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Circular dichroism is a technologically important phenomenon contrasting the absorption and resultant emission properties between left- and right-handed circularly polarized light. While the chiral handedness of systems mainly determines the mechanism of the circular dichroism in linear optics, the counterpart in the nonlinear optical regime is nontrivial. Here, in contrast to traditional nonlinear circular dichroism responses from structured surfaces, we report on an unprecedented bulk-material-induced circular dichroism of second harmonic generation with a massive g-factor up to 1.8.

Sessile droplets of a ferroelectric nematic liquid crystalline material were exposed to surface electric fields produced by pyroelectric and photogalvanic (photovoltaic) effects in X-cut iron-doped lithium niobate crystals. The resulting dynamic processes were monitored by polarization optical (video)microscopy (POM). During heating/cooling cycles, at first, the droplets change their shape from spherical to extended ellipsoidal. Then they start to move rapidly along the surface electric field, i.e., along the crystal's polar axis (c-axis). During this motion, several droplets merge into running streams (tendrils) extending towards the edges of the top surface area. Finally, practically all liquid crystalline material is transported from the top surface to the side surfaces of the crystal. At stabilized temperature, laser illumination of the assembly causes dynamic processes that are localized to the illuminated area. Also, in this case, the LC droplets merge into several tendril-like formations that are preferentially oriented along the c-axis of the crystal. The pattern of tendrils fluctuates with time, but it persists as long as the illumination is present. In this case, the LC material is transported between the central and the edge region of the illuminated area., 16 pages, 5 figures. arXiv admin note: text overlap with arXiv:2208.02318

Second-order optical nonlinearity is the essential concept for realizing modern technologies of optical wavelength conversion. The emerging helical polarization fluid, dubbed helielectric nematic, now makes it possible to design and easily fabricate various polarization structures and control their optical responses. The matter family is demonstrated as an ideal liquid platform for nonlinear optical conversion and amplification with electric-reconfigurable tunability. We here develop a universal phase matching theory and reveal a nonclassic chirality-sensitive phase-matching condition in the polarization helices through both the numerical calculation and the experimental validations. The nonlinear optical amplification can be dramatically modulated with a contrast ratio of >100:1 by an in-plane electric field. Furthermore, we employ the director relaxation under electric fields coupled with nonlinear optical simulation to clarify the topology–light interactions.

The generation of spatially localized, soliton-like hydrodynamic disturbances in microscale fluidic systems is an intriguing challenge. Herein, we introduce nonequilibrium solitons in nematic liquid crystals stimulated by an electric field. These dynamic solitons are robust as long as the electric field is maintained. Interestingly, their kinetic behaviours depend on the field condition—Tuning of the amplitude and frequency of the applied electric field alters the solitons to self-assemble into lattice ordering like physical particles or to command them to various dynamic states. Our key property to the realisation is the electrohydrodynamic instability due to the coupling between the fluid elasticity and the background convection. This paper describes a new mechanism for realising dynamic solitons in fluid systems on the basis of the electrohydrodynamic phenomena., Electric field induced convective instabilities in liquid crystal slabs can assume a localized shape. The authors show how to generate, manipulate and shepard these dissipative solitary excitations that do not require topological constraints for stabilization.

Just like in living organisms, if precise coherent operation of tiny movable components is possible, one may generate a macroscopic mechanical motion. Here we report that ~1010 pieces of colloidally dispersed nanosheets in aqueous media can be made to operate coherently to generate a propagating macroscopic wave under a non-equilibrium state. The nanosheets are initially forced to adopt a monodomain cofacial geometry with a large and uniform plane-to-plane distance of ~420 nm, where they are strongly correlated by competitive electrostatic repulsion and van der Waals attraction. When the electrostatic repulsion is progressively attenuated by the addition of ionic species, the nanosheets sequentially undergo coherent motions, generating a propagating wave. This elaborate wave in time and space can transport microparticles over a long distance in uniform direction and velocity. The present discovery may provide a general principle for the design of macroscopically movable devices from huge numbers of tiny components., Tiny movable components could generate macroscopic mechanical motion if precise coherent operation can be exerted simultaneously. Here, the authors demonstrate this by using 10^10 pieces of colloidally dispersed nanosheets to generate wave under non-equilibrium state.

Significance The recent discovery of the emerging ferroelectric nematics opens an avenue not only for exploring exotic polar matter states in condensed matter physics but also for providing opportunities toward brand new liquid crystal technologies. Here, we revealed the existence of a helielectric nematic state by introducing the chirality into the ferroelectric nematics. Combining multiple intercorrelated measurements, we confirmed a helicoidal-type polar vector field in the helielectric nematics. The emergent polar symmetry triggers distinctions in topology to the dielectric cholesterics. Via proper doping of chiral generators, the helielectric state can survive down to room temperature, retaining excellent nonlinear optical and dielectric properties. Hence, it offers a stable material platform for exploring unidentified polarity–chirality–coupled textures and developing functional electrooptical devices.

Pearl-shaped polar molecules with high enough dipole moment enable the creation of the giant-ε ferroelectric nematics., Superhigh-ε materials that exhibit exceptionally high dielectric permittivity are recognized as potential candidates for a wide range of next-generation photonic and electronic devices. In general, achieving a high-ε state requires low material symmetry, as most known high-ε materials are symmetry-broken crystals. There are few reports on fluidic high-ε dielectrics. Here, we demonstrate how small molecules with high polarity, enabled by rational molecular design and machine learning analyses, enable the development of superhigh-ε fluid materials (dielectric permittivity, ε > 104) with strong second harmonic generation and macroscopic spontaneous polar ordering. The polar structures are confirmed to be identical for all the synthesized materials. Furthermore, adapting this strategy to high–molecular weight systems allows us to generalize this approach to polar polymeric materials, creating polar soft matters with spontaneous symmetry breaking.

Smart viscoelastic materials that respond to specific stimuli are one of the most attractive classes of materials important to future technologies, such as on-demand switchable adhesion technologies, actuators, molecular clutches, and nano-/microscopic mass transporters. Recently it was found that through a special solid-liquid transition, rheological properties can exhibit significant changes, thus providing suitable smart viscoelastic materials. However, designing materials with such a property is complex, and forward and backward switching times are usually long. Therefore, it is important to explore new working mechanisms to realize solid-liquid transitions, shorten the switching time, and enhance the contrast of rheological properties during switching. Here, a light-induced crystal-liquid phase transition is observed, which is characterized by means of polarizing light microscopy (POM), photorheometry, photo-differential scanning calorimetry (photo-DSC), and X-ray diffraction (XRD). The light-induced crystal-liquid phase transition presents key features such as (1) fast switching of crystal-liquid phases for both forward and backward reactions and (2) a high contrast ratio of viscoelasticity. In the characterization, POM is advantageous in offering information on the spatial distribution of LC molecule orientations, determining the type of liquid crystalline phases appearing in the material, and studying the orientation of LCs. Photorheometry allows measurement of a material's rheological properties under light stimuli and can reveal the photorheological switching properties of materials. Photo-DSC is a technique to investigate thermodynamic information of materials in darkness and under light irradiation. Lastly, XRD allows studying of microscopic structures of materials. The goal of this article is to clearly present how to prepare and measure the discussed properties of a photorheological material.

The construction of hierarchical nanostructures with precise morphological and dimensional control has been one of the ultimate goals of contemporary materials science and chemistry, and the emulation of tailor-made nanoscale superstructures realized in the nature, using artificial building blocks, poses outstanding challenges. Herein we report a one-pot strategy to precisely synthesize hierarchical nanostructures through an in-situ initiation-growth process from a liquid crystalline block copolymer. The assembly process, analogous to living chain polymerization, can be triggered by small-molecule, macromolecule or even nanoobject initiators to produce various hierarchical superstructures with highly uniform morphologies and finely tunable dimensions. Because of the high degree of controllability and predictability, this assembly strategy opens the avenue to the design and construction of hierarchical structures with broad utility and accessibility., Construction of hierarchical nanostructures is important in material science, but precise morphological control remains a challenge. Here, the authors report a one-pot in-situ initiation-growth process from a liquid crystalline block copolymer to precisely control the morphology and dimensions of hierarchical nanostructures.

Azodendrimer is a class of branched polymer, whose structure can be modulated by light irradiation. Recently, a new type of liquid crystalline dendrimers that serve as a command surface has been reported. They received tremendous attention due to the fundamental interests of the variation of their properties (e.g., alignment, topology) in response to light. Here, we explore the properties of the surface anchoring, molecular conformation and the phase structure of a model azodendrimer. We proposed a proper molecular conformation of the azodendrimer based on density functional theory analysis and molecular dynamics. Also, we reveal (1) the minimum coverage ratio of the dendrimer for inducing homeotropic alignment of host liquid crystals and the polar anchoring strength; (2) unlike typical low-molecular-weight LC molecules, different conformational states can coexist at single liquid crystalline phase; (3) the phase transition behavior of the azodendrimer is significantly affected by cooling rate because the molecular kinetics cannot follow too fast cooling.

In liquid crystal (LC) physical chemistry, molecules near the surface play a great role in controlling bulk orientation. Thus far, mainly to achieve desired molecular orientation states in LC displays, the "static" surface property of LCs, so-called surface anchoring, has been intensively studied. As a rule of thumb, once the initial orientation of LCs is "locked" by specific surface treatments, such as rubbing or treatment with a specific alignment layer, it hardly changes with temperature. Here, we present a system exhibiting an orientational transition upon temperature variation, which conflicts with the consensus. Right on the transition, the bulk LC molecules experience the orientational rotation, with 90° between the planar (P) orientation at high temperatures and the vertical (V) orientation at low temperatures in the first-order transitional manner. We have tracked thermodynamic surface anchoring behavior by means of polarizing optical microscopy (POM), dielectric spectroscopy (DS), high-resolution differential scanning calorimetry (HR-DSC), and grazing incidence X-ray diffraction (GI-XRD) and reached a plausible physical explanation: that the transition is triggered by a growth of surface wetting sheets, which impose the V orientation locally against the P orientation in the bulk. This landscape would provide a general link explaining how the equilibrium bulk orientation is affected by surface-localized orientation in many LC systems. In our characterization, POM and DS are advantageous by offering information on the spatial distribution of the orientation of LC molecules. HR-DSC gives information about the precise thermodynamic information on transitions, which cannot be addressed by conventional DSC instruments due to limited resolution. GI-XRD provides information on surface-specific molecular orientation and short-range orderings. The goal of this paper is to present a protocol for preparing a sample that exhibits the transition and to demonstrate how the thermodynamic structural variation, both in the bulk and on surfaces, can be analyzed through the abovementioned methods.

We report that an asymmetric bent dimer, consisting of a rod mesogen and a cholesterol mesogen linked by a flexible spacer with 9 carbon atoms, was found to form blue phases with a record-wide temperature range. Moreover, highly stable, fast electro-optic switching is possible. In addition to the stable Kerr effect, the electrostriction effect was also observed.