Dynamical heterogeneity in aging colloidal glasses of Laponite

Soft Matter (Impact Factor: 4.03). 01/2012; 8:5507. DOI: 10.1039/c2sm25171j
Source: arXiv


Glasses behave as solids due to their long relaxation time; however the
origin of this slow response remains a puzzle. Growing dynamic length scales
due to cooperative motion of particles are believed to be central to the
understanding of both the slow dynamics and the emergence of rigidity. Here, we
provide experimental evidence of a growing dynamical heterogeneity length scale
that increases with increasing waiting time in an aging colloidal glass of
Laponite. The signature of heterogeneity in the dynamics follows from dynamic
light scattering measurements in which we study both the rotational and
translational diffusion of the disk-shaped particles of Laponite in suspension.
These measurements are accompanied by simultaneous microrheology and
macroscopic rheology experiments. We find that rotational diffusion of
particles slows down at a faster rate than their translational motion. Such
decoupling of translational and orientational degrees of freedom finds its
origin in the dynamic heterogeneity since rotation and translation probe
different length scales in the sample. The macroscopic rheology experiments
show that the low frequency shear viscosity increases at a much faster rate
than both rotational and translational diffusive relaxation times.

  • Source
    • "Due to the non-equilibrium nature of these arrested states, they exhibit aging, with the dynamical and thermodynamical properties of these suspensions evolving as the waiting time (measured after the time of preparation) increases. Aging in these systems occurs by the spatially and temporally correlated local rearrangements of particles that can overcome local energy barriers, with the system exploring progressively deeper energy wells in phase space [3]. The different arrested phases exhibit viscoelastic properties under different applied stress-strain conditions. "
    [Show abstract] [Hide abstract]
    ABSTRACT: The dispersion processes of aqueous samples of clay are studied using ultrasound attenuation spectroscopy. The attenuation spectra that are acquired in the frequency range 10-100 MHz are used to determine the particle size distributions (PSDs) for different concentrations and ages of the clay suspensions. Our analysis, using equivalent spherical diameter (ESD) for circular discs under Stokes drag in samples of concentrations greater than 1.5% w/v, shows that a substantial fraction of the aggregates in suspension are actually tactoids that are composed of more than one platelet. This is in contrast to the general belief that clay disperses into individual platelets in the concentration range where their suspensions exhibit glassy behavior. We conclude that the incomplete fragmentation of the clay tactoids arises from the rapid enhancement of the intertactoid Coulombic repulsion.
    Full-text · Article · Oct 2013 · Langmuir
  • [Show abstract] [Hide abstract]
    ABSTRACT: The stiction properties of a star polyisoprene (PIP) melt (having 22 arms and an arm molecular weight of around 5000, M(w) ≈ 110 000) confined between mica surfaces were investigated using the surface forces apparatus. Stop-start experiments were carried out and the stiction spike was measured as a function of surface stopping (aging) time t and applied pressure P; the time constants of the phase transitions in the stiction dynamics (freezing on stopping and melting on starting) were obtained from the force relaxation behaviors. The results were compared with those of a confined linear-PIP melt (M(w) ≈ 48 000) and other confined fluid systems; the effect of star architecture on the phase transitions in confinement during aging is discussed. Estimation of the molecular size gives that the confined star-PIP films consist of three molecular layers; a non-adsorbed layer sandwiched between two layers adsorbed on opposed mica surfaces. There are (at least) four time constants in the freezing transition of the confined star-PIP melt; fast (τ(1)) and slow (τ(2)) time constants for lateral force relaxation on stopping, critical aging time for freezing (τ(f)), and the logarithmic increase of the spike height against t. The three time constants on stopping, τ(1), τ(2), and τ(f), increase with the increase of P (decrease of the thickness D). As regards the melting transition on starting, spike force decay was fitted by a single exponential function and one time constant was obtained, which is insensitive to P (D). Comparison of the time constants between freezing and melting, and also with the results of linear-PIP reveals that the stiction dynamics of the star-PIP system involves the relaxation and rearrangement of segmental-level and whole molecular motions. Lateral force relaxation on stopping is governed by the individual and cooperative rearrangements of local PIP segments and chain ends of the star, which do not directly lead to the freezing of the system. Instead, geometrical rearrangements of the soft star-PIP spheres into dense packing between surfaces (analogous to the concept of a colloidal glass transition) are the major mechanism of the freezing transition (stiction) after aging. Interdigitation of PIP segments∕chain ends between neighboring star molecules also contributes to the spike growth along with aging, and the melting transition on starting.
    No preview · Article · Nov 2012 · The Journal of Chemical Physics
  • [Show abstract] [Hide abstract]
    ABSTRACT: Polyamorphism and dynamical heterogeneities in network-forming liquids (SiO2, GeO2, Al2O3) at 3200 K and in a wide pressure range are investigated by molecular dynamics simulation. Results show that their structure comprises three structural phases: TO4-, TO5-, and TO6-phases (T = Si, Ge, or Al). The size of structural phase regions significantly depends on compression. Besides, the mobility of atoms in different structural phases is different. For SiO2 and GeO2 systems, the TO5-phase forms mobile regions. For Al2O3 system, AlO6-phase forms mobile regions. The coexistence of TOx-phases (x = 4, 5, 6) in the network-forming liquids is origin of the spatially dynamical heterogeneity.
    No preview · Article · May 2013 · Applied Physics Letters
Show more