Optimization of the Reax force field for the lithium-oxygen system using a high fidelity charge model

Kurt A. O'Hearn, Michael W. Swift, Jialin Liu, Ilias Magoulas, Piotr Piecuch, Adri C.T. Van Duin, H. Metin Aktulga, Yue Qi

Research output: Contribution to journalArticlepeer-review

10 Scopus citations


Studies using molecular dynamics (MD) have long struggled to simulate the failure modes of materials, predicting unrealistically high ductility and failing to capture brittle fracture. The primary cause of this shortcoming is an inadequate description of bond breaking. While reactive force fields such as ReaxFF show improvements compared to traditional force fields, the charge models used yield unphysical partial charges, especially during dissociation of ionic bonds. This flaw may be remedied by using the atom-condensed Kohn-Sham density functional theory (DFT) approximated to a second order (ACKS2) charge model for determining partial charges. In this work, we present a new ACKS2- enabled Reax force field for fracture simulations of lithium oxide systems, which was obtained by training against an extensive set of DFT, multireference configuration interaction (MRCI), and MRCI+Q reference data using genetic optimization techniques. This new force field significantly improves the bond breaking behavior, but still cannot fully capture the brittle fracture in MD simulations, suggesting more research is needed to improve simulation of brittle fracture.

Original languageEnglish (US)
Article number084107
JournalJournal of Chemical Physics
Issue number8
StatePublished - Aug 28 2020

All Science Journal Classification (ASJC) codes

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry


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