Transferable density functional tight binding for carbon, hydrogen, nitrogen, and oxygen: Application to shock compression
Abstract
A new parameterization for density functional tight binding (DFTB) theory, lanl31, has been developed for molecules containing carbon, hydrogen, nitrogen, and oxygen. Optimal values for the Hubbard Us, onsite energies, and the radial dependences of the bond integrals and repulsive potentials were determined by numerical optimization using simulated annealing to a modest database of ab initiocalculated atomization energies and interatomic forces. The transferability of the optimized DFTB parameterization has been assessed using the CHNO subset of the QM9 database [R. Ramakrishnan et al., Sci. Data, 1, 140022 (2014)]. These analyses showed that the errors in the atomization energies and interatomic forces predicted by our model are small and in the vicinity of the di erences between density functional theory calculations with di erent basis sets and exchangecorrelation functionals. Good correlations between the molecular dipole moments and HOMOLUMO gaps predicted by lanl31 and the QM9 data set are also found. Furthermore, the errors in the atomization energies and forces derived from lanl31 are signi cantly smaller than those obtained from the ReaxFFlg reactive force eld for organic materials [L. Liu et al., J. Phys. Chem. A, 115, 11016 (2011)]. The lanl31 DFTB parameterization for C, H, N, and O has beenmore »
 Authors:

 Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
 Publication Date:
 Research Org.:
 Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
 Sponsoring Org.:
 USDOE
 OSTI Identifier:
 1492539
 Report Number(s):
 LAUR1829043
Journal ID: ISSN 00219606
 Grant/Contract Number:
 89233218CNA000001
 Resource Type:
 Accepted Manuscript
 Journal Name:
 Journal of Chemical Physics
 Additional Journal Information:
 Journal Volume: 150; Journal Issue: 2; Journal ID: ISSN 00219606
 Publisher:
 American Institute of Physics (AIP)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Cawkwell, M. J., and Perriot, R.. Transferable density functional tight binding for carbon, hydrogen, nitrogen, and oxygen: Application to shock compression. United States: N. p., 2019.
Web. doi:10.1063/1.5063385.
Cawkwell, M. J., & Perriot, R.. Transferable density functional tight binding for carbon, hydrogen, nitrogen, and oxygen: Application to shock compression. United States. https://doi.org/10.1063/1.5063385
Cawkwell, M. J., and Perriot, R.. Thu .
"Transferable density functional tight binding for carbon, hydrogen, nitrogen, and oxygen: Application to shock compression". United States. https://doi.org/10.1063/1.5063385. https://www.osti.gov/servlets/purl/1492539.
@article{osti_1492539,
title = {Transferable density functional tight binding for carbon, hydrogen, nitrogen, and oxygen: Application to shock compression},
author = {Cawkwell, M. J. and Perriot, R.},
abstractNote = {A new parameterization for density functional tight binding (DFTB) theory, lanl31, has been developed for molecules containing carbon, hydrogen, nitrogen, and oxygen. Optimal values for the Hubbard Us, onsite energies, and the radial dependences of the bond integrals and repulsive potentials were determined by numerical optimization using simulated annealing to a modest database of ab initiocalculated atomization energies and interatomic forces. The transferability of the optimized DFTB parameterization has been assessed using the CHNO subset of the QM9 database [R. Ramakrishnan et al., Sci. Data, 1, 140022 (2014)]. These analyses showed that the errors in the atomization energies and interatomic forces predicted by our model are small and in the vicinity of the di erences between density functional theory calculations with di erent basis sets and exchangecorrelation functionals. Good correlations between the molecular dipole moments and HOMOLUMO gaps predicted by lanl31 and the QM9 data set are also found. Furthermore, the errors in the atomization energies and forces derived from lanl31 are signi cantly smaller than those obtained from the ReaxFFlg reactive force eld for organic materials [L. Liu et al., J. Phys. Chem. A, 115, 11016 (2011)]. The lanl31 DFTB parameterization for C, H, N, and O has been applied the to the molecular dynamics simulation of the principal Hugoniot of liquid nitromethane, liquid benzene, liquid nitrogen, pentaerythritol tetranitrate, trinitrotoluene, and cyclotetramethylene tetranitramine. The computed and measured Hugoniot loci are in excellent agreement with experiment and we discuss the sensitivity of the loci to the underestimated shock heating that is a characteristic of classical molecular dynamics simulations.},
doi = {10.1063/1.5063385},
journal = {Journal of Chemical Physics},
number = 2,
volume = 150,
place = {United States},
year = {2019},
month = {1}
}
Web of Science
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