Nematic Surface Research Articles

Improved Cell Adhesion on Self-Assembled Chiral Nematic Cellulose Nanocrystal Films.

Chirality is ubiquitous in nature, and closely related to biological phenomena. Nature-originated nanomaterials such as cellulose nanocrystals (CNCs) are able to self-assemble into hierarchical chiral nematic CNC films and impart handedness to nano and micro scale. However, the effects of the chiral nematic surfaces on cell adhesion are still unknown. Herein, this work presents evidence that the left-handed self-assembled chiral nematic CNC films (L-CNC) significantly improve the adhesion of L929 fibroblasts compared to randomly arranged isotropic CNC films (I-CNC). The fluidic force microscopy-based single-cell force spectroscopy is introduced to assess the cell adhesion forces on the substrates of L-CNC and I-CNC, respectively. With this method, a maximum adhesion force of 133.2 nN is quantified for mature L929 fibroblasts after culturing for 24h on L-CNC, whereas the L929 fibroblasts exert a maximum adhesion force of 78.4 nN on I-CNC under the same condition. Moreover, the instant SCFS reveals that the integrin pathways are involved in sensing the chirality of substrate surfaces. Overall, this work offers a starting point for the regulation of cell adhesion via the self-assembled nano and micro architecture of chiral nematic CNC films, with potential practical applications in tissue engineering and regenerative medicine.

Effect of a surface polarized layer on the optical properties of a nematic cell

The optical properties of a cell of nematic liquid crystal presenting a tilted surface polarization submitted to an electric field are theoretically investigated. The origin of the surface polarization is assumed to be related to the interaction of the nematic molecules with the substrate and to the polar order due to the cell filling procedure. The analysis shows that the coupling of the surface polarization with the external field has different effects on the two surfaces limiting the sample. On one of them, the coupling gives rise, in an unbounded sample, to a continuous variation of the easy angle, whereas on the other one it is responsible for a first-order like transition of the easy axis orientation. For a sample of finite thickness our analysis shows that in the presence of a coupling between the two surfaces, operated by the elastic properties of the liquid crystal, the abrupt variation of the easy axis on one of the surfaces induces also on the other surface a discontinuity on the nematic surface orientation. The optical transmission of the cell versus the amplitude of the applied voltage, for an impinging monochromatic linearly polarized light, presents a discontinuity for the critical voltage at which the first-order transition of the surface tilt angles appears.

Continuum theory of a nematic liquid crystal with a nonideal physical surface and the surfacelike elasticity

ABSTRACT The nematic surface violates the translational symmetry of unrestricted medium and induces novel elastic effects. An ideal surface, where the nematic order parameter and density vanish abruptly, induces the surface elastic term that cancels out the Nehring-Saupe divergence term. A more realistic, nonideal surface is represented by a thin layer where the order parameter and density smoothly vary from their bulk values to zero. This surface is shown to induce additional contributions to the effective surface elastic and terms. These terms are no longer total divergences which is employed to incorporate them in the elastic theory. It is shown how the higher order elasticity and the finite surface layer provide the lower free energy bound both for nonzero term and for term violating Ericksen’s stability condition for the uniform director ground state. The effective boundary condition and procedure of the free energy minimisation for arbitrary and are derived. It is shown how Ericksen’s condition is modified by the presence of the term, anchoring, and spatial boundedness. An example of the surfacelike-elasticity-induced spontaneous modulations of the uniform director ground state is presented.

Theory of nematic and polar active fluid surfaces

We derive a fully covariant theory of the hydrodynamics of nematic and polar active surfaces, subjected to internal and external forces and torques. We study the symmetries of polar and nematic surfaces and find that in addition to 5 different types of in-plane isotropic surfaces, polar and nematic surfaces can be classified into 5 polar, 2 pseudopolar, 5 nematic and 2 pseudonematic types of surfaces. We give examples of physical realisations of the different types of surfaces we have identified. We obtain expressions for the equilibrium tensions, moments, and external forces and torques acting on a passive polar or nematic surface. We calculate the entropy production rate using the framework of thermodynamics close to equilibrium and find constitutive equations for polar and nematic active surfaces with different symmetries. We study the instabilities of a confined flat planar-chiral polar active layer and of a confined deformable polar active surface with broken up-down symmetry.

Intrinsic nature of chiral charge order in the kagome superconductor RbV3Sb5

Superconductors with kagome lattices have been identified for over 40 years, with a superconducting transition temperature TC up to 7K. Recently, certain kagome superconductors have been found to exhibit an exotic charge order, which intertwines with superconductivity and persists to a temperature being one order of magnitude higher than TC. In this work, we use scanning tunneling microscopy (STM) to study the charge order in kagome superconductor RbV3Sb5. We observe both a 2x2 chiral charge order and nematic surface superlattices (predominantly 1x4). We find that the 2x2 charge order exhibits intrinsic chirality with magnetic field tunability. Defects can scatter electrons to introduce standing waves, which couple with the charge order to cause extrinsic effects. While the chiral charge order resembles that discovered in KV3Sb5, it further interacts with the nematic surface superlattices that are absent in KV3Sb5 but exist in CsV3Sb5.

Liquid Crystal Films as Active Substrates for Nanoparticle Control

Organizing nanoparticles in a controlled way allows us to monitor their optical properties. It is particularly interesting to organize them on top of liquid crystal films to take advantage, in a second step, of the easy actuation of liquid crystals with external parameters such as temperature, electric fields, and so forth. We show that despite their fluidity, nematic and smectic films allow the formation of well-ordered hexagonal domains of gold spherical nanoparticles (AuNPs) at their surface, but we also show that both nematic films and AuNP domains impact each other. Using optical microscopy, atomic force microscopy (AFM), scanning electron microscopy (SEM), and spectrophotometry, we compare nematic, polymer-stabilized nematic, and smectic films with AuNP domains made of NPs of diameter 6 nm. On the liquid crystal films, depressions are revealed below the AuNP domains, whereas the AuNP domains appear well-organized but with a hexagonal period shortened with respect to AuNP monolayers formed on hard substrates. We interpret these features by the anchoring tilt imposed by the AuNP domains on the liquid crystal molecules. The smectic-A layers characteristic of the nematic surface transform into smectic-C layers, which induce the formation of depression. The energy penalty associated with the local smectic-A/smectic-C transition induces the shortening of the AuNP domain period in order to decrease the AuNP domain surface. The observed large depth of the polymer-stabilized nematic depressions below AuNP domains may be explained either by an increased size of the polymer-stabilized smectic layers close to the surface or by an increased number of polymer-stabilized smectic liquid crystal smectic layers close to the surface with respect to pure nematic films.

Thickness Induced Line-Defect Reconfigurations in Thin Nematic Cell

We studied the impact of the cell thickness on configurations of line disclinations within a plane-parallel nematic cell. The Lebwohl-Lasher semimicroscopic approach was used and (meta)stable nematic configurations were calculated using Brownian molecular dynamics. Defect patterns were enforced topologically via boundary conditions. We imposed periodic circular nematic surface fields at each confining surface. The resulting structures exhibit line defects which either connect the facing plates or remain confined within the layers near confining plates. The first structure is stable in relatively thin cells and the latter one in thick cells. We focused on structures at the threshold regime where both structures compete. We demonstrated that “history” of samples could have strong impact on resulting nematic configurations.

Curvature generation in nematic surfaces.

In recent years there has been a growing interest in the study of shape formation using modern responsive materials that can be preprogrammed to undergo spatially inhomogeneous local deformations. In particular, nematic liquid crystalline solids offer exciting possibilities in this context. Considerable recent progress has been made in achieving a variety of shape transitions in thin sheets of nematic solids by engineering isolated points of concentrated Gaussian curvature using topological defects in the nematic director field across textured surfaces. In this paper, we consider ways of achieving shape transitions in thin sheets of nematic glass by generation of nonlocalized Gaussian curvature in the absence of topological defects in the director field. We show how one can blueprint any desired Gaussian curvature in a thin nematic sheet by controlling the nematic alignment angle across the surface and highlight specific patterns which present feasible initial targets for experimental verification of the theory.

Non-equilibrium nature of two-dimensional isotropic and nematic coexistence in amyloid fibrils at liquid interfaces

Two-dimensional alignment of shape-anisotropic colloids is ubiquitous in nature, ranging from interfacial virus assembly to amyloid plaque formation. The principles governing two-dimensional self-assembly have therefore long been studied, both theoretically and experimentally, leading, however, to diverging fundamental interpretations on the nature of the two-dimensional isotropic-nematic phase transition. Here we employ single-molecule atomic force microscopy, cryogenic scanning electron microscopy and passive probe particle tracking to study the adsorption and liquid crystalline ordering of semiflexible β-lactoglobulin fibrils at liquid interfaces. Fibrillar rigidity changes on increasing interfacial density, with a maximum caused by alignment and a subsequent decrease stemming from crowding and domain bending. Coexistence of nematic and isotropic regions is resolved and quantified by a length scale-dependent order parameter S(2D)(d). The nematic surface fraction increases with interfacial fibril density, but depends, for a fixed interfacial density, on the initial bulk concentration, ascribing the observed two-dimensional isotropic-nematic coexistence to non-equilibrium phenomena.

Surface and bulk contributions to nematic order reconstruction

Nematic molecules confined in an asymmetric π cell and subjected to strong electric fields exhibit textural distortions involving nematic order variations, described by the Landau-de Gennes Q-tensor theory. We investigated the evolution of order variations as function of the applied electric pulse amplitude and of the nematic surface pretilt anchoring angles by implementing a Q-tensor model with a moving mesh finite element method. The proposed technique is able to clearly distinguish the bulk and the surface order reconstruction which occur in the cell.

Effect of Photo-Isomerization of Azo Dyes on the Photonic Bandgap in Chiral Nematics

Chiral nematic liquid crystals prepared with Grandjean texture demonstrate a photonic bandgap whose central wavelength is proportional to the pitch length, P, of the liquid crystal and whose width is given by (ne – no)P. We show that methyl red doped chiral nematics undergo a shift in the photonic bandgap upon photo-isomerization. This shift is a result of (1) photo-induced change in anchoring energy on the nematic surface, and (2) change in the natural pitch length from the photo-isomerization of the azo dye.

Rotational Solid Friction of a Nematic Liquid Crystal

Liquid crystal defects are used as probes to study the local reorientation dynamics of the nematic surface director on SiO(x) alignment layers. The tracking of the defect's motion reveals the presence of solid friction forces, unexpected in this complex viscous fluid. We identify the director pinning due to a surface quenched disorder as a possible mechanism that gives rise to the measured solid friction.

Orientational Quenched Disorder of a Nematic Liquid Crystal

By means of direct imaging, we map the surface heterogeneities of the nematic director orientation on a SiOx anchoring layer. The spatial correlations of surface director orientations are well fitted with a compressed exponential with exponent of 1.5 and typical correlation length of few microns. To discuss these results a formal analogy is established between the equation governing the nematic surface torques and the Langevin equation. Based on this analogy we prove that the disorder is spatially correlated orientational quenched disorder. The measured correlation length is discussed in terms of substrate morphology and molecular adsorption.

Colloid-wall interaction in a nematic liquid crystal: The mirror-image method of colloidal nematostatics

The new area of nematic colloidal systems (or nematic emulsions) has been greatly guided by the fruitful analogy between the colloidal nematostatics and electrostatics. The elastic charge density representation of the colloidal nematostatics [V. M. Pergamenshchik and V. O. Uzunova, Eur. Phys. J. E 23, 161 (2007); Phys. Rev. E 76, 011707 (2007)] develops this analogy at the level of charge density and Coulomb interaction. It shows, however, that the colloidal nematostatics in three dimensions substantially differs from the electrostatics both in its mathematical structure and physical implications: the elastic charge and multipoles are dyads; similar charges attract while opposite charges repel each other, and so on. In this paper we consider the interaction between an elastic charge and elastic dipole with a nematic surface (wall) at which the director alignment is fixed. Using the mirror image method of electrostatics as a guiding idea, we develop the mirror image method in the nematostatics for arbitrary director tilt at the wall. A wall is shown to induce a repulsive 1R{4} force on the elastic dipole which, in general, is accompanied by its reorientation. External torque on the colloid induces an elastic charge therein and triggers switching to the 1R{2} repulsion. The dyadic nature of an elastic dipole is shown to be essential: a particle-wall interaction potential cannot be obtained in phenomenological theories with a single component dipole. In the introductory sections we discuss connection between the director-mediated interaction in two and three dimensions and the electrostatic interaction and consider different symmetries of elastic dipoles. Conservation of the torque components exerted upon colloids is shown to play the role of Gauss' theorem and determines the elastic charge dyad.

Computational modelling of nematic phase ordering by film and droplet growth over heterogeneous substrates

This paper presents a computational study of defect nucleation associated with the kinetics of the isotropic‐to‐nematic phase ordering transition over heterogeneous substrates, as it occurs in new liquid crystal biosensor devices, based on the Landau–de Gennes model for rod‐like thermotropic nematic liquid crystals. Two regimes are identified due to interfacial tension inequalities: (i) nematic surface film nucleation and growth normal to the heterogeneous substrate, and (ii) nematic surface droplet nucleation and growth. The former, known as wetting regime, leads to interfacial defect shedding at the moving nematic‐isotropic interface. The latter droplet regime, involves a moving contact line, and exhibits two texturing mechanisms that also lead to interfacial defect shedding: (a) small and large contact angles of drops spreading over a heterogeneous substrate, and (b) small drops with large curvature growing over homogeneous patches of the substrate. The numerical results are consistent with qualitative defect nucleation models based on the kinematics of the isotropic–nematic interface and the substrate–nematic–isotropic contact line. The results extend current understanding of phase ordering over heterogeneous substrates by elucidating generic defect nucleation processes at moving interfaces and moving contact lines.

Influence of anchoring at a nematic cell surface on threshold spatially periodic reorientation of a director

We have analysed the influence of surface director anchoring in a planar flexoelectric nematic cell on the threshold spatially periodic reorientation of the director in an external dc electric field. By minimizing the free energy of the nematic cell we obtained the equations for a director and numerically solved them in the one elastic constant approximation. The dependences of the threshold electric field and the spatial period of director structure on the azimuthal and polar anchoring energy, as well as the flexoelectric parameters, are determined. It is shown that the domain of the flexoelectric parameter values, at which the spatially periodic reorientation of a director takes place, increases with decreasing azimuthal anchoring energy and increasing polar anchoring energy.

Defect-enhanced nematic surface order reconstruction

Within the Landau-de Gennes phenomenological theory, we study the influence of an applied electric field with average strength E{a} on the position of a nematic line defect with topological charge M=+/-1/2 in a hybrid cell. We explore the biaxial structure of the defect core and we describe its expulsion from the cell upon increasing E{a}. We show that prior to the expulsion the defect core displays dramatic changes for strong enough surface anchorings. At a critical value of E{a}, the core broadens and merges into a surface layer with a large biaxiality. This transition corresponds to the reconstruction of the nematic order already observed in the bulk in response to an applied electric field. A similar order reconstruction could take place even in the absence of defects, but at a higher threshold.

Smectic order induced at homeotropically aligned nematic surfaces: A neutron reflection study

Neutron reflection was used to measure the buildup of layers at a solid surface as the smectic phase is approached from higher temperatures in a nematic liquid crystal. The liquid crystal was 4-octyl-4'-cyanobiphenyl (8CB), and the solid was silicon with one of five different surface treatments that induce homeotropic alignment: (i) silicon oxide; (ii) a cetyltrimethylammonium bromide coating; (iii) an octadecyltrichlorosilane monolayer; (iv) an n-n-dimethyl-n-octadecyl-3- aminopropyltrimethyloxysilyl chloride monolayer; and (v) a lecithin coating. The development of surface smectic layers in the nematic phase of 8CB was followed by measuring specular reflectivity and monitoring the pseudo-Bragg peak from the layers. The scattering data were processed to remove the scattering from short-ranged smecticlike fluctuations in the bulk nematic phase from the specular reflection. The pseudo-Bragg peak at scattering vector Q approximately 0.2 A(-1) therefore corresponded to the formation of long-range smectic layers at the surface. The amplitude of the smectic density wave decayed with increasing distance from the surface, and the characteristic thickness of this smectic region diverged as the transition temperature was approached. It was found that the characteristic thickness for some of the surface treatments was greater than the correlation length in the bulk nematic. The different surfaces gave different values of the smectic order parameter at the surface. This suggests that the interaction with the surface is significantly different from a "hard wall" which would give the same values of the smectic order parameter and penetration depths similar to the bulk correlation length. Comparison of the different surfaces also suggested that the strength and range of the surface smectic ordering may be varied independently.

Influence of the bias-voltage on the anchoring energy for nematic liquid crystals.

The influence of the bias-voltage on the anisotropic part of the nematic surface energy is analyzed. The experimental data show a strong dependence of the anchoring strength on the bias-voltage when the electrodes of the nematic cell are covered with WO3. The observed dependence can be interpreted taking into account the ions dissolved in the liquid crystal. We propose a model in which the effect of the bias-voltage is to collect the ions near the electrodes, in a surface layer whose thickness is of the order of the Debye's screening length. The surplus of electric field due to this ions confinement gives rise to an electrostatic contribution to the total energy that can be considered as a surface energy. The proposed model is in good agreement with the experimental data. The model is used to interpret the observed independence of the anchoring strength on the bias-voltage when the (indium-tin-oxide) electrode is covered with a film of polyimide, or it is without any covering. The influence of a charge emission from the electrodes under the bias voltage on the anchoring energy is also analyzed. Possible applications of the observed phenomenon are discussed.

Thermodynamics of soft anisotropic interfaces

The Gibbs-Duhem equation for interfaces between nematic liquid crystals and isotropic fluids is formulated and shown to be a generic equation for soft anisotropic surfaces. The one-to-one correspondence between the nematic and crystalline surface Gibbs-Duhem equations is established. Consistency between the surface Gibbs-Duhem equation and the classical equations of interfacial nematostatics is shown. Using a phase space that takes into account thermodynamics, liquid crystalline order, and geometric variables, the generalized nematic surface Gibbs-Duhem equation reveals the presence of couplings between shape, adsorption, temperature, and average molecular orientation. Merging the thermodynamic analysis with nematostatics results in a model for morphactancy, that is, adsorption-induced interfacial shape selection. The specific roles of gradient bulk Frank elasticity, interfacial tension, and anchoring energy are elucidated by analyzing particular paths in the thermodynamic-geometric phase space.