Searcharxiv⌕ Search
Home/Archive/arXiv

arXiv · 1106.5978

Resolving the controversy on the glass transition temperature of water?

S. Capaccioli·K. L. Ngai
View original source ↗Read source document ↗Export metadata ↓

Abstract

We consider experimental data on the dynamics of water (1) in glass-forming aqueous mixtures with glass transition temperature Tg approaching the putative Tg=136 K of water from above and below, (2) in confined spaces of nanometer in size and (3) in the bulk at temperatures above the homogeneous nucleation temperature. Altogether, the considered relaxation times from the data range nearly over 15 decades from 10-12 to 103 s. Assisted by the various features in the isothermal spectra and theoretical interpretation, these considerations enable us to conclude that relaxation of un-crystallized water is highly non-cooperative. The exponent Beta_K of its Kohlrausch stretched exponential correlation function is not far from having the value of one, and hence the deviation from exponential time decay is slight. Albeit the temperature dependence of its alpha-relaxation time being non-Arrhenius, the corresponding Tg-scaled temperature dependence has small steepness index m, likely less than 44 at Tg, and hence water is not 'fragile' as a glassformer. The separation in time scale of the alpha- and the beta-relaxations is small at Tg, becomes smaller at higher temperatures, and they merge together shortly above Tg. From all these properties and by inference, water is highly non-cooperative as a glass-former, it has short cooperative length-scale, and possibly minimal configurational entropy and small change of heat capacity at Tg compared with other organic glass-formers. This conclusion is perhaps unsurprising because water is the smallest molecule. Our deductions from the data rule out that the Tg of water is higher than 160 K, and suggest that it is close to the traditional value of 136 K.

Explore related subjects

cond-mat.stat-mechcond-mat.soft

Keep this discovery

BibTeXRIS

S. Capaccioli, K. L. Ngai. 2011-06-29. Resolving the controversy on the glass transition temperature of water?. https://doi.org/10.1063/1.3633242

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

arXiv2026

Universal sampling of spin systems across quenched disorder

Statistical physics extracts macroscopic laws by averaging over the many microscopic degrees of freedom of a system. Disordered systems demand a second and far harder average, one over the quenched randomness itself. The classic analytical routes, the replica and cavity methods, become uncontrolled outside mean-field or tree-like limits, and conventional numerical algorithms like parallel tempering require expensive, independent equilibration for every disorder realization. In this work, we introduce a universal neural variational framework that amortizes inference across the disorder ensemble, eliminating both the need for per-instance Markov chain equilibration and the cost of retraining instance-specific variational ansatzes. Built on an encoder-decoder Transformer architecture, after training once, it produces an explicit approximation to the Boltzmann distribution given previously unseen disorder realizations without further optimization. We validate this framework on 2D Edwards-Anderson models, and apply it to the random-bond Ising model, successfully capturing the Binder cumulant crossings near the Nishimori multicritical point. These results shift the object of variational inference from the single instance to the disorder ensemble, opening a route to frustrated many-body systems where instance-by-instance computation is prohibitive.

cond-mat.stat-mech↗
arXiv2026

Information-Theoretic Characterization of Macroscopic Chaos Emerging from the Chemical Master Equation

Open chemical reaction networks exhibit stochastic concentration dynamics at finite system sizes, whereas their macroscopic limit is governed by deterministic rate equations that can display chaos. In this Letter, we show theoretically that a rate of information loss constructed from two-time mutual information recovers the Kolmogorov-Sinai entropy in the deterministic limit. We verify this result through numerical simulations of a Markov jump process for a three-species system involving seven reactions.

cond-mat.stat-mech↗
arXiv2026

Orientational order on non-orientable domains

We study the statistical properties of passive and active many-body systems with orientational degrees of freedom on non-orientable domains. By rephrasing topological constraints as non-local symmetry relations on an orientable double-cover, we show that non-orientability eliminates global rotational soft modes without acting like an external field. In a passive XY model, this results in topological caging, where orientational fluctuations that exhibit conventional diffusive behavior on a torus saturate on a Klein bottle to a finite value that we compute exactly in the thermodynamic limit. In models of active self-propelled particles with orientational degrees of freedom, topological caging persists despite continuously changing interaction neighborhoods. In an active Ising spin model, non-orientability enforces the coexistence of ordered anti-parallel domains with vanishing global polar order, a state that is absent on orientable domains.

cond-mat.stat-mech↗