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NASA NTRS2009

Appendix C: First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

Carbonyl chlorofluoride (COCIF) is an important reservoir of chlorine and Fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COCIF, obtained by Received in revised form the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong Accepted 18 February 2009 source region for COCIF in the tropical stratosphere near 27 km. A layer of enhanced COCIF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts Per trillion by volume, largest in the tropics and decreasing toward the poles. The COCIF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

Fu, Djian↗
NASA NTRS2010

Layered Model for Radiation-Induced Chemical Evolution of Icy Surface Composition on Kuiper Belt and Oort Cloud Bodies

The diversity of albedos and surface colors on observed Kuiper Belt and Inner Oort Cloud objects remains to be explained in terms of competition between primordial intrinsic versus exogenic drivers of surface and near-surface evolution. Earlier models have attempted without success to attribute this diversity to the relations between surface radiolysis from cosmic ray irradiation and gardening by meteoritic impacts. A more flexible approach considers the different depth-dependent radiation profiles produced by low-energy plasma, suprathermal, and maximally penetrating charged particles of the heliospheric and local interstellar radiation environments. Generally red objects of the dynamically cold (low inclination, circular orbit) Classical Kuiper Belt might be accounted for from erosive effects of plasma ions and reddening effects of high energy cosmic ray ions, while suprathermal keV-MeV ions could alternatively produce more color neutral surfaces. The deepest layer of more pristine ice can be brought to the surface from meter to kilometer depths by larger impact events and potentially by cryovolcanic activity. The bright surfaces of some larger objects, e.g. Eris, suggest ongoing resurfacing activity. Interactions of surface irradiation, resultant chemical oxidation, and near-surface cryogenic fluid reservoirs have been proposed to account for Enceladus cryovolcanism and may have further applications to other icy irradiated bodies. The diversity of causative processes must be understood to account for observationally apparent diversities of the object surfaces.

Cooper, John F.↗
NASA NTRS1999

Administrative Report on Training Awards

During the tenure of this award, the recipient (David Harker) conducted areas of research which resulted in the award of a doctorate degree (August 1999) from the University of Wyoming. The primary science activity was investigation of silicate dust mineralogy in comets, particularly comet C/1995 O1 (Hale-Bopp). Determination of the dust mineralogy permits us to address an important astrophysical question of relevance to the origins and evolution of solar systems, "Do comets contain relic interstellar dust grains? Since, comets represent the frozen reservoirs of primitive proto-solar dust and ice, we can gain insight into the problem of understanding the formation of protoplanetesimals in the. early solar nebula. Mid-infrared spectrophotometry (7 - 14 micron, R approx. = 180 - 360) of Hale-Bopp was obtained with the NASA/Ames HIFOGS at four distinct epochs pre- and post- perihelion ion from 1996 October through 1997 June. These observations were conducted at the Wyoming Infrared Observatory and the NASA Infrared Telescope Facility, and were supported by funds from this training grant. The emission at mid-IR wavelengths in cometary comae arises from carbon grains, and small silicate grains which produce resonance features. Hale-Bopp had the strongest silicate feature observed from any comet to date. Theoretical calculations utilizing Mie Scattering Theory were employed to construct Synthetic cometary spectra to fit with the observed HIFOGS 10 microns spectral feature of Hale-Bopp. Our analysis suggests that the observed spectra can be modeled with the Hanner grain size distribution peaked at alpha((sub p) = 0.2 microns of fractal porous grains with porosity parameter D = 2.5. This model spectrum also fits photometry points in the 3 - 5 microns region. Comparison with the ISO SWS spectrum of Hale-Bopp obtained 1996 October reveals that the crystalline olivine grains must be at it temperature hotter than computed from Mie theory.

Woodward, Charles E.↗
NASA NTRS1994

Observations of stratospheric hydrogen fluoride by halogen occultation experiment (HALOE)

The Halogen Occultation Experiment (HALOE) Hydrogen Fluoride (HF) channel on the Upper Atmospheric Research Satellite (UARS) is providing the first global measurements of stratospheric HF, the dominant flourine reservoir in the atmosphere. This paper describes the latitudinal and seasonal variations of HALOE-observed HF in terms of vertical profiles, altitude/latitude cross sections, and column abundances. The HF global distribution shows a 'tracerlike' structure and its column amount increases with latitude, in agreement with previous aircraft measurements of the HF column amount. A comparison between the HALOE HF column above 20 km and the ATMOS 1985 measurements is used to estimate the annual rate of increase of stratospheric HF. Exponential rates of 4.9-6.6%/yr and linear growth rates of 6-8.6%/yr in 1985 and 4.3-5.5%/yr in 1992-1993 are found. HALOE HF measurements during the 1993 Antarctic spring are briefly described. This species behaves like a conserved tracer and its distribution shows an area of enhanced mixing ratios correlated with the polar vortex that has a clear latitude boundary. Finally, simulated HF distributions by the National Center for Atmospheric Research (NCAR) two-dimensional model are used to compare with HALOE observations of HF. Reasonable agreements in the global structure and the absolute amount of HF are found. The differences between the model and the observed results indicate the need for improving treatment of atmospheric dynamics and fluorine-related chemical parameters in the model simulations.

Luo, M.↗
NASA NTRS2006

Constraints on the Formation of the Moon from High-Precision ND-Isotopic Measurements of Lunar Basalts

The most widely accepted theory for the formation of the Earth-Moon system proposes a giant impact model, where Earth collided in its later stages of accretion with a body of the approximate size of Mars [1, 2]. In this model, the Moon ultimately formed from hot debris generated during this giant impact. Short-lived radioisotopes such as Sm-146 (t(sub 1/2) = 103 Ma) may be useful in determining the chronology of the events that formed the Earth-Moon system and for how these terrestrial bodies evolved following accretion. New high-precision samarium-neodymium data showed that chondritic meteorites are on average 20 ppm lower in 142Nd/144Nd than terrestrial samples [3]. These data suggest that if the bulk silicate Earth (BSE) has a Sm/Nd ratio within the range measured for chondrites, the higher-than-chondritic Nd-142/Nd-144 ratio of terrestrial materials requires that the silicate Earth experienced a global chemical differentiation during the lifetime of Sm-146. If the Moon has super-chondritic Nd-142/Nd-144 identical to the Earth, as suggested by available data [4], then the giant impact must have occurred into an already differentiated Earth, predominantly sampling the Nd-depleted reservoir. In order to test this hypothesis, high-precision Nd-isotope ratios were obtained on a Thermo-Finnigan Triton TIMS for six lunar basalts that span the compositional range of lavas from the Moon: Samples 15555 and LAP 02205 represent low-Ti basalts; 70017 and 74275 are high-Ti basalts; 15386 and SAU 169 are KREEP basalts.

Rankenburg, K.↗
NASA NTRS2000

Implications of SWAS Observations for Interstellar Chemistry and Star Formation

A long standing prediction of steady state gas-phase chemical theory is that H2O and O2 are important reservoirs of elemental oxygen and major coolants of the interstellar medium. Analysis of SWAS observations has set sensitive upper limits on the abundance Of O2 and has provided H2O abundances toward a variety of star forming regions. Based on these results, we show that gaseous H2O and O2 are not dominant carriers of elemental oxygen in molecular clouds. Instead the available oxygen is presumably frozen on dust grains in the form of molecular ices, with a significant portion potentially remaining in atomic form, along with CO, in the gas phase. H2O and O2 are also not significant coolants for quiescent molecular gas. In the case of H2O, a number of known chemical processes can locally elevate its abundance in regions with enhanced temperatures, such as warm regions surrounding young stars or in hot shocked gas. Thus, water can be a locally important coolant. The new information provided by SWAS, when combined with recent results from the Infrared Space Observatory, also provide several hard observational constraints for theoretical models of the chemistry in molecular clouds and we discuss various models that satisfy these conditions.

Bergin, Edwin A.↗
NASA NTRS2017

Synthetic Scenarios from CMIP5 Model Simulations for Climate Change Impact Assessments in Managed Ecosystems and Water Resources: Case Study in South Asian Countries

Increasing population, urbanization, and associated demand for food production compounded by climate change and variability have important implications for the managed ecosystems and water resources of a region. This is particularly true for south Asia, which supports one quarter of the global population, half of whom live below the poverty line. This region is largely dependent on monsoon precipitation for water. Given the limited resources of the developing countries in this region, the objective of our study was to empirically explore climate change in south Asia up to the year 2099 using monthly simulations from 35 global climate models (GCMs) participating in the fifth phase of the Climate Model Inter-comparison Project (CMIP5) for two future emission scenarios (representative concentration pathways RCP4.5 and RCP8.5) and provide a wide range of potential climate change outcomes. This was carried out using a three-step procedure: calculating the mean annual, monsoon, and non-monsoon precipitation and temperatures; estimating the percent change from historical conditions; and developing scenario funnels and synthetic scenarios. This methodology was applied for the entire south Asia region; however, the percent change information generated at 1.5deg grid scale can be used to generate scenarios at finer spatial scales. Our results showed a high variability in the future change in precipitation (-23% to 52%, maximum in the non-monsoon season) and temperature (0.8% to 2.1%) in the region. Temperatures in the region consistently increased, especially in the Himalayan region, which could have impacts including a faster retreat of glaciers and increased floods. It could also change rivers from perennial to seasonal, leading to significant challenges in water management. Increasing temperatures could further stress groundwater reservoirs, leading to withdrawal rates that become even more unsustainable. The high precipitation variability (with higher propensity for localized intense rainfall events) observed in the region can be a key factor for managed ecosystems and water management and could also lead to more incidence of severe urban flooding. The results could be used to assess both mitigation and adaptation alternatives to reduce vulnerabilities in managed ecosystems (agricultural and urban) and water resources.

agriculture↗
NASA NTRS2020

FOSSIL—Finding Our Cosmic Roots

FOSSIL (Fragments from the Origins of the Solar System and our Interstellar Locale) is a concept to explore the largest solar system object visible to the unaided eye—the zodiacal cloud. The cloud’s many dust particles are each a tiny time capsule from a comet or asteroid. The FOSSIL concept is for the in situ compositional analysis of interplanetary dust particles, and also of the particles passing through the solar system from interstellar space. By measuring the zodiacal and interstellar particles’ velocity vectors and compositions, the approach resolves fundamental questions about the solar system’s origins. The FOSSIL concept is to: (1) Discover whether today’s local interstellar dust matches the composition of the feedstock from which the solar system formed; (2) Determine whether comets’ fine-grained component preserves unprocessed pre-solar dust or shows signs of processing in the early solar system; and (3) Learn whether comets’ and asteroids’ organic material share a common source or formed from distinct reservoirs. The FOSSIL concept is based on the use of a Dust Telescope (DT) with the capability to measure the composition and the velocity vector of dust particles to unambiguously separate interstellar from interplanetary particles, and identify a subset of zodiacal particles that are exclusively cometary. In the DT, particles pass through the trajectory sensor unharmed and impact a target plate, where they are vaporized and partially ionized. The ions are electrostatically focused onto a detector where the time-of-flight mass spectrum is recorded, enabling measurement of the composition of the interstellar solids, detection of cometary minerals altered by high temperatures or exposure to liquid water in the early solar system, and the characterization of the organic materials from the comets and asteroids that are still being delivered to the Earth today. FOSSIL’s objectives crosscut several disciplines with planetary science. Astrophysics interests lie in understanding interstellar solar matter and the only debris disk accessible in situ. Heliophysics interest is in the verification of large-scale heliospheric magnetic field models by the measured effect on the motion of electrically charged interstellar dust. Reporting the makeup of interplanetary dust that ablates in our atmosphere is valuable to Earth sciences. FOSSIL’s DT is scalable and can be accommodated to a variety of mission opportunities, without restriction on launch dates, and for a large number of possible orbits.

Turner, Neal↗
NASA NTRS2013

Anhydrous Liquid Line of Descent of Yamato 980459 and Evolution of Martian Parental Magmas

Martian basalts represented by the shergottite meteorites reflect derivation from highly depleted mantle sources (high Nd, strong LREE depletions, low fO2)[1-3], with evidence of mixing with a much more enriched and oxidized reservoir, most likely a late-stage product of crystallization of an initial martian magma ocean [3-6]. The martian basaltic meteorites Yamato 980459 (Y98) and QUE 94201 (QUE) have bulk compositions that appear to represent bonafide liquids, rather than products of protracted crystallization. These two meteorites also represent the most primitive and evolved examples of the depleted basaltic shergottite suite. Magmatic liquids serve as effective probes of their source regions, and thus studying the potential relationship between magmas represented by Y98 and QUE can yield important information on the formation and evolution of martian basalts. Although the ages of these meteorites preclude that they are petrogenetically related to each other, they represent the best existing candidates for genuine liquids (other meteorites are suggested to represent liquid compositions, including LAR 06319 [7] and NWA 5789 [8], but only Y98 and QUE have been verified experimentally). They span much of the bulk-compositional range of martian basaltic meteorites, and represent end-member liquid compositions likely to arise from partial melting of the martian mantle. Recent efforts to model Y98-like parent liquid evolution by fractional crystallization using MELTS [6] produced a derivative liquid composition that closely matches QUE bulk composition, although it required a some-what unusual crystallization sequence. Experimental endeavours to verify this result at 1 bar have, however, been inconclusive [9].

Rapp, J. F.↗
NASA NTRS2000

Thermocapillary Flow and Aggregation of Bubbles on a Solid Wall

During the electrolytic evolution of oxygen bubbles forming on a vertically oriented transparent tin oxide electrode, bubbles were found to be mutually attractive. The mechanism of the aggregation had never been explained satisfactorily until Guelcher et al. attributed it to thermocapillary flow. The gradient of surface tension of the liquid at the bubble's surface, which was established because of reaction heat and ohmic heat loss at the electrode wall, drives flow of the liquid adjacent to each bubble; the bubble "pumps" fluid along its surface away from the wall. Fluid flows toward the bubble to conserve mass and entrains nearby bubbles in the flow pattern. The same logic would apply when two bubbles of equal size are adjacent to each other on a warm wall. Each bubble drives thermocapillary flow and hence entrains the other in its flow pattern, which drives the aggregation. Our objective here is to perform experiments where the temperature gradient at the wall is well known and controlled. The theory can be quantitatively tested by studying aggregation of bubble pairs of equal size, and by varying system parameters such as temperature gradient, bubble size and fluid viscosity. The results are then compared with the theory in a quantitatively rigorous manner. We demonstrate that the theory without adjustable parameters is capable of quantitatively modeling the rate of aggregation of two bubbles. The equations governing the thermocapillary flow around a single stationary bubble on a heated or cooled wall in a semi-infinite domain were solved. Both Reynolds number and Marangoni number were much less than unity. The critical result is that liquid in the vicinity of a warm wall flows toward a stationary collector bubble. Consequently the thermocapillary flow around the stationary bubble entrains another bubble toward itself. The bubbles undergo hindered translation parallel to the wall with velocity U while the fluid flow field is described with u. Two velocities were equated by using a wall hindrance parameter q: U = qu [1] which shows the velocity of bubble is proportional to the entraining velocity. The hindrance parameter q can experimentally be measured independently. q can also be calculated by solving the equations of motion for a bubble translating parallel to a solid wall. The experimental cell is cylindrical with an ID of 10 cm and consists of a 1 cm deep main cell filled with silicone oil and flanked by two thermal reservoirs. The upper thermal reservoir was heated and the lower thermal reservoir was cooled so that the bubbles aggregate. Two types of silicone oil (eta = 0.02 and 0.50 Pa s) were used. Two equal sized air bubbles were injected into the cell with a syringe. The center-to-center distance of bubbles was observed through a microscope. Bubble radius ranged from 0.40 mm to 0.65 mm and the temperature gradients along with the cell ranged from 1400 to 5000 K/m. The bubbles aggregated when heat flows from the wall to the fluid. The velocities of bubbles were in the range of 1 - 10 microns/s. The separation r decreased more quickly when the temperature gradient was higher, bubble size was larger, and the oil viscosity was lower. r decreased more rapidly as the bubbles approached each other. Dimensionless time was arbitrarily set to be zero when the dimensionless center-to-center distance between the bubbles was 4. All the bubble trajectories fall onto one line, especially in the range of dimensionless distance from 4 to 3. This means the relative movement of the bubble pair is proportional to the temperature gradient and bubble size and it is inversely proportional to the viscosity of the oil. This result strongly suggests that the thermocapillary flow-based aggregation mechanism is correct. A value of q can be estimated by fitting the scaled data to Eq. [1]. A best fit value of q was obtained as q = 0.26 with a standard deviation of 0.03. Independent experimental results for q for a 0.5 mm radius bubble, give values of q in the range 0.11 to 0.23. The value of q obtained from solving the equations of motion reveals q has values in the range 0.23 - 0.30. Since the full scale of possible values of q is zero to one, the maximum deviation of independently determined values of q from the best fit value was 15% of this full scale. Thus reasonable quantitative agreement between theory and experiment has been obtained.

Kasumi, Hiroki↗
NASA NTRSDate not supplied

The Application of Remote Sensing and Machine Learning to Improve Early Warning Systems for Harmful Algal Events in the Highland Lake Chain, TX

Beginning in 2019, harmful algal events have caused canine deaths in both Lady Bird Lake and Lake Travis located near Austin, Texas. These two reservoirs are part of the larger Highland Lakes chain, managed by the City of Austin Department of Watershed Protection (COA DWP) and the Lower Colorado River Authority (LCRA), which fulfill municipal, commercial, and agricultural water demands. Given the recent increase in favorable environmental conditions for algal events in central Texas, NASA DEVELOP partnered with LCRA and COA DWP to improve monitoring and early detection of algal events, utilizing satellite remote sensing and machine learning. Spatially and temporally varied chlorophyll a concentrations, cyanobacteria detections, turbidity, and water surface temperature products are used as environmental proxies. Landsat 8 Operational Land Imager (OLI) and the Sentinel-2 MultiSpectral Instrument (MSI) data were used to provide a combined revisit time of up to ~3 days and < 30 m per pixel products. Chlorophyll a concentrations were estimated using a pre-trained Mixture Density Network, and cyanobacteria detection was accomplished using the Broad Wavelength Algae Index, which can differentiate algal blooms from algal proliferations (mats). In situ data were used to validate remotely sensed measurements and quantify uncertainties. Preliminary results show a good fit between the modeled output and in situ observations, suggesting that remote sensing data can be used to retrieve biogeochemical properties and/or inherent optical properties (IOPs) of water columns in these inland human-made lakes. Uncertainties were introduced from the sensitivity to atmospheric correction, inherent mismatch between satellite and sampling data, and a relatively lower signal-to-noise ratio over water. The resulting products enable near real-time monitoring of environmental proxies relevant to algal event presence in the Highland Lakes chain, and will ultimately support water management, decision making, and risk communication.

Shuyu Chang↗
NASA NTRS1992

Multi-resolution processing for fractal analysis of airborne remotely sensed data

Fractal geometry is increasingly becoming a useful tool for modeling natural phenomenon. As an alternative to Euclidean concepts, fractals allow for a more accurate representation of the nature of complexity in natural boundaries and surfaces. Since they are characterized by self-similarity, an ideal fractal surface is scale-independent; i.e. at different scales a fractal surface looks the same. This is not exactly true for natural surfaces. When viewed at different spatial resolutions parts of natural surfaces look alike in a statistical manner and only for a limited range of scales. Images acquired by NASA's Thermal Infrared Multispectral Scanner are used to compute the fractal dimension as a function of spatial resolution. Three methods are used to determine the fractal dimension - Schelberg's line-divider method, the variogram method, and the triangular prism method. A description of these methods and the results of applying these methods to a remotely-sensed image is also presented. Five flights were flown in succession at altitudes of 2 km (low), 6 km (mid), 12 km (high), and then back again at 6 km and 2 km. The area selected was the Ross Barnett reservoir near Jackson, Mississippi. The mission was flown during the predawn hours of 1 Feb. 1992. Radiosonde data was collected for that duration to profile the characteristics of the atmosphere. This corresponds to 3 different pixel sizes - 5m, 15m, and 30m. After, simulating different spatial sampling intervals within the same image for each of the 3 image sets, the results are cross-correlated to compare the extent of detail and complexity that is obtained when data is taken at lower spatial intervals.

Jaggi, S.↗
NASA NTRS2000

Photodissociation Regions

The interstellar medium of galaxies is the reservoir out of which stars are born and into which stars inject newly created elements as they age. The physical properties of the interstellar medium are governed in part by the radiation emitted by these stars. Far-ultraviolet (6 eV< hNu < 13.6 eV) photons from massive stars dominate the heating and influence the chemistry of the neutral atomic gas and much of the molecular gas in galaxies. Predominantly neutral regions of the interstellar medium in which the heating and chemistry are regulated by far ultraviolet photons are termed Photodissociation Regions (PDRs). These regions are the origin of most of the non-stellar infrared (IR) and the millimeter and submillimeter CO emission from galaxies. The importance of PDRs has become increasingly apparent with the advances in IR and submillimeter astronomy. The IR emission from PDRs includes fine structure lines of C, C(+) and O; rovibrational lines of H2; rotational lines of CO; broad mid-IR features of polycyclic aromatic hydrocarbons; and a luminous underlying IR continuum from interstellar dust. The transition of H to H2 and C(+) to CO occurs within PDRs. Comparison of observations with theoretical models of PDRs enables one to determine the density and temperature structure, the elemental abundances, the level of ionization, and the radiation field. PDR models have been applied to interstellar clouds near massive stars, planetary nebulae, red giant outflows, photoevaporating planetary disks around newly formed stars, diffuse clouds, the neutral intercloud medium, and molecular clouds in the interstellar radiation field-in summary, much of the interstellar medium in galaxies. Theoretical PDR models explain the observed correlations of the [CII] 158, micrometers with the CO J=1-0 emission, the CO J=1-0 luminosity with the interstellar molecular mass, and the [CII] 158 micrometers plus [OI] 63 micrometers luminosity with the IR continuum luminosity. On a more global scale, PDR models predict the existence of two stable neutral phases of the interstellar medium, elucidate the formation and destruction of star-forming molecular clouds, and suggest radiation-induced feedback mechanisms that may regulate star formation rates and the column density of gas through giant molecular clouds.

Hollenbach, David J.↗
NASA NTRS1999

Photodissociation Regions in the Interstellar Medium of Galaxies

The interstellar medium of galaxies is the reservoir out of which stars are born and into which stars inject newly created elements as they age. The physical properties of the interstellar medium are governed in part by the radiation emitted by these stars. Far-ultraviolet (6 eV less than h(nu) less than 13.6 eV) photons from massive stars dominate the heating and influence the chemistry of the neutral atomic gas and much of the molecular gas in galaxies. Predominantly neutral regions of the interstellar medium in which the heating and chemistry are regulated by far ultraviolet photons are termed Photo-Dissociation Regions (PDRs). These regions are the origin of most of the non-stellar infrared (IR) and the millimeter and submillimeter CO emission from galaxies. The importance of PDRs has become increasingly apparent with advances in IR and submillimeter astronomy. The IR emission from PDRs includes fine structure lines of C, C+, and O; rovibrational lines of H2, rotational lines of CO; broad middle features of polycyclic aromatic hydrocarbons; and a luminous underlying IR continuum from interstellar dust. The transition of H to H2 and C+ to CO occurs within PDRs. Comparison of observations with theoretical models of PDRs enables one to determine the density and temperature structure, the elemental abundances, the level of ionization, and the radiation field. PDR models have been applied to interstellar clouds near massive stars, planetary nebulae, red giant outflows, photoevaporating planetary disks around newly formed stars, diffuse clouds, the neutral intercloud medium, and molecular clouds in the interstellar radiation field-in summary, much of the interstellar medium in galaxies. Theoretical PDR models explain the observed correlations of the [CII] 158 microns with the COJ = 1-0 emission, the COJ = 1-0 luminosity with the interstellar molecular mass, and the [CII] 158 microns plus [OI] 63 microns luminosity with the IR continuum luminosity. On a more global scale, MR models predict the existence of two stable neutral phases of the interstellar medium, elucidate the formation and destruction of star-forming molecular clouds, and suggest radiation-induced feedback mechanisms that may regulate star formation rates and the column density of gas through giant molecular clouds.

Hollenbach, David J.↗
NASA NTRS2018

Core-Mantle Fractionation of Carbon in Earth and Mars: the Effects of Sulfur

Constraining carbon (C) fractionation between silicate magma ocean (MO) and core-forming alloy liquid during early differentiation is essential to understand the origin and early distribution of C between reservoirs such as the crust-atmosphere, mantle, and core of Earth and other terrestrial planets. Yet experimental data at high pressure (P)-temperature (T) on the effect of other light elements such as sulfur (S) in alloy liquid on alloy-silicate partitioning of C and C solubility in Fe-alloy compositions relevant for core formation is lacking. Here we have performed multi-anvil experiments at 6–13 GPa and 1800–2000 °C to examine the effects of S and Ni on the solubility limit of C in Fe-rich alloy liquid as well as partitioning behavior of C between alloy liquid and silicate melt (𝐷𝐷(sub C)(sup alloy/silicate)). The results show that C solubility in the alloy liquid as well as 𝐷𝐷(sub C)(sup alloy/silicate) decreases with increasing in S content in the alloy liquid. Empirical regression on C solubility in alloy liquid using our new experimental data and previous experiments demonstrates that C solubility significantly increases with increasing temperature, whereas unlike in S-poor or S-free alloy compositions, there is no discernible effect of Ni on C solubility in S-rich alloy liquid. Our modelling results confirm previous findings that in order to satisfy the C budget of BSE, the bulk Earth C undergoing alloy-silicate fractionation needs to be as high as those of CI-type carbonaceous chondrite, i.e., not leaving any room for volatility-induced loss of carbon during accretion. For Mars, on the other hand, an average single-stage core formation at relatively oxidized conditions (1.0 log unit below IW buffer) with 10-16 wt.% S in the core could yield a Martian mantle with a C budget similar to that of Earth’s BSE for a bulk C content of ~0.25-0.9 wt.%. For the scenario where C was delivered to the proto-Earth by a S-rich differentiated impactor at a later stage, our model calculations predict that bulk C content in the impactor can be as low as ~0.5 wt.% for an impactor mass that lies between 9-20% of present day Earth’s mass. This value is much higher than 0.05-0.1 wt.% bulk C in the impactor predicted by Li et al. (2016) because C-solubility limit of 0.3 wt.% in a S-rich alloy predicted by their models is significantly lower than the experimentally derived C-solubility of ~1.6 wt. % for the relevant S-content in the core of the impactor.

Carbon↗
NASA NTRS2015

Lead Isotopes in Olivine-Phyric Shergottite Tissint: Implications for the Geochemical Evolution of the Shergottite Source Mantle

Geochemically-depleted shergottites are basaltic rocks derived from a martian mantle source reservoir. Geochemical evolution of the martian mantle has been investigated mainly based on the Rb-Sr, Sm-Nd, and Lu-Hf isotope systematics of the shergottites [1]. Although potentially informative, U-Th- Pb isotope systematics have been limited because of difficulties in interpreting the analyses of depleted meteorite samples that are more susceptible to the effects of near-surface processes and terrestrial contamination. This study conducts a 5-step sequential acid leaching experiment of the first witnessed fall of the geochemically-depleted olivinephyric shergottite Tissint to minimize the effect of low temperature distrubence. Trace element analyses of the Tissint acid residue (mostly pyroxene) indicate that Pb isotope compositions of the residue do not contain either a martian surface or terrestrial component, but represent the Tissint magma source [2]. The residue has relatively unradiogenic initial Pb isotopic compositions (e.g., 206Pb/204Pb = 10.8136) that fall within the Pb isotope space of other geochemically-depleted shergottites. An initial μ-value (238U/204Pb = 1.5) of Tissint at the time of crystallization (472 Ma [3]) is similar to a time-integrated mu- value (1.72 at 472 Ma) of the Tissint source mantle calculated based on the two-stage mantle evolution model [1]. On the other hand, the other geochemically-depleted shergottites (e.g., QUE 94201 [4]) have initial μ-values of their parental magmas distinctly lower than those of their modeled source mantle. These results suggest that only Tissint potentially reflects the geochemical signature of the shergottite mantle source that originated from cumulates of the martian magma ocean

Moriwaki, R.↗
NASA NTRS2012

Sources of Sulfate Found in Mounds and Lakes at the Lewis Cliffs Ice Tongue, Transantarctic

Massive but highly localized Na-sulfate mounds (mirabilite, Na2SO4.10H2O) have been found at the terminal moraine of the Lewis Cliffs Ice Tongue (LCIT), Antarctica. (Sigma)34S and (Sigma)18O values of LCIT mirabilite range from +48.8 to +49.3% (CDT), and -16.6 to -17.1% (V-SMOW), respectively, while (Delta)17O average -0.37% (V-SMOW). LCIT mirabilite mounds are isotopically different from other mirabilite mounds found in coastal regions of Antarctica, which have isotope values close to seawater compositions. (Sigma)18O and (Delta)17O values suggest the incorporation of isotopically light glacial water. Data point to initial sulfate formation in an anoxic water body, either as a stratified anoxic deep lake on the surface, a sub-glacial water reservoir, or a sub-glacial lake. Several surface lakes of varying size are also present within this region of the LCIT, and in some cases are adjacent to the mirabilite mounds. O and D isotope compositions of surface lakes confirm they are derived from a mixture of glacial ice and snow that underwent moderate evaporation. (Sigma)18O and (Sigma)D (V-SMOW) values of snow, ice, and lake water range from -64.2 to -29.7%, and -456.0 to -231.7%, respectively. However, the isotope chemistry of these surface lakes is extremely different from the mounds. Dissolved SO4-2 (Sigma)34S and (Sigma)18O values range from +12.0 to +20.0% and -12.8 to -22.2% (the most negative (Sigma)18O of terrestrial sulfate ever reported), respectively, with sulfate (Delta)17O ranging from +0.93 to 2.24%. Ion chromatography data show that lake water is fresh to brackish in origin, with TDS less than 1500 ppm, and sulfate concentration less than 431 ppm. Isotope and chemical data suggest that these lakes are unlikely the source of the mirabilite mounds. We suggest that lake water sulfate is potentially composed of a mixture of atmospheric sulfate and minor components of sulfate of weathering origin, much like the sulfate in the polar plateau soils of the McMurdo Dry Valleys. A simple model explains mirabilite mound formation at the LCIT. Sulfur redox processes could occur sub-glacially as a result of liquid-water-based glacial conditions (Alpine style glacier), most likely formed by pressure melting of overlying ice (Aharon, GCA, 52, 2321-2331). We suggest that the aqueous base of the LCIT contains dissolved SO42- and is anoxic where sulfate reduction to H2S, HS-, or native sulfur takes place. Sulfide is removed by either precipitation as sulfide minerals or by escape of H2S (neither of which have been observed). Mirabilite precipitation is likely the result of evaporation or freezing of sulfate-rich brines as they reach the surface where they manifest themselves as mounds. Pressure from the overlying ice contributing to a pressure-melting scenario that creates the sub-glacial aqueous environment also contributes to the mechanism of upward transport of the sulfate-rich fluids. Further evidence to support this upward transport model comes from the nature of ice motion at the LCIT. Cassidy et al (Meteoritics, 27, 490-525, 1992) pointed out that it is the vertical ice motion in this area that creates the meteorite-stranding surface that could also account for upward transport of sulfate-rich fluids. Alternatively, mirabilite was deposited in a similar condition as present-day coastal Antarctica when the LCIT was wetter and warmer

Socki, Richard↗
NASA NTRS2018

Understanding the Water Cycle Above the North Polar Cap on Mars Using MRO CRISM Retrievals of Water Vapor

The north polar cap (NPC) on Mars is the major reservoir of atmospheric water (H2O) currently on Mars. The retrieval and monitoring of atmospheric water vapor abundance are crucial for tracking the cycle of water above the NPC. The Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) aboard the Mars Reconnaissance Orbiter (MRO) has provided a wealth of data that extend over 5 + Martian years, covering the time period between 2006 and 2016. CRISM is ideally suited for spring and summer observations of the north polar region (latitudes poleward of 60 °N). The retrievals of water vapor column abundances over this extended period of time were performed over both ice-free and water ice covered surfaces, extending the coverage of the water vapor maps to include the permanent cap, where a maximum value of 90 precipitable micrometers (pr–µm) is retrieved, as compared to 60 pr–µm over ice-free regions in the North Polar Region. Away from summertime maximum, modest interannual variability in the water vapor abundance is observed. Zonal averages over all the observed Martian years combined show a developing water front that shifts northward towards summer, before dissipating over the permanent cap during mid-summer. A prominent feature at latitudes around 75 °N shows large abundances of water vapor, indicating a water vapor annulus encircling the retreating edge of the seasonal polar cap during late spring. Meridional transport of water modeled here show that the annulus may be a result of the convergence of water vapor from both south and north along the retreating edge of the NPC.

Khayat, Alain S. J.↗