Controlling the shape and topology of two-component colloidal membranes.

Changes in the geometry and topology of self-assembled membranes underlie diverse processes across cellular biology and engineering. Similar to lipid bilayers, monolayer colloidal membranes have in-plane fluid-like dynamics and out-of-plane bending elasticity. Their open edges and micrometer-length scale provide a tractable system to study the equilibrium energetics and dynamic pathways of membrane assembly and reconfiguration. Here, we find that doping colloidal membranes with short miscible rods transforms disk-shaped membranes into saddle-shaped surfaces with complex edge structures. The saddle-shaped membranes are well approximated by Enneper's minimal surfaces. Theoretical modeling demonstrates that their formation is driven by increasing the positive Gaussian modulus, which in turn, is controlled by the fraction of short rods. Further coalescence of saddle-shaped surfaces leads to diverse topologically distinct structures, including shapes similar to catenoids, trinoids, four-noids, and higher-order structures. At long timescales, we observe the formation of a system-spanning, sponge-like phase. The unique features of colloidal membranes reveal the topological transformations that accompany coalescence pathways in real time. We enhance the functionality of these membranes by making their shape responsive to external stimuli. Our results demonstrate a pathway toward control of thin elastic sheets' shape and topology-a pathway driven by the emergent elasticity induced by compositional heterogeneity.

Flow states of two dimensional active gels driven by external shear.

Using a minimal hydrodynamic model, we theoretically and computationally study the Couette flow of active gels in straight and annular two-dimensional channels subject to an externally imposed shear. The gels are isotropic in the absence of externally- or activity-driven shear, but have nematic order that increases with shear rate. Using the finite element method, we determine the possible flow states for a range of activities and shear rates. Linear stability analysis of an unconfined gel in a straight channel shows that an externally imposed shear flow can stabilize an extensile fluid that would be unstable to spontaneous flow in the absence of the shear flow, and destabilize a contractile fluid that would be stable against spontaneous flow in the absence of shear flow. These results are in rough agreement with the stability boundaries between the base shear flow state and the nonlinear flow states that we find numerically for a confined active gel. For extensile fluids, we find three kinds of nonlinear flow states in the range of parameters we study: unidirectional flows, oscillatory flows, and dancing flows. To highlight the activity-driven spontaneous component of the nonlinear flows, we characterize these states by the average volumetric flow rate and the wall stress. For contractile fluids, we only find the linear shear flow and a nonlinear unidirectional flow in the range of parameters that we studied. For large magnitudes of the activity, the unidirectional contractile flow develops a boundary layer. Our analysis of annular channels shows how curvature of the streamlines in the base flow affects the transitions among flow states.

Chiral fluid membranes with orientational order and multiple edges.

We carry out Monte Carlo simulations on fluid membranes with orientational order and multiple edges in the presence and absence of external forces. The membrane resists bending and has an edge tension, the orientational order couples with the membrane surface normal through a cost for tilting, and there is a chiral liquid crystalline interaction. In the absence of external forces, a membrane initialized as a vesicle will form a disk at low chirality, with the directors forming a smectic-A phase with alignment perpendicular to the membrane surface except near the edge. At large chirality a catenoid-like shape or a trinoid-like shape is formed, depending on the number of edges in the initial vesicle. This shape change is accompanied by cholesteric ordering of the directors and multiple π walls connecting the membrane edges and wrapping around the membrane neck. If the membrane is initialized instead in a cylindrical shape and stretched by an external force, it maintains a nearly cylindrical shape but additional liquid crystalline phases appear. For large tilt coupling and low chirality, a smectic-A phase forms where the directors are normal to the surface of the membrane. For lower values of the tilt coupling, a nematic phase appears at zero chirality with the average director oriented perpendicular to the long axis of the membrane, while for nonzero chirality a cholesteric phase appears. The π walls are tilt walls at low chirality and transition to twist walls as chirality is increased. We construct a continuum model of the director field to explain this behavior.

Deformation and orientational order of chiral membranes with free edges.

Motivated by experiments on colloidal membranes composed of chiral rod-like viruses, we use Monte Carlo methods to simulate these systems and determine the phase diagram for the liquid crystalline order of the rods and the membrane shape. We generalize the Lebwohl-Lasher model for a nematic with a chiral coupling to a curved surface with edge tension and a resistance to bending, and include an energy cost for tilting of the rods relative to the local membrane normal. The membrane is represented by a triangular mesh of hard beads joined by bonds, where each bead is decorated by a director. The beads can move, the bonds can reconnect and the directors can rotate at each Monte Carlo step. When the cost of tilt is small, the membrane tends to be flat, with the rods only twisting near the edge for low chiral coupling, and remaining parallel to the normal in the interior of the membrane. At high chiral coupling, the rods twist everywhere, forming a cholesteric state. When the cost of tilt is large, the emergence of the cholesteric state at high values of the chiral coupling is accompanied by the bending of the membrane into a saddle shape. Increasing the edge tension tends to flatten the membrane. These results illustrate the geometric frustration arising from the inability of a surface normal to have twist.

Axisymmetric membranes with edges under external force: buckling, minimal surfaces, and tethers.

We use theory and numerical computation to determine the shape of an axisymmetric fluid membrane with a resistance to bending and constant area. The membrane connects two rings in the classic geometry that produces a catenoidal shape in a soap film. In our problem, we find infinitely many branches of solutions for the shape and external force as functions of the separation of the rings, analogous to the infinite family of eigenmodes for the Euler buckling of a slender rod. Special attention is paid to the catenoid, which emerges as the shape of maximal allowable separation when the area is less than a critical area equal to the planar area enclosed by the two rings. A perturbation theory argument directly relates the tension of catenoidal membranes to the stability of catenoidal soap films in this regime. When the membrane area is larger than the critical area, we find additional cylindrical tether solutions to the shape equations at large ring separation, and that arbitrarily large ring separations are possible. These results apply for the case of vanishing Gaussian curvature modulus; when the Gaussian curvature modulus is nonzero and the area is below the critical area, the force and the membrane tension diverge as the ring separation approaches its maximum value. We also examine the stability of our shapes and analytically show that catenoidal membranes have markedly different stability properties than their soap film counterparts.

Force-Induced Formation of Twisted Chiral Ribbons.

We demonstrate that an achiral stretching force transforms disk-shaped colloidal membranes composed of chiral rods into twisted ribbons with handedness opposite the preferred twist of the rods. Using an experimental technique that enforces torque-free boundary conditions we simultaneously measure the force-extension curve and the ribbon shape. An effective theory that accounts for the membrane bending energy and uses geometric properties of the edge to model the internal liquid crystalline degrees of freedom explains both the measured force-extension curve and the force-induced twisted shape.

Stability of the interface of an isotropic active fluid.

We study the linear stability of an isotropic active fluid in three different geometries: a film of active fluid on a rigid substrate, a cylindrical thread of fluid, and a spherical fluid droplet. The active fluid is modeled by the hydrodynamic theory of an active nematic liquid crystal in the isotropic phase. In each geometry, we calculate the growth rate of sinusoidal modes of deformation of the interface. There are two distinct branches of growth rates; at long wavelength, one corresponds to the deformation of the interface, and one corresponds to the evolution of the liquid crystalline degrees of freedom. The passive cases of the film and the spherical droplet are always stable. For these geometries, a sufficiently large activity leads to instability. Activity also leads to propagating damped or growing modes. The passive cylindrical thread is unstable for perturbations with wavelength longer than the circumference. A sufficiently large activity can make any wavelength unstable, and again leads to propagating damped or growing modes. Our calculations are carried out for the case of zero Frank elasticity. While Frank elasticity is a stabilizing mechanism as it penalizes distortions of the order parameter tensor, we show that it has a small effect on the instabilities considered here.

Enhancement of Microorganism Swimming Speed in Active Matter.

We study a swimming undulating sheet in the isotropic phase of an active nematic liquid crystal. Activity changes the effective shear viscosity, reducing it to zero at a critical value of activity. Expanding in the sheet amplitude, we find that the correction to the swimming speed due to activity is inversely proportional to the effective shear viscosity. Our perturbative calculation becomes invalid near the critical value of activity; using numerical methods to probe this regime, we find that activity enhances the swimming speed by an order of magnitude compared to the passive case.

Shapes of fluid membranes with chiral edges.

We carry out Monte Carlo simulations of a colloidal fluid membrane with a free edge and composed of chiral rodlike viruses. The membrane is modeled by a triangular mesh of beads connected by bonds in which the bonds and beads are free to move at each Monte Carlo step. Since the constituent viruses are experimentally observed to twist only near the membrane edge, we use an effective energy that favors a particular sign of the geodesic torsion of the edge. The effective energy also includes the membrane bending stiffness, edge bending stiffness, and edge tension. We find three classes of membrane shapes resulting from the competition of the various terms in the free energy: branched shapes, chiral disks, and vesicles. Increasing the edge bending stiffness smooths the membrane edge, leading to correlations among the membrane normals at different points along the edge. The normalized power spectrum for edge displacements shows a peak with increasing preferred geodesic torsion. We also consider membrane shapes under an external force by fixing the distance between two ends of the membrane and finding the shape for increasing values of the distance between the two ends. As the distance increases, the membrane twists into a ribbon, with the force eventually reaching a plateau.

Topological structure and dynamics of three-dimensional active nematics.

Topological structures are effective descriptors of the nonequilibrium dynamics of diverse many-body systems. For example, motile, point-like topological defects capture the salient features of two-dimensional active liquid crystals composed of energy-consuming anisotropic units. We dispersed force-generating microtubule bundles in a passive colloidal liquid crystal to form a three-dimensional active nematic. Light-sheet microscopy revealed the temporal evolution of the millimeter-scale structure of these active nematics with single-bundle resolution. The primary topological excitations are extended, charge-neutral disclination loops that undergo complex dynamics and recombination events. Our work suggests a framework for analyzing the nonequilibrium dynamics of bulk anisotropic systems as diverse as driven complex fluids, active metamaterials, biological tissues, and collections of robots or organisms.

Direct measurement of the twist penetration length in a single smectic A layer of colloidal virus particles.

In the 1970s, deGennes discussed the fundamental geometry of smectic liquid crystals and established an analogy between the smectic A phase and superconductors. It follows that smectic layers expel twist deformations in the same way that superconductors expel magnetic field. We make a direct observation of the penetration of twist at the edge of a single isolated smectic A layer composed of chiral fd virus particles subjected to a depletion interaction. Using the LC-PolScope, we make quantitative measurements of the spatial dependence of the birefringence due to molecular tilt near the layer edges. We match data to theory for the molecular tilt penetration profile and determine the twist penetration length for this system.

Nematic cells with quasicrystalline-patterned alignment layers.

Nematic cells with surface anchoring fields exhibiting quasicrystalline symmetry can be fabricated using linear photopolymerizable polymers and suitable optics. Using the Lebwohl-Lasher model we carry out Monte Carlo simulations of a nematic cell where the top and bottom surfaces have an anchoring field with the symmetry of a periodic approximant to a Penrose lattice. We show that the anchoring field has point topological defects, nearly all with topological charge +/-1 . Our simulations, which assume infinitely strong anchoring of the nematic to the anchoring field, show that half-integer disclination lines emerge from the point defects and either traverse the thickness of the cell for small cell thicknesses, hug the patterned surfaces for large thicknesses, or combine these behaviors for intermediate thicknesses. We show that estimates of the values of the thicknesses separating these three behaviors can be obtained using the properties of Penrose tilings.

Nematic cells with defect-patterned alignment layers.

Using Monte Carlo simulations of the Lebwohl-Lasher model we study the director ordering in a nematic cell where the top and bottom surfaces are patterned with a lattice of +/-1 point topological defects of lattice spacing a . As expected on general physical grounds we find that the nematic order depends on the ratio of the height of the cell H to a . For thick cells (Ha > or = 0.9) we find that the system is very well ordered and the frustration induced by the lattice of defects is relieved in a novel way by a network of half-integer defect lines which emerge from the point defects and hug the top and bottom surfaces of the cell. When Ha < or = 0.9 the system has zero nematic order parameter and the half-integer defect lines thread through the cell joining point defects on the top and bottom surfaces. We present a simple physical argument in terms of the length of the defect lines to explain these results. To facilitate eventual comparison with experimental systems we also simulate optical textures in the presence of crossed polarizers.

Role of electrostatics in the texture of islands in free-standing ferroelectric liquid crystal films.

Curved textures of ferroelectric smectic-C* liquid crystals produce space charge when they involve divergence of the spontaneous polarization field. Impurity ions can partially screen this space charge, reducing long-range interactions to local ones. Through studies of the textures of islands on very thin free-standing smectic films, we see evidence of this effect, in which materials with a large spontaneous polarization have static structures described by a large effective bend elastic constant. To address this issue, we calculated the electrostatic free energy of a free-standing film of ferroelectric liquid crystal, showing how the screened Coulomb interaction contributes a term to the effective bend elastic constant, in the static long-wavelength limit. We report experiments which support the main features of this model.

Dynamics of the molecular orientation field coupled to ions in two-dimensional ferroelectric liquid crystals.

Molecular orientation fluctuations in ferroelectric smectic liquid crystals produce space charges, due to the divergence of the spontaneous polarization. These space charges interact with mobile ions, so that one must consider the coupled dynamics of the orientation and ionic degrees of freedom. Previous theory and light scattering experiments on thin free-standing films of ferroelectric liquid crystals have not included this coupling, possibly invalidating their quantitative conclusions. We consider the most important case of very slow ionic dynamics, compared to rapid orientational fluctuations, and focus on the use of a short electric field pulse to quench orientational fluctuations. We find that the resulting change in scattered light intensity must include a term due to the quasistatic ionic configuration, which has previously been ignored. In addition to developing the general theory, we present a simple model to demonstrate the role of this added term.

Vesicle shape, molecular tilt, and the suppression of necks.

Can the presence of molecular-tilt order significantly affect the shapes of lipid bilayer membranes, particularly membrane shapes with narrow necks? Motivated by the propensity for tilt order and the common occurrence of narrow necks in the intermediate stages of biological processes such as endocytosis and vesicle trafficking, we examine how tilt order inhibits the formation of necks in the equilibrium shapes of vesicles. For vesicles with a spherical topology, point defects in the molecular order with a total strength of +2 are required. We study axisymmetric shapes and suppose that there is a unit-strength defect at each pole of the vesicle. The model is further simplified by the assumption of tilt isotropy: invariance of the energy with respect to rotations of the molecules about the local membrane normal. This isotropy condition leads to a minimal coupling of tilt order and curvature, giving a high energetic cost to regions with Gaussian curvature and tilt order. Minimizing the elastic free energy with constraints of fixed area and fixed enclosed volume determines the allowed shapes. Using numerical calculations, we find several branches of solutions and identify them with the branches previously known for fluid membranes. We find that tilt order changes the relative energy of the branches, suppressing thin necks by making them costly, leading to elongated prolate vesicles as a generic family of tilt-ordered membrane shapes.

Unwinding of a strained cholesteric elastomer by disclination loop nucleation.

The application of a sufficiently strong strain perpendicular to the pitch axis of a monodomain cholesteric elastomer unwinds the cholesteric helix. Previous theoretical analyses of this transition ignored the effects of Frank elasticity which we include here. We find that the strain needed to unwind the helix is reduced because of the Frank penalty and the cholesteric state becomes metastable above the transition. We consider in detail a previously proposed mechanism by which the topologically stable helical texture is removed in the metastable state: namely, by the nucleation of twist disclination loops in the plane perpendicular to the pitch axis. We present an approximate calculation of the barrier energy for this nucleation process which neglects possible spatial variation of the strain fields in the elastomer, as well as a more accurate calculation based on a finite-element modeling of the elastomer.

Chiral edge fluctuations of colloidal membranes.

We study edge fluctuations of a flat colloidal membrane comprised of a monolayer of aligned filamentous viruses. Experiments reveal that a peak in the spectrum of the in-plane edge fluctuations arises for sufficiently strong virus chirality. Accounting for internal liquid crystalline degrees of freedom by the length, curvature, and geodesic torsion of the edge, we calculate the spectrum of the edge fluctuations. The theory quantitatively describes the experimental data, demonstrating that chirality couples in-plane and out-of-plane edge fluctuations to produce the peak.

Simulation and visualization of topological defects in nematic liquid crystals.

We present a method of visualizing topological defects arising in numerical simulations of liquid crystals. The method is based on scientific visualization techniques developed to visualize second-rank tensor fields, yielding information not only on the local structure of the field but also on the continuity of these structures. We show how these techniques can be used to first locate topological defects in fluid simulations of nematic liquid crystals where the locations are not known a priori and then study the properties of these defects including the core structure. We apply these techniques to simulation data obtained by previous authors who studied a rapid quench and subsequent equilibration of a Gay-Berne nematic. The quench produces a large number of disclination loops which we locate and track with the visualization methods. We show that the cores of the disclination lines have a biaxial region and the loops themselves are of a hybrid wedge-twist variety.

Techniques for the visualization of topological defect behavior in nematic liquid crystals.

We present visualization tools for analyzing molecular simulations of liquid crystal (LC) behavior. The simulation data consists of terabytes of data describing the position and orientation of every molecule in the simulated system over time. Condensed matter physicists study the evolution of topological defects in these data, and our visualization tools focus on that goal. We first convert the discrete simulation data to a sampled version of a continuous second-order tensor field and then use combinations of visualization methods to simultaneously display combinations of contractions of the tensor data, providing an interactive environment for exploring these complicated data. The system, built using AVS, employs colored cutting planes, colored isosurfaces, and colored integral curves to display fields of tensor contractions including Westin's scalar cl, cp, and cs metrics and the principal eigenvector. Our approach has been in active use in the physics lab for over a year. It correctly displays structures already known; it displays the data in a spatially and temporally smoother way than earlier approaches, avoiding confusing grid effects and facilitating the study of multiple time steps; it extends the use of tools developed for visualizing diffusion tensor data, re-interpreting them in the context of molecular simulations; and it has answered long-standing questions regarding the orientation of molecules around defects and the conformational changes of the defects.