Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: 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, on-site 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 initio-calculated atomization energies and interatomic forces. The transferability of the optimized DFTB parameterization has been assessed using the CHNO subset of the QM-9 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 exchange-correlation functionals. Good correlations between the molecular dipole moments and HOMO-LUMO gaps predicted by lanl31 and the QM-9 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 ReaxFF-lg 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 » 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.« less

Authors:
ORCiD logo [1];  [1]
+ Show Author Affiliations
  1. 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):
LA-UR-18-29043
Journal ID: ISSN 0021-9606
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 0021-9606
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.
Copy to clipboard
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
Copy to clipboard
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.
Copy to clipboard
@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, on-site 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 initio-calculated atomization energies and interatomic forces. The transferability of the optimized DFTB parameterization has been assessed using the CHNO subset of the QM-9 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 exchange-correlation functionals. Good correlations between the molecular dipole moments and HOMO-LUMO gaps predicted by lanl31 and the QM-9 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 ReaxFF-lg 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}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.5063385
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Energy conserving, linear scaling Born-Oppenheimer molecular dynamics
journal, October 2012

  • Cawkwell, M. J.; Niklasson, Anders M. N.
  • The Journal of Chemical Physics, Vol. 137, Issue 13
  • DOI: 10.1063/1.4755991

Time-reversible ab initio molecular dynamics
journal, April 2007

  • Niklasson, Anders M. N.; Tymczak, C. J.; Challacombe, Matt
  • The Journal of Chemical Physics, Vol. 126, Issue 14
  • DOI: 10.1063/1.2715556

C 6 Coefficients and Dipole Polarizabilities for All Atoms and Many Ions in Rows 1–6 of the Periodic Table
journal, July 2016

  • Gould, Tim; Bučko, Tomáš
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 8
  • DOI: 10.1021/acs.jctc.6b00361

Graph-based linear scaling electronic structure theory
journal, June 2016

  • Niklasson, Anders M. N.; Mniszewski, Susan M.; Negre, Christian F. A.
  • The Journal of Chemical Physics, Vol. 144, Issue 23
  • DOI: 10.1063/1.4952650

Extending the Density Functional Tight Binding Method to Carbon Under Extreme Conditions
journal, November 2011

  • Goldman, Nir; Fried, Laurence E.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 3
  • DOI: 10.1021/jp206768x

Efficient Parallel Linear Scaling Construction of the Density Matrix for Born–Oppenheimer Molecular Dynamics
journal, September 2015

  • Mniszewski, S. M.; Cawkwell, M. J.; Wall, M. E.
  • Journal of Chemical Theory and Computation, Vol. 11, Issue 10
  • DOI: 10.1021/acs.jctc.5b00552

Automatized Parameterization of DFTB Using Particle Swarm Optimization
journal, December 2015

  • Chou, Chien-Pin; Nishimura, Yoshifumi; Fan, Chin-Chai
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 1
  • DOI: 10.1021/acs.jctc.5b00673

In situ parameterisation of SCC-DFTB repulsive potentials by iterative Boltzmann inversion
journal, December 2013

A Density Functional Tight Binding Model with an Extended Basis Set and Three-Body Repulsion for Hydrogen under Extreme Thermodynamic Conditions
journal, July 2014

  • Srinivasan, Sriram Goverapet; Goldman, Nir; Tamblyn, Isaac
  • The Journal of Physical Chemistry A, Vol. 118, Issue 29
  • DOI: 10.1021/jp5036713

Generalized Density-Functional Tight-Binding Repulsive Potentials from Unsupervised Machine Learning
journal, March 2018

  • Kranz, Julian J.; Kubillus, Maximilian; Ramakrishnan, Raghunathan
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 5
  • DOI: 10.1021/acs.jctc.7b00933

Plato: A localised orbital based density functional theory code
journal, December 2009

Simulations of Shocked Methane Including Self-Consistent Semiclassical Quantum Nuclear Effects
journal, October 2012

  • Qi, Tingting; Reed, Evan J.
  • The Journal of Physical Chemistry A, Vol. 116, Issue 42
  • DOI: 10.1021/jp308068c

Polymorphism in 2-4-6 Trinitrotoluene
journal, November 2003

  • Vrcelj, Ranko M.; Sherwood, John N.; Kennedy, Alan R.
  • Crystal Growth & Design, Vol. 3, Issue 6
  • DOI: 10.1021/cg0340704

Free Energy Based Equation of State for Pentaerythritol Tetranitrate
journal, December 2016

  • Cawkwell, M. J.; Montgomery, D. S.; Ramos, K. J.
  • The Journal of Physical Chemistry A, Vol. 121, Issue 1
  • DOI: 10.1021/acs.jpca.6b09284

Density-functional tight binding-an approximate density-functional theory method: DFTB-an approximate DFT method
journal, January 2012

  • Seifert, Gotthard; Joswig, Jan-Ole
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 3
  • DOI: 10.1002/wcms.1094

\mathcal{O}(N) methods in electronic structure calculations
journal, February 2012

Density functional tight binding
journal, March 2014

  • Elstner, Marcus; Seifert, Gotthard
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 372, Issue 2011
  • DOI: 10.1098/rsta.2012.0483

Where does tight binding go from here?
journal, December 2011

NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations
journal, September 2010

  • Valiev, M.; Bylaska, E. J.; Govind, N.
  • Computer Physics Communications, Vol. 181, Issue 9, p. 1477-1489
  • DOI: 10.1016/j.cpc.2010.04.018

Using Force-Matched Potentials To Improve the Accuracy of Density Functional Tight Binding for Reactive Conditions
journal, September 2015

  • Goldman, Nir; Fried, Laurence E.; Koziol, Lucas
  • Journal of Chemical Theory and Computation, Vol. 11, Issue 10
  • DOI: 10.1021/acs.jctc.5b00742

Numerical Optimization of Density Functional Tight Binding Models: Application to Molecules Containing Carbon, Hydrogen, Nitrogen, and Oxygen
journal, November 2017

  • Krishnapriyan, A.; Yang, P.; Niklasson, A. M. N.
  • Journal of Chemical Theory and Computation, Vol. 13, Issue 12
  • DOI: 10.1021/acs.jctc.7b00762

Self-consistent tight-binding formalism for charged systems
journal, September 1998

Nested Markov chain Monte Carlo sampling of a density functional theory potential: Equilibrium thermodynamics of dense fluid nitrogen
journal, August 2009

  • Coe, Joshua D.; Sewell, Thomas D.; Shaw, M. Sam
  • The Journal of Chemical Physics, Vol. 131, Issue 7
  • DOI: 10.1063/1.3200904

Thermal Expansion of HMX
journal, February 2011

  • Deschamps, Jeffrey R.; Frisch, Mark; Parrish, Damon
  • Journal of Chemical Crystallography, Vol. 41, Issue 7
  • DOI: 10.1007/s10870-011-0026-6

Extended Lagrangian Born–Oppenheimer molecular dynamics with dissipation
journal, June 2009

  • Niklasson, Anders M. N.; Steneteg, Peter; Odell, Anders
  • The Journal of Chemical Physics, Vol. 130, Issue 21
  • DOI: 10.1063/1.3148075

Extended Lagrangian Born-Oppenheimer molecular dynamics simulations of the shock-induced chemistry of phenylacetylene
journal, February 2015

  • Cawkwell, M. J.; Niklasson, Anders M. N.; Dattelbaum, Dana M.
  • The Journal of Chemical Physics, Vol. 142, Issue 6
  • DOI: 10.1063/1.4907909

A comparison of linear scaling tight-binding methods
journal, May 1997

  • Bowler, D. R.; Aoki, M.; Goringe, C. M.
  • Modelling and Simulation in Materials Science and Engineering, Vol. 5, Issue 3
  • DOI: 10.1088/0965-0393/5/3/002

Linear scaling electronic structure methods
journal, July 1999

Temperature measurements and an improved equation of state for shocked liquid benzene
journal, May 2013

  • Lacina, D.; Gupta, Y. M.
  • The Journal of Chemical Physics, Vol. 138, Issue 17
  • DOI: 10.1063/1.4803138

DFTB Parameters for the Periodic Table: Part 1, Electronic Structure
journal, August 2013

  • Wahiduzzaman, Mohammad; Oliveira, Augusto F.; Philipsen, Pier
  • Journal of Chemical Theory and Computation, Vol. 9, Issue 9
  • DOI: 10.1021/ct4004959

Comparison of DFT Methods for Molecular Orbital Eigenvalue Calculations
journal, March 2007

  • Zhang, Gang; Musgrave, Charles B.
  • The Journal of Physical Chemistry A, Vol. 111, Issue 8
  • DOI: 10.1021/jp061633o

Shock Wave Compression of Benzene, Carbon Disulfide, Carbon Tetrachloride, and Liquid Nitrogen
journal, June 1970

  • Dick, Richard D.
  • The Journal of Chemical Physics, Vol. 52, Issue 12
  • DOI: 10.1063/1.1672902

Equation of state and temperature measurements for shocked nitromethane
journal, November 2000

  • Winey, J. M.; Duvall, G. E.; Knudson, M. D.
  • The Journal of Chemical Physics, Vol. 113, Issue 17, p. 7492-7501
  • DOI: 10.1063/1.1312271

ReaxFF- l g: Correction of the ReaxFF Reactive Force Field for London Dispersion, with Applications to the Equations of State for Energetic Materials
journal, October 2011

  • Liu, Lianchi; Liu, Yi; Zybin, Sergey V.
  • The Journal of Physical Chemistry A, Vol. 115, Issue 40
  • DOI: 10.1021/jp201599t

Extensions of the S66 Data Set: More Accurate Interaction Energies and Angular-Displaced Nonequilibrium Geometries
journal, October 2011

  • Řezáč, Jan; Riley, Kevin E.; Hobza, Pavel
  • Journal of Chemical Theory and Computation, Vol. 7, Issue 11
  • DOI: 10.1021/ct200523a

Lagrangian formulation with dissipation of Born-Oppenheimer molecular dynamics using the density-functional tight-binding method
journal, July 2011

  • Zheng, Guishan; Niklasson, Anders M. N.; Karplus, Martin
  • The Journal of Chemical Physics, Vol. 135, Issue 4
  • DOI: 10.1063/1.3605303

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495

Crystal Structures of Zirconia from First Principles and Self-Consistent Tight Binding
journal, December 1998

Optimization by Simulated Annealing
journal, May 1983

Quantum chemistry structures and properties of 134 kilo molecules
journal, August 2014

  • Ramakrishnan, Raghunathan; Dral, Pavlo O.; Rupp, Matthias
  • Scientific Data, Vol. 1, Issue 1
  • DOI: 10.1038/sdata.2014.22

Density functional tight binding: application to organic and biological molecules: Density functional tight binding
journal, June 2013

  • Gaus, Michael; Cui, Qiang; Elstner, Marcus
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 4, Issue 1
  • DOI: 10.1002/wcms.1156

Transferable atomic-type orbital basis sets for solids
journal, August 2000

Automatized Parametrization of SCC-DFTB Repulsive Potentials: Application to Hydrocarbons †
journal, October 2009

  • Gaus, Michael; Chou, Chien-Pin; Witek, Henryk
  • The Journal of Physical Chemistry A, Vol. 113, Issue 43
  • DOI: 10.1021/jp902973m

Simulations of Shocked Methane Including Self-consistent Semiclassical Quantum Nuclear Effects
journal, January 2013

Generalized Density-Functional Tight-Binding Repulsive Potentials from Unsupervised Machine Learning
text, January 2018

  • Kranz, Julian J.; Kubillus, Maximilian; Ramakrishnan, Raghunathan
  • American Chemical Society
  • DOI: 10.5451/unibas-ep68688

Extended Lagrangian Born–Oppenheimer molecular dynamics with dissipation
text, January 2009

  • Niklasson, A. M. N.; Steneteg, P.; Odell, A.
  • American Institute of Physics
  • DOI: 10.5167/uzh-19937

Graph-based linear scaling electronic structure theory
text, January 2016

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Parallel replica dynamics simulations of reactions in shock compressed liquid benzene
    journal, June 2019

    • Martínez, E.; Perriot, R.; Kober, E. M.
    • The Journal of Chemical Physics, Vol. 150, Issue 24
    • DOI: 10.1063/1.5092209

    Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy
    journal, May 2019

    • Bowlan, Pamela; Powell, Michael; Perriot, Romain
    • The Journal of Chemical Physics, Vol. 150, Issue 20
    • DOI: 10.1063/1.5092242
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: