Magnetocontrollable droplet mobility on liquid crystal-infused porous surfaces.

Magnetocontrollable droplet mobility on surfaces of both solids and simple fluids have been widely used in a wide range of applications. However, little is understood about the effect of the magnetic field on the wettability and mobility of droplets on structured fluids. Here, we report the manipulation of the dynamic behaviors of water droplets on a film of thermotropic liquid crystals (LCs). We find that the static wetting behavior and static friction of water droplets on a 4'-octyl-4-biphenylcarbonitrile (8CB) film strongly depend on the LC mesophases, and that a magnetic field caused no measurable change to these properties. However, we find that the droplet dynamics can be affected by a magnetic field as it slides on a nematic 8CB film, but not on isotropic 8CB, and is dependent on both the direction and strength of the magnetic field. By measuring the dynamic friction of a droplet sliding on a nematic 8CB film, we find that a magnetic field alters the internal orientational ordering of the 8CB which in turn affects its viscosity. We support this interpretation with a scaling argument using the LC magnetic coherence length that includes (i) the elastic energy from the long-range orientational ordering of 8CB and (ii) the free energy from the interaction between 8CB and a magnetic field. Overall, these results advance our understanding of droplet mobility on LC films and enable new designs for responsive surfaces that can manipulate the mobility of water droplets. Electronic Supplementary Material: Supplementary material (further details of the stability of LCIPS against water-induced dewetting, the interfacial tension and contact angle measurement using a goniometer, the estimation of the thickness of LC wrapping layer at air-water interface on droplets, SEM measurements, the average sliding velocity of a water droplet on 5CB, E7, silicone oil, and mineral oil films with and without a magnetic field, representative force diagram (Fd versus time) of a 3-µL water droplet moving at a speed of 0.1 mm/s on a nematic 8CB film, Fdynamic acting on 3 µL water droplets moving at speeds of 0.1-1 mm/s on an isotropic 8CB film, the calculated magnetic coherence length as a function of the magnitude of the magnetic field applied to the nematic LCIPS, and the apparent advancing and receding contact angles of a moving water droplet on nematic LCIPS as a function of time, and polarized light micrographs (top view) of a nematic 8CB film between two DMOAP-functionalized glass slides before and after applying a horizontal magnetic field) is available in the online version of this article at 10.1007/s12274-022-5318-y.

Dense packings of geodesic hard ellipses on a sphere.

Packing problems are abundant in nature and have been researched thoroughly both experimentally and in numerical models. In particular, packings of anisotropic, elliptical particles often emerge in models of liquid crystals, colloids, and granular and jammed matter. While most theoretical studies on anisotropic particles have thus far dealt with packings in Euclidean geometry, there are many experimental systems where anisotropically-shaped particles are confined to a curved surface, such as Pickering emulsions stabilized by ellipsoidal particles or protein adsorbates on lipid vesicles. Here, we study random close packing configurations in a two-dimensional model of spherical geodesic ellipses. We focus on the interplay between finite-size effects and curvature that is most prominent at smaller system sizes. We demonstrate that on a spherical surface, monodisperse ellipse packings are inherently disordered, with a non-monotonic dependence of both their packing fraction and the mean contact number on the ellipse aspect ratio, as has also been observed in packings of ellipsoids in both 2D and 3D flat space. We also point out some fundamental differences with previous Euclidean studies and discuss the effects of curvature on our results. Importantly, we show that the underlying spherical surface introduces frustration and results in disordered packing configurations even in systems of monodispersed particles, in contrast to the 2D Euclidean case of ellipse packing. This demonstrates that closed curved surfaces can be effective at introducing disorder in a system and could facilitate the study of monodispersed random packings.

Measure of overlap between two arbitrary ellipses on a sphere.

Various packing problems and simulations of hard and soft interacting particles, such as microscopic models of nematic liquid crystals, reduce to calculations of intersections and pair interactions between ellipsoids. When constrained to a spherical surface, curvature and compactness lead to non-trivial behaviour that finds uses in physics, computer science and geometry. A well-known idealized isotropic example is the Tammes problem of finding optimal non-intersecting packings of equal hard disks. The anisotropic case of elliptic particles remains, on the other hand, comparatively unexplored. We develop an algorithm to detect collisions between ellipses constrained to the two-dimensional surface of a sphere based on a solution of an eigenvalue problem. We investigate and discuss topologically distinct ways two ellipses may touch or intersect on a sphere, and define a contact function that can be used for construction of short- and long-range pair potentials.

From coffee stains to uniform deposits: Significance of the contact-line mobility.

HYPOTHESIS: Contact-line motion upon drying of a sessile droplet strongly affects the solute transport and solvent evaporation profile. Hence, it should have a strong impact on the deposit formation and might be responsible for volcano-like, dome-like and flat deposit morphologies. EXPERIMENTS: A method based on a thin-film interference was used to track the drop height profile and contact line motion during the drying. A diverse set of drying scenarios was obtained by using inks with different solvent compositions and by adjusting the substrate wetting properties. The experimental data was compared to the predictions of a phenomenological model. FINDINGS: We highlight the essential role of contact-line mobility on the deposit morphology of solution-based inks. A pinned contact line produces exclusively ring-like deposits under normal conditions. On the contrary, drops with a mobile contact line can produce ring-, flat- or dome-like morphology. The developed phenomenological model shows that the deposit morphology depends on solvent evaporation profile, evolution of the drop radius relative to its contact angle, and the ratio between initial and maximal (gelling) solute concentration. These parameters can be adjusted by the ink solvent composition and substrate wetting behaviour, which provides a way for deposition of uniform and flat deposits via inkjet printing.

Self-shaping liquid crystal droplets by balancing bulk elasticity and interfacial tension.

The shape diversity and controlled reconfigurability of closed surfaces and filamentous structures, universally found in cellular colonies and living tissues, are challenging to reproduce. Here, we demonstrate a method for the self-shaping of liquid crystal (LC) droplets into anisotropic and three-dimensional superstructures, such as LC fibers, LC helices, and differently shaped LC vesicles. The method is based on two surfactants: one dissolved in the LC dispersed phase and the other in the aqueous continuous phase. We use thermal stimuli to tune the bulk LC elasticity and interfacial energy, thereby transforming an emulsion of polydispersed, spherical nematic droplets into numerous, uniform-diameter fibers with multiple branches and vice versa. Furthermore, when the nematic LC is cooled to the smectic-A LC phase, we produce monodispersed microdroplets with a tunable diameter dictated by the cooling rate. Utilizing this temperature-controlled self-shaping of LCs, we demonstrate life-like smectic LC vesicle structures analogous to the biomembranes in living systems. Our experimental findings are supported by a theoretical model of equilibrium interface shapes. The shape transformation is induced by negative interfacial energy, which promotes a spontaneous increase of the interfacial area at a fixed LC volume. The method was successfully applied to many different LC materials and phases, demonstrating a universal mechanism for shape transformation in complex fluids.

Long-range order in quadrupolar systems on spherical surfaces.

The interplay between curvature, confinement and ordering on curved manifolds, with anisotropic interactions between building blocks, takes a central role in many fields of physics. In this paper, we investigate the effects of lattice symmetry and local positional order on orientational ordering in systems of long-range interacting point quadrupoles on a sphere in the zero temperature limit. Locally triangular spherical lattices show long-range ordered quadrupolar configurations only for specific symmetric lattices as strong geometric frustration prevents general global ordering. Conversely, the ground states on Caspar-Klug lattices are more diverse, with many different symmetries depending on the position of quadrupoles within the fundamental domain. We also show that by constraining the quadrupole tilts with respect to the surface normal, which models interactions with the substrate, and by considering general quadrupole tensors, we can manipulate the ground state configuration symmetry.

Periodic Arrays of Chiral Domains Generated from the Self-Assembly of Micropatterned Achiral Lyotropic Chromonic Liquid Crystal.

Achiral building blocks forming achiral structures is a common occurrence in nature, while chirality emerging spontaneously from an achiral system is usually associated with important scientific phenomena. We report on the spontaneous chiral symmetry-breaking phenomena upon the topographic confinement of achiral lyotropic chromonic liquid crystals in periodically arranged micrometer scale air pillars. The anisotropic fluid arranges into chiral domains that depend on the arrangement and spacing of the pillars. We characterize the resulting domains by polarized optical microscopy, support their reconstruction by numerical calculations, and extend the findings with experiments, which include chiral dopants. Well-controlled and addressed chiral structures will be useful in potential applications like programmable scaffolds for living liquid crystals and as sensors for detecting chirality at the molecular level.

Three-Dimensional Active Defect Loops.

We describe the flows and morphological dynamics of topological defect lines and loops in three-dimensional active nematics and show, using theory and numerical modeling, that they are governed by the local profile of the orientational order surrounding the defects. Analyzing a continuous span of defect loop profiles, ranging from radial and tangential twist to wedge ±1/2 profiles, we show that the distinct geometries can drive material flow perpendicular or along the local defect loop segment, whose variation around a closed loop can lead to net loop motion, elongation, or compression of shape, or buckling of the loops. We demonstrate a correlation between local curvature and the local orientational profile of the defect loop, indicating dynamic coupling between geometry and topology. To address the general formation of defect loops in three dimensions, we show their creation via bend instability from different initial elastic distortions.

Microfluidic control over topological states in channel-confined nematic flows.

Compared to isotropic liquids, orientational order of nematic liquid crystals makes their rheological properties more involved, and thus requires fine control of the flow parameters to govern the orientational patterns. In microfluidic channels with perpendicular surface alignment, nematics discontinuously transition from perpendicular structure at low flow rates to flow-aligned structure at high flow rates. Here we show how precise tuning of the driving pressure can be used to stabilize and manipulate a previously unresearched topologically protected chiral intermediate state which arises before the homeotropic to flow-aligned transition. We characterize the mechanisms underlying the transition and construct a phenomenological model to describe the critical behaviour and the phase diagram of the observed chiral flow state, and evaluate the effect of a forced symmetry breaking by introduction of a chiral dopant. Finally, we induce transitions on demand through channel geometry, application of laser tweezers, and careful control of the flow rate.

Spotting plants' microfilament morphologies and nanostructures.

The tracheary system of plant leaves is composed of a cellulose skeleton with diverse hierarchical structures. It is built of polygonally bent helical microfilaments of cellulose-based nanostructures coated by different layers, which provide them high compression resistance, elasticity, and roughness. Their function includes the transport of water and nutrients from the roots to the leaves. Unveiling details about local interactions of tracheary elements with surrounding material, which varies between plants due to adaptation to different environments, is crucial for understanding ascending fluid transport and for tracheary mechanical strength relevant to potential applications. Here we show that plant tracheary microfilaments, collected from Agapanthus africanus and Ornithogalum thyrsoides leaves, have different surface morphologies, revealed by nematic liquid crystal droplets. This results in diverse interactions among microfilaments and with the environment; the differences translate to diverse mechanical properties of entangled microfilaments and their potential applications. The presented study also introduces routes for accurate characterization of plants' microfilaments.

Spherical structure factor and classification of hyperuniformity on the sphere.

Understanding how particles are arranged on the surface of a sphere is not only central to numerous physical, biological, soft matter, and materials systems but also finds applications in computational problems, approximation theory, and analysis of geophysical and meteorological measurements. Objects that lie on a sphere experience constraints that are not present in Euclidean (flat) space and that influence both how the particles can be arranged as well as their statistical properties. These constraints, coupled with the curved geometry, require a careful extension of quantities used for the analysis of particle distributions in Euclidean space to distributions confined to the surface of a sphere. Here, we introduce a framework designed to analyze and classify structural order and disorder in particle distributions constrained to the sphere. The classification is based on the concept of hyperuniformity, which was first introduced 15 years ago and since then studied extensively in Euclidean space, yet has only very recently been considered also for spherical surfaces. We employ a generalization of the structure factor on the sphere, related to the power spectrum of the corresponding multipole expansion of particle density distribution. The spherical structure factor is then shown to couple with cap number variance, a measure of density variations at different scales, allowing us to analytically derive different forms of the variance pertaining to different types of distributions. Based on these forms, we construct a classification of hyperuniformity for scale-free particle distributions on the sphere and show how it can be extended to include other distribution types as well. We demonstrate that hyperuniformity on the sphere can be defined either through a vanishing spherical structure factor at low multipole numbers or through a scaling of the cap number variance-in both cases extending the Euclidean definition, while at the same time pointing out crucial differences. Our work thus provides a comprehensive tool for detecting global, long-range order on spheres and for the analysis of spherical computational meshes, biological and synthetic spherical assemblies, and ordering phase transitions in spherically distributed particles.

Sculpting stable structures in pure liquids.

Pure liquids in thermodynamic equilibrium are structurally homogeneous. In liquid crystals, flow and light pulses are used to create reconfigurable domains with polar order. Moreover, through careful engineering of concerted microfluidic flows and localized optothermal fields, it is possible to achieve complete control over the nucleation, growth, and shape of such domains. Experiments, theory, and simulations indicate that the resulting structures can be stabilized indefinitely, provided the liquids are maintained in a controlled nonequilibrium state. The resulting sculpted liquids could find applications in microfluidic devices for selective encapsulation of solutes and particles into optically active compartments that interact with external stimuli.

Orientation, elastic interaction and magnetic response of asymmetric colloids in a nematic liquid crystal.

Colloidal particles in nematic liquid crystals create elastic distortion and experience long-range forces. The symmetry of elastic distortion and consequently the complexity of interaction strongly depends largely on the liquid crystal anchoring, topology and shape of the particles. Here, we introduce a new nematic colloidal system made of peanut-shaped hematite particles. We report experimental studies on spontaneous orientation, mutual interaction, laser assisted self-assembly and the effect of external magnetic fields on the colloids. Majority of the colloids spontaneously orient either parallel or perpendicular to the nematic director. The colloids that are oriented perpendicularly exhibit two types of textures due to the out of plane tilting, which is corroborated by the Landau-de Gennes Q-tensor modelling. The transverse magnetic moment of the peanut-shaped colloids is estimated by using a simple analysis based on the competing effects of magnetic and elastic torques.

Mosaics of topological defects in micropatterned liquid crystal textures.

Topological defects in the orientational order that appear in thin slabs of a nematic liquid crystal, as seen in the standard schlieren texture, behave as a random quasi-two-dimensional system with strong optical birefringence. We present an approach to creating and controlling the defects using air pillars, trapped by micropatterned holes in the silicon substrate. The defects are stabilized and positioned by the arrayed air pillars into regular two-dimensional lattices. We explore the effects of hole shape, lattice symmetry, and surface treatment on the resulting lattices of defects and explain their arrangements by application of topological rules. Last, we show the formation of detailed kaleidoscopic textures after the system is cooled down across the nematic-smectic A phase transition, frustrating the defects and surrounding structures with the equal-layer spacing condition of the smectic phase.

Topology-commanded optical properties of bistable electric-field-induced torons in cholesteric bubble domains.

Nowadays, complicated topological defects enable many experimental manipulations and configurational simulations of active soft matter for optical and photonic applications. Investigation of topological defects in soft anisotropic materials enables one to better understand three-dimensional orientation fields in cholesteric liquid crystals. Here, we describe optical properties of bistable bubble domain (BD) texture torons in a thin layer of cholesteric liquid crystal (CLC), frustrated by homeotropic anchoring conditions, and reliably switchable by a random process. The control of macroscopic optical density and diffraction efficiency of the BD texture is demonstrated by a selection of a confinement ratio of the CLC. Experimentally reconstructed CLC director profile reveals the topology of BD torons allowing consideration of naturally occurring BD texture for applications in optical and photonic devices, which are bistably switchable between active and transparent optical states.

Field-controlled structures in ferromagnetic cholesteric liquid crystals.

One of the advantages of anisotropic soft materials is that their structures and, consequently, their properties can be controlled by moderate external fields. Whereas the control of materials with uniform orientational order is straightforward, manipulation of systems with complex orientational order is challenging. We show that a variety of structures of an interesting liquid material, which combine chiral orientational order with ferromagnetic one, can be controlled by a combination of small magnetic and electric fields. In the suspensions of magnetic nanoplatelets in chiral nematic liquid crystals, the platelet's magnetic moments orient along the orientation of the liquid crystal and, consequently, the material exhibits linear response to small magnetic fields. In the absence of external fields, orientations of the liquid crystal and magnetization have wound structure, which can be either homogeneously helical, disordered, or ordered in complex patterns, depending on the boundary condition at the surfaces and the history of the sample. We demonstrate that by using different combinations of small magnetic and electric fields, it is possible to control reversibly the formation of the structures in a layer of the material. In such a way, different periodic structures can be explored and some of them may be suitable for photonic applications. The material is also a convenient model system to study chiral magnetic structures, because it is a unique liquid analog of a solid helimagnet.

Action of fields on captive disclination loops.

We report on two effects observed in experiments with captive disclination loops on polymeric fibers immersed in nematics and submitted to electric and/or magnetic fields. We show that the magnetic field oblique to a fiber with axial or helicoidal anchoring on its surface induces translation of disclination loops. Fields orthogonal to fibers with helicoidal anchoring make disclination loops rotate around the field direction. In the linear regime of this last chirogyral effect, the angle of rotation is proportional to the helix wave vector and its sense unveils the chirality of the helix. We propose a model explaining the origin and all features of these two effects.

Hidden topological constellations and polyvalent charges in chiral nematic droplets.

Topology has an increasingly important role in the physics of condensed matter, quantum systems, material science, photonics and biology, with spectacular realizations of topological concepts in liquid crystals. Here we report on long-lived hidden topological states in thermally quenched, chiral nematic droplets, formed from string-like, triangular and polyhedral constellations of monovalent and polyvalent singular point defects. These topological defects are regularly packed into a spherical liquid volume and stabilized by the elastic energy barrier due to the helical structure and confinement of the liquid crystal in the micro-sphere. We observe, for the first time, topological three-dimensional point defects of the quantized hedgehog charge q=-2, -3. These higher-charge defects act as ideal polyvalent artificial atoms, binding the defects into polyhedral constellations representing topological molecules.

Hedgehogs in the dowser state.

We show how to easily generate point defects called hedgehogs, in the so-called quasi-planar texture --the dowser state-- of a nematic layer confined between surfaces with homeotropic anchoring conditions. We point out that the dowser texture can be preserved infinitely in spite of its higher energy with respect to the homogeneous homeotropic texture. For topological reasons the dowser state in a squeezed droplet must contain at least one hedgehog. We submitted this hedgehog to a rotating magnetic field and controlled the continuous evolution, transitioning continuously between radial, hyperbolic and circular hedgehogs, which, just as in previous experiments by Lavrentovich et al., are topologically equivalent states. The dynamics of this transformation is shown to be directly sensitive to energy costs of different geometric configurations of the hedgehog defect and therefore can be used as a rough probe for elastic constants; knowing the principal elastic constants K1,2,3, one can retrieve information about the K24 constant. We propose also a method of generation of hedgehog pairs by application of a Poiseuille flow to a dowser state wound by a rotating magnetic field.

Persistent quasiplanar nematic texture: Its properties and topological defects.

In the so-called quasiplanar texture of a nematic layer confined between parallel plates with homeotropic anchoring conditions, the director field rotates by π between limit surfaces so that field lines have the shape of a dowsing Y-shaped wooden tool. The orientation of the director field at midheight of the layer is arbitrary for symmetry reasons and is thus very sensitive to perturbations. We point out that contrary to accepted ideas the quasiplanar texture can be preserved infinitely in spite of its metastability with respect to the homogeneous homeotropic texture. We propose to call such a long-lived version of the quasiplanar texture the dowser texture. We demonstrate both experimentally and theoretically that in samples of variable thickness, the director field is sensitive to the gradient of the sample thickness through a linear coupling term. As a result, it has a tendency to follow the direction of the thickness gradient. Because of its sensitivity to perturbations we propose to call the midplane director field the dowser field and its tendency to follow the thickness gradient cuneitropism. Under effect of the gradient field, the dowser field obeys the sine-Gordon equation and exhibits domain walls that correspond to the well-known solitonic solutions of the sine-Gordon model.