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  4. Equation of State of Fluid Methane from First Principles with Machine Learning Potentials
 
research article

Equation of State of Fluid Methane from First Principles with Machine Learning Potentials

Veit, Max  
•
Jain, Sandeep Kumar
•
Bonakala, Satyanarayana
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April 1, 2019
Journal of Chemical Theory and Computation

The predictive simulation of molecular liquids requires potential energy surface (PES) models that are not only accurate but also computationally efficient enough to handle the large systems and long time scales required for reliable prediction of macroscopic properties. We present a new approach to the systematic approximation of the first-principles PES of molecular liquids using the GAP (Gaussian Approximation Potential) framework. The approach allows us to create potentials at several different levels of accuracy in reproducing the true PES and thus to determine the level of quantum chemistry that is necessary to accurately predict macroscopic properties. We test the approach by building a series of many-body potentials for liquid methane (CH4), which is difficult to model from first principles because its behavior is dominated by weak dispersion interactions with a significant many-body component. The increasing accuracy of the potentials in predicting the bulk density correlates with their fidelity to the true PES, whereas the trend with the empirical potentials tested is surprisingly the opposite. We conclude that an accurate, consistent prediction of its bulk density across wide ranges of temperature and pressure requires not only many-body dispersion but also quantum nuclear effects to be modeled accurately.

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Type
research article
DOI
10.1021/acs.jctc.8b01242
Web of Science ID

WOS:000464475500038

Author(s)
Veit, Max  
Jain, Sandeep Kumar
Bonakala, Satyanarayana
Rudra, Indranil
Hohl, Detlef
Csanyi, Gabor
Date Issued

2019-04-01

Publisher

AMER CHEMICAL SOC

Published in
Journal of Chemical Theory and Computation
Volume

15

Issue

4

Start page

2574

End page

2586

Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

molecular-dynamics simulations

•

atom force-field

•

transferable potentials

•

phase-equilibria

•

alkane

•

hydrocarbons

•

energies

•

proteins

•

scheme

•

approximation

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
Available on Infoscience
June 18, 2019
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/157593
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