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Quantum Dynamics of Water from Møller-Plesset Perturbation Theory via a Neural Network Potential

Year:    2025

Author:    Mengxu Li, Jinggang Lan, David M. Wilkins, Vladimir V. Rybkin, Marcella Iannuzzi, Jürg Hutter

Communications in Computational Chemistry, Vol. 7 (2025), Iss. 2 : pp. 88–96

Abstract

We report the static and dynamical properties of liquid water at the level of second-order Møller-Plesset perturbation theory (MP2) with classical and quantum nuclear dynamics using a neural network potential. We examined the temperature-dependent radial distribution functions, diffusion, and vibrational dynamics. MP2 theory predicts over-structured liquid water as well as a lower diffusion coefficient at ambient conditions compared to experiments, which may be attributed to the incomplete basis set. A better agreement with experimental structural properties and the diffusion constant are observed at an elevated temperature of 340 K from our simulations. Although the high-level electronic structure calculations are expensive, training a neural network potential requires only a few thousand frames. This approach shows great potential, requiring modest human effort, and is straightforwardly extensible to other simple liquids.

Journal Article Details

Publisher Name:    Global Science Press

Language:    English

DOI:    https://doi.org/10.4208/cicc.2025.88.01

Communications in Computational Chemistry, Vol. 7 (2025), Iss. 2 : pp. 88–96

Published online:    2025-01

AMS Subject Headings:    Global Science Press

Copyright:    COPYRIGHT: © Global Science Press

Pages:    9

Keywords:    MP2 machine learning quantum simulation diffusion coefficient.

Author Details

Mengxu Li

Jinggang Lan

David M. Wilkins

Vladimir V. Rybkin

Marcella Iannuzzi

Jürg Hutter