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Title: Toward Automated Sampling of Polymorph Nucleation and Free Energies with the SGOOP and Metadynamics

Abstract

Understanding the driving forces behind the nucleation of different polymorphs is of great importance for material sciences and the pharmaceutical industry. This includes understanding the reaction coordinate that governs the nucleation process and correctly calculating the relative free energies of different polymorphs. Here, we demonstrate, for the prototypical case of urea nucleation from the melt, how one can learn such a one-dimensional reaction coordinate as a function of prespecified order parameters and use it to perform efficient biased all-atom molecular dynamics simulations. The reaction coordinate is learnt as a function of the generic thermodynamic and structural order parameters using the “spectral gap optimization of order parameters (SGOOP)” approach [Tiwary, P. and Berne, B. J. Proc. Natl. Acad. Sci. U.S.A. (2016)] and is biased using well-tempered metadynamics simulations. The reaction coordinate gives insights into the role played by different structural and thermodynamics order parameters, and the biased simulations obtain accurate relative free energies for different polymorphs. This includes an accurate prediction of the approximate pressure at which urea undergoes a phase transition and one of the metastable polymorphs becomes the most stable conformation. Here, we believe the ideas demonstrated in this work will facilitate efficient sampling of nucleation in complex, genericmore » systems.« less

Authors:
 [1];  [1]; ORCiD logo [1]
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  1. University of Maryland, College Park, MD (United States)
Publication Date:
Research Org.:
Univ. of Maryland, College Park, MD (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1991192
Grant/Contract Number:  
SC0021009
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B
Additional Journal Information:
Journal Volume: 125; Journal Issue: 47; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Computer simulations; Entropy; Free energy; Nucleation; Urea

Citation Formats

Zou, Ziyue, Tsai, Sun-Ting, and Tiwary, Pratyush. Toward Automated Sampling of Polymorph Nucleation and Free Energies with the SGOOP and Metadynamics. United States: N. p., 2021. Web. doi:10.1021/acs.jpcb.1c07595.
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Zou, Ziyue, Tsai, Sun-Ting, & Tiwary, Pratyush. Toward Automated Sampling of Polymorph Nucleation and Free Energies with the SGOOP and Metadynamics. United States. https://doi.org/10.1021/acs.jpcb.1c07595
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Zou, Ziyue, Tsai, Sun-Ting, and Tiwary, Pratyush. Wed . "Toward Automated Sampling of Polymorph Nucleation and Free Energies with the SGOOP and Metadynamics". United States. https://doi.org/10.1021/acs.jpcb.1c07595. https://www.osti.gov/servlets/purl/1991192.
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@article{osti_1991192,
title = {Toward Automated Sampling of Polymorph Nucleation and Free Energies with the SGOOP and Metadynamics},
author = {Zou, Ziyue and Tsai, Sun-Ting and Tiwary, Pratyush},
abstractNote = {Understanding the driving forces behind the nucleation of different polymorphs is of great importance for material sciences and the pharmaceutical industry. This includes understanding the reaction coordinate that governs the nucleation process and correctly calculating the relative free energies of different polymorphs. Here, we demonstrate, for the prototypical case of urea nucleation from the melt, how one can learn such a one-dimensional reaction coordinate as a function of prespecified order parameters and use it to perform efficient biased all-atom molecular dynamics simulations. The reaction coordinate is learnt as a function of the generic thermodynamic and structural order parameters using the “spectral gap optimization of order parameters (SGOOP)” approach [Tiwary, P. and Berne, B. J. Proc. Natl. Acad. Sci. U.S.A. (2016)] and is biased using well-tempered metadynamics simulations. The reaction coordinate gives insights into the role played by different structural and thermodynamics order parameters, and the biased simulations obtain accurate relative free energies for different polymorphs. This includes an accurate prediction of the approximate pressure at which urea undergoes a phase transition and one of the metastable polymorphs becomes the most stable conformation. Here, we believe the ideas demonstrated in this work will facilitate efficient sampling of nucleation in complex, generic systems.},
doi = {10.1021/acs.jpcb.1c07595},
journal = {Journal of Physical Chemistry. B},
number = 47,
volume = 125,
place = {United States},
year = {Wed Nov 17 00:00:00 EST 2021},
month = {Wed Nov 17 00:00:00 EST 2021}
}
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