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result(s) for
"Aloni, Shaul"
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Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage
2016
Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H
2
per litre in the total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. These multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments.
Hydrogen fuel cell electric vehicles are poised to transform the automotive industry, but the lack of safe, high density solid state hydrogen storage solutions is stifling progress. Here, the authors develop a graphene oxide/magnesium nanocomposite which appears to overcome many of the existing challenges.
Journal Article
Complete composition tunability of InGaN nanowires using a combinatorial approach
by
Aloni, Shaul
,
Ulrich, Philipp
,
Kuykendall, Tevye
in
Biomaterials
,
Chemistry and Materials Science
,
Combinatorics
2007
The III nitrides have been intensely studied in recent years because of their huge potential for everything from high-efficiency solid-state lighting and photovoltaics to high-power and temperature electronics
1
,
2
,
3
. In particular, the InGaN ternary alloy is of interest for solid-state lighting and photovoltaics because of the ability to tune the direct bandgap of this material from the near-ultraviolet to the near-infrared region. In an effort to synthesize InGaN nitride, researchers have tried many growth techniques
4
,
5
,
6
,
7
,
8
,
9
,
10
,
11
,
12
,
13
. Nonetheless, there remains considerable difficulty in making high-quality InGaN films and/or freestanding nanowires with tunability across the entire range of compositions. Here we report for the first time the growth of single-crystalline In
x
Ga
1−
x
N nanowires across the entire compositional range from
x
=0 to 1; the nanowires were synthesized by low-temperature halide chemical vapour deposition
9
and were shown to have tunable emission from the near-ultraviolet to the near-infrared region. We propose that the exceptional composition tunability is due to the low process temperature and the ability of the nanowire morphology to accommodate strain-relaxed growth
14
, which suppresses the tendency toward phase separation that plagues the thin-film community.
Journal Article
Nanoscale temperature mapping in operating microelectronic devices
2015
Modern microelectronic devices have nanoscale features that dissipate power nonuniformly, but fundamental physical limits frustrate efforts to detect the resulting temperature gradients. Contact thermometers distrub the temperature of a small system, while radiation thermometers struggle to beat the diffraction limit. Exploiting the same physics as Fahrenheit's glass-bulb thermometer, we mapped the thermal expansion of Joule-heated, 80-nanometer-thick aluminum wires by precisely measuring changes in density. With a scanning transmission electron microscope and electron energy loss spectroscopy, we quantified the local density via the energy of aluminum's bulk plasmon. Rescaling density to temperature yields maps with a statistical precision of 3 kelvin/hertz–1/2, an accuracy of 10%, and nanometer-scale resolution. Many common metals and semiconductors have sufficiently sharp plasmon resonances to serve as their own thermometers.
Journal Article
Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides
2019
Chalcogen vacancies are generally considered to be the most common point defects in transition metal dichalcogenide (TMD) semiconductors because of their low formation energy in vacuum and their frequent observation in transmission electron microscopy studies. Consequently, unexpected optical, transport, and catalytic properties in 2D-TMDs have been attributed to in-gap states associated with chalcogen vacancies, even in the absence of direct experimental evidence. Here, we combine low-temperature non-contact atomic force microscopy, scanning tunneling microscopy and spectroscopy, and state-of-the-art ab initio density functional theory and GW calculations to determine both the atomic structure and electronic properties of an abundant chalcogen-site point defect common to MoSe
2
and WS
2
monolayers grown by molecular beam epitaxy and chemical vapor deposition, respectively. Surprisingly, we observe no in-gap states. Our results strongly suggest that the common chalcogen defects in the described 2D-TMD semiconductors, measured in vacuum environment after gentle annealing, are oxygen substitutional defects, rather than vacancies.
The nature of defects in transition metal dichalcogenide semiconductors is still under debate. Here, the authors determine the atomic structure and electronic properties of chalcogen-site point defects common to monolayer MoSe
2
and WS
2
, and find that these are substitutional defects, where a chalcogen atom is substituted by an oxygen atom, rather than vacancies.
Journal Article
Fabrication of Subnanometer-Precision Nanopores in Hexagonal Boron Nitride
2017
We demonstrate the fabrication of individual nanopores in hexagonal boron nitride (h-BN) with atomically precise control of the pore shape and size. Previous methods of pore production in other 2D materials typically create pores with irregular geometry and imprecise diameters. In contrast, other studies have shown that with careful control of electron irradiation, defects in h-BN grow with pristine zig-zag edges at quantized triangular sizes, but they have failed to demonstrate production and control of isolated defects. In this work, we combine these techniques to yield a method in which we can create individual size-quantized triangular nanopores through an h-BN sheet. The pores are created using the electron beam of a conventional transmission electron microscope; which can strip away multiple layers of h-BN exposing single-layer regions, introduce single vacancies, and preferentially grow vacancies only in the single-layer region. We further demonstrate how the geometry of these pores can be altered beyond triangular by changing beam conditions. Precisely size- and geometry-tuned nanopores could find application in molecular sensing, DNA sequencing, water desalination, and molecular separation.
Journal Article
Visualizing nanoscale excitonic relaxation properties of disordered edges and grain boundaries in monolayer molybdenum disulfide
by
Weber-Bargioni, Alexander
,
Fan, Wen
,
Cabrini, Stefano
in
140/125
,
639/301/119/1000
,
639/624/400
2015
Two-dimensional monolayer transition metal dichalcogenide semiconductors are ideal building blocks for atomically thin, flexible optoelectronic and catalytic devices. Although challenging for two-dimensional systems, sub-diffraction optical microscopy provides a nanoscale material understanding that is vital for optimizing their optoelectronic properties. Here we use the ‘Campanile’ nano-optical probe to spectroscopically image exciton recombination within monolayer MoS
2
with sub-wavelength resolution (60 nm), at the length scale relevant to many critical optoelectronic processes. Synthetic monolayer MoS
2
is found to be composed of two distinct optoelectronic regions: an interior, locally ordered but mesoscopically heterogeneous two-dimensional quantum well and an unexpected ∼300-nm wide, energetically disordered edge region. Further, grain boundaries are imaged with sufficient resolution to quantify local exciton-quenching phenomena, and complimentary nano-Auger microscopy reveals that the optically defective grain boundary and edge regions are sulfur deficient. The nanoscale structure–property relationships established here are critical for the interpretation of edge- and boundary-related phenomena and the development of next-generation two-dimensional optoelectronic devices.
Understanding the dynamics of light-induced carriers is vital for employing two-dimensional materials in optoelectronic applications. Here, the authors use a sub diffraction-limit optical technique to reveal the excitonic properties of monolayer molybdenum disulfide at the nanoscale.
Journal Article
Three-dimensional periodic supramolecular organic framework ion sponge in water and microcrystals
2014
Self-assembly has emerged as a powerful approach to generating complex supramolecular architectures. Despite there being many crystalline frameworks reported in the solid state, the construction of highly soluble periodic supramolecular networks in a three-dimensional space is still a challenge. Here we demonstrate that the encapsulation motif, which involves the dimerization of two aromatic units within cucurbit[8]uril, can be used to direct the co-assembly of a tetratopic molecular block and cucurbit[8]uril into a periodic three-dimensional supramolecular organic framework in water. The periodicity of the supramolecular organic framework is supported by solution-phase small-angle X-ray-scattering and diffraction experiments. Upon evaporating the solvent, the periodicity of the framework is maintained in porous microcrystals. As a supramolecular ‘ion sponge’, the framework can absorb different kinds of anionic guests, including drugs, in both water and microcrystals, and drugs absorbed in microcrystals can be released to water with selectivity.
The construction of soluble periodic supramolecular three-dimensional networks is challenging. Here, the authors use an encapsulated dimerization strategy to direct the assembly of a periodic three-dimensional supramolecular organic framework and evaluate its absorption properties.
Journal Article
Bright sub-20-nm cathodoluminescent nanoprobes for electron microscopy
by
Prigozhin, Maxim B
,
Macfarlane, Roger M
,
Tian Bining
in
Biomolecules
,
Cathodoluminescence
,
Electron imaging
2019
Electron microscopy has been instrumental in our understanding of complex biological systems. Although electron microscopy reveals cellular morphology with nanoscale resolution, it does not provide information on the location of different types of proteins. An electron-microscopy-based bioimaging technology capable of localizing individual proteins and resolving protein–protein interactions with respect to cellular ultrastructure would provide important insights into the molecular biology of a cell. Here, we synthesize small lanthanide-doped nanoparticles and measure the absolute photon emission rate of individual nanoparticles resulting from a given electron excitation flux (cathodoluminescence). Our results suggest that the optimization of nanoparticle composition, synthesis protocols and electron imaging conditions can lead to sub-20-nm nanolabels that would enable high signal-to-noise localization of individual biomolecules within a cellular context. In ensemble measurements, these labels exhibit narrow spectra of nine distinct colours, so the imaging of biomolecules in a multicolour electron microscopy modality may be possible.Lanthanide-doped nanoparticles could be used as labels for the imaging of biomolecules, potentially leading to a multicolour modality in electron microscopy.
Journal Article
Non-blinking and photostable upconverted luminescence from single lanthanide-doped nanocrystals
2009
The development of probes for single-molecule imaging has dramatically facilitated the study of individual molecules in cells and other complex environments. Single-molecule probes ideally exhibit good brightness, uninterrupted emission, resistance to photobleaching, and minimal spectral overlap with cellular autofluorescence. However, most single-molecule probes are imperfect in several of these aspects, and none have been shown to possess all of these characteristics. Here we show that individual lanthanide-doped upconverting nanoparticles (UCNPs)--specifically, hexagonal phase NaYF₄ (β-NaYF₄) nanocrystals with multiple Yb³⁺ and Er³⁺ dopants--emit bright anti-Stokes visible upconverted luminescence with exceptional photostability when excited by a 980-nm continuous wave laser. Individual UCNPs exhibit no on/off emission behavior, or \"blinking,\" down to the millisecond timescale, and no loss of intensity following an hour of continuous excitation. Amphiphilic polymer coatings permit the transfer of hydrophobic UCNPs into water, resulting in individual water-soluble nanoparticles with undiminished photophysical characteristics. These UCNPs are endocytosed by cells and show strong upconverted luminescence, with no measurable anti-Stokes background autofluorescence, suggesting that UCNPs are ideally suited for single-molecule imaging experiments.
Journal Article
Observation of interface piezoelectricity in superconducting devices on silicon
by
Zhou, Haoxin
,
Aloni, Shaul
,
Godeneli, Kadircan
in
639/766/1130/1064
,
639/766/483/2802
,
Aluminum
2025
The development of superconducting quantum processors relies on understanding and mitigating decoherence in superconducting qubits. Piezoelectric coupling contributes to decoherence by mediating energy exchange between microwave photons and acoustic phonons. Although bulk centrosymmetric materials like silicon and sapphire are non-piezoelectric and commonly used as qubit substrates, the lack of centrosymmetry at interfaces may induce piezoelectric losses. This effect was predicted decades ago but never experimentally observed in superconducting devices. Here, we report interface piezoelectricity at aluminum-silicon junctions and demonstrate it as a significant loss channel in superconducting devices. Using aluminum interdigital transducers on silicon, we observe piezoelectric transduction from room to millikelvin temperatures, with an effective electromechanical coupling factor
K
2
≈ (3 ± 0.4) × 10
−5
%, comparable to weakly piezoelectric substrates. Modeling shows this mechanism limits qubit quality factors to
Q
~ 10
4
− 10
8
, depending on surface participation and mode matching. These findings reveal interface piezoelectricity as a major dissipation channel and highlight the need for heterostructure and phononic engineering in next-generation superconducting qubits.
Superconducting qubits are sensitive to multiple noise sources that compromise their coherence. Here the authors report a piezoelectric effect in aluminum-silicon junctions, revealing a previously unexplored mechanism that may limit superconducting quantum processor performance.
Journal Article