Transformation of polar nematic phases in the presence of an electric field.

Only a few years have passed since the discovery of polar nematics, and now they are becoming the most actively studied liquid-crystal materials. Despite numerous breakthrough findings made recently, a theoretical systematization is still lacking. In the present paper, we take a step toward systematization. The powerful technique of molecular-statistical physics has been applied to an assembly of polar molecules influenced by electric field. Three polar nematic phases were found to be stable at various conditions: the double-splay ferroelectric nematic N_{F}^{2D} (observed in the lower-temperature range in the absence of or at low electric field), the double-splay antiferroelectric nematic N_{AF} (observed at intermediate temperature in the absence of or at low electric field), and the single-splay ferroelectric nematic N_{F}^{1D} (observed at moderate electric field at any temperature below transition into paraelectric nematic N and in the higher-temperature range (also below N) at low electric field or without it. A paradoxical transition from N_{F}^{1D} to N induced by application of higher electric field has been found and explained. A transformation of the structure of polar nematic phases at the application of electric field has also been investigated by Monte Carlo simulations and experimentally by observation of polarizing optical microscope images. In particular, it has been realized that, at planar anchoring, N_{AF} in the presence of a moderate out-of-plane electric field exhibits twofold splay modulation: antiferroelectric in the plane of the substrate and ferroelectric in the plane normal to the substrate. Several additional subtransitions related to fitting the confined geometry of the cell by the structure of polar phases were detected.

Optical nonlinearity of a dual-frequency nematic liquid crystal via temperature-mediated mapping of dielectric anisotropy.

Liquid crystals are of great interest in the field of nonlinear optics due to their efficient response to low intensity light fields. Here we present a new, to the best of our knowledge, mechanism of a nonlinear optical response which is observed for a dye-doped dual-frequency nematic liquid crystal. The local increase in temperature caused by the absorption of light beam in the liquid crystal medium leads to spatial variation and inversion of the sign of the dielectric anisotropy. When an alternating current electric field with a frequency close to the cross-over frequency is applied to the liquid crystal cell, the planar orientation sustains at the beam periphery, but elastic deformation occurs in the irradiation region. In the case of a dye dopant with negative absorption dichroism, a first-order orientational transition with large bistability region is obtained.

Emergence of paraelectric, improper antiferroelectric, and proper ferroelectric nematic phases in a liquid crystal composed of polar molecules.

We have elaborated a theoretical approach for the description of polar nematic phases observed by Nishikawa et al. [Adv. Mater. 29, 1702354 (2017)0935-964810.1002/adma.201702354], their structures, and transitions between them. Specific symmetry contributions to the pair molecular potentials provide the molecular mechanisms responsible for the formation of proper and improper polarity on the macroscopic level. An improper antiferroelectric nematic M2 phase can arise between paraelectric nematic M1 and proper ferroelectric nematic MP in the temperature scale. The local polarization in M2 arises mostly due to the local splay deformation. The director distribution in M2 represents the conjugation of cylindrical waves with opposite splay and polarization signs. The director and polarization are parallel to the cylindrical domain axes in the middle of each cylinder but exhibit considerable (mostly radial) deformation on the periphery of each cylinder. Polarization vectors are mostly stacked antiparallel on the borders between the domains without the director disruption. The domain size decreases with the decreasing temperature, the percentage of the antiferroelectric decouplings increases, and M2 exhibits the first-order phase transition into proper ferroelectric MP. With the increasing temperature the domain size in the M2 phase increases, the domination of particular polar orientation of molecules reduces, and finally, the domain size diverges at particular temperature corresponding to the second-order phase transition from M2 to paraelectric M1. Variations of the polar and nonpolar orientational order parameters are estimated within each phase and between the phases. Our experimental and computer simulation results (also presented in the paper) fully support our theoretical findings.

Highly efficient optical director reorientation of liquid-crystalline polymer induced by dye additives.

Light-induced director orientation of polymeric liquid-crystalline systems was investigated. The materials under study were composed of a nematic liquid-crystalline polymer (NLCP) and a small amount (0.05-0.5 wt.%) of conformationally active (azobenzene) or stable (anthraquinone) dye impurity. Light action on the homogeneously aligned polymer films above glass transition temperature leads to the director reorientation and, consequently, to a change in the extraordinary refractive index. The effect is associated with the dye molecule excitation and related change of intermolecular forces. In the case of NLCP with conformationally active dye dopant, an extremely high orientational optical response was detected (nonlinear coefficient is n_{2}∼0.1cm^{2}/W). In contrast, the efficiency of orientational light action on NLCP with conformationally stable dye dopant is of the same order of magnitude as that of dye-doped low-molar-mass liquid crystals. At the normal light incidence on the NLCP doped with azo-dye, the threshold director orientation is observed which is similar to the Fréedericksz transition under the action of magnetic and electric fields. The obtained high-orientational optical response of NLCP caused by azo-dye dopant in combination with the possibility of the recording of deformed structure in the glassy state, typical for polymer compounds, reveals new opportunities in photonics applications.

Light- and electric-field-induced first-order orientation transitions in a dendrimer-doped nematic liquid crystal.

Interaction of light and ac electric fields with a nematic liquid crystal (NLC) doped with nanosized second-generation carbosilane codendrimers containing terminal azobenzene fragments has been studied. A first-order Freedericksz transition in the linearly polarized light, accompanied by an intrinsic bistability in a wide region, was observed. An additional ac electric field decreases the light-induced Freedericksz transition threshold and narrows the bistability region. Light illumination transforms the second-order electric-field-induced Freedericksz transition to a first-order one. The width of the bistability region increases with the light wave intensity. The theory of the interaction of light and ac electric fields with the dendrimer-doped NLCs is developed taking into account an additional (with respect to the undoped nematic host) dependence of the optical torque on the angle between the director and the light field.