Mohammad Amin Alibakhshi

Label-Free Electrical Detection of Enzymatic Reactions in Nanochannels.

We report label-free electrical detection of enzymatic reactions using 2-D nanofluidic channels and investigate reaction kinetics of enzymatic reactions on immobilized substrates in nanoscale-confined spaces. Trypsin proteolysis is chosen for demonstration of the detection scheme. When trypsin cleaves poly-l-lysine coated on the surface of silica nanochannels, the resulting change of surface charge density can be detected by monitoring the ionic conductance of the nanochannels. Our results show that detection of such surface enzymatic reactions is faster than detection of surface binding reactions in nanochannels for low-concentration analytes. Furthermore, the nanochannel sensor has a sensitivity down to 5 ng/mL, which statistically corresponds to a single enzyme per nanochannel. Our results also suggest that enzyme kinetics in nanochannels is fundamentally different from that in bulk solutions or plain surfaces. Such enzymatic reactions form two clear self-propagating reaction fronts inside the nanochannels, and the reaction fronts follow square-root time dependences at high enzyme concentrations due to significant nonspecific adsorption. However, at low enzyme concentrations when nonspecific adsorption is negligible, the reaction fronts propagate linearly with time, and the corresponding propagation speed is related to the channel geometry, enzyme concentration, catalytic reaction constant, diffusion coefficient, and substrate surface density. Optimization of this nanochannel sensor could lead to a quick-response, highly sensitive, and label-free sensor for enzyme assay and kinetic studies.

Accurate measurement of liquid transport through nanoscale conduits

Nanoscale liquid transport governs the behaviour of a wide range of nanofluidic systems, yet remains poorly characterized and understood due to the enormous hydraulic resistance associated with the nanoconfinement and the resulting minuscule flow rates in such systems. To overcome this problem, here we present a new measurement technique based on capillary flow and a novel hybrid nanochannel design and use it to measure water transport through single 2-D hydrophilic silica nanochannels with heights down to 7 nm. Our results show that silica nanochannels exhibit increased mass flow resistance compared to the classical hydrodynamics prediction. This difference increases with decreasing channel height and reaches 45% in the case of 7 nm nanochannels. This resistance increase is attributed to the formation of a 7-angstrom-thick stagnant hydration layer on the hydrophilic surfaces. By avoiding use of any pressure and flow sensors or any theoretical estimations the hybrid nanochannel scheme enables facile and precise flow measurement through single nanochannels, nanotubes, or nanoporous media and opens the prospect for accurate characterization of both hydrophilic and hydrophobic nanofluidic systems.

Effects of multi-scattering on the performance of a single-beam acoustic manipulation device

The effects of multiple scattering on acoustic manipulation of spherical particles using helicoidal Bessel-beams are discussed. A closed-form analytical solution is developed to calculate the acoustic radiation force resulting from a Besselbeam on an acoustically reflective sphere, in the presence of an adjacent spherical particle, immersed in an unbounded fluid medium. The solution is based on the standard Fourier decomposition method and the effect of multi-scattering is taken into account using the addition theorem for spherical coordinates. Of particular interest here is the investigation of the effects of multiple scattering on the emergence of negative axial forces. To investigate the effects, the radiation force applied on the target particle resulting from a helicoidal Bessel-beam of different azimuthal indexes (m = 1 to 4), at different conical angles, is computed. Results are presented for soft and rigid spheres of various sizes, separated by a finite distance. Results have shown that the emergence of negative force regions is very sensitive to the level of cross-scattering between the particles. It has also been shown that in multiple scattering media, the negative axial force may occur at much smaller conical angles than previously reported for single particles, and that acoustic manipulation of soft spheres in such media may also become possible.

Exploring Ultimate Water Capillary Evaporation in Nanoscale Conduits

Capillary evaporation in nanoscale conduits is an efficient heat/mass transfer strategy that has been widely utilized by both nature and mankind. Despite its broad impact, the ultimate transport limits of capillary evaporation in nanoscale conduits, governed by the evaporation/condensation kinetics at the liquid-vapor interface, have remained poorly understood. Here we report experimental study of the kinetic limits of water capillary evaporation in two dimensional nanochannels using a novel hybrid channel design. Our results show that the kinetic-limited evaporation fluxes break down the limits predicated by the classical Hertz-Knudsen equation by an order of magnitude, reaching values up to 37.5 mm/s with corresponding heat fluxes up to 8500 W/cm2. The measured evaporation flux increases with decreasing channel height and relative humidity but decreases as the channel temperature decreases. Our findings have implications for further understanding evaporation at the nanoscale and developing capillary evaporation-based technologies for both energy- and bio-related applications.

Geometrical control of ionic current rectification in a configurable nanofluidic diode

Control of ionic current in a nanofluidic system and development of the elements analogous to electrical circuits have been the subject of theoretical and experimental investigations over the past decade. Here, we theoretically and experimentally explore a new technique for rectification of ionic current using asymmetric 2D nanochannels. These nanochannels have a rectangular cross section and a stepped structure consisting of a shallow and a deep side. Control of height and length of each side enables us to obtain optimum rectification at each ionic strength. A 1D model based on the Poisson-Nernst-Planck equation is derived and validated against the full 2D numerical solution, and a nondimensional concentration is presented as a function of nanochannel dimensions, surface charge, and the electrolyte concentration that summarizes the rectification behavior of such geometries. The rectification factor reaches a maximum at certain electrolyte concentration predicted by this nondimensional number and decays away from it. This method of fabrication and control of a nanofluidic diode does not require modification of the surface charge and facilitates the integration with lab-on-a-chip fluidic circuits. Experimental results obtained from the stepped nanochannels are in good agreement with the 1D theoretical model.

Instantaneous beamwidth measurements of an electrohydraulic lithotripter

Acoustic field measurements of electrohydraulic lithotripters (EHL) are typically conducted with single-element hydrophones and are subject to spatial averaging errors because the spark source location varies from shock to shock. Linear hydrophone arrays provide a means of obtaining the instantaneous sound field of EHLs and a more detailed understanding of EHL sound fields. Here, 20-element hydrophone arrays were used to study the variability of the instantaneous acoustic field of an experimental EHL. Calibrated arrays were placed at the geometric focus of an EHL and exposed to as many as 1500 shock waves using excitations of 14, 17 and 20 kV. Instantaneous data were acquired from all 20 hydrophone elements and then were processed for beamwidth, peak pressure location, and peak pressure. Instantaneous beamwidths were found to be smaller than when using a single-element hydrophone approach and peak pressures were observed to vary more as the excitation voltage increased.

Single-shot measurements of the acoustic field of an electrohydraulic lithotripter using a hydrophone array.

Piezopolymer-based hydrophone arrays consisting of 20 elements were fabricated and tested for use in measuring the acoustic field from a shock-wave lithotripter. The arrays were fabricated from piezopolymer films and were mounted in a housing to allow submersion into water. The motivation was to use the array to determine how the shot-to-shot variability of the spark discharge in an electrohydraulic lithotripter affects the resulting focused acoustic field. It was found that the dominant effect of shot-to-shot variability was to laterally shift the location of the focus by up to 5 mm from the nominal acoustic axis of the lithotripter. The effect was more pronounced when the spark discharge was initiated with higher voltages. The lateral beamwidth of individual, instantaneous shock waves were observed to range from 1.5 mm to 24 mm. Due to the spatial variation of the acoustic field, the average of instantaneous beamwidths were observed to be 1 to 2 mm narrower than beamwidths determined from traditional single-point measurements that average the pressure measured at each location before computing beamwidth.