Curved particles have been shown to stabilize a range of states with unique order in dense suspensions of colloidal bent core liquid crystals. The shape of the colloidal rods encourages the formation of curved director fields. However, states of constant bend cannot uniformly fill either two or three dimensional Euclidean space and are therefore geometrically frustrated. As a result, curved rods are forced to couple their preference for bend with additional twist and splay deformations, giving rise to twist-bend and splay-bend states of nematic and smectic order. In this article, we study the effect of rod curvature on these diverse states of liquid crystalline order using molecular dynamics simulations of a bonded particle model of curved rods with tunable shape elasticity. Focusing on the case of intermediately curved rods, we find that curved rods go through a sequence of isotropic, nematic twist-bend and smectic splay-bend ordering as the density is increased from the dilute limit, in agreement with previous studies of rigid rods. As the rods become more elastic, the critical concentration separating these phases is shifted to higher density. Lastly, we find that flexibility weakens the first-order phase transition separating the isotropic and nematic twist-bend phases.
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.
Using numerical and analytical calculations we study the structure of vacancies and interstitials in two-dimensional colloidal crystals. In particular, we compare the displacement fields of the defect obtained numerically with the predictions of continuum elasticity theory for a simple defect model. In such a comparison it is of crucial importance to employ corresponding boundary conditions both in the particle and in the continuum calculations. Here, we formulate the continuum problem in a way that makes it analogous to the electrostatics problem of finding the potential of a point charge in …
The flow of colloidal suspensions is ubiquitous in nature and industry. Colloidal suspensions exhibit a wide range of rheological behavior, which should be closely related to the microscopic structure of the systems. With in-situ small-angle neutron scattering complemented by rheological measurements, we investigated the deformation behavior of a charge-stabilized colloidal glass at particle level undergoing steady shear. A short-lived, localized elastic response at particle level, termed as transient elasticity zone (TEZ), was identified from the neutron spectra. The existence of the TEZ is a…
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 physical mechanism of elasticity of liquid surfaces coated with colloidal particles is proposed. It is suggested that particles are separated by water clearings and the capillary interaction between them is negligible. The case is treated when the colloidal layer is deformed normally to its surface. The elasticity arises as an interfacial effect. The effective Young modulus of a surface depends on the interfacial tension, equilibrium contact angle, radius of colloidal particles and their surface density. For the nanometrically scaled particles the line tension becomes essential and has an …
We consider the theory of fluctuations of a colloidal solid observed in a confocal slice. For a cubic crystal we study the evolution of the projected elastic properties as a function of the anisotropy of the crystal using numerical methods based on the fast Fourier transform. In certain situations of high symmetry we find exact analytic results for the projected fluctuations.
Several recent experiments suggest that sharply bent DNA has a surprisingly high bending flexibility, but the cause of this flexibility is poorly understood. Although excitation of flexible defects can explain these results, whether such excitation can occur with the level of DNA bending in these experiments remains unclear. Intriguingly, the DNA contained preexisting nicks in most of these experiments but whether nicks might play a role in flexibility has never been considered in the interpretation of experimental results. Here, using full-atom molecular dynamics simulations, we show that nic…
The physical gelation of colloids produces elastic structures that are commonly used to stabilize complex fluids in multiple industries. However, the ability to control the level of elastic modulus of these materials is limited by the universality of the arrested spinodal decomposition mechanism that governs their formation. We demonstrate that manipulating particle shape can yield very large shifts in gel elasticity relative to this universal behavior, and that these changes are generated by a set of independent mechanisms that act multiplicatively. Modeling demonstrates that this efficient g…
Rheological measurements of model colloidal gels reveal that large variations in the shear moduli as colloidal volume-fraction changes are not reflected by simple structural parameters such as the coordination number, which remains almost a constant. We resolve this apparent contradiction by conducting a normal mode analysis of experimentally measured bond networks of the gels. We find that structural heterogeneity of the gels, which leads to floppy modes and a nonaffine-affine crossover as frequency increases, evolves as a function of the volume fraction and is key to understand the frequency…
We theoretically study the effect of external deformation on activated structural relaxation and elementary aspects of the nonlinear mechanical response of glassy hard sphere fluids in the context of the nonequilibrium version of the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory. ECNLE theory describes activated relaxation as a coupled local-nonlocal event involving local caging and longer range collective elasticity, with the latter becoming more important with increasing packing fraction. The central new question is how this physical picture, and the relative importance o…
We propose a microscopic picture for understanding the nonlinear rheology of supercooled liquids with soft-repulsive potentials. Based on Brownian dynamics simulations of supercooled charge-stabilized colloidal suspensions, our analysis shows that the shear thinning of viscosity (eta) at large enough shear rates (sr), expressed as eta~sr^(-lambda), originates from the evolution of the localized elastic region (LER). An LER is a transient region composed of the first several coordination shells of a reference particle. In response to the external shear, particles within LER undergo nearly affin…
Attractive colloidal gels exhibit solid-like behavior at vanishingly small fractions of solids, owing to ramified space-spanning networks that form due to particle-particle interactions. These networks give the gel its rigidity, and as the attraction between the particles grows, so does the elasticity of the colloidal network formed. The emergence of this rigidity can be described through a mean field approach; nonetheless, fundamental understanding of how rigidity varies in gels of different attraction strengths is lacking. Moreover, recovering an accurate gelation phase diagram based on the …
Colloidal rods immersed in a thermotropic liquid-crystalline solvent are at the basis of so-called hybrid liquid crystals which are characterized by tunable nematic fluidity with symmetries ranging from conventional uniaxial nematic or anti-nematic to orthorhombic [Mundoor et al., Science 360, 768 (2018)]. We provide a theoretical analysis of the elastic moduli of such systems by considering interactions between the individual rods with the embedding solvent through surface-anchoring forces, as well as steric and electrostatic interactions between the rods themselves. For uniaxial systems the …
Colloidal gels are out of equilibrium soft solids composed of attractive Brownian particles that form a space-spanning network at low volume fractions. The elastic properties of these systems result from the network microstructure, which is very sensitive to shear history. Here, we take advantage of such sensitivity to tune the viscoelastic properties of a colloidal gel made of carbon black nanoparticles. Starting from a fluidized state under an applied shear rate $\dot γ_0$, we use an abrupt flow cessation to trigger a liquid-to-solid transition. We observe that the resulting gel is all the m…
A general Monte Carlo simulation method of calculating the elastic constants of polydisperse hard-sphere colloidal crystal was developed. The elastic constants of a size polydisperse hard sphere fcc crystal is calculated. The pressure and three elastic constants(C11, C12 and C44) increase significantly with the polydispersity. It was also found from extrapolation that there is a mechanical terminal polydispersity above which a fcc crystal will be mechanically unstable.
We report studies of the frequency dependent shear modulus, $G^*(ω)=G'(ω)+iG''(ω)$, of the liquid crystal octylcyanobiphenyl (8CB) confined in a colloidal aerosil gel. With the onset of smectic order, $G'$ grows approximately linearly with decreasing temperature, reaching values that exceed by more than three orders of magnitude the values for pure 8CB. The modulus at low temperatures possesses a power-law component, $G^*(ω) \sim ω^α$, with exponent $α$ that approaches zero with increasing gel density. The amplitude of $G'$ and its variation with temperature and gel density indicate that the l…
By mapping the interactions of colloidal particles onto the problem of minimizing areas, the physics of foams can be used to understand the phase diagrams of both charged and fuzzy colloids. We extend this analogy to study the elastic properties of such colloidal crystals and consider the face-centered cubic, body-centered cubic and A15 lattices. We discuss two types of soft interparticle potentials corresponding to charged and fuzzy colloids, respectively, and we analyze the dependence of the elastic constants on density as well as on the parameters of the potential. We show that the bulk mod…
Point defects such as interstitials, vacancies, and impurities in otherwise perfect crystals induce complex displacement fields that are of long-range nature. In the present paper we study numerically the response of a two-dimensional colloidal crystal on a triangular lattice to the introduction of an interstitial particle. While far from the defect position the resulting displacement field is accurately described by linear elasticity theory, lattice effects dominate in the vicinity of the defect. In comparing the results of particle based simulations with continuum theory, it is crucial to em…
Resonant x-ray scattering shows that the bulk structure of the twist-bend liquid crystal phase, recently discovered in bent molecular dimers, has spatial periodicity without electron density modulation, indicating a lattice-free heliconical nematic precession of orientation that has helical glide symmetry. In situ study of the bulk helix texture for the dimer CB7CB shows an elastically-confined temperature-dependent minimum helix pitch, but a remarkable elastic softness of pitch in response to dilative stresses. Scattering from the helix is not detectable in the higher temperature nematic phas…
The progress of realizing colloidal structures mimicking natural forms of organization in condensed matter is inherently limited by the availability of suitable colloidal building blocks. To enable new forms of crystalline and quasicrystalline self-organization of colloids, we develop truncated pyramidal particles that form nematic elastic dipoles with long-range electrostaticlike and geometry-guided low-symmetry short-range interactions. Using a combination of nonlinear optical imaging, laser tweezers, and video microscopy, we characterize colloidal pair interactions and demonstrate unusual f…
In titration experiments with NaOH we have determined the full phase diagram of charged colloidal spheres in dependence on the particle density n, the particle effective charge Zeff and the concentration of screening electrolyte c using microscopy, light and Ultra Small Angle X-Ray Scattering (USAXS). For sufficiently large n the system crystallizes upon increasing Zeff at constant c and melts upon increasing c at only slightly altered Zeff. In contrast to earlier work equilibrium phase boundaries are consistent with a universal melting line prediction from computer simulation, if the elastici…
Colloidal particles at complex fluid interfaces and within films assemble to form ordered structures with high degrees of symmetry via interactions that include capillarity, elasticity, and other fields like electrostatic charge. Here we study microparticle interactions within free-standing smectic-A films, in which the elasticity arising from the director field distortion and capillary interactions arising from interface deformation compete to direct the assembly of motile particles. New colloidal assemblies and patterns, ranging from 1D chains to 2D aggregates, sensitive to the initial wetti…
Using self-consistent field and density-functional theories, we first investigate colloidal self-assembling of colloid/polymer films confined between two soft surfaces grafted by polymers. With the increase of colloidal concentrations, the film undergoes a series of transitions from disordered liquid $\to$ sparse square $\to$ hexagonal (or mixed square-hexagonal) $\to$ dense square $\to$ cylindric structures in plane, which results from the competition between the entropic elasticity of polymer brushes and the steric packing effect of colloidal particles. A phase diagram displays the stable re…
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…
We demonstrate a novel method of introducing point defects (mono and di-vacancies) in a confined mono-layer colloidal crystal by manipulating individual particles with optical tweezers. Digital video microscopy is used to study defect dynamics in real space and time. We analyze the topological arrangements of the particles in the defect core and establish their connection with the energetics of the system. It is found that thermal fluctuations excite point defects into \textit{dislocation multipole} configurations. We extract the dislocation pair potential at near field, where cores overlap an…
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 …
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 micron 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…
In the presence of a non-adsorbing polymer, monodisperse rod-like particles assemble into colloidal membranes, which are one rod-length thick liquid-like monolayers of aligned rods. Unlike 3D edgeless bilayer vesicles, colloidal monolayer membranes form open structures with an exposed edge, thus presenting an opportunity to study physics of thin elastic sheets. Membranes assembled from single-component chiral rods form flat disks with uniform edge twist. In comparison, membranes comprised of mixture of rods with opposite chiralities can have the edge twist of either handedness. In this limit d…
We study mutual alignment and interactions between colloidal particles of dissimilar shapes and dimensions when dispersed in a nematic host fluid. Convex pentagonal and concave starfruit-shaped nanoprisms and microspheres induce dipolar or quadrupolar director structures. The ensuing elastic pair interactions between microspheres and nanoprisms are highly dependent on the nanoparticle shape being omnidirectionally attractive for convex prisms but strongly anisotropic for concave prisms. Elastic deformations due to spherical particles cause well-defined alignment of complex-shaped nanoparticles…
Atomic Force Microscopy (AFM) has a great potential as a tool to characterize mechanical and morphological properties of living cells; these properties have been shown to correlate with cells' fate and patho-physiological state in view of the development of novel early-diagnostic strategies. Although several reports have described experimental and technical approaches for the characterization of cell elasticity by means of AFM, a robust and commonly accepted methodology is still lacking. Here we show that micrometric spherical probes (also known as colloidal probes) are well suited for perform…
We investigate the response of colloidal flocks to external fields. We first show that individual colloidal rollers align with external flows as would a classical spin with magnetic fields. Assembling polar active liquids from colloidal rollers, we experimentally demonstrate their hysteretic response: confined colloidal flocks can proceed against external flows. We theoretically explain this collective robustness, using an active hydrodynamic description, and show how orientational elasticity and confinement protect the direction of collective motion. Finally, we exploit the intrinsic bistabil…
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…
Colloidal particles disturb the alignment of rod-like molecules of liquid crystals, giving rise to long-range interactions that minimize the free energy of distorted regions. Particle shape and topology are known to guide this self-assembly process. However, how chirality of colloidal inclusions affects these long-range interactions is unclear. Here we study the effects of distortions caused by chiral springs and helices on the colloidal self-organization in a nematic liquid crystal using laser tweezers, particle tracking and optical imaging. We show that chirality of colloidal particles inter…
We show how including attraction in interparticle interactions reverses the effect of fluctuations in ordering of a prototypical artificial frustrated system. Buckled colloidal monolayers exhibit the same ground state as the Ising antiferromagnet on a deformable triangular lattice, but it is unclear if ordering in the two systems is driven by the same geometric mechanism. By a real-space expansion we find that for buckled colloids bent stripes constitute the stable phase, whereas in the Ising antiferromagnet straight stripes are favored. For generic pair potentials we show that attraction gove…
We present an elastic model of B-form DNA as a stack of thin, rigid plates or base pairs that are not permitted to deform. The symmetry of DNA and the constraint of plate rigidity limit the number of bulk elastic constants contributing to a macroscopic elasticity theory of DNA to four. We derive an effective twist-stretch energy in terms of the macroscopic stretch epsilon along and relative excess twist sigma about the DNA molecular axis. In addition to the bulk stretch and twist moduli found previously, we obtain a twist-stretch modulus with the following remarkable properties: 1) it vanishes…
Macroscopic elastic core-shell systems can be generated as toy models to be deformed and haptically studied by hand. On the mesoscale, colloidal core-shell particles and microgels are fabricated and investigated by different types of microscopy. We analyse, using linear elasticity theory, the response of spherical core-shell systems under the influence of a line density of force that is oriented radially and acts along the equator of the outer surface. Interestingly, deformational coupling of the shell to the core can determine the resulting overall appearance in response to the forces. We add…
Tensegrity structures are special architectures made by floating compressed struts kept together by a continuous system of tensed cables. The multiplicity of shapes that tensegrity structures can assume and their intrinsic capability to be deployable and assembled, so storing (and releasing) elastic energy, have motivated their success as paradigm -pioneeringly proposed by Donald E. Ingber- to explain some underlying mechanisms regulating dynamics of living cells. The interlaced structure of the cell cytoskeleton, constituted by actin and intermediate filaments and microtubules which continuou…
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…
The observation recently of 12-fold quasicrystals in polymers, nanoparticle mixture and 12-fold and 18-fold quasicrystals in colloidal solutions are important events for the study of quasicrystals. To describe the mechanical behaviour we propose a new solid-liquid phase quasicrystal model for some soft matters including polymers and colloids. The so-called new solid-liquid phase, is a new phase model of anisotropic fluid, but different from liquid crystal phase, here the structure presents quasiperiodic symmetry. Based on the model, the elasticity, fluidity and viscosity of the material have b…
Colloidal particles in liquid crystals tend to induce topological defects and distortions of the molecular alignment within the surrounding anisotropic host medium, which results in elasticity-mediated interactions not accessible to their counterparts within isotropic fluid hosts. Such particle-induced coronae of perturbed nematic order are highly responsive to external electric fields, even when the uniformly aligned host medium away from particles exhibits no response to fields below the realignment threshold. Here we harness the non-reciprocal nature of these facile electric responses to de…
Amorphous solids, such as glasses, have complex responses to deformations, with significant consequences in material design and applications. In this respect two intertwined aspects are important: stability and reversibility. It is crucial to understand on the one hand how a glass may become unstable due to increased plasticity under shear deformations; on the other hand, to what extent the response is reversible, meaning how much a system is able to recover the original configuration once the perturbation is released. Here we focus on assemblies of hard spheres as the simplest model of amorph…
A high-resolution calorimetric study has been carried out on nano-colloidal dispersions of aerosils in the liquid crystal 4-\textit{n}-pentylphenylthiol-4'-\textit{n}-octyloxybenzoate ($\bar{8}$S5) as a function of aerosil concentration and temperature spanning the smectic-\textit{C} to nematic phases. Over this temperature range, this liquid crystal possesses two continuous XY phase transitions: a fluctuation dominated nematic to smectic-\textit{A} transition with $α\approx α_{XY} = -0.013$ and a mean-field smectic-\textit{A} to smectic-\textit{C} transition. The effective critical character …
Microbullet particles, cylinders with one blunt and one spherical end, offer a novel platform to study the effects of anisotropy and curvature on colloidal assembly in complex fluids. Here, we disperse microbullets in 4-cyano-4'-pentylbiphenyl (5CB) nematic liquid crystal (NLC) cells and form oriented elastic dipoles with a nematic point defect located near the curved end. This feature allows us to study particle interactions as a function of dipole alignment. By careful control of the surface anchoring at the particle surface and the confining boundaries, we study the interactions and assembl…
