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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. 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.

  4. 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

  5. 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.

  6. 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.

  7. Estimating Effects of Atmospheric Deposition and Peat Decomposition Processes on Mercury and Sulfur Accumulation and Retention in Northern Peatlands, Minnesota

    NASA Astrophysics Data System (ADS)

    Furman, O.; Nater, E.; Toner, B. M.; Sebestyen, S. D.; Tfaily, M. M.; Chanton, J.; Kolka, R. K.

    2013-12-01

    Northern peatland ecosystems play an important role in mercury (Hg) and sulfur (S) co-cycling. Peatlands are sinks for total Hg and sources for methyl Hg through the activity of sulfate-reducing bacteria. These ecosystems are vulnerable to environmental change, and projected changes in climate for the north-central U.S. have the potential to affect Hg and S stores and cycling in the subsurface, which may stimulate the release of bioaccumulative methyl Hg to receiving water bodies. SPRUCE (Spruce and Peatland Responses under Climate and Environmental change experiment) is an interdisciplinary study of the effects of temperature and enriched carbon dioxide on the responses of northern peatland ecosystems at the Marcell Experimental Forest, Minnesota. In the first year of SPRUCE, we are investigating Hg and S accumulation rates in 12-m diameter experimental plots on a black spruce bog before peatland heating experiments start in 2014. Understanding Hg and S accumulation rates and their retention mechanisms in the subsurface are needed in order to reconstruct historical trends in Hg and S deposition, and predict peatland responses to climate change. In this study, we will attempt to separate the effects of atmospheric deposition vs peat humification on Hg and S retention. As such, peat cores were sampled from sixteen experimental SPRUCE plots in August 2012. These 'Time 0' peat subsamples have been analyzed for total Hg, methyl Hg and total S, and bulk density as a function of depth (<2 m). In addition, peat subsamples have been analyzed for 14C and 13C to determine the age of peat and derive peat, Hg and S accumulation rates. Our preliminary results indicate that both total and methyl Hg, and total S concentrations reached the peak value in the 20-40 cm peat section, which is the transition zone between transiently oxidized acrotelm and permanently saturated anaerobic catotelm. Total and methyl Hg concentrations were several times lower in deeper profiles (>50 cm

  8. SOLID SORBENT FOR COLLECTING ATMOSPHERIC SULFUR DIOXIDE

    EPA Science Inventory

    A solid sorbent for collecting atmospheric SO2 was evaluated as part of an overall effort to develop a replacement method for the West-Gaeke method presently used to measure 24-hour ambient sulfur dioxide concentrations in ambient air. Research showed that a solid sorbent, consis...

  9. Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling

    NASA Astrophysics Data System (ADS)

    Eckhardt, S.; Prata, A. J.; Seibert, P.; Stebel, K.; Stohl, A.

    2008-07-01

    An analytical inversion method has been developed to estimate the vertical profile of SO2 emissions from volcanic eruptions. The method uses satellite-observed total SO2 columns and an atmospheric transport model (FLEXPART) to exploit the fact that winds change with altitude thus, the position and shape of the volcanic plume bear information on its emission altitude. The method finds the vertical emission distribution which minimizes the total difference between simulated and observed SO2 columns while also considering a priori information. We have tested the method with the eruption of Jebel at Tair, Yemen, on 30 September 2007 for which a comprehensive observational data set from various satellite instruments (AIRS, OMI, SEVIRI, CALIPSO) is available. Using satellite data from the first 24 h after the eruption for the inversion, we found an emission maximum near 16 km above sea level (a.s.l.), and secondary maxima near 5, 9, 12 and 14 km a.s.l. 60% of the emission occurred above the tropopause. The emission profile obtained in the inversion was then used to simulate the transport of the plume over the following week. The modeled plume agrees very well with SO2 total columns observed by OMI, and its altitude agrees with CALIPSO aerosol observations to within 1 2 km. The inversion result is robust against various changes in both the a priori and the observations. Even when using only SEVIRI data from the first 15 h after the eruption, the emission profile was reasonably well estimated. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic ash for air traffic. It could also be helpful for assessing the sulfur input into the stratosphere, be it in the context of volcanic processes or also for proposed geo-engineering techniques to counteract global warming.

  10. Estimation of the vertical profile of sulfur dioxide injection into the atmosphere by a volcanic eruption using satellite column measurements and inverse transport modeling

    NASA Astrophysics Data System (ADS)

    Eckhardt, S.; Prata, A. J.; Seibert, P.; Stebel, K.; Stohl, A.

    2008-02-01

    An analytical inversion method has been developed to estimate the vertical profile of SO2 emissions from volcanic eruptions. The method uses satellite-observed total SO2 columns and an atmospheric transport model (FLEXPART) to exploit the fact that winds change with altitude - thus, the position and shape of the volcanic plume bear information on its emission altitude. The method finds the vertical emission distribution which minimizes the total difference between simulated and observed SO2 columns while also considering a priori information. We have tested the method with the eruption of Jebel at Tair on 30 September 2007 for which a comprehensive observational data set from various satellite instruments (AIRS, OMI, SEVIRI, CALIPSO) is available. Using satellite data from the first 24 h after the eruption for the inversion, we found an emission maximum near 16 km above sea level (asl), and secondary maxima near 5, 9, 12 and 14 km a.s.l. 60% of the emission occurred above the tropopause. The emission profile obtained in the inversion was then used to simulate the transport of the plume over the following week. The modeled plume agrees very well with SO2 total columns observed by OMI, and its altitude and width agree mostly within 1-2 km with CALIPSO observations of stratospheric aerosol produced from the SO2. The inversion result is robust against various changes in both the a priori and the observations. Even when using only SEVIRI data from the first 15 h after the eruption, the emission profile was reasonably well estimated. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic ash for air traffic. It could also be helpful for assessing the sulfur input into the stratosphere, be it in the context of volcanic processes or also for proposed geo-engineering techniques to counteract global warming.

  11. TOTAL SULFUR DEPOSITION (WET+DRY) FROM THE ATMOSPHERE

    EPA Science Inventory

    Sulfur Dioxide (SO2) is emitted primarily as a by-product of coal combustion from power plants. Sulfur Dioxide reacts in the atmosphere to form other chemical such as Sulfuric Acid and Amonium Sulfate. These compounds and their secondarily formed constituents deposit to the sur...

  12. 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.

  13. A sensitive method for measuring atmospheric concentrations of sulfur dioxide

    NASA Technical Reports Server (NTRS)

    Klemm, O.; Talbot, R. W.

    1991-01-01

    A new method for measuring tropospheric sulfur dioxide concentrations is proposed which is based on the mist chamber sampling method. At the present stage of development, the detection limit of the method is approximately 20 parts per trillion for a 45-min sampling time, with lower concentrations detectable with lower precision. The overall reproducibility of the method (+/-95 percent confidence intervals) is estimated at +/-10 percent. The technique is relatively simple, inexpensive, and lightweight, making it ideally suited for numerous field applications in atmospheric chemistry and biogeochemical studies from both ground-based and airborne platforms.

  14. 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.

  15. 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).

  16. Atmospheric deposition of nitrogen and sulfur in Louisiana

    NASA Astrophysics Data System (ADS)

    Zhang, H.; Guo, H.

    2015-12-01

    Wet deposition and dry deposition reduce their concentrations of sulfur and nitrogen contained air pollutants in atmosphere, but lead to increase of sulfur and nitrogen fluxes to the surface. Atmospheric deposition of sulfur and nitrogen can lead to acidification of surface water bodies (lakes, rivers, and coasts) and subsequent damage to aquatic ecosystems as well as damage to forests and vegetation. Louisiana has abundant water resources with approximately 11% of the total surface area composed of water bodies. It is important to protect water resources from excessive atmospheric deposition of sulfur and nitrogen. However, the information obtained from the observation systems for understanding the deposition of sulfur and nitrogen and the adverse effects in Louisiana is limited. This study uses a source-oriented CMAQ model to simulate emission, formation, transport, and deposition of sulfur and nitrogen species in Louisiana. WRF is used to generate the meteorological inputs and SMOKE is used to generate the emissions based on national emission inventory (NEI). The forms and quantities of sulfur and nitrogen deposition from wet and dry processes in Louisiana will be discovered. The spatial and temporal variations of sulfur and nitrogen fluxes will be quantified and contributions of major source sectors or source regions will be quantified.

  17. 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.

  18. 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.

  19. 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.

  20. Relations between sulfur and heavy elements in rural atmospheres

    NASA Astrophysics Data System (ADS)

    Navarre, J. L.; Priest, P.; Ronneau, C.

    Sulfur dioxide was used as an indicator of the occurrence of air pollution episodes in a rural area of Belgium. Provided air particulates sampling operations are strictly synchronized with SO 2 immission episodes, correlations appeared between the levels in air of sulfur and the levels of some toxic metals. Comparing the relative proportions of sulfur and metals in air with emission data for combustion sources in Belgium (coal especially) leads to the conclusion that combustion is probably the main source of toxic elements likely to contaminate rural atmospheres. On the other hand, it appears that industrial zone characterization is feasible by comparing the relative proportions of some specific metals in air.

  1. Atmospheric sulfur hexafluoride: Sources, sinks and greenhouse warming

    SciTech Connect

    Ko, M.K.W.; Sze, N.D.; Wang, W.C.

    1993-06-20

    Model calculations using estimated reaction rates of sulfur hexafluoride (SF{sub 6}) with OH and O({sup 1}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 SF{sub 6}. An estimate of the current production rate of SF{sub 6} is about 5 kt/yr. Based on historical emission rates, the authors calculated a present-day atmospheric concentrations for SF{sub 6} of about 2.5 parts per trillion by volume (pptv) and compared the results with available atmospheric measurements. 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 SF{sub 6} 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 SF{sub 6} in the lower stratosphere will help to narrow the uncertainty in the lifetime. Based on laboratory-measured IR absorption cross section for SF{sub 6}, the authors showed that SF{sub 6} 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. The authors estimated the future concentration of SF{sub 6} at 2010 to be 8 and 10 pptv based on two projected emission scenarios. The corresponding equilibrium warming of 0.0035{degrees}C is to be compared with the estimated warming due to CO{sub 2} increase of about 0.8{degrees}C in the same period. 45 refs., 8 figs., 5 tabs.

  2. BIOGENIC SULFUR COMPOUNDS IN COASTAL ATMOSPHERES OF NORTH CAROLINA

    EPA Science Inventory

    Atmospheric H2S, SO2, and particulate SO4(-2), Na(+), C1(-), NH4(-), and NO3(-) were measured in two experiments on the North Carolina coast to determine the levels of biogenic sulfur species at marsh and estuarine locations where dissimilatory bacterial sulfate reduction produce...

  3. ACCUMULATION OF ATMOSPHERIC SULFUR BY PLANTS AND SULFUR-SUPPLYING CAPACITY OF SOILS

    EPA Science Inventory

    The Tennessee Valley Authority conducted studies to measure the amount of sulfur (S) that is transferred from the atmosphere to agro-ecosystems and to determine the S-supplying capacity of soils in the Tennessee Valley. Three techniques were tested for determining the fractional ...

  4. Atmospheric sulfur and hydroxyl radical measurements at Palmer Station

    SciTech Connect

    Berresheim, H.; Eisele, F.L.; Tanner, D.J.

    1994-12-31

    The emission of dimethylsulfide (DMS) by marine algae represents the dominant natural contribution to reactive sulfur in the lower atmosphere. On a global scale, antarctic coastal waters are among the most productive oceanic regions and show extremely high DMS emission rates during austral summer. Following its release into the atmosphere, DMS is rapidly oxidized by the hydroxyl radical (OH), which itself is produced via photolysis of ozone and subsequent reaction of excited singlet oxygen [O({sup 1}D)] with water vapor. The most important stable products of the DMS+OH reaction are believed to be sulfur dioxide (SO{sub 2}), sulfuric acid (H{sub 2}SO{sub 4}), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), and dimethylsulfone (DMSO{sub 2}). Under atmospheric conditions, both H{sub 2}SO{sub 4} and MSA, due to their low vapor pressures, rapidly condense onto existing aerosol particles, thus contributing to the growth of these particles and their potential activation as cloud condensation nuclei. In addition, gas phase H{sub 2}SO{sub 4} (and, to a lesser extent, MSA) may also be responsible for new particle production via the poorly understood gas-to-particle conversion process. This potential for new particle formation is maximized (and can be most easily studied) in remote regions such as Antarctica where background levels of existing particles and rates of H{sub 2}SO{sub 4} loss onto particles are very low. In January and Bebruary 1994, project SCATE (Sulfur chemistry in the antarctic trophosphere experiment) was conducted at Palmer Station with the goal of obtaining a comprehensive database for modeling atmopsheric sulfur chemistry in high latitudes. 12 refs., 3 figs., 1 tab.

  5. 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

  6. Contribution of anthropogenic and natural sources to atmospheric sulfur in parts of the United States

    NASA Astrophysics Data System (ADS)

    Rice, Harbert; Nochumson, D. H.; Hidy, G. M.

    This paper presents an estimate of the contributions to atmospheric sulfur of natural vs anthropogenic processes in areas of the United States. The areas were selected on the basis of population density, industrialization and potential for different kinds of geographically unique natural emissions. The sulfur emissions were estimated in part from land use practice and from geochemical arguments relating sulfur to biological carbon cycling. The natural or quasi-natural processes considered include sulfur gas production in freshwater sediments and intertidal mudflats, soil processes and vegetation. Agricultural activities and acid mine drainage were also taken into account as a perturbation to the available natural sulfur resources. The emissions appear to be heavily influenced by contributions from sulfate reduction in freshwater sediments and intertidal mudflats, and acid mine drainage. The anthropogenic emissions were calculated from the U.S. Environmental Protection Agency's inventories in the late 1960s. The natural vs man-derived sulfur were compared for 2° longitude by 2° latitude sectors in New England, the mid-Atlantic States, the Atlantic Coastal South, the Midwest, and the arid Southwest. In the sample regions where the anthropogenic emissions exceed 50-100 × 10 3 tonne S y -1 over a 2 × 2° sector, or ≳ 15-30 kg(S) ha -1 y -1, they tend to dominate the biogenic emissions. This appears to be the case for industrialized Ohio, Illinois, and New England. If 10% of the available biogenic sulfur is released to the atmosphere, natural or quasi-natural emissions may be a significant contributor in air over Minnesota and Wisconsin, Florida, and perhaps the rural areas of Virginia and remote parts of Arizona and Utah.

  7. 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.

  8. The atmospheric sulfur cycle over the Amazon Basin. II - Wet season

    NASA Technical Reports Server (NTRS)

    Andreae, M. O.; Bingemer, H.; Berresheim, H.; Jacob, D. J.; Lewis, B. L.

    1990-01-01

    The fluxes and concentrations of atmospheric sulfur species were determined at ground level and from aircraft over the Amazon Basin during the 1987 wet season, providing a comprehensive description of the sulfur cycle over a remote tropical region. The vertical profile of dimethylsulfide (DMS) during the wet season was found to be very similar to that measured during the dry season, suggesting little seasonal variation in DMS fluxes. The concentrations of H2S were almost an order of magnitude higher than those of DMS, which makes H2S the most important biogenic source species in the atmosheric sulfur cycle over the Amazon Basin. Using the gradient-flux approach, the flux of DMS at the top of the tree canopy was estimated. The canopy was a source of DMS during the day, and a weak sink during the night. Measurements of sulfur gas emissions from soils, using the chamber method, showed very small fluxes, consistent with the hypothesis that the forest canopy is the major source of sulfur gases. The observed soil and canopy emission fluxes are similar to those measured in temperate regions. The concentrations of SO2 and sulfate aerosol in the wet season atmosphere were similar to dry season values.

  9. Sulfur speciation and bioaccumulation in camphor tree leaves as atmospheric sulfur indicator analyzed by synchrotron radiation XRF and XANES.

    PubMed

    Zeng, Jianrong; Zhang, Guilin; Bao, Liangman; Long, Shilei; Tan, Mingguang; Li, Yan; Ma, Chenyan; Zhao, Yidong

    2013-03-01

    Analyzing and understanding the effects of ambient pollution on plants is getting more and more attention as a topic of environmental biology. A method based on synchrotron radiation X-ray fluorescence and X-ray absorption near edge structure spectroscopy was established to analyze the sulfur concentration and speciation in mature camphor tree leaves (CTLs), which were sampled from 5 local fields in Shanghai, China. Annual SO2 concentration, SO4(2-) concentration in atmospheric particulate, SO4(2-) and sulfur concentration in soil were also analyzed to explore the relationship between ambient sulfur sources and the sulfur nutrient cycling in CTLs. Total sulfur concentration in mature camphor tree leaves was 766-1704 mg/kg. The mainly detected sulfur states and their corresponding compounds were +6 (sulfate, include inorganic sulfate and organic sulfate), +5.2 (sulfonate), +2.2 (suloxides), +0.6 (thiols and thiothers), +0.2 (organic sulfides). Total sulfur concentration was strongly correlated with sulfate proportion with a linear correlation coefficient up to 0.977, which suggested that sulfur accumulated in CTLs as sulfate form. Reduced sulfur compounds (organic sulfides, thiols, thioethers, sulfoxide and sulfonate) assimilation was sufficed to meet the nutrient requirement for growth at a balanced level around 526 mg/kg. The sulfate accumulation mainly caused by atmospheric sulfur pollution such as SO2 and airborne sulfate particulate instead of soil contamination. From urban to suburb place, sulfate in mature CTLs decreased as the atmospheric sulfur pollution reduced, but a dramatic increase presented near the seashore, where the marine sulfate emission and maritime activity pollution were significant. The sulfur concentration and speciation in mature CTLs effectively represented the long-term biological accumulation of atmospheric sulfur pollution in local environment. PMID:23923435

  10. The atmospheric sulfur cycle over the Amazon Basin. 2. Wet season

    SciTech Connect

    Andreae, M.O.; Berresheim, H.; Lewis, B.L.; Li, S. ); Jacob, D.J. ); Talbot, R.W. ); Bingemer, H.

    1990-09-20

    The authors determined the fluxes and concentrations of atmospheric sulfur species at ground level and from aircraft over the Amazon Basin during the 1987 wet season, providing a comprehensive description of the sulfur cycle over a remote tropical region. The vertical profile of dimethylsulfide (DMS) during the wet season was found to be very similar to that measured during the dry season. The concentrations of hydrogen sulfide (H{sub 2}S) were almost an order of magnitude higher than those of DMS, which makes H{sub 2}S the most important biogenic source species in the atmospheric sulfur cycle over the Amazon Basin. Using the gradient-flux approach, estimated the flux of DMS at the top of the tree canopy. The canopy was a source of DMS during the day, and a weak sink during the night. Measurements of sulfur gas emissions from soils, using the chamber method, showed very small fluxes, consistent with the hypothesis that the forest canopy is the major source of sulfur gases. The observed soil and canopy emission fluxes are similar to those measured in temperate regions. The concentrations of SO{sub 2} and sulfate aerosol in the wet season atmosphere were similar to dry season values. The sulfate concentration in rainwater, on the other hand, was lower by about a factor of 5 during the wet season. Due to the higher precipitation rate, however, the wet deposition flux of sulfate was not significantly different between the seasons. The measured fluxes and concentrations of DMS, H{sub 2}S, and SO{sub 2} were consistent with a model describing transport and chemistry of these sulfur species in the boundary layer. The concentrations of aerosol and the sulfate deposition rate, on the other hand, could only be explained by import of significant amounts of marine and anthropogenic sulfate aerosol into the Amazon Basin.

  11. 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.

  12. 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.

  13. 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.

  14. 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)

  15. Marine sulfur cycling and the atmospheric aerosol over the springtime North Atlantic.

    PubMed

    Andreae, M O; Andreae, T W; Meyerdierks, D; Thiel, C

    2003-09-01

    We investigated the distribution of phytoplankton species and the associated dimethyl sulfur species, dimethylsulfoniopropionate (DMSP) and dimethylsulfide (DMS) on a cruise into the spring bloom region of the northern North Atlantic (near 47 degrees N, 19 degrees W). The cruise was timed to characterize the relationship between plankton dynamics and sulfur species production during the spring plankton bloom period. At the same time, we measured the DMS concentrations in the atmospheric boundary layer and determined the abundance and composition of the atmospheric aerosol. The water column studies showed that the interplay of wind-driven mixing and stratification due to solar heating controlled the evolution of the plankton population, and consequently the abundance of particulate and dissolved DMSP and DMS. The sea-to-air transfer of DMS was modulated by strong variations in wind speed, and was found to be consistent with currently available transfer parameterizations. The atmospheric concentration of DMS was strongly dependent on the sea surface emission, the depth of the atmospheric boundary layer and the rate of photooxidation as inferred from UV irradiance. Sea-salt and anthropogenic sulfate were the most abundant components of the atmospheric aerosol. On two days, a strong dust episode was observed bringing mineral dust aerosol from the Sahara desert to our northerly study region. The background concentrations of marine biogenic sulfate aerosol were low, near 30-60 ppt. These values were consistent with the rate of sulfate production estimated from the abundance of DMS in the marine boundary layer. PMID:12852983

  16. Organic reactions increasing the absorption index of atmospheric sulfuric acid aerosols

    NASA Astrophysics Data System (ADS)

    Nozière, B.; Esteve, W.

    2005-02-01

    Unlike most environments present at Earth's surface atmospheric aerosols can be favorable to organic reactions. Among them, the acid-catalyzed aldol condensation of aldehydes and ketones produces light-absorbing compounds. In this work the increase of the absorption index of sulfuric acid solutions 50-96 wt. % resulting from the uptake of gas-phase acetaldehyde, acetone, and 2-butanone (methyl ethyl ketone), has been measured in the near UV and visible range. Our results indicate that the absorption index between 200 and 500 nm for stratospheric sulfuric aerosols exposed to 100 pptV of acetaldehyde (1 pptV = 10-12 v/v) would increase by four orders of magnitude over a two-year lifetime. Rough estimates based on previous radiative calculations suggest that this reaction could result in an increase of the radiative forcing of sulfate aerosols of the order of 0.01 W m-2, and that these processes are worth further investigation.

  17. 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).

  18. 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.

  19. 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.

  20. Estimating uncertainty in policy analysis: health effects from inhaled sulfur oxides

    SciTech Connect

    Amaral, D.A.L.

    1983-01-01

    This study presents methods for the incorporation of uncertainty into quanitative analysis of the problem of estimating health risks from coal-fired power plants. Probabilistic long-range models of sulfur material balance and sets of plume trajectories are combined to produce probabilistic estimates of population exposure to sulfur air pollution for the addition of a hypothetical coal-burning power plant in the Ohio River Valley. In another segment, the change in population exposure which might occur if ambient sulfate were to be reduced everywhere in the northeastern United States is calculated. A third case is made up of a set of hypothetical urban and rural scenarios representing typical northeastern situations. Models of health impacts obtained through the elicitation of subjective expert judgment are applied to each of these population exposure estimates. Seven leading experts in the field of sulfur air pollution and health participated, yielding five quantitative models for morbidity and/or mortality effects from human exposure to ambient sulfate. In each case analyzed, the predictions based on probability distributions provided by the experts spanned several orders of magnitude, including some predictions of zero effects and some of up to a few percent of the total morality. It is concluded that uncertainty about whether sulfate has adverse effects dominates the scientific uncertainty about the atmospheric processes which generate and transport this pollutant.

  1. 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.

  2. 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.

  3. Sulfur Mass-Independent Fractionation in Atmospheric Formation of Volcanic Sulfate

    NASA Astrophysics Data System (ADS)

    Lanciki, A.; Cole-Dai, J.; Thiemens, M. H.; Savarino, J. P.

    2009-12-01

    Volcanic eruptions emit sulfur dioxide which oxidizes to sulfuric acid aerosols in the atmosphere. Sulfate aerosols affect global climate by altering the atmospheric radiative properties. Sulfate aerosols from stratospheric eruptions can impact global climate, through their widespread distribution and relatively long atmospheric residence times (months to years). Ice cores volcanic sulfate records are often used to assess the volcanic contribution to climate change. However, sulfate signals of tropospheric eruptions in the ice core records make it difficult to evaluate the climatic impact of stratospheric eruptions in a glaciological record. But, the isotope composition of the volcanic sulfate can be used to distinguish between sulfate from stratospheric eruptions and that of tropospheric eruptions. Mass-independent fractionation (MIF) of sulfur isotopes in sulfate aerosols arises from the high-energy UV photo-oxidation of SO2, and this can be used to determine if a volcanic eruption is stratospheric, since high-energy UV is available only in the stratosphere. The stable isotopes of sulfur are compared to a standard (Canyon Diablo Triolite, FeS) in equation 1. The small delta (δ) represents the ratio of the isotope of interest to the most abundant isotope.

    δxS (‰) = [(xS/32S)sample/ [(xS/32S)std - 1] × 1000 (1)33S, calculated with the equation below. Any significant, non-zero Δ33S values indicate that the sulfate is formed via the UV-catalyzed oxidation of SO2 in the stratosphere.
    Δ33S = δ33S - 1000 × [(1 + δ34S/1000)0.515 - 1] (2)33S MIF values and have been deemed stratospheric events by this study. The 1259 AD eruption has the largest Δ33S values ever reported, beginning at +1.63 ‰ and ending with -1.49 ‰. Tambora, which has been estimated to be 2-3 times smaller in magnitude than the 1259 event, had measured Δ33S values of +0.25 ‰ to -0.28 ‰ along the timeframe of the eruption. Two of the measured events did not exhibit any

  4. 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.

  5. 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

  6. Global atmospheric sulfur budget under volcanically quiescent conditions: Aerosol-chemistry-climate model predictions and validation

    NASA Astrophysics Data System (ADS)

    Sheng, Jian-Xiong; Weisenstein, Debra K.; Luo, Bei-Ping; Rozanov, Eugene; Stenke, Andrea; Anet, Julien; Bingemer, Heinz; Peter, Thomas

    2015-01-01

    The global atmospheric sulfur budget and its emission dependence have been investigated using the coupled aerosol-chemistry-climate model SOCOL-AER. The aerosol module comprises gaseous and aqueous sulfur chemistry and comprehensive microphysics. The particle distribution is resolved by 40 size bins spanning radii from 0.39 nm to 3.2 μm, including size-dependent particle composition. Aerosol radiative properties required by the climate model are calculated online from the aerosol module. The model successfully reproduces main features of stratospheric aerosols under nonvolcanic conditions, including aerosol extinctions compared to Stratospheric Aerosol and Gas Experiment II (SAGE II) and Halogen Occultation Experiment, and size distributions compared to in situ measurements. The calculated stratospheric aerosol burden is 109 Gg of sulfur, matching the SAGE II-based estimate (112 Gg). In terms of fluxes through the tropopause, the stratospheric aerosol layer is due to about 43% primary tropospheric aerosol, 28% SO2, 23% carbonyl sulfide (OCS), 4% H2S, and 2% dimethyl sulfide (DMS). Turning off emissions of the short-lived species SO2, H2S, and DMS shows that OCS alone still establishes about 56% of the original stratospheric aerosol burden. Further sensitivity simulations reveal that anticipated increases in anthropogenic SO2 emissions in China and India have a larger influence on stratospheric aerosols than the same increase in Western Europe or the U.S., due to deep convection in the western Pacific region. However, even a doubling of Chinese and Indian emissions is predicted to increase the stratospheric background aerosol burden only by 9%. In contrast, small to moderate volcanic eruptions, such as that of Nabro in 2011, may easily double the stratospheric aerosol loading.

  7. Parameter Estimation in Atmospheric Data Sets

    NASA Technical Reports Server (NTRS)

    Wenig, Mark; Colarco, Peter

    2004-01-01

    In this study the structure tensor technique is used to estimate dynamical parameters in atmospheric data sets. The structure tensor is a common tool for estimating motion in image sequences. This technique can be extended to estimate other dynamical parameters such as diffusion constants or exponential decay rates. A general mathematical framework was developed for the direct estimation of the physical parameters that govern the underlying processes from image sequences. This estimation technique can be adapted to the specific physical problem under investigation, so it can be used in a variety of applications in trace gas, aerosol, and cloud remote sensing. As a test scenario this technique will be applied to modeled dust data. In this case vertically integrated dust concentrations were used to derive wind information. Those results can be compared to the wind vector fields which served as input to the model. Based on this analysis, a method to compute atmospheric data parameter fields will be presented. .

  8. 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.

  9. 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.

  10. 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

  11. 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.

  12. 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

  13. 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

  14. Relation of long- and short-term atmospheric sulfur concentrations to sulfate deposition in New York State

    USGS Publications Warehouse

    Barnes, C.R.

    1987-01-01

    Records from 1965-80 indicate an annual decrease of 1.9% in sulfur dioxide emissions upwind of New York, an annual decrease of 1.5% in atmospheric particulate sulfate concentration in New York, and an annual decrease of 2.0% in sulfate-deposition rate in New York. Sulfate-deposition rates in bulk sampling in New York during 1965-80 were approximately 40% of the average sulfur-emission rate for the Northeast. Sulfate-deposition rates in bulk and wetfall collectors were nearly equal and were five times greater than in the dryfall collector. Scavenging ratios for sulfate averaged 8.9 ?? 105; those for sulfate plus sulfur dioxide averaged 4.6 ?? 105. Sulfate concentrations in wet deposition averaged more than twice those estimated from published regional-scale washout equations, whereas those in dry deposition averaged only 22% of those computed from deposition velocities of 0.1 cm/s for sulfate and 1.0 cm/s for sulfur dioxide. Discrepancies in the dryfalls are attributed to inefficiency of dryfall-collection equipment. -from Author

  15. 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.

  16. 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. PMID:27128188

  17. OXYGEN ISOTOPES IN ATMOSPHERIC SULFATES, SULFUR DIOXIDE, AND WATER VAPORS FIELD MEASUREMENTS, JULY 1975

    EPA Science Inventory

    Oxygen isotope ratios were determined for atmospheric samples of sulfate aerosols, sulfur dioxide, and water vapor collected simultaneously during a six-day period in July, 1975, at St. Louis, MO; Auburn, IL; and Glasgow, IL. The collection sites were located about 100km apart. C...

  18. PROTON INDUCED GAMMA-RAY ANALYSIS OF ATMOSPHERIC AEROSOLS FOR CARBON, NITROGEN, AND SULFUR COMPOSITION

    EPA Science Inventory

    A technique for the simultaneous quantitative analysis of carbon, nitrogen, and sulfur using in-beam gamma-ray spectrometry has been developed for use with atmospheric aerosol samples. Samples are collected on quartz filters, and the aerosol composition is determined by analyzing...

  19. Biogeochemical context impacts seawater pH changes resulting from atmospheric sulfur and nitrogen deposition

    NASA Astrophysics Data System (ADS)

    Hagens, Mathilde; Hunter, Keith A.; Liss, Peter S.; Middelburg, Jack J.

    2014-02-01

    Seawater acidification can be induced both by absorption of atmospheric carbon dioxide (CO2) and by atmospheric deposition of sulfur and nitrogen oxides and ammonia. Their relative significance, interplay, and dependency on water column biogeochemistry are not well understood. Using a simple biogeochemical model we show that the initial conditions of coastal systems are not only relevant for CO2-induced acidification but also for additional acidification due to atmospheric acid deposition. Coastal areas undersaturated with respect to CO2 are most vulnerable to CO2-induced acidification but are relatively least affected by additional atmospheric deposition-induced acidification. In contrast, the pH of CO2-supersaturated systems is most sensitive to atmospheric deposition. The projected increment in atmospheric CO2 by 2100 will increase the sensitivity of coastal systems to atmospheric deposition-induced acidification by up to a factor 4, but the additional annual change in proton concentration is at most 28%.

  20. 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.

  1. Atmospheric dry deposition of sulfur and nitrogen in the Athabasca Oil Sands Region, Alberta, Canada.

    PubMed

    Hsu, Yu-Mei; Bytnerowicz, Andrzej; Fenn, Mark E; Percy, Kevin E

    2016-10-15

    Due to the potential ecological effects on terrestrial and aquatic ecosystems from atmospheric deposition in the Athabasca Oil Sands Region (AOSR), Alberta, Canada, this study was implemented to estimate atmospheric nitrogen (N) and sulfur (S) inputs. Passive samplers were used to measure ambient concentrations of ammonia (NH3), nitrogen dioxide (NO2), nitric acid/nitrous acid (HNO3/HONO), and sulfur dioxide (SO2) in the AOSR. Concentrations of NO2 and SO2 in winter were higher than those in summer, while seasonal differences of NH3 and HNO3/HONO showed an opposite trend, with higher values in summer. Concentrations of NH3, NO2 and SO2 were high close to the emission sources (oil sands operations and urban areas). NH3 concentrations were also elevated in the southern portion of the domain indicating possible agricultural and urban emission sources to the southwest. HNO3, an oxidation endpoint, showed wider ranges of concentrations and a larger spatial extent. Concentrations of NH3, NO2, HNO3/HONO and SO2 from passive measurements and their monthly deposition velocities calculated by a multi-layer inference model (MLM) were used to calculate dry deposition of N and S. NH3 contributed the largest fraction of deposited N across the network, ranging between 0.70-1.25kgNha(-1)yr(-1), HNO3/HONO deposition ranged between 0.30-0.90kgNha(-1)yr(-1), and NO2 deposition between 0.03-0.70kgNha(-1)yr(-1). During the modeled period, average dry deposition of the inorganic gaseous N species ranged between 1.03 and 2.85kgNha(-1)yr(-1) and SO4-S deposition ranged between 0.26 and 2.04kgha(-1)yr(-1). Comparisons with co-measured ion exchange resin throughfall data (8.51kgSha(-1)yr(-1)) indicate that modeled dry deposition combined with measured wet deposition (1.37kgSha(-1)yr(-1)) underestimated S deposition. Gas phase NH3 (71%) and HNO3 plus NO2 (79%) dry deposition fluxes dominated the total deposition of NH4-N and NO3-N, respectively. PMID:27295600

  2. Atmospheric corrections for TIMS estimated emittance

    NASA Technical Reports Server (NTRS)

    Warner, T. A.; Levandowski, D. W.

    1992-01-01

    The estimated temperature of the average of 500 lines of Thermal Infrared Multispectral Scanner (TIMS) data of the Pacific Ocean, from flight line 94, collected on 30 Sep. 1988, at 1931 GMT is shown. With no atmospheric corrections, estimated temperature decreases away from nadir (the center of the scan line). A LOWTRAN modeled correction, using local radiosonde data and instrument scan angle information, results in reversed limb darkening effects for most bands, and does not adequately correct all bands to the same temperature. The atmosphere tends to re-radiate energy at the wavelengths at which it most absorbs, and thus the overall difference between corrected and uncorrected temperatures is approximately 40 C, despite the average LOWTRAN calculated transmittance of only 60 percent between 8.1 and 11.6 microns. An alternative approach to atmospheric correction is a black body normalization. This is done by calculating a normalization factor for each pixel position and wavelength, which when applied results in a single calculated temperature, as would be expected for a gray body with near uniform emittance. The black body adjustment is based on the atmospheric conditions over the sea. The ground elevation profile along the remaining 3520 scan lines (approximately 10 km) of flight line 94, up the slopes of Kilauea, determined from aircraft pressure and laser altimeter data is shown. This flight line includes a large amount of vegetation that is clearly discernible on the radiance image, being much cooler than the surrounding rocks. For each of the 3520 scan lines, pixels were classified as vegetation or 'other'. A moving average of 51 lines was applied to the composite vegetation emittance for each scan line, to reduce noise. Assuming vegetation to be like water, and to act as gray body with an emittance of 0.986 across the spectrum, it is shown that that the LOWTRAN induced artifacts are severe, and other than for the 0.9.9 micron channel, not significantly

  3. Theoretical and modeling studies of the atmospheric chemistry of sulfur oxide and hydroxyl radical systems

    NASA Astrophysics Data System (ADS)

    El-Zanan, Hazem S.

    Models are the tools that integrate our understanding of the atmospheric processes. Box models are utilized frequently and used to simulate the fates and transformation of atmospheric pollutants. The results from models are usually used to produce one integrated system and further help the policy makers to develop control strategies. We have investigated the atmospheric chemistry of the SOx and HOx systems. The results of 15 laboratory experiments that involved the studies of the HO-SO2, reaction have been analyzed. Mixtures of HONO, NO, NO2, H2O, SO2 and CO were photolyzed in synthetic air or in nitrogen containing approximately 50 ppm oxygen. Upon analyzing the data we have found that a very large amount of the observed SO2 oxidation (70.0 +/- 9.1%) can not be explained through the gas phase reaction of HO + SO2 reaction alone. The Regional Atmospheric Chemistry Mechanism, Version 2 (RACM2) was used to investigate additional chemical pathways for the oxidation of SO2. The results indicate that a mechanism(s) involving photochemical heterogeneous reactions could account for the observed additional sulfur dioxide oxidation not accounted for by gas phase oxidation alone. We have also investigated the distribution of the hydroxyl radical in different urban and rural areas. Photolysis of ozone and its reactions with nitrogen oxides and organic compounds, including both anthropogenic and biogenic volatile organic compounds (VOCs), control the mixing ratios of the hydroxyl radical (HO). Measurements of ozone, nitrogen oxides and volatile hydrocarbons from a deciduous forest in July 1999 and six sites located in the San Joaquin Valley obtained during the Central California Ozone Study (CCOS) measured in July 2000 and September 2000 were used to estimate the hydroxyl radical concentrations. Two methods were employed to determine the concentrations: (1) box model simulations and (2) steady state approximation of the species concentrations (Production-Loss Method). The

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

    PubMed

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

    2014-08-19

    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 (Δ(33)S = +1.66‰ and Δ(36)S = +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 (Δ(36)S = -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

  5. 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

  6. 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.

  7. 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.

  8. 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.

  9. 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

  10. 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

  11. Stability of mechanical properties of vanadium catalysts for sulfuric acid manufacture in a humid atmosphere

    SciTech Connect

    Manaeva, L.N.; Malikman, V.I.; Dobkina, E.I.; Mukhlenov, I.P.

    1982-01-10

    Experience of the industrial use of catalysts in sulfuric acid manufacture shows that as the result of saturation with moisture the catalyst grains may lose strength and disintegrate during use. However, this question has not been examined experimentally and the mechanism of the effect has not been studied. Fresh catalyst may come into contact with atmospheric moisture during storage, and used catalyst as the result of uncontrolled leakages during stoppages and recharging of the catalytic converters. In the course of normal operation water vapor enters the catalytic converters together with sulfuric acid mist with the gas stream if the latter has not been adequately dried. The purpose of the present work was to study the mechanical stability, in a humid atmosphere, of industrial sulfuric acid catalysts: granulated SVD (5 mm in diameter) and SVS rings (8 x 8 x 2.5 mm). The catalysts were studied both in the fresh state and after use in a laboratory catalytic apparatus of the flow type.

  12. Assessment of the health effects of atmospheric sulfur oxides and particulate matter: evidence from observational studies.

    PubMed Central

    Ware, J H; Thibodeau, L A; Speizer, F E; Colome, S; Ferris, B G

    1981-01-01

    Steadily rising energy costs have increased the need for reliable information on the health effects of atmospheric sulfur oxides and particulate matter. Because ethical and practical considerations limit studies of this question under controlled conditions, observational studies provide an important part of the relevant information. This paper examines the currently available epidemiologic evidence from population studies of the health effects of these pollutants. Nonexperimental studies also have important limitations, including the inability to measure accurately the exposure burden of free living individuals, and the potential for serious confounding by other factors affecting health. We begin with a discussion of some of these methodologic issues. The evidence is then reviewed, first in association with fluctuations in 24 hr mean concentration of sulfur oxides and particulate matter, and then in association with differences in mean annual concentration. In the last section, this evidence is summarized and used to approximate the exposure-response relationship linking pollutant concentrations with mortality and morbidity levels. PMID:6977444

  13. 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).

  14. 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.

  15. 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

  16. A Sulfur-Based Survival Strategy for Putative Phototrophic Life in the Venusian Atmosphere

    NASA Astrophysics Data System (ADS)

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

    2004-03-01

    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 S8, 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.

  17. 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.

  18. 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.

  19. Sulfur Isotope Fractionation Due to SO2 Photolysis in the Atmosphere

    NASA Astrophysics Data System (ADS)

    Lyons, J. R.; Blackie, D.; Stark, G.; Pickering, J.

    2012-12-01

    The discovery of unusual (i.e. mass-independent) sulfur isotope fractionation (or MIF) in Archean and Paleoproterozoic sedimentary rocks has promised to yield insights into the rise of O2 and the nature of the sulfur cycle on ancient Earth [1], but interpretation has been hampered by the lack of a clear mechanism for the sulfur isotope signature. Proposed MIF mechanisms include SO2 photolysis [1-4], atmospheric S3 (thiozone) formation, and thermal sulfate reduction in sediments [5]. Studies focusing only on SO2 photolysis, including measurements of isotopic cross sections [6], have yielded results differing greatly from theory [4], and have resulted in improbable interpretations [7]. In addition to ancient rocks, there are sulfur isotope MIF signatures in polar ice core sulfates associated with massive Plinian eruptions over the past ~1000 years (e.g., [8]). The ice core MIF signatures differ significantly from the ancient Earth MIF signatures, suggesting a different source mechanism. SO2 photolysis can generate sulfur isotope MIF signatures in two ways: 1) self-shielding by an optically-thick column of SO2, and 2) isotope-dependent differences in absorption line intensities and widths, which are espcially important for optically-thin conditions. The MIF signatures in ice core sulfates appear to be consistent with self-shielding in an optically-thick plume, but the Archean MIF clearly is not. To address the optically-thin case, we've made high-resolution ultraviolet cross section measurements of the sulfur isotopologues of SO2 made with the UV FTS at Imperial College. We measured cross sections at 1 cm-1 spectral resolution for 32SO2, 33SO2, 34SO2 and for a 36SO2/34SO2 mixture. Incorporating these cross sections into a simple atmospheric photochemical model with a solar UV flux, we find sulfur MIF signatures for SO and S that.are consistent with the Archean pyrites. We also find that additional mass-dependent fractionation during self-shielding by 32SO2 places an

  20. 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. PMID:22243850

  1. Constraining CO emission estimates using atmospheric observations

    NASA Astrophysics Data System (ADS)

    Hooghiemstra, P. B.

    2012-06-01

    We apply a four-dimensional variational (4D-Var) data assimilation system to optimize carbon monoxide (CO) emissions and to reduce the uncertainty of emission estimates from individual sources using the chemistry transport model TM5. In the first study only a limited amount of surface network observations from the National Oceanic and Atmospheric Administration Earth System Research Laboratory (NOAA/ESRL) Global Monitoring Division (GMD) is used to test the 4D-Var system. Uncertainty reduction up to 60% in yearly emissions is observed over well-constrained regions and the inferred emissions compare well with recent studies for 2004. However, since the observations only constrain total CO emissions, the 4D-Var system has difficulties separating anthropogenic and biogenic sources in particular. The inferred emissions are validated with NOAA aircraft data over North America and the agreement is significantly improved from the prior to posterior simulation. Validation with the Measurements Of Pollution In The Troposphere (MOPITT) instrument shows a slight improved agreement over the well-constrained Northern Hemisphere and in the tropics (except for the African continent). However, the model simulation with posterior emissions underestimates MOPITT CO total columns on the remote Southern Hemisphere (SH) by about 10%. This is caused by a reduction in SH CO sources mainly due to surface stations on the high southern latitudes. In the second study, we compare two global inversions to estimate carbon monoxide (CO) emissions for 2004. Either surface flask observations from NOAA or CO total columns from the MOPITT instrument are assimilated in a 4D-Var framework. In the Southern Hemisphere (SH) three important findings are reported. First, due to their different vertical sensitivity, the stations-only inversion increases SH biomass burning emissions by 108 Tg CO/yr more than the MOPITT-only inversion. Conversely, the MOPITT-only inversion results in SH natural emissions

  2. 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.

  3. 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.

  4. 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.

  5. Abatement of sulfur hexafluoride emissions from the semiconductor manufacturing process by atmospheric-pressure plasmas.

    PubMed

    Lee, How Ming; Chang, Moo Been; Wu, Kuan Yu

    2004-08-01

    Sulfur hexafluoride (SF6) is an important gas for plasma etching processes in the semiconductor industry. SF6 intensely absorbs infrared radiation and, consequently, aggravates global warming. This study investigates SF6 abatement by nonthermal plasma technologies under atmospheric pressure. Two kinds of nonthermal plasma processes--dielectric barrier discharge (DBD) and combined plasma catalysis (CPC)--were employed and evaluated. Experimental results indicated that as much as 91% of SF6 was removed with DBDs at 20 kV of applied voltage and 150 Hz of discharge frequency for the gas stream containing 300 ppm SF6, 12% oxygen (O2), and 40% argon (Ar), with nitrogen (N2) as the carrier gas. Four additives, including Ar, O2, ethylene (C2H4), and H2O(g), are effective in enhancing SF6 abatement in the range of conditions studied. DBD achieves a higher SF6 removal efficiency than does CPC at the same operation condition. But CPC achieves a higher electrical energy utilization compared with DBD. However, poisoning of catalysts by sulfur (S)-containing species needs further investigation. SF6 is mainly converted to SOF2, SO2F4, sulfur dioxide (SO2), oxygen difluoride (OF2), and fluoride (F2). They do not cause global warming and can be captured by either wet scrubbing or adsorption. This study indicates that DBD and CPC are feasible control technologies for reducing SF6 emissions. PMID:15373364

  6. 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

  7. 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. PMID:24101502

  8. 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.

  9. Fractionation of sulfur isotopes during heterogeneous oxidation of SO2 in the atmosphere

    NASA Astrophysics Data System (ADS)

    Harris, E. J.; Sinha, B.; Hoppe, P.; Crowley, J.; Borrmann, S.; Foley, S. F.; Gnauk, T.; Van Pinxteren, D.; Herrmann, H.

    2011-12-01

    Sulfate and sulfur dioxide play an important role in environmental chemistry and climate, particularly through their effect on aerosols. Processing of aerosol through sulfate addition in clouds, which causes both hygroscopicity changes and mass increases, has been shown to modify the cloud condensation nucleus spectrum, leading to important climatological effects (Bower et al. 1997, Hegg et al. 2004). However, the uptake of sulfate and SO2 to aerosol in clouds is not well constrained, nor is it resolved for different particle types and sizes (Kasper-Giebl et al. 2000, Barrie et al. 2001). Measurements of stable sulfur isotopes can be used to investigate the chemistry of SO2 in the environment, providing insight into sources, sinks and oxidation pathways. Typical isotopic compositions for many sources have been measured, and the major current limitation is the lack of reliable fractionation factors - characteristic changes in isotopic composition caused by chemical reactions - with which to interpret the data. Laboratory values of fractionation factors for the major oxidation reactions have been measured in previous work, however there are no measurements or models to represent isotopic fractionation during heterogeneous oxidation on complex atmospheric surfaces. In this work the sulfur isotopic fractionation factors for SO2 oxidation have been measured on Sahara dust, obtained from the Cape Verde Islands, and sea salt aerosol, which was synthesised in the laboratory according to Millero (1974), modified to contain no sulfate. Sulfur dioxide with a known isotopic composition was oxidised on these surfaces under a variety of conditions including irradiation and ozonation, and the sulfur isotopic composition of the product sulfate was measured with the Cameca NanoSIMS 50. These laboratory results were then used to investigate the uptake of sulfur to particles in an orographic cloud during the HCCT campaign. The campaign took place at the Schmücke mountain in Germany

  10. Analysis of the 1987 Southern California Air Quality Study (SCAQS) sulfur hexafluoride atmospheric tracer data. Final report

    SciTech Connect

    Shair, F.H.

    1991-10-01

    Eight sets of atmospheric tracer experiment data obtained during the 1987 Southern California Air Quality Study (SCAQS) are analyzed by mass balance and qualitative agreement with surface winds gathered during the same period. The sulfur hexafluoride tracer releases done near downtown Los Angeles reveal aspects of the complexity of the atmospheric emission transport from the location. The total material release of sulfur hexafluoride can be accounted for by mass balancing. The mass balances are used to examine the residence time of the tracer in the basin. The residence time for the sulfur hexafluoride tracer released from Vernon CA is 10 hours in the summer, and exceeds 24 hours for the fall. The primary exit route of the sulfur hexafluoride tracer during the summer releases was the San Fernando Valley to the northwest of downtown. The surface-level diagnostic wind model (DWM) was made operational on a PC.

  11. 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. PMID:17804807

  12. Kinetics studies of aqueous phase reactions of Cl atoms and Cl2(-) radicals with organic sulfur compounds of atmospheric interest.

    PubMed

    Zhu, Lei; Nicovich, J Michael; Wine, Paul H

    2005-05-01

    A laser flash photolysis-long path UV-visible absorption technique has been employed to investigate the kinetics of aqueous phase reactions of chlorine atoms (Cl) and dichloride radicals (Cl2(-)) with four organic sulfur compounds of atmospheric interest, dimethyl sulfoxide (DMSO; CH3S(O)CH3), dimethyl sulfone (DMSO2; CH3(O)S(O)CH3), methanesulfinate (MSI; CH3S(O)O-), and methanesulfonate (MS; CH3(O)S(O)O-). Measured rate coefficients at T = 295 +/- 1 K (in units of M(-1) s(-1)) are as follows: Cl + DMSO, (6.3 +/- 0.6) x 10(9); Cl2(-) + DMSO, (1.6 +/- 0.8) x 10(7); Cl + DMSO2, (8.2 +/- 1.6) x 10(5); Cl2(-) + DMSO2, (8.2 +/- 5.5) x 10(3); Cl2(-) + MSI, (8.0 +/- 1.0) x 10(8); Cl + MS, (4.9 +/- 0.6) x 10(5); Cl2(-) + MS, (3.9 +/- 0.7) x 10(3). Reported uncertainties are estimates of accuracy at the 95% confidence level and the rate coefficients for MSI and MS reactions with Cl2(-) are corrected to the zero ionic strength limit. The absorption spectrum of the DMSO-Cl adduct is reported; peak absorbance is observed at 390 nm and the peak extinction coefficient is found to be 5760 M(-1) cm(-1) with a 2sigma uncertainty of +/-30%. Some implications of the new kinetics results for understanding the atmospheric sulfur cycle are discussed. PMID:16833708

  13. 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

  14. Sulfur in the early martian atmosphere revisited: Experiments with a 3-D Global Climate Model

    NASA Astrophysics Data System (ADS)

    Kerber, Laura; Forget, François; Wordsworth, Robin

    2015-11-01

    Volcanic SO2 in the martian atmosphere has been invoked as a way to create a sustained or transient greenhouse during early martian history. Many modeling studies have been performed to test the feasibility of this hypothesis, resulting in a range of conclusions, from highly feasible to highly improbable. In this study we perform a wide range of simulations using the 3-D Laboratoire de Météorologie Dynamique Generic Global Climate Model (GCM) in order to place earlier results into context and to explore the sensitivity of model outcomes to parameters such as SO2 mixing ratio, atmospheric H2O content, background atmospheric pressure, and aerosol size, abundance, and composition. We conclude that SO2 is incapable of creating a sustained greenhouse on early Mars, and that even in the absence of aerosols, local and daily temperatures rise above 273 K for only for limited periods with favorable background CO2 pressures. In the presence of even small amounts of aerosols, the surface is dramatically cooled for realistic aerosol sizes. Brief, mildly warm conditions require the co-occurrence of many improbable factors, while cooling is achieved for a wide range of model parameters. Instead of causing warming, sulfur in the martian atmosphere may have caused substantial cooling, leading to the end of clement climate conditions on early Mars.

  15. Decreased atmospheric sulfur deposition across the Southeastern U.S.: when will watersheds release stored sulfate?

    PubMed

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

    2014-09-01

    Emissions of sulfur dioxide (SO2) to the atmosphere lead to atmospheric deposition of sulfate (SO4(2-)), which is the dominant strong acid anion causing acidification of surface waters and soils in the eastern United States. 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 streamwater SO4(2-) concentrations have been observed in unglaciated watersheds. We calculated SO4(2-) 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 SO4(2-), 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 SO4(2-) over the next two decades. The specific years when the watersheds crossover from retaining to releasing SO4(2-) 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 SO4(2-) retention to release anticipates more widespread reductions in streamwater SO4(2-) concentrations in this region. PMID:25046800

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

    USGS Publications Warehouse

    Rice, Karen C.; Scanlon, Todd S.; 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.

  17. 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.

  18. 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.

  19. 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

  20. Reduced sulfur compounds in the atmosphere of sewer networks in Australia: geographic (and seasonal) variations.

    PubMed

    Wang, B; Sivret, E C; Parcsi, G; Le, N M; Kenny, S; Bustamante, H; Stuetz, R M

    2014-01-01

    The management of odorous emissions from sewer networks has become an important issue for sewer system operators resulting in the need to better understand the composition of reduced sulfur compounds (RSCs). Gaseous RSCs including hydrogen sulfide (H2S), methanethiol (MeSH), dimethyl sulfide (DMS), carbon disulfide (CS2), dimethyl disulfide (DMDS) and dimethyl trisulfide (DMTS) were measured in the atmosphere of selected sewer networks in two major Australian cities (Sydney and Melbourne) during 2011-2012. The RSC concentrations in the sewer air were detected in a highly variable range. H2S and MeSH were found at the highest concentrations, followed by DMS (39.2-94.0 μg/m(3)), CS2 (18.3-19.6 μg/m(3)), DMDS (7.8-49.6 μg/m(3)) and DMTS (10.4-35.3 μg/m(3)). Temporal trends in the occurrence of targeted RSCs were observed and the highest sulfur concentration occurred either in summer or spring, which are typically regarded as the warmer seasons. Statistical significant difference in the magnitude of targeted RSCs was found between samples collected in Sydney and Melbourne. PMID:24647180

  1. 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. PMID:25288761

  2. 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

  3. 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.

  4. 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.

  5. Evaluation of atmosphere-biosphere exchange estimations with TCCON measurements

    NASA Astrophysics Data System (ADS)

    Messerschmidt, J.; Parazoo, N.; Deutscher, N. M.; Roehl, C.; Warneke, T.; Wennberg, P. O.; Wunch, D.

    2012-05-01

    Three estimates of the atmosphere-biosphere exchange are evaluated using Total Carbon Column Observing Network (TCCON) measurements. We investigate the Carnegie-Ames-Stanford Approach (CASA), the Simple Biosphere (SiB) and the GBiome-BGC models transported by the GEOS-Chem model to simulate atmospheric CO2 concentrations for the time period between 2006 and 2010. The CO2 simulations are highly dependent on the choice of the atmosphere-biosphere model and large-scale errors in the estimates are identified through a comparison with TCCON data. Enhancing the CO2 uptake in the boreal forest by 40% and shifting the onset of the growing season significantly improve the simulated seasonal CO2 cycle using CASA estimates. The SiB model gives the best estimate for the atmosphere-biosphere exchange in the comparison with TCCON measurements.

  6. 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...

  7. Multiple oxygen and sulfur isotope compositions of atmospheric sulfate in Baton Rouge, LA, USA

    NASA Astrophysics Data System (ADS)

    Jenkins, Kathryn A.; Bao, Huiming

    Secondary atmospheric sulfates (SAS) is the ultimate oxidation product and sink for sulfur gases of biological, volcanic, and anthropogenic origins on Earth. Their presence in the atmosphere as aqueous or solid phases contributes to acid rain and climate change, thus, understanding SAS formation pathways is pertinent. There has been extensive measurement of δ34S values for SAS, which mainly aimed at source identification. Relatively fewer oxygen isotope compositions ( δ18O, Δ 17O), which are most useful for resolving competing oxidation pathways, were available, however. This study represents the first effort to characterize the Δ 17O, δ18O, and δ34S simultaneously for SAS in a tropospheric air shed. We measured a total of 20 samples collected in Baton Rouge (LA, USA) during a 600-day period. The isotope compositions for atmospheric sulfate range from +0.25‰ to +1.43‰ for Δ 17O, +11.8‰ to +19.3‰ for δ18O, and -1.4‰ to +3.8‰ for δ34S. No apparent correlation is found among Δ 17O, δ18O, or δ34S values. The Δ 17O has no seasonal variation and its values are consistent with an oxidation pathway dominated by aqueous H 2O 2. The δ18O and δ34S are within the range of those observed in other sites around the world and are not characteristic for Baton Rouge. Despite the huge variability in atmospheric condition among mid-latitude sites, the long-term average Δ 17O value for SAS appears to fall within a fairly narrow range from +0.6‰ to +0.8‰, which is ˜1‰ to 2‰ lower than those in polar sites.

  8. Bidirectional Interaction of Alanine with Sulfuric Acid in the Presence of Water and the Atmospheric Implication.

    PubMed

    Wang, Chun-Yu; Ma, Yan; Chen, Jiao; Jiang, Shuai; Liu, Yi-Rong; Wen, Hui; Feng, Ya-Juan; Hong, Yu; Huang, Teng; Huang, Wei

    2016-04-21

    Amino acids are recognized as important components of atmospheric aerosols, which impact on the Earth's climate directly and indirectly. However, much remains unknown about the initial events of nucleation. In this work, the interaction of alanine [NH2CH(CH3)COOH or Ala], one of the most abundant amino acids in the atmosphere, with sulfuric acid (SA) and water (W) has been investigated at the M06-2X/6-311++G(3df, 3pd) level of theory. We have studied thermodynamics of the hydrated (Ala)(SA) core system with up to four water molecules. We found that Ala, with one amino group and one carboxyl group, can interact with H2SO4 and H2O in two directions and that it has a high cluster stabilizing effect similar to that of ammonia, which is one of the key nucleation precursor. The corresponding Gibbs free energies of the (Ala)(SA)(W)n (n = 0-4) clusters formation at 298.15 K predicted that Ala can contribute to the stabilization of small binary clusters. Our results showed that the hydrate distribution is temperature-dependent and that a higher humidity and temperature can contribute to the formation of hydrated clusters. PMID:26997115

  9. Exploring the Capabilities of Satellite Observation of Anthropogenic Sulfur Dioxide (SO2) in the Lower Atmosphere

    NASA Astrophysics Data System (ADS)

    Yang, K.; Krotkov, N. A.; Li, C.; He, H.; Dickerson, R. R.

    2012-12-01

    Anthropogenic activities, such as fuel combustion, oil refining, and metal smelting, emit sulfur dioxide (SO2) into the atmospheric planetary boundary layer (PBL), leading to air quality degradation near the source regions. SO2 in the air is oxidized to form sulfate aerosols, which may have a significant impact on regional air quality and climate. Sulfate aerosols are usually removed from the atmosphere through acid deposition, which can damage the environment and ecosystems. SO2 and sulfate aerosols are sometimes lifted into the middle or upper troposphere and subsequently transported over long distances, affecting remote regions. Space-borne UV instruments, such as Aura/OMI, MetOp/GOME-2, and NPP/OMPS, provide a unique perspective on the spatial and temporal distribution of SO2 over the globe. In this presentation, we will describe the recent advances in retrieval algorithm that provide improved detection and quantification of PBL SO2, and compare the new retrievals with the operational OMI SO2 products to show significant reduction in noise and bias. We will also present validation results obtained by the comparisons with co-located in-situ aircraft measurements to illustrate improved accuracy achieved with the advanced algorithm.

  10. Interaction of mineral dust with gas phase nitric acid and sulfur dioxide during the MINATROC II field campaign: First estimate of the uptake coefficient from atmospheric data

    NASA Astrophysics Data System (ADS)

    Umann, B.; Arnold, F.; Schaal, C.; Hanke, M.; Uecker, J.; Aufmhoff, H.; Balkanski, Y.; van Dingenen, R.

    2005-11-01

    Mineral dust, one of the most abundant aerosols by mass in the atmosphere, may have a lasting but to date almost unexplored effect on the trace gases nitric acid (HNO3) and sulfur dioxide (SO2). These gases have an important influence on, for example, the tropospheric ozone cycle, aerosol formation or acid rain. Within the second part of the MINATROC project (Mineral Dust and Tropospheric Chemistry) we investigated the interaction of mineral dust with gaseous HNO3 and SO2. The measurements were performed on a high mountain plateau (Izaña, Tenerife, 2367 m asl) using the highly sensitive CIMS (Chemical Ionization Mass Spectrometry) technique. During five periods of medium and one period of high atmospheric dust load, the HNO3 concentration decreased with increasing dust concentrations, and in all cases the HNO3 detection limit was reached. From the HNO3 decrease the uptake coefficient ? was calculated for the first time on the basis of in situ measurements. For the observed events, ? varied between 0.017 and 0.054. Moreover, during the dust events a significant decrease of ozone (O3) of the order of 30% was detected. The measurements and the analyses made in this paper show that the direct uptake of O3 on dust is a minor pathway for O3 depletion compared to the indirect effect, i.e., HNO3 depletion on dust which takes away a source of the O3 precursors nitrogen oxides. In contrast, a general interaction between SO2 and mineral dust was not observed. Positive as well as negative and no correlations between SO2 and mineral dust were detected.

  11. [Investigations on Sulfur and Carbon Isotopic Compositions of Potential Polluted Sources in Atmospheric PM₂.₅ in Nanjing Region].

    PubMed

    Shi, Lei; Guo, Zhao-bing; Jiang, Wen-juan; Rui, Mao-ling; Zeng, Gang

    2016-01-15

    Potential pollution sources of atmospheric PM₂.₅ in Nanjing region were collected, and sulfur and carbon isotopic compositions were determined by EA-IRMS synchronously. The results showed that δ³⁴S and δ¹³C values ranged from 1.8‰-3.7‰ and -25.50‰- -23.57‰ in coal soot particles; 4.6‰-9.7‰ and -26.32‰- -23.57‰ in vehicle exhaust; 5.2‰-9.9‰ and -19.30‰- -30.42‰ in straw soot particles, respectively. Besides, the δ¹³C value of dust was -13.45‰. It can be observed that sulfur isotopic compositions in coal soot were lower, while the carbon isotopic composition in dust was higher. Comparing with δ³⁴S and δ¹³C values in domestic and foreign polluted sources, we found that sulfur and carbon isotopes in atmospheric PM₂.₅ in Nanjing region presented an obvious regional characteristics. Therefore, the source spectrum of sulfur and carbon isotopic compositions in Nanjing region might provide an insight into source apportionment of atmospheric PM₂.₅. PMID:27078936

  12. 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. PMID:19785272

  13. 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.

  14. Atmospheric sulfur hexafluoride in-situ measurements at the Shangdianzi regional background station in China.

    PubMed

    Yao, Bo; Zhou, Lingxi; Xia, Lingjun; Zhang, Gen; Guo, Lifeng; Liu, Zhao; Fang, Shuangxi

    2014-12-01

    We present in-situ measurements of atmospheric sulfur hexafluoride (SF6) conducted by an automated gas chromatograph-electron capture detector system and a gas chromatography/mass spectrometry system at a regional background site, Shangdianzi, in China, from June 2009 to May 2011, using the System for Observation of Greenhouse gases in Europe and Asia and Advanced Global Atmospheric Gases Experiment (AGAGE) techniques. The mean background and polluted mixing ratios for SF6 during the study period were 7.22 × 10⁻¹² (mol/mol, hereinafter) and 8.66 × 10⁻¹², respectively. The averaged SF6 background mixing ratios at Shangdianzi were consistent with those obtained at other AGAGE stations located at similar latitudes (Trinidad Head and Mace Head), but larger than AGAGE stations in the Southern Hemisphere (Cape Grim and Cape Matatula). SF6 background mixing ratios increased rapidly during our study period, with a positive growth rate at 0.30 × 10⁻¹² year⁻¹. The peak to peak amplitude of the seasonal cycle for SF6 background conditions was 0.07 × 10⁻¹², while the seasonal fluctuation of polluted conditions was 2.16 × 10⁻¹². During the study period, peak values of SF6 mixing ratios occurred in autumn when local surface horizontal winds originated from W/WSW/SW/SWS/S sectors, while lower levels of SF6 mixing ratios appeared as winds originated from N/NNE/NE/ENE/E sectors. PMID:25499493

  15. 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.

  16. 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.

  17. Origins of sulfur compounds in the atmosphere of a zone of high productivity (Gulf of Guinea)

    SciTech Connect

    Delmas, R.; Servant, J.

    1982-12-20

    Recent observations have suggested substantial emission of sulfur compounds by oceanic water which could explain the presence of SO/sub 2/ and SO/sup +//sub 4/ in the air above these waters. The emission is thought to increase with the productivity of the oceanic zones. This point is discussed in relation to the Gulf of Guinea, a zone of high productivity. During the first two campaigns between Dakar, Abidjan, and the Gulf of Guinea SO/sup +//sub 4/ concentrations were measured in the air. Between Abidjan and the Gulf of Guinea the atmospheric SO= /sub 4/ concentrations decreased from 800 to 400 ng m/sup -3/. During the third campaign, between Abidjan and the South Equatorial Current (latitude 1/sup 0/S), the H/sub 2/S and SO/sub 2/ concentrations were measured. The mean H/sub 2/S concentration was 20 ng m/sup -3/, and that of SO/sub 2/ varied between 120 and under 50 ng m/sup -3/. The origins of SO/sub 2/ and SO/sup +//sub 4/ in the air of this area are discussed through the daily variations of the H/sub 2/S content of the air and a contribution from the forested zones of West Africa.

  18. 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. PMID:26000788

  19. 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.

  20. Effect of atmospheric sulfur pollutants derived from acid precipitation on the benthic dynamics of lakes

    SciTech Connect

    Mitchell, M.J.

    1982-11-01

    Sulfuric acid is a major contributor to acid precipitation in the United States. The relationship of acid precipitation to the sulfur dynamics of three lakes in New York was studied. For South Lake, which has probably been acidified, the sulfur profile in the sediment corresponded to historical changes in anthropogenic sulfur inputs. In all three study lakes, the organic sulfur constituents, which generally have been ignored in limnological investigations, played a major role in sulfur dynamics. The transformations and fluxes of inorganic and organic sulfur differed among the lakes and reflected characteristic abiotic and biotic properties, including productivity parameters. The community structure and secondary production of the invertebrate benthos were ascertained and, for South Lake, were similar to other acidified lakes. The importance of benthic insects on sulfur dynamics was demonstrated. Further studies on sulfur in lakes will enhance the understanding of the role of these anthropogenic inputs on lake systems and permit a more accurate appraisal of the present and future impacts of acidic deposition on water quality. 10 references.

  1. The carbon and sulfur cycles and atmospheric oxygen from middle Permian to middle Triassic

    NASA Astrophysics Data System (ADS)

    Berner, Robert A.

    2005-07-01

    The results of a theoretical isotope mass balance model are presented for the time dependence of burial and weathering-plus-degassing fluxes within the combined long-term carbon and sulfur cycles. Averaged data for oceanic δ 13C and δ 34S were entered for every million years from 270 to 240 Ma (middle Permian to middle Triassic) to study general trends across the Permian-Triassic boundary. Results show a drop in the rate of global organic matter burial during the late Permian and a predominance of low values during the early-to-middle Triassic. This overall decrease with time is ascribed mainly to epochs of conversion of high biomass forests to low biomass herbaceous vegetation resulting in a decrease in the production of terrestrially derived organic debris. Additional contributions to lessened terrestrial carbon burial were increased aridity and a drop in sea level during the late Permian which led to smaller areas of low-lying coastal wetlands suitable for coal and peat deposition. Mirroring the drop in organic matter deposition was an increase in the burial of sedimentary pyrite, and a dramatic increase in the calculated global mean ratio of pyrite-S to organic-C. High S/C values resulted from an increase of deposition in marine euxinic basins combined with a decrease in the burial of low-pyrite associated terrestrial organic matter. The prediction of increased oceanic anoxia during the late Permian and early Triassic agrees with independent studies of the composition of sedimentary rocks. Weathering plus burial fluxes for organic carbon and pyrite sulfur were used to calculate changes in atmospheric oxygen. The striking result is a continuous drop in O 2 concentration from ˜30% to ˜13% over a twenty million year period. This drop was brought about mainly by a decrease in the burial of terrestrially derived organic matter. but with a possible contribution from the weathering of older organic matter on land. It must have exerted a considerable influence on

  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. Atmospheric density estimation using satellite precision orbit ephemerides

    NASA Astrophysics Data System (ADS)

    Arudra, Anoop Kumar

    The current atmospheric density models are not capable enough to accurately model the atmospheric density, which varies continuously in the upper atmosphere mainly due to the changes in solar and geomagnetic activity. Inaccurate atmospheric modeling results in erroneous density values that are not accurate enough to calculate the drag estimates acting on a satellite, thus leading to errors in the prediction of satellite orbits. This research utilized precision orbit ephemerides (POE) data from satellites in an orbit determination process to make corrections to existing atmospheric models, thus resulting in improved density estimates. The work done in this research made corrections to the Jacchia family atmospheric models and Mass Spectrometer Incoherent Scatter (MSIS) family atmospheric models using POE data from the Ice, Cloud and Land Elevation Satellite (ICESat) and the Terra Synthetic Aperture Radar-X Band (TerraSAR-X) satellite. The POE data obtained from these satellites was used in an orbit determination scheme which performs a sequential filter/smoother process to the measurements and generates corrections to the atmospheric models to estimate density. This research considered several days from the year 2001 to 2008 encompassing all levels of solar and geomagnetic activity. Density and ballistic coefficient half-lives with values of 1.8, 18, and 180 minutes were used in this research to observe the effect of these half-life combinations on density estimates. This research also examined the consistency of densities derived from the accelerometers of the Challenging Mini Satellite Payload (CHAMP) and Gravity Recovery and Climate Experiment (GRACE) satellites by Eric Sutton, from the University of Colorado. The accelerometer densities derived by Sutton were compared with those derived by Sean Bruinsma from CNES, Department of Terrestrial and Planetary Geodesy, France. The Sutton densities proved to be nearly identical to the Bruinsma densities for all the

  4. 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. PMID:27380080

  5. In situ total-electron-yield sulfur K-edge XAFS measurements during exposure of copper to an SO 2-containing humid atmosphere

    NASA Astrophysics Data System (ADS)

    Song, Inho; Rickett, Brett; Janavicius, Paul; Payer, Joe H.; Antonio, Mark R.

    1995-02-01

    A total-electron-yield (TEY) detector was designed and constructed for in situ X-ray absorption fine structure (XAFS) measurements of the sulfur-containing species formed during exposure of copper to a humid atmosphere containing SO 2. Using the detector, gas phase XAFS spectra were also collected for both dry and humid SO 2 atmospheres. This work presents the experimental technique and examples of the sulfur K-edge spectra collected during the study.

  6. [Atmospheric parameter estimation for LAMOST/GUOSHOUJING spectra].

    PubMed

    Lu, Yu; Li, Xiang-Ru; Yang, Tan

    2014-11-01

    It is a key task to estimate the atmospheric parameters from the observed stellar spectra in exploring the nature of stars and universe. With our Large Sky Area Multi-Object Fiber Spectroscopy Telescope (LAMOST) which begun its formal Sky Survey in September 2012, we are obtaining a mass of stellar spectra in an unprecedented speed. It has brought a new opportunity and a challenge for the research of galaxies. Due to the complexity of the observing system, the noise in the spectrum is relatively large. At the same time, the preprocessing procedures of spectrum are also not ideal, such as the wavelength calibration and the flow calibration. Therefore, there is a slight distortion of the spectrum. They result in the high difficulty of estimating the atmospheric parameters for the measured stellar spectra. It is one of the important issues to estimate the atmospheric parameters for the massive stellar spectra of LAMOST. The key of this study is how to eliminate noise and improve the accuracy and robustness of estimating the atmospheric parameters for the measured stellar spectra. We propose a regression model for estimating the atmospheric parameters of LAMOST stellar(SVM(lasso)). The basic idea of this model is: First, we use the Haar wavelet to filter spectrum, suppress the adverse effects of the spectral noise and retain the most discrimination information of spectrum. Secondly, We use the lasso algorithm for feature selection and extract the features of strongly correlating with the atmospheric parameters. Finally, the features are input to the support vector regression model for estimating the parameters. Because the model has better tolerance to the slight distortion and the noise of the spectrum, the accuracy of the measurement is improved. To evaluate the feasibility of the above scheme, we conduct experiments extensively on the 33 963 pilot surveys spectrums by LAMOST. The accuracy of three atmospheric parameters is log Teff: 0.006 8 dex, log g: 0.155 1 dex

  7. Stereo image motion monitor for atmospheric mitigation and estimation

    NASA Astrophysics Data System (ADS)

    Gibson, Kristofor B.

    2015-09-01

    The knowledge of the turbulence strength in the atmosphere is important for many applications. Imagery in the atmosphere experience significant blur when the turbulence is strong. This can be automatically improved (without user intervention) if the turbulence strength is known. The performance of a high-power laser emitting in the atmosphere can be predicted if the statistics of the turbulence strength is known. If not predicted correctly, the laser may unintentionally destroy a target or fail to be able to disable a target. In this article, we review existing methods that estimate turbulence strength, provide a more in depth error analysis, and propose a new method for estimating and mitigating turbulence in the atmosphere. We focus on methods that are passive in design in order to prevent detection in surveillance scenarios and tactical situations. We also propose a new method, stereo image motion monitor (SIMM) which is a system containing two independent apertures. Our goal in this approach is threefold: 1) We can measure r0 using the DIMM method 2) We can simultaneously estimate r0 individually for each aperture and 3) We have multiple views of the same scene thus can increase the number of frames used in turbulence mitigation methods.

  8. Net atmospheric mercury deposition to Svalbard: Estimates from lacustrine sediments

    NASA Astrophysics Data System (ADS)

    Drevnick, Paul E.; Yang, Handong; Lamborg, Carl H.; Rose, Neil L.

    2012-11-01

    In this study we used lake sediments, which faithfully record Hg inputs, to derive estimates of net atmospheric Hg deposition to Svalbard, Norwegian Arctic. With the exception of one site affected by local pollution, the study lakes show twofold to fivefold increases in sedimentary Hg accumulation since 1850, likely due to long-range atmospheric transport and deposition of anthropogenic Hg. Sedimentary Hg accumulation in these lakes is a linear function of the ratio of catchment area to lake area, and we used this relationship to model net atmospheric Hg flux: preindustrial and modern estimates are 2.5 ± 3.3 μg m-2 y-1 and 7.0 ± 3.0 μg m-2 y-1, respectively. The modern estimate, by comparison with data for Hg wet deposition, indicates that atmospheric mercury depletion events (AMDEs) or other dry deposition processes contribute approximately half (range 0-70%) of the net flux. Hg from AMDEs may be moving in significant quantities into aquatic ecosystems, where it is a concern because of contamination of aquatic food webs.

  9. 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. PMID:25806615

  10. Multiple oxygen and sulfur isotope compositions of secondary atmospheric sulfate in a mega-city in central China

    NASA Astrophysics Data System (ADS)

    Li, Xiaoqian; Bao, Huiming; Gan, Yiqun; Zhou, Aiguo; Liu, Yunde

    2013-12-01

    Sulfate aerosol is an important atmosphere constituent that can be formed secondarily through the oxidation of sulfur gases. Atmospheric sulfur oxidation can take different pathways depending on meteorological conditions, which affects sulfate aerosol size and composition and therefore local or global climate. The magnitude of 17O enrichment (Δ17O) in secondary atmospheric sulfate (SAS) is a tracer for the apportionment of different sulfur oxidation pathways. Atmospheric chemistry-transport models predict a low 17O enrichment (Δ17O < 1‰) for SAS in mid-latitude continental sites. However, there are few long-term site observations to test the prediction, and data from interior metropolitan sites are entirely absent. We report here multiple oxygen and sulfur isotope compositions (Δ17O, δ18O, and δ34S) of SAS collected over a 950-day period in the city of Wuhan, central China, and to compare to data from a similar sampling campaign in the city of Baton Rouge, LA, U.S.A. The isotope compositions of bulk atmospheric sulfate closely reflect those of SAS in Wuhan, with the Δ17O ranging from 0.14‰ to 1.02‰, the δ18O from 8.0‰ to 16.1‰, and the δ34S from 2.1‰ to 7.3‰. The average Δ17O value at 0.53‰-0.59‰ is consistent with model prediction for continental interior, mid-latitude sites. The Asian monsoon-influenced meteorological condition in Wuhan appears to produce a weak but discernible seasonal pattern for Δ17O and δ18O of the SAS. The average rainwater pH value is higher in Wuhan than in Baton Rouge (5.47 versus 4.78) while the two cities have a statistically identical average SAS Δ17O value. We suggest that the higher pH does result in a higher fraction of SAS generated by aqueous O3 oxidation, but the resulted higher Δ17O value for SAS is diluted by the 17O-normal SAS generated from an enhanced transition-metal-catalyzed O2 oxidation pathway. The enhancement is corroborated with the much higher content of atmospheric particulate matter

  11. Biomonitoring of Sulfur-Containing Pollutants in an Urban Atmosphere by FTIR Spectroscopy

    NASA Astrophysics Data System (ADS)

    Meysurova, A. F.; Khizhnyak, S. D.; Notov, A. A.; Pakhomov, P. M.

    2014-09-01

    The relative content of sulfur-containing compounds in samples of epiphytic lichens Hypogymnia physodes collected at recreation zones of Tver city with different levels of air pollution was determined using FTIR spectroscopy. The sulfur dioxide (SO2) concentration was also measured at the same recreation zones using an IR gas analyzer. The measurements were compared by two methods. Maps of SO2 air pollution in Tver city were constructed.

  12. 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.

  13. [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. PMID:26978937

  14. Atmospheric Density Corrections Estimated from Fitted Drag Coefficients

    NASA Astrophysics Data System (ADS)

    McLaughlin, C. A.; Lechtenberg, T. F.; Mance, S. R.; Mehta, P.

    2010-12-01

    Fitted drag coefficients estimated using GEODYN, the NASA Goddard Space Flight Center Precision Orbit Determination and Geodetic Parameter Estimation Program, are used to create density corrections. The drag coefficients were estimated for Stella, Starlette and GFZ using satellite laser ranging (SLR) measurements; and for GEOSAT Follow-On (GFO) using SLR, Doppler, and altimeter crossover measurements. The data analyzed covers years ranging from 2000 to 2004 for Stella and Starlette, 2000 to 2002 and 2005 for GFO, and 1995 to 1997 for GFZ. The drag coefficient was estimated every eight hours. The drag coefficients over the course of a year show a consistent variation about the theoretical and yearly average values that primarily represents a semi-annual/seasonal error in the atmospheric density models used. The atmospheric density models examined were NRLMSISE-00 and MSIS-86. The annual structure of the major variations was consistent among all the satellites for a given year and consistent among all the years examined. The fitted drag coefficients can be converted into density corrections every eight hours along the orbit of the satellites. In addition, drag coefficients estimated more frequently can provide a higher frequency of density correction.

  15. 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. PMID:25525712

  16. 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

  17. 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. PMID:25561552

  18. Estimating stellar atmospheric parameters based on Lasso features

    NASA Astrophysics Data System (ADS)

    Liu, Chuan-Xing; Zhang, Pei-Ai; Lu, Yu

    2014-04-01

    With the rapid development of large scale sky surveys like the Sloan Digital Sky Survey (SDSS), GAIA and LAMOST (Guoshoujing telescope), stellar spectra can be obtained on an ever-increasing scale. Therefore, it is necessary to estimate stellar atmospheric parameters such as Teff, log g and [Fe/H] automatically to achieve the scientific goals and make full use of the potential value of these observations. Feature selection plays a key role in the automatic measurement of atmospheric parameters. We propose to use the least absolute shrinkage selection operator (Lasso) algorithm to select features from stellar spectra. Feature selection can reduce redundancy in spectra, alleviate the influence of noise, improve calculation speed and enhance the robustness of the estimation system. Based on the extracted features, stellar atmospheric parameters are estimated by the support vector regression model. Three typical schemes are evaluated on spectral data from both the ELODIE library and SDSS. Experimental results show the potential performance to a certain degree. In addition, results show that our method is stable when applied to different spectra.

  19. 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

  20. Hubble space telescope far-ultraviolet observations of Io: Determining atmospheric abundances, mapping the sulfur dioxide distribution, and correlating the molecular and atomic atmosphere

    NASA Astrophysics Data System (ADS)

    Feaga, Lori Michelle

    2006-05-01

    Io's molecular and atomic atmosphere has been studied via far-ultraviolet spectroscopy obtained with the Hubble Space Telescope . Examination of an extensive data set reveals a sunlit SO 2 atmosphere which is temporally stable on a global scale, with only small local changes. An anti-/sub-Jovian asymmetry in the SO 2 distribution persists in all of the observations. The atmosphere is densest in the anti-Jovian equatorial regions, with a maximum column density of 5.0 × 10^16 cm -2 at 140° longitude. The SO 2 atmosphere also has greater latitudinal extent on the anti-Jovian hemisphere as compared to the sub-Jovian. The atmospheric distribution is best correlated with the location of known volcanic plumes. Theoretical sublimation atmosphere models cannot reproduce the asymmetry alone. Atomic S, O and Cl are also detected. Their abundances are derived and compared to the SO 2 . Sulfur is measured at a relative abundance of 9 × 10^-3 compared to SO 2 , oxygen at 0.05, and chlorine at 3-8.5 × 10^-4 .

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

    NASA Astrophysics Data System (ADS)

    Bao, Huiming; Reheis, Marith C.

    2003-07-01

    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 (δ34S and δ18O) are 5.8 ± 1.4 (CDT) and 11.2 ± 1.9 (SMOW) (n = 47), respectively. Samples have an oxygen 17 anomaly (Δ17O), with an average value of 1.0 ± 0.6‰. Except for a weak positive correlation between δ18O and Δ17O values (r2 ≈ 0.4), no correlation exists for δ18O versus δ34S, Δ17O versus δ34S, or any of the three isotopic compositions versus elevation of the sample site. Exceptional positive Δ17O values (up to 4.23‰) are found in samples from sites in the vicinity of large cities or major highways, and near-zero Δ17O 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 δ18O, ˜2.1‰ higher for δ34S, and ˜0.3‰ lower for Δ17O 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.

  2. 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.

  3. 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.

  4. LOREP 1993 summary report: Airborne measurements of meteorological variables, atmospheric particles and sulfur hexafluoride. Technical memo

    SciTech Connect

    Wilkison, S.W.; Wellman, D.L.

    1996-03-01

    Meteorological variables and sulfur hexafluoride (SF6) were measured using the NOAA King Air research aircraft during February and March, 1993, over the Sierra Nevada Range of northern California as part of the Lake Oroville Runoff Enhancement Prototype Program (LOREP 1993). Race track pattern flights were made from approximately Sierraville, CA, to Gasner, CA. Airborne sampling was used to locate a plume containing sulfur hexafluoride as a tracer and propane as a seeding agent. The aircraft also carried an optical imaging probe. This report introduces the program in general, discusses the objectives of LOREP 1993, the instrumentation used and the data obtained by the NOAA airborne operation.

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

    PubMed

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

    2016-07-01

    Sulfur isotopic anomalies (∆(33)S and ∆(36)S) 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 δ(34)S 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 ∆(33)S 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 δ(34)S peak at +9‰ is associated with non-(33)S-anomalous barites displaying negative ∆(36)S 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

  6. 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.

  7. Estimation of Dynamical Parameters in Atmospheric Data Sets

    NASA Technical Reports Server (NTRS)

    Wenig, Mark O.

    2004-01-01

    In this study a new technique is used to derive dynamical parameters out of atmospheric data sets. This technique, called the structure tensor technique, can be used to estimate dynamical parameters such as motion, source strengths, diffusion constants or exponential decay rates. A general mathematical framework was developed for the direct estimation of the physical parameters that govern the underlying processes from image sequences. This estimation technique can be adapted to the specific physical problem under investigation, so it can be used in a variety of applications in trace gas, aerosol, and cloud remote sensing. The fundamental algorithm will be extended to the analysis of multi- channel (e.g. multi trace gas) image sequences and to provide solutions to the extended aperture problem. In this study sensitivity studies have been performed to determine the usability of this technique for data sets with different resolution in time and space and different dimensions.

  8. 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.

  9. Estimation of stellar atmospheric parameters from SDSS/SEGUE spectra

    NASA Astrophysics Data System (ADS)

    Re Fiorentin, P.; Bailer-Jones, C. A. L.; Lee, Y. S.; Beers, T. C.; Sivarani, T.; Wilhelm, R.; Allende Prieto, C.; Norris, J. E.

    2007-06-01

    We present techniques for the estimation of stellar atmospheric parameters (T_eff, log~g, [Fe/H]) for stars from the SDSS/SEGUE survey. The atmospheric parameters are derived from the observed medium-resolution (R = 2000) stellar spectra using non-linear regression models trained either on (1) pre-classified observed data or (2) synthetic stellar spectra. In the first case we use our models to automate and generalize parametrization produced by a preliminary version of the SDSS/SEGUE Spectroscopic Parameter Pipeline (SSPP). In the second case we directly model the mapping between synthetic spectra (derived from Kurucz model atmospheres) and the atmospheric parameters, independently of any intermediate estimates. After training, we apply our models to various samples of SDSS spectra to derive atmospheric parameters, and compare our results with those obtained previously by the SSPP for the same samples. We obtain consistency between the two approaches, with RMS deviations on the order of 150 K in T_eff, 0.35 dex in log~g, and 0.22 dex in [Fe/H]. The models are applied to pre-processed spectra, either via Principal Component Analysis (PCA) or a Wavelength Range Selection (WRS) method, which employs a subset of the full 3850-9000Å spectral range. This is both for computational reasons (robustness and speed), and because it delivers higher accuracy (better generalization of what the models have learned). Broadly speaking, the PCA is demonstrated to deliver more accurate atmospheric parameters when the training data are the actual SDSS spectra with previously estimated parameters, whereas WRS appears superior for the estimation of log~g via synthetic templates, especially for lower signal-to-noise spectra. From a subsample of some 19 000 stars with previous determinations of the atmospheric parameters, the accuracies of our predictions (mean absolute errors) for each parameter are T_eff to 170/170 K, log~g to 0.36/0.45 dex, and [Fe/H] to 0.19/0.26 dex, for methods (1

  10. Validation of aerosol estimation in atmospheric correction algorithm ATCOR

    NASA Astrophysics Data System (ADS)

    Pflug, B.; Main-Knorn, M.; Makarau, A.; Richter, R.

    2015-04-01

    Atmospheric correction of satellite images is necessary for many applications of remote sensing, i.e. computation of vegetation indices and biomass estimation. The first step in atmospheric correction is estimation of the actual aerosol properties. Due to the spatial and temporal variability of aerosol amount and type, this step becomes crucial for an accurate correction of satellite data. Consequently, the validation of aerosol estimation contributes to the validation of atmospheric correction algorithms. In this study we present the validation of aerosol estimation using own sun photometer measurements in Central Europe and measurements of AERONET-stations at different locations in the world. Our ground-based sun photometer measurements of vertical column aerosoloptical thickness (AOT) spectra are performed synchronously to overpasses of the satellites RapidEye, Landsat 5, Landsat 7 and Landsat 8. Selected AERONET data are collocated to Landsat 8 overflights. The validation of the aerosol retrieval is conducted by a direct comparison of ground-measured AOT with satellite derived AOT using the ATCOR tool for the selected satellite images. The mean uncertainty found in our experiments is AOT550nm ~ 0.03±0.02 for cloudless conditions with cloud+haze fraction below 1%. This AOT uncertainty approximately corresponds to an uncertainty in surface albedo of ρ ~ 0.003. Inclusion of cloudy and hazy satellite images into the analysis results in mean AOT550nm ~ 0.04±0.03 for both RapidEye and Landsat imagery. About 1/3 of samples perform with the AOT uncertainty better than 0.02 and about 2/3 perform with AOT uncertainty better than 0.05.

  11. 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)

  12. 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.

  13. 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.

  14. Sulfuric acid vapor in the atmosphere of Venus as observed by the Venus Express Radio Science experiment VeRa

    NASA Astrophysics Data System (ADS)

    Oschlisniok, Janusz; Pätzold, Martin; Häusler, Bernd; Tellmann, Silvia; Bird, Mike; Andert, Tom

    2016-04-01

    The cloud deck within Venus' atmosphere, which covers the entire planet between approx. 50 and 70 km altitude, consists mostly of liquid and gaseous sulfuric acid. The gaseous part increases strongly just below the main clouds and builds an approx. 15 km thick haze layer of H2SO4. This region is responsible for a strong absorption of radio waves as seen in VeRa radio science observations. The amount of the absorption, which is used to derive the abundance of gaseous sulfuric acid, depends on the signal frequency. VeRa probed the atmosphere of Venus between 2006 and 2015 with radio signals at 13 cm (S-band) and 3.6 cm (X-band) wavelengths. We present H2SO4 profiles derived from S-band and X-band absorption during the first occultation season in 2006. The comparison of the H2SO4 profiles derived from both frequency bands provides a reliable picture of the H2SO4 abundance. Distinct differences in the S- and X-band profiles may give a clue to increased SO2 abundances. The derived VeRa results shall be compared with results provided by other experiments onboard Venus Express as well as with previous missions.

  15. UPPER-BOUND QUANTITATIVE CANCER RISK ESTIMATES FOR POPULATION ADJACENT TO SULFUR MUSTARD INCINERATION FACILITIES

    EPA Science Inventory

    This document characterizes the potential cancer hazard to populations residing near sulfur mustard incineration facilities while the incineration is taking place. he carcinogenicity of sulfur mustard is reviewed briefly to show what evidence has lead to the previously-accepted c...

  16. 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

  17. 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.

  18. 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.

  19. 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.

  20. 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

  1. Background error covariance estimation for atmospheric CO2 data assimilation

    NASA Astrophysics Data System (ADS)

    Chatterjee, Abhishek; Engelen, Richard J.; Kawa, Stephan R.; Sweeney, Colm; Michalak, Anna M.

    2013-09-01

    any data assimilation framework, the background error covariance statistics play the critical role of filtering the observed information and determining the quality of the analysis. For atmospheric CO2 data assimilation, however, the background errors cannot be prescribed via traditional forecast or ensemble-based techniques as these fail to account for the uncertainties in the carbon emissions and uptake, or for the errors associated with the CO2 transport model. We propose an approach where the differences between two modeled CO2 concentration fields, based on different but plausible CO2 flux distributions and atmospheric transport models, are used as a proxy for the statistics of the background errors. The resulting error statistics: (1) vary regionally and seasonally to better capture the uncertainty in the background CO2 field, and (2) have a positive impact on the analysis estimates by allowing observations to adjust predictions over large areas. A state-of-the-art four-dimensional variational (4D-VAR) system developed at the European Centre for Medium-Range Weather Forecasts (ECMWF) is used to illustrate the impact of the proposed approach for characterizing background error statistics on atmospheric CO2 concentration estimates. Observations from the Greenhouse gases Observing SATellite "IBUKI" (GOSAT) are assimilated into the ECMWF 4D-VAR system along with meteorological variables, using both the new error statistics and those based on a traditional forecast-based technique. Evaluation of the four-dimensional CO2 fields against independent CO2 observations confirms that the performance of the data assimilation system improves substantially in the summer, when significant variability and uncertainty in the fluxes are present.

  2. 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.

  3. 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

  4. 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

  5. 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. PMID:26650082

  6. 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

  7. 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).

  8. 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.

  9. Key unknowns in estimating atmospheric emissions from UK land management

    NASA Astrophysics Data System (ADS)

    Misselbrook, T. H.; Cape, J. N.; Cardenas, L. M.; Chadwick, D. R.; Dragosits, U.; Hobbs, P. J.; Nemitz, E.; Reis, S.; Skiba, U.; Sutton, M. A.

    2011-02-01

    Robust emission inventories of atmospheric pollutants are critical to understanding and predicting impacts, identifying key sources and mitigation opportunities. The objective of this study was to review the extent to which UK land management is accounted for as a source of emission of ammonia (NH 3), nitrous oxide (N 2O), nitrogen oxides (NO x), organic nitrogen (N org), methane (CH 4), non-methane volatile organic compounds (NMVOC), particulate matter (PM) and heavy metals (HM), in comparison with the current state of scientific knowledge; to ascertain whether there is evidence for significant gaps or that key emission sources have been overlooked. The processes leading to emissions of NH 3, N 2O and CH 4 are largely understood and all major sources are thought to be captured in the current inventory. Quantification of uncertainties in the estimates for some of these sources is still required, as is an assessment of the potential improvement in accuracy of estimates through the development of country-specific emission factors for N 2O and CH 4 in particular. There is limited knowledge about sources and processes leading to emissions of N org and the role that these may play in local and global nitrogen budgets. Land management is known to be a source of NO x, NMVOC and PM emissions, and potentially also HM emissions. Improved quantification is required to assess the importance of land management as a source of these pollutants in comparison with other sectors and, if appropriate, to determine the potential for mitigation.

  10. The estimated atmospheric lead emissions in China, 1990-2009

    NASA Astrophysics Data System (ADS)

    Li, Qian; Cheng, Hongguang; Zhou, Tan; Lin, Chunye; Guo, Shu

    2012-12-01

    Estimates of atmospheric emissions of lead from anthropogenic sources in China from 1990 to 2009 are presented with the information on emissions of both total lead and its spatial distribution in regions. The total emissions during the period 1990-2009 are nearly 200 000 tons. Motor vehicle gasoline combustion was the largest source of anthropogenic emissions. The estimated release of 117 800 t of lead represented 60% of the total emissions. Substantial decline occurred in 2001, when the total emissions were about 81% less than the 2000 value. The reduced lead content of motor vehicle gasoline is the primary reason for the decreased in lead emissions in 2001. After leaded gasoline was phased out, coal combustion became the principal source of emissions. Based on data on emissions from 2005 through 2009, the emissions are concentrated in eastern and central China due to the high level of coal consumption and non-ferrous metal smelting. The five provinces with the largest amounts of lead emissions are Shandong, Hebei, Shanxi, Henan and Jiangsu. These five regions produced nearly 40% of the total.

  11. Modeling Atmospheric Sulfur Over the Northern Hemisphere during the Aerosol Characterization Experiment 2 Experimental Period

    SciTech Connect

    Benkovitz, C; Schwartz, Stephen E.; Jensen, Michael P.; Miller, Mark A.; Easter, Richard C.; Bates, Timothy S.

    2004-11-25

    A high-resolution (1{sup o} x 1{sup o}, 27 vertical levels) Eulerian chemical transport and transformation model for sulfate, SO{sub 2}, and related species driven by analyzed forecast meteorological data has been run for the Northern Hemisphere for June-July 1997 and extensively evaluated with observational data, mainly from air-quality and precipitation chemistry networks. For {approx}5000 evaluations, 50% of the modeled sulfate 24-h mixing ratios were within a factor of 1.85 of the observations; 50% of {approx}328 concurrent subgrid observations were within a factor of 1.33. Much greater subgrid variation for 24-h SO{sub 2} mixing ratios (50% of {approx}3552 observations were within a factor of 2.32) reflects high variability of this primary species; for {approx}12,600 evaluations 50% of modeled mixing ratios were within a factor of 2.54 of the observations. These results indicate that a substantial fraction of the modeled and observed differences is due to subgrid variation and/or measurement error. Sulfate mixing ratios are identified by source type (biogenic, volcanic, and anthropogenic) and production mechanism (primary and by gas-phase and aqueous-phase oxidation). Examination of key diagnostics showed substantial variation for the different types of sulfur, e.g., SO{sub 2} aqueous-phase oxidation rates of 29 to 102% day{sup -1}, sulfate residence times of 4 to 9 days. Volcanic emissions contributed 10% of the sulfate burden and 6% of emissions, because the elevated release allows 2 large fractional conversion of SO{sub 2} and long residence time. Biogenic SO{sub 2} was generally at lower concentrations than H{sub 2}O{sub 2}, resulting in efficient aqueous-phase oxidation; this source type contributed 13% of emissions but only 5% of sulfate burden. Anthropogenic sources were the dominant contributors to sulfur emissions, 80%, and sulfate burden, 84%.

  12. Continuous-flow determination of aqueous sulfur by atmospheric-pressure helium microwave-induced plasma atomic emission spectrometry with gas-phase sample introduction

    NASA Astrophysics Data System (ADS)

    Nakahara, Taketoshi; Mori, Toshio; Morimoto, Satoru; Ishikawa, Hiroshi

    1995-06-01

    A simple continuous-flow generation of volatile hydrogen sulfide and sulfur dioxide by acidification of aqueous sulfide and sulfite ions, respectively, is described for the determination of low concentrations of sulfur by atmospheric-pressure helium microwave-induced plasma atomic emission spectrometry (MIP-AES) in the normal ultraviolet (UV) and vacuum ultraviolet (VUV) regions of the spectrum. For measuring spectral lines in the VUV region, the monochromator and the enclosed external optical path between the MIP source and the entrance slit of the monochromator have both been purged with nitrogen to minimize oxygen absorption below 190 nm. Sulfur atomic emission lines at 180.73, 182.04 and 217.05 nm have been selected as the analytical lines. Of the various acids examined, 1.0 M hydrochloric acid is the most favorable for both the generation of hydrogen sulfide from sulfide ions and sulfur dioxide from sulfite ions. Either generated hydrogen sulfide or sulfur dioxide is separated from the solution in a simple gas-liquid separator and swept into the helium stream of a microwave-induced plasma for analysis. The best attainable detection limits (3 σ criterion) for sulfur at 180.73 nm were 0.13 and 1.28 ng ml -1 for the generation of hydrogen sulfide and sulfur dioxide, respectively, with the corresponding background equivalent concentrations of 20.9 and 62.2 ng ml -1 in sulfur concentration. The typical analytical working graphs obtained under the optimized experimental conditions were rectilinear over approximately four orders of magnitude in sulfur concentration. The present method has been successfully applied to the recovery test of the sulfide spiked to waste water samples and to the determination of sulfite in some samples of commercially available wine.

  13. INTERMEDIATE-RANGE GRID MODEL FOR ATMOSPHERIC SULFUR DIOXIDE AND SULFATE CONCENTRATIONS AND DEPOSITIONS

    EPA Science Inventory

    A three-dimensional time-dependent grid type model for two chemically reacting species which undergo atmospheric transport, diffusion and wet and dry deposition over a region of several hundred km is presented. Accuracy and sensitivity of the model are discussed. The model is app...

  14. 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.

  15. 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

  16. 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

  17. Estimation of atmospheric mixing layer height from radiosonde data

    NASA Astrophysics Data System (ADS)

    Wang, X. Y.; Wang, K. C.

    2014-06-01

    Mixing layer height (h) is an important parameter for understanding the transport process in the troposphere, air pollution, weather and climate change. Many methods have been proposed to determine h by identifying the turning point of the radiosonde profile. However, substantial differences have been observed in the existing methods (e.g. the potential temperature (θ), relative humidity (RH), specific humidity (q) and atmospheric refractivity (N) methods). These differences are associated with the inconsistency of the temperature and humidity profiles in a boundary layer that is not well mixed, the changing measurability of the specific humidity and refractivity with height, the measurement error of humidity instruments within clouds, and the general existence of clouds. This study proposes a method to integrate the information of temperature, humidity and cloud to generate a consistent estimate of h. We apply this method to high vertical resolution (~ 30 m) radiosonde data that were collected at 79 stations over North America during the period from 1998 to 2008. The data are obtained from the Stratospheric Processes and their Role in Climate Data Center (SPARC). The results show good agreement with those from N method as the information of temperature and humidity contained in N; however, cloud effects that are included in our method increased the reliability of our estimated h. From 1988 to 2008, the climatological h over North America was 1675 ± 303 m with a strong east-west gradient: higher values (generally greater than 1800 m) occurred over the Midwest US, and lower values (usually less than 1400 m) occurred over Alaska and the US West Coast.

  18. 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

  19. 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

  20. 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

  1. Estimates of Ground Temperature and Atmospheric Moisture from CERES Observations

    NASA Technical Reports Server (NTRS)

    Wu, Man Li C.; Schubert, Siegfried; Einaudi, Franco (Technical Monitor)

    2000-01-01

    A method is developed to retrieve surface ground temperature (Tg) and atmospheric moisture using clear sky fluxes (CSF) from CERES-TRMM observations. In general, the clear sky outgoing long-wave radiation (CLR) is sensitive to upper level moisture (q(sub h)) over wet regions and Tg over dry regions The clear sky window flux from 800 to 1200 /cm (RadWn) is sensitive to low level moisture (q(sub j)) and Tg. Combining these two measurements (CLR and RadWn), Tg and q(sub h) can be estimated over land, while q(sub h) and q(sub t) can be estimated over the oceans. The approach capitalizes on the availability of satellite estimates of CLR and RadWn and other auxiliary satellite data. The basic methodology employs off-line forward radiative transfer calculations to generate synthetic CSF data from two different global 4-dimensional data assimilation products. Simple linear regression is used to relate discrepancies in CSF to discrepancies in Tg, q(sub h) and q(sub t). The slopes of the regression lines define sensitivity parameters that can be exploited to help interpret mismatches between satellite observations and model-based estimates of CSF. For illustration, we analyze the discrepancies in the CSF between an early implementation of the Goddard Earth Observing System Data Assimilation System (GEOS-DAS) and a recent operational version of the European Center for Medium-Range Weather Prediction data assimilation system. In particular, our analysis of synthetic total and window region SCF differences (computed from two different assimilated data sets) shows that simple linear regression employing (Delta)Tg and broad layer (Delta)q(sub l) from 500 hPa to surface and (Delta)q(sub h) from 200 to 500 hPa provides a good approximation to the full radiative transfer calculations, typically explaining more than 90% of the 6-hourly variance in the flux differences. These simple regression relations can be inverted to "retrieve" the errors in the geophysical parameters

  2. Estimates of Ground Temperature and Atmospheric Moisture from CERES Observations

    NASA Technical Reports Server (NTRS)

    Wu, Man Li C.; Schubert, Siegfried; Einaudi, Franco (Technical Monitor)

    2000-01-01

    A method is developed to retrieve surface ground temperature (T(sub g)) and atmospheric moisture using clear sky fluxes (CSF) from CERES-TRMM observations. In general, the clear sky outgoing longwave radiation (CLR) is sensitive to upper level moisture (q(sub l)) over wet regions and (T(sub g)) over dry regions The clear sky window flux from 800 to 1200/cm (RadWn) is sensitive to low level moisture (q(sub t)) and T(sub g). Combining these two measurements (CLR and RadWn), Tg and q(sub h) can be estimated over land, while q(sub h) and q(sub l) can be estimated over the oceans. The approach capitalizes on the availability of satellite estimates of CLR and RadWn and other auxiliary satellite data. The basic methodology employs off-line forward radiative transfer calculations to generate synthetic CSF data from two different global 4-dimensional data assimilation products. Simple linear regression is used to relate discrepancies in CSF to discrepancies in T(sub g), q(sub h) and q(sub l). The slopes of the regression lines define sensitivity parameters that can be exploited to help interpret mismatches between satellite observations and model-based estimates of CSF. For illustration, we analyze the discrepancies in the CSF between an early implementation of the Goddard Earth Observing System Data Assimilation System (GEOS-DAS) and a recent operational version of the European Center for Medium-Range Weather Prediction data assimilation system. In particular, our analysis of synthetic total and window region SCF differences (computed from two different assimilated data sets) shows that simple linear regression employing Delta(T(sub g)) and broad layer Delta(q(sub l) from .500 hPa to surface and Delta(q(sub h)) from 200 to .300 hPa provides a good approximation to the full radiative transfer calculations. typically explaining more than 90% of the 6-hourly variance in the flux differences. These simple regression relations can be inverted to "retrieve" the errors in the

  3. Estimates of atmospheric O2 in the Paleoproterozoic from paleosols

    NASA Astrophysics Data System (ADS)

    Kanzaki, Yoshiki; Murakami, Takashi

    2016-02-01

    A weathering model was developed to constrain the partial pressure of atmospheric O2 (PO2) in the Paleoproterozoic from the Fe records in paleosols. The model describes the Fe behavior in a weathering profile by dissolution/precipitation of Fe-bearing minerals, oxidation of dissolved Fe(II) to Fe(III) by oxygen and transport of dissolved Fe by water flow, in steady state. The model calculates the ratio of the precipitated Fe(III)-(oxyhydr)oxides from the dissolved Fe(II) to the dissolved Fe(II) during weathering (ϕ), as a function of PO2 . An advanced kinetic expression for Fe(II) oxidation by O2 was introduced into the model from the literature to calculate accurate ϕ-PO2 relationships. The model's validity is supported by the consistency of the calculated ϕ-PO2 relationships with those in the literature. The model can calculate PO2 for a given paleosol, once a ϕ value and values of the other parameters relevant to weathering, namely, pH of porewater, partial pressure of carbon dioxide (PCO2), water flow, temperature and O2 diffusion into soil, are obtained for the paleosol. The above weathering-relevant parameters were scrutinized for individual Paleoproterozoic paleosols. The values of ϕ, temperature, pH and PCO2 were obtained from the literature on the Paleoproterozoic paleosols. The parameter value of water flow was constrained for each paleosol from the mass balance of Si between water and rock phases and the relationships between water saturation ratio and hydraulic conductivity. The parameter value of O2 diffusion into soil was calculated for each paleosol based on the equation for soil O2 concentration with the O2 transport parameters in the literature. Then, we conducted comprehensive PO2 calculations for individual Paleoproterozoic paleosols which reflect all uncertainties in the weathering-relevant parameters. Consequently, robust estimates of PO2 in the Paleoproterozoic were obtained: 10-7.1-10-5.4 atm at ∼2.46 Ga, 10-5.0-10-2.5 atm at ∼2

  4. Estimation of atmospheric mixing layer height from radiosonde data

    NASA Astrophysics Data System (ADS)

    Wang, X. Y.; Wang, K. C.

    2014-02-01

    Mixing layer height (h) is an important parameter for understanding the transport process in the troposphere, air pollution, weather and climate change. Many methods have been proposed to determine h by identifying the turning point of the radiosonde profile. However, substantial differences have been observed in the existing methods (e.g., the potential temperature (θ), relative humidity (RH), specific humidity (q) and atmospheric refractivity (N) methods). These differences are associated with the inconsistency of the temperature and humidity profiles in a boundary layer that is not well mixed, the changing measurability of the specific humidity and refractivity with height, the measurement error of humidity instruments within clouds, and the general existence of clouds. This study proposes a method to integrate the information of temperature, humidity and cloud to generate a consistent estimate of h. We apply this method to high vertical resolution (~ 30 m) radiosonde data that were collected at 79 stations over North America during the period from 1998 to 2008; the data are obtained from the Stratospheric Processes and their Role in Climate Data Center (SPARC). The results show good agreement with those from N method as the information of temperature and humidity contained in N; however cloud effects that are included in our method increased the reliability of h. Furthermore, our results agree well with the independent h that was determined from lidar observations. From 1988 to 2008, the climatological h over North America was 1675± 303 m with a strong east-west gradient: higher values (generally greater than 1800 m) occurred over the Midwest US, and lower values (usually less than 1400 m) occurred over Alaska and the US west coast.

  5. Comparison of emissions estimates derived from atmospheric measurements with national estimates of HFCs, PFCs and SF6.

    PubMed

    Harnisch, Jochen; Höhne, Niklas

    2002-01-01

    This paper assesses the feasibility of using atmospheric measurement of fluorinated greenhouse gases (HFCs, PFCs and SF6) for the review and verification of greenhouse gas inventories provided by national governments. For this purpose, available data were compiled. It was found that atmospheric measurements of these gases are available and provide an indication of global annual emissions with sufficient certainty to reach the following conclusions: Within the uncertainty of the method, it was found that emissions of HFC-23, a by-product of HCFC-22 production, as obtained from atmospheric measurements did not decrease as fast, as the countries have reported. In contrast, SF6 concentrations in the atmosphere suggest higher emissions than reported by countries. Regional emission estimates from atmospheric measurements are still in a more pioneering state and cannot be compared to national estimates. Intensified efforts to measure HFCs, PFCs and SF6 in the atmosphere are recommended. PMID:12391806

  6. 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.

  7. Streamwater acid-base chemistry and critical loads of atmospheric sulfur deposition in Shenandoah National Park, Virginia.

    PubMed

    Sullivan, T J; Cosby, B J; Webb, J R; Dennis, R L; Bulger, A J; Deviney, F A

    2008-02-01

    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 neutralizing capacity (ANC) less than 20 microeq/L, levels at which chronic and/or episodic adverse impacts on native brook trout are possible. Model hindcasts suggested that none of these streams had ANC less than 50 microeq/L in 1900. Model projections, based on atmospheric emissions controls representative of laws already enacted as of 2003, suggested that the ANC of those streams simulated to have experienced the largest historical decreases in ANC will increase in the future. The levels of S deposition that were simulated to cause streamwater ANC to increase or decrease to three specified critical levels (0, 20, and 50 microeq/L) ranged from less than zero (ANC level not attainable) to several hundred kg/ha/year, depending on the selected site and its inherent acid-sensitivity, selected ANC endpoint criterion, and evaluation year for which the critical load was calculated. Several of the modeled streams situated on siliciclastic geology exhibited critical loads <0 kg/ha/year to achieve ANC >50 microeq/L in the year 2040, probably due at least in part to base cation losses from watershed soil. The median modeled siliciclastic stream had a calculated critical load to achieve ANC >50 microeq/L in 2100 that was about 3 kg/ha/year, or 77% lower than deposition in 1990, representing the time of model calibration. PMID:17492359

  8. Atmospheric SO2 emissions since the late 1800s change organic sulfur forms in humic substance extracts of soils.

    PubMed

    Lehmann, Johannes; Solomon, Dawit; Zhao, Fang-Jie; McGrath, Steve P

    2008-05-15

    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 extracts-reverting 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. PMID:18546688

  9. 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.

  10. 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.

  11. Vertical Distributions of Sulfur Species Simulated by Large Scale Atmospheric Models in COSAM: Comparison with Observations

    SciTech Connect

    Lohmann, U.; Leaitch, W. R.; Barrie, Leonard A.; Law, K.; Yi, Y.; Bergmann, D.; Bridgeman, C.; Chin, M.; Christensen, J.; Easter, Richard C.; Feichter, J.; Jeuken, A.; Kjellstrom, E.; Koch, D.; Land, C.; Rasch, P.; Roelofs, G.-J.

    2001-11-01

    A comparison of large-scale models simulating atmospheric sulfate aerosols (COSAM) was conducted to increase our understanding of global distributions of sulfate aerosols and precursors. Earlier model comparisons focused on wet deposition measurements and sulfate aerosol concentrations in source regions at the surface. They found that different models simulated the observed sulfate surface concentrations mostly within a factor of two, but that the simulated column burdens and vertical profiles were very different amongst different models. In the COSAM exercise, one aspect is the comparison of sulfate aerosol and precursor gases above the surface. Vertical profiles of SO2, SO42-, oxidants and cloud properties were measured by aircraft during the North Atlantic Regional Experiment (NARE) experiment in August/September 1993 off the coast of Nova Scotia and during the Second Eulerian Model Evaluation Field Study (EMEFSII) in central Ontario in March/April 1990. While no single model stands out as being best or worst, the general tendency is that those models simulating the full oxidant chemistry tend to agree best with observations although differences in transport and treatment of clouds are important as well.

  12. Modification of the method of parametric estimation of atmospheric distortion in MODTRAN model

    NASA Astrophysics Data System (ADS)

    Belov, A. M.

    2015-12-01

    The paper presents a modification of the method of parametric estimation of atmospheric distortion in MODTRAN model as well as experimental research of the method. The experimental research showed that the base method does not take into account physical meaning of atmospheric spherical albedo parameter and presence of outliers in source data that results to overall atmospheric correction accuracy decreasing. Proposed modification improves the accuracy of atmospheric correction in comparison with the base method. The modification consists in the addition of nonnegativity constraint on the atmospheric spherical albedo estimated value and the addition of preprocessing stage aimed to adjust source data.

  13. 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.

  14. NITROGEN BOUNDING STUDY: METHODS FOR ESTIMATING THE RELATIVE EFFECTS OF SULFUR AND NITROGEN DEPOSITION ON SURFACE WATER CHEMISTRY

    EPA Science Inventory

    The leaching of atmospherically deposited nitrogen from forested watersheds may acidify lakes and streams. he Nitrogen Bounding Study evaluates the potential range of such adverse effects. he study estimates bounds on changes in regional-scale surface water acidification that mig...

  15. 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

  16. Satellite Estimates of Precipitation-Induced Dissipation in the Atmosphere

    NASA Astrophysics Data System (ADS)

    Pauluis, Olivier; Dias, Juliana

    2012-02-01

    A substantial amount of frictional dissipation in the atmosphere occurs in the microphysical shear zones surrounding falling precipitation. The dissipation rate is computed here from recently available satellite retrieval from the Tropical Rainfall Measurement Missions and is found to average 1.8 watts per square meter between 30°S and 30°N. The geographical distribution of the precipitation-induced dissipation is closely tied to that of precipitation but also reveals a stronger dissipation rate for continental convection than for maritime convection. Because the precipitation-induced dissipation is of the same magnitude as the turbulent dissipation of the kinetic energy in the atmosphere, changes in the hydrological cycle could potentially have a direct impact on the amount of kinetic energy generated and dissipated by the atmospheric circulation.

  17. 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.

  18. Estimate of the 42Ar content in the Earth's atmosphere

    NASA Astrophysics Data System (ADS)

    Barabash, A. S.; Kornoukhov, V. N.; Jants, V. E.

    1997-02-01

    42Ar is a potential source of background in large volume argon-based detectors. The production of the 42Ar isotope both by cosmic rays and by neutrons produced by testing of nuclear weapons is discussed. We demonstrate that main channel of the 42Ar production is from atmospheric testing of nuclear bombs from 1945 to 1962 and the 42Ar content must be less than 1.3 × 10 -23 parts of 42Ar per part of natAr.

  19. 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.

  20. 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.

  1. 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

  2. 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

  3. 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.

  4. 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.

  5. Laboratory Measurments 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.; Barisich, C.

    2012-10-01

    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. Since the emission morphology is related both to surface features and to deep atmospheric absorption from CO2 and SO2 (see, e.g., Butler et al., Icarus 154, 2001), 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 et al., JGR 71, 1966), no measurements of the centimeter-wavelength properties of any Venus atmospheric constituent have been conducted under conditions characteristic of the deep atmosphere (pressures from 10-92 Bars and temperatures from 400-700 K). New measurements of the microwave properties of SO2 and CO2 at wavelengths from 3.7-20 cm are now being conducted under simulated conditions for the deep atmosphere of Venus, using a new high-pressure system. Initial results from this measurement campaign conducted at 430 K and at pressures up to 92 Bars will be presented. This work is supported by the NASA Planetary Atmospheres Program under Grant NNX11AD66G.

  6. 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.

  7. 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...

  8. 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

    2015-04-01

    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. PMID:25734883

  9. 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.

  10. 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.

  11. 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

  12. Measuring OH Reaction Rate Constants and Estimating the Atmospheric Lifetimes of Trace Gases.

    NASA Astrophysics Data System (ADS)

    Orkin, Vladimir; Kurylo, Michael

    2015-04-01

    Reactions with hydroxyl radicals and photolysis are the main processes dictating a compound's residence time in the atmosphere for a majority of trace gases. In case of very short-lived halocarbons their reaction with OH dictates both the atmospheric lifetime and active halogen release. Therefore, the accuracy of OH kinetic data is of primary importance for the comprehensive modeling of a compound's impact on the atmosphere, such as in ozone depletion (i.e., the Ozone Depletion Potential, ODP) and climate change (i.e., the Global Warming Potential, GWP), each of which are dependent on the atmospheric lifetime of the compound. We have demonstrated the ability to conduct very high accuracy determinations of OH reaction rate constants over the temperature range of atmospheric interest, thereby decreasing the uncertainty of kinetic data to 2-3%. The atmospheric lifetime of a well-mixed compound due to its reaction with tropospheric hydroxyl radicals can be estimated by using a simple scaling procedure that is based on the results of field observations of methyl chloroform concentrations and detailed modeling of the OH distribution in the atmosphere. The currently available modeling results of the atmospheric fate of various trace gases allow for an improved understanding of the ability and accuracy of simplified semi-empirical estimations of atmospheric lifetimes. These aspects will be illustrated in this presentation for a variety of atmospheric trace gases.

  13. Measuring OH Reaction Rate Constants and Estimating the Atmospheric Lifetimes of Trace Gases.

    NASA Astrophysics Data System (ADS)

    Orkin, V. L.; Kurylo, M. J., III

    2014-12-01

    Reactions with hydroxyl radicals and photolysis are the main processes dictating a compound's residence time in the atmosphere for a majority of trace gases. In case of very short-lived halocarbons their reaction with OH dictates both the atmospheric lifetime and active halogen release. Therefore, the accuracy of OH kinetic data is of primary importance for the comprehensive modeling of a compound's impact on the atmosphere, such as in ozone depletion (i.e., the Ozone Depletion Potential, ODP) and climate change (i.e., the Global Warming Potential, GWP), each of which are dependent on the atmospheric lifetime of the compound. We have demonstrated the ability to conduct very high accuracy determinations of OH reaction rate constants over the temperature range of atmospheric interest, thereby decreasing the uncertainty of kinetic data to 2-3%. The atmospheric lifetime of a tropospherically well-mixed compound due to its reaction with tropospheric hydroxyl radicals can be estimated by using a simple scaling procedure that is based on the results of field observations of methyl chloroform concentrations and detailed modeling of the OH distribution in the atmosphere. The currently available modeling results of the atmospheric fate of various trace gases allow for an improved understanding of the ability and accuracy of simplified semi-empirical estimations of atmospheric lifetimes. These aspects will be illustrated in this presentation for a variety of atmospheric trace gases.

  14. Protocol for estimating historic atmospheric mercury deposition. Final report

    SciTech Connect

    1996-08-01

    The varied chemical phases and forms of mercury promote its transport and cycling in the environment between water, soil, and air. Many sources--both natural and anthropogenic--contribute to the atmospheric mercury cycle, while several factors modify its deposition and subsequent transformation, distribution, and bioaccumulation. This report introduces a protocol for quantifying spatial and temporal mercury deposition and improving site-to-site comparability of mercury accumulation measurements in natural archives. The report describes the selection of appropriate coring sites to measure mercury accumulation, field methods for lake sediment coring, analysis of sediments, and interpretation of the results from stratigraphic mercury analyses. The new EPRI protocol is expected not only to spur research methods but also to facilitate the global picture of historic mercury deposition needed by policymakers in public organizations, industry, and government.

  15. 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.

  16. 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. PMID:23506443

  17. Regional earth-atmosphere energy balance estimates based on assimilations with a GCM

    NASA Technical Reports Server (NTRS)

    Alexander, Michael A.; Schubert, Siegfried D.

    1990-01-01

    The Oort and Vonder Haar (1976) column-budget technique is presently used to evaluate the physical consistency and accuracy of regional earth-atmosphere energy balance estimates for (1) atmospheric budget terms, (2) net radiation at the top of the atmosphere, and (3) time tendency and flux divergence of energy, for Special Observing Periods of the FGGE year. It is found that, during winter, the midlatitude oceans supply large quantities of energy to the overlying atmosphere, which then transports the energy to the continental heat-sinks; the energy flows in the opposite direction during summer.

  18. 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;…

  19. Approaches for Improved Doppler Estimation in Lidar Remote Sensing of Atmospheric Dynamics

    NASA Astrophysics Data System (ADS)

    Bhaskaran, Sreevatsan; Calhoun, Ronald

    2016-06-01

    Laser radar (Lidar) has been used extensively for remote sensing of wind patterns, turbulence in the atmospheric boundary layer and other important atmospheric transport phenomenon. As in most narrowband radar application, radial velocity of remote objects is encoded in the Doppler shift of the backscattered signal relative to the transmitted signal. In contrast to many applications, however, the backscattered signal in atmospheric Lidar sensing arises from a multitude of moving particles in a spatial cell under examination rather than from a few prominent "target" scattering features. This complicates the process of extracting a single Doppler value and corresponding radial velocity figure to associate with the cell. This paper summarizes the prevalent methods for Doppler estimation in atmospheric Lidar applications and proposes a computationally efficient scheme for improving Doppler estimation by exploiting the local structure of spectral density estimates near spectral peaks.

  20. 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.

  1. 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.

  2. 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.

  3. Development of local atmospheric model for estimating solar irradiance in Peninsular Malaysia

    NASA Astrophysics Data System (ADS)

    Yeap, E. C.; Lau, A. M. S.; Busu, I.; Kanniah, K. D.; Rasib, A. W.; Kadir, W. H. W.

    2014-02-01

    Incoming solar irradiance covers a wide range of wavelengths with different intensities which drives almost every biological and physical cycle on earth at a selective wavelength. Estimation of the intensities of each wavelength for the solar irradiance on the earth surface provides a better way to understand and predict the radiance energy. It requires that the atmospheric and geometric input and the availability of atmospheric parameter is always the main concern in estimating solar irradiance. In this study, a local static atmospheric model for Peninsular Malaysia was built to provide the atmospheric parameters in the estimation of solar irradiance. Ten years of monthly Atmospheric Infrared Sounder (AIRS) average data (water vapor, temperature, humidity and pressure profile) of the Peninsular Malaysia was used for the building of the atmospheric model and the atmospheric model were assessed based on the measured meteorological data with RMSE of 4.7% and 0.7k for both humidity and temperature respectively. The atmospheric model were applied on a well-established radiative transfer model namely SMARTS2. Some modifications are required in order to include the atmospheric model into the radiative transfer model. The solar irradiance results were then assessed with measured irradiance data and the results show that both the radiative transfer model and atmospheric model were reliable with RMSE value of 0.5 Wm-2. The atmospheric model was further validated based on the measured meteorological data (temperature and humidity) provided by the Department of Meteorology, Malaysia and high coefficient of determination with R2 value of 0.99 (RMSE value = 4.7%) and 0.90 (RMSE value = 0.7k) were found for both temperature and humidity respectively.

  4. Atmospheric H2S and SO2 as sulfur source for Brassica juncea and Brassica rapa: impact on the glucosinolate composition

    PubMed Central

    Aghajanzadeh, Tahereh; Kopriva, Stanislav; Hawkesford, Malcolm J.; Koprivova, Anna; De Kok, Luit J.

    2015-01-01

    The impact of sulfate deprivation and atmospheric H2S and SO2 nutrition on the content and composition of glucosinolates was studied in Brassica juncea and B. rapa. Both species contained a number of aliphatic, aromatic and indolic glucosinolates. The total glucosinolate content was more than 5.5-fold higher in B. juncea than in B. rapa, which could solely be attributed to the presence of high levels of sinigrin, which was absent in the latter species. Sulfate deprivation resulted in a strong decrease in the content and an altered composition of the glucosinolates of both species. Despite the differences in patterns in foliarly uptake and metabolism, their exposure hardly affected the glucosinolate composition of the shoot, both at sulfate-sufficient and sulfate-deprived conditions. This indicated that the glucosinolate composition in the shoot was hardly affected by differences in sulfur source (viz., sulfate, sulfite and sulfide). Upon sulfate deprivation, where foliarly absorbed H2S and SO2 were the sole sulfur source for growth, the glucosinolate composition of roots differed from sulfate-sufficient B. juncea and B. rapa, notably the fraction of the indolic glucosinolates was lower than that observed in sulfur-sufficient roots. PMID:26579170

  5. 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 ...

  6. 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

  7. Sulfur and phosphorus distribution between liquid iron and magnesia-saturated slag in molecular hydrogen/water atmosphere relevant to a novel green ironmaking technology

    NASA Astrophysics Data System (ADS)

    Mohassab Ahmed, Mohassab Yousef

    As an integral part of a research project which aimed to develop a novel green ironmaking process, an experimental determination of the sulfur and phosphorus distribution ratios, LS and LP, respectively, between molten iron and CaO-MgO(Saturated)-SiO2-Al 3O3-FeO slag was determined in the temperature range 1550-1650°C. Oxygen partial pressure was controlled by H2/H2O equilibrium in the range of 10-10-10-8 atm. For sulfur distribution, it was found that the trend of the distribution is the same as the previous work done under CO/CO2 atmosphere but LS in this case is 38-44 times less under similar oxygen partial pressure. This might be attributed to the impact of H2 on the distribution. Considering the fact that the input sulfur in the proposed process is approximately 34 times less than the blast furnace process, the proposed process would produce hot metal with approximately the same sulfur content to the hot metal produced by the blast furnace. For phosphorus distribution, LP was 450-1050 times that of the blast furnace. Also considering the amount of phosphorus input in the two processes, it was found that the expected P content in iron in the new process would be approximately three times less than in the blast furnace hot metal. This means that the proposed process will produce hot metal with much lower phosphorus which will minimize the need for dephosphorization in the steelmaking stage.

  8. 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.

  9. Models for the Centimeter-Wavelength Opacity of Sulfur Dioxide and Carbon Dioxide based on Laboratory Measurements Conducted under Simulated Conditions for the Deep Atmosphere of Venus

    NASA Astrophysics Data System (ADS)

    Steffes, Paul G.; Shahan, P. M.

    2013-10-01

    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. Since the emission morphology is related both to surface features and to deep atmospheric absorption from CO2 and SO2 (see, e.g., Butler et al., Icarus 154, 2001), 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. Initial measurements of the centimeter-wavelength (3.7-20 cm) of SO2 and CO2 under simulated conditions for the deep atmosphere of Venus, conducted using a new high-pressure system operating at 430 K and at pressures up to 92 Bars, were presented by Steffes and Barisich (DPS-2012, B.A.A.S., v.44, p.241). Over the past year, we have completed this measurement campaign for temperatures up to 550 K, so as to better understand the effects of SO2 and CO2 on the microwave emission from the Venus boundary layer. Results indicate that the model for the centimeter-wavelength opacity from pure CO2 (developed over 40 years ago -- Ho et al., JGR 71, 1966), is valid over the entire centimeter-wavelength range under simulated conditions for the deep atmosphere of Venus. Additionally, the laboratory results indicate that the model for the centimeter-wavelength opacity of SO2 in a CO2 atmosphere from Suleiman et al. (JGR-Planets, 101, Feb. 1996) can reliably be used under conditions of the deep atmosphere of Venus with the modifications described in this paper . This work is supported by the NASA Planetary Atmospheres Program under Grant NNX11AD66G.

  10. The formation of acid rain in the atmosphere, adjacent to the TTP with the joint-condensing of sulfur dioxide and water vapor

    NASA Astrophysics Data System (ADS)

    Gvozdyakov, D. V.; Gubin, V. E.; Matveeva, A. A.

    2014-08-01

    Presents the results of mathematical simulation of the condensation process of sulphur dioxide and water vapor on the condensation nuclei surface under the action of natural factors. Numerical investigations were carried out for the summer at a moderate speed of the wind. The influence of the parameter of condensation on the speed of the process of sulfuric acid drops formation in the air space was analyzed. Time ranges, sufficient for the formation of the acid rain sedimentation in the atmosphere, adjacent to the areas of thermal power station work were established. It is shown that the speed of air masses movement effects on the process of acid anthropogenic admixtures dispersion in the atmosphere. Approbation of the obtained results was carried out by checking the difference scheme conservative and solution of test problems.

  11. 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.

  12. 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.

  13. Sulfur and Sulfuric Acid

    NASA Astrophysics Data System (ADS)

    D'Aquin, Gerard E.; Fell, Robert C.

    Sulfur is one of the few elements that is found in its elemental form in nature. Typical sulfur deposits occur in sedimentary limestone/gypsum formations, in limestone/anhydrite formations associated with salt domes, or in volcanic rock.1 A yellow solid at normal temperatures, sulfur becomes progressively lighter in color at lower temperatures and is almost white at the temperature of liquid air. It melts at 114-119°C (depending on crystalline form) to a transparent light yellow liquid as the temperature is increased. The low viscosity of the liquid begins to rise sharply above 160°C, peaking at 93 Pa·s at 188°C, and then falling as the temperature continues to rise to its boiling point of 445°C. This and other anomalous properties of the liquid state are due to equilibria between the various molecular species of sulfur, which includes small chains and rings.

  14. 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.

  15. 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. PMID:11489528

  16. Dependence of Mercurian Atmospheric Column Abundance Estimations on Surface-Reflectance Modeling

    NASA Technical Reports Server (NTRS)

    Domingue, Deborah L.; Sprague, Ann L.; Hunten, Donald M.

    1997-01-01

    Column abundance estimates of sodium, and analogously, potassium, in Mercury's exosphere are strongly correlated to the surface reflection model used to calibrate the spectral data and the surface reflection model incorporated into the atmospheric radiative transfer solution. Depending on the surface reflection model parameters used, there can be differences in calibration factors of up to +/- 30% and differences in estimated column abundance of up to +/- 35%. Although the surface reflectance may not be used in the calibration of spacecraft measurements, the interaction between the reflected surface light and the atmospheric brightness remains important.

  17. MECHANISM AND RATES OF THE GAS PHASE OXIDATIONS OF SULFUR DIOXIDE AND THE NITROGEN OXIDES IN THE ATMOSPHERE

    EPA Science Inventory

    As our knowledge of the atmospheric chemistry of the SO2, NO, and NO2 continues to grow, it becomes increasingly clear that many different chemical reactions contribute to the oxidation of these oxides in the atmosphere. Solution phase and gas phase chemistry are both important t...

  18. 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

    ... requirements of section 7 of 40 CFR part 58, appendix E (Teflon ® or glass with residence time less than 20 sec... at the sample manifold, with the excess flow vented at atmospheric pressure. The absorbers are then... Anomalous Behavior in Tetrachloromercurate (II). Submitted for publication in Atmospheric Environment,...

  19. Estimates of changes in the rate of methane sink from the atmosphere under climate warming

    NASA Astrophysics Data System (ADS)

    Dzyuba, A. V.; Eliseev, A. V.; Mokhov, I. I.

    2012-05-01

    The temperature dependence of the methane oxidation rate is estimated. The methane lifetime in the atmosphere is shown to decrease by about 3% from 1900 to 2005. The overwhelming fraction of the total methane content is removed from the atmosphere at intratropical latitudes during the daytime. The methane oxidation rate growth due to the temperature increase in the troposphere generates negative feedback in the methane cycle and, accordingly, climatic feedback with the same sign. According to the estimates performed, the halt in methane concentration growth in the atmosphere observed in recent years can be associated with a decrease in the lifetime of methane in the atmosphere. According to the results of numerical experiments with the climatic model of the Institute of Atmospheric Physics, Russian Academy of Sciences (IAP RAS), the climatic effect of negative feedback of the tropospheric temperature and the methane lifetime in the atmosphere is not large and is comparable with the climatic forcing of the methane emission growth from bog ecosystems.

  20. The Boston Methane Project: Mapping Surface Emissions to Inform Atmospheric Estimation of Urban Methane Flux

    NASA Astrophysics Data System (ADS)

    Phillips, N.; Crosson, E.; Down, A.; Hutyra, L.; Jackson, R. B.; McKain, K.; Rella, C.; Raciti, S. M.; Wofsy, S. C.

    2012-12-01

    Lost and unaccounted natural gas can amount to over 6% of Massachusetts' total annual greenhouse gas inventory (expressed as equivalent CO2 tonnage). An unknown portion of this loss is due to natural gas leaks in pipeline distribution systems. The objective of the Boston Methane Project is to estimate the overall leak rate from natural gas systems in metropolitan Boston, and to compare this flux with fluxes from the other primary methane emissions sources. Companion talks at this meeting describe the atmospheric measurement and modeling framework, and chemical and isotopic tracers that can partition total atmospheric methane flux into natural gas and non-natural gas components. This talk focuses on estimation of surface emissions that inform the atmospheric modeling and partitioning. These surface emissions include over 3,300 pipeline natural gas leaks in Boston. For the state of Massachusetts as a whole, the amount of natural gas reported as lost and unaccounted for by utility companies was greater than estimated landfill emissions by an order of magnitude. Moreover, these landfill emissions were overwhelmingly located outside of metro Boston, while gas leaks are concentrated in exactly the opposite pattern, increasing from suburban Boston toward the urban core. Work is in progress to estimate spatial distribution of methane emissions from wetlands and sewer systems. We conclude with a description of how these spatial data sets will be combined and represented for application in atmospheric modeling.

  1. 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.

  2. 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

  3. 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

  4. 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

  5. Atmospheric water balance over oceanic regions as estimated from satellite, merged, and reanalysis data

    NASA Astrophysics Data System (ADS)

    Park, Hyo-Jin; Shin, Dong-Bin; Yoo, Jung-Moon

    2013-05-01

    The column integrated atmospheric water balance over the ocean was examined using satellite-based and merged data sets for the period from 2000 to 2005. The data sets for the components of the atmospheric water balance include evaporation from the HOAPS, GSSTF, and OAFlux and precipitation from the HOAPS, CMAP, and GPCP. The water vapor tendency was derived from water vapor data of HOAPS. The product for water vapor flux convergence estimated using satellite observation data was used. The atmospheric balance components from the MERRA reanalysis data were also examined. Residuals of the atmospheric water balance equation were estimated using nine possible combinations of the data sets over the ocean between 60°N and 60°S. The results showed that there was considerable disagreement in the residual intensities and distributions from the different combinations of the data sets. In particular, the residuals in the estimations of the satellite-based atmospheric budget appear to be large over the oceanic areas with heavy precipitation such as the intertropical convergence zone, South Pacific convergence zone, and monsoon regions. The lack of closure of the atmospheric water cycle may be attributed to the uncertainties in the data sets and approximations in the atmospheric water balance equation. Meanwhile, the anomalies of the residuals from the nine combinations of the data sets are in good agreement with their variability patterns. These results suggest that significant consideration is needed when applying the data sets of water budget components to quantitative water budget studies, while climate variability analysis based on the residuals may produce similar results.

  6. 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

  7. 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

    2015-01-01

    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

  8. A simplified method to estimate atmospheric water vapor using MODIS near-infrared data

    NASA Astrophysics Data System (ADS)

    Wang, Xinming; Gu, Xiaoping; Wu, Zhanping

    2016-03-01

    Atmospheric water vapor plays a significant role in the study of climate change and hydrological cycle processes. In order to acquire the accurate distribution of atmospheric water vapor which is varying with time, location, and altitude, it is necessary to monitor it at high spatial and temporal resolution. Unfortunately, it is difficult to map the spatial distribution of atmospheric water vapor due to the lack of meteorological instrumentation at adequate spatial and temporal observation scales. This paper introduces a simplified method to retrieve Precipitable Water Vapor (PWV) using the ratio of the apparent reflectance values of the 18th and 19th band of Moderate Resolution Imaging Spectroradiometer (MODIS). Compared to the EOS PWV products of the same time and area, the PWV estimated using this simplified method is closer to the radiosonde results which is considered as the true PWV value. Results reveal that this simplified method is applicable over cloud-free atmospheric conditions of the mid-latitude regions.

  9. 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.

  10. A new tracer experiment to estimate the methane emissions from a dairy cow shed using sulfur hexafluoride (SF6)

    NASA Astrophysics Data System (ADS)

    Marik, Thomas; Levin, Ingeborg

    1996-09-01

    Methane emission from livestock and agricultural wastes contribute globally more than 30% to the anthropogenic atmospheric methane source. Estimates of this number have been derived from respiration chamber experiments. We determined methane emission rates from a tracer experiment in a modern cow shed hosting 43 dairy cows in their accustomed environment. During a 24-hour period the concentrations of CH4, CO2, and SF6, a trace gas which has been released at a constant rate into the stable air, have been measured. The ratio between SF6 release rate and measured SF6 concentration was then used to estimate the ventilation rate of the stable air during the course of the experiment. The respective ratio between CH4 or CO2 and SF6 concentration together with the known SF6 release rate allows us to calculate the CH4 (and CO2) emissions in the stable. From our experiment we derive a total daily mean CH4 emission of 441 LSTP per cow (9 cows nonlactating), which is about 15% higher than previous estimates for German cows with comparable milk production obtained during respiration chamber experiments. The higher emission in our stable experiment is attributed to the contribution of CH4 release from about 50 m3 of liquid manure present in the cow shed in underground channels. Also, considering measurements we made directly on a liquid manure tank, we obtained an estimate of the total CH4 production from manure: The normalized contribution of methane from manure amounts to 12-30% of the direct methane release of a dairy cow during rumination. The total CH4 release per dairy cow, including manure, is 521-530 LSTP CH4 per day.