Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Stable Solid Molecular Hydrogen above 900 K from a Machine-Learned Potential Trained with Diffusion Quantum Monte Carlo

Journal Article · · Physical Review Letters
 [1];  [2];  [3];  [4];  [5];  [3]
  1. Harbin Inst. of Technology, Heilongjiang (China); University of Illinois at Urbana-Champaign
  2. Flatiron Inst., New York, NY (United States); Univ. of Illinois, Urbana, IL (United States)
  3. Univ. of Illinois, Urbana, IL (United States)
  4. Univ. Grenoble Alpes (France)
  5. Univ. of L’Aquila (Italy)
+ Show Author Affiliations

Here, we survey the phase diagram of high-pressure molecular hydrogen with path integral molecular dynamics using a machine-learned interatomic potential trained with quantum Monte Carlo forces and energies. Besides the HCP and C2/c–24 phases, we find two new stable phases both with molecular centers in the Fmmm–4 structure, separated by a molecular orientation transition with temperature. The high temperature isotropic Fmmm–4 phase has a reentrant melting line with a maximum at higher temperature (1450 K at 150 GPa) than previously estimated and crosses the liquid-liquid transition line around 1200 K and 200 GPa.

Research Organization:
Univ. of Illinois at Urbana-Champaign, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; NSF of China
Grant/Contract Number:
SC0020177; AC05-00OR22725
OSTI ID:
1958013
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 7 Vol. 130; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (47)

Monte Carlo and molecular dynamics of condensed matter systems: K. Binder and G. Ciccotti, eds., Editrice Compositori, Bologna, Italy, 1996 journal May 1997
Molecular dynamics of MgSiO3 perovskite at high pressures: Equation of state, structure, and melting transition journal October 1994
i-PI 2.0: A universal force engine for advanced molecular simulations journal March 2019
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales journal February 2022
Anomalous Melting Behavior of Solid Hydrogen at High Pressures journal May 2013
Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures journal July 2015
Raman spectroscopy of hot hydrogen above 200 GPa journal February 2015
Structure of phase III of solid hydrogen journal May 2007
Understanding high pressure molecular hydrogen with a hierarchical machine-learned potential journal October 2020
Semimetallic molecular hydrogen at pressure above 350 GPa journal September 2019
Ultrahigh-pressure isostructural electronic transitions in hydrogen journal September 2019
Synchrotron infrared spectroscopic evidence of the probable transition to metal hydrogen journal January 2020
Evidence for supercritical behaviour of high-pressure liquid hydrogen journal September 2020
On the liquid–liquid phase transition of dense hydrogen journal December 2021
Accurate Computation of Vibronic Energies and of Some Expectation Values for H 2 , D 2 , and T 2 journal December 1964
Nonadiabatic corrections to the wave function and energy journal July 2008
QMCPACK: Advances in the development, efficiency, and application of auxiliary field and real-space variational and diffusion quantum Monte Carlo journal May 2020
Bonding changes in hot fluid hydrogen at megabar pressures journal March 2011
Liquid–liquid phase transition in hydrogen by coupled electron–ion Monte Carlo simulations journal April 2016
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal September 2009
Advanced capabilities for materials modelling with Quantum ESPRESSO journal October 2017
QMCPACK : an open source ab initio quantum Monte Carlo package for the electronic structure of atoms, molecules and solids journal April 2018
On-the-fly machine learning force field generation: Application to melting points journal July 2019
High-pressure hydrogen by machine learning and quantum Monte Carlo journal July 2022
Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals journal June 1984
Principal Hugoniot, reverberating wave, and mechanical reshock measurements of liquid deuterium to 400 GPa using plate impact techniques journal April 2004
Evidence from x-ray diffraction of orientational ordering in phase III of solid hydrogen at pressures up to 183 GPa journal August 2010
Multiphase equation of state of hydrogen from ab initio calculations in the range 0.2 to 5 g/cc up to 10 eV journal March 2011
Benchmarking density functionals for hydrogen-helium mixtures with quantum Monte Carlo: Energetics, pressures, and forces journal January 2016
Theory of finite size effects for electronic quantum Monte Carlo calculations of liquids and solids journal July 2016
Melting Line of Hydrogen at High Pressures journal April 2008
Gaussian Approximation Potentials: The Accuracy of Quantum Mechanics, without the Electrons journal April 2010
Nuclear Quantum Effects and Nonlocal Exchange-Correlation Functionals Applied to Liquid Hydrogen at High Pressure journal February 2013
High-Precision Shock Wave Measurements of Deuterium: Evaluation of Exchange-Correlation Functionals at the Molecular-to-Atomic Transition journal January 2017
Melting and High P − T Transitions of Hydrogen up to 300 GPa journal August 2017
Deep Potential Molecular Dynamics: A Scalable Model with the Accuracy of Quantum Mechanics journal April 2018
Energy Gap Closure of Crystalline Molecular Hydrogen with Pressure journal March 2020
Compression of D2 to 460 GPa and Isotopic Effects in the Path to Metal Hydrogen journal July 2022
Semiempirical, Quantum Mechanical Calculation of Hydrogen Embrittlement in Metals journal April 1983
Accurate, Efficient, and Simple Forces Computed with Quantum Monte Carlo Methods journal January 2005
Finite-Size Error in Many-Body Simulations with Long-Range Interactions journal August 2006
The properties of hydrogen and helium under extreme conditions journal November 2012
FINDSYM : program for identifying the space-group symmetry of a crystal journal January 2005
Observation of the Wigner-Huntington transition to metallic hydrogen journal January 2017
Insulator-metal transition in dense fluid deuterium journal August 2018
Evidence of maximum in the melting curve of hydrogen at megabar pressures journal April 2009
Deep Potential: A General Representation of a Many-Body Potential Energy Surface journal January 2018

Similar Records

First-principles temperature-pressure phase diagram of magnesium
Journal Article · Tue Feb 28 23:00:00 EST 1995 · Physical Review, B: Condensed Matter; (United States) · OSTI ID:6450462
Liquid-liquid phase transition of hydrogen and its critical point: Analysis from ab initio simulation and a machine-learned potential
Journal Article · Mon Apr 21 00:00:00 EDT 2025 · Physical Review. E · OSTI ID:2561245
High temperature melting of dense molecular hydrogen from machine-learning interatomic potentials trained on quantum Monte Carlo
Journal Article · Tue Feb 04 23:00:00 EST 2025 · Journal of Chemical Physics · OSTI ID:2561243

Related Subjects

08 HYDROGEN
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
artificial neural networks
compressed hydrogen
deep learning
diffusion quantum Monte Carlo
electronic structure
equations of state
first-principles calculations
high pressure
hydrogen
machine learning
molecular dynamics
path-integral Monte Carlo
path-integral methods
phase diagrams
phase transitions
quantum monte Carlo