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  1. Free, publicly-accessible full text available January 4, 2025
  2. Abstract

    Modern scanning microscopes can image materials with up to sub-atomic spatial and sub-picosecond time resolutions, but these capabilities come with large volumes of data, which can be difficult to store and analyze. We report the Fast Autonomous Scanning Toolkit (FAST) that addresses this challenge by combining a neural network, route optimization, and efficient hardware controls to enable a self-driving experiment that actively identifies and measures a sparse but representative data subset in lieu of the full dataset. FAST requires no prior information about the sample, is computationally efficient, and uses generic hardware controls with minimal experiment-specific wrapping. We test FAST in simulations and a dark-field X-ray microscopy experiment of a WSe2film. Our studies show that a FAST scan of <25% is sufficient to accurately image and analyze the sample. FAST is easy to adapt for any scanning microscope; its broad adoption will empower general multi-level studies of materials evolution with respect to time, temperature, or other parameters.

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    Free, publicly-accessible full text available September 7, 2024
  3. Free, publicly-accessible full text available July 4, 2024
  4. Lead (Pb) solubility is commonly limited by dissolution–precipitation reactions of secondary mineral phases in contaminated soils and water. In the research described here, Pb solubility and free Pb2+ ion activities were measured following the precipitation of Pb minerals from aqueous solutions containing sulfate or carbonate in a 1:5 mole ratio in the absence and presence of phosphate over the pH range 4.0–9.0. Using X-ray diffraction and Fourier-transform infrared spectroscopic analysis, we identified anglesite formed in sulfate-containing solutions at low pH. At higher pH, Pb carbonate and carbonate-sulfate minerals, hydrocerussite and leadhillite, were formed in preference to anglesite. Precipitates formed in the Pb-carbonate systems over the pH range of 6 to 9 were composed of cerussite and hydrocerussite, with the latter favored only at the highest pH investigated. The addition of phosphate into the Pb-sulfate and Pb-carbonate systems resulted in the precipitation of Pb3(PO4)2 and structurally related pyromorphite minerals and prevented Pb sulfate and carbonate mineral formation. Phosphate increased the efficiency of Pb removal from solution and decreased free Pb2+ ion activity, causing over 99.9% of Pb to be precipitated. Free Pb2+ ion activities measured using the ion-selective electrode revealed lower values than predicted from thermodynamic constants, indicating that the precipitated minerals may have lower KSP values than generally reported in thermodynamic databases. Conversely, dissolved Pb was frequently greater than predicted based on a speciation model using accepted thermodynamic constants for Pb ion-pair formation in solution. The tendency of the thermodynamic models to underestimate Pb solubility while overestimating free Pb2+ activity in these systems, at least in the higher pH range, indicates that soluble Pb ion-pair formation constants and KSP values need correction in the models. 
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  5. In this work, photoluminescence (PL), quantum efficiency and carrier dynamics are investigated in indium arsenide (InAs) nanowires (NWs) with various surface treatments, including a molecular beam epitaxy (MBE)-grown semiconductor shell passivation, sulfur-passivation, alumina (Al2O3) coating by atomic layer deposition (ALD) and polydimethylsiloxane (PDMS) spin-coating. The ALD-dielectric layer-coated InAs core-shell NWs show a maximum 13-fold increase in PL intensity. In contrast to the previous reports, this enhancement is found to be due to increased radiative rate from an enhanced Purcell factor, better thermal conductance and higher carrier injection within the NWs instead of improved surface quality. Numeric simulations confirm the experimentally observed increased radiative rate. Further improvements are suggested with even thicker capped InAs NWs. Carrier lifetime in surface-treated NWs is extended and shows long-term stability, critical for practical devices.

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  6. Catalyst-free, position-controlled indium arsenide (InAs) nanowires (NWs) of variable diameters were grown on Si (111) by selective-area epitaxy (SAE). Ultrafast pump-probe spectroscopy was conducted, from which carrier recombination mechanisms on the NW surface and interior were resolved and characterized. NWs grown using SAE demonstrated high optical quality, showing minority carrier lifetimes more than two-fold longer than that of the randomly-positioned (RP) NWs. The extracted SAE-InAs NW interior recombination lifetime was found to be as long as 7.2ns, 13X longer than previous measurements on RP-NWs; and the surface recombination velocity 4154cm·s- 1. Transmission electron microscopy revealed a high density of stacking defects within the NWs, suggesting that interior recombination lifetime can be further increased by improving NW interior crystalline quality.

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