We demonstrate a pH sensor based on ultrasensitive nanosize Schottky junctions formed within bottom-up grown dopant-free arrays of assembled silicon nanowires. A new measurement concept relying on a continuous gate sweep is presented, which allows the straightforward determination of the point of maximum sensitivity of the device and allows sensing experiments to be performed in the optimum regime. Integration of devices into a portable fluidic system and an electrode isolation strategy affords a stable environment and enables long time robust FET sensing measurements in a liquid environment to be carried out. Investigations of the physical and chemical sensitivity of our devices at different pH values and a comparison with theoretical limits are also discussed. We believe that such a combination of nanofabrication and engineering advances make this Schottky barrier-powered silicon nanowire lab-on-a-chip platform suitable for efficient biodetection and even for more complex biochemical analysis
Abstract:We present a biosensor chip with integrated large area silicon nanowire-based field effect transistors (FET) for human α-thrombin detection and propose to implement the hysteresis width of the FET transfer curve as a reliable parameter to quantify the concentration of biomolecules in the solution. We further compare our results to conventional surface potential based measurements and demonstrate that both parameters distinctly respond at a different analyte concentration range. A combination of the two approaches would provide broader possibilities for detecting biomolecules that are present in a sample with highly variable concentrations, or distinct biomolecules that can be found at very different levels. Finally, we qualitatively discuss the physical and chemical origin of the hysteresis signal and associate it with the polarization of thrombin molecules upon binding to the receptor at the nanowire surface.
Here we propose a platform for the detection of unlabeled human α-thrombin down to the picomolar range in a fluorescence-based aptamer assay. In this concept, thrombin is captured between two different thrombin binding aptamers, TBA1 (15mer) and TBA2 (29mer), each labeled with a specific fluorescent dye. One aptamer is attached to the surface, the second one is in solution and recognizes surface-captured thrombin. To improve the limit of detection and the comparability of measurements, we employed and compared two approaches to pattern the chip substrate−microcontact printing of organosilanes onto bare glass slides, and controlled printing of the capture aptamer TBA1 in arrays onto functionalized glass substrates using a nanoplotter device. The parallel presence of functionalized and control areas acts as an internal reference. We demonstrate that both techniques enable the detection of thrombin concentrations in a wide range from 0.02 to 200 nM with a detection limit at 20 pM. Finally, the developed method could be transferred to any substrate to probe different targets that have two distinct possible receptors without the need for direct target labeling.
The combination of nanoscaled materials and biological self-assembly is a key step for the development of novel approaches for biotechnology and bionanoelectronic devices. Here we propose a route to merge these two subsystems and report on the formation of highly concentrated aqueous solutions of silanized silicon nanowires wrapped in a lipid bilayer shell. We developed protocols and investigated the dynamics of lipid films on both planar surfaces and silicon nanowires using fluorescence recovery after photobleaching, demonstrating fully intact and fluid bilayers without the presence of a lipid molecule reservoir. Finally, the experimental setup allowed for in situ observation of spontaneous bilayer formation around the nanowire by lipid diffusion from a vesicle to the nanowire. Such aqueous solutions of lipid coated nanowires are a versatile tool for characterization purposes and are relevant for newly emerging bioinspired electronics and nanosensorics.
Detonation nanodiamonds (NDs) are a novel class of carbon-based nanomaterials, and have received a great deal of attention in biomedical applications, due to their high biocompatibility, facile surface functionalization, and commercialized synthetic fabrication. We were able to transfer the NDs from large-size agglomerate suspensions to homogenous coatings. ND suspensions have been used in various techniques to coat on commercially available substrates of pure Ti and Si. Scanning electron microscopy (SEM) imaging and nanoindentation show that the densest and strongest coating of NDs was generated when using 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide and N-hydroxysuccinimide (EDC/NHS)-mediated coupling to macroscopic silanized surfaces. In the next step, the feasibility of DNA-mediated coupling of NDs on macroscopic surfaces is discussed using fluorescent microscopy and additional particle size distribution, as well as zeta potential measurements. This work compares different ND coating strategies and describes the straightforward technique of grafting single-stranded DNA onto carboxylated NDs via thioester bridges.
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