High-Order Nonlinear Electrophoresis in a Nematic Liquid Crystal.

Electrophoresis is the motion of particles relative to a surrounding fluid driven by a uniform electric field. In conventional electrophoresis, the electrophoretic velocity grows linearly with the applied field. Nonlinear effects with a quadratic speed vs field dependence are gaining research interest since an alternating current field could drive them. Here, we report on the giant nonlinearity of electrophoresis in a nematic liquid crystal in which the speed grows with the fourth and sixth powers of the electric field. The mechanism is attributed to the shear thinning of the nematic environment induced by the moving colloid. The observed giant nonlinear effect dramatically enhances the efficiency of electrophoretic transport.

Dielectric Properties of a Ferroelectric Nematic Material: Quantitative Test of the Polarization-Capacitance Goldstone Mode.

The recently discovered ferroelectric nematic (N_{F}) liquid crystals (LC) have been reported to show an extraordinarily large value of the real part of the dielectric constant (ϵ^{'}>10^{3}) at low frequencies. However, it was argued by Clark et al. in Phys. Rev. Res. 6, 013195 (2024)PPRHAI2643-156410.1103/PhysRevResearch.6.013195 that what was measured was the capacitance of the insulating layer at LC or electrode surface and not that of the liquid crystal. Here we describe the results of dielectric spectroscopy measurements of an N_{F} material in cells with variable thickness of the insulating layers. Our measurements quantitatively verify the model by Clark et al. Additionally, our measurements in cells with bare conducting indium tin oxide surface provide a crude estimate of ϵ_{⊥}∼10^{2} in the N_{F} phase.

Polar Self-Organization of Ferroelectric Nematic-Liquid-Crystal Molecules on Atomically Flat Au(111) Surface.

Understanding nanoscale mechanisms responsible for the recently discovered ferroelectric nematics can be helped by direct visualization of self-assembly of strongly polar molecules. Here, we report on scanning tunneling microscopy studies of monomolecular layers of a ferroelectric nematic liquid crystal on a reconstructed Au(111) surface. The monolayers are obtained by deposition from a solution at ambient conditions. The adsorbed ferroelectric nematic molecules self-assemble into regular rows with tilted orientation, resembling a layered structure of a smectic C. Remarkably, each molecular dipole in this architecture is oriented along the same direction giving rise to polar ferroelectric ordering.

Toroidal nuclei of columnar lyotropic chromonic liquid crystals coexisting with an isotropic phase.

Nuclei of ordered materials emerging from the isotropic state usually show a shape topologically equivalent to a sphere; the well-known examples are crystals and nematic liquid crystal droplets. In this work, we explore experimentally and theoretically the toroidal in shape nuclei of columnar lyotropic chromonic liquid crystals coexisting with the isotropic phase. The geometry of these toroids depends strongly on concentrations of the disodium cromoglycate (DSCG) and the crowding agent, polyethylene glycol (PEG). High concentrations of DSCG and PEG result in thick toroids with small central holes, while low concentrations yield thin toroids with wide holes. The multitude of the observed shapes is explained by the balance of bending elasticity and anisotropic interfacial tension.

Correction: Shear-induced polydomain structures of nematic lyotropic chromonic liquid crystal disodium cromoglycate.

Correction for 'Shear-induced polydomain structures of nematic lyotropic chromonic liquid crystal disodium cromoglycate' by Hend Baza et al., Soft Matter, 2020, 16, 8565-8576.

Shear-induced polydomain structures of nematic lyotropic chromonic liquid crystal disodium cromoglycate.

Lyotropic chromonic liquid crystals (LCLCs) represent aqueous dispersions of organic disk-like molecules that form cylindrical aggregates. Despite the growing interest in these materials, their flow behavior is poorly understood. Here, we explore the effect of shear on dynamic structures of the nematic LCLC, formed by 14 wt% water dispersion of disodium cromoglycate (DSCG). We employ in situ polarizing optical microscopy (POM) and small-angle and wide-angle X-ray scattering (SAXS/WAXS) to obtain independent and complementary information on the director structures over a wide range of shear rates. The DSCG nematic shows a shear-thinning behavior with two shear-thinning regions (Region I at [small gamma, Greek, dot above] < 1 s-1 and Region III at [small gamma, Greek, dot above] > 10 s-1) separated by a pseudo-Newtonian Region II (1 s-1 < [small gamma, Greek, dot above] < 10 s-1). The material is of a tumbling type. In Region I, [small gamma, Greek, dot above] < 1 s-1, the director realigns along the vorticity axis. An increase of [small gamma, Greek, dot above] above 1 s-1 triggers nucleation of disclination loops. The disclinations introduce patches of the director that deviates from the vorticity direction and form a polydomain texture. Extension of the domains along the flow and along the vorticity direction decreases with the increase of the shear rate to 10 s-1. Above 10 s-1, the domains begin to elongate along the flow. At [small gamma, Greek, dot above] > 100 s-1, the texture evolves into periodic stripes in which the director is predominantly along the flow with left and right tilts. The period of stripes decreases with an increase of [small gamma, Greek, dot above]. The shear-induced transformations are explained by the balance of the elastic and viscous energies. In particular, nucleation of disclinations is associated with an increase of the elastic energy at the walls separating nonsingular domains with different director tilts. The uncovered shear-induced structural effects would be of importance in the further development of LCLC applications.

Periodic assembly of nanoparticle arrays in disclinations of cholesteric liquid crystals.

An important goal of the modern soft matter science is to discover new self-assembly modalities to precisely control the placement of small particles in space. Spatial inhomogeneity of liquid crystals offers the capability to organize colloids in certain regions such as the cores of the topological defects. Here we report two self-assembly modes of nanoparticles in linear defects-disclinations in a lyotropic colloidal cholesteric liquid crystal: a continuous helicoidal thread and a periodic array of discrete beads. The beads form one-dimensional arrays with a periodicity that matches half a pitch of the cholesteric phase. The periodic assembly is governed by the anisotropic surface tension and elasticity at the interface of beads with the liquid crystal. This mode of self-assembly of nanoparticles in disclinations expands our ability to use topological defects in liquid crystals as templates for the organization of nanocolloids.

Dye-doped dual-frequency nematic cells as fast-switching polarization-independent shutters.

We present polarization-independent optical shutters with a sub-millisecond switching time. The approach utilizes dual-frequency nematics doped with a dichroic dye. Two nematic cells with orthogonal alignment are driven simultaneously by a low-frequency or high-frequency electric field to switch the shutter either into a transparent or a light-absorbing state. The switching speed is accelerated via special short pulses of high amplitude voltage. The approach can be used in a variety of electro-optical devices.

Polarization-Modulated Bent-Core Liquid Crystal Thin Films without Layer Undulation.

Spatial confinement is known to affect molecular organizations of soft matter. We present an important manifestation of this statement for thin films of bent-core smectic liquid crystals. Prior freeze-fracture transmission electron microscopy (FFTEM) studies carried out on nitro-substituted bent-core mesogens (n-OPIMB-NO_{2}) revealed an undulated smectic layer structure with an undulation periodicity of ∼8 nm. We report cryogenic TEM measurements on ∼100 nm thick 8-OPIMB-NO_{2} films. In contrast to FFTEM results, our studies show only density modulation with periodicity b=16.2 nm, and no smectic layer undulation. We show that the discrepancy between the FFTEM and cryogenic transmission electron microscopy (cryo-TEM) results can be attributed to the different sample thicknesses used in the experiments. FFTEM monitors cracked surfaces of a relatively thick (5-10 µm) frozen sample, whereas cryo-TEM visualizes the volume of a thin (0.1 µm) film that was quenched from its partially fluid phase. These results have importance in possible photovoltaics and organic electronics applications where submicron thin films are used.

Pretransitional behavior of viscoelastic parameters at the nematic to twist-bend nematic phase transition in flexible n-mers.

We report dynamic light scattering measurements of the orientational (Frank) elastic constants and associated viscosities among a homologous series of a liquid crystalline dimer, trimer, and tetramer exhibiting a uniaxial nematic (N) to twist-bend nematic (NTB) phase transition. The elastic constants for director splay (K11), twist (K22) and bend (K33) exhibit the relations K11 > K22 > K33 and K11/K22 > 2 over the bulk of the N phase. Their behavior near the N-NTB transition shows dependency on the parity of the number (n) of the rigid mesomorphic units in the flexible n-mers. Namely, the bend constant K33 in the dimer and tetramer turns upward and starts increasing close to the transition, following a monotonic decrease through most of the N phases. In contrast, K33 for the trimer flattens off just above the transition and shows no pretransitional enhancement. The twist constant K22 increases pretransitionally in both even and odd n-mers, but more weakly so in the trimer, while K11 increases steadily on cooling without evidence of pretransitional behavior in any n-mer. The viscosities associated with pure splay, twist-dominated twist-bend, and pure bend fluctuations in the N phase are comparable in magnitude to those of rod-like monomers. All three viscosities increase with decreasing temperature, but the bend viscosity in particular grows sharply near the N-NTB transition. The N-NTB pretransitional behavior is shown to be in qualitative agreement with the predictions of a coarse-grained theory, which models the NTB phase as a "pseudo-layered" structure with the symmetry (but not the mass density wave) of a smectic-A* phase.

Electrically tunable laser based on oblique heliconical cholesteric liquid crystal.

A cholesteric liquid crystal (CLC) formed by chiral molecules represents a self-assembled one-dimensionally periodic helical structure with pitch [Formula: see text] in the submicrometer and micrometer range. Because of the spatial periodicity of the dielectric permittivity, a CLC doped with a fluorescent dye and pumped optically is capable of mirrorless lasing. An attractive feature of a CLC laser is that the pitch [Formula: see text] and thus the wavelength of lasing [Formula: see text] can be tuned, for example, by chemical composition. However, the most desired mode to tune the laser, by an electric field, has so far been elusive. Here we present the realization of an electrically tunable laser with [Formula: see text] spanning an extraordinarily broad range (>100 nm) of the visible spectrum. The effect is achieved by using an electric-field-induced oblique helicoidal (OH) state in which the molecules form an acute angle with the helicoidal axis rather than align perpendicularly to it as in a field-free CLC. The principal advantage of the electrically controlled CLCOH laser is that the electric field is applied parallel to the helical axis and thus changes the pitch but preserves the single-harmonic structure. The preserved single-harmonic structure ensures efficiency of lasing in the entire tunable range of emission. The broad tuning range of CLCOH lasers, coupled with their microscopic size and narrow line widths, may enable new applications in areas such as diagnostics, sensing, microscopy, displays, and holography.

Tuning selective reflection of light by surface anchoring in cholesteric cells with oblique helicoidal structures.

Selective reflection of light by oblique helicoidal cholesteric (ChOH) can be tuned in a very broad spectral range by an applied electric field. In this Letter, we demonstrate that the peak wavelength of the selective reflection can be controlled by the surface alignment of the director in sandwich cells. The peak wavelength is blue-shifted when the surface alignment is perpendicular to the bounding plates and red-shifted when it is planar. The effect is explained by the electric field redistribution within the cell caused by a spatially varying heliconical ChOH structure. The observed phenomenon can be used in sensing applications.

Order parameters and time evolution of mesophases in the lyotropic chromonic liquid crystal Sunset Yellow FCF by DNMR.

Uniaxial order parameters of the nematic and columnar mesophases in the lyotropic chromonic liquid crystal Sunset Yellow FCF have been determined from deuteron nuclear magnetic resonance, where random confinement of the system by the dispersion of aerosil nanoparticles has been performed to help obtain the angular dependent spectra. The long-time evolution study of the order parameters shows that the system requires tens of hours to stabilize after a deep change in temperature, in contrast with the very fast assembly process of the aggregates. Finally, the degree of order of the water molecules, forced by the uniaxial environment, has been determined.

Living liquid crystals.

Collective motion of self-propelled organisms or synthetic particles, often termed "active fluid," has attracted enormous attention in the broad scientific community because of its fundamentally nonequilibrium nature. Energy input and interactions among the moving units and the medium lead to complex dynamics. Here, we introduce a class of active matter--living liquid crystals (LLCs)--that combines living swimming bacteria with a lyotropic liquid crystal. The physical properties of LLCs can be controlled by the amount of oxygen available to bacteria, by concentration of ingredients, or by temperature. Our studies reveal a wealth of intriguing dynamic phenomena, caused by the coupling between the activity-triggered flow and long-range orientational order of the medium. Among these are (i) nonlinear trajectories of bacterial motion guided by nonuniform director, (ii) local melting of the liquid crystal caused by the bacteria-produced shear flows, (iii) activity-triggered transition from a nonflowing uniform state into a flowing one-dimensional periodic pattern and its evolution into a turbulent array of topological defects, and (iv) birefringence-enabled visualization of microflow generated by the nanometers-thick bacterial flagella. Unlike their isotropic counterpart, the LLCs show collective dynamic effects at very low volume fraction of bacteria, on the order of 0.2%. Our work suggests an unorthodox design concept to control and manipulate the dynamic behavior of soft active matter and opens the door for potential biosensing and biomedical applications.

Reversible Isothermal Twist-Bend Nematic-Nematic Phase Transition Driven by the Photoisomerization of an Azobenzene-Based Nonsymmetric Liquid Crystal Dimer.

The liquid crystal nonsymmetric dimer, 1-(4-butoxyazobenzene-4'-yloxy)-6-(4-cyanobiphenyl-4'-yl) hexane (CB6OABOBu), shows enantiotropic twist-bend nematic, NTB, and nematic, N, phases. The NTB phase has been confirmed using polarized light microscopy, freeze fracture transmission electron microscopy, and X-ray diffraction. The helicoidal pitch in the NTB phase is 18 nm. The NTB-N (TNTBN) and N-I (TNI) transition temperatures are reduced upon UV light irradiation, with the reduction in TNTBN being much larger than that in TNI. An isothermal, reversible NTB-N transition may be driven photochemically. These observations are attributed to a trans-cis photoisomerization of the azobenzene fragment on UV irradiation, with the cis isomers stabilizing the standard nematic phase and the trans isomers stabilizing the NTB phase. The dramatic changes in TNTBN provide evidence that the transition between the normal nematic and twist-bend nematic with spontaneous breaking of chiral symmetry is crucially dependent on the shape of molecular dimers, which changes greatly during the trans-cis isomerization.

Nanosecond switching of micrometer optical retardance by an electrically controlled nematic liquid crystal cell.

Electro-optic response of liquid crystals in mainstream display applications exhibits a millisecond switching of optical retardance on the order of one micrometer. We demonstrate that a similarly large optical retardance can be switched much faster, within 10-100 nanoseconds, by using multiple passes of light through a cell filled with the nematic liquid crystal. The fast response is based on the so-called nanosecond electric modification of order parameters (NEMOP) effect. The described approach can be used to develop ultrafast optical shutters and modulators.

Cholesteric liquid crystals in rectangular microchannels: skyrmions and stripes.

In this paper, we present experimental and numerical studies on the microstructures of a cholesteric liquid crystal (CLC) confined in rectangular micron-channels. By using a sequence of microfabrication techniques we fabricated the micro-sized channels with accurately controlled size, aspect ratio and homeotropic surface anchoring. Through optical microscopic studies we established a phase diagram for the liquid crystal defect textures as a function of the channel depth and width. For the channel width larger than ∼2 times the cholesteric pitch p, the LC molecules are oriented primarily vertical to the channel when the channel depth is below 0.75p, form bubble domain defects when the channel depth is around 0.75p, and form stripe textures when the cell depth is above the cholesteric pitch p. In addition, the bubble domain size and the stripe texture periodicity are found to grow with the increase of the channel width. For the channel width smaller than ∼2p and the channel depth between 0.6p to 1.1p, no textures can be observed in the channels. Numerical simulations based on a director tensor relaxation approach yield detailed molecular director fields, and show that the bubble domain defects are baby-skyrmions and that the stripes are the first type of cholesteric fingerprints. A comparison with previous experiments and numerical simulations indicates that the size of the microchannels also influences what type of soliton-like topological textures form in the CLCs confined in the channels.

Correction: Cholesteric liquid crystals in rectangular microchannels: skyrmions and stripes.

Correction for 'Cholesteric liquid crystals in rectangular microchannels: skyrmions and stripes' by Yubing Guo et al., Soft Matter, 2016, DOI: 10.1039/c6sm01190j.

Understanding the twist-bend nematic phase: the characterisation of 1-(4-cyanobiphenyl-4'-yloxy)-6-(4-cyanobiphenyl-4'-yl)hexane (CB6OCB) and comparison with CB7CB.

The synthesis and characterisation of the nonsymmetric liquid crystal dimer, 1-(4-cyanobiphenyl-4'-yloxy)-6-(4-cyanobiphenyl-4'-yl)hexane (CB6OCB) is reported. An enantiotropic nematic (N)-twist-bend nematic (NTB) phase transition is observed at 109 °C and a nematic-isotropic phase transition at 153 °C. The NTB phase assignment has been confirmed using polarised light microscopy, freeze fracture transmission electron microscopy (FFTEM), (2)H-NMR spectroscopy, and X-ray diffraction. The effective molecular length in both the NTB and N phases indicates a locally intercalated arrangement of the molecules, and the helicoidal pitch length in the NTB phase is estimated to be 8.9 nm. The surface anchoring properties of CB6OCB on a number of aligning layers is reported. A Landau model is applied to describe high-resolution heat capacity measurements in the vicinity of the NTB-N phase transition. Both the theory and heat capacity measurements agree with a very weak first-order phase transition. A complementary extended molecular field theory was found to be in suggestive accord with the (2)H-NMR studies of CB6OCB-d2, and those already known for CB7CB-d4. These include the reduced transition temperature, TNTBN/TNI, the order parameter of the mesogenic arms in the N phase close to the NTB-N transition, and the order parameter with respect to the helix axis which is related to the conical angle for the NTB phase.