Publications

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We study nanoporous-carbon (NPC) grown via pulsed laser deposition (PLD) as a sorbent coating on 96.5-MHz surface-acousticwave (SAW) devices to detect trihalomethanes (THMs), regulated byproducts from the chemical treatment of drinking water. Using both insertion-loss and isothermal-response measurements from known quantities of chloroform, the highest vapor pressure THM, we optimize the NPC mass-density at 1.05 ± 0.08 g/cm³ by controlling the background argon pressure during PLD. Precise THM quantities in a chlorobenzene solvent are directly injected into a separation column and detected as the phase-angle shift of the SAW device output compared to the drive signal. Using optimized NPC-coated SAWs, we study the chloroform response as a function of operating temperatures ranging from 10.50°C. Finally, we demonstrate individual responses from complex mixtures of all four THMs, with masses ranging from 10.2000 ng, after gas chromatography separation. Estimates for each THM detection limit using a simple peak-height response evaluation are 4.4 ng for chloroform and 1 ng for bromoform; using an integrated-peak area response analysis improves the detection limits to 0.73 ng for chloroform and 0.003 ng bromoform.

Vertically aligned, untangled planarized arrays of multiwall carbon nanotubes (MWNTs) with Ohmic back contacts were grown in nanopore templates on arbitrary substrates. The templates were prepared by sputter depositing Nd-doped Al films onto W-coated substrates, followed by anodization to form an aluminum oxide nanopore array. The W underlayer helps eliminate the aluminum oxide barrier that typically occurs at the nanopore bottoms by instead forming a thin WO3 layer. The WO3 can be selectively etched to enable electrodeposition of Co catalysts with control over the Co site density. This led to control of the site density of MWNTs grown by thermal chemical vapor deposition, with W also serving as a back electrical contact. Ohmic contact to MWNTs was confirmed, even following ultrasonic cutting of the entire array to a uniform height.

Using galvanostatic pulse deposition, we studied the factors influencing the quality of electroformed Bi1-xSbxnanowires with respect to composition, crystallinity, and preferred orientation for high thermoelectric performance. Two nonaqueous baths with different Sb salts were investigated. The Sb salts used played a major role in both crystalline quality and preferred orientations. Nanowire arrays electroformed using an SbI3-based chemistry were polycrystalline with no preferred orientation, whereas arrays electroformed from an SbCl3-based chemistry were strongly crystallographically textured with the desired trigonal orientation for optimal thermoelectric performance. From the SbCl3 bath, the electroformed nanowire arrays were optimized to have nanocompositional uniformity, with a nearly constant composition along the nanowire length. Nanowires harvested from the center of the array had an average composition of Bi0.75Sb0.25. However, the nanowire compositions were slightly enriched in Sb in a small region near the edges of the array, with the composition approaching Bi0.700.30.

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We present the results of a three year LDRD project that focused on understanding the impact of defects on the electrical, optical and thermal properties of GaN-based nanowires (NWs). We describe the development and application of a host of experimental techniques to quantify and understand the physics of defects and thermal transport in GaN NWs. We also present the development of analytical models and computational studies of thermal conductivity in GaN NWs. Finally, we present an atomistic model for GaN NW electrical breakdown supported with experimental evidence. GaN-based nanowires are attractive for applications requiring compact, high-current density devices such as ultraviolet laser arrays. Understanding GaN nanowire failure at high-current density is crucial to developing nanowire (NW) devices. Nanowire device failure is likely more complex than thin film due to the prominence of surface effects and enhanced interaction among point defects. Understanding the impact of surfaces and point defects on nanowire thermal and electrical transport is the first step toward rational control and mitigation of device failure mechanisms. However, investigating defects in GaN NWs is extremely challenging because conventional defect spectroscopy techniques are unsuitable for wide-bandgap nanostructures. To understand NW breakdown, the influence of pre-existing and emergent defects during high current stress on NW properties will be investigated. Acute sensitivity of NW thermal conductivity to point-defect density is expected due to the lack of threading dislocation (TD) gettering sites, and enhanced phonon-surface scattering further inhibits thermal transport. Excess defect creation during Joule heating could further degrade thermal conductivity, producing a viscous cycle culminating in catastrophic breakdown. To investigate these issues, a unique combination of electron microscopy, scanning luminescence and photoconductivity implemented at the nanoscale will be used in concert with sophisticated molecular-dynamics calculations of surface and defect-mediated NW thermal transport. This proposal seeks to elucidate long standing material science questions for GaN while addressing issues critical to realizing reliable GaN NW devices.

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Nanoporous carbon (NPC) is a purely graphitic material with highly controlled densities ranging from less than 0.1 to 2.0 g/cm3, grown via pulsed-laser deposition. Decreasing the density of NPC increases the interplanar spacing between graphene-sheet fragments. This ability to tune the interplanar spacing makes NPC an ideal model system to study the behavior of carbon electrodes in electrochemical capacitors and batteries. We examine the capacitance of NPC films in alkaline and acidic electrolytes, and measure specific capacitances as high as 242 F/g.

Nanoporous carbon (NPC) is a purely graphitic material with highly controlled densities ranging from less than 0.1 to 2.0 g/cm3, grown via pulsed-laser deposition. Decreasing the density of NPC increases the interplanar spacing between graphene-sheet fragments. This ability to tune the interplanar spacing makes NPC an ideal model system to study the behavior of carbon electrodes in electrochemical capacitors and batteries. We examine the capacitance of NPC films in alkaline and acidic electrolytes, and measure specific capacitances as high as 242 F/g.