Microfluidic Tensiometry Technique for the Characterization of the Interfacial Tension between Immiscible Liquids.

The interfacial tension between two immiscible fluids is of critical importance for understanding many natural phenomena as well as in industrial production processes; however, it can be challenging to measure this parameter with high accuracy. Most commonly used techniques have significant shortcomings because of their reliance on other data such as density or viscosity. To overcome these issues, we devise a technique that works with very small sample quantities and does not require any data about either fluid, based on micropipette aspiration techniques. The method facilitates the generation of a droplet of one fluid inside of the other, followed by immediate in situ aspiration of the droplet into a constricted channel. A modified Young-Laplace equation is then used to relate the pressure needed to produce a given deformation of the droplet's radius to the interfacial tension. We demonstrate this technique on different systems with interfacial tensions ranging from sub-millinewton per meter to several hundred millinewton per meter, thus over 4 orders of magnitude, obtaining precise results in agreement with the literature solely from experimental observations of the droplet deformation.

Direct visualization of spatiotemporal structure of self-assembled colloidal particles in electrohydrodynamic flow of a nematic liquid crystal.

Characterization of spatiotemporal dynamics is of vital importance to soft matter systems far from equilibrium. Using a confocal laser scanning microscopy, we directly reveal three-dimensional motion of surface-modified particles in the electrohydrodynamic convection of a nematic liquid crystal. Particularly, visualizing a caterpillar-like motion of a self-assembled colloidal chain demonstrates the mechanism of the persistent transport enabled by the elastic, electric, and hydrodynamic contributions. We also precisely show how the particles' trajectory is spatially modified by simply changing the surface boundary condition.

Stabilisation of 2D colloidal assemblies by polymerisation of liquid crystalline matrices for photonic applications.

Colloidal crystals in anisotropic matrices are extremely stable and versatile, but disassemble as soon as the anisotropy of the matrix disappears. We present an approach to first custom-assemble colloidal structures and subsequently stabilize them through photo-polymerisation of the liquid crystalline matrix. The resulting 2D colloidal assemblies are stable at high temperatures and can even be obtained as free-standing films without a decrease in the degree of organization. This approach could be used to stabilize and extract recently proposed soft-matter photonic microcircuits based on liquid crystal optical microresonators, microlasers and microfibers, and opens up routes towards real soft matter photonic devices that are stable over extended time and temperatures.

Colloidal caterpillars for cargo transportation.

Tunable transport of tiny objects in fluid systems is demanding in diverse fields of science such as drug delivery, active matter far from equilibrium, and lab-on-a-chip applications. Here, we report the directed motion of colloidal particles and self-assembled colloidal chains in a nematic liquid crystal matrix using electrohydrodynamic convection (EHC) rolls. The asymmetric distortion of the molecular orientation around the particles results - for single particles - in a hopping motion from one EHC roll to the next and - for colloidal chains - in a caterpillar-like motion in the direction perpendicular to the roll axes. We demonstrate the use of colloidal chains as microtraction engines for the transport of various types of microcargo.

Resonant transport of light from planar polymer waveguide into liquid-crystal microcavity.

We demonstrate the resonant transfer of light from a planar waveguide to a nematic liquid-crystal microdroplet immersed in water. A wide spectrum of light from a supercontinuum laser source is coupled into a high-refractive-index polymer waveguide using a prism-film coupler. The waveguide is in contact with a water dispersion of droplets from the nematic liquid-crystal 5CB. The evanescent field of the light in the waveguide is resonantly coupled to the whispering-gallery mode resonances, sustained by 5 - 20 µm-sized nematic liquid-crystal droplets, which are in close proximity to the waveguide. The resonant transfer of light is tuned by the temperature-induced shifting of the WGM resonances due to the temperature dependence of the refractive index of the nematic liquid crystal. The measurements are compared to the calculations of the coupled-mode theory.

Laser-driven microflow-induced bistable orientation of a nematic liquid crystal in perfluoropolymer-treated unrubbed cells.

We demonstrate laser-driven microflow-induced orientational change (homeotropic to planar) in a dye-doped nematic liquid crystal. The homeotropic to planar director alignment is achieved in unrubbed cells in the thermal hysteresis range of a discontinuous anchoring reorientation transition due to the local heating by light absorption in dye-doped sample. Various bistable patterns were recorded in the cell by a programmable laser tweezers. The width of the patterns depend on the scanning speed of the tightly focussed laser beam and the minimum width obtained is approximately equal to 0.57µm which is about 35 times smaller than the earlier report in the rubbed cells. We show that the motion of the microbeam spot causes local flow as a result the liquid crystal director is aligned along that direction.

Lasing and waveguiding in smectic A liquid crystal optical fibers.

We demonstrate a new class of soft matter optical fibers, which are self-assembled in a form of smectic-A liquid crystal microtubes grown in an aqueous surfactant dispersion of a smectic-A liquid crystal. The diameter of the fibers is highly uniform and the fibers are highly birefringent. They are characterized by a line topological defect in the core of the fiber with an optical axis pointing from the defect core towards the surface. We demonstrate guiding of light along the fiber and Whispering Gallery Mode (WGM) lasing in a plane perpendicular to the fiber. The light guiding as well as the lasing threshold are significantly dependent on the polarization of the excitation beam. The observed threshold for WGM lasing is very low (≈ 75µJ/cm(2)) when the pump beam polarization is perpendicular to the direction of the laser dye alignment and is similar to the lasing threshold in nematic droplets. The smectic-A fibers are soft and flexible and can be manipulated with laser tweezers demonstrating a promising approach for realization of soft photonic circuits.

Chirality screening and metastable states in chiral nematic colloids.

We show that forces between two colloidal particles in a thin layer of a chiral nematic liquid crystal strongly depend on the chirality of the liquid crystal. The observed pair potentials are attractive, but are oscillatory functions of colloidal separation. The number and the position of local energy minima increase with increasing chirality. The pair interaction is the strongest for the pitch equal to the colloidal diameter and decreases with increasing chirality. We show that the chirality of the medium is responsible for this oscillatory nature and screening of the colloidal interaction in the far and near field. The measurements are in agreement with numerical calculations using Landau-de Gennes theory.

Light-induced rewiring and winding of Saturn ring defects in photosensitive chiral nematic colloids.

We study the winding and unwinding of Saturn ring defects around silica microspheres with homeotropic surface anchoring in a cholesteric liquid crystal with a variable pitch. We use mixtures of a nematic liquid crystal 5CB and various photoresponsive chiral dopants to vary the helical pitch and sense of the helical winding by illuminating the mixtures with UV or visible light. Upon illumination, we observe motion of the Grandjean-Cano disclination lines in wedge-like cells. When the line touches the colloidal particle, we observe topological reconstruction of the Grandjean-Cano line and the Saturn ring. The result of this topological reconstruction is either an increase or decrease of the degree of winding of the Saturn ring around the colloidal particle. This phenomenon is similar to topological rewiring of -1/2 disclination lines, observed recently in chiral nematic colloids.

Liquid crystal elastomer shell actuators with negative order parameter.

Liquid crystals (LCs) are nonsolids with long-range orientational order, described by a scalar order parameter 〈 P 2 〉 = 1 2 〈 3 cos 2 ß - 1 〉 . Despite the vast set of existing LC materials, one-third of the order parameter value range, -1/2 < 〈P 2〉 < 0, has until now been inaccessible. Here, we present the first material with negative LC order parameter in its ground state, in the form of elastomeric shells. The optical and actuation characteristics are opposite to those of conventional LC elastomers (LCEs). This novel class of anti-ordered elastomers gives access to the previously secluded range of liquid crystallinity with 〈P 2〉 < 0, providing new challenges for soft matter physics and adding a complementary type of LCE actuator that is attractive for applications in, e.g., soft robotics.

Large-scale self-organization of reconfigurable topological defect networks in nematic liquid crystals.

Topological defects in nematic liquid crystals are ubiquitous. The defects are important in understanding the fundamental properties of the systems, as well as in practical applications, such as colloidal self-assembly, optical vortex generation and templates for molecular self-assembly. Usually, spatially and temporally stable defects require geometrical frustration imposed by surfaces; otherwise, the system relaxes because of the high cost of the elastic energy. So far, multiple defects are kept in bulk nematic liquid crystals by top-down lithographic techniques. In this work, we stabilize a large number of umbilical defects by doping with an ionic impurity. This method does not require pre-patterned surfaces. We demonstrate that molecular reorientation controlled by an AC voltage induces periodic density modulation of ions accumulated at an electrically insulating polymer interface, resulting in self-organization of a two-dimensional square array of umbilical defects that is reconfigurable and tunable.

Viscoelasticity of ambient-temperature nematic binary mixtures of bent-core and rodlike molecules.

We report measurements of the temperature variations of physical parameters in ambient-temperature nematic liquid crystal mixtures of bent-core (BC) and rodlike molecules (5CB): birefringence Δn; static dielectric constants ε(||) and ε(⊥); splay K(11) and bend K(33) elastic constants; rotational viscosity γ(1); and diffusion coefficients D(||) and D(⊥) of a microsphere. Both Δn and ε(||) decreases rapidly with increasing BC concentration, whereas ε(⊥) remains almost constant. At a shifted temperature (e.g., T-T(NI)=-10 °C), K(11) increases by ~50% and K(33) decreases by ~80% compared to pure 5CB when the BC concentration is increased to ~43 mol % in the mixture. Viscosities parallel and perpendicular to the director, η(||), η(⊥), which are nearly equal to the Miesowicz viscosities η(2) and η(3), respectively, were obtained by D(||) and D(⊥) using the Stokes-Einstein relation. Both the viscosities at room temperature increase by 60 and 50 times, respectively, whereas γ(1) increases by 180 times (at ~43 mol %) compared to the corresponding values of pure 5CB. The stiffening of K(11) and exorbitantly large enhancement in all the viscosities at a higher mol % of BC indicate that the viscoelastic properties are highly impacted by the presence of smectic clusters of BC molecules that results from the restricted free rotation of the molecules along the bow axis in the nematic phase. A possible attachment model of smectic type clusters of BC molecules surrounding the microparticle is presented.

Colloidal entanglement in highly twisted chiral nematic colloids: twisted loops, Hopf links, and trefoil knots.

The topology and geometry of closed defect loops is studied in chiral nematic colloids with variable chirality. The colloidal particles with perpendicular surface anchoring of liquid crystalline molecules are inserted in a twisted nematic cell with the thickness that is only slightly larger than the diameter of the colloidal particle. The total twist of the chiral nematic structure in cells with parallel boundary conditions is set to 0, π, 2π, and 3π, respectively. We use the laser tweezers to discern the number and the topology of the -1/2 defect loops entangling colloidal particles. For a single colloidal particle, we observe that a single defect loop is winding around the particle, with the winding pattern being more complex in cells with higher total twist. We observe that colloidal dimers and colloidal clusters are always entangled by one or several -1/2 defect loops. For colloidal pairs in π-twisted cells, we identify at least 17 different entangled structures, some of them exhibiting linked defect loops-Hopf link. Colloidal entanglement is even richer with a higher number of colloidal particles, where we observe not only linked, but also colloidal clusters knotted into the trefoil knot. The experiments are in good agreement with numerical modeling using Landau-de Gennes theory coupled with geometrical and topological considerations using the method of tetrahedral rotation.