arXiv subjects

Mark J. Bowick

Publications and source records attributed to Mark J. Bowick.

At least 55 records · Page 3Linked to original sources

arXiv2013

Fractionalization of Interstitials in Curved Colloidal Crystals

Understanding the out-of equilibrium behaviour of point defects in crystals, yields insights into the nature and fragility of the ordered state, as well as being of great practical importance. In some rare cases defects are spontaneously healed - a one-dimensional crystal formed by a line of identical charged particles, for example, can accommodate an interstitial (extra particle) by a re-adjusting all particle positions to even out the spacing. In sharp contrast, particles organized into a perfect hexagonal crystal in the plane cannot accommodate an interstitial by a simple re-adjustment of the particle spacing - the interstitial remains instead trapped between lattice sites and diffuses by hopping, leaving the crystal permanently defected. Here we report on the behavior of interstitials in colloidal crystals on curved surfaces. Using optical tweezers operated independently of three dimensional imaging, we insert a colloidal interstitial in a lattice of similar particles on flat and curved (positively and negatively) oil-glycerol interfaces and image the ensuing dynamics. We find that, unlike in flat space, the curved crystals self-heal through a collective rearrangement that re-distributes the increased density associated with the interstitial. The self-healing process can be interpreted in terms of an out of equilibrium interaction of topological defects with each other and with the underlying curvature. Our observations suggest the existence of "particle fractionalization" on curved surface crystals.

cond-mat.soft↗

arXiv2013

Crystalline Particle Packings on Constant Mean Curvature (Delaunay) Surfaces

We investigate the structure of crystalline particle arrays on constant mean curvature (CMC) surfaces of revolution. Such curved crystals have been realized physically by creating charge-stabilized colloidal arrays on liquid capillary bridges. CMC surfaces of revolution, classified by Charles Delaunay in 1841, include the 2-sphere, the cylinder, the vanishing mean curvature catenoid (a minimal surface) and the richer and less investigated unduloid and nodoid. We determine numerically candidate ground state configurations for 1000 point-like particles interacting with a pairwise-repulsive dipole-dipole interaction potential. We mimic stretching of capillary bridges by determining the equilibrium configurations of particles arrayed on a sequence of Delaunay surfaces obtained by increasing or decreasing the height at constant volume starting from a given initial surface, either a fat cylinder or a square cylinder. In this case the stretching process takes one through a complicated sequence of Delaunay surfaces each with different geometrical parameters including the aspect ratio, mean curvature and maximal Gaussian curvature. Unduloids, catenoids and nodoids all appear in this process. Defect motifs in the ground state evolve from dislocations at the boundary to dislocations in the interior to pleats and scars in the interior and then isolated 7-fold disclinations in the interior as the capillary bridge narrows at the waist (equator) and the maximal (negative) Gaussian curvature grows. We also check theoretical predictions that the isolated disclinations are present in the ground state when the surface contains a geodesic disc with integrated Gaussian curvature exceeding -pi/3. Finally we explore minimal energy configurations on sets of slices of a given Delaunay surface and obtain configurations and defect motifs consistent with those seen in stretching.

cond-mat.soft↗

arXiv2013

Defect annihilation and proliferation in active nematics

Liquid crystals inevitably possess topological defect excitations generated through boundary conditions, applied fields or in quenches to the ordered phase. In equilibrium pairs of defects coarsen and annihilate as the uniform ground state is approached. Here we show that defects in active liquid crystals exhibit profoundly different behavior, depending on the degree of activity and its contractile or extensile character. While contractile systems enhance the annihilation dynamics of passive systems, extensile systems act to drive defects apart so that they swarm around in the manner of topologically well-characterized self-propelled particles. We develop a simple analytical model for the defect dynamics which reproduces the key features of both the numerical solutions and recent experiments on microtuble-kinesin assemblies.

cond-mat.soft↗

arXiv2013

Delaunay Surfaces

We derive parametrizations of the Delaunay constant mean curvature surfaces of revolution that follow directly from parametrizations of the conics that generate these surfaces via the corresponding roulette. This uniform treatment exploits the natural geometry of the conic (parabolic, elliptic or hyperbolic) and leads to simple expressions for the mean and Gaussian curvatures of the surfaces as well as the construction of new surfaces.

math.DG↗

arXiv2012

The Electric Double Layer Structure Around Charged Spherical Interfaces

We derive a formally simple approximate analytical solution to the Poisson-Boltzmann equation for the spherical system via a geometric mapping. Its regime of applicability in the parameter space of the spherical radius and the surface potential is determined, and its superiority over the linearized solution is demonstrated.

cond-mat.soft↗

arXiv2011

Molecular Tilt on Monolayer-Protected Nanoparticles

The structure of the tilted phase of monolayer-protected nanoparticles is investigated by means of a simple Ginzburg-Landau model. The theory contains two dimensionless parameters representing the preferential tilt angle and the ratio epsilon between the energy cost due to spatial variations in the tilt of the coating molecules and that of the van der Waals interactions which favors uniform tilt. We analyze the model for both spherical and octahedral particles. On spherical particles, we find a transition from a tilted phase, at small epsilon, to a phase where the molecules spontaneously align along the surface normal and tilt disappears. Octahedral particles have an additional phase at small epsilon characterized by the presence of six topological defects. These defective configurations provide preferred sites for the chemical functionalization of monolayer-protected nanoparticles via place-exchange reactions and their consequent linking to form molecules and bulk materials.

cond-mat.soft↗

arXiv2011

Morphology of Nematic and Smectic Vesicles

Recent experiments on vesicles formed from block copolymers with liquid-crystalline side-chains reveal a rich variety of vesicle morphologies. The additional internal order ("structure") developed by these self-assembled block copolymer vesicles can lead to significantly deformed vesicles as a result of the delicate interplay between two-dimensional ordering and vesicle shape. The inevitable topological defects in structured vesicles of spherical topology also play an essential role in controlling the final vesicle morphology. Here we develop a minimal theoretical model for the morphology of the membrane structure with internal nematic/smectic order. Using both analytic and numerical approaches, we show that the possible low free energy morphologies include nano-size cylindrical micelles (nano-fibers), faceted tetrahedral vesicles, and ellipsoidal vesicles, as well as cylindrical vesicles. The tetrahedral vesicle is a particularly fascinating example of a faceted liquid-crystalline membrane. Faceted liquid vesicles may lead to the design of supra-molecular structures with tetrahedral symmetry and new classes of nano-carriers.

cond-mat.soft↗

arXiv2011

Self-Propulsion of Droplets by Spatially-Varying Roughness

Under partial wetting conditions, making a substrate uniformly rougher enhances the wetting characteristics of the corresponding smooth substrate {--} hydrophilic systems become even more hydrophilic and hydrophobic systems even more hydrophobic. Here we show that spatial texturing of the roughness may lead to spontaneous propulsion of droplets. Individual droplets are driven toward regions of maximal roughness for intrinsically hydrophilic systems and toward regions of minimal roughness for intrinsically hydrophobic systems. Spatial texturing can be achieved by wrinkling the substrate with sinusoidal grooves whose wavelength varies in one direction (inhomogeneous wrinkling) or lithographically etching a radial pattern of fractal (Koch curve) grooves on the substrate. Richer energy landscapes for droplet trajectories can be designed by combining roughness texturing with chemical or material patterning of the substrate.

cond-mat.soft↗

arXiv2010

Crystalline Order on Catenoidal Capillary Bridges

We study the defect structure of crystalline particle arrays on negative Gaussian curvature capillary bridges with vanishing mean curvature (catenoids). The threshold aspect ratio for the appearance of isolated disclinations is found and the optimal positions for dislocations determined. We also discuss the transition from isolated disclinations to scars as particle number and aspect ratio are varied.

cond-mat.soft↗

arXiv2009

Two-Dimensional Matter: Order, Curvature and Defects

Many systems in nature and the synthetic world involve ordered arrangements of units on two-dimensional surfaces. We review here the fundamental role payed by both the topology of the underlying surface and its detailed curvature. Topology dictates certain broad features of the defect structure of the ground state but curvature-driven energetics controls the detailed structured of ordered phases. Among the surprises are the appearance in the ground state of structures that would normally be thermal excitations and thus prohibited at zero temperature. Examples include excess dislocations in the form of grain boundary scars for spherical crystals above a minimal system size, dislocation unbinding for toroidal hexatics, interstitial fractionalization in spherical crystals and the appearance of well-separated disclinations for toroidal crystals. Much of the analysis leads to universal predictions that do not depend on the details of the microscopic interactions that lead to order in the first place. These predictions are subject to test by the many experimental soft and hard matter systems that lead to curved ordered structures such as colloidal particles self-assembling on droplets of one liquid in a second liquid. The defects themselves may be functionalized to create ligands with directional bonding. Thus nano to meso scale superatoms may be designed with specific valency for use in building supermolecules and novel bulk materials. Parameters such as particle number, geometrical aspect ratios and anisotropy of elastic moduli permit the tuning of the precise architecture of the superatoms and associated supermolecules. Thus the field has tremendous potential from both a fundamental and materials science/supramolecular chemistry viewpoint.

cond-mat.soft↗

arXiv2009

Smectic Polymer Vesicles

Polymer vesicles are stable robust vesicles made from block copolymer amphiphiles. Recent progress in the chemical design of block copolymers opens up the exciting possibility of creating a wide variety of polymer vesicles with varying fine structure, functionality and geometry. Polymer vesicles not only constitute useful systems for drug delivery and micro/nano-reactors but also provide an invaluable arena for exploring the ordering of matter on curved surfaces embedded in three dimensions. By choosing suitable liquid-crystalline polymers for one of the copolymer components one can create vesicles with smectic stripes. Smectic order on shapes of spherical topology inevitably possesses topological defects (disclinations) that are themselves distinguished regions for potential chemical functionalization and nucleators of vesicle budding. Here we report on glassy striped polymer vesicles formed from amphiphilic block copolymers in which the hydrophobic block is a smectic liquid crystal polymer containing cholesteryl-based mesogens. The vesicles exhibit two-dimensional smectic order and are ellipsoidal in shape with defects, or possible additional budding into isotropic vesicles, at the poles.

cond-mat.soft↗

arXiv2008

Elastic Theory of Defects in Toroidal Crystals

We report a comprehensive analysis of the ground state properties of axisymmetric toroidal crystals based on the elastic theory of defects on curved substrates. The ground state is analyzed as a function of the aspect ratio of the torus, which provides a non-local measure of the underlying Gaussian curvature, and the ratio of the defect core-energy to the Young modulus. Several structural features are discussed,including a spectacular example of curvature-driven amorphization in the limit of the aspect ratio approaching one. The outcome of the elastic theory is then compared with the results of a numerical study of a system of point-like particles constrained on the surface of a torus and interacting via a short range potential.

cond-mat.soft↗

arXiv2008

Topological Defects in Spherical Nematics

We study the organization of topological defects in a system of nematogens confined to the two-dimensional sphere (S^2). We first perform Monte Carlo simulations of a fluid system of hard rods (spherocylinders) living in the tangent plane of S^2. The sphere is adiabatically compressed until we reach a jammed nematic state with maximum packing density. The nematic state exhibits four +1/2 disclinations arrayed on a great circle rather than at the vertices of a regular tetrahedron. This arises from the high elastic anisotropy of the system in which splay (K_1) is far softer than bending (K_3). We also introduce and study a lattice nematic model on S^2 with tunable elastic constants and map out the preferred defect locations as a function of elastic anisotropy. We establish the existence of a one-parameter family of degenerate ground states in the extreme splay-dominated limit K_1/K_3 -> 0. Thus the global defect geometry is controllable by tuning the relative splay to bend modulus.

cond-mat.soft↗

arXiv2008

Vacancy diffusion in the triangular lattice dimer model

We study vacancy diffusion on the classical triangular lattice dimer model, sub ject to the kinetic constraint that dimers can only translate, but not rotate. A single vacancy, i.e. a monomer, in an otherwise fully packed lattice, is always localized in a tree-like structure. The distribution of tree sizes is asymptotically exponential and has an average of 8.16 \pm 0.01 sites. A connected pair of monomers has a finite probability of being delocalized. When delocalized, the diffusion of monomers is anomalous:

cond-mat.stat-mech↗

arXiv2008

Toroidal Crystals

Crystalline assemblages of identical sub-units packed together and elastically bent in the form of a torus have been found in the past ten years in a variety of systems of surprisingly different nature, such as viral capsids, self-assembled monolayers and carbon nanomaterials. In this Letter we analyze the structural properties of toroidal crystals and we provide a unified description based on the elastic theory of defects in curved geometries. We find ground states characterized by the presence of 5-fold disclinations on the exterior of the torus and 7-fold disclinations in the interior. The number of excess disclinations is controlled primarily by the aspect ratio of the torus, suggesting a novel mechanism for creating toroidal templates with precisely controlled valency via functionalization of the defect sites.

cond-mat.soft↗

arXiv2007

Bubble Raft Model for a Paraboloidal Crystal

We investigate crystalline order on a two-dimensional paraboloid of revolution by assembling a single layer of millimeter-sized soap bubbles on the surface of a rotating liquid, thus extending the classic work of Bragg and Nye on planar soap bubble rafts. Topological constraints require crystalline configurations to contain a certain minimum number of topological defects such as disclinations or grain boundary scars whose structure is analyzed as a function of the aspect ratio of the paraboloid. We find the defect structure to agree with theoretical predictions and propose a mechanism for scar nucleation in the presence of large Gaussian curvature.

cond-mat.soft↗

arXiv2007

Interstitial Fractionalization and Spherical Crystallography

Finding the ground states of identical particles packed on spheres has relevance for stabilizing emulsions and a venerable history in the literature of theoretical physics and mathematics. Theory and experiment have confirmed that defects such as disclinations and dislocations are an intrinsic part of the ground state. Here we discuss the remarkable behavior of vacancies and interstitials in spherical crystals. The strain fields of isolated disclinations forced in by the spherical topology literally rip interstitials and vacancies apart, typically into dislocation fragments that combine with the disclinations to create small grain boundary scars. The fractionation is often into three charge-neutral dislocations, although dislocation pairs can be created as well. We use a powerful, freely available computer program to explore interstitial fractionalization in some detail, for a variety of power law pair potentials. We investigate the dependence on initial conditions and the final state energies, and compare the position dependence of interstitial energies with the predictions of continuum elastic theory on the sphere. The theory predicts that, before fragmentation, interstitials are repelled from 5-fold disclinations and vacancies are attracted. We also use vacancies and interstitials to study low energy states in the vicinity of "magic numbers" that accommodate regular icosadeltahedral tessellations.

cond-mat.soft↗

arXiv2007

Crystalline Order On Riemannian Manifolds With Variable Gaussian Curvature And Boundary

We investigate the zero temperature structure of a crystalline monolayer constrained to lie on a two-dimensional Riemannian manifold with variable Gaussian curvature and boundary. A full analytical treatment is presented for the case of a paraboloid of revolution. Using the geometrical theory of topological defects in a continuum elastic background we find that the presence of a variable Gaussian curvature, combined with the additional constraint of a boundary, gives rise to a rich variety of phenomena beyond that known for spherical crystals. We also provide a numerical analysis of a system of classical particles interacting via a Coulomb potential on the surface of a paraboloid.

cond-mat.soft↗