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We present a combined theoretical and experimental analysis of the solid-liquid interface of fused-silica nanofabricated channels with and without a hydrophilic 3-cyanopropyldimethylchlorosilane (cyanosilane) coating. We develop a model that relaxes the assumption that the surface parameters C(1), C(2), and pK(+) are constant and independent of surface composition. Our theoretical model consists of three parts: (i) a chemical equilibrium model of the bare or coated wall, (ii) a chemical equilibrium model of the buffered bulk electrolyte, and (iii) a self-consistent Gouy-Chapman-Stern triple-layer model of the electrochemical double layer coupling these two equilibrium models. To validate our model, we used both pH-sensitive dye-based capillary filling experiments as well as electro-osmotic current-monitoring measurements. Using our model we predict the dependence of ζ potential, surface charge density, and capillary filling length ratio on ionic strength for different surface compositions, which can be difficult to achieve otherwise., (Copyright © 2010 Elsevier Inc. All rights reserved.)

In this paper we evaluate the rotational viscosity and the two spin viscosities for liquid water using equilibrium molecular dynamics. Water is modeled via the flexible SPC/Fw model where the Coulomb interactions are calculated via the Wolf method which enables the long simulation times required. We find that the rotational viscosity is independent of the temperature in the range from 284 to 319 K. The two spin viscosities, on the other hand, decrease with increasing temperature and are found to be two orders of magnitude larger than that estimated by Bonthuis et al. [Phys. Rev. Lett. 103, 144503 (2009)] We apply the results from molecular dynamics simulations to the extended Navier-Stokes equations that include the coupling between intrinsic angular momentum and linear momentum. For a flow driven by an external field the coupling will reduce the flow rate significantly for nanoscale geometries. The coupling also enables conversion of rotational electrical energy into fluid linear momentum and we find that in order to obtain measurable flow rates the electrical field strength must be in the order of 0.1 MV m(-1) and rotate with a frequency of more than 100 MHz.

We study the response of a model microelectrochemical cell to a large ac voltage of frequency comparable to the inverse cell relaxation time. To bring out the basic physics, we consider the simplest possible model of a symmetric binary electrolyte confined between parallel-plate blocking electrodes, ignoring any transverse instability or fluid flow. We analyze the resulting one-dimensional problem by matched asymptotic expansions in the limit of thin double layers and extend previous work into the strongly nonlinear regime, which is characterized by two features--significant salt depletion in the electrolyte near the electrodes and, at very large voltage, the breakdown of the quasiequilibrium structure of the double layers. The former leads to the prediction of "ac capacitive desalination" since there is a time-averaged transfer of salt from the bulk to the double layers, via oscillating diffusion layers. The latter is associated with transient diffusion limitation, which drives the formation and collapse of space-charge layers, even in the absence of any net Faradaic current through the cell. We also predict that steric effects of finite ion sizes (going beyond dilute-solution theory) act to suppress the strongly nonlinear regime in the limit of concentrated electrolytes, ionic liquids, and molten salts. Beyond the model problem, our reduced equations for thin double layers, based on uniformly valid matched asymptotic expansions, provide a useful mathematical framework to describe additional nonlinear responses to large ac voltages, such as Faradaic reactions, electro-osmotic instabilities, and induced-charge electrokinetic phenomena.

We report the first use of ultrasonic standing waves to achieve cell cycle phase synchronization in mammalian cells in a high-throughput and reagent-free manner. The acoustophoretic cell synchronization (ACS) device utilizes volume-dependent acoustic radiation force within a microchannel to selectively purify target cells of desired phase from an asynchronous mixture based on cell cycle-dependent fluctuations in size. We show that ultrasonic separation allows for gentle, scalable, and label-free synchronization with high G(1) phase synchrony (approximately 84%) and throughput (3 x 10(6) cells/h per microchannel).

A new method is reported on how to measure the local pressure amplitude and the Q factor of ultrasound resonances in microfluidic chips designed for acoustophoresis of particle suspensions. The method relies on tracking individual polystyrene tracer microbeads in straight water-filled silicon/glass microchannels. The system is actuated by a PZT piezo transducer attached beneath the chip and driven by an applied ac voltage near its eigenfrequency of 2 MHz. For a given frequency a number of particle tracks are recorded by a CCD camera and fitted to a theoretical expression for the acoustophoretic motion of the microbeads. From the curve fits we obtain the acoustic energy density, and hence the pressure amplitude as well as the acoustophoretic force. By plotting the obtained energy densities as a function of applied frequency, we obtain Lorentzian line shapes, from which the resonance frequency and the Q factor for each resonance peak are derived. Typical measurements yield acoustic energy densities of the order of 10 J/m(3), pressure amplitudes of 0.2 MPa, and Q factors around 500. The observed half wavelength of the transverse acoustic pressure wave is equal within 2% to the measured width w = 377 microm of the channel.

With a growing number of cell-based biotechnological applications, there is a need for particle separation systems capable of multiparameter separations at high purity and throughput, beyond what is presently offered by traditional methods including fluorescence activated cell sorting and column-based magnetic separation. Toward this aim, we report on the integration of microfluidic acoustic and magnetic separation in a monolithic device for multiparameter particle separation. Using our device, we demonstrate high-purity separation of a multicomponent particle mixture at a throughput of up to 10(8) particleshr.

We have fabricated lab-on-a-chip systems with microchannels separated by integrated membranes allowing for osmotically driven microflows. We have investigated these flows experimentally by studying the dynamics and structure of the front of a sugar solution travelling in 200 microm wide and 50-200 microm deep microchannels. We find that the sugar front travels at a constant speed, and that this speed is proportional to the concentration of the sugar solution and inversely proportional to the depth of the channel. We propose a theoretical model, which, in the limit of low axial flow resistance, predicts that the sugar front should indeed travel with a constant velocity. The model also predicts an inverse relationship between the depth of the channel and the speed, and a linear relation between the sugar concentration and the speed. We thus find good qualitative agreement between the experimental results and the predictions of the model. Our motivation for studying osmotically driven microflows is that they are believed to be responsible for the translocation of sugar in plants through the phloem sieve element cells. Also, we suggest that osmotic elements can act as on-chip integrated pumps with no movable parts in lab-on-a-chip systems.

For a microchamber filled with a binary electrolyte and containing a flat unbiased center electrode at one wall, we employ three numerical models to study the strength of the resulting induced-charge electro-osmotic (ICEO) flow rolls: (i) a full nonlinear continuum model resolving the double layer, (ii) a linear slip-velocity model not resolving the double layer and without tangential charge transport inside this layer, and (iii) a nonlinear slip-velocity model extending the linear model by including the tangential charge transport inside the double layer. We show that, compared to the full model, the slip-velocity models significantly overestimate the ICEO flow. This provides a partial explanation of the quantitative discrepancy between observed and calculated ICEO velocities reported in the literature. The discrepancy increases significantly for increasing Debye length relative to the electrode size, i.e., for nanofluidic systems. However, even for electrode dimensions in the micrometer range, the discrepancies in velocity due to the finite Debye length can be more than 10% for an electrode of zero height and more than 100% for electrode heights comparable to the Debye length.

We demonstrate and investigate multiple localized ultrasonic manipulation functions in series in microfluidic chips. The manipulation functions are based on spatially separated and confined ultrasonic primary radiation force fields, obtained by local matching of the resonance condition of the microfluidic channel. The channel segments are remotely actuated by the use of frequency-specific external transducers with refracting wedges placed on top of the chips. The force field in each channel segment is characterized by the use of micrometer-resolution particle image velocimetry (micro-PIV). The confinement of the ultrasonic fields during single- or dual-segment actuation, as well as the cross-talk between two adjacent fields, is characterized and quantified. Our results show that the field confinement typically scales with the acoustic wavelength, and that the cross-talk is insignificant between adjacent fields. The goal is to define design strategies for implementing several spatially separated ultrasonic manipulation functions in series for use in advanced particle or cell handling and processing applications. One such proof-of-concept application is demonstrated, where flow-through-mode operation of a chip with flow splitting elements is used for two-dimensional pre-alignment and addressable merging of particle tracks.

We describe experimental and theoretical studies dedicated to establishing the physics of formation of double droplets in microfluidic systems. We show that the morphologies (complete engulfing, partial engulfing, and nonengulfing) obtained at late times minimize the interfacial energy of the system. We explain that nonequilibrium morphologies generated in the system can have long lifetimes. Remarkably, the physics of formation of the double droplets with microfluidics allows the synthesis of particles with new morphologies.

Deterministic lateral displacement (DLD) devices separate micrometer-scale particles in solution based on their size using a laminar microfluidic flow in an array of obstacles. We investigate array geometries with rational row-shift fractions in DLD devices by use of a simple model including both advection and diffusion. Our model predicts multidirectional sorting modes that could be experimentally tested in high-throughput DLD devices containing obstacles that are much smaller than the separation between obstacles.

Microfluidic chips have been fabricated in Pyrex glass to study electrokinetic pumping generated by a low-voltage ac bias applied to an in-channel asymmetric metallic electrode array. A measurement procedure has been established and followed carefully resulting in a high degree of reproducibility of the measurements over several days. A large coverage fraction of the electrode array in the microfluidic channels has led to an increased sensitivity allowing for pumping measurements at low bias voltages. Depending on the ionic concentration a hitherto unobserved reversal of the pumping direction has been measured in a regime, where both the applied voltage and the frequency are low, V(rms)<1.5 V and f<20 kHz , compared to previously investigated parameter ranges. The impedance spectrum has been thoroughly measured and analyzed in terms of an equivalent circuit diagram to rule out trivial circuit explanations of our findings. Our observations agree qualitatively, but not quantitatively, with theoretical electrokinetic models published in the literature.

We present two new types of microfluidic passive magnetic bead separator systems as well as methods for performing quantitative characterizations of them. Both systems consist of a microfluidic channel with long rectangular magnetic elements of permalloy that are placed by the sides of the channel and magnetized by an external magnetic field. In one of the systems, a staggered herringbone microfluidic mixer is integrated in the channel. The characterization of the systems includes magnetic measurements of the capture-and-release efficiencies, estimates of distributions of captured beads in a channel from micrographs, and simulations and analytical models of bead trajectories, capture efficiencies, and capture distributions. We show that the efficiencies of both systems compare favorably to those in the literature. For the studied geometries, the mixer is demonstrated to increase the bead capture-and-release efficiency for a fixed flow rate by up to a factor of two. Moreover, high capture efficiencies can be achieved in the system with mixer at up to ten times higher flow rates than in the system without mixer.

In this study of catalytic microfluidic reactors we show that, when optimally structured, these reactors share underlying scaling properties. The scaling is predicted theoretically and verified numerically. Furthermore, we show how to increase the reaction rate significantly by distributing the active porous material within the reactor using a high-level implementation of topology optimization.

The dynamics in the onset of a Hagen-Poiseuille flow of an incompressible liquid in a channel of circular cross section is well-studied theoretically. We use an eigenfunction expansion in a Hilbert space formalism to generalize the results to channels of an arbitrary cross section. We find that the steady state is reached after a characteristic time scale tau=(A/P)2(1/nu), where A and P are the cross-sectional area and perimeter, respectively, and nu is the kinematic viscosity of the liquid. For the initial dynamics of the flow rate Q for t<

Recent experiments have demonstrated that ac electrokinetic micropumps permit integrable, local, and fast pumping (velocities approximately mm/s) with low driving voltage of a few volts only. However, they also displayed many quantitative and qualitative discrepancies with existing theories. We therefore extend the latter theories to account for three experimentally relevant effects: (i) vertical confinement of the pumping channel, (ii) Faradaic currents from electrochemical reactions at the electrodes, and (iii) nonlinear surface capacitance of the Debye layer. We report here that these effects indeed affect the pump performance in a way that we can rationalize by physical arguments.

We present the design, test and theoretical analysis of a novel micropump. The purpose is to make a pump with large flow rate (approximately 10 microL min-1) and high pressure capacity (approximately 1 bar) powered by a low voltage DeltaV<30 V. The pump is operated in AC mode with an electroosmotic actuator in connection with a full wave rectifying valve system. Individual valves are based on a flexible membrane with a slit. Bubble-free palladium electrodes are implemented in order to increase the range of applications and reduce maintenance.

We study theoretically the capturing of paramagnetic beads by a magnetic field gradient in a microfluidic channel treating the beads as a continuum. Bead motion is affected by both fluidic and magnetic forces. The transfer of momentum from beads to the fluid creates an effective bead-bead interaction that greatly aids capturing. We demonstrate that for a given inlet flow speed a critical density of beads exists above which complete capturing takes place.

We present a capillary flow system for liquid transport in microsystems. Our simple microfluidic system consists of two planar parallel surfaces, separated by spacers. One of the surfaces is entirely hydrophobic, the other mainly hydrophobic, but with hydrophilic pathways defined on it by photolithographic means. By controlling the wetting properties of the surfaces in this manner, the liquid can be confined to certain areas defined by the hydrophilic pathways. This technique eliminates the need for alignment of the two surfaces. Patterned plasma-polymerized hexafluoropropene constitutes the hydrophobic areas, whereas the untreated glass surface constitutes the hydrophilic pathways. We developed a theoretical model of the capillary flow and obtained analytical solutions which are in good agreement with the experimental results. The capillarity-driven microflow system was also used to pattern and immobilize biological material on planar substrates: well-defined 200 microm wide strips of human cells (HeLa) and fluorescence labelled proteins (fluorescein isothiocyanate-labelled bovine serum albumin, i.e., FITC-BSA) were fabricated using the capillary flow system presented here.

We present the design, fabrication and test of a novel inline frit-based electroosmotic (EO) pump with ion exchange membranes. The pump is more stable than previous types due to a new flow component that ensures a controlled width of the diffusion layer close to the ion exchange membranes. The pump casing is constructed in polymers while the EO active part, the frit, is made in a nanoporous silica. The pressure capability of the pump is Deltapm/DeltaV = 0.15 bar V(-1). The flow rate to current ratio is Qm/I = 6 microL min(-1) mA(-1). This translates to Deltapm = 4.5 bar and Qm = 6 microL min(-1) at DeltaV = 30 V. The pump has been tested with four different buffer concentrations. In order to investigate day-to-day reproducibility each Q-p pump characteristic has been recorded several times during hour-long operation runs under realistic operating conditions.

We consider pressure-driven, steady-state Poiseuille flow in straight channels with various cross-sectional shapes: elliptic, rectangular, triangular, and harmonic-perturbed circles. A given shape is characterized by its perimeter P and area A which are combined into the dimensionless compactness number C= P2/A, while the hydraulic resistance is characterized by the well-known dimensionless geometrical correction factor alpha. We find that alpha depends linearly on C, which points out C as a single dimensionless measure characterizing flow properties as well as the strength and effectiveness of surface-related phenomena central to lab-on-a-chip applications. This measure also provides a simple way to evaluate the hydraulic resistance for the various shapes.

A disposable single use polymer microfluidics chip has been developed and manufactured by micro injection molding. The chip has the same outer dimensions as a standard microscope slide (25 x 76 x 1.1 mm) and is designed to be compatible with existing microscope slide handling equipment like microarray scanners. The chip contains an inlet, a 10 microL hybridization chamber capable of holding a 1000 spot array, a waste chamber and a vent to allow air to escape when sample is injected. The hybridization chamber ensures highly homogeneous hybridization conditions across the microarray. We describe the use of this chip in a flexible setup with fluorescence based detection, temperature control and liquid handling by computer controlled syringe pumps. The chip and the setup presented in this article provide a powerful tool for highly parallel studies of kinetics and thermodynamics of duplex formation in DNA microarrays. The experimental setup presented in this article enables the on-chip microarray to be hybridized and monitored at several different stringency conditions during a single assay. The performance of the chip and the setup is demonstrated by on-line measurements of a hybridization of a DNA target solution to a microarray. A presented numerical model indicates that the hybridization process in microfluidic hybridization assays is diffusion limited, due to the low values of the diffusion coefficients D of the DNA and RNA molecules involved.