arXiv subjects

Vinothan N. Manoharan

Publications and source records attributed to Vinothan N. Manoharan.

27 records · Page 2Linked to original sources

arXiv2016

Colloidal particle adsorption at liquid interfaces: Capillary driven dynamics and thermally activated kinetics

The adsorption of single colloidal microparticles (0.5--1 $μ$m radius) at a water-oil interface has been recently studied experimentally using digital holographic microscopy [Kaz \textit{et al., Nat. Mater.}, 2012, \textbf{11}, 138--142]. An initially fast adsorption dynamics driven by capillary forces is followed by an unexpectedly slow relaxation to equilibrium that is logarithmic in time and can span hours or days. The slow relaxation kinetics has been attributed to the presence of surface "defects" with nanoscale dimensions (1--5\,nm) that induce multiple metastable configurations of the contact line perimeter. A kinetic model considering thermally activated transitions between such metastable configurations has been proposed [Colosqui \textit{et al., Phys. Rev. Lett.}, 2013, \textbf{111}, 028302] to predict both the relaxation rate and the crossover point to the slow logarithmic regime. However, the adsorption dynamics observed experimentally before the crossover point has remained unstudied. In this work, we propose a Langevin model that is able to describe the entire adsorption process of single colloidal particles by considering metastable states produced by surface defects and thermal motion of the particle and liquid interface. Invoking the fluctuation dissipation theorem, we introduce a drag term that considers significant dissipative forces induced by thermal fluctuations of the liquid interface. Langevin dynamics simulations based on the proposed adsorption model yield close agreement with experimental observations for different microparticles, capturing the crossover from (fast) capillary driven dynamics to (slow) thermally activated kinetics.

cond-mat.soft↗

arXiv2015

Imaging Multiple Colloidal Particles by Fitting Electromagnetic Scattering Solutions to Digital Holograms

Digital holographic microscopy is a fast three-dimensional (3D) imaging tool with many applications in soft matter physics. Recent studies have shown that electromagnetic scattering solutions can be fit to digital holograms to obtain the 3D positions of isolated colloidal spheres with nanometer precision and millisecond temporal resolution. Here we describe the results of new techniques that extend the range of systems that can be studied with fitting. We show that an exact multisphere superposition scattering solution can be used to fit holograms of colloidal clusters containing up to six spheres. We also introduce an approximate and computationally simpler solution, Mie superposition, that is valid for multiple spheres spaced several wavelengths or more from one another. We show that this method can be used to fit holograms of several spheres on an emulsion droplet, and we give a quantitative criterion for assessing its validity.

physics.optics↗

arXiv2015

Using the Discrete Dipole Approximation and Holographic Microscopy to Measure Rotational Dynamics of Non-spherical Colloidal Particles

We present a new, high-speed technique to track the three-dimensional translation and rotation of non-spherical colloidal particles. We capture digital holograms of micrometer-scale silica rods and sub-micrometer-scale Janus particles freely diffusing in water, and then fit numerical scattering models based on the discrete dipole approximation to the measured holograms. This inverse-scattering approach allows us to extract the the position and orientation of the particles as a function of time, along with static parameters including the size, shape, and refractive index. The best-fit sizes and refractive indices of both particles agree well with expected values. The technique is able to track the center of mass of the rod to a precision of 35 nm and its orientation to a precision of 1.5$^\circ$, comparable to or better than the precision of other 3D diffusion measurements on non-spherical particles. Furthermore, the measured translational and rotational diffusion coefficients for the silica rods agree with hydrodynamic predictions for a spherocylinder to within 0.3%. We also show that although the Janus particles have only weak optical asymmetry, the technique can track their 2D translation and azimuthal rotation over a depth of field of several micrometers, yielding independent measurements of the effective hydrodynamic radius that agree to within 0.2%. The internal and external consistency of these measurements validate the technique. Because the discrete dipole approximation can model scattering from arbitrarily shaped particles, our technique could be used in a range of applications, including particle tracking, microrheology, and fundamental studies of colloidal self-assembly or microbial motion.

physics.optics↗

arXiv2015

Fast, label-free tracking of single viruses and weakly scattering nanoparticles in a nano-fluidic optical fiber

High-speed tracking of single particles is a gateway to understanding physical, chemical, and biological processes at the nanoscale. It is also a major experimental challenge, particularly for small, nanometer-scale particles. Although methods such as confocal or fluorescence microscopy offer both high spatial resolution and high signal-to-background ratios, the fluorescence emission lifetime limits the measurement speed, while photobleaching and thermal diffusion limit the duration of measurements. Here we present a tracking method based on elastic light scattering that enables long-duration measurements of nanoparticle dynamics at rates of thousands of frames per second. We contain the particles within a single-mode silica fiber containing a sub-wavelength, nano-fluidic channel and illuminate them using the fiber's strongly confined optical mode. The diffusing particles in this cylinderical geometry are continuously illuminated inside the collection focal plane. We show that the method can track unlabeled dielectric particles as small as 20 nm as well as individual cowpea chlorotic mottle virus (CCMV) virions - 4.6 megadaltons in size - at rates of over 2 kHz for durations of tens of seconds. Our setup is easily incorporated into common optical microscopes and extends their detection range to nanometer-scale particles and macromolecules. The ease-of-use and performance of this technique support its potential for widespread applications in medical diagnostics and micro total analysis systems.

physics.optics↗

arXiv2015

Two-Dimensional Clusters of Colloidal Spheres: Ground States, Excited States, and Structural Rearrangements

We study experimentally what is arguably the simplest yet non-trivial colloidal system: two-dimensional clusters of 6 spherical particles bound by depletion interactions. These clusters have multiple, degenerate ground states whose equilibrium distribution is determined by entropic factors, principally the symmetry. We observe the equilibrium rearrangements between ground states as well as all of the low-lying excited states. In contrast to the ground states, the excited states have soft modes and low symmetry, and their occupation probabilities depend on the size of the configuration space reached through internal degrees of freedom, as well as a single "sticky parameter" encapsulating the depth and curvature of the potential. Using a geometrical model that accounts for the entropy of the soft modes and the diffusion rates along them, we accurately reproduce the measured rearrangement rates. The success of this model, which requires no fitting parameters or measurements of the potential, shows that the free-energy landscape of colloidal systems and the dynamics it governs can be understood geometrically.

cond-mat.soft↗

arXiv2014

Absence of Red Structural Color in Photonic Glasses, Bird Feathers and Certain Beetles

Colloidal glasses, bird feathers, and beetle scales can all show structural colors arising from short-ranged spatial correlations between scattering centers. Unlike the structural colors arising from Bragg diffraction in ordered materials like opals, the colors of these photonic glasses are independent of orientation, owing to their disordered, isotropic microstructures. However, there are few examples of photonic glasses with angle-independent red colors in nature, and colloidal glasses with particle sizes chosen to yield structural colors in the red show weak color saturation. Using scattering theory, we show that the absence of angle-independent red color can be explained by the tendency of individual particles to backscatter light more strongly in the blue. We discuss how the backscattering resonances of individual particles arise from cavity-like modes, and how they interact with the structural resonances to prevent red. Finally, we use the model to develop design rules for colloidal glasses with red, angle-independent structural colors.

cond-mat.soft↗

arXiv2013

Holographic Measurements of Anisotropic Three-Dimensional Diffusion of Colloidal Clusters

We measure all nonzero elements of the three-dimensional (3D) diffusion tensor D for clusters of colloidal spheres to a precision of 1% or better using digital holographic microscopy. We study both dimers and triangular trimers of spheres, for which no analytical calculations of the diffusion tensor exist. We observe anisotropic rotational and translational diffusion arising from the asymmetries of the clusters. In the case of the three-particle triangular cluster, we also detect a small but statistically significant difference in the rotational diffusion about the two in-plane axes. We attribute this difference to weak breaking of threefold rotational symmetry due to a small amount of particle polydispersity. Our experimental measurements agree well with numerical calculations and show how diffusion constants can be measured under conditions relevant to colloidal self-assembly, where theoretical and even numerical prediction is difficult.

cond-mat.soft↗

arXiv2012

Tetrahedral colloidal clusters from random parking of bidisperse spheres

Using experiments and simulations, we investigate the clusters that form when colloidal spheres stick irreversibly to -- or "park" on -- smaller spheres. We use either oppositely charged particles or particles labeled with complementary DNA sequences, and we vary the ratio $α$ of large to small sphere radii. Once bound, the large spheres cannot rearrange, and thus the clusters do not form dense or symmetric packings. Nevertheless, this stochastic aggregation process yields a remarkably narrow distribution of clusters with nearly 90% tetrahedra at $α=2.45$. The high yield of tetrahedra, which reaches 100% in simulations at $α=2.41$, arises not simply because of packing constraints, but also because of the existence of a long-time lower bound that we call the "minimum parking" number. We derive this lower bound from solutions to the classic mathematical problem of spherical covering, and we show that there is a critical size ratio $α_c=(1+\sqrt{2})\approx 2.41$, close to the observed point of maximum yield, where the lower bound equals the upper bound set by packing constraints. The emergence of a critical value in a random aggregation process offers a robust method to assemble uniform clusters for a variety of applications, including metamaterials.

cond-mat.soft↗

arXiv2011

Deriving Finite Sphere Packings

Sphere packing problems have a rich history in both mathematics and physics; yet, relatively few analytical analyses of sphere packings exist, and answers to seemingly simple questions are unknown. Here, we present an analytical method for deriving all packings of n spheres in R^3 satisfying minimal rigidity constraints (>= 3 contacts per sphere and >= 3n-6 total contacts). We derive such packings for n <= 10, and provide a preliminary set of maximal contact packings for 10 < n <= 20. The resultant set of packings has some striking features, among them: (i) all minimally rigid packings for n <= 9 have 3n-6 contacts, (ii) non-rigid packings satisfying minimal rigidity constraints arise for n >= 9, (iii) the number of ground states (i.e. packings with the maximal number of contacts) oscillates with respect to n, (iv) for 10 <= n <= 20 there are only a small number of packings with the maximal number of contacts, and for 10 <= n < 13 these are all commensurate with the HCP lattice. The general method presented here may have applications to other related problems in mathematics, such as the Erdos repeated distance problem and Euclidean distance matrix completion problems.

cond-mat.soft↗