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1.
ACS Nano ; 18(16): 10768-10775, 2024 Apr 23.
Artículo en Inglés | MEDLINE | ID: mdl-38597971

RESUMEN

Solitons in nematic liquid crystals facilitate the rapid transport and sensing in microfluidic systems. Little is known about the elementary conditions needed to create solitons in nematic materials. In this study, we apply a combination of theory, computational simulations, and experiments to examine the formation and propagation of solitary waves, or "solitons", in nematic liquid crystals under the influence of an alternating current (AC) electric field. We find that these solitary waves exhibit "butterfly"-like or "bullet"-like structures that travel in the direction perpendicular to the applied electric field. Such structures propagate over long distances without losing their initial shape. The theoretical framework adopted here helps identify several key factors leading to the formation of solitons in the absence of electrostatic interactions. These factors include surface irregularities, flexoelectric polarization, unequal elastic constants, and negative anisotropic dielectric permittivity. The results of simulations are shown to be in good agreement with our own experimental observations, serving to establish the validity of the theoretical concepts and ideas advanced in this work.

2.
Soft Matter ; 20(2): 397-406, 2024 Jan 03.
Artículo en Inglés | MEDLINE | ID: mdl-38105746

RESUMEN

The optical properties of liquid crystals serve as the basis for display, diagnostic, and sensing technologies. Such properties are generally controlled by relying on electric fields. In this work, we investigate the effects of microfluidic flows and acoustic fields on the molecular orientation and the corresponding optical response of nematic liquid crystals. Several previously unknown structures are identified, which are rationalized in terms of a state diagram as a function of the strengths of the flow and the acoustic field. The new structures are interpreted by relying on calculations with a free energy functional expressed in terms of the tensorial order parameter, using continuum theory simulations in the Landau-de Gennes framework. Taken together, the findings presented here offer promise for the development of new systems based on combinations of sound, flow, and confinement.

3.
Phys Rev Lett ; 131(18): 188101, 2023 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-37977640

RESUMEN

Solitons in liquid crystals have generated considerable interest. Several hypotheses of varying complexity have been advanced to explain how they arise, but consensus has not emerged yet about the underlying forces responsible for their formation or their structure. In this work, we present a minimal model for solitons in achiral nematic liquid crystals, which reveals the key requirements needed to generate them in the absence of added charges. These include a surface inhomogeneity, consisting of an adsorbed particle capable of producing a twist, flexoelectricity, dielectric contrast, and an applied ac electric field that can couple to the director's orientation. Our proposed model is based on a tensorial representation of a confined liquid crystal, and it predicts the formation of "butterfly" structures, quadrupolar in character, in regions of a slit channel where the director is twisted by the surface imperfection. As the applied electric field is increased, solitons (or "bullets") become detached from the wings of the butterfly, and then propagate rapidly throughout the system. The main observations that emerge from the model, including the formation and structure of butterflies, bullets, and stripes, as well as the role of surface inhomogeneity and the strength of the applied field, are consistent with experimental findings presented here for nematic LCs confined between two chemically treated parallel plates.

4.
Phys Rev Lett ; 131(9): 098101, 2023 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-37721844

RESUMEN

Solitons are highly confined, propagating waves that arise from nonlinear feedback in natural (e.g., shallow and confined waters) and engineered systems (e.g., optical wave propagation in fibers). Solitons have recently been observed in thin films of liquid crystals (LCs) in the presence of ac electric fields, where localized LC director distortions arise and propagate due to flexoelectric polarization. Here we report that collisions between LC solitons and interfaces to isotropic fluids can generate a range of interfacial hydrodynamic phenomena. We find that single solitons can either generate single droplets or, alternatively, form jets of LC that subsequently break up into organized assemblies of droplets. We show that the influence of key parameters, such as electric field strength, LC film thickness, and LC-oil interfacial tension, map onto a universal state diagram that characterizes the transduction of soliton flexoelectric energy into droplet interfacial energy. Overall, we reveal that solitons in LCs can be used to focus the energy of nonlocalized electric fields to generate a new class of nonlinear electrohydrodynamic effects at fluid interfaces, including jetting and emulsification.

5.
Langmuir ; 38(11): 3575-3584, 2022 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-35263108

RESUMEN

AC electric fields cause three-dimensional orientational fluctuations (solitons) to form and rapidly propagate in confined films of liquid crystals (LCs), offering the basis of a new class of active soft matter (e.g., for accelerating mixing and transport processes in microscale chemical systems). How surface chemistry impacts the formation and trajectories of solitons, however, is not understood. Here, we show that self-assembled monolayers (SAMs) formed from alkanethiols on gold, which permit precise control over surface chemistry, are electrochemically stable over voltage and frequency windows (<100 V; 1 kHz) that lead to soliton formation in achiral nematic films of 4'-butyl-4-heptyl-bicyclohexyl-4-carbonitrile (CCN-47). By comparing soliton formation in LC films confined by SAMs formed from hexadecanethiol (C16SH) or pentadecanethiol (C15SH), we reveal that the electric field required for soliton formation increases with the LC anchoring energy: surfaces patterned with regions of C16SH and C15SH SAMs thus permit spatially controlled creation and annihilation of solitons necessary to generate a net flux of solitons. We also show that solitons propagate in orthogonal directions when confined by obliquely deposited gold films decorated with SAMs formed from C16SH or C15SH and that the azimuthal direction of propagation of solitons within achiral LC films possessing surface-induced twists is not unique but reflects variation in the spatial location of the solitons across the thickness of the twisted LC film. Finally, discontinuous changes in LC orientation induced by patterned surface anchoring lead to a range of new soliton behaviors including refraction, reflection, and splitting of solitons at the domain boundaries. Overall, our results provide new approaches for the controlled generation and programming of solitons with complex and precise trajectories, principles that inform new designs of chemical soft matter.

6.
Phys Rev Lett ; 126(22): 227801, 2021 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-34152186

RESUMEN

Topological defects in active liquid crystals can be confined by introducing gradients of activity. Here, we examine the dynamical behavior of two defects confined by a sharp gradient of activity that separates an active circular region and a surrounding passive nematic material. Continuum simulations are used to explain how the interplay among energy injection into the system, hydrodynamic interactions, and frictional forces governs the dynamics of topologically required self-propelling +1/2 defects. Our findings are rationalized in terms of a phase diagram for the dynamical response of defects in terms of activity and frictional damping strength. Different regions of the underlying phase diagram correspond to distinct dynamical modes, namely immobile defects, steady rotation of defects, bouncing defects, bouncing-cruising defects, dancing defects, and multiple defects with irregular dynamics. These dynamic states raise the prospect of generating synchronized defect arrays for microfluidic applications.

7.
Langmuir ; 36(25): 7074-7082, 2020 Jun 30.
Artículo en Inglés | MEDLINE | ID: mdl-31990557

RESUMEN

Liquid crystals (LCs) are easily influenced by external interactions, particularly at interfaces. When rod-like LC molecules are confined to spherical droplets, they experience a competition between interfacial tension and elastic deformations. The configuration of LCs inside a droplet can be controlled using surfactants that influence the interfacial orientation of the LC molecules in the oil-phase of an oil in water emulsion. Here, we used the surfactant sodium dodecyl sulfate (SDS) to manipulate the orientation of 5CB molecules in a polydisperse emulsion and examined the configuration of the droplets as a function of SDS concentration. We triggered pronounced morphological transitions by altering the SDS concentration while observing an individual LC droplet held in place using an optical tweezer. We compared the experimental configuration changes to predictions from simulations. We observed a hysteresis in the SDS concentration that induced the morphological transition from radial to bipolar and back as well as a fluctuations in the configuration during the transition.

8.
Phys Rev E ; 97(6-1): 062704, 2018 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-30011549

RESUMEN

We modeled the experimentally observed self-assembly of nanoparticles (NPs) into shells with diameters up to 10 µm, via segregation from growing nematic domains. Using field-based Monte Carlo simulations, we found the equilibrium configurations of the system by minimizing a free-energy functional that includes effects of excluded-volume interactions among NPs, orientational elasticity, and the isotropic-nematic phase-transition energy. We developed a Gaussian-profile approximation for the liquid crystal (LC) order-parameter field that provides accurate analytical values for the free energy of LC droplets and the associated microshells. This analytical model reveals a first-order transition between equilibrium states with and without microshells, governed mainly by the competition of excluded-volume and phase-transition energies. By contrast, the LC elasticity effects are much smaller and mostly confined to setting the size of the activation barrier for the transition. In conclusion, field-based thermodynamic methods provide a theoretical framework for the self-assembly of NP shells in liquid crystal hosts and suggest that field-based kinetic methods could be useful to simulate and model the time evolution of NP self-assembly coupled to phase separation.

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