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Title: Determination of a Density Functional Tight Binding Model with an Extended Basis Set and Three-Body Repulsion for Carbon Under Extreme Pressures and Temperatures

Abstract

In this paper, we report here on development of a density functional tight binding (DFTB) simulation approach for carbon under extreme pressures and temperatures that includes an expanded basis set and an environmentally dependent repulsive energy. We find that including d-orbital interactions in the DFTB Hamiltonian improves determination of the electronic states at high pressure–temperature conditions, compared to standard DFTB implementations that utilize s- and p-orbitals only for carbon. We then determine a three-body repulsive energy through fitting to diamond, BC8, and simple cubic cold compression curve data, as well pressures from metallic liquid configurations from density functional theory (DFT) simulations. Our new model (DFTB-p3b) yields approximately 2 orders of magnitude increase in computational efficiency over standard DFT while retaining its accuracy for condensed phases of carbon under a wide range of conditions, including the metallic liquid phase at conditions up to 2000 GPa and 30 000 K. Finally, our results provide a straightforward method by which DFTB can be extended to studies of covalently bonded materials under extremely high pressures and temperatures such as the interiors of planets and other large celestial bodies.

Authors:
 [1];  [2];  [1];  [1];  [3];  [4]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate
  2. Pennsylvania State University, State College PA (United States). Department of Mechanical and Nuclear Engineering
  3. Univ. of Wisconsin, Madison, WI (United States). Department of Chemistry and Theoretical Chemistry Institute
  4. Karlsruhe Inst. of Technology (KIT) (Germany). Institute of Physical Chemistry
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1466147
Report Number(s):
LLNL-JRNL-608994
Journal ID: ISSN 1932-7447; 709498
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 117; Journal Issue: 15; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Goldman, Nir, Goverapet Srinivasan, Sriram, Hamel, Sebastien, Fried, Laurence E., Gaus, Michael, and Elstner, Marcus. Determination of a Density Functional Tight Binding Model with an Extended Basis Set and Three-Body Repulsion for Carbon Under Extreme Pressures and Temperatures. United States: N. p., 2013. Web. doi:10.1021/jp312759j.
Goldman, Nir, Goverapet Srinivasan, Sriram, Hamel, Sebastien, Fried, Laurence E., Gaus, Michael, & Elstner, Marcus. Determination of a Density Functional Tight Binding Model with an Extended Basis Set and Three-Body Repulsion for Carbon Under Extreme Pressures and Temperatures. United States. doi:10.1021/jp312759j.
Goldman, Nir, Goverapet Srinivasan, Sriram, Hamel, Sebastien, Fried, Laurence E., Gaus, Michael, and Elstner, Marcus. Wed . "Determination of a Density Functional Tight Binding Model with an Extended Basis Set and Three-Body Repulsion for Carbon Under Extreme Pressures and Temperatures". United States. doi:10.1021/jp312759j. https://www.osti.gov/servlets/purl/1466147.
@article{osti_1466147,
title = {Determination of a Density Functional Tight Binding Model with an Extended Basis Set and Three-Body Repulsion for Carbon Under Extreme Pressures and Temperatures},
author = {Goldman, Nir and Goverapet Srinivasan, Sriram and Hamel, Sebastien and Fried, Laurence E. and Gaus, Michael and Elstner, Marcus},
abstractNote = {In this paper, we report here on development of a density functional tight binding (DFTB) simulation approach for carbon under extreme pressures and temperatures that includes an expanded basis set and an environmentally dependent repulsive energy. We find that including d-orbital interactions in the DFTB Hamiltonian improves determination of the electronic states at high pressure–temperature conditions, compared to standard DFTB implementations that utilize s- and p-orbitals only for carbon. We then determine a three-body repulsive energy through fitting to diamond, BC8, and simple cubic cold compression curve data, as well pressures from metallic liquid configurations from density functional theory (DFT) simulations. Our new model (DFTB-p3b) yields approximately 2 orders of magnitude increase in computational efficiency over standard DFT while retaining its accuracy for condensed phases of carbon under a wide range of conditions, including the metallic liquid phase at conditions up to 2000 GPa and 30 000 K. Finally, our results provide a straightforward method by which DFTB can be extended to studies of covalently bonded materials under extremely high pressures and temperatures such as the interiors of planets and other large celestial bodies.},
doi = {10.1021/jp312759j},
journal = {Journal of Physical Chemistry. C},
number = 15,
volume = 117,
place = {United States},
year = {2013},
month = {3}
}

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Cited by: 16 works
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