Sulfur deposition changes under sulfate geoengineering conditions: quasi-biennial oscillation effects on the transport and lifetime of stratospheric aerosols

Science.gov (United States)

Visioni, Daniele; Pitari, Giovanni; Tuccella, Paolo; Curci, Gabriele

2018-02-01

Sustained injection of sulfur dioxide (SO2) in the tropical lower stratosphere has been proposed as a climate engineering technique for the coming decades. Among several possible environmental side effects, the increase in sulfur deposition deserves additional investigation. In this study we present results from a composition-climate coupled model (University of L'Aquila Composition-Chemistry Model, ULAQ-CCM) and a chemistry-transport model (Goddard Earth Observing System Chemistry-Transport Model, GEOS-Chem), assuming a sustained lower-stratospheric equatorial injection of 8 Tg SO2 yr-1. Total S deposition is found to globally increase by 5.2 % when sulfate geoengineering is deployed, with a clear interhemispheric asymmetry (+3.8 and +10.3 % in the Northern Hemisphere (NH) and the Southern Hemisphere (SH), due to +2.2 and +1.8 Tg S yr-1, respectively). The two models show good consistency, both globally and on a regional scale under background and geoengineering conditions, except for S-deposition changes over Africa and the Arctic. The consistency exists with regard to time-averaged values but also with regard to monthly and interannual deposition changes. The latter is driven essentially by the variability in stratospheric large-scale transport associated with the quasi-biennial oscillation (QBO). Using an externally nudged QBO, it is shown how a zonal wind E shear favors aerosol confinement in the tropical pipe and a significant increase in their effective radius (+13 % with respect to W shear conditions). The net result is an increase in the downward cross-tropopause S flux over the tropics with dominant E shear conditions with respect to W shear periods (+0.61 Tg S yr-1, +42 %, mostly due to enhanced aerosol gravitational settling) and a decrease over the extratropics (-0.86 Tg S yr-1, -35 %, mostly due to decreased large-scale stratosphere-troposphere exchange of geoengineering sulfate). This translates into S-deposition changes that are significantly

Laboratory studies of stratospheric aerosol chemistry

Science.gov (United States)

Molina, Mario J.

1996-01-01

In this report we summarize the results of the two sets of projects funded by the NASA grant NAG2-632, namely investigations of various thermodynamic and nucleation properties of the aqueous acid system which makes up stratospheric aerosols, and measurements of reaction probabilities directly on ice aerosols with sizes corresponding to those of polar stratospheric cloud particles. The results of these investigations are of importance for the assessment of the potential stratospheric effects of future fleets of supersonic aircraft. In particular, the results permit to better estimate the effects of increased amounts of water vapor and nitric acid (which forms from nitrogen oxides) on polar stratospheric clouds and on the chemistry induced by these clouds.

Stratospheric sulfate from the Gareloi eruption, 1980: Contribution to the ''ambient'' aerosol by a poorly documented volcanic eruption

International Nuclear Information System (INIS)

Sedlacek, W.A.; Mroz, E.J.; Heiken, G.

1981-01-01

While sampling stratospheric aerosols during July--August 1980 a plume of ''fresh'' volcanic debris was observed in the Northern hemisphere. The origin of this material seems to be a poorly documented explosive eruption of Gareloi valcano in the Aleutian Islands. The debris was sampled at an altitude of 19.2 km: almost twice the height of observed eruption clouds. Such remote, unobserved or poorly documented eruptions may be a source that helps maintain the ''ambient'' stratospheric aerosol background

Geo-Engineering Climate Change with Sulfate Aerosol

Science.gov (United States)

Rasch, P. J.; Crutzen, P. J.

2006-12-01

We explore the impact of injecting a precursor of sulfate aerosols into the middle atmosphere where they would act to increase the planetary albedo and thus counter some of the effects of greenhouse gase forcing. We use an atmospheric general circulation model (CAM, the Community Atmosphere Model) coupled to a slab ocean model for this study. Only physical effects are examined, that is we ignore the biogeochemical and chemical implications of changes to greenhouse gases and aerosols, and do not explore the important ethical, legal, and moral issues that are associated with deliberate geo-engineering efforts. The simulations suggest that the sulfate aerosol produced from the SO2 source in the stratosphere is sufficient to counterbalance most of the warming associated with the greenhouse gas forcing. Surface temperatures return to within a few tenths of a degree(K) of present day levels. Sea ice and precipitation distributions are also much closer to their present day values. The polar region surface temperatures remain 1-3 degrees warm in the winter hemisphere than present day values. This study is very preliminary. Only a subset of the relevant effects have been explored. The effect of such an injection of aerosols on middle atmospheric chemistry, and the effect on cirrus clouds are obvious missing components that merit scrutiny. There are probably others that should be considered. The injection of such aerosols cannot help in ameliorating the effects of CO2 changes on ocean PH, or other effects on the biogeochemistry of the earth system.

Condensed Acids In Antartic Stratospheric Clouds

Science.gov (United States)

Pueschel, R. F.; Snetsinger, K. G.; Toon, O. B.; Ferry, G. V.; Starr, W. L.; Oberbeck, V. R.; Chan, K. R.; Goodman, J. K.; Livingston, J. M.; Verma, S.;

Volcanic Plume Impact on the Atmosphere and Climate: O- and S-Isotope Insight into Sulfate Aerosol Formation

Directory of Open Access Journals (Sweden)

Erwan Martin

2018-05-01

Full Text Available The impact of volcanic eruptions on the climate has been studied over the last decades and the role played by sulfate aerosols appears to be major. S-bearing volcanic gases are oxidized in the atmosphere into sulfate aerosols that disturb the radiative balance on earth at regional to global scales. This paper discusses the use of the oxygen and sulfur multi-isotope systematics on volcanic sulfates to understand their formation and fate in more or less diluted volcanic plumes. The study of volcanic aerosols collected from air sampling and ash deposits at different distances from the volcanic systems (from volcanic vents to the Earth poles is discussed. It appears possible to distinguish between the different S-bearing oxidation pathways to generate volcanic sulfate aerosols whether the oxidation occurs in magmatic, tropospheric, or stratospheric conditions. This multi-isotopic approach represents an additional constraint on atmospheric and climatic models and it shows how sulfates from volcanic deposits could represent a large and under-exploited archive that, over time, have recorded atmospheric conditions on human to geological timescales.

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

Directory of Open Access Journals (Sweden)

A. C. Jones

2016-03-01

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 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.

International Workshop on Stratospheric Aerosols: Measurements, Properties, and Effects

Science.gov (United States)

Pueschel, Rudolf F. (Editor)

1991-01-01

Following a mandate by the International Aerosol Climatology Program under the auspices of International Association of Meteorology and Atmospheric Physics International Radiation Commission, 45 scientists from five nations convened to discuss relevant issues associated with the measurement, properties, and effects of stratospheric aerosols. A summary is presented of the discussions on formation and evolution, transport and fate, effects on climate, role in heterogeneous chemistry, and validation of lidar and satellite remote sensing of stratospheric aerosols. Measurements are recommended of the natural (background) and the volcanically enhanced aerosol (sulfuric acid and silica particles), the exhaust of shuttle, civil aviation and supersonic aircraft operations (alumina, soot, and ice particles), and polar stratospheric clouds (ice, condensed nitric and hydrochloric acids).

Lidar observations and transfer of stratospheric aerosol over Tomsk in summer period

Science.gov (United States)

Novikov, P. V.; Cheremisin, A. A.; Marichev, V. N.; Barashkov, T. O.

2015-11-01

The analysis of the stratospheric aerosol origin was carried out by the method of Lagrangian particle trajectories. Stratospheric aerosol was registered by lidar sounding of atmosphere above Tomsk in 2008-2013 in summer time. The analysis of the results had shown that the aerosol content at altitudes of 13-125 km with maximum at 16-18 km can be associated with aerosol transfer from tropical stratospheric reservoir.

Stratospheric Aerosol and Gas Experiment (SAGE) IV Pathfinder

Data.gov (United States)

National Aeronautics and Space Administration — The Clean Air Act mandates NASA to monitor stratospheric ozone, and stratospheric aerosol measurements are vital to our understanding of climate.  Maintaining...

Cosmogenic 35S as a Novel Detector of Stratospheric Air at the Earth's Surface: Key Findings from the Western United States and New Insights into the Seasonal Variations of Ozone and Sulfate in East Asia

Science.gov (United States)

Lin, M.; Thiemens, M. H.; Shaheen, R.; Biglari, S.; Crocker, D.; Zhang, Z.; Tao, J.; Su, L.; Fung, J. C. H.; Su, B.; Liu, L.

2016-12-01

The extent to which stratospheric intrusions on synoptic scales influence the tropospheric ozone (O3) levels remains poorly understood because quantitative detection of stratosphere air at the Earth's surface has been challenging. Cosmogenic 35S is invaluable in such quantification, but this has not yet been unambiguously demonstrated. As a global hot spot for stratospheric intrusions, the western United States (US) is a natural laboratory for testing the validity of this approach. Here, we present measurements of 35S in sulfate aerosols during a well-defined deep stratospheric intrusion event in the western US, which led to a regional O3 pollution event across southern California. The surprisingly high 35S activity in this episode is greater than any other natural radiogenic sulfate aerosols reported in the literature, providing the first and direct field-based evidence that 35S is a sensitive tracer for air mass of stratospheric origin and transported downward. Using this novel tracer, we quantify the seasonal variation for the strength of downward transport of stratospheric air to the planetary boundary layer in East Asia (EA) and what it may mean for surface O3 and sulfate levels. Our 35S measurements in sulfate aerosols collected from a background site (Mount Wuyi; 27.72°N, 117.68°E) during 2014-2015 show peaks in spring and autumn and the temporal variations of 35S were in tandem with surface O3 levels. These results imply that stratospheric O3 in aged stratospheric air masses may contribute to surface O3 levels in the study region in these two seasons. Along with radiogenic 35S analysis, measuring all seven stable isotopes (16O, 17O, 18O, 32S, 33S, 34S and 36S) in the same sulfate samples provides significantly deeper understanding of the atmospheric sulfur cycle in this region. Triple oxygen isotopes are being measured and preliminary results show that the relative importance of different formation pathways of secondary sulfate in EA is likely altitude

Benefits, risks, and costs of stratospheric geoengineering

KAUST Repository

Robock, Alan

2009-10-02

Injecting sulfate aerosol precursors into the stratosphere has been suggested as a means of geoengineering to cool the planet and reduce global warming. The decision to implement such a scheme would require a comparison of its benefits, dangers, and costs to those of other responses to global warming, including doing nothing. Here we evaluate those factors for stratospheric geoengineering with sulfate aerosols. Using existing U.S. military fighter and tanker planes, the annual costs of injecting aerosol precursors into the lower stratosphere would be several billion dollars. Using artillery or balloons to loft the gas would be much more expensive. We do not have enough information to evaluate more exotic techniques, such as pumping the gas up through a hose attached to a tower or balloon system. Anthropogenic stratospheric aerosol injection would cool the planet, stop the melting of sea ice and land-based glaciers, slow sea level rise, and increase the terrestrial carbon sink, but produce regional drought, ozone depletion, less sunlight for solar power, and make skies less blue. Furthermore it would hamper Earth-based optical astronomy, do nothing to stop ocean acidification, and present many ethical and moral issues. Further work is needed to quantify many of these factors to allow informed decision-making.

Satellite studies of the stratospheric aerosol

International Nuclear Information System (INIS)

McCormick, M.P.; Hamill, P.; Pepin, T.J.; Chu, W.P.; Swissler, T.J.; McMaster, L.R.

1979-01-01

The potential climatological and environmental importance of the stratospheric aerosol layer has prompted great interest in measuring the properties of this aerosol. In this paper we report on two recently deployed NASA satellite systems (SAM II and SAGE) that are monitoring the stratospheric aerosol. The satellite orbits are such that nearly global coverage is obtained. The instruments mounted in the spacecraft are sun photometers that measure solar intensity at specific wavelengths as it is moderated by atmospheric particulates and gases during each sunrise and sunset encountered by the satellites. The data obtained are ''inverted'' to yield vertical aerosol and gaseous (primarily ozone) extinction profiles with 1 km vertical resolution. Thus, latitudinal, longitudinal, and temporal variations in the aerosol layer can be evaluated. The satellite systems are being validated by a series of ground truth experiments using airborne and ground lidar, balloon-borne dustsondes, aircraft-mounted impactors, and other correlative sensors. We describe the SAM II and SAGE satellite systems, instrument characteristics, and mode of operation; outline the methodology of the experiments; and describe the ground truth experiments. We present preliminary results from these measurements

A stratospheric aerosol increase

Science.gov (United States)

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

1980-01-01

Large disturbances were noted in the stratospheric aerosol content in the midlatitude Northern Hemisphere commencing about 7 months after the eruption of La Soufriere and less than 1 month after the eruption of Sierra Negra. The aerosol was characterized by a very steep size distribution in the 0.15 to 0.25 micron radius range and contained a volatile component. Measurements near the equator and at the South Pole indicate that the disturbance was widespread. These observations were made before the May 18 eruption of Mt. St. Helens.

Reduction of photosynthetically active radiation under extreme stratospheric-aerosol loads

International Nuclear Information System (INIS)

Gerstl, S.A.W.; Zardecki, A.

1981-01-01

The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10 16 g is sufficient to reduce photosynthesis to 10 3 of normal. We also infer from this result that the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al., is thus shown to be a possible extinction mechanism, even with smaller size asteroids or comets than previously estimated

Reduction of photosynthetically active radiation under extreme stratospheric aerosol loads

International Nuclear Information System (INIS)

Gerstl, S.A.W.; Zardecki, A.

1981-08-01

The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10 1 g is sufficient to reduce photosynthesis to 10 -3 of normal. We also infer from this result tha the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al. is thus shown to be a possible extinction mechanism, even with smaller size asteroids of comets than previously estimated

SAGE measurements of the stratospheric aerosol dispersion and loading from the Soufriere Volcano

Science.gov (United States)

Mccormick, M. P.; Kent, G. S.; Yue, G. K.; Cunnold, D. M.

1981-01-01

Explosions of the Soufriere volcano on the Caribbean Island of St. Vincent reduced two major stratospheric plumes which the stratospheric aerosol and gas experiment (SAGE) satellite tracked to West Africa and the North Atlantic Ocean. The total mass of the stratospheric ejecta measured is less than 0.5% of the global stratospheric aerosol burden. No significant temperature or climate perturbation is expected. It is found that the movement and dispersion of the plumes agree with those deduced from high altitude meteorological data and dispersion theory. The stratospheric aerosol dispersion and loading from the Soufrier volcano was measured.

The effect of stratospheric sulfur from Mount Pinatubo on tropospheric oxidizing capacity and methane

NARCIS (Netherlands)

Banda, Narcissa; Krol, Maarten; van Noije, Twan; van Weele, Michiel; Williams, Jason E.; Sager, Philippe Le; Niemeier, Ulrike; Thomason, Larry; Röckmann, Thomas

2015-01-01

The eruption of Mount Pinatubo in 1991 injected a large amount of SO2 into the stratosphere, which formed sulfate aerosols. Increased scattering and absorption of UV radiation by the enhanced stratospheric SO2 and aerosols decreased the amount of UV radiation reaching the troposphere, causing

Odin-OSIRIS stratospheric aerosol data product and SAGE III intercomparison

Directory of Open Access Journals (Sweden)

A. E. Bourassa

2012-01-01

Full Text Available The scattered sunlight measurements made by the Optical Spectrograph and InfraRed Imaging System (OSIRIS on the Odin spacecraft are used to retrieve vertical profiles of stratospheric aerosol extinction at 750 nm. The recently released OSIRIS Version 5 data product contains the first publicly released stratospheric aerosol extinction retrievals, and these are now available for the entire Odin mission, which extends from the present day back to launch in 2001. A proof-of-concept study for the retrieval of stratospheric aerosol extinction from limb scatter measurements was previously published and the Version 5 data product retrievals are based on this work, but incorporate several important improvements to the algorithm. One of the primary changes is the use of a new retrieval vector that greatly improves the sensitivity to aerosol scattering by incorporating a forward modeled calculation of the radiance from a Rayleigh atmosphere. Additional improvements include a coupled retrieval of the effective albedo, a new method for normalization of the retrieval vector to improve signal-to-noise, and the use of an initial guess that is representative of very low background aerosol loading conditions, which allows for maximal retrieval range. Furthermore, the Version 5 data set is compared to Stratospheric Aerosol and Gas Experiment (SAGE III 755 nm extinction profiles during the almost four years of mission overlap from 2002 to late 2005. The vertical structure in coincident profile measurements is well correlated and the statistics on a relatively large set of tight coincident measurements show agreement between the measurements from the two instruments to within approximately 10% throughout the 15 to 25 km altitude range, which covers the bulk of the stratospheric aerosol layer for the mid and high latitude cases studied here.

The effect of stratospheric sulfur from Mount Pinatubo on tropospheric oxidizing capacity and methane

NARCIS (Netherlands)

Bândə, Narcisa; Krol, Maarten; Noije, Van Twan; Weele, Van Michiel; Williams, Jason E.; Sager, Philippe Le; Niemeier, Ulrike; Thomason, Larry; Röckmann, Thomas

2015-01-01

The eruption of Mount Pinatubo in 1991 injected a large amount of SO₂ into the stratosphere, which formed sulfate aerosols. Increased scattering and absorption of UV radiation by the enhanced stratospheric SO₂ and aerosols decreased the amount of UV radiation reaching the

Measurements of stratospheric Pinatubo aerosol extinction profiles by a Raman lidar

International Nuclear Information System (INIS)

Abo, Makoto; Nagasawa, Chikao.

1992-01-01

The Raman lidar has been used for remote measurements of water vapor, ozone and atmospheric temperature in the lower troposphere because the Raman cross section is three orders smaller than the Rayleigh cross section. The authors estimated the extinction coefficients of the Pinatubo volcanic aerosol in the stratosphere using a Raman lidar. If the precise aerosol extinction coefficients are derived, the backscatter coefficient of a Mie scattering lidar will be more accurately estimated. The Raman lidar has performed to measure density profiles of some species using Raman scattering. Here the authors used a frequency-doubled Nd:YAG laser for transmitter and received nitrogen vibrational Q-branch Raman scattering signal. Ansmann et al. (1990) derived tropospherical aerosol extinction profiles with a Raman lidar. The authors think that this method can apply to dense stratospheric aerosols such as Pinatubo volcanic aerosols. As dense aerosols are now accumulated in the stratosphere by Pinatubo volcanic eruption, the error of Ramen lidar signal regarding the fluctuation of air density can be ignored

Development of the Multi-Angle Stratospheric Aerosol Radiometer (MASTAR) Instrument

Science.gov (United States)

DeLand, M. T.; Colarco, P. R.; Kowalewski, M. G.; Gorkavyi, N.; Ramos-Izquierdo, L.

2017-12-01

Aerosol particles in the stratosphere ( 15-25 km altitude), both produced naturally and perturbed by volcanic eruptions and anthropogenic emissions, continue to be a source of significant uncertainty in the Earth's energy budget. Stratospheric aerosols can offset some of the warming effects caused by greenhouse gases. These aerosols are currently monitored using measurements from the Ozone Mapping and Profiling Suite (OMPS) Limb Profiler (LP) instrument on the Suomi NPP satellite. In order to improve the sensitivity and spatial coverage of these aerosol data, we are developing an aerosol-focused compact version of the OMPS LP sensor called Multi-Angle Stratospheric Aerosol Radiometer (MASTAR) to fly on a 3U Cubesat satellite, using a NASA Instrument Incubator Program (IIP) grant. This instrument will make limb viewing measurements of the atmosphere in multiple directions simultaneously, and uses only a few selected wavelengths to reduce size and cost. An initial prototype version has been constructed using NASA GSFC internal funding and tested in the laboratory. Current design work is targeted towards a preliminary field test in Spring 2018. We will discuss the scientific benefits of MASTAR and the status of the project.

Sulphur-rich volcanic eruptions and stratospheric aerosols

Science.gov (United States)

Rampino, M. R.; Self, S.

1984-01-01

Data from direct measurements of stratospheric optical depth, Greenland ice-core acidity, and volcanological studies are compared, and it is shown that relatively small but sulfur-rich volcanic eruptions can have atmospheric effects equal to or even greater than much larger sulfur-poor eruptions. These small eruptions are probably the most frequent cause of increased stratospheric aerosols. The possible sources of the excess sulfur released in these eruptions are discussed.

A global space-based stratospheric aerosol climatology: 1979-2016

Science.gov (United States)

Thomason, Larry W.; Ernest, Nicholas; Millán, Luis; Rieger, Landon; Bourassa, Adam; Vernier, Jean-Paul; Manney, Gloria; Luo, Beiping; Arfeuille, Florian; Peter, Thomas

2018-03-01

We describe the construction of a continuous 38-year record of stratospheric aerosol optical properties. The Global Space-based Stratospheric Aerosol Climatology, or GloSSAC, provided the input data to the construction of the Climate Model Intercomparison Project stratospheric aerosol forcing data set (1979-2014) and we have extended it through 2016 following an identical process. GloSSAC focuses on the Stratospheric Aerosol and Gas Experiment (SAGE) series of instruments through mid-2005, and on the Optical Spectrograph and InfraRed Imager System (OSIRIS) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) data thereafter. We also use data from other space instruments and from ground-based, air, and balloon borne instruments to fill in key gaps in the data set. The end result is a global and gap-free data set focused on aerosol extinction coefficient at 525 and 1020 nm and other parameters on an "as available" basis. For the primary data sets, we developed a new method for filling the post-Pinatubo eruption data gap for 1991-1993 based on data from the Cryogenic Limb Array Etalon Spectrometer. In addition, we developed a new method for populating wintertime high latitudes during the SAGE period employing a latitude-equivalent latitude conversion process that greatly improves the depiction of aerosol at high latitudes compared to earlier similar efforts. We report data in the troposphere only when and where it is available. This is primarily during the SAGE II period except for the most enhanced part of the Pinatubo period. It is likely that the upper troposphere during Pinatubo was greatly enhanced over non-volcanic periods and that domain remains substantially under-characterized. We note that aerosol levels during the OSIRIS/CALIPSO period in the lower stratosphere at mid- and high latitudes is routinely higher than what we observed during the SAGE II period. While this period had nearly continuous low-level volcanic activity, it

Correlative measurements of the stratospheric aerosols

Science.gov (United States)

Santer, R.; Brogniez, C.; Herman, M.; Diallo, S.; Ackerman, M.

1992-12-01

Joint experiments were organized or available during stratospheric flights of a photopolarimeter, referred to as RADIBAL (radiometer balloon). In May 1984, RADIBAL flew simultaneously with another balloonborne experiment conducted by the Institut d'Aeronomie Spatiale de Belgique (IASB), which provides multiwavelength vertical profiles of the aerosol scattering coefficient. At this time, the El Chichon layer was observable quite directly from mountain sites. A ground-based station set up at Pic du Midi allowed an extensive description of the aerosol optical properties. The IASB and the Pic du Midi observations are consistent with the aerosol properties derived from the RADIBAL measurement analysis.

Engineering assessment of in situ sulfate production onboard aircraft at high altitude

Science.gov (United States)

Smith, J.; Dykema, J. A.; Keith, D.

2016-12-01

Stratospheric injection of scattering aerosols has been proposed as a way to reduce global temperature increases by decreasing net atmospheric radiative forcing. Several methods have been suggested as a means of implementing solar geoengineering, and high altitude aircraft have been identified as an accessible means delivering sulfate aerosols to the lower and mid-stratosphere. This research initiative analyzes the design features of an onboard open cycle chemical plant capable of in situ sulfur to sulfate conversion, and compares the required mass to that of transporting pre-fabricated gaseous or liquid sulfate aerosol precursors. Scaling from aero-derivative gas turbine engines, commercial catalytic converters, and existing aerospace materials indicate that aircraft equipped with such a system could provide a substantial mass benefit compared to direct transport of compound sulfate products.

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

International Nuclear Information System (INIS)

Geogdzhayev, Igor V.; Mishchenko, Michael I.; Liu Li; Remer, Lorraine

2004-01-01

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

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

1997-12-31

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

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

Stratospheric aerosols and precursor gases

Science.gov (United States)

1982-01-01

Measurements were made of the aerosol size, height and geographical distribution, their composition and optical properties, and their temporal variation with season and following large volcanic eruptions. Sulfur-bearing gases were measured in situ in the stratosphere, and studied of the chemical and physical processes which control gas-to-particle conversion were carried out in the laboratory.

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

Science.gov (United States)

Malinina, Elizaveta; Rozanov, Alexei; Rozanov, Vladimir; Liebing, Patricia; Bovensmann, Heinrich; Burrows, John P.

2018-04-01

health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N-20° S) for 10 years (2002-2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size distribution parameters showed clear increases in the mode radius after the tropical volcanic eruptions, whereas no distinct behaviour of the absolute distribution width could be identified. A tape recorder

Influence of Aerosol Heating on the Stratospheric Transport of the Mt. Pinatubo Eruption

Science.gov (United States)

Aquila, Valentina; Oman, Luke D.; Stolarski, Richard S.

2011-01-01

On June 15th, 1991 the eruption of Mt. Pinatubo (15.1 deg. N, 120.3 Deg. E) in the Philippines injected about 20 Tg of sulfur dioxide in the stratosphere, which was transformed into sulfuric acid aerosol. The large perturbation of the background aerosol caused an increase in temperature in the lower stratosphere of 2-3 K. Even though stratospheric winds climatological]y tend to hinder the air mixing between the two hemispheres, observations have shown that a large part of the SO2 emitted by Mt. Pinatubo have been transported from the Northern to the Southern Hemisphere. We simulate the eruption of Mt. Pinatubo with the Goddard Earth Observing System (GEOS) version 5 global climate model, coupled to the aerosol module GOCART and the stratospheric chemistry module StratChem, to investigate the influence of the eruption of Mt. Pinatubo on the stratospheric transport pattern. We perform two ensembles of simulations: the first ensemble consists of runs without coupling between aerosol and radiation. In these simulations the plume of aerosols is treated as a passive tracer and the atmosphere is unperturbed. In the second ensemble of simulations aerosols and radiation are coupled. We show that the set of runs with interactive aerosol produces a larger cross-equatorial transport of the Pinatubo cloud. In our simulations the local heating perturbation caused by the sudden injection of volcanic aerosol changes the pattern of the stratospheric winds causing more intrusion of air from the Northern into the Southern Hemisphere. Furthermore, we perform simulations changing the injection height of the cloud, and study the transport of the plume resulting from the different scenarios. Comparisons of model results with SAGE II and AVHRR satellite observations will be shown.

Benefits, risks, and costs of stratospheric geoengineering

KAUST Repository

Robock, Alan; Marquardt, Allison; Kravitz, Ben; Stenchikov, Georgiy L.

2009-01-01

Injecting sulfate aerosol precursors into the stratosphere has been suggested as a means of geoengineering to cool the planet and reduce global warming. The decision to implement such a scheme would require a comparison of its benefits, dangers

Stratospheric aerosol effects from Soufriere Volcano as measured by the SAGE satellite system

Science.gov (United States)

Mccormick, M. P.; Kent, G. S.; Yue, G. K.; Cunnold, D. M.

1982-01-01

During its April 1979 eruption series, Soufriere Volcano produced two major stratospheric plumes that the SAGE (Stratospheric Aerosol and Gas Experiment) satellite system tracked to West Africa and the North Atlantic Ocean. The total mass of these plumes, whose movement and dispersion are in agreement with those deduced from meteorological data and dispersion theory, was less than 0.5 percent of the global stratospheric aerosol burden; no significant temperature or climate perturbation is therefore expected.

A global space-based stratospheric aerosol climatology: 1979–2016

Directory of Open Access Journals (Sweden)

L. W. Thomason

2018-03-01

Full Text Available We describe the construction of a continuous 38-year record of stratospheric aerosol optical properties. The Global Space-based Stratospheric Aerosol Climatology, or GloSSAC, provided the input data to the construction of the Climate Model Intercomparison Project stratospheric aerosol forcing data set (1979–2014 and we have extended it through 2016 following an identical process. GloSSAC focuses on the Stratospheric Aerosol and Gas Experiment (SAGE series of instruments through mid-2005, and on the Optical Spectrograph and InfraRed Imager System (OSIRIS and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO data thereafter. We also use data from other space instruments and from ground-based, air, and balloon borne instruments to fill in key gaps in the data set. The end result is a global and gap-free data set focused on aerosol extinction coefficient at 525 and 1020 nm and other parameters on an "as available" basis. For the primary data sets, we developed a new method for filling the post-Pinatubo eruption data gap for 1991–1993 based on data from the Cryogenic Limb Array Etalon Spectrometer. In addition, we developed a new method for populating wintertime high latitudes during the SAGE period employing a latitude-equivalent latitude conversion process that greatly improves the depiction of aerosol at high latitudes compared to earlier similar efforts. We report data in the troposphere only when and where it is available. This is primarily during the SAGE II period except for the most enhanced part of the Pinatubo period. It is likely that the upper troposphere during Pinatubo was greatly enhanced over non-volcanic periods and that domain remains substantially under-characterized. We note that aerosol levels during the OSIRIS/CALIPSO period in the lower stratosphere at mid- and high latitudes is routinely higher than what we observed during the SAGE II period. While this period had nearly continuous low

Interpretation of DIAL Measurements of Lower Stratospheric Ozone in Regions with Pinatubo Aerosols

Science.gov (United States)

Grant, William B.; Browell, Edward V.; Fenn, Marta A.; Butler, Carolyn F.; Brackett, Vincent G.; Veiga, Robert E.; Mayor, Shane D.; Fishman, Jack; Nganga, D.; Minga, A.

1992-01-01

The influence of volcanic aerosols on stratospheric ozone is a topic of current interest, especially with the June 15, 1991 eruption of Mt. Pinatubo in the Philippines. Lidar has been used in the past to provide aerosol profiles which could be compared with ozone profiles measured using ozonesondes to look for coincidences between volcanic aerosols and ozone decreases. The differential absorption lidar (DIAL) technique has the advantages of being able to measure ozone and aerosol profiles simultaneously as well as being able to cover large geographical regions rapidly. While there are problems associated with correcting the ozone profiles for the presence of aerosols, the corrections can be made reliably when the wavelengths are closely spaced and the Bernoulli method is applied. The DIAL measurements considered in this paper are those obtained in the tropical stratosphere in January 1992 during the Airborne Arctic Stratospheric Expedition (AASE-II). The determination of ozone profiles in the presence of Pinatubo aerosols is discussed in a companion paper.

Influence of stratospheric aerosol on albedo

Energy Technology Data Exchange (ETDEWEB)

Gormatyuk, Yu K; Kaufman, Yu G; Kolomeev, M P

1985-06-01

The influence of stratospheric aerosol (SA) on the transfer of solar radiation in the atmosphere is the principal factor determining the effect of SA on climate. The change in the radiation balance under the influence of SA is computed most precisely in radiative-convective models. However, the complex method used in these models cannot be used for other types of climate models. The objective of the study was to obtain a quantitative evaluation of the influence of SA on albedo without the use of simplifying assumptions. In the approximation of single scattering an expression is derived for change in albedo under the influence of stratospheric aerosol taking into account the dependence of albedo of the atmosphere-earth's surface system on solar zenith distance. The authors give the results of computations of the response of mean annual albedo to sulfuric acid aerosol for 10/sup 0/ latitude zones in the Northern Hemisphere. Specifically, computations of the optical characteristics of aerosol were made using the Mie theory for 10 spectral intervals taking in the range of wavelengths of solar radiation from 0.29 to 4.0 ..mu.. m. The refractive index of aerosol was stipulated in accordance with Palmer and Williams. The angular dependence of albedo for cloudless and cloudy atmospheres given by Harshvardhan was used. The values of undisturbed albedo were assumed to be identical for all wavelengths due to lack of climatological data on the spectral dependence of albedo of the atmosphere-earth's surface system. The angular distribution of the intensity of solar radiation for each of the latitude zones was computed by the method described by I.M. Alekseyev, et al.

Stratospheric sulfur and its implications for radiative forcing simulated by the chemistry climate model EMAC.

Science.gov (United States)

Brühl, C; Lelieveld, J; Tost, H; Höpfner, M; Glatthor, N

2015-03-16

Multiyear simulations with the atmospheric chemistry general circulation model EMAC with a microphysical modal aerosol module at high vertical resolution demonstrate that the sulfur gases COS and SO 2 , the latter from low-latitude and midlatitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. Marine dimethyl sulfide (DMS) and other SO 2 sources, including strong anthropogenic emissions in China, are found to play a minor role except in the lowermost stratosphere. Estimates of volcanic SO 2 emissions are based on satellite observations using Total Ozone Mapping Spectrometer and Ozone Monitoring Instrument for total injected mass and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat or Stratospheric Aerosol and Gases Experiment for the spatial distribution. The 10 year SO 2 and COS data set of MIPAS is also used for model evaluation. The calculated radiative forcing of stratospheric background aerosol including sulfate from COS and small contributions by DMS oxidation, and organic aerosol from biomass burning, is about 0.07W/m 2 . For stratospheric sulfate aerosol from medium and small volcanic eruptions between 2005 and 2011 a global radiative forcing up to 0.2W/m 2 is calculated, moderating climate warming, while for the major Pinatubo eruption the simulated forcing reaches 5W/m 2 , leading to temporary climate cooling. The Pinatubo simulation demonstrates the importance of radiative feedback on dynamics, e.g., enhanced tropical upwelling, for large volcanic eruptions.

Lidar observations of stratospheric aerosol layer after the Mt. Pinatubo volcanic eruption

International Nuclear Information System (INIS)

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

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.

Efficient transport of tropospheric aerosol into the stratosphere via the Asian summer monsoon anticyclone

Science.gov (United States)

Yu, Pengfei; Rosenlof, Karen H.; Liu, Shang; Telg, Hagen; Thornberry, Troy D.; Rollins, Andrew W.; Portmann, Robert W.; Bai, Zhixuan; Ray, Eric A.; Duan, Yunjun; Pan, Laura L.; Toon, Owen B.; Bian, Jianchun; Gao, Ru-Shan

2017-07-01

An enhanced aerosol layer near the tropopause over Asia during the June-September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (˜15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (˜35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.

Effects of stratospheric aerosol surface processes on the LLNL two-dimensional zonally averaged model

International Nuclear Information System (INIS)

Connell, P.S.; Kinnison, D.E.; Wuebbles, D.J.; Burley, J.D.; Johnston, H.S.

1992-01-01

We have investigated the effects of incorporating representations of heterogeneous chemical processes associated with stratospheric sulfuric acid aerosol into the LLNL two-dimensional, zonally averaged, model of the troposphere and stratosphere. Using distributions of aerosol surface area and volume density derived from SAGE 11 satellite observations, we were primarily interested in changes in partitioning within the Cl- and N- families in the lower stratosphere, compared to a model including only gas phase photochemical reactions

Quantifying the temperature-independent effect of stratospheric aerosol geoengineering on global-mean precipitation in a multi-model ensemble

International Nuclear Information System (INIS)

Ferraro, Angus J; Griffiths, Hannah G

2016-01-01

The reduction in global-mean precipitation when stratospheric aerosol geoengineering is used to counterbalance global warming from increasing carbon dioxide (CO 2 ) concentrations has been mainly attributed to the temperature-independent effect of CO 2 on atmospheric radiative cooling. We demonstrate here that stratospheric sulphate aerosol itself also acts to reduce global-mean precipitation independent of its effects on temperature. The temperature-independent effect of stratospheric aerosol geoenginering on global-mean precipitation is calculated by removing temperature-dependent effects from climate model simulations of the Geoengineering Model Intercomparison Project (GeoMIP). When sulphate aerosol is injected into the stratosphere at a rate of 5 Tg SO 2 per year the aerosol reduces global-mean precipitation by approximately 0.2 %, though multiple ensemble members are required to separate this effect from internal variability. For comparison, the precipitation reduction from the temperature-independent effect of increasing CO 2 concentrations under the RCP4.5 scenario of the future is approximately 0.5 %. The temperature-independent effect of stratospheric sulphate aerosol arises from the aerosol’s effect on tropospheric radiative cooling. Radiative transfer calculations show this is mainly due to increasing downward emission of infrared radiation by the aerosol, but there is also a contribution from the stratospheric warming the aerosol causes. Our results suggest climate model simulations of solar dimming can capture the main features of the global-mean precipitation response to stratospheric aerosol geoengineering. (letter)

Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS)

Science.gov (United States)

Gasbarre, Joseph; Walker, Richard; Cisewski, Michael; Zawodny, Joseph; Cheek, Dianne; Thornton, Brooke

2015-01-01

The Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS) mission will extend the SAGE data record from the ideal vantage point of the International Space Station (ISS). The ISS orbital inclination is ideal for SAGE measurements providing coverage between 70 deg north and 70 deg south latitude. The SAGE data record includes an extensively validated data set including aerosol optical depth data dating to the Stratospheric Aerosol Measurement (SAM) experiments in 1975 and 1978 and stratospheric ozone profile data dating to the Stratospheric Aerosol and Gas Experiment (SAGE) in 1979. These and subsequent data records, notably from the SAGE II experiment launched on the Earth Radiation Budget Satellite in 1984 and the SAGE III experiment launched on the Russian Meteor-3M satellite in 2001, have supported a robust, long-term assessment of key atmospheric constituents. These scientific measurements provide the basis for the analysis of five of the nine critical constituents (aerosols, ozone (O3), nitrogen dioxide (NO2), water vapor (H2O), and air density using O2) identified in the U.S. National Plan for Stratospheric Monitoring. SAGE III on ISS was originally scheduled to fly on the ISS in the same timeframe as the Meteor-3M mission, but was postponed due to delays in ISS construction. The project was re-established in 2009.

Lidar measurements of ozone and aerosol distributions during the 1992 airborne Arctic stratospheric expedition

Science.gov (United States)

Browell, Edward V.; Butler, Carolyn F.; Fenn, Marta A.; Grant, William B.; Ismail, Syed; Carter, Arlen F.

1994-01-01

The NASA Langley airborne differential absorption lidar system was operated from the NASA Ames DC-8 aircraft during the 1992 Airborne Arctic Stratospheric Expedition to investigate the distribution of stratospheric aerosols and ozone (O3) across the Arctic vortex from January to March 1992. Aerosols from the Mt. Pinatubo eruption were found outside and inside the Arctic vortex with distinctly different scattering characteristics and spatial distributions in the two regions. The aerosol and O3 distributions clearly identified the edge of the vortex and provided additional information on vortex dynamics and transport processes. Few polar stratospheric clouds were observed during the AASE-2; however, those that were found had enhanced scattering and depolarization over the background Pinatubo aerosols. The distribution of aerosols inside the vortex exhibited relatively minor changes during the AASE-2. Ozone depletion inside the vortex as limited to less than or equal to 20 percent in the altitude region from 15-20 km.

Easy Volcanic Aerosol (EVA v1.0: an idealized forcing generator for climate simulations

Directory of Open Access Journals (Sweden)

M. Toohey

2016-11-01

Full Text Available Stratospheric sulfate aerosols from volcanic eruptions have a significant impact on the Earth's climate. To include the effects of volcanic eruptions in climate model simulations, the Easy Volcanic Aerosol (EVA forcing generator provides stratospheric aerosol optical properties as a function of time, latitude, height, and wavelength for a given input list of volcanic eruption attributes. EVA is based on a parameterized three-box model of stratospheric transport and simple scaling relationships used to derive mid-visible (550 nm aerosol optical depth and aerosol effective radius from stratospheric sulfate mass. Precalculated look-up tables computed from Mie theory are used to produce wavelength-dependent aerosol extinction, single scattering albedo, and scattering asymmetry factor values. The structural form of EVA and the tuning of its parameters are chosen to produce best agreement with the satellite-based reconstruction of stratospheric aerosol properties following the 1991 Pinatubo eruption, and with prior millennial-timescale forcing reconstructions, including the 1815 eruption of Tambora. EVA can be used to produce volcanic forcing for climate models which is based on recent observations and physical understanding but internally self-consistent over any timescale of choice. In addition, EVA is constructed so as to allow for easy modification of different aspects of aerosol properties, in order to be used in model experiments to help advance understanding of what aspects of the volcanic aerosol are important for the climate system.

Aerosol-associated changes in tropical stratospheric ozone following the eruption of Mount Pinatubo

Science.gov (United States)

Grant, William B.; Browell, Edward V.; Fishman, Jack; Brackett, Vincent G.; Veiga, Robert E.; Nganga, Dominique; Minga, A.; Cros, Bernard; Butler, Carolyn F.; Fenn, Marta A.

1994-01-01

The large amount of sulfuric acid aerosol formed in the stratosphere by conversion of sulfur dioxide emitted by the eruption of Mount Pinatubo (15.14 deg N, 120.35 deg E) in the Philippines around June 15, 1991, has had a pronounced effect on lower stratospheric ozone in the tropics. Measurements of stratospheric ozone in the tropics using electrochemical concentration cell (ECC) sondes before and after the eruption and the airborne UV differential absorption lidar (DIAL) system after the eruption are compared with Stratospheric Aerosol and Gas Experiment II (SAGE II) measurements from several years before the eruption and ECC sonde measurements from the year prior to the eruption to determine the resulting changes. Ozone decreases of up to 33 % compared with SAGE II climatological values were found to be directly correlated with altitude regions of enhanced aerosol loading in the 16- to 28-km range. A maximum partial-column decrease of 29 +/- Dobson units (DU) was found over the 16- to 28-km range in September 1991 along with small increases (to 5.9 +/- 2 DU) from 28 to 31.5 km. A large decrease of ozone was also found at 4 deg to 8 deg S from May to August 1992, with a maximum decrease of 33 +/- 7 DU found above Brazzaville in July. Aerosol data form the visible channel of the advanced very high resolution radiometer (AVHRR) and the visible wavelength of the UV DIAL system were used to examine the relationship between aerosol (surface area) densities and ozone changes. The tropical stratospheric ozone changes we observed in 1991 and 1992 are likely be explained by a combination of dynamical (vertical transport) perturbations, radiative perturbations on ozone photochemistry, and heterogeneous chemistry.

Relevant climate response tests for stratospheric aerosol injection: A combined ethical and scientific analysis

Science.gov (United States)

Lenferna, Georges Alexandre; Russotto, Rick D.; Tan, Amanda; Gardiner, Stephen M.; Ackerman, Thomas P.

2017-06-01

In this paper, we focus on stratospheric sulfate injection as a geoengineering scheme, and provide a combined scientific and ethical analysis of climate response tests, which are a subset of outdoor tests that would seek to impose detectable and attributable changes to climate variables on global or regional scales. We assess the current state of scientific understanding on the plausibility and scalability of climate response tests. Then, we delineate a minimal baseline against which to consider whether certain climate response tests would be relevant for a deployment scenario. Our analysis shows that some climate response tests, such as those attempting to detect changes in regional climate impacts, may not be deployable in time periods relevant to realistic geoengineering scenarios. This might pose significant challenges for justifying stratospheric sulfate aerosol injection deployment overall. We then survey some of the major ethical challenges that proposed climate response tests face. We consider what levels of confidence would be required to ethically justify approving a proposed test; whether the consequences of tests are subject to similar questions of justice, compensation, and informed consent as full-scale deployment; and whether questions of intent and hubris are morally relevant for climate response tests. We suggest further research into laboratory-based work and modeling may help to narrow the scientific uncertainties related to climate response tests, and help inform future ethical debate. However, even if such work is pursued, the ethical issues raised by proposed climate response tests are significant and manifold.

SAGE II observations of a previously unreported stratospheric volcanic aerosol cloud in the northern polar summer of 1990

Science.gov (United States)

Yue, Glenn K.; Veiga, Robert E.; Wang, Pi-Huan

1994-01-01

Analysis of aerosol extinction profiles obtained by the spaceborne SAGE II sensor reveals that there was an anomalous increase of aerosol extinction below 18.5 km at latitudes poleward of 50 deg N from July 28 to September 9, 1990. This widespread increase of aerosol extinction in the lower stratosphere was apparently due to a remote high-latitude volcanic eruption that has not been reported to date. The increase in stratospheric optical depth in the northern polar region was about 50% in August and had diminished by October 1990. This eruption caused an increase in stratospheric aerosol mass of about 0.33 x 10(exp 5) tons, assuming the aerosol was composed of sulfuric acid and water.

A global, space-based stratospheric aerosol climatology: 1979 to 2014

Science.gov (United States)

Thomason, L. W.; Vernier, J. P.; Bourassa, A. E.; Millan, L.; Manney, G. L.

2016-12-01

Herein, we report on a global space-based stratospheric aerosol climatology (GloSSAC) that has been developed to support Coupled Model Intercomparison Project Phase 6 (CMIP6) (REF to CMIP6 and ETH work). GloSSAC is most closely related to the ASAP[SPARC, 2006] and CCMI data sets and follows a similar approach used to produce those data sets. It is primarily built using space-based measurements by a number of instruments including the SAGE series, OSIRIS, CALIPSO, CLAES and HALOE. The data set is presented as monthly depictions for 80S to 80N and from at least the tropopause to 40 km. The data set consists primarily of measurements by the instruments at their native wavelength and measurement type (e.g., extinction coefficient). However, every bin in these monthly grids receives measured or indirectly inferred values for aerosol extinction coefficient at 525 and 1020 nm. Generally, bins where no data are available are filled via simple linear interpolation in time only. The exceptions are in the SAGE I/II gap from 1982 to 1984 where data from SAM II and ground-based and airborne lidar data sets are used to span the 3 years between the end of the SAGE I mission in November 1981 and the beginning of the SAGE II mission in October 1984. Ground-based lidar also supplements space-based data in the months following the Pinatubo eruption when much of the lower stratosphere is too optically opaque for occultation measurements. This data set includes total aerosol surface area density and volume estimates based on Thomason et al.[2008] though these should be interpreted as bounding values (low and high) rather than functional aerosol parameters that are generally produced from this and predecessor data sets by other parties. Unlike previous versions of this data set, GloSSAC has been permanently archived at NASA's Atmospheric Science Data Center and a digital object identifier (doi) for GloSSAC is available. SPARC (2006), Assessment of Stratospheric Aerosol Properties (ASAP

Major Influence of Tropical Volcanic Eruptions on the Stratospheric Aerosol Layer During the Last Decade

Science.gov (United States)

Vernier, Jean-Paul; Thomason, Larry W.; Pommereau, J.-P.; Bourassa, Adam; Pelon, Jacques; Garnier, Anne; Hauchecorne, A.; Blanot, L.; Trepte, Charles R.; Degenstein, Doug;

A sensitivity analysis of volcanic aerosol dispersion in the stratosphere. [Mt. Fuego, Guatemala eruptions

Science.gov (United States)

Butler, C. F.

1979-01-01

A computer sensitivity analysis was performed to determine the uncertainties involved in the calculation of volcanic aerosol dispersion in the stratosphere using a 2 dimensional model. The Fuego volcanic event of 1974 was used. Aerosol dispersion processes that were included are: transport, sedimentation, gas phase sulfur chemistry, and aerosol growth. Calculated uncertainties are established from variations in the stratospheric aerosol layer decay times at 37 latitude for each dispersion process. Model profiles are also compared with lidar measurements. Results of the computer study are quite sensitive (factor of 2) to the assumed volcanic aerosol source function and the large variations in the parameterized transport between 15 and 20 km at subtropical latitudes. Sedimentation effects are uncertain by up to a factor of 1.5 because of the lack of aerosol size distribution data. The aerosol chemistry and growth, assuming that the stated mechanisms are correct, are essentially complete in several months after the eruption and cannot explain the differences between measured and modeled results.

Cloud albedo changes in response to anthropogenic sulfate and non-sulfate aerosol forcings in CMIP5 models

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L. Frey

2017-07-01

Full Text Available The effects of different aerosol types on cloud albedo are analysed using the linear relation between total albedo and cloud fraction found on a monthly mean scale in regions of subtropical marine stratocumulus clouds and the influence of simulated aerosol variations on this relation. Model experiments from the Coupled Model Intercomparison Project phase 5 (CMIP5 are used to separately study the responses to increases in sulfate, non-sulfate and all anthropogenic aerosols. A cloud brightening on the month-to-month scale due to variability in the background aerosol is found to dominate even in the cases where anthropogenic aerosols are added. The aerosol composition is of importance for this cloud brightening, that is thereby region dependent. There is indication that absorbing aerosols to some extent counteract the cloud brightening but scene darkening with increasing aerosol burden is generally not supported, even in regions where absorbing aerosols dominate. Month-to-month cloud albedo variability also confirms the importance of liquid water content for cloud albedo. Regional, monthly mean cloud albedo is found to increase with the addition of anthropogenic aerosols and more so with sulfate than non-sulfate. Changes in cloud albedo between experiments are related to changes in cloud water content as well as droplet size distribution changes, so that models with large increases in liquid water path and/or cloud droplet number show large cloud albedo increases with increasing aerosol. However, no clear relation between model sensitivities to aerosol variations on the month-to-month scale and changes in cloud albedo due to changed aerosol burden is found.

Relative importance of nitrate and sulfate aerosol production mechanisms in urban atmospheres

International Nuclear Information System (INIS)

Middleton, P.; Kiang, C.S.

1979-01-01

The relative importance of the various sulfate and nitrate aerosol production mechanisms is calculated for different atmospheric conditions. The calculation scheme used to determine the rates of nitrate and sulfate production, based on the concept that vapor transfer to the aerosols and nitrate and sulfate formation within the aerosols are coupled kinetic processes, considers sulfate formation by ozone and hydrogen peroxide oxidation and catalytic oxidation in the presence of soot, iron and manganese of sulfite solutions and sulfuric acid condensation and nitrate formation by the liquid-phase oxidation of dissolved nitrogen oxides for different initial gas concentrations and particle compositions and sizes. It is found that sulfate production is higher under daytime conditions, primarily proceeding by mechanisms involving sulfuric acid and hydrogen peroxide, while at night oxidation processes on the surface of the aerosol film are more important. Nitrate tends to decrease nighttime sulfate production due to an increase in aerosol acidity and nitrate production is found to be higher under nighttime conditions and in the winter

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.

The ten-year pattern (1978-1987) of stratospheric aerosol loading using ground-based radiometry

International Nuclear Information System (INIS)

Michalsky, J.J.; Pearson, E.W.; LeBaron, B.A.

1988-09-01

In this paper the procedures used to obtain a stratospheric measurement with ground-based sun radiometry are reviewed briefly. The five-wavelength optical depths are then used to study the evolution of aerosol size during the decade. The time history of loading from the instruments described are compared. Particular emphasis will be placed on the Garmisch-Partenkirchen data because their latitude is very nearly that of the PNL site. The most useful data for this study are those observational records that measure total stratospheric aerosol burden and include the early period and continue throughout the eruption and decay of El Chichon. The lidar data from Langley Research Center and Fraunhofer-Institute for Atmospheric Environmental Research at Garmisch-Partenkirchen, the SAM II satellite data, and the Pacific Northwest Laboratory (PNL) sun radiometry are the published contiguous measurements of the stratosphere aerosol burden during this period. 16 refs., 6 figs

Unexpected high 35S concentration revealing strong downward transport of stratospheric air during the monsoon transitional period in East Asia

Science.gov (United States)

Lin, Mang; Zhang, Zhisheng; Su, Lin; Su, Binbin; Liu, Lanzhong; Tao, Jun; Fung, Jimmy C. H.; Thiemens, Mark H.

2016-03-01

October is the monsoon transitional period in East Asia (EA) involving a series of synoptic activities that may enhance the downward transport of stratospheric air to the planetary boundary layer (PBL). Here we use cosmogenic 35S in sulfate aerosols (35SO42-) as a tracer for air masses originating from the stratosphere and transported downward to quantify these mixing processes. From 1 year 35SO42- measurements (March 2014 to February 2015) at a background station in EA we find remarkably enhanced 35SO42- concentration (3150 atoms m-3) in October, the highest value ever reported for natural sulfate aerosols. A four-box 1-D model and meteorological analysis reveal that strong downward transport from the free troposphere is a vital process entraining aged stratospheric air masses to the PBL. The aged stratospheric masses are accumulated in the PBL, accelerating the SO2 transformation to SO42-. Implications for the tropospheric O3 budget and the CO2 biogeochemical cycle are discussed.

Stratospheric aerosol geoengineering

Energy Technology Data Exchange (ETDEWEB)

Robock, Alan [Department of Environmental Sciences, Rutgers University, 14 College Farm Road, New Brunswick, NJ 08901 (United States)

2015-03-30

The Geoengineering Model Intercomparison Project, conducting climate model experiments with standard stratospheric aerosol injection scenarios, has found that insolation reduction could keep the global average temperature constant, but global average precipitation would reduce, particularly in summer monsoon regions around the world. Temperature changes would also not be uniform; the tropics would cool, but high latitudes would warm, with continuing, but reduced sea ice and ice sheet melting. Temperature extremes would still increase, but not as much as without geoengineering. If geoengineering were halted all at once, there would be rapid temperature and precipitation increases at 5–10 times the rates from gradual global warming. The prospect of geoengineering working may reduce the current drive toward reducing greenhouse gas emissions, and there are concerns about commercial or military control. Because geoengineering cannot safely address climate change, global efforts to reduce greenhouse gas emissions and to adapt are crucial to address anthropogenic global warming.

Stratospheric aerosol geoengineering

International Nuclear Information System (INIS)

Robock, Alan

2015-01-01

The Geoengineering Model Intercomparison Project, conducting climate model experiments with standard stratospheric aerosol injection scenarios, has found that insolation reduction could keep the global average temperature constant, but global average precipitation would reduce, particularly in summer monsoon regions around the world. Temperature changes would also not be uniform; the tropics would cool, but high latitudes would warm, with continuing, but reduced sea ice and ice sheet melting. Temperature extremes would still increase, but not as much as without geoengineering. If geoengineering were halted all at once, there would be rapid temperature and precipitation increases at 5–10 times the rates from gradual global warming. The prospect of geoengineering working may reduce the current drive toward reducing greenhouse gas emissions, and there are concerns about commercial or military control. Because geoengineering cannot safely address climate change, global efforts to reduce greenhouse gas emissions and to adapt are crucial to address anthropogenic global warming

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.

Volcanic eruptions and the increases in the stratospheric aerosol content: Lidar measurements from 1982 to 1986

Science.gov (United States)

Hayashida, S.; Iikura, Y.; Shimizu, H.; Sasano, Y.; Nakane, H.; Sugimoto, N.; Matsui, I.; Takeuchi, N.

1986-01-01

The results of the observation for stratospheric aerosols which were carried out since the autumn of 1982 by using the NIES large lidar are described. Specifications of the lidar system are shown. The lidar has two wavelenghts of 1.06 and 0.53 micrometers. The 0.53 micrometer is mainly used for the stratospheric aerosols, because the PMT for 0.53 micrometers has higher sensitivity that that for 1.06 micrometers and the total efficiency is higher in the former. A switching circuit is used to control the PMT gain for avoiding signal induced noise in PMT. For the last four years, the stratospheric aerosol layer which was significantly perturbed by the El Chichon volcanic eruption was observed. The scattering ratio profiles observed from 1982 through 1983 are given.

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Science.gov (United States)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

Biogenic, anthropogenic and sea salt sulfate size-segregated aerosols in the Arctic summer

Directory of Open Access Journals (Sweden)

R. Ghahremaninezhad

2016-04-01

Full Text Available Size-segregated aerosol sulfate concentrations were measured on board the Canadian Coast Guard Ship (CCGS Amundsen in the Arctic during July 2014. The objective of this study was to utilize the isotopic composition of sulfate to address the contribution of anthropogenic and biogenic sources of aerosols to the growth of the different aerosol size fractions in the Arctic atmosphere. Non-sea-salt sulfate is divided into biogenic and anthropogenic sulfate using stable isotope apportionment techniques. A considerable amount of the average sulfate concentration in the fine aerosols with a diameter  <  0.49 µm was from biogenic sources (>  63 %, which is higher than in previous Arctic studies measuring above the ocean during fall (<  15 % (Rempillo et al., 2011 and total aerosol sulfate at higher latitudes at Alert in summer (>  30 % (Norman et al., 1999. The anthropogenic sulfate concentration was less than that of biogenic sulfate, with potential sources being long-range transport and, more locally, the Amundsen's emissions. Despite attempts to minimize the influence of ship stack emissions, evidence from larger-sized particles demonstrates a contribution from local pollution. A comparison of δ34S values for SO2 and fine aerosols was used to show that gas-to-particle conversion likely occurred during most sampling periods. δ34S values for SO2 and fine aerosols were similar, suggesting the same source for SO2 and aerosol sulfate, except for two samples with a relatively high anthropogenic fraction in particles  <  0.49 µm in diameter (15–17 and 17–19 July. The high biogenic fraction of sulfate fine aerosol and similar isotope ratio values of these particles and SO2 emphasize the role of marine organisms (e.g., phytoplankton, algae, bacteria in the formation of fine particles above the Arctic Ocean during the productive summer months.

Possible effect of strong solar energetic particle events on polar stratospheric aerosol: a summary of observational results

International Nuclear Information System (INIS)

Mironova, I A; Usoskin, I G

2014-01-01

This letter presents a summary of a phenomenological study of the response of the polar stratosphere to strong solar energetic particle (SEP) events corresponding to ground level enhancements (GLEs) of cosmic rays. This work is focused on evaluation of the possible influence of the atmospheric ionization caused by SEPs upon formation of aerosol particles in the stratosphere over polar regions. Following case studies of two major SEP/GLE events, in January 2005 and September 1989, and their possible effects on polar stratospheric aerosols, we present here the results of an analysis of variations of the daily profiles of the stratospheric aerosol parameters (aerosol extinction for different wavelengths, as well as Ångstrom exponent) for both polar hemispheres during SEP/GLE events of July 2000, April 2001 and October 2003, which form already five clear cases corresponding to extreme and strong SEP/GLE events. The obtained results suggest that an enhancement of ionization rate by a factor of about two in the polar region with night/cold/winter conditions can lead to the formation/growing of aerosol particles in the altitude range of 10–25 km. We also present a summary of the investigated effects based on the phenomenological study of the atmospheric application of extreme SEP events. (paper)

Comparison of the impact of volcanic eruptions and aircraft emissions on the aerosol mass loading and sulfur budget in the stratosphere

Science.gov (United States)

Yue, Glenn K.; Poole, Lamont R.

1992-01-01

Data obtained by the Stratospheric Aerosol and Gas Experiment (SAGE) 1 and 2 were used to study the temporal variation of aerosol optical properties and to assess the mass loading of stratospheric aerosols from the eruption of volcanos Ruiz and Kelut. It was found that the yearly global average of optical depth at 1.0 micron for stratospheric background aerosols in 1979 was 1.16 x 10(exp -3) and in 1989 was 1.66 x 10(exp -3). The eruptions of volcanos Ruiz and Kelut ejected at least 5.6 x 10(exp 5) and 1.8 x 10(exp 5) tons of materials into the stratosphere, respectively. The amount of sulfur emitted per year from the projected subsonic and supersonic fleet is comparable to that contained in the background aerosol particles in midlatitudes from 35 deg N to 55 deg N.

Sulfate Formation on Mars by Volcanic Aerosols: A New Look

Science.gov (United States)

Blaney, D. L.

1996-03-01

Sulfur was measured at both Viking Lander sites in abundances of 5-9 wt % SO3. Because the sulfur was more concentrated in clumps which disintegrated and the general oxidized nature of the Martian soil, these measurements led to the assumption that a sulfate duricrust existed. Two types of models for sulfate formation have been proposed. One is a formation by upwardly migrating ground water. The other is the formation of sulfates by the precipitation of volcanic aerosols. Most investigators have tended to favor the ground water origin of sulfates on Mars. However, evidence assemble since Viking may point to a volcanic aerosol origin.

The role of carbonyl sulphide as a source of stratospheric sulphate aerosol and its impact on climate

Directory of Open Access Journals (Sweden)

C. Brühl

2012-02-01

Full Text Available Globally, carbonyl sulphide (COS is the most abundant sulphur gas in the atmosphere. Our chemistry-climate model (CCM of the lower and middle atmosphere with aerosol module realistically simulates the background stratospheric sulphur cycle, as observed by satellites in volcanically quiescent periods. The model results indicate that upward transport of COS from the troposphere largely controls the sulphur budget and the aerosol loading of the background stratosphere. This differs from most previous studies which indicated that short-lived sulphur gases are also important. The model realistically simulates the modulation of the particulate and gaseous sulphur abundance in the stratosphere by the quasi-biennial oscillation (QBO. In the lowermost stratosphere organic carbon aerosol contributes significantly to extinction. Further, using a chemical radiative convective model and recent spectra, we compute that the direct radiative forcing efficiency by 1 kg of COS is 724 times that of 1 kg CO₂. Considering an anthropogenic fraction of 30% (derived from ice core data, this translates into an overall direct radiative forcing by COS of 0.003 W m⁻². The direct global warming potentials of COS over time horizons of 20 and 100 yr are GWP(20 yr = 97 and GWP(100 yr = 27, respectively (by mass. Furthermore, stratospheric aerosol particles produced by the photolysis of COS (chemical feedback contribute to a negative direct solar radiative forcing, which in the CCM amounts to −0.007 W m⁻² at the top of the atmosphere for the anthropogenic fraction, more than two times the direct warming forcing of COS. Considering that the lifetime of COS is twice that of stratospheric aerosols the warming and cooling tendencies approximately cancel.

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

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......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......-limiting step may be the oxidation of sulfite to sulfate, rather than the oxidation of SO2 to SO3 proposed previously. Even though the proposed model is consistent with experimental observations, experiments in a rigorously homogeneous system are called for to test its validity....

Possible effect of extreme solar energetic particle event of 20 January 2005 on polar stratospheric aerosols: direct observational evidence

Directory of Open Access Journals (Sweden)

I. A. Mironova

2012-01-01

Full Text Available Energetic cosmic rays are the main source of ionization of the low-middle atmosphere, leading to associated changes in atmospheric properties. Via the hypothetical influence of ionization on aerosol growth and facilitated formation of clouds, this may be an important indirect link relating solar variability to climate. This effect is highly debated, however, since the proposed theoretical mechanisms still remain illusive and qualitative, and observational evidence is inconclusive and controversial. Therefore, important questions regarding the existence and magnitude of the effect, and particularly the fraction of aerosol particles that can form and grow, are still open. Here we present empirical evidence of the possible effect caused by cosmic rays upon polar stratospheric aerosols, based on a case study of an extreme solar energetic particle (SEP event of 20 January 2005. Using aerosol data obtained over polar regions from different satellites with optical instruments that were operating during January 2005, such as the Stratospheric Aerosol and Gas Experiment III (SAGE III, and Optical Spectrograph and Infrared Imaging System (OSIRIS, we found a significant simultaneous change in aerosol properties in both the Southern and Northern Polar regions in temporal association with the SEP event. We speculate that ionization of the atmosphere, which was abnormally high in the lower stratosphere during the extreme SEP event, might have led to formation of new particles and/or growth of preexisting ultrafine particles in the polar stratospheric region. However, a detailed interpretation of the effect is left for subsequent studies. This is the first time high vertical resolution measurements have been used to discuss possible production of stratospheric aerosols under the influence of cosmic ray induced ionization. The observed effect is marginally detectable for the analyzed severe SEP event and can be undetectable for the majority of weak

Possible effect of extreme solar energetic particle event of 20 January 2005 on polar stratospheric aerosols: direct observational evidence

Science.gov (United States)

Mironova, I. A.; Usoskin, I. G.; Kovaltsov, G. A.; Petelina, S. V.

2012-01-01

Energetic cosmic rays are the main source of ionization of the low-middle atmosphere, leading to associated changes in atmospheric properties. Via the hypothetical influence of ionization on aerosol growth and facilitated formation of clouds, this may be an important indirect link relating solar variability to climate. This effect is highly debated, however, since the proposed theoretical mechanisms still remain illusive and qualitative, and observational evidence is inconclusive and controversial. Therefore, important questions regarding the existence and magnitude of the effect, and particularly the fraction of aerosol particles that can form and grow, are still open. Here we present empirical evidence of the possible effect caused by cosmic rays upon polar stratospheric aerosols, based on a case study of an extreme solar energetic particle (SEP) event of 20 January 2005. Using aerosol data obtained over polar regions from different satellites with optical instruments that were operating during January 2005, such as the Stratospheric Aerosol and Gas Experiment III (SAGE III), and Optical Spectrograph and Infrared Imaging System (OSIRIS), we found a significant simultaneous change in aerosol properties in both the Southern and Northern Polar regions in temporal association with the SEP event. We speculate that ionization of the atmosphere, which was abnormally high in the lower stratosphere during the extreme SEP event, might have led to formation of new particles and/or growth of preexisting ultrafine particles in the polar stratospheric region. However, a detailed interpretation of the effect is left for subsequent studies. This is the first time high vertical resolution measurements have been used to discuss possible production of stratospheric aerosols under the influence of cosmic ray induced ionization. The observed effect is marginally detectable for the analyzed severe SEP event and can be undetectable for the majority of weak-moderate events. The present

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

Science.gov (United States)

Toohey, M.; Krüger, K.; Bittner, M.; Timmreck, C.; Schmidt, H.

2014-12-01

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 simulated 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 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. Both observation-based forcing sets result in insignificant changes in vortex strength. For the model-based forcing sets, the vortex response is found to be sensitive to the structure of the forcing, with one forcing set leading to significant strengthening of the polar vortex in rough agreement with observation-based expectations. Differences in the dynamical response to the forcing sets imply that reproducing the polar vortex responses to past eruptions, or predicting the response to future eruptions, depends on accurate representation of the space-time structure of the volcanic aerosol forcing.

Characteristics of Volcanic Stratospheric Aerosol Layer Observed by CALIOP and Ground Based Lidar at Equatorial Atmosphere Radar Site

Science.gov (United States)

Abo, Makoto; Shibata, Yasukuni; Nagasawa, Chikao

2018-04-01

We investigated the relation between major tropical volcanic eruptions in the equatorial region and the stratospheric aerosol data, which have been collected by the ground based lidar observations at at Equatorial Atmosphere Radar site between 2004 and 2015 and the CALIOP observations in low latitude between 2006 and 2015. We found characteristic dynamic behavior of volcanic stratospheric aerosol layers over equatorial region.

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.

Modeling of Solar Radiation Management: A Comparison of Simulations Using Reduced Solar Constant and Stratospheric Sulphate Aerosols

Science.gov (United States)

Bala, G.; Kalidindi, S.; Modak, A.; Caldeira, K.

2014-12-01

Several climate modelling studies in the past have used reduction in solar constant to simulate the climatic effects of Solar Radiation Management (SRM) geoengineering. This is most likely valid only for space-based mirrors/reflectors but not for SRM methods that rely on stratospheric aerosols. In this study, we use a climate model to evaluate the differences in climate response to SRM by uniform solar constant reduction and stratospheric aerosols. The experiments are designed such that global mean warming from a doubling of atmospheric CO2 concentration (2xCO2) is nearly cancelled in each case. In such a scenario, the residual climate effects are similar when important surface and tropospheric climate variables such as temperature and precipitation are considered. However, there are significant differences in stratospheric temperature response and diffuse and direct radiation reaching the surface. A difference of 1K in the global mean stratospheric (61-9.8 hPa) temperature is simulated between the two SRM methods, with warming in the aerosol scheme and a slight cooling for sunshades. While the global mean surface diffuse radiation increases by ~23% and direct radiation decreases by about 9% in the case of aerosol SRM method, both direct and diffuse radiation decrease by similar fractional amounts (~1.0%) when solar constant is reduced. When CO2 fertilization effects from elevated CO2 concentration levels are removed, the contribution from shaded leaves to gross primary productivity (GPP) increases by 1.8 % in aerosol SRM because of increased diffuse light. However, this increase is almost offset by a 15.2% decline in sunlit contribution due to reduced direct light. Overall both the SRM simulations show similar decrease in GPP (~ 8%) and NPP (~3%) relative to 2xCO2, indicating the negligible effect of the fractional changes in direct/diffuse radiation on the overall plant productivity. Based on our modelling study, we conclude that the climate states produced by a

A risk-based framework for assessing the effectiveness of stratospheric aerosol geoengineering.

Directory of Open Access Journals (Sweden)

Angus J Ferraro

Full Text Available Geoengineering by stratospheric aerosol injection has been proposed as a policy response to warming from human emissions of greenhouse gases, but it may produce unequal regional impacts. We present a simple, intuitive risk-based framework for classifying these impacts according to whether geoengineering increases or decreases the risk of substantial climate change, with further classification by the level of existing risk from climate change from increasing carbon dioxide concentrations. This framework is applied to two climate model simulations of geoengineering counterbalancing the surface warming produced by a quadrupling of carbon dioxide concentrations, with one using a layer of sulphate aerosol in the lower stratosphere, and the other a reduction in total solar irradiance. The solar dimming model simulation shows less regional inequality of impacts compared with the aerosol geoengineering simulation. In the solar dimming simulation, 10% of the Earth's surface area, containing 10% of its population and 11% of its gross domestic product, experiences greater risk of substantial precipitation changes under geoengineering than under enhanced carbon dioxide concentrations. In the aerosol geoengineering simulation the increased risk of substantial precipitation change is experienced by 42% of Earth's surface area, containing 36% of its population and 60% of its gross domestic product.

A Risk-Based Framework for Assessing the Effectiveness of Stratospheric Aerosol Geoengineering

Science.gov (United States)

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

2014-01-01

Geoengineering by stratospheric aerosol injection has been proposed as a policy response to warming from human emissions of greenhouse gases, but it may produce unequal regional impacts. We present a simple, intuitive risk-based framework for classifying these impacts according to whether geoengineering increases or decreases the risk of substantial climate change, with further classification by the level of existing risk from climate change from increasing carbon dioxide concentrations. This framework is applied to two climate model simulations of geoengineering counterbalancing the surface warming produced by a quadrupling of carbon dioxide concentrations, with one using a layer of sulphate aerosol in the lower stratosphere, and the other a reduction in total solar irradiance. The solar dimming model simulation shows less regional inequality of impacts compared with the aerosol geoengineering simulation. In the solar dimming simulation, 10% of the Earth's surface area, containing 10% of its population and 11% of its gross domestic product, experiences greater risk of substantial precipitation changes under geoengineering than under enhanced carbon dioxide concentrations. In the aerosol geoengineering simulation the increased risk of substantial precipitation change is experienced by 42% of Earth's surface area, containing 36% of its population and 60% of its gross domestic product. PMID:24533155

Effects on stratospheric moistening by rates of change of aerosol optical depth and ozone due to solar activity in extra-tropics

Science.gov (United States)

Saha, U.; Maitra, A.

2014-11-01

The solar-induced changes in ozone and aerosol optical depth have relative effects on stratospheric moistening at upper troposphere/lower stratosphere region. Wavelet-based multi-scale principal component analysis technique has been applied to de-noise component of quasi-biennial oscillation and El Niño-Southern Oscillation from ozone and aerosol optical depth variations. Rate of change of aerosol optical depth sharply increases indicating a positive gradient whereas rate of change of ozone sharply decreases indicating a negative gradient with solar activity during the years 2004-2010. It is also observed that with increase of rate of change of aerosol optical depth, there is a sharp increase of stratospheric moistening caused by enhanced deep convection. On the contrary, with the increase of stratospheric moistening, there is a sharp decrease of rate of change of ozone resulting in a cross-over between the two parameters. An increase in aerosol optical depth may cause a significant increase in the gradient of vertical temperature profile, as well as formation of cloud condensation nuclei, clouds and hence rainfall. This may lead to formation of strong convective system in the atmosphere that is essential for vertical transfer of water vapour in the tropics percolating tropical tropopause layer and depleting stratospheric ozone in the extra-tropics.

Effect of Sulfate Aerosol Geoengineering on Tropical cyclones

Science.gov (United States)

Wang, Q.; Moore, J.; Ji, D.

2017-12-01

Variation in tropical cyclone (TC) number and intensity is driven in part by changes in the thermodynamics that can be defined by ocean and atmospheric variables. Genesis Potential Index (GPI) and ventilation index (VI) are combinations of potential intensity, vertical wind shear, relative humidity, midlevel entropy deficit, and absolute vorticity that quantify thermodynamic forcing of TC activity under changed climates, and can be calculated from climate model output. Here we use five CMIP5 models running the RCP45 experiment the Geoengineering Model Intercomparison Project (GeoMIP) stratospheric aerosol injection G4 experiment to calculate the two indices over the 2020 to 2069 period. Globally, GPI under G4 is lower than under RCP45, though both have a slight increasing trend. Spatial patterns in the relative effectiveness of geoengineering show reductions in TC in all models in the North Atlantic basin, and northern Indian Ocean in all except NorESM1-M. In the North Pacific, most models also show relative reductions under G4. VI generally coincide with the GPI patterns. Most models project Potential intensity and Relative Humidity to be the dominant variable to affect genesis potential. Changes in vertical wind shear and vorticity are small with scatter across different models and ocean basins. We find that tropopause temperature maybe as important as sea surface temperature in effecting TC genesis. Thus stratospheric aerosol geoengineering impacts on potential intensity and hence TC intensity are reasonably consistent, but probably underestimated by statistical forecasts of Tropical North Atlantic hurricane activity driven by sea surface temperatures alone. However the impacts of geoengineering on other ocean basins are more difficult to assess, and require more complete understanding of their driving parameters under present day climates. Furthermore, the possible effects of stratospheric injection on chemical reactions in the stratosphere, such as ozone, are

Global source attribution of sulfate aerosol and its radiative forcing

Science.gov (United States)

Yang, Y.; Wang, H.; Smith, S.; Easter, R. C.; Ma, P. L.; Qian, Y.; Li, C.; Yu, H.; Rasch, P. J.

2017-12-01

Sulfate is an important aerosol that poses health risks and influences climate. Due to long-range atmospheric transport, local sulfate pollution could result from intercontinental influences, making domestic efforts of improving air quality inefficient. Accurate understanding of source attribution of sulfate and its radiative forcing is important for both regional air quality improvement and global climate mitigation. In this study, for the first time, a sulfur source-tagging capability is implemented in the Community Atmosphere Model (CAM5) to quantify the global source-receptor relationships of sulfate and its direct and indirect radiative forcing (DRF and IRF). Near-surface sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate is primarily attributed to non-local sources from long-range transport. The export of SO2 and sulfate from Europe contributes 20% of sulfate concentrations over North Africa, Russia and Central Asia. Sources from the Middle East account for 20% of sulfate over North Africa, Southern Africa and Central Asia in winter and autumn, and 20% over South Asia in spring. East Asia accounts for about 50% of sulfate over Southeast Asia in winter and autumn, 15% over Russia in summer, and 10% over North America in spring. South Asia contributes to 25% of sulfate over Southeast Asia in spring. Lifetime of aerosols, together with regional export, is found to determine regional air quality. The simulated global total sulfate DRF is -0.42 W m-2, with 75% contributed by anthropogenic sulfate and 25% contributed by natural sulfate. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes the most to the total DRF. East Asia has the largest contribution of 20-30% over the Northern Hemisphere mid- and high-latitudes. A 20% perturbation of sulfate and its precursor emissions gives a sulfate IRF of -0.44 W m-2. DMS has the

30-year lidar observations of the stratospheric aerosol layer state over Tomsk (Western Siberia, Russia)

Science.gov (United States)

Zuev, Vladimir V.; Burlakov, Vladimir D.; Nevzorov, Aleksei V.; Pravdin, Vladimir L.; Savelieva, Ekaterina S.; Gerasimov, Vladislav V.

2017-02-01

There are only four lidar stations in the world which have almost continuously performed observations of the stratospheric aerosol layer (SAL) state over the last 30 years. The longest time series of the SAL lidar measurements have been accumulated at the Mauna Loa Observatory (Hawaii) since 1973, the NASA Langley Research Center (Hampton, Virginia) since 1974, and Garmisch-Partenkirchen (Germany) since 1976. The fourth lidar station we present started to perform routine observations of the SAL parameters in Tomsk (56.48° N, 85.05° E, Western Siberia, Russia) in 1986. In this paper, we mainly focus on and discuss the stratospheric background period from 2000 to 2005 and the causes of the SAL perturbations over Tomsk in the 2006-2015 period. During the last decade, volcanic aerosol plumes from tropical Mt. Manam, Soufrière Hills, Rabaul, Merapi, Nabro, and Kelut and extratropical (northern) Mt. Okmok, Kasatochi, Redoubt, Sarychev Peak, Eyjafjallajökull, and Grímsvötn were detected in the stratosphere over Tomsk. When it was possible, we used the NOAA HYSPLIT trajectory model to assign aerosol layers observed over Tomsk to the corresponding volcanic eruptions. The trajectory analysis highlighted some surprising results. For example, in the cases of the Okmok, Kasatochi, and Eyjafjallajökull eruptions, the HYSPLIT air mass backward trajectories, started from altitudes of aerosol layers detected over Tomsk with a lidar, passed over these volcanoes on their eruption days at altitudes higher than the maximum plume altitudes given by the Smithsonian Institution Global Volcanism Program. An explanation of these facts is suggested. The role of both tropical and northern volcanic eruptions in volcanogenic aerosol loading of the midlatitude stratosphere is also discussed. In addition to volcanoes, we considered other possible causes of the SAL perturbations over Tomsk, i.e., the polar stratospheric cloud (PSC) events and smoke plumes from strong forest fires. At least

Toward a combined SAGE II-HALOE aerosol climatology: an evaluation of HALOE version 19 stratospheric aerosol extinction coefficient observations

Directory of Open Access Journals (Sweden)

L. W. Thomason

2012-09-01

Full Text Available Herein, the Halogen Occultation Experiment (HALOE aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 μm is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 μm is biased by about 10% throughout the lower stratosphere due to the failure to clear NO₂ but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 μm aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40 μm aerosol extinction coefficient measurements can be improved through the inclusion of an NO₂ correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 μm channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived

Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

Science.gov (United States)

Thomason, L. W.

2012-01-01

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

Stratospheric changes caused by geoengineering applications: potential repercussions and uncertainties

Science.gov (United States)

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

2009-04-01

not capable to reliably predict the changes in stratospheric climate following geoengineering applications. Rasch, P. J. et al. (2008), Exploring the geoengineering of climate using stratospheric sulfate aerosols: The role of particle size, Geophysical Research Letters, 35 (2), L02,809. Tilmes, S. et al. (2008), The sensitivity of polar ozone depletion to proposed geoengineering schemes, Science, 320 (5880), 1201-1204.

The Stratospheric Aerosol and Gas Experiment (SAGE III) on the International Space Station (ISS) Mission

Science.gov (United States)

Cisewski, Michael; Zawodny, Joseph; Gasbarre, Joseph; Eckman, Richard; Topiwala, Nandkishore; Rodriquez-Alvarez, Otilia; Cheek, Dianne; Hall, Steve

2014-01-01

The Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS) mission will provide the science community with high-vertical resolution and nearly global observations of ozone, aerosols, water vapor, nitrogen dioxide, and other trace gas species in the stratosphere and upper-troposphere. SAGE III/ISS measurements will extend the long-term Stratospheric Aerosol Measurement (SAM) and SAGE data record begun in the 1970s. The multi-decadal SAGE ozone and aerosol data sets have undergone intense scrutiny and are considered the international standard for accuracy and stability. SAGE data have been used to monitor the effectiveness of the Montreal Protocol. Key objectives of the mission are to assess the state of the recovery in the distribution of ozone, to re-establish the aerosol measurements needed by both climate and ozone models, and to gain further insight into key processes contributing to ozone and aerosol variability. The space station mid-inclination orbit allows for a large range in latitude sampling and nearly continuous communications with payloads. The SAGE III instrument is the fifth in a series of instruments developed for monitoring atmospheric constituents with high vertical resolution. The SAGE III instrument is a moderate resolution spectrometer covering wavelengths from 290 nm to 1550 nm. Science data is collected in solar occultation mode, lunar occultation mode, and limb scatter measurement mode. A SpaceX Falcon 9 launch vehicle will provide access to space. Mounted in the unpressurized section of the Dragon trunk, SAGE III will be robotically removed from the Dragon and installed on the space station. SAGE III/ISS will be mounted to the ExPRESS Logistics Carrier-4 (ELC-4) location on the starboard side of the station. To facilitate a nadir view from this location, a Nadir Viewing Platform (NVP) payload was developed which mounts between the carrier and the SAGE III Instrument Payload (IP).

A simple method to compute the change in earth-atmosphere radiative balance due to a stratospheric aerosol layer

Science.gov (United States)

Lenoble, J.; Tanre, D.; Deschamps, P. Y.; Herman, M.

1982-01-01

A computer code was developed in terms of a three-layer model for the earth-atmosphere system, using a two-stream approximation for the troposphere and stratosphere. The analysis was limited to variable atmosphere loading by solar radiation over an unperturbed section of the atmosphere. The scattering atmosphere above a Lambertian ground layer was considered in order to derive the planar albedo and the spherical albedo. Attention was given to the influence of the aerosol optical thickness in the stratosphere, the single scattering albedo and asymmetry factor, and the sublayer albedo. Calculations were performed of the zonal albedo and the planetary radiation balance, taking into account a stratospheric aerosol layer containing H2SO4 droplets and volcanic ash. The resulting ground temperature disturbance was computed using a Budyko (1969) climate model. Local decreases in the albedo in the summer were observed in high latitudes, implying a heating effect of the aerosol. An accompanying energy loss of 23-27 W/sq m was projected, which translates to surface temperature decreases of either 1.1 and 0.45 C, respectively, for background and volcanic aerosols.

Comparing Simultaneous Stratospheric Aerosol and Ozone Lidar Measurements with SAGE 2 Data after the Mount Pinatubo Eruption

Science.gov (United States)

Yue, G. K.; Poole, L. R.; McCormick, M. P.; Veiga, R. E.; Wang, P.-H.; Rizi, V.; Masci, F.; DAltorio, A.; Visconti, G.

1995-01-01

Stratospheric aerosol and ozone profiles obtained simultaneously from the lidar station at the University of L'Aquila (42.35 deg N, 13.33 deg E, 683 m above sea level) during the first 6 months following the eruption of Mount Pinatubo are compared with corresponding nearby Stratospheric Aerosol and Gas Experiment (SAGE) 2 profiles. The agreement between the two data sets is found to be reasonably good. The temporal change of aerosol profiles obtained by both techniques showed the intrusion and growth of Pinatubo aerosols. In addition, ozone concentration profiles derived from an empirical time-series model based on SAGE 2 ozone data obtained before the Pinatubo eruption are compared with measured profiles. Good agreement is shown in the 1991 profiles, but ozone concentrations measured in January 1992 were reduced relative to time-series model estimates. Possible reasons for the differences between measured and model-based ozone profiles are discussed.

Temperature thresholds for chlorine activation and ozone loss in the polar stratosphere

Energy Technology Data Exchange (ETDEWEB)

Drdla, K. [NASA Ames Research Center, Moffett Field, CA (United States); Mueller, R. [Forschungszentrum Juelich (DE). Inst. of Energy and Climate Research (IEK-7)

2012-07-01

Low stratospheric temperatures are known to be responsible for heterogeneous chlorine activation that leads to polar ozone depletion. Here, we discuss the temperature threshold below which substantial chlorine activation occurs. We suggest that the onset of chlorine activation is dominated by reactions on cold binary aerosol particles, without the formation of polar stratospheric clouds (PSCs), i.e. without any significant uptake of HNO{sub 3} from the gas phase. Using reaction rates on cold binary aerosol in a model of stratospheric chemistry, a chlorine activation threshold temperature, T{sub ACL}, is derived. At typical stratospheric conditions, T{sub ACL} is similar in value to T{sub NAT} (within 1-2 K), the highest temperature at which nitric acid trihydrate (NAT) can exist. T{sub NAT} is still in use to parameterise the threshold temperature for the onset of chlorine activation. However, perturbations can cause T{sub ACL} to differ from T{sub NAT}: T{sub ACL} is dependent upon H{sub 2} O and potential temperature, but unlike T{sub NAT} is not dependent upon HNO3. Furthermore, in contrast to T{sub NAT}, T{sub ACL} is dependent upon the stratospheric sulfate aerosol loading and thus provides a means to estimate the impact on polar ozone of strong volcanic eruptions and some geo-engineering options, which are discussed. A parameterisation of T{sub ACL} is provided here, allowing it to be calculated for low solar elevation (or high solar zenith angle) over a comprehensive range of stratospheric conditions. Considering T{sub ACL} as a proxy for chlorine activation cannot replace a detailed model calculation, and polar ozone loss is influenced by other factors apart from the initial chlorine activation. However, T{sub ACL} provides a more accurate description of the temperature conditions necessary for chlorine activation and ozone loss in the polar stratosphere than T{sub NAT}. (orig.)

Sulfates, Clouds and Radiation Brazil (SCAR-B) AERONET (AErosol RObotic NETwork) Data

Data.gov (United States)

National Aeronautics and Space Administration — SCAR_B_AERONET data are Smoke, Clouds and Radiation Brazil (SCARB) Aerosol Robotic Network (AERONET) data for aerosol characterization.Smoke/Sulfates, Clouds and...

Effects of Volcanic Eruptions on Stratospheric Ozone Recovery

Science.gov (United States)

Rosenfield, Joan E.

2002-01-01

The effects of the stratospheric sulfate aerosol layer associated with the Mt. Pinatubo volcano and future volcanic eruptions on the recovery of the ozone layer is studied with an interactive two-dimensional photochemical model. The time varying chlorine loading and the stratospheric cooling due to increasing carbon dioxide have been taken into account. The computed ozone and temperature changes associated with the Mt. Pinatubo eruption in 1991 agree well with observations. Long model runs out to the year 2050 have been carried out, in which volcanoes having the characteristics of the Mount Pinatubo volcano were erupted in the model at 10-year intervals starting in the year 2010. Compared to a non-volcanic run using background aerosol loading, transient reductions of globally averaged column ozone of 2-3 percent were computed as a result of each of these eruptions, with the ozone recovering to that computed for the non-volcanic case in about 5 years after the eruption. Computed springtime Arctic column ozone losses of from 10 to 18 percent also recovered to the non-volcanic case within 5 years. These results suggest that the long-term recovery of ozone would not be strongly affected by infrequent volcanic eruptions with a sulfur loading approximating Mt. Pinatubo. Sensitivity studies in which the Arctic lower stratosphere was forced to be 4 K and 10 K colder resulted in transient ozone losses of which also recovered to the non-volcanic case in 5 years. A case in which a volcano five times Mt. Pinatubo was erupted in the year 2010 led to maximum springtime column ozone losses of 45 percent which took 10 years to recover to the background case. Finally, in order to simulate a situation in which frequent smaller volcanic eruptions result in increasing the background sulfate loading, a simulation was made in which the background aerosol was increased by 10 percent per year. This resulted in a delay of the recovery of column ozone to 1980 values of more than 10 years.

Stratospheric Aerosol and Gas Experiments 1 and 2: Comparisons with ozonesondes

Science.gov (United States)

Veiga, Robert E.; Cunnold, Derek M.; Chu, William P.; McCormick, M. Patrick

1995-01-01

Ozone profiles measured by the Stratospheric Aerosol and Gas Experiments (SAGE) 1 and 2 are compared with ozonesonde profiles at 24 stations over the period extending from 1979 through 1991. Ozonesonde/satellite differences at 21 stations with SAGE 2 overpasses were computed down to 11.5 km in midlatitudes, to 15.5 km in the lower latitudes, and for nine stations with SAGE 1 overpasses down to 15.5 km. The set of individual satellite and ozonesonde profile comparisons most closely colocated in time and space shows mean absolute differences relative to the satellite measurement of 6 +/- 2% for SAGE 2 and 8 +/- 3% for SAGE 1. The ensemble of ozonesonde/satellite differences, when averaged over all altitudes, shows that for SAGE 2, 70% were less than 5%, whereas for SAGE 1, 50% were less than 5%. The best agreement occurred in the altitude region near the ozone density maximum where almost all the relative differences were less than 5%. Most of the statistically significant differences occurred below the ozone maximum down to the tropopause in the region of steepest ozone gradients and typically ranged between 0 and -20%. Correlations between ozone and aerosol extinction in the northern midlatitudes indicate that aerosols had no discernible impact on the ozonesonde/satellite differences and on the SAGE 2 ozone retrieval for the levels of extinction encountered in the lower stratosphere during 1984 to mid-1991.

The background aerosol in the lower stratosphere and the tropospheric aerosol in the Alps. Final report; Das Hintergrundaerosol der unteren Stratosphaere und das troposphaerische Aerosol der Alpen. Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Jaeger, H.; Trickl, T.

2001-06-04

As a contribution to the German Aerosol-Lidar Network lidar backscatter measurements have been carried out at Garmisch-Partenkirchen in a wide range of the atmosphere from next to the ground to altitudes beyond 30 km. The investigations, on one hand, were devoted to establishing a climatology of the aerosol extinction coefficient for the northern Alps and to prolonging the long-term measurement series of the stratospheric aerosol. On the other hand, aerosol was used as a tracer of polluted air masses in atmospheric transport studies (orographically induced vertical transport, advection of Saharan dust, as well as aerosol advection from the North american boundary layer and from large-scale wild fire in the United States and Canada). These transport processes given the seasonal cycle of the aerosol throughout the troposphere. In the free troposphere a pronounced spring-time aerosol maximum was found. The stratospheric aerosol concentration had decayed to a background-type level during the reporting period. As a consequence, the influence of smaller aerosol contributions could be distinguished such as the eruption of the volcano Shishaldin (Alaska) and aircraft emissions. (orig.) [German] Im Rahmen des deutschen Aerosollidarnetzes wurden in Garmisch-Partenkirchen Lidar-Rueckstreumessungen in einem weiten Bereich der Atmosphaere von Bodennaehe bis in ueber 30 km Hoehe durchgefuehrt. Die Arbeiten dienten zum einen der Erstellung einer Klimatologie des Aerosol-Extinktionskoeffizienten fuer die Nordalpen sowie der Verlaengerung der seit 1976 erstellten Langzeitmessreihe des stratosphaerischen Aerosols. Zum anderen fanden atmosphaerische Transportstudien statt, bei denen das Aerosol als 'Tracer' fuer Luftverschmutzung verwendet wurde (orographisch induzierter Vertikaltransport, Advektion von Saharastaub und Aerosoladvektion aus der nordamerikanischen Genzschicht und von grossflaechigen Waldbraenden in den U.S.A. und Kanada). Diese Transportprozesse bestimmen den

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.

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

1998-12-31

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.

Volatility of Organic Aerosol: Evaporation of Ammonium Sulfate/Succinic Acid Aqueous Solution Droplets

Science.gov (United States)

2013-01-01

Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol. PMID:24107221

Quantifying the risks of solid aerosol geoengineering: the role of fundamental material properties

Science.gov (United States)

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

2017-12-01

Solid aerosols have been considered as an alternative to sulfate aerosols for solar geoengineering due to their optical and chemical properties, which lead to different and possibly more attractive risk profiles. Solid aerosols can achieve higher solar scattering efficiency due to their higher refractive index, and in some cases may also be less effective absorbers of thermal infrared radiation. The optical properties of solid aerosols are however sensitive functions of the detailed physical properties of solid materials in question. The relevant details include the exact crystalline structure of the aerosols, the physical size of the particles, and interactions with background stratospheric molecular and particulate constituents. In this work, we examine the impact of these detailed physical properties on the radiative properties of calcite (CaCO3) solid aerosols. We examine how crystal morphology, size, chemical reactions, and interaction with background stratospheric aerosol may alter the scattering and absorption properties of calcite aerosols for solar and thermal infrared radiation. For example, in small particles, crystal lattice vibrations associated with the particle surface may lead to substantially different infrared absorption properties than bulk materials. We examine the wavelength dependence of absorption by the particles, which may lead to altered patterns of stratospheric radiative heating and equilibrium temperatures. Such temperature changes can lead to dynamical changes, with consequences for both stratospheric composition and tropospheric climate. We identify important uncertainties in the current state of understanding, investigate risks associated with these uncertainties, and survey potential approaches to quantitatively improving our knowledge of the relevant material properties.

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.

Evidence of transport, sedimentation and coagulation mechanisms in the relaxation of post-volcanic stratospheric aerosols

Directory of Open Access Journals (Sweden)

D. Fussen

2001-09-01

Full Text Available Spatio-temporal distributions of stratospheric aerosols, measured by the ORA instrument from August 1992 until May 1993, are presented in the latitude range (40° S–40° N. Particle total number density, mode radius and distribution width are derived and interpreted. The respective roles of advection, sedimentation and coagulation are discussed. We also identify clear transport/sedimentation patterns and we show the enhancement of coagulation in stagnation regions. Efficient transport of aerosol particles up to 50 km is suggested.Key words. Atmospheric composition and structure (aerosols and particles; middle atmosphere-composition and chemistry; volcanic effects

Long Term Stratospheric Aerosol Lidar Measurements in Kyushu

Science.gov (United States)

Fujiwara, Motowo

1992-01-01

Lidar soundings of the stratospheric aerosols have been made since 1972 at Fukuoka, Kyushu Island of Japan. Volcanic clouds from eruptions of La Soufriere, Sierra Negra, St. Helens, Uluwan, Alaid, unknown volcano, and El Chichon were detected one after another in only three years from 1979 to 1982. In july 1991 strong scattering layers which were originated from the serious eruptions of Pinatubo in June and were almost comparable to the El Chichon clouds were detected. Volcanic clouds from pinatubo and other volcanos mentioned are examined and carefully compared to each other and to the wind and temperature which was measured by Fukuoka Meteorological Observatory almost at the same time as the lidar observation was made.

Ruby lidar observations and trajectory analysis of stratospheric aerosols injected by the volcanic eruptions of El Chichon

Science.gov (United States)

Uchino, O.; Tabata, T.; Akita, I.; Okada, Y.; Naito, K.

1985-01-01

Large amounts of aerosol particles and gases were injected into the lower stratosphere by the violet volcanic eruptions of El Chichon on March 28, and April 3 and 4, 1982. Observational results obtained by a ruby lidar at Tsukuba (36.1 deg N, 140.1 deg E) are shown, and some points of latitude dispersion processes of aerosols are discussed.

Stratospheric sulfate geoengineering impacts on global agriculture

Science.gov (United States)

Xia, L.; Robock, A.; Lawrence, P.; Lombardozzi, D.

2015-12-01

Stratospheric sulfate geoengineering has been proposed to reduce the impacts of anthropogenic climate change. If it is ever used, it would change agricultural production, and so is one of the future climate scenarios for the third phase of the Global Gridded Crop Model Intercomparison. As an example of those impacts, we use the Community Land Model (CLM-crop 4.5) to simulate how climate changes from the G4 geoengineering scenario from the Geoengineering Modeling Intercomparison Project. The G4 geoengineering scenario specifies, in combination with RCP4.5 forcing, starting in 2020 daily injections of a constant amount of SO2 at a rate of 5 Tg SO2 per year at one point on the Equator into the lower stratosphere. Eight climate modeling groups have completed G4 simulations. We use the crop model to simulate the impacts of climate change (temperature, precipitation, and solar radiation) on the global agriculture system for five crops - rice, maize, soybeans, cotton, and sugarcane. In general, without irrigation, compared with the reference run (RCP4.5), global production of cotton, rice and sugarcane would increase significantly due to the cooling effect. Maize and soybeans show different regional responses. In tropical regions, maize and soybean have a higher yield in G4 compared with RCP4.5, while in the temperate regions they have a lower yield under a geoengineered climate. Impacts on specific countries in terms of different crop production depend on their locations. For example, the United States and Argentina show soybean production reduction of about 15% under G4 compared to RCP4.5, while Brazil increases soybean production by about 10%.

Long-range transport of stratospheric aerosols in the Southern Hemisphere following the 2015 Calbuco eruption

Directory of Open Access Journals (Sweden)

N. Bègue

2017-12-01

Full Text Available After 43 years of inactivity, the Calbuco volcano, which is located in the southern part of Chile, erupted on 22 April 2015. The space–time evolutions (distribution and transport of its aerosol plume are investigated by combining satellite (CALIOP, IASI, OMPS, in situ aerosol counting (LOAC OPC and lidar observations, and the MIMOSA advection model. The Calbuco aerosol plume reached the Indian Ocean 1 week after the eruption. Over the Reunion Island site (21° S, 55.5° E, the aerosol signal was unambiguously enhanced in comparison with background conditions, with a volcanic aerosol layer extending from 18 to 21 km during the May–July period. All the data reveal an increase by a factor of  ∼  2 in the SAOD (stratospheric aerosol optical depth with respect to values observed before the eruption. The aerosol mass e-folding time is approximately 90 days, which is rather close to the value ( ∼  80 days reported for the Sarychev eruption. Microphysical measurements obtained before, during, and after the eruption reflecting the impact of the Calbuco eruption on the lower stratospheric aerosol content have been analyzed over the Reunion Island site. During the passage of the plume, the volcanic aerosol was characterized by an effective radius of 0.16 ± 0.02 µm with a unimodal size distribution for particles above 0.2 µm in diameter. Particle concentrations for sizes larger than 1 µm are too low to be properly detected by the LOAC OPC. The aerosol number concentration was  ∼  20 times higher that observed before and 1 year after the eruption. According to OMPS and lidar observations, a tendency toward conditions before the eruption was observed by April 2016. The volcanic aerosol plume is advected eastward in the Southern Hemisphere and its latitudinal extent is clearly bounded by the subtropical barrier and the polar vortex. The transient behavior of the aerosol layers observed above Reunion Island

On numerical simulation of the global distribution of sulfate aerosol produced by a large volcanic eruption

Energy Technology Data Exchange (ETDEWEB)

Pudykiewicz, J.A.; Dastoor, A.P. [Atmospheric Environment Service, Quebec (Canada)

1994-12-31

Volcanic eruptions play an important role in the global sulfur cycle of the Earth`s atmosphere and can significantly perturb the global atmospheric chemistry. The large amount of sulfate aerosol produced by the oxidation of SO{sub 2} injected into the atmosphere during volcanic eruptions also has a relatively big influence on the radiative equilibrium of the Earth`s climatic system. The submicron particles of the sulfate aerosol reflect solar radiation more effectively than they trap radiation in the infrared range. The effect of this is observed as cooling of the Earth`s surface. The modification of the global radiation budget following volcanic eruption can subsequently cause significant fluctuations of atmospheric variables on a subclimatic scale. The resulting perturbation of weather patterns has been observed and well documented since the eruptions of Mt. Krakatau and Mt. Tambora. The impact of the sulfate aerosol from volcanic eruptions on the radiative equilibrium of the Earth`s atmosphere was also confirmed by the studies done with Global Circulation Models designed to simulate climate. The objective of the present paper is to present a simple and effective method to estimate the global distribution of the sulfate aerosol produced as a consequence of volcanic eruptions. In this study we will present results of the simulation of global distribution of sulfate aerosol from the eruption of Mt Pinatubo.

Chemistry and Microphysics of Lower Stratospheric Aerosols Determined by Satellite Remote Sensing

Science.gov (United States)

Zasetsky, A. Y.; Khalizov, A.; Sloan, J.

2003-12-01

Observations of broadband Infrared satellites such as ILAS-II (Ministry of the Environment, Japan, launched 14 December 2002) and SciSat-1 (Canadian Space Agency, launched 12 August 2003) can provide details of the chemical composition and particle size of atmospheric aerosols by direct inversion without recourse to models. During the past decade, we have developed mathematical methods to achieve this inversion by working with FTIR observations of model atmospheric aerosols in cryogenic flowtubes. More recently, we have converted these to operational algorithms for use in the above missions. In this presentation, we will briefly outline these procedures and illustrate their capabilities using laboratory data. These laboratory results show that the chemical compositions, phases and sizes of ensembles of particles can be obtained simultaneously using these procedures. We will also report chemical and microphysical properties of lower stratospheric clouds and aerosols derived by applying these procedures to observations from space.

Aerosol vertical distribution characteristics over the Tibetan Plateau

International Nuclear Information System (INIS)

Deng, Z Q; Han, Y X; Zhao, Q; Li, J

2014-01-01

The Stratospheric Aerosol and Gas Experiment II (SAGE II) aerosol products are widely used in climatic characteristic studies and stratospheric aerosol pattern research. Some SAGE II products, e.g., temperature, aerosol surface area density, 1020 nm aerosol extinction coefficient and dust storm frequency, from ground-based observations were analysed from 1984 to 2005. This analysis explored the time and spatial variations of tropospheric and stratospheric aerosols on the Tibet Plateau. The stratospheric aerosol extinction coefficient increased more than two orders of magnitude because of a large volcanic eruption. However, the tropospheric aerosol extinction coefficient decreased over the same period. Removing the volcanic eruption effect, the correlation coefficient for stratospheric AOD (Aerosol Optical Depth) and tropospheric AOD was 0.197. Moreover, the correlation coefficient for stratospheric AOD and dust storm frequency was 0.315. The maximum stratospheric AOD was attained in January, the same month as the tropospheric AOD, when the Qaidam Basin was the centre of low tropospheric AOD and the large mountains coincided with high stratospheric AOD. The vertical structure generated by westerly jet adjustment and the high altitude of the underlying surface of the Tibetan Plateau were important factors affecting winter stratospheric aerosols

On the recent measurements of the electric parameters and aerosols in the lower stratosphere

International Nuclear Information System (INIS)

Morita, Yasuhiro; Ishikawa, Haruji; Takagi, Masumi

1979-01-01

In Sanriku (Iwate), Laramie (Wyoming) and Hilo (Hawaii), ionization intensity, electric conductivity, atmospheric ion density and aerosol were observed by balloon flights simultaneously from October, 1973, to September, 1976. On the basis of these results, the influences of aerosol and geomagnetic latitude upon the electric conductivity and atmospheric ion density were examined. From the simultaneous observation of electric conductivity and ion density, the average electrical mobility of ions and also its vertical distribution were obtained. In the simultaneous observation of electric conductivity and aerosol at altitude below about 10 km, the effect of aerosol on ion annihilation was detectable. In the stratosphere above this level, the electric conductivity (or the atmospheric ion density) is determined only by the ionization intensity, and there was little effect of aerosol. This was also confirmed by the comparative observations in Japan and U.S. with different geomagnetic latitudes. The average vertical mobility of ions increased with altitude at Laramie and decreased at Hilo. (J.P.N.)

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

Science.gov (United States)

Potter, Lauren E.

Sulfate aerosol in the atmosphere has substantial impacts on human health and environmental quality. Most notably, atmospheric sulfate has the potential to modify the earth's climate system through both direct and indirect radiative forcing mechanisms (Meehl et al., 2007). Emissions of sulfur dioxide, the primary precursor of sulfate aerosol, are now globally dominated by anthropogenic sources as a result of widespread fossil fuel combustion. Economic development in Asian countries since 1990 has contributed considerably to atmospheric sulfur loading, particularly China, which currently emits approximately 1/3 of global anthropogenic SO2 (Klimont et al., 2013). Observational and modeling studies have confirmed that anthropogenic pollutants from Asian sources can be transported long distances with important implications for future air quality and global climate change. Located in the remote Pacific Ocean (19.54°N, 155.58°W) at an elevation of 3.4 kilometers above sea level, Mauna Loa Observatory (MLO) is an ideal measurement site for ground-based, free tropospheric observations and is well situated to experience influence from springtime Asian outflow. This study makes use of a 14-year data set of aerosol ionic composition, obtained at MLO by the University of Hawaii at Manoa. Daily filter samples of total aerosol concentrations were made during nighttime downslope (free-tropospheric) transport conditions, from 1995 to 2008, and were analyzed for aerosol-phase concentrations of the following species: nitrate (NO3-), sulfate (SO42-), methanesulfonate (MSA), chloride (Cl-), oxalate, sodium (Na+), ammonium (NH 4+), potassium (K+), magnesium (Mg 2+), and calcium (Ca2+). An understanding of the factors controlling seasonal and interannual variations in aerosol speciation and concentrations at this site is complicated by the relatively short lifetimes of aerosols, compared with greenhouse gases which have also been sampled over long time periods at MLO. Aerosol filter

On the cryogenic removal of NOy from the Antarctic polar stratosphere

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S. Smyshlyaev

2003-06-01

Full Text Available We review current knowledge about the annual cycle of transport of nitrogen oxides to, and removal from, the polar stratosphere, with particular attention to Antarctica where the annual winter denitrifi cation process is both regular in occurrence and severe in effect. Evidence for a large downward fl ux of NOy from the mesosphere to the stratosphere, fi rst seen briefl y in the Limb Infrared Monitor of the Stratosphere (LIMS data from the Arctic winter of 1978-1979, has been found during the 1990s in both satellite and ground-based observations, though this still seems to be omitted from many atmospheric models. When incorporated in the Stony Brook- St. Petersburg two dimensional (2D transport and chemistry model, more realistic treatment of the NOy fl ux, along with sulfate transport from the mesosphere, sulfate aerosol formation where temperature is favorable, and the inclusion of a simple ion-cluster reaction, leads to good agreement with observed HNO3 formation in the mid-winter middle to upper stratosphere. To further emphasize the importance of large fl uxes of thermospheric and mesospheric NOy into the polar stratosphere, we have used observations, supplemented with model calculations, to defi ne new altitude dependent correlation curves between N2O and NOy. These are more suitable than those previously used in the literature to represent conditions within the Antarctic vortex region prior to and during denitrifi cation by Polar Stratospheric Cloud (PSC particles. Our NOy -N2O curves lead to a 40% increase in the average amount of NOy removed during the Antarctic winter with respect to estimates calculated using NOy-N2O curves from the Atmospheric Trace Molecule Spectroscopy (ATMOS/ATLAS-3 data set.

Sensitivity of the radiative forcing by stratospheric sulfur geoengineering to the amount and strategy of the SO2injection studied with the LMDZ-S3A model

Science.gov (United States)

Kleinschmitt, Christoph; Boucher, Olivier; Platt, Ulrich

2018-02-01

The enhancement of the stratospheric sulfate aerosol layer has been proposed as a method of geoengineering to abate global warming. Previous modelling studies found that stratospheric aerosol geoengineering (SAG) could effectively compensate for the warming by greenhouse gases on the global scale, but also that the achievable cooling effect per sulfur mass unit, i.e. the forcing efficiency, decreases with increasing injection rate. In this study we use the atmospheric general circulation model LMDZ with the sectional aerosol module S3A to determine how the forcing efficiency depends on the injected amount of SO2, the injection height, and the spatio-temporal pattern of injection. We find that the forcing efficiency may decrease more drastically for larger SO2 injections than previously estimated. As a result, the net instantaneous radiative forcing does not exceed the limit of -2 W m-2 for continuous equatorial SO2 injections and it decreases (in absolute value) for injection rates larger than 20 Tg S yr-1. In contrast to other studies, the net radiative forcing in our experiments is fairly constant with injection height (in a range 17 to 23 km) for a given amount of SO2 injected. Also, spreading the SO2 injections between 30° S and 30° N or injecting only seasonally from varying latitudes does not result in a significantly larger (i.e. more negative) radiative forcing. Other key characteristics of our simulations include a consequent stratospheric heating, caused by the absorption of solar and infrared radiation by the aerosol, and changes in stratospheric dynamics, with a collapse of the quasi-biennial oscillation at larger injection rates, which has impacts on the resulting spatial aerosol distribution, size, and optical properties. But it has to be noted that the complexity and uncertainty of stratospheric processes cause considerable disagreement among different modelling studies of stratospheric aerosol geoengineering. This may be addressed through detailed

Mt. St. Helens' aerosols: some tropospheric and stratospheric effects

International Nuclear Information System (INIS)

Michalsky, J.J.; Stokes, G.M.

1983-01-01

Aerosol optical depth measurements based on the attenuation of direct solar radiation before and after the six major explosive eruptions of Mt. St. Helens during 1980 are presented. These automated measurements are from a site 200 km mostly east and slightly north of the volcano. From the analysis it was concluded that in several cases the conversion of sulfur gases to sulfates proceeded much more rapidly (hours) than is usually found for tropospheric conditions. A possible explanation may be the greater availability of OH due to the presence of substantial water in the plume. The second major result of the analysis was that there was no evidence of a residual aerosol burden. Turbidity data taken between eruptions in 1980 were virtually identical in terms of magnitude and wavelength dependence to 1979 turbidity

Impacts of East Asian Sulfate Aerosols on Local and Remote Climate

Science.gov (United States)

Bartlett, R. E.; Bollasina, M. A.

2017-12-01

Anthropogenic aerosols exert significant climate forcing, which increases with emissions following trends of growing population and industry. Globally, aerosols cause a net cooling, counteracting greenhouse gas warming; however, regional impacts vary since emissions are spatially and temporally heterogeneous. While European and North American emissions have decreased in recent decades, Asian, particularly East Asian, emissions continued to rise into the 21st century. In addition to links between Asian anthropogenic aerosols and significant local climate impacts - for example, changes to the Asian monsoon system - studies have also shown influences on remote climate. Sulfate aerosols are particularly important for East Asia, remaining at constant levels higher than column burdens of other aerosol species. If a concerted effort - as laid out by government policies aiming to improve air quality - is made, the effects of anthropogenic aerosols (due to their short atmospheric lifetime) could be quickly reversed. Thus, it is vital to understand the climate impact aerosols have had up to now to aid in determining what will happen in the future. We use transient climate modelling experiments with the Community Earth System Model to investigate the impacts of East Asian sulfate aerosols in the present day compared to 1950 (i.e. before rapid industrialisation in this region), focusing on dynamical mechanisms leading to the occurrence of such impacts, and how their influence can spread to remote regions. We find, in addition to significant monsoon impacts, noticeable shifts in large-scale circulation features such as the ITCZ and the Pacific Walker cell. Through diabatic heating responses, changes to upper-level atmospheric dynamics are evident, leading to downstream effects on surface climate - for example, surface cooling over Europe. Understanding of these impacts is vital when considering how the good intentions of air quality improvement might inadvertently have

Tiny Ultraviolet Polarimeter for Earth Stratosphere from Space Investigation

Science.gov (United States)

Nevodovskyi, P. V.; Morozhenko, O. V.; Vidmachenko, A. P.; Ivakhiv, O.; Geraimchuk, M.; Zbrutskyi, O.

2015-09-01

One of the reasons for climate change (i.e., stratospheric ozone concentrations) is connected with the variations in optical thickness of aerosols in the upper sphere of the atmosphere (at altitudes over 30 km). Therefore, aerosol and gas components of the atmosphere are crucial in the study of the ultraviolet (UV) radiation passing upon the Earth. Moreover, a scrupulous study of aerosol components of the Earth atmosphere at an altitude of 30 km (i.e., stratospheric aerosol), such as the size of particles, the real part of refractive index, optical thickness and its horizontal structure, concentration of ozone or the upper border of the stratospheric ozone layer is an important task in the research of the Earth climate change. At present, the Main Astronomical Observatory of the National Academy of Sciences (NAS) of Ukraine, the National Technical University of Ukraine "KPI"and the Lviv Polytechnic National University are engaged in the development of methodologies for the study of stratospheric aerosol by means of ultraviolet polarimeter using a microsatellite. So fare, there has been created a sample of a tiny ultraviolet polarimeter (UVP) which is considered to be a basic model for carrying out space experiments regarding the impact of the changes in stratospheric aerosols on both global and local climate.

Estimated SAGE II ozone mixing ratios in early 1993 and comparisons with Stratospheric Photochemistry, Aerosols and Dynamic Expedition measurements

Science.gov (United States)

Yue, G. K.; Veiga, R. E.; Poole, L. R.; Zawodny, J. M.; Proffitt, M. H.

1994-01-01

An empirical time-series model for estimating ozone mixing ratios based on Stratospheric Aerosols and Gas Experiment II (SAGE II) monthly mean ozone data for the period October 1984 through June 1991 has been developed. The modeling results for ozone mixing ratios in the 10- to 30- km region in early months of 1993 are presented. In situ ozone profiles obtained by a dual-beam UV-absorption ozone photometer during the Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE) campaign, May 1-14, 1993, are compared with the model results. With the exception of two profiles at altitudes below 16 km, ozone mixing ratios derived by the model and measured by the ozone photometer are in relatively good agreement within their individual uncertainties. The identified discrepancies in the two profiles are discussed.

Observations of Stratospheric Gravity Waves During the WB57F Aerosol Mission and Modeling with Mesoscale Model 5

Science.gov (United States)

Mahoney, M.; Hicke, J.; Rosenlof, K.; Tuck, A.; Hovde, S.

2000-01-01

On April 11, 1998 WB57F aircraft flew northwest at lower stratospheric altitudes from Houston, Texas, over eastern Wyoming as part of the WB57F Aerosol Mission to sample a vortex filament forecast to pass over that region.

Observation of an unusual mid-stratospheric aerosol layer in the Arctic: possible sources and implications for polar vortex dynamics

Directory of Open Access Journals (Sweden)

M. Gerding

Full Text Available By the beginning of winter 2000/2001, a mysterious stratospheric aerosol layer had been detected by four different Arctic lidar stations. The aerosol layer was observed first on 16 November 2000, at an altitude of about 38 km near Søndre Strømfjord, Greenland (67° N, 51° W and on 19 November 2000, near Andenes, Norway (69°  N, 16°  E. Subsequently, in early December 2000, the aerosol layer was observed near Kiruna, Sweden (68°  N, 21°  E and Ny-Ålesund, Spitsbergen (79°  N, 12°  E. No mid-latitude lidar station observed the presence of aerosols in this altitude region. The layer persisted throughout the winter 2000/2001, at least up to 12 February 2001. In November 2000, the backscatter ratio at a wavelength of 532 nm was up to 1.1, with a FWHM of about 2.5 km. By early February 2001, the layer had sedimented from an altitude of 38 km to about 26 km. Measurements at several wavelengths by the ALOMAR and Koldewey lidars indicate the particle size was between 30 and 50 nm. Depolarisation measurements reveal that the particles in the layer are aspherical, hence solid. In the mid-stratosphere, the ambient atmospheric temperature was too high to support in situ formation or existence of cloud particles consisting of ice or an acid-water solution. Furthermore, in the year 2000 there was no volcanic eruption, which could have injected aerosols into the upper stratosphere. Therefore, other origins of the aerosol, such as meteoroid debris, condensed rocket fuel, or aerosols produced under the influence of charged solar particles, will be discussed in the paper. Trajectory calculations illustrate the path of the aerosol cloud within the polar vortex and are used to link the observations at the different lidar sites. From the descent rate of  the layer and particle sedimentation rates, the mean down-ward motion of air within the polar vortex was estimated to be about 124 m/d between 35 and 30 km, with higher values at the edge of the

Observation of an unusual mid-stratospheric aerosol layer in the Arctic: possible sources and implications for polar vortex dynamics

Directory of Open Access Journals (Sweden)

M. Gerding

2003-04-01

Full Text Available By the beginning of winter 2000/2001, a mysterious stratospheric aerosol layer had been detected by four different Arctic lidar stations. The aerosol layer was observed first on 16 November 2000, at an altitude of about 38 km near Søndre Strømfjord, Greenland (67° N, 51° W and on 19 November 2000, near Andenes, Norway (69°  N, 16°  E. Subsequently, in early December 2000, the aerosol layer was observed near Kiruna, Sweden (68°  N, 21°  E and Ny-Ålesund, Spitsbergen (79°  N, 12°  E. No mid-latitude lidar station observed the presence of aerosols in this altitude region. The layer persisted throughout the winter 2000/2001, at least up to 12 February 2001. In November 2000, the backscatter ratio at a wavelength of 532 nm was up to 1.1, with a FWHM of about 2.5 km. By early February 2001, the layer had sedimented from an altitude of 38 km to about 26 km. Measurements at several wavelengths by the ALOMAR and Koldewey lidars indicate the particle size was between 30 and 50 nm. Depolarisation measurements reveal that the particles in the layer are aspherical, hence solid. In the mid-stratosphere, the ambient atmospheric temperature was too high to support in situ formation or existence of cloud particles consisting of ice or an acid-water solution. Furthermore, in the year 2000 there was no volcanic eruption, which could have injected aerosols into the upper stratosphere. Therefore, other origins of the aerosol, such as meteoroid debris, condensed rocket fuel, or aerosols produced under the influence of charged solar particles, will be discussed in the paper. Trajectory calculations illustrate the path of the aerosol cloud within the polar vortex and are used to link the observations at the different lidar sites. From the descent rate of  the layer and particle sedimentation rates, the mean down-ward motion of air within the polar vortex was estimated to be about 124 m/d between 35 and 30 km, with higher values at the edge of the

Global Distribution of Solid Ammonium Sulfate Aerosols and their Climate Impact Acting as Ice Nuclei

Science.gov (United States)

Zhou, C.; Penner, J.

2017-12-01

Laboratory experiments show that liquid ammonium sulfate particles effloresce when RHw is below 34% to become solid and dissolve when RHw is above 79%. Solid ammonium sulfate aerosols can act as heterogeneous ice nuclei particles (INPs) to form ice particles in deposition mode when the relative humidity over ice is above 120%. In this study we used the coupled IMPACT/CAM5 model to track the efflorescence and deliquescence processes of ammonium sulfate. Results show that about 20% of the total simulated pure sulfate aerosol mass is in the solid state and is mainly distributed in the northern hemisphere (NH) from 50 hPa to 200 hPa. When these solid ammonium sulfate aerosols are allowed to act as ice nuclei particles, they act to increase the ice water path in the NH and reduce ice water path in the tropics. The addition of these particles leads to a positive net radiative effect at the TOA ranging from 0.5-0.9 W/m2 depending on the amounts of other ice nuclei particles (e.g., dust, soot) used in the ice nucleation process. The short-term climate feedback shows that the ITCZ shifts northwards and precipitation increases in the NH. There is also an average warming of 0.05-0.1 K near the surface (at 2 meter) in the NH which is most obvious in the Arctic region.

Long-term evolution of upper stratospheric ozone at selected stations of the Network for the Detection of Stratospheric Change (NDSC)

NARCIS (Netherlands)

Steinbrecht, W; Claude, H; Schönenborn, F; McDermid, I S; Leblanc, T; Godin, S; Song, T; Swart, D P J; Meijer, Y J; Bodeker, G E; Connor, B J; Kämpfer, N; Hocke, K; Calisesi, Y; Schneider, N; Noë, J de la; Parrish, A D; Boyd, I S; Brühl, C; Steil, B; Giorgetta, M A; Manzini, E; Thomason, L W; Zawodny, J M; McCormick, M P; Russell, J M; Bhartia, P K; Stolarski, R S; Hollandsworth-Frith, S M

2006-01-01

The long-term evolution of upper stratospheric ozone has been recorded by lidars and microwave radiometers within the ground-based Network for the Detection of Stratospheric Change (NDSC), and by the space-borne Solar Backscatter Ultra-Violet instruments (SBUV), Stratospheric Aerosol and Gas

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.

On recent (2008–2012 stratospheric aerosols observed by lidar over Japan

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O. Uchino

2012-12-01

Full Text Available An increase in stratospheric aerosols caused by the volcanic eruption of Mt. Nabro (13.37° N, 41.70° E on 12 June 2011 was detected by lidar at Tsukuba (36.05° N, 140.13° E and Saga (33.24° N, 130.29° E in Japan. The maximum backscattering ratios at a wavelength of 532 nm were 2.0 at 17.0 km on 10 July 2011 at Tsukuba and 3.6 at 18.2 km on 23 June 2011 at Saga. The maximum integrated backscattering coefficients (IBCs at 532 nm above the first tropopause height were 4.18×10⁻⁴ sr⁻¹ on 11 February 2012 at Tsukuba and 4.19×10⁻⁴ sr⁻¹ on 23 June 2011 at Saga, respectively.

A time series of lidar observational results at Tsukuba have also been reported from January 2008 through May 2012. Increases in stratospheric aerosols were observed after the volcanic eruptions of Mt. Kasatochi (52.18° N, 175.51° E in August 2008 and Mt. Sarychev Peak (48.09° N, 153.20° E in June 2009. The yearly averaged IBCs at Tsukuba were 2.54×10⁻⁴ sr⁻¹, 2.48×10⁻⁴ sr⁻¹, 2.45×10⁻⁴ sr⁻¹, and 2.20×10⁻⁴ sr⁻¹ for 2008, 2009, 2010, and 2011, respectively. These values were about twice the IBC background level (1.21×10⁻⁴ sr⁻¹ from 1997 to 2001 at Tsukuba. We briefly discuss the influence of the increased aerosols on climate and the implications for analysis of satellite data.

The Influence of Stratospheric Sulphate Aerosol Deployment on the Surface Air Temperature and the Risk of an Abrupt Global Warming

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Roland von Glasow

2010-12-01

Full Text Available We used the ‘Radiative-Convective Model of the Earth-atmosphere system’ (OGIM to investigate the cooling effects induced by sulphur injections into the stratosphere. The ensemble of numerical calculations was based on the A1B scenario from the IPCC Special Report on Emissions Scenarios (SRES. Several geoengineered scenarios were analysed, including the abrupt interruption of these injections in different scenarios and at different dates. We focused on the surface air temperature (SAT anomalies induced by stratospheric sulphate aerosol generated in order to compensate future warming. Results show that continuous deployment of sulphur into the stratosphere could induce a lasting decrease in SAT. Retaining a constant aerosol loading equivalent to 6 TgS would delay the expected global warming by 53 years. Keeping the SAT constant in a context of increasing greenhouse gases (GHGs means that the aerosol loading needs to be increased by 1.9% annually. This would offset the effect of increasing GHG under the A1B scenario. A major focus of this study was on the heating rates of SAT that would arise in different scenarios in case of an abrupt cessation of sulphur injections into the stratosphere. Our model results show that heating rates after geoengineering interruption would be 15–28 times higher than in a case without geoengineering, with likely important consequences for life on Earth. Larger initial sulphate loadings induced more intense warming rates when the geoengineering was stopped at the same time. This implies that, if sulphate loading was increased to maintain constant SAT in the light of increasing GHG concentrations, the later the geoengineering interruption was to occur, the higher the heating rates would be. Consequently, geoengineering techniques like this should only be regarded as last-resort measures and require intense further research should they ever become necessary.

Multi-model comparison of the volcanic sulfate deposition from the 1815 eruption of Mt. Tambora

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L. Marshall

2018-02-01

Full Text Available The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 year without a summer, and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic sulfate signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP, five state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora and volcanic (with Tambora sulfate deposition to polar regions and compare to ice core records. The models simulate overall similar patterns of background sulfate deposition, although there are differences in regional details and magnitude. However, the volcanic sulfate deposition varies considerably between the models with differences in timing, spatial pattern and magnitude. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kg km−2 and on Greenland from 31 to 194 kg km−2, as compared to the mean ice-core-derived estimates of roughly 50 kg km−2 for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results suggest that deriving relationships between sulfate deposited on ice sheets and atmospheric sulfate burdens from model simulations may be associated with greater uncertainties than previously thought.

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

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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.

Preliminary assessment of possible aerosol contamination effects on SAGE ozone trends in the lower stratosphere

Science.gov (United States)

Cunnold, Derek M.; Veiga, Robert E.

1991-01-01

An investigation of the validity of long-term ozone trends in the lower stratosphere derived from SAGE I and II measurements is described. At altitudes below approximately 20 km, it is important to separate the ozone and aerosol contributions to SAGE extinction at 600 nm. The correlation between SAGE II measurements of ozone and aerosols indicates that most of the variability in these parameters is associated with physically induced variations resulting from quasi-horizontal motions of air parcels. The SAGE ozone measurements are however found to be as much as 20 percent larger than coincident ozonesonde measurements between 15 and 20 km altitude. A sudden change in the difference at approximately 14.5 km altitude for which there is a change in the SAGE aerosol retrieval procedure suggests that SAGE ozone trends below 20 km altitude may be more sensitive to aerosol variations. Between 20 and 25 km altitude, however, both SAGE and the ozonesondes indicate a reduction in ozone of approximately 0.5 percent/year over the period 1979 to 1989 at midlatitudes of the Northern Hemisphere.

Sources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights

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Johan Friberg

2014-03-01

Full Text Available This study focuses on sulphurous and carbonaceous aerosol, the major constituents of particulate matter in the lowermost stratosphere (LMS, based on in situ measurements from 1999 to 2008. Aerosol particles in the size range of 0.08–2 µm were collected monthly during intercontinental flights with the CARIBIC passenger aircraft, presenting the first long-term study on carbonaceous aerosol in the LMS. Elemental concentrations were derived via subsequent laboratory-based ion beam analysis. The stoichiometry indicates that the sulphurous fraction is sulphate, while an O/C ratio of 0.2 indicates that the carbonaceous aerosol is organic. The concentration of the carbonaceous component corresponded on average to approximately 25% of that of the sulphurous, and could not be explained by forest fires or biomass burning, since the average mass ratio of Fe to K was 16 times higher than typical ratios in effluents from biomass burning. The data reveal increasing concentrations of particulate sulphur and carbon with a doubling of particulate sulphur from 1999 to 2008 in the northern hemisphere LMS. Periods of elevated concentrations of particulate sulphur in the LMS are linked to downward transport of aerosol from higher altitudes, using ozone as a tracer for stratospheric air. Tropical volcanic eruptions penetrating the tropical tropopause are identified as the likely cause of the particulate sulphur and carbon increase in the LMS, where entrainment of lower tropospheric air into volcanic jets and plumes could be the cause of the carbon increase.

Stratospheric Aerosol and Gas Experiment II measurements of the quasi-biennial oscillations in ozone and nitrogen dioxide

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Zawodny, Joseph M.; Mccormick, M. P.

1991-01-01

The first measurements ever to show a quasi-biennial oscillation (QBO) in NO2 have been made by the Stratospheric Aerosol and Gas Experiment II) (SAGE II) and are presented in this work along with observations of the well-known QBO in stratospheric ozone. The SAGE II instrument was launched aboard the Earth Radiation Budget satellite near the end of 1984. Measurements of ozone and nitrogen dioxide through early 1990 are analyzed for the presence of a quasi-biennial oscillation. The measurements show the global extent of both the O3 and NO2 QBO in the 25- to 40-km region of the stratosphere. The SAGE II QBO results for ozone compare favorably to theory and previous measurements. The QBO in NO2 is found to be consistent with the vertical and horizontal transport of NOy. Both species exhibit a QBO at extratropical latitudes consistent with strong meridional transport into the winter hemisphere.

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

International Nuclear Information System (INIS)

Liu Junfeng; Mauzerall, Denise L

2007-01-01

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 SO 2 emissions from a source region. We find that due to the non-linear nature of sulfate production, regions with low SO 2 emissions usually have large domestic IP, and vice versa. An exception is East Asia (EA), which has both high SO 2 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. SO 2 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 SO 2 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 SO 2 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

Evaluation of sulfate aerosol optical depths over the North Atlantic and comparison with satellite observations

International Nuclear Information System (INIS)

Berkowitz, C.M.; Ghan, S.J.; Benkovitz, C.M.; Wagener, R.; Nemesure, S.; Schwartz, S.E.

1993-11-01

It has been postulated that scattering of sunlight by aerosols can significantly reduce the amount of solar energy absorbed by the climate system. Aerosol measurement programs alone cannot provide all the information needed to evaluate the radiative forcing due to anthropogenic aerosols. Thus, comprehensive global-scale aerosol models, properly validated against surface-based and satellite measurements, are a fundamental tool for evaluating the impacts of aerosols on the planetary radiation balance. Analyzed meteorological fields from the European Centre for Medium-Range Weather Forecasts are used to drive a modified version of the PNL Global Chemistry Model, applied to the atmospheric sulfur cycle. The resulting sulfate fields are used to calculate aerosol optical depths, which in turn are compared to estimates of aerosol optical depth based on satellite observations

Investigating the influence of volcanic sulfate aerosol on cloud properties Along A-Train tracks

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Mace, G. G.

2017-12-01

Marine boundary layer (MBL) clouds are central actors in the climate system given their extensive coverage on the Earth's surface, their 1-way influence on the radiative balance (cooling), and their intimate coupling between air motions, anthropogenic and natural aerosol sources, and processes within the upper ocean mixed layer. Knowledge of how MBL shallow cumulus clouds respond to changes in aerosol is central to understanding how MBL clouds modulate the climate system. A frequent approach to investigating how sulfate aerosol influences MBL clouds has been to examine sulfate plumes extending downstream of active island volcanoes. This approach is challenging due to modification of the air motions in the plumes downstream of islands and due to the tendency of most researchers to examine only level-2 retrievals ignoring the actual data collected by sensors such as MODIS. Past studies have concluded that sulfate aerosols have large effects consistent with the 1st aerosol indirect effect (AIE). We reason that if such effects are as large as suggested in level-2 retrievals then evidence should also be present in the raw MODIS reflectance data as well as other data sources. In this paper we will build on our recently published work where we tested that hypothesis from data collected near Mount Kilauea during a 3-year period. Separating data into aerosol optical depth (A) quartiles, we found little support for a large 1st AIE response. We did find an unambiguous increase in sub 1km-scale cloud fraction with A. This increase in sub 1 km cloud fraction was entirely consistent with increased reflectance with increasing A that is used, via the level 2 retrievals, to argue for a large AIE response of MBL clouds. While the 1-km pixels became unambiguously brighter, that brightening was due to increased sub 1 km cloud fraction and not necessarily due to changes in pixel-level cloud microphysics. We also found that MBL cloud top heights increase as do surface wind speeds as

Aerosol pH buffering in the southeastern US: Fine particles remain highly acidic despite large reductions in sulfate

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Weber, R. J.; Guo, H.; Russell, A. G.; Nenes, A.

2015-12-01

pH is a critical aerosol property that impacts many atmospheric processes, including biogenic secondary organic aerosol formation, gas-particle phase partitioning, and mineral dust or redox metal mobilization. Particle pH has also been linked to adverse health effects. Using a comprehensive data set from the Southern Oxidant and Aerosol Study (SOAS) as the basis for thermodynamic modeling, we have shown that particles are currently highly acidic in the southeastern US, with pH between 0 and 2. Sulfate and ammonium are the main acid-base components that determine particle pH in this region, however they have different sources and their concentrations are changing. Over 15 years of network data show that sulfur dioxide emission reductions have resulted in a roughly 70 percent decrease in sulfate, whereas ammonia emissions, mainly link to agricultural activities, have been largely steady, as have gas phase ammonia concentrations. This has led to the view that particles are becoming more neutralized. However, sensitivity analysis, based on thermodynamic modeling, to changing sulfate concentrations indicates that particles have remained highly acidic over the past decade, despite the large reductions in sulfate. Furthermore, anticipated continued reductions of sulfate and relatively constant ammonia emissions into the future will not significantly change particle pH until sulfate drops to clean continental background levels. The result reshapes our expectation of future particle pH and implies that atmospheric processes and adverse health effects linked to particle acidity will remain unchanged for some time into the future.

Black Carbon and Sulfate Aerosols in the Arctic: Long-term Trends, Radiative Impacts, and Source Attributions

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Wang, H.; Zhang, R.; Yang, Y.; Smith, S.; Rasch, P. J.

2017-12-01

The Arctic has warmed dramatically in recent decades. As one of the important short-lived climate forcers, aerosols affect the Arctic radiative budget directly by interfering radiation and indirectly by modifying clouds. Light-absorbing particles (e.g., black carbon) in snow/ice can reduce the surface albedo. The direct radiative impact of aerosols on the Arctic climate can be either warming or cooling, depending on their composition and location, which can further alter the poleward heat transport. Anthropogenic emissions, especially, BC and SO2, have changed drastically in low/mid-latitude source regions in the past few decades. Arctic surface observations at some locations show that BC and sulfate aerosols had a decreasing trend in the recent decades. In order to understand the impact of long-term emission changes on aerosols and their radiative effects, we use the Community Earth System Model (CESM) equipped with an explicit BC and sulfur source-tagging technique to quantify the source-receptor relationships and decadal trends of Arctic sulfate and BC and to identify variations in their atmospheric transport pathways from lower latitudes. The simulation was conducted for 36 years (1979-2014) with prescribed sea surface temperatures and sea ice concentrations. To minimize potential biases in modeled large-scale circulations, wind fields in the simulation are nudged toward an atmospheric reanalysis dataset, while atmospheric constituents including water vapor, clouds, and aerosols are allowed to evolve according to the model physics. Both anthropogenic and open fire emissions came from the newly released CMIP6 datasets, which show strong regional trends in BC and SO2 emissions during the simulation time period. Results show that emissions from East Asia and South Asia together have the largest contributions to Arctic sulfate and BC concentrations in the upper troposphere, which have an increasing trend. The strong decrease in emissions from Europe, Russia and

Investigations of the Background Stratospheric Aerosol Using Multicolor Wide-Angle Measurements of the Twilight Glow Background

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Ugolnikov, O. S.; Maslov, I. A.

2018-03-01

The first results of multiwave measurements of twilight background and the all-sky camera with a color (RGB) CCD matrix conducted in the spring and summer of 2016 in Central Russia (55.2° N, 37.5° E) have been discussed. The observations reveal the effect of aerosol scattering at heights of up to 35 km, which is substantially enhanced in the long-wave part of the spectrum (R band with an effective wavelength of 624 nm). An analysis of the behavior of the sky color during light period of twilight with allowance for the absorption by ozone in the Chappuis bands make it possible to restore the angular dependences of the intensity of the aerosol scattering of the light. This is used to determine the parameters of the lognormal distribution of aerosol particles over their sizes with a mean radius of 0.08 μm and a width of 1.5-1.6 for the stratospheric height interval.

Earth Science With the Stratospheric Aerosol and Gas Experiment III (SAGE III) on the International Space Station

Science.gov (United States)

Zawodny, Joe; Vernier, Jean-Paul; Thomason, Larry; Roell, Marilee; Pitts, Mike; Moore, Randy; Hill, Charles; Flittner, David; Damadeo, Rob; Cisewski, Mike

2015-01-01

The Stratospheric Aerosol and Gas Experiment (SAGE) III is the fourth generation of solar occultation instruments operated by NASA, the first coming under a different acronym, to investigate the Earth's upper atmosphere. Three flight-ready SAGE III instruments were built by Ball Aerospace in the late 1990s, with one launched aboard the former Russian Aviation and Space Agency (now known as Roskosmos) Meteor-3M platform on 10 December 2001 (continuing until the platform lost power in 2006). Another of the original instruments was manifested for the ISS in the 2004 time frame, but was delayed because of budgetary considerations. Fortunately, that SAGE III/ISS mission was restarted in 2009 with a major focus upon filling an anticipated gap in ozone and aerosol observation in the second half of this decade. Here we discuss the mission architecture, its implementation, and data that will be produced by SAGE III/ISS, including their expected accuracy and coverage. The 52-degree inclined orbit of the ISS is well-suited for solar occultation and provides near-global observations on a monthly basis with excellent coverage of low and mid-latitudes. This is similar to that of the SAGE II mission (1985-2005), whose data set has served the international atmospheric science community as a standard for stratospheric ozone and aerosol measurements. The nominal science products include vertical profiles of trace gases, such as ozone, nitrogen dioxide and water vapor, along with multi-wavelength aerosol extinction. Though in the visible portion of the spectrum the brightness of the Sun is one million times that of the full Moon, the SAGE III instrument is designed to cover this large dynamic range and also perform lunar occultations on a routine basis to augment the solar products. The standard lunar products were demonstrated during the SAGE III/M3M mission and include ozone, nitrogen dioxide & nitrogen trioxide. The operational flexibility of the SAGE III spectrometer accomplishes

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

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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

Could aerosol emissions be used for regional heat wave mitigation?

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D. N. Bernstein

2013-07-01

Full Text Available Geoengineering applications by injection of sulfate aerosols into the stratosphere are under consideration as a measure of last resort to counter global warming. Here a potential regional-scale application to offset the impacts of heat waves is critically examined. Using the Weather Research and Forecasting model with fully coupled chemistry (WRF-Chem, the effect of regional-scale sulfate aerosol emission over California in each of two days of the July 2006 heat wave is used to quantify potential reductions in surface temperature as a function of emission rates in a layer at 12 km altitude. Local meteorological factors yield geographical differences in surface air temperature sensitivity. For emission rates of approximately 30 μg m−2 s−1 of sulfate aerosols (with standard WRF-Chem size distribution over the region, temperature decreases of around 7 °C result during the middle part of the day over the Central Valley, one of the areas hardest hit by the heat wave. Regions more ventilated with oceanic air such as Los Angeles have slightly smaller reductions. The length of the hottest part of the day is also reduced. Advection effects on the aerosol cloud must be more carefully forecast for smaller injection regions. Verification of the impacts could be done via measurements of differences in reflected and surface downward shortwave. Such regional geoengineering applications with specific near-term target effects but smaller cost and side effects could potentially provide a means of testing larger scale applications. However, design considerations for regional applications, such as a preference for injection at a level of relatively low wind speed, differ from those for global applications. The size of the required injections and the necessity of injection close to the target region raise substantial concerns. The evaluation of this regional-scale application is thus consistent with global model evaluations, emphasizing that mitigation via

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Science.gov (United States)

Stevens, R. G.; Pierce, J. R.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.

2012-01-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

The Climate Response to Stratospheric Aerosol Geoengineering Can Be Tailored Using Multiple Injection Locations

Energy Technology Data Exchange (ETDEWEB)

MacMartin, Douglas G. [Mechanical and Aerospace Engineering, Cornell University, Ithaca NY USA; Department of Computing and Mathematical Sciences, California Institute of Technology, Pasadena CA USA; Kravitz, Ben [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Tilmes, Simone [Atmospheric Chemistry, Observations, and Modeling Laboratory, National Center for Atmospheric Research, Boulder CO USA; Climate and Global Dynamics Laboratory, National Center for Atmospheric Research, Boulder CO USA; Richter, Jadwiga H. [Climate and Global Dynamics Laboratory, National Center for Atmospheric Research, Boulder CO USA; Mills, Michael J. [Atmospheric Chemistry, Observations, and Modeling Laboratory, National Center for Atmospheric Research, Boulder CO USA; Lamarque, Jean-Francois [Atmospheric Chemistry, Observations, and Modeling Laboratory, National Center for Atmospheric Research, Boulder CO USA; Climate and Global Dynamics Laboratory, National Center for Atmospheric Research, Boulder CO USA; Tribbia, Joseph J. [Climate and Global Dynamics Laboratory, National Center for Atmospheric Research, Boulder CO USA; Vitt, Francis [Atmospheric Chemistry, Observations, and Modeling Laboratory, National Center for Atmospheric Research, Boulder CO USA

2017-12-07

The climate response to geoengineering with stratospheric aerosols has the potential to be designed to achieve some chosen objectives. By injecting different amounts of SO2 at multiple different latitudes, the spatial pattern of aerosol optical depth (AOD) can be partially controlled. We use simulations from the fully-coupled whole-atmosphere chemistry-climate model CESM1(WACCM), to demonstrate that three spatial degrees of freedom of AOD can be achieved by appropriately combining injection at different locations: an approximately spatially-uniform AOD distribution, the relative difference in AOD between Northern and Southern hemispheres, and the relative AOD in high versus low latitudes. For forcing levels that yield 1–2°C cooling, the AOD and surface temperature response are sufficiently linear in this model so that many climate effects can be predicted from single-latitude injection simulations. Optimized injection at multiple locations is predicted to improve compensation of CO2-forced climate change, relative to a case using only equatorial aerosol injection. The additional degrees of freedom can be used, for example, to balance interhemispheric temperature differences and the equator to pole temperature difference in addition to the global mean temperature; this is projected in this model to reduce the mean-square error in temperature compensation by 30%.

The observation of nitric acid-containing particles in the tropical lower stratosphere

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P. J. Popp

2006-01-01

Full Text Available Airborne in situ measurements over the eastern Pacific Ocean in January 2004 have revealed a new category of nitric acid (HNO3-containing particles in the tropical lower stratosphere. These particles are most likely composed of nitric acid trihydrate (NAT. They were intermittently observed in a narrow layer above the tropopause (18±0.1 km and over a broad geographic extent (>1100 km. In contrast to the background liquid sulfate aerosol, these particles are solid, much larger (1.7-4.7 µm vs. 0.1µm in diameter, and significantly less abundant (-4 cm-3 vs. 10 cm-3. Microphysical trajectory models suggest that the NAT particles grow over a 6-14 day period in supersaturated air that remains close to the tropical tropopause and might be a common feature in the tropics. The small number density of these particles implies a highly selective or slow nucleation process. Understanding the formation of solid NAT particles in the tropics could improve our understanding of stratospheric nucleation processes and, therefore, dehydration and denitrification.

On particles in the Arctic stratosphere

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T. S. Jørgensen

2003-06-01

Full Text Available Soon after the discovery of the Antarctic ozone hole it became clear that particles in the polar stratosphere had an infl uence on the destruction of the ozone layer. Two major types of particles, sulphate aerosols and Polar Stratospheric Clouds (PSCs, provide the surfaces where fast heterogeneous chemical reactions convert inactive halogen reservoir species into potentially ozone-destroying radicals. Lidar measurements have been used to classify the PSCs. Following the Mt. Pinatubo eruption in June 1991 it was found that the Arctic stratosphere was loaded with aerosols, and that aerosols observed with lidar and ozone observed with ozone sondes displayed a layered structure, and that the aerosol and ozone contents in the layers frequently appeared to be negatively correlated. The layered structure was probably due to modulation induced by the dynamics at the edge of the polar vortex. Lidar observations of the Mt. Pinatubo aerosols were in several cases accompanied by balloon-borne backscatter soundings, whereby backscatter measurements in three different wavelengths made it possible to obtain information about the particle sizes. An investigation of the infl uence of synoptic temperature histories on the physical properties of PSC particles has shown that most of the liquid type 1b particles were observed in the process of an ongoing, relatively fast, and continuous cooling from temperatures clearly above the nitric acid trihydrate condensation temperature (TNAT. On the other hand, it appeared that a relatively long period, with a duration of at least 1-2 days, at temperatures below TNAT provide the conditions which may lead to the production of solid type 1a PSCs.

A Chronology of Annual-Mean Effective Radii of Stratospheric Aerosols from Volcanic Eruptions During the Twentieth Century as Derived From Ground-based Spectral Extinction Measurements

Science.gov (United States)

Strothers, Richard B.; Hansen, James E. (Technical Monitor)

2001-01-01

Stratospheric extinction can be derived from ground-based spectral photometric observations of the Sun and other stars (as well as from satellite and aircraft measurements, available since 1979), and is found to increase after large volcanic eruptions. This increased extinction shows a characteristic wavelength dependence that gives information about the chemical composition and the effective (or area weighted mean) radius of the particles responsible for it. Known to be tiny aerosols constituted of sulfuric acid in a water solution, the stratospheric particles at midlatitudes exhibit a remarkable uniformity of their column-averaged effective radii r(sub eff) in the first few months after the eruption. Considering the seven largest eruptions of the twentieth century, r(sub eff) at this phase of peak aerosol abundance is approx. 0.3 micrometers in all cases. A year later, r(sub eff) either has remained about the same size (almost certainly in the case of the Katmai eruption of 1912) or has increased to approx. 0.5 micrometers (definitely so for the Pinatubo eruption of 1991). The reasons for this divergence in aerosol growth are unknown.

The fate of atmospheric phosgene and the stratospheric chlorine loadings of its parent compounds: CCl4, C2Cl4, C2HCL3, CH3CCl3, and CHCl3

Science.gov (United States)

Kindler, T. P.; Chameides, W. L.; Wine, P. H.; Cunnold, D. M.; Alyea, F. N.; Franklin, J. A.

1995-01-01

of reaction of phosgene with sulfate aerosols. However, on the basis of the observed vertical distribution of COCl2, we estimate that the reaction of COCl2 with sulfate aerosol most likely has a gamma less than 5 x 10(exp -5) and, as a result, has a negligible impact on the stratospheric chlorine loadings of the phosgene parent compounds.

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Directory of Open Access Journals (Sweden)

R. G. Stevens

2012-01-01

Full Text Available New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO₂ with condensation of H₂SO₄ onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM, a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM. The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H₂SO₄ condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NO_x since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

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

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

Science.gov (United States)

Wurl, D.; Grainger, R. G.; McDonald, A. J.; Deshler, T.

2010-05-01

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 distributions naturally

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

Forcing of stratospheric chemistry and dynamics during the Dalton Minimum

Science.gov (United States)

Anet, J. G.; Muthers, S.; Rozanov, E.; Raible, C. C.; Peter, T.; Stenke, A.; Shapiro, A. I.; Beer, J.; Steinhilber, F.; Brönnimann, S.; Arfeuille, F.; Brugnara, Y.; Schmutz, W.

2013-11-01

The response of atmospheric chemistry and dynamics to volcanic eruptions and to a decrease in solar activity during the Dalton Minimum is investigated with the fully coupled atmosphere-ocean chemistry general circulation model SOCOL-MPIOM (modeling tools for studies of SOlar Climate Ozone Links-Max Planck Institute Ocean Model) covering the time period 1780 to 1840 AD. We carried out several sensitivity ensemble experiments to separate the effects of (i) reduced solar ultra-violet (UV) irradiance, (ii) reduced solar visible and near infrared irradiance, (iii) enhanced galactic cosmic ray intensity as well as less intensive solar energetic proton events and auroral electron precipitation, and (iv) volcanic aerosols. The introduced changes of UV irradiance and volcanic aerosols significantly influence stratospheric dynamics in the early 19th century, whereas changes in the visible part of the spectrum and energetic particles have smaller effects. A reduction of UV irradiance by 15%, which represents the presently discussed highest estimate of UV irradiance change caused by solar activity changes, causes global ozone decrease below the stratopause reaching as much as 8% in the midlatitudes at 5 hPa and a significant stratospheric cooling of up to 2 °C in the mid-stratosphere and to 6 °C in the lower mesosphere. Changes in energetic particle precipitation lead only to minor changes in the yearly averaged temperature fields in the stratosphere. Volcanic aerosols heat the tropical lower stratosphere, allowing more water vapour to enter the tropical stratosphere, which, via HOx reactions, decreases upper stratospheric and mesospheric ozone by roughly 4%. Conversely, heterogeneous chemistry on aerosols reduces stratospheric NOx, leading to a 12% ozone increase in the tropics, whereas a decrease in ozone of up to 5% is found over Antarctica in boreal winter. The linear superposition of the different contributions is not equivalent to the response obtained in a simulation

A unified approach to infrared aerosol remote sensing and type specification

Directory of Open Access Journals (Sweden)

L. Clarisse

2013-02-01

Full Text Available Atmospheric aerosols impact air quality and global climate. Space based measurements are the best way to observe their spatial and temporal distributions, and can also be used to gain better understanding of their chemical, physical and optical properties. Aerosol composition is the key parameter affecting the refractive index, which determines how much radiation is scattered and absorbed. Composition of aerosols is unfortunately not measured by state of the art satellite remote sounders. Here we use high resolution infrared measurements for aerosol type differentiation, exploiting, in that part of spectrum, the dependency of their refractive index on wavelength. We review existing detection methods and present a unified detection method based on linear discrimination analysis. We demonstrate this method on measurements of the Infrared Atmospheric Sounding Interferometer (IASI and five different aerosol types, namely volcanic ash, windblown sand, sulfuric acid droplets, ammonium sulfate and smoke particles. We compare these with traditional MODIS AOD measurements. The detection of the last three types is unprecedented in the infrared in nadir mode, but is very promising, especially for sulfuric acid droplets which are detected in the lower troposphere and up to 6 months after injection in the upper troposphere/lower stratosphere.

Organic aerosols

International Nuclear Information System (INIS)

Penner, J.E.

1994-01-01

Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN

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

Directory of Open Access Journals (Sweden)

J.-E. Tesdal

2016-09-01

Full Text Available 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.

Visualizing Volcanic Clouds in the Atmosphere and Their Impact on Air Traffic.

Science.gov (United States)

Gunther, Tobias; Schulze, Maik; Friederici, Anke; Theisel, Holger

2016-01-01

Volcanic eruptions are not only hazardous in the direct vicinity of a volcano, but they also affect the climate and air travel for great distances. This article sheds light on the Grímsvötn, Puyehue-Cordón Caulle, and Nabro eruptions in 2011. The authors study the agreement of the complementary satellite data, reconstruct sulfate aerosol and volcanic ash clouds, visualize endangered flight routes, minimize occlusion in particle trajectory visualizations, and focus on the main pathways of Nabro's sulfate aerosol into the stratosphere. The results here were developed for the 2014 IEEE Scientific Visualization Contest, which centers around the fusion of multiple satellite data modalities to reconstruct and assess the movement of volcanic ash and sulfate aerosol emissions. Using data from three volcanic eruptions that occurred in the span of approximately three weeks, the authors study the agreement of the complementary satellite data, reconstruct sulfate aerosol and volcanic ash clouds, visualize endangered flight routes, minimize occlusion in particle trajectory visualizations, and focus on the main pathways of sulfate aerosol into the stratosphere. This video provides animations of the reconstructed ash clouds. https://youtu.be/D9DvJ5AvZAs.

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)

H2SO4-HNO3-H2O ternary system in the stratosphere

Science.gov (United States)

Kiang, C. S.; Hamill, P.

1974-01-01

Estimation of the equilibrium vapor pressure over the ternary system H2SO4-HNO3-H2O to study the possibility of stratospheric aerosol formation involving HNO3. It is shown that the vapor pressures for the ternary system H2SO4-HNO3-H2O with weight composition around 70-80% H2SO4, 10-20% HNO3, 10-20% H2O at -50 C are below the order of 10 to the minus 8th mm Hg. It is concluded that there exists more than sufficient nitric acid and water vapor in the stratosphere to participate in ternary system aerosol formation at -50 C. Therefore, HNO3 should be present in stratospheric aerosols, provided that H2SO4 is also present.

Simulated responses of terrestrial aridity to black carbon and sulfate aerosols

Science.gov (United States)

Lin, L.; Gettelman, A.; Xu, Y.; Fu, Q.

2016-01-01

Aridity index (AI), defined as the ratio of precipitation to potential evapotranspiration (PET), is a measure of the dryness of terrestrial climate. Global climate models generally project future decreases of AI (drying) associated with global warming scenarios driven by increasing greenhouse gas and declining aerosols. Given their different effects in the climate system, scattering and absorbing aerosols may affect AI differently. Here we explore the terrestrial aridity responses to anthropogenic black carbon (BC) and sulfate (SO4) aerosols with Community Earth System Model simulations. Positive BC radiative forcing decreases precipitation averaged over global land at a rate of 0.9%/°C of global mean surface temperature increase (moderate drying), while BC radiative forcing increases PET by 1.0%/°C (also drying). BC leads to a global decrease of 1.9%/°C in AI (drying). SO4 forcing is negative and causes precipitation a decrease at a rate of 6.7%/°C cooling (strong drying). PET also decreases in response to SO4 aerosol cooling by 6.3%/°C cooling (contributing to moistening). Thus, SO4 cooling leads to a small decrease in AI (drying) by 0.4%/°C cooling. Despite the opposite effects on global mean temperature, BC and SO4 both contribute to the twentieth century drying (AI decrease). Sensitivity test indicates that surface temperature and surface available energy changes dominate BC- and SO4-induced PET changes.

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)

SPICE Work Package 3: Modelling the Effects of Stratospheric Aerosol Geoengineering

Science.gov (United States)

Driscoll, Simon

2015-04-01

This talk presents the results of the SPICE Work Package 3. There is an obvious need for methods to verify the accuracy of geoengineering given no observations of a geoengineering programme. Accordingly, model ability in reproducing the observed dynamical response to volcanic eruptions is discussed using analysis of CMIP5 data and different configurations of the HadGEM2 model. With the HadGEM2-L60 model shown to be substantially better in reproducing the observed dynamical response to volcanic eruptions, simulations of GeoMIP's G4 scenario are performed. Simulated impacts of geoengineering are described, and asymmetries between the immediate onset and immediate cessation ('termination') of geoengineering are analysed. Whilst a rapid large increase in stratospheric sulphate aerosols (such as from volcanic eruptions) can cause substantial damage, most volcanic eruptions in general are not catastrophic. One may therefore suspect that an 'equal but opposite' change in radiative forcing from termination may therefore not be catastrophic, if the climatic response is simulated to be symmetric. HadGEM2 simulations reveal a substantially more rapid change in variables such as near-surface temperature and precipitation following termination than the onset, indicating that termination may be substantially more damaging and even catastrophic. Some suggestions for hemispherically asymmetric geoengineering have been proposed as a way to reduce Northern Hemisphere sea ice, for example, with lesser impacts on the rest of the climate. However, HadGEM2 simulations are performed and observations analysed following volcanic eruptions. Both indicate substantial averse consequences from hemispherically asymmetric loading of stratospheric loading on precipitation in the Sahelian region - a vulnerable region where drought has caused hundreds of thousands of deaths and created millions of refugees in the past.

Stratospheric controlled perturbation experiment (SCoPEx): overview, status, and results from related laboratory experiments

Science.gov (United States)

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

2017-12-01

Stratospheric Controlled Perturbation Experiment (SCoPEx), is a scientific experiment to advance understanding of stratospheric aerosols. It aims to make quantitative measurements of aerosol microphysics and atmospheric chemistry to improve large-scale models used to assess the risks and benefits of solar geoengineering. A perturbative experiment requires: (a) means to create a well-mixed, small perturbed volume, and (b) observation of time evolution of chemistry and aerosols in the volume. SCoPEx will used a propelled balloon gondola containing all instruments and drive system. The propeller wake forms a well-mixed volume (roughly 1 km long and 100 meters in diameter) that serves as an experimental `beaker' into which aerosols (e.g., budget, etc; (d) results from CFD simulation of propeller wake and simulation of chemistry and aerosol microphysics; and finally (e) proposed concept of operations and schedule. We will also provide an overview of the plans for governance including management of health safety and environmental risks, transparency, public engagement, and larger questions about governance of solar geoengineering experiments. Finally, we will briefly present results of laboratory experiments of the interaction of chemical such as ClONO2 and HCl on particle surfaces relevant for stratospheric solar geoengineering.

Lower stratospheric observations from aircraft and satellite during the 2015/2016 El Nino

Science.gov (United States)

Rosenlof, K. H.; Avery, M. A.; Davis, S. M.; Gao, R. S.; Thornberry, T. D.

2016-12-01

Winter 2015/2016 experienced a strong El Nino that was heavily observed by aircraft, radiosonde and satellite platforms. During the National Oceanographic and Atmospheric Administration's (NOAA) Sensing Hazards with Operational Unmanned Technology (SHOUT)/El Nino Rapid Response (ENRR) flights of the NASA Global Hawk, in situ ozone measurements were made in the lower stratosphere over the Pacific. These will be contrasted with ozone measurements taken during La Nina and ENSO neutral conditions during past Global Hawk aircraft campaigns. Additionally, lower stratospheric water vapor and ozone measurements from the Microwave Limb Sounder satellite instrument and stratospheric ice measurements above the tropopause from the Cloud-Aerosol Aerosol Lidar with Orthogonal Polarization (CALIOP) will be presented. Our aircraft ozone measurements are higher for the El Nino flights than during other missions previously sampled, while zonally averaged lower stratospheric water vapor and central Pacific ice path above the tropopause reached record highs. Implications and possible reasons for these anomalous observations will be discussed. Winter 2015/2016 experienced a strong El Nino that was heavily observed by aircraft, radiosonde and satellite platforms. During the National Oceanographic and Atmospheric Administration's (NOAA) Sensing Hazards with Operational Unmanned Technology (SHOUT)/El Nino Rapid Response (ENRR) flights of the NASA Global Hawk, in situ ozone measurements were made in the upper troposphere and lower stratosphere (UTLS) over the Pacific. These will be contrasted with ozone measurements made during La Nina and ENSO neutral conditions during past Global Hawk aircraft campaigns. Additionally, UTLS water vapor and ozone measurements from the Microwave Limb Sounder (MLS) satellite instrument and stratospheric ice measurements above the tropopause from the Cloud-Aerosol Aerosol Lidar with Orthogonal Polarization (CALIOP) will be presented. Our aircraft ozone

New stratospheric UV/visible radiance measurements

Directory of Open Access Journals (Sweden)

F. J. Marceau

1994-01-01

Full Text Available A stratospheric balloon was launched on 12 October 1986 from the "CNES" base at Aire sur l'Adour (France to record twilight radiance in the stratosphere. The near-UV and visible radiances were continuously monitored by a photometer during sunrise. Some observations are presented for different viewing azimuthal planes and viewing elevation angles. They show the influence of aerosols layers and clouds which can be also seen on related photographs. The results as a whole may be used for testing some radiative models, especially for twilight conditions.

Impact of major volcanic eruptions on stratospheric water vapour

Directory of Open Access Journals (Sweden)

M. Löffler

2016-05-01

Full Text Available 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.

SAM II aerosol profile measurements, Poker Flat, Alaska; July 16-19, 1979

Science.gov (United States)

Mccormick, M. P.; Chu, W. P.; Mcmaster, L. R.; Grams, G. W.; Herman, B. M.; Pepin, T. J.; Russell, P. B.; Swissler, T. J.

1981-01-01

SAM II satellite measurements during the July 1979 Poker Flat mission, yielded an aerosol extinction coefficient of 0.0004/km at 1.0 micron wavelength, in the region of the stratospheric aerosol mixing ratio peak (12-16 km). The stratospheric aerosol optical depth for these data, calculated from the tropopause through 30 km, is approximately 0.001. These results are consistent with the average 1979 summertime values found throughout the Arctic.

Elemental concentrations in tropospheric and lower stratospheric air in a Northeastern region of Poland

Science.gov (United States)

Braziewicz, Janusz; Kownacka, Ludwika; Majewska, Urszula; Korman, Andrzej

Element concentrations of K, Ca, Ti, Cr, Fe, Ni, Cu, Zn, Se, Br, Sr and Pb as well as the activity of natural radionuclides 210Pb and 226Ra in air were measured. The aerosol samples were collected during tropospheric and stratospheric aircraft flights over the Northeastern region of Poland, which is mostly an agricultural and wooded area. The air volumes were filtered using Petrianov filters at 1, 3, 6, 9, 12 and 15 km above the ground level by special equipment attached to a jet plane. Aircraft flights were provided from September 1997 to August 1998 in 5 separate sampling runs. The long sampling distances served as a good representation of mean aerosol composition and distribution. Concentrations of the same elements were also measured using stationary equipment near the ground level at the outskirts of Warsaw. The vertical profiles of element concentration were obtained and the elemental compositions for the tropospheric and stratospheric aerosols were compared with those from the near-ground level. Contribution of K, Ca, Ti and Fe, which are the main components of soil, in total mass of all detected ones was estimated. Relative concentrations of all measured elements, which show any differences in the composition of the aerosol were calculated. The results obtained confirm the fact that the stratospheric reservoir is observed in the bottom stratosphere. The XRF method based on molybdenum X-ray tube was used as an analytical tool in the determination of aerosols trace elements. The altitude distributions of radioactivity of 226Ra and 210Pb were determined using radiochemical methods.

Mount St. Helens aerosol evolution

Energy Technology Data Exchange (ETDEWEB)

Oberbeck, V.R.; Farlow, N.H.

1982-08-01

Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mount St. Helens. Analysis of samples shows that aerosol volume increased for 6 months due to gas-to-particle conversion and then decreased to background levels in the following 6 months.

Mount St. Helens aerosol evolution

Energy Technology Data Exchange (ETDEWEB)

Oberbeck, V.R.; Farlow, N.H.; Fong, W.; Snetsinger, K.G.; Ferry, G.V.; Hayes, D.M.

1982-09-01

Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mt. St. Helens. Analysis of samples show that aerosol volume increased for 6 months due to gas-to-particle conversion and then decreased to background levels in the following 6 months.

El Chichon and 'mystery cloud' aerosols between 30 and 55 km Global observations from the SME visible spectrometer

Science.gov (United States)

Clancy, R. T.

1986-01-01

Visible limb radiances measured by the Solar Mesosphere Explorer (SME) are used to obtain volume scattering ratios for aerosol loading in the 30-55 km altitude range of the stratosphere. Global maps of these ratios are presented for the period January 1982 to August 1984. Significant aerosol scattering from the 'mystery cloud' and El Chichon aerosol layers are found above 30 km. A timescale of approximately 2 months between the appearance of the aerosol at 30.5 km and at 37.5 km is consistent with vertical transport of aerosol or vapor by eddy diffusion above 30 km. An anticorrelation exists between aerosol scattering and stratospheric temperatures. Periods of lower stratospheric temperatures may account for the formation of aerosol between 40 and 55 km altitude.

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

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

Science.gov (United States)

Adachi, K.; Buseck, P. R.

2008-05-01

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.

Hygroscopicity of organic surrogate compounds from biomass burning and their effect on the efflorescence of ammonium sulfate in mixed aerosol particles

Science.gov (United States)

Lei, Ting; Zuend, Andreas; Cheng, Yafang; Su, Hang; Wang, Weigang; Ge, Maofa

2018-01-01

Hygroscopic growth factors of organic surrogate compounds representing biomass burning and mixed organic-inorganic aerosol particles exhibit variability during dehydration experiments depending on their chemical composition, which we observed using a hygroscopicity tandem differential mobility analyzer (HTDMA). We observed that levoglucosan and humic acid aerosol particles release water upon dehumidification in the range from 90 to 5 % relative humidity (RH). However, 4-Hydroxybenzoic acid aerosol particles remain in the solid state upon dehumidification and exhibit a small shrinking in size at higher RH compared to the dry size. For example, the measured growth factor of 4-hyroxybenzoic acid aerosol particles is ˜ 0.96 at 90 % RH. The measurements were accompanied by RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model and Extended Aerosol Inorganics Model (E-AIM), the Zdanovskii-Stokes-Robinson (ZSR) relation, and a fitted hygroscopicity expression. We observed several effects of organic components on the hygroscopicity behavior of mixtures containing ammonium sulfate (AS) in relation to the different mass fractions of organic compounds: (1) a shift of efflorescence relative humidity (ERH) of ammonium sulfate to higher RH due to the presence of 25 wt % levoglucosan in the mixture. (2) There is a distinct efflorescence transition at 25 % RH for mixtures consisting of 25 wt % of 4-hydroxybenzoic acid compared to the ERH at 35 % for organic-free AS particles. (3) There is indication for a liquid-to-solid phase transition of 4-hydroxybenzoic acid in the mixed particles during dehydration. (4) A humic acid component shows no significant effect on the efflorescence of AS in mixed aerosol particles. In addition, consideration of a composition-dependent degree of dissolution of crystallization AS (solid-liquid equilibrium) in the AIOMFAC and E-AIM models leads to a

Agglomerated novel spray-dried lactose-leucine tailored as a carrier to enhance the aerosolization performance of salbutamol sulfate from DPI formulations.

Science.gov (United States)

Molina, Carlos; Kaialy, Waseem; Chen, Qiao; Commandeur, Daniel; Nokhodchi, Ali

2017-12-19

Spray-drying allows to modify the physicochemical/mechanical properties of particles along with their morphology. In the present study, L -leucine with varying concentrations (0.1, 0.5, 1, 5, and 10% w/v) were incorporated into lactose monohydrate solution for spray-drying to enhance the aerosolization performance of dry powder inhalers containing spray-dried lactose-leucine and salbutamol sulfate. The prepared spray-dried lactose-leucine carriers were analyzed using laser diffraction (particle size), differential scanning calorimetry (thermal behavior), scanning electron microscopy (morphology), powder X-ray diffraction (crystallinity), Fourier transform infrared spectroscopy (interaction at molecular level), and in vitro aerosolization performance (deposition). The results showed that the efficacy of salbutamol sulfate's aerosolization performance was, in part, due to the introduction of L -leucine in the carrier, prior to being spray-dried, accounting for an increase in the fine particle fraction (FPF) of salbutamol sulfate from spray-dried lactose-leucine (0.5% leucine) in comparison to all other carriers. It was shown that all of the spray-dried carriers were spherical in their morphology with some agglomerates and contained a mixture of amorphous, α-lactose, and β-lactose. It was also interesting to note that spray-dried lactose-leucine particles were agglomerated during the spray-drying process to make coarse particles (volume mean diameter of 79 to 87 μm) suitable as a carrier in DPI formulations.

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

Science.gov (United States)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

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.

Detection and mapping of polar stratospheric clouds using limb scattering observations

Directory of Open Access Journals (Sweden)

C. von Savigny

2005-01-01

Full Text Available Satellite-based measurements of Visible/NIR limb-scattered solar radiation are well suited for the detection and mapping of polar stratospheric clouds (PSCs. This publication describes a method to detect PCSs from limb scattering observations with the Scanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY on the European Space Agency's Envisat spacecraft. The method is based on a color-index approach and requires a priori knowledge of the stratospheric background aerosol loading in order to avoid false PSC identifications by stratospheric background aerosol. The method is applied to a sample data set including the 2003 PSC season in the Southern Hemisphere. The PSCs are correlated with coincident UKMO model temperature data, and with very few exceptions, the detected PSCs occur at temperatures below 195–198 K. Monthly averaged PSC descent rates are about 1.5 km/month for the −50° S to −75° S latitude range and assume a maximum between August and September with a value of about 2.5 km/month. The main cause of the PSC descent is the slow descent of the lower stratospheric temperature minimum.

Stratospheric Aerosol and Gas Experiment, SAGE III on ISS, An Earth Science Mission on the International Space Station, Schedule Risk Analysis, A Project Perspective

Science.gov (United States)

Bonine, Lauren

2015-01-01

The presentation provides insight into the schedule risk analysis process used by the Stratospheric Aerosol and Gas Experiment III on the International Space Station Project. The presentation focuses on the schedule risk analysis process highlighting the methods for identification of risk inputs, the inclusion of generic risks identified outside the traditional continuous risk management process, and the development of tailored analysis products used to improve risk informed decision making.

Particulate sulfur in the upper troposphere and lowermost stratosphere – sources and climate forcing

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B. G. Martinsson

2017-09-01

Full Text Available This study is based on fine-mode aerosol samples collected in the upper troposphere (UT and the lowermost stratosphere (LMS of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8–12 km altitude of the IAGOS-CARIBIC platform in the time period 1999–2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission and PESA (particle elastic scattering analysis. Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL. Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of

How stratospheric are deep stratospheric intrusions? LUAMI 2008

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T. Trickl

2016-07-01

Full Text Available A large-scale comparison of water-vapour vertical-sounding instruments took place over central Europe on 17 October 2008, during a rather homogeneous deep stratospheric intrusion event (LUAMI, Lindenberg Upper-Air Methods Intercomparison. The measurements were carried out at four observational sites: Payerne (Switzerland, Bilthoven (the Netherlands, Lindenberg (north-eastern Germany, and the Zugspitze mountain (Garmisch-Partenkichen, German Alps, and by an airborne water-vapour lidar system creating a transect of humidity profiles between all four stations. A high data quality was verified that strongly underlines the scientific findings. The intrusion layer was very dry with a minimum mixing ratios of 0 to 35 ppm on its lower west side, but did not drop below 120 ppm on the higher-lying east side (Lindenberg. The dryness hardens the findings of a preceding study (“Part 1”, Trickl et al., 2014 that, e.g., 73 % of deep intrusions reaching the German Alps and travelling 6 days or less exhibit minimum mixing ratios of 50 ppm and less. These low values reflect values found in the lowermost stratosphere and indicate very slow mixing with tropospheric air during the downward transport to the lower troposphere. The peak ozone values were around 70 ppb, confirming the idea that intrusion layers depart from the lowermost edge of the stratosphere. The data suggest an increase of ozone from the lower to the higher edge of the intrusion layer. This behaviour is also confirmed by stratospheric aerosol caught in the layer. Both observations are in agreement with the idea that sections of the vertical distributions of these constituents in the source region were transferred to central Europe without major change. LAGRANTO trajectory calculations demonstrated a rather shallow outflow from the stratosphere just above the dynamical tropopause, for the first time confirming the conclusions in “Part 1” from the Zugspitze CO observations. The

Post-entry and volcanic contaminant abundances of zinc, copper, selenium, germanium and gallium in stratospheric micrometeorites

Science.gov (United States)

Rietmeijer, Frans J. M.

1995-01-01

Some fraction of Zn, Cu, Se, Ga and Ge in chondritic interplanetary dust particles (IDPs) collected in the lower stratosphere between 1981 May and 1984 June has a volcanic origin. I present a method to evaluate the extent of this unavoidable type of stratospheric contamination for individual particles. The mass-normalized abundances for Cu and Ge as a function of mass-normalized stratospheric residence time show their time-integrated stratospheric aerosol abundances. The Zn, Se and Ga abundances show a subdivision into two groups that span approximately two-year periods following the eruptions of the Mount St. Helens (1980 May) and El Chichon (1982 April) volcanoes. Elemental abundances in particles collected at the end of each two-year period indicate low, but not necessarily ambient, volcanic stratospheric abundances. Using this time-integrated baseline, I calculate the straospheric contaminant fractions in nine IDPs and show that Zn, SE and Ga abundances in chondritic IDPs derive in part from stratospheric aerosol contaminants. Post-entry elemental abundances (i.e., the amount that survived atmospheric entry heating of the IDP) show enrichments relative to the CI abundances but in a smaller number of particles than previously suggested.

Stratospheric cooling and polar ozone loss due to H2 emissions of a global hydrogen economy

Science.gov (United States)

Feck, T.; Grooß, J.-U.; Riese, M.; Vogel, B.

2009-04-01

"Green" hydrogen is seen as a major element of the future energy supply to reduce greenhouse gas emissions substantially. However, due to the possible interactions of hydrogen (H2) with other atmospheric constituents there is a need to analyse the implications of additional atmospheric H2 that could result from hydrogen leakage of a global hydrogen infrastructure. Emissions of molecular H2 can occur along the whole hydrogen process chain which increase the tropospheric H2 burden. Across the tropical tropopause H2 reaches the stratosphere where it is oxidised and forms water vapour (H2O). This causes increased IR-emissions into space and hence a cooling of the stratosphere. Both effects, the increase of stratospheric H2O and the cooling, enhances the potential of chlorine activation on liquid sulfate aerosol and polar stratospheric clouds (PSCs), which increase polar ozone destruction. Hence a global hydrogen economy could provoke polar ozone loss and could lead to a substantial delay of the current projected recovery of the stratospheric ozone layer. Our investigations show that even if 90% of the current global fossil primary energy input could be replaced by hydrogen and approximately 9.5% of the product gas would leak to the atmosphere, the ozone loss would be increased between 15 to 26 Dobson Units (DU) if the stratospheric CFC loading would retain unchanged. A consistency check of the used approximation methods with the Chemical Lagrangian Model of the Stratosphere (CLaMS) shows that this additional ozone loss can probably be treated as an upper limit. Towards more realistic future H2 leakage rate assumptions (< 3%) the additional ozone loss would be rather small (? 10 DU). However, in all cases the full damage would only occur if stratospheric CFC-levels would retain unchanged. Due to the CFC-prohibition as a result of the Montreal Protocol the forecasts suggest a decline of the stratospheric CFC loading about 50% until 2050. In this case our calculations

High Altitude Emissions of Black Carbon Aerosols: Potential Climate Implications

Science.gov (United States)

Satheesh, S. K.

2017-12-01

Synthesizing a series of ground-based and airborne measurements of aerosols over the Indian region during summer and pre-monsoon seasons have revealed the persistence of elevated absorbing aerosol layers over most of the Indian region; more than 50% of which located above clouds. Subsequent, in situ measurements of black carbon (BC) using high-altitude balloons, showed surprising layers with high concentrations in the middle and upper troposphere even at an altitude of 8 to 10 kms. Simultaneous measurements of the vertical thermal structure have shown localized warming due to BC absorption leading to large reduction in lapse rate and sharp temperature inversion, which in turn increases the atmospheric stability. This aerosol-induced stable layer is conducive for maintaining the black carbon layer longer at that level, leading thereby to further solar absorption and subsequently triggering dry convection. These observations support the `solar escalator' concept through which absorption-warming-convection cycles lead to self-lifting of BC to upper troposphere or even to lower stratosphere under favorable conditions in a matter of a few days. Employing an on-line regional chemistry transport model (WRF-Chem), incorporating aircraft emissions, it is shown that emissions from high-flying aircrafts as the most likely source of these elevated black carbon layers. These in-situ injected particles, produce significant warming of the thin air in those heights and lift these layers to even upper tropospheric/lower stratospheric heights, aided by the strong monsoonal convection occurring over the region, which are known to overshoot the tropical tropopause leading to injection of tropospheric air mass (along with its constituent aerosols) into the stratosphere, especially during monsoon season when the tropical tropopause layer is known to be thinnest. These simulations are further supported by the CALIPSO space-borne LIDAR derived extinction coefficient profiles. Based on

Observed perturbations of the Earth's Radiation Budget - A response to the El Chichon stratospheric aerosol layer?

Science.gov (United States)

Ardanuy, P. E.; Kyle, H. L.

1986-01-01

The Earth Radiation Budget experiment, launched aboard the Nimbus-7 polar-orbiting spacecraft in late 1978, has now taken over seven years of measurements. The dataset, which is global in coverage, consists of the individual components of the earth's radiation budget, including longwave emission, net radiation, and both total and near-infrared albedos. Starting some six months after the 1982 eruption of the El Chichon volcano, substantial long-lived positive shortwave irradiance anomalies were observed by the experiment in both the northern and southern polar regions. Analysis of the morphology of this phenomena indicates that the cause is the global stratospheric aerosol layer which formed from the cloud of volcanic effluents. There was little change in the emitted longwave in the polar regions. At the north pole the largest anomaly was in the near-infrared, but at the south pole the near UV-visible anomaly was larger. Assuming an exponential decay, the time constant for the north polar, near-infrared anomaly was 1.2 years. At mid- and low latitudes the effect of the El Chichon aerosol layer could not be separated from the strong reflected-shortwave and emitted-longwave perturbations issuing from the El Nino/Southern Oscillation event of 1982-83.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

Science.gov (United States)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Tropical stratospheric water vapor measured by the microwave limb sounder (MLS)

Science.gov (United States)

Carr, E. S.; Harwood, R. S.; Mote, P. W.; Peckham, G. E.; Suttie, R. A.; Lahoz, W. A.; O'Neill, A.; Froidevaux, L.; Jarnot, R. F.; Read, W. G.

1995-01-01

The lower stratospheric variability of equatorial water vapor, measured by the Microwave Limb Sounder (MLS), follows an annual cycle modulated by the quasi-biennial oscillation. At levels higher in the stratosphere, water vapor measurements exhibit a semi-annual oscillatory signal with the largest amplitudes at 2.2 and 1hPa. Zonal-mean cross sections of MLS water vapor are consistent with previous satellite measurements from the limb infrared monitor of the stratosphere (LIMS) and the stratospheric Aerosol and Gas Experiment 2 (SAGE 2) instruments in that they show water vapor increasing upwards and the polewards from a well defined minimum in the tropics. The minimum values vary in height between the retrieved 46 and 22hPa pressure levels.

Climate forcing by anthropogenic aerosols

Energy Technology Data Exchange (ETDEWEB)

Charlson, R J; Schwartz, S E; Hales, J M; Cess, R D; Coakley, Jr, J A; Hansen, J E; Hofmann, D J [University of Washington, Seattle, WA (USA). Inst. for Environmental Studies, Dept. of Atmospheric Sciences

1992-01-24

Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol in particular has imposed a major perturbation to this forcing. Both the direct scattering of short wavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square metre, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes. 73 refs., 4 figs., 2 tabs.

Climate forcing by anthropogenic aerosols.

Science.gov (United States)

Charlson, R J; Schwartz, S E; Hales, J M; Cess, R D; Coakley, J A; Hansen, J E; Hofmann, D J

1992-01-24

Although long considered to be of marginal importance to global climate change, tropospheric aerosol contributes substantially to radiative forcing, and anthropogenic sulfate aerosol in particular has imposed a major perturbation to this forcing. Both the direct scattering of shortwavelength solar radiation and the modification of the shortwave reflective properties of clouds by sulfate aerosol particles increase planetary albedo, thereby exerting a cooling influence on the planet. Current climate forcing due to anthropogenic sulfate is estimated to be -1 to -2 watts per square meter, globally averaged. This perturbation is comparable in magnitude to current anthropogenic greenhouse gas forcing but opposite in sign. Thus, the aerosol forcing has likely offset global greenhouse warming to a substantial degree. However, differences in geographical and seasonal distributions of these forcings preclude any simple compensation. Aerosol effects must be taken into account in evaluating anthropogenic influences on past, current, and projected future climate and in formulating policy regarding controls on emission of greenhouse gases and sulfur dioxide. Resolution of such policy issues requires integrated research on the magnitude and geographical distribution of aerosol climate forcing and on the controlling chemical and physical processes.

Researchers, other experts examine climate engineering issues

International Nuclear Information System (INIS)

Baum, R.

1994-01-01

The feasibility of deliberately engineering Earth's climate--and the social, economic, political, and ethical issues raised by such projects--were explored by two panels at the annual meeting of the American Association for the Advancement of Science (AAAS), held in late February in San Francisco. These projects include dispersal of sulfate particles in the stratosphere to reflect sunlight, fertilizing the southern oceans with iron to stimulate phytoplankton growth, and injecting ethane or propane into the stratosphere over Antarctica to counteract ozone-depleting chemical reactions. The feasibility of such projects was the focus of the first panel. Joyce E. Penner, of Lawrence Livermore National Laboratory, describes studies of natural and anthropogenic sulfate aerosols that suggest that these chemical species reduce the solar flux reaching the Earth's surface. The research indicates it might be possible to counteract greenhouse warming, at least in part, by injecting sulfate aerosols into the stratosphere. Should such an approach be used to counteract greenhouse warming? Should any climate engineering project be considered? These sorts of questions were the focus of the second panel

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z.; Young, S.E.; Becker, C.H.; Coggiola, M.J. [SRI International, Menlo Park, CA (United States); Wollnik, H. [Giessen Univ. (Germany)

1997-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z; Young, S E; Becker, C H; Coggiola, M J [SRI International, Menlo Park, CA (United States); Wollnik, H [Giessen Univ. (Germany)

1998-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Optical properties and microphysical characterization of single levitated aerosol particles. Final report; Optische Eigenschaften und mikrophysikalische Charakterisierung von einzeln levitierten Aerosolpartikeln. Schlussbericht

Energy Technology Data Exchange (ETDEWEB)

Leisner, T.; Vortisch, H.

2002-07-01

Composition, micro structure and phase of the sulfate aerosol particles in the stratosphere are crucial for their activity in the polar stratospheric ozone depletion and not well known until now. We have performed Raman spectroscopic laboratory investigations with model particles levitated in an electrodynamic balance under stratospheric conditions. We were able to obtain new results on the dynamics of phase transitions in such particles and on the type of metastable structures encountered after the freezing of heavily supercooled sulfuric acid solution. The compositions found were usually not consistent with the phase diagram. Sulfuric acid tetrahydrate was the dominant compound even when dilute solution nucleated. It was formed crystalline not immediately after nucleation but only when the particles approached the melting point. At lower temperatures a nanocrystalline and strongly disordered hydrate was observed. Our investigations help to arrive at a better understanding of the role of the sulfuric acid aerosol in stratospheric chemistry. (orig.) [German] Zusammensetzung, Mikrostruktur und Aggregatzustand der stratosphaerischen Schwefelsaeureaerosole bestimmen deren Aktivitaet im polaren Ozonabbau und sind bislang kaum erforscht. Unsere ramanspektroskopischen Laboruntersuchungen an Modellpartikeln in einem elektrodynamischen Levitator konnten hier neue Erkenntnisse zur Dynamik von Phasenumwandlungen sowie der Struktur metastabiler Zustaende liefern. Insbesondere wurden stark vom Phasendiagramm abweichende Zusammensetzungen als typisch erkannt. So konnte Schwefelsaeuretetrahydrat als das dominierende Hydrat bei der Nukleation auch verduennter Schwefelsaeureloesungen erkannt werden. Es bildet sich kritallin jedoch nicht direkt beim Gefrieren unterkuehlter Schwefelsaeureloesungen, sondern erst bei deren Annaeherung an den Schmelzpunkt. Vorher liegt ein nanokristallines und stark ungeordnetes Hydrat vor. Durch derartige Untersuchungen wird ein besseres Verstaendnis

Comparison of aerosol extinction between lidar and SAGE II over Gadanki, a tropical station in India

Directory of Open Access Journals (Sweden)

P. Kulkarni

2015-03-01

Full Text Available An extensive comparison of aerosol extinction has been performed using lidar and Stratospheric Aerosol and Gas Experiment (SAGE II data over Gadanki (13.5° N, 79.2° E, a tropical station in India, following coincident criteria during volcanically quiescent conditions from 1998 to 2005. The aerosol extinctions derived from lidar are higher than SAGE II during all seasons in the upper troposphere (UT, while in the lower-stratosphere (LS values are closer. The seasonal mean percent differences between lidar and SAGE II aerosol extinctions are > 100% in the UT and Ba (sr−1, the ratio between aerosol backscattering and extinction, are needed for the tropics for a more accurate derivation of aerosol extinction.

Laboratory chemistry and stratospheric clouds

Science.gov (United States)

Molina, Mario J.

1989-01-01

Results are presented from laboratory experiments on the chemistry of ice particles to study the role of HCl and ClONO2 from CFCs in stratospheric ozone depletion over Antarctica. It is found that gaseous HCl is scavenged with high efficiency by the ice and the gas phase chlorine nitrate may react with the HCL-containing ice to produce Cl2. Also, consideration is given ot the behavior of solid nitric acid trihydrate and sulfuric acid aerosols.

Radiative and Dynamical Feedbacks Limit the Climate Response to Extremely Large Volcanic Eruptions

Science.gov (United States)

Wade, D. C.; Vidal, C. M.; Keeble, J. M.; Griffiths, P. T.; Archibald, A. T.

2017-12-01

Explosive volcanic eruptions are a major cause of chemical and climatic perturbations to the atmosphere, injecting chemically and radiatively active species such as sulfur dioxide (SO2) into the stratosphere. The rate determining step for sulfate aerosol production is SO2 + OH +M → HSO3 +M. This means that chemical feedbacks on the hydroxyl radical, OH, can modulate the production rate of sulfate aerosol and hence the climate effects of large volcanic eruptions. Radiative feedbacks due to aerosols, ozone and sulfur dioxide and subsequent dynamical changes also affect the evolution of the aerosol cloud. Here we assess the role of radiative and chemical feedbacks on sulfate aerosol production using UM-UKCA, a chemistry-climate model coupled to GLOMAP, a prognostic modal aerosol model. A 200 Tg (10x Pinatubo) emission scenario is investigated. Accounting for radiative feedbacks, the SO2 lifetime is 55 days compared to 26 days in the baseline 20 Tg (1x Pinatubo) simulation. By contrast, if all radiative feedbacks are neglected the lifetime is 73 days. Including radiative feedbacks reduces the SO2 lifetime: heating of the lower stratosphere by aerosol increases upwelling and increases transport of water vapour across the tropopause, increasing OH concentrations. The maximum effective radius of the aerosol particles increases from 1.09 µm to 1.34 µm as the production of aerosol is quicker. Larger and fewer aerosol particles are produced which are less effective at scattering shortwave radiation and will more quickly sediment from the stratosphere. As a result, the resulting climate cooling by the eruption will be less strong when accounting for these radiative feedbacks. We illustrate the consequences of these effects for the 1257 Samalas eruption, the largest common era volcanic eruption, using UM-UKCA in a coupled atmosphere-ocean configuration. As a potentially halogen rich eruption, we investigate the differing ozone response to halogen-rich and halogen

Coupled Aerosol-Chemistry-Climate Twentieth-Century Transient Model Investigation: Trends in Short-Lived Species and Climate Responses

Science.gov (United States)

Koch, Dorothy; Bauer, Susanne E.; Del Genio, Anthony; Faluvegi, Greg; McConnell, Joseph R.; Menon, Surabi; Miller, Ronald L.; Rind, David; Ruedy, Reto; Schmidt, Gavin A.;

Persistence of Antarctic polar stratospheric clouds

Science.gov (United States)

Mccormick, M. Patrick; Trepte, C. R.

1988-01-01

The persistence of Polar Stratospheric Clouds (PSCs) observed by the Stratospheric Aerosol Measurement (SAM) 2 satellite sensor over a 9-year period is compared and contrasted. Histograms of the SAM 2 1.0 micron extinction ratio data (aerosol extinction normalized by the molecular extinction) at an altitude of 18 km in the Antarctic have been generated for three 10-day periods in the month of September. Statistics for eight different years (1979 to 1982 and 1984 to 1987) are shown in separate panels for each figure. Since the SAM 2 system is a solar occultation experiment, observations are limited to the edge of the polar night and no measurements are made deep within the vortex where temperatures could be colder. For this reason, use is made of the NMC global gridded fields and the known temperature-extinction relationship to infer additional information on the occurrence and areal coverage of PSCs. Calculations of the daily areal coverage of the 195 K isotherm will be presented for this same period of data. This contour level lies in the range of the predicted temperature for onset of the Type 1 particle enhancement mode at 50 mb (Poole and McCormick, 1988b) and should indicate approximately when formation of the binary HNO3-H2O particles begins.

Optical properties of the urban aerosol and their relation to chemical composition

International Nuclear Information System (INIS)

Leaderer, B.P.; Stolwijk, J.A.J.

1980-01-01

Light extinction and resulting visibility degradation in an unsaturated precipitation-free atmosphere are determined by light absorption and scattering and are caused by a complex mix of natural components and anthropogenic pollutants. The paper reviews correlation studies relating light scattering and light extinction (visibility) to concentrations of sulfate mass, nitrate mass, the remainder of the mass, and in some cases organic aerosol mass, while accounting for variations in relative humidity. It is found that sulfate aerosol mass is the dominant chemical aerosol species affecting light scattering and extinction. The dominant effect of sulfate mass on light scattering and extinction, even when sulfates account for a relatively small fraction of the total mass, results from the fact that sulfates are secondary aerosols and are mostly found in the 0.1-1.0 micron size range

Atmospheric Sampling of Aerosols to Stratospheric Altitudes using High Altitude Balloons

Science.gov (United States)

Jerde, E. A.; Thomas, E.

2010-12-01

Although carbon dioxide represents a long-lived atmospheric component relevant to global climate change, it is also understood that many additional contributors influence the overall climate of Earth. Among these, short-lived components are more difficult to incorporate into models due to uncertainties in the abundances of these both spatially and temporally. Possibly the most significant of these short-lived components falls under the heading of “black carbon” (BC). There are numerous overlapping definitions of BC, but it is basically carbonaceous in nature and light absorbing. Due to its potential as a climate forcer, an understanding of the BC population in the atmosphere is critical for modeling of radiative forcing. Prior measurements of atmospheric BC generally consist of airplane- and ground-based sampling, typically below 5000 m and restricted in time and space. Given that BC has a residence time on the order of days, short-term variability is easily missed. Further, since the radiative forcing is a result of BC distributed through the entire atmospheric column, aircraft sampling is by definition incomplete. We are in the process of planning a more comprehensive sampling of the atmosphere for BC using high-altitude balloons. Balloon-borne sampling is a highly reliable means to sample air through the entire troposphere and into the lower stratosphere. Our system will incorporate a balloon and a flight train of two modules. One module will house an atmospheric sampler. This sampler will be single-stage (samples all particle sizes together), and will place particles directly on an SEM sample stub for analysis. The nozzle depositing the sample will be offset from the center of the stub, placing the aerosol particles toward the edge. At various altitudes, the stub will be rotated 45 degrees, providing 6-8 sample “cuts” of particle populations through the atmospheric column. The flights will reach approximately 27 km altitude, above which the balloons

Weakened tropical circulation and reduced precipitation in response to geoengineering

International Nuclear Information System (INIS)

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

2014-01-01

Geoengineering by injection of reflective aerosols into the stratosphere has been proposed as a way to counteract the warming effect of greenhouse gases by reducing the intensity of solar radiation reaching the surface. Here, climate model simulations are used to examine the effect of geoengineering on the tropical overturning circulation. The strength of the circulation is related to the atmospheric static stability and has implications for tropical rainfall. The tropical circulation is projected to weaken under anthropogenic global warming. Geoengineering with stratospheric sulfate aerosol does not mitigate this weakening of the circulation. This response is due to a fast adjustment of the troposphere to radiative heating from the aerosol layer. This effect is not captured when geoengineering is modelled as a reduction in total solar irradiance, suggesting caution is required when interpreting model results from solar dimming experiments as analogues for stratospheric aerosol geoengineering. (letter)

Sub-micrometer scale minor element mapping in interplanetary dust particles: a test for stratospheric contamination

International Nuclear Information System (INIS)

Flynn, G.J.; Keller, L.P.; Sutton, S.R.

2006-01-01

We mapped the spatial distribution of minor elements including K, Mn, and Zn in 3 IDPs and found no evidence for the surface coatings (rims) of these elements that would be expected if the enrichments previously reported were due to contamination. Combined X-ray microprobe (XRM), energy dispersive x-ray fluorescence using a Transmission Electron Microscope (TEM), and electron microprobe measurements have determined that the average bulk chemical composition of the interplanetary dust particles (IDPs) collected from the Earth's stratosphere is enriched relative to the CI meteorite composition by a factor of 2 to 4 for carbon and for the moderately volatile elements Na, K, P, Mn, Cu, Zn, Ga, Ge, and Se, and enriched to ∼30 times CI for Br. However, Jessberger et al., who have reported similar bulk enrichments using Proton Induced X-ray Emission (PIXE), attribute the enrichments to contamination by meteor-derived atmospheric aerosols during the several weeks these IDPs reside in the Earth's atmosphere prior to collection. Using scanning Auger spectroscopy, a very sensitive surface analysis technique, Mackinnon and Mogk have observed S contamination on the surface of IDPs, presumably due to the accretion of sulfate aerosols during stratospheric residence. But the S-rich layer they detected was so thin (∼100 angstroms thick) that the total amount of S on the surface was too small to significantly perturb the bulk S-content of a chondritic IDP. Stephan et al. provide support for the contamination hypothesis by reporting the enrichment of Br on the edges of the IDPs using Time-of-Flight Secondary-Ion Mass-Spectrometry (TOF-SIMS), but TOF-SIMS is notorious for producing false edge-effects, particularly on irregularly-shaped samples like IDPs. Sutton et al. mapped the spatial distribution of Fe, Ni, Zn, Br, and Sr, at the ∼2 (micro)m scale, in four IDPs using element-specific x-ray fluorescence (XRF) computed microtomography. They found the moderately volatile

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

Science.gov (United States)

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

1983-01-01

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

Isotopic constraints on heterogeneous sulfate production in Beijing haze

Science.gov (United States)

He, Pengzhen; Alexander, Becky; Geng, Lei; Chi, Xiyuan; Fan, Shidong; Zhan, Haicong; Kang, Hui; Zheng, Guangjie; Cheng, Yafang; Su, Hang; Liu, Cheng; Xie, Zhouqing

2018-04-01

Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter) in Beijing is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. Here we present observations of the oxygen-17 excess of PM2.5 sulfate (Δ17O(SO42-)) collected in Beijing haze from October 2014 to January 2015 to constrain possible sulfate formation pathways. Throughout the sampling campaign, the 12-hourly averaged PM2.5 concentrations ranged from 16 to 323 µg m-3 with a mean of (141 ± 88 (1σ)) µg m-3, with SO42- representing 8-25 % of PM2.5 mass. The observed Δ17O(SO42-) varied from 0.1 to 1.6 ‰ with a mean of (0.9 ± 0.3) ‰. Δ17O(SO42-) increased with PM2.5 levels in October 2014 while the opposite trend was observed from November 2014 to January 2015. Our estimate suggested that in-cloud reactions dominated sulfate production on polluted days (PDs, PM2.5 ≥ 75 µg m-3) of Case II in October 2014 due to the relatively high cloud liquid water content, with a fractional contribution of up to 68 %. During PDs of Cases I and III-V, heterogeneous sulfate production (Phet) was estimated to contribute 41-54 % to total sulfate formation with a mean of (48 ± 5) %. For the specific mechanisms of heterogeneous oxidation of SO2, chemical reaction kinetics calculations suggested S(IV) ( = SO2 ⚫ H2O + HSO3- + SO32-) oxidation by H2O2 in aerosol water accounted for 5-13 % of Phet. The relative importance of heterogeneous sulfate production by other mechanisms was constrained by our observed Δ17O(SO42-). Heterogeneous sulfate production via S(IV) oxidation by O3 was estimated to contribute 21-22 % of Phet on average. Heterogeneous sulfate production pathways that result in zero-Δ17O(SO42-), such as S(IV) oxidation by NO2 in aerosol water and/or by O2 via a radical chain mechanism, contributed the remaining 66-73 % of Phet. The assumption about the thermodynamic state of aerosols

Volcanic signals in oceans

KAUST Repository

Stenchikov, Georgiy L.; Delworth, Thomas L.; Ramaswamy, V.; Stouffer, Ronald J.; Wittenberg, Andrew; Zeng, Fanrong

2009-01-01

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

Synergistic reaction between SO2 and NO2 on mineral oxides: a potential formation pathway of sulfate aerosol.

Science.gov (United States)

Liu, Chang; Ma, Qingxin; Liu, Yongchun; Ma, Jinzhu; He, Hong

2012-02-07

Sulfate is one of the most important aerosols in the atmosphere. A new sulfate formation pathway via synergistic reactions between SO(2) and NO(2) on mineral oxides was proposed. The heterogeneous reactions of SO(2) and NO(2) on CaO, α-Fe(2)O(3), ZnO, MgO, α-Al(2)O(3), TiO(2), and SiO(2) were investigated by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in situ DRIFTS) at ambient temperature. Formation of sulfate from adsorbed SO(2) was promoted by the coexisting NO(2), while surface N(2)O(4) was observed as the crucial oxidant for the oxidation of surface sulfite. This process was significantly promoted by the presence of O(2). The synergistic effect between SO(2) and NO(2) was not observed on other mineral particles (such as CaCO(3) and CaSO(4)) probably due to the lack of the surface reactive oxygen sites. The synergistic reaction between SO(2) and NO(2) on mineral oxides resulted in the formation of internal mixtures of sulfate, nitrate, and mineral oxides. The change of mixture state will affect the physicochemical properties of atmospheric particles and therefore further influence their environmental and climate effects.

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.

Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities.

Science.gov (United States)

Van Wyngarden, A L; Pérez-Montaño, S; Bui, J V H; Li, E S W; Nelson, T E; Ha, K T; Leong, L; Iraci, L T

Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H 2 SO 4 ) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and 1 H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal

Investigations of the Climate System Response to Climate Engineering in a Hierarchy of Models

Science.gov (United States)

McCusker, Kelly E.

Global warming due to anthropogenic emissions of greenhouse gases is causing negative impacts on diverse ecological and human systems around the globe, and these impacts are projected to worsen as climate continues to warm. In the absence of meaningful greenhouse gas emissions reductions, new strategies have been proposed to engineer the climate, with the aim of preventing further warming and avoiding associated climate impacts. We investigate one such strategy here, falling under the umbrella of `solar radiation management', in which sulfate aerosols are injected into the stratosphere. We use a global climate model with a coupled mixed-layer depth ocean and with a fully-coupled ocean general circulation model to simulate the stabilization of climate by balancing increasing carbon dioxide with increasing stratospheric sulfate concentrations. We evaluate whether or not severe climate impacts, such as melting Arctic sea ice, tropical crop failure, or destabilization of the West Antarctic ice sheet, could be avoided. We find that while tropical climate emergencies might be avoided by use of stratospheric aerosol injections, avoiding polar emergencies cannot be guaranteed due to large residual climate changes in those regions, which are in part due to residual atmospheric circulation anomalies. We also find that the inclusion of a fully-coupled ocean is important for determining the regional climate response because of its dynamical feedbacks. The efficacy of stratospheric sulfate aerosol injections, and solar radiation management more generally, depends on its ability to be maintained indefinitely, without interruption from a variety of possible sources, such as technological failure, a breakdown in global cooperation, lack of funding, or negative unintended consequences. We next consider the scenario in which stratospheric sulfate injections are abruptly terminated after a multi- decadal period of implementation while greenhouse gas emissions have continued unabated

Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing

Directory of Open Access Journals (Sweden)

J. E. Penner

2009-02-01

Full Text Available Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm⁻² while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm⁻² and −0.16 to −0.12 Wm⁻², respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.

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.

Drift-corrected Odin-OSIRIS ozone product: algorithm and updated stratospheric ozone trends

Directory of Open Access Journals (Sweden)

A. E. Bourassa

2018-01-01

Full Text Available A small long-term drift in the Optical Spectrograph and Infrared Imager System (OSIRIS stratospheric ozone product, manifested mostly since 2012, is quantified and attributed to a changing bias in the limb pointing knowledge of the instrument. A correction to this pointing drift using a predictable shape in the measured limb radiance profile is implemented and applied within the OSIRIS retrieval algorithm. This new data product, version 5.10, displays substantially better both long- and short-term agreement with Microwave Limb Sounder (MLS ozone throughout the stratosphere due to the pointing correction. Previously reported stratospheric ozone trends over the time period 1984–2013, which were derived by merging the altitude–number density ozone profile measurements from the Stratospheric Aerosol and Gas Experiment (SAGE II satellite instrument (1984–2005 and from OSIRIS (2002–2013, are recalculated using the new OSIRIS version 5.10 product and extended to 2017. These results still show statistically significant positive trends throughout the upper stratosphere since 1997, but at weaker levels that are more closely in line with estimates from other data records.

Review of recent research on the climatic effect of aerosols

International Nuclear Information System (INIS)

Charlock, T.P.; Kondratyev, K.; Prokofyev, M.

1993-01-01

A review of relatively recent research on the climatic effects of aerosols is presented. Most of the inferences of the climatic effects of aerosols have been obtained through assuming a certain aerosol model in conjunction with a particular climate model. The following radiative effects of aerosols are identified: The planetary albedo is generally increased due to the backscatter of solar radiation by aerosols, with the exception of aerosols situated above a highly reflecting surface. Solar radiation absorption by some aerosols can offset the cooling due to aerosol backscatter. Although aerosol effects dominate for short-wave radiation, absorption and emission of terrestrial radiation by aerosols produces a warming effect. Various climate models are used to assess the impact of aerosols on climate. A two-stream approximation to the radiation transfer equation is adequate for optically thin layers where single scattering is applicable. Improved models to include aerosol terrestrial radiation effects, important feedback mechanisms, and the prediction of globally and seasonally averaged surface and atmospheric temperatures are provided by the so-called radiative-convective models (RCM's). The basic structure of the RCM's, which is regarded as adequate for many aerosol climate applications, is described. The general circulation model (GCM) is also described briefly. A full-scale GCM incorporating realistic aerosol inputs is yet to be formulated to include regional variability of the aerosol. Moreover, detailed computer modeling associated with GCM climate models can often confuse the basic physics. Because volcanic aerosols injected into the stratosphere have long residence times, they provide a good case study of the climate response to a change in the atmospheric aerosol. The chapter gives a critique of modeling work done to establish climatic effects of stratospheric aerosols

Balance of the tropospheric ozone and its relation to stratospheric intrusions indicated by cosmogenic radionuclides. Part 13. Annual report, 1 February 1982-31 January 1983

International Nuclear Information System (INIS)

Reiter, R.; Kanter, H.J.; Jaeger, H.; Munzert, K.

1985-06-01

A statistical evaluation of tropospheric ozone concentrations in the air obtained at 3 different levels is presented from data covering 1977 to 1984. Annual and interannual variations are used to project a trend. To clarify the climatology of the stratospheric exchange, the measuring series of cosmogenic radionuclides Be7, P32, P33 covering the period 1970 through 1981 are statistically analyzed with regard to the ozone concentration recorded on the Zugspitze. The statistics of stratospheric intrusions is shown and the stratospheric residence time is estimated. Effects of the eruption of volcano El Chichon in April 1982 on the concentration of the stratospheric aerosol are documented. The time variation of the concentration of the stratospheric aerosol is studied with consideration of the stratospheric circulation. The noted effects are weighed by a comparison with earlier volcanic eruptions. First results of CO 2 recordings in the lower stratosphere are presented. Based on CO 2 recording series from two different levels (740 m and 1780 m a.s.1) from the years 1978 to 1980, systematic differences are shown as a function of height. The question of sources and sinks is discussed to assess the contribution from anthropogenic sources

Improved SAGE II cloud/aerosol categorization and observations of the Asian tropopause aerosol layer: 1989–2005

Directory of Open Access Journals (Sweden)

L. W. Thomason

2013-05-01

Full Text Available We describe the challenges associated with the interpretation of extinction coefficient measurements by the Stratospheric Aerosol and Gas Experiment (SAGE II in the presence of clouds. In particular, we have found that tropospheric aerosol analyses are highly dependent on a robust method for identifying when clouds affect the measured extinction coefficient. Herein, we describe an improved cloud identification method that appears to capture cloud/aerosol events more effectively than early methods. In addition, we summarize additional challenges to observing the Asian Tropopause Aerosol Layer (ATAL using SAGE II observations. Using this new approach, we perform analyses of the upper troposphere, focusing on periods in which the UTLS (upper troposphere/lower stratosphere is relatively free of volcanic material (1989–1990 and after 1996. Of particular interest is the Asian monsoon anticyclone where CALIPSO (Cloud-Aerosol Lidar Pathfinder Satellite Observations has observed an aerosol enhancement. This enhancement, called the ATAL, has a similar morphology to observed enhancements in long-lived trace gas species like CO. Since the CALIPSO record begins in 2006, the question of how long this aerosol feature has been present requires a new look at the long-lived SAGE II data sets despite significant hurdles to its use in the subtropical upper troposphere. We find that there is no evidence of ATAL in the SAGE II data prior to 1998. After 1998, it is clear that aerosol in the upper troposphere in the ATAL region is substantially enhanced relative to the period before that time. In addition, the data generally supports the presence of the ATAL beginning in 1999 and continuing through the end of the mission, though some years (e.g., 2003 are complicated by the presence of episodic enhancements most likely of volcanic origin.

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.

Post-flame gas-phase sulfation of potassium chloride

DEFF Research Database (Denmark)

Li, Bo; Sun, Zhiwei; Li, Zhongshan

2013-01-01

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 homogene......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 ASSET intercomparison of stratosphere and lower mesosphere humidity analyses

Directory of Open Access Journals (Sweden)

H. E. Thornton

2009-02-01

Full Text Available This paper presents results from the first detailed intercomparison of stratosphere-lower mesosphere water vapour analyses; it builds on earlier results from the EU funded framework V "Assimilation of ENVISAT Data" (ASSET project. Stratospheric water vapour plays an important role in many key atmospheric processes and therefore an improved understanding of its daily variability is desirable. With the availability of high resolution, good quality Michelson Interferometer for Passive Atmospheric Sounding (MIPAS water vapour profiles, the ability of four different atmospheric models to assimilate these data is tested. MIPAS data have been assimilated over September 2003 into the models of the European Centre for Medium Range Weather Forecasts (ECMWF, the Belgian Institute for Space and Aeronomy (BIRA-IASB, the French Service d'Aéronomie (SA-IPSL and the UK Met Office. The resultant middle atmosphere humidity analyses are compared against independent satellite data from the Halogen Occultation Experiment (HALOE, the Polar Ozone and Aerosol Measurement (POAM III and the Stratospheric Aerosol and Gas Experiment (SAGE II. The MIPAS water vapour profiles are generally well assimilated in the ECMWF, BIRA-IASB and SA systems, producing stratosphere-mesosphere water vapour fields where the main features compare favourably with the independent observations. However, the models are less capable of assimilating the MIPAS data where water vapour values are locally extreme or in regions of strong humidity gradients, such as the southern hemisphere lower stratosphere polar vortex. Differences in the analyses can be attributed to the choice of humidity control variable, how the background error covariance matrix is generated, the model resolution and its complexity, the degree of quality control of the observations and the use of observations near the model boundaries. Due to the poor performance of the Met Office analyses the results are not included in

The ASSET intercomparison of stratosphere and lower mesosphere humidity analyses

Science.gov (United States)

Thornton, H. E.; Jackson, D. R.; Bekki, S.; Bormann, N.; Errera, Q.; Geer, A. J.; Lahoz, W. A.; Rharmili, S.

2009-02-01

This paper presents results from the first detailed intercomparison of stratosphere-lower mesosphere water vapour analyses; it builds on earlier results from the EU funded framework V "Assimilation of ENVISAT Data" (ASSET) project. Stratospheric water vapour plays an important role in many key atmospheric processes and therefore an improved understanding of its daily variability is desirable. With the availability of high resolution, good quality Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) water vapour profiles, the ability of four different atmospheric models to assimilate these data is tested. MIPAS data have been assimilated over September 2003 into the models of the European Centre for Medium Range Weather Forecasts (ECMWF), the Belgian Institute for Space and Aeronomy (BIRA-IASB), the French Service d'Aéronomie (SA-IPSL) and the UK Met Office. The resultant middle atmosphere humidity analyses are compared against independent satellite data from the Halogen Occultation Experiment (HALOE), the Polar Ozone and Aerosol Measurement (POAM III) and the Stratospheric Aerosol and Gas Experiment (SAGE II). The MIPAS water vapour profiles are generally well assimilated in the ECMWF, BIRA-IASB and SA systems, producing stratosphere-mesosphere water vapour fields where the main features compare favourably with the independent observations. However, the models are less capable of assimilating the MIPAS data where water vapour values are locally extreme or in regions of strong humidity gradients, such as the southern hemisphere lower stratosphere polar vortex. Differences in the analyses can be attributed to the choice of humidity control variable, how the background error covariance matrix is generated, the model resolution and its complexity, the degree of quality control of the observations and the use of observations near the model boundaries. Due to the poor performance of the Met Office analyses the results are not included in the intercomparison

Photothermal spectroscopy of aerosols

International Nuclear Information System (INIS)

Campillo, A.J.; Lin, H.B.

1981-04-01

In situ aerosol absorption spectroscopy was performed using two novel photothermal detection schemes. The first, based on a photorefractive effect and coherent detection, called phase fluctuation optical heterodyne (PFLOH) spectroscopy, could, depending on the geometry employed, yield particle specific or particle and gas absorption data. Single particles of graphite as small as 1 μm were detected in the particle specific mode. In another geometrical configuration, the total absorption (both gas and particle) of submicron sized aerosols of ammonium sulfate particles in equilibrium with gaseous ammonia and water vapor were measured at varying CO 2 laser frequencies. The specific absorption coefficient for the sulfate ion was measured to be 0.5 m 2 /g at 1087 cm -1 . The absorption coefficient sensitivity of this scheme was less than or equal to 10 -8 cm -1 . The second scheme is a hybrid visible Mie scattering scheme incorporating photothermal modulation. Particle specific data on ammonium sulfate droplets were obtained. For chemically identical species, the relative absorption spectrum versus laser frequency can be obtained for polydisperse aerosol distributions directly from the data without the need for complex inverse scattering calculations

Potential impact of carbonaceous aerosol on the upper troposphere and lower stratosphere (UTLS) and precipitation during Asian summer monsoon in a global model simulation

KAUST Repository

Fadnavis, Suvarna

2017-09-28

Recent satellite observations show efficient vertical transport of Asian pollutants from the surface to the upper-level anticyclone by deep monsoon convection. In this paper, we examine the transport of carbonaceous aerosols, including black carbon (BC) and organic carbon (OC), into the monsoon anticyclone using of ECHAM6-HAM, a global aerosol climate model. Further, we investigate impacts of enhanced (doubled) carbonaceous aerosol emissions on the upper troposphere and lower stratosphere (UTLS), underneath monsoon circulation and precipitation from sensitivity simulations. The model simulation shows that boundary layer aerosols are transported into the monsoon anticyclone by the strong monsoon convection from the Bay of Bengal, southern slopes of the Himalayas and the South China Sea. Doubling of emissions of both BC and OC aerosols over Southeast Asia (10° S–50° N, 65–155° E) shows that lofted aerosols produce significant warming (0.6–1 K) over the Tibetan Plateau (TP) near 400–200 hPa and instability in the middle/upper troposphere. These aerosols enhance radiative heating rates (0.02–0.03 K day−1) near the tropopause. The enhanced carbonaceous aerosols alter aerosol radiative forcing (RF) at the surface by −4.74 ± 1.42 W m−2, at the top of the atmosphere (TOA) by +0.37 ± 0.26 W m−2 and in the atmosphere by +5.11 ± 0.83 W m−2 over the TP and Indo-Gangetic Plain region (15–35° N, 80–110° E). Atmospheric warming increases vertical velocities and thereby cloud ice in the upper troposphere. Aerosol induced anomalous warming over the TP facilitates the relative strengthening of the monsoon Hadley circulation and increases moisture inflow by strengthening the cross-equatorial monsoon jet. This increases precipitation amounts over India (1–4 mm day−1) and eastern China (0.2–2 mm day−1). These results are significant at the 99 % confidence level.

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.

Isotopic constraints on heterogeneous sulfate production in Beijing haze

Directory of Open Access Journals (Sweden)

P. He

2018-04-01

Full Text Available Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter in Beijing is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. Here we present observations of the oxygen-17 excess of PM2.5 sulfate (Δ17O(SO42− collected in Beijing haze from October 2014 to January 2015 to constrain possible sulfate formation pathways. Throughout the sampling campaign, the 12-hourly averaged PM2.5 concentrations ranged from 16 to 323 µg m−3 with a mean of (141  ±  88 (1σ µg m−3, with SO42− representing 8–25 % of PM2.5 mass. The observed Δ17O(SO42− varied from 0.1 to 1.6 ‰ with a mean of (0.9  ±  0.3 ‰. Δ17O(SO42− increased with PM2.5 levels in October 2014 while the opposite trend was observed from November 2014 to January 2015. Our estimate suggested that in-cloud reactions dominated sulfate production on polluted days (PDs, PM2.5  ≥  75 µg m−3 of Case II in October 2014 due to the relatively high cloud liquid water content, with a fractional contribution of up to 68 %. During PDs of Cases I and III–V, heterogeneous sulfate production (Phet was estimated to contribute 41–54 % to total sulfate formation with a mean of (48  ±  5 %. For the specific mechanisms of heterogeneous oxidation of SO2, chemical reaction kinetics calculations suggested S(IV ( =  SO2 ⚫ H2O + HSO3−  +  SO32− oxidation by H2O2 in aerosol water accounted for 5–13 % of Phet. The relative importance of heterogeneous sulfate production by other mechanisms was constrained by our observed Δ17O(SO42−. Heterogeneous sulfate production via S(IV oxidation by O3 was estimated to contribute 21–22 % of Phet on average. Heterogeneous sulfate production pathways that result in zero-Δ17O(SO42−, such as S(IV oxidation by NO2 in aerosol water and/or by O2 via a

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

Science.gov (United States)

Harris, E.; Sinha, B.; Hoppe, P.; Foley, S.; Borrmann, S.

2012-05-01

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 the alkalinity non

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

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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

Impact of idealized future stratospheric aerosol injection on the large-scale ocean and land carbon cycles

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Tjiputra, J. F.; Grini, A.; Lee, H.

2016-01-01

Using an Earth system model, we simulate stratospheric aerosol injection (SAI) on top of the Representative Concentration Pathways 8.5 future scenario. Our idealized method prescribes aerosol concentration, linearly increasing from 2020 to 2100, and thereafter remaining constant until 2200. In the aggressive scenario, the model projects a cooling trend toward 2100 despite warming that persists in the high latitudes. Following SAI termination in 2100, a rapid global warming of 0.35 K yr-1 is simulated in the subsequent 10 years, and the global mean temperature returns to levels close to the reference state, though roughly 0.5 K cooler. In contrast to earlier findings, we show a weak response in the terrestrial carbon sink during SAI implementation in the 21st century, which we attribute to nitrogen limitation. The SAI increases the land carbon uptake in the temperate forest-, grassland-, and shrub-dominated regions. The resultant lower temperatures lead to a reduction in the heterotrophic respiration rate and increase soil carbon retention. Changes in precipitation patterns are key drivers for variability in vegetation carbon. Upon SAI termination, the level of vegetation carbon storage returns to the reference case, whereas the soil carbon remains high. The ocean absorbs nearly 10% more carbon in the geoengineered simulation than in the reference simulation, leading to a ˜15 ppm lower atmospheric CO2 concentration in 2100. The largest enhancement in uptake occurs in the North Atlantic. In both hemispheres' polar regions, SAI delays the sea ice melting and, consequently, export production remains low. In the deep water of North Atlantic, SAI-induced circulation changes accelerate the ocean acidification rate and broaden the affected area.

Chapter 3: Evaluating the impacts of carbonaceous aerosols on clouds and climate

Energy Technology Data Exchange (ETDEWEB)

Menon, Surabi; Del Genio, Anthony D.

2007-09-03

contribute to melting of ice and permafrost and change in the length of the season (e.g. early arrival of Spring) (Hansen and Nazarenko, 2004). Besides the impacts of aerosols on the surface albedos in the polar regions, and the thermodynamical impacts of Arctic haze (composed of water soluble sulfates, nitrates, organic and black carbon (BC)), the dynamical response to Arctic haze (through the radiation-circulation feedbacks that cause changes in pressure patterns) is thought to have the potential to modify the mode and strength of large-scale teleconnection patterns such as the Barrents Sea Oscillation that could affect other climate regimes (mainly Europe) (Rinke et al. 2004). Additionally, via the Asian monsoon, wind patterns over the eastern Mediterranean and lower stratospheric pollution at higher latitudes (Lelieveld et al. 2002) are thought to be linked to the pollutants found in Asia, indicating the distant climate impacts of aerosols.

Impact of Idealized Stratospheric Aerosol Injection on the Future Ocean and Land Carbon Cycles

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Tjiputra, J.; Lauvset, S.

2017-12-01

Using a state-of-the-art Earth system model, we simulate stratospheric aerosol injection (SAI) on top of the Representative Concentration Pathways 8.5 future scenario. Our idealized method prescribes aerosol concentration, linearly increasing from 2020 to 2100, and thereafter remaining constant until 2200. In one of the scenarios, the model able to project future warming below 2 degree toward 2100, despite greatier warming persists in the high latitudes. When SAI is terminated in 2100, a rapid global warming of 0.35 K yr-1 (as compared to 0.05 K yr-1 under RCP8.5) is simulated in the subsequent 10 years, and the global mean temperature rapidly returns to levels close to the reference state. In contrast to earlier findings, we show a weak response in the terrestrial carbon sink during SAI implementation in the 21st century, which we attribute to nitrogen limitation. The SAI increases the land carbon uptake in the temperate forest-, grassland-, and shrub-dominated regions. The resultant lower temperatures lead to a reduction in the heterotrophic respiration rate and increase soil carbon retention. Changes in precipitation patterns are key drivers for variability in vegetation carbon. Upon SAI termination, the level of vegetation carbon storage returns to the reference case, whereas the soil carbon remains high. The ocean absorbs nearly 10% more carbon in the geoengineered simulation than in the reference simulation, leading to a ˜15 ppm lower atmospheric CO2 concentration in 2100. The largest enhancement in uptake occurs in the North Atlantic. In both hemispheres' polar regions, SAI delays the sea ice melting and, consequently, export production remains low. Despite inducing little impact on surface acidification, in the deep water of North Atlantic, SAI-induced circulation changes accelerate the ocean acidification rate and broaden the affected area. Since the deep ocean provides vital ecosystem function and services, e.g., fish stocks, this accelerated changes

Pinatubo Emulation in Multiple Models (POEMs): co-ordinated experiments in the ISA-MIP model intercomparison activity component of the SPARC Stratospheric Sulphur and it's Role in Climate initiative (SSiRC)

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Lee, Lindsay; Mann, Graham; Carslaw, Ken; Toohey, Matthew; Aquila, Valentina

2016-04-01

The World Climate Research Program's SPARC initiative has a new international activity "Stratospheric Sulphur and its Role in Climate" (SSiRC) to better understand changes in stratospheric aerosol and precursor gaseous sulphur species. One component of SSiRC involves an intercomparison "ISA-MIP" of composition-climate models that simulate the stratospheric aerosol layer interactively. Within PoEMS each modelling group will run a "perturbed physics ensemble" (PPE) of interactive stratospheric aerosol (ISA) simulations of the Pinatubo eruption, varying several uncertain parameters associated with the eruption's SO2 emissions and model processes. A powerful new technique to quantify and attribute sources of uncertainty in complex global models is described by Lee et al. (2011, ACP). The analysis uses Gaussian emulation to derive a probability density function (pdf) of predicted quantities, essentially interpolating the PPE results in multi-dimensional parameter space. Once trained on the ensemble, a Monte Carlo simulation with the fast Gaussian emulator enabling a full variance-based sensitivity analysis. The approach has already been used effectively by Carslaw et al., (2013, Nature) to quantify the uncertainty in the cloud albedo effect forcing from a 3D global aerosol-microphysics model allowing to compare the sensitivy of different predicted quantities to uncertainties in natural and anthropogenic emissions types, and structural parameters in the models. Within ISA-MIP, each group will carry out a PPE of runs, with the subsequent analysis with the emulator assessing the uncertainty in the volcanic forcings predicted by each model. In this poster presentation we will give an outline of the "PoEMS" analysis, describing the uncertain parameters to be varied and the relevance to further understanding differences identified in previous international stratospheric aerosol assessments.

Observations of the loss of stratospheric NO2 following volcanic eruptions

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Coffey, M. T.; Mankin, William G.

1993-01-01

Observations of stratospheric column amounts of nitrogen dioxide (NO2), nitric oxide (NO) and nitric acid (HNO3) have been made following major eruptions of the El Chichon and Mt. Pintatubo volcanoes. Midlatitude abundances of NO2 and NO were reduced by as much as 70% in the months following the appearance of the volcanic aerosols as compared to volcanically quite periods. There are heterogeneous reactions which could occur on the volcanic aerosols to convert NO2 into HNO3 but no commensurate increase in HNO3 column amounts was observed at the times of NO2 decrease.

Lifting options for stratospheric aerosol geoengineering: advantages of tethered balloon systems.

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Davidson, Peter; Burgoyne, Chris; Hunt, Hugh; Causier, Matt

2012-09-13

The Royal Society report 'Geoengineering the Climate' identified solar radiation management using albedo-enhancing aerosols injected into the stratosphere as the most affordable and effective option for geoengineering, but did not consider in any detail the options for delivery. This paper provides outline engineering analyses of the options, both for batch-delivery processes, following up on previous work for artillery shells, missiles, aircraft and free-flying balloons, as well as a more lengthy analysis of continuous-delivery systems that require a pipe connected to the ground and supported at a height of 20 km, either by a tower or by a tethered balloon. Towers are shown not to be practical, but a tethered balloon delivery system, with high-pressure pumping, appears to have much lower operating and capital costs than all other delivery options. Instead of transporting sulphuric acid mist precursors, such a system could also be used to transport slurries of high refractive index particles such as coated titanium dioxide. The use of such particles would allow useful experiments on opacity, coagulation and atmospheric chemistry at modest rates so as not to perturb regional or global climatic conditions, thus reducing scale-up risks. Criteria for particle choice are discussed, including the need to minimize or prevent ozone destruction. The paper estimates the time scales and relatively modest costs required if a tethered balloon system were to be introduced in a measured way with testing and development work proceeding over three decades, rather than in an emergency. The manufacture of a tether capable of sustaining the high tensions and internal pressures needed, as well as strong winds, is a significant challenge, as is the development of the necessary pumping and dispersion technologies. The greatest challenge may be the manufacture and launch of very large balloons, but means have been identified to significantly reduce the size of such balloons or aerostats.

Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

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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.

Environmental Temperature Effect on the Far-Infrared Absorption Features of Aromatic-Based Titan's Aerosol Analogs

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Gautier, Thomas; Trainer, Melissa G.; Loeffler, Mark J.; Sebree, Joshua A.; Anderson, Carrie M.

2016-01-01

Benzene detection has been reported in Titans atmosphere both in the stratosphere at ppb levels by remote sensing and in the thermosphere at ppm levels by the Cassini's Ion and Neutral Mass Spectrometer. This detection supports the idea that aromatic and heteroaromatic reaction pathways may play an important role in Titans atmospheric chemistry, especially in the formation of aerosols. Indeed, aromatic molecules are easily dissociated by ultraviolet radiation and can therefore contribute significantly to aerosol formation. It has been shown recently that aerosol analogs produced from a gas mixture containing a low concentration of aromatic and/or heteroaromatic molecules (benzene, naphthalene, pyridine, quinoline and isoquinoline) have spectral signatures below 500/cm, a first step towards reproducing the aerosol spectral features observed by Cassini's Composite InfraRed Spectrometer (CIRS) in the far infrared. In this work we investigate the influence of environmental temperature on the absorption spectra of such aerosol samples, simulating the temperature range to which aerosols, once formed, are exposed during their transport through Titans stratosphere. Our results show that environmental temperature does not have any major effect on the spectral shape of these aerosol analogs in the far-infrared, which is consistent with the CIRS observations.

Sulfate Aerosol in the Arctic: Source Attribution and Radiative Forcing

Energy Technology Data Exchange (ETDEWEB)

Yang, Yang [Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Wang, Hailong [Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Smith, Steven J. [Joint Global Change Research Institute, Pacific Northwest National Laboratory, College Park MD USA; Easter, Richard C. [Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA; Rasch, Philip J. [Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland WA USA

2018-02-08

Source attributions of Arctic sulfate and its direct radiative effect for 2010–2014 are quantified in this study using the Community Earth System Model (CESM) equipped with an explicit sulfur source-tagging technique. Regions that have high emissions and/or are near/within the Arctic present relatively large contributions to Arctic sulfate burden, with the largest contribution from sources in East Asia (27%). East Asia and South Asia together have the largest contributions to Arctic sulfate concentrations at 9–12 km, whereas sources within or near the Arctic account largely below 2 km. For remote sources with strong emissions, their contributions to Arctic sulfate burden are primarily driven by meteorology, while contributions of sources within or near the Arctic are dominated by their emission strength. The sulfate direct radiative effect (DRE) is –0.080 W m-2 at the Arctic surface, offsetting the net warming effect from the combination of in-snow heating and DRE cooling from black carbon. East Asia, Arctic local and Russia/Belarus/Ukraine sources contribute –0.017, –0.016 and –0.014 W m-2, respectively, to Arctic sulfate DRE. A 20% reduction in anthropogenic SO2 emissions leads to a net increase of +0.013 W m-2 forcing at the Arctic surface. These results indicate that a joint reduction in BC emissions could prevent possible Arctic warming from future reductions in SO2 emissions. Sulfate DRE efficiency calculations suggest that short transport pathways together with meteorology favoring long sulfate lifetimes make certain sources more efficient in influencing the Arctic sulfate DRE.

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

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P. S. Bhattacharjee

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.

Effects of the Mt. Pinatubo eruption on the chemistry, radiative, and transport processes in the stratosphere

International Nuclear Information System (INIS)

Wuebbles, D.J.; Kinnison, D.E.; Grant, K.E.; Connell, P.S.

1992-09-01

Volcanic eruptions can significantly impact trace gas distribution in the upper troposphere and lower stratosphere. Massive eruptions, produce large quantities of SO 2 , H 2 O, chlorine compounds, and particulates. Modeling the effects of these impulsive increases in traces gases and comparing the results with observations from ground and satellite measurements provide unique opportunities to test current multi-dimensional chemical-radiative-transport models of the global atmosphere. Since these models are currently being used in assessment studies for future anthropogenic emissions of trace gases quantitative understanding of the accuracy of these models is essential. In this study, we have used observed data from the Stratospheric Aerosol and Gas Experiment II (SAGE II) aboard the Earth Radiation Budget Satellite (ERBS) to realistically represent both the time dependent change in aerosol surface area density and wavelength dependent extinction values from the Mt. Pinatubo Eruption. Increases in the aerosol loading increase the rate of important heterogeneous chemical reactions converting odd nitrogen in both ClONO 2 and N 2 O 5 to HNO 3 . Radiative effects of increases aerosol optical thickness include changes to net radiative heating rates and to actinic fluxes. Changes to heating rates will indirectly change chemical reaction rates via changes in atmospheric temperatures. changes in actinic fluxes will directly modify photodissociation rates

Antarctic aerosols - A review

Science.gov (United States)

Shaw, Glenn E.

1988-02-01

Tropospheric aerosols with the diameter range of half a micron reside in the atmosphere for tens of days and teleconnect Antarctica with other regions by transport that reaches planetary scales of distances; thus, the aerosol on the Antarctic ice represents 'memory modules' of events that took place at regions separated from Antarctica by tens of thousands of kilometers. In terms of aerosol mass, the aerosol species include insoluble crustal products (less than 5 percent), transported sea-salt residues (highly variable but averaging about 10 percent), Ni-rich meteoric material, and anomalously enriched material with an unknown origin. Most (70-90 percent by mass) of the aerosol over the Antarctic ice shield, however, is the 'natural acid sulfate aerosol', apparently deriving from biological processes taking place in the surrounding oceans.

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.

Model simulations of the chemical and aerosol microphysical evolution of the Sarychev Peak 2009 eruption cloud compared to in situ and satellite observations

Science.gov (United States)

Lurton, Thibaut; Jégou, Fabrice; Berthet, Gwenaël; Renard, Jean-Baptiste; Clarisse, Lieven; Schmidt, Anja; Brogniez, Colette; Roberts, Tjarda J.

2018-03-01

Volcanic eruptions impact climate through the injection of sulfur dioxide (SO2), which is oxidized to form sulfuric acid aerosol particles that can enhance the stratospheric aerosol optical depth (SAOD). Besides large-magnitude eruptions, moderate-magnitude eruptions such as Kasatochi in 2008 and Sarychev Peak in 2009 can have a significant impact on stratospheric aerosol and hence climate. However, uncertainties remain in quantifying the atmospheric and climatic impacts of the 2009 Sarychev Peak eruption due to limitations in previous model representations of volcanic aerosol microphysics and particle size, whilst biases have been identified in satellite estimates of post-eruption SAOD. In addition, the 2009 Sarychev Peak eruption co-injected hydrogen chloride (HCl) alongside SO2, whose potential stratospheric chemistry impacts have not been investigated to date. We present a study of the stratospheric SO2-particle-HCl processing and impacts following Sarychev Peak eruption, using the Community Earth System Model version 1.0 (CESM1) Whole Atmosphere Community Climate Model (WACCM) - Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics model (with no a priori assumption on particle size). The Sarychev Peak 2009 eruption injected 0.9 Tg of SO2 into the upper troposphere and lower stratosphere (UTLS), enhancing the aerosol load in the Northern Hemisphere. The post-eruption evolution of the volcanic SO2 in space and time are well reproduced by the model when compared to Infrared Atmospheric Sounding Interferometer (IASI) satellite data. Co-injection of 27 Gg HCl causes a lengthening of the SO2 lifetime and a slight delay in the formation of aerosols, and acts to enhance the destruction of stratospheric ozone and mono-nitrogen oxides (NOx) compared to the simulation with volcanic SO2 only. We therefore highlight the need to account for volcanic halogen chemistry when simulating the impact of eruptions such as Sarychev on

Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

Science.gov (United States)

Lohmann, U.; Hoose, C.

2009-11-01

Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m-2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

Tethered balloon-borne aerosol measurements: seasonal and vertical variations of aerosol constituents over Syowa Station, Antarctica

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K. Hara

2013-09-01

Full Text Available Tethered balloon-borne aerosol measurements were conducted at Syowa Station, Antarctica, during the 46th Japanese Antarctic expedition (2005–2006. Direct aerosol sampling was operated from near the surface to the lower free troposphere (approximately 2500 m using a balloon-borne aerosol impactor. Individual aerosol particles were analyzed using a scanning electron microscope equipped with an energy dispersive X-ray spectrometer. Seasonal and vertical features of aerosol constituents and their mixing states were investigated. Results show that sulfate particles were predominant in the boundary layer and lower free troposphere in summer, whereas sea-salt particles were predominant during winter through spring. Minerals, MgSO4, and sulfate containing K were identified as minor aerosol constituents in both boundary layer and free troposphere over Syowa Station. Although sea-salt particles were predominant during winter through spring, the relative abundance of sulfate particles increased in the boundary layer when air masses fell from the free troposphere over the Antarctic coast and continent. Sea-salt particles were modified considerably through heterogeneous reactions with SO42− CH3SO3− and their precursors during summer, and were modified slightly through heterogeneous reactions with NO3− and its precursors. During winter through spring, sea-salt modification was insignificant, particularly in the cases of high relative abundance of sea-salt particles and higher number concentrations. In August, NO3− and its precursors contributed greatly to sea-salt modification over Syowa Station. Because of the occurrence of sea-salt fractionation on sea ice, Mg-rich sea-salt particles were identified during the months of April through November. In contrast, Mg-free sea-salt particles and slightly Mg-rich sea-salt particles coexisted in the lower troposphere during summer. Thereby, Mg separation can proceed by sea-salt fractionation during summer in

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China.

Science.gov (United States)

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Li, Lei

2018-02-01

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer (AMS) and Single Particle Aerosol Mass Spectrometer (SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2-1.0μm, accounting for over 97% of the total particles measured by both instruments. Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH 4 + was obtained by AMS, while extremely low value of NH 4 + was detected by SPAMS. Contrarily, high particle number counts of NO 3 - and Cl - were given by SPAMS while low concentrations of NO 3 - and Cl - were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments. Copyright © 2017. Published by Elsevier B.V.

The global warming potential of methane reassessed with combined stratosphere and troposphere chemistry

Science.gov (United States)

Holmes, C. D.; Archibald, A. T.; Eastham, S. D.; Søvde, O. A.

2017-12-01

Methane is a direct and indirect greenhouse gas. The direct greenhouse effect comes from the radiation absorbed and emitted by methane itself. The indirect greenhouse effect comes from radiatively active gases that are produced during methane oxidation: principally O3, H2O, and CO2. Methane also suppresses tropospheric OH, which indirectly affects numerous greenhouses gases and aerosols. Traditionally, the methane global warming potential (GWP) has included the indirect effects on tropospheric O3 and OH and stratospheric H2O, with these effects estimated independently from unrelated tropospheric and stratospheric chemistry models and observations. Using this approach the CH4 is about 28 over 100 yr (without carbon cycle feedbacks, IPCC, 2013). Here we present a comprehensive analysis of the CH4 GWP in several 3-D global atmospheric models capable of simulating both tropospheric and stratospheric chemistry (GEOS-Chem, Oslo CTM3, UKCA). This enables us to include, for the first time, the indirect effects of CH4 on stratospheric O3 and stratosphere-troposphere coupling. We diagnose the GWP from paired simulations with and without a 5% perturbation to tropospheric CH4 concentrations. Including stratospheric chemistry nearly doubles the O3 contribution to CH4 GWP because of O3 production in the lower stratosphere and because CH4 inhibits Cl-catalyzed O3 loss in the upper stratosphere. In addition, stratosphere-troposphere coupling strengthens the chemical feedback on its own lifetime. In the stratosphere, this feedback operates by a CH4 perturbation thickening the stratospheric O3 layer, which impedes UV-driven OH production in the troposphere and prolongs the CH4 lifetime. We also quantify the impact of CH4-derived H2O on the stratospheric HOx cycles but these effects are small. Combining all of the above, these models suggest that the 100-yr GWP of CH4 is over 33.5, a 20% increase over the latest IPCC assessment.

Formation of aqueous-phase sulfate during the haze period in China: Kinetics and atmospheric implications

Science.gov (United States)

Zhang, Haijie; Chen, Shilu; Zhong, Jie; Zhang, Shaowen; Zhang, Yunhong; Zhang, Xiuhui; Li, Zesheng; Zeng, Xiao Cheng

2018-03-01

Sulfate is one of the most important components in the aerosol due to its key role in air pollution and global climate change. Recent work has suggested that reactive nitrogen chemistry in aqueous water can explain the missing source of sulfate in the aqueous water. Herein, we have mapped out the energy profile of the oxidization process of SO2 leading from NO2 and two feasible three-step mechanisms have been proposed. For the oxidation of HOSO2- and HSO3- by the dissolved NO2 in weakly acidic and neutral aerosol (pH ≤ 7), the main contribution to the missing sulfate production comes from the oxidation of HOSO2-. The whole process is a self-sustaining process. For the oxidation of SO32- in alkaline aerosol (pH > 7), the third step - decomposition step of H2O or hydrolysis of SO3 step which are two parallel processes are the rate-limiting steps. The present results are of avail to better understand the missing source of sulfate in the aerosol and hence may lead to better science-based solutions for resolving the severe haze problems in China.

Vacuum FTIR Observation on the Dynamic Hygroscopicity of Aerosols under Pulsed Relative Humidity.

Science.gov (United States)

Leng, Chun-Bo; Pang, Shu-Feng; Zhang, Yun; Cai, Chen; Liu, Yong; Zhang, Yun-Hong

2015-08-04

A novel approach based on a combination of a pulse RH controlling system and a rapid scan vacuum FTIR spectrometer (PRHCS-RSVFTIR) was utilized to investigate dynamic hygroscopicity of two atmospheric aerosols: ammonium sulfate ((NH4)2SO4) and magnesium sulfate (MgSO4). In this approach, rapid-scan infrared spectra of water vapor and aerosols were obtained to determine relative humidity (RH) in sample cell and hygroscopic property of aerosols with a subsecond time resolution. Heterogeneous nucleation rates of (NH4)2SO4 were, for the first time, measured under low RH conditions (nucleation kinetics of liquid aerosols.

Climate effects of anthropogenic sulfate: Simulations from a coupled chemistry/climate model

International Nuclear Information System (INIS)

Chuang, C.C.; Penner, J.E.; Taylor, K.E.; Walton, J.J.

1993-09-01

In this paper, we use a more comprehensive approach by coupling a climate model with a 3-D global chemistry model to investigate the forcing by anthropogenic aerosol sulfate. The chemistry model treats the global-scale transport, transformation, and removal of SO 2 , DMS and H 2 SO 4 species in the atmosphere. The mass concentration of anthropogenic sulfate from fossil fuel combustion and biomass burning is calculated in the chemistry model and provided to the climate model where it affects the shortwave radiation. We also investigate the effect, with cloud nucleation parameterized in terms of local aerosol number, sulfate mass concentration and updraft velocity. Our simulations indicate that anthropogenic sulfate may result in important increases in reflected solar radiation, which would mask locally the radiative forcing from increased greenhouse gases. Uncertainties in these results will be discussed

Impacts of Four SO2 Oxidation Pathways on Wintertime Sulfate Concentrations

Science.gov (United States)

Sarwar, G.; Fahey, K.; Zhang, Y.; Kang, D.; Mathur, R.; Xing, J.; Wei, C.; Cheng, Y.

2017-12-01

Air quality models tend to under-estimate winter-time sulfate concentrations compared to observed data. Such under-estimations are particularly acute in China where very high concentrations of sulfate have been measured. Sulfate is produced by oxidation of sulfur dioxide (SO2) in gas-phase by hydroxyl radical and in aqueous-phase by hydrogen peroxide, ozone, etc. and most air quality models employ such typical reactions. Several additional SO2 oxidation pathways have recently been proposed. Heterogeneous reaction on dust has been suggested to be an important sink for SO2. Oxidation of SO2 on fine particles in presence of nitrogen dioxide (NO2) and ammonia (NH3) at high relative humidity has been implicated for sulfate formation in Chinese haze and London fog. Reactive nitrogen chemistry in aerosol water has also been suggested to produce winter-time sulfate in China. Specifically, high aerosol water can trap SO2 which can be subsequently oxidized by NO2 to form sulfate. Aqueous-phase (in-cloud) oxidation of SO2 by NO2 can also produce sulfate. Here, we use the hemispheric Community Multiscale Air Quality (CMAQ) modeling system to examine the potential impacts of these SO2 oxidation pathways on sulfate formation. We use anthropogenic emissions from the Emissions Database for Global Atmospheric Research and biogenic emissions from Global Emissions InitiAtive. We performed simulations without and with these SO2 oxidation pathways for October-December of 2014 using meteorological fields obtained from the Weather Research and Forecasting model. The standard CMAQ model contains one gas-phase chemical reaction and five aqueous-phase chemical reactions for SO2 oxidation. We implement four additional SO2 oxidation pathways into the CMAQ model. Our preliminary results suggest that the dust chemistry enhances mean sulfate over parts of China and Middle-East, the in-cloud SO2 oxidation by NO2 enhances sulfate over parts of western Europe, oxidation of SO2 by NO2 and NH3 on

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

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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.

Unexpected variations in the triple oxygen isotope composition of stratospheric carbon dioxide

Science.gov (United States)

Wiegel, Aaron A.; Cole, Amanda S.; Hoag, Katherine J.; Atlas, Elliot L.; Schauffler, Sue M.; Boering, Kristie A.

2013-10-01

We report observations of stratospheric CO2 that reveal surprisingly large anomalous enrichments in 17O that vary systematically with latitude, altitude, and season. The triple isotope slopes reached 1.95 ± 0.05(1σ) in the middle stratosphere and 2.22 ± 0.07 in the Arctic vortex versus 1.71 ± 0.03 from previous observations and a remarkable factor of 4 larger than the mass-dependent value of 0.52. Kinetics modeling of laboratory measurements of photochemical ozone-CO2 isotope exchange demonstrates that non-mass-dependent isotope effects in ozone formation alone quantitatively account for the 17O anomaly in CO2 in the laboratory, resolving long-standing discrepancies between models and laboratory measurements. Model sensitivities to hypothetical mass-dependent isotope effects in reactions involving O3, O(1D), or CO2 and to an empirically derived temperature dependence of the anomalous kinetic isotope effects in ozone formation then provide a conceptual framework for understanding the differences in the isotopic composition and the triple isotope slopes between the laboratory and the stratosphere and between different regions of the stratosphere. This understanding in turn provides a firmer foundation for the diverse biogeochemical and paleoclimate applications of 17O anomalies in tropospheric CO2, O2, mineral sulfates, and fossil bones and teeth, which all derive from stratospheric CO2.

Model simulations of the chemical and aerosol microphysical evolution of the Sarychev Peak 2009 eruption cloud compared to in situ and satellite observations

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T. Lurton

2018-03-01

Full Text Available Volcanic eruptions impact climate through the injection of sulfur dioxide (SO2, which is oxidized to form sulfuric acid aerosol particles that can enhance the stratospheric aerosol optical depth (SAOD. Besides large-magnitude eruptions, moderate-magnitude eruptions such as Kasatochi in 2008 and Sarychev Peak in 2009 can have a significant impact on stratospheric aerosol and hence climate. However, uncertainties remain in quantifying the atmospheric and climatic impacts of the 2009 Sarychev Peak eruption due to limitations in previous model representations of volcanic aerosol microphysics and particle size, whilst biases have been identified in satellite estimates of post-eruption SAOD. In addition, the 2009 Sarychev Peak eruption co-injected hydrogen chloride (HCl alongside SO2, whose potential stratospheric chemistry impacts have not been investigated to date. We present a study of the stratospheric SO2–particle–HCl processing and impacts following Sarychev Peak eruption, using the Community Earth System Model version 1.0 (CESM1 Whole Atmosphere Community Climate Model (WACCM – Community Aerosol and Radiation Model for Atmospheres (CARMA sectional aerosol microphysics model (with no a priori assumption on particle size. The Sarychev Peak 2009 eruption injected 0.9 Tg of SO2 into the upper troposphere and lower stratosphere (UTLS, enhancing the aerosol load in the Northern Hemisphere. The post-eruption evolution of the volcanic SO2 in space and time are well reproduced by the model when compared to Infrared Atmospheric Sounding Interferometer (IASI satellite data. Co-injection of 27 Gg HCl causes a lengthening of the SO2 lifetime and a slight delay in the formation of aerosols, and acts to enhance the destruction of stratospheric ozone and mono-nitrogen oxides (NOx compared to the simulation with volcanic SO2 only. We therefore highlight the need to account for volcanic halogen chemistry when simulating the impact of eruptions

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.

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.

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

KAUST Repository

Weil, Martin; Grassl, Hartmut; Hoshyaripour, Gholamali; Kloster, Silvia; Kominek, Jasmin; Misios, Stergios; Scheffran, Juergen; Starr, Steven; Stenchikov, Georgiy L.; Sudarchikova, Natalia; Timmreck, Claudia; Zhang, Dan; Kalinowski, Martin

2012-01-01

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.

On the detection of the solar signal in the tropical stratosphere

Directory of Open Access Journals (Sweden)

G. Chiodo

2014-06-01

Full Text Available We investigate the relative role of volcanic eruptions, El Niño–Southern Oscillation (ENSO, and the quasi-biennial oscillation (QBO in the quasi-decadal signal in the tropical stratosphere with regard to temperature and ozone commonly attributed to the 11 \\unit{yr} solar cycle. For this purpose, we perform transient simulations with the Whole Atmosphere Community Climate Model forced from 1960 to 2004 with an 11 yr solar cycle in irradiance and different combinations of other forcings. An improved multiple linear regression technique is used to diagnose the 11 yr solar signal in the simulations. One set of simulations includes all observed forcings, and is thereby aimed at closely reproducing observations. Three idealized sets exclude ENSO variability, volcanic aerosol forcing, and QBO in tropical stratospheric winds, respectively. Differences in the derived solar response in the tropical stratosphere in the four sets quantify the impact of ENSO, volcanic events and the QBO in attributing quasi-decadal changes to the solar cycle in the model simulations. The novel regression approach shows that most of the apparent solar-induced lower-stratospheric temperature and ozone increase diagnosed in the simulations with all observed forcings is due to two major volcanic eruptions (i.e., El Chichón in 1982 and Mt. Pinatubo in 1991. This is caused by the alignment of these eruptions with periods of high solar activity. While it is feasible to detect a robust solar signal in the middle and upper tropical stratosphere, this is not the case in the tropical lower stratosphere, at least in a 45 yr simulation. The present results suggest that in the tropical lower stratosphere, the portion of decadal variability that can be unambiguously linked to the solar cycle may be smaller than previously thought.

Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

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C. Hoose

2009-11-01

Full Text Available Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO₄-crit, which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m⁻². This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.

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.;

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

Science.gov (United States)

Sareen, N.; McNeill, V. F.

2011-12-01

In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

Effects of the Mt. Pinatubo eruption on the radiative and chemical processes in the troposphere and stratosphere

International Nuclear Information System (INIS)

Kinnison, D.E.; Grant, K.E.; Connell, P.S.; Wuebbles, D.J.

1992-01-01

The LLNL 2-D zonally averaged chemical-radiative transport model of the global atmosphere was used to study the effects of the June 15, 1991 eruption of the Mt. Pinatubo volcano on stratospheric processes. SAGE-11 time-dependent aerosol surface area density and optical extinction data were used as input into the model. By the winter solstice, 1991, a maximum change in column ozone was observed in the equatorial region of -2% (with heterogeneous chemical reactions on sulfuric acid aerosols) and -5.5% (including heterogeneous reactions plus radiative feedbacks). Maximum local ozone decreases of 12% were derived in the equatorial region, at 25 km, for winter solstice 1991. Column NO 2 peaked (-14%) at 30 S in October 1991. Local concentrations of NO x , Cl x , and HO x , in the lower stratosphere, were calculated to have changed between 30 S and 30 N by -40%, +80%, and +60% respectively

Aerosol Climate Time Series Evaluation In ESA Aerosol_cci

Science.gov (United States)

Popp, T.; de Leeuw, G.; Pinnock, S.

2015-12-01

Within the ESA Climate Change Initiative (CCI) Aerosol_cci (2010 - 2017) conducts intensive work to improve algorithms for the retrieval of aerosol information from European sensors. By the end of 2015 full mission time series of 2 GCOS-required aerosol parameters are completely validated and released: Aerosol Optical Depth (AOD) from dual view ATSR-2 / AATSR radiometers (3 algorithms, 1995 - 2012), and stratospheric extinction profiles from star occultation GOMOS spectrometer (2002 - 2012). Additionally, a 35-year multi-sensor time series of the qualitative Absorbing Aerosol Index (AAI) together with sensitivity information and an AAI model simulator is available. Complementary aerosol properties requested by GCOS are in a "round robin" phase, where various algorithms are inter-compared: fine mode AOD, mineral dust AOD (from the thermal IASI spectrometer), absorption information and aerosol layer height. As a quasi-reference for validation in few selected regions with sparse ground-based observations the multi-pixel GRASP algorithm for the POLDER instrument is used. Validation of first dataset versions (vs. AERONET, MAN) and inter-comparison to other satellite datasets (MODIS, MISR, SeaWIFS) proved the high quality of the available datasets comparable to other satellite retrievals and revealed needs for algorithm improvement (for example for higher AOD values) which were taken into account for a reprocessing. The datasets contain pixel level uncertainty estimates which are also validated. The paper will summarize and discuss the results of major reprocessing and validation conducted in 2015. The focus will be on the ATSR, GOMOS and IASI datasets. Pixel level uncertainties validation will be summarized and discussed including unknown components and their potential usefulness and limitations. Opportunities for time series extension with successor instruments of the Sentinel family will be described and the complementarity of the different satellite aerosol products

Observations of reduced ozone concentrations in the tropical stratosphere after the eruption of Mt. Pinatubo

Science.gov (United States)

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

1992-01-01

Two independent sets of data, one of aerosols from an airborne lidar system, and one of ozone from ozonesonde measurements indicate that significant ozone decreases may have happened as a result of the injection of debris by the Mt. Pinatubo volcano in June 1991. The amount of this reduction maximizes at 24-25 km, near the peak of the aerosol distribution, though a deficit is seen throughout the lower stratosphere between 19 and 28 km. The greatest differences observed prior and subsequent to the eruptions at these altitudes is 18-20 percent.

Study of the behaviour of artificial radioactive aerosols. Applications to some problems of atmospheric circulation (1963)

International Nuclear Information System (INIS)

Lambert, G.

1963-11-01

The aim of this work, consists in the examination of the behaviour of radioactive aerosols produced in the atmosphere by nuclear explosions, in order to deduce the most general laws governing atmospheric circulation and diffusion. After having given a general table of the radioactive aerosols present the authors consider the validity and the precision of the measurement methods and the concentration of the aerosols at ground level and in the upper atmosphere, as well as their deposition on the ground. The existence is thus demonstrated of a tropospheric equatorial barrier and of discontinuous and seasonal aspects of stratosphere-troposphere transfers. The role is shown of precipitations and dry auto-filtration in the lower atmosphere cleaning processes. This work makes it possible to describe the general behaviour of dust from the stratosphere, and to improve the total radioactive contamination of the globe. (author) [fr

Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

Science.gov (United States)

Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

2018-04-01

In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude. The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires. In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and

Is Distant Pollution Contaminating Local Air? Analyzing the Origins of Atmospheric Aerosols

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David Geng

2012-01-01

Full Text Available Understanding the origin of aerosols in the atmosphere is important because of visual pollution, climate impacts, and deleterious health effects due to the inhalation of fine particles. This research analyzed aerosols characterized by their chloride, sulfate, and nitrate content as a function of size over a 3-month period. Due to wind patterns over coal-burning power plants, a higher concentration of local sulfate pollution was expected. Aerosols were harvested on the Purdue University campus using a high-volume air sampler with glass fiber filters and a five-stage impactor that separates the aerosols into five sizes. The filters were extracted in water to dissolve anions and the solution was analyzed using high-pressure liquid ion chromatography. Only trace amounts of chloride with no distinct patterns in size were detected. In total, nitrate content ranged from 0.12 to 2.10 μg/m3 and sulfate content ranged from 0.44 to 6.45 μg/m3 over a 3-month period. As for fine particles, a higher concentration of sulfate was observed. The Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT model determines air mass origin, and in this study, higher total sulfate content was observed when the air mass moved out of the southwest, and higher total nitrate content was observed when the air mass originated from the southeast. The author concluded that small particles resulted in sulfate from sulfur dioxide, typically from gas to particle conversion. High sulfur dioxide levels are directly correlated with coal-burning power plant density. Small particulate sulfate found in West Lafayette, Indiana, was determined to originate primarily from power plants in southwest Indiana. Though the results do show a significant amount of potentially harmful aerosols in West Lafayette, there is still further research to be done concerning isotopic composition of those particles in attempts to better explain the chemical pathways.

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

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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

Study of the behaviour of artificial radioactive aerosols. Applications to some problems of atmospheric circulation (1963); Etude du comportement dcs aerosols radioactifs artificiels. Applications a quelques problemes de circulation atmospherique (1963)

Energy Technology Data Exchange (ETDEWEB)

Lambert, G [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1963-11-15

The aim of this work, consists in the examination of the behaviour of radioactive aerosols produced in the atmosphere by nuclear explosions, in order to deduce the most general laws governing atmospheric circulation and diffusion. After having given a general table of the radioactive aerosols present the authors consider the validity and the precision of the measurement methods and the concentration of the aerosols at ground level and in the upper atmosphere, as well as their deposition on the ground. The existence is thus demonstrated of a tropospheric equatorial barrier and of discontinuous and seasonal aspects of stratosphere-troposphere transfers. The role is shown of precipitations and dry auto-filtration in the lower atmosphere cleaning processes. This work makes it possible to describe the general behaviour of dust from the stratosphere, and to improve the total radioactive contamination of the globe. (author) [French] L'objectif de ce travail consiste a examiner le comportement des aerosols radioactifs introduits dans l'atmosphere par les explosions nucleaires, pour en deduire les lois les plus generals de la circulation et diffusion atmospheriques. Apres avoir dresse un tableau d'ensemble des aerosols radioactifs presents, on examine la validite et la precision des methodes de mesure de leur concentration, au niveau du sol et en haute atmosphere, ainsi que de leur depot a la surface du sol. On met ainsi en evidence l'existence d'une barriere equatoriale tropospherique; l'aspect discontinu et saisonnier des transferts stratosphere-troposphere; le role des precipitations et de l'auto-filtration seche, dans les processus de nettoyage de la basse atmosphere. Ces etudes permettent de decrire le comportement general des poussieres d'origine stratospherique et d'ameliorer le bilan de la contamination radioactive du globe. (auteur)

Study of the behaviour of artificial radioactive aerosols. Applications to some problems of atmospheric circulation (1963); Etude du comportement dcs aerosols radioactifs artificiels. Applications a quelques problemes de circulation atmospherique (1963)

Energy Technology Data Exchange (ETDEWEB)

Lambert, G. [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1963-11-15

The aim of this work, consists in the examination of the behaviour of radioactive aerosols produced in the atmosphere by nuclear explosions, in order to deduce the most general laws governing atmospheric circulation and diffusion. After having given a general table of the radioactive aerosols present the authors consider the validity and the precision of the measurement methods and the concentration of the aerosols at ground level and in the upper atmosphere, as well as their deposition on the ground. The existence is thus demonstrated of a tropospheric equatorial barrier and of discontinuous and seasonal aspects of stratosphere-troposphere transfers. The role is shown of precipitations and dry auto-filtration in the lower atmosphere cleaning processes. This work makes it possible to describe the general behaviour of dust from the stratosphere, and to improve the total radioactive contamination of the globe. (author) [French] L'objectif de ce travail consiste a examiner le comportement des aerosols radioactifs introduits dans l'atmosphere par les explosions nucleaires, pour en deduire les lois les plus generals de la circulation et diffusion atmospheriques. Apres avoir dresse un tableau d'ensemble des aerosols radioactifs presents, on examine la validite et la precision des methodes de mesure de leur concentration, au niveau du sol et en haute atmosphere, ainsi que de leur depot a la surface du sol. On met ainsi en evidence l'existence d'une barriere equatoriale tropospherique; l'aspect discontinu et saisonnier des transferts stratosphere-troposphere; le role des precipitations et de l'auto-filtration seche, dans les processus de nettoyage de la basse atmosphere. Ces etudes permettent de decrire le comportement general des poussieres d'origine stratospherique et d'ameliorer le bilan de la contamination radioactive du globe. (auteur)

Modelling of Aerosol Chemistry and Transport over Europe and Comparison with Measurements

NARCIS (Netherlands)

Jeuken, A.; Veefkind, J.P.; Metzger, S.; Denter, F.; Velthoven, P.

1999-01-01

Because of the short lifetime of aerosols (days-weeks), the radiative forcing associated with aerosols varies strongly spatially and temporally (see van Dorland et al., poster) Current measurement networks of sulfate and other aerosol species are unable to provide a representative picture of the

Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

Science.gov (United States)

Kaul, D. S.; Gupta, T.; Tripathi, S. N.

2012-06-01

An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

Evolution of Asian aerosols during transpacific transport in INTEX-B

Energy Technology Data Exchange (ETDEWEB)

Dunlea, E. J.; DeCarlo, Peter; Aiken, Allison; Kimmel, Joel; Peltier, R. E.; Weber, R. J.; Tomlinson, Jason M.; Collins, Donald R.; Shinozuka, Yohei; McNaughton, C. S.; Howell, S. G.; Clarke, A. D.; Emmons, L.; Apel, Eric; Pfister, G. G.; van Donkelaar, A.; Martin, R. V.; Millet, D. B.; Heald, C. L.; Jimenez, J. L.

2009-10-01

Measurements of aerosol composition were made with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) on board the NSF/NCAR C-130 aircraft as part of the Intercontinental Chemical Transport Experiment Phase B 5 (INTEX-B) field campaign over the Eastern Pacific Ocean. The HR-ToF-AMS measurements of non-refractory submicron aerosol mass are shown to compare well with other aerosol instrumentation in the INTEX-B field study. Two case studies are described for pollution layers transported across the Pacific from the Asian continent, intercepted 3–4 days and 7–10 days downwind of Asia, respectively. Aerosol chemistry is shown to 10 be a robust tracer for air masses originating in Asia, specifically the presence of sulfate dominated aerosol is a distinguishing feature of Asian pollution layers that have been transported to the Eastern Pacific. We examine the time scales of processing for sulfate and organic aerosol in the atmosphere and show that our observations confirm a conceptual model for transpacific transport from Asia proposed by Brock et al. (2004). 15 Our observations of both sulfate and organic aerosol in aged Asian pollution layers are consistent with fast formation near the Asian continent, followed by washout during lofting and subsequent transformation during transport across the Pacific. Our observations are the first atmospheric measurements to indicate that although secondary organic aerosol (SOA) formation from pollution happens on the timescale of one day, 20 the oxidation of organic aerosol continues at longer timescales in the atmosphere. Comparisons with chemical transport models of data from the entire campaign reveal an under-prediction of SOA mass in the MOZART model, but much smaller discrepancies with the GEOS-Chem model than found in previous studies over the Western Pacific. No evidence is found to support a previous hypothesis for significant secondary 25 organic aerosol formation in the free troposphere.

On the aliasing of the solar cycle in the lower stratospheric tropical temperature

Science.gov (United States)

Kuchar, Ales; Ball, William T.; Rozanov, Eugene V.; Stenke, Andrea; Revell, Laura; Miksovsky, Jiri; Pisoft, Petr; Peter, Thomas

2017-09-01

The double-peaked response of the tropical stratospheric temperature profile to the 11 year solar cycle (SC) has been well documented. However, there are concerns about the origin of the lower peak due to potential aliasing with volcanic eruptions or the El Niño-Southern Oscillation (ENSO) detected using multiple linear regression analysis. We confirm the aliasing using the results of the chemistry-climate model (CCM) SOCOLv3 obtained in the framework of the International Global Atmospheric Chemisty/Stratosphere-troposphere Processes And their Role in Climate Chemistry-Climate Model Initiative phase 1. We further show that even without major volcanic eruptions included in transient simulations, the lower stratospheric response exhibits a residual peak when historical sea surface temperatures (SSTs)/sea ice coverage (SIC) are used. Only the use of climatological SSTs/SICs in addition to background stratospheric aerosols removes volcanic and ENSO signals and results in an almost complete disappearance of the modeled solar signal in the lower stratospheric temperature. We demonstrate that the choice of temporal subperiod considered for the regression analysis has a large impact on the estimated profile signal in the lower stratosphere: at least 45 consecutive years are needed to avoid the large aliasing effect of SC maxima with volcanic eruptions in 1982 and 1991 in historical simulations, reanalyses, and observations. The application of volcanic forcing compiled for phase 6 of the Coupled Model Intercomparison Project (CMIP6) in the CCM SOCOLv3 reduces the warming overestimation in the tropical lower stratosphere and the volcanic aliasing of the temperature response to the SC, although it does not eliminate it completely.

Aerosol Climate Time Series in ESA Aerosol_cci

Science.gov (United States)

Popp, Thomas; de Leeuw, Gerrit; Pinnock, Simon

2016-04-01

Within the ESA Climate Change Initiative (CCI) Aerosol_cci (2010 - 2017) conducts intensive work to improve algorithms for the retrieval of aerosol information from European sensors. Meanwhile, full mission time series of 2 GCOS-required aerosol parameters are completely validated and released: Aerosol Optical Depth (AOD) from dual view ATSR-2 / AATSR radiometers (3 algorithms, 1995 - 2012), and stratospheric extinction profiles from star occultation GOMOS spectrometer (2002 - 2012). Additionally, a 35-year multi-sensor time series of the qualitative Absorbing Aerosol Index (AAI) together with sensitivity information and an AAI model simulator is available. Complementary aerosol properties requested by GCOS are in a "round robin" phase, where various algorithms are inter-compared: fine mode AOD, mineral dust AOD (from the thermal IASI spectrometer, but also from ATSR instruments and the POLDER sensor), absorption information and aerosol layer height. As a quasi-reference for validation in few selected regions with sparse ground-based observations the multi-pixel GRASP algorithm for the POLDER instrument is used. Validation of first dataset versions (vs. AERONET, MAN) and inter-comparison to other satellite datasets (MODIS, MISR, SeaWIFS) proved the high quality of the available datasets comparable to other satellite retrievals and revealed needs for algorithm improvement (for example for higher AOD values) which were taken into account for a reprocessing. The datasets contain pixel level uncertainty estimates which were also validated and improved in the reprocessing. For the three ATSR algorithms the use of an ensemble method was tested. The paper will summarize and discuss the status of dataset reprocessing and validation. The focus will be on the ATSR, GOMOS and IASI datasets. Pixel level uncertainties validation will be summarized and discussed including unknown components and their potential usefulness and limitations. Opportunities for time series extension

Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate

Science.gov (United States)

Chung Kwong, Kai; Chim, Man Mei; Davies, James F.; Wilson, Kevin R.; Nin Chan, Man

2018-02-01

Organosulfates are important organosulfur compounds present in atmospheric particles. While the abundance, composition, and formation mechanisms of organosulfates have been extensively investigated, it remains unclear how they transform and evolve throughout their atmospheric lifetime. To acquire a fundamental understanding of how organosulfates chemically transform in the atmosphere, this work investigates the heterogeneous OH radical-initiated oxidation of sodium methyl sulfate (CH3SO4Na) droplets, the smallest organosulfate detected in atmospheric particles, using an aerosol flow tube reactor at a high relative humidity (RH) of 85 %. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (direct analysis in real time, DART) coupled with a high-resolution mass spectrometer showed that neither functionalization nor fragmentation products are detected. Instead, the ion signal intensity of the bisulfate ion (HSO4-) has been found to increase significantly after OH oxidation. We postulate that sodium methyl sulfate tends to fragment into a formaldehyde (CH2O) and a sulfate radical anion (SO4 ṡ -) upon OH oxidation. The formaldehyde is likely partitioned back to the gas phase due to its high volatility. The sulfate radical anion, similar to OH radical, can abstract a hydrogen atom from neighboring sodium methyl sulfate to form the bisulfate ion, contributing to the secondary chemistry. Kinetic measurements show that the heterogeneous OH reaction rate constant, k, is (3.79 ± 0.19) × 10-13 cm3 molecule-1 s-1 with an effective OH uptake coefficient, γeff, of 0.17 ± 0.03. While about 40 % of sodium methyl sulfate is being oxidized at the maximum OH exposure (1.27 × 1012 molecule cm-3 s), only a 3 % decrease in particle diameter is observed. This can be attributed to a small fraction of particle mass lost via the formation and volatilization of formaldehyde. Overall, we firstly demonstrate that the heterogeneous OH oxidation of an

Stratospheric minor species vertical distributions during polar winter by balloon borne UV-Vis spectrometry

Science.gov (United States)

Pommereau, J. P.; Piquard, J.

1994-01-01

A light, relatively cheap and easy to operate balloonborne UV-visible spectrometer was designed for investigating ozone photochemistry in the Arctic winter. The instrument was flown 11 times during the European Arctic Stratospheric Ozone Experiment (EASOE) in winter 1991-92 in Northern Scandinavia. The first simultaneous measurements of vertical distributions of aerosols, PSC's, O3, NO2 and OClO inside the vortex during flight no. 6 on 16 January, in cold conditions are reported, which show that nitrogen oxides were almost absent (lower than 100 ppt) in the stratosphere below 22 km, while a layer of relatively large OClO concentration (15 ppt) was present at the altitude of the minimum temperature.

Is there an aerosol signature of aqueous processing?

Science.gov (United States)

Ervens, B.; Sorooshian, A.

2017-12-01

The formation of aerosol mass in cloud water has been recognized as a substantial source of atmospheric aerosol mass. While sulfate formation can be relatively well constrained, the formation of secondary organic aerosol mass in the aqueous phase (aqSOA) is much more complex due to the multitude of precursors and variety in chemical processes. Aqueous phase processing adds aerosol mass to the droplet mode, which is formed due to mass addition to activated particles in clouds. In addition, it has been shown that aqSOA mass has specific characteristics in terms of oxidation state and hygroscopicity that might help to distinguish it from other SOA sources. Many models do not include detailed chemical mechanisms of sulfate and aqSOA formation and also lack details on the mass distribution of newly formed mass. Mass addition inside and outside clouds modifies different parts of an aerosol population and consequently affects predictions of properties and lifetime of particles. Using a combination of field data analysis and model studies for a variety of air masses, we will show which chemical and physical aerosol properties can be used, in order to identify an `aqueous phase signature' in processed aerosol populations. We will discuss differences in this signature in clean (e.g., background), moderately polluted (e.g., urban) and highly polluted (e.g., biomass burning) air masses and suggest air-mass-specific chemical and/or physical properties that will help to quantify the aqueous-phase derived aerosol mass.

Modulations of stratospheric ozone by volcanic eruptions

Science.gov (United States)

Blanchette, Christian; Mcconnell, John C.

1994-01-01

We have used a time series of aerosol surface based on the measurements of Hofmann to investigate the modulation of total column ozone caused by the perturbation to gas phase chemistry by the reaction N2O5(gas) + H2O(aero) yields 2HNO3(gas) on the surface of stratospheric aerosols. We have tested a range of values for its reaction probability, gamma = 0.02, 0.13, and 0.26 which we compared to unperturbed homogeneous chemistry. Our analysis spans a period from Jan. 1974 to Oct. 1994. The results suggest that if lower values of gamma are the norm then we would expect larger ozone losses for highly enhanced aerosol content that for larger values of gamma. The ozone layer is more sensitive to the magnitude of the reaction probability under background conditions than during volcanically active periods. For most conditions, the conversion of NO2 to HNO3 is saturated for reaction probability in the range of laboratory measurements, but is only absolutely saturated following major volcanic eruptions when the heterogeneous loss dominates the losses of N2O5. The ozone loss due to this heterogeneous reaction increases with the increasing chlorine load. Total ozone losses calculated are comparable to ozone losses reported from TOMS and Dobson data.

The Asian Tropopause Aerosol Layer: Balloon-Borne Measurements, Satellite Observations and Modeling Approaches

Science.gov (United States)

Fairlie, T. D.; Vernier, J.-P.; Natarajan, M.; Deshler, Terry; Liu, H.; Wegner, T.; Baker, N.; Gadhavi, H.; Jayaraman, A.; Pandit, A.;

Refinements in the use of equivalent latitude for assimilating sporadic inhomogeneous stratospheric tracer observations, 1: Detecting transport of Pinatubo aerosol across a strong vortex edge

Directory of Open Access Journals (Sweden)

P. Good

2004-01-01

Full Text Available The use of PV equivalent latitude for assimilating stratospheric tracer observations is discussed - with particular regard to the errors in the equivalent latitude coordinate, and to the assimilation of sparse data. Some example measurements are assimilated: they sample the stratosphere sporadically and inhomogeneously. The aim was to obtain precise information about the isentropic tracer distribution and evolution as a function of equivalent latitude. Precision is important, if transport across barriers like the vortex edge are to be detected directly. The main challenges addressed are the errors in modelled equivalent latitude, and the non-ideal observational sampling. The methods presented allow first some assessment of equivalent latitude errors and a picture of how good or poor the observational coverage is. This information determines choices in the approach for estimating as precisely as possible the true equivalent latitude distribution of the tracer, in periods of good and poor observational coverage. This is in practice an optimisation process, since better understanding of the equivalent latitude distribution of the tracer feeds back into a clearer picture of the errors in the modelled equivalent latitude coordinate. Error estimates constrain the reliability of using equivalent latitude to make statements like 'this observation samples air poleward of the vortex edge' or that of more general model-measurement comparisons. The approach is demonstrated for ground-based lidar soundings of the Mount Pinatubo aerosol cloud, focusing on the 1991-92 arctic vortex edge between 475-520K. Equivalent latitude is estimated at the observation times and locations from Eulerian model tracers initialised with PV and forced by UK Meteorological Office analyses. With the model formulation chosen, it is shown that tracer transport of a few days resulted in an error distribution that was much closer to Gaussian form, although the mean error was not

Evaluation of simulated aerosol properties with the aerosol-climate model ECHAM5-HAM using observations from the IMPACT field campaign

Directory of Open Access Journals (Sweden)

G.-J. Roelofs

2010-08-01

Full Text Available In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the associated aerosol optical thickness (AOT for the campaign period. Synoptic scale meteorology is represented realistically through nudging of the vorticity, the divergence, the temperature and the surface pressure. Simulated concentrations of aerosol sulfate and organics at the surface are generally within a factor of two from observed values. The monthly averaged AOT from the model is 0.33, about 20% larger than observed. For selected periods of the month with relatively dry and moist conditions discrepancies are approximately −30% and +15%, respectively. Discrepancies during the dry period are partly caused by inaccurate representation of boundary layer (BL dynamics by the model affecting the simulated AOT. The model simulates too strong exchange between the BL and the free troposphere, resulting in weaker concentration gradients at the BL top than observed for aerosol and humidity, while upward mixing from the surface layers into the BL appears to be underestimated. The results indicate that beside aerosol sulfate and organics also aerosol ammonium and nitrate significantly contribute to aerosol water uptake. The simulated day-to-day variability of AOT follows synoptic scale advection of humidity rather than particle concentration. Even for relatively dry conditions AOT appears to be strongly influenced by the diurnal cycle of RH in the lower boundary layer, further enhanced by uptake and release of nitric acid and ammonia by aerosol water.

Organics, Meteoritic Material, and other Elements in High Altitude Aerosols

Science.gov (United States)

Mahoney, M.; Murphy, D. M.; Thomson, D. S.

1998-01-01

Recent in situ measurements of the chemical composition of single aerosol particles at altitudes up to 19 km have revealed a number of surprising features about ambient particles. Upper tropospheric aerosols in the study region often contained more organic material than sulfate.

Global source attribution of sulfate concentration and direct and indirect radiative forcing

Science.gov (United States)

Yang, Yang; Wang, Hailong; Smith, Steven J.; Easter, Richard; Ma, Po-Lun; Qian, Yun; Yu, Hongbin; Li, Can; Rasch, Philip J.

2017-07-01

The global source-receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF) from 16 regions/sectors for years 2010-2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggesting that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is -0.42 W m-2, with -0.31 W m-2 contributed by anthropogenic sulfate and -0.11 W m-2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17-84 % to the total DRF. East Asia has the largest contribution of 20-30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of -0.44 W m-2. DMS has the largest contribution, explaining -0.23 W m-2 of the global sulfate incremental IRF. Incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.

Sulfate cooling effects on climate through in-cloud oxidation of anthropogenic SO2

International Nuclear Information System (INIS)

Lelieveld, J.; Heintzenberg, J.

1992-01-01

Anthropogenic SO 2 emissions may exert a significant cooling effect on climate in the Northern Hemisphere through backscattering of solar radiation by sulfate particles. Earlier estimates of the sulfate climate forcing were based on a limited number of sulfate-scattering correlation measurements from which a high sulfate-scattering efficiency was derived. Model results suggest that cloud processing of air is the underlying mechanism. aqueous phase oxidation of SO 2 into sulfate and the subsequent release of the dry aerosol by cloud evaporation render sulfate a much more efficient scatterer than through gas-phase SO 2 oxidation

Aerosol quantification with the Aerodyne Aerosol Mass Spectrometer: detection limits and ionizer background effects

Directory of Open Access Journals (Sweden)

S. Borrmann

2009-02-01

Full Text Available Systematic laboratory experiments were performed to investigate quantification of various species with two versions of the Aerodyne Aerosol Mass Spectrometer, a Quadrupole Aerosol Mass Spectrometer (Q-AMS and a compact Time-of-Flight Aerosol Mass Spectrometer (c-ToF-AMS. Here we present a new method to continuously determine the detection limits of the AMS analyzers during regular measurements, yielding detection limit (DL information under various measurement conditions. Minimum detection limits range from 0.03 μg m⁻³ (nitrate, sulfate, and chloride up to 0.5 μg m⁻³ (organics for the Q-AMS. Those of the c-ToF-AMS are found between 0.003 μg m⁻³ (nitrate, sulfate and 0.03 μg m⁻³ (ammonium, organics. The DL values found for the c-ToF-AMS were ~10 times lower than those of the Q-AMS, mainly due to differences in ion duty cycle. Effects causing an increase of the detection limits include long-term instrument contamination, measurement of high aerosol mass concentrations and short-term instrument history. The self-cleaning processes which reduce the instrument background after measurement of large aerosol concentrations as well as the influences of increased instrument background on mass concentration measurements are discussed. Finally, improvement of detection limits by extension of averaging time intervals, selected or reduced ion monitoring, and variation of particle-to-background measurement ratio are investigated.

Field and Laboratory Studies of Atmospheric Organic Aerosol

Science.gov (United States)

Coggon, Matthew Mitchell

of oxidized organic compounds contributed nearly an order of magnitude more cloud condensation nuclei (CCN) than less oxidized particles formed under cloudy conditions. The processing time necessary for particles to become CCN active was short ( 4 hr). Laboratory chamber experiments were also conducted to evaluate particle-phase processes influencing aerosol phase and composition. In one study, ammonium sulfate seed was coated with a layer of secondary organic aerosol (SOA) from toluene oxidation followed by a layer of SOA from α-pinene oxidation. The system exhibited different evaporative properties than ammonium sulfate seed initially coated with α-pinene SOA followed by a layer of toluene SOA. This behavior is consistent with a shell-and-core model and suggests limited mixing among different SOA types. Another study investigated the reactive uptake of isoprene epoxy diols (IEPOX) onto non-acidified aerosol. It was demonstrated that particle acidity has limited influence on organic aerosol formation onto ammonium sulfate seed, and that the chemical system is limited by the availability of nucleophiles such as sulfate. Flow tube experiments were conducted to examine the role of iron in the reactive uptake and chemical oxidation of glycolaldehyde. Aerosol particles doped with iron and hydrogen peroxide were mixed with gas-phase glycolaldehyde and photochemically aged in a custom-built flow reactor. Compared to particles free of iron, iron-doped aerosols significantly enhanced the oxygen to carbon (O/C) ratio of accumulated organic mass. The primary oxidation mechanism is suggested to be a combination of Fenton and photo-Fenton reactions which enhance particle-phase OH radical concentrations.

Effects of cloudy/clear air mixing and droplet pH on sulfate aerosol formation in a coupled chemistry/climate global model

Energy Technology Data Exchange (ETDEWEB)

Molenkamp, C.R.; Atherton, C.A. [Lawrence Livermore National Lab., CA (United States); Penner, J.E.; Walton, J.J. [Michigan Univ., Ann Arbor, MI (United States). Dept. of Atmospheric, Oceanic and Space Sciences

1996-10-01

In this paper we will briefly describe our coupled ECHAM/GRANTOUR model, provide a detailed description of our atmospheric chemistry parameterizations, and discuss a couple of numerical experiments in which we explore the influence of assumed pH and rate of mixing between cloudy and clear air on aqueous sulfate formation and concentration. We have used our tropospheric chemistry and transport model, GRANTOUR, to estimate the life cycle and global distributions of many trace species. Recently, we have coupled GRANTOUR with the ECHAM global climate model, which provides several enhanced capabilities in the representation of aerosol interactions.

Geochemical, Sulfur Isotopic Characteristics and Source Contributions of Size-Aggregated Aerosols Collected in Baring Head, New Zealand.

Science.gov (United States)

Li, J.; Michalski, G. M.; Davy, P.; Harvey, M.; Wilkins, B. P.; Katzman, T. L.

2017-12-01

Sulfate aerosols are critical to the climate, human health, and the hydrological cycle in the atmosphere, yet the sources of sulfate in aerosols are not completely understood. In this work, we evaluated the sources of sulfate in size-aggregated aerosols from the Southern Pacific Ocean and the land of New Zealand using geochemical and isotopic analyses. Aerosols were collected at Baring Head, New Zealand between 6/30/15 to 8/4/16 using two collectors, one only collects Southern Pacific Ocean derived aerosols (open-ocean collector), the other collects aerosols from both the ocean and the land (all-direction collector). Each collector is equipped with two filters to sample size-aggregated aerosols (fine aerosols: NSS-SO42-, 70%), while coarse aerosols are dominated by sea-salt sulfate. However, some NSS-SO42- was also observed in coarse aerosols collected in summer, suggesting the presence of accumulation mode NSS-SO42- aerosols, which is possibly due to high summer biogenic DMS flux. The sources of sulfur in NSS-SO42- could be further determined by their d34S values. DMS emission is likely the sole sulfur source in the open-ocean collector as it shows constant DMS-like d34S signatures (15-18‰) throughout the year. Meanwhile, the d34S of NSS-SO42- in the all-direction collector display a seasonal trend: summer time d34S values are higher and DMS-like (15-18‰), indicating DMS emission is the dominant sulfur source; winter time d34S values are lower ( 6-12‰), therefore the sulfur is likely sourced from both DMS emission and terrestrial S input with low d34S values, such as volcanic activities, fossil fuel and wood burning.

ATMOS Stratospheric Deuterated Water and Implications for Tropospheric-Stratospheric Transport

Science.gov (United States)

Moyer, Elisabeth J.; Irion, Fredrick W.; Yung, Yuk L.; Gunson, Michael R.

1996-01-01

Measurements of the isotopic composition of stratospheric water by the ATMOS instrument are used to infer the convective history of stratospheric air. The average water vapor entering the stratosphere is found to be highly depleted of deuterium, with delta-D(sub w) of -670 +/- 80 (67% deuterium loss). Model calculations predict, however, that under conditions of thermodynamic equilibrium, dehydration to stratospheric mixing ratios should produce stronger depletion to delta-D(sub w) of -800 to 900 (80-90% deuterium loss). Deuterium enrichment of water vapor in ascending parcels can occur only in conditions of rapid convection; enrichments persisting into the stratosphere require that those conditions continue to near-tropopause altitudes. We conclude that either the predominant source of water vapor to the uppermost troposphere is enriched convective water, most likely evaporated cloud ice, or troposphere-stratosphere transport occurs closely associated with tropical deep convection.

Coastal Antarctic aerosol: the seasonal pattern of its chemical composition and radionuclide content

International Nuclear Information System (INIS)

Wagenbach, D.; Goerlach, U.; Moser, K.; Muennich, K.O.

1988-01-01

At the German Antarctic research station (70 degrees S, 8 degrees W), long-term observations of the chemical and radio-chemical composition of atmospheric particulate matter were started in spring 1983. Based on the analysis of high-volume aerosol filters sampled continuously for nearly 5 years, concentration records of the following aerosol components are presented here: (a) major ions (sea-salt, sulfate, nitrate); (b) cosmogenic 7 Be and terrigeneous 210 Pb; (c) trace elements (crustal Mn, heavy metal Pb). All species mentioned, with the exception of stable and radioactive Pb, show annual cycles. The maximum occurs in austral summer for 7 Be, sulfate, and crustal Mn. For sea-salt, however, the maximum is found in local autumn, and for nitrate in local spring. In local summer, the enhanced 7 Be to 210 Pb ratio is attributed to intenser large scale vertical mixing. The pattern of total sulfate seems to be controlled by the nss-sulfate production from marine organo-sulfur species during local summer, whereas in polar night, nss-sulfate shows very low or even negative concentration. Crustal aerosol (indicated by Mn) shows a mean summer contribution of 16 ng/SCM which exceeds the mean winter level by more than a factor of two. Based on a mean wash-out ratio of 0.27x10 6 observed for 210 Pb bearing aerosol particles, a Pb snow concentration of 3.0 pg/g is deduced from the mean air concentration of 11 pg/SCM. (authors)

SAGE II measurements of early Pinatubo aerosols

Science.gov (United States)

Mccormick, M. P.; Veiga, R. E.

1992-01-01

SAGE II satellite measurements of the Mt. Pinatubo eruption cloud in the stratosphere during June, July, and early August 1991 show that aerosols in the tropics reached as high as 29 km altitude with most of the cloud between 20 and 25 km. The most optically thick portions of the cloud covered latitudes from 10 deg S to 30 deg N during the early part of this period. By late July, high stratospheric optical depths were observed to at least 70 deg N, with the high values north of about 30 deg N from layers below 20 km. High pressure systems in both hemispheres were observed to be correlated with the movement of volcanic material at 21 km into the westerly jet stream at high southern latitudes and similarly to high northern latitudes at 16 km. By August, the entire Southern Hemisphere had experienced a 10-fold increase in optical depth relative to early July due to layers above 20 km. Initial mass calculations using SAGE II data place the aerosol produced from this eruption at 20 to 30 megatons, well above the 12 megatons produced by El Chichon.

In situ trace gas and particle measurements in the summer lower stratosphere during STREAM II. Implications for O{sub 3} production

Energy Technology Data Exchange (ETDEWEB)

Bregman, A; Lelieveld, J; Scheeren, H A [Institute for Marine and Atmospheric Sciences, Utrecht (Netherlands); Arnold, F; Buerger, V; Schneider, J [Max-Planck-Inst. for Nuclear Physics, Heidelberg (Germany); Fischer, H; Waibel, A [Max-Planck-Inst. fuer Chemie, Mainz (Germany); Siegmund, P C; Wauben, W M.F. [Koninklijk Nederlands Meteorologisch Inst., De Bilt (Netherlands); Stroem, J [Stockholm Univ. (Sweden). Dept. of Meteorology

1998-12-31

In situ aircraft measurements of O{sub 3}, CO, HNO{sub 3}, and aerosol particles are presented, performed over the North Sea region in the summer lower stratosphere during the STREAM-II campaign (Stratosphere Troposphere Experiments by Aircraft Measurements). Elevated CO mixing ratios are attributed to mixing of polluted tropospheric air into the lowermost extra-tropical stratosphere. Model calculations illustrate that the O{sub 3} production efficiency of NO{sub x} is smaller than previously assumed, under conditions with relatively high HNO{sub 3} mixing ratios, as observed during STREAM-II. The model simulations further suggest a relatively high O{sub 3} production efficiency from CO oxidation, as a result of the relatively high ambient HNO{sub 3} and NO{sub x} concentrations, implying that upward transport of CO rich air enhances O{sub 3} production in the lowermost stratosphere. (author) 13 refs.

In situ trace gas and particle measurements in the summer lower stratosphere during STREAM II. Implications for O{sub 3} production

Energy Technology Data Exchange (ETDEWEB)

Bregman, A.; Lelieveld, J.; Scheeren, H.A. [Institute for Marine and Atmospheric Sciences, Utrecht (Netherlands); Arnold, F.; Buerger, V.; Schneider, J. [Max-Planck-Inst. for Nuclear Physics, Heidelberg (Germany); Fischer, H.; Waibel, A. [Max-Planck-Inst. fuer Chemie, Mainz (Germany); Siegmund, P.C.; Wauben, W.M.F. [Koninklijk Nederlands Meteorologisch Inst., De Bilt (Netherlands); Stroem, J. [Stockholm Univ. (Sweden). Dept. of Meteorology

1997-12-31

In situ aircraft measurements of O{sub 3}, CO, HNO{sub 3}, and aerosol particles are presented, performed over the North Sea region in the summer lower stratosphere during the STREAM-II campaign (Stratosphere Troposphere Experiments by Aircraft Measurements). Elevated CO mixing ratios are attributed to mixing of polluted tropospheric air into the lowermost extra-tropical stratosphere. Model calculations illustrate that the O{sub 3} production efficiency of NO{sub x} is smaller than previously assumed, under conditions with relatively high HNO{sub 3} mixing ratios, as observed during STREAM-II. The model simulations further suggest a relatively high O{sub 3} production efficiency from CO oxidation, as a result of the relatively high ambient HNO{sub 3} and NO{sub x} concentrations, implying that upward transport of CO rich air enhances O{sub 3} production in the lowermost stratosphere. (author) 13 refs.

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......, but the concentration of glacial sulfate does not distinguish between tropospheric and stratospheric eruptions. Stable sulfur isotope abundances contain additional information, and recent studies show a correlation between volcanic plumes that reach the stratosphere and mass-independent anomalies in sulfur isotopes...... 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...

Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

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J. Schmale

2013-09-01

Full Text Available Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS, was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass, a methanesulfonic acid OA factor (MSA-OA, 25%, a marine oxygenated OA factor (M-OOA, 41%, a sea spray OA fraction (SS-OA, 7% and locally produced hydrocarbon-like OA (HOA, 9%. The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13, has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA. However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not

Modeling the Sulfate Deposition to the Greenland Ice Sheet From the Laki Eruption

Science.gov (United States)

Oman, L.; Robock, A.; Stenchikov, G.; Thordarson, T.; Gao, C.

2005-12-01

Using the state of the art Goddard Institute for Space Studies (GISS) modelE general circulation model, simulations were conducted of the chemistry and transport of aerosols resulting from the 1783-84 Laki (64°N) flood lava eruption. A set of 3 ensemble simulations from different initial conditions were conducted by injecting our estimate of the SO2 gas into the atmosphere by the 10 episodes of the eruption and allowing the sulfur chemistry model to convert this gas into sulfate aerosol. The SO2 gas and sulfate aerosol is transported by the model and wet and dry deposition is calculated over each grid box during the simulation. We compare the resulting sulfate deposition to the Greenland Ice Sheet in the model to 23 ice core measurements and find very good agreement. The model simulation deposits a range of 169 to over 300 kg/km2 over interior Greenland with much higher values along the coastal areas. This compares to a range of 62 to 324 kg/km2 for the 23 ice core measurements with an average value of 158 kg/km2. This comparison is one important model validation tool. Modeling and observations show fairly large spatial variations in the deposition of sulfate across the Greenland Ice Sheet for the Laki eruption, but the patterns are similar to those we modeled for the 1912 Katmai and 1991 Pinatubo eruptions. Estimates of sulfate loading based on single ice cores can show significant differences, so ideally several ice cores should be combined in reconstructing the sulfate loading of past volcanic eruptions, taking into account the characteristic spatial variations in the deposition pattern.

Development of an Operational Multi-sensor and Multi-channel Aerosol Assimilation Package Using NAAPS and NAVDAS

Science.gov (United States)

2010-09-30

5593-1, 2010, EGU General Assembly 2010. Shi, Y., J. Zhang, J. S. Reid, E. Hyer, Evaluation of MISR Aerosol Optical Depth Product for Aerosol Data...a surrogate for aerosol type, as large η values are generally related to fine mode aerosols, such as sulfate and smoke aerosols, and small η values

Global direct radiative forcing by process-parameterized aerosol optical properties

Science.gov (United States)

KirkevâG, Alf; Iversen, Trond

2002-10-01

A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

Size-specific composition of aerosols in the El Chichon volcanic cloud

Science.gov (United States)

Woods, D. C.; Chuan, R. L.

1983-01-01

A NASA U-2 research aircraft flew sampling missions in April, May, July, November, and December 1982 aimed at obtaining in situ data in the stratospheric cloud produced from the March-April 1982 El Chichon eruptions. Post flight analyses provided information on the aerosol composition and morphology. The particles ranged in size from smaller than 0.05 m to larger than 20 m diameter and were quite complex in composition. In the April, May, and July samples the aerosol mass was dominated by magmatic and lithic particles larger than about 3 m. The submicron particles consisted largely of sulfuric acid. Halite particles, believed to be related to a salt dome beneath El Chichon, were collected in the stratosphere in April and May. On the July 23 flight, copper-zinc oxide particles were collected. In July, November, and December, in addition to the volcanic ash and acid particles, carbon-rich particles smaller than about 0.1 m aerodynamic diameter were abundant.

Global source attribution of sulfate concentration and direct and indirect radiative forcing

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Y. Yang

2017-07-01

Full Text Available The global source–receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF from 16 regions/sectors for years 2010–2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggesting that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is −0.42 W m−2, with −0.31 W m−2 contributed by anthropogenic sulfate and −0.11 W m−2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS contributes 17–84 % to the total DRF. East Asia has the largest contribution of 20–30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of −0.44 W m−2. DMS has the largest contribution, explaining −0.23 W m−2 of the global sulfate incremental IRF. Incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.

Aerosols at the poles: an AeroCom Phase II multi-model evaluation

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M. Sand

2017-10-01

Full Text Available Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC from fossil fuel and biomass burning, sulfate, organic aerosols (OAs, dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs, we document the role of these aerosols at high latitudes.The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt and spring (dust, whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N. The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE associated with BC and OA from fossil fuel and biofuel (FF, sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (−0.12 W m−2, dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity

Removal of sulfur dioxide and formation of sulfate aerosol in Tokyo

Science.gov (United States)

Miyakawa, T.; Takegawa, N.; Kondo, Y.

2007-07-01

Ground-based in situ measurements of sulfur dioxide (SO2) and submicron sulfate aerosol (SO42-) together with carbon monoxide (CO) were conducted at an urban site in Tokyo, Japan from spring 2003 to winter 2004. The observed concentrations of SO2 were affected dominantly by anthropogenic emissions (for example, manufacturing industries) in source areas, while small fraction of the data (sulfur compounds (SOx = SO2 + SO42-) and the remaining fraction of SOx, which is derived as the ratio of the linear regression slope of the SOx-CO correlation, is used as measures for the formation of SO42- and removal of SOx, respectively. Using these parameters, the average formation efficiency of SO42- (i.e., amount of SO42- produced per SO2 emitted from emission sources) are estimated to be 0.18 and 0.03 in the summer and winter periods, respectively. A simple box model was developed to estimate the lifetime of SOx. The lifetime of SOx for the summer period (26 h) is estimated to be about two times longer than that for the winter period (14 h). The seasonal variations of the remaining fraction of SOx, estimated formation efficiency of SO42-, and lifetime of SOx are likely due to those of the boundary layer height and photochemical activity (i.e., hydroxyl radical). These results provide useful insights into the formation and removal processes of sulfur compounds exported from an urban area.

The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore–Washington, D.C. region

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A. J. Beyersdorf

2016-01-01

Full Text Available In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites and mass measurements of aerosol loading (PM2.5 used for air quality monitoring must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH, and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 % and organics (57 %. A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs. The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35�

Importance of sulfate radical anion formation and chemistry in heterogeneous OH oxidation of sodium methyl sulfate, the smallest organosulfate

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K. C. Kwong

2018-02-01

Full Text Available Organosulfates are important organosulfur compounds present in atmospheric particles. While the abundance, composition, and formation mechanisms of organosulfates have been extensively investigated, it remains unclear how they transform and evolve throughout their atmospheric lifetime. To acquire a fundamental understanding of how organosulfates chemically transform in the atmosphere, this work investigates the heterogeneous OH radical-initiated oxidation of sodium methyl sulfate (CH3SO4Na droplets, the smallest organosulfate detected in atmospheric particles, using an aerosol flow tube reactor at a high relative humidity (RH of 85 %. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (direct analysis in real time, DART coupled with a high-resolution mass spectrometer showed that neither functionalization nor fragmentation products are detected. Instead, the ion signal intensity of the bisulfate ion (HSO4− has been found to increase significantly after OH oxidation. We postulate that sodium methyl sulfate tends to fragment into a formaldehyde (CH2O and a sulfate radical anion (SO4 ⋅ − upon OH oxidation. The formaldehyde is likely partitioned back to the gas phase due to its high volatility. The sulfate radical anion, similar to OH radical, can abstract a hydrogen atom from neighboring sodium methyl sulfate to form the bisulfate ion, contributing to the secondary chemistry. Kinetic measurements show that the heterogeneous OH reaction rate constant, k, is (3.79 ± 0.19  ×  10−13 cm3 molecule−1 s−1 with an effective OH uptake coefficient, γeff, of 0.17 ± 0.03. While about 40 % of sodium methyl sulfate is being oxidized at the maximum OH exposure (1.27  ×  1012 molecule cm−3 s, only a 3 % decrease in particle diameter is observed. This can be attributed to a small fraction of particle mass lost via the formation and volatilization of formaldehyde. Overall, we

Aerosol composition and source apportionment in Santiago de Chile

Science.gov (United States)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dpsource apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.

SECONDARY ORGANIC AEROSOL FORMATION FROM THE OXIDATION OF AROMATIC HYDROCARBONS IN THE PRESENCE OF DRY SUBMICRON AMMONIUM SULFATE AEROSOL

Science.gov (United States)

A laboratory study was conducted to examine formation of secondary organic aerosols. A smog chamber system was developed for studying gas-aerosol interactions in a dynamic flow reactor. These experiments were conducted to investigate the fate of gas and aerosol phase compounds ...

Future aerosols of the southwest - Implications for fundamental aerosol research

International Nuclear Information System (INIS)

Friedlander, S.K.

1980-01-01

It is shown that substantial increases in the use of coal in the U.S. will lead to substantial increases in emissions of particulate matter, SO/sub x/, and NO/sub x/ in the part of the U.S. west of the Mississippi. A shift in the primary particulate emissions from coarse to submicron particles is predicted. Attention is given to the nature of the submicron aerosol in the southwest, the distribution of sulfur with respect to particle size, the formation of new particles in the atmosphere, and the ammonium nitrate equilibrium. It is concluded that increased coal use will result in a 50% increase in SO/sub x/ emissions and a doubling of NO/sub x/ emissions in the western U.S. by the year 2000, that ambient levels of aerosol sulfates and nitrates will increase, and that a large increase in submicron aerosol mass is likely

Characterizing the Asian Tropopause Aerosol Layer (ATAL) Using Satellite Observations, Balloon Measurements and a Chemical Transport Model

Science.gov (United States)

Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.;

Effects of tropospheric aerosols on radiative flux calculations at UV and visible wavelengths

International Nuclear Information System (INIS)

Grossman, A.S.; Grant, K.E.

1994-08-01

The surface fluxes in the wavelength range 175 to 735nm have been calculated for an atmosphere which contains a uniformly mixed aerosol layer of thickness 1km at the earth's surface. Two different aerosol types were considered, a rural aerosol, and an urban aerosol. The visibility range for the aerosol layers was 95 to 15 km. Surface flux ratios (15km/95km) were in agreement with previously published results for the rural aerosol layer to within about 2%. The surface flux ratios vary from 7 to 14% for the rural aerosol layer and from 13 to 23% for the urban aerosol layer over the wavelength range. A tropospheric radiative forcing of about 1.3% of the total tropospheric flux was determined for the 95km to 15km visibility change in the rural aerosol layer, indicating the potential of tropospheric feedback effects on the surface flux changes. This effect was found to be negligible for the urban aerosol layer. Stratospheric layer heating rate changes due to visibility changes in either the rural or urban aerosol layer were found to be negligible

On the composition and optical extinction of particles in the tropopause region

Energy Technology Data Exchange (ETDEWEB)

Kaercher, B. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Solomon, S. [National Oceanic and Atmospheric Administration, Boulder, CO (United States). Aeronomy Lab.

1999-06-01

Liquid aerosol particles and ice crystals in subvisible cirrus clouds in the tropopause region are characterized in terms of size distributions, chemical composition, and optical extinction. These particle properties are studied by means of simple models and are related to satellite extinction measurements, particularly for midlatitudes. Sulfuric acid aerosols can take up nitric acid near the ice frost point, just before ice nucleation. Aerosols in the tropopause region may show a larger spread of extinction and extinction ratios at different wavelengths than background stratospheric aerosols. The high surface areas and low extinction ratios of subvisible cirrus deduced from satellite observations are unlikely to be due purely to aerosols, except for high sulfate loadings. It is shown that mixtures of liquid aerosols and ice particles can more readily explain these data with only small cloud fractions along the line of sight of the optical sensors. The efficiency of heterogeneous chlorine activation in aerosol/cloud mixtures, the availability of water vapor, sulfate, and nitrate, and the effects of temperature, ammonium, ice nuclei and aircraft emissions on the properties of particles in the tropopause region are explored. (orig.)

Impact of high speed civil transports on stratospheric ozone. A 2-D model investigation

Energy Technology Data Exchange (ETDEWEB)

Kinnison, D E; Connell, P S [Lawrence Livermore National Lab., CA (United States)

1998-12-31

This study investigates the effect on stratospheric ozone from a fleet of proposed High Speed Civil Transports (HSCTs). The new LLNL 2-D operator-split chemical-radiative-transport model of the troposphere and stratosphere is used for this HSCT investigation. This model is integrated in a diurnal manner, using an implicit numerical solver. Therefore, rate coefficients are not modified by any sort of diurnal average factor. This model also does not make any assumptions on lumping of chemical species into families. Comparisons to previous model-derived HSCT assessment of ozone change are made, both to the previous LLNL 2-D model and to other models from the international assessment modeling community. The sensitivity to the NO{sub x} emission index and sulfate surface area density is also explored. (author) 7 refs.

Impact of high speed civil transports on stratospheric ozone. A 2-D model investigation

Energy Technology Data Exchange (ETDEWEB)

Kinnison, D.E.; Connell, P.S. [Lawrence Livermore National Lab., CA (United States)

1997-12-31

This study investigates the effect on stratospheric ozone from a fleet of proposed High Speed Civil Transports (HSCTs). The new LLNL 2-D operator-split chemical-radiative-transport model of the troposphere and stratosphere is used for this HSCT investigation. This model is integrated in a diurnal manner, using an implicit numerical solver. Therefore, rate coefficients are not modified by any sort of diurnal average factor. This model also does not make any assumptions on lumping of chemical species into families. Comparisons to previous model-derived HSCT assessment of ozone change are made, both to the previous LLNL 2-D model and to other models from the international assessment modeling community. The sensitivity to the NO{sub x} emission index and sulfate surface area density is also explored. (author) 7 refs.

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

Aerosols: connection between regional climatic change and air quality (Iupac Technical Report)

NARCIS (Netherlands)

Slanina, J.; Zhang, Y.H.

2004-01-01

yAerosols play an important role in all problems connected with air pollution, ranging from very local effects and human health problems to regional problems such as acid deposition and eutrophication up to continental and global questions such as stratospheric ozone loss and climatic change. In

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.

Operational aerosol and dust storm forecasting

International Nuclear Information System (INIS)

Westphal, D L; Curtis, C A; Liu, M; Walker, A L

2009-01-01

The U. S. Navy now conducts operational forecasting of aerosols and dust storms on global and regional scales. The Navy Aerosol Analysis and Prediction System (NAAPS) is run four times per day and produces 6-day forecasts of sulfate, smoke, dust and sea salt aerosol concentrations and visibility for the entire globe. The Coupled Ocean Atmosphere Mesoscale Prediction System (COAMPS (registered) ) is run twice daily for Southwest Asia and produces 3-day forecasts of dust, smoke, and visibility. The graphical output from these models is available on the Internet (www.nrlmry.navy.mil/aerosol/). The aerosol optical properties are calculated for each specie for each forecast output time and used for sea surface temperature (SST) retrieval corrections, regional electro-optical (EO) propagation assessments, and the development of satellite algorithms. NAAPS daily aerosol optical depth (AOD) values are compared with the Advanced Very High Resolution Radiometer (AVHRR) and Moderate Resolution Imaging Spectroradiometer (MODIS) AOD values. Visibility forecasts are compared quantitatively with surface synoptic reports.

Lightning-produced NOx in an explicit electrical scheme tested in a Stratosphere-Troposphere Experiment: Radiation, Aerosols, and Ozone case study

Science.gov (United States)

Barthe, Christelle; Pinty, Jean-Pierre; Mari, CéLine

2007-02-01

An explicit lightning-produced nitrogen oxide (LNOx) scheme has been implemented in a 3-D mesoscale model. The scheme is based on the simulation of the electrical state of the cloud and provides a prediction of the temporal and spatial distribution of the lightning flashes. The frequency and the 3-D morphology of the lightning flashes are captured realistically so fresh nitrogen oxide molecules can be added along the complex flash path as a function of the pressure, as suggested by results from laboratory experiments. The scheme is tested on the 10 July 1996 Stratosphere-Troposphere Experiment: Radiation, Aerosols, and Ozone (STERAO) storm. The model reproduces many features of the observed increase of electrical activity and LNOx flux density between the multicell and supercell stages. LNOx dominates the NOx budget in the upper part of the cells with instantaneous peak concentrations exceeding 4 ppbv, as observed. The computed flux of NOx across the anvil shows a mean value of 6 mol m-2 s-1 during the last 90 min of the simulation. This value is remarkably stable and compares favorably with the observations.

Observation of stratospheric ozone with NIES lidar system in Tsukuba, Japan

International Nuclear Information System (INIS)

Nakane, H.; Hayashida, S.; Sasano, Y.; Sugimoto, N.; Matsui, I.; Minato, A.

1992-01-01

Lidars are expected to play important roles in an international monitoring network of the stratosphere such as the Network for the Detection of Stratospheric Change (NDSC). The National Institute for Environmental Studies (NIES) in Tsukuba constructed an ozone lidar system in March 1988 and started observation in August 1988. The lidar system has a 2-m telescope and injection locked XeCl and XeF excimer lasers which can measure ozone profiles (15-45 km) and temperature profiles (30-80 km). From December 1991, lidar observations have been carried out in which the second Stokes line of the stimulated Raman scattering of a KrF laser has been used. Ozone profiles obtained with the NIES lidar system are compared with the data provided by the SAGE II satellite sensor. Results showed good agreement for the individual and the zonal mean profiles. Variations of ozone with various time scales at each altitude can be studied using the data obtained with the NIES ozone lidar system. Seasonal variations are easily found at 20 km, 30 km, and 35 km, which are qualitatively understood as a result of dynamical and photochemical effects. Systematic errors of ozone profiles due to the Pinatubo stratospheric aerosols have been detected using multi-wavelength observation

Sensitivity of aerosol loading and properties to cloudiness

Science.gov (United States)

Iversen, T.; Seland, O.; Kirkevag, A.; Kristjansson, J. E.

2005-12-01

Clouds influence aerosols in various ways. Sulfate is swiftly produced in liquid phase provided there is both sulfur dioxide and oxidants available. Nucleation and Aitken mode aerosol particles efficiently grow in size by collision and coagulation with cloud droplets. When precipitation is formed, aerosol and precursor gases may be quickly removed bay rainout. The dynamics associated with clouds in some cases may swiftly mix aerosols deeply into the troposphere. In some cases Aitken-mode particles may be formed in cloud droplets by splitting agglomerates of particulate matter such as black carbon In this presentation we will discuss how global cloudiness may influence the burden, residence time, and spatial distribution of sulfate, black carbon and particulate organic matter. A similar physico-chemical scheme for there compounds has been implemented in three generations of the NCAR community climate model (CCM3, CAM2 and CAM3). The scheme is documented in the literature and is a part of the Aerocom-intercomparison. There are many differences between these models. With respect to aerosols, a major difference is that CAM3 has a considerably higher global cloud volume and more then twice the amount of cloud water than CAM2 and CCM3. Atmospheric simulations have been made with prescribed ocean temperatures. It is slightly surprising to discover that certain aspects of the aerosols are not particularly sensitive to these differences in cloud availability. This sensitivity will be compared to sensitivities with respect to processing in deep convective clouds.

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

Science.gov (United States)

Wang, Xiaowei; Jing, Bo; Tan, Fang; Ma, Jiabi; Zhang, Yunhong; Ge, Maofa

2017-10-01

Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA) and mixed particles composed of ammonium sulfate (AS) and OA with different organic to inorganic molar ratios (OIRs) have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH), and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH) for mixed OA / AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH) of AS in mixed OA / AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA / AS droplets indicate the formation of ammonium hydrogen oxalate (NH4HC2O4) and ammonium hydrogen sulfate (NH4HSO4) from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA / AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH4)2SO4 into NH4HC2O4 with a high DRH. Although the hygroscopic growth of mixed OA / AS droplets is comparable to that of AS or OA at high RH during the dehydration process, Raman growth

Sudden Stratospheric Warming Compendium

Data.gov (United States)

National Oceanic and Atmospheric Administration, Department of Commerce — Sudden Stratospheric Warming Compendium (SSWC) data set documents the stratospheric, tropospheric, and surface climate impacts of sudden stratospheric warmings. This...

MIRAGE: Model description and evaluation of aerosols and trace gases

Science.gov (United States)

Easter, Richard C.; Ghan, Steven J.; Zhang, Yang; Saylor, Rick D.; Chapman, Elaine G.; Laulainen, Nels S.; Abdul-Razzak, Hayder; Leung, L. Ruby; Bian, Xindi; Zaveri, Rahul A.

2004-10-01

The Model for Integrated Research on Atmospheric Global Exchanges (MIRAGE) modeling system, designed to study the impacts of anthropogenic aerosols on the global environment, is described. MIRAGE consists of a chemical transport model coupled online with a global climate model. The chemical transport model simulates trace gases, aerosol number, and aerosol chemical component mass (sulfate, methane sulfonic acid (MSA), organic matter, black carbon (BC), sea salt, and mineral dust) for four aerosol modes (Aitken, accumulation, coarse sea salt, and coarse mineral dust) using the modal aerosol dynamics approach. Cloud-phase and interstitial aerosol are predicted separately. The climate model, based on Community Climate Model, Version 2 (CCM2), has physically based treatments of aerosol direct and indirect forcing. Stratiform cloud water and droplet number are simulated using a bulk microphysics parameterization that includes aerosol activation. Aerosol and trace gas species simulated by MIRAGE are presented and evaluated using surface and aircraft measurements. Surface-level SO2 in North American and European source regions is higher than observed. SO2 above the boundary layer is in better agreement with observations, and surface-level SO2 at marine locations is somewhat lower than observed. Comparison with other models suggests insufficient SO2 dry deposition; increasing the deposition velocity improves simulated SO2. Surface-level sulfate in North American and European source regions is in good agreement with observations, although the seasonal cycle in Europe is stronger than observed. Surface-level sulfate at high-latitude and marine locations, and sulfate above the boundary layer, are higher than observed. This is attributed primarily to insufficient wet removal; increasing the wet removal improves simulated sulfate at remote locations and aloft. Because of the high sulfate bias, radiative forcing estimates for anthropogenic sulfur given in 2001 by S. J. Ghan and

Observational evidence for pollution-influenced selective uptake contributing to biogenic secondary organic aerosols in the southeastern U.S.

Science.gov (United States)

Liu, J.; Russell, L. M.; Lee, A. K. Y.; McKinney, K. A.; Surratt, J. D.; Ziemann, P. J.

2017-08-01

During the 2013 Southern Oxidant and Aerosol Study, aerosol mass spectrometer measurements of submicron mass and single particles were taken at Look Rock, Tennessee. Their concentrations increased during multiday stagnation events characterized by low wind, little rain, and increased daytime isoprene emissions. Organic mass (OM) sources were apportioned as 42% "vehicle-related" and 54% biogenic secondary organic aerosol (bSOA), with the latter including "sulfate-related bSOA" that correlated to sulfate (r = 0.72) and "nitrate-related bSOA" that correlated to nitrate (r = 0.65). Single-particle mass spectra showed three composition types that corresponded to the mass-based factors with spectra cosine similarity of 0.93 and time series correlations of r > 0.4. The vehicle-related OM with m/z 44 was correlated to black carbon, "sulfate-related bSOA" was on particles with high sulfate, and "nitrate-related bSOA" was on all particles. The similarity of the m/z spectra (cosine similarity = 0.97) and the time series correlation (r = 0.80) of the "sulfate-related bSOA" to the sulfate-containing single-particle type provide evidence for particle composition contributing to selective uptake of isoprene oxidation products onto particles that contain sulfate from power plants.

Probability Density Functions for the CALIPSO Lidar Version 4 Cloud-Aerosol Discrimination (CAD) Algorithm

Science.gov (United States)

Liu, Z.; Kar, J.; Zeng, S.; Tackett, J. L.; Vaughan, M.; Trepte, C. R.; Omar, A. H.; Hu, Y.; Winker, D. M.

2017-12-01

In the CALIPSO retrieval algorithm, detection layers in the lidar measurements is followed by their classification as a "cloud" or "aerosol" using 5-dimensional probability density functions (PDFs). The five dimensions are the mean attenuated backscatter at 532 nm, the layer integrated total attenuated color ratio, the mid-layer altitude, integrated volume depolarization ratio and latitude. The new version 4 (V4) level 2 (L2) data products, released in November 2016, are the first major revision to the L2 product suite since May 2010. Significant calibration changes in the V4 level 1 data necessitated substantial revisions to the V4 L2 CAD algorithm. Accordingly, a new set of PDFs was generated to derive the V4 L2 data products. The V4 CAD algorithm is now applied to layers detected in the stratosphere, where volcanic layers and occasional cloud and smoke layers are observed. Previously, these layers were designated as `stratospheric', and not further classified. The V4 CAD algorithm is also applied to all layers detected at single shot (333 m) resolution. In prior data releases, single shot detections were uniformly classified as clouds. The CAD PDFs used in the earlier releases were generated using a full year (2008) of CALIPSO measurements. Because the CAD algorithm was not applied to stratospheric features, the properties of these layers were not incorporated into the PDFs. When building the V4 PDFs, the 2008 data were augmented with additional data from June 2011, and all stratospheric features were included. The Nabro and Puyehue-Cordon volcanos erupted in June 2011, and volcanic aerosol layers were observed in the upper troposphere and lower stratosphere in both the northern and southern hemispheres. The June 2011 data thus provides the stratospheric aerosol properties needed for comprehensive PDF generation. In contrast to earlier versions of the PDFs, which were generated based solely on observed distributions, construction of the V4 PDFs considered the

AOD Distributions and Trends of Major Aerosol Species over a Selection of the World's Most Populated Cities Based on the 1st Version of NASA's MERRA Aerosol Reanalysis

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Provencal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

2017-01-01

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to

Reevaluation of Stratospheric Ozone Trends From SAGE II Data Using a Simultaneous Temporal and Spatial Analysis

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Damadeo, R. P.; Zawodny, J. M.; Thomason, L. W.

2014-01-01

This paper details a new method of regression for sparsely sampled data sets for use with time-series analysis, in particular the Stratospheric Aerosol and Gas Experiment (SAGE) II ozone data set. Non-uniform spatial, temporal, and diurnal sampling present in the data set result in biased values for the long-term trend if not accounted for. This new method is performed close to the native resolution of measurements and is a simultaneous temporal and spatial analysis that accounts for potential diurnal ozone variation. Results show biases, introduced by the way data is prepared for use with traditional methods, can be as high as 10%. Derived long-term changes show declines in ozone similar to other studies but very different trends in the presumed recovery period, with differences up to 2% per decade. The regression model allows for a variable turnaround time and reveals a hemispheric asymmetry in derived trends in the middle to upper stratosphere. Similar methodology is also applied to SAGE II aerosol optical depth data to create a new volcanic proxy that covers the SAGE II mission period. Ultimately this technique may be extensible towards the inclusion of multiple data sets without the need for homogenization.

Production of Highly Charged Pharmaceutical Aerosols Using a New Aerosol Induction Charger.

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Golshahi, Laleh; Longest, P Worth; Holbrook, Landon; Snead, Jessica; Hindle, Michael

2015-09-01

Properly charged particles can be used for effective lung targeting of pharmaceutical aerosols. The objective of this study was to characterize the performance of a new induction charger that operates with a mesh nebulizer for the production of highly charged submicrometer aerosols to bypass the mouth-throat and deliver clinically relevant doses of medications to the lungs. Variables of interest included combinations of model drug (albuterol sulfate) and charging excipient (NaCl) as well as strength of the charging field (1-5 kV/cm). Aerosol charge and size were measured using a modified electrical low pressure impactor system combined with high performance liquid chromatography. At the approximate mass median aerodynamic diameter (MMAD) of the aerosol (~0.4 μm), the induction charge on the particles was an order of magnitude above the field and diffusion charge limit. The nebulization rate was 439.3 ± 42.9 μl/min, which with a 0.1% w/v solution delivered 419.5 ± 34.2 μg of medication per minute. A new correlation was developed to predict particle charge produced by the induction charger. The combination of the aerosol induction charger and predictive correlations will allow for the practical generation and control of charged submicrometer aerosols for targeting deposition within the lungs.

Fine resolution atmospheric sulfate model driven by operational meteorological data: Comparison with observations

International Nuclear Information System (INIS)

Benkovitz, C.M.; Schwartz, S.E.; Berkowitz, C.M.; Easter, R.C.

1993-09-01

The hypothesis that anthropogenic sulfur aerosol influences clear-sky and cloud albedo and can thus influence climate has been advanced by several investigators; current global-average climate forcing is estimated to be of comparable magnitude, but opposite sign, to longwave forcing by anthropogenic greenhouse gases. The high space and time variability of sulfate concentrations and column aerosol burdens have been established by observational data; however, geographic and time coverage provided by data from surface monitoring networks is very limited. Consistent regional and global estimates of sulfate aerosol loading, and the contributions to this loading from different sources can be obtained only by modeling studies. Here we describe a sub-hemispheric to global-scale Eulerian transport and transformation model for atmospheric sulfate and its precursors, driven by operational meteorological data, and report results of calculations for October, 1986 for the North Atlantic and adjacent continental regions. The model, which is based on the Global Chemistry Model uses meteorological data from the 6-hour forecast model of the European Center for Medium-Range Weather Forecast to calculate transport and transformation of sulfur emissions. Time- and location-dependent dry deposition velocities were estimated using the methodology of Wesely and colleagues. Chemical reactions includes gaseous oxidation of SO 2 and DMS by OH, and aqueous oxidation of SO 2 by H 2 O 2 and O 3 . Anthropogenic emissions were from the NAPAP and EMEP 1985 inventories and biogenic emissions based on Bates et al. Calculated sulfate concentrations and column burdens exhibit high variability on spatial scale of hundreds of km and temporal scale of days. Calculated daily average sulfate concentrations closely reproduce observed concentrations at locations widespread over the model domain

Photochemical aging of aerosol particles in different air masses arriving at Baengnyeong Island, Korea

Science.gov (United States)

Kang, Eunha; Lee, Meehye; Brune, William H.; Lee, Taehyoung; Park, Taehyun; Ahn, Joonyoung; Shang, Xiaona

2018-05-01

Atmospheric aerosol particles are a serious health risk, especially in regions like East Asia. We investigated the photochemical aging of ambient aerosols using a potential aerosol mass (PAM) reactor at Baengnyeong Island in the Yellow Sea during 4-12 August 2011. The size distributions and chemical compositions of aerosol particles were measured alternately every 6 min from the ambient air or through the highly oxidizing environment of a potential aerosol mass (PAM) reactor. Particle size and chemical composition were measured by using the combination of a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Inside the PAM reactor, O3 and OH levels were equivalent to 4.6 days of integrated OH exposure at typical atmospheric conditions. Two types of air masses were distinguished on the basis of the chemical composition and the degree of aging: air transported from China, which was more aged with a higher sulfate concentration and O : C ratio, and the air transported across the Korean Peninsula, which was less aged with more organics than sulfate and a lower O : C ratio. For both episodes, the particulate sulfate mass concentration increased in the 200-400 nm size range when sampled through the PAM reactor. A decrease in organics was responsible for the loss of mass concentration in 100-200 nm particles when sampled through the PAM reactor for the organics-dominated episode. This loss was especially evident for the m/z 43 component, which represents less oxidized organics. The m/z 44 component, which represents further oxidized organics, increased with a shift toward larger sizes for both episodes. It is not possible to quantify the maximum possible organic mass concentration for either episode because only one OH exposure of 4.6 days was used, but it is clear that SO2 was a primary precursor of secondary aerosol in northeast Asia, especially during long-range transport from China. In addition

Prediction of health effects of cross-border atmospheric pollutants using an aerosol forecast model.

Science.gov (United States)

Onishi, Kazunari; Sekiyama, Tsuyoshi Thomas; Nojima, Masanori; Kurosaki, Yasunori; Fujitani, Yusuke; Otani, Shinji; Maki, Takashi; Shinoda, Masato; Kurozawa, Youichi; Yamagata, Zentaro

2018-08-01

Health effects of cross-border air pollutants and Asian dust are of significant concern in Japan. Currently, models predicting the arrival of aerosols have not investigated the association between arrival predictions and health effects. We investigated the association between subjective health symptoms and unreleased aerosol data from the Model of Aerosol Species in the Global Atmosphere (MASINGAR) acquired from the Japan Meteorological Agency, with the objective of ascertaining if these data could be applied to predicting health effects. Subjective symptom scores were collected via self-administered questionnaires and, along with modeled surface aerosol concentration data, were used to conduct a risk evaluation using generalized estimating equations between October and November 2011. Altogether, 29 individuals provided 1670 responses. Spearman's correlation coefficients were determined for the relationship between the proportion of the participants reporting the maximum score of two or more for each symptom and the surface concentrations for each considered aerosol species calculated using MASINGAR; the coefficients showed significant intermediate correlations between surface sulfate aerosol concentration and respiratory, throat, and fever symptoms (R = 0.557, 0.454, and 0.470, respectively; p < 0.01). In the general estimation equation (logit link) analyses, a significant linear association of surface sulfate aerosol concentration, with an endpoint determined by reported respiratory symptom scores of two or more, was observed (P trend = 0.001, odds ratio [OR] of the highest quartile [Q4] vs. the lowest [Q1] = 5.31, 95% CI = 2.18 to 12.96), with adjustment for potential confounding. The surface sulfate aerosol concentration was also associated with throat and fever symptoms. In conclusion, our findings suggest that modeled data are potentially useful for predicting health risks of cross-border aerosol arrivals. Copyright © 2018 Elsevier Ltd

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

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Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Shrivastava, Manish; Thomas, Jennie L.

2017-10-01

In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain-Fritsch + Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

Dry deposition of sulfate to Quercus rubra and Liriodendron tulipifera foliage

International Nuclear Information System (INIS)

Vandenberg, J.J.

1987-01-01

Estimates were made of the rate of dry deposition to red oak (Quercus rubra) and tulip poplar (Liriodendron tulipifera) foliage. In the laboratory, radioactive ammonium sulfate aerosols were generated in an exposure chamber. These aerosols were dry deposited onto leaves that were sequentially washed to examine the efficacy of washing procedures in removal of surface deposits. Over 90% of dry deposited sulfate was removed after a 30 second wash duration. Laboratory procedures also estimated the magnitude of foliar sulfur that leached into leaf wash solutions. The majority of laboratory leaves demonstrated no leaching of sulfur from the internal pool. However, some leaves showed significant sulfur leaching. It was concluded that leaching of internal sulfur was highly leaf specific. This indicated that each leaf used in field experiments needed to be individually examined for leaching

Fine aerosol bulk composition measured on WP-3D research aircraft in vicinity of the Northeastern United States – results from NEAQS

Directory of Open Access Journals (Sweden)

C. Warneke

2007-06-01

Full Text Available During the New England Air Quality Study (NEAQS in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC of the submicron (PM1.0 aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S. and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (~60% μg μg−1 and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km, but was significantly higher at altitude layers in the free troposphere (above 2.5 km. A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were

Characterization of distinct Arctic aerosol accumulation modes and their sources

Science.gov (United States)

Lange, R.; Dall'Osto, M.; Skov, H.; Nøjgaard, J. K.; Nielsen, I. E.; Beddows, D. C. S.; Simo, R.; Harrison, R. M.; Massling, A.

2018-06-01

In this work we use cluster analysis of long term particle size distribution data to expand an array of different shorter term atmospheric measurements, thereby gaining insights into longer term patterns and properties of Arctic aerosol. Measurements of aerosol number size distributions (9-915 nm) were conducted at Villum Research Station (VRS), Station Nord in North Greenland during a 5 year record (2012-2016). Alongside this, measurements of aerosol composition, meteorological parameters, gaseous compounds and cloud condensation nuclei (CCN) activity were performed during different shorter occasions. K-means clustering analysis of particle number size distributions on daily basis identified several clusters. Clusters of accumulation mode aerosols (main size modes > 100 nm) accounted for 56% of the total aerosol during the sampling period (89-91% during February-April, 1-3% during June-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking in February-April, with highest loadings of sulfate and black carbon concentrations. (2) Accumulation mode Bimodal aerosol shows two modes, at 38 nm and 150 nm, peaking in June-August, with the highest ratio of organics to sulfate concentrations. (3) Aged accumulation mode aerosol shows a single mode at 213 nm, peaking in September-October and is associated with cloudy and humid weather conditions during autumn. The three aerosol clusters were considered alongside CCN concentrations. We suggest that organic compounds, that are likely marine biogenic in nature, greatly influence the Bimodal cluster and contribute significantly to its CCN activity. This stresses the importance of better characterizing the marine ecosystem and the aerosol-mediated climate effects in the

Mid-infrared mapping of Jupiter's temperatures, aerosol opacity and chemical distributions with IRTF/TEXES

Science.gov (United States)

Fletcher, Leigh N.; Greathouse, T. K.; Orton, G. S.; Sinclair, J. A.; Giles, R. S.; Irwin, P. G. J.; Encrenaz, T.

2016-11-01

Global maps of Jupiter's atmospheric temperatures, gaseous composition and aerosol opacity are derived from a programme of 5-20 μm mid-infrared spectroscopic observations using the Texas Echelon Cross Echelle Spectrograph (TEXES) on NASA's Infrared Telescope Facility (IRTF). Image cubes from December 2014 in eight spectral channels, with spectral resolutions of R ∼2000 - 12 , 000 and spatial resolutions of 2-4° latitude, are inverted to generate 3D maps of tropospheric and stratospheric temperatures, 2D maps of upper tropospheric aerosols, phosphine and ammonia, and 2D maps of stratospheric ethane and acetylene. The results are compared to a re-analysis of Cassini Composite Infrared Spectrometer (CIRS) observations acquired during Cassini's closest approach to Jupiter in December 2000, demonstrating that this new archive of ground-based mapping spectroscopy can match and surpass the quality of previous investigations, and will permit future studies of Jupiter's evolving atmosphere. The visibility of cool zones and warm belts varies from channel to channel, suggesting complex vertical variations from the radiatively-controlled upper troposphere to the convective mid-troposphere. We identify mid-infrared signatures of Jupiter's 5-μm hotspots via simultaneous M, N and Q-band observations, which are interpreted as temperature and ammonia variations in the northern Equatorial Zone and on the edge of the North Equatorial Belt (NEB). Equatorial plumes enriched in NH3 gas are located south-east of NH3-desiccated 'hotspots' on the edge of the NEB. Comparison of the hotspot locations in several channels across the 5-20 μm range indicate that these anomalous regions tilt westward with altitude. Aerosols and PH3 are both enriched at the equator but are not co-located with the NH3 plumes. The equatorial temperature minimum and PH3/aerosol maxima have varied in amplitude over time, possibly as a result of periodic equatorial brightenings and the fresh updrafts of

The influence of different black carbon and sulfate mixing methods on their optical and radiative properties

Science.gov (United States)

Zhang, Hua; Zhou, Chen; Wang, Zhili; Zhao, Shuyun; Li, Jiangnan

2015-08-01

Three different internal mixing methods (Core-Shell, Maxwell-Garnett, and Bruggeman) and one external mixing method are used to study the impact of mixing methods of black carbon (BC) with sulfate aerosol on their optical properties, radiative flux, and heating rate. The optical properties of a mixture of BC and sulfate aerosol particles are considered for three typical bands. The results show that mixing methods, the volume ratio of BC to sulfate, and relative humidity have a strong influence on the optical properties of mixed aerosols. Compared to internal mixing, external mixing underestimates the particle mass absorption coefficient by 20-70% and the particle mass scattering coefficient by up to 50%, whereas it overestimates the particle single scattering albedo by 20-50% in most cases. However, the asymmetry parameter is strongly sensitive to the equivalent particle radius, but is only weakly sensitive to the different mixing methods. Of the internal methods, there is less than 2% difference in all optical properties between the Maxwell-Garnett and Bruggeman methods in all bands; however, the differences between the Core-Shell and Maxwell-Garnett/Bruggeman methods are usually larger than 15% in the ultraviolet and visible bands. A sensitivity test is conducted with the Beijing Climate Center Radiation transfer model (BCC-RAD) using a simulated BC concentration that is typical of east-central China and a sulfate volume ratio of 75%. The results show that the internal mixing methods could reduce the radiative flux more effectively because they produce a higher absorption. The annual mean instantaneous radiative force due to BC-sulfate aerosol is about -3.18 W/m2 for the external method and -6.91 W/m2 for the internal methods at the surface, and -3.03/-1.56/-1.85 W/m2 for the external/Core-Shell/(Maxwell-Garnett/Bruggeman) methods, respectively, at the tropopause.

Aerosol influence on energy balance of the middle atmosphere of Jupiter.

Science.gov (United States)

Zhang, Xi; West, Robert A; Irwin, Patrick G J; Nixon, Conor A; Yung, Yuk L

2015-12-22

Aerosols are ubiquitous in planetary atmospheres in the Solar System. However, radiative forcing on Jupiter has traditionally been attributed to solar heating and infrared cooling of gaseous constituents only, while the significance of aerosol radiative effects has been a long-standing controversy. Here we show, based on observations from the NASA spacecraft Voyager and Cassini, that gases alone cannot maintain the global energy balance in the middle atmosphere of Jupiter. Instead, a thick aerosol layer consisting of fluffy, fractal aggregate particles produced by photochemistry and auroral chemistry dominates the stratospheric radiative heating at middle and high latitudes, exceeding the local gas heating rate by a factor of 5-10. On a global average, aerosol heating is comparable to the gas contribution and aerosol cooling is more important than previously thought. We argue that fractal aggregate particles may also have a significant role in controlling the atmospheric radiative energy balance on other planets, as on Jupiter.

SAGE aerosol measurements. Volume 1, February 21, 1979 to December 31, 1979

International Nuclear Information System (INIS)

Mccormick, M.P.

1985-10-01

The Stratospheric Aerosol and Gas Experiment (SAGE) satellite system, launched on February 18, 1979, provides profiles of aerosol extinction, ozone concentration, and nitrogen dioxide concentration between about 80 N and 80 S. Zonal averages, separated into sunrise and sunset events, and seasonal averages of the aerosol extinction at 1.00 microns and 0.45 microns ratios of the aerosol extinction to the molecular extinction at 1.00 microns, and ratios of the aerosol extinction at 0.45 microns to the aerosol extinction at 1.00 microns are given. The averages for 1979 are shown in tables and in profile and contour plots (as a function of altitude and latitude). In addition, temperature data provided by the National Oceanic and Atmospheric Administration (NOAA) for the time and location of each SAGE measurement are averaged and shown in a similar format. Typical values of the peak aerosol extinction were 0.0001 to 0.0002 km at 1.00 microns depth values for the 1.00 microns channel varied between 0.001 and 0.002 over all latitudes

Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

Science.gov (United States)

Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

2017-12-01

The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

AOD distributions and trends of major aerosol species over a selection of the world’s most populated cities based on the 1st Version of NASA’s MERRA Aerosol Reanalysis

Science.gov (United States)

Provençal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

2018-01-01

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003–2015) and over a selection of 200 of the world’s most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don’t tend

Small molecules as tracers in atmospheric secondary organic aerosol

Science.gov (United States)

Yu, Ge

Secondary organic aerosol (SOA), formed from in-air oxidation of volatile organic compounds, greatly affects human health and climate. Although substantial research has been devoted to SOA formation and evolution, the modeled and lab-generated SOA are still low in mass and degree of oxidation compared to ambient measurements. In order to compensate for these discrepancies, the aqueous processing pathway has been brought to attention. The atmospheric waters serve as aqueous reaction media for dissolved organics to undergo further oxidation, oligomerization, or other functionalization reactions, which decreases the vapor pressure while increasing the oxidation state of carbon atoms. Field evidence for aqueous processing requires the identification of tracer products such as organosulfates. We synthesized the standards for two organosulfates, glycolic acid sulfate and lactic acid sulfate, in order to measure their aerosol-state concentration from five distinct locations via filter samples. The water-extracted filter samples were analyzed by LC-MS. Lactic acid sulfate and glycolic acid sulfate were detected in urban locations in the United States, Mexico City, and Pakistan with varied concentrations, indicating their potential as tracers. We studied the aqueous processing reaction between glyoxal and nitrogen-containing species such as ammonium and amines exclusively by NMR spectrometry. The reaction products formic acid and several imidazoles along with the quantified kinetics were reported. The brown carbon generated from these reactions were quantified optically by UV-Vis spectroscopy. The organic-phase reaction between oxygen molecule and alkenes photosensitized by alpha-dicarbonyls were studied in the same manner. We observed the fast kinetics transferring alkenes to epoxides under simulated sunlight. Statistical estimations indicate a very effective conversion of aerosol-phase alkenes to epoxides, potentially forming organosulfates in a deliquescence event and

TEM study of soot, organic aerosol, and sea-salt particles collected during CalNex

Science.gov (United States)

Adachi, K.; Buseck, P. R.

2010-12-01

Anthropogenic aerosol particles are emitted in abundance from megacities. Those particles can have important effects on both human health and climate. In this study, aerosol particles having aerodynamic diameters between 50 and 300 nm were collected during the CalNex campaign at the Pasadena ground site from May 15 to June 15, 2010, ~15 km northeast of downtown Los Angeles. The samples were analyzed using transmission electron microscopes (TEMs) to characterize particle shapes and compositions. Most samples are dominated by soot, organic aerosol (OA), sulfate, sea salt, or combinations thereof. Sizes and amounts of OA particles increased during the afternoons, and most soot particles were internally mixed with OA and sulfate in the afternoons. The proportion of soot to other material in individual particles increased and soot particles were more compact during the nights and early mornings. Sea-salt particles were commonly internally mixed with other materials. They have high Na contents with lesser N, Mg, S, K, and Ca and almost no Cl, suggesting that the Cl was replaced by sulfate or nitrate in the atmosphere. There is less OA and more sea salt and sulfate in the CalNex samples than in the samples from Mexico City that were collected during the MILAGRO campaign. Our study indicates that compositions of internally mixed aerosol particles and shapes of soot particles change significantly within a day. These changes probably influence the estimates of their effects on human health and climate.

Composite study of aerosol export events from East Asia and North America

Directory of Open Access Journals (Sweden)

Y. Luan

2013-02-01

Full Text Available We use satellite observations of aerosol optical depth (AOD from the Moderate Resolution Imaging Spectrometer (MODIS together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30% is found in the model fine mode AOD, particularly during summer. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-year study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward to the Arctic in 3–4 days, with the other crossing the Pacific Ocean in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High during spring and summer. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. This dipole structure during outflow events is a strong feature for all seasons except summer, when convection becomes more important. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a broad spring/summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO₂ from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow

Online Simulations of Global Aerosol Distributions in the NASA GEOS-4 Model and Comparisons to Satellite and Ground-Based Aerosol Optical Depth

Science.gov (United States)

Colarco, Peter; daSilva, Arlindo; Chin, Mian; Diehl, Thomas

2010-01-01

We have implemented a module for tropospheric aerosols (GO CART) online in the NASA Goddard Earth Observing System version 4 model and simulated global aerosol distributions for the period 2000-2006. The new online system offers several advantages over the previous offline version, providing a platform for aerosol data assimilation, aerosol-chemistry-climate interaction studies, and short-range chemical weather forecasting and climate prediction. We introduce as well a methodology for sampling model output consistently with satellite aerosol optical thickness (AOT) retrievals to facilitate model-satellite comparison. Our results are similar to the offline GOCART model and to the models participating in the AeroCom intercomparison. The simulated AOT has similar seasonal and regional variability and magnitude to Aerosol Robotic Network (AERONET), Moderate Resolution Imaging Spectroradiometer, and Multiangle Imaging Spectroradiometer observations. The model AOT and Angstrom parameter are consistently low relative to AERONET in biomass-burning-dominated regions, where emissions appear to be underestimated, consistent with the results of the offline GOCART model. In contrast, the model AOT is biased high in sulfate-dominated regions of North America and Europe. Our model-satellite comparison methodology shows that diurnal variability in aerosol loading is unimportant compared to sampling the model where the satellite has cloud-free observations, particularly in sulfate-dominated regions. Simulated sea salt burden and optical thickness are high by a factor of 2-3 relative to other models, and agreement between model and satellite over-ocean AOT is improved by reducing the model sea salt burden by a factor of 2. The best agreement in both AOT magnitude and variability occurs immediately downwind of the Saharan dust plume.

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

Science.gov (United States)

Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

Aerosol Formation during the Combustion of Straw with Addition of Sorbents

DEFF Research Database (Denmark)

Zeuthen, Frederik Jacob; Jensen, Peter Arendt; Jensen, Jørgen P.

2007-01-01

, calcium phosphate, Bentonite, ICA5000, and clay. The addition of chalk increased the aerosol mass concentration by 24%. Experiments in a laminar flow aerosol condenser with the six sorbents were carried out in the laboratory using a synthetic flue gas to avoid fluctuations in the alkali feeding......The influence of six sorbents on aerosol formation during the combustion of straw in a 100 MW boiler on a Danish power plant has been studied in full-scale. The following sorbents were studied: ammonium sulfate, monocalcium phosphate, Bentonite, ICA5000, clay, and chalk. Bentonite and ICA5000...... are mixtures of clay minerals and consist mainly of the oxides from Fe, Al, and Si. The straw used was Danish wheat and seed grass. Measurements were also made with increased flow of primary air. The experiments showed between 46% and 70% reduction in particle mass concentrations when adding ammonium sulfate...

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.

A polar stratospheric cloud parameterization for the global modeling initiative three-dimensional model and its response to stratospheric aircraft

International Nuclear Information System (INIS)

Considine, D. B.; Douglass, A. R.; Connell, P. S.; Kinnison, D. E.; Rotman, D. A.

2000-01-01

We describe a new parameterization of polar stratospheric clouds (PSCs) which was written for and incorporated into the three-dimensional (3-D) chemistry and transport model (CTM) developed for NASA's Atmospheric Effects of Aviation Project (AEAP) by the Global Modeling Initiative (GMI). The parameterization was designed to respond to changes in NO y and H 2 O produced by high-speed civilian transport (HSCT) emissions. The parameterization predicts surface area densities (SADs) of both Type 1 and Type 2 PSCs for use in heterogeneous chemistry calculations. Type 1 PSCs are assumed to have a supercooled ternary sulfate (STS) composition, and Type 2 PSCs are treated as water ice with a coexisting nitric acid trihydrate (NAT) phase. Sedimentation is treated by assuming that the PSC particles obey lognormal size distributions, resulting in a realistic mass flux of condensed phase H 2 O and HNO 3 . We examine a simulation of the Southern Hemisphere high-latitude lower stratosphere winter and spring seasons driven by temperature and wind fields from a modified version of the National Center for Atmospheric Research (NCAR) Middle Atmosphere Community Climate Model Version 2 (MACCM2). Predicted PSC SADs and median radii for both Type 1 and Type 2 PSCs are consistent with observations. Gas phase HNO 3 and H 2 O concentrations in the high-latitude lower stratosphere qualitatively agree with Cryogenic Limb Array Etalon Spectrometer (CLAES) HNO 3 and Microwave Limb Sounder (MLS) H 2 O observations. The residual denitrification and dehydration of the model polar vortex after polar winter compares well with atmospheric trace molecule spectroscopy (ATMOS) observations taken during November 1994. When the NO x and H 2 O emissions of a standard 500-aircraft HSCT fleet with a NO x emission index of 5 are added, NO x and H 2 O concentrations in the Southern Hemisphere polar vortex before winter increase by up to 3%. This results in earlier onset of PSC formation, denitrification, and

Aerosol composition and source apportionment in Santiago de Chile

International Nuclear Information System (INIS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-01-01

Santiago de Chile, Sao Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3 . Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10 ). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2 . In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of

The influence of different black carbon and sulfate mixing methods on their optical and radiative properties

International Nuclear Information System (INIS)

Zhang, Hua; Zhou, Chen; Wang, Zhili; Zhao, Shuyun; Li, Jiangnan

2015-01-01

Three different internal mixing methods (Core–Shell, Maxwell-Garnett, and Bruggeman) and one external mixing method are used to study the impact of mixing methods of black carbon (BC) with sulfate aerosol on their optical properties, radiative flux, and heating rate. The optical properties of a mixture of BC and sulfate aerosol particles are considered for three typical bands. The results show that mixing methods, the volume ratio of BC to sulfate, and relative humidity have a strong influence on the optical properties of mixed aerosols. Compared to internal mixing, external mixing underestimates the particle mass absorption coefficient by 20–70% and the particle mass scattering coefficient by up to 50%, whereas it overestimates the particle single scattering albedo by 20–50% in most cases. However, the asymmetry parameter is strongly sensitive to the equivalent particle radius, but is only weakly sensitive to the different mixing methods. Of the internal methods, there is less than 2% difference in all optical properties between the Maxwell-Garnett and Bruggeman methods in all bands; however, the differences between the Core–Shell and Maxwell-Garnett/Bruggeman methods are usually larger than 15% in the ultraviolet and visible bands. A sensitivity test is conducted with the Beijing Climate Center Radiation transfer model (BCC-RAD) using a simulated BC concentration that is typical of east-central China and a sulfate volume ratio of 75%. The results show that the internal mixing methods could reduce the radiative flux more effectively because they produce a higher absorption. The annual mean instantaneous radiative force due to BC–sulfate aerosol is about –3.18 W/m 2 for the external method and –6.91 W/m 2 for the internal methods at the surface, and –3.03/–1.56/–1.85 W/m 2 for the external/Core–Shell/(Maxwell-Garnett/Bruggeman) methods, respectively, at the tropopause. - Highlights: • The aerosol optical properties with different mixing

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

Directory of Open Access Journals (Sweden)

L. Marelle

2017-10-01

Full Text Available In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols (1 a correction to the sedimentation of aerosols, (2 dimethyl sulfide (DMS oceanic emissions and gas-phase chemistry, (3 an improved representation of the dry deposition of trace gases over seasonal snow, and (4 an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5 correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6 couple and further test the recent KF-CuP (Kain–Fritsch + Cumulus Potential cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC, sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone, the improved surface temperatures over sea ice (surface ozone, BC, and sulfate, and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone. DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

Long-term changes of the upper stratosphere as seen by Japanese rocketsondes at Ryori (39°N, 141°E

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P. Keckhut

1999-09-01

Full Text Available Wind and temperature profiles measured routinely by rockets at Ryori (Japan since 1970 are analysed to quantify interannual changes that occur in the upper stratosphere. The analysis involved using a least square fitting of the data with a multiparametric adaptative model composed of a linear combination of some functions that represent the main expected climate forcing responses of the stratosphere. These functions are seasonal cycles, solar activity changes, stratospheric optical depth induced by volcanic aerosols, equatorial wind oscillations and a possible linear trend. Step functions are also included in the analyses to take into account instrumental changes. Results reveal a small change for wind data series above 45 km when new corrections were introduced to take into account instrumental changes. However, no significant change of the mean is noted for temperature even after sondes were improved. While wind series reveal no significant trends, a significant cooling of 2.0 to 2.5 K/decade is observed in the mid upper stratosphere using this analysis method. This cooling is more than double the cooling predicted by models by a factor of more than two. In winter, it may be noted that the amplitude of the atmospheric response is enhanced. This is probably caused by the larger ozone depletion and/or by some dynamical feedback effects. In winter, cooling tends to be smaller around 40-45 km (in fact a warming trend is observed in December as already observed in other data sets and simulated by models. Although the winter response to volcanic aerosols is in good agreement with numerical simulations, the solar signature is of the opposite sign to that expected. This is not understood, but it has already been observed with other data sets.Key words. Atmospheric composition and structure (evolution of one atmosphere; pressure · density · and temperature · Meteorology and atmospheric dynamics (middle atmosphere dynamics

Linking remotely sensed aerosol types to their chemical composition

Science.gov (United States)

Dawson, K. W.; Kacenelenbogen, M. S.; Johnson, M. S.; Burton, S. P.; Hostetler, C. A.; Meskhidze, N.

2016-12-01

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% ± 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into `dark' and `light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

Aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing in Guangzhou during the 2006 Pearl River Delta campaign.

Science.gov (United States)

Jung, Jinsang; Lee, Hanlim; Kim, Young J; Liu, Xingang; Zhang, Yuanhang; Gu, Jianwei; Fan, Shaojia

2009-08-01

Optical and chemical aerosol measurements were obtained from 2 to 31 July 2006 at an urban site in the metropolitan area of Guangzhou (China) as part of the Program of Regional Integrated Experiment of Air Quality over Pearl River Delta (PRIDE-PRD2006) to investigate aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing. During the PRIDE-PRD2006 campaign, the average contributions of ammonium sulfate, organic mass by carbon (OMC), elemental carbon (EC), and sea salt (SS) to total PM(2.5) mass were measured to be 36.5%, 5.7%, 27.1%, 7.8%, and 3.7%, respectively. Compared with the clean marine period, (NH(4))(2)SO(4), NH(4)NO(3), and OMC were all greatly enhanced (by up to 430%) during local haze periods via the accumulation of a secondary aerosol component. The OMC dominance increased when high levels of biomass burning influenced the measurement site while (NH(4))(2)SO(4) and OMC did when both biomass burning and industrial emissions influenced it. The effect of aerosol water content on the total light-extinction coefficient was estimated to be 34.2%, of which 25.8% was due to aerosol water in (NH(4))(2)SO(4), 5.1% that in NH(4)NO(3), and 3.3% that in SS. The average mass-scattering efficiency (MSE) of PM(10) particles was determined to be 2.2+/-0.6 and 4.6+/-1.7m(2)g(-1) under dry (RHwater content, but MSE and SSA are also highly sensitive. It can be concluded that sulfate and carbonaceous aerosol, as well as aerosol water content, play important roles in the processes that determine visibility impairment and radiative forcing in the ambient atmosphere of the Guangzhou urban area.

Increases to Biogenic Secondary Organic Aerosols from SO2 and NOx in the Southeastern US

Science.gov (United States)

Russell, L. M.; Liu, J.; Ruggeri, G.; Takahama, S.; Claflin, M. S.; Ziemann, P. J.; Lee, A.; Murphy, B.; Pye, H. O. T.; Ng, N. L.; McKinney, K. A.; Surratt, J. D.

2017-12-01

During the 2013 Southern Oxidant and Aerosol Study, Fourier Transform Infrared Spectroscopy (FTIR) and Aerosol Mass Spectrometer (AMS) measurements of submicron mass were collected at Look Rock, Tennessee, and Centreville, Alabama. The low NOx, low wind, little rain, and increased daytime isoprene emissions led to multi-day stagnation events at Look Rock that provided clear evidence of particle-phase sulfate enhancing biogenic secondary organic aerosol (bSOA) by selective uptake. Organic mass (OM) sources were apportioned as 42% "vehicle-related" and 54% bSOA, with the latter including "sulfate-related bSOA" that correlated to sulfate (r=0.72) and "nitrate-related bSOA" that correlated to nitrate (r=0.65). Single-particle mass spectra showed three composition types that corresponded to the mass-based factors with spectra cosine similarity of 0.93 and time series correlations of r>0.4. The vehicle-related OM with m/z 44 was correlated to black carbon, "sulfate-related bSOA" was on particles with high sulfate, and "nitrate-related bSOA" was on all particles. The similarity of the m/z spectra (cosine similarity=0.97) and the time series correlation (r=0.80) of the "sulfate-related bSOA" to the sulfate-containing single-particle type provide evidence for particle composition contributing to selective uptake of isoprene oxidation products onto particles that contain sulfate from power plants. Since Look Rock had much less NOx than Centreville, comparing the bSOA at the two sites provides an evaluation of the role of NOx for bSOA. CO and submicron sulfate and OM concentrations were 15-60 % higher at Centreville than at Look Rock but their time series had moderate correlations of r= 0.51, 0.54, and 0.47, respectively. However, NOx had no correlation (r=0.08) between the two sites. OM correlated with the higher NOx levels at Centreville but with O3 at Look Rock. OM sources identified by Positive Matrix Factorization had three very similar factors at both sites from FTIR

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

Science.gov (United States)

Hattori, Shohei; Schmidt, Johan A.; Johnson, Matthew S.; Danielache, Sebastian O.; Yamada, Akinori; Ueno, Yuichiro; Yoshida, Naohiro

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, but the concentration of glacial sulfate does not distinguish between tropospheric and stratospheric eruptions. Stable sulfur isotope abundances contain additional information, and recent studies show a correlation between volcanic plumes that reach the stratosphere and mass-independent anomalies in sulfur isotopes in glacial sulfate. We describe a mechanism, photoexcitation of SO2, that links the two, yielding a useful metric of the explosivity of historic volcanic events. A plume model of S(IV) to S(VI) conversion was constructed including photochemistry, entrainment of background air, and sulfate deposition. Isotopologue-specific photoexcitation rates were calculated based on the UV absorption cross-sections of 32SO2, 33SO2, 34SO2, and 36SO2 from 250 to 320 nm. The model shows that UV photoexcitation is enhanced with altitude, whereas mass-dependent oxidation, such as SO2 + OH, is suppressed by in situ 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 Δ33S/δ34S and Δ36S/Δ33S found in glacial samples. We are able to identify the process controlling mass-independent sulfur isotope anomalies in the modern atmosphere. This mechanism is the basis of identifying the magnitude of historic volcanic events. PMID:23417298

Presence of PAH or HAC below 900 km in the Titan's stratosphere?

Science.gov (United States)

Cordier, Daniel; COURS, Thibaud; Rey, Michael; Maltagliati, Luca; Seignovert, Benoit; Biennier, Ludovic

2016-10-01

In 2006, during Cassini's 10th flyby of Titan (T10), Bellucci et al. (2009) observed a solar occultation by Titan's atmosphere through the solar port of the Cassini/VIMS instrument. These authors noticed the existence of an unexplained additional absorption superimposed to the CH4 3.3 microns band. Because they were unable to model this absorption with gases, they attributed this intriguing feature to the signature of solid state organic components. Kim et al. (2011) revisited the data collected by Bellucci et al. (2009) and they considered the possible contribution of aerosols formed by hydrocarbon ices. They specifically took into account C2H6, CH4, CH3CN, C5H12 and C6H12 ices. More recently, Maltagliati et al. (2015) analyzed a set of four VIMS solar occultations, corresponding to flybys performed between January 2006 and September 2011 at different latitudes. They confirmed the presence of the 3.3 µm absorption in all occultations and underlined the possible importance of gaseous ethane, which has a strong plateau of absorption lines in that wavelength range. In this work, we show that neither hydrocarbon ices nor molecular C2H6 cannot satisfactorily explain the observed absorption. Our simulations speak in favor of an absorption due to the presence of PAH molecules or HAC in the stratosphere of Titan. PAH have been already considered by Lopes-Puertas et al. (2013) at altitudes larger than ~900 km and tentatively identified in the stratosphere by Maltagliati et al. (2015); PAH and HAC are good candidates for Titan's aerosols precursors.

Intercontinental Transport of Aerosols: Implication for Regional Air Quality

Science.gov (United States)

Chin, Mian; Diehl, Thomas; Ginoux, Paul

2006-01-01

Aerosol particles, also known as PM2.5 (particle diameter less than 2.5 microns) and PM10 (particle diameter less than 10 microns), is one of the key atmospheric components that determine ambient air quality. Current US air quality standards for PM10 (particles with diameter air pollution problems, aerosols can be transported on a hemispheric or global scale. In this study, we use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to quantify contributions of long-range transport vs. local/regional pollution sources and from natural vs. anthropogenic sources to PM concentrations different regions. In particular, we estimate the hemispheric impact of anthropogenic sulfate aerosols and dust from major source areas on other regions in the world. The GOCART model results are compared with satellite remote sensing and ground-based network measurements of aerosol optical depth and concentrations.

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

Directory of Open Access Journals (Sweden)

X. Wang

2017-10-01

Full Text Available Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA and mixed particles composed of ammonium sulfate (AS and OA with different organic to inorganic molar ratios (OIRs have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH, and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH for mixed OA ∕ AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH of AS in mixed OA ∕ AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA ∕ AS droplets indicate the formation of ammonium hydrogen oxalate (NH4HC2O4 and ammonium hydrogen sulfate (NH4HSO4 from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA ∕ AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH42SO4 into NH4HC2O4 with a high DRH. Although the hygroscopic growth of mixed OA�

Isolating the Roles of Different Forcing Agents in Global Stratospheric Temperature Changes Using Model Integrations with Incrementally Added Single Forcings

Science.gov (United States)

Aquila, V.; Swartz, W. H.; Waugh, D. W.; Colarco, P. R.; Pawson, S.; Polvani, L. M.; Stolarski, R. S.

2016-01-01

Satellite instruments show a cooling of global stratospheric temperatures over the whole data record (1979-2014). This cooling is not linear and includes two descending steps in the early 1980s and mid-1990s. The 1979-1995 period is characterized by increasing concentrations of ozone depleting substances (ODS) and by the two major volcanic eruptions of El Chichon (1982) and Mount Pinatubo (1991). The 1995-present period is characterized by decreasing ODS concentrations and by the absence of major volcanic eruptions. Greenhouse gas (GHG) concentrations increase over the whole time period. In order to isolate the roles of different forcing agents in the global stratospheric temperature changes, we performed a set of AMIP-style simulations using the NASA Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). We find that in our model simulations the cooling of the stratosphere from 1979 to present is mostly driven by changes in GHG concentrations in the middle and upper stratosphere and by GHG and ODS changes in the lower stratosphere. While the cooling trend caused by increasing GHGs is roughly constant over the satellite era, changing ODS concentrations cause a significant stratospheric cooling only up to the mid-1990s, when they start to decrease because of the implementation of the Montreal Protocol. Sporadic volcanic events and the solar cycle have a distinct signature in the time series of stratospheric temperature anomalies but do not play a statistically significant role in the long-term trends from 1979 to 2014. Several factors combine to produce the step-like behavior in the stratospheric temperatures: in the lower stratosphere, the flattening starting in the mid-1990s is due to the decrease in ozone-depleting substances; Mount Pinatubo and the solar cycle cause the abrupt steps through the aerosol-associated warming and the volcanically induced ozone depletion. In the middle and upper stratosphere, changes in solar irradiance are largely

Interim Proposal for Molecular Beam Studies of Surfactants in Sulfuric Acid Aerosols: Comparisons Between Hydrocarbon and Fluorocarbon Alcohols

National Research Council Canada - National Science Library

Nathanson, Gilbert

2003-01-01

.... These processes include the acid-catalyzed reactions of HCI and HBr with CIONO2 (BrONO2) and HOCI (HOBr) to generate photoactive halogen molecules, particularly in colder regions of the stratosphere where they are more soluble in the water-rich aerosols...

Composition and sources of winter and summertime aerosols at Ny Alesund, Spitsbergen

International Nuclear Information System (INIS)

Maenhaut, W.; Cornille, P.; Pacyna, J.M.

1991-01-01

Filter samples of < 2.5 μm aerosol were collected in (late) winter of 1983, 1984, 1986, and 1987 and in the summer of 1984, 1986, and 1987 at Ny Alesund, Spitsbergen, and analyzed for over 40 elements by a combination of INAA and PIXE. The data sets of the various sampling campaigns and the combined winter and combined summer data were examined by receptor modeling, including absolute principal component analysis (APCA), chemical mass balance (CMB) and multiple linear regression (MLR) techniques. APCA yielded four components, both for the winter and for the summer aerosol. For the winter aerosol, the components were identified as a general pollution component, crustal dust, sea-salt, and a halogen (Br,I) component. The CMB and MLR calculations were used to obtain source (source region) apportionments for the anthropogenic trace elements and for sulfate. For the summer, about 50% of the sulfate was attributed to a marine biogenic source

Impact of palmitic acid coating on the water uptake and loss of ammonium sulfate particles

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R. M. Garland

2005-01-01

Full Text Available While water insoluble organics are prevalent in the atmosphere, it is not clear how the presence of such species alters the chemical and physical properties of atmospheric aerosols. Here we use a combination of FTIR spectroscopy, Transmission Electron Microscopy (TEM and Aerosol Mass Spectrometry (AMS to characterize ammonium sulfate particles coated with palmitic acid. Coated aerosols were generated by atomizing pure ammonium sulfate, mixing the particles with a heated flow of nitrogen with palmitic acid vapor, and then flowing the mixture through an in-line oven to create internally mixed particles. The mixing state of the particles was probed using the AMS data and images from the TEM. Both of these probes suggest that the particles were internally mixed. Water uptake by the mixed particles was then probed at 273 K. It was found that for ammonium sulfate containing ~20 wt% palmitic acid the deliquescence relative humidity (DRH was the same as for pure ammonium sulfate (80±3% RH. For particles with ~50 wt% palmitic acid however, the mixed particles began to take up water at relative humidities as low at 69% and continued to slowly take up water to 85% RH without fully deliquescing. In addition to studies of water uptake, water loss was also investigated. Here coatings of up to 50 wt% had no impact on the efflorescence relative humidity. These studies suggest that even if insoluble substances coat salt particles in the atmosphere, there may be relatively little effect on the resulting water uptake and loss.

Characterization of aerosol over the Northern South China Sea during two cruises in 2003

Science.gov (United States)

Zhang, Xingying; Zhuang, Guoshun; Guo, Jinghua; Yin, Kedong; Zhang, Peng

Atmospheric transport of trace elements has been found to be an important pathway for their input to the ocean. TSP, PM10, and PM2.5 aerosol samples were collected over the Northern South China Sea in two cruises in 2003 to estimate the input of aerosol from continent to the ocean. About 23 elements and 14 soluble ions in aerosol samples were measured. The average mass concentration of TSP in Cruise I in January (78 μg m -3) was ˜twice of that in Cruise II in April (37 μg m -3). Together with the crustal component, heavy metals from pollution sources over the land (especially from the industry and automobiles in Guangzhou) were transported to and deposited into the ocean. The atmospheric MSA concentrations in PM2.5 (0.048 μg m -3 in Cruise I and 0.043 μg m -3 in Cruise II) over Northern South China Sea were comparable to those over other coastal regions. The ratio of non-sea-salt (NSS)-sulfate to MSA is 103-655 for Cruise I and 15-440 for Cruise II in PM2.5 samples, which were much higher than those over remote oceans. The estimated anthropogenic sulfate accounts for 83-98% in Cruise I and 63-95% in Cruise II of the total NSS-sulfate. Fe (II) concentration in the aerosols collected over the ocean ranged from 0.1 to 0.9 μg m -3, accounting for 16-82% of the total iron in the aerosol, which could affect the marine biogeochemical cycle greatly.

Source apportionment of size and time resolved trace elements and organic aerosols from an urban courtyard site in Switzerland

Science.gov (United States)

Richard, A.; Gianini, M. F. D.; Mohr, C.; Furger, M.; Bukowiecki, N.; Minguillón, M. C.; Lienemann, P.; Flechsig, U.; Appel, K.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Baltensperger, U.; Prévôt, A. S. H.

2011-09-01

Time and size resolved data of trace elements were obtained from measurements with a rotating drum impactor (RDI) and subsequent X-ray fluorescence spectrometry. Trace elements can act as indicators for the identification of sources of particulate matter Switzerland. Eight different sources were identified for the three examined size ranges (PM1-0.1, PM2.5-1 and PM10-2.5): secondary sulfate, wood combustion, fire works, road traffic, mineral dust, de-icing salt, industrial and local anthropogenic activities. The major component was secondary sulfate for the smallest size range; the road traffic factor was found in all three size ranges. This trace element analysis is complemented with data from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS), assessing the PM1 fraction of organic aerosols. A separate PMF analysis revealed three factors related to three of the sources found with the RDI: oxygenated organic aerosol (OOA, related to inorganic secondary sulfate), hydrocarbon-like organic aerosol (HOA, related to road traffic) and biomass burning organic aerosol (BBOA), explaining 60 %, 22 % and 17 % of total measured organics, respectively. Since different compounds are used for the source classification, a higher percentage of the ambient PM10 mass concentration can be apportioned to sources by the combination of both methods.

A review of optical measurements at the aerosol and cloud chamber AIDA

International Nuclear Information System (INIS)

Wagner, Robert; Linke, Claudia; Naumann, Karl-Heinz; Schnaiter, Martin; Vragel, Marlen; Gangl, Martin; Horvath, Helmuth

2009-01-01

This paper provides a survey of recent studies on the optical properties of aerosol and cloud particles that have been conducted at the AIDA facility of Forschungszentrum Karlsruhe (Aerosol Interactions and Dynamics in the Atmosphere). Reflecting the broad accessible temperature range of the AIDA chamber which extends from ambient temperature down to 183 K, the investigations feature a broad diversity of research topics, such as the wavelength-dependence of the specific absorption cross sections of soot and mineral dust aerosols at room temperature, depolarization and infrared extinction measurements of ice crystal clouds generated at temperatures below 235 K, and the optical properties of polar stratospheric cloud constituents whose formation was studied in chamber experiments at temperatures well below 200 K. After reviewing the AIDA research activity of the past decade and introducing the optical instrumentation of the AIDA facility, this paper presents illustrative examples of ongoing and already published work on optical measurements of soot aerosols, mineral dust particles, and ice crystal clouds.

Lipid organics in background aerosols, cloudwater, and snow and implication for organic scavenging

International Nuclear Information System (INIS)

Groellert, C.

1998-01-01

During three years free tropospheric snow, aerosol, and cloudwater samples were collected at Mount Sonnblick, Austria, at an elevation of 3106 m a.s.l. The samples were analyzed for their lipid organic trace components using extraction with n-hexane as sample pretreatment and gas chromatography-mass spectrometry-flame ionization detection for identification and quantification of the substances. The main components identified in all the samples were the phthalic acid esters which are of anthropogenic origin. Of further interest were aliphatic alcohols (not detected in aerosols) and phenols. They are of biogenic origin. The concentrations were found to be higher in spring than in the fall season. To compare the concentrations of aerosol, cloudwater and snow samples scavenging ratios (aerosol to snow), scavenging efficiencies (aerosol to cloud) and cloud to snow ratios were calculated for the first time for organic compounds. Scavenging ratios were 10 to 100 times lower, scavenging efficiencies 2 to 10 times lower than sulfate. This can result from the poor watersolubility of the compounds or from gas phase sorptions on the filter surface (overestimation of aerosol concentrations). The cloud to snow ratios were generally higher than for sulfate. However, a few components exhibited very low cloud to snow ratios which might be due to additional sources in snow for these substances (alcohols). (author)

In vitro tests for aerosol deposition. III: effect of inhaler insertion angle on aerosol deposition.

Science.gov (United States)

Delvadia, Renish R; Longest, P Worth; Hindle, Michael; Byron, Peter R

2013-06-01

Inhaler orientation with respect to a patient's mouth may be an important variable determining the efficiency of aerosol lung delivery. The effect of insertion angle on regional deposition was evaluated for a series of inhalers using concurrent in vitro and computational fluid dynamics (CFD) analysis. Geometrically realistic physical mouth-throat (MT) and upper tracheobronchial (TB) models were constructed to connect different inhalers at a series of insertion angles relative to the horizontal plane of the model. These models were used to assess albuterol sulfate deposition from the Novolizer(®) dry powder inhaler (DPI), Proventil(®) HFA pressurized metered dose inhaler (MDI), and Respimat(®) Soft Mist™ Inhaler (SMI) following the actuation of a single dose. Drug deposition from Novolizer DPI was studied for Salbulin(®) and an experimental "drug only" formulation. Albuterol sulfate was recovered and quantified from the device and the MT and TB regions. Significant differences in MT and total lung dose (TLD) of albuterol sulfate deposition were not observed for Salbulin Novolizer DPI and Respimat SMI inserted at different angles. In contrast, drug-only Novolizer DPI and Proventil HFA MDI showed a significant difference in MT and TLD deposition using different insertion angles. For drug-only Novolizer DPI and Proventil HFA MDI, the lowest and the highest MT depositions were observed at +10° and -20°, respectively; for Respimat SMI and Salbulin Novolizer DPI, these angles were -10° and +10°, and +20° and -20°, respectively. CFD simulations were in agreement with the experimental results and illustrated shifts in local particle deposition associated with changes in insertion angle. The effect of inhaler orientation at the inhaler-mouth interface on MT aerosol deposition appeared to be dependent on velocity, aerosol size, and formulation. These findings not only demonstrate the need for patient education on correct inhaler orientation, but provide important

Direct Observations of Isoprene Secondary Organic Aerosol Formation in Ambient Cloud Droplets

Science.gov (United States)

Zelenyuk, A.; Bell, D.; Thornton, J. A.; Fast, J. D.; Shrivastava, M. B.; Berg, L. K.; Imre, D. G.; Mei, F.; Shilling, J.; Suski, K. J.; Liu, J.; Tomlinson, J. M.; Wang, J.

2017-12-01

Multiphase chemistry of isoprene photooxidation products has been shown to be one of the major sources of secondary organic aerosol (SOA) in the atmosphere. A number of recent studies indicate that aqueous aerosol phase provides a medium for reactive uptake of isoprene photooxidation products, and in particular, isomeric isoprene epoxydiols (IEPOX), with reaction rates and yields being dependent on aerosol acidity, water content, sulfate concentration, and organic coatings. However, very few studies focused on chemistry occurring within actual cloud droplets. We will present data acquired during recent Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) Campaign, which provide direct evidence for IEPOX-SOA formation in cloud droplets. Single particle mass spectrometer, miniSPLAT, and a high-resolution, time-of-flight aerosol mass spectrometer were used to characterize the composition of aerosol particles and cloud droplet residuals, while a high-resolution, time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) was used to characterize gas-phase compounds. We find that the composition of cloud droplet residuals was markedly different than that of aerosol particles sampled outside the cloud. Cloud droplet residuals were comprised of individual particles with high relative fractions of sulfate and nitrate and significant fraction of particles with mass spectra that are nearly identical to those of laboratory-generated IEPOX-SOA particles. The observed cloud-induced formation of IEPOX-SOA was accompanied by simultaneous decrease in measured concentrations of IEPOX and other gas-phase isoprene photooxidation products. Ultimately, the combined cloud, aerosol, and gas-phase measurements conducted during HI-SCALE will be used to develop and evaluate model treatments of aqueous-phase isoprene SOA formation.

Effects of Greenhouse Gas Increase and Stratospheric Ozone Depletion on Stratospheric Mean Age of Air in 1960-2010

Science.gov (United States)

Li, F.; Newman, P. A.; Pawson, S.; Perlwitz, J.

2017-12-01

The strength of the stratospheric Brewer-Dobson circulation (BDC) in a changing climate has been extensively studied, but the relative importance of greenhouse gas (GHG) increases and stratospheric ozone depletion in driving the BDC changes remains uncertain. This study separates the impacts of GHG and stratospheric ozone forcings on stratospheric mean age of air in the 1960-2010 period using the Goddard Earth Observing System Model (GEOS) Chemistry-Climate Model (CCM). The experiment compares a set of controlled simulations using a coupled atmosphere-ocean version of the GEOS CCM, in which either GHGs, or stratospheric ozone, or both factors evolve over time. The model results show that GHGs and stratospheric ozone have about equal contributions to the simulated mean age decrease. It is also found that GHG increases account for about two thirds of the enhanced strength of the lower stratospheric residual circulation. The results show that ozone depletion causes an increase in the mean age of air in the Antarctic summer lower stratosphere through two processes: 1) a seasonal delay in the Antarctic polar vortex breakup, that inhibits young mid-latitude air from mixing with the older air inside the vortex; and 2) enhanced Antarctic downwelling, that brings older air from middle and upper stratosphere into the lower stratosphere.

Aircraft measurements over Europe of an air pollution plume from Southeast Asia – aerosol and chemical characterization

Directory of Open Access Journals (Sweden)

A. Stohl

2007-01-01

.70 Mm−1, as was the fraction of non-volatile Aitken particles. This indicates that black carbon (BC was an important aerosol component. During the flight on 25 March, which took place on the rear of a trough located over Europe, a mixture of Asian pollution and stratospheric air was found. Asian pollution was mixing into the lower stratosphere, and stratospheric air was mixing into the pollution plume in the troposphere. Turbulence was encountered by the aircraft in the mixing regions, where the thermal stability was low and Richardson numbers were below 0.2. The result of the mixing can clearly be seen in the trace gas data, which are following mixing lines in correlation plots. This mixing with stratospheric air is likely very typical of Asian air pollution, which is often lifted to the upper troposphere and, thus, transported in the vicinity of stratospheric air.

On the contribution of organics to the North East Atlantic aerosol number concentration

International Nuclear Information System (INIS)

Bialek, Jakub; Dall’Osto, Manuel; Monahan, Ciaran; O’Dowd, Colin; Beddows, David

2012-01-01

k-means statistical-cluster analysis of submicron aerosol size distributions is combined with coincident humidity tandem differential mobility analyser data, leading to five unique aerosol categories for hygroscopic growth factors (HGFs): low sea-salt background marine, high sea-salt background marine, coastal nucleation, open ocean nucleation and anthropogenically influenced scenarios. When considering only marine conditions, and generic aerosol species associated with this environment (e.g. non-sea-salt sulfate, sea-salt, partly soluble organic matter and water insoluble organic matter), the two-year annual average contribution to aerosol number concentration from the different generic species was made up as follows: 46% (30–54%) of partially modified ammonium sulfate particles; 23% (11–40%) of partially modified sea-salt; and the remaining 31% (25–35%) contribution attributed to two distinct organic species as evidenced by different, but low, HGFs. The analysis reveals that on annual timescales, ∼30% of the submicron marine aerosol number concentration is sourced from predominantly organic aerosol while 60% of the anthropogenic aerosol number is predominantly organic. Coastal nucleation events show the highest contribution of the lowest HGF mode (1.19), although this contribution is more likely to be influenced by inorganic iodine oxides. While organic mass internally mixed with inorganic salts will lower the activation potential of these mixed aerosol types, thereby potentially reducing the concentration of cloud condensation nuclei (CCN), pure organic water soluble particles are still likely to be activated into cloud droplets, thereby increasing the concentration of CCN. A combination of dynamics and aerosol concentrations will determine which effect will prevail under given conditions. (letter)