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At least 433 records · Page 24

Selected Area Manipulation of MoS 2 via Focused Electron Beam-Induced Etching for Nanoscale Device Editing

Here we demonstrate direct-write patterning of single and multilayer MoS 2 via a focused electron beam-induced etching (FEBIE) process mediated with the XeF 2 precursor. MoS 2 etching is performed at various currents, areal doses, on different substrates, and characterized using scanning electron and atomic force microscopies as well as Raman and photoluminescence spectroscopies. Scanning transmission electron microscopy reveals a sub-40 nm etching resolution and the progression of point defects and lateral etching of the consequent unsaturated bonds. The results confirm that the electron beam-induced etching process is minimally invasive to the underlying material in comparison to ion beam techniques, which damage the subsurface material. Single-layer MoS 2 field-effect transistors are fabricated, and device characteristics are compared for channels that are edited via the selected area etching process. The source–drain current at constant gate and source–drain voltage scale linearly with the edited channel width. Moreover, the mobility of the narrowest channel width decreases, suggesting that backscattered and secondary electrons collaterally affect the periphery of the removed area. Focused electron beam doses on single-layer transistors below the etching threshold were also explored as a means to modify/thin the channel layer. The FEBIE exposures showed demonstrative effects via the transistor transfer characteristics, photoluminescence spectroscopy, and Raman spectroscopy. While strategies to minimize backscattered and secondary electron interactions outside of the scanned regions require further investigation, here, we show that FEBIE is a viable approach for selective nanoscale editing of MoS 2 devices.

36 MATERIALS SCIENCE↗

Moiré Patterns in Pt Overlayers on Gold: A Graph Neural Network Interatomic Potential Study

Overlayer structures in bimetallic catalysts are relevant to a variety of catalytic reactions, particularly in electrocatalysis for fuel cell applications. Previous computational studies largely consider these overlayer structures to be those of a pseudomorphic overlayer, where there is a 1:1 atomic ratio between the overlayer and the support metal. Our previous work based on density functional theory (DFT) has shown that there exist nonstoichiometric overlayer structures that are more stable than the stoichiometric ones. Here, in this work, we developed a graph neural network interatomic potential (GNN-IP) to analyze structures formed in Pt overlayers on Au(111). The GNN-IP was used to explore properties of nonstoichiometric overlayers at length scales that are prohibitively expensive to pursue with planewave DFT calculations. In particular, we examined large Pt islands on top of a 48 × 48 Au(111) unit cell to explore the influence of the rotational angle (α) between the Pt overlayer and support Au(111) on both the stability of and the preferred atomic density in the overlayer. Island structures with smaller rotational angles between the Pt overlayer and Au(111) tend to be more stable. Further, smaller rotational angles tend to result in lower atomic density in the Pt overlayer.

chemical structure↗

Testing strong-field QED with the avalanche precursor

A two-beam high-power laser facility is essential for the study of one of the most captivating phenomena predicted by strong-field quantum electrodynamics (QED) and yet unobserved experimentally: the avalanche-type cascade. In such a cascade, the energy of intense laser light can be efficiently transformed into high-energy radiation and electron–positron pairs. The future 50-petawatt-scale laser facility NSF OPAL will provide unique opportunities for studying such strong-field QED effects, as it is designed to deliver two ultra-intense, tightly focused laser pulses onto the interaction point. In this work, we investigate the potential of such a facility for studying elementary particle and plasma dynamics deeply in the quantum radiation-dominated (RD) regime, and the generation of QED avalanches. With three-dimensional particle-in-cell simulations, we demonstrate that QED avalanche precursors can be reliably triggered under realistic laser parameters and layout (namely, focusing f/2, tilted optical axes, and non-ideal co-pointing) with the anticipated capabilities of NSF OPAL. We demonstrate that seed electrons can be efficiently injected into the laser focus by using targets of three types: a gas of heavy atoms, an overcritical plasma, and a thin foil. A strong positron and high-energy photon signal is generated in all cases. The cascade properties can be identified from the final particle distributions, which have a clear directional pattern. At increasing laser field intensity, such distributions provide signatures of the transition, first, to the RD interaction regime, and then to a QED avalanche. Our findings can also be used for designing related future experiments.

Lasers↗

Energy calibration of germanium detectors for the Majorana Demonstrator

The Majorana Demonstrator was a search for neutrinoless double-beta decay (0νββ) in the 76 Ge isotope. It was staged at the 4850-foot level of the Sanford Underground Research Facility (SURF) in Lead, SD. The experiment consisted of 58 germanium detectors housed in a low background shield and was calibrated once per week by deploying a 228 Th line source for 1 to 2 hours. The energy scale calibration determination for the detector array was automated using custom analysis tools. We describe the offline procedure for calibration of the Demonstrator germanium detectors, including the simultaneous fitting of multiple spectral peaks, estimation of energy scale uncertainties, and the automation of the calibration procedure.

47 OTHER INSTRUMENTATION↗

Fleetite, Cu 2 RhIrSb 2 , a New Species of Platinum-Group Mineral from the Miass Placer Zone, Southern Urals, Russia

Fleetite, Cu 2 RhIrSb 2 , a new species of platinum-group mineral (PGM), was discovered intergrown with an Os–Ir–Ru alloy in the Miass Placer Zone (Au–PGE), southern Urals, Russia. A single grain 50 μm across was found. Osmium, ruthenium, and iridium are the main associated minerals; also present are Pt–Fe alloys, laurite, Sb-rich irarsite, Rh-rich tolovkite, kashinite, anduoite, ferronickelplatinum, heazlewoodite, PGE-bearing pentlandite and digenite, as well as micrometric inclusions of forsterite (Fo 93.7 ), chromite–magnesiochromite, and Mg-rich edenite. In reflected light, fleetite is light gray; it is opaque, isotropic, non-pleochroic, and non-bireflectant. We report reflectance values measured in air. A mean of seven point-analyses (wavelength-dispersive spectrometry) gave Cu 13.93, Ni 8.60, Fe 0.10, Ir 28.07, Rh 7.91, Ru 1.96, Sb 39.28, total 99.85 wt.%, corresponding to (Cu 1.41 Ni 0.58 Fe 0.01 ) Σ2.00 (Rh 0.49 Ni 0.36 Ru 0.12 ) Σ0.97 Ir 0.95 Sb 2.08 on the basis of six atoms per formula unit, taking into account the structural results. The calculated density is 10.83 g/cm 3 . Single-crystal X-ray studies show that fleetite is cubic, space group Fdm (#227), a = 11.6682(8) Å, V = 1588.59(19) Å 3 , and Z = 16. A least-squares refinement of X-ray powder-diffraction data gave a = 11.6575(5) Å and V = 1584.22(19) Å 3 . The strongest five reflections in the powder pattern [d in Å(I)(hkl)] are: 6.70(75)(111), 4.13(100)(220), 3.52(30)(311), 2.380(50)(422), 2.064(40)(440). Results of synchrotron micro-Laue diffraction experiments are consistent [a = 11.66(2) Å]. The crystal structure of fleetite was solved and refined to R = 0.0340 based upon 153 reflections with F o > 4σ(F o ). It is isotypic with Pd 11 Bi 2 Se 2 and best described as intermetallic, with all metal atoms in 12-fold coordination. Fleetite and other late exotic phases were formed by reaction of the associated alloy phases with a fluid phase enriched in Sb, As, and S in circulation in the cooling ophiolite source-rock. The mineral is named after Michael E. Fleet (1938–2017) in recognition of his significant contributions to the Earth Sciences.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

X-ray powder diffraction study of poly/carbon monofluoride/, CF/1.12/

Data from X-ray diffraction studies of the poly(carbon monofluoride) with empirical formula CF(1.09-1.15) are reported, and possible intercalation arrangements for the substance are discussed. The data do not conform to true hexagonal symmetry, indicating that the carbon atoms are not coplanar. Each bond angle of carbon is 118.8 deg, and the carbon-carbon distance is 1.47 A. The interlayer distance is 5.76 A. A total absence of (hkl) reflections in the X-ray pattern shows that the separate CF layers are not regularly arranged with respect to one another.

Mahajan, V. K.↗

Scanning transmission election microscopy observations of twisted epitaxial gold nanodiscs in twisted molybdenum disulfide bilayers

Atomic scale, scanning transmission electron microscopy (STEM) analysis of the moiré structures in twisted epitaxial gold nanodiscs encapsulated in twisted bilayer molybdenum disulfide is presented. High angle annular dark field STEM imaging reveals that the period of the moiré patterns between gold and molybdenum disulfide varies with different twist angles of the bilayer molybdenum disulfide, ranging from 1.80 nm (epitaxial alignment of gold) to 1.53 nm (twisted epitaxial alignment of gold). Additionally, bright field STEM imaging reveals a faint, larger "moiré of moiré" structure in cases where the bilayer molybdenum disulfide twist angle is small (~6°), arising from the overlapping three-layers, which is not visible in conventional transmission electron microscopy images. In conclusion, our experiments indicate that scanning transmission electron microscopy as a suitable tool for moiré analysis of twisted multilayer planar heterostructures, complementary to information provided by conventional transmission electron microscopy and diffraction.

Au↗

The role of chalcogen vacancies for atomic defect emission in MoS 2

For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Here, we correlate generation, optical spectroscopy, atomic resolution imaging, and ab initio theory of chalcogen vacancies in monolayer MoS 2 . Chalcogen vacancies are selectively generated by in-vacuo annealing, but also focused ion beam exposure. The defect generation rate, atomic imaging and the optical signatures support this claim. We discriminate the narrow linewidth photoluminescence signatures of vacancies, resulting predominantly from localized defect orbitals, from broad luminescence features in the same spectral range, resulting from adsorbates. Vacancies can be patterned with a precision below 10 nm by ion beams, show single photon emission, and open the possibility for advanced defect engineering of 2D semiconductors at the ultimate scale.

36 MATERIALS SCIENCE↗

Particle–hole asymmetric superconducting coherence peaks in overdoped cuprates

As doping increases in cuprate superconductors, the superconducting transition temperature increases to a maximum at the so-called optimal doping, and then decreases in the overdoped regime. In the past few decades, research has primarily focused on the underdoped and optimally doped regions of the phase diagram. Here, phenomena such as the pseudogap and strange metal non-superconducting states make it difficult to determine the superconducting pairing mechanism. More recently, experiments have shown unconventional behaviour in strongly overdoped cuprates, in both the normal and superconducting states. However, a real-space investigation of the unconventional superconductivity in the absence of the pseudogap is lacking, and the superconductor-to-metal phase transition in the overdoped regime remains controversial. Here we use scanning tunnelling microscopy to investigate the atomic-scale electronic structure of overdoped Bi 2 Sr 2 Ca n–1 Cu n O 2n + 4 + δ cuprates. We show that, at low energies, the spectroscopic maps are well described by dispersive d-wave quasiparticle interference patterns. However, as the bias increases to the superconducting coherence peak energy, a periodic and non-dispersive pattern emerges. The position of the coherence peaks exhibits particle–hole asymmetry that modulates with the same period. Finally, we propose that this behaviour is due to quasiparticle interference caused by pair-breaking scattering between flat antinodal Bogoliubov bands.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impact of thermodynamic fluctuations and pattern size on the nucleation behavior during area selective deposition

In this work, the authors explore the impact that thermodynamic fluctuations have on the spontaneous appearance of defects during area selective deposition on patterned surfaces that are fully covered by adsorbates under local thermodynamic equilibrium, such as self-assembled monolayers. By using a simple lattice gas model for the adsorbed monolayer, the authors were able to track the spontaneous formation of defects in the monolayer as a function of the pattern width. The results indicate that, for pattern widths of the order of tens of nanometers, roughening effects at the pattern edge can be the leading source for the spontaneous appearance of nucleation defects. This leads to an enhancement of the density of defects that can be up to three orders of magnitude higher than those expected in uniform (not patterned) surfaces. The model also predicts a density of defects that is inversely proportional to the pattern width. Finally, if the dynamic nucleation of defects during area selective deposition is driven by thermodynamic fluctuations, the model predicts that the nucleation rate should be proportional to the total precursor fluency and independent of purge times. Moreover, a tight confinement of the monolayer through a high quality smooth interface in the patterned substrate and strong cohesive interactions between adsorbates should each contribute to a reduction of the overall defect density.

36 MATERIALS SCIENCE↗

Structural Model for the Flip-Flop Action in Thiamin Pyrophosphate-Dependent Human Pyruvate Dehydrogenase

The derivative of vitamin B1 thiamin pyrophosphate (TPP) is a cofactor of enzymes performing catalysis in pathways of energy production, including (i) decarboxylation of alpha-keto acids followed by (ii) transketolation. These enzymes have shown a common mechanism of TPP activation by imposing an active V-conformation of this coenzyme that brings the N4 atom of the aminopyrimidine ring to the distance required for the intramolecular C-H N hydrogen-bonding with the C2- atom of the thiazolium ring. The reactive C2 atom of TPP is the nucleophile that attacks the carbonyl carbon of different substrates used by the TPP-dependent enzymes. The structure of the heterotetrameric human pyruvate dehydrogenase (Elp) recently determined in our laboratory (1) revealed the association pattern of the subunits and the specifics of two chemically equivalent cofactor binding sites. Dynamic nonequivalence of these two cofactor sites directs the flip-flop action of this enzyme, depending upon which two active sites effect each other (2). The crystal structure derived from the holo-form of Elp provided the basis for the model of the flip-flop action of Elp in which different steps of the catalytic reaction are performed in each of the two cofactor sites at any given moment, where these steps are governed by the concerted shuttle-like motion of the subunits. It is further proposed that balancing a hydrogen-bond network and related cofactor geometry determine the continuity of catalytic events.

Ciszak, Ewa↗

Parylene C as a Sacrificial Material for Microfabrication

Parylene C has been investigated for use as a sacrificial material in microfabrication. Although Parylene C cannot be patterned lithographically like photoresists, it nevertheless extends the range of processing options by offering a set of properties that are suitable for microfabrication and are complementary to those of photoresists. The compatibility of Parylene C with several microfabrication processes was demonstrated in experiments in which a thin film of Parylene C was deposited on a silicon wafer, then several thin metal films were deposited and successfully patterned, utilizing the Parylene C pads as a sacrificial layer. The term "parylene" -- a contraction of "poly(para-xylene)" -- denotes a family of vapor-deposited polymers. In Parylene C (the most common form of parylene), a chlorine atom is substituted for one of the hydrogen atoms on the benzene ring of each para-xylene moiety. Heretofore, parylenes have been used as conformal coating materials in diverse applications.

Beamesderfer, Michael↗

Statistical Modeling and Analysis of k -Layer Coverage of Two-Dimensional Materials in Inkjet Printing Processes

Two-dimensional layered materials/flakes, also known as crystalline atom-thick layer nanosheets, have recently been receiving great attention in electronics fabrication due to their unique and intriguing properties. The k-layer coverage area (i.e., the area covered by k number of overlapping layers) of the printed flake pattern significantly impacts on the properties of the printed electronics. In this work, we constructed a statistical model to describe the k-layer coverage of randomly distributed two-dimensional materials. A series of results are obtained to provide not only the expectation but also the variance of the coverage area. The boundary effects on the random flakes coverage are also studied. In addition, an approximated statistical testing approach is also developed in this work to detect abnormal coverage patterns. Furthermore, the case studies based on simulated data and real flakes images obtained from the inkjet printing process demonstrate the accuracy and effectiveness of the proposed model and analysis methods.

36 MATERIALS SCIENCE↗

Semiempirical Theories of the Affinities of Negative Atomic Ions

The determination of the electron affinities of negative atomic ions by means of direct experimental investigation is limited. To supplement the meager experimental results, several semiempirical theories have been advanced. One commonly used technique involves extrapolating the electron affinities along the isoelectronic sequences, The most recent of these extrapolations Is studied by extending the method to Include one more member of the isoelectronic sequence, When the results show that this extension does not increase the accuracy of the calculations, several possible explanations for this situation are explored. A different approach to the problem is suggested by the regularities appearing in the electron affinities. Noting that the regular linear pattern that exists for the ionization potentials of the p electrons as a function of Z, repeats itself for different degrees of ionization q, the slopes and intercepts of these curves are extrapolated to the case of the negative Ion. The method is placed on a theoretical basis by calculating the Slater parameters as functions of q and n, the number of equivalent p-electrons. These functions are no more than quadratic in q and n. The electron affinities are calculated by extending the linear relations that exist for the neutral atoms and positive ions to the negative ions. The extrapolated. slopes are apparently correct, but the intercepts must be slightly altered to agree with experiment. For this purpose one or two experimental affinities (depending on the extrapolation method) are used in each of the two short periods. The two extrapolation methods used are: (A) an isoelectronic sequence extrapolation of the linear pattern as such; (B) the same extrapolation of a linearization of this pattern (configuration centers) combined with an extrapolation of the other terms of the ground configurations. The latter method Is preferable, since it requires only experimental point for each period. The results agree within experimental error with all data, except with the most recent value of C, which lies 10% lower.

Edie, John W.↗

Magnetic metamaterials by ion-implantation

We present a method for the additive fabrication of planar magnetic nanoarrays with minimal surface roughness. Synthesis is accomplished by combining electron-beam lithography, used to generate nanometric patterned masks, with ion implantation in thin films. By implanting 56 Fe + ions, we are able to introduce magnetic functionality in a controlled manner into continuous Pd thin films, achieving 3D spatial resolution down to a few tens of nanometers. Our results demonstrate the application of this technique in fabricating square artificial spin ice lattices, which exhibit well-defined magnetization textures and interactions among the patterned magnetic elements.

36 MATERIALS SCIENCE↗

Structural trends in atomic nuclei from laser spectroscopy of tin

Tin is the chemical element with the largest number of stable isotopes. Its complete proton shell, comparable with the closed electron shells in the chemically inert noble gases, is not a mere precursor to extended stability; since the protons carry the nuclear charge, their spatial arrangement also drives the nuclear electromagnetism. We report high-precision measurements of the electromagnetic moments and isomeric differences in charge radii between the lowest 1/2 + , 3/2 + , and 11/2 - states in 117–131 Sn, obtained by collinear laser spectroscopy. Supported by state-of-the-art atomic-structure calculations, the data accurately show a considerable attenuation of the quadrupole moments in the closed-shell tin isotopes relative to those of cadmium, with two protons less. Linear and quadratic mass-dependent trends are observed. While microscopic density functional theory explains the global behaviour of the measured quantities, interpretation of the local patterns demands higher-fidelity modelling.

74 ATOMIC AND MOLECULAR PHYSICS↗

Quantifying dislocation density in Al-Cu coatings produced by cold spray deposition

This work quantifies the plastic deformation in terms of dislocation density for a series of cold sprayed Al-Cu coatings with copper contents from 2 mass% to 5 mass%. The success of the deposition and consolidation of the feedstock powders during the cold spray process rely on the occurrence of significant plastic deformation. Inert gas atomized Al-Cu alloy powders were sprayed onto substrates made of an Al-Cu-Mg-Mn alloy (AA2024) to produce dense coatings using a low pressure cold spray system with helium as the carrier gas. X-ray diffraction patterns were obtained from the Al-Cu feedstock powder material and the cold sprayed coatings using a monochromatic X-ray source, and the dislocation density was determined via an X-ray whole profile analysis. Increasing the Cu alloy content (from 2 mass% to 5 mass%) systematically increased the dislocation density in the Al-Cu coatings from (4.3 ± 0.5) × 10 14 m -2 to (7.5 ± 0.8) × 10 14 m -2 . The dislocation densities in the feedstock powders ranging from (0.4 ± 0.1) × 10 14 m -2 to (1.8 ± 0.2) × 10 14 m -2 were all lower than the dislocation densities in the corresponding coatings. The increasing deformation level in the Al-Cu coatings with Cu additions were confirmed by the classic and modified Williamson-Hall analyses of X-ray diffraction data, and peak breadth measurements from neutron diffraction data. Finally, a high density of dislocations was also observed in these coatings via electron backscatter diffraction and transmission electron microscopy.

36 MATERIALS SCIENCE↗

Engineering the fracture resistance of 2H-transition metal dichalcogenides using vacancies: An in-silico investigation based on HRTEM images

Vacancy engineering of 2H-transition metal dichalcogenides (2H-TMDs) has recently attracted great attention due to its potential to fine-tune the phonon and opto-electric properties of these materials. From a mechanical perspective, this symmetry-breaking process typically reduces the overall crack resistance of the material and adversely affects its reliability. However, vacancies can trigger the formation of heterogeneous phases that synergistically improve fracture properties. In this study, using MoSe2 as an example, we characterize the types and density of vacancies that can emerge under electron irradiation and quantify their effect on fracture. Molecular dynamic (MD) simulations, employing a re-parameterized Tersoff potential capable of accurately capturing bond dissociation and structural phase changes, reveal that isolated transition metal monovacancies or chalcogenide divacancies tend to arrest the crack tip and hence enhance the monolayer toughness. In contrast, isolated chalcogenide monovacancies do not significantly affect toughness. The investigation further reveals that selenium vacancy lines, formed by high electron dose rates, alter the crack propagating direction and lead to multiple crack kinking. Using atomic displacements and virial stresses together with a continuum mapping, displacement, strain, and stress fields are computed to extract mechanistic information, e.g., conditions for crack kinking and size effects in fracture events. The study also reveals the potential of specific defect patterns, “vacancy engineering,” to improve the toughness of 2H-TMDs materials.

36 MATERIALS SCIENCE↗