arXiv subjects

Rajesh Ganapathy

Publications and source records attributed to Rajesh Ganapathy.

23 records · Page 2Linked to original sources

arXiv2014

Direct measurements of growing amorphous order and non-monotonic dynamic correlations in a colloidal glass-former

While the transformation of flowing liquids into rigid glasses is omnipresent, a complete understanding of vitrification remains elusive. Of the numerous approaches aimed at solving the glass transition problem, the Random First-Order Theory (RFOT) is the most prominent. However, the existence of the underlying thermodynamic phase transition envisioned by RFOT remains debatable, since its key microscopic predictions concerning the growth of amorphous order and the nature of dynamic correlations lack experimental verification. Here, by using holographic optical tweezers, we freeze a wall of particles in an equilibrium configuration of a 2D colloidal glass-forming liquid and provide direct evidence for growing amorphous order in the form of a static point-to-set length. Most remarkably, we uncover the non-monotonic dependence of dynamic correlations on area fraction and show that this non-monotonicity follows directly from the change in morphology of cooperatively rearranging regions, as predicted by RFOT. Our findings suggest that the glass transition has a thermodynamic origin.

cond-mat.soft↗

arXiv2014

Dynamical facilitation governs glassy dynamics in suspensions of colloidal ellipsoids

One of the greatest challenges in contemporary condensed matter physics is to ascertain whether the formation of glasses from liquids is fundamentally thermodynamic or dynamic in origin. While the thermodynamic paradigm has dominated theoretical research for decades, the purely kinetic perspective of the dynamical facilitation (DF) theory has attained prominence in recent times. In particular, recent experiments and simulations have highlighted the importance of facilitation using simple model systems composed of spherical particles. However, an overwhelming majority of liquids possess anisotropy in particle shape and interactions and it is therefore imperative to examine facilitation in complex glass-formers. Here, we apply the DF theory to systems with orientational degrees of freedom as well as anisotropic attractive interactions. By analyzing data from experiments on colloidal ellipsoids, we show that facilitation plays a pivotal role in translational as well as orientational relaxation. Further, we demonstrate that the introduction of attractive interactions leads to spatial decoupling of translational and rotational facilitation, which subsequently results in the decoupling of dynamical heterogeneities. Most strikingly, the DF theory can predict the existence of reentrant glass transitions based on the statistics of localized dynamical events, called excitations, whose duration is substantially smaller than the structural relaxation time. Our findings pave the way for systematically testing the DF approach in complex glass-formers and also establish the significance of facilitation in governing structural relaxation in supercooled liquids.

cond-mat.soft↗

arXiv2014

Growing Dynamical Facilitation on Approaching the Random Pinning Colloidal Glass Transition

Despite decades of research, it remains to be established whether the transformation of a liquid into a glass is fundamentally thermodynamic or dynamic in origin. While observations of growing length scales are consistent with thermodynamic perspectives like the Random First-Order Transition theory (RFOT), the purely dynamic approach of the Dynamical Facilitation (DF) theory lacks experimental validation. Further, for glass transitions induced by randomly freezing a subset of particles in the liquid phase, simulations support the predictions of RFOT, whereas the DF theory remains unexplored. Here, using video microscopy and holographic optical tweezers, we show that dynamical facilitation in a colloidal glass-forming liquid unambiguously grows with density as well as the fraction of pinned particles. In addition, we show that heterogeneous dynamics in the form of string-like cooperative motion, which is believed to be consistent with RFOT, emerges naturally within the framework of facilitation. Most importantly, our findings demonstrate that a purely dynamic origin of the glass transition cannot be ruled out.

cond-mat.soft↗

arXiv2014

Direct Evidence for an Absorbing Phase Transition Governing Yielding of a Soft Glass

We present the first direct experimental evidence showing that yielding of a prototypical soft solid - a colloidal glass - is a non-equilibrium 'absorbing' phase transition. By simultaneously quantifying single-particle dynamics and bulk mechanical response, we extracted critical exponents for the order parameter and the relaxation time and found that this transition belongs to the conserved directed percolation universality class. In addition, the observed critical slowing down is accompanied by a growing correlation length associated with the size of regions of high Debye-Waller factor which are precursors to yield events in glasses. Our results show unambiguously that yielding of soft solids falls squarely in the realm of non-equilibrium critical phenomena.

cond-mat.soft↗

arXiv2007

Granger Causality and Cross Recurrence Plots in Rheochaos

Our stress relaxation measurements on wormlike micelles using a Rheo-SALS (rheology + small angle light scattering) apparatus allow simultaneous measurements of the stress and the scattered depolarised intensity. The latter is sensitive to orientational ordering of the micelles. To determine the presence of causal influences between the stress and the depolarised intensity time series, we have used the technique of linear and nonlinear Granger causality. We find there exists a feedback mechanism between the two time series and that the orientational order has a stronger causal effect on the stress than vice versa. We have also studied the phase space dynamics of the stress and the depolarised intensity time series using the recently developed technique of cross recurrence plots (CRPs). The presence of diagonal line structures in the CRPs unambiguously proves that the two time series share similar phase space dynamics.

nlin.CD↗