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At least 649 records · Page 36

The Wavelength-Dispersive Spectrometer and Its Proposed Use in the Analytical Electron Microscope

The Analytical Electron Microscope (AEM) equipped with a wavelength-dispersive spectrometer (WDS) should have the ability to resolve peaks which normally overlap in the spectra from an energy-dispersive spectrometer (EDS). With a WDS it should also be possible to measure lower concentrations of elements in thin foils due to the increased peak-to-background ratio compared with EDS. The WDS will measure X-ray from the light elements (4 less than Z less than 1O) more effectively. This paper addresses the possibility of interfacing a compact WDS with a focussing circle of approximately 4 cm to a modem AEM with a high-brightness (field emission) source of electrons.

Goldstein, Joseph I.↗

Continuous, edge localized ion heating during non-solenoidal plasma startup and sustainment in a low aspect ratio tokamak

Plasmas in the Pegasus spherical tokamak are initiated and grown by the non-solenoidal local helicity injection (LHI) current drive technique. The LHI system consists of three adjacent electron current sources that inject multiple helical current filaments that can reconnect with each other. Anomalously high impurity ion temperatures are observed during LHI with T i,OV ≤ 650 eV, which is in contrast to T i,OV ≤ 70 eV from Ohmic heating alone. Spatial profiles of T i,OV indicate an edge localized heating source, with T i,OV ~ 650 eV near the outboard major radius of the injectors and dropping to ~150 eV near the plasma magnetic axis. Experiments without a background tokamak plasma indicate the ion heating results from magnetic reconnection between adjacent injected current filaments. In these experiments, the HeII T i perpendicular to the magnetic field is found to scale with the reconnecting field strength, local density, and guide field, while ${{T}_{\text{i},\parallel}}$ experiences little change, in agreement with two-fluid reconnection theory. In conclusion, this ion heating is not expected to significantly impact the LHI plasma performance in Pegasus, as it does not contribute significantly to the electron heating. However, estimates of the power transfer to the bulk ion are quite large, and thus LHI current drive provides an auxiliary ion heating mechanism to the tokamak plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

New space processing experiments for the Skylab missions.

The M512 Materials Processing Facility, which is the main item of equipment for the Skylab space manufacturing experiments is described. It is basically an electron-beam welding apparatus, consisting of a battery power supply, a 20-kV electron beam source, and a spherical 40-cm-diam vacuum chamber. It will be used to perform the M551 Metals Melting Experiment, the M552 Exothermic Brazing Experiment, the M553 Sphere Forming Experiment, the M554 Composite Casting Experiment, the M555 Gallium Arsenide Crystal Growth Experiment, the M561 Whisker-Reinforced Composites Experiment, the M562 Indium Antimonide Crystal Growth, Experiment, the M563 Mixed III-V Crystal Growth Experiment, the M564 Alkali Halide Eutectics Experiment, the M565 Silver Grids Melted in Space Experiment, and the M566 Copper-Aluminum Eutectic Experiment. Three apparatus systems designed to broaden the technical scope of the experiments and to gain experience with new experimental techniques are described. These are an electrophoretic separator, an electromagnetic levitation system, and a versatile electric furnace with an electronic control system.

Bredt, J. H.↗

Inorganic Halide Perovskitoid TlPbI 3 for Ionizing Radiation Detection

Room temperature semiconductor detector (RTSD) materials for γ-ray and X-ray radiation are in great demand for the nonproliferation of nuclear materials as well as for biomedical imaging applications. Halide perovskites have attracted great attention as emerging and promising RTSD materials. In this contribution, the material synthesis, purification, crystal growth, crystal structure, photoluminescence properties, ionizing radiation detection performance, and electronic structure of the inorganic halide perovskitoid compound TlPbI 3 are reported on. This compound crystallizes in the ABX 3 non-perovskite crystal structure with a high density of d = 6.488 g·cm –3 , has a wide bandgap of 2.25 eV, and melts congruently at a low temperature of 360 °C without phase transitions, which allows for facile growth of high quality crystals with few thermally-activated defects. High-quality TlPbI 3 single crystals of centimeter-size are grown using the vertical Bridgman method using purified raw materials. A high electrical resistivity of ≈10 12 Ω·cm is readily obtainable, and detectors made of TlPbI 3 single crystals are highly photoresponsive to Ag K α X-rays (22.4 keV), and detects 122 keV γ-rays from 57 Co radiation source. The electron mobility-lifetime product µ e τ e was estimated at 1.8 × 10 –5 cm 2 ·V –1 . A high relative static dielectric constant of 35.0 indicates strong capability in screening carrier scattering and charged defects in TlPbI 3 .

36 MATERIALS SCIENCE↗

On the Source of Conductivity in Alkaline Zn Anodes: Zn Percolation and ZnO Bridging

Alkaline Zn anodes are fundamental to commercial Zn-MnO 2 batteries as well as emerging rechargeable designs. In these electrodes, Zn particles are both the active material and source of electronic conduction. However, there are known cases in which electronic connectivity between Zn particles or the current collecting pin is lost even though the battery continues to function. Here we use X-ray computed tomography (CT) of AA batteries to demonstrate several examples of Zn particle-to-particle connectivity breakdown, which is observed even in cases at relatively high discharge rate. This indicates maintenance of the electronic network through the less-conductive ZnO discharge product. We introduce a new equation for electronic conductivity maintained through bridges of ZnO formed between percolating Zn particles. This necessitates discarding the Bruggeman correlation and instead redefining effective electronic conductivity using percolation theory. We demonstrate that such a model for conduction enables prediction of an inverted reaction zone, which is an experimentally observed case in which significant Zn dissolution and ZnO formation occurs heavily near the current collecting pin. Current computational Zn-MnO 2 models never predict an inverted reaction zone, and thus the updated conductivity enables models to accurately explain a wider range of experimental conditions.

Guida, Dominick P. [Northeastern Univ., Boston, MA↗

Prototype Stilbene Neutron Collar II

A neutron collar using stilbene organic scintillator cells for fast neutron counting is described for the assay of fresh low enriched uranium (LEU) fuel assemblies. The prototype stilbene collar has a form factor similar to standard He-3 based collars and uses an AmLi interrogation neutron source. This report describes the simulation, using a custom LLNL developed MCNPX, of list mode neutron correlation data on various fuel assemblies. Some of these fuel assemblies have neutron absorbers (burnable Gd poisons) and partial defect s (DU, Fe, Pb pins). Calibration curves (doubles vs 235 U linear mass density) are presented for fast (with Cd lining) mode of operation. The modeling incorporates LLNL developed neutron crosstalk correction algorithms and stilbene light output detector response quench function. Pileup issues are addressed using the LLNL code GamGen / RadSrc to estimate the flux of alpha decay gammas from the fuel assemblies on the stilbene cells with and without Pb shielding. One panel of the prototype collar using 10 high-efficiency 4”x2” stilbene cells from Inrad Optics, using LLNL developed technology, has been constructed and calibrated for optimal PSD and data acquisition electronics. Several sources (AmLi, AmBe, Cf, DD, and DT) have been measured with the single panel and the measured data is consistent with the modeling. A novel part of our work was to determine the light output (LO) quench function for the Inrad 4” x 2” stilbene crystals through a LLNL-MCNPX simulation based optimized fitting of the measured LO data.

42 ENGINEERING↗

Preface to the JPCM special issue on intense radiation sources in condensed matter and materials physics

This special issue is designed to honour the contributions of our colleague Neville Greaves who was among the first to apply newly-available synchrotron x-ray techniques to study the synthesis, structures and properties of advanced materials [1, 2]. His wide ranging work on ceramics, glasses and nanomaterials was celebrated in a recent issue of the J. Non-Cryst. Solids [3]. Neville's contributions to synchrotron research, highlighted here, focussed on design and construction of new beamline capabilities and sample environments to probe materials under different physical and chemical conditions, integrating various techniques to obtain complementary data on structure and bonding. The innovative nature of his work is illustrated by his studies of liquids and glasses, where he incorporated aerodynamic levitation into these experimental techniques, using both synchrotron x-ray and neutron beams to probe the structural transformations and dynamics combined with molecular dynamics simulations to study atomic scale organisation. His work has had a major impact on fundamental condensed matter physics and chemistry as well as applied materials science; and in this issue, we present contributions from colleagues using and developing new experimental techniques at current and next-generation synchrotron, neutron and free-electron laser sources and in their own laboratories, that probe the fundamental physics, chemistry and functional properties of novel materials and processes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Characterization of iron oxide nanoparticle films at the air–water interface in Arctic tundra waters

Here, massive amounts of organic carbon have accumulated in Arctic permafrost and soils due to anoxic and low temperature conditions that limit aerobic microbial respiration. Alternative electron acceptors are thus required for microbes to degrade organic carbon in these soils. Iron or iron oxides have been recognized to play an important role in carbon cycle processes in Arctic soils, although the exact form and role as an electron acceptor or donor remain poorly understood. Here, Arctic biofilms collected during the summers of 2016 and 2017 from tundra surface waters on the Seward Peninsula of western Alaska were characterized with a suite of microscopic and spectroscopic methods. We hypothesized that these films contain redox-active minerals bound to biological polymers. The major components of the films were found to be iron oxide nanoparticle aggregates associated with extracellular polymeric substances. The observed mineral phases varied between films collected in different years with magnetite (Fe 2+ Fe 2 3+ O 4 ) nanoparticles (<5 nm) predominantly identified in the 2016 films, while for films collected in 2017 ferrihydrite-like amorphous iron oxyhydroxides were found. While the exact formation mechanism of these Artic iron oxide films remains to be explored, the presence of magnetite and other iron oxide/oxyhydroxide nanoparticles at the air–water interface may represent a previously unknown source of electron acceptors for continual anaerobic microbial respiration of organic carbon within poorly drained Arctic tundra.

54 ENVIRONMENTAL SCIENCES↗

Modeling Ionosphere Environments: Creating an ISS Electron Density Tool

The International Space Station (ISS) maintains an altitude typically between 300 km and 400 km in low Earth orbit (LEO) which itself is situated in the Earth's ionosphere. The ionosphere is a region of partially ionized gas (plasma) formed by the photoionization of neutral atoms and molecules in the upper atmosphere of Earth. It is important to understand what electron density the spacecraft is/will be operating in because the ionized gas along the ISS orbit interacts with the electrical power system resulting in charging of the vehicle. One instrument that is already operational onboard the ISS with a goal of monitoring electron density, electron temperature, and ISS floating potential is the Floating Potential Measurement Unit (FPMU). Although this tool is a valuable addition to the ISS, there are limitations concerning the data collection periods. The FPMU uses the Ku band communication frequency to transmit data from orbit. Use of this band for FPMU data runs is often terminated due to necessary observation of higher priority Extravehicular Activities (EVAs) and other operations on ISS. Thus, large gaps are present in FPMU data. The purpose of this study is to solve the issue of missing environmental data by implementing a secondary electron density data source, derived from the COSMIC satellite constellation, to create a model of ISS orbital environments. Extrapolating data specific to ISS orbital altitudes, we model the ionospheric electron density along the ISS orbit track to supply a set of data when the FPMU is unavailable. This computer model also provides an additional new source of electron density data that is used to confirm FPMU is operating correctly and supplements the original environmental data taken by FPMU.

Gurgew, Danielle N.↗

Photochemical pathways in nucleobases measured with an X-ray FEL

The conversion of light energy into other molecular energetic degrees of freedom is often dominated by ultrafast, non-adiabatic processes. Femtosecond spectroscopy with optical pulses has helped in shaping our understanding of crucial processes in molecular energy-conversion. The advent of new, ultrashort and bright X-ray free electron laser sources opens the possibility to use X-ray-typical element and site sensitivity for ultrafast molecular research. We introduce two types of spectroscopy, ultrafast Auger and ultrafast X-ray absorption spectroscopy, and discuss their sensitivity to molecular processes. While Auger spectroscopy is able to monitor bond distance changes in the vicinity of an X-ray created core hole, near-edge absorption spectroscopy can deliver high-fidelity information on non-adiabatic transitions involving lone-pair orbitals. We display these features on the example of the UV-excited nucleobase thymine, investigated at the oxygen K-edge. We find a C–O bond elongation in the Auger data in addition to ππ*/nπ* non-adiabatic transition in X-ray near-edge absorption. We compare the results from both methods and draw a conclusive scenario of non-adiabatic molecular relaxation after UV excitation. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Estimation of isotope variation of N 2 O during denitrification by Pseudomonas aureofaciens and Pseudomonas chlororaphis: implications for N 2 O source apportionment

Soil microbial processes, stimulated by agricultural fertilization, account for 90 % of anthropogenic nitrous oxide ( N 2 O ), the leading source of ozone depletion and a potent greenhouse gas. Efforts to reduce N 2 O flux commonly focus on reducing fertilization rates. Management of microbial processes responsible for N 2 O production may also be used to reduce N 2 O emissions, but this requires knowledge of the prevailing process. To this end, stable isotopes of N 2 O have been applied to differentiate N 2 O produced by nitrification and denitrification. To better understand the factors contributing to isotopic variation during denitrification, we characterized the δ 15 N, δ 18 O and site preference (SP; the intramolecular distribution of 15 N in N 2 O ) of N 2 O produced during NO 3 - reduction by Pseudomonas chlororaphis subsp. aureofaciens and P. c. subsp. chlororaphis . The terminal product of denitrification for these two species is N 2 O because they lack thegene nitrous oxide reductase, which is responsible for the reduction of N 2 O to N 2 . In addition to species, treatments include delectron donor (citrate and succinate) and electron donor concentration(0.01, 0.1, 1 and 10 mM) as factors. In contrast to the expectation of a Rayleigh model, all treatments exhibited curvilinear behaviour between δ 15 N or δ 18 O and the extent of the reaction. The curvilinear behaviour indicates that the fractionation factor changed over the course of the reaction, something that is not unexpected for a multi-step process such as denitrification. Using the derivative of the equation, we estimated that the net isotope effects ( η ) vary by as much as 100 ‰ over the course of a single reaction, presenting challenges for using δ 15 N and δ 18 O as apportionment tools. In contrast, SP for denitrification was not affected by the extent of the reaction, the electron donor source or concentration, although the mean SP of N 2 O produced by each species differed. Hence, SP remains a robust indicator of the origin of N 2 O . To improve apportionment estimates with SP, future studies could evaluate other factors that contribute to the variation in SP.

54 ENVIRONMENTAL SCIENCES↗

A sensitive high repetition rate arrival time monitor for X-ray free electron lasers

X-ray free-electron laser sources enable time-resolved X-ray studies with unmatched temporal resolution. To fully exploit ultrashort X-ray pulses, timing tools are essential. However, new high repetition rate X-ray facilities present challenges for currently used timing tool schemes. Here we address this issue by demonstrating a sensitive timing tool scheme to enhance experimental time resolution in pump-probe experiments at very high pulse repetition rates. Our method employs a self-referenced detection scheme using a time-sheared chirped optical pulse traversing an X-ray stimulated diamond plate. By formulating an effective medium theory, we confirm subtle refractive index changes, induced by sub-milli-Joule intense X-ray pulses, that are measured in our experiment. The system utilizes a Common-Path-Interferometer to detect X-ray-induced phase shifts of the optical probe pulse transmitted through the diamond sample. Owing to the thermal stability of diamond, our approach is well-suited for MHz pulse repetition rates in superconducting linear accelerator-based free-electron lasers.

47 OTHER INSTRUMENTATION↗

Electron Cloud Simulations for the Electron-Ion Collider in Brookhaven National Laboratory

For high-intensity circular accelerators and storage rings, if the secondary electron emission yield (SEY) of the vacuum chamber surfaces is high, an EC (Electron Cloud) could build up with the passage of the circulating beam. The presence of EC can strongly affect the beam quality, such as transverse instabilities, transverse emittance growth, and beam loss. Furthermore, the heat load from EC can exceed the available cryogenic capability. For the RHIC superconducting (SC) arc magnets, to be used for the hadron storage ring of the Electron-Ion Collider (EIC), the dynamic heat load budget is 0.5 W/m to the 4.5 K stainless steel beam pipe. This can limit the maximum beam bunches or intensity of the EIC, hence diminishing the luminosity provided by the EIC. The EC has affected the beam instability and significantly contributed to cryogenic heat load in the Large Hadron Collider (LHC). Positron storage rings for which ECs have been a critical factor in the design and performance include KEKB in Japan and EC buildup remains one of the concerns for future high-intensity accelerators design. EC considerations have driven the SuperKEKB collider design and the positron damping ring for the proposed International Linear Collider (ILC). The LHC luminosity upgrade is contingent on reducing the bunch spacing to 25 ns; at this bunch spacing, severe EC buildup has been observed. The success of the upgrade is likely contingent on limiting EC buildup. To study the EC heat load, we did some EC simulations with PyECLOUD code for the dipole, quadrupole, sextupole magnets, and the warm (drift) section of the EIC hadron storage ring. PyECLOUD is an EC simulation code developed by CERN. The code has been validated and used to study EC in the LHC, SPS, and PS. To eliminate EC buildup, the sources of electrons must be minimized. First, we will reduce the production of electrons due to residual gas ionization by specifying the maximum gas density, which requires a vacuum chamber with low electron-stimulated desorption (ESD) yields and a sufficient (preferably distributed) pumping speed. Second, we should reduce the secondary electrons with a lower secondary electron yield (SEY) material.

43 PARTICLE ACCELERATORS↗

Dynamics of Molecular Hydrogen in Hypersaline Microbial Mars

Early Earth microbial communities that centered around the anaerobic decomposition of organic molecular hydrogen as a carrier of electrons, regulator of energy metabolism, and facilitator of syntroph'c microbial interactions. The advent of oxygenic photosynthetic organisms added a highly dynamic and potentially dominant term to the hydrogen economy of these communities. We have examined the daily variations of hydrogen concentrations in cyanobacteria-dominated microbial mats from hypersaline ponds in Baja California Sur, Mexico. These mats bring together phototrophic and anaerobic bacteria (along with virtually all other trophic groups) in a spatially ordered and chemically dynamic matrix that provides a good analog for early Earth microbial ecosystems. Hydrogen concentrations in the photic zone of the mat can be three orders of magnitude or more higher than in the photic zone, which are, in turn, an order of magnitude higher than in the unconsolidated sediments underlying the mat community. Within the photic zone, hydrogen concentrations can fluctuate dramatically during the diel (24 hour day-night) cycle, ranging from less than 0.001% during the day to nearly 10% at night. The resultant nighttime flux of hydrogen from the mat to the environment was up to 17% of the daytime oxygen flux. The daily pattern observed is highly dependent on cyanobacterial species composition within the mat, with Lyngbya-dominated systems having a much greater dynamic range than those dominated by Microcoleus; this may relate largely to differing degrees of nitrogen-fixing and fermentative activity in the two mats. The greatest H2 concentrations and fluxes were observed in the absence of oxygen, suggesting an important potential feedback control in the context of the evolution of atmospheric composition. The impact of adding this highly dynamic photosynthetic term to the hydrogen economy of early microbial ecosystems must have been substantial. From an evolutionary standpoint, the H2 generated in mats could have represented a very important new source of electrons and energy - but one that could not be harnessed without substantial adaptation to the highly variable chemistry of the mat surface. In addition, the emergent chemistry of anaerobic communities is often highly dependent on ambient hydrogen concentrations, so that incorporation of these communities into photosynthetic mats could have significantly affected the composition and flux of reduced "biosignature' gases to the environment.

Hoehler, Tori M.↗

Modular multi-interface nanocrystals for enhanced ethanol oxidation electrocatalysis

Electrochemical processes that utilize biomass-derived ethanol as a source of electrons and protons offer a sustainable energy strategy, yet their practical implementation is limited by sluggish ethanol oxidation reaction (EOR) kinetics and catalyst poisoning. Here, in this study, we report a modular multi-interface nanocrystal catalyst comprising core/shell Co 2 P/Pd and Pd-Au heterostructured interfaces that exhibit complementary functions for the enhanced EOR catalysis. The Co 2 P/Pd interface boosts Pd atom utilization and lowers the kinetic barriers for ethanol-to-acetate conversion, while the Pd-Au interface effectively alleviates CO poisoning caused by C–C bond cleavage of ethanol. In-depth analyses using in situ attenuated total reflectance-surface-enhanced infrared absorption spectroscopy, differential electrochemical mass spectrometry, and density functional theory calculations elucidate the mechanistic roles of these interfaces. The optimized Co 2 P/Pd-Au 0.08 nanorods achieve an excellent mass activity, underscoring the potential of modular, multi-interface nanocrystals for advancing EOR catalysis and offering a generalizable strategy for broader catalytic innovations.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

On ultrafast x-ray scattering methods for magnetism

With the introduction of x-ray free electron laser sources around the world, new scientific approaches for visualizing matter at fundamental length and time-scales have become possible. As it relates to magnetism and ‘magnetic-type’ systems, advanced methods are being developed for studying ultrafast magnetic responses on the time-scales at which they occur. We describe three capabilities which have the potential to seed new directions in this area and present original results from each: pump-probe x-ray scattering with low energy excitation, x-ray photon fluctuation spectroscopy, and ultrafast diffuse x-ray scattering. By combining these experimental techniques with advanced modeling together with machine learning, we describe how the combination of these domains allows for a new understanding in the field of magnetism. Finally, we give an outlook for future areas of investigation and the newly developed instruments which will take us there.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Search for sterile neutrinos in gallium experiments with artificial neutrino sources

The possibility of the BEST experiment on electron neutrino disappearance with intense artificial sources of electron neutrino {sup 51}Cr is considered. BEST has the great potential to search for transitions of active neutrinos to sterile states with Δm{sup 2} ∼ 1 eV{sup 2} and to set the limits on short baseline electron neutrino disappearance oscillation parameters. The possibility of the further constraints the oscillation parameters region with using {sup 65}Zn source is discussed.

07 ISOTOPE AND RADIATION SOURCES↗

Position-specific carbon isotope analysis of serine by gas chromatography/Orbitrap mass spectrometry, and an application to plant metabolism

Position-specific 13 C/ 12 C ratios within amino acids remain largely unexplored in environmental samples due to methodological limitations. We hypothesized that natural-abundance isotope patterns in serine may serve as a proxy for plant metabolic fluxes including photorespiration. Here we describe an Orbitrap method optimized for the position-specific carbon isotope analysis of serine to test our hypothesis and discuss the generalizability of this method to other amino acids. Position-specific carbon isotope ratios of serine were measured using a Thermo Scientific™ Q Exactive™ GC Orbitrap™. Amino acids were hydrolyzed from Arabidopsis biomass, purified from potential matrix interferences, and derivatized alongside standards. Derivatized serine (N,O-bis(trifluoroacetyl)methyl ester) was isolated using gas chromatography, trapped in a reservoir, and purged into the electron ionization source over tens of minutes, producing fragment ions containing different combinations of atoms from the serine-derivative molecule. The 13 C/ 12 C ratios of fragments with monoisotopic masses of 110.0217, 138.0166, and 165.0037 Da were monitored in the mass analyzer and used to calculate position-specific δ 13 C values relative to a working standard. This methodology constrains position-specific δ 13 C values for nanomole amounts of serine isolated from chemically complex mixtures. The δ 13 C values of fragment ions of serine were characterized with ≤1‰ precisions, leading to propagated standard errors of 0.7–5‰ for each carbon position. Position-specific δ 13 C values differed by up to ca 28 ± 5‰ between serine molecules hydrolyzed from plants grown under contrasting pCO 2 , selected to promote different fluxes through photosynthesis and photorespiration. The method was validated using pure serine standards characterized offline. Here this study presents the first Orbitrap-based measurements of natural-abundance, position-specific carbon isotope variation in an amino acid isolated from a biological matrix. We present a method for the precise characterization of isotope ratios in serine and propose applications probing metabolism in plants. We discuss the potential for extending these approaches to other amino acids, paving the way for novel applications.

59 BASIC BIOLOGICAL SCIENCES↗