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At least 19 records

Ice Radiation Chemistry as a Source of Potential False Biomarkers on the Surface of Europa

If we find evidence of Life elsewhere in the Solar System it will probably be in form of chemical biomarkers, quintessentially biological molecules that indicate the presence of micro-organisms. While molecules such as amino acids and nucleo-bases might seem to be biomarkers, and alkyl substituted aromatics have been invoked as such, they are not necessarily. These molecules are present in some meteorites and are expected to be present on the surface of other planets even in the absence of life. Understanding the range of non-biological organic molecules which could act as false biomarkers in space is a prerequisite for any reasonable search for true biomarkers on other worlds. Our experiments have shown that some organic molecules in meteorites that appear biological in nature are formed by energetic processing of extraterrestrial ices can account for amino acids, quinones and other functionalized aromatic compounds. In the past, such molecules have been proposed as biomarkers. For example, alkylated aromatics were invoked as biomarkers in the Alan Hills 84001 'Martian meteorite.' When simple organics arrive at the surface of a body like Europa, either from below or from space, how long do they survive and what do they make? How can we distinguish these from real biomarkers?

Bernstein, Max P.↗

First-of-a-Kind Fuel-bearing Molten Chloride Irradiation Experiment

As a dozen MSR developers in the U.S. work toward an aggressive commercialization timeline, many of their fueled-salts—notably, chloride-based compositions—have never been irradiated. Licensing and operating these reactors requires an understanding of (1) the source term, radiation chemistry, and gas generation; (2) unanticipated irradiation-induced corrosion effects; and (3) the impact of burnup on thermophysical properties, all of which can be deduced through irradiation testing. Idaho National Laboratory (INL) is ideally suited to leverage its expertise in chloride salt chemistry, as well as its Neutron Radiography Reactor (NRAD) facility in the Hot Fuels Examination Facility (HFEF) at the Materials and Fuels Complex (MFC), to conduct the world’s first fuel-bearing chloride salt irradiation and fill in the knowledge gaps pertaining to salt chemistry under irradiation. Molten-salt Research Temperature-controlled Irradiation (MRTI) consists of a salt-containing capsule that is internally heated inside of a secondary containment. The experiment must rely on resistive heating to melt the salt before irradiation (to avoid the impact of radiolysis) and once the reactor is turned on and fission reactions commence in the salt, the resistive power can then be reduced. Salt-immersed thermocouples coupled to a controller allow for the heater power to be adjusted as needed to meet experimental objectives. The bulk of the experimental results will be achieved through Post-Irradiation Examination (PIE). At which point a range of different measurements are anticipated to assess the salt/plenum/wall composition, the capsule corrosion rate, and the evolution of salt properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Ice photochemistry as a source of amino acids and other organic molecules in meteorites, and implications for the origin of life and the search for life in the Solar System

The tons of extraterrestrial organic material that come to the Earth every day probably helped to made the Earth habitable, and possibly played a role in the origin of life. At the astrochemistry lab (http://www.astrochem.orq) we investigate the formation and distribution of organic molecules in space and consider the impact such molecules may have on the habitability of planets and the search for life in the Solar System. The organic compounds in meteorites include amino acids, aromatics of various sorts including purine and pyrimidine bases, and fatty acids that form bi-layer vesicles. The origin of many of these species remains mysterious, but in recent years we and others have performed experiments that suggest low temperature radiation chemistry could account for the presence and deuterium enrichment of many of these molecules. . I will present our laboratory experiments that show the viability of low temperature radiation chemistry as a source of organic molecules such as;amino acids (Nature, 2002, 416, 401-403), amphiphiles (Astrobiology, 2003, 2, 371, Proc. Nat. Acad. Sci. 2001, 98, 815), quinones (Science, 1999, 283, 1135) and other functionalized aromatic compounds (Meteoritics, 2001, 36, 351 ; Astrophysical Journal., 2003, 582, L25), some of which were invoked as potential biomarkers in the Alan Hills 84001 Martian meteorite. Understanding how components of proteins and DNA could form in sterile space environments is also of relevance to our search for life elsewhere in the Solar System, the great task now ahead of NASA. If we find evidence of Life elsewhere in the Solar System it will probably be in form of chemical biomarkers, quintessentially biological molecules that indicate the presence of micro-organisms. While most people think of molecules such as amino acids, and nucleo-bases as good candidate biomarkers, these molecules are produced non-biotically in space and are expected to be present on the surface of other planets even in the absence of Life. Understanding the range of non-biological organic molecules which could act as false biomarkers in space is a prerequisite for any reasonable search for Life on other worlds.

Bernstein, Max↗

Cosmogenic nuclides in the Martian surface: Constraints for sample recovery and transport

Stable and radioactive cosmogenic nuclides and radiation damage effects such as cosmic ray tracks can provide information on the surface history of Mars. A recent overview on developments in cosmogenic nuclide research for historical studies of predominantly extraterrestrial materials was published previously. The information content of cosmogenic nuclides and radiation damage effects produced in the Martian surface is based on the different ways of interaction of the primary galactic and solar cosmic radiation (GCR, SCR) and the secondary particle cascade. Generally the kind and extent of interactions as seen in the products depend on the following factors: (1) composition, energy and intensity of the primary SCR and GCR; (2) composition, energy and intensity of the GCR-induced cascade of secondary particles; (3) the target geometry, i.e., the spatial parameters of Martian surface features with respect to the primary radiation source; (4) the target chemistry, i.e., the chemical composition of the Martian surface at the sampling location down to the minor element level or lower; and (5) duration of the exposure. These factors are not independent of each other and have a major influence on sample taking strategies and techniques.

Englert, Peter A. J.↗

Benchmarking GOCART-2G in the Goddard Earth Observing System (GEOS)

The Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which controls the sources sinks and chemistry within the Goddard Earth Observing System, recently underwent a major refactoring and update to the representation of physical processes. The code refactoring increases flexibility such multiple instances of an aerosol species can be run and interact with radiation and cloud microphysics, in addition to the output of multiple wavelength aerosol optical properties in support of data assimilation. From a science perspective, a new radiatively active tracer, brown carbon, was added to distinguish smoke from other sources of organic aerosol thereby improving optical properties entering the radiative calculations. A four-year benchmark simulation was evaluated using in situ and space borne measurements to develop a baseline and prioritize future development. A comparison of simulated aerosol optical depth between GOCART-2G and MODIS retrievals indicates the model captures the overall spatial pattern and seasonal cycle of aerosol optical depth but overestimates aerosol extinction over dusty regions and underestimates aerosol extinction over northern hemisphere boreal forests, requiring further tuning of emissions. This MODIS-based analysis is corroborated by comparisons to MISR and selected AERONET stations. Despite the underestimate of aerosol optical depth in biomass burning regions in GEOS, there is an overestimate in the surface mass of organic carbon in the United States, especially during the summer months.

Allison Collow↗

Benchmarking GOCART-2G in the Goddard Earth Observing System (GEOS)

The Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which controls the sources sinks and chemistry within the Goddard Earth Observing System, recently underwent a major refactoring and update to the representation of physical processes. This paper serves to document code changes that were included in GOCART 2nd Generation (GOCART-2G) and establishes a benchmark simulation that is to be used for future development of the system. The code refactoring increases flexibility such multiple instances of an aerosol species can be run and interact with radiation and cloud microphysics, in addition to the output of multiple wavelength aerosol optical properties in support of data assimilation. From a science perspective, a new radiatively active tracer, brown carbon, was added to distinguish smoke from other sources of organic aerosol thereby improving optical properties entering the radiative calculations. A four-year benchmark simulation was evaluated using in situ and space borne measurements to develop a baseline and prioritize future development. A comparison of simulated aerosol optical depth between GOCART-2G and MODIS retrievals indicates the model captures the overall spatial pattern and seasonal cycle of aerosol optical depth but overestimates aerosol extinction over dusty regions and underestimates aerosol extinction over northern hemisphere boreal forests, requiring further tuning of emissions. This MODIS-based analysis is corroborated by comparisons to MISR and selected AERONET stations. Despite the underestimate of aerosol optical depth in biomass burning regions in GEOS, there is an overestimate in the surface mass of organic carbon in the United States, especially during the summer months.

Allison B Collow↗

Radiative interactions in a hydrogen-fueled supersonic combustor

The two-dimensional, elliptic Navier-Stokes equations are used to investigate supersonic flows with finite-rate chemistry and radiation, for hydrogen-air systems. The chemistry source term in the species equation is treated implicitly to alleviate the stiffness associated with fast reactions. The explicit, unsplit MacCormack finite-difference scheme is used to advance the governing equations in time, until convergence is achieved. The specific problem considered is the premixed flow in a channel with a 10-deg compression ramp. Three different chemistry models are used, accounting for increasing number of reactions and participating species. Two chemistry models assume nitrogen as inert, while the third model accounts for nitrogen reactions and NO(x) formation. The tangent slab approximation is used in the radiative flux formulation. A pseudogray model is used to represent the absorption-emission characteristics of the participating species. Results otained for specific conditions indicate that the radiative interactions vary substantially, depending on reactions involving HO2 and NO species, and that this can have a significant influence on the flowfield.

Chandrasekhar, R.↗

Radiative interactions in chemically reacting supersonic internal flows

The two-dimensional, elliptic Navier-Stokes equations are used to investigate supersonic flows with finite-rate chemistry and radiation for hydrogen-air systems. The chemistry source terms in the species equation is treated implicitly to alleviate the stiffness associated with fast reactions. The explicit, unsplit MacCormack finite-difference scheme is used to advance the governing equations in time, until convergence is achieved. The specific problem considered is the premixed flow in a channel with a ten-degree compression ramp. Three different chemistry models are used, accounting for increasing number of reactions and participating species. Two chemistry models assure nitrogen as inert, while the third model accounts for nitrogen reactions and NO(x) formation. The tangent slab approximation is used in the radiative flux formulation. A pseudo-gray model is used to represent the absorption-emission characteristics of the participating species. Results obtained for specific conditions indicate that the radiative interactions vary substantially, depending on reactions involving HO2 and NO species and that this can have a significant influence on the flowfield.

Tiwari, S. N.↗

Thermochemical nonequilibrium and radiative interactions in supersonic hydrogen-air combustion

The two-dimensional, elliptic Navier-Stokes equations are used to investigate supersonic flows with nonequilibrium chemistry and thermodynamics, coupled with radiation, for hydrogen-air systems. The chemistry source term in the species equation is treated implicitly to alleviate the stiffness associated with fast reactions. The explicit, unsplit MacCormack finite-difference scheme is used to advance the governing equations in time, until convergence is achieved. The specific problem considered is the premixed, expanding flow in a supersonic nozzle. The reacting flow consists of seven species, one of which is the inert N2 molecule. The thermal state of the gas is modeled with one translational-rotational temperature and five vibrational temperatures. The harmonic oscillator model is used in the formulation for vibrational relaxation. The tangent slab approximation is used in the radiative flux formulation. A pseudo-gray model is used to represent the absorption-emission characteristics of the participating species. Results obtained for specific conditions indicate the presence of nonequilibrium in the expansion region. This reduces the radiative interactions and can have a significant influence on the flowfield.

Chandrasekhar, R.↗

Gamma Driven Catalysis of Ammonia

Experiments were conducted to investigate a passive production mechanism for the world’s most energy intensive commodity, ammonia. A novel method, gamma catalyzed ammonia production at ambient conditions, was investigated. Ammonia is currently produced through the highly energy intensive Haber-Fritz process, which requires an operation pressure of 400 atmosphere and 600 degrees Celsius. Due to the high demand and need for ammonia, the Haber-Bosch process consumes 25% all energy produced globally. Reported herein was an attempt to produce ammonia at ambient temperature (20 C) and ambient pressure (1 atm), through a novel process developed at PNNL, gamma driven catalysis of ammonia. Although the measurements of the ammonia production suggest wild success, reports in the literature by Gao et.al. suggest an experimental positive bias in the results. To rule out the potential positive bias, multiple additional production campaigns would be needed to with an alternate analysis technique such as ion chromatography, as suggested by Gao et.al. Unfortunately, due to this late determination of potential positive bias, the results of this study remain inconclusive to the feasibility of gamma driven catalysis of ammonia and more work is needed to describe the chemical evolution with time. The results are a first step and demonstrate that gamma-catalyst mediated reactions are possible. This represents a key opportunity to explore the fundamental chemistry of high band gap catalysts that can change the paradigm of radiation, transforming it from a waste to a valuable energy source.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Relative Contributions of the Saharan and Sahelian Sources to the Atmospheric Dust Load Over the North Atlantic

It has long been recognized that Saharan desert is the major source for long range transport of mineral dust over the Atlantic. The contribution from other natural sources to the dust load over the Atlantic has generally been ignored in previous model studies or been replaced by anthropogenically disturbed soil emissions. Recently, Prospero et.at. have identified the major dust sources over the Earth using TOMS aerosol index. They showed that these sources correspond to dry lakes with layers of sediment deposed in the late Holocene or Pleistocene. One of the most active of these sources seem to be the Bodele depression. Chiapello et al. have analyzed the mineralogical composition of dust on the West coast of Africa. They found that Sahelian dust events are the most intense but are less frequent than Saharan plumes. This suggests that the Bodele depression could contribute significantly to the dust load over the Atlantic. The relative contribution of the Sahel and Sahara dust sources is of importance for marine biogeochemistry or atmospheric radiation, because each source has a distinct mineralogical composition. We present here a model study of the relative contributions of Sahara and Sahel sources to the atmospheric dust aerosols over the North Atlantic. The Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model is used to simulate dust distribution in 1996-1997. Dust particles are labeled depending on their sources. In this presentation, we will present the comparison between the model results and observations from ground based measurements (dust concentration, optical thickness and size distribution) and satellite data (TOMS aerosol index). The relative contribution of each source will then be analyzed spatially and temporally.

Ginoux, Paul↗

The effects of chromospheric radiation on the circumstellar chemistry of evolved stars

Astrophysical situations are discussed in which radiation sources other than interstellar are important, and the atomic abundances of the Alpha Ori circumstellar envelope (CSE) are related to the chromospheric and interstellar radiation fields, and to the temperature distribution. The most common Alpha Ori CSE species are neutral atoms and first ions, and the electron fraction is high throughout the entire CSE. A peak in the neutral abundances in the outer CSE appears close to where the chromospheric and interstellar radiation fields are equal. The present theory predicts that the slope of the K I density should change from about -1.5 to -3.5 in the outer envelope, with the mass loss rate implied by this K I density being of the order of 4 x 10 to the -6th solar masses/yr.

Glassgold, A. E.↗

Approaches for Exploring the Organic Evolution of Titan's Surface

Saturn's largest moon Titan has a cold, very dense nitrogen atmosphere rich in methane and the hydrocarbon and nitride products of methane photolysis. Sources of energy for atmospheric chemistry include solar ultraviolet radiation, Saturn magnetospheric particles, and galactic cosmic rays. The chemistry of Titan's atmosphere, while interesting from the point of view of planetary photochemistry, is largely free radical driven and therefore not particularly suited to the synthesis of polymeric biomolecules or even their precursors. However, the nature of Titan's atmosphere, in particular its redox state (hydrogen escapes rapidly and is under abundant compared to in the giant planets), and the presence of a variegated surface make consideration of surface chemistry on Titan interesting from an astrobiological viewpoint. Additional information is contained in the original extended abstract.

Beauchamp, P.↗

Application of a Reynolds stress turbulence model to a supersonic radiating hydrogen-air diffusion flame

A second-order differential Reynolds Stress turbulence model has been applied to the Favre-averaged Navier-Stokes equations for the study of supersonic flows with finite-rate chemistry and radiation. An assumed Beta Probability Density Function is applied to account for the chemical source terms and the radiative flux terms in the conservation equations. A seven-species, seven-reaction finite rate chemistry mechanism is used to simulate the combustion process. The tangent slab approximation is used in radiative flux formulation. A pseudo-gray gas model is used to represent the absorption-emission characteristics of the participating species. The turbulence/radiation interaction is achieved via a new formulation. The resulting formulation is validated by comparison with experimental data on reacting supersonic axisymmetric jets. Results obtained for specific conditions indicate that the effect of chemical reaction on the turbulence is significant. Also, the radiative heat transfer is enhanced by the turbulence.

Chandrasekhar, R.↗

Multisensor satellites and data systems for earth observations

The applications of multisensor satellites for earth sciences studies in the next two decades are discussed in terms of instrumentation and expected technology developments. Passive microwave and IR sounders with better resolution than currently available are forecast for the mid- to late-1980's, enabling improved understanding of the coupling between the atmosphere, ocean, land, and the biosphere. The global troposphere will be examined for sources, sinks, and fluxes of its chemistry, and interactions among radiation, chemistry, and dynamics in the upper atmosphere. The Landsat 4 Thematic Mapper, along with imagers, radars, and spectrometers carried aloft on the Shuttle are being used and tested to characterize the relative utility of various parts of the electromagnetic spectrum. Hydrologic studies with spacecraft imagery have led to the development of moisture models that will give improved predictive ability to soil moisture, snow cover variations, and the distribution and magnitude of global precipitation and evapotranspiration.

Thome, P. G.↗

Middle Atmosphere Program. Handbook for MAP, volume 19

This MAP handbook is concerned with rocket techniques and instrumentation as they are currently employed in the middle atmosphere. It is composed of nine chapters, written by experts on rocket experiments. The emphasis is on measurement techniques rather than results, although results are incorporated wherever they provide examples which illustrate the measurement features. The chapters first cover techniques relating to measurements of neutral dynamics and chemistry, then measurements of the various intermittent and excessive radiation sources which effect the middle atmospheric environment, and finally measurements of the plasma environment including electric fields. The weighting toward plasma related parameters is not accidental, but reflects both the historical headstart given by early development of radio wave and probe techniques to measure electron density, and by the relatively limited number of techniques available for neutral atmospheric measurements.

Goldberg, R. A.↗

Warm neutral halos around molecular clouds. V - OH (1665 and 1667 MHz) observations

Ten strip maps of 1665- and 1667-MHz OH emission, traversing the outer boundaries of five molecular clouds, were made. The OH emission is found to be significantly extended relative to CO, from which it inferred that OH is to be found in abundance in the shell of partly atomic, partly molecular gas surrounding the dense molecular clouds. The fractional OH abundance is calculated using existing H I and CO observations, and detailed source models which include a complete chemistry network and a radiative transfer code. It is concluded that the extended OH is formed, not by the exothermic reaction of O with H3(+), but by the endothermic reaction, H(+) + O yields H + O(+).

Wannier, Peter G.↗

Dynamics and Properties of Global Aerosol using MODIS, AERONET and GOCART Model

Recently produced daily Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol data for the whole year of 2001 are used to show the concentration and dynamics of aerosol over ocean and large parts of the continents. The data were validated against the Aerosol Robotic Network (AERONET) measurements over land and ocean in a special issue in GRL now in press. Monthly averages and a movie based on the daily data are produced and used to demonstrate the spatial and temporal evolution of aerosol. The MODIS wide spectral range is used to distinguish fine smoke and pollution aerosol from coarse dust and salt. The aerosol is observed above ocean and land. The movie produced from the MODIS data provides a new dimension to aerosol observations by showing the dynamics of the system. For example in February smoke and dust emitted from the Sahel and West Africa is shown to travel to the North-East Atlantic. In April heavy dust and pollution from East Asia is shown to travel to North America. In May-June pollution and dust play a dynamical dance in the Arabian Sea and Bay of Bengal. In Aug-September smoke from South Africa and South America is shown to pulsate in tandem and to periodically to be transported to the otherwise pristine Southern part of the Southern Hemisphere. The MODIS data are compared with the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation Transport (GOCART) model to test and adjust source and sink strengths in the model and to study the effect of clouds on the representation of the satellite data.

Kaufman, Yoram↗