Sujit S. Datta

Crystallographic Etching of Few-Layer Graphene

We demonstrate a method by which few-layer graphene samples can be etched along crystallographic axes by thermally activated metallic nanoparticles. The technique results in long (>1 microm) crystallographic edges etched through to the insulating substrate, making the process potentially useful for atomically precise graphene device fabrication. This advance could enable atomically precise construction of integrated circuits from single graphene sheets with a wide range of technological applications.

25th Anniversary Article: Double Emulsion Templated Solid Microcapsules: Mechanics And Controlled Release

How droplet microfluidics can be used to fabricate solid-shelled microcapsules having precisely controlled release behavior is described. Glass capillary devices enable the production of monodisperse double emulsion drops, which can then be used as templates for microcapsule formation. The exquisite control afforded by microfluidics can be used to tune the compositions and geometrical characteristics of the microcapsules with exceptional precision. The use of this approach to fabricate microcapsules that only release their contents when exposed to a specific stimulus--such as a change in temperature, exposure to light, a change in the chemical environment, or an external stress--only after a prescribed time delay, and at a prescribed rate is reviewed.

Delayed Buckling and Guided Folding of Inhomogeneous Capsules

Colloidal capsules can sustain an external osmotic pressure; however, for a sufficiently large pressure, they will ultimately buckle. This process can be strongly influenced by structural inhomogeneities in the capsule shells. We explore how the time delay before the onset of buckling decreases as the shells are made more inhomogeneous; this behavior can be quantitatively understood by coupling shell theory with Darcys law. In addition, we show that the shell inhomogeneity can dramatically change the folding pathway taken by a capsule after it buckles.

Ultrathin Shell Double Emulsion Templated Giant Unilamellar Lipid Vesicles with Controlled Microdomain Formation

A microfluidic approach is reported for the high-throughput, continuous production of giant unilamellar vesicles (GUVs) using water-in-oil-in-water double emulsion drops as templates. Importantly, these emulsion drops have ultrathin shells; this minimizes the amount of residual solvent that remains trapped within the GUV membrane, overcoming a major limitation of typical microfluidic approaches for GUV fabrication. This approach enables the formation of microdomains, characterized by different lipid compositions and structures within the GUV membranes. This work therefore demonstrates a straightforward and versatile approach to GUV fabrication with precise control over the GUV size, lipid composition and the formation of microdomains within the GUV membrane.

Controlled Buckling and Crumpling of Nanoparticle-Coated Droplets

We introduce a new experimental approach to study the structural transitions of large numbers of nanoparticle-coated droplets as their volume is reduced. We use an emulsion system where the dispersed phase is slightly soluble in the continuous phase. By adding a fixed amount of unsaturated continuous phase, the volume of the droplets can be controllably reduced, causing them to buckle or crumple, thereby becoming nonspherical. The resultant morphologies depend both on the extent of volume reduction and the average droplet size. The buckling and crumpling behavior implies that the droplet surfaces are solid.

Controlling release from pH-responsive microcapsules.

We report a microfluidic approach to produce monodisperse pH-responsive microcapsules with precisely controlled release behavior. The solid microcapsule shells are composed of a biocompatible pH-responsive polymer and robustly encapsulate an active material; however, when exposed to a trigger pH, the shells degrade and ultimately release the microcapsule contents. We control the trigger pH by using polymers that dissolve at different pH values. We independently control the time at which the microcapsule contents are released by carefully controlling the shell thickness. Moreover, we independently control the rate at which the encapsulated contents are released by making hybrid shells composed of a mixture of a pH-responsive polymer and varying proportions of another, solid, pH-unresponsive polymer. This enables us to achieve monodisperse microcapsules that robustly encapsulate an active material, only releasing it when exposed to a desired pH, after a prescribed time delay, and at a prescribed rate.

Spatial fluctuations of fluid velocities in flow through a three-dimensional porous medium.

We use confocal microscopy to directly visualize the spatial fluctuations in fluid flow through a three-dimensional porous medium. We find that the velocity magnitudes and the velocity components both along and transverse to the imposed flow direction are exponentially distributed, even with residual trapping of a second immiscible fluid. Moreover, we find pore-scale correlations in the flow that are determined by the geometry of the medium. Our results suggest that despite the considerable complexity of the pore space, fluid flow through it is not completely random.

Rheology of attractive emulsions.

We show how attractive interactions dramatically influence emulsion rheology. Unlike the repulsive case, attractive emulsions below random close packing, φ(RCP), can form soft gel-like elastic solids. However, above φ(RCP), attractive and repulsive emulsions have similar elasticities. Such compressed attractive emulsions undergo an additional shear-driven relaxation process during yielding. Our results suggest that attractive emulsions begin to yield at weak points through the breakage of bonds, and, above φ(RCP), also undergo droplet configurational rearrangements.

Mobilization of a trapped non-wetting fluid from a three-dimensional porous medium

We use confocal microscopy to directly visualize the formation and complex morphologies of trapped non-wetting fluid ganglia within a model 3D porous medium. The wetting fluid continues to flow around the ganglia after they form; this flow is characterized by a capillary number, Ca. We find that the ganglia configurations do not vary for small Ca; by contrast, as Ca is increased above a threshold value, the largest ganglia start to become mobilized and are ultimately removed from the medium. By combining our 3D visualization with measurements of the bulk transport, we show that this behavior can be quantitatively understood by balancing the viscous forces exerted on the ganglia with the pore-scale capillary forces that keep them trapped within the medium. Our work thus helps elucidate the fluid dynamics underlying the mobilization of a trapped non-wetting fluid from a 3D porous medium.

Fluid breakup during simultaneous two-phase flow through a three-dimensional porous medium

We use confocal microscopy to directly visualize the simultaneous flow of both a wetting and a non-wetting fluid through a model three-dimensional (3D) porous medium. We find that, for small flow rates, both fluids flow through unchanging, distinct, connected 3D pathways; in stark contrast, at sufficiently large flow rates, the non-wetting fluid is broken up into discrete ganglia. By performing experiments over a range of flow rates, using fluids of different viscosities, and with porous media having different geometries, we show that this transition can be characterized by a state diagram that depends on the capillary numbers of both fluids, suggesting that it is controlled by the competition between the viscous forces exerted on the flowing oil and the capillary forces at the pore scale. Our results thus help elucidate the diverse range of behaviors that arise in two-phase flow through a 3D porous medium.