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Title: Optical properties of high-pressure fluid hydrogen across molecular dissociation

Abstract

Optical properties of compressed fluid hydrogen in the region where dissociation and metallization is observed are computed by ab initio methods and compared with recent experimental results. We confirm that at T > 3,000 K, both processes are continuous, while at T < 1,500 K, the first-order phase transition is accompanied by a discontinuity of the dc conductivity and the thermal conductivity, while both the reflectivity and absorption coefficient vary rapidly but continuously. Our results support the recent analysis of National Ignition Facility (NIF) experiments [Celliers PM, et al. (2018) Science 361:677–682], which assigned the inception of metallization to pressures where the reflectivity is ~0.3. Furthermore, our results also support the conclusion that the temperature plateau seen in laser-heated diamond-anvil cell (DAC) experiments at temperatures higher than 1,500 K corresponds to the onset of optical absorption, not to the phase transition.

Authors:
; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1509943
Alternate Identifier(s):
OSTI ID: 1545367
Grant/Contract Number:  
2911; AC52-07NA27344; HyLightExtreme
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; hydrogen; high pressure; metal insulator; optical properties; quantum Monte Carlo

Citation Formats

Rillo, Giovanni, Morales, Miguel A., Ceperley, David M., and Pierleoni, Carlo. Optical properties of high-pressure fluid hydrogen across molecular dissociation. United States: N. p., 2019. Web. doi:10.1073/pnas.1818897116.
Rillo, Giovanni, Morales, Miguel A., Ceperley, David M., & Pierleoni, Carlo. Optical properties of high-pressure fluid hydrogen across molecular dissociation. United States. https://doi.org/10.1073/pnas.1818897116
Rillo, Giovanni, Morales, Miguel A., Ceperley, David M., and Pierleoni, Carlo. Tue . "Optical properties of high-pressure fluid hydrogen across molecular dissociation". United States. https://doi.org/10.1073/pnas.1818897116.
@article{osti_1509943,
title = {Optical properties of high-pressure fluid hydrogen across molecular dissociation},
author = {Rillo, Giovanni and Morales, Miguel A. and Ceperley, David M. and Pierleoni, Carlo},
abstractNote = {Optical properties of compressed fluid hydrogen in the region where dissociation and metallization is observed are computed by ab initio methods and compared with recent experimental results. We confirm that at T > 3,000 K, both processes are continuous, while at T < 1,500 K, the first-order phase transition is accompanied by a discontinuity of the dc conductivity and the thermal conductivity, while both the reflectivity and absorption coefficient vary rapidly but continuously. Our results support the recent analysis of National Ignition Facility (NIF) experiments [Celliers PM, et al. (2018) Science 361:677–682], which assigned the inception of metallization to pressures where the reflectivity is ~0.3. Furthermore, our results also support the conclusion that the temperature plateau seen in laser-heated diamond-anvil cell (DAC) experiments at temperatures higher than 1,500 K corresponds to the onset of optical absorption, not to the phase transition.},
doi = {10.1073/pnas.1818897116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = ,
volume = ,
place = {United States},
year = {Tue Apr 30 00:00:00 EDT 2019},
month = {Tue Apr 30 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1073/pnas.1818897116

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Cited by: 27 works
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Works referenced in this record:

Pathways to metallic hydrogen
journal, April 2009

  • Silvera, I. F.; Deemyad, S.
  • Low Temperature Physics, Vol. 35, Issue 4
  • DOI: 10.1063/1.3115820

Phase boundary of hot dense fluid hydrogen
journal, November 2015

  • Ohta, Kenji; Ichimaru, Kota; Einaga, Mari
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep16560

Benchmarking vdW-DF first-principles predictions against Coupled Electron-Ion Monte Carlo for high-pressure liquid hydrogen
journal, February 2019

  • Gorelov, Vitaly; Pierleoni, Carlo; Ceperley, David M.
  • Contributions to Plasma Physics, Vol. 59, Issue 4-5
  • DOI: 10.1002/ctpp.201800185

Metallization of fluid hydrogen
journal, January 1998

  • Nellis, W. J.; Louis, A. A.; Ashcroft, N. W.
  • Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 356, Issue 1735
  • DOI: 10.1098/rsta.1998.0153

Optical Properties of Fluid Hydrogen at the Transition to a Conducting State
journal, June 2016


Critical point and mechanism of the fluid–fluid phase transition in warm dense hydrogen
journal, June 2017


Quantum Monte Carlo Simulation of the High-Pressure Molecular-Atomic Crossover in Fluid Hydrogen
journal, December 2006


Hydrogen-helium mixtures in the interiors of giant planets
journal, January 2007


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Properties of Dense Fluid Hydrogen and Helium in Giant Gas Planets
journal, July 2007

  • Vorberger, J.; Tamblyn, I.; Bonev, St. A.
  • Contributions to Plasma Physics, Vol. 47, Issue 4-5
  • DOI: 10.1002/ctpp.200710050

Energy band gaps and lattice parameters evaluated with the Heyd-Scuseria-Ernzerhof screened hybrid functional
journal, November 2005

  • Heyd, Jochen; Peralta, Juan E.; Scuseria, Gustavo E.
  • The Journal of Chemical Physics, Vol. 123, Issue 17
  • DOI: 10.1063/1.2085170

Striking isotope effect on the metallization phase lines of liquid hydrogen and deuterium
journal, September 2018


Molecular Dissociation in Hot, Dense Hydrogen
journal, February 1996


Local structure in dense hydrogen at the liquid-liquid phase transition by coupled electron-ion Monte Carlo
journal, December 2017

  • Pierleoni, Carlo; Holzmann, Markus; Ceperley, David M.
  • Contributions to Plasma Physics, Vol. 58, Issue 2-3
  • DOI: 10.1002/ctpp.201700184

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

  • Pierleoni, Carlo; Morales, Miguel A.; Rillo, Giovanni
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 18
  • DOI: 10.1073/pnas.1603853113

Electron localization properties in high pressure hydrogen at the liquid-liquid phase transition by Coupled Electron-Ion Monte Carlo
journal, December 2018


Free energy methods in coupled electron ion Monte Carlo
journal, December 2011


Evidence of a liquid-liquid phase transition in hot dense hydrogen
journal, April 2013

  • Dzyabura, V.; Zaghoo, M.; Silvera, I. F.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 20
  • DOI: 10.1073/pnas.1300718110

Direct observation of an abrupt insulator-to-metal transition in dense liquid deuterium
journal, June 2015


Minimum metallic conductivity of fluid hydrogen at 140 GPa (1.4 Mbar)
journal, February 1999


Insulator-metal transition in dense fluid deuterium
journal, August 2018


Phase Diagram of Hydrogen and a Hydrogen-Helium Mixture at Planetary Conditions by Quantum Monte Carlo Simulations
journal, January 2018


Electronic transport coefficients from ab initio simulations and application to dense liquid hydrogen
journal, June 2011


The properties of hydrogen and helium under extreme conditions
journal, November 2012

  • McMahon, Jeffrey M.; Morales, Miguel A.; Pierleoni, Carlo
  • Reviews of Modern Physics, Vol. 84, Issue 4
  • DOI: 10.1103/RevModPhys.84.1607

Plasma phase transition in hydrogen
journal, March 1985


A quantum fluid of metallic hydrogen suggested by first-principles calculations
journal, October 2004

  • Bonev, Stanimir A.; Schwegler, Eric; Ogitsu, Tadashi
  • Nature, Vol. 431, Issue 7009
  • DOI: 10.1038/nature02968

Conductivity and dissociation in liquid metallic hydrogen and implications for planetary interiors
journal, October 2017

  • Zaghoo, Mohamed; Silvera, Isaac F.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 45
  • DOI: 10.1073/pnas.1707918114

Metallization of Fluid Molecular Hydrogen at 140 GPa (1.4 Mbar)
journal, March 1996


Electronic excitations and metallization of dense solid hydrogen
journal, July 2013

  • Cohen, R. E.; Naumov, Ivan I.; Hemley, Russell J.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 34
  • DOI: 10.1073/pnas.1312256110

Thermophysical properties of warm dense hydrogen using quantum molecular dynamics simulations
journal, May 2008


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

  • Morales, M. A.; Pierleoni, C.; Schwegler, E.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 29
  • DOI: 10.1073/pnas.1007309107

Nuclear Quantum Effects and Nonlocal Exchange-Correlation Functionals Applied to Liquid Hydrogen at High Pressure
journal, February 2013


Phase Transition in a Strongly Nonideal Deuterium Plasma Generated by Quasi-Isentropical Compression at Megabar Pressures
journal, October 2007


Fluid hydrogen at high density: The plasma phase transition
journal, May 1989


First-order liquid-liquid phase transition in dense hydrogen
journal, November 2010


Liquid-liquid phase transition in compressed hydrogen from first-principles simulations
journal, March 2003


The Boltzmann Equation in the Theory of Electrical Conduction in Metals
journal, April 1958


Evidence of a first-order phase transition to metallic hydrogen
journal, April 2016