Accurate Density Functional Theory for Non-Covalent Interactions in Charged Systems Article Swipe

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Heng Zhao , Balázs D. Lőrincz , Tobias Henkes , Dénes Berta , Péter R. Nagy , Alexandre Tkatchenko , Stefan Vuckovic ·

YOU? · · 2025 · Open Access · · DOI: https://doi.org/10.26434/chemrxiv-2025-jx112

Accurately modeling non-covalent interactions (NCIs) involving charged systems remains an outstanding challenge in Density Functional Theory (DFT), with implications across natural and life sciences, engineering, e.g., in biochemistry, catalysis, and materials science. For these interactions, the interplay between electrostatics, polarization, and dispersion leads to systematic errors of up to tens of kcal/mol in standard dispersion-enhanced DFT methods. We solve this problem by introducing (r2SCAN+MBD)@HF, a DFT method without empirically fitted parameters that combines the r2SCAN functional and many-body dispersion, both evaluated on Hartree-Fock densities. We show that the unique synergy of these three components enables balanced treatment of short- and long-range correlation, which is crucial for accurate description of NCIs involving charged systems. Evaluations on standard benchmarks and a new Metal Ion Protein Clusters dataset introduced here show that (r2SCAN+MBD)@HF significantly improves accuracy for NCIs involving charged systems while maintaining robust performance for neutral systems. Given the ubiquity of such interactions, (r2SCAN+MBD)@HF is broadly applicable from biochemistry and materials science, including for generating high-quality data to train machine-learning force fields.

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Density functional theory Covalent bond Computer science Physics Chemistry Computational chemistry Quantum mechanics

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Type: preprint
Language: en
Landing Page: https://doi.org/10.26434/chemrxiv-2025-jx112
PDF: https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/6823e916927d1c2e66a1e612/original/accurate-density-functional-theory-for-non-covalent-interactions-in-charged-systems.pdf
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DOI: https://doi.org/10.26434/chemrxiv-2025-jx112

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Title: Accurate Density Functional Theory for Non-Covalent Interactions in Charged Systems

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Type: preprint

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Language: en

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Publication year: 2025

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Publication date: 2025-05-19

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Authors: Heng Zhao, Balázs D. Lőrincz, Tobias Henkes, Dénes Berta, Péter R. Nagy, Alexandre Tkatchenko, Stefan Vuckovic

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Landing page: https://doi.org/10.26434/chemrxiv-2025-jx112

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PDF URL: https://chemrxiv.org/engage/api-gateway/chemrxiv/assets/orp/resource/item/6823e916927d1c2e66a1e612/original/accurate-density-functional-theory-for-non-covalent-interactions-in-charged-systems.pdf

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Concepts: Density functional theory, Covalent bond, Computer science, Physics, Chemistry, Computational chemistry, Quantum mechanics

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abstract_inverted_index.(r2SCAN+MBD)@HF,	63
abstract_inverted_index.machine-learning	167
abstract_inverted_index.dispersion-enhanced	54
cited_by_percentile_year
countries_distinct_count	3
institutions_distinct_count	7
citation_normalized_percentile.value	0.1578099
citation_normalized_percentile.is_in_top_1_percent	False
citation_normalized_percentile.is_in_top_10_percent	False