Thomas Boatwright

Probing interfacial dynamics and mechanics using submerged particle microrheology. II. Experiment

A non-contact microrheological technique to probe the mechanics of the air/water interface is explored. Polystyrene spheres dissolved in water are trapped with an optical tweezer near the free surface of water, allowing the response functions of the particles to be measured as a function of the distance from the air/water interface. These measurements show that at the surface, the imaginary part of the response function increases by approximately 30% from the Stokes value measured in the bulk. As the particle is moved away from the surface via an optical trap, the response function returns to the bulk value. The method is tested by comparing the response function of particles near a rigid wall to the theory developed by Faxen. A newly developed hydrodynamic theory is used to explain the results at the free interface through a calculation of the linear response function as a function of depth. These results show a range of sensitivity that can be utilized to study the microrheology of a Langmuir monolayer without distorting its structure.

Investigating the effect of particle size on pulmonary surfactant phase behavior.

We study the impact of the addition of particles of a range of sizes on the phase transition behavior of lung surfactant under compression. Charged particles ranging from micro- to nanoscale are deposited on lung surfactant films in a Langmuir trough. Surface area versus surface pressure isotherms and fluorescent microscope observations are utilized to determine changes in the phase transition behavior. We find that the deposition of particles close to 20 nm in diameter significantly impacts the coexistence of the liquid-condensed phase and liquid-expanded phase. This includes morphological changes of the liquid-condensed domains and the elimination of the squeeze-out phase in isotherms. Finally, a drastic increase of the domain fraction of the liquid-condensed phase can be observed for the deposition of 20-nm particles. As the particle size is increased, we observe a return to normal phase behavior. The net result is the observation of a critical particle size that may impact the functionality of the lung surfactant during respiration.

Probing interfacial dynamics and mechanics using submerged particle microrheology. I. Theory

Microrheology relies on tracking the thermal or driven motion of microscopic particles in a soft material. It is well suited to the study of materials that have no three-dimensional realization, which makes them difficult to study using a macroscopic rheometer. For this reason, microrheology is becoming an important rheological probe of Langmuir monolayers and membranes. Interfacial microrheology, however, has been difficult to reconcile quantitatively with more traditional macroscopic approaches. We suggest that uncertainties in accounting for the mechanical coupling of the tracer particle to the interface or membrane are responsible for these discrepancies. To resolve them, we propose a new non-contact approach to interfacial microrheology that uses particles submerged in the subphase a known distance below the interface. In this first of two papers, we present calculations of the response function (and thus the equilibrium fluctuation spectrum) of a spherical particle submerged below a viscoelastic surface that has a finite surface tension and/or bending modulus. In the second paper, we compare these results to submerged particle microrheology in a few example systems, showing quantitative agreement.

Particle Size Effects on Collapse in Monolayers

We report on the impact of differently sized particles on the collapse of a Langmuir monolayer. We use an SDS-DODAB monolayer because it is known to collapse reversibly under compression and expansion cycles. Particles with diameters of 1 μm, 0.5 μm, 0.1 μm, and 20 nm are deposited on the SDS-DODAB monolayer. We find a critical particle size range of 0.1 to 0.5 μm that produces a transition from reversible to irreversible collapse. The nature of the collapse is determined through optical observations and surface pressure measurements. In addition, although 20 nm particles do not cause irreversible collapse in the monolayer, they significantly decrease the collapse pressure relative to the other systems. Therefore, we observe three distinct collapse behaviors-reversible, irreversible, and reversible at a reduced surface pressure.

Tracking giant folds in a monolayer.

The collapse dynamics of giant folds in a catanionic monolayer at the air-water interface are examined. A monolayer of dioctadecyldimethylammonium bromide (DODAB) and sodium dodecyl sulfate (SDS) in a 1:1 ratio is the system of study that previously was found to fold upon compression in a Langmuir trough. Carboxylate-coated polystyrene beads (1 microm diameter) are deposited and bound to the monolayer. Displacement of the beads is measured with epifluorescence microscopy and particle image velocimetry, yielding a measurement of the velocity of the monolayer around the fold. Reversibility is confirmed by measuring the amount of monolayer material entering and leaving the fold. Material near folds are found to have a maximum relative velocity on the order of 0.1 mm/s, and fold depths are found to be on the order of 1 mm. The folds exhibit regular unfolding behavior, which can be explained qualitatively by a simple mechanical model.

Mechanical reorganization of cross-linked F-actin networks at the air-buffer interface

The response of an F-actin network at the air-buffer interface to nonlinear compression is studied. We observe two distinct classes of behavior: a mechanically induced structural reorganization of the monolayer and a subsequent reversible, nonlinear mechanical response. Measurements of pressure area isotherms, bulk modulus, and the epifluorescence microscopy of tracer beads provide evidence that an initial structural reorganization occurs that corresponds to the mechanically induced formation of bundles of actin. Once a steady state structure is formed, subsequent compressions exhibit four distinct regimes as a function of decreasing total area: a low density fragile network, a relatively uniform film of cross-linked bundles, a region characterized by a buckling instability, and finally, a close packed region. Evidence for the distinct regions comes from the epifluorescence microscopy of tracer beads and measurements of the bulk modulus. Key features of the dynamics include domain rearrangements in the fragile network and an irregular, jerk-like motion during the buckling transition.