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Anand Yethiraj

Publications and source records attributed to Anand Yethiraj.

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Insights into the electrorheological and electrohydrodynamic regimes in electrically driven emulsion

Recently, we reported the electrorheoimaging (ERI) technique (Bahraminasr et al, 2026), and found that frequency-dependent electric field of an oil-in-oil emulsion yields two distinct regimes: a high-frequency dipolar, electrorheological (ER) regime and a low-frequency electrohydrodynamic (EHD) regime. In this work, we identify a phenomenological model to fit the results in the ER regime to a classic yield-stress fluid, and find collapse onto a master curve upon rescaling, consistent with a yield stress that grows approximately as $E^2$. Macroscopic small-amplitude oscillatory shear (SAOS) rheology is compared with passive microrheology employing differential dynamic microscopy (DDM), with the close agreement implying scale independence of the ER behaviour, and indicating that, unlike steady shear, SAOS measurements do not restructure these samples and probe underlying material properties. Finally, under the presence of both steady shear and electric fields in the EHD regime, the emulsion forms banded structures composed of alternating droplet-rich and droplet-depleted regions. We explore recurrence and divergence in the location of these bands: they emerge within seconds of field application and decay rapidly after the field is switched off. Using the Jensen--Shannon divergence between radial intensity profiles, we show that the driven structure loses memory on timescales of order $1~s$ commensurate with the timescale of the EHD convection roll. For much longer field-off intervals successive banding events become statistically independent.

cond-mat.soft

Tunable turbulence in driven microscale emulsions

We present a tunable, non-equilibrium oil-in-oil emulsion that serves as a model system for investigating the transition from controlled droplet deformation to multiscale flows reminiscent of turbulence. By utilizing a miscible mixture of silicone and motor oils as the continuous phase and the immiscible castor oil as the droplet phase, we isolate electrical conductivity as a single experimental control parameter, varying it by over two orders of magnitude while keeping viscosity and permittivity nearly constant. This high degree of control allows us to systematically traverse the electrohydrodynamic (EHD) phase diagram with dielectric constant and conductivity as control parameters. We validate small-deformation theory at low fields before driving the system into a regime of multiscale, unsteady flows at high fields. We employ three complementary approaches on the same system (particle image velocimetry (PIV), used to map velocity fields, and rheometry and differential dynamic microscopy (DDM), two techniques used to probe viscosity and diffusion) to quantify the emergence of scale invariance in the energy spectra with increasing field strength. Above a threshold field, we find that the spatio-temporal energy spectra obtained by PIV analysis of droplet dynamics display power-law scaling, $E(k) \sim k^{-α_k}$, where $α_k$ approaches the inertial turbulence exponent of $5/3$ at high fields. Energy spectra from rheometry also yield a power law, $S(ν) \sim ν^{-α_ν}$, with $α_ν= 5/3$ at high fields. Mean square displacement (MSD) analyses on the same datasets reveal super-diffusive behavior, $\mathrm{MSD} \sim t^γ$, with $γ= 3/2$. These observations provide strong evidence of a conductivity-tunable transition to EHD-driven turbulence in a microscale emulsion.

cond-mat.soft

Physical Properties of Dextran Solutions as Model Crowding Media

The role of macromolecular crowding in living systems is widely appreciated, but artificial crowders used to model these effects in vitro are often inadequately characterized. In this work, we examine density, viscosity, polymer self-diffusion and water diffusion in crowded dextran systems. Dextran viscosity and self-diffusion follow size-dependent trends, collectively described by universal functions of the overlap concentration corresponding to a Flory exponent of 0.44, characteristic of branched polymers. Viscosity increases with concentration as a power law, with a crossover from dilute to semi-dilute behaviors. Dextran self-diffusion decays exponentially: this can be interpreted in light of Rosenfeld's excess entropy scaling hypothesis. Water self-diffusivity and specific volume decrease with concentration, but show no dependence on polymer size. We show how these results can be used to construct the true volume fraction of crowders, which takes into account bound water. Overall, our findings showcase the power of polymer physics concepts in macromolecular crowding studies in vitro.

cond-mat.soft

Concentration Dependence of Elastic and Viscoelastic Properties of Aqueous Solutions of Ficoll and Bovine Serum Albumin by Brillouin Light Scattering Spectroscopy

The cellular environment is crowded with macromolecules of different shapes and sizes. The effect of this macromolecular crowding has been studied in a variety of synthetic crowding environments: two popular examples are the compact colloid-like Ficoll macromolecule, and the globular protein bovine serum albumin (BSA). Recent studies have indicated a significant component of bound or surface-associated water in these crowders reduces the available free volume. In this work, Brillouin light scattering experiments were performed on aqueous solutions of Ficoll 70 and Ficoll 400 with concentrations ranging from 1 wt% to 35 wt% and BSA with concentrations of 1 wt% to 27 wt%. From the dependence of spectral peak parameters on polymer concentration, we determined fundamental solution properties: hypersound velocity, adiabatic bulk modulus and compressibility, apparent viscosity, and hypersound attenuation. Existing theory that ignores intermolecular interactions can only capture the observed linear trends in the frequency shift up to a threshold concentration, beyond which a quadratic term accounting for intermolecular interactions is necessary. This likely indicates a transition from the dilute to semi-dilute regime. In the Ficoll solutions (but not BSA) we see evidence for a central mode, with a characteristic relaxation time of 20 ps, that we attribute to exchange of the bound water.

cond-mat.soft

Anomalous dynamics in tracer-particle motions in an electrohydrodynamically driven oil-in-oil system

We characterize the super-diffusive dynamics of tracer particles in an electrohydrodynamically driven emulsion of oil droplets in an immiscible oil medium, where the amplitude and frequency of an external electric field are the control parameters. In the weakly-driven electrohydrodynamic regime, the droplets are trapped dielectrophoretically on a patterned electrode, and the driving is therefore spatially varying. We find excellent agreement with a $\langle x^2 \rangle \sim t^{1.5}$ power law, and find that this superdiffusive dynamics arises from an underlying displacement distribution that is distinctly non-Gaussian, and exponential for small displacements and short times. While these results are comparable with a random-velocity field model, the tracer particle speeds are in fact spatially varying in 2 dimensions, arising from a spatially varying electrohydrodynamic driving force. This suggests that the important ingredient for the super-diffusive $t^{1.5}$ behaviour observed is a velocity field that is isotropic in the plane and spatially correlated. Finally, we can extract, from the superdiffusive dynamics, a experimental lengthscale that corresponds to the lateral range of the hydrodynamic flows. This experimental length scale is only non-zero above a threshold ion mobility length.

physics.app-ph

Dynamics and complex formation in charged and uncharged Ficoll70 solutions

We apply pulsed-field-gradient NMR (PFG NMR) technique to measure the translational diffusion for both uncharged and charged polysaccharide (Ficoll70) in water. Analysis of the data indicate that NMR signal attenuation above a certain packing fraction can be adequately fitted with a bi-exponential function. The self-diffusion measurements show also that the Ficoll70, an often-used compact, spherical polysucrose molecule, is itself non-ideal, exhibiting signs of both softness and attractive interactions in the form of a stable suspension consisting of monomers and clusters. Further, we can quantify the fraction of monomer and cluster. This work strengthens the picture of the existence of a bound water layer within and around a porous Ficoll70 particle.

cond-mat.soft

Contrasting the dynamics of elastic and non-elastic deformations across an experimental colloidal Martensitic transition

We present a framework to segregate the roles of elastic and non-elastic deformations in the examination of real-space experiments of solid-solid Martensitic transitions. The Martensitic transformation of a body-centred-tetragonal(BCT) to a body-centred-orthorhombic(BCO) crystal structure has been studied in a model system of micron-scale ionic microgel colloids. Non-affine fluctuations, i.e., displacement fluctuations that do not arise from purely elastic(affine) deformations, are detected in particle configurations acquired from the experiment. Tracking these fluctuations serves as a highly sensitive tool in signaling the onset of the Martensitic transition and precisely locating particle rearrangements occurring at length scales of a few particle diameters. Particle rearrangements associated with non-affine displacement modes become increasingly favorable during the transformation process. The nature of the displacement fluctuation modes that govern the transformation are shown to be different from those predominant in an equilibrium crystal. We show that BCO crystallites formed through shear may, remarkably, co-exist with those resulting from local rearrangements within the same sample.

cond-mat.soft

Clusters in sedimentation equilibrium for an experimental hard-sphere-plus-dipolar Brownian colloidal system

In this work, we use structure and dynamics in sedimentation equilibrium, in the presence of gravity, to examine, $via$ confocal microscopy, a Brownian colloidal system in the presence of an external electric field. The zero field equation of state (EOS) is hard sphere without any re-scaling of particle size, and the hydrodynamic corrections to the long-time self-diffusion coefficient are quantitatively consistent with the expected value for hard spheres. Care is taken to ensure that both the dimensionless gravitational energy, which is equivalent to a Peclet number $Pe_g$, and dipolar strength $Λ$ are of order unity. In the presence of an external electric field, anisotropic chain-chain clusters form; this cluster formation manifests itself with the appearance of a plateau in the diffusion coefficient when the dimensionless dipolar strength $Λ\sim 1$. The structure and dynamics of this chain-chain cluster state is examined for a monodisperse system for two particle sizes.

cond-mat.soft

Electric-field-induced turbulent energy cascade in an oil-in-oil emulsion

We observe electro-hydrodynamically driven turbulent flows at low Reynolds numbers in a two-fluid emulsion consisting of micron-scale droplets. In the presence of electric fields, the droplets produce interacting hydrodynamic flows which result in a dynamical organization at a spatial scale much larger than the size of the individual droplets. We characterize the dynamics associated with these structures by both video imaging and a simultaneous, in situ, measurement of the time variation of the bulk Reynolds stress with a rheometer. The results display scale invariance in the energy spectra in both space and time.

cond-mat.soft

Diffusion NMR study of complex formation in membrane-associated peptides

Pulsed-field-gradient nuclear magnetic resonance (PFG-NMR) is used to obtain the true hydrodynamic size of complexes of peptides with sodium dodecyl sulfate SDS micelles. The peptide used in this study is a 19-residue antimicrobial peptide, GAD-2. Two smaller dipeptides, alanine-glycine (Ala-Gly) and tyrosine-leucine (Tyr-Leu), are used for comparison. We use PFG-NMR to simultaneously measure diffusion coefficients of both peptide and surfactant. These two inputs, as a function of SDS concentration, are then fit to a simple two species model that neglects hydrodynamic interactions between complexes. From this we obtain the fraction of free SDS, and the hydrodynamic size of complexes in a GAD-2--SDS system as a function of SDS concentration. These results are compared to those for smaller dipeptides and for peptide-free solutions. At low SDS concentrations ([SDS] $\leq$ 25 mM), the results self-consistently point to a GAD-2--SDS complex of fixed hydrodynamic size R =(5.5 $\pm$ 0.3) nm. At intermediate SDS concentrations (25 mM $<$ [SDS] $<$ 60 mM), the apparent size of a GAD-2--SDS complex shows almost a factor of two increase without a significant change in surfactant-to-peptide ratio within a complex, most likely implying an increase in the number of peptides in a complex. For peptide-free solutions, the self-diffusion coefficients of SDS with and without buffer are significantly different at low SDS concentrations but merge above [SDS]=60 mM. We find that in order to obtain unambiguous information about the hydrodynamic size of a peptide-surfactant complex from diffusion measurements, experiments must be carried out at or below [SDS] = 25 mM.

cond-mat.soft

Dynamics, crystallization and structures in colloid spin coating

Spin coating is an out-of-equilibrium technique for producing polymer films and colloidal crystals quickly and reproducibly. In this review, we present an overview of theoretical and experimental studies of the spin coating of colloidal suspensions. The dynamics of the spin coating process is discussed first, and we present insights from both theory and experiment. A key difference between spin coating with polymer solutions and with monodisperse colloidal suspensions is the emergence of long range (centimeter scale) orientational correlations in the latter. We discuss experiments in different physical regimes that shed light on the many unusual partially-ordered structures that have long-range orientational order, but no long-range translational order. The nature of these structures can be tailored by adding electric or magnetic fields during the spin coating procedure. These partially-ordered structures can be considered as model systems for studying the fundamentals of poorly crystalline and defect-rich solids, and they can also serve as templates for patterned and/or porous optical and magnetic materials.

cond-mat.soft

Effect of order-parameter fluctuations on the Halperin-Lubensky-Ma first-order transition in superconductors and liquid crystals

We show that order-parameter fluctuations in a good type-I superconductor or a liquid crystal always increase the size of the first-order transition. This behavior is eventually changed when the system crosses over to inverted-XY critical behavior, with the size of the first-order transition vanishing as a power law with a crossover exponent. We find a good agreement between our theory and a recent experiment on the nematic-smectic-A first-order transition in 8CB-10CB mixtures of liquid crystals.

cond-mat.soft

Two Experimental Tests of the Halperin-Lubensky-Ma Effect at the Nematic-Smectic-A Phase Transition

We have conducted two quantitative tests of predictions based on the Halperin-Lubensky-Ma (HLM) theory of fluctuation-induced first-order phase transitions. First, we explore the effect of an external magnetic field on the nematic-smectic-A (NA) transition in a liquid crystal. Second, we examine the dependence of the first-order discontinuity as a function of mixture concentration in pure 8CB and three 8CB-10CB mixtures. We find the first quantitative evidence for deviations from the HLM theory.

cond-mat.soft

External-field-induced tricritical point in a fluctuation-driven nematic-smectic-A transition

We study theoretically the effect of an external field on the nematic-smectic-A (NA) transition close to the tricritical point, where fluctuation effects govern the qualitative behavior of the transition. An external field suppresses nematic director fluctuations, by making them massive. For a fluctuation-driven first-order transition, we show that an external field can drive the transition second-order. In an appropriate liquid crystal system, we predict the required magnetic field to be of order 10 T. The equivalent electric field is of order $1 V/μm$.

cond-mat.soft