EReaxFF: A Pseudoclassical Treatment of Explicit Electrons within Reactive Force Field Simulations

Md Mahbubul Islam, Grigory Kolesov, Toon Verstraelen, Efthimios Kaxiras, Adri C.T. Van Duin

Research output: Contribution to journalArticle

27 Scopus citations

Abstract

We present a computational tool, eReaxFF, for simulating explicit electrons within the framework of the standard ReaxFF reactive force field method. We treat electrons explicitly in a pseudoclassical manner that enables simulation several orders of magnitude faster than quantum chemistry (QC) methods, while retaining the ReaxFF transferability. We delineate here the fundamental concepts of the eReaxFF method and the integration of the Atom-condensed Kohn-Sham DFT approximated to second order (ACKS2) charge calculation scheme into the eReaxFF. We trained our force field to capture electron affinities (EA) of various species. As a proof-of-principle, we performed a set of molecular dynamics (MD) simulations with an explicit electron model for representative hydrocarbon radicals. We establish a good qualitative agreement of EAs of various species with experimental data, and MD simulations with eReaxFF agree well with the corresponding Ehrenfest dynamics simulations. The standard ReaxFF parameters available in the literature are transferrable to the eReaxFF method. The computationally economic eReaxFF method will be a useful tool for studying large-scale chemical and physical systems with explicit electrons as an alternative to computationally demanding QC methods.

Original languageEnglish (US)
Pages (from-to)3463-3472
Number of pages10
JournalJournal of Chemical Theory and Computation
Volume12
Issue number8
DOIs
StatePublished - Aug 9 2016

All Science Journal Classification (ASJC) codes

  • Computer Science Applications
  • Physical and Theoretical Chemistry

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