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Register a new userAnatomy of cage formation in a 2D glass-forming liquid
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The solidity of glassy materials is believed to be due to the cage formed around each particle by its neighbors, but in reality the details of cage-formation remain elusive [1-4]. This cage starts to be formed at the onset temperature/density at which the normal liquid begins to show the first signs of glassy dynamics. To study cage-formation we use here focused lasers to produce a local perturbation of the structure on the particle level in 2D colloidal suspensions and monitor by means of video microscopy the systems non-linear dynamic response. All observables we probed show a response which is non-monotonic as a function of the packing fraction, peaking at the onset density. Video microscopic images reveal that this maximum response is due to the buildup of domains with cooperative dynamics that become increasingly rigid and start to dominate the particle dynamics. This proof-of-concept from microrheological deformation demonstrates that in this glass-forming liquid cage formation is directly related to the merging of these domains, thus elucidating the first step in glass-formation [1, 5].
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The sluggish and heterogeneous dynamics of glass forming liquids is frequently associated to the transient coexistence of two phases of particles, respectively with an high and low mobility. In the absence of a dynamical order parameter that acquires a transient bimodal shape, these phases are commonly identified empirically, which makes difficult investigating their relation with the structural properties of the system. Here we show that the distribution of single particle diffusivities can be accessed within a Continuous Time Random Walk description of the intermittent motion, and that this distribution acquires a transient bimodal shape in the deeply supercooled regime, thus allowing for a clear identification of the two coexisting phase. In a simple two-dimensional glass forming model, the dynamic phase coexistence is accompanied by a striking structural counterpart: the distribution of the crystalline-like order parameter becomes also bimodal on cooling, with increasing overlap between ordered and immobile particles. This simple structural signature is absent in other models, such as the three-dimesional Kob-Andersen Lennard-Jones mixture, where more sophisticated order parameters might be relevant. In this perspective, the identification of the two dynamical coexisting phases opens the way to deeper investigations of structure-dynamics correlations.
We analyze multiple new issues concerning activated relaxation in glassy hard sphere fluids and molecular and polymer liquids based on the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory. By invoking a high temperature reference state, a near universality of the apparent dynamic localization length scale is predicted for liquids of widely varying fragility, a result that is relevant to recent simulation studies and quasi-elastic neutron scattering measurements. In contrast, in the same format strongly non-universal behavior is found for the activation barrier that controls long time relaxation. Two measures of cooperativity in ECNLE theory are analyzed. A particle-level total displacement associated with the alpha relaxation event is found to be only of order 1-2 particle diameters and weakly increases with cooling. In contrast, an alternative cooperativity length is defined as the spatial scale required to recover the full barrier and bulk alpha time. This length scale grows strongly with cooling due to the emergence in the deeply supercooled regime of collective long range elastic fluctuations required to allow local hopping. It becomes very large as the laboratory Tg is approached, though is relatively modest at degrees of supercooling accessible with molecular dynamics simulation. The alpha time is found to be exponentially related to this cooperativity length over an enormous number of decades of relaxation time that span the lightly to deeply supercooled regimes. Moreover, the effective barrier height increases almost linearly with the growing cooperativity length scale. An alternative calculation of the collective elastic barrier based on a literal continuum mechanics approach is shown to result in very little change of the theoretical results for bulk properties, but leads to a much smaller and less temperature-sensitive cooperativity length scale.
We study numerically the glass formation and depinning transition of a system of two-dimensional cluster-forming monodisperse particles in presence of pinning disorder. The pairwise interaction potential is nonmonotonic, and is motivated by the intervortex forces in type-$1.5$ superconductors. Such systems can form cluster glasses due to the intervortex interactions following a thermal quench, without underlying disorder. We study the effects of vortex pinning in these systems. We find that a small density of pinning centers of moderate depth has limited effect on vortex glass formation, i.e., formation of vortex glasses is dominated by intervortex interactions. At higher densities pinning can significantly affect glass formation. The cluster glass depinning, under a constant driving force, is found to be plastic, with features distinct from non-cluster-forming systems such as clusters merging and breaking. We find that in general vortices with cluster-forming interaction forces can exhibit stronger pinning effects than regular vortices.
A longstanding open problem in condensed matter physics is whether or not a strongly disordered interacting insulator can be mapped to a system of effectively non-interacting localized excitations. We investigate this issue on the insulating side of the 3D metal-insulator transition (MIT) in phosphorus doped silicon using the new technique of terahertz two dimensional coherent spectroscopy. Despite the intrinsically disordered nature of these materials, we observe coherent excitations and strong photon echoes that provide us with a powerful method for the study of their decay processes. We extract the first measurements of energy relaxation ($T_1$) and decoherence ($T_2$) times close to the MIT in this classic system. We observe that (i) both relaxation rates are linear in excitation frequency with a slope close to unity, (ii) the energy relaxation timescale $T_1$ counterintuitively increases with increasing temperature and (iii) the coherence relaxation timescale $T_2$ has little temperature dependence between 5 K and 25 K, but counterintuitively increases as the material is doped towards the MIT. We argue that these features imply that (a) the system behaves as a well isolated electronic system on the timescales of interest, and (b) relaxation is controlled by electron-electron interactions. We discuss the potential relaxation channels that may explain the behavior. Our observations constitute a qualitatively new phenomenology, driven by the interplay of strong disorder and strong electron-electron interactions, which we dub the marginal Fermi glass.
We study the disordered, multi-spiral solutions of two-dimensional homogeneous oscillatory media for parameter values at which the single spiral/vortex solution is fully stable. In the framework of the complex Ginzburg-Landau (CGLE) equation, we show that these states, heretofore believed to be static, actually evolve on ultra-slow timescales. This is achieved via a reduction of the CGLE to the evolution of the sole vortex position and phase coordinates. This true defect-mediated turbulence occurs in two distinct phases, a vortex liquid characterized by normal diffusion of individual spirals, and a slowly relaxing, intermittent, ``vortex glass.
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