Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations

Pierleoni, Carlo; Morales, Miguel A.; Rillo, Giovanni; Holzmann, Markus; Ceperley, David M.

doi:10.1073/pnas.1603853113

Title: Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations

Abstract

We report results of quantum Monte Carlo simulations that indicate that the two phenomena occur simultaneously through a first-order phase transition in fluid hydrogen at megabar pressures and temperatures of 1,000 K. The predicted pressures are close to claims of metallization based on static compression experiments but are lower than that of recent dynamic compression measurements. The simulation results represent the most reliable theoretical prediction yet of the liquid–liquid transition in hydrogen and provide constraints for future experiments.

Authors:

; Morales, Miguel A.; Rillo, Giovanni; Holzmann, Markus; Ceperley, David M.

Publication Date:: Wed Apr 20 00:00:00 EDT 2016

Research Org.:: Univ. of Illinois at Urbana-Champaign, IL (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1248409

Alternate Identifier(s):: OSTI ID: 1335030; OSTI ID: 1358614; OSTI ID: 1368010

Report Number(s):: LLNL-JRNL-680318
Journal ID: ISSN 0027-8424

Grant/Contract Number:: AC52-07NA27344; NA0001789; NA0002911

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 Volume: 113 Journal Issue: 18; Journal ID: ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)

Country of Publication:: United States

Language:: English

Subject:: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 97 MATHEMATICS AND COMPUTING; high pressure; phase transitions; quantum Monte Carlo; hydrogen metallization; molecular dissociation; 97 MATHEMATICS, COMPUTING, AND INFORMATION SCIENCE

Citation Formats


                    Pierleoni, Carlo, Morales, Miguel A., Rillo, Giovanni, Holzmann, Markus, and Ceperley, David M. Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations.  United States: N. p., 2016. 
Web.  doi:10.1073/pnas.1603853113.

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                    Pierleoni, Carlo, Morales, Miguel A., Rillo, Giovanni, Holzmann, Markus, & Ceperley, David M. Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations.  United States.  https://doi.org/10.1073/pnas.1603853113

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                    Pierleoni, Carlo, Morales, Miguel A., Rillo, Giovanni, Holzmann, Markus, and Ceperley, David M. Wed .  
"Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations".  United States.  https://doi.org/10.1073/pnas.1603853113.

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@article{osti_1248409,

  title        = {Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations},

  author       = {Pierleoni, Carlo and Morales, Miguel A. and Rillo, Giovanni and Holzmann, Markus and Ceperley, David M.},

  abstractNote = {We report results of quantum Monte Carlo simulations that indicate that the two phenomena occur simultaneously through a first-order phase transition in fluid hydrogen at megabar pressures and temperatures of 1,000 K. The predicted pressures are close to claims of metallization based on static compression experiments but are lower than that of recent dynamic compression measurements. The simulation results represent the most reliable theoretical prediction yet of the liquid–liquid transition in hydrogen and provide constraints for future experiments.},

  doi          = {10.1073/pnas.1603853113},

  journal      = {Proceedings of the National Academy of Sciences of the United States of America},

  number       = 18,

  volume       = 113,

  place        = {United States},

  year         = {Wed Apr 20 00:00:00 EDT 2016},

  month        = {Wed Apr 20 00:00:00 EDT 2016}

}

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Title: Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations

Abstract

Citation Formats

Phase boundary of hot dense fluid hydrogen journal, November 2015

Progress in Warm Dense Matter and Planetary Physics book, January 2014

Synchrotron Infrared Measurements of Dense Hydrogen to 360 GPa journal, April 2012

High-Pressure Measurements of Hydrogen Phase IV Using Synchrotron Infrared Spectroscopy journal, May 2013

First Principles Methods: A Perspective from Quantum Monte Carlo journal, December 2013

Quantum Monte Carlo simulations of solids journal, January 2001

Molecular Dissociation in Hot, Dense Hydrogen journal, February 1996

Dynamic compression of materials: metallization of fluid hydrogen at high pressures journal, April 2006

The solid molecular hydrogens in the condensed phase: Fundamentals and static properties journal, April 1980

Unexpectedly high pressure for molecular dissociation in liquid hydrogen by electronic simulation journal, March 2014

Mixed Molecular and Atomic Phase of Dense Hydrogen journal, March 2012

Hydrogen at high pressure journal, November 1999

Optical studies of solid hydrogen to 320 GPa and evidence for black hydrogen journal, April 2002

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

Thermodynamic properties and electrical conductivity of hydrogen under multiple shock compression to 150 GPa journal, April 1999

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

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

Distinct Metallization and Atomization Transitions in Dense Liquid Hydrogen journal, March 2015

Raman spectroscopy of hot hydrogen above 200 GPa journal, February 2015

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

Plasma phase transition in hydrogen journal, March 1985

Raman measurements of phase transitions in dense solid hydrogen and deuterium to 325 GPa journal, March 2014

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

On the Possibility of a Metallic Modification of Hydrogen journal, December 1935

Ultrahigh-pressure transitions in solid hydrogen journal, April 1994

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

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

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

Benchmarking exchange-correlation functionals for hydrogen at high pressures using quantum Monte Carlo journal, May 2014

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

Pressure-produced ionization of nonideal plasma in a megabar range of dynamic pressures journal, August 2003

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

Conductive dense hydrogen journal, November 2011

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

Phase boundary of hot dense fluid hydrogen
journal, November 2015

Progress in Warm Dense Matter and Planetary Physics
book, January 2014

Synchrotron Infrared Measurements of Dense Hydrogen to 360 GPa
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High-Pressure Measurements of Hydrogen Phase IV Using Synchrotron Infrared Spectroscopy
journal, May 2013

First Principles Methods: A Perspective from Quantum Monte Carlo
journal, December 2013

Quantum Monte Carlo simulations of solids
journal, January 2001

Molecular Dissociation in Hot, Dense Hydrogen
journal, February 1996

Dynamic compression of materials: metallization of fluid hydrogen at high pressures
journal, April 2006

The solid molecular hydrogens in the condensed phase: Fundamentals and static properties
journal, April 1980

Unexpectedly high pressure for molecular dissociation in liquid hydrogen by electronic simulation
journal, March 2014

Mixed Molecular and Atomic Phase of Dense Hydrogen
journal, March 2012

Hydrogen at high pressure
journal, November 1999

Optical studies of solid hydrogen to 320 GPa and evidence for black hydrogen
journal, April 2002

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

Thermodynamic properties and electrical conductivity of hydrogen under multiple shock compression to 150 GPa
journal, April 1999

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

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

Distinct Metallization and Atomization Transitions in Dense Liquid Hydrogen
journal, March 2015

Raman spectroscopy of hot hydrogen above 200 GPa
journal, February 2015

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

Plasma phase transition in hydrogen
journal, March 1985

Raman measurements of phase transitions in dense solid hydrogen and deuterium to 325 GPa
journal, March 2014

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

On the Possibility of a Metallic Modification of Hydrogen
journal, December 1935

Ultrahigh-pressure transitions in solid hydrogen
journal, April 1994

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

Evidence for a first-order liquid-liquid transition in high-pressure hydrogen from ab initio simulations
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Nuclear Quantum Effects and Nonlocal Exchange-Correlation Functionals Applied to Liquid Hydrogen at High Pressure
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Benchmarking exchange-correlation functionals for hydrogen at high pressures using quantum Monte Carlo
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Phase Transition in a Strongly Nonideal Deuterium Plasma Generated by Quasi-Isentropical Compression at Megabar Pressures
journal, October 2007

Pressure-produced ionization of nonideal plasma in a megabar range of dynamic pressures
journal, August 2003

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

Conductive dense hydrogen
journal, November 2011

Evidence of a first-order phase transition to metallic hydrogen
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