skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Path integral Monte Carlo simulations of dense carbon-hydrogen plasmas

Abstract

Carbon-hydrogen plasmas and hydrocarbon materials are of broad interest to laser shock experimentalists, high energy density physicists, and astrophysicists. Accurate equations of state (EOSs) of hydrocarbons are valuable for various studies from inertial confinement fusion to planetary science. By combining path integral Monte Carlo (PIMC) results at high temperatures and density functional theory molecular dynamics results at lower temperatures, we compute the EOSs for hydrocarbons from simulations performed at 1473 separate (ρ, T)-points distributed over a range of compositions. These methods accurately treat electronic excitation effects with neither adjustable parameter nor experimental input. PIMC is also an accurate simulation method that is capable of treating many-body interaction and nuclear quantum effects at finite temperatures. These methods therefore provide a benchmark-quality EOS that surpasses that of semi-empirical and Thomas-Fermi-based methods in the warm dense matter regime. By comparing our first-principles EOS to the LEOS 5112 model for CH, we validate the specific heat assumptions in this model but suggest that the Grüneisen parameter is too large at low temperatures. Based on our first-principles EOSs, we predict the principal Hugoniot curve of polystyrene to be 2%-5% softer at maximum shock compression than that predicted by orbital-free density functional theory and SESAME 7593.more » By investigating the atomic structure and chemical bonding of hydrocarbons, we show a drastic decrease in the lifetime of chemical bonds in the pressure interval from 0.4 to 4 megabar. We find the assumption of linear mixing to be valid for describing the EOS and the shock Hugoniot curve of hydrocarbons in the regime of partially ionized atomic liquids. We make predictions of the shock compression of glow-discharge polymers and investigate the effects of oxygen content and C:H ratio on its Hugoniot curve. In conclusion, our full suite of first-principles simulation results may be used to benchmark future theoretical investigations pertaining to hydrocarbon EOSs and should be helpful in guiding the design of future experiments on hydrocarbons in the gigabar regime.« less

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [2];  [3];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, 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:
1474357
Alternate Identifier(s):
OSTI ID: 1420621
Report Number(s):
LLNL-JRNL-736960
Journal ID: ISSN 0021-9606; 889714
Grant/Contract Number:  
AC52-07NA27344; NA0001859; SC0010517; SC0016248
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 10; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Citation Formats

Zhang, Shuai, Militzer, Burkhard, Benedict, Lorin X., Soubiran, François, Sterne, Philip A., and Driver, Kevin P. Path integral Monte Carlo simulations of dense carbon-hydrogen plasmas. United States: N. p., 2017. Web. doi:10.1063/1.5001208.
Zhang, Shuai, Militzer, Burkhard, Benedict, Lorin X., Soubiran, François, Sterne, Philip A., & Driver, Kevin P. Path integral Monte Carlo simulations of dense carbon-hydrogen plasmas. United States. https://doi.org/10.1063/1.5001208
Zhang, Shuai, Militzer, Burkhard, Benedict, Lorin X., Soubiran, François, Sterne, Philip A., and Driver, Kevin P. 2017. "Path integral Monte Carlo simulations of dense carbon-hydrogen plasmas". United States. https://doi.org/10.1063/1.5001208. https://www.osti.gov/servlets/purl/1474357.
@article{osti_1474357,
title = {Path integral Monte Carlo simulations of dense carbon-hydrogen plasmas},
author = {Zhang, Shuai and Militzer, Burkhard and Benedict, Lorin X. and Soubiran, François and Sterne, Philip A. and Driver, Kevin P.},
abstractNote = {Carbon-hydrogen plasmas and hydrocarbon materials are of broad interest to laser shock experimentalists, high energy density physicists, and astrophysicists. Accurate equations of state (EOSs) of hydrocarbons are valuable for various studies from inertial confinement fusion to planetary science. By combining path integral Monte Carlo (PIMC) results at high temperatures and density functional theory molecular dynamics results at lower temperatures, we compute the EOSs for hydrocarbons from simulations performed at 1473 separate (ρ, T)-points distributed over a range of compositions. These methods accurately treat electronic excitation effects with neither adjustable parameter nor experimental input. PIMC is also an accurate simulation method that is capable of treating many-body interaction and nuclear quantum effects at finite temperatures. These methods therefore provide a benchmark-quality EOS that surpasses that of semi-empirical and Thomas-Fermi-based methods in the warm dense matter regime. By comparing our first-principles EOS to the LEOS 5112 model for CH, we validate the specific heat assumptions in this model but suggest that the Grüneisen parameter is too large at low temperatures. Based on our first-principles EOSs, we predict the principal Hugoniot curve of polystyrene to be 2%-5% softer at maximum shock compression than that predicted by orbital-free density functional theory and SESAME 7593. By investigating the atomic structure and chemical bonding of hydrocarbons, we show a drastic decrease in the lifetime of chemical bonds in the pressure interval from 0.4 to 4 megabar. We find the assumption of linear mixing to be valid for describing the EOS and the shock Hugoniot curve of hydrocarbons in the regime of partially ionized atomic liquids. We make predictions of the shock compression of glow-discharge polymers and investigate the effects of oxygen content and C:H ratio on its Hugoniot curve. In conclusion, our full suite of first-principles simulation results may be used to benchmark future theoretical investigations pertaining to hydrocarbon EOSs and should be helpful in guiding the design of future experiments on hydrocarbons in the gigabar regime.},
doi = {10.1063/1.5001208},
url = {https://www.osti.gov/biblio/1474357}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 10,
volume = 148,
place = {United States},
year = {Mon Nov 20 00:00:00 EST 2017},
month = {Mon Nov 20 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Properties of hydrogen, helium, and silicon dioxide mixtures in giant planet interiors
text, January 2017


Characterization of the State of Hydrogen at High Temperature and Density
journal, January 1999


UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992


Dynamic Behavior of Materials
book, September 1994


First Principles Calculations of Shock Compressed Fluid Helium
journal, October 2006


High-temperature miscibility of iron and rock during terrestrial planet formation
journal, January 2015


Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges
journal, April 2016


Calculation of a Deuterium Double Shock Hugoniot from Ab Initio Simulations
journal, December 2001


Plastic ablator and hydrodynamic instabilities: A first-principles set of microscopic coefficients
journal, August 2012


Synthesis of the elements in stars: forty years of progress
text, January 1997


Hydrogen-Helium Mixtures in the Interiors of Giant Planets
text, January 2006


Absolute measurements of the equations of state of low-Z materials in the multi-Mbar regime using laser-driven shocks
journal, May 1997


Evidence for a first-order liquid-liquid transition in high-pressure hydrogen from ab initio simulations
journal, June 2010


Path integral Monte Carlo simulations of warm dense sodium
journal, December 2016


Brominated plastic equation of state measurements using laser driven shocks
journal, March 1998


A new quotidian equation of state (QEOS) for hot dense matter
journal, January 1988


A new global equation of state model for hot, dense matter
journal, September 1995


First-principles equation of state and shock compression predictions of warm dense hydrocarbons
journal, July 2017


Hydrogen–Helium Mixtures at High Pressure
journal, June 2005


Quantum nature of the hydrogen bond
journal, April 2011


X-ray Thomson scattering as a temperature probe for Gbar shock experiments
journal, May 2014


Inertial-confinement fusion with lasers
journal, May 2016


Shock Hugoniot and temperature data for polystyrene obtained with quartz standard
journal, June 2009


Equation of state and optical luminosity of benzene, polybutene, and polyethylene shocked to 210 GPa (2.1 Mbar)
journal, March 1984


Hydrogen Bonding in Water
journal, November 2003


Equation of State of the Hydrogen Plasma by Path Integral Monte Carlo Simulation
journal, October 1994


Probing matter at Gbar pressures at the NIF
journal, March 2014


High-pressure, temperature elasticity of Fe- and Al-bearing MgSiO3: Implications for the Earth's lower mantle
journal, January 2016


Path-integral molecular dynamics simulation of diamond
journal, June 2006


Hugoniot and mean ionization of laser-shocked Ge-doped plastic
journal, December 2013


Thermophysical properties for shock compressed polystyrene
journal, August 2011


Equations of state and thermodynamic properties of hot plasma
journal, January 2017


Equation-of-state measurements for polystyrene at multi-TPa pressures in laser direct-drive experiments
journal, December 2005


Gigabar material properties experiments on nif and omega
conference, January 2012

  • Swift, Damian; Hawreliak, James; Braun, David
  • SHOCK COMPRESSION OF CONDENSED MATTER - 2011: Proceedings of the Conference of the American Physical Society Topical Group on Shock Compression of Condensed Matter, AIP Conference Proceedings
  • https://doi.org/10.1063/1.3686321

Instantaneous x-ray radiation energy from laser produced polystyrene plasmas for shock ignition conditions
journal, October 2013


Shock Hugoniot measurements of CH at Gbar pressures at the NIF
journal, March 2016


Time‐resolved measurements of laser‐induced shock waves in deuterated polystyrene porous targets by x‐ray backlighting
journal, March 1991


Simulation and understanding of atomic and molecular quantum crystals
journal, August 2017


Nuclear Quantum Effects in Water
journal, July 2008


Indirect drive ignition at the National Ignition Facility
journal, October 2016


First-principles equation of state calculations of warm dense nitrogen
journal, February 2016


Crystallization of the One-Component Plasma at Finite Temperature
journal, June 1996


Ab initio simulations of hot dense methane during shock experiments
journal, December 2012


High-precision measurements of the equation of state of hydrocarbons at 1–10 Mbar using laser-driven shock waves
journal, May 2010


First-principles equation of state and electronic properties of warm dense oxygen
journal, October 2015


Equation of State of Polystyrene and Polymethylmethacrylate from Ultrasonic Measurements at Moderate Pressures
journal, March 1972


Frontiers and Challenges in Warm Dense Matter
book, January 2014


Measuring high pressure equation of state of polystyrene using laser driven shock wave
journal, November 2015


A simulation-based and analytic analysis of the off-Hugoniot response of alternative inertial confinement fusion ablator materials
journal, September 2016


Path integral Monte Carlo simulation of the low-density hydrogen plasma
journal, May 2001


Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations
journal, April 2016


Quantum Nuclear Motion of Helium and Molecular Nitrogen Clusters in Carbon Nanotubes
journal, February 2017


Multiphase equation of state for carbon addressing high pressures and temperatures
journal, June 2014


Path Integral Monte Carlo Calculation of the Deuterium Hugoniot
journal, August 2000


Nuclear quantum dynamics in dense hydrogen
journal, June 2014


National direct-drive program on OMEGA and the National Ignition Facility
journal, October 2016


A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984


Purgatorio—a new implementation of the Inferno algorithm
journal, May 2006


Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981


Simulation of quantum many-body systems by path-integral methods
journal, September 1984


Shock-timing experiments in polystyrene target [透明材料中冲击波传播的时间特性研究]
journal, January 2010


Heat of polymerization of alpha-methylstyrene from heats of combustion of monomer and 4 polymer fractions
journal, January 1951


THE INTERIORS OF GIANT PLANETS: Models and Outstanding Questions
journal, May 2005


Properties of hydrogen, helium, and silicon dioxide mixtures in giant planet interiors
journal, April 2017


Anomalous Nuclear Quantum Effects in Ice
journal, May 2012


An Optimized Method for Treating Long-Range Potentials
journal, March 1995


Quantum effects on phase transitions in high-pressure ice
journal, February 1998


Quantum molecular dynamics study on the structures and dc conductivity of warm dense silane
journal, February 2014


Equations of State for Ablator Materials in Inertial Confinement Fusion Simulations
journal, May 2016


Absolute entropies, conformation, and Debye temperatures of bicyclo[2.2.2]octane- and of bicyclo[3.2.2]nonane-type molecules
journal, April 1971


Nuclear quantum effects in water
text, January 2008


Simulations of dense atomic hydrogen in the Wigner crystal phase
journal, September 2006


Using neutrons to measure keV temperatures in highly compressed plastic at multi-Gbar pressures
journal, December 2016


Optical properties of highly compressed polystyrene using laser-driven shockwaves
journal, July 2003


Superionic to Superionic Phase Change in Water: Consequences for the Interiors of Uranus and Neptune
journal, April 2013


Development of Path Integral Monte Carlo Simulations with Localized Nodal Surfaces for Second-Row Elements
journal, October 2015


Equation of state and shock compression of warm dense sodium—A first-principles study
journal, February 2017


The Gru¨neisen Parameter in Fluids
journal, June 1984


First-principles prediction of the softening of the silicon shock Hugoniot curve
journal, September 2016


An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+
journal, June 1998


Fermion nodes
journal, June 1991


Works referencing / citing this record:

Preface: Special Topic on Nuclear Quantum Effects
journal, March 2018


High Pressure Hydrocarbons Revisited: From van der Waals Compounds to Diamond
journal, May 2019


Equation of state of boron nitride combining computation, modeling, and experiment
journal, April 2019


First-Principles Equation of State Database for Warm Dense Matter Computation
text, January 2020


Magnesium oxide at extreme temperatures and pressures studied with first-principles simulations
journal, December 2019


Development and modeling of a polar-direct-drive exploding pusher platform at the National Ignition Facility
journal, July 2018


Application of quantum-statistical methods to studies of thermodynamic and radiative processes in hot dense plasmas
journal, September 2019