TY - JOUR
T1 - Recent Advances for Improving the Accuracy, Transferability, and Efficiency of Reactive Force Fields
AU - Leven, Itai
AU - Hao, Hongxia
AU - Tan, Songchen
AU - Guan, Xingyi
AU - Penrod, Katheryn A.
AU - Akbarian, Dooman
AU - Evangelisti, Benjamin
AU - Hossain, Md Jamil
AU - Islam, Md Mahbubul
AU - Koski, Jason P.
AU - Moore, Stan
AU - Aktulga, Hasan Metin
AU - Van Duin, Adri C.T.
AU - Head-Gordon, Teresa
N1 - Funding Information:
This work was supported by the National Science Foundation under Grant CHE-1955643 (I.L. and T.H.-G.). We also acknowledge the CPIMS program by the Director, Office of Science, Office of Basic Energy Sciences, Chemical Sciences Division of the U.S. Department of Energy, under Contract No. DE-AC02-05CH11231 for the reverse micelle study (X.G., H.H., I.L., T.H.-G.). S.T. thanks the University of California Education Aboard Program (UCEAP) for financial and visa support. M.A. was supported in part by a Strategic Partnership Grant from the Michigan State University Foundation, an NSF CDS&E grant (award number 1807622), and an NIH grant (award number GM130641). A.C.T.v.D., K.A.P., D.A. B.E., and Md.J.H. were supported by NSF CDS&E grant no. 1807622, the U.S. Army Research Laboratory through the Collaborative Research Alliance for Multi-Scale Multidisciplinary Modeling of Electronic Materials (MSME) under Cooperative Agreement No. W911NF- 12-2-0023, and NSF NRT Grant No. DGE-1449785. This work used computational resources provided by the Institute for Cyber-Enabled Research at Michigan State University and the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231. This project was supported by LDRD project 218473. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the US Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. This work describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the work do not necessarily represent the views of the US Department of Energy or the United States Government.
Publisher Copyright:
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PY - 2021/6/8
Y1 - 2021/6/8
N2 - 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.
AB - 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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U2 - 10.1021/acs.jctc.1c00118
DO - 10.1021/acs.jctc.1c00118
M3 - Review article
C2 - 33970642
AN - SCOPUS:85106457731
VL - 17
SP - 3237
EP - 3251
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
SN - 1549-9618
IS - 6
ER -