This paper reports measurements of particle-wall and particle-particle interactions in levitated colloidal ensembles using integrated total internal reflection microscopy (TIRM) and video microscopy (VM) techniques. In levitated colloidal ensembles with area fractions of phiA = 0.03-0.25, ensemble TIRM measured height distribution functions are used to interpret particle-wall interactions, and VM measured pair distribution functions are used to interpret particle-particle interactions using inverse Ornstein-Zernike (OZ) and three-dimensional inverse Monte Carlo (MC) analyses. An inconsistent finding is the observation of an anomalous long-range particle-particle attraction and recovery of the expected Derjaguin-Landau-Verwey-Overbeek (DLVO) particle-wall interactions for all concentrations examined. Because particle-wall and particle-particle potentials are expected to be consistent in several respects, the analytical and experimental methods employed in this investigation are examined for possible sources of error. Comparison of inverse OZ and three-dimensional inverse MC analyses are used to address uncertainties related to dimensionality, effects of particle concentration, and assumptions of the OZ theory and closure relations. The possible influence of charge heterogeneity and particle size polydispersity on measured distribution functions is discussed with regard to inconsistent particle-wall and particle-particle potentials. Ultimately, achieving a consistent understanding of particle-wall and particle-particle interactions in interfacial and confined colloidal systems is essential to numerous complex fluid and advanced material technologies.
We present a refractometric sensor based on quantum dot-embedded polystyrene microspheres. Optical resonances within a microsphere, known as whispering-gallery modes ͑WGMs͒, produce narrow spectral peaks. For sensing applications, spectral shifts of these peaks are sensitive to changes in the local refractive index. In this work, two-photon excited luminescence from the quantum dots couples into several WGMs within the microresonator. By optimizing the detection area, the spectral visibility of the WGMs is improved. The spectral shifts are measured as the surrounding index of the refraction changes. The experimental sensitivity is about five times greater than that predicted by the Mie theory.
This paper reports confocal microscopy measurements of inhomogeneous colloidal sedimentation equilibrium profiles near planar wall surfaces for conditions when colloid dimensions are comparable to the characteristic gravitational length scale. The intensity based confocal method developed in this work enables real-space measurements of one-dimensional density profiles of Brownian colloids without identifying many single colloid centers in large imaging volumes. Measured sedimentation equilibrium profiles for single-phase interfacial fluids and for coexisting inhomogeneous fluid and solid phases are in agreement with a perturbation theory and Monte Carlo simulations within the local density approximation. Monte Carlo simulated colloid scale density profiles display some minor differences with confocal images in terms of microstructural transitions involving the onset of interfacial crystallization and the precise elevation of the fluid-solid interface. These discrepancies are attributed to polydispersity unaccounted for in the analyses, sensitivity of the perturbation theory to the effective hard sphere size, and the influence of ensemble, system size, and box shape in Monte Carlo simulations involving anisotropic/inhomogeneous solids. Successful demonstration of intensity based confocal microscopy provides a basis for future measurements of three-dimensional colloidal interactions, dynamics, and structure near surfaces.
Evanescent wave excited luminescence of quantum dot modified polystyrene (QDPS) colloids is investigated to measure potential energy profiles of QDPS colloids electrostatically levitated above a planar glass surface. Luminescence is characterized for three different-sized PS colloids modified with three different-sized QDs using confocal microscopy, emission spectra, flow cytometry, and temporal measurements of levitated and deposited colloids. Colloid-surface potential energy profiles constructed from scattering and luminescence intensity data display excellent agreement with each other, theoretical predictions, and independently measured parameters. QDPS luminescence intensity is indirectly confirmed to have an exponential dependence on height similar to conventional colloidal evanescent wave scattering. Our findings indicate that evanescent wave excited QDPS luminescence could enable total internal reflection microscopy measurements of index-matched hard spheres, multiple specific biomolecular interactions via spectral multiplexing, enhanced morphology-dependent resonance modes, and integrated evanescent wave-video-confocal microscopy experiments not possible with scattering.
Naturally occurring seismic events and artificially generated low-frequency (1 to 500 Hz) elastic waves have been observed to alter the production rates of oil and water wells, sometimes increasing and sometimes decreasing production, and to influence the turbidity of surface and well water. The decreases in production are of particular concern, especially when artificially generated elastic waves are applied as a method for enhanced oil recovery. The exact conditions that result in a decrease in production remain unknown. Although the underlying environment is certainly complex, the observed increase in water well turbidity after natural seismic events suggests the existence of a mechanism that can affect both the subsurface flow paths and the mobilization of in situ colloidal particles. This article explores the macroscopic and microscopic effects of low-frequency dynamic stress stimulations on the release of colloidal particles from an analog core representing an infinitesimal section along the propagation paths of an elastic wave. Experiments on a column packed with 1 mm borosilicate beads and loaded with polystyrene microparticles demonstrate that axial mechanical stress oscillations enhance the mobilization of captured microparticles. Increasing the amplitude of the oscillations increases the number of microparticles released and can also result in cyclical spikes in effluent microparticle concentration during stimulation. Under a prolonged period of stimulation, the cyclical effluent spikes coincided with fluctuations in the column pressure data and continued at a diminished level after stimulation. This behavior can be attributed to rearrangements of the beads in the column, resulting in possible changes in the void space and/or tortuosity of the packing. Optical microscopy observations of the beads during low-frequency oscillations reveal that individual beads rotate, thereby rubbing against each other and scraping away portions of the adsorbed microparticles. These results support the theory that mechanical interactions between porous matrix grains are important mechanisms in flow path alteration and the mobilization of naturally occurring colloidal particles during elastic wave stimulation. These results also point to both continuous and discrete en masse releases of colloidal particles, perhaps because of circulation cells within the packing material.
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