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  1. Tangential flow interfacial self-assembly (TaFISA) is a promising scalable technique enabling uniformly aligned carbon nanotubes for high-performance semiconductor electronics. In this process, flow is utilized to induce global alignment in two-dimensional nematic carbon nanotube assemblies trapped at a liquid/liquid interface, and these assemblies are subsequently deposited on target substrates. Here, we present an observational study of experimental parameters that affect the interfacial assembly and subsequent aligned nanotube deposition. We specifically study the water contact angle (WCA) of the substrate, nanotube ink composition, and water subphase and examine their effects on liquid crystal defects, overall and local alignment, and nanotube bunching or crowding. By varying the substrate chemical functionalization, we determine that highly aligned, densely packed, individualized nanotubes deposit only at relatively small WCA between 35 and 65°. At WCA (< 10°), high nanotube bunching or crowding occurs, and the film is nonuniform, while aligned deposition ceases to occur at higher WCA (>65°). We find that the best alignment, with minimal liquid crystal defects, occurs when the polymer-wrapped nanotubes are dispersed in chloroform at a low (0.6:1) wrapper polymer to nanotube ratio. We also demonstrate that modifying the water subphase through the addition of glycerol not only improves overall alignment and reduces liquid crystal defects but also increases local nanotube bunching. These observations provide important guidance for the implementation of TaFISA and its use toward creating technologies based on aligned semiconducting carbon nanotubes. 
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    Free, publicly-accessible full text available October 10, 2024
  2. We examine if the bundling of semiconducting carbon nanotubes (CNTs) can increase the transconductance and on-state current density of field effect transistors (FETs) made from arrays of aligned, polymer-wrapped CNTs. Arrays with packing density ranging from 20 to 50 bundles  μm −1 are created via tangential flow interfacial self-assembly, and the transconductance and saturated on-state current density of FETs with either (i) strong ionic gel gates or (ii) weak 15 nm SiO 2 back gates are measured vs the degree of bundling. Both transconductance and on-state current significantly increase as median bundle height increases from 2 to 4 nm, but only when the strongly coupled ionic gel gate is used. Such devices tested at −0.6 V drain voltage achieve transconductance as high as 50 μS per bundle and 2 mS  μm −1 and on-state current as high as 1.7 mA  μm −1 . At low drain voltages, the off-current also increases with bundling, but on/off ratios of ∼10 5 are still possible if the largest (95th percentile) bundles in an array are limited to ∼5 nm in size. Radio frequency devices with strong, wraparound dielectric gates may benefit from increased device performance by using moderately bundled as opposed to individualized CNTs in arrays. 
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  3. null (Ed.)
    Selective deposition of semiconducting carbon nanotubes (s-CNTs) into densely packed, aligned arrays of individualized s-CNTs is necessary to realize their potential in semiconductor electronics. We report the combination of chemical contrast patterns, topography, and pre-alignment of s-CNTs via shear to achieve selective-area deposition of aligned arrays of s-CNTs. Alternate stripes of surfaces favorable and unfavorable to s-CNT adsorption were patterned with widths varying from 2000 nm down to 100 nm. Addition of topography to the chemical contrast patterns combined with shear enabled the selective-area deposition of arrays of quasi-aligned s-CNTs (∼14°) even in patterns that are wider than the length of individual nanotubes (>500 nm). When the width of the chemical and topographical contrast patterns is less than the length of individual nanotubes (<500 nm), confinement effects become dominant enabling the selective-area deposition of much more tightly aligned s-CNTs (∼7°). At a trench width of 100 nm, we demonstrate the lowest standard deviation in alignment degree of 7.6 ± 0.3° at a deposition shear rate of 4600 s −1 , while maintaining an individualized s-CNT density greater than 30 CNTs μm −1 . Chemical contrast alone enables selective-area deposition, but chemical contrast in addition to topography enables more effective selective-area deposition and stronger confinement effects, with the advantage of removal of nanotubes deposited in spurious areas via selective lift-off of the topographical features. These findings provide a methodology that is inherently scalable, and a means to deposit spatially selective, aligned s-CNT arrays for next-generation semiconducting devices. 
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  4. null (Ed.)