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Liquid-liquid phase transition of hydrogen and its critical point: Analysis from ab initio simulation and a machine-learned potential

Journal Article · · Physical Review. E
 [1];  [2];  [3];  [4];  [5];  [2]
  1. Univ. Grenoble Alpes (France); University of Illinois
  2. University of Illinois, Urbana, IL (United States)
  3. Flatiron Institute, New York, NY (United States); Hofstra University, Hempstead, NY (United States)
  4. Univ. Grenoble Alpes (France)
  5. University of L'Aquila (Italy)
+ Show Author Affiliations

We simulate high-pressure hydrogen in its liquid phase close to molecular dissociation using a machine-learned interatomic potential. The model is trained with density functional theory (DFT) forces and energies, with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional. We show that an accurate NequIP model, an E(3)-equivariant neural network potential, accurately reproduces the phase transition present in PBE. Moreover, the computational efficiency of this model allows for substantially longer molecular dynamics trajectories, enabling us to perform a finite-size scaling (FSS) analysis to distinguish between a crossover and a true first-order phase transition. Here, we locate the critical point of this transition, the liquid-liquid phase transition (LLPT), at 1200-1300 K and 155-160 GPa, a temperature lower than most previous estimates and close to the melting transition.

Research Organization:
University of Illinois, Urbana, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
SC0020177
OSTI ID:
2561245
Journal Information:
Physical Review. E, Journal Name: Physical Review. E Journal Issue: 4 Vol. 111; ISSN 2470-0045
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

08 HYDROGEN
Ab initio molecular dynamics
Finite-size scaling
Molecular dynamics