In search of a theory of supercooled liquids

Kivelson, Steven; Tarjus, Gilles

doi:10.1038/nmat2304

Cited by 126 publications

(152 citation statements)

References 22 publications

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“…5), 22 SNGN shows clear deviations. 20 6,51 This proportionality is demonstrated in Fig. 5 by the reasonable agreement of the H(T) and scaled N corr (T) curves (lines and symbols, respectively) shown for the structural glass formers investigated in Ref.…”

Section: Sn-40gnsupporting

confidence: 62%

Nonlinear dielectric spectroscopy in a fragile plastic crystal

Michl

Bauer

Lunkenheimer

et al. 2016

The Journal of Chemical Physics

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In this work we provide a thorough examination of the nonlinear dielectric properties of a succinonitrileglutaronitrile mixture, representing one of the rare example of a plastic crystal with fragile glassy dynamics. The detected alteration of the complex dielectric permittivity under high fields can be explained considering the heterogeneous nature of glassy dynamics and a field-induced variation of entropy. While the first mechanism was also found in structural glass formers, the latter effect seems to be typical for plastic crystals. Morover, the third harmonic component of the dielectric susceptibility is reported, revealing a spectral shape as predicted for cooperative molecular dynamics. In accord with the fragile nature of the glass transition in this plastic crystal, we deduce a relatively strong temperature dependence of the number of correlated molecules, in contrast to the much weaker temperature dependence in plasticcrystalline cyclo-octanol, whose glass transition is of strong nature.

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Section: Sn-40gnsupporting

confidence: 62%

Nonlinear dielectric spectroscopy in a fragile plastic crystal

Michl

Bauer

Lunkenheimer

et al. 2016

The Journal of Chemical Physics

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“…The following discussion is a simplification for a didactic purpose of a very complicated and still controversial issue. The mechanism involved in convex curvature of Arrhenius plots in supercooled liquids is one of the less understood unsolved processes in condensed matter science [58,69,70]. An interesting example is the diffusion of krypton in methanol and ethanol mixtures at low temperature near their glass transition temperatures [71][72][73] liquids with different composition exhibit variations of the temperature-dependent viscosity [75].…”

Section: (A) Super-arrheniusmentioning

confidence: 99%

Kinetics of low-temperature transitions and a reaction rate theory from non-equilibrium distributions

Aquilanti

Coutinho

Carvalho-Silva

2017

Phil. Trans. R. Soc. A.

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relaxing the thermodynamic equilibrium limit, either for a binomial distribution if d > 0 or for a negative binomial distribution if d < 0, formally corresponding to Fermionlike or Boson-like statistics, respectively. The current status of the phenomenology is illustrated emphasizing case studies; specifically (i) the super-Arrhenius kinetics, where transport phenomena accelerate processes as the temperature increases; (ii) the sub-Arrhenius kinetics, where quantum mechanical tunnelling propitiates low-temperature reactivity; (iii) the anti-Arrhenius kinetics, where processes with no energetic obstacles are rate-limited by molecular reorientation requirements. Particular attention is given for case (i) to the treatment of diffusion and viscosity, for case (ii) to formulation of a transition rate theory for chemical kinetics including quantum mechanical tunnelling, and for case (iii) to the stereodirectional specificity of the dynamics of reactions strongly hindered by the increase of temperature.This article is part of the themed issue 'Theoretical and computational studies of nonequilibrium and non-statistical dynamics in the gas phase, in the condensed phase and at interfaces'.

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“…It is an obvious, but controversially debated approach to trace these deviations back to a temperature-dependent apparent activation energy, strongly increasing towards low temperatures (Fig. 2(b) with inset) [1,3,4,5,47,48]. Such a behaviour may arise from an increase in cooperativity of molecular motions when the glass transition is approached [1,3,49,50].…”

Section: Glassy Dynamics As Revealed By Linear Dielectric Spectroscopymentioning

confidence: 99%

Investigation of nonlinear effects in glassy matter using dielectric methods

Lunkenheimer

Michl

Bauer

et al. 2017

Eur. Phys. J. Spec. Top.

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Abstract. We summarize current developments in the investigation of glassy matter using nonlinear dielectric spectroscopy. This work also provides a brief introduction into the phenomenology of the linear dielectric response of glassforming materials and discusses the main mechanisms that can give rise to nonlinear dielectric response in this material class. Here we mainly concentrate on measurements of the conventional dielectric permittivity at high fields and the higher-order susceptibilities characterizing the 3 and 5 components of the dielectric response as performed in our group. Typical results on canonical glass-forming liquids and orientationally disordered plastic crystals are discussed, also treating the special case of supercooled monohydroxy alcohols.

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In search of a theory of supercooled liquids

Cited by 126 publications

References 22 publications

Nonlinear dielectric spectroscopy in a fragile plastic crystal

Nonlinear dielectric spectroscopy in a fragile plastic crystal

Kinetics of low-temperature transitions and a reaction rate theory from non-equilibrium distributions

Investigation of nonlinear effects in glassy matter using dielectric methods

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