Topological defect-mediated morphodynamics of active-active interfaces.

Physical interfaces widely exist in nature and engineering. Although the formation of passive interfaces is well elucidated, the physical principles governing active interfaces remain largely unknown. Here, we combine simulation, theory, and cell-based experiment to investigate the evolution of an active-active interface. We adopt a biphasic framework of active nematic liquid crystals. We find that long-lived topological defects mechanically energized by activity display unanticipated dynamics nearby the interface, where defects perform "U-turns" to keep away from the interface, push the interface to develop local fingers, or penetrate the interface to enter the opposite phase, driving interfacial morphogenesis and cross-interface defect transport. We identify that the emergent interfacial morphodynamics stems from the instability of the interface and is further driven by the activity-dependent defect-interface interactions. Experiments of interacting multicellular monolayers with extensile and contractile differences in cell activity have confirmed our predictions. These findings reveal a crucial role of topological defects in active-active interfaces during, for example, boundary formation and tissue competition that underlie organogenesis and clinically relevant disorders.

Chiral Pearlescent Cellulose Nanocrystals Films with Broad-Range Tunable Optical Properties for Anti-Counterfeiting Applications.

Pearlescent materials are of technological importance in a diverse array of industries from cosmetics to premium paints; however, chiral pearlescent materials remain unexplored. Here, chiral pearlescent films with on-demand iridescence and metallic appearance are simply organized by leveraging vertical pressure to direct the self-assembly of cellulose nanocrystals. The films are formed with a bilayer planar anchored left-handed chiral nematic architecture, in which the bottom layer is featured with a vertical gradient pitch, and the top layer is featured with a uniform pitch. Simultaneous reflection of the rainbow colors and an on-demand color of left-handed polarized light with angle-dependent wavelength and polarization state accounts for the unique optical phenomenon based on experimental observation and theoretical analysis. Such chiroptical property can be readily tuned with architectural design, enabling reproducible optical appearance with high fidelity. Bringing the pearlescence, iridescence, and specular reflection together endows cellulose nanocrystal films with rich and tunable chiroptical properties that can be used for anti-counterfeiting applications. The current work marks the beginning of chiral pearlescent materials from renewable resources, while the pressure-directed self-assembly provides a step toward scalable production.

Structures and topological defects in pressure-driven lyotropic chromonic liquid crystals.

Lyotropic chromonic liquid crystals are water-based materials composed of self-assembled cylindrical aggregates. Their behavior under flow is poorly understood, and quantitatively resolving the optical retardance of the flowing liquid crystal has so far been limited by the imaging speed of current polarization-resolved imaging techniques. Here, we employ a single-shot quantitative polarization imaging method, termed polarized shearing interference microscopy, to quantify the spatial distribution and the dynamics of the structures emerging in nematic disodium cromoglycate solutions in a microfluidic channel. We show that pure-twist disclination loops nucleate in the bulk flow over a range of shear rates. These loops are elongated in the flow direction and exhibit a constant aspect ratio that is governed by the nonnegligible splay-bend anisotropy at the loop boundary. The size of the loops is set by the balance between nucleation forces and annihilation forces acting on the disclination. The fluctuations of the pure-twist disclination loops reflect the tumbling character of nematic disodium cromoglycate. Our study, including experiment, simulation, and scaling analysis, provides a comprehensive understanding of the structure and dynamics of pressure-driven lyotropic chromonic liquid crystals and might open new routes for using these materials to control assembly and flow of biological systems or particles in microfluidic devices.

Alkylbenzoic and Alkyloxybenzoic Acid Blending for Expanding the Liquid Crystalline State and Improving Its Rheology.

Thermotropic mesogens typically exist as liquid crystals (LCs) in a narrow region of high temperatures, making lowering their melting point with the temperature expansion of the mesophase state an urgent task. Para-substituted benzoic acids can form LCs through noncovalent dimerization into homodimers via hydrogen bonds, whose strength and, consequently, the temperature region of the mesophase state can be potentially altered by creating asymmetric heterodimers from different acids. This work investigates equimolar blends of p-n-alkylbenzoic (kBA, where k is the number of carbon atoms in the alkyl radical) and p-n-alkyloxybenzoic (kOBA) acids by calorimetry and viscometry to establish their phase transitions and regions of mesophase existence. Non-symmetric dimerization of acids leads to the extension of the nematic state region towards low temperatures and the appearance of new monotropic and enantiotropic phase transitions in several cases. Moreover, the crystal-nematic and nematic-isotropic phase changes have a two-step character for some acid blends, suggesting the formation of symmetric and asymmetric associates from heterodimers. The mixing of 6BA and 8OBA most strongly extends the region of the nematic state towards low temperatures (from 95-114 °C and 108-147 °C for initial homodimers, respectively, to 57-133 °C for the resulting heterodimer), whereas the combination of 4OBA and 5OBA gives the most extended high-temperature nematic phase (up to 156 °C) and that of 6BA and 9OBA (or 12OBA) provides the existence of a smectic phase at the lowest temperatures (down to 51 °C).

Data-driven quantitative modeling of bacterial active nematics.

Active matter comprises individual units that convert energy into mechanical motion. In many examples, such as bacterial systems and biofilament assays, constituent units are elongated and can give rise to local nematic orientational order. Such "active nematics" systems have attracted much attention from both theorists and experimentalists. However, despite intense research efforts, data-driven quantitative modeling has not been achieved, a situation mainly due to the lack of systematic experimental data and to the large number of parameters of current models. Here, we introduce an active nematics system made of swarming filamentous bacteria. We simultaneously measure orientation and velocity fields and show that the complex spatiotemporal dynamics of our system can be quantitatively reproduced by a type of microscopic model for active suspensions whose important parameters are all estimated from comprehensive experimental data. This provides unprecedented access to key effective parameters and mechanisms governing active nematics. Our approach is applicable to different types of dense suspensions and shows a path toward more quantitative active matter research.

Director alignment at the nematic-isotropic interface: elastic anisotropy and active anchoring.

Activity in nematics drives interfacial flows that lead to preferential alignment that is tangential or planar for extensile systems (pushers) and perpendicular or homeotropic for contractile ones (pullers). This alignment is known as active anchoring and has been reported for a number of systems and described using active nematic hydrodynamic theories. The latter are based on the one-elastic constant approximation, i.e. they assume elastic isotropy of the underlying passive nematic. Real nematics, however, have different elastic constants, which lead to interfacial anchoring. In this paper, we consider elastic anisotropy in multiphase and multicomponent hydrodynamic models of active nematics and investigate the competition between the interfacial alignment driven by the elastic anisotropy of the passive nematic and the active anchoring. We start by considering systems with translational invariance to analyse the alignment at flat interfaces and, then, consider two-dimensional systems and active nematic droplets. We investigate the competition of the two types of anchoring over a wide range of the other parameters that characterize the system. The results of the simulations reveal that the active anchoring dominates except at very low activities, when the interfaces are static. In addition, we found that the elastic anisotropy does not affect the dynamics but changes the active length that becomes anisotropic. This article is part of the theme issue 'Progress in mesoscale methods for fluid dynamics simulation'.

A nonequilibrium force can stabilize 2D active nematics.

Suspensions of actively driven anisotropic objects exhibit distinctively nonequilibrium behaviors, and current theories predict that they are incapable of sustaining orientational order at high activity. By contrast, here we show that nematic suspensions on a substrate can display order at arbitrarily high activity due to a previously unreported, potentially stabilizing active force. This force moreover emerges inevitably in theories of active orientable fluids under geometric confinement. The resulting nonequilibrium ordered phase displays robust giant number fluctuations that cannot be suppressed even by an incompressible solvent. Our results apply to virtually all experimental assays used to investigate the active nematic ordering of self-propelled colloids, bacterial suspensions, and the cytoskeleton and have testable implications in interpreting their nonequilibrium behaviors.

Nematic twist-bend phase in an external field.

The response of the nematic twist-bend ([Formula: see text]) phase to an applied field can provide important insight into the structure of this liquid and may bring us closer to understanding mechanisms generating mirror symmetry breaking in a fluid of achiral molecules. Here we investigate theoretically how an external uniform field can affect structural properties and the stability of [Formula: see text] Assuming that the driving force responsible for the formation of this phase is packing entropy, we show, within Landau-de Gennes theory, that [Formula: see text] can undergo a rich sequence of structural changes with the field. For the systems with positive anisotropy of permittivity, we first observe a decrease of the tilt angle of [Formula: see text] until it transforms through a field-induced phase transition to the ordinary prolate uniaxial nematic phase (N). Then, at very high fields, this nematic phase develops polarization perpendicular to the field ([Formula: see text]). For systems with negative anisotropy of permittivity, the results reveal new modulated structures. Even an infinitesimally small field transforms [Formula: see text] to its elliptical counterpart ([Formula: see text]), where the circular base of the cone of the main director becomes elliptic. With stronger fields, the ellipse degenerates to a line, giving rise to a nonchiral periodic structure, the nematic splay-bend ([Formula: see text]), where the two nematic directors are restricted to a plane. The three structures-[Formula: see text], [Formula: see text], and [Formula: see text]-with a modulated polar order are globally nonpolar. But further increase of the field induces phase transitions into globally polar structures with nonvanishing polarization along the field's direction. We found two such structures, one of which is a polar and chiral modification of [Formula: see text], where splay and bend deformations are accompanied by weak twist deformations ([Formula: see text]). Further increase of the field unwinds this structure into a polar nematic ([Formula: see text]) of polarization parallel to the field.

Wrinkling Instability in 3D Active Nematics.

In nature, interactions between biopolymers and motor proteins give rise to biologically essential emergent behaviors. Besides cytoskeleton mechanics, active nematics arise from such interactions. Here we present a study on 3D active nematics made of microtubules, kinesin motors, and depleting agent. It shows a rich behavior evolving from a nematically ordered space-filling distribution of microtubule bundles toward a flattened and contracted 2D ribbon that undergoes a wrinkling instability and subsequently transitions into a 3D active turbulent state. The wrinkle wavelength is independent of the ATP concentration and our theoretical model describes its relation with the appearance time. We compare the experimental results with a numerical simulation that confirms the key role of kinesin motors in cross-linking and sliding the microtubules. Our results on the active contraction of the network and the independence of wrinkle wavelength on ATP concentration are important steps forward for the understanding of these 3D systems.

Experimental and Computational Study of a Liquid Crystalline Dimesogen Exhibiting Nematic, Twist-Bend Nematic, Intercalated Smectic, and Soft Crystalline Mesophases.

Liquid crystalline dimers and dimesogens have attracted significant attention due to their tendency to exhibit twist-bend modulated nematic (NTB) phases. While the features that give rise to NTB phase formation are now somewhat understood, a comparable structure-property relationship governing the formation of layered (smectic) phases from the NTB phase is absent. In this present work, we find that by selecting mesogenic units with differing polarities and aspect ratios and selecting an appropriately bent central spacer we obtain a material that exhibits both NTB and intercalated smectic phases. The higher temperature smectic phase is assigned as SmCA based on its optical textures and X-ray scattering patterns. A detailed study of the lower temperature smectic ''X'' phase by optical microscopy and SAXS/WAXS demonstrates this phase to be smectic, with an in-plane orthorhombic or monoclinic packing and long (>100 nm) out of plane correlation lengths. This phase, which has been observed in a handful of materials to date, is a soft-crystal phase with an anticlinic layer organisation. We suggest that mismatching the polarities, conjugation and aspect ratios of mesogenic units is a useful method for generating smectic forming dimesogens.

Pentaerythritol Derived Tetrapode Exhibiting a Nematic-Like Mesophase at Ambient Temperatures.

The nematic liquid-crystalline phase exhibits average orientational order, with no positional organisation. So-called modulated nematic phases exhibit this same orientational order with an additional spatially periodic modulation of the nematic director, the most common of which is the twist-bend nematic phase. We report a pentaerythritol derived tetrapode which exhibits a nematic-like mesophase at ambient temperature, and we denote this new mesophase 'NX ' to indicate a nematic phase of unknown structure. X-ray scattering experiments refute the possibility of positional order, yet optical textures are consistent with a periodic structure. We suggest that the mesophase exhibited by this material is a new type of nematic-like mesophase with some form of modulated structure. We find the NX phase to exhibit an electrooptic response consistent with a nematic-like phase.

A Nanohelicoidal Nematic Liquid Crystal Formed by a Non-Linear Duplexed Hexamer.

The twist-bend modulated nematic liquid-crystal phase exhibits formation of a nanometre-scale helical pitch in a fluid and spontaneous breaking of mirror symmetry, leading to a quasi-fluid state composed of chiral domains despite being composed of achiral materials. This phase was only observed for materials with two or more mesogenic units, the manner of attachment between which is always linear. Non-linear oligomers with a H-shaped hexamesogen are now found to exhibit both nematic and twist-bend modulated nematic phases. This shatters the assumption that a linear sequence of mesogenic units is a prerequisite for this phase, and points to this state of matter being exhibited by a wider range of self-assembling structures than was previously envisaged. These results support the double helix model of the TB phase as opposed to the simple heliconical model. This new class of materials could act as low-molecular-weight surrogates for cross-linked liquid-crystalline elastomers.

Quinquephenyl: the simplest rigid-rod-like nematic liquid crystal, or is it? An atomistic simulation.

We have performed an atomistic molecular-dynamics study on the molecular organization and liquid-crystalline properties of quinquephenyl (P5), a prototypical mesogen that is of interest for organic electronics. The thermotropic behavior reveals different mesophases. When cooling down from the isotropic phase, a transition to nematic (≈715 K) is found, then a smectic SA (≈657 K) and another smectic, SXA (≈642 K), before a crystalline phase is recovered (≈617 K). This phase sequence is compared with experimental findings. The different phases are described in terms of their molecular organization, orientational and positional order parameters, and pair distribution functions, as well as of their dynamics properties. In particular, the smectic phases that have not yet been characterized experimentally are discussed. By analyzing the effective shape of P5, it is concluded that its internal torsions and bending make it less rigid than could be expected.

The Casimir-like effect induced by active nematics.

We consider an active nematic phase and use hydrodynamical equations of it to model the activity as an internal field. The interaction of this field with the nematic director in a confined geometry is included in the Hamiltonian of the system. Based on this model Hamiltonian and the standard field theoretical approach, the Casimir-like force induced between the boundaries of such a confined film is discussed. The force depends on the geometrical shape and the dynamical character of the constituents of our active phase, as well as the anchoring conditions. For homeotropically aligned rod-like particles which in principle tend to align along a planar flow field, extensile activity enhances the attraction present in a thin nematic film. As the film thickness increases the force reduces. Beyond a critical thickness, a planar flow field instantaneous to a bend distortion sets in. Near but below the threshold of this activity-induced instability, the force crosses zero and repulsively diverges right at the critical threshold of this so-called flow instability. For contractile rods, in the same geometry as above, the structure is stable and the Casimir-like force diminishes by an exponential factor as a function of the film thickness. On the other side for a planar director alignment, rod-like contractile particles can induce opposite shear flows at the boundaries creating a splay distortion for the director between the plates. In this configuration, we obtain the same universal pretransitional behavior for the force as above. Vice versa, for extensile rod-like particles in this geometry, the director fluctuations become massive and the Casimir-like force diminishes again by an exponential factor as the film thickness increases. The effect of the active field on thermal fluctuations of the director and the fluctuation-induced Casimir force per area is derived through a "semi"-dynamical approach as well. However, the results of the calculation due to a mathematical sum over the fluctuating modes do not lead to an approved closed form.

The TV in your pocket: development of liquid-crystal materials for the new millennium.

New liquid crystals with very low viscosity, good mesophase behavior, and high reliability are necessary to achieve the breakthrough from flat computer monitors to large displays for television. Fluorine plays a decisive role not only because of the polarity it induces in organic molecules but also because of its low polarizability and weak propensity for ion solvation. In addition, subtle stereoelectronic effects in fluorine-containing liquid crystals influence material properties and allow these to be tuned to some extent to achieve the desired outcome. Some fairly sophisticated chemistry is required that is normally ruled out in the specialty chemicals industry because of cost. The television display market is now entering a phase of saturation. The broad availability of the internet has led to an ever increasing tendency for mobile products. Tablet PCs and smartphones require touch-panel functionality and low power consumption. New LCD modes with high-performance liquid crystals and additional components, such as polymerizable materials, can be used in such products.

Molecular-scale substrate anisotropy, crowding and division drive collective behaviours in cell monolayers.

The ability of cells to reorganize in response to external stimuli is important in areas ranging from morphogenesis to tissue engineering. While nematic order is common in biological tissues, it typically only extends to small regions of cells interacting via steric repulsion. On isotropic substrates, elongated cells can co-align due to steric effects, forming ordered but randomly oriented finite-size domains. However, we have discovered that flat substrates with nematic order can induce global nematic alignment of dense, spindle-like cells, thereby influencing cell organization and collective motion and driving alignment on the scale of the entire tissue. Remarkably, single cells are not sensitive to the substrate's anisotropy. Rather, the emergence of global nematic order is a collective phenomenon that requires both steric effects and molecular-scale anisotropy of the substrate. To quantify the rich set of behaviours afforded by this system, we analyse velocity, positional and orientational correlations for several thousand cells over days. The establishment of global order is facilitated by enhanced cell division along the substrate's nematic axis, and associated extensile stresses that restructure the cells' actomyosin networks. Our work provides a new understanding of the dynamics of cellular remodelling and organization among weakly interacting cells.

Defect self-propulsion in active nematic films with spatially varying activity.

We study the dynamics of topological defects in active nematic films with spatially varying activity and consider two set-ups: (i) a constant activity gradient and (ii) a sharp jump in activity. A constant gradient of extensile (contractile) activity endows the comet-like +1/2 defect with a finite vorticity that drives the defect to align its nose in the direction of decreasing (increasing) gradient. A constant gradient does not, however, affect the known self-propulsion of the +1/2 defect and has no effect on the -1/2 that remains a non-motile particle. A sharp jump in activity acts like a wall that traps the defects, affecting the translational and rotational motion of both charges. The +1/2 defect slows down as it approaches the interface and the net vorticity tends to reorient the defect polarization so that it becomes perpendicular to the interface. The -1/2 defect acquires a self-propulsion towards the activity interface, while the vorticity-induced active torque tends to align the defect to a preferred orientation. This effective attraction of the negative defects to the wall is consistent with the observation of an accumulation of negative topological charge at both active/passive interfaces and physical boundaries.

Crisscross multilayering of cell sheets.

Hydrostatic skeletons such as the Hydra's consist of two stacked layers of muscle cells perpendicularly oriented. In vivo, these bilayers first assemble, and then the muscle fibers of both layers develop and organize with this crisscross orientation. In the present work, we identify an alternative mechanism of crisscross bilayering of myoblasts in vitro, which results from the prior local organization of these active cells in the initial monolayer. The myoblast sheet can be described as a contractile active nematic in which, as expected, most of the +1/2 topological defects associated with this nematic order self-propel. However, as a result of the production of extracellular matrix (ECM) by the cells, a subpopulation of these comet-like defects does not show any self-propulsion. Perpendicular bilayering occurs at these stationary defects. Cells located at the head of these defects converge toward their core where they accumulate until they start migrating on top of the tail of the first layer, while the tail cells migrate in the opposite direction under the head. Since the cells keep their initial orientations, the two stacked layers end up perpendicularly oriented. This concerted process leading to a crisscross bilayering is mediated by the secretion of ECM.

Collective rotational motion of freely expanding T84 epithelial cell colonies.

Coordinated rotational motion is an intriguing, yet still elusive mode of collective cell migration, which is relevant in pathological and morphogenetic processes. Most of the studies on this topic have been carried out on epithelial cells plated on micropatterned substrates, where cell motion is confined in regions of well-defined shapes coated with extracellular matrix adhesive proteins. The driver of collective rotation in such conditions has not been clearly elucidated, although it has been speculated that spatial confinement can play an essential role in triggering cell rotation. Here, we study the growth of epithelial cell colonies freely expanding (i.e. with no physical constraints) on the surface of cell culture plates and focus on collective cell rotation in such conditions, a case which has received scarce attention in the literature. One of the main findings of our work is that coordinated cell rotation spontaneously occurs in cell clusters in the free growth regime, thus implying that cell confinement is not necessary to elicit collective rotation as previously suggested. The extent of collective rotation was size and shape dependent: a highly coordinated disc-like rotation was found in small cell clusters with a round shape, while collective rotation was suppressed in large irregular cell clusters generated by merging of different clusters in the course of their growth. The angular motion was persistent in the same direction, although clockwise and anticlockwise rotations were equally likely to occur among different cell clusters. Radial cell velocity was quite low as compared to the angular velocity, in agreement with the free expansion regime where cluster growth is essentially governed by cell proliferation. A clear difference in morphology was observed between cells at the periphery and the ones in the core of the clusters, the former being more elongated and spread out as compared to the latter. Overall, our results, to our knowledge, provide the first quantitative and systematic evidence that coordinated cell rotation does not require a spatial confinement and occurs spontaneously in freely expanding epithelial cell colonies, possibly as a mechanism for the system.

Tilt-induced polar order and topological defects in growing bacterial populations.

Rod-shaped bacteria, such as Escherichia coli, commonly live forming mounded colonies. They initially grow two-dimensionally on a surface and finally achieve three-dimensional growth. While it was recently reported that three-dimensional growth is promoted by topological defects of winding number +1/2 in populations of motile bacteria, how cellular alignment plays a role in nonmotile cases is largely unknown. Here, we investigate the relevance of topological defects in colony formation processes of nonmotile E. coli populations, and found that both ±1/2 topological defects contribute to the three-dimensional growth. Analyzing the cell flow in the bottom layer of the colony, we observe that +1/2 defects attract cells and -1/2 defects repel cells, in agreement with previous studies on motile cells, in the initial stage of the colony growth. However, later, cells gradually flow toward -1/2 defects as well, exhibiting a sharp contrast to the existing knowledge. By investigating three-dimensional cell orientations by confocal microscopy, we find that vertical tilting of cells is promoted near the defects. Crucially, this leads to the emergence of a polar order in the otherwise nematic two-dimensional cell orientation. We extend the theory of active nematics by incorporating this polar order and the vertical tilting, which successfully explains the influx toward -1/2 defects in terms of a polarity-induced force. Our work reveals that three-dimensional cell orientations may result in qualitative changes in properties of active nematics, especially those of topological defects, which may be generically relevant in active matter systems driven by cellular growth instead of self-propulsion.