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NASA NTRS2018

Stable Isotope Fractionation in Titan Aerosol Formation

Stable isotope ratio measurements are a powerful tool used to understand both ancient and modern planetary processes. Instruments on the Cassini- Huygens spacecraft along with ground-based observations have measured several isotope pairs, including C-13/C-12 and N-15/N-14, in Titan's atmosphere. This includes isotopic measurements of the major atmospheric species, CH4 and N2, along with HCN, HC3N, C2H2. C2H6 and C4H2. However, the isotopic fractionation of Titan's organic aerosol has not conclusively been measured and therefore the effect of aerosol formation as an isotopic fractionation pathway in Titan's atmosphere has not been considered. Laboratory studies have measured the carbon and/or nitrogen isotopic fractionation of Titan aerosol analogs. [18] found that the carbon fractionation of photochemical organic aerosol analogs are more enriched in C-13. This enrichment in the aerosol analogs is opposite of what is predicted for photochemical products by the kinetic isotope effect. Additionally, both [16] and [18] found that the nitrogen fractionation in the organic aerosol analogs are opposite of what is observed in Titan's atmospheric N2 and HCN, with the aerosol analogs being a light nitrogen sink. Here we monitor the gas phase during photochemical aerosol analog production as a function of reaction time. In a recirculation experiment, the isotopic fractionation of carbon within the gas-phase products is measured as the CH4 reservoir is depleted. This allows us to monitor the isotopic fractionation pathway during photochemical aerosol analog formation.

Ugelow, M. S.↗
NASA NTRS1983

A measurement of the (C-12)O/(C-13)O) ratio in the mesosphere of Venus

Measurements of the absorptions in the Venus atmosphere by (C-12)O and (C-13)O in the J = 1-2 microwave, rotational transitions are reported. Radiative transfer models were fitted to the spectra in order to estimate the isotopic ratio (C-12)O/(C-13)O = 185. Based on an extensive error analysis it is suggested that the standard deviation of this value is + or - 69. This result applies to the mesosphere of Venus, i.e., from about 80 to 110 km. Values of the (C-12)O/(C-13)O ratio measured deeper in the Venus atmosphere are closer to the terrestrial value of 89. Several possible, qualitative mechanisms to explain the higher value of (C-12)O/(C-13)O found for the nightside mesosphere of Venus are offered.

Clancy, R. T.↗
NASA NTRS1982

Noble gases in planetary atmospheres - Implications for the origin and evolution of atmospheres

The radiogenic and primordial noble gas contents of the Venus, earth, and Mars atmospheres are compared with one another and with the noble gas content of other extraterrestrial samples, particularly meteorites. Key trends in the primordial noble gas content of terrestrial planetary atmospheres are shown to include: (1) a several-orders-of-magnitude decrease in Ne-20 and Ar-36 from Venus to earth to Mars; (2) a nearly constant Ne-20/Ar-36 ratio, which is comparable to that found in the more primitive carbonaceous chondrites and which is two orders of magnitude smaller than the solar ratio; (3) a sizable fractionation of Ar, Kr, and Xe from their solar ratios, though the degree of fractionation (especially for Ar-36/Xe-132) appears to decrease systematically from carbonaceous chondrites to Mars to earth to Venus; and (4) large differences in Ne and Xe isotopic ratios among earth, meteorites, and the sun. It is suggested that the grain-accretion hypothesis can explain all four trends, though the assumptions needed to achieve this agreement are far from proven.

Pollack, J. B.↗
NASA NTRS2013

What Are Space Exposure Histories Telling Us about CM Carbonaceous Chondrites?

Chondrites are chemically primitive and carbonaceous (C) chondrites are potentially the most primitive among them because they mostly escaped thermal metamor-phism that affected the other chondrite groups and ratios of their major, non-volatile and most of the volatile elements are similar to those of the Sun. Therefore, C chondrites are ex-pected to retain a good record of the origin and early history of the solar system. Carbonaceous chondrites are chemically differentiated from other chondrites by their high Mg/Si ratios and refractory elements, and have experienced various degrees of aqueous alteration. They are subdivided into eight subgroups (CI, CM, CO, CV, CK, CR, CB and CH) based on major element and oxygen isotopic ratios. Their elemental ratios spread over a wide range though those of ordinary and enstatite chondrites are relatively uniform. It is critical to know how many sepa-rate bodies are represented by the C chondrites. In this study, CM chondrites, the most abundant carbona-ceous chondrites, are examined. They are water-rich, chon-drule- and CAI-bearing meteorites and most of them are brec-cias. High-temperature components such as chondrules, iso-lated olivine and CAIs in CMs are frequently altered and some of them are replaced by clay minerals and surrounded by sul-fides whose Fe was derived from mafic silicates. On the basis of degrees of aqueous alteration, CMs have been classified into subtypes from 1 to 2, although Rubin et al. [1] assigned subtype 1 to subtype 2 and subtype 2 to subtype 2.6 using various petrologic properties. The classification is based on petrographic and mineralogic properties. For example, though tochilinite (2[(Fe, Mg, Cu, Ni[])S] 1.57-1.85 [(Mg, Fe, Ni, Al, Ca)(HH)2]) clumps are produced during aqueous alteration, they disappear and sulfide appears with increasing degrees of aqueous alteration. Cosmic-ray exposure (CRE) age measurements of CM chondrites reveal an unusual feature. Though CRE ages of other chondrite groups range from several Myr to tens of Myr, CMs exposure ages are not longer than 7 Myr with one-third of the CM having less than 1 Myr CRE age. For those CM chondrites that have CRE ages <1 Myr, there are two discern-able CRE peaks. Because a CRE age reflects how long a me-teorite is present as a separate body in space, the peaks pre-sumably represent collisional events on the parent body (ies) [2]. In this study we defined 4 distinct CRE age groups of CMs and systematically characterized the petrography in each of the 4 CRE age groups to determine whether the groups have significant petrographic differences, with such differences probably reflecting different parent body (asteroid) geological processing, or multiple original bodies.

Takenouchi, A.↗
NASA NTRS2014

On the Relationship between Cosmic Ray Exposure Ages and Petrography of CM Chondrites

Carbonaceous (C) chondrites are potentially the most primitive among chondrites because they mostly escaped thermal metamorphism that affected the other chondrite groups. C chondrites are chemically distinguished from other chondrites by their high Mg/Si ratios and refractory elements, and have experienced various degrees of aqueous alteration. They are subdivided into eight subgroups (CI, CM, CO, CV, CK, CR, CB and CH) based on major element and oxygen isotopic ratios. Their elemental ratios vary over a wide range, in contrast to those of ordinary and enstatite chondrites which are relatively uniform. It is critical to know how many separate bodies are represented by the C chondrites. In this study we defined 4 distinct cosmic-ray exposure (CRE) age groups of CMs and systematically characterized the petrography in each of the 4 CRE age groups to determine whether the groups have significant petrographic differences with such differences probably reflecting different parent body (asteroid) geological processing, or multiple original bodies. We have reported the results of a preliminary grouping at the NIPR Symp. in 2013 [3], however, we revised the grouping and here report our new results.

Takenouchi, A.↗
NASA NTRS2015

Investigation of Benthic Foraminiferal Non-Traditional Stable Isotopes to Reconstruct Methane Fluxes in Sedimentary Environments

Methane (CH4) is an important greenhouse gas, with a global warming potential much higher than carbon dioxide (CO2) on a short time scale. Even if the residence time of CH4 in the atmosphere is relatively short (tens of years), one of the products of CH4 oxidation is CO2, a greenhouse gas with a much longer residence time in the atmosphere (tens to hundreds of years). CH4 has been proposed as one of the trigger mechanisms for rapid global climate change today and in the geological past. With regards to the geological past, numerous studies proposed the benthic foraminiferal carbon isotope ratio (Delta13C) as a tool to reconstruct the impact of marine CH4 on rapid climate changes; however, the investigation of modern benthic foraminiferal Delta13C have produced inconclusive results. CH4 has a distinctive hydrogen isotope (Delta(D)) and Delta13C signature compared to seawater, and sulfate reduction, often coupled to CH4 anaerobic oxidation in sediments, changes the sulfur isotope signature (Delta34S) of the remaining sulfate in porewater. Therefore, we hypothesize that the Delta(D) and Delta34S signature of infaunal benthic foraminiferal species can provide a complementary approach to Delta13C to study CH4 dynamics in sedimentary environments. Here, we present the preliminary results obtained analyzing Uvigerina peregrina Delta(D) and Delta34S from three different locations at Hydrate Ridge, offshore Oregon. Unfortunately, the lack of chemical data related to the moment of foraminiferal calcification makes difficult to build a robust relationship among the U. peregrina stable isotopes and the CH4 fluxes at the sampling sites. However, our results look very promising, as each site is characterized by a different Delta(D) and Delta34S signature. We emphasize that this study represents the first step in the development of new proxies (Delta(D)) and Delta34S), which may complement the more traditional benthic foraminiferal Delta13C values, to reconstruct marine CH4 fluxes in the geological past.

Borrelli, C.↗
NASA NTRS2024

Precipitation -17 O-Excess Altered During Tropical Convection: Evidence From Monsoon Cold Surges in Singapore

Despite the recent recognition of -17 O-excess as a promising new tracer for hydrological processes, our knowledge of the control mechanisms underlying -17 O-excess in tropical regions remains limited. To understand how microphysical processes during tropical convection affect precipitation isotope ratios, particularly -17 O-excess, in Singapore, we collected precipitation samples at minute intervals from six rain events associated with cold surges during the Northeast Monsoon seasons and analyzed their triple oxygen isotopes. Our results show that precipitation δ -18 O decreases in the convective zones and then gradually increases in the stratiform zones, while d-excess exhibits an inverse trend. This correlation between δ -18 O and d-excess indicates that rain evaporation plays a crucial role in regulating precipitation isotopes. Moreover, the rain events with a higher upstream rainout amount have lower δ -18 O and higher -17 O-excess values, suggesting that precipitation δ -18 O and -17 O-excess likely reflect the integrated upstream convective activity. Microphysical processes associated with upstream convection, such as rain evaporation and vapor recycling, are potential mechanisms that increase -17 O-excess values along moisture transport pathways for a rain event, and hence, undermine the effectiveness of -17 O-excess as a tracer of moisture source humidity. Contrary to the negative correlation observed in monthly precipitation, there is generally a positive correlation between d-excess and -17 O-excess at the event scale. However, this correlation weakens as convective rain intensifies, suggesting that stronger convection can attenuate the positive correlation between d-excess and -17 O-excess. Therefore, it is crucial to consider how tropical convection alters -17 O-excess when utilizing this tracer to interpret atmospheric dynamics and hydrological processes.

tropical weather systems↗
NASA NTRS2010

Ground Based Observation of Isotopic Oxygen in the Martian Atmosphere Using Infrared Heterodyne Spectroscopy

Infrared heterodyne spectra of isotopic CO2 in the Martian atmosphere were obtained using the Goddard Heterodyne Instrument for Planetary Wind and Composition, HIPWAC, which was interfaced with the 3-meter telescope at the NASA Infrared Telescope Facility- Spectra were colle cted at a resolution of lambda/delta lambda=10(exp 7). Absorption fea tures of the CO2 isotopologues have been identified from which isotop ic ratios of oxygen have been determined. The isotopic ratios O-17/O -16 and O-18/O-16 in the Martian atmosphere can be related to Martian atmospheric evolution and can be compared to isotopic ratios of oxyg en in the Earth's atmosphere. Isotopic carbon and oxygen are importa nt constraints on any theory for the erosion of the Martian primordia l atmosphere and the interaction between the atmosphere and surface o r subsurface chemical reservoirs. This investigation explored the pr esent abundance of the stable isotopes of oxygen in Mars' atmospheric carbon dioxide by measuring rovibrational line absorption in isotop ic species of CO2 using groundbased infrared heterodyne spectroscopy in the vicinity of the 9.6 micron and 10.6 micron CO2 lasing bands. T he target transitions during this observation were O-18 C-12 O-16 as well as O-178 C-12 O-16 and O-16 C-113 O-16 at higher resolving power of lambda/delta lambda=10(exp 7) and with high signal-to-noise ratio (longer integration time) in order to fully characterize the absorpt ion line profiles. The fully-resolved lineshape of both the strong n ormal-isotope and the weak isotopic CO2 lines were measured simultane ously in a single spectrum.

Smith, R. L.↗
NASA NTRS1980

Evidence for a secular variation in the C-13/C-12 ratio of carbon implanted in lunar soils

A curve of delta(C-13) vs delta(N-15) for lunar soils and breccias shows that the previously recorded 30% change in delta(N-15) is associated with a change in delta(C-13). The correlation represents concurrent changes in the isotope ratios of both elements at their source, and does not result from maturation effects or nonselective sample contamination. A computation of the relative production rates of C-13 and N-15 shows that spallation reactions in the sun could produce the observed ratio of the delta(C-13) to delta (N-15) variations.

Becker, R. H.↗
NASA NTRS1985

Trapped Xe components in etched samples of the Murray (C2) and Murchison (C2) carbonaceous chondrites

Xe isotopic measurements are described. The samples analyzed were bulk chips of the Murray (C2) and Murchison (C2) carbonaceous chondrites that had been freeze-thaw disaggregated, etched with H2O2, and then split into colloidal and noncolloidal fractions using methanol. The etching removed a substantial portion of the trapped Xe and increased variations in measured isotopic ratios compared with bulk sample analyses. The Murray samples appeared to contain a binary mixture of U-Xe and H+L-Xe. The Murchison data concur with the Murray data for the heavy isotopes, but the structure at the light isotopes is obscured by spallation Xe. There is no evidence in these data for the separability of H-Xe and L-Xe. The fact that H2O2 etching removes Xe without prior demineralization supports the view that the carrier of a substantial portion of trapped Xe may reside on grain surfaces.

Jones, C. M.↗
NASA NTRS1993

On the Bur Gheluai H5 chondrite and other meteorites with complex exposure histories

Isotopic concentrations and track densities measured in 13 samples of the Bur Gheluai meteorite fall are presented. Experimental methods are described and results are presented for isotopic ratios of noble gases and cosmogenic radionuclide contents. Evidence for complex irradiation is discussed and a model for two-stage exposure histories is presented. The duration of each irradiation stage and possible effects on isotope production rates are considered. Explanations are suggested for the discrepant Ne production rates.

Vogt, S. K.↗
NASA NTRS1976

Characterization of lunar nitrogen components

Rocks of known and disparate cosmic-ray ages are analyzed to find the spallation production rate of N-15. A soil breccia of known formation age was analyzed for its bearing on the antiquity of the isotopically light component. Further stepwise heating analysis of soils shed further light on occurrences of the components. Lunar soil samples were etched slightly by fluorine, revealing significant differences in isotopic ratios between carbon on grain surfaces and bulk carbon; the surface carbon is not retained during agglutinate formation. Etching revealed that about 25% of the total nitrogen resides on the surface of grains; the nitrogen is isotopically heavy. Etching also revealed about 50% of helium in soils residing below the readily etched outermost 1% of soil grain surfaces.

Becker, R. H.↗
NASA NTRS1986

Aleutian terranes from Nd isotopes

Nd isotope ratios substantiate the identification of oceanic crustal terranes within the continental crustal basement of the Aleutian island arc. The oceanic terranes are exposed in the westernmost Aleutians, but to the east, they are completely buried by isotopically distinct arc-volcanic rocks. Analogous oceanic terranes may be important components of the terrane collages that comprise the continents.

Kay, R. W.↗
NASA NTRS1978

Comparisons between observed and predicted cosmogenic noble gases in lunar samples

Comparisons are made between cosmogenic production rates and isotopic ratios predicted on the basis of nuclear systematics with those observed in well-documented lunar samples. Although some significant differences are found, the agreement in general is surprisingly good. The predicted production rates for Ar-38 and Xe-126 agree reasonably well with observation but the predicted rate for Ne-21 appears to be too high; in most cases the predicted rate for Kr-83 agrees to within 50%, although some larger differences are apparent. There are some prominent cases in which predicted isotopic compositons differ from observation: Kr-78/Kr-83 trends in the wrong sense with the Zr/Sr ratio; Xe-124/Xe-126 is too large by about 13%; Xe-128/Xe-126 is too small by about 6%; Xe-130/Xe-126 is too low by 30-40%.

Hohenberg, C. M.↗
NASA NTRS1983

The C-12/C-13 ratio in Jupiter from the Voyager infrared investigation

An analysis of the v(4) band of CH4 in the spectra recorded by the Voyager 1 IRIS experiment has yielded a C-12/C-13 ratio in Jupiter that is 160 plus 40 or minus 55, or 1.8 plus 0.4 or minus 0.6 times the terrestrial value. It is noted that while no plausible theory predicts such a difference between the C-12/C-13 ratio values of Jupiter and the inner solar system, values of this ratio in the solar neighborhood 4.5 million years ago, inferred from recent interstellar medium measurements, are compatible with the present determination in Jupiter. The Jovian, rather than the terrestrial value, would then be representative of the carbon isotope ratio in the primitive solar nebula.

Courtin, R.↗
NASA NTRS2013

Potassium Isotopic Compositions of NIST Potassium Standards and 40Ar/39Ar Mineral Standards

Knowledge of the isotopic ratios of standards, spikes, and reference materials is fundamental to the accuracy of many geochronological methods. For example, the 238U/235U ratio relevant to U-Pb geochronology was recently re-determined [1] and shown to differ significantly from the previously accepted value employed during age determinations. These underlying values are fundamental to accurate age calculations in many isotopic systems, and uncertainty in these values can represent a significant (and often unrecognized) portion of the uncertainty budget for determined ages. The potassium isotopic composition of mineral standards, or neutron flux monitors, is a critical, but often overlooked component in the calculation of K-Ar and 40Ar/39Ar ages. It is currently assumed that all terrestrial materials have abundances indistinguishable from that of NIST SRM 985 [2]; this is apparently a reasonable assumption at the 0.25per mille level (1σ) [3]. The 40Ar/39Ar method further relies on the assumption that standards and samples (including primary and secondary standards) have indistinguishable 40K/39K values. We will present data establishing the potassium isotopic compositions of NIST isotopic K SRM 985, elemental K SRM 999b, and 40Ar/39Ar biotite mineral standard GA1550 (sample MD-2). Stable isotopic compositions (41K/39K) were measured by the peak shoulder method with high resolution MC-ICP-MS (Thermo Scientific NEPTUNE Plus), using the accepted value of NIST isotopic SRM 985 [2] for fractionation [4] corrections [5]. 40K abundances were measured by TIMS (Thermo Scientific TRITON), using 41K/39K values from ICP-MS measurements (or, for SRM 985, values from [2]) for internal fractionation corrections. Collectively these data represent an important step towards a metrologically traceable calibration of 40K concentrations in primary 40Ar/39Ar mineral standards and improve uncertainties by ca. an order of magnitude in the potassium isotopic compositions of standards.

Morgan, Leah↗
NASA NTRS2017

Distinct Chlorine Isotopic Reservoirs on Mars: Implications for Character, Extent and Relative Timing of Crustal Interaction with Mantle-Derived Magmas, Evolution of the Martian Atmosphere, and the Building Blocks of an Early Mars

The style, magnitude, timing, and mixing components involved in the interaction between mantle derived Martian magmas and Martian crust have long been a point of debate. Understanding this process is fundamental to deciphering the composition of the Martian crust and its interaction with the atmosphere, the compositional diversity and oxygen fugacity variations in the Martian mantle, the bulk composition of Mars and the materials from which it accreted, and the noble gas composition of Mars and the Sun. Recent studies of the chlorine isotopic composition of Martian meteorites imply that although the variation in delta (sup 37) Cl is limited (total range of approximately14 per mille), there appears to be distinct signatures for the Martian crust and mantle. However, there are potential issues with this interpretation. New Cl isotope data from the SAM (Sample Analysis at Mars) instrument on the Mars Science Lab indicate a very wide range of Cl isotopic compositions on the Martian surface. Recent measurements by [10] duplicated the results of [7,8], but placed them within the context of SAM surface data. In addition, Martian meteorite Chassigny contains trapped noble gases with isotopic ratios similar to solar abundance, and has long been considered a pristine, mantle derived sample. However, previous studies of apatite in Chassigny indicate that crustal fluids have interacted with regions interstitial to the cumulus olivine. The initial Cl isotope measurements of apatite in Chassigny suggest an addition of crustal component to this lithology, apparently contradicting the rare gas data. Here, we examine the Cl isotopic composition of multiple generations and textures of apatite in Chassigny to extricate the crustal and mantle components in this meteorite and to reveal the style and timing of the addition of crustal components to mantle-derived magmas. These data reveal distinct Martian Cl sources whose signatures have their origins linked to both the early Solar System and the evolving Martian atmosphere.

Shearer, C. K.↗
NASA NTRS1980

Carbon dioxide measurements in the stratosphere

A mass spectrometer experiment for the analysis of minor constituents in the stratosphere has been flown successfully four times from Palestine, Texas on board a balloon gondola. The carbon dioxide mixing ratio, which shows unexpectedly large variations in the stratosphere, reached 400 ppm in one particular night flight. This is about 20% higher than the ground value. Evidence is presented that the experiment performed well during each of the balloon flights. The isotopic ratio C-12/C-13 was measured and found in good agreement with previous air analyses showing a depletion of C-13.

Mauersberger, K.↗