Starting from the amorphous ground state: Linking landscape thermodynamics to slow dynamics and crossover
A microscopic understanding of low-temperature thermodynamics and its relation to dynamical features, such as a fragile-to-strong crossover (FSC) remains a central challenge in glass physics. Using swap Monte Carlo combined with a full potential-energy-landscape (PEL) analysis of a non-network-forming model, we obtain equilibrium data deep into the glassy regime and identify a finite system size that simultaneously reproduces bulk behavior for T ≳ Tg/2 and allows complete sampling of the PEL down to its lowest-energy amorphous states. This enables the direct computation of the configurational entropy over the full temperature range of the finite system without relying on liquid-state thermodynamic integration. We find a pronounced depletion of low-energy states relative to the Gaussian regime of the PEL, which governs the low-temperature curvature of the configurational entropy. Numerically, the apparent activation energy of the diffusivity closely follows the temperature dependence of the mean inherent structure energy and exhibits a gradual crossover toward Arrhenius-like behavior. This correlation is consistent with a trap-model description of the PEL, in which the FSC emerges naturally as a consequence of the depletion of low-energy states and, thus, of the lower bound of the PEL. We further argue, as illustrated analytically for a simple binomial model of the PEL, that the observability of a FSC depends on whether the depletion regime is reached within the accessible temperature window.
Authors
- Andreas Heuer (ORCID: https://orcid.org/0000-0003-2592-0287)
- Anshul D. S. Parmar (ORCID: https://orcid.org/0000-0002-0380-8393)
- Simon G. Kellers (ORCID: https://orcid.org/0009-0008-1525-5758)
Institutions
- University of Münster (DE)
- Helmholtz-Institute Münster (DE)
- FH Münster University of Applied Sciences (DE)
Publication Details
- Journal
- The Journal of Chemical Physics
- Published
- 2026-05-21
- DOI
- https://doi.org/10.1063/5.0325432
- Primary Topic
- Material Dynamics and Properties
- Type
- article
- Field-Weighted Citation Impact
- 0.00