We predict theoretically the existence of a class of colloidal structures in nematic liquid crystal (NLC) cells, which are induced by surface patterns on the plates of the cell (like cells with UV-irradiated polyimide surfaces using micron size masks). These bulk structures arise from non-zero boundary conditions for the director distortions at the confining surfaces. In particular, we demonstrate that quadrupole spherical particles (like spheres with boojums or Saturn-ring director configurations) form a square lattice inside a planar NLC cell, which has checkerboard patterns on both its plates.
Control of physical behaviors of nematic colloids and colloidal crystals has been demonstrated by tuning particle shape, topology, chirality and surface charging. However, the capability of altering physical behaviors of such soft matter systems by changing particle shape and the ensuing responses to external stimuli has remained elusive. We fabricated genus-one nematic elastomeric colloidal ring-shaped particles and various microstructures using two-photon photopolymerization. Nematic ordering within both the nano-printed particle and the surrounding medium leads to anisotropic responses and …
Mixing colloid shapes with distinctly different anisotropy generates composite nematics in which the order of the individual components can be fundamentally different. In colloidal rod-disk mixtures or hybrid nematics composed of anisotropic colloids immersed in a thermotropic liquid crystal, one of the components may adopt so-called anti-nematic order while the other exhibits conventional nematic alignment. Focussing on simple models for hard rods and disks, we employ Onsager-Straley's second-virial theory to derive scaling expressions for the elastic moduli of rods and disks in both nematic …
The assembly of colloids in nematic liquid crystals via topological defects has been extensively studied for spherical particles, and investigations of other colloid shapes have revealed a wide array of new assembly behaviors. We show, using Landau-de Gennes numerical modeling, that nematic defect configurations and colloidal assembly can be strongly influenced by fine details of colloid shape, in particular the presence of sharp edges. For cylinder, microbullet, and cube colloid geometries, we obtain the particles' equilibrium alignment directions and effective pair interaction potentials as …
In an elegant paper, D. Nelson suggested a method to produce tetravalent colloids based on a tetrahedral configuration created on the surface of a spherical particle. It emerges from a two-dimensional nematic liquid crystal placed on a sphere due to the presence of four 1/2 disclinations, i.e., topological defects in the orientational order. In this paper we show that such a tetrahedral configuration also occurs in the wetting layers which form around spheres dispersed in a liquid crystal above the nematic-isotropic phase transition. Nematic wetting therefore offers an alternative route toward…
We propose a simple theoretical model which explains a formation of dipolar 2D and 3D colloidal structures in nematic liquid crystal. Colloidal particles are treated as effective hard spheres interacting via their elastic dipole, quadrupole and octopole moments. It is shown that octopole moment plays an important role in the formation of 2D and 3D nematic colloidal crystals. We generalize this assumption on the case of the external electric field and theoretically explain a giant electrostriction effect in 3D crystals observed recently [A. Nych et al., Nature Communications \textbf{4}, 1489 (2…
Three-body effective interactions emerging between parallel cylindrical rods immersed in a nematic liquid crystals are calculated within the Landau-de Gennes free energy description. Collinear, equilateral and midplane configurations of the three colloidal particles are considered. In the last two cases the effective triplet interaction is of the same magnitude and range as the pair one.
Nematic colloids exhibit a large diversity of topological defects and structures induced by colloidal particles in the orientationally ordered liquid crystal host fluids. These defects and field configurations define elastic interactions and medium-mediated self-assembly, as well as serve as model systems in exploiting the richness of interactions between topologies and geometries of colloidal surfaces, nematic fields, and topological singularities induced by particles in the nematic bulk and at nematic-colloidal interfaces. Here we demonstrate formation of quarter-strength surface-pinned disc…
The Landau-de Gennes free energy is used to study theoretically the interaction of parallel cylindrical colloidal particles trapped at a nematic-isotropic interface. We find that the effective interaction potential is non-monotonic. The corresponding force-distance curves exhibit jumps and hysteresis upon approach/separation due to the creation/annihilation of topological defects. Minimization results suggest a simple empirical pair potential for the effective colloid-colloid interaction at the interface. We propose that the interface-mediated interaction can play an important role in self-org…
Self-assembly of colloidal particles is poised to become a powerful composite material fabrication technique, but remains challenged by a limited control over the ensuing structures. We develop a new breed of nematic colloids that are physical analogs of a mathematical surface with boundary, interacting with the molecular alignment field without inducing defects when flat. However, made from a thin nanofoil, they can be shaped to prompt formation of self-compensating defects that drive pre-programmed elastic interactions mediated by the nematic host. To show this, we wrap the nanofoil on all t…
Using laser tweezers and fluorescence confocal polarizing microscopy, we study colloidal interactions of solid microspheres in the nematic bulk caused by elastic distortions around the particles with strong tangential surface anchoring. The particles aggregate into chains directed at about 30 degrees to the far field director and, at higher concentrations, form complex kinetically trapped structures. We characterize the distance and angular dependencies of the colloidal interaction forces.
The new free energy functional that describes general elastic interaction between colloidal particles and nematic liquid crystal has been proposed. It generalizes results of the paper \cite{lupe} on the case of arbitrary orientation of colloidal particles and is valid for arbitrary surface anchoring strength. Formal analogies and differences between electric particles and colloidal particles in LC are found. It is first time shown that spur of the quadrupole moment tensor is different from zero $Sp\hat{Q}_μ\neq 0$ in the case of axial symmetry breaking of the director field around colloidal pa…
Spherical microparticles dispersed in nematic liquid crystals have been extensively investigated in the past years. Here, we report experimental studies on the elastic deformation, colloidal interaction and self-assembly of hematite microcubes with homeotropic surface anchoring in a nematic liquid crystal. We demonstrate that the colloidal interaction and self-assembly of cubic colloids are orientation dependent. In a notable departure from the conventional microspheres, the microcubes stabilise diverse structures, such as bent chains, branches, kinks and closed-loops. The microcubes reorient …
The elastic and capillary interactions between a pair of colloidal particles trapped on top of a nematic film are studied theoretically for large separations $d$. The elastic interaction is repulsive and of quadrupolar type, varying as $d^{-5}$. For macroscopically thick films, the capillary interaction is likewise repulsive and proportional to $d^{-5}$ as a consequence of mechanical isolation of the system comprised of the colloids and the interface. A finite film thickness introduces a nonvanishing force on the system (exerted by the substrate supporting the film) leading to logarithmically …
Colloids self-assemble into various organized superstructures determined by particle interactions. There is a tremendous progress in both the scientific understanding and applications of self-assemblies of single-type identical particles. Forming superstructures in which the colloidal particles occupy predesigned sites and remain in these sites despite thermal fluctuations represents a major challenge of the current state-of-the art. Here we propose a versatile approach to direct placement of colloids using nematic liquid crystals with spatially varying molecular orientation pre-imposed by sub…
The Landau-de Gennes free energy is used to calculate the interaction between long cylindrical colloids and the nematic-isotropic (NI) interface. This interaction has two contributions: one is specific of liquid crystals and results from the deformation of the director field close to the particles or to the interface, while the other is generic and results from wetting and surface tension effects. Deep in the nematic phase the director field of long cylindrical colloids, with strong homeotropic anchoring, exhibits two half-integer defect lines. As the colloid moves towards the interface, the d…
Using extensive Monte Carlo (MC) simulations of colloids immersed in a nematic liquid crystal we compute an effective interaction potential via the local nematic director field and its associated order parameter. The effective potential consists of a local Landau-de Gennes (LdG) and a Frank elastic contribution. Molecular expressions for the LdG expansion coefficients are obtained via classical density functional theory (DFT). The DFT result for the LdG parameter $A$ is improved by locating the phase transition through finite-size scaling theory. We consider effective interactions between a pa…
We consider the interaction of two-dimensional colloids, in nematic liquid crystals, with walls or geometrical boundaries. The interactions between colloidal disks and flat walls, with homeotropic boundary conditions, are always repulsive. The repulsions may be turned into strong attractions at structured or sculpted walls with cavities, matching closely the shape and size of the colloids. This key-lock type of interaction is analyzed in detail for spherocylindrical cavities of various length to breath ratios, by minimizing the Landau-de Gennes free energy functional of the orientational order…
Self-assembly of nanoparticles can enable composites with pre-designed properties but remains challenged by reproducing structural diversity of atomic and molecular crystals. We combine anisotropic elastic and weakly screened electrostatic interactions to guide both orientational and triclinic positional self-ordering of inorganic nanocrystals in a nematic fluid host. The lattice periodicity of these low-symmetry colloidal crystals is more than an order of magnitude larger than the nanoparticle size. Orientations of nanocrystals, as well as crystallographic axes of ensuing triclinic colloidal …
As recently reported [Turiv T. et al., Science, 2013, Vol. 342, 1351], fluctuations in the orientation of the liquid crystal (LC) director can transfer momentum from the LC to a colloid, such that the diffusion of the colloid becomes anomalous on a short time scale. Using video microscopy and single particle tracking, we investigate random thermal motion of colloidal particles in a nematic liquid crystal for the time scales shorter than the expected time of director fluctuations. At long times, compared to the characteristic time of the nematic director relaxation we observe typical anisotropi…
We demonstrate a novel method to assemble and transport swarms of colloidal particles by combining liquid crystals enabled electrophoresis and photo-sensitive surface patterning. Colloidal particles are propelled in a nematic liquid crystal via application of an alternating current electric field. Swarms of particles are assembled into a rotating mill cluster, or moved as a whole along predefined paths photo-imprinted on chemically functionalized substrates. This technique represents an alternative approach to fluid based lab-on-a-chip technologies guiding the motion of large ensembles of micr…
One of the central experimental efforts in nematic colloids research aims to explore how the interplay between the geometry of particles along with the accompanying nematic director deformations and defects around them can provide a means of guiding particle self-assembly and controlling the structure of particle-induced defects. In this work, we design, fabricate, and disperse low-symmetry colloidal particles with shapes of spirals, double spirals, and triple spirals in a nematic fluid. These spiral-shaped particles, which are controlled by varying their surface functionalization to provide t…
We propose the use of topographic modulation of surfaces to select and localize particles in nematic colloids. By considering convex and concave deformations of one of the confining surfaces we show that the colloid-flat surface repulsion may be enhanced or switched into an attraction. In particular, we find that when the colloidal particles have the same anchoring conditions as the patterned surfaces, they are strongly attracted to concave dimples, while if they exhibit different anchoring conditions they are pinned at the top of convex protrusions. Although dominated by elastic interactions …
We perform Dynamic Monte Carlo simulations to investigate the equilibrium dynamics of hard colloidal cuboids in oblate and prolate nematic liquid crystals. In particular, we characterise the particles' diffusion along the nematic director and perpendicularly to it, and observe a structural relaxation decay that strongly depend on the particle anisotropy. To assess the Gaussianity of their dynamics and eventual occurrence of collective motion, we calculate two- and four-point correlation functions that incorporate the instantaneous values of the diffusion coefficients parallel and perpendicular…
Up to now it is commonly believed that a colloidal particle suspended in a nematic liquid crystal never produces elastic monopoles because this violates the mechanical equilibrium condition. And the only way to obtain deformations of director field falling off with distance as r^{-1} is to exert an external torque Γ_{ext} on the colloid \cite{de_Gennes}. In this paper we demonstrate that this statement is not quite correct and elastic monopoles, as well as dipoles and quadrupoles, can be induced without any external influence just by the particle itself. A behavior of a spherical colloidal par…
We present experiments where anisometric colloidal microparticles dispersed in a nematic liquid crystal cell with homeotropic anchoring conditions are dynamically assembled by means of liquid-crystal-enabled electrophoresis (LCEEP) using an AC electric field perpendicular to the confining plates. A nematic host with negative dielectric anisotropy leads to a driving force parallel to the cell plates. We take advantage of the resulting gliding anchoring conditions and the degeneracy in the direction of particle motion to design reconfigurable trajectories using a photosensitive anchoring layer (…
The ability to dictate colloid motion is an important challenge in fields ranging from materials science to living systems. Here, by embedding energy landscapes in confined nematic liquid crystals, we design a versatile platform to define colloidal migration. This is achieved by placing a wavy wall, with alternating hills and wells, in nematic liquid crystals, to impose a smooth elastic energy field with alternating splay and bend distortions. This domain generates (meta) stable loci that act as attractors and unstable loci that repel colloids over distances large compared to the colloid radiu…
Using molecular dynamics (MD) simulations we study the interactions between elongated colloidal particles (length to breath ratio > 1) in a nematic host. The simulation results are compared to the results of a Landau-de Gennes elastic free energy. We find that depletion forces dominate for the sizes of the colloidal particles studied. The tangential component of the force, however, allows us to resolve the elastic contribution to the total interaction. We find that this contribution differs from the quadrupolar interaction predicted at large separations. The difference is due to the presence o…
We examine the behavior of spherical silica particles trapped at an air-nematic liquid crystal interface. When a strong normal anchoring is imposed, the beads spontaneously form various structures depending on their area density and the nematic thickness. Using optical tweezers, we determine the pair potential and explain the formation of these patterns. The energy profile is discussed in terms of capillary and elastic interactions. Finally, we detail the mechanisms that control the formation of an hexagonal lattice and analyze the role of gravity for curved interfaces.
In the simplest realization of Brownian motion, a colloidal sphere moves randomly in an isotropic fluid; its mean squared displacement (MSD) grows linearly with time $\textitτ$. Brownian motion in an orientationally ordered fluid, a nematic, is anisotropic, with the MSD being larger along the axis of molecular orientation, called the director. We show that at short time scales, the anisotropic diffusion in a nematic becomes also anomalous, with the MSD growing slower (subdiffusion) and faster (superdiffusion) than $\textitτ$. The anomalous diffusion occurs at time scales that correspond to the…
Non-equilibrium dynamics of topological defects can be used as a fundamental propulsion mechanism in microscopic active matter. Here, we demonstrate swimming of topological defect-propelled colloidal particles in (passive) nematic fluids through experiments and numerical simulations. Dynamic swim strokes of the topological defects are driven by colloidal rotation in an external magnetic field, causing periodic defect rearrangement which propels the particles. The swimming velocity is determined by the colloid's angular velocity, sense of rotation and defect polarity. By controlling them we can…
We combine experiments, theory, and simulations to investigate the coexistence of nonequilibrium phases emerging from interacting colloidal particles that are electrokinetically propelled in a nematic liquid crystal solvent. We directly determine the mechanical pressure within the radial assemblies and measure a non-equilibrium equation of state for this athermal driven system. A generic model combines phoretic propulsion with the interplay between electrostatic effects and liquid-crystal-mediated hydrodynamics, which are effectively cast into a long-range interparticle repulsion, while elasti…
Topological defects that form on surfaces of ordered media, dubbed boojums, are ubiquitous in superfluids, liquid crystals (LCs), Langmuir monolayers, and Bose-Einstein condensates. They determine supercurrents in superfluids, impinge on electrooptical switching in polymer-dispersed LCs, and mediate chemical response at nematic-isotropic fluid interfaces, but the role of surface topology in the appearance, stability, and core structure of these defects remains poorly understood. Here, we demonstrate robust generation of boojums by controlling surface topology of colloidal particles that impose…
We present the first systematic measurements of the dynamic response of a glassy soft-solid formed on dispersing colloids in a thermotropic nematic liquid crystal. Through applying a simple theoretical model, we reveal that the nematic elasticity dominates at low frequencies (longest timescales) and prevents flow. The Ericksen number $E_R$, determines a critical frequency $ω_c$, above which the viscous component $G'' \propto ω^{1/2}$. We find that the value of tan$δ$ is independent of the colloidal volume fraction ($ϕ$), and is determined by the ratio of lengthscales associated with the defect…
Placing colloidal particles in predesigned sites represents a major challenge of the current state-of-the-art colloidal science. Nematic liquid crystals with spatially varying director patterns represent a promising approach to achieve a well-controlled placement of colloidal particles thanks to the elastic forces between the particles and the surrounding landscape of molecular orientation. Here we demonstrate how the spatially varying director field can be used to control placement of non-spherical particles of boomerang shape. The boomerang colloids create director distortions of a dipolar s…
The Landau-de Gennes free energy is used to study theoretically the effective interaction of a spherical "key" and an anisotropic "lock" colloidal particles. We assume identical anchoring properties of the surfaces of the key and of the lock particles, and consider planar degenerate and perpendicular anchoring conditions separately. {The lock particle is modeled} as a spherical particle with a spherical dimple. When such a particle is introduced into a nematic liquid crystal, it orients its dimple at an oblique angle $θ_{eq}$ with respect to the far field director ${\bf n}_{\infty}$. This angl…
The behavior of a colloidal suspension of rod-like {\it fd} viruses in the nematic phase, subjected to steady state and transient shear flows is studied. The monodisperse nature of these rods combined with relatively small textural contribution to the overall stress make this a suitable model system to investigate the effects of flow on the non-equilibrium phase diagram. Transient rheological experiments are used to determine the critical shear rates at which director tumbling, wagging and flow-aligning occurs. The present model system enables us to study the effect of rod concentration on the…
The effective interaction between spherical colloids in nematic liquid crystals is investigated in the framework of the Landau-de Gennes theory. The colloids differ through their interaction with the nematic. While both particles induce quadrupolar far-field distortions in the nematic matrix, with unlike quadrupole moments, one favours homeotropic and the other degenerate planar anchoring of the nematic director. In the strong anchoring regime the colloids with homeotropic anchoring are accompanied by an equatorial disclination line defect, known as "Saturn-ring", while the colloids with degen…
We investigated the physical properties of low concentration ferroelectric nematic colloids, using calorimetry, optical methods, infra-red spectroscopy and capacitance studies. The resulting colloids normally remain homogeneous, but the nematic orientational coupling is significantly amplified. In particular cases, the nematic orientation coupling increases by 10% for particle concentrations of 0.2%. A manifestation of the increased orientational order is that the clearing temperature of a nematic colloid increases up to 40 Celsius degrees compared to the pure LC host. A theoretical model is p…
We apply the method developed in Ref. [S.B.Chernyshuk and B.I.Lev, Phys.Rev.E, \textbf{81}, 041701 (2010)] for theoretical investigation of colloidal elastic interactions between axially symmetric particles in the confined nematic liquid crystal (NLC) near one wall and in the nematic cell with thickness $L$. Both cases of homeotropic and planar director orientations are considered. Particularly dipole-dipole, dipole-quadrupole and quadrupole-quadrupole interactions of the \textit{one} particle with the wall and within the nematic cell are found as well as corresponding \textit{two particle} el…
The Green function method developed in Ref.[S. B. Chernyshuk and B. I. Lev, Phys. Rev. E \textbf{81}, 041707 (2010)] is used to describe elastic interactions between axially symmetric colloidal particles in the nematic cell in the presence of the external electric or magnetic field. General formulas for dipole-dipole, dipole-quadrupole and quadrupole-quadrupole interactions in the homeotropic and planar nematic cells with parallel and perpendicular field orientations are obtained. A set of new results has been predicted: 1) \textit{Deconfinement effect} for dipole particles in the homeotropic …
Recent experiments have shown how nematically-ordered tactoid shaped actin droplets can be reorganized and divided by the action of myosin molecular motors. In this paper, we consider how similar morphological changes can potentially be achieved under equilibrium conditions. Using simulations, both atomistic and continuum, and a phenomenological model, we explore how the nucleation dynamics, shape changes, and the final steady state of a nematic tactoid droplet can be modified by interactions with model adhesive colloids that mimic a myosin motor cluster. Our results provide a prescription for…
Biological motors are marvels of nature that inspire creation of their synthetic counterparts with comparable nanoscale dimensions, high efficiency and diverse functions. Molecular motors have been synthesized, but obtaining nanomotors through self-assembly remains challenging. Here we describe a self-assembled colloidal motor with a repetitive light-driven rotation of transparent micro-particles immersed in a liquid crystal and powered by a continuous exposure to unstructured ~1 nW light. A monolayer of azobenzene molecules defines how the liquid crystal's optical axis mechanically couples to…
We calculate the interaction between two spherical colloidal particles embedded in the isotropic phase of a nematogenic liquid. The surface of the particles induces wetting nematic coronas that mediate an elastic interaction. In the weak wetting regime, we obtain exact results for the interaction energy and the texture, showing that defects and biaxiality arise, although they are not topologically required. We evidence rich behaviors, including the possibility of reversible colloidal aggregation and dispersion. Complex anisotropic self-assembled phases might be formed in dense suspensions.
We show that the elastic charge of colloids in a nematic liquid crystal can be generated by the vector of external torque. The torque components play the role of two component charge (dyad) and give rise to the Coulomb-like potential, while their conservation law plays the role similar to that of Gauss' theorem in the electrostatics. The theory is applied to the colloid-surface interaction. A wall with homeotropic or planar director is shown to induce a repulsive 1/r^4 force on the elastic dipole. The external torque, however, induces the elastic charge in this colloid and triggers switching t…
We create controllable active particles in the form of metal-dielectric Janus colloids which acquire motility through a nematic liquid crystal film by transducing the energy of an imposed perpendicular AC electric field. We achieve complete command over trajectories by varying field amplitude and frequency, piloting the colloids at will in the plane spanned by the axes of the particle and the nematic. The underlying mechanism exploits the sensitivity of electro-osmotic flow to the asymmetries of the particle surface and the liquid-crystal defect structure. We present a calculation of the dipol…
Different phoretic driving mechanisms have been proposed for the transport of solid or liquid microscopic inclusions in integrated chemical processes. However, the ability to reversibly address both the flow path, rate, and local reactant concentration has not yet been realized. Here we show that a substrate chemically modified with photosensitive self-assembled monolayers allows to directly command the assembly and transport of large ensembles of micron-size particles and drops dispersed in a thin layer of anisotropic fluid. Our strategy separates particle driving, realized via AC electrophor…
Outermost occupied electron shells of chemical elements can have symmetries resembling that of monopoles, dipoles, quadrupoles and octupoles corresponding to filled s-, p-, d- and forbitals. Theoretically, elements with hexadecapolar outer shells could also exist, but none of the known elements have filled g-orbitals. On the other hand, the research paradigm of "colloidal atoms" displays complexity of particle behaviour exceeding that of atomic counterparts, which is driven by DNA functionalization, geometric shape and topology and weak external stimuli. Here we describe elastic hexadecapoles …
We report an extensive molecular dynamics study on the translational dynamics of a hybrid system composed of dipolar soft spheres (DSS), representing ferromagnetic particles, suspended in a liquid crystal (LC) matrix. We observe that the LC matrix strongly modifies the dynamics of the DSS. In the isotropic regime, the DSS show a crossover from subdiffusive to normal diffusive behavior at long times, with an increase of the subdiffusive regime as the dipolar coupling strength is increased. In the nematic regime, the LC matrix, due to collective reorientation of LC particles, imposes a cylindric…
Physically intelligent micro-robotic systems exploit information embedded in micro-robots, their colloidal cargo, and their milieu to interact, assemble and form functional structures. Nonlinear anisotropic fluids like nematic liquid crystals (NLCs) provide untapped opportunities to embed interactions via their topological defects, complex elastic responses, and their ability to dramatically restructure in dynamic settings. Here we design and fabricate a 4-armed ferromagnetic micro-robot to embed and dynamically reconfigure information in the nematic director field, generating a suite of physi…
Understanding the relaxation dynamics of colloidal suspensions is crucial to identify the elements that influence the mobility of their constituents, assess their macroscopic response across the relevant time and length scales, and thus disclose the fundamentals underpinning their exploitation in formulation engineering. In this work, we specifically assess the impact of long-ranged ordering on the relaxation dynamics of suspensions of soft-repulsive rod-like particles, which are able to self-organise into nematic and smectic liquid-crystalline phases. By performing Dynamic Monte Carlo simulat…
The theory of elastic interaction of micron size axially symmetric colloidal particles immersed into confined nematic liquid crystal has been proposed. General formulas are obtained for the self energy of one colloidal particle and interaction energy between two particles in arbitrary confined NLC with strong anchoring condition on the bounding surface. Particular cases of dipole-dipole interaction in the homeotropic and planar nematic cell with thickness $L$ are considered and found to be exponentially screened on far distances with decay length $λ_{dd}=\frac{L}π$. It is predicted that boundi…
