Interactions between large molecules pose a puzzle for reference quantum mechanical methods

Yasmine S. Al-Hamdani, Péter R. Nagy, Andrea Zen, Dennis Barton, Mihály Kállay, Jan Gerit Brandenburg () and Alexandre Tkatchenko ()
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Yasmine S. Al-Hamdani: University of Zurich
Péter R. Nagy: Budapest University of Technology and Economics
Andrea Zen: Università di Napoli Federico II, Monte S. Angelo
Dennis Barton: University of Luxembourg
Mihály Kállay: Budapest University of Technology and Economics
Jan Gerit Brandenburg: Merck Data Office, Merck KGaA
Alexandre Tkatchenko: University of Luxembourg

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: Abstract Quantum-mechanical methods are used for understanding molecular interactions throughout the natural sciences. Quantum diffusion Monte Carlo (DMC) and coupled cluster with single, double, and perturbative triple excitations [CCSD(T)] are state-of-the-art trusted wavefunction methods that have been shown to yield accurate interaction energies for small organic molecules. These methods provide valuable reference information for widely-used semi-empirical and machine learning potentials, especially where experimental information is scarce. However, agreement for systems beyond small molecules is a crucial remaining milestone for cementing the benchmark accuracy of these methods. We show that CCSD(T) and DMC interaction energies are not consistent for a set of polarizable supramolecules. Whilst there is agreement for some of the complexes, in a few key systems disagreements of up to 8 kcal mol−1 remain. These findings thus indicate that more caution is required when aiming at reproducible non-covalent interactions between extended molecules.

Date: 2021
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DOI: 10.1038/s41467-021-24119-3

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