Multiple Glass Singularities and Isodynamics in a Core-Softened Model for Glass-Forming Systems

Gnan, Nicoletta; Das, Gayatri; Sperl, Matthias; Sciortino, Francesco; Zaccarelli, Emanuela

doi:10.1103/physrevlett.113.258302

Cited by 23 publications

(15 citation statements)

References 43 publications

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“…Previous works have shown that one can estimate the locus of the glass transition by monitoring the so-called isodiffusivity (iso-D) lines [77][78][79], along which D remains constant. Importantly, it has been shown that the iso-D lines always maintain, for not too large values of the probed D, the same shape as the ultimate line of arrest.…”

Section: Multiparticle Dynamical Responsementioning

confidence: 99%

Microgels at Interfaces Behave as 2D Elastic Particles Featuring Reentrant Dynamics

et al. 2020

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Soft colloids are increasingly used as model systems to address fundamental issues such as crystallization and the glass and jamming transitions. Among the available classes of soft colloids, microgels are emerging as the gold standard. Since their great internal complexity makes their theoretical characterization very hard, microgels are commonly modeled, at least in the small-deformation regime, within the simple framework of linear elasticity theory. Here we show that there exist conditions where its range of validity can be greatly extended, providing strong numerical evidence that microgels adsorbed at an interface follow the two-dimensional Hertzian theory, and hence behave like 2D elastic particles, up to very large deformations, in stark contrast to what found in bulk conditions. We are also able to estimate Young's modulus of the individual particles and, by comparing it with its counterpart in bulk conditions, we demonstrate a significant stiffening of the polymer network at the interface. Finally, by analyzing dynamical properties, we predict multiple reentrant phenomena: By a continuous increase of particle density, microgels first arrest and then refluidify due to the high penetrability of their extended coronas. We observe this anomalous behavior in a range of experimentally accessible conditions for small and loosely cross-linked microgels. The present work thus establishes microgels at interfaces as a new model system for fundamental investigations, paving the way for the experimental synthesis and research on unique highdensity liquidlike states. In addition, these results can guide the development of novel assembly and patterning strategies on surfaces and the design of novel materials with desired interfacial behavior.

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Section: Multiparticle Dynamical Responsementioning

confidence: 99%

Microgels at Interfaces Behave as 2D Elastic Particles Featuring Reentrant Dynamics

et al. 2020

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“…The structural relaxation of dense liquids exceeds microscopic time scales by orders of magnitude upon approaching the glass transition via compression or cooling the system. The origin of the glass transition remains heavily debated [1][2][3][4][5][6][7][8][9][10][11][12][13][14] and still constitutes a challenge for theory, simulation, and laboratory experiments, although many facets of the phenomena associated with the glass transition have been rationalized successfully within the mode-coupling theory of the glass transition [15][16][17][18][19] developed during the last thirty years.…”

Section: Introductionmentioning

confidence: 99%

Nonergodicity parameters of confined hard-sphere glasses

et al. 2017

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Within a recently developed mode-coupling theory for fluids confined to a slit we elaborate numerical results for the long-time limits of suitably generalized intermediate scattering functions. The theory requires as input the density profile perpendicular to the plates, which we obtain from density functional theory within the fundamental-measure framework, as well as symmetry-adapted static structure factors, which can be calculated relying on the inhomogeneous Percus-Yevick closure. Our calculations for the nonergodicity parameters for both the collective as well as for the self motion are in qualitative agreement with our extensive event-driven molecular dynamics simulations for the intermediate scattering functions for slightly polydisperse hard-sphere systems at high packing fraction. We show that the variation of the nonergodicity parameters as a function of the wavenumber correlates with the in-plane static structure factors, while subtle effects become apparent in the structure factors and relaxation times of higher mode indices. A criterion to predict the multiple reentrant from the variation of the in-plane static structure is presented.

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“…Typical of an approach to a glass, the mean square displacement (MSD) averaged over all the passive particles shows a plateauing and cage hopping dynamics, as the density φ is increased (Fig. S1) [30,[39][40][41]. From these graphs we extract the long time diffusivity D ∞ (Supplementary Information Sec.…”

Section: Interplay Between Active Self-propulsion and Viscoelasticitymentioning

confidence: 99%

Active ploughing through a compressible viscoelastic fluid: Unjamming and emergent nonreciprocity

Banerjee,

Mandal,

Banerjee

et al. 2021

Preprint

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We study the dynamics of a dilute suspension of active Brownian particles in a dense compressible viscoelastic fluid, as a function of the magnitude f and orientational decorrelation time τ of the active force, using agent-based simulations and hydrodynamic theory. We first demonstrate a crossover in the transport of the motile particles, from activity dominated to cage-hopping dominated to eventual dynamical arrest, as a function of the density of the medium. In the process, the compressible medium is actively churned up -for low τ , the active particle gets self-trapped in a spherical cavity of its own making, for large τ , the movement of the active particle is accompanied by an anisotropic wake, while for large f , the active particle ploughs through the medium rendering it porous. We derive hydrodynamic equations describing how the motile particles drive the compressible fluid, and show within a linearised approach, that the active particle generates a long range density wake which breaks fore-aft symmetry, consistent with the simulations. The back reaction of the compressible medium leads to (i) dynamical jamming of the active particle, and (ii) a dynamical non-reciprocal attraction between two active particles moving along the same direction, with the trailing particle catching up with the leading one in finite time.

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Multiple Glass Singularities and Isodynamics in a Core-Softened Model for Glass-Forming Systems

Cited by 23 publications

References 43 publications

Microgels at Interfaces Behave as 2D Elastic Particles Featuring Reentrant Dynamics

Microgels at Interfaces Behave as 2D Elastic Particles Featuring Reentrant Dynamics

Nonergodicity parameters of confined hard-sphere glasses

Active ploughing through a compressible viscoelastic fluid: Unjamming and emergent nonreciprocity

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