arXiv subjects

David G. Grier

Publications and source records attributed to David G. Grier.

At least 19 recordsLinked to original sources

arXiv2025

Nonreciprocal wave-mediated interactions power a classical time crystal

An acoustic standing wave acts as a lattice of evenly spaced potential energy wells for sub-wavelength-scale objects. Trapped particles interact with each other by exchanging waves that they scatter from the standing wave. Unless the particles have identical scattering properties, their wave-mediated interactions are nonreciprocal. Pairs of particles can use this nonreciprocity to harvest energy from the wave to sustain steady-state oscillations despite viscous drag and the absence of periodic driving. We show in theory and experiment that a minimal system composed of two acoustically levitated particles can access four distinct dynamical states, two of which are emergently active steady states. Under some circumstances, these emergently active steady states break spatiotemporal symmetry and therefore constitute a classical time crystal.

cond-mat.soft↗

arXiv2025

A Quantitative Holographic Agglutination Assay for Immunoglobulin A

This study introduces a Holographic Agglutination Assay for quantifying levels of the immunoglobulin protein IgA in biological samples. This is the first example of a label-free and bead-free assay that quantifies protein agglutinates by direct detection using Total Holographic Characterization. A proof-of-concept assay for human serum immunoglobulins is demonstrated using Jacalin, the galactose-specific plant lectin, to induce selective agglutination. By analyzing the size, refractive index, and number of particles in an assay sample, we obtain a reproducible and quantitative measurement of galactosylated immunoglobulins in a given sample. The assay is calibrated for a physiologically relevant reference interval of IgA concentrations in a 10x diluted emulated biological sample from low (80 mg/dL, 5 μM) to high (320 mg/dL, 20 μM) levels. The assay clearly distinguishes samples containing IgA from samples containing IgG. More broadly, this study introduces a platform for creating lectin-mediated Holographic Agglutination Assays to monitor levels of immunoglobulins in biological samples. The ability to quantify immunoglobulin levels efficiently in clinical samples is likely to be valuable for diagnostics and will provide a basis for assaying other proteins that can be induced to agglutinate.

physics.optics↗

arXiv2025

Multiplexed holographic molecular binding assays with internal calibration standards

Holographic molecular binding assays detect macromolecules binding to colloidal probe beads by monitoring nanometer-scale changes in the beads' diameters with holographic microscopy. Measured changes are interpreted with Maxwell Garnett effective-medium theory to infer the surface coverage of analyte molecules and therefore to measure the analyte concentration in solution. The precision and accuracy of those measurements can be degraded by run-to-run instrumental variations, which introduce systematic errors in the holographic characterization measurements. We detect and mitigate these errors by introducing a class of inert reference beads whose polymer brush coating resists macromolecular binding. The holographically measured diameter and refractive index of those beads serve as internal standards for THC measurements. To characterize the reference beads, we introduce a general all-optical method to measure the grafting density of the polymer brush that combines holographic characterization of the bead diameter with a refractometry measurement of the polymer's specific volume. The latter technique shows the specific volume of poly(ethylene oxide) to be 1.308(4) cubic nanometers per kilodalton. We use this suite of techniques to demonstrate a multiplexed immunoassay for immunoglobulin G (IgG) whose success validates the effective-medium analysis of holographic characterization measurements. Internal negative controls provided by the reference beads are validated by negative control measurements on alcohol dehydrogenase (ADH), which has a similar molecular weight to IgG but does not bind to the probe beads' binding sites.

cond-mat.soft↗

arXiv2025

Worm-like emulsion droplets

Forming an interface between immiscible fluids incurs a free-energy cost that usually favors minimizing the interfacial area. An emulsion droplet of fixed volume therefore tends to form a sphere, and pairs of droplets tend to coalesce. Surfactant molecules adsorbed to the droplets' surfaces stabilize emulsions by providing a kinetic barrier to coalescence. Here, we show that the bound surfactants' osmotic pressure also competes with the droplet's intrinsic surface tension and can reverse the sign of the overall surface free energy. The onset of negative surface tension favors maximizing surface area and therefore favors elongation into a worm-like morphology. Analyzing this system in the Gibbs grand canonical ensemble reveals a phase transition between spherical and worm-like emulsions that is governed by the chemical potential of surfactant molecules in solution. Predictions based on this model agree with the observed behavior of an experimental model system composed of lipid-stabilized silicone oil droplets in an aqueous surfactant solution.

cond-mat.soft↗

arXiv2024

Scattered waves fuel emergent activity

Active matter taps into external energy sources to power its own processes. Systems of passive particles ordinarily lack this capacity, but can become active if the constituent particles interact with each other nonreciprocally. By reformulating the theory of classical wave-matter interactions, we demonstrate that interactions mediated by scattered waves generally are not constrained by Newton's third law. The resulting center-of-mass forces propel clusters of scatterers, enabling them to extract energy from the wave and rendering them active. This form of activity is an emergent property of the scatterers' state of organization and can arise in any system where mobile objects scatter waves. Emergent activity flips the script on conventional active matter whose nonreciprocity emerges from its activity, and not the other way around. We combine theory, experiment and simulation to illustrate how emergent activity arises in wave-matter composite systems and to explore the phenomenology of emergent activity in experimentally accessible models. These preliminary studies suggest that heterogeneity is a singular perturbation to the dynamics of wave-matter composite systems, and induces emergent activity under all but the most limited circumstances.

cond-mat.soft↗

arXiv2024

Complex Dynamics of an Acoustically Levitated Fluid Droplet Captured by a Low-Order Immersed Boundary Method

We present a novel immersed boundary method that implements acoustic perturbation theory to model an acoustically levitated droplet. Instead of resolving sound waves numerically, our hybrid method solves acoustic scattering semi-analytically and models the corresponding time-averaged acoustic forces on the droplet. This framework allows the droplet to be simulated on inertial timescales of interest, and thereby admit a much larger time resolution than traditional compressible flow solvers. To benchmark this technique and demonstrate its utility, we implement the hybrid IBM for a single droplet in a standing wave. Simulated droplet shape deformations and streaming profile agree with theoretical predictions. Our simulations also yield new insights on the streaming profiles for elliptical droplets, for which a comprehensive analytic solution does not exist.

cond-mat.soft↗

arXiv2024

Measuring Colloidomer Hydrodynamics with Holographic Video Microscopy

In-line holographic video microscopy records a wealth of information about the microscopic structure and dynamics of colloidal materials. Powerful analytical techniques are available to retrieve that information when the colloidal particles are well-separated. Large assemblies of close-packed particles create holograms that are substantially more challenging to interpret. We demonstrate that Rayleigh-Sommerfeld back-propagation is useful for analyzing holograms of colloidomer chains, close-packed linear assemblies of micrometer-scale emulsion droplets. Colloidomers are fully flexible chains and undergo three-dimensional configurational changes under the combined influence of random thermal forces and hydrodynamic forces. We demonstrate the ability of holographic reconstruction to track these changes as colloidomers sediment through water in a horizontal slit pore. Comparing holographically measured configurational trajectories with predictions of hydrodynamic models both validates the analytical technique for this valuable class of self-organizing materials and also provides insights into the influence of geometric confinement on colloidomer hydrodynamics.

cond-mat.soft↗

arXiv2023

Spectral holographic trapping: Creating dynamic force landscapes with polyphonic waves

Acoustic trapping uses forces exerted by sound waves to transport small objects along specified trajectories in three dimensions. The structure of the acoustic force landscape is governed by the amplitude and phase profiles of the sound's pressure wave. These profiles can be controlled through deliberate spatial modulation of monochromatic waves, by analogy to holographic optical trapping. Alternatively, spatial and temporal control can be achieved by interfering a small number of sound waves at multiple frequencies to create acoustic holograms based on spectral content. We demonstrate spectral holographic trapping by projecting acoustic conveyor beams that move millimeter-scale objects along prescribed paths, and control the complexity of particle trajectories by tuning the strength of weak reflections. Illustrative spectral superpositions of static and dynamic force landscapes enable us to realize two variations on the theme of a wave-driven oscillator, a deceptively simple dynamical system with surprisingly complex phenomenology.

cond-mat.soft↗

arXiv2023

Acoustodynamic mass determination: Accounting for inertial effects in acoustic levitation of granular materials

Acoustic traps use forces exerted by sound waves to confine and transport small objects. The dynamics of an object moving in the force landscape of an acoustic trap can be significantly influenced by the inertia of the surrounding fluid medium. These inertial effects can be observed by setting a trapped object in oscillation and tracking it as it relaxes back to mechanical equilibrium in its trap. Large deviations from Stokesian dynamics during this process can be explained quantitatively by accounting for boundary-layer effects in the fluid. The measured oscillations of a perturbed particle then can be used not only to calibrate the trap but also to characterize the particle.

cond-mat.soft↗

arXiv2023

Anomalous tumbling of colloidal ellipsoids in Poiseuille flows

Shear flows cause aspherical colloidal particles to tumble so that their orientations trace out complex trajectories known as Jeffery orbits. The Jeffery orbit of a prolate ellipsoid is predicted to align the particle's principal axis preferentially in the plane transverse to the axis of shear. Holographic microscopy measurements reveal instead that colloidal ellipsoids' trajectories in Poiseuille flows strongly favor an orientation inclined by roughly $π/8$ relative to this plane. This anomalous observation is consistent with at least two previous reports of colloidal rods and dimers of colloidal spheres in Poiseuille flow and therefore appears to be a generic, yet unexplained feature of colloidal transport at low Reynolds numbers.

cond-mat.soft↗

arXiv2022

Multi-angle holographic characterization of individual fractal aggregates

Holographic particle characterization uses quantitative analysis of holographic microscopy data to precisely and rapidly measure the diameter and refractive index of individual colloidal spheres in their native media. When this technique is applied to inhomogeneous or aspherical particles, the measured diameter and refractive index represent properties of an effective sphere enclosing each particle. Effective-sphere analysis has been applied successfully to populations of fractal aggregates, yielding an overall fractal dimension for the population as a whole. Here, we demonstrate that holographic characterization also can measure the fractal dimensions of an individual fractal cluster by probing how its effective diameter and refractive index change as it undergoes rotational diffusion. This procedure probes the structure of a cluster from multiple angles and thus constitutes a form of tomography. Here we demonstrate and validate this effective-sphere interpretation of aspherical particles' holograms through experimental studies on aggregates of silica nanoparticles grown under a range of conditions.

cond-mat.soft↗

arXiv2022

Dexterous holographic trapping of dark-seeking particles with Zernike holograms

The intensity distribution of a holographically-projected optical trap can be tailored to the physical properties of the particles it is intended to trap. Dynamic optimization is especially desirable for manipulating dark-seeking particles that are repelled by conventional optical tweezers, and even more so when dark-seeking particles coexist in the same system as light-seeking particles. We address the need for dexterous manipulation of dark-seeking particles by introducing a class of "dark" traps created from the superposition of two out-of-phase Gaussian modes with different waist diameters. Interference in the difference-of-Gaussians (DoG) trap creates a dark central core that is completely surrounded by light and therefore can trap dark-seeking particles rigidly in three dimensions. DoG traps can be combined with conventional optical tweezers and other types of traps for use in heterogeneous samples. The ideal hologram for a DoG trap being purely real-valued, we introduce a general method based on the Zernike phase-contrast principle to project real-valued holograms with the phase-only diffractive optical elements used in standard holographic optical trapping systems. We demonstrate the capabilities of DoG traps (and Zernike holograms) through experimental studies on high-index, low-index and absorbing colloidal particles dispersed in fluid media.

physics.optics↗

arXiv2021

Ultrasonic chaining of emulsion droplets

Emulsion droplets trapped in an ultrasonic levitator behave in two ways that solid spheres do not: (1) Individual droplets spin rapidly about an axis parallel to the trapping plane, and (2) coaxially spinning droplets form long chains aligned with their common axis of rotation. Acoustically-organized chains interact hydrodynamically, either to merge into longer chains or to form three-dimensional bundles of chains. Solid spheres, by contrast, form close-packed planar crystals drawn together by the sound-mediated secondary Bjerknes interaction. We demonstrate the chain-to-crystal transition with a model system in which fluid emulsion droplets can be photopolymerized into solid spheres without significantly changing other material properties. The behavior of this experimental system is quantitatively consistent with an acoustohydrodynamic model for spinning spheres in an acoustic levitator. This study therefore introduces acoustically-driven spinning as a mechanism for guiding self-organization of acoustically levitated matter.

cond-mat.soft↗

arXiv2020

Holographic characterization and tracking of colloidal dimers in the effective-sphere approximation

An in-line hologram of a colloidal sphere can be analyzed with the Lorenz-Mie theory of light scattering to measure the sphere's three-dimensional position with nanometer-scale precision while also measuring its diameter and refractive index with part-per-thousand precision. Applying the same technique to aspherical or inhomogeneous particles yields the position, diameter and refractive index of an effective sphere that represents an average over the particle's geometry and composition. This effective-sphere interpretation has been applied successfully to porous, dimpled and coated spheres, as well as to fractal clusters of nanoparticles, all of whose inhomogeneities appear on length scales smaller than the wavelength of light. Here, we combine numerical and experimental studies to investigate effective-sphere characterization of symmetric dimers of micrometer-scale spheres, a class of aspherical objects that appear commonly in real-world dispersions. Our studies demonstrate that the effective-sphere interpretation usefully identifies dimers in holographic characterization studies of monodisperse colloidal spheres. The effective-sphere estimate for a dimer's axial position closely follows the ground truth for its center of mass. Trends in the effective-sphere diameter and refractive index, furthermore, can be used to measure a dimer's three-dimensional orientation. When applied to colloidal dimers transported in a Poiseuille flow, the estimated orientation distribution is consistent with expectations for Brownian particles undergoing Jeffery orbits.

cond-mat.soft↗

arXiv2020

Dynamics of an acoustically trapped sphere in beating sound waves

A focused acoustic standing wave creates a Hookean potential well for a small sphere and can levitate it stably against gravity. Exposing the trapped sphere to a second transverse traveling sound wave imposes an additional acoustical force that drives the sphere away from its mechanical equilibrium. The driving force is shaped by interference between the standing trapping wave and the traveling driving. If, furthermore, the traveling wave is detuned from the standing wave, the driving force oscillates at the difference frequency. Far from behaving like a textbook driven harmonic oscillator, however, the wave-driven harmonic oscillator instead exhibits a remarkably rich variety of dynamical behaviors arising from the spatial dependence of the driving force. These include oscillations at both harmonics and subharmonics of the driving frequency, period-doubling routes to chaos and Fibonacci cascades. This model system therefore illustrates opportunities for dynamic acoustical manipulation based on spectral control of the sound field, rather than spatial control.

cond-mat.soft↗

arXiv2020

Holographic immunoassays

The size of a probe bead reported by holographic particle characterization depends on the proportion of the surface area covered by bound target molecules and so can be used as an assay for molecular binding. We validate this technique by measuring the kinetics of irreversible binding for the antibodies immunoglobulin G (IgG) and immunoglobulin M (IgM) as they attach to micrometer-diameter colloidal beads coated with protein A. These measurements yield the antibodies' binding rates and can be inverted to obtain the concentration of antibodies in solution. Holographic molecular binding assays therefore can be used to perform fast quantitative immunoassays that are complementary to conventional serological tests.

cond-mat.soft↗

arXiv2020

Interpreting Holographic Molecular Binding Assays with Effective Medium Theory

Holographic molecular binding assays use holographic video microscopy to directly detect molecules binding to the surfaces of micrometer-scale colloidal beads by monitoring associated changes in the beads' light-scattering properties. Holograms of individual spheres are analyzed by fitting to a generative model based on the Lorenz-Mie theory of light scattering. Each fit yields an estimate of a probe bead's diameter and refractive index with sufficient precision to watch the beads grow as molecules bind. Rather than modeling the molecular-scale coating, however, these fits use effective medium theory, treating the coated sphere as if it were homogeneous. This effective-sphere analysis is rapid and numerically robust and so is useful for practical implementations of label-free immunoassays. Here, we assess how effective-sphere properties reflect the properties of molecular-scale coatings by modeling coated spheres with the discrete-dipole approximation and analyzing their holograms with the effective-sphere model.

cond-mat.soft↗

arXiv2020

Quantitative differentiation of protein aggregates from other subvisible particles in viscous mixtures through holographic characterization

We demonstrate the use of holographic video microscopy to detect individual subvisible particles dispersed in biopharmaceutical formulations and to differentiate them based on material characteristics measured from their holograms. The result of holographic analysis is a precise and accurate measurement of the concentrations and size distributions of multiple classes of subvisible contaminants dispersed in the same product simultaneously. We demonstrate this analytical technique through measurements on model systems consisting of human IgG aggregates in the presence of common contaminants such as silicone oil emulsion droplets and fatty acids. Holographic video microscopy also clearly identifies metal particles and air bubbles. Being able to differentiate and characterize the individual components of such heterogeneous dispersions provides a basis for tracking other factors that influence the stability of protein formulations including handling and degradation of surfactant and other excipients.

cond-mat.soft↗