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Investigating the Accuracy of Water Models through the Van Hove Correlation Function
journal contribution
posted on 2021-09-13, 21:04 authored by Ray A. Matsumoto, Matthew W. Thompson, Van Quan Vuong, Weiwei Zhang, Yuya Shinohara, Adri C. T. van Duin, Paul R. C. Kent, Stephan Irle, Takeshi Egami, Peter T. CummingsWe
present molecular-simulation-based calculations of the Van Hove
correlation function (VHF) of water using multiple modeling approaches:
classical molecular dynamics with simple three-site nonpolarizable
models, with a polarizable model, and with a reactive force field;
density functional tight-binding molecular dynamics; and ab
initio molecular dynamics. Due to the many orders of magnitude
difference in the computational cost of these approaches, we investigate
how small and short the simulations can be while still yielding sufficiently
accurate and interpretable results for the VHF. We investigate the
accuracy of the different models by comparing them to recently published
inelastic X-ray scattering measurements of the VHF. We find that all
of the models exhibit qualitative agreement with the experiments,
and in some models and for some properties, the agreement is quantitative.
This work lays the foundation for future simulation approaches to
calculating the VHF for aqueous solutions in bulk and under nanoconfinement.
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reactive force fieldray scattering measurementsdensity functional tightab initio classical molecular dynamicsbinding molecular dynamicssite nonpolarizable modelsfuture simulation approachesmolecular dynamicspresent molecularwork layswater modelssimple threepolarizable modelmany ordersmagnitude differenceinterpretable resultsdifferent modelscomputational costbased calculationsaqueous solutions