Non-Classical Euler Buckling and Brazier Instability in Cylindrical Liquid Droplets.

Crystalline monolayers prevalent in nature and technology possess elusive elastic properties with important implications in fundamental physics, biology, and nanotechnology. Leveraging the recently discovered shape transitions of oil-in-water emulsion droplets, upon which these droplets adopt cylindrical shapes and elongate, we investigate the elastic characteristics of the crystalline monolayers covering their interfaces. To unravel the conditions governing Euler buckling and Brazier kink formation in these cylindrical tubular interfacial crystals, we strain the elongating cylindrical droplets within confining microfluidic wells.

"Magic Numbers" in Self-Faceting of Alcohol-Doped Emulsion Droplets.

Oil-in-water emulsion droplets spontaneously adopt, below some temperature T , counterintuitive faceted and complex non-spherical shapes while remaining liquid. This transition is driven by a crystalline monolayer formed at the droplets' surface. Here, we show that ppm-level doping of the droplet's bulk by long-chain alcohols allows tuning T by >50 °C, implying formation of drastically different interfacial structures.

Counterions under a Surface-Adsorbed Cationic Surfactant Monolayer: Structure and Thermodynamics.

The surface adsorption of ionic surfactants is fundamental for many widespread phenomena in life sciences and for a wide range of technological applications. However, direct atomic-resolution structural experimental studies of noncrystalline surface-adsorbed films are scarce. Thus, even the most central physical aspects of these films, such as their charge density, remain uncertain.

Salt-induced stability and modified interfacial energetics in self-faceting emulsion droplets.

Hypothesis: The counterintuitive temperature-controlled self-faceting of water-suspended, surfactant-stabilized, liquid oil droplets provides new opportunities in engineering of smart liquids, the properties of which are controllable by external stimuli. However, many emulsions exhibiting self-faceting phenomena have limited stability due to surfactant precipitation. The emulsions' stability may be enhanced, and their inter-droplet electrostatic repulsion tuned, through controlled charge screening driven by varying-concentration added salts.

Anomalous Temperature-Controlled Concave-Convex Switching of Curved Oil-Water Menisci.

While the curvature of the classical liquid surfaces exhibits only a weak temperature dependence, we demonstrate here a reversible temperature-tunable concave-convex shape switching in capillary-contained, surfactant-decorated, oil-water interfaces. The observed switching gives rise to a concave-convex shape transition, which takes place as a function of the width of the containing capillary. This apparent violation of Young's equation results from a hitherto-unreported sharp reversible hydrophobic-hydrophilic transition of the glass capillary walls.

Faceting and Flattening of Emulsion Droplets: A Mechanical Model.

When cooled down, emulsion droplets stabilized by a frozen interface of alkane molecules and surfactants have been observed to undergo a spectacular sequence of morphological transformations: from spheres to faceted liquid icosahedra, down to flattened liquid platelets. While generally ascribed to the interplay between the elasticity of the frozen interface and surface tension, the physical mechanisms underpinning these transitions have remained elusive, despite different theoretical pictures having been proposed in recent years. In this Letter, we introduce a comprehensive mechanical model of morphing emulsion droplets, which quantitatively accounts for various experimental observations, including the size scaling behavior of the faceting transition.

Polyhedral Water Droplets: Shape Transitions and Mechanism.

While classical liquid droplets are rounded, transitions have recently been discovered which render polyhedral water-suspended droplets of several oils. Yet, the mechanism of these transitions and the role of the droplets' interfacial curvature in inducing these transitions remain controversial. In particular, one of the two mechanisms suggested mandates a convex interface, in a view from the oil side.

Precise Self-Positioning of Colloidal Particles on Liquid Emulsion Droplets.

Decorating emulsion droplets by particles stabilizes foodstuff and pharmaceuticals. Interfacial particles also influence aerosol formation, thus impacting atmospheric CO exchange. While studies of particles at disordered droplet interfaces abound in the literature, such studies for ubiquitous ordered interfaces are not available.

Periodic buckling and grain boundary slips in a colloidal model of solid friction.

The intermittent 'stick-slip' dynamics in frictional sliding of solid bodies is common in everyday life and technology. This dynamics has been widely studied on a macroscopic scale, where the thermal motion can usually be neglected. However, the microscopic mechanisms behind the periodic stick-slip events are yet unclear.

Nanostructures, Faceting, and Splitting in Nanoliter to Yoctoliter Liquid Droplets.

Contrary to everyday experience, where all liquid droplets assume rounded, near-spherical shapes, the temperature-tuning of liquid droplets to faceted polyhedral shapes and to spontaneous splitting has been recently demonstrated in oil-in-water emulsions. However, the elucidation of the mechanism driving these surprising effects, as well as their many potential applications, ranging from faceted nanoparticle synthesis through new industrial emulsification routes to controlled-release drug delivery within the human body, have been severely hampered by the micron-scale resolution of the light microscopy employed to date in all in situ studies. Thus, the thickness of the interfacially frozen crystalline monolayer, suggested to drive these effects, could not be directly measured, and the low limit on the droplet size still showing these effects remained unknown.

Imaging of nanoparticle dynamics in live and apoptotic cells using temporally-modulated polarization.

Gold nanoparticles are widely exploited in phototherapy. Owing to their biocompatibility and their strong visible-light surface plasmonic resonance, these particles also serve as contrast agents for cell image enhancement and super-resolved imaging. Yet, their optical signal is still insufficiently strong for many important real-life applications.

Self-faceting of emulsion droplets as a route to solid icosahedra and other polyhedra.

Hypothesis: Temperature-controlled self-faceting of liquid droplets has been recently discovered in surfactant-stabilized alkane-in-water emulsions. We hypothesize that similar self-faceting may occur in emulsion droplets of UV-polymerizable linear hydrocarbons. We further hypothesize that the faceted droplet shapes can be fixed by UV-initiated polymerization, thus providing a new route towards the production of solid polyhedra.

Axial Confocal Tomography of Capillary-Contained Colloidal Structures.

Confocal microscopy is widely used for three-dimensional (3D) sample reconstructions. Arguably, the most significant challenge in such reconstructions is posed by the resolution along the optical axis being significantly lower than in the lateral directions. In addition, the imaging rate is lower along the optical axis in most confocal architectures, prohibiting reliable 3D reconstruction of dynamic samples.

Temperature-Tuned Faceting and Shape Changes in Liquid Alkane Droplets.

Recent extensive studies reveal that surfactant-stabilized spherical alkane emulsion droplets spontaneously adopt polyhedral shapes upon cooling below a temperature T while remaining liquid. Further cooling induces the growth of tails and spontaneous droplet splitting. Two mechanisms were offered to account for these intriguing effects.

Photo-Crosslinkable Colloids: From Fluid Structure and Dynamics of Spheres to Suspensions of Ellipsoids.

Recently-developed photo-crosslinkable PMMA (polymethylmethacrylate) colloidal spheres are a highly promising system for fundamental studies in colloidal physics and may have a wide range of future technological applications. We synthesize these colloids and characterize their size distribution. Their swelling in a density- and index- matching organic solvent system is demonstrated and we employ dynamic light scattering (DLS), as also the recently-developed confocal differential dynamic microscopy (ConDDM), to characterize the structure and the dynamics of a fluid bulk suspension of such colloids at different particle densities, detecting significant particle charging effects.

Dipolar colloids in apolar media: direct microscopy of two-dimensional suspensions.

Spherical colloids, in an absence of external fields, are commonly assumed to interact solely through rotationally-invariant potentials, u(r). While the presence of permanent dipoles in aqueous suspensions has been previously suggested by some experiments, the rotational degrees of freedom of spherical colloids are typically neglected. We prove, by direct experiments, the presence of permanent dipoles in commonly used spherical poly(methyl methacrylate) (PMMA) colloids, suspended in an apolar organic medium.

Optical-tweezing-based linear-optics nanoscopy.

Previous works reported that linear optics could be used to observe sub-wavelength features with a conventional optical microscope. Yet, the ability to reach a sub-200 nm resolution with a visible light remains limited. We present a novel widely-applicable method, where particle trapping is employed to overcome this limit.

How faceted liquid droplets grow tails.

Liquid droplets, widely encountered in everyday life, have no flat facets. Here we show that water-dispersed oil droplets can be reversibly temperature-tuned to icosahedral and other faceted shapes, hitherto unreported for liquid droplets. These shape changes are shown to originate in the interplay between interfacial tension and the elasticity of the droplet's 2-nm-thick interfacial monolayer, which crystallizes at some T = Ts above the oil's melting point, with the droplet's bulk remaining liquid.

Crystallization and reentrant melting of charged colloids in nonpolar solvents.

We explore the crystallization of charged colloidal particles in a nonpolar solvent mixture. We simultaneously charge the particles and add counterions to the solution with aerosol-OT (AOT) reverse micelles. At low AOT concentrations, the charged particles crystallize into body-centered-cubic (bcc) or face-centered-cubic (fcc) Wigner crystals; at high AOT concentrations, the increased screening drives a thus far unobserved reentrant melting transition.

Surfactant-induced phases in water-supported alkane monolayers: II. Structure.

The structure of the Langmuir-Gibbs films of normal alkanes C(n) of length n = 12-21 formed at the surface of aqueous solutions of C(m)TAB surfactants, m = 14, 16, and 18, was studied by surface-specific synchrotron X-ray methods. At high temperatures, a laterally disordered monolayer of mixed alkane molecules and surface-adsorbed surfactant tails is found, having thicknesses well below those of the alkanes' and surfactant tails' extended length. The mixed monolayer undergoes a freezing transition at a temperature T(s)(n,m), which forms, for n ≤ m + 1, a crystalline monolayer of mixed alkane molecules and surfactant tails.

Surfactant-induced phases in water-supported alkane monolayers: I. Thermodynamics.

Alkanes longer than n = 6 carbons do not spread on the water surface, but condense in a macroscopic lens. However, adding trimethylammonium-based surfactants, C(m)TAB, in submillimolar concentrations causes the alkanes to spread and form a single Langmuir-Gibbs (LG) monolayer of mixed alkanes and surfactant tails, which coexists with the alkane lenses. Upon cooling, this LG film surface-freezes at a temperature T(s) above the bulk freezing temperature T(b).

Denser fluids of charge-stabilized colloids form denser sediments.

Granular matter, where solid-like elasticity emerges in the absence of crystalline order, has been actively studied over the last few decades, targeting fundamental physical understanding of granular packings and glasses, abundant in everyday life and technology. We employ charge-stabilized sub-micron particles in a solvent, known as colloids, to form granular packings through a well-controlled process, where initially homogeneous and thermodynamically equilibrated colloidal fluids form solid sediments, when subjected to an effective gravity in a centrifuge. We demonstrate that particles' volume fraction φj in these sediments increases linearly with that in the initial fluid φ0, setting an upper limit φRCP≈ 0.

Locating particles accurately in microscope images requires image-processing kernels to be rotationally symmetric.

Computerized image-analysis routines deployed widely to locate and track the positions of particles in microscope images include several steps where images are convolved with kernels to remove noise. In many common implementations, some kernels are rotationally asymmetric. Here we show that the use of these asymmetric kernels creates significant artifacts, distorting apparent particle positions in a way that gives the artificial appearance of orientational crystalline order, even in such fully-disordered isotropic systems as simple fluids of hard-sphere-like colloids.

Dense colloidal fluids form denser amorphous sediments.

We relate, by simple analytical centrifugation experiments, the density of colloidal fluids with the nature of their randomly packed solid sediments. We demonstrate that the most dilute fluids of colloidal hard spheres form loosely packed sediments, where the volume fraction of the particles approaches in frictional systems the random loose packing limit, ϕRLP = 0.55.