Advanced search
1 file | 4.14 MB

eReaxFF : a pseudoclassical treatment of explicit electrons within reactive force field simulations

Author
Organization
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.
Keywords
MOLECULAR-DYNAMICS SIMULATIONS, DENSITY-FUNCTIONAL THEORY, ELECTRONEGATIVITY EQUALIZATION, ATOMIC CHARGES, REAXFF, HYDROCARBONS, INTERFACE, CHEMISTRY, SYSTEMS, STATES

Downloads

  • (...).pdf
    • full text
    • |
    • UGent only
    • |
    • PDF
    • |
    • 4.14 MB

Citation

Please use this url to cite or link to this publication:

Chicago
Islam, Md Mahbubul, Grigory Kolesov, Toon Verstraelen, Efthimios Kaxiras, and Adri CT van Duin. 2016. “eReaxFF : a Pseudoclassical Treatment of Explicit Electrons Within Reactive Force Field Simulations.” Journal of Chemical Theory and Computation 12 (8): 3463–3472.
APA
Islam, Md Mahbubul, Kolesov, G., Verstraelen, T., Kaxiras, E., & van Duin, A. C. (2016). eReaxFF : a pseudoclassical treatment of explicit electrons within reactive force field simulations. JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 12(8), 3463–3472.
Vancouver
1.
Islam MM, Kolesov G, Verstraelen T, Kaxiras E, van Duin AC. eReaxFF : a pseudoclassical treatment of explicit electrons within reactive force field simulations. JOURNAL OF CHEMICAL THEORY AND COMPUTATION. 2016;12(8):3463–72.
MLA
Islam, Md Mahbubul, Grigory Kolesov, Toon Verstraelen, et al. “eReaxFF : a Pseudoclassical Treatment of Explicit Electrons Within Reactive Force Field Simulations.” JOURNAL OF CHEMICAL THEORY AND COMPUTATION 12.8 (2016): 3463–3472. Print.
@article{8158010,
  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.},
  author       = {Islam, Md Mahbubul and Kolesov, Grigory and Verstraelen, Toon and Kaxiras, Efthimios and van Duin, Adri CT},
  issn         = {1549-9618},
  journal      = {JOURNAL OF CHEMICAL THEORY AND COMPUTATION},
  keyword      = {MOLECULAR-DYNAMICS SIMULATIONS,DENSITY-FUNCTIONAL THEORY,ELECTRONEGATIVITY EQUALIZATION,ATOMIC CHARGES,REAXFF,HYDROCARBONS,INTERFACE,CHEMISTRY,SYSTEMS,STATES},
  language     = {eng},
  number       = {8},
  pages        = {3463--3472},
  title        = {eReaxFF : a pseudoclassical treatment of explicit electrons within reactive force field simulations},
  url          = {http://dx.doi.org/10.1021/acs.jctc.6b00432},
  volume       = {12},
  year         = {2016},
}

Altmetric
View in Altmetric
Web of Science
Times cited: