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.

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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
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article

Starting from the amorphous ground state: Linking landscape thermodynamics to slow dynamics and crossover

Andreas Heuer, Anshul D. S. Parmar, Simon G. Kellers
The Journal of Chemical Physics
Material Dynamics and Properties
article

Starting from the amorphous ground state: Linking landscape thermodynamics to slow dynamics and crossover

Andreas Heuer, Anshul D. S. Parmar, Simon G. Kellers
article en

Abstract

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.

The Journal of Chemical PhysicsVol. 164(19)
University of Münster (DE), Helmholtz-Institute Münster (DE), FH Münster University of Applied Sciences (DE)
Openalex Percentile: Top 12%
Material Dynamics and Properties
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