The End of Chaos at the Ideal Glass Transition

The ideal glass transition has often been associated with the extrapolated vanishing of configurational entropy $S_c$, yet how this thermodynamic criterion is reflected in microscopic dynamics remains unclear. Here, we show that the vanishing of deterministic chaos quantified by the maximum Lyapunov exponent $λ_{\mathrm{max}}$ provides such a dynamical signature. Using molecular dynamics simulations across diverse model glass-forming liquids in two and three dimensions, we show that $λ_{\mathrm{max}}$ follows an approximate scaling $λ_{\mathrm{max}} \propto (T-T_λ)^{1/2}$ and extrapolates to zero at a temperature $T_λ$ consistent with the Kauzmann temperature $T_{\mathrm{K}}$. Furthermore, we establish the quantitative relation $λ_{\mathrm{max}}^2 \propto T S_c$, directly linking chaotic dynamics to configurational entropy. By demonstrating that $λ_{\mathrm{max}}^2 \propto σ_K^2$, where $σ_K^2$ is the variance of local potential energy landscape curvature fluctuations, we connect the suppression of chaos directly to landscape geometry. These results provide a unified thermodynamic, dynamical, and geometric framework for glass formation, identifying the ideal glass transition as the endpoint of chaotic exploration of the energy landscape.

Authors

Publication Details

Journal
arXiv (Cornell University)
Published
2026-10-29
DOI
https://doi.org/10.48550/arxiv.2610.39098
Primary Topic
Material Dynamics and Properties
Type
preprint
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preprint

The End of Chaos at the Ideal Glass Transition

Matteo Baggioli, Wen-Sheng Xu, Jack Douglas, Zi-Long Wang et al.
arXiv (Cornell University)
Material Dynamics and Properties
preprint

The End of Chaos at the Ideal Glass Transition

Matteo Baggioli, Wen-Sheng Xu, Jack Douglas, Zi-Long Wang, Zhao-Yan Sun
preprint en

Abstract

The ideal glass transition has often been associated with the extrapolated vanishing of configurational entropy $S_c$, yet how this thermodynamic criterion is reflected in microscopic dynamics remains unclear. Here, we show that the vanishing of deterministic chaos quantified by the maximum Lyapunov exponent $λ_{\mathrm{max}}$ provides such a dynamical signature. Using molecular dynamics simulations across diverse model glass-forming liquids in two and three dimensions, we show that $λ_{\mathrm{max}}$ follows an approximate scaling $λ_{\mathrm{max}} \propto (T-T_λ)^{1/2}$ and extrapolates to zero at a temperature $T_λ$ consistent with the Kauzmann temperature $T_{\mathrm{K}}$. Furthermore, we establish the quantitative relation $λ_{\mathrm{max}}^2 \propto T S_c$, directly linking chaotic dynamics to configurational entropy. By demonstrating that $λ_{\mathrm{max}}^2 \propto σ_K^2$, where $σ_K^2$ is the variance of local potential energy landscape curvature fluctuations, we connect the suppression of chaos directly to landscape geometry. These results provide a unified thermodynamic, dynamical, and geometric framework for glass formation, identifying the ideal glass transition as the endpoint of chaotic exploration of the energy landscape.

arXiv (Cornell University)
Material Dynamics and Properties
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