Growing correlation length on cooling below the onset of caging in a simulated glass-forming liquid

Lacevic, Naida; Starr, Francis W.; Schrøder, Thomas B.; Novikov, V. N.; Glotzer, Sharon C.

doi:10.1103/physreve.66.030101

Cited by 97 publications

(133 citation statements)

References 45 publications

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“…Indeed we observe the sharpening of the first peak in g(r) (not shown here, see e. g. Ref. [72]) in our system as T decreases, but the peak in P (F ) is absent for T < T 0 . Recall that the jamming transition in granular materials is equivalent to the macroscopic structural arrest of the system.…”

Section: Average Force and Instantaneous Force Distribution Functmentioning

confidence: 74%

Dynamical Heterogeneity and Jamming in Glass-Forming Liquids

Lacevic

Glotzer

2004

J. Phys. Chem. B

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The relationship between spatially heterogeneous dynamics (SHD) and jamming is studied in a glass-forming binary Lennard-Jones system via molecular dynamics simulations. It has been suggested by O'Hern et al. [1] that the probability distribution of interparticle forces P (F ) develops a peak at the glass transition temperature Tg, and that the large force inhomogeneities, responsible for structural arrest in granular materials, are related to dynamical heterogeneities in supercooled liquids that form glasses. It has been further suggested that "force chains" present in granular materials may exist in supercooled liquids, and may provide an order parameter for the glass transition. Our goal is to investigate the extent to which the forces experienced by particles in a glass-forming liquid are related to SHD, and compare these forces to those observed in granular materials and other glass-forming systems. Our results are summarized as follows. We find no peak in P (F ) at any temperature in our system, even below Tg. We also find that particles that have been localized for a long time are less likely to experience high relative force and that mobile particles experience higher relative forces at shorter time scales, indicating a correlation between pairwise forces and particle mobility. We construct force chains based on the magnitude of pairwise forces. We find that force chains constructed in this manner are composed of both localized and mobile particles, therefore there is no one-to-one correspondence between force chains as defined here and locally mobile or immobile regions of the liquid. We also find that force chains do not play the same role as force chains in granular materials, but may indicate a difference in the evolution of the local environment of particles with different mobility. We also discuss a possible relationship between force chains found here and the development of string-like motion found in other glass-forming liquids [2,3].

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Section: Average Force and Instantaneous Force Distribution Functmentioning

confidence: 74%

Dynamical Heterogeneity and Jamming in Glass-Forming Liquids

Lacevic

Glotzer

2004

J. Phys. Chem. B

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“…6. We should emphasize that unlike in some other studies [38][39][40] we do not use this four-point function for a quantitative examination of the slow particles correlations. For the latter task we found it more convenient to analyze the wave-vector dependent analog of G 4 (r; t).…”

Section: Dynamic Susceptibility and Correlation Lengthmentioning

confidence: 99%

Analysis of a growing dynamic length scale in a glass-forming binary hard-sphere mixture

2011

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We examine a length scale that characterizes the spatial extent of heterogeneous dynamics in a glass-forming binary hard-sphere mixture up to the mode-coupling volume fraction φc. First, we characterize the system's dynamics. Then, we utilize a new method [Phys. Rev. Lett. 105, 217801 (2010)] to extract and analyze the ensemble independent dynamic susceptibility χ4(t) and the dynamic correlation length ξ(t) for a range of times between the β and α relaxation times. We find that in this time range the dynamic correlation length follows a volume fraction independent curve ξ(t) ∼ ln(t). For longer times, ξ(t) departs from this curve and remains constant up to the largest time at which we can determine the length accurately. In addition to the previously established correlation τα ∼ exp[ξ(τα)] between the α relaxation time, τα, and the dynamic correlation length at this time, ξ(τα), we also find a similar correlation for the diffusion coefficient D ∼ exp[ξ(τα) θ ] with θ ≈ 0.6. We discuss the relevance of these findings for different theories of the glass transition.

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“…[15][16][17][18][19][20][21][22][23][24][25][26][27][28][29][30][31] This type of dynamics is commonly referred to as spatially heterogeneous dynamics. [32][33][34][35][36] Numerous computer simulations [39][40][41][42][43][44][45][46] and experimental works 47 have clearly identified transient correlated regions of enhanced mobility. These regions form well-defined clusters, that can typically be decomposed further into groups of particles or molecules that follow each other in a stringlike fashion.…”

Section: Introductionmentioning

confidence: 99%

Spatially Heterogeneous Dynamics and the Adam−Gibbs Relation in the Dzugutov Liquid

et al. 2005

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We perform molecular dynamics simulations of a one-component glass-forming liquid and use the inherent structure formalism to test the predictions of the Adam-Gibbs (AG) theory and to explore the possible connection between these predictions and spatially heterogeneous dynamics. We calculate the temperature dependence of the average potential energy of the equilibrium liquid and show that it obeys the RosenfeldTarazona T 3/5 law for low temperature T, while the average inherent structure energy is found to be inversely proportional to temperature at low T, consistent with a Gaussian distribution of potential energy minima. We investigate the shape of the basins around the local minima in configuration space via the average basin vibrational frequency and show that the basins become slightly broader upon cooling. We evaluate the configurational entropy S conf , a measure of the multiplicity of potential energy minima sampled by the system, and test the validity of the AG relation between S conf and the bulk dynamics. We quantify the dynamically heterogeneous motion by analyzing the motion of particles that are mobile on short and intermediate time scales relative to the characteristic bulk relaxation time. These mobile particles move in one-dimensional "strings", and these strings form clusters with a well-defined average cluster size. The AG approach predicts that the minimum size of cooperatively rearranging regions (CRR) of molecules is inversely proportional to S conf , and recently (Phys. Rev. Lett. 2003, 90, 085506) it has been shown that the mobile-particle clusters are consistent with the CRR envisaged by Adam and Gibbs. We test the possibility that the mobile-particle strings, rather than clusters, may describe the CRR of the Adam-Gibbs approach. We find that the strings also follow a nearly inverse relation with S conf . We further show that the logarithm of the time when the strings and clusters are maximum, which occurs in the late--relaxation regime of the intermediate scattering function, follows a linear relationship with 1/TS conf , in agreement with the AG prediction for the relationship between the configurational entropy and the characteristic time for the liquid to undergo a transition to a new configuration. Since strings are the basic elements of the clusters, we propose that strings are a more appropriate measure of the minimum size of a CRR that leads to configurational transitions. That the cluster size also has an inverse relationship with S conf may be a consequence of the fact that the clusters are composed of strings.

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Growing correlation length on cooling below the onset of caging in a simulated glass-forming liquid

Cited by 97 publications

References 45 publications

Dynamical Heterogeneity and Jamming in Glass-Forming Liquids

Dynamical Heterogeneity and Jamming in Glass-Forming Liquids

Analysis of a growing dynamic length scale in a glass-forming binary hard-sphere mixture

Spatially Heterogeneous Dynamics and the Adam−Gibbs Relation in the Dzugutov Liquid

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