunji Sim; Kieron Burke

doi:10.1038/s41467-023-36094-y

Extending density functional theory with near chemical accuracy beyond pure water

Nat Commun. 2023 Feb 13;14(1):799. doi: 10.1038/s41467-023-36094-y.

Authors

Suhwan Song^{1

2}, Stefan Vuckovic^{3

4}, Youngsam Kim¹, Hayoung Yu¹, Eunji Sim⁵, Kieron Burke^{2

6}

Affiliations

¹ Department of Chemistry, Yonsei University, 50 Yonsei-ro Seodaemun-gu, Seoul, 03722, Korea.
² Department of Chemistry, University of California, Irvine, CA, 92697, USA.
³ Institute for Microelectronics and Microsystems (CNR-IMM), Via Monteroni, Campus Unisalento, 73100, Lecce, Italy.
⁴ Departments of Chemistry & Pharmaceutical Sciences and Amsterdam Institute of Molecular and Life Sciences (AIMMS), Faculty of Science, Vrije Universiteit, De Boelelaan 1083, 1081HV, Amsterdam, The Netherlands.
⁵ Department of Chemistry, Yonsei University, 50 Yonsei-ro Seodaemun-gu, Seoul, 03722, Korea. esim@yonsei.ac.kr.
⁶ Departments of Physics & Astronomy, University of California, Irvine, CA, 92697, USA.

Abstract

Density functional simulations of condensed phase water are typically inaccurate, due to the inaccuracies of approximate functionals. A recent breakthrough showed that the SCAN approximation can yield chemical accuracy for pure water in all its phases, but only when its density is corrected. This is a crucial step toward first-principles biosimulations. However, weak dispersion forces are ubiquitous and play a key role in noncovalent interactions among biomolecules, but are not included in the new approach. Moreover, naïve inclusion of dispersion in HF-SCAN ruins its high accuracy for pure water. Here we show that systematic application of the principles of density-corrected DFT yields a functional (HF-r²SCAN-DC4) which recovers and not only improves over HF-SCAN for pure water, but also captures vital noncovalent interactions in biomolecules, making it suitable for simulations of solutions.

Abstract

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