An improved method for the metallization of DNA origami is examined in this work. DNA origami, a simple and robust method for creating a wide variety of nanostructured shapes and patterns, provides an enabling template for bottom-up fabrication of next-generation nanodevices. Selective metallization of these DNA templates is needed to make nanoelectronic devices. Here, we demonstrate a metallization process that uses gold nanorod seeds followed by anisotropic plating to provide improved morphology and greater control of the final metallized width of the structure. In our approach, gold nanorods are attached to an origami template to create a seed layer. Electroless gold deposition is then used to fill the gaps between seeds in order to create continuous, conductive nanowires. Importantly, growth during electroless deposition occurs preferentially in the length direction at a rate that is approximately 4 times the growth rate in the width direction, which enables fabrication of narrow, continuous wires. The electrical properties of 49 nanowires with widths ranging from 13 to 29 nm were characterized, and resistivity values as low as 8.9 × 10 Ω·m were measured. The anisotropic metallization process presented here represents important progress toward the creation of nanoelectronic devices by molecularly directed placement of functional components onto self-assembled biological templates.
We have developed microfluidic devices with pressure-driven injection for electrophoretic analysis of amino acids, peptides, and proteins. The novelty of our approach lies in the use of an externally actuated on-chip peristaltic pump and closely spaced pneumatic valves that allow well-defined, small-volume sample plugs to be injected and separated by microchip electrophoresis. We fabricated three-layer poly(dimethylsiloxane) (PDMS) microfluidic devices. The fluidic layer had injection and separation channels, and the control layer had an externally actuated on-chip peristaltic pump and four pneumatic valves around the T-intersection to carry out sample injection. An unpatterned PDMS membrane layer was sandwiched between the fluidic and control layers as the actuated component in pumps and valves. Devices with the same peristaltic pump design but different valve spacings (100, 200, 300, and 400 μm) from the injection intersection were fabricated using soft lithographic techniques. Devices were characterized through fluorescent imaging of captured plugs of a fluorescein-labeled amino acid mixture, and through microchip electrophoresis separations. A suitable combination of peak height, separation efficiency, and analysis time was obtained with a peristaltic pump actuation rate of 50 ms, an injection time of 30 s, and a 200 μm valve spacing. We demonstrated the injection of samples in different solutions and were able to achieve a 2.4-fold improvement in peak height and a 2.8-fold increase in separation efficiency though sample stacking. A comparison of pressure-driven injection and electrokinetic injection with the same injection time and separation voltage showed a 3.9-fold increase in peak height in pressure-based injection with comparable separation efficiency. Finally, the microchip systems were used to separate biomarkers implicated in pre-term birth. Although these devices have initially been demonstrated as a stand-alone microfluidic separation tool, they have strong potential to be integrated within more complex systems.
This work examines the anisotropic electroless plating of DNA-functionalized gold nanorods attached to a DNA origami template to fabricate continuous metal structures of rectanglar, square, and T shapes. DNA origami, a versatile method for assembling a variety of 2- and 3-D nanostructures, is utilized to construct the DNA breadboard template used for this study. Staple strands on selective sites of the breadboard template are extended with an additional nucleotide sequence for the attachment of DNA-functionalized gold nanorods to the template via base pairing. The nanorod-seeded DNA templates are then introduced into an electroless gold plating solution to determine the extent to which the anisotropic growth of the nanorods is able to fill the gaps between seeds to create continuous structures. Our results show that the DNA-functionalized nanorods grow anisotropically during plating at a rate that is approximately 4 times faster in the length direction than in the width direction to effectively fill gaps of up to 11-13 nm in length. The feasibility of using this directional growth at specific sites to enable the fabrication of continuous metal nanostructures with diameters as thin as 10 nm is demonstrated and represents important progress toward the creation of devices and systems based on self-assembled biological templates.
DNA origami is a valuable technique in arranging nanoparticles into various geometries with a $100 nm footprint, high resolution, and experimental simplicity. Aligned nanoparticles, in addition to being used for photonics, can also be utilized to create thin metal wires with intricate and asymmetric junctions.Many factors affect the yield and density of nanoparticles attached to DNA origami structures, including the length and number of attachment sequences, the reaction ratio of nanoparticles to DNA origami, the hybridization temperature, and age of the solutions. This work investigates the alignment of closely packed 5 nm gold nanoparticles along thin DNA origami structures. Several reaction conditions, including hybridization time, magnesium ion concentration, ratio of nanoparticles to DNA origami, and age of the nanoparticle solution, were explored to optimize nanoparticle attachment density and spacing. Optimum ranges of conditions were identified, yielding new insights into high-density nanoparticle attachment to thin DNA origami structures, with potential for application in nanowire and nanoelectronics construction.
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