<i>Colloquium</i>: The glass transition and elastic models of glass-forming liquids

Dyre, Jeppe C.

doi:10.1103/revmodphys.78.953

Cited by 1,175 publications

(1,352 citation statements)

References 182 publications

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“…[8][9][10][11][12][13][14][15][16][17][18] Thus it has been shown that strongly correlating viscous liquids to a good approximation have all eight frequency-dependent thermoviscoelastic response functions [19][20][21] given in terms of just one 22 (i.e., are single-parameter liquids in the sense of having dynamic Prigogine-Defay ratio 19 close to unity 2,20,22 ). Strongly correlating viscous liquids moreover obey density scaling [23][24][25][26][27] to a good approximation, i.e., their dimensionless relaxation timeτ ≡ τρ 1/3 √ k B T /m (where m is the average particle mass) depends on density ρ = N /V and temperature as τ = F(ρ γ /T ).…”

Section: Introductionmentioning

confidence: 99%

Pressure-energy correlations in liquids. V. Isomorphs in generalized Lennard-Jones systems

Schrøder

Gnan

Pedersen

et al. 2011

The Journal of Chemical Physics

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This series of papers is devoted to identifying and explaining the properties of strongly correlating liquids, i.e., liquids with more than 90% correlation between their virial W and potential energy U fluctuations in the N V T ensemble. Paper IV [N. Gnan et al., J. Chem. Phys. 131, 234504 (2009)] showed that strongly correlating liquids have "isomorphs," which are curves in the phase diagram along which structure, dynamics, and some thermodynamic properties are invariant in reduced units. In the present paper, using the fact that reduced-unit radial distribution functions are isomorph invariant, we derive an expression for the shapes of isomorphs in the WU phase diagram of generalized Lennard-Jones systems of one or more types of particles. The isomorph shape depends only on the Lennard-Jones exponents; thus all isomorphs of standard Lennard-Jones systems (with exponents 12 and 6) can be scaled onto a single curve. Two applications are given. One tests the prediction that the solid-liquid coexistence curve follows an isomorph by comparing to recent simulations by Ahmed and Sadus [J. Chem. Phys. 131, 174504 (2009)]. Excellent agreement is found on the liquid side of the coexistence curve, whereas the agreement is less convincing on the solid side. A second application is the derivation of an approximate equation of state for generalized Lennard-Jones systems by combining the isomorph theory with the Rosenfeld-Tarazona expression for the temperature dependence of the potential energy on isochores. It is shown that the new equation of state agrees well with simulations.

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Section: Introductionmentioning

confidence: 99%

Pressure-energy correlations in liquids. V. Isomorphs in generalized Lennard-Jones systems

Schrøder

Gnan

Pedersen

et al. 2011

The Journal of Chemical Physics

Self Cite

116

115

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“…Although these materials are commonly regarded as disordered systems, crucial features of the glass transition, such as the increase in heterogeneity and the larger cooperativity of the liquid dynamics approaching solidification [6][7][8][9] , can be rationalized by the presence of medium-range ordered regions (MRO) in the liquid phase.…”

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confidence: 99%

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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“…However, as long as the glasses are chemically similar and thus have the same average intermolecular distance [55], the proportionality is usually observed. Here, we have found a relatively strong correlation (R 2 = 0.87) between G at room temperature and T g,vis for the aluminosilicate glasses (Fig.…”

Section: Test Of the Shoving Modelmentioning

confidence: 99%

“…As the elastic properties are correlated with the short-and intermediate range order [43], here we consider the phenomenological "shoving model" of Dyre et al [51][52][53][54][55], in which the dynamics of the glass-forming liquid are considered to be controlled by the elasticity through the instantaneous (infinite frequency) shear modulus G ∞ . According to the shoving model, the non-Arrhenius scaling of relaxation time (i.e., the fragility) is …”

Section: Introductionmentioning

confidence: 99%

Elastic interpretation of the glass transition in aluminosilicate liquids

et al. 2012

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One of the remaining puzzles of the glass transition is the origin of a glass-forming liquid's "fragility," which quantifies the departure of its relaxation time from Arrhenius activated kinetics. According to the shoving model proposed by Dyre, fragility is controlled by the instantaneous shear modulus of the liquid, since any flow event requires a local volume increase and the related activation energy is equal to the work done in shoving aside the surrounding atoms. Here, we present an in situ high-temperature Brillouin spectroscopy test of the shoving model near the glass transition of eight aluminosilicate glass-forming systems. We find that the measured viscosity data agree qualitatively with the measured temperature dependence of shear moduli, as predicted by the shoving model. However, the model systematically underpredicts the values of fragility for our aluminosilicate liquids. This suggests that the dynamics of the glass transition are governed by additional factors beyond the evolution of the shear modulus, such as configurational entropy. We have also compared the glass transition temperature T g,vis obtained from viscosity (temperature at 10 12 Pa s) with the onset temperatures of the decrease in elastic moduli (T g,elas ) and increase in the thermal expansion coefficient (T g,CTE ) during heating. While we find an approximate one-toone correlation between T g,vis and T g,CTE , it is clear that the elastic moduli probe a different frequency response of the glass structure since T g,elas is systematically lower than T g,vis .2

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Colloquium: The glass transition and elastic models of glass-forming liquids

Cited by 1,175 publications

References 182 publications

Pressure-energy correlations in liquids. V. Isomorphs in generalized Lennard-Jones systems

Pressure-energy correlations in liquids. V. Isomorphs in generalized Lennard-Jones systems

Supercooled liquids with enhanced orientational order

Elastic interpretation of the glass transition in aluminosilicate liquids

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