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Microbial biomass and productivity in seagrass beds

Different methods for measuring the rates of processes mediated by bacteria in sediments and the rates of bacterial cell production have been compared. In addition, net production of the seagrass Zostera capricorni and bacterial production have been compared and some interrelationships with the nitrogen cycle discussed. Seagrass productivity was estimated by measuring the plastochrone interval using a leaf stapling technique. The average productivity over four seasons was 1.28 +/- 0.28 g C m-2 day-1 (mean +/- standard deviation, n = 4). Bacterial productivity was measured five times throughout a year using the rate of tritiated thymidine incorporated into DNA. Average values were 33 +/- 12 mg C m-2 day-1 for sediment and 23 +/- 4 for water column (n = 5). Spatial variability between samples was greater than seasonal variation for both seagrass productivity and bacterial productivity. On one occasion, bacterial productivity was measured using the rate of 32P incorporated into phospholipid. The values were comparable to those obtained with tritiated thymidine. The rate of sulfate reduction was 10 mmol SO4(-2) m-2 day-1. The rate of methanogenesis was low, being 5.6 mg CH4 produced m-2 day-1. A comparison of C flux measured using rates of sulfate reduction and DNA synthesis indicated that anaerobic processes were predominant in these sediments. An analysis of microbial biomass and community structure, using techniques of phospholipid analysis, showed that bacteria were predominant members of the microbial biomass and that of these, strictly anaerobic bacteria were the main components. Ammonia concentration in interstitial water varied from 23 to 71 micromoles. Estimates of the amount of ammonia required by seagrass showed that the ammonia would turn over about once per day. Rapid recycling of nitrogen by bacteria and bacterial grazers is probably important.

NASA Program CELSS↗

Formation of ferrihydrite and associated iron corrosion products in permeable reactive barriers of zero-valent iron

Ferrihydrite, which is known to form in the presence of oxygen and to be stabilized by the adsorption of Si, PO4 and SO4, is ubiquitous in the fine-grained fractions of permeable reactive barrier (PRB) samples from the U.S. Coast Guard Support Center (Elizabeth City, NC) and the Denver Federal Center (Lakewood, CO) studied by high-resolution transmission electron microscopy and selected area electron diffraction. The concurrent energy-dispersive X-ray data indicate a strong association between ferrihydrite and metals such as Si, Ca, and Cr. Magnetite, green rust 1, aragonite, calcite, mackinawite, greigite and lepidocrocite were also present, indicative of a geochemical environment that is temporally and spatially heterogeneous. Whereas magnetite, which is known to form due to anaerobic Fe0 corrosion, passivates the Fe0 surface, ferrihydrite precipitation occurs away from the immediate Fe0 surface, forming small (<0.1 microm) discrete clusters. Consequently, Fe0-PRBs may remain effective for a longer period of time in slightly oxidized groundwater systems where ferrihydrite formation occurs compared to oxygen-depleted systems where magnetite passivation occurs. The ubiquitous presence of ferrihydrite suggests that the use of Fe0-PRBs may be extended to applications that require contaminant adsorption rather than, or in addition to, redox-promoted contaminant degradation.

Metals/chemistry↗

Aerosol Chemical Composition in Asian Continental Outflow during the TRACE-P Campaign: Comparison with PEM-West B

Aerosol associated soluble ions and the radionuclide tracers (7)Be and (210)Pb were quantified in 414 filter samples collected in spring 2001 from the DC-8 during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign. Binning the data into near Asia (flights from Hong Kong and Japan) and remote Pacific (all other flights) revealed large enhancements of NO3(-), SO4(-), C2O4(-), NH4(+), K(+), Mg2(+), and Ca2(+) near Asia. The boundary layer and lower troposphere were most strongly influenced by continental outflow, and the largest enhancements were seen in Ca2(+) (a dust tracer) and NO3(-) (reflecting uptake of HNO3 onto the dust). Comparing the TRACE P near Asia bin with earlier results from the same region during PEM-West B (in 1994) shows at least twofold enhancements during TRACE P in most of the ions listed above. Calcium and NO3(-) were most enhanced in this comparison as well (more than sevenfold higher in the boundary layer and threefold higher in the lower troposphere). Independent estimation of Asian emissions of gaseous precursors of the aerosol-associated ions suggest only small changes between the two missions, and precipitation fields do not suggest any significant difference in the efficiency of the primary sink, precipitation scavenging. It thus appears that with the possible exception of dust, the enhancements of aerosol-associated species during TRACE P cannot be explained by stronger sources or weaker sinks. We argue that the enhancements largely reflect the fact that TRACE P focused on characterizing Asian outflow, and thus the DC-8 was more frequently flown into regions that were influenced by well-organized flow off the continent.

Dibb, Jack E.↗

Chemical Composition of Asian Continental Outflow over the Western Pacific: Results from Transport and Chemical Evolution over the Pacific (TRACE-P)

We characterize the chemical composition of Asian continental outflow observed during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) mission during February-April 2001 in the western Pacific using data collected on the NASA DC-8 aircraft. A significant anthropogenic impact was present in the free troposphere and as far east as 150degE longitude reflecting rapid uplift and transport of continental emissions. Five-day backward trajectories were utilized to identify five principal Asian source regions of outflow: central, coastal, north-northwest(NNW), southeast (SE), and west-southwest (WSW). The maximum mixing ratios for several species, such as CO, C2Cl4, CH3Cl, and hydrocarbons, were more than a factor of 2 larger in the boundary layer of the central and coastal regions due to industrial activity in East Asia. CO was well correlated with C2H2, C2H6, C2Cl4, and CH3Cl at low altitudes in these two regions (r(sup 2) approx. 0.77-0.97). The NNW, WSW, and SE regions were impacted by anthropogenic sources above the boundary layer presumably due to the longer transport distances of air masses to the western Pacific. Frontal and convective lifting of continental emissions was most likely responsible for the high altitude outflow in these three regions. Photochemical processing was influential in each source region resulting in enhanced mixing ratios of O3, PAN, HNO3, H2O2, and CH3OOH. The air masses encountered in all five regions were composed of a complex mixture of photcrchemically aged air with more recent emissions mixed into the outflow as indicated by enhanced hydrocarbon ratios (C2H2/CO greater than or equal to 3 and C3H8/C2H6 greater than or equal to 0.2). Combustion, industrial activities, and the burning of biofuels and biomass all contributed to the chemical composition of air masses from each source region as demonstrated by the H6, SO2, and C2Cl4 were compared for the TRACE-P and PEM-West B missions. In the more northern regions, O3, CO, and SO2 were higher at low altitudes during TRACE-P. In general, mixing ratios were fairly similar between the two missions in the southern regions. A comparison between CO/CO2, CO/CH4, C2H6/C3H8, NO(x)/SO2, and NO(y)/(SO2 + nss-SO4) ratios for the five source regions and for the 2000 Asian emissions summary showed vay close agreement indicating that Asian emissions were well represented by the TRACE-P data and tbe emissions inventory.

Russo, R. S.↗

Metabolic Reactions among Organic Sulfur Compounds

Sulfur is central to the metabolisms of many organisms that inhabit extreme environments. Numerous authors have addressed the energy available from a variety of inorganic sulfur redox pairs. Less attention has been paid, however, to the energy required or gained from metabolic reactions among organic sulfur compounds. Work in this area has focused on the oxidation of alkyl sulfide or disulfide to thiol and formaldehyde, e.g. (CH3)2S + H2O yields CH3SH + HCHO + H2, eventually resulting in the formation of CO2 and SO4(-2). It is also found that reactions among thiols and disulfides may help control redox disequilibria between the cytoplasm and the periplasm. Building on our earlier efforts for thiols, we have compiled and estimated thermodynamic properties for alkyl sulfides. We are investigating metabolic reactions among various sulfur compounds in a variety of extreme environments, ranging from sea floor hydrothermal systems to organic-rich sludge. Using thermodynamic data and the revised HKF equation of state, along with constraints imposed by the geochemical environments sulfur-metabolizing organisms inhabit, we are able to calculate the amount of energy available to these organisms.

Schulte, M.↗

Generation and Performance of Automated Jarosite Mineral Detectors for Vis/NIR Spectrometers at Mars

Sulfate salt discoveries at the Eagle and Endurance craters in Meridiani Planum by the Mars Exploration Rover Opportunity have proven mineralogically the existence and involvement of water in Mars past. Visible and near infrared spectrometers like the Mars Express OMEGA, the Mars Reconnaissance Orbiter CRISM and the 2009 Mars Science Laboratory Rover cameras are powerful tools for the identification of water-bearing salts and other high priority minerals at Mars. The increasing spectral resolution and rover mission lifetimes represented by these missions currently necessitate data compression in order to ease downlink restrictions. On board data processing techniques can be used to guide the selection, measurement and return of scientifically important data from relevant targets, thus easing bandwidth stress and increasing scientific return. We have developed an automated support vector machine (SVM) detector operating in the visible/near-infrared (VisNIR, 300-2500 nm) spectral range trained to recognize the mineral jarosite (typically KFe3(SO4)2(OH)6), positively identified by the Mossbauer spectrometer at Meridiani Planum. Additional information is included in the original extended abstract.

Gilmore, M. S.↗

Fundamental Mvssbauer Parameters of Hydrous Iron Sulfates

Hydrous iron sulfates, which form as alteration products of sulfides, are rare on Earth. On Mars, the low temperature and pH found in the martian permafrost create ideal conditions for the formation of this group of minerals [1], which includes such phases as coquimbite (Fe2(SO4) 9H2O) and amarantite (FeSO4(OH) 3H2O). Viking, Mars Pathfinder, MER and OMEGA data [e.g., [2]] have all indicated the presence of high sulfur contents on the surface of Mars, but the mineralogy of the sulfur-rich phases has not been well constrained. Recent work by [3] suggests that hydrous iron sulfates might satisfy the Martian thermal emission, vis-near IR, and M ssbauer spectra. These data suggest that sulfide and sulfate minerals might be significant contributors to all types of spectra acquired on the Martian surface.

Rothstein, Y.↗

Summertime Influence of Asian Pollution in the Free Troposphere over North America

We analyze aircraft observations obtained during INTEX-A (1 July 14 - August 2004) to examine the summertime influence of Asian pollution in the free troposphere over North America. By applying correlation analysis and Principal Component Analysis (PCA) to the observations between 6-12 km, we find dominant influences from recent convection and lightning (13 percent of observations), Asia (7 percent), the lower stratosphere (7 percent), and boreal forest fires (2 percent), with the remaining 71 percent assigned to background. Asian airmasses are marked by high levels of CO, O3, HCN, PAN, acetylene, benzene, methanol, and SO4(2-). The partitioning of reactive nitrogen species in the Asian plumes is dominated by peroxyacetyl nitrate (PAN) (approximately 600 pptv), with varying NO(x)/HNO3 ratios in individual plumes consistent with different plumes ages ranging from 3 to 9 days. Export of Asian pollution in warm conveyor belts of mid-latitude cyclones, deep convection, and lifting in typhoons all contributed to the five major Asian pollution plumes. Compared to past measurement campaigns of Asian outflow during spring, INTEX-A observations display unique characteristics: lower levels of anthropogenic pollutants (CO, propane, ethane, benzene) due to their shorter summer lifetimes; higher levels of biogenic tracers (methanol and acetone) because of a more active biosphere; as well as higher levels of PAN, NO(x), HNO3, and O3 (more active photochemistry possibly enhanced by injection of lightning NO(x)). The high delta O3/delta CO ratio (0.76 mol mol(exp -1)) of Asian plumes during INTEX-A is due to a combination of strong photochemical production and mixing with stratospheric air along isentropic surfaces. The GEOS-Chem global chemical transport model captures the timing and location of the Asian plumes remarkably well. However, it significantly underestimates the magnitude of the enhancements.

Liang, Q.↗

Fluid-Evaporation Records Preserved in Meridiani Rocks

We have shown earlier that the high SO3/Cl ratios found in secondary mineral assemblages in shergottite GRIM glasses (Gas-Rich Impact-Melt) likely resulted from interactions of regolith materials with sulfate-rich (and Cl-poor) solutions. The low SO3/Cl ratios determined in secondary salts in nakhalite fracture-fillings presumably formed by rock interactions with chloride-rich (and SO4-poor) solutions near Mars surface. The SO3 and Cl abundances determined by APXS in abraded rocks (RAT) from Endurance, Fram and Eagle craters indicate that these salt assemblages likely formed by evaporative concentration of brine fluids at Meridiani. The SO3/Cl ratios in the abraded rocks are examined here, instead of their absolute abundances, because the abundance ratios might provide better guide-lines for tracking the evolution of evaporating fluids at Meridiani. The SO3/Cl ratios in these samples, in turn, might provide clues for the mobile element ratios of the altering fluids that infiltrated into the Meridiani rocks.

Rao, M. N.↗

Jarosite in the Shergottite Que 94201

Veins of the hydroxylated, potassium ferric sulfate mineral jarosite - KFe3(SO4)2(OH)6 - have been identified in the martian meteorite Queen Alexandra Range (QUE) 94201. Iron potassium sulfate had been reported in QUE 94201 by Wentworth and Gooding. Jarosite has been reported in other Martian meteorites - Roberts Massif (RBT) 04262, Miller Range (MIL) 03346, and Yamato 000593 - and it has been identified on the Martian surface by Moessbauer spectroscopy. Given the presence of jarosite on Mars, and the burgeoning interest in water-rock interactions on Mars, the question arises whether jarosite in Martian meteorites is formed by aqueous alteration on Mars, or in Antarctica. Hydrogen isotopes are potentially sensitive indicators of the site of formation or last equilibration of hydrous alteration minerals, because of the large difference between D/H ratio of the Martian atmosphere (and also presumably the cryosphere) and terrestrial hydrogen. The Martian atmospheric delta D(sub SMOW) ratio is approximately +4200%o, igneous minerals with substantial hydrogen (phosphates) have high D, ~ +2000%o to +4700%o versus terrestrial waters with approximately 480%o to +130%o. The crystal chemistry and structure of jarosite are reviewed in Papi ke et al. Here we report hydrogen isotopes measured in jarosite in QUE 94201 by ion microprobe, and also report on the major element composition of jarosite measured by electron microprobe.

Ross, D. K.↗

Thermal Reactions Between Sulfur Dioxide and H202 and Their Relevance to the Jovian Icy Satellites and Other Small Bodies

Laboratory experiments have demonstrated that magnetospheric radiation in the Jovian system drives reaction chemistry in ices at temperatures relevant to Europa and other icy satellites. Here we present new results on thermally-induced reactions occurring between 50 and 130 K in solid H2O + H2O2 + SO2 samples. In our studies, we find that warming our three component mixtures induces a thermal reaction that produces SO4(2-), and this reaction appears to consume equal amounts of H2O2 and SO2. We suspect that the results may explain some of the observations related to the presence and distribution H2O2 across Europa's surface as well as the lack of H2O2 on Ganymede and Callisto. If other molecules prove to be reactive with H2O2 at these or at even lower temperatures, then it may also explain why H2O2 has been absent from surfaces of many of the small icy bodies that are known to be exposed to ionizing radiation.

Loefler, Mark J.↗

Characteristics and Composition of Atmospheric Aerosols in Phimai, Central Thailand During BASE-ASIA

Popular summary: Atmospheric aerosols play an important role in the Earth's climate system, and can also have adverse effects on air quality and human health. The environmental impacts of aerosols, on the other hand, are highly regional, since their temporal/spatial distribution is inhomogeneous and highly depends on the regional emission sources. To better understand the effects of aerosols, intensive field experiments are necessary to characterize the chemical and physical properties on a region-by-region basis. From late February to early May in 2006, NASA/GSFC's SMARTLabs facility was deployed at a rural site in central Thailand, Southeast Asia, to conduct a field experiment dubbed BASE-ASIA (Biomass-burning Aerosols in South East-Asia: Smoke Impact Assessment). The group was joined by scientists from the University of Hawaii and other regional institutes. Comprehensive measurements were made during the experiment, including aerosol chemical composition, optical and microphysical properties, as well as surface energetics and local . meteorology. This study analyzes part of the data from the BASE-ASIA experiment. It was found that, even for the relatively remote rural site, the aerosol loading was still substantial. Besides agricultural burning in the area, industrial pollution near the Bangkok metropolitan area, about 200 km southeast of the site, and even long-range transport from China, also contribute to the area's aerosol loading. The results indicate that aerosol pollution has developed into a regional problem for northern Indochina, and may become more severe as the region's population and economy continue to grow. Abstract: Comprehensive measurements of atmospheric aerosols were made in Phimai, central Thailand (15.l83 N, 102.565 E, elevation: 206 m) during the BASE-ASIA field experiment from late February to early May in 2006. The observed aerosol loading was sizable for this rural site (mean aerosol scattering: 108 +/- 64 Mm(exp -1); absorption: 15 +/- 8 Mm(exp -1); PM(sub 10) concentration: 33 +/- 17 miro-g/ cubic m and dominated by submicron particles. Major aerosol compounds included carbonaceous (OC: 9.5 +/- 3.6miro-g/ cubic m; EC: 2.0 2.3 miro-g/ cubic m and secondary species (SO4(2-): 6.4 +/- 3.7 miro-g/ cubic m, NH4(+): 2.2 +/- 1.3 miro-g/ cubic m). While the site was seldom under the direct influence of large forest fires to its north, agricultural fires were ubiquitous during the experiment, as suggested by the substantial concentration of K+ (0.56 +/- 0.33 micro-g/ cubic m). Besides biomass burning, aerosols in Phimai during the experiment were also strongly influenced by industrial and vehicular emissions from the Bangkok metropolitan region and long-range transport from southern China. High humidity played an important role in determining the aerosol composition and properties in the region. Sulfate was primarily formed via aqueous phase reactions, and hygroscopic growth could enhance the aerosol light scattering by up to 60%, at the typical morning RH level of 85%. The aerosol single scattering albedo demonstrated distinct diurnal variation, ranging from 0.86 +/- 0.04 in the evening to 0.92 +/- 0.02 in the morning. This experiment marks the first time such comprehensive characterization of aerosols was made for rural central Thailand. Our results indicate that aerosol pollution has developed into a regional problem for northern Indochina, and may become more severe as the region's population and economy continue to grow.

Li, Can↗

Radiolysis of Sulfuric Acid, Sulfuric Acid Monohydrate, and Sulfuric Acid Tetrahydrate and Its Relevance to Europa

We report laboratory studies on the 0.8 MeV proton irradiation of ices composed of sulfuric acid (H2SO4), sulfuric acid monohydrate (H2SO4 H2O), and sulfuric acid tetrahydrate (H2SO4 4H2O) between 10 and 180 K. Using infrared spectroscopy, we identify the main radiation products as H2O, SO2, (S2O3)x, H3O+, HSO4(exp -), and SO4(exp 2-). At high radiation doses, we find that H2SO4 molecules are destroyed completely and that H2SO4 H2O is formed on subsequent warming. This hydrate is significantly more stable to radiolytic destruction than pure H2SO4, falling to an equilibrium relative abundance of 50% of its original value on prolonged irradiation. Unlike either pure H2SO4 or H2SO4 H2O, the loss of H2SO4 4H2O exhibits a strong temperature dependence, as the tetrahydrate is essentially unchanged at the highest irradiation temperatures and completely destroyed at the lowest ones, which we speculate is due to a combination of radiolytic destruction and amorphization. Furthermore, at the lower temperatures it is clear that irradiation causes the tetrahydrate spectrum to transition to one that closely resembles the monohydrate spectrum. Extrapolating our results to Europa s surface, we speculate that the variations in SO2 concentrations observed in the chaotic terrains are a result of radiation processing of lower hydration states of sulfuric acid and that the monohydrate will remain stable on the surface over geological times, while the tetrahydrate will remain stable in the warmer regions but be destroyed in the colder regions, unless it can be reformed by other processes, such as thermal reactions induced by diurnal cycling.

Loeffler, M. J.↗

Descent with Modification: Thermal Reactions of Subsurface H2O2 of Relevance to Icy Satellites and Other Small Bodies

Laboratory experiments have demonstrated that magnetospheric radiation in the Jovian system drives reaction chemistry in ices at temperatures relevant to Europa and other icy satellites. Similarly, cosmic radiation (mainly protons) acting on cometary and interstellar ices can promote extensive chemical change. Among the products that have been identified in irradiated H20-ice is hydrogen peroxide (H202), which has been observed on Europa and is suspected on other worlds. Although the infrared spectra and radiation chemistry of H2O2-containing ices are well documented, the thermally-induced solid-phase chemistry of H2O2 is largely unknown. Therefore, in this presentation we report new laboratory results on reactions at 50 - 130 K in ices containing H2O2 and other molecules, both in the presence and absence of H2O. As an example of our results, we find that warming H2O + H2O2 + SO2 ices promotes SO2 oxidation to SO4(2-). We suspect that such redox chemistry may explain some of the observations related to the presence and distribution of H2O2 across Europa's surface as well as the lack of H2O2 on Ganymede and Callisto. If other molecules prove to be just as reactive with frozen H2O2 then it may explain why H2O2 has been absent from surfaces of many of the small icy bodies that are known to be exposed to ionizing radiation. Our results also have implications for the survival of H2O2 as it descends towards a subsurface ocean on Europa.

Hudson, Reggie L.↗

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↗

Evaluating Ammonium, Nitrate and Sulfate Aerosols in 3-Dimensions

The effect aerosols have on climate and air quality is a func-on of their chemical composi-on, concentra-on and spa-al distribu-on. These parameters are controlled by emissions, heterogeneous and homogeneous chemistry, where thermodynamics plays a key role, transport, which includes stratospheric-­‐ tropospheric exchange, and deposi-onal sinks. In this work we demonstrate the effect of some of these processes on the SO4‐NH4­‐NO3 system using the GISS ModelE2 Global Circula-on Model (GCM).

Aerosols↗

Daily Ambient Air Pollution Metrics for Five Cities: Evaluation of Data Fusion-Based Estimates and Uncertainties

Spatiotemporal characterization of ambient air pollutant concentrations is increasingly relying on the combination of observations and air quality models to provide well-constrained, spatially and temporally complete pollutant concentration fields. Air quality models, in particular, are attractive, as they characterize the emissions, meteorological, and physiochemical process linkages explicitly while providing continuous spatial structure. However, such modeling is computationally intensive and has biases. The limitations of spatially sparse and temporally incomplete observations can be overcome by blending the data with estimates from a physically and chemically coherent model, driven by emissions and meteorological inputs. We recently developed a data fusion method that blends ambient ground observations and chemical transport-modeled (CTM) data to estimate daily, spatially resolved pollutant concentrations and associatedcorrelations. In this study, we assess the ability of the data fusion method to produce daily metrics (i.e., 1-hr max, 8-hr max, and 24-hr average) of ambient air pollution that capture spatiotemporal air pollution trends for 12 pollutants (CO, NO2, NOx, O3, SO2, PM (sub10), PM (sub 2.5), and five PM (sub 2.5) components) across five metropolitan areas (Atlanta, Birmingham, Dallas, Pittsburgh, and St. Louis), from 2002 to 2008. Three sets of comparisons are performed: (1) the CTM concentrations are evaluated for each pollutant and metropolitan domain, (2) the data fusion concentrations are compared with the monitor data, (3) a comprehensive cross-validation analysis against observed data evaluates the quality of the data fusion model simulations across multiple metropolitan domains. The resulting daily spatial field estimates of air pollutant concentrations and uncertainties are not only consistent with observations, emissions, andmeteorology, but substantially improve CTM-derived results for nearly all pollutants and all cities, with the exception of NO2 for Birmingham. The greatest improvements occur for O3 and PM (sub 2.5). Squared spatiotemporal correlation coefficients range between simulations and observations determined using cross-validation across all cities for air pollutants of secondary and mixed origins are R-squared equal to 0.88-0.93 (O3), 0.81-0.89 (SO4), 0.67-0.83 (PM (sub 2.5)), 0.52-0.72 (NO3), 0.43-0.80 (NH4), 0.32-0.51 (OC), and 0.14-0.71 (PM (sub 10)). Results for relatively homogeneous pollutants of secondary origin, tend to be better than those for more spatially heterogeneous (larger spatial gradients) pollutants of primary origin (NOx, CO, SO2 and EC). Generally, background concentrations and spatial concentration gradients reflect interurban airshed complexity and the effects of regional transport, whereas daily spatial pattern variability shows intra urban consistency in the fused data. With sufficiently high CTM spatial resolution, traffic-related pollutants exhibit gradual concentration gradients that peak toward the urban centers. Ambient pollutant concentration uncertainty estimates for the fused data are both more accurate and smaller than those for either the observations or the model simulations alone.

spatiotemporal fusion↗

FUTURE LEVELS OF AEROSOLS & RADIATIVE FORCING OVER THE ARCTIC

The Arctic Monitoring and Assessment Programme (AMAP) is currently assessing the impacts of Short-Lived Climate Forcers (SLCF) on Arctic climate and air quality. In support of the assessment, we used the NASA Goddard Institute of Space Sciences (GISS) Earth System Model (modelE2.1), with prescribed sea surface temperature and sea-ice fraction, to simulate SLCF concentrations globally between 1995 and 2015. Two simulations were conducted, using the One-Moment Aerosol (OMA) and the Multiconfiguration Aerosol TRacker of mIXing state (MATRIX) aerosol modules. OMA is a mass-based scheme in which aerosols are assumed to remain externally mixed and have a prescribed and constant size distribution, while MATRIX is an aerosol microphysics scheme based on the quadrature method of moments, which is able to explicitly simulate the mixing state of aerosols. Anthropogenic emissions from the ECLIPSE v6b emissions database were used, along with emissions from aircrafts and open biomass burning from the Coupled Model Intercomparison Project Phase 6 (CMIP6), while the natural emissions of sea salt, DMS, isoprene and dust are calculated interactively. The simulated monthly surface concentrations of sulfate (SO4), black carbon (BC), organic carbon (OA), and ozone (O3) are compared with observations from a set of Arctic stations, extracted from the EBAS and IMPROVE databases, as well as a few additional locations. Simulated aerosol optical depths (AOD) are also compared with Advanced Very-High Resolution Radiometer (AVHRR). The study will present the evaluation of the modelE2.1 in simulating SLCF levels over the Arctic using different aerosol schemes, along with observed and simulated trends of SLCFs over the Arctic between 1995 and 2015.

Aersosols↗