SearcharxivSearch

arXiv subjects

Arjun G. Yodh

Publications and source records attributed to Arjun G. Yodh.

7 recordsLinked to original sources

Arrested coalescence drives helical coiling and networking of filamentous smectic condensates

Liquid-liquid crystal phase separation (LLCPS) occurs in many industrial and biological settings. Interestingly, when smectic phases demix from the homogeneous mixture, they can form filamentous condensates that spontaneously assemble into sparse networks with rich life-like dynamics. Here, we study the underlying process of filament networking. Microscopy reveals that new linkages between filaments are initiated by an adhesive interaction between straight filaments; parallel filaments snap into contact and then rapidly wind into helical coils, despite the absence of molecular chirality or transitions between mesophases. Using polarized optical microscopy, theoretical modeling, and simulation, we show that parallel filaments coalesce, but are arrested in double-barreled ``ribbon'' structures. This arrested coalescence is driven purely by interfacial energy minimization under the constraints of smectic layering. The arrested ribbons spontaneously coil into double helices to further reduce interfacial area, thus driving compaction into networks. We propose a microstructure consistent with this interpretation, which quantitatively predicts the extent of arrested coalescence. In total, these findings suggest a generic pathway for network formation in liquid crystals that provides insight about the formation of condensate networks in other engineered or biological materials.

cond-mat.soft

Scaling of relaxation and excess entropy in plastically deformed amorphous solids

When stressed sufficiently, solid materials yield and deform plastically via reorganization of microscopic constituents. Indeed, it is possible to alter the micro-structure of materials by judicious application of stress, an empirical pro- cess utilized in practice to enhance the mechanical properties of metals. Un- derstanding the interdependence of plastic flow and microscopic structure in these non-equilibrium states, however, remains a major challenge. Here, we ex- perimentally investigate this relationship, between the relaxation dynamics and microscopic structure of disordered colloidal solids during plastic deformation. We apply oscillatory shear to solid colloidal monolayers and study their particle trajectories as a function of shear rate in the plastic regime. Under these cir- cumstances, the strain rate, the relaxation rate associated with plastic flow, and the sample microscopic structure oscillate together but with different phases. Interestingly, the experiments reveal that the relaxation rate associated with plastic flow at time t is correlated with the strain rate and sample microscopic structure measured at earlier and later times, respectively. The relaxation rate, in this non-stationary condition, exhibits power-law shear-thinning behavior and scales exponentially with sample excess entropy. Thus, measurement of sample static structure (excess entropy) provides insight about both strain-rate and constituent rearrangement dynamics in the sample at earlier times.

cond-mat.soft

Elasticity-Dependent Self-assembly of Micro-Templated Chromonic Liquid Crystal Films

We explore micropatterned director structures of aqueous lyotropic chromonic liquid crystal (LCLC) films created on square lattice cylindrical-micropost substrates. The structures are manipulated by modulating the LCLC mesophases and their elastic properties via concentration through drying. Nematic LCLC films exhibit preferred bistable alignment along the diagonals of the micropost lattice. Columnar LCLC films, dried from nematics, form two distinct director and defect configurations: a diagonally aligned director pattern with local squares of defects, and an off-diagonal configuration with zig-zag defects. The formation of these states appears to be tied to the relative splay and bend free energy costs of the initial nematic films. The observed nematic and columnar configurations are understood numerically using a Landau-de Gennes free energy model. Among other attributes, the work provide first examples of quasi-2D micropatterning of LC films in the columnar phase and lyotropic LC films in general, and it demonstrates alignment and configuration switching of typically difficult-to-align LCLC films via bulk elastic properties.

cond-mat.soft

Phonon Spectra, Nearest Neighbors, and Mechanical Stability of Disordered Colloidal Clusters with Attractive Interactions

We investigate the influence of morphology and size on the vibrational properties of disordered clusters of colloidal particles with attractive interactions. From measurements of displacement correlations between particles in each cluster, we extract vibrational properties of the corresponding "shadow" glassy cluster, with the same geometric configuration and interactions as the "source" cluster but without damping. Spectral features of the vibrational modes are found to depend strongly on the average number of nearest neighbors, $\bar{NN}$, but only weakly on the number of particles in each glassy cluster. In particular, the median phonon frequency, $ω_{med}$, is essentially constant for $\bar{NN}$ $<2$ and then grows linearly with $\bar{NN}$ for $\bar{NN}$ $>2$. This behavior parallels concurrent observations about local isostatic structures, which are absent in clusters with $\bar{NN}$ $<2$ and then grow linearly in number for $\bar{NN}$$>2$. Thus, cluster vibrational properties appear to be strongly connected to cluster mechanical stability (i.e., fraction of locally isostatic regions), and the scaling of $ω_{med}$ with $\bar{NN}$ is reminiscent of the behavior of packings of spheres with repulsive interactions at the jamming transition. Simulations of random networks of springs corroborate observations and suggest that connections between phonon spectra and nearest neighbor number are generic to disordered networks.

cond-mat.soft

Helical Packings and Phase Transformations of Soft Spheres in Cylinders

The phase behavior of helical packings of thermoresponsive microspheres inside glass capillaries is studied as a function of volume fraction. Stable packings with long-range orientational order appear to evolve abruptly to disordered states as particle volume fraction is reduced, consistent with recent hard sphere simulations. We quantify this transition using correlations and susceptibilities of the orientational order parameter psi_6. The emergence of coexisting metastable packings, as well as coexisting ordered and disordered states, is also observed. These findings support the notion of phase transition-like behavior in quasi-1D systems.

cond-mat.soft

Geometric Frustration in Buckled Colloidal Monolayers

Geometric frustration arises when lattice structure prevents simultaneous minimization of local interactions. It leads to highly degenerate ground states and, subsequently, complex phases of matter such as water ice, spin ice and frustrated magnetic materials. Here we report a simple geometrically frustrated system composed of closely packed colloidal spheres confined between parallel walls. Diameter-tunable microgel spheres are self-assembled into a buckled triangular lattice with either up or down displacements analogous to an antiferromagnetic Ising model on a triangular lattice. Experiment and theory reveal single-particle dynamics governed by in-plane lattice distortions that partially relieve frustration and produce ground-states with zigzagging stripes and subextensive entropy, rather than the more random configurations and extensive entropy of the antiferromagnetic Ising model. This tunable soft matter system provides an uncharted arena in which the dynamics of frustration, thermal excitations and defects can be directly visualized.

cond-mat.soft

Electronic Devices Based on Purified Carbon Nanotubes Grown By High Pressure Decomposition of Carbon Monoxide

The excellent properties of transistors, wires, and sensors made from single-walled carbon nanotubes (SWNTs) make them promising candidates for use in advanced nanoelectronic systems. Gas-phase growth procedures such as the high pressure decomposition of carbon monoxide (HiPCO) method yield large quantities of small diameter semiconducting SWNTs, which are ideal for use in nanoelectronic circuits. As-grown HiPCO material, however, commonly contains a large fraction of carbonaceous impurities that degrade properties of SWNT devices. Here we demonstrate a purification, deposition, and fabrication process that yields devices consisting of metallic and semiconducting nanotubes with electronic characteristics vastly superior to those of circuits made from raw HiPCO. Source-drain current measurements on the circuits as a function of temperature and backgate voltage are used to quantify the energy gap of semiconducting nanotubes in a field effect transistor geometry. This work demonstrates significant progress towards the goal of producing complex integrated circuits from bulk-grown SWNT material.

cond-mat.mes-hall