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At least 1,495 records · Page 83

Tunable rainbow light trapping in ultrathin resonator arrays

Abstract Rainbow light trapping in plasmonic devices allows for field enhancement of multiple wavelengths within a single device. However, many of these devices lack precise control over spatial and spectral enhancement profiles and cannot provide extremely high localised field strengths. Here we present a versatile, analytical design paradigm for rainbow trapping in nanogroove arrays by utilising both the groove-width and groove-length as tuning parameters. We couple this design technique with fabrication through multilayer thin-film deposition and focused ion beam milling, which enables the realisation of unprecedented feature sizes down to 5 nm and corresponding extreme normalised local field enhancements up to 10 3 . We demonstrate rainbow trapping within the devices through hyperspectral microscopy and show agreement between the experimental results and simulation. The combination of expeditious design and precise fabrication underpins the implementation of these nanogroove arrays for manifold applications in sensing and nanoscale optics.

42 ENGINEERING↗

Layered metals as polarized transparent conductors

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Technological solutions reflect this trade-off, achieving the desired transparencies only by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. We demonstrate that slabs of the layered oxides Sr 2 RuO 4 and Tl 2 Ba 2 CuO 6+δ are optically transparent even at macroscopic thicknesses >2 μm for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens.

36 MATERIALS SCIENCE↗

Anisotropic resistance with a 90° twist in a ferromagnetic Weyl semimetal, Co 2 MnGa

Weyl semimetals exhibit exotic magnetotransport phenomena such as the chiral anomaly and surface-to-bulk quantum oscillations (Weyl orbits) due to chiral bulk states and topologically protected surface states. Here we report a unique transport property in crystals of the ferromagnetic nodal-line Weyl semimetal Co 2 MnGa that have been polished to micron thicknesses using a focused ion beam. These thin crystals exhibit a large planar resistance anisotropy (10 × ) with axes that rotate by 90 degrees between opposite faces of the crystal. We use symmetry arguments and electrostatic simulations to show that the observed anisotropy resembles that of an isotropic conductor with surface states that are impeded from hybridization with bulk states. The origin of these states awaits further experiments that can correlate the surface bands with the observed 90° twist.

36 MATERIALS SCIENCE↗

Effect of solid-electrolyte pellet density on failure of solid-state batteries

Abstract Despite the potentially higher energy density and improved safety of solid-state batteries (SSBs) relative to Li-ion batteries, failure due to Li-filament penetration of the solid electrolyte and subsequent short circuit remains a critical issue. Herein, we show that Li-filament growth is suppressed in solid-electrolyte pellets with a relative density beyond ~95%. Below this threshold value, however, the battery shorts more easily as the density increases due to faster Li-filament growth within the percolating pores in the pellet. The microstructural properties (e.g., pore size, connectivity, porosity, and tortuosity) of $$75\%{{{{{\rm{L}}}}}}{{{{{{\rm{i}}}}}}}_{2}{{{{{\rm{S}}}}}}-25\%{{{{{{\rm{P}}}}}}}_{2}{{{{{{\rm{S}}}}}}}_{5}$$ 75 % L i 2 S − 25 % P 2 S 5 with various relative densities are quantified using focused ion beam–scanning electron microscopy tomography and permeability tests. Furthermore, modeling results provide details on the Li-filament growth inside pores ranging from 0.2 to 2 μm in size. Our findings improve the understanding of the failure modes of SSBs and provide guidelines for the design of dendrite-free SSBs.

25 ENERGY STORAGE↗

Enhanced sensitivity for electron affinity measurements of rare elements

The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements.

Maier, F. M. [Univ. of Greifswald (Germany); Europ↗

Extracellular filaments revealed by affinity capture cryogenic-electron tomography

Cryogenic-electron tomography (cryo-ET) has provided an unprecedented glimpse into the nanoscale architecture of cells by combining cryogenic preservation of biological structures with electron tomography. Micropatterning of extracellular matrix proteins is increasingly used as a method to prepare adherent cell types for cryo-ET as it promotes optimal positioning of cells and subcellular regions of interest for vitrification, cryo-focused ion beam (cryo-FIB) milling, and data acquisition. Here we demonstrate a micropatterning workflow for capturing minimally adherent cell types, human T cells and Jurkat cells, for cryo-FIB and cryo-ET. Our affinity capture system facilitated the nanoscale imaging of Jurkat cells, revealing extracellular filamentous structures. It improved workflow efficiency by consistently producing grids with a sufficient number of well-positioned cells for an entire cryo-FIB session. Affinity capture can be extended to facilitate high-resolution imaging of other adherent and non-adherent cell types with cryo-ET.

Biochemistry↗

Intergranular corrosion of Ni-30Cr in high-temperature hydrogenated water after removing surface passivating film

Abstract High-resolution transmission electron microscopy and atom probe tomography are used to characterize the initial passivation and subsequent intergranular corrosion of degraded grain boundaries in a model Ni-30Cr alloy exposed to 360 °C hydrogenated water. Upon initial exposure for 1000 h, the alloy surface directly above the grain boundary forms a thin passivating film of Cr 2 O 3 , protecting the underlying grain boundary from intergranular corrosion. However, the metal grain boundary experiences severe Cr depletion and grain boundary migration during this initial exposure. To understand how Cr depletion affects further corrosion, the local protective film was sputtered away using a glancing angle focused ion beam. Upon further exposure, the surface fails to repassivate, and intergranular corrosion is observed through the Cr-depleted region. Through this combination of high-resolution microscopy and localized passive film removal, we show that, although high-Cr alloys are resistant to intergranular attack and stress corrosion cracking, degradation-induced changes in the underlying metal at grain boundaries make the material more susceptible once the initial passive film is breached.

(S)TEM↗

Directional ballistic transport in the two-dimensional metal PdCoO2

Abstract In an idealized infinite crystal, the material properties are constrained by the symmetries of the unit cell. The point-group symmetry is broken by the sample shape of any finite crystal, but this is commonly unobservable in macroscopic metals. To sense the shape-induced symmetry lowering in such metals, long-lived bulk states originating from an anisotropic Fermi surface are needed. Here we show how a strongly facetted Fermi surface and the long quasiparticle mean free path present in microstructures of PdCoO 2 yield an in-plane resistivity anisotropy that is forbidden by symmetry on an infinite hexagonal lattice. We fabricate bar-shaped transport devices narrower than the mean free path from single crystals using focused ion beam milling, such that the ballistic charge carriers at low temperatures frequently collide with both of the side walls that define the channel. Two symmetry-forbidden transport signatures appear: the in-plane resistivity anisotropy exceeds a factor of 2, and a transverse voltage appears in zero magnetic field. Using ballistic Monte Carlo simulations and a numerical solution of the Boltzmann equation, we identify the orientation of the narrow channel as the source of symmetry breaking.

36 MATERIALS SCIENCE↗

Correlative montage parallel array cryo-tomography for in situ structural cell biology

Abstract Imaging large fields of view while preserving high-resolution structural information remains a challenge in low-dose cryo-electron tomography. Here we present robust tools for montage parallel array cryo-tomography (MPACT) tailored for vitrified specimens. The combination of correlative cryo-fluorescence microscopy, focused-ion-beam milling, substrate micropatterning, and MPACT supports studies that contextually define the three-dimensional architecture of cells. To further extend the flexibility of MPACT, tilt series may be processed in their entirety or as individual tiles suitable for sub-tomogram averaging, enabling efficient data processing and analysis.

59 BASIC BIOLOGICAL SCIENCES↗

Heavy-ion production of 77 Br and 76 Br

Many radioisotopes with potential medical applications are difficult to produce routinely, especially those on the proton-rich side of the valley of stability. Current production methods typically use light-ion (protons or deuteron) reactions on materials of similar mass to the target radioisotope, which limits the elemental target material available and may require the use of targets with poor thermal properties (as is the case for the production of radiobromine). These reactions may also create significant amounts of proton-rich decay products which require chemical separation from the desired product in a highly radioactive environment. A promising alternative method using heavy-ion fusion-evaporation reactions for the production of the medically relevant bromine radioisotopes 76 Br (t 1/2 = 16.2 h) and 77 Br (t 1/2 = 57.0 h) is presented. Heavy-ion beams of 28 Si and 16 O were used to bombard natural chromium and copper targets just above the Coulomb barrier at the University of Notre Dame's Nuclear Science Laboratory to produce these bromine and precursor radioisotopes by fusion-evaporation reactions. Production yields for these reactions were measured and compared to PACE4 calculations. In addition to using more robust targets for irradiation, a simple physical–chemical separation method is proposed that will lead to very high radiopurity yields. A summary of accelerator facility requirements needed for routine production of these radioisotopes is also presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Origin of the enhanced Nb3Sn performance by combined Hf and Ta doping

Abstract In recent years there has been an increasing effort in improving the performance of Nb 3 Sn for high-field applications, in particular for the fabrication of conductors suitable for the realization of the Future Circular Collider (FCC) at CERN. This challenging task has led to the investigation of new routes to advance the high-field pinning properties, the irreversibility and the upper critical fields ( H Irr and H c2 , respectively). The effect of hafnium addition to the standard Nb-4Ta alloy has been recently demonstrated to be particularly promising and, in this paper, we investigate the origins of the observed improvements of the superconducting properties. Electron microscopy, Extended X-ray Absorption Fine Structure Spectroscopy (EXAFS) and Atom Probe Tomography (APT) characterization clearly show that, in presence of oxygen, both fine Nb 3 Sn grains and HfO 2 nanoparticles form. Although EXAFS is unable to detect significant amounts of Hf in the A15 structure, APT does indeed reveal some residual intragrain metallic Hf. To investigate the layer properties in more detail, we created a microbridge from a thin lamella extracted by Focused Ion Beam (FIB) and measured the transport properties of Ta-Hf-doped Nb 3 Sn. H c2 (0) is enhanced to 30.8 T by the introduction of Hf, ~ 1 T higher than those of only Ta-doped Nb 3 Sn, and, even more importantly the position of the pinning force maximum exceeds 6 T, against the typical ~ 4.5–4.7 T of the only Ta-doped material. These results show that the improvements generated by Hf addition can significantly enhance the high-field performance, bringing Nb 3 Sn closer to the requirements necessary for FCC realization.

36 MATERIALS SCIENCE↗

Quantification of defects engineered in single layer MoS 2

Atomic defects are controllably introduced in suspended single layer molybdenum disulfide (1L MoS 2 ) using helium ion beam. Vacancies exhibit one missing atom of molybdenum and a few atoms of sulfur. Quantification was done using a Scanning Transmission Electron Microscope (STEM) with an annular detector. Experimentally accessible inter-defect distance was employed to measure the degree of crystallinity in 1L MoS 2 . A correlation between the appearance of an acoustic phonon mode in the Raman spectra and the inter-defect distance was established, which introduces a new methodology for quantifying defects in two-dimensional materials such as MoS 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing the hydrolytic degradation of UF 4 in humid air

This manuscript describes the chemical transformations that occur during hydrolysis of uranium tetrafluoride (UF 4 ) due to its storage in humid air (85% and 50% relative humidity) at ambient temperatures. This hydrolysis was previously reported to proceed slowly or not at all (depending on the percent relative humidity); however, previous reports relied primarily on X-ray diffraction methods to probe uranium speciation. Here, we employ a battery of physiochemical probing techniques to explore potential hydrolysis, including Raman spectroscopy, powder X-ray diffraction, 19 F nuclear magnetic resonance spectroscopy, scanning electron microscopy, and focused ion beam microscopy with energy-dispersive X-ray spectroscopy. Of these, only Raman spectroscopy proved to be particularly useful at observing chemical changes to UF 4 . It was found that anhydrous UF 4 slightly oxidizes over the course of thirteen days to Schoepite-like uranium complexes and possibly UO 3 . In contrast, UF 4 exposed to 50% relative humidity slightly decomposes into UO 2 F 2 , Schoepite-like uranium complexes, and possibly a high order uranium oxide that eluded chemical assignment (U x O y ). Despite the rich chemical speciation observed in our Raman spectroscopy measurements, X-ray diffraction and 19 F NMR measurements on the same material showed no changes. Microscopy measurements suggest that the observed reactions between UF 4 and water occur primarily on the surface of UF 4 particulates via a method that is visually similar to surface corrosion of metals. Therefore, we postulate that NMR spectroscopy and X-ray diffraction, which are well-suited for bulk analysis, are less suited than Raman spectroscopy to observe the surface-based reactions that occur to UF 4 when exposed to humid air. Considering the importance of UF 4 in the production of nuclear fuel and weapons, the results presented herein are widely applicable to numerous nuclear science fields where uranium detection and speciation in humid environments is of value, including nuclear nonproliferation and nuclear forensics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Light-enhanced oxygen degradation of MAPbBr 3 single crystal

Organometal halide perovskites are promising materials for optoelectronic applications, whose commercial realization depends critically on their stability under multiple environmental factors. In this study, a methylammonium lead bromide (MAPbBr 3 ) single crystal was cleaved and exposed to simultaneous oxygen and light illumination under ultrahigh vacuum (UHV). The exposure process was monitored using X-ray photoelectron spectroscopy (XPS) with precise control of the exposure time and oxygen pressure. It was found that the combination of oxygen and light accelerated the degradation of MAPbBr 3 , which could not be viewed as a simple addition of that by oxygen-only and light-only exposures. The XPS spectra showed significant loss of carbon, bromine, and nitrogen at an oxygen exposure of 10 10 Langmuir with light illumination, approximately 17 times of the additive effects of oxygen-only and light-only exposures. It was also found that the photoluminescence (PL) emission was much weakened by oxygen and light co-exposure, while previous reports had shown that PL was substantially enhanced by oxygen-only exposure. Measurements using a scanning electron microscope (SEM) and focused ion beam (FIB) demonstrated that the crystal surface was much roughened by the co-exposure. Furthermore, Density functional theory (DFT) calculations revealed the formation of superoxide and oxygen induced gap state, suggesting the creation of oxygen radicals by light illumination as a possible microscopic driving force for enhanced degradation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Lithium isotope analysis on the Neoma MS/MS MC-ICP-MS

Accurate and precise lithium isotopic composition measurements are achieved on the Neoma MS/MS after careful tuning of the prefilter lenses to allow both Li ion beams to pass through unimpeded.

07 ISOTOPE AND RADIATION SOURCES↗

First (p,n) reaction measurement in inverse kinematics with SECAR

Nucleosynthesis in the νp-process occurs in regions of slightly proton-rich nuclei in the neutrino-driven wind of core-collapse supernovae. The process proceeds via a sequence of (p,γ) and (n,p) reactions, and depending on the conditions, may produce elements between Ni and Sn. Recent studies show that a few key (n,p) reactions regulate the efficiency of the neutrino-p process (νp-process). We performed a study of one of such (n,p) reactions via the measurement of the reverse (p,n) in inverse kinematics with SECAR at NSCL/FRIB.Such proton-induced reaction measurements are particularly challenging, as the recoils and the unreacted projectiles have nearly identical masses. An appropriate separation level can be achieved with SECAR, and along with the incoincidence detection of neutrons these measurements become attainable. The preparation of the SECAR system for accommodating its first (p,n) reaction measurement, including the development of alternative ion beam optics, and the setup of the in-coincidence neutron detection, along with discussion on preliminary results from the p(58Fe,n)58Co reaction measurement are presented and discussed.

Tsintari, P↗

Decay spectroscopy in the neutron-rich Mo–Ru–Pd region

A leading challenge of nuclear-structure research is to understand the properties of nuclides of extreme isospin. Experiments at radioactive-ion-beam facilities, such as the Facility for Rare Isotope Beams in the US, may answer key questions that address diverse topics including fundamental nuclear physics, stellar nucleosynthesis and nuclear applications. The neutron-rich Mo–Ru–Pd (Z = 42 – 46) nuclides are hypothesised to exhibit triaxial-oblate deformation. We performed an experiment with the Facility for Rare Isotope Beams Decay Station initiator (FDSi) to study the structure and decay properties of nuclides in this region. Over 100 different nuclides have been identified in a preliminary analysis of the data. This work presents a first look at several examples between Rb (Z = 37) and Ag (Z = 47). Performance of the FDSi and methods developed to measure ground-state and excited-state lifetimes are presented, and plans for future work are also discussed.

Allmond, James [ORNL] (ORCID:0000000165338721)↗