Development and validation of a general-purpose ReaxFF reactive force field for earth material modeling

Yingchun Zhang; Xiandong Liu; Adri C T van Duin; Xiancai Lu; Evert Jan Meijer

doi:10.1063/5.0194486

Development and validation of a general-purpose ReaxFF reactive force field for earth material modeling

J Chem Phys. 2024 Mar 7;160(9):094103. doi: 10.1063/5.0194486.

Authors

Yingchun Zhang^{1

2

3}, Xiandong Liu^{1

2}, Adri C T van Duin³, Xiancai Lu^{1

2}, Evert Jan Meijer⁴

Affiliations

¹ State Key Laboratory for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, Nanjing, Jiangsu 210023, People's Republic of China.
² Frontiers Science Center for Critical Earth Material Cycling, Nanjing University, Nanjing, Jiangsu 210023, People's Republic of China.
³ Department of Mechanical Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, USA.
⁴ Van 't Hoff Institute for Molecular Sciences, University of Amsterdam, Amsterdam 1012 WX, The Netherlands.

PMID: 38426512
DOI: 10.1063/5.0194486

Abstract

ReaxFF reactive force field bridges the gap between nonreactive molecular simulations and quantum mechanical calculations and has been widely applied during the past two decades. However, its application to earth materials, especially those under high T-P conditions relevant to Earth's interior, is still limited due to the lack of available parameters. Here, we present the development and validation of a ReaxFF force field containing several of the most common elements in Earth's crust, i.e., Si/Al/O/H/Na/K. The force field was trained against a large data set obtained from density functional theory (DFT) calculations, including charges, bond/angle distortion curves, equation of states, ion migration energy profiles, and condensation reaction energies. Different coordination environments were considered in the training set. The fitting results showed that the current force field can well reproduce the DFT data (the Pearson correlation coefficient, Rp, is 0.95). We validated the force field on mineral-water interfaces, hydrous melts/supercritical geofluids, and bulk crystals. It was found that the current force field performed excellently in predicting the structural, thermodynamic, and transport properties of various systems (Rp = 0.95). Moreover, possible applications and future development have been discussed. The results obtained in this study suggest that the current force field holds good promise to model a wide range of processes and thus open opportunities to advance the application of ReaxFF in earth material modeling.