Theory for solvent, momentum, and energy transfer between a surfactant solution and a vapor atmosphere

We develop a complete set of equations governing the evolution of a sharp interface separating a volatile-solvent/nonvolatile-surfactant solution from a vapor atmosphere. In addition to a sorption isotherm equation and the conventional balances for mass, linear momentum, and energy, these equations include a counterpart of the Hertz???Knudsen???Langmuir equation familiar from conventional theories of evaporation-condensation. This additional equation arises from a consideration of configurational forces within a thermodynamical framework. While the notion of configurational forces is well-developed and understood for the description of materials, like crystalline solids, that possess natural reference configurations, very little has been done regarding their role in materials, such as viscous fluids, that do not possess preferred reference states. We therefore provide a comprehensive discussion of configurational forces, the balance of configurational momentum, and configurational thermodynamics that does not require a choice of reference configuration. The general evolution equations arising from our theory account for the thermodynamic structure of the solution and the interface and for sources of dissipation related to the transport of surfactant, momentum, and heat in the solution, the transport of surfactant and momentum within the interface, and the transport of solute, momentum, kinetic energy, and heat across the interface. Due to the complexity of these equations, we provide approximate equations which we compare to relations that appear in the literature.published or submitted for publicationis peer reviewe

Microscopic Investigation of Vortex Breakdown in a Dividing T-Junction Flow

3D-printed microfluidic devices offer new ways to study fluid dynamics. We present the first clear visualization of vortex breakdown in a dividing T-junction flow. By individual control of the inflow and two outflows, we decouple the effects of swirl and rate of vorticity decay. We show that even slight outflow imbalances can greatly alter the structure of vortex breakdown, by creating a net pressure difference across the junction. Our results are summarized in a dimensionless phase diagram, which will guide the use of vortex breakdown in T-junctions to achieve specific flow manipulation.Comment: 5 pages, 5 figure

Optimized Immobilization of Biomolecules on Nonspherical Gold Nanostructures for Efficient Localized Surface Plasmon Resonance Biosensing

Plasmonic biosensing techniques employ metal nanostructures, commonly gold (Au), often with biomolecules attached to their surfaces either directly or via other linkers. Various surface chemistry methods based on dispersion and covalent interactions are used to attach biomolecules to Au. As a result, when immobilizing a molecule on a metal surface, quantitative estimates of binding efficiency and stability of these surface chemistry methods are needed. Most prior work to compare such methods deals with bulk/thin film configurations or spherical nanoparticles, and very little is known about immobilization of biomolecules on plasmonic nanostructures of different shapes. Besides, due to rapid advancement of modern nanofabrication techniques, there is a growing need to determine an efficient surface chemistry method for immobilization of biomolecules on nonspherical plasmonic nanostructures. Previous comparison of immobilization methods on spherical Au nanoparticles has shown that physical adsorption resulted in the highest concentration of immobilized antibodies. In our work, we conducted a similar study and compared four representative Au surface functionalization methods as well as estimated how efficient these methods are at attaching biomolecules to nonspherical plasmonic Au nanostructures. We estimated the concentration of immobilized antibody that is specific to human C-reactive protein (anti-hCRP) by measuring the localized surface plasmon resonance (LSPR) shifts after exposing the surface of Au nanostructures to the antibody. Our results differ from the previously reported ones since the highest concentration of anti-hCRP was immobilized using 11-mercaptoundecanoic acid (MUA) chemistry. We demonstrated that immobilized antibodies retained their stability and specificity toward hCRP throughout the immunoassay when diluted hCRP or hCRP-spiked human serum samples were used. These findings have important implications for the fields of biosensing and diagnostics that employ nonspherical plasmonic nanostructures since an overall performance of these devices depends on efficient biomolecule immobilization

Detecting Escherichia coli Biofilm Development Stages on Gold and Titanium by Quartz Crystal Microbalance

Bacterial biofilms are responsible for persistent infections and biofouling, raising serious concerns in both medical and industrial processes. These motivations underpin the need to develop methodologies to study the complex biological structures of biofilms and prevent their formation on medical implants, tools, and industrial apparatuses. Here, we report the detailed comparison of Escherichia coli biofilm development stages (adhesion, maturation, and dispersion) on gold and titanium surfaces by monitoring the changes in both frequency and dissipation of a quartz crystal microbalance (QCM) device, a cheap and reliable microgravimetric sensor which allows the real-time and label-free characterization of various stages of biofilm development. Although gold is the most common electrode material used for QCM sensors, the titanium electrode is also readily available for QCM sensors; thus, QCM sensors with different metal electrodes serve as a simple platform to probe how pathogens interact with different metal substrates. The QCM outcomes are further confirmed by atomic force microscopy and crystal violet staining, thus validating the effectiveness of this surface sensitive sensor for microbial biofilm research. Moreover, because QCM technology can easily modify the substrate types and coatings, QCM sensors also provide well-controlled experimental conditions to study antimicrobial surface treatments and eradication procedures, even on mature biofilms

Air Plasma-Enhanced Covalent Functionalization of Poly(methyl methacrylate): High-Throughput Protein Immobilization for Miniaturized Bioassays

Miniaturized systems, such as integrated microarray and microfluidic devices, are constantly being developed to satisfy the growing demand for sensitive and high-throughput biochemical screening platforms. Owing to its recyclability, and robust mechanical and optical properties, poly(methyl methacrylate) (PMMA) has become the most sought after material for the large-scale fabrication of these platforms. However, the chemical inertness of PMMA entails the use of complex chemical surface treatments for covalent immobilization of proteins. In addition to being hazardous and incompatible for large-scale operations, conventional biofunctionalization strategies pose high risks of compromising the biomolecular conformations, as well as the stability of PMMA. By exploiting radio frequency (RF) air plasma and standard 1-ethyl-3-(3-(dimethylamino)propyl) carbodiimide (EDC) and N-hydroxysuccinimide (NHS) chemistry in tandem, we demonstrate a simple yet scalable PMMA functionalization strategy for covalent immobilization (chemisorption) of proteins, such as green fluorescent protein (GFP), while preserving the structural integrities of the proteins and PMMA. The surface density of chemisorbed GFP is shown to be highly dependent on the air plasma energy, initial GFP concentration, and buffer pH, where a maximum GFP surface density of 4 × 10–7 mol/m2 is obtained, when chemisorbed on EDC–NHS-activated PMMA exposed to 27 kJ of air plasma, at pH 7.4. Furthermore, antibody-binding studies validate the preserved biofunctionality of the chemisorbed GFP molecules. Finally, the coupled air plasma and EDC–NHS PMMA biofunctionalization strategy is used to fabricate microfluidic antibody assay devices to detect clinically significant concentrations of Chlamydia trachomatis specific antibodies. By coupling our scalable and tailored air plasma-enhanced PMMA biofunctionalization strategy with microfluidics, we elucidate the potential of fabricating sensitive, reproducible, and sustainable high-throughput protein screening systems, without the need for harsh chemicals and complex instrumentation

Proof‐of‐concept modular fluid handling prototype integrated with microfluidic biochemical assay modules for point‐of‐care testing

Large populations around the world suffer from numerous but treatable health issues, caused by either lifestyle choices or environmental factors. Over the past decades, point-of-care testing kits have been developed to circumvent the reliance on laboratories, by allowing users to perform preliminary health or environmental testing from the privacy of their homes. However, these kits heavily rely on the precision of the user to perform the procedures, leading to increased variability in final assessments. To eliminate user-induced errors, we present an integrated, completely sealed, and disposable point-of-care testing prototype that exploits the benefits of microfluidics and 3D-printing fabrication techniques. The palm-sized modular prototype consists of a manually operated fluid handling device that allows precise mixing, filtration, and delivery of fluids to an on-board microfluidic assay unit for subsequent detection of specific biochemical analytes, with a minimized risk of contamination

Elastic instabilities in planar elongational flow of monodisperse polymer solutions

We investigate purely elastic flow instabilities in the almost ideal planar stagnation point elongational flow field generated by a microfluidic optimized-shape cross-slot extensional rheometer (OSCER). We use time-resolved flow velocimetry and full-field birefringence microscopy to study the behavior of a series of well-characterized viscoelastic polymer solutions under conditions of low fluid inertia and over a wide range of imposed deformation rates. At low deformation rates the flow is steady and symmetric and appears Newtonian-like, while at high deformation rates we observe the onset of a flow asymmetry resembling the purely elastic instabilities reported in standard-shaped cross-slot devices. However, for intermediate rates, we observe a new type of elastic instability characterized by a lateral displacement and time-dependent motion of the stagnation point. At the onset of this new instability, we evaluate a well-known dimensionless criterion M that predicts the onset of elastic instabilities based on geometric and rheological scaling parameters. The criterion yields maximum values of M which compare well with critical values of M for the onset of elastic instabilities in viscometric torsional flows. We conclude that the same mechanism of tension acting along curved streamlines governs the onset of elastic instabilities in both extensional (irrotational) and torsional (rotational) viscoelastic flows

Steady viscoelastic flow around high-aspect-ratio, low-blockage-ratio microfluidic cylinders

We employ a state-of-the-art microfabrication technique (selective laser-induced etching, SLE) to produce microfluidic cylinder geometries that explore new geometrical regimes. Using SLE, two microchannels are fabricated in monolithic fused silica substrate with height H = 2 mm and width W = 0.4 mm (aspect ratio α = H/W = 5) containing cylinders of radius r = 0.02 mm (blockage ratio β = 2r/W = 0.1), centered at the channel mid-width, W/2. An ‘sc’ channel contains a single cylinder, while a ‘dc’ channel contains two axiallyaligned cylinders separated by a distance L = 1 mm (L = 50r). Compared with cylinder geometries fabricated by soft lithography (which typically have α ≪ 1 and β ≳ 0.5), these rigid glass devices provide a quasi-two-dimensional flow along the direction of the cylinder axis and also more clearly reveal the effects of the strong extensional wake regions located at the leading and trailing stagnation points. Using flow velocimetry and quantitative birefringence measurement techniques, we study the behaviour of a well-characterized viscoelastic polymer solution in flow around the cylinders. The small cylinder radii result in low inertia and very high elasticity numbers El ≈ 2400. For the sc device, we report strong flow modification effects around the cylinder as the flow rate is incremented. This is associated with the deformation of polymer molecules primarily in the upstream wake region, leading to the onset of a purely elastic flow asymmetry upstream of the cylinder. Stretched polymer molecules are advected around the cylinder and relax downstream of the cylinder, resulting in an extremely long elastic wake extending for > 300r downstream. In the dc channel, at lower flow rates, similar flow modification effects are observed to develop around, and downstream of, both cylinders. However, at higher flow rates the wake of the first cylinder extends > 50r downstream, and begins to interact with the second cylinder. The second cylinder becomes encapsulated by the wake of the first and is effectively obviated from the flow field. The results will be of relevance to understanding practical applications of viscoelastic fluids, for example in particle suspension and porous media flows, and also for benchmarking against numerical simulations using viscoelastic constitutive models

Tristability in viscoelastic flow past side-by-side microcylinders

Viscoelastic flows through microscale porous arrays exhibit complex path-selection and switching phenomena. However, understanding this process is limited by a lack of studies linking between a single object and large arrays. Here, we report experiments on viscoelastic flow past side-by-side microcylinders with variable intercylinder gap. With increasing flow rate, a sequence of two imperfect symmetry-breaking bifurcations forces selection of either one or two of the three possible flow paths around the cylinders. Tuning the gap length through the value where the first bifurcation becomes perfect reveals regions of bi and tristability in a dimensionless flow rate-gap length `phase' diagram.Comment: 5 pages, 4 figure

Asymmetric flow of polymer solutions around microfluidic cylinders: Interaction between shear-thinning and viscoelasticity

Viscoelastic flow around a cylinder is a model problem representing a wide range of relevant industrial processing and biological applications. Reducing the cylinder to microscopic dimensions conveniently enables the problem to be examined in the absence of inertia. Recently, we have developed glass microfluidic geometries containing long and slender, yet rigidly fixed, microfluidic cylinders, which present a low blockage ratio β=2r/W=0.1, where r=20μm is the cylinder radius and W=400μm is the channel width. Using a shear-banding viscoelastic wormlike micellar (WLM) solution, we showed how the flow around such a cylinder could destabilize beyond a critical Weissenberg number (Wi=λU/r, where λ is a characteristic time of the fluid and U is the average flow velocity), resulting in the asymmetric division of the fluid around either side of the cylinder [Haward et al, Soft Matter 15:1927]. In the present work we investigate this flow instability in greater detail using a range of polymer solutions formulated from hydrolyzed poly(acrylamide) (HPAA) dissolved at different concentrations in deionized water. The test fluids present a range of shear-thinning responses under steady shear, and also a wide variety of characteristic times. At low HPAA concentrations, the flow around the cylinder remains essentially symmetric for all Wi, but as the concentration increases, so does the maximum degree of the flow asymmetry observed with increasing Wi. Interestingly, at intermediate concentrations, the flow can resymmetrize at very high Wi. We understand these effects by considering simultaneously both the degree of shear-thinning of the fluid and the imposed Wi, and our analysis shows that both strong shear-thinning and high elasticity are required for the formation of strongly asymmetric flows. Our results represent the first report of this highly asymmetric flow state in polymer solutions, showing that it is a general phenomenon and not only specific to WLM. Our analysis provides a clear insight into the origins of this unusual flow state and may also be relevant to understanding other instances of asymmetries arising in shear-thinning viscoelastic flows