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

Journal of Chemical Theory and Computation
Max VeitG Csányi

Abstract

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 requir...Continue Reading

References

Feb 1, 1996·Journal of Molecular Graphics·W HumphreyK Schulten
Mar 1, 1985·Physical Review A: General Physics·W G Hoover
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Jul 23, 2004·The Journal of Chemical Physics·D Quigley, M I J Probert
Aug 31, 2004·The Journal of Chemical Physics·X Chu, A Dalgarno
Oct 8, 2004·Journal of Computational Chemistry·Joseph M HayesDavid A Morton-Blake
Jan 18, 2006·The Journal of Chemical Physics·Axel D Becke, Erin R Johnson
Aug 25, 2006·The Journal of Physical Chemistry. a·Rafał PodeszwaKrzysztof Szalewicz
Sep 7, 2006·Journal of Computational Chemistry·Stefan Grimme
May 16, 2007·Physical Review Letters·Jörg Behler, Michele Parrinello
Dec 18, 2007·The Journal of Chemical Physics·Thomas B AdlerHans-Joachim Werner
Jun 10, 2008·The Journal of Chemical Physics·Robert HellmannEckhard Vogel
Dec 19, 2008·Journal of Computational Chemistry·Shih-Wei ChaoSheng D Chao
Feb 12, 2009·The Journal of Chemical Physics·Gerald KniziaHans-Joachim Werner
Feb 21, 2009·Journal of Computational Chemistry·L MartínezJ M Martínez
Mar 5, 2009·Physical Review Letters·Alexandre Tkatchenko, Matthias Scheffler
Aug 8, 2009·Physical Review Letters·Michele CeriottiMichele Parrinello
May 21, 2010·Physical Review Letters·Albert P BartókGábor Csányi
Oct 5, 2010·The Journal of Chemical Physics·Michele CeriottiDavid E Manolopoulos
Sep 8, 2011·The Journal of Chemical Physics·Andrew Jones, Ben Leimkuhler
Dec 20, 2011·Chemical Reviews·Liguo KongEdward F Valeev
Sep 26, 2012·Physical Review Letters·Alexandre TkatchenkoMatthias Scheffler
Sep 26, 2012·Physical Review Letters·Michele Ceriotti, David E Manolopoulos
Jan 7, 2014·The Journal of Chemical Physics·M J GillanG Csányi
May 17, 2014·The Journal of Chemical Physics·Alberto AmbrosettiAlexandre Tkatchenko
Nov 18, 2015·Journal of Chemical Theory and Computation·Tristan BereauO Anatole von Lilienfeld
Apr 9, 2016·Journal of Chemical Theory and Computation·Daniel J ColeWilliam L Jorgensen
Apr 15, 2016·Chemical Reviews·Stefan GrimmeChristoph Bannwarth
Apr 23, 2016·Physical Chemistry Chemical Physics : PCCP·Sandip DeMichele Ceriotti
Jun 24, 2016·Journal of Chemical Theory and Computation·Mary J Van VleetJ R Schmidt
Jul 13, 2016·Proceedings of the National Academy of Sciences of the United States of America·Tobias MorawietzJörg Behler
Dec 10, 2016·Journal of Chemical Theory and Computation·Steven VandenbrandeToon Verstraelen
Dec 25, 2016·The Journal of Chemical Physics·Venkat KapilMichele Ceriotti
Feb 17, 2017·Journal of Cheminformatics·Sandip DeMichele Ceriotti
Mar 23, 2017·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Ask Hjorth LarsenKarsten W Jacobsen
May 11, 2017·Journal of Chemical Theory and Computation·Robert M ParrishC David Sherrill
Aug 29, 2017·Science Advances·Ciprian G PruteanuJohn S Loveday
Sep 30, 2017·Chemical Science·Alexander G ShtukenbergBart Kahr
Apr 1, 1986·Journal of Computational Chemistry·Scott J WeinerDavid A Case
Nov 22, 2017·Journal of Chemical Theory and Computation·Alice E A AllenDaniel J Cole
Dec 16, 2017·Science Advances·Albert P BartókMichele Ceriotti
Dec 22, 2017·Journal of Chemical Theory and Computation·Mary J Van VleetJ R Schmidt
May 15, 2018·The Journal of Physical Chemistry Letters·Volker L DeringerGábor Csányi
May 15, 2018·Physical Review Letters·Volker L DeringerGábor Csányi
May 15, 2018·Physical Review Letters·Miguel A CaroGábor Csányi

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Citations

Jul 17, 2020·The Journal of Chemical Physics·Max VeitMichele Ceriotti
Dec 10, 2020·The Journal of Chemical Physics·Janus J Eriksen
Jun 11, 2020·Chemical Reviews·Kevin Maik JablonkaBerend Smit
Mar 24, 2021·The Journal of Chemical Physics·Félix MusilMichele Ceriotti
Nov 20, 2020·Chemical Reviews·Julia Westermayr, Philipp Marquetand
Jun 25, 2021·Chemical Science·Andrea GrisafiMichele Ceriotti
Jul 27, 2021·Chemical Reviews·Felix MusilMichele Ceriotti
Jun 20, 2020·Journal of Chemical Theory and Computation·Paraskevi GkekaTony Lelièvre
Aug 17, 2021·Chemical Reviews·Volker L DeringerGábor Csányi
Oct 12, 2019·Journal of Chemical Theory and Computation·Jonny ProppeMarkus Reiher
Nov 25, 2020·The Journal of Physical Chemistry. B·Marc RieraFrancesco Paesani
Nov 10, 2020·Chemical Reviews·Peng XuMark S Gordon
Jan 17, 2020·Journal of Chemical Theory and Computation·Verena A Neufeld, Alex J W Thom
Sep 4, 2021·Chemical Science·Tom A YoungFernanda Duarte
Jun 4, 2021··Yuliana ZamoraHenry Hoffmann

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