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Lisa Tran

Publications and source records attributed to Lisa Tran.

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Lipid Hydrocarbon Tail Structure Governs Interfacial Anchoring and Stripe Morphology in Cholesteric Liquid Crystals

Liquid crystal-based biosensors exploit the sensitivity of interfacial anchoring to molecular adsorption. Cholesteric liquid crystals are especially useful because their helical structure supports multiple optically distinct textures that evolve with anchoring strength. Here, we compare saturated 1,2-dilauroyl-sn-glycero-3-phosphocholine (DLPC) and unsaturated 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) monolayers to determine how lipid acyl chain structure governs interfacial organization and director alignment. Mapping stripe spacing across lipid concentration, mixing ratio, cholesteric pitch, and confinement shows that the transition from fingerprint textures toward homeotropic alignment depends on both lipid structure and collective interfacial organization. DLPC produces comparatively regular textures and more readily promotes helix unwinding at high coverage, consistent with more spatially uniform collective anchoring. DOPC-containing interfaces show greater morphological heterogeneity, consistent with strong local anchoring from longer tails together with less uniform organization arising from cis-unsaturation. FRAP measurements provide complementary information on fluorescent-probe mobility, which becomes strongly restricted at high lipid concentration for both systems. Variations in pitch and film thickness further modulate the response, producing coexisting regular, distorted, and lipid-enriched textures. Together, these results show that lipid acyl chain structure regulates cholesteric anchoring through its effects on local interactions, collective interfacial organization, and mobility, providing design principles for responsive liquid-crystal interfaces.

cond-mat.soft

Lipid-Mediated Control of Thermally Induced Shape Transformations in Liquid Crystal Droplets

Lipids and liquid crystals provide a useful platform for addressing how molecular-scale organization is translated into mesoscale shape transformation. Variations in hydrocarbon-chain packing can modify interfacial order, anchoring conditions, and elastic stresses, potentially coupling molecular organization to droplet morphology. Here, we investigate the temperature-dependent structural evolution of monoolein-doped 4-octyl-4'-cyanobiphenyl (8CB) droplets dispersed in aqueous phospholipid solutions. Using polarized optical microscopy, we show that the internal monoolein concentration and the external lipid environment jointly regulate phase transitions, thin filamentation, and larger deformations during heating. The droplets undergo coupled smectic-nematic-isotropic transitions, with extended thin filaments observed exclusively in the smectic regime. At the smectic-to-nematic transition, we observe an abrupt and discontinuous onset of droplet shape deformation, revealing a shape-change transition coupled to the bulk mesophase transition. To our knowledge, this is the first report of a discontinuous droplet-shape-change transition coincident with a smectic-to-nematic phase transition. Varying the internal and external lipid contents redirects the reconfiguration pathway between filament-dominated smectic responses and more amorphous nematic shape changes. Interfacial tension measurements further show that stronger reductions in liquid-crystal-aqueous interfacial tension do not necessarily produce filamentation or deformation. Instead, the observed morphodynamics arise from the coupling between bulk elasticity, mesophase structure, and lipid-mediated interfacial organization. These findings establish lipid composition and hydrocarbon-chain architecture as key parameters governing thermally induced shape transformations in liquid crystal droplets.

cond-mat.soft

Tuning cholesteric cellulose nanocrystal self-assembly in spherical confinement via salt and sonication

Cellulose nanocrystals (CNCs) self-assemble into cholesteric liquid crystals that produce structural color upon solvent removal. Although most studies examine this process in planar films, confinement within micron-sized water-in-oil droplets provides a powerful platform for resolving self-assembly dynamics in real time. Here, we investigate how two common pitch-tuning strategies, sodium chloride addition and tip sonication, govern the kinetics and structure of CNC self-assembly under spherical confinement. Polarized optical microscopy timelapses capture the evolution from isotropic suspension through tactoid nucleation and annealing to kinetic arrest and final buckling. Consistent with prior work, pitch-concentration analysis reveals a universal post-arrest regime governed by droplet shrinkage. Beyond this established behavior, we identify a pre-arrest regime in which pitch decreases rapidly and whose kinetics accelerate with increasing salt concentration and sonication dose. These parameters shift the onset of cholesteric order and gelation, thereby tuning the concentration window for tactoid coalescence. Together, these results establish droplet confinement as a quantitative platform for probing out-of-equilibrium CNC self-assembly and for kinetically programming structurally colored soft materials.

cond-mat.soft

Controlling viscosity to engineer focal conic domains in photonic cellulose nanocrystal films

Cellulose nanocrystals (CNCs) form cholesteric architectures that can have color specific reflectivity and enable sustainable photonic films. However, achieving uniform color, suppressing iridescence, and accessing ordered defect structures such as focal conic domains remain challenging. Here, we control the photonic properties of CNC films by steering the self assembly process. Across 24 dish-cast films with varying salt concentrations and sonication doses, we combine viscosity measurements, timelapse polarized optical microscopy, and angle-resolved reflectance spectroscopy to correlate evaporation dynamics with photonic structure. We show that viscosity, jointly controlled by NaCl-mediated electrostatic screening and sonication-induced bundle fragmentation, dictates the extent of tactoid coalescence. Low-viscosity suspensions generate large, homogeneous cholesteric domains and narrow spectral responses, while high viscosity leads to arrested, heterogenous domains and increased diffuse light reflection. Critically, within a narrow parameter window of intermediate ionic strength and moderate sonication, we reproducibly engineer photonically active focal conic domains. These results identify viscosity-driven flow as a key, previously underappreciated factor in CNC self-assembly and establish design rules for producing structurally colored films with tunable photonic response, reduced iridescence, and controllable defect architectures.

cond-mat.soft

Shaping boundaries to control and transport topological defects in colloidal nematic liquid crystals

Anisotropic rod-like particles form liquid crystalline phases with varying degrees of orientational and translational order. When confined geometrically, these phases can give rise to topological defects, which can be selected and controlled by tuning how the rods align near boundaries, known as anchoring. While anchoring in molecular liquid crystals can be controlled through surface functionalization, this approach is not easily applicable to microscale colloidal systems, which have so far been limited to planar anchoring. Here, using particle-based simulations, Landau-de Gennes theory, and experiments on colloidal rods, we demonstrate that topographical patterning of the boundary can effectively control the anchoring type and, in turn, the defect state in two-dimensional confined nematics. Building on this, we numerically predict that dynamically shape-shifting the boundaries can transform and transport topological defects.

cond-mat.soft

Flexible, photonic films of surfactant-functionalized cellulose nanocrystals for pressure and humidity sensing

Most paints contain pigments that absorb light and fade over time. A robust alternative can be found in nature, where structural coloration arises from the interference of light with submicron features. Plant-derived, cellulose nanocrystals (CNCs) mimic these features by self-assembling into a cholesteric liquid crystal that exhibits structural coloration when dried. While much research has been done on CNCs in aqueous solutions, less is known about transferring CNCs to apolar solvents that are widely employed in paints. This study uses a common surfactant in agricultural and industrial products to suspend CNCs in toluene that are then dried into structurally colored films. Surprisingly, a stable liquid crystal phase is formed within hours, even with concentrations of up to 50 wt.-%. Evaporating the apolar CNC suspensions results in photonic films with peak wavelengths ranging from 660 to 920 nm. The resulting flexible films show increased mechanical strength, enabling a blue-shift into the visible spectrum with applied force. The films also act as humidity sensors, with increasing relative humidity yielding a red-shift. With the addition of a single surfactant, CNCs can be made compatible with existing production methods of industrial coatings, while improving the strength and responsiveness of structurally-colored films to external stimuli.

cond-mat.soft

Curvature directed anchoring and defect structure of colloidal smectic liquid crystals in confinement

Rod-like objects at high packing fractions can form smectic phases, where the rods break rotational and translational symmetry by forming lamellae. Smectic defects thereby include both discontinuities in the rod orientational order (disclinations), as well as in the positional order (dislocations). In this work, we use both experiments and simulations to probe how local and global geometrical frustrations affect defect formation in hard-rod smectics. We confine a particle-resolved, colloidal smectic within elliptical wells of varying size and shape for a smooth variation of the boundary curvature. We find that the rod orientation near a boundary - the anchoring - depends upon the boundary curvature, with an anchoring transition observed at a critical radius of curvature approximately twice the rod length. The anchoring controls the smectic defect structure. By analyzing local and global order parameters, and the topological charges and loops of networks made of the density maxima (rod centers) and density minima (rod ends), we quantify the amount of disclinations and dislocations formed with varying confinement geometry. More circular confinements, having only planar anchoring, promote disclinations, while more elliptical confinements, with antipodal regions of homeotropic anchoring, promote long-range smectic ordering and dislocation formation. Our findings demonstrate how geometrical constraints can control the anchoring and defect structures of liquid crystals - a principle that is applicable from molecular to colloidal length scales.

cond-mat.soft

Helfrich-Hurault elastic instabilities driven by geometrical frustration

The Helfrich-Hurault (HH) elastic instability is a well-known mechanism behind patterns that form as a result of strain upon liquid crystal systems with periodic ground states. In the HH model, layered structures undulate and buckle in response to local, geometric incompatibilities, in order to maintain the preferred layer spacing. Classic HH systems include cholesteric liquid crystals under electromagnetic field distortions and smectic liquid crystals under mechanical strains, where both materials are confined between rigid substrates. However, richer phenomena are observed when undulation instabilities occur in the presence of deformable interfaces and variable boundary conditions. Understanding how the HH instability is affected by deformable surfaces is imperative for applying the instability to a broader range of materials. In this review, we re-examine the HH instability and give special focus to how the boundary conditions influence the mechanical response of lamellar systems to geometrical frustration. We use lamellar liquid crystals confined within a spherical shell geometry as our model system. Made possible by the relatively recent advances in microfluidics within the past 15 years, liquid crystal shells are composed entirely of fluid interfaces and have boundary conditions that can be dynamically controlled at will. We examine past and recent work that exemplifies how topological constraints, molecular anchoring conditions, and boundary curvature can trigger the HH instability in liquid crystals with periodic ground states. We then end by identifying similar phenomena across a wide variety of materials, both biological and synthetic. With this review, we aim to highlight that the HH instability is a generic and often overlooked response of periodic materials to geometrical frustration.

cond-mat.soft

Undulation instabilities in cholesteric liquid crystals induced by anchoring transitions

Cholesteric liquid crystals (CLCs) have a characteristic length scale given by the pitch of the twisted stacking of their constituent rod-like molecules. Under homeotropic anchoring conditions where the molecules prefer to orient perpendicular to an interface, cholesteric interfaces exhibit striped phases with stripe widths commensurate with the pitch. Conversely, planar anchoring conditions have the molecules remain in the plane of the interface so that the CLC twists perpendicular to it. Recent work [L. Tran et al. Phys. Rev. X 7, 041029 (2017)] shows that varying the anchoring conditions dramatically rearranges the CLC stripe pattern, exchanging defects in the stripe pattern with defects in the molecular orientation of the liquid crystal molecules. We show with experiments and numerical simulations that the CLC stripes also undergo an undulation instability when we transition from homeotropic to planar anchoring conditions and vice versa. The undulation can be interpreted as a transient relaxation of the CLC resulting from a strain in the cholesteric layers due to a tilting pitch axis, with properties analogous to the classic Helfrich-Hurault instability. We focus on CLC shells in particular and show that the spherical topology of the shell also plays an important role in shaping the undulations.

cond-mat.soft

Swelling cholesteric liquid crystal shells to direct colloids at the interface

Cholesteric liquid crystals can exhibit spatial patterns in molecular alignment at interfaces that can be exploited for particle assembly. These patterns emerge from the competition between bulk and surface energies, tunable with the system geometry. In this work, we use the osmotic swelling of cholesteric double emulsions to assemble colloidal particles through a pathway-dependent process. Particles can be repositioned from a surface-mediated to an elasticity-mediated state through dynamically thinning the cholesteric shell at a rate comparable to that of colloidal adsorption. By tuning the balance between surface and bulk energies with the system geometry, colloidal assemblies on the cholesteric interface can be molded by the underlying elastic field to form linear aggregates. The transition of adsorbed particles from surface regions with homeotropic anchoring to defect regions is accompanied by a reduction in particle mobility. The arrested assemblies subsequently map out and stabilize topological defects. These results demonstrate the kinetic arrest of interfacial particles within definable patterns by regulating the energetic frustration within cholesterics. This work highlights the importance of kinetic pathways for particle assembly in liquid crystals, of relevance to optical and energy applications.

cond-mat.soft

Shaping nanoparticle fingerprints at the interface of cholesteric droplets

The ordering of nanoparticles into predetermined configurations is of importance to the design of advanced technologies. In this work, we moderate the surface anchoring against the bulk elasticity of liquid crystals to dynamically shape nanoparticle assemblies at a fluid interface. By tuning the degree of nanoparticle hydrophobicity with surfactants that alter the molecular anchoring of liquid crystals, we pattern nanoparticles at the interface of cholesteric liquid crystal emulsions. Adjusting the particle hydrophobicity more finely further modifies the rigidity of assemblies. We establish that patterns are tunable by varying both surfactant and chiral dopant concentrations. Since particle assembly occurs at the interface with the desired structures exposed to the surrounding phase, we demonstrate that particles can be readily crosslinked and manipulated, forming structures that retain their shape under external perturbations. This study establishes the templating of nanomaterials into reconfigurable arrangements. Interfacial assembly is tempered by elastic patterns that arise from the geometric frustration of confined cholesterics. This work serves as a basis for creating materials with chemical heterogeneity and with linear, periodic structures, essential for optical and energy applications.

cond-mat.soft

A change in stripes for cholesteric shells via anchoring in moderation

Chirality, ubiquitous in complex biological systems, can be controlled and quantified in synthetic materials such as cholesteric liquid crystal (CLC) systems. In this work, we study spherical shells of CLC under weak anchoring conditions. We induce anchoring transitions at the inner and outer boundaries using two independent methods: by changing the surfactant concentration or by raising the temperature close to the clearing point. The shell confinement leads to new states and associated surface structures: a state where large stripes on the shell can be filled with smaller, perpendicular sub-stripes, and a focal conic domain (FCD) state, where thin stripes wrap into at least two, topologically required, double spirals. Focusing on the latter state, we use a Landau-de Gennes model of the CLC to simulate its detailed configurations as a function of anchoring strength. By abruptly changing the topological constraints on the shell, we are able to study the interconversion between director defects and pitch defects, a phenomenon usually restricted by the complexity of the cholesteric phase. This work extends the knowledge of cholesteric patterns, structures that not only have potential for use as intricate, self-assembly blueprints but are pervasive in biological systems.

cond-mat.soft

Lassoing saddle splay and the geometrical control of topological defects

Systems with holes, such as colloidal handlebodies and toroidal droplets, have been studied in the nematic liquid crystal (NLC) 4-cyano-4'-pentylbiphenyl (5CB): both point and ring topological defects can occur within each hole and around the system, while conserving the system's overall topological charge. However, what has not been fully appreciated is the ability to manipulate the hole geometry with homeotropic (perpendicular) anchoring conditions to induce complex, saddle-like deformations. We exploit this by creating an array of holes suspended in an NLC cell with oriented planar (parallel) anchoring at the cell boundaries. We study both 5CB and a binary mixture of bicyclohexane derivatives (CCN-47 and CCN-55). Through simulations and experiments, we study how the bulk saddle deformations of each hole interact to create novel defect structures, including an array of disclination lines, reminiscent of those found in liquid crystal blue phases. The line locations are tunable via the NLC elastic constants, the cell geometry, and the size and spacing of holes in the array. This research lays the groundwork for the control of complex elastic deformations of varying length scales via geometrical cues in materials that are renowned in the display industry for their stability and easy manipulability.

cond-mat.soft