We demonstrate rectification of ionic transport in a nanofluidic diode fabricated by introducing a surface charge discontinuity in a nanofluidic channel. Device current-voltage (I-V) characteristics agree qualitatively with a one-dimensional model at moderate to high ionic concentrations. This study illustrates ionic flow control using surface charge patterning in nanofluidic channels under high bias voltages.
Conductance characteristics of nanofluidic channels (nanochannels) fall into two regimes: at low ionic concentrations, conductance is governed by surface charge while at high ionic concentrations it is determined by nanochannel geometry and bulk ionic concentration. We used aminosilane chemistry and streptavidin-biotin binding to study the effects of surface reactions on nanochannel conductance at different ionic concentrations. Immobilization of small molecules such as aminosilane or biotin mainly changes surface charge, affecting conductance only in the low concentration regime. However, streptavidin not only modifies surface charge but also occludes part of the channel, resulting in observable conductance changes in both regimes. Our observations reflect the interplay between the competing effects of charge and size of streptavidin on nanochannel conductance.
The acoustic mismatch model (AMM) and the diffuse mismatch model (DMM) have been traditionally used to calculate the thermal boundary conductance of interfaces. In these calculations, the phonon dispersion relationship is usually approximated by a linear relationship (Debye approximation). This is accurate for wave vectors close to the zone center, but deviates significantly for wave vectors near the zone edges. Here, we present DMM calculations of the thermal conductance of Al–Si, Al–Ge, Cu–Si, and Cu–Ge interfaces by taking into account the full phonon dispersion relationship over the entire Brillouin zone obtained using the Born-von Karman model (BKM). The thermal boundary conductance thus calculated deviates significantly from DMM predictions obtained using the Debye model in all cases.
Electrostatic interactions play an important role in nanofluidic channels when the channel size is comparable to the Debye screening length. Electrostatic fields have been used to control concentration and transport of ions in nanofluidic transistors. Here, we report a transistor-reservoir-transistor circuit that can be used to turn “on” or “off” protein transport using electrostatic fields with gate voltages of ±1V. Our results suggest that global electrostatic interactions of the protein were dominant over other interactions in the nanofluidic transistor. The fabrication technique also demonstrates the feasibility of nanofluidic integrated circuits for the manipulation of biomolecules in picoliter volumes.
When biomolecular reactions occur on one surface of a microcantilever beam, changes in intermolecular forces create surface stresses that bend the cantilever. While this phenomenon has been exploited to create label-free biosensors and biomolecular actuators, the mechanisms through which chemical free energy is transduced to mechanical work in such hybrid systems are not fully understood. To gain insight into these mechanisms, we use DNA hybridization as a model reaction system. We first show that the surface grafting density of single-stranded probe DNA (sspDNA) on a surface is strongly correlated to its radius of gyration in solution, which in turn depends on its persistence length and the DNA chain length. Since the persistence length depends on ionic strength, the grafting density of sspDNA can be controlled by changing a solution's ionic strength. The surface stresses produced by the reaction of complementary single-stranded target DNA (sstDNA) to sspDNA depend on the length of DNA, the grafting density, and the hybridization efficiency. We, however, observe a remarkable trend: regardless of the length and grafting density of sspDNA, the surface stress follows an exponential scaling relation with the density of hybridized sspDNA.
Solar cells made from blends of conjugated polymers and nanostructured inorganic materials are an important class of organic photovoltaic devices. However, there has been no systematic theoretical analysis of their operation and performance. In this paper, we develop a theoretical model to analyze the performance of two classes of heterojunction solar cells composed of ordered nanostructures. Based on the simulations, we conclude that in order to obtain reasonable efficiencies, the size and spacing of the nanostructures must be on the order of the exciton diffusion length scale. Possible quantum and other confinement effects are qualitatively discussed.
The surface grafting density of biomolecules is an important factor for quantitative assays using a wide range of biological sensors. We use a fluorescent measurement technique to characterize the immobilization density of thiolated probe DNA on gold and hybridization efficiency of target DNA as a function of oligonucleotide length and salt concentration. The results indicate the dominance of osmotic and hydration forces in different regimes of salt concentration, which was used to validate previous simulations and to optimize the performance of surface-stress based microcantilever biosensors. The difference in hybridization density between complementary and mismatched target sequences was also measured to understand the response of these sensors in base-pair mismatch detection experiments. Finally, two different techniques for immobilizing proteins on gold were considered and the surface densities obtained in both cases were compared.
Diffusion-limited patterning (DLP) is a new technique that enables patterning of labile molecular species in solution phase onto surfaces that are not easily accessible. This technique is self-aligning and is simple to implement for patterning multiple species. We demonstrated DLP by patterning alternating bands of fluorescently labeled and unlabeled streptavidin in biotin-functionalized nanofluidic channels with spatial resolution better than 1 microm. The methodology of DLP also enables experimental measurement of a unique parameter that relates molecular surface grafting density, concentration, diffusivity, and channel geometry.
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