[Show abstract][Hide abstract] ABSTRACT: This paper presents a study of electrokinetic transport in single nanopores integrated into vertically stacked three-dimensional hybrid microfluidicnanofluidic structures. In these devices, single nanopores, created by focused ion beam (FIB) milling in thin polymer films, provide fluidic connection between two vertically separated, perpendicular microfluidic channels. Experiments address both systems in which the nanoporous membrane is composed of the same (homojunction) or different (heterojunction) polymer as the microfluidic channels. These devices are then used to study the electrokinetic transport properties of synthetic (i.e., polystyrene sulfonate and polyallylamine) and biological (i.e., DNA) polyelectrolytes across these nanopores using both electrical current measurements and confocal microscopy. Both optical and electrical measurements indicate that electro-osmotic transport is predominant over electrophoresis in single nanopores with d>180 nm, consistent with results obtained under similar conditions for nanocapillary array membranes.
[Show abstract][Hide abstract] ABSTRACT: Ionic transport in nanopores is dependent on the nature of the electrical communication between the pores and the surrounding environment. A particularly useful fluidic device structure uses nanopores in nanocapillary array membranes (NCAMs) as electrically switchable valves between vertically separated microfluidic channels. In the off-state, the gate isolates the fluidic environments in the microchannels, but when the appropriate forward-bias voltage is applied, it selectively allows ions and analytes to move between the microchannels. However, the populations of species in the microfluidic channels are perturbed from their steady-state values due to ion accumulation and depletion effects. Experiments conducted here characterize the electrical conduction along the length of a microfluidic channel, and laser-induced fluorescence probes the formation of a high-and low-concentration regions of fluorescent dye before and after application of forward-and reverse-bias voltage pulses in both small (a) 10 nm) and large (a) 100 nm) pore NCAMs. In all cases, switching from injection (transport across the NCAM) to microfluidic flow (transport only in the microfluidic channel) results in a multiphasic current recovery profile, signifying the presence of ion accumulation and depletion regions at the microfluidic-nanofluidic boundary, that is, in the region adjacent to the NCAM. The behavior is consistent with a model in which a volume of altered ion concentration is created at the microfluidic-nanofluidic boundary upon injection. Switching back to microfluidic flow causes this altered conductivity region to be swept from the microfluidic channel, re-establishing the steady state conduction properties.
The Journal of Physical Chemistry C 12/2008; 112(49). DOI:10.1021/jp806257d · 4.77 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Nanofluidics presents growing and exciting opportunities for conducting fundamental studies for processes and systems that govern molecular-scale operations in science and engineering. In addition, nanofluidics provides a rapidly growing platform for developing new systems and technologies for an ever-growing list of applications. This review presents a summary of the transport phenomena in nanofluidics with a focus on several systems and applications important to problems of public health and welfare. Special emphasis is afforded to the role of the electric double layer and the molecular-scale interactions that occur within confined nanoscale systems.
[Show abstract][Hide abstract] ABSTRACT: Hybrid micro-nanofluidic interconnect devices can be used to control analyte transfer from one microchannel to the other through a nanochannel under rest, injection, and recovery stages of operation by varying the applied potential bias. Using numerical simulations based on coupled transient Poisson-Nernst-Planck and Stokes equations, we examine the electrokinetic transport in a gateable device consisting of two 100 microm long, 1 microm wide negatively charged microchannels connected by a 1 microm long, 10 nm wide positively charged nanochannel under both positive and negative bias potentials. During injection, accumulation of ions is observed at the micro-nano interface region with the positive potential and depletion of ions is observed at the other micro-nano junction region. Net space charge in the depletion region gives rise to nonlinear electrokinetic transport during the recovery stage due to induced pressure, induced electroosmotic flow of the second kind, and complex flow circulations. Ionic currents are computed as a function of time for both positive and negative bias potentials for the three stages. Analytical expressions derived for ion current variation are in agreement with the simulated results. In the presence of multiple accumulation or depletion regions, we show that a hybrid micro-nano device can be designed to function as a logic gate.
[Show abstract][Hide abstract] ABSTRACT: The extension of microfluidic devices to three dimensions requires innovative methods to interface fluidic layers. Externally controllable interconnects employing nanocapillary array membranes (NCAMs) have been exploited to produce hybrid three-dimensional fluidic architectures capable of performing linked sequential chemical manipulations of great power and utility. Because the solution Debye length, kappa(-1), is of the order of the channel diameter, a, in the nanopores, fluidic transfer is controlled through applied bias, polarity and density of the immobile nanopore surface charge, solution ionic strength and the impedance of the nanopore relative to the microfluidic channels. Analyte transport between vertically separated microchannels can be saturated at two stable transfer levels, corresponding to reverse and forward bias. These NCAM-mediated integrated microfluidic architectures have been used to achieve highly reproducible and tunable injections down to attoliter volumes, sample stacking for preconcentration, preparative analyte band collection from an electrophoretic separation, and an actively-tunable size-dependent transport in hybrid structures with grafted polymers displaying thermally-regulated swelling behavior. The synthetic elaboration of the nanopore interior has also been used to great effect to realize molecular separations of high efficiency. All of these manipulations depend critically on the transport properties of individual nanocapillaries, and the study of transport in single nanopores has recently attracted significant attention. Both computation and experimental studies have utilized single nanopores as test beds to understand the fundamental chemical and physical properties of chemistry and fluid flow at nanometer length scales.
[Show abstract][Hide abstract] ABSTRACT: Integrated microfluidic structures, comprised of three-dimensional assemblies of microfluidic channels, can effect sequentially-linked analytical operations with mass-limited samples. This three-dimensional operation is enabled by electrically-switchable nanocapillary array membranes with novel transport properties.
The Analyst 07/2006; 131(6):705-9. DOI:10.1039/b600158k · 4.11 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Electrokinetic fluid flow in nanocapillary array (NCA) membranes between vertically separated microfluidic channels offers an attractive alternative to using mechanical action to achieve fluidic communication between different regions of lab-on-a-chip devices. By adjusting the channel diameter, a, and the inverse Debye length, к, and applying the appropriate external potential, the nanochannel arrays, can be made to behave like digital fluidic switches, and the movement of molecules from one side of the array to the other side can be controlled. However, inherent differences in ionic mobility lead to non-equilibrium ion populations on the downstream side, which, in turn, shows up through transient changes in the microchannel conductance. Here we describe coupled calculations and experiments in which the electrical properties of a microfluidic–nanofluidic hybrid architecture are simulated by a combination of a compact model for the bulk electrical properties and iterative self-consistent solutions of the coupled Poisson, Nernst–Planck, and Navier–Stokes equations to recover the detailed ion motion in the nanopores. The transient electrical conductivity in the microchannel, after application of a forward bias pulse to the NCA membrane, is recovered in quantitative detail. The surface charge density of the nanopores and the capacitance of the membrane, which are critical determinants of electrokinetic flow through NCA, fall out of the analysis in a natural way, providing a clear mechanism to determine these critically important parameters.
Journal of Nanoparticle Research 09/2005; 7(4):507-516. DOI:10.1007/s11051-005-5133-x · 2.18 Impact Factor