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Kinetics of the glass transition of fragile soft colloidal suspensions  [PDF]
Debasish Saha,Yogesh M. Joshi,Ranjini Bandyopadhyay
Physics , 2015,
Abstract: Microscopic relaxation timescales are estimated from the autocorrelation functions obtained by dynamic light scattering experiments for Laponite suspensions with different concentrations ($C_{L}$), added salt concentrations ($C_{S}$) and temperatures ($T$). It has been shown in an earlier work [Soft Matter, 10, 3292-3300 (2014)] that the evolutions of relaxation timescales of colloidal glasses can be compared with molecular glass formers by mapping the waiting time ($t_{w}$) of the former with the inverse of thermodynamic temperature ($1/T$) of the latter. In this work, the fragility parameter $D$, which signifies the deviation from Arrhenius behavior, is obtained from fits to the time evolutions of the structural relaxation timescales. For the Laponite suspensions studied in this work, $D$ is seen to be independent of $C_{L}$ and $C_{S}$, but is weakly dependent on $T$. Interestingly, the behavior of $D$ corroborates the behavior of fragility in molecular glass formers with respect to equivalent variables. Furthermore, the stretching exponent $\beta$, which quantifies the width $w$ of the spectrum of structural relaxation timescales is seen to depend on $t_{w}$. A hypothetical Kauzmann time $t_{k}$, analogous to the Kauzmann temperature for molecular glasses, is defined as the timescale at which $w$ diverges. Corresponding to the Vogel temperature defined for molecular glasses, a hypothetical Vogel time $t^{\infty}_{\alpha}$ is also defined as the time at which the structural relaxation time diverges. Interestingly, a correlation is observed between $t_{k}$ and $t^{\infty}_{\alpha}$, which is remarkably similar to that known for fragile molecular glass formers. A coupling model that accounts for the $t_{w}$-dependence of the stretching exponent is used to analyse and explain the observed correlation between $t_{k}$ and $t^{\infty}_{\alpha}$.
Investigation of the dynamical slowing down process in soft glassy colloidal suspensions: comparisons with supercooled liquids  [PDF]
Debasish Saha,Yogesh M. Joshi,Ranjini Bandyopadhyay
Physics , 2013,
Abstract: The primary and secondary relaxation timescales of aging colloidal suspensions of Laponite are estimated from intensity autocorrelation functions obtained in dynamic light scattering (DLS) experiments. The dynamical slowing down of these relaxation processes are compared with observations in fragile supercooled liquids by establishing a one-to-one mapping between the waiting time since filtration of a Laponite suspension and the inverse of the temperature of a supercooled liquid that is rapidly quenched towards its glass transition temperature. New timescales, such as the Vogel time and the Kauzmann time, are extracted to describe the phenomenon of dynamical arrest in Laponite suspensions. In results that are strongly reminiscent of those extracted from supercooled liquids approaching their glass transitions, it is demonstrated that the Vogel time calculated for each Laponite concentration is approximately equal to the Kauzmann time, and that a strong coupling exists between the primary and secondary relaxation processes of aging Laponite suspensions. Furthermore, the experimental data presented here clearly demonstrates the self-similar nature of the aging dynamics of Laponite suspensions within a range of sample concentrations.
Can secondary nucleation exist in ice banding of freezing colloidal suspensions?  [PDF]
Jiaxue You,Jincheng Wang,Lilin Wang,Zhijun Wang,Xiaobing Hu,Junjie Li,Xin Lin
Physics , 2015,
Abstract: The formation mechanism of ice banding in the system of freezing colloidal suspensions, which is of significance in frost heaving, ice-templating porous materials and biological materials, still remains a mystery. Recently, the theory of secondary nucleation and growth of ice has been proposed to explain the emergence of a new ice lens. However, this theory has not been quantitatively examined. Here, we quantitatively measured the initial interfacial undercooling of a new ice lens and the nucleation undercoolings of suspensions. We found that the interfacial undercooling can not satisfy the nucleation undercooling of ice and hence disprove the secondary nucleation mechanism for ice banding.
Shear Thickening in Concentrated Soft Sphere Colloidal Suspensions: A Shear Induced Phase Transition  [PDF]
Joachim Kaldasch,Bernhard Senge,Jozua Laven
Physics , 2013, DOI: 10.1155/2015/153854
Abstract: A model of shear thickening in dense suspensions of Brownian soft sphere colloidal particles is established. It suggests that shear thickening in soft sphere suspensions can be interpreted as a shear induced phase transition. Based on a Landau model of the coagulation transition of stabilized colloidal particles, taking the coupling between order parameter fluctuations and the local strain-field into account, the model suggests the occurrence of clusters of coagulated particles (subcritical bubbles) by applying a continuous shear perturbation.The critical shear stress of shear thickening in soft sphere suspensions is derived while reversible shear thickening and irreversible shear thickening have the same origin. The comparison of the theory with an experimental investigation of electrically stabilized colloidal suspensions confirms the presented approach.
Three-dimensional jamming and flows of soft glassy materials  [PDF]
Guillaume Ovarlez,Quentin Barral,Philippe Coussot
Physics , 2009, DOI: 10.1038/nmat2615
Abstract: Various disordered dense systems such as foams, gels, emulsions and colloidal suspensions, exhibit a jamming transition from a liquid state (they flow) to a solid state below a yield stress. Their structure, thoroughly studied with powerful means of 3D characterization, exhibits some analogy with that of glasses which led to call them soft glassy materials. However, despite its importance for geophysical and industrial applications, their rheological behavior, and its microscopic origin, is still poorly known, in particular because of its nonlinear nature. Here we show from two original experiments that a simple 3D continuum description of the behaviour of soft glassy materials can be built. We first show that when a flow is imposed in some direction there is no yield resistance to a secondary flow: these systems are always unjammed simultaneously in all directions of space. The 3D jamming criterion appears to be the plasticity criterion encountered in most solids. We also find that they behave as simple liquids in the direction orthogonal to that of the main flow; their viscosity is inversely proportional to the main flow shear rate, as a signature of shear-induced structural relaxation, in close similarity with the structural relaxations driven by temperature and density in other glassy systems.
Stress Relaxation in Aging Soft Colloidal Glasses  [PDF]
Ranjini Bandyopadhyay,P. Harsha Mohan,Yogesh M. Joshi
Physics , 2009,
Abstract: We investigate the stress relaxation behavior on the application of step strains to aging aqueous suspensions of the synthetic clay Laponite. The stress exhibits a two-step decay, from which the slow relaxation modes are extracted as functions of the sample ages and applied step strain deformations. Interestingly, the slow time scales that we estimate show a dramatic enhancement with increasing strain amplitudes. We argue that the system ends up exploring the deeper sections of its energy landscape following the application of the step strain.
Aspects of the dynamics of colloidal suspensions: Further results of the mode-coupling theory of structural relaxation  [PDF]
M. Fuchs,M. R. Mayr
Physics , 1999, DOI: 10.1103/PhysRevE.60.5742
Abstract: Results of the idealized mode-coupling theory for the structural relaxation in suspensions of hard-sphere colloidal particles are presented and discussed with regard to recent light scattering experiments. The structural relaxation becomes non-diffusive for long times, contrary to the expectation based on the de Gennes narrowing concept. A semi-quantitative connection of the wave vector dependences of the relaxation times and amplitudes of the final $\alpha$-relaxation explains the approximate scaling observed by Segr{\`e} and Pusey [Phys. Rev. Lett. {\bf 77}, 771 (1996)]. Asymptotic expansions lead to a qualitative understanding of density dependences in generalized Stokes-Einstein relations. This relation is also generalized to non-zero frequencies thereby yielding support for a reasoning by Mason and Weitz [Phys. Rev. Lett {\bf 74}, 1250 (1995)]. The dynamics transient to the structural relaxation is discussed with models incorporating short-time diffusion and hydrodynamic interactions for short times.
Highly cooperative stress relaxation in two-dimensional soft colloidal crystals  [PDF]
B. van der Meer,W. Qi,R. Fokkink,J. van der Gucht,M. Dijkstra,J. Sprakel
Physics , 2013, DOI: 10.1073/pnas.1411215111
Abstract: Stress relaxation in crystalline solids is mediated by the formation and diffusion of defects. While it is well established how externally-generated stresses relax, through the proliferation and motion of dislocations in the lattice, it remains relatively unknown how crystals cope with internal stresses. We investigate, both experimentally and in simulations, how highly localized stresses relax in two-dimensional soft colloidal crystals. When a single particle is actively excited, by means of optical tweezing, a rich variety of highly collective stress relaxation mechanisms results. These manifest in the form of open strings of cooperatively moving particles through the motion of dissociated vacancy-interstitial pairs, and closed loops of mobile particles, which either result from cooperative rotations in transiently generated circular grain boundaries or through the closure of an open string by annihilation of a vacancy-interstitial pair. Surprisingly, we find that the same collective events occur in crystals which are excited by thermal fluctuations alone; a large thermal agitation inside the crystal lattice can trigger the irreversible displacements of hundreds of particles. Our results illustrate how local stresses can induce large scale cooperative dynamics in two-dimensional soft colloidal crystals and shed new light on the stabilisation mechanisms in ultrasoft crystals.
Modeling dependence of creep recovery behavior on relaxation time distribution of ageing colloidal suspensions  [PDF]
Yogesh M. Joshi
Physics , 2009,
Abstract: A scaling model is developed to correlate relaxation time distribution of soft glassy materials to ultimate recovery. We propose that in the limit of creep-recovery time smaller than age, time translational invariance can be applied to ageing soft materials. In such limit, multimode linear viscoelastic model with Spriggs relaxation spectrum predicts enhancement in the ultimate recovery with broadening of the relaxation time distribution. We analyze these results in the context of creep-recovery behavior of aqueous suspension of laponite with varying concentration of salt.
Theory of nonlinear rheology and yielding of dense colloidal suspensions  [PDF]
Matthias Fuchs,Michael E. Cates
Physics , 2002, DOI: 10.1103/PhysRevLett.89.248304
Abstract: A first principles approach to the nonlinear flow of dense suspensions is presented which captures shear thinning of colloidal fluids and dynamical yielding of colloidal glasses. The advection of density fluctuations plays a central role, suppressing the caging of particles and speeding up structural relaxation. A mode coupling approach is developed to explore these effects.
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