Highly parallel simulation tool for the design of isotachophoresis experiments.

Background: Isotachophoresis (ITP) is a well-established electrokinetic method for separation and preconcentration of analytes. Several simulation tools for ITP have been published, but their use for experimental design is limited by the computational time for a single run and/or by the number of conditions that can be investigated per simulation run. A large fraction of the existing solvers also do not account for ionic strength effects, which can influence whether an analyte focuses in ITP.

Mechanism of sinuous and varicose modes in electrokinetic instability.

The flow of miscible electrolyte streams with mismatched electrical conductivities in the presence of a parallel applied electric field is known to exhibit electrokinetic instability (EKI). This paper deals with EKI in a configuration where the base state is established by electro-osmotic flow (EOF) of three coflowing streams, with the center stream having different conductivity than the sheath streams. All reported experiments of this EKI have shown that the instability exhibits either sinuous or varicose modes depending upon whether the center stream has higher or lower conductivity than the sheath streams, respectively.

A neural network model for rapid prediction of analyte focusing in isotachophoresis.

We present the development and demonstration of a neural network (NN) model for fast and accurate prediction of whether or not a chosen analyte is focused by an isotachophoresis (ITP) buffer system. The NN model is useful in the rapid evaluation of possible ITP chemistries applicable to analytes of interest. We trained and tested the NN model for univalent species based on extensive data sets of over 10,000 anionic and 10,000 cationic ITP simulations.

Lattice Boltzmann finite-difference-based model for fully nonlinear electrohydrodynamic deformation of a liquid droplet.

Electric field-induced flows involving multiple fluid components with a range of different electrical properties are described by the coupled Taylor-Melcher leaky-dielectric model. We present a lattice Boltzmann (LB)-finite difference (FD) method-based hybrid framework to solve the complete Taylor-Melcher leaky-dielectric model considering the nonlinear surface charge convection effects. Unlike the existing LB-based models, we treat the interfacial discontinuities using direction-specific continuous gradients, which prevents the miscalculation arising due to volumetric gradients without directional derivatives, simultaneously maintaining the electroneutrality of the bulk.

Physics of moderately stretched electrified jets in electrohydrodynamic jet printing.

Electrohydrodynamic (EHD) jet printing involves the deposition of a liquid jet issuing from a needle stretched under the effect of a strong electric field between the needle and a collector plate. Unlike the geometrically independent classical cone-jet observed at low flow rates and high applied electric fields, at a relatively high flow rate and moderate electric field, EHD jets are moderately stretched. Jetting characteristics of such moderately stretched EHD jets differ from the typical cone-jet due to the nonlocalized cone-to-jet transition.

Rapid prototyping of polydimethylsiloxane (PDMS) microchips using electrohydrodynamic jet printing: Application to electrokinetic assays.

Polydimethylsiloxane (PDMS) based microfluidic devices have found increasing utility for electrophoretic and electrokinetic assays because of their ease of fabrication using replica molding. However, the fabrication of high-resolution molds for replica molding still requires the resource-intensive and time-consuming photolithography process, which precludes quick design iterations and device optimization. We here demonstrate a low-cost, rapid microfabrication process, based on electrohydrodynamic jet printing (EJP), for fabricating non-sacrificial master molds for replica molding of PDMS microfluidic devices.

A simplified model of oscillating electrolytes.

Unstable electrophoretic transport leading to oscillations in concentration profiles occur in certain electrolyte systems known as oscillating electrolytes whose eigenmobilities are complex valued. The study of the nonlinear behavior of such systems is of great interest but is constrained due to a high degree of complexity in the governing equations. Here we present a simplified model of unstable electrophoretic transport in a binary system that reduces the governing equations to two partial differential equations only and does away with other equations that characterize acid-base dissociation reactions and electroneutrality.

Electrophoresis simulations using Chebyshev pseudo-spectral method on a moving mesh.

We present the implementation and demonstration of the Chebyshev pseudo-spectral method coupled with an adaptive mesh method for performing fast and highly accurate electrophoresis simulations. The Chebyshev pseudo-spectral method offers higher numerical accuracy than all other finite difference methods and is applicable for simulating all electrophoresis techniques in channels with open or closed boundaries. To improve the computational efficiency, we use a novel moving mesh scheme that clusters the grid points in the regions with poor numerical resolution.

Web-Based Open-Source Tool for Isotachophoresis.

We present the development of a client-side web-based simulator for complex electrophoresis phenomena, including isotachophoresis. The simulation tool is called Client-based Application for Fast Electrophoresis Simulation (CAFES). CAFES uses the broad cross-browser compatibility of JavaScript to provide a rapid and easy-to-use tool for coupled unsteady electromigration, diffusion, and equilibrium electrolyte reactions among multiple weak electrolytes.

An inexpensive microfluidic device for three-dimensional hydrodynamic focusing in imaging flow cytometry.

We present design, characterization, and testing of an inexpensive, sheath-flow based microfluidic device for three-dimensional (3D) hydrodynamic focusing of cells in imaging flow cytometry. In contrast to other 3D sheathing devices, our device hydrodynamically focuses the cells in a single-file near the bottom wall of the microchannel that allows imaging cells with high magnification and low working distance objectives, without the need for small device dimensions. The relatively large dimensions of the microchannels enable easy fabrication using less-precise fabrication techniques, and the simplicity of the device design avoids the need for tedious alignment of various layers.

High-resolution numerical simulations of electrophoresis using the Fourier pseudo-spectral method.

We present the formulation, implementation, and performance evaluation of the Fourier pseudo-spectral method for performing fast and accurate simulations of electrophoresis. We demonstrate the applicability of this method for simulating a wide variety of electrophoretic processes such as capillary zone electrophoresis, transient-isotachophoresis, field amplified sample stacking, and oscillating electrolytes. Through these simulations, we show that the Fourier pseudo-spectral method yields accurate and stable solutions on coarser computational grids compared with other nondissipative spatial discretization schemes.

A fully coupled hybrid lattice Boltzmann and finite difference method-based study of transient electrokinetic flows.

Transient electrokinetic (EK) flows involve the transport of conductivity gradients developed as a result of mixing of ionic species in the fluid, which in turn is affected by the electric field applied across the channel. The presence of three different coupled equations with corresponding different time scales makes it difficult to model the problem using the lattice Boltzmann method (LBM). The present work aims to develop a hybrid LBM and finite difference method (FDM)-based model which can be used to study the electro-osmotic flows (EOFs) and the onset of EK instabilities using an Ohmic model, where fluid and conductivity transport are solved using LBM and the electric field is solved using FDM.

Effect of surface conduction-induced electromigration on current monitoring method for electroosmotic flow measurement.

Current monitoring method for measurement of EOF in microchannels involves measurement of time-varying current while an electrolyte displaces another electrolyte having different conductivity due to EOF. The basic premise of the current monitoring method is that an axial gradient in conductivity of a binary electrolyte in a microchannel advects only due to EOF. In the current work, using theory and experiments, we show that this assumption is not valid for low concentration electrolytes and narrow microchannels wherein surface conduction is comparable with bulk conduction.

Scaling behavior in on-chip field-amplified sample stacking.

Field amplified sample stacking (FASS) uses differential electrophoretic velocity of analyte ions in the high-conductivity background electrolyte zone and low conductivity sample zone for increasing the analyte concentration. The stacking rate of analyte ions in FASS is limited by molecular diffusion and convective dispersion due to nonuniform electroosmotic flow (EOF). We present a theoretical scaling analysis of stacking dynamics in FASS and its validation with a large set of on-chip sample stacking experiments and numerical simulations.

Electrohydrodynamic instability of ion-concentration shock wave in electrophoresis.

Capillary electrophoresis techniques often involve ion-concentration shock waves in an electrolyte solution, propagating under the effect of an external electric field. These shock waves are characterized by self-sharpening gradients in ion concentrations and electrical conductivity that are collinear with the electric field. The coupling of electric field and fluid motion at the shock interface sometimes leads to an undesirable electrohydrodynamic (EHD) instability.

Mechanism of electrohydrodynamic instability with collinear conductivity gradient and electric field.

We describe the physical mechanism responsible for electrohydrodynamic (EHD) instability of a fluid layer with collinear conductivity gradient and electric field. In particular, we resolve the ambiguity in literature regarding the cause for switching between stationary and oscillatory modes of EHD instability. Using linear stability analysis, we show that a small perturbation in conductivity field perturbs the local electric field and also induces a perturbation charge.

Capillary Displacement of Viscous Liquids in Geometries with Axial Variations.

Axial variations in geometry and presence of viscous displaced fluid are known to alter the diffusive-dynamics of capillary imbibition of a wetting liquid. We here show that the coupled effect of axially varying capillary geometry and finite viscosity of the displaced fluid can lead to significant variations in both short and long time dynamics of imbibition. Based on a theoretical model and lattice Boltzmann simulations, we analyze capillary displacement of a viscous liquid in straight and diverging capillaries.

Theory of multi-species electrophoresis in the presence of surface conduction.

Electrophoresis techniques are characterized by concentration disturbances (or waves) propagating under the effect of an electric field. These techniques are usually performed in microchannels where surface conduction through the electric double layer (EDL) at channel walls is negligible compared with bulk conduction. However, when electrophoresis techniques are integrated in nanochannels, shallow microchannels or charged porous media, surface conduction can alter bulk electrophoretic transport.

Uncertainty quantification in modeling of microfluidic T-sensor based diffusion immunoassay.

Comparison of experimental data with modeling predictions is essential for making quantitative measurements of species properties, such as diffusion coefficients and species concentrations using a T-sensor. To make valid comparisons between experimental data and model predictions, it is necessary to account for uncertainty in model predictions due to uncertain values of model parameters. We present an analysis of uncertainty induced in model predictions of a T-sensor based competitive diffusion immunoassay due to uncertainty in diffusion constants, binding reaction rate constants, and inlet flow speed.

Stability of electrophoretic transport of ions.

We present an investigation of instability during electrophoretic transport of ions in a class of electrolytes called oscillating electrolytes. We analyze the onset of instability in electrophoretic transport in a binary electrolyte by modeling growth of small concentration disturbances over a base state with uniform acid and base concentrations. Our linear stability analysis shows that the growth rate of low wave-number concentration disturbances increases with an increase in wave number.

Coupling isotachophoresis and capillary electrophoresis: a review and comparison of methods.

We present a comprehensive review and comparison of the methodologies for increasing sensitivity and resolution of capillary electrophoresis (CE) using online transient isotachophoresis (tITP). We categorize the diverse set of coupled tITP and CE (tITP-CE) methods based on their fundamental principles for disrupting isotachophoretic preconcentration and triggering electrophoretic separation. Based on this classification, we discuss important features, advantages, limitations, and optimization principles of various tITP-CE methods.

Integration of rapid DNA hybridization and capillary zone electrophoresis using bidirectional isotachophoresis.

We present a method for rapid, sequence-specific detection of multiple DNA fragments by integrating isotachophoresis (ITP) based DNA hybridization and capillary zone electrophoresis (CZE) using bidirectional ITP. Our method leverages the high preconcentration ability of ITP to accelerate slow, second-order DNA hybridization kinetics, and the high resolving power of CZE to separate and identify reaction products. We demonstrate the speed and sensitivity of our assay by detecting 5 pM, 39 nt ssDNA target within 3 min, using a molecular beacon probe.

Effect of PVP on the electroosmotic mobility of wet-etched glass microchannels.

We present an experimental study on the effect of polymer PVP on EOF mobility of microchannels wet etched into optical white soda lime glass, also known as Crown glass. We performed experiments to evaluate the effect of PVP concentration and pH on EOF mobility. We used on-chip capillary zone electrophoresis and a neutral fluorescent dye as a passive marker to quantify the electroosmotic flow.

Robust and high-resolution simulations of nonlinear electrokinetic processes in variable cross-section channels.

We present a model and an associated numerical scheme to simulate complex electrokinetic processes in channels with nonuniform cross-sectional area. We develop a quasi-1D model based on local cross-sectional area averaging of the equations describing unsteady, multispecies, electromigration-diffusion transport. Our approach uses techniques of lubrication theory to approximate electrokinetic flows in channels with arbitrary variations in cross-section; and we include chemical equilibrium calculations for weak electrolytes, Taylor-Aris type dispersion due of nonuniform bulk flow, and the effects of ionic strength on species mobility and on acid-base equilibrium constants.

Desalination and hydrogen, chlorine, and sodium hydroxide production via electrophoretic ion exchange and precipitation.

We demonstrate and analyze a novel desalination method which works by electrophoretically replacing sodium and chloride in feed salt water with a pair of ions, calcium and carbonate, that react and precipitate out. The resulting calcium carbonate precipitate is benign to health, and can be filtered or settled out, yielding low ionic strength product water. The ion exchange and precipitation employs self-sharpening interfaces induced by movement of multiple ions in an electric field to prevent contamination of the product water.