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Nitrogen and xenon isotopic disequilibrium in Bachmut (L6) chondrule J2689 and matrix

Chondrule J2689, a large (8-mm) RP chondrule from Bachmut (L6) was previously found to be in disequilibrium with its host in a variety of features: (1) It has a fine-grained hornfelsic texture; (2) it contains low amounts of metal with a low-Ni taenite composition not found in the matrix; (3) the Ni/Co ratio of that metal is close to the solar ratio, which is equal to the bulk Ni/Co ratio (23) of the chondrule; (4) the bulk alkali content of the chondrule is high and the Na/K ratio is fractionated with respect to the average L chondrite ratio of 8; (5) Cr is depleted in spite of the high pyroxene content; (6) the siderophile elements are strongly depleted but are fractionated with their abundances increasing with volatility; and (7) the O isotopes of the chondrule and the host are out of equilibrium. However, the (Fe,Mg) silicates, feldspar, and chromite have chemical compositions indistinguishable from that of the host chondrite. We have studied a chip of the chondrite and of adjacent matrix by stepwise heating and by combustion in O for N and Xe isotopic abundances. (1) The chondrule preserved distinct bulk, metal, and O isotopic compositional features. It is therefore unlikely that the 'equilibration' of the major silicates Fe/Mg ratios could have taken place after accretion; (2) the chondrule was well equilibrated before break-up and exposure to cosmic rays; (3) two N signatures in the matrix also indicate that the matrix is not equilibrated; and (4) all data collected so far point toward the presence of unequilibrated Bachmut components. Very few reactions took place after accretion.

Kim, Y.↗

Isotopic Evidence for a Martian Regolith Component in Martian Meteorites

Noble gas measurements in gas-rich impact-melt (GRIM) glasses in EET79001 shergottite showed that their elemental and isotopic composition is similar to that of the Martian atmosphere [1-3]. The GRIM glasses contain large amounts of Martian atmospheric gases. Those measurements further suggested that the Kr isotopic composition of Martian atmosphere is approximately similar to that of solar Kr. The (80)Kr(sub n) - (80)Kr(sub M) mixing ratio in the Martian atmosphere reported here is approximately 3%. These neutron-capture reactions presumably occurred in the glass-precursor regolith materials containing Sm- and Br- bearing mineral phases near the EET79001/ Shergotty sites on Mars. The irradiated materials were mobilized into host rock voids either during shock-melting or possibly by earlier aeolian / fluvial activity.

Rao, M. N.↗

Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment (BIRDIE) (Final Report)

The Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment or BIRDIE was a precipitation collection campaign designed to measure cosmogenic isotopes of beryllium in rainfall and other forms of precipitation across the DOE Southern Great Plains (SGP) Atmospheric Radiation Measurement (ARM) site. Precipitation samples were collected over three weeks (May 21-June 10, 2022) at 11 SGP sites across a 120 km 2 domain in northern and central Oklahoma. The field campaign targeted summer-time convection rain events. We aimed to capture any spatial and/or temporal variability in the concentrations of beryllium-10 (10Be) and beryllium-7 (7Be) across the SGP ARM site during these rainfall events. The ratio of 10Be to 7Be (10/7Be) has been shown to be a powerful tracer for transport processes in the stratosphere-troposphere exchange (STE) system (e.g., Koch and Rind 1998). Any observed variability is analyzed to see if it could be linked to STE processes, including overshooting of deep convection clouds which penetrate the lower stratosphere. Six wet weather system events were collected within our three-week span. Five out of six of these rainfall events are classified as moderately to strongly convective. Those events are studied in more detail. The five systems also follow each other over a short time period of eleven days. In our rainfall samples we observed spatial and event variability in the concentrations of beryllium-10 and -7 which resulted in variability of 10/7 Be ratios. Each weather event appeared to exhibit a unique 10/7Be pattern across the domain that was not directly linked to storm total precipitation amount. To better understand the causes for this spatial variability, cloud characteristics in the domain were looked at to assess cloud type, cloud height and depth information. We also ran Hysplit back trajectories to identify possible air mass and moisture origins across our events. Detailed analysis is still on-going. The purpose of this technical report is to provide background on using cosmogenic isotopes as atmospheric tracers, describe the experimental design, and present the beryllium concentration and ratio data.

58 GEOSCIENCES↗

Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment (BIRDIE) (Field Campaign Report)

The Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment or BIRDIE was a precipitation collection campaign designed to measure cosmogenic isotopes of beryllium in rainfall and other forms of precipitation across the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) atmospheric observatory. Precipitation samples were collected over three weeks (May 21-June 10, 2022) at 11 SGP sites across a 120-km 2 domain in northern and central Oklahoma. The field campaign targeted summertime convection rain events. We aimed to capture any spatial and/or temporal variability in the concentrations of beryllium-10 (10Be) and beryllium-7 (7Be) across the ARM SGP site during these rainfall events. The ratio of 10Be to 7Be (10/7Be) has been shown to be a powerful tracer for transport processes in the stratosphere-troposphere exchange (STE) system (e.g., Koch and Rind 1998). Any observed variability is analyzed to see if it could be linked to STE processes, including overshooting of deep convection clouds that penetrate the lower stratosphere. Six wet weather system events were collected within our three-week span. Five out of six of these rainfall events are classified as moderately to strongly convective. Those events are studied in more detail. The five systems also follow each other over a short period of 11 days. In our rainfall samples we observed spatial and event variability in the concentrations of beryllium-10 and -7 that resulted in variability of 10/7Be ratios. Each weather event appeared to exhibit a unique 10/7Be pattern across the domain that was not directly linked to storm total precipitation amount. To better understand the causes for this spatial variability, cloud characteristics in the domain were looked at to assess cloud type, cloud height, and depth information. We also ran Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model back trajectories to identify possible air mass and moisture origins across our events. Detailed analysis is ongoing. The purpose of this technical report is to provide background on using cosmogenic isotopes as atmospheric tracers, describe the experimental design, and present the beryllium concentration and ratio data. Lastly, we note that BIRDIE coincided with two other deep convection field campaigns in the area: The National Aeronautics and Space Administration (NASA)’s Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) experiment (https://dcotss.org/) centered in Salina, Kansas, and the Targeted Observation by Radars and (uncrewed aerial systems) UAS of Supercells (TORUS) experiment (https://catalog.eol.ucar.edu/torus_2022) across the U.S. Central Plains. Additionally, a Lawrence Livermore National Laboratory ( LLNL) team at DCOTSS attempted to measure 10Be/7Be ratios on aerosols collected in situ in the lower and mid-stratosphere over Kansas using high-altitude balloons. Precipitation samples were also collected on the ground in Salina, Kansas.

54 ENVIRONMENTAL SCIENCES↗

Removal of Tc-99, Zr-95, and Nb-95, From Solutions Obtained After Dissolution of Irradiated Mo Targets

Decontamination of 99 Tc, Nb, and Zr impurities in dissolved irradiated Mo disks can be accomplished using Fe(II) precipitation. Here, we report bench-scale experiments and large-scale demonstrations on removal of 99 Tc (0.1 mM), 95 Nb, and 95 Zr from dissolved Mo disk simulant solutions. Tc removal is accomplished through the reduction and simultaneous immobilization of Tc(VII) by Fe(II), producing an insoluble, Tcincorporated Fe(II)-Fe(III) solid that is removed by filtration. Large-scale testing showed that Tc (97.6% ± 1.7%) is removed without affecting 99 Mo yields. Other important side reaction product impurities in irradiated Mo targets, namely various isotopes of Nb and Zr, are also removed (>99%) in this process. The effects of metal (Fe, Tc, Mo) concentrations, Fe(II)/Fe(III) ratio, pH, temperature, Fe addition method, and hydrogen peroxide addition were tested. The minimum amount of Fe(II) needed to remove up to 99% Tc is 10 mM and the optimal pH value for simultaneous removal of Tc, Nb, and Zr impurities is pH 13.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Review and Revalidation of Equivalency Factors in H-Canyon

In recent years, an effort has begun to validate and reaffirm long-existing limits and equivalency factors in use at the H-Canyon (HCA) facility located at the Savanah River Site. Equivalency factors (EF) are coefficients used to express the reactivity of a quantity of a given isotope in terms of an equivalent amount of another isotope’s reactivity, commonly termed Fissile Gram Equivalent (FGE). For criticality safety purposes, EFs are often used to conservatively determine if a given mixed-isotope system is within previously established limits. These EFs are calculated by taking ratios of established subcritical limits for a given system or process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

SPRUCE Sphagnum Phytobiome Responses to Whole Ecosystem Warming and Elevated Atmospheric CO2 in July, 2017-2021

This dataset reports the carbon (C) and nitrogen (N) isotopic composition of Sphagnum moss tissue collected from the Spruce and Peatland Responses Under Changing Environments (SPRUCE) experimental site within the Marcell Experimental Forest in northern Minnesota, USA. Tissues were collected inside the SPRUCE experimental study plot, where air and peat warming are combined in whole-ecosystem warming treatments, from 2019-2021. Additionally, rates of nitrogen fixation and methane oxidation measured for Sphagnum from 2017, 2019, and 2021. Sphagnum tissue % water content was measured at all timepoints. This dataset was used to conduct analyses within Petro et al (2023). Sphagnum C and N concentrations and 13C and 15N isotopic natural abundance were determined for three replicate Sphagnum tissue samples collected from inside the SPRUCE enclosures in July 2019-2021. Elemental and isotope analyses were conducted at the University of Georgia – Center for Applied Isotope Studies (CAIS; https://cais.uga.edu/). Plant elemental analysis was performed by the micro-Dumas method, while isotopic natural abundance was measured by isotope ratio mass spectrometry. 13C natural abundance is expressed as the per mille (‰) deviation from the Pee Dee Belemnite standard (PDB) 13C:12C ratio (δ13C), while 15N natural abundance is expressed as the ‰ deviation from the N2 atmospheric 15N:14N ratio (δ15N). Rates of nitrogen fixation and methane oxidation were measured using serum bottle incubations performed with Sphagnum collected inside the SPRUCE enclosures in July 2017, 2019, and 2021. Rates were calculated according to the amount of 15N-N2 or 13C-CH4 (methane) incorporated into the Sphagnum tissue or incubation headspace over the 48-hour intion period. In 2017, incubations were performed in growth chambers set to the temperature of the experimental plots during Sphagnum sampling. In 2019 and 2021, the incubations were performed directly inside the experimental plots. The 13C and 15N isotopic natural abundance data and rate measurements presented in this dataset provide insight into the impacts of whole-ecosystem warming and elevated atmospheric carbon dioxide (CO2) on N and C cycling within the Sphagnum phytobiome. This dataset contains two data files in comma-separate values (*.csv) format. Additional metadata are provided: two data dictionaries and a file-level metadata file in comma-separate values (.csv) format and a user guide in PDF (*.pdf) format. Additional datasets on NH4-N availability, porewater concentrations of CH4 and CO2, and Sphagnum groundcover within the SPRUCE experimental plots are available. These are outlined in the Related Datasets section in the user guide.

delta 13 carbon↗

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↗

The Interstellar Gas Experiment (IGE)

The Interstellar Gas Experiment (IGE) exposed thin metallic foils in order to collect neutral particles from the interstellar gas. These particles were entrapped in the foils along with precipitating magnetospheric and ambient atmospheric particles. Seven of these foils collected particles arriving from seven different directions as seen from the spacecraft for the entire duration of the Long Duration Exposure Facility (LDEF) mission. The authors' mass spectroscopy analysis of the noble gas component of these interstellar particles detected isotopes of helium and neon. These preliminary measurements suggest that the various isotopes are occurring in approximately the expected amounts and that their distribution in direction of arrival is close to what models predict. The analysis to subtract the background fluxes of magnetospheric and atmospheric particles is still in progress. The hope of this experiment is to investigate the noble gas isotopic ratios of this interstellar sample of matter which originated outside the solar system.

Lind, Don↗

Asymptotic Giant Branch stars as a source of short-lived radioactive nuclei in the solar nebula

We carried out a theoretical evaluation of the contribution of Asymptotic Giant Branch (AGB) stars to some short-lived (10(exp 6) less than or equal to Tau-bar less than or equal to 2 x 10(exp 7) yr) isotopes in the Interstellar Medium (ISM) and in the early solar system using stellar model calculations for thermally pulsing evolutionary phases of low-mass stars. The yields of s-process nuclei in the convective He-shell for different neutron exposures tau(sub 0) were obtained, and AGB stars were shown to produce several radioactive nuclei (especially Pd-107, Pb-205, Fe-60, Zr-93, Tc-99, Cs-135, and Hf-182) in diferent amounts. Assuming either contamination of the solar nebula from a single AGB star or models for continuous injection and mixing from many stars into the ISM, we calculate the ratios of radioactive to stable nuclei at the epoch of the Sun's formation. The dilution factor between the AGB ejecta and the early solar system matter is obtained by matching the observed Pd-107/Pd-108 and depends on the value of tau(sub 0). It is found that small masses M(sub He) of He-shell material (10(exp -4)-10(exp -7) solar mass) enriched in s-process nuclei are sufficient to contaminate 1 solar mass of the ISM to produce the Pd-107 found in the early solar system. Predictions are made for all of the other radioactive isotopes. The optimal model to explain several observed radioactive species at different states of the proto-solar nebula involves a single AGB star with a low neutron exposure (tau(sub 0) = 0.03 mbarn(sup -1)) which contaminated the cloud with a dilution factor of M(sub He)/solar mass approximately 1.5 x 10(exp -4). This will also contribute newly synthesized stable s-process nuclei in the amount of approximately 10(exp -4) of their abundances already present in the proto-solar cloud. Variations in the degree of homogenization (approximately 30%) of the injected material may account for some of the small general isotopic anomalies found in meteorites. It is also found that Fe-60 is produced in small but significant quantities that may be sufficient to explain the observations if the time elapsed delta from the contamination of the ISM to the formation of protoplanetary bodies is not higher than delta = 5 x 10(exp 6) yr. If delta is longer, up to 10 x 10(exp 6) yr, this would require the single AGB star to experience enhanced neutron densities (n(sub n) approximately 3 x 10(exp 9)n/cu cm) in the s-processing zone in order to compensate for the branching at Fe-59. The alternative model of long-term continuous ejection of matter from many AGB stars does not appear to match the observations. We also estimate the Al-26 production from the H-shell and find that the Al-26 abundance in the early solar system may be readily explained in a self-consistent manner. Moreover, Al-26 from AGB stars may contribute substantially to the galactic Al-26 gamma-source, while no significant gamma-flux from Co-60 (deriving from Fe-60 decay) is to be expected.

Wasserburg, G. J.↗

Silica-rich orthopyroxenite in the Bovedy chondrite

A large (greater than 4.5 x 7 x 4 mm), igneous-textured clast in the Bovedy (L3) chondrite is notable for its high bulk SiO2 content (is approximately equal to 57.5 wt%). The clast consists of normally zoned orthopyroxene (83.8 vol%), tridymite (6.2%), an intergrowth of feldspar (5.8%) and sodic glass (3.1%), pigeonite (1.0%), and small amounts of chromite (0.2%), augite, and Fe,Ni-metal; it is best described as a silica-rich orthopyroxenite. The oxygen-isotopic composition of the clast is similar, but not identical, to Bovedy and other ordinary chondrites. The clast has a superchondritic Si/Mg ratio, but has Mg/(Mg + Fe) and Fe/Mn ratios that are similar to ordinary chondrite silicate. The closest chemical analogues to the clast are radial-pyroxene chondrules, diogenites, pyroxene-silica objects in ordinary chondrites, and silicates in the IIE iron meteorite Weekeroo Station. The clast crystallized from a siliceous melt that cooled fast enough to prevent complete attainment of equilibrium but slow enough to allow nearly complete crystallization. The texture, form, size and composition of the clast suggestion that it is an igneous differentiate from an asteroid or planetesimal that formed in the vicinity of ordinary chondrites. The melt probably cooled in the near-surface region of the parent object. It appears that in the source region of the clast, metallic and silicate partial melt were largely-to-completely lost during a relatively low degree of melting, and that during a higher degree of melting, olivine and low-Ca pyroxene separated from the remaining liquid, which ultimately solidified to form the clast. While these fractionation steps could not have all occurred at the same temperature, they could have been accomplished in a single melting episode, possibly as a result of heating by radionuclides or by electromagnetic induction. Fractionated magmas can also account for other Si-rich objects in chondrites.

Ruzicka, Alex↗

Ambient Mass Spectrometry Rapid Analysis Methods for Trace Inorganics

The ability to rapidly detect and characterize the chemistry of trace quantities of inorganic species has multiple potential applications, including nuclear safeguards, nuclear forensics, and environmental monitoring. Some mass spectrometric methods currently exist, but they are costly and time-intensive, often destroying chemical information in the process of ionization. Ambient mass spectrometry is a relatively new analytical method in which samples are introduced to the mass spectrometer from atmospheric pressure, rather than from high vacuum. Ambient MS can operate with gentler ionization methods such as electrospray ionization (ESI) and paper-spray ionization (PSI), reducing fragmentation and preserving the chemical information of the analyte. This may be useful for determining the intended purpose of material in a sample. Strontium, part of nuclear fallout, is analyzed here to test these new analytical methods for viability. Electrospray ionization mass spectrometry functions by spraying the sample as a solution through a needle charged to a few kV. A nebulizing gas flows out along with the sample to create the spray before droplets enter a drying chamber with heated drying gas to remove the solvent molecules. From there bare analyte ions enter the mass spectrometer. This method has the advantage of relatively fast sample preparation and stable ionization. More stable ionization produces higher-quality data. Paper-spray ionization mass spectrometry operates by applying sample to a paper triangle. The paper triangle is then electrified in a metal clamp to a few kV before spray solvent is applied. The spray solvent transports analyte in the sample to the tip, where it is ionized and enters the mass spectrometer. One advantage of this method is reduced sample preparation - an analyst can even swipe a surface and cut a triangle directly from the swipe. The data analysis serves to rapidly process tens of samples all at once. The mass spectrometer outputs a file containing a few hundred spectra for each sample. The pipeline processes each one to identify peaks of interest. A full palette of data analysis metrics are generated, including plots of the raw data and plots of calculated values such as isotopic ratios. The pipeline filters the raw data to remove noise and background peaks, as well as peaks representing detector saturation. A heat map is generated to show the overall spectrum in mass-time- intensity space. Post-processing, we obtained the desired calibration curves, demonstrating that both ESI-MS and PSI-MS are viable methods for quantifying trace amounts of inorganics while retaining their chemical speciation information. ESI-MS demonstrated a linear response region of 100 ppb to 20 ppm, with a limit-of-detection of around 100 ppb. At top left is an example spectrum with the {sup 88}SrNO{sub 3} peak identified to show the retention of chemical speciation. PSI-MS showed a linear response region of around 1 ppb to 1 ppm, with a limit-of-detection of near 1 ppb. PSI-MS produced more erratic results than ESI-MS, likely due to the variability in ionization resulting from manual positioning of the paper triangle near the MS inlet. Future efforts will focus on improving the repeatability of PSI-MS as well as analyzing other species of interest such as cerium and uranium. Improvements will also be made to create more reliable data extraction and intelligent data filtering.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

First in-situ Nitrogen Isotope Measurements in Martian Meteorites

The origin and timing of the accretion of volatile elements on the terrestrial planets remains a subject of controversy. Nitrogen and hydrogen isotopes are powerful tools to constrain the source(s) of primordial volatiles accreted by planetary bodies because their isotope ratios (15N/14N; D/H) differ significantly between different solar system reservoirs (e.g., solar, chondritic, cometary). Hf-W data of martian samples indicate that Mars accreted very rapidly in the inner solar system and reached half ofits size in 1.8 Myr [1]. Therefore, martian samples are key to understand the distribution of volatile elements in the inner solar system during the early stages of planetary formation. Since no space missions have yet returned samples from Mars, martian meteorites (Shergottites, Nakhlites, Chassignites) are unique samples to constrain the source(s) of volatiles present in the martian mantle. The goal of this study was to target pristine phases(e.g., melt inclusions, mesostasis) for in-situ measurements of their nitrogen content and isotopic ratios to access the most primitive melt of the Chassignites and Nakhlites reservoirs. Five different Nakhlites (Nakhla, NWA 998, MIL 03346, Y 000593,NWA 6148) and Chassigny were analysed [2] using a recent high-resolution analytical technique that allows constraining the nitrogen composition of both carbon-bearing and carbon-free phases in natural and synthetic samples. Nitrogen was measured in the form of 14N16O- and 15N16O- with the CAMECA 1280-HR2 at the CRPG [3]. A significant amount of nitrogen was detected in melt inclusions in Chassigny and in the mesostasis of Nakhla, Y000593, MIL 03346, and NWA 6148. Nitrogen isotope signatures of Chassigny and Nakhlites exhibit a heavy isotope enrichment compared to Earth's mantle, and are consistent with a carbonaceous chondrite-like source [4]. This suggests that Earth and Mars accreted nitrogen from different chondritic sources. Overall, our in-situ technique is a unique and powerful tool to characterize the nitrogen abundance and isotopic composition of natural samples.

C Deligny↗

Relationships Between HED's, Mesosiderites, and Ungrouped Achondrites: Trace Element Analyses of Mesosiderite RKPA 79015 and Ungrouped Achondrite QUE 93148

Achondritic meteorites are a diverse group of meteorites that formed by igneous activity in asteroids. These meteorites can provide important information about early differentiation processes on asteroidal bodies. The howardite-eucrite-diogenite (HED) meteorites, the largest group of achondrites, are the only group of meteorites for which a potential parent body has been identified (4 Vesta) [e.g., 1]. Mesosiderites are stony-iron meteorites composed of roughly equal amounts of metal and silicates and silicates are broadly similar to HED meteorites [2]. They may have been formed by impact-mixing of crustal and core materials of differentiated meteorite parent bodies. Chemical and oxygen isotopic compositional data suggest that the HED meteorites and silicate portions of mesosiderites originated on the same or closely related parent bodies. Pallasites and IIIAB irons also have similar oxygen isotope compositions and have been thought to be related to the HEDs [3,4]. However, recent high resolution analyses have shown that pallasites and HED's have different oxygen isotopic values, but mesosiderites and HED s have the same isotope compositions implying a close connection [5]. QUE 93148 is a small (1.1g) olivine-rich (mg 86) achondrite that contains variable amounts of orthopyroxenene (mg 87) and kamacite (6.7 wt% Ni), with minor augite [6]. This meteorite was originally classified as a lodranite [7], but it s oxygen isotopic composition precludes a genetic relationship to the acapulcoites and lodranites. And also this meteorite has a lower Mn/Mg ratio than any major group of primitive or evolved achondrites and suggested that QUE 93148 may be a piece of the deep mantle of the HED parent body [6]. To better understand the relationship between HED s, mesosiderites and related achondrites, we have measured trace elements in the individual metallic and silicate phases. In this study, abundances of a suite of elements were measured for the unusual mesosiderite RKPA 79015 and a ungrouped achondrite QUE93148.

Righter, M.↗

Laser-induced fluorescence of filament-produced plasmas

Self-guided ultrafast laser filaments are a promising method for laser beam delivery and plasma generation for standoff and remote detection of elements and isotopes via filament-induced breakdown spectroscopy (FIBS). Yet, there are several challenges associated with the practical application of FIBS, including delivery of sufficient laser energy at the target for generating plasma with a copious amount of emission signals for obtaining a high signal-to-noise ratio. Here, in this study, we use laser-induced fluorescence (LIF) to boost the emission signal and reduce self-reversal in the spectral profiles. Ultrafast laser filaments were used to produce plasmas from an Al 6061 alloy target at various standoff distances from 1 to 10 m. For LIF emission enhancement, a narrow linewidth continuous-wave laser was used in resonance with a 394.40 nm Al I resonant transition, and the emission signal was monitored from the directly coupled transition at 396.15 nm. Emission signal features of Al I are significantly enhanced by resonant excitation. In addition, LIF of filament ablation plumes reduces the self-reversal features seen in the thermally excited spectral profiles. Time-resolved two-dimensional fluorescence spectroscopy was performed for evaluating the optical saturation effects, which are found to be non-negligible due to high Al atomic densities in the filament-produced plasmas.

47 OTHER INSTRUMENTATION↗

Stratospheric HBr mixing ratio obtained from far infrared emission spectra

Emission features of HBr isotopes have been identified in high-resolution FIR emission spectra obtained with a balloon-borne Fourier-transform spectrometer in the spring of 1979 at 32 deg N latitude. When six single-scan spectra at a zenith angle of 93.2 deg were averaged, two features of HBr isotopes at 50.054 and 50.069/cm were obtained with a signal-to-noise ratio of 2.5. The volume mixing ratio retrieved from the average spectrum is 2.0 x 10 to the -11th, which is assumed to be constant above 28 km, with an uncertainty of 35 percent. This stratospheric amount of HBr is about the same as the current level of tropospheric organic bromine compounds, 25 pptv. Thus HBr could be the major stratospheric bromine species.

Park, J. H.↗

The role of isotope mass on neutral fueling and density pedestal structure in the DIII-D tokamak

Abstract Experimental measurements on DIII-D of hydrogen neutral penetration lengths ( λ n 0 ) on the high field side (HFS) are longer by a factor of 2 than for deuterium consistent with the thermal velocity ratio for neutrals at the same temperature ( v t h H / v t h D = 2 ) . This ratio is constant for both low and high pedestal electron density. At low pedestal density ( n e ∼ 4 × 10 19 m − 3 ) , the neutral penetration length is greater than the density pedestal width for both isotopes, and the additional 40% increase of neutral penetration in hydrogen widens the pedestal by the same amount. As the density pedestal height increases ( n e ∼ 6 × 10 19 m − 3 ) , the neutral penetration lengths drop below the density pedestal widths for both isotopes, and the increased penetration of hydrogen has no increased effect on the pedestal width compared to deuterium. Extrapolating to future reactor-relevant high electron density pedestals, the isotope-mass change in neutral fueling on the HFS from the deepest neutral penetration of hydrogen, to the shortest neutral penetration of tritium will be negligible (0.2–0.4 cm) in comparison to estimates of the density pedestal width (6–8.5 cm).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Re-Os Isotopic Constraints on the Chemical Evolution and Differentiation of the Martian Mantle

The (187)Re-187Os isotopic systematics of SNC meteorites, thought to be from Mars, provide valuable information regarding the chemical processes that affected the Martian mantle, particularly with regard to the relative abundances of highly siderophile elements (HSE). Previously published data (Birck and Allegre 1994, Brandon et al. 2000), and new data obtained since these studies, indicate that the HSE and Os isotopic composition of the Martian mantle was primarily set in its earliest differentiation history. If so, then these meteorites provide key constraints on the processes that lead to variation in HSE observed in not only Mars, but also Earth, the Moon and other rocky bodies in the Solar System. Processes that likely have an effect on the HSE budgets of terrestrial mantles include core formation, magma ocean crystallization, development of juvenile crust, and the addition of a late veneer. Each of these processes will result in different HSE variation and the isotopic composition of mantle materials and mantle derived lavas. Two observations on the SNC data to present provide a framework for which to test the importance of each of these processes. First, the concentrations of Re and Os in SNC meteorites indicate that they are derived from a mantle that has similar concentrations to the Earth's mantle. Such an observation is consistent with a model where a chondritic late veneer replenished the Earth and Martian mantles subsequent to core formation on each planet. Alternative models to explain this observation do exist, but will require additional data to test the limitations of each. Second, Re-Os isotopic results from Brandon et al. (2000) and new data presented here, show that initial yos correlates with variations in the short-lived systems of (182)Hf- (182)W and (142)Sm-142Nd in the SNC meteorites (epsilon(sub W) and epsilon(sub 142Nd)). These systematics require an isolation of mantle reservoirs during the earliest differentiation history of Mars, and subsequent inefficient mixing between these reservoirs. These data show that models for the origin of isotopic variation for SNC meteorites require at least two long-lived mantle reservoirs, and possibly three. The range in the projected present day gamma(sub Os) of these reservoirs is from -5.4+/-2.6, to +4+/-1. The isotopic systematics of these reservoirs may be linked to development of cumulate crystal piles in a Martian magma ocean and variable amounts of late stage intercumulus melt. In this model, fractional crystallization of olivine and possibly other phases with slightly subchondritic Re/Os, from a solidifying magma ocean, resulted in a lower Re/Os ratio early cumulates, and a resultant low gamma(sub Os). Later cumulates or evolved melts crystallized with higher Re/Os ratios to produce the mantle reservoir(s) with consequent higher gamma(sub Os). Crystallization of the Martian magma ocean followed earliest core formation, as indicated by the correlation of epsilon(sub W) with epsilon(sub 142Nd) and initial gamma(sub Os).

Brandon, Alan D.↗