Non-Gaussian energy landscape of a simple model for strong network-forming liquids: Accurate evaluation of the configurational entropy

Moreno, Angel J.; Saika‐Voivod, Ivan; Zaccarelli, Emanuela; Nave, E. La; Buldyrev, Sergey V.; Tartaglia, P.; Sciortino, Francesco

doi:10.1063/1.2196879

Cited by 23 publications

(32 citation statements)

References 84 publications

(128 reference statements)

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“…8. First, for the large θ , noncrystallizing model, panels (a) and (b) report the iso-diffusivity line for the smallest value of the diffusion coefficient which it was possible to estimate in lengthy simulations (the computer analog of the glass line 35,38 ). Indeed, the nucleation rate, besides depending on β μ, is also affected by particle mobility and hence there is the possibility that crystallization is further suppressed for kinetic reasons.…”

Section: Resultsmentioning

confidence: 99%

Crystallization of tetrahedral patchy particles in silico

Romano

Sanz

Sciortino

2011

The Journal of Chemical Physics

133

225

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The stability of a crystal with diamond structure for patchy particles with tetrahedral symmetry J. Chem. Phys. 132, 234511 (2010); 10.1063/1.3454907Reuse of AIP Publishing content is subject to the terms: https://publishing.aip.org/authors/rights-and-permissions. • . Evaluating the temperature and density dependence of the chemical potential of the fluid and of the crystal phases, we find that adjusting the patch width affects the fluid and crystal in different ways. As a result of the different scaling, the driving force for spontaneous self-assembly rapidly grows as the fluid is undercooled for small-width patches, while it only grows slowly for large-width patches, in which case crystallization is pre-empted by dynamic arrest into a network glass.

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Section: Resultsmentioning

confidence: 99%

Crystallization of tetrahedral patchy particles in silico

Romano

Sanz

Sciortino

2011

The Journal of Chemical Physics

133

225

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“…16 Of course, the data in Fig. 2 do not rule out the existence, at some yet inaccessible temperature, of a crossover in the behavior of S conf that makes it smoothly vanish at T = 0, 46,47 or remain finite with an equilibrium residual entropy in classical systems, [48][49][50][51][52] or a discontinuous jump due to an unavoidable crystallization, 29,53,54 or a liquid-liquid transition, 22 or a conventional (kinetic) glass transition. 55 These alternative pos-sibilities are not supported by data any better than the entropy crisis they try to avoid.…”

Section: B Why the Configurational Entropy?mentioning

confidence: 92%

Configurational entropy of glass-forming liquids

Berthier

Ozawa

Scalliet

2019

The Journal of Chemical Physics

100

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The configurational entropy is one of the most important thermodynamic quantities characterizing supercooled liquids approaching the glass transition. Despite decades of experimental, theoretical, and computational investigation, a widely accepted definition of the configurational entropy is missing, its quantitative characterization remains fraud with difficulties, misconceptions and paradoxes, and its physical relevance is vividly debated. Motivated by recent computational progress, we offer a pedagogical perspective on the configurational entropy in glass-forming liquids. We first explain why the configurational entropy has become a key quantity to describe glassy materials, from early empirical observations to modern theoretical treatments. We explain why practical measurements necessarily require approximations that make its physical interpretation delicate. We then demonstrate that computer simulations have become an invaluable tool to obtain precise, non-ambiguous, and experimentally-relevant measurements of the configurational entropy. We describe a panel of available computational tools, offering for each method a critical discussion. This perspective should be useful to both experimentalists and theoreticians interested in glassy materials and complex systems. I. CONFIGURATIONAL ENTROPY AND GLASS FORMATION A. The glass transitionWhen a liquid is cooled, it can either form a crystal or avoid crystallization and become a supercooled liquid. In the latter case, the liquid remains structurally disordered, but its relaxation time increases so fast that there exists a temperature, called the glass temperature T g , below which structural relaxation takes such a long time that it becomes impossible to observe. The liquid is then trapped virtually forever in one of many possible structurally disordered states: this is the basic phenomenology of the glass transition. 1-4 Clearly, T g depends on the measurement timescale and shifts to lower temperatures for longer observation times. The experimental glass transition is not a genuine phase transition, as it is not defined independently of the observer.The rich phenomenology characterizing the approach to the glass transition has given rise to a thick literature. It is not our goal to review it, and we refer instead to previous articles. 1-9 There are convincing indications that the dynamic slowing down of supercooled liquids is accompanied by an increasingly collective relaxation dynamics. This is seen directly by the measurement of growing lengthscales for these dynamic heterogeneities, 10-12 or more indirectly by the growth of the apparent activation energy for structural relaxation, as seen in its non-Arrhenius temperature dependence. These observations suggest an interpretation of the experimental glass transition in terms of a generic, collective mechanism possibly controlled by a sharp phase transition. 13 'Solving the glass problem' thus amounts to identifying and obtaining direct experimental signatures about the fundamental nature and the mathematical des...

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“…3(d). These considerations suggest that further analysis of the potential enery landscape properties of the present system and comparison with model landscapes [26,27] could be very valuable.…”

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confidence: 96%

Compressing nearly hard sphere fluids increases glass fragility

Berthier¹,

Witten²

2009

Europhys. Lett.

135

265

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Computational methods in statistical physics and nonlinear dynamics PACS 05.20.Jj -Statistical mechanics of classical fluids PACS 64.70.P--Glass transitions of specific systems Abstract -We use molecular dynamics to investigate the glass transition occurring at large volume fraction, ϕ, and low temperature, T , in assemblies of soft repulsive particles. We find that equilibrium dynamics in the (ϕ, T )-plane obey a form of dynamic scaling in the proximity of a critical point at T =0 and ϕ = ϕ0, which should correspond to the ideal glass transition of hard spheres. This glass point, "point G", is distinct from athermal jamming thresholds. A remarkable consequence of scaling behaviour is that the dynamics at fixed ϕ passes smoothly from that of a strong glass to that of a very fragile glass as ϕ increases beyond ϕ0. Correlations between fragility and various physical properties are explored.

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Non-Gaussian energy landscape of a simple model for strong network-forming liquids: Accurate evaluation of the configurational entropy

Cited by 23 publications

References 84 publications

Crystallization of tetrahedral patchy particles in silico

Crystallization of tetrahedral patchy particles in silico

Configurational entropy of glass-forming liquids

Compressing nearly hard sphere fluids increases glass fragility

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