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Research Nuggets

Research

IRG I

IRG 1. Fluid Flows- Singularities and Microscales

Faculty (* = coordinators): I. Gruzberg, R. Ismagilov, H. Jaeger, L. Kadanoff*, W. Kang, K.Y.C. Lee*, S. Nagel, P. Wiegmann, T. Witten, W. Zhang
Affiliates: T. Dupont, M. Silber

IRG1 is the direct descendant of the program that first introduced fluid flow and its accompanying singularities as topics for investigation in a materials laboratory. It is also among the first to bring out the connections between fluid and particulate flows (granular fluids). Our results have proven the aptness and importance of these investigations for the materials science community. The study of singularities provides an appropriate paradigm not only because they are mathematically deep and physically robust, but more especially because they offer a method of understanding and controlling small-scale flows which prove to be practically important. Many of the technologically interesting flow effects are also the most intellectually challenging. Our reported and proposed work is directed at the robust effects of singularities, aimed at studying the effects of microscales upon flows and of flows upon microscale phenomena.


Thin Necks, Slender Bridges, Close Approaches: Zhang, Nagel and Kadanoff are investigat-ing topological changes in fluids related to small structures produced when two different masses of fluids are pulled apart or pushed together. These small-scale structures are likely to have technological implications. One outgrowth of this project points to the kinds of successes we are aiming at. Nagel, Mrksich (IRG4), and M. Garfinkel, M.D. in surgery at U of C, are using the very thin spouts formed by ‘selective withdrawal’ to ‘shrink-wrap’ irregularly shaped cells with a uniform coating. This coating keeps pig pancreatic cells within a human body but separated from human immunological response. This approach seems to be promising for the treatment of type I diabetes. The collaboration has demonstrated that the encapsulated coat is indeed permeable to glucose and insulin but impermeable to larger molecules responsible for immune reactions.


The basic research underpinning this kind of work is being continued as well. The Zhang & Nagel groups have made fundamental advances in understanding the flow-driven topological transition that underlies the formation of the thin liquid spout. A simplified numerical model capturing the key ingredients in the selective withdrawal processes identified the transition as a discontinuous saddle-node bifurcation. In particular, the original interpretation of an approach towards a singular shape is shown to result from an unusual, approximately logarithmic coupling between the smallest and the largest lengthscales that persist until transition. Viscous entrainment experiments have identified multiple distinctive spout states. Simulation and theoretical analysis to characterize the dynamics of these spout states are underway.


Bouncing Droplets
: Blanchette and Bigioni, two postdocs in the Zhang & Jaeger groups, collaborated to uncover the mechanism for the unusual cascade of coalescences observed when a liquid drop impacts a deep layer of the same liquid at very small speeds. Using simulation and experiment, they showed that coalescence initiates capillary waves that propagate along the interface and collapse at the top of the liquid drop. This wave pulls the drop away from the interface so violently that the drop pinches into two pieces instead of coalescing in one step. [Nature Physics, 2, 254-257, (2006)]


Two-Dimensional Flow and Growth: Gruzberg, Wiegmann, and Kadanoff have been co-mentoring a group including a postdoc and five graduate students who are using a new approach to explore singular growth and flow processes in 2D. The physical processes under study include the spread of an almost inviscid fluid in a viscous fluid (Hele-Shaw flow), diffusion-limited aggregation (DLA), dielectric breakdown, electrodeposition, mineral dendrites, and droplets of electronic fluid in the quantum Hall effect (QHE). The new theoretical approach is based on Laplacian Growth, SLE (Schramm-Loewner evolution), and a special case of Schwarz-Christoffel (SC) transformations. In the Laplacian growth part, an essential role is played by the integrable structure of the growth. It was shown that singularities of the growth are related to the genus of transitions associated with the Whitham universal hierarchy. This connection allowed us to classify singularities and analyze singularities occurring at droplet break-up, during the creation of new droplets, and shock-wave-type singularities. A variant of SLE where the driving function is a combination of a continuous Brownian motion and stochastic process with jumps has been considered, and this work involves the formation of line defects in 2D materials. Kadanoff and Gruzberg are working on the mathematical theory of such line defects using "Toeplitz matrices” and have developed a new application to the 2D Ising model and discovered new information about the eigenvalues of these matrices. The SC transformation has been applied to describe lattice DLA using polygons diffusing on a lattice. The elementary polygons assemble into more complicated ones, but at any stage of the aggregation one can use SC conformal mapping to describe the growing cluster. The parameters of this mapping evolve during growth and also influence it. This stochastic motion of the parameters has been described analytically and also simulated numerically using SC-tools set of routines designed for MatLab. Connections of these findings are now being made with QHE experiments by Kang and granular flow experiments by Nagel and Jaeger.


Feasibility for kilometer-scale liquid films in spac
e. The Witten group showed that appropriate fluid design can surmount most of the obstacles to achieving a fluid film of kilometer diameter outside Earth's atmosphere and gravity [PRE 74, 051602 (2006)]. They identified the chief impediment to creating such a film as puncture by micrometeoroids, and suggested a way of curing this impediment via physico-chemical means. If puncture damage can be prevented, Reynolds numbers of the order of 107 appear feasible. Witten, Jaeger and Lee will identify a suitable surfactant system to test the stability under vacuum at small scale.


Chiral sedimentation. A principal means of characterizing chiral molecules is optical rotatory dispersion. The rotatory power of a molecule is a known spatial moment of its polarizability tensor. Chiral sedimentation is an analogous property of a chiral object: the object rotates as it sinks, at a rate characteristic of its chirality.The Witten group has shown that objects consisting of as few as three Stokeslet drag centers can show chiral sedimentation and that the chiral effect requires hydrodynamic interaction among the Stokeslets. They are developing a formalism and numerical procedure for predicting the chiral sedimentation of arbitrary configurations of Stokeslets. The Witten, Cluzel and Scherer groups will explore the feasibility of measuring chiral sedimentation for self-complexed RNA in solution.


Flow in Microfluidic Channels: Using multiphase flows within microfluidic channels, Ismagilov has shown that nanoliter-sized droplets (plugs) of aqueous reagents can be formed within flows of immiscible oil. Together with Witten, Nagel, Zhang, and Kadanoff, the group has developed a better understanding of mixing by chaotic advection in fluid plugs traveling through winding channels. As slow chaotic mixing is most efficient at inducing nucleation due to the long lifetime of interfaces generated, they have applied this technique to investigate the effect of mixing on nucleation of protein crystals. This system was first extended to three-phase liquid-liquid-gas flow, and stable regimes of flow were identified and shown to correlate with the capillary number. Most recently, this system has been extended to three-phase liquid-liquid-liquid flow and criteria for identifying immiscible liquids for use as effective spacers to prevent droplet coalescence were identified. This system eliminates the undesirable drop merger effect as it does not suffer from the problem of gas bubble compressibility. Theory describing the flow of such fluids and stability criteria was initially derived by an exchange student from Chile under the joint mentorship of Ismagilov and Witten. Furthermore, this three-phase liquid-liquid-liquid flow system was shown to be compatible with protein crystallization in plugs. This work has enabled the development of cartridge-based screening tools for protein crystallization and enzymatic assays in IRG4. Future work will involve the continued development of experimental systems for protein crystallization based on these systems and testing and refining these theories with support from Kadanoff, Silber, Witten and Zhang.


Lipid Membranes. The collaboration between the Lee, Nagel and Witten groups has made further progress in understanding the structure of lipid mono- and multilayers. Extending earlier work on monolayer collapse, the Lee group has shown that fluid monolayers undergo collapse at lower pressures, and give rise to a variety of 3D collapse structures that are distinct from the folds observed in solid-like monolayers (IRG3). The spontaneous curvature of lipid molecules and their dipole density are found to dictate the final collapse structure, and theoretical understanding of this structural formation is provided by the Witten group. While membrane fluidity can be systematically tuned by adding a varied amount of a secondary lipid to the primary one, the Lee group has recently discovered that ganglioside GM1, a glycosphingolipid containing sialic acid, can be both a rigidifier and a fluidizer for the same lipid system. At low concentrations, GM1 has a condensing effect while at higher concentrations, it acts to fluidize, with a switch-over point between the two given by a stoichiometric ratio. To pinpoint the structural aspect of GM1 that gives rise to the observed effect, experiments with other gangiosides, ceramides, and PEGylated lipids are underway.


The Nagel and Witten groups made further progress in exploring the multilamellar surfactant cylinders known as myelins [PRL 96, 138301 (2006); Eur. Phys. J. E 18, 279 (2005)]. L. N. Zou in the Nagel group demonstrated an indentation-triggered mechanism for creating single myelins with unprecedented control. J. R. Huang in the Witten group [Eur. Phys. J. E 19, 399 (2006)] extended his theory of myelin formation to explain the twisted structure often observed in myelins. Future work will test the predicted scaling of minimal myelin diameter with degree of dehydration of the parent smectic phase.


Splashes in Fluids and Granular Matter. Nagel and Zhang have been collaborating on studying the dynamics of splashing. Their dramatic discovery [PRL 94, 184505 (2005)] that the presence of surrounding air was important in creating the splash has led to a number of different projects. The experimental data support a model by Zhang in which compressible effects in the gas are responsible for splashing in liquid/solid impacts. Thus they found that for a smooth substrate splashing can be completely suppressed by decreasing the pressure of the surrounding gas. They have now also found that a drop can produce a “prompt” splash even in the absence of air if the substrate is sufficiently rough. Simulations by Zhang’s group including the effect of air are being compared with experiments in Nagel’s lab. Experiments show that there are several different regimes for splashing. Zhang’s and Nagel’s groups are jointly attempting to establish the causes for the different regimes. Their collaborative work is shedding light on the mechanisms for how the energy, originally distributed uniformly as kinetic energy throughout the drop, becomes partitioned into small regions as the liquid disintegrates into thousands of disconnected pieces.


In a complementary system, Jaeger has been investigating the disintegration of a granular “liquid”. A liquid-like granular jet was formed by the impact of a solid body onto a volume of fine granular matter. In fluids, impact-induced jets are held together by surface tension. The granular jet exists in the absence of both surface tension and cohesion. Using high-speed x-ray radiography at Argonne and digital video, jet formation both inside and above the bed was tracked [Nature Physics 1, 164 (2005)]. Intriguingly, the jet breaks up into smaller “droplets” similar to what would be expected from a slender column of ordinary liquid (Rayleigh-Plateau instability). This breaking-up for fine-grained powders also occurs in a different experimental geometry: gravity-driven flow out of a vertical funnel [PRE 74, 051304, (2006)]. As in the liquid case, the gas appears to play a significant role in determining the evolution of the droplets.

From annual report to the NSF, March 2007