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The nature of glassy dynamics and the glass transition are long-standing problems under active debate. In the presence of a structural disorder widely believed to be an essential characteristic of structural glass, identifying and understanding key dynamical behaviors are very challenging. In this work, we demonstrate that an energetic disorder, which usually results from a structural disorder, is instead a more essential feature of glass. Specifically, we develop a distinguishable-particle glassy crystal (DPGC) in which particles are ordered in a face-centered cubic lattice and follow particle-dependent random interactions, leading to an energetic disorder in the particle configuration space. Molecular dynamics simulations in the presence of vacancy-induced particle diffusion show typical glassy behaviors. A unique feature of this molecular model is the knowledge of the complete set of inherent structures with easily calculable free energies, implying a well-understood potential energy landscape. Due to its simplicity, the study of the DPGC provides a promising direction to unlock the mysteries of glass.

Chiral active particles (CAPs) are self-propelling particles that break time-reversal symmetry by orbiting or spinning, leading to intriguing behaviors. Here, we examined the dynamics of CAPs moving in 2D lattices of disk obstacles through active Brownian dynamics simulations and granular experiments with grass seeds. We find that the effective diffusivity of the CAPs is sensitive to the structure of the obstacle lattice, a feature absent in achiral active particles. We further studied the transport of CAPs in obstacle arrays under an external field and found a reentrant directional locking effect, which can be used to sort CAPs with different activities. Finally, we demonstrated that the parallelogram lattice of obstacles without mirror symmetry can separate clockwise and counter-clockwise CAPs. The mechanisms of the above three novel phenomena are qualitatively explained. As such, our work provides a basis for designing chirality-based tools for single-cell diagnosis and separation, and active particle-based environmental sensors.

Characterizing the local structural evolution is an essential step in understanding the nature of glass transition. In this work, we probe the evolution of Voronoi cell geometry in simple glass models, and find that the individual particle cages deform anisotropically in supercooled liquid and isotropically in glass. We introduce an anisotropy parameter $k$ for each Voronoi cell, which mean value exhibits a sharp change at the mode-coupling glass transition $\phi_\mathrm{c}$. Moreover, a power law of packing fraction $\phi\propto q_1^{-d}$ is discovered in the liquid regime with $d>D$, in contrast to $d=D$ in the glass regime, where $q_1$ is the first peak position of structure factor, and $D$ is the space dimension. This power law is explained by the change of $k$. The active motions in supercooled liquid are spatially correlated with long axes rather than short axes of Voronoi cells. In addition, the dynamic slowing down approaching the glass transition can be well characterized through a modified free volume model based on $k$. These findings reveal that the nonagnostic structural parameter $k$ determines glassy dynamics and is effective in identifying the structure-dynamics correlations and the glass transition., Comment: 10 pages, 5 figures

Particle dynamics in supercooled liquids are often dominated by string-like motions in which lines of particles perform activated hops cooperatively. The structural features triggering these motions, crucial in understanding glassy dynamics, remain highly controversial. We experimentally study microscopic particle dynamics in colloidal glass formers at high packing fractions. With a small polydispersity leading to glass-crystal coexistence, a void in the form of a vacancy in the crystal can diffuse reversibly into the glass and further induces string-like motions. In the glass, a void takes the form of a quasi-void consisting of a few neighboring free volumes and is transported by the string-like motions it induces. In fully glassy systems with a large polydispersity, similar quasi-void actions are observed. The mobile particles cluster into string-like or compact geometries, but the compact ones can further be broken down into connected sequences of strings, establishing their general importance., Comment: main text 5 pages 4 figures + supplymentary material 24 pages 23 figures (Ancillary files), 2020 Nov accepted by Physical Review Letter

An arxiv paper, ref. [1] by Cao et al., claimed that the tunable attraction reported in our ref. [2] could not be detected. Ref. [1] was submitted to Nature in Apr. 2016 as a Comment on our ref. [2]. Our reply in May 2016 responded to ref. [1] and was reviewed by the editor of Nature and an external referee. Ref. [1] was rejected by Nature in Aug. 2016. We provide our reply, which answers all of the criticisms in ref. [1], in Appendix I. The main text contains a brief reply to the main criticisms., Comment: 11 pages, 13 figures

Vapour deposition can directly produce ultrastable glasses, which are similar to conventional glasses aged over thousands of years. The highly mobile surface layer is believed to accelerate the ageing process of vapour-deposited glasses, but its microscopic kinetics has not been experimentally observed. Here we studied the deposition growth kinetics of a two-dimensional colloidal glass at the single-particle level using video microscopy. We found that newly deposited particles in the surface layer (depth $d<14$ particles) relaxed via frequent out-of-cage motions, while particles in the deeper middle layer ($14

Micrometre sized colloidal particles can be viewed as large atoms with tailorable size, shape and interactions. These building blocks can assemble into extremely rich structures and phases, in which the thermal motions of particles can be directly imaged and tracked using optical microscopy. Hence, colloidal particles are excellent model systems for studying phase transitions, especially for poorly understood kinetic and nonequilibrium microscale processes. Advances in colloid fabrication, assembly and computer simulations have opened up numerous possibilities for such research. In this Review, we describe recent progress in the study of colloidal crystals composed of tunable isotropic spheres, anisotropic particles and active particles. We focus on advances in crystallization, melting and solid solid transitions, and highlight challenges and future perspectives in phase transition studies within colloidal crystals., Comment: 18 pages, 5 figures, 2 boxes, Nature Review Materials, 2015

We observed a two-step glass transition in monolayers of colloidal ellipsoids by video microscopy. The glass transition in the rotational degree of freedom was at a lower density than that in the translational degree of freedom. Between the two transitions, ellipsoids formed an orientational glass. Approaching the respective glass transitions, the rotational and translational fastest-moving particles in the supercooled liquid moved cooperatively and formed clusters with power-law size distributions. The mean cluster sizes diverge in power law as approaching the glass transitions. The clusters of translational and rotational fastest-moving ellipsoids formed mainly within pseudo-nematic domains, and around the domain boundaries, respectively.

We studied the self-diffusion of colloidal ellipsoids in a monolayer near a flat wall by video microscopy. The image processing algorithm can track the positions and orientations of ellipsoids with sub-pixel resolution. The translational and rotational diffusions were measured in both the lab frame and the body frame along the long and short axes. The long-time and short-time diffusion coefficients of translational and rotational motions were measured as functions of the particle concentration. We observed sub-diffusive behavior in the intermediate time regime due to the caging of neighboring particles. Both the beginning and the ending times of the intermediate regime exhibit power-law dependence on concentration. The long-time and short-time diffusion anisotropies change non-monotonically with concentration and reach minima in the semi-dilute regime because the motions along long axes are caged at lower concentrations than the motions along short axes. The effective diffusion coefficients change with time t as a linear function of (lnt)/t for the translational and rotational diffusions at various particle densities. This indicates that their relaxation functions decay according to 1/t which provides new challenges in theory. The effects of coupling between rotational and translational Brownian motions were demonstrated and the two time scales corresponding to anisotropic particle shape and anisotropic neighboring environment were measured.

This paper has been withdrawn by the author due to need for more improvement., Comment: This paper has been withdrawn

Geometric frustration leads to complex phases of matter with exotic properties. Antiferromagnets on triangular lattices and square ice are two simple models of geometrical frustration. We map their highly degenerated ground-state phase spaces as discrete networks such that network analysis tools can be introduced to phase-space studies. The resulting phase spaces establish a novel class of complex networks with Gaussian spectral densities. Although phase-space networks are heterogeneously connected, the systems are still ergodic except under periodic boundary conditions. We elucidate the boundary effects by mapping the two models as stacks of cubes and spheres in higher dimensions. Sphere stacking in various containers, i.e. square ice under various boundary conditions, reveals challenging combinatorial questions. This network approach can be generalized to phase spaces of some other complex systems.

We study colloidal particle dynamics of a model glass system using confocal and fluorescence microscopy as the sample evolves from a hard-sphere glass to a liquid with attractive interparticle interactions. The transition from hard-sphere glass to attractive liquid is induced by short-range depletion forces. The development of liquid-like structure is indicated by particle dynamics. We identify particles which exhibit substantial motional events and characterize the transition using the properties of these motional events. As samples enter the attractive liquid region, particle speed during these motional events increases by about one order of magnitude, and the particles move more cooperatively. Interestingly, colloidal particles in the attractive liquid phase do not exhibit significantly larger displacements than particles in the hard-sphere glass.