Glymphatic-assisted perivascular brain delivery of intrathecal small gold nanoparticles.

Nanoparticles are ultrafine particulate matter having considerable potential for treatment of central nervous system (CNS) disorders. Despite their tiny size, the blood-brain barrier (BBB) restricts their access to the CNS. Their direct cerebrospinal fluid (CSF) administration bypasses the BBB endothelium, but still fails to give adequate brain uptake. We present a novel approach for efficient CNS delivery of 111In-radiolabelled gold nanoparticles (AuNPs; 10-15 nm) via intra-cisterna magna administration, with tracking by SPECT imaging. To accelerate CSF brain influx, we administered AuNPs intracisternally in conjunction with systemic hypertonic saline, which dramatically increased the parenchymal AuNP uptake, especially in deep brain regions. AuNPs entered the CNS along periarterial spaces as visualized by MRI of gadolinium-labelled AuNPs and were cleared from brain within 24 h and excreted through the kidneys. Thus, the glymphatic-assisted perivascular network augment by systemic hypertonic saline is a pathway for highly efficient brain-wide distribution of small AuNPs.

Superconductivity and Parity Preservation in As-Grown In Islands on InAs Nanowires.

We report in situ synthesis of crystalline indium islands on InAs nanowires grown by molecular beam epitaxy. Structural analysis by transmission electron microscopy showed that In crystals grew in a tetragonal body-centered crystal structure within two families of orientations relative to wurtzite InAs. The crystalline islands had lengths < 500 nm and low-energy surfaces, suggesting that growth was driven mainly by surface energy minimization. Electrical transport through In/InAs devices exhibited Cooper pair charging, evidencing charge parity preservation and a pristine In/InAs interface, with an induced superconducting gap ∼ 0.45 meV. Cooper pair charging persisted to temperatures > 1.2 K and magnetic fields ∼ 0.7 T, demonstrating that In/InAs hybrids belong to an expanding class of semiconductor/superconductor hybrids operating over a wider parameter space than state-of-the-art Al-based hybrids. Engineering crystal morphology while isolating single islands using shadow epitaxy provides an interesting alternative to previous semiconductor/superconductor hybrid morphologies and device geometries.

Highly Transparent Gatable Superconducting Shadow Junctions.

Gate-tunable junctions are key elements in quantum devices based on hybrid semiconductor-superconductor materials. They serve multiple purposes ranging from tunnel spectroscopy probes to voltage-controlled qubit operations in gatemon and topological qubits. Common to all is that junction transparency plays a critical role. In this study, we grow single-crystalline InAs, InSb, and InAs1-xSbx semiconductor nanowires with epitaxial Al, Sn, and Pb superconductors and in situ shadowed junctions in a single-step molecular beam epitaxy process. We investigate correlations between fabrication parameters, junction morphologies, and electronic transport properties of the junctions and show that the examined in situ shadowed junctions are of significantly higher quality than the etched junctions. By varying the edge sharpness of the shadow junctions, we show that the sharpest edges yield the highest junction transparency for all three examined semiconductors. Further, critical supercurrent measurements reveal an extraordinarily high ICRN, close to the KO-2 limit. This study demonstrates a promising engineering path toward reliable gate-tunable superconducting qubits.

Shadow Epitaxy for In Situ Growth of Generic Semiconductor/Superconductor Hybrids.

Uniform, defect-free crystal interfaces and surfaces are crucial ingredients for realizing high-performance nanoscale devices. A pertinent example is that advances in gate-tunable and topological superconductivity using semiconductor/superconductor electronic devices are currently built on the hard proximity-induced superconducting gap obtained from epitaxial indium arsenide/aluminum heterostructures. Fabrication of devices requires selective etch processes; these exist only for InAs/Al hybrids, precluding the use of other, potentially superior material combinations. This work introduces a crystal growth platform-based on 3D structuring of growth substrates-which enables synthesis of semiconductor nanowire hybrids with in situ patterned superconductor shells. The platform eliminates the need for etching, thereby enabling full freedom in the choice of hybrid constituents. All of the most frequently used superconducting hybrid device architectures are realized and characterized. These devices exhibit increased yield and electrostatic stability compared to etched devices, and evidence of ballistic superconductivity is observed. In addition to aluminum, hybrid structures based on tantalum, niobium, and vanadium are presented.

Evolution of intermetallic GaPd2/SiO2 catalyst and optimization for methanol synthesis at ambient pressure.

The CO2 hydrogenation to methanol is efficiently catalyzed at ambient pressure by nanodispersed intermetallic GaPd2/SiO2 catalysts prepared by incipient wetness impregnation. Here we optimize the catalyst in terms of metal content and reduction temperature in relation to its catalytic activity. We find that the intrinsic activity is higher for the GaPd2/SiO2 catalyst with a metal loading of 13 wt.% compared to catalysts with 23 wt.% and 7 wt.%, indicating that there is an optimum particle size for the reaction of around 8 nm. The highest catalytic activity is measured on catalysts reduced at 550°C. To unravel the formation of the active phase, we studied calcined GaPd2/SiO2 catalysts with 23 wt.% and 13 wt.% using a combination of in situ techniques: X-ray diffraction (XRD), X-ray absorption near edge fine structure (XANES) and extended X-ray absorption fine structure (EXAFS). We find that the catalyst with higher metal content reduces to metallic Pd in a mixture of H2/Ar at room temperature, while the catalyst with lower metal content retains a mixture of PdO and Pd up to 140°C. Both catalysts form the GaPd2 phase above 300°C, albeit the fraction of crystalline intermediate Pd nanoparticles of the catalyst with higher metal loading reduces at higher temperature. In the final state, the catalyst with higher metal loading contains a fraction of unalloyed metallic Pd, while the catalyst with lower metal loading is phase pure. We discuss the alloying mechanism leading to the catalyst active phase formation selecting three temperatures: 25°C, 320°C and 550°C.

Superconducting vanadium/indium-arsenide hybrid nanowires.

We report MBE synthesis of InAs/vanadium hybrid nanowires. The vanadium was deposited without breaking ultra-high vacuum after InAs nanowire growth, minimizing any effect of oxidation and contamination at the interface between the two materials. We investigated four different substrate temperatures during vanadium deposition, ranging from -150 °C to 250 °C. The structural relation between vanadium and InAs depended on the deposition temperature. The three lower temperature depositions gave vanadium shells with a polycrystalline, granular morphology and the highest temperature resulted in vanadium reacting with the InAs nanowire. We fabricated electronic devices from the hybrid nanowires and obtained a high out-of-plane critical magnetic field, exceeding the bulk value for vanadium. However, size effects arising from the nanoscale grains resulted in the absence of a well-defined critical temperature, as well as device-to-device variation in the resistivity versus temperature dependence during the transition to the superconducting state.

GaP nanowire betavoltaic device.

A betavoltaic device is reported that directly converts beta energy from a 63Ni radioisotope into electrical energy by impact ionization in a GaP nanowire array. The GaP nanowires are grown in a periodic array by molecular beam epitaxy on silicon using the self-assisted vapor-liquid-solid method. By growing GaP nanowires with large packing fraction and length on the order of the maximum beta range, the nanowires can efficiently capture the betas with high energy conversion efficiency while using inexpensive Si substrates. Monte Carlo simulations predict a betavoltaic efficiency in agreement with experimental results. The nanowire betavoltaic device can be used as a power source for nano-/micro-systems such as mobile electronic devices, implantable medical devices, and wireless sensor networks.

Stable amorphous georgeite as a precursor to a high-activity catalyst.

Copper and zinc form an important group of hydroxycarbonate minerals that include zincian malachite, aurichalcite, rosasite and the exceptionally rare and unstable--and hence little known and largely ignored--georgeite. The first three of these minerals are widely used as catalyst precursors for the industrially important methanol-synthesis and low-temperature water-gas shift (LTS) reactions, with the choice of precursor phase strongly influencing the activity of the final catalyst. The preferred phase is usually zincian malachite. This is prepared by a co-precipitation method that involves the transient formation of georgeite; with few exceptions it uses sodium carbonate as the carbonate source, but this also introduces sodium ions--a potential catalyst poison. Here we show that supercritical antisolvent (SAS) precipitation using carbon dioxide (refs 13, 14), a process that exploits the high diffusion rates and solvation power of supercritical carbon dioxide to rapidly expand and supersaturate solutions, can be used to prepare copper/zinc hydroxycarbonate precursors with low sodium content. These include stable georgeite, which we find to be a precursor to highly active methanol-synthesis and superior LTS catalysts. Our findings highlight the value of advanced synthesis methods in accessing unusual mineral phases, and show that there is room for exploring improvements to established industrial catalysts.