Recent Advances for Improving the Accuracy, Transferability, and Efficiency of Reactive Force Fields

I Leven and HX Hao and SC Tan and XY Guan and KA Penrod and D Akbarian and B Evangelisti and MJ Hossain and MM Islam and JP Koski and S Moore and HM Aktulga and ACT van Duin and T Head-Gordon, JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 17, 3237-3251 (2021).

DOI: 10.1021/acs.jctc.1c00118

Reactive force fields provide an affordable model for simulating chemical reactions at a fraction of the cost of quantum mechanical approaches. However, classically accounting for chemical reactivity often comes at the expense of accuracy and transferability, while computational cost is still large relative to nonreactive force fields. In this Perspective, we summarize recent efforts for improving the performance of reactive force fields in these three areas with a focus on the ReaxFF theoretical model. To improve accuracy, we describe recent reformulations of charge equilibration schemes to overcome unphysical long-range charge transfer, new ReaxFF models that account for explicit electrons, and corrections for energy conservation issues of the ReaxFF model. To enhance transferability we also highlight new advances to include explicit treatment of electrons in the ReaxFF and hybrid nonreactive/reactive simulations that make it possible to model charge transfer, redox chemistry, and large systems such as reverse micelles within the framework of a reactive force field. To address the computational cost, we review recent work in extended Lagrangian schemes and matrix preconditioners for accelerating the charge equilibration method component of ReaxFF and improvements in its software performance in LAMMPS.

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