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At least 1,531 records · Page 85

Complete resolution across the neodymium/samarium isotopic envelope with a liquid sampling‐atmospheric pressure glow discharge — Orbitrap mass spectrometer

Rationale Nd and Sm isotope ratios play an important role in geological dating and as nuclear forensic signatures; however, the overlap of the respective 144, 148, 150 Nd/Sm isobars requires prior separations to be performed before analysis on typical MS platforms. The work presented here overcomes these isobaric interferences using ultrahigh‐mass resolution to alleviate interference without prior chemical separations. Methods A liquid sampling‐atmospheric pressure glow discharge ion source was coupled to a standard, QExactive Focus Orbitrap mass spectrometer, providing a mass resolution of ~80 k. A Spectroswiss FTMS booster X2 data acquisition package was used to collect extended transients, providing much higher mass resolution; ~230 k and ~600 k are employed here for Nd and Sm isotopes. Results While the standard Orbitrap resolution is far greater than typical “atomic” MS platforms, it was insufficient to alleviate all isobars. The use of a resolution of ~230 k resulted in baseline separation across the entire isotopic envelope for both Nd and Sm. Isotope ratios obtained from Nd:Sm mixtures using high‐resolution were equivalent to those found for individual‐element solutions, while isotope ratios obtained at a resolution of ~80 k (standard for the OEM data system) showed large deviations. Conclusions Use of ultrahigh‐resolution is an attractive alternative to extensive chemical separations to alleviate severe isobaric interferences. Sufficient mass resolution greatly reduces/eliminates the need for sample manipulations (separations) before analysis while reducing costs and total analysis times.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of proton-tagged, central (semi)exclusive production of high-mass lepton pairs in pp collisions at 13 TeV with the CMS-TOTEM precision proton spectrometer

The process pp → pℓ$^{+}$ℓ$^{−}$p$^{(*)}$, with ℓ$^{+}$ℓ$^{−}$ a muon or an electron pair produced at midrapidity with mass larger than 110 GeV, has been observed for the first time at the LHC in pp collisions at $ \sqrt{s}=13 $ TeV. One of the two scattered protons is measured in the CMS-TOTEM precision proton spectrometer (CT-PPS), which operated for the first time in 2016. The second proton either remains intact or is excited and then dissociates into a low-mass state p$^{*}$, which is undetected. The measurement is based on an integrated luminosity of 9.4 fb$^{−1}$ collected during standard, high-luminosity LHC operation. A total of 12 μ$^{+}$μ$^{−}$ and 8 e$^{+}$e$^{−}$ pairs with m(ℓ$^{+}$ℓ$^{−}$) > 110 GeV, and matching forward proton kinematics, are observed, with expected backgrounds of 1.49 ± 0.07 (stat) ± 0.53 (syst) and 2.36 ± 0.09 (stat) ± 0.47 (syst), respectively. This corresponds to an excess of more than five standard deviations over the expected background. The present result constitutes the first observation of proton-tagged γγ collisions at the electroweak scale. This measurement also demonstrates that CT-PPS performs according to the design specifications.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Compact Highly Sensitive Multi-species Airborne Mid-IR Spectrometer

We report on the development and airborne field deployment of a mid-IR laser based spectrometer. The instrument was configured for the simultaneous in-situ detection of formaldehyde (CH2O) and ethane (C2H6). Numerous mechanical, optical, electronic, and software improvements over a previous instrument design resulted in reliable highly sensitive airborne operation with long stability times yielding 90% airborne measurement coverage during the recent air quality study over the Colorado front range, FRAPPÉ 2014. Airborne detection sensitivities of ~ 15 pptv (C2H6) and ~40 pptv (CH2O) were generally obtained for 1 s of averaging for simultaneous detection.

Richter, Dirk↗

Development of a multidimensional gamma-spectrometer

A high-sensitivity multidimensional gamma-spectrometer is being developed within the shallow underground laboratory at Pacific Northwest National Laboratory (PNNL, USA). The system consists of two Broad Energy Germanium (BEGe) detectors, inside a low-background lead and copper shield, fitted with a cosmic veto background reduction system. The detector has advanced functionality, including operation in single or combined detector mode, with reductions in the cosmic background by 49.6% and Compton suppression of 6.5%. For selected radionuclides this provides an overall MDA improvement of 52.7%. Utilizing both detectors for simultaneous measurements of thermally irradiated highly enriched uranium (HEU) increased peak identification and reduced uncertainty by 27.6%. The design uses commercially off-the-shelf (COTS) components, for which the configuration is described, to provide a practical and powerful solution for low-level nuclear measurements.

Compton suppression↗

Preliminary investigation of an uncertainty budget for uranium isotope ratio analysis using a liquid sampling—atmospheric pressure glow discharge—orbitrap mass spectrometer system

The liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source has proven to be an effective analysis tool for making uranium isotope ratio measurements when coupled to high-resolution mass spectrometers, such as the Orbitrap. While previous studies have shown the capabilities of the LS-APGD for isotope ratio determination, a systematic evaluation of the measurement uncertainty of the technique has not been conducted. To this end, the International Standards Organizations (ISO) guidelines to the expression of uncertainty in measurement (GUM analysis) have been applied to generate an uncertainty budget. For this work, a preliminary assessment derived from the GUM analysis was performed. The uncertainty in the instrument blank determination has been identified as a primary factor contributing to measurement uncertainty for the LS-APGD-Orbitrap method. These findings for the specific test case of uranium isotopic analysis will be invaluable in applications across the breadth of isotope ratio mass spectrometry performed on this unique instrumental platform.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

GeMini: A High-Resolution, Low-Resource, Gamma-Ray Spectrometer for Planetary Science Applications

GeMini is a high-resolution gamma-ray spectrometer designed for planetary-science exploration. GeMini serves as the basis for instruments being flown on three upcoming deep-space missions: NASA’s mission to the M-class asteroid (16) Psyche, the Japan Aerospace Exploration Agency sample-return mission to the moons of Mars, and NASA’s Dragonfly mission that will land on Saturn’s largest moon, Titan. These science missions require high-resolution spectroscopy in a low-power, low-mass, rugged design that can survive in a variety of environments. GeMini addresses these needs by providing a cryogenically cooled crystal of high-purity germanium that can operate with as little as 10 to 20 watts, depending on the implementation and mission, and has a mass of less than 2 kg. GeMini helps determine the elemental composition of planetary bodies by measuring gamma rays emitted from the surface. This paper describes the mechanical, thermal, and electrical design of GeMini as well as its performance. Further, it describes testing that was performed to validate the design with respect to launch loads and radiation damage. Although the basic design of GeMini is common to all three missions, each planetary body has unique environmental conditions and mission specifications. This paper concludes by describing these upcoming missions and how GeMini is customized for each.

79 ASTRONOMY AND ASTROPHYSICS↗

The Magnetic Electron Ion Spectrometer: A Review of On-Orbit Sensor Performance, Data, Operations, and Science

Measurements from NASA’s Van Allen Probes have transformed our understanding of the dynamics of Earth’s geomagnetically-trapped, charged particle radiation. The Van Allen Probes were equipped with the Magnetic Electron Ion Spectrometers (MagEIS) that measured energetic and relativistic electrons, along with energetic ions, in the radiation belts. Accurate and routine measurement of these particles was of fundamental importance towards achieving the scientific goals of the mission. We provide a comprehensive review of the MagEIS suite’s on-orbit performance, operation, and data products, along with a summary of scientific results. The purpose of this review is to serve as a complement to the MagEIS instrument paper, which was largely completed before flight and thus focused on pre-flight design and performance characteristics. As is the case with all space-borne instrumentation, the anticipated sensor performance was found to be different once on orbit. Our intention is to provide sufficient detail on the MagEIS instruments so that future generations of researchers can understand the subtleties of the sensors, profit from these unique measurements, and continue to unlock the mysteries of the near-Earth space radiation environment.

47 OTHER INSTRUMENTATION↗

UV–Vis Photodissociation Action Spectroscopy on Thermo LTQ-XL ETD and Bruker amaZon Ion Trap Mass Spectrometers: a Practical Guide

We report automated procedures for multiple tandem mass spectra acquisition allowing UV–Vis photodissociation action spectroscopy measurements of ions and radicals. The procedures were developed for two commercial ion trap mass spectrometers and applied to collision-induced and electron–transfer dissociation tandem mass spectrometry modes of ion generation. .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Analysis of passivated A-286 stainless steel surfaces for mass spectrometer inlet systems by Auger electron and X-ray photoelectron spectroscopy and scanning electron microscopy

In this study, various commercially available surface treatments are being explored for use on stainless steel components in mass spectrometer inlet systems. Type A-286 stainless steel coupons, approximately 12.5 mm in diameter and 3 mm thick, were passivated with one of five different surface treatments; an untreated coupon served as a control. The surface and near-surface microstructure and chemistry of the coupons were investigated using sputter depth profiling using Auger electron spectroscopy, x-ray photoelectron spectroscopy, and scanning electron microscopy (SEM). All the surface treatments studied appeared to change the surface morphology dramatically, as evidenced by lack of tool marks on the treated samples in SEM images. In terms of the passivation treatment, Vendors A-D appeared to have oxide layers that were very similar in thickness to each other (0.7–0.9 nm thick), as well as to the untreated samples (the untreated sample oxide layers appeared to be somewhat larger). Vendor E’s silicon coating appears to be on the order of 200 nm thick.

36 MATERIALS SCIENCE↗

Combining selection valve and mixing chamber for nanoflow gradient generation: Toward developing a liquid chromatography cartridge coupled with mass spectrometer for protein and peptide analysis

In relation to developing a micro HPLC cartridge, we have recently built a high-pressure electroosmotic pump (EOP). However, we do not recommend people to use this pump to deliver an organic solvent directly, because it often makes the pump rate unstable. We have experimented several approaches to address this issue, but none of them are satisfactory. Here, we develop an innovative approach to address this issue. We first create an abruption (a dead-volume) within a fluid conduit. We then utilize an EOP to withdraw, via a selection valve, a train of eluent solutions having decreasing eluting power into the fluid conduit. When these solutions are further aspirated through the dead-volume, these solutions are partially mixed, smoothening concentration transitions between two adjacent eluent solutions. As these solutions are pushed back, through the dead-volume again, a smooth gradient profile is formed. In this work, we characterize this scheme for gradient formation, and we incorporate this approach with a high-pressure EOP, a nanoliter injection valve, and a capillary column, yielding a micro HPLC system. Lastly, we then couple this micro HPLC with an electrospray ionization – mass spectrometer for peptide and protein separations and identifications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Upgrade of the mechanically pumped CO 2 two-phase cooling system for the alpha magnetic spectrometer on the international space station

This study describes the successful upgrade of a mechanically pumped CO 2 two-phase cooling system in space by designing a new pump module for the Alpha Magnetic Spectrometer-02 on the International Space Station. Key factors for mission success are emphasized, including achieving high coolant filling accuracy within 10% of the target and maintaining system stability within ±1 °C. The impact of adding radiators to improve cooling efficiency is examined, and it is found that operating multi-radiators out-of-phase does not significantly affect system reliability. The centrifugal pump design is shown to allow for better lubricant circulation, while the in-house designed controller incorporates protective measures to prevent cavitation, overheating, and over-current. Further, this research advances the understanding of circulation loop systems and their upgrades in space and demonstrates the potential for extending the lifetime of space-borne mechanically pumped two-phase cooling systems.

42 ENGINEERING↗

New and Extended Data Processing of Mars Odyssey Neutron Spectrometer Data

The Los Alamos National Laboratory designed and built Mars Odyssey Neutron Spectrometer (MONS) has been operating and collecting data from February 2002 to the present. MONS measures the neutron leakage albedo from galactic cosmic ray bombardment of Mars. These signals can indicate the presence of near-surface water deposits on Mars, and can also be used to study properties of the seasonal polar CO 2 ice caps. This work outlines a new analysis of the MONS data that results in new and extended time-series maps of MONS thermal and epithermal neutron data. The new data are compared to previous publications on the MONS instrument. We then present preliminary results studying the inter-annual variability in the polar regions of Mars based on 8 Mars-Years of MONS data from the new dataset.

79 ASTRONOMY AND ASTROPHYSICS↗

Development towards stable chlorine isotope measurements of astromaterials using the modified Middleton source of an accelerator mass spectrometer

The volatile element Cl can be lost during the formation and evolution of planetary bodies, leading to fractionation of its two stable isotopes 35 Cl and 37 Cl. Chlorine isotope variations (reported as δ 37 Cl in parts per thousand (‰) relative to Standard Mean Ocean Chloride, SMOC) are documented to exceed 80‰ between different lunar rock samples and have been variably interpreted as the fingerprint of degassing during accretion, magma ocean, or volcanic portions of lunar history. The large intersample and intrasample variations observed by both bulk isotope ratio mass spectrometry (IRMS) and in-situ secondary ion mass spectrometry (SIMS) methods are difficult to interpret in part because of a paucity of bulk Cl isotope measurements. This lack of high-precision bulk data is due to the relative rarity of IRMS laboratories capable of making these high precision measurements on small samples of precious planetary materials such as those returned by human or robotic exploration. Here we present a new method for performing high precision δ 37 Cl measurements using the modified Middleton ion source of an existing accelerator mass spectrometer. For samples with as little as 1 μg Cl–the equivalent of 2–4 mm 3 of a typical lunar rock sample–the average cathode accuracy is ~1‰. Finally, cathode reproducibility is typically ~1‰ (2σ) for samples with at least 10 μg of Cl, increasing to ~3–6‰ for aliquots with ~1–2 μg Cl, similar to published SIMS results and sufficient to study astromaterials from the Moon, Mars, or 4 Vesta, which have tens of ‰ observed variations.

07 ISOTOPE AND RADIATION SOURCES↗

Parametric optimization of the liquid sampling-atmospheric pressure glow discharge ionization source coupled to an Orbitrap mass spectrometer for neodymium isotope ratio determinations

Isotope ratio determinations are a valuable tool in several application areas. In nuclear forensics, the isotope ratios of uranium and plutonium are commonly used as a signature for the nuclear material's provenance and processing history. However, signatures from other coexisting elements, such as neodymium and samarium, can offer additional insights. Here, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source coupled to an Orbitrap mass spectrometer (MS) has demonstrated its utility for actinide measurements. This instrumental platform can leverage the high resolution offered by the Orbitrap MS to overcome potential isobaric interferences, such as 144 Nd- 144 Sm, 148 Nd- 148 Sm, and 150 Nd- 150 Sm pairs. The work presented herein demonstrates the rapid, accurate, and precise determination of the isotope ratios for neodymium using the LS-APGD/Orbitrap MS. Both the LS-APGD and Orbitrap MS parameters were optimized systematically, with NdO + found to be the most abundant, most reduced species after applying the optimal collision-induced dissociation modalities. A limit of detection of 3 pg of 142 Nd was achieved when data was acquired and processed using the FTMS Booster, an external data acquisition and processing system offered by Spectroswiss. Excellent accuracy of better than 99 % and precision of <1 % RSD were achieved when a solution of the well-characterized neodymium standard (JNdi-1 standard) was analyzed under the optimized condition, indicating the LS-APGD/Orbitrap's great potential for isotope ratio analysis of Nd and other REEs for diverse applications.

47 OTHER INSTRUMENTATION↗

Rapid measurement of sub-micrometer aerosol size distribution using a fast integrated mobility spectrometer

We present rapid measurement of submicron particle size distributions enables the characterization of aerosols with fast changing properties, and is often necessary for measurements onboard mobile platforms (e.g., research aircraft). Aerosol mobility size distribution is commonly measured by a scanning mobility particle sizer (SMPS), which relies on voltage scanning or stepping to classify particles of different sizes, and may take up to several minutes to obtain a complete size spectrum of aerosol particles. The recently developed fast integrated mobility spectrometer (FIMS) with enhanced dynamic size range classifies and detects particles from 10 to ~600 nm simultaneously, allowing submicron aerosol mobility size distributions to be captured at a time resolution of 1 second. In this study, we present a detailed data inversion routine for deriving aerosol size distribution from FIMS measurements. The inversion routine takes into consideration the FIMS transfer function, particle penetration efficiency in the FIMS, and multiple charging of aerosols. The accuracy of the FIMS measurement is demonstrated by comparing parallel FIMS and SMPS measurements of stable aerosols with a wide range of size spectrum shapes, including ambient aerosols and aerosols classified by a differential mobility analyzer (DMA). The FIMS and SMPS-derived size distributions show excellent agreements for all aerosols tested. In addition, total number concentrations of ambient aerosols were integrated from 1 Hz FIMS size distributions, and compared with those directly measured by a condensation particle counter (CPC) operated in parallel. Finally, the integrated and measured total particle concentrations agree well within 5%.

54 ENVIRONMENTAL SCIENCES↗

First Results from the Modular Total Absorption Spectrometer at the HRIBF

A Modular Total Absorption Spectrometer constructed at the Holifield Radioactive Ion Beam Facility has been applied to decay studies of over 20 {sup 238}U fission products. The measurements were focused on nuclei identified as important for decay heat analysis during a nuclear fuel cycle. Preliminary results on the average electromagnetic (EM) energy release in the β decay of {sup 89}Kr and {sup 139}Xe isotopes yielded values of 2446 keV and 1126 keV, respectively. It represents an increase of over 35% and 20%, respectively, when compared to the average EM energies deduced using the ENSDF database.

43 PARTICLE ACCELERATORS↗

An alpha–gamma coincidence spectrometer based on the Photon–Electron Rejecting Alpha Liquid Scintillation (PERALS®) system

Here, an alpha–gamma coincidence spectrometer has been developed for the measurement of selected actinide isotopes in the presence of high beta/gamma fields. The system is based on a PERALS® liquid scintillation counter for beta/alpha discrimination and was successfully tested with both high purity germanium and bismuth germanate, gamma-ray detectors using conventional analog electronics.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The nonlinear light output of NaI(Tl) detectors in the Modular Total Absorption Spectrometer

New detector array, the Modular Total Absorption Spectrometer (MTAS),was commissioned at the Holifield Radioactive Ion Beam Facility (HRIBF) at Oak Ridge National Lab(ORNL).Total absorption gamma spectra measured with MTAS are expected to improve beta-feeding patterns and beta strength functions in fission products.MTAS is constructed out of hexagonal NaI(Tl) detectors with a unique central module surrounded by 18 identical crystals assembled in three rings. The total NaI(Tl) mass of MTAS is over1000 kg.The response of the central and other 18 MTAS modules to -radiation was simulated using the GEANT4 tool kit modified to analyze the nonlinear light output of NaI(Tl).A detailed description oftheGEANT4modifications madeisdiscussed.SimulatedenergyresolutionofMTAS modules is found to agree well with the measurements for single transitions of 662keV (137Cs) with 8.2% full width half maximum (FWHM),835keV (54Mn) with FWHM of 7.5% FWHM, and 1115keV (65Zn) with FWHM of 6.5%.Simulations of single and multiple -rays from 60Co are also discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗