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

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.Comment: 13 pages, 3 figures. Submitted to Nature Communications on the 17th of March, 201

Deconstructing the glass transition through critical experiments on colloids

The glass transition is the most enduring grand-challenge problem in contemporary condensed matter physics. Here, we review the contribution of colloid experiments to our understanding of this problem. First, we briefly outline the success of colloidal systems in yielding microscopic insights into a wide range of condensed matter phenomena. In the context of the glass transition, we demonstrate their utility in revealing the nature of spatial and temporal dynamical heterogeneity. We then discuss the evidence from colloid experiments in favor of various theories of glass formation that has accumulated over the last two decades. In the next section, we expound on the recent paradigm shift in colloid experiments from an exploratory approach to a critical one aimed at distinguishing between predictions of competing frameworks. We demonstrate how this critical approach is aided by the discovery of novel dynamical crossovers within the range accessible to colloid experiments. We also highlight the impact of alternate routes to glass formation such as random pinning, trajectory space phase transitions and replica coupling on current and future research on the glass transition. We conclude our review by listing some key open challenges in glass physics such as the comparison of growing static lengthscales and the preparation of ultrastable glasses, that can be addressed using colloid experiments.Comment: 137 pages, 45 figure

The pace of evolution across fitness valleys

How fast does a population evolve from one fitness peak to another? We study the dynamics of evolving, asexually reproducing populations in which a certain number of mutations jointly confer a fitness advantage. We consider the time until a population has evolved from one fitness peak to another one with a higher fitness. The order of mutations can either be fixed or random. If the order of mutations is fixed, then the population follows a metaphorical ridge, a single path. If the order of mutations is arbitrary, then there are many ways to evolve to the higher fitness state. We address the time required for fixation in such scenarios and study how it is affected by the order of mutations, the population size, the fitness values and the mutation rate

Distorted wurtzite unit cells: Determination of lattice parameters of non-polar a-plane AlGaN and estimation of solid phase Al content

Unlike c-plane nitrides, ``non-polar" nitrides grown in e.g. the a-plane or m-plane orientation encounter anisotropic in-plane strain due to the anisotropy in the lattice and thermal mismatch with the substrate or buffer layer. Such anisotropic strain results in a distortion of the wurtzite unit cell and creates difficulty in accurate determination of lattice parameters and solid phase group-III content (x_solid) in ternary alloys. In this paper we show that the lattice distortion is orthorhombic, and outline a relatively simple procedure for measurement of lattice parameters of non-polar group III-nitrides epilayers from high resolution x-ray diffraction measurements. We derive an approximate expression for x_solid taking into account the anisotropic strain. We illustrate this using data for a-plane AlGaN, where we measure the lattice parameters and estimate the solid phase Al content, and also show that this method is applicable for m-plane structures as well

Influence of an amorphous wall on the distribution of localized excitations in a colloidal glass-forming liquid

Elucidating the nature of the glass transition has been the holy grail of condensed matter physics and statistical mechanics for several decades. A phenomenological aspect that makes glass formation a conceptually formidable problem is that structural and dynamic correlations in glass-forming liquids are too subtle to be captured at the level of conventional two-point functions. As a consequence, a host of theoretical techniques, such as quenched amorphous configurations of particles, have been devised and employed in simulations and colloid experiments to gain insights into the mechanisms responsible for these elusive correlations. Very often, though, the analysis of spatio-temporal correlations is performed in the context of a single theoretical framework, and critical comparisons of microscopic predictions of competing theories are thereby lacking. Here, we address this issue by analysing the distribution of localized excitations, which are building blocks of relaxation as per the Dynamical Facilitation (DF) theory, in the presence of an amorphous wall, a construct motivated by the Random First-Order Transition theory (RFOT). We observe that spatial profiles of the concentration of excitations exhibit complex features such as non-monotonicity and oscillations. Moreover, the smoothly varying part of the concentration profile yields a length scale $\xi_c$, which we compare with a previously computed length scale $\xi_{dyn}$. Our results suggest a method to assess the role of dynamical facilitation in governing structural relaxation in glass-forming liquids.Comment: 19 pages, 7 figure

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.Comment: 22 pages, 3 main figues, 3 supplementary figures. Submitted to Proceedings of the National Academy of Sciences, USA, on the 15th of July, 201