A thermodynamic theory of supercooled liquids

Kivelson, Daniel; Kivelson, Steven; Zhao, Xiaolin; Nussinov, Zohar; Tarjus, Gilles

doi:10.1016/0378-4371(95)00140-3

Cited by 424 publications

(469 citation statements)

References 38 publications

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“…Such a trend is in further agreement with the idea that the more fragile glass formers (m xylitol 4m threitol 4m glycerol , (ref. 32) with m the fragility) are characterized by lower frustration, that is, by a lower concentration of (locally) ordered structures 11,28 , which explains the smaller increase in polarization with increasing molecular size. Lifetime and length scale of the enhancement in polarization.…”

Section: Resultsmentioning

confidence: 99%

“…The MRO enrichment should persist as long as the LPSs have not recovered their equilibrium concentration at a given temperature. Until the achievement of this condition, the MRO regions continuously destroy and nucleate, driven by the minimization of local free energy, achieved via spatial reorganization at the time scale of t (refs 11,28). This long-lasting behaviour permitted us to detect the differences in the orientational polarization.…”

Section: Discussionmentioning

confidence: 97%

“…This long-lasting behaviour permitted us to detect the differences in the orientational polarization. At present, no simulation methods are available to compute the distribution and the exact lifetime of these metastable structures, even using state-of-the-art computer resources 11 . However, recent Monte Carlo simulations have verified that metastable states associated with lower inherent structure energy (that is, LPSs) can survive for lifetimes longer than the lifetimes predicted by simple diffusion models and can thus coexist with the isotropic liquid 38 .…”

Section: Discussionmentioning

confidence: 99%

“…Frustration models [10][11][12] , developed in the past few decades, ascribe this behaviour to the presence of icosahedra, locally preferred structures (LPSs) present in the isotropic liquid at temperatures below the melting point, T m . The formation of these solid-like clusters is driven by maximizing the number of directional bonds that lock the system to local minima in the free-energy landscape.…”

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confidence: 99%

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Supercooled liquids with enhanced orientational order

2012

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The nature of the glass transition, the transformation of a liquid into a disordered solid, still remains one of the most intriguing unsolved problems in materials science. Recent models rationalize crucial features of vitrification with the presence of medium-range ordered regions coexisting with the isotropic liquid. Here, in line with this prediction, we report an extraordinary enhancement in bond orientational order in ultrathin films of supercooled polyols, grown by physical vapour deposition. By varying the deposition conditions and the molecular size, we could tune the kinetic stability of the liquid phase enriched in bond orientational order towards conversion into the ordinary liquid phase. We observed a strong increase in the dielectric strength with respect to the ordinary supercooled liquid and slower structural dynamics, suggesting the existence of a metastable liquid phase with improved orientational correlations.

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Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 97%

Section: Discussionmentioning

confidence: 99%

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confidence: 99%

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Supercooled liquids with enhanced orientational order

2012

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“…Our results, together with some other recent studies [38,44,45,48,53,60,62,63,64,68], suggest that several essential features of the dynamics of supercooled liquids need to be recognized and we now list some of them.…”

Section: Discussionmentioning

confidence: 96%

Real space origin of temperature crossovers in supercooled liquids

2003

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We show that the various crossovers between dynamical regimes observed in experiments and simulations of supercooled liquids can be explained in simple terms from the existence and statistical properties of dynamical heterogeneities. We confirm that dynamic heterogeneity is responsible for the slowing down of glass formers at temperatures well above the dynamic singularity Tc predicted by mode coupling theory. Our results imply that activated processes govern the long-time dynamics even in the temperature regime where they are neglected by mode-coupling theory. We show that alternative interpretations based on topographic properties of the potential energy landscape are complicated and inefficient ways of describing simple physical features which are naturally accounted for within our approach. We show in particular that the reported links between mode coupling and landscape singularities do not exist.

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