Nonlinear molecular deformations and solitons in a nematic liquid crystal

We studied nonlinear molecular deformations in a nematic liquid crystal with homeotropically aligned molecules and hard boundaries. As the basic dynamical equation for the director axis of the liquid crystal resembles the Landau-Lifshitz equation representing spin dynamics in a one dimensional classical continuum isotropic Heisenberg ferromagnetic spin chain, we invoke here the space curve formalism and the stereographic projection technique used in the case of the Heisenberg spin chain. Under space curve mapping, the director dynamics with elastic deformation is found to be governed by a perturbed nonlinear Schrödinger equation. A multiple-scale perturbation analysis brings out perturbed solitons to represent molecular deformations in the nematic liquid crystal. However, when a constant electric field is applied, the director dynamics is expressed under stereographic projection and the molecular deformations are found to be governed by periodic and localized static planar director configurations. A linear stability analysis on the static planar configurations shows that the system exhibits stable deformations.     

c-director relaxation around a vortex of strength +1 in free-standing smectic-C films

The relaxation of director fields in freely suspended smectic films is studied experimentally by means of polarizing microscopy, and analyzed by solving the torque balance equation under appropriate initial and boundary conditions. We consider in particular the role of anchoring conditions of the c-director at particles and defects in the film. The structure of regular relaxation patterns allows to determine the elastic anisotropy of smectic materials. The splay elastic constant can exceed the bend constant by a factor of two and more. A remarkable consequence of this anisotropy is the stick-slip-like relaxation around a central defect of topological strength s = + 1.     

Electroconvection in nematics above the splay Fréedericksz transition

We present a basic model for an instability leading to a novel type of electroconvection patterns observed above the splay Fréedericksz transition in nematics. Such patterns, with wave vector perpendicular to the director easy axis, are found in planar sandwich cells under crossed polarizers, they do not produce shadowgraph images at onset. An adaptation of the classical Carr Helfrich mechanism is introduced. The ground state is a tilted director field uniform in the cell plane. The proposed mechanism destabilizes this director field and leads to a structure with modulated out-of-plane (twist) deformations. Experimental confirmation is provided by polarizing microscopy. All experimental observations are qualitatively explained with the proposed model.     

Deformation of cholesteric elastomers by uniaxial stress along the helix axis

The deformation of cholesteric elastomers by mechanical stress applied parallel to the helix axis is studied by calculation of the free-energy density. The Frank-elasticity contribution is taken into account. A chiral solvent, present at cross-linking time, is in general considered to be replaced after cross-linking by a solvent with different chirality. Two special cases considered are zero and unchanged solvent chirality, the first known as that of imprinted cholesteric elastomers, the latter equivalent to intrinsic cholesteric elastomers with chemically attached chiral groups. Depending on material parameters and imposed strain, the director can show a tilt towards the helix axis up to the maximum tilt, corresponding to a nematic state. In case of intrinsic elastomers with low conformation anisotropy, direct transitions from untilted to nematic states can be induced by straining. The helix structure of the director field is coarsened with an average wave number different to that of the information inscribed in the network at cross-linking time, if this lowers the average free-energy density. Switching between different states can be achieved with electric fields of reasonable values applied parallel to the helix axis. Spectra of the reflection of polarized light are calculated.     

Critical exponents for Fréedericskz transition in nematics between concentric cylinders

The equilibrium tilt angle profile in a cell limited by two concentric cylinders filled with nematic liquid crystals is determined for strong homeotropic anchoring at the surfaces. The anchoring condition is such that the nematic director is perpendicular to the cylinder axes and a radial nonuniform electric field is applied to investigate a Fréedericksz transition. The distortions induced by the field remain in the plane perpendicular to the cylinder axes, and a threshold field is analytically determined indicating a transition from a pure splay to a splay-bend conformation of the director. It is shown that this transition can be induced by the thickness of the region between the two cylinders, and can be detected even in the absence of an external field. If the maximum value of the tilt angle is assumed as an order parameter, its behavior near to the transition can be used to obtain the critical exponent, which is the same as the one obtained in the mean field approximation. These results are indications that nontrivial consequences may occur when complex fluids are subject to non-planar geometries.     

Deformation of a pretilted nematic liquid crystal layer in an electric field

The deformation of the optical axis of a nematic liquid crystal layer under the influence of an electric field is caused by the dielectric torque. This momentum counteracts with an elastic torque generated by interfacial forces between the surface of the electrode and the liquid crystal. By means of a variational analysis, the deformation profiles within the liquid crystal layer are calculated, assuming large interfacial energies and various angles of pretilt of the liquid crystal directors with respect to the electrodes. Both the extreme case of a homeotropic (vertical) alignment on one electrode and a homogeneous (parallel) alignment on the opposite electrode, as well as the general case of arbitrary and different alignments on both electrodes, lead to heavily pretilted liquid crystal layers, resulting in definite deformation profiles without disclinations. Liquid crystal cells prepared in this way neither show threshold voltages nor delay times when electrical fields are applied. Measured and calculated characteristics of such liquid crystal cells are presented, they show good agreement.     

Effect of surface electric field on the anchoring of nematic liquid crystals

We analyse the influence of adsorbed ions and the resulting surface electric field and its gradient on the anchoring properties of nematics with ionic conductivity. We take into account two physical mechanisms for the coupling of the nematic director with the surface electric field: (i) the dielectric anisotropy and (ii) the coupling of the quadrupolar component of the flexoelectric coefficient with the field gradient. It is shown that for sufficiently large fields near saturated coverage of the adsorbed ions, there can be a spontaneous curvature distortion in the cell even when the anchoring energy is infinitely strong. We also discuss the director distortion when the anchoring energy of the surface is finite. Received: 29 September 1997 / Received in final from: 10 November 1997 / Accepted: 18 November 1997     

Nematic ordering in anisotropic elastomers: Effect of frozen anisotropy

Nematic ordering in anisotropic non-Gaussian elastomers is considered theoretically using mean field approximation. We focus on the effect of anisotropy during network cross-linking on the system elasticity and, in particular, on the so-called soft deformation mode. As the main result, we calculate the dependence of the elastomer free energy on the angle between the axis of “frozen” anisotropy and the nematic director. The dependence of the isotropic-nematic transition point on the orientational field acting on the monomers during the cross-linking process is also calculated. Received: 5 November 1997 / Revised and Accepted: 29 June 1998     

Colloidal inclusions in smectic films with spontaneous bend

Inclusions in free-standing smectic films are simple model systems for two-dimensional anisotropic dispersions. From theory and experiment, different topologies of elastic distortions of the embedding liquid crystal are known. Quadrupolar and different dipolar defect configurations in the vicinity of the inclusion are possible, and these configurations determine the type of interactions between the inclusions. The quadrupolar configuration is often energetically preferred. We show, however, that dipolar director configurations around inclusions can be energetically favourable over quadrupolar arrangements in chiral smectics, as a consequence of a spontaneous-bend term in the elastic-energy formulation. As the inclusion size influences the selection of the deformation types, the corresponding spontaneous-bend constant can be estimated for the strong anchoring limit if the c -director fields around inclusions of different diameters are taken into account.     

Energetics of 2D colloids in free-standing smectic-C films

The formation of regular colloid patterns in free-standing smectic films at the transition from the smectic-C to the isotropic or nematic phase is well known experimentally. The self-organization of isotropic or nematic droplets is caused by their mutual interaction, mediated by elastic distortions of the local director in the surrounding liquid crystal. These distortions are related to the anchoring conditions of the director at the droplet border. We describe analytically the energetics of the liquid crystal environment of a single droplet in one-constant approximation. A method of complex analysis, Conformal Mapping, is employed. Following a suggestion of Dolganov et al. (Phys. Rev. E. 73, 041706 (2006)), energetics of chain and grid patterns built from the colloids are investigated numerically in order to explain experimentally observed formations and their director fields.     

Structure and elastic properties of a nematic liquid crystal: A theoretical treatment and molecular dynamics simulation

The Frank elasticity constants which describe splay (K ₁), twist (K ₂), and bend (K ₃) distortion modes are investigated for 4-n-pentyl-4'-cyanobiphenyl (5CB) in the nematic liquid crystal. The calculations rest on statistical-mechanical approaches where the absolute values of K _i (i=1,2,3) are dependent on the direct correlation function (DCF) of the corresponding nematic state. The DCF was determined using the pair correlation function by solving the Ornstein-Zernike equation. The pair correlation function, in turn, was obtained from molecular dynamics (MD) trajectory. Three different approaches for calculations of the elasticity constants were employed based on different level of approximation about the orientational order and molecular correlations. The best agreement with experimental values of elasticity constants was obtained in a model where the full orientational distribution function was used. In addition we have investigated the approximation about spherical distribution of the intermolecular vectors in the nematic phase, often used in derivation of various mean-field theories and employed here for the construction of the DCF. We found that this assumption is not strictly valid, in particular a strong deviation from the isotropic distribution is observed for short intermolecular distances. Received 22 March 2000 and Received in final form 9 June 2000     

Orientational diffusivities measured by Rayleigh scattering in a lyotropic calamitic nematic () liquid crystal phase: the backflow problem revisited

Using a light-beating technique we have measured the damping time of thermal fluctuations of the nematic director for the so called cylindrical or calamitic nematic (N_C) phase of the lyotropic system K-laurate/decanol/. By varying the scattering angle in suitable geometries, we have been able to estimate the orientational diffusivities associated to the three pure deformations of splay, twist and bend. A former measurement made in the disk-like N_D phase of the same system yielded a large deviation between the splay and twist diffusivities. The effect was then attributed to induced flows, or backflow, which could be responsible for the reduction of the splay viscosity. In fact, this is the analogous effect, for disks, to the one recognized since long time ago arriving for rod-like molecules in a classical nematic, though in this case it is associated with bend deformations. The analogy comes about thanks to the interchange of the role played by disks and cylinders for, respectively, splay and bend fluctuations.The measurements reported here provide a new test on the applicability of the backflow model to a nematic system composed of micelles, that is, aggregates made of amphiphilic (surfactant) molecules, in its cylindrical-like variant, i.e. the N_C phase. In addition, the comparative study made here with the previous results existing in the literature for the N_D phase, allows us to conjecture on structural issues concerning lyotropic nematics. Received: 29 April 1998 / Revised: 19 August 1998 / Accepted: 31 August 1998     

Novel twist grain boundary smectic-C phases

Several new kinds of smectic-C twist grain boundary phases (TGBC) have been observed during the last few years. These pure compounds or mixtures exhibit unusual textures with polygonal lattices (square or hexagonal grids) in the plane normal to the TGB helix. The structure of these new phases seems to be complex and different from reported and predicted TGBC phases. In this article, we review the main results obtained on these different new phases, and we propose new TGBC structures based on the well-known splayed polarization --twisted director structures adopted by chiral smectic-C's in planar aligned (bookshelf) cells. The observed square or hexagonal lattices are made of superimposed pairs of unwinding lines due to the suppression of the helix within smectic-C blocks by the grain boundaries (unwinding walls). A lattice-free TGBC occurs if the helix within smectic-C blocks is suppressed completely. Received 15 March 2001     

The elastic anisotropy of nematic elastomers

We examine the robustness of order in nematic elastomers under mechanical strains imposed along and perpendicularly to the director when director rotation is prohibited. In contrast to electric and magnetic fields applied to conventional nematics, mechanical fields are shown theoretically and experimentally to greatly affect the degree of nematic order and related quantities. Unlike in liquid nematics, one can impose fields perpendicular to the director, thereby inducing biaxial order which should be susceptible to experimental detection. Nematic elastomers with unchanging director and degree of order should theoretically have the same elastic moduli for longitudinal and transverse extensions. This is violated when nematic order is permitted to relax in response to strains. Near the transition we predict the longitudinal modulus to be smaller than the transverse modulus; at lower temperatures the converse is true, with a crossover a few degrees below the transition. The differences are ascribed to the different temperature dependence of the stiffness of uniaxial and biaxial order. We synthesised side chain single-crystal nematic polymer networks, performed DSC, X-ray, birefringence, and thermo-mechanical characterisations, and then obtained linear moduli from stress-strain measurements. Received 29 September 2000     

Director reorientation in twisted nematic liquid crystals due to thermomechanical effect

We have studied molecular director reorientation in a twisted nematic liquid crystal induced by a two-dimensional temperature gradient. We studied the effect of rate change between the temperature gradients in two directions. Our obtained director reorientations are in the range that can be observed experimentally very easily.     

Transient grating optical nonlinearities in nematic,cholesteric and smectic liquid crystals

The transients of Kerr-like optical nonlinearities in various liquid crystals observed with picosecond light-induced dynamic gratings are discussed. It is shown that relatively high intensities and strong optical fields of short laser pulses lead to rapid molecular reorientation, ultrasound generation, multiphoton absorption, cholesteric helix deformation and other new phenomena which are not only of interest for basic liquid-crystal research but also determine photonic switching times in liquid crystalline all-optical devices.     

The role of Frank elasticity in cholesteric elastomers

The effect of Frank elasticity on deformations of cholesteric elastomers by mechanical stress applied perpendicular to the helix axis is studied by numerical minimization of the free energy. Above a critical strain, a solution with an only oscillating director is found to be stable in comparison to a distorted helix. At the critical strain, the contractions perpendicular to stress change discontinuously. The critical strain is found to increase with increasing Frank elasticity contribution to the free energy density, and to diverge when the conformation anisotropy of the polymer backbone vanishes. The results are compared with recent experiments which indicated that, in case of weak conformation anisotropies, the Frank elasticity contribution to the free energy cannot be neglected.     

Effect of magnetic fields on out-of-plane orientations of nematic liquid crystalline polymers under simple shear flow

The effect of magnetic fields on out-of-plane orientations of liquid crystalline polymers (LCPs) under simple shear flows is numerically analyzed using the Doi–Hess equation. The evolution equation for the probability distribution function of the LCP molecules is directly solved without any approximation closure. The initial director is parallel to the vorticity direction. Two cases of the magnetic fields are considered (1) the magnetic field parallel to the flow direction, and (2) the magnetic field parallel to the velocity gradient direction. For both cases a log-rolling orientation state is detected at low shear rates. However, the director is quickly aligned along the direction of magnetic fields because of the deformation of molecules. The field affects on the scalar order parameter rather than the major orientation direction for the magnetic field parallel to the flow direction. On the other hand regarding the magnetic field along the vorticity gradient direction, the effect of the magnetic field is more remarkable on the major orientation in comparison with the effect on the scalar order parameter. Also it is be found that the order parameter is increased obviously with increasing the magnetic fields. It is an efficient way to improve the performance of LCP materials.     

Effect of high electric fields on the nematic to isotropic transition in a material exhibiting large negative dielectric anisotropy

We report the experimental high electric field phase diagram of a nematic liquid crystal which exhibits a large negative dielectric anisotropy. We measure simultaneously the birefringence (Δn) and the dielectric constant (epsilon_⊥) at various applied fields as functions of the local temperature of an aligned sample. We also measure the higher harmonics of the electrical response of the medium. The following experimental results are noted: (i) enhancement of orientational order parameter S in the nematic phase due to both the Kerr effect and quenching of director fluctuations; (ii) enhancement in the paranematic to nematic transition temperature (T_PN) with field; (iii) divergence of the order parameter susceptibility beyond the tricritical point as measured by third harmonic electrical signal; (iv) a small second harmonic electrical signal which also diverges near T_PN, indicating the presence of polarised domains. Our measurements show that ΔT_PN(= T_PN(E)-T_NI(0)) varies linearly with |E| whereas the Landau de Gennes theory predicts a dependence on E². It is argued that the quenching of director fluctuations by the field makes the dominant contribution to all the observations, including the thermodynamics of the transition.