Nonequilibrium static growing length scales in supercooled liquids on approaching the glass transition

The small wavenumber $k$ behavior of the structure factor $S(k)$ of overcompressed amorphous hard-sphere configurations was previously studied for a wide range of densities up to the maximally random jammed state, which can be viewed as a prototypical glassy state [A. Hopkins, F. H. Stillinger and S. Torquato, Phys. Rev. E, 86, 021505 (2012)]. It was found that a precursor to the glassy jammed state was evident long before the jamming density was reached as measured by a growing nonequilibrium length scale extracted from the volume integral of the direct correlation function $c(r)$, which becomes long-ranged as the critical jammed state is reached. The present study extends that work by investigating via computer simulations two different atomic models: the single-component Z2 Dzugutov potential in three dimensions and the binary-mixture Kob-Andersen potential in two dimensions. Consistent with the aforementioned hard-sphere study, we demonstrate that for both models a signature of the glass transition is apparent well before the transition temperature is reached as measured by the length scale determined from from the volume integral of the direct correlation function in the single-component case and a generalized direct correlation function in the binary-mixture case. The latter quantity is obtained from a generalized Orstein-Zernike integral equation for a certain decoration of the atomic point configuration. We also show that these growing length scales, which are a consequence of the long-range nature of the direct correlation functions, are intrinsically nonequilibrium in nature as determined by an index $X$ that is a measure of deviation from thermal equilibrium. It is also demonstrated that this nonequilibrium index, which increases upon supercooling, is correlated with a characteristic relaxation time scale.Comment: 26 pages, 14 figure

Toward the Jamming Threshold of Sphere Packings: Tunneled Crystals

We have discovered a new family of three-dimensional crystal sphere packings that are strictly jammed (i.e., mechanically stable) and yet possess an anomalously low density. This family constitutes an uncountably infinite number of crystal packings that are subpackings of the densest crystal packings and are characterized by a high concentration of self-avoiding "tunnels" (chains of vacancies) that permeate the structures. The fundamental geometric characteristics of these tunneled crystals command interest in their own right and are described here in some detail. These include the lattice vectors (that specify the packing configurations), coordination structure, Voronoi cells, and density fluctuations. The tunneled crystals are not only candidate structures for achieving the jamming threshold (lowest-density rigid packing), but may have substantially broader significance for condensed matter physics and materials science.Comment: 19 pages, 5 figure

Basic Understanding of Condensed Phases of Matter via Packing Models

Packing problems have been a source of fascination for millenia and their study has produced a rich literature that spans numerous disciplines. Investigations of hard-particle packing models have provided basic insights into the structure and bulk properties of condensed phases of matter, including low-temperature states (e.g., molecular and colloidal liquids, crystals and glasses), multiphase heterogeneous media, granular media, and biological systems. The densest packings are of great interest in pure mathematics, including discrete geometry and number theory. This perspective reviews pertinent theoretical and computational literature concerning the equilibrium, metastable and nonequilibrium packings of hard-particle packings in various Euclidean space dimensions. In the case of jammed packings, emphasis will be placed on the "geometric-structure" approach, which provides a powerful and unified means to quantitatively characterize individual packings via jamming categories and "order" maps. It incorporates extremal jammed states, including the densest packings, maximally random jammed states, and lowest-density jammed structures. Packings of identical spheres, spheres with a size distribution, and nonspherical particles are also surveyed. We close this review by identifying challenges and open questions for future research.Comment: 33 pages, 20 figures, Invited "Perspective" submitted to the Journal of Chemical Physics. arXiv admin note: text overlap with arXiv:1008.298

Irreversibility and Chaos in Active Particle Suspensions

Active matter has been the object of huge amount of research in recent years for its important fundamental and applicative properties. In this paper we investigate active suspensions of micro-swimmers through direct numerical simulation, so that no approximation is made at the continuous level other than the numerical one. We consider both pusher and puller organisms, with a spherical or ellipsoidal shape. We analyse the velocity and the characteristic scales for an homogeneous two-dimensional suspension and the effective viscosity under shear. We bring evidences that the complex features displayed are related to a spontaneous breaking of the time-reversal symmetry. We show that chaos is not a key ingredient, whereas a large enough number of interacting particles and a non-spherical shape are needed to break the symmetry and are therefore at the basis of the phenomenology. Our numerical study also shows that pullers display some collective motion, though with different characteristics from pushers

Hyperuniformity Order Metric of Barlow Packings

The concept of hyperuniformity has been a useful tool in the study of large-scale density fluctuations in systems ranging across the natural and mathematical sciences. One can rank a large class of hyperuniform systems by their ability to suppress long-range density fluctuations through the use of a hyperuniformity order metric $\bar{\Lambda}$. We apply this order metric to the Barlow packings, which are the infinitely degenerate densest packings of identical rigid spheres that are distinguished by their stacking geometries and include the commonly known fcc lattice and hcp crystal. The "stealthy stacking" theorem implies that these packings are all stealthy hyperuniform, a strong type of hyperuniformity which involves the suppression of scattering up to a wavevector $K$. We describe the geometry of three classes of Barlow packings, two disordered classes and small-period packings. In addition, we compute a lower bound on $K$ for all Barlow packings. We compute $\bar{\Lambda}$ for the aforementioned three classes of Barlow packings and find that to a very good approximation, it is linear in the fraction of fcc-like clusters, taking values between those of least-ordered hcp and most-ordered fcc. This implies that the $\bar{\Lambda}$ of all Barlow packings is primarily controlled by the local cluster geometry. These results indicate the special nature of anisotropic stacking disorder, which provides impetus for future research on the development of anisotropic order metrics and hyperuniformity properties.Comment: 13 pages, 7 figure

Spatial modeling of the 3D morphology of hybrid polymer-ZnO solar cells, based on electron tomography data

A spatial stochastic model is developed which describes the 3D nanomorphology of composite materials, being blends of two different (organic and inorganic) solid phases. Such materials are used, for example, in photoactive layers of hybrid polymer zinc oxide solar cells. The model is based on ideas from stochastic geometry and spatial statistics. Its parameters are fitted to image data gained by electron tomography (ET), where adaptive thresholding and stochastic segmentation have been used to represent morphological features of the considered ET data by unions of overlapping spheres. Their midpoints are modeled by a stack of 2D point processes with a suitably chosen correlation structure, whereas a moving-average procedure is used to add the radii of spheres. The model is validated by comparing physically relevant characteristics of real and simulated data, like the efficiency of exciton quenching, which is important for the generation of charges and their transport toward the electrodes.Comment: Published in at http://dx.doi.org/10.1214/11-AOAS468 the Annals of Applied Statistics (http://www.imstat.org/aoas/) by the Institute of Mathematical Statistics (http://www.imstat.org

Equilibrium Phase Behavior and Maximally Random Jammed State of Truncated Tetrahedra

Systems of hard nonspherical particles exhibit a variety of stable phases with different degrees of translational and orientational order, including isotropic liquid, solid crystal, rotator and a variety of liquid crystal phases. In this paper, we employ a Monte Carlo implementation of the adaptive-shrinking-cell (ASC) numerical scheme and free-energy calculations to ascertain with high precision the equilibrium phase behavior of systems of congruent Archimedean truncated tetrahedra over the entire range of possible densities up to the maximal nearly space-filling density. In particular, we find that the system undergoes two first-order phase transitions as the density increases: first a liquid-solid transition and then a solid-solid transition. The isotropic liquid phase coexists with the Conway-Torquato (CT) crystal phase at intermediate densities. At higher densities, we find that the CT phase undergoes another first-order phase transition to one associated with the densest-known crystal. We find no evidence for stable rotator (or plastic) or nematic phases. We also generate the maximally random jammed (MRJ) packings of truncated tetrahedra, which may be regarded to be the glassy end state of a rapid compression of the liquid. We find that such MRJ packings are hyperuniform with an average packing fraction of 0.770, which is considerably larger than the corresponding value for identical spheres (about 0.64). We conclude with some simple observations concerning what types of phase transitions might be expected in general hard-particle systems based on the particle shape and which would be good glass formers