WorldWideScience

Sample records for volcanic sulfate aerosol

  1. Transient Sulfate Aerosols as a Signature of Exoplanet Volcanism

    CERN Document Server

    Misra, Amit; Koehler, Matthew C; Sholes, Steven

    2015-01-01

    Geological activity is thought to be important for the origin of life and for maintaining planetary habitability. We show that transient sulfate aerosols could be a signature of exoplanet volcanism, and therefore a geologically active world. A detection of transient aerosols, if linked to volcanism, could thus aid in habitability evaluations of the exoplanet. On Earth, subduction-induced explosive eruptions inject SO2 directly into the stratosphere, leading to the formation of sulfate aerosols with lifetimes of months to years. We demonstrate that the rapid increase and gradual decrease in sulfate aerosol loading associated with these eruptions may be detectable in transit transmission spectra with future large-aperture telescopes, such as the James Webb Space Telescope (JWST) and European Extremely-Large Telescope (E-ELT) for a planetary system at a distance of 10 pc, assuming an Earth-like atmosphere, bulk composition, and size. Specifically, we find that a S/N of 12.1 and 7.1 could be achieved with E-ELT (...

  2. Small volcanic eruptions and the stratospheric sulfate aerosol burden

    Science.gov (United States)

    Pyle, David M.

    2012-09-01

    Understanding of volcanic activity and its impacts on the atmosphere has evolved in discrete steps, associated with defining eruptions. The eruption of Krakatau, Indonesia, in August 1883 was the first whose global reach was recorded through observations of atmospheric phenomena around the world (Symons 1888). The rapid equatorial spread of Krakatau's ash cloud revealed new details of atmospheric circulation, while the vivid twilights and other optical phenomena were soon causally linked to the effects of particles and gases released from the volcano (e.g. Stothers 1996, Schroder 1999, Hamilton 2012). Later, eruptions of Agung, Bali (1963), El Chichón, Mexico (1982) and Pinatubo, Philippines (1991) led to a fuller understanding of how volcanic SO2 is transformed to a long-lived stratospheric sulfate aerosol, and its consequences (e.g. Meinel and Meinel 1967, Rampino and Self 1982, Hoffman and Rosen 1983, Bekki and Pyle 1994, McCormick et al 1995). While our ability to track the dispersal of volcanic emissions has been transformed since Pinatubo, with the launch of fleets of Earth-observing satellites (e.g. NASA's A-Train; ESA's MetOp) and burgeoning networks of ground-based remote-sensing instruments (e.g. lidar and sun-photometers; infrasound and lightning detection systems), there have been relatively few significant eruptions. Thus, there have been limited opportunities to test emerging hypotheses including, for example, the vexed question of the role of 'smaller' explosive eruptions in perturbations of the atmosphere—those that may just be large enough to reach the stratosphere (of size 'VEI 3', Newhall and Self 1982, Pyle 2000). Geological evidence, from ice-cores and historical eruptions, suggests that small explosive volcanic eruptions with the potential to transport material into the stratosphere should be frequent (5-10 per decade), and responsible for a significant proportion of the long-term time-averaged flux of volcanic sulfur into the stratosphere

  3. Detection of volcanic sulfate aerosol with Envisat MIPAS shown for the Kasatochi, Sarychev, and Nabro eruptions

    Science.gov (United States)

    Griessbach, Sabine; Hoffmann, Lars; Spang, Reinhold; von Hobe, Marc; Müller, Rolf; Riese, Martin

    2013-04-01

    Stratospheric sulfate aerosol is known to have a strong impact on climate. Transport pathways of sulfur dioxide and sulfate aerosol to the stratosphere are still discussed. It is known that volcanic eruptions can inject significant amounts of sulfur directly into the stratosphere. Most sulfur, however, is injected into the troposphere and only a fraction of it can make its way into the stratosphere. Global and altitude resolved time series of observations are a valuable source of information for sulfur dioxide and sulfate aerosol detection. Here we present a new aerosol detection method for the infrared limb sounder Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the results for the Kasatochi, Sarychev, and Nabro eruptions. The new detection method utilizes three infrared window regions that are located around 830, 960, and 1224 cm-1. The combination of these three windows allows for a better detection of enhanced aerosol events in the troposphere as well as the discrimination from ice clouds. With this new method the 10 year record of MIPAS measurements was analyzed. The most remarkable sulfate aerosol events follow the Kasatochi, Sarychev, and Nabro eruptions. After these eruptions enhanced aerosol is detected in the upper troposphere and lower stratosphere (UTLS) region. Within one to two months it spreads over most of the northern hemisphere. In the tropics the aerosol reaches altitudes up to around 20 km and in the Arctic up to 15 km. The enhanced aerosol signal can be observed for about 5, 7, and up to 10 month for the Kasatochi, Sarychev, and Nabro eruptions, respectively. During this period the enhanced aerosol detections decrease in number, strength, and observation altitude. After the Nabro eruption on 13 June 2011 volcanic aerosol is detected in the UTLS region two days after the initial eruption. The following days the aerosol moves around the northern edge of the Asian monsoon region, is then transported southwards and later

  4. Fingerprinting Volcanic and Anthropogenic Sulfur Dioxide in the Air: A 25 Year Record of Sulfate Aerosols from the South Pole Snowpit, Antarctica

    Science.gov (United States)

    Shaheen, R.; Abaunza-Quintero, M.; Jackson, T. L.; McCabe, J.; Savarino, J. P.; Thiemens, M. H.

    2012-12-01

    Sulfate aerosols, unlike greenhouse gases, cause cooling effect (-0.4 ± 0.2 W.m-2) by scattering incoming solar radiation and by acting as cloud condensation nuclei (IPCC 2007). Volcanic eruptions with explosivity Indices >5 inject large amounts of SO2 and particles into the stratosphere causing a significant decrease in temperature. For example a 0.7oC decrease in Earth's temperature was observed following the Pinatubo eruption in 1991. Stratospheric injection of sulfate aerosols has been suggested as a geoengineering effort to mitigate global warming caused by a significant increase in greenhouse gases. To understand the impact of volcanic events on the stratospheric sulfate aerosol layer and subsequent changes in the dynamics of the upper atmosphere, a long term and high temporal resolution record of sulfate aerosol is needed. Here we present a 25 year (1978 to 2003) high resolution record of sulfate aerosols which covers largest volcanic eruptions of the 20th century namely, El-Chichón 1982 and Pinatubo 1991. Sulfate aerosol samples were obtained from a 1x1m snowpit at the South Pole, Antarctica with approximately 6 month time steps. Sulfate concentrations vary from 30 to 70 ppb depending on the season with exceptions during volcanic events which contributed a three to four folds increase in sulfate concentration Sulfate concentrations of120 ppb following El Chichón and 190 ppb after Pinatubo eruptions were observed. The oxygen isotopic anomaly varied from 0.7‰ to 3.9‰ with the highest anomaly occurring after the Pinatubo eruption. The positive Δ17O of sulfate derives from aqueous phase oxidation of SO2 by H2O2 and O3 oxidation and involves transfer of the isotopic anomaly from the oxidant to the product sulfate. Coupled with kinetic analysis the relative reaction rates the relative proportions of oxidation can be calculated. All other sulfate sources such as sea salt sulfates, primary sulfates from fossil fuel combustion, metal catalyzed oxidation of S

  5. Constraining the long-term climate reponse to stratospheric sulfate aerosols injection by the short-term volcanic climate response

    Science.gov (United States)

    Plazzotta, M.; Seferian, R.; Douville, H.; Kravitz, B.; Tilmes, S.; Tjiputra, J.

    2016-12-01

    Rising greenhouse gas emissions are leading to global warming and climate change, which will have multiple impacts on human society. Geoengineering methods like solar radiation management by stratospheric sulfate aerosols injection (SSA-SRM) aim at treating the symptoms of climate change by reducing the global temperature. Since a real-world testing cannot be implemented, Earth System Models (ESMs) are useful tools to assess the climate impacts of such geoengineering methods. However, coordinated simulations performed with the Geoengineering Model Intercomparison Project (GeoMIP) have shown that climate cooling in response to a continuous injection of 5Tg of SO2 per year under RCP45 future projection (the so-called G4 experiment) differs substantially between ESMs. Here, we employ a volcano analog approach to constrain the climate response in SSA-SRM geoengineering simulations across an ensemble of 10 ESMs. We identify an emergent relationship between the long-term cooling in responses to the mitigation of the clear-sky surface downwelling shortwave radiation (RSDSCS), and the short-term cooling related to the change in RSDSCS during the major tropical volcanic eruptions observed over the historical period (1850-2005). This relationship explains almost 80% of the multi-model spread. Combined with contemporary observations of the latest volcanic eruptions (satellite observations and model reanalyzes), this relationship provides a tight constraint on the climate impacts of SSA-SRM. We estimate that a continuous injection of SO2 aerosols into the stratosphere will reduce the global average temperature of continental land surface by 0.47 K per W m-2, impacting both hydrological and carbon cycles. Compared with the unconstrained ESMs ensemble (range from 0.32 to 0.92 K per W m-2 ), our estimate represents much higher confidence ways to assess the impacts of SSA-SRM on the climate while ruling the most extreme projections of the unconstrained ensemble extremely unlikely.

  6. Rare Isotope Insights into Supereruptions: Rare Sulfur and Triple Oxygen Isotope Geochemistry of Stratospheric Sulfate Aerosols Absorbed on Volcanic Ash Particles

    Science.gov (United States)

    Bindeman, I. N.; Eiler, J.; Wing, B.; Farquhar, J.

    2006-12-01

    We present analyses of stable isotopic ratios of 17O/16O, 18O/16O, 34S/32S, and 33S/32S, 36S/32S of sulfate leached from volcanic ash of a series of well-known volcanic eruptions. This list covers much of the diversity of sizes and the character of volcanic eruptions. Particular emphasis is paid to the Lava Creek Tuff of Yellowstone and we present wide geographic sample coverage for this unit. This global dataset spans a significant range in δ34S, δ18O, and Δ17O of sulfate (29, 30 and 3.3 permil respectively) with oxygen isotopes recording mass-independent fractionation and sulfur isotopes exhibiting mass-dependent behavior. These ranges are defined by the isotopic compositions of products of large caldera forming eruptions. Proximal ignimbrites and coarse ash typically do not contain sulfate. The presence of sulfate with Δ17O > 0.2 permil is characteristic of small distal ash particles, suggesting that sulfate aerosols were scavenged after they underwent atmospheric photochemical reactions. Additionally, sediments that embed ash layers either do not contain sulfate or contain minor sulfate with Δ17O near 0 permil, suggesting that the observed sulfate in ash is of volcanic origin. Mass-dependent sulfur isotopic compositions suggest that sulfate-forming reactions did not involve photolysis of SO2, unlike the situation inferred for some pre-2.3 Ga sulfates or hypothesized to occur during the formation of sulfate associated with plinian eruptions that pierce the ozone layer. However, sulfate in the products of caldera-forming eruptions display a large δ34S range and fractionation relationships that do not follow equilibrium slopes of 0.515 and 1.90 for 33S/32S vs. 34S/32S and 36S/32S vs. 34S/32S, respectively. This implies that the sulfur isotopic characteristics of these sulfates were not set by a single stage, high-temperature equilibrium process in the volcanic plum. The data presented here are consistent with a single stage kinetic fractionation of sulfur

  7. Volcanic aerosols: Chemistry, evolution, and effects

    Science.gov (United States)

    Turco, Richard

    1991-01-01

    Stratospheric aerosols have been the subject of scientific speculation since the 1880s, when the powerful eruption of Krakatoa attracted worldwide attention to the upper atmosphere through spectacular optical displays. The presence of a permanent tenuous dust layer in the lower stratosphere was postulated in the 1920s following studies of the twilight glow. Junge collected the first samples of these 'dust' particles and demonstrated that they were actually composed of sulfates, most likely concentrated sulfuric acid (Junge and Manson, 1961; Junge, 1963). Subsequent research has been spurred by the realization that stratospheric particles can influence the surface climate of earth through their effects on atmospheric radiation. Such aerosols can also influence, through chemical and physical effects, the trace composition of the atmosphere, ozone concentrations, and atmospheric electrical properties. The properties of stratospheric aerosols (both the background particles and those enhanced by volcanic eruptions) were measured in situ by balloon ascents and high altitude aircraft sorties. The aerosols were also observed remotely from the ground and from satellites using both active (lidar) and passive (solar occultation) techniques (remote sensing instruments were carried on aircraft and balloon platforms as well). In connection with the experimental work, models were developed to test theories of particle formation and evolution, to guide measurement strategies, to provide a means of connecting laboratory and field data, and to apply the knowledge gained to answer practical questions about global changes in climate, depletion of the ozone layer, and related environmental problems.

  8. Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

    Energy Technology Data Exchange (ETDEWEB)

    Mills, Michael J. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Schmidt, Anja [School of Earth and Environment, University of Leeds, Leeds UK; Easter, Richard [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Solomon, Susan [Department of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge Massachusetts USA; Kinnison, Douglas E. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Ghan, Steven J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Neely, Ryan R. [School of Earth and Environment, University of Leeds, Leeds UK; National Centre for Atmospheric Science, University of Leeds, Leeds UK; Marsh, Daniel R. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Conley, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Bardeen, Charles G. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Gettelman, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA

    2016-03-06

    Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptions between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.

  9. 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

    Science.gov (United States)

    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.

  10. A Model Simulation of Pinatubo Volcanic Aerosols in the Stratosphere

    Science.gov (United States)

    Zhao , Jing-xia; Turco, Richard P.; Toon, Owen B.

    1995-01-01

    A one-dimensional, time-dependent model is used to study the chemical, microphysical, and radiative properties of volcanic aerosols produced by the Mount Pinatubo eruption on June 15, 1991. Our model treats gas-phase sulfur photochemistry, gas-to-particle conversion of sulfur, and the microphysics of sulfate aerosols and ash particles under stratospheric conditions. The dilution and diffusion of the volcanic eruption clouds are also accounted for in these conditions. Heteromolecular homogeneous and heterogeneous binary H2SO4/H2O nucleation, acid and water condensational growth, coagulation, and gravitational sedimentation are treated in detail in the model. Simulations suggested that after several weeks, the volcanic cloud was composed mainly of sulfuric acid/water droplets produced in situ from the SO2 emissions. The large amounts of SO2 (around 20 Mt) injected into the stratosphere by the Pinatubo eruption initiated homogeneous nucleation which generated a high concentration of small H2SO4/H2O droplets. These newly formed particles grew rapidly by condensation and coagulation in the first few months and then reach their stabilized sizes with effective radii in a range between 0.3 and 0.5 micron approximately one-half year after the eruption. The predicted volcanic cloud parameters reasonably agree with measurements in term of the vertical distribution and lifetime of the volcanic aerosols, their basic microphysical structures (e.g., size distribution, concentration, mass ratio, and surface area) and radiative properties. The persistent volcanic aerosols can produce significant anomalies in the radiation field, which have important climatic consequences. The large enhancement in aerosol surface area can result in measurable global stratospheric ozone depletion.

  11. Formation of the natural sulfate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Kerminen, V.M.; Hillamo, R.; Maekinen, M.; Virkkula, A.; Maekelae, T.; Pakkanen, T. [Helsinki Univ. (Finland). Dept. of Physics

    1996-12-31

    Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

  12. Carbonate-Sulfate Volcanism on Venus?

    Science.gov (United States)

    Kargel, J.S.; Kirk, R.L.; Fegley, B.; Treiman, A.H.

    1994-01-01

    Venusian canali, outflow channels, and associated volcanic deposits resemble fluvial landforms more than they resemble volcanic features on Earth and Mars. Some canali have meandering habits and features indicative of channel migration that are very similar to meandering river channels and flood plains on Earth, venusian outflow channels closely resemble water-carved outflow channels on Mars and the Channeled Scabland in Washington, collapsed terrains at the sources of some venusian channels resemble chaotic terrains at the sources of martian outflow channels, venusian lava deltas are similar to bird's-foot deltas such as the Mississippi delta, and venusian valley networks indicate sapping. The depositional fluvial-type features (deltas, braided bars, and channeled plains) are generally among the smoothest terrains at the Magellan radar wavelength (12.6 cm) on Venus. These features suggest the involvement of an unusual lava, unexpected processes, and/or extraordinary eruption conditions. Possibly the lava was an ordinary silicate lava such as basalt or a less common type of silicate lava, and conditions unique to Venus or to those particular eruptions may have caused an unusual volcanological behavior. We have developed the alternative possibility that the lava had a water-like rheology and a melting point slightly greater than Venus' surface temperature, thus accounting for the unusual behavior of the lava. Unlike silicate lavas, some carbonatites (including carbonate-sulfate-rich liquids) have these properties; thus they can flow great distances while retaining a high fluidity, significant mechanical erosiveness, and substantial capacity to transport and deposit sediment. Venusian geochemistry and petrology are consistent with extensive eruptions of carbonatite lavas, which could have crustal and/or mantle origins. Venus' atmosphere (especially CO2, HCl, and HF abundances) and rocks may be in local chemical equilibrium, which suggests that the upper crust

  13. The Influence of Volcanic Aerosols on Planetary Habitability

    Science.gov (United States)

    Chen, Howard; Horton, Daniel Ethan

    2017-01-01

    On rocky planetary bodies such as Proxima Centuri b, the detection of sulphate aerosols may indicate volcanism and tectonic activity; ingredients hypothesized to be necessary for planetary habitability. However, due to the effect of atmospheric aerosols on a planet’s energy balance, coupled with eruption constituent and frequency uncertainties, the potential impact of volcanic activity on planetary habitability remains unresolved. Here, we employ multi-column climate models in conjunction with a parameter space approach to test the effect of volcanic aerosols on planetary climate with various climate sensitivities. Preliminary results indicate that volcanic activity could provide a means of extending the inner edge of the habitable zone (IHZ), depending on eruption constituents and frequency. Previous work using transit spectra simulations have demonstrated the possibility of detecting transient aerosols of volcanic origin. Our work investigates the range of habitability implications detection of such aerosols would imply.

  14. Dispersion of the Volcanic Sulfate Cloud from the Mount Pinatubo Eruption

    Science.gov (United States)

    Aquila, Valentina; Oman, Luke D.; Stolarski, Richard S.; Colarco, Peter R.; Newman, Paul A.

    2012-01-01

    We simulate the transport of the volcanic cloud from the 1991 eruption of Mount Pinatubo with the GEOS-5 general circulation model. Our simulations are in good agreement with observational data. We tested the importance of initial condition corresponding to the specific meteorological situation at the time of the eruption by employing reanalysis from MERRA. We found no significant difference in the transport of the cloud. We show how the inclusion of the interaction between volcanic sulfate aerosol and radiation is essential for a reliable simulation of the transport of the volcanic cloud. The absorption of long wave radiation by the volcanic sulfate induces a rising of the volcanic cloud up to the middle stratosphere, combined with divergent motion from the latitude of the eruption to the tropics. Our simulations indicate that the cloud diffuses to the northern hemisphere through a lower stratospheric pathway, and to mid- and high latitudes of the southern hemisphere through a middle stratospheric pathway, centered at about 30 hPa. The direction of the middle stratospheric pathway depends on the season. We did not detect any significant change of the mixing between tropics and mid- and high latitudes in the southern hemisphere.

  15. Distribution of sulfur aerosol precursors in the SPCZ released by continuous volcanic degassing at Ambrym, Vanuatu

    Science.gov (United States)

    Lefèvre, Jérôme; Menkes, Christophe; Bani, Philipson; Marchesiello, Patrick; Curci, Gabriele; Grell, Georg A.; Frouin, Robert

    2016-08-01

    The Melanesian Volcanic Arc (MVA) emits about 12 kT d- 1 of sulfur dioxide (SO2) to the atmosphere from continuous passive (non-explosive) volcanic degassing, which contributes 20% of the global SO2 emission from volcanoes. Here we assess, from up-to-date and long-term observations, the SO2 emission of the Ambrym volcano, one of the dominant volcanoes in the MVA, and we investigate its role as sulfate precursor on the regional distribution of aerosols, using both satellite observations and model results at 1° × 1° spatial resolution from WRF-Chem/GOCART. Without considering aerosol forcing on clouds, our model parameterizations for convection, vertical mixing and cloud properties provide a reliable chemical weather representation, making possible a cross-examination of model solution and observations. This preliminary work enables the identification of biases and limitations affecting both the model (missing sources) and satellite sensors and algorithms (for aerosol detection and classification) and leads to the implementation of improved transport and aerosol processes in the modeling system. On the one hand, the model confirms a 50% underestimation of SO2 emissions due to satellite swath sampling of the Ozone Monitoring Instrument (OMI), consistent with field studies. The OMI irregular sampling also produces a level of noise that impairs its monitoring capacity during short-term volcanic events. On the other hand, the model reveals a large sensitivity on aerosol composition and Aerosol Optical Depth (AOD) due to choices of both the source function in WRF-Chem and size parameters for sea-salt in FlexAOD, the post-processor used to compute offline the simulated AOD. We then proceed to diagnosing the role of SO2 volcanic emission in the regional aerosol composition. The model shows that both dynamics and cloud properties associated with the South Pacific Convergence Zone (SPCZ) have a large influence on the oxidation of SO2 and on the transport pathways of

  16. Why Is the Climate Forcing of Sulfate Aerosols So Uncertain?

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Sulfate aerosol particles have strong scattering effect on the solar radiation transfer which results in increasing the planet albedo and, hence, tend to cool the earth-atmosphere system. Also, aerosols can act as the cloud condensation nuclei (CCN) which tend to increase the albedo of clouds and cool the global warming. The ARPEGE-Climat version 3 AGCM with FMR radiation scheme is used to estimate the direct and indirect radiative forcing of sulfate aerosols. For minimizing the uncertainties in assessing this kind of cooling effect, all kinds of factors are analyzed which have been mixed in the assessment process and may lead to the different results of the radiative forcing of aerosols. It is noticed that one of the uncertainties to assess the climate forcing of aerosols by GCM results from the different definition of radiative forcing that was used. In order to clarify this vague idea, the off-line case for considering no feedbacks and on-line case for including all the feedbacks have been used for assessment. The direct forcing of sulfate aerosols in off-line case is -0.57 W/m2 and -0.38 W/m2 for the clear sky and all sky respectively. The value of on-line case appears to be a little larger than that in off-line case chiefly due to the feedback of clouds. The indirect forcing of sulfate aerosols in off-line case is -1.4 W / m2 and -1.0 W / m2 in on-line case. The radiative forcing of sulfate aerosols has obvious regional characteristics. There is a larger negative radiative forcing over North America, Europe and East Asia. If the direct and indirect forcing are added together, it is enough to offset the positive radiative forcing induced by the greenhouse gases in these regions.

  17. Observation and Model Comparison on Precipitation response to Volcanic Aerosols in the Asian Monsoon Region

    Science.gov (United States)

    Zhuo, Z.; Gao, C.

    2014-12-01

    Disagreement between observation and models were shown on the volcanic sulfate aerosols' effect on precipitation in Asia monsoon region. Here, we investigate it by classifying two groups of historical volcanism between AD 1300 and AD 1850 to 2, 1, and 0.5 times Pinatubo sulfate injection into the northern hemisphere (NH) stratosphere based on IVI2 and Crowley2013 volcanic reconstructions, then comparing precipitation response of BCC-CSM1 and CCSM4 model outputs under past1000 scenario to IVI2 volcanic group, and that of MIROC-ESM and MPI-ESM-P to Crowley2013 group with tree-ring reconstruction data MADA. In both groups, Superposed Epoch Analysis (SEA) of MADA and four model outputs show a drying trend over Asia monsoon regions after the NH injections and drier with larger sulfate magnitude, with a 1 or 2 year time lag in MADA comparing to the model outputs, this may result from the biological response of tree ring data that lag behind the meteorological forcing of model outputs. On the other hand, different responses to Southern Hemisphere (SH) only injections were found between the two groups as well as MADA and model outputs. Most of the results were found significant at 90% or even 95% significance level with a 10,000 Monte Carlo resampling procedure. Spatial variation of MADA show a significant drying effect in central Asia in year 1, and then move westward in year 2 and 3 after 2, 1×Pinatubo eruptions of IVI2, while a significant wetting effect in northwest Asia but drying effect in south Asia were shown in Crowley2013 group. However, model outputs did not show spatial variation, with a pattern drier in northwest than in southeast Asia along the years after the eruptions in both volcanic groups. Thus, observation and model outputs are well consistent on precipitation response to NH aerosol injections, but models may need large improvement on the response to SH aerosol injection as well as the spatial variation. Besides, opposite precipitation response to SH

  18. Ozone Depletion at Mid-Latitudes: Coupling of Volcanic Aerosols and Temperature Variability to Anthropogenic Chlorine

    Science.gov (United States)

    Solomon, S.; Portmann, R. W.; Garcia, R. R.; Randel, W.; Wu, F.; Nagatani, R.; Gleason, J.; Thomason, L.; Poole, L. R.; McCormick, M. P.

    1998-01-01

    Satellite observations of total ozone at 40-60 deg N are presented from a variety of instruments over the time period 1979-1997. These reveal record low values in 1992-3 (after Pinatubo) followed by partial but incomplete recovery. The largest post-Pinatubo reductions and longer-term trends occur in spring, providing a critical test for chemical theories of ozone depletion. The observations are shown to be consistent with current understanding of the chemistry of ozone depletion when changes in reactive chlorine and stratospheric aerosol abundances are considered along with estimates of wave-driven fluctuations in stratospheric temperatures derived from global temperature analyses. Temperature fluctuations are shown to make significant contributions to model calculated northern mid-latitude ozone depletion due to heterogeneous chlorine activation on liquid sulfate aerosols at temperatures near 200-210 K (depending upon water vapor pressure), particularly after major volcanic eruptions. Future mid-latitude ozone recovery will hence depend not only on chlorine recovery but also on temperature trends and/or variability, volcanic activity, and any trends in stratospheric sulfate aerosol.

  19. Modeling of 2008 Kasatochi volcanic sulfate direct radiative forcing: assimilation of OMI SO2 plume height data and comparison with MODIS and CALIOP observations

    Directory of Open Access Journals (Sweden)

    A. H. Omar

    2012-10-01

    Full Text Available Volcanic SO2 column amount and injection height retrieved from the Ozone Monitoring Instrument (OMI with the Extended Iterative Spectral Fitting (EISF technique are used to initialize a global chemistry transport model (GEOS-Chem to simulate the atmospheric transport and lifecycle of volcanic SO2 and sulfate aerosol from the 2008 Kasatochi eruption, and to subsequently estimate the direct shortwave, top-of-the-atmosphere radiative forcing of the volcanic sulfate aerosol. Analysis shows that the integrated use of OMI SO2 plume height in GEOS-Chem yields: (a good agreement of the temporal evolution of 3-D volcanic sulfate distributions between model simulations and satellite observations from the Moderate Resolution Imaging Spectroradiometer (MODIS and Cloud-Aerosol Lidar with Orthogonal Polarisation (CALIOP, and (b a e-folding time for volcanic SO2 that is consistent with OMI measurements, reflecting SO2 oxidation in the upper troposphere and stratosphere is reliably represented in the model However, a consistent (~25% low bias is found in the GEOS-Chem simulated SO2 burden, and is likely due to a high (~20% bias of cloud liquid water amount (as compared to the MODIS cloud product and the resultant stronger SO2 oxidation in the GEOS meteorological data during the first week after eruption when part of SO2 underwent aqueous-phase oxidation in clouds. Radiative transfer calculations show that the forcing by Kasatochi volcanic sulfate aerosol becomes negligible 6 months after the eruption, but its global average over the first month is −1.3 W m−2 with the majority of the forcing-influenced region located north of 20° N, and with daily peak values up to −2 W m−2 on days 16–17. Sensitivity experiments show that every 2 km decrease of SO2 injection height in the GEOS-Chem simulations will result in a ~25% decrease in volcanic sulfate forcing; similar sensitivity but opposite sign also holds for a 0.03 μm increase of geometric radius of the

  20. Modeling of 2008 Kasatochi volcanic sulfate direct radiative forcing: assimilation of OMI SO2 plume height data and comparison with MODIS and CALIOP observations

    Directory of Open Access Journals (Sweden)

    N. Krotkov

    2013-02-01

    Full Text Available Volcanic SO2 column amount and injection height retrieved from the Ozone Monitoring Instrument (OMI with the Extended Iterative Spectral Fitting (EISF technique are used to initialize a global chemistry transport model (GEOS-Chem to simulate the atmospheric transport and lifecycle of volcanic SO2 and sulfate aerosol from the 2008 Kasatochi eruption, and to subsequently estimate the direct shortwave, top-of-the-atmosphere radiative forcing of the volcanic sulfate aerosol. Analysis shows that the integrated use of OMI SO2 plume height in GEOS-Chem yields: (a good agreement of the temporal evolution of 3-D volcanic sulfate distributions between model simulations and satellite observations from the Moderate Resolution Imaging Spectroradiometer (MODIS and Cloud-Aerosol Lidar with Orthogonal Polarisation (CALIOP, and (b an e-folding time for volcanic SO2 that is consistent with OMI measurements, reflecting SO2 oxidation in the upper troposphere and stratosphere is reliably represented in the model. However, a consistent (~25% low bias is found in the GEOS-Chem simulated SO2 burden, and is likely due to a high (~20% bias of cloud liquid water amount (as compared to the MODIS cloud product and the resultant stronger SO2 oxidation in the GEOS meteorological data during the first week after eruption when part of SO2 underwent aqueous-phase oxidation in clouds. Radiative transfer calculations show that the forcing by Kasatochi volcanic sulfate aerosol becomes negligible 6 months after the eruption, but its global average over the first month is −1.3 Wm−2, with the majority of the forcing-influenced region located north of 20° N, and with daily peak values up to −2 Wm−2 on days 16–17. Sensitivity experiments show that every 2 km decrease of SO2 injection height in the GEOS-Chem simulations will result in a ~25 % decrease in volcanic sulfate forcing; similar sensitivity but opposite sign also holds for a 0.03 μm increase of geometric radius of

  1. Modeling of 2008 Kasatochi Volcanic Sulfate Direct Radiative Forcing: Assimilation of OMI SO2 Plume Height Data and Comparison with MODIS and CALIOP Observations

    Science.gov (United States)

    Wang, J.; Park, S.; Zeng, J.; Ge, C.; Yang, K.; Carn, S.; Krotkov, N.; Omar, A. H.

    2013-01-01

    Volcanic SO2 column amount and injection height retrieved from the Ozone Monitoring Instrument (OMI) with the Extended Iterative Spectral Fitting (EISF) technique are used to initialize a global chemistry transport model (GEOS-Chem) to simulate the atmospheric transport and lifecycle of volcanic SO2 and sulfate aerosol from the 2008 Kasatochi eruption, and to subsequently estimate the direct shortwave, top-of-the-atmosphere radiative forcing of the volcanic sulfate aerosol. Analysis shows that the integrated use of OMI SO2 plume height in GEOS-Chem yields: (a) good agreement of the temporal evolution of 3-D volcanic sulfate distributions between model simulations and satellite observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarisation (CALIOP), and (b) an e-folding time for volcanic SO2 that is consistent with OMI measurements, reflecting SO2 oxidation in the upper troposphere and stratosphere is reliably represented in the model. However, a consistent (approx. 25 %) low bias is found in the GEOS-Chem simulated SO2 burden, and is likely due to a high (approx.20 %) bias of cloud liquid water amount (as compared to the MODIS cloud product) and the resultant stronger SO2 oxidation in the GEOS meteorological data during the first week after eruption when part of SO2 underwent aqueous-phase oxidation in clouds. Radiative transfer calculations show that the forcing by Kasatochi volcanic sulfate aerosol becomes negligible 6 months after the eruption, but its global average over the first month is -1.3W/sq m, with the majority of the forcing-influenced region located north of 20degN, and with daily peak values up to -2W/sq m on days 16-17. Sensitivity experiments show that every 2 km decrease of SO2 injection height in the GEOS-Chem simulations will result in a approx.25% decrease in volcanic sulfate forcing; similar sensitivity but opposite sign also holds for a 0.03 m increase of geometric radius of

  2. The Sectional Stratospheric Sulfate Aerosol module (S3A-v1) within the LMDZ general circulation model: description and evaluation against stratospheric aerosol observations

    Science.gov (United States)

    Kleinschmitt, Christoph; Boucher, Olivier; Bekki, Slimane; Lott, François; Platt, Ulrich

    2017-09-01

    Stratospheric aerosols play an important role in the climate system by affecting the Earth's radiative budget as well as atmospheric chemistry, and the capabilities to simulate them interactively within global models are continuously improving. It is important to represent accurately both aerosol microphysical and atmospheric dynamical processes because together they affect the size distribution and the residence time of the aerosol particles in the stratosphere. The newly developed LMDZ-S3A model presented in this article uses a sectional approach for sulfate particles in the stratosphere and includes the relevant microphysical processes. It allows full interaction between aerosol radiative effects (e.g. radiative heating) and atmospheric dynamics, including e.g. an internally generated quasi-biennial oscillation (QBO) in the stratosphere. Sulfur chemistry is semi-prescribed via climatological lifetimes. LMDZ-S3A reasonably reproduces aerosol observations in periods of low (background) and high (volcanic) stratospheric sulfate loading, but tends to overestimate the number of small particles and to underestimate the number of large particles. Thus, it may serve as a tool to study the climate impacts of volcanic eruptions, as well as the deliberate anthropogenic injection of aerosols into the stratosphere, which has been proposed as a method of geoengineering to abate global warming.

  3. Spectral signatures of polar stratospheric clouds and sulfate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Massie, S.T.; Bailey, P.L.; Gille, J.C. [National Center for Atmospheric Research, Boulder, CO (United States); Lee, E.C. [Princeton Univ., NJ (United States); Mergenthaler, J.L.; Roche, A.E.; Kumer, J.B. [Lockheed Palo Alto Research Lab., CA (United States); Fishbein, E.F.; Waters, J.W. [California Institute of Technology, Pasadena, CA (United States); Lahoz, W.A. [Univ. of Reading (United Kingdom)

    1994-10-15

    Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605 cm{sup {minus}1} (10.8, 8.0, and 6.2 {mu}m) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheroidal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculation and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles. 47 refs., 22 figs., 3 tabs.

  4. The Pacific Marine aerosol: Evidence for natural acid sulfates

    Science.gov (United States)

    Clarke, Antony D.; Ahlquist, Norman C.; Covert, David S.

    1987-04-01

    Optical, chemical, and physical measurements of marine boundary layer aerosol were made during two oceanographic cruises in the central Pacific in the fall of 1983 and spring of 1984. Both cruises revealed a ubiquitous accumulation mode atmospheric aerosol that showed marked increases in the region of equatorial upwelling, 4°N to 15°S, between Hawaii and Tahiti. Changes in the aerosol size distribution in response to thermal conditioning revealed properties consistent with those of sulfuric acid and/or ammonium sulfate/bisulfate depending upon the sampling location. Changes in the apparent acidity of the accumulation mode varied in conjunction with physical and chemical properties of the region sampled, while the number concentration suggests that it is the dominant and possibly limiting aerosol for cloud condensation nuclei in the remote central Pacific.

  5. Measuring 35S of Aerosol Sulfate: Techniques and First Results

    Science.gov (United States)

    Brothers, L. A.; Dominguez, G.; Bluen, B.; Corbin, A.; Abramian, A.; Thiemens, M. H.

    2007-12-01

    On a global and regional level, the cycling of sulfur in the environment has consequences for air quality, human health, and may contribute to global climate change. Due to its multiple oxidation states, the sulfur cycle is very complex and poorly understood. Stable isotopes are currently used to understand reaction pathways as well as sources and sinks of sulfurous compounds in the environment. Sulfur also has one short lived (τ1/2 ~87 d) radioactive isotope (35S) which is continuously made in the atmosphere by the cosmic ray spallation of argon, is then quickly oxidized to 35SO2 and enters the atmospheric sulfur cycle. The short-lived radioactive nature of this isotope of sulfur provides us with potentially powerful tracer for understanding the time scales at which sulfur is oxidized, deposited, and transported in the atmosphere and the deposition of atmospheric sulfate into rivers and water catchments. However, despite its potential, the use of 35S as a tracer of aerosol chemistry has not been fully exploited, Here we present details of instrumental set up for measuring 35S in aerosol sulfate and some preliminary results of measurements of 35S abundances in aerosols from Riverside (inland) and La Jolla (coastal) CA and discuss the sensitivity and limitations of the measurements in providing insights into day/night aerosol chemistry (Riverside) as well as the uptake of SO2 pollution in coastal environments by sea-salt aerosols. Also, we present preliminary results from measurement of sulfate in river water in Ecuador before and after precipitation events.

  6. Tales of volcanoes and El-Nino southern oscillations with the oxygen isotope anomaly of sulfate aerosol.

    Science.gov (United States)

    Shaheen, Robina; Abauanza, Mariana; Jackson, Teresa L; McCabe, Justin; Savarino, Joel; Thiemens, Mark H

    2013-10-29

    The ability of sulfate aerosols to reflect solar radiation and simultaneously act as cloud condensation nuclei renders them central players in the global climate system. The oxidation of S(IV) compounds and their transport as stable S(VI) in the Earth's system are intricately linked to planetary scale processes, and precise characterization of the overall process requires a detailed understanding of the linkage between climate dynamics and the chemistry leading to the product sulfate. This paper reports a high-resolution, 22-y (1980-2002) record of the oxygen-triple isotopic composition of sulfate (SO4) aerosols retrieved from a snow pit at the South Pole. Observed variation in the O-isotopic anomaly of SO4 aerosol is linked to the ozone variation in the tropical upper troposphere/lower stratosphere via the Ozone El-Niño Southern Oscillations (ENSO) Index (OEI). Higher (17)O values (3.3‰, 4.5‰, and 4.2‰) were observed during the three largest ENSO events of the past 2 decades. Volcanic events inject significant quantities of SO4 aerosol into the stratosphere, which are known to affect ENSO strength by modulating stratospheric ozone levels (OEI = 6 and (17)O = 3.3‰, OEI = 11 and (17)O = 4.5‰) and normal oxidative pathways. Our high-resolution data indicated that (17)O of sulfate aerosols can record extreme phases of naturally occurring climate cycles, such as ENSOs, which couple variations in the ozone levels in the atmosphere and the hydrosphere via temperature driven changes in relative humidity levels. A longer term, higher resolution oxygen-triple isotope analysis of sulfate aerosols from ice cores, encompassing more ENSO periods, is required to reconstruct paleo-ENSO events and paleotropical ozone variations.

  7. Sulfuric acid deposition from stratospheric geoengineering with sulfate aerosols

    KAUST Repository

    Kravitz, Ben

    2009-07-28

    We used a general circulation model of Earth\\'s climate to conduct geoengineering experiments involving stratospheric injection of sulfur dioxide and analyzed the resulting deposition of sulfate. When sulfur dioxide is injected into the tropical or Arctic stratosphere, the main additional surface deposition of sulfate occurs in midlatitude bands, because of strong cross-tropopause flux in the jet stream regions. We used critical load studies to determine the effects of this increase in sulfate deposition on terrestrial ecosystems by assuming the upper limit of hydration of all sulfate aerosols into sulfuric acid. For annual injection of 5 Tg of SO2 into the tropical stratosphere or 3 Tg of SO2 into the Arctic stratosphere, neither the maximum point value of sulfate deposition of approximately 1.5 mEq m−2 a−1 nor the largest additional deposition that would result from geoengineering of approximately 0.05 mEq m−2 a−1 is enough to negatively impact most ecosystems.

  8. Strong Constraints on Aerosol-Cloud Interactions from Volcanic Eruptions

    Science.gov (United States)

    Malavelle, Florent F.; Haywood, Jim M.; Jones, Andy; Gettelman, Andrew; Clarisse, Lieven; Bauduin, Sophie; Allan, Richard P.; Karset, Inger Helene H.; Kristjansson, Jon Egill; Oreopoulos, Lazaros; hide

    2017-01-01

    Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets - consistent with expectations - but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around minus 0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.

  9. Characterizing the influence of anthropogenic emissions and transport variability on sulfate aerosol concentrations at Mauna Loa Observatory

    Science.gov (United States)

    Potter, Lauren E.

    data were supplemented with observations of gaseous radon (Rn222) and carbon monoxide (CO), used as tracers of long distance continental influence. Our study applied trajectory analysis and multiple linear regression to interpret the relative roles of aerosol precursor emissions and large-scale transport characteristics on observed MLO sulfate aerosol variability. We conclude that observed sulfate aerosol at MLO likely originated from a combination of anthropogenic, volcanic, and biogenic sources that varied seasonally and from year to year. Analysis of chemical continental tracer concentrations and HYSPLIT back trajectories suggests that non-negligible long distance influence from either the Asian or North American continents can be detected at MLO during all seasons although large interannual variability was observed. Possible influence of circulation changes in the Pacific Basin related to the El Nino-Southern Oscillation were found to be both species and seasonally dependent. We further found an increasing trend in monthly mean sulfate aerosol concentrations at MLO of 4.8% (7.3 ng m-3) per year during 1995-2008, significant at the 95% confidence level. Multiple linear regression results suggest that the observed trend in sulfate concentrations at MLO cannot reasonably be explained by variations in meteorology and transport efficiency alone. An increasing sulfate trend of 5.8 ng m-3 per year, statistically significant at the 90% confidence level, was found to be associated with the variable representing East Asian SO2 emissions. The results of this study provide evidence that MLO sulfate aerosol observations during 1995-2008 reflect, in part, recent trends in anthropogenic SO2 emissions which are superimposed onto the natural meteorological variability affecting transport efficiency.

  10. Controlled exposures of human volunteers to sulfate aerosols. Health effects and aerosol characterization.

    Science.gov (United States)

    Avol, E L; Jones, M P; Bailey, R M; Chang, N M; Kleinman, M T; Linn, W S; Bell, K A; Hackney, J D

    1979-08-01

    Our laboratory has undertaken the study of possible acute adverse health effects of sulfate aerosols through controlled exposures of volunteer human subjects. Both healthy and asthmatic adult men were exposed for 2-hour periods (with intermittent exercise) to ammonium sulfate, ammonium bisulfate, and sulfuric acid of particle size distributions and concentrations intended to simulate "worst case" exposures during Los Angeles smog episodes. Lung function tests were performed by the subjects on entering and before exiting from a carefully controlled environmental chamber. Subject symptoms were evluated in a standardized manner. Aerosol concentrations and size distributions were determined by an on-line computer/aerometric monitoring system; gravimetric and chemical analyses were performed on impactor and total filter samples after test exposures. We found little or no evidence of adverse health effects from 2-hour multiple-day exposures to any of the compounds at "worst case" ambient concentrations.

  11. Parameterization of the Optical Properties of Sulfate Aerosols.

    Science.gov (United States)

    Li, J.; Wong, J. G. D.; Dobbie, J. S.; Chýlek, P.

    2001-01-01

    Parameterizations of the shortwave optical properties of ammonium sulfate [(NH4)2SO4], ammonium bisulfate (NH4HSO4), and sulfuric acid (H2SO4) are provided as functions of relative humidity for high and low spectral resolution band models. The optical property parameterization is simple in form and in its dependence on relative humidity. The growth of the aerosol particles is based on equilibrium saturation theory, and the optical properties are computed from Mie theory. The optical properties necessary for the most commonly used radiative transfer methods are provided.Results show that when relative humidity effects are included in the backscatter fraction the radiative forcing is found to be a more sensitive function of near infrared wavelengths compared to visible wavelengths. For increasing relative humidity, sulfuric acid is found to have a larger effect on radiative forcing compared to the forcing by ammonium sulfate or ammonium bisulfate. Also, as relative humidity increases, forcing increases to higher values for smaller mode size distributions compared to forcing by larger mode distributions. These parameterizations will enable climate forcing studies to be performed with radiative transfer schemes that more accurately represent sulfate influences on the radiation balance.

  12. Likely seeding of cirrus clouds by stratospheric Kasatochi volcanic aerosol particles near a mid-latitude tropopause fold

    Science.gov (United States)

    Campbell, James R.; Welton, Ellsworth J.; Krotkov, Nickolay A.; Yang, Kai; Stewart, Sebastian A.; Fromm, Michael D.

    2012-01-01

    Following the explosive 7-8 August 2008 Mt. Kasatochi volcanic eruption in southwestern Alaska, a segment of the dispersing stratospheric aerosol layer was profiled beginning 16 August in continuous ground-based lidar measurements over the Mid-Atlantic coast of the eastern United States. On 17-18 August, the layer was displaced downward into the upper troposphere through turbulent mixing near a tropopause fold. Cirrus clouds and ice crystal fallstreaks were subsequently observed, having formed within the entrained layer. The likely seeding of these clouds by Kasatochi aerosol particles is discussed. Cloud formation is hypothesized as resulting from either preferential homogenous freezing of relatively large sulfate-based solution droplets deliquesced after mixing into the moist upper troposphere or through heterogeneous droplet activation by volcanic ash. Satellite-borne spectrometer measurements illustrate the evolution of elevated Kasatochi SO 2 mass concentrations regionally and the spatial extent of the cirrus cloud band induced by likely particle seeding. Satellite-borne polarization lidar observations confirm ice crystal presence within the clouds. Geostationary satellite-based water vapor channel imagery depicts strong regional subsidence, symptomatic of tropopause folding, along a deepening trough in the sub-tropical westerlies. Regional radiosonde profiling confirms both the position of the fold and depth of upper-tropospheric subsidence. These data represent the first unambiguous observations of likely cloud seeding by stratospheric volcanic aerosol particles after mixing back into the upper troposphere.

  13. The impact of stratospheric volcanic aerosol on decadal-scale climate predictions

    Science.gov (United States)

    Timmreck, Claudia; Pohlmann, Holger; Illing, Sebastian; Kadow, Christopher

    2016-04-01

    The possibility of a large future volcanic eruption provides arguably the largest uncertainty concerning the evolution of the climate system on the time scale of a few years; but also the greatest opportunity to learn about the behavior of the climate system, and our models thereof. So the question emerges how large will the uncertainty be for future decadal climate predictions if no volcanic aerosol is taken into account? And how strong has volcanic aerosol affected decadal prediction skill on annual and multi-year seasonal scales over the CMIP5 hindcast period? To understand the impact of volcanic aerosol on multi-year seasonal and decadal climate predictions we performed CMIP5-type hindcasts without volcanic aerosol using the German MiKlip prediction system system baseline 1 from 1961 to 1991 and compared them to the corresponding simulations including aerosols. Our results show that volcanic aerosol significantly affects the prediction skill for global mean surface air temperature in the first five years after strong volcanic eruptions. Also on the regional scale a volcanic imprint on decadal-scale variability is detectable. Neglecting volcanic aerosol leads to a reduced prediction skill over the tropical and subtropical Atlantic, Indic and West Pacific but to an improvement over the tropical East-Pacific, where the model has in general no skill. Multi-seasonal differences in the skill for seasonal-mean temperatures are evident over Continental Europe with significant skill loss due to neglection of volcanic aerosol in boreal winter over central Europe, Scandinavia and over south-eastern Europe and the East-Mediterranean in boreal summer.

  14. Sensitivity studies for incorporating the direct effect of sulfate aerosols into climate models

    Science.gov (United States)

    Miller, Mary Rawlings Lamberton

    2000-09-01

    Aerosols have been identified as a major element of the climate system known to scatter and absorb solar and infrared radiation, but the development of procedures for representing them is still rudimentary. This study addresses the need to improve the treatment of sulfate aerosols in climate models by investigating how sensitive radiative particles are to varying specific sulfate aerosol properties. The degree to which sulfate particles absorb or scatter radiation, termed the direct effect, varies with the size distribution of particles, the aerosol mass density, the aerosol refractive indices, the relative humidity and the concentration of the aerosol. This study develops 504 case studies of altering sulfate aerosol chemistry, size distributions, refractive indices and densities at various ambient relative humidity conditions. Ammonium sulfate and sulfuric acid aerosols are studied with seven distinct size distributions at a given mode radius with three corresponding standard deviations implemented from field measurements. These test cases are evaluated for increasing relative humidity. As the relative humidity increases, the complex index of refraction and the mode radius for each distribution correspondingly change. Mie theory is employed to obtain the radiative properties for each case study. The case studies are then incorporated into a box model, the National Center of Atmospheric Research's (NCAR) column radiation model (CRM), and NCAR's community climate model version 3 (CCM3) to determine how sensitive the radiative properties and potential climatic effects are to altering sulfate properties. This study found the spatial variability of the sulfate aerosol leads to regional areas of intense aerosol forcing (W/m2). These areas are particularly sensitive to altering sulfate properties. Changes in the sulfate lognormal distribution standard deviation can lead to substantial regional differences in the annual aerosol forcing greater than 2 W/m 2. Changes in the

  15. Effects of brief and intermediate exposures to sulfate submicron aerosols and sulfate injections on cardiopulmonary function of dogs and tracheal mucous velocity of sheep

    Energy Technology Data Exchange (ETDEWEB)

    Sackner, M.A. (Mount Sinai Medical Center, Miami Beach, FL); Dougherty, R.L.; Chapman, G.A.; Cipley, J.; Perez, D.; Kwoka, M.; Reinhart, M.; Brito, M.; Schreck, R.

    1981-06-01

    Pulmonary mechanics of anesthetized dogs were not changed or were minimally altered by breathing the following compounds as submicron aerosols in concentrations up to 17.3 mg/m/sup 3/ for 7.5 min: (1) sodium chloride (as a control), (2) sodium sulfate, (3) ammonium sulfate, (4) zinc sulfate, (5) zinc ammonium sulfate, (6) ammonium bisulfate, (7) aluminum sulfate, (8) manganese sulfate, (9) nickel sulfate, (10) copper sulfate, (11) ferrous fulfate, and (12) ferric sulfate. Submicron aerosols of these compounds in concentrations of 4.1 to 8.8 mg/m/sup 3/, administered for 4 h to anesthetized dogs, did not affect mechanics of breathing, hemodynamics, and arterial blood gases. In conscious sheep, tracheal mucous velocity was not altered by exposure to the submicron aerosols of the sulfate compounds. None of these compounds, injected iv in a dose of 1 mg, had adverse effects on mechanics of breathing, pulmonary and systemic hemodynamics, or arterial blood gases. In 100-mg injections, zinc sulfate and zinc ammonium sulfate produced a fall in cardiac output, systemic hypotension, hypoxemia, and metabolic acidosis. Copper sulfate at this dose produced pulmonary hypertension, a fall in cardiac output, hypoxemia, respiratory acidosis, and a decrease of specific total respiratory conductance. It is concluded that submicron aerosols of sulfate salts do not have adverse cardiopulmonary effects when administered in high concentrations for up to 4 h. However, prolonged exposure to high concentrations of zinc sulfate, zinc ammonium sulfate, and copper sulfate aerosols might have adverse cardiopulmonary effects.

  16. Regional radiative impact of volcanic aerosol from the 2009 eruption of Redoubt volcano

    Directory of Open Access Journals (Sweden)

    C. L. Young

    2011-09-01

    Full Text Available High northern latitude eruptions have the potential to release volcanic aerosol into the Arctic environment, perturbing the Arctic's climate system. In this study, we present assessments of shortwave (SW, longwave (LW and net direct aerosol radiative forcings (DARFs and atmospheric heating/cooling rates caused by volcanic aerosol from the 2009 eruption of Redoubt Volcano by performing radiative transfer modeling constrained by NASA A-Train satellite data. The Ozone Monitoring Instrument (OMI, the Moderate Resolution Imaging Spectroradiometer (MODIS, and the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT model for volcanic ash were used to characterize aerosol across the region. A representative range of aerosol optical depths (AODs at 550 nm were obtained from MODIS, and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO was used to determine the altitude and thickness of the plumes. The optical properties of volcanic aerosol were calculated using a compositionally resolved microphysical model developed for both ash and sulfates. Two compositions of volcanic aerosol were considered in order to examine a fresh, ash rich plume and an older, ash poor plume. Optical models were incorporated into a modified version of the Santa Barbara Disort Atmospheric Radiative Transfer (SBDART model. Radiative transfer calculations were made for a range of surface albedos and solar zenith angles (SZA representative of the region. We find that the total DARF caused by a fresh, thin plume (~2.5–7 km at an AOD (550 nm range of 0.16–0.58 and SZA = 55° is –46 W m−2AOD−1 at the top of the atmosphere (TOA, 110 W m−2AOD−1 in the aerosol layer, and – 150 W m−2AOD−1 at the surface over seawater. However, the total DARF for the same plume over snow and at the same SZA at TOA, in the layer, and at the surface is 170, 170, and −2 W m−2

  17. The influence of cloud droplet heterogeneity on sulfate production mechanisms constrained by isotopic measurements of sulfate aerosol

    Science.gov (United States)

    Alexander, B.; Allman, D. J.; Amos, H. M.; Fairlie, T. D.; Dachs, J.; Hegg, D.; Sletten, R. S.

    2011-12-01

    Observations and modeling studies have shown that heterogeneity in fog and cloud drop size and chemical composition can significantly impact in-cloud sulfate production rates due to the strong pH dependence of the ozone oxidation pathway. Averaging cloud water pH tends to underestimate the fraction of S(IV) that is SO32- leading to underestimates of in-cloud sulfate production rates. Large scale models typically do not account for this heterogeneity due to the large computational expense associated with this calculation, and instead employ bulk calculations or assumptions of cloud water pH. Modeling studies have consistently shown that calculated sulfate production rates using bulk cloud pH treatments tend to underestimate in-cloud sulfate production rates compared to more explicit treatment of cloud drop heterogeneity by underestimating the ozone oxidation pathway. Here, we utilize a global chemical transport model (GEOS-Chem) and observations of the oxygen isotopic composition of sulfate aerosol collected during a ship cruise in the subtropical northeast Atlantic Ocean to quantify sulfate formation pathways in the marine boundary layer. The oxygen isotopic composition of sulfate aerosol is particularly sensitive to the importance of the ozone oxidation pathway due to its large isotopic signature. We employ a model parameterization by Yuen et al. (1996) that accounts for the impact of alkaline, coarse-mode sea salt aerosols on in-cloud sulfate production rates. As sulfate formation in cloud droplets formed on alkaline coarse-mode sea salt aerosols is thought to be dominated by the ozone oxidation pathway, observations of the oxygen isotopic composition of sulfate aerosol provide a robust test of this parameterization. Including the Yuen et al. (1996) parameterization of cloud droplet heterogeneity improves the model's agreement with the observed sulfate oxygen isotopes. Accounting for the impact of cloud droplet heterogeneity on in-cloud sulfate production rates

  18. INVESTIGATION ON PROPERTIES OF CONCRETE CONTAINING NATURAL POZZOLAN VOLCANIC ORIGIN DUE TO SULFATE ATTACK

    OpenAIRE

    MERIDA AHCENE; KHARCHI FATTOUM

    2013-01-01

    Sulfate attack and its effects are important from both scientific and industrial viewpoints. It is perceived that concretes containing pozzolan have better performance in sulfate solutions, since the pozzolanic reactions reduce the quantity of calcium hydroxide and increase calcium silicate hydrate. This paper investigates thecontribution of natural pozzolan volcanic origin on the physico - mechanical and physico-chemical characteristics of the concretes. When it is coupled to a water reducin...

  19. Phosphorus-bearing Aerosol Particles From Volcanic Plumes

    Science.gov (United States)

    Obenholzner, J. H.; Schroettner, H.; Poelt, P.; Delgado, H.; Caltabiano, T.

    2003-12-01

    Particles rich in P or bulk geochemical data of volcanic aerosol particles showing high P contents are known from many volcanic plumes (Stanton, 1994; Obenholzner et al., 2003). FESEM/EDS analysis of individual particles obtained from the passively degassing plume of Popocatepetl volcano, Mx. (1997) and from the plume of Stromboli (May 2003) show P frequently. Even at the high resolution of the FESEM, euhedral apatite crystals could not be observed. At Popocatepetl (1997) spherical Ca-P-O particles are common. Fluffy, fractal or botryoidal particles also can contain EDS-detectable amounts of P. The EDS spectrum of such particles can comprise various elements. However most particles show P, S and Cl. P-S and P-S-metal species are known in chemistry but do they occur in volcanic plumes? Stoichiometric considerations had been made in the past suggesting the existence of P-S species in plumes (Stanton 1994), gas sampling and remote gas monitoring systems have not detected yet such molecules in plumes. The particle spectrum of the reawakened Popocateptel volcano might be related to accumulation of volatiles at the top of a magma chamber during the phase of dormancy. P-Fe rich, Ca-free aggregates are also known from the eruption of El Chichon 1982 (SEM/EDS by M. Sheridan, per. comm. 08-24-2003). Persistently active volcanoes (i.e. Stromboli) represent a different category according to continuous degassing and aerosol particle formation. A particle collector ( ca. 90 ml/min) accompanied a COSPEC helicopter flight at Stromboli (May 15, 2003) after one of the rare types of sub-plinian events on April 5 2003. P-bearing particles are very common. For instance, an Fe oxide grain (diam. = 2 æm) is partially covered by fluffy and euhedral P-bearing matter. The elements detected are P, Cl, Na, Mg, Al, Si, K, Ca, Ti and (Fe). The fluffy and the euhedral (rhombohedral?) matter show in SE-BSE-mix image almost identical grey colors. At Stromboli and Popocatepetl particles on which

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

    Science.gov (United States)

    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.

  1. The partitioning of Nitric Acid between the gas phase and condensed phase of aqueous sulfate aerosols.

    Science.gov (United States)

    Mentel, T. F.; Folkers, M.; Sebald, H.; Wahner, A.

    2001-12-01

    The heterogeneous hydrolysis of N2O_5 on aqueous aerosol surfaces is an important source of atmospheric HNO3. We generated HNO3 by heterogeneous hydrolysis of N2O_5 on aqueous ammonium and sodium sulfate aerosols and studied its partitioning between the gas phase and the aerosol phase. The experiments were performed in the large aerosol chamber at the FZ-Jülich at several relative humidities. Gas phase processes and the composition of the aerosols were monitored on-line simultaneously by FTIR spectroscopy and by Steam Jet Aerosol Collection/Ion Chromatography. The aerosol size distributions in the range of 20 nm to 5 μ m were measured by differential electromobility classification and by aerodynamic particle sizing. In the presence of aqueous bisulfate and sulfate aerosols a fast heterogeneous formation HNO3 is observed. (The reaction probability of N2O_5 is about 0.02.) In the case of the acidic bisulfate aerosols the major fraction of heterogeneously formed HNO3 resides in the gas phase. For neutral sulfate aerosols a significant fraction of HNO3 is taken up by the condensed phase of the aerosols. This leads to a distinctive growth of the aerosol population during the heterogeneous hydrolysis of N2O_5, which is observable in the number size distribution as well as in IR extinction measurements. The observed partitioning of HNO3 between gas phase and aqueous aerosol phase can be quantitatively understood by a Pitzer based thermodynamic model for salt solutions of high ionic strength. The model calculations and low resolution FTIR spectroscopy demonstrate that protonation of sulfate to bisulfate is the driving force for the uptake of HNO3 in neutral sulfate aerosols.

  2. Glass shards, pumice fragments and volcanic aerosol particles - diagenesis a recorder of volcanic activity?

    Science.gov (United States)

    Obenholzner, J. H.; Schroettner, H.; Poelt, P.; Delgado, H.

    2003-04-01

    Detailed SEM/EDS studies of Triassic (Southern Alps, A, I, Sl) and Miocene (Mixteca Alta, Mexico) tuffs revealed that volcanic glass shards can be replaced by zeolites (analcite), chlorites and smectites preserving the shape of primary shards (1). The Triassic pyroclastic deposits have been incorporated in the pre-Alpine burial diagenesis, the Miocene pyroclastic deposits are bentonites. The volcanologist is impressed by the circumstances that million years old pyroclast relict textures can be sized. Shape parameters obtained by image analysis can be compared with much younger pyroclastic deposits (2). Both deposits have not been effected by shearing. The alteration of pumice fragments of Triassic age is not a simple replacement process. Intergrowth of different illites and chlorites and probably vesicle filling by SiO2 and subsequent overgrowth make a reconstruction sometimes difficult. These processes are accompanied by the formation of REE-, Y- and Zr-bearing minerals as well as with the alteration of zircons. Studies of recently erupted ash from Popocatepetl volcano reveal the presence of a variety of µm-sized contact-metamorphosed clasts being a part of the volcanic ash (3). Such clasts should be present in many older pyroclastic deposits, especially where volcanoes had been situated on massive sedimentary units providing contact metamorphism in the realm of a magma chamber or during magma ascent. Volcanic aerosol particles collected in 1997 from the passively degassing plume of Popocatepetl volcano revealed in FESEM/EDS analysis (H. Schroettner and P. Poelt) a wide spectrum of fluffy, spherical and coagulated spherical particles (µm-sized). Under pre-vacuum conditions they remained stable for ca. 3 years (3). In nature the fate of these particles in the atmosphere is unknown. Are there relicts in marine, lacustrine sediments and ice cores, which could be used as proxies of volcanic activity? (1) Obenholzner &Heiken,1999. Ann.Naturhist.Mus.Wien, 100 A, 13

  3. An exploratory study of alkali sulfate aerosol formation during biomass combustion

    DEFF Research Database (Denmark)

    Løj, Lusi Hindiyarti; Frandsen, Flemming; Livbjerg, Hans;

    2008-01-01

    It is still in discussion to what extent alkali sulfate aerosols in biomass combustion are formed in the gas phase by a homogeneous mechanism or involve heterogeneous or catalyzed reactions. The present study investigates sulfate aerosol formation based on calculations with a detailed gas phase...... mechanism. The modeling predictions are compared to data from laboratory experiments and entrained flow reactor experiments available in the literature. The analysis support that alkali sulfate aerosols are formed from homogeneous nucleation following a series of steps occurring in the gas phase. The rate...

  4. Heterogenous uptake of gaseous N(sub 2)O(sub 5) by sulfate aerosols

    Science.gov (United States)

    Leu, M. -T.; Kane, S. M.; Caloz, F.

    2001-01-01

    The heterogeneous uptake of gaseous N sub 2 O sub 5 by ammonium sulfate, ammonium bisulfate, and sulfuric acid aerosols as a function of relative humididty has been investigated at room temperature and atmsopheric pressure.

  5. Sulfuric acid-ammonium sulfate aerosol: optical detection in the St. Louis region.

    Science.gov (United States)

    Charlson, R J; Vanderpol, A H; Covert, D S; Waggnoner, A P; Ahlquist, N C

    1974-04-12

    Nephelometric sensing of the deliquescence of ammonium sulfate produced by the reaction of sulfuric acid or ammonium bisulfate aerosol with ammonia provides a means for detecting these substances in air. Field experiments show them to be the dominant substances in the submicrometer, light-scattering aerosol in the St. Louis region.

  6. Particle size distribution and behavior of sulfate aerosols in a coastal region

    Energy Technology Data Exchange (ETDEWEB)

    Fujimura, M.; Hashimoto, Y.

    1979-01-01

    To obtain fundamental knowledge about sulfate aerosols, a field research was conducted in a coastal region distant from industrial pollution sources. The aerosol samples were analyzed for some elements, sulfate and ammonium ions. Sulfate was determined by the turbidimetry with 2-aminoperimidine, and ammonium was by the colorimetry of indophenol method. Trace elements with short-lived nuclides were analyzed by instrumental neutron activation analysis. The mass-size distribution curve of total aerosols was the general bimodal pattern, although the concentration level was very low. Most of sulfate and ammonium salts were distributed in the fine particle range less than 2 microns in aerodynamic diameter, but sulfate had another peak, thought to be of maritime origin, in the coarse particle range. Nevertheless, many fine sulfate particles that had been produced secondarily in the atmosphere were found in such a less polluted coastal region. The change of the sulfate concentrations obtained by the two-stage Andersen type sampler showed a correlation with the humidity. This may suggest that the formation of sulfate aerosols from sulfur dioxide could be related to a catalytic oxidation process in water drops.

  7. Total Volcanic Stratospheric Aerosol Optical Depths and Implications for Global Climate Change

    Science.gov (United States)

    Ridley, D. A.; Solomon, S.; Barnes, J. E.; Burlakov, V. D.; Deshler, T.; Dolgii, S. I.; Herber, A. B.; Nagai, T.; Neely, R. R., III; Nevzorov, A. V.; Ritter, C.; Sakai, T.; Santer, B. D.; Sato, M.; Schmidt, A.; Uchino, O.; Vernier, J. P.

    2014-01-01

    Understanding the cooling effect of recent volcanoes is of particular interest in the context of the post-2000 slowing of the rate of global warming. Satellite observations of aerosol optical depth above 15 km have demonstrated that small-magnitude volcanic eruptions substantially perturb incoming solar radiation. Here we use lidar, Aerosol Robotic Network, and balloon-borne observations to provide evidence that currently available satellite databases neglect substantial amounts of volcanic aerosol between the tropopause and 15 km at middle to high latitudes and therefore underestimate total radiative forcing resulting from the recent eruptions. Incorporating these estimates into a simple climate model, we determine the global volcanic aerosol forcing since 2000 to be 0.19 +/- 0.09W/sq m. This translates into an estimated global cooling of 0.05 to 0.12 C. We conclude that recent volcanic events are responsible for more post-2000 cooling than is implied by satellite databases that neglect volcanic aerosol effects below 15 km.

  8. The role of sulfate aerosol in the formation of cloudiness over the sea

    Science.gov (United States)

    Aloyan, A. E.; Yermakov, A. N.; Arutyunyan, V. O.

    2016-07-01

    We estimate the impact of sulfate aerosols on cloudiness formation over the sea in the middle troposphere and the involvement of these particles in the formation of polar stratospheric clouds (PSCs) in the lower stratosphere. The first of these problems is solved using a combined model of moist convection and the formation of cloudiness and sulfate aerosols in the troposphere and lower stratosphere over the sea, incorporating natural emissions of sulfur-containing compounds. We have found that a significant source of condensation nuclei in the troposphere is the photochemical transformation of biogenic dimethyl sulfide (in addition to NaCl). The results of numerical experiments indicate that the absence of sulfate aerosols hinders the cloudiness formation over the sea in the middle and upper troposphere. The problem of sulfate aerosol involvement in the formation of supercooled ternary solutions (STSs) (PSC Type Ib) in the lower stratosphere is solved using a mathematical model of global transport of multicomponent gas pollutants and aerosols in the atmosphere. Using the combined model, numerical experiments were performed for the winter season in both hemispheres. Sulfate aerosols were found to really participate in the formation of STS particles. Without their participation, the formation of STS particles in the lower stratosphere would be hindered. We present the results of numerical calculations and discuss the distribution of concentrations of gaseous nitric and sulfuric acids, as well as mass concentrations of these components in STS particles.

  9. High aerosol acidity despite declining atmospheric sulfate concentrations over the past 15 years

    Science.gov (United States)

    Weber, Rodney J.; Guo, Hongyu; Russell, Armistead G.; Nenes, Athanasios

    2016-04-01

    Particle acidity affects aerosol concentrations, chemical composition and toxicity. Sulfate is often the main acid component of aerosols, and largely determines the acidity of fine particles under 2.5 μm in diameter, PM2.5. Over the past 15 years, atmospheric sulfate concentrations in the southeastern United States have decreased by 70%, whereas ammonia concentrations have been steady. Similar trends are occurring in many regions globally. Aerosol ammonium nitrate concentrations were assumed to increase to compensate for decreasing sulfate, which would result from increasing neutrality. Here we use observed gas and aerosol composition, humidity, and temperature data collected at a rural southeastern US site in June and July 2013 (ref. ), and a thermodynamic model that predicts pH and the gas-particle equilibrium concentrations of inorganic species from the observations to show that PM2.5 at the site is acidic. pH buffering by partitioning of ammonia between the gas and particle phases produced a relatively constant particle pH of 0-2 throughout the 15 years of decreasing atmospheric sulfate concentrations, and little change in particle ammonium nitrate concentrations. We conclude that the reductions in aerosol acidity widely anticipated from sulfur reductions, and expected acidity-related health and climate benefits, are unlikely to occur until atmospheric sulfate concentrations reach near pre-anthropogenic levels.

  10. Importance of tropospheric volcanic aerosol for indirect radiative forcing of climate

    Directory of Open Access Journals (Sweden)

    A. Schmidt

    2012-03-01

    Full Text Available Observations and models have shown that continuously degassing volcanoes have a potentially large effect on the natural background aerosol loading and the radiative state of the atmosphere. Here, we use a global aerosol microphysics model to quantify the impact of these volcanic emissions on the cloud albedo radiative forcing under pre-industrial (PI and present-day (PD conditions. We find that volcanic degassing increases global annual mean cloud droplet number concentrations by 40% under PI conditions, but by only 10% under PD conditions. Consequently, volcanic degassing causes a global annual mean cloud albedo effect of −1.06 W m−2 in the PI era but only −0.56 W m−2 in the PD era. This non-equal effect is explained partly by the lower background aerosol concentrations in the PI era, but also because more aerosol particles are produced per unit of volcanic sulphur emission in the PI atmosphere. The higher sensitivity of the PI atmosphere to volcanic emissions has an important consequence for the anthropogenic cloud radiative forcing because the large uncertainty in volcanic emissions translates into an uncertainty in the PI baseline cloud radiative state. Assuming a −50/+100% uncertainty range in the volcanic sulphur flux, we estimate the annual mean anthropogenic cloud albedo forcing to lie between −1.16 W m−2 and −0.86 W m−2. Therefore, the volcanically induced uncertainty in the PI baseline cloud radiative state substantially adds to the already large uncertainty in the magnitude of the indirect radiative forcing of climate.

  11. Effects of El Chichon volcanic effluents on stratospheric aerosol dynamics

    Science.gov (United States)

    Pueschel, R. F.; Snetsinger, K. G.; Russell, P. B.; Oberbeck, V. R.; Livingston, J. M.

    1988-01-01

    The effects of El Chichon's April 1982 eruption on stratospheric aerosol dynamics are presently discussed in terms of log-normal size distributions over 15-20 km sample altitudes between 30 and 45 deg N over the contiguous U.S. After collection, samples were studied by SEM, and log-normal size distributions were fitted to the data-points obtained. It is found that stratospheric aerosol behavior is explainable by the laws of aerosol mechanics more easily than has been the case for tropospheric aerosol, for which the source-sink relationship is much more complex.

  12. Lidar Observations of Stratospheric Aerosol Layer After the Mt. Pinatubo Volcanic Eruption

    Science.gov (United States)

    Nagai, Tomohiro; Uchino, Osamu; Fujimoto, Toshifumi

    1992-01-01

    The volcano Mt. Pinatubo located on the Luzon Island, Philippines, had explosively erupted on June 15, 1991. The volcanic eruptions such as volcanic ash, SO2 and H2O reached into the stratosphere over 30 km altitude by the NOAA-11 satellite observation and this is considered one of the biggest volcanic eruptions in this century. A grandiose volcanic eruption influences the atmosphere seriously and causes many climatic effects globally. There had been many impacts on radiation, atmospheric temperature and stratospheric ozone after some past volcanic eruptions. The main cause of volcanic influence depends on stratospheric aerosol, that stay long enough to change climate and other meteorological conditions. Therefore it is very important to watch stratospheric aerosol layers carefully and continuously. Standing on this respect, we do not only continue stratospheric aerosol observation at Tsukuba but also have urgently developed another lidar observational point at Naha in Okinawa Island. This observational station could be thought valuable since there is no lidar observational station in this latitudinal zone and it is much nearer to Mt. Pinatubo. Especially, there is advantage to link up these two stations on studying the transportation mechanism in the stratosphere. In this paper, we present the results of lidar observations at Tsukuba and Naha by lidar systems with Nd:YAG laser.

  13. Volcanic aerosol and ozone depletion within the Antarctic polar vortex during the austral spring of 1991

    Energy Technology Data Exchange (ETDEWEB)

    Deshler, T.; Adriani, A.; Gobbi, G.P.; Hofmann, D.J.; Donfrancesco, G. di; Johnson, B.J. (Wyoming Univ., Laramie (United States) CNR, Ist. de Fisica dell' Atmosfera, Frascati (Italy) NOAA, Climate Monitoring and Diagnostics Lab., Boulder, CO (United States) ENEA, Centro Ricerche Energia Casaccia, Rome (Italy))

    1992-09-01

    In the spring of 1991 the Antarctic lower stratosphere was characterized by a layer of volcanic aerosol from the Cerro Hudson eruption. This aerosol layer was observed from McMurdo Station, Antarctica, with both lidar and balloonborne particle counters beginning around 10 September. After 20 September the aerosol was observed daily between 9 and 13 km. In this layer homogeneous nucleation of new aerosol was observed with concentrations greater than 6000/cu cm. Comparisons of scattering ratio calculated from measured particle size distributions agree best with the lidar measurements when a real index of refraction near 1.5 is used. In the past 5 years of measurements, ozone below 13 km has been relatively unchanged during the annual Antartic ozone depletion; however, in 1991 ozone below 13 km decreased at a rate of 4 - 8 ppb/day over 30 days. This change began shortly after the appearance of the volcanic aerosol, providing direct measurements correlating volcanic aerosol and ozone depletion. 16 refs.

  14. THE IMPACT OF RELATIVE HUMIDITY ON THE RADIATIVE PROPERTY AND RADIATIVE FORCING OF SULFATE AEROSOL

    Institute of Scientific and Technical Information of China (English)

    张立盛; 石广玉

    2001-01-01

    With the data of complex refractive index of sulfate aerosol, the radiative properties of the aerosol under 8 relative humidity conditions are calculated in this paper. By using the concentration distribution from two CTM models and LASG GOALS/AGCM, the radiative forcing due to hygroscopic sulfate aerosol is simulated. The results show that: (1) With the increase of relative humidity, the mass extinction coefficiency factor decreases in the shortwave spectrum: single scattering albedo keeps unchanged except for a little increase in longwave spectrum, and asymmetry factor increases in whole spectrum. (2) Larger differences occur in radiative forcing simulated by using two CTM data, and the global mean forcing is -0. 268 and -0. 816 W/m2,respectively. (3) When the impact of relative humidity on radiative property is taken into account,the distribution pattern of radiative forcing due to the wet particles is very similar to that of dry sulfate, but the forcing value decreases by 6%.

  15. Parameterization of the Optical Properties of Sulfate Aerosols in the Infrared.

    Science.gov (United States)

    Li, J.; Min, Qilong

    2002-11-01

    Parameterizations of absorptance depth for ammonium sulfate [(NH4)2SO4], ammonium bisulfate (NH4HSO4), and sulfuric acid (H2SO4) in the infrared are provided for an eight-band model (covering 340-2500 cm1) and for 32 individual wavenumbers in order to generate other band schemes. The parameterization is simple in form and in its dependence on relative humidity.It is found that the aerosol surface infrared forcing can cancel about 12%-24% aerosol surface solar forcing in a clear sky condition. Also the existence of clouds could enhance the ratio of aerosol surface infrared forcing to the aerosol surface solar forcing. In contrast to the solar case, a small mode size distribution does not always produce a larger aerosol surface forcing. Also it is found that the aerosol surface forcing is dependent on the aerosol location. Very simple analysis is presented to help understand the related physics on sulfate aerosol infrared radiative forcing.

  16. Effective Henry's law partitioning and the salting constant of glyoxal in aerosols containing sulfate.

    Science.gov (United States)

    Kampf, Christopher J; Waxman, Eleanor M; Slowik, Jay G; Dommen, Josef; Pfaffenberger, Lisa; Praplan, Arnaud P; Prévôt, André S H; Baltensperger, Urs; Hoffmann, Thorsten; Volkamer, Rainer

    2013-05-07

    The reversible partitioning of glyoxal was studied in simulation chamber experiments for the first time by time-resolved measurements of gas-phase and particle-phase concentrations in sulfate-containing aerosols. Two complementary methods for the measurement of glyoxal particle-phase concentrations are compared: (1) an offline method utilizing filter sampling of chamber aerosols followed by HPLC-MS/MS analysis and (2) positive matrix factorization (PMF) analysis of aerosol mass spectrometer (AMS) data. Ammonium sulfate (AS) and internally mixed ammonium sulfate/fulvic acid (AS/FA) seed aerosols both show an exponential increase of effective Henry's law coefficients (KH,eff) with AS concentration (cAS, in mol kg(-1) aerosol liquid water, m = molality) and sulfate ionic strength, I(SO4(2-)) (m). A modified Setschenow plot confirmed that "salting-in" of glyoxal is responsible for the increased partitioning. The salting constant for glyoxal in AS is K(S)CHOCHO = (-0.24 ± 0.02) m(-1), and found to be independent of the presence of FA. The reversible glyoxal uptake can be described by two distinct reservoirs for monomers and higher molecular weight species filling up at characteristic time constants. These time constants are τ1 ≈ 10(2) s and τ2 ≈ 10(4) s at cAS < 12 m, and about 1-2 orders of magnitude slower at higher cAS, suggesting that glyoxal uptake is kinetically limited at high salt concentrations.

  17. Airway responses to sulfate and sulfuric acid aerosols in asthmatics. An exposure-response relationship.

    Science.gov (United States)

    Utell, M J; Morrow, P E; Speers, D M; Darling, J; Hyde, R W

    1983-09-01

    Epidemiologic studies support an association between elevated levels of sulfates and increased symptoms in asthmatics. To determine if these pollutants produce airway responses, 17 asthmatics inhaled the following sulfates: sodium bisulfate, ammonium sulfate, ammonium bisulfate (NH4HSO4), or sulfuric acid (H2SO4) aerosols with an aerodynamic diameter of 0.80 micron at concentrations of 100 micrograms/m3, 450 micrograms/m3, and 1,000 micrograms/m3. A sodium chloride (NaCl) aerosol of similar characteristics, administered by double-blind randomization, served as a control. Subjects breathed these aerosols for a 16-minute period via a mouthpiece. Deposition studies showed 54 to 65% retention of the inhaled aerosols. At the 1,000 micrograms/m3 concentration, the Threshold Limit Value for occupational exposure, H2SO4 and NH4HSO4 inhalation produced significant reductions in specific airway conductance (SGaw) (p less than 0.05) and forced expiratory volume in one second (p less than 0.01) compared with NaCl or pre-exposure values. At the 450 micrograms/m3 concentration, only H2SO4 inhalation produced a significant reduction in SGaw (p less than 0.01). At 100 micrograms/m3, a level 3 to 5 times greater than peak urban levels, no significant change in airway function occurred after any sulfate exposure. These data indicate that asthmatics demonstrate bronchoconstriction after brief exposure to common acidic sulfate pollutants.

  18. Massive Volcanic SO2 Oxidation and Sulphate Aerosol Deposition in Cenozoic North America

    Science.gov (United States)

    Volcanic eruptions release a large amount of sulphur dioxide (SO2) into the atmosphere. SO2 is oxidized to sulphate and can subsequently form sulphate aerosol, which can affect the Earth's radiation balance, biologic productivity and high-altitude ozone co...

  19. Second organic aerosol formation from the ozonolysis of α-pinene in the presence of dry submicron ammonium sulfate aerosol

    Institute of Scientific and Technical Information of China (English)

    ZHAO Zhe; HAO Jiming; LI Junhua; WU Shan

    2008-01-01

    An indoor chamber facility is described for investigation of atmospheric aerosol chemistry. Two sets of α-pinene ozonolysisexperiments were conducted in the presence of dry ammonium sulfate seed particle: ozone limited experiments and α-pinene limitedexperiments. The concentration of gas phase and particle phase species was monitored continuously by on-line instruments andrecorded automatically by data sampling system. The evolution of size distribution was measured by a scanning mobility particlesizer (SMPS), and α-pinene consumed was measured using GC-FID. Secondary organic aerosol (SOA) produced for seed-free systemis 100% organic in content, resulting from a sufficient supersaturation of low volatility organics to produce homogeneous nucleationfollowed by condensation to the aerosol. Secondary organic aerosol produced in seeded system is a mixture of organic and inorganicconstituents, initially forms via condensation onto the inorganic particles, and subsequent growth occurs via absorption into the organicsurface coating the inorganic core. Although the formation process and the size distribution for seed-free system and seeded system isdifferent, the ultimate mass of SOA formed is equal, and SOA yield for the two system located in the same regression line when usingone-product model, suggesting that the presence of dry ammonium sulfate seed has no measurable effect on the total aerosol yield, and the dry seed particle acts solely as a site upon which organic deposition occurs.

  20. INVESTIGATION ON PROPERTIES OF CONCRETE CONTAINING NATURAL POZZOLAN VOLCANIC ORIGIN DUE TO SULFATE ATTACK

    Directory of Open Access Journals (Sweden)

    MERIDA AHCENE

    2013-05-01

    Full Text Available Sulfate attack and its effects are important from both scientific and industrial viewpoints. It is perceived that concretes containing pozzolan have better performance in sulfate solutions, since the pozzolanic reactions reduce the quantity of calcium hydroxide and increase calcium silicate hydrate. This paper investigates thecontribution of natural pozzolan volcanic origin on the physico - mechanical and physico-chemical characteristics of the concretes. When it is coupled to a water reducing superplasticizer by a correct adjustment of the composition, it greatly improves the concrete properties. The analysis of the experimental results on pozzolan concrete at 5% content and sharpness of 9600cm2/g, in a sulphated environment, showed that it contributes positively to the improvement of its mechanical characteristics and its durability with respect towater absorption, and to the permeability to the chlorine ions as well as to the resistance to the sulphates.

  1. Effect of sulfate aerosol on tropospheric NOx and ozone budgets: Model simulations and TOPSE evidence

    Science.gov (United States)

    Tie, Xuexi; Emmons, Louisa; Horowitz, Larry; Brasseur, Guy; Ridley, Brian; Atlas, Elliot; Stround, Craig; Hess, Peter; Klonecki, Andrzej; Madronich, Sasha; Talbot, Robert; Dibb, Jack

    2003-02-01

    The distributions of NOx and O3 are analyzed during TOPSE (Tropospheric Ozone Production about the Spring Equinox). In this study these data are compared with the calculations of a global chemical/transport model (Model for OZone And Related chemical Tracers (MOZART)). Specifically, the effect that hydrolysis of N2O5 on sulfate aerosols has on tropospheric NOx and O3 budgets is studied. The results show that without this heterogeneous reaction, the model significantly overestimates NOx concentrations at high latitudes of the Northern Hemisphere (NH) in winter and spring in comparison to the observations during TOPSE; with this reaction, modeled NOx concentrations are close to the measured values. This comparison provides evidence that the hydrolysis of N2O5 on sulfate aerosol plays an important role in controlling the tropospheric NOx and O3 budgets. The calculated reduction of NOx attributed to this reaction is 80 to 90% in winter at high latitudes over North America. Because of the reduction of NOx, O3 concentrations are also decreased. The maximum O3 reduction occurs in spring although the maximum NOx reduction occurs in winter when photochemical O3 production is relatively low. The uncertainties related to uptake coefficient and aerosol loading in the model is analyzed. The analysis indicates that the changes in NOx due to these uncertainties are much smaller than the impact of hydrolysis of N2O5 on sulfate aerosol. The effect that hydrolysis of N2O5 on global NOx and O3 budgets are also assessed by the model. The results suggest that in the Northern Hemisphere, the average NOx budget decreases 50% due to this reaction in winter and 5% in summer. The average O3 budget is reduced by 8% in winter and 6% in summer. In the Southern Hemisphere (SH), the sulfate aerosol loading is significantly smaller than in the Northern Hemisphere. As a result, sulfate aerosol has little impact on NOx and O3 budgets of the Southern Hemisphere.

  2. Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NOx photooxidation

    Institute of Scientific and Technical Information of China (English)

    Biwu CHU; Jiming HAO; Junhua LI; Hideto TAKEKAWA; Kun WANG; Jingkun JIANG

    2013-01-01

    Aerosol phase reactions play a very important role on secondary organic aerosol (SOA) formation, and metal-containing aerosols are important components in the atmosphere. In this study, we tested the effects of two transition metal sulfate salts, manganese sulfate (MnSO4) and zinc sulfate (ZnSO4), on the photochemical reactions of a toluene/NOx photooxidation system in a 2 m3 smog chamber. By comparing photochemical reaction products of experiments with and without transition metal sulfate seed aerosols, we evaluated the effects of transition metal sulfate seed aerosols on toluene consumption, NOx conversion and the formation of ozone and SOA. MnSO4 and ZnSO4 seed aerosols were found to have similar effects on photochemical reactions, both enhance the SOA production, while showing negligible effects on the gas phase compounds. These observations are consistent when varying metal sulfate aerosol concentrations. This is attributed to the catalytic effects of MnSO4 and ZnSO4 seed aerosols which may enhance the formation of condensable semivolatile compounds. Their subsequent partitioning into the aerosol phase leads to the observed SOA formation enhancement.

  3. Characteristics of Anthropogenic Sulfate and Carbonaceous Aerosols over East Asia: Regional Modeling and Observation

    Institute of Scientific and Technical Information of China (English)

    Yan HUANG; William L. CHAMEIDES; Qian TAN; Robert E. DICKINSON

    2008-01-01

    The authors present spatial and temporal characteristics of anthropogenic sulfate and carbonaceous aerosols over East Asia using a 3-D coupled regional climate-chemistry-aerosol model, and compare the simulation with the limited aerosol observations over the region. The aerosol module consists of SO2, SO42-, hydrophobic and hydrophilic black carbon (BC) and organic carbon compounds (OC), including emission, advections, dry and wet deposition, and chemical production and conversion. The simulated patterns of SO2 are closely tied to its emission rate, with sharp gradients between the highly polluted regions and more rural areas. Chemical conversion (especially in the aqueous phase) and dry deposition remove 60% and 30% of the total SO2 emission, respectively. The SO42- shows less horizontal gradient and seasonality than SO2, with wet deposition (60%) and export (27%) being two major sinks. Carbonaceous aerosols are spatially smoother than sulfur species. The aging process transforms more than 80% of hydrophobic BC and OC to hydrophilic components, which are removed by wet deposition (60%) and export (30%). The simulated spatial and seasonal SO42-, BC and OC aerosol concentrations and total aerosol optical depth are generally consistent with the observations in rural areas over East Asia, with lower bias in simulated OC aerosols, likely due to the underestimation of anthropogenic OC emissions and missing treatment of secondary organic carbon. The results suggest that our model is a useful tool for characterizing the anthropogenic aerosol cycle and for assessing its potential climatic and environmental effects in future studies.

  4. Using stable isotopes to trace sources and formation processes of sulfate aerosols from Beijing, China.

    Science.gov (United States)

    Han, Xiaokun; Guo, Qingjun; Liu, Congqiang; Fu, Pingqing; Strauss, Harald; Yang, Junxing; Hu, Jian; Wei, Lianfang; Ren, Hong; Peters, Marc; Wei, Rongfei; Tian, Liyan

    2016-07-20

    Particulate pollution from anthropogenic and natural sources is a severe problem in China. Sulfur and oxygen isotopes of aerosol sulfate (δ(34)Ssulfate and δ(18)Osulfate) and water-soluble ions in aerosols collected from 2012 to 2014 in Beijing are being utilized to identify their sources and assess seasonal trends. The mean δ(34)S value of aerosol sulfate is similar to that of coal from North China, indicating that coal combustion is a significant contributor to atmospheric sulfate. The δ(34)Ssulfate and δ(18)Osulfate values are positively correlated and display an obvious seasonality (high in winter and low in summer). Although an influence of meteorological conditions to this seasonality in isotopic composition cannot be ruled out, the isotopic evidence suggests that the observed seasonality reflects temporal variations in the two main contributions to Beijing aerosol sulfate, notably biogenic sulfur emissions in the summer and the increasing coal consumption in winter. Our results clearly reveal that a reduction in the use of fossil fuels and the application of desulfurization technology will be important for effectively reducing sulfur emissions to the Beijing atmosphere.

  5. TOTAL PARTICLE, SULFATE, AND ACIDIC AEROSOL EMISSIONS FROM KEROSENE SPACE HEATERS

    Science.gov (United States)

    Chamber studies were conducted on four unvented kerosene space heaters to assess emissions of total particle, sulfate, and acidic aerosol. The heaters tested represented four burner designs currently in use by the public. Kerosene space heaters are a potential source of fine part...

  6. Using stable isotopes to trace sources and formation processes of sulfate aerosols from Beijing, China

    Science.gov (United States)

    Han, Xiaokun; Guo, Qingjun; Liu, Congqiang; Fu, Pingqing; Strauss, Harald; Yang, Junxing; Hu, Jian; Wei, Lianfang; Ren, Hong; Peters, Marc; Wei, Rongfei; Tian, Liyan

    2016-07-01

    Particulate pollution from anthropogenic and natural sources is a severe problem in China. Sulfur and oxygen isotopes of aerosol sulfate (δ34Ssulfate and δ18Osulfate) and water-soluble ions in aerosols collected from 2012 to 2014 in Beijing are being utilized to identify their sources and assess seasonal trends. The mean δ34S value of aerosol sulfate is similar to that of coal from North China, indicating that coal combustion is a significant contributor to atmospheric sulfate. The δ34Ssulfate and δ18Osulfate values are positively correlated and display an obvious seasonality (high in winter and low in summer). Although an influence of meteorological conditions to this seasonality in isotopic composition cannot be ruled out, the isotopic evidence suggests that the observed seasonality reflects temporal variations in the two main contributions to Beijing aerosol sulfate, notably biogenic sulfur emissions in the summer and the increasing coal consumption in winter. Our results clearly reveal that a reduction in the use of fossil fuels and the application of desulfurization technology will be important for effectively reducing sulfur emissions to the Beijing atmosphere.

  7. The impact of dust on sulfate aerosol, CN and CCN during an East Asian dust storm

    Science.gov (United States)

    Manktelow, P. T.; Carslaw, K. S.; Mann, G. W.; Spracklen, D. V.

    2010-01-01

    A global model of aerosol microphysics is used to simulate a large East Asian dust storm during the ACE-Asia experiment. We use the model together with size resolved measurements of aerosol number concentration and composition to examine how dust modified the production of sulfate aerosol and the particle size distribution in East Asian outflow. Simulated size distributions and mass concentrations of dust, sub- and super-micron sulfate agree well with observations from the C-130 aircraft. Modeled mass concentrations of fine sulfate (Dp1.0 μm) by more than an order of magnitude, but total sulfate concentrations increase by less than 2% because decreases in fine sulfate have a compensating effect. Our analysis shows that the sulfate associated with dust can be explained largely by the uptake of H2SO4 rather than reaction of SO2 on the dust surface, which we assume is suppressed once the particles are coated in sulfate. We suggest that many previous model investigations significantly overestimated SO2 oxidation on East Asian dust, possibly due to the neglect of surface saturation effects. We extend previous model experiments by examining how dust modified existing particle concentrations in Asian outflow. Total particle concentrations (condensation nuclei, CN) modeled in the dust-pollution plume are reduced by up to 20%, but we predict that dust led to less than 10% depletion in particles large enough to act as cloud condensation nuclei (CCN). Our analysis suggests that E. Asian dust storms have only a minor impact on sulfate particles present at climate-relevant sizes.

  8. The effect of volcanic aerosols on the thermal infrared budget of the lower stratosphere

    Science.gov (United States)

    Charlock, T. P.

    1983-01-01

    The thermal IR heating of the stratosphere due to volcanic aerosols such as those released by the eruption of El Chichon is investigated by means of clear-sky model computations using a LOWTRAN5 radiance code (Kneizys et al., 1980) modified by Charlock (1983) to increase its vertical resolution. The results are presented graphically for 4-km-thick aerosol layers at altitudes 18, 22, and 25 km and at latitudes 0 deg and 35 deg N, and the effects of tropospheric cloud height (0-10 km) are taken into account. The aerosol-induced IR divergence is shown to depend on aerosol height and to be highly and nonlinearly sensitive to the location of underlying water clouds.

  9. Modeling the spectral optical properties of ammonium sulfate and biomass burning aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Grant, K.E.; Chuang, C.C.; Grossman, A.S.; Penner, J.E. [Michigan Univ., Ann Arbor, MI (United States)

    1997-09-01

    The importance of including the global and regional radiative effects of aerosols in climate models has increasingly been realized. Accurate modeling of solar radiative forcing due to aerosols from anthropogenic sulfate and biomass burning emissions requires adequate spectral resolution and treatment of spatial and temporal variability. The variation of aerosol spectral optical properties with local relative humidity and dry aerosol composition must be considered. Because the cost of directly including Mie calculations within a climate model is prohibitive, parameterizations from offline calculations must be used. Starting from a log-normal size distribution of dry ammonium sulfate, we developed optical properties for tropospheric sulfate aerosol at 15 relative humidities up to 99 percent. The resulting aerosol size distributions were then used to calculate bulk optical properties at wavelengths between 0.175 {micro}m and 4 {micro}m. Finally, functional fits of optical properties were made for each of 12 wavelength bands as a function of relative humidity. Significant variations in optical properties occurred across the total solar spectrum. Relative increases in specific extinction and asymmetry factor with increasing relative humidity became larger at longer wavelengths. Significant variation in single-scattering albedo was found only in the longest near-IR band. This is also the band with the lowest albedo. A similar treatment was done for aerosols from biomass burning. In this case, size distributions were taken as having two carbonaceous size modes and a larger dust mode. The two carbonaceous modes were considered to be humidity dependent. Equilibrium size distributions and compositions were calculated for 15 relative humidities and five black carbon fractions. Mie calculations and Chandrasekhar averages of optical properties were done for each of the resulting 75 cases. Finally, fits were made for each of 12 spectral bands as functions of relative humidity

  10. Evidence for surface nucleation: efflorescence of ammonium sulfate and coated ammonium sulfate aerosol particles

    Science.gov (United States)

    Ciobanu, V. Gabriela; Marcolli, Claudia; Krieger, Ulrich K.; Zuend, Andreas; Peter, Thomas

    2010-05-01

    Aerosol particles are ubiquitous in the atmosphere and can undergo different phase transitions, such as deliquescence and efflorescence. Using optical microscopy, we investigated the efflorescence of ammonium sulfate (AS) in supersaturated AS and 1:1 and 8:1 (by weight) poly(ethylene glycol)-400 (PEG-400)/AS particles, which were deposited as droplets with diameters in the 16 - 35 μm range on a hydrophobically coated slide. The PEG-400/AS particles that are exposed to decreasing relative humidity (RH) exhibit a liquid-liquid phase separation below 90 % RH with the PEG-400 phase surrounding the aqueous AS inner phase (Marcolli and Krieger, 2006; Ciobanu et al., 2009). Pure AS particles effloresced in the RH range from 36.3 to 43.7 % RH, in agreement with literature data (31 - 48 % RH). In contrast, 1:1 PEG-400/AS particles with diameters of the AS phase from 7.2 - 19.2 μm effloresced between 26.8 - 33.9 % RH and 8:1 PEG-400/AS particles with diameters of the AS phase from 1.8 - 7.3 μm between 24.3 - 29.3 % RH. Such low efflorescence relative humidity (ERH) values have never been reached before for AS particles of this size range. We show that neither a potential inhibition of water evaporation via anomalously slow diffusion through the PEG coating, nor the presence of low amounts of PEG-400 in the AS phase, nor different timescales between various experimental techniques could possibly explain the low AS ERH values of PEG-400/AS particles in our setup. High-speed photography of the efflorescence process allowed to monitor the proceeding of the AS crystallization fronts within the particles with millisecond time resolution. The nucleation locations were deduced based on the initial crystals growth locations. Statistical analysis of 31 and 19 efflorescence events for pure AS and 1:1 PEG-400/AS particles, respectively, identified the air/droplet/substrate contact line and the air/droplet interface as preferred nucleation locations in the case of pure AS particles

  11. Comparative irritant potency of inhaled sulfate aerosols--effects on bronchial mucociliary clearance.

    Science.gov (United States)

    Schlesinger, R B

    1984-08-01

    The effect of 1-hr oral inhalation exposures to submicrometer aerosols of ammonium bisulfate (NH4HSO4), ammonium sulfate [NH4)2SO4), and sodium sulfate (Na2SO4) upon mucociliary clearance from the bronchial tree of rabbits was examined. Exposures to NH4HSO4 at concentrations of approximately 600-1700 micrograms/m3 produced a significant depression of clearance rate only at the highest exposure level. No significant effects were observed with the other sulfates at levels up to approximately 2000 micrograms/m3. When results were compared to those from another study in this laboratory using sulfuric acid (H2SO4) aerosol, the ranking of irritant potency was H2SO4 greater than NH4HSO4 greater than (NH4)2SO4, Na2SO4. Alteration in bronchial mucociliary clearance due to sulfate aerosols appears to be related to the deposition of [H+] on the mucus lining of conducting airways.

  12. Evaluating Ammonium, Nitrate and Sulfate Aerosols in 3-Dimensions

    Science.gov (United States)

    Mezuman, Keren; Bauer, Susanne E.; Tsigaridis, Kostas

    2015-01-01

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

  13. Understanding Hydrological and Climate Conditions on Early Mars Through Sulfate Cycling and Microbial Activity in Terrestrial Volcanic Systems

    Science.gov (United States)

    Szynkiewicz, A.; Mikucki, J.; Vaniman, D.

    2017-10-01

    Our study is a type of Earth-based investigation in a Mars-analog environment that allows for determination of how changing wet and dry conditions in active volcanic/hydrothermal system affect sulfate fluxes into surface water and groundwater.

  14. Cloud, Aerosol, and Volcanic Ash Retrievals Using ASTR and SLSTR with ORAC

    Science.gov (United States)

    McGarragh, Gregory; Poulsen, Caroline; Povey, Adam; Thomas, Gareth; Christensen, Matt; Sus, Oliver; Schlundt, Cornelia; Stapelberg, Stefan; Stengel, Martin; Grainger, Don

    2015-12-01

    The Optimal Retrieval of Aerosol and Cloud (ORAC) is a generalized optimal estimation system that retrieves cloud, aerosol and volcanic ash parameters using satellite imager measurements in the visible to infrared. Use of the same algorithm for different sensors and parameters leads to consistency that facilitates inter-comparison and interaction studies. ORAC currently supports ATSR, AVHRR, MODIS and SEVIRI. In this proceeding we discuss the ORAC retrieval algorithm applied to ATSR data including the retrieval methodology, the forward model, uncertainty characterization and discrimination/classification techniques. Application of ORAC to SLSTR data is discussed including the additional features that SLSTR provides relative to the ATSR heritage. The ORAC level 2 and level 3 results are discussed and an application of level 3 results to the study of cloud/aerosol interactions is presented.

  15. NUMERICAL SIMULATION WITH A COMPREHENSIVE CHEMICAL TRANSPORT MODEL OF NITRATE, SULFATE, AND AMMONIUM AEROSOL DISTRIBUTIONS OVER EAST ASIA

    Institute of Scientific and Technical Information of China (English)

    Meigen Zhang

    2005-01-01

    The transport and chemical production processes of nitrate, sulfate, and ammonium aerosols over East Asia were investigated by use of the Models-3 Community Multi-scale Air Quality (CMAQ) modeling system coupled with the Regional Atmospheric Modeling System (RAMS). For the evaluation of the model's ability in depicting their3-dimensional concentration distributions and temporal variations, modeled concentrations of nitrate, sulfate, and ammonium aerosols are compared with the observations obtained at a ground station in Japan in March 2001 and onboard of an aircraft DC-8 on 18 and 21 March 2001 during the Transport and Chemical Evolution over the Pacific (TRACE-P)field campaign. Comparison shows that simulated values of nitrate, sulfate, and ammonium aerosols are generally in good agreement with their observed data, and the model captures most important observed features, and reproduces temporal and spatial variations of nitrate, sulfate, and ammonium aerosol concentrations reasonably well, e.g., the timing and locations of the concentration spikes of nitrate, sulfate, and ammonium aerosols are well reproduced, but large discrepancies between observed and simulated values are also clearly seen at some points and some times due to the coarse grid resolution and uncertainties of the emissions used in this study. This comparison results indicate that CMAQ is able to simulate the distributions of nitrate, sulfate, and ammonium aerosols and their related species in the troposphere over East Asia reasonably well.

  16. Effects of sulfate aerosol forcing on East Asian summer monsoon for 1985-2010

    Science.gov (United States)

    Kim, Minjoong J.; Yeh, Sang-Wook; Park, Rokjin J.

    2016-02-01

    We examine the effect of anthropogenic aerosol forcing on the East Asian summer monsoon (EASM) using the Community Atmosphere Model version 5.1.1. One control and two sensitivity model experiments were conducted in order to diagnose the separate roles played by sea surface temperature (SST) variations and anthropogenic sulfate aerosol forcing changes in East Asia. We find that the SST variation has been a major driver for the observed weakening of the EASM, whereas the effect of the anthropogenic aerosol forcing has been opposite and has slightly intensified the EASM over the recent decades. The reinforcement of the EASM results from radiative cooling by the sulfate aerosol forcing, which decelerates the jet stream around the jet's exit region. Subsequently, the secondary circulation induced by such a change in the jet stream leads to the increase in precipitation around 18-23°N. This result indicates that the increase in anthropogenic emissions over East Asia may play a role in compensating for the weakening of the EASM caused by the SST forcing.

  17. Ice Formation by Sulfate and Sulfuric Acid Aerosol Particles under Upper-Tropospheric Conditions.

    Science.gov (United States)

    Chen, Yalei; Demott, Paul J.; Kreidenweis, Sonia M.; Rogers, David C.; Eli Sherman, D.

    2000-11-01

    Ice formation in ammoniated sulfate and sulfuric acid aerosol particles under upper-tropospheric conditions was studied using a continuous flow thermal diffusion chamber. This technique allowed for particle exposure to controlled temperatures and relative humidities for known residence times. The phase states of (NH4)2SO4 and NH4HSO4 particles were found to have important impacts on their ice formation capabilities. Dry (NH4)2SO4 particles nucleated ice only at high relative humidity (RH 94%) with respect to water at temperatures between 40° and 60°C. This result suggested either an impedance or finite time dependence to deliquescence and subsequent homogeneous freezing nucleation. Ammonium sulfate particles that entered the diffusion chamber in a liquid state froze homogeneously at relative humidities that were 10% lower than where ice nucleated on initially dry particles. Likewise, crystalline or partially crystallized (as letovicite) NH4HSO4 particles required higher relative humidities for ice nucleation than did initially liquid bisulfate particles. Liquid particles of size 0.2 m composed of either ammonium sulfate or bisulfate froze at lower relative humidity at upper-tropospheric temperatures than did 0.05-m sulfuric acid aerosol particles. Comparison of calculated homogeneous freezing point depressions suggest that size effects on freezing may be more important than the degree of ammoniation of the sulfate compound.

  18. Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

    Directory of Open Access Journals (Sweden)

    K. Adachi

    2008-11-01

    Full Text Available Soot particles, which are aggregated carbonaceous spherules with graphitic structures, are major aerosol constituents that result from burning of fossil fuel, biofuel, and biomass. Their properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using a transmission electron microscope (TEM for both imaging and chemical analysis, we measured ~8000 particles (25 samples with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC and adjacent areas. Most particles are coated, consist of aggregates, or both. For example, almost all analyzed particles contain S and 70% also contain K, suggesting coagulation and condensation of sulfates and particles derived from biomass and biofuel burning. In the MC plumes, over half of all particles contained soot coated by organic matter and sulfates. The median value of the soot volume fraction in such coated particles is about 15%. In contrast to the assumptions used in many climate models, the soot particles did not become compact even when coated. Moreover, about 80% by volume of the particles consisting of organic matter with sulfate also contained soot, indicating the important role of soot in the formation of secondary aerosol particles. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetimes. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate of MC than uncoated soot particles.

  19. Hygroscopic behavior of multicomponent organic aerosols and their internal mixtures with ammonium sulfate

    Directory of Open Access Journals (Sweden)

    B. Jing

    2015-08-01

    Full Text Available Water soluble organic compounds (WSOCs are important components of organics in the atmospheric fine particulate matter. Although WSOCs play an important role in the hygroscopicity of aerosols, water uptake behavior of internally mixed WSOC aerosols remains limited characterization. Here, the hygroscopic properties of single component such as levoglucosan, oxalic acid, malonic acid, succinic acid and phthalic acid and multicomponent WSOC aerosols mainly involving oxalic acid are investigated with the hygroscopicity tandem differential mobility analyzer (HTDMA. The coexisting hygroscopic species including levoglucosan, malonic acid and phthalic acid have strong influence on the hygroscopic growth and phase behavior of oxalic acid, even suppress its crystallization completely. The interactions between oxalic acid and levoglucosan are confirmed by infrared spectra. The discrepancies between measured growth factors and predictions from Extended Aerosol Inorganics Model (E-AIM with UNIFAC method and Zdanovskii–Stokes–Robinson (ZSR approach increase at medium and high relative humidity (RH assuming oxalic acid in a solid state. For the internal mixture of oxalic acid with levoglucosan or succinic acid, there is enhanced water uptake at high RH due to positive chemical interactions between solutes. Organic mixture has more complex effect on the hygroscopicity of ammonium sulfate than single species. Although hygroscopic species such as levoglucosan accounts for a small fraction in the multicomponent aerosols, they may still strongly influence the hygroscopic behavior of ammonium sulfate by changing phase state of oxalic acid which plays the role of "intermediate" species. Considering the abundance of oxalic acid in the atmospheric aerosols, its mixtures with hygroscopic species may significantly promote water uptake under high RH conditions and thus affect the cloud condensation nuclei (CCN activity, optical properties and chemical reactivity of

  20. Imaginary refractive index and other microphysical properties of volcanic ash, Sarahan dust, and other mineral aerosols

    Science.gov (United States)

    Rocha Lima, A.; Martins, J.; Krotkov, N. A.; Artaxo, P.; Todd, M.; Ben Ami, Y.; Dolgos, G.; Espinosa, R.

    2013-12-01

    Aerosol properties are essential to support remote sensing measurements, atmospheric circulation and climate models. This research aims to improve the understanding of the optical and microphysical properties of different types of aerosols particles. Samples of volcanic ash, Saharan dust and other mineral aerosols particles were analyzed by different techniques. Ground samples were sieved down to 45um, de-agglomerated and resuspended in the laboratory using a Fluidized Bed Aerosol Generator (FBAG). Particles were collected on Nuclepore filters into PM10, PM2.5, or PM1.0. and analyzed by different techniques, such as Scanning Electron Microscopy (SEM) for determination of size distribution and shape, spectral reflectance for determination of the optical absorption properties as a function of the wavelength, material density, and X-Ray fluorescence for the elemental composition. The spectral imaginary part of refractive index from the UV to the short wave infrared (SWIR) wavelength was derived empirically from the measurements of the spectral mass absorption coefficient, size distribution and density of the material. Some selected samples were also analyzed with the Polarized Imaging Nephelometer (PI-Neph) instrument for the characterization of the aerosol polarized phase function. This work compares results of the spectral refractive index of different materials obtained by our methodology with those available in the literature. In some cases there are significant differences both in magnitude and spectral dependence of the imaginary refractive index. These differences are evaluated and discussed in this work.

  1. The impact of volcanic aerosol on the Northern Hemisphere stratospheric polar vortex: mechanisms and sensitivity to forcing structure

    Directory of Open Access Journals (Sweden)

    M. Toohey

    2014-06-01

    Full Text Available Observations and simple theoretical arguments suggest that the Northern Hemisphere (NH stratospheric polar vortex is stronger in winters following major volcanic eruptions. However, recent studies show that climate models forced by prescribed volcanic aerosol fields fail to reproduce this effect. We investigate the impact of volcanic aerosol forcing on stratospheric dynamics, including the strength of the NH polar vortex, in ensemble simulations with the Max Planck Institute Earth System Model. The model is forced by four different prescribed forcing sets representing the radiative properties of stratospheric aerosol following the 1991 eruption of Mt. Pinatubo: two forcing sets are based on observations, and are commonly used in climate model simulations, and two forcing sets are constructed based on coupled aerosol–climate model simulations. For all forcings, we find that temperature and zonal wind anomalies in the NH high latitudes are not directly impacted by anomalous volcanic aerosol heating. Instead, high latitude effects result from robust enhancements in stratospheric residual circulation, which in turn result, at least in part, from enhanced stratospheric wave activity. High latitude effects are therefore much less robust than would be expected if they were the direct result of aerosol heating. While there is significant ensemble variability in the high latitude response to each aerosol forcing set, the mean response is sensitive to the forcing set used. Significant differences, for example, are found in the NH polar stratosphere temperature and zonal wind response to two different forcing data sets constructed from different versions of SAGE II aerosol observations. Significant strengthening of the polar vortex, in rough agreement with the expected response, is achieved only using aerosol forcing extracted from prior coupled aerosol–climate model simulations. Differences in the dynamical response to the different forcing sets used

  2. Evaporation of sulfate aerosols at low relative humidity

    Science.gov (United States)

    Tsagkogeorgas, Georgios; Roldin, Pontus; Duplissy, Jonathan; Rondo, Linda; Tröstl, Jasmin; Slowik, Jay G.; Ehrhart, Sebastian; Franchin, Alessandro; Kürten, Andreas; Amorim, Antonio; Bianchi, Federico; Kirkby, Jasper; Petäjä, Tuukka; Baltensperger, Urs; Boy, Michael; Curtius, Joachim; Flagan, Richard C.; Kulmala, Markku; Donahue, Neil M.; Stratmann, Frank

    2017-07-01

    Evaporation of sulfuric acid from particles can be important in the atmospheres of Earth and Venus. However, the equilibrium constant for the dissociation of H2SO4 to bisulfate ions, which is the one of the fundamental parameters controlling the evaporation of sulfur particles, is not well constrained. In this study we explore the volatility of sulfate particles at very low relative humidity. We measured the evaporation of sulfur particles versus temperature and relative humidity in the CLOUD chamber at CERN. We modelled the observed sulfur particle shrinkage with the ADCHAM model. Based on our model results, we conclude that the sulfur particle shrinkage is mainly governed by H2SO4 and potentially to some extent by SO3 evaporation. We found that the equilibrium constants for the dissociation of H2SO4 to HSO4-(KH2SO4) and the dehydration of H2SO4 to SO3 (xKSO3) are KH2SO4 = 2-4 × 109 mol kg-1 and xKSO3 ≥ 1.4 × 1010 at 288.8 ± 5 K.

  3. Role of volcanic and anthropogenic aerosols in the recent global surface warming slowdown

    Science.gov (United States)

    Smith, Doug M.; Booth, Ben B. B.; Dunstone, Nick J.; Eade, Rosie; Hermanson, Leon; Jones, Gareth S.; Scaife, Adam A.; Sheen, Katy L.; Thompson, Vikki

    2016-10-01

    The rate of global mean surface temperature (GMST) warming has slowed this century despite the increasing concentrations of greenhouse gases. Climate model experiments show that this slowdown was largely driven by a negative phase of the Pacific Decadal Oscillation (PDO), with a smaller external contribution from solar variability, and volcanic and anthropogenic aerosols. The prevailing view is that this negative PDO occurred through internal variability. However, here we show that coupled models from the Fifth Coupled Model Intercomparison Project robustly simulate a negative PDO in response to anthropogenic aerosols implying a potentially important role for external human influences. The recovery from the eruption of Mount Pinatubo in 1991 also contributed to the slowdown in GMST trends. Our results suggest that a slowdown in GMST trends could have been predicted in advance, and that future reduction of anthropogenic aerosol emissions, particularly from China, would promote a positive PDO and increased GMST trends over the coming years. Furthermore, the overestimation of the magnitude of recent warming by models is substantially reduced by using detection and attribution analysis to rescale their response to external factors, especially cooling following volcanic eruptions. Improved understanding of external influences on climate is therefore crucial to constrain near-term climate predictions.

  4. Climate impact of volcanic aerosol in the stratosphere and upper troposphere - CALIPSO observations from 2006-2015

    Science.gov (United States)

    Friberg, Johan; Martinsson, Bengt G.; Andersson, Sandra M.; Sandvik, Oscar S.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, Andreas

    2017-04-01

    We have investigated the climate impact of volcanic eruptions in the period 2006-2015, and found that the volcanic perturbations of the stratospheric aerosol is stronger and lasts longer than previously thought. Recent studies (Ridley et al., 2014, Andersson et al., 2015) show that a large portion of volcanic climate impact stems from aerosol in the LMS (lowermost stratosphere). Although the LMS holds >40% of the stratospheric mass (Appenzeller et al., 1996) it is generally neglected in estimations of the stratospheric AOD (aerosol optical depth). In the past decade the stratospheric aerosol load was perturbed by a number of volcanic eruptions. We cover that period by using the CALIPSO level 1b night-time data to study the volcanic influence on the global and regional climate. CALIPSO data were averaged to a resolution of 180 m vertically and 1×1° horizontally, cleaned from ice clouds by means of the depolarization ratio (Vernier et al., 2009), and a method was developed to remove polar stratospheric clouds (PSC). This approach enables identification of aerosol also at low altitudes (currently using 4 km minimum altitude) and in the Antarctic region (60 to 90°S) where PSCs are frequent during winter. In the current study, we estimate the total stratospheric AOD and radiative forcing and find that significant fractions of volcanic aerosol were located below the static tropopause after volcanic eruptions. Volcanic aerosol was generally observed down to the dynamic tropopause, and detected down to potential vorticities of 1.5-2 PVU (almost 1 km below the static tropopause). Hence, the dynamic tropopause was found to better enclose the volcanic aerosol. Furthermore, large concentrations of aerosol from the Kasatochi eruption (Aug 2008) is found to linger in the extratropical UT (upper troposphere) for several months after the eruption. Sulphate-rich volcanic aerosol transported from the LMS may influence cirrus clouds in the extratropical UT, inducing an indirect

  5. Assessment of the first indirect radiative effect of ammonium-sulfate-nitrate aerosols in East Asia

    Science.gov (United States)

    Han, Xiao; Zhang, Meigen; Skorokhod, Andrei

    2016-09-01

    A physically based cloud nucleation parameterization was introduced into an optical properties/radiative transfer module incorporated with the off-line air quality modeling system Regional Atmospheric Modeling System (RAMS)-Models-3 Community Multi Scale Air Quality (CMAQ) to investigate the distribution features of the first indirect radiative effects of sulfate, nitrate, and ammonium-sulfate-nitrate (ASN) over East Asia for the years of 2005, 2010, and 2013. The relationship between aerosol particles and cloud droplet number concentration could be properly described by this parameterization because the simulated cloud fraction and cloud liquid water path were generally reliable compared with Moderate Resolution Imaging Spectroradiometer (MODIS) retrieved data. Simulation results showed that the strong effect of indirect forcing was mainly concentrated in Southeast China, the East China Sea, the Yellow Sea, and the Sea of Japan. The highest indirect radiative forcing of ASN reached -3.47 W m-2 over Southeast China and was obviously larger than the global mean of the indirect forcing of all anthropogenic aerosols. In addition, sulfate provided about half of the contribution to the ASN indirect forcing effect. However, the effect caused by nitrate was weak because the mass burden of nitrate was very low during summer, whereas the cloud fraction was the highest. The analysis indicated that even though the interannual variation of indirect forcing magnitude generally followed the trend of aerosol mass burden from 2005 to 2013, the cloud fraction was an important factor that determined the distribution pattern of indirect forcing. The heaviest aerosol loading in North China did not cause a strong radiative effect because of the low cloud fraction over this region.

  6. Evaluating the potential influence of inter-continental transport of sulfate aerosols on air quality

    Science.gov (United States)

    Mauzerall, D. L.; Liu, J.

    2007-12-01

    In this study, we compare the potential influence of inter-continental transport of sulfate aerosols on the air quality of continental regions. We use a global chemical transport model, Model of Ozone and Related Tracers, version 2 (MOZART-2), to quantify the source-receptor relationships of inter-continental transport of sulfate aerosols among ten regions in 2000. In order to compare the importance of foreign emissions relative to domestic emissions and estimate the effect of future changes in emissions on human exposure, we define an "influence potential" (IP). The IP quantifies the human exposure that occurs in a receptor region as a result of a unit of SO2 emissions from a source region. We find that due to the non-linear nature of sulfate production, regions with low SO2 emissions usually have large domestic IP, and vice versa. An exception is East Asia (EA), which has both high SO2 emissions and relatively large domestic IP, mostly caused by the spatial coincidence of emissions and population. We find that intercontinental IPs are usually less than domestic IPs by 1-3 orders of magnitude. SO2 emissions from the Middle East (ME) and Europe (EU) have the largest potential to influence populations in surrounding regions. By comparing the IP ratios (IPR) between foreign and domestic SO2 emissions, we find that the IPR values range from 0.00001 to 0.16 and change with season. Therefore, if reducing human exposure to sulfate aerosols is the objective, all regions should first focus on reducing domestic SO2 emissions. In addition, we find that relatively high IPR values exist among the EU, ME, the former Soviet Union (FSU) and African (AF) regions. Therefore, based on the IP and IPR values, we conclude that a regional agreement among EA countries, and an inter-regional agreement among EU, ME, FSU and north AF regions to control sulfur emissions would benefit public health in these regions.

  7. Potential influence of inter-continental transport of sulfate aerosols on air quality

    Science.gov (United States)

    Liu, Junfeng; Mauzerall, Denise L.

    2007-10-01

    In this study, we compare the potential influence of inter-continental transport of sulfate aerosols on the air quality of (different) continental regions. We use a global chemical transport model, Model of Ozone and Related Tracers, version 2 (MOZART-2), to quantify the source receptor relationships of inter-continental transport of sulfate aerosols among ten regions in 2000. In order to compare the importance of foreign with domestic emissions and to estimate the effect of future changes in emissions on human exposure, we define an 'influence potential' (IP). The IP quantifies the human exposure that occurs in a receptor region as a result of a unit of SO2 emissions from a source region. We find that due to the non-linear nature of sulfate production, regions with low SO2 emissions usually have large domestic IP, and vice versa. An exception is East Asia (EA), which has both high SO2 emissions and relatively large domestic IP, mostly caused by the spatial coincidence of emissions and population. We find that inter-continental IPs are usually less than domestic IPs by 1 3 orders of magnitude. SO2 emissions from the Middle East (ME) and Europe (EU) have the largest potential to influence populations in surrounding regions. By comparing the IP ratios (IPR) between foreign and domestic SO2 emissions, we find that the IPR values range from 0.000 01 to 0.16 and change with season. Therefore, if reducing human exposure to sulfate aerosols is the objective, all regions should first focus on reducing domestic SO2 emissions. In addition, we find that relatively high IPR values exist among the EU, ME, the former Soviet Union (FSU) and African (AF) regions. Therefore, on the basis of the IP and IPR values, we conclude that a regional agreement among EA countries, and an inter-regional agreement among EU, ME, FSU and (north) AF regions to control sulfur emissions could benefit public health in these regions.

  8. Effects of ammonium sulfate aerosols on vegetation—II. Mode of entry and responses of vegetation

    Science.gov (United States)

    Gmur, Nicholas F.; Evans, Lance S.; Cunningham, Elizabeth A.

    These experiments were designed to provide information on the rates of aerosol deposition, mode of entry, and effects of deposition of submicrometer ammonium sulfate aerosols on foliage of Phaseolus vulgaris L. A deposition velocity of 3.2 × 10 3cms-1 was constant during 3-week exposures of plants to aerosol concentrations of 26mg m -3 (i.e. about two orders of magnitude above ambient episode concentrations). Mean deposition rate on foliage was 4.1 × 10 -11 μg cm -2s -1. Visible injury symptoms included leaf chlorosis, necrosis and loss of turgor. Chlorosis was most frequent near leaf margins causing epinasty and near major veins. Internal injury occurred initially in spongy mesophyll cells. Eventually abaxial epidermal and palisade parenchyma cells were injured. These results suggest that submicrometer aerosols enter abaxial stomata and affect more internal cells before affecting leaf surface cells. Exposure to aerosols decreased both abaxial and adaxial leaf resistances markedly. Although visible injury to foliage occurred, no changes in dry mass of roots and shoots or leaf area occurred. These results suggest that for the plant developmental stage studied, while leaf resistances decreased and cellular injury occurred in foliage, these factors were not significantly related to plant growth and development.

  9. Effects of ammonium sulfate aerosols on vegetation--II. Mode of entry and responses of vegetation

    Energy Technology Data Exchange (ETDEWEB)

    Gmur, N.F. (Brookhaven National Lab., Upton, NY); Evans, L.S.; Cunningham, E.A.

    1983-01-01

    These experiments were designed to provide information on the rates of aerosol deposition, mode of entry, and effects of deposition of submicrometer ammonium sulfate aerosols on foliage of Phaseolus vulgaris L. A deposition velocity of 3.2 x 10/sup -3/ cm s/sup -1/ was constant during 3-week exposures of plants to aerosol concentrations of 26mg m/sup -3/ (i.e., about two orders of magnitude above ambient episode concentrations). Mean deposition rate on foliage was 4.1 x 10/sup -11/ ..mu..g cm/sup -2/ s/sup -1/. Visible injury symptoms included leaf chlorosis, necrosis, and loss of turgor. Chlorosis was most frequent near leaf margins causing epinasty and near major veins. Internal injury occurred initially in spongy mesophyll cells. Eventually abaxial epidermal and palisade parenchyma cells were injured. These results suggest that submicrometer aerosols enter abaxial stomata and affect more internal cells before affecting leaf surface cells. Exposure to aerosols decreased both abaxial and adaxial leaf resistances markedly. Although visible injury to foliage occurred, no change in dry mass of roots and shoots or leaf area occurred. These results suggest that for the plant developmental stage studied, while leaf resistances decreased and cellular injury occurred in foliage, these factors were not significantly related to plant growth and development.

  10. Heterogeneous Uptake of Gaseous N2O5 by Sulfate Aerosols

    Science.gov (United States)

    Leu, M.; Kane, S. M.; Caloz, F.

    2001-12-01

    The heterogeneous uptake of gaseous N2O5 by ammonium sulfate [(NH4)2SO4], ammonium bisulfate [NH4HSO4], and sulfuric acid [H2SO4] aerosols as a function of relative humidity has been investigated at room temperature and atmospheric pressure. Ammonium-containing aerosols were generated by a constant output atomizer and conditioned by passing through a diffusion dryer. Sulfuric acid aerosols were produced by the homogeneous reaction of SO3 and H2O in a borosilicate vessel. Addition of a dry or wet N2 flow controlled the relative humidity (RH) of these aerosol flows. Using a chemical ionization mass spectrometer (CIMS) for N2O5 concentration monitoring and a scanning mobility particle spectrometer (SMPS) for aerosol characterization, reaction probabilities (g) in the range of 0.001 to 0.1 for the uptake of N2O5 were determined as a function of RH. The results are expressed as follows: gamma[(NH4)2SO4] = 2.79 x 10-4 + 1.30 x 10-4 x (RH) -3.43 x 10-6 x (RH)2 + 7.52 x 10-8 x (RH)3, gamma[NH4HSO4] = 2.07 x 10-3 - 1.48 x 10-4 x (RH) + 8.26 x 10-6 x (RH)2, and gamma[H2SO4] = 0.052 - 2.79 x 10-4 x (RH) . We suggest that the water content and phase in the ammonium-containing aerosols control the reactivity of N2O5 while liquid-phase ionic reactions primarily dominate the uptake in sulfuric acid aerosols.

  11. Continuous Monitoring of Nitrate and Sulfate in Aerosols with Microchip Electrophoresis

    Science.gov (United States)

    Noblitt, S. D.; Henry, C. S.; Collett, J. L.; Hering, S. V.

    2007-12-01

    Routine monitoring of aerosol composition is important since aerosols can negatively affect both the environment and health. Water-soluble inorganic ions are commonly monitored using the particle-into-liquid-sampler coupled to ion chromatography (PILS-IC). However, a less-expensive, faster, and more portable analysis system is desirable. Here, we present the coupling of microchip capillary electrophoresis (MCE) to a water-based condensation particle counter (WCPC) for rapid and continuous monitoring of chloride, nitrate, and sulfate in atmospheric aerosols. To achieve a working system, several obstacles were overcome. A working interface between the electrophoresis microchip and the WCPC sampler was developed. This interface was designed to remove insoluble particles from the analysis stream and to prevent the sampling-induced pressure gradient from altering flow in the microfluidic device. The electrophoresis separation chemistry was optimized for the small chip size, to be free from potential interfering compounds, and to operate continuously for several hours. In-field performance of the integrated system was tested with ambient aerosols. Anion analyses can be performed in less than two minutes with aerosol detection limits similar to the PILS-IC, but with greater portability and reduced cost. Coupling microfluidic devices to aerosol sampling technology proves successful for inorganic anion analysis and shows potential for faster and more sensitive measurements as well as monitoring of other water- soluble aerosol components such as organic acids, cations, and carbohydrates. The reduced cost and size relative to current technology indicate that greater deployment of monitoring stations or the advent of portable analyzers may be feasible.

  12. A study of the phase transition behavior of internally mixed ammonium sulfate - malonic acid aerosols

    Directory of Open Access Journals (Sweden)

    C. F. Braban

    2004-01-01

    Full Text Available This is a study into the phase transitions of aerosol composed of the ternary system ammonium sulfate (AS - malonic acid (MA - water using infrared extinction spectroscopy. Twelve compositions were studied in both deliquescence and efflorescence mode experiments. The presence of a MA fraction, by dry mass, (fMA of 0.1 in an AS aerosol altered the relative humidity at which the phase transitions occur in an atmospherically significant manner. For compositions with 0.25fMAfMA=0.9, the crystallization relative humidity of MA was lowered from RH=6% to less than 1%. Similarly, at fMA=0.4, the AS component did not crystallize. The atmospheric implications of the results are discussed.

  13. Effective Henry's Law constant measurements for glyoxal in model aerosols containing sulfate

    Science.gov (United States)

    Kampf, C.; Waxman, E.; Slowik, J.; Dommen, J.; Prevot, A.; Baltensperger, U.; Noziere, B.; Hoffmann, T.; Volkamer, R.

    2012-04-01

    Traditional models represent secondary organic aerosol (SOA) formation based on the gas-phase oxidation of a limited set of precursor molecules. However, these models tend to under-estimate the amounts and degree of oxygenation of actual SOA, indicating missing processes. One such source that has become increasingly important in recent years is glyoxal (CHOCHO, the smallest alpha-dicarbonyl). Unlike traditional SOA precursors, glyoxal forms SOA by partitioning to the aqueous phase according to Henry's Law. This work presents an analysis of Henry's Law constants for glyoxal uptake to laboratory-generated aerosols in a dynamically coupled gas-aerosol system. We combine CU LED-CE-DOAS measurements of gas-phase glyoxal with online HR-Tof-AMS and time-resolved HPLC ESI MS/MS particle-phase measurements to characterize the time resolved evolution of glyoxal partitioning, and relate molecular-specific measurements to AMS mass spectra. The experiments were performed in the simulation chamber facility at PSI, Switzerland, and investigate ammonium sulfate (AS), and mixed AS / fulvic acid seed aerosols under relative humidity conditions ranging from 50 to 85% RH. The Henry's Law and effective Henry's Law constants are compared with other values reported in the literature.

  14. Simulation of nitrate, sulfate, and ammonium aerosols over the United States

    Directory of Open Access Journals (Sweden)

    J. M. Walker

    2012-11-01

    Full Text Available Atmospheric concentrations of inorganic gases and aerosols (nitrate, sulfate, and ammonium are simulated for 2009 over the United States using the chemical transport model GEOS-Chem. Predicted aerosol concentrations are compared with surface-level measurement data from the Interagency Monitoring of Protected Visual Environments (IMPROVE, the Clean Air Status and Trends Network (CASTNET, and the California Air Resources Board (CARB. Sulfate predictions nationwide are in reasonably good agreement with observations, while nitrate and ammonium are over-predicted in the East and Midwest, but under-predicted in California, where observed concentrations are the highest in the country. Over-prediction of nitrate in the East and Midwest is consistent with results of recent studies, which suggest that nighttime nitric acid formation by heterogeneous hydrolysis of N2O5 is over-predicted based on current values of the N2O5 uptake coefficient, γ, onto aerosols. After reducing the value of γ by a factor of 10, predicted nitrate levels in the US Midwest and East still remain higher than those measured, and over-prediction of nitrate in this region remains unexplained. Comparison of model predictions with satellite measurements of ammonia from the Tropospheric Emissions Spectrometer (TES indicates that ammonia emissions in GEOS-Chem are underestimated in California and that the nationwide seasonality applied to ammonia emissions in GEOS-Chem does not represent California very well, particularly underestimating winter emissions. An ammonia sensitivity study indicates that GEOS-Chem simulation of nitrate is ammonia-limited in southern California and much of the state, suggesting that an underestimate of ammonia emissions is likely the main cause for the under-prediction of nitrate aerosol in many areas of California. An approximate doubling of ammonia emissions is needed to reproduce observed nitrate concentrations in

  15. A model study of Fuego volcanic aerosol dispersion in the lower stratosphere

    Science.gov (United States)

    Remsberg, E. E.; Turner, R. E.; Butler, C. F.

    1982-01-01

    A zonally averaged time-dependent primitive equation model is used to simulate the dispersion of both a carbon 14 injection and the volcanic aerosol from the 1974 Fuego eruption. It is noted that both injections occurred at low latitudes to midlatitudes in the Northern Hemisphere. The eddy flux terms, which account for the major portion of the transport in the lower stratosphere of this model, are specified in a manner similar to that of Harwood and Pyle (1975). Comparisons with data underline the ability of the model to simulate the vertical character of the tracer while maintaining reasonable meridional transport times. For the aerosol study, the simulated 1/e decay time at 37 deg N and for the 16- to 21-km altitude region is 9 months, whereas lidar measurements at the same latitude give a decay time of 8 months. The simulated vertical width at half-maximum for the aerosol tracer at 37 deg N and 19 deg N and for 6 months after the event possesses values of 5.0 km and 3.6 km, respectively, whereas the observed lidar values are 4.4 km and 3.0 km, respectively. The tracer transport to the Southern Hemisphere also is in qualitative agreement with the limited data that are available.

  16. Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

    Directory of Open Access Journals (Sweden)

    K. Adachi

    2008-05-01

    Full Text Available Soot particles are major aerosol constituents that result from emissions of burning of fossil fuel and biomass. Because they both absorb sunlight and contribute to cloud formation, they are an influence on climate on local, regional, and global scales. It is therefore important to evaluate their optical and hygroscopic properties and those effects on the radiation budget. Those properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using transmission electron microscopy, we measured ~8000 particles (25 samples with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC and adjacent areas. More than 50% of the particles consist of internally mixed soot, organic matter, and sulfate. Imaging combined with chemical analysis of individual particles show that many are coated, consist of aggregates, or both. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetime. Our results suggest that a mixture of materials from multiple sources such as vehicles, power plants, and biomass burning occurs in individual particles, thereby increasing their complexity. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate than uncoated soot particles. Moreover, soot occurs in more than 60% of all particles in the MC plumes, suggesting its important role in the formation of secondary aerosol particles.

  17. A study of the phase transition behavior of mixed ammonium sulfate – malonic acid aerosols

    Directory of Open Access Journals (Sweden)

    C. F. Braban

    2004-06-01

    Full Text Available This is a study into the phase transitions of aerosol composed of the ternary system ammonium sulfate (AS – malonic acid (MA – water using infrared extinction spectroscopy. Twelve compositions were studied in both deliquescence and efflorescence mode experiments. The presence of a MA fraction, by dry mass, (fMA of 0.1 in an AS aerosol altered the relative humidity at which the phase transitions occur in an atmospherically significant manner. For compositions with 0.25<fMA<0.90, no distinct "deliquescence" was observed, contrary to the observed behavior in the binary systems. The crystallization of both the MA and AS components is suppressed by the presence of the other component in the aerosol. At fMA=0.9, the crystallization relative humidity of MA was lowered from RH=6% to less than 1%. Similarly, at fMA=0.4, the AS component did not crystallize. The atmospheric implications of the results are discussed.

  18. Importance of including ammonium sulfate ((NH42SO4 aerosols for ice cloud parameterization in GCMs

    Directory of Open Access Journals (Sweden)

    R. Yang

    2010-02-01

    Full Text Available A common deficiency of many cloud-physics parameterizations including the NASA's microphysics of clouds with aerosol-cloud interactions (hereafter called McRAS-AC is that they simulate lesser (larger than the observed ice cloud particle number (size. A single column model (SCM of McRAS-AC physics of the GEOS4 Global Circulation Model (GCM together with an adiabatic parcel model (APM for ice-cloud nucleation (IN of aerosols were used to systematically examine the influence of introducing ammonium sulfate (NH42SO4 aerosols in McRAS-AC and its influence on the optical properties of both liquid and ice clouds. First an (NH42SO4 parameterization was included in the APM to assess its effect on clouds vis-à-vis that of the other aerosols. Subsequently, several evaluation tests were conducted over the ARM Southern Great Plain (SGP and thirteen other locations (sorted into pristine and polluted conditions distributed over marine and continental sites with the SCM. The statistics of the simulated cloud climatology were evaluated against the available ground and satellite data. The results showed that inclusion of (NH42SO4 into McRAS-AC of the SCM made a remarkable improvement in the simulated effective radius of ice cloud particulates. However, the corresponding ice-cloud optical thickness increased even more than the observed. This can be caused by lack of horizontal cloud advection not performed in the SCM. Adjusting the other tunable parameters such as precipitation efficiency can mitigate this deficiency. Inclusion of ice cloud particle splintering invoked empirically further reduced simulation biases. Overall, these changes make a substantial improvement in simulated cloud optical properties and cloud distribution particularly over the Intertropical Convergence Zone (ITCZ in the GCM.

  19. Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing

    Directory of Open Access Journals (Sweden)

    S. T. Martin

    2004-01-01

    Full Text Available The effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US and once for lower side (LS of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2 (g SO4-2-1, which compare to US values of 0.030 and 13.9 m2 (g SO4-2-1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m-2 are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL=-0.750, FU=-0.930, and DFU,L=24% for full sky calculations without clouds and FL=-0.485, FU=-0.605, and DFU,L=25% when clouds are included. Regionally, DFU,L=48% over the USA, 55% over Europe

  20. Direct shortwave forcing of climate by anthropogenic sulfate aerosol: Sensitivity to particle size, composition, and relative humidity

    Energy Technology Data Exchange (ETDEWEB)

    Nemesure, S.; Wagener, R.; Schwartz, S.E. [Brookhaven National Lab., Upton, New York (United States)

    1996-04-01

    Recent estimates of global or hemispheric average forcing of climate by anthropogenic sulfate aerosol due to scattering of shortwave radiation are uncertain by more than a factor of 2. This paper examines the sensitivity of forcing to these microphysical properties for the purposes of obtaining a better understanding of the properties required to reduce the uncertainty in the forcing.

  1. SO2 photoexcitation mechanism links mass-independent sulfur isotopic fractionation in cryospheric sulfate to climate impacting volcanism

    DEFF Research Database (Denmark)

    Hattori, Shohei; Schmidt, Johan Albrecht; Johnson, Matthew Stanley

    2013-01-01

    Natural climate variation, such as that caused by volcanoes, is the basis for identifying anthropogenic climate change. However, knowledge of the history of volcanic activity is inadequate, particularly concerning the explosivity of specific events. Some material is deposited in ice cores...... plume chemistry, allowing the production and preservation of a mass-independent sulfur isotope anomaly in the sulfate product. The model accounts for the amplitude, phases, and time development of Δ(33)S/δ(34)S and Δ(36)S/Δ(33)S found in glacial samples. We are able to identify the process controlling...

  2. PSC and volcanic aerosol routine observations in Antarctica by UV-visible ground-based spectrometry

    Science.gov (United States)

    Sarkissian, A.; Pommereau, J. P.; Goutail, F.

    1994-01-01

    Polar statospheric clouds (PSC) and stratospheric aerosol can be observed by ground-based UV-visible spectrometry by looking at the variation of the color of the sky during twilight. A radiative transfer model shows that reddenings are caused by high altitude (22-28 km) thin layers of scatterers, while low altitude (12-20 km) thick ones result in blueings. The color index method applied on 4 years of observations at Dumont d'Urville (67 deg S), from 1988 to 1991, shows that probably because the station is located at the edge of the vortex, dense PSC are uncommon. More unexpected is the existence of a systematic seasonal variation of the color of the twilight sky - bluer at spring - which reveals the formation of a dense scattering layer at or just above the tropopause at the end of the winter. Large scattering layers are reported above the station in 1991, first in August around 12-14 km, later in September at 22-24 km. They are attributed to volcanic aerosol from Mt Hudson and Mt Pinatubo respectively, which erupted in 1991. Inspection of the data shows that the lowest entered rapidly into the polar vortex but not the highest which remained outside, demonstrating that the vortex was isolated at 22-26 km.

  3. Microphysical, Macrophysical and Radiative Signatures of Volcanic Aerosols in Trade Wind Cumulus Observed by the A-Train

    Science.gov (United States)

    Yuan, T.; Remer, L. A.; Yu, H.

    2011-01-01

    Increased aerosol concentrations can raise planetary albedo not only by reflecting sunlight and increasing cloud albedo, but also by changing cloud amount. However, detecting aerosol effect on cloud amount has been elusive to both observations and modeling due to potential buffering mechanisms and convolution of meteorology. Here through a natural experiment provided by long-tem1 degassing of a low-lying volcano and use of A-Train satellite observations, we show modifications of trade cumulus cloud fields including decreased droplet size, decreased precipitation efficiency and increased cloud amount are associated with volcanic aerosols. In addition we find significantly higher cloud tops for polluted clouds. We demonstrate that the observed microphysical and macrophysical changes cannot be explained by synoptic meteorology or the orographic effect of the Hawaiian Islands. The "total shortwave aerosol forcin", resulting from direct and indirect forcings including both cloud albedo and cloud amount. is almost an order of magnitude higher than aerosol direct forcing alone. Furthermore, the precipitation reduction associated with enhanced aerosol leads to large changes in the energetics of air-sea exchange and trade wind boundary layer. Our results represent the first observational evidence of large-scale increase of cloud amount due to aerosols in a trade cumulus regime, which can be used to constrain the representation of aerosol-cloud interactions in climate models. The findings also have implications for volcano-climate interactions and climate mitigation research.

  4. Microphysical, macrophysical and radiative signatures of volcanic aerosols in trade wind cumulus observed by the A-Train

    Directory of Open Access Journals (Sweden)

    T. Yuan

    2011-07-01

    Full Text Available Increased aerosol concentrations can raise planetary albedo not only by reflecting sunlight and increasing cloud albedo, but also by changing cloud amount. However, detecting aerosol effect on cloud amount has been elusive to both observations and modeling due to potential buffering mechanisms and convolution of meteorology. Here through a natural experiment provided by long-term degassing of a low-lying volcano and use of A-Train satellite observations, we show modifications of trade cumulus cloud fields including decreased droplet size, decreased precipitation efficiency and increased cloud amount are associated with volcanic aerosols. In addition we find significantly higher cloud tops for polluted clouds. We demonstrate that the observed microphysical and macrophysical changes cannot be explained by synoptic meteorology or the orographic effect of the Hawaiian Islands. The "total shortwave aerosol forcin", resulting from direct and indirect forcings including both cloud albedo and cloud amount, is almost an order of magnitude higher than aerosol direct forcing alone. Furthermore, the precipitation reduction associated with enhanced aerosol leads to large changes in the energetics of air-sea exchange and trade wind boundary layer. Our results represent the first observational evidence of large-scale increase of cloud amount due to aerosols in a trade cumulus regime, which can be used to constrain the representation of aerosol-cloud interactions in climate models. The findings also have implications for volcano-climate interactions and climate mitigation research.

  5. Isotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layer

    Science.gov (United States)

    Chen, Qianjie; Geng, Lei; Schmidt, Johan A.; Xie, Zhouqing; Kang, Hui; Dachs, Jordi; Cole-Dai, Jihong; Schauer, Andrew J.; Camp, Madeline G.; Alexander, Becky

    2016-09-01

    Sulfate is an important component of global atmospheric aerosol, and has partially compensated for greenhouse gas-induced warming during the industrial period. The magnitude of direct and indirect radiative forcing of aerosols since preindustrial times is a large uncertainty in climate models, which has been attributed largely to uncertainties in the preindustrial environment. Here, we report observations of the oxygen isotopic composition (Δ17O) of sulfate aerosol collected in the remote marine boundary layer (MBL) in spring and summer in order to evaluate sulfate production mechanisms in pristine-like environments. Model-aided analysis of the observations suggests that 33-50 % of sulfate in the MBL is formed via oxidation by hypohalous acids (HOX = HOBr + HOCl), a production mechanism typically excluded in large-scale models due to uncertainties in the reaction rates, which are due mainly to uncertainties in reactive halogen concentrations. Based on the estimated fraction of sulfate formed via HOX oxidation, we further estimate that daily-averaged HOX mixing ratios on the order of 0.01-0.1 parts per trillion (ppt = pmol/mol) in the remote MBL during spring and summer are sufficient to explain the observations.

  6. The optical constants of several atmospheric aerosol species - Ammonium sulfate, aluminum oxide, and sodium chloride

    Science.gov (United States)

    Toon, O. B.; Pollack, J. B.; Khare, B. N.

    1976-01-01

    An investigation is conducted of problems which are related to a use of measured optical constants in the simulation of the optical constants of real atmospheric aerosols. The techniques of measuring optical constants are discussed, taking into account transmission measurements through homogeneous and inhomogeneous materials, the immersion of a material in a liquid of a known refractive index, the consideration of the minimum deviation angle of prism measurement, the interference of multiply reflected light, reflectivity measurements, and aspects of mathematical analysis. Graphs show the real and the imaginary part of the refractive index as a function of wavelength for aluminum oxide, NaCl, and ammonium sulfate. Tables are provided for the dispersion parameters and the optical constants.

  7. Impact of Stratospheric Volcanic Aerosols on Age-of-Air and Transport of Long-Lived Species

    Directory of Open Access Journals (Sweden)

    Giovanni Pitari

    2016-11-01

    Full Text Available The radiative perturbation associated to stratospheric aerosols from major explosive volcanic eruptions may induce significant changes in stratospheric dynamics. The aerosol heating rates warm up the lower stratosphere and cause a westerly wind anomaly, with additional tropical upwelling. Large scale transport of stratospheric trace species may be perturbed as a consequence of this intensified Brewer–Dobson circulation. The radiatively forced changes of the stratospheric circulation during the first two years after the eruption of Mt. Pinatubo (June 1991 may help explain the observed trend decline of long-lived greenhouse gases at surface stations (approximately −8 and −0.4 ppbv/year for CH4 and N2O, respectively. This decline is partly driven by the increased mid- to high-latitude downward flux at the tropopause and also by an increased isolation of the tropical pipe in the vertical layer near the tropopause, with reduced horizontal eddy mixing. Results from a climate-chemistry coupled model are shown for both long-lived trace species and the stratospheric age-of-air. The latter results to be younger by approximately 0.5 year at 30 hPa for 3–4 years after the June 1991 Pinatubo eruption, as a result of the volcanic aerosols radiative perturbation and is consistent with independent estimates based on long time series of in situ profile measurements of SF6 and CO2. Younger age of air is also calculated after Agung, El Chichón and Ruiz eruptions, as well as negative anomalies of the N2O growth rate at the extratropical tropopause layer. This type of analysis is made comparing the results of two ensembles of model simulations (1960–2005, one including stratospheric volcanic aerosols and their radiative interactions and a reference case where the volcanic aerosols do not interact with solar and planetary radiation.

  8. Sensitivity of modelled sulfate aerosol and its radiative effect on climate to ocean DMS concentration and air-sea flux

    Science.gov (United States)

    Tesdal, Jan-Erik; Christian, James R.; Monahan, Adam H.; von Salzen, Knut

    2016-09-01

    Dimethylsulfide (DMS) is a well-known marine trace gas that is emitted from the ocean and subsequently oxidizes to sulfate in the atmosphere. Sulfate aerosols in the atmosphere have direct and indirect effects on the amount of solar radiation reaching the Earth's surface. Thus, as a potential source of sulfate, ocean efflux of DMS needs to be accounted for in climate studies. Seawater concentration of DMS is highly variable in space and time, which in turn leads to high spatial and temporal variability in ocean DMS emissions. Because of sparse sampling (in both space and time), large uncertainties remain regarding ocean DMS concentration. In this study, we use an atmospheric general circulation model with explicit aerosol chemistry (CanAM4.1) and several climatologies of surface ocean DMS concentration to assess uncertainties about the climate impact of ocean DMS efflux. Despite substantial variation in the spatial pattern and seasonal evolution of simulated DMS fluxes, the global-mean radiative effect of sulfate is approximately linearly proportional to the global-mean surface flux of DMS; the spatial and temporal distribution of ocean DMS efflux has only a minor effect on the global radiation budget. The effect of the spatial structure, however, generates statistically significant changes in the global-mean concentrations of some aerosol species. The effect of seasonality on the net radiative effect is larger than that of spatial distribution and is significant at global scale.

  9. A multi-faceted approach to characterize acid-sulfate alteration processes in volcanic hydrothermal systems on Earth and Mars

    Science.gov (United States)

    Marcucci, Emma Cordts

    Acid-sulfate alteration is a dominant weathering process in high temperature, low pH, sulfur-rich volcanic environments. Additionally, hydrothermal environments have been proposed as locations where life could have originated on Earth. Based on the extensive evidence of flowing surface water and persistent volcanism, similar locations and processes could have existed on early Mars. Globally observed alteration mineral assemblages likely represent relic Martian hydrothermal settings. Yet the limited understanding of environmental controls, limits the confidence of interpreting the paleoconditions of these hydrothermal systems and assessing their habitability to support microbial life. This thesis presents a series of laboratory experiments, geochemical models, analog fieldwork, and Martian remote sensing to characterize distinguishing features and controls of acid-sulfate alteration. The experiments and models were designed to replicate alteration is a highly acidic, sulfurous, and hot field sites. The basaltic minerals were individually reacted in both experimental and model simulations with varying initial parameters to infer the geochemical pathways of acid-sulfate alteration on Earth and Mars. It was found that for a specific starting material, secondary mineralogies were consistent. Variations in pH, temperature and duration affected the abundance, shape, and size of mineral products. Additionally evaporation played a key role in secondary deposits; therefore, both alteration and evaporitic processes need to be taken into consideration. Analog volcanic sites in Nicaragua were used to supplement this work and highlight differences between natural and simulated alteration. In situ visible near-infrared spectroscopy demonstrated that primary lithology and gas chemistry were dominant controls of alteration, with secondary effects from environmental controls, such as temperature and pH. The spectroscopic research from the field was directly related to Mars

  10. Study of pH Stability of R-Salbutamol Sulfate Aerosol Solution and Its Antiasthmatic Effects in Guinea Pigs.

    Science.gov (United States)

    Liu, Qing; Li, Qingrui; Han, Ting; Hu, Tingting; Zhang, Xuemei; Hu, Junhua; Hu, Hui; Tan, Wen

    2017-09-01

    Currently, all commercial available nebulized salbutamol in China is in its racemic form. It is known that only R-salbutamol (eutomer) has therapeutic effects, while S-salbutamol (distomer) may exacerbate asthma after chronic use. Therefore, it is an unmet clinical need to develop R-salbutamol as a nebulized product that is more convenient for young and old patients. In our study, a stable aerosol solution of R-salbutamol sulfate was established, and its antiasthmatic effects were confirmed. The decomposition rate and racemization effect of the R-salbutamol sulfate solution were evaluated over a pH range from 1 to 10 (except pH=7, 8) at 60°C. The aerodynamic particle size of the R-salbutamol sulfate solution and commercial RS-salbutamol sulfate solution were both tested in vitro by Next-Generation Impactor (NGI) in 5°C. Laser diffractometer was used to characterize the droplet-size distribution (DSD) of both solutions. We next conducted an in vivo animal study to document the antiasthmatic effect of R-salbutamol aerosol sulfate solution and determine the relationship to RS-salbutamol. The results showed that the R-salbutamol sulfate solution was more stable at pH 6. In vitro comparison studies indicated that there was no distribution difference between R-salbutamol sulfate solution and the commercial RS-salbutamol solution. The animal results showed that R-salbutamol was more potent than RS-salbutamol against the same dose of histamine challenge. Unlike commercial RS-salbutamol, which was acidified to a pH of 3.5 to extend bench life but may cause bronchoconstriction in asthmatic patients, the neutralized R-salbutamol solution was more suitable for clinic use.

  11. Glacier evolution in high-mountain Asia under stratospheric sulfate aerosol injection geoengineering

    Science.gov (United States)

    Zhao, Liyun; Yang, Yi; Cheng, Wei; Ji, Duoying; Moore, John C.

    2017-06-01

    Geoengineering by stratospheric sulfate aerosol injection may help preserve mountain glaciers by reducing summer temperatures. We examine this hypothesis for the glaciers in high-mountain Asia using a glacier mass balance model driven by climate simulations from the Geoengineering Model Intercomparison Project (GeoMIP). The G3 and G4 schemes specify use of stratospheric sulfate aerosols to reduce the radiative forcing under the Representative Concentration Pathway (RCP) 4.5 scenario for the 50 years between 2020 and 2069, and for a further 20 years after termination of geoengineering. We estimate and compare glacier volume loss for every glacier in the region using a glacier model based on surface mass balance parameterization under climate projections from three Earth system models under G3, five models under G4, and six models under RCP4.5 and RCP8.5. The ensemble projections suggest that glacier shrinkage over the period 2010-2069 is equivalent to sea-level rise of 9.0 ± 1.6 mm (G3), 9.8 ± 4.3 mm (G4), 15.5 ± 2.3 mm (RCP4.5), and 18.5 ± 1.7 mm (RCP8.5). Although G3 keeps the average temperature from increasing in the geoengineering period, G3 only slows glacier shrinkage by about 50 % relative to losses from RCP8.5. Approximately 72 % of glaciated area remains at 2069 under G3, as compared with about 30 % for RCP8.5. The widely reported reduction in mean precipitation expected for solar geoengineering is unlikely to be as important as the temperature-driven shift from solid to liquid precipitation for forcing Himalayan glacier change. The termination of geoengineering at 2069 under G3 leads to temperature rise of about 1.3 °C over the period 2070-2089 relative to the period 2050-2069 and corresponding increase in annual mean glacier volume loss rate from 0.17 to 1.1 % yr-1, which is higher than the 0.66 % yr-1 under RCP8.5 during 2070-2089.

  12. Glacier evolution in high-mountain Asia under stratospheric sulfate aerosol injection geoengineering

    Directory of Open Access Journals (Sweden)

    L. Zhao

    2017-06-01

    Full Text Available Geoengineering by stratospheric sulfate aerosol injection may help preserve mountain glaciers by reducing summer temperatures. We examine this hypothesis for the glaciers in high-mountain Asia using a glacier mass balance model driven by climate simulations from the Geoengineering Model Intercomparison Project (GeoMIP. The G3 and G4 schemes specify use of stratospheric sulfate aerosols to reduce the radiative forcing under the Representative Concentration Pathway (RCP 4.5 scenario for the 50 years between 2020 and 2069, and for a further 20 years after termination of geoengineering. We estimate and compare glacier volume loss for every glacier in the region using a glacier model based on surface mass balance parameterization under climate projections from three Earth system models under G3, five models under G4, and six models under RCP4.5 and RCP8.5. The ensemble projections suggest that glacier shrinkage over the period 2010–2069 is equivalent to sea-level rise of 9.0 ± 1.6 mm (G3, 9.8 ± 4.3 mm (G4, 15.5 ± 2.3 mm (RCP4.5, and 18.5 ± 1.7 mm (RCP8.5. Although G3 keeps the average temperature from increasing in the geoengineering period, G3 only slows glacier shrinkage by about 50 % relative to losses from RCP8.5. Approximately 72 % of glaciated area remains at 2069 under G3, as compared with about 30 % for RCP8.5. The widely reported reduction in mean precipitation expected for solar geoengineering is unlikely to be as important as the temperature-driven shift from solid to liquid precipitation for forcing Himalayan glacier change. The termination of geoengineering at 2069 under G3 leads to temperature rise of about 1.3 °C over the period 2070–2089 relative to the period 2050-2069 and corresponding increase in annual mean glacier volume loss rate from 0.17 to 1.1 % yr−1, which is higher than the 0.66 % yr−1 under RCP8.5 during 2070–2089.

  13. Role of sucrose in the heterogeneous uptake of dimethylamine by ammonium sulfate aerosol particles

    Science.gov (United States)

    Chu, Y.; Chan, C. K.

    2016-12-01

    Alkyl amines are important alkaline gases besides ammonia in the atmosphere and widely detected in both gas and particle phases. Heterogeneous uptake by pre-existing particles containing acids as well as ammonium salts is one of the major pathways of alkyl amines partitioning into aerosols. Recently, phase state of ammonium salt particles has been revealed to largely affect the degree of alkyl amines uptake. Using an electrodynamic balance coupled with Raman spectroscopy, we extend the study by investigating the alkyl amine uptake by ammonium sulfate (AS) - sucrose mixed particles, since ambient aerosols usually consist of a mixed phase of organics and inorganics. Sucrose is a surrogate of hydrophilic viscous organics that can alter the phase of AS at low relative humidity (RH) and dimethylamine (DMA) is selected for its abundance amongst alkyl amine compounds. DMA uptake occurred effectively at not only 70% RH but also RH as low as 10%, significantly below the AS crystallization point. The net uptake coefficient decreased as RH decreased for fixed initial AS - sucrose particle compositions. Interestingly, it followed a first increasing then decreasing trend as sucrose molar fraction increased from 0 to 0.5, at RH below 30%. Sucrose, albeit inert to DMA vapor, indirectly affected the interaction between DMA and AS - sucrose particles. On one hand, it absorbed water at low RH and delayed the efflorescence of AS to promote DMA uptake. On the other hand, the particle became more viscous with higher sucrose concentration and exhibited an effective mass transport barrier. Hence, the uptake of alkyl amines may occur slowly once ammonium salts are mixed with viscous organics, such as those secondary organic materials formed via the oxidation of biogenic volatile organic compounds, in the particle phase. Acknowledgment This work is supported by Research Grants Council (RGC) of Hong Kong Special Administrative Region, China (GRF 16300214). The grant from Hong Kong RGC Ph

  14. Volcanic signals in oceans

    KAUST Repository

    Stenchikov, Georgiy L.

    2009-08-22

    Sulfate aerosols resulting from strong volcanic explosions last for 2–3 years in the lower stratosphere. Therefore it was traditionally believed that volcanic impacts produce mainly short-term, transient climate perturbations. However, the ocean integrates volcanic radiative cooling and responds over a wide range of time scales. The associated processes, especially ocean heat uptake, play a key role in ongoing climate change. However, they are not well constrained by observations, and attempts to simulate them in current climate models used for climate predictions yield a range of uncertainty. Volcanic impacts on the ocean provide an independent means of assessing these processes. This study focuses on quantification of the seasonal to multidecadal time scale response of the ocean to explosive volcanism. It employs the coupled climate model CM2.1, developed recently at the National Oceanic and Atmospheric Administration\\'s Geophysical Fluid Dynamics Laboratory, to simulate the response to the 1991 Pinatubo and the 1815 Tambora eruptions, which were the largest in the 20th and 19th centuries, respectively. The simulated climate perturbations compare well with available observations for the Pinatubo period. The stronger Tambora forcing produces responses with higher signal-to-noise ratio. Volcanic cooling tends to strengthen the Atlantic meridional overturning circulation. Sea ice extent appears to be sensitive to volcanic forcing, especially during the warm season. Because of the extremely long relaxation time of ocean subsurface temperature and sea level, the perturbations caused by the Tambora eruption could have lasted well into the 20th century.

  15. Aerosols upwind of Mexico City during the MILAGRO campaign: regional scale biomass burning, dust and volcanic ash from aircraft measurements

    Science.gov (United States)

    Junkermann, W.; Steinbrecher, R.

    2009-04-01

    During the MILAGRO Campaign March/April 2006 a series of aircraft flights with the FZK microlight D-MIFU were performed in the area southeast of Mexico City starting from Puebla airport, circling the national park area of Ixtachiuatl and Popocatepetl and scanning the Chalco valley down to Cuautla in the Cuernavaca province. All flights were combined with vertical profiles up to 4500 m a.s.l. in several locations, typically north of volcano Ixtachiuatl on the Puebla side, above Chalco or Tenago del Aire and south of volcano Popocatepetl, either at Cuautla or Atlixco. In Tenango del Aire a ceilometer was additionally operated continuously for characterization of the planetary boundary layer. The aircraft carried a set of aerosol instrumentation, fine and coarse particles and size distributions as well as a 7 wavelength aethalometer. Additionally meteorological parameters, temperature and dewpoint, global radiation and actinic radiation balance, respectively photolysis rates, and ozone concentrations were measured. The instrumentation allowed to characterize the aerosol according to their sources and also their impact on radiation transfer. Biomass burning aerosol, windblown dust and volcanic ash were identified within the upwind area of Mexico City with large differences between the dry season in the first weeks of the campaign and the by far cleaner situation after beginning thunderstorm activity towards the end of the campaign. Also the aerosol characteristics inside and outside the Mexico City basin were often completely different. With wind speeds of ~ 5 m/sec from southerly directions in the Chalco valley the aerosol mixture can reach the City within ~ 2 h. Rural aerosol mixtures from the Cuernavaca plain were mixed during the transport with dust from the MC basin. Very high intensity biomass burning plumes normally reached higher altitudes and produced pyrocumulus clouds. These aerosols were injected mainly into the free troposphere. Within the MC basin a large

  16. Uptake of Organic Vapors by Sulfate Aerosols: Physical and Chemical Processes

    Science.gov (United States)

    Michelsen, R. R.; Ashbourn, S. F. M.; Iraci, L.T.; Staton, S. J. R.

    2003-01-01

    While it is known that upper tropospheric sulfate particles contain a significant amount of organic matter, both the source of the organic fraction and its form in solution are unknown. These studies explore how the chemical characteristics of the molecules and surfaces in question affect heterogeneous interactions. The solubilities of acetaldehyde [CH3CHO] and ethanol [CH3CH20H] in cold, aqueous sulfuric acid solutions have been measured by Knudsen cell studies. Henry's law solubility coefficients range from 10(exp 2) to 10(exp 5) M/atm for acetaldehyde, and from 10(exp 4) to 10(exp 9) M/atm for ethanol under upper tropospheric conditions (210-240 K, 40-80 wt. % H2S04). The multiple solvation pathways (protonation, enolization, etc.) available to these compounds in acidic aqueous environments will be discussed. Preliminary results from the interaction of acetaldehyde with solutions of formaldehyde in sulfuric acid will be presented as well. The physical and chemical processes that affect organic uptake by aqueous aerosols will be explored, with the aim of evaluating organic species not yet studied in low temperature aqueous sulfuric acid.

  17. Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing

    Directory of Open Access Journals (Sweden)

    S. T. Martin

    2003-10-01

    Full Text Available The effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US and once for lower side (LS of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2  (g SO42−−1, which compare to US values of 0.030 and 13.9 m2 (g SO42−−1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m2− are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL = −0.750, FU = −0.930, and

  18. Gas/aerosol-ash interaction in volcanic plumes: New insights from surface analyses of fine ash particles

    Science.gov (United States)

    Delmelle, Pierre; Lambert, Mathieu; Dufrêne, Yves; Gerin, Patrick; Óskarsson, Niels

    2007-07-01

    The reactions occurring between gases/aerosols and silicate ash particles in volcanic eruption plumes remain poorly understood, despite the fact that they are at the origin of a range of volcanic, environmental, atmospheric and health effects. In this study, we apply X-ray photoelectron spectroscopy (XPS), a surface-sensitive technique, to determine the chemical composition of the near-surface region (2-10 nm) of nine ash samples collected from eight volcanoes. In addition, atomic force microscopy (AFM) is used to image the nanometer-scale surface structure of individual ash particles isolated from three samples. We demonstrate that rapid acid dissolution of ash occurs within eruption plumes. This process is favoured by the presence of fluoride and is believed to supply the cations involved in the deposition of sulphate and halide salts onto ash. AFM imaging also has permitted the detection of extremely thin (< 10 nm) coatings on the surface of ash. This material is probably composed of soluble sulphate and halide salts mixed with sparingly soluble fluoride compounds. The surface approach developed here offers promising aspects for better appraising the role of gas/aerosol-ash interaction in dictating the ability of ash to act as sinks for various volcanic and atmospheric chemical species as well as sources for others.

  19. Aerosol optical thickness of Mt. Etna volcanic plume retrieved by means of the Airborne Multispectral Imaging Spectrometer (MIVIS

    Directory of Open Access Journals (Sweden)

    L. Merucci

    2003-06-01

    Full Text Available Within the framework of the European MVRRS project (Mitigation of Volcanic Risk by Remote Sensing Techniques, in June 1997 an airborne campaign was organised on Mt. Etna to study different characteristics of the volcanic plume emitted by the summit craters in quiescent conditions. Digital images were collected with the Airborne Multispectral Imaging Spectrometer (MIVIS, together with ground-based measurements. MIVIS images were used to calculate the aerosol optical thickness of the volcanic plume. For this purpose, an inversion algorithm was developed based on radiative transfer equations and applied to the upwelling radiance data measured by the sensor. This article presents the preliminary results from this inversion method. One image was selected following the criteria of concomitant atmospheric ground-based measurements necessary to model the atmosphere, plume centrality in the scene to analyse the largest plume area and cloudless conditions. The selected image was calibrated in radiance and geometrically corrected. The 6S (Second Simulation of the Satellite Signal in the Solar Spectrum radiative transfer model was used to invert the radiative transfer equation and derive the aerosol optical thickness. The inversion procedure takes into account both the spectral albedo of the surface under the plume and the topographic effects on the refl ected radiance, due to the surface orientation and elevation. The result of the inversion procedure is the spatial distribution of the plume optical depth. An average value of 0.1 in the wavelength range 454-474 nm was found for the selected measurement day.

  20. Cryo-transmission electron microscopy imaging of the morphology of submicrometer aerosol containing organic acids and ammonium sulfate.

    Science.gov (United States)

    Veghte, Daniel P; Bittner, Danielle Rae; Freedman, Miriam Arak

    2014-03-04

    The effects of aerosol particles on heterogeneous atmospheric chemistry and climate are determined in part by the internal arrangement of compounds within the particles. To characterize the morphology of internally mixed aerosol particles in the accumulation mode size regime, we have used cryo-transmission electron microscopy to investigate the phase separation behavior of dry, submicrometer particles composed of ammonium sulfate mixed with carboxylic acids (adipic, azelaic, citric, glutaric, malonic, pimelic, suberic, and succinic acid). Determining the morphology of dry particles is important for understanding laboratory studies of aerosol optical properties, reactivity, and cloud condensation nucleus activity, results from field instruments where aerosol particles are dried prior to analysis, and atmospheric processes like deposition mode heterogeneous ice nucleation that occur on dried particles. We observe homogeneous morphologies for highly soluble organic compounds. For organic compounds with limited aqueous solubility, partially engulfed structures are observed. At intermediate aqueous solubilities, small particles are homogeneous and larger particles are partially engulfed. Results are compared to previous studies of liquid-liquid phase separation in supermicrometer particles and the impact of these dry particle morphologies on aerosol-climate interactions are discussed.

  1. Comparative biological potency of acidic sulfate aerosols: implications for the interpretation of laboratory and field studies.

    Science.gov (United States)

    Schlesinger, R B; Chen, L C

    1994-04-01

    Biological responses to inhaled acid sulfates result from the deposition of hydrogen ion (H+) on airway surfaces. Thus, effects from sulfuric acid and ammonium bisulfate, the two major ambient species, have been assumed to be the same for a given H+ concentration within the exposure atmosphere, assuming similar respiratory tract deposition patterns. However, recent inhalation studies have indicated that sulfuric acid is disproportionately potent compared to ammonium bisulfate when the H+ content of the exposure atmosphere is considered, suggesting that some factors following inhalation affect the amount of H+ contacting airway surfaces. This study assessed a mechanism potentially underlying this phenomenon, namely, the extent of neutralization by respiratory tract ammonia. This was evaluated using a physical model system designed to mimic transit of these aerosols in the upper respiratory tract of the animal model used in this laboratory, the rabbit. The results suggest that for equal exposure quantities of H+, more acid would be deposited when sulfuric acid is inhaled than when ammonium bisulfate is inhaled. Furthermore, results from a series of in vitro exposures of tracheal epithelial cells to sulfuric acid and ammonium bisulfate aerosols indicated that the biological response is a function of the total mass (ionic) concentration of H+ deliverable to the cells or the total extractable H+ per particle. The results of this study have possible implications for ambient monitoring of particulate-associated strong acidity, suggesting that it may be necessary to specilate such measures into the relative amounts of H+ as sulfuric acid or ammonium bisulfate in order to most accurately relate atmospheric acid levels to observed health effects. In addition, since much of the ambient particulate-associated H+ exists as sulfuric acid/ammonium bisulfate mixtures rather than pure compounds, H(+)-associated health effects from controlled exposure studies of sulfuric acid may

  2. Effect of volcanic aerosol on stratospheric NO2 and N2O5 from 2002–2014 as measured by Odin-OSIRIS and Envisat-MIPAS

    Directory of Open Access Journals (Sweden)

    C. Adams

    2017-07-01

    Full Text Available Following the large volcanic eruptions of Pinatubo in 1991 and El Chichón in 1982, decreases in stratospheric NO2 associated with enhanced aerosol were observed. The Optical Spectrograph and Infrared Imaging Spectrometer (OSIRIS measured the widespread enhancements of stratospheric aerosol following seven volcanic eruptions between 2002 and 2014, although the magnitudes of these eruptions were all much smaller than the Pinatubo and El Chichón eruptions. In order to isolate and quantify the relationship between volcanic aerosol and NO2, NO2 anomalies were calculated using measurements from OSIRIS and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS. In the tropics, variability due to the quasi-biennial oscillation was subtracted from the time series. OSIRIS profile measurements indicate that the strongest anticorrelations between NO2 and volcanic aerosol extinction were for the 5 km layer starting  ∼  3 km above the climatological mean tropopause at the given latitude. OSIRIS stratospheric NO2 partial columns in this layer were found to be smaller than background NO2 levels during these aerosol enhancements by up to  ∼  60 % with typical Pearson correlation coefficients of R ∼ −0. 7. MIPAS also observed decreases in NO2 partial columns during periods affected by volcanic aerosol, with percent differences of up to  ∼  25 % relative to background levels. An even stronger anticorrelation was observed between OSIRIS aerosol optical depth and MIPAS N2O5 partial columns, with R ∼ −0. 9, although no link with MIPAS HNO3 was observed. The variation in OSIRIS NO2 with increasing aerosol was found to be consistent with simulations from a photochemical box model within the estimated model uncertainty.

  3. What We Can Learn from the Next Large Volcanic Eruption

    Science.gov (United States)

    Robock, A.

    2015-12-01

    The April 1982 eruption of El Chichón in México stimulated interest in the climate response to volcanic eruptions and produced very useful observations and modeling studies. The last large volcanic eruption, the June 15, 1991 eruption of Mt. Pinatubo in the Philippines, was the best observed eruption ever, and serves as a canonical example for studies of aerosol production and transport, climate response, and deposition on ice sheets. However, many aspects of both eruptions were poorly observed, climate model simulations of the response are imperfect, and new scientific issues, such as stratospheric sulfate geoengineering, raise new scientific questions that could be answered by better observations of the next large volcanic eruption. In this talk I will summarize what we know and do not know about large volcanic eruptions, and discuss new questions that can be addressed by being prepared for the next large eruption. These include: How and how fast will SO2 convert to sulfate aerosols? How will the aerosols grow? What will be the size distribution of the resulting sulfate aerosol particles? How will the aerosols be transported throughout the stratosphere? How much fine ash gets to the stratosphere, how long does it stay there, and what are its radiative and chemical impacts? How will temperatures change in the stratosphere as a result of the aerosol interactions with shortwave (particularly near IR) and longwave radiation? Are there large stratospheric water vapor changes associated with stratospheric aerosols? Is there an initial injection of water from the eruption? Is there ozone depletion from heterogeneous reactions on the stratospheric aerosols? As the aerosols leave the stratosphere, and as the aerosols affect the upper troposphere temperature and circulation, are there interactions with cirrus and other clouds?

  4. Optimal estimation retrieval of aerosol microphysical properties from SAGE II satellite observations in the volcanically unperturbed lower stratosphere

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    T. Deshler

    2010-05-01

    Full Text Available Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003. An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities, even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal size

  5. Raman Spectra and Nucleation Rates of Sulfuric Acid and Ammonium Sulfate Aerosols Supercooled with Respect to Ice

    Science.gov (United States)

    Knopf, D. A.; Koop, T.; Weers, U. G.; Krieger, U. K.; Peter, T.

    2001-12-01

    Sulfuric acid and ammonium sulfate aerosol particles can serve as ice condensation nuclei for the formation of upper tropospheric cirrus clouds. These clouds influence the global radiation budget by scattering of short wavelength (solar) radiation as well as by absorbing long wavelength (terrestrial) radiation. Knowledge of the thermodynamics and the nucleation rates of aerosols is fundamental for the understanding of formation processes of cirrus clouds. Here, we present a new investigation tool to observe phase transitions of aerosols supercooled with respect to ice. Confocal Raman microscopy is used to determine the phase changes and the morphology of the particles. Raman spectroscopy is employed to distinguish and to characterize the different phases inside the frozen particles. Single droplets with a diameter of typically 20-120 μ m are deposited on a hydrophobically coated Herasil-plate that is covered by a spacer and another plate. Since the gas phase volume of the cell is small compared to the liquid droplet volume the composition of the droplets remains fixed during temperature changes. The temperature of the droplets can be varied between 150-350~K. We present the first Raman spectra of aqueous H2SO4/H2O and (NH4)2SO4/H2O droplets for several concentrations and temperatures to the homogeneous ice nucleation limits. The analysis of the speciation of the components inside the droplets (e.g. sulfate vs. bisulfate ions) is compared to results from thermodynamic models. Evaluation of the freezing data gives upper limits for ice nucleation rates of droplets as a function of sulfuric acid or ammonium sulfate concentration.

  6. Sensitivity of thermal infrared nadir instruments to the chemical and microphysical properties of UTLS secondary sulfate aerosols

    Science.gov (United States)

    Sellitto, P.; Legras, B.

    2016-01-01

    Monitoring upper-tropospheric-lower-stratospheric (UTLS) secondary sulfate aerosols and their chemical and microphysical properties from satellite nadir observations is crucial to better understand their formation and evolution processes and then to estimate their impact on UTLS chemistry, and on regional and global radiative balance. Here we present a study aimed at the evaluation of the sensitivity of thermal infrared (TIR) satellite nadir observations to the chemical composition and the size distribution of idealised UTLS sulfate aerosol layers. The extinction properties of sulfuric acid/water droplets, for different sulfuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indices taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. IASI (Infrared Atmospheric Sounding Interferometer) pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealised aerosol layers, at typical UTLS conditions, on the brightness temperature spectra observed by this satellite instrument. We found a marked and typical spectral signature of these aerosol layers between 700 and 1200 cm-1, due to the absorption bands of the sulfate and bisulfate ions and the undissociated sulfuric acid, with the main absorption peaks at 1170 and 905 cm-1. The dependence of the aerosol spectral signature to the sulfuric acid mixing ratio, and effective number concentration and radius, as well as the role of interfering parameters like the ozone, sulfur dioxide, carbon dioxide and ash absorption, and temperature and water vapour profile uncertainties

  7. SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels

    Science.gov (United States)

    Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas

    2008-01-01

    Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.

  8. Characterization of particulate products for aging of ethylbenzene secondary organic aerosol in the presence of ammonium sulfate seed aerosol.

    Science.gov (United States)

    Huang, Mingqiang; Zhang, Jiahui; Cai, Shunyou; Liao, Yingmin; Zhao, Weixiong; Hu, Changjin; Gu, Xuejun; Fang, Li; Zhang, Weijun

    2016-09-01

    Aging of secondary organic aerosol (SOA) particles formed from OH- initiated oxidation of ethylbenzene in the presence of high mass (100-300μg/m(3)) concentrations of (NH4)2SO4 seed aerosol was investigated in a home-made smog chamber in this study. The chemical composition of aged ethylbenzene SOA particles was measured using an aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with a Fuzzy C-Means (FCM) clustering algorithm. Experimental results showed that nitrophenol, ethyl-nitrophenol, 2,4-dinitrophenol, methyl glyoxylic acid, 5-ethyl-6-oxo-2,4-hexadienoic acid, 2-ethyl-2,4-hexadiendioic acid, 2,3-dihydroxy-5-ethyl-6-oxo-4-hexenoic acid, 1H-imidazole, hydrated N-glyoxal substituted 1H-imidazole, hydrated glyoxal dimer substituted imidazole, 1H-imidazole-2-carbaldehyde, N-glyoxal substituted hydrated 1H-imidazole-2-carbaldehyde and high-molecular-weight (HMW) components were the predominant products in the aged particles. Compared to the previous aromatic SOA aging studies, imidazole compounds, which can absorb solar radiation effectively, were newly detected in aged ethylbenzene SOA in the presence of high concentrations of (NH4)2SO4 seed aerosol. These findings provide new information for discussing aromatic SOA aging mechanisms.

  9. Fingerprinting El Nino Southern Ocean events using oxygen triple isotopic composition of aerosol sulfate from the South Pole snow pit samples

    Science.gov (United States)

    Thiemens, M. H.; Abaunza Quintero, M. M.; Shaheen, R.; Jackson, T. L.; McCabe, J.; Savarino, J. P.

    2011-12-01

    According to the Intergovernmental Panel on Climate Change 4th assessment report [IPCC 2007], aerosols are the largest source of uncertainty in modeling the earth's radiative budget. Sulfate aerosols contributes to global cooling that may mask warming effect by greenhouse gases, therefore, high resolution record of aerosol sulfate can help to understand the impact of anthropogenic activities and natural variations on climate change. Sulfate aerosols were extracted from the ice pit samples obtained from the South Pole (1979-2002) at a high resolution temporal record of the winter and summer seasons. To insure highest measurement ability of very small samples (few nano moles) a hydrogen peroxide cleaning method was developed to remove organic impurities from aerosols which otherwise significantly affect O-triple isotopic measurement of the sulfates. Preliminary data indicated non sea salt contributions of 70-95% with a range in δ18OVSMOW = -1.86 -12% and Δ17O = 0.8-3.7% for the years 1990-2001. The positive Δ17O of sulfate derives from aqueous phase oxidation of SO2 by H2O2 and O3 and involves transfer of the isotopic anomaly from the oxidant to the product sulfate. All other sulfate sources (sea salt sulfates and primary sulfates from fossil fuel combustion), including gas-phase oxidation by OH in the troposphere, metal catalyzed oxidation of S(IV) to S(VI), are strictly mass dependent (Δ17O = 0%). The magnitude of the transfer of the Δ17O varies according to the relative contribution from H2O2 at pH 6 (Δ17O = 8%). Seasonal variations of these oxidants and their contribution to S(IV) oxidation will be discussed. Since our samples include the time period 1977-2002, each year divided into two parts (winter and summer season's aerosols), in addition to seasonal variation in sulfate oxidation pathways, we may also be able to assess if the oxidation cycle of sulfate changes during El Niño years.

  10. The influence of eruption season on the global aerosol evolution and radiative impact of tropical volcanic eruptions

    Directory of Open Access Journals (Sweden)

    M. Toohey

    2011-08-01

    Full Text Available Simulations of tropical volcanic eruptions using a general circulation model with coupled aerosol microphysics are used to assess the influence of season of eruption on the aerosol evolution and radiative impacts at the Earth's surface. This analysis is presented for eruptions with SO2 injection magnitudes of 17 and 700 Tg, the former consistent with estimates of the 1991 Mt. Pinatubo eruption, the later a near-"super eruption". For each eruption magnitude, simulations are performed with eruptions at 15° N, at four equally spaced times of year, and sensitivity to eruption season is quantified as the difference between the maximum and minimum cumulative anomalies.

    Eruption season has a significant influence on aerosol optical depth (AOD and clear-sky shortwave (SW radiative flux anomalies for both eruption magnitudes. The sensitivity to eruption season for both fields is generally weak in the tropics, but increases in the mid- and high latitudes, reaching maximum values of ~80 %. Global mean AOD and clear-sky SW anomalies show sensitivity to eruption season on the order of 15–20 %, which results from differences in aerosol effective radius for the different eruption seasons. Smallest aerosol size and largest cumulative impact result from a January eruption for the Pinatubo-magnitude, and from a July eruption for the near-super eruption. In contrast to AOD and clear-sky SW anomalies, all-sky SW anomalies are found to be insensitive to season of eruption for the Pinatubo-magnitude eruption experiment, due to the reflection of solar radiation by clouds in the mid- to high latitudes. However, differences in all-sky SW anomalies between eruptions in different seasons are significant for the larger eruption magnitude, and the ~15 % sensitivity to eruption season of the global mean all-sky SW anomalies is comparable to the sensitivity of global mean AOD and clear-sky SW anomalies. Our estimates of sensitivity to eruption season

  11. The influence of eruption season on the global aerosol evolution and radiative impact of tropical volcanic eruptions

    Directory of Open Access Journals (Sweden)

    M. Toohey

    2011-12-01

    Full Text Available Simulations of tropical volcanic eruptions using a general circulation model with coupled aerosol microphysics are used to assess the influence of season of eruption on the aerosol evolution and radiative impacts at the Earth's surface. This analysis is presented for eruptions with SO2 injection magnitudes of 17 and 700 Tg, the former consistent with estimates of the 1991 Mt. Pinatubo eruption, the later a near-"super eruption". For each eruption magnitude, simulations are performed with eruptions at 15° N, at four equally spaced times of year. Sensitivity to eruption season of aerosol optical depth (AOD, clear-sky and all-sky shortwave (SW radiative flux is quantified by first integrating each field for four years after the eruption, then calculating for each cumulative field the absolute or percent difference between the maximum and minimum response from the four eruption seasons. Eruption season has a significant influence on AOD and clear-sky SW radiative flux anomalies for both eruption magnitudes. The sensitivity to eruption season for both fields is generally weak in the tropics, but increases in the mid- and high latitudes, reaching maximum values of ~75 %. Global mean AOD and clear-sky SW anomalies show sensitivity to eruption season on the order of 15–20 %, which results from differences in aerosol effective radius for the different eruption seasons. Smallest aerosol size and largest cumulative impact result from a January eruption for Pinatubo-magnitude eruption, and from a July eruption for the near-super eruption. In contrast to AOD and clear-sky SW anomalies, all-sky SW anomalies are found to be insensitive to season of eruption for the Pinatubo-magnitude eruption experiment, due to the reflection of solar radiation by clouds in the mid- to high latitudes. However, differences in all-sky SW anomalies between eruptions in different seasons are significant for the larger eruption magnitude, and the ~15 % sensitivity to

  12. Physical and Radiative Properties of Aerosol Particles in the Caribbean: Influence of African Dust and Soufriere Volcanic Ash

    Science.gov (United States)

    Villanueva-Birriel, C. M.; Mayol-Bracero, O. L.; Sheridan, P.; Ogren, J. A.

    2007-12-01

    Atmospheric particles such as dust and volcanic ash have the potential of influencing the earth's radiative budget directly by scattering or absorbing solar radiation in the atmosphere and indirectly by affecting cloud condensation nuclei (CCN) concentrations and, therefore, cloud albedo. The radiatively-important properties of atmospheric particles are determined at the most fundamental level by their chemical composition and size distributions; therefore, the importance of studying the chemical, physical, and optical aerosol properties. Over the summer months, the island of Puerto Rico receives African dust incursions that reduce visibility and have an impact on public health, ecosystem, and climate. Visibility is also negatively affected when the island receives south-east winds and the Soufriere volcano (Montserrat Island) has been active. Here we present preliminary results of measurements performed during 2006 and 2007 at Cape San Juan, a ground-based station located at the northeastern tip of Puerto Rico. The cases investigated showed three possible types of air masses: clean (C), with African Dust (AD), and with volcanic ash (VA) from the Soufriere. We used a condensation particle counter to determine the particle number concentration, a sunphotometer (part of the AERONET) to determine volume size distributions and aerosol optical thickness (AOT), a 3-wavelength nephelometer to determine the scattering coefficients, and a 3-wavelength particle/soot absorption photometer (PSAP) for the absorption coefficients. The particle number concentrations were higher for AD and VA periods (up to about 700 cm-3 on average for both cases) in contrast to ~400 cm-3 for the C period. Volume size distributions showed bimodal distributions for the three cases with a greater influence of the coarse fraction for the C and VA periods and an increase in the fine particles for the AD period. The total scattering coefficient showed higher values for the AD (30 Mm-1) and the VA (26

  13. A study of uncertainties in the sulfate distribution and its radiative forcing associated with sulfur chemistry in a global aerosol model

    Directory of Open Access Journals (Sweden)

    D. Goto

    2011-04-01

    Full Text Available The direct radiative forcing by sulfate aerosols is still uncertain, mainly because the uncertainties are largely derived from differences in sulfate column burdens and its vertical distributions among global aerosol models. One of possible reasons of the large difference in the computed values is that the radiative forcing delicately depends on various simplifications of the sulfur processes made in the models. In this study, therefore, we investigated impacts of different parts of the sulfur chemistry module in a global aerosol model, SPRINTARS, on the sulfate distribution and its radiative forcing. Important studies were effects of simplified and more physical-based sulfur processes in terms of treatment of sulfur chemistry, oxidant chemistry, and dry deposition process of sulfur components. The results showed that the difference in the aqueous-phase sulfur chemistry among these treatments has the largest impact on the sulfate distribution. Introduction of all the improvements mentioned above brought the model values noticeably closer to in-situ measurements than those in the simplified methods used in the original SPRINTARS model. At the same time, these improvements also led the computed sulfate column burdens and its vertical distributions in good agreement with other AEROCOM model values. The global annual mean radiative forcings due to aerosol direct effect of anthropogenic sulfate was thus estimated to be −0.3 W m−2, whereas the original SPRINTARS model showed −0.2 W m−2. The magnitude of the difference between original and improved methods was approximately 50% of the uncertainty among estimates by the world's global aerosol models reported by the IPCC-AR4 assessment report. Findings in the present study, therefore, may suggest that the model differences in the simplifications of the sulfur processes are still a part of the large uncertainty in their simulated radiative forcings.

  14. What do we need to know to model the microphysical evolution of volcanic clouds and how can we make these measurements?

    Science.gov (United States)

    English, J. M.; Toon, O. B.; Mills, M. J.

    2015-12-01

    Large volcanic eruptions can inject millions of tons of ash, sulfate and gaseous precursors into the stratosphere. The magnitude and duration of the volcanic cloud on Earth's temperatures, circulation, clouds, and stratospheric ozone is strongly affected by the microphysical properties of the aerosol size distribution, which can evolve in complex ways. This presentation will cover the impacts and uncertainties associated with microphysical aerosol measurements and modeling of the 1991 Mount Pinatubo eruption, and valuable future measurements after the next large volcanic eruption. These additional measurements can help improve our understanding of stratospheric processes as well as possible consequences of large volcanic eruptions and hypothetical geoengineering scenarios on radiative forcing and chemistry.

  15. Volcanic-aerosol-induced changes in stratospheric ozone following the eruption of Mount Pinatubo

    Science.gov (United States)

    Grant, W. B.; Browell, E. V.; Fishman, J.; Brackett, V. G.; Fenn, M. A.; Butler, C. F.; Nganga, D.; Minga, A.; Cros, B.; Mayor, S. D.

    1994-01-01

    Measurements of lower stratospheric ozone in the Tropics using electrochemical concentrations cell (ECC) sondes and the airborne UV Differential Absorption Lidar (DIAL) system after the eruption of Mt. Pinatubo are compared with the Stratospheric Aerosol and Gas Experiment 2 (SAGE 2) and ECC sonde measurements from below the eruption to determine what changes have occurred as a result. Aerosol data from the Advanced Very High Resolution Radiometer (AVHRR) and the visible and IR wavelengths of the lidar system are used to examine the relationship between aerosols and ozone changes. Ozone decreases of 30 percent at altitudes between 19 and 26 km, partial column (16-28 km) decreases of about 27 D.U., and slight increases (5.4 D.U.) between 28 and 31 km are found in comparison with SAGE 2 climatological values.

  16. Lidar Observation of the 2014 Kelut Volcanic Stratospheric Aerosols at Kototabang, Indonesia

    Science.gov (United States)

    Abo, Makoto; Shibata, Yasukuni; Nagasawa, Chikao

    2016-06-01

    The Kelut (Kelud) volcano (7.9S, 112.3E) in the Java island of Indonesia erupted on 13 February 2014. The CALIOP observed that the eruption cloud reached 26km above sea level. We have observed this stratospheric aerosol from 28 February 2014 at equatorial lidar site located in the Sumatra island of Indonesia (0.2S, 100.3E). We observed the depolarization maximum to be up to 2km below the backscatter maximum in April 2014. We also observed the vertical transportation process of stratospheric aerosol to troposphere by equatorial Kelvin wave.

  17. Water-soluble material on aerosols collected within volcanic eruption clouds ( Fuego, Pacaya, Santiaguito, Guatamala).

    Science.gov (United States)

    Smith, D.B.; Zielinski, R.A.; Rose, W.I.; Huebert, B.J.

    1982-01-01

    In Feb. and March of 1978, filter samplers mounted on an aircraft were used to collect the aerosol fraction of the eruption clouds from three active Guatemalan volcanoes (Fuego, Pacaya, and Santiaguito). The elements dissolved in the aqueous extracts represent components of water-soluble material either formed directly in the eruption cloud or derived from interaction of ash particles and aerosol components of the plume. Calculations of enrichment factors, based upon concentration ratios, showed the elements most enriched in the extracts relative to bulk ash composition were Cd, Cu, V, F, Cl, Zn, and Pb.-from Authors

  18. Geophysical Fluid Dynamics Laboratory general circulation model investigation of the indirect radiative effects of anthropogenic sulfate aerosol

    Science.gov (United States)

    Ming, Yi; Ramaswamy, V.; Ginoux, Paul A.; Horowitz, Larry W.; Russell, Lynn M.

    2005-11-01

    The Geophysical Fluid Dynamics Laboratory (GFDL) atmosphere general circulation model, with its new cloud scheme, is employed to study the indirect radiative effect of anthropogenic sulfate aerosol during the industrial period. The preindustrial and present-day monthly mean aerosol climatologies are generated from running the Model for Ozone And Related chemical Tracers (MOZART) chemistry-transport model. The respective global annual mean sulfate burdens are 0.22 and 0.81 Tg S. Cloud droplet number concentrations are related to sulfate mass concentrations using an empirical relationship (Boucher and Lohmann, 1995). A distinction is made between "forcing" and flux change at the top of the atmosphere in this study. The simulations, performed with prescribed sea surface temperature, show that the first indirect "forcing" ("Twomey" effect) amounts to an annual mean of -1.5 W m-2, concentrated largely over the oceans in the Northern Hemisphere (NH). The annual mean flux change owing to the response of the model to the first indirect effect is -1.4 W m-2, similar to the annual mean forcing. However, the model's response causes a rearrangement of cloud distribution as well as changes in longwave flux (smaller than solar flux changes). There is thus a differing geographical nature of the radiation field than for the forcing even though the global means are similar. The second indirect effect, which is necessarily an estimate made in terms of the model's response, amounts to -0.9 W m-2, but the statistical significance of the simulated geographical distribution of this effect is relatively low owing to the model's natural variability. Both the first and second effects are approximately linearly additive, giving rise to a combined annual mean flux change of -2.3 W m-2, with the NH responsible for 77% of the total flux change. Statistically significant model responses are obtained for the zonal mean total indirect effect in the entire NH and in the Southern Hemisphere low

  19. Insulation effects of Icelandic dust and volcanic aerosols on snow and ice

    Science.gov (United States)

    Dragosics, Monika; Meinander, Outi; Jónsdóttir, Tinna; Dürig, Tobias; De Leeuw, Gerrit; Pálsson, Finnur; Dagsson-Waldhauserová, Pavla; Thorsteinsson, Throstur

    2016-04-01

    In the Arctic region, Iceland is an important source of dust due to ash production from volcanic eruptions. In addition dust is resuspended from the surface into the atmosphere as several dust storms occur each year. During volcanic eruptions and dust storms, material is deposited on the glaciers where it influences their energy balance. The effects of deposited volcanic ash on ice and snow melt were examined using laboratory and outdoor experiments. These experiments were made during the snow melt period using two different ash grain sizes (1 ϕ and 3.5 ϕ) from the Eyjafjallajökull 2010 eruption, collected on the glacier. Different amounts of ash were deposited on snow or ice after which the snow properties and melt were measured. The results show that a thin ash layer increases the snow and ice melt but an ash layer exceeding a certain critical thickness caused insulation. Ash with 1 ϕ in grain size insulated the ice below at a thickness of 9-15 mm. For the 3.5 ϕ grain size the insulation thickness is 13 mm. The maximum melt occurred at a thickness of 1 mm for the 1 ϕ and only 1-2 mm for 3.5 ϕ ash. A map of dust concentrations on Vatnajökull that represents the dust deposition during the summer of 2013 is presented with concentrations ranging from 0.2 up to 16.6 g m-2.

  20. Dry powder aerosols generated by standardized entrainment tubes from drug blends with lactose monohydrate: 1. Albuterol sulfate and disodium cromoglycate.

    Science.gov (United States)

    Xu, Zhen; Mansour, Heidi M; Mulder, Tako; McLean, Richard; Langridge, John; Hickey, Anthony J

    2010-08-01

    The major objective of this study was: discriminatory assessment of dry powder aerosol performance using standardized entrainment tubes (SETs) and lactose-based formulations with two model drugs. Drug/lactose interactive physical mixtures (2%w/w) were prepared. Their properties were measured: solid-state characterization of phase behavior and molecular interactions by differential scanning calorimetry and X-ray powder diffraction; particle morphology and size by scanning electron microscopy and laser diffraction; aerosol generation by SETs and characterization by twin-stage liquid impinger and Andersen cascade impactor operated at 60 L/min. The fine particle fraction (FPF) was correlated with SET shear stress (tau(s)), using a novel powder aerosol deaggregation equation (PADE). Drug particles were <5 microm in volume diameter with narrow unimodal distribution (Span <1). The lowest shear SET (tau(s) = 0.624 N/m(2)) gave a higher emitted dose (ED approximately 84-93%) and lower FPF (FPF(6.4) approximately 7-25%). In contrast, the highest shear SET (tau(s) = 13.143 N/m(2)) gave a lower ED (ED approximately 75-89%) and higher FPF (FPF(6.4) approximately 15-46%). The performance of disodium cromoglycate was superior to albuterol sulfate at given tau(s), as was milled with respect to sieved lactose monohydrate. Excellent correlation was observed (R(2) approximately 0.9804-0.9998) when pulmonary drug particle release from the surface of lactose carriers was interpreted by PADE linear regression for dry powder formulation evaluation and performance prediction.

  1. Catastrophic volcanism

    Science.gov (United States)

    Lipman, Peter W.

    1988-01-01

    Since primitive times, catastrophes due to volcanic activity have been vivid in the mind of man, who knew that his activities in many parts of the world were threatened by lava flows, mudflows, and ash falls. Within the present century, increasingly complex interactions between volcanism and the environment, on scales not previously experienced historically, have been detected or suspected from geologic observations. These include enormous hot pyroclastic flows associated with collapse at source calderas and fed by eruption columns that reached the stratosphere, relations between huge flood basalt eruptions at hotspots and the rifting of continents, devastating laterally-directed volcanic blasts and pyroclastic surges, great volcanic-generated tsunamis, climate modification from volcanic release of ash and sulfur aerosols into the upper atmosphere, modification of ocean circulation by volcanic constructs and attendent climatic implications, global pulsations in intensity of volcanic activity, and perhaps triggering of some intense terrestrial volcanism by planetary impacts. Complex feedback between volcanic activity and additional seemingly unrelated terrestrial processes likely remains unrecognized. Only recently has it become possible to begin to evaluate the degree to which such large-scale volcanic processes may have been important in triggering or modulating the tempo of faunal extinctions and other evolutionary events. In this overview, such processes are examined from the viewpoint of a field volcanologist, rather than as a previous participant in controversies concerning the interrelations between extinctions, impacts, and volcanism.

  2. Volcanic Eruptions and Climate

    Science.gov (United States)

    Robock, A.

    2012-12-01

    Large volcanic eruptions inject sulfur gases into the stratosphere, which convert to sulfate aerosols with an e-folding residence time of about one year. The radiative and chemical effects of these aerosol clouds produce responses in the climate system. Observations and numerical models of the climate system show that volcanic eruptions produce global cooling and were the dominant natural cause of climate change for the past millennium, on timescales from annual to century. Major tropical eruptions produce winter warming of Northern Hemisphere continents for one or two years, while high latitude eruptions in the Northern Hemisphere weaken the Asian and African summer monsoon. The Toba supereruption 74,000 years ago caused very large climate changes, affecting human evolution. However, the effects did not last long enough to produce widespread glaciation. An episode of four large decadally-spaced eruptions at the end of the 13th century C.E. started the Little Ice Age. Since the Mt. Pinatubo eruption in the Philippines in 1991, there have been no large eruptions that affected climate, but the cumulative effects of small eruptions over the past decade had a small effect on global temperature trends. The June 13, 2011 Nabro eruption in Eritrea produced the largest stratospheric aerosol cloud since Pinatubo, and the most of the sulfur entered the stratosphere not by direct injection, but by slow lofting in the Asian summer monsoon circulation. Volcanic eruptions warn us that while stratospheric geoengineering could cool the surface, reducing ice melt and sea level rise, producing pretty sunsets, and increasing the CO2 sink, it could also reduce summer monsoon precipitation, destroy ozone, allowing more harmful UV at the surface, produce rapid warming when stopped, make the sky white, reduce solar power, perturb the ecology with more diffuse radiation, damage airplanes flying in the stratosphere, degrade astronomical observations, affect remote sensing, and affect

  3. Radiative forcing estimates of sulfate aerosol in coupled climate-chemistry models with emphasis on the role of the temporal variability

    Directory of Open Access Journals (Sweden)

    C. Déandreis

    2012-06-01

    Full Text Available This paper describes the impact on the sulfate aerosol radiative effects of coupling the radiative code of a global circulation model with a chemistry-aerosol module. With this coupling, temporal variations of sulfate aerosol concentrations influence the estimate of aerosol radiative impacts. Effects of this coupling have been assessed on net fluxes, radiative forcing and temperature for the direct and first indirect effects of sulfate.

    The direct effect respond almost linearly to rapid changes in concentrations whereas the first indirect effect shows a strong non-linearity. In particular, sulfate temporal variability causes a modification of the short wave net fluxes at the top of the atmosphere of +0.24 and +0.22 W m−2 for the present and preindustrial periods, respectively. This change is small compared to the value of the net flux at the top of the atmosphere (about 240 W m−2. The effect is more important in regions with low-level clouds and intermediate sulfate aerosol concentrations (from 0.1 to 0.8 μg (SO4 m−3 in our model.

    The computation of the aerosol direct radiative forcing is quite straightforward and the temporal variability has little effect on its mean value. In contrast, quantifying the first indirect radiative forcing requires tackling technical issues first. We show that the preindustrial sulfate concentrations have to be calculated with the same meteorological trajectory used for computing the present ones. If this condition is not satisfied, it introduces an error on the estimation of the first indirect radiative forcing. Solutions are proposed to assess radiative forcing properly. In the reference method, the coupling between chemistry and climate results in a global average increase of 8% in the first indirect radiative forcing. This change reaches 50% in the most sensitive regions. However, the reference method is not suited to run long climate

  4. Aerosols Monitoring Network to Create a Volcanic ASH Risk Management System in Argentina and Chile

    Directory of Open Access Journals (Sweden)

    Quel Eduardo

    2016-01-01

    Full Text Available Two main decisions were made in Argentina to mitigate the impact of the recent volcanic activity in de country basically affected by the presence of volcanic ash in the air and deposited over the Argentinean territory. The first one was to create a risk management commission were this risk between others were studied, and second to develop new ground based remote sensing technologies to be able to identify and inform the risk close to the airports. In addition the Japanese government program for Science and Technology joint Research Partnership between Argentina, Chile and Japan for Sustainable Development (SATREPS accepted to fund this cooperation due to the potential future utilization of the research outcomes to the benefit of the society. This work present the actual achievements and expected advance of these projects that try to joint efforts between national and international agencies as well as countries on behalf of a better understanding of the risks and a joint collaboration on the mitigation of suspended ashes impact over the aerial navigation.

  5. Aerosols Monitoring Network to Create a Volcanic ASH Risk Management System in Argentina and Chile

    Science.gov (United States)

    Quel, Eduardo; Sugimoto, Nobuo; Otero, Lidia; Jin, Yoshitaka; Ristori, Pablo; Nishizawa, Tomoaki; González, Francisco; Papandrea, Sebastián; Shimizu, Atsushi; Mizuno, Akira

    2016-06-01

    Two main decisions were made in Argentina to mitigate the impact of the recent volcanic activity in de country basically affected by the presence of volcanic ash in the air and deposited over the Argentinean territory. The first one was to create a risk management commission were this risk between others were studied, and second to develop new ground based remote sensing technologies to be able to identify and inform the risk close to the airports. In addition the Japanese government program for Science and Technology joint Research Partnership between Argentina, Chile and Japan for Sustainable Development (SATREPS) accepted to fund this cooperation due to the potential future utilization of the research outcomes to the benefit of the society. This work present the actual achievements and expected advance of these projects that try to joint efforts between national and international agencies as well as countries on behalf of a better understanding of the risks and a joint collaboration on the mitigation of suspended ashes impact over the aerial navigation.

  6. Formation of Secondary Particulate Matter by Reactions of Gas Phase Hexanal with Sulfate Aerosol Particles

    Science.gov (United States)

    Zhang, J.

    2003-12-01

    The formation of secondary particulate matter from the atmospheric oxidation of organic compounds can significantly contribute to the particulate burden, but the formation of organic secondary particulate matter is poorly understood. One way of producing organic secondary particulate matter is the oxidation of hydrocarbons with seven or more carbon atoms to get products with low vapor pressure. However, several recent reports suggest that relatively low molecular weight carbonyls can enter the particle phase by undergoing heterogeneous reactions. This may be a very important mechanism for the formation of organic secondary particulate matter. Atmospheric aldehydes are important carbonyls in the gas phase, which form via the oxidation of hydrocarbons emitted from anthropogenic and biogenic sources. In this poster, we report the results on particle growth by the heterogeneous reactions of hexanal. A 5 L Continuous Stirred Tank Reactor (CSTR) is set up to conduct the reactions in the presence of seed aerosol particles of deliquesced ammonia bisulfate. Hexanal is added into CSTR by syringe pump, meanwhile the concentrations of hexanal are monitored with High Pressure Liquid Chromatograph (HPLC 1050). A differential Mobility Analyzer (TSI 3071) set to an appropriate voltage is employed to obtain monodisperse aerosols, and another DMA associated with a Condensation Nuclear Counter (TSI 7610) is used to measure the secondary particle size distribution by the reaction in CSTR. This permits the sensitive determination of particle growth due to the heterogeneous reaction, very little growth occurs when hexanal added alone. Results for the simultaneous addition of hexanal and alcohols will also be presented.

  7. A study of uncertainties in the sulfate distribution and its radiative forcing associated with sulfur chemistry in a global aerosol model

    Directory of Open Access Journals (Sweden)

    D. Goto

    2011-11-01

    Full Text Available The direct radiative forcing by sulfate aerosols is still uncertain, mainly because the uncertainties are largely derived from differences in sulfate column burdens and its vertical distributions among global aerosol models. One possible reason for the large difference in the computed values is that the radiative forcing delicately depends on various simplifications of the sulfur processes made in the models. In this study, therefore, we investigated impacts of different parts of the sulfur chemistry module in a global aerosol model, SPRINTARS, on the sulfate distribution and its radiative forcing. Important studies were effects of simplified and more physical-based sulfur processes in terms of treatment of sulfur chemistry, oxidant chemistry, and dry deposition process of sulfur components. The results showed that the difference in the aqueous-phase sulfur chemistry among these treatments has the largest impact on the sulfate distribution. Introduction of all the improvements mentioned above brought the model values noticeably closer to in-situ measurements than those in the simplified methods used in the original SPRINTARS model. At the same time, these improvements also brought the computed sulfate column burdens and its vertical distributions into good agreement with other AEROCOM model values. The global annual mean radiative forcing due to the direct effect of anthropogenic sulfate aerosol was thus estimated to be −0.26 W m−2 (−0.30 W m−2 with a different SO2 inventory, whereas the original SPRINTARS model showed −0.18 W m−2 (−0.21 W m−2 with a different SO2 inventory. The magnitude of the difference between original and improved methods was approximately 50% of the uncertainty among estimates by the world's global aerosol models reported by the IPCC-AR4 assessment report. Findings in the present study, therefore, may suggest that the model differences in the

  8. Effects of NO{sub x} and SO{sub 2} injections by supersonic aviation on sulfate aerosol and ozone in the troposphere and stratosphere

    Energy Technology Data Exchange (ETDEWEB)

    Dyominov, I.G.; Zadorozhny, A.M. [Novosibirsk State Univ. (Russian Federation); Elansky, N.F. [Russian Academy of Sciences, Moscow (Russian Federation). Inst. of Atmospheric Physics

    1997-12-31

    The impact of supersonic aviation on atmospheric ozone and sulfate aerosol is examined with the help of a two-dimensional dynamical/radiative/chemical model of ozonosphere including aerosol physics. For SO{sub 2} emissions from aircraft as gas, gas/particles (90%/10%) mix, and particles of 0.01 {mu}m radius the sulphate aerosol surface density at maximum of changes increases against its background value by {approx}50%, {approx}75%, and {approx}200%, respectively. This effect of SO{sub 2} emissions with insignificant NO{sub x} injection leads to a significant decrease of total ozone by 2015 in the entire atmosphere. For NO{sub x} emissions which are anticipated in future (EI(NO{sub x}) = 15) any kind of SO{sub 2} emission results in significant weakening of supersonic aviation impact on ozone layer in the Northern Hemisphere. (author) 14 refs.

  9. Particle morphologies and formation mechanisms of fine volcanic ash aerosol collected from the 2006 eruption of Augustine Volcano, Alaska

    Science.gov (United States)

    Rinkleff, P. G.; Cahill, C. F.

    2010-12-01

    Fine volcanic ash aerosol (35-0.09um) erupted in 2006 by Augustine Volcano, southwest of Anchorage, Alaska was collected by a DRUM cascade impactor and analyzed by scanning electron microscopy for individual particle chemistry and morphology. Results of these analyses show ash particles occur as either individual glass shard and mineral phase (plagioclase, magnetite, ilmenite, hornblende, etc.) particles or aggregates thereof. Individual glass shard ash particles are angular, uniformly-sized, consist of calc-alkaline whole-rock elements (Si, Al, Fe, Na, and Ca) and are not collocated on the sample media with non-silicate, Cl and S bearing sea salt particles. Aggregate particles occur as two types: pure ash aggregates and sea salt-cored aggregates. Pure ash aggregates are made up of only ash particles and contain no other constituents. Sea salt-cored aggregates are ash particles commingled with sea salts. Determining the formation processes of the different ash particle types need further investigation but some possibilities are proposed here. Individual ash particles may exist when the ambient air is generally dry, little electrical charge exists on ash particles, the eruptive cloud is generally dry, or the number of individual particles exceeds the scavenging capacity of the water droplets present. Another possibility is that ash aggregates may break apart as relative humidity drops over time and causes ash-laden water droplets to evaporate and subsequently break apart. Pure ash aggregates may form when the ambient air and plume is relatively dry but the ash has a significant charge to cause ash to aggregate. Or they could form during long-range transport when turbulent or Brownian motion can cause ash particles to collide and coagulate. Pure ash aggregates could also form as a result of water droplet scavenging and subsequent evaporation of water droplets, leaving behind only ash. In this case, droplets would not have interacted with a sea salt

  10. Aerosol properties and meteorological conditions in the city of Buenos Aires, Argentina, during the resuspension of volcanic ash from the Puyehue-Cordón Caulle eruption

    Science.gov (United States)

    Graciela Ulke, Ana; Torres Brizuela, Marcela M.; Raga, Graciela B.; Baumgardner, Darrel

    2016-09-01

    The eruption in June 2011 of the Puyehue-Cordón Caulle Volcanic Complex in Chile impacted air traffic around the Southern Hemisphere for several months after the initial ash emissions. The ash deposited in vast areas of the Patagonian Steppe was subjected to the strong wind conditions prevalent during the austral winter and spring experiencing resuspension over various regions of Argentina. In this study we analyze the meteorological conditions that led to the episode of volcanic ash resuspension which impacted the city of Buenos Aires and resulted in the closure of the two main airports in Buenos Aires area (Ezeiza and Aeroparque) on 16 October 2011. A relevant result is that resuspended material (volcanic ash plus dust) imprints a distinguishable feature within the atmospheric thermodynamic vertical profiles. The thermodynamic soundings show the signature of "pulses of drying" in layers associated with the presence of hygroscopic ash in the atmosphere that has already been reported in similar episodes after volcanic eruptions in other parts of the world. This particular footprint can be used to detect the probable existence of volcanic ash layers. This study also illustrates the utility of ceilometers to detect not only cloud base at airports but also volcanic ash plumes at the boundary layer and up to 7 km altitude. Aerosol properties measured in the city during the resuspension episode indicate the presence of enhanced concentrations of aerosol particles in the boundary layer along with spectral signatures in the measurements at the Buenos Aires AERONET site typical of ash plus dust advected towards the city. The mandatory aviation reports from the National Weather Service about airborne and deposited volcanic ash at the airport near the measurement site (Aeroparque) correlate in time with the enhanced concentrations. The presence of the resuspended material was detected by the CALIOP lidar overpassing the region. Since the dynamics of ash resuspension and

  11. Volcanic forcing for climate modeling: a new microphysics-based dataset covering years 1600–present

    Directory of Open Access Journals (Sweden)

    T. Peter

    2013-02-01

    Full Text Available As the understanding and representation of the impacts of volcanic eruptions on climate have improved in the last decades, uncertainties in the stratospheric aerosol forcing from large eruptions are now not only linked to visible optical depth estimates on a global scale but also to details on the size, latitude and altitude distributions of the stratospheric aerosols. Based on our understanding of these uncertainties, we propose a new model-based approach to generating a volcanic forcing for General-Circulation-Model (GCM and Chemistry-Climate-Model (CCM simulations. This new volcanic forcing, covering the 1600–present period, uses an aerosol microphysical model to provide a realistic, physically consistent treatment of the stratospheric sulfate aerosols. Twenty-six eruptions were modeled individually using the latest available ice cores aerosol mass estimates and historical data on the latitude and date of eruptions. The evolution of aerosol spatial and size distribution after the sulfur dioxide discharge are hence characterized for each volcanic eruption. Large variations are seen in hemispheric partitioning and size distributions in relation to location/date of eruptions and injected SO2 masses. Results for recent eruptions are in good agreement with observations. By providing accurate amplitude and spatial distributions of shortwave and longwave radiative perturbations by volcanic sulfate aerosols, we argue that this volcanic forcing may help refine the climate model responses to the large volcanic eruptions since 1600. The final dataset consists of 3-D values (with constant longitude of spectrally resolved extinction coefficients, single scattering albedos and asymmetry factors calculated for different wavelength bands upon request. Surface area densities for heterogeneous chemistry are also provided.

  12. Infrared limb emission measurements of aerosol in the troposphere and stratosphere

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    S. Griessbach

    2015-04-01

    Full Text Available Altitude resolved aerosol detection in the upper troposphere and lower stratosphere (UTLS is a challenging task for remote sensing instruments. Here, we introduce a new method for detecting aerosol in the UTLS based on infrared limb emission measurements. The method applies an improved aerosol-cloud-index that indicates infrared limb spectra affected by aerosol and ice clouds. For the discrimination between aerosol and ice clouds we developed a new method based on brightness temperature difference correlations. The discrimination thresholds for the new method were derived from radiative transfer simulations (including scattering and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS/Envisat measurements obtained in 2011. The method not only reliably separates aerosol from ice clouds, but also provides characteristic yet overlapping correlation patterns for volcanic ash and sulfate aerosol. We demonstrate the value of the new approach for volcanic ash and sulfate aerosol originating from the Grímsvötn (Iceland, Puyehue-Cordón Caulle (Chile and Nabro (Eritrea eruptions by comparing with Atmospheric Infrared Sounder (AIRS volcanic ash and SO2 measurements.

  13. In situ and space-based observations of the Kelud volcanic plume: The persistence of ash in the lower stratosphere

    Science.gov (United States)

    Vernier, Jean-Paul; Fairlie, T. Duncan; Deshler, Terry; Natarajan, Murali; Knepp, Travis; Foster, Katie; Wienhold, Frank G.; Bedka, Kristopher M.; Thomason, Larry; Trepte, Charles

    2016-09-01

    Volcanic eruptions are important causes of natural variability in the climate system at all time scales. Assessments of the climate impact of volcanic eruptions by climate models almost universally assume that sulfate aerosol is the only radiatively active volcanic material. We report satellite observations from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite after the eruption of Mount Kelud (Indonesia) on 13 February 2014 of volcanic materials in the lower stratosphere. Using these observations along with in situ measurements with the Compact Optical Backscatter AerosoL Detector (COBALD) backscatter sondes and optical particle counters (OPCs) made during a balloon field campaign in northern Australia, we find that fine ash particles with a radius below 0.3 µm likely represented between 20 and 28% of the total volcanic cloud aerosol optical depth 3 months after the eruption. A separation of 1.5-2 km between the ash and sulfate plumes is observed in the CALIOP extinction profiles as well as in the aerosol number concentration measurements of the OPC after 3 months. The settling velocity of fine ash with a radius of 0.3 µm in the tropical lower stratosphere is reduced by 50% due to the upward motion of the Brewer-Dobson circulation resulting a doubling of its lifetime. Three months after the eruption, we find a mean tropical clear-sky radiative forcing at the top of the atmosphere from the Kelud plume near -0.08 W/m2 after including the presence of ash; a value 20% higher than if sulfate alone is considered. Thus, surface cooling following volcanic eruptions could be affected by the persistence of ash and should be considered in climate simulations.

  14. Volcanic Eruptions and Climate: Outstanding Research Issues

    Science.gov (United States)

    Robock, Alan

    2016-04-01

    Large volcanic eruptions inject sulfur gases into the stratosphere, which convert to sulfate aerosols with an e-folding residence time of about one year. The radiative and chemical effects of this aerosol cloud produce responses in the climate system. Based on observations after major eruptions of the past and experiments with numerical models of the climate system, we understand much about their climatic impact, but there are also a number of unanswered questions. Volcanic eruptions produce global cooling, and are an important natural cause of interannual, interdecadal, and even centennial-scale climate change. One of the most interesting volcanic effects is the "winter warming" of Northern Hemisphere continents following major tropical eruptions. During the winter in the Northern Hemisphere following every large tropical eruption of the past century, surface air temperatures over North America, Europe, and East Asia were warmer than normal, while they were colder over Greenland and the Middle East. This pattern and the coincident atmospheric circulation correspond to the positive phase of the Arctic Oscillation. While this response is observed after recent major eruptions, most state-of-the-art climate models have trouble simulating winter warming. Why? High latitude eruptions in the Northern Hemisphere, while also producing global cooling, do not have the same impact on atmospheric dynamics. Both tropical and high latitude eruptions can weaken the Indian and African summer monsoon, and the effects can be seen in past records of flow in the Nile and Niger Rivers. Since the Mt. Pinatubo eruption in the Philippines in 1991, there have been no large eruptions that affected climate, but the cumulative effects of small eruptions over the past decade have had a small effect on global temperature trends. Some important outstanding research questions include: How much seasonal, annual, and decadal predictability is possible following a large volcanic eruption? Do

  15. Reactive bromine chemistry in Mt. Etna's volcanic plume: the influence of total Br, high temperature processing, aerosol loading and plume-air mixing

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    T. J. Roberts

    2014-03-01

    Full Text Available Volcanic emissions present a source of reactive halogens to the troposphere, through rapid plume chemistry that converts the emitted HBr to more reactive forms such as BrO. The nature of this process is poorly quantified, yet is of interest to understand volcanic impacts on the troposphere, and infer volcanic activity from volcanic gas measurements (i.e. BrO / SO2 ratios. Recent observations from Etna report an initial increase and subsequent plateau or decline in BrO / SO2 ratios with distance downwind. We present daytime PlumeChem model simulations that reproduce and explain the reported trend in BrO / SO2 at Etna including the initial rise and subsequent plateau. Through suites of model simulations we also investigate the influences of volcanic aerosol loading, bromine emission, and plume-air mixing rate on the downwind plume chemistry. Emitted volcanic HBr is converted into reactive bromine by autocatalytic bromine chemistry cycles whose onset is accelerated by the model high-temperature initialisation. These rapid chemistry cycles also impact the reactive bromine speciation through inter-conversion of Br, Br2, BrO, BrONO2, BrCl, HOBr. Formation of BrNO2 is also discussed. We predict a new evolution of Br-speciation in the plume, with BrO, Br2, Br and HBr as the main plume species in the near downwind plume whilst BrO, and HOBr are present in significant quantities further downwind (where BrONO2 and BrCl also make up a minor fraction. The initial rise in BrO / SO2 occurs as ozone is entrained into the plume whose reaction with Br promotes net formation of BrO. Aerosol has a modest impact on BrO / SO2 near-downwind (2 occurs as entrainment of oxidants HO2 and NO2 promotes net formation of HOBr and BrONO2, whilst the plume dispersion dilutes volcanic aerosol so slows the heterogeneous loss rates of these species. A higher volcanic aerosol loading enhances BrO / SO2 in the (> 6 km downwind plume. Simulations assuming low/medium and high Etna

  16. Effects of salbutamol aerosol combined with magnesium sulfate on T-lymphocyte subgroup and Th1/Th2 cytokines of pediatric asthma

    Science.gov (United States)

    Diao, Min; Min, Jie; Guo, Fei; Zhang, Chong-Lin

    2017-01-01

    The aim of the study was to analyze the effects of the intravenous infusion of salbutamol aerosol combined with magnesium sulfate in the treatment of pediatric asthma and the subsequent effects on the levels of T-lymphocyte subgroups and Th1/Th2 cytokines. A total of 86 patients with pediatric asthma, first diagnosed and treated at the Xuzhou Children's Hospital, were continuously selected and randomly divided into an observation group of 44 cases and control group of 42 cases. The patients in the control group were treated with budesonide atomization inhalation, while the children in the observation group were treated with intravenous infusion of salbutamol aerosol combined with magnesium sulfate. The therapeutic effects in the groups were compared. After treatment, the levels of serum CD3+ and CD8+ decreased when compared to before treatment; the levels of CD4+ and CD4+/CD8+ also increased, but the observation group had more significant improvement. Differences were statistically significant (P<0.05). After treatment, the levels of serum interleukin-2 (IL-2) and interferon-γ (IFN-γ) increased when compared to before, while levels of IL-4 and IL-6 decreased, and the observation group had more significant improvement. The differences were statistically significant (P<0.05). After treatment, the levels of VT, t-PTEF/t-E, MTIF/MTEF and TEF75/PTEF increased when compared to before; the observation group had more significant improvement. The differences were statistically significant (P<0.05). The effective rate and degree of treatment for the observation group were significantly higher than those of the control group and differences were statistically significant (P<0.05). The intravenous infusion of salbutamol aerosol combined with magnesium sulfate in the treatment of pediatric asthma can significantly improve therapeutic effects and lung functions, improve immune functions and relieve inflammatory reactions. Therefore, it indicates better clinical application and

  17. Size Distributions of Aerosol Sulfates and Nitrates in Beijing during the 2008 Olympic Games: Impacts of Pollution Control Measures and Regional Transport

    Institute of Scientific and Technical Information of China (English)

    WANG Xinfeng; WANG Tao; Ravi Kant PATHAK; Mattias HALLQUIST; GAO Xiaomei; NIE Wei; XUE Likun

    2013-01-01

    For the 2008 Olympic Games,drastic control measures were implemented on industrial and urban emissions of sulfur dioxide (SO2),nitrogen oxides (NOx) and other pollutants to address the issues of poor air quality in Beijing.To investigate the effects of SO2 and NOx reductions on the particulate sulfate and nitrate concentrations as well as their size distributions,size-segregated aerosol samples were collected using micro-orifice uniform deposit impactors (MOUDIs) at urban and downwind rural sites in Beijing before and after full-scale controls.During the sampling period,the mass concentrations of fine particles (PM1.8) at the urban and rural sites were 94.0 and 85.9 μg m-3,respectively.More than 90% of the sulfates and ~60%of nitrates formed as fine particles.Benefiting from the advantageous meteorological conditions and the source controls,sulfates were observed in rather low concentrations and primarily in condensation mode during the Olympics.The effects of the control measures were separately analyzed for the northerly and the southerly air-mass-dominated days to account for any bias.After the control measures were implemented,PM,sulfates,and nitrates were significantly reduced when the northerly air masses prevailed,with a higher percentage of reduction in larger particles.The droplet mode particles,which dominated the sulfates and nitrates before the controls were implemented,were remarkably reduced in mass concentration after the control measures were implemented.Nevertheless,when the polluted southerly air masses prevailed,the local source control measures in Beijing did not effectively reduce the ambient sulfate concentration due to the enormous regional contribution from the North China Plain.

  18. Size distributions of aerosol sulfates and nitrates in Beijing during the 2008 Olympic Games: Impacts of pollution control measures and regional transport

    Science.gov (United States)

    Wang, Xinfeng; Wang, Tao; Pathak, Ravi Kant; Hallquist, Mattias; Gao, Xiaomei; Nie, Wei; Xue, Likun; Gao, Jian; Gao, Rui; Zhang, Qingzhu; Wang, Wenxing; Wang, Shulan; Chai, Fahe; Chen, Yizhen

    2013-03-01

    For the 2008 Olympic Games, drastic control measures were implemented on industrial and urban emissions of sulfur dioxide (SO2), nitrogen oxides (NO x ) and other pollutants to address the issues of poor air quality in Beijing. To investigate the effects of SO2 and NO x reductions on the particulate sulfate and nitrate concentrations as well as their size distributions, size-segregated aerosol samples were collected using micro-orifice uniform deposit impactors (MOUDIs) at urban and downwind rural sites in Beijing before and after full-scale controls. During the sampling period, the mass concentrations of fine particles (PM1.8) at the urban and rural sites were 94.0 and 85.9 μg m-3, respectively. More than 90% of the sulfates and ˜60% of nitrates formed as fine particles. Benefiting from the advantageous meteorological conditions and the source controls, sulfates were observed in rather low concentrations and primarily in condensation mode during the Olympics. The effects of the control measures were separately analyzed for the northerly and the southerly air-mass-dominated days to account for any bias. After the control measures were implemented, PM, sulfates, and nitrates were significantly reduced when the northerly air masses prevailed, with a higher percentage of reduction in larger particles. The droplet mode particles, which dominated the sulfates and nitrates before the controls were implemented, were remarkably reduced in mass concentration after the control measures were implemented. Nevertheless, when the polluted southerly air masses prevailed, the local source control measures in Beijing did not effectively reduce the ambient sulfate concentration due to the enormous regional contribution from the North China Plain.

  19. Volcanic Eruptions and Climate

    Science.gov (United States)

    LeGrande, Allegra N.; Anchukaitis, Kevin J.

    2015-01-01

    Volcanic eruptions represent some of the most climatically important and societally disruptive short-term events in human history. Large eruptions inject ash, dust, sulfurous gases (e.g. SO2, H2S), halogens (e.g. Hcl and Hbr), and water vapor into the Earth's atmosphere. Sulfurous emissions principally interact with the climate by converting into sulfate aerosols that reduce incoming solar radiation, warming the stratosphere and altering ozone creation, reducing global mean surface temperature, and suppressing the hydrological cycle. In this issue, we focus on the history, processes, and consequences of these large eruptions that inject enough material into the stratosphere to significantly affect the climate system. In terms of the changes wrought on the energy balance of the Earth System, these transient events can temporarily have a radiative forcing magnitude larger than the range of solar, greenhouse gas, and land use variability over the last millennium. In simulations as well as modern and paleoclimate observations, volcanic eruptions cause large inter-annual to decadal-scale changes in climate. Active debates persist concerning their role in longer-term (multi-decadal to centennial) modification of the Earth System, however.

  20. Halogen Chemistry in Volcanic Plumes (Invited)

    Science.gov (United States)

    Roberts, Tjarda

    2017-04-01

    only partially constrained by available observations. Reactions on aerosol are a key driver of the chemistry and are affected by uncertainties in both the HOBr reactive uptake coefficient and the aerosol surface area. Recent work has explored the reactive uptake of HOBr on sulfate-rich aerosol, whilst field-measurements at Mt Etna have aimed to quantify the size-resolved primary aerosol emission, towards improving model representations of this highly non-linear volcanic plume halogen chemistry.

  1. Microphysical, macrophysical and radiative signatures of volcanic aerosols in trade wind cumulus observed by the A-Train

    Directory of Open Access Journals (Sweden)

    T. Yuan

    2011-02-01

    Full Text Available Increased aerosol concentrations can raise planetary albedo not only by reflecting sunlight and increasing cloud albedo, but also by changing cloud amount. However, detecting aerosol effect on cloud amount has been elusive to both observations and modeling due to potential buffering mechanisms and convolution of meteorology. Here through a natural experiment provided by long-term degassing of a low-lying volcano and use of A-Train satellite observations, we show aerosols are associated strongly with modification of trade cumulus cloud fields including decreased droplet size, decreased precipitation efficiency and increased cloud amount. We also demonstrate that the observed microphysical and macrophysical changes cannot be explained by synoptic meteorology or the orographic effect of the Hawaiian Islands. The "total shortwave aerosol forcing", resulting from direct and indirect forcings including both cloud albedo and cloud amount, is almost an order of magnitude higher than aerosol direct forcing alone. The precipitation reduction associated with enhanced aerosol leads to large changes in the energetics of air-sea exchange. Our results represent the first observational evidence of large-scale increase of cloud amount due to aerosols in a trade cumulus regime, which can be used to constrain the representation of aerosol-cloud interactions in climate models. The findings also have implications for volcano-climate interactions and climate mitigation research.

  2. Physical and optical properties of 2010 Eyjafjallajökull volcanic eruption aerosol: ground-based, Lidar and airborne measurements in France

    Directory of Open Access Journals (Sweden)

    M. Hervo

    2012-02-01

    Full Text Available During the Eyjafjallajökull eruption (14 April to 24 May 2010, the volcanic aerosol cloud was observed across Europe by several airborne in situ and ground-based remote-sensing instruments. On 18 and 19 May, layers of depolarizing particles (i.e. non-spherical particles were detected in the free troposphere above the Puy de Dôme station, (PdD, France with a Rayleigh-Mie LIDAR emitting at a wavelength of 355 nm, with parallel and crossed polarization channels. These layers in the free troposphere (FT were also well captured by simulations with the Lagrangian particle dispersion model FLEXPART, which furthermore showed that the ash was eventually entrained into the planetary boundary layer (PBL. Indeed, the ash cloud was then detected and characterized with a comprehensive set of in situ instruments at the Puy de Dôme station (PdD. In agreement with the FLEXPART simulation, up to 65 μg m−3 of particle mass and 2.2 ppb of SO2 were measured at PdD, corresponding to concentrations higher than the 95 percentile of 2 yr of measurements at PdD. Moreover, the number concentration of particles increased to 24 000 cm−3, mainly in the submicronic mode, but a supermicronic mode was also detected with a modal diameter of 2 μm. The resulting optical properties of the ash aerosol were characterized by a low scattering Ångström exponent (0.98, showing the presence of supermicronic particles. For the first time to our knowledge, the combination of in situ optical and physical characterization of the volcanic ash allowed the calculation of the mass-to-extinction ratio (η with no assumptions on the aerosol density. The mass-to-extinction ratio was found to be significantly different from the background boundary layer aerosol (max: 1.57 g m−2 as opposed to 0.33 ± 0.03 g m−2. Using this ratio, ash mass concentration in the volcanic plume derived from LIDAR measurements was found to be 655 ± 23

  3. Physical and optical properties of 2010 Eyjafjallajökull volcanic eruption aerosol: ground-based, Lidar and airborne measurements in France

    Science.gov (United States)

    Hervo, M.; Quennehen, B.; Kristiansen, N. I.; Boulon, J.; Stohl, A.; Fréville, P.; Pichon, J.-M.; Picard, D.; Labazuy, P.; Gouhier, M.; Roger, J.-C.; Colomb, A.; Schwarzenboeck, A.; Sellegri, K.

    2012-02-01

    During the Eyjafjallajökull eruption (14 April to 24 May 2010), the volcanic aerosol cloud was observed across Europe by several airborne in situ and ground-based remote-sensing instruments. On 18 and 19 May, layers of depolarizing particles (i.e. non-spherical particles) were detected in the free troposphere above the Puy de Dôme station, (PdD, France) with a Rayleigh-Mie LIDAR emitting at a wavelength of 355 nm, with parallel and crossed polarization channels. These layers in the free troposphere (FT) were also well captured by simulations with the Lagrangian particle dispersion model FLEXPART, which furthermore showed that the ash was eventually entrained into the planetary boundary layer (PBL). Indeed, the ash cloud was then detected and characterized with a comprehensive set of in situ instruments at the Puy de Dôme station (PdD). In agreement with the FLEXPART simulation, up to 65 μg m-3 of particle mass and 2.2 ppb of SO2 were measured at PdD, corresponding to concentrations higher than the 95 percentile of 2 yr of measurements at PdD. Moreover, the number concentration of particles increased to 24 000 cm-3, mainly in the submicronic mode, but a supermicronic mode was also detected with a modal diameter of 2 μm. The resulting optical properties of the ash aerosol were characterized by a low scattering Ångström exponent (0.98), showing the presence of supermicronic particles. For the first time to our knowledge, the combination of in situ optical and physical characterization of the volcanic ash allowed the calculation of the mass-to-extinction ratio (η) with no assumptions on the aerosol density. The mass-to-extinction ratio was found to be significantly different from the background boundary layer aerosol (max: 1.57 g m-2 as opposed to 0.33 ± 0.03 g m-2). Using this ratio, ash mass concentration in the volcanic plume derived from LIDAR measurements was found to be 655 ± 23 μg m-3 when the plume was located in the FT (3000 m above the sea level

  4. Present and potential future contributions of sulfate, black and organic carbon aerosols from China to global air quality, premature mortality and radiative forcing

    Science.gov (United States)

    Saikawa, Eri; Naik, Vaishali; Horowitz, Larry W.; Liu, Junfeng; Mauzerall, Denise L.

    Aerosols are harmful to human health and have both direct and indirect effects on climate. China is a major contributor to global emissions of sulfur dioxide (SO 2), a sulfate (SO 42-) precursor, organic carbon (OC), and black carbon (BC) aerosols. Although increasingly examined, the effect of present and potential future levels of these emissions on global premature mortality and climate change has not been well quantified. Through both direct radiative effects and indirect effects on clouds, SO 42- and OC exert negative radiative forcing (cooling) while BC exerts positive forcing (warming). We analyze the effect of China's emissions of SO 2, SO 42-, OC and BC in 2000 and for three emission scenarios in 2030 on global surface aerosol concentrations, premature mortality, and radiative forcing (RF). Using global models of chemical transport (MOZART-2) and radiative transfer (GFDL RTM), and combining simulation results with gridded population data, mortality rates, and concentration-response relationships from the epidemiological literature, we estimate the contribution of Chinese aerosols to global annual premature mortality and to RF in 2000 and 2030. In 2000, we estimate these aerosols cause approximately 470 000 premature deaths in China and an additional 30 000 deaths globally. In 2030, aggressive emission controls lead to a 50% reduction in premature deaths from the 2000 level to 240 000 in China and 10 000 elsewhere, while under a high emissions scenario premature deaths increase 50% from the 2000 level to 720 000 in China and to 40 000 elsewhere. Because the negative RF from SO 42- and OC is larger than the positive forcing from BC, Chinese aerosols lead to global net direct RF of -74 mW m -2 in 2000 and between -15 and -97 mW m -2 in 2030 depending on the emissions scenario. Our analysis indicates that increased effort to reduce greenhouse gases is essential to address climate change as China's anticipated reduction of aerosols will result in the

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

    Science.gov (United States)

    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.

  6. Triple oxygen and sulfur isotope analyses of sulfate extracted from voluminous volcanic ashes in the Oligocene John Day Formation: insight into dry climate conditions and ozone contribution to supereruptions

    Science.gov (United States)

    Workman, J.; Bindeman, I. N.; Martin, E.; Retallack, G.; Palandri, J. L.; Weldon, N.

    2014-12-01

    Large volume pyroclastic silicic eruptions emit hundreds of megatons of SO2 into the troposphere and stratosphere that is oxidized into sulfuric acid (H2SO4) by a variety of reactions with mass independent oxygen signatures (MIF), Δ17O>0. Sulfuric acid is then preserved as gypsum in parental volcanic deposits. Diagenic effects are mass dependent and can dilute, but otherwise do not affect MIF ratios. Pleistocene Yellowstone and Bishop tuffs and modern volcanic eruptions preserved under arid climate conditions in North American playa lakes, preserve small amounts of volcanic sulfate as gypsum. This gypsum's Δ17O>0, in combination with isotopic variations of δ18O, δ33S and δ34S is distinct from sedimentary sulfate and reveals its original MIF sulfate isotopic signal and the effect of super eruptions on the atmosphere, and ozone consumption in particular. We use linear algebraic equations to resolve volcanic versus sedimentary (MIF=0) sources. We have found that many large volume ignimbrites have very high initial Δ17O in volcanic sulfate that can only be acquired from reaction with stratospheric ozone. We here investigate nine thick (>2 m) ash beds ranging in age from ~33-23 Ma in the John Day Formation of central Oregon, including massive 28.6 Ma Picture Gorge tuff of newly identified Crooked River supercaldera. The 28.6 Ma Picture Gorge tuff (PGT) has the highest measured Δ17O of 3.5‰, and other tuffs (Tin Roof, Biotite, Deep Creek) have +1.3 to 3.4‰ Δ17O excesses. Sulfate from modern smaller tropospheric eruptions studied for comparison have a resolvable 0.4‰ range consistent with liquid-phase based H2O2 oxidation. The PGT is coeval with the ignimbrite flare-up in western N. America, the 28-29 Ma eruption of the 5000 km3 Fish Canyon tuff and the 28 Ma Never Summer Field eruption in Nebraska-Colorado that have the highest measured Δ17O of 6‰ (Bao et al. 2003). We speculate on the climatic/atmospheric effects of these multiple ~28 Ma supereruptions

  7. Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

    Directory of Open Access Journals (Sweden)

    Y. Wang

    2013-03-01

    Full Text Available We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3 from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60% and 80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC and Sichuan Basin (SCB, while nitrate and sulfate contribute equally over North China (NC. Based on emission reduction targets in the 12th (2011–2015 Five-Year Plan (FYP, China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. The amount of NH3 emissions in 2015 is uncertain, given the lack of sufficient information on the past and present levels of NH3 emissions in China. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their 2006 levels, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC, for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

  8. Role of soot particles and NO/sub x/ in the oxidation of SO/sub 2/ in aqueous solution: kinetics, mechanism, and impact on sulfate-aerosol formation

    Energy Technology Data Exchange (ETDEWEB)

    Chang, S.G.; Brodzinsky, R.; Oblath, S.; Markowitz, S.; Toossi, R.; Novakov, T.

    1980-11-01

    Two previously unrecognized processes were identified which could play an important role in terms of acid rain and sulfate aerosol formation: (1) the oxidation of SO/sub 2/ in water droplets containing soot particles, and (2) the oxidation of SO/sub 2/ by NO/sub x/ in water droplets. 6 figures, 3 tables.

  9. THE ROLE OF SOOT PARTICLES AND NO{sub x} IN THE OXIDATION OF SO{sub 2} IN AQUEOUS SOLUTION: KINETICS, MECHANISM, AND IMPACT ON SULFATE AEROSOL FORMATION

    Energy Technology Data Exchange (ETDEWEB)

    Chang, S.G.; Brodzinsky, R.; Oblath, S.; Markowitz, S.; Toossi, R.; Novakov, T.

    1980-11-01

    We have identified two previously unrecognized processes which could play an important role in terms of acid rain and sulfate aerosol formation: 1) the oxidation of SO{sub 2} in water droplets containing soot particles, and 2) the oxidation of SO{sub 2} by NO{sub x} in water droplets. The results of our investigation on these two systems are outlined.

  10. Real-world healthcare utilization in asthma patients using albuterol sulfate inhalation aerosol (ProAir® HFA with and without integrated dose counters

    Directory of Open Access Journals (Sweden)

    Kerwin EM

    2017-05-01

    Full Text Available Edward M Kerwin,1 Thomas J Ferro,2 Rinat Ariely,3 Debra E Irwin,4 Ruchir Parikh3 1Clinical Trials Division, Clinical Research Institute of Southern Oregon, PC, Medford, OR, 2Global Medical Affairs, 3Global Health Economics and Outcome Research, Teva Pharmaceuticals, Frazer, PA, 4Outcomes Research, Truven Health Analytics, Durham, NC, USA Background: Accurate tracking of the administered dose of asthma rescue inhalers is critical for optimal disease management and is related to reductions in rates of unscheduled health care utilization in asthma patients. There are few published data on the real-world impact of rescue inhalers with integrated dose counters (IDCs on health care resource utilization (HRU for asthma patients. This study evaluates HRU among users of ProAir® hydrofluoroalkane (HFA (albuterol sulfate inhalation aerosol, with IDC versus without IDC, in asthma patients.Methods: This was a retrospective administrative claims study of asthma patients receiving a new prescription for albuterol inhalation aerosol without IDC during 2 years (January 2011–December 2012 or with IDC during the first full year after IDC implementation in the USA (July 2013–July 2014. Six months of continuous enrollment with medical and prescription drug benefits were required before and after the first prescription during the study period. Data on respiratory-related hospitalizations and emergency department (ED visits were collected during the follow-up period.Results: A total of 135,305 (32% patients used albuterol inhalation aerosol with IDC, and 287,243 (68% patients received albuterol inhalation aerosol without IDC. After adjusting for baseline confounding factors, the odds ratio (OR for experiencing a respiratory-related hospitalization (OR=0.92; 95% confidence interval [CI] 0.88–0.96 or ED visit (OR=0.92; 95% CI 0.90–0.94 was significantly lower among patients using albuterol inhalation aerosol with IDC versus without IDC.Conclusion: In a real

  11. The impact of geoengineering aerosols on stratospheric temperature and ozone

    Energy Technology Data Exchange (ETDEWEB)

    Heckendorn, P; Luo, B P; Rozanov, E; Schraner, M; Peter, T [Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich (Switzerland); Weisenstein, D [AER, Lexington, MA (United States); Fueglistaler, S [DAMTP, University of Cambridge (United Kingdom); Thomason, L W, E-mail: patricia.heckendorn@env.ethz.c [NASA Langley Research Center, Hampton, VA (United States)

    2009-10-15

    Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model, to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H{sub 2}O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will be significantly reduced.

  12. The Impact of Geoengineering Aerosols on Stratospheric Temperature and Ozone

    Science.gov (United States)

    Heckendorn, P.; Weisenstein, D.; Fueglistaler, S.; Luo, B. P.; Rozanov, E.; Schraner, M.; Thomason, L. W.; Peter, T.

    2011-01-01

    Anthropogenic greenhouse gas emissions are warming the global climate at an unprecedented rate. Significant emission reductions will be required soon to avoid a rapid temperature rise. As a potential interim measure to avoid extreme temperature increase, it has been suggested that Earth's albedo be increased by artificially enhancing stratospheric sulfate aerosols. We use a 3D chemistry climate model, fed by aerosol size distributions from a zonal mean aerosol model. to simulate continuous injection of 1-10 Mt/a into the lower tropical stratosphere. In contrast to the case for all previous work, the particles are predicted to grow to larger sizes than are observed after volcanic eruptions. The reason is the continuous supply of sulfuric acid and hence freshly formed small aerosol particles, which enhance the formation of large aerosol particles by coagulation and, to a lesser extent, by condensation. Owing to their large size, these particles have a reduced albedo. Furthermore, their sedimentation results in a non-linear relationship between stratospheric aerosol burden and annual injection, leading to a reduction of the targeted cooling. More importantly, the sedimenting particles heat the tropical cold point tropopause and, hence, the stratospheric entry mixing ratio of H2O increases. Therefore, geoengineering by means of sulfate aerosols is predicted to accelerate the hydroxyl catalyzed ozone destruction cycles and cause a significant depletion of the ozone layer even though future halogen concentrations will he significantly reduced.

  13. Reconstructing Volcanic Forcing of Climate: Past, Present and Future

    Science.gov (United States)

    Toohey, M.; Timmreck, C.; Sigl, M.

    2015-12-01

    Radiative forcing resulting from major volcanic eruptions has been a dominant driver of climate variability during Earth's history. Including volcanic forcing in climate model simulations is therefore essential to recreate past climate variability, and provides the opportunity to test the ability of models to respond accurately to external forcing. Ice cores provide estimates of the volcanic sulfate loadings from past eruptions, from which radiative forcing can be reconstructed, with associated uncertainties. Using prior reconstructions, climate models have reproduced the gross features of global mean temperature variability reconstructed from climate proxies, although some significant differences between model results and reconstructions remain. There is much less confidence in the accuracy of the dynamical responses to volcanic forcing produced by climate models, and thus the regional aspects of post-volcanic climate anomalies are much more uncertain—a result which mirrors uncertainties in the dynamical responses to future climate change. Improvements in model's response to volcanic forcing may be possible through improving the accuracy of the forcing data. Recent advances on multiple fronts have motivated the development of a next-generation volcanic forcing timeseries for use in climate models, based on (1) improved dating and precision of ice core records, (2) better understanding of the atmospheric transport and microphysical evolution of volcanic aerosol, including its size distribution, and (3) improved representations of the spatiotemporal structure of volcanic radiative forcing. A new volcanic forcing data set, covering the past 2500 years, will be introduced and compared with prior reconstructions. Preliminary results of climate model simulations using the new forcing will also be shown, and current and future applications of the forcing set discussed.

  14. Improved aerosolization performance of salbutamol sulfate formulated with lactose crystallized from binary mixtures of ethanol-acetone.

    Science.gov (United States)

    Kaialy, Waseem; Ticehurst, Martyn D; Murphy, John; Nokhodchi, Ali

    2011-07-01

    It has been shown that dry powder inhaler (DPI) formulations typically achieve low fine particle fractions (poor performance). A commonly held theory is that this is due, at least in part, to low levels of detachment of drug from lactose during aerosolization as a result of strong adhesion of drug particles to the carrier surfaces. Therefore, the purpose of the present study is to overcome poor aerosolization performance of DPI formulation by modification of lactose particles. Lactose particles were crystallized by adding solution in water to different ratios of binary mixtures of ethanol-acetone. The results showed that modified lactose particles had exceptional aerosolization performance that makes them superior to commercial lactose particles. Morphology assessment showed that crystallized lactose particles were less elongated, more irregular in shape, and composed of smaller primary lactose particles compared with commercial lactose. Solid-state characterization showed that commercial lactose particles were α-lactose monohydrate, whereas crystallized lactose particles were a mixture of α-lactose monohydrate and β-lactose according to the ratio of ethanol-acetone used during crystallization process. The enhanced performance could be mainly due to rougher surface and/or higher amounts of fines compared with the lactose crystallized from pure ethanol or commercial lactose. Copyright © 2011 Wiley-Liss, Inc. and the American Pharmacists Association

  15. Lidar Observations of Aerosol Disturbances of the Stratosphere over Tomsk (56.5∘N; 85.0∘E in Volcanic Activity Period 2006–2011

    Directory of Open Access Journals (Sweden)

    Oleg E. Bazhenov

    2012-01-01

    Full Text Available The lidar measurements (Tomsk: 56.5∘N; 85.0∘E of the optical characteristics of the stratospheric aerosol layer (SAL in the volcanic activity period 2006–2011 are summarized and analyzed. The background SAL state with minimum aerosol content, observed since 1997 under the conditions of long-term volcanically quiet period, was interrupted in October 2006 by series of explosive eruptions of volcanoes of Pacific Ring of Fire: Rabaul (October 2006, New Guinea; Okmok and Kasatochi (July-August 2008, Aleutian Islands; Redoubt (March-April 2009, Alaska; Sarychev Peak (June 2009, Kuril Islands; Grimsvötn (May 2011, Iceland. A short-term and minor disturbance of the lower stratosphere was also observed in April 2010 after eruption of the Icelandic volcano Eyjafjallajokull. The developed regional empirical model of the vertical distribution of background SAL optical characteristics was used to identify the periods of elevated stratospheric aerosol content after each of the volcanic eruptions. Trends of variations in the total ozone content are also considered.

  16. Simulations of sulfate-nitrate-ammonium (SNA) aerosols during the extreme haze events over northern China in October 2014

    Science.gov (United States)

    Chen, Dan; Liu, Zhiquan; Fast, Jerome; Ban, Junmei

    2016-08-01

    Extreme haze events have occurred frequently over China in recent years. Although many studies have investigated the formation mechanisms associated with PM2.5 for heavily polluted regions in China based on observational data, adequately predicting peak PM2.5 concentrations is still challenging for regional air quality models. In this study, we evaluate the performance of one configuration of the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) and use the model to investigate the sensitivity of heterogeneous reactions on simulated peak sulfate, nitrate, and ammonium concentrations in the vicinity of Beijing during four extreme haze episodes in October 2014 over the North China Plain. The highest observed PM2.5 concentration of 469 µg m-3 occurred in Beijing. Comparisons with observations show that the model reproduced the temporal variability in PM2.5 with the highest PM2.5 values on polluted days (defined as days in which observed PM2.5 is greater than 75 µg m-3), but predictions of sulfate, nitrate, and ammonium were too low on days with the highest observed concentrations. Observational data indicate that the sulfur/nitric oxidation rates are strongly correlated with relative humidity during periods of peak PM2.5; however, the model failed to reproduce the highest PM2.5 concentrations due to missing heterogeneous/aqueous reactions. As the parameterizations of those heterogeneous reactions are not well established yet, estimates of SO2-to-H2SO4 and NO2/NO3-to-HNO3 reaction rates that depend on relative humidity were applied, which improved the simulation of sulfate, nitrate, and ammonium enhancement on polluted days in terms of both concentrations and partitioning among those species. Sensitivity simulations showed that the extremely high heterogeneous reaction rates and also higher emission rates than those reported in the emission inventory were likely important factors contributing to those peak PM2.5 concentrations.

  17. Simulations of Sulfate-Nitrate-Ammonium (SNA) aerosols during the extreme haze events over Northern China in 2014

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Dan; Liu, Zhiquan; Fast, Jerome D.; Ban, Junmei

    2016-08-30

    Extreme haze events have occurred frequently over China in recent years. Although many studies have investigated the formation mechanisms associated with PM2.5 for heavily polluted regions in China based on observational data, adequately predicting peak PM2.5 concentrations is still challenging for regional air quality models. In this study, we evaluate the performance of one configuration of the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) and use the model to investigate the sensitivity of heterogeneous reactions on simulated peak sulfate, nitrate, and ammonium concentrations in the vicinity of Beijing during four extreme haze episodes in October 2014 over the North China Plain. The highest observed PM2.5 concentration of 469 μg m-3 occurred in Beijing. Comparisons with observations show that the model reproduced the temporal variability in PM2.5 with the highest PM2.5 values on polluted days (defined as days in which observed PM2.5 is greater than 75 μg m-3), but predictions of sulfate, nitrate, and ammonium were too low on days with the highest observed concentrations. Observational data indicate that the sulfur/nitric oxidation rates are strongly correlated with relative humidity during periods of peak PM2.5; however, the model failed to reproduce the highest PM2.5 concentrations due to missing heterogeneous reactions. As the parameterizations of those reactions is not well established yet, estimates of SO2-to-H2SO4 and NO2/NO3-to-HNO3 reaction rates that depend on relative humidity were applied which improved the simulation of sulfate, nitrate, and ammonium enhancement on polluted days in terms of both concentrations and partitioning among those species. Sensitivity simulations showed that the extremely high heterogeneous reaction rates and also higher emission rates than those reported in the emission inventory

  18. Risk assessment of the impact of future volcanic eruptions on direct normal irradiance

    Science.gov (United States)

    Pagh Nielsen, Kristian; Blanc, Philippe; Vignola, Frank

    2016-04-01

    Stratospheric sulfate aerosols from Plinian volcanic eruptions affect the solar surface irradiance forcing by scattering the solar radiation as it passes through the Earth atmosphere. Since these aerosols have high single scattering albedos they mostly affect direct normal irradiances (DNI). The effect on global horizontal irradiance (GHI) is less because some of the scattered irradiance reaches the surface as diffuse horizontal irradiance (DHI) and adds to the GHI. DNI is the essential input to concentrating solar thermal electric power (CSP/STE) and concentrated photovoltaic (CPV) plants. Therefore, an assessment of the future potential variability in the DNI resource caused by Plinian volcanic eruptions is desirable. Based on investigations of the El Chichón and Pinatubo eruptions, the microphysical, and thereby optical, properties of the stratospheric sulfate aerosols are well known. Given these, radiative transfer computations of the DNI resource can be made. The DNI resource includes forward scattered irradiance within the acceptance angle of a given CSP/STE or CPV plant. The rarity of Plinian eruptions poses a challenge for assessing the statistical risk of future eruptions and its potential of risk in the electricity production. Here we present and discuss methods to account for these potential volcanic eruptions for technical and economical studies including scenarios with very high probability of exceedance (e.g. P99 scenarios) for risk assessment of DNI-based solar power projects.

  19. The Persistence of Volcanic Ash in the Tropical Stratosphere after the Kelud Eruption

    Science.gov (United States)

    Vernier, J. P.; Fairlie, T. D.; Deshler, T.; Knepp, T. N.; Natarajan, M.; Foster, K.; Trepte, C. R.; Thomason, L. W.; Bedka, K. M.; Wienhold, F.

    2014-12-01

    An increase of volcanic activity over the past decade is thought to have contributed significantly to the global warming "hiatus". Thus, it is important to improve our understanding of the microphysical and optical properties of even small volcanic plumes as well as their associated climate impacts. On February 13th, 2014, the Mt Kelud volcano, located near 4°S on the island of Java (Indonesia), injected volcanic gases and ash into the tropical stratosphere. An overpass of the CALIPSO lidar during the active phase of the eruption showed volcanic materials reaching 26 km with the main volcanic cloud near 18-19 km. This is the highest altitude volcanic injection since Mt Pinatubo in 1991. CALIPSO has tracked the dispersion of the Kelud plume throughout the tropical lower stratosphere (~20N-20S) since then. Depolarization lidar measurements (0.3-0.4) indicate that the plume was likely composed of irregularly shaped ash particles during the first few days after the eruption, and that sulfate aerosol (spherical droplets) formed thereafter, gradually lowering the mean depolarization to 0.1-0.2. In May, 2014, we mounted a 2-week campaign to Darwin (Australia) to measure several profiles of backscatter in red and blue channels, and one profile of aerosol size distribution using two optical particle counters, one with an inlet heated to 200°C. The purpose was to characterize particle sizes, optical properties, and sulfate fraction from a relatively fresh volcanic plume in the low stratosphere. Preliminary results from the campaign suggest the persistence of ash particles at the bottom of the Kelud plume 3 months after the eruption. This is significant because the climate impact of ash is neglected in most climate models.

  20. Comparison of TOMS and AVHRR imagery of volcanic clouds

    Science.gov (United States)

    Rose, William I.

    1994-01-01

    This project consisted of merging volcanic cloud data from initial studies from TOMS and AVHRR sensors. Because of the different data acquisition platforms and processing algorithms and formats, the combination of the two data required special consideration. Once the registration technique was perfected, several eruptions with data from both sensors were studied. The conclusion showed that, from the initial work, the positions of the volcanic clouds as detected by the two sensors are very similar. Because the AVHRR algorithm is now capable of retrieving masses of ash and sulfate aerosol, the capability of comparing data from the two sensors now allows changes in SO2, H2SO4, and silicated ash in drifting clouds to be described. The results of this study culminated in several presentations, and a master's thesis, which in turn was converted into a paper submitted to the Journal of Geophysical Research. Abstracts of two presentations are attached.

  1. Infrared remote sensing of atmospheric aerosols; Apports du sondage infrarouge a l'etude des aerosols atmospheriques

    Energy Technology Data Exchange (ETDEWEB)

    Pierangelo, C.

    2005-09-15

    The 2001 report from the Intergovernmental Panel on Climate Change emphasized the very low level of understanding of atmospheric aerosol effects on climate. These particles originate either from natural sources (dust, volcanic aerosols...) or from anthropogenic sources (sulfates, soot...). They are one of the main sources of uncertainty on climate change, partly because they show a very high spatio-temporal variability. Observation from space, being global and quasi-continuous, is therefore a first importance tool for aerosol studies. Remote sensing in the visible domain has been widely used to obtain a better characterization of these particles and their effect on solar radiation. On the opposite, remote sensing of aerosols in the infrared domain still remains marginal. Yet, not only the knowledge of the effect of aerosols on terrestrial radiation is needed for the evaluation of their total radiative forcing, but also infrared remote sensing provides a way to retrieve other aerosol characteristics (observations are possible at night and day, over land and sea). In this PhD dissertation, we show that aerosol optical depth, altitude and size can be retrieved from infrared sounder observations. We first study the sensitivity of aerosol optical properties to their micro-physical properties, we then develop a radiative transfer code for scattering medium adapted to the very high spectral resolution of the new generation sounder NASA-Aqua/AIRS, and we finally focus on the inverse problem. The applications shown here deal with Pinatubo stratospheric volcanic aerosol, observed with NOAA/HIRS, and with the building of an 8 year climatology of dust over sea and land from this sounder. Finally, from AIRS observations, we retrieve the optical depth at 10 {mu}m, the average altitude and the coarse mode effective radius of mineral dust over sea. (author)

  2. Olivine Weathering aud Sulfate Formation Under Cryogenic Conditions

    Science.gov (United States)

    Niles, Paul B.; Golden, D. C.; Michalski, J.

    2013-01-01

    sulfur-rich volcanism, and sulfur-rich surface deposits also makes it very likely that sulfate aerosols have also been an important component of the martian atmosphere. Thus mixtures of ice, dust, and sulfate aerosols are likely to have been common on the martian surface. Given the fact that it is not difficult to achieve surface temperatures above -40degC on Mars throughout its history, it seems likely that sulfate formation on Mars is controlled by the availability of sulfate aerosols and not by the martian climate. The current polar regions of Mars and Earth provide interesting analogs. Large regions of sulfaterich material have been detected on and around the modern north polar region of Mars. The prevalence of ice-dust mixtures in this region and the existence of sulfates within the ice cap itself are strong evidence for the origin of the sulfates from inside the ice deposits. In addition sulfates have been found in ice deposits in Greenland and Mount Fuji on Earth that have been attributed to forming within the ice deposit. These sulfates can form either through interaction with dust particles in the atmosphere or through weathering inside the ice itself.

  3. Evaluation of climate impacts after a large volcanic eruption during stratospheric sulfur injections

    Science.gov (United States)

    Laakso, Anton; Kokkola, Harri; Partanen, Antti-Ilari; Niemeier, Ulrike; Timmreck, Claudia; Lehtinen, Kari; Hakkarainen, Hanne; Korhonen, Hannele

    2016-04-01

    Solar radiation management (SRM) by injecting sulfur to the stratosphere is one of the most discussed geoengineering methods, because it has been suggested to be affordable and effective and its impacts have been thought to be predictable based on volcanic eruptions. Injecting sulfur to the stratosphere could be seen as an analogy of large volcanic eruptions, where large amounts of sulfur dioxide are released into the stratosphere. In the atmosphere sulfur dioxide oxidizes and forms aqueous sulfuric acid aerosols which reflect incoming solar radiation back to space. If SRM is ever used to cool the climate it is possible that a large volcanic eruption could happen also during the SRM, which would lead temporally to a very strong cooling. The simulations in this study were performed in two steps. In the first step, we used the aerosol-climate model MAECHAM5-HAM-SALSA to define global aerosol fields in scenarios with stratospheric sulfur injections and/or a volcanic eruption. In the second step of the study we performed climate simulations using Max-Planck-Institute's Earth system model (MPI-ESM) by using aerosol fields defined by MAECHAM5-HAM-SALSA. We studied scenarios of volcanic eruptions in two different locations and seasons and during the SRM sulfur injections and without injections. According to our simulations the radiative impacts of the eruption and SRM are not additive and the radiative effects and climate changes occurring after the eruption depend strongly on whether SRM is continued or suspended after the eruption. Adding to this, sulfate burden and radiative forcing after the volcanic eruption decrease significantly faster if the volcanic eruption happens during the geoengineering injections. In this situation, sulfur from the eruption does not only form new particles but it also condenses into pre-existing particles. Furthermore, the new small particles that are formed after the eruption coagulate effectively with the existing larger particles from

  4. How Volcanism Controls Climate Change

    Science.gov (United States)

    Ward, P. L.

    2013-12-01

    Large explosive volcanoes eject megatons of sulfur dioxide into the lower stratosphere where it spreads around the world within months and is oxidized slowly to form a sulfuric-acid aerosol with particle sizes that grow large enough to reflect and scatter solar radiation, cooling Earth ~0.5C for up to 3 years. Explosive eruptions also deplete total column ozone ~6% causing up to 3C winter warming at mid-latitudes over continents. Global cooling predominates. Extrusive, basaltic volcanoes deplete ozone ~6% but do not eject much sulfur dioxide into the lower stratosphere, causing net global warming. Anthropogenic chlorofluorocarbons (CFCs) deplete ozone ~3% for up to a century while each volcanic eruption, even small ones, depletes ozone twice as much but for less than a decade through eruption of halogens and ensuing photochemical processes. The 2010 eruption of Eyjafjallajökull, the 2011 eruption of Grímsvötn, plus anthropogenic CFCs depleted ozone over Toronto Canada 14% in 2012, causing an unusually warm winter and drought. Total column ozone determines how much solar ultraviolet energy with wavelengths between 290 and 340 nanometers reaches Earth where it is absorbed most efficiently by the ocean. A 25% depletion of ozone increases the amount of this radiation reaching Earth by 1 W m-2 for overhead sun and 0.25 W m-2 for a solar zenith angle of 70 degrees. The tropopause is the boundary between the troposphere heated from below by a sun-warmed Earth and the stratosphere heated from above by the Sun through photodissociation primarily of oxygen and ozone. The mean annual height of the tropopause increased ~160 m between 1980 and 2004 at the same time that northern mid-latitude total column ozone was depleted by ~4%, the lower stratosphere cooled ~2C, the upper troposphere warmed ~0.1C, and mean surface temperatures in the northern hemisphere rose ~0.5C. Regional total ozone columns are observed to increase as rapidly as 20% within 5 hours with an associated 5

  5. Volcanic forcing improves Atmosphere-Ocean Coupled General Circulation Model scaling performance

    CERN Document Server

    Vyushin, D; Havlin, S; Bunde, A; Brenner, S; Vyushin, Dmitry; Zhidkov, Igor; Havlin, Shlomo; Bunde, Armin; Brenner, Stephen

    2004-01-01

    Recent Atmosphere-Ocean Coupled General Circulation Model (AOGCM) simulations of the twentieth century climate, which account for anthropogenic and natural forcings, make it possible to study the origin of long-term temperature correlations found in the observed records. We study ensemble experiments performed with the NCAR PCM for 10 different historical scenarios, including no forcings, greenhouse gas, sulfate aerosol, ozone, solar, volcanic forcing and various combinations, such as it natural, anthropogenic and all forcings. We compare the scaling exponents characterizing the long-term correlations of the observed and simulated model data for 16 representative land stations and 16 sites in the Atlantic Ocean for these scenarios. We find that inclusion of volcanic forcing in the AOGCM considerably improves the PCM scaling behavior. The scenarios containing volcanic forcing are able to reproduce quite well the observed scaling exponents for the land with exponents around 0.65 independent of the station dista...

  6. Tellurium in active volcanic environments: Preliminary results

    Science.gov (United States)

    Milazzo, Silvia; Calabrese, Sergio; D'Alessandro, Walter; Brusca, Lorenzo; Bellomo, Sergio; Parello, Francesco

    2014-05-01

    Tellurium is a toxic metalloid and, according to the Goldschmidt classification, a chalcophile element. In the last years its commercial importance has considerably increased because of its wide use in solar cells, thermoelectric and electronic devices of the last generation. Despite such large use, scientific knowledge about volcanogenic tellurium is very poor. Few previous authors report result of tellurium concentrations in volcanic plume, among with other trace metals. They recognize this element as volatile, concluding that volcanic gases and sulfur deposits are usually enriched with tellurium. Here, we present some results on tellurium concentrations in volcanic emissions (plume, fumaroles, ash leachates) and in environmental matrices (soils and plants) affected by volcanic emissions and/or deposition. Samples were collected at Etna and Vulcano (Italy), Turrialba (Costa Rica), Miyakejima, Aso, Asama (Japan), Mutnovsky (Kamchatka) at the crater rims by using common filtration techniques for aerosols (polytetrafluoroethylene filters). Filters were both eluted with Millipore water and acid microwave digested, and analyzed by inductively coupled plasma mass spectrometry (ICP-MS). Volcanic ashes emitted during explosive events on Etna and Copahue (Argentina) were analyzed for tellurium bulk composition and after leaching experiments to evaluate the soluble fraction of tellurium. Soils and leaves of vegetation were also sampled close to active volcanic vents (Etna, Vulcano, Nisyros, Nyiragongo, Turrialba, Gorely and Masaya) and investigated for tellurium contents. Preliminary results showed very high enrichments of tellurium in volcanic emissions comparing with other volatile elements like mercury, arsenic, thallium and bismuth. This suggests a primary transport in the volatile phase, probably in gaseous form (as also suggested by recent studies) and/or as soluble salts (halides and/or sulfates) adsorbed on the surface of particulate particles and ashes. First

  7. Characterization of a volcanic ash episode in southern Finland caused by the Grimsvötn eruption in Iceland in May 2011

    Directory of Open Access Journals (Sweden)

    V.-M. Kerminen

    2011-09-01

    Full Text Available The volcanic eruption of Grimsvötn in Iceland in May 2011, affected surface-layer air quality at several locations in Northern Europe. In Helsinki, Finland, the main pollution episode lasted for more than 8 h around the noon of 25 May. We characterized this episode by relying on detailed physical, chemical and optical aerosol measurements. The analysis was aided by air mass trajectory calculations, satellite measurements, and dispersion model simulations. During the episode, volcanic ash particles were present at sizes from less than 0.5 μm up to sizes >10 μm. The mass mean diameter of ash particles was a few μm in the Helsinki area, and the ash enhanced PM10 mass concentrations up to several tens of μg m−3. Individual particle analysis showed that some ash particles appeared almost non-reacted during the atmospheric transportation, while most of them were mixed with sea salt or other type of particulate matter. Also sulfate of volcanic origin appeared to have been transported to our measurement site, but its contribution to the aerosol mass was minor due the separation of ash-particle and sulfur dioxide plumes shortly after the eruption. The volcanic material had very little effect on PM1 mass concentrations or sub-micron particle number size distributions in the Helsinki area. The aerosol scattering coefficient was increased and visibility was slightly decreased during the episode, but in general changes in aerosol optical properties due to volcanic aerosols seem to be difficult to be distinguished from those induced by other pollutants present in a continental boundary layer. The case investigated here demonstrates clearly the power of combining surface aerosol measurements, dispersion model simulations and satellite measurements in analyzing surface air pollution episodes caused by volcanic eruptions. None of these three approaches alone would be sufficient to forecast, or even to unambiguously

  8. Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

    Science.gov (United States)

    Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

    2004-01-01

    During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic

  9. Physical and Radiative Properties of Aerosol Particles across the Caribbean Basin: A Comparison between Clean and Perturbed African Dust and Volcanic Ash Air Masses

    Science.gov (United States)

    Rivera, H.; Ogren, J. A.; Sheridan, P. J.; Mayol-Bracero, O.

    2009-12-01

    Aerosol’s optical and physical properties were measured during year 2007 at Cape San Juan, a ground-based station located at the northeastern tip of Puerto Rico. The three cases investigated were classified according to the origin of the air masses: clean (C), African dust (AD), and volcanic ash (VA). The instrumentation used included a sunphotometer to determine volume size distributions and aerosol optical thickness (AOT), a 3-wavelength nephelometer to determine the scattering coefficient (σsp), and a 3-wavelength particle/soot absorption photometer (PSAP) to measure the absorption coefficient (σap). The average volume size distributions were trimodal for the C (peaks at 0.14, 0.99 and 4.25 µm radius) and AD (peaks at 0.11, 1.30 and 2.00 µm radius) cases and bimodal for the VA (peaks at 0.19 and 2.75 µm radius) case. Fine and coarse modes maxima for AD occurred at radii smaller than for VA, confirming the different origins of those particles. The average values for the total σsp were higher for AD (82.9 Mm-1) and VA (33.7 Mm-1) compared to C (16.6 Mm-1). The same happened for the AOT maximum values at 500 nm with 0.92, 0.30, and 0.06 for AD, VA, and C, respectively. The observed increase in the values of the Angstrom exponent (å) is indicative of a decrease in the size of the particles associated to VA (å= 0.27) and AD (å =0.89) when compared to C (å =0.24). The volume size distributions and thus the mass were dominated by the coarse mode (> 1.0 µm) especially for the AD case. Results have shown that AD as well as VA has a significant impact on the physical and radiative properties across Puerto Rico and the Caribbean. Additional results on the AOT wavelength dependence and on the annual variability of the properties under study will be presented.

  10. Fractionation of sulfur isotopes during heterogeneous oxidation of SO2 on sea salt aerosol: a new tool to investigate non-sea salt sulfate production in the marine boundary layer

    Directory of Open Access Journals (Sweden)

    S. Borrmann

    2012-05-01

    Full Text Available The oxidation of SO2 to sulfate on sea salt aerosols in the marine environment is highly important because of its effect on the size distribution of sulfate and the potential for new particle nucleation from H2SO4 (g. However, models of the sulfur cycle are not currently able to account for the complex relationship between particle size, alkalinity, oxidation pathway and rate – which is critical as SO2 oxidation by O3 and Cl catalysis are limited by aerosol alkalinity, whereas oxidation by hypohalous acids and transition metal ions can continue at low pH once alkalinity is titrated. We have measured 34S/32S fractionation factors for SO2 oxidation in sea salt, pure water and NaOCl aerosol, as well as the pH dependency of fractionation. Oxidation of SO2 by NaOCl aerosol was extremely efficient, with a reactive uptake coefficient of ≈0.5, and produced sulfate that was enriched in 32S with αOCl = 0.9882±0.0036 at 19 °C. Oxidation on sea salt aerosol was much less efficient than on NaOCl aerosol, suggesting alkalinity was already exhausted on the short timescale of the experiments. Measurements at pH = 2.1 and 7.2 were used to calculate fractionation factors for each step from SO2(g → multiple steps → SOOCl2−. Oxidation on sea salt aerosol resulted in a lower fractionation factor than expected for oxidation of SO32− by O3 (αseasalt = 1.0124±0.0017 at 19 °C. Comparison of the lower fractionation during oxidation on sea salt aerosol to the fractionation factor for high pH oxidation shows HOCl contributed 29% of S(IV oxidation on sea salt in the short experimental timescale, highlighting the potential importance of hypohalous acids in the marine environment. The sulfur isotope fractionation factors measured in this study allow differentiation between the alkalinity-limited pathways – oxidation by O3 and by Cl catalysis (α34 = 1.0163±0.0018 at 19 °C in pure water or 1.0199±0.0024 at pH = 7.2 – which favour the heavy isotope, and

  11. Development of a new corona discharge based ion source for high resolution time-of-flight chemical ionization mass spectrometer to measure gaseous H2SO4 and aerosol sulfate

    Science.gov (United States)

    Zheng, Jun; Yang, Dongsen; Ma, Yan; Chen, Mindong; Cheng, Jin; Li, Shizheng; Wang, Ming

    2015-10-01

    A new corona discharge (CD) based ion source was developed for a commercial high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS) (Aerodyne Research Inc.) to measure both gaseous sulfuric acid (H2SO4) and aerosol sulfate after thermal desorption. Nitrate core ions (NO3-) were used as reagent ions and were generated by a negative discharge in zero air followed by addition of excess nitrogen dioxide (NO2) to convert primary ions and hydroxyl radicals (OH) into NO3- ions and nitric acid (HNO3). The CD-HRToF-CIMS showed no detectable interference from hundreds parts per billion by volume (ppbv) of sulfur dioxide (SO2). Unlike the atmospheric pressure ionization (API) ToF-CIMS, the CD ion source was integrated onto the ion-molecule reaction (IMR) chamber and which made it possible to measure aerosol sulfate by coupling to a filter inlet for gases and aerosols (FIGAERO). Moreover, compared with a quadrupole-based mass spectrometer, the desired HSO4- signal was detected by its exact mass of m/z 96.960, which was well resolved from the potential interferences of HCO3-ṡ(H2O)2 (m/z 97.014) and O-ṡH2OṡHNO3 (m/z 97.002). In this work, using laboratory-generated standards the CD-HRToF-CIMS was demonstrated to be able to detect as low as 3.1 × 105 molecules cm-3 gaseous H2SO4 and 0.5 μg m-3 ammonium sulfate based on 10-s integration time and two times of the baseline noise. The CD ion source had the advantages of low cost and a simple but robust structure. Since the system was non-radioactive and did not require corrosive HNO3 gas, it can be readily field deployed. The CD-HRToF-CIMS can be a powerful tool for both field and laboratory studies of aerosol formation mechanism and the chemical processes that were critical to understand the evolution of aerosols in the atmosphere.

  12. New AgMIP Scenarios: Impacts of Volcanic Eruptions, Geoengineering, or Nuclear War on Agriculture

    Science.gov (United States)

    Robock, A.; Xia, L.

    2016-12-01

    Climate is one of the most important factors determining crop yields and world food supplies. To be well prepared for possible futures, it is necessary to study yield changes of major crops in response to different climate forcings. Previous studies mainly focus on the impact from global warming. Here we propose that the AgMIP community also study the impacts of stratospheric aerosols on agriculture. While nature can load the stratosphere with sulfate aerosols for several years from large volcanic eruptions, humans could also put sulfate aerosols into the stratosphere on purpose through geoengineering or soot as a result of the fires from a nuclear war. Stratospheric aerosols would change the temperature, precipitation, total insolation, and fraction of diffuse radiation due to their radiative impacts, and could produce more ultraviolet radiation by ozone destruction. Surface ozone concentration could also change by changed transport from the stratosphere as well as changed tropospheric chemistry. As a demonstration of these effects, using the crop model in the NCAR Community Land Model (CLM-crop), we have studied sulfate injection geoengineering and nuclear war impacts on global agriculture in response to temperature, precipitation and radiation changes, and found significant changes in patterns of global food production. With the new ozone module in CLM-crop, we simulated how surface ozone concentration change under sulfate injection geoengineering would change the agriculture response. Agriculture would benefit from less surface ozone concentration associated with the specific geoengineering scenario comparing with the global warming scenario. Here, we would like to encourage more crop modelers to improve crop models in terms of crop responses to ozone, ultraviolet radiation, and diffuse radiation. We also invite more global crop modeling groups to use the climate forcing we would be happy to provide to gain a better understanding of global agriculture responses

  13. Sensitivity of high-spectral resolution and broadband thermal infrared nadir instruments to the chemical and microphysical properties of secondary sulfate aerosols in the upper-troposphere/lower-stratosphere

    Science.gov (United States)

    Sellitto, Pasquale; Legras, Bernard

    2016-04-01

    The observation of upper-tropospheric/lower-stratospheric (UTLS) secondary sulfate aerosols (SSA) and their chemical and microphysical properties from satellite nadir observations (with better spatial resolution than limb observations) is a fundamental tool to better understand their formation and evolution processes and then to estimate their impact on UTLS chemistry, and on regional and global radiative balance. Thermal infrared (TIR) observations are sensitive to the chemical composition of the aerosols due to the strong spectral variations of the imaginary part of the refractive index in this band and, correspondingly, of the absorption, as a function of the composition Then, these observations are, in principle, well adapted to detect and characterize UTLS SSA. Unfortunately, the exploitation of nadir TIR observations for sulfate aerosol layer monitoring is today very limited. Here we present a study aimed at the evaluation of the sensitivity of TIR satellite nadir observations to the chemical composition and the size distribution of idealised UTLS SSA layers. The sulfate aerosol particles are assumed as binary systems of sulfuric acid/water solution droplets, with varying sulphuric acid mixing ratios. The extinction properties of the SSA, for different sulfuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indices taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. High-spectral resolution pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealised aerosol layers, at typical UTLS conditions, on

  14. Sulfur K-edge XANES study of S sorbed onto volcanic ashes

    Energy Technology Data Exchange (ETDEWEB)

    Farges, F; Keppler, H [Bayerische Geoinsitut, Universitaet Bayreuth, Bayreuth (Germany); Flank, A-M; Lagarde, P, E-mail: farges@mnhn.f [CNRS UR1 Synchrotron Soleil, BP 48, 91192 Gif sur Yvette (France)

    2009-11-15

    Powders of four synthetic glasses of volcanic composition, a silica glass and crystalline quartz were equilibrated with SO{sub 2} to study the speciation of S sorbed onto their surface. These samples mimic the aerosols injected into the atmosphere during volcanic eruptions. Volcanic sulfur is known to globally affect the Earth's climate with an opposite effect to CO{sub 2}. However, absorption on ashes may reduce the amount of sulfur entering the stratosphere. S K-edge micro-XANES ({mu}XANES) spectra and {mu}XRF maps were collected at the LUCIA beamline (SOLEIL) at the SLS (Switzerland). When photoreduction is minimized, SO{sub 2} is sorbed mostly as sulfates moieties. The sorption of S is controlled by the surface structure of the powders probed. Presence of defects, non-bridging oxygens and network-modifiers (alkali and alkali-earths) enhance S-sorption as sulfate moieties onto the powders surface. Therefore, the quantity of S released to the atmosphere is highly dependant on the type of ash produced during eruptions that help to better model the climatic impact of volcanic S.

  15. Effect of nitrate and sulfate relative abundance in PM2.5 on liquid water content explored through half-hourly observations of inorganic soluble aerosols at a polluted receptor site

    Science.gov (United States)

    Xue, Jian; Griffith, Stephen M.; Yu, Xin; Lau, Alexis K. H.; Yu, Jian Zhen

    2014-12-01

    Liquid water content (LWC) is the amount of liquid water on aerosols. It contributes to visibility degradation, provides a surface for gas condensation, and acts as a medium for heterogeneous gas/particle reactions. In this study, 520 half-hourly measurements of ionic chemical composition in PM2.5 at a receptor site in Hong Kong are used to investigate the dependence of LWC on ionic chemical composition, particularly on the relative abundance of sulfate and nitrate. LWC was estimated using a thermodynamic model (AIM-III). Within this data set of PM2.5 ionic compositions, LWC was highly correlated with the multivariate combination of sulfate and nitrate concentrations and RH (R2 = 0.90). The empirical linear regression result indicates that LWC is more sensitive to nitrate mass than sulfate. During a nitrate episode, the highest LWC (80.6 ± 17.9 μg m-3) was observed and the level was 70% higher than that during a sulfate episode despite a similar ionic PM2.5 mass concentration. A series of sensitivity tests were conducted to study LWC change as a function of the relative nitrate and sulfate abundance, the trend of which is expected to shift to more nitrate in China as a result of SO2 reduction and increase in NOx emission. Starting from a base case that uses the average of measured PM2.5 ionic chemical composition (63% SO42-, 11% NO3-, 19% NH4+, and 7% other ions) and an ionic equivalence ratio, [NH4+]/(2[SO42-] + [NO3-]), set constant to 0.72, the results show LWC would increase by 204% at RH = 40% when 50% of the SO42- is replaced by NO3- mass concentration. This is largely due to inhibition of (NH4)3H(SO4)2 crystallization while PM2.5 ionic species persist in the aqueous phase. At RH = 90%, LWC would increase by 12% when 50% of the SO42- is replaced by NO3- mass concentration. The results of this study highlight the important implications to aerosol chemistry and visibility degradation associated with LWC as a result of a shift in PM2.5 ionic chemical

  16. Acidic aerosol in urban air

    Energy Technology Data Exchange (ETDEWEB)

    Fukuda, M.; Yamaoka, S.; Miyazaki, T.; Oka, M.

    1982-01-01

    The distribution and chemical composition of acidic aerosol in Osaka City were investigated. Samples were collected at five sites in the city from June to September, 1979. Acidic aerosol was determined by the acid-base titration method, sulfate ion by barium chloride turbidimetry, nitrate ion by the xylenol method, and chloride ion by the mercury thiocyanate method. The concentration of acidic aerosol at five sites ranged from 7.7 micrograms per cubic meter to 10.0 micrograms per cubic meter, but mean concentrations in the residential area were slightly higher than those in the industrial area. When acidic aerosol concentrations were compared with concentrations of sulfate, nitrate, and chloride ions, a significant correlation was found between acidic aerosol and sulfate ion. The sum of the ion equivalents of the three types showed good correlation with the acidic aerosol equivalent during the whole period.

  17. Assessing estimates of radiative forcing for solar geoengineering starts with accurate aerosol radiative properties

    Science.gov (United States)

    Dykema, J. A.; Keith, D.; Keutsch, F. N.

    2016-12-01

    The deliberate modification of Earth's albedo as a complement to mitigation in order to slow climate change brings with it a range of risks. A range of different approaches have been studied, including the injection of aerosol particles into the stratosphere to decrease solar energy input into the climate system. Key side effects from this approach include ozone loss and radiative heating. Both of these side effects may produce dynamical changes with further consequences for stratospheric and tropospheric climate. Studies of past volcanic eruptions suggest that sulfate aerosol injection may be capable of achieving a compensating radiative forcing of -1 W m-2 or more. It is also expected that such injection of sulfate aerosols will result in loss of stratospheric ozone and of significant infrared heating. The problems resulting from sulfate aerosols intended have motivated the investigation of alternative materials, including high refractive index solid materials. High refractive index materials have the potential to scatter more efficiently per unit mass, leading to a reduction in surface area for heterogeneous chemistry, and, depending on details of absorption, less radiative heating. Fundamentally, assessing these trade-offs requires accurate knowledge of the complex refractive index of materials being considered over the full range of wavelengths relevant to atmospheric radiative transfer, that is, from ultraviolet to far-infrared. Our survey of the relevant literature finds that such measurements are not available for all materials of interest at all wavelengths. We utilize a method developed in astrophysics to fill in spectral gaps, and find that some materials may heat the stratosphere substantially more than was found in previous work. Stratospheric heating can warm the tropical tropopause layer, increasing the flux of water vapor into the stratosphere, with further consequences for atmospheric composition and radiative forcing. We analyze this consequence

  18. Hemispherically asymmetric volcanic forcing of tropical hydroclimate during the last millennium

    Science.gov (United States)

    Colose, Christopher M.; LeGrande, Allegra N.; Vuille, Mathias

    2016-08-01

    Volcanic aerosols exert the most important natural radiative forcing of the last millennium. State-of-the-art paleoclimate simulations of this interval are typically forced with diverse spatial patterns of volcanic forcing, leading to different responses in tropical hydroclimate. Recently, theoretical considerations relating the intertropical convergence zone (ITCZ) position to the demands of global energy balance have emerged in the literature, allowing for a connection to be made between the paleoclimate simulations and recent developments in the understanding of ITCZ dynamics. These energetic considerations aid in explaining the well-known historical, paleoclimatic, and modeling evidence that the ITCZ migrates away from the hemisphere that is energetically deficient in response to asymmetric forcing.Here we use two separate general circulation model (GCM) suites of experiments for the last millennium to relate the ITCZ position to asymmetries in prescribed volcanic sulfate aerosols in the stratosphere and related asymmetric radiative forcing. We discuss the ITCZ shift in the context of atmospheric energetics and discuss the ramifications of transient ITCZ migrations for other sensitive indicators of changes in the tropical hydrologic cycle, including global streamflow. For the first time, we also offer insight into the large-scale fingerprint of water isotopologues in precipitation (δ18Op) in response to asymmetries in radiative forcing. The ITCZ shifts away from the hemisphere with greater volcanic forcing. Since the isotopic composition of precipitation in the ITCZ is relatively depleted compared to areas outside this zone, this meridional precipitation migration results in a large-scale enrichment (depletion) in the isotopic composition of tropical precipitation in regions the ITCZ moves away from (toward). Our results highlight the need for careful consideration of the spatial structure of volcanic forcing for interpreting volcanic signals in proxy records

  19. Using CATS Near-Real-time Lidar Observations to Monitor and Constrain Volcanic Sulfur Dioxide (SO2) Forecasts

    Science.gov (United States)

    Hughes, E. J.; Yorks, J.; Krotkov, N. A.; da Silva, A. M.; Mcgill, M.

    2016-01-01

    An eruption of Italian volcano Mount Etna on 3 December 2015 produced fast-moving sulfur dioxide (SO2) and sulfate aerosol clouds that traveled across Asia and the Pacific Ocean, reaching North America in just 5 days. The Ozone Profiler and Mapping Suite's Nadir Mapping UV spectrometer aboard the U.S. National Polar-orbiting Partnership satellite observed the horizontal transport of the SO2 cloud. Vertical profiles of the colocated volcanic sulfate aerosols were observed between 11.5 and 13.5 km by the new Cloud Aerosol Transport System (CATS) space-based lidar aboard the International Space Station. Backward trajectory analysis estimates the SO2 cloud altitude at 7-12 km. Eulerian model simulations of the SO2 cloud constrained by CATS measurements produced more accurate dispersion patterns compared to those initialized with the back trajectory height estimate. The near-real-time data processing capabilities of CATS are unique, and this work demonstrates the use of these observations to monitor and model volcanic clouds.

  20. A decade of global volcanic SO2 emissions measured from space

    Science.gov (United States)

    Carn, S. A.; Fioletov, V. E.; McLinden, C. A.; Li, C.; Krotkov, N. A.

    2017-03-01

    The global flux of sulfur dioxide (SO2) emitted by passive volcanic degassing is a key parameter that constrains the fluxes of other volcanic gases (including carbon dioxide, CO2) and toxic trace metals (e.g., mercury). It is also a required input for atmospheric chemistry and climate models, since it impacts the tropospheric burden of sulfate aerosol, a major climate-forcing species. Despite its significance, an inventory of passive volcanic degassing is very difficult to produce, due largely to the patchy spatial and temporal coverage of ground-based SO2 measurements. We report here the first volcanic SO2 emissions inventory derived from global, coincident satellite measurements, made by the Ozone Monitoring Instrument (OMI) on NASA’s Aura satellite in 2005-2015. The OMI measurements permit estimation of SO2 emissions from over 90 volcanoes, including new constraints on fluxes from Indonesia, Papua New Guinea, the Aleutian Islands, the Kuril Islands and Kamchatka. On average over the past decade, the volcanic SO2 sources consistently detected from space have discharged a total of ~63 kt/day SO2 during passive degassing, or ~23 ± 2 Tg/yr. We find that ~30% of the sources show significant decadal trends in SO2 emissions, with positive trends observed at multiple volcanoes in some regions including Vanuatu, southern Japan, Peru and Chile.

  1. Observations of volcanic SO2 from MLS on Aura

    Directory of Open Access Journals (Sweden)

    H. C. Pumphrey

    2015-01-01

    Full Text Available Sulfur dioxide (SO2 is an important atmospheric constituent, particularly in the aftermath of volcanic eruptions. These events can inject large amounts of SO2 into the lower stratosphere, where it is oxidised to form sulfate aerosols; these in turn have a significant effect on the climate. The MLS instrument on the Aura satellite has observed the SO2 mixing ratio in the upper troposphere and lower stratosphere from August 2004 to the present, during which time a number of volcanic eruptions have significantly affected those regions of the atmosphere. We describe the MLS SO2 data and how various volcanic events appear in the data. As the MLS SO2 data are currently not validated we take some initial steps towards their validation. First we establish the level of internal consistency between the three spectral regions in which MLS is sensitive to SO2. We compare SO2 column values calculated from MLS data to total column values reported by the OMI instrument. The agreement is good (within about 1 DU in cases where the SO2 is clearly at altitudes above 147 hPa.

  2. Season - dependent and source-influenced aerosol in Northern Siberia

    Science.gov (United States)

    Popovicheva, Olga; Makshtas, Alexander; Bogorodsky, Peter; Eleftheriadis, Kostantinos; Diapouli, Evangelia; Shonia, Natalia; Uttal, Taneil

    2016-04-01

    Aerosol may serve as a tracer of arctic pollution, allowing a link to climate response if its major characteristics relating to natural and anthropogeneous sources are defined. It has been shown that BC and sulfates are the most important aerosol constituents measured in the Arctic boundary layer; these species demonstrate similar seasonal variations with a peak during winter to early spring and a minimum in summer. Long - time gap in consistent aerosol observations in the Russian Arctic strongly limits the assessment of air pollution and climate impacts. On-line monitoring, sampling, and analyses of atmospheric aerosols were carried out at the Tiksi Hydrometeorological Observatory, Northern Siberia, during one year from September 2014 to 2015. Physico-chemical characterization combining aethalometry, thermo-optical analysis, and analytical chemistry was used in order to identify the seasonal variability of aerosols and to link their composition to possible sources, as well as to characterize the differences in aerosol chemical composition between natural background conditions and BC-pollution episodes. The present study reports the first results from the Tiksi Observatory on season-dependent and source-influenced characteristics of aerosol species, such as carbon fractions (OC, EC), inorganic and organic functionalities of chemical compounds, sulfates, nitrates and other ion components, and elements. In addition, data obtained by individual particles analysis provide insight into micromarkers of combustion sources. Aerosol at the Tiksi Observatory is found to be originated from natural marine, biogenic, and continental sources as well as influenced by local residential activity and regional pollution. Characterization of aerosols during OC and BC-pollution episodes, combined with analysis of the wind direction, atmosphere stability, and air mass trajectories, allows for the identification of the sources which are responsible for the emission of hazardous compounds

  3. MSA in Beijing aerosol

    Institute of Scientific and Technical Information of China (English)

    YUAN Hui; WANG Ying; ZHUANG Guoshun

    2004-01-01

    Methane sulphonate (MSA) and sulfate (SO42-), the main oxidation products of dimethyl sulfide (DMS), are the target of atmospheric chemistry study, as sulfate aerosol would have important impact on the global climate change. It is widely believed that DMS is mainly emitted from phytoplankton production in marine boundary layer (MBL), and MSA is usually used as the tracer of non-sea-salt sulfate (nss- SO42-) in marine and coastal areas (MSA/SO42- = 1/18). Many observations of MSA were in marine and coastal aerosols. To our surprise, MSA was frequently (>60%) detected in Beijing TSP, PM10, and PM2.5 aerosols, even in the samples collected during the dust storm period. The concentrations of MSA were higher than those measured in marine aerosols. Factor analysis, correlation analysis and meteorology analysis indicated that there was no obvious marine influence on Beijing aerosols. DMS from terrestrial emissions and dimethyl sulphoxide (DMSO) from industrial wastes could be the two possible precursors of MSA. Warm and low-pressure air masses and long time radiation were beneficial to the formation of MSA. Anthropogenic pollution from regional and local sources might be the dominant contributor to MSA in Beijing aerosol. This was the first report of MSA in aerosols collected in an inland site in China. This new finding would lead to the further study on the balance of sulfur in inland cities and its global biogeochemical cycle.

  4. Impacts of volcanic eruptions and geoengineering on Arctic climate

    Science.gov (United States)

    Berdahl, Mira

    Stratospheric aerosols can produce large radiative forcing and climate response, often amplified in the Arctic. Here I study the Arctic response to natural (volcanic eruptions) and potential anthropogenic (geoengineering) stratospheric sulfate aerosols. I use a regional climate model and global climate model output from two modeling intercomparison projects. First, I investigate the relative impacts of changes in radiation and advection on snow extent over Baffin Island with the Weather Research and Forecasting model. Model results show it is possible to suddenly lower the snowline by amounts comparable to those seen during the Little Ice Age with an average temperature decrease of --3.9 +/- 1.1 K from present. Further, sea ice expansion following large volcanic eruptions would have significant affects on inland temperatures, especially in the fall. Next, I analyze Last Millennium simulations from the Paleoclimate Modeling Intercomparison Project 3 to assess whether state-of-the-art global climate models produce sudden changes and persistence of cold conditions after large volcanic eruptions as inferred by geological records and previous climate modeling. North Atlantic sea ice and Baffin Island snow cover showed large-scale expansion in the simulations, but none of the models produced significant centennial-scale effects. Warm Baffin Island summer climates stunt snow expansion in some models completely, and model topography misses the critical elevations that could sustain snow on the island. This has critical consequences for ice and snow formation and persistence in regions such as the Arctic where temperatures are near freezing and small temperature changes affect the state of water. Finally, I analyze output from the Geoengineering Modeling Intercomparison Project to examine whether geoengineering by injection of sulfate aerosols into the lower stratosphere prevents the demise of minimum annual sea ice extent, or slows spring snow cover loss. Despite

  5. Aerosol nucleation over oceans and the role of galactic cosmic rays

    Directory of Open Access Journals (Sweden)

    J. Kazil

    2006-06-01

    Full Text Available We investigate formation of sulfate aerosol in the marine troposphere from neutral and charged nucleation of H2SO4 and H2O. A box model of neutral and charged aerosol processes is run on a grid covering the oceans. Input data are taken from a model of galactic cosmic rays in the atmosphere, and from global chemistry and transport models. We find a weak aerosol production over the tropical oceans in the lower and middle troposphere, and a stronger production at higher latitudes, most notably downwind of industrial regions. The highest aerosol production, however, occurs in the upper troposphere, in particular in the tropics. This finding supports the proposition by which non-sea salt marine boundary layer aerosol in tropical regions does not form in situ, but nucleates in the upper troposphere from convectively lifted and cloud processed boundary layer air rich in aerosol precursor gases, from where it descends in subsiding air masses compensating convection. Convection of boundary layer air also appears to drive the formation of condensation nuclei in the tropical upper troposphere which maintains the stratospheric aerosol layer in the absence of volcanic activity. Neutral nucleation contributes only marginally to aerosol production in our simulations. This highlights the importance of charged binary and of ternary nucleation involving ammonia for aerosol formation. In clean marine regions however, ammonia concentrations seem too low to support ternary nucleation, making binary nucleation from ions a likely pathway for sulfate aerosol formation. On the other hand, our analysis indicates that the variation of ionization by galactic cosmic rays over the decadal solar cycle does not entail a response in aerosol production and cloud cover via the second indirect aerosol effect that would explain observed variations in global cloud cover. We estimate that the variation in radiative forcing resulting from a response of

  6. Impact of geoengineered aerosols on the troposphere and stratosphere

    Energy Technology Data Exchange (ETDEWEB)

    Tilmes, S.; Garcia, Rolando R.; Kinnison, Douglas E.; Gettelman, A.; Rasch, Philip J.

    2009-06-27

    A coupled chemistry climate model, the Whole Atmosphere Community Climate Model was used to perform a transient climate simulation to quantify the impact of geoengineered aerosols on atmospheric processes. In contrast to previous model studies, the impact on stratospheric chemistry, including heterogeneous chemistry in the polar regions, is considered in this simulation. In the geoengineering simulation, a constant stratospheric distribution of volcanic-sized, liquid sulfate aerosols is imposed in the period 2020–2050, corresponding to an injection of 2 Tg S/a. The aerosol cools the troposphere compared to a baseline simulation. Assuming an Intergovernmental Panel on Climate Change A1B emission scenario, global warming is delayed by about 40 years in the troposphere with respect to the baseline scenario. Large local changes of precipitation and temperatures may occur as a result of geoengineering. Comparison with simulations carried out with the Community Atmosphere Model indicates the importance of stratospheric processes for estimating the impact of stratospheric aerosols on the Earth’s climate. Changes in stratospheric dynamics and chemistry, especially faster heterogeneous reactions, reduce the recovery of the ozone layer in middle and high latitudes for the Southern Hemisphere. In the geoengineering case, the recovery of the Antarctic ozone hole is delayed by about 30 years on the basis of this model simulation. For the Northern Hemisphere, a onefold to twofold increase of the chemical ozone depletion occurs owing to a simulated stronger polar vortex and colder temperatures compared to the baseline simulation, in agreement with observational estimates.

  7. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  8. Climatic impact of volcanic eruptions

    Science.gov (United States)

    Rampino, Michael R.

    1991-01-01

    Studies have attempted to 'isolate' the volcanic signal in noisy temperature data. This assumes that it is possible to isolate a distinct volcanic signal in a record that may have a combination of forcings (ENSO, solar variability, random fluctuations, volcanism) that all interact. The key to discovering the greatest effects of volcanoes on short-term climate may be to concentrate on temperatures in regions where the effects of aerosol clouds may be amplified by perturbed atmospheric circulation patterns. This is especially true in subpolar and midlatitude areas affected by changes in the position of the polar front. Such climatic perturbation can be detected in proxy evidence such as decrease in tree-ring widths and frost rings, changes in the treeline, weather anomalies, severity of sea-ice in polar and subpolar regions, and poor grain yields and crop failures. In low latitudes, sudden temperature drops were correlated with the passage overhead of the volcanic dust cloud (Stothers, 1984). For some eruptions, such as Tambora, 1815, these kinds of proxy and anectdotal information were summarized in great detail in a number of papers and books (e.g., Post, 1978; Stothers, 1984; Stommel and Stommel, 1986; C. R. Harrington, in press). These studies lead to the general conclusion that regional effects on climate, sometimes quite severe, may be the major impact of large historical volcanic aerosol clouds.

  9. Effects of volcanic eruptions on China's monsoon precipitation over the past 700 years

    Science.gov (United States)

    Zhuo, Z.; Gao, C.

    2013-12-01

    Tropical volcanic eruptions were found to affect precipitation especially in Asia and Africa monsoon region. However, studies with different types of eruptions suggested different impacts as well as the spatial patterns. In this study, we combined the Monsoon Asia Drought Atlas (MADA, [Cook et al., 2010]) and the Chinese Historical Drought Disaster Index (CHDDI) compiled from the historic meteorological records to study the effect of volcanic eruptions on China's monsoon precipitation over the past 700 years. Histories of past volcanism were compiled from the IVI2[Gao et al., 2008] and Crowley2013[Crowley and Unterman, 2013] reconstructions. Volcanic events were classified into 2×Pinatubo, 1×Pinatubo , ≥5 Tg sulfate aerosols injection in the northern hemisphere (NH) stratosphere for IVI2; and NH sulfate flux more than 20/15/10/5 kg km-2 for Crowley2013. In both cases, average MADA show a drying trend over mainland China from year zero(0) to year three(+3) after the eruption; and the more sulfate aerosol injected into the NH stratosphere or the larger the sulfate flux, the more severe this drying trend seem to reveal. In comparison, a wetting trend was found in the eruption year with Southern Hemisphere (SH) only injections. Superposed epoch analysis with a 10,000 Monte Carlo resampling procedure showed that 97.9% (96.9%) of the observed MADA values are statistically significant at the 95% (99%) confidence level. The drying is probably caused by a reduction of the latent heat flux due to volcanic aerosol' cooling effect, leading to the weakening of south Asian monsoon and decrease of moisture vapor over tropical oceans, which contribute to a reduced moisture flux over china. Spatial distribution of the average MADA show a southward movement of the driest areas in eastern China from year zero to year three after the 1×Pinatubo and 2×Pinatubo eruptions, whereas part of north china experienced unusual wetting condition. This is in good agreement with CHDDI, which

  10. Radiative and climate impacts of a large volcanic eruption during stratospheric sulfur geoengineering

    Directory of Open Access Journals (Sweden)

    A. Laakso

    2015-08-01

    Full Text Available Both explosive volcanic eruptions, which emit sulfur dioxide into the stratosphere, and stratospheric geoengineering via sulfur injections can potentially cool the climate by increasing the amount of scattering particles in the atmosphere. Here we employ a global aerosol-climate model and an earth system model to study the radiative and climate impacts of an erupting volcano during solar radiation management (SRM. According to our simulations, the radiative impacts of an eruption and SRM are not additive: in the simulated case of concurrent eruption and SRM, the peak increase in global forcing is about 40 % lower compared to a corresponding eruption into a clean background atmosphere. In addition, the recovery of the stratospheric sulfate burden and forcing was significantly faster in the concurrent case since the sulfate particles grew larger and thus sedimented faster from the stratosphere. In our simulation where we assumed that SRM would be stopped immediately after a volcano eruption, stopping SRM decreased the overall stratospheric aerosol load. For the same reasons, a volcanic eruption during SRM lead to only about 1/3 of the peak global ensemble-mean cooling compared to an eruption under unperturbed atmospheric conditions. Furthermore, the global cooling signal was seen only for 12 months after the eruption in the former scenario compared to over 40 months in the latter. In terms of the global precipitation rate, we obtain a 36 % smaller decrease in the first year after the eruption and again a clearly faster recovery in the concurrent eruption and SRM scenario. We also found that an explosive eruption could lead to significantly different regional climate responses depending on whether it takes place during geoengineering or into an unperturbed background atmosphere. Our results imply that observations from previous large eruptions, such as Mt Pinatubo in 1991, are not directly applicable when estimating the potential consequences of a

  11. Temporal variations of flux and altitude of sulfur dioxide emissions during volcanic eruptions: implications for long-range dispersal of volcanic clouds

    Directory of Open Access Journals (Sweden)

    M. Boichu

    2015-07-01

    exploiting the high spectral resolution of IASI. The validity of the modelled SO2 altitude is further confirmed by the detection of a layer of particles at the same altitude by the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP. Analysis of CALIOP colour and depolarization ratios suggests that these particles consist of sulfate aerosols formed from precursory volcanic SO2. The reconstruction of emission altitude, through inversion procedures which assimilate volcanic SO2 column amounts, requires specific meteorological conditions, especially sufficient wind shear so that gas parcels emitted at different altitudes follow distinct trajectories. We consequently explore the possibility and limits of assimilating in inverse schemes infrared (IR imagery of the volcanic SO2 cloud altitude which will render the inversion procedure independent of the wind shear prerequisite.

  12. The influence of volcanic eruptions on growth of central European trees in NE Germany during the last Millennium

    Science.gov (United States)

    Pieper, H.; Heinrich, I.; Heussner, K. U.; Helle, G.

    2011-12-01

    Large volcanic eruptions have strong impacts on the global climate, lowering the global temperature and increasing the diffuse light fraction for one to several years after the eruptions. It has been argued that due to scattering by volcanic sulfur aerosol the more diffuse light fraction can be used more efficiently by forests. However, other observations suggest a growth decrease because of the cooler conditions following large eruption. Trees growing to the north of the temperate zone are mainly temperature-limited and therefore a reduction in ring width after large volcanic eruptions seems inevitable. Since tree growth in the temperate zone is less limited by temperature than by other climate parameters such as precipitation, it was hypothesized that tree growth may not suffer from lower temperatures so much but profit from increased diffuse light and reduced water stress. Therefore, a database of long tree-ring chronologies originating from several sites in NE-Germany was used to test whether tree growth suffered or profited from the globally changed conditions after large eruptions. The growth relationships were tested against 49 individual large volcanic eruptions from the last 1000 years. High-resolution ice core records of sulfate measurements calibrated against atmospheric observations after modern eruptions identified the timing and magnitude of the eruptions since 1000 CE. A more negative influence on tree growth was detected in two tree-ring width chronologies of oak and pine (Quercus robur L. and Pinus sylvestris L.) originating from three different sites (Greifswald, Eberswalde and Saxony) in eastern Germany for up to four years after large eruptions. Overall, the long tree-ring chronologies covering more or less the last millennium indicated a more negative relationship to volcanic eruptions. In comparison, the chronologies of Q. robur reveal a more negative response after large eruptions than those of P. sylvestris. Only in Greifswald both tree

  13. Sulfur Geochemistry of a Lacustrine Record from Taiwan Reveals Enhanced Marine Aerosol Input during the Early Holocene.

    Science.gov (United States)

    Ding, Xiaodong; Li, Dawei; Zheng, Liwei; Bao, Hongyan; Chen, Huei-Fen; Kao, Shuh-Ji

    2016-12-12

    Lacustrine record of marine aerosol input has rarely been documented. Here, we present the sulfur geochemistry during the last deglaciation and early Holocene of a sediment core retrieved from the Dongyuan Lake in southern Taiwan. An unusually high sulfur peak accompanying pyrite presence is observed at 10.5 ka BP. Such high sulfur content in lacustrine record is unusual. The δ(34)S of sulfur varied from +9.5 to + 17.1‰ with two significant positive shifts at 10.5 and 9.4 ka BP. The sources of sulfur and potential processes involving the sulfur isotope variation including bacterial sulfate reduction, volcanic emissions, in-catchment sulfide oxidation and marine aerosol input are discussed. Enhanced marine aerosol input is the most likely explanation for such sulfur peaks and δ(34)S shifts. The positive δ(34)S shifts appeared concurrently with the maximum landslide events over Taiwan resulted from enhanced typhoon activities. The synchronicity among records suggests that increased typhoon activities promoted sea spray, and consequently enhanced the marine aerosol input with (34)S-enriched sulfate. Our sulfur geochemistry data revealed sea spray history and marine influence onto terrestrial environment at coastal regions. Wider coverage of spatial-temporal lacustrine sulfur geochemistry record is needed to validate the applicability of sulfur proxy in paleoenvironmental research.

  14. Sulfur Geochemistry of a Lacustrine Record from Taiwan Reveals Enhanced Marine Aerosol Input during the Early Holocene

    Science.gov (United States)

    Ding, Xiaodong; Li, Dawei; Zheng, Liwei; Bao, Hongyan; Chen, Huei-Fen; Kao, Shuh-Ji

    2016-12-01

    Lacustrine record of marine aerosol input has rarely been documented. Here, we present the sulfur geochemistry during the last deglaciation and early Holocene of a sediment core retrieved from the Dongyuan Lake in southern Taiwan. An unusually high sulfur peak accompanying pyrite presence is observed at 10.5 ka BP. Such high sulfur content in lacustrine record is unusual. The δ34S of sulfur varied from +9.5 to + 17.1‰ with two significant positive shifts at 10.5 and 9.4 ka BP. The sources of sulfur and potential processes involving the sulfur isotope variation including bacterial sulfate reduction, volcanic emissions, in-catchment sulfide oxidation and marine aerosol input are discussed. Enhanced marine aerosol input is the most likely explanation for such sulfur peaks and δ34S shifts. The positive δ34S shifts appeared concurrently with the maximum landslide events over Taiwan resulted from enhanced typhoon activities. The synchronicity among records suggests that increased typhoon activities promoted sea spray, and consequently enhanced the marine aerosol input with 34S-enriched sulfate. Our sulfur geochemistry data revealed sea spray history and marine influence onto terrestrial environment at coastal regions. Wider coverage of spatial-temporal lacustrine sulfur geochemistry record is needed to validate the applicability of sulfur proxy in paleoenvironmental research.

  15. Characterization of the Eyjafjallajökull volcanic plume over the Iberian Peninsula by lidar remote sensing and ground-level data collection

    Science.gov (United States)

    Revuelta, M. A.; Sastre, M.; Fernández, A. J.; Martín, L.; García, R.; Gómez-Moreno, F. J.; Artíñano, B.; Pujadas, M.; Molero, F.

    2012-03-01

    long distance transport suffered by the plume and by the secondary formation of particulate sulfate from the gaseous sulfur dioxide. The information on volcanic aerosol characteristics after long-range transport provided by this study might contribute to better assess the type of aerosol that reach distant locations.

  16. Climate effects of high-latitude volcanic eruptions: Role of the time of year

    Science.gov (United States)

    Kravitz, Ben; Robock, Alan

    2011-01-01

    We test how the time of year of a large Arctic volcanic eruption determines the climate impacts by conducting simulations with a general circulation model of Earth's climate. For eruptions injecting less than about 3 Tg of SO2 into the lower stratosphere, we expect no detectable climatic effect, no matter what the season of the eruption. For an injection of 5 Tg of SO2 into the lower stratosphere, an eruption in the summer would cause detectable climate effects, whereas an eruption at other times of the year would cause negligible effects. This is mainly due to the seasonal variation in insolation patterns and sulfate aerosol deposition rates. In all cases, the sulfate aerosols that form get removed from the atmosphere within a year after the eruption by large-scale deposition. Our simulations of a June eruption have many similar features to previous simulations of the eruption of Katmai in 1912, including some amount of cooling over Northern Hemisphere continents in the summer of the eruption, which is an expected climate response to large eruptions. Previous Katmai simulations show a stronger climate response, which we attribute to differences in choices of climate model configurations, including their specification of sea surface temperatures rather than the use of a dynamic ocean model as in the current simulations.

  17. The Many Problems with Geoengineering Using Stratospheric Aerosols

    Science.gov (United States)

    Robock, Alan

    2009-05-01

    In response to the global warming problem, there has been a recent renewed call for geoengineering ``solutions'' involving injecting particles into the stratosphere or blocking sunlight with satellites between the Sun and Earth. While volcanic eruptions have been suggested as innocuous examples of stratospheric aerosols cooling the planet, the volcano analog actually argues against geoengineering because of ozone depletion and regional hydrologic and temperature responses. In this talk, I consider the suggestion to create an artificial stratospheric aerosol layer. No systems to conduct geoengineering now exist, but a comparison of different proposed stratospheric injection schemes, airplanes, balloons, artillery, and a space elevator, shows that using airplanes would not be that expensive. We simulated the climate response to both tropical and Arctic stratospheric injection of sulfate aerosol precursors using a comprehensive atmosphere-ocean general circulation model, the National Aeronautics and Space Administration Goddard Institute for Space Studies ModelE. We simulated the injection of SO2 and the model converts it to sulfate aerosols, transports them and removes them through dry and wet deposition, and calculates the climate response to the radiative forcing from the aerosols. We conducted simulations of future climate with the Intergovernmental Panel on Climate Change A1B business-as-usual scenario both with and without geoengineering, and compare the results. We found that if there were a way to continuously inject SO2 into the lower stratosphere, it would produce global cooling. Acid deposition from the sulfate would not be enough to disturb most ecosystems. Tropical SO2 injection would produce sustained cooling over most of the world, with more cooling over continents. Arctic SO2 injection would not just cool the Arctic. But both tropical and Arctic SO2 injection would disrupt the Asian and African summer monsoons, reducing precipitation to the food supply

  18. Climatic impacts of stratospheric geoengineering with sulfate, black carbon and titania injection

    Directory of Open Access Journals (Sweden)

    A. C. Jones

    2015-11-01

    Full Text Available In this paper, we examine the potential climatic effects of geoengineering by sulfate, black carbon and titania injection against a baseline RCP8.5 scenario. We use the HadGEM2-CCS model to simulate scenarios in which the top-of-the-atmosphere radiative imbalance due to rising greenhouse gas concentrations is offset by sufficient aerosol injection throughout the 2020–2100 period. We find that the global-mean temperature is effectively maintained at historical levels for the entirety of the period for all 3 aerosol-injection scenarios, though there are a wide range of side-effects which are discussed in detail. The most prominent conclusion is that although the BC injection rate necessary to produce an equivalent global mean temperature-response is much lower, the severity of stratospheric temperature changes (> +70 °C and precipitation impacts effectively exclude BC from being a viable option for geoengineering. Additionally, while it has been suggested that titania would be an effective particle because of its high scattering efficiency, it also efficiently absorbs solar ultraviolet radiation producing a significant stratospheric warming (> +20 °C. As injection rates for titania are close to those for sulfate, there appears little benefit of using titania when compared to injection of sulfur dioxide, which has the added benefit of being well modelled through extensive research that has been carried out on naturally occurring explosive volcanic eruptions.

  19. Climatic impacts of stratospheric geoengineering with sulfate, black carbon and titania injection

    Science.gov (United States)

    Jones, Anthony C.; Haywood, James M.; Jones, Andy

    2016-03-01

    In this paper, we examine the potential climatic effects of geoengineering by sulfate, black carbon and titania injection against a baseline RCP8.5 scenario. We use the HadGEM2-CCS model to simulate scenarios in which the top-of-the-atmosphere radiative imbalance due to rising greenhouse gas concentrations is offset by sufficient aerosol injection throughout the 2020-2100 period. We find that the global-mean temperature is effectively maintained at historical levels for the entirety of the period for all three aerosol-injection scenarios, though there is a wide range of side-effects which are discussed in detail. The most prominent conclusion is that although the BC injection rate necessary to produce an equivalent global mean temperature response is much lower, the severity of stratospheric temperature changes (> +70 °C) and precipitation impacts effectively exclude BC from being a viable option for geoengineering. Additionally, while it has been suggested that titania would be an effective particle because of its high scattering efficiency, it also efficiently absorbs solar ultraviolet radiation producing a significant stratospheric warming (> +20 °C). As injection rates and climatic impacts for titania are close to those for sulfate, there appears to be little benefit in terms of climatic influence of using titania when compared to the injection of sulfur dioxide, which has the added benefit of being well-modeled through extensive research that has been carried out on naturally occurring explosive volcanic eruptions.

  20. Coupled Model Intercomparison Project 5 (CMIP5) simulations of climate following volcanic eruptions

    KAUST Repository

    Driscoll, Simon

    2012-09-16

    The ability of the climate models submitted to the Coupled Model Intercomparison Project 5 (CMIP5) database to simulate the Northern Hemisphere winter climate following a large tropical volcanic eruption is assessed. When sulfate aerosols are produced by volcanic injections into the tropical stratosphere and spread by the stratospheric circulation, it not only causes globally averaged tropospheric cooling but also a localized heating in the lower stratosphere, which can cause major dynamical feedbacks. Observations show a lower stratospheric and surface response during the following one or two Northern Hemisphere (NH) winters, that resembles the positive phase of the North Atlantic Oscillation (NAO). Simulations from 13 CMIP5 models that represent tropical eruptions in the 19th and 20th century are examined, focusing on the large-scale regional impacts associated with the large-scale circulation during the NH winter season. The models generally fail to capture the NH dynamical response following eruptions. They do not sufficiently simulate the observed post-volcanic strengthened NH polar vortex, positive NAO, or NH Eurasian warming pattern, and they tend to overestimate the cooling in the tropical troposphere. The findings are confirmed by a superposed epoch analysis of the NAO index for each model. The study confirms previous similar evaluations and raises concern for the ability of current climate models to simulate the response of a major mode of global circulation variability to external forcings. This is also of concern for the accuracy of geoengineering modeling studies that assess the atmospheric response to stratosphere-injected particles.

  1. Initial fate of fine ash and sulfur from large volcanic eruptions

    Directory of Open Access Journals (Sweden)

    U. Niemeier

    2009-08-01

    Full Text Available Large volcanic eruptions emit huge amounts of sulfur and fine ash into the stratosphere. These products cause an impact on radiative processes, temperature and wind patterns. In simulations with a General Circulation Model including detailed aerosol microphysics, the relation between the impact of sulfur and fine ash is determined for different eruption strengths and locations, one in the tropics and one in high Northern latitudes. Fine ash with effective radii between 1 μm and 15 μm has a lifetime of several days only. Nevertheless, the strong absorption of shortwave and longwave radiation causes additional heating and cooling of ±20 K/day and impacts the evolution of the volcanic cloud. Depending on the location of the volcanic eruption, transport direction changes due to the presence of fine ash, vortices develop and temperature anomalies at ground increase. The results show substantial impact on the local scale but only minor impact on the evolution of sulfate in the stratosphere in the month after the simulated eruptions.

  2. Initial fate of fine ash and sulfur from large volcanic eruptions

    Directory of Open Access Journals (Sweden)

    S. Self

    2009-11-01

    Full Text Available Large volcanic eruptions emit huge amounts of sulfur and fine ash into the stratosphere. These products cause an impact on radiative processes, temperature and wind patterns. In simulations with a General Circulation Model including detailed aerosol microphysics, the relation between the impact of sulfur and fine ash is determined for different eruption strengths and locations, one in the tropics and one in high Northern latitudes. Fine ash with effective radii between 1 μm and 15 μm has a lifetime of several days only. Nevertheless, the strong absorption of shortwave and long-wave radiation causes additional heating and cooling of ±20 K/day and impacts the evolution of the volcanic cloud. Depending on the location of the volcanic eruption, transport direction changes due to the presence of fine ash, vortices develop and temperature anomalies at ground increase. The results show substantial impact on the local scale but only minor impact on the evolution of sulfate in the stratosphere in the month after the simulated eruptions.

  3. Solar geoengineering using solid aerosol in the stratosphere

    Science.gov (United States)

    Weisenstein, D. K.; Keith, D. W.; Dykema, J. A.

    2015-10-01

    Solid aerosol particles have long been proposed as an alternative to sulfate aerosols for solar geoengineering. Any solid aerosol introduced into the stratosphere would be subject to coagulation with itself, producing fractal aggregates, and with the natural sulfate aerosol, producing liquid-coated solids. Solid aerosols that are coated with sulfate and/or have formed aggregates may have very different scattering properties and chemical behavior than uncoated non-aggregated monomers do. We use a two-dimensional (2-D) chemistry-transport-aerosol model to capture the dynamics of interacting solid and liquid aerosols in the stratosphere. As an example, we apply the model to the possible use of alumina and diamond particles for solar geoengineering. For 240 nm radius alumina particles, for example, an injection rate of 4 Tg yr-1 produces a global-average shortwave radiative forcing of -1.2 W m-2 and minimal self-coagulation of alumina although almost all alumina outside the tropics is coated with sulfate. For the same radiative forcing, these solid aerosols can produce less ozone loss, less stratospheric heating, and less forward scattering than sulfate aerosols do. Our results suggest that appropriately sized alumina, diamond or similar high-index particles may have less severe technology-specific risks than sulfate aerosols do. These results, particularly the ozone response, are subject to large uncertainties due to the limited data on the rate constants of reactions on the dry surfaces.

  4. Sulfur and nitrogen compounds in urban aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Tanner, R L

    1979-01-01

    This paper reports results from a detailed chemical and meteorological data base that has been accumulated for the New York City subregion. Aerosol sampling during August 1976 and February 1977 sampling periods was done only in an urban New York site and a background site at High Point, NJ. The sampling program was expanded to Brookhaven (Long Island) and New Haven, Connecticut sites during summer 1977 and winter 1978 sampling. Time resolution for aerosol filter samples was 6 hr, with some 3 hr sampling for the latter three periods. Parameters measured included chemical constituents: strong acid (quartz filters only), ammonium, sulfate and nitrate, sulfuric acid (limited data); physical parameters: aerosol size distributions by cascade impactor, cyclone sampler, EAA, on optical counter and a special diffusion battery-CNC apparatus; light scattering nephelometer and other instrumentation; chemically-speciated size classification by diffusion sampler; trace metals by atomic absorption; halogen compounds by NAA; meteorological measurements of RH, temperature, wind speed and direction; gaseous measurements of SO/sub 2/, ozone, NO/sub x/ and hydrocarbons at some locations for some sampling periods. The existence of aerosol sulfate in the ambient environment predominantly in the chemical form of sulfuric acid mostly neutralized by ammonia is now well documented. The average composition of fine particle (< 3.5 ..mu..m) sulfate in summer 1976 aerosols was approximately that letovicite ((NH/sub 4/)/sub 3/H(SO/sub 4/)/sub 2/). Based on the impactor data, about 85% of the aerosol sulfate mass was in the fine particle fraction. About 50% of this aerosol sulfate was deduced to be in the suboptical size regime (< 0.25 ..mu..m) from diffusion processor data. The H/sup +//SO/sub 4//sup 2 -/ ratio in suboptical aerosols did not significantly differ from that in fine fraction aerosol. The coarse particle sulfate was not associated with H/sup +/ or NH/sub 4//sup +/ and comprised

  5. Atmospheric chemistry in volcanic plumes.

    Science.gov (United States)

    von Glasow, Roland

    2010-04-13

    Recent field observations have shown that the atmospheric plumes of quiescently degassing volcanoes are chemically very active, pointing to the role of chemical cycles involving halogen species and heterogeneous reactions on aerosol particles that have previously been unexplored for this type of volcanic plumes. Key features of these measurements can be reproduced by numerical models such as the one employed in this study. The model shows sustained high levels of reactive bromine in the plume, leading to extensive ozone destruction, that, depending on plume dispersal, can be maintained for several days. The very high concentrations of sulfur dioxide in the volcanic plume reduces the lifetime of the OH radical drastically, so that it is virtually absent in the volcanic plume. This would imply an increased lifetime of methane in volcanic plumes, unless reactive chlorine chemistry in the plume is strong enough to offset the lack of OH chemistry. A further effect of bromine chemistry in addition to ozone destruction shown by the model studies presented here, is the oxidation of mercury. This relates to mercury that has been coemitted with bromine from the volcano but also to background atmospheric mercury. The rapid oxidation of mercury implies a drastically reduced atmospheric lifetime of mercury so that the contribution of volcanic mercury to the atmospheric background might be less than previously thought. However, the implications, especially health and environmental effects due to deposition, might be substantial and warrant further studies, especially field measurements to test this hypothesis.

  6. Aviation response to a widely dispersed volcanic ash and gas cloud from the August 2008 eruption of Kasatochi, Alaska, USA

    Science.gov (United States)

    Guffanti, Marianne; Schneider, David J.; Wallace, Kristi L.; Hall, Tony; Bensimon, Dov R.; Salinas, Leonard J.

    2010-01-01

    The extensive volcanic cloud from Kasatochi's 2008 eruption caused widespread disruptions to aviation operations along Pacific oceanic, Canadian, and U.S. air routes. Based on aviation hazard warnings issued by the National Oceanic and Atmospheric Administration, U.S. Geological Survey, the Federal Aviation Administration, and Meteorological Service of Canada, air carriers largely avoided the volcanic cloud over a 5 day period by route modifications and flight cancellations. Comparison of time coincident GOES thermal infrared (TIR) data for ash detection with Ozone Monitoring Instrument (OMI) ultraviolet data for SO2 detection shows congruent areas of ash and gas in the volcanic cloud in the 2 days following onset of ash production. After about 2.5 days, the area of SO2 detected by OMI was more extensive than the area of ash indicated by TIR data, indicating significant ash depletion by fall out had occurred. Pilot reports of visible haze at cruise altitudes over Canada and the northern United States suggested that SO2 gas had converted to sulfate aerosols. Uncertain about the hazard potential of the aging cloud, airlines coped by flying over, under, or around the observed haze layer. Samples from a nondamaging aircraft encounter with Kasatochi's nearly 3 day old cloud contained volcanic silicate particles, confirming that some fine ash is present in predominantly gas clouds. The aircraft's exposure to ash was insufficient to cause engine damage; however, slightly damaging encounters with volcanic clouds from eruptions of Reventador in 2002 and Hekla in 2000 indicate the possibility of lingering hazards associated with old and/or diffuse volcanic clouds.

  7. Building a Sectional Aerosol Model in CAM5

    Science.gov (United States)

    Yu, P.; Toon, O. B.

    2013-12-01

    Aerosols are widely distributed around the globe. In the current study I use a sectional aerosol microphysics model (CARMA) coupled with the NCAR global climate model, CAM5, to simulate the spatial-temporal distribution of various types of aerosols including organics, black carbon, sulfate, sea salt and dust. Organics and black carbon surface concentrations are simulated within ~50% over the U.S, and Europe compared with observations; the amount of modeled sulfate and organics are equal in UTLS region as observed by the Pre-AVE field campaign; aerosol extinction in the UTLS observed by SAGEII can be explained by secondary organic aerosols combined with sulfate aerosol. For treating secondary organic aerosols, the volatility-basis-set method improves the budget at surface level relative to the traditional two-product partitioning method; black carbon global budget is largely improved especially in high latitudes by introducing new emission database.

  8. Temporal variations of flux and altitude of sulfur dioxide emissions during volcanic eruptions: implications for long-range dispersal of volcanic clouds

    Directory of Open Access Journals (Sweden)

    M. Boichu

    2015-02-01

    of the modeled SO2 altitude is further confirmed by the detection of a layer of particles at the same altitude by the spaceborne CALIOP LiDAR. Analysis of CALIOP color and depolarization ratios suggests that these particles consist of sulfate aerosols formed from precursory volcanic SO2. The reconstruction of emission altitude, through inversion procedures which assimilate volcanic SO2 column amounts, requires specific meteorological conditions, especially sufficient wind shear so that gas parcels emitted at different altitudes follow distinct trajectories. We consequently explore the possibility and limits of assimilating in inverse schemes infrared (IR imagery of the volcanic SO2 cloud altitude which will render the inversion procedure independent of the wind shear prerequisite.

  9. Volcanic gas

    Science.gov (United States)

    McGee, Kenneth A.; Gerlach, Terrance M.

    1995-01-01

    In Roman mythology, Vulcan, the god of fire, was said to have made tools and weapons for the other gods in his workshop at Olympus. Throughout history, volcanoes have frequently been identified with Vulcan and other mythological figures. Scientists now know that the “smoke" from volcanoes, once attributed by poets to be from Vulcan’s forge, is actually volcanic gas naturally released from both active and many inactive volcanoes. The molten rock, or magma, that lies beneath volcanoes and fuels eruptions, contains abundant gases that are released to the surface before, during, and after eruptions. These gases range from relatively benign low-temperature steam to thick hot clouds of choking sulfurous fume jetting from the earth. Water vapor is typically the most abundant volcanic gas, followed by carbon dioxide and sulfur dioxide. Other volcanic gases are hydrogen sulfide, hydrochloric acid, hydrogen, carbon monoxide, hydrofluoric acid, and other trace gases and volatile metals. The concentrations of these gas species can vary considerably from one volcano to the next.

  10. Solar geoengineering using solid aerosol in the stratosphere

    Directory of Open Access Journals (Sweden)

    D. K. Weisenstein

    2015-04-01

    Full Text Available Solid aerosol particles have long been proposed as an alternative to sulfate aerosols for solar geoengineering. Any solid aerosol introduced into the stratosphere would be subject to coagulation with itself, producing fractal aggregates, and with the natural sulfate aerosol, producing liquid-coated solids. Solid aerosols that are coated with sulfate and/or have formed aggregates may have very different scattering properties and chemical behavior than do uncoated non-aggregated monomers. We use a two-dimensional chemical transport model to capture the dynamics of interacting solid and liquid aerosols in the stratosphere. As an example, we apply the model to the possible use of alumina and diamond particles for solar geoengineering. For 240 nm radius alumina particles, for example, an injection rate of 4 Mt yr−1 produces a global-average radiative forcing of 1.3 W m−2 and minimal self-coagulation of alumina yet almost all alumina outside the tropics is coated with sulfate. For the same radiative forcing, these solid aerosols can produce less ozone loss, less stratospheric heating, and less forward scattering than do sulfate aerosols. Our results suggest that appropriately sized alumina, diamond or similar high-index particles may have less severe technology-specific risks than do sulfate aerosols. These results, particularly the ozone response, are subject to large uncertainties due the limited data on the rate constants of reactions on the dry surfaces.

  11. 硫酸沙丁胺醇气雾剂吸入与茶碱控释片治疗老年哮喘的疗效%Effect of inhaled salbutamol sulfate aerosol and sustained release theophylline treatment of elderly asthma

    Institute of Scientific and Technical Information of China (English)

    禤肇泉; 谭力雄

    2016-01-01

    目的:对硫酸沙丁胺醇气雾剂吸入与茶碱控释片急诊治疗老年哮喘患者的临床效果进行分析探讨。方法选取我院急诊科收治的120例老年哮喘患者随机分为研究组与参考组,各60例,参考组患者仅应用硫酸沙丁胺醇气雾剂治疗,研究组患者应用硫酸沙丁胺醇气雾剂吸入与茶碱控释片治疗。结果研究组患者哮喘症状消失时间、肺功能改善、治疗有效率、生存质量以及不良反应等指标均优于参考组(P<0.05)。结论应用硫酸沙丁胺醇气雾剂吸入与茶碱控释片急诊治疗老年哮喘患者,能够明显改善患者肺功能,提高生存质量与治疗有效率,并降低不良反应。%Objective To analyze and study the clinical effect of inhaled salbutamol sulfate aerosol and sustained release theophylline in the emergency treatment of patients with elderly asthma. Methods 120 patients with elderly asthma, who were received and treated in emergency department of our hospital,were selected and were randomly divided into study group and control group,with 60 cases in each group.To treat single with inhaled salbutamol sulfate aerosol on patients in control group,to treat with inhaled salbutamol sulfate aerosol and sustained release theophylline on patients in study group. Results The asthma symptoms disappeared time,the improvement of pulmonary function, the treatment effective rate,the quality of life,and the adverse reactions and etc.of patients in study group were better than which in control group(P < 0.05). Conclusion Inhaled salbutamol sulfate aerosol and sustained release theophylline in the emergency treatment of patients with elderly asthma could obviously improve the pulmonary function of patients,could improve the quality of life and treatment effective rate, could reduce the adverse reactions.

  12. Calibration and measurement uncertainties of a continuous-flow cloud condensation nuclei counter (DMT-CCNC: CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment

    Directory of Open Access Journals (Sweden)

    D. Rose

    2007-06-01

    Full Text Available Experimental and theoretical uncertainties in the measurement of cloud condensation nuclei (CCN with a continuous-flow thermal-gradient CCN counter from Droplet Measurement Technologies (DMT-CCNC have been assessed by model calculations and calibration experiments with ammonium sulfate and sodium chloride aerosol particles in the diameter range of 20–220 nm. Experiments have been performed in the laboratory and during field measurement campaigns, extending over a period of more than one year and covering a wide range of operating conditions (650–1020 hPa ambient pressure, 0.5–1.0 L min−1 aerosol flow rate, 20–30°C inlet temperature, 4–34 K m−1 temperature gradient. For each set of conditions, the effective water vapor supersaturation (Seff in the CCNC was determined from the measured CCN activation spectra and Köhler model calculations.

    High measurement precision was achieved under stable laboratory conditions, where relative variations of Seff in the CCNC were generally less than ±2%. During field measurements, however, the relative variability increased up to ±5–7%, which can be mostly attributed to variations of the CCNC column top temperature with ambient temperature.

    To assess the accuracy of the Köhler models used to calculate Seff, we have performed a comprehensive comparison and uncertainty analysis of the various Köhler models and thermodynamic parameterizations commonly used in CCN studies. For the relevant supersaturation range (0.05–2%, the relative deviations between different modeling approaches were as high as 25% for (NH42SO4 and 16% for NaCl. The deviations were mostly caused by the different parameterizations for the activity of water in aqueous solutions of (NH42SO4 and NaCl (activity parameterization, osmotic coefficient, and van't Hoff

  13. Volcanic Catastrophes

    Science.gov (United States)

    Eichelberger, J. C.

    2003-12-01

    The big news from 20th century geophysics may not be plate tectonics but rather the surprise return of catastrophism, following its apparent 19th century defeat to uniformitarianism. Divine miracles and plagues had yielded to the logic of integrating observations of everyday change over time. Yet the brilliant interpretation of the Cretaceous-Tertiary Boundary iridium anomaly introduced an empirically based catastrophism. Undoubtedly, decades of contemplating our own nuclear self-destruction played a role in this. Concepts of nuclear winter, volcanic winter, and meteor impact winter are closely allied. And once the veil of threat of all-out nuclear exchange began to lift, we could begin to imagine slower routes to destruction as "global change". As a way to end our world, fire is a good one. Three-dimensional magma chambers do not have as severe a magnitude limitation as essentially two-dimensional faults. Thus, while we have experienced earthquakes that are as big as they get, we have not experienced volcanic eruptions nearly as great as those preserved in the geologic record. The range extends to events almost three orders of magnitude greater than any eruptions of the 20th century. Such a calamity now would at the very least bring society to a temporary halt globally, and cause death and destruction on a continental scale. At maximum, there is the possibility of hindering photosynthesis and threatening life more generally. It has even been speculated that the relative genetic homogeneity of humankind derives from an evolutionary "bottleneck" from near-extinction in a volcanic cataclysm. This is somewhat more palatable to contemplate than a return to a form of Original Sin, in which we arrived at homogeneity by a sort of "ethnic cleansing". Lacking a written record of truly great eruptions, our sense of human impact must necessarily be aided by archeological and anthropological investigations. For example, there is much to be learned about the influence of

  14. Model guidance for deployment of observational resources following a major volcanic eruption

    Science.gov (United States)

    Colarco, P. R.; Aquila, V.; LeGrande, A. N.; Tsigaridis, K.; Newman, P. A.

    2016-12-01

    The 1991 eruption of Mt. Pinatubo in the Philippines increased the stratospheric aerosol burden by orders of magnitude and perturbed the global Earth system by modifying the atmosphere's radiation balance, perturbing tropospheric and stratospheric temperatures, increasing stratospheric water vapor concentration, changing the chemical balance of the stratosphere, enhancing ozone depletion, and modifying the dynamics of the stratosphere. We know from the smaller El Chichón eruption in Mexico in 1982 that the climate response to large eruptions is not simply proportional to the amount of sulfur emitted: while Mt. Pinatubo injected more than twice as much sulfate aerosol as El Chichón, it produced a much smaller tropical stratospheric warming. The climate response to a major volcanic eruption depends thus on a number of factors, including the amount of material released (including sulfur, water, and halogen compounds), the altitude of injection, the latitude, and season. Characterizing important parameters following an eruption and monitoring the subsequent volcanic plume evolution will be important activities for the international research community in the weeks-to-months-to-years following a major eruption. In order to provide NASA advance guidance to support its deployment of airborne and in situ resources following a major eruption, we have performed a series of simulations with two Earth system models—the NASA GSFC Goddard Earth Observing System, version 5 (GEOS-5), and the GISS ModelE—in which we explore the evolution of the volcanic plume resulting from a Pinatubo-magnitude eruption. In particular, we explore the evolution of the resulting aerosol plume, including its amount, altitude, lifetime, and particle size distribution, as well as recovery of the perturbed atmosphere to pre-eruption conditions. Our suite of simulations investigates both the month and latitude of the eruption as important factors in determining the plume evolution. We use two Earth

  15. Attachment behavior of fission products to solution aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Takamiya, Koichi; Tanaka, Toru; Nitta, Shinnosuke; Itosu, Satoshi; Sekimoto, Shun; Oki, Yuichi; Ohtsuki, Tsutomu [Research Reactor Institute, Kyoto University, Osaka (Japan)

    2016-12-15

    Various characteristics such as size distribution, chemical component and radioactivity have been analyzed for radioactive aerosols released from Fukushima Daiichi Nuclear Power Plant. Measured results for radioactive aerosols suggest that the potential transport medium for radioactive cesium was non-sea-salt sulfate. This result indicates that cesium isotopes would preferentially attach with sulfate compounds. In the present work the attachment behavior of fission products to aqueous solution aerosols of sodium salts has been studied using a generation system of solution aerosols and spontaneous fission source of {sup 248}Cm. Attachment ratios of fission products to the solution aerosols were compared among the aerosols generated by different solutions of sodium salt. A significant difference according as a solute of solution aerosols was found in the attachment behavior. The present results suggest the existence of chemical effects in the attachment behavior of fission products to solution aerosols.

  16. Effects of seed aerosols on the growth of secondary organic aerosols from the photooxidation of toluene

    Institute of Scientific and Technical Information of China (English)

    HAO Li-qing; WANG Zhen-ya; HUANG Ming-qiang; FANG Li; ZHANG Wei-jun

    2007-01-01

    Hydroxyl radical (·OH)-initiated photooxidation reaction of toluene was carried out in a self-made smog chamber. Four individual seed aerosols such as ammonium sulfate, ammonium nitrate, sodium silicate and calcium chloride, were introduced into the chamber to assess their influence on the growth of secondary organic aerosols (SOA). It was found that the low concentration of seed aerosols might lead to high concentration of SOA particles. Seed aerosols would promote rates of SOA formation at the start of the reaction and inhibit its formation rate with prolonging the reaction time. In the case of cv. 9000 pt/cm3 seed aerosol load, the addition of sodium silicate induced a same effect on the SOA formation as ammonium nitrate. The influence of the four individual seed aerosols on the generation of SOA increased in the order of calcium chloride>sodium silicate and ammonium nitrate> ammonium sulfate.

  17. Sensitivity of aerosol radiative forcing calculations to spectral resolution

    Energy Technology Data Exchange (ETDEWEB)

    Grant, K.E.

    1996-10-01

    Potential impacts of aerosol radiative forcing on climate have generated considerable recent interest. An important consideration in estimating the forcing from various aerosol components is the spectral resolution used for the solar radiative transfer calculations. This paper examines the spectral resolution required from the viewpoint of overlapping spectrally varying aerosol properties with other cross sections. A diagnostic is developed for comparing different band choices, and the impact of these choices on the radiative forcing calculated for typical sulfate and biomass aerosols was investigated.

  18. Link of volcanic activity and climate change in Altai studied in the ice core from Belukha Mountain

    OpenAIRE

    N. S. Malygina; T. V. Barlyaeva; T. S. Papina

    2013-01-01

    In the present research we discuss a role of volcanic activity in Altai thermal regime. Here we analyses the sulfate and temperature data reconstructed from the natural paleoarchive – ice core from the Belukha Mountain saddle. Sulfate ice-core reconstructions can serve as volcanic markers. The both – sulfate and temperature reconstructions – are for the last 750 years. As the characteristic of volcanic activity we consider Volcanic Explosivity Index (VEI), Dust Veil Index (DVI) and Ice core v...

  19. Aerosol optical depths and their contributing sources in Taiwan

    Science.gov (United States)

    Chan, K. L.; Chan, K. L.

    2017-01-01

    In this paper, we present a quantitative investigation of the contributions of different aerosols to the aerosol optical depths (AODs) in Taiwan using a global chemical transport model (GEOS-Chem) and remote sensing measurements. The study focus is on the period from June 2012 to October 2013. Five different types of aerosols are investigated: sea salt, dust, sulfate, organic carbon and black carbon. Three of these aerosols, namely sulfate, organic carbon and black carbon, have significant anthropogenic sources. Model simulation results were compared with both ground based sun photometer measurements and MODerate resolution Imaging Spectroradiometer (MODIS) satellite observations. The model data shows good agreement with satellite observations (R = 0.72) and moderate correlation with sun photometer measurements (R = 0.52). Simulation results show the anthropogenic aerosols contribute ∼65% to the total AOD in Taipei, while natural originated aerosols only show a minor impact (∼35%). Among all the aerosols, sulfate is the dominating species, contributing 62.4% to the annual average total AOD. Organic carbon and black carbons respectively contribute 7.3% and 1.5% to the annual averaged total AOD. The annual average contributions of sea salt and dust aerosols to the total AOD are 26.4% and 2.4%, respectively. A sensitivity study was performed to identify the contributions of anthropogenic aerosol sources in each region to the AODs in Taipei. North-East Asia was identified as the major contributing source region of anthropogenic aerosols to Taipei, accounting for more than 50% of total sulfate, 32% of total organic carbon and 51% of total black carbon aerosols. South-East Asia is the second largest contributing source region, contributing 35%, 24% and 34% of total sulfate, organic carbon and black carbon aerosols, respectively. The aerosols from continents other than Asia only show minor impacts to the aerosol load in Taipei. In addition, a case study of a biomass

  20. Ensemble Forecasting of Volcanic Emissions in Hawai’i

    Directory of Open Access Journals (Sweden)

    Andre Kristofer Pattantyus

    2015-03-01

    Full Text Available Deterministic model forecasts do not convey to the end users the forecast uncertainty the models possess as a result of physics parameterizations, simplifications in model representation of physical processes, and errors in initial conditions. This lack of understanding leads to a level of uncertainty in the forecasted value when only a single deterministic model forecast is available. Increasing computational power and parallel software architecture allows multiple simulations to be carried out simultaneously that yield useful measures of model uncertainty that can be derived from ensemble model results. The Hybrid Single Particle Lagrangian Integration Trajectory and Dispersion model has the ability to generate ensemble forecasts. A meteorological ensemble was formed to create probabilistic forecast products and an ensemble mean forecast for volcanic emissions from the Kilauea volcano that impacts the state of Hawai’i. The probabilistic forecast products show uncertainty in pollutant concentrations that are especially useful for decision-making regarding public health. Initial comparison of the ensemble mean forecasts with observations and a single model forecast show improvements in event timing for both sulfur dioxide and sulfate aerosol forecasts.  

  1. Time-slice last millennium experiments with interactive gas-phase chemistry and aerosols

    Science.gov (United States)

    Tsigaridis, K.; Legrande, A. N.; Koch, D. M.

    2010-12-01

    Preliminary results from coupled atmosphere-ocean simulations with interactive gas-phase chemistry and aerosols are presented. These experiments are decadal scale time-slices within millennial-length simulations performed with the GISS GCM (ModelE), using two different ocean models. The boundary conditions for the transient simulations follow the last millennium coordinated PMIP3 experiment protocol. This experiment directly links in with other pre-Industrial experiments being completed as part of IPCC AR5, using the same model and resolution as in GISS IPCC AR5. Preliminary time-slice results from the early medieval and Maunder Minimum periods will be presented. The impact of the presence of short-lived gases and aerosols on the simulated climate is studied. An initial attempt to identify previously omitted additional forcing mechanisms will be performed during these contrasting climate periods, in short duration experiments driven by ocean conditions from the transient experiments. The results presented are the initial runs from a larger set of experiments that will assess the climate impact of changes to dust, sea-salt, and ocean-derived sulfate, biomass burning ozone-precursors and aerosols, organic carbon, wetland methane emissions, and a final set with all components. These species are standard components in the GISS model’s 20th century simulations, so that we may compare millennial variability characteristics with those better constrained from more recent climate periods. Dust and sea-salt are wind-driven aerosols from deserts and oceans, sulfate comes from oxidation of volcanic and oceanic precursors, while organic carbon comes from biomass burning, secondary plant sources and primary oceanic emissions. Comparison of model and proxy records will test model-simulated mechanisms while the model provides insight into factors contributing to proxy variability. The addition of potentially important forcing mechanisms will enable a more comprehensive

  2. Climate Throughout Geologic Time Was Cooled by Sequences of Explosive Volcanic Eruptions Forming Aerosols That Reflect and Scatter Ultraviolet Solar Radiation and Warmed by Relatively Continuous Extrusion of Basaltic Lava that Depletes Ozone, Allowing More Solar Ultraviolet Radiation to Reach Earth

    Science.gov (United States)

    Ward, P. L.

    2015-12-01

    Active volcanoes of all sizes and eruptive styles, emit chlorine and bromine gases observed to deplete ozone. Effusive, basaltic volcanic eruptions, typical in Hawaii and Iceland, extrude large lava flows, depleting ozone and causing global warming. Major explosive volcanoes also deplete ozone with the same emissions, causing winter warming, but in addition eject megatons of water and sulfur dioxide into the lower stratosphere where they form sulfuric-acid aerosols whose particles grow large enough to reflect and scatter ultraviolet sunlight, causing net global cooling for a few years. The relative amounts of explosive and effusive volcanism are determined by the configuration of tectonic plates moving around Earth's surface. Detailed studies of climate change throughout geologic history, and since 1965, are not well explained by greenhouse-gas theory, but are explained quite clearly at OzoneDepletionTheory.info. Ozone concentrations vary substantially by the minute and show close relationships to weather system highs and lows (as pointed out by Dobson in the 1920s), to the height of the tropopause, and to the strength and location of polar vortices and jet streams. Integrating the effects of volcanism on ozone concentrations and the effects of ozone concentrations on synoptic weather patterns should improve weather forecasting. For example, the volcano Bárðarbunga, in central Iceland, extruded 85 km2 of basaltic lava between August 29, 2014, and February 28, 2015, having a profound effect on weather. Most surprising, more than a week before the March 4 eruption of Eyjafjallajökull in 2010, substantial amounts of ozone were released in the vicinity of the volcano precisely when surface deformation showed that magma first began moving up from sills below 4 km depth. Ozone similarly appears to have been emitted 3.5 months before the Pinatubo eruption in 1991. Readily available daily maps of ozone concentrations may allow early warning of an imminent volcanic

  3. Aerosol modeling in CNRM-CM: evaluation of recent developments on natural aerosols and implications for aerosol radiative forcing

    Science.gov (United States)

    Nabat, Pierre; Michou, Martine; Watson, Laura; Saint-Martin, David

    2017-04-01

    Aerosols interact with shortwave and longwave radiation with ensuing consequences on the radiative budget and climate. Their representation in climate models is consequently essential to estimate their radiative forcing and their role in the climate system. However, up to now, the evaluation of these aerosol schemes is often limited to the integrated atmospheric aerosol content given by the aerosol optical depth (AOD). In the climate model CNRM-CM, the TACTIC (Tropospheric Aerosols for ClimaTe in CNRM-CM, Michou et al., 2015) aerosol scheme includes the five main aerosol species (desert dust, sea-salt, sulfate, black carbon and organic matter). Recent developments have been carried out to improve the representation of natural aerosols, namely the inclusion of the parameterization of Grythe et al. (2014) for sea-salt emissions, the revision of the size distribution of sea-salt aerosols, and the increase of the number of bins to represent dust aerosols. The objective of this work is to evaluate the contribution of these developments to the representation of aerosols in CNRM-CM, using not only AOD from satellite data, but also aerosol vertical distribution and concentrations from in-situ measurements. Simulations have thus been carried out using different configurations of the aerosol scheme over the period 2000-2015, to allow for an evaluation against available measurements. The results show a relatively good performance of the model, but also reveal some discrepancies in the aerosol vertical distribution. The impact on the radiative budget of these changes in aerosol loads has been estimated, and shows the importance of the representation of natural aerosols for the estimation of aerosol radiative forcing.

  4. Composition of Aerosols Over the Continential U.S.

    Science.gov (United States)

    1991-07-12

    term associated with sulfate. For ammonium sulfate D =4.5, for bisulfate D = 3.8, and D =1 for sulfuric acid . In order to estimate the organics via the... ammonium sulfate. Figure 16. The 3rd quarter aerosol constituents at each eastern location. The sulfate is assumed to be in the form of sulfuric acid , and...degree of neutralization by ammonium . The three common forms of particulate sulfate are ammonium sulfate ((NH4)2SO4), bisulfate (NH4 HSO4), and sulfuric

  5. Volcanic ash plume identification using polarization lidar: Augustine eruption, Alaska

    Science.gov (United States)

    Sassen, Kenneth; Zhu, Jiang; Webley, Peter W.; Dean, K.; Cobb, Patrick

    2007-01-01

    During mid January to early February 2006, a series of explosive eruptions occurred at the Augustine volcanic island off the southern coast of Alaska. By early February a plume of volcanic ash was transported northward into the interior of Alaska. Satellite imagery and Puff volcanic ash transport model predictions confirm that the aerosol plume passed over a polarization lidar (0.694 mm wavelength) site at the Arctic Facility for Atmospheric Remote Sensing at the University of Alaska Fairbanks. For the first time, lidar linear depolarization ratios of 0.10 – 0.15 were measured in a fresh tropospheric volcanic plume, demonstrating that the nonspherical glass and mineral particles typical of volcanic eruptions generate strong laser depolarization. Thus, polarization lidars can identify the volcanic ash plumes that pose a threat to jet air traffic from the ground, aircraft, or potentially from Earth orbit.

  6. Sulfate inhibition effect on sulfate reducing bacteria

    Directory of Open Access Journals (Sweden)

    Sulaiman Al Zuhair

    2008-12-01

    Full Text Available There is an increasing interest in the potential of bacterial sulfate reduction as an alternative method for sulfate removal from wastewater. Under anaerobic conditions, sulfate-reducing bacteria (SRB utilize sulfate to oxidize organic compounds and generate sulfide (S2-. SRB were successfully isolated from sludge samples obtained from a local petroleum refinery, and used for sulfate removal. The effects of initial sulfate concentration, temperature and pH on the rate of bacterial growth and anaerobic sulfate removal were investigated and the optimum conditions were identified. The experimental data were used to determine the parameters of two proposed kinetic model, which take into consideration substrate inhibition effect. Keywords: Sulfate Reducing Bacteria, Sulfate, Kinetic Model, Biotreatement, Inhibition Received: 31 August 2008 / Received in revised form: 18 September 2008, Accepted: 18 September 2008 Published online: 28 September 2008

  7. Evidence For Volcanic Initiation Of Cretaceous Ocean Anoxic Events (Invited)

    Science.gov (United States)

    Sageman, B. B.; Hurtgen, M. T.; McElwain, J.; Adams, D.; Barclay, R. S.; Joo, Y.

    2010-12-01

    Increasing evidence from studies of Cretaceous ocean anoxic events (OAE’s) has suggested that major changes in volcanic activity may have played a significant role in their genesis. Numerous specific mechanisms of have been proposed, including increases in atmospheric CO2 and surface temperature, leading to enhanced chemical weathering and terrestrial nutrient release, or increases in reduced trace metal fluxes, leading to oxygen depletion and possibly providing micronutrients for enhanced primary production. An additional pathway by which the byproducts of enhanced volcanic activity may have contributed to OAE genesis involves relationships between the biogeochemical cycles sulfur, iron, and phosphorus. Recent analysis of S-isotope data from carbonate-associated sulfate and pyrite collected across the Cenomanian-Turonian OAE2 in the Western Interior basin suggest that increases in sulfate to an initially sulfate-depleted ocean preceded onset of the event. Modern lake data support the idea that increases in sulfate concentration drive microbial sulfate reduction, leading to more efficient regeneration of P from sedimentary organic matter. If the early Cretaceous opening of the South Atlantic was accompanied by evaporite deposition sufficient to draw down global marine sulfate levels, and widespread anoxia leading to elevated pyrite burial helped maintain these low levels for the succeeding 30 myr, during which most Cretaceous OAE’s are found, perhaps pulses of volcanism that rapidly introduced large volumes of sulfate may have played a key role in OAE initiation. The eventually burial of S in the form of pyrite may have returned sulfate levels to a low background, thus providing a mechanism to terminate the anoxic events. This talk will review the evidence for volcanic initiation of OAE’s in the context of the sulfate-phosphorus regeneration model.

  8. Experimental generation of volcanic lightning

    Science.gov (United States)

    Cimarelli, Corrado; Alatorre-Ibargüengoitia, Miguel; Kueppers, Ulrich; Scheu, Bettina; Dingwell, Donald B.

    2014-05-01

    Ash-rich volcanic plumes that are responsible for injecting large quantities of aerosols into the atmosphere are often associated with intense electrical activity. Direct measurement of the electric potential at the crater, where the electric activity in the volcanic plume is first observed, is severely impeded, limiting progress in its investigation. We have achieved volcanic lightning in the laboratory during rapid decompression experiments of gas-particle mixtures under controlled conditions. Upon decompression (from ~100 bar argon pressure to atmospheric pressure), loose particles are vertically accelerated and ejected through a nozzle of 2.8 cm diameter into a large tank filled with air at atmospheric conditions. Because of their impulsive character, our experiments most closely represent the conditions encountered in the gas-thrust region of the plume, when ash is first ejected from the crater. We used sieved natural ash with different grain sizes from Popocatépetl (Mexico), Eyjafjallajökull (Iceland), and Soufrière Hills (Montserrat) volcanoes, as well as micrometric glass beads to constrain the influence of material properties on lightning. We monitored the dynamics of the particle-laden jets with a high-speed camera and the pressure and electric potential at the nozzle using a pressure transducer and two copper ring antennas connected to a high-impedance data acquisition system, respectively. We find that lightning is controlled by the dynamics of the particle-laden jet and by the abundance of fine particles. Two main conditions are required to generate lightning: 1) self-electrification of the particles and 2) clustering of the particles driven by the jet fluid dynamics. The relative movement of clusters of charged particles within the plume generates the gradient in electrical potential, which is necessary for lightning. In this manner it is the gas-particle dynamics together with the evolving particle-density distribution within different regions of

  9. Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign

    Science.gov (United States)

    DeCarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.; Zhou, J.; Tomlinson, J.; Collins,D. R.; Knapp, D.; Weinheimer, A. J.; Montzka,D. D.; Campos,T.; Jimenez, J. L.

    2007-01-01

    The concentration, size, and composition of non-refractory submicron aerosol (NR-PM(sub l)) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS. During the campaign the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM(sub l) mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 microg/cubic m (STP) ppm(exp -1). This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2008). The stability of the OA/CO while O/C increases with photochemical age implies a net loss of carbon from the OA. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major regional source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city

  10. Fast airborne aerosol size and chemistry measurements with the high resolution aerosol mass spectrometer during the MILAGRO Campaign

    Science.gov (United States)

    Decarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.; Zhou, J.; Tomlinson, J.; Collins, D. R.; Knapp, D.; Weinheimer, A. J.; Montzka, D. D.; Campos, T.; Jimenez, J. L.

    2007-12-01

    The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS, in which the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m-3 (STP) ppm-1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2007b). BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city likely due to evaporation. BB does not appear to be a strong source of nitrate despite its high emissions of nitrogen oxides, presumably due to low ammonia

  11. Fast airborne aerosol size and chemistry measurements with the high resolution aerosol mass spectrometer during the MILAGRO Campaign

    Directory of Open Access Journals (Sweden)

    P. F. DeCarlo

    2007-12-01

    Full Text Available The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1 was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS, in which the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA and biomass burning (BB are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m−3 (STP ppm−1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006 and Kleinman et al. (2007b. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city likely due to evaporation. BB does not appear to be a strong source of nitrate

  12. Volcanic hazard management in dispersed volcanism areas

    Science.gov (United States)

    Marrero, Jose Manuel; Garcia, Alicia; Ortiz, Ramon

    2014-05-01

    Traditional volcanic hazard methodologies were developed mainly to deal with the big stratovolcanoes. In such type of volcanoes, the hazard map is an important tool for decision-makers not only during a volcanic crisis but also for territorial planning. According to the past and recent eruptions of a volcano, all possible volcanic hazards are modelled and included in the hazard map. Combining the hazard map with the Event Tree the impact area can be zoned and defining the likely eruptive scenarios that will be used during a real volcanic crisis. But in areas of disperse volcanism is very complex to apply the same volcanic hazard methodologies. The event tree do not take into account unknown vents, because the spatial concepts included in it are only related with the distance reached by volcanic hazards. The volcanic hazard simulation is also difficult because the vent scatter modifies the results. The volcanic susceptibility try to solve this problem, calculating the most likely areas to have an eruption, but the differences between low and large values obtained are often very small. In these conditions the traditional hazard map effectiveness could be questioned, making necessary a change in the concept of hazard map. Instead to delimit the potential impact areas, the hazard map should show the expected behaviour of the volcanic activity and how the differences in the landscape and internal geo-structures could condition such behaviour. This approach has been carried out in La Palma (Canary Islands), combining the concept of long-term hazard map with the short-term volcanic scenario to show the expected volcanic activity behaviour. The objective is the decision-makers understand how a volcanic crisis could be and what kind of mitigation measurement and strategy could be used.

  13. Volcanic loading: The dust veil index

    Energy Technology Data Exchange (ETDEWEB)

    Lamb, H.H. [Univ. of East Anglia, Norwich (United Kingdom). Climatic Research Unit

    1985-09-01

    Dust ejected into the high atmosphere during explosive volcanic eruptions has been considered as a possible cause for climatic change. Dust veils created by volcanic eruptions can reduce the amount of light reaching the Earth`s surface and can cause reductions in surface temperatures. These climatic effects can be seen for several years following some eruptions and the magnitude and duration of the effects depend largely on the density or amount of tephra (i.e. dust) ejected, the latitude of injection, and atmospheric circulation patterns. Lamb (1970) formulated the Dust Veil Index (DVI) in an attempt to quantify the impact on the Earth`s energy balance of changes in atmospheric composition due to explosive volcanic eruptions. The DVI is a numerical index that quantifies the impact on the Earth`s energy balance of changes in atmospheric composition due to explosive volcanic eruptions. The DVI is a numerical index that quantifies the impact of a particular volcanic eruptions release of dust and aerosols over the years following the event. The DVI for any volcanic eruptions are available and have been used in estimating Lamb`s dust veil indices.

  14. Atmosphere aerosol satellite project Aerosol-UA

    Science.gov (United States)

    Milinevsky, Gennadi; Yatskiv, Yaroslav; Syniavskyi, Ivan; Bovchaliuk, Andrii; Degtyaryov, Oleksandr; Sosonkin, Mikhail; Mishchenko, Michael; Danylevsky, Vassyl; Ivanov, Yury; Oberemok, Yevgeny; Masley, Volodymyr; Rosenbush, Vera; Moskalev, Sergii

    2017-04-01

    The experiment Aerosol-UA is Ukrainian space mission aimed to the terrestrial atmospheric aerosol spatial distribution and microphysics investigations. The experiment concept is based on idea of Glory/APS mission of precise orbital measurements of polarization and intensity of the sunlight scattered by the atmosphere, aerosol and the surface the multichannel Scanning Polarimeter (ScanPol) with narrow field-of-view. ScanPol measurements will be accompanied by the wide-angle MultiSpectral Imager-Polarimeter (MSIP). The ScanPol is designed to measure Stokes parameters I, Q, U within the spectral range from the UV to the SWIR in a wide range of phase angles along satellite ground path. Expected ScanPol polarimetric accuracy is 0.15%. A high accuracy measurement of the degree of linear polarization is provided by on-board calibration of the ScanPol polarimeter. On-board calibration is performed for each scan of the mirror scanning system. A set of calibrators is viewed during the part of the scan range when the ScanPol polarimeter looks in the direction opposite to the Earth's surface. These reference assemblies provide calibration of the zero of the polarimetric scale (unpolarized reference assembly) and the scale factor for the polarimetric scale (polarized reference assembly). The zero of the radiometric scale is provided by the dark reference assembly.The spectral channels of the ScanPol are used to estimate the tropospheric aerosol absorption, the aerosol over the ocean and the land surface, the signals from cirrus clouds, stratospheric aerosols caused by major volcanic eruptions, and the contribution of the Earth's surface. The imager-polarimeter MSIP will collect 60°x60° field-of-view images on the state of the atmosphere and surface in the area, where the ScanPol polarimeter will measure, to retrieve aerosol optical depth and polarization properties of aerosol by registration of three Stokes parameters simultaneously in three spectral channels. The two more

  15. Cemented Volcanic Soils, Martian Spectra and Implications for the Martian Climate

    Science.gov (United States)

    Bishop, J. L.; Schiffman, P.; Drief, A.; Southard, R. J.

    2004-03-01

    Cemented volcanic crusts are studied to learn about their composition, formation processes, and implications for climate interactions with the surface on Mars. Such carbonate, sulfate and opal crusts may be present in cemented soil units on Mars.

  16. On the evaporation of ammonium sulfate solution

    Energy Technology Data Exchange (ETDEWEB)

    Drisdell, Walter S.; Saykally, Richard J.; Cohen, Ronald C.

    2009-07-16

    Aqueous evaporation and condensation kinetics are poorly understood, and uncertainties in their rates affect predictions of cloud behavior and therefore climate. We measured the cooling rate of 3 M ammonium sulfate droplets undergoing free evaporation via Raman thermometry. Analysis of the measurements yields a value of 0.58 {+-} 0.05 for the evaporation coefficient, identical to that previously determined for pure water. These results imply that subsaturated aqueous ammonium sulfate, which is the most abundant inorganic component of atmospheric aerosol, does not affect the vapor-liquid exchange mechanism for cloud droplets, despite reducing the saturation vapor pressure of water significantly.

  17. Volcanic hazard assessment in monogenetic volcanic fields

    OpenAIRE

    Bartolini, Stefania

    2014-01-01

    [eng] One of the most important tasks of modern volcanology, which represents a significant socio-economic implication, is to conduct hazard assessment in active volcanic systems. These volcanological studies are aimed at hazard that allows to constructing hazard maps and simulating different eruptive scenarios, and are mainly addressed to contribute to territorial planning, definition of emergency plans or managing volcanic crisis. The impact of a natural event, as a volcanic eruption, can s...

  18. A general circulation model (GCM) parameterization of Pinatubo aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Lacis, A.A.; Carlson, B.E.; Mishchenko, M.I. [NASA Goddard Institute for Space Studies, New York, NY (United States)

    1996-04-01

    The June 1991 volcanic eruption of Mt. Pinatubo is the largest and best documented global climate forcing experiment in recorded history. The time development and geographical dispersion of the aerosol has been closely monitored and sampled. Based on preliminary estimates of the Pinatubo aerosol loading, general circulation model predictions of the impact on global climate have been made.

  19. Effects of aerosols on tropospheric oxidants: A global model study

    Science.gov (United States)

    Tie, Xuexi; Brasseur, Guy; Emmons, Louisa; Horowitz, Larry; Kinnison, Douglas

    2001-10-01

    The global distributions of sulfate and soot particles in the atmosphere are calculated, and the effect of aerosol particles on tropospheric oxidants is studied using a global chemical/transport/aerosol model. The model is developed in the framework of the National Center for Atmospheric Research (NCAR) global three-dimensional chemical/transport model (Model for Ozone and Related Chemical Tracers (MOZART)). In addition to the gas-phase photochemistry implemented in the MOZART model, the present study also accounts for the formation of sulfate and black carbon aerosols as well as for heterogeneous reactions on particles. The simulated global sulfate aerosol distributions and seasonal variation are compared with observations. The seasonal variation of sulfate aerosols is in agreement with measurements, except in the Arctic region. The calculated vertical profiles of sulfate aerosol agree well with the observations over North America. In the case of black carbon the calculated surface distribution is in fair agreement with observations. The effects of aerosol formation and heterogeneous reactions on the surface of sulfate aerosols are studied. The model calculations show the following: (1) The concentration of H2O2 is reduced when sulfate aerosols are formed due to the reaction of SO2 + H2O2 in cloud droplets. The gas-phase reaction SO2 + OH converts OH to HO2, but the reduction of OH and enhancement of HO2 are insignificant (<3%). (2) The heterogeneous reaction of HO2 on the surface of sulfate aerosols produces up to 10% reduction of hydroperoxyl radical (HO2) with an uptake coefficient of 0.2. However, this uptake coefficient could be overestimated, and the results should be regard as an upper limit estimation. (3) The N2O5 reaction on the surface of sulfate aerosols leads to an 80% reduction of NOx at middle to high latitudes during winter. Because ozone production efficiency is low in winter, ozone decreases by only 10% as a result of this reaction. However

  20. Sulfur-rich geothermal emissions elevate acid aerosol levels in metropolitan Taipei.

    Science.gov (United States)

    Lin, Chih-Hung; Mao, I-Fang; Tsai, Pei-Hsien; Chuang, Hsin-Yi; Chen, Yi-Ju; Chen, Mei-Lien

    2010-08-01

    Several studies have demonstrated that millions of people globally are potentially exposed to volcanic gases. Hydrogen sulfide is a typical gas in volcanic and geothermal areas. The gas is toxic at high concentrations that predominantly affects the nervous, cardiovascular, and respiratory systems. The WHO air quality guideline for hydrogen sulfide is 150 microg m(-3) (105 ppb). The northwest part of Taipei is surrounded by sulfur-rich geothermal and hot springs. Active fumaroles and bubbling springs around the geothermal area emit acidic gases. In combination with automobile emissions, the pollution of acid aerosols is characteristic of the metropolis. This study considered sulfur-rich geothermal, suburban and downtown locations of this metropolis to evaluate geothermally emitted acid aerosol and H(2)S pollution. Acid aerosols were collected using a honeycomb denuder filter pack sampling system (HDS), and then analyzed by ion chromatography (IC). Results indicated that long-term geothermal emissions, automobile emissions and photochemical reactions have led to significant variations in air pollution among regions of metropolitan Taipei. The highest H(2)S concentration was 1705 ppb in the geothermal area with low traffic density and the mean concentration was 404.06 ppb, which was higher than WHO guideline and might cause eye irritation. The SO(2) concentrations were relatively low (mean concentration was 3.9 ppb) in this area. It may partially result from the chemical reduction reaction in the geothermal emission, which converted the SO(2) gas into SO(4)(2-) and H(2)S. Consequently, very high sulfate concentrations (mean concentration higher than 25.0 microg m(-3)) were also observed in the area. The geothermal areas also emitted relatively high levels of aerosol acidity, Cl(-), F(-), PO(4)(3-), and N-containing aerosols. As a result, concentrations of HNO(3), NO(2)(-), PO(4)(3-), and SO(4)(2-) in metropolitan Taipei are significantly higher than those in other

  1. Stratospheric Aerosol Measurements

    Science.gov (United States)

    Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

    1998-01-01

    Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

  2. Evaluations of tropospheric aerosol properties simulated by the community earth system model with a sectional aerosol microphysics scheme

    Science.gov (United States)

    Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.

    2015-01-01

    Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data. PMID:27668039

  3. An empirical model of global climate – Part 1: A critical evaluation of volcanic cooling

    Directory of Open Access Journals (Sweden)

    T. Canty

    2013-04-01

    Full Text Available Observed reductions in Earth's surface temperature following explosive volcanic eruptions have been used as a proxy for geoengineering of climate by the artificial enhancement of stratospheric sulfate. Earth cools following major eruptions due to an increase in the reflection of sunlight caused by a dramatic enhancement of the stratospheric sulfate aerosol burden. Significant global cooling has been observed following the four major eruptions since 1900: Santa María, Mount Agung, El Chichón and Mt. Pinatubo, leading IPCC (2007 to state "major volcanic eruptions can, thus, cause a drop in global mean surface temperature of about half a degree Celsius that can last for months and even years". We use a multiple linear regression model applied to the global surface temperature anomaly to suggest that exchange of heat between the atmosphere and ocean, driven by variations in the strength of the Atlantic Meridional Overturning Circulation (AMOC, has been a factor in the decline of global temperature following these eruptions. The veracity of this suggestion depends on whether sea surface temperature (SST in the North Atlantic, sometimes called the Atlantic Multidecadal Oscillation, but here referred to as Atlantic Multidecadal Variability (AMV, truly represents a proxy for the strength of the AMOC. Also, precise quantification of global cooling due to volcanoes depends on how the AMV index is detrended. If the AMV index is detrended using anthropogenic radiative forcing of climate, we find that surface cooling attributed to Mt. Pinatubo, using the Hadley Centre/University of East Anglia surface temperature record, maximises at 0.14 °C globally and 0.32 °C over land. These values are about a factor of 2 less than found when the AMV index is neglected in the model and quite a bit lower than the canonical 0.5 °C cooling usually attributed to Pinatubo. This result is driven by the high amplitude, low frequency component of the AMV index

  4. Stratospheric Aerosol--Observations, Processes, and Impact on Climate

    Science.gov (United States)

    Kresmer, Stefanie; Thomason, Larry W.; von Hobe, Marc; Hermann, Markus; Deshler, Terry; Timmreck, Claudia; Toohey, Matthew; Stenke, Andrea; Schwarz, Joshua P.; Weigel, Ralf; Fueglistaler, Stephan; Prata, Fred J.; Vernier, Jean-Paul; Schlager, Hans; Barnes, John E.; Antuna-Marrero, Juan-Carlos; Fairlie, Duncan; Palm, Mathias; Mahieu, Emmanuel; Notholt, Justus; Rex, Markus; Bingen, Christine; Vanhellemont, Filip; Bourassa, Adam; Plane, John M. C.; Klocke, Daniel; Carn, Simon A.; Clarisse, Lieven; Trickl, Thomas; Neeley, Ryan; James, Alexander D.; Rieger, Landon; Wilson, James C.; Meland, Brian

    2016-01-01

    Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfatematter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

  5. Evaluating aerosol indirect effect through marine stratocumulus clouds

    Energy Technology Data Exchange (ETDEWEB)

    Kogan, Z.N.; Kogan, Y.L.; Lilly, D.K. [Univ. of Oklahoma, Norman, OK (United States)

    1996-04-01

    During the last decade much attention has been focused on anthropogenic aerosols and their radiative influence on the global climate. Charlson et al. and Penner et al. have demonstrated that tropospheric aerosols and particularly anthropogenic sulfate aerosols may significantly contribute to the radiative forcing exerting a cooling influence on climate (-1 to -2 W/m{sup 2}) which is comparable in magnitude to greenhouse forcing, but opposite in sign. Aerosol particles affect the earth`s radiative budget either directly by scattering and absorption of solar radiation by themselves or indirectly by altering the cloud radiative properties through changes in cloud microstructure. Marine stratocumulus cloud layers and their possible cooling influence on the atmosphere as a result of pollution are of special interest because of their high reflectivity, durability, and large global cover. We present an estimate of thet aerosol indirect effect, or, forcing due to anthropogenic sulfate aerosols.

  6. Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

    Science.gov (United States)

    Logan, Timothy S.

    selected four Asian sites. A strongly absorbing mineral dust influence is seen at the Xianghe, Taihu, and SACOL sites during the spring months (MAM) as given by coarse mode dominance. There is a shift towards weakly absorbing pollution (sulfate) and biomass (OC) aerosol dominance in the summer (JJA) and autumn (SON) months as given by a strong fine mode influence. A winter season (DJF) shift toward strongly fine mode, absorbing particles (BC and OC) is observed at Xianghe and Taihu. At Mukdahan, a strong fine mode influence is evident year round with weakly and strongly absorbing biomass particles dominant in the autumn and winter months, respectively, while particles exhibit variable absorption during the spring season. To address SQ2, four cases are selected in Asia to investigate how the optical properties of Asian aerosol plumes change during transport across the remote Pacific Ocean. In addition, six strong smoke events are selected to investigate how the physical and chemical properties of biomass smoke aerosols change during transport in North America. From four selected Asian cases, it was shown by DC-8 aircraft in situ measurements that the Asian plumes contained varying amounts of mineral dust and pollution aerosols during transport. In addition, backward trajectory analysis identified two main dust source regions (Gobi and Taklamakan deserts) and urban/industrial pollution regions in central and eastern China. During the anomalously active wildfire season of 2012 in North America, strong smoke events were observed over the Northern Great Plains region by the Grand Forks, North Dakota, AERONET site and selected as cases. The spectral dependences of absorption aerosol optical depth (AAOD) and o oabs illustrated the varying absorption of the smoke plumes due to carbonaceous particle influences. The AAOD parameter was found to be primarily influenced by aerosol particle size while ooabs was more sensitive to the carbonaceous content. The aerosols likely contain

  7. Statistical extraction of volcanic sulphate from non-Polar ice cores

    NARCIS (Netherlands)

    Moore, J.C.; Beaudon, E.; Kang, S.; Divine, D.; Isaksson, E.; Pohjola, V.A.; van de Wal, R.S.W.

    2012-01-01

    Ice cores from outside the Greenland and Antarctic ice sheets are difficult to date because of seasonal melting and multiple sources (terrestrial, marine, biogenic and anthropogenic) of sulfates deposited onto the ice. Here we present a method of volcanic sulfate extraction that relies on fitting

  8. Statistical extraction of volcanic sulphate from non-Polar ice cores

    NARCIS (Netherlands)

    Moore, J.C.; Beaudon, E.; Kang, S.; Divine, D.; Isaksson, E.; Pohjola, V.A.; van de Wal, R.S.W.

    2012-01-01

    Ice cores from outside the Greenland and Antarctic ice sheets are difficult to date because of seasonal melting and multiple sources (terrestrial, marine, biogenic and anthropogenic) of sulfates deposited onto the ice. Here we present a method of volcanic sulfate extraction that relies on fitting su

  9. Reversible and irreversible processing of biogenic olefins on acidic aerosols

    OpenAIRE

    J. Liggio; Li, S.-M.

    2007-01-01

    Recent evidence has suggested that heterogeneous chemistry of oxygenated hydrocarbons, primarily carbonyls, plays a role in the formation of secondary organic aerosol (SOA); however, evidence is emerging that direct uptake of alkenes on acidic aerosols does occur and can contribute to SOA formation. In the present study, significant uptake of monoterpenes, oxygenated monoterpenes and sesquiterpenes to acidic sulfate aerosols is found under various conditions in a reaction chamber. Proton tran...

  10. Assessment of the global impact of aerosols on tropospheric oxidants

    Science.gov (United States)

    Tie, Xuexi; Madronich, Sasha; Walters, Stacy; Edwards, David P.; Ginoux, Paul; Mahowald, Natalie; Zhang, Renyi; Lou, Chao; Brasseur, Guy

    2005-02-01

    We present here a fully coupled global aerosol and chemistry model for the troposphere. The model is used to assess the interactions between aerosols and chemical oxidants in the troposphere, including (1) the conversion from gas-phase oxidants into the condensed phase during the formation of aerosols, (2) the heterogeneous reactions occurring on the surface of aerosols, and (3) the effect of aerosols on ultraviolet radiation and photolysis rates. The present study uses the global three-dimensional chemical/transport model, Model for Ozone and Related Chemical Tracers, version 2 (MOZART-2), in which aerosols are coupled with the model. The model accounts for the presence of sulfate, soot, primary organic carbon, ammonium nitrate, secondary organic carbon, sea salt, and mineral dust particles. The simulated global distributions of the aerosols are analyzed and evaluated using satellite measurements (Moderate-Resolution Imaging Spectroradiometer (MODIS)) and surface measurements. The results suggest that in northern continental regions the tropospheric aerosol loading is highest in Europe, North America, and east Asia. Sulfate, organic carbon, black carbon, and ammonium nitrate are major contributions for the high aerosol loading in these regions. Aerosol loading is also high in the Amazon and in Africa. In these areas the aerosols consist primarily of organic carbon and black carbon. Over the southern high-latitude ocean (around 60°S), high concentrations of sea-salt aerosol are predicted. The concentration of mineral dust is highest over the Sahara and, as a result of transport, spread out into adjacent regions. The model and MODIS show similar geographical distributions of aerosol particles. However, the model overestimates the sulfate and carbonaceous aerosol in the eastern United States, Europe, and east Asia. In the region where aerosol loading is high, aerosols have important impacts on tropospheric ozone and other oxidants. The model suggests that

  11. Sulfate-rich Archean Oceans

    Science.gov (United States)

    Brainard, J. L.; Choney, A. P.; Ohmoto, H.

    2012-12-01

    There is a widely held belief that prior to 2.4 Ga, the Archean oceans and atmosphere were reducing, and therefore sulfate poor (concentrations 100 m), widely distributed (> km2), and contain only minor amounts of sulfides. These barite beds may have developed from reactions between Ba-rich hydrothermal fluids and evaporate bodies. Simple mass balance calculations suggest that the sulfate contents of the pre-evaporitic seawater must have been greater than ~1 mM. Some researchers have suggested that the SO4 for these beds was derived from the hydrolysis of SO2-rich magmatic fluids. However, this was unlikely as the reaction, 4SO2 + 4H2O → 3H2SO4 + H2S would have produced large amounts of sulfide, as well as sulfate minerals. Many Archean-aged volcanogenic massive sulfide (VMS) deposits, much like those of the younger ages, record evidence for abundant seawater sulfate. As VMS deposits are most likely formed by submarine hydrothermal fluids that developed from seawater circulating through the seafloor rock, much of the seawater sulfate is reduced to from sulfides at depths. However, some residual sulfate in the hydrothermal fluids, with or without the addition of sulfate from the local seawater, can form sulfate minerals such as barite at near the seafloor. The d34S relationships between barites and pyrites in the Archean VMS deposits are similar to those of the younger VMS deposits, except for the lower d34S values for the seawater SO4. The abundance of pyrite in Archean black shales is also evidence of sulfate rich seawater. Pyrites in Archean-aged black shales were most likely the products of either bacterial or thermochemical sulfate reduction during diagenesis of the sediments. Their abundance in sedimentary rocks is determined by: (a) the availability of reactive carbon; (b) the availability of reactive Fe (Fe3+ hydroxides and Fe2+-rich pore fluid); (c) the sedimentation rate; and (d) the flux of SO42- in the sediments, which depends on the seawater SO42

  12. Perturbation of the aerosol layer by aviation-produced aerosols: a parametrization of plume processes

    Energy Technology Data Exchange (ETDEWEB)

    Kaercher, B. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Meilinger, S. [Max-Planck-Institut fuer Chemie (Otto-Hahn-Institut), Mainz (Germany)

    1998-11-01

    The perturbation of the sulfate surface area density (SAD) in the tropopause region and the lower stratosphere by subsonic and supersonic aircraft fleets is examined. The background aerosol surface area, the conversion of fuel sulfur into new sulfate particles in aircraft plumes, and the plume mixing with ambient air control this perturbation. The background aerosol surface area is enhanced by the addition of ultrafine aerosol particles at cruise altitudes. The study includes recent findings concerning the formation and development of these particles in aircraft plumes. Large-scale SAD enhancements become relevant for background SAD levels below about 10 {mu}m{sup 2}/cm{sup 3}, even for moderate sulfate conversion fractions of 5%. Results from an analytic expression for the surface area changes are presented which contains the dependences on these parameters and can be employed in large-scale atmospheric models. (orig.) 11 refs.

  13. Light absorption by secondary organic aerosol from α-pinene: Effects of oxidants, seed aerosol acidity, and relative humidity

    Energy Technology Data Exchange (ETDEWEB)

    Song, Chen [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Now at R. J. Reynolds Tobacco Company, Winston-Salem North Carolina USA; Gyawali, Madhu [Department of Physics, University of Nevada Reno, Nevada System of Higher Education, Reno Nevada USA; Now at Desert Research Institute, Nevada System of Higher Education, Reno Nevada USA; Zaveri, Rahul A. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Shilling, John E. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Arnott, W. Patrick [Department of Physics, University of Nevada Reno, Nevada System of Higher Education, Reno Nevada USA

    2013-10-25

    It is well known that light absorption from dust and black carbon aerosols has a warming effect on climate while light scattering from sulfate, nitrate, and sea salt aerosols has a cooling effect. However, there are large uncertainties associated with light absorption and scattering by different types of organic aerosols, especially in the near-UV and UV spectral regions. In this paper, we present the results from a systematic laboratory study focused on measuring light absorption by secondary organic aerosols (SOAs) generated from dark α-pinene + O3 and α-pinene + NOx + O3 systems in the presence of neutral and acidic sulfate seed aerosols. Light absorption was monitored using photoacoustic spectrometers at four different wavelengths: 355, 405, 532, and 870 nm. Significant light absorption at 355 and 405 nm was observed for the SOA formed from α-pinene + O3 + NO3 system only in the presence of highly acidic sulfate seed aerosols under dry conditions. In contrast, no absorption was observed when the relative humidity was elevated to greater than 27% or in the presence of neutral sulfate seed aerosols. Organic nitrates in the SOA formed in the presence of neutral sulfate seed aerosols were found to be nonabsorbing, while the light-absorbing compounds are speculated to be aldol condensation oligomers with nitroxy organosulfate groups that are formed in highly acidic sulfate aerosols. Finally and overall, these results suggest that dark α-pinene + O3 and α-pinene + NOx + O3 systems do not form light-absorbing SOA under typical atmospheric conditions.

  14. Modeling aerosol processes at the local scale

    Energy Technology Data Exchange (ETDEWEB)

    Lazaridis, M.; Isukapalli, S.S.; Georgopoulos, P.G. [Environmental and Occupational Health Sciences Inst., NJ (United States)

    1998-12-31

    This work presents an approach for modeling photochemical gaseous and aerosol phase processes in subgrid plumes from major localized (e.g. point) sources (plume-in-grid modeling), thus improving the ability to quantify the relationship between emission source activity and ambient air quality. This approach employs the Reactive Plume Model (RPM-AERO) which extends the regulatory model RPM-IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, sodium, chloride and crustal material of aerosols are treated and attributed to the PM size distribution. A modified version of the Carbon Bond IV chemical mechanism is included to model the formation of organic aerosol, and the inorganic multicomponent atmospheric aerosol equilibrium model, SEQUILIB is used for calculating the amounts of inorganic species in particulate matter. Aerosol dynamics modeled include mechanisms of nucleation, condensation and gas/particle partitioning of organic matter. An integrated trajectory-in-grid modeling system, UAM/RPM-AERO, is under continuing development for extracting boundary and initial conditions from the mesoscale photochemical/aerosol model UAM-AERO. The RPM-AERO is applied here to case studies involving emissions from point sources to study sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions.

  15. The relationship between aerosol and cloud drop number concentrations in a global aerosol microphysics model

    Directory of Open Access Journals (Sweden)

    K. J. Pringle

    2009-01-01

    Full Text Available Empirical relationships that link cloud droplet number (CDN to aerosol number or mass are commonly used to calculate global fields of CDN for climate forcing assessments. In this work we use a sectional global model of sulfate and sea-salt aerosol coupled to a mechanistic aerosol activation scheme to explore the limitations of this approach. We find that a given aerosol number concentration produces a wide range of CDN concentrations due to variations in the shape of the aerosol size distribution. On a global scale, the dependence of CDN on the size distribution results in regional biases in predicted CDN (for a given aerosol number. Empirical relationships between aerosol number and CDN are often derived from regional data but applied to the entire globe. In an analogous process, we derive regional "correlation-relations" between aerosol number and CDN and apply these regional relations to calculations of CDN on the global scale. The global mean percentage error in CDN caused by using regionally derived CDN-aerosol relations is 20 to 26%, which is about half the global mean percentage change in CDN caused by doubling the updraft velocity. However, the error is as much as 25–75% in the Southern Ocean, the Arctic and regions of persistent stratocumulus when an aerosol-CDN correlation relation from the North Atlantic is used. These regions produce much higher CDN concentrations (for a given aerosol number than predicted by the globally uniform empirical relations. CDN-aerosol number relations from different regions also show very different sensitivity to changing aerosol. The magnitude of the rate of change of CDN with particle number, a measure of the aerosol efficacy, varies by a factor 4. CDN in cloud processed regions of persistent stratocumulus is particularly sensitive to changing aerosol number. It is therefore likely that the indirect effect will be underestimated in these important regions.

  16. The relationship between aerosol and cloud drop number concentrations in a global aerosol microphysics model

    Directory of Open Access Journals (Sweden)

    K. J. Pringle

    2009-06-01

    Full Text Available Empirical relationships that link cloud droplet number (CDN to aerosol number or mass are commonly used to calculate global fields of CDN for climate forcing assessments. In this work we use a sectional global model of sulfate and sea-salt aerosol coupled to a mechanistic aerosol activation scheme to explore the limitations of this approach. We find that a given aerosol number concentration produces a wide range of CDN concentrations due to variations in the shape of the aerosol size distribution. On a global scale, the dependence of CDN on the size distribution results in regional biases in predicted CDN (for a given aerosol number. Empirical relationships between aerosol number and CDN are often derived from regional data but applied to the entire globe. In an analogous process, we derive regional "correlation-relations" between aerosol number and CDN and apply these regional relations to calculations of CDN on the global scale. The global mean percentage error in CDN caused by using regionally derived CDN-aerosol relations is 20 to 26%, which is about half the global mean percentage change in CDN caused by doubling the updraft velocity. However, the error is as much as 25–75% in the Southern Ocean, the Arctic and regions of persistent stratocumulus when an aerosol-CDN correlation relation from the North Atlantic is used. These regions produce much higher CDN concentrations (for a given aerosol number than predicted by the globally uniform empirical relations. CDN-aerosol number relations from different regions also show very different sensitivity to changing aerosol. The magnitude of the rate of change of CDN with particle number, a measure of the aerosol efficacy, varies by a factor 4. CDN in cloud processed regions of persistent stratocumulus is particularly sensitive to changing aerosol number. It is therefore likely that the indirect effect will be underestimated in these important regions.

  17. Ferrous Sulfate (Iron)

    Science.gov (United States)

    Ferrous sulfate provides the iron needed by the body to produce red blood cells. It is used ... Ferrous sulfate comes as regular, coated, and extended-release (long-acting) tablets; regular and extended-release capsules; ...

  18. Possible connection between large volcanic eruptions and level rise episodes in the Dead Sea Basin

    Science.gov (United States)

    Bookman, R.; Filin, S.; Avni, Y.; Rosenfeld, D.; Marco, S.

    2014-12-01

    The June 1991 Pinatubo volcanic eruption perturbed the atmosphere, triggering short-term worldwide changes in climate. The following winter was anomalously wet in the Levant, with a ~2-meter increase in the Dead Sea level that created a morphological terrace along the lake's shore. Given the global effects of volcanogenic aerosols, we tested the hypothesis that the 1991-92 shore terrace is a modern analogue to the linkage between past volcanic eruptions and a sequence of shore terraces in the Dead Sea Basin. Analysis of precipitation series from Jerusalem showed a significant positive correlation between the Dust Veil Index (DVI) of the modern eruptions and annual rainfall. The DVI was found to explain nearly 50% of the variability in the annual rainfall, such that greater DVI means more rainfall. Other factors that may affect the annual rainfall in the region as the Southern Oscillation Index (SOI) and the North Atlantic oscillations (NAO) were incorporated along with the DVI in a linear multiple regression model. It was found that the NAO did not contribute anything except for increased noise, but the added SOI increased the explained variability of rainfall to more than 60%. Volcanic eruptions with a VEI of 6, as in the Pinatubo, occurred about once a century during the Holocene and the last glacial-interglacial cycle. This occurrence is similar to the frequency of shore terrace build-up during the Lake Lisan desiccation. Sixteen shore terraces, detected using airborne laser scanning data, were interpreted as indicating short-term level rises due to episodes of enhanced precipitation and runoff during the dramatic drop in Lake Lisan's (palaeo-Dead Sea) level at the end of the LGM. The terraces were compared with a time series of volcanogenic sulfate from the GISP2 record, and similar numbers of sulfate concentration peaks and terraces were found. Furthermore, a significant correlation was found between SO4 concentration peaks and the terraces heights. This

  19. A possible pathway for rapid growth of sulfate during haze days in China

    Science.gov (United States)

    Li, Guohui; Bei, Naifang; Cao, Junji; Huang, Rujin; Wu, Jiarui; Feng, Tian; Wang, Yichen; Liu, Suixin; Zhang, Qiang; Tie, Xuexi; Molina, Luisa T.

    2017-03-01

    Rapid industrialization and urbanization have caused frequent occurrence of haze in China during wintertime in recent years. The sulfate aerosol is one of the most important components of fine particles (PM2. 5) in the atmosphere, contributing significantly to the haze formation. However, the heterogeneous formation mechanism of sulfate remains poorly characterized. The relationships of the observed sulfate with PM2. 5, iron, and relative humidity in Xi'an, China have been employed to evaluate the mechanism and to develop a parameterization of the sulfate heterogeneous formation involving aerosol water for incorporation into atmospheric chemical transport models. Model simulations with the proposed parameterization can successfully reproduce the observed sulfate rapid growth and diurnal variations in Xi'an and Beijing, China. Reasonable representation of sulfate heterogeneous formation in chemical transport models considerably improves the PM2. 5 simulations, providing the underlying basis for better understanding the haze formation and supporting the design and implementation of emission control strategies.

  20. Photochemical organonitrate formation in wet aerosols

    Science.gov (United States)

    Lim, Yong Bin; Kim, Hwajin; Kim, Jin Young; Turpin, Barbara J.

    2016-10-01

    Water is the most abundant component of atmospheric fine aerosol. However, despite rapid progress, multiphase chemistry involving wet aerosols is still poorly understood. In this work, we report results from smog chamber photooxidation of glyoxal- and OH-containing ammonium sulfate or sulfuric acid particles in the presence of NOx and O3 at high and low relative humidity. Particles were analyzed using ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). During the 3 h irradiation, OH oxidation products of glyoxal that are also produced in dilute aqueous solutions (e.g., oxalic acids and tartaric acids) were formed in both ammonium sulfate (AS) aerosols and sulfuric acid (SA) aerosols. However, the major products were organonitrogens (CHNO), organosulfates (CHOS), and organonitrogen sulfates (CHNOS). These were also the dominant products formed in the dark chamber, indicating non-radical formation. In the humid chamber (> 70 % relative humidity, RH), two main products for both AS and SA aerosols were organonitrates, which appeared at m / z- 147 and 226. They were formed in the aqueous phase via non-radical reactions of glyoxal and nitric acid, and their formation was enhanced by photochemistry because of the photochemical formation of nitric acid via reactions of peroxy radicals, NOx and OH during the irradiation.

  1. Sulfur isotope analyses of individual aerosol particles in the urban aerosol at a central European site (Mainz, Germany

    Directory of Open Access Journals (Sweden)

    B. Winterholler

    2008-05-01

    Full Text Available Sulfur isotope analysis of atmospheric aerosols is a well established tool for identifying sources of sulfur in the atmosphere, estimating emission factors, and tracing the spread of sulfur from anthropogenic sources through ecosystems. Conventional gas mass spectrometry averages the isotopic compositions of several different types of sulfur aerosol particles, and therefore masks the individual isotopic signatures. In contrast, the new single particle technique presented here determines the isotopic signature of the individual particles.

    Primary aerosol particles retain the original isotopic signature of their source. The isotopic composition of secondary sulfates depends on the isotopic composition of precursor SO2 and the oxidation process. The fractionation with respect to the source SO2 is −9‰ for homogeneous and +16.5‰ for heterogeneous oxidation. The sulfur isotope ratio of secondary sulfate particles can therefore be used to identify the oxidation pathway by which this sulfate was formed. With the new single particle technique, different types of primary and secondary sulfates were first identified based on their chemical composition, and then their individual isotopic signature was measured separately. Our samples were collected in Mainz, Germany, in an urban environment. Secondary sulfates (ammonium sulfate, gypsum, mixed sulfates and coatings on silicates or organic aerosol dominated sulfate loadings in our samples. Comparison of the chemical and isotopic composition of secondary sulfates showed that the isotopic composition was homogeneous, independent of the chemical composition. This is typical for particles that derive from in-cloud processing. The isotopic composition of the source SO2 of secondary sulfates was calculated based on the isotopic composition of particles with known oxidation pathway and showed a strong dependence on wind direction. The contribution of heterogeneous

  2. Acid fog Deposition of Crusts on Basaltic Tephra Deposits in the Sand Wash Region of Kilauea Volcano: A Possible Mechanism for Siliceous-Sulfatic Crusts on Mars

    Science.gov (United States)

    Schiffman, P.; Zierenberg, R.; Marks, N.; Bishop, J. L.

    2004-12-01

    Although the presence of sulfate minerals in martian outcrops may imply the prior existence of standing bodies of surface water, in terrestrial volcanic settings, sulfatic alteration may also occur above the water table within the vadose zone. On the summit of Kilauea volcano, sulfur dioxide, which is continuously emitted from Halemaumau crater and rapidly sequestered into sulfuric acid-rich aerosol entrained in the prevailing trade winds, is subsequently precipitated as acid-fog immediately downwind from the caldera in the Kau Desert. The characteristic pH of surface tephra deposits is < 4.0 in Sand Wash, a region of continuous, acidic aerosol fall-out immediately SW of the caldera. The upper portion of the Keanakakoi Ash tephra in Sand Wash, deposited in the late 18th century, has a ubiquitous, 0.1-0.2 mm-thick coating of amorphous silica. Conversely, vertical walls of unconsolidated tephra, exposed within small, dry gullies eroded into the ca. 3-4 m-thick Keanakakoi section at Sand Wash, are coated with ca. 0.5-1.0 mm-thick, mixed amorphous silica and jarosite-bearing crusts. Since these crusts are denuded from their outcrops during ephemeral, but probably annual flooding events in Sand Wash, we believe that they must accumulate rapidly. These crusts are apparently formed via an evaporative mechanism whereby acidic pore fluids, circulating in the upper few m's within the highly porous tephra, are wicked towards the walls of the gullies. Geochemical modeling of the crust-forming process implies that the sulfate formation via evaporation occurs subsequent to minimal interaction of acidic pore fluids with the basaltic tephra. This also suggests that the cycle from acid-fog fall-out to precipitation of the siliceous-sulfatic crusts must occur quite rapidly. Production of siliceous-sulfatic crusts via acid-fog alteration may also be occurring on Mars. The occurrence of evaporitic sulfate and silica at Sand Wash in Kilauea may serve as an example of how the jarosite

  3. Photophoretic levitation of engineered aerosols for geoengineering

    Science.gov (United States)

    Keith, David W.

    2010-01-01

    Aerosols could be injected into the upper atmosphere to engineer the climate by scattering incident sunlight so as to produce a cooling tendency that may mitigate the risks posed by the accumulation of greenhouse gases. Analysis of climate engineering has focused on sulfate aerosols. Here I examine the possibility that engineered nanoparticles could exploit photophoretic forces, enabling more control over particle distribution and lifetime than is possible with sulfates, perhaps allowing climate engineering to be accomplished with fewer side effects. The use of electrostatic or magnetic materials enables a class of photophoretic forces not found in nature. Photophoretic levitation could loft particles above the stratosphere, reducing their capacity to interfere with ozone chemistry; and, by increasing particle lifetimes, it would reduce the need for continual replenishment of the aerosol. Moreover, particles might be engineered to drift poleward enabling albedo modification to be tailored to counter polar warming while minimizing the impact on equatorial climates. PMID:20823254

  4. Photophoretic levitation of engineered aerosols for geoengineering.

    Science.gov (United States)

    Keith, David W

    2010-09-21

    Aerosols could be injected into the upper atmosphere to engineer the climate by scattering incident sunlight so as to produce a cooling tendency that may mitigate the risks posed by the accumulation of greenhouse gases. Analysis of climate engineering has focused on sulfate aerosols. Here I examine the possibility that engineered nanoparticles could exploit photophoretic forces, enabling more control over particle distribution and lifetime than is possible with sulfates, perhaps allowing climate engineering to be accomplished with fewer side effects. The use of electrostatic or magnetic materials enables a class of photophoretic forces not found in nature. Photophoretic levitation could loft particles above the stratosphere, reducing their capacity to interfere with ozone chemistry; and, by increasing particle lifetimes, it would reduce the need for continual replenishment of the aerosol. Moreover, particles might be engineered to drift poleward enabling albedo modification to be tailored to counter polar warming while minimizing the impact on equatorial climates.

  5. Global modeling of nitrate and ammonium aerosols using EQSAM3

    Science.gov (United States)

    Xu, L.; Penner, J. E.

    2009-12-01

    Atmospheric aerosols, particles suspending in air, are important as they affect human health, air quality, and visibility as well as climate. Sulfate, nitrate, ammonium, chloride and sodium are among the most important inorganic aerosol species in the atmosphere. These compounds are hygroscopic and absorb water under almost all ambient environmental conditions. The uptake of water alters the aerosol size, and causes water to become the constituent with the largest atmospheric aerosol mass, especially when the aerosols grow into fog, haze or clouds. Furthermore, several global model studies have demonstrated that rapid increases in nitrogen emissions could produce enough nitrate in aerosols to offset the expected decline in sulfate forcing by 2100 for the extreme IPCC A2 scenario (Bauer et al., 2007). Although nitrate and ammonium were identified as significant anthropogenic sources of aerosols by a number of modeling studies, most global aerosol models still exclude ammonium-nitrate when the direct aerosol forcing is studied. In this study, the computationally efficient equilibrium model, EQSAM3, is incorporated into the UMICH-IMPACT-nitrate model using the hybrid dynamical solution method (Feng and Penner, 2007). The partitioning of nitrate and ammonium along with the corresponding water uptake is evaluated by comparing the model to the EQUISOLVE II method used in Feng and Penner (2007). The model is also evaluated by comparison with the AERONET data base and satellite-based aerosol optical depths.

  6. Nanoscale surface modification of Mt. Etna volcanic ashes

    Science.gov (United States)

    Barone, G.; Mazzoleni, P.; Corsaro, R. A.; Costagliola, P.; Di Benedetto, F.; Ciliberto, E.; Gimeno, D.; Bongiorno, C.; Spinella, C.

    2016-02-01

    Ashes emitted during volcanic explosive activity present peculiar surface chemical and mineralogical features related in literature to the interaction in the plume of solid particles with gases and aerosols. The compositional differences of magmas and gases, the magnitude, intensity and duration of the emission and the physical condition during the eruption, strongly influence the results of the modification processes. Here we report the characterization of the products emitted during the 2013 paroxysmal activity of Mt. Etna. The surface features of the ash particles were investigated through X-ray photoelectron spectroscopy (XPS) and Transmission electron microscopy (TEM) allowing the analysis at nanometer scale. TEM images showed on the surface the presence of composite structures formed by Ca, Mg and Na sulphates and halides and of droplets and crystals of chlorides; nanometric magnesioferrite and metallic iron dendrites are observable directly below the surface. From the chemical point of view, the most external layer of the volcanic glassy particles (XPS, presents depletion in Si, Mg, Ca, Na and K and strong enrichment in volatile elements especially F and S, with respect to the inner zone, which represents the unaltered counterpart. Below this external layer, a transition glassy shell (thick 50-100 nm) is characterized by Fe, Mg and Ca enrichments with respect to the inner zone. We propose that the ash particle surface composition is the result of a sequence of events which start at shallow depth, above the exsolution surface, where gas bubbles nucleate and the interfaces between bubbles and melt represent proto-surfaces of future ash particles. Enrichment of Ca, Mg and Fe and halides may be due to the early partition of F and Cl in the gas phase and their interaction with the melt layer located close to the bubbles. Furthermore the formation of volatile SiF4 and KF explain the observed depletion of Si and K. The F enrichment in the external ∼50 nm thick

  7. Impact of volcanic eruptions on the climate of the 1st millennium AD in a comprehensive climate simulation

    Science.gov (United States)

    Wagner, Sebastian; Zorita, Eduardo

    2015-04-01

    The climate of the 1st millennium AD shows some remarkable differences compared to the last millennium concerning variation in external forcings. Together with an orbitally induced increased solar insolation during the northern hemisphere summer season and a general lack of strong solar minima, the frequency and intensity of large tropical and extratropical eruptions is decreased. Here we present results of a new climate simulation carried out with the comprehensive Earth System Model MPI-ESM-P forced with variations in orbital, solar, volcanic and greenhouse gas variations and land use changes for the last 2,100 years. The atmospheric model has a horizontal resolution of T63 (approx. 125x125 km) and therefore also allows investigations of regional-to-continental scale climatic phenomena. The volcanic forcing was reconstructed based on a publication by Sigl et al. (2013) using the sulfate records of the NEEM and WAIS ice cores. To obtain information on the aerosol optical depth (AOD) these sulfate records were scaled to an established reconstruction from Crowley and Unterman (2010), which is also a standard forcing in the framework of CMIP5/PMIP3. A comparison between the newly created data set with the Crowley and Unterman dataset reveals that the new reconstruction shows in general weaker intensities, especially of the large tropical outbreaks and fewer northern hemispheric small-to-medium scale eruptions. However, the general pattern in the overlapping period is similar. A hypothesis that can be tested with the simulation is whether the reduced volcanic intensity of the 1st millennium AD contributed to the elevated temperature levels over Europe, evident within a new proxy-based reconstruction. On the other hand, the few but large volcanic eruptions, e.g. the 528 AD event, also induced negative decadal-scale temperature anomalies. Another interesting result of the simulation relates to the 79 AD eruption of the Vesuvius, which caused the collapse of the city of

  8. Application of the VH-TDMA technique to coastal ambient aerosols

    Science.gov (United States)

    Johnson, G.; Ristovski, Z.; Morawska, L.

    2004-08-01

    A newly developed VH-TDMA has been used for the first time to measure the volatile fractions and post volatilization hygroscopic growth factors of ambient aerosols in the coastal marine and urban environments. The results are compared with comparable data for laboratory generated aerosols of known composition. Measurements conducted on coastal Aitken mode particles showed volatilization behavior similar to laboratory generated aerosols composed of methane sulfonic acid and ammonium sulfate. Measurements conducted on 60 nm particles during nucleation events contained a greater fraction of material with similar volatility to ammonium sulfate than was found at other times. These particles were hygroscopic but less so than pure ammonium sulfate. Measurements conducted in the Brisbane central business district during sea breeze conditions show similar behavior to the coastal aerosol, but with additional low volatility species. This aerosol may originate from urban sources or from marine particles acquiring additional secondary aerosol species during transport.

  9. Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2010-05-01

    Full Text Available Aged organic aerosol (OA was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008, which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM1, and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM1 sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM1 such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×1011 molecules cm−3 s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.

  10. Aged organic aerosol in the Eastern Mediterranean: the Finokalia aerosol measurement experiment-2008

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2010-01-01

    Full Text Available Aged organic aerosol (OA was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008, which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM1, and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM1 sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM1 such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with time of day, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×1011 molecules cm−3 s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.

  11. Pacific trade winds accelerated by aerosol forcing over the past two decades

    Science.gov (United States)

    Takahashi, Chiharu; Watanabe, Masahiro

    2016-08-01

    The Pacific trade winds, coupled with the zonal sea surface temperature gradient in the equatorial Pacific Ocean, control regional sea levels, and therefore their trend is a great concern in the Pacific Rim. Over the past two decades, easterly winds have been accelerated in association with eastern tropical Pacific cooling. They may represent natural interdecadal variability in the Pacific and possibly explain the recent global warming hiatus. However, the intensification of the winds has been the strongest ever observed in the past century, the reason for which is still unclear. Here we show, using multiple climate simulations for 1921-2014 by a global climate model, that approximately one-third of the trade-wind intensification for 1991-2010 can be attributed to changes in sulfate aerosols. The multidecadal sea surface temperature anomaly induced mostly by volcanic aerosols dominates in the western North Pacific, and its sign changed rapidly from negative to positive in the 1990s, coherently with Atlantic multidecadal variability. The western North Pacific warming resulted in intensification of trade winds to the west of the dateline. These trends have not contributed much to the global warming hiatus, but have greatly impacted rainfall over the western Pacific islands.

  12. eVolv2k: A new ice core-based volcanic forcing reconstruction for the past 2000 years

    Science.gov (United States)

    Toohey, Matthew; Sigl, Michael

    2016-04-01

    Radiative forcing resulting from stratospheric aerosols produced by major volcanic eruptions is a dominant driver of climate variability in the Earth's past. The ability of climate model simulations to accurately recreate past climate is tied directly to the accuracy of the volcanic forcing timeseries used in the simulations. We present here a new volcanic forcing reconstruction, based on newly updated ice core composites from Antarctica and Greenland. Ice core records are translated into stratospheric aerosol properties for use in climate models through the Easy Volcanic Aerosol (EVA) module, which provides an analytic representation of volcanic stratospheric aerosol forcing based on available observations and aerosol model results, prescribing the aerosol's radiative properties and primary modes of spatial and temporal variability. The evolv2k volcanic forcing dataset covers the past 2000 years, and has been provided for use in the Paleo-Modeling Intercomparison Project (PMIP), and VolMIP experiments within CMIP6. Here, we describe the construction of the eVolv2k data set, compare with prior forcing sets, and show initial simulation results.

  13. Post-flame gas-phase sulfation of potassium chloride

    DEFF Research Database (Denmark)

    Li, Bo; Sun, Zhiwei; Li, Zhongshan;

    2013-01-01

    homogeneous systems are required to characterize the gas-phase formation of alkali sulfates. We have measured the temperature and gas-phase concentrations of KCl and HCl, and detected the presence of aerosols in the post-flame region of a range of hydrocarbon flames seeded with KCl, with and without......The sulfation of KCl during biomass combustion has implications for operation and emissions: it reduces the rates of deposition and corrosion, it increases the formation of aerosols, and it leads to higher concentrations of HCl and lower concentrations of SO2 in the gas phase. Rigorously...... the addition of SO2. Dilution of the flame products with different amounts of N2 ensured post-flame temperatures in the range 950–1400K. In the absence of SO2, KCl levels were constant in the post-flame zone and no aerosols were formed, even at the lowest temperatures. In the presence of SO2, KCl was consumed...

  14. The Impact of Aerosol Direct and Indirect Effects on Climate

    Science.gov (United States)

    Schwarzkopf, M. D.; Levy, H.; Horowitz, L. W.; Ming, Y.; Golaz, J.; Naik, V.; Ramaswamy, V.

    2012-12-01

    We employ GFDL's new fully-coupled chemistry-climate (ocean/atmosphere/land/sea ice) model (CM3) with an explicit physical representation of aerosol indirect effects (cloud-water droplet activation) to find a global-averaged cooling of ~1K due to aerosol forcing in the historical (1860-2005) period, and that the aerosol indirect effect accounts for almost all of this cooling. In the 21st Century, employing the RCP 4.5 scenario, with projected reductions in emissions of anthropogenic aerosols and their precursors, we find ~1 K of additional warming and 0.1 mm/day of additional precipitation, both globally averaged, by the end of the 21st Century, compared with a simulation in which aerosol and precursor emissions are fixed at 2005 values. The impact of these projected reductions in aerosol emissions on simulated globally averaged surface temperature and precipitation becomes apparent by ~ 2050. The reduction in aerosols increases precipitation in East and South Asia by as much as 0.5-1.0 mm/day in the latter part of the 21st Century. The simulated temperature and precipitation responses in CM3 are significantly stronger than the previously simulated responses in our earlier climate model (CM2.1) that only considered direct radiative forcing by aerosols. We conclude that sulfate aerosol indirect effects greatly enhance the impacts of aerosols on surface temperature in CM3, while both sulfate aerosol indirect effects and BC aerosol absorption contribute to a strong precipitation response. CM3 produces late 21st Century surface warming patterns that are uncorrelated with the spatial distribution of the changes in aerosol loading, a result similar to CM2.1. However, unlike temperature, the largest precipitation increases and aerosol decreases in CM3 are co-located in and downwind of Asia.

  15. Aerosolized Antibiotics.

    Science.gov (United States)

    Restrepo, Marcos I; Keyt, Holly; Reyes, Luis F

    2015-06-01

    Administration of medications via aerosolization is potentially an ideal strategy to treat airway diseases. This delivery method ensures high concentrations of the medication in the targeted tissues, the airways, with generally lower systemic absorption and systemic adverse effects. Aerosolized antibiotics have been tested as treatment for bacterial infections in patients with cystic fibrosis (CF), non-CF bronchiectasis (NCFB), and ventilator-associated pneumonia (VAP). The most successful application of this to date is treatment of infections in patients with CF. It has been hypothesized that similar success would be seen in NCFB and in difficult-to-treat hospital-acquired infections such as VAP. This review summarizes the available evidence supporting the use of aerosolized antibiotics and addresses the specific considerations that clinicians should recognize when prescribing an aerosolized antibiotic for patients with CF, NCFB, and VAP.

  16. Sensitivity of direct climate forcing by atmospheric aerosols to aerosol size and composition

    Science.gov (United States)

    Pilinis, Christodoulos; Pandis, Spyros N.; Seinfeld, John H.

    1995-09-01

    significant even for single scatter albedo values of ω=0.93-0.97. The absorbing aerosol component reduces the aerosol forcing from that in its absence by roughly 30% at 60% RH and 20% at 90% RH. The mixing state of the aerosol (internal versus external) for the particular aerosol considered here is found to be of secondary importance. While sulfate mass scattering efficiency (m2 (g SO42-)-1) and the normalized sulfate forcing (W (g SO42-)-1) increase strongly with RH, total mass scattering efficiency (m2 g-1) and normalized forcing (W g-1) are relatively insensitive to RH, wherein the mass of all species, including water, are accounted for. Following S. Nemesure et al. (Direct shortwave forcing of climate by anthropogenic sulfate aerosol: sensitivity to particle size, composition, and relative humidity, submitted to Journal of Geophysical Research, 1995), we find that aerosol feeing achieves a maximum at a particular solar zenith angle, reflecting a balance between increasing upscatter fraction with increasing solar zenith angle and decreasing solar flux (from Rayleigh scattering) with increasing solar zenith angle.

  17. An independently dated 2000-yr volcanic record from Law Dome, East Antarctica, including a new perspective on the dating of the c. 1450s eruption of Kuwae, Vanuatu

    Directory of Open Access Journals (Sweden)

    C. T. Plummer

    2012-05-01

    Full Text Available Volcanic eruptions are an important cause of natural climate variability. In order to improve the accuracy of climate models, precise dating and magnitude of the climatic effects of past volcanism are necessary. Here we present a 2000-yr record of Southern Hemisphere volcanism recorded in ice cores from the high accumulation Law Dome site, East Antarctica. The ice cores were analyzed for a suite of chemistry signals and are independently dated via annual layer counting, with 11 ambiguous years by the end of the record. Independently dated records are important to avoid circular dating where volcanic signatures are assigned a date from some external information rather than using the date it is found in the ice core. Forty-five volcanic events have been identified using the sulfate chemistry of the Law Dome record. Comparisons between Law Dome and NGRIP (Greenland volcanic records suggest Law Dome is the most accurately dated Antarctic volcanic dataset and allows for the records to be synchronized with NGRIP, leading to an improved global volcanic forcing dataset. Volcanic sulfate deposition estimates are important for modeling the climatic response to eruptions. The largest volcanic sulfate events in our record are dated at 1458 CE (Kuwae, Vanuatu, 1257 and 423 CE (unidentified. Using our record we refine the dating of previously known volcanic events and present evidence for two separate eruptions during the period 1450–1460 CE, potentially causing confusion in the assignment of the Kuwae (Vanuatu eruption to volcanic signatures during this time interval.

  18. A missing source of aerosols in Antarctica - beyond long-range transport, phytoplankton, and photochemistry

    Science.gov (United States)

    Giordano, Michael R.; Kalnajs, Lars E.; Avery, Anita; Goetz, J. Douglas; Davis, Sean M.; DeCarlo, Peter F.

    2017-01-01

    Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS - soot particle aerosol mass spectrometer - or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition

  19. Link of volcanic activity and climate change in Altai studied in the ice core from Belukha Mountain

    Directory of Open Access Journals (Sweden)

    N. S. Malygina

    2013-01-01

    Full Text Available In the present research we discuss a role of volcanic activity in Altai thermal regime. Here we analyses the sulfate and temperature data reconstructed from the natural paleoarchive – ice core from the Belukha Mountain saddle. Sulfate ice-core reconstructions can serve as volcanic markers. The both – sulfate and temperature reconstructions – are for the last 750 years. As the characteristic of volcanic activity we consider Volcanic Explosivity Index (VEI, Dust Veil Index (DVI and Ice core volcanic index (IVI. The analysis was done using wavelet analysis and analysis of wavelet cross coherence and phase. As the result, we conclude that observed increases in the values of the indexes VEI, DVI, IVI basically correspond to decreases of temperature and increases of sulfate concentrations. This confirms the dependence of changes in the thermal regime of the Altai from volcanic activity. But in the 1750–1850 years period there is a delay of the changes in temperature with respect to the changes in volcanic activity. We suggest that it can be due to the superposition of the influence of solar and volcanic activity on changes in the thermal regime of Altai.

  20. Real Time Volcanic Cloud Products and Predictions for Aviation Alerts

    Science.gov (United States)

    Krotkov, Nickolay A.; Habib, Shahid; da Silva, Arlindo; Hughes, Eric; Yang, Kai; Brentzel, Kelvin; Seftor, Colin; Li, Jason Y.; Schneider, David; Guffanti, Marianne; Hoffman, Robert L.; Myers, Tim; Tamminen, Johanna; Hassinen, Seppo

    2014-01-01

    Volcanic eruptions can inject significant amounts of sulfur dioxide (SO2) and volcanic ash into the atmosphere, posing a substantial risk to aviation safety. Ingesting near-real time and Direct Readout satellite volcanic cloud data is vital for improving reliability of volcanic ash forecasts and mitigating the effects of volcanic eruptions on aviation and the economy. NASA volcanic products from the Ozone Monitoring Insrument (OMI) aboard the Aura satellite have been incorporated into Decision Support Systems of many operational agencies. With the Aura mission approaching its 10th anniversary, there is an urgent need to replace OMI data with those from the next generation operational NASA/NOAA Suomi National Polar Partnership (SNPP) satellite. The data provided from these instruments are being incorporated into forecasting models to provide quantitative ash forecasts for air traffic management. This study demonstrates the feasibility of the volcanic near-real time and Direct Readout data products from the new Ozone Monitoring and Profiling Suite (OMPS) ultraviolet sensor onboard SNPP for monitoring and forecasting volcanic clouds. The transition of NASA data production to our operational partners is outlined. Satellite observations are used to constrain volcanic cloud simulations and improve estimates of eruption parameters, resulting in more accurate forecasts. This is demonstrated for the 2012 eruption of Copahue. Volcanic eruptions are modeled using the Goddard Earth Observing System, Version 5 (GEOS-5) and the Goddard Chemistry Aerosol and Radiation Transport (GOCART) model. A hindcast of the disruptive eruption from Iceland's Eyjafjallajokull is used to estimate aviation re-routing costs using Metron Aviation's ATM Tools.

  1. The Role of Volcanic Activity in Climate and Global Change

    KAUST Repository

    Stenchikov, Georgiy L.

    2015-09-23

    Explosive volcanic eruptions are magnificent events that in many ways affect the Earth\\'s natural processes and climate. They cause sporadic perturbations of the planet\\'s energy balance, activating complex climate feedbacks and providing unique opportunities to better quantify those processes. We know that explosive eruptions cause cooling in the atmosphere for a few years, but we have just recently realized that volcanic signals can be seen in the subsurface ocean for decades. The volcanic forcing of the previous two centuries offsets the ocean heat uptake and diminishes global warming by about 30%. The explosive volcanism of the twenty-first century is unlikely to either cause any significant climate signal or to delay the pace of global warming. The recent interest in dynamic, microphysical, chemical, and climate impacts of volcanic eruptions is also excited by the fact that these impacts provide a natural analogue for climate geoengineering schemes involving deliberate development of an artificial aerosol layer in the lower stratosphere to counteract global warming. In this chapter we aim to discuss these recently discovered volcanic effects and specifically pay attention to how we can learn about the hidden Earth-system mechanisms activated by explosive volcanic eruptions. To demonstrate these effects we use our own model results when possible along with available observations, as well as review closely related recent publications.

  2. Persistent sulfate formation from London Fog to Chinese haze

    Science.gov (United States)

    Wang, Gehui; Zhang, Renyi; Gomez, Mario E.; Yang, Lingxiao; Levy Zamora, Misti; Hu, Min; Lin, Yun; Peng, Jianfei; Guo, Song; Meng, Jingjing; Li, Jianjun; Cheng, Chunlei; Hu, Tafeng; Ren, Yanqin; Wang, Yuesi; Gao, Jian; Cao, Junji; An, Zhisheng; Zhou, Weijian; Li, Guohui; Wang, Jiayuan; Tian, Pengfei; Marrero-Ortiz, Wilmarie; Secrest, Jeremiah; Du, Zhuofei; Zheng, Jing; Shang, Dongjie; Zeng, Limin; Shao, Min; Wang, Weigang; Huang, Yao; Wang, Yuan; Zhu, Yujiao; Li, Yixin; Hu, Jiaxi; Pan, Bowen; Cai, Li; Cheng, Yuting; Ji, Yuemeng; Zhang, Fang; Rosenfeld, Daniel; Liss, Peter S.; Duce, Robert A.; Kolb, Charles E.; Molina, Mario J.

    2016-11-01

    Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO2 by NO2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH3 neutralization or under cloud conditions. Under polluted environments, this SO2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH3 and NO2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world.

  3. Linkages between ozone depleting substances, tropospheric oxidation and aerosols

    Directory of Open Access Journals (Sweden)

    A. Voulgarakis

    2012-09-01

    Full Text Available Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric Ozone Depleting Substances (ODS on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O emissions. We also find that without the regulation of chlorofluorocarbons (CFCs through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The historical radiative forcing of CFCs through their indirect effects on methane (−22.6 mW m−2 and sulfate aerosols (−3.0 mW m−2 discussed here is non-negligible when compared to known historical CFC forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

  4. Impact of major volcanic eruptions on stratospheric water vapour

    Science.gov (United States)

    Löffler, Michael; Brinkop, Sabine; Jöckel, Patrick

    2016-05-01

    Volcanic eruptions can have a significant impact on the Earth's weather and climate system. Besides the subsequent tropospheric changes, the stratosphere is also influenced by large eruptions. Here changes in stratospheric water vapour after the two major volcanic eruptions of El Chichón in Mexico in 1982 and Mount Pinatubo on the Philippines in 1991 are investigated with chemistry-climate model simulations. This study is based on two simulations with specified dynamics of the European Centre for Medium-Range Weather Forecasts Hamburg - Modular Earth Submodel System (ECHAM/MESSy) Atmospheric Chemistry (EMAC) model, performed within the Earth System Chemistry integrated Modelling (ESCiMo) project, of which only one includes the long-wave volcanic forcing through prescribed aerosol optical properties. The results show a significant increase in stratospheric water vapour induced by the eruptions, resulting from increased heating rates and the subsequent changes in stratospheric and tropopause temperatures in the tropics. The tropical vertical advection and the South Asian summer monsoon are identified as sources for the additional water vapour in the stratosphere. Additionally, volcanic influences on tropospheric water vapour and El Niño-Southern Oscillation (ENSO) are evident, if the long-wave forcing is strong enough. Our results are corroborated by additional sensitivity simulations of the Mount Pinatubo period with reduced nudging and reduced volcanic aerosol extinction.

  5. Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

    Science.gov (United States)

    Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

    2015-06-01

    Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

  6. Relative impact of climate indicators and aerosols on tropical cyclones

    Science.gov (United States)

    Chiacchio, Marc; Pausata, Francesco; Messori, Gabriele; Hannachi, Abdel; Chin, Mian; Ekman, Annica; Barrie, Leonard

    2015-04-01

    This study assesses the most important environmental variables modulating tropical cyclone (TC) frequency in six different oceanic basins such as the East Pacific, West Pacific, North Atlantic, North Indian Ocean, South Indian Ocean, and South Pacific. To determine their influence, we used multiple linear regression between TC frequency and variations in meteorological variables and circulation indices as well as aerosol optical depth (AOD) anomalies over the tropical cyclone development areas for the period 1980-2009 (where the AOD was separated into the compounds black and organic carbon, sulfate dust and sea salt). Overall the low-level relative humidity in the North Atlantic, stratospheric aerosol burden in the East Pacific, and the black carbon burden in the North Indian basin showed the greatest relation with TC activity and were all with statistically significant and explained variances of 28%. Amongst the circulation modes of variability, the Atlantic Multidecadal Oscillation (AMO) and the El Nino Southern Oscillation (ENSO) appeared to be most important to TC activity with significant variances of 29% in the South Indian Ocean and 25% in the East Pacific basins, respectively. We also examined the inter-basin relationship between the different environmental variables in one basin and the cyclone frequency in another basin. Overall the strongest connections were found between North Atlantic basin variables and North Indian TCs while the weakest links were found between West Pacific basin variables and South Pacific TCs. Lastly, because the strongest cooling of the lower stratospheric temperature was found over the North Atlantic since the last few decades and because the cooling could explain a variance of 15% of TC frequency in that same basin, we investigated five global climate models from the historical runs of the CMIP5 archive to determine whether they were able to capture this cooling in the lower stratosphere. Although the models were able to

  7. Tyrosine Sulfation of Statherin

    Directory of Open Access Journals (Sweden)

    C. Kasinathan, N. Gandhi, P. Ramaprasad, P. Sundaram, N. Ramasubbu

    2007-01-01

    Full Text Available Tyrosylprotein sulfotransferase (TPST, responsible for the sulfation of a variety of secretory and membrane proteins, has been identified and characterized in submandibular salivary glands (William et al. Arch Biochem Biophys 1997; 338: 90-96. In the present study we demonstrate the sulfation of a salivary secretory protein, statherin, by the tyrosylprotein sulfotransferase present in human saliva. Optimum statherin sulfation was observed at pH 6.5 and at 20 mm MnCl2. Increase in the level of total sulfation was observed with increasing statherin concentration. The Km value of tyrosylprotein sulfotransferase for statherin was 40 μM. Analysis of the sulfated statherin product on SDS-polyacrylamide gel electrophoresis followed by autoradiography revealed 35S-labelling of a 5 kDa statherin. Further analysis of the sulfated statherin revealed the sulfation on tyrosyl residue. This study is the first report demonstrating tyrosine sulfation of a salivary secretory protein. The implications of this sulfation of statherin in hydroxyapatite binding and Actinomyces viscosus interactions are discussed.

  8. The ice-core record of volcanism: Status and future directions

    Science.gov (United States)

    Sigl, Michael; McConnell, Joseph R.; Chellman, Nathan; Ludlow, Francis; Curran, Mark; Plunkett, Gill; Büntgen, Ulf; Toohey, Matthew; Burke, Andrea; Grieman, Mackenzie

    2016-04-01

    Radiative forcing resulting from stratospheric aerosols produced by major volcanic eruptions is a dominant driver of climate variability in the Earth's past. Accurate knowledge of the climate anomalies resulting from volcanic eruptions provides important information for understanding the global and regional responses of the Earth system to external forcing agents. Based on a unique compilation of newly obtained, high-resolution, ice-core measurements, as well as palaeo-climatic evidence inferred from existing tree-ring records and historical documentary sources, we revised the dating of ice-core based reconstructions of past volcanic eruptions and confirmed the dominant role of explosive volcanism on short-term summer temperature variability throughout the past 2,500 years. Continuous weekly surface snow measurements obtained from Summit, Greenland (2005-2014) further allow placing volcanic sulphate emissions arising from a series of moderate volcanic eruptions during the last decade into a multi-millennial context. While these updated ice core records provide a more accurate constraint on the timing and magnitude of volcanic eruptions, there is also new data emerging on the geographic locations of past eruptions, atmospheric transport of volcanic fallout and climatic consequences (e.g. sea-ice; hydro-climate) from studying volcanic deposits (e.g. extent of volcanic ash deposition), proxy data and historical records. On the basis of selected case studies we will discuss the role volcanic eruptions have played in the Earth's climate system during the past and identify potential additional constraints provided by ice cores.

  9. MATRIX (Multiconfiguration Aerosol TRacker of mIXing state: an aerosol microphysical module for global atmospheric models

    Directory of Open Access Journals (Sweden)

    S. E. Bauer

    2008-05-01

    Full Text Available A new aerosol microphysical module MATRIX, the Multiconfiguation Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS climate model (ModelE is described. This module, which is based on the quadrature method of moments (QMOM, represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol mode, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble modes. A detailed model description and results of box-model simulations of various mode configurations are presented. The number concentration of aerosol particles activated to cloud drops depends on the mode configuration. Simulations on the global scale with the GISS climate model are evaluated against aircraft and station measurements of aerosol mass and number concentration and particle size. The model accurately captures the observed size distributions in the aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment.

  10. Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

    OpenAIRE

    G. P. Schill; Tolbert, M. A.

    2013-01-01

    Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescen...

  11. Global two-channel AVHRR aerosol climatology: effects of stratospheric aerosols and preliminary comparisons with MODIS and MISR retrievals

    Energy Technology Data Exchange (ETDEWEB)

    Geogdzhayev, Igor V. [Department of Applied Physics and Applied Mathematics, Columbia University, 2880 Broadway, New York, NY 10025 (United States); NASA Goddard Institute for Space Studies, 2880 Broadway, New York, NY 10025 (United States); Mishchenko, Michael I. [NASA Goddard Institute for Space Studies, 2880 Broadway, New York, NY 10025 (United States)]. E-mail: crmim@giss.nasa.gov; Liu Li [NASA Goddard Institute for Space Studies, 2880 Broadway, New York, NY 10025 (United States); Department of Earth and Environmental Sciences, Columbia University, 2880 Broadway, New York, NY 10025 (United States); Remer, Lorraine [NASA Goddard Space Flight Center, Code 913, Greenbelt, MD 20771 (United States)

    2004-10-15

    We present an update on the status of the global climatology of the aerosol column optical thickness and Angstrom exponent derived from channel-1 and -2 radiances of the Advanced Very High Resolution Radiometer (AVHRR) in the framework of the Global Aerosol Climatology Project (GACP). The latest version of the climatology covers the period from July 1983 to September 2001 and is based on an adjusted value of the diffuse component of the ocean reflectance as derived from extensive comparisons with ship sun-photometer data. We use the updated GACP climatology and Stratospheric Aerosol and Gas Experiment (SAGE) data to analyze how stratospheric aerosols from major volcanic eruptions can affect the GACP aerosol product. One possible retrieval strategy based on the AVHRR channel-1 and -2 data alone is to infer both the stratospheric and the tropospheric aerosol optical thickness while assuming fixed microphysical models for both aerosol components. The second approach is to use the SAGE stratospheric aerosol data in order to constrain the AVHRR retrieval algorithm. We demonstrate that the second approach yields a consistent long-term record of the tropospheric aerosol optical thickness and Angstrom exponent. Preliminary comparisons of the GACP aerosol product with MODerate resolution Imaging Spectrometer (MODIS) and Multiangle Imaging Spectro-Radiometer aerosol retrievals show reasonable agreement, the GACP global monthly optical thickness being lower than the MODIS one by approximately 0.03. Larger differences are observed on a regional scale. Comparisons of the GACP and MODIS Angstrom exponent records are less conclusive and require further analysis.

  12. Atmospheric responses to stratospheric aerosol geoengineering

    Science.gov (United States)

    Ferraro, Angus; Highwood, Eleanor; Charlton-Perez, Andrew

    2013-04-01

    Stratospheric aerosol geoengineering, also called solar radiation management (SRM), involves the injection of aerosol into the stratosphere to increase the planetary albedo. It has been conceieved as a policy option in response to human-induced global warming. It is well-established from modelling studies and observations following volcanic eruptions that stratospheric sulphate aerosols cause global cooling. Some aspects of the climate response, especially those involving large-scale dynamical changes, are more uncertain. This work attempts to identify the physical mechanisms operating in the climate response to stratospheric aerosol geoengineering using idealised model experiments. The radiative forcing produced by the aerosol depends on its type (species) and size. Aerosols absorb terrestrial and solar radiation, which drives stratospheric temperature change. The stratospheric temperature change also depends on aerosol type and size. We calculate the stratospheric temperature change due to geoengineering with sulphate, titania, limestone and soot in a fixed-dynamical-heating radiative model. Sulphate produces tropical heating of up to ~6 K. Titania produces much less heating, whereas soot produces much more. Most aerosols increase the meridional temperature gradient in the lower stratosphere which, by thermal wind balance, would be expected to intensify the zonal winds in the polar vortex. An intermediate-complexity general circulation model is used to investigate the dynamical response to geoengineering aerosols. Atmospheric carbon dioxide concentrations are quadrupled. The carbon dioxide forcing is then balanced using stratospheric sulphate aerosol. We assess dynamical changes in the stratosphere, for example, the frequency of stratospheric sudden warmings and the strength of the Brewer-Dobson overturning circulation. We also assess changes in the strength and position of the tropospheric jets. We compare results for sulphate with those for titania.

  13. Pathways, Impacts, and Policies on Severe Aerosol Injections into the Atmosphere: 2011 Severe Atmospheric Aerosols Events Conference

    KAUST Repository

    Weil, Martin

    2012-09-01

    The 2011 severe atmospheric events conference, held on August 11-12, 2011, Hamburg, Germany, discussed climatic and environmental changes as a result of various kinds of huge injections of aerosols into the atmosphere and the possible consequences for the world population. Various sessions of the conference dealt with different aspects of large aerosol injections and severe atmospheric aerosol events along the geologic time scale. A presentation about radiative heating of aerosols as a self-lifting mechanism in the Australian forest fires discussed the question of how the impact of tropical volcanic eruptions depends on the eruption season. H.-F. Graf showed that cloud-resolving plume models are more suitable to predict the volcanic plume height and dispersion than one-dimensional models. G. Stenchikov pointed out that the absorbing smoke plumes in the upper troposphere can be partially mixed into the lower stratosphere because of the solar heating and lofting effect.

  14. Roles of heparan sulfate sulfation in dentinogenesis.

    Science.gov (United States)

    Hayano, Satoru; Kurosaka, Hiroshi; Yanagita, Takeshi; Kalus, Ina; Milz, Fabian; Ishihara, Yoshihito; Islam, Md Nurul; Kawanabe, Noriaki; Saito, Masahiro; Kamioka, Hiroshi; Adachi, Taiji; Dierks, Thomas; Yamashiro, Takashi

    2012-04-06

    Cell surface heparan sulfate (HS) is an essential regulator of cell signaling and development. HS traps signaling molecules, like Wnt in the glycosaminoglycan side chains of HS proteoglycans (HSPGs), and regulates their functions. Endosulfatases Sulf1 and Sulf2 are secreted at the cell surface to selectively remove 6-O-sulfate groups from HSPGs, thereby modifying the affinity of cell surface HSPGs for its ligands. This study provides molecular evidence for the functional roles of HSPG sulfation and desulfation in dentinogenesis. We show that odontogenic cells are highly sulfated on the cell surface and become desulfated during their differentiation to odontoblasts, which produce tooth dentin. Sulf1/Sulf2 double null mutant mice exhibit a thin dentin matrix and short roots combined with reduced expression of dentin sialophosphoprotein (Dspp) mRNA, encoding a dentin-specific extracellular matrix precursor protein, whereas single Sulf mutants do not show such defective phenotypes. In odontoblast cell lines, Dspp mRNA expression is potentiated by the activation of the Wnt canonical signaling pathway. In addition, pharmacological interference with HS sulfation promotes Dspp mRNA expression through activation of Wnt signaling. On the contrary, the silencing of Sulf suppresses the Wnt signaling pathway and subsequently Dspp mRNA expression. We also show that Wnt10a protein binds to cell surface HSPGs in odontoblasts, and interference with HS sulfation decreases the binding affinity of Wnt10a for HSPGs, which facilitates the binding of Wnt10a to its receptor and potentiates the Wnt signaling pathway, thereby up-regulating Dspp mRNA expression. These results demonstrate that Sulf-mediated desulfation of cellular HSPGs is an important modification that is critical for the activation of the Wnt signaling in odontoblasts and for production of the dentin matrix.

  15. Atmospheric constituents and surface-level UVB: implications for a paleoaltimetry proxy and attempts to reconstruct UV exposure during volcanic episodes

    CERN Document Server

    Thomas, Brian C; Dalton, Sean M

    2016-01-01

    Chemical and morphological features of spores and pollens have been linked to changes in solar ultraviolet radiation (specifically UVB, 280-315 nm) at Earth's surface. Variation in UVB exposure as inferred from these features has been suggested as a proxy for paleoaltitude. While UVB irradiance does increase with altitude above sea level, a number of other factors affect the irradiance at any given place and time. In this modeling study we use the TUV atmospheric radiative transfer model to investigate dependence of surface-level UVB irradiance and relative biological impact on a number of constituents in Earth's atmosphere that are variable over long and short time periods. We consider changes in O3 column density, and SO2 and sulfate aerosols due to periods of volcanic activity, including that associated with the formation of the Siberian Traps. We find that UVB irradiance may be highly variable under volcanic conditions and variations in several of these atmospheric constituents can easily mimic or overwhe...

  16. The effect of interactive gas-phase chemistry and aerosols on climate simulations over the last millennium

    Science.gov (United States)

    Tsigaridis, K.; LeGrande, A. N.; Healy, R. J.; Schmidt, G. A.

    2013-12-01

    emissions, and a final set with all components. These species are standard components in the GISS model's 20th century simulations, so that we may compare millennial variability characteristics with those better constrained from more recent climate periods. Dust and sea-salt are wind-driven aerosols from deserts and oceans, sulfate comes from oxidation of volcanic and oceanic precursors, while organic carbon comes from biomass burning, secondary plant sources and primary oceanic emissions. Comparison of model and proxy records will test model-simulated mechanisms while the model provides insight into factors contributing to proxy variability. The addition of potentially important forcing mechanisms will enable a more comprehensive evaluation of the climate sensitivity.

  17. Anthropogenic Aerosols in Asia, Radiative Forcing, and Climate Change

    Science.gov (United States)

    Ramaswamy, V.; Bollasina, M. A.; Ming, Y.; Ocko, I.; Persad, G.

    2014-12-01

    Aerosols arising as a result of human-induced emissions in Asia form a key 'driver' in causing pollution and in the forcing of anthropogenic climate change. The manner of the forced climate change is sensitive to the scattering and absorption properties of the aerosols and the aerosol-cloud microphysical interactions. Using the NOAA/ GFDL global climate models and observations from multiple platforms, we investigate the radiative perturbations due to the 20th Century sulfate and carbonaceous aerosol emissions and the resultant impacts on surface temperature, tropical precipitation, Indian monsoon, hemispheric circulation, and atmospheric and oceanic heat transports. The influence of the aerosol species has many contrasts with that due to the anthropogenic well-mixed greenhouse gas emissions e.g., the asymmetry in the hemispheric climate response, but is subject to larger uncertainties. The aerosol forcing expected in the future indicates a significant control on the 21st Century anthropogenic climate change in Asia.

  18. Heterogeneous Chemistry: Understanding Aerosol/Oxidant Interactions

    Energy Technology Data Exchange (ETDEWEB)

    Joyce E. Penner

    2005-03-14

    Global radiative forcing of nitrate and ammonium aerosols has mostly been estimated from aerosol concentrations calculated at thermodynamic equilibrium or using approximate treatments for their uptake by aerosols. In this study, a more accurate hybrid dynamical approach (DYN) was used to simulate the uptake of nitrate and ammonium by aerosols and the interaction with tropospheric reactive nitrogen chemistry in a three-dimensional global aerosol and chemistry model, IMPACT, which also treats sulfate, sea salt and mineral dust aerosol. 43% of the global annual average nitrate aerosol burden, 0.16 TgN, and 92% of the global annual average ammonium aerosol burden, 0.29 TgN, exist in the fine mode (D<1.25 {micro}m) that scatters most efficiently. Results from an equilibrium calculation differ significantly from those of DYN since the fraction of fine-mode nitrate to total nitrate (gas plus aerosol) is 9.8%, compared to 13% in DYN. Our results suggest that the estimates of aerosol forcing from equilibrium concentrations will be underestimated. We also show that two common approaches used to treat nitrate and ammonium in aerosol in global models, including the first-order gas-to-particle approximation based on uptake coefficients (UPTAKE) and a hybrid method that combines the former with an equilibrium model (HYB), significantly overpredict the nitrate uptake by aerosols especially that by coarse particles, resulting in total nitrate aerosol burdens higher than that in DYN by +106% and +47%, respectively. Thus, nitrate aerosol in the coarse mode calculated by HYB is 0.18 Tg N, a factor of 2 more than that in DYN (0.086 Tg N). Excessive formation of the coarse-mode nitrate in HYB leads to near surface nitrate concentrations in the fine mode lower than that in DYN by up to 50% over continents. In addition, near-surface HNO{sub 3} and NO{sub x} concentrations are underpredicted by HYB by up to 90% and 5%, respectively. UPTAKE overpredicts the NO{sub x} burden by 56% and near

  19. The ceric sulfate dosimeter

    DEFF Research Database (Denmark)

    Bjergbakke, Erling

    1970-01-01

    The process employed for the determination of absorbed dose is the reduction of ceric ions to cerous ions in a solution of ceric sulfate and cerous sulfate in 0.8N sulfuric acid: Ce4+→Ce 3+ The absorbed dose is derived from the difference in ceric ion concentration before and after irradiation...

  20. Particle analysis of volcanic ash with Electron Microscopy

    Science.gov (United States)

    Lieke, K. I.; Kristensen, T. B.; Koch, C. B.; Korsholm, U. S.; Sørensen, J. H.; Bilde, M.

    2012-04-01

    Since the airspace closure over Europe due to the Eyjafjalla eruption in 2010, volcanic ash has come more in the focus of atmospheric science. The airspace closure accompanying the Grímsvötn eruption in 2011 clearly indicates that there is still a great need to increase the scientific understanding of the properties and impacts of volcanic ash particles. Determination of particle characteristics, preferably in near real time, serves as an important input to transport models in operational use for decision support and guidance of authorities. We collected particles before and after the Grímsvötn volcanic ash arrived at Copenhagen, Denmark, between 23 May and 31 May 2011, as well as at a number of other locations. The analysis of meteorological conditions shows that the particle collection performed before arrival of the volcanic ash may serve as a good reference sample. We have thus been able to identify significant differences in aerosol chemical composition during a volcanic ash event over Copenhagen. These results are compared to volcanic ash particles collected on Iceland. We provide unique data about single-particle structure, chemical composition, size and morphology of volcanic ash particles. Single-particle analysis by SEM, and mineralogical studies by XRD and TEM prove that the particles are composed of glass of a characteristic composition and small, nm sized minerals attached to the large (up to tens of µm) glass fragments. The derived information about volcanic ash particles can be used by transport models, resulting in improved information to the authorities in case of new volcanic ash events over Scandinavia or Europe.

  1. Factors Affecting Aerosol Radiative Forcing

    Science.gov (United States)

    Wang, Jingxu; Lin, Jintai; Ni, Ruijing

    2016-04-01

    Rapid industrial and economic growth has meant a large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RF of aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissions per unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size. South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions, its aerosol RF is alleviated by its lowest chemical efficiency. The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is lowered by a small per capita GDP. Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The

  2. Factors Affecting Aerosol Radiative Forcing

    Science.gov (United States)

    Wang, J.; Lin, J.; Ni, R.

    2016-12-01

    Rapid industrial and economic growth has meant large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RFof aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissionsper unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size.South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions,its aerosol RF is alleviated by its lowest chemical efficiency.The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is loweredbyasmall per capita GDP.Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The resulting

  3. Volcanic Rocks and Features

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — Volcanoes have contributed significantly to the formation of the surface of our planet. Volcanism produced the crust we live on and most of the air we breathe. The...

  4. Improved aerosol radiative properties as a foundation for solar geoengineering risk assessment

    Science.gov (United States)

    Dykema, J. A.; Keith, D. W.; Keutsch, F. N.

    2016-07-01

    Side effects resulting from the deliberate injection of sulfate aerosols intended to partially offset climate change have motivated the investigation of alternatives, including solid aerosol materials. Sulfate aerosols warm the tropical tropopause layer, increasing the flux of water vapor into the stratosphere, accelerating ozone loss, and increasing radiative forcing. The high refractive index of some solid materials may lead to reduction in these risks. We present a new analysis of the scattering efficiency and absorption of a range of candidate solid aerosols. We utilize a comprehensive radiative transfer model driven by updated, physically consistent estimates of optical properties. We compute the potential increase in stratospheric water vapor and associated longwave radiative forcing. We find that the stratospheric heating calculated in this analysis indicates some materials to be substantially riskier than previous work. We also find that there are Earth-abundant materials that may reduce some principal known risks relative to sulfate aerosols.

  5. Modelling of aerosol processes in plumes

    Energy Technology Data Exchange (ETDEWEB)

    Lazaridis, M.; Isukapalli, S.S.; Georgopoulos, P.G. [Norwegian Institute of Air Research, Kjeller (Norway)

    2001-07-01

    A modelling platform for studying photochemical gaseous and aerosol phase processes from localized (e.g., point) sources has been presented. The current approach employs a reactive plume model which extends the regulatory model RPM-IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, nitrate, ammonium material of aerosols are treated and attributed to the PM size distribution. A modified version of the carbon bond IV chemical mechanism is included to model the formation of organic aerosol. Aerosol dynamics modeled include mechanisms of nucleation, condensation, dry deposition and gas/particle partitioning of organic matter. The model is first applied to a number of case studies involving emissions from point sources and sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions. In addition, the model is compared with field data from power plant plumes with satisfactory predictions against gaseous species and total sulphate mass measurements. Finally, the plume model is applied to study secondary organic matter formation due to various emission categories such as vehicles and the oil production sector.

  6. Heparan sulfate biosynthesis

    DEFF Research Database (Denmark)

    Multhaupt, Hinke A B; Couchman, John R

    2012-01-01

    Heparan sulfate is perhaps the most complex polysaccharide known from animals. The basic repeating disaccharide is extensively modified by sulfation and uronic acid epimerization. Despite this, the fine structure of heparan sulfate is remarkably consistent with a particular cell type. This suggests...... that the synthesis of heparan sulfate is tightly controlled. Although genomics has identified the enzymes involved in glycosaminoglycan synthesis in a number of vertebrates and invertebrates, the regulation of the process is not understood. Moreover, the localization of the various enzymes in the Golgi apparatus has......-quality resolution of the distribution of enzymes. The EXT2 protein, which when combined as heterodimers with EXT1 comprises the major polymerase in heparan sulfate synthesis, has been studied in depth. All the data are consistent with a cis-Golgi distribution and provide a starting point to establish whether all...

  7. Self-limiting physical and chemical effects in volcanic eruption clouds

    Science.gov (United States)

    Pinto, Joseph P.; Toon, Owen B.; Turco, Richard P.

    1989-01-01

    One-dimensional aerosol microphysical and photochemical models are used to study the chemistry of stratospheric volcanic clouds. The results indicate that the aerosol microphysical processes of condensation and coagulation produce larger particles as the SO2 injection rate is increased. Larger particles have a smaller optical depth per unit mass and settle out of the stratosphere at a faster rate than smaller ones, restricting the total number of particles in the stratosphere. The microphysical processes moderate the impact of volcanic clouds on the earth's radiation budget and climate, suggesting that volcanic effects may be self limiting. It is noted that the injection of HCl into the stratosphere, which could lead to large ozone changes, is limited by a cold trap effect in which HCl and water vapor condense on ash particles in the rising volcanic plume and fall out as ice.

  8. Coarse mode aerosols in the High Arctic

    Science.gov (United States)

    Baibakov, K.; O'Neill, N. T.; Chaubey, J. P.; Saha, A.; Duck, T. J.; Eloranta, E. W.

    2014-12-01

    Fine mode (submicron) aerosols in the Arctic have received a fair amount of scientific attention in terms of smoke intrusions during the polar summer and Arctic haze pollution during the polar winter. Relatively little is known about coarse mode (supermicron) aerosols, notably dust, volcanic ash and sea salt. Asian dust is a regular springtime event whose optical and radiative forcing effects have been fairly well documented at the lower latitudes over North America but rarely reported for the Arctic. Volcanic ash, whose socio-economic importance has grown dramatically since the fear of its effects on aircraft engines resulted in the virtual shutdown of European civil aviation in the spring of 2010 has rarely been reported in the Arctic in spite of the likely probability that ash from Iceland and the Aleutian Islands makes its way into the Arctic and possibly the high Arctic. Little is known about Arctic sea salt aerosols and we are not aware of any literature on the optical measurement of these aerosols. In this work we present preliminary results of the combined sunphotometry-lidar analysis at two High Arctic stations in North America: PEARL (80°N, 86°W) for 2007-2011 and Barrow (71°N,156°W) for 2011-2014. The multi-years datasets were analyzed to single out potential coarse mode incursions and study their optical characteristics. In particular, CIMEL sunphotometers provided coarse mode optical depths as well as information on particle size and refractive index. Lidar measurements from High Spectral Resolution lidars (AHSRL at PEARL and NSHSRL at Barrow) yielded vertically resolved aerosol profiles and gave an indication of particle shape and size from the depolarization ratio and color ratio profiles. Additionally, we employed supplementary analyses of HYSPLIT backtrajectories, OMI aerosol index, and NAAPS (Navy Aerosol Analysis and Prediction System) outputs to study the spatial context of given events.

  9. Ice nucleating properties of volcanic ash particles from the Eyjafjallajökull volcanic eruption

    Science.gov (United States)

    Kulkarni, G.; Zelenyuk, A.; Beranek, J.

    2011-12-01

    The volcanic ash from the volcanic emissions can significantly contribute to the natural source of aerosols in the atmosphere. In the vicinity and downwind of eruption site, the transported ash might have a stronger impact on the aviation industry, regional air quality, and climate. Despite the environmental significance of ash, our understanding of ash particles reacting with other volcanic plume constituents is rudimentary. In particular, the complex interactions between the water vapor and ash particles under different meteorological conditions that lead to cloud hydrometeors are poorly understood. To improve our understanding, we focus on investigating the ice formation properties of ash particles collected from the recent volcanic eruption. It was observed that the ash particles are less efficient ice nuclei compared to the natural dust particles in the deposition nucleation regime, but have similar efficiencies in the condensation freezing mode. The ice nucleated ash particles are separated from the interstitial particles, and further evaporated to understand the elemental composition, size, shape and morphology of the ice residue using the single particle mass spectrometer. The elemental composition reveals that majority of the elements are also present in the natural dust particles, but subtle differences are observed. This suggests that particle properties play an important role in the ice nucleation process.

  10. MICS Asia Phase II - Sensitivity to the aerosol module

    CERN Document Server

    Sartelet, Karine; Sportisse, Bruno

    2007-01-01

    In the framework of the model inter-comparison study - Asia Phase II (MICS2), where eight models are compared over East Asia, this paper studies the influence of different parameterizations used in the aerosol module on the aerosol concentrations of sulfate and nitrate in PM10. An intracomparison of aerosol concentrations is done for March 2001 using different configurations of the aerosol module of one of the model used for the intercomparison. Single modifications of a reference setup for model configurations are performed and compared to a reference case. These modifications concern the size distribution, i.e. the number of sections, and physical processes, i.e. coagulation, condensation/evaporation, cloud chemistry, heterogeneous reactions and sea-salt emissions. Comparing monthly averaged concentrations at different stations, the importance of each parameterization is first assessed. It is found that sulfate concentrations are little sensitive to sea-salt emissions and to whether condensation is computed...

  11. Computational study of the effect of glyoxal-sulfate clustering on the Henry's Law coefficient of glyoxal

    DEFF Research Database (Denmark)

    Kurtén, Theo; Elm, Jonas; Prisle, Nønne L.

    2015-01-01

    -containing aerosol particles. This promotes the participation of glyoxal in reactions leading to secondary organic aerosol formation, especially in regions with high sulfate concentrations. We used our computed equilibrium constants for the complexation reactions to assess the magnitude of the Henry's law...

  12. Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

    Science.gov (United States)

    Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

    2012-07-01

    Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

  13. Radiative and climate impacts of a large volcanic eruption during stratospheric sulfur geoengineering

    Directory of Open Access Journals (Sweden)

    A. Laakso

    2016-01-01

    Full Text Available Both explosive volcanic eruptions, which emit sulfur dioxide into the stratosphere, and stratospheric geoengineering via sulfur injections can potentially cool the climate by increasing the amount of scattering particles in the atmosphere. Here we employ a global aerosol-climate model and an Earth system model to study the radiative and climate changes occurring after an erupting volcano during solar radiation management (SRM. According to our simulations the radiative impacts of the eruption and SRM are not additive and the radiative effects and climate changes occurring after the eruption depend strongly on whether SRM is continued or suspended after the eruption. In the former case, the peak burden of the additional stratospheric sulfate as well as changes in global mean precipitation are fairly similar regardless of whether the eruption takes place in a SRM or non-SRM world. However, the maximum increase in the global mean radiative forcing caused by the eruption is approximately 21 % lower compared to a case when the eruption occurs in an unperturbed atmosphere. In addition, the recovery of the stratospheric sulfur burden and radiative forcing is significantly faster after the eruption, because the eruption during the SRM leads to a smaller number and larger sulfate particles compared to the eruption in a non-SRM world. On the other hand, if SRM is suspended immediately after the eruption, the peak increase in global forcing caused by the eruption is about 32 % lower compared to a corresponding eruption into a clean background atmosphere. In this simulation, only about one-third of the global ensemble-mean cooling occurs after the eruption, compared to that occurring after an eruption under unperturbed atmospheric conditions. Furthermore, the global cooling signal is seen only for the 12 months after the eruption in the former scenario compared to over 40 months in the latter. In terms of global precipitation rate, we obtain a 36

  14. Radiative and climate impacts of a large volcanic eruption during stratospheric sulfur geoengineering

    Science.gov (United States)

    Laakso, A.; Kokkola, H.; Partanen, A.-I.; Niemeier, U.; Timmreck, C.; Lehtinen, K. E. J.; Hakkarainen, H.; Korhonen, H.

    2016-01-01

    Both explosive volcanic eruptions, which emit sulfur dioxide into the stratosphere, and stratospheric geoengineering via sulfur injections can potentially cool the climate by increasing the amount of scattering particles in the atmosphere. Here we employ a global aerosol-climate model and an Earth system model to study the radiative and climate changes occurring after an erupting volcano during solar radiation management (SRM). According to our simulations the radiative impacts of the eruption and SRM are not additive and the radiative effects and climate changes occurring after the eruption depend strongly on whether SRM is continued or suspended after the eruption. In the former case, the peak burden of the additional stratospheric sulfate as well as changes in global mean precipitation are fairly similar regardless of whether the eruption takes place in a SRM or non-SRM world. However, the maximum increase in the global mean radiative forcing caused by the eruption is approximately 21 % lower compared to a case when the eruption occurs in an unperturbed atmosphere. In addition, the recovery of the stratospheric sulfur burden and radiative forcing is significantly faster after the eruption, because the eruption during the SRM leads to a smaller number and larger sulfate particles compared to the eruption in a non-SRM world. On the other hand, if SRM is suspended immediately after the eruption, the peak increase in global forcing caused by the eruption is about 32 % lower compared to a corresponding eruption into a clean background atmosphere. In this simulation, only about one-third of the global ensemble-mean cooling occurs after the eruption, compared to that occurring after an eruption under unperturbed atmospheric conditions. Furthermore, the global cooling signal is seen only for the 12 months after the eruption in the former scenario compared to over 40 months in the latter. In terms of global precipitation rate, we obtain a 36 % smaller decrease in the

  15. Aerosol measurements over South Africa using LIDAR, Satellite and Sun Photometer

    CSIR Research Space (South Africa)

    Sivakumar, V

    2010-05-01

    Full Text Available of South Africa. 1. Introduction Aerosols (solid particles suspended in the air) play an important role in the global climate, the radiative forcing of the climate, and the Earth?s radiative balance. The interaction between atmospheric aerosol... pollution as well as from natural processes, such as wind generated dust and sea spray, volcanic eruptions and smoke from natural forest fires, etc. The knowledge of aerosol characteristics at a local and global scale, their temporal change interrelations...

  16. Volcanic ash: What it is and how it forms

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, G.

    1991-09-13

    There are four basic eruption processes that produce volcanic ash: (1) decompression of rising magma, gas bubble growth, and fragmentation of the foamy magma in the volcanic vent (magmatic), (2) explosive mixing of magma with ground or surface water (hydrovolcanic), (3) fragmentation of country rock during rapid expansion of steam and/or hot water (phreatic), and (4) breakup of lava fragments during rapid transport from the vent. Variations in eruption style and the characteristics of volcanic ashes produced during explosive eruptions depend on many factors, including magmatic temperature, gas content, viscosity and crystal content of the magma before eruption, the ratio of magma to ground or surface water, and physical properties of the rock enclosing the vent. Volcanic ash is composed of rock and mineral fragments, and glass shards, which is less than 2 mm in diameter. Glass shard shapes and sizes depend upon size and shape of gas bubbles present within the magma immediately before eruption and the processes responsible for fragmentation of the magma. Shards range from slightly curved, thin glass plates, which were broken from large, thin-walled spherical bubble walls, to hollow needles broken from pumiceous melts containing gas bubbles stretched by magma flow within the volcanic vent. Pumice fragments make up the coarser-grained portions of the glass fraction. Particle sizes range from meters for large blocks expelled near the volcanic vent to nanometers for fine ash and aerosol droplets within well-dispersed eruption plumes. 18 refs., 6 figs., 1 tab.

  17. Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

    Science.gov (United States)

    Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

    2015-11-01

    To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

  18. Impacts of East Asian aerosols on the Asian monsoon

    Science.gov (United States)

    Bartlett, Rachel; Bollasina, Massimo; Booth, Ben; Dunstone, Nick; Marenco, Franco

    2016-04-01

    Over recent decades, aerosol emissions from Asia have increased rapidly. Aerosols are able to alter radiative forcing and regional hydroclimate through direct and indirect effects. Large emissions within the geographical region of the Asian monsoon have been found to impact upon this vital system and have been linked to observed drying trends. The interconnected nature of smaller regional monsoon components (e.g. the Indian monsoon and East Asian monsoon) presents the possibility that aerosol sources could have far-reaching impacts. Future aerosol emissions are uncertain and may continue to dominate regional impacts on the Asian monsoon. Standard IPCC future emissions scenarios do not take a broad sample of possible aerosol pathways. We investigate the sensitivity of the Asian monsoon to East Asian aerosol emissions. Experiments carried out with HadGEM2-ES use three time-evolving future anthropogenic aerosol emissions scenarios with similar time-evolving greenhouse gases. We find a wetter summer over southern China and the Indochina Peninsula associated with increased sulfate aerosol over China. The southern-flood-northern-drought pattern seen in observations is reflected in these results. India is found to be drier in the summer overall, although wetter in June. These precipitation changes are linked to the increase in sulfate through the alteration of large scale dynamics. Sub-seasonal changes are also seen, with an earlier withdrawal of the monsoon over East Asia.

  19. MATRIX (Multiconfiguration Aerosol TRacker of mIXing state: an aerosol microphysical module for global atmospheric models

    Directory of Open Access Journals (Sweden)

    S. E. Bauer

    2008-10-01

    Full Text Available A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS climate model (ModelE are described. This module, which is based on the quadrature method of moments (QMOM, represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations.

    A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment

  20. MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models

    Energy Technology Data Exchange (ETDEWEB)

    Bauer,S.E.; Wright, D.L.; Koch, D.; Lewis, E.R.; McGraw, R.; Chang, L.-S.; Schwartz, S.E.; Ruedy, R.

    2008-10-21

    A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) are described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations. A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 {micro}m, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment. This is more likely due

  1. Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis

    Directory of Open Access Journals (Sweden)

    K. S. Johnson

    2006-05-01

    Full Text Available Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA. The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish effective pollution control standards. For these reasons, samples of particulate matter ≤2.5 μm (PM2.5 were collected during the MCMA-2003 Field Campaign for elemental and multivariate analyses. Proton-Induced X-ray Emission (PIXE, Proton-Elastic Scattering Analysis (PESA and Scanning Transmission Ion Microscopy (STIM techniques were done to determine concentrations of 19 elements from Na to Pb, hydrogen, and total mass, respectively. The most abundant elements from PIXE analysis were S, Si, K, Fe, Ca, and Al, while the major emissions sources associated with these elements were industry, wind-blown soil, and biomass burning. Wind trajectories suggest that metals associated with industrial emissions came from northern areas of the city whereas soil aerosols came from the southwest and increased in concentration during dry conditions. Elemental markers for fuel oil combustion V and Ni correlated with a large SO2 plume to suggest an anthropogenic, rather than volcanic, emissions source. By subtracting major components of soil and sulfate determined by PIXE analysis from STIM total mass measurements, we estimate that approximately 50% of non-volatile PM2.5 consisted of carbonaceous material.

  2. Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis

    Directory of Open Access Journals (Sweden)

    K. S. Johnson

    2006-01-01

    Full Text Available Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA. The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish effective pollution control standards. For these reasons, samples of particulate matter ≤2.5 μm (PM2.5 were collected during the MCMA-2003 Field Campaign for elemental and multivariate analyses. Proton-Induced X-ray Emission (PIXE, Proton-Elastic Scattering Analysis (PESA and Scanning Transmission Ion Microscopy (STIM measurements were done to determine concentrations of 19 elements from Na to Pb, hydrogen, and total mass, respectively. The most abundant elements from PIXE analysis were S, Si, K, Fe, Ca, and Al, while the major emissions sources associated with these elements were industry, wind-blown soil, and biomass burning. Wind trajectories suggest that metals associated with industrial emissions came from northern areas of the city whereas soil aerosols came from the southwest and increased in concentration during dry conditions. Elemental markers for fuel oil combustion, V and Ni, correlated with a large SO2 plume to suggest an anthropogenic, rather than volcanic, emissions source. By subtracting major components of soil and sulfates determined by PIXE analysis from STIM total mass measurements, we estimate that approximately 50% of non-volatile PM2.5 consisted of carbonaceous material.

  3. Secondary organic material formed by methylglyoxal in aqueous aerosol mimics – Part 2: Product identification using Aerosol-CIMS

    Directory of Open Access Journals (Sweden)

    V. F. McNeill

    2009-07-01

    Full Text Available We used chemical ionization mass spectrometry with a volatilization flow tube inlet (Aerosol-CIMS to characterize secondary organic material formed by methylglyoxal with ammonium sulfate in aqueous aerosol mimics. Bulk reaction mixtures were diluted and atomized to form submicron aerosol particles. Organics were detected using Aerosol-CIMS in positive and negative ion mode using I− and H3O+·(H2On as reagent ions. The results are consistent with aldol condensation products, carbon-nitrogen species, sulfur-containing compounds, and oligomeric species up to 759 amu. These results support previous observations by us and others that ammonium sulfate plays a critical role in the SOA formation chemistry of dicarbonyl compounds.

  4. Evidence for marine biogenic influence on summertime Arctic aerosol

    Science.gov (United States)

    Willis, Megan D.; Köllner, Franziska; Burkart, Julia; Bozem, Heiko; Thomas, Jennie L.; Schneider, Johannes; Aliabadi, Amir A.; Hoor, Peter M.; Schulz, Hannes; Herber, Andreas B.; Leaitch, W. Richard; Abbatt, Jonathan P. D.

    2017-06-01

    We present vertically resolved observations of aerosol composition during pristine summertime Arctic background conditions. The methansulfonic acid (MSA)-to-sulfate ratio peaked near the surface (mean 0.10), indicating a contribution from ocean-derived biogenic sulfur. Similarly, the organic aerosol (OA)-to-sulfate ratio increased toward the surface (mean 2.0). Both MSA-to-sulfate and OA-to-sulfate ratios were significantly correlated with FLEXPART-WRF-predicted air mass residence time over open water, indicating marine-influenced OA. External mixing of sea salt aerosol from a larger number fraction of organic, sulfate, and amine-containing particles, together with low wind speeds (median 4.7 m s-1), suggests a role for secondary organic aerosol formation. Cloud condensation nuclei concentrations were nearly constant (˜120 cm-3) when the OA fraction was <60% and increased to 350 cm-3 when the organic fraction was larger and residence times over open water were longer. Our observations illustrate the importance of marine-influenced OA under Arctic background conditions, which are likely to change as the Arctic transitions to larger areas of open water.

  5. General Motors sulfate dispersion experiment: experimental procedures and results

    Energy Technology Data Exchange (ETDEWEB)

    Cadle, S.H.; Chock, D.P.; Monson, P.R.; Heuss, J.M.

    1977-01-01

    A massive experiment was conducted at the General Motors Proving Ground to measure the dispersion of sulfates generated by catalyst equipped vehicles. 352 cars equipped with catalysts and air pumps were driven on a 10 kilometer test track to provide a simulated freeway situation with a traffic density of 5462 cars/hour. Experiments were conducted on 17 days in October 1975, providing sixty-six 30 min data sets. On most days, the experiment was carried out early in the morning in order to run under the most adverse meteorological conditions available. Samples of airborne sulfate and a gas tracer, sulfur hexafluoride, as well as extensive meteorological data were collected simultaneously at 20 sampling points under a wide variety of meteorological conditions. The maximum measured increase in sulfate from each 30 min data set was generally found next to the roadway at the lowest level and varied from 3 to 15 ..mu..g/m/sup 3/. This increase in sulfate over background fell off rapidly with height and distance. Sulfate increases in vehicles (2 hr averages) ranged from 0 to 20 ..mu..g/m/sup 3/, and averaged 4 ..mu..g/m/sup 3/. Within experimental uncertainty, the sulfate aerosol and the gas tracer were found to disperse in the same manner. The tracer data have also been used to calculate the sulfate emission rate of the vehicles.

  6. Atmospheric constituents and surface-level UVB: Implications for a paleoaltimetry proxy and attempts to reconstruct UV exposure during volcanic episodes

    Science.gov (United States)

    Thomas, Brian C.; Goracke, Byron D.; Dalton, Sean M.

    2016-11-01

    Chemical and morphological features of spores and pollens have been linked to changes in solar ultraviolet radiation (specifically UVB, 280-315 nm) at Earth's surface. Variation in UVB exposure as inferred from these features has been suggested as a proxy for paleoaltitude; such proxies are important in understanding the uplift history of high altitude plateaus, which in turn is important for testing models of the tectonic processes responsible for such uplift. While UVB irradiance does increase with altitude above sea level, a number of other factors affect the irradiance at any given place and time. In this modeling study we use the TUV atmospheric radiative transfer model to investigate dependence of surface-level UVB irradiance and relative biological impact on a number of constituents in Earth's atmosphere that are variable over long and short time periods. We consider changes in O3 column density, and SO2 and sulfate aerosols due to periods of volcanic activity, including that associated with the formation of the Siberian Traps. We find that UVB irradiance may be highly variable under volcanic conditions and variations in several of these atmospheric constituents can easily mimic or overwhelm changes in UVB irradiance due to changes in altitude. On the other hand, we find that relative change with altitude is not very sensitive to different sets of atmospheric conditions. Any paleoaltitude proxy based on UVB exposure requires confidence that the samples under comparison were located at roughly the same latitude, under very similar O3 and SO2 columns, with similar atmospheric aerosol conditions. In general, accurate estimates of the surface-level UVB exposure at any time and location require detailed radiative transfer modeling taking into account a number of atmospheric factors; this result is important for paleoaltitude proxies as well as attempts to reconstruct the UV environment through geologic time and to tie extinctions, such as the end-Permian mass

  7. WRF-Chem Simulations of Aerosols and Anthropogenic Aerosol Radiative Forcing in East Asia

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Yi; Zhao, Chun; Liu, Xiaohong; Zhang, Meigen; Leung, Lai-Yung R.

    2014-08-01

    This study aims to provide a first comprehensive evaluation of WRF-Chem for modeling aerosols and anthropogenic aerosol radiative forcing (RF) over East Asia. Several numerical experiments were conducted from November 2007 to December 2008. Comparison between model results and observations shows that the model can generally reproduce the observed spatial distributions of aerosol concentration, aerosol optical depth (AOD) and single scattering albedo (SSA) from measurements at different sites, including the relatively higher aerosol concentration and AOD over East China and the relatively lower AOD over Southeast Asia, Korean, and Japan. The model also depicts the seasonal variation and transport of pollutions over East Asia. Particulate matter of 10 um or less in the aerodynamic diameter (PM10), black carbon (BC), sulfate (SO42-), nitrate (NO3-) and ammonium (NH4+) concentrations are higher in spring than other seasons in Japan due to the pollutant transport from polluted area of East Asia. AOD is high over Southwest and Central China in winter, spring and autumn and over North China in summer while is low over South China in summer due to monsoon precipitation. SSA is lowest in winter and highest in summer. The model also captures the dust events at the Zhangye site in the semi-arid region of China. Anthropogenic aerosol RF is estimated to range from -5 to -20 W m-2 over land and -20 to -40 W m-2 over ocean at the top of atmosphere (TOA), 5 to 30 W m-2 in the atmosphere (ATM) and -15 to -40 W m-2 at the bottom (BOT). The warming effect of anthropogenic aerosol in ATM results from BC aerosol while the negative aerosol RF at TOA is caused by scattering aerosols such as SO4 2-, NO3 - and NH4+. Positive BC RF at TOA compensates 40~50% of the TOA cooling associated with anthropogenic aerosol.

  8. Dispersion of the Nabro volcanic plume and its relation to the Asian summer monsoon

    OpenAIRE

    Fairlie, T. D.; Vernier, J.-P.; M. Natarajan; Bedka, K M

    2014-01-01

    We use nighttime measurements from the Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, together with a Lagrangian trajectory model, to study the initial dispersion of volcanic aerosol from the eruption of Mt. Nabro (Ethiopia/Eritrea) in June 2011. The Nabro eruption reached the upper troposphere and lower stratosphere (UTLS) directly, and the plume was initially entrained by the flow surrounding the Asian anticyclone, which prevails in ...

  9. Atmospheric and environmental impacts of volcanic ash particle emissions

    Science.gov (United States)

    Durant, Adam

    2010-05-01

    Globally, at any one time, there may be 20 volcanoes erupting that collectively emit a constant flux of gases and aerosol, including silicate particles (tephra), to the atmosphere which influences processes including cloud microphysics, heterogeneous chemistry and radiative balance. The nature and impact of atmospheric volcanic particle fluxes depend on total mass erupted, emission rate, emission source location, physical and chemical properties of the particles, and the location and residence time of the particles in the atmosphere. Removal of ash particles from the atmosphere through sedimentation is strongly influenced by particle aggregation through hydrometeor formation, and convective instabilities such as mammatus. I will address the following questions: What are the atmospheric impacts of volcanic ash emissions? What controls the residence time of volcanic particles in the atmosphere? What affects particle accumulation at the surface? And what are the human and environmental impacts of ash fallout?

  10. Volcanism and global change conference set for 1992

    Science.gov (United States)

    Papers are solicited for the AGU Chapman Conference on Climate, Volcanism, and Global Change, to be held March 23-27, 1992, in Hilo, Hawaii. Conference conveners are Stephen Self, University of Hawaii at Manoa, and Richard P. Turco, University of California, Los Angeles. Papers should focus on areas related to volcanic eruption dynamics and geochemistry, dispersion and removal of volcanogenic aerosols, effects on the atmosphere and climate, and signatures in sediments, ice cores, and tree rings. The conference will bring together a broad range of geophysicists whose research or interests involve volcanic eruptions and their impact. Results obtained from investigations of the El Chichón 1982 event and its aftermath are of particular interest for sessions dedicated to this specific, well-documented atmospheric perturbation.

  11. Solfataric Alteration in Hawaii as a Mechanism for Formation of the Sulfates Observed on Mars by OMEGA and the MER Instruments

    Science.gov (United States)

    Bishop, J. L.; Schiffman, P.; Lane, M. D.; Dyar, M. D.

    2005-03-01

    Solfataric alteration in the Kilauea caldera, HI, forms sulfates and hydrated phases from volcanic ash. Spectral analyses are presented for detection of these minerals/phases on Mars by OMEGA and for groundtruthing the OMEGA spectra with MER data.

  12. Satellite Observations of Atmospheric SO2 from Volcanic Eruptions

    Science.gov (United States)

    Khokhar, M. F.; Platt, U.; Wagner, T.

    Volcanoes are an important source of various atmospheric trace gases. Volcanic eruptions and their emissions are sporadic and intermittent and often occur in uninhabited regions. Therefore assessing the amount and size of the gaseous and particulate emission from volcanoes is difficult. Satellite remote sensing measurements provide one well suited opportunity to overcome this difficulty. Onboard ERS-2, GOME's moderate spectral resolution enables us to apply the Differential Optical Absorption Spectroscopy (DOAS) algorithm to retrieve SO2 column densities from radiance/irradiance measurements in UV spectral region. Volcanic emissions can cause significant variations of climate on a variety of time scales; just one very large eruption can cause a measurable change in the Earth's climate with a time scale of a few years. Stratospheric aerosols produced by volcanic eruptions can influence stratospheric chemistry both through chemical reactions that take place on the surface of the aerosols and through temperature changes induced by their presence in the stratosphere. In this work we give a comprehensive overview on several volcanoes and the retrieval of SO2 column densities from GOME data for the years 1996 - 2002. The focus is on both eruption and out gassing scenarios from different volcanic eruptions in Italy, Iceland, Congo/ Zaire, Ecuador and Mexico.

  13. Volcanic hazards to airports

    Science.gov (United States)

    Guffanti, M.; Mayberry, G.C.; Casadevall, T.J.; Wunderman, R.

    2009-01-01

    Volcanic activity has caused significant hazards to numerous airports worldwide, with local to far-ranging effects on travelers and commerce. Analysis of a new compilation of incidents of airports impacted by volcanic activity from 1944 through 2006 reveals that, at a minimum, 101 airports in 28 countries were affected on 171 occasions by eruptions at 46 volcanoes. Since 1980, five airports per year on average have been affected by volcanic activity, which indicates that volcanic hazards to airports are not rare on a worldwide basis. The main hazard to airports is ashfall, with accumulations of only a few millimeters sufficient to force temporary closures of some airports. A substantial portion of incidents has been caused by ash in airspace in the vicinity of airports, without accumulation of ash on the ground. On a few occasions, airports have been impacted by hazards other than ash (pyroclastic flow, lava flow, gas emission, and phreatic explosion). Several airports have been affected repeatedly by volcanic hazards. Four airports have been affected the most often and likely will continue to be among the most vulnerable owing to continued nearby volcanic activity: Fontanarossa International Airport in Catania, Italy; Ted Stevens Anchorage International Airport in Alaska, USA; Mariscal Sucre International Airport in Quito, Ecuador; and Tokua Airport in Kokopo, Papua New Guinea. The USA has the most airports affected by volcanic activity (17) on the most occasions (33) and hosts the second highest number of volcanoes that have caused the disruptions (5, after Indonesia with 7). One-fifth of the affected airports are within 30 km of the source volcanoes, approximately half are located within 150 km of the source volcanoes, and about three-quarters are within 300 km; nearly one-fifth are located more than 500 km away from the source volcanoes. The volcanoes that have caused the most impacts are Soufriere Hills on the island of Montserrat in the British West Indies

  14. Analysis and quantification of the diversities of aerosol life cycles within AeroCom

    NARCIS (Netherlands)

    Textor, C.; Schulz, M.; Guibert, S.; Kinne, S.; Balkanski, Y.; Bauer, S.; Berntsen, T.; Berglen, T.; Boucher, O.; Chin, M.; Dentener, F.; Diehl, T.; Easter, R.; Feichter, H.; Fillmore, D.; Ghan, S.; Ginoux, P.; Gong, S.; Grini, A.; Hendricks, J.; Horowitz, L.; Huang, P.; Isaksen, I.; Iversen, T.; Kloster, S.; Koch, D.; Kirkevåg, A.; Kristjansson, J.E.; Krol, M.C.; Lauer, A.; Lamarque, J.F.; Liu, X.; Montanaro, V.; Myhre, G.; Penner, J.; Pitari, G.; Reddy, S.; Seland, O.; Stier, P.; Takemura, T.; Tie, X.

    2006-01-01

    Simulation results of global aerosol models have been assembled in the framework of the AeroCom intercomparison exercise. In this paper, we analyze the life cycles of dust, sea salt, sulfate, black carbon and particulate organic matter as simulated by sixteen global aerosol models. The differences a

  15. Enhancement of aerosol responses to changes in emissions over East Asia by gas-oxidant-aerosol coupling and detailed aerosol processes

    Science.gov (United States)

    Matsui, H.; Koike, M.

    2016-06-01

    We quantify the responses of aerosols to changes in emissions (sulfur dioxide, black carbon (BC), primary organic aerosol, nitrogen oxides (NOx), and volatile organic compounds) over East Asia by using simulations including gas-oxidant-aerosol coupling, organic aerosol (OA) formation, and BC aging processes. The responses of aerosols to NOx emissions are complex and are dramatically changed by simulating gas-phase chemistry and aerosol processes online. Reduction of NOx emissions by 50% causes a 30-40% reduction of oxidant (hydroxyl radical and ozone) concentrations and slows the formation of sulfate and OA by 20-30%. Because the response of OA to changes in NOx emissions is sensitive to the treatment of emission and oxidation of semivolatile and intermediate volatility organic compounds, reduction of the uncertainty in these processes is necessary to evaluate gas-oxidant-aerosol coupling accurately. Our simulations also show that the sensitivity of aerosols to changes in emissions is enhanced by 50-100% when OA formation and BC aging processes are resolved in the model. Sensitivity simulations show that the increase of NOx emissions from 1850 to 2000 explains 70% (40%) of the enhancement of aerosol mass concentrations (direct radiative effects) over East Asia during that period through enhancement of oxidant concentrations and that this estimation is sensitive to the representation of OA formation and BC aging processes. Our results demonstrate the importance of simultaneous simulation of gas-oxidant-aerosol coupling and detailed aerosol processes. The impact of NOx emissions on aerosol formation will be a key to formulating effective emission reduction strategies such as BC mitigation and aerosol reduction policies in East Asia.

  16. Upper tropospheric ice sensitivity to sulfate geoengineering

    Science.gov (United States)

    Visioni, Daniele; Pitari, Giovanni; Mancini, Eva

    2017-04-01

    In light of the Paris Agreement which aims to keep global warming under 2 °C in the next century and considering the emission scenarios produced by the IPCC for the same time span, it is likely that to remain below that threshold some kind of geoengineering technique will have to be deployed. Amongst the different methods, the injection of sulfur into the stratosphere has received much attention considering its effectiveness and affordability. Aside from the rather well established surface cooling sulfate geoengineering (SG) would produce, the investigation on possible side-effects of this method is still ongoing. For instance, some recent studies have investigated the effect SG would have on upper tropospheric cirrus clouds, expecially on the homogenous freezing mechanisms that produces the ice particles (Kuebbeler et al., 2012). The goal of the present study is to better understand the effect of thermal and dynamical anomalies caused by SG on the formation of ice crystals via homogeneous freezing by comparing a complete SG simulation with a RCP4.5 reference case and with a number of sensitivity studies where atmospheric temperature changes in the upper tropospheric region are specified in a schematic way as a function of the aerosol driven stratospheric warming and mid-lower tropospheric cooling. These changes in the temperature profile tend to increase atmospheric stabilization, thus decreasing updraft and with it the amount of water vapor available for homogeneous freezing in the upper troposphere. However, what still needs to be assessed is the interaction between this dynamical effect and the thermal effects of tropospheric cooling (which would increase ice nucleation rates) and stratospheric warming (which would probably extend to the uppermost troposphere via SG aerosol gravitational settling, thus reducing ice nucleation rates), in order to understand how they combine together. Changes in ice clouds coverage could be important for SG, because cirrus ice

  17. Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

    Directory of Open Access Journals (Sweden)

    G. J. Roelofs

    2006-01-01

    Full Text Available A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by cloud droplets growing on particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.

  18. Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

    Directory of Open Access Journals (Sweden)

    G. J. Roelofs

    2006-01-01

    Full Text Available A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.

  19. A characterization of Arctic aerosols on the basis of aerosol optical depth and black carbon measurements

    Directory of Open Access Journals (Sweden)

    R. S. Stone

    2014-06-01

    Full Text Available Abstract Aerosols, transported from distant source regions, influence the Arctic surface radiation budget. When deposited on snow and ice, carbonaceous particles can reduce the surface albedo, which accelerates melting, leading to a temperature-albedo feedback that amplifies Arctic warming. Black carbon (BC, in particular, has been implicated as a major warming agent at high latitudes. BC and co-emitted aerosols in the atmosphere, however, attenuate sunlight and radiatively cool the surface. Warming by soot deposition and cooling by atmospheric aerosols are referred to as “darkening” and “dimming” effects, respectively. In this study, climatologies of spectral aerosol optical depth AOD (2001–2011 and Equivalent BC (EBC (1989–2011 from three Arctic observatories and from a number of aircraft campaigns are used to characterize Arctic aerosols. Since the 1980s, concentrations of BC in the Arctic have decreased by more than 50% at ground stations where in situ observations are made. AOD has increased slightly during the past decade, with variations attributed to changing emission inventories and source strengths of natural aerosols, including biomass smoke and volcanic aerosol, further influenced by deposition rates and airflow patterns.

  20. Direct radiative effect by multicomponent aerosol over China

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Xin; Song, Yu; Zhao, Chun; Cai, Xuhui; Zhang, Hongsheng; Zhu, Tong

    2015-05-01

    The direct radiative effect (DRE) of multiple aerosol species (sulfate, nitrate, ammonium, black carbon (BC), organic carbon (OC), and mineral aerosol) and their spatiotemporal variations over China were investigated using a fully coupled meteorology–chemistry model (WRF-Chem) for the entire year of 2006. We made modifications to improve model performance, including updating land surface parameters, improving the calculation of transition metal-catalyzed oxidation of SO2, and adding in heterogeneous reactions between mineral aerosol and acid gases. The modified model well reproduced the magnitude, seasonal pattern, and spatial distribution of the measured meteorological conditions, concentrations of PM10 and its components, and aerosol optical depth (AOD). A diagnostic iteration method was used to estimate the overall DRE of aerosols and contributions from different components. At the land surface, all kinds of aerosol species reduced the incident net radiation flux with a total DRE of 10.2 W m-2 over China. Aerosols significantly warm the atmosphere with the national mean DRE of +10.8 W m-2. BC was the leading radiative-heating component (+8.7 W m-2), followed by mineral aerosol (+1.1 W m-2). At the top of the atmosphere (TOA), BC introduced the largest radiative perturbation (+4.5 W m-2), followed by sulfate (-1.4 W m-2). The overall perturbation of aerosols on radiation transfer is quite small over China, demonstrating the counterbalancing effect between scattering and adsorbing aerosols. Aerosol DRE at the TOA had distinct seasonality, generally with a summer maximum and winter minimum, mainly determined by mass loadings, hygroscopic growth, and incident radiation flux.

  1. Modelled and observed changes in aerosols and surface solar radiation over Europe between 1960 and 2009

    Science.gov (United States)

    Turnock, S. T.; Spracklen, D. V.; Carslaw, K. S.; Mann, G. W.; Woodhouse, M. T.; Forster, P. M.; Haywood, J.; Johnson, C. E.; Dalvi, M.; Bellouin, N.; Sanchez-Lorenzo, A.

    2015-08-01

    Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry-climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry-climate model for the period 1960-2009 against extensive ground-based observations of sulfate aerosol mass (1978-2009), total suspended particle matter (SPM, 1978-1998), PM10 (1997-2009), aerosol optical depth (AOD, 2000-2009), aerosol size distributions (2008-2009) and surface solar radiation (SSR, 1960-2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = -0.4), SPM (NMBF = -0.9), PM10 (NMBF = -0.2), aerosol number concentrations (N30 NMBF = -0.85; N50 NMBF = -0.65; and N100 NMBF = -0.96) and AOD (NMBF = -0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of -68 % (-78 %), SPM of -42 % (-20 %), PM10 of -9 % (-8 %) and AOD of -11 % (-14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990-2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m-2 during the period 1970-2009 in response to changes in anthropogenic emissions and aerosol concentrations.

  2. MODELING THE EFFECTS OF ANTHROPOGENIC SULFATE IN CLIMATE CHANGE BY USING A REGIONAL CLIMATE MODEL

    Institute of Scientific and Technical Information of China (English)

    高学杰; 林一骅; 赵宗慈

    2003-01-01

    Effects of aerosol with focus on the direct climate effect of anthropogenic sulfate aerosol under 2×CO2 condition were investigated by introducing aerosol distribution into the latest version of RegCM2. Two experiments, first run(2×CO2 + 0 aerosol concentration) and second run (2×CO2 + aerosol distribution), were made for 5 years respectively. Preliminary analysis shows that the direct climate effect of aerosol might cause a decrease of surface air temperature.The decrease might be larger in winter and in South China. The regional-averaged monthly precipitation might also decrease in most of the months due to the effect. The annual mean change of precipitation might be a decrease in East and an increase in West China. But the changes of both temperature and precipitation simulated were much smaller as compared to the greenhouse effect.

  3. TOMS Absorbing Aerosol Index

    Data.gov (United States)

    Washington University St Louis — TOMS_AI_G is an aerosol related dataset derived from the Total Ozone Monitoring Satellite (TOMS) Sensor. The TOMS aerosol index arises from absorbing aerosols such...

  4. Direct Sulfation of Limestone

    DEFF Research Database (Denmark)

    Hu, Guilin; Dam-Johansen, Kim; Wedel, Stig

    2007-01-01

    The direct sulfation of limestone was studied in a laboratory fixed-bed reactor. It is found that the direct sulfation of limestone involves nucleation and crystal grain growth of the solid product (anhydrite). At 823 K and at low-conversions (less than about 0.5 %), the influences of SO2, O-2...... and CO2 on the direct sulfation of limestone corresponds to apparent reaction orders of about 0.2, 0.2 and -0.5, respectively. Water is observed to promote the sulfation reaction and increase the apparent reaction orders of SO2 and O-2. The influence of O-2 at high O-2 concentrations (> about 15...... %) becomes negligible. In the temperature interval from 723 K to 973 K, an apparent activation energy of about 104 kJ/mol is observed for the direct sulfation of limestone. At low temperatures and low conversions, the sulfation process is most likely under mixed control by chemical reaction and solid...

  5. Discovery and measurement of an isotopically distinct source of sulfate in Earth's atmosphere.

    Science.gov (United States)

    Dominguez, Gerardo; Jackson, Terri; Brothers, Lauren; Barnett, Burton; Nguyen, Bryan; Thiemens, Mark H

    2008-09-01

    Sulfate (SO(4)) and its precursors are significant components of the atmosphere, with both natural and anthropogenic sources. Recently, our triple-isotope ((16)O, (17)O, (18)O) measurements of atmospheric sulfate have provided specific insights into the oxidation pathways leading to sulfate, with important implications for models of the sulfur cycle and global climate change. Using similar isotopic measurements of aerosol sulfate in a polluted marine boundary layer (MBL) and primary sulfate (p-SO(4)) sampled directly from a ship stack, we quantify the amount of p-SO(4) found in the atmosphere from ships. We find that ships contribute between 10% and 44% of the non-sea-salt sulfate found in fine [diameter (D) international maritime law, and atmospheric chemistry.

  6. Horizontal distributions of aerosol constituents and their mixing states in Antarctica during the JASE traverse

    Directory of Open Access Journals (Sweden)

    K. Hara

    2014-05-01

    Full Text Available Measurements of aerosol number concentrations and direct aerosol sampling were conducted on continental Antarctica during the traverse of Japanese–Swedish joint Antarctic expedition (JASE from 14 November 2007 until 24 January 2008. Aerosol concentrations in background conditions decreased gradually with latitude in inland regions during the traverse. The lowest aerosol number concentrations were 160 L−1 in Dp > 0.3 μm, and 0.5 L−1 in Dp > 2 μm. In contrast, aerosol concentrations reached 3278 L−1 in Dp > 0.3 μm, and 215 L−1 in Dp > 2 μm under strong wind conditions. The estimated aerosol mass concentrations were 0.04–5.7 μg m−3. Single particle analysis of aerosol particles collected during the JASE traverse was conducted using a scanning electron microscope equipped with an energy dispersive X-ray spectrometer. Major aerosol constituents were sulfates in fine mode, and sulfate, sea-salts, modified sea-salts, and fractionated sea-salts in coarse mode. K-rich sulfates, Mg-rich sulfate, Ca-rich sulfates, and minerals were identified as minor aerosol constituents. Sea-salt particles were modified greatly with SO42− and NO3− in coarse mode, and dominantly with SO42− in fine mode during the traverse. Most sea-salt particles in the continental region were modified with sulfate and methanesulfonate near the coast, although NO3− contributed markedly to sea-salt modification in inland areas during summer. Mg-rich sea-salt particles and Mg-free sea-salt particles were present in coarse and fine modes from the coast to inland areas. These sea-salt particles might be associated with sea-salt fractionation on the snow surface of continental Antarctica.

  7. Precambrian Lunar Volcanic Protolife

    Directory of Open Access Journals (Sweden)

    Jack Green

    2009-06-01

    Full Text Available Five representative terrestrial analogs of lunar craters are detailed relevant to Precambrian fumarolic activity. Fumarolic fluids contain the ingredients for protolife. Energy sources to derive formaldehyde, amino acids and related compounds could be by flow charging, charge separation and volcanic shock. With no photodecomposition in shadow, most fumarolic fluids at 40 K would persist over geologically long time periods. Relatively abundant tungsten would permit creation of critical enzymes, Fischer-Tropsch reactions could form polycyclic aromatic hydrocarbons and soluble volcanic polyphosphates would enable assembly of nucleic acids. Fumarolic stimuli factors are described. Orbital and lander sensors specific to protolife exploration including combined Raman/laser-induced breakdown spectrocsopy are evaluated.

  8. Data assimilation of CALIPSO aerosol observations

    Directory of Open Access Journals (Sweden)

    T. T. Sekiyama

    2010-01-01

    Full Text Available We have developed an advanced data assimilation system for a global aerosol model with a four-dimensional ensemble Kalman filter in which the Level 1B data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO were successfully assimilated for the first time, to the best of the authors' knowledge. A one-month data assimilation cycle experiment for dust, sulfate, and sea-salt aerosols was performed in May 2007. The results were validated via two independent observations: 1 the ground-based lidar network in East Asia, managed by the National Institute for Environmental Studies of Japan, and 2 weather reports of aeolian dust events in Japan. Detailed four-dimensional structures of aerosol outflows from source regions over oceans and continents for various particle types and sizes were well reproduced. The intensity of dust emission at each grid point was also corrected by this data assimilation system. These results are valuable for the comprehensive analysis of aerosol behavior as well as aerosol forecasting.

  9. Fast airborne aerosol size and chemistry measurements above Mexico City and Central Mexico during the MILAGRO campaign

    Directory of Open Access Journals (Sweden)

    P. F. DeCarlo

    2008-07-01

    Full Text Available The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1 was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS. During the campaign the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA and biomass burning (BB are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m−3 (STP ppm−1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006 and Kleinman et al. (2008. The stability of the OA/CO while O/C increases with photochemical age implies a net loss of carbon from the OA. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major regional source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance

  10. Fast airborne aerosol size and chemistry measurements above Mexico City and Central Mexico during the MILAGRO campaign

    Science.gov (United States)

    Decarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.; Zhou, J.; Tomlinson, J.; Collins, D. R.; Knapp, D.; Weinheimer, A. J.; Montzka, D. D.; Campos, T.; Jimenez, J. L.

    2008-07-01

    The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS. During the campaign the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m-3 (STP) ppm-1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2008). The stability of the OA/CO while O/C increases with photochemical age implies a net loss of carbon from the OA. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major regional source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city likely due to

  11. Atmospheric ice nuclei in the Eyjafjallajökull volcanic ash plume

    Directory of Open Access Journals (Sweden)

    H. Bingemer

    2012-01-01

    Full Text Available We have sampled atmospheric ice nuclei (IN and aerosol in Germany and in Israel during spring 2010. IN were analyzed by the static vapor diffusion chamber FRIDGE, as well as by electron microscopy. During the Eyjafjallajökull volcanic eruption of April 2010 we have measured the highest ice nucleus number concentrations (>600 l−1 in our record of 2 yr of daily IN measurements in central Germany. Even in Israel, located about 5000 km away from Iceland, IN were as high as otherwise only during desert dust storms. The fraction of aerosol activated as ice nuclei at −18 °C and 119% rhice and the corresponding area density of ice-active sites per aerosol surface were considerably higher than what we observed during an intense outbreak of Saharan dust over Europe in May 2008.

    Pure volcanic ash accounts for at least 53–68% of the 239 individual ice nucleating particles that we collected in aerosol samples from the event and analyzed by electron microscopy. Volcanic ash samples that had been collected close to the eruption site were aerosolized in the laboratory and measured by FRIDGE. Our analysis confirms the relatively poor ice nucleating efficiency (at −18 °C and 119% ice-saturation of such "fresh" volcanic ash, as it had recently been found by other workers. We find that both the fraction of the aerosol that is active as ice nuclei as well as the density of ice-active sites on the aerosol surface are three orders of magnitude larger in the samples collected from ambient air during the volcanic peaks than in the aerosolized samples from the ash collected close to the eruption site. From this we conclude that the ice-nucleating properties of volcanic ash may be altered substantially by aging and processing during long-range transport in the atmosphere, and that global volcanism deserves further attention as a potential source of atmospheric ice nuclei.

  12. Analysis of anions in ambient aerosols by microchip capillary electrophoresis.

    Science.gov (United States)

    Liu, Yan; MacDonald, David A; Yu, Xiao-Ying; Hering, Susanne V; Collett, Jeffrey L; Henry, Charles S

    2006-11-01

    We describe a microchip capillary electrophoresis method for the analysis of nitrate and sulfate in ambient aerosols. Investigating the chemical composition of ambient aerosol particles is essential for understanding their sources and effects. Significant progress has been made towards developing mass spectrometry-based instrumentation for rapid qualitative analysis of aerosols. Alternative methods for rapid quantification of selected high abundance compounds are needed to augment the capacity for widespread routine analysis. Such methods could provide much higher temporal and spatial resolution than can be achieved currently. Inorganic anions comprise a large percentage of particulate mass, with nitrate and sulfate among the most abundant species. While ion chromatography has proven very useful for analyzing extracts of time-integrated ambient aerosol samples collected on filters and for semi-continuous, on-line particle composition measurements, there is a growing need for development of new compact, inexpensive approaches to routine on-line aerosol ion analysis for deployment in spatially dense, atmospheric measurement networks. Microchip capillary electrophoresis provides the necessary speed and portability to address this need. In this report, on-column contact conductivity detection is used with hydrodynamic injection to create a simple microchip instrument for analysis of nitrate and sulfate. On-column contact conductivity detection was achieved using a Pd decoupler placed upstream from the working electrodes. Microchips containing two Au or Pd working electrodes showed a good linear range (5-500 microM) and low limits-of-detection for sulfate and nitrate, with Au providing the lowest detection limits (1 microM) for both ions. The completed microchip system was used to analyze ambient aerosol filter samples. Nitrate and sulfate concentrations measured by the microchip matched the concentrations measured by ion chromatography.

  13. Aerosol Observation System

    Data.gov (United States)

    Oak Ridge National Laboratory — The aerosol observation system (AOS) is the primary Atmospheric Radiation Measurement (ARM) platform for in situ aerosol measurements at the surface. The principal...

  14. Aurorae and Volcanic Eruptions

    Science.gov (United States)

    2001-06-01

    Thermal-IR Observations of Jupiter and Io with ISAAC at the VLT Summary Impressive thermal-infrared images have been obtained of the giant planet Jupiter during tests of a new detector in the ISAAC instrument on the ESO Very Large Telescope (VLT) at the Paranal Observatory (Chile). . They show in particular the full extent of the northern auroral ring and part of the southern aurora. A volcanic eruption was also imaged on Io , the very active inner Jovian moon. Although these observations are of an experimental nature, they demonstrate a great potential for regular monitoring of the Jovian magnetosphere by ground-based telescopes together with space-based facilities. They also provide the added benefit of direct comparison with the terrestrial magnetosphere. PR Photo 21a/01 : ISAAC image of Jupiter (L-band: 3.5-4.0 µm) . PR Photo 21b/01 : ISAAC image of Jupiter (Narrow-band 4.07 µm) . PR Photo 21c/01 : ISAAC image of Jupiter (Narrow-band 3.28 µm) . PR Photo 21d/01 : ISAAC image of Jupiter (Narrow-band 3.21 µm) . PR Photo 21e/01 : ISAAC image of the Jovian aurorae (false-colour). PR Photo 21f/01 : ISAAC image of volcanic activity on Io . Addendum : The Jovian aurorae and polar haze. Aladdin Meets Jupiter Thermal-infrared images of Jupiter and its volcanic moon Io have been obtained during a series of system tests with the new Aladdin detector in the Infrared Spectrometer And Array Camera (ISAAC) , in combination with an upgrade of the ESO-developed detector control electronics IRACE. This state-of-the-art instrument is attached to the 8.2-m VLT ANTU telescope at the ESO Paranal Observatory. The observations were made on November 14, 2000, through various filters that isolate selected wavebands in the thermal-infrared spectral region [1]. They include a broad-band L-filter (wavelength interval 3.5 - 4.0 µm) as well as several narrow-band filters (3.21, 3.28 and 4.07 µm). The filters allow to record the light from different components of the Jovian atmosphere

  15. Lung problems and volcanic smog

    Science.gov (United States)

    ... releases gases into the atmosphere. Volcanic smog can irritate the lungs and make existing lung problems worse. ... deep into the lungs. Breathing in volcanic smog irritates the lungs and mucus membranes. It can affect ...

  16. Evolution of Organic Aerosols in the Atmosphere.

    Energy Technology Data Exchange (ETDEWEB)

    Jimenez, J. L.; Canagaratna, M. R.; Donahue, N. M.; Prevot, A. S. H.; Zhang, Qi; Kroll, Jesse H.; DeCarlo, Peter F.; Allan, James D.; Coe, H.; Ng, N. L.; Aiken, Allison; Docherty, Kenneth S.; Ulbrich, Ingrid M.; Grieshop, A. P.; Robinson, A. L.; Duplissy, J.; Smith, J. D.; Wilson, K. R.; Lanz, V. A.; Hueglin, C.; Sun, Y. L.; Tian, J.; Laaksonen, A.; Raatikainen, T.; Rautiainen, J.; Vaattovaara, P.; Ehn, M.; Kulmala, M.; Tomlinson, Jason M.; Collins, Donald R.; Cubison, Michael J.; Dunlea, E. J.; Huffman, John A.; Onasch, Timothy B.; Alfarra, M. R.; Williams, Paul I.; Bower, K.; Kondo, Yutaka; Schneider, J.; Drewnick, F.; Borrmann, S.; Weimer, S.; Demerjian, K.; Salcedo, D.; Cottrell, L.; Griffin, Robert; Takami, A.; Miyoshi, T.; Hatakeyama, S.; Shimono, A.; Sun, J. Y.; Zhang, Y. M.; Dzepina, K.; Kimmel, Joel; Sueper, D.; Jayne, J. T.; Herndon, Scott C.; Trimborn, Achim; Williams, L. R.; Wood, Ezra C.; Middlebrook, A. M.; Kolb, C. E.; Baltensperger, Urs; Worsnop, Douglas R.

    2009-12-11

    Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework that describes the atmospheric evolution of OA and is constrained and motivated by new, high time resolution, experimental characterizations of their composition, volatility, and oxidation state. OA and OA-precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of large amounts of oxygenated organic aerosol (OOA) mass that has comparable concentrations to sulfate aerosol over the Northern Hemisphere. Our new model framework captures the dynamic aging behavior observed in the atmosphere and the laboratory and can serve as a basis for improving parameterizations in regional and global models.

  17. Volcanism and Oil & Gas In Northeast China

    Institute of Scientific and Technical Information of China (English)

    Shan Xuanlong

    2000-01-01

    Based on study on the relation with volcanic rock and oil & gas in Songliao Basin and Liaohe Basin in northeast China, author proposes that material from deep by volcanism enrichs the resources in basins, that heat by volcanism promotes organic matter transforming to oil and gas, that volcanic reservoir is fracture, vesicular, solution pore, intercrystal pore.Lava facies and pyroclastic facies are favourable reservoir. Mesozoic volcanic reservoir is majority of intermediate, acid rock,but Cenozoic volcanic reservoir is majority of basalt. Types of oil and gas pool relating to volcanic rock include volcanic fracture pool, volcanic unconformity pool, volcanic rock - screened pool, volcanic darpe structural pool.

  18. Overview of ACE-Asia Spring 2001 Investigations on Aerosol Radiative Effects and Related Aerosol Properties

    Science.gov (United States)

    Russell, Philip B.; Valero, F. P. J.; Flatau, P. J.; Bergin, M.; Holben, B.; Nakajima, T.; Pilewskie, P.; Bergstrom, R.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    depth gradient, with AOD(500 nm) extremes from 0.1 to 1.1. On the Pacific transit from Honolulu to Hachijo AOD(500 nm) averaged 0.2, including increases to 0.4 after several storms, suggesting the strong impact of wind-generated seasalt. The AOD maximum, found in the Sea of Japan, was influenced by dust and anthropogenic sources. (4) In Beijing, single scattering albedo retrieved from AERONET sun-sky radiometry yielded midvisible SSA=0.88 with strong wavelength dependence, suggesting a significant black carbon component. SSA retrieved during dust episodes was approx. 0.90 and variable but wavelength neutral reflecting the presence of urban haze with the dust. Downwind at Anmyon Island SSA was considerably higher, approx. 0.94, but wavelength neutral for dust episodes and spectrally dependent during non dust periods. (5) Satellite retrievals show major aerosol features moving from Asia over the Pacific; however, determining seasonal-average aerosol effects is hampered by sampling frequency and large-scale cloud systems that obscure key parts of aerosol patterns. Preliminary calculations using, satellite-retrieved AOD fields and initial ACE-Asia aerosol properties (including sulfates, soot, and dust) yield clear-sky aerosol radiative effects in the seasonal-average ACE-Asia plume exceeding those of manmade greenhouse gases. Quantifying all-sky direct aerosol radiative effects is complicated by the need to define the height of absorbing aerosols with respect to cloud decks.

  19. Offsetting features of climate responses to anthropogenic sulfate and black carbon direct radiative forcings

    Science.gov (United States)

    Ocko, I.; Ramaswamy, V.

    2012-12-01

    The two most prominent anthropogenic aerosols—sulfate and black carbon—affect Earth's radiation budget in opposing ways. Here we examine how these aerosols independently impact the climate, by simulating climate responses from pre-industrial times (1860) to present-day (2000) for isolated sulfate and black carbon direct radiative forcings. The NOAA Geophysical Fluid Dynamics Laboratory CM2.1 global climate model is employed with prescribed distributions of externally mixed aerosols. We find that sulfate and black carbon induce opposite effects for a myriad of climate variables. Sulfate (black carbon) is generally cooling (warming), shifts the ITCZ southward (northward), reduces (enhances) the SH Hadley Cell, enhances (reduces) the NH Hadley Cell, and increases (decreases) total sea ice volume. Individually, sulfate and black carbon affect Hadley Cell circulation more than long-lived greenhouse gases, but the net aerosol effect is a weakened response due to opposite behaviors somewhat canceling out the individual effects. Because anthropogenic aerosols are a critical contributor to Earth's climate conditions, this study has implications for future climate changes as well.

  20. Modeling volcanic ash dispersal

    CERN Document Server

    CERN. Geneva

    2010-01-01

    The assessment of volcanic fallout hazard is an important scientific, economic, and political issue, especially in densely populated areas. From a scientific point of view, considerable progress has been made during the last two decades through the use of increasingly powerful computational models and capabilities. Nowadays, models are used to quantify hazard...

  1. In-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010

    Directory of Open Access Journals (Sweden)

    E. Harris

    2014-01-01

    Full Text Available In-cloud production of sulfate modifies the aerosol size distribution, with important implications for the magnitude of indirect and direct aerosol cooling and the impact of SO2 emissions on the environment. We investigate which sulfate sources dominate the in-cloud addition of sulfate to different particle classes as an air parcel passes through an orographic cloud. Sulfate aerosol, SO2 and H2SO4 were collected upwind, in-cloud and downwind of an orographic cloud for three cloud measurement events during the Hill Cap Cloud Thuringia campaign in Autumn, 2010 (HCCT-2010. Combined SEM and NanoSIMS analysis of single particles allowed the δ34S of particulate sulfate to be resolved for particle size and type. The most important in-cloud SO2 oxidation pathway at HCCT-2010 was aqueous oxidation catalysed by transition metal ions (TMI catalysis, which was shown with single particle isotope analyses to occur primarily in cloud droplets nucleated on coarse mineral dust. In contrast, direct uptake of H2SO4(g and ultrafine particulate were the most important sources modifying fine mineral dust, increasing its hygroscopicity and facilitating activation. Sulfate addition to "mixed" particles (secondary organic and inorganic aerosol and coated soot was dominated by in-cloud aqueous SO2 oxidation by H2O2 and direct uptake of H2SO4(g and ultrafine particle sulfate, depending on particle size mode and time of day. These results provide new insight into in-cloud sulfate production mechanisms, and show the importance of single particle measurements and models to accurately assess the environmental effects of cloud processing.

  2. Global monsoon precipitation responses to large volcanic eruptions.

    Science.gov (United States)

    Liu, Fei; Chai, Jing; Wang, Bin; Liu, Jian; Zhang, Xiao; Wang, Zhiyuan

    2016-04-11

    Climate variation of global monsoon (GM) precipitation involves both internal feedback and external forcing. Here, we focus on strong volcanic forcing since large eruptions are known to be a dominant mechanism in natural climate change. It is not known whether large volcanoes erupted at different latitudes have distinctive effects on the monsoon in the Northern Hemisphere (NH) and the Southern Hemisphere (SH). We address this issue using a 1500-year volcanic sensitivity simulation by the Community Earth System Model version 1.0 (CESM1). Volcanoes are classified into three types based on their meridional aerosol distributions: NH volcanoes, SH volcanoes and equatorial volcanoes. Using the model simulation, we discover that the GM precipitation in one hemisphere is enhanced significantly by the remote volcanic forcing occurring in the other hemisphere. This remote volcanic forcing-induced intensification is mainly through circulation change rather than moisture content change. In addition, the NH volcanic eruptions are more efficient in reducing the NH monsoon precipitation than the equatorial ones, and so do the SH eruptions in weakening the SH monsoon, because the equatorial eruptions, despite reducing moisture content, have weaker effects in weakening the off-equatorial monsoon circulation than the subtropical-extratropical volcanoes do.

  3. Syndecan heparan sulfate proteoglycans

    DEFF Research Database (Denmark)

    Gomes, Angélica Maciel; Sinkeviciute, Dovile; Multhaupt, Hinke A.B.

    2016-01-01

    Virtually all animal cells express heparan sulfate proteoglycans on the cell surface and in the extracellular matrix. Syndecans are a major group of transmembrane proteoglycans functioning as receptors that mediate signal transmission from the extracellular microenvironment to the cell. Their hep......Virtually all animal cells express heparan sulfate proteoglycans on the cell surface and in the extracellular matrix. Syndecans are a major group of transmembrane proteoglycans functioning as receptors that mediate signal transmission from the extracellular microenvironment to the cell....... Their heparan sulfate chains, due to their vast structural diversity, interact with a wide array of ligands including potent regulators of adhesion, migration, growth and survival. Frequently, ligands interact with cell surface heparan sulfate in conjunction with high affinity receptors. The consequent...... signaling can therefore be complex, but it is now known that syndecans are capable of independent signaling. This review is divided in two sections, and will first discuss how the assembly of heparan sulfate, the anabolic process, encodes information related to ligand binding and signaling. Second, we...

  4. Characteristics of Carbonaceous and Ionic Species and Direct Aerosol Forcing of the Aerosols over Gosan, Jeju, Korea

    Science.gov (United States)

    Kim, N.; Kim, Y.; Kang, C.

    2010-12-01

    Carbonaceous aerosols, consisting of elemental carbon (EC) are emitted into the atmosphere through incomplete combustion of biomass and fossil fuel. It directly warms the air by absorbing solar radiation. Another major pollutant emitted by fossil fuel combustion is SO2, which result in the formation of particulate sulfate (SO42-) compounds, contribute substantially to cool the air by scattering solar radiation. Therefore, carbonaceous and sulfate aerosols play an important role in regulating the amount of solar radiation absorbed by the earth atmosphere. (Charlson et al. 1992; Jacobson, 2004; Khan et al., 2010) Carbonaceous and sulfate aerosols are both temporally and spatially variable. Northeast Asia is characterized by high energy consumption. China, Japan, and South Korea have consumed 16.8%, 4.7%, and 2.1% of the world total primary energy, respectively in 2007 (BP, 2008). Consequently, there are resultant huge emissions of anthropogenic air pollutants. Therefore, the effect on climate forcing by carbonaceous and sulfate aerosols are even more important in this region. In this study, PM2.5 intensive measurement data for 18 separate periods at Gosan, Jeju, Korea from 1994 to 2006 were analyzed. Gosan is one of the cleanest areas in Korea and an excellent location to study the ambient aerosols in Northeast Asia (Kim et al., 2009). The characteristics of carbonaceous aerosols and anthropogenic ions such as SO42-, NO3-, NH4+ were analyzed. Also, direct aerosol forcing due to EC and SO42- were calculated. The net aerosol forcing were about -0.5 W m-2 to -0.1 W m-2 at Gosan. References BP, www.bp.com/statisticalreview, 2008. Charlson, R.J., Schwartz, S.E., Hales, J.M., Cess, R.D., Coakley, J.A.Jr., Hansen, J.E., and Hofmann, D.J. (1992) Climate Forcing by Anthropogenic Aerosols, Science, 255, 423-430. Jacobson, M.Z. (2004) Climate response of fossil fuel and biofuel soot, accounting for soot's feedback to snow and sea ice albedo and emissivity, Journal of

  5. Global climate forcing of aerosols embodied in international trade

    Science.gov (United States)

    Lin, Jintai; Tong, Dan; Davis, Steven; Ni, Ruijing; Tan, Xiaoxiao; Pan, Da; Zhao, Hongyan; Lu, Zifeng; Streets, David; Feng, Tong; Zhang, Qiang; Yan, Yingying; Hu, Yongyun; Li, Jing; Liu, Zhu; Jiang, Xujia; Geng, Guannan; He, Kebin; Huang, Yi; Guan, Dabo

    2016-10-01

    International trade separates regions consuming goods and services from regions where goods and related aerosol pollution are produced. Yet the role of trade in aerosol climate forcing attributed to different regions has never been quantified. Here, we contrast the direct radiative forcing of aerosols related to regions' consumption of goods and services against the forcing due to emissions produced in each region. Aerosols assessed include black carbon, primary organic aerosol, and secondary inorganic aerosols, including sulfate, nitrate and ammonium. We find that global aerosol radiative forcing due to emissions produced in East Asia is much stronger than the forcing related to goods and services ultimately consumed in that region because of its large net export of emissions-intensive goods. The opposite is true for net importers such as Western Europe and North America: global radiative forcing related to consumption is much greater than the forcing due to emissions produced in these regions. Overall, trade is associated with a shift of radiative forcing from net importing to net exporting regions. Compared to greenhouse gases such as carbon dioxide, the short atmospheric lifetimes of aerosols cause large localized differences between consumption- and production-related radiative forcing. International efforts to reduce emissions in the exporting countries will help alleviate trade-related climate and health impacts of aerosols while lowering global emissions.

  6. Aerosol light scattering measurements as a function of relative humidity.

    Science.gov (United States)

    Day, D E; Malm, W C; Kreidenweis, S M

    2000-05-01

    The hygroscopic nature of atmospheric fine aerosol was investigated at a rural site in the Great Smoky Mountains National Park during July and August 1995. Passing the sample aerosol through an inlet, which housed an array of Perma Pure diffusion dryers, controlled the sample aerosol's relative humidity (RH). After conditioning the aerosol sample in the inlet, the light scattering coefficient and the aerosol size distribution were simultaneously measured. During this study, the conditioned aerosol's humidity ranged between 5% < RH < 95%. Aerosol response curves were produced using the ratio bspw/bspd; where bspw is the scattering coefficient measured at some RH greater than 20% and bspd is the scattering coefficient of the "dry" aerosol. For this work, any sample RH values below 15% were considered dry. Results of this investigation showed that the light scattering ratio increased continuously and smoothly over the entire range of relative humidity. The magnitude of the ratio at a particular RH value, however, varied considerably in time, particularly for RH values greater than approximately 60%. Curves of the scattering coefficient ratios as a function of RH were generated for each day and compared to the average 12-hour chemical composition of the aerosol. This comparison showed that for any particular RH value the ratio was highest during time periods of high sulfate concentrations and lowest during time periods of high soil or high organic carbon concentrations.

  7. Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

    Directory of Open Access Journals (Sweden)

    B. Croft

    2009-10-01

    Full Text Available A diagnostic nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. Sensitivity studies are presented, which compare aerosol concentrations, and deposition between a variety of in-cloud scavenging approaches, including prescribed fractions, several diagnostic schemes, and a prognostic aerosol cloud processing treatment that passes aerosol in-droplet and in-ice crystal concentrations between model time steps. For one sensitivity study, assuming 100% of the in-cloud aerosol is scavenged into the cloud droplets and ice crystals, the annual global mean accumulation mode number burden is decreased by 65%, relative to a simulation with prognostic aerosol cloud processing. Diagnosing separate nucleation scavenging ratios for aerosol number and mass distributions, as opposed to equating the aerosol mass scavenging to the number scavenging ratios, reduces the annual global mean sulfate burden by near to 10%. The annual global mean sea salt burden is 30% lower for the diagnostic approach, which does not carry aerosol in-droplet and in-crystal concentrations between model time-steps as compared to the prognostic scheme. Implementation of in-cloud impaction scavenging reduced the annual, global mean black carbon burden by 30% for the prognostic aerosol cloud processing scheme. Better agreement with observations of black carbon profiles from aircraft (changes near to one order of magnitude for mixed phase clouds, 210Pb surface layer concentrations and wet deposition, and the geographic distribution of aerosol optical depth are found for the new diagnostic scavenging as compared to prescribed ratio

  8. A study of the relationship between anthropogenic sulfate and cloud drop nucleation

    Energy Technology Data Exchange (ETDEWEB)

    Chuang, C. C..; Penner, J. E.

    1994-09-01

    This document investigates the relationship between anthropogenic sulfate-containing aerosols and the condensationally produced cloud drops. The changes in aerosol size distribution associated with anthropogenic sulfur emissions may increase the number of cloud drops with subsequent influence on cloud albedo and climate. It has been suggested that the increase in CCN in industrial regions might explain why the Northern Hemisphere has not been warming as rapidly as the Southern Hemisphere over the last 50 Years (Wigley, 1989). In reality, the aerosol size distribution is the result of processes working simultaneously and continuously with such sources as sulfur, soot, particulate organic carbon, nitrate, ammonium, etc. Instead of applying a complete aerosol model to investigate the effect of anthropogenic sulfur emissions on the aerosol size distribution, we simply derived the anthropogenic sulfate-containing aerosol distribution by assuming that 75% of the anthropogenic was formed through aqueous-phase oxidation and the remaining 25% condensed onto a Prescribed preexisting particle distribution. Uncertainties may arise from the assumed fraction of sulfate produced by condensation and in cloud oxidation. In addition, new particle formation through homogeneous nucleation of H{sub 2}SO{sub 4}/H{sub 2}O is ignored in this paper.

  9. The direct radiative forcing effects of aerosols on the climate in California

    Science.gov (United States)

    Du, Hui

    The Weather Research and Forecast (WRF) model is used to explore the influence of aerosol direct radiative effects on regional climate of California. Aerosol data is provided by the MOZART global chemistry transport model and includes sulfate, black carbon, organic carbon, dust and sea salt. To investigate the sensitivity of aerosol radiative effects to different aerosol species and to the quantity of sulfate and dust, tests are conducted by using different combinations of aerosols and by resetting the quantity of sulfate and dust. The model results show that all the considered aerosols could have a cooling effect of one half to one degree in terms of temperature and that dust and sulfate are the most important aerosols. However, large uncertainties exist. The results suggest that the dust from MOZART is greatly overestimated over the simulation domain. The single scattering albedo (SSA) values of dust used in some global climate models are likely underestimated compared to recent studies on dust optical properties and could result in overestimating the corresponding cooling effects by approximately 0.1 degree. Large uncertainties exist in estimating the roles of different forcing factors which are causing the observed temperature change in the past century in California.

  10. Gravimetric analysis, ionic composition, and associated water mass of the marine aerosol

    Science.gov (United States)

    McInnes, L. M.; Quinn, P. K.; Covert, D. S.; Anderson, T. L.

    Measurements of the total aerosol mass and ionic composition were obtained for submicrometer ( Dp ⩽ 1.0 μm) aerosol particles from the remote Pacific boundary layer by gravimetric and ion chromatography analysis. Discrepancies were found to exist between the absolute mass determined by the separate techniques suggesting aerosol components in addition to sea salt and sulfate particles exist at significant mass concentrations. The gravimetric mass was equal to or significantly larger than the sum of the ionic masses, suggesting additional aerosol components contribute between 0 and 75% of the submicrometer aerosol mass. Measurements of the elemental composition of individual particles by electron microscopy confirmed the presence of mineral and carbonaceous particles which contributed 0-86% of the total number concentration for the particle-size range of interest. The relative number of submicrometer sulfate particles with respect to the total was low during periods with the largest discrepancy between the gravimetric and ionic mass. The amount of water associated with the submicrometer aerosol at 47% relative humidity made up 29% of the total aerosol mass collected on the filters (and 9% of the total mass at 35%). Laboratory studies determined the relative amount of water associated with sea salt, sulfate, and sodium chloride particles on a filter substrate, with sea-salt particles containing 27% water and ammonium sulfate particles containing only 4% water at 40% r.h.

  11. X-Ray Microspectroscopic Investigations of Remote Aerosol Composition and Changes in Aerosol Microstructure and Phase State upon Hydration

    Science.gov (United States)

    Andreae, M. O.; Artaxo, P.; Bechtel, M.; Förster, J. D.; Kilcoyne, A. L. D.; Krüger, M. L.; Pöhlker, C.; Saturno, J.; Weigand, M.; Wiedemann, K. T.

    2014-12-01

    Atmospheric aerosols play a crucial role in the Earth's climate system and hydrological cycle by scattering and absorbing sunlight and affecting the formation and development of clouds and precipitation. Our research focuses on aerosols in remote regions, in order to characterize the properties and sources of natural aerosol particles and the extent of human perturbations of the aerosol burden. The phase and mixing state of atmospheric aerosols, and particularly their hygroscopic response to relative humidity (RH) variations, is a central determinant of their atmospheric life cycle and impacts. We present an investigation using X-ray microspectroscopy on submicrometer aerosols under variable RH conditions, showing in situ changes in morphology, microstructure, and phase state upon humidity cycling. We applied Scanning Transmission X-ray Microscopy with Near-Edge X-ray Absorption Fine Structure spectroscopy (STXM-NEXAFS) under variable RH conditions to standard aerosols for a validation of the experimental approach and to internally mixed aerosol particles from the Amazonian rain forest collected during periods with anthropogenic pollution. The measurements were conducted at X-ray microscopes at the synchrotron facilities Advanced Light Source (ALS) in Berkeley, USA, and BESSY II in Berlin, Germany. Upon hydration, we observed substantial and reproducible changes in microstructure of the Amazonian particles (internal mixture of secondary organic material, ammoniated sulfate, and soot), which appear as mainly driven by efflorescence and recrystallization of sulfate salts. Multiple solid and liquid phases were found to coexist, especially in intermediate humidity regimes (60-80% RH). This shows that X-ray microspectroscopy under variable RH is a valuable technique to analyze the hygroscopic response of individual ambient aerosol particles. Our initial results underline that RH changes can trigger strong particle restructuring, in agreement with previous studies on

  12. In situ measurements constraining the role of sulphate aerosols in mid-latitude ozone depletion

    Science.gov (United States)

    Fahey, D. W.; Kawa, S. R.; Woodbridge, E. L.; Tin, P.; Wilson, J. C.; Jonsson, H. H.; Dye, J. E.; Baumgardner, D.; Borrmann, S.; Toohey, D. W.

    1993-01-01

    In situ measurements of stratospheric sulphate aerosol, reactive nitrogen and chlorine concentrations at middle latitudes confirm the importance of aerosol surface reactions that convert active nitrogen to a less active, reservoir form. This makes mid-latitude stratospheric ozone less vulnerable to active nitrogen and more vulnerable to chlorine species. The effect of aerosol reactions on active nitrogen depends on gas phase reaction rates, so that increases in aerosol concentration following volcanic eruptions will have only a limited effect on ozone depletion at these latitudes.

  13. Exploring Hawaiian Volcanism

    Science.gov (United States)

    Poland, Michael P.; Okubo, Paul G.; Hon, Ken

    2013-02-01

    In 1912 the Hawaiian Volcano Observatory (HVO) was established by Massachusetts Institute of Technology professor Thomas A. Jaggar Jr. on the island of Hawaii. Driven by the devastation he observed while investigating the volcanic disasters of 1902 at Montagne Pelée in the Caribbean, Jaggar conducted a worldwide search and decided that Hawai`i provided an excellent natural laboratory for systematic study of earthquake and volcano processes toward better understanding of seismic and volcanic hazards. In the 100 years since HVO's founding, surveillance and investigation of Hawaiian volcanoes have spurred advances in volcano and seismic monitoring techniques, extended scientists' understanding of eruptive activity and processes, and contributed to development of global theories about hot spots and mantle plumes.

  14. Exploring Hawaiian volcanism

    Science.gov (United States)

    Poland, Michael P.; Okubo, Paul G.; Hon, Ken

    2013-01-01

    In 1912 the Hawaiian Volcano Observatory (HVO) was established by Massachusetts Institute of Technology professor Thomas A. Jaggar Jr. on the island of Hawaii. Driven by the devastation he observed while investigating the volcanic disasters of 1902 at Montagne Pelée in the Caribbean, Jaggar conducted a worldwide search and decided that Hawai‘i provided an excellent natural laboratory for systematic study of earthquake and volcano processes toward better understanding of seismic and volcanic hazards. In the 100 years since HVO’s founding, surveillance and investigation of Hawaiian volcanoes have spurred advances in volcano and seismic monitoring techniques, extended scientists’ understanding of eruptive activity and processes, and contributed to development of global theories about hot spots and mantle plumes.

  15. Variation of the vertical distribution of Nabro volcano aerosol layers in the stratosphere observed by LIDAR

    Science.gov (United States)

    Noh, Young Min; Shin, Dong Ho; Müller, Detlef

    2017-04-01

    We present results of the vertical distribution variation of volcanic aerosol layers in the upper troposphere and lower stratosphere. The data were taken with our multiwavelength aerosol Raman lidar at Gwangju (35.10° N, 126.53° E), Korea. The volcanic ash particles and gases were released around 12 June 2011 during the eruption of the Nabro volcano (13.37° N, 41.7° E) in Eritrea, east Africa. Forward trajectory computations show that the volcanic aerosols were advected from North Africa to East Asia. The first measurement of the aerosol layer over Korea was on 19 June 2011. The aerosol layers appeared between 15 km and 17 km height asl (above sea level). The maximum value of the aerosol layer of the particle backscatter coefficient (1.5 ± 0.3 Mm-1 sr-1) and the linear particle depolarization ratio at 532 nm (2.2%) were observed at 16.4 km height asl. We continuously probed the upper troposphere and lower stratosphere for this volcanic aerosol layer during the following 6 months, until December 2011. The volcanic aerosol layer showed a single-peak of the particle backscatter coefficient and a comparably narrow vertical thickness at our observation site at the beginning of our observation period (i.e. comparably soon after the initial eruption period). After that initial period the vertical distribution of the plume changed. Multiple peaks and a comparably broad geometrical thickness developed with progressing observation time. The vertical thickness of the volcanic aerosol layer expanded up to 10 km by 3 August 2011. The linear particle depolarization ratios were larger in the lower part of the aerosol layer than the upper part of the aerosol layer. We observed a strong variation of the AOD (aerosol optical depth) in the first two months of our lidar observations. After these two months the AOD gradually decreased with time from September to December 20111 and the maximum particle backscatter coefficients consistently decreased. The corresponding e

  16. Subdiffusion of volcanic earthquakes

    CERN Document Server

    Abe, Sumiyoshi

    2016-01-01

    A comparative study is performed on volcanic seismicities at Mt.Eyjafjallajokull in Iceland and Mt. Etna in Sicily, Italy, from the viewpoint of science of complex systems, and the discovery of remarkable similarities between them regarding their exotic spatio-temporal properties is reported. In both of the volcanic seismicities as point processes, the jump probability distributions of earthquakes are found to obey the exponential law, whereas the waiting-time distributions follow the power law. In particular, a careful analysis is made about the finite size effects on the waiting-time distributions, and accordingly, the previously reported results for Mt. Etna [S. Abe and N. Suzuki, EPL 110, 59001 (2015)] are reinterpreted. It is shown that spreads of the volcanic earthquakes are subdiffusive at both of the volcanoes. The aging phenomenon is observed in the "event-time-averaged" mean-squared displacements of the hypocenters. A comment is also made on presence/absence of long term memories in the context of t...

  17. Aerosols at the Poles: An AeroCom Phase II Multi-Model Evaluation

    Science.gov (United States)

    Sand, M.; Samset, B. H.

    2016-12-01

    Atmospheric aerosols from anthropogenic and natural sources reach the Polar Regions through long-range transport. By scattering and absorbing solar radiation, aerosols perturb the energy balance in the region and may have played a significant role in recent Arctic warming. Aerosols in Polar regions are however, poorly constrained in present day global climate models. Here we compare aerosol burdens from simulations with 16 global aerosol models from the Aerocom phase II model inter-comparison project with available observations at both Poles. We show that the annual mean multi-model median Aerosol Optical Depth (AOD) is not a bad representation of the measured AOD in Arctic, even though the model spread is large. The models tend to underestimate the spring maximum and overestimate the summer/autumn minimum. We also document the geographical distribution and seasonal cycle of aerosol burdens and shortwave anthropogenic direct radiative forcing (DRF) of the total aerosol and the individual aerosol species; black carbon (BC), sulfate, and primary organic aerosols from fossil/bio fuel and biomass burning, dust and sea-salt. A subset of models has also reported nitrate and secondary organic aerosols. The models produce an annual mean median AOD 0.07 in the Arctic and 0.01 the Antarctic. The Arctic modeled annual mean DRF is slightly negative -0.12 Wm-2, dominated by a positive black carbon DRF during spring and a negative sulfate DRF during summer. We perform sensitivity experiments with one of the Aerocom models (GISS modelE) to investigate how regional emissions of BC and sulfate and the lifetime of BC influence the Arctic and Antarctic aerosol burdens.

  18. Natural or anthropogenic? On the origin of atmospheric sulfate deposition in the Andes of southeastern Ecuador

    Directory of Open Access Journals (Sweden)

    S. Makowski Giannoni

    2014-05-01

    Full Text Available Atmospheric sulfur deposition above certain limits can represent a threat to tropical forests, causing nutrient imbalances and mobilizing toxic elements that impact biodiversity and forest productivity. Atmospheric sources of sulfur deposited by precipitation have being roughly identified in only a few lowland tropical forests. Even scarcer are these type of studies in tropical mountain forests, many of them megadiversity hotspots and especially vulnerable to acidic deposition. Here, the topographic complexity and related streamflow condition the origin, type, and intensity of deposition. Furthermore, in regions with a variety of natural and anthropogenic sulfur sources, like active volcanoes and biomass-burning, no source-emission data has been used for determining the contribution of each of them to the deposition. The main goal of the current study is to evaluate sulfate (SO4− deposition by rain and occult precipitation at two topographic locations in a tropical mountain forest of southern Ecuador, and to trace back the deposition to possible emission sources applying back trajectory modeling. To link upwind natural (volcanic and anthropogenic (urban/industrial and biomass-burning sulfur emissions and observed sulfate deposition, we employed state of the art inventory and satellite data, including volcanic passive degassing as well. We conclude that biomass-burning sources generally dominate sulfate deposition at the evaluated sites. Minor sulfate transport occurs during the shifting of the predominant winds to the north and west. Occult precipitation sulfate deposition and likely rain sulfate deposition are mainly linked to biomass-burning emissions from the Amazon lowlands. Volcanic and anthropogenic emissions from the north and west contribute to occult precipitation sulfate deposition at the mountain crest Cerro del Consuelo meteorological station and to rain-deposited sulfate at the upriver mountain-pass El Tiro meteorological station.

  19. Do atmospheric aerosols form glasses?

    Science.gov (United States)

    Zobrist, B.; Marcolli, C.; Pedernera, D. A.; Koop, T.

    2008-09-01

    A new process is presented by which water soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline) solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulfate and mixtures of dicarboxylic acids (M5), of dicarboxylic acids and ammonium sulfate (M5AS), of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K). To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger (≳150 g mol-1) and more hydrophobic organic molecules are more likely to form glasses at intermediate to high relative humidities in the upper troposphere

  20. Do atmospheric aerosols form glasses?

    Directory of Open Access Journals (Sweden)

    D. A. Pedernera

    2008-09-01

    Full Text Available A new process is presented by which water soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulfate and mixtures of dicarboxylic acids (M5, of dicarboxylic acids and ammonium sulfate (M5AS, of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K. To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger (≳150 g mol−1 and

  1. Long-Term Variation of Stratospheric Aerosols Observed With Lidar from 1982 to 2014 Over Tsukuba, Japan

    Science.gov (United States)

    Sakai, Tetsu; Uchino, Osamu; Nagai, Tomohiro; Fujimoto, Toshifumi; Tabata, Isao

    2016-06-01

    The vertical distribution of stratospheric aerosols has been measured with lidars at the Meteorological Research Institute (MRI) over Tsukuba since 1982. After two major volcanic eruptions (Mt. El Chichón in 1982 and Mt. Pinatubo in 1991), stratospheric aerosol loading increased about 50-100 times compared with the background level which was observed for 1997-2000. From 2000 to 2012, a slight increase (5.3% year-1) was observed by some volcanic eruptions. This long-term lidar data have been used for assessing of impact of the stratospheric aerosols on climate and the ozone layer.

  2. Indoor aerosols

    DEFF Research Database (Denmark)

    Morawska, L.; Afshari, Alireza; N. Bae, G.

    2013-01-01

    Motivated by growing considerations of the scale, severity, and risks associated with human exposure to indoor particulate matter, this work reviewed existing literature to: (i) identify state-of-the-art experimental techniques used for personal exposure assessment; (ii) compare exposure levels...... reported for domestic/school settings in different countries (excluding exposure to environmental tobacco smoke and particulate matter from biomass cooking in developing countries); (iii) assess the contribution of outdoor background vs indoor sources to personal exposure; and (iv) examine scientific...... understanding of the risks posed by personal exposure to indoor aerosols. Limited studies assessing integrated daily residential exposure to just one particle size fraction, ultrafine particles, show that the contribution of indoor sources ranged from 19% to 76%. This indicates a strong dependence on resident...

  3. Climatic Impacts of a Volcanic Double Event: 536/540 CE

    Science.gov (United States)

    Toohey, M.; Krüger, K.; Sigl, M.; Stordal, F.; Svensen, H.

    2015-12-01

    Volcanic activity in and around the year 536 CE led to the coldest decade of the Common Era, and has been speculatively linked to large-scale societal crises around the world. Using a coupled aerosol-climate model, with eruption parameters constrained by recently re-dated ice core records and historical observations of the aerosol cloud, we reconstruct the radiative forcing resulting from a sequence of two major volcanic eruptions in 536 and 540 CE. Comparing with a reconstruction of volcanic forcing over the past 1200 years, we estimate that the decadal-scale Northern Hemisphere (NH) extra-tropical radiative forcing from this volcanic "double event" was larger than that of any known period. Earth system model simulations including the volcanic forcing are used to explore the temperature and precipitation anomalies associated with the eruptions, and compared to available proxy records, including maximum latewood density (MXD) temperature reconstructions. Special attention is placed on the decadal persistence of the cooling signal in tree rings, and whether the climate model simulations reproduce such long-term climate anomalies. Finally, the climate model results will be used to explore the probability of socioeconomic crisis resulting directly from the volcanic radiative forcing in different regions of the world.

  4. Radiative absorption enhancement from coatings on black carbon aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Cui, Xinjuan; Wang, Xinfeng; Yang, Lingxiao [Environmental Research Institute, School of Environmental Science and Engineering, Shandong University, Jinan 250100 (China); Chen, Bing, E-mail: bingchen@sdu.edu.cn [Environmental Research Institute, School of Environmental Science and Engineering, Shandong University, Jinan 250100 (China); Chen, Jianmin, E-mail: jmchen@sdu.edu.cn [Environmental Research Institute, School of Environmental Science and Engineering, Shandong University, Jinan 250100 (China); Andersson, August; Gustafsson, Örjan [Department of Environmental Science and Analytical Chemistry (ACES) and the Bolin Centre for Climate Research, Stockholm University, SE-10691 Stockholm (Sweden)

    2016-05-01

    The radiative absorption enhancement of ambient black carbon (BC), by light-refractive coatings of atmospheric aerosols, constitutes a large uncertainty in estimates of climate forcing. The direct measurements of radiative absorption enhancement require the experimentally-removing the coating materials in ambient BC-containing aerosols, which remains a challenge. Here, the absorption enhancement of the BC core by non-absorbing aerosol coatings was quantified using a two-step removal of both inorganic and organic matter coatings of ambient aerosols. The mass absorption cross-section (MAC) of decoated/pure atmospheric BC aerosols of 4.4 ± 0.8 m{sup 2}g{sup −1} was enhanced to 9.6 ± 1.8 m{sup 2}g{sup −1} at 678-nm wavelength for ambiently-coated BC aerosols at a rural Northern China site. The enhancement of MAC (E{sub MAC}) rises from 1.4 ± 0.3 in fresh combustion emissions to ~ 3 for aged ambient China aerosols. The three-week high-intensity campaign observed an average E{sub MAC} of 2.25 ± 0.55, and sulfates were primary drivers of the enhanced BC absorption. - Highlights: • A method was developed to remove coatings surrounding BC in ambient aerosols. • The MAC of decoated BC of 4.4 was enhanced to 9.6 m{sup 2}g{sup −1} for ambient BC aerosols. • BC radiative forcing in the ambient atmosphere was enhanced by a factor of ~ 2. • BC absorption enhancement peaked in day time driven by secondary sulfate.

  5. Weekly patterns of aerosol in the United States

    Directory of Open Access Journals (Sweden)

    D. M. Murphy

    2008-01-01

    Full Text Available Data from the Interagency Monitoring of Protected Visual Environments (IMPROVE network of aerosol samplers and NOAA monitoring sites are examined for weekly cycles. Fine particle elemental carbon, crustal elements, and coarse particle mass had pronounced (up to 20% weekly cycles with minima on Sunday or Monday. Fine particle organic carbon and mass had smaller amplitude cycles, also with Sunday or Monday minima. There was no statistically significant weekly cycle in fine particle sulfate despite a 10 to 15% weekly cycle in power plant SO2 emissions. Although results for nitrate must be treated with caution, it showed a pronounced weekly cycle with an amplitude similar to elemental carbon. The only species found with a weekend maximum was Pb, probably from general aviation on weekends. Aerosol optical properties at NOAA monitoring sites were consistent with the IMPROVE chemical data, with significant weekly cycles in aerosol light absorption but not light scattering. These results support a large role of diesel emissions in elemental carbon aerosol over the entire United States and suggest that a large fraction of the airborne soil dust is anthropogenic. They also suggest that studies of weekly cycles in temperature, cloudiness, or precipitation should look for causes more in light-absorbing particles and dust rather than sulfate or total aerosol. There are also implications for personal exposure and epidemiological studies of aerosol health effects.

  6. Weekly patterns of aerosol in the United States

    Directory of Open Access Journals (Sweden)

    D. M. Murphy

    2008-05-01

    Full Text Available Data from the Interagency Monitoring of Protected Visual Environments (IMPROVE network of aerosol samplers and NOAA monitoring sites are examined for weekly cycles. At remote and rural sites, fine particle elemental carbon, crustal elements, and coarse particle mass had pronounced (up to 20% weekly cycles with minima on Sunday or Monday. Fine particle organic carbon and mass had smaller amplitude cycles, also with Sunday or Monday minima. There was no statistically significant weekly cycle in fine particle sulfate despite a 5 to 15% weekly cycle in power plant SO2 emissions. Although results for nitrate may be more susceptible to sampling artifacts, nitrate also showed a pronounced weekly cycle with an amplitude similar to elemental carbon. The only species found with a weekend maximum was Pb, probably from general aviation on weekends. Aerosol optical properties at NOAA monitoring sites were consistent with the IMPROVE chemical data, with significant weekly cycles in aerosol light absorption but not light scattering. These results support a large role of diesel emissions in elemental carbon aerosol over the entire United States and suggest that a large fraction of the airborne soil dust is anthropogenic. They also suggest that studies of weekly cycles in temperature, cloudiness, precipitation, or other meteorological variables should look for causes more in light-absorbing particles and possible ice nucleation by dust rather than sulfate or total aerosol. There are also implications for personal exposure and epidemiological studies of aerosol health effects.

  7. Multidecadal trends in aerosol radiative forcing over the Arctic: Contribution of changes in anthropogenic aerosol to Arctic warming since 1980

    Science.gov (United States)

    Breider, Thomas J.; Mickley, Loretta J.; Jacob, Daniel J.; Ge, Cui; Wang, Jun; Payer Sulprizio, Melissa; Croft, Betty; Ridley, David A.; McConnell, Joseph R.; Sharma, Sangeeta; Husain, Liaquat; Dutkiewicz, Vincent A.; Eleftheriadis, Konstantinos; Skov, Henrik; Hopke, Phillip K.

    2017-03-01

    Arctic observations show large decreases in the concentrations of sulfate and black carbon (BC) aerosols since the early 1980s. These near-term climate-forcing pollutants perturb the radiative balance of the atmosphere and may have played an important role in recent Arctic warming. We use the GEOS-Chem global chemical transport model to construct a 3-D representation of Arctic aerosols that is generally consistent with observations and their trends from 1980 to 2010. Observations at Arctic surface sites show significant decreases in sulfate and BC mass concentrations of 2-3% per year. We find that anthropogenic aerosols yield a negative forcing over the Arctic, with an average 2005-2010 Arctic shortwave radiative forcing (RF) of -0.19 ± 0.05 W m-2 at the top of atmosphere (TOA). Anthropogenic sulfate in our study yields more strongly negative forcings over the Arctic troposphere in spring (-1.17 ± 0.10 W m-2) than previously reported. From 1980 to 2010, TOA negative RF by Arctic aerosol declined, from -0.67 ± 0.06 W m-2 to -0.19 ± 0.05 W m-2, yielding a net TOA RF of +0.48 ± 0.06 W m-2. The net positive RF is due almost entirely to decreases in anthropogenic sulfate loading over the Arctic. We estimate that 1980-2010 trends in aerosol-radiation interactions over the Arctic and Northern Hemisphere midlatitudes have contributed a net warming at the Arctic surface of +0.27 ± 0.04 K, roughly one quarter of the observed warming. Our study does not consider BC emissions from gas flaring nor the regional climate response to aerosol-cloud interactions or BC deposition on snow.

  8. A new source of oxygenated organic aerosol and oligomers

    Directory of Open Access Journals (Sweden)

    J. Liggio

    2013-03-01

    Full Text Available A large oxygenated organic uptake to aerosols was observed when exposing ambient urban air to inorganic acidic and non-acidic sulfate seed aerosol. For non-acidic seed aerosol the uptake was attributed to the direct dissolution of primary vehicle exhaust gases into the aqueous aerosol fraction, and was correlated to the initial seed sulphate mass. The uptake of primary oxygenated organic gases to aerosols in this study represents a significant amount of organic aerosol (OA that may be considered primary when compared to that reported for primary organic aerosol (POA, but is considerably more oxygenated (O : C ~ 0.3 than traditional POA. Consequently, a fraction of measured ambient oxygenated OA, which correlates with secondary sulphate, may in fact be of a primary, rather than secondary source. These results represent a new source of oxygenated OA on neutral aerosol and imply that the uptake of primary organic gases will occur in the ambient atmosphere, under dilute conditions, and in the presence of pre-existing SO4 aerosols which contain water. Conversely, under acidic seed aerosol conditions, oligomer formation was observed with the uptake of organics being enhanced by a factor of three or more compared to neutral aerosols, and in less than 2 min, representing an additional source of SOA to the atmosphere. This resulted in a trajectory in Van Krevelen space towards higher O : C (slope ~ −1.5, despite a lack of continual gas-phase oxidation in this closed system. The results demonstrate that high molecular weight species will form on acidic aerosols at the ambient level and mixture of organic gases, but are otherwise unaffected by subsequent aerosol neutralization, and that aerosol acidity will affect the organic O : C via aerosol-phase reactions. These two processes, forming oxygenated POA under neutral conditions and SOA under acidic conditions can contribute to the total ambient OA mass and the evolution of ambient aerosol O : C ratios

  9. Long term aerosol and trace gas measurements in Central Amazonia

    Science.gov (United States)

    Artaxo, Paulo; Barbosa, Henrique M. J.; Ferreira de Brito, Joel; Carbone, Samara; Rizzo, Luciana V.; Andreae, Meinrat O.; Martin, Scot T.

    2016-04-01

    The central region of the Amazonian forest is a pristine region in terms of aerosol and trace gases concentrations. In the wet season, Amazonia is actually one of the cleanest continental region we can observe on Earth. A long term observational program started 20 years ago, and show important features of this pristine region. Several sites were used, between then ATTO (Amazon Tall Tower Observatory) and ZF2 ecological research site, both 70-150 Km North of Manaus, receiving air masses that traveled over 1500 km of pristine tropical forests. The sites are GAW regional monitoring stations. Aerosol chemical composition (OC/EC and trace elements) is being analysed using filters for fine (PM2.5) and coarse mode aerosol as well as Aerodyne ACSM (Aerosol Chemical Speciation Monitors). VOCs are measured using PTR-MS, while CO, O3 and CO2 are routinely measured. Aerosol absorption is being studied with AE33 aethalometers and MAAP (Multi Angle Absorption Photometers). Aerosol light scattering are being measured at several wavelengths using TSI and Ecotech nephelometers. Aerosol size distribution is determined using scanning mobility particle sizer at each site. Lidars measure the aerosol column up to 12 Km providing the vertical profile of aerosol extinction. The aerosol column is measures using AERONET sun photometers. In the wet season, organic aerosol comprises 75-85% of fine aerosol, and sulfate and nitrate concentrations are very low (1-3 percent). Aerosols are dominated by biogenic primary particles as well as SOA from biogenic precursors. Black carbon in the wet season accounts for 5-9% of fine mode aerosol. Ozone in the wet season peaks at 10-12 ppb at the middle of the day, while carbon monoxide averages at 50-80 ppb. Aerosol optical thickness (AOT) is a low 0.05 to 0.1 at 550 nm in the wet season. Sahara dust transport events sporadically enhance the concentration of soil dust aerosols and black carbon. In the dry season (August-December), long range transported

  10. Laboratory and field based evaluation of chromatography related performance of the Monitor for Aerosols and Gases in Ambient Air (MARGA)

    Science.gov (United States)

    The Monitor for AeRosols and GAses in ambient air (MARGA) is an on-line ion-chromatography-based instrument designed for speciation of the inorganic gas and aerosol ammonium-nitrate-sulfate system. Previous work to characterize the performance of the MARGA has been primarily base...

  11. Aerosol typing - key information from aerosol studies

    Science.gov (United States)

    Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  12. Thermodynamic characterization of Mexico City aerosol during MILAGRO 2006

    Directory of Open Access Journals (Sweden)

    C. Fountoukis

    2009-03-01

    Full Text Available Fast measurements of aerosol and gas-phase constituents coupled with the ISORROPIA-II thermodynamic equilibrium model are used to study the partitioning of semivolatile inorganic species and phase state of Mexico City aerosol sampled at the T1 site during the MILAGRO 2006 campaign. Overall, predicted semivolatile partitioning agrees well with measurements. PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. For particle sizes up to 1μm diameter, semi-volatile partitioning requires 15–30 min to equilibrate; longer time is typically required during the night and early morning hours. Aerosol and gas-phase speciation always exhibits substantial temporal variability, so that aerosol composition measurements (bulk or size-resolved obtained over large integration periods are not reflective of its true state. When the aerosol sulfate-to-nitrate molar ratio is less than unity, predictions improve substantially if the aerosol is assumed to follow the deliquescent phase diagram. Treating crustal species as "equivalent sodium" (rather than explicitly in the thermodynamic equilibrium calculations introduces important biases in predicted aerosol water uptake, nitrate and ammonium; neglecting crustals further increases errors dramatically. This suggests that explicitly considering crustals in the thermodynamic calculations is required to accurately predict the partitioning and phase state of aerosols.

  13. Volcanism on Mars. Chapter 41

    Science.gov (United States)

    Zimbelman, J. R.; Garry, W. B.; Bleacher, J. E.; Crown, D. A.

    2015-01-01

    Spacecraft exploration has revealed abundant evidence that Mars possesses some of the most dramatic volcanic landforms found anywhere within the solar system. How did a planet half the size of Earth produce volcanoes like Olympus Mons, which is several times the size of the largest volcanoes on Earth? This question is an example of the kinds of issues currently being investigated as part of the space-age scientific endeavor called "comparative planetology." This chapter summarizes the basic information currently known about volcanism on Mars. The volcanoes on Mars appear to be broadly similar in overall morphology (although, often quite different in scale) to volcanic features on Earth, which suggests that Martian eruptive processes are not significantly different from the volcanic styles and processes on Earth. Martian volcanoes are found on terrains of different age, and Martian volcanic rocks are estimated to comprise more than 50% of the Martian surface. This is in contrast to volcanism on smaller bodies such as Earth's Moon, where volcanic activity was mainly confined to the first half of lunar history (see "Volcanism on the Moon"). Comparative planetology supports the concept that volcanism is the primary mechanism for a planetary body to get rid of its internal heat; smaller bodies tend to lose their internal heat more rapidly than larger bodies (although, Jupiter's moon Io appears to contradict this trend; Io's intense volcanic activity is powered by unique gravitational tidal forces within the Jovian system; see "Volcanism on Io"), so that volcanic activity on Mars would be expected to differ considerably from that found on Earth and the Moon.

  14. Reconstruction of the Tambora forcing with global aerosol models : Challenges and limitations

    Science.gov (United States)

    Khodri, Myriam; Zanchettin, Davide; Timmreck, Claudia

    2016-04-01

    It is now generally recognised that volcanic eruptions have an important effect on climate variability from inter-annual to decadal timescales. For the largest tropical volcanic eruptions of the last millennium, simulated volcanic surface cooling derived from climate models often disagrees with the cooling seen in tree-ring-based proxies. Furthermore, cooling estimates from simulations show large uncertainties. Such disagreement can be related to several sources, including inconsistency of the currently available volcanic forcing datasets, unrealistic modelled volcanic forcing, insufficient representation of relevant climate processes, and different background climate states simulated at the time of the eruption. In particular, for eruptions that occurred before the observational period forcing characteristics related to the eruption magnitude and stratospheric aerosol properties are deduced from indirect evidences. So, while climatically relevant forcing properties for recent volcanic eruptions are relatively well constrained by direct observations, large uncertainties remain regarding processes of aerosol formation and evolution in the stratosphere after large tropical eruptions of the remote past. Several coordinated modelling assessments have been defined to frame future modeling activities and constrain the above-mentioned uncertainties. Among these, the sixth phase of the Coupled Model Intercomparison Project (CMIP6) has endorsed a multi-model assessment focused on the climatic response to strong volcanic eruptions (VolMIP). VolMIP defines a protocol for idealized volcanic-perturbation experiments to improve comparability among climate model results. Identification of a consensual volcanic forcing dataset for the 1815 Tambora eruption is a key step of VolMIP, as it is the largest-magnitude volcanic eruption of the past five centuries and reference for the VolMIP core experiments. Therefore, as a first key step, five current/state-of-the-art global aerosol

  15. Volcanic Ash Nephelometer Probe Project

    Data.gov (United States)

    National Aeronautics and Space Administration — Advanced dropsondes that could effectively be guided through atmospheric regions of interest such as volcanic plumes may enable unprecedented observations of...

  16. Hydrocarbon- Generating Model of the Area Covered With Volcanic Rock

    Institute of Scientific and Technical Information of China (English)

    Guo Zhanqian; Zhang Yuwei

    2000-01-01

    The distribution of Oil & gas fields shows their close relationship with the most active tectonic regions. This is not a coincidence but having a scientific reasons. The crustal active regions, refer to the places where the active natural earthquake, volcanic activities, underground water happened, and the areas of the leaking off of natural gas to the surface of the crust. The magma of volcanic activities brings the organic "kitchen range body" hydrocarbon- generating model and inorganic genetic hydrocarbon to the regions covered by volcanic rock. Underground water brings a catalytic hydrocarbongenerating model for organic matter, and the leaking- off of H2 and CO2 contributes a synthetic hydrocarbon - generating model. Volcanic activities bring the assemblage of Source, Reservoir and Seal formed by the sediments and magma the sedimentary basins, and the hydrocarbon - generating system with a "water - volcano" binary structure is formed. All these conditions are favorable and excellent for the formation of oil & gas fields. The distribution of American oil & gas fields have very close relationship with the mines of Fe, Mn, Ct, Mo, W and V, deposits of Zn, Cu, V, Pb, Al and Hg, and the deposits of fluorite, sulfur, potassium salt, phosphate and halite, and the distribution of sulfate- chloride of river water. The reason why few oil & gas fields discovered in the regions covered by volcanic rock in western America maybe because of the view of "inconsistency between petroleum and volcano". Further more, It's very difficult to carry out a geophysical exploration in such kinds of regions.This paper examined a few hydrocarbon-generating models (systems) mentioned above and came up with some fresh ideas on the exploration in the areas covered with volcanic rocks.

  17. Controlling barium sulfate

    Energy Technology Data Exchange (ETDEWEB)

    Greenley, R.

    Even though for several years success has been realized in controlling barium sulfate scale deposition in relatively shallow, low pressure oil wells--by squeezing an organic phosphonate scale inhibitor into the producing zone--barium sulfate scale depositon in deep, high pressure/high temperature wells usually meant an expensive workover operation. A case history of a deep (16,000 ft) well in St. Mary Parish, Louisiana, and the scale inhibitor squeeze operation are described. Based on the successful results obtained in treating this well, a generalized treating procedure for combating downhole scale deposition in high pressure/high temperature gas wells is presented. Formation squeezing with such an inhibitor represents a significant breakthrough for the oil and gas industry.

  18. An investigation of aerosol optical properties: Atmospheric implications and influences

    Science.gov (United States)

    Penaloza-Murillo, Marcos A.

    An experimental, observational, and theoretical investigation of aerosol optical properties has been made in this work to study their implications and influences on the atmosphere. In the laboratory the scientific and instrumental methodology consisted of three parts, namely, aerosol generation, optical and mass concentration measurements, and computational calculations. In particular the optical properties of ammonium sulfate and caffeine aerosol were derived from measurements made with a transmissometer cell-reciprocal- integrating nephelometer (TCRIN), equipped with a laser beam at 632.8 nm, and by applying a Mie theory computer code The aerosol generators, optical equipment and calibration procedures were reviewed. The aerosol shape and size distribution were studied by means of scanning electron microscopy and the Gumprecht- Sliepcevich/Lipofsky-Green extinction-sedimentation method. In particular the spherical and cylindrical shape were considered. During this investigation, an alternative method for obtaining the optical properties of monodisperse spherical non-absorbing aerosol using a cell-transmissometer, which is based on a linearisation of the Lambert-Beer law, was found. In addition, adapting the TCRIN to electrooptical aerosol studies, the optical properties of a circular-cylindrical aerosol of caffeine were undertaken under the condition of random orientation in relation with the laser beam, and perpendicular orientation to it. A theoretical study was conducted to assess the sensitivity of aerosol to a change of shape under different polarisation modes. The aerosol optical properties, obtained previously in the laboratory, were then used to simulate the direct radiative forcing. The calculations and results were obtained by applying a one- dimensional energy-balance box model. The influence of atmospheric aerosol on the sky brightness due to a total solar eclipse was studied using the photometric and meteorological observations made during the

  19. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    Energy Technology Data Exchange (ETDEWEB)

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-04-09

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m{sup 2} between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m{sup 2} depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  20. System of Volcanic activity

    Directory of Open Access Journals (Sweden)

    P. HÉDERVARI

    1972-06-01

    Full Text Available A comparison is made among the systems of B. G.
    Escher (3, of R. W. van Bemmelen (1 and that of the author (4. In this
    connection, on the basis of Esclier's classification, the terms of "constructiv
    e " and "destructive" eruptions are introduced into the author's system and
    at the same time Escher's concept on the possible relation between the depth
    of magma-chamber and the measure of the gas-pressure is discussed briefly.
    Three complementary remarks to the first paper (4 011 the subject of system
    of volcanic activity are added.