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At least 181 records · Page 10

CO2 DIAL sensitivity studies for measurements of atmospheric trace gases

An analysis is presented of the accuracy of infrared differential absorption lidar (DIAL) measurements of trace constituents in the atmosphere. Expressions are derived for the signal-to-noise ratios applicable in the detection of a signal from a scattering cell for the cases of single-detection heterodyne detection and direct detection. Results of computer simulations of the expectation value of the measured return for various measurement conditions are presented which illustrate the sensitivities of plume measurements for horizontal range-resolved and vertical content measurements of NH3 in heterodyne and direct detection. Advantages for long-range measurements of the use of rare isotope laser frequencies, tuning by collision broadening, and closely spaced on and off frequencies are pointed out.

Brockman, P.↗

Dust in the Solar System - Properties and Origins

Interplanetary dust pervades the inner Solar System, giving rise to a prominent glow above the horizon at sunrise and sunset known as the zodiacal light. This dust derives from the disintegration of comets as they approach the Sun and from collisions among main-belt asteroids. The Earth accretes roughly 4x10(exp 6) kg/year of 1 - 1,000 micron dust particles as they spiral into the Sun under the influence of Poynting-Robertson drag and solar wind drag. Samples of these grains have been collected from deep sea sediments, Antarctic ice and by high-altitude aircraft and balloon flights. Interplanetary dust particles (IDPs) collected in the stratosphere have been classified by their IR spectra into olivine, pyroxene, and hydrated silicate-dominated classes. Most IDPs have bulk major and minor element abundances that are similar to carbonaceous chondrite meteorites. Hydrated silicate-rich IDPs are thought to derive from asteroids based on their mineralogy and low atmospheric entry velocities estimated from peak temperatures reached during atmospheric entry. Anhydrous IDPs are typically aggregates of 0.1 - approx. 1 micron Mg-rich olivine and pyroxene, amorphous silicates (GEMS), Fe, Nisulfides and rare spinel and oxides bound together by carbonaceous material. These IDPs are often argued to derive from comets based on compositional similarities and high atmospheric entry velocities that imply high eccentricity orbits. Infrared spectra obtained from anhydrous IDPs closely match remote IR spectra obtained from comets. The most primitive (anhydrous) IDPs appear to have escaped the parent-body thermal and aqueous alteration that has affected meteorites. These samples thus consist entirely of grains that formed in the ancient solar nebula and pre-solar interstellar and circumstellar environments. Isotopic studies of IDPs have identified silicate stardust grains that formed in the outflows of red giant and asymptotic giant branch stars and supernovae]. These stardust grains include both amorphous and crystalline silicates. The organic matter in these samples also exhibits highly anomalous H, C, and N isotopic compositions that are consistent with formation in low temperature environments at the outermost regions of the solar nebula or presolar cold molecular cloud. The scientific frontiers for these samples include working toward a better understanding of the origins of the solar system amorphous and crystalline grains in IDPs and the very challenging task of determining the chemical composition of sub-micron organic grains. Laboratory studies of ancient and present-day dust in the Solar System thus reveal in exquisite detail the chemistry, mineralogy and isotopic properties of materials that derive from a range of astrophysical environments. These studies are an important complement to astronomical observations that help to place the laboratory observations into broader context.

Messenger, Scott↗

Resonance Ionization Spectroscopy Experiment at Facility for Rare Isotope Beams

This manuscript reports on the commissioning of the Resonance Ionization Spectroscopy Experiment (RISE) at the BEam COoler and LAser spectroscopy (BECOLA) facility at Facility for Rare Isotope Beams (FRIB). The instrument implements the collinear resonance ionization spectroscopy technique for sensitive measurements of isotope shifts and hyperfine structure of short-lived isotopes produced at FRIB. The existing BECOLA beamline was extended to integrate an electrostatic ion-beam bender and an ion detector at ultrahigh vacuum. An injection-seeded titanium-sapphire laser and a multiharmonic pulsed neodymium-doped yttrium aluminum garnet laser were installed to perform resonant excitation and selective ionization. Commissioning tests were performed to demonstrate the capabilities of the instrument by measuring the hyperfine structure of stable 27 Al produced in an offline ion source. The RISE instrument is ready and operational for future studies of short-lived isotopes at FRIB.

Atomic spectra↗

Adsorption Studies of Dilute Krypton and Xenon from Nitrogen on SBMOF-1 and Activated Charcoal for Applications in Isotope Harvesting

Adsorptive partitioning of dilute krypton (Kr) and xenon (Xe) onto Stony Brook Metal–Organic Framework (SBMOF-1) and activated charcoal (AC) from carrier nitrogen was experimentally measured at temperatures ranging from 195 to 293 K. For this purpose, a closed-loop system for gas adsorption experiments was developed. From the Kr adsorption measurements, the adsorption equilibrium constant for Kr on SBMOF-1 was calculated, yielding a value for the enthalpy of adsorption of −19 ± 1 kJ·mol –1 . The partition coefficients were utilized to estimate the extraction rates of 76 Kr, 77 Kr, and 122 Xe isotopes during isotope harvesting at the Facility for Rare Isotope Beams (FRIB). We conclude that both materials showed promising results for the extraction of noble gases from FRIB effluents using temperature swing adsorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Landscape of pear-shaped even-even nuclei

The phenomenon of reflection-asymmetric nuclear shapes is relevant to nuclear stability, nuclear spectroscopy, nuclear decays and fission, and the search for new physics beyond the standard model. Global surveys of ground-state octupole deformation, performed with a limited number of models, suggest that the number of pear-shaped isotopes is fairly limited across the nuclear landscape. Here, we carry out a global analysis of ground-state octupole deformations for particle-bound even-even nuclei with Z ≤ 110 and N ≤ 210 using nuclear density functional theory (DFT) with several nonrelativistic and covariant energy density functionals. In this way, we can identify the best candidates for reflection-asymmetric shapes. The calculations are performed in the frameworks of axial reflection-asymmetric Hartree-Fock-Bogoliubov theory and relativistic Hartree-Bogoliubov theory using DFT solvers employing harmonic oscillator basis expansion. We consider five Skyrme and four covariant energy density functionals. We predict several regions of ground-state octupole deformation. In addition to the “traditional” regions of neutron-deficient actinide nuclei around 224 Ra and neutron-rich lanthanides around 146 Ba, we identified vast regions of reflection-asymmetric shapes in very neutron-rich nuclei around 200 Gd and 288 Pu, as well as in several nuclei around 112 Ba. Our analysis suggests several promising candidates with stable ground-state octupole deformation, primarily in the neutron-deficient actinide region, that can be reached experimentally. Detailed comparison between Skyrme and covariant models is performed. Octupole shapes predicted in this study are consistent with the current experimental information. This work can serve as the starting point of a systematic search for parity doublets in odd-mass and odd-odd nuclei, which will be of interest in the context of new physics searches.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Variations in the HCN/HNC abundance ratio in the Orion molecular cloud

Observations of the rare isotopes of HCN and HNC have been used to determine the relative abundance of these two chemical isomers along the central ridge of the Orion molecular cloud. The abundance ratio HCN/HNC decreases by more than an order of magnitude from the relatively warm plateau and hot core sources toward the KL nebula to the colder, more quiescent clouds to the north and south. Even in the cooler regions, however, the ratio is an order of magnitude larger than that found in previous investigations of cold dark clouds. The kinetic temperature in the regions studied is determined from new observations of methylacetylene (CH3CCH), together with other recent estimates of the gas temperature near KL. The results suggest that the warmer portions of the cloud are dominated by different chemical pathways that those in the general instellar cloud material.

Goldsmith, Paul F.↗

NdPO 4 solubility and aqueous Neodymium speciation in supercritical fluids: An experimental study at 500–700 °C and 1.7 kbar

A key aspect in the formation of rare earth elements (REE) deposits is the role of REE transport as aqueous REE complexes in supercritical hydrothermal solutions, where the nature of the aqueous complex is controlled by solution composition, temperature and pressure. Despite chloride being considered as one of the most abundant transporting ligands in magmatic-hydrothermal fluids, experimental investigations on the stability of aqueous REE chloride complexes are scarce above 300 °C. In this study, synthetic NdPO 4 crystals were reacted with non-saline and saline (0, 0.05 and 0.5 mNaCl), acidic (0.01 mHCl) aqueous solutions in a series of solubility experiments conducted at 500–700 °C and 1.7 kbar, where the solubilities were determined using a stable Nd isotope ( 145 Nd isotope spike) dilution technique. NdPO 4 solubility ranges between 28 ppm and 10,858 ppm, where solubility increases with both temperature and salinity. At 500 °C, log mNdPO 4 increases from –3.93 to –1.60 and there is a strong correlation between NdPO 4 solubility and NaCl concentrations (slope of 1.2 ± 0.3), indicating stabilization of the Nd chloride aqueous complexes with a stoichiometry corresponding to NdCl 2+ . At 600 °C, this correlation is weaker (slope of 0.4, log mNdPO 4 increases from –2.63 to –1.88) indicating the stabilization of both Nd chloride and hydroxyl species controlling solubility. At 700 °C, NdPO 4 solubility is largely independent of NaCl concentration indicating that solubility is controlled by Nd hydroxyl complexes, where stoichiometry suggests the neutral Nd(OH) 3 0 species is dominant. The solubility product (Ksp) of NdPO4 is derived from experimental data with the relation: log K sp = -41.81 – 0.057T – 20987/T, with T temperature in Kelvin. Comparison of the measured Nd phosphate solubility to thermodynamic predictions using the available Helgeson-Kirkham-Flowers equation of state parameters for aqueous Nd complexes indicate that predictions are up to three orders of magnitude lower compared to experimental observations. This discrepancy is most pronounced in saline solutions, suggesting that thermodynamic properties of the REE chloride species in supercritical fluids require revision. Numerical simulations of fluid-rock interaction between acidic, saline fluids and a Strange Lake felsic mineral assemblage demonstrates that NdPO 4 solubility predictions from models are four to six orders of magnitude lower than those calculated based on empirical fits from experiments, which suggests that acidic, saline fluids may play an important role in mobilizing large amounts of light REE from 450 to 700 °C.

58 GEOSCIENCES↗

Rare Potassium-Bearing Mica in Allan Hills 84001: Additional Constraints on Carbonate Formation

There have been presented several intriguing observations suggesting evidence of fossil life in martian orthopyroxenite ALH 84001. These exciting and controversial observations have stimulated extensive debate over the origin and history of ALH 84001, but many issues still remain unresolved. Among the most important is the question of the temperature at which the carbonates, which host the putative microfossils, formed. Oxygen- isotopic data, while showing that the carbonates are generally out of isotopic equilibria with the host rock, cannot constrain their temperature of formation. Both low- and high-temperature scenarios are plausible depending on whether carbonate growth occurred in an open or closed system. Petrographic arguments have generally been used to support a high-temperature origin but these appear to be suspect because they assume equilibrium between carbonate compositions that are not in contact. Some observations appear to be consistent with shock mobilization and growth from immiscible silicate-carbonate melts at high temperatures. Proponents of a low-temperature origin for the carbonates are hampered by the fact that there is currently no evidence of hydrous phases that would indicate low temperatures and the presence of a hydrous fluid during the formation of the carbonates. However, the absence of hydrous phases does not rule out carbonate formation at low temperatures, because the carbonate forming fluids may have been extremely CO2 rich, such that hydrous phases would not have been stabilized. In this study, I have carried out additional Transmission electron microscopy (TEM) studies of ALH-84001 and have found evidence of very rare phyllosilicates, which appear to be convincingly of pre-terrestrial origin. At present these observations are limited to one occurrence: further studies are in progress to determine if the phyllosilicates are more widespread.

Brearley, A. J.↗

R Coronae Borealis Star Evolution: Simulating 3D Merger Events to 1D Stellar Evolution Including Large-scale Nucleosynthesis

R Coronae Borealis (RCB) stars are rare hydrogen-deficient carbon-rich variable supergiants thought to be the result of dynamically unstable white dwarf mergers. In this article, we attempt to model RCB stars through all the relevant timescales by simulating a merger event in Octo-tiger, a 3D adaptive mesh refinement (AMR) hydrodynamics code, and mapping the post-merger object into MESA, a 1D stellar evolution code. We then post-process the nucleosynthesis on a much larger nuclear reaction network to study the enhancement of s-process elements. We present models that match observations or previous studies in most surface abundances, isotopic ratios, early evolution, and lifetimes. We also observe similar mixing behavior to previous modeling attempts that result in the partial He-burning products visible on the surface in observations. However, we do note that our subsolar models lack any enhancement in s-process elements, which we attribute to a lack of hydrogen in the envelope. We also find that the 16 O/ 18 O isotopic ratio is very sensitive to initial hydrogen abundance and increases outside of the acceptable range with a hydrogen mass fraction greater than 10 -4 .

79 ASTRONOMY AND ASTROPHYSICS↗

Modeling 238U/204Pb (μ) and Initial Pb of Lunar Meteorite Northwest Africa 12593

Apatite Ca 5 (PO 4 ) 3 (F, Cl, OH) serves as a valuable analytical resource. It is the only nominally hydrous phase on the moon and possesses the capacity to concentrate elements like U, Th, Pb, and rare earth elements (REE). This characteristic facilitates its use in U-Pb and Pb-Pb geochronology, allowing for the determination of the initial isotopic Pb and the -238 U/ -204 Pb ratio (μ) of the parent melt. In situ analysis of apatite grains can provide a detailed record of geochemical changes, revealing the broader petrogenetic and volatile history of the source material. This mineral is particularly informative in understanding the developmental history of its source. In situ analyses are crucial for lunar samples, predominantly composed of breccias, where correlating distinct grains with whole rock analyses poses challenges. This study utilizes in situ apatite isotopic analysis of apatite grains in lunar meteorite Northwest Africa 12593 and model the initial Pb isotopic composition and -238 U/ -204 Pb (μ) of the source. We present in situ Secondary Ionization Mass Spectrometry (SIMS) Pb-Pb analyses of 12 apatite grains in Northwest Africa (NWA) 12593 to test two hypotheses: 1) NWA 12593 clasts and matrix are closely related and from the same source, and 2) the matrix material previously documented as having a highland affinity has a lower modeled μ then KREEP.

K M Lehman Franco↗

Pristine nonmare rocks and the nature of the lunar crust

It is shown that the interdisciplinary study of the nonmare lunar rocks based on trace element, major element, and isotopic data plus petrographic evidence can succeed in amassing a large suite of demonstrably pristine rocks, and that the relative numbers of these rocks are not in accord with statistics amassed on soil fragments and glasses. The term 'pristine' is taken to mean rocks with primary compositions (albeit not necessarily textures) produced by lunar endogenous igneous processes. Melt rocks and crystalline matrix breccias produced by impact processes are excluded. A petrographic synonym for pristine would be 'unremelted, monomict'. It is found that anorthositic norites and noritic anorthosites were rare as primary nonmare rocks. Mechanical mixing appears to have been the dominant petrogenetic process on the highlands.

Warren, P. H.↗

Meteoritic parent bodies - Nature, number, size and relation to present-day asteroids

The relationship between meteoritic parent bodies and the present-day asteroids is discussed. Results on oxygen isotopic signatures and chemical distinctions among meteorite classes indicate that meteorites derive from a small number of parent bodies relative to the number of asteroids. The spectral properties of the ordinary chondrites and similar inclusions in meteoritic breccias differ from those of the abundant S asteroids (with no process known that can account for these differences); the closest spectral analogs of these chondrites are the rare near-earth Q-type asteroids. These facts lead to the question of why abundant meteorites have rare asteroidal analogs, while the abundant asteroids have rare meteoritic analogs. This question constitutes a prime topic for future studies.

Lipschutz, Michael E.↗

High-resolution spectroscopy of barium monofluoride: Odd isotopologues, hyperfine structure, and isotope shifts

Barium monofluoride (BaF) is a promising molecular species for precision tests of fundamental symmetries and interactions. We present a combined theoretical and experimental study of BaF spectra and isotope shifts, focusing in particular on the poorly understood odd isotopologues 137 BaF and 135 BaF. By comparing state-of-the-art ab initio calculations with high-resolution fluorescence and absorption spectroscopy data, we provide a benchmark for electronic structure theory and disentangle the hyperfine and rovibrational spectra of the five most abundant isotopologues, from 138 BaF to 134 BaF. The comprehensive knowledge gained enables a King plot analysis of the isotope shifts that reveals the odd-even staggering of the barium nuclear charge radii. It also paths the way for improved laser cooling of rare BaF isotopologues and crucially supports future measurements of nuclear anapole and Schiff moments.

Kogel, Felix [Univ. of Stuttgart (Germany)] (ORCID↗

Strangelove ocean at era boundaries, terrestrial or extraterrestrial cause

Negative perturbations in carbon-isotope value of calcite in pelagic sediments were found at times of biotic crisis, marking horizons which are, or were proposed as era boundaries: Cretaceous/Tertiary (K/T), Permian/Triassic (P/T), and Precambrian/Cambrian (PreC/C). The anomaly was also found at several other mass-extinction horizons, such as terminal Ordovician, Frasnian-Famenian, etc. Studies of K/T boundary indicate that only the planktic fraction of the sediments has the negative isotope anomaly, whereas the benthic fraction has the same value across the boundary. This geochemical signal is thus considered a record of strangelove ocean, or an ocean where isotope fractionation of dissolved carbonate ions in surface waters (by biotic function of planktic organisms) has been significantly reduced because of the drastic reduction of the biomass in the oceans. The reduction of marine biomass at each of the era boundaries was related to chemical pollution of the oceans as a consequence of a catastrophic event; a pH decrease of 0.5 could inhibit the fertility of planktons. Studies of earthquakes, volcanic eruptions, and meteorite-impact occurrences have indicated a linearly inverse log/log relationship between the magnitude and frequency of events. The frequency of era boundaries in geologic history supports the postulate that the rare events causing those biotic crises were large bolide-impacts.

Hsue, Kenneth J.↗

Rock-Sourced Nitrogen in Semi-Arid, Shale-Derived California Soils

Models suggest that rock-derived nitrogen (N) inputs are of global importance to ecosystem N budgets; however, field studies demonstrating the significance of rock N inputs are rare. We examined rock-derived N fluxes in soils derived from sedimentary rocks along a catena formed under a semi-arid climate. Our measurements demonstrate that there are distinct and traceable pools of N in the soil and bedrock and that the fraction of rock-derived N declines downslope along the catena. We used geochemical mass balance weathering flux measurements to estimate a rock-derived N flux of 0.145 to 0.896 kg ha -1 yr -1 at the ridgecrest. We also developed independent N flux estimates using a 15 N-based isotope mixing model. While geochemical mass-balance-based estimates fell within the 95% confidence range derived from the isotope mixing model (-1.1 to 44.3 kg ha -1 yr -1 ), this range was large due to uncertainty in values for atmospheric 15 N deposition. Along the catena, N isotopes suggest a diminishing effect of rock-derived N downslope. Overall, we found that despite relatively large N pools within the saprolite and bedrock, slow chemical weathering and landscape denudation limit the influence of rock-derived N, letting atmospheric N deposition (7.1 kg ha -1 yr -1 ) and N fixation (0.9-3.1 kg ha -1 yr -1 ) dominate N inputs to this grassland ecosystem.

54 ENVIRONMENTAL SCIENCES↗

The Effects of Experimentally Induced Zircon Annealing on Melt Inclusion-Zircon Geochemistry: A Case Study of Archean Zircon From the Barberton Complex

Crystalline melt inclusions (MIs) in Archean zircons can potentially constrain the evolution of magmatic processes. However, to obtain a homogeneous glassy MI representative of the parent melt, devitrified MIs must be heated at temperatures above the liquidus. Although, it is well known that radiation damaged domains in MI-host zircon undergo temperature-time dependent annealing, the effects of annealing on zircon stable isotope and trace element compositions has received less attention. In this study, we heated multiple aliquots of low-magnetism zircons with relatively low levels of radiation damage (Deff<9.6x1014 α-events/mg) from a 3.304 Ga tonalite gneiss xenolith from the Barberton greenstone belt (sample B87-18; Kamo and Davis, 1994) in an internally-heated pressure vessel at 0.4GPa and 1000–1200°C. Zircons were imaged by SEM (CL, BSE) to determine the zoning patterns around the MIs. The radiation damage preserved in the heated and unheated zircons was determined by measuring broadening of the 3(SiO4) Raman stretching band of zircon (FWHM). Oxygen isotope ratios (δ18O), OH/O ratios, and trace and rare earth element (TREE) concentrations were measured in the zircons and MIs using SIMS. The FWHM and Raman shift of the zircon 3(SiO4) band show a systematic increase of zircon crystallinity with increasing experimental temperature. Despite increasing crystallinity, the 3(SiO4) FWHM is not correlated with δ18O(Zrn) values in the heated or unheated zircons, suggesting that δ18O was not altered by laboratory heating in these low initial radiation damage zircons. FWHM and OH/O are positively correlated in both heated and unheated zircons. The unheated zircons have the largest FWHM and OH/O (OH/OMAX=3.5×10-4) suggesting that H2O was lost during experimental heating due to the progressive annealing of radiation-damaged domains in the zircons. Zircon TREE concentrations and FWHM values are not correlated despite the presence of TREE altered domains in both the heated and unheated zircons. Our results demonstrate that pre-experimental zircon TREE concentrations and δ18O(Zrn) remain intact during laboratory heating of crystalline MIs in zircon, while secondary H2O hosted in radiation damaged domains is partially lost. Thus, MIs in low initial radiation damage Archean zircon are a potentially viable tool for constraining melt compositions.

Joseph P. Gonzalez↗

Signal Processing and Calibration of Continuous-Wave Focused CO2 Doppler Lidars for Atmospheric Backscatter Measurement

Two continuous-wave(CW)focused C02 Doppler lidars (9.1 and 10.6 micrometers) were developed for airborne in situ aerosol backscatter measurements. The complex path of reliably calibrating these systems, with different signal processors, for accurate derivation of atmospheric backscatter coefficients is documented. Lidar calibration for absolute backscatter measurement for both lidars is based on range response over the lidar sample volume, not solely at focus. Both lidars were calibrated with a new technique using well-characterized aerosols as radiometric standard targets and related to conventional hard-target calibration. A digital signal processor (DSP), a surface acoustic and spectrum analyzer and manually tuned spectrum analyzer signal analyzers were used. The DSP signals were analyzed with an innovative method of correcting for systematic noise fluctuation; the noise statistics exhibit the chi-square distribution predicted by theory. System parametric studies and detailed calibration improved the accuracy of conversion from the measured signal-to-noise ratio to absolute backscatter. The minimum backscatter sensitivity is approximately 3 x 10(exp -12)/m/sr at 9.1 micrometers and approximately 9 x 10(exp -12)/m/sr at 10.6 micrometers. Sample measurements are shown for a flight over the remote Pacific Ocean in 1990 as part of the NASA Global Backscatter Experiment (GLOBE) survey missions, the first time to our knowledge that 9.1-10.6 micrometer lidar intercomparisons were made. Measurements at 9.1 micrometers, a potential wavelength for space-based lidar remote-sensing applications, are to our knowledge the first based on the rare isotope C-12 O(2)-18 gas.

Rothermel, Jeffry↗