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On the liquid–liquid phase transition of dense hydrogen

Nature volume 600, pages E12–E14 (2021)Cite this article

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Matters Arising to this article was published on 15 December 2021

The Original Article was published on 09 September 2020

arising from B. Cheng et al. Nature https://doi.org/10.1038/s41586-020-2677-y (2020)

Until recently, the consensus theoretical and computational interpretation of the liquid–liquid phase transition (LLPT) of high-pressure hydrogen—which has proved challenging to determine—has been that it is first order1,2,3,4,5. Cheng et al.6 developed a machine learning potential (MLP) that, in larger-than-previous molecular dynamics (MD) simulations, gives a continuous transition instead. We show that the MLP does not reproduce our still larger density functional theory MD (DFT-MD) calculations as it should. As the MLP is not a faithful surrogate for the DFT-MD, the prediction of a supercritical atomic liquid by Cheng et al.6 is unfounded.

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Fig. 1: Comparison of MD results from the PBE exchange-correlation-based MLP and ab initio DFT-MD NPT simulations.
Fig. 2: The LLPT boundary from the present large-scale DFT-MD (DFT/PBE) simulations compared to MLP (MLP/PBE) CPmax and ρmax curves.

Data availability

The data that support the findings shown in the figures are available from the corresponding author upon reasonable request.

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Acknowledgements

This report was prepared as an account of work sponsored by an agency of the U.S. Government. Neither the U.S. Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark,manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the U.S. Government orany agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the U.S. Government or any agency thereof. V.V.K., J.H. and S.X.H. were supported by the Department of Energy National Nuclear Security Administration Award Number DE-NA0003856 and US National Science Foundation PHY Grant No. 1802964. Partial funding for S.X.H. was provided by the NSF Physics Frontier Center Award PHY-2020249. S.B.T. was supported by Department of Energy Grant DE-SC0002139. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Part of the computations were performed on the Laboratory for Laser Energetics HPC systems.

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Authors and Affiliations

  1. Laboratory for Laser Energetics, University of Rochester, Rochester, NY, USA

    Valentin V. Karasiev, Joshua Hinz & S. X. Hu

  2. Quantum Theory Project, Department of Physics, University of Florida, Gainesville, FL, USA

    S. B. Trickey

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  1. Valentin V. Karasiev
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Contributions

V.V.K. conceived the project and designed the study. V.V.K. and J.H. performed the DFT-MD simulations and postprocessed the data. V.V.K. wrote the initial manuscript with inputs from S.X.H. S.B.T. revised the conception and scope. V.V.K. and S.B.T rewrote the manuscript. All authors discussed the results and revised the paper extensively.

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Correspondence to Valentin V. Karasiev.

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This file contains Supplementary Information, Figs. 1–3, refs. 1–7.

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Karasiev, V.V., Hinz, J., Hu, S.X. et al. On the liquid–liquid phase transition of dense hydrogen. Nature 600, E12–E14 (2021). https://doi.org/10.1038/s41586-021-04078-x

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