- Physical Review Journals
All JournalsPhysics Magazine

Physical Review Research

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Opposite quantum fluctuation effects on the vitrification of two atomic model liquids

Yang Zhou1,2,*, Ali Eltareb1,2, Gustavo E. Lopez3,4,†, and Nicolas Giovambattista1,2,4,‡

  • *Contact author: yzhou4@gradcenter.cuny.edu
  • †Contact author: gustavo.lopez1@lehman.cuny.edu
  • ‡Contact author: ngiovambattista@brooklyn.cuny.edu
PDF

Phys. Rev. Research 8, 043110 – Published 30 October, 2026

DOI: https://doi.org/10.1103/xfmw-ynv4

Abstract

Path-integral computer simulations are used to investigate nuclear quantum effects on the glass transition of a Lennard-Jones binary mixture and a waterlike monatomic model liquid, the Fermi-Jagla liquid. As in previous studies, we find that introducing realistic atoms delocalization (nuclear quantum effects) suppresses atomic diffusivity in the Lennard-Jones binary mixture. Instead, nuclear quantum effects enhance the dynamics of the Fermi-Jagla liquid. Hence, nuclear quantum effects can either inhibit or promote the vitrification of atomic liquids depending on the atomic interactions. Notably, both systems exhibit qualitatively similar atoms delocalization and become less structured upon the inclusion of nuclear quantum effects, despite the divergent effects on their dynamics. A qualitative explanation of the different nuclear quantum effects on the dynamics of the Lennard-Jones binary mixture and Fermi-Jagla liquid is provided in terms of the features in the corresponding pair potential interactions. Our observations can be naturally interpreted through the potential energy landscape (PEL) formalism for quantum liquids. At a given temperature, introducing nuclear quantum effects forces the Lennard-Jones binary mixture to explore deeper regions of the PEL, where topographical features significantly affect the dynamics, while the Fermi-Jagla liquid is driven to explore higher regions of the PEL, where the PEL topography plays a secondary role. This is ultimately due to the opposite nuclear quantum effects on the PEL basins’ shape (curvature) of the Lennard-Jones binary mixture and Fermi-Jagla liquid.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (34)

  1. P. G. Debenedetti and F. H. Stillinger, Supercooled liquids and the glass transition, Nature (London) 410, 259 (2001).
  2. L. Berthier and G. Biroli, Theoretical perspective on the glass transition and amorphous materials, Rev. Mod. Phys. 83, 587 (2011).
  3. C. Gainaru, A. L. Agapov, V. Fuentes-Landete, K. Amann-Winkel, H. Nelson, K. W. Köster, A. I. Kolesnikov, V. N. Novikov, R. Richert, R. Böhmer, T. Loerting, and A. P. Sokolov, Anomalously large isotope effect in the glass transition of water, Proc. Natl. Acad. Sci. USA 111, 17402 (2014).
  4. M. Ceriotti, W. Fang, P. G. Kusalik, R. H. McKenzie, A. Michaelides, M. A. Morales, and T. E. Markland, Nuclear quantum effects in water and aqueous systems: Experiment, theory, and current challenges, Chem. Rev. 116, 7529 (2016).
  5. A. Amir, Y. Oreg, and Y. Imry, Slow relaxations and aging in the electron glass, Phys. Rev. Lett. 103, 126403 (2009).
  6. W. Wu, B. Ellman, T. F. Rosenbaum, G. Aeppli, and D. H. Reich, From classical to quantum glass, Phys. Rev. Lett. 67, 2076 (1991).
  7. A. D. King, J. Raymond, T. Lanting, R. Harris, A. Zucca, F. Altomare, A. J. Berkley, K. Boothby, S. Ejtemaee, C. Enderud, et al., Quantum critical dynamics in a 5,000-qubit programmable spin glass, Nature (London) 617, 61 (2023).
  8. T. E. Markland, J. A. Morrone, B. J. Berne, K. Miyazaki, E. Rabani, and D. R. Reichman, Quantum fluctuations can promote or inhibit glassformation, Nat. Phys. 7, 134 (2011).
  9. G. Biroli and F. Zamponi, A tentative replica theory of glassy helium 4, J. Low Temp. Phys. 168, 101 (2012).
  10. T. E. Markland, J. A. Morrone, K. Miyazaki, B. J. Berne, D. R. Reichman, and E. Rabani, Theory and simulations of quantum glass forming liquids, J. Chem. Phys. 136, 074511 (2012).
  11. W. Kob and H. C. Andersen, Testing mode-coupling theory for a supercooled binary Lennard-Jones mixture I: The van Hove correlation function, Phys. Rev. E 51, 4626 (1995).
  12. J. Y. Abraham, S. V. Buldyrev, and N. Giovambattista, Liquid and glass polymorphism in a monatomic system with isotropic, smooth pair interactions, J. Phys. Chem. B 115, 14229 (2011).
  13. G. Sun, L. Xu, and N. Giovambattista, Relationship between the potential energy landscape and the dynamic crossover in a water-like monatomic liquid with a liquid-liquid phase transition, J. Chem. Phys. 146, 014503 (2017).
  14. N. Giovambattista and G. E. Lopez, Potential energy landscape formalism for quantum liquids, Phys. Rev. Res. 2, 043441 (2020).
  15. Y. Zhou, G. E. Lopez, and N. Giovambattista, The harmonic and Gaussian approximations in the potential energy landscape formalism for quantum liquids, J. Chem. Theory Comput. 20, 1847 (2024).
  16. L. Xu, S. V. Buldyrev, N. Giovambattista, and H. E. Stanley, Liquid-liquid phase transition and glass transition in a monoatomic model system, Int. J. Mol. Sci. 11, 5184 (2010).
  17. N. Giovambattista, The liquid-liquid phase transition, anomalous properties, and glass behavior of polymorphic liquids, in Advances in Chemical Physics, edited by H. E. Stanley, 1st ed. (Wiley, Hoboken, New Jersey, 2013), Vol. 152, pp. 113–138.
  18. B. Nguyen, G. E. Lopez, and N. Giovambattista, Nuclear quantum effects on the liquid–liquid phase transition of a water-like monatomic liquid, Phys. Chem. Chem. Phys. 20, 8210 (2018).
  19. A. Eltareb, G. E. Lopez, and N. Giovambattista, Nuclear quantum effects on the dynamics and glass behavior of a monatomic liquid with two liquid states, J. Chem. Phys. 156, 204502 (2022).
  20. A. Eltareb, G. E. Lopez, and N. Giovambattista, Nuclear quantum effects on the thermodynamic, structural, and dynamical properties of water, Phys. Chem. Chem. Phys. 23, 6914 (2021).
  21. A. Eltareb, G. E. Lopez, and N. Giovambattista, Nuclear quantum effects on the equation of state of water: Insights from the potential energy landscape formalism, J. Chem. Theory Comput. 22 3208 (2026).
  22. B. E. Ugur and M. A. Webb, Nuclear quantum effects in molecular liquids across chemical space, Nat. Commun. 16, 5786 (2025).
  23. I. R. Craig and D. E. Manolopoulos, Quantum statistics and classical mechanics: Real time correlation functions from ring polymer molecular dynamics, J. Chem. Phys. 121, 3368 (2004).
  24. P. Eastman, J. Swails, J. D. Chodera, R. T. McGibbon, Y. Zhao, K. A. Beauchamp, L.-P. Wang, A. C. Simmonett, M. P. Harrigan, C. D. Stern, R. P. Wiewiora, B. R. Brooks, and V. S. Pande, OpenMM 7: Rapid development of high performance algorithms for molecular dynamics, PLoS Comput. Biol. 13, e1005659 (2017).
  25. C. P. Herrero and R. Ramírez, Path-integral simulation of solids, J. Phys.: Condens. Matter 26, 233201 (2014).
  26. Y. Zhou, A. Eltareb, G. E. Lopez, and N. Giovambattista, Configurational entropy and Adam-Gibbs relation for quantum liquids, Nat. Commun. 17, 4843 (2026).
  27. F. H. Stillinger, Energy Landscapes, Inherent Structures, and Condensed-Matter Phenomena (Princeton University Press, Princeton, New Jersey, 2015).
  28. P. Virtanen, R. Gommers, T. E. Oliphant, M. Haberland, T. Reddy, D. Cournapeau, E. Burovski, P. Peterson, W. Weckesser, J. Bright, et al., SciPy 1.0: Fundamental algorithms for scientific computing in Python, Nat. Methods 17, 261 (2020).
  29. S. Sastry, P. G. Debenedetti, and F. H. Stillinger, Signatures of distinct dynamical regimes in the energy landscape of a glass-forming liquid, Nature (London) 393, 554 (1998).
  30. F. Zamponi, Quantum glass forging, Nat. Phys. 7, 99 (2011).
  31. A. Eltareb, Y. Zhou, G. E. Lopez, and N. Giovambattista, Potential energy landscape formalism for quantum molecular liquids, Commun. Chem. 7, 289 (2024).
  32. A. Eltareb, G. E. Lopez, and N. Giovambattista, Isotope-substitution effects on the thermodynamic, dynamic, and structural properties of water: H2O, HDO, D2O, and T2O, J. Phys. Chem. B 129, 6886 (2025).
  33. F. H. Stillinger and T. A. Weber, Hidden structure in liquids, Phys. Rev. A 25, 978 (1982).
  34. F. Sciortino, Potential energy landscape description of supercooled liquids and glasses, J. Stat. Mech. (2005) P05015.

Outline

Information

Phys. Rev. Research 8, 043110– Published 30 October, 2026
  • Received 18 June 2026
  • Accepted 8 October 2026
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation