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Title: Benchmarking boron carbide equation of state using computation and experiment

Abstract

Boron carbide ( B 4 C ) is of both fundamental scientific and practical interest due to its structural complexity and how it changes upon compression, as well as its many industrial uses and potential for use in inertial confinement fusion (ICF) and high-energy density physics experiments. Here, we report the results of a comprehensive computational study of the equation of state (EOS) of B 4 C in the liquid, warm dense matter, and plasma phases. Our calculations are cross-validated by comparisons with Hugoniot measurements up to 61 megabar from planar shock experiments performed at the National Ignition Facility (NIF). Our computational methods include path integral Monte Carlo, activity expansion, as well as all-electron Green's function Korringa-Kohn-Rostoker and molecular dynamics that are both based on density functional theory. We calculate the pressure-internal energy EOS of B 4 C over a broad range of temperatures ( ~ 6 × 10 3 – 5 × 10 8 K) and densities (0.025–50 g / cm 3 ). We assess that the largest discrepancies between theoretical predictions are ≲ 5 % near the compression maximum at 1– 2 × 106 K. This is the warm-dense state in which the K shell significantly ionizes and has posed grand challenges to theory and experiment. By comparing with different EOS models, we find a Purgatorio model (LEOS 2122) that agrees with our calculations. The maximum discrepancies in pressure between our first-principles predictions and LEOS 2122 are ~ 18 % and occur at temperatures between 6 × 10 3 – 2 × 10 5 K, which we believe originate from differences in the ion thermal term and the cold curve that are modeled in LEOS 2122 in comparison with our first-principles calculations. To account for potential differences in the ion thermal term, we have developed three new equation-of-state models that are consistent with theoretical calculations and experiment. We apply these new models to 1D hydrodynamic simulations of a polar direct-drive NIF implosion, demonstrating that these new models are now available for future ICF design studies.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2];  [2];  [3]; ORCiD logo [2];  [2];  [2];  [2];  [2];  [2]; ORCiD logo [2];  [2];  [2];  [2];  [2]
+ Show Author Affiliations
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of Rochester, NY (United States). Lab. for Laser Energetics
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1775037
Report Number(s):
LLNL-JRNL-812984
Journal ID: ISSN 2470-0045; 1020196; TRN: US2209296
Grant/Contract Number:  
AC52-07NA27344; SC0016248
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. E
Additional Journal Information:
Journal Volume: 102; Journal Issue: 5; Journal ID: ISSN 2470-0045
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; equations of state; high-energy-density plasmas; plasma ionization; shock waves; hot dense plasma; warm-dense matter; density functional calculations; path-integral Monte Carlo

Citation Formats

Zhang, Shuai, Marshall, Michelle C., Yang, Lin H., Sterne, Philip A., Militzer, Burkhard, Däne, Markus, Gaffney, James A., Shamp, Andrew, Ogitsu, Tadashi, Caspersen, Kyle, Lazicki, Amy E., Erskine, David, London, Richard A., Celliers, Peter M., Nilsen, Joseph, and Whitley, Heather D. Benchmarking boron carbide equation of state using computation and experiment. United States: N. p., 2020. Web. doi:10.1103/physreve.102.053203.
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Zhang, Shuai, Marshall, Michelle C., Yang, Lin H., Sterne, Philip A., Militzer, Burkhard, Däne, Markus, Gaffney, James A., Shamp, Andrew, Ogitsu, Tadashi, Caspersen, Kyle, Lazicki, Amy E., Erskine, David, London, Richard A., Celliers, Peter M., Nilsen, Joseph, & Whitley, Heather D. Benchmarking boron carbide equation of state using computation and experiment. United States. https://doi.org/10.1103/physreve.102.053203
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Zhang, Shuai, Marshall, Michelle C., Yang, Lin H., Sterne, Philip A., Militzer, Burkhard, Däne, Markus, Gaffney, James A., Shamp, Andrew, Ogitsu, Tadashi, Caspersen, Kyle, Lazicki, Amy E., Erskine, David, London, Richard A., Celliers, Peter M., Nilsen, Joseph, and Whitley, Heather D. Tue . "Benchmarking boron carbide equation of state using computation and experiment". United States. https://doi.org/10.1103/physreve.102.053203. https://www.osti.gov/servlets/purl/1775037.
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@article{osti_1775037,
title = {Benchmarking boron carbide equation of state using computation and experiment},
author = {Zhang, Shuai and Marshall, Michelle C. and Yang, Lin H. and Sterne, Philip A. and Militzer, Burkhard and Däne, Markus and Gaffney, James A. and Shamp, Andrew and Ogitsu, Tadashi and Caspersen, Kyle and Lazicki, Amy E. and Erskine, David and London, Richard A. and Celliers, Peter M. and Nilsen, Joseph and Whitley, Heather D.},
abstractNote = {Boron carbide (B4C) is of both fundamental scientific and practical interest due to its structural complexity and how it changes upon compression, as well as its many industrial uses and potential for use in inertial confinement fusion (ICF) and high-energy density physics experiments. Here, we report the results of a comprehensive computational study of the equation of state (EOS) of B4C in the liquid, warm dense matter, and plasma phases. Our calculations are cross-validated by comparisons with Hugoniot measurements up to 61 megabar from planar shock experiments performed at the National Ignition Facility (NIF). Our computational methods include path integral Monte Carlo, activity expansion, as well as all-electron Green's function Korringa-Kohn-Rostoker and molecular dynamics that are both based on density functional theory. We calculate the pressure-internal energy EOS of B4C over a broad range of temperatures (~6×103–5×108 K) and densities (0.025–50 g/cm3). We assess that the largest discrepancies between theoretical predictions are ≲5% near the compression maximum at 1–2×106 K. This is the warm-dense state in which the K shell significantly ionizes and has posed grand challenges to theory and experiment. By comparing with different EOS models, we find a Purgatorio model (LEOS 2122) that agrees with our calculations. The maximum discrepancies in pressure between our first-principles predictions and LEOS 2122 are ~18% and occur at temperatures between 6×103–2×105 K, which we believe originate from differences in the ion thermal term and the cold curve that are modeled in LEOS 2122 in comparison with our first-principles calculations. To account for potential differences in the ion thermal term, we have developed three new equation-of-state models that are consistent with theoretical calculations and experiment. We apply these new models to 1D hydrodynamic simulations of a polar direct-drive NIF implosion, demonstrating that these new models are now available for future ICF design studies.},
doi = {10.1103/physreve.102.053203},
journal = {Physical Review. E},
number = 5,
volume = 102,
place = {United States},
year = {Tue Nov 03 00:00:00 EST 2020},
month = {Tue Nov 03 00:00:00 EST 2020}
}
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