Science.gov

Sample records for estimate atmospheric sulfur

  1. Atmospheric Sulfur Hexafluoride: Measurements and Emission Estimates from 1970 - 2008

    NASA Astrophysics Data System (ADS)

    Rigby, M. L.; Prinn, R. G.; Muhle, J.; Miller, B. R.; Dlugokencky, E. J.; Krummel, P. B.; Steele, L. P.; Fraser, P. J.; Leist, M.; Weiss, R. F.; Harth, C. M.; O'Doherty, S. J.; Greally, B. R.; Simmonds, P. G.; Derek, N.; Vollmer, M. K.; Kim, J.; Kim, K.; Porter, L. W.

    2009-12-01

    We present an air history of atmospheric sulfur hexafluoride (SF6) from the early 1970s through 2008. During this period, concentrations of this extremely potent and long-lived greenhouse gas have increased by more than an order of magnitude, and its growth has accelerated in recent years. In this study, historical concentrations are determined from archived air samples measured on the Advanced Global Atmospheric Gases Experiment (AGAGE) ‘Medusa’ gas chromatography/mass spectrometry system. These data are combined with modern high-frequency measurements from the AGAGE and National Oceanic and Atmospheric Administration (NOAA) in situ networks and ˜weekly samples from the NOAA flask network, to produce a unique time series with increasing global coverage spanning almost four decades. Using the three-dimensional chemical transport Model for Ozone and Related Tracers (MOZART v4.5) and a discrete Kalman filter, we derive estimates of the annual emission strength of SF6 on hemispheric scales from 1970 - 2004 and on continental scales from 2004 - 2008. Our emission estimates are compared to the recently compiled Emissions Database for Global Atmospheric Research (EDGAR v4), and emissions reported under the United Nations Framework Convention on Climate Change (UNFCCC). The cause of the recent growth rate increase is also investigated, indicating that the origin of the required emissions rise is likely to be South-East Asia.

  2. Chlorine, fluorine, and sulfur emissions from Mount Erebus, Antarctica and estimated contributions to the Antarctic atmosphere

    NASA Astrophysics Data System (ADS)

    Zreda-Gostynska, Grazyna; Kyle, Philip R.; Finnegan, David L.

    1993-09-01

    The discharge rates of halogens in aerosols and gases emitted from Mount Erebus between December 1986 and January 1991 were estimated by combining element-to-sulfur ratios on filter samples with SO2 output measured by COSPEC. The halogen and sulfur content of the gas vary in a quasi-cyclical pattern possibly because of a heterogeneous distribution of volatiles in the Erebus magmatic system. The emission rates of HF and HCl have increased twofold since 1986 reaching 6 and 13.3 Gg/yr, respectively, in 1991, making Erebus an important contributor of halogens to the Antarctic atmosphere.

  3. Estimates of the atmospheric deposition of sulfur and nitrogen species: Clean Air Status and Trends Network 1990-2000.

    PubMed

    Baumgardner, Ralph E; Lavery, Thomas F; Rogers, Christopher M; Isil, Selma S

    2002-06-15

    The Clean Air Status and Trends Network (CASTNet) was established by the U.S. EPA in response to the requirements of the 1990 Clean Air Act Amendments. To satisfy these requirements CASTNet was designed to assess and report on geographic patterns and long-term, temporal trends in ambient air pollution and acid deposition in order to gauge the effectiveness of current and future mandated emission reductions. This paper presents an analysis of the spatial patterns of deposition of sulfur and nitrogen pollutants for the period 1990-2000. Estimates of deposition are provided for two 4-yr periods: 1990-1993 and 1997-2000. These two periods were selected to contrast deposition before and after the large decrease in SO2 emissions that occurred in 1995. Estimates of dry deposition were obtained from measurements at CASTNet sites combined with deposition velocities that were modeled using the multilayer model, a 20-layer model that simulates the various atmospheric processes that contribute to dry deposition. Estimates of wet deposition were obtained from measurements at sites operated bythe National Atmospheric Deposition Program. The estimates of dry and wet deposition were combined to calculate total deposition of atmospheric sulfur (dry SO2, dry and wet SO4(2-)) and nitrogen (dry HNO3, dry and wet NO3-, dry and wet NH4+). An analysis of the deposition estimates showed a significant decline in sulfur deposition and no change in nitrogen deposition. The highest rates of sulfur deposition were observed in the Ohio River Valley and downwind states. This region also observed the largest decline in sulfur deposition. The highest rates of nitrogen deposition were observed in the Midwest from Illinois to southern New York State. Sulfur and nitrogen deposition fluxes were significantly higher in the eastern United States as compared to the western sites. Dry deposition contributed approximately 38% of total sulfur deposition and 30% of total nitrogen deposition in the eastern

  4. Ahead of his time: Jacob Lipman's 1930 estimate of atmospheric sulfur deposition for the conterminous United States

    USGS Publications Warehouse

    Landa, Edward R.; Shanley, James B.

    2015-01-01

    A 1936 New Jersey Agricultural Experiment Station Bulletin provided an early quantitative assessment of atmospheric deposition of sulfur for the United States that has been compared in this study with more recent assessments. In the early 20th century, anthropogenic sulfur additions from the atmosphere to the soil by the combustion of fossil fuels were viewed as part of the requisite nutrient supply of crops. Jacob G. Lipman, the founding editor of Soil Science, and his team at Rutgers University, made an inventory of such additions to soils of the conterminous United States during the economic depression of the 1930s as part of a federally funded project looking at nutrient balances in soils. Lipman's team gathered data compiled by the US Bureau of Mines on coal and other fuel consumption by state and calculated the corresponding amounts of sulfur emitted. Their work pioneered a method of assessment that became the norm in the 1970s to 1980s—when acid rain emerged as a national issue. Lipman's estimate of atmospheric sulfur deposition in the 1930 is in reasonable agreement with recent historic reconstructions.

  5. Estimating Sulfur hexafluoride (SF6) emissions in China using atmospheric observations and inverse modeling

    NASA Astrophysics Data System (ADS)

    Fang, X.; Thompson, R.; Saito, T.; Yokouchi, Y.; Li, S.; Kim, J.; Kim, K.; Park, S.; Graziosi, F.; Stohl, A.

    2013-12-01

    With a global warming potential of around 22800 over a 100-year time horizon, sulfur hexafluoride (SF6) is one of the greenhouse gases regulated under the Kyoto Protocol. Global SF6 emissions have been increasing since circa the year 2000. The reason for this increase has been inferred to be due to rapidly increasing emissions in developing countries that are not obligated to report their annual emissions to the United Nations Framework Convention on Climate Change, notably China. In this study, SF6 emissions during the period 2006-2012 for China and other East Asian countries were determined using in-situ atmospheric measurements and inverse modeling. We performed various inversion sensitivity tests, which show the largest uncertainties in the a posteriori Chinese emissions are associated with the a priori emissions used and their uncertainty, the station network, as well as the meteorological input data. The overall relative uncertainty of the a posteriori emissions in China is estimated to be 17% in 2008. Based on sensitivity tests, we employed the optimal parameters in our inversion setup and performed yearly inversions for the study period. Inversion results show that the total a posteriori SF6 emissions from China increased from 1420 × 245 Mg/yr in 2006 to 2741 × 472 Mg/yr in 2009 and stabilized thereafter. The rapid increase in emissions reflected a fast increase in SF6 consumption in China, a result also found in bottom-up estimates. The a posteriori emission map shows high emissions concentrated in populated parts of China. During the period 2006-2012, emissions in northwestern and northern China peaked around the year 2009, while emissions in eastern, central and northeastern China grew gradually during almost the whole period. Fluctuating emissions are observed for southwestern China. These regional differences should be caused by changes of provincial SF6 usage and by shifts of usage among different sectors. Fig. 1. Footprint emission sensitivity

  6. Chlorine, fluorine, and sulfur emissions from Mount Erebus, Antarctica and estimated contributions to the Antarctic atmosphere

    SciTech Connect

    Zreda-Gostynska, G.; Kyle, P.R. ); Finnegan, D.L. )

    1993-09-15

    The authors report a study of the atmospheric release of gases from Mount Erebus, in continental Antarctica, over the period Dec 1986 to Jan 1991. This provides a case study of gas releases in a region of the planet almost devoid of anthropogenic sources. The discharge rates of chlorine, fluorine, and sulfur compounds have been monitored. The emission rates of HF and HCl were observed to double over this period to levels of 6 and 13.3 Gg/yr. Measurements were made from filter paper samples, relative to SO[sub 2] emission rates measured independently of the filter samples.

  7. Can sulfate fluxes in forest canopy throughfall be used to estimate atmospheric sulfur deposition

    SciTech Connect

    Lindberg, S.E.; Garten, C.T. Jr. ); Cape, J.N. ); Ivens, W. )

    1991-01-01

    The flux of sulfate is forest throughfall and stemflow (the sum of which is designated here as TF) may be an indicator of the atmospheric deposition of S, particularly if foliar leaching of internal plant S is small relative to washoff of deposition. Extensive data from 13 forests indicate that annual sulfate fluxes in TF and in atmospheric deposition are very similar, and recent studies with {sup 35}S tracers indicate that leaching is only a few percent of total TF. However, some short-term deposition/TF comparisons show large differences, and there remain questions about interpretation of tracer results. Considering the data, we conclude that TF may be used under some conditions to estimate deposition within acceptable uncertainty limits, but that some assumptions need further testing. If TF does reflect deposition, these data suggest that commonly used methods and models seriously underestimate total S deposition at some sites. 39 refs. ,4 figs., 1 tab.

  8. Sulfur dioxide contributions to the atmosphere by volcanoes.

    PubMed

    Stoiber, R E; Jepsen, A

    1973-11-09

    The first extensive measurements by remote-sensing correlation spectrometry of the sulfur dioxide emitted by volcanic plumes indicate that on the order of 10(3) metric tons of sulfur dioxide gas enter the atmosphere daily from Central American volcanoes. Extrapolation gives a minimum estimate of the annual amount of sulfur dioxide emitted from the world's volcanoes of about 10(7) metric tons.

  9. Pacific Atmospheric Sulfur Experiment (PASE): An Overview

    NASA Astrophysics Data System (ADS)

    Bandy, A. R.; Blomquist, B.; Huebert, B.; Howell, S.; Clarke, T.; Hudson, J.; Faloona, I.; Wang, Y.; Mauldin, R. L.; Heikes, B.; Merrill, J.; O'Sullivan, D.

    2008-12-01

    The Pacific Atmospheric Sulfur Experiment (PASE) was a study of the chemistry of sulfur in a cloud free region of the equatorial Pacific Ocean. The experiment was conducted aboard the NSF C130 just east of Christmas Island during August and early September of 2007 in the prevailing southeasterly trade wind flow. PASE is envisioned as the first of a series of experiments focused on developing an understanding of how the chemistry of sulfur affects climate in general but especially with respect to its impact on cloud chemistry and physics. Being the first of this series, PASE was focused on (but not limited to) clear air to narrow the scope of the science to control costs and to reflect the fact that most of the available instrumentation cannot make effective measurements in clouds. PASE is unique in that it brought together several instruments (SO2, DMS, O3 and H2O) that make measurements fast enough to permit the computation of vertical fluxes by eddy covariance allowing the flux terms in chemical budgets to be determined quantitatively. The PASE instrument payload also made a large suite of slower measurements including but not limited to OH, HO2, RO2, H2SO4, methane sulfonic acid (MSA), H2O2, CH3COOH, thermally resolved CN(>15nm), ultrafine CN (>3 nm), bulk aerosol composition, and cloud condensation nuclei (CCN). The high rate instruments enabled quantification of the vertical exchange that could be generalized to estimate the mixing of the slower analytes. One of the surprising results from PASE was the large and very steady levels of CCN observed throughout the experiment. Furthermore, the vertical gradient indicated that boundary layer venting via shallow convection was a persistent sink of the CCN. Taken in concert the unique data set renders a picture of marine air that has not been purged by precipitation in a long while, allowing it to build up large amounts of volatile sulfur in the condensed phase and providing a superb environment to investigate

  10. New methodology for estimating biofuel consumption for cooking: Atmospheric emissions of black carbon and sulfur dioxide from India

    NASA Astrophysics Data System (ADS)

    Habib, Gazala; Venkataraman, Chandra; Shrivastava, Manish; Banerjee, Rangan; Stehr, J. W.; Dickerson, Russell R.

    2004-09-01

    The dominance of biofuel combustion emissions in the Indian region, and the inherently large uncertainty in biofuel use estimates based on cooking energy surveys, prompted the current work, which develops a new methodology for estimating biofuel consumption for cooking. This is based on food consumption statistics, and the specific energy for food cooking. Estimated biofuel consumption in India was 379 (247-584) Tg yr-1. New information on the user population of different biofuels was compiled at a state level, to derive the biofuel mix, which varied regionally and was 74:16:10%, respectively, of fuelwood, dung cake and crop waste, at a national level. Importantly, the uncertainty in biofuel use from quantitative error assessment using the new methodology is around 50%, giving a narrower bound than in previous works. From this new activity data and currently used black carbon emission factors, the black carbon (BC) emissions from biofuel combustion were estimated as 220 (65-760) Gg yr-1. The largest BC emissions were from fuelwood (75%), with lower contributions from dung cake (16%) and crop waste (9%). The uncertainty of 245% in the BC emissions estimate is now governed by the large spread in BC emission factors from biofuel combustion (122%), implying the need for reducing this uncertainty through measurements. Emission factors of SO2 from combustion of biofuels widely used in India were measured, and ranged 0.03-0.08 g kg-1 from combustion of two wood species, 0.05-0.20 g kg-1 from 10 crop waste types, and 0.88 g kg-1 from dung cake, significantly lower than currently used emission factors for wood and crop waste. Estimated SO2 emissions from biofuels of 75 (36-160) Gg yr-1 were about a factor of 3 lower than that in recent studies, with a large contribution from dung cake (73%), followed by fuelwood (21%) and crop waste (6%).

  11. Accumulation of atmospheric sulfur in some Costa Rican soils

    USGS Publications Warehouse

    Bern, Carleton R.; Townsend, Alan R.

    2013-01-01

    Sulfur is one of the macronutrient elements whose sources to terrestrial ecosystems should shift from dominance by rock-weathering to atmospheric deposition as soils and underlying substrate undergo progressive weathering and leaching. However, the nature and timing of this transition is not well known. We investigated sources of sulfur to tropical rain forests growing on basalt-derived soils in the Osa Peninsula region of Costa Rica. Sulfur sources were examined using stable isotope ratios (δ34S) and compared to chemical indices of soil development. The most weathered soils, and the forests they supported, are dominated by atmospheric sulfur, while a less weathered soil type contains both rock-derived and atmospheric sulfur. Patterns of increasing δ34S with increasing soil sulfur concentration across the landscape suggest atmospheric sulfur is accumulating, and little rock-derived sulfur has been retained. Soil sulfur, minus adsorbed sulfate, is correlated with carbon and nitrogen, implying that sulfur accumulation occurs as plants and microbes incorporate sulfur into organic matter. Only the lower depth increments of the more weathered soils contained significant adsorbed sulfate. The evidence suggests a pattern of soil development in which sulfur-bearing minerals in rock, such as sulfides, weather early relative to other minerals, and the released sulfate is leached away. Sulfur added via atmospheric deposition is retained as organic matter accumulates in the soil profile. Adsorbed sulfate accumulates later, driven by changes in soil chemistry and mineralogy. These aspects of sulfur behavior during pedogenesis in this environment may hasten the transition to dominance by atmospheric sources.

  12. Sulfur Chemistry in the Early and Present Atmosphere of Mars

    NASA Technical Reports Server (NTRS)

    Levine, Joel S.; Summers, M. E.

    2011-01-01

    Atmospheric sulfur species resulting from volcanic emissions impact the composition and chemistry of the atmosphere, impact the climate, and hence, the habitability of Mars and impact the mineralogy and composition of the surface of Mars. The geochemical/ photochemical cycling of sulfur species between the interior (via volcanism), the atmosphere (atmospheric photochemical and chemical processes) and the deposition of sulfuric acid on the surface of Mars is an important, but as yet poorly understood geochemical/ photochemical cycle on Mars. There is no observational evidence to indicate that Mars is volcanically active at the present time, however, there is strong evidence that volcanism was an important and widespread process on early Mars. The chemistry and photochemistry of sulfur species in the early and present atmosphere of Mars will be assessed using a one-dimensional photochemical model. Since it is generally assumed that the atmosphere of early Mars was significantly denser than the present 6-millibar atmosphere, photochemical calculations were performed for the present atmosphere and for the atmosphere of early Mars with assumed surface pressures of 60 and 350-millibars, where higher surface pressure resulted from enhanced atmospheric concentrations of carbon dioxide (CO2). The following sections include the results of earlier modeling studies, a summary of the one-dimensional photochemical model used in this study, a summary of the photochemistry and chemistry of sulfur species in the atmosphere of Mars and some of the results of the calculations.

  13. Heterogeneous atmospheric reactions - Sulfuric acid aerosols as tropospheric sinks

    NASA Technical Reports Server (NTRS)

    Baldwin, A. C.; Golden, D. M.

    1979-01-01

    The reaction probabilities of various atmospheric species incident on a bulk sulfuric acid surface are measured in order to determine the role of sulfuric acid aerosols as pollutant sinks. Reaction products and unreacted starting materials leaving a Knudsen cell flow reactor after collision at 300 K with a H2SO4 surface or a soot surface were detected by mass spectrometry. Significant collision reaction probabilities are observed on a H2SO4 surface for H2O2, HNO3, HO2NO2, ClONO2, N2O5, H2O and NH3, and on soot for NH3. Estimates of the contribution of heterogeneous reactions to pollutant removal under atmospheric conditions indicate that while aerosol removal in the stratosphere is insignificant (loss rate constants approximately 10 to the -10th/sec), heterogeneous reactions may be the dominant loss process for several tropospheric species (loss rate constant approximately 10 to the -5th/sec, comparable to photolysis rate constants).

  14. Atmospheric Sulfur Hexafluoride: Sources, Sinks and Greenhouse Warming

    NASA Technical Reports Server (NTRS)

    Sze, Nien Dak; Wang, Wei-Chyung; Shia, George; Goldman, Aaron; Murcray, Frank J.; Murcray, David G.; Rinsland, Curtis P.

    1993-01-01

    Model calculations using estimated reaction rates of sulfur hexafluoride (SF6) with OH and 0('D) indicate that the atmospheric lifetime due to these processes may be very long (25,000 years). An upper limit for the UV cross section would suggest a photolysis lifetime much longer than 1000 years. The possibility of other removal mechanisms are discussed. The estimated lifetimes are consistent with other estimated values based on recent laboratory measurements. There appears to be no known natural source of SF6. An estimate of the current production rate of SF6 is about 5 kt/yr. Based on historical emission rates, we calculated a present-day atmospheric concentrations for SF6 of about 2.5 parts per trillion by volume (pptv) and compared the results with available atmospheric measurements. It is difficult to estimate the atmospheric lifetime of SF6 based on mass balance of the emission rate and observed abundance. There are large uncertainties concerning what portion of the SF6 is released to the atmosphere. Even if the emission rate were precisely known, it would be difficult to distinguish among lifetimes longer than 100 years since the current abundance of SF6 is due to emission in the past three decades. More information on the measured trends over the past decade and observed vertical and latitudinal distributions of SF6 in the lower stratosphere will help to narrow the uncertainty in the lifetime. Based on laboratory-measured IR absorption cross section for SF6, we showed that SF6 is about 3 times more effective as a greenhouse gas compared to CFC 11 on a per molecule basis. However, its effect on atmospheric warming will be minimal because of its very small concentration. We estimated the future concentration of SF6 at 2010 to be 8 and 10 pptv based on two projected emission scenarios. The corresponding equilibrium warming of 0.0035 C and 0.0043 C is to be compared with the estimated warming due to CO2 increase of about 0.8 C in the same period.

  15. The transport of atmospheric sulfur over Cape Town

    NASA Astrophysics Data System (ADS)

    Jenner, Samantha L.; Abiodun, Babatunde J.

    2013-11-01

    Cape Town, renowned for its natural beauty, is troubled by an unpleasant brown haze pollution, in which atmospheric sulfur plays a major role. This study investigates whether Cape Town is a net producer or recipient of anthropogenic sulfur pollution. In the study, two atmospheric chemistry-transport models (RegCM and WRF) are used to simulate atmospheric flow and chemistry transport over South Africa for two years (2001 and 2002). Both models reproduce the observed seasonal variability in the atmospheric flow and SO2 concentration over Cape Town. The models simulations agree on the seasonal pattern of SO2 over South Africa but disagree on that of SO4. The simulations show that ambient sulfur in Cape Town may be linked with pollutant emissions from the Mpumalanga Highveld, South Africa's most industrialized region. While part of atmospheric SO2 from the Highveld is transported at 700 hPa level toward the Indian Ocean (confirming previous studies), part is transported at low level from the Highveld toward Cape Town. In April, a band of high concentration SO2 extends between the Highveld and Cape Town, following the south coast. Extreme sulfur pollution events in Cape Town are associated with weak flow convergence or stagnant conditions over the city, both of which encourage the accumulation of pollution. However the study suggests that atmospheric sulfur is being advected from Mpumalanga Highveld to Cape Town and this may contribute to atmospheric pollution problems in Cape Town.

  16. Sulfuric acid aerosols in the atmospheres of the terrestrial planets

    NASA Astrophysics Data System (ADS)

    McGouldrick, Kevin; Toon, Owen B.; Grinspoon, David H.

    2011-08-01

    Clouds and hazes composed of sulfuric acid are observed to exist or postulated to have once existed on each of the terrestrial planets with atmospheres in our solar system. Venus today maintains a global cover of clouds composed of a sulfuric acid/water solution that extends in altitude from roughly 50 km to roughly 80 km. Terrestrial polar stratospheric clouds (PSCs) form on stratospheric sulfuric acid aerosols, and both PSCs and stratospheric aerosols play a critical role in the formation of the ozone hole. Stratospheric aerosols can modify the climate when they are enhanced following volcanic eruptions, and are a current focus for geoengineering studies. Rain is made more acidic by sulfuric acid originating from sulfur dioxide generated by industry on Earth. Analysis of the sulfur content of Martian rocks has led to the hypothesis that an early Martian atmosphere, rich in SO 2 and H 2O, could support a sulfur-infused hydrological cycle. Here we consider the plausibility of frozen sulfuric acid in the upper clouds of Venus, which could lead to lightning generation, with implications for observations by the European Space Agency's Venus Express and the Japan Aerospace Exploration Agency's Venus Climate Orbiter (also known as Akatsuki). We also present simulations of a sulfur-rich early Martian atmosphere. We find that about 40 cm/yr of precipitation having a pH of about 2.0 could fall in an early Martian atmosphere, assuming a surface temperature of 273 K, and SO 2 generation rates consistent with the formation of Tharsis. This modeled acid rain is a powerful sink for SO 2, quickly removing it and preventing it from having a significant greenhouse effect.

  17. Atmospheric sulfur deposition and streamwater quality in Finland

    NASA Astrophysics Data System (ADS)

    Lahermo, P. W.; Tarvainen, T.; Tuovinen, J.-P.

    1994-10-01

    The correlation between sulfate concentrations in Finnish headwater streams and atmospheric sulfate deposition has been studied by using data from the streamwater chemistry in August September 1990 and computed S deposition from the anthropogenic emissions. The sulfate concentrations and acidity in water are interpolated and smoothed into a deposition model grid. These data are compared with geological and pedogeochemical (glacial till) background information. The areas where the streamwater SO4 concentrations are mainly controlled by either anthropogenic S deposition or sulfur in till is estimated by applying the fuzzy Gustafsson-Kessel algorithm, which provides a soft clustering suitable for overlapping control factors. Residual areas can be well explained by the SO4-rich Littorina clay deposits. The higher overall background SO4 concentrations in streams in south Finland compared with central and northern Finland are an indisputable consequence of the heavier S deposition load in the south. However, anthropogenic sulfur deposition has a clear correlation with the sulfates in streamwaters only in northeastern Lapland impacted by the large industrial emissions in the Kola Peninsula. The secondary sulfide and sulfate minerals of marine Littorina sediments are dominating sources in the broad coastal belts, as are the primary sulfide minerals locally in the Pori-Vammala area, at the eastern end of the main sulfide ore belt between Lake Ladoga and the Gulf of Bothnia, in the Outokumpu area, and in the Peräpohja and central Lapland schist belts. Consequently, in addition to the anthropogenic deposition, there are natural sources of sulfur which cause acidity of streamwaters.

  18. Homogenous nucleation of sulfuric acid and water at close to atmospherically relevant conditions

    NASA Astrophysics Data System (ADS)

    Brus, D.; Neitola, K.; Hyvärinen, A.-P.; Petäjä, T.; Vanhanen, J.; Sipilä, M.; Paasonen, P.; Kulmala, M.; Lihavainen, H.

    2011-06-01

    In this study the homogeneous nucleation rates in the system of sulfuric acid and water were measured by using a flow tube technique. The goal was to directly compare particle formation rates obtained from atmospheric measurements with nucleation rates of freshly nucleated particles measured with particle size magnifier (PSM) which has detection efficiency of unity for particles having mobility diameter of 1.5 nm. The gas phase sulfuric acid concentration in this study was measured with the chemical ionization mass spectrometer (CIMS), commonly used in field measurements. The wall losses of sulfuric acid were estimated from measured concentration profiles along the flow tube. The initial concentrations of sulfuric acid estimated from loss measurements ranged from 108 to 3 × 109 molecules cm-3. The nucleation rates obtained in this study cover about three orders of magnitude from 10-1 to 102 cm-3 s-1 for commercial ultrafine condensation particle counter (UCPC) TSI model 3025A and from 101 to 104 cm-3 s-1 for PSM. The nucleation rates and the slopes (dlnJ/dln [H2SO4]) show satisfactory agreement when compared to empirical kinetic and activation models and the latest atmospheric nucleation data. To the best of our knowledge, this is the first experimental work providing temperature dependent nucleation rate measurements using a high efficiency particle counter with a cut-off-size of 1.5 nm together with direct measurements of gas phase sulfuric acid concentration.

  19. Connection of sulfuric acid to atmospheric nucleation in boreal forest.

    PubMed

    Nieminen, T; Manninen, H E; Sihto, S L; Yli-Juuti, T; Mauldin, R L; Petäjä, T; Riipinen, I; Kerminen, V M; Kulmala, M

    2009-07-01

    Gas to particle conversion in the boundary layer occurs worldwide. Sulfuric acid is considered to be one of the key components in these new particle formation events. In this study we explore the connection between measured sulfuric acid and observed formation rate of both charged 2 nm as well as neutral clusters in a boreal forest environment A very short time delay of the order of ten minutes between these two parameters was detected. On average the event days were clearly associated with higher sulfuric acid concentrations and lower condensation sink (CS) values than the nonevent days. Although there was not a clear sharp boundary between the nucleation and no-nucleation days in sulfuric acid-CS plane, at our measurement site a typical threshold concentration of 3.10(5) molecules cm(-3) of sulfuric acid was needed to initiate the new particle formation. Two proposed nucleation mechanisms were tested. Our results are somewhat more in favor of activation type nucleation than of kinetic type nucleation, even though our data set is too limited to omit either of these two mechanisms. In line with earlier studies, the atmospheric nucleation seems to start from sizes very close to 2 nm.

  20. Consistency Between Measurements and Theory for Sulfur Gases and Oxidants During the Pacific Atmospheric Sulfur Experiment

    NASA Astrophysics Data System (ADS)

    Heikes, B. G.; Higbie, A.; O'Sullivan, D. W.; Bandy, A. R.; Mauldin, L.; Cantrell, C.; Anderson, R. S.; Campos, T.; Huebert, B.; Bloomquist, B.; Wang, Y.; Heizer, C. G.; Pollack, I. B.; Weinheimer, A. J.

    2008-12-01

    Airborne gas phase measurements of sulfur dioxide, dimethylsulfide, dimethylsulfoxide, methane sulfonic acid, sulfuric acid, hydroxyl, perhydroxyl, hydrogen peroxide, methylhydroperoxide, ozone, and carbon monoxide together with aerosol microphysical properties and bulk and size-dependent aerosol composition are examined for consistency with photochemical theory. The observations come from 14 research flights using the NCAR C-130 flown mostly southeast of Kiritimati in relatively cloud-free marine boundary layer air. This region was chosen because of its extremely low nitrogen oxide mixing ratios and minimal horizontal gradients in composition. A size-dependent gas-particle mass-transfer model is used to calculate the exchange rates of dimethylsulfoxide, methanesulfonic acid and sulfuric acid between the gas and aerosol. Gas kinetic reactions, aqueous reactions, and heterogeneous processes are used in the evaluation. Mass accommodation coefficients, Henry's Law solubilities, and the effective yields of methanesulfonic acid, sulfur dioxide, sulfuric acid and dimethylsulfoxide from dimethylsulfide are estimated and consistent with the literature. Gas phase hydroxyl chemistry alone is sufficient to explain observed methanesulfonic acid and sulfuric acid vapor concentrations.

  1. Thermochemistry of substellar atmospheres: Water, oxygen, sulfur, and phosphorus

    NASA Astrophysics Data System (ADS)

    Visscher, Channon Wayne

    2006-09-01

    Thermochemical equilibrium and kinetic calculations are used to investigate atmospheric chemistry in substellar objects: giant planets, extrasolar giant planets (EGPs), and brown dwarfs. These studies include an assessment of the water and total oxygen inventories in the interiors of Jupiter and Saturn, and detailed modeling of sulfur and phosphorus chemistry in the atmospheres of substellar objects. In the first part of the dissertation, the water and total oxygen abundances in the deep atmospheres of Jupiter and Saturn are determined by considering the effects of H 2 O and O on the chemistry of CO, PH 3 , and SiH 4 . On Jupiter, the observed CO abundance indicates a water abundance of 0.4--1.4 times the protosolar H 2 O/H 2 ratio (8.96 × 10 -4 ). On Saturn, a combination of CO and PH 3 chemical constraints requires a water abundance of 1.9--6.1 times the protosolar abundance. Combining these results with Si mass balance considerations gives a total oxygen abundance of 0.7--1.7 and 3.2--6.4 times the protosolar O/H 2 ratio (1.16 × 10 -3 ) on Jupiter and Saturn, respectively. In both planets, oxygen is less enriched than other heavy elements (such as carbon) relative to hydrogen and the solar system composition. These results provide important constraints for giant planet formation mechanisms and models of tropospheric chemistry. The second part of the dissertation is a detailed study of sulfur and phosphorus chemistry in substellar atmospheres. The chemical behavior of individual S- and P-bearing gases and condensates is determined as a function of temperature, total pressure, and metallicity. Aside from minor amounts of sulfur removed by metal sulfide cloud formation, H 2 S is approximately representative of the sulfur inventory throughout substellar atmospheres. Silicon sulfide (SiS) is a potential tracer of weather in EGPs and L dwarfs. Phosphorus chemistry is considerably more complex than that of sulfur. Disequilibrium abundances of PH 3 approximately

  2. An estimate of the juvenile sulfur content of basalt

    USGS Publications Warehouse

    Moore, J.G.; Fabbi, Brent P.

    1971-01-01

    Sulfur analyses by X-ray fluorescence give an average content of 107 ppm for 9 samples of fresh subaerially-erupted oceanic basalt and 680 ppm for 38 samples of submarine erupted basalt. This difference is the result of retention of sulfur in basalt quenched on the sea floor and loss of sulfur in basalt by degassing at the surface. The outer glassy part of submarine erupted basalt contains 800??150 ppm sulfur, and this amount is regarded as an estimate of the juvenile sulfur content of the basalt melt from the mantle. The slower cooled interiors of basalt pillows are depleted relative to the rims owing to degassing and escape through surface fractures. Available samples of deep-sea basalts do not indicate a difference in original sulfur content between low-K tholeiite, Hawaiian tholeiite, and alkali basalt. The H2O/S ratio of analyzed volcanic gases is generally lower than the H2O/S ratio of gases presumed lost from surface lavas as determined by chemical differences between pillow rims and surface lavas. This enrichment of volcanic gases in sulfur relative to water may result from a greater degassing of sulfur relative to water from shallow intrusive bodies beneath the volcano. ?? 1971 Springer-Verlag.

  3. Composition and oxidation state of sulfur in atmospheric particulate matter

    NASA Astrophysics Data System (ADS)

    Longo, Amelia F.; Vine, David J.; King, Laura E.; Oakes, Michelle; Weber, Rodney J.; Huey, Lewis Gregory; Russell, Armistead G.; Ingall, Ellery D.

    2016-10-01

    The chemical and physical speciation of atmospheric sulfur was investigated in ambient aerosol samples using a combination of sulfur near-edge x-ray fluorescence spectroscopy (S-NEXFS) and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the composition and oxidation state of sulfur in common primary emission sources and ambient particulate matter collected from the greater Atlanta area. Ambient particulate matter samples contained two oxidation states: S0 and S+VI. Ninety-five percent of the individual aerosol particles (> 1 µm) analyzed contain S0. Linear combination fitting revealed that S+VI in ambient aerosol was dominated by ammonium sulfate as well as metal sulfates. The finding of metal sulfates provides further evidence for acidic reactions that solubilize metals, such as iron, during atmospheric transport. Emission sources, including biomass burning, coal fly ash, gasoline, diesel, volcanic ash, and aerosolized Atlanta soil, and the commercially available bacterium Bacillus subtilis, contained only S+VI. A commercially available Azotobacter vinelandii sample contained approximately equal proportions of S0 and S+VI. S0 in individual aerosol particles most likely originates from primary emission sources, such as aerosolized bacteria or incomplete combustion.

  4. Sulfur during the Transition from Anoxic to Oxic Atmospheres

    NASA Technical Reports Server (NTRS)

    Zahnle, Kevin; Catling, David; Claire, Mark

    2006-01-01

    The invention of oxygenic photosynthesis was likely accompanied by the introduction of large amounts of O2 and complementary reduced gases (chiefly CH4) into the atmosphere. To first approximation the venting of O2 and CH4 are stochiometrically linked. We therefore present a suite of numerical photochemical models that address the anoxic-oxic transition in an atmosphere driven by large linked inputs of biogenic 02 and CH4. We find in general that, in steady state, there are two solutions, one oxic and the other anoxic. The anoxic solution appears to be linearly stable. If volcanic SO2 fluxes are large, S disproportionates into oxidized (H2S04) and reduced (S8) exit channels. As elemental sulfur is insoluble it provides a means of preserving photochemical mass-independent fractionation (MIF). On the other hand, if the source of volcanic SO2 is smaller than today, all S can leave the atmosphere as S8. Under these conditions there would be no MIF signal. The oxic solution appears to be linearly unstable. In the oxic solutions S is invariably oxidized to sulfate, and the MIF signal would be absent. The transitional atmosphere is relatively unstable and is also the most photochemically active. Consequently it is the transitional atmosphere, not the oxic or anoxic atmospheres, that has the lowest CH4 levels and weakest greenhouse warming. As a practical matter we expect the transitional atmospheres to vary strongly in response to diurnal and seasonal biological forcing.

  5. International Global Atmospheric Chemistry Programme global emissions inventory activity: Sulfur emissions from volcanoes, current status

    SciTech Connect

    Benkovitz, C.M.

    1995-07-01

    Sulfur emissions from volcanoes are located in areas of volcanic activity, are extremely variable in time, and can be released anywhere from ground level to the stratosphere. Previous estimates of global sulfur emissions from all sources by various authors have included estimates for emissions from volcanic activity. In general, these global estimates of sulfur emissions from volcanoes are given as global totals for an ``average`` year. A project has been initiated at Brookhaven National Laboratory to compile inventories of sulfur emissions from volcanoes. In order to complement the GEIA inventories of anthropogenic sulfur emissions, which represent conditions circa specific years, sulfur emissions from volcanoes are being estimated for the years 1985 and 1990.

  6. The role of cluster energy nonaccommodation in atmospheric sulfuric acid nucleation

    SciTech Connect

    Kurten, T.; Kuang, C.; Gomez, P.; McMurry, P. H.; Vehkamaki, H.; Ortega, I.; Noppel, M.; Kulmala, M.

    2010-01-11

    We discuss the possible role of energy nonaccommodation (monomer-cluster collisions that do not result in stable product formation due to liberated excess energy) in atmospheric nucleation processes involving sulfuric acid. Qualitative estimates of the role of nonaccommodation are computed using quantum Rice-Ramsberger-Kassel theory together with quantum chemically calculated vibrational frequencies and anharmonic coupling constants for small sulfuric acid-containing clusters. We find that energy nonaccommodation effects may, at most, decrease the net formation rate of sulfuric acid dimers by up to a factor of 10 with respect to the hard-sphere collision rate. A decrease in energy nonaccommodation due to an increasing number of internal degrees of freedom may kinetically slightly favor the participation of amines rather than ammonia as stabilizing agents in sulfuric acid nucleation, though the kinetic enhancement factor is likely to be less than three. However, hydration of the clusters (which always occurs in ambient conditions) is likely to increase the energy accommodation factor, reducing the role that energy nonaccommodation plays in atmospheric nucleation.

  7. The Sulfur Cycle

    ERIC Educational Resources Information Center

    Kellogg, W. W.; And Others

    1972-01-01

    A model estimating the contributions of sulfur compounds by natural and human activities, and the rate of removal of sulfur from the atmosphere, is based on a review of the existing literature. Areas requiring additional research are identified. (AL)

  8. A descriptive model for sulfur capture in bubbling atmospheric pressure fluidized bed combustors

    SciTech Connect

    Walsh, P.M.

    1995-12-31

    A model of sorbent behavior is proposed for interpretation of measurements of sulfur capture in large-scale bubbling atmospheric pressure fluidized bad combustors (AFBC). The objective is to account for effects of the stone feed size distribution, attrition, recycle ratio, sulfation capacity, and sulfation rate on sulfur capture in practical systems. The parameters used in the simulation are limited to those whose values can be estimated from measurements in full-scale plants. Fines introduced with the limestone feed or formed on calcination, fines generated by attrition of bed particles, sulfur capture in the freeboard, and fines recycle were included in the description of the system. The sorbent was characterized by its sulfation capacity, fines content, attrition coefficient, and a first-order rate coefficient for reaction with SO{sub 2}. The model was compared with measurements by the Tennessee Valley Authority (TVA) and Electric Power Research Institute (EPRI) in the TVA 20 MW AFBC (TVA and EPRI, 1984), Measurements of sulfur capture over the range of recycle ratios from 0 to 4 kg recycle/kg coal, and calcium-to-sulfur ratios from 1.5 to 5 kmol Ca/kmol S, were reproduced with an average error of 5% sulfur capture. The principal source of error is thought to be neglect of fines formation during calcination of the stone. With further refinement the approach may be useful for characterization of sorbents in pilot and industrial-scale systems, and for evaluation of the effects of changes in operating conditions on sorbent performance in existing units.

  9. Oxaldihydroxamic acid as a new reagent for the fixation of atmospheric sulfur dioxide

    NASA Astrophysics Data System (ADS)

    Paul, Khana Rani; Gupta, V. K.

    In the present investigation 0.01 M aqueous oxaldihydroxamic acid has been used to stabilize the atmospheric sulfur dioxide. The collection efficiency of the reagent was found to be ~ 100% and the sulfite solution was stable for ⩾ 30 days at room temperature. The sulfite ion was estimated colorimetrically using acidified p-aminoazobenzene and formaldehyde. The pink coloured dye, λmax 505 nm, obeys Beer's law in the range of 0.1-1 ppm. The procedure has been optimized with respect to the acidity, time and reagent concentration. The method is simple, free from pH dependence and several commonly present air pollutants do not interfere.

  10. The molecular physics of photolytic fractionation of sulfur and oxygen isotopes in planetary atmospheres (Invited)

    NASA Astrophysics Data System (ADS)

    Johnson, M. S.; Schmidt, J. A.; Hattori, S.; Danielache, S.; Meusinger, C.; Schinke, R.; Ueno, Y.; Nanbu, S.; Kjaergaard, H. G.; Yoshida, N.

    2013-12-01

    Atmospheric photochemistry is able to produce large mass independent anomalies in atmospheric trace gases that can be found in geological and cryospheric records. This talk will present theoretical and experimental investigations of the molecular mechanisms producing photolytic fractionation of isotopes with special attention to sulfur and oxygen. The zero point vibrational energy (ZPE) shift and reflection principle theories are starting points for estimating isotopic fractionation, but these models ignore effects arising from isotope-dependent changes in couplings between surfaces, excited state dynamics, line densities and hot band populations. The isotope-dependent absorption spectra of the isotopologues of HCl, N2O, OCS, CO2 and SO2 have been examined in a series of papers and these results are compared with experiment and ZPE/reflection principle models. Isotopic fractionation in planetary atmospheres has many interesting applications. The UV absorption of CO2 is the basis of photochemistry in the CO2-rich atmospheres of the ancient Earth, and of Mars and Venus. For the first time we present accurate temperature and isotope dependent CO2 absorption cross sections with important implications for photolysis rates of SO2 and H2O, and the production of a mass independent anomaly in the Ox reservoir. Experimental and theoretical results for OCS have implications for the modern stratospheric sulfur budget. The absorption bands of SO2 are complex with rich structure producing isotopic fractionation in photolysis and photoexcitation.

  11. Isotopic evidence in tree rings for historical changes in atmospheric sulfur sources.

    PubMed

    Kawamura, Hidehisa; Matsuoka, Nobuaki; Momoshima, Noriyuki; Koike, Masami; Takashima, Yoshimasa

    2006-09-15

    Little is understood about the usefulness of sulfur isotopic ratios (sigma 34S) in tree rings because the sulfur content in rings is generally insufficient for analysis using conventional methods. We present sigma 34S values of the water-soluble and the organically bound sulfur fractions in rings of coniferous trees grown in Japan, analyzed using a large-volume oxygen bomb. Comparing the sigma 34S values of the organically bound fraction in tree rings with past atmospheric sulfur concentrations and with those of their sources, we find clear evidence that the sigma 34S values of the organically bound fraction in the rings are dependent upon the values of the atmospheric sulfur sources. The evidence suggests that the sigma 34S values in tree rings are a useful chronological proxy for evaluating possible causes of past atmospheric sulfur pollution.

  12. Atmospheric sulfur hexafluoride - Sources, sinks and greenhouse warming

    NASA Technical Reports Server (NTRS)

    Ko, Malcolm K. W.; Sze, Nien D.; Wang, Wei-Chyung; Shia, George; Goldman, Aaron; Murcray, Frank J.; Murcray, David G.; Rinsland, Curtis P.

    1993-01-01

    An estimate is obtained of worldwide production of SF6, from which a global emission rate is derived and extrapolated for the next 20 years. The atmospheric lifetime of SF6 is then estimated based on a known mechanism (e.g., photolysis and atmospheric oxidation) and/or on the mass balance method. Finally, the radiative forcing of SF6 is calculated based on recent laboratory IR absorption data, and the expected warming over the time period 1950-2010 is computed for several emission scenarios. Calculations showed that SF6 is 3 times more effective as a greenhouse gas compared to CFC 11 on a per-molecule basis. However, based on projected emission scenarios, the expected warming from SF6 through 2010 is small (0.004 C), compared to the warming from CO2 and other trace gases (0.8 C).

  13. Atmospheric DMS and Biogenic Sulfur aerosol measurements in the Arctic

    NASA Astrophysics Data System (ADS)

    Ghahremaninezhadgharelar, R.; Norman, A. L.; Wentworth, G.; Burkart, J.; Leaitch, W. R.; Abbatt, J.; Sharma, S.; Desiree, T. S.

    2014-12-01

    Dimethyl Sulfide (DMS) and its oxidation products were measured on the board of the Canadian Coast Guard Ship (CCGS) Amundsen and above melt ponds in the Arctic during July 2014 in the context of the NETCARE study which seeks to understand the effect of DMS and its oxidation products with respect to aerosol nucleation, as well as its effect on cloud and precipitation properties. The objective of this study is to quantify the role of DMS in aerosol growth and activation in the Arctic atmosphere. Atmospheric DMS samples were collected from different altitudes, from 200 to 9500 feet, aboard the POLAR6 aircraft expedition to determine variations in the DMS concentration and a comparison was made to shipboard DMS measurements and its effects on aerosol size fractions. The chemical and isotopic composition of sulfate aerosol size fractions was studied. Sulfur isotope ratios (34S/32S) offer a way to determine the oceanic DMS contribution to aerosol growth. The results are expected to address the contribution of anthropogenic as well as biogenic sources of aerosols to the growth of the different aerosol size fractions. In addition, aerosol sulfate concentrations were measured at the same time within precipitation and fogs to compare with the characteristics of aerosols in each size fraction with the characteristics of the sulfate in each medium. This measurement is expected to explain the contribution of DMS oxidation in aerosol activation in the Arctic summer. Preliminary results from the measurement campaign for DMS and its oxidation products in air, fog and precipitation will be presented.

  14. Changes in Atmospheric Sulfur Dioxide (SO2) over the English Channel - 1.5 Years of Measurements from the Penlee Point Atmospheric Observatory

    NASA Astrophysics Data System (ADS)

    Yang, Mingxi; Bell, Thomas; Hopkins, Frances; Smyth, Timothy

    2016-04-01

    Atmospheric sulfur dioxide (SO2) was measured continuously from the Penlee Point Atmospheric Observatory near Plymouth, United Kingdom between May 2014 and November 2015. This coastal site is exposed to marine air across a wide wind sector. The predominant southwesterly winds carry relatively clean background Atlantic air. In contrast, air from the southeast is heavily influenced by exhaust plumes from ships in the English Channel as well as near near the Plymouth Sound. International Maritime Organization regulation came into force in January 2015 to reduce sulfur emissions tenfold in Sulfur Emission Control Areas such as the English Channel. We observed a three-fold reduction from 2014 to 2015 in the estimated ship-emitted SO2 during southeasterly winds. Dimethylsulfide (DMS) is an important source of atmospheric SO2 even in this semi-polluted region. The relative contribution of DMS oxidation to the SO2 burden over the English Channel increased from ~1/3 in 2014 to ~1/2 in 2015 due to the reduction in ship sulfur emissions. Our diel analysis suggests that SO2 is removed from the marine atmospheric boundary layer in about half a day, with dry deposition to the ocean accounting for a quarter of the total loss.

  15. Sulfur isotopic signatures in rainwater and moss Haplocladium microphyllum indicating atmospheric sulfur sources in Nanchang City (SE China).

    PubMed

    Xiao, Hua-Yun; Zhu, Ren-Guo; Lin, Bi-Na; Liu, Cong-Qiang

    2011-05-01

    Sulfur source identification previously reported has been based on sulfur isotopic ratios in either rainwater or mosses. The δ(34)S values of rainwater sulfate and the epilithic moss Haplocladium microphyllum in Nanchang region (China) were determined for comparisons and used to delineate atmospheric sulfur sources. At the urban and rural sites, similar mean δ(34)S values were observed between rainwater sulfate (+1.6‰ and -0.2‰, respectively) and epilithic mosses (+1.7‰ and +0.6‰, respectively), suggesting that mosses acquire δ(34)S values similar to those found for rainwater sulfate. This has further demonstrated that moss δ(34)S signatures hold valuable source-specific information as rainwater δ(34)S values do. The δ(34)S values of both rainwater sulfate and epilithic mosses indicated that atmospheric sulfur in Nanchang region was mainly associated with coal combustion. The lower δ(34)S values at the rural site can be explained by higher contribution of local coals (lower δ(34)S values relative to those of north Chinese coals) and biogenic sulfur.

  16. Kinetics of Thermochemical Reactions Important in the Venus Atmospheric Sulfur Cycle

    NASA Technical Reports Server (NTRS)

    Fegley, Bruce, Jr.

    1997-01-01

    The purpose of this project was to experimentally measure the rates of several thermochemical gas-solid reactions between sulfur gases in the Venus atmosphere and reactive minerals on the hot Venus surface. Despite the great importance of these reactions for the maintenance of significant amounts of sulfur gases (and thus for the maintenance of the global cloud cover) in the atmosphere of Venus, essentially no kinetic data are currently available for them.

  17. Atmospheric Sulfur Cycle Simulated in The Global Model GOCART: Model Description and Global Properties

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Rood, Richard B.; Lin, Shian-Jiann; Mueller, Jean-Francois; Thompson, Anne M.

    2000-01-01

    The Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model is used to simulate the atmospheric sulfur cycle. The model uses the simulated meteorological data from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). Global sulfur budgets from a 6-year simulation for SO2, sulfate, dimethylsulfide (DMS), and methanesulfonic acid (MSA) are presented in this paper. In a normal year without major volcanic perturbations, about 20% of the sulfate precursor emission is from natural sources (biogenic and volcanic) and 80% is anthropogenic: the same sources contribute 339% and 67% respectively to the total sulfate burden. A sulfate production efficiency of 0.41 - 0.42 is estimated in the model, an efficiency which is defined as a ratio of the amount oi sulfate produced to the total amount of SO2 emitted and produced in the atmosphere. This value indicates that less than half of the SO2 entering the atmosphere contributes to the sulfate production, the rest being removed by dry and wet depositions. In a simulation for 1990, we estimate a total sulfate production of 39 Tg S /yr with 36% and 64% respectively from in-air and in-cloud oxidation of SO2. We also demonstrate that major volcanic eruptions, such as the Mt. Pinatubo eruption in 1991, can significantly change the sulfate formation pathways, distributions, abundance, and lifetime. Comparison with other models shows that the parameterizations for wet removal or wet production of sulfate are the most critical factors in determining the burdens of SO2 and sulfate. Therefore, a priority for future research should be to reduce the large uncertainties associated with the wet physical and chemical processes.

  18. Identifying the change in atmospheric sulfur sources in China using isotopic ratios in mosses

    NASA Astrophysics Data System (ADS)

    Xiao, Hua-Yun; Tang, Cong-Guo; Xiao, Hong-Wei; Liu, Xue-Yan; Liu, Cong-Qiang

    2009-08-01

    A considerable number of studies on rainwater sulfur isotopic ratios (δ34Srain) have been conducted to trace sulfur sources at a large number of sites in the past. If longitudinal studies on the isotope composition of precipitation sulfate were conducted, it is possible to relate that to changes in sulfur emissions. But direct measurement needs considerable labor and time. So, in this study, sulfur isotopic ratios in rainwater and mosses were analyzed at Guiyang and Nanchang to evaluate the possibility of using mosses as a substitute for rainwater. We found that present moss sulfur isotopic ratios were comparable to those of present rainwater. Additionally, we investigated the changes of atmospheric sulfur sources and sulfur concentrations using an isotopic graphic analysis at five industrial cities, two forested areas, and two remote areas in China. Mosses in industrial cities show a wide range of δ34S values, with the highest occurring at Chongqing (+3.9‰) and the lowest at Guiyang (-3.1‰). But as compared to those in forested and remote areas, δ34S values of mosses in all the five industrial cities are lower. On the basis of isotopic comparisons between past rainwater (reported in the literature) and present mosses, in the plot of δ34Smoss versus δ34Srain, six zones indicating different atmospheric sulfur change are separated by the 1:1 line and δ34S values of potential sulfur sources. Our results indicate that atmospheric sulfur pollution in most of the industrial cities decreased, while at the two forested areas, no significant changes were observed, and a new anxiousness coming from new energy sources (e.g., oil) appeared in some cities. Studies on the change of ambient SO2 concentrations support these results.

  19. Sulfur

    USGS Publications Warehouse

    Apodaca, L.E.

    2012-01-01

    In 2011, elemental sulfur and the byproduct sulfuric acid were produced at 109 operations in 29 states and the U.S. Virgin Islands. Total shipments were valued at about $1.6 billion. Elemental sulfur production was 8.2 Mt (9 million st); Louisiana and Texas accounted for about 53 percent of domestic production.

  20. Atmospheric Sulfur Cycle Effects of Carbonyl Sulfide (OCS)

    NASA Technical Reports Server (NTRS)

    McBee, Joshua

    1996-01-01

    Carbonyl Sulfide(OCS) is considered to be one of the major sources of sulfur appearing in the stratosphere due to its relative inertness, about I to 10 yearsl. However, the roles of OCS as well as other reduced sulfur compounds such as carbon disulfide (CS2), hydrogen sulfide (H2S), and dimethyl disulfide(CH3)2S2, are not completely understood in the atmosphenc sulfur cycle. Consequently vely little information is available about the effect of sulfur compounds in the stratosphere. The ability of OCS to penetrate into the stratosphere makes it an excellent tracer for study of the role of the sulfi r cycle in stratospheric chemistry. Previously techniques such as gas chromatography and whole air sampling have been used to measure OCS analytically. Each technique had its drawbacks however, with both being quite slow, and whole air sampling being somewhat unreliable. With molecular spectroscopy, however, it has been found in recent years that the tunable diode laser absorption spectrometer (TDL) provides a very rapid and accurate method of measuring OCS and other trace gases

  1. ZASPE: Zonal Atmospheric Stellar Parameters Estimator

    NASA Astrophysics Data System (ADS)

    Brahm, Rafael; Jordan, Andres; Hartman, Joel; Bakos, Gaspar

    2016-07-01

    ZASPE (Zonal Atmospheric Stellar Parameters Estimator) computes the atmospheric stellar parameters (Teff, log(g), [Fe/H] and vsin(i)) from echelle spectra via least squares minimization with a pre-computed library of synthetic spectra. The minimization is performed only in the most sensitive spectral zones to changes in the atmospheric parameters. The uncertainities and covariances computed by ZASPE assume that the principal source of error is the systematic missmatch between the observed spectrum and the sythetic one that produces the best fit. ZASPE requires a grid of synthetic spectra and can use any pre-computed library minor modifications.

  2. Photon and Water Mediated Sulfur Oxide and Acid Chemistry in the Atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Kroll, Jay A.; Vaida, Veronica

    2014-06-01

    Sulfur compounds have been observed in the atmospheres of a number of planetary bodies in our solar system including Venus, Earth, Mars, Io, Europa, and Callisto. The global cloud cover on Venus located at an altitude between 50 and 80 kilometers is composed primarily of sulfuric acid (H_2SO_4) and water. Planetary photochemical models have attempted to explain observations of sulfuric acid and sulfur oxides with significant discrepancies remaining between models and observation. In particular, high SO_2 mixing ratios are observed above 90 km which exceed model predictions by orders of magnitude. Work recently done in the Vaida lab has shown red light can drive photochemistry through overtone pumping for acids like H_2SO_4 and has been successful in explaining much of the sulfur chemistry in Earth's atmosphere. Water can have a number of interesting effects such as catalysis, suppression, and anti-catalysis of thermal and photochemical processes. We investigate the role of water complexes in the hydration of sulfur oxides and dehydration of sulfur acids and present spectroscopic studies to document such effects. We investigate these reactions using FTIR and UV/Vis spectroscopy and will report on our findings.

  3. Source estimation methods for atmospheric dispersion

    NASA Astrophysics Data System (ADS)

    Shankar Rao, K.

    Both forward and backward transport modeling methods are being developed for characterization of sources in atmospheric releases of toxic agents. Forward modeling methods, which describe the atmospheric transport from sources to receptors, use forward-running transport and dispersion models or computational fluid dynamics models which are run many times, and the resulting dispersion field is compared to observations from multiple sensors. Forward modeling methods include Bayesian updating and inference schemes using stochastic Monte Carlo or Markov Chain Monte Carlo sampling techniques. Backward or inverse modeling methods use only one model run in the reverse direction from the receptors to estimate the upwind sources. Inverse modeling methods include adjoint and tangent linear models, Kalman filters, and variational data assimilation, among others. This survey paper discusses these source estimation methods and lists the key references. The need for assessing uncertainties in the characterization of sources using atmospheric transport and dispersion models is emphasized.

  4. Sulfur, Chlorine, and Flourine Degassing and Atmospheric Loading by the 1783 - 1784 AD Laki (Skaftar Fires) Eruption in Iceland

    NASA Technical Reports Server (NTRS)

    Thordarson, T.; Self, S.; Hulsebosch, T.; Oskarsson, N.; McPhie, Jocelyn (Editor)

    1996-01-01

    The 1783-1784 Laki tholeiitic basalt fissure eruption in Iceland was one of the greatest atmospheric pollution events of the past 250 years, with widespread effects in the northern hemisphere. The degassing history and volatile budget of this event are determined by measurements of pre-eruption and residual contents of sulfur, chlorine, and fluorine in the products of all phases of the eruption. In fissure eruptions such as Laki, degassing occurs in two stages: by explosive activity or lava fountaining at the vents, and from the lava as it flows away from the vents. Using the measured sulfur concentrations in glass inclusions in phenocrysts and in groundmass glasses of quenched eruption products, we calculate that the total accumulative atmospheric mass loading of sulfur dioxide was 122 Mt over a period of 8 months. This volatile release is sufficient to have generated approximately 250 Mt of H2SO4 aerosols, an amount which agrees with an independent estimate of the Laki aerosol yield based on atmospheric turbidity measurements. Most of this volatile mass (approximately 60 wt.%) was released during the first 1.5 months of activity. The measured chlorine and fluorine concentrations in the samples indicate that the atmospheric loading of hydrochloric acid and hydrofluoric acid was approximately 7.0 and 15.0 Mt, respectively. Furthermore, approximately 75% of the volatile mass dissolved by the Laki magma was released at the vents and carried by eruption columns to altitudes between 6 and 13 km. The high degree of degassing at the vents is attributed to development of a separated two-phase flow in the upper magma conduit, and implies that high-discharge basaltic eruptions such as Laki are able to loft huge quantities of gas to altitudes where the resulting aerosols can reside for months, or even 1-2 years. The atmospheric volatile contribution due to subsequent degassing of the Laki lava flow is only 18 wt.% of the total dissolved in the magma, and these emissions were

  5. Low level atmospheric sulfur dioxide pollution and childhood asthma

    SciTech Connect

    Tseng, R.Y.; Li, C.K. )

    1990-11-01

    Quarterly analysis (1983-1987) of childhood asthma in Hong Kong from 13,620 hospitalization episodes in relation to levels of pollutants (SO{sub 2}, NO{sub 2}, NO, O{sub 3}, TSP, and RSP) revealed a seasonal pattern of attack rates that correlates inversely with exposure to sulfur dioxide (r = -.52, P less than .05). The same cannot be found with other pollutants. Many factors may contribute to the seasonal variation of asthma attacks. We speculate that prolonged exposure (in terms of months) to low level SO{sub 2} is one factor that might induce airway inflammation and bronchial hyperreactivity and predispose to episodes of asthma.

  6. Laboratory measurements and modeling of molecular photoabsorption in the ultraviolet for planetary atmospheres applications: diatomic sulfur and sulfur monoxide

    NASA Astrophysics Data System (ADS)

    Stark, Glenn

    2016-07-01

    Our research program comprises the measurement and modeling of ultraviolet molecular photoabsorption cross sections with the highest practical resolution. It supports efforts to interpret and model observations of planetary atmospheres. Measurement and modeling efforts on diatomic sulfur (S _{2}) and sulfur monoxide (SO) are in progress. S _{2}: Interpretations of atmospheric (Io, Jupiter, cometary comae) S _{2} absorption features are hindered by a complete lack of laboratory cross section data in the ultraviolet. We are working to quantify the photoabsorption spectrum of S _{2} from 240 to 300 nm based on laboratory measurements and theoretical calculations. We have constructed an experimental apparatus to produce a stable column of S _{2} vapor at a temperature of 800 K. High-resolution measurements of the absorption spectrum of the strong B - X system of S _{2} were completed using the NIST VUV-FTS at Gaithersburg, Maryland. These measurements are currently being incorporated into a coupled-channel model of the absorption spectrum of S _{2} to quantify the contributions from individual band features and to establish the mechanisms responsible for the strong predissociation signature of the B - X system. A successful coupled channels model can then be used to calculate the B - X absorption spectrum at any temperature. SO: There has been a long-standing need for high-resolution cross sections of sulfur monoxide radicals in the ultraviolet and vacuum ultraviolet regions, where the molecule strongly predissociates, for modeling the atmospheres of Io and Venus, and most recently for understanding sulfur isotope effects in the ancient (pre-O _{2}) atmosphere of Earth. We have produced a measurable column of SO in a continuous-flow DC discharge cell, using SO _{2} as a parent molecule. Photoabsorption measurements were recently recorded on the DESIRS beamline of the SOLEIL synchrotron, taking advantage of the high-resolution VUV-FTS on that beamline. A number of

  7. Missing SO2 oxidant in the coastal atmosphere? - Evidence from high resolution measurements of OH and atmospheric sulfur compounds

    NASA Astrophysics Data System (ADS)

    Berresheim, H.; Adam, M.; Monahan, C.; O'Dowd, C.; Plane, J. M. C.; Bohn, B.; Rohrer, F.

    2014-01-01

    Diurnal and seasonal variations of gaseous sulfuric acid (H2SO4) and methane sulfonic acid (MSA) were measured in N.E. Atlantic air at the Mace Head atmospheric research station during the years 2010 and 2011. The measurements utilized selected ion/chemical ionization mass spectrometry (SI/CIMS) with a detection limit for both compounds of 4.3 × 10 4 cm-3 at 5 min signal integration. The H2SO4 and MSA gas-phase concentrations were analysed in conjunction with the condensational sink for both compounds derived from 3 nm-10 μm (diameter) aerosol size distributions. Accommodation coefficients of 1.0 for H2SO4 and 0.12 for MSA were assumed leading to estimated atmospheric lifetimes of the order of 7 min and 25 min, respectively. With the SI/CIMS instrument in OH measurement mode alternating between OH signal and background (non-OH) signal evidence was obtained for the presence of one or more unknown oxidants of SO2 in addition to OH. Depending on the nature of the oxidant(s) their ambient concentration may be enhanced in the CIMS inlet system by additional production. The apparent unknown SO2 oxidant was additionally confirmed by direct measurements of SO2 in conjunction with calculated H2SO4 concentrations. The calculated concentrations were consistently lower than the measured concentrations by a factor 4.8 ± 3.4 when considering the oxidation of SO2 by OH as the only source of H2SO4. Both the OH and the background signal were also observed to increase significantly during daytime aerosol nucleation events, independent of the ozone photolysis frequency, J(O1D), and were followed by peaks in both H2SO4 and MSA concentrations. This suggests a strong relation between the unknown oxidant(s), OH chemistry, and the atmospheric photo-oxidation of biogenic iodine compounds. As to the identity of the oxidant(s), we have been able to exclude ClO, BrO, IO, and OIO as possible candidates based on ab initio calculations. Stabilized Criegee intermediates (sCI) produced from

  8. Reevaluating the contribution of sulfuric acid and the origin of organic compounds in atmospheric nanoparticle growth

    NASA Astrophysics Data System (ADS)

    Vakkari, Ville; Tiitta, Petri; Jaars, Kerneels; Croteau, Philip; Beukes, Johan Paul; Josipovic, Miroslav; Kerminen, Veli-Matti; Kulmala, Markku; Venter, Andrew D.; Zyl, Pieter G.; Worsnop, Douglas R.; Laakso, Lauri

    2015-12-01

    Aerosol particles formed in the atmosphere are important to the Earth's climate system due to their ability to affect cloud properties. At present, little is known about the atmospheric chemistry responsible for the growth of newly formed aerosol particles to climate-relevant sizes. Here combining detailed aerosol measurements with a theoretical framework we found that depending on the gaseous precursors and size of the newly formed particles, the growth was dominated by either sulfuric acid accompanied by ammonium or organic compounds originating in either biogenic emissions or savannah fires. The contribution of sulfuric acid was larger during the early phases of the growth, but in clean conditions organic compounds dominated the growth from 1.5 nm up to climatically relevant sizes. Furthermore, our analysis indicates that in polluted environments the contribution of sulfuric acid to the growth may have been underestimated by up to a factor of 10.

  9. Strong Hydrogen Bonded Molecular Interactions between Atmospheric Diamines and Sulfuric Acid.

    PubMed

    Elm, Jonas; Jen, Coty N; Kurtén, Theo; Vehkamäki, Hanna

    2016-05-26

    We investigate the molecular interaction between methyl-substituted N,N,N',N'-ethylenediamines, propane-1,3-diamine, butane-1,4-diamine, and sulfuric acid using computational methods. Molecular structure of the diamines and their dimer clusters with sulfuric acid is studied using three density functional theory methods (PW91, M06-2X, and ωB97X-D) with the 6-31++G(d,p) basis set. A high level explicitly correlated CCSD(T)-F12a/VDZ-F12 method is used to obtain accurate binding energies. The reaction Gibbs free energies are evaluated and compared with values for reactions involving ammonia and atmospherically relevant monoamines (methylamine, dimethylamine, and trimethylamine). We find that the complex formation between sulfuric acid and the studied diamines provides similar or more favorable reaction free energies than dimethylamine. Diamines that contain one or more secondary amino groups are found to stabilize sulfuric acid complexes more efficiently. Elongating the carbon backbone from ethylenediamine to propane-1,3-diamine or butane-1,4-diamine further stabilizes the complex formation with sulfuric acid by up to 4.3 kcal/mol. Dimethyl-substituted butane-1,4-diamine yields a staggering formation free energy of -19.1 kcal/mol for the clustering with sulfuric acid, indicating that such diamines could potentially be a key species in the initial step in the formation of new particles. For studying larger clusters consisting of a diamine molecule with up to four sulfuric acid molecules, we benchmark and utilize a domain local pair natural orbital coupled cluster (DLPNO-CCSD(T)) method. We find that a single diamine is capable of efficiently stabilizing sulfuric acid clusters with up to four acid molecules, whereas monoamines such as dimethylamine are capable of stabilizing at most 2-3 sulfuric acid molecules.

  10. Estimating Atmospheric Turbulence From Flight Records

    NASA Technical Reports Server (NTRS)

    Wingrove, R. C.; Bach, R. E., Jr.; Schultz, T. A.

    1991-01-01

    Method for estimation of atmospheric turbulence encountered by airplanes utilizes wealth of data captured by multichannel digital flight-data recorders and air-traffic-control radar. Developed as part of continuing effort to understand how airplanes respond to such potentially hazardous phenomena as: clear-air turbulence generated by destabilized wind-shear layers above mountains and thunderstorms, and microbursts (intense downdrafts striking ground), associated with thunderstorms. Reconstructed wind fields used to predict and avoid future hazards.

  11. Sulfur Isotopes in Swaziland System Barites and the Evolution of the Earth's Atmosphere.

    PubMed

    Perry, E C; Monster, J; Reimer, T

    1971-03-12

    Sedimentary barites from the Swaziland System of South Africa (more than 3000 million years old) have sulfur-34 ratios that are enriched by only 2.5 per mil with respect to contemporary sulfides. To explain this small fractionation, it is proposed that oxygen pressure in the earth's atmosphere was very low and that local oxidation occurred in a photosynthetic layer of the ocean.

  12. Modeling the signature of sulfur mass-independent fractionation produced in the Archean atmosphere

    NASA Astrophysics Data System (ADS)

    Claire, Mark W.; Kasting, James F.; Domagal-Goldman, Shawn D.; Stüeken, Eva E.; Buick, Roger; Meadows, Victoria S.

    2014-09-01

    Minor sulfur isotope anomalies indicate the absence of O2 from the Archean atmosphere. A rich dataset showing large variations in magnitude and sign of Δ33S and Δ36S, preserved in both sulfates and sulfides, suggests that further constraints on Archean atmospheric chemistry are possible. We review previous quantitative constraints on atmospheric Δ33S production, and suggest that a new approach is needed. We added sulfur species containing 33S and 34S to a 1-D photochemical model and describe the numerical methodology needed to ensure accurate prediction of the magnitude and sign of Δ33S produced by and deposited from the Archean atmosphere. This methodology can test multiple MIF-S formation mechanisms subject to a variety of proposed atmospheric compositions, yielding Δ33S predictions that can be compared to the rock record. We systematically test SO2 isotopologue absorption effects in SO2 photolysis (Danielache et al., 2008), one of the primary proposed mechanisms for Δ33S formation. We find that differential absorption through the Danielache et al. (2008) cross sections is capable of altering predicted Δ33S as a function of multiple atmospheric variables, including trace O2 concentration, total sulfur flux, CO2 content, and the presence of hydrocarbons, but find a limited role for OCS and H2S. Under all realistic conditions, the Danielache et al. (2008) cross sections yield Δ33S predictions at odds with the geologic record, implying that additional pathways for sulfur MIF formation exist and/or the cross sections have significant errors. The methodology presented here will allow for quantitative constraints on the Archean atmosphere beyond the absence of O2, as soon as additional experimental measurements of MIF-S producing processes become available.

  13. [Research on determination of total volatile organic sulfur compounds in the atmosphere].

    PubMed

    Wang, Yan-Jun; Zheng, Xiao-Ling; He, Ying; Zhang, Dong; Wang, Bao-Dong

    2011-12-01

    A detection technology was established comprising trap, desorption, oxidation and UV fluorescence determination process, and used for the test of total concentration of trace volatile sulfur compounds (VSCs) in the atmosphere. A cryogenic trap-thermal desorption device was developed, integrating the advantages of solid retention method and cryogenic condensation method, which was applied to capture and enrich trace volatile organic sulfur compounds. Under high temperature and combustion-supporting gas, the VSCs were completely oxidized into sulfur dioxide. By analyzing the content of sulfur dioxide through ultraviolet fluorescence method indirectly calculated to gain the total concentration of volatile organic sulfur compounds. The trapping temperature, desorption temperature and the oxidation temperature were 5 degrees C, 150 degrees C and 1 000 degrees C, and the precision and recovery of the method were 5.46% and 99.6%-109.2%, respectively. The content of trace amounts of atmospheric VSCs determined from February to April at Qingdao was 42-195 ng x m(-3).

  14. Attribution of atmospheric sulfur dioxide over the English Channel to dimethyl sulfide and changing ship emissions

    NASA Astrophysics Data System (ADS)

    Yang, Mingxi; Bell, Thomas G.; Hopkins, Frances E.; Smyth, Timothy J.

    2016-04-01

    Atmospheric sulfur dioxide (SO2) was measured continuously from the Penlee Point Atmospheric Observatory (PPAO) near Plymouth, United Kingdom, between May 2014 and November 2015. This coastal site is exposed to marine air across a wide wind sector. The predominant southwesterly winds carry relatively clean background Atlantic air. In contrast, air from the southeast is heavily influenced by exhaust plumes from ships in the English Channel as well as near Plymouth Sound. A new International Maritime Organization (IMO) regulation came into force in January 2015 to reduce the maximum allowed sulfur content in ships' fuel 10-fold in sulfur emission control areas such as the English Channel. Our observations suggest a 3-fold reduction in ship-emitted SO2 from 2014 to 2015. Apparent fuel sulfur content calculated from coincidental SO2 and carbon dioxide (CO2) peaks from local ship plumes show a high level of compliance to the IMO regulation (> 95 %) in both years (˜ 70 % of ships in 2014 were already emitting at levels below the 2015 cap). Dimethyl sulfide (DMS) is an important source of atmospheric SO2 even in this semi-polluted region. The relative contribution of DMS oxidation to the SO2 burden over the English Channel increased from about one-third in 2014 to about one-half in 2015 due to the reduction in ship sulfur emissions. Our diel analysis suggests that SO2 is removed from the marine atmospheric boundary layer in about half a day, with dry deposition to the ocean accounting for a quarter of the total loss.

  15. High-Southern Latitudes Sulfur Cycle in an Atmospheric General Circulation Model

    NASA Astrophysics Data System (ADS)

    Cosme, E.; Genthon, C.; Martinerie, P.; Boucher, O.; Pham, M.

    2002-05-01

    This modeling study (Cosme et al., Sulfur cycle in the high southern latitudes in the LMD-ZT General Circulation Model, submitted to JGR) was motivated by the recent publication of annual time-scale records of dimethylsulfide (DMS) and dimethylsulfoxide (DMSO) in Antarctica, completing the available series of sulfate and methanesulfonic acid (MSA). Sulfur chemistry has been incorporated in the Laboratoire de Météorologie Dynamique Atmospheric General Circulation Model (AGCM), LMD-ZT, with high resolution and improved physics in the high-southern latitudes. The model predicts the concentration of 6 major sulfur species through emissions, transport, wet and dry deposition and chemistry in both gaseous and aqueous phases. Model results are broadly realistic when compared with measurements in air and snow or ice, and to results of other modeling studies, at high- and mid- southern latitudes. Although not corrected in this work, defects are identified and discussed: Atmospheric MSA concentrations are underestimated and DMSO concentrations are overestimated in summer, reflecting the lack of a DMSO sink leading to MSA; the deposition scheme used in the model may not be adapted to polar regions; DMS concentrations are underestimated in winter, and the model does not adequately reproduces interannual variability. Oceanic DMS sources appear deciding for the description of the sulfur cycle in these regions. The model suggests that ground atmospheric DMS concentrations are higher in winter than in summer, in a large part of central Antarctica. In the high-southern latitudes, high loads of DMS and DMSO are found and the main chemical sink of sulfur dioxide (SO2) is aqueous oxidation by ozone (O3), whereas oxidation by hydrogen peroxide (H2O2) dominates at the global scale.

  16. Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere

    PubMed Central

    Shaheen, Robina; Abaunza, Mariana M.; Jackson, Teresa L.; McCabe, Justin; Savarino, Joël; Thiemens, Mark H.

    2014-01-01

    Sulfur-isotopic anomalies have been used to trace the evolution of oxygen in the Precambrian atmosphere and to document past volcanic eruptions. High-precision sulfur quadruple isotope measurements of sulfate aerosols extracted from a snow pit at the South Pole (1984–2001) showed the highest S-isotopic anomalies (Δ33S = +1.66‰ and Δ36S = +2‰) in a nonvolcanic (1998–1999) period, similar in magnitude to Pinatubo and Agung, the largest volcanic eruptions of the 20th century. The highest isotopic anomaly may be produced from a combination of different stratospheric sources (sulfur dioxide and carbonyl sulfide) via SOx photochemistry, including photoexcitation and photodissociation. The source of anomaly is linked to super El Niño Southern Oscillation (ENSO) (1997–1998)-induced changes in troposphere–stratosphere chemistry and dynamics. The data possess recurring negative S-isotope anomalies (Δ36S = −0.6 ± 0.2‰) in nonvolcanic and non-ENSO years, thus requiring a second source that may be tropospheric. The generation of nonvolcanic S-isotopic anomalies in an oxidizing atmosphere has implications for interpreting Archean sulfur deposits used to determine the redox state of the paleoatmosphere. PMID:25092338

  17. Sulfur-containing particles emitted by concealed sulfide ore deposits: an unknown source of sulfur-containing particles in the atmosphere

    NASA Astrophysics Data System (ADS)

    Cao, J. J.; Li, Y. K.; Jiang, T.; Hu, G.

    2015-06-01

    Sources of sulfur dioxide, sulfates, and organic sulfur compounds, such as fossil fuels, volcanic eruptions, and animal feeding operations, have attracted considerable attention. In this study, we collected particles carried by geogas flows ascending through soil, geogas flows above the soil that had passed through the soil, and geogas flows ascending through deep faults of concealed sulfide ore deposits, and analysed them using transmission electron microscopy. Numerous crystalline and amorphous sulfur-containing particles or particle aggregations were found in the ascending geogas flows. In addition to S, the particles contained O, Ca, K, Mg, Fe, Na, Pb, Hg, Cu, Zn, As, Ti, Sr, Ba, Si, etc. Such particles are usually a few to several hundred nanometres in diameter with either regular or irregular morphology. The sulfur-containing particles originated from deep-seated weathering or faulting products of concealed sulfide ore deposits. The particles suspended in the ascending geogas flow migrated through faults from deep-seated sources to the atmosphere. This is a previously unknown source of the atmospheric particles. This paper reports, for the first time, the emission of sulfur-containing particles into the atmosphere from concealed sulfide ore deposits. The climatic and ecological influences of these sulfur-containing particles and particle aggregations should be assessed.

  18. Sulfur-containing particles emitted by concealed sulfide ore deposits: an unknown source of sulfur-containing particles in the atmosphere

    NASA Astrophysics Data System (ADS)

    Cao, J.; Li, Y.; Jiang, T.; Hu, G.

    2014-11-01

    Sources of sulfur dioxide, sulfates, and organic sulfur compounds, such as fossil fuels, volcanic eruptions, and animal feeding operations, have attracted considerable attention. In this study, we collected particles carried by geogas flows ascending through soil, geogas flows above the soil that had passed through the soil, and geogas flows ascending through deep faults of concealed sulfide ore deposits and analyzed them using transmission electron microscopy. Numerous crystalline and amorphous sulfur-containing particles or particle aggregations were found in the ascending geogas flows. In addition to S, the particles contained O, Ca, K, Mg, Fe, Na, Pb, Hg, Cu, Zn, As, Ti, Sr, Ba, Si, etc. Such particles are usually a few to several hundred nanometers in diameter with either regular or irregular morphology. The sulfur-containing particles originated from deep-seated weathering or faulting products of concealed sulfide ore deposits. The particles suspended in the ascending geogas flow migrated through faults from deep-seated sources to the atmosphere. This is a previously unknown source of the atmospheric particles. This paper reports, for the first time, the emission of sulfur-containing particles into the atmosphere from concealed sulfide ore deposits. The climatic and ecological influences of these sulfur-containing particles and particle aggregations should to be assessed.

  19. Erosion and landscape development decouple strontium and sulfur in the transition to dominance by atmospheric inputs

    USGS Publications Warehouse

    Bern, C.R.; Porder, S.; Townsend, A.R.

    2007-01-01

    Weathering and leaching can progressively deplete the pools of soluble, rock-derived elements in soils and ecosystems over millennial time-scales, such that productivity increasingly relies on inputs from atmospheric deposition. This transition has been explored using strontium isotopes, which have been widely assumed to be a proxy for the provenance of other rock-derived elements. We compared rock versus atmospheric proportions of strontium to those for sulfur, a plant macronutrient, at several tropical forest sites in Hawaii and Costa Rica. Isotopic analyses reveal that sulfur is often decoupled from strontium in the transition to atmospheric dependence. Decoupling is likely the result of differences in chemical factors such as atmospheric input rates, mobility in the soil environment, and mineral weathering susceptibility. Strontium and sulfur decoupling appears to be accentuated by the physical process of erosion. Erosion rates are presumed to be high on the Osa Peninsula of Costa Rica, where the recent onset of rapid tectonic uplift has placed the landscape in a transient state. Decoupling is strong there, as erosion has rejuvenated the supply of rock-derived strontium but not sulfur. The landscape response to changes in tectonic uplift on the Osa Peninsula has produced decoupling at the landscape scale. Decoupling is more variable along a Hawaiian catena, presumably due to smaller scale variations in erosion rates and their influence on rejuvenation of rock-strontium inputs. These results illustrate how chemical and physical processes can interact to produce contrasting origins for different nutrient elements in soils and the ecosystems they support. ?? 2007 Elsevier B.V. All rights reserved.

  20. Sulfur Hazes in Giant Exoplanet Atmospheres: Impacts on Reflected Light Spectra

    NASA Astrophysics Data System (ADS)

    Gao, Peter; Marley, Mark S.; Zahnle, Kevin; Robinson, Tyler D.; Lewis, Nikole K.

    2017-03-01

    Recent work has shown that sulfur hazes may arise in the atmospheres of some giant exoplanets, due to the photolysis of H2S. We investigate the impact such a haze would have on an exoplanet’s geometric albedo spectrum and how it may affect the direct imaging results of the Wide Field Infrared Survey Telescope (WFIRST), a planned NASA space telescope. For temperate (250 K < T eq < 700 K) Jupiter-mass planets, photochemical destruction of H2S results in the production of ∼1 ppmv of S8 between 100 and 0.1 mbar, which, if cool enough, will condense to form a haze. Nominal haze masses are found to drastically alter a planet’s geometric albedo spectrum: whereas a clear atmosphere is dark at wavelengths between 0.5 and 1 μm, due to molecular absorption, the addition of a sulfur haze boosts the albedo there to ∼0.7, due to scattering. Strong absorption by the haze shortward of 0.4 μm results in albedos <0.1, in contrast to the high albedos produced by Rayleigh scattering in a clear atmosphere. As a result, the color of the planet shifts from blue to orange. The existence of a sulfur haze masks the molecular signatures of methane and water, thereby complicating the characterization of atmospheric composition. Detection of such a haze by WFIRST is possible, though discriminating between a sulfur haze and any other highly reflective, high-altitude scatterer will require observations shortward of 0.4 μm, which is currently beyond WFIRST’s design.

  1. Missing SO2 oxidant in the coastal atmosphere? - observations from high-resolution measurements of OH and atmospheric sulfur compounds

    NASA Astrophysics Data System (ADS)

    Berresheim, H.; Adam, M.; Monahan, C.; O'Dowd, C.; Plane, J. M. C.; Bohn, B.; Rohrer, F.

    2014-11-01

    Diurnal and seasonal variations of gaseous sulfuric acid (H2SO4) and methane sulfonic acid (MSA) were measured in NE Atlantic air at the Mace Head atmospheric research station during the years 2010 and 2011. The measurements utilized selected-ion chemical ionization mass spectrometry (SI/CIMS) with a detection limit for both compounds of 4.3 × 104 cm-3 at 5 min signal integration. The H2SO4 and MSA gas-phase concentrations were analyzed in conjunction with the condensational sink for both compounds derived from 3 nm to 10 μm (aerodynamic diameter) aerosol size distributions. Accommodation coefficients of 1.0 for H2SO4 and 0.12 for MSA were assumed, leading to estimated atmospheric lifetimes on the order of 7 and 25 min, respectively. With the SI/CIMS instrument in OH measurement mode alternating between OH signal and background (non-OH) signal, evidence was obtained for the presence of one or more unknown oxidants of SO2 in addition to OH. Depending on the nature of the oxidant(s), its ambient concentration may be enhanced in the CIMS inlet system by additional production. The apparent unknown SO2 oxidant was additionally confirmed by direct measurements of SO2 in conjunction with calculated H2SO4 concentrations. The calculated H2SO4 concentrations were consistently lower than the measured concentrations by a factor of 4.7 ± 2.4 when considering the oxidation of SO2 by OH as the only source of H2SO4. Both the OH and the background signal were also observed to increase significantly during daytime aerosol nucleation events, independent of the ozone photolysis frequency, J(O1D), and were followed by peaks in both H2SO4 and MSA concentrations. This suggests a strong relation between the unknown oxidant(s), OH chemistry, and the atmospheric photolysis and photooxidation of biogenic iodine compounds. As to the identity of the atmospheric SO2 oxidant(s), we have been able to exclude ClO, BrO, IO, and OIO as possible candidates based on {ab initio} calculations

  2. Formic Sulfuric Anhydride: a New Chemical Species with Possible Implications for Atmospheric Aerosol

    NASA Astrophysics Data System (ADS)

    Mackenzie, Becca; Dewberry, Chris; Leopold, Ken

    2015-06-01

    Aerosols are important players in the Earth's atmosphere, affecting climate, cloud formation, and human health. In this work, we report the discovery of a previously unknown molecule, formic sulfuric anhydride (FSA), that may influence the formation and composition of atmospheric aerosol particles. Five isotopologues of FSA have been observed by microwave spectroscopy and further characterized using DFT calculations. The system has dipole moment components along all three inertial axes, and indeed a, b, and c-type transitions have been observed. A π2 + π2 + σ2 cycloaddition reaction between SO3 and HCOOH is proposed as a possible mechanism for the formation of FSA and calculations indicate that the transformation is effectively barrierless. Facile formation of the anhydride followed by hydrolysis in small water-containing clusters or liquid droplets may provide a mechanism of incorporating volatile organics into atmospheric aerosol. We suggest that FSA and its derivatives be considered in future atmospheric and climate models.

  3. Atmospheric sulfur rearrangement 2.7 billion years ago: Evidence for oxygenic photosynthesis

    NASA Astrophysics Data System (ADS)

    Kurzweil, Florian; Claire, Mark; Thomazo, Christophe; Peters, Marc; Hannington, Mark; Strauss, Harald

    2013-03-01

    Mass-independently fractionated sulfur isotopes (MIF-S) provide strong evidence for an anoxic atmosphere during the Archean. Moreover, the temporal evolution of MIF-S shows increasing magnitudes between 2.7 and 2.5 Ga until the start of the Great Oxidation Event (G.O.E.) at around 2.4 Ga. The conclusion of a completely anoxic atmosphere up to the G.O.E. is in contrast to recent studies on redox-sensitive elements, which suggest slightly oxidizing conditions during continental weathering already several hundred million years prior to the G.O.E. In order to investigate this apparent inconsistency, we present multiple sulfur isotopes for 2.71 Ga pyritic black shales derived from the Kidd Creek area, Ontario, Canada. These samples display high positive Δ33S values up to 3.8‰ and the typical late Archean slope in Δ36S/Δ33S of -0.9. In contrast, the time period before (3.2-2.73 Ga) is characterized by greatly attenuated MIF-S magnitudes and a slope in Δ36S/Δ33S of -1.5. We attribute the increase in Δ33S magnitude as well as the contemporaneous change in the slope of Δ36S/Δ33S to changes in the relative reaction rate of different MIF-S source reactions and changes in atmospheric sulfur exit channels. Both of these are dependent on atmospheric CH4:CO2 and O2 mixing ratios. We propose a distinct change in atmospheric composition at 2.7 Ga resulting from increased fluxes of oxygen and methane as the best explanation for the observed Neoarchean MIF-S record. Our data and modeling results suggest that oxygenic photosynthesis was a major contributor to primary productivity 2.7 billion years ago.

  4. Sulfur dioxide estimations in the planetary boundary layer using dispersion models and satellite retrievals

    NASA Astrophysics Data System (ADS)

    Zarauz, Jorge V.

    The health and environmental conditions in the Central Andes city La Oroya, Peru, have been seriously damaged by the heavy metal mining activities in the region. The situation has been exacerbated by the complex topography, which prevents proper mixing and dissolution of particles and gases released into the atmosphere. Understanding how pollutants are dispersed in populated regions, especially in complex terrain, would help to create mitigation strategies. The present study uses CALPUFF and HYSPLIT dispersion/deposition models to estimate sulfur dioxide (SO2) dispersion from the main stack of the La Oroya metallurgical plant. Due to the lack of meteorological data in the area, the Weather Research and Forecasting model (WRF) is used with observational nudging for temperature, relative humidity, and wind fields of three surface meteorological stations specifically installed for the study. The pollutant dispersion models are sensitive to a precise estimation of the turbulent vertical transport of mass, energy and moisture in the low atmosphere; therefore, two planetary boundary layer (PBL) schemes are tested, the Mellor-Yamada-Janjic and Yonsei University models. The dispersion models are run and results compared with field measurements at La Oroya, and Huancayo. The observation-nudging and YSU scheme considerably improved the prognostic variables. CALPUFF and HYSPLIT models showed similar patterns; however, HYSPLIT overestimated SO2 concentrations for low PBLs. Moreover, recent enhancements on spectral, spatial and temporal resolution of atmospheric scanning sensors of chemical constituents from the space, have led to detecting trace gases of anthropogenic origin in the lower troposphere. This contribution also explores the SO2 level 2 dataset from Ozone Mapping Instrument (OMI), in conjunction with atmospheric optical depth and Angstrom coefficient data products, extracted from MODerate Resolution Imaging Spectroradiometer (MODIS) to estimate SO2 loads in the PBL

  5. Observation of dipropenyldisulfide and other organic sulfur compounds in the atmosphere of a beech forest with Allium ursinum ground cover

    NASA Astrophysics Data System (ADS)

    Puxbaum, H.; König, G.

    Dipropenyldisulfide, methylpropenyldisulfide, cis-propenylpropyldisulfide, diallylsulfide, dimethyldisulfide and 3-methylthiopropene were detected in the atmosphere of a beech forest with Allium ursinum (broad-leaved garlic) ground cover plants. Furthermore, it was shown that the Allium plants were the source of the organic sulfur compounds. The atmospheric concentrations of the organic sulfur observed on one day in May 1994 in a suburban forest in Vienna ranged from 0.3 to 7.8 ppb S with an average level of 2.9 ppb S. The atmospheric emission rate of organic sulfur species from A. ursinum determined with an enclosure box was the highest ever reported for terrestrial continental plants. The total organic sulfur flux on the average was at least 1 jug g-1h-1 (plant dry weight) or 60 gmgm-2 h-1 (per unit of ground area).

  6. Sulfuric acid vapor and other cloud-related gases in the Venus atmosphere - Abundances inferred from observed radio opacity

    NASA Technical Reports Server (NTRS)

    Steffes, P. G.; Eshleman, V. R.

    1982-01-01

    It is suggested that the absorbing characteristics of sulfuric acid vapor appear to reconcile what had been thought to be an inconsistency among measurements and deductions regarding the constituents of the Venus atmosphere and radio occultation, radar reflection, and radio emission measurements of its opacity. Laboratory measurements of sulfuric acid, sulfur dioxide, water vapor, and carbon dioxide are used to model relative contributions to opacity as a function of height in a way that is consistent with observations of the constituents and absorbing properties of the atmosphere. It is concluded that sulfuric acid vapor is likely to be the principal microwave absorber in the 30-50 km altitude range of the middle atmosphere of Venus.

  7. Mass-independent fractionation of sulfur isotopes in Archean sediments: strong evidence for an anoxic Archean atmosphere.

    PubMed

    Pavlov, A A; Kasting, J F

    2002-01-01

    Mass-independent fractionation (MIF) of sulfur isotopes has been reported in sediments of Archean and Early Proterozoic Age (> 2.3 Ga) but not in younger rocks. The only fractionation mechanism that is consistent with the data on all four sulfur isotopes involves atmospheric photochemical reactions such as SO2 photolysis. We have used a one-dimensional photochemical model to investigate how the isotopic fractionation produced during SO2 photolysis would have been transferred to other gaseous and particulate sulfur-bearing species in both low-O2 and high-O2 atmospheres. We show that in atmospheres with O2 concentrations < 10(-5) times the present atmospheric level (PAL), sulfur would have been removed from the atmosphere in a variety of different oxidation states, each of which would have had its own distinct isotopic signature. By contrast, in atmospheres with O2 concentrations > or = 10(-5) PAL, all sulfur-bearing species would have passed through the oceanic sulfate reservoir before being incorporated into sediments, so any signature of MIF would have been lost. We conclude that the atmospheric O2 concentration must have been < 10(-5) PAL prior to 2.3 Ga.

  8. Estimation of microwave absorption in the Jupiter atmosphere

    NASA Technical Reports Server (NTRS)

    Coombs, W. C.

    1971-01-01

    A procedure for estimating the microwave absorption loss of the Jupiter atmosphere is presented. Estimation of microwave absorption by planetary atmospheres involves two different investigative disciplines (1) the determination of an acceptable model of the atmosphere itself and (2) the determination of the microwave attenuation rate applicable to each different volume sample of the atmosphere, and the integration of this loss over the varying radio propagation path for any given entry trajectory to obtain the total loss.

  9. Sulfur isotope dynamics in two central european watersheds affected by high atmospheric deposition of SO x

    NASA Astrophysics Data System (ADS)

    Novák, Martin; Kirchner, James W.; Groscheová, Hana; Havel, Miroslav; Černý, Jiří; Krejčí, Radovan; Buzek, František

    2000-02-01

    Sulfur fluxes and δ34S values were determined in two acidified small watersheds located near the Czech-German border, Central Europe. Sulfur of sulfate aerosol in the broader region (mean δ 34S of 7.5‰ CDT) was isotopically heavier than sulfur of airborne SO 2 (mean δ 34S of 4.7‰). The annual atmospheric S deposition to the Jezeřı´ watershed decreased markedly in 1993, 1994, and 1995 (40, 33, and 29 kg/ ha · yr), reflecting reductions in industrial S emissions. Sulfur export from Jezeří via surface discharge was twice atmospheric inputs, and increased from 52 to 58 to 85 kg/ha · yr over the same three-year period. The δ 34S value of Jezeřı´ streamflow was 4.5 ± 0.3‰, intermediate between the average atmospheric deposition (5.4 ± 0.2‰) and soil S (4.0 ± 0.5‰), suggesting that the excess sulfate in runoff comes from release of S from the soil. Bedrock is not a plausible source of the excess S, because its S concentration is very low (<0.003 wt.%) and because its δ 34S value is too high (5.8‰) to be consistent with the δ 34S of runoff. A sulfur isotope mixing model indicated that release of soil S accounted for 64 ± 33% of sulfate S in Jezeřı´ discharge. Approximately 30% of total sulfate S in the discharge were organically cycled. At Načetı´n, the same sequence of δ34S IN > δ34S OUT > δ34S SOIL was observed. The seasonality found in atmospheric input (higher δ 34S in summer, lower δ 34S in winter) was preserved in shallow (<10 cm) soil water, but not in deeper soil water. δ 34S values of deeper (>10 cm) soil water (4.8 ± 0.2‰) were intermediate between those of atmospheric input (5.9 ± 0.3‰) and Nac̆etín soils (2.4 ± 0.1‰), again suggesting that remobilization of soil S accounts for a significant fraction (roughly 40 ± 10%) of the S in soil water at Načetı´n. The inventories of soil S at both of these sites are legacies of more intense atmospheric pollution during previous decades, and are large enough (740

  10. Massive impact-induced release of carbon and sulfur gases in the early Earth's atmosphere

    NASA Astrophysics Data System (ADS)

    Marchi, S.; Black, B. A.; Elkins-Tanton, L. T.; Bottke, W. F.

    2016-09-01

    Recent revisions to our understanding of the collisional history of the Hadean and early-Archean Earth indicate that large collisions may have been an important geophysical process. In this work we show that the early bombardment flux of large impactors (>100 km) facilitated the atmospheric release of greenhouse gases (particularly CO2) from Earth's mantle. Depending on the timescale for the drawdown of atmospheric CO2, the Earth's surface could have been subject to prolonged clement surface conditions or multiple freeze-thaw cycles. The bombardment also delivered and redistributed to the surface large quantities of sulfur, one of the most important elements for life. The stochastic occurrence of large collisions could provide insights on why the Earth and Venus, considered Earth's twin planet, exhibit radically different atmospheres.

  11. A sulfur-based survival strategy for putative phototrophic life in the venusian atmosphere.

    PubMed

    Schulze-Makuch, Dirk; Grinspoon, David H; Abbas, Ousama; Irwin, Louis N; Bullock, Mark A

    2004-01-01

    Several observations indicate that the cloud deck of the venusian atmosphere may provide a plausible refuge for microbial life. Having originated in a hot proto-ocean or been brought in by meteorites from Earth (or Mars), early life on Venus could have adapted to a dry, acidic atmospheric niche as the warming planet lost its oceans. The greatest obstacle for the survival of any organism in this niche may be high doses of ultraviolet (UV) radiation. Here we make the argument that such an organism may utilize sulfur allotropes present in the venusian atmosphere, particularly S(8), as a UV sunscreen, as an energy-converting pigment, or as a means for converting UV light to lower frequencies that can be used for photosynthesis. Thus, life could exist today in the clouds of Venus.

  12. Unsteady absorption of sulfur dioxide by an atmospheric water droplet with internal circulation

    NASA Astrophysics Data System (ADS)

    Chen, Wei-Hsin

    Unsteady absorption characteristics of sulfur dioxide by an atmospheric water droplet in motion are predicted numerically and analyzed theoretically to recognize the physical mass transport processes inside an aerosol droplet, which is frequently encountered in the atmosphere. Considering the absorption of sulfur dioxide by a droplet in cloud or fog with various velocities, three different Reynolds numbers, viz., Reg=0.643, 1.287, and 12.87 are studied and compared with each other. The results indicate that for the Reynolds number of 0.643, sulfur dioxide always penetrates toward the droplet centerline throughout the entire absorption period. This is due to the mass transfer dominated by diffusion along the radial direction. In contrast, when the Reynolds number is 12.87, the strength of the vortex motion inside the droplet is strong enough. It results in that, most of the time the concentration contours parallel the streamlines and the lowest SO 2 concentration is located at the vortex center. As a consequence, the diffusion distance is reduced by a factor of three and the absorption time for the droplet reaching the saturated state is shortened in a significant way. With regard to an intermediate Reynolds number such as 1.287, a two-stage mass transfer process can be clearly identified. In the first stage, it is dominated by one-dimensional diffusion, in which over 50% sulfur dioxide is absorbed before the saturated state is reached. In the second stage, the vortex motion mainly controls the mass transfer. However, the contour core is inconsistent with the vortex center. This is because the characteristic time of mass diffusion is in a comparable state with that of droplet internal circulation. The present study elucidates that the strength of a droplet's internal motion plays a vital role in determining SO 2 absorption process.

  13. Estimating atmospheric parameters and reducing noise for multispectral imaging

    DOEpatents

    Conger, James Lynn

    2014-02-25

    A method and system for estimating atmospheric radiance and transmittance. An atmospheric estimation system is divided into a first phase and a second phase. The first phase inputs an observed multispectral image and an initial estimate of the atmospheric radiance and transmittance for each spectral band and calculates the atmospheric radiance and transmittance for each spectral band, which can be used to generate a "corrected" multispectral image that is an estimate of the surface multispectral image. The second phase inputs the observed multispectral image and the surface multispectral image that was generated by the first phase and removes noise from the surface multispectral image by smoothing out change in average deviations of temperatures.

  14. Indicating atmospheric sulfur by means of S-isotope in leaves of the plane, osmanthus and camphor trees.

    PubMed

    Xiao, Hua-Yun; Wang, Yan-Li; Tang, Cong-Guo; Liu, Cong-Qiang

    2012-03-01

    Foliar δ(34)S values of three soil-growing plant species (Platanus Orientalis L., Osmanthus fragrans L. and Cinnamomum camphora) have been analyzed to indicate atmospheric sulfur. The foliar δ(34)S values of the three plant species averaged -3.11±1.94‰, similar to those of both soil sulfur (-3.73±1.04‰) and rainwater sulfate (-3.07±2.74‰). This may indicate that little isotopic fractionation had taken place in the process of sulfur uptake by root or leaves. The δ(34)S values changed little in the transition from mature leaves to old/senescing leaves for both the plane tree and the osmanthus tree, suggestive of little isotope effect during sulfur redistribution in plant tissues. Significantly linear correlation between δ(34)S values of leaves and rainwater sulfate for the plane and osmanthus trees allowed the tracing of temporal variations of atmospheric sulfur by means of foliar sulfur isotope, while foliage δ(34)S values of the camphor is not an effective indicator of atmospheric sulfur.

  15. Trifluoromethyl sulfur pentafluoride and its relationship to sulfur hexafluoride and chlorofluorocarbon-12 in the atmosphere near the New York City metropolitan area

    NASA Astrophysics Data System (ADS)

    Erboy, Yasemin; Smethie, William M.

    2012-08-01

    Trifluoromethyl sulfur pentafluoride (SF5CF3), sulfur hexafluoride (SF6) and dichlorodifluoromethane (CCl2F2) (also referred to as CFC-12) were measured simultaneously in the atmosphere at a site 25 km north of New York City over a period of 6 months with continuous measurements every 25 min for 4 months. The SF5CF3 record showed little variability and its concentration appeared close to the remote atmospheric concentration. The concentrations of SF6 and CFC-12 had numerous spikes well in excess of their remote atmospheric concentrations indicating the presence of local sources. The lack of SF5CF3 spikes reveals that the usage of SF6 in the New York metropolitan area does not result in significant production of SF5CF3, and also that there is no significant production by industrial and manufacturing processes in the region.

  16. Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules

    PubMed Central

    Schobesberger, Siegfried; Junninen, Heikki; Bianchi, Federico; Lönn, Gustaf; Ehn, Mikael; Lehtipalo, Katrianne; Dommen, Josef; Ehrhart, Sebastian; Ortega, Ismael K.; Franchin, Alessandro; Nieminen, Tuomo; Riccobono, Francesco; Hutterli, Manuel; Duplissy, Jonathan; Almeida, João; Amorim, Antonio; Breitenlechner, Martin; Downard, Andrew J.; Dunne, Eimear M.; Flagan, Richard C.; Kajos, Maija; Keskinen, Helmi; Kirkby, Jasper; Kupc, Agnieszka; Kürten, Andreas; Kurtén, Theo; Laaksonen, Ari; Mathot, Serge; Onnela, Antti; Praplan, Arnaud P.; Rondo, Linda; Santos, Filipe D.; Schallhart, Simon; Schnitzhofer, Ralf; Sipilä, Mikko; Tomé, António; Tsagkogeorgas, Georgios; Vehkamäki, Hanna; Wimmer, Daniela; Baltensperger, Urs; Carslaw, Kenneth S.; Curtius, Joachim; Hansel, Armin; Petäjä, Tuukka; Kulmala, Markku; Donahue, Neil M.; Worsnop, Douglas R.

    2013-01-01

    Atmospheric aerosols formed by nucleation of vapors affect radiative forcing and therefore climate. However, the underlying mechanisms of nucleation remain unclear, particularly the involvement of organic compounds. Here, we present high-resolution mass spectra of ion clusters observed during new particle formation experiments performed at the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research. The experiments involved sulfuric acid vapor and different stabilizing species, including ammonia and dimethylamine, as well as oxidation products of pinanediol, a surrogate for organic vapors formed from monoterpenes. A striking resemblance is revealed between the mass spectra from the chamber experiments with oxidized organics and ambient data obtained during new particle formation events at the Hyytiälä boreal forest research station. We observe that large oxidized organic compounds, arising from the oxidation of monoterpenes, cluster directly with single sulfuric acid molecules and then form growing clusters of one to three sulfuric acid molecules plus one to four oxidized organics. Most of these organic compounds retain 10 carbon atoms, and some of them are remarkably highly oxidized (oxygen-to-carbon ratios up to 1.2). The average degree of oxygenation of the organic compounds decreases while the clusters are growing. Our measurements therefore connect oxidized organics directly, and in detail, with the very first steps of new particle formation and their growth between 1 and 2 nm in a controlled environment. Thus, they confirm that oxidized organics are involved in both the formation and growth of particles under ambient conditions. PMID:24101502

  17. Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules.

    PubMed

    Schobesberger, Siegfried; Junninen, Heikki; Bianchi, Federico; Lönn, Gustaf; Ehn, Mikael; Lehtipalo, Katrianne; Dommen, Josef; Ehrhart, Sebastian; Ortega, Ismael K; Franchin, Alessandro; Nieminen, Tuomo; Riccobono, Francesco; Hutterli, Manuel; Duplissy, Jonathan; Almeida, João; Amorim, Antonio; Breitenlechner, Martin; Downard, Andrew J; Dunne, Eimear M; Flagan, Richard C; Kajos, Maija; Keskinen, Helmi; Kirkby, Jasper; Kupc, Agnieszka; Kürten, Andreas; Kurtén, Theo; Laaksonen, Ari; Mathot, Serge; Onnela, Antti; Praplan, Arnaud P; Rondo, Linda; Santos, Filipe D; Schallhart, Simon; Schnitzhofer, Ralf; Sipilä, Mikko; Tomé, António; Tsagkogeorgas, Georgios; Vehkamäki, Hanna; Wimmer, Daniela; Baltensperger, Urs; Carslaw, Kenneth S; Curtius, Joachim; Hansel, Armin; Petäjä, Tuukka; Kulmala, Markku; Donahue, Neil M; Worsnop, Douglas R

    2013-10-22

    Atmospheric aerosols formed by nucleation of vapors affect radiative forcing and therefore climate. However, the underlying mechanisms of nucleation remain unclear, particularly the involvement of organic compounds. Here, we present high-resolution mass spectra of ion clusters observed during new particle formation experiments performed at the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research. The experiments involved sulfuric acid vapor and different stabilizing species, including ammonia and dimethylamine, as well as oxidation products of pinanediol, a surrogate for organic vapors formed from monoterpenes. A striking resemblance is revealed between the mass spectra from the chamber experiments with oxidized organics and ambient data obtained during new particle formation events at the Hyytiälä boreal forest research station. We observe that large oxidized organic compounds, arising from the oxidation of monoterpenes, cluster directly with single sulfuric acid molecules and then form growing clusters of one to three sulfuric acid molecules plus one to four oxidized organics. Most of these organic compounds retain 10 carbon atoms, and some of them are remarkably highly oxidized (oxygen-to-carbon ratios up to 1.2). The average degree of oxygenation of the organic compounds decreases while the clusters are growing. Our measurements therefore connect oxidized organics directly, and in detail, with the very first steps of new particle formation and their growth between 1 and 2 nm in a controlled environment. Thus, they confirm that oxidized organics are involved in both the formation and growth of particles under ambient conditions.

  18. Target loads of atmospheric sulfur and nitrogen deposition for protection of acid sensitive aquatic resources in the Adirondack Mountains, New York

    USGS Publications Warehouse

    Sullivan, T.J.; Cosby, B.J.; Driscoll, C.T.; McDonnell, T.C.; Herlihy, A.T.; Burns, Douglas A.

    2012-01-01

    The dynamic watershed acid-base chemistry model of acidification of groundwater in catchments (MAGIC) was used to calculate target loads (TLs) of atmospheric sulfur and nitrogen deposition expected to be protective of aquatic health in lakes in the Adirondack ecoregion of New York. The TLs were calculated for two future dates (2050 and 2100) and three levels of protection against lake acidification (acid neutralizing capacity (ANC) of 0, 20, and 50 eq L -1). Regional sulfur and nitrogen deposition estimates were combined with TLs to calculate exceedances. Target load results, and associated exceedances, were extrapolated to the regional population of Adirondack lakes. About 30% of Adirondack lakes had simulated TL of sulfur deposition less than 50 meq m -2 yr to protect lake ANC to 50 eq L -1. About 600 Adirondack lakes receive ambient sulfur deposition that is above this TL, in some cases by more than a factor of 2. Some critical criteria threshold values were simulated to be unobtainable in some lakes even if sulfur deposition was to be decreased to zero and held at zero until the specified endpoint year. We also summarize important lessons for the use of target loads in the management of acid-impacted aquatic ecosystems, such as those in North America, Europe, and Asia. Copyright 2012 by the American Geophysical Union.

  19. Venus volcanism: Rate estimates from laboratory studies of sulfur gas-solid reactions

    NASA Technical Reports Server (NTRS)

    Ehlers, K.; Fegley, B., Jr.; Prinn, R. G.

    1989-01-01

    Thermochemical reactions between sulfur-bearing gases in the atmosphere of Venus and calcium-, iron-, magnesium-, and sulfur-bearing minerals on the surface of Venus are an integral part of a hypothesized cycle of thermochemical and photochemical reactions responsible for the maintenance of the global sulfuric acid cloud cover on Venus. SO2 is continually removed from the Venus atmosphere by reaction with calcium bearing minerals on the planet's surface. The rate of volcanism required to balance SO2 depletion by reactions with calcium bearing minerals on the Venus surface can therefore be deduced from a knowledge of the relevant gas-solid reaction rates combined with reasonable assumptions about the sulfur content of the erupted material (gas + magma). A laboratory program was carried out to measure the rates of reaction between SO2 and possible crustal minerals on Venus. The reaction of CaCO3(calcite) + SO2 yields CaSO4 (anhydrite) + CO was studied. Brief results are given.

  20. Variations in the magnitude of non mass dependent sulfur fractionation in the Archean atmosphere

    NASA Astrophysics Data System (ADS)

    Claire, M.; Kasting, J. F.

    2010-12-01

    Recent experimental data have enabled quantitatively meaningful computations of the non-mass dependent fractionation of sulfur’s isotopes (Δ33S) that exemplify the Archean rock record. The Δ33S signal originates as a result of fine structure in the absorption cross-section of SO2 isotopologues [1], which only undergo significant photolysis in reducing atmospheres [2]. The Δ33S signal produced by SO2 photolysis varies significantly between 190 and 220 nm, and thus is strongly dependent on any other atmospheric gases which absorb photons in this range [3], as well as the height at which photolysis occurs. A model that is capable of resolving the altitude-dependent radiative transfer through a realistic self-consistent reducing atmosphere is therefore essential when making direct comparisons between atmospheric Δ33S production and the rock record. In this work, we investigate how the magnitude of Δ33S might vary as function of atmospheric composition, which in turn allows the rock record to constrain the Archean atmosphere. Other recent work on this topic using simplied atmospheric models has implicated large concentrations of SO2 [5], OCS [3], and CO2 [6] as being responsible for the variations in Archean Δ33S. We present results from an altitude-dependent photochemical model of Archean photochemistry [4] of necessary complexity to resolve the complicated redox structure of the Archean atmosphere. We show that while increased concentrations of these gases all affect Δ33S in an unconstrained model, the atmospheric conditions required for OCS or SO2 shielding are unlikely to occur in an Archean atmosphere constrained by reasonable expectations of volcanic and biogenic fluxes. Within the context of plausible Archean atmospheres, we investigate how shielding due to changing amounts of CO2, biogenic sulfur gases, and fractal organic haze [7] affect the magnitude of Δ33S produced by the Archean atmosphere, and show why simplified atmospheric modeling may lead to

  1. Laboratory studies of atmospheric sulfur chemistry using tunable diode laser probes

    SciTech Connect

    Stickel, R.E.; Urbanski, S.P.; Zhao, Z.; Wine, P.H.

    1996-12-31

    Tunable lead-salt diode laser absorption spectroscopy (TDLAS) provides a sensitive and versatile probe for the study of the kinetics and mechanisms of atmospheric reactions. In the laboratory, the combination of laser flash photolysis with TDLAS detection of reactant and/or product species has proven useful in several studies of the gas phase oxidation of the atmospheric sulfur compound dimethylsulfide (DMS), a process which may play an important role in global climate modification/regulation. Typically a radical species is produced by UV laser photolysis of a stable precursor in a slowly flowing mixture of reactant and buffer gases. The concentration of this radical or a selected reaction product is then followed by TDLAS on a time scale of microseconds to milliseconds. This method allows direct determination of reaction rates and product branching ratios over a range of temperature, pressure and reactant concentrations in complete isolation from reactor surfaces.

  2. Impact of anthropogenic atmospheric nitrogen and sulfur deposition on ocean acidification and the inorganic carbon system.

    PubMed

    Doney, Scott C; Mahowald, Natalie; Lima, Ivan; Feely, Richard A; Mackenzie, Fred T; Lamarque, Jean-Francois; Rasch, Phil J

    2007-09-11

    Fossil fuel combustion and agriculture result in atmospheric deposition of 0.8 Tmol/yr reactive sulfur and 2.7 Tmol/yr nitrogen to the coastal and open ocean near major source regions in North America, Europe, and South and East Asia. Atmospheric inputs of dissociation products of strong acids (HNO(3) and H2SO(4)) and bases (NH(3)) alter surface seawater alkalinity, pH, and inorganic carbon storage. We quantify the biogeochemical impacts by using atmosphere and ocean models. The direct acid/base flux to the ocean is predominately acidic (reducing total alkalinity) in the temperate Northern Hemisphere and alkaline in the tropics because of ammonia inputs. However, because most of the excess ammonia is nitrified to nitrate (NO(3)(-)) in the upper ocean, the effective net atmospheric input is acidic almost everywhere. The decrease in surface alkalinity drives a net air-sea efflux of CO(2), reducing surface dissolved inorganic carbon (DIC); the alkalinity and DIC changes mostly offset each other, and the decline in surface pH is small. Additional impacts arise from nitrogen fertilization, leading to elevated primary production and biological DIC drawdown that reverses in some places the sign of the surface pH and air-sea CO(2) flux perturbations. On a global scale, the alterations in surface water chemistry from anthropogenic nitrogen and sulfur deposition are a few percent of the acidification and DIC increases due to the oceanic uptake of anthropogenic CO(2). However, the impacts are more substantial in coastal waters, where the ecosystem responses to ocean acidification could have the most severe implications for mankind.

  3. Enhanced acid rain and atmospheric deposition of nitrogen, sulfur and heavy metals in Northern China

    NASA Astrophysics Data System (ADS)

    Pan, Y.; Wang, Y.

    2013-12-01

    Atmospheric deposition is known to be important mechanism reducing air pollution. In response to the growing concern on the potential effects of the deposited material entering terrestrial and aquatic environments as well as their subsequent health effects, since 2007 we have established a 10-site monitoring network in Northern China, where particularly susceptible to severe air pollution. Wet and dry deposition was collected using an automatic wet-dry sampler. The presentation will focus on the new results of atmospheric deposition flux for a number of chemical species, such as nutrients (e.g. nitrogen and phosphorus), acidic matters (e.g. sulfur and proton), heavy metals and Polycyclic Aromatic Hydrocarbons, etc. This is to our knowledge the first detailed element budget study in the atmosphere across Northern China. We find that: (1) Over the 3 year period, 26% of precipitation events in the target area were more acid than pH 5.60 and these acidic events occurred in summer and autumn. The annual volume-weighted mean (VWM) pH value of precipitation was lower than 5.60 at most sites, which indicated the acidification of precipitation was not optimistic. The primary ions in precipitation were NH4+, Ca2+, SO42- and NO3-, with 10-sites-average concentrations of 221, 216, 216 and 80 μeq L-1, respectively. The ratio of SO42- to NO3- was 2.7; suggesting SO42- was the dominant acid component. (2) The deposited particles were neutral in general and the pH value increased from rural area to industrial and coastal sites. It is not surprising to note that the annual VWM pH value of precipitation was higher than 5.60 at three urban sites (Beijing and Tianjin mega cities) and one coastal site near the Bohai Bay, considering the fact that high buffer capacity of alkaline component, gas NH3 and mineral aerosols, at these sites compared to other places. (3) The 10-sites annual total deposition amounts for sulfur and nitrogen compounds were 60 and 65 kg N/S ha-1 yr-1

  4. Multiple sulfur isotope geochemistry of Dharwar Supergroup, Southern India: Late Archean record of changing atmospheric chemistry

    NASA Astrophysics Data System (ADS)

    Mishima, Kaoru; Yamazaki, Rie; Satish-Kumar, Madhusoodhan; Ueno, Yuichiro; Hokada, Tomokazu; Toyoshima, Tsuyoshi

    2017-04-01

    Earth's tectonic and climatic systems may have changed fundamentally before the Great Oxidation Event (GOE) at about 2.3 Ga. Sulfur Mass Independent Fractionation (S-MIF) has demonstrated that Earth's atmosphere was virtually oxygen-free before the GOE. During 3.0 to 2.4 Ga, the change in Δ33S and Δ36S signals may reflect the perturbation of atmospheric chemistry, though the mechanisms of the change are uncertain. Here, we reported multiple sulfur isotopic studies of Archean volcano-sedimentary sequences of the Dharwar Supergroup, distributed in the Chitradurga Schist Belt (CSB), Southern India. New field mapping and zircon U-Pb dating allows us to reconstruct detailed lithostratigraphy of the Dharwar Supergroup. The lower unit consists of post-3.0 Ga conglomerate, stromatolitic carbonate, siliciclastics with diamictite, chert/BIF and pillowed basalt in ascending order, all of which are older than the 2676 Ma dacite dyke that had intruded into the lower unit. The upper unit unconformably overlies the pillow basalts at the top of the lower unit, and consists of conglomerate/sandstone with ∼2600 Ma detrital zircons, komatiitic basalt, BIF and siliciclastic sequence with mafic volcanics. Sulfur isotope analysis of extracted sulfides shows MIF signals (Δ33S > + 1 ‰) with clear Δ33S- Δ36S correlations. The lower group of the Dharwar Supergroup shows a Δ36S / Δ33S slope of -1.48, the middle group shows -1.16 and -1.07, and the upper group shows -0.94. Reassessment of all the Archean S-MIF records from sedimentary rocks indicates that the Δ36S / Δ33S slope systematically changed during the Archean period. The observed trend in the Indian section is similar to those of its Pilbara-Kaapvaal equivalents, thus it could reflect a global atmospheric signature. Moreover, the isotopic trend seems to correlate with mid-Archean glaciation. Thus, the Δ36S / Δ33S slope could be a useful tracer for atmospheric chemistry and its link with climate change before the GOE.

  5. Atmospheric visibility estimation and image contrast calibration

    NASA Astrophysics Data System (ADS)

    Hermansson, Patrik; Edstam, Klas

    2016-10-01

    A method, referred to as contrast calibration, has been developed for transforming digital color photos of outdoor scenes from the atmospheric conditions, illumination and visibility, prevailing at the time of capturing the image to a corresponding image for other atmospheric conditions. A photo captured on a hazy day can, for instance, be converted to resemble a photo of the same scene for good visibility conditions. Converting digital color images to specified lightning and transmission conditions is useful for image based assessment of signature suppression solutions. The method uses "calibration objects" which are photographed at about the same time as the scene of interest. The calibration objects, which (indirectly) provide information on visibility and lightning conditions, consist of two flat boards, painted in different grayscale colors, and a commercial, neutral gray, reference card. Atmospheric extinction coefficient and sky intensity can be determined, in three wavelength bands, from image pixel values on the calibration objects and using this information the image can be converted to other atmospheric conditions. The image is transformed in contrast and color. For illustration, contrast calibration is applied to sample images of a scene acquired at different times. It is shown that contrast calibration of the images to the same reference values of extinction coefficient and sky intensity results in images that are more alike than the original images. It is also exemplified how images can be transformed to various other atmospheric weather conditions. Limitations of the method are discussed and possibilities for further development are suggested.

  6. Decreased atmospheric sulfur deposition across the southeastern U.S.: When will watersheds release stored sulfate?

    USGS Publications Warehouse

    Rice, Karen C.; Scanlon, Todd M.; Lynch, Jason A.; Cosby, Bernard J.

    2014-01-01

    Emissions of sulfur dioxide (SO2) to the atmosphere lead to atmospheric deposition of sulfate (SO42-), which is the dominant strong acid anion causing acidification of surface waters and soils in the eastern United States (U.S.). Since passage of the Clean Air Act and its Amendments, atmospheric deposition of SO2 in this region has declined by over 80%, but few corresponding decreases in stream-water SO42- concentrations have been observed in unglaciated watersheds. We calculated SO42- mass balances for 27 forested, unglaciated watersheds from Pennsylvania to Georgia, by using total atmospheric deposition (wet plus dry) as input. Many of these watersheds still retain SO42-, unlike their counterparts in the northeastern U.S. and southern Canada. Our analysis showed that many of these watersheds should convert from retaining to releasing SO42- over the next two decades. The specific years when the watersheds crossover from retaining to releasing SO42- correspond to a general geographical pattern of later net watershed release from north to south. The single most important variable that explained the crossover year was the runoff ratio, defined as the ratio of annual mean stream discharge to precipitation. Percent clay content and mean soil depth were secondary factors in predicting crossover year. The conversion of watersheds from net SO42- retention to release anticipates more widespread reductions in stream-water SO42- concentrations in this region.

  7. Decreased Atmospheric Sulfur Deposition Across the Southeastern U.S.: When Will Watersheds Release Stored Sulfate?

    NASA Astrophysics Data System (ADS)

    Rice, K. C.; Scanlon, T. M.; Lynch, J. A.; Cosby, B. J., Jr.

    2014-12-01

    Emissions of sulfur dioxide (SO2) to the atmosphere lead to atmospheric deposition of sulfate (SO42-), which is the dominant strong acid anion causing acidification of surface waters and soils in the eastern United States (U.S.). Since passage of the Clean Air Act and its Amendments, atmospheric deposition of SO2 in this region has declined by over 80%, but few corresponding decreases in stream-water SO42- concentrations have been observed in unglaciated watersheds. We calculated SO42- mass balances for 27 forested, unglaciated watersheds from Pennsylvania to Georgia, by using total atmospheric deposition (wet plus dry) as input. Many of these watersheds still retain SO42-, unlike their counterparts in the northeastern U.S. and southern Canada. Our analysis showed that many of these watersheds should convert from retaining to releasing SO42- over the next two decades. The specific years when the watersheds crossover from retaining to releasing SO42- correspond to a general geographical pattern of later net watershed release from north to south. The single most important variable that explained the crossover year was the runoff ratio, defined as the ratio of annual mean stream discharge to precipitation. Percent clay content and mean soil depth were secondary factors in predicting crossover year. The conversion of watersheds from net SO42- retention to release anticipates more widespread reductions in stream-water SO42- concentrations in this region.

  8. Atmospheric Turbulence Estimates from a Pulsed Lidar

    NASA Technical Reports Server (NTRS)

    Pruis, Matthew J.; Delisi, Donald P.; Ahmad, Nash'at N.; Proctor, Fred H.

    2013-01-01

    Estimates of the eddy dissipation rate (EDR) were obtained from measurements made by a coherent pulsed lidar and compared with estimates from mesoscale model simulations and measurements from an in situ sonic anemometer at the Denver International Airport and with EDR estimates from the last observation time of the trailing vortex pair. The estimates of EDR from the lidar were obtained using two different methodologies. The two methodologies show consistent estimates of the vertical profiles. Comparison of EDR derived from the Weather Research and Forecast (WRF) mesoscale model with the in situ lidar estimates show good agreement during the daytime convective boundary layer, but the WRF simulations tend to overestimate EDR during the nighttime. The EDR estimates from a sonic anemometer located at 7.3 meters above ground level are approximately one order of magnitude greater than both the WRF and lidar estimates - which are from greater heights - during the daytime convective boundary layer and substantially greater during the nighttime stable boundary layer. The consistency of the EDR estimates from different methods suggests a reasonable ability to predict the temporal evolution of a spatially averaged vertical profile of EDR in an airport terminal area using a mesoscale model during the daytime convective boundary layer. In the stable nighttime boundary layer, there may be added value to EDR estimates provided by in situ lidar measurements.

  9. Properties and Atmospheric Implication of Methylamine-Sulfuric Acid-Water Clusters.

    PubMed

    Lv, Sha-Sha; Miao, Shou-Kui; Ma, Yan; Zhang, Miao-Miao; Wen, Yang; Wang, Chun-Yu; Zhu, Yu-Peng; Huang, Wei

    2015-08-13

    The presence of amines can increase aerosol formation rates. Most studies have been devoted to dimethylamine as the representative of amine; however, there have been a few works devoted to methylamine. In this study, theoretical calculations are performed on CH3NH2(H2SO4)m(H2O)n (m = 0-3, n = 0-3) clusters. In addition to the structures and energetics, we focused on determining the following characteristics: (1) the growth mechanism, (2) the hydrate distributions and the influences of humidity and temperature, (3) Rayleigh scattering properties. We explored the cluster growth mechanism from a thermodynamics aspect by calculating the Gibbs free energy of adding a water or sulfuric acid molecule step by step at three atmospherically relevant temperatures. The relative ease of the reaction at each step is discussed. From the analysis of hydrate distributions, we find that CH3NH2(H2SO4)(H2O)2, CH3NH2(H2SO4)2, and CH3NH2(H2SO4)3 are most likely to exist in the atmosphere. The general trend of hydration in all cases is more extensive with the growing relative humidity (RH), whereas the distributions do not significantly change with the temperature. Analysis of the Rayleigh scattering properties showed that both H2SO4 and H2O molecules could increase the Rayleigh scattering intensities and isotropic mean polarizabilities, with greater influence by the sulfuric acid molecules. This work sheds light on the mechanism for further research on new particle formation (NPF) containing methylamine in the atmosphere.

  10. Modelling of the Chemistry of Sulfur Oxides in the Middle Atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Mills, F. P.; Johri, S.; Yung, Y. L.; Allen, M.

    2009-05-01

    Venus' middle atmosphere (˜ 60-110 km) is a dynamic region in which photochemistry dominates and the time scales for chemical loss and transport are roughly comparable for many species. It is also a region where it has been difficult to observe the abundances of species that play important roles in two of the dominant chemical cycles on Venus. The CO2 cycle comprises photodissociation of CO2 to produce CO and O, transport of some CO and O to the night side, production of O2 from 2O+M→O2+M on the day and night sides, and production of CO2 from CO and O2. The sulfur oxidation cycle comprises oxidation of SO2 to form H2SO4, condensation, subsidence of some particles to the lower atmosphere, evaporation, and thermal decomposition or photodissociation to produce SO2 and H2O. Recent mesospheric observations have provided clear evidence of diurnal variability in the abundances of sulfur oxides. Observed SO has its peak abundance on the day side and observed SO2 has its peak abundance on the night side (Sandor et al, 2008). We have used global average model calculations (Pernice et al, 2004; Mills and Allen, 2007) to derive approximate analytic expressions for [SO], [SO2], and [SO]/[SO2] on the day and night sides. The results are generally consistent across a broad range of atmospheric oxidation states (Mills and Allen, 2007). Our model results and the key uncertainties will be discussed. A related topic is the identity of the UV-blue absorber that is responsible for the absorption observed in the upper cloud layer (˜ 60-70 km) at 320-500 nm. One proposed suggestion is S2O (Hapke and Graham, 1985; Na and Esposito, 1997). Our model results for S2O and their implications will be discussed and compared with previous work.

  11. Spatial distribution and seasonal variations of atmospheric sulfur deposition over Northern China

    NASA Astrophysics Data System (ADS)

    Pan, Y. P.; Wang, Y. S.; Tang, G. Q.; Wu, D.

    2012-09-01

    The increasing anthropogenic emissions of acidic compounds have induced acid deposition accompanied by acidification in the aquatic and terrestrial ecosystems worldwide. However, comprehensive assessment of spatial patterns and long-term trends of acid deposition in China remains a challenge due to a paucity of field-based measurement data, in particular for dry deposition. Here we quantify the sulfur (S) deposition on a regional scale via precipitation, particles and gases during a 3-yr observation campaign at ten selected sites in Northern China. Results show that the total S deposition flux in the target area ranged from 35.0 to 100.7 kg S ha-1 yr-1, categorized as high levels compared to those documented in Europe, North America, and East Asia. The ten-site, 3-yr average total S deposition was 64.8 kg S ha-1 yr-1, with 32% attributed to wet deposition, and the rest attributed to dry deposition. Compared with particulate sulfate, gaseous SO2 was the major contributor of dry-deposited S, contributing approximately 49% to the total flux. Wet deposition of sulfate showed pronounced seasonal variations with maximum in summer and minimum in winter, corresponding to precipitation patterns in Northern China. However, the spatial and inter-annual differences in the wet deposition were not significant, which were influenced by the precipitation amount, scavenging ratio and the concentrations of atmospheric S compounds. In contrast, the relatively large dry deposition of SO2 and sulfate during cold season, especially at industrial areas, was reasonably related to the local emissions from home heating. Although seasonal fluctuations were constant, clear spatial differences were observed in the total S deposition flux and higher values were also found in industrial areas with huge emissions of SO2. These findings indicate that human activity has dramatically altered the atmospheric S deposition and thus regional S cycles. To systematically illustrate the potential effects

  12. Atmospheric Observations of Aerosol Sizes, Sulfuric Acid and Ammonia Measured in Kent, Ohio

    NASA Astrophysics Data System (ADS)

    Pavuluri, C.; Benson, D. R.; Dailey, B.; Lee, S.

    2008-12-01

    Atmospheric particles affect atmospheric composition, cloud formation, global radiation budget, and human health. Nucleation is a gas-to-particle conversion process in which new particles form directly from gas phase species and is a key process that controls particle number concentrations. The most common feature of the new particle formation events is a substantial increase of number concentrations of nucleation mode particles reaching up to 105-106 cm-3 in the condensable vapor-laden air. There are several nucleation mechanisms for tropopsheric aerosol formation, but it is unclear which nucleation process dominates. In particular, observations and modeling studies show that ammonia can be important for atmospheric nucleation in the boundary layer, but simultaneous measurements of aerosol sizes and precursors including sulfuric acid and ammonia are critically lacking. In order to overcome these shortcomings, we conduct atmospheric observations of new particle formation in Kent, OH. We have measured aerosol sizes and concentrations for particles in the size range from 3-102 nm semi- continuously from December 2005 and for particles from 3-1000 nm continuously from September 2007 in Kent State campus, Kent, OH (with an inlet placed at ~11.5 m above ground level). We also simultaneously measure sulfuric acid and ammonia, two most important inorganic aerosol precursors, with two chemical ionization mass spectrometers (CIMS) from August 2008. Kent, located in Northeastern Ohio, is relatively rural itself, but is also surrounded by several urban cities within 40 miles. Because of the combination of its relatively rural environment (hence low surface areas of aerosol particles), active vegetation (organic and NH3 emissions), and possible transport of aerosol precursors from the surrounding urban and industrialized areas, Kent is a unique location to make new particle formation studies. So far, most of new particle formation observations made typically in US were at

  13. Sulfur dioxide in the atmosphere of Venus 1 sounding rocket observations

    NASA Technical Reports Server (NTRS)

    Mcclintock, William E.; Barth, Charles A.; Kohnert, Richard A.

    1994-01-01

    In this paper we present ultraviolet reflectance spectra obtained during two sounding rocket observations of Venus made during September 1988 and March 1991. We describe the sensitivity of the derived reflectance to instrument calibration and show that significant artifacts can appear in that spectrum as a result of using separate instruments to observe both the planetary radiance and the solar irradiance. We show that sulfur dioxide is the primary spectral absorber in the 190 - 230 nm region and that the range of altitudes probed by these wavelengths is very sensitive to incidence and emission angles. In a following paper Na et. al. (1994) show that sulfur monoxide features are also present in these data. Accurate identification and measurement of additional species require observations in which both the planetary radiance and the solar irradiance are measured with the same instrument. The instrument used for these observations is uniquely suited for obtaining large phase angle coverage and for studying transient atmospheric events on Venus because it can observe targets within 18 deg of the sun while earth orbiting instruments are restricted to solar elongation angles greater than or equal to 45 deg.

  14. Kalman-variant estimators for state of charge in lithium-sulfur batteries

    NASA Astrophysics Data System (ADS)

    Propp, Karsten; Auger, Daniel J.; Fotouhi, Abbas; Longo, Stefano; Knap, Vaclav

    2017-03-01

    Lithium-sulfur batteries are now commercially available, offering high specific energy density, low production costs and high safety. However, there is no commercially-available battery management system for them, and there are no published methods for determining state of charge in situ. This paper describes a study to address this gap. The properties and behaviours of lithium-sulfur are briefly introduced, and the applicability of 'standard' lithium-ion state-of-charge estimation methods is explored. Open-circuit voltage methods and 'Coulomb counting' are found to have a poor fit for lithium-sulfur, and model-based methods, particularly recursive Bayesian filters, are identified as showing strong promise. Three recursive Bayesian filters are implemented: an extended Kalman filter (EKF), an unscented Kalman filter (UKF) and a particle filter (PF). These estimators are tested through practical experimentation, considering both a pulse-discharge test and a test based on the New European Driving Cycle (NEDC). Experimentation is carried out at a constant temperature, mirroring the environment expected in the authors' target automotive application. It is shown that the estimators, which are based on a relatively simple equivalent-circuit-network model, can deliver useful results. If the three estimators implemented, the unscented Kalman filter gives the most robust and accurate performance, with an acceptable computational effort.

  15. Direct night-time ejection of particle-phase reduced biogenic sulfur compounds from the ocean to the atmosphere.

    PubMed

    Gaston, Cassandra J; Furutani, Hiroshi; Guazzotti, Sergio A; Coffee, Keith R; Jung, Jinyoung; Uematsu, Mitsuo; Prather, Kimberly A

    2015-04-21

    The influence of oceanic biological activity on sea spray aerosol composition, clouds, and climate remains poorly understood. The emission of organic material and gaseous dimethyl sulfide (DMS) from the ocean represents well-documented biogenic processes that influence particle chemistry in marine environments. However, the direct emission of particle-phase biogenic sulfur from the ocean remains largely unexplored. Here we present measurements of ocean-derived particles containing reduced sulfur, detected as elemental sulfur ions (e.g., (32)S(+), (64)S2(+)), in seven different marine environments using real-time, single particle mass spectrometry; these particles have not been detected outside of the marine environment. These reduced sulfur compounds were associated with primary marine particle types and wind speeds typically between 5 and 10 m/s suggesting that these particles themselves are a primary emission. In studies with measurements of seawater properties, chlorophyll-a and atmospheric DMS concentrations were typically elevated in these same locations suggesting a biogenic source for these sulfur-containing particles. Interestingly, these sulfur-containing particles only appeared at night, likely due to rapid photochemical destruction during the daytime, and comprised up to ∼67% of the aerosol number fraction, particularly in the supermicrometer size range. These sulfur-containing particles were detected along the California coast, across the Pacific Ocean, and in the southern Indian Ocean suggesting that these particles represent a globally significant biogenic contribution to the marine aerosol burden.

  16. Comparison between Sulfur Dioxide estimates using COSPEC and MODIS images

    NASA Astrophysics Data System (ADS)

    Jimenez-Escalona, Jose Carlos; Monsivais-Huertero, Alejandro; Ddelgado-Granados, Hugo

    2015-04-01

    The purpose of this work is to show the synergy of both remote sensing methods in order to utilize information derived from these two techniques for continuous volcano monitoring. Particularly, this paper aims at (1) showing the advantages and disadvantages of both techniques individually and (2) Comparing both sources of measurements and (3) coupling the dynamics showed by COSPEC measurements and static satellite image (MODIS) information. For this end, we use as a case of study the emissions of Popocatépetl volcano between November 2006 and February 2007. During this period, Popocatépetl volcano showed a phase of increased activity, and COSPEC measurement campaigns were made. A few days the dates and times of acquisition of MODIS images coincide with the COSPEC measurements. In the case to make a comparison of both techniques some considerations must be made in such a way that seeks to reproduce the conditions that used a method and the other. In the case of COSPEC is to be understood that measurements are carried out in transects of the plume. On the other hand, we must consider the vehicle that transports the COSPEC, which in this case was terrain, Δt takes a while to cross the plume from side to side and you need to consider that the plume is moving at all times measuring the effect of the prevailing wind at the height where it is located. On the other hand, a satellite image provides instant volcanic plume. It also has information of the whole event in a given time. The resolution of each pixel is one square kilometer while for COSPEC the resolution is a few hundred meters. Results showed that the SO2 estimates data could be comparable in magnitude but should take into account gaps and drawbacks for both methods such as the time spent in making the measurement COSPEC and the route used to transect the plume. While for MODIS, it should be taken into account the image resolution that limits the ability to measure relatively small areas of SO2 concentration

  17. Neutral molecular cluster formation of sulfuric acid-dimethylamine observed in real time under atmospheric conditions.

    PubMed

    Kürten, Andreas; Jokinen, Tuija; Simon, Mario; Sipilä, Mikko; Sarnela, Nina; Junninen, Heikki; Adamov, Alexey; Almeida, João; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; Dommen, Josef; Donahue, Neil M; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Hutterli, Manuel; Kangasluoma, Juha; Kirkby, Jasper; Laaksonen, Ari; Lehtipalo, Katrianne; Leiminger, Markus; Makhmutov, Vladimir; Mathot, Serge; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud P; Riccobono, Francesco; Rissanen, Matti P; Rondo, Linda; Schobesberger, Siegfried; Seinfeld, John H; Steiner, Gerhard; Tomé, António; Tröstl, Jasmin; Winkler, Paul M; Williamson, Christina; Wimmer, Daniela; Ye, Penglin; Baltensperger, Urs; Carslaw, Kenneth S; Kulmala, Markku; Worsnop, Douglas R; Curtius, Joachim

    2014-10-21

    For atmospheric sulfuric acid (SA) concentrations the presence of dimethylamine (DMA) at mixing ratios of several parts per trillion by volume can explain observed boundary layer new particle formation rates. However, the concentration and molecular composition of the neutral (uncharged) clusters have not been reported so far due to the lack of suitable instrumentation. Here we report on experiments from the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research revealing the formation of neutral particles containing up to 14 SA and 16 DMA molecules, corresponding to a mobility diameter of about 2 nm, under atmospherically relevant conditions. These measurements bridge the gap between the molecular and particle perspectives of nucleation, revealing the fundamental processes involved in particle formation and growth. The neutral clusters are found to form at or close to the kinetic limit where particle formation is limited only by the collision rate of SA molecules. Even though the neutral particles are stable against evaporation from the SA dimer onward, the formation rates of particles at 1.7-nm size, which contain about 10 SA molecules, are up to 4 orders of magnitude smaller compared with those of the dimer due to coagulation and wall loss of particles before they reach 1.7 nm in diameter. This demonstrates that neither the atmospheric particle formation rate nor its dependence on SA can simply be interpreted in terms of cluster evaporation or the molecular composition of a critical nucleus.

  18. Neutral molecular cluster formation of sulfuric acid–dimethylamine observed in real time under atmospheric conditions

    PubMed Central

    Kürten, Andreas; Jokinen, Tuija; Simon, Mario; Sipilä, Mikko; Sarnela, Nina; Junninen, Heikki; Adamov, Alexey; Almeida, João; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; Dommen, Josef; Donahue, Neil M.; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Hutterli, Manuel; Kangasluoma, Juha; Kirkby, Jasper; Laaksonen, Ari; Lehtipalo, Katrianne; Leiminger, Markus; Makhmutov, Vladimir; Mathot, Serge; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud P.; Riccobono, Francesco; Rissanen, Matti P.; Rondo, Linda; Schobesberger, Siegfried; Seinfeld, John H.; Steiner, Gerhard; Tomé, António; Tröstl, Jasmin; Winkler, Paul M.; Williamson, Christina; Wimmer, Daniela; Ye, Penglin; Baltensperger, Urs; Carslaw, Kenneth S.; Kulmala, Markku; Worsnop, Douglas R.; Curtius, Joachim

    2014-01-01

    For atmospheric sulfuric acid (SA) concentrations the presence of dimethylamine (DMA) at mixing ratios of several parts per trillion by volume can explain observed boundary layer new particle formation rates. However, the concentration and molecular composition of the neutral (uncharged) clusters have not been reported so far due to the lack of suitable instrumentation. Here we report on experiments from the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research revealing the formation of neutral particles containing up to 14 SA and 16 DMA molecules, corresponding to a mobility diameter of about 2 nm, under atmospherically relevant conditions. These measurements bridge the gap between the molecular and particle perspectives of nucleation, revealing the fundamental processes involved in particle formation and growth. The neutral clusters are found to form at or close to the kinetic limit where particle formation is limited only by the collision rate of SA molecules. Even though the neutral particles are stable against evaporation from the SA dimer onward, the formation rates of particles at 1.7-nm size, which contain about 10 SA molecules, are up to 4 orders of magnitude smaller compared with those of the dimer due to coagulation and wall loss of particles before they reach 1.7 nm in diameter. This demonstrates that neither the atmospheric particle formation rate nor its dependence on SA can simply be interpreted in terms of cluster evaporation or the molecular composition of a critical nucleus. PMID:25288761

  19. Emissions of industrial furnaces burning diesel fuel oils of various sulfur contents with NaCl - contained atmospheric air

    SciTech Connect

    Lin, C.Y.; Hsieh, M.J.

    1996-04-01

    A small furnace associated with an industrial automatic burner was employed in this study to investigate the influences of sulfur content of fuel oils burned with NaCl contained atmospheric air on the emission characteristics of marine or industrial power-plants. The sulfur contents of 0.3 wt% and 1.0 wt% were considered. Diesel fuel oil A which approximates ASTM No. 2 fuel oil was atomized by the inlet air added with NaCl of 1.5 ppm concentration and thereafter burned within the furnace. It was found that under this burning condition the CO, SO{sub 2}, and O{sub 2} emissions increased with the addition of sulfur in the fuel oil. However, the gas temperature and NO{sub x} concentration were affected by the increase of sulfur content to only a minor extent. 14 refs., 10 figs.

  20. Production of furfural from xylose at atmospheric pressure by dilute sulfuric acid and inorganic salts.

    PubMed

    Rong, Chunguang; Ding, Xuefeng; Zhu, Yanchao; Li, Ying; Wang, Lili; Qu, Yuning; Ma, Xiaoyu; Wang, Zichen

    2012-03-01

    In this paper, the dehydration of xylose to furfural was carried out under atmospheric pressure and at the boiling temperature of a biphasic mixture of toluene and an aqueous solution of xylose, with sulfuric acid as catalyst plus an inorganic salt (NaCl or FeCl(3)) as promoter. The best yield of furfural was 83% under the following conditions: 150 mL of toluene and 10 mL of aqueous solution of 10% xylose (w/w), 10% H(2)SO(4) (w/w), 2.4g NaCl , and heating for 5h. FeCl(3) as promoter was found to be more efficient than NaCl. The addition of DMSO to the aqueous phase in the absence of an inorganic salt was shown to improve the yield of furfural.

  1. Titanium leaching from red mud by diluted sulfuric acid at atmospheric pressure.

    PubMed

    Agatzini-Leonardou, S; Oustadakis, P; Tsakiridis, P E; Markopoulos, Ch

    2008-09-15

    Laboratory-scale research has focused on the recovery of titanium from red mud, which is obtained from bauxite during the Bayer process for alumina production. The leaching process is based on the extraction of this element with diluted sulfuric acid from red mud under atmospheric conditions and without using any preliminary treatment. Statistical design and analysis of experiments were used, in order to determine the main effects and interactions of the leaching process factors, which were: acid normality, temperature and solid to liquid ratio. The titanium recovery efficiency on the basis of red mud weight reached 64.5%. The characterization of the initial red mud, as well as this of the leached residues was carried out by X-ray diffraction, TG-DTA and scanning electron microscopy.

  2. Theoretical and global scale model studies of the atmospheric sulfur/aerosol system

    NASA Technical Reports Server (NTRS)

    Kasibhatla, Prasad

    1996-01-01

    The primary focus during the third-phase of our on-going multi-year research effort has been on 3 activities. These are: (1) a global-scale model study of the anthropogenic component of the tropospheric sulfur cycle; (2) process-scale model studies of the factors influencing the distribution of aerosols in the remote marine atmosphere; and (3) an investigation of the mechanism of the OH-initiated oxidation of DMS in the remote marine boundary layer. In this paper, we describe in more detail our research activities in each of these areas. A major portion of our activities during the fourth and final phase of this project will involve the preparation and submission of manuscripts describing the results from our model studies of marine boundary-layer aerosols and DMS-oxidation mechanisms.

  3. Estimating lake-atmosphere CO2 exchange

    USGS Publications Warehouse

    Anderson, D.E.; Striegl, R.G.; Stannard, D.I.; Michmerhuizen, C.M.; McConnaughey, T.A.; LaBaugh, J.W.

    1999-01-01

    Lake-atmosphere CO2 flux was directly measured above a small, woodland lake using the eddy covariance technique and compared with fluxes deduced from changes in measured lake-water CO2 storage and with flux predictions from boundary-layer and surface-renewal models. Over a 3-yr period, lake-atmosphere exchanges of CO2 were measured over 5 weeks in spring, summer, and fall. Observed springtime CO2 efflux was large (2.3-2.7 ??mol m-2 s-1) immediately after lake-thaw. That efflux decreased exponentially with time to less than 0.2 ??mol m-2 s-1 within 2 weeks. Substantial interannual variability was found in the magnitudes of springtime efflux, surface water CO2 concentrations, lake CO2 storage, and meteorological conditions. Summertime measurements show a weak diurnal trend with a small average downward flux (-0.17 ??mol m-2 s-1) to the lake's surface, while late fall flux was trendless and smaller (-0.0021 ??mol m-2 s-1). Large springtime efflux afforded an opportunity to make direct measurement of lake-atmosphere fluxes well above the detection limits of eddy covariance instruments, facilitating the testing of different gas flux methodologies and air-water gas-transfer models. Although there was an overall agreement in fluxes determined by eddy covariance and those calculated from lake-water storage change in CO2, agreement was inconsistent between eddy covariance flux measurements and fluxes predicted by boundary-layer and surface-renewal models. Comparison of measured and modeled transfer velocities for CO2, along with measured and modeled cumulative CO2 flux, indicates that in most instances the surface-renewal model underpredicts actual flux. Greater underestimates were found with comparisons involving homogeneous boundary-layer models. No physical mechanism responsible for the inconsistencies was identified by analyzing coincidentally measured environmental variables.

  4. A three-dimensional modelling study of the seasonal cycle of sulfur species in the Antarctic atmosphere

    NASA Astrophysics Data System (ADS)

    Cosme, E.; Boucher, O.; Genthon, C.; Hourdin, F.; Krinner, G.; Legrand, M.; Martinerie, P.; Pham, M.

    2002-12-01

    The high-southern latitudes are one of the last regions of the globe where the sulfur cycle remains dominated by its natural component. Moreover, a good understanding of the processes involved in dimethylsulfide (DMS) oxidation is needed to interpret polar ice core records of sulfate and methanesulfonic acid (MSA). Both reasons motivated this modelling study of the sulfur cycle in Antarctica. For this purpose, the Antarctic version (with high resolution and improved physics in the high-southern latitudes) and the sulfur version of the Laboratoire de Météorologie Dynamique Atmospheric General Circulation Model (AGCM), LMD-ZT, have been merged and used to study the seasonal cycle of sulfur species. In a first step, the model results are compared with available measurements of sulfur compounds at high- and mid- southern latitudes. They are realistic but some defects are identified (Cosme et al., Sulfur cycle in the high southern latitudes in the LMD-ZT General Circulation Model, JGR, in press). In a second step, the seasonal cycle of sulfur compounds at an inland site (Dome Concordia) is presented and compared to the analogous results at the coastal site Dumont d'Urville. This comparison suggests that the relative roles of each process of the sulfur cycle (emissions, chemistry, transport) strongly differ from the coastal site to the inland site. At last, an adjoint of the model has been run to provide an inverse history of DMS, sulfate and MSA observed at two Antarctic sites: Dumont d'Urville (coastal Antarctica) and Vostok (inland Antarctica). For both sites, the origins of the sulfur species (type of sources, age, and latitudinal origin) are presented and discussed.

  5. STREAMWATER ACID-BASED CHEMISTRY AND CRITICAL LOADS OF ATMOSPHERIC SULFUR DEPOSITION IN SHENANDOAH NATIONAL PARK, VIRGINIA

    EPA Science Inventory

    A modeling study was conducted to evaluate the acid-base chemistry of streams within Shenandoah National Park, Virginia and to project future responses to sulfur (S) and nitrogen (N) atmospheric emissions controls. Many of the major stream systems in the Park have acid neutraliz...

  6. A comparison of sulfur-free and ambient air enclosure techniques for measuring the exchange of reduced sulfur gases between soils and the atmosphere

    NASA Astrophysics Data System (ADS)

    Castro, Mark S.; Galloway, James N.

    1991-08-01

    The exchange of reduced sulfur gases between the atmosphere and forest soils in the Shaver Hollow watershed (Shenandoah National Park, Virginia) were measured with sulfur-free and ambient air enclosures at least twice a month from March through November 1989. Soils within sulfur-free enslosures were sources of carbonyl sulfide (COS) and carbon disulfide (CS2). Atmospheric fluxes of COS and CS2 ranged from 0.77 to 13.03 ng COS-S/sq m-min and from 2.04 to 15.74 ng CS2-S/sq m-min. In contrast, soils within ambient air enclosures were sinks for COS and CS2. Uptake rates of COS and CS2 ranged from 2.78 to 16.20 ng COS-S/sq m-min and from 3.42 to 26.62 ng CS2-S/sq m-min. The discrepancy in the direction of these fluxes was caused by the flux-measurement techniques.

  7. Identification of sources and formation processes of atmospheric sulfate by sulfur isotope and scanning electron microscope measurements

    NASA Astrophysics Data System (ADS)

    Guo, Zhaobing; Li, Zhanqing; Farquhar, James; Kaufman, Alan J.; Wu, Nanping; Li, Can; Dickerson, Russell R.; Wang, Pucai

    2010-04-01

    Atmospheric sulfate aerosols have a cooling effect on the Earth's surface and can change cloud microphysics and precipitation. China has heavy loading of sulfate, but their sources and formation processes remain uncertain. In this study we characterize possible sources and formation processes of atmospheric sulfate by analyzing sulfur isotope abundances (32S, 33S, 34S, and 36S) and by detailed X-ray diffraction and scanning electron microscope (SEM) imaging of aerosol samples acquired at a rural site in northern China from March to August 2005. The comparison of SEM images from coal fly ash and the atmospheric aerosols suggests that direct emission from coal combustion is a substantial source of primary atmospheric sulfate in the form of CaSO4. Airborne gypsum (CaSO4·2H2O) is usually attributed to eolian dust or atmospheric reactions with H2SO4. SEM imaging also reveals mineral particles with soot aggregates adhered to the surface where they could decrease the single scattering albedo of these aerosols. In summer months, heterogeneous oxidation of SO2, derived from coal combustion, appears to be the dominant source of atmospheric sulfate. Our analyses of aerosol sulfate show a seasonal variation in Δ33S (Δ33S describes either a 33S excess or depletion relative to that predicted from consideration of classical mass-dependent isotope effects). Similar sulfur isotope variations have been observed in other atmospheric samples and in (homogenous) gas-phase reactions. On the basis of atmospheric sounding and satellite data as well as a possible relationship between Δ33S and Convective Available Potential Energy (CAPE) during the sampling period, we attribute the sulfur isotope anomalies (Δ33S and Δ36S) in Xianghe aerosol sulfates to another atmospheric source (upper troposphere or lower stratosphere).

  8. Using high time resolution aerosol and number size distribution measurements to estimate atmospheric extinction.

    PubMed

    Malm, William C; McMeeking, Gavin R; Kreidenweis, Sonia M; Levin, Ezra; Carrico, Christian M; Day, Derek E; Collett, Jeffrey L; Lee, Taehyoung; Sullivan, Amy P; Raja, Suresh

    2009-09-01

    Rocky Mountain National Park is experiencing reduced visibility and changes in ecosystem function due to increasing levels of oxidized and reduced nitrogen. The Rocky Mountain Atmospheric Nitrogen and Sulfur (RoMANS) study was initiated to better understand the origins of sulfur and nitrogen species as well as the complex chemistry occurring during transport from source to receptor. As part of the study, a monitoring program was initiated for two 1-month time periods--one during the spring and the other during late summer/fall. The monitoring program included intensive high time resolution concentration measurements of aerosol number size distribution, inorganic anions, and cations, and 24-hr time resolution of PM2.5 and PM10 mass, sulfate, nitrate, carbon, and soil-related elements concentrations. These data are combined to estimate high time resolution concentrations of PM2.5 and PM10 aerosol mass and fine mass species estimates of ammoniated sulfate, nitrate, and organic and elemental carbon. Hour-by-hour extinction budgets are calculated by using these species concentration estimates and measurements of size distribution and assuming internal and external particle mixtures. Summer extinction was on average about 3 times higher than spring extinction. During spring months, sulfates, nitrates, carbon mass, and PM10 - PM2.5 mass contributed approximately equal amounts of extinction, whereas during the summer months, carbonaceous material extinction was 2-3 times higher than other species.

  9. Atmospheric water on Mars, energy estimates for extraction

    NASA Technical Reports Server (NTRS)

    Meyer, Tom

    1991-01-01

    The Mars atmosphere is considered as a resource for water to support a human expedition. Information obtained from the Viking mission is used to estimate the near-surface water vapor level. The variability over the diurnal cycle is examined and periods of greatest water abundance are identified. Various methods for extracting atmospheric water are discussed including energy costs and the means for optimizing water extraction techniques.

  10. Early Mars volcanic sulfur storage in the upper cryosphere and formation of transient SO2-rich atmospheres during the Hesperian

    NASA Astrophysics Data System (ADS)

    Schmidt, F.; Chassefière, E.; Tian, F.; Dartois, E.; Herri, J.-M.; Mousis, O.

    2016-11-01

    In a previous paper (Chassefière et al.), we have shown that most volcanic sulfur released to the early Mars atmosphere could have been trapped in the upper cryosphere under the form of CO2-SO2 clathrates. Huge amounts of sulfur, up to the equivalent of an 1 bar atmosphere of SO2, would have been stored in the Noachian upper cryosphere, then massively released to the atmosphere during the Hesperian due to rapidly decreasing CO2 pressure. It could have resulted in the formation of the large sulfate deposits observed mainly in Hesperian terrains, whereas no or little sulfates are found at the Noachian. In the present paper, we first clarify some aspects of our previous work. We discuss the possibility of a smaller cooling effect of sulfur particles, or even of a net warming effect. We point out the fact that CO2-SO2 clathrates formed through a progressive enrichment of a pre-existing reservoir of CO2 clathrates and discuss processes potentially involved in the slow formation of a SO2-rich upper cryosphere. We show that episodes of sudden destabilization at the Hesperian may generate 1000 ppmv of SO2 in the atmosphere and contribute to maintaining the surface temperature above the water freezing point.

  11. Spatial and seasonal variations of atmospheric sulfur concentrations and dry deposition at 16 rural and suburban sites in China

    NASA Astrophysics Data System (ADS)

    Luo, Xiaosheng; Pan, Yuepeng; Goulding, Keith; Zhang, Lin; Liu, Xuejun; Zhang, Fusuo

    2016-12-01

    The large emissions of sulfur dioxide (SO2) in China have raised worldwide concerns due to its contribution to acid rain and particulate pollution. Monitoring sulfur (S) concentrations and estimating its deposition are important for evaluating air quality and its effects on ecosystems and human health. To date atmospheric dry S deposition in China remains unclear due to the paucity of measurements, especially in rural regions where the ecosystems are sensitive to acid deposition. In this study, we monitored both SO2 and particulate SO42- (pSO42-) concentrations at 8 sites south and 8 sites north of the Huai River in rural and suburban parts of China between 2010 and 2012. The measured concentration of SO2 and pSO42- were combined with GEOS-Chem modeled dry deposition velocities to estimate dry S deposition inputs to the surfaces. SO2 and pSO42- concentrations were high from October/November to next March/April and they (esp. SO2) decreased sharply since March/April at the northern sites, reflecting elevated SO2 emissions by winter heating (which normally starts in October/November and ends in March/April in the north of the Huai River). However the southern sites did not show this trend. Annual dry deposition of SO2 plus pSO42- in this study ranged from 3.1 to 27.1 kg S ha-1 across all the sites in the year 2011 (except one site from May 2011 to April 2012) and showed large spatial variation. The sites in northern China had greater dry deposition due to the higher S concentrations compared with sites in southern China. We also found relatively low pSO42-/pNO3- ratios at most sites, reflecting NOx emissions had a larger influence than SO2 emissions on particle composition during the 2010-2012 period at the measurement sites. Our results suggest that dry S deposition is still important input to ecosystems in spite of slow reduction of Chinese national SO2 emissions since 2005. More research on both wet and dry S deposition and their impacts on the environment and

  12. Bimodal Distribution of Sulfuric Acid Aerosols in the Atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Gao, Peter; Zhang, X.; Crisp, D.; Bardeen, C. G.; Yung, Y. L.

    2013-10-01

    Observations by the SPICAV/SOIR instruments aboard Venus Express have revealed that the upper haze of Venus, between 70 and 90 km, is variable on the order of days and that it is populated by two particle modes. In this work, we posit that the observed phenomena are caused by the transient mixing of the clouds and the haze, as well as another source of sulfuric acid aerosols in the upper haze that nucleate on meteoric dust. We test this hypothesis by simulating a column of the Venus atmosphere from 40 to 100 km above the surface using a model based upon the Community Aerosol and Radiation Model for Atmospheres and consider the effects of meteoric dust and polysulfur acting as condensation nuclei in the upper haze and upper cloud, respectively, as well as transient winds at the cloud tops caused by subsolar convection. Our aerosol number density results are consistent with Pioneer Venus data from Knollenberg and Hunten (1980), while our gas distribution results match the Magellan radio occultation data as analyzed by Kolodner and Steffes (1998) below 55 km. The size distribution of cloud particles shows two distinct modes in the upper clouds region and three distinct modes in the middle and lower clouds regions, qualitatively matching the observations of Pioneer Venus. The UH size distribution shows one distinct mode that is likely an upwelled cloud particle population with which an in situ meteoric dust condensation particle population has coagulated. The results of the transient wind simulations yield a variability timescale that is consistent with Venus Express observations, as well as a clear bimodal size distribution in the UH.

  13. Atmospheric measurements of carbonyl sulfide, dimethyl sulfide, and carbon disulfide using the electron capture sulfur detector

    NASA Technical Reports Server (NTRS)

    Johnson, James E.; Bates, Timothy S.

    1993-01-01

    Measurements of atmospheric dimethyl sulfide (DMS), carbonyl sulfide (COS), and carbon disulfide (CS2) were conducted over the Atlantic Ocean on board the NASA Electra aircraft during the Chemical Instrumentation Test and Evaluation (CITE 3) project using the electron capture sulfur detector (ECD-S). The system employed cryogenic preconcentration of air samples, gas chromatographic separation, catalytic fluorination, and electron capture detection. Samples collected for DMS analysis were scrubbed of oxidants with NaOH impregnated glass fiber filters to preconcentration. The detection limits (DL) of the system for COS, DMS, and CS2 were 5, 5, and 2 ppt, respectively. COS concentrations ranged from 404 to 603 ppt with a mean of 489 ppt for measurements over the North Atlantic Ocean (31 deg N to 41 deg N), and from 395 to 437 ppt with a mean of 419 ppt for measurements over the Tropical Atlantic Ocean (11 deg S to 2 deg N). DMS concentrations in the lower marine boundary layer, below 600-m altitude, ranged from below DL to 150 ppt from flights over the North Atlantic, and from 9 to 104 ppt over the Tropical Atlantic. CS2 concentrations ranged from below DL to 29 ppt over the North Atlantic. Almost all CS2 measurements over the Tropical Atlantic were below DL.

  14. The impact of particle size, relative humidity, and sulfur dioxide on iron solubility in simulated atmospheric marine aerosols.

    PubMed

    Cartledge, Benton T; Marcotte, Aurelie R; Herckes, Pierre; Anbar, Ariel D; Majestic, Brian J

    2015-06-16

    Iron is a limiting nutrient in about half of the world's oceans, and its most significant source is atmospheric deposition. To understand the pathways of iron solubilization during atmospheric transport, we exposed size segregated simulated marine aerosols to 5 ppm sulfur dioxide at arid (23 ± 1% relative humidity, RH) and marine (98 ± 1% RH) conditions. Relative iron solubility increased as the particle size decreased for goethite and hematite, while for magnetite, the relative solubility was similar for all of the fine size fractions (2.5-0.25 μm) investigated but higher than the coarse size fraction (10-2.5 μm). Goethite and hematite showed increased solubility at arid RH, but no difference (p > 0.05) was observed between the two humidity levels for magnetite. There was no correlation between iron solubility and exposure to SO2 in any mineral for any size fraction. X-ray absorption near edge structure (XANES) measurements showed no change in iron speciation [Fe(II) and Fe(III)] in any minerals following SO2 exposure. SEM-EDS measurements of SO2-exposed goethite revealed small amounts of sulfur uptake on the samples; however, the incorporated sulfur did not affect iron solubility. Our results show that although sulfur is incorporated into particles via gas-phase processes, changes in iron solubility also depend on other species in the aerosol.

  15. Hydrogen Peroxide and Methylhydroperoxide Budgets in the Marine Boundary Layer During the Pacific Atmospheric Sulfur Experiment

    NASA Astrophysics Data System (ADS)

    O'Sullivan, D. W.; Heikes, B. G.; Higbie, A.; Merrill, J. T.; Bandy, A. R.; Mauldin, L.; Cantrell, C.; Anderson, R. S.; Campos, T.; Lenschow, D.; Bloomquist, B.; Faloona, I. C.; Conley, S. A.; Wang, Y.; Pollack, I. B.; Heizer, C. G.; Weinheimer, A. J.

    2008-12-01

    Airborne gas phase measurements of hydrogen peroxide, methylhydroperoxide, ozone, carbon monoxide, dimethylsulfide, sulfur dioxide, hydroxyl, and perhydroxyl, together with meteorological parameters are used to assess the photochemical budget of hydrogen peroxide and methylhydroperoxide in the marine boundary layer (MBL). The observations come from 14 research flights using the NCAR C-130 flown mostly southeast of Kiritimati in relatively cloud- and precipitation-free MBL air. This region was expected to have extremely low nitrogen oxide mixing ratios and minimal horizontal gradients in composition. Eddy-correlation methods are used to estimate entrainment rates at the top of the MBL. Surface deposition rates are calculated from wind and molecular properties. Gas phase photolysis rates are calculated and reaction rate constants are estimated from the literature. The measurements and budgets are discussed in terms of their ability to constrain net ozone production, nitrogen oxide levels, reactive hydrocarbons, and halogen radical chemistry. On occasion the aircraft flew within its advected exhaust plume and a decrease in methylhydroperoxide, but not in hydrogen peroxide, was noted.

  16. Estimate of mercury emissions to the atmosphere from petroleum.

    PubMed

    Wilhelm, S M

    2001-12-15

    An estimate of the contribution of mercury to the atmospheric environment from petroleum processed in the United States is constructed from recent data. The estimate is based on a mass balance approach for mercury in crude oil, in refined products, and in waste streams (air, water, solid waste) from refineries. Although there are insufficient data at present to have a high degree of confidence in the mean amount and range of mercury concentrations in crude oil or in refined products, the framework of the estimate should assist direction for the acquisition of additional data. On the basis of selected data that put the estimated mean concentration of total mercury in crude oil close to 10 ppb, it is calculated that the total amount of mercury in U.S. petroleum processed yearly is slightly over 8000 kg/yr. Of this amount, approximately 6000 kg/yr is estimated to be emitted to the atmosphere from combustion of liquid hydrocarbon fuels, which represents about 10% of the U.S. yearly emission rate of atmospheric mercury from coal combustion. The material balance predicts that the amount of mercury in air emissions from all U.S. refineries is on the order of 1500 kg/yr based on the assumption that fugitive mercury emissions from refineries are negligible. Atmospheric emissions of mercury from fuel oil burned in the United States are estimated in the U.S. EPA Mercury Report to Congress to be approximately 10000 kg/yr, and this estimate may be in error on the high side by a factor of 3-10. If the mean amounts of mercury in U.S. distillate and residual fuel oils are in the range of 5-15 ppb, as suggested by more recent data, then U.S. fuel oil combustion should contribute no more that about 1000-3000 kg/yr (emission ratio = 1) of mercury to the atmospheric burden.

  17. Atmospheric Chemistry in Giant Planets, Brown Dwarfs, and Low-Mass Dwarf Stars. II. Sulfur and Phosphorus

    NASA Astrophysics Data System (ADS)

    Visscher, Channon; Lodders, Katharina; Fegley, Bruce, Jr.

    2006-09-01

    Thermochemical equilibrium and kinetic calculations are used to model sulfur and phosphorus chemistry in giant planets, brown dwarfs, and extrasolar giant planets (EGPs). The chemical behavior of individual S- and P-bearing gases and condensates is determined as a function of pressure, temperature, and metallicity. The results are independent of particular model atmospheres, and in principle, the equilibrium composition along the pressure-temperature profile of any object can be determined. Hydrogen sulfide (H2S) is the dominant S-bearing gas throughout substellar atmospheres and approximately represents the atmospheric sulfur inventory. Silicon sulfide (SiS) is a potential tracer of weather in substellar atmospheres. Disequilibrium abundances of phosphine (PH3) approximately representative of the total atmospheric phosphorus inventory are expected to be mixed upward into the observable atmospheres of giant planets and T dwarfs. In hotter objects, several P-bearing gases (e.g., P2, PH3, PH 2, PH, and HCP) become increasingly important at high temperatures.

  18. Estimate of sulfur, arsenic, mercury, fluorine emissions due to spontaneous combustion of coal gangue: An important part of Chinese emission inventories.

    PubMed

    Wang, Shaobin; Luo, Kunli; Wang, Xing; Sun, Yuzhuang

    2016-02-01

    A rough estimate of the annual amount of sulfur, arsenic, mercury and fluoride emission from spontaneous combustion of coal gangue in China was determined. The weighted mean concentrations of S, As, Hg, and F in coal gangue are 1.01%, 7.98, 0.18, and 365.54 mg/kg, respectively. Amounts of S, As, Hg, and F emissions from coal gangue spontaneous combustion show approximately 1.13 Mt, and 246, 45, and 63,298 tons in 2013, respectively. The atmospheric release amount of sulfur from coal gangue is more than one tenth of this from coal combustion, and the amounts of As, Hg, and F are close to or even exceed those from coal combustion. China's coal gangue production growth from 1992 to 2013 show an obvious growth since 2002. It may indicate that Chinese coal gangue has become a potential source of air pollution, which should be included in emission inventories.

  19. Recombination reactions as a possible mechanism of mass-independent fractionation of sulfur isotopes in the Archean atmosphere of Earth.

    PubMed

    Babikov, Dmitri

    2017-03-21

    A hierarchy of isotopically substituted recombination reactions is formulated for production of sulfur allotropes in the anoxic atmosphere of Archean Earth. The corresponding system of kinetics equations is solved analytically to obtain concise expressions for isotopic enrichments, with focus on mass-independent isotope effects due to symmetry, ignoring smaller mass-dependent effects. Proper inclusion of atom-exchange processes is shown to be important. This model predicts significant and equal depletions driven by reaction stoichiometry for all rare isotopes: (33)S, (34)S, and (36)S. Interestingly, the ratio of capital [Formula: see text] values obtained within this model for (33)S and (36)S is -1.16, very close to the mass-independent fractionation line of the Archean rock record. This model may finally offer a mechanistic explanation for the striking mass-independent fractionation of sulfur isotopes that took place in the Archean atmosphere of Earth.

  20. Submillimeter spectroscopy of Venus's atmosphere with ALMA: CO, HDO and sulfur species

    NASA Astrophysics Data System (ADS)

    Moullet, Arielle; Moreno, R.; Encrenaz, T.; Lellouch, E.; Fouchet, T.

    2013-10-01

    The study of the composition of the upper mesosphere of Venus is necessary to characterize several atmospheric processes such as photochemistry, condensation and dynamics. At this altitude level (80-110 km), several species have been detected thanks to their (sub)millimeter rotational lines, in particular sulfur species SO2 and SO, that may be indicative of Venus' volcanic activity, and showed an abundance increase with altitude suggesting a local sulfur-bearing aerosol source[1,2]. H2O, which takes part in the formation of H2SO4 clouds, was also detected as well as its isotope HDO; their analyses revealed significant diurnal and long-term temporal variations [3,4]. To explore this case in greater detail and better assess local, diurnal and temporal variations of minor species, heterodyne spectroscopic observations were obtained in November 2011 during the first Early Science observation cycle of the Atacama Large Millimeter Array (ALMA), the largest (sub)millimeter interferometer, which at the time offered 16 12-m large antennas. These observations allowed us to map the day side of Venus with a spatial resolution down to 1.2-2.4"" (for a disk of 11"), targeting SO2, SO, HDO and CO transitions around 0.85mm (335-346 GHz). All of these transitions were well detected and their modeling yielded abundances consistent with previous single-dish assessments. We will present a detailed analysis of the data in terms of spatial distribution (horizontal and vertical) and temporal variations, and we will discuss their interpretation with regard to the efficiency of photochemical destruction in the mesosphere and aerosol sources. In addition, by mapping the CO(3-2) line's Doppler-shifts, we have been able to derive the wind field near the upper boundary of the mesosphere, whichs corresponds to a region of dynamic transition between the retrograde zonal wind regime of the troposphere and the subsolar-to-antisolar flow that dominates at higher altitudes. [1] Sandor et al., 2010

  1. Spectral estimation of global levels of atmospheric pollutants.

    PubMed

    Fernández-Macho, Javier

    2011-10-01

    Underlying levels of atmospheric pollutants, assumed to be governed by smoothing mechanisms due to atmospheric dispersion, can be estimated from global emissions source databases on greenhouse gases and ozone-depleting compounds. However, spatial data may be contaminated with noise or even missing or zero-valued at many locations. Therefore, a problem that arises is how to extract the underlying smooth levels. This paper sets out a structural spatial model that assumes data evolve across a global grid constrained by second-order smoothing restrictions. The frequency-domain approach is particularly suitable for global datasets, reduces the computational burden associated with two-dimensional models and avoids cumbersome zero-inflated skewed distributions. Confidence intervals of the underlying levels are also obtained. An application to the estimation of global levels of atmospheric pollutants from anthropogenic emissions illustrates the technique which may also be useful in the analysis of other environmental datasets of similar characteristics.

  2. Range estimation of passive infrared targets through the atmosphere

    NASA Astrophysics Data System (ADS)

    Cho, Hoonkyung; Chun, Joohwan; Seo, Doochun; Choi, Seokweon

    2013-04-01

    Target range estimation is traditionally based on radar and active sonar systems in modern combat systems. However, jamming signals tremendously degrade the performance of such active sensor devices. We introduce a simple target range estimation method and the fundamental limits of the proposed method based on the atmosphere propagation model. Since passive infrared (IR) sensors measure IR signals radiating from objects in different wavelengths, this method has robustness against electromagnetic jamming. The measured target radiance of each wavelength at the IR sensor depends on the emissive properties of target material and various attenuation factors (i.e., the distance between sensor and target and atmosphere environment parameters). MODTRAN is a tool that models atmospheric propagation of electromagnetic radiation. Based on the results from MODTRAN and atmosphere propagation-based modeling, the target range can be estimated. To analyze the proposed method's performance statistically, we use maximum likelihood estimation (MLE) and evaluate the Cramer-Rao lower bound (CRLB) via the probability density function of measured radiance. We also compare CRLB and the variance of MLE using Monte-Carlo simulation.

  3. Rayleigh light scattering properties of atmospheric molecular clusters consisting of sulfuric acid and bases.

    PubMed

    Elm, Jonas; Norman, Patrick; Mikkelsen, Kurt V

    2015-06-28

    The Rayleigh light scattering properties of (H2SO4)a(NH3)b and (H2SO4)a((CH3)2NH)b atmospheric molecular clusters have been investigated using a response theory approach. Using density functional theory the molecular structures and stepwise formation free energies of clusters with a and b up to 4 have been re-investigated. The Rayleigh scattering intensities are calculated from the dipole polarizability tensor α using the CAM-B3LYP functional by applying linear response methods. The intrinsic scattering properties of (H2SO4)a(NH3)b and (H2SO4)a((CH3)2NH)b indicate that amine containing clusters scatter light significantly more efficiently then their ammonia containing counterparts. Using the Atmospheric Cluster Dynamics Code (ACDC) the steady state cluster concentrations are estimated and the effective scattering is calculated. The effective scattering is shown to be highly dependent on the estimated concentrations and indicates that there exist competitive pathways, such as nucleation and coagulation, which influence the cluster distributions. The frequency dependence of the scattering is found to depend on the cluster composition and show increased responses when clusters contain more bases than acid molecules. Based on structures obtained using semi-empirical molecular dynamics simulations the Rayleigh scattering properties of clusters with up to 20 acid-base pairs are evaluated. This study represents the first step towards gaining a fundamental understanding of the scattering properties of small atmospheric clusters in the ambient atmosphere.

  4. Planetary Probe Entry Atmosphere Estimation Using Synthetic Air Data System

    NASA Technical Reports Server (NTRS)

    Karlgaard, Chris; Schoenenberger, Mark

    2017-01-01

    This paper develops an atmospheric state estimator based on inertial acceleration and angular rate measurements combined with an assumed vehicle aerodynamic model. The approach utilizes the full navigation state of the vehicle (position, velocity, and attitude) to recast the vehicle aerodynamic model to be a function solely of the atmospheric state (density, pressure, and winds). Force and moment measurements are based on vehicle sensed accelerations and angular rates. These measurements are combined with an aerodynamic model and a Kalman-Schmidt filter to estimate the atmospheric conditions. The new method is applied to data from the Mars Science Laboratory mission, which landed the Curiosity rover on the surface of Mars in August 2012. The results of the new estimation algorithm are compared with results from a Flush Air Data Sensing algorithm based on onboard pressure measurements on the vehicle forebody. The comparison indicates that the new proposed estimation method provides estimates consistent with the air data measurements, without the use of pressure measurements. Implications for future missions such as the Mars 2020 entry capsule are described.

  5. Riverine Response of Sulfate to Declining Atmospheric Sulfur Deposition in Agricultural Watersheds.

    PubMed

    David, Mark B; Gentry, Lowell E; Mitchell, Corey A

    2016-07-01

    Sulfur received extensive study as an input to terrestrial ecosystems from acidic deposition during the 1980s. With declining S deposition inputs across the eastern United States, there have been many studies evaluating ecosystem response, with the exception of agricultural watersheds. We used long-term (22 and 18 yr) sulfate concentration data from two rivers and recent (6 yr) data from a third river to better understand cycling and transport of S in agricultural, tile-drained watersheds. Sulfate concentrations and yields steadily declined in the Embarras (from ∼10 to 6 mg S L) and Kaskaskia rivers (from 7 to 3.5 mg S L) during the sampling period, with an overall -23.1 and -12.8 kg S ha yr balance for the two watersheds. There was evidence of deep groundwater inputs of sulfate in the Salt Fork watershed, with a much smaller input to the Embarras and none to the Kaskaskia. Tiles in the watersheds had low sulfate concentrations (<10 mg S L), similar to the Kaskaskia River, unless the field had received some form of S fertilizer. A multiple regression model of runoff (cm) and S deposition explained much of the variation in Embarras River sulfate ( = 0.86 and 0.80 for concentrations and yields; = 46). Although atmospheric deposition was much less than outputs (grain harvest + stream export of sulfate), riverine transport of sulfate reflected the decline in inputs. Watershed S balances suggest a small annual depletion of soil organic S pools, and S fertilization will likely be needed at some future date to maintain crop yields.

  6. Atmospheric wet deposition of sulfur and nitrogen in Jiuzhaigou National Nature Reserve, Sichuan Province, China.

    PubMed

    Qiao, Xue; Xiao, Weiyang; Jaffe, Daniel; Kota, Sri Harsha; Ying, Qi; Tang, Ya

    2015-04-01

    In the last two decades, remarkable ecological changes have been observed in Jiuzhaigou National Nature Reserve (JNNR). Some of these changes might be related to excessive deposition of sulfur (S) and nitrogen (N), but the relationship has not been quantified due to lack of monitoring data, particularly S and N deposition data. In this study, we investigated the concentrations, fluxes, and sources of S and N wet deposition in JNNR from April 2010 to May 2011. The results show that SO4(2-), NO3-, and NH4+ concentrations in the wet deposition were 39.4-170.5, 6.2-34.8, and 0.2-61.2 μeq L(-1), with annual Volume-Weighted Mean (VWM) concentrations of 70.5, 12.7, and 13.4 μeq L(-1), respectively. Annual wet deposition fluxes of SO4(2-), NO3-, and NH4+ were 8.06, 1.29, and 1.39 kg S(N)ha(-1), respectively, accounting for about 90% of annual atmospheric inputs of these species at the monitoring site. The results of Positive Matrix Factorization (PMF) analysis show that fossil fuel combustion, agriculture, and aged sea salt contributed to 99% and 83% of annual wet deposition fluxes of SO4(2-) and NO3-, respectively. Agriculture alone contributed to 89% of annual wet deposition flux of NH4+. Although wet deposition in JNNR was polluted by anthropogenic acids, the acidity was largely neutralized by the Ca2+ from crust and 81% of wet deposition samples had a pH higher than 6.00. However, acid rain mainly caused by SO4(2-) continued to occur in the wet season, when ambient alkaline dust concentration was lower. Since anthropogenic emissions have elevated S and N deposition and caused acid rain in JNNR, further studies are needed to better quantify the regional sources and ecological effects of S and N deposition for JNNR.

  7. Estimation of atmospheric parameters from time-lapse imagery

    NASA Astrophysics Data System (ADS)

    McCrae, Jack E.; Basu, Santasri; Fiorino, Steven T.

    2016-05-01

    A time-lapse imaging experiment was conducted to estimate various atmospheric parameters for the imaging path. Atmospheric turbulence caused frame-to-frame shifts of the entire image as well as parts of the image. The statistics of these shifts encode information about the turbulence strength (as characterized by Cn2, the refractive index structure function constant) along the optical path. The shift variance observed is simply proportional to the variance of the tilt of the optical field averaged over the area being tracked. By presuming this turbulence follows the Kolmogorov spectrum, weighting functions can be derived which relate the turbulence strength along the path to the shifts measured. These weighting functions peak at the camera and fall to zero at the object. The larger the area observed, the more quickly the weighting function decays. One parameter we would like to estimate is r0 (the Fried parameter, or atmospheric coherence diameter.) The weighting functions derived for pixel sized or larger parts of the image all fall faster than the weighting function appropriate for estimating the spherical wave r0. If we presume Cn2 is constant along the path, then an estimate for r0 can be obtained for each area tracked, but since the weighting function for r0 differs substantially from that for every realizable tracked area, it can be expected this approach would yield a poor estimator. Instead, the weighting functions for a number of different patch sizes can be combined through the Moore-Penrose pseudo-inverse to create a new weighting function which yields the least-squares optimal linear combination of measurements for estimation of r0. This approach is carried out, and it is observed that this approach is somewhat noisy because the pseudo-inverse assigns weights much greater than one to many of the observations.

  8. Estimation of Residual Peritoneal Volume Using Technetium-99m Sulfur Colloid Scintigraphy.

    PubMed

    Katopodis, Konstantinos P; Fotopoulos, Andrew D; Balafa, Olga C; Tsiouris, Spyridon Th; Triandou, Eleni G; Al-Bokharhli, Jichad B; Kitsos, Athanasios C; Dounousi, Evagelia C; Siamopoulos, Konstantinos C

    2015-01-01

    Residual peritoneal volume (RPV) may contribute in the development of ultrafiltration failure in patients with normal transcapillary ultrafiltration. The aim of this study was to estimate the RPV using intraperitoneal technetium-99m Sulfur Colloid (Tc). Twenty patients on peritoneal dialysis were studied. RPV was estimated by: 1) intraperitoneal instillation of Tc (RPV-Tc) and 2) classic Twardowski calculations using endogenous solutes, such as urea (RPV-u), creatinine (RPV-cr), and albumin (RPV-alb). Each method's reproducibility was assessed in a subgroup of patients in two consecutive measurements 48 h apart. Both methods displayed reproducibility (r = 0.93, p = 0.001 for RPVTc and r = 0.90, p = 0.001 for RPV-alb) between days 1 and 2, respectively. We found a statistically significant difference between RPV-Tc and RPV-cr measurements (347.3 ± 116.7 vs. 450.0 ± 67.8 ml; p =0.001) and RPV-u (515.5 ± 49.4 ml; p < 0.001), but not with RPV-alb (400.1 ± 88.2 ml; p = 0.308). A good correlation was observed only between RPV-Tc and RPV-alb (p < 0.001). The Tc method can estimate the RPV as efficiently as the high molecular weight endogenous solute measurement method. It can also provide an imaging estimate of the intraperitoneal distribution of RPV.

  9. [Automatic Measurement of the Stellar Atmospheric Parameters Based Mass Estimation].

    PubMed

    Tu, Liang-ping; Wei, Hui-ming; Luo, A-li; Zhao, Yong-heng

    2015-11-01

    We have collected massive stellar spectral data in recent years, which leads to the research on the automatic measurement of stellar atmospheric physical parameters (effective temperature Teff, surface gravity log g and metallic abundance [Fe/ H]) become an important issue. To study the automatic measurement of these three parameters has important significance for some scientific problems, such as the evolution of the universe and so on. But the research of this problem is not very widely, some of the current methods are not able to estimate the values of the stellar atmospheric physical parameters completely and accurately. So in this paper, an automatic method to predict stellar atmospheric parameters based on mass estimation was presented, which can achieve the prediction of stellar effective temperature Teff, surface gravity log g and metallic abundance [Fe/H]. This method has small amount of computation and fast training speed. The main idea of this method is that firstly it need us to build some mass distributions, secondly the original spectral data was mapped into the mass space and then to predict the stellar parameter with the support vector regression (SVR) in the mass space. we choose the stellar spectral data from the United States SDSS-DR8 for the training and testing. We also compared the predicted results of this method with the SSPP and achieve higher accuracy. The predicted results are more stable and the experimental results show that the method is feasible and can predict the stellar atmospheric physical parameters effectively.

  10. Atmospheric record in the Hadean Eon from multiple sulfur isotope measurements in Nuvvuagittuq Greenstone Belt (Nunavik, Quebec)

    PubMed Central

    Thomassot, Emilie; O’Neil, Jonathan; Francis, Don; Cartigny, Pierre; Wing, Boswell A.

    2015-01-01

    Mass-independent fractionation of sulfur isotopes (S-MIF) results from photochemical reactions involving short-wavelength UV light. The presence of these anomalies in Archean sediments [(4–2.5 billion years ago, (Ga)] implies that the early atmosphere was free of the appropriate UV absorbers, of which ozone is the most important in the modern atmosphere. Consequently, S-MIF is considered some of the strongest evidence for the lack of free atmospheric oxygen before 2.4 Ga. Although temporal variations in the S-MIF record are thought to depend on changes in the abundances of gas and aerosol species, our limited understanding of photochemical mechanisms complicates interpretation of the S-MIF record in terms of atmospheric composition. Multiple sulfur isotope compositions (δ33S, δ34S, and δ36S) of the >3.8 billion-year-old Nuvvuagittuq Greenstone Belt (Ungava peninsula) have been investigated to track the early origins of S-MIF. Anomalous S-isotope compositions (Δ33S up to +2.2‰) confirm a sedimentary origin of sulfide-bearing banded iron and silica-rich formations. Sharp isotopic transitions across sedimentary/igneous lithological boundaries indicate that primary surficial S-isotope compositions have been preserved despite a complicated metamorphic history. Furthermore, Nuvvuagittuq metasediments recorded coupled variations in 33S/32S, 34S/32S, and 36S/32S that are statistically indistinguishable from those identified several times later in the Archean. The recurrence of the same S-isotope pattern at both ends of the Archean Eon is unexpected, given the complex atmospheric, geological, and biological pathways involved in producing and preserving this fractionation. It implies that, within 0.8 billion years of Earth’s formation, a common mechanism for S-MIF production was established in the atmosphere. PMID:25561552

  11. Atmospheric record in the Hadean Eon from multiple sulfur isotope measurements in Nuvvuagittuq Greenstone Belt (Nunavik, Quebec).

    PubMed

    Thomassot, Emilie; O'Neil, Jonathan; Francis, Don; Cartigny, Pierre; Wing, Boswell A

    2015-01-20

    Mass-independent fractionation of sulfur isotopes (S-MIF) results from photochemical reactions involving short-wavelength UV light. The presence of these anomalies in Archean sediments [(4-2.5 billion years ago, (Ga)] implies that the early atmosphere was free of the appropriate UV absorbers, of which ozone is the most important in the modern atmosphere. Consequently, S-MIF is considered some of the strongest evidence for the lack of free atmospheric oxygen before 2.4 Ga. Although temporal variations in the S-MIF record are thought to depend on changes in the abundances of gas and aerosol species, our limited understanding of photochemical mechanisms complicates interpretation of the S-MIF record in terms of atmospheric composition. Multiple sulfur isotope compositions (δ(33)S, δ(34)S, and δ(36)S) of the >3.8 billion-year-old Nuvvuagittuq Greenstone Belt (Ungava peninsula) have been investigated to track the early origins of S-MIF. Anomalous S-isotope compositions (Δ(33)S up to +2.2‰) confirm a sedimentary origin of sulfide-bearing banded iron and silica-rich formations. Sharp isotopic transitions across sedimentary/igneous lithological boundaries indicate that primary surficial S-isotope compositions have been preserved despite a complicated metamorphic history. Furthermore, Nuvvuagittuq metasediments recorded coupled variations in (33)S/(32)S, (34)S/(32)S, and (36)S/(32)S that are statistically indistinguishable from those identified several times later in the Archean. The recurrence of the same S-isotope pattern at both ends of the Archean Eon is unexpected, given the complex atmospheric, geological, and biological pathways involved in producing and preserving this fractionation. It implies that, within 0.8 billion years of Earth's formation, a common mechanism for S-MIF production was established in the atmosphere.

  12. Mechanism of the atmospheric oxidation of sulfur dioxide - Catalysis by hydroxyl radicals

    NASA Technical Reports Server (NTRS)

    Margitan, J. J.

    1984-01-01

    A flash photolysis/resonance fluorescence technique was used to investigate the decay of OH due to the reaction OH + SO2 (+M) to HOSO2 (+M). In the presence of small amounts of NO (10 to the 14th per cu cm), the decays deviated from the normal semilogarithmic linearity due to reformation of OH. On the basis of computer simulations of the decay curves, it is suggested that the reactions HOSO2 + O2 to HO2 + SO3 (k3), and HO2 + HO to OH + NO2 are the likely subsequent steps in SO2 oxidation. The upper limit for the binding energy of HOSO2 relative to OH + SO2 is estimated to be 32 kcal/mol. The atmospheric implications of a catalytic oxidation mechanism are briefly discussed.

  13. Atmospheric Inverse Estimates of Methane Emissions from Central California

    SciTech Connect

    Zhao, Chuanfeng; Andrews, Arlyn E.; Bianco, Laura; Eluszkiewicz, Janusz; Hirsch, Adam; MacDonald, Clinton; Nehrkorn, Thomas; Fischer, Marc L.

    2008-11-21

    Methane mixing ratios measured at a tall-tower are compared to model predictions to estimate surface emissions of CH{sub 4} in Central California for October-December 2007 using an inverse technique. Predicted CH{sub 4} mixing ratios are calculated based on spatially resolved a priori CH{sub 4} emissions and simulated atmospheric trajectories. The atmospheric trajectories, along with surface footprints, are computed using the Weather Research and Forecast (WRF) coupled to the Stochastic Time-Inverted Lagrangian Transport (STILT) model. An uncertainty analysis is performed to provide quantitative uncertainties in estimated CH{sub 4} emissions. Three inverse model estimates of CH{sub 4} emissions are reported. First, linear regressions of modeled and measured CH{sub 4} mixing ratios obtain slopes of 0.73 {+-} 0.11 and 1.09 {+-} 0.14 using California specific and Edgar 3.2 emission maps respectively, suggesting that actual CH{sub 4} emissions were about 37 {+-} 21% higher than California specific inventory estimates. Second, a Bayesian 'source' analysis suggests that livestock emissions are 63 {+-} 22% higher than the a priori estimates. Third, a Bayesian 'region' analysis is carried out for CH{sub 4} emissions from 13 sub-regions, which shows that inventory CH{sub 4} emissions from the Central Valley are underestimated and uncertainties in CH{sub 4} emissions are reduced for sub-regions near the tower site, yielding best estimates of flux from those regions consistent with 'source' analysis results. The uncertainty reductions for regions near the tower indicate that a regional network of measurements will be necessary to provide accurate estimates of surface CH{sub 4} emissions for multiple regions.

  14. Sulfur isotope fractionation by broadband UV radiation to optically thin SO2 under reducing atmosphere

    NASA Astrophysics Data System (ADS)

    Endo, Yoshiaki; Ueno, Yuichiro; Aoyama, Shinnosuke; Danielache, Sebastian O.

    2016-11-01

    Photochemical mechanisms of Sulfur Mass-Independent Fractionation (S-MIF) are still poorly understood. Previous laboratory experiments have indicated that the S-MIF depends largely on the spectrum of the incident light source and the partial pressure of SO2, though the basic character of the Archean S-MIF (Δ36S / Δ33S = ∼ - 1) has never been reproduced. We have conducted new photochemical experiments at low pSO2 (1-10 Pa) conditions under the presence of CO and found a reasonable mechanism to reproduce the Δ36S/Δ33S slope about -1. As previously suggested (Ono et al., 2013), the low pSO2 is key to studying the self-shielding effect within a range of realistic atmospheric conditions. Also, reducing conditions are critical for simulating the O2-poor atmosphere, whereas photolysis of pure SO2 provides excess O atoms that significantly change the overall chemistry. Our experimental results confirmed that significant S-MIF (Δ36S / Δ33S = - 2.4) can be produced by self-shielding in the SO2 photolysis band (185-220 nm), even if the SO2 column density is as low as 1016 molecules cm-2. Thus, photolysis within a volcanic plume of ∼0.1 ppm SO2 is capable of producing a large S-MIF signature. The isotopic fractionations originating from the different absorption cross sections of SO2 isotopologues (i.e. wavelength dependent effect; without self-shielding) are only minor (potentially up to +4‰ for Δ33S). Under reducing conditions, however, another S-MIF signal with Δ36S/Δ33S ratio of ∼+0.7 is produced due to collision-induced intersystem crossing (ISC) from singlet to triplet states of SO2 (Whitehill et al., 2013), and should also be transferred into the final product that is responsible for changing the Δ36S/Δ33S slope. Based on a photochemical model of the S-O-C system with the two S-MIF-yielding reactions, the largest S-MIF observed in the late Archean Mt. McRae Fm. (Δ33S = + 9.4 ‰, Δ36S = - 7.5 ‰) can be reproduced by solar UV irradiation of a SO2

  15. Multiple oxygen and sulfur isotopic analyses on water-soluble sulfate in bulk atmospheric deposition from the southwestern United States

    USGS Publications Warehouse

    Bao, H.; Reheis, M.C.

    2003-01-01

    Sulfate is a major component of bulk atmospheric deposition (including dust, aerosol, fog, and rain). We analyzed sulfur and oxygen isotopic compositions of water-soluble sulfate from 40 sites where year-round dust traps collect bulk atmospheric deposition in the southwestern United States. Average sulfur and oxygen isotopic compositions (??34S and ??18O) are 5.8 ?? 1.4 (CDT) and 11.2 ?? 1.9 (SMOW) (n = 47), respectively. Samples have an oxygen 17 anomaly (?? 17O), with an average value of 1.0 ?? 0.6???. Except for a weak positive correlation between ??18O and ??17O values (r2 ??? 0.4), no correlation exists for ??18O versus ??34S, ?? 17O versus ??34S, or any of the three isotopic compositions versus elevation of the sample site. Exceptional positive ?? 17O values (up to 4.23???) are found in samples from sites in the vicinity of large cities or major highways, and near-zero ?? 17O values are found in samples close to dry lakes. Comparison of isotopic values of dust trap sulfate and desert varnish sulfate from the region reveals that varnish sulfate has average isotopic values that are ???4.8??? lower for ??18O, ???2.1??? higher for ??34S , and ???0.3??? lower for ?? 17O than those of the present-day bulk deposition sulfate. Although other factors could cause the disparity, this observation suggests a possibility that varnish sulfate may have recorded a long-term atmospheric sulfate deposition during the Holocene or Pleistocene, as well as the differences between sulfur and oxygen isotopic compositions of the preindustrial bulk deposition sulfate and those of the industrial era.

  16. Characterization, parameter estimation, and aircraft response statistics of atmospheric turbulence

    NASA Technical Reports Server (NTRS)

    Mark, W. D.

    1981-01-01

    A nonGaussian three component model of atmospheric turbulence is postulated that accounts for readily observable features of turbulence velocity records, their autocorrelation functions, and their spectra. Methods for computing probability density functions and mean exceedance rates of a generic aircraft response variable are developed using nonGaussian turbulence characterizations readily extracted from velocity recordings. A maximum likelihood method is developed for optimal estimation of the integral scale and intensity of records possessing von Karman transverse of longitudinal spectra. Formulas for the variances of such parameter estimates are developed. The maximum likelihood and least-square approaches are combined to yield a method for estimating the autocorrelation function parameters of a two component model for turbulence.

  17. Multiple sulfur-isotope signatures in Archean sulfates and their implications for the chemistry and dynamics of the early atmosphere

    PubMed Central

    Muller, Élodie; Philippot, Pascal; Rollion-Bard, Claire; Cartigny, Pierre

    2016-01-01

    Sulfur isotopic anomalies (∆33S and ∆36S) have been used to trace the redox evolution of the Precambrian atmosphere and to document the photochemistry and transport properties of the modern atmosphere. Recently, it was shown that modern sulfate aerosols formed in an oxidizing atmosphere can display important isotopic anomalies, thus questioning the significance of Archean sulfate deposits. Here, we performed in situ 4S-isotope measurements of 3.2- and 3.5-billion-year (Ga)-old sulfates. This in situ approach allows us to investigate the diversity of Archean sulfate texture and mineralogy with unprecedented resolution and from then on to deconvolute the ocean and atmosphere Archean sulfur cycle. A striking feature of our data is a bimodal distribution of δ34S values at ∼+5‰ and +9‰, which is matched by modern sulfate aerosols. The peak at +5‰ represents barite of different ages and host-rock lithology showing a wide range of ∆33S between −1.77‰ and +0.24‰. These barites are interpreted as primary volcanic emissions formed by SO2 photochemical processes with variable contribution of carbonyl sulfide (OCS) shielding in an evolving volcanic plume. The δ34S peak at +9‰ is associated with non–33S-anomalous barites displaying negative ∆36S values, which are best interpreted as volcanic sulfate aerosols formed from OCS photolysis. Our findings confirm the occurrence of a volcanic photochemical pathway specific to the early reduced atmosphere but identify variability within the Archean sulfate isotope record that suggests persistence throughout Earth history of photochemical reactions characteristic of the present-day stratosphere. PMID:27330111

  18. Multiple sulfur-isotope signatures in Archean sulfates and their implications for the chemistry and dynamics of the early atmosphere

    NASA Astrophysics Data System (ADS)

    Muller, Élodie; Philippot, Pascal; Rollion-Bard, Claire; Cartigny, Pierre

    2016-07-01

    Sulfur isotopic anomalies (∆33S and ∆36S) have been used to trace the redox evolution of the Precambrian atmosphere and to document the photochemistry and transport properties of the modern atmosphere. Recently, it was shown that modern sulfate aerosols formed in an oxidizing atmosphere can display important isotopic anomalies, thus questioning the significance of Archean sulfate deposits. Here, we performed in situ 4S-isotope measurements of 3.2- and 3.5-billion-year (Ga)-old sulfates. This in situ approach allows us to investigate the diversity of Archean sulfate texture and mineralogy with unprecedented resolution and from then on to deconvolute the ocean and atmosphere Archean sulfur cycle. A striking feature of our data is a bimodal distribution of δ34S values at ˜+5‰ and +9‰, which is matched by modern sulfate aerosols. The peak at +5‰ represents barite of different ages and host-rock lithology showing a wide range of ∆33S between -1.77‰ and +0.24‰. These barites are interpreted as primary volcanic emissions formed by SO2 photochemical processes with variable contribution of carbonyl sulfide (OCS) shielding in an evolving volcanic plume. The δ34S peak at +9‰ is associated with non-33S-anomalous barites displaying negative ∆36S values, which are best interpreted as volcanic sulfate aerosols formed from OCS photolysis. Our findings confirm the occurrence of a volcanic photochemical pathway specific to the early reduced atmosphere but identify variability within the Archean sulfate isotope record that suggests persistence throughout Earth history of photochemical reactions characteristic of the present-day stratosphere.

  19. Solar Radiation Estimated Through Mesoscale Atmospheric Modeling over Northeast Brazil

    NASA Astrophysics Data System (ADS)

    de Menezes Neto, Otacilio Leandro; Costa, Alexandre Araújo; Ramalho, Fernando Pinto; de Maria, Paulo Henrique Santiago

    2009-03-01

    The use of renewable energy sources, like solar, wind and biomass is rapidly increasing in recent years, with solar radiation as a particularly abundant energy source over Northeast Brazil. A proper quantitative knowledge of the incoming solar radiation is of great importance for energy planning in Brazil, serving as basis for developing future projects of photovoltaic power plants and solar energy exploitation. This work presents a methodology for mapping the incoming solar radiation at ground level for Northeast Brazil, using a mesoscale atmospheric model (Regional Atmospheric Modeling System—RAMS), calibrated and validated using data from the network of automatic surface stations from the State Foundation for Meteorology and Water Resources from Ceará (Fundação Cearense de Meteorologia e Recursos Hídricos- FUNCEME). The results showed that the model exhibits systematic errors, overestimating surface radiation, but that, after the proper statistical corrections, using a relationship between the model-predicted cloud fraction, the ground-level observed solar radiation and the incoming solar radiation estimated at the top of the atmosphere, a correlation of 0.92 with a confidence interval of 13.5 W/m2 is found for monthly data. Using this methodology, we found an estimate for annual average incoming solar radiation over Ceará of 215 W/m2 (maximum in October: 260 W/m2).

  20. Theoretical estimates of equilibrium sulfur isotope effects in aqueous sulfur systems: Highlighting the role of isomers in the sulfite and sulfoxylate systems

    NASA Astrophysics Data System (ADS)

    Eldridge, D. L.; Guo, W.; Farquhar, J.

    2016-12-01

    We present theoretical calculations for all three isotope ratios of sulfur (33S/32S, 34S/32S, 36S/32S) at the B3LYP/6-31+G(d,p) level of theory for aqueous sulfur compounds modeled in 30-40H2O clusters spanning the range of sulfur oxidation state (Sn, n = -2 to +6) for estimating equilibrium fractionation factors in aqueous systems. Computed 34β values based on major isotope (34S/32S) reduced partition function ratios (RPFRs) scale to a first order with sulfur oxidation state and coordination, where 34β generally increase with higher oxidation state and increasing coordination of the sulfur atom. Exponents defining mass dependent relationships based on β values (x/34κ = ln(xβ)/ln(34β), x = 33 or 36) conform to tight ranges over a wide range of temperature for all aqueous compounds (33/34κ ≈ 0.5148-0.5159, 36/34κ ≈ 1.89-1.90 from T ⩾ 0 °C). The exponents converge near a singular value for all compounds at the high temperature limit (33/34κT→∞ = 0.51587 ± 0.00003 and 36/34κT→∞ = 1.8905 ± 0.0002; 1 s.d. of all computed compounds), and typically follow trends based on oxidation state and coordination similar to those seen in 34β values at lower temperatures. Theoretical equilibrium fractionation factors computed from these β-values are compared to experimental constraints for HSO3-T(aq)/SO2(g, aq), SO2(aq)/SO2(g), H2S(aq)/H2S(g), H2S(aq)/HS-(aq), SO42-(aq)/H2ST(aq), S2O32-(aq) (intramolecular), and S2O32-(aq)/H2ST(aq), and generally agree within a reasonable estimation of uncertainties. We make predictions of fractionation factors where other constraints are unavailable. Isotope partitioning of the isomers of protonated compounds in the sulfite and sulfoxylate systems depend strongly on whether protons are bound to either sulfur or oxygen atoms. The magnitude of the HSO3-T/SO32- major isotope (34S/32S) fractionation factor is predicted to increase with temperature from 0 to 70 °C due to the combined effects of the large magnitude (HS)O3

  1. Development of a pretreatment system for the analysis of atmospheric reduced sulfur compounds.

    PubMed

    Son, Youn-Suk; Lee, Gangwoong; Kim, Jo-Chun; Han, Jin-Seok

    2013-11-05

    A new pretreatment system was used to evaluate a technology to analyze reduced sulfur compounds (RSCs). To conduct this research, a self-developed custom dryer (Desolvator) and a thermal desorber system (TDS) were installed in the front of GC/PFPD. The syringe pump inside the TDS was devised in such a way that it can be desorbed in a relatively low desorption temperature and low vacuum (730 Pa). When comparing water removal efficiency of the Desolvator and frequently used Nafion dryer, the removal efficiency of the Desolvator stood between 94.6 and 96.1%, considerably higher and more stable than the Nafion dryer (81.3-94.5%). Moreover, analyses were made under various conditions in order to minimize the loss of samples when analyzing sulfur compounds using the TDS, and it was determined that adsorption temperatures less than -25 °C and a flow rate of 50 mL/min were appropriate for the efficient analysis of these sulfur compounds. Moreover, the desorption flow rate and the degree of a vacuum were found to be significant variables for the RSCs desorption. Besides, it was observed that a peculiar peak was formed by thermal decomposition when some sulfur compounds were rapidly desorbed at high desorption temperatures.

  2. Atmospheric Sulfur Dioxide in the United States: Can the Standards be Justified or Afforded?

    ERIC Educational Resources Information Center

    Megonnell, William H.

    1975-01-01

    Recent reviews have concluded that there is no basis for changing the standards set by the EPA in 1971, even though the data base was insufficient then for a quantifiable, scientific definition of clean air. Examination of data shows that the United States does not have a sulfur dioxide problem. (Author/BT)

  3. Regional source identification of atmospheric aerosols in Beijing based on sulfur isotopic compositions

    NASA Astrophysics Data System (ADS)

    Lianfang, Wei; Pingqing, Fu; Xiaokun, Han; Qingjun, Guo; Yele, Sun; Zifa, Wang

    2016-04-01

    65 daily PM2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months representing the four seasons between September 2013 and July 2014. Inorganic ions, organic/elemental carbon and stable sulfur isotopes of sulfate aerosols were analyzed systematically. The "fingerprint" characteristics of the stable sulfur isotopic composition, together with trajectory clustering modeled by HYSPLIT-4 and potential source contribution function (PSCF), were employed for identifying potential regional sources. Results obviously exhibited the distinctive seasonality for various aerosol speciation associated with PM2.5 in Beijing with sulfate, nitrate, ammonium, organic matter, and element carbon being the dominant species. Elevated chloride associated with higher concentration of organics were found in autumn and winter, due to enhanced coal combustion emissions. The δ34S values of Beijing aerosol samples ranged from 2.94‰ to 10.2‰ with an average value of 6.18±1.87‰ indicating that the major sulfur source is direct fossil fuel burning-related emissions. Owning to a temperature-dependent fractionation and elevated biogenic sources of isotopically light sulfur in summer, the δ34S values had significant seasonal variations with a winter maximum ( 8.6‰)and a summer minimum ( 5.0‰). The results of trajectory clustering and the PSCF method demonstrated that higher concentrations of sulfate with lower sulfur isotope ratios ( 4.83‰) were associated with air masses from the south, southeast or east, whereas lower sulfate concentrations with higher δ34S values ( 6.69‰) when the air masses were mainly from north or northwest. These results suggested two main different kinds of regional coal combustion sources contributed to the pollution in Beijing.

  4. Theoretical studies of the marine sulfur cycle

    NASA Technical Reports Server (NTRS)

    Toon, Owen B.; Kasting, James B.; Liu, May S.

    1985-01-01

    Several reduced sulfur compounds are produced by marine organisms and then enter the atmosphere, where they are oxidized and ultimately returned to the ocean or the land. The oceanic dimethyl sulfide (DMS) flux, in particular, represents a significant fraction of the annual global sulfur input to the atmosphere. In the atmosphere, this gas is converted to sulfur dioxide (SO2), methane sulfonic acid, and other organic acids which are relatively stable and about which little is known. SO2 is a short lived gas which, in turn, is converted to sulfuric acid and other sulfate compounds which contribute significantly to acid rain. Because of the complexity of the sulfur system, it is not well understood even in the unperturbed atmosphere. However, a number of new observations and experiments have led to a significant increase in the understanding of this system. A number of one dimensional model experiments were conducted on the gas phase part of the marine sulfur cycle. The results indicate the measured concentration of DMS and the amplitude of its diurnal cycle are in agreement with estimates of its global flux. It was also found that DMS can make a large contribution to the background SO2 concentration in the free troposphere. Estimates of CS2 concentrations in the atmosphere are inconsistent with estimated fluxes; however, measured reaction rates are consistent with the observed steep tropospheric gradient in CS2. Observations of CS2 are extremely sparse. Further study is planned.

  5. Theoretical estimation of equilibrium sulfur isotope fractionations among aqueous sulfite species: Implications for isotope models of microbial sulfate reduction

    NASA Astrophysics Data System (ADS)

    Eldridge, D. L.; Farquhar, J.; Guo, W.

    2015-12-01

    Sulfite (sensu lato), an intermediate in a variety sulfur redox processes, plays a particularly important role in microbial sulfate reduction. It exists intracellularly as multiple species between sets of enzymatic reactions that transform sulfate to sulfide, with the exact speciation depending on pH, T, and ionic strength. However, the complex speciation of sulfite is ignored in current isotope partitioning models of microbial sulfate reduction and simplified solely to the pyramidal SO32- (sulfite sensu stricto), due to a lack of appropriate constraints. We theoretically estimated the equilibrium sulfur isotope fractionations (33S/32S, 34S/32S, 36S/32S) among all documented sulfite species in aqueous solution, including sulfite (SO32-), bisulfite isomers and dimers ((HS)O3-, (HO)SO2-, S2O52-), and SO2(aq), through first principles quantum mechanical calculations. The calculations were performed at B3LYP/6-31+G(d,p) level using cluster models with 30-40 water molecules surrounding the solute. Our calculated equilibrium fractionation factors compare well to the available experimental constraints and suggest that the minor and often-ignored tetrahedral (HS)O3- isomer of bisulfite strongly influences isotope partitioning behavior in the sulfite system under most environmentally relevant conditions, particularly fractionation magnitudes and unusual temperature dependence. For example, we predict that sulfur isotope fractionation between sulfite and bulk bisulfite in solution should have an apparent inverse temperature dependence due to the influence of (HS)O3- and its increased stability at higher temperatures. Our findings highlight the need to appropriately account for speciation/isomerization of sulfur species in sulfur isotope studies. We will also present similar calculation results of other aqueous sulfur compounds (e.g., H2S/HS-, SO42-, S2O32-, S3O62-, and poorly documented SO22- species), and discuss the implication of our results for microbial sulfate

  6. Atmospheric trend and emission estimates for HFC-43-10mee (1999 to 2010)

    NASA Astrophysics Data System (ADS)

    Arnold, T.; Ivy, D. J.; Muhle, J.; Harth, C. M.; Salameh, P.; Weiss, R. F.

    2010-12-01

    We present the first atmospheric measurements of HFC-43-10mee (1,1,1,2,2,3,4,5,5,5-decafluoropentane), an anthropogenic gas introduced in the mid-1990s as a substitute for CFC-113 (1,1,2-trichlorotrifluoroethane). The global warming potential of this HFC (hydrofluorocarbon) has been reported as 1640 (100-year time horizon), hence, its inclusion within a class of chemicals in the Kyoto Protocol and now its consideration for addition in the Montreal Protocol. Commercial HFC-43-10mee is a mixture of two diastereomers; both detectable using the Medusa GC-MS cryogenic trapping system (Miller et al., 2008), and included in our calculations for total HFC-43-10mee concentration. Chen et al. [2010] recently reported that the diastereomers have identical lifetimes in the troposphere of ≈18 years. Our northern hemisphere (NH) tropospheric record spans from 1999 to present day, utilizing 12 archive samples together with recent in situ measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) program at Trinidad Head and La Jolla, California. Precisions of < 0.01 ppt (parts-per-trillion, dry air mole fraction) allow for observation of an accelerated rise from 0.04 ppt in 2000 (growth rate of 0.01 ppt/yr) to 0.10 ppt in 2005 (0.02 ppt/yr) and 0.21 ppt in 2010 (0.03 ppt/yr). From the experimentally defined mole fractions in the background NH, we estimate the growth trend in the southern hemisphere using a simple box model which includes the stratosphere. Further, we estimate ‘top-down’ emissions to the global atmosphere for 2009 at ≈ 1200 tonnes. ‘Bottom-up’ estimates from the Emission Database for Global Atmospheric Research (EDGAR) v.4.0 only include emissions from Austria and France in 2005, which total 206 tonnes. For comparison, the global emissions in 2005 from our model equate to ≈ 800 tonnes. Further measurement and modeling efforts are warranted together with projections of future consumption. References: Miller, B. R., R. F. Weiss, P. K

  7. Reactions of SIV species with organic compounds: formation mechanisms of organo-sulfur derivatives in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Passananti, Monica; Shang, Jing; Dupart, Yoan; Perrier, Sébastien; George, Christian

    2015-04-01

    Secondary organic aerosol (SOA) have an important impact on climate, air quality and human health. However the chemical reactions involved in their formation and growth are not fully understood or well-constrained in climate models. It is well known that inorganic sulfur (mainly in oxidation states (+IV) and (+VI)) plays a key role in aerosol formation, for instance sulfuric acid is known to be a good nucleating gas. In addition, acid-catalyzed heterogeneous reactions of organic compounds has shown to produce new particles, with a clear enhancement in the presence of ozone (Iinuma 2013). Organosulfates have been detected in tropospheric particles and aqueous phases, which suggests they are products of secondary organic aerosol formation process (Tolocka 2012). Originally, the production of organosulfates was explained by the esterification reaction of alcohols, but this reaction in atmosphere is kinetically negligible. Other formation pathways have been suggested such as hydrolysis of peroxides and reaction of organic matter with sulfite and sulfate radical anions (SO3-, SO4-) (Nozière 2010), but it remains unclear if these can completely explain atmospheric organo-sulfur aerosol loading. To better understand the formation of organo-sulfur compounds, we started to investigate the reactivity of SIV species (SO2 and SO32-) with respect to specific functional groups (organic acids and double bonds) on atmospherically relevant carboxylic acids and alkenes. The experiments were carried out in the homogeneous aqueous phase and at the solid-gas interface. A custom built coated-wall flow tube reactor was developed to control relativity humidity, SO2 concentration, temperature and gas flow rate. Homogeneous and heterogeneous reaction kinetics were measured and resulting products were identified using liquid chromatography coupled with an orbitrap mass spectrometer (LC-HR-MS). The experiments were performed with and without the presence of ozone in order to evaluate any

  8. A study of the total atmospheric sulfur dioxide load using ground-based measurements and the satellite derived Sulfur Dioxide Index

    NASA Astrophysics Data System (ADS)

    Georgoulias, A. K.; Balis, D.; Koukouli, M. E.; Meleti, C.; Bais, A.; Zerefos, C.

    We present characteristics of the sulfur dioxide (SO 2) loading over Thessaloniki, Greece, and seven other selected sites around the world using SO 2 total column measurements from Brewer spectrophotometers together with satellite estimates of the Version 8 TOMS Sulfur Dioxide Index (SOI) over the same locations, retrieved from Nimbus 7 TOMS (1979-1993), Earth Probe TOMS (1996-2003) and OMI/Aura (2004-2006). Traditionally, the SOI has been used to quantify the SO 2 quantities emitted during great volcanic eruptions. Here, we investigate whether the SOI can give an indication of the total SO 2 load for areas and periods away from eruptive volcanic activity by studying its relative changes as a correlative measure to the SO 2 total column. We examined time series from Thessaloniki and another seven urban and non-urban stations, five in the European Union (Arosa, De Bilt, Hohenpeissenberg, Madrid, Rome) and two in India (Kodaikanal, New Delhi). Based on the Brewer data, Thessaloniki shows high SO 2 total columns for a European Union city but values are still low if compared to highly affected regions like those in India. For the time period 1983-2006 the SO 2 levels above Thessaloniki have generally decreased with a rate of 0.028 Dobson Units (DU) per annum, presumably due to the European Union's strict sulfur control policies. The seasonal variability of the SO 2 total column exhibits a double peak structure with two maxima, one during winter and the second during summer. The winter peak can be attributed to central heating while the summer peak is due to synoptic transport from sources west of the city and sources in the north of Greece. A moderate correlation was found between the seasonal levels of Brewer total SO 2 and SOI for Thessaloniki, Greece ( R = 0.710-0.763) and Madrid, Spain ( R = 0.691) which shows that under specific conditions the SOI might act as an indicator of the SO 2 total load.

  9. Observation of wavelength-sensitive mass-independent sulfur isotope effects during SO2 photolysis: Implications for the early atmosphere

    NASA Astrophysics Data System (ADS)

    Farquhar, James; Savarino, Joel; Airieau, Sabine; Thiemens, Mark H.

    2001-12-01

    Mass-independent isotopic signatures for δ33S, δ34S, and δ36S produced in the photolysis of sulfur dioxide exhibit a strong wavelength dependence. Photolysis experiments with three light sources (ArF excimer laser (193 nm), mercury resonance lamp (184.9 and 253.7 nm), and KrF excimer laser (248 nm) are presented. Products of sulfur dioxide photolysis undertaken with 193-nm radiation exhibit characteristics that are similar to sulfur multiple-isotope data for terrestrial sedimentary rock samples older than 2450 Ma (reported by Farquhar et al. [2000a]), while photolysis experiments undertaken with radiation at other wavelengths (longer than 220 nm and at 184.9 nm) exhibit different characteristics. The spectral window between 190 and 220 nm falls between the Schumann-Runge bands of oxygen and the Hartley bands of ozone, and its absorption is therefore more sensitive to changes in altitude and atmospheric oxygen content than neighboring wavelengths. These two observations are used to suggest a link between sulfur dioxide photolysis at 193 nm and sulfur isotope anomalies in Archean rocks. This hypothesis includes the suggestion that UV wavelengths shorter than 200 nm penetrated deep in the Earth's atmosphere during the Archean. Potential implications of this hypothesis for the chemistry, composition, and UV absorption of the atmosphere are explored. We also explore the implications of these observations for documentation of bacterial sulfur metabolisms early in Earth's history.

  10. A Direct Estimate of Climate Sensitivity from Atmospheric Structure

    NASA Astrophysics Data System (ADS)

    Lacis, A. A.

    2014-12-01

    The nominal equilibrium climate sensitivity of about 3°C for doubled CO2 is obtained from direct climate model calculations and from simulations of the historical surface temperature record. A similar value of equilibrium climate sensitivity has been inferred from the geological ice core record. A further independent estimate of climate sensitivity can be derived directly from the atmospheric temperature, cloud, and absorbing gas structure. Attribution of individual contributions to the terrestrial greenhouse effect by individual atmospheric constituents shows that water vapor and clouds account for about 75% of the total greenhouse effect, while CO2 and the other minor non-condensing green house gases account for the remaining 25%. It is generally understood that water vapor and cloud contributions to the greenhouse effect arise as feedback effects, and that the non-condensing greenhouse gas contribution can be identified as the radiative forcing component. From this alone, a climate feedback sensitivity of f = 4, or about 5°C for doubled CO2 can be inferred. Accounting further for the negative temperature lapse rate feedback that is not directly included in the attribution analysis, and allowing for a residual non-condensing component of the water vapor feedback, brings the equilibrium climate sensitivity that is inferred from atmospheric structural analysis to the 3°C range for doubled CO2, in good agreement with the equilibrium climate sensitivity that is obtained from comparisons to historical and geological global temperature changes.

  11. Uncertainties associated with parameter estimation in atmospheric infrasound arrays

    NASA Astrophysics Data System (ADS)

    Szuberla, Curt A. L.; Olson, John V.

    2004-01-01

    This study describes a method for determining the statistical confidence in estimates of direction-of-arrival and trace velocity stemming from signals present in atmospheric infrasound data. It is assumed that the signal source is far enough removed from the infrasound sensor array that a plane-wave approximation holds, and that multipath and multiple source effects are not present. Propagation path and medium inhomogeneities are assumed not to be known at the time of signal detection, but the ensemble of time delays of signal arrivals between array sensor pairs is estimable and corrupted by uncorrelated Gaussian noise. The method results in a set of practical uncertainties that lend themselves to a geometric interpretation. Although quite general, this method is intended for use by analysts interpreting data from atmospheric acoustic arrays, or those interested in designing and deploying them. The method is applied to infrasound arrays typical of those deployed as a part of the International Monitoring System of the Comprehensive Nuclear-Test-Ban Treaty Organization.

  12. Solubility of methanol in low-temperature aqueous sulfuric acid and implications for atmospheric particle composition

    NASA Technical Reports Server (NTRS)

    Iraci, Laura T.; Essin, Andrew M.; Golden, David M.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    Using traditional Knudsen cell techniques, we find well-behaved Henry's law uptake of methanol in aqueous 45 - 70 wt% H2SO4 solutions at temperatures between 197 and 231 K. Solubility of methanol increases with decreasing temperature and increasing acidity, with an effective Henry's law coefficient ranging from 10(exp 5) - 10(exp 8) M/atm. Equilibrium uptake of methanol into sulfuric acid aerosol particles in the upper troposphere and lower stratosphere will not appreciably alter gas-phase concentrations of methanol. The observed room temperature reaction between methanol and sulfuric acid is too slow to provide a sink for gaseous methanol at the temperatures of the upper troposphere and lower stratosphere. It is also too slow to produce sufficient quantities of soluble reaction products to explain the large amount of unidentified organic material seen in particles of the upper troposphere.

  13. Estimating Longwave Atmospheric Emissivity in the Canadian Rocky Mountains

    NASA Astrophysics Data System (ADS)

    Ebrahimi, S.; Marshall, S. J.

    2014-12-01

    Incoming longwave radiation is an important source of energy contributing to snow and glacier melt. However, estimating the incoming longwave radiation from the atmosphere is challenging due to the highly varying conditions of the atmosphere, especially cloudiness. We analyze the performance of some existing models included a physically-based clear-sky model by Brutsaert (1987) and two different empirical models for all-sky conditions (Lhomme and others, 2007; Herrero and Polo, 2012) at Haig Glacier in the Canadian Rocky Mountains. Models are based on relations between readily observed near-surface meteorological data, including temperature, vapor pressure, relative humidity, and estimates of shortwave radiation transmissivity (i.e., clear-sky or cloud-cover indices). This class of models generally requires solar radiation data in order to obtain a proxy for cloud conditions. This is not always available for distributed models of glacier melt, and can have high spatial variations in regions of complex topography, which likely do not reflect the more homogeneous atmospheric longwave emissions. We therefore test longwave radiation parameterizations as a function of near-surface humidity and temperature variables, based on automatic weather station data (half-hourly and mean daily values) from 2004 to 2012. Results from comparative analysis of different incoming longwave radiation parameterizations showed that the locally-calibrated model based on relative humidity and vapour pressure performs better than other published models. Performance is degraded but still better than standard cloud-index based models when we transfer the model to another site, roughly 900 km away, Kwadacha Glacier in the northern Canadian Rockies.

  14. Nitrogen trifluoride global emissions estimated from updated atmospheric measurements

    PubMed Central

    Arnold, Tim; Harth, Christina M.; Mühle, Jens; Manning, Alistair J.; Salameh, Peter K.; Kim, Jooil; Ivy, Diane J.; Steele, L. Paul; Petrenko, Vasilii V.; Severinghaus, Jeffrey P.; Baggenstos, Daniel; Weiss, Ray F.

    2013-01-01

    Nitrogen trifluoride (NF3) has potential to make a growing contribution to the Earth’s radiative budget; however, our understanding of its atmospheric burden and emission rates has been limited. Based on a revision of our previous calibration and using an expanded set of atmospheric measurements together with an atmospheric model and inverse method, we estimate that the global emissions of NF3 in 2011 were 1.18 ± 0.21 Gg⋅y−1, or ∼20 Tg CO2-eq⋅y−1 (carbon dioxide equivalent emissions based on a 100-y global warming potential of 16,600 for NF3). The 2011 global mean tropospheric dry air mole fraction was 0.86 ± 0.04 parts per trillion, resulting from an average emissions growth rate of 0.09 Gg⋅y−2 over the prior decade. In terms of CO2 equivalents, current NF3 emissions represent between 17% and 36% of the emissions of other long-lived fluorinated compounds from electronics manufacture. We also estimate that the emissions benefit of using NF3 over hexafluoroethane (C2F6) in electronics manufacture is significant—emissions of between 53 and 220 Tg CO2-eq⋅y−1 were avoided during 2011. Despite these savings, total NF3 emissions, currently ∼10% of production, are still significantly larger than expected assuming global implementation of ideal industrial practices. As such, there is a continuing need for improvements in NF3 emissions reduction strategies to keep pace with its increasing use and to slow its rising contribution to anthropogenic climate forcing. PMID:23341630

  15. Watershed-scale changes in terrestrial nitrogen cycling during a period of decreased atmospheric nitrate and sulfur deposition

    NASA Astrophysics Data System (ADS)

    Sabo, Robert D.; Scanga, Sara E.; Lawrence, Gregory B.; Nelson, David M.; Eshleman, Keith N.; Zabala, Gabriel A.; Alinea, Alexandria A.; Schirmer, Charles D.

    2016-12-01

    sites. Other factors, such as decreased sulfur deposition, disturbance, long-term successional trends, and/or increasing atmospheric CO2 concentrations, may also influence trends in tree-ring δ15N values. Furthermore, declines in terrestrial N availability inferred from tree-ring δ15N values do not always correspond with decreased stream nitrate export or increased retention of atmospherically deposited N.

  16. Stratospheric sulfuric acid fraction and mass estimate for the 1982 volcanic eruption of El Chichon

    NASA Technical Reports Server (NTRS)

    Hofmann, D. J.; Rosen, J. M.

    1983-01-01

    The stratospheric sulfuric acid fraction and mass for the 1982 volcanic eruptions of El Chichon are investigated using data from balloon soundings at Laramie (41 deg N) and in southern Texas (27-29 deg N). The total stratospheric mass of these eruptions is estimated to be approximately 8 Tg about 6.5 months after the eruption with possibly as much as 20 Tg in the stratosphere about 45 days after the eruption. Observations of the aerosol in Texas revealed two primary layers, both highly volatile at 150 C. Aerosol in the upper layer at about 25 km was composed of an approximately 80 percent H2SO4 solution while the lower layer at approximately 18 km was composed of a 60-65 percent H2SO4 solution aerosol. It is calculated that an H2SO4 vapor concentration of at least 3 x 10 to the 7th molecules/cu cm is needed to sustain the large droplets in the upper layer. An early bi-modal nature in the size distribution indicates droplet nucleation from the gas phase during the first 3 months, while the similarity of the large particle profiles 2 months apart shows continued particle growth 6.5 months after the explosion.

  17. Mass independent oxygen and sulfur isotopic compositions of environmental sulfate and nitrate. A new probe of atmospheric, hydrospheric and geological processes

    NASA Astrophysics Data System (ADS)

    Thiemens, M.; Michalski, G.; Romero, A.; McCabe, J.

    2003-04-01

    Aerosol sulfate is well known to exert a significant influence on the Earth’s atmosphere and surface. They mediate climate in its capacity as a cloud condensation nuclei (CCN) and as a visible light scattering agent. These particles are respirable, with severe cardiovascular disease consequences. Removal by wet and dry depositions is well known to cause surficial damage to biota, biodiversity, and structures. Despite decades of high precision global concentration measurements, single isotope ratio measurements (d18O, d34S) and high quality modeling efforts, there remain unresolved issues with respect to resolution of relative oxidative processes (homogenous vs. heterogeneous), transformation mechanisms, and identification of sources, proximal and distal. Mass independent oxygen isotopic compositions have added new insights un attainable by other techniques. These observations ideally complement other measurements in an effort to improve parameters used in modeling aerosols and climate. Recent sulfur mass independent compositions have potentially added a new means to recognize upper atmospheric photolytic processes. Aerosol nitrate is estimated to nearly double in the next half century, with potentially severe consequences which include soil acidification, loss of biodiversity, eutrophication of coastal and freshwaters, and, human cardiovascular disease. Loss of fresh water lake clarity, e.g. Lake Tahoe is also believed to occur due to increased nitrogen levels. As in the case of atmospheric sulfate, mass independent oxygen isotopic signatures have been observed in nitrate. The D17O is one of the largest mass independent isotopic signatures observed in any environmental species with the exception of ozone. These measurements have demonstrated the ability to provide new insight into the nitrogen cycle, including atmospheric, hydrospheric and geologic processes.

  18. Estimating Uncertainty in Atmospheric Models - Application and new Approaches of Lyapunov Vector Estimations

    NASA Astrophysics Data System (ADS)

    Keller, J. D.; Hense, A.; Rhodin, A.

    2010-12-01

    The atmosphere, like other geophysical non-linear systems, is chaotic by nature. Therefore, estimating the predictability of the atmosphere is among the main focuses of the scientific community. The degree of chaos or predictability of a system can be expressed by the Lyapunov exponents which represents the temporal growth rate of the distance between two system states initially lying close to another. The corresponding spatial representations of uncertainty are the Lyapunov vectors. The estimation or approximation of Lyapunov vectors is therefore of great interest to the researcher dealing with a chaotic system. However, for the atmosphere estimation methods often tend to approximate the leading Lyapunov vectors or the vectors corresponding to the largest Lyapunov exponents. Depending on the system and situation, smaller Lyapunov exponents may indeed be of more interest. We therefore present research results from two fields of work: (1) uncertainty estimation applied to weather forecasting using techniques adapted to the given practical limitations and (2) idealized Lyapunov analysis using a simple global circulation model (GCM). Perturbation structures intended for ensemble initialization and generated using the Bred Vector (BV) technique for example, tend to converge with the Leading Lyapunov vector disregarding other possibly important information on system/model uncertainty. Our Ensemble Transform Bred Vector (ETBV) approach (Keller et al., 2010) based on the exploitation of the similarities in the BV structures to generate perturbations with different error growth characteristics. We present results from ETBV-driven ensemble forecasts with a global numerical weather prediction model and the performance gain over forecasts driven by simple BVs. We further investigate the effect of downscaling of the resulting large scale uncertainty patterns as forcing for meso-scale weather prediction, thereby testing several different downscaling approaches. We also consider

  19. Estimating sources, sinks and fluxes of reactive atmospheric compounds within a forest canopy

    NASA Astrophysics Data System (ADS)

    Ghannam, K.; Duman, T.; Walker, J. T.; Bash, J. O.; Huang, C. W.; Khlystov, A.; Katul, G. G.

    2015-12-01

    While few dispute the significance of within-canopy sources or sinks of reactive gaseous and particulate compounds, their estimation continues to be the subject of active research and debate. Reactive species undergo turbulent dispersion within an inhomogeneous flow field, and may be subjected to chemical, biological and/or physical deposition, emissions or transformations on leaves, woody elements, and the forest floor. This system involves chemical reactions and biological processes with multiple time scales and represents the terrestrial ecosystem's exposure to nutrient and acid deposition and atmospheric oxidants. The quantification of these processes is a first step in better understanding the ecological impact of air pollution and feedback to atmospheric composition. Hence, it follows that direct measurements of sources or sinks is difficult to conduct in the presence of all these processes. However, mean scalar concentration profiles measured within the canopy can be used to infer the profile distribution of effective sinks and sources if the flow field is known. This is commonly referred to as the 'inverse problem'. In-canopy and above-canopy multi-level concentration measurements of reactive nitrogen compounds (ammonia, nitric acid, nitrous acid), as well as other compounds that are highly reactive to ammonia and its secondary products (hydrochloric acid and sulfur dioxide), are presented within a deciduous second-growth 180 year old oak-hickory forest situated within the Southeastern U.S. Two different approaches are used to solve for the source-sink distribution from the measured mean scalar concentration profiles: (1) an Eulerian high-order closure model that solves the scalar flux budget equation and (2) a new Lagrangian stochastic model that estimates the dispersion matrix. As each of these methods is subject to different assumptions, the combination of the two can be used to constrain the solution to the inverse problem and permit inference on the

  20. Holocene Concentrations of Methane in the Atmosphere are in Part Proportional to Concentrations of Sulfur Dioxide and Inversely Proportional to the Oxidizing Capacity of the Atmosphere

    NASA Astrophysics Data System (ADS)

    Ward, P. L.

    2008-12-01

    The atmosphere cleans itself by oxidizing pollutants. The primary oxidant is the hydroxyl radical (OH) formed by photodissociation of ozone in the near ultra-violet. Ozone and OH are in limited supply. Sulfur dioxide (SO2) absorbs near ultraviolet light limiting production of OH and reacts immediately with any available OH, forming sulfuric acid. Methane reacts more slowly with OH and will typically not be oxidized until there is little SO2. Thus a high concentration of methane indicates low oxidizing capacity. The rate at which SO2 is injected into the atmosphere controls oxidizing capacity and climate change in four ways: 1. Moderate rate: Large volcanic eruptions (VEI >=6) lower global temperatures for a few years when they are separated by years to decades so the oxidizing capacity of the atmosphere can fully recover. In 1991, Pinatubo volcano in the Philippines erupted 20 Mt SO2 and 491 Mt H2O, the largest volcanic eruption since 1912. The SO2 was oxidized primarily by OH to form a 99% pure aerosol of sulfuric acid and water at an elevation of 20-23 km. This aerosol reflected sunlight, lowering the world's temperature on average 0.4°C for three years. Ozone levels were reduced by 10%. Methane increased by 15 ppb for a year. The e-folding time for SO2 was 35 days. 2. High rate: When large eruptions occur once to several times per year, there is insufficient oxidizing capacity leading to increases in methane and other greenhouse gases and global warming. There were 15 times in the Holocene when large volcanoes erupted on average at least every year for 7 to 21 years. Man is now putting as much SO2 from burning fossil fuels into the atmosphere every year as one large volcano, causing current global warming. The two previous times were from 818-838 AD, the onset of the Medieval Warming Period, and from 180-143 BC, the onset of the Roman Warm Period. 3. Low rate: When there are no large eruptions for decades, the oxidizing capacity can catch up, cleaning the

  1. Modeling HOx/O3 chemistry in the tropical marine boundary during the Pacific Atmospheric Sulfur Experiment

    NASA Astrophysics Data System (ADS)

    Gu, D.; Gray, B. A.; Wang, Y.; Mauldin, L.; Cantrell, C.; Heikes, B. G.; Higbie, A.; O'Sullivan, D. W.; Campos, T.; Pollack, I. B.; Heizer, C. G.; Weinheimer, A. J.

    2008-12-01

    C-130 observations of OH, RO2, O3, CO, H2O2, and CH3OOH in the tropical marine boundary layer during the 2007 Pacific Atmospheric Sulfur Experiment are analyzed using a one- dimensional chemistry transport model. Meteorological parameters are simulated from the Weather Research and Forecasting model. The coupling of low-NOx photochemistry and mixing processes is examined over the relatively homogeneous region. Simulated vertical profiles of HOx radicals and peroxides are not always in agreement with the measurements. Potential factors contributing to the discrepancies are investigated. The large ozone decrease towards the surface is driven in part by large photochemical loss in the marine boundary layer. The vertical gradient is also regulated by the influx of ozone from free troposphere and diffusion transport in the boundary layer. This experimental constraint on model simulated vertical transport is evaluated.

  2. The influence of sulfur and hair growth on stable isotope diet estimates for grizzly bears

    PubMed Central

    Curtis, P. Jeff; Lafferty, Diana J. R.

    2017-01-01

    Stable isotope ratios of grizzly bear (Ursus arctos) guard hair collected from bears on the lower Stikine River, British Columbia (BC) were analyzed to: 1) test whether measuring δ34S values improved the precision of the salmon (Oncorhynchus spp.) diet fraction estimate relative to δ15N as is conventionally done, 2) investigate whether measuring δ34S values improves the separation of diet contributions of moose (Alces alces), marmot (Marmota caligata), and mountain goat (Oreamnos americanus) and, 3) examine the relationship between collection date and length of hair and stable isotope values. Variation in isotope signatures among hair samples from the same bear and year were not trivial. The addition of δ34S values to mixing models used to estimate diet fractions generated small improvement in the precision of salmon and terrestrial prey diet fractions. Although the δ34S value for salmon is precise and appears general among species and areas, sulfur ratios were strongly correlated with nitrogen ratios and therefore added little new information to the mixing model regarding the consumption of salmon. Mean δ34S values for the three terrestrial herbivores of interest were similar and imprecise, so these data also added little new information to the mixing model. The addition of sulfur data did confirm that at least some bears in this system ate marmots during summer and fall. We show that there are bears with short hair that assimilate >20% salmon in their diet and bears with longer hair that eat no salmon living within a few kilometers of one another in a coastal ecosystem. Grizzly bears are thought to re-grow hair between June and October however our analysis of sectioned hair suggested at least some hairs begin growing in July or August, not June and, that hair of wild bears may grow faster than observed in captive bears. Our hair samples may have been from the year of sampling or the previous year because samples were collected in summer when bears were

  3. The influence of sulfur and hair growth on stable isotope diet estimates for grizzly bears.

    PubMed

    Mowat, Garth; Curtis, P Jeff; Lafferty, Diana J R

    2017-01-01

    Stable isotope ratios of grizzly bear (Ursus arctos) guard hair collected from bears on the lower Stikine River, British Columbia (BC) were analyzed to: 1) test whether measuring δ34S values improved the precision of the salmon (Oncorhynchus spp.) diet fraction estimate relative to δ15N as is conventionally done, 2) investigate whether measuring δ34S values improves the separation of diet contributions of moose (Alces alces), marmot (Marmota caligata), and mountain goat (Oreamnos americanus) and, 3) examine the relationship between collection date and length of hair and stable isotope values. Variation in isotope signatures among hair samples from the same bear and year were not trivial. The addition of δ34S values to mixing models used to estimate diet fractions generated small improvement in the precision of salmon and terrestrial prey diet fractions. Although the δ34S value for salmon is precise and appears general among species and areas, sulfur ratios were strongly correlated with nitrogen ratios and therefore added little new information to the mixing model regarding the consumption of salmon. Mean δ34S values for the three terrestrial herbivores of interest were similar and imprecise, so these data also added little new information to the mixing model. The addition of sulfur data did confirm that at least some bears in this system ate marmots during summer and fall. We show that there are bears with short hair that assimilate >20% salmon in their diet and bears with longer hair that eat no salmon living within a few kilometers of one another in a coastal ecosystem. Grizzly bears are thought to re-grow hair between June and October however our analysis of sectioned hair suggested at least some hairs begin growing in July or August, not June and, that hair of wild bears may grow faster than observed in captive bears. Our hair samples may have been from the year of sampling or the previous year because samples were collected in summer when bears were

  4. Atmospheric dispersion estimates in the vicinity of buildings

    SciTech Connect

    Ramsdell, J.V. Jr.; Fosmire, C.J.

    1995-01-01

    A model describing atmospheric dispersion in the vicinity of buildings was developed for the U.S. Nuclear Regulatory Commission (NRC) in the late 1980s. That model has recently undergone additional peer review. The reviewers identified four areas of concern related to the model and its application. This report describes revisions to the model in response to the reviewers concerns. Model revision involved incorporation of explicit treatment of enhanced dispersion at low wind speeds in addition to explicit treatment of enhanced dispersion at high speeds resulting from building wakes. Model parameters are evaluated from turbulence data. Experimental diffusion data from seven reactor sites are used for model evaluation. Compared with models recommended in current NRC guidance to licensees, the revised model is less biased and shows more predictive skill. The revised model is also compared with two non-Gaussian models developed to estimate maximum concentrations in building wakes. The revised model concentration predictions are nearly the same as the predictions of the non-Gaussian models. On the basis of these comparisons of the revised model concentration predictions with experimental data and the predictions of other models, the revised model is found to be an appropriate model for estimating concentrations in the vicinity of buildings.

  5. Microwave Remote Sensing of the Temperature and Distribution of Sulfur Compounds in the Lower Atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Jenkins, Jon M.; Kolodner, Marc A.; Butler, Bryan J.; Suleiman, Shady H.; Steffes, Paul G.

    2002-08-01

    A multi-wavelength radio frequency observation of Venus was performed on April 5, 1996, with the Very Large Array to investigate potential variations in the vertical and horizontal distribution of temperature and the sulfur compounds sulfur dioxide (SO 2) and sulfuric acid vapor (H 2SO 4(g)) in the atmosphere of the planet. Brightness temperature maps were produced which feature significantly darkened polar regions compared to the brighter low-latitude regions at both observed frequencies. This is the first time such polar features have been seen unambiguously in radio wavelength observations of Venus. The limb-darkening displayed in the maps helps to constrain the vertical profile of H 2SO 4(g), temperature, and to some degree SO 2. The maps were interpreted by applying a retrieval algorithm to produce vertical profiles of temperature and abundance of H 2SO 4(g) given an assumed sub-cloud abundance of SO 2. The results indicate a substantially higher abundance of H 2SO 4(g) at high latitudes (above 45°) than in the low-latitude regions. The retrieved temperature profiles are up to 25 K warmer than the profile obtained by the Pioneer Venus sounder probe at altitudes below 40 km (depending on location and assumed SO 2 abundance). For 150 ppm of SO 2, it is more consistent with the temperature profile obtained by Mariner 5, extrapolated to the surface via a dry adiabat. The profiles obtained for H 2SO 4(g) at high latitudes are consistent with those derived from the Magellan radio occultation experiments, peaking at around 8 ppm at an altitude of 46 km and decaying rapidly away from that altitude. At low latitudes, no significant H 2SO 4(g) is observed, regardless of the assumed SO 2 content. This is well below that measured by Mariner 10 (Lipa and Tyler 1979, Icarus39, 192-208), which peaked at ˜14 ppm near 47 km. Our results favor ≤100 ppm of SO 2 at low latitudes and ≤50 ppm in polar regions. The low-latitude value is statistically consistent with the

  6. Spectral properties of condensed phases of disulfur monoxide, polysulfur oxide, and irradiated sulfur. [in planetary atmospheres

    NASA Technical Reports Server (NTRS)

    Hapke, Bruce; Graham, Francis

    1989-01-01

    The spectral reflectances of S2O, as well as the polysulfur oxide (PSO) condensate dissociation products of SO2 and condensates of elemental sulfur irradiated with UV light and X-rays, have been ascertained in the 200-1700 nm range with a view to the relevance of these compounds to the interpretation of planetary data. While S2O is a dark red solid, PSO is a pale yellow one that absorbs strongly in the UV but exhibits no bands in either the visible or near IR. Elemental S produces strong bands in the UV, and while it is normally white at room temperature, UV irradiation causes it to turn yellow. X-ray irradiation of S turns it orange.

  7. Spectral properties of condensed phases of disulfur monoxide, polysulfur oxide, and irradiated sulfur. [In planetary atmospheres

    SciTech Connect

    Hapke, B.; Graham, F. )

    1989-05-01

    The spectral reflectances of S2O, as well as the polysulfur oxide (PSO) condensate dissociation products of SO2 and condensates of elemental sulfur irradiated with UV light and X-rays, have been ascertained in the 200-1700 nm range with a view to the relevance of these compounds to the interpretation of planetary data. While S2O is a dark red solid, PSO is a pale yellow one that absorbs strongly in the UV but exhibits no bands in either the visible or near IR. Elemental S produces strong bands in the UV, and while it is normally white at room temperature, UV irradiation causes it to turn yellow. X-ray irradiation of S turns it orange. 24 refs.

  8. Stability of chromium (III) sulfate in atmospheres containing oxygen and sulfur

    NASA Technical Reports Server (NTRS)

    Jacob, K. T.; Rao, B. D.; Nelson, H. G.

    1978-01-01

    The stability of chromium sulfate in the temperature range from 880 K to 1040 K was determined by employing a dynamic gas-solid equilibration technique. The solid chromium sulfate was equilibrated in a gas stream of controlled SO3 potential. Thermogravimetric and differential thermal analyses were used to follow the decomposition of chromium sulfate. X-ray diffraction analysis indicated that the decomposition product was crystalline Cr2O3 and that the mutual solubility between Cr2(SO4)3 and Cr2O3 was negligible. Over the temperature range investigated, the decomposition pressure were significantly high so that chromium sulfate is not expected to form on commercial alloys containing chromium when exposed to gaseous environments containing oxygen and sulfur (such as those encountered in coal gasification).

  9. Atmospheric transport and deposition of acidic air pollutants

    SciTech Connect

    Murphy, C.E. Jr.

    1981-01-01

    Although general principles which govern atmospheric chemistry of sulfur are understood, a purely theoretical estimation of the magnitude of the processes is not likely to be useful. Furthermore, the data base necessary to make empirical estimates does not yet exist. The sulfur budget of the atmosphere appears to be dominated by man-associated sulfur. The important processes in deposition of man-associated sulfur are wet deposition of sulfate and dry deposition of SO/sub 2/. The relative importance of sulfate and SO/sub 2/ to sulfur deposition (input to watersheds) depends on the air concentrations, and either compound may be the greater contributor depending on conditions. (PSB)

  10. N2-, O2- and He-collision-induced broadening of sulfur dioxide ro-vibrational lines in the 9.2 μm atmospheric window

    NASA Astrophysics Data System (ADS)

    Tasinato, Nicola; Pietropolli Charmet, Andrea; Stoppa, Paolo; Giorgianni, Santi; Buffa, Giovanni

    2014-01-01

    Sulfur dioxide (SO2) is a molecule of considerable interest for both atmospheric chemistry and astrophysics. In the Earth's atmosphere, it enters in the sulfur cycle and it is ubiquitous present in polluted atmospheres, where it is responsible for acid rains. It is also of astrophysical and planetological importance, being present on Venus and in interstellar clouds. In this work the collisional broadening of a number of ν1 ro-vibrational lines of SO2 perturbed by N2, O2 and He are investigated at room temperature in the 9 μm atmospheric region by means of high resolution tunable diode laser (TDL) infrared spectroscopy. From N2- and O2-broadening coefficients, the broadening parameters of sulfur dioxide in air, useful for atmospheric applications, are derived as well. From the present measurements some conclusions on the quantum number dependence of the N2-, O2- and He-broadening coefficients are drawn. While the J dependence is weak for all the perturbers investigated, different trends with Ka are reported. N2-broadening coefficients show a slight decrease with increasing values of Ka, whereas O2 and He broadening cross sections first increase up to Ka″≈6 and then they keep a nearly constant value. A comparison and a brief discussion on the efficiency of self-, N2-, O2- and He-collisional dynamics are given. The data obtained represent a significant analysis on foreign broadening of SO2 useful for atmospheric remote sensing and astrophysical applications.

  11. Determination of the atmospheric lifetime and global warming potential of sulfur hexafluoride using a three-dimensional model

    NASA Astrophysics Data System (ADS)

    Kovács, Tamás; Feng, Wuhu; Totterdill, Anna; Plane, John M. C.; Dhomse, Sandip; Gómez-Martín, Juan Carlos; Stiller, Gabriele P.; Haenel, Florian J.; Smith, Christopher; Forster, Piers M.; García, Rolando R.; Marsh, Daniel R.; Chipperfield, Martyn P.

    2017-01-01

    We have used the Whole Atmosphere Community Climate Model (WACCM), with an updated treatment of loss processes, to determine the atmospheric lifetime of sulfur hexafluoride (SF6). The model includes the following SF6 removal processes: photolysis, electron attachment and reaction with mesospheric metal atoms. The Sodankylä Ion Chemistry (SIC) model is incorporated into the standard version of WACCM to produce a new version with a detailed D region ion chemistry with cluster ions and negative ions. This is used to determine a latitude- and altitude-dependent scaling factor for the electron density in the standard WACCM in order to carry out multi-year SF6 simulations. The model gives a mean SF6 lifetime over an 11-year solar cycle (τ) of 1278 years (with a range from 1120 to 1475 years), which is much shorter than the currently widely used value of 3200 years, due to the larger contribution (97.4 %) of the modelled electron density to the total atmospheric loss. The loss of SF6 by reaction with mesospheric metal atoms (Na and K) is far too slow to affect the lifetime. We investigate how this shorter atmospheric lifetime impacts the use of SF6 to derive stratospheric age of air. The age of air derived from this shorter lifetime SF6 tracer is longer by 9 % in polar latitudes at 20 km compared to a passive SF6 tracer. We also present laboratory measurements of the infrared spectrum of SF6 and find good agreement with previous studies. We calculate the resulting radiative forcings and efficiencies to be, on average, very similar to those reported previously. Our values for the 20-, 100- and 500-year global warming potentials are 18 000, 23 800 and 31 300, respectively.

  12. TRENDS IN ATMOSPHERIC SULFUR AND NITROGEN SPECIES IN THE EASTERN UNITED STATES 1989-1995

    EPA Science Inventory

    Emission reductions were mandated in the Clean Air Act Amendments of 1990 with the expectation that they would result in major reductions in the concentrations of atmospherically transported pollutants. This paper investigates the form and magnitude of trends from 1989 to 1995 i...

  13. Laboratory Measurement of the Temperature Dependence of Gaseous Sulfur Dioxide (SO2) Microwave Absorption with Application to the Venus Atmosphere

    NASA Technical Reports Server (NTRS)

    Suleiman, Shady H.; Kolodner, Marc A.; Steffes, Paul G.

    1996-01-01

    High-accuracy laboratory measurements of the temperature dependence of the opacity from gaseous sulfur dioxide (SO2) in a carbon dioxide (CO2) atmosphere at temperatures from 290 to 505 K and at pressures from 1 to 4 atm have been conducted at frequencies of 2.25 GHz (13.3 cm), 8.5 GHz (3.5 cm), and 21.7 GHz (1.4 cm). Based on these absorptivity measurements, a Ben-Reuven (BR) line shape model has been developed that provides a more accurate characterization of the microwave absorption of gaseous S02 in the Venus atmosphere as compared with other formalisms. The developed BR formalism is incorporated into a radiative transfer model. The resulting microwave emission spectrum of Venus is then used to set an upper limit on the disk-averaged abundance of gaseous S02 below the main cloud layer. It is found that gaseous S02 has an upper limit of 150 ppm, which compares well with previous spacecraft in situ measurements and Earth-based radio astronomical observations.

  14. The Effects of Particle Size, Relative Humidity, and Sulfur Dioxide on Iron Solubility in Atmospheric Particulate Matter

    NASA Astrophysics Data System (ADS)

    Cartledge, B. T.; Marcotte, A.; Anbar, A. D.; Herckes, P.; Majestic, B. J.

    2014-12-01

    The current study focuses on studying how iron (Fe) solubility is affected by particle size, relative humidity, and exposure to sulfur dioxide (SO2). Fe, the most abundant transition metal in atmospheric particulate matter, plays a critical role in the atmospheric sulfur cycle and is a micronutrient for phytoplankton in remote regions of the ocean. To mimic oceanic particles, iron-containing minerals (hematite, magnetite, goethite, and illite) were resuspended with sodium chloride and size-segregated on Teflon filters into five different size fractions: 10-2.5 μm, 2.5-1.0 μm, 1.0-0.5 μm, 0.5-0.25 μm, and <0.25 μm. Mineral phases were then exposed to 5 ppm SO2 in air at marine environment humidity (>80%) and arid environment humidity (24%). Trials with no SO2 ­were also performed as comparisons. Total Fe was determined by using microwave-assisted acid digestion and soluble Fe was determined by extracting the samples in a simulated cloud water buffer (pH 4.25, 0.5 mM acetate, 0.5 mM formate, and 0.2 mM ammonium nitrate). Both total and soluble Fe concentrations were determined via inductively-coupled plasma mass spectrometry (ICP-MS). We found that, as particle size decreased, Fe percent solubility increased for hematite, magnetite, and goethite. The percent solubility of Fe in these mineral phases steadily increased from 0.5-10% as particle size decreased. In contrast, the Fe percent solubility in illite was relatively constant for the largest four size fractions but increased dramatically in the smallest size fraction. The percent solubility of Fe in illite ranged from 5-20% as the particle size decreased. Additionally, increased Fe solubility was linked to increased relative humidity with higher percent solubility generally observed in all mineral phases for the samples exposed at the higher humidity. No correlation was observed for the effects of the SO2 on Fe percent solubility. The likely lack of Fe-SO2 interactions were also supported by synchrotron

  15. Multiple oxygen and sulfur isotope compositions of secondary atmospheric sulfate in the city of Wuhan, central China

    NASA Astrophysics Data System (ADS)

    Li, X.; Bao, H.; Zhou, A.; Wang, D.

    2012-12-01

    Secondary atmospheric sulfate (SAS) is the oxidation product and sink for sulfur gases of biological, volcanic, and anthropogenic origins on Earth. SAS can be produced from gas-phase OH-radical oxidation and five aqueous-phase chemical reactions including aqueous-phase S (IV) oxidation reactions by H2O2, O3, oxygen catalyzed by Fe3+ and Mn2+, and methyle hydrogen peroxide and peroxyacetic acid. The tropospheric sulfur oxidation pathway is therefore determined by cloud-water pH, dissolved [Fe2+] or [Mn2+] content, S emission rate, meteorological condition, and other factors. The S isotope composition is a good tracer for the source while the O isotopes, especially the triple O isotope compositions are a good tracer for S oxidation pathway. Jerkins and Bao (2006) provided the first set of multiple stable isotope compositions (δ34S, δ18O and Δ17O) for SAS collected from bulk atmosphere in Baton Rouge in the relatively rural southern USA. Their study revealed a long-tern average Δ17O value of ~+0.7‰ for SAS, and speculated that much of the Earth mid-latitudes may have a similar average SAS Δ17O value. Additional sampling campaign at different sites is necessarily for constructing and testing models on sulfur oxidation and transport in the troposphere. A total of 33 sulfate samples were collected from bulk atmospheric deposition over a 950-day period from May 2009 to December 2011 in the city of Wuhan, Hubei Province, China. Differing from Baton Rouge, Wuhan is an industrial metropolis with a population of 9.8 million and a high particulate matter content (115 μg/m3). It also has a subtropical monsoon climate, with rainwater pH at ~5.3 year-around. The rainwater ion concentrations have seasonal variations, typically low in summer and high in winter. The anions are dominated by SO42-, at an average concentration of 8.5 mg/L. There is little sulfate contribution from sea-salt (SS) sulfate or dusts in Wuhan. The isotopic compositions for bulk atmospheric sulfate

  16. Spatial patterns of atmospheric deposition of nitrogen and sulfur using ion-exchange resin collectors in Rocky Mountain National Park, USA

    NASA Astrophysics Data System (ADS)

    Clow, David W.; Roop, Heidi A.; Nanus, Leora; Fenn, Mark E.; Sexstone, Graham A.

    2015-01-01

    Lakes and streams in Class 1 wilderness areas in the western United States (U.S.) are at risk from atmospheric deposition of nitrogen (N) and sulfur (S), and protection of these resources is mandated under the Federal Clean Air Act and amendments. Assessment of critical loads, which are the maximum exposure to pollution an area can receive without adverse effects on sensitive ecosystems, requires accurate deposition estimates. However, deposition is difficult and expensive to measure in high-elevation wilderness, and spatial patterns in N and S deposition in these areas remain poorly quantified. In this study, ion-exchange resin (IER) collectors were used to measure dissolved inorganic N (DIN) and S deposition during June 2006-September 2007 at approximately 20 alpine/subalpine sites spanning the Continental Divide in Rocky Mountain National Park. Results indicated good agreement between deposition estimated from IER collectors and commonly used wet + dry methods during summer, but poor agreement during winter. Snowpack sampling was found to be a more accurate way of quantifying DIN and S deposition during winter. Summer DIN deposition was significantly greater on the east side of the park than on the west side (25-50%; p ≤ 0.03), consistent with transport of pollutants to the park from urban and agricultural areas to the east. Sources of atmospheric nitrate (NO3-) were examined using N isotopes. The average δ15N of NO3- from IER collectors was 3.5‰ higher during winter than during summer (p < 0.001), indicating a seasonal shift in the relative importance of regional NOx sources, such as coal combustion and vehicular sources of atmospheric NO3-. There were no significant differences in δ15N of NO3- between east and west sides of the park during summer or winter (p = 0.83), indicating that the two areas may have similar sources of atmospheric NO3-. Results from this study indicate that a combination of IER collectors and snowpack sampling can be used to

  17. Spatial patterns of atmospheric deposition of nitrogen and sulfur using ion-exchange resin collectors in Rocky Mountain National Park, USA

    USGS Publications Warehouse

    Clow, David W.; Roop, Heidi; Nanus, Leora; Fenn, Mark; Sexstone, Graham A.

    2015-01-01

    Lakes and streams in Class 1 wilderness areas in the western United States (U.S.) are at risk from atmospheric deposition of nitrogen (N) and sulfur (S), and protection of these resources is mandated under the Federal Clean Air Act and amendments. Assessment of critical loads, which are the maximum exposure to pollution an area can receive without adverse effects on sensitive ecosystems, requires accurate deposition estimates. However, deposition is difficult and expensive to measure in high-elevation wilderness, and spatial patterns in N and S deposition in these areas remain poorly quantified. In this study, ion-exchange resin (IER) collectors were used to measure dissolved inorganic N (DIN) and S deposition during June 2006–September 2007 at approximately 20 alpine/subalpine sites spanning the Continental Divide in Rocky Mountain National Park. Results indicated good agreement between deposition estimated from IER collectors and commonly used wet + dry methods during summer, but poor agreement during winter. Snowpack sampling was found to be a more accurate way of quantifying DIN and S deposition during winter. Summer DIN deposition was significantly greater on the east side of the park than on the west side (25–50%; p ≤ 0.03), consistent with transport of pollutants to the park from urban and agricultural areas to the east. Sources of atmospheric nitrate (NO3−) were examined using N isotopes. The average δ15N of NO3− from IER collectors was 3.5‰ higher during winter than during summer (p < 0.001), indicating a seasonal shift in the relative importance of regional NOxsources, such as coal combustion and vehicular sources of atmospheric NO3−. There were no significant differences in δ15N of NO3− between east and west sides of the park during summer or winter (p = 0.83), indicating that the two areas may have similar sources of atmospheric NO3−. Results from this study indicate that a combination of IER collectors and snowpack

  18. Sulfur in the Early Martian Atmosphere Revisited: Experiments with a 3-D Global Climate Model

    NASA Astrophysics Data System (ADS)

    Kerber, L.; Forget, F.; Wordsworth, R.

    2013-09-01

    Data returned from the surface of Mars during the 1970s revealed intriguing geological evidence for a warmer and wetter early martian climate. Dendritic valley networks were discovered by Mariner 9 on ancient Noachian terrain [1], indicating that liquid water had flowed across the surface in the distant past. Since this time, geological investigations into early Martian history have attempted to ascertain the nature and level of activity of the early Martian hydrological cycle [e.g. 2-5] while atmospheric modeling efforts have focused on how the atmosphere could be warmed to temperatures great enough to sustain such activity [see 6-7 for reviews]. Geological and spectroscopic investigations have refined the history and chronology of Noachian Mars over time, and circulation of liquid water has been invoked to explain several spatially and temporally distinct morphological and chemical signatures found in the geological record. Detections of iron and magnesium-rich clays are widespread in the oldest Martian terrains, suggesting a period of pH-neutral aqueous alteration [e.g., 8]. Valley network incision also took place during the Noachian period [9]. Some chains of river valleys and craters lakes extend for thousands of kilometers, suggesting temperatures at least clement enough for sustained ice-covered flow [3,10]. The commencement of valley network incision is not well constrained, but the period of Mg/Fe clay formation appears to have ended before the termination of valley network formation, as the visible fluvial systems appear to have remobilized existing clays rather than forming them [5,8]. There is also evidence that the cessation of valley network formation was abrupt [11]. Towards the end of the Noachian, erosion rates appear to have been significantly higher than during subsequent periods, a process that has also been attributed to aqueous processes [12]. A period of sulfate formation followed, likely characterized by acidic, evaporitic playa environments

  19. Effects of background gas on sulfur hexafluoride removal by atmospheric dielectric barrier discharge plasma

    NASA Astrophysics Data System (ADS)

    Zhang, Xiaoxing; Xiao, Hanyan; Hu, Xiongxiong; Gui, Yingang

    2016-11-01

    The effects of background gases (He, Ar, N2 and air) on SF6 removal in a dielectric barrier reactor were investigated at atmospheric pressure. A comparison among these background gases was performed in terms of discharge voltage, discharge power, mean electron energy, electron density, removal efficiency and energy yield for the destruction of SF6. Results showed that the discharge voltage of He and Ar was lower than that of N2 and air, but the difference of their discharge power was small. Compared with three other background gases, Ar had a relatively superior destruction and removal rate and energy yield since the mean electron energy and electron density in SF6/H2O/Ar plasma were both maintained at a high level. Complete removal of 2% SF6 could be achieved at a discharge power of 48.86 W with Ar and the corresponding energy yield can reach 4.8 g/kWh.

  20. Atmospheric wet deposition of nitrogen and sulfur in the agroecosystem in developing and developed areas of Southeastern China

    NASA Astrophysics Data System (ADS)

    Cui, Jian; Zhou, Jing; Peng, Ying; He, Yuanqiu; Yang, Hao; Mao, Jingdong; Zhang, Mingli; Wang, Yanhua; Wang, Shuwei

    2014-06-01

    Atmospheric nitrogen (N) and sulfur (S) deposition is a significant and growing issue for ecological environment in many parts of the world such as China. However, the study on atmospheric deposition, especially N deposition, is still at the initial stage and usually neglected in agro-ecosystems. To assess the characteristics of N and S wet deposition in agro-ecosystems, we selected Yingtan Station (YTS) located in the developing area and Changshu Station (CSS) in the developed area as typical, agricultural study sites in Southeastern China during 2010-2011. In the two areas, the total N and S wet deposition were in ranges of 30.49-37.37 kg ha-1 year-1 N and 56.02-59.06 kg ha-1 year-1 S, respectively, surpassing their corresponding critical loads in China. The annual means of NH4+-N, NO3--N and dissolved organic N (DON) deposition contributed 49.6%, 26.4% and 24.0% of the total deposition, respectively. Similar total N and S deposition data were observed in the two sites, but their N species, especially DON, were different due to different numbers of slaughter pigs and types of N fertilizers applied. In conclusion, DON was identified as an important contributor to the total N deposition and should also be monitored in the future. Such high N and S deposition would deteriorate agroecosystems in Southeastern China. Related political measures on livestock industries, managements of motor vehicles and technologies of coal and oil combustion should be improved timely and implemented effectively for reducing the regional N emission and deposition in the future.

  1. Atmospheric So2 Emissions Since the Late 1800s Change Organic Sulfur Forms in Humic Substance Extracts of Soils

    SciTech Connect

    Lehmann,J.; Solomon, D.; Zhao, F.; McGrath, S.

    2008-01-01

    Atmospheric SO2 emissions in the UK and globally increased 6- and 20-fold, respectively, from the mid-1800s to the 1960s resulting in increased S deposition, acid rain, and concurrent acidification of terrestrial and aquatic ecosystems. Structural analyses using synchrotron-based X-ray near-edge spectroscopy (XANES) on humic substance extracts of archived samples from the Rothamsted Park Grass Experiment reveal a significant (R2 = -0.58; P < 0.05; N = 7) shift in soil organic sulfur (S) forms, from reduced to more oxidized organic S between 1876 and 1981, even though soil total S contents remained relatively constant. Over the last 30 years, a decrease in emissions and consequent S deposition has again corresponded with a change of organic S structures of humic extractsreverting in the direction of their early industrial composition. However, the observed reversal lagged behind reductions in emissions by 19 years, which was computed using cross correlations between time series data (R2 = 0.66; P = 0.0024; N = 11). Presently, the ratio of oxidized-to-reduced organic S in humic substance extracts is nearly double that of early industrial times at identical SO2 emission loads. The significant and persistent structural changes of organic S in humic substances as a response to SO2 emissions and S deposition may have effects on recuperation of soils and surface waters from acidification.

  2. Effect of ions on sulfuric acid-water binary particle formation: 1. Theory for kinetic- and nucleation-type particle formation and atmospheric implications

    NASA Astrophysics Data System (ADS)

    Merikanto, Joonas; Duplissy, Jonathan; Määttänen, Anni; Henschel, Henning; Donahue, Neil M.; Brus, David; Schobesberger, Siegfried; Kulmala, Markku; Vehkamäki, Hanna

    2016-02-01

    We derive a version of Classical Nucleation Theory normalized by quantum chemical results on sulfuric acid-water hydration to describe neutral and ion-induced particle formation in the binary sulfuric acid-water system. The theory is extended to treat the kinetic regime where the nucleation free energy barrier vanishes at high sulfuric acid concentrations or low temperatures. In the kinetic regime particle formation rates become proportional to sulfuric acid concentration to second power in the neutral system or first power in the ion-induced system. We derive simple general expressions for the prefactors in kinetic-type and activation-type particle formation calculations applicable also to more complex systems stabilized by other species. The theory predicts that the binary water-sulfuric acid system can produce strong new particle formation in the free troposphere both through barrier crossing and through kinetic pathways. At cold stratospheric and upper free tropospheric temperatures neutral formation dominates the binary particle formation rates. At midtropospheric temperatures the ion-induced pathway becomes the dominant mechanism. However, even the ion-induced binary mechanism does not produce significant particle formation in warm boundary layer conditions, as it requires temperatures below 0°C to take place at atmospheric concentrations. The theory successfully reproduces the characteristics of measured charged and neutral binary particle formation in CERN CLOUD3 and CLOUD5 experiments, as discussed in a companion paper.

  3. Spectral Dark Subtraction: A MODTRAN-Based Algorithm for Estimating Ground Reflectance without Atmospheric Information

    NASA Technical Reports Server (NTRS)

    Freedman, Ellis; Ryan, Robert; Pagnutti, Mary; Holekamp, Kara; Gasser, Gerald; Carver, David; Greer, Randy

    2007-01-01

    Spectral Dark Subtraction (SDS) provides good ground reflectance estimates across a variety of atmospheric conditions with no knowledge of those conditions. The algorithm may be sensitive to errors from stray light, calibration, and excessive haze/water vapor. SDS seems to provide better estimates than traditional algorithms using on-site atmospheric measurements much of the time.

  4. Estimation of Atmospheric Mixing Layer Height from radiosonde data

    NASA Astrophysics Data System (ADS)

    Wang, X.; Wang, K.

    2013-12-01

    Mixing layer is the lowest layer of the troposphere where surface turbulence can reach during the daytime. Mixing layer height (MLH) is an important parameter for understanding the transport process, air pollution, weather and climate change. MLH can be determined from the radiosonde profiles of relative humidity (RH), specific humidity (q), potential temperature (θ) and atmospheric refractivity (N) by searching for the strongest gradients of these parameters within a specific height above the surface. However, substantially different MLHs have been found from different parameters. The occurrence of cloud impacts on MLHs derived in two ways: (1) clouds impact the measurements of θ and RH, resulting in spurious MLHs derived by θ and RH, (2) clouds may amplify or depress turbulence, that is MLH can be at cloud top or cloud base when it occurs. However, MLHs determined by existing methods can generally be at cloud top. To solve these problems, we propose a method to estimate MLH by integrating the information of θ, RH, q, N and discriminating different cloud impacts on MLH. We apply this method to high vertical resolution (~30 m) radiosonde data collected at the 79 stations over North America during the period of 1998 to 2008 released by the Stratospheric Processes and their Role in Climate Data Center. The results show good agreement with those from N as the information of temperature and humidity contained in N, however the impact of clouds including in the new method has increased the reliability of MLH. The new results show good agreement with independent MLH determined from Lidar observations. MLH over the North America is 1647×323 meter with a strong east-west gradient, higher MLH (generally greater than 1800 m) over the Midwest America and lower MLH (less than 1300 m) over Alaska and west coast of America. The scatter plot of climatological MLHnew with MLHθ, MLHRH, MLHq, MLHN and MLHint for the period of 1998 to 2008. Pattern of climatological MLH of our

  5. Target loads of atmospheric sulfur deposition for the protection and recovery of acid-sensitive streams in the Southern Blue Ridge Province.

    PubMed

    Sullivan, Timothy J; Cosby, Bernard J; Jackson, William A

    2011-11-01

    An important tool in the evaluation of acidification damage to aquatic and terrestrial ecosystems is the critical load (CL), which represents the steady-state level of acidic deposition below which ecological damage would not be expected to occur, according to current scientific understanding. A deposition load intended to be protective of a specified resource condition at a particular point in time is generally called a target load (TL). The CL or TL for protection of aquatic biota is generally based on maintaining surface water acid neutralizing capacity (ANC) at an acceptable level. This study included calibration and application of the watershed model MAGIC (Model of Acidification of Groundwater in Catchments) to estimate the target sulfur (S) deposition load for the protection of aquatic resources at several future points in time in 66 generally acid-sensitive watersheds in the southern Blue Ridge province of North Carolina and two adjoining states. Potential future change in nitrogen leaching is not considered. Estimated TLs for S deposition ranged from zero (ecological objective not attainable by the specified point in time) to values many times greater than current S deposition depending on the selected site, ANC endpoint, and evaluation year. For some sites, one or more of the selected target ANC critical levels (0, 20, 50, 100μeq/L) could not be achieved by the year 2100 even if S deposition was reduced to zero and maintained at that level throughout the simulation. Many of these highly sensitive streams were simulated by the model to have had preindustrial ANC below some of these target values. For other sites, the watershed soils contained sufficiently large buffering capacity that even very high sustained levels of atmospheric S deposition would not reduce stream ANC below common damage thresholds.

  6. Coupled Inertial Navigation and Flush Air Data Sensing Algorithm for Atmosphere Estimation

    NASA Technical Reports Server (NTRS)

    Karlgaard, Christopher D.; Kutty, Prasad; Schoenenberger, Mark

    2016-01-01

    This paper describes an algorithm for atmospheric state estimation based on a coupling between inertial navigation and flush air data-sensing pressure measurements. The navigation state is used in the atmospheric estimation algorithm along with the pressure measurements and a model of the surface pressure distribution to estimate the atmosphere using a nonlinear weighted least-squares algorithm. The approach uses a high-fidelity model of atmosphere stored in table-lookup form, along with simplified models propagated along the trajectory within the algorithm to aid the solution. Thus, the method is a reduced-order Kalman filter in which the inertial states are taken from the navigation solution and atmospheric states are estimated in the filter. The algorithm is applied to data from the Mars Science Laboratory entry, descent, and landing from August 2012. Reasonable estimates of the atmosphere are produced by the algorithm. The observability of winds along the trajectory are examined using an index based on the observability Gramian and the pressure measurement sensitivity matrix. The results indicate that bank reversals are responsible for adding information content. The algorithm is applied to the design of the pressure measurement system for the Mars 2020 mission. A linear covariance analysis is performed to assess estimator performance. The results indicate that the new estimator produces more precise estimates of atmospheric states than existing algorithms.

  7. Organic Sulfur Gas Production in Sulfidic Caves

    NASA Astrophysics Data System (ADS)

    Stern, L. A.; Engel, A. S.; Bennett, P. C.

    2001-12-01

    Lower Kane Cave, Big Horn Basin, WY, permits access to an environment where anaerobic sulfide-rich groundwater meets the aerobic vadose zone. At this interface microorganisms thrive on diverse metabolic pathways including autotrophic sulfur oxidation, sulfate reduction, and aerobic heterotrophy. Springs introduce groundwater rich in H2S to the cave where it both degasses into the cave atmosphere and is used by chemautotrophic sulfur oxidizing bacteria in the cave spring and stream habitat. The cave atmosphere in the immediate vicinity of the springs has elevated levels of CO2, H2S and methane, mirroring the higher concentration of H2S and methane in the spring water. The high CO2 concentrations are attenuated toward the two main sources of fresh air, the cave entrance and breathing holes at the rear of the cave. Conventional toxic gas monitors permit estimations of H2S concentrations, but they have severe cross sensitivity with other reduced sulfur gases, and thus are inadequate for characterization of sulfur cave gases. However employment of a field-based GC revealed elevated concentrations of carbonyl sulfide in cave atmosphere. Cultures of microorganisms collected from the cave optimized for enriching fermenters and autotrophic and heterophic sulfate reducing bacteria each produced carbonyl sulfide suggesting a biogenic in origin of the COS in addition to H2S. Enrichment cultures also produced methanethiol (methyl mercaptan) and an additional as yet undetermined volatile organic sulfur compound. In culture, the organo-sulfur compounds were less abundant than H2S, whereas in the cave atmosphere the organo-sulfur compounds were the dominant sulfur gases. Thus, these organo-sulfur gases may prove to be important sources of both reduced sulfur and organic carbon to microorganisms living on the cave wall in a subaerial habitat. Moreover groundwater has not yet been recognized as a source of sulfur gases to the atmosphere, but with the abundance of sulfidic

  8. The role of crystallization-driven exsolution on the sulfur mass balance in volcanic arc magmas

    NASA Astrophysics Data System (ADS)

    Su, Y.; Huber, Christian; Bachmann, Olivier; Zajacz, Zoltán.; Wright, Heather; Vazquez, Jorge

    2016-08-01

    The release of large amounts of sulfur to the stratosphere during explosive eruptions affects the radiative balance in the atmosphere and consequentially impacts climate for up to several years after the event. Quantitative estimations of the processes that control the mass balance of sulfur between melt, crystals, and vapor bubbles is needed to better understand the potential sulfur yield of individual eruption events and the conditions that favor large sulfur outputs to the atmosphere. The processes that control sulfur partitioning in magmas are (1) exsolution of volatiles (dominantly H2O) during decompression (first boiling) and during isobaric crystallization (second boiling), (2) the crystallization and breakdown of sulfide or sulfate phases in the magma, and (3) the transport of sulfur-rich vapor (gas influx) from deeper unerupted regions of the magma reservoir. Vapor exsolution and the formation/breakdown of sulfur-rich phases can all be considered as closed-system processes where mass balance arguments are generally easier to constrain, whereas the contribution of sulfur by vapor transport (open system process) is more difficult to quantify. The ubiquitous "excess sulfur" problem, which refers to the much higher sulfur mass released during eruptions than what can be accounted for by amount of sulfur originally dissolved in erupted melt, as estimated from melt inclusion sulfur concentrations (the "petrologic estimate"), reflects the challenges in closing the sulfur mass balance between crystals, melt, and vapor before and during a volcanic eruption. In this work, we try to quantify the relative importance of closed- and open-system processes for silicic arc volcanoes using kinetic models of sulfur partitioning during exsolution. Our calculations show that crystallization-induced exsolution (second boiling) can generate a significant fraction of the excess sulfur observed in crystal-rich arc magmas. This result does not negate the important role of vapor

  9. Uncertainties in BC Estimations: the Role of Atmospheric Processes

    NASA Astrophysics Data System (ADS)

    Vignati, E.; Kloster, S.; Koch, D.; Bauer, S. E.; Dentener, F.; Bond, T.; Sun, H.

    2006-12-01

    Modelling physical and chemical processes involving aerosol particles remains a large source of uncertainties. To characterize the range of uncertainty in these processes on atmospheric BC concentrations, three global models (CTM-TM5, GCM ECHAM5-HAM and GISS GCM) were run using identical BC, particulate organic matter and SO2 emission inventories provided by IIASA for the year 2000. The first two models have the same aerosol dynamic module, while TM5 is also run with a bulk aerosol scheme; the GISS model uses both bulk aerosol and a method of moments aerosol microphysical schemes. We can thus specifically assess the differences in predicted BC concentrations from using the bulk approach and the two microphysical schemes. By comparing the modeled concentrations with an extensive data set of observations, distinguished by measurement methodology, season and region, we will critically evaluate the benefit of using microphysical schemes to simulate the atmospheric BC cycle.

  10. Estimation of the efficiency of atmospheric ozone aerosol sink

    NASA Astrophysics Data System (ADS)

    Sirota, Vitaly

    1993-11-01

    The interaction of ozone with oxides occurring in aerosols (Al2O3, ZnO, MgO, TiO2) at temperatures 22 divided by -63.5 degree(s)C was provided. Laboratory experiments have shown that activity of investigated oxides with respect to ozone grows under irradiation of their surface. To calculate correctly atmospheric ozone aerosol sink one must take account of both heterogeneous processes proceeding without action of light and photocatalytic ones.

  11. Spatial variation of biogenic sulfur in the south Yellow Sea and the East China Sea during summer and its contribution to atmospheric sulfate aerosol.

    PubMed

    Zhang, Sheng-Hui; Yang, Gui-Peng; Zhang, Hong-Hai; Yang, Jian

    2014-08-01

    Spatial distributions of biogenic sulfur compounds including dimethylsulfide (DMS), dissolved and particulate dimethylsulfoniopropionate (DMSPd and DMSPp) were investigated in the South Yellow Sea (SYS) and the East China Sea (ECS) in July 2011. The concentrations of DMS and DMSPp were significantly correlated with the levels of chlorophyll a in the surface water. Simultaneously, relatively high ratio values of DMSP/chlorophyll a and DMS/chlorophyll a occurred in the areas where the phytoplankton community was dominated by dinoflagellates. The DMSPp and chlorophyll a size-fractionation showed that larger nanoplankton (5-20 μm) was the most important producer of DMSPp in the study area. The vertical profiles of DMS and DMSP were characterized by a maximum at the upper layer and the bottom concentrations were also relatively higher compared with the overlying layer of the bottom. In addition, a positive linear correlation was observed between dissolved dimethylsulfoxide (DMSOd) and DMS concentrations in the surface waters. The sea-to-air fluxes of DMS in the study area were estimated to be from 0.03 to 102.35 μmol m(-2) d(-1) with a mean of 16.73 μmol m(-2) d(-1) and the contribution of biogenic non-sea-salt SO4(2-) (nss-SO4(2-)) to the measured total nss-SO4(2-) in the atmospheric aerosol over the study area varied from 1.42% to 30.98%, with an average of 8.2%.

  12. Equipment Design and Cost Estimation for Small Modular Biomass Systems, Synthesis Gas Cleanup, and Oxygen Separation Equipment; Task 2.3: Sulfur Primer

    SciTech Connect

    Nexant Inc.

    2006-05-01

    This deliverable is Subtask 2.3 of Task 2, Gas Cleanup Design and Cost Estimates, of NREL Award ACO-5-44027, ''Equipment Design and Cost Estimation for Small Modular Biomass Systems, Synthesis Gas Cleanup and Oxygen Separation Equipment''. Subtask 2.3 builds upon the sulfur removal information first presented in Subtask 2.1, Gas Cleanup Technologies for Biomass Gasification by adding additional information on the commercial applications, manufacturers, environmental footprint, and technical specifications for sulfur removal technologies. The data was obtained from Nexant's experience, input from GTI and other vendors, past and current facility data, and existing literature.

  13. Coupled Inertial Navigation and Flush Air Data Sensing Algorithm for Atmosphere Estimation

    NASA Technical Reports Server (NTRS)

    Karlgaard, Christopher D.; Kutty, Prasad; Schoenenberger, Mark

    2015-01-01

    This paper describes an algorithm for atmospheric state estimation that is based on a coupling between inertial navigation and flush air data sensing pressure measurements. In this approach, the full navigation state is used in the atmospheric estimation algorithm along with the pressure measurements and a model of the surface pressure distribution to directly estimate atmospheric winds and density using a nonlinear weighted least-squares algorithm. The approach uses a high fidelity model of atmosphere stored in table-look-up form, along with simplified models of that are propagated along the trajectory within the algorithm to provide prior estimates and covariances to aid the air data state solution. Thus, the method is essentially a reduced-order Kalman filter in which the inertial states are taken from the navigation solution and atmospheric states are estimated in the filter. The algorithm is applied to data from the Mars Science Laboratory entry, descent, and landing from August 2012. Reasonable estimates of the atmosphere and winds are produced by the algorithm. The observability of winds along the trajectory are examined using an index based on the discrete-time observability Gramian and the pressure measurement sensitivity matrix. The results indicate that bank reversals are responsible for adding information content to the system. The algorithm is then applied to the design of the pressure measurement system for the Mars 2020 mission. The pressure port layout is optimized to maximize the observability of atmospheric states along the trajectory. Linear covariance analysis is performed to assess estimator performance for a given pressure measurement uncertainty. The results indicate that the new tightly-coupled estimator can produce enhanced estimates of atmospheric states when compared with existing algorithms.

  14. Estimating spatial veriability in atmospheric properties over remotely sensed land-surface conditions

    Technology Transfer Automated Retrieval System (TEKTRAN)

    This paper investigates the spatial relationships between land-surface fluxes and near-surface atmospheric properties (AP), and the potential errors in flux estimation due to homogeneous atmospheric inputs over heterogeneous landscapes. A Large Eddy Simulation (LES) model is coupled to a surface ene...

  15. Sulfur mass loading of the atmosphere from volcanic eruptions: Calibration of the ice core record on basis of sulfate aerosol deposition in polar regions from the 1982 El Chichon eruption. Semiannual progress report

    SciTech Connect

    Sigurdsson, H.; Laj, P.

    1990-09-01

    Major volcanic eruptions disperse large quantities of sulfur compound throughout the Earth's atmosphere. The sulfuric acid aerosols resulting from such eruptions are scavenged by snow within the polar regions and appear in polar ice cores as elevated acidity layers. Glacio-chemical studies of ice cores can, thus, provide a record of past volcanism, as well as the means for understanding the fate of volcanic sulfur in the atmosphere. The primary objectives of this project are to study the chemistry and physical properties of volcanic fallout in a Greenland Ice Core in order to evaluate the impact of the volcanic gases on the atmospheric chemistry and the total atmospheric mass of volcanic aerosols emitted by major volcanic eruptions. The authors propose to compare the ice core record to other atmospheric records performed during the last 10 years to investigate transport and deposition of volcanic materials.

  16. Sulfur mass loading of the atmosphere from volcanic eruptions: Calibration of the ice core record on basis of sulfate aerosol deposition in polar regions from the 1982 El Chichon eruption

    NASA Technical Reports Server (NTRS)

    Sigurdsson, Haraldur; Laj, Paolo

    1990-01-01

    Major volcanic eruptions disperse large quantities of sulfur compound throughout the Earth's atmosphere. The sulfuric acid aerosols resulting from such eruptions are scavenged by snow within the polar regions and appear in polar ice cores as elevated acidity layers. Glacio-chemical studies of ice cores can, thus, provide a record of past volcanism, as well as the means for understanding the fate of volcanic sulfur in the atmosphere. The primary objectives of this project are to study the chemistry and physical properties of volcanic fallout in a Greenland Ice Core in order to evaluate the impact of the volcanic gases on the atmospheric chemistry and the total atmospheric mass of volcanic aerosols emitted by major volcanic eruptions. We propose to compare the ice core record to other atmospheric records performed during the last 10 years to investigate transport and deposition of volcanic materials.

  17. Stellar atmospheric parameter estimation using Gaussian process regression

    NASA Astrophysics Data System (ADS)

    Bu, Yude; Pan, Jingchang

    2015-02-01

    As is well known, it is necessary to derive stellar parameters from massive amounts of spectral data automatically and efficiently. However, in traditional automatic methods such as artificial neural networks (ANNs) and kernel regression (KR), it is often difficult to optimize the algorithm structure and determine the optimal algorithm parameters. Gaussian process regression (GPR) is a recently developed method that has been proven to be capable of overcoming these difficulties. Here we apply GPR to derive stellar atmospheric parameters from spectra. Through evaluating the performance of GPR on Sloan Digital Sky Survey (SDSS) spectra, Medium resolution Isaac Newton Telescope Library of Empirical Spectra (MILES) spectra, ELODIE spectra and the spectra of member stars of galactic globular clusters, we conclude that GPR can derive stellar parameters accurately and precisely, especially when we use data preprocessed with principal component analysis (PCA). We then compare the performance of GPR with that of several widely used regression methods (ANNs, support-vector regression and KR) and find that with GPR it is easier to optimize structures and parameters and more efficient and accurate to extract atmospheric parameters.

  18. Modelling the atmospheric boundary layer for remotely sensed estimates of daily evaporation

    NASA Technical Reports Server (NTRS)

    Gurney, R. J.; Blyth, K.; Camillo, P. J.

    1984-01-01

    An energy and moisture balance model of the soil surface was used to estimate daily evaporation from wheat and barley fields in West Germany. The model was calibrated using remotely sensed surface temperature estimates. Complete atmospheric boundary layer models are difficult to use because of the number of parameters involved and a simplified model was used here. The resultant evaporation estimates were compared to eddy correlation evaporation estimates and good agreement was found.

  19. Sulfur, Chlorine and Fluorine Degassing and Atmospheric Loading by the Roza eruption, Columbia River Basalt Group, Washington

    NASA Technical Reports Server (NTRS)

    Thordarson, Th.; Self, S

    1996-01-01

    In this study we attempt to quantify the amount of S, Cl and F released by the 1300 cu km Roza member (approximately 14.7 Ma) of the Columbia River Basalt Group, which was produced by a moderate-size flood basalt eruption in the mid-Miocene. Our results are the first indication of the potential atmospheric SO2 yield from a flood basalt eruption, and indicate the mechanism by which flood basalt eruptions may have seriously affected the environment. Glass inclusions in phenocrysts and quenched glass in products from various stages of the eruption were analyzed for concentrations of S, Cl and F and major elements. Glass inclusions contain 1965 +/- 110 ppm S, 295 +/- 65 ppm Cl and 1310 +/- 110 ppm F. Groundmass glass of Roza dike selvages contains considerably lower concentrations: 1110 +/- 90 ppm S, 245 +/- 30 ppm Cl and 1020 +/- 25 ppm F. Scoria clasts from near vent deposits contain 665 +/- 75 ppm S, 175 +/- 5 ppm Cl and 950 +/- 20 ppm F, and the groundmass glass of lava selvages contains 520 +/- 30 ppm S, 190 +/- 30 ppm Cl and 890 +/- 55 ppm F. In crystalline lava, the concentrations are 195 ppm S, 100 ppm Cl and 830 ppm F. Volatile element concentrations in these samples represent the progress of degassing through the eruption and can be used to estimate the potential amount of the volatiles S, Cl and F released by the magma into the atmosphere, as well as to evaluate the amount liberated by various phases of the eruption. The total amount of volatiles released by the Roza eruption is estimated to have been approximately 12,420 MtSO2, approximately 710 MtHCI and approximately 1780 MtHF. The Roza magma liberated approximately 9620 MtSO, (77% of the total volatile mass released), approximately 400 MtHCI (56%) and approximately 1450 MtHF (81%) at the vents and lofted by the eruption columns to altitudes of 7-13 km. Degassing of the lava is estimated to have released an additional approximately 2810 MtSO2, approximately 310 MtHCI and approximately 330 MtHF. The Roza

  20. Hydrogen Sulfide Sequestration and Storage in Geothermal System: New Mitigation Strategy to Reduce H2S from the Atmosphere and Detect its Mineralization with Multiple Sulfur Isotopic Systematics

    NASA Astrophysics Data System (ADS)

    Marieni, C.; Stefansson, A.; Gudbrandsson, S.; Gunnarsson, I.; Aradottir, E. S.; Gunnarsson Robin, J.; Ono, S.

    2015-12-01

    Hydrogen sulfide (H2S) is one of the major components in geothermal fluids and is commonly emitted into the atmosphere from geothermal power plants causing potential environmental problems. Among several mitigation methods proposed to reduce the H2S emissions, is H2S sequestration into geothermal systems. Reykjavík Energy is undertaking a pilot project at Hellisheidi geothermal system (SW Iceland) called Sulfix project where H2S is being injected into the geothermal reservoir for permanent sequestration into pyrite. The SulFix project started its operation in June 2014: the soluble geothermal gases are dissolved in geothermal waste water, and injected at 8 bars into the high temperature reservoir (>200˚C) at 750 m below the wellhead. The reactions involving sulfur in the geothermal reservoir may be traced using sulfur fluid chemistry and multiple sulfur isotope systematics (32S, 33S, 34S and 36S), including mixing between the reservoir geothermal fluid and the injection fluid, sulfide mineralization and oxidation of sulfide to sulfate. In this study we investigated the multiple sulfur isotope systematics upon sulfide mineralization under geothermal conditions. High temperature flow through experiments were carried out in basaltic glass at 200-250°C and ~5 mmol/kg H2S to study the fluid-rock interaction. The results indicate that the sulfide mineralization occurs rapidly under geothermal conditions, highlighting the leaching rate of iron from the basaltic glass as the mineralization rate determining factor. Moreover, the formation of sulfide may be traced using the δ34S-Δ33S relationship in the fluids and pyrite formation - for example to determine if non-reactive mixing between the injection fluids and reservoir fluids occurs at Hellisheidi. The experimental results have been further supported by geochemical modeling involving multiple sulfur isotope fractionation between aqueous sulfide species and rocks upon basalt dissolution and secondary pyrite formation.

  1. Atmospheric evolution of sulfur emissions from Kı̅lauea: real-time measurements of oxidation, dilution, and neutralization within a volcanic plume.

    PubMed

    Kroll, Jesse H; Cross, Eben S; Hunter, James F; Pai, Sidhant; Wallace, Lisa M M; Croteau, Philip L; Jayne, John T; Worsnop, Douglas R; Heald, Colette L; Murphy, Jennifer G; Frankel, Sheila L

    2015-04-07

    The high atmospheric concentrations of toxic gases, particulate matter, and acids in the areas immediately surrounding volcanoes can have negative impacts on human and ecological health. To better understand the atmospheric fate of volcanogenic emissions in the near field (in the first few hours after emission), we have carried out real-time measurements of key chemical components of the volcanic plume from Kı̅lauea on the Island of Hawai'i. Measurements were made at two locations, one ∼ 3 km north-northeast of the vent and the other 31 km to the southwest, with sampling at each site spanning a range of meteorological conditions and volcanic influence. Instrumentation included a sulfur dioxide monitor and an Aerosol Chemical Speciation Monitor, allowing for a measurement of the partitioning between the two major sulfur species (gas-phase SO2 and particulate sulfate) every 5 min. During trade wind conditions, which sent the plume toward the southwest site, sulfur partitioning exhibited a clear diurnal pattern, indicating photochemical oxidation of SO2 to sulfate; this enabled the quantitative determination of plume age (5 h) and instantaneous SO2 oxidation rate (2.4 × 10(-6) s(-1) at solar noon). Under stagnant conditions near the crater, the extent of SO2 oxidation was substantially higher, suggesting faster oxidation. The particles within the plume were extremely acidic, with pH values (controlled largely by ambient relative humidity) as low as -0.8 and strong acidity (controlled largely by absolute sulfate levels) up to 2200 nmol/m(3). The high variability of sulfur partitioning and particle composition underscores the chemically dynamic nature of volcanic plumes, which may have important implications for human and ecological health.

  2. Using CFCs and Sulfur Hexafluoride to Improve Estimates of Ventilation Rate Changes and Anthropogenic CO2 Uptake Along CLIVAR Repeat Hydrography Sections

    NASA Astrophysics Data System (ADS)

    Bullister, J. L.; Sonnerup, R. E.; Warner, M. J.

    2008-12-01

    A number of key hydrographic sections sampled in the 1990s as part of the World Ocean Circulation Experiment (WOCE) are being re-occupied at approximately decadal intervals as part of the CLIVAR Repeat Hydrography Program. Measurements of a number of physical and chemical properties are made at full depth, closely spaced (nominally 30 nautical mile) CTD/rosette stations, with water samples collected at between 24 and 36 depths per station. Among the central goals of the program are the detection of changes in ventilation, carbon uptake and storage, dissolved oxygen and water properties on decadal time scales. Repeat measurements of dissolved chlorofluorocarbon (CFC) CFC-11 and CFC-12 concentrations show significant decadal increases. Water mass ages derived from CFCs (pCFC ages) also show substantial changes (typically increases) with time along the repeat sections. Simple models indicate that much of the observed pCFC age increases are due to the impacts of mixing in the ocean interior. Measurements of sulfur hexafluoride (SF6), a transient tracer that has been rapidly increasing in the atmosphere during the past several decades, have been included along with CFCs on some recent CLIVAR repeat sections. Because the atmospheric history of SF6 differs substantially from that of the CFCs, concurrent SF6 and CFC measurements can be used to help diagnose the impacts of mixing on pCFC ages and on decadal changes in pCFC ages. We are exploiting this twin-tracer strategy in an attempt to improve estimates of ventilation rate changes and anthropogenic CO2 uptake rates along the CLIVAR repeat sections.

  3. Sulfur Earth

    NASA Astrophysics Data System (ADS)

    de Jong, B. H.

    2007-12-01

    Variations in surface tension affect the buoyancy of objects floating in a liquid. Thus an object floating in water will sink deeper in the presence of dishwater fluid. This is a very minor but measurable effect. It causes for instance ducks to drown in aqueous solutions with added surfactant. The surface tension of liquid iron is very strongly affected by the presence of sulfur which acts as a surfactant in this system varying between 1.9 and 0.4 N/m at 10 mass percent Sulfur (Lee & Morita (2002), This last value is inferred to be the maximum value for Sulfur inferred to be present in the liquid outer core. Venting of Sulfur from the liquid core manifests itself on the Earth surface by the 105 to 106 ton of sulfur vented into the atmosphere annually (Wedepohl, 1984). Inspection of surface Sulfur emission indicates that venting is non-homogeneously distributed over the Earth's surface. The implication of such large variation in surface tension in the liquid outer core are that at locally low Sulfur concentration, the liquid outer core does not wet the predominantly MgSiO3 matrix with which it is in contact. However at a local high in Sulfur, the liquid outer core wets this matrix which in the fluid state has a surface tension of 0.4 N/m (Bansal & Doremus, 1986), couples with it, and causes it to sink. This differential and diapiric movement is transmitted through the essentially brittle mantle (1024 Pa.s, Lambeck & Johnson, 1998; the maximum value for ice being about 1030 Pa.s at 0 K, in all likely hood representing an upper bound of viscosity for all materials) and manifests itself on the surface by the roughly 20 km differentiation, about 0.1 % of the total mantle thickness, between topographical heights and lows with concomitant lateral movement in the crust and upper mantle resulting in thin skin tectonics. The brittle nature of the medium though which this movement is transmitted suggests that the extremes in topography of the D" layer are similar in range to

  4. Time and space variability of spectral estimates of atmospheric pressure

    NASA Technical Reports Server (NTRS)

    Canavero, Flavio G.; Einaudi, Franco

    1987-01-01

    The temporal and spatial behaviors of atmospheric pressure spectra over the northern Italy and the Alpine massif were analyzed using data on surface pressure measurements carried out at two microbarograph stations in the Po Valley, one 50 km south of the Alps, the other in the foothills of the Dolomites. The first 15 days of the study overlapped with the Alpex Intensive Observation Period. The pressure records were found to be intrinsically nonstationary and were found to display substantial time variability, implying that the statistical moments depend on time. The shape and the energy content of spectra depended on different time segments. In addition, important differences existed between spectra obtained at the two stations, indicating a substantial effect of topography, particularly for periods less than 40 min.

  5. Atmospheric deposition of sulfur and inorganic nitrogen in the Southern Canadian Rocky Mountains from seasonal snowpacks and bulk summer precipitation

    NASA Astrophysics Data System (ADS)

    Wasiuta, Vivian; Lafrenière, Melissa J.; Norman, Ann-Lise

    2015-04-01

    This study quantified atmospheric deposition of sulfur (S) and nitrogen (N) in the alpine of the Southern Canadian Rocky Mountains and evaluated loads relative to critical limits for ecologic effects on alpine ecosystems from N saturation and acidification. Deposition was evaluated by collecting seasonal snowpack and summer bulk precipitation samples along elevational transects in the alpine Haig Valley and given regional context using snowpack samples from six additional glacier sites. S and N deposition were evaluated in terms of two conceptual models. Model 1 representing deposition from emissions that are mainly distant and Model 2 representing deposition from a mixture of distant and local to regional emissions. Annual S and N (including ammonium (NH4+), nitrate (NO3-) and nitrite (NO2-)) deposition in the alpine Haig Valley was 0.74 ± 0.18 kg S ha-1 and 1.10 ± 0.18 kg N ha-1 yr-1, which is sufficiently high for the occurrence of detrimental ecologic effects related to N saturation in the most sensitive alpine ecosystems, but lower than the critical limit for acidification. Snowpack S and N deposition was consistent with well mixed air mainly from distant sources (Model 1), therefore indicating S and N were largely transported within the precipitating air mass and or picked up by the air mass in transit to the alpine Haig Valley. Relatively consistent deposition of S and N in seasonal glacier snowpacks at sites extending 210 km along the Continental Divide and 100 km west of the divide supports the interpretation that Model 1 describes deposition in alpine glacier snowpack. Similar deposition values for the highest site in the Haig Valley and the mean from the regional snowpack study indicate the highest site in the Haig Valley represents regional conditions of S and N deposition. Summer deposition of sulfate (SO42-) and ammonium (NH4+) was also consistent with dominantly distant emission sources (Model 1). In contrast there was enhanced transport and

  6. Fast single image haze removal via local atmospheric light veil estimation

    PubMed Central

    Sun, Wei; Wang, Hao; Sun, Changhao; Guo, Baolong; Jia, Wenyan; Sun, Mingui

    2015-01-01

    In this study, a novel single-image based dehazing framework is proposed to remove haze artifacts from images through local atmospheric light estimation. We use a novel strategy based on a physical model where the extreme intensity of each RGB pixel is used to define an initial atmospheric veil (local atmospheric light veil). Across bilateral filter is applied to each veil to achieve both local smoothness and edge preservation. A transmission map and a reflection component of each RGB channel are constructed from the physical atmospheric scattering model. The proposed approach avoids adverse effects caused by the error in estimating the global atmospheric light. Experimental results on outdoor hazy images demonstrate that the proposed method produces image output with satisfactory visual quality and color fidelity. Our comparative study demonstrates a higher performance of our method over several state-of-the-art methods. PMID:26744548

  7. A Vertical Diffusion Scheme to estimate the atmospheric rectifier effect

    NASA Astrophysics Data System (ADS)

    Chen, Baozhang; Chen, Jing M.; Liu, Jane; Chan, Douglas; Higuchi, Kaz; Shashkov, Alexander

    2004-02-01

    The magnitude and spatial distribution of the carbon sink in the extratropical Northern Hemisphere remain uncertain in spite of much progress made in recent decades. Vertical CO2 diffusion in the planetary boundary layer (PBL) is an integral part of atmospheric CO2 transport and is important in understanding the global CO2 distribution pattern, in particular, the rectifier effect on the distribution [Keeling et al., 1989; Denning et al., 1995]. Attempts to constrain carbon fluxes using surface measurements and inversion models are limited by large uncertainties in this effect governed by different processes. In this study, we developed a Vertical Diffusion Scheme (VDS) to investigate the vertical CO2 transport in the PBL and to evaluate CO2 vertical rectification. The VDS was driven by the net ecosystem carbon flux and the surface sensible heat flux, simulated using the Boreal Ecosystem Productivity Simulator (BEPS) and a land surface scheme. The VDS model was validated against half-hourly CO2 concentration measurements at 20 m and 40 m heights above a boreal forest, at Fraserdale (49°52'29.9''N, 81°34'12.3''W), Ontario, Canada. The amplitude and phase of the diurnal/seasonal cycles of simulated CO2 concentration during the growing season agreed closely with the measurements (linear correlation coefficient (R) equals 0.81). Simulated vertical and temporal distribution patterns of CO2 concentration were comparable to those measured at the North Carolina tower. The rectifier effect, in terms of an annual-mean vertical gradient of CO2 concentration in the atmosphere that decreases from the surface to the top of PBL, was found at Fraserdale to be about 3.56 ppmv. Positive covariance between the seasonal cycles of plant growth and PBL vertical diffusion was responsible for about 75% of the effect, and the rest was caused by covariance between their diurnal cycles. The rectifier effect exhibited strong seasonal variations, and the contribution from the diurnal cycle

  8. CO2 flux estimation errors associated with moist atmospheric processes

    NASA Astrophysics Data System (ADS)

    Parazoo, N. C.; Denning, A. S.; Kawa, S. R.; Pawson, S.; Lokupitiya, R.

    2012-04-01

    Vertical transport by moist sub-grid scale processes such as deep convection is a well-known source of uncertainty in CO2 source/sink inversion. However, a dynamical link between moist transport, satellite CO2 retrievals, and source/sink inversion has not yet been established. Here we examine the effect of moist processes on (1) synoptic CO2 transport by Version-4 and Version-5 NASA Goddard Earth Observing System Data Assimilation System (NASA-DAS) meteorological analyses, and (2) source/sink inversion. We find that synoptic transport processes, such as fronts and dry/moist conveyors, feed off background vertical CO2 gradients, which are modulated by sub-grid vertical transport. The implication for source/sink estimation is two-fold. First, CO2 variations contained in moist poleward moving air masses are systematically different from variations in dry equatorward moving air. Moist poleward transport is hidden from orbital sensors on satellites, causing a sampling bias, which leads directly to continental scale source/sink estimation errors of up to 0.25 PgC yr-1 in northern mid-latitudes. Second, moist processes are represented differently in GEOS-4 and GEOS-5, leading to differences in vertical CO2 gradients, moist poleward and dry equatorward CO2 transport, and therefore the fraction of CO2 variations hidden in moist air from satellites. As a result, sampling biases are amplified, causing source/sink estimation errors of up to 0.55 PgC yr-1 in northern mid-latitudes. These results, cast from the perspective of moist frontal transport processes, support previous arguments that the vertical gradient of CO2 is a major source of uncertainty in source/sink inversion.

  9. Using optimal estimation method for upper atmospheric Lidar temperature retrieval

    NASA Astrophysics Data System (ADS)

    Zou, Rongshi; Pan, Weilin; Qiao, Shuai

    2016-07-01

    Conventional ground based Rayleigh lidar temperature retrieval use integrate technique, which has limitations that necessitate abandoning temperatures retrieved at the greatest heights due to the assumption of a seeding value required to initialize the integration at the highest altitude. Here we suggests the use of a method that can incorporate information from various sources to improve the quality of the retrieval result. This approach inverts lidar equation via optimal estimation method(OEM) based on Bayesian theory together with Gaussian statistical model. It presents many advantages over the conventional ones: 1) the possibility of incorporating information from multiple heterogeneous sources; 2) provides diagnostic information about retrieval qualities; 3) ability of determining vertical resolution and maximum height to which the retrieval is mostly independent of the a priori profile. This paper compares one-hour temperature profiles retrieved using conventional and optimal estimation methods at Golmud, Qinghai province, China. Results show that OEM results show a better agreement with SABER profile compared with conventional one, in some region it is much lower than SABER profile, which is a very different results compared with previous studies, further studies are needed to explain this phenomenon. The success of applying OEM on temperature retrieval is a validation for using as retrieval framework in large synthetic observation systems including various active remote sensing instruments by incorporating all available measurement information into the model and analyze groups of measurements simultaneously to improve the results.

  10. Differentiating atmospheric and mineral sources of sulfur during snowmelt using δ 34S, 35S activity, and δ 18O of sulfate and water as tracers

    NASA Astrophysics Data System (ADS)

    Shanley, J. B.; Mayer, B.; Mitchell, M. J.; Michel, R. L.; Bailey, S.; Kendall, C.

    2003-12-01

    The biogeochemical cycling of sulfur was studied during the 2000 snowmelt at Sleepers River Research Watershed in northeastern Vermont, USA using a combination of isotopic, chemical, and hydrometric measurements. The snowpack and 10 streams of varying size and land use were sampled for sulfate concentrations and isotopic analyses of 35S, δ 34S, and δ 18O of sulfate. Values of δ 18O of water were measured at one of the streams. Apportionment of atmospheric and mineral S sources based on δ 34S was possible at 7 of the 10 streams. Weathering of S-containing minerals was a major contributor to sulfate flux in streamwater, but atmospheric contributions exceeded 50% in several of the streams at peak snowmelt and averaged 41% overall. In contrast, δ 18Osulfate values of streamwater remained significantly lower than those of atmospheric sulfate throughout the melt period, indicating that atmospheric sulfate undergoes microbial redox reactions in the soil that replace the oxygen of atmospheric sulfate with isotopically lighter oxygen from soil water. Streamwater 35S activities were low relative to those of the snowpack; the youngest 35S-ages of the atmospheric S component in each of the 7 streams ranged from 184 to 320 days. Atmospheric S contributions to streamwater, as determined by δ 34S values, co-varied both with 35S activity and new water contributions as determined by δ 18Owater. However, the δ 18Osulfate and 35S ages clearly show that this new water carries very little of the atmospheric sulfate entering with the current snowmelt to the stream. Most incoming atmospheric sulfate first cycles through the organic soil S pool and ultimately reaches the stream as pedogenic sulfate.

  11. Air Quality Criteria for Sulfur Oxides.

    ERIC Educational Resources Information Center

    National Air Pollution Control Administration (DHEW), Washington, DC.

    Included is a literature review which comprehensively discusses knowledge of the sulfur oxides commonly found in the atmosphere. The subject content is represented by the 10 chapter titles: Physical and Chemical Properties and the Atmospheric Reactions of the Oxides of Sulfur; Sources and Methods of Measurements of Sulfur Oxides in the Atmosphere;…

  12. The role of crystallization-driven exsolution on the sulfur mass balance in volcanic arc magmas

    USGS Publications Warehouse

    Su, Yanqing; Huber, Christian; Bachmann, Olivier; Zajacz, Zoltán; Wright, Heather M.; Vazquez, Jorge A.

    2016-01-01

    The release of large amounts of sulfur to the stratosphere during explosive eruptions affects the radiative balance in the atmosphere and consequentially impacts climate for up to several years after the event. Quantitative estimations of the processes that control the mass balance of sulfur between melt, crystals, and vapor bubbles is needed to better understand the potential sulfur yield of individual eruption events and the conditions that favor large sulfur outputs to the atmosphere. The processes that control sulfur partitioning in magmas are (1) exsolution of volatiles (dominantly H2O) during decompression (first boiling) and during isobaric crystallization (second boiling), (2) the crystallization and breakdown of sulfide or sulfate phases in the magma, and (3) the transport of sulfur-rich vapor (gas influx) from deeper unerupted regions of the magma reservoir. Vapor exsolution and the formation/breakdown of sulfur-rich phases can all be considered as closed-system processes where mass balance arguments are generally easier to constrain, whereas the contribution of sulfur by vapor transport (open system process) is more difficult to quantify. The ubiquitous “excess sulfur” problem, which refers to the much higher sulfur mass released during eruptions than what can be accounted for by amount of sulfur originally dissolved in erupted melt, as estimated from melt inclusion sulfur concentrations (the “petrologic estimate”), reflects the challenges in closing the sulfur mass balance between crystals, melt, and vapor before and during a volcanic eruption. In this work, we try to quantify the relative importance of closed- and open-system processes for silicic arc volcanoes using kinetic models of sulfur partitioning during exsolution. Our calculations show that crystallization-induced exsolution (second boiling) can generate a significant fraction of the excess sulfur observed in crystal-rich arc magmas. This result does not negate the important role of

  13. Sulfur hexafluoride (SF6) emission estimates for China: an inventory for 1990-2010 and a projection to 2020.

    PubMed

    Fang, Xuekun; Hu, Xia; Janssens-Maenhout, Greet; Wu, Jing; Han, Jiarui; Su, Shenshen; Zhang, Jianbo; Hu, Jianxin

    2013-04-16

    Sulfur hexafluoride (SF6) is the most potent greenhouse gas regulated under the Kyoto Protocol, with a high global warming potential. In this study, SF6 emissions from China were inventoried for 1990-2010 and projected to 2020. Results reveal that the highest SF6 emission contribution originates from the electrical equipment sector (about 70%), followed by the magnesium production sector, the semiconductor manufacture sector and the SF6 production sector (each about 10%). Both agreements and discrepancies were found in comparisons of our estimates with previously published data. An accelerated growth rate was found for Chinese SF6 emissions during 1990-2010. Because the relative growth rate of SF6 emissions is estimated to be much higher than those of CO2, CH4, and N2O, SF6 will play an increasing role in greenhouse gas emissions in China. Global contributions from China increased rapidly from 0.9 ± 0.3% in 1990 to 22.8 ± 6.3% in 2008, making China one of the crucial contributors to the recent growth in global emissions. Under the examined Business-as-usual (BAU) Scenario, projected emissions will reach 4270 ± 1020 t in 2020, but a reduction of about 90% of the projected BAU emissions would be obtained under the Alternative Scenario.

  14. Method for preventing sulfur emissions from vessels containing molten sulfur

    SciTech Connect

    Hass, R. H.

    1984-10-23

    Emissions from sulfur pits or other vessels containing molten sulfur are prevented or minimized by use of an air purge drawn into the vessel from the atmosphere and subsequently utilized as a portion of the oxidant required in a process for oxidizing hydrogen sulfide to elemental sulfur.

  15. A Comparison of Estimates of Atmospheric Effects on Signal Propagation Using ITU Models: Initial Study Results

    NASA Astrophysics Data System (ADS)

    Morabito, D. D.

    2014-11-01

    This article provides details on a comparison performed on calculated atmospheric effects on signal propagation using different methods for the Deep Space Network (DSN) and two Near Earth Network (NEN) sites commonly used in telecommunications link budgets. Atmospheric attenuation and scintillation fading are two of the many contributors that need to be taken into account in such link budgets between transmitter and receiver. Although atmospheric noise temperature increase is another contributor (at the receiver), it is well related to atmospheric attenuation through appropriate model equations. Telecommunication engineers working NEN link budgets make use of data and models obtained from the International Telecommunication Union (ITU) in order to estimate atmospheric effects. Such effects include atmospheric attenuation (gaseous, rain, and cloud), atmospheric noise temperature contribution, and scintillation. Because most NEN links usually operate at very high margins, uncertainties in the ITU models were not much of a concern in the past as they tended to be conservative, in comparison to links of the DSN that operate at low margins and thus require more accurate statistics on atmospheric effects. Such statistics for the DSN links make use of brightness temperature measurements from multiyear water vapor radiometer (WVR) data from instruments operating at the DSN sites. Atmospheric attenuation statistics derived from WVR data are well documented and are published by the DSN. Thus, the DSN sites make a good testbed in which to cross-compare atmospheric loss statistics with those derived from ITU data and models.

  16. An adaptive technique for estimating the atmospheric density profile during the AE mission

    NASA Technical Reports Server (NTRS)

    Argentiero, P.

    1973-01-01

    A technique is presented for processing accelerometer data obtained during the AE missions in order to estimate the atmospheric density profile. A minimum variance, adaptive filter is utilized. The trajectory of the probe and probe parameters are in a consider mode where their estimates are unimproved but their associated uncertainties are permitted an impact on filter behavior. Simulations indicate that the technique is effective in estimating a density profile to within a few percentage points.

  17. Automatic parameter estimation for atmospheric turbulence mitigation techniques

    NASA Astrophysics Data System (ADS)

    Kozacik, Stephen; Paolini, Aaron; Kelmelis, Eric

    2015-05-01

    Several image processing techniques for turbulence mitigation have been shown to be effective under a wide range of long-range capture conditions; however, complex, dynamic scenes have often required manual interaction with the algorithm's underlying parameters to achieve optimal results. While this level of interaction is sustainable in some workflows, in-field determination of ideal processing parameters greatly diminishes usefulness for many operators. Additionally, some use cases, such as those that rely on unmanned collection, lack human-in-the-loop usage. To address this shortcoming, we have extended a well-known turbulence mitigation algorithm based on bispectral averaging with a number of techniques to greatly reduce (and often eliminate) the need for operator interaction. Automations were made in the areas of turbulence strength estimation (Fried's parameter), as well as the determination of optimal local averaging windows to balance turbulence mitigation and the preservation of dynamic scene content (non-turbulent motions). These modifications deliver a level of enhancement quality that approaches that of manual interaction, without the need for operator interaction. As a consequence, the range of operational scenarios where this technology is of benefit has been significantly expanded.

  18. Evaluation of sulfur dioxide-generating pads and modified atmosphere packaging for control of postharvest diseases in blueberries

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Postharvest diseases are a limiting factor of storage and shelf life of blueberries. Gray mold caused by Botrytis cinerea is one of the most important postharvest diseases in blueberries grown in California. In this study, we evaluated the effects of sulfur dioxide (SO2)-generating pads (designated ...

  19. CO2 Flux Estimation Errors Associated with Moist Atmospheric Processes

    NASA Technical Reports Server (NTRS)

    Parazoo, N. C.; Denning, A. S.; Kawa, S. R.; Pawson, S.; Lokupitiya, R.

    2012-01-01

    Vertical transport by moist sub-grid scale processes such as deep convection is a well-known source of uncertainty in CO2 source/sink inversion. However, a dynamical link between vertical transport, satellite based retrievals of column mole fractions of CO2, and source/sink inversion has not yet been established. By using the same offline transport model with meteorological fields from slightly different data assimilation systems, we examine sensitivity of frontal CO2 transport and retrieved fluxes to different parameterizations of sub-grid vertical transport. We find that frontal transport feeds off background vertical CO2 gradients, which are modulated by sub-grid vertical transport. The implication for source/sink estimation is two-fold. First, CO2 variations contained in moist poleward moving air masses are systematically different from variations in dry equatorward moving air. Moist poleward transport is hidden from orbital sensors on satellites, causing a sampling bias, which leads directly to small but systematic flux retrieval errors in northern mid-latitudes. Second, differences in the representation of moist sub-grid vertical transport in GEOS-4 and GEOS-5 meteorological fields cause differences in vertical gradients of CO2, which leads to systematic differences in moist poleward and dry equatorward CO2 transport and therefore the fraction of CO2 variations hidden in moist air from satellites. As a result, sampling biases are amplified and regional scale flux errors enhanced, most notably in Europe (0.43+/-0.35 PgC /yr). These results, cast from the perspective of moist frontal transport processes, support previous arguments that the vertical gradient of CO2 is a major source of uncertainty in source/sink inversion.

  20. CO2 flux estimation errors associated with moist atmospheric processes

    NASA Astrophysics Data System (ADS)

    Parazoo, N. C.; Denning, A. S.; Kawa, S. R.; Pawson, S.; Lokupitiya, R.

    2012-07-01

    Vertical transport by moist sub-grid scale processes such as deep convection is a well-known source of uncertainty in CO2 source/sink inversion. However, a dynamical link between vertical transport, satellite based retrievals of column mole fractions of CO2, and source/sink inversion has not yet been established. By using the same offline transport model with meteorological fields from slightly different data assimilation systems, we examine sensitivity of frontal CO2 transport and retrieved fluxes to different parameterizations of sub-grid vertical transport. We find that frontal transport feeds off background vertical CO2 gradients, which are modulated by sub-grid vertical transport. The implication for source/sink estimation is two-fold. First, CO2 variations contained in moist poleward moving air masses are systematically different from variations in dry equatorward moving air. Moist poleward transport is hidden from orbital sensors on satellites, causing a sampling bias, which leads directly to small but systematic flux retrieval errors in northern mid-latitudes. Second, differences in the representation of moist sub-grid vertical transport in GEOS-4 and GEOS-5 meteorological fields cause differences in vertical gradients of CO2, which leads to systematic differences in moist poleward and dry equatorward CO2 transport and therefore the fraction of CO2 variations hidden in moist air from satellites. As a result, sampling biases are amplified and regional scale flux errors enhanced, most notably in Europe (0.43 ± 0.35 PgC yr-1). These results, cast from the perspective of moist frontal transport processes, support previous arguments that the vertical gradient of CO2 is a major source of uncertainty in source/sink inversion.

  1. Estimating Sulfur Dioxide in Volcanic Plumes Using an Ultraviolet Camera. First Results from Lascar, Ollagüe and Irruputuncu Volcanoes

    NASA Astrophysics Data System (ADS)

    Geoffroy, C. A.; Amigo, A.

    2014-12-01

    Volcanic gas fluxes give important information on both the amount of degassing and magma reservoirs. In most of magmas, water vapor (H2O) and carbon dioxide (CO2) are major components of volcanic gas. However, sulfur dioxide (SO2) is one of the targets of remote sensing due to their low concentration in the environment and easy detection by ultraviolet spectroscopy. Accordingly, plume imaging using passive ultraviolet cameras is a relatively simple method to study volcanic degassing, expeditious manner and can be used up from distances of about 10 km from source of emissions. We estimated SO2 concentrations and fluxes in volcanic plumes with the ultraviolet camera Envicam-2, developed by Nicarnica Aviation, acquired by the Geological Survey of Chile (SERNAGEOMIN). The camera has filters that allow passage of ultraviolet radiation at wavelengths of interest. For determining whether there is absorption of radiation associated with the presence of SO2 the Beer-Lambert law was used for quantifying concentrations using appropriate calibration cells. SO2 emissions to the atmosphere were estimated using wind speed as an approximation to the plume transport. In this study we reported the implementation of a new methodology for using Envicam-2 and subsequent collection of SO2 concentrations and fluxes in passive degassing volcanoes. Measurements were done at Lascar, Ollagüe and Irruputuncu volcanoes, located in northern Chile. The volcanoes were chosen because of optimal atmospheric conditions for ultraviolet imaging. Results indicate concentrations within the expected ranges for three volcanoes generally between 400-1700 ppm•m. In the case of Láscar volcano, the emission rates of SO2 range from 250 to 500 tonnes/day for a same image of the plume. In particular, wind speed was determined from scaling images and are consistent with data from regional numerical models, as well as records of the meteorological stations installed at the ALMA astronomical center, located

  2. MAXINE: An improved methodology for estimating maximum individual dose from chronic atmospheric radioactive releases

    SciTech Connect

    Hamby, D.M.

    1994-02-01

    An EXCEL{reg_sign} spreadsheet has been developed that, when combined with the PC version of XOQDOQ, will generate estimates of maximum individual dose from routine atmospheric releases of radionuclides. The spreadsheet, MAXINE, utilizes a variety of atmospheric dispersion factors to calculate radiation dose as recommended by the US Nuclear Regulatory Commission in Regulatory Guide 1.109 [USNRC 1977a]. The methodology suggested herein includes use of both the MAXINE spreadsheet and the PC version of XOQDOQ.

  3. Improving Estimates of Atmosphere-Ocean Greenhouse Gas Fluxes for Earth-System Modelling

    NASA Astrophysics Data System (ADS)

    Vieira, V. M. N. C. S.; Sahlee, E.; Jurus, P.; Clementi, E.; Pettersson, H.; Mateus, M.

    2016-08-01

    Accurate estimates of atmosphere-ocean balances and fluxes of greenhouse gases and aerosols are fundamental for Earth-System models forecasting the climate change, and for Earth Observation estimates of oceanic sinks and sources coupling satellite imagery with reverse modelling. The standard formulations are 24 and 36 years old, and recent alternatives have emerged. We developed a framework congregating the geophysical processes involved, customizable with alternative formulations, and that can be used as basis for novel couplers of atmospheric and oceanographic model components. We tested it with fine resolution data from the European coastal ocean. Although the solubility formulations agreed well, their minor divergences yielded differences of many tons of greenhouse gases dissolved at the ocean surface. The transfer velocities largely mismatched their estimates, in part consequence of the standard formulation not considering factors that were proved determinant at the coastal ocean. Climate Change research requires further calibration and validation of atmosphere-ocean interactions.

  4. Estimation of the atmospheric corrosion on metal containers in industrial waste disposal.

    PubMed

    Baklouti, M; Midoux, N; Mazaudier, F; Feron, D

    2001-08-17

    Solid industrial waste are often stored in metal containers filled with concrete, and placed in well-aerated warehouses. Depending on meteorological conditions, atmospheric corrosion can induce severe material damages to the metal casing, and this damage has to be predicted to achieve safe storage. This work provides a first estimation of the corrosivity of the local atmosphere adjacent to the walls of the container through a realistic modeling of heat transfer phenomena which was developed for this purpose. Subsequent simulations of condensation/evaporation of the water vapor in the atmosphere were carried out. Atmospheric corrosion rates and material losses are easily deduced. For handling realistic data and comparison, two different meteorological contexts were chosen: (1) an oceanic and damp atmosphere and (2) a drier storage location. Some conclusions were also made for the storage configuration in order to reduce the extent of corrosion phenomena.

  5. Zeolites Remove Sulfur From Fuels

    NASA Technical Reports Server (NTRS)

    Voecks, Gerald E.; Sharma, Pramod K.

    1991-01-01

    Zeolites remove substantial amounts of sulfur compounds from diesel fuel under relatively mild conditions - atmospheric pressure below 300 degrees C. Extracts up to 60 percent of sulfur content of high-sulfur fuel. Applicable to petroleum refineries, natural-gas processors, electric powerplants, and chemical-processing plants. Method simpler and uses considerably lower pressure than current industrial method, hydro-desulfurization. Yields cleaner emissions from combustion of petroleum fuels, and protects catalysts from poisoning by sulfur.

  6. Analysis of organic sulfur compounds in atmospheric aerosols at the HKUST supersite in Hong Kong using HR-ToF-AMS.

    PubMed

    Huang, Dan Dan; Li, Yong Jie; Lee, Berto P; Chan, Chak K

    2015-03-17

    Organic sulfur compounds have been identified in ambient secondary organic aerosols, but their contribution to organic mass is not well quantified. In this study, using a high-resolution time-of-flight aerosol mass spectrometer (AMS), concentrations of organic sulfur compounds were estimated based on the high-resolution fragmentation patterns of methanesulfonic acid (MSA), and organosulfates (OS), including alkyl, phenyl, and cycloalkyl sulfates, obtained in laboratory experiments. Mass concentrations of MSA and minimum mass concentrations of OS were determined in a field campaign conducted at a coastal site of Hong Kong in September 2011. MSA and OS together accounted for at least 5% of AMS detected organics. MSA is of marine origin with its formation dominated by local photochemical activities and enhanced by aqueous phase processing. OS concentrations are better correlated with particle liquid water content (LWC) than with particle acidity. High-molecular-weight OS were detected in the continental influenced period probably because they had grown into larger molecules during long-range transport or they were formed from large anthropogenic precursors. This study highlights the importance of both aqueous-phase processing and regional influence, i.e., different air mass origins, on organic sulfur compound formation in coastal cities like Hong Kong.

  7. The Abundance of Sulfur in Venus Magmas

    NASA Astrophysics Data System (ADS)

    Bullock, M. A.; Grinspoon, D. H.

    1999-09-01

    Outgassing of sulfur gases due to volcanism within the past 100 My on Venus is probably responsible for the planet's globally encircling H2SO4 cloud layers. Dramatic changes in volcanic output on Venus would have altered the atmospheric inventory of sulfur gases, and hence the structure of its clouds (Bullock and Grinspoon, Icarus, submitted 1999). Although Magellan radar images provide some constraints on the magnitude of volcanism in the geologically recent past, little is known of the sulfur content of Venus lavas. In order to assess the effects that Venus' volcanic history may have had on cloud and therefore climate change, it is desirable to place some constraints on the abundance of sulfur in Venus magmas. The sulfur content of terrestrial volcanic lavas varies widely, depending upon the local sedimentary environment and the source and history of upwelling magmas. We estimate the average abundance of sulfur in Venus lavas from an analysis of the production and loss of atmospheric SO2. The volumetric rate of resurfacing on Venus in the recent past is approximately 0.1 to 2 km3/yr (Bullock et al., JGR 20, 1993, Basilevsky and Head, GRL 23, 1996). Outgassed SO2 reacts quickly with crustal carbonate -- residence times in the atmosphere with respect to the reaction SO2 + CaCO3 <=> CaSO4 + CO are about 2-30 My (Fegley and Prinn, Nature 337, 1989, Bullock and Grinspoon, Icarus, submitted 1999). Assuming steady state conditions and an abundance of 25-180 ppm of atmospheric SO2 (Oyama et al., JGR 85, 1980, Bertaux et al., JGR 101, 1996), we will discuss constraints on the abundance of this important greenhouse and cloud-precursor gas in Venus lavas.

  8. Atmospheric corrections of passive microwave data for estimating land surface temperature.

    PubMed

    Liu, Zeng-Lin; Wu, Hua; Tang, Bo-Hui; Qiu, Shi; Li, Zhao-Liang

    2013-07-01

    Quantitative analysis of the atmospheric effects on observations made by the Advanced Microwave Scanning Radiometer-Earth Observing System (AMSR-E) has been performed. The differences between observed brightness temperatures at the top of the atmosphere and at the bottom of the atmosphere were analyzed using a database of simulated observations, which were configured to replicate AMSR-E data. The differences between observed brightness temperatures at the top of the atmosphere and land surface-emitted brightness temperatures were also computed. Quantitative results show that the atmosphere has different effects on brightness temperatures in different AMSR-E channels. Atmospheric effects can be neglected at 6.925 and 10.65 GHz, when the standard deviation is less than 1 K. However, at other frequencies and polarizations, atmospheric effects on observations should not be neglected. An atmospheric correction algorithm was developed at 18.7 GHz vertical polarization, based on the classic split-window algorithm used in thermal remote sensing. Land surface emission can be estimated with RMSE = 0.99 K using the proposed method. Using the known land surface emissivity, Land Surface Temperature (LST) can be retrieved. The RMSE of retrieved LST is 1.17 K using the simulated data.

  9. Inverse estimation of radon flux distribution for East Asia using measured atmospheric radon concentration.

    PubMed

    Hirao, S; Hayashi, R; Moriizumi, J; Yamazawa, H; Tohjima, Y; Mukai, H

    2015-11-01

    In this study, the (222)Rn flux density distribution at surface was estimated in East Asia with the Bayesian synthesis inversion using measurement data and a long-range atmospheric (222)Rn transport model. Surface atmospheric (222)Rn concentrations measured at Hateruma Island in January 2008 were used. The estimated (222)Rn flux densities were generally higher than the prior ones. The area-weighted mean (222)Rn flux density for East Asia in January 2008 was estimated to be 44.0 mBq m(-2) s(-1). The use of the estimated (222)Rn flux density improved the discrepancy of the model-calculated concentrations with the measurements at Hateruma Island.

  10. Formic acid catalyzed hydrolysis of SO3 in the gas phase: a barrierless mechanism for sulfuric acid production of potential atmospheric importance.

    PubMed

    Hazra, Montu K; Sinha, Amitabha

    2011-11-02

    Computational studies at the B3LYP/6-311++G(3df,3pd) and MP2/6-311++G(3df,3pd) levels are performed to explore the changes in reaction barrier height for the gas phase hydrolysis of SO(3) to form H(2)SO(4) in the presence of a single formic acid (FA) molecule. For comparison, we have also performed calculations for the reference reaction involving water assisted hydrolysis of SO(3) at the same level. Our results show that the FA assisted hydrolysis of SO(3) to form H(2)SO(4) is effectively a barrierless process. The barrier heights for the isomerization of the SO(3)···H(2)O···FA prereactive collision complex, which is the rate limiting step in the FA assisted hydrolysis, are found to be respectively 0.59 and 0.08 kcal/mol at the B3LYP/6-311++G(3df,3pd) and MP2/6-311++G(3df,3pd) levels. This is substantially lower than the ~7 kcal/mol barrier for the corresponding step in the hydrolysis of SO(3) by two water molecules--which is currently the accepted mechanism for atmospheric sulfuric acid production. Simple kinetic analysis of the relative rates suggests that the reduction in barrier height facilitated by FA, combined with the greater stability of the prereactive SO(3)···H(2)O···FA collision complex compared to SO(3)···H(2)O···H(2)O and the rather plentiful atmospheric abundance of FA, makes the formic acid mediated hydrolysis reaction a potentially important pathway for atmospheric sulfuric acid production.

  11. The Ability of Atmospheric Data to Reduce Disagreements in Wetland Methane Flux Estimates over North America

    NASA Astrophysics Data System (ADS)

    Miller, S. M.; Andrews, A. E.; Benmergui, J. S.; Commane, R.; Dlugokencky, E. J.; Janssens-Maenhout, G.; Melton, J. R.; Michalak, A. M.; Sweeney, C.; Worthy, D. E. J.

    2015-12-01

    Existing estimates of methane fluxes from wetlands differ in both magnitude and distribution across North America. We discuss seven different bottom-up methane estimates in the context of atmospheric methane data collected across the US and Canada. In the first component of this study, we explore whether the observation network can even detect a methane pattern from wetlands. We find that the observation network can identify a methane pattern from Canadian wetlands but not reliably from US wetlands. Over Canada, the network can even identify spatial patterns at multi-provence scales. Over the US, by contrast, anthropogenic emissions and modeling errors obscure atmospheric patterns from wetland fluxes. In the second component of the study, we then use these observations to reconcile disagreements in the magnitude, seasonal cycle, and spatial distribution of existing estimates. Most existing estimates predict fluxes that are too large with a seasonal cycle that is too narrow. A model known as LPJ-Bern has a spatial distribution most consistent with atmospheric observations. By contrast, a spatially-constant model outperforms the distribution of most existing flux estimates across Canada. The results presented here provide several pathways to reduce disagreements among existing wetland flux estimates across North America.

  12. A Useful Tool for Atmospheric Correction and Surface Temperature Estimation of Landsat Infrared Thermal Data

    NASA Astrophysics Data System (ADS)

    Rivalland, Vincent; Tardy, Benjamin; Huc, Mireille; Hagolle, Olivier; Marcq, Sébastien; Boulet, Gilles

    2016-04-01

    Land Surface temperature (LST) is a critical variable for studying the energy and water budgets at the Earth surface, and is a key component of many aspects of climate research and services. The Landsat program jointly carried out by NASA and USGS has been providing thermal infrared data for 40 years, but no associated LST product has been yet routinely proposed to community. To derive LST values, radiances measured at sensor-level need to be corrected for the atmospheric absorption, the atmospheric emission and the surface emissivity effect. Until now, existing LST products have been generated with multi channel methods such as the Temperature/Emissivity Separation (TES) adapted to ASTER data or the generalized split-window algorithm adapted to MODIS multispectral data. Those approaches are ill-adapted to the Landsat mono-window data specificity. The atmospheric correction methodology usually used for Landsat data requires detailed information about the state of the atmosphere. This information may be obtained from radio-sounding or model atmospheric reanalysis and is supplied to a radiative transfer model in order to estimate atmospheric parameters for a given coordinate. In this work, we present a new automatic tool dedicated to Landsat thermal data correction which improves the common atmospheric correction methodology by introducing the spatial dimension in the process. The python tool developed during this study, named LANDARTs for LANDsat Automatic Retrieval of surface Temperature, is fully automatic and provides atmospheric corrections for a whole Landsat tile. Vertical atmospheric conditions are downloaded from the ERA Interim dataset from ECMWF meteorological organization which provides them at 0.125 degrees resolution, at a global scale and with a 6-hour-time step. The atmospheric correction parameters are estimated on the atmospheric grid using the commercial software MODTRAN, then interpolated to 30m resolution. We detail the processing steps

  13. Channel estimation for OFDM system in atmospheric optical communication based on compressive sensing

    NASA Astrophysics Data System (ADS)

    Zhao, Qingsong; Hao, Shiqi; Geng, Hongjian; Sun, Han

    2015-10-01

    Orthogonal frequency division multiplexing (OFDM) technique applied to the atmospheric optical communication can improve data transmission rate, restrain pulse interference, and reduce effect of multipath caused by atmospheric scattering. Channel estimation, as one of the important modules in OFDM, has been investigated thoroughly and widely with great progress. In atmospheric optical communication system, channel estimation methods based on pilot are common approaches, such as traditional least-squares (LS) algorithm and minimum mean square error (MMSE) algorithm. However, sensitivity of the noise effects and high complexity of computation are shortcomings of LS algorithm and MMSE algorithm, respectively. Here, a new method based on compressive sensing is proposed to estimate the channel state information of atmospheric optical communication OFDM system, especially when the condition is closely associated with turbulence. Firstly, time-varying channel model is established under the condition of turbulence. Then, in consideration of multipath effect, sparse channel model is available for compressive sensing. And, the pilot signal is reconstructed with orthogonal matching tracking (OMP) algorithm, which is used for reconstruction. By contrast, the work of channel estimation is completed by LS algorithm as well. After that, simulations are conducted respectively in two different indexes -signal error rate (SER) and mean square error (MSE). Finally, result shows that compared with LS algorithm, the application of compressive sensing can improve the performance of SER and MSE. Theoretical analysis and simulation results show that the proposed method is reasonable and efficient.

  14. Comparison of Mars Atmospheric Density Estimates from Models to Measurements from Mars Global Surveyor (MGS) Data

    NASA Technical Reports Server (NTRS)

    Justh, Hilary L.; Justus, C. G.

    2009-01-01

    A recent study (Desai, 2008) has shown that the actual landing sites of Mars Pathfinder, the Mars Exploration Rovers (Spirit and Opportunity) and the Phoenix Mars Lander have been further downrange than predicted by models prior to landing Desai's reconstruction of their entries into the Martian atmosphere showed that the models consistently predicted higher densities than those found upon entry, descent and landing. Desai's results have raised a question as to whether there is a systemic problem within Mars atmospheric models. Proposal is to compare Mars atmospheric density estimates from Mars atmospheric models to measurements made by Mars Global Surveyor (MGS). Comparison study requires the completion of several tasks that would result in a greater understanding of reasons behind the discrepancy found during recent landings on Mars and possible solutions to this problem.

  15. Estimation of Atmospheric Path Delays in TerraSAR-X Data using Models vs. Measurements

    PubMed Central

    Jehle, Michael; Perler, Donat; Small, David; Schubert, Adrian; Meier, Erich

    2008-01-01

    Spaceborne synthetic aperture radar (SAR) measurements of the Earth's surface depend on electromagnetic waves that are subject to atmospheric path delays, in turn affecting geolocation accuracy The atmosphere influences radar signal propagation by modifying its velocity and direction, effects which can be modeled. We use TerraSAR-X (TSX) data to investigate improvements in the knowledge of the scene geometry. To precisely estimate atmospheric path delays, we analyse the signal return of four corner reflectors with accurately surveyed positions (based on differential GPS), placed at different altitudes yet with nearly identical slant ranges to the sensor. The comparison of multiple measurements with path delay models under these geometric conditions also makes it possible to evaluate the corrections for the atmospheric path delay made by the TerraSAR processor and to propose possible improvements. PMID:27873997

  16. Optimal Atmospheric Correction for Above-Ground Forest Biomass Estimation with the ETM+ Remote Sensor.

    PubMed

    Nguyen, Hieu Cong; Jung, Jaehoon; Lee, Jungbin; Choi, Sung-Uk; Hong, Suk-Young; Heo, Joon

    2015-07-31

    The reflectance of the Earth's surface is significantly influenced by atmospheric conditions such as water vapor content and aerosols. Particularly, the absorption and scattering effects become stronger when the target features are non-bright objects, such as in aqueous or vegetated areas. For any remote-sensing approach, atmospheric correction is thus required to minimize those effects and to convert digital number (DN) values to surface reflectance. The main aim of this study was to test the three most popular atmospheric correction models, namely (1) Dark Object Subtraction (DOS); (2) Fast Line-of-sight Atmospheric Analysis of Spectral Hypercubes (FLAASH) and (3) the Second Simulation of Satellite Signal in the Solar Spectrum (6S) and compare them with Top of Atmospheric (TOA) reflectance. By using the k-Nearest Neighbor (kNN) algorithm, a series of experiments were conducted for above-ground forest biomass (AGB) estimations of the Gongju and Sejong region of South Korea, in order to check the effectiveness of atmospheric correction methods for Landsat ETM+. Overall, in the forest biomass estimation, the 6S model showed the bestRMSE's, followed by FLAASH, DOS and TOA. In addition, a significant improvement of RMSE by 6S was found with images when the study site had higher total water vapor and temperature levels. Moreover, we also tested the sensitivity of the atmospheric correction methods to each of the Landsat ETM+ bands. The results confirmed that 6S dominates the other methods, especially in the infrared wavelengths covering the pivotal bands for forest applications. Finally, we suggest that the 6S model, integrating water vapor and aerosol optical depth derived from MODIS products, is better suited for AGB estimation based on optical remote-sensing data, especially when using satellite images acquired in the summer during full canopy development.

  17. Optimal Atmospheric Correction for Above-Ground Forest Biomass Estimation with the ETM+ Remote Sensor

    PubMed Central

    Nguyen, Hieu Cong; Jung, Jaehoon; Lee, Jungbin; Choi, Sung-Uk; Hong, Suk-Young; Heo, Joon

    2015-01-01

    The reflectance of the Earth’s surface is significantly influenced by atmospheric conditions such as water vapor content and aerosols. Particularly, the absorption and scattering effects become stronger when the target features are non-bright objects, such as in aqueous or vegetated areas. For any remote-sensing approach, atmospheric correction is thus required to minimize those effects and to convert digital number (DN) values to surface reflectance. The main aim of this study was to test the three most popular atmospheric correction models, namely (1) Dark Object Subtraction (DOS); (2) Fast Line-of-sight Atmospheric Analysis of Spectral Hypercubes (FLAASH) and (3) the Second Simulation of Satellite Signal in the Solar Spectrum (6S) and compare them with Top of Atmospheric (TOA) reflectance. By using the k-Nearest Neighbor (kNN) algorithm, a series of experiments were conducted for above-ground forest biomass (AGB) estimations of the Gongju and Sejong region of South Korea, in order to check the effectiveness of atmospheric correction methods for Landsat ETM+. Overall, in the forest biomass estimation, the 6S model showed the bestRMSE’s, followed by FLAASH, DOS and TOA. In addition, a significant improvement of RMSE by 6S was found with images when the study site had higher total water vapor and temperature levels. Moreover, we also tested the sensitivity of the atmospheric correction methods to each of the Landsat ETM+ bands. The results confirmed that 6S dominates the other methods, especially in the infrared wavelengths covering the pivotal bands for forest applications. Finally, we suggest that the 6S model, integrating water vapor and aerosol optical depth derived from MODIS products, is better suited for AGB estimation based on optical remote-sensing data, especially when using satellite images acquired in the summer during full canopy development. PMID:26263996

  18. Estimation of absolute water surface temperature based on atmospherically corrected thermal infrared multispectral scanner digital data

    NASA Technical Reports Server (NTRS)

    Anderson, James E.

    1986-01-01

    Airborne remote sensing systems, as well as those on board Earth orbiting satellites, sample electromagnetic energy in discrete wavelength regions and convert the total energy sampled into data suitable for processing by digital computers. In general, however, the total amount of energy reaching a sensor system located at some distance from the target is composed not only of target related energy, but, in addition, contains a contribution originating from the atmosphere itself. Thus, some method must be devised for removing or at least minimizing the effects of the atmosphere. The LOWTRAN-6 Program was designed to estimate atmospheric transmittance and radiance for a given atmospheric path at moderate spectral resolution over an operational wavelength region from 0.25 to 28.5 microns. In order to compute the Thermal Infrared Multispectral Scanner (TIMS) digital values which were recorded in the absence of the atmosphere, the parameters derived from LOWTRAN-6 are used in a correction equation. The TIMS data were collected at 1:00 a.m. local time on November 21, 1983, over a recirculating cooling pond for a power plant in southeastern Mississippi. The TIMS data were analyzed before and after atmospheric corrections were applied using a band ratioing model to compute the absolute surface temperature of various points on the power plant cooling pond. The summarized results clearly demonstrate the desirability of applying atmospheric corrections.

  19. Laboratory measurements of the 3.7-20 cm wavelength opacity of sulfur dioxide and carbon dioxide under simulated conditions for the deep atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Steffes, Paul G.; Shahan, Patrick; Christopher Barisich, G.; Bellotti, Amadeo

    2015-01-01

    In the past two decades, multiple observations of Venus have been made at X-Band (3.6 cm) using the Jansky Very Large Array (VLA), and maps have been created of the 3.6 cm emission from Venus (see, e.g., Devaraj, K. [2011]. The Centimeter- and Millimeter-Wavelength Ammonia Absorption Spectra under Jovian Conditions. PhD Thesis, Georgia Institute of Technology, Atlanta, GA). Since the emission morphology is related both to surface features and to deep atmospheric absorption from CO2 and SO2 (see, e.g., Butler, B.J., Steffes, P.G., Suleiman, S.H., Kolodner, M.A., Jenkins, J.M. [2001]. Icarus 154, 226-238), knowledge of the microwave absorption properties of sulfur dioxide in a carbon dioxide atmosphere under conditions for the deep atmosphere of Venus is required for proper interpretation. Except for a single measurement campaign conducted at a single wavelength (3.2 cm) over 40 years ago (Ho, W., Kaufman, I.A., Thaddeus, P. [1966]. J. Geophys. Res. 71, 5091-5108), no measurements of the centimeter-wavelength properties of any Venus atmospheric constituent have been conducted under conditions characteristic of the deep atmosphere (pressures from 10 to 92 bars and temperatures from 400 to 700 K). New measurements of the microwave properties of SO2 and CO2 at wavelengths from 3.7 to 20 cm have been conducted under simulated conditions for the deep atmosphere of Venus, using a new high-pressure system. Results from this measurement campaign conducted at temperatures from 430 K to 560 K and at pressures up to 92 bars are presented. Results indicate that the model for the centimeter-wavelength opacity from pure CO2 (Ho, W., Kaufman, I.A., Thaddeus, P. [1966]. J. Geophys. Res. 71, 5091-5108), is valid over the entire centimeter-wavelength range under simulated conditions for the deep atmosphere of Venus. Additionally, the laboratory results indicate that both of the models for the centimeter-wavelength opacity of SO2 in a CO2 atmosphere from Suleiman et al. (Suleiman, S

  20. Long-term variations in abundance and distribution of sulfuric acid vapor in the Venus atmosphere inferred from Pioneer Venus and Magellan radio occultation studies

    NASA Technical Reports Server (NTRS)

    Jenkins, J. M.; Steffes, P. G.

    1992-01-01

    Radio occultation experiments have been used to study various properties of planetary atmospheres, including pressure and temperature profiles, and the abundance profiles of absorbing constituents in those planetary atmospheres. However, the reduction of amplitude data from such experiments to determine abundance profiles requires the application of the inverse Abel transform (IAT) and numerical differentiation of experimental data. These two operations preferentially amplify measurement errors above the true signal underlying the data. A new technique for processing radio occultation data has been developed that greatly reduces the errors in the derived absorptivity and abundance profiles. This technique has been applied to datasets acquired from Pioneer Venus Orbiter radio occultation studies and more recently to experiments conducted with the Magellan spacecraft. While primarily designed for radar studies of the Venus surface, the high radiated power (EIRP) from the Magellan spacecraft makes it an ideal transmitter for measuring the refractivity and absorptivity of the Venus atmosphere by such experiments. The longevity of the Pioneer Venus Orbiter has made it possible to study long-term changes in the abundance and distribution of sulfuric acid vapor, H2SO4(g), in the Venus atmosphere between 1979 and 1992. The abundance of H2SO4(g) can be inferred from vertical profiles of 13-cm absorptivity profiles retrieved from radio occultation experiments. Data from 1979 and 1986-87 suggest that the abundance of H2SO4(g) at latitudes northward of 70 deg decreased over this time period. This change may be due to a period of active volcanism in the late 1970s followed by a relative quiescent period, or some other dynamic process in the Venus atmosphere. While the cause is not certain, such changes must be incorporated into dynamic models of the Venus atmosphere. Potentially, the Magellan spacecraft will extend the results of Pioneer Venus Orbiter and allow the continued

  1. Improved estimates of ventilation rate changes and CO2 uptake in the Pacific Ocean using chlorofluorocarbons and sulfur hexafluoride

    NASA Astrophysics Data System (ADS)

    Sonnerup, Rolf E.; Bullister, John L.; Warner, Mark J.

    2008-12-01

    Depth profiles of dissolved sulfur hexafluoride (SF6) were measured at 10 stations during the 2006 Climate Variability and Predictability (CLIVAR) Repeat Hydrography reoccupation of the 1991 World Ocean Circulation Experiment P16 section along 152°W between 14°S and 52°N. Ventilation ages calculated from the partial pressure of SF6 (pSF6 ages) were generally 6-10 years younger than those calculated from concurrent CFC-12 partial pressures (pCFC-12 ages). A one-dimensional parameterization of transit time distributions is utilized to demonstrate the potential of SF6, as a complement to the CFCs, to constrain the impact of mixing on the tracer-derived ages. The two-tracer approach provides an estimate of the mixing-induced tendency of pCFC-12 ages to change with time by correcting their bias to younger ages in older waters and their bias to older ages in younger waters. Model scenarios that match both the 2006 pSF6 and pCFC-12 ages predict a mixing-induced increase in pCFC-12 ages of 6-10 years between the 1991 and 2006 occupations of P16, similar to the increase in pCFC-12 ages observed. Model scenarios tuned to the pCFC-12 and pSF6 ages from 2006 are used to calculate anthropogenic CO2 along the section and yield slightly smaller anthropogenic CO2 burdens than calculated solely from the pCFC-12 ages in waters with pCFC-12 ages >36 years in 2006.

  2. The atmospheric CH4 increase since the Last Glacial Maximum. I - Source estimates

    NASA Technical Reports Server (NTRS)

    Chappellaz, Jerome A.; Fung, Inez Y.; Thompson, Anne M.

    1993-01-01

    An estimate of the distribution of wetland area and associated CH4 emission is presented for the Last Glacial Maximum (LGM, 18 kyr BP, kiloyear Before Present) and the Pre-Industrial Holocene (PIH, 9000-200 years BP). The wetland source, combined with estimates of the other biogenic sources and sink, yields total source strengths of 120 and 180 Tg CH4/yr for LGM and PIH respectively. These source strengths are shown to be consistent with source estimates inferred from a photochemical model, and point to changes in wetland CH4 source as a major factor driving the atmospheric CH4 increase from LGM to PIH.

  3. Estimating annual precipitation for the Colorado River Basin using oceanic-atmospheric oscillations

    NASA Astrophysics Data System (ADS)

    Kalra, Ajay; Ahmad, Sajjad

    2012-06-01

    Estimating long-lead time precipitation under the stress of increased climatic variability is a challenging task in the field of hydrology. A modified Support Vector Machine (SVM) based framework is proposed to estimate annual precipitation using oceanic-atmospheric oscillations. Oceanic-atmospheric oscillations, consisting of Pacific Decadal Oscillation (PDO), North Atlantic Oscillation (NAO), Atlantic Multidecadal Oscillation (AMO), and El Niño-Southern Oscillation (ENSO) for a period of 1900-2008, are used to generate annual precipitation estimates with a 1 year lead time. The SVM model is applied to 17 climate divisions encompassing the Colorado River Basin in the western United States. The overall results revealed that the annual precipitation in the Colorado River Basin is significantly influenced by oceanic-atmospheric oscillations. The long-term precipitation predictions for the Upper Colorado River Basin can be successfully obtained using a combination of PDO, NAO, and AMO indices, whereas coupling AMO and ENSO results in improved precipitation predictions for the Lower Colorado River Basin. The results also show that the SVM model provides better precipitation estimates compared to the Artificial Neural Network and Multivariate Linear Regression models. The annual precipitation estimates obtained using the modified SVM modeling framework may assist water managers in statistically understanding the hydrologic response in relation to large scale climate patterns within the Colorado River Basin.

  4. Atmospheric channel transfer function estimation from experimental free-space optical communications data

    NASA Astrophysics Data System (ADS)

    Reinhardt, Colin N.; Tsintikidis, Dimitris; Hammel, Stephen; Kuga, Yasuo; Ritcey, James A.; Ishimaru, Akira

    2012-03-01

    Using an 850-nanometer-wavelength free-space optical (FSO)communications system of our own design, we acquired field data for the transmitted and received signals in fog at Point Loma, CA for a range of optical depths within the multiple-scattering regime. Statistical estimators for the atmospheric channel transfer function and the related coherency function were computed directly from the experimental data. We interpret the resulting channel transfer function estimates in terms of the physics of the atmospheric propagation channel and fog aerosol particle distributions. We investigate the behavior of the estimators using both real field-test data and simulated propagation data. We compare the field-data channel transfer function estimates against the outputs from a computationally-intensive radiative-transfer theory model-based approach, which we also developed previously for the FSO multiple-scattering atmospheric channel. Our results show that the data-driven channel transfer function estimates are in close agreement with the radiative transfer modeling, and provide comparable receiver signal detection performance improvements while being significantly less time and computationally-intensive.

  5. Medusa: a sample preconcentration and GC/MS detector system for in situ measurements of atmospheric trace halocarbons, hydrocarbons, and sulfur compounds.

    PubMed

    Miller, Benjamin R; Weiss, Ray F; Salameh, Peter K; Tanhua, Toste; Greally, Brian R; Mühle, Jens; Simmonds, Peter G

    2008-03-01

    Significant changes have occurred in the anthropogenic emissions of many compounds related to the Kyoto and Montreal Protocols within the past 20 years and many of their atmospheric abundances have responded dramatically. Additionally, there are a number of related natural compounds with underdetermined source or sink budgets. A new instrument, Medusa, was developed to make the high frequency in situ measurements required for the determination of the atmospheric lifetimes and emissions of these compounds. This automated system measures a wide range of halocarbons, hydrocarbons, and sulfur compounds involved in ozone depletion and/or climate forcing, from the very volatile perfluorocarbons (PFCs, e.g., CF(4) and CH(3)CF(3)) and hydrofluorocarbons (HFCs, e.g., CH(3)CF(3)) to the higher-boiling point solvents (such as CH(3)Cl(3) and CCl(2)=CCl(2)) and CHBr(3). A network of Medusa systems worldwide provides 12 in situ ambient air measurements per day of more than 38 compounds of part per trillion mole fractions and precisions up to 0.1% RSD at the five remote field stations operated by the Advanced Global Atmospheric Gases Experiment (AGAGE). This custom system couples gas chromatography/mass spectrometry (GC/MSD) with a novel scheme for cryogen-free low-temperature preconcentration (-165 degrees C) of analytes from 2 L samples in a two-trap process using HayeSep D adsorbent.

  6. A sparse reconstruction method for the estimation of multi-resolution emission fields via atmospheric inversion

    DOE PAGES

    Ray, J.; Lee, J.; Yadav, V.; ...

    2015-04-29

    Atmospheric inversions are frequently used to estimate fluxes of atmospheric greenhouse gases (e.g., biospheric CO2 flux fields) at Earth's surface. These inversions typically assume that flux departures from a prior model are spatially smoothly varying, which are then modeled using a multi-variate Gaussian. When the field being estimated is spatially rough, multi-variate Gaussian models are difficult to construct and a wavelet-based field model may be more suitable. Unfortunately, such models are very high dimensional and are most conveniently used when the estimation method can simultaneously perform data-driven model simplification (removal of model parameters that cannot be reliably estimated) and fitting.more » Such sparse reconstruction methods are typically not used in atmospheric inversions. In this work, we devise a sparse reconstruction method, and illustrate it in an idealized atmospheric inversion problem for the estimation of fossil fuel CO2 (ffCO2) emissions in the lower 48 states of the USA. Our new method is based on stagewise orthogonal matching pursuit (StOMP), a method used to reconstruct compressively sensed images. Our adaptations bestow three properties to the sparse reconstruction procedure which are useful in atmospheric inversions. We have modified StOMP to incorporate prior information on the emission field being estimated and to enforce non-negativity on the estimated field. Finally, though based on wavelets, our method allows for the estimation of fields in non-rectangular geometries, e.g., emission fields inside geographical and political boundaries. Our idealized inversions use a recently developed multi-resolution (i.e., wavelet-based) random field model developed for ffCO2 emissions and synthetic observations of ffCO2 concentrations from a limited set of measurement sites. We find that our method for limiting the estimated field within an irregularly shaped region is about a factor of 10 faster than conventional approaches. It also

  7. Linearly Supporting Feature Extraction for Automated Estimation of Stellar Atmospheric Parameters

    NASA Astrophysics Data System (ADS)

    Li, Xiangru; Lu, Yu; Comte, Georges; Luo, Ali; Zhao, Yongheng; Wang, Yongjun

    2015-05-01

    We describe a scheme to extract linearly supporting (LSU) features from stellar spectra to automatically estimate the atmospheric parameters {{T}{\\tt{eff} }}, log g, and [Fe/H]. “Linearly supporting” means that the atmospheric parameters can be accurately estimated from the extracted features through a linear model. The successive steps of the process are as follow: first, decompose the spectrum using a wavelet packet (WP) and represent it by the derived decomposition coefficients; second, detect representative spectral features from the decomposition coefficients using the proposed method Least Absolute Shrinkage and Selection Operator (LARS)bs; third, estimate the atmospheric parameters {{T}{\\tt{eff} }}, log g, and [Fe/H] from the detected features using a linear regression method. One prominent characteristic of this scheme is its ability to evaluate quantitatively the contribution of each detected feature to the atmospheric parameter estimate and also to trace back the physical significance of that feature. This work also shows that the usefulness of a component depends on both the wavelength and frequency. The proposed scheme has been evaluated on both real spectra from the Sloan Digital Sky Survey (SDSS)/SEGUE and synthetic spectra calculated from Kurucz's NEWODF models. On real spectra, we extracted 23 features to estimate {{T}{\\tt{eff} }}, 62 features for log g, and 68 features for [Fe/H]. Test consistencies between our estimates and those provided by the Spectroscopic Parameter Pipeline of SDSS show that the mean absolute errors (MAEs) are 0.0062 dex for log {{T}{\\tt{eff} }} (83 K for {{T}{\\tt{eff} }}), 0.2345 dex for log g, and 0.1564 dex for [Fe/H]. For the synthetic spectra, the MAE test accuracies are 0.0022 dex for log {{T}{\\tt{eff} }} (32 K for {{T}{\\tt{eff} }}), 0.0337 dex for log g, and 0.0268 dex for [Fe/H].

  8. [Quantitative estimation source of urban atmospheric CO2 by carbon isotope composition].

    PubMed

    Liu, Wei; Wei, Nan-Nan; Wang, Guang-Hua; Yao, Jian; Zeng, You-Shi; Fan, Xue-Bo; Geng, Yan-Hong; Li, Yan

    2012-04-01

    To effectively reduce urban carbon emissions and verify the effectiveness of currently project for urban carbon emission reduction, quantitative estimation sources of urban atmospheric CO2 correctly is necessary. Since little fractionation of carbon isotope exists in the transportation from pollution sources to the receptor, the carbon isotope composition can be used for source apportionment. In the present study, a method was established to quantitatively estimate the source of urban atmospheric CO2 by the carbon isotope composition. Both diurnal and height variations of concentrations of CO2 derived from biomass, vehicle exhaust and coal burning were further determined for atmospheric CO2 in Jiading district of Shanghai. Biomass-derived CO2 accounts for the largest portion of atmospheric CO2. The concentrations of CO2 derived from the coal burning are larger in the night-time (00:00, 04:00 and 20:00) than in the daytime (08:00, 12:00 and 16:00), and increase with the increase of height. Those derived from the vehicle exhaust decrease with the height increase. The diurnal and height variations of sources reflect the emission and transport characteristics of atmospheric CO2 in Jiading district of Shanghai.

  9. Biases in atmospheric CO2 estimates from correlated meteorology modeling errors

    NASA Astrophysics Data System (ADS)

    Miller, S. M.; Hayek, M. N.; Andrews, A. E.; Fung, I.; Liu, J.

    2015-03-01

    Estimates of CO2 fluxes that are based on atmospheric measurements rely upon a meteorology model to simulate atmospheric transport. These models provide a quantitative link between the surface fluxes and CO2 measurements taken downwind. Errors in the meteorology can therefore cause errors in the estimated CO2 fluxes. Meteorology errors that correlate or covary across time and/or space are particularly worrisome; they can cause biases in modeled atmospheric CO2 that are easily confused with the CO2 signal from surface fluxes, and they are difficult to characterize. In this paper, we leverage an ensemble of global meteorology model outputs combined with a data assimilation system to estimate these biases in modeled atmospheric CO2. In one case study, we estimate the magnitude of month-long CO2 biases relative to CO2 boundary layer enhancements and quantify how that answer changes if we either include or remove error correlations or covariances. In a second case study, we investigate which meteorological conditions are associated with these CO2 biases. In the first case study, we estimate uncertainties of 0.5-7 ppm in monthly-averaged CO2 concentrations, depending upon location (95% confidence interval). These uncertainties correspond to 13-150% of the mean afternoon CO2 boundary layer enhancement at individual observation sites. When we remove error covariances, however, this range drops to 2-22%. Top-down studies that ignore these covariances could therefore underestimate the uncertainties and/or propagate transport errors into the flux estimate. In the second case study, we find that these month-long errors in atmospheric transport are anti-correlated with temperature and planetary boundary layer (PBL) height over terrestrial regions. In marine environments, by contrast, these errors are more strongly associated with weak zonal winds. Many errors, however, are not correlated with a single meteorological parameter, suggesting that a single meteorological proxy is

  10. Multi-model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation Historical and Projected Changes

    NASA Technical Reports Server (NTRS)

    Lamarque, J.-F.; Dentener, F.; McConnell, J.; Ro, C.-U.; Shaw, M.; Vet, R.; Bergmann, D.; Cameron-Smith, P.; Doherty, R.; Faluvegi, G.; Ghan, S. J.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Plummer, D.; Shindell, D. T.; Stevenson, D. S.; Strode, S.; Zeng, G.

    2013-01-01

    We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice-core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present-day (year 2000 ACCMIP time-slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multi-model mean deposition of 50 Tg(N) yr1 from nitrogen oxide emissions, 60 Tg(N) yr1 from ammonia emissions, and 83 Tg(S) yr1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards misrepresentation of 1980 NH3 emissions over North America. Based on ice-core records, the 1850 deposition fluxes agree well with Greenland ice cores but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double 2000 in some scenarios and reaching 1300 mg(N) m2 yr1 averaged over regional to continental scale regions in RCP 2.6 and 8.5, 3050 larger than the values in any region currently (2000). The new ACCMIP deposition dataset provides novel, consistent and evaluated global gridded deposition fields for use in a wide range of climate and ecological studies.

  11. Sulfur deposition and cycling in two forests of the Georgia Piedmont

    SciTech Connect

    Cappellato, R. )

    1994-06-01

    Because of the increase in SO[sub 2] emissions in Georgia since the late 70's, a study was undertaken in adjacent deciduous and coniferous forests to estimate the atmospheric input and above-ground cycling of sulfur. During this study, which was conducted in 1988-89, total annual sulfur input to these forests was 17 kg/ha, which was comparable to sulfur inputs to other sites in the eastern United States. Dry deposition accounted for more than 50% of the total atmospheric sulfur input, and SO[sub 2] was the major source of dry deposition of the canopy. Net flux of sulfur in (throughfall flux minus precipitation flux) under the deciduous canopy was 1.8 times higher than that under the conferous canopy. Although the net sulfur throughfall flux was very similar to the total sulfur dry deposition in the deciduous forest, the net sulfur throughfall was only about half of the total sulfur dry deposition. The lower throughfall sulfur flux in the coniferous forest was attributed to retention of SO[sub 2] by the canopy. Lower sulfur concentration in needles from the litterfall (0.68 mg/g) than in needles from the canopy (1.38 mg/g) indicates that sulfur could be accumulating in coniferous wood. Total annual sulfur deposition to the forest floor by throughfall, stemflow, and litterfall was 2.3 and 1.3 times greater than the sulfur required by the deciduous and coniferous forests, respectively, for annual wood and foliage production.

  12. Adjoint-Based Methods for Estimating CO2 Sources and Sinks from Atmospheric Concentration Data

    NASA Technical Reports Server (NTRS)

    Andrews, Arlyn E.

    2003-01-01

    Work to develop adjoint-based methods for estimating CO2 sources and sinks from atmospheric concentration data was initiated in preparation for last year's summer institute on Carbon Data Assimilation (CDAS) at the National Center for Atmospheric Research in Boulder, CO. The workshop exercises used the GSFC Parameterized Chemistry and Transport Model and its adjoint. Since the workshop, a number of simulations have been run to evaluate the performance of the model adjoint. Results from these simulations will be presented, along with an outline of challenges associated with incorporating a variety of disparate data sources, from sparse, but highly precise, surface in situ observations to less accurate, global future satellite observations.

  13. Limitation of Ground-based Estimates of Solar Irradiance Due to Atmospheric Variations

    NASA Technical Reports Server (NTRS)

    Wen, Guoyong; Cahalan, Robert F.; Holben, Brent N.

    2003-01-01

    The uncertainty in ground-based estimates of solar irradiance is quantitatively related to the temporal variability of the atmosphere's optical thickness. The upper and lower bounds of the accuracy of estimates using the Langley Plot technique are proportional to the standard deviation of aerosol optical thickness (approx. +/- 13 sigma(delta tau)). The estimates of spectral solar irradiance (SSI) in two Cimel sun photometer channels from the Mauna Loa site of AERONET are compared with satellite observations from SOLSTICE (Solar Stellar Irradiance Comparison Experiment) on UARS (Upper Atmospheric Research Satellite) for almost two years of data. The true solar variations related to the 27-day solar rotation cycle observed from SOLSTICE are about 0.15% at the two sun photometer channels. The variability in ground-based estimates is statistically one order of magnitude larger. Even though about 30% of these estimates from all Level 2.0 Cimel data fall within the 0.4 to approx. 0.5% variation level, ground-based estimates are not able to capture the 27-day solar variation observed from SOLSTICE.

  14. Estimating Bacteria Emissions from Inversion of Atmospheric Transport: Sensitivity to Modelled Particle Characteristics

    SciTech Connect

    Burrows, Susannah M.; Rayner, Perter; Butler, T.; Lawrence, M.

    2013-06-04

    Model-simulated transport of atmospheric trace components can be combined with observed concentrations to obtain estimates of ground-based sources using various inversion techniques. These approaches have been applied in the past primarily to obtain source estimates for long-lived trace gases such as CO2. We consider the application of similar techniques to source estimation for atmospheric aerosols, by using as a case study the estimation of bacteria emissions from different ecosystem regions in the global atmospheric chemistry and climate model ECHAM5/MESSy-Atmospheric Chemistry (EMAC). Simulated particle concentrations in the tropopause region and at high latitudes, as well as transport of particles to tundra and land ice regions are shown to be highly sensitive to scavenging in mixed-phase clouds, which is poorly characterized in most global climate models. This may be a critical uncertainty in correctly simulating the transport of aerosol particles to the Arctic. Source estimation via Monte Carlo Markov Chain is applied to a suite of sensitivity simulations and the global mean emissions are estimated. We present an analysis of the partitioning of uncertainties in the global mean emissions that are attributable to particle size, CCN activity, the ice nucleation scavenging ratios for mixed-phase and cold clouds, and measurement error. Uncertainty due to CCN activity or to a 1 um error in particle size is typically between 10% and 40% of the uncertainty due to data uncertainty, as measured by the 5%-ile to 95%-ile range of the Monte Carlo ensemble. Uncertainty attributable to the ice nucleation scavenging ratio in mized-phase clouds is as high as 10% to 20% of the data uncertainty. Taken together, the four model 20 parameters examined contribute about half as much to the uncertainty in the estimated emissions as do the measurements. This was a surprisingly large contribution from model uncertainty in light of the substantial data uncertainty, which ranges from 81

  15. Radar Estimations of Atmospheric Winds in the Troposphere and Lower Stratosphere

    NASA Astrophysics Data System (ADS)

    Sheppard, Emory Lamar

    This dissertation deals with the estimation of atmospheric flow field parameters using the spaced antenna (SA) and spatial interferometer (SI) methods. In the first section, a computer simulation of scattering from inhomogeneities in the refractive index is used to compare the SA and SI methods for measuring winds in clear air both with and without turbulent fading. The results show that the SA analysis which is carried out in the time domain and the SI analysis which is carried out in the frequency domain are equivalent in terms of the information that the two methods yield. A data analysis method equivalent to full correlation analysis, which can be carried out in the frequency domain, is presented. The method is applied to model-generated data in order to extract the typical full correlation analysis output parameters such as the apparent and true velocities. The results obtained are consistent with the model input parameters. In the second section a statistical comparison of the SA and SI methods for estimating horizontal winds in the troposphere and the lower stratosphere is presented. The data analyzed were obtained with the Middle and Upper (MU) atmosphere radar from 1910 LT on June 29, 1990, through 0950 LT on July 2, 1990. At all heights, velocity estimates based on frequency domain data are within 4% of those based on time domain data. We conclude that frequency domain techniques provide an alternate method for estimating true horizontal velocity. Nevertheless, it is not clear that they offer any significant advantage over time domain methods. In fact, the results obtained indicate that the SI method for estimating horizontal velocity may be slightly more difficult to apply in practice. The final section presents an analytical evaluation of SA-based instrumental setups with the potential for estimating the vertical component of atmospheric vorticity from a single-radar location. Methods considered are the oblique spaced antenna (OAS) method and a modified

  16. Correcting atmospheric effects in thermal ground observations for hyperspectral emissivity estimation

    NASA Astrophysics Data System (ADS)

    Timmermans, Joris; Buitrago, Maria

    2014-05-01

    Knowledge of Land surface temperature is of crucial importance in energy balance studies and environmental modeling. Accurate retrieval of land surface temperature (LST) demands detailed knowledge of the land surface emissivity. Measured radiation by remote sensing sensors to land surface temperature can only be performed using a-priori knowledge of the emissivity. Uncertainties in the retrieval of this emissivity can cause huge errors in LST estimations. The retrieval of emissivity (and LST) is per definition an underdetermined inversion, as only one observation is made while two variables are to be estimated. Several researches have therefore been performed on measuring emissivity, such as the normalized emissivity method, the temperature-emissivity separation (TES) using the minimum and maximum difference of emissivity and the use of vegetation indices. In each of these approaches atmospherically corrected radiance measurements by remote sensing sensors are correlated to ground measurements. Usually these ground measurements are performed with the ground equivalent of the remote sensing sensors; the CIMEL 312-2 has the same spectral bands as ASTER. This way parameterizations acquired this way are only usable for specific sensors and need to be redone for newer sensors. Recently hyperspectral thermal radiometers, such as the MIDAC, have been developed that can solve this problem. By using hyperspectral observations of emissivity, together with sensor simulators, ground measurements of different satellite sensor can be simulated. This facilitates the production of validation data for the different TES algorithms. However before such measurements can be performed extra steps of processing need to be performed. Atmospheric correction becomes more important in hyperspectral observations than for broadband observations, as energy levels measured per band is lower. As such the atmosphere has a relative larger contribution if bandwidths become smaller. The goal of this

  17. A Green Planet versus a Desert World: Estimating the Effect of Vegetation Extremes on the Atmosphere.

    NASA Astrophysics Data System (ADS)

    Fraedrich, Klaus; Kleidon, Axel; Lunkeit, Frank

    1999-10-01

    The effect of vegetation extremes on the general circulation is estimated by two atmospheric GCM simulations using global desert and forest boundary conditions over land. The difference between the climates of a `green planet' and a `desert world' is dominated by the changes of the hydrological cycle, which is intensified substantially. Enhanced evapotranspiration over land reduces the near-surface temperatures; enhanced precipitation leads to a warmer mid- and upper troposphere extending from the subtropics (induced by ITCZ, monsoon, and Hadley cell dynamics) to the midlatitudes (over the cyclogenesis area of Northern Hemisphere storm tracks). These regional changes of the surface water and energy balances, and of the atmospheric circulation, have potential impact on the ocean and the atmospheric greenhouse.

  18. Depletions of sulfur and/or zinc in IDPs: Are they reliable indicators of atmospheric entry heating?

    NASA Technical Reports Server (NTRS)

    Flynn, G. J.; Sutton, S. R.; Bajt, S.; Kloeck, W.; Thomas, K. L.; Keller, L. P.

    1993-01-01

    The degree of heating of interplanetary dust particles (IDP's) on Earth atmospheric entry is important in distinguishing cometary particles from main-belt asteroidal particles. Depletions in the volatile elements S and Zn were proposed as chemical indicators of significant entry heating. The S and Zn contents of cosmic dust particles were correlated with physical indicators of atmospheric entry heating, such as the production of magnetite and the loss of solar wind implanted He. The results indicate that the Zn content of IDP's is a useful indicator of entry heating, but the S content seems to be less useful.

  19. State and Parameter Estimation for a Coupled Ocean--Atmosphere Model

    NASA Astrophysics Data System (ADS)

    Ghil, M.; Kondrashov, D.; Sun, C.

    2006-12-01

    The El-Nino/Southern-Oscillation (ENSO) dominates interannual climate variability and plays, therefore, a key role in seasonal-to-interannual prediction. Much is known by now about the main physical mechanisms that give rise to and modulate ENSO, but the values of several parameters that enter these mechanisms are an important unknown. We apply Extended Kalman Filtering (EKF) for both model state and parameter estimation in an intermediate, nonlinear, coupled ocean--atmosphere model of ENSO. The coupled model consists of an upper-ocean, reduced-gravity model of the Tropical Pacific and a steady-state atmospheric response to the sea surface temperature (SST). The model errors are assumed to be mainly in the atmospheric wind stress, and assimilated data are equatorial Pacific SSTs. Model behavior is very sensitive to two key parameters: (i) μ, the ocean-atmosphere coupling coefficient between SST and wind stress anomalies; and (ii) δs, the surface-layer coefficient. Previous work has shown that δs determines the period of the model's self-sustained oscillation, while μ measures the degree of nonlinearity. Depending on the values of these parameters, the spatio-temporal pattern of model solutions is either that of a delayed oscillator or of a westward propagating mode. Estimation of these parameters is tested first on synthetic data and allows us to recover the delayed-oscillator mode starting from model parameter values that correspond to the westward-propagating case. Assimilation of SST data from the NCEP-NCAR Reanalysis-2 shows that the parameters can vary on fairly short time scales and switch between values that approximate the two distinct modes of ENSO behavior. Rapid adjustments of these parameters occur, in particular, during strong ENSO events. Ways to apply EKF parameter estimation efficiently to state-of-the-art coupled ocean--atmosphere GCMs will be discussed.

  20. Constraining Methane Flux Estimates Using Atmospheric Observations of Methane and 1^3C in Methane

    NASA Astrophysics Data System (ADS)

    Mikaloff Fletcher, S. E.; Tans, P. P.; Miller, J. B.; Bruhwiler, L. M.

    2002-12-01

    Understanding the budget of methane is crucial to predicting climate change and managing earth's carbon reservoirs. Methane is responsible for approximately 15% of the anthropogenic greenhouse forcing and has a large impact on the oxidative capacity of Earth's atmosphere due to its reaction with hydroxyl radical. At present, many of the sources and sinks of methane are poorly understood due in part to the large spatial and temporal variability of the methane flux. Model simulations of methane mixing ratios using most process-based source estimates typically over-predict the latitudinal gradient of atmospheric methane relative to the observations; however, the specific source processes responsible for this discrepancy have not been identified definitively. The aim of this work is to use the isotopic signatures of the sources to attribute these discrepancies to a source process or group of source processes and create global and regional budget estimates that are in agreement with both the atmospheric observations of methane and 1^3C in methane. To this end, observations of isotopic ratios of 1^3C in methane and isotopic signatures of methane source processes are used in conjunction with an inverse model of the methane budget. Inverse modeling is a top-down approach which uses observations of trace gases in the atmosphere, an estimate of the spatial pattern of trace gas fluxes, and a model of atmospheric transport to estimate the sources and sinks. The atmospheric transport was represented by the TM3 three-dimensional transport model. The GLOBALVIEW 2001 methane observations were used along with flask measurements of 1^3C in methane at six of the CMDL-NOAA stations by INSTAAR. Initial results imply interesting differences from previous methane budget estimates. For example, the 1^3C isotope observations in methane call for an increase in southern hemisphere sources with a bacterial isotopic signature such as wetlands, rice paddies, termites, and ruminant animals. The

  1. Sulfur-rich Sediments

    NASA Astrophysics Data System (ADS)

    Goldhaber, M. B.

    2003-12-01

    Marine sediments with more than a few tenths of a percent of organic carbon, as well as organic-matter-bearing, nonmarine sediments with significant concentrations of sulfate in the depositional waters contain the mineral pyrite (FeS2). Pyrite, along with sulfur-bearing organic compounds, form indirectly through the metabolic activities of sulfate-reducing microorganisms. The geochemical transformations of sulfur in sediments leading to these products significantly impact the pathway of early sedimentary diagenesis, conditions for the localization of mineral deposits (Ohmoto and Goldhaber, 1997), the global cycling of sulfur and carbon, the abundance of oxygen in the Earth's atmosphere, and perhaps even the emergence of life on Earth (e.g., Russell and Hall, 1997). This chapter provides an overview of sedimentary-sulfur geochemistry from its microbial and abiologic pathways to the global consequences of these processes.The geochemistry of sulfur is complicated by its wide range of oxidation states (Table 1). Under oxidizing conditions (e.g., in the presence of atmospheric oxygen) sulfate, with sulfur in the +6 valence state, is the stable form of sulfur. Under reducing conditions (e.g., in the presence of H2), sulfide (S=-2 valent) is the stable oxidation state. However, a range of additional aqueous and solid-phase sulfur species exist with valences between these two end-members. What makes the study of sulfur geochemistry so exciting and challenging is that many of these intermediate-valent forms play key roles in sedimentary-sulfur transformations. Furthermore, many of these reactions are microbially mediated. As detailed below, these complex biogeochemical pathways are now yielding to research whose scope ranges from molecular to global level. Table 1. Forms of sulfur in marine sediments and their oxidation states Aqueous species or mineralFormulaOxidation state(s) of sulfur SulfideH2S(aq), HS-(aq)-2 Iron sulfideaFeS(s)-2 GreigiteFe3S4(s)-2, 0 PyriteFeS2(s)-2

  2. Atmospheric channel transfer function estimation from experimental free-space optical communications data

    NASA Astrophysics Data System (ADS)

    Reinhardt, Colin N.; Kuga, Yasuo; Ritcey, James A.; Ishimaru, Akira; Hammel, Stephen; Tsintikidis, Dimitris

    2011-09-01

    The performance of terrestrial free-space optical communications systems is severely impaired by atmospheric aerosol particle distributions where the particle size is on the order of the operating wavelength. For optical and near-infrared wavelengths, fog droplets cause multiple-scattering and absorption effects which rapidly degrade received symbol detection performance as the optical depth parameter increases (visibility decreases). Using a custom free-space optical communications system we measured field data in fog within the optical multiple-scattering regime. We investigate the behavior of the estimated channel transfer function using both real field-test data and simulated propagation data based on field-test conditions. We then compare the channel transfer function estimates against the predictions computed using a radiative-transfer theory model-based approach which we also developed previously for the free-space optical atmospheric channel.

  3. Geodesy by radio interferometry - Effects of atmospheric modeling errors on estimates of baseline length

    NASA Technical Reports Server (NTRS)

    Davis, J. L.; Herring, T. A.; Shapiro, I. I.; Rogers, A. E. E.; Elgered, G.

    1985-01-01

    Analysis of very long baseline interferometry data indicates that systematic errors in prior estimates of baseline length, of order 5 cm for approximately 8000-km baselines, were due primarily to mismodeling of the electrical path length of the troposphere and mesosphere ('atmospheric delay'). Here observational evidence for the existence of such errors in the previously used models for the atmospheric delay is discussed, and a new 'mapping' function for the elevation angle dependence of this delay is developed. The delay predicted by this new mapping function differs from ray trace results by less than approximately 5 mm, at all elevations down to 5 deg elevation, and introduces errors into the estimates of baseline length of less than about 1 cm, for the multistation intercontinental experiment analyzed here.

  4. Accurate group velocity estimation for unmanned aerial vehicle-based acoustic atmospheric tomography.

    PubMed

    Rogers, Kevin J; Finn, Anthony

    2017-02-01

    Acoustic atmospheric tomography calculates temperature and wind velocity fields in a slice or volume of atmosphere based on travel time estimates between strategically located sources and receivers. The technique discussed in this paper uses the natural acoustic signature of an unmanned aerial vehicle as it overflies an array of microphones on the ground. The sound emitted by the aircraft is recorded on-board and by the ground microphones. The group velocities of the intersecting sound rays are then derived by comparing these measurements. Tomographic inversion is used to estimate the temperature and wind fields from the group velocity measurements. This paper describes a technique for deriving travel time (and hence group velocity) with an accuracy of 0.1% using these assets. This is shown to be sufficient to obtain highly plausible tomographic inversion results that correlate well with independent SODAR measurements.

  5. 40 CFR Appendix A to Part 50 - Reference Method for the Determination of Sulfur Dioxide in the Atmosphere (Pararosaniline Method)

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... at the sample manifold, with the excess flow vented at atmospheric pressure. The absorbers are then... calibration points. A data form (Figure 5) is supplied for easily organizing calibration data when the slope... sampled, std L (from Section 12.2). Data Form Calibration point no. Micro- grams So2 Absor- bance units...

  6. Sea ice-atmospheric interaction: Application of multispectral satellite data in polar surface energy flux estimates

    NASA Technical Reports Server (NTRS)

    Steffen, Konrad; Key, J.; Maslanik, J.; Schweiger, A.

    1993-01-01

    This is the third annual report on: Sea Ice-Atmosphere Interaction - Application of Multispectral Satellite Data in Polar Surface Energy Flux Estimates. The main emphasis during the past year was on: radiative flux estimates from satellite data; intercomparison of satellite and ground-based cloud amounts; radiative cloud forcing; calibration of the Advanced Very High Resolution Radiometer (AVHRR) visible channels and comparison of two satellite derived albedo data sets; and on flux modeling for leads. Major topics covered are arctic clouds and radiation; snow and ice albedo, and leads and modeling.

  7. Considerations on Estimating Upper Bounds of Neutron Doses Equivalents to Military Participants at Atmospheric Nuclear Tests

    DTIC Science & Technology

    2007-04-01

    Tissue kerma for monoenergetic neutrons of energy up to 14 MeV and contributions from different interactions that produce charged ionizing particles...fluence for each energy group obtained from calculations for monoenergetic neutrons similar to calculations in Figure 2-I, and the energy dependence of the...Considerations on Estimating Upper Bounds of Neutron Dose Equivalents to Military Partici pants at Atmospheric Nuclear Tests Approved for public release

  8. Estimating Dust and Water Ice Content of the Martian Atmosphere From THEMIS Data

    NASA Technical Reports Server (NTRS)

    Bandfield, Joshua

    2007-01-01

    Researchers at JPL and Arizona State University conducted a comparative study of three candidate algorithms for estimating components of the Martian atmosphere, using raw (uncalibrated) data collected by the Thermal Emission Imaging System (THEMIS). THEMIS is an instrument onboard the Mars Odyssey spacecraft that acquires image data in five visible and nine infrared (IR) wavelength bands. The algorithms under study used data collected from eight of the nine IR bands to estimate the dust and water ice content of the atmosphere. Such an algorithm could be used in onboard data processing to trigger other algorithms that search for features of scientific interest and to reduce the volume of data transmitted to Earth. The algorithms studied were based on regression models. In the study, the optical depths estimated by these algorithms were compared with optical depths estimated in ground-based processing using fully calibrated data from both THEMIS and the Thermal Emission Spectrometer (TES). TES is an instrument onboard the Mars Global Surveyor spacecraft that also observes the planet at infrared wavelengths, but at a lower spatial resolution than THEMIS does. Of the algorithms studied, the one that performed best was based on a Gaussian Support Vector Machine regression model. The test results indicated that this algorithm, operating on the raw data, had error rates that were within the uncertainty associated with the estimates obtained by the groundbased analysis of the fully calibrated data. This level of fidelity demonstrates that these algorithms are sufficiently accurate for use in an onboard setting.

  9. Radiance and atmosphere propagation-based method for the target range estimation

    NASA Astrophysics Data System (ADS)

    Cho, Hoonkyung; Chun, Joohwan

    2012-06-01

    Target range estimation is traditionally based on radar and active sonar systems in modern combat system. However, the performance of such active sensor devices is degraded tremendously by jamming signal from the enemy. This paper proposes a simple range estimation method between the target and the sensor. Passive IR sensors measures infrared (IR) light radiance radiating from objects in dierent wavelength and this method shows robustness against electromagnetic jamming. The measured target radiance of each wavelength at the IR sensor depends on the emissive properties of target material and is attenuated by various factors, in particular the distance between the sensor and the target and atmosphere environment. MODTRAN is a tool that models atmospheric propagation of electromagnetic radiation. Based on the result from MODTRAN and measured radiance, the target range is estimated. To statistically analyze the performance of proposed method, we use maximum likelihood estimation (MLE) and evaluate the Cramer-Rao Lower Bound (CRLB) via the probability density function of measured radiance. And we also compare CRLB and the variance of and ML estimation using Monte-Carlo.

  10. CarbonTracker-CH4: an assimilation system for estimating emissions of atmospheric methane

    NASA Astrophysics Data System (ADS)

    Bruhwiler, L.; Dlugokencky, E.; Masarie, K.; Ishizawa, M.; Andrews, A.; Miller, J.; Sweeney, C.; Tans, P.; Worthy, D.

    2014-08-01

    We describe an assimilation system for atmospheric methane (CH4), CarbonTracker-CH4, and demonstrate the diagnostic value of global or zonally averaged CH4 abundances for evaluating the results. We show that CarbonTracker-CH4 is able to simulate the observed zonal average mole fractions and capture inter-annual variability in emissions quite well at high northern latitudes (53-90° N). In contrast, CarbonTracker-CH4 is less successful in the tropics where there are few observations and therefore misses significant variability and is more influenced by prior flux estimates. CarbonTracker-CH4 estimates of total fluxes at high northern latitudes are about 81 ± 7 Tg CH4 yr-1, about 12 Tg CH4 yr-1 (13%) lower than prior estimates, a result that is consistent with other atmospheric inversions. Emissions from European wetlands are decreased by 30%, a result consistent with previous work by Bergamaschi et al. (2005); however, unlike their results, emissions from wetlands in boreal Eurasia are increased relative to the prior estimate. Although CarbonTracker-CH4 does not estimate an increasing trend in emissions from high northern latitudes for 2000 through 2010, significant inter-annual variability in high northern latitude fluxes is recovered. Exceptionally warm growing season temperatures in the Arctic occurred in 2007, a year that was also anonymously wet. Estimated emissions from natural sources were greater than the decadal average by 4.4 ± 3.8 Tg CH4 yr-1 in 2007. CarbonTracker-CH4 estimates for temperate latitudes are only slightly increased over prior estimates, but about 10 Tg CH4 yr-1 is redistributed from Asia to North America. This difference exceeds the estimated uncertainty for North America (±3.5 Tg CH4 yr-1). We used time invariant prior flux estimates, so for the period from 2000 to 2006, when the growth rate of global atmospheric CH4 was very small, the assimilation does not produce increases in natural or anthropogenic emissions in contrast to bottom

  11. Estimating European historical production, consumption and atmospheric emissions of decabromodiphenyl ether.

    PubMed

    Earnshaw, Mark R; Jones, Kevin C; Sweetman, Andy J

    2013-03-01

    A European scale production, consumption and environmental emissions inventory is produced for decabromodiphenyl ether (DecaBDE) for the period 1970-2020. A dynamic substance flow analysis model of DecaBDE is developed and emission of the main congener, BDE-209, to environmental compartments is estimated. From 1970 to 2010, it is estimated that a total of 185,000-250,000 tonnes of DecaBDE was consumed in Europe. Consumption peaked in the late 1990s at approximately 9,000 tonnes/year and has declined by ~30% in 2010. Predicted BDE-209 atmospheric emissions peak in 2004 at 10 tonnes/year. The waste management phase of the BDE-209 life cycle is responsible for the majority of atmospheric emissions via volatilisation and particle bound emissions from landfills, whilst leakage from Sewerage systems is the major source of emissions to the hydrosphere. Use of sewage sludge from wastewater treatment works as an agricultural fertiliser is the most important pathway of BDE-209 to soil. Although DecaBDE consumption has declined in recent years, the stock in use for 2010 remains considerable (60,000 tonnes) and is likely to act as a source of atmospheric emissions for several decades. Uncertainties exist in these estimations and more field or experimental data is needed to clarify the significance of certain emission pathways, in particular, emissions from landfill sites.

  12. Vibronic origin of sulfur mass-independent isotope effect in photoexcitation of SO2 and the implications to the early earth’s atmosphere

    PubMed Central

    Whitehill, Andrew R.; Xie, Changjian; Hu, Xixi; Xie, Daiqian; Guo, Hua; Ono, Shuhei

    2013-01-01

    Signatures of mass-independent isotope fractionation (MIF) are found in the oxygen (16O,17O,18O) and sulfur (32S, 33S, 34S, 36S) isotope systems and serve as important tracers of past and present atmospheric processes. These unique isotope signatures signify the breakdown of the traditional theory of isotope fractionation, but the physical chemistry of these isotope effects remains poorly understood. We report the production of large sulfur isotope MIF, with Δ33S up to 78‰ and Δ36S up to 110‰, from the broadband excitation of SO2 in the 250–350-nm absorption region. Acetylene is used to selectively trap the triplet-state SO2 (3B1), which results from intersystem crossing from the excited singlet (1A2/1B1) states. The observed MIF signature differs considerably from that predicted by isotopologue-specific absorption cross-sections of SO2 and is insensitive to the wavelength region of excitation (above or below 300 nm), suggesting that the MIF originates not from the initial excitation of SO2 to the singlet states but from an isotope selective spin–orbit interaction between the singlet (1A2/1B1) and triplet (3B1) manifolds. Calculations based on high-level potential energy surfaces of the multiple excited states show a considerable lifetime anomaly for 33SO2 and 36SO2 for the low vibrational levels of the 1A2 state. These results demonstrate that the isotope selectivity of accidental near-resonance interactions between states is of critical importance in understanding the origin of MIF in photochemical systems. PMID:23836655

  13. Vibronic origin of sulfur mass-independent isotope effect in photoexcitation of SO2 and the implications to the early earth's atmosphere.

    PubMed

    Whitehill, Andrew R; Xie, Changjian; Hu, Xixi; Xie, Daiqian; Guo, Hua; Ono, Shuhei

    2013-10-29

    Signatures of mass-independent isotope fractionation (MIF) are found in the oxygen ((16)O,(17)O,(18)O) and sulfur ((32)S, (33)S, (34)S, (36)S) isotope systems and serve as important tracers of past and present atmospheric processes. These unique isotope signatures signify the breakdown of the traditional theory of isotope fractionation, but the physical chemistry of these isotope effects remains poorly understood. We report the production of large sulfur isotope MIF, with Δ(33)S up to 78‰ and Δ(36)S up to 110‰, from the broadband excitation of SO2 in the 250-350-nm absorption region. Acetylene is used to selectively trap the triplet-state SO2 ( (3)B1), which results from intersystem crossing from the excited singlet ( (1)A2/ (1)B1) states. The observed MIF signature differs considerably from that predicted by isotopologue-specific absorption cross-sections of SO2 and is insensitive to the wavelength region of excitation (above or below 300 nm), suggesting that the MIF originates not from the initial excitation of SO2 to the singlet states but from an isotope selective spin-orbit interaction between the singlet ( (1)A2/ (1)B1) and triplet ( (3)B1) manifolds. Calculations based on high-level potential energy surfaces of the multiple excited states show a considerable lifetime anomaly for (33)SO2 and (36)SO2 for the low vibrational levels of the (1)A2 state. These results demonstrate that the isotope selectivity of accidental near-resonance interactions between states is of critical importance in understanding the origin of MIF in photochemical systems.

  14. Use of personal-indoor-outdoor sulfur concentrations to estimate the infiltration factor and outdoor exposure factor for individual homes and persons.

    PubMed

    Wallace, Lance; Williams, Ron

    2005-03-15

    A study of personal, indoor, and outdoor exposure to PM2.5 and associated elements has been carried out for 37 residents of the Research Triangle Park area in North Carolina. Participants were selected from persons expected to be at elevated risk from exposure to particles, and included 29 persons with hypertension and 8 cardiac patients with implanted defibrillators. Participants were monitored for 7 consecutive days in each of four seasons. One goal of the study was to estimate the contribution of outdoor PM2.5 to indoor concentrations. This depends on the infiltration factor Finf, the fraction of outdoor PM2.5 remaining airborne after penetrating indoors. After confirming with our measurements the findings of previous studies that sulfur has few indoor sources, we estimated an average Finf for each house based on indoor/outdoor sulfur ratios. These estimates ranged from 0.26 to 0.87, with a median value of 0.55. Since these estimates apply only to particles of size similar to that of sulfur particles (0.06-0.5 microm diameter), and since larger particles (0.5-2.5 microm) have lower penetration rates and higher deposition rates, these estimates are likely to be higher than the true infiltration factors for PM2.5 as a whole. In summer when air conditioners were in use, the sulfur-based infiltration factor was at its lowest (averaging 0.50) for most homes, whereas the average Finf for the other three seasons was 0.62-0.63. Using the daily estimated infiltration factor for each house, we calculated the contribution of outdoor PM2.5 to indoor air concentrations. The indoor-generated contributions to indoor PM2.5 had a wider range (0-33 microg/m3) than the outdoor contributions (5-22 microg/m3). However, outdoor contributions exceeded the indoor-generated contributions in 27 of 36 homes. A second goal of the study was to determine the contribution of outdoor particles to personal exposure. This is determined by the "outdoor exposure factor" Fpex, the fraction of

  15. Perfluorocarbons in the global atmosphere: b) Emission estimates using inversions of atmospheric observations of tetrafluoromethane, hexafluoroethane, and octafluoropropane

    NASA Astrophysics Data System (ADS)

    Ganesan, A. L.; Muhle, J.; Rigby, M. L.; Miller, B. R.; Salameh, P. K.; Harth, C. M.; Greally, B. R.; O'Doherty, S. J.; Trudinger, C. M.; Porter, L. W.; Steele, P.; Krummel, P. B.; Petrenko, V. V.; Simmonds, P. G.; Fraser, P. J.; Prinn, R. G.; Weiss, R. F.

    2009-12-01

    The perfluorocarbons (PFCs) are long-lived potent greenhouse gases with mixing ratios that have been steadily increasing in the modern measurement record that extends from the 1970s. We present optimized emissions from 1973-present of three perfluorocarbons: tetrafluoromethane (CF4), hexafluoroethane (C2F6) and octafluoropropane (C3F8). The dominant sources of the PFCs are primary aluminum and semiconductor production. CF4 also has a significant pre-industrial abundance from the build-up of very small natural emissions. The inversions were performed with atmospheric measurements made by the Advanced Global Atmospheric Gases Experiment (AGAGE) network as well as using stored samples from the Commonwealth Scientific and Industrial Research Organization (CSIRO) Southern Hemisphere archive and from several Northern Hemisphere sources. Inverse estimates of surface flux were derived from the measurements using a discrete Kalman filter, the annual pulse method of Chen and Prinn (J. Geophys. Res., 111, D10307, doi:10.1029/2005JD006058), and a 2D 12-box chemical transport model. CF4 emissions have decreased from ~20 Gg/yr in 1981 to the present value of ~11 Gg/yr. Conversely, C2F6 and C3F8 exhibit an early increase in emissions, peaking much later around 2000 at ~3 Gg/yr and ~1 Gg/yr, respectively, and subsequently declining. The incongruity in the emission profiles is discussed in the context of different relative emissions of CF4 and the other measured PFCs from the two main sources, efforts by the aluminum industry to reduce the emission factor of CF4 (kg CF4 /ton Al), and published emission inventories. In all cases, over 90% of emissions are from the Northern Hemisphere.

  16. Is it possible to estimate atmospheric deposition of heavy metals by analysis of terrestrial mosses?

    PubMed

    Aboal, J R; Fernández, J A; Boquete, T; Carballeira, A

    2010-11-15

    Here we present a critical review of diverse research studies involving estimation of atmospheric deposition of heavy metals from the concentrations of the contaminants in terrestrial moss. The findings can be summarized as follows: i) significant correlations between the concentrations of contaminants in moss and bulk deposition were observed in only 40.1% of the cases in which the relationship was studied and in only 14.1% of the cases, the coefficient of correlation was >0.7; ii) some method-related problems were identified (i.e. small sample sizes, elimination of some data from the regression analyses, large distances between the moss sampling sites and the bulk precipitation collectors, differences in times of exposure of the moss samples and collection times for the bulk precipitation), so that the results of the studies may not be completely valid, and iii) evidence was found in the relevant literature that moss does not actually integrate the atmospheric deposition received. We also discuss the reason why, in accordance with the published data, bulk deposition cannot be correctly estimated by determination of the final concentrations of contaminants in the organism, such as the existence of different sources of contamination, the physicochemical characteristics of the sources of deposition, physicochemical processes to which the organism is subjected and the biological processes that take place in the moss. Taking into account the above findings, it was concluded that, except for certain elements and specific cases (i.e. Pb and Cd), atmospheric deposition of elements cannot be accurately estimated from the concentrations of metals and metalloids in moss tissues. However, the analysis of moss does provide information about the presence of contaminants in the atmosphere, their spatial and temporal patterns of distribution and how they are taken up by live organisms. Use of mosses is therefore recommended as a complementary (rather than an alternative

  17. Estimates of atmospheric CO2 in the Neoarchean-Paleoproterozoic from paleosols

    NASA Astrophysics Data System (ADS)

    Kanzaki, Yoshiki; Murakami, Takashi

    2015-06-01

    Atmospheric CO2 levels reflect Earth's surface temperatures directly, and have been discussed especially in association with the faint young Sun and Snowball Earth in the Precambrian. In addition, atmospheric O2 levels in the Precambrian have been estimated from paleosols, fossil weathering profiles, based on the estimates of atmospheric CO2 levels. Nevertheless, atmospheric CO2 levels in the Neoarchean and the Paleoproterozoic have remained as a debatable topic. In order to precisely estimate atmospheric CO2 levels in the Neoarchean-Paleoproterozoic, we developed a new method that calculates CO2 levels from the chemical compositions of paleosols. The new method (i) calculates the cation concentrations in porewaters at the time of weathering from those of paleosols, (ii) describes the relationships between partial pressure of atmospheric CO2 (PCO2), pH and cation concentrations based on the charge balance between the cations and anions including carbonate species in porewaters, and (iii) finally calculates PCO2 levels at a given temperature constraining pH by thermodynamics of weathering secondary-minerals. By applying the new method to modern weathering profiles, we obtained a good agreement between the calculated and observed PCO2 levels. The weathering rate deduced from the new method was proportional to PCO2 with fractional dependence of 0.18 and the apparent activation energy of weathering was 40-55 kJ mol-1, which is consistent with the laboratory and field results. The application to modern weathering and the formulated characteristics of weathering strongly indicate that the new method is valid and robust. The new method was then applied to eight paleosols formed in the Neoarchean-Paleoproterozoic. We made constraints on the local temperatures, at which the paleosols were formed, mainly by the temperature and solute-concentration relationships in the literature, because they should have been different between the paleosols and from the average global

  18. Regional river sulfur runoff

    SciTech Connect

    Husar, R.B.; Husar, J.D.

    1985-01-20

    The water and sulfur runoff data for 54 large river basins were assembled, covering 65% of the nondesert land area of the world. The sulfur concentration ranges from 0.5 mg S/L for the West African rivers Niger and Volta to 100 mg S/L in the Colorado River; the world average is 3.2 mg S/L. The concentrations in central and eastern Europe as well as central and eastern North America exceed 8 mg S/L. The sulfur runoff density is also highest in the river basins over these industrialized regions, exceeding 2 g S/m/sup 2//yr. However, high sulfur runoff density in excess of 3 g S/m/sup 2//yr is also measured over the Pacific islands New Zealand and New Guinea and the archipelagos of Indonesia and the Philippines. The natural background sulfur runoff was estimated by assuming that South America, Africa, Australia, and the Pacific Islands are unperturbed by man and that the average river sulfur concentration is in the range 1--3 mg S/L. Taking these background concentration values, the man-induced sulfur runoff for Europe ranges between 2 and 8 times the natural flow, and over North America, man's contribution ranges between 1 and 5 times the natural runoff. The global sulfur flow from nondesert land to the oceans and the Caspian Sea is estimated as 131 Tg S/yr, of which 46--85 Tg S/yr is attributed to natural causes. The regional river sulfur runoff pattern discussed in this paper does not have enough spatial resolution to be directly applicable to studies of the environmental effects of man-induced sulfur flows. However, it points to the continental-size regions where those perturbations are most evident and to the magnitude of the perturbations as expressed in units of the natural flows.

  19. Regional river sulfur runoff

    NASA Astrophysics Data System (ADS)

    Husar, Rudolf B.; Husar, Janja Djukic

    1985-01-01

    The water and sulfur runoff data for 54 large river basins were assembled, covering 65% of the nondesert land area of the world. The sulfur concentration ranges from 0.5 mg S/L for the West African rivers Niger and Volta to 100 mg S/L in the Colorado River; the world average is 3.2 mg S/L. The concentrations in central and eastern Europe as well as central and eastern North America exceed 8 mg S/L. The sulfur runoff density is also highest in the river basins over these industrialized regions, exceeding 2 g S/m2/yr. However, high sulfur runoff density in excess of 3 g S/m2/yr is also measured over the Pacific islands New Zealand and New Guinea and the archipelagos of Indonesia and the Philippines. The natural background sulfur runoff was estimated by assuming that South America, Africa, Australia, and the Pacific Islands are unperturbed by man and that the average river sulfur concentration is in the range 1-3 mg S/L. Taking these background concentration values, the man-induced sulfur runoff for Europe ranges between 2 and 8 times the natural flow, and over North America, man's contribution ranges between 1 and 5 times the natural runoff. The global sulfur flow from nondesert land to the oceans and the Caspian Sea is estimated as 131 Tg S/yr, of which 46-85 Tg S/yr is attributed to natural causes. The regional river sulfur runoff pattern discussed in this paper does not have enough spatial resolution to be directly applicable to studies of the environmental effects of man-induced sulfur flows. However, it points to the continental-size regions where those perturbations are most evident and to the magnitude of the perturbations as expressed in units of the natural flows.

  20. Emission rate estimation through data assimilation of gamma dose measurements in a Lagrangian atmospheric dispersion model.

    PubMed

    Tsiouri, V; Kovalets, I; Andronopoulos, S; Bartzis, J G

    2012-01-01

    This paper presents an efficient algorithm for estimating the unknown emission rate of radionuclides in the atmosphere following a nuclear accident. The algorithm is based on assimilation of gamma dose rate measured data in a Lagrangian atmospheric dispersion model. Such models are used in the framework of nuclear emergency response systems (ERSs). It is shown that the algorithm is applicable in both deterministic and stochastic modes of operation of the dispersion model. The method is evaluated by computational simulations of a 3-d field experiment on atmospheric dispersion of ⁴¹Ar emitted routinely from a research reactor. Available measurements of fluence rate (photons flux) in air are assimilated in the Lagrangian dispersion model DIPCOT and the ⁴¹Ar emission rate is estimated. The statistical analysis shows that the model-calculated emission rates agree well with the real ones. In addition the model-predicted fluence rates at the locations of the sensors, which were not used in the data assimilation procedure are in better agreement with the measurements. The first evaluation results of the method presented in this study show that the method performs satisfactorily and therefore it is applicable in nuclear ERSs provided that more comprehensive validation studies will be performed.

  1. Towards estimation of atmospheric tidal effects on the ionosphere via data assimilation

    NASA Astrophysics Data System (ADS)

    Solomentsev, Dmitry; Cherniak, Yakov; Titov, Anton; Khattatov, Boris; Khattatov, Vyacheslav

    2015-11-01

    The impact of atmospheric tides on the night time ionosphere is now being a subject of the extensive research within the scientific community. The plausible effect has been observed using the multiple space-borne instruments (e.g. COSMIC/FORMOSAT-3 constellation, TIMED GUVI and NASA IMAGE). Along with the observations, several modelling attempts has been undertaken to prove or refute the interrelation between the atmospheric tides and the wave-four longitudinal night time ionosphere structure. The scope of the current article is to assess the data assimilation ionosphere model capabilities in representing the longitudinal effect in the night time ionosphere induced by the DE3 atmospheric tide. Along with this, the core physics-based model capabilities in estimating the same effect are presented and discussed. For the current research, two periods were taken into consideration: the autumn equinox of the years 2006 and 2012. In the current article the data assimilation and physics-based models calculation results are presented and discussed along with the models' error estimation and analysis.

  2. Can we estimate the fog-top height from atmospheric turbulent measurements at surface?

    NASA Astrophysics Data System (ADS)

    Román-Cascón, Carlos; Yagüe, Carlos; Steeneveld, Gert-Jan; Sastre, Mariano; Arrillaga, Jon A.; Maqueda, Gregorio

    2016-04-01

    The knowledge of the fog-top height (fog thickness) can be very meaningful for aircraft maneuvers, data assimilation/validation of Numerical Weather Prediction models or nowcasting of fog dissipation. However, its value is usually difficult to determine and it is sometimes approximated with satellite data, ground remote-sensing instruments or atmospheric soundings. These instruments are expensive and their data not always available. In this work, we show how the fog-top height shows a linear correlation with atmospheric turbulent variables measured close to the surface. This relation is statistically calculated from observational data of several radiation-fog events at two research sites: The Research Centre for the Lower Atmosphere (CIBA) in Spain and the Cabauw Experimental Site for Atmospheric Research (CESAR) in The Netherlands. Thus, surface friction velocity and buoyancy heat flux are presented as potential indicators of fog thickness. These methods are also evaluated over a long-lasting radiation-fog event at CESAR. The proposed methods could be operationally implemented for providing a continuous estimation of fog-top height through the deployment of a sonic anemometer close to the surface.

  3. Modified ensemble Kalman filter for nuclear accident atmospheric dispersion: prediction improved and source estimated.

    PubMed

    Zhang, X L; Su, G F; Yuan, H Y; Chen, J G; Huang, Q Y

    2014-09-15

    Atmospheric dispersion models play an important role in nuclear power plant accident management. A reliable estimation of radioactive material distribution in short range (about 50 km) is in urgent need for population sheltering and evacuation planning. However, the meteorological data and the source term which greatly influence the accuracy of the atmospheric dispersion models are usually poorly known at the early phase of the emergency. In this study, a modified ensemble Kalman filter data assimilation method in conjunction with a Lagrangian puff-model is proposed to simultaneously improve the model prediction and reconstruct the source terms for short range atmospheric dispersion using the off-site environmental monitoring data. Four main uncertainty parameters are considered: source release rate, plume rise height, wind speed and wind direction. Twin experiments show that the method effectively improves the predicted concentration distribution, and the temporal profiles of source release rate and plume rise height are also successfully reconstructed. Moreover, the time lag in the response of ensemble Kalman filter is shortened. The method proposed here can be a useful tool not only in the nuclear power plant accident emergency management but also in other similar situation where hazardous material is released into the atmosphere.

  4. CarbonTracker-CH4: an assimilation system for estimating emissions of atmospheric methane

    NASA Astrophysics Data System (ADS)

    Bruhwiler, L. M.; Dlugokencky, E.; Masarie, K.; Ishizawa, M.; Andrews, A.; Miller, J.; Sweeney, C.; Tans, P.; Worthy, D.

    2014-01-01

    We describe an assimilation system for atmospheric methane (CH4), CarbonTracker-CH4, and demonstrate the diagnostic value of global or zonally averaged CH4 abundances for evaluating the results. We show that CarbonTracker-CH4 is able to simulate the observed zonal average mole fractions and capture inter-annual variability in emissions quite well at high northern latitudes (53-90° N). CarbonTracker-CH4 estimates of total fluxes at high northern latitudes are about 81 Tg CH4 yr-1, about 12 Tg CH4 yr-1 (13%) lower than prior estimates, a result that is consistent with other atmospheric inversions. Emissions from European wetlands are decreased by 30%, a result consistent with previous; however, emissions from wetlands in Boreal Eurasia are increased relative to the prior estimate. Although CarbonTracker-CH4 does not estimate increases in emissions from high northern latitudes for 2000 through 2010, significant inter-annual variability in high northern latitude fluxes is recovered. During the exceptionally warm Arctic summer of 2007, estimated emissions were greater than the decadal average by 4.4 Tg CH4 yr-1. In 2008, temperatures returned to more normal values over Arctic North America while they stayed above normal over Arctic Eurasia. CarbonTracker-CH4 estimates were 2.4 Tg CH4 yr-1 higher than the decadal average, and the anomalous emissions occurred over Arctic Eurasia, suggesting that the data allow discrimination between these two source regions. Also, the emission estimates respond to climate variability without having the system constrained by climate parameters. CarbonTracker-CH4 estimates for temperate latitudes are only slightly increased over prior estimates, but about 10 Tg CH4 yr-1 is redistributed from Asia to North America. We used time invariant prior flux estimates, so for the period from 2000 to 2006, when the growth rate of global atmospheric CH4 was very small, the assimilation does not produce increases in natural or anthropogenic emissions in

  5. Ice core sulfur and methanesulfonic acid (MSA) records from southern Greenland document North American and European air pollution and suggest a decline in regional biogenic sulfur emissions.

    NASA Astrophysics Data System (ADS)

    Pasteris, D. R.; McConnell, J. R.; Burkhart, J. F.; Saltzman, E. S.

    2014-12-01

    Sulfate aerosols have an important cooling effect on the Earth because they scatter sunlight back to space and form cloud condensation nuclei. However, understanding of the atmospheric sulfur cycle is incomplete, leading to uncertainty in the assessment of past, present and future climate forcing. Here we use annually resolved observations of sulfur and methanesulfonic acid (MSA) concentration in an array of precisely dated Southern Greenland ice cores to assess the history of sulfur pollution emitted from North America and Europe and the history of biogenic sulfate aerosol derived from the North Atlantic Ocean over the last 250 years. The ice core sulfur time series is found to closely track sulfur concentrations in North American and European precipitation since records began in 1965, and also closely tracks estimated sulfur emissions since 1850 within the air mass source region as determined by back trajectory analysis. However, a decline to near-preindustrial sulfur concentrations in the ice cores after 1995 that is not so extensive in the source region emissions indicates that there has been a change in sulfur cycling over the last 150 years. The ice core MSA time series shows a decline of 60% since the 1860s, and is well correlated with declining sea ice concentrations around Greenland, suggesting that the phytoplankton source of biogenic sulfur has declined due to a loss of marginal sea ice zone habitat. Incorporating the implied decrease in biogenic sulfur in our analysis improves the match between the ice core sulfur record and the source region emissions throughout the last 150 years, and solves the problem of the recent return to near-preindustrial levels in the Greenland ice. These findings indicate that the transport efficiency of sulfur air pollution has been relatively stable through the industrial era and that biogenic sulfur emissions in the region have declined.

  6. Static stability of the Jovian atmospheres estimated from moist adiabatic profiles

    NASA Astrophysics Data System (ADS)

    Sugiyama, Ko-ichiro; Odaka, Masatsugu; Kuramoto, Kiyoshi; Hayashi, Yoshi-Yuki

    2006-02-01

    The dependency of static stability N2 of the Jovian atmospheres on the abundances of condensible elements is considered by calculating the moist adiabatic profiles. An optimal minimization method of the Gibbs free energy is utilized to obtain equilibrium compositions in order to cover a variety of basic elements. It is shown that CH4 is one of the dominant contributors to producing a stable layer in the Uranian atmosphere. On Jupiter, R. K. Achterberg and A. P. Ingersoll (1989) have shown that, at low water abundances, N2 is proportional to the H2O abundance. In the present study, we show that this relationship does not hold when the H2O abundance is larger than approximately 5 × solar. A rough estimation of wave speed indicates that the abundance of 10 × solar is marginal to explain the SL9-induced wave speed as that of an internal gravity wave.

  7. Comparison of CO2 fluxes estimated using atmospheric and oceanic inversions, and role of fluxes and their interannual variability in simulating atmospheric CO2 concentrations

    NASA Astrophysics Data System (ADS)

    Patra, P. K.; Mikaloff Fletcher, S. E.; Ishijima, K.; Maksyutov, S.; Nakazawa, T.

    2006-07-01

    We use a time-dependent inverse (TDI) model to estimate regional sources and sinks of atmospheric CO2 from 64 and then 22 regions based on atmospheric CO2 observations at 87 stations. The air-sea fluxes from the 64-region atmospheric-CO2 inversion are compared with fluxes from an analogous ocean inversion that uses ocean interior observations of dissolved inorganic carbon (DIC) and other tracers and an ocean general circulation model (OGCM). We find that, unlike previous atmospheric inversions, our flux estimates in the southern hemisphere are generally in good agreement with the results from the ocean inversion, which gives us added confidence in our flux estimates. In addition, a forward tracer transport model (TTM) is used to simulate the observed CO2 concentrations using (1) estimates of fossil fuel emissions and a priori estimates of the terrestrial and oceanic fluxes of CO2, and (2) two sets of TDI model corrected fluxes. The TTM simulations of TDI model corrected fluxes show improvements in fitting the observed interannual variability in growth rates and seasonal cycles in atmospheric CO2. Our analysis suggests that the use of interannually varying (IAV) meteorology and a larger observational network have helped to capture the regional representation and interannual variabilities in CO2 fluxes realistically.

  8. Atmosphere-Truth Z-R Rainfall Estimates: A Fresh Approach to an Old Problem

    NASA Astrophysics Data System (ADS)

    Henz, J. F.

    2010-12-01

    Common modeling practice for basin calibration uses rainfall fields developed by the statistical use of surface rain gauge observed data or the direct application of NEXRAD National Weather Service WSR-88D Doppler radar Storm Total Rainfall or 1-hr rainfall estimations. Each of these approaches has significant limitations. Rain gages often lack sufficient spatial coverage to measure true storm intensity or the distribution of rainfall in a basin. The NWS WSR-88D Doppler radar algorithms are constantly being improved but still fail to deliver consistent rainfall estimates. Significant problems are caused by an under-estimation of warm coalescence rains and an over-estimation of rainfall in both dry environments and storms with hail contamination. Finally, storm updraft areas are frequently counted as raining portions of the storm producing immediate errors. The statistical techniques often under-estimate rainfall when the heavy rain core of the storm misses the rain gauges or if high winds cause an under-catchment of rainfall. Gauge-adjusted rainfall estimates are also dependant on the core of the storm being observed by a gauge. Statistical approaches often under-estimate rainfall producing insufficient runoff to drive the observed flooding runoffs. The Atmosphere-Truth ZR (ATZR) technique uses an atmosphere-truthed algorithm to produce highly accurate estimates of surface rainfall from Doppler radar data. This approach relies on using a cloud physics approach to determine the atmosphere’s ability to produce 15-min to hourly rain rates. The atmsopheric rainfall is utilizes surface, boundary layer and cloud layer observations of temperature and moisture from conventional National Weather Service observations. The depth of the thunderstorm updraft region that exceeds 0C is used with the precipitable water index and updraft speeds to provide estimates of 15-min to hourly rainfall rates from radar reflectivity areas in the storm greather than 50 dBZ. Rainfall rates

  9. Chlorophyll Concentration Estimates for Coastal Waters using Pixel-Based Atmospheric Correction of Landsat Images

    NASA Astrophysics Data System (ADS)

    Kouba, E.; Xie, H.

    2014-12-01

    Ocean color analysis is more challenging for coastal regions than the global ocean due the effects of optical brightness, shallow and turbid water, higher phytoplankton growth rates, and the complex geometry of coastal bays and estuaries. Also, one of the key atmospheric correction assumptions (zero water leaving radiance in the near infrared) is not valid for these complex conditions. This makes it difficult to estimate the spectral radiance noise caused by atmospheric aerosols, which can vary rapidly with time and space. This project evaluated using Landsat-7 ETM+ observations over a set of coastal bays, and allowing atmospheric correction calculations to vary with time and location as much as practical. Precise satellite orbit vector data was combined with operational weather and climate data to create interpolated arrays of atmospheric profiles which varied with time and location, allowing separate calculation of the Rayleigh and aerosol radiance corrections for all pixels. The resulting normalized water-leaving radiance values were compared with chlorophyll fluorescence measurements made at five in-situ stations inside a set of Texas coastal bays: the Mission-Aransas National Estuarine Research Reserve. Curve-fitting analysis showed it was possible to estimate chlorophyll surface area concentrations by using ETM+ water-leaving radiance values and a third-order polynomial equation. Two pairs of ETM+ bands were identified as inputs (Bands 1 and 3, and the Log10 values of Bands 3 and 4), both achieving R2 of 0.69. Additional research efforts were recommended to obtain additional data, identify better curve fitting equations, and potentially extend the radiative transfer model into the water column.

  10. Chlorophyll concentration estimates for coastal water using pixel-based atmospheric correction of Landsat images

    NASA Astrophysics Data System (ADS)

    Kouba, Eric

    Ocean color analysis is more challenging for coastal regions than the global ocean due the effects of optical brightness, shallow and turbid water, higher phytoplankton growth rates, and the complex geometry of coastal bays and estuaries. Also, one of the key atmospheric correction assumptions (zero water leaving radiance in the near infrared) is not valid for these complex conditions. This makes it difficult to estimate the spectral radiance noise caused by atmospheric aerosols, which can vary rapidly with time and space. This study conducts pixel-based atmospheric correction of Landsat-7 ETM+ images over the Texas coast. Precise satellite orbit data, operational weather data, and climate data are combined to create interpolated arrays of viewing angles and atmospheric profiles. These arrays vary with time and location, allowing calculation of the Rayleigh and aerosol radiances separately for all pixels. The resulting normalized water-leaving radiances are then compared with in situ chlorophyll fluorescence measurements from five locations inside a set of Texas coastal bays: the Mission-Aransas National Estuarine Research Reserve. Curve-fitting analysis shows it is possible to estimate chlorophyll-a surface area concentrations by using ETM+ water-leaving radiance values and a third-order polynomial equation. Two pairs of ETM+ bands are identified as inputs (Bands 1 and 3, and the Log10 values of Bands 3 and 4), both achieving good performance (R2 of 0.69). Further research efforts are recommended to obtain additional data, identify better curve fitting equations, and potentially extend the radiative transfer model into the water column.

  11. Estimation of methane fluxes in the high northern latitudes from a Bayesian atmospheric inversion

    NASA Astrophysics Data System (ADS)

    Thompson, R.; Stohl, A.; Lund myhre, C.; Sasakawa, M.; Machida, T.; Aalto, T.; Dlugokencky, E. J.; Worthy, D. E. J.

    2015-12-01

    Methane (CH4) is the second most important anthropogenic greenhouse gas after CO2. Globally, atmospheric CH4 concentrations have increased since direct measurements began, in the early 1980s, but then stabilized from the mid 1990s to the mid 2000s. Since 2007, the atmospheric CH4 growth rate has become positive again causing concern that it may be the response to climate feedbacks, especially in the Arctic, where there is a potential for a large release of CH4 to the atmosphere under warmer conditions. Such feedbacks include high latitude wetlands, permafrost and the destabilization of methane hydrates. We present CH4 emission estimates for the high northern latitudes (i.e., north of 50°N) from 2005 to 2012 using atmospheric mole fraction observations in a Bayesian inversion framework. This framework is based on the Lagrangian Particle Dispersion model, FLEXPART, run with ECMWF meteorological analyses. Emissions were optimized monthly and on a spatial grid of variable resolution. Background mixing ratios were found by coupling FLEXPART to output from the optimized Eulerian chemistry transport model, TM5. Meteorological models tend to overestimate the boundary layer heights (BLH) in the Arctic, especially in winter, which can lead to biases in the estimated fluxes. Therefore, we explored a number of data selection criteria to avoid assimilating data at times when significant errors in BLH were likely. Overall, the inversion found higher emissions in Northern Eurasia and North America compared to the prior in both summer and winter. The inversion fluxes also displayed considerable inter-annual variability, which appears to be related to climate variability.

  12. On-line estimation of error covariance parameters for atmospheric data assimilation

    NASA Technical Reports Server (NTRS)

    Dee, Dick P.

    1995-01-01

    A simple scheme is presented for on-line estimation of covariance parameters in statistical data assimilation systems. The scheme is based on a maximum-likelihood approach in which estimates are produced on the basis of a single batch of simultaneous observations. Simple-sample covariance estimation is reasonable as long as the number of available observations exceeds the number of tunable parameters by two or three orders of magnitude. Not much is known at present about model error associated with actual forecast systems. Our scheme can be used to estimate some important statistical model error parameters such as regionally averaged variances or characteristic correlation length scales. The advantage of the single-sample approach is that it does not rely on any assumptions about the temporal behavior of the covariance parameters: time-dependent parameter estimates can be continuously adjusted on the basis of current observations. This is of practical importance since it is likely to be the case that both model error and observation error strongly depend on the actual state of the atmosphere. The single-sample estimation scheme can be incorporated into any four-dimensional statistical data assimilation system that involves explicit calculation of forecast error covariances, including optimal interpolation (OI) and the simplified Kalman filter (SKF). The computational cost of the scheme is high but not prohibitive; on-line estimation of one or two covariance parameters in each analysis box of an operational bozed-OI system is currently feasible. A number of numerical experiments performed with an adaptive SKF and an adaptive version of OI, using a linear two-dimensional shallow-water model and artificially generated model error are described. The performance of the nonadaptive versions of these methods turns out to depend rather strongly on correct specification of model error parameters. These parameters are estimated under a variety of conditions, including

  13. Methane fluxes in the high northern latitudes estimated using a Bayesian atmospheric inversion

    NASA Astrophysics Data System (ADS)

    Thompson, Rona; Stohl, Andreas; Myhre, Cathrine Lund; Sasakawa, Motoki; Machida, Toshinobu; Aalto, Tuula; Dlugokencky, Edward; Worthy, Douglas; Skorokhod, Andrey

    2016-04-01

    Methane (CH4) is the second most important anthropogenic greenhouse gas after CO2. Atmospheric CH4 increased from pre-industrial concentrations of around 850 ppb (parts-per-billion) to 1773 ppb in the late 1990s and then remained approximately stable until the mid 2000s. However, since 2006 atmospheric CH4 has begun to increase again. The reasons for the stabilization and subsequent increase are likely to be a combination of changes in anthropogenic emissions such as from fossil fuels, as well as natural wetland sources. While global atmospheric inversions indicate that natural wetland sources in the tropics and subtropics have contributed to the recent increase, land surface and ecosystem models generally indicate no increase in these sources. Another potential source for the change in CH4 concentration could be wetlands in the high northern latitudes, which comprise about 44% of global wetland area. These latitudes are also undergoing rapid warming, which will impact wetland emissions of CH4. We present CH4 fluxes for the high northern latitudes (>50°N) from 2005 to 2012 estimated from a Bayesian atmospheric inversion. The inversion incorporates observations from 17 in-situ and 6 discrete-sample sites across North America and Northern Eurasia. Atmospheric transport is based on the Lagrangian particle dispersion model, FLEXPART, run with ECMWF meteorological analyses. Emissions were optimized monthly and on a spatial grid of variable resolution (from 1°×1° to 4°×4°). Background concentrations were estimated by coupling FLEXPART to monthly global 2-D fields of CH4 concentration from a bivariate interpolation of smoothed data from the NOAA ESRL network. We estimate the total mean North American flux (>50°N) to be 18 -- 27 Tg y-1, and the total mean Northern Eurasian flux (>50°N) to be 55 -- 66 Tg y-1, both substantially higher than the prior (based on LPX-Bern for wetland and EDGAR-4.2FT2010 for anthropogenic fluxes). We also find a small trend in the

  14. Estimating tropospheric phase delay in SAR interferograms using Global Atmospheric Models

    NASA Astrophysics Data System (ADS)

    Doin, M.; Lasserre, C.; Peltzer, G.; Cavalie, O.; Doubre, C.

    2008-12-01

    The main limiting factor on the accuracy of Interferometric SAR (InSAR) measurements comes from phase propagation delays through the Earth's troposphere. The delay can be divided into a stratified component, which correlates with the topography and often dominates the tropospheric signal in InSAR data, and a turbulent component. The stratified delay can be expressed as a function of atmospheric pressure P, temperature T, and water vapor partial pressure e vertical profiles. We compare the stratified delay computed using results from global atmospheric models with the topography-dependent signal observed in interferograms covering three test areas in different geographic and climatic environments: Lake Mead, Nevada, USA, the Haiyuan fault area, Gansu, China, and Afar, Republic of Djibouti. For each site we compute a multi-year series of interferograms. The phase-elevation ratio is estimated for each interferogram and the series is inverted to form a timeline of delay-elevation ratios characterizing each epoch of data acquisition. InSAR derived ratios are in good agreement with the ratios computed from global atmospheric models. This agreement shows that both estimations of the delay-elevation ratio can be used to perform a first order correction of the InSAR phase. Seasonal variations of the atmosphere significantly affect the phase delay throughout the year, aliasing the results of time series inversions using temporal smoothing or data stacking when the acquisitions are not evenly distributed in time. This is particularly critical when the spatial shape of the signal of interest correlates with topography. In the Lake Mead area, the irregular temporal sampling of our SAR data results in an interannual bias of amplitude ~2~cm on range change estimates. In the Haiyuan Fault area, the coarse and uneven data sampling results in a bias of up to ~0.5~cm/yr on the line of sight velocity across the fault. In the Afar area, the seasonal signal exceeds the deformation

  15. An attempt at estimating Paris area CO2 emissions from atmospheric concentration measurements

    NASA Astrophysics Data System (ADS)

    Bréon, F. M.; Broquet, G.; Puygrenier, V.; Chevallier, F.; Xueref-Rémy, I.; Ramonet, M.; Dieudonné, E.; Lopez, M.; Schmidt, M.; Perrussel, O.; Ciais, P.

    2014-04-01

    Atmospheric concentration measurements are used to adjust the daily to monthly budget of CO2 emissions from the AirParif inventory of the Paris agglomeration. We use 5 atmospheric monitoring sites including one at the top of the Eiffel tower. The atmospheric inversion is based on a Bayesian approach, and relies on an atmospheric transport model with a spatial resolution of 2 km with boundary conditions from a global coarse grid transport model. The inversion tool adjusts the CO2 fluxes (anthropogenic and biogenic) with a temporal resolution of 6 h, assuming temporal correlation of emissions uncertainties within the daily cycle and from day to day, while keeping the a priori spatial distribution from the emission inventory. The inversion significantly improves the agreement between measured and modelled concentrations. However, the amplitude of the atmospheric transport errors is often large compared to the CO2 gradients between the sites that are used to estimate the fluxes, in particular for the Eiffel tower station. In addition, we sometime observe large model-measurement differences upwind from the Paris agglomeration, which confirms the large and poorly constrained contribution from distant sources and sinks included in the prescribed CO2 boundary conditions These results suggest that (i) the Eiffel measurements at 300 m above ground cannot be used with the current system and (ii) the inversion shall rely on the measured upwind-downwind gradients rather than the raw mole fraction measurements. With such setup, realistic emissions are retrieved for two 30 day periods. Similar inversions over longer periods are necessary for a proper evaluation of the results.

  16. Neural Partial Differentiation for Aircraft Parameter Estimation Under Turbulent Atmospheric Conditions

    NASA Astrophysics Data System (ADS)

    Kuttieri, R. A.; Sinha, M.

    2012-07-01

    An approach based on neural partial differentiation is suggested for aircraft parameter estimation using the flight data gathered under turbulent atmospheric conditions. The classical methods such as output error and equation error methods suffer from severe convergence issues; resulting in biased, inaccurate, and inconsistent estimates. Though filter error method yields better estimates while dealing with the flight data having process noise, it has few demerits like computational overheads and it allows estimation of a single set of process noise distribution matrix. The proposed neural method does not face any such problem of the classical methods. Moreover, the neural method does not require parameter initialization and a priori knowledge of the model structure. The neural network maps the aircraft state and control variables into the output variables corresponding to aerodynamic forces and moments. The parameter estimation, pertaining to lateral-directional motion, of the research aircraft de Havilland DHC-2 with simulated process noise, is presented. The results obtained using the neural partial differentiation are compared with the nominal values given in literature and with the classical methods. The neural method yields the aerodynamic derivatives very close to the nominal values and having quite low standard deviation. The neural methodology is also validated by comparing actual output variables with the neural predicted and neural reconstructed variables.

  17. Impact of meteorological inflow uncertainty on tracer transport and source estimation in urban atmospheres

    NASA Astrophysics Data System (ADS)

    Lucas, Donald D.; Gowardhan, Akshay; Cameron-Smith, Philip; Baskett, Ronald L.

    2016-10-01

    A computational Bayesian inverse technique is used to quantify the effects of meteorological inflow uncertainty on tracer transport and source estimation in a complex urban environment. We estimate a probability distribution of meteorological inflow by comparing wind observations to Monte Carlo simulations from the Aeolus model. Aeolus is a computational fluid dynamics model that simulates atmospheric and tracer flow around buildings and structures at meter-scale resolution. Uncertainty in the inflow is propagated through forward and backward Lagrangian dispersion calculations to determine the impact on tracer transport and the ability to estimate the release location of an unknown source. Our uncertainty methods are compared against measurements from an intensive observation period during the Joint Urban 2003 tracer release experiment conducted in Oklahoma City. The best estimate of the inflow at 50 m above ground for the selected period has a wind speed and direction of 4.6-2.5+2.0 m s-1 and 158.0-23+16 , where the uncertainty is a 95% confidence range. The wind speed values prescribed in previous studies differ from our best estimate by two or more standard deviations. Inflow probabilities are also used to weight backward dispersion plumes and produce a spatial map of likely tracer release locations. For the Oklahoma City case, this map pinpoints the location of the known release to within 20 m. By evaluating the dispersion patterns associated with other likely release locations, we further show that inflow uncertainty can explain the differences between simulated and measured tracer concentrations.

  18. Multi-model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation of Historical and Projected Future Changes

    SciTech Connect

    Lamarque, Jean-Francois; Dentener, Frank; McConnell, J.R.; Ro, C-U; Shaw, Mark; Vet, Robert; Bergmann, D.; Cameron-Smith, Philip; Dalsoren, S.; Doherty, R.; Faluvegi, G.; Ghan, Steven J.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Plummer, David; Shindell, Drew; Skeie, R. B.; Stevenson, D. S.; Strode, S.; Zeng, G.; Curran, M.; Dahl-Jensen, D.; Das, S.; Fritzsche, D.; Nolan, M.

    2013-08-20

    We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice-core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present-day (year 2000 ACCMIP time-slice), the ACCMIP results perform similarly to previously published multi-model assessments. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States, but less so over Europe. This difference points towards misrepresentation of 1980 NH3 emissions over North America. Based on ice-core records, the 1850 deposition fluxes agree well with Greenland ice cores but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double 2000 in some scenarios and reaching >1300 mgN/m2/yr averaged over regional to continental scale regions in RCP 2.6 and 8.5, ~30-50% larger than the values in any region currently (2000). Despite known issues, the new ACCMIP deposition dataset provides novel, consistent and evaluated global gridded deposition fields for use in a wide range of climate and ecological studies.

  19. A simple algorithm to estimate the effective regional atmospheric parameters for thermal-inertia mapping

    USGS Publications Warehouse

    Watson, K.; Hummer-Miller, S.

    1981-01-01

    A method based solely on remote sensing data has been developed to estimate those meteorological effects which are required for thermal-inertia mapping. It assumes that the atmospheric fluxes are spatially invariant and that the solar, sky, and sensible heat fluxes can be approximated by a simple mathematical form. Coefficients are determined from least-squares method by fitting observational data to our thermal model. A comparison between field measurements and the model-derived flux shows the type of agreement which can be achieved. An analysis of the limitations of the method is also provided. ?? 1981.

  20. To estimation of the fluxes of carbon dioxide in the Lake Baikal water-atmosphere system

    NASA Astrophysics Data System (ADS)

    Pestunov, D. A.; Panchenko, Mikhail V.; Domysheva, V. M.; Belan, Boris D.

    2004-12-01

    Separate many-day series of measurements of the carbon dioxide concentration were carried out at the stationary site of the Limnological Institute SB RAS near village Bol"shie Koty in July, August and October 2003. The CO2 fluxes from the water surface are estimated. Maximum amplitude of the diurnal variations of the CO2 concentration in the chamber in August was 100 ppmV, and minimum was 45 ppmV. Comparison with the results of measurements in the atmosphere and the data on the CO2 content in the near-surface water of Lake Baikal is performed.

  1. A case study of the relative effects of power plant nitrogen oxides and sulfur dioxide emission reductions on atmospheric nitrogen deposition.

    PubMed

    Vijayaraghavan, Krish; Seigneur, Christian; Bronson, Rochelle; Chen, Shu-Yun; Karamchandani, Prakash; Walters, Justin T; Jansen, John J; Brandmeyer, Jo Ellen; Knipping, Eladio M

    2010-03-01

    The contrasting effects of point source nitrogen oxides (NOx) and sulfur dioxide (SO2) air emission reductions on regional atmospheric nitrogen deposition are analyzed for the case study of a coal-fired power plant in the southeastern United States. The effect of potential emission reductions at the plant on nitrogen deposition to Escambia Bay and its watershed on the Florida-Alabama border is simulated using the three-dimensional Eulerian Community Multiscale Air Quality (CMAQ) model. A method to quantify the relative and individual effects of NOx versus SO2 controls on nitrogen deposition using air quality modeling results obtained from the simultaneous application of NOx and SO2 emission controls is presented and discussed using the results from CMAQ simulations conducted with NOx-only and SO2-only emission reductions; the method applies only to cases in which ambient inorganic nitrate is present mostly in the gas phase; that is, in the form of gaseous nitric acid (HNO3). In such instances, the individual effects of NOx and SO2 controls on nitrogen deposition can be approximated by the effects of combined NOx + SO2 controls on the deposition of NOy, (the sum of oxidized nitrogen species) and reduced nitrogen species (NHx), respectively. The benefit of controls at the plant in terms of the decrease in nitrogen deposition to Escambia Bay and watershed is less than 6% of the overall benefit due to regional Clean Air Interstate Rule (CAIR) controls.

  2. Observation of vanadyl porphyrins and sulfur-containing vanadyl porphyrins in a petroleum asphaltene by atmospheric pressure photonionization Fourier transform ion cyclotron resonance mass spectrometry.

    PubMed

    Qian, Kuangnan; Mennito, Anthony S; Edwards, Kathleen E; Ferrughelli, Dave T

    2008-07-01

    Vanadyl (VO) porphyrins and sulfur-containing vanadyl (VOS) porphyrins of a wide carbon number range (C(26) to C(52)) and Z-number range (-28 to -54) were detected and identified in a petroleum asphaltene by atmospheric pressure photonionization (APPI) and Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). APPI provides soft ionization of asphaltene molecules (including VO and VOS porphyrins), generating primarily molecular ions (M(+.)). The ultra-high mass resolving power (m/Delta m(FWHM) approximately 500 K) of FTICR-MS enabled resolution and positive identification of elemental formulae for the entire family of VO and VOS porphyrins in a complicated asphaltene matrix. Deocophylerythro-etioporphyrin (DPEP) is found to be the most prevalent structure, followed by etioporphyrins (etio)- and rhodo (benzo)-DPEP. The characteristic Z-distribution of VO porphyrins suggests benzene and naphthene increment in the growth of porphyrin ring structures. Bimodal carbon number distributions of VO porphyrins suggest possible different origins of low and high molecular weight species. To our knowledge, the observation of VOS porphyrins in a petroleum product has not previously been reported. The work is also the first direct identification of the entire vanadyl porphyrin family by ultra-high resolution mass spectrometry without chromatographic separation or demetallation.

  3. Atmospheric wet deposition of nitrogen and sulfur to a typical red soil agroecosystem in Southeast China during the ten-year monsoon seasons (2003-2012)

    NASA Astrophysics Data System (ADS)

    Cui, Jian; Zhou, Jing; Peng, Ying; He, Yuanqiu; Yang, Hao; Mao, Jingdong

    2014-01-01

    Biological processes in agroecosystems have been affected by atmospheric nitrogen (N) and sulfur (S) deposition, but there is uncertainty about their deposition characteristics in the monsoon season. We collected rain samples using an ASP-2 sampler, recorded rainfall and rain frequency by an auto-meteorological experiment sub-station, and determined total N, NO3--N and NH4+-N levels in precipitation with an AutoAnalyzer 3 and SO42--S with a chromatography, in order to characterize the wet deposition of N and S to a typical red soil agroecosystem by a ten-year monitoring experiment in Southeast China. The results indicated that N and S wet deposition had an increased trend with the flux of total N (3.34-65.17 kg ha-1 N) and total S (SO42--S) (7.17-23.44 kg ha-1 S) during the monsoon seasons. The additional applications of pig mature in 2006 and 2007 led to the peaks of DON (dissolved organic nitrogen) and total N wet deposition. On average, NH4+-N was the major N form, accounting for 48.5% of total N wet deposition and DON was not a negligible N form, accounting for 20.8% during the ten-year monsoon seasons (except 2006 and 2007). Wet deposition of N and S has been intensively influenced by human activities in the monsoon season, and would increase the potential ecological risk in the red soil agricultural ecosystem.

  4. Biomass burning in Asia : annual and seasonal estimates and atmospheric emissions.

    SciTech Connect

    Streets, D. G.; Yarber, K. F.; Woo, J.-H.; Carmichael, G. R.; Decision and Information Sciences; Univ. of Iowa

    2003-10-15

    Estimates of biomass burning in Asia are developed to facilitate the modeling of Asian and global air quality. A survey of national, regional, and international publications on biomass burning is conducted to yield consensus estimates of 'typical' (i.e., non-year-specific) estimates of open burning (excluding biofuels). We conclude that 730 Tg of biomass are burned in a typical year from both anthropogenic and natural causes. Forest burning comprises 45% of the total, the burning of crop residues in the field comprises 34%, and 20% comes from the burning of grassland and savanna. China contributes 25% of the total, India 18%, Indonesia 13%, and Myanmar 8%. Regionally, forest burning in Southeast Asia dominates. National, annual totals are converted to daily and monthly estimates at 1{sup o} x 1{sup o} spatial resolution using distributions based on AVHRR fire counts for 1999--2000. Several adjustment schemes are applied to correct for the deficiencies of AVHRR data, including the use of moving averages, normalization, TOMS Aerosol Index, and masks for dust, clouds, landcover, and other fire sources. Good agreement between the national estimates of biomass burning and adjusted fire counts is obtained (R{sup 2} = 0.71--0.78). Biomass burning amounts are converted to atmospheric emissions, yielding the following estimates: 0.37 Tg of SO{sub 2}, 2.8 Tg of NO{sub x}, 1100 Tg of CO{sub 2}, 67 Tg of CO, 3.1 Tg of CH{sub 4}, 12 Tg of NMVOC, 0.45 Tg of BC, 3.3 Tg of OC, and 0.92 Tg of NH{sub 3}. Uncertainties in the emission estimates, measured as 95% confidence intervals, range from a low of {+-}65% for CO{sub 2} emissions in Japan to a high of {+-}700% for BC emissions in India.

  5. Forest biomass estimation with hemispherical photography for multiple forest types and various atmospheric conditions

    NASA Astrophysics Data System (ADS)

    Clark, Joshua Andrew

    The importance of accurately identifying inventories of domestic energy, including forest biomass, has increasingly become a priority of the US government and its citizens as the cost of fossil fuels has risen. It is useful to identify which of these resources can be processed and transported at the lowest cost for both private and public landowners. Accurate spatial inventories of forest biomass can help landowners allocate resources to maximize forest biomass utilization and provide information regarding current forest health (e.g., forest fire potential, insect susceptibility, wildlife habitat range). This research has indicated that hemispherical photography (HP) may be an accurate and low cost sensing technique for forest biomass measurements. In this dissertation: (1) It is shown that HP gap fraction measurements and both above ground biomass and crown biomass have a linear relationship. (2) It is demonstrated that careful manipulation of images improves gap fraction estimates, even under unfavorable atmospheric conditions. (3) It is shown that estimates of Leaf Area Index (LAI), based on transformations of gap fraction measurements, are the best estimator for both above ground forest biomass and crown biomass. (4) It is shown that many factors negatively influence the utility of HP for biomass estimation. (5) It is shown that biomass of forests stands with regular spacing is not modeled well using HP. As researchers continue to explore different methods for forest biomass estimation, HP is likely to remain as a viable technique, especially if LAI can be accurately estimated. However, other methods should be compared with HP, particularly for stands where LAI is poorly estimated by HP.

  6. The Surface-Forced Overturning of the North Atlantic: Estimates from Modern Era Atmospheric Reanalysis Datasets

    NASA Astrophysics Data System (ADS)

    Grist, Jeremy; Josey, Simon; Marsh, Robert; Kwon, Young-Oh; Bingham, Rory; Blaker, Adam

    2014-05-01

    Estimates of the recent mean and time varying water mass transformation rates associated with North Atlantic surface-forced overturning are presented. The estimates are derived from heat and freshwater surface fluxes and sea surface temperature fields from six atmospheric reanalyses (JRA, NCEP-1, NCEP-2, ERA-I, CFSR and MERRA) together with sea surface salinity fields from two globally gridded data sets (World Ocean Atlas and EN3). The resulting twelve estimates of the 1979-2007 mean surface-forced streamfunction all depict a sub-polar cell, with maxima north of 45oN, near σ = 27.5 kgm-3, and a sub-tropical cell between 20oN and 40oN, near σ = 26.1 kgm-3. The mean magnitude of the sub-polar cell varies between 12-18 Sv, consistent with estimates of the overturning circulation from sub-surface observations. Analysis of the thermal and haline components of the surface density fluxes indicate large differences in the inferred low latitude circulation are largely due to the biases in reanalysis net heat flux fields, which range in the global mean from -13 Wm-2 to 19 Wm-2. The different estimates of temporal variability in the sub-polar cell are well correlated with each other. This suggests the uncertainty associated with the choice of reanalysis product does not critically limit the ability of the method to infer the variability in the sub-polar overturning. In contrast, the different estimates of sub-tropical variability are poorly correlated with each other, and only a subset of them capture a significant fraction of the variability in independently estimated North Atlantic Sub-Tropical Mode Water volume.

  7. Improving North American gross primary production (GPP) estimates using atmospheric measurements of carbonyl sulfide (COS)

    NASA Astrophysics Data System (ADS)

    Chen, Huilin; Montzka, Steve; Andrews, Arlyn; Sweeney, Colm; Jacobson, Andy; Miller, Ben; Masarie, Ken; Jung, Martin; Gerbig, Christoph; Campbell, Elliott; Abu-Naser, Mohammad; Berry, Joe; Baker, Ian; Tans, Pieter

    2013-04-01

    Understanding the responses of gross primary production (GPP) to climate change is essential for improving our prediction of climate change. To this end, it is important to accurately partition net ecosystem exchange of carbon into GPP and respiration. Recent studies suggest that carbonyl sulfide is a useful tracer to provide a constraint on GPP, based on the fact that both COS and CO2 are simultaneously taken up by plants and the quantitative correlation between GPP and COS plant uptake. We will present an assessment of North American GPP estimates from the Simple Biosphere (SiB) model, the Carnegie-Ames-Stanford Approach (CASA) model, and the MPI-BGC model through atmospheric transport simulations of COS in a receptor oriented framework. The newly upgraded Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) will be employed to compute the influence functions, i.e. footprints, to link the surface fluxes to the concentration changes at the receptor observations. The HYSPLIT is driven by the 3-hourly archived NAM 12km meteorological data from NOAA NCEP. The background concentrations are calculated using empirical curtains along the west coast of North America that have been created by interpolating in time and space the observations at the NOAA/ESRL marine boundary layer stations and from aircraft vertical profiles. The plant uptake of COS is derived from GPP estimates of biospheric models. The soil uptake and anthropogenic emissions are from Kettle et al. 2002. In addition, we have developed a new soil flux map of COS based on observations of molecular hydrogen (H2), which shares a common soil uptake term but lacks a vegetative sink. We will also improve the GPP estimates by assimilating atmospheric observations of COS in the receptor oriented framework, and then present the assessment of the improved GPP estimates against variations of climate variables such as temperature and precipitation.

  8. Spaceborne estimate of atmospheric CO2 column by use of the differential absorption method: error analysis.

    PubMed

    Dufour, Emmanuel; Bréon, François-Marie

    2003-06-20

    For better knowledge of the carbon cycle, there is a need for spaceborne measurements of atmospheric CO2 concentration. Because the gradients are relatively small, the accuracy requirements are better than 1%. We analyze the feasibility of a CO2-weighted-column estimate, using the differential absorption technique, from high-resolution spectroscopic measurements in the 1.6- and 2-microm CO2 absorption bands. Several sources of uncertainty that can be neglected for other gases with less stringent accuracy requirements need to be assessed. We attempt a quantification of errors due to the radiometric noise, uncertainties in the temperature, humidity and surface pressure uncertainty, spectroscopic coefficients, and atmospheric scattering. Atmospheric scattering is the major source of error [5 parts per 10 (ppm) for a subvisual cirrus cloud with an assumed optical thickness of 0.03], and additional research is needed to properly assess the accuracy of correction methods. Spectroscopic data are currently a major source of uncertainty but can be improved with specific ground-based sunphotometry measurements. The other sources of error amount to several ppm, which is less than, but close to, the accuracy requirements. Fortunately, these errors are mostly random and will therefore be reduced by proper averaging.

  9. A comparison of state-level estimation techniques for utility atmospheric emission factors

    SciTech Connect

    Schrock, D.; Baechler, M.

    1995-10-01

    Atmospheric emission factors provide a link between the electricity saved in buildings and the associated decrease in fossil fuel use in the electric supply sector. Understanding this link is important to meet the requirements of Section 1605(b) of the Energy Policy act of 1992, which established the voluntary program for reporting reductions in greenhouse gases. As part of the development process for Section 1605(b), several national workshops were held by the US Department of Energy (DOE) and the Energy Information Administration (EIA). Workshop participants expressed the need for DOE to supply default atmospheric emission facets. Based upon the response from the workshop participants, it was decided that emission factors would be aggregated to the state level (e.g., California, Connecticut, etc.). Emission factors for electricity generation are generally quantified as a quantity of impact to an amount of fuel used to produce the emission. In the electric supply sector, factors are often expressed in units of pounds or tons of emission per megawatt-hours (MWh) of electricity produced. In this paper, the authors examine and compare the estimates from three methodologies for developing state-level emission facets. In addition, they compare the results to those obtained using emissions data calculated by the EIA. Although the examples presented in this paper depict the development of state-level factors, the same methodologies can be applied by an individual utility to generate utility-specific atmospheric emission factors.

  10. Estimation of atmospheric sea salt dry deposition: Wind speed and particle size dependence

    NASA Astrophysics Data System (ADS)

    McDonald, R. L.; Unni, C. K.; Duce, R. A.

    1982-02-01

    Cascade impactor and bulk filter samples of atmospheric sea salt were collected at wind speeds from 3.4 to 10 m/s at coastal tower sites in the Florida Keys and Enewetak Atoll as part of the SEAREX (Sea Air Exchange) Program. Simultaneous dry deposition measurements were made to polyethylene plates. The samples were analyzed for Na as an indicator of sea salt. If the observed atmospheric sea salt particle mass distributions are corrected for the reduced collection efficiency of large particles, the observed dry deposition rates agree well with rates estimated from atmospheric sea salt particle concentrations and theoretical particle deposition velocities derived from gravitational settling velocities or from the equations of Slinn and Slinn (1980, 1981) for deposition to smooth, solid surfaces as well as natural water surfaces. The results emphasize the fact that even though large particles may represent only a small fraction of the total mass of sea salt over the ocean, they can dominate the dry deposition rates of the sea salt aerosol.

  11. An Aerosol Condensation Model for Sulfur Trioxide

    SciTech Connect

    Grant, K E

    2008-02-07

    This document describes a model for condensation of sulfuric acid aerosol given an initial concentration and/or source of gaseous sulfur trioxide (e.g. fuming from oleum). The model includes the thermochemical effects on aerosol condensation and air parcel buoyancy. Condensation is assumed to occur heterogeneously onto a preexisting background aerosol distribution. The model development is both a revisiting of research initially presented at the Fall 2001 American Geophysical Union Meeting [1] and a further extension to provide new capabilities for current atmospheric dispersion modeling efforts [2]. Sulfuric acid is one of the most widely used of all industrial chemicals. In 1992, world consumption of sulfuric acid was 145 million metric tons, with 42.4 Mt (mega-tons) consumed in the United States [10]. In 2001, of 37.5 Mt consumed in the U.S., 74% went into producing phosphate fertilizers [11]. Another significant use is in mining industries. Lawuyi and Fingas [7] estimate that, in 1996, 68% of use was for fertilizers and 5.8% was for mining. They note that H{sub 2}SO{sub 4} use has been and should continue to be very stable. In the United States, the elimination of MTBE (methyl tertiary-butyl ether) and the use of ethanol for gasoline production are further increasing the demand for petroleum alkylate. Alkylate producers have a choice of either a hydrofluoric acid or sulfuric acid process. Both processes are widely used today. Concerns, however, over the safety or potential regulation of hydrofluoric acid are likely to result in most of the growth being for the sulfuric acid process, further increasing demand [11]. The implication of sulfuric acid being a pervasive industrial chemical is that transport is also pervasive. Often, this is in the form of oleum tankers, having around 30% free sulfur trioxide. Although sulfuric acid itself is not a volatile substance, fuming sulfuric acid (referred to as oleum) is [7], the volatile product being sulfur trioxide

  12. Biogenic sulfur emissions and aerosols over the tropical South Atlantic: 3. Atmospheric dimethylsulfide, aerosols and cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Andreae, Meinrat O.; Elbert, Wolfgang; de Mora, Stephen J.

    1995-06-01

    We measured dimethylsulfide in air (DMSa) and the number concentration, size distribution, and chemical composition of atmospheric aerosols, including the concentration of cloud condensation nuclei (CCN), during February-March 1991 over the tropical South Atlantic along 19°S (F/S Meteor, cruise 15/3). Aerosol number/size distributions were determined with a laser-optical particle counter, condensation nuclei (CN) concentrations with a TSI 3020, and cloud condensation nuclei (CCN) with a Hudson-type supersaturation chamber. Aerosol samples were collected on two-stage stacked filters and analyzed by ion chromatography for soluble ion concentrations. Black carbon in aerosols was measured by visible light absorption and used to identify and eliminate periods with anthropogenic pollution from the data set. Meteorological analysis shows that most of the air masses sampled had spent extended periods over remote marine areas in the tropical and subtropical region. DMSa was closely correlated with the sea-to- air DMS flux calculated from DMS concentrations in seawater and meteorological data. Sea salt made the largest contribution to aerosol mass and volume but provided only a small fraction of the aerosol number concentration. The submicron aerosol had a mean composition close to ammonium bisulfate, with the addition of some methanesulfonate. Aerosol (CN and CCN) number and non-sea-salt sulfate concentrations were significantly correlated with DMS concentration and flux. This suggests that DMS oxidation followed by aerosol nucleation and growth in the marine boundary layer is an important, if not dominating, source of CN and possibly CCN. The degree of correlation between DMS and particle concentrations in the marine boundary layer may be strongly influenced by the different time scales of the processes regulating these concentrations. Our results provide strong support for several aspects of the CLAW hypothesis, which proposes the existence of a feedback loop linking DMS

  13. Sea ice-atmosphere interaction. Application of multispectral satellite data in polar surface energy flux estimates

    NASA Technical Reports Server (NTRS)

    Steffen, Konrad; Key, Jeff; Maslanik, Jim; Haefliger, Marcel; Fowler, Chuck

    1992-01-01

    Satellite data for the estimation of radiative and turbulent heat fluxes is becoming an increasingly important tool in large-scale studies of climate. One parameter needed in the estimation of these fluxes is surface temperature. To our knowledge, little effort has been directed to the retrieval of the sea ice surface temperature (IST) in the Arctic, an area where the first effects of a changing climate are expected to be seen. The reason is not one of methodology, but rather our limited knowledge of atmospheric temperature, humidity, and aerosol profiles, the microphysical properties of polar clouds, and the spectral characteristics of the wide variety of surface types found there. We have developed a means to correct for the atmospheric attenuation of satellite-measured clear sky brightness temperatures used in the retrieval of ice surface temperature from the split-window thermal channels of the advanced very high resolution radiometer (AVHRR) sensors on-board three of the NOAA series satellites. These corrections are specified for three different 'seasons' and as a function of satellite viewing angle, and are expected to be applicable to the perennial ice pack in the central Arctic Basin.

  14. An adaptive Bayesian inference algorithm to estimate the parameters of a hazardous atmospheric release

    NASA Astrophysics Data System (ADS)

    Rajaona, Harizo; Septier, François; Armand, Patrick; Delignon, Yves; Olry, Christophe; Albergel, Armand; Moussafir, Jacques

    2015-12-01

    In the eventuality of an accidental or intentional atmospheric release, the reconstruction of the source term using measurements from a set of sensors is an important and challenging inverse problem. A rapid and accurate estimation of the source allows faster and more efficient action for first-response teams, in addition to providing better damage assessment. This paper presents a Bayesian probabilistic approach to estimate the location and the temporal emission profile of a pointwise source. The release rate is evaluated analytically by using a Gaussian assumption on its prior distribution, and is enhanced with a positivity constraint to improve the estimation. The source location is obtained by the means of an advanced iterative Monte-Carlo technique called Adaptive Multiple Importance Sampling (AMIS), which uses a recycling process at each iteration to accelerate its convergence. The proposed methodology is tested using synthetic and real concentration data in the framework of the Fusion Field Trials 2007 (FFT-07) experiment. The quality of the obtained results is comparable to those coming from the Markov Chain Monte Carlo (MCMC) algorithm, a popular Bayesian method used for source estimation. Moreover, the adaptive processing of the AMIS provides a better sampling efficiency by reusing all the generated samples.

  15. Military Participants at U.S. Atmospheric Nuclear Weapons Testing— Methodology for Estimating Dose and Uncertainty

    PubMed Central

    Till, John E.; Beck, Harold L.; Aanenson, Jill W.; Grogan, Helen A.; Mohler, H. Justin; Mohler, S. Shawn; Voillequé, Paul G.

    2014-01-01

    Methods were developed to calculate individual estimates of exposure and dose with associated uncertainties for a sub-cohort (1,857) of 115,329 military veterans who participated in at least one of seven series of atmospheric nuclear weapons tests or the TRINITY shot carried out by the United States. The tests were conducted at the Pacific Proving Grounds and the Nevada Test Site. Dose estimates to specific organs will be used in an epidemiological study to investigate leukemia and male breast cancer. Previous doses had been estimated for the purpose of compensation and were generally high-sided to favor the veteran's claim for compensation in accordance with public law. Recent efforts by the U.S. Department of Defense (DOD) to digitize the historical records supporting the veterans’ compensation assessments make it possible to calculate doses and associated uncertainties. Our approach builds upon available film badge dosimetry and other measurement data recorded at the time of the tests and incorporates detailed scenarios of exposure for each veteran based on personal, unit, and other available historical records. Film badge results were available for approximately 25% of the individuals, and these results assisted greatly in reconstructing doses to unbadged persons and in developing distributions of dose among military units. This article presents the methodology developed to estimate doses for selected cancer cases and a 1% random sample of the total cohort of veterans under study. PMID:24758578

  16. A sparse reconstruction method for the estimation of multiresolution emission fields via atmospheric inversion

    DOE PAGES

    Ray, J.; Lee, J.; Yadav, V.; ...

    2014-08-20

    We present a sparse reconstruction scheme that can also be used to ensure non-negativity when fitting wavelet-based random field models to limited observations in non-rectangular geometries. The method is relevant when multiresolution fields are estimated using linear inverse problems. Examples include the estimation of emission fields for many anthropogenic pollutants using atmospheric inversion or hydraulic conductivity in aquifers from flow measurements. The scheme is based on three new developments. Firstly, we extend an existing sparse reconstruction method, Stagewise Orthogonal Matching Pursuit (StOMP), to incorporate prior information on the target field. Secondly, we develop an iterative method that uses StOMP tomore » impose non-negativity on the estimated field. Finally, we devise a method, based on compressive sensing, to limit the estimated field within an irregularly shaped domain. We demonstrate the method on the estimation of fossil-fuel CO2 (ffCO2) emissions in the lower 48 states of the US. The application uses a recently developed multiresolution random field model and synthetic observations of ffCO2 concentrations from a limited set of measurement sites. We find that our method for limiting the estimated field within an irregularly shaped region is about a factor of 10 faster than conventional approaches. It also reduces the overall computational cost by a factor of two. Further, the sparse reconstruction scheme imposes non-negativity without introducing strong nonlinearities, such as those introduced by employing log-transformed fields, and thus reaps the benefits of simplicity and computational speed that are characteristic of linear inverse problems.« less

  17. Estimating Terrestrial Wood Biomass from Observed Concentrations of Atmospheric Carbon Dioxide

    NASA Astrophysics Data System (ADS)

    Schaefer, K. M.; Peters, W.; Carvalhais, N.; van der Werf, G.; Miller, J.

    2008-12-01

    We estimate terrestrial disequilibrium state and wood biomass from observed concentrations of atmospheric CO2 using the CarbonTracker system coupled to the SiBCASA biophysical model. Starting with a priori estimates of carbon flux from the land, ocean, and fossil fuels, CarbonTracker estimates net carbon sources and sinks from 2000 to 2007 that are optimally consistent with observed CO2 concentrations. The a priori terrestrial Net Primary Productivity (NPP) and heterotrophic respiration (Rh) from SiBCASA assume steady state conditions for initial biomass, implying mature ecosystems with no disturbances where growth balances decay and the long-term, net carbon flux is zero. In reality, harvest, fires, and other disturbances reduce available biomass for decay, thus reducing Rh and resulting in a long-term carbon sink. The disequilibrium state is the ratio of Rh estimated from CarbonTracker to the steady state Rh from SiBCASA. Wood is the largest carbon pool in forest ecosystems and the dominant source of dead organic matter to the soil and litter pools. With much faster turnover times, the soil and litter pools reach equilibrium relative to the wood pool long before the wood pool itself reaches equilibrium. We take advantage of this quasi-steady state to estimate the size of the wood pool that will produce an Rh that corresponds to the net carbon sink from CarbonTracker. We then compare this estimated wood biomass to regional maps of observed above ground wood biomass from the US Forest Inventory Analysis.

  18. Measurement of Sulfur Isotope Ratios in Micrometer-Sized Aerosol Samples by NanoSIMS

    NASA Astrophysics Data System (ADS)

    Winterholler, B.; Hoppe, P.; Foley, S.; Andreae, M. O.

    2005-12-01

    The isotopic composition of sulfur in the atmosphere is highly variable and source dependent. Sulfur isotopic ratios are a well established tool for identifying sources of sulfur in the environment, estimating emission factors, and tracing the spread of sulfur from anthropogenic point sources in terrestrial ecosystems. Conventional mass spectrometry needs a minimum of 1 micromol of sulfur to perform one analysis. In the case of atmospheric aerosol particles the results of such an analysis averages the isotopic compositions of millions of aerosol particles, and thus normally includes several different types of sulfur aerosol. The new Cameca NanoSIMS 50 ion microprobe technique permits analysis of individual aerosol particles with volumes down to 0.3 cubic micron and a precision for delta34S of 3-10 (2 sigma). As a result, this technique is able to introduce a new scale into the study of the atmospheric sulfur cycle. Linking the chemical, mineralogical, morphological and isotopic information of individual particles will allow a better understanding of external and internal mixing states by analyzing more than one spot on coarse mode particles. Moreover it will improve source identification by complementing the chemical and isotopic information. First samples have been collected from the Sahara desert, an urban site in central Europe, and a costal site in Western Ireland and show the potentials of this new technique.

  19. Hydrate sulfuric acid after sulfur implantation in water ice

    NASA Astrophysics Data System (ADS)

    Strazzulla, G.; Baratta, G. A.; Leto, G.; Gomis, O.

    2007-12-01

    For many years an ongoing research program performed at our laboratory has had the aim to investigate the implantation of reactive ions in ices relevant to planetology by using IR spectroscopy. We present new results obtained by implanting 200 keV sulfur ions into water ice at 80 K. We have looked at the formation of sulfur-bearing molecules such as sulfuric acid, sulfur dioxide and hydrogen sulfide. We find that hydrated sulfuric acid is formed with high yield ( 0.65±0.1 molecules/ion). An upper limit to the production yield of SO 2 ( Y⩽0.025 molecules/ion) has been estimated; no hydrogen sulfide has been detected. The formation of hydrogen peroxide is confirmed. Ozone is not detected. The results are discussed relevant to the inquiry on the radiolytic sulfur cycle considered responsible for the formation of sulfur-bearing molecules on the surfaces of the Galilean satellites. We demonstrate that sulfur implantation efficiently forms hydrated sulfuric acid whose observed abundance is explained as caused by an exogenic process. It is more difficult to say if the observed sulfur dioxide is quantitatively supported by only sulfur implantation; additional experimental studies are necessary along with direct observations, especially at UV wavelengths such as those that could be performed by instruments on board Hubble Space Telescope or by the forthcoming World Space Observatory (WSO/UV).

  20. Sulfur Cycle

    NASA Technical Reports Server (NTRS)

    Hariss, R.; Niki, H.

    1985-01-01

    Among the general categories of tropospheric sulfur sources, anthropogenic sources have been quantified the most accurately. Research on fluxes of sulfur compounds from volcanic sources is now in progress. Natural sources of reduced sulfur compounds are highly variable in both space and time. Variables, such as soil temperature, hydrology (tidal and water table), and organic flux into the soil, all interact to determine microbial production and subsequent emissions of reduced sulfur compounds from anaerobic soils and sediments. Available information on sources of COS, CS2, DMS, and H2S to the troposphere in the following paragraphs are summarized; these are the major biogenic sulfur species with a clearly identified role in tropospheric chemistry. The oxidation of SO2 to H2SO4 can often have a significant impact on the acidity of precipitation. A schematic representation of some important transformations and sinks for selected sulfur species is illustrated.

  1. Sulfur revisited.

    PubMed

    Lin, A N; Reimer, R J; Carter, D M

    1988-03-01

    Sulfur is a time-honored therapeutic agent useful in a variety of dermatologic disorders. Its keratolytic action is due to formation of hydrogen sulfide through a reaction that depends upon direct interaction between sulfur particles and keratinocytes. The smaller the particle size, the greater the degree of such interaction and the greater the therapeutic efficacy. When applied topically, sulfur induces various histologic changes, including hyperkeratosis, acanthosis, and dilatation of dermal vasculature. One study showed that sulfur was comedogenic when applied onto human and rabbit skin, findings that were not reproduced in other studies. About 1% of topically applied sulfur is systemically absorbed. Adverse effects from topically applied sulfur are uncommon and are mainly limited to the skin. In infants, however, fatal outcome after extensive application has been reported.

  2. Estimate of Top-of-Atmosphere Albedo for a Molecular Atmosphere over Ocean using Clouds and the Earth's Radiant Energy System (CERES) Measurements

    NASA Technical Reports Server (NTRS)

    Kato, S.; Loeb, N. G.; Rutledge, C. K.

    2002-01-01

    The shortwave broadband albedo at the top of a molecular atmosphere over ocean between 40deg N and 40deg S is estimated using radiance measurements from the Clouds and the Earth's Radiant Energy System (CERES) instrument and the Visible Infrared Scanner (VIRS) aboard the Tropical Rainfall Measuring Mission (TRMM) satellite. The albedo monotonically increases from 0.059 at a solar zenith angle of 10deg to 0.107 at a solar zenith angle of 60deg. The estimated uncertainty in the albedo is 3.5 x 10(exp -3) caused by the uncertainty in CERES-derived irradiances, uncertainty in VIRS-derived aerosol optical thicknesses, variations in ozone and water vapor, and variations in surface wind speed. The estimated uncertainty is similar in magnitude to the standard deviation of 0.003 that is derived from 72 areas divided by 20deg latitude by 20deg longitude grid boxes. The empirically estimated albedo is compared with the modeled albedo using a radiative transfer model combined with an ocean surface bidirectional reflectivity model. The modeled albedo with standard tropical atmosphere is 0.061 and 0.111 at the solar zenith angles of 10deg and 60deg, respectively. This empirically estimated albedo can be used to estimate the direct radiative effect of aerosols at the top of the atmosphere over oceans.

  3. Estimation of organophosphoric acid triesters in soft polyurethane foam using a concentrated sulfuric acid dissolution technique and gas chromatography with flame photometric detection.

    PubMed

    Nagase, Makoto; Toba, Mineki; Kondo, Hiroyuki; Yasuhara, Akio; Hasebe, Kiyoshi

    2003-12-01

    A concentrated sulfuric acid dissolution technique and a GC method are described for the estimation of tributyl phosphate, tris(2-chloroethyl) phosphate, tris(chloropropyl) phosphate, tris(1,3-dichloro-2-propyl) phosphate, triphenyl phosphate and tris(butoxyethyl) phosphate in soft polyurethane foam. A soft polyurethane foam sample containing organophosphoric acid triesters was dissolved in concentrated sulfuric acid. The solution was added to water, where only the polyurethane was separated out. The pH of the solution was adjusted, and organophosphoric acid triesters were extracted with toluene. After purification, the compounds were determined by GC. The detection limits of the organophosphoric acid triesters were 0.3 - 0.9 microg g(-1). The recoveries of the organophosphoric acid triesters from a 0.05 g sample of soft polyurethane foam were 80.0 - 90.0%, when the spiked amounts were 0.25 - 1 microg. The compounds were detected from soft polyurethane foam at the level of 0.4 - 23.3 microg g(-1).

  4. Sensitivity of Active Remotely Sensed Total Column Observations to Atmospheric State Estimation Errors

    NASA Astrophysics Data System (ADS)

    Crowell, S.; Rayner, P. J.; Moore, B.

    2013-12-01

    The proposed Active Sensing of CO2 Emissions over Nights, Days and Seasons (ASCENDS) mission will retrieve total column CO2 using a laser-based measurement. The differential absorption lidar (DIAL) approach utilizes the difference in absorption between neighboring spectral lines to effectively determine the difference in absorption due to CO2. The actual measured quantity is equivalent to the differential absorption, defined by Δτ = ∫ q(p) Δξ(p) dp / g m, where m is the molar mass of air and Δξ is the differential absorption cross section. The main use of the measurement is the characterization of sources and sinks using atmospheric inverse methods. Changes in surface pressure or Δξ can change Δτ independent of sources and sinks and are, thus "nuisance variables". Δξ is strongly dependent on variations in temperature (T) and water vapor (w), which are usually taken from numerical models as estimates of the local atmospheric state. The authors seek to determine observable that contains the most information on the model column of CO2, which will provide the best estimates of sources and sinks in a transport model inversion. Three candidate observables are the differential optical depth on a CO2 line, the ratio of this to the differential optical depth on an O2 line, the weighting function averaged column CO2. Each of these observables will have different sensitivities to surface pressure and spectroscopy by virtue of the functional form that defines them. For example, the O2 measurement should be less sensitive to surface pressure fluctuations due to the near constancy of O2 in the atmosphere. The information contained in the observation about the model state is encapsulated in the quantity HTR-1H, where R is the observation error covariance and H is the Jacobian of the observation operator with respect to the model mixing ratio of CO2. We can decompose the error variance for a particular observation into contributions from the surface pressure errors

  5. Sulfur compounds in coal

    NASA Technical Reports Server (NTRS)

    Attar, A.; Corcoran, W. H.

    1977-01-01

    The literature on the chemical structure of the organic sulfur compounds (or functional groups) in coal is reviewed. Four methods were applied in the literature to study the sulfur compounds in coal: direct spectrometric and chemical analysis, depolymerization in drastic conditions, depolymerization in mild conditions, and studies on simulated coal. The data suggest that most of the organic sulfur in coal is in the form of thiophenic structures and aromatic and aliphatic sulfides. The relative abundance of the sulfur groups in bituminous coal is estimated as 50:30:20%, respectively. The ratio changes during processing and during the chemical analysis. The main effects are the transformation during processing of sulfides to the more stable thiophenic compounds and the elimination of hydrogen sulfide.

  6. SDSS/SEGUE spectral feature analysis for stellar atmospheric parameter estimation

    SciTech Connect

    Li, Xiangru; Lu, Yu; Yang, Tan; Wang, Yongjun; Wu, Q. M. Jonathan; Luo, Ali; Zhao, Yongheng; Zuo, Fang

    2014-08-01

    Large-scale and deep sky survey missions are rapidly collecting a large amount of stellar spectra, which necessitate the estimation of atmospheric parameters directly from spectra and make it feasible to statistically investigate latent principles in a large data set. We present a technique for estimating parameters T{sub eff}, log g, and [Fe/H] from stellar spectra. With this technique, we first extract features from stellar spectra using the LASSO algorithm; then, the parameters are estimated from the extracted features using the support vector regression. On a subsample of 20,000 stellar spectra from the Sloan Digital Sky Survey (SDSS) with reference parameters provided by the SDSS/SEGUE Spectroscopic Parameter Pipeline, estimation consistency are 0.007458 dex for log T{sub eff} (101.609921 K for T{sub eff}), 0.189557 dex for log g, and 0.182060 for [Fe/H], where the consistency is evaluated by mean absolute error. Prominent characteristics of the proposed scheme are sparseness, locality, and physical interpretability. In this work, each spectrum consists of 3821 fluxes, and 10, 19, and 14 typical wavelength positions are detected, respectively, for estimating T{sub eff}, log g, and [Fe/H]. It is shown that the positions are related to typical lines of stellar spectra. This characteristic is important in investigating physical indications from analysis results. Then, stellar spectra can be described by the individual fluxes on the detected positions (PD) or local integration of fluxes near them (LI). The aforementioned consistency is the result based on features described by LI. If features are described by PD, consistency is 0.009092 dex for log T{sub eff} (124.545075 K for T{sub eff}), 0.198928 dex for log g, and 0.206814 dex for [Fe/H].

  7. A Site Atmospheric State Best Estimate of Temperature for Lauder, New Zealand

    NASA Astrophysics Data System (ADS)

    Tradowsky, J. S.; Bodeker, G. E.; Querel, R.; Builtjes, P. J. H.; Fischer, J.; Lewis, J.

    2015-12-01

    To detect and attribute changes in local and global climate, long-term observations of the atmosphere are essential. The Global Climate Observing System (GCOS) has defined 50 Essential Climate Variables (ECVs), which are fundamental for understanding the climate system. To fill a long recognized need of the climate monitoring community for reference quality measurements of upper air ECVs, the GCOS Reference Upper Air Network (GRUAN) was established and is now operational. This study presents a temporally highly-resolved Site Atmospheric State Best Estimate of temperature (T-SASBE) for the GRUAN site at Lauder, New Zealand. In a SASBE all available measurements of a selected ECV at one specific site (and possibly including estimates obtained from measurements made elsewhere) are merged to produce a best estimate of the value of that ECV and the uncertainty on each datum.The first version of T-SASBE, extending from 1996 to 2006, combines measurements from: (i) weekly radiosondes launched at Lauder, (ii) 10-minute data obtained from the surface weather station at Lauder and (iii) twice-daily radiosondes launched at Invercargill, about 200km south-west of Lauder. Later versions of T-SASBE will extend the time period and include further measurements made at Lauder.The temperature profiles measured at Invercargill are included in T-SASBE to provide an estimate of the vertical structure in temperature at times between the once-weekly radiosonde flights at Lauder. Corrections to the Invercargill measurements were derived by applying a regression model to temperature profiles measured at Lauder and Invercargill within 12 hours of each other. Different predictor variables, including wind speed and surface pressure, were tested and the quality of the regression model was evaluated. The regression model with the best combination of the predictor variables was used to correct the Invercargill temperature profiles and use them as a valid proxy for 12-hourly temperature profiles

  8. Influence of Fossil Fuel Emissions on CO2 Flux Estimation by Atmospheric Inversions

    NASA Astrophysics Data System (ADS)

    Saeki, T.; Patra, P. K.; van der Laan-Luijkx, I. T.; Peters, W.

    2015-12-01

    Top-down approaches (or atmospheric inversions) using atmospheric transport models with CO2 observations are an effective way to estimate carbon fluxes at global and regional scales. CO2 flux estimation by Bayesian inversions require a priori knowledge of terrestrial biosphere and oceanic fluxes and fossil fuel (FF) CO2 emissions. In most inversion frameworks, FF CO2 is assumed to be a known quantity because FF CO2 based on world statistics are thought to be more reliable than natural CO2 fluxes. However different databases of FF CO2 emissions may have different temporal and spatial variations especially at locations where statistics are not so accurate. In this study, we use 3 datasets of fossil fuel emissions in inversion estimations and evaluate the sensitivity of the optimized CO2 fluxes to FF emissions with two different inverse models, JAMSTEC's ACTM and CarbonTracker Europe (CTE). Interannually varying a priori FF CO2 emissions were based on 1) CDIAC database, 2) EDGARv4.2 database, and 3) IEA database, with some modifications. Biosphere and oceanic fluxes were optimized. Except for FF emissions, other conditions were kept the same in our inverse experiments. The three a priori FF emissions showed ~5% (~0.3GtC/yr) differences in their global total emissions in the early 2000's and the differences reached ~9% (~0.9 GtC/yr) in 2010. This resulted in 0.5-1 GtC/yr (2001-2011) and 0.3-0.6 GtC/yr (2007-2011) differences in the estimated global total emissions for the ACTM and CTE inversions, respectively. Regional differences in the FF emissions were relatively large in East Asia (~0.5 GtC/yr for ACTM and ~0.3 GtC/yr for CTE) and Europe (~0.3 GtC/yr for ACTM). These a priori flux differences caused differences in the estimated biosphere fluxes for ACTM in East Asia and Europe and also their neighboring regions such as West Asia, Boreal Eurasia, and North Africa. The main differences in the biosphere fluxes for CTE were found in Asia and the Americas.

  9. An attempt at estimating Paris area CO2 emissions from atmospheric concentration measurements

    NASA Astrophysics Data System (ADS)

    Bréon, F. M.; Broquet, G.; Puygrenier, V.; Chevallier, F.; Xueref-Remy, I.; Ramonet, M.; Dieudonné, E.; Lopez, M.; Schmidt, M.; Perrussel, O.; Ciais, P.

    2015-02-01

    Atmospheric concentration measurements are used to adjust the daily to monthly budget of fossil fuel CO2 emissions of the Paris urban area from the prior estimates established by the Airparif local air quality agency. Five atmospheric monitoring sites are available, including one at the top of the Eiffel Tower. The atmospheric inversion is based on a Bayesian approach, and relies on an atmospheric transport model with a spatial resolution of 2 km with boundary conditions from a global coarse grid transport model. The inversion adjusts prior knowledge about the anthropogenic and biogenic CO2 fluxes from the Airparif inventory and an ecosystem model, respectively, with corrections at a temporal resolution of 6 h, while keeping the spatial distribution from the emission inventory. These corrections are based on assumptions regarding the temporal autocorrelation of prior emissions uncertainties within the daily cycle, and from day to day. The comparison of the measurements against the atmospheric transport simulation driven by the a priori CO2 surface fluxes shows significant differences upwind of the Paris urban area, which suggests a large and uncertain contribution from distant sources and sinks to the CO2 concentration variability. This contribution advocates that the inversion should aim at minimising model-data misfits in upwind-downwind gradients rather than misfits in mole fractions at individual sites. Another conclusion of the direct model-measurement comparison is that the CO2 variability at the top of the Eiffel Tower is large and poorly represented by the model for most wind speeds and directions. The model's inability to reproduce the CO2 variability at the heart of the city makes such measurements ill-suited for the inversion. This and the need to constrain the budgets for the whole city suggests the assimilation of upwind-downwind mole fraction gradients between sites at the edge of the urban area only. The inversion significantly improves the agreement

  10. Subdiurnal atmospheric and oceanic excitation of Earth rotation estimated from 3-hourly AAM and OAM data

    NASA Astrophysics Data System (ADS)

    Brzezinski, A.; Dobslaw, H.; Thomas, M.; Slusarczyk, L.

    2012-04-01

    Diurnal and subdiurnal variations of global atmospheric and nontidal oceanic angular momenta (AAM, OAM) contribute at measurable level to all components of Earth rotation, including precession-nutation, polar motion and universal time UT1. Here we study this problem using a new set of 3-hourly AAM and OAM series covering 1990-2009. The data is based on the ERA Interim short-term forecasts, which have been both used to derive AAM as well as force a OMCT (Ocean Model for Circulation and Tides) simulation that provides the corresponding OAM. We apply the complex demodulation technique to extract the diurnal, semidiurnal and terdiurnal signals from both the equatorial and axial components of the excitation series. Next we estimate parameters of the harmonic components of excitation and perform spectral analysis of the nonharmonic residuals. The estimated contributions to Earth rotation are compared to other results which are either estimated from alternative geophysical models or are expected from analysis of Earth rotation data.

  11. A new estimation of the recent tropospheric molecular hydrogen budget using atmospheric observations and variational inversion

    NASA Astrophysics Data System (ADS)

    Yver, C.; Pison, I.; Fortems-Cheiney, A.; Schmidt, M.; Bousquet, P.; Ramonet, M.; Jordan, A.; Søvde, A.; Engel, A.; Fisher, R.; Lowry, D.; Nisbet, E.; Levin, I.; Hammer, S.; Necki, J.; Bartyzel, J.; Reimann, S.; Vollmer, M. K.; Steinbacher, M.; Aalto, T.; Maione, M.; Arduini, I.; O'Doherty, S.; Grant, A.; Sturges, W.; Lunder, C. R.; Privalov, V.; Paramonova, N.

    2010-11-01

    This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, soil uptake distinct from surface emissions and finally, soil uptake, biomass burning, anthropogenic emissions and N2 fixation-related emissions separately were inverted in several scenarios. The various inversions generate an estimate for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between -8 and 8 Tg yr-1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on soil uptake measurements. Our estimate of global H2 soil uptake is -59 ± 4.0 Tg yr-1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions considering their respective uncertainties. To constrain a more robust partition of H2 sources and sinks would need additional constraints, such as isotopic measurements.

  12. Atmospheric methane time series from Finland and Siberia: source areas and surface flux estimates

    NASA Astrophysics Data System (ADS)

    Kilkki, Juho; Aalto, Tuula; Kouznetsov, Rostislav; Hatakka, Juha; Makelä, Timo; Leskinen, Ari; Laurila, Tuomas

    2016-04-01

    We present atmospheric methane concentrations from a diverse set of Finnish stations and Tiksi, northeastern Siberia, and associate them with source areas and surface fluxes. In Finland, synoptic time scale concentrations are consistent with observations from the WMO/GAW site Pallas, with little difference in mean concentration in well-mixed cases. However, source areas determined with a backward dispersion model show that there is a gradient in sensitivity to both anthropogenic and wetland emissions among the stations. We estimate these flux components in the northern parts of Europe using the available observations. In Tiksi, the concentrations are consistent with nearby micrometeorological measurements and a remote-sensed wetness distribution in the region. Wintertime concentrations are usually close to background concentrations in a global transport model, and overall there are few events attributable to the ocean. In a Bayesian atmospheric inversion with weather-independent emissions, the oceanic source is about a third of wetland emissions in our study area that covers most of northern Yakutia and the East-Siberian Arctic Shelf.

  13. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Zhao, Y.

    2015-12-01

    To better understand the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations in China, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal and spatial distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols. The national OC emissions are estimated to have increased 29% from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37% (from 1356 to 1857 Gg). Updated emission factors based on the most recent local field measurements, particularly for biofuel stoves, lead to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while SOC/OC ratios are found in southern cities, due to the joint effects of primary emissions and meteorology. Higher OC/EC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, smaller SOC/OC is found for cold seasons, particularly at rural and remote sites, attributed partly to weaker atmospheric oxidation and SOC formation in winter. Enhanced SOC formation from oxidization and anthropogenic activities like biomass combustion is judged to have crucial effects on severe haze events characterized by high particle concentrations. Several observational studies indicate an increasing trend in ambient OC/EC (but not in OC or EC individually) from 2000 to 2010, confirming increased atmospheric oxidation of OC across the country. Combining the results of

  14. A multiyear estimate of methane fluxes in Alaska from CARVE atmospheric observations

    NASA Astrophysics Data System (ADS)

    Miller, Scot M.; Miller, Charles E.; Commane, Roisin; Chang, Rachel Y.-W.; Dinardo, Steven J.; Henderson, John M.; Karion, Anna; Lindaas, Jakob; Melton, Joe R.; Miller, John B.; Sweeney, Colm; Wofsy, Steven C.; Michalak, Anna M.

    2016-10-01

    Methane (CH4) fluxes from Alaska and other arctic regions may be sensitive to thawing permafrost and future climate change, but estimates of both current and future fluxes from the region are uncertain. This study estimates CH4 fluxes across Alaska for 2012-2014 using aircraft observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) and a geostatistical inverse model (GIM). We find that a simple flux model based on a daily soil temperature map and a static map of wetland extent reproduces the atmospheric CH4 observations at the statewide, multiyear scale more effectively than global-scale process-based models. This result points to a simple and effective way of representing CH4 fluxes across Alaska. It further suggests that process-based models can improve their representation of key processes and that more complex processes included in these models cannot be evaluated given the information content of available atmospheric CH4 observations. In addition, we find that CH4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.26 Tg CH4 (for May-October). Global-scale process models only attribute an average of 3% of the total flux to this region. This mismatch occurs for two reasons: process models likely underestimate wetland extent in regions without visible surface water, and these models prematurely shut down CH4 fluxes at soil temperatures near 0°C. Lastly, we find that the seasonality of CH4 fluxes varied during 2012-2014 but that total emissions did not differ significantly among years, despite substantial differences in soil temperature and precipitation.

  15. Atmospheric ammonia over China: emission estimates and impacts on air quality

    NASA Astrophysics Data System (ADS)

    Zhang, Lin; Zhao, Yuanhong; Chen, Youfan; Henze, Daven

    2016-04-01

    Ammonia (NH3) in the atmosphere is an important precursor of inorganic aerosols, and its deposition through wet and dry processes can cause adverse effects on ecosystems. The ammonia emissions over China are particularly large due to intensive agricultural activities, yet our current estimates of Chinese ammonia emissions and associated consequences on air quality are subject to large errors. Here we use the GEOS-Chem chemical transport model and its adjoint model to better quantify this issue. The TES satellite observations of ammonia concentrations and surface measurements of wet deposition fluxes are assimilated into the model to constrain the ammonia emissions over China. Optimized emissions show a strong seasonal variability with emissions in summer a factor of 3 higher than winter. We improve the bottom-up estimate of Chinese ammonia emissions from fertilizer use by using more practical feritilizer application rates for different crop types, which explains most of the discrepancies between our top-down estimates and prior emission estimates. We further use the GEOS-Chem adjoint at 0.25x0.3125 degree resolution to examine the sources contributing to the PM2.5 air pollution over North China. We show that wintertime PM2.5 over Beijing is largely contributed by residential and industrial sources, and ammonia emissions from agriculture activities. PM2.5 concentrations over North China are particularly sensitive to NH3 emissions in cold seasons due to strong nitrate formation. By converting shorted-lived nitric acid to aerosol nitrate, NH3 significantly promotes the regional transport influences of PM2.5 sources.

  16. A new estimation of the recent tropospheric molecular hydrogen budget using atmospheric observations and variational inversion

    NASA Astrophysics Data System (ADS)

    Yver, C. E.; Pison, I. C.; Fortems-Cheiney, A.; Schmidt, M.; Chevallier, F.; Ramonet, M.; Jordan, A.; Søvde, O. A.; Engel, A.; Fisher, R. E.; Lowry, D.; Nisbet, E. G.; Levin, I.; Hammer, S.; Necki, J.; Bartyzel, J.; Reimann, S.; Vollmer, M. K.; Steinbacher, M.; Aalto, T.; Maione, M.; Arduini, J.; O'Doherty, S.; Grant, A.; Sturges, W. T.; Forster, G. L.; Lunder, C. R.; Privalov, V.; Paramonova, N.; Werner, A.; Bousquet, P.

    2011-04-01

    This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and European surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, then deposition velocity and surface emissions and finally, deposition velocity, biomass burning, anthropogenic and N2 fixation-related emissions were simultaneously inverted in several scenarios. These scenarios have focused on the sensibility of the soil uptake value to different spatio-temporal distributions. The range of variations of these diverse inversion sets generate an estimate of the uncertainty for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between -8 and +8 Tg yr-1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on bottom-up and top-down estimations. Our estimate of global H2 soil uptake is -59±9 Tg yr-1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions within the range of their respective uncertainties. Additional constraints, such as isotopic measurements would be needed to infer a more robust partition of H2 sources and sinks.

  17. Ammonia emissions from an anaerobic digestion plant estimated using atmospheric measurements and dispersion modelling.

    PubMed

    Bell, Michael W; Tang, Y Sim; Dragosits, Ulrike; Flechard, Chris R; Ward, Paul; Braban, Christine F

    2016-10-01

    Anaerobic digestion (AD) is becoming increasingly implemented within organic waste treatment operations. The storage and processing of large volumes of organic wastes through AD has been identified as a significant source of ammonia (NH3) emissions, however the totality of ammonia emissions from an AD plant have not been previously quantified. The emissions from an AD plant processing food waste were estimated through integrating ambient NH3 concentration measurements, atmospheric dispersion modelling, and comparison with published emission factors (EFs). Two dispersion models (ADMS and a backwards Lagrangian stochastic (bLS) model) were applied to calculate emission estimates. The bLS model (WindTrax) was used to back-calculate a total (top-down) emission rate for the AD plant from a point of continuous NH3 measurement downwind from the plant. The back-calculated emission rates were then input to the ADMS forward dispersion model to make predictions of air NH3 concentrations around the site, and evaluated against weekly passive sampler NH3 measurements. As an alternative approach emission rates from individual sources within the plant were initially estimated by applying literature EFs to the available site parameters concerning the chemical composition of waste materials, room air concentrations, ventilation rates, etc. The individual emission rates were input to ADMS and later tuned by fitting the simulated ambient concentrations to the observed (passive sampler) concentration field, which gave an excellent match to measurements after an iterative process. The total emission from the AD plant thus estimated by a bottom-up approach was 16.8±1.8mgs(-1), which was significantly higher than the back-calculated top-down estimate (7.4±0.78mgs(-1)). The bottom-up approach offered a more realistic treatment of the source distribution within the plant area, while the complexity of the site was not ideally suited to the bLS method, thus the bottom-up method is believed

  18. Automated source term and wind parameter estimation for atmospheric transport and dispersion applications

    NASA Astrophysics Data System (ADS)

    Bieringer, Paul E.; Rodriguez, Luna M.; Vandenberghe, Francois; Hurst, Jonathan G.; Bieberbach, George; Sykes, Ian; Hannan, John R.; Zaragoza, Jake; Fry, Richard N.

    2015-12-01

    Accurate simulations of the atmospheric transport and dispersion (AT&D) of hazardous airborne materials rely heavily on the source term parameters necessary to characterize the initial release and meteorological conditions that drive the downwind dispersion. In many cases the source parameters are not known and consequently based on rudimentary assumptions. This is particularly true of accidental releases and the intentional releases associated with terrorist incidents. When available, meteorological observations are often not representative of the conditions at the location of the release and the use of these non-representative meteorological conditions can result in significant errors in the hazard assessments downwind of the sensors, even when the other source parameters are accurately characterized. Here, we describe a computationally efficient methodology to characterize both the release source parameters and the low-level winds (eg. winds near the surface) required to produce a refined downwind hazard. This methodology, known as the Variational Iterative Refinement Source Term Estimation (STE) Algorithm (VIRSA), consists of a combination of modeling systems. These systems include a back-trajectory based source inversion method, a forward Gaussian puff dispersion model, a variational refinement algorithm that uses both a simple forward AT&D model that is a surrogate for the more complex Gaussian puff model and a formal adjoint of this surrogate model. The back-trajectory based method is used to calculate a "first guess" source estimate based on the available observations of the airborne contaminant plume and atmospheric conditions. The variational refinement algorithm is then used to iteratively refine the first guess STE parameters and meteorological variables. The algorithm has been evaluated across a wide range of scenarios of varying complexity. It has been shown to improve the source parameters for location by several hundred percent (normalized by the

  19. A multi-year estimate of methane fluxes in Alaska from CARVE atmospheric observations.

    PubMed

    Miller, Scot M; Miller, Charles E; Commane, Roisin; Chang, Rachel Y-W; Dinardo, Steven J; Henderson, John M; Karion, Anna; Lindaas, Jakob; Melton, Joe R; Miller, John B; Sweeney, Colm; Wofsy, Steven C; Michalak, Anna M

    2016-10-01

    Methane (CH4) fluxes from Alaska and other arctic regions may be sensitive to thawing permafrost and future climate change, but estimates of both current and future fluxes from the region are uncertain. This study estimates CH4 fluxes across Alaska for 2012-2014 using aircraft observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) and a geostatistical inverse model (GIM). We find that a simple flux model based on a daily soil temperature map and a static map of wetland extent reproduces the atmospheric CH4 observations at the state-wide, multi-year scale more effectively than global-scale, state-of-the-art process-based models. This result points to a simple and effective way of representing CH4 flux patterns across Alaska. It further suggests that contemporary process-based models can improve their representation of key processes that control fluxes at regional scales, and that more complex processes included in these models cannot be evaluated given the information content of available atmospheric CH4 observations. In addition, we find that CH4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.44 Tg CH4 (for May-Oct.). Contemporary global-scale process models only attribute an average of 3% of the total flux to this region. This mismatch occurs for two reasons: process models likely underestimate wetland area in regions without visible surface water, and these models prematurely shut down CH4 fluxes at soil temperatures near 0°C. As a consequence, wetlands covered by vegetation and wetlands with persistently cold soils could be larger contributors to natural CH4 fluxes than in process estimates. Lastly, we find that the seasonality of CH4 fluxes varied during 2012-2014, but that total emissions did not differ significantly among years, despite substantial differences in soil temperature and precipitation; year-to-year variability in these environmental conditions did not affect obvious

  20. Climate Science for a Sustainable Energy Future Atmospheric Radiation Measurement Best Estimate (CSSEFARMBE)

    SciTech Connect

    Riihimaki, Laura D.; Gaustad, Krista L.; McFarlane, Sally A.

    2012-09-28

    The Climate Science for a Sustainable Energy Future (CSSEF) project is working to improve the representation of the hydrological cycle in global climate models, critical information necessary for decision-makers to respond appropriately to predictions of future climate. In order to accomplish this objective, CSSEF is building testbeds to implement uncertainty quantification (UQ) techniques to objectively calibrate and diagnose climate model parameterizations and predictions with respect to local, process-scale observations. In order to quantify the agreement between models and observations accurately, uncertainty estimates on these observations are needed. The DOE Atmospheric Radiation Measurement (ARM) program takes atmospheric and climate related measurements at three permanent locations worldwide. The ARM VAP called the ARM Best Estimate (ARMBE) [Xie et al., 2010] collects a subset of ARM observations, performs quality control checks, averages them to one hour temporal resolution, and puts them in a standard format for ease of use by climate modelers. ARMBE has been widely used by the climate modeling community as a summary product of many of the ARM observations. However, the ARMBE product does not include uncertainty estimates on the data values. Thus, to meet the objectives of the CSSEF project and enable better use of this data with UQ techniques, we created the CSSEFARMBE data set. Only a subset of the variables contained in ARMBE is included in CSSEFARMBE. Currently only surface meteorological observations are included, though this may be expanded to include other variables in the future. The CSSEFARMBE VAP is produced for all extended facilities at the ARM Southern Great Plains (SGP) site that contain surface meteorological equipment. This extension of the ARMBE data set to multiple facilities at SGP allows for better comparison between model grid boxes and the ARM point observations. In the future, CSSEFARMBE may also be created for other ARM sites. As

  1. A multi-year estimate of methane fluxes in Alaska from CARVE atmospheric observations

    PubMed Central

    Miller, Scot M.; Miller, Charles E.; Commane, Roisin; Chang, Rachel Y.-W.; Dinardo, Steven J.; Henderson, John M.; Karion, Anna; Lindaas, Jakob; Melton, Joe R.; Miller, John B.; Sweeney, Colm; Wofsy, Steven C.; Michalak, Anna M.

    2016-01-01

    Methane (CH4) fluxes from Alaska and other arctic regions may be sensitive to thawing permafrost and future climate change, but estimates of both current and future fluxes from the region are uncertain. This study estimates CH4 fluxes across Alaska for 2012–2014 using aircraft observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) and a geostatistical inverse model (GIM). We find that a simple flux model based on a daily soil temperature map and a static map of wetland extent reproduces the atmospheric CH4 observations at the state-wide, multi-year scale more effectively than global-scale, state-of-the-art process-based models. This result points to a simple and effective way of representing CH4 flux patterns across Alaska. It further suggests that contemporary process-based models can improve their representation of key processes that control fluxes at regional scales, and that more complex processes included in these models cannot be evaluated given the information content of available atmospheric CH4 observations. In addition, we find that CH4 emissions from the North Slope of Alaska account for 24% of the total statewide flux of 1.74 ± 0.44 Tg CH4 (for May–Oct.). Contemporary global-scale process models only attribute an average of 3% of the total flux to this region. This mismatch occurs for two reasons: process models likely underestimate wetland area in regions without visible surface water, and these models prematurely shut down CH4 fluxes at soil temperatures near 0°C. As a consequence, wetlands covered by vegetation and wetlands with persistently cold soils could be larger contributors to natural CH4 fluxes than in process estimates. Lastly, we find that the seasonality of CH4 fluxes varied during 2012–2014, but that total emissions did not differ significantly among years, despite substantial differences in soil temperature and precipitation; year-to-year variability in these environmental conditions did not affect

  2. The atmospheric footprint of preindustrial, anthropogenic, and contemporary air-sea fluxes of CO2 estimated from an ocean inversion

    NASA Astrophysics Data System (ADS)

    Mikaloff Fletcher, S. E.; Gruber, N. P.; Sarmiento, J. L.; Jacobson, A. R.

    2006-12-01

    Air-sea exchange is a primary determinant of the spatial pattern of atmospheric carbon dioxide, yet there are substantial gaps in our understanding of the impact of the oceans on these gradients. Recent inverse modeling studies have used ocean interior observations of dissolved inorganic carbon (DIC) and other tracers and Ocean General Circulation Models (OGCMs) to estimate separately the natural air-sea flux that already existed in preindustrial times and the component of the air-sea flux that is due to the anthropogenic perturbation of atmospheric CO2. The sum of these components is the contemporary air-sea flux. Furthermore, the results from the ocean inversion have been combined with an analogous atmospheric inversion using surface observations of atmospheric carbon dioxide concentrations and atmospheric transport models to estimate air- sea and air-land fluxes. This work suggested that there might be an unexpectedly large source of carbon dioxide to the atmosphere from tropical land regions. We use the air-sea fluxes estimated from this ocean inversion together with estimates of the seasonal cycle of these fluxes from ΔpCO2 observations and bulk parameterizations as boundary conditions for the Model for Ozone And Related chemical Tracers (MOZART). The effects of preindustrial, anthropogenic, and contemporary air-sea fluxes on the spatial pattern of atmospheric CO2 are analyzed and the implications for ocean interior transport are discussed. In addition, we use atmospheric observations of 13C/12C isotopic ratios in carbon dioxide to independently test the finding of a large terrestrial source in the tropics, since the terrestrial biosphere discriminates against 13C much more strongly than the oceans.

  3. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-08-01

    , attributed partly to weaker atmospheric oxidation and SOC formation compared to summer. Enhanced SOC formation from oxidization and anthropogenic activities like biomass combustion is judged to have crucial effects on severe haze events characterized by high particle concentrations. Several observational studies indicate an increasing trend in ambient OC / EC (but not in OC or EC individually) from 2000 to 2010, confirming increased atmospheric oxidation of OC across the country. Combining the results of emission estimation and observations, the improvement over prior emission inventories is indicated by inter-annual comparisons and correlation analysis. It is also indicated, however, that the estimated growth in emissions might be faster than observed growth, and that some sources with high primary OC / EC, such as burning of biomass, are still underestimated. Further studies to determine changing EFs over time in the residential sector and to compare to other measurements, such as satellite observations, are thus suggested to improve understanding of the levels and trends of primary carbonaceous aerosol emissions in China.

  4. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-03-01

    remote sites, attributed partly to weaker atmospheric oxidation and SOC formation compared to summer. Enhanced SOC formation from oxidization and anthropogenic activities like biomass combustion is judged to have crucial effects on severe haze events characterized by high particle concentrations. Several observational studies indicate an increasing trend in ambient OC/EC (but not in OC or EC individually) from 2000 to 2010, confirming increased atmospheric oxidation of OC across the country. Combining the results of emission estimation and observations, the improvement over prior emission inventories is indicated by inter-annual comparisons and correlation analysis. It is also indicated, however, that the estimated growth in emissions might be faster than observed growth, and that some sources with high primary OC/EC like burning of biomass are still underestimated. Further studies to determine changing emission factors over time in the residential sector and to compare to other measurements such as satellite observations are thus suggested to improve understanding of the levels and trends of primary carbonaceous aerosol emissions in China.

  5. Sulfur isotope homogeneity of oceanic DMSP and DMS.

    PubMed

    Amrani, Alon; Said-Ahmad, Ward; Shaked, Yeala; Kiene, Ronald P

    2013-11-12

    Oceanic emissions of volatile dimethyl sulfide (DMS) represent the largest natural source of biogenic sulfur to the global atmosphere, where it mediates aerosol dynamics. To constrain the contribution of oceanic DMS to aerosols we established the sulfur isotope ratios ((34)S/(32)S ratio, δ(34)S) of DMS and its precursor, dimethylsulfoniopropionate (DMSP), in a range of marine environments. In view of the low oceanic concentrations of DMS/P, we applied a unique method for the analysis of δ(34)S at the picomole level in individual compounds. Surface water DMSP collected from six different ocean provinces revealed a remarkable consistency in δ(34)S values ranging between +18.9 and +20.3‰. Sulfur isotope composition of DMS analyzed in freshly collected seawater was similar to δ(34)S of DMSP, showing that the in situ fractionation between these species is small (<+1‰). Based on volatilization experiments, emission of DMS to the atmosphere results in a relatively small fractionation (-0.5 ± 0.2‰) compared with the seawater DMS pool. Because δ(34)S values of oceanic DMS closely reflect that of DMSP, we conclude that the homogenous δ(34)S of DMSP at the ocean surface represents the δ(34)S of DMS emitted to the atmosphere, within +1‰. The δ(34)S of oceanic DMS flux to the atmosphere is thus relatively constant and distinct from anthropogenic sources of atmospheric sulfate, thereby enabling estimation of the DMS contribution to aerosols.

  6. Estimating Latest Cretaceous and Tertiary Atmospheric PCO2 from Stomatal Indices

    NASA Astrophysics Data System (ADS)

    Royer, D. L.; Wing, S. L.; Beerling, D. J.

    2001-05-01

    Most modern C3 seed plants show an inverse relationship between PCO2 and stomatal index (SI), where SI is the proportion of epidermal cells that are stomatal packages. This plant-atmosphere response therefore provides a reliable approach for estimating paleo-CO2 levels. Since stomatal responses to CO2 are generally species-specific, one is limited in paleo-reconstructions to species that exist both in the fossil record and living today. Fossils morphologically similar to living Ginkgo biloba and Metasequoia glyptostroboides extend back to the early and late Cretaceous, respectively, indicating that the fossil and living forms are very closely related. Measurements of SI made on fossil Ginkgo and Metasequoia were calibrated with historical collections of G. biloba and M. glyptostroboides leaves from sites that developed during the anthropogenically-driven CO2 increases of the past 145 years (288-369 ppmv) and with saplings of G. biloba and M. glyptostroboides grown in CO2 controlled growth chambers (350-800 ppmv). Both nonlinear regressions are highly significant (Ginkgo: n = 40, r2 = 0.91; Metasequoia: n = 18; r2 = 0.85). Results from a sequence of 23 latest Cretaceous to early Eocene-aged Ginkgo-bearing sites indicate that CO2 remained between 300 and 450 ppmv with the exception of one high estimate ( ~800 ppmv) near the Paleocene/Eocene boundary, and results from 4 middle Miocene-aged Ginkgo- and Metasequoia-bearing sites indicate that CO2 was between 320 and 400 ppmv. If correct, the CO2 values estimated here are too low to explain via the CO2 greenhouse effect alone the higher global mean temperatures (e.g., 3-4 ° C for the early Eocene) inferred from models and geological data for these two intervals.

  7. Using stable isotope ratios to estimate atmospheric nitrogen fixed by cyanobacteria at the ecosystem scale.

    PubMed

    Woodland, Ryan J; Cook, Perran L M

    2014-04-01

    Diazotrophic cyanobacteria are capable of fixing atmospheric N2 to satisfy their physiological nitrogen requirements. This process can result in the transfer of substantial amounts of "new" diazotrophic nitrogen (ND) to aquatic ecosystems during blooms of these taxa. Using in situ measurements of plankton natural abundance stable isotope composition and a combination of underway and fixed site survey data, the total N(D) flux into the Gippsland Lakes estuary (Australia) was estimated during a summer bloom of the diazotrophic cyanobacterium Nodularia spumigena. Over the course of the bloom, N(D) increased in the upper water column of the estuary from 33% +/- 17% (mean +/- SD) to 73% +/- 13% of the standing pool of total particulate N. A conservative estimate of total N(D) flux (146 Mg) equates to an estimated 177% of the summer total N load and 22% of the annual total N load to the estuary. Combining natural abundance stable isotope measurements with relatively simple fixed and underway survey designs can provide a cost-effective approach for monitoring the N(D) flux into estuary or lacustrine environments. This approach relies on an isotopic differential between the diazotrophic and the non-diazotrophic components of the plankton community; it may not be appropriate in ecosystems that experience low-level blooms or blooms of intermittent N-fixing cyanobacteria. Large-scale blooms of diazotrophic cyanobacteria are considered uncommon in estuaries, yet it is clear that these blooms can represent major sources of new N to estuarine ecosystems when and where they occur.

  8. The contribution of evaporation from the Great Lakes to the continental atmosphere: estimate based on stable isotope data

    USGS Publications Warehouse

    Gat, Joel R.; Bowser, Carl J.; Kendall, Carol

    1994-01-01

    The isotopic composition of precipitation and river runoff in the vicinity of the North American Great Lakes is characterized by a higher deuterium-excess value than observed in the advecting air masses. It is suggested that this indicates that evaporated moisture from the surface waters is mixed with the atmosphere waters. A preliminary estimate of the atmospheric water balance during summer and autumn indicates that between 4.6%–15.7% of the atmospheric water content downwind from the Great Lakes is derived from lake evaporation during summer.

  9. Lunar sulfur

    NASA Technical Reports Server (NTRS)

    Kuck, David L.

    1991-01-01

    Ideas introduced by Vaniman, Pettit and Heiken in their 1988 Uses of Lunar Sulfur are expanded. Particular attention is given to uses of SO2 as a mineral-dressing fluid. Also introduced is the concept of using sulfide-based concrete as an alternative to the sulfur-based concretes proposed by Leonard and Johnson. Sulfur is abundant in high-Ti mare basalts, which range from 0.16 to 0.27 pct. by weight. Terrestrial basalts with 0.15 pct. S are rare. For oxygen recovery, sulfur must be driven off with other volatiles from ilmenite concentrates, before reduction. Troilite (FeS) may be oxidized to magnetite (Fe3O4) and SO2 gas, by burning concentrates in oxygen within a magnetic field, to further oxidize ilmenite before regrinding the magnetic reconcentration. SO2 is liquid at -20 C, the mean temperature underground on the Moon, at a minimum of 0.6 atm pressure. By using liquid SO2 as a mineral dressing fluid, all the techniques of terrestrial mineral separation become available for lunar ores and concentrates. Combination of sulfur and iron in an exothermic reaction, to form iron sulfides, may be used to cement grains of other minerals into an anhydrous iron-sulfide concrete. A sulfur-iron-aggregate mixture may be heated to the ignition temperature of iron with sulfur to make a concrete shape. The best iron, sulfur, and aggregate ratios need to be experimentally established. The iron and sulfur will be by-products of oxygen production from lunar minerals.

  10. The potential for regional-scale bias in top-down CO2 flux estimates due to atmospheric transport errors

    NASA Astrophysics Data System (ADS)

    Miller, S. M.; Fung, I.; Liu, J.; Hayek, M. N.; Andrews, A. E.

    2014-09-01

    Estimates of CO2 fluxes that are based on atmospheric data rely upon a meteorological model to simulate atmospheric CO2 transport. These models provide a quantitative link between surface fluxes of CO2 and atmospheric measurements taken downwind. Therefore, any errors in the meteorological model can propagate into atmospheric CO2 transport and ultimately bias the estimated CO2 fluxes. These errors, however, have traditionally been difficult to characterize. To examine the effects of CO2 transport errors on estimated CO2 fluxes, we use a global meteorological model-data assimilation system known as "CAM-LETKF" to quantify two aspects of the transport errors: error variances (standard deviations) and temporal error correlations. Furthermore, we develop two case studies. In the first case study, we examine the extent to which CO2 transport uncertainties can bias CO2 flux estimates. In particular, we use a common flux estimate known as CarbonTracker to discover the minimum hypothetical bias that can be detected above the CO2 transport uncertainties. In the second case study, we then investigate which meteorological conditions may contribute to month-long biases in modeled atmospheric transport. We estimate 6 hourly CO2 transport uncertainties in the model surface layer that range from 0.15 to 9.6 ppm (standard deviation), depending on location, and we estimate an average error decorrelation time of ∼2.3 days at existing CO2 observation sites. As a consequence of these uncertainties, we find that CarbonTracker CO2 fluxes would need to be biased by at least 29%, on average, before that bias were detectable at existing non-marine atmospheric CO2 observation sites. Furthermore, we find that persistent, bias-type errors in atmospheric transport are associated with consistent low net radiation, low energy boundary layer conditions. The meteorological model is not necessarily more uncertain in these conditions. Rather, the extent to which meteorological uncertainties

  11. The influence of diesel-truck exhaust particles on the kinetics of the atmospheric oxidation of dissolved sulfur dioxide by oxygen.

    PubMed

    Meena, Vimlesh Kumar; Dhayal, Yogpal; Saxena, Deepa; Rani, Ashu; Chandel, C P Singh; Gupta, K S

    2016-09-01

    The automobile exhausts are one of the major sources of particulate matter in urban areas and these particles are known to influence the atmospheric chemistry in a variety of ways. Because of this, the oxidation of dissolved sulfur dioxide by oxygen was studied in aqueous suspensions of particulates, obtained by scraping the particles deposited inside a diesel truck exhaust pipe (DEP). A variation in pH showed the rate to increase with increase in pH from 5.22 to about ∼6.3 and to decrease thereafter becoming very slow at pH = 8.2. In acetate-buffered medium, the reaction rate was higher than the rate in unbuffered medium at the same pH. Further, the rate was found to be higher in suspension than in the leachate under otherwise identical conditions. And, the reaction rate in the blank reaction was the slowest. This appears to be due to catalysis by leached metal ions in leachate and due to catalysis by leached metal ions and particulate surface both in suspensions. The kinetics of dissolved SO2 oxidation in acetate-buffered medium as well as in unbuffered medium at pH = 5.22 were defined by rate law: k obs  = k 0 + k cat [DEP], where k obs and k 0 are observed rate constants in the presence and the absence of DEP and k cat is the rate constant for DEP-catalyzed pathway. At pH = 8.2, the reaction rate was strongly inhibited by DEP in buffered and unbuffered media. Results suggest that the DEP would have an inhibiting effect in those areas where rainwater pH is 7 or more. These results at high pH are of particular significance to the Indian subcontinent, because of high rainwater pH. Conversely, it indicates the DEP to retard the oxidation of dissolved SO2 and control rainwater acidification.

  12. Assessment of model estimates of land-atmosphere CO2 exchange across northern Eurasia

    USGS Publications Warehouse

    Rawlins, M.A.; McGuire, A.D.; Kimball, J.S.; Dass, P.; Lawrence, D.; Burke, E.; Chen, X.; Delire, C.; Koven, C.; MacDougall, A.; Peng, S.; Rinke, A.; Saito, K.; Zhang, W.; Alkama, R.; Bohn, T. J.; Ciais, P.; Decharme, B.; Gouttevin, I.; Hajima, T.; Ji, D.; Krinner, G.; Lettenmaier, D.P.; Miller, P.; Moore, J.C.; Smith, B.; Sueyoshi, T.

    2015-01-01

    A warming climate is altering land-atmosphere exchanges of carbon, with a potential for increased vegetation productivity as well as the mobilization of permafrost soil carbon stores. Here we investigate land-atmosphere carbon dioxide (CO2) cycling through analysis of net ecosystem productivity (NEP) and its component fluxes of gross primary productivity (GPP) and ecosystem respiration (ER) and soil carbon residence time, simulated by a set of land surface models (LSMs) over a region spanning the drainage basin of Northern Eurasia. The retrospective simulations cover the period 1960–2009 at 0.5° resolution, which is a scale common among many global carbon and climate model simulations. Model performance benchmarks were drawn from comparisons against both observed CO2 fluxes derived from site-based eddy covariance measurements as well as regional-scale GPP estimates based on satellite remote-sensing data. The site-based comparisons depict a tendency for overestimates in GPP and ER for several of the models, particularly at the two sites to the south. For several models the spatial pattern in GPP explains less than half the variance in the MODIS MOD17 GPP product. Across the models NEP increases by as little as 0.01 to as much as 0.79 g C m−2 yr−2, equivalent to 3 to 340 % of the respective model means, over the analysis period. For the multimodel average the increase is 135 % of the mean from the first to last 10 years of record (1960–1969 vs. 2000–2009), with a weakening CO2 sink over the latter decades. Vegetation net primary productivity increased by 8 to 30 % from the first to last 10 years, contributing to soil carbon storage gains. The range in regional mean NEP among the group is twice the multimodel mean, indicative of the uncertainty in CO2 sink strength. The models simulate that inputs to the soil carbon pool exceeded losses, resulting in a net soil carbon gain amid a decrease in residence time. Our analysis points to improvements in model

  13. Testing a Simple Recipe for Estimating Thermal Hydrodynamic Escape Rates in Primitive Terrestrial Atmospheres

    NASA Astrophysics Data System (ADS)

    Friedson, A. J.; Yung, Y. L.; Chen, P.

    2014-12-01

    During the first billion years of the Sun's history, the emission of ultraviolet and X-ray radiation varied from ~100 to ~6 times greater than its present level. The absorption of this intense radiation in the upper atmospheres of the terrestrial planets is believed to have driven rapid hydrodynamic escape, either in the form of energy-limited escape or transonic blow-off. The calculation of escape rates under these circumstances, and in particular the nature of the correct condition to apply at the upper boundary, depends on whether or not the flow remains subsonic below the exobase. If the flow remains subsonic, the kinetic Jeans equations may be applied at the exobase; otherwise, the radius of the sonic point must be located and then appropriate boundary conditions applied at this radius. This seems to suggest that the full hydrodynamic escape problem needs to be solved iteratively to determine where the sonic radius falls and the type of boundary conditions that should be applied. Such an arduous undertaking is generally impractical for standard application in chemical evolution models or related studies. Fortunately, a much easier but still accurate approach to determining whether the flow remains subsonic below the exobase for a given amount of energy deposition has been provided by Johnson et al. (2013, Ap. J. Lett. 768:L4), who base their results on rigorous Discrete Simulation Monte Carlo models. Their model provides the ratio of the escape rate to the energy-limited value as a function of the total XUV heating. The XUV heating, however, is itself coupled to the escape rate through the radial structure of the upper atmosphere, which can become greatly distended for large heating rates. Here we present a simple recipe for estimating the hydrodynamic escape rate that includes the coupling between the escape rate, the radial structure, and the XUV heating while avoiding the use of demanding numerical calculations. The approach involves an iterative semi

  14. Assessment of model estimates of land-atmosphere CO2 exchange across Northern Eurasia

    DOE PAGES

    Rawlins, M. A.; McGuire, A. D.; Kimball, J. S.; ...

    2015-07-28

    A warming climate is altering land-atmosphere exchanges of carbon, with a potential for increased vegetation productivity as well as the mobilization of permafrost soil carbon stores. Here we investigate land-atmosphere carbon dioxide (CO2) cycling through analysis of net ecosystem productivity (NEP) and its component fluxes of gross primary productivity (GPP) and ecosystem respiration (ER) and soil carbon residence time, simulated by a set of land surface models (LSMs) over a region spanning the drainage basin of Northern Eurasia. The retrospective simulations cover the period 1960–2009 at 0.5° resolution, which is a scale common among many global carbon and climate modelmore » simulations. Model performance benchmarks were drawn from comparisons against both observed CO2 fluxes derived from site-based eddy covariance measurements as well as regional-scale GPP estimates based on satellite remote-sensing data. The site-based comparisons depict a tendency for overestimates in GPP and ER for several of the models, particularly at the two sites to the south. For several models the spatial pattern in GPP explains less than half the variance in the MODIS MOD17 GPP product. Across the models NEP increases by as little as 0.01 to as much as 0.79 g C m⁻² yr⁻², equivalent to 3 to 340 % of the respective model means, over the analysis period. For the multimodel average the increase is 135 % of the mean from the first to last 10 years of record (1960–1969 vs. 2000–2009), with a weakening CO2 sink over the latter decades. Vegetation net primary productivity increased by 8 to 30 % from the first to last 10 years, contributing to soil carbon storage gains. The range in regional mean NEP among the group is twice the multimodel mean, indicative of the uncertainty in CO2 sink strength. The models simulate that inputs to the soil carbon pool exceeded losses, resulting in a net soil carbon gain amid a decrease in residence time. Our analysis points to improvements in

  15. Estimates of radioxenon released from Southern Hemisphere medical isotope production facilities using measured air concentrations and atmospheric transport modeling.

    PubMed

    Eslinger, Paul W; Friese, Judah I; Lowrey, Justin D; McIntyre, Justin I; Miley, Harry S; Schrom, Brian T

    2014-09-01

    The International Monitoring System (IMS) of the Comprehensive-Nuclear-Test-Ban-Treaty monitors the atmosphere for radioactive xenon leaking from underground nuclear explosions. Emissions from medical isotope production represent a challenging background signal when determining whether measured radioxenon in the atmosphere is associated with a nuclear explosion prohibited by the treaty. The Australian Nuclear Science and Technology Organisation (ANSTO) operates a reactor and medical isotope production facility in Lucas Heights, Australia. This study uses two years of release data from the ANSTO medical isotope production facility and (133)Xe data from three IMS sampling locations to estimate the annual releases of (133)Xe from medical isotope production facilities in Argentina, South Africa, and Indonesia. Atmospheric dilution factors derived from a global atmospheric transport model were used in an optimization scheme to estimate annual release values by facility. The annual releases of about 6.8 × 10(14) Bq from the ANSTO medical isotope production facility are in good agreement with the sampled concentrations at these three IMS sampling locations. Annual release estimates for the facility in South Africa vary from 2.2 × 10(16) to 2.4 × 10(16) Bq, estimates for the facility in Indonesia vary from 9.2 × 10(13) to 3.7 × 10(14) Bq and estimates for the facility in Argentina range from 4.5 × 10(12) to 9.5 × 10(12) Bq.

  16. A semiempirical error estimation technique for PWV derived from atmospheric radiosonde data

    NASA Astrophysics Data System (ADS)

    Castro-Almazán, Julio A.; Pérez-Jordán, Gabriel; Muñoz-Tuñón, Casiana

    2016-09-01

    A semiempirical method for estimating the error and optimum number of sampled levels in precipitable water vapour (PWV) determinations from atmospheric radiosoundings is proposed. Two terms have been considered: the uncertainties in the measurements and the sampling error. Also, the uncertainty has been separated in the variance and covariance components. The sampling and covariance components have been modelled from an empirical dataset of 205 high-vertical-resolution radiosounding profiles, equipped with Vaisala RS80 and RS92 sondes at four different locations: Güímar (GUI) in Tenerife, at sea level, and the astronomical observatory at Roque de los Muchachos (ORM, 2300 m a.s.l.) on La Palma (both on the Canary Islands, Spain), Lindenberg (LIN) in continental Germany, and Ny-Ålesund (NYA) in the Svalbard Islands, within the Arctic Circle. The balloons at the ORM were launched during intensive and unique site-testing runs carried out in 1990 and 1995, while the data for the other sites were obtained from radiosounding stations operating for a period of 1 year (2013-2014). The PWV values ranged between ˜ 0.9 and ˜ 41 mm. The method sub-samples the profile for error minimization. The result is the minimum error and the optimum number of levels. The results obtained in the four sites studied showed that the ORM is the driest of the four locations and the one with the fastest vertical decay of PWV. The exponential autocorrelation pressure lags ranged from 175 hPa (ORM) to 500 hPa (LIN). The results show a coherent behaviour with no biases as a function of the profile. The final error is roughly proportional to PWV whereas the optimum number of levels (N0) is the reverse. The value of N0 is less than 400 for 77 % of the profiles and the absolute errors are always < 0.6 mm. The median relative error is 2.0 ± 0.7 % and the 90th percentile P90 = 4.6 %. Therefore, whereas a radiosounding samples at least N0 uniform vertical levels, depending on the water

  17. Reduced models of atmospheric low-frequency variability: Parameter estimation and comparative performance

    NASA Astrophysics Data System (ADS)

    Strounine, K.; Kravtsov, S.; Kondrashov, D.; Ghil, M.

    2010-02-01

    Low-frequency variability (LFV) of the atmosphere refers to its behavior on time scales of 10-100 days, longer than the life cycle of a mid-latitude cyclone but shorter than a season. This behavior is still poorly understood and hard to predict. The present study compares various model reduction strategies that help in deriving simplified models of LFV. Three distinct strategies are applied here to reduce a fairly realistic, high-dimensional, quasi-geostrophic, 3-level (QG3) atmospheric model to lower dimensions: (i) an empirical-dynamical method, which retains only a few components in the projection of the full QG3 model equations onto a specified basis, and finds the linear deterministic and the stochastic corrections empirically as in Selten (1995) [5]; (ii) a purely dynamics-based technique, employing the stochastic mode reduction strategy of Majda et al. (2001) [62]; and (iii) a purely empirical, multi-level regression procedure, which specifies the functional form of the reduced model and finds the model coefficients by multiple polynomial regression as in Kravtsov et al. (2005) [3]. The empirical-dynamical and dynamical reduced models were further improved by sequential parameter estimation and benchmarked against multi-level regression models; the extended Kalman filter was used for the parameter estimation. Overall, the reduced models perform better when more statistical information is used in the model construction. Thus, the purely empirical stochastic models with quadratic nonlinearity and additive noise reproduce very well the linear properties of the full QG3 model’s LFV, i.e. its autocorrelations and spectra, as well as the nonlinear properties, i.e. the persistent flow regimes that induce non-Gaussian features in the model’s probability density function. The empirical-dynamical models capture the basic statistical properties of the full model’s LFV, such as the variance and integral correlation time scales of the leading LFV modes, as well as

  18. Dissimilarity between temperature-humidity in the atmospheric surface layer and implications for estimates of evaporation

    NASA Astrophysics Data System (ADS)

    Cancelli, D. M.; Dias, N. L.; Chamecki, M.

    2012-12-01

    In several methods used in water resources to estimate evaporation from land and water surfaces, a fundamental assumption is that temperature (T) and specific humidity (q) fluctuations behave similarly in the atmospheric surface layer (ASL). In the Energy-Budget Bowen Ratio method it is assumed that both eddy diffusivities are equal, while in the variance method it is often assumed that all the Monin-Obukhov Similarity (MOS) functions for the two scalars are equal. However, it is well-known that the T-q similarity does not always hold and that the dissimilarity found in practice can significantly impact the estimates of evaporation. Given the frequent dissimilarity between temperature and humidity, two important problems arise. The first one is related to the choice of the function used to characterize scalar similarity, given that not all commonly used functions are equally capable of identifying scalar dissimilarity. The second problem is associated with the identification of the physical mechanisms behind scalar dissimilarity in each particular case: local advection, nonstationarity, surface heterogeneity, active/passive roles of the scalars, entrainment fluxes at the top of the atmospheric boundary layer are typically cited as possible causes, but seldom a convincing argument is presented. In this work we combine experimental data and numerical simulations to study similarity between T and q in the ASL. Data measured over a lake in Brazil suggests a strong relationship between scalar similarity and the balance between local production and dissipation of scalar variance, which is in practice related to the strength of the surface forcing. Scalar variance and covariance budgets are used to derive a set of dimensionless Scalar Flux numbers that are capable of diagnosing the balance between gradient production and molecular dissipation of scalar variance and covariance. Experimental data shows that these Scalar Flux numbers are good predictors of scalar (dis

  19. Estimates of Methane and Ethane Emissions from the Barnett Shale Using Atmospheric Measurements

    NASA Astrophysics Data System (ADS)

    Karion, A.; Sweeney, C.; Kort, E. A.; Shepson, P. B.; Conley, S. A.; Lauvaux, T.; Davis, K. J.; Deng, A.; Lyon, D. R.; Smith, M. L.

    2015-12-01

    Recent development of horizontal drilling technology and advances in hydraulic fracturing techniques by the oil and gas industry have dramatically increased onshore U.S. natural gas and oil production in the last several years. The primary component of natural gas is methane (CH4), a powerful greenhouse gas; therefore, natural gas leakage into the atmosphere affects its climate impact. We present estimates of regional methane (CH4) and ethane (C2H6) emissions from oil and natural gas operations in the Barnett Shale, Texas, made in March and October 2013 as part of the Environmental Defense Fund's Barnett Coordinated Campaign. The Barnett is one of the largest production basins in the United States, with 8% of total U.S. natural gas production, and thus, our results represent a crucial step toward determining the greenhouse gas footprint of U.S. onshore natural gas production. Using a mass balance approach on eight different flight days the total CH4 emissions for the region are estimated to be 76 ± 13x 103 kg/hr, or 0.66 ± 0.11 Tg CH4 /yr; (95% CI). Repeated mass balance flights in the same basin on eight different days and two seasons demonstrate the consistency of the mass balance approach. On the basis of airborne C2H6 and CH4 measurements, we find 71-85% of the observed CH4 emissions quantified in the Barnett Shale are derived from fossil sources. The average C2H6 flux was 6.6 ± 0.2 x 103 kg/hr and consistent across six days in spring and fall of 2013. This result is the first demonstration of this approach for C2H6. We estimate that 60±11x103 kg CH4/hr (95% CI) are emitted by natural gas and oil operations, including production, processing, and distribution in the urban areas of Dallas and Fort Worth. This estimate is significantly higher than emissions reported by the EDGAR inventory or by industry to EPA's Greenhouse Gas Reporting Program.

  20. Refining our estimate of atmospheric CO2 across the Eocene-Oligocene climatic transition

    NASA Astrophysics Data System (ADS)

    Heureux, Ana M. C.; Rickaby, Rosalind E. M.

    2015-01-01

    The Eocene-Oligocene transition (EOT) followed by Oligocene isotope event 1 (Oi-1) is a dramatic global switch in climate characterized by deep-sea cooling and the first formation of permanent Antarctic ice. Models and proxy evidence suggest that declining partial pressure of atmospheric carbon dioxide (CO2atm) below a threshold may explain the onset of global cooling and associated ice formation at Oi-1. However, significant uncertainty remains in the estimated values and salient features of reconstructed CO2atm across this interval. In this study, we present novel carbon isotope records from size separated diatom associated organic matter (δ13Cdiatom) preserved in silica frustules. Physical preservation of this material allows concurrent investigation of isotopic and cell size information, providing two input parameters for biogeochemical models and the reconstruction of CO2atm. We estimate CO2atm in two ways; first we use size and reaction-diffusion kinetics of a cell to calculate a CO2atm threshold. Second we use the calibrated relationship between ɛp(diatom) and carbon dioxide from culture and field studies to create a record of CO2atm prior to and across the transition. Our study, from site 1090 in the Atlantic sector of the Southern Ocean, shows CO2atm values fluctuating between 900 and 1700 ± 100 p.p.m.v. across the EOT followed by a drop to values in the order of 700 to 800 ± 100 p.p.m.v. just prior to the onset of Oi-1. Our values and magnitude of CO2atm change differ from previous estimates, but confirm the overall trends inferred from boron isotopes and alkenones, including a marked rebound following Oi-1. Due to the intricate nature of the climate system and complexities in constraining paleo-proxies, this work emphasizes the importance of a multi-proxy approach to estimating of CO2atm in order to elucidate its role in the emplacement of Antarctic ice-sheets at the EOT.

  1. Are the clouds of Venus sulfuric acid.

    NASA Technical Reports Server (NTRS)

    Young, A. T.

    1973-01-01

    It is shown that strong aqueous sulfuric acid solutions have the right refractive index and freeze at Venusian cloud temperature, explain the dryness of the Venusian stratosphere, are consistent with some features of the Venusian IR spectrum, and do not absorb in highly reflecting areas of Venus. It is also indicated that such solutions should be produced by reactions between known atmospheric constituents and most sulfur-bearing rock at the Venusian surface temperature, and require only small amounts of sulfur consistent with its cosmic abundance and with the amounts of other volatile elements present in the atmosphere. It is believed therefore that the clouds of Venus consist of sulfuric acid solutions.

  2. Assessment of an atmospheric transport model for annual inverse estimates of California greenhouse gas emissions

    NASA Astrophysics Data System (ADS)

    Bagley, Justin E.; Jeong, Seongeun; Cui, Xinguang; Newman, Sally; Zhang, Jingsong; Priest, Chad; Campos-Pineda, Mixtli; Andrews, Arlyn E.; Bianco, Laura; Lloyd, Matthew; Lareau, Neil; Clements, Craig; Fischer, Marc L.

    2017-02-01

    Atmospheric inverse estimates of gas emissions depend on transport model predictions, hence driving a need to assess uncertainties in the transport model. In this study we assess the uncertainty in WRF-STILT (Weather Research and Forecasting and Stochastic Time-Inverted Lagrangian Transport) model predictions using a combination of meteorological and carbon monoxide (CO) measurements. WRF configurations were selected to minimize meteorological biases using meteorological measurements of winds and boundary layer depths from surface stations and radar wind profiler sites across California. We compare model predictions with CO measurements from four tower sites in California from June 2013 through May 2014 to assess the seasonal biases and random errors in predicted CO mixing ratios. In general, the seasonal mean biases in boundary layer wind speed (< 0.5 m/s), direction (< 15°), and boundary layer height (< 200 m) were small. However, random errors were large ( 1.5-3.0 m/s for wind speed, 40-60° for wind direction, and 300-500 m for boundary layer height). Regression analysis of predicted and measured CO yielded near-unity slopes (i.e., within 1.0 ± 0.20) for the majority of sites and seasons, though a subset of sites and seasons exhibit larger ( 30%) uncertainty, particularly when weak winds combined with complex terrain in the South Central Valley of California. Looking across sites and seasons, these results suggest that WRF-STILT simulations are sufficient to estimate emissions of CO to up to 15% on annual time scales across California.

  3. Assessment of model land skin temperature and surface-atmosphere coupling using remotely sensed estimates

    NASA Astrophysics Data System (ADS)

    Trigo, Isabel; Boussetta, Souhail; Balsamo, Gianpaolo; Viterbo, Pedro; Beljaars, Anton; Sandu, Irina

    2016-04-01

    The coupling between land surface and the atmosphere is a key feature in Earth System Modelling for exploiting the predictability of slowly evolving geophysical variables (e.g., soil moisture or vegetation state), and for correctly representing rapid variations within the diurnal cycle, particularly relevant in data assimilation applications. Land Surface Temperature (LST) routinely estimated from Meteosat Second Generation (MSG) by the LandSAF is used to assess the European Centre for Medium-range Weather Forecasts (ECMWF) skin temperature. LST can be interpreted as a radiative temperature of the model surface, which is close to the ECMWF modelled skin temperature. It is shown that the model tends to slightly overestimate skin temperature during night-time and underestimate daytime values. Such underestimation of daily amplitudes is particularly pronounced in (semi-)arid regions, suggesting a misrepresentation of surface energy fluxes in those areas. The LST estimated from MSG is used to evaluate the impact of changes in some of the ECMWF model surface parameters. The introduction of more realistic model vegetation is shown to have a positive, but limited impact on skin temperature: long integration leads to an equilibrium state where changes in the latent heat flux and soil moisture availability compensate each other. Revised surface roughness lengths for heat and momentum, however, lead to overall positive impact on daytime skin temperature, mostly due to a reduction of sensible heat flux. This is particularly relevant in non-vegetated areas, unaffected by model vegetation. The reduction of skin conductivity, a parameter which controls the heat transfer to ground by diffusion, is shown to further improve the model skin temperature. A revision of the vertical soil discretization is also expected to improve the match to the LST, particularly over sparsely vegetated areas. The impact of a finer discretization (10-layer soil) is currently ongoing; preliminary

  4. Top-of-the-Atmosphere Shortwave Flux Estimation from UV Observations: An Empirical Approach

    NASA Technical Reports Server (NTRS)

    Gupta, P.; Joiner, Joanna; Vasilkov, A.; Bhartia, P. K.; da Silva, Arlindo

    2012-01-01

    Measurements of top of the atmosphere (TOA) radiation are essential to the understanding of Earth's climate. Clouds, aerosols, and ozone (0,) are among the most important agents impacting the Earth's short-wave (SW) radiation budget. There are several sensors in orbit that provide independent information related to the Earth's SW radiation budget. Having coincident information from these sensors is important for understanding their potential contributions. The A-train constellation of satellites provides a unique opportunity to analyze near-simultaneous data from several of these sensors. They include the Ozone Monitoring Instrument (OMI), on the NASA Aura satellite, that makes TOA hyper-spectral measurements from ultraviolet (UV) to visible wavelengths, and Clouds and the Earth's Radiant Energy System (CERES) instrument, on the NASA Aqua satellite, that makes broadband measurements in both the long- and short-wave. OMI measurements have been successfully utilized to derive the information on trace gases (e.g., 0 1, NO" and SO,), clouds, and absorbing aerosols. TOA SW fluxes are estimated using a combination of data from CERES and the Aqua MODerate-resolution Imaging Spectroradiometer (MODIS). In this paper, OMI retrievals of cloud/aerosol parameters and 0 1 have been collocated with CERES TOA SW flux retrievals. We use this collocated data to develop a neural network that estimates TOA shortwave flux globally over ocean using data from OMI and meteorological analyses. This input data include the effective cloud fraction, cloud optical centroid pressure (OCP), total-column 0" and sun-satellite viewing geometry from OMI as well as wind speed and water vapor from the Goddard Earth Observing System 5 Modern Era Retrospective-analysis for Research and Applications (GEOS-5 MERRA) along with a climatology of chlorophyll content. We train the neural network using a subset of CERES retrievals of TOA SW flux as the target output (truth) and withhold a different subset of

  5. Methane emissions in East Asia for 2000-2011 estimated using an atmospheric Bayesian inversion

    NASA Astrophysics Data System (ADS)

    Thompson, R. L.; Stohl, A.; Zhou, L. X.; Dlugokencky, E.; Fukuyama, Y.; Tohjima, Y.; Kim, S.-Y.; Lee, H.; Nisbet, E. G.; Fisher, R. E.; Lowry, D.; Weiss, R. F.; Prinn, R. G.; O'Doherty, S.; Young, D.; White, J. W. C.

    2015-05-01

    We present methane (CH4) emissions for East Asia from a Bayesian inversion of CH4 mole fraction and stable isotope (δ13C-CH4) measurements. Emissions were estimated at monthly resolution from 2000 to 2011. A posteriori, the total emission for East Asia increased from 43 ± 4 to 59 ± 4 Tg yr-1 between 2000 and 2011, owing largely to the increase in emissions from China, from 39 ± 4 to 54 ± 4 Tg yr-1, while emissions in other East Asian countries remained relatively stable. For China, South Korea, and Japan, the total emissions were smaller than the prior estimates (i.e., Emission Database for Global Atmospheric Research 4.2 FT2010 for anthropogenic emissions) by an average of 29%, 20%, and 23%, respectively. For Mongolia, Taiwan, and North Korea, the total emission was less than 2 Tg yr-1 and was not significantly different from the prior. The largest reductions in emissions, compared to the prior, occurred in summer in regions important for rice agriculture suggesting that this source is overestimated in the prior. Furthermore, an analysis of the isotope data suggests that the prior underestimates emissions from landfills and ruminant animals for winter 2010 to spring 2011 (no data available for other times). The inversion also found a lower average emission trend for China, 1.2 Tg yr-1 compared to 2.8 Tg yr-1 in the prior. This trend was not constant, however, and increased significantly after 2005, up to 2.0 Tg yr-1. Overall, the changes in emissions from China explain up to 40% of the increase in global emissions in the 2000s.

  6. Sulfuric acid as autocatalyst in the formation of sulfuric acid.

    PubMed

    Torrent-Sucarrat, Miquel; Francisco, Joseph S; Anglada, Josep M

    2012-12-26

    Sulfuric acid can act as a catalyst of its own formation. We have carried out a computational investigation on the gas-phase formation of H(2)SO(4) by hydrolysis of SO(3) involving one and two water molecules, and also in the presence of sulfuric acid and its complexes with one and two water molecules. The hydrolysis of SO(3) requires the concurrence of two water molecules, one of them acting as a catalyzer, and our results predict an important catalytic effect, ranging between 3 and 11 kcal·mol(-1) when the catalytic water molecule is substituted by a sulfuric acid molecule or one of its hydrates. In these cases, the reaction products are either bare sulfuric acid dimer or sulfuric acid dimer complexed with a water molecule. There are broad implications from these new findings. The results of the present investigation show that the catalytic effect of sulfuric acid in the SO(3) hydrolysis can be important in the Earth's stratosphere, in the heterogeneous formation of sulfuric acid and in the formation of aerosols, in H(2)SO(4) formation by aircraft engines, and also in understanding the formation of sulfuric acid in the atmosphere of Venus.

  7. Spacebased Estimation of Moisture Transport in Marine Atmosphere Using Support Vector Regression

    NASA Technical Reports Server (NTRS)

    Xie, Xiaosu; Liu, W. Timothy; Tang, Benyang

    2007-01-01

    An improved algorithm is developed based on support vector regression (SVR) to estimate horizonal water vapor transport integrated through the depth of the atmosphere ((Theta)) over the global ocean from observations of surface wind-stress vector by QuikSCAT, cloud drift wind vector derived from the Multi-angle Imaging SpectroRadiometer (MISR) and geostationary satellites, and precipitable water from the Special Sensor Microwave/Imager (SSM/I). The statistical relation is established between the input parameters (the surface wind stress, the 850 mb wind, the precipitable water, time and location) and the target data ((Theta) calculated from rawinsondes and reanalysis of numerical weather prediction model). The results are validated with independent daily rawinsonde observations, monthly mean reanalysis data, and through regional water balance. This study clearly demonstrates the improvement of (Theta) derived from satellite data using SVR over previous data sets based on linear regression and neural network. The SVR methodology reduces both mean bias and standard deviation comparedwith rawinsonde observations. It agrees better with observations from synoptic to seasonal time scales, and compare more favorably with the reanalysis data on seasonal variations. Only the SVR result can achieve the water balance over South America. The rationale of the advantage by SVR method and the impact of adding the upper level wind will also be discussed.

  8. Estimation of explosive gas ejected in the atmosphere at different stages of the 2013 Tolbachik eruption

    NASA Astrophysics Data System (ADS)

    Makarov, Evgeny; Makhmudov, Evgeny; Firstov, Pavel; Akbashev, Rinat

    2014-05-01

    The Tolbachik Fissure eruption named after the 50-th Anniversary of the Institute of Volcanology and Seismology FEB RAS (TFE-50) occurred on 26-th November 2012 in the southern areal zone of NNE cinder cones called "Tolbachik Dol". The 1975 -1976 Great Tolbachik Fissure Eruption (GTFE) occurred in the same area and resulted in three cones of the North Vent and one cone of the South Vent located 18 km and 28 km of Plosky Tolbachik Volcano, respectively. The GTFE was a good example to study air shock waves that accompanied various types of activity. It was suggested for the first time in the worldwide volcanological investigations that acoustic signals in a range of 1-10 Hz associated with the burst of gas bubbles during Strombolian eruptions and the processes related to the fragmentation of magma during Vulcanian eruptions, are revealed to be the air shock waves (ASW). The amount of gas ejected during the eruption is one of the key features of the volcano's activity. In a case study of three Strombolian eruptions, it was suggested that the volume of liberated gas can be estimated by acoustic emission that occurred during the destruction of bubble gases [Firstov, Kravchenko, 199]. Moreover, the calculation of the discharge of lava made possible to estimate the weight content of gas. This paper provides the estimation of explosive gas at various phases of the TFE-50 activity. In the area of TFE-50 infrasound vibrations in the atmosphere were recorded by P. Izbekov in February 11-13, 2013 and by the authors in May 13 and from August 12 to August 20, 2013. Besides, from August 14 to August 27 we recorded the volumenous activity of radon (OA Rn) in the soil air at a distance of 7 km of the TFE-50 crater. During the three periods of observations, we recorded weak air shock waves (ASW) accompanied the destruction of large lava bubbles at the surface of the lava lake and "lava fountains". Infrasound waves generated during the destruction of small bubbles were observed as

  9. Estimates of Radioxenon Released from Southern Hemisphere Medical isotope Production Facilities Using Measured Air Concentrations and Atmospheric Transport Modeling

    SciTech Connect

    Eslinger, Paul W.; Friese, Judah I.; Lowrey, Justin D.; McIntyre, Justin I.; Miley, Harry S.; Schrom, Brian T.

    2014-09-01

    Abstract The International Monitoring System (IMS) of the Comprehensive-Nuclear-Test-Ban-Treaty monitors the atmosphere for radioactive xenon leaking from underground nuclear explosions. Emissions from medical isotope production represent a challenging background signal when determining whether measured radioxenon in the atmosphere is associated with a nuclear explosion prohibited by the treaty. The Australian Nuclear Science and Technology Organisation (ANSTO) operates a reactor and medical isotope production facility in Lucas Heights, Australia. This study uses two years of release data from the ANSTO medical isotope production facility and Xe-133 data from three IMS sampling locations to estimate the annual releases of Xe-133 from medical isotope production facilities in Argentina, South Africa, and Indonesia. Atmospheric dilution factors derived from a global atmospheric transport model were used in an optimization scheme to estimate annual release values by facility. The annual releases of about 6.8×1014 Bq from the ANSTO medical isotope production facility are in good agreement with the sampled concentrations at these three IMS sampling locations. Annual release estimates for the facility in South Africa vary from 1.2×1016 to 2.5×1016 Bq and estimates for the facility in Indonesia vary from 6.1×1013 to 3.6×1014 Bq. Although some releases from the facility in Argentina may reach these IMS sampling locations, the solution to the objective function is insensitive to the magnitude of those releases.

  10. Cloud Effects on Meridional Atmospheric Energy Budget Estimated from Clouds and the Earth's Radiant Energy System (CERES) Data

    NASA Technical Reports Server (NTRS)

    Kato, Seiji; Rose, Fred G.; Rutan, David A.; Charlock, Thomas P.

    2008-01-01

    The zonal mean atmospheric cloud radiative effect, defined as the difference of the top-of-atmosphere (TOA) and surface cloud radiative effects, is estimated from three years of Clouds and the Earth's Radiant Energy System (CERES) data. The zonal mean shortwave effect is small, though it tends to be positive (warming). This indicates that clouds increase shortwave absorption in the atmosphere, especially in midlatitudes. The zonal mean atmospheric cloud radiative effect is, however, dominated by the longwave effect. The zonal mean longwave effect is positive in the tropics and decreases with latitude to negative values (cooling) in polar regions. The meridional gradient of cloud effect between midlatitude and polar regions exists even when uncertainties in the cloud effect on the surface enthalpy flux and in the modeled irradiances are taken into account. This indicates that clouds increase the rate of generation of mean zonal available potential energy. Because the atmospheric cooling effect in polar regions is predominately caused by low level clouds, which tend to be stationary, we postulate that the meridional and vertical gradients of cloud effect increase the rate of meridional energy transport by dynamics in the atmosphere from midlatitude to polar region, especially in fall and winter. Clouds then warm the surface in polar regions except in the Arctic in summer. Clouds, therefore, contribute in increasing the rate of meridional energy transport from midlatitude to polar regions through the atmosphere.

  11. Atmospheric observations and emissions estimates of methane and nitrous oxide from regional to global scale

    NASA Astrophysics Data System (ADS)

    Kort, Eric Adam

    2011-12-01

    Methane (CH4) and Nitrous Oxide (N2O) are the two most significant anthropogenic, long-lived, non-CO2 greenhouse gases, together perturbing the earth's energy balance by an amount comparable to that of CO2. This dissertation will focus on the use of atmospheric observations to quantify emissions of CH4 and N2O. First top-down emissions constraints on the regional scale, covering large areas of the U.S and southern Canada, are derived from airborne observations made in Spring of 2003. Using a receptor-oriented Lagrangian particle dispersion model provides robust validation of bottom-up emission estimates from EDGAR 32FT2000 and GEIA inventories. It is found that EDGAR CH4 emission rates are slightly low by a factor of 1.08 +/- 0.15 (2 sigma), while both EDGAR and GEIA N2O emissions are significantly too low, by factors of 2.62 +/- 0.50 and 3.05 +/- 0.61 respectively. This analysis is then extended over a full calendar year in 2004 with observations from NOAA's tall tower and aircraft profile network. EDGAR 32FT2000 CH 4 emissions are found to be consistent with observations, though the newer EDGAR v4.0 reduces CH4 emissions by 30%, and this reduction is not consistent with this study. Scaling factors found for N2O in May/June of 2003 (2.62 & 3.05) are found to hold for February-May of 2004, suggesting inventories are significantly too low in primary growing season coincident with significant fertilizer inputs. A new instrument for airborne observation of CO2, CH 4, N2O, and CO is introduced, and its operation and in-field performance are highlighted (demonstrated 1-sec precisions of 20 ppb, 0.5 ppb, 0.09 ppb, and 0.15 ppb respectively). Finally, global N2O observations collected with this sensor on the HIPPO (Hlaper Pole to Pole Observations) campaign are assessed. Comparison with a global model and subsequent inversion indicates strong, episodic inputs of nitrous oxide from tropical regions are necessary to bring observations and model in agreement. Findings

  12. Quantitative estimates of past changes in ITCZ position and cross-equatorial atmospheric heat transport

    NASA Astrophysics Data System (ADS)

    McGee, D.; Donohoe, A.; Marshall, J.; Ferreira, D.

    2012-12-01

    The mean position and seasonal migration of the Intertropical Convergence Zone (ITCZ) govern the intensity, spatial distribution and seasonality of precipitation throughout the tropics as well as the magnitude and direction of interhemispheric atmospheric heat transport (AHT). As a result of these links to global tropical precipitation and hemispheric heat budgets, paleoclimate studies have commonly sought to use reconstructions of local precipitation and surface winds to identify past shifts in the ITCZ's mean position or seasonal extent. Records indicate close ties between ITCZ position and interhemispheric surface temperature gradients in past climates, with the ITCZ shifting toward the warmer hemisphere. This shift would increase AHT into the cooler hemisphere to at least partially compensate for cooling there. Despite widespread qualitative evidence consistent with ITCZ shifts, few proxy records offer quantitative estimates of the distance of these shifts or of the associated changes in AHT. Here we present a strategy for placing quantitative limits on past changes in mean annual ITCZ position and interhemispheric AHT based on explorations of the modern seasonal cycle and models of present and past climates. We use reconstructions of tropical sea surface temperature gradients to place bounds on globally averaged ITCZ position and interhemispheric AHT during the Last Glacial Maximum, Heinrich Stadial 1, and the Mid-Holocene (6 ka). Though limited by the small number of SST records available, our results suggest that past shifts in the global mean ITCZ were small, typically less than 1 degree of latitude. Past changes in interhemispheric AHT may have been substantial, with anomalies approximately equal to the magnitude of modern interhemispheric AHT. Using constraints on the invariance of the total (ocean+atmosphere) heat transport we suggest possible bounds on fluctuations of the OHT and AMOC during Heinrich Stadial 1. We also explore ITCZ shifts in models and

  13. A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles

    NASA Astrophysics Data System (ADS)

    Hennigan, C. J.; Izumi, J.; Sullivan, A. P.; Weber, R. J.; Nenes, A.

    2014-11-01

    Given significant challenges with available measurements of aerosol acidity, proxy methods are frequently used to estimate the acidity of atmospheric particles. In this study, four of the most common aerosol acidity proxies are evaluated and compared: (1) the ion balance method, (2) the molar ratio method, (3) thermodynamic equilibrium models, and (4) the phase partitioning of ammonia. All methods are evaluated against predictions of thermodynamic models and against direct observations of aerosol-gas equilibrium partitioning acquired in Mexico City during the MILAGRO study. The ion balance and molar ratio methods assume that any deficit in inorganic cations relative to anions is due to the presence of H+; and that a higher H+ loading and lower cation/anion ratio both correspond to increasingly acidic particles (i.e., lower pH). Based on the MILAGRO measurements, no correlation is observed between H+ levels inferred with the ion balance and aerosol pH predicted by the thermodynamic models and ammonia-ammonium (NH3-NH4+) partitioning. Similarly, no relationship is observed between the cation / anion molar ratio and predicted aerosol pH. Using only measured aerosol chemical composition as inputs without any constraint for the gas phase, the Extended Aerosol Inorganics Model (E-AIM) and ISORROPIA-II thermodynamic equilibrium models tend to predict aerosol pH levels that are inconsistent with the observed NH3-NH4+ partitioning. The modeled pH values from both models run with gas + aerosol inputs agreed well with the aerosol pH predicted by the phase partitioning of ammonia. It appears that (1) thermodynamic models constrained by gas + aerosol measurements, and (2) the phase partitioning of ammonia provide the best available predictions of aerosol pH. Furthermore, neither the ion balance nor the molar ratio can be used as surrogates for aerosol pH, and published studies to date with conclusions based on such acidity proxies may need to be reevaluated. Given the

  14. A critical evaluation of proxy methods used to estimate the acidity of atmospheric particles

    NASA Astrophysics Data System (ADS)

    Hennigan, C. J.; Izumi, J.; Sullivan, A. P.; Weber, R. J.; Nenes, A.

    2015-03-01

    Given significant challenges with available measurements of aerosol acidity, proxy methods are frequently used to estimate the acidity of atmospheric particles. In this study, four of the most common aerosol acidity proxies are evaluated and compared: (1) the ion balance method, (2) the molar ratio method, (3) thermodynamic equilibrium models, and (4) the phase partitioning of ammonia. All methods are evaluated against predictions of thermodynamic models and against direct observations of aerosol-gas equilibrium partitioning acquired in Mexico City during the Megacity Initiative: Local and Global Research Objectives (MILAGRO) study. The ion balance and molar ratio methods assume that any deficit in inorganic cations relative to anions is due to the presence of H+ and that a higher H+ loading and lower cation / anion ratio both correspond to increasingly acidic particles (i.e., lower pH). Based on the MILAGRO measurements, no correlation is observed between H+ levels inferred with the ion balance and aerosol pH predicted by the thermodynamic models and NH3-NH4+ partitioning. Similarly, no relationship is observed between the cation / anion molar ratio and predicted aerosol pH. Using only measured aerosol chemical composition as inputs without any constraint for the gas phase, the E-AIM (Extended Aerosol Inorganics Model) and ISORROPIA-II thermodynamic equilibrium models tend to predict aerosol pH levels that are inconsistent with the observed NH3-NH4+ partitioning. The modeled pH values from both E-AIM and ISORROPIA-II run with gas + aerosol inputs agreed well with the aerosol pH predicted by the phase partitioning of ammonia. It appears that (1) thermodynamic models constrained by gas + aerosol measurements and (2) the phase partitioning of ammonia provide the best available predictions of aerosol pH. Furthermore, neither the ion balance nor the molar ratio can be used as surrogates for aerosol pH, and previously published studies with conclusions based

  15. Using the Coupled Biosphere-Atmosphere Model SiB3-RAMS to Evaluate Fossil Fuel Emissions Estimates

    NASA Astrophysics Data System (ADS)

    Corbin, K. D.; Denning, A. S.; Parazoo, N.; Schuh, A.; Baker, I.; Lu, L.

    2006-12-01

    Using atmospheric tracer transport models, inverse modelers can estimate the strengths and spatial distribution of carbon sources and sinks; however, fossil fuel CO2 emissions must be accurately estimated to isolate and quantify biospheric and oceanic fluxes. To help achieve unbiased estimates of carbon exchange, high-resolution fossil fuel emissions estimates (36 km spatial resolution at timescales of one hour) are being produced for the United States [Gurney, 2006]. The goal of this research is use the coupled biosphere-atmosphere model SiB-RAMS to evaluate these emissions estimates. We have coupled the latest version of the Simple Biosphere Model (SiB3) to the CSU Regional Atmospheric Modeling System (RAMS) and have developed the capability to calculate the respiration factor and initial soil moisture for each grid cell using offline SiB3. In addition, we have implemented the capability to set the initial CO2 field to concentrations from the Parameterized Chemical Transport Model (PCTM) and to nudge lateral boundary concentrations to PCTM mixing ratios, which have a three-hour time-step. Carbon monoxide production and oxidation will be simulated using prescribed fields of the hydroxyl radical and methane. To investigate fossil fuel emissions, SiB3-RAMS simulations across large urban airsheds will be evaluated against CO and CO2 observations.

  16. Atmospheric Nitrogen Trifluoride: Optimized emission estimates using 2-D and 3-D Chemical Transport Models from 1973-2008

    NASA Astrophysics Data System (ADS)

    Ivy, D. J.; Rigby, M. L.; Prinn, R. G.; Muhle, J.; Weiss, R. F.

    2009-12-01

    We present optimized annual global emissions from 1973-2008 of nitrogen trifluoride (NF3), a powerful greenhouse gas which is not currently regulated by the Kyoto Protocol. In the past few decades, NF3 production has dramatically increased due to its usage in the semiconductor industry. Emissions were estimated through the 'pulse-method' discrete Kalman filter using both a simple, flexible 2-D 12-box model used in the Advanced Global Atmospheric Gases Experiment (AGAGE) network and the Model for Ozone and Related Tracers (MOZART v4.5), a full 3-D atmospheric chemistry model. No official audited reports of industrial NF3 emissions are available, and with limited information on production, a priori emissions were estimated using both a bottom-up and top-down approach with two different spatial patterns based on semiconductor perfluorocarbon (PFC) emissions from the Emission Database for Global Atmospheric Research (EDGAR v3.2) and Semiconductor Industry Association sales information. Both spatial patterns used in the models gave consistent results, showing the robustness of the estimated global emissions. Differences between estimates using the 2-D and 3-D models can be attributed to transport rates and resolution differences. Additionally, new NF3 industry production and market information is presented. Emission estimates from both the 2-D and 3-D models suggest that either the assumed industry release rate of NF3 or industry production information is still underestimated.

  17. The impact of Mount Etna sulfur emissions on the atmospheric composition and aerosol properties in the central Mediterranean: A statistical analysis over the period 2000-2013 based on observations and Lagrangian modelling

    NASA Astrophysics Data System (ADS)

    Sellitto, Pasquale; Zanetel, Claudia; di Sarra, Alcide; Salerno, Giuseppe; Tapparo, Andrea; Meloni, Daniela; Pace, Giandomenico; Caltabiano, Tommaso; Briole, Pierre; Legras, Bernard

    2017-01-01

    The emission of gases and aerosols due to volcanic activity may impact significantly atmospheric composition, cloud occurrence and properties, and the regional and global climate. While the effects of strong explosive (stratospheric) eruptions are relatively well known, limited information on the impacts of small to moderate volcanic activities, including passive degassing, is available. In this paper, the downwind impact of Mount Etna's sulfur emissions on the central Mediterranean is investigated on a statistical basis over the period 2000-2013 using: (a) daily sulfur dioxide emission rates measured near crater at Mount Etna with ground-based ultraviolet spectrophotometers, (b) Lagrangian trajectories and simulated plume dispersion obtained with the FLEXPART (FLEXible PARTicle dispersion) model, and (c) long-term observations of column SO2 concentration and aerosol Ångström exponent α at Lampedusa (35.5° N, 12.6° E). This statistical analysis has allowed, for the first time, the characterization of decadal impact of Mount Etna's sulfur emissions on the sulfur dioxide and the aerosol microphysical/optical properties in the central Mediterranean. On average, statistically significant higher SO2 concentrations and smaller aerosol sizes are present when air masses from Mount Etna overpass Lampedusa. Despite being upwind of Lampedusa for only 5% of the time, Mount Etna is potentially responsible for up to 40% and 20% of the SO2 and α extreme values (exceedances of a fixed threshold), respectively, at this location. The most important factor determining this perturbation is the prevailing dynamics, while the magnitude of the SO2 emission rates from Mount Etna appears to be likely important only for relatively strong emissions. The observed perturbations to the aerosol size distribution are expected to produce a direct regional radiative effect in this area.

  18. Estimating the contribution of point sources to atmospheric metals using single-particle mass spectrometry

    NASA Astrophysics Data System (ADS)

    Snyder, David C.; Schauer, James J.; Gross, Deborah S.; Turner, Jay R.

    Single-particle mass spectra were collected using an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) during December of 2003 and February of 2004 at an industrially impacted location in East St. Louis, IL. Hourly integrated peak areas for twenty ions were evaluated for their suitability in representing metals/metalloids, particularly those reported in the US EPA Toxic Release Inventory (TRI). Of the initial twenty ions examined, six (Al, As, Cu, Hg, Ti, and V) were found to be unsuitable due to strong isobaric interferences with commonly observed organic fragments, and one (Be) was found to have no significant signal. The usability of three ions (Co, Cr, and Mn) was limited due to suspected isobaric interferences based on temporal comparisons with commonly observed organic fragments. The identity of the remaining ions (Sb, Ba, Cd, Ca, Fe, Ni, Pb, K, Se, and Zn) was substantiated by comparing their signals with the integrated hourly signals of one or more isotope ions. When compared with one-in-six day integrated elemental data as determined by X-ray fluorescence spectroscopy (XRF), the daily integrated ATOFMS signal for several metal ions revealed a semi-quantitative relationship between ATOFMS peak area and XRF concentrations, although in some cases comparison of these measurements were poor at low elemental concentrations/ion signals due to isobaric interferences. A method of estimating the impact of local point sources was developed using hourly integrated ATOFMS peak areas, and this method attributed as much as 85% of the concentration of individual metals observed at the study site to local point sources. Hourly surface wind data were used in conjunction with TRI facility emissions data to reveal likely point sources impacting metal concentrations at the study site and to illustrate the utility of using single-particle mass spectral data to characterize atmospheric metals and identify point sources.

  19. On the estimation of heating effects in the atmosphere because of seismic activities

    NASA Astrophysics Data System (ADS)

    Meister, Claudia-Veronika; Hoffmann, Dieter H. H.

    2014-05-01

    The dielectric model for waves in the Earth's ionosphere is further developed and applied to possible electro-magnetic phenomena in seismic regions. In doing so, in comparison to the well-known dielectric wave model by R.O. Dendy [Plasma dynamics, Oxford University Press, 1990] for homogeneous systems, the stratification of the atmosphere is taken into account. Moreover, within the frame of many-fluid magnetohydrodynamics also the momentum transfer between the charged and neutral particles is considered. Discussed are the excitation of Alfvén and magnetoacoustic waves, but also their variations by the neutral gas winds. Further, also other current driven waves like Farley-Buneman ones are studied. In the work, models of the altitudinal scales of the plasma parameters and the electromagnetic wave field are derived. In case of the electric wave field, a method is given to calculate the altitudinal scale based on the Poisson equation for the electric field and the magnetohydrodynamic description of the particles. Further, expressions are derived to estimate density, pressure, and temperatur changes in the E-layer because of the generation of the electromagnetic waves. Last not least, formulas are obtained to determine the dispersion and polarisation of the excited electromagnetic waves. These are applied to find quantitative results for the turbulent heating of the ionospheric E-layer. Concerning the calculation of the dispersion relation, in comparison to a former work by Meister et al. [Contr. Plasma Phys. 53 (4-5), 406-413, 2013], where a numerical double-iteration method was suggested to obtain results for the wave dispersion relations, now further analytical calculations are performed. In doing so, different polynomial dependencies of the wave frequencies from the wave vectors are treated. This helped to restrict the numerical calculations to only one iteration process.

  20. Position and volume estimation of atmospheric nuclear detonations from video reconstruction

    NASA Astrophysics Data System (ADS)

    Schmitt, Daniel T.

    Recent work in digitizing films of foundational atmospheric nuclear detonations from the 1950s provides an opportunity to perform deeper analysis on these historical tests. This work leverages multi-view geometry and computer vision techniques to provide an automated means to perform three-dimensional analysis of the blasts for several points in time. The accomplishment of this requires careful alignment of the films in time, detection of features in the images, matching of features, and multi-view reconstruction. Sub-explosion features can be detected with a 67% hit rate and 22% false alarm rate. Hotspot features can be detected with a 71.95% hit rate, 86.03% precision and a 0.015% false positive rate. Detected hotspots are matched across 57-109 degree viewpoints with 76.63% average correct matching by defining their location relative to the center of the explosion, rotating them to the alternative viewpoint, and matching them collectively. When 3D reconstruction is applied to the hotspot matching it completes an automated process that has been used to create 168 3D point clouds with 31.6 points per reconstruction with each point having an accuracy of 0.62 meters with 0.35, 0.24, and 0.34 meters of accuracy in the x-, y- and z-direction respectively. As a demonstration of using the point clouds for analysis, volumes are estimated and shown to be consistent with radius-based models and in some cases improve on the level of uncertainty in the yield calculation.

  1. Investigation of Atmospheric Modelling Framework for Better Reconstruction on Historical Extreme Precipitation Event in PMP Estimation

    NASA Astrophysics Data System (ADS)

    Chen, X.; Hossain, F.; Leung, L. R.

    2015-12-01

    During May 1-2, 2010, a record-breaking storm hit Nashville, and caused huge humanity and societal loss. It raises the importance of forecasting/reconstructing these types of extreme weather systems once again, in the meanwhile providing an excellent case for such atmospheric modelling studies. However, earlier studies suggest that successful reconstruction of this event depends on and is sensitive to a number of model options, making it difficult to establish a better model framework with more confidence. In this study we employed the Weather Research and Forecast (WRF) model to investigate how this extreme precipitation event is sensitive to the model configuration, and identified options that would produce better results. We tested several combinations of modelling grid sizes together with initial/boundary conditions (IC/BC). At different grid sizes, we conducted a set of tests on various combinations of microphysics (Morrison, new Thompson and WSM5) and cumulus process (Kain-Fristch, Grell-Devenyi and Grell-Freitas) parameterization schemes. The model results were intensively evaluated under bias analysis as well as other metrics (probability of detection, bias, false alerts, HSS, ETS). The evaluation suggests that in general, simulation results benefit from finer model grids (5km). At 5km level, NCEP2 or NAM IC/BCs are more representative for the 2010 Nashville storm. There are no universally good parameterization schemes, but the WSM5 microphysics scheme, Kain-Fristch and Grell-Freitas cumulus schemes are recommended over other tested schemes. These better schemes would help to make better estimation of PMP in the region.

  2. Use of Atmospheric Budget to Reduce Uncertainty in Estimated Water Availability over South Asia from Different Reanalyses.

    PubMed

    Sebastian, Dawn Emil; Pathak, Amey; Ghosh, Subimal

    2016-07-08

    Disagreements across different reanalyses over South Asia result into uncertainty in assessment of water availability, which is computed as the difference between Precipitation and Evapotranspiration (P-E). Here, we compute P-E directly from atmospheric budget with divergence of moisture flux for different reanalyses and find improved correlation with observed values of P-E, acquired from station and satellite data. We also find reduced closure terms for water cycle computed with atmospheric budget, analysed over South Asian landmass, when compared to that obtained with individual values of P and E. The P-E value derived with atmospheric budget is more consistent with energy budget, when we use top-of-atmosphere radiation for the same. For analysing water cycle, we use runoff from Global Land Data Assimilation System, and water storage from Gravity Recovery and Climate Experiment. We find improvements in agreements across different reanalyses, in terms of inter-annual cross correlation when atmospheric budget is used to estimate P-E and hence, emphasize to use the same for estimations of water availability in South Asia to reduce uncertainty. Our results on water availability with reduced uncertainty over highly populated monsoon driven South Asia will be useful for water management and agricultural decision making.

  3. Use of Atmospheric Budget to Reduce Uncertainty in Estimated Water Availability over South Asia from Different Reanalyses

    PubMed Central

    Sebastian, Dawn Emil; Pathak, Amey; Ghosh, Subimal

    2016-01-01

    Disagreements across different reanalyses over South Asia result into uncertainty in assessment of water availability, which is computed as the difference between Precipitation and Evapotranspiration (P–E). Here, we compute P–E directly from atmospheric budget with divergence of moisture flux for different reanalyses and find improved correlation with observed values of P–E, acquired from station and satellite data. We also find reduced closure terms for water cycle computed with atmospheric budget, analysed over South Asian landmass, when compared to that obtained with individual values of P and E. The P–E value derived with atmospheric budget is more consistent with energy budget, when we use top-of-atmosphere radiation for the same. For analysing water cycle, we use runoff from Global Land Data Assimilation System, and water storage from Gravity Recovery and Climate Experiment. We find improvements in agreements across different reanalyses, in terms of inter-annual cross correlation when atmospheric budget is used to estimate P–E and hence, emphasize to use the same for estimations of water availability in South Asia to reduce uncertainty. Our results on water availability with reduced uncertainty over highly populated monsoon driven South Asia will be useful for water management and agricultural decision making. PMID:27388837

  4. Atmospheric water vapor transport: Estimation of continental precipitation recycling and parameterization of a simple climate model. M.S. Thesis

    NASA Technical Reports Server (NTRS)

    Brubaker, Kaye L.; Entekhabi, Dara; Eagleson, Peter S.

    1991-01-01

    The advective transport of atmospheric water vapor and its role in global hydrology and the water balance of continental regions are discussed and explored. The data set consists of ten years of global wind and humidity observations interpolated onto a regular grid by objective analysis. Atmospheric water vapor fluxes across the boundaries of selected continental regions are displayed graphically. The water vapor flux data are used to investigate the sources of continental precipitation. The total amount of water that precipitates on large continental regions is supplied by two mechanisms: (1) advection from surrounding areas external to the region; and (2) evaporation and transpiration from the land surface recycling of precipitation over the continental area. The degree to which regional precipitation is supplied by recycled moisture is a potentially significant climate feedback mechanism and land surface-atmosphere interaction, which may contribute to the persistence and intensification of droughts. A simplified model of the atmospheric moisture over continents and simultaneous estimates of regional precipitation are employed to estimate, for several large continental regions, the fraction of precipitation that is locally derived. In a separate, but related, study estimates of ocean to land water vapor transport are used to parameterize an existing simple climate model, containing both land and ocean surfaces, that is intended to mimic the dynamics of continental climates.

  5. Revised estimates of atmospheric CO/sub 2/ variations based on the tree ring /sup 13/C record

    SciTech Connect

    Peng, T.H.; Freyer, H.D.

    1983-01-01

    The composite mean /sup 13/C record for the Northern Hemisphere was revised. The overall decrease of delta /sup 13/C from 1800 to 1980 was estimated to be about -1.5/sup 0///sub 00/, which is 0.5/sup 0///sub 00/ less than the previous estimate. Therefore, the contribution of /sup 13/C-depleted CO/sub 2/ to the atmosphere from the forest and soil source was reevaluated, using the modified box-diffusion ocean model and Freyer's revised /sup 13/C record. On the basis of the assumption that this revised tree ring /sup 13/C record represents changes in the /sup 13/C//sup 12/C ratio induced in atmospheric CO/sub 2/ due to deforestation and soil manipulation and combustion of fossil fuels, the following results are obtained: (1) the magnitude of the integrated CO/sub 2/ release from the terrestrial biosphere since 1800 is about 90% of that from fossil fuel; (2) over the two-decade period covered by the Mauna Loa atmospheric CO/sub 2/ record, the input from the forest plus soil source is about 15% of that from fossil fuels; (3) the /sup 13/C//sup 12/C trend over the last two decades has been dominated by the input of fossil fuel CO/sub 2/; and (4) the pre-1850 atmospheric CO/sub 2/ content is estimated to be about 266 x 10/sup -6/ atm. 15 references, 5 figures, 1 table.

  6. Decadal emission estimates of carbon dioxide, sulfur dioxide, and nitric oxide emissions from coal burning in electric power generation plants in India.

    PubMed

    Mittal, Moti L; Sharma, Chhemendra; Singh, Richa

    2014-10-01

    This study aims to estimate the emissions of carbon dioxide (CO₂), sulfur dioxide (SO₂), and nitric oxide (NO) for coal combustion in thermal power plants in India using plant-specific emission factors during the period of 2001/02 to 2009/10. The mass emission factors have been theoretically calculated using the basic principles of combustion under representative prevailing operating conditions in the plants and fuel composition. The results show that from 2001/02 to 2009/10 period, total CO₂ emissions have increased from 324 to 499 Mt/year; SO₂ emissions have increased from 2,519 to 3,840 kt/year; and NO emissions have increased from 948 to 1,539 kt/year from the Indian coal-fired power plants. National average emissions per unit of electricity from the power plants do not show a noticeable improvement during this period. Emission efficiencies for new plants that use improved technology are found to be better than those of old plants. As per these estimates, the national average of CO₂ emissions per unit of electricity varies between 0.91 and 0.95 kg/kWh while SO₂ and NO emissions vary in the range of 6.9 to 7.3 and 2.8 to 2.9 g/kWh, respectively. Yamunagar plant in Haryana state showed the highest emission efficiencies with CO₂ emissions as 0.58 kg/kWh, SO₂ emissions as 3.87 g/kWh, and NO emissions as 1.78 g/kWh, while the Faridabad plant has the lowest emission efficiencies with CO₂ emissions as 1.5 kg/kWh, SO₂ emissions as 10.56 g/kWh, and NO emissions as 4.85 g/kWh. Emission values at other plants vary between the values of these two plants.

  7. Evaluating the Impact of Vegetation Cover and Atmospheric Characteristics on the Estimation of Snow Water Equivalent from Spaceborne Microwave Radiometry

    NASA Technical Reports Server (NTRS)

    Choudhury, Bhaskar J.; Foster, James L.

    2010-01-01

    A radiative transfer model for estimating snow water equivalent (SWE, mm) from satellite-observed brightness temperature (K) at 19 and 37 GHz (respectively, T(sub B(sub, sat,19)) and T(sub B(sub, sat,37)) over partially forested area is presented, as an extension of a previously published model, by considering scattering of radiation within the canopy. For the specific case of dense vegetation covering fractional area f, the model can be written as, SWE = alpha{ A. delta (T(sub B(sub, sat)) + B - C. f}/(l f), where delta T(sub B(sub, sat)), is the difference of T(sub B(sub, sat,19)) and T(sub B(sub, sat,37)), alpha(mm/K) is the slope of SWE vs. brightness temperature difference at 19 and 37 GHz that would be obtained by ignoring the presence of atmosphere, delta(T(sub B)sub g)), for a homogeneous snow cover (which varies with grain size). The parameters A, B, and C, are determined primarily by atmospheric characteristics, and for a likely range of atmospheric conditions appear to be in the range of, respectively, 1.15-1.63, 0.69-2.84 K and 0.59-2.39 K. Ignoring atmospheric correction would introduce bias towards underestimation of SWE (and also, snow cover area and snow depth). Increasing cloud liquid water path (L) has the effect of increasing A, and ignoring this variation of A with L would have the impact of biasing the estimate of SWE (and snow extent). Such biasing is further exacerbated with increasing f, because of the appearance of term (l-f) in the denominator. The impact of ignoring the intercept parameters (B and C) would be noticeable at low values of SWE (appearing as a bias towards underestimation of SWE), which has been determined to be about 6 mm for average environmental conditions. The uncertainty in estimating SWE due to variations in the atmospheric characteristics is likely to be less than 15%, but could be up to 25% for non-vegetated snow-covered areas. Better estimates of SWE (and snow extent) would be obtained by adjusting the parameters of

  8. An Estimate of the Global Burden of Anthropogenic Ozone and Fine Particulate Matter on Premature Human Mortality Using Atmospheric Modeling

    PubMed Central

    Anenberg, Susan C.; Horowitz, Larry W.; Tong, Daniel Q.; West, J. Jason

    2010-01-01

    Background Ground-level concentrations of ozone (O3) and fine particulate matter [≤ 2.5 μm in aerodynamic diameter (PM2.5)] have increased since preindustrial times in urban and rural regions and are associated with cardiovascular and respiratory mortality. Objectives We estimated the global burden of mortality due to O3 and PM2.5 from anthropogenic emissions using global atmospheric chemical transport model simulations of preindustrial and present-day (2000) concentrations to derive exposure estimates. Methods Attributable mortalities were estimated using health impact functions based on long-term relative risk estimates for O3 and PM2.5 from the epidemiology literature. Using simulated concentrations rather than previous methods based on measurements allows the inclusion of rural areas where measurements are often unavailable and avoids making assumptions for background air pollution. Results Anthropogenic O3 was associated with an estimated 0.7 ± 0.3 million respiratory mortalities (6.3 ± 3.0 million years of life lost) annually. Anthropogenic PM2.5 was associated with 3.5 ± 0.9 million cardiopulmonary and 220,000 ± 80,000 lung cancer mortalities (30 ± 7.6 million years of life lost) annually. Mortality estimates were reduced approximately 30% when we assumed low-concentration thresholds of 33.3 ppb for O3 and 5.8 μg/m3 for PM2.5. These estimates were sensitive to concentration thresholds and concentration–mortality relationships, often by > 50%. Conclusions Anthropogenic O3 and PM2.5 contribute substantially to global premature mortality. PM2.5 mortality estimates are about 50% higher than previous measurement-based estimates based on common assumptions, mainly because of methodologic differences. Specifically, we included rural populations, suggesting higher estimates; however, the coarse resolution of the global atmospheric model may underestimate urban PM2.5 exposures. PMID:20382579

  9. An empirical model for estimating the atmospheric transmittance of upward infrared radiation at different altitudes

    NASA Astrophysics Data System (ADS)

    Dai, Qiumin; Fang, Xiande; Zhao, Yingjie; Xing, Daoming

    2016-12-01

    The upward infrared (IR) radiation is one of the most important factors that affect the thermal characteristics of light-than-air (LTA) vehicles. Therefore, it is necessary to propose an accurate model to evaluate the upward atmospheric transmittance. The upward IR atmospheric transmittances of 6 different atmospheric models at the altitude from sea level to 30 km are obtained from the MODTRAN atmospheric radiative transfer code. Based on the data, a new upward IR atmospheric transmittance correlation related to pressure and vertical water column is proposed by regression analysis. It has excellent prediction accuracy with the coefficient of determination of 0.928, the root mean square error of 0.028, and the mean absolute percentage error of 2.68% for the database. Based on the new correlation, the thermal characteristics of a stratospheric airship located in tropics in midsummer are numerical studied and discussed.

  10. Technical note: Evaluation of markers for estimating duodenal digesta flow and ruminal digestibility: Acid detergent fiber, sulfuric acid detergent lignin, and n-alkanes.

    PubMed

    Kozloski, G V; Stefanello, C M; Mesquita, F R; Alves, T P; Ribeiro Filho, H M N; Almeida, J G R; Moraes Genro, T C

    2014-03-01

    The amount of digesta flowing to the duodenum is a relevant measurement for the evaluation of nutrient supply to ruminants, which is usually estimated in animals fitted with a duodenal T-type cannula using internal or external markers. This study evaluated acid detergent fiber (ADF) compared with external (C32n-alkane) and internal [sulfuric acid lignin (ADL) and n-alkanes C31 and C33] markers for estimating duodenal flow and(or) ruminal digestibility of dry matter (DM) in cattle and sheep. In the first assay, 4 duodenally cannulated Holstein steers housed in metabolism cages, dosed with C32n-alkane, and fed Avena strigosa plus concentrate and increasing levels of tannin extract to reduce ruminal digestibility, were used in a Latin square design. The mobile-bag technique was used to measure the intestinal disappearance of ADL and ADF from forage (Avena strigosa, Pennisetum purpureum, Cynodon dactylon, and Medicago sativa) and concentrate (corn grain, soybean meal, and sunflower meal) samples that were previously incubated in the rumen of additional fistulated steer for 12, 24, 36, or 48 h. The ADF concentration in residues recovered in the feces was strongly related to the ADF concentration in residues at the duodenum (R(2)=0.93, standard deviation=30.0, n=901). This relationship showed a lower precision for ADL fraction (R(2)=0.88, standard deviation=12.6, n=590). In a second assay, duodenal flow and ruminal DM digestibility were calculated from the duodenal and fecal concentration of either marker. We observed a significant effect of marker type on ruminal DM digestibility values, and the effect of tannin treatments was observed only when ADF or ADL was used as the marker. The lowest residual error was obtained for ADF. Ruminal DM digestibility was, on average, higher for C31 and C(33)n-alkanes, and the use of dosed C(32)n-alkane resulted in a negative value. In the third assay, a data set of 235 individual observations was compiled from digestibility trials to

  11. Low-dimensional models for the estimation of anthropogenic CO2 emissions from atmospheric observations

    NASA Astrophysics Data System (ADS)

    van Bloemen Waanders, B.; Ray, J.; McKenna, S. A.; Yadav, V.; Michalak, A. M.

    2011-12-01

    The estimation of anthropogenic fossil fuel emissions using atmospheric observations of CO2 has recently attracted increasing interest due to its relevance to monitoring of CO2 mitigation treaties and programs. To date, techniques to perform large-scale inversions had primarily been developed within the context of understanding biospheric and oceanic fluxes. Such fluxes tend to vary relatively smoothly in space and time, making it possible to use multiGaussian models to parameterize and regularize such inversions, predicated on limited measurements of CO2 concentrations. However, the spatial distribution of anthropogenic emissions is non-stationary and multiscale, and therefore makes the use of multiGaussians models less suitable. Thus, a need exists to identify how anthropogenic emissions may be represented in a low-dimensional manner (i.e., with few parameters), for use in top-down estimation. Certain aspects of the spatial extent of anthropogenic emissions can be represented using easily measurable proxies such as nightlights, population density and GDP; in fact, fossil fuel inventories regularly use them to disaggregate regional emission budgets to finer spatial resolutions. However, such proxies can also be used to construct a priori models for anthropogenic emissions, which can then be updated, with data, through inverse modeling. In this presentation, we compare 3 low-dimensional parameterizations to characterize anthropogenic sources. The models are derived from images of nightlights over the continental USA, but adopt different arguments to achieve their dimensionality reduction. In the first model, we threshold nightlights and fit bivariate Gaussian kernels over clusters to represent emission sources; the emission field is modeled as a weighted sum of the kernels. The second approach models emissions as a weighted superposition of a filtered nightlight-distribution and a multiresolution defect, modeled with Haar wavelet. The nightlight-based methods

  12. Atmosphere-based nation-wide emission estimates of hydrofluorocarbons and hydrochlorofluorocarbons from the U.S

    NASA Astrophysics Data System (ADS)

    Hu, L.; Montzka, S. A.; Miller, J. B.; Andrews, A. E.; Miller, B. R.; Thoning, K. W.; Sweeney, C.; Chen, H.; Bruhwiler, L.; Masarie, K.; Miller, S. M.; Fischer, M. L.; Saikawa, E.; Elkins, J. W.; Tans, P. P.

    2013-12-01

    Limiting the warming influence induced by greenhouse gases (GHGs) ultimately requires reductions in emissions. To evaluate emission magnitudes and their changes over time, we recommend verifying self-reported emission inventories with independent, atmosphere-based, 'top-down' estimates. Hydrochlorofluorocarbons (HCFCs) and hydrofluorocarbons (HFCs) are potent GHGs with global warming potentials up to thousands of times larger than CO2 over a 100-year time horizon. Reductions in HCFC production and consumption were required by the Montreal Protocol in developed countries beginning in 2004. However, it is uncertain whether emissions of these gases are declining within the US because emissions are not linearly related to production or consumption due to the existence of substantial 'banks' (stores of in-use chemicals that have not yet escaped to the atmosphere). HFCs are replacements for CFCs and HCFCs. Without regulation, CO2 equivalent emissions of HFCs could become substantial in the future relative to CO2. In this study, we estimated emissions of HCFC-22 and HFC-134a within the US from 2008 - 2012 using a Bayesian approach of a regional inverse model with atmospheric observations from 8 tall-tower sites, 5 surface flask sites and 19 aircraft sites. We used a maximum likelihood estimation to estimate model-data mismatch errors, prior flux uncertainty, and temporal and spatial correlations in flux deviations between prior and posterior fluxes. We optimized our model design and tested our model performance by conducting synthetic data experiments. With this optimized design and boundary mixing ratios calculated with three different approaches, we derived national emissions of HCFC-22 and HFC-134a. This study provides the first multi-year atmosphere-based national emission estimates of HCFC-22 and HFC-134a, derived from multiple sites distributed across the US.

  13. Atmospheric OH reactivity in central London: observations, model predictions and estimates of in situ ozone production

    NASA Astrophysics Data System (ADS)

    Whalley, Lisa K.; Stone, Daniel; Bandy, Brian; Dunmore, Rachel; Hamilton, Jacqueline F.; Hopkins, James; Lee, James D.; Lewis, Alastair C.; Heard, Dwayne E.

    2016-02-01

    Near-continuous measurements of hydroxyl radical (OH) reactivity in the urban background atmosphere of central London during the summer of 2012 are presented. OH reactivity behaviour is seen to be broadly dependent on air mass origin, with the highest reactivity and the most pronounced diurnal profile observed when air had passed over central London to the east, prior to measurement. Averaged over the entire observation period of 26 days, OH reactivity peaked at ˜ 27 s-1 in the morning, with a minimum of ˜ 15 s-1 during the afternoon. A maximum OH reactivity of 116 s-1 was recorded on one day during morning rush hour. A detailed box model using the Master Chemical Mechanism was used to calculate OH reactivity, and was constrained with an extended measurement data set of volatile organic compounds (VOCs) derived from a gas chromatography flame ionisation detector (GC-FID) and a two-dimensional GC instrument which included heavier molecular weight (up to C12) aliphatic VOCs, oxygenated VOCs and the biogenic VOCs α-pinene and limonene. Comparison was made between observed OH reactivity and modelled OH reactivity using (i) a standard suite of VOC measurements (C2-C8 hydrocarbons and a small selection of oxygenated VOCs) and (ii) a more comprehensive inventory including species up to C12. Modelled reactivities were lower than those measured (by 33 %) when only the reactivity of the standard VOC suite was considered. The difference between measured and modelled reactivity was improved, to within 15 %, if the reactivity of the higher VOCs (⩾ C9) was also considered, with the reactivity of the biogenic compounds of α-pinene and limonene and their oxidation products almost entirely responsible for this improvement. Further improvements in the model's ability to reproduce OH reactivity (to within 6 %) could be achieved if the reactivity and degradation mechanism of unassigned two-dimensional GC peaks were estimated. Neglecting the contribution of the higher VOCs (⩾ C

  14. Atmospheric OH reactivity in central London: observations, model predictions and estimates of in situ ozone production

    NASA Astrophysics Data System (ADS)

    Whalley, L. K.; Stone, D.; Bandy, B.; Dunmore, R.; Hamilton, J. F.; Hopkins, J.; Lee, J. D.; Lewis, A. C.; Heard, D. E.

    2015-11-01

    Near-continuous measurements of OH reactivity in the urban background atmosphere of central London during the summer of 2012 are presented. OH reactivity behaviour is seen to be broadly dependent on airmass origin with the highest reactivity and the most pronounced diurnal profile observed when air had passed over central London to the East, prior to measurement. Averaged over the entire observation period of 26 days, OH reactivity peaked at ~ 27 s-1 in the morning with a minimum of ~ 15 s-1 during the afternoon. A maximum OH reactivity of 116 s-1 was recorded on one day during morning rush hour. A detailed box model using the Master Chemical Mechanism was used to calculate OH reactivity, and was constrained with an extended measurement dataset of volatile organic compounds (VOCs) derived from GC-FID and a two-dimensional GC instrument which included heavier molecular weight (up to C12) aliphatic VOCs, oxygenated VOCs and the biogenic VOCs of α pinene and limonene. Comparison was made between observed OH reactivity and modelled OH reactivity using (i) a standard suite of VOC measurements (C2-C8 hydrocarbons and a small selection of oxygenated VOCs) and (ii) a more comprehensive inventory including species up to C12. Modelled reactivities were lower than those measured (by 33 %) when only the reactivity of the standard VOC suite was considered. The difference between measured and modelled reactivity was improved, to within 15 %, if the reactivity of the higher VOCs (≥ C9) was also considered, with the reactivity of the biogenic compounds of α pinene and limonene and their oxidation products almost entirely responsible for this improvement. Further improvements in the model's ability to reproduce OH reactivity (to within 6 %) could be achieved if the reactivity and degradation mechanism of unassigned two-dimensional GC peaks were estimated. Neglecting the contribution of the higher VOCs (≥ C9) (particularly α pinene and limonene) and model

  15. Estimation of Footprints of Observation Sites Using NIES and FLEXPART Atmospheric Transport Models

    NASA Astrophysics Data System (ADS)

    Belikov, D.; Maksyutov, S. S.; Ganshin, A.; Zhuravlev, R.; Aoki, S.; Wunch, D.; Griffith, D. W. T.; Notholt, J.; Wennberg, P. O.

    2015-12-01

    The Total Carbon Column Observing Network (TCCON) is a network of ground-based Fourier Transform Spectrometers (FTS) that record near-infrared (NIR) spectra of the sun. From these spectra, accurate and precise column-averaged abundances of atmospheric constituents including CO2, CH4, H2O, and others are retrieved. Use of TCCON FTS observations is an appropriate way to validate satellite observations (SCIAMACHY, GOSAT, OCO-2). However, our knowledge about TCCON observations is limited. The retrievals from the ground based FTSs report column-averaged abundances, so the concentration distribution along the vertical profile as well as value and location of sources affecting the concentration are mainly unknown. Studying the footprint is especially important for sites located near regions with different emissions or sinks of GHG's, e.g. for coastal stations, where marine air masses are mixed with continental ones. In this work, we use the National Institute for Environmental Studies (NIES) Eulerian three-dimensional transport model (TM) and the FLEXPART Lagrangian plume diffusion model (LPDM) to determine footprints of operational and future TCCON FTS observational sites. The NIES model was previously used to study the seasonal and inter-annual variability of CO2 and CH4. In paper by Belikov at al. (ACP, 2013) we shows, that the NIES model is able to successfully reproduce the vertical profile of greenhouse gases (CO2, CH4, SF6) and the seasonal and inter-annual variability of XCO2 and XCH4. Using this fact, NIES TM CO2concentrations sampled at the level of 1 km above ground and at 13:00 of local time were used to initialize backward tracer simulation with FLEXPART model. The sampling time is selected to fit the overpass time of satellites measuring greenhouse gases and because the NIES TM is more successful at reproducing diurnal tracer variations. Based on the FLEXPART back-trajectory simulations, we estimate footprints of operational and future TCCON FTS sites. These

  16. PARMA: PHITS-based Analytical Radiation Model in the Atmosphere--Verification of Its Accuracy in Estimating Cosmic Radiation Doses

    SciTech Connect

    Sato, Tatsuhiko; Satoh, Daiki; Endo, Akira; Yasuda, Hiroshi; Takada, Masashi; Nakamura, Takashi; Niita, Koji; Sihver, Lembit

    2008-08-07

    Estimation of cosmic-ray spectra in the atmosphere has been an essential issue in the evaluation of the aircrew doses. We therefore developed an analytical model that can predict the terrestrial neutron, proton, He nucleus, muon, electron, positron and photon spectra at altitudes below 20 km, based on the Monte Carlo simulation results of cosmic-ray propagation in the atmosphere performed by the PHITS code. The model was designated PARMA. In order to examine the accuracy of PARMA in terms of the neutron dose estimation, we measured the neutron dose rates at the altitudes between 20 to 10400 m, using our developed dose monitor DARWIN mounted on an aircraft. Excellent agreement was observed between the measured dose rates and the corresponding data calculated by PARMA coupled with the fluence-to-dose conversion coefficients, indicating the applicability of the model to be utilized in the route-dose calculation.

  17. Estimation of propagation losses for infrared laser beam in turbulent atmosphere

    NASA Astrophysics Data System (ADS)

    Zaponov, A. E.; Sakharov, M. V.

    2016-11-01

    In present work, the radiation propagation in atmosphere from laser source to the receiver is considered by taking into account deviations of optical beam due to turbulence. The photon flux density on the receiver has been evaluated.

  18. Method of estimating time scales of atmospheric piston and its application at Dome C (Antarctica)

    SciTech Connect

    Kellerer, A.; Sarazin, M.; Butterley, T.; Wilson, R

    2007-07-20

    Temporal fluctuations of the atmospheric piston are critical for interferometers as they determine their sensitivity. We characterize an instrumental setup,termed the piston scope, that aims at measuring the atmospheric time constant, {tau}0, through the image motion in the focal plane of a Fizeau interferometer.High-resolution piston scope measurements have been obtained at the observatory of Paranal, Chile in April 2006. The derived atmospheric parameters are shown to be consistent with data from the astronomical site monitor, provided that the atmospheric turbulence is displaced along a single direction.The piston scope measurements of lower temporal and spatial resolution were recorded for what is believed to be the first time in February 2005 at the Antarctic site of Dome C. Their reanalysis in terms of the new data calibration sharpens the conclusions of a first qualitative examination [Appl. Opt. 45, 5709 (2006)].

  19. Method of estimating time scales of atmospheric piston and its application at Dome C (Antarctica).

    PubMed

    Kellerer, A; Sarazin, M; Butterley, T; Wilson, R

    2007-07-20

    Temporal fluctuations of the atmospheric piston are critical for interferometers as they determine their sensitivity. We characterize an instrumental setup, termed the piston scope, that aims at measuring the atmospheric time constant, tau(0), through the image motion in the focal plane of a Fizeau interferometer. High-resolution piston scope measurements have been obtained at the observatory of Paranal, Chile in April 2006. The derived atmospheric parameters are shown to be consistent with data from the astronomical site monitor, provided that the atmospheric turbulence is displaced along a single direction. The piston scope measurements of lower temporal and spatial resolution were recorded for what is believed to be the first time in February 2005 at the Antarctic site of Dome C. Their reanalysis in terms of the new data calibration sharpens the conclusions of a first qualitative examination [Appl. Opt. 45, 5709 (2006)].

  20. ESTIMATING GASEOUS EXCHANGES BETWEEN THE ATMOSPHERE AND PLANTS USING A COUPLED BIOCHEMICAL DRY DEPOSITION MODEL

    EPA Science Inventory

    To study gaseous exchanges between the soil, biosphere and atmosphere, a biochemical model was coupled with the latest version of Meyers Multi-Layer Deposition Model. The biochemical model describes photosynthesis and respiration and their coupling with stomatal resistance for...

  1. Application of the Approximate Bayesian Computation methods in the stochastic estimation of atmospheric contamination parameters for mobile sources

    NASA Astrophysics Data System (ADS)

    Kopka, Piotr; Wawrzynczak, Anna; Borysiewicz, Mieczyslaw

    2016-11-01

    In this paper the Bayesian methodology, known as Approximate Bayesian Computation (ABC), is applied to the problem of the atmospheric contamination source identification. The algorithm input data are on-line arriving concentrations of the released substance registered by the distributed sensors network. This paper presents the Sequential ABC algorithm in detail and tests its efficiency in estimation of probabilistic distributions of atmospheric release parameters of a mobile contamination source. The developed algorithms are tested using the data from Over-Land Atmospheric Diffusion (OLAD) field tracer experiment. The paper demonstrates estimation of seven parameters characterizing the contamination source, i.e.: contamination source starting position (x,y), the direction of the motion of the source (d), its velocity (v), release rate (q), start time of release (ts) and its duration (td). The online-arriving new concentrations dynamically update the probability distributions of search parameters. The atmospheric dispersion Second-order Closure Integrated PUFF (SCIPUFF) Model is used as the forward model to predict the concentrations at the sensors locations.

  2. Comparison of Kalman filter estimates of zenith atmospheric path delays using the global positioning system and very long baseline interferometry

    NASA Astrophysics Data System (ADS)

    Tralli, David M.; Lichten, Stephen M.; Herring, Thomas A.

    1992-12-01

    Kalman filter estimates of zenith nondispersive atmospheric path delays at Westford, Massachusetts, Fort Davis, Texas, and Mojave, California, were obtained from independent analyses of data collected during January and February 1988 using the GPS and VLBI. The apparent accuracy of the path delays is inferred by examining the estimates and covariances from both sets of data. The ability of the geodetic data to resolve zenith path delay fluctuations is determined by comparing further the GPS Kalman filter estimates with corresponding wet path delays derived from water vapor radiometric data available at Mojave over two 8-hour data spans within the comparison period. GPS and VLBI zenith path delay estimates agree well within one standard deviation formal uncertainties (from 10-20 mm for GPS and 3-15 mm for VLBI) in four out of the five possible comparisons, with maximum differences of 5 and 21 mm over 8- to 12-hour data spans.

  3. Comparison of Kalman filter estimates of zenith atmospheric path delays using the global positioning system and very long baseline interferometry

    NASA Technical Reports Server (NTRS)

    Tralli, David M.; Lichten, Stephen M.; Herring, Thomas A.

    1992-01-01

    Kalman filter estimates of zenith nondispersive atmospheric path delays at Westford, Massachusetts, Fort Davis, Texas, and Mojave, California, were obtained from independent analyses of data collected during January and February 1988 using the GPS and VLBI. The apparent accuracy of the path delays is inferred by examining the estimates and covariances from both sets of data. The ability of the geodetic data to resolve zenith path delay fluctuations is determined by comparing further the GPS Kalman filter estimates with corresponding wet path delays derived from water vapor radiometric data available at Mojave over two 8-hour data spans within the comparison period. GPS and VLBI zenith path delay estimates agree well within one standard deviation formal uncertainties (from 10-20 mm for GPS and 3-15 mm for VLBI) in four out of the five possible comparisons, with maximum differences of 5 and 21 mm over 8- to 12-hour data spans.

  4. Estimation of the Atmospheric Refraction Effect in Airborne Images Using Radiosonde Data

    NASA Astrophysics Data System (ADS)

    Beisl, U.; Tempelmann, U.

    2016-06-01

    The influence of the atmospheric refraction on the geometric accuracy of airborne photogrammetric images was already considered in the days of analogue photography. The effect is a function of the varying refractive index on the path from the ground to the image sensor. Therefore the effect depends on the height over ground, the view zenith angle and the atmospheric constituents. It is leading to a gradual increase of the scale towards the borders of the image, i.e. a magnification takes place. Textbooks list a shift of several pixels at the borders of standard wide angle images. As it was the necessity of that time when images could only be acquired at good weather conditions, the effect was calculated using standard atmospheres for good atmospheric conditions, leading to simple empirical formulas. Often the pixel shift caused by refraction was approximated as linear with height and compensated by an adjustment of the focal length. With the advent of sensitive digital cameras, the image dynamics allows for capturing images at adverse weather conditions. So the influence of the atmospheric profiles on the geometric accuracy of the images has to be investigated and the validity of the standard correction formulas has to be checked. This paper compares the results from the standard formulas by Saastamoinen with the results calculated from a broad selection of atmospheres obtained from radiosonde profile data. The geometric deviation is calculated by numerical integration of the refractive index as a function of the height using the refractive index formula by Ciddor. It turns out that the effect of different atmospheric profiles (including inversion situations) is generally small compared to the overall effect except at low camera heights. But there the absolute deviation is small. Since the necessary atmospheric profile data are often not readily available for airborne images a formula proposed by Saastamoinen is verified that uses only camera height, the pressure

  5. Use of health effect risk estimates and uncertainty in formal regulatory proceedings: a case study involving atmospheric particulates

    SciTech Connect

    Habegger, L.J.; Oezkaynak, A.H.

    1984-01-01

    Coal combustion particulates are released to the atmosphere by power plants supplying electrical to the nuclear fuel cycle. This paper presents estimates of the public health risks associated with the release of these particulates at a rate associated with the annual nuclear fuel production requirements for a nuclear power plan. Utilization of these risk assessments as a new component in the formal evaluation of total risks from nuclear power plants is discussed. 23 references, 3 tables.

  6. The use of multispectral thermal infrared image data to estimate the sulfur dioxide flux from volcanoes: A case study from Mount Etna, Sicily, July 29, 1986

    SciTech Connect

    Realmuto, V.J.; Abrams, M.J.; Buongiorno, M.F.; Pieri, D.C. )

    1994-01-10

    The authors have found that image data acquired with NASA's airborne Thermal Infrared Multispectral Scanner (TIMS) can be used to make estimates of the SO[sub 2] content of volcanic plumes. TIMS image data are most applicable to the study of partially transparent SO[sub 2] plumes, such as those released during quiescent periods or nonexplosive eruptions. The estimation procedure is based on the LOWTRAN 7 radiative transfer code, which the authors use to model the radiance perceived by TIMS as it views the ground through an SO[sub 2] plume. The input to the procedure includes the altitudes of the aircraft and ground, the altitude and thickness of the SO[sub 2] plume, the emissivity of the ground, and altitude profiles of the atmospheric pressure, temperature, and relative humidity. They use the TIMS data to estimate both ground temperatures beneath a plume and SO[sub 2] concentrations within a plume. Applying this procedure to TIMS data acquired over Mount Etna, Sicily, on July 29, 1986, the authors estimate that the SO[sub 2] flux from the volcano was approximately 6700 t d[sup [minus]1]. The use of TIMS to study SO[sub 2] plumes represents a bridge between highly localized methods, such as correlation spectroscopy or direct sampling, and small-scale mapping techniques involving satellite instruments such as the Total Ozone Mapping Spectrometer or Microwave Limb Sounder. The authors require further airborne experiments to refine their estimation procedure. This refinement is a necessary preparation for the scheduled 1998 launch of the Advanced Spaceborne Thermal Emission and Reflectance Radiometer, which will allow large-scale multispectral thermal infrared image data to be collected over virtually any volcano on Earth at least once every 16 days.

  7. The use of multispectral thermal infrared image data to estimate the sulfur dioxide flux from volcanoes: A case study from Mount Etna, Sicily, July 29, 1986

    NASA Technical Reports Server (NTRS)

    Realmuto, Vincent J.; Abrams, Michael J.; Buongiorno, M. Fabrizia; Pieri, David C.

    1994-01-01

    We have found that image data acquired with NASA's airborne Thermal Infrared Multispectral Scanner (TIMS) can be used to make estimates of the SO2 content of volcanic plumes. TIMS image data are most applicable to the study of partially transparent SO2 plumes, such as those released during quiescent periods or nonexplosive eruptions. The estimation procedure is based on the LOWTRAN 7 radiative transfer code, which we use to model the radiance perceived by TIMS as it views the ground through an SO2 plume. The input to the procedure includes the altitudes of the aircraft and ground, the altitude and thickness of the SO2 plume, the emissivity of the ground, and altitude profiles of the atmospheric pressure, temperature, and relative humidity. We use the TIMS data to estimate both ground temperatures beneath a plume and SO2 concentrations within a plume. Applying our procedure to TIMS data acquired over Mount Etna, Sicily, on July 29, 1986, we estimate that the SO2 flux from the volcano was approximately 6700 t d(exp -1). The use of TIMS to study SO2 plumes represents a bridge between highly localized methods, such as correlation spectroscopy or direct sampling, and small-scale mapping techniques involving satellite instruments such as the Total Ozone Mapping Spectrometer or Microwave Limb Sounder. We require further airborne experiments to refine our estimation procedure. This refinement is a necessary preparation for the schedueled 1998 launch of the Advanced Spaceborne Thermal Emission and Reflectance Radiometer, which will allow large-scale multispectral thermal infrared image data to be collected over virtually any volcano on Earth at least once every 16 days.

  8. Low palaeopressure of the martian atmosphere estimated from the size distribution of ancient craters

    NASA Astrophysics Data System (ADS)

    Kite, Edwin S.; Williams, Jean-Pierre; Lucas, Antoine; Aharonson, Oded

    2014-05-01

    The decay of the martian atmosphere--which is dominated by carbon dioxide--is a component of the long-term environmental change on Mars from a climate that once allowed rivers to flow to the cold and dry conditions of today. The minimum size of craters serves as a proxy for palaeopressure of planetary atmospheres, because thinner atmospheres permit smaller objects to reach the surface at high velocities and form craters. The Aeolis Dorsa region near Gale crater on Mars contains a high density of preserved ancient craters interbedded with river deposits and thus can provide constraints on atmospheric density at the time of fluvial activity. Here we use high-resolution images and digital terrain models from the Mars Reconnaissance Orbiter to identify ancient craters in deposits in Aeolis Dorsa that date to about 3.6 Gyr ago and compare their size distribution with models of atmospheric filtering of impactors. We obtain an upper limit of 0.9 +/- 0.1 bar for the martian atmospheric palaeopressure, rising to 1.9 +/- 0.2 bar if rimmed circular mesas--interpreted to be erosionally-resistant fills or floors of impact craters--are excluded. We assume target properties appropriate for desert alluvium: if sediment had rock-mass strength similar to bedrock at the time of impact, the paleopressure upper limit increases by a factor of up to two. If Mars did not have a stable multibar atmosphere at the time that the rivers were flowing--as suggested by our results--then a warm and wet CO2/H2O greenhouse is ruled out, and long-term average temperatures were most likely below freezing.

  9. TRENDS IN RURAL SULFUR CONCENTRATIONS

    EPA Science Inventory

    This paper presents an analysis of regional trends in atmospheric concentrations in sulfur dioxide (502) and particulate sulfate (50~- ) at rural monitoring sites in the Clean Air Act Status and Trends Monitoring Network (CAsTNet) from 1990 to 1999. A two-stage approach is used t...

  10. Estimation of the Ocean Skin Temperature using the NASA GEOS Atmospheric Data Assimilation System

    NASA Technical Reports Server (NTRS)

    Koster, Randal D.; Akella, Santha; Todling, Ricardo; Suarez, Max

    2016-01-01

    This report documents the status of the development of a sea surface temperature (SST) analysis for the Goddard Earth Observing System (GEOS) Version-5 atmospheric data assimilation system (ADAS). Its implementation is part of the steps being taken toward the development of an integrated earth system analysis. Currently, GEOS-ADAS SST is a bulk ocean temperature (from ocean boundary conditions), and is almost identical to the skin sea surface temperature. Here we describe changes to the atmosphere-ocean interface layer of the GEOS-atmospheric general circulation model (AGCM) to include near surface diurnal warming and cool-skin effects. We also added SST relevant Advanced Very High Resolution Radiometer (AVHRR) observations to the GEOS-ADAS observing system. We provide a detailed description of our analysis of these observations, along with the modifications to the interface between the GEOS atmospheric general circulation model, gridpoint statistical interpolation-based atmospheric analysis and the community radiative transfer model. Our experiments (with and without these changes) show improved assimilation of satellite radiance observations. We obtained a closer fit to withheld, in-situ buoys measuring near-surface SST. Evaluation of forecast skill scores corroborate improvements seen in the observation fits. Along with a discussion of our results, we also include directions for future work.

  11. Active microbial sulfur disproportionation in the Mesoproterozoic.

    PubMed

    Johnston, David T; Wing, Boswell A; Farquhar, James; Kaufman, Alan J; Strauss, Harald; Lyons, Timothy W; Kah, Linda C; Canfield, Donald E

    2005-12-02

    The environmental expression of sulfur compound disproportionation has been placed between 640 and 1050 million years ago (Ma) and linked to increases in atmospheric oxygen. These arguments have their basis in temporal changes in the magnitude of 34S/32S fractionations between sulfate and sulfide. Here, we present a Proterozoic seawater sulfate isotope record that includes the less abundant sulfur isotope 33S. These measurements imply that sulfur compound disproportionation was an active part of the sulfur cycle by 1300 Ma and that progressive Earth surface oxygenation may have characterized the Mesoproterozoic.

  12. Regional characteristics of dry deposition of sulfur and nitrogen compounds at EANET sites in Japan from 2003 to 2008

    NASA Astrophysics Data System (ADS)

    Endo, Tomomi; Yagoh, Hiroaki; Sato, Keiichi; Matsuda, Kazuhide; Hayashi, Kentaro; Noguchi, Izumi; Sawada, Kiyoshi

    2011-02-01

    The regional characteristics of estimated dry deposition and total atmospheric deposition, including dry and wet deposition, at 10 EANET sites in Japan from April 2003 to March 2008 are discussed. The components examined for dry deposition were sulfur compounds (SO 2 and particulate SO 42-) and nitrogen compounds (HNO 3, NH 3, particulate NO 3-, and NH 4+). Dry deposition was calculated by the product of the deposition velocity estimated by the inferential method for forest and grass surfaces and the air concentration of each compound. The 5-year mean annual dry deposition amounts for sulfur and nitrogen compounds were in the range of 5-37 and 7-50 mmol m -2 year -1, respectively. The regional characteristics of dry deposition amounts were similar between sulfur and nitrogen compounds, which showed higher deposition in the Sea of Japan side and in the Western Japan. The 5-year mean annual total deposition amounts for sulfur and nitrogen compounds were in the range of 28-77 and 22-130 mmol m -2 year -1, respectively. The contribution of dry deposition to the total deposition amounts was 10-55% and 13-56% for sulfur and nitrogen compounds, respectively. The regional characteristic of total deposition was different between sulfur and nitrogen compounds. Total deposition amounts in Japan were larger than those in CASTNET and EMEP because of high wet deposition, which implied that the increasing emissions of air pollutants in East Asia caused high atmospheric depositions.

  13. A differential absorption technique to estimate atmospheric total water vapor amounts

    NASA Technical Reports Server (NTRS)

    Frouin, Robert; Middleton, Elizabeth

    1990-01-01

    Vertically integrated water-vapor amounts can be remotely determined by measuring the solar radiance reflected by the earth's surface with satellites or aircraft-based instruments. The technique is based on the method by Fowle (1912, 1913) and utilizes the 0.940-micron water-vapor band to retrieve total-water-vapor data that is independent of surface reflectance properties and other atmospheric constituents. A channel combination is proposed to provide more accurate results, the SE-590 spectrometer is used to verify the data, and the effects of atmospheric photon backscattering is examined. The spectrometer and radiosonde data confirm the accuracy of using a narrow and a wide channel centered on the same wavelength to determine water vapor amounts. The technique is suitable for cloudless conditions and can contribute to atmospheric corrections of land-surface parameters.

  14. Development of a model of atmospheric oxygen variations to estimate terrestrial carbon storage and release

    NASA Technical Reports Server (NTRS)

    Najjar, Raymond G.; Keeling, Ralph F.; Erickson, David J., III

    1995-01-01

    Two years of work has been completed towards the development of a model of atmospheric oxygen variations on seasonal to decadal timescales. During the first year we (1) constructed a preliminary monthly-mean climatology of surface ocean oxygen anomalies, (2) began modeling studies to assess the importance of short term variability on the monthly-mean oxygen flux, and (3) conducted preliminary simulations of the annual mean cycle of oxygen in the atmosphere. Most of the second year was devoted to improving the monthly mean climatology of oxygen in the surface ocean.

  15. Estimation of the production, consumption, and atmospheric emissions of pentabrominated diphenyl ether in Europe between 1970 and 2000.

    PubMed

    Prevedouros, K; Jones, K C; Sweetman, A J

    2004-06-15

    A European consumption and atmospheric emissions inventory for pentabrominated diphenyl ethers (PeBDEs) is derived for the period 1970-2000. This time frame has seen a rise in the widespread usage of PeBDE, followed by more recent restrictions/bans. It is estimated that a total of 3000-5000 t of PeBDEs was produced in Europe during this period, with a further 9000-10,000 t imported in finished articles. The main uses for PeBDE are to flame retard consumer products as well as in packaging and solid elastomers. Their major stocks are predicted to be in polyurethane (flexible) foams with up to 30% in cars; more than 10% in furniture foam; and the rest in textiles, building material, packaging, and solid applications. Release of PeBDEs from treated products into environmental media are estimated with a focus on atmospheric inputs via volatilization from their use in cars, upholstered furniture, textiles, television sets, personal computers, and other recycled material. Different emission factors are used to derive different emission scenarios. A peak in atmospheric emissions of between 22 and 31 t of BDE-47 is estimated to have occurred around 1997, with a decline of approximately 20% in 2000. Comparisons with long-term environmental monitoring data revealed that the time trends of human blood and milk concentrations follow similar patterns to the generated emissions, while sediment core levels increase more slowly, probably because they respond to a mix of atmospheric and catchment inputs. The emissions data derived here can be used in a spatially and temporally resolved form as input data for multi-media environmental fate modeling.

  16. Determination of uncertainty in the estimation of velocity and direction-of-arrival for atmospheric infrasound signals

    NASA Astrophysics Data System (ADS)

    Szuberla, Curt A. L.; Olson, John V.

    2002-11-01

    Upon the detection of an atmospheric infrasound signal, the problem of precisely estimating the signal's velocity (v) and direction-of-arrival (theta) arises. Multiple sources, multipath, medium anisotropies, and other propagation effects can all degrade precision; however, uncertainty in the estimates of v and theta is fundamentally governed by array geometry and the estimation of time delays across the array. Typically, as in the Comprehensive Test Ban Treaty Organzation Provisional Technical Secretariat (CTBTO/PTS) specification for data from infrasound stations, the Cramer-Rao lower bound is invoked to ascertain the uncertainties associated with v and theta. As this theoretical lower limit is often overly conservative, a more general, and useful, approach to calculate these uncertainties is developed. Examples of this uncertainty determination are presented for typical impulsive and continuous atmospheric infrasound signals received at arrays in Windless Bight, Antarctica and Fairbanks, Alaska. Since the determination of v and theta serves as primary input to any propogation model, it is critical that uncertainties in these estimates be addressed. As an extension of this work, an interactive graphical tool is constructed to assist in the analysis of performance bounds for arbitrary array geometries and signal characteristics.

  17. Combining Satellite Microwave Radiometer and Radar Observations to Estimate Atmospheric Latent Heating Profiles

    NASA Technical Reports Server (NTRS)

    Grecu, Mircea; Olson, William S.; Shie, Chung-Lin; L'Ecuyer, Tristan S.; Tao, Wei-Kuo

    2009-01-01

    In this study, satellite passive microwave sensor observations from the TRMM Microwave Imager (TMI) are utilized to make estimates of latent + eddy sensible heating rates (Q1-QR) in regions of precipitation. The TMI heating algorithm (TRAIN) is calibrated, or "trained" using relatively accurate estimates of heating based upon spaceborne Precipitation Radar (PR) observations collocated with the TMI observations over a one-month period. The heating estimation technique is based upon a previously described Bayesian methodology, but with improvements in supporting cloud-resolving model simulations, an adjustment of precipitation echo tops to compensate for model biases, and a separate scaling of convective and stratiform heating components that leads to an approximate balance between estimated vertically-integrated condensation and surface precipitation. Estimates of Q1-QR from TMI compare favorably with the PR training estimates and show only modest sensitivity to the cloud-resolving model simulations of heating used to construct the training data. Moreover, the net condensation in the corresponding annual mean satellite latent heating profile is within a few percent of the annual mean surface precipitation rate over the tropical and subtropical oceans where the algorithm is applied. Comparisons of Q1 produced by combining TMI Q1-QR with independently derived estimates of QR show reasonable agreement with rawinsonde-based analyses of Q1 from two field campaigns, although the satellite estimates exhibit heating profile structure with sharper and more intense heating peaks than the rawinsonde estimates. 2

  18. Estimates of radiative flux divergence in the atmosphere from satellite data

    NASA Technical Reports Server (NTRS)

    Smith, G. L.; Charlock, Thomas P.; Bess, T. D.; Gupta, Shashi; Rutan, David; Rose, Fred G.

    1990-01-01

    Several options for the inference of the atmospheric radiative flux divergence (ARD) on the basis of satellite data are discussed. Attention is given to the clear-sky case and the cloudy-sky case. LW ARD profiles for different climatological regimes are presented and the effect of cloud base height on LW ARD divergence at various heights is illustrated.

  19. Satellite estimates of shortwave surface radiation and atmospheric meteorology for the BOREAS experiment region

    NASA Technical Reports Server (NTRS)

    Moats, C. D.; Whitlock, C. H.; Lecroy, S. R.; Dipasquale, R. C.

    1994-01-01

    This report provides background data for the Boreal Ecosystem Atmosphere Study (BOREAS) sites, including daily, seasonal, interannual, and spatial variability of shortwave (SW) radiation at the Earth's surface. This background data, from the Version 1.1 SW data set, was provided by the Surface Radiation Budget (SRB) Climatology Project established by the World Climate Research Program (WCRP).

  20. SMOG-CHAMBER TOXICOLOGY BETTER ESTIMATES THE TRUE TOXIC POTENTIAL OF ATMOSPHERIC MIXTURES

    EPA Science Inventory

    The chemistry of hazardous air pollutants (HAPs) have been studied for many years, yet little is known about how these chemicals, once interacted with urban atmospheres, affect healthy and susceptible individuals. The toxic potential of these very reactive compounds once they int...

  1. Further evaluation of wetland emission estimates from the JULES land surface model using SCIAMACHY and GOSAT atmospheric column methane measurements

    NASA Astrophysics Data System (ADS)

    Hayman, Garry; Comyn-Platt, Edward; McNorton, Joey; Chipperfield, Martyn; Gedney, Nicola

    2016-04-01

    The atmospheric concentration of methane began rising again in 2007 after a period of near-zero growth [1,2], with the largest increases observed over polar northern latitudes and the Southern Hemisphere in 2007 and in the tropics since then. The observed inter-annual variability in atmospheric methane concentrations and the associated changes in growth rates have variously been attributed to changes in different methane sources and sinks [2,3]. Wetlands are generally accepted as being the largest, but least well quantified, single natural source of CH4, with global emission estimates ranging from 142-284 Tg yr-1 [3]. The modelling of wetlands and their associated emissions of CH4 has become the subject of much current interest [4]. We have previously used the HadGEM2 chemistry-climate model to evaluate the wetland emission estimates derived using the UK community land surface model (JULES, the Joint UK Land Earth Simulator) against atmospheric observations of methane, including SCIAMACHY total methane columns [5] up to 2007. We have undertaken a series of new HadGEM2 runs using new JULES emission estimates extended in time to the end of 2012, thereby allowing comparison with both SCIAMACHY and GOSAT atmospheric column methane measurements. We will describe the results of these runs and the implications for methane wetland emissions. References [1] Rigby, M., et al.: Renewed growth of atmospheric methane. Geophys. Res. Lett., 35, L22805, 2008; [2] Nisbet, E.G., et al.: Methane on the Rise-Again, Science 343, 493, 2014; [3] Kirschke, S., et al.,: Three decades of global methane sources and sinks, Nature Geosciences, 6, 813-823, 2013; [4] Melton, J. R., et al.: Present state of global wetland extent and wetland methane modelling: conclusions from a model inter-comparison project (WETCHIMP), Biogeosciences, 10, 753-788, 2013; [5] Hayman, G.D., et al.: Comparison of the HadGEM2 climate-chemistry model against in situ and SCIAMACHY atmospheric methane data, Atmos. Chem

  2. Estimating Atmospheric Fe Deposition to the Remote Ocean: the Problems Posed by Solubility Control

    NASA Astrophysics Data System (ADS)

    Measures, C. I.

    2001-12-01

    John Edmond's scientific career was dedicated to exploiting the tracer properties of chemical distributions in the ocean and using these to further our understanding of Earth and ocean processes. He realised that since chemical distributions result from geological, physical and biological processes, their interpretation is a powerful tool that can be used to explain many disparate elements of Earth sciences. In addition, the natural integrating power of chemical distributions over long time scales provides a unique opportunity to temporally average high frequency processes. The ability to apply these tools to current problems requires development and application of methodology that can be used over large temporal and spatial scales. John helped foster the development of real time trace element determinations at sea. A particularly good example of the results that this work has produced is using surface water trace element distributions to develop an understanding of the role that atmospheric deposition processes play in biogeochemical cycles. The partial dissolution of atmospheric dust in surface waters leaves a chemical wake that can be used to determine the magnitude and locus of atmospheric deposition events. In particular, dissolved aluminium concentrations in surface waters appear to be largely driven by atmospheric processes. Thus, modeling of the distribution of this element is being used to develop an understanding of atmospheric deposition processes in oceanic regions that are not suitable for direct sampling. When used in conjunction with surface water distributions of iron, the role of atmospheric deposition for this biologically important element can also be studied. However, the few existing data sets indicate that current models of iron deposition to the surface ocean, which simply apply a fixed fractional solubility of iron in dust, are unlikely to succeed, since the absolute solubility of iron limits the addition of this element to the surface ocean

  3. A comprehensive estimate for loss of atmospheric carbon tetrachloride (CCl4) to the ocean

    NASA Astrophysics Data System (ADS)

    Butler, James H.; Yvon-Lewis, Shari A.; Lobert, Jurgen M.; King, Daniel B.; Montzka, Stephen A.; Bullister, John L.; Koropalov, Valentin; Elkins, James W.; Hall, Bradley D.; Hu, Lei; Liu, Yina

    2016-09-01

    Extensive undersaturations of carbon tetrachloride (CCl4) in Pacific, Atlantic, and Southern Ocean surface waters indicate that atmospheric CCl4 is consumed in large amounts by the ocean. Observations made on 16 research cruises between 1987 and 2010, ranging in latitude from 60° N to 77° S, show that negative saturations extend over most of the surface ocean. Corrected for physical effects associated with radiative heat flux, mixing, and air injection, these anomalies were commonly on the order of -5 to -10 %, with no clear relationship to temperature, productivity, or other gross surface water characteristics other than being more negative in association with upwelling. The atmospheric flux required to sustain these undersaturations is 12.4 (9.4-15.4) Gg yr-1, a loss rate implying a partial atmospheric lifetime with respect to the oceanic loss of 183 (147-241) yr and that ˜ 18 (14-22) % of atmospheric CCl4 is lost to the ocean. Although CCl4 hydrolyzes in seawater, published hydrolysis rates for this gas are too slow to support such large undersaturations, given our current understanding of air-sea gas exchange rates. The even larger undersaturations in intermediate depth waters associated with reduced oxygen levels, observed in this study and by other investigators, strongly suggest that CCl4 is ubiquitously consumed at mid-depth, presumably by microbiota. Although this subsurface sink creates a gradient that drives a downward flux of CCl4, the gradient alone is not sufficient to explain the observed surface undersaturations. Since known chemical losses are likewise insufficient to sustain the observed undersaturations, this suggests a possible biological sink for CCl4 in surface or near-surface waters of the ocean. The total atmospheric lifetime for CCl4, based on these results and the most recent studies of soil uptake and loss in the stratosphere is now 32 (26-43) yr.

  4. The estimation of 550 km x 550 km mean gravity anomalies. [from free atmosphere gravimetry data

    NASA Technical Reports Server (NTRS)

    Williamson, M. R.; Gaposchkin, E. M.

    1975-01-01

    The calculation of 550 km X 550 km mean gravity anomalies from 1 degree X 1 degree mean free-air gravimetry data is discussed. The block estimate procedure developed by Kaula was used, and estimates for 1452 of the 1654 blocks were obtained.

  5. Parameter estimation of atmospheric refractivity from radar clutter using the particle swarm optimization via Lévy flight

    NASA Astrophysics Data System (ADS)

    Zhang, Zhi-Hua; Sheng, Zheng; Shi, Han-Qing

    2015-01-01

    Estimating refractivity profiles from radar sea clutter is a complex nonlinear optimization problem. To deal with the ill-posed difficulties, an inversion algorithm, particle swarm optimization with a Lévy flight (LPSO), was proposed to be applied in the refractivity from clutter (RFC) technique to retrieve atmospheric duct in this paper. PSO has many advantages in solving continuous optimization problems, while in its late period it has slow convergence speed and low precision. Therefore, we integrate the Lévy flights into the standard PSO algorithm to improve the precision and enhance the capability of jumping out of the local optima. To verify the feasibility and validation of the LPSO for estimating atmospheric duct parameters based on the RFC method, the synthetic and Wallops98 experimental data are implemented. Numerical experiments demonstrate that the optimal solutions obtained from the hybrid algorithm are more precise and efficient. Additionally, to test the algorithm inversion performance, the antinoise ability of LPSO is analyzed. The results indicate that the LPSO algorithm has a certain antinoise ability. Finally, according to the experiment results, it can be concluded that the LPSO algorithm can provide a more precise and efficient method for near-real-time inversion of atmospheric refractivity from radar clutter.

  6. Advanced Sulfur Control Processing

    SciTech Connect

    Gangwal, S.K.; Portzer, J.W.; Turk, B.S.; Gupta, R.

    1996-12-31

    The primary objective of this project is to determine the feasibility of an alternate concept for the regeneration of high temperature desulfurization sorbents in which elemental sulfur, instead of SO{sub 2}, is produced. If successful, this concept will eliminate or alleviate problems caused by the highly exothermic nature of the regeneration reaction, the tendency for metal sulfate formation, and the need to treat the regeneration off-gas to prevent atmospheric SO{sub 2}, emissions. Iron and cerium-based sorbents were chosen on the basis of thermodynamic analysis to determine the feasibility of elemental sulfur production. The ability of both to remove H{sub 2}S during the sulfidation phase is less than that of zinc-based sorbents, and a two-stage desulfurization process will likely be required. Preliminary experimental work used electrobalance reactors to compare the relative rates of reaction of O{sub 2} and H{sub 2}O with FeS. More detailed studies of the regeneration of FeS as well as the sulfidation of CeO{sub 2} and regeneration of Ce{sub 2}O{sub 2}S are being carried out in a laboratory-scale fixed-bed reactor equipped with a unique analytical system which permits semi-continuous analysis of the distribution of elemental sulfur, H{sub 2}S, and SO{sub 2} in the reaction product gas.

  7. Mass-independent sulfur of inclusions in diamond and sulfur recycling on early Earth.

    PubMed

    Farquhar, J; Wing, B A; McKeegan, K D; Harris, J W; Cartigny, P; Thiemens, M H

    2002-12-20

    Populations of sulfide inclusions in diamonds from the Orapa kimberlite pipe in the Kaapvaal-Zimbabwe craton, Botswana, preserve mass-independent sulfur isotope fractionations. The data indicate that material was transferred from the atmosphere to the mantle in the Archean. The data also imply that sulfur is not well mixed in the diamond source regions, allowing for reconstruction of the Archean sulfur cycle and possibly offering insight into the nature of mantle convection through time.

  8. Detailed source term estimation of atmospheric release during the Fukushima Dai-ichi nuclear power plant accident by coupling atmospheric and oceanic dispersion models

    NASA Astrophysics Data System (ADS)

    Katata, Genki; Chino, Masamichi; Terada, Hiroaki; Kobayashi, Takuya; Ota, Masakazu; Nagai, Haruyasu; Kajino, Mizuo

    2014-05-01

    Temporal variations of release amounts of radionuclides during the Fukushima Dai-ichi Nuclear Power Plant (FNPP1) accident and their dispersion process are essential to evaluate the environmental impacts and resultant radiological doses to the public. Here, we estimated a detailed time trend of atmospheric releases during the accident by combining environmental monitoring data and coupling atmospheric and oceanic dispersion simulations by WSPEEDI-II (Worldwide version of System for Prediction of Environmental Emergency Dose Information) and SEA-GEARN developed by the authors. New schemes for wet, dry, and fog depositions of radioactive iodine gas (I2 and CH3I) and other particles (I-131, Te-132, Cs-137, and Cs-134) were incorporated into WSPEEDI-II. The deposition calculated by WSPEEDI-II was used as input data of ocean dispersion calculations by SEA-GEARN. The reverse estimation method based on the simulation by both models assuming unit release rate (1 Bq h-1) was adopted to estimate the source term at the FNPP1 using air dose rate, and air sea surface concentrations. The results suggested that the major release of radionuclides from the FNPP1 occurred in the following periods during March 2011: afternoon on the 12th when the venting and hydrogen explosion occurred at Unit 1, morning on the 13th after the venting event at Unit 3, midnight on the 14th when several openings of SRV (steam relief valve) were conducted at Unit 2, morning and night on the 15th, and morning on the 16th. The modified WSPEEDI-II using the newly estimated source term well reproduced local and regional patterns of air dose rate and surface deposition of I-131 and Cs-137 obtained by airborne observations. Our dispersion simulations also revealed that the highest radioactive contamination areas around FNPP1 were created from 15th to 16th March by complicated interactions among rainfall (wet deposition), plume movements, and phase properties (gas or particle) of I-131 and release rates

  9. Improving Wind Predictions in the Marine Atmospheric Boundary Layer through Parameter Estimation in a Single-Column Model

    SciTech Connect

    Lee, Jared A.; Hacker, Joshua P.; Delle Monache, Luca; Kosović, Branko; Clifton, Andrew; Vandenberghe, Francois; Rodrigo, Javier Sanz

    2016-12-14

    A current barrier to greater deployment of offshore wind turbines is the poor quality of numerical weather prediction model wind and turbulence forecasts over open ocean. The bulk of development for atmospheric boundary layer (ABL) parameterization schemes has focused on land, partly due to a scarcity of observations over ocean. The 100-m FINO1 tower in the North Sea is one of the few sources worldwide of atmospheric profile observations from the sea surface to turbine hub height. These observations are crucial to developing a better understanding and modeling of physical processes in the marine ABL. In this study, we use the WRF single column model (SCM), coupled with an ensemble Kalman filter from the Data Assimilation Research Testbed (DART), to create 100-member ensembles at the FINO1 location. The goal of this study is to determine the extent to which model parameter estimation can improve offshore wind forecasts.

  10. Estimating the effectiveness of using atmospheric deaerators for decarbonizing makeup water

    NASA Astrophysics Data System (ADS)

    Larin, B. M.; Larin, A. B.

    2015-02-01

    According to the water coolant quality standards, the makeup water supplied to a thermal power plant's (TPP) steam-generating systems must not have any content of free carbonic acid. As a rule, free and partially bound carbonic acid is removed from makeup water supplied to the power-generating boilers at TPPs in atmospheric deaerators. Their performance as decarbonizers can be evaluated by measuring the pH values of water supplied to the deaerator and of the deaerated water. A procedure for calculating the residual concentration of carbonic acid in deaerated water and the decarbonization effect from the change in the pH value (ΔpH) is presented together with an example of calculation carried out by specialists of the Ivanovo State Power Engineering University based on a long-term industrial experiment performed on DSA-300 atmospheric deaerators.

  11. Estimation of synoptic fields of middle atmosphere parameters from Nimbus-7 LIMS profile data

    NASA Technical Reports Server (NTRS)

    Remsberg, Ellis E.; Haggard, Kenneth V.; Russell, James M., III

    1990-01-01

    The most widely used version of the Nimbus-7 middle atmosphere dataset is the set of high quality, daily, and zonal Fourier coefficients that resolve information out to six wavenumbers at 12 UTC. A Kalman filter algorithm was applied to the original profile data in order to generate those fields for the data archive or LAMAT product. The characteristics and implementation of the algorithm are described in some detail, along with examples of the output for each of the LIMS parameters.

  12. Improving Wind Predictions in the Marine Atmospheric Boundary Layer Through Parameter Estimation in a Single Column Model

    SciTech Connect

    Lee, Jared A.; Hacker, Joshua P.; Monache, Luca Delle; Kosovic, Branko; Clifton, Andrew; Vandenberghe, Francois; Rodrigo, Javier Sanz

    2016-08-03

    A current barrier to greater deployment of offshore wind turbines is the poor quality of numerical weather prediction model wind and turbulence forecasts over open ocean. The bulk of development for atmospheric boundary layer (ABL) parameterization schemes has focused on land, partly due to a scarcity of observations over ocean. The 100-m FINO1 tower in the North Sea is one of the few sources worldwide of atmospheric profile observations from the sea surface to turbine hub height. These observations are crucial to developing a better understanding and modeling of physical processes in the marine ABL. In this paper we use the WRF single column model (SCM), coupled with an ensemble Kalman filter from the Data Assimilation Research Testbed (DART), to create 100-member ensembles at the FINO1 location. The goal of this study is to determine the extent to which model parameter estimation can improve offshore wind forecasts. Combining two datasets that provide lateral forcing for the SCM and two methods for determining z0, the