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Sample records for aerosol chemical transport

  1. Parameterization of Aerosol Sinks in Chemical Transport Models

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2012-01-01

    The modelers point of view is that the aerosol problem is one of sources, evolution, and sinks. Relative to evolution and sink processes, enormous attention is given to the problem of aerosols sources, whether inventory based (e.g., fossil fuel emissions) or dynamic (e.g., dust, sea salt, biomass burning). On the other hand, aerosol losses in models are a major factor in controlling the aerosol distribution and lifetime. Here we shine some light on how aerosol sinks are treated in modern chemical transport models. We discuss the mechanisms of dry and wet loss processes and the parameterizations for those processes in a single model (GEOS-5). We survey the literature of other modeling studies. We additionally compare the budgets of aerosol losses in several of the ICAP models.

  2. REPRESENTING AEROSOL DYNAMICS AND PROPERTIES IN CHEMICAL TRANSPORT MODELS BY THE METHOD OF MOMENTS.

    SciTech Connect

    SCHWARTZ, S.E.; MCGRAW, R.; BENKOVITZ, C.M.; WRIGHT, D.L.

    2001-04-01

    Atmospheric aerosols, suspensions of solid or liquid particles, are an important multi-phase system. Aerosols scatter and absorb shortwave (solar) radiation, affecting climate (Charlson et al., 1992; Schwartz, 1996) and visibility; nucleate cloud droplet formation, modifying the reflectivity of clouds (Twomey et al., 1984; Schwartz and Slingo, 1996) as well as contributing to composition of cloudwater and to wet deposition (Seinfeld and Pandis, 1998); and affect human health through inhalation (NRC, 1998). Existing and prospective air quality regulations impose standards on concentrations of atmospheric aerosols to protect human health and welfare (EPA, 1998). Chemical transport and transformation models representing the loading and geographical distribution of aerosols and precursor gases are needed to permit development of effective and efficient strategies for meeting air quality standards, and for examining aerosol effects on climate retrospectively and prospectively for different emissions scenarios. Important aerosol properties and processes depend on their size distribution: light scattering, cloud nucleating properties, dry deposition, and penetration into airways of lungs. The evolution of the mass loading itself depends on particle size because of the size dependence of growth and removal processes. For these reasons it is increasingly recognized that chemical transport and transformation models must represent not just the mass loading of atmospheric particulate matter but also the aerosol microphysical properties and the evolution of these properties if aerosols are to be accurately represented in these models. If the size distribution of the aerosol is known, a given property can be evaluated as the integral of the appropriate kernel function over the size distribution. This has motivated the approach of determining aerosol size distribution, and of explicitly representing this distribution and its evolution in chemical transport models.

  3. Validation of the assimilation of satellite-based aerosol measurements into a chemical transport model using aerosol component information

    NASA Astrophysics Data System (ADS)

    Martynenko, Dmytro; Holzer-Popp, Thomas; Schroedter-Homscheidt, Marion

    Aerosol monitoring is of growing interest due to the impact of aerosol particle concentration on human health and the global climate. The key question of this paper is to understand how the assimilation of satellite atmospheric aerosol observations with enhanced observation and background covariance matrices improves the capability of a chemical transport model in reproducing the distribution of tropospheric particles. The task of this study is a validation of assimilation results by using ground-based AERONET measurements for 2006-2008 at stations from Europe and Africa regions. The study is carried out using the Model for Atmospheric Transport and Chemistry (MATCH operated at DLR). As measurement input vector for as-similation satellite data from SCIAMACHY and AATSR instruments onboard ENVISAT was used. Synergetic Aerosol Retrieval (SYNAER) observational and model data have been cou-pled by means of data the two-dimensional variational assimilation. SYNAER measurements are able to distinguish between different aerosol components such as water-soluble, soot, sea salt and long-range transported mineral aerosols. The final analysis is highly dependent on the specification of the error covariance matrices. Since observation and background error covari-ance matrices are not perfectly known, a large potential for improvements of the analyses is offered by methods allowing their constructing and tuning. In this study, a method proposed by Desroziers and Ivanov (2001) is used to tune background and observational error statistics of the 2D-Var assimilation procedure by using information content analysis of the retrieval algorithm.

  4. Aerosols and clouds in chemical transport models and climate models.

    SciTech Connect

    Lohmann,U.; Schwartz, S. E.

    2008-03-02

    Clouds exert major influences on both shortwave and longwave radiation as well as on the hydrological cycle. Accurate representation of clouds in climate models is a major unsolved problem because of high sensitivity of radiation and hydrology to cloud properties and processes, incomplete understanding of these processes, and the wide range of length scales over which these processes occur. Small changes in the amount, altitude, physical thickness, and/or microphysical properties of clouds due to human influences can exert changes in Earth's radiation budget that are comparable to the radiative forcing by anthropogenic greenhouse gases, thus either partly offsetting or enhancing the warming due to these gases. Because clouds form on aerosol particles, changes in the amount and/or composition of aerosols affect clouds in a variety of ways. The forcing of the radiation balance due to aerosol-cloud interactions (indirect aerosol effect) has large uncertainties because a variety of important processes are not well understood precluding their accurate representation in models.

  5. Application of Aerosol Assimilation System of MODIS Radiances to Regional Chemical Transport Model

    NASA Astrophysics Data System (ADS)

    D'Allura, A.; Charmichael, G. R.; Tang, Y.; Chai, T.; Chung, C. E.; Anderson, T. L.

    2006-12-01

    We present results from an assimilation system of radiances from the MODIS channels that sense atmospheric aerosols over land and ocean on the chemical transport model STEM. A test case is designed to simulate transport of aerosols tracers over the area of interest which includes India, east and south Asia at 50km horizontal resolution. A detailed treatment of the source, transport and deposition of the aerosol species are included. The model simulates five aerosol components: sulfate, organic carbon, black carbon, dust and sea salt. Total AODs at 550nm wavelength over land and ocean and fine mode AODs at 550nm wavelength over ocean are the level 2 aerosol products from Terra MODIS channel four used in this application. The intent of the study is to verify the improvement in the model performances while the initial conditions are corrected using an Optimum Interpolation technique to assimilate the MODIS data. The model results are compared with ground-based measurements of aerosol optical depth (AOD) from the AERONET network. Sensitivity analyses are provided in order to describe the effect of changing in assimilation technique's free parameters. The method is designed to optimize the use of the information provided by fine mode AODs, which are available over ocean, coupled with the total AODs available also over land. Improvements on the model results using this approach are highlighted during specific event where the model has experienced low agreement with observed data. Results are also compared to other assimilations methods.

  6. Modelling the optical properties of aerosols in a chemical transport model

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

    According to the IPCC fifth assessment report (2013), clouds and aerosols still contribute to the largest uncertainty when estimating and interpreting changes to the Earth's energy budget. Therefore, understanding the interaction between radiation and aerosols is both crucial for remote sensing observations and modelling the climate forcing arising from aerosols. Carbon particles are the largest contributor to the aerosol absorption of solar radiation, thereby enhancing the warming of the planet. Modelling the radiative properties of carbon particles is a hard task and involves many uncertainties arising from the difficulties of accounting for the morphologies and heterogeneous chemical composition of the particles. This study aims to compare two ways of modelling the optical properties of aerosols simulated by a chemical transport model. The first method models particle optical properties as homogeneous spheres and are externally mixed. This is a simple model that is particularly easy to use in data assimilation methods, since the optics model is linear. The second method involves a core-shell internal mixture of soot, where sulphate, nitrate, ammonia, organic carbon, sea salt, and water are contained in the shell. However, by contrast to previously used core-shell models, only part of the carbon is concentrated in the core, while the remaining part is homogeneously mixed with the shell. The chemical transport model (CTM) simulations are done regionally over Europe with the Multiple-scale Atmospheric Transport and CHemistry (MATCH) model, developed by the Swedish Meteorological and Hydrological Institute (SMHI). The MATCH model was run with both an aerosol dynamics module, called SALSA, and with a regular "bulk" approach, i.e., a mass transport model without aerosol dynamics. Two events from 2007 are used in the analysis, one with high (22/12-2007) and one with low (22/6-2007) levels of elemental carbon (EC) over Europe. The results of the study help to assess the

  7. Seasonal contrast in aerosol abundance over northern south Asia using a chemical transport model

    NASA Astrophysics Data System (ADS)

    Venkataraman, C.; Sadavarte, P.; Madhavan, B. L.; Kulkarni, S.; Carmichael, G. R.; Adhikary, B.; D'Allura, A.; Cherian, R.; Das, S.; Gupta, T.; Streets, D. G.; Wei, C.; Zhang, Q.

    2012-12-01

    Northern South-Asia, home to about half a billion people, experiences large aerosol abundances almost all year around. There are gaps in our understanding of seasonal variations in regional aerosol emissions, abundance and radiative effects. The present study uses chemical transport model simulations (at ~ 60km resolution), with regionally estimated emissions, to investigate the contrast in aerosol surface and columnar abundance during pre-monsoon transition, monsoon and inter-monsoon transition periods over than Gangetic plain (GP) and Tibetan plateau. The interplay between aerosol emissions and atmospheric transport is examined to explain the variability. Model predictions were evaluated with available in-situ measurements and AOD from AERONET and MODIS level-2 retrievals (at 10 km resolution) processed with quality weighting to the model resolution. During April, AOD was dominated by dust at most sites across the GP and Tibet. However, AOD from organic carbon (emitted from agricultural residue burning) is also significant at several sites (Pantnagar, Godavari, Kolkata, Dhaka, and at high altitude Pyramid and Lhasa sites), consistent with recently reported MISR climatology in this region. In contrast, during July and September, AOD was dominated by sulfate at all sites. In April, aerosols over the GP could be attributed to emissions from large industrial sources (thermal power plant, cement industries, iron & steel and other industries) and agricultural residue burning transported from the northwest, along with forest burning emissions transported from the east. Large fluxes of open burning emissions in the east GP, along with prevailing easterly wind flow into the GP led to an east-west gradient in anthropogenic aerosols. During July, there was little open burning, so aerosol concentrations were largely from industrial emissions transported out through the north. In the Tibet region, dust was predominant during both April and July. During September

  8. Chemical and Aerosol Signatures of Biomass Burning via Long Range Transport observed at Storm Peak Laboratory

    NASA Astrophysics Data System (ADS)

    Hallar, A. G.; Obrist, D.; McCubbin, I. B.; Fain, X.; Rahn, T.

    2008-12-01

    The Desert Research Institute operates a high elevation facility, Storm Peak Laboratory (SPL), located on the Steamboat Springs Ski Resort in Colorado at an elevation 3.2 km. During the spring of 2008, two field projects were conducted at SPL; Storm Peak Cloud and Aerosol Characterization (SPACC) and a State of Colorado Mercury Monitoring project. Measurements of gaseous elemental mercury (GEM), along with CO, ozone and aerosol concentrations and aerosol size distributions will be presented from April 28 to July 1st 2008. This work focuses on specific case studies pertaining to long range transport events. Specifically, high levels of GEM and CO will be presented from May 15, 2008. This data will be coupled with HYSPLIT backtrajectories, chemical modeling via MOZART, and satellite imagery (MODIS) to present evidence that Siberian wildfires impacted the air quality at Storm Peak Laboratory.

  9. Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

    NASA Astrophysics Data System (ADS)

    Sič, B.; El Amraoui, L.; Marécal, V.; Josse, B.; Arteta, J.; Guth, J.; Joly, M.; Hamer, P.

    2014-04-01

    This paper deals with recent improvements to the chemical transport model of Météo-France MOCAGE that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging, and by changing in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI), the ground (AERONET), and a model inter-comparison project (AeroCom) is compared with MOCAGE simulations and showed that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD) observations over the oceans, the updated model configuration shows a decrease in the bias (from 0.032 to 0.002) and a better correlation (from 0.062 to 0.322) in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive bias in the sea salt representation at high latitudes (from 0.153 to 0.026), and a negative bias in the desert dust representation in the African dust outflow region (from -0.179 to -0.051). The updates in sedimentation produced a modest difference; the bias with MODIS data from 0.002 in the updated configuration went to

  10. High resolution simulations of aerosol microphysics in a global and regionally nested chemical transport model

    NASA Astrophysics Data System (ADS)

    Adams, P. J.; Marks, M.

    2015-12-01

    The aerosol indirect effect is the largest source of forcing uncertainty in current climate models. This effect arises from the influence of aerosols on the reflective properties and lifetimes of clouds, and its magnitude depends on how many particles can serve as cloud droplet formation sites. Assessing levels of this subset of particles (cloud condensation nuclei, or CCN) requires knowledge of aerosol levels and their global distribution, size distributions, and composition. A key tool necessary to advance our understanding of CCN is the use of global aerosol microphysical models, which simulate the processes that control aerosol size distributions: nucleation, condensation/evaporation, and coagulation. Previous studies have found important differences in CO (Chen, D. et al., 2009) and ozone (Jang, J., 1995) modeled at different spatial resolutions, and it is reasonable to believe that short-lived, spatially-variable aerosol species will be similarly - or more - susceptible to model resolution effects. The goal of this study is to determine how CCN levels and spatial distributions change as simulations are run at higher spatial resolution - specifically, to evaluate how sensitive the model is to grid size, and how this affects comparisons against observations. Higher resolution simulations are necessary supports for model/measurement synergy. Simulations were performed using the global chemical transport model GEOS-Chem (v9-02). The years 2008 and 2009 were simulated at 4ox5o and 2ox2.5o globally and at 0.5ox0.667o over Europe and North America. Results were evaluated against surface-based particle size distribution measurements from the European Supersites for Atmospheric Aerosol Research project. The fine-resolution model simulates more spatial and temporal variability in ultrafine levels, and better resolves topography. Results suggest that the coarse model predicts systematically lower ultrafine levels than does the fine-resolution model. Significant

  11. Optical, physical and chemical properties of transported African mineral dust aerosols in the Mediterranean region

    NASA Astrophysics Data System (ADS)

    Denjean, Cyrielle; Di Biagio, Claudia; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Loisil, Rodrigue; Triquet, Sylvain; Zapf, Pascal; Roberts, Greg; Bourrianne, Thierry; Torres, Benjamin; Blarel, Luc; Sellegri, Karine; Freney, Evelyn; Schwarzenbock, Alfons; Ravetta, François; Laurent, Benoit; Mallet, Marc; Formenti, Paola

    2014-05-01

    The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), two intensive airborne campaigns (TRAQA, TRansport and Air QuAlity, 18 June - 11 July 2012, and ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) have been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to

  12. Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

    NASA Astrophysics Data System (ADS)

    Sič, B.; El Amraoui, L.; Marécal, V.; Josse, B.; Arteta, J.; Guth, J.; Joly, M.; Hamer, P. D.

    2015-02-01

    This paper deals with recent improvements to the global chemical transport model of Météo-France MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle) that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species: desert dust, sea salt, black carbon, organic carbon, and also volcanic ash in the case of large volcanic eruptions. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging and by changing the in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI), the ground (AERONET, EMEP), and a model inter-comparison project (AeroCom) are compared with MOCAGE simulations and show that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD) observations over the oceans, the updated model configuration shows a decrease in the modified normalized mean bias (MNMB; from 0.42 to 0.10) and a better correlation (from 0.06 to 0.32) in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive MNMB in the sea salt representation at high latitudes (from 0.65 to 0.16), and a negative MNMB in the desert

  13. Coupling aerosol optics to the MATCH (v5.5.0) chemical transport model and the SALSA (v1) aerosol microphysics module

    NASA Astrophysics Data System (ADS)

    Andersson, Emma; Kahnert, Michael

    2016-05-01

    A new aerosol-optics model is implemented in which realistic morphologies and mixing states are assumed, especially for black carbon particles. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey-shell" model. Simulated results of aerosol optical properties, such as aerosol optical depth, backscattering coefficients and the Ångström exponent, as well as radiative fluxes are computed with the new optics model and compared with results from an older optics-model version that treats all particles as externally mixed homogeneous spheres. The results show that using a more detailed description of particle morphology and mixing state impacts the aerosol optical properties to a degree of the same order of magnitude as the effects of aerosol-microphysical processes. For instance, the aerosol optical depth computed for two cases in 2007 shows a relative difference between the two optics models that varies over the European region between -28 and 18 %, while the differences caused by the inclusion or omission of the aerosol-microphysical processes range from -50 to 37 %. This is an important finding, suggesting that a simple optics model coupled to a chemical transport model can introduce considerable errors affecting radiative fluxes in chemistry-climate models, compromising comparisons of model results with remote sensing observations of aerosols, and impeding the assimilation of satellite products for aerosols into chemical-transport models.

  14. Evaluation of the performance of four chemical transport models in predicting the aerosol chemical composition in Europe in 2005

    NASA Astrophysics Data System (ADS)

    Prank, Marje; Sofiev, Mikhail; Tsyro, Svetlana; Hendriks, Carlijn; Semeena, Valiyaveetil; Vazhappilly Francis, Xavier; Butler, Tim; Denier van der Gon, Hugo; Friedrich, Rainer; Hendricks, Johannes; Kong, Xin; Lawrence, Mark; Righi, Mattia; Samaras, Zissis; Sausen, Robert; Kukkonen, Jaakko; Sokhi, Ranjeet

    2016-05-01

    Four regional chemistry transport models were applied to simulate the concentration and composition of particulate matter (PM) in Europe for 2005 with horizontal resolution ~ 20 km. The modelled concentrations were compared with the measurements of PM chemical composition by the European Monitoring and Evaluation Programme (EMEP) monitoring network. All models systematically underestimated PM10 and PM2.5 by 10-60 %, depending on the model and the season of the year, when the calculated dry PM mass was compared with the measurements. The average water content at laboratory conditions was estimated between 5 and 20 % for PM2.5 and between 10 and 25 % for PM10. For majority of the PM chemical components, the relative underestimation was smaller than it was for total PM, exceptions being the carbonaceous particles and mineral dust. Some species, such as sea salt and NO3-, were overpredicted by the models. There were notable differences between the models' predictions of the seasonal variations of PM, mainly attributable to different treatments or omission of some source categories and aerosol processes. Benzo(a)pyrene concentrations were overestimated by all the models over the whole year. The study stresses the importance of improving the models' skill in simulating mineral dust and carbonaceous compounds, necessity for high-quality emissions from wildland fires, as well as the need for an explicit consideration of aerosol water content in model-measurement comparison.

  15. Development and application of a three-dimensional aerosol chemical transport model, PMCAMx

    NASA Astrophysics Data System (ADS)

    Gaydos, Timothy M.; Pinder, Rob; Koo, Bonyoung; Fahey, Kathleen M.; Yarwood, Gregory; Pandis, Spyros N.

    A three-dimensional chemical transport model (PMCAMx) is used to simulate PM mass and composition in the eastern United States for a July 2001 pollution episode. The performance of the model in this region is evaluated, taking advantage of the highly time and size-resolved PM and gas-phase data collected during the Pittsburgh Air Quality Study (PAQS). PMCAMx uses the framework of CAMx and detailed aerosol modules to simulate inorganic aerosol growth, aqueous-phase chemistry, secondary organic aerosol formation, nucleation, and coagulation. The model predictions are compared to hourly measurements of PM 2.5 mass and composition at Pittsburgh, as well as to measurements from the AIRS and IMPROVE networks. The performance of the model for the major PM 2.5 components (sulfate, ammonium, and organic carbon) is encouraging (fractional errors are in general smaller than 50%). Additional improvements are possible if the rainfall measurements are used instead of the meteorological model predictions. The modest errors in ammonium predictions and the lack of bias for the total (gas and particulate) ammonium suggest that the improved ammonia inventory used is reasonable. The significant errors in aerosol nitrate predictions are mainly due to difficulties in simulating the nighttime formation of nitric acid. The concentrations of elemental carbon (EC) in the urban areas are significantly overpredicted. This is a problem related to both the emission inventory but also the different EC measurement methods that have been used in the two measurement networks (AIRS and IMPROVE) and the actual development of the inventory. While the ability of the model to reproduce OC levels is encouraging, additional work is necessary to confirm that that this is due to the right reasons and not offsetting errors in the primary emissions and the secondary formation. The model performance against the semi-continuous measurements in Pittsburgh appears to be quite similar to its performance against

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

    NASA Technical Reports Server (NTRS)

    Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.; Jayaraman, A.; Pandit, A.; Raj, A.; Kumar, H.; Kumar, S.; Singh, A.; Stenchikov, G.; Wienhold, F.; Bian, J.

    2016-01-01

    Satellite observations and numerical modeling studies have demonstrated that the Asian Summer Monsoon (ASM) provide a conduit for gas-phase pollutants in south Asia to reach the lower stratosphere. Now, observations from the CALIPSO satellite have revealed the Asian Tropopause Aerosol Layer (ATAL), a summertime accumulation of aerosols in the upper troposphere and lower stratosphere (UTLS), associated with the ASM anticyclone. The ATAL has potential implications for regional cloud properties, climate, and chemical processes in the UTLS. Here, we show in situ measurements from balloon-borne instruments, aircraft, and satellite observations, together with trajectory and chemical transport model (CTM) simulations to explore the origin, composition, physical, and optical properties of aerosols in the ATAL. In particular, we show balloon-data from our BATAL-2015 field campaign to India and Saudi Arabia in summer 2015, which includes in situ backscatter measurements from COBALD instruments, and the first observations of size and volatility of aerosols in the ATAL layer using optical particle counters (OPCs). Back trajectory calculations initialized from CALIPSO observations point to deep convection over North India as a principal source of ATAL aerosols. Available aircraft observations suggest significant sulfur and carbonaceous components to the ATAL, which is supported by simulations using the GEOS-Chem CTM. Source elimination studies conducted with the GEOS-Chem indicate that ATAL aerosols originate primary from south Asian sources, in contrast with some earlier studies.

  17. Aerosol Types using Passive Remote Sensing: Global Distribution, Consistency Check, Total-Column Investigation and Translation into Composition Derived from Climate and Chemical Transport Model

    NASA Astrophysics Data System (ADS)

    Kacenelenbogen, M. S.; Dawson, K. W.; Johnson, M. S.; Burton, S. P.; Redemann, J.; Hasekamp, O. P.; Hair, J. W.; Ferrare, R. A.; Butler, C. F.; Holben, B. N.; Beyersdorf, A. J.; Ziemba, L. D.; Froyd, K. D.; Dibb, J. E.; Shingler, T.; Sorooshian, A.; Jimenez, J. L.; Campuzano Jost, P.; Jacob, D. J.

    2015-12-01

    To improve the predictions of aerosol composition in chemical transport models (CTMs) and global climate models (GCMs), we have developed an aerosol classification algorithm (called Specified Clustering and Mahalanobis Classification, SCMC) that assigns an aerosol type to multi-parameter retrievals by spaceborne, airborne or ground based passive remote sensing instruments [Russell et al., 2014]. The aerosol types identified by our scheme are pure dust, polluted dust, urban-industrial/developed economy, urban-industrial/developing economy, dark biomass smoke, light biomass smoke and pure marine. We apply the SCMC method to two different total-column datasets of aerosol optical properties: inversions from the ground-based AErosol RObotic NETwork (AERONET) and retrievals from the space-borne POLDER (Polarization and Directionality of Earth's Reflectances) instrument. The POLDER retrievals that we use differ from the standard POLDER retrievals [Deuzé et al., 2001] as they make full use of multi-angle, multispectral polarimetric data [Hasekamp et al., 2011]. We analyze agreement in the aerosol types inferred from both AERONET and POLDER globally. Then, we investigate how our total-column "effective" SCMC aerosol types relate to different aerosol types within the column (i.e. either a mixture of different types within one layer in the vertical or the stacking of different aerosol types within the vertical column). For that, we compare AERONET-SCMC aerosol types to collocated NASA LaRC HSRL vertically resolved aerosol types [Burton et al., 2012] during the SEAC4RS and DISCOVER-AQ airborne field experiments, mostly over Texas in Aug-Sept 2013. Finally, in order to evaluate the GEOS-Chem CTM aerosol types, we translate each of our SCMC aerosol type into a unique distribution of GEOS-Chem aerosol composition (e.g. biomass burning, dust, sulfate, sea salt). We bridge the gap between remote sensing and model-inferred aerosol types by using multiple years of collocated AERONET

  18. Characterizing the long-range transport of black carbon aerosols during Transport and Chemical Evolution over the Pacific (TRACE-P) experiment.

    PubMed

    Verma, Sunita; Worden, John; Payra, Swagata; Jourdain, Line; Shim, Changsub

    2009-07-01

    A major aircraft experiment Transport and Chemical Evolution over the Pacific (TRACE-P) mission over the NW Pacific in March-April 2001 was conducted to better understand how outflow from the Asian continent affects the composition of the global atmosphere. In this paper, a global climate model, GEOS-Chem is used to investigate possible black carbon aerosol contributions from TRACE-P region. Our result depicts that absorbing black carbon ("soot") significantly outflow during lifting to the free troposphere through warm conveyor belt and convection associated with this lifting. The GEOS-Chem simulation results show significant transport of black carbon aerosols from Asian regions to the Western Pacific region during the spring season. As estimated by GEOS-Chem simulations, approximately 25% of the black carbon concentrations over the western pacific originate from SE Asia in the spring.

  19. Influence of anthropogenic aerosol on cloud optical depth and albedo shown by satellite measurements and chemical transport modeling.

    PubMed

    Schwartz, Stephen E; Harshvardhan; Benkovitz, Carmen M

    2002-02-19

    The Twomey effect of enhanced cloud droplet concentration, optical depth, and albedo caused by anthropogenic aerosols is thought to contribute substantially to radiative forcing of climate change over the industrial period. However, present model-based estimates of this indirect forcing are highly uncertain. Satellite-based measurements would provide global or near-global coverage of this effect, but previous efforts to identify and quantify enhancement of cloud albedo caused by anthropogenic aerosols in satellite observations have been limited, largely because of strong dependence of albedo on cloud liquid water path (LWP), which is inherently highly variable. Here we examine satellite-derived cloud radiative properties over two 1-week episodes for which a chemical transport and transformation model indicates substantial influx of sulfate aerosol from industrial regions of Europe or North America to remote areas of the North Atlantic. Despite absence of discernible dependence of optical depth or albedo on modeled sulfate loading, examination of the dependence of these quantities on LWP readily permits detection and quantification of increases correlated with sulfate loading, which are otherwise masked by variability of LWP, demonstrating brightening of clouds because of the Twomey effect on a synoptic scale. Median cloud-top spherical albedo was enhanced over these episodes, relative to the unperturbed base case for the same LWP distribution, by 0.02 to 0.15.

  20. Improving the representation of secondary organic aerosol (SOA) in the MOZART-4 global chemical transport model

    NASA Astrophysics Data System (ADS)

    Mahmud, A.; Barsanti, K.

    2013-07-01

    The secondary organic aerosol (SOA) module in the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) was updated by replacing existing two-product (2p) parameters with those obtained from two-product volatility basis set (2p-VBS) fits (MZ4-C1), and by treating SOA formation from the following additional volatile organic compounds (VOCs): isoprene, propene and lumped alkenes (MZ4-C2). Strong seasonal and spatial variations in global SOA distributions were demonstrated, with significant differences in the predicted concentrations between the base case and updated model simulations. Updates to the model resulted in significant increases in annual average SOA mass concentrations, particularly for the MZ4-C2 simulation in which the additional SOA precursor VOCs were treated. Annual average SOA concentrations predicted by the MZ4-C2 simulation were 1.00 ± 1.04 μg m-3 in South America, 1.57 ± 1.88 μg m-3 in Indonesia, 0.37 ± 0.27 μg m-3 in the USA, and 0.47 ± 0.29 μg m-3 in Europe with corresponding increases of 178, 406, 311 and 292% over the base-case simulation, respectively, primarily due to inclusion of isoprene. The increases in predicted SOA mass concentrations resulted in corresponding increases in SOA contributions to annual average total aerosol optical depth (AOD) by ~ 1-6%. Estimated global SOA production was 5.8, 6.6 and 19.1 Tg yr-1 with corresponding burdens of 0.22, 0.24 and 0.59 Tg for the base-case, MZ4-C1 and MZ4-C2 simulations, respectively. The predicted SOA budgets fell well within reported ranges for comparable modeling studies, 6.7 to 96 Tg yr-1, but were lower than recently reported observationally constrained values, 50 to 380 Tg yr-1. For MZ4-C2, simulated SOA concentrations at the surface also were in reasonable agreement with comparable modeling studies and observations. Total organic aerosol (OA) mass concentrations at the surface, however, were slightly over-predicted in Europe, Amazonian regions and Malaysian Borneo

  1. Improving the representation of secondary organic aerosol (SOA) in the MOZART-4 global chemical transport model

    NASA Astrophysics Data System (ADS)

    Mahmud, A.; Barsanti, K. C.

    2012-12-01

    The secondary organic aerosol (SOA) module in the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) has been updated by replacing existing two-product (2p) parameters with those obtained from two-product volatility basis set (2p-VBS) fits, and by treating SOA formation from the following volatile organic compounds (VOCs): isoprene, propene and lumped alkenes. Strong seasonal and spatial variations in global SOA distributions were demonstrated, with significant differences in the predicted concentrations between the base-case and updated model versions. The base-case MOZART-4 predicted annual average SOA of 0.36 ± 0.50 μg m-3 in South America, 0.31 ± 0.38 μg m-3 in Indonesia, 0.09 ± 0.05 μg m-3 in the USA, and 0.12 ± 0.07 μg m-3 in Europe. Concentrations from the updated versions of the model showed a~marked increase in annual average SOA. Using the updated set of parameters alone (MZ4-v1) increased annual average SOA by ~8%, ~16%, ~56%, and ~108% from the base-case in South America, Indonesia, USA, and Europe, respectively. Treatment of additional parent VOCs (MZ4-v2) resulted in an even more dramatic increase of ~178-406% in annual average SOA for these regions over the base-case. The increases in predicted SOA concentrations further resulted in increases in corresponding SOA contributions to annual average total aerosol optical depth (AOD) by <1% for MZ4-v1 and ~1-6% for MZ4-v2. Estimated global SOA production was ~6.6 Tg yr-1 and ~19.1 Tg yr-1 with corresponding burdens of ~0.24 Tg and ~0.59 Tg using MZ4-v1 and MZ4-v2, respectively. The SOA budgets predicted in the current study fall well within reported ranges for similar modeling studies, 6.7 to 96 Tg yr-1, but are lower than recently reported observationally-constrained values, 50 to 380 Tg yr-1. With MZ4-v2, simulated SOA concentrations at the surface were also in reasonable agreement with comparable modeling studies and observations. Concentrations of estimated organic aerosol (OA

  2. Measurements of HNO3, SO2 High Resolution Aerosol SO4 (sup 2-), and Selected Aerosol Species Aboard the NASA DC-8 Aircraft: During the Transport and Chemical Evolution Over the Pacific Airborne Mission (TRACE-P)

    NASA Technical Reports Server (NTRS)

    Talbot, Robert W.; Dibb, Jack E.

    2004-01-01

    The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.

  3. Top-Down Inversion of Aerosol Emissions through Adjoint Integration of Satellite Radiance and GEOS-Chem Chemical Transport Model

    NASA Astrophysics Data System (ADS)

    Xu, X.; Wang, J.; Henze, D. K.; Qu, W.; Kopacz, M.

    2012-12-01

    The knowledge of aerosol emissions from both natural and anthropogenic sources are needed to study the impacts of tropospheric aerosol on atmospheric composition, climate, and human health, but large uncertainties persist in quantifying the aerosol sources with the current bottom-up methods. This study presents a new top-down approach that spatially constrains the amount of aerosol emissions from satellite (MODIS) observed reflectance with the adjoint of a chemistry transport model (GEOS-Chem). We apply this technique with a one-month case study (April 2008) over the East Asia. The bottom-up estimated sulfate-nitrate-ammonium precursors, such as sulfur dioxide (SO2), ammonia (NH3), and nitrogen oxides (NOx), all from INTEX-B 2006 inventory, emissions of black carbon (BC), organic carbon (OC) from Bond-2007 inventory, and mineral dust simulated from DEAD dust mobilization scheme, are spatially optimized from the GEOS-Chem model and its adjoint constrained by the aerosol optical depth (AOD) that are derived from MODIS reflectance with the GEOS-Chem aerosol single scattering properties. The adjoint inverse modeling for the study period yields notable decreases in anthropogenic aerosol emissions over China: 436 Gg (33.5%) for SO2, 378 Gg (34.5%) for NH3, 319 (18.8%) for NOx, 10 Gg (9.1%) for BC, and 30 Gg (15.0%) for OC. The total amount of the mineral dust emission is reduced by 56.4% from the DEAD mobilization module which simulates dust production of 19020 Gg. Sub-regional adjustments are significant and directions of changes are spatially different. The model simulation with optimized aerosol emissions shows much better agreement with independent observations from sun-spectrophotometer observed AOD from AERONET, MISR (Multi-angle Imaging SpectroRadiometer) AOD, OMI (Ozone Monitoring Instrument) NO2 and SO2 columns, and surface aerosol concentrations measured over both anthropogenic pollution and dust source regions. Assuming the used bottom-up anthropogenic

  4. Sources, seasonality, and trends of Southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

    NASA Astrophysics Data System (ADS)

    Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

    2015-07-01

    We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the Southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 km × 25 km resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the Southeast US. GEOS-Chem simulation of sulfate requires a missing oxidant, taken here to be stabilized Criegee intermediates, but which could alternatively reflect an unaccounted for heterogeneous process. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 20 % in the cloud convective layer at 1.5-3 km, and 20 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-])) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by organic aerosol. This would explain the long-term decline of ammonium aerosol in the Southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the Southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the Southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 21 %. The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from

  5. Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

    NASA Astrophysics Data System (ADS)

    Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

    2015-09-01

    We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5-3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-]) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8-28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines

  6. Aerosol Transport Over Equatorial Africa

    NASA Technical Reports Server (NTRS)

    Gatebe, C. K.; Tyson, P. D.; Annegarn, H. J.; Kinyua, A. M.; Piketh, S.; King, M.; Helas, G.

    1999-01-01

    Long-range and inter-hemispheric transport of atmospheric aerosols over equatorial Africa has received little attention so far. Most aerosol studies in the region have focussed on emissions from rain forest and savanna (both natural and biomass burning) and were carried out in the framework of programs such as DECAFE (Dynamique et Chimie Atmospherique en Foret Equatoriale) and FOS (Fires of Savanna). Considering the importance of this topic, aerosols samples were measured in different seasons at 4420 meters on Mt Kenya and on the equator. The study is based on continuous aerosol sampling on a two stage (fine and coarse) streaker sampler and elemental analysis by Particle Induced X-ray Emission. Continuous samples were collected for two seasons coinciding with late austral winter and early austral spring of 1997 and austral summer of 1998. Source area identification is by trajectory analysis and sources types by statistical techniques. Major meridional transports of material are observed with fine-fraction silicon (31 to 68 %) in aeolian dust and anthropogenic sulfur (9 to 18 %) being the major constituents of the total aerosol loading for the two seasons. Marine aerosol chlorine (4 to 6 %), potassium (3 to 5 %) and iron (1 to 2 %) make up the important components of the total material transport over Kenya. Minimum sulfur fluxes are associated with recirculation of sulfur-free air over equatorial Africa, while maximum sulfur concentrations are observed following passage over the industrial heartland of South Africa or transport over the Zambian/Congo Copperbelt. Chlorine is advected from the ocean and is accompanied by aeolian dust recirculating back to land from mid-oceanic regions. Biomass burning products are transported from the horn of Africa. Mineral dust from the Sahara is transported towards the Far East and then transported back within equatorial easterlies to Mt Kenya. This was observed during austral summer and coincided with the dying phase of 1997/98 El

  7. Chemical Properties of Combustion Aerosols: An Overview

    EPA Science Inventory

    A wide variety of pyrogenic and anthropogenic sources emit fine aerosols to the atmosphere. The physical and chemical properties of these aerosols are of interest due to their influence on climate, human health, and visibility. Aerosol chemical composition is remarkably complex. ...

  8. Detection of chemical agent aerosols

    NASA Astrophysics Data System (ADS)

    Fox, Jay A.; Ahl, Jeffrey L.; D'Amico, Francis M.; Vanderbeek, Richard G.; Moon, Raphael; Swim, Cynthia R.

    1999-05-01

    One of the major threats presented by a chemical agent attack is that of a munition exploding overhead and 'raining' aerosols which can contaminate surfaces when they impact. Since contact with these surfaces can be fatal, it is imperative to know when such an attack has taken place and the likely threat density and location. We present the results of an experiment designed to show the utility of a CO2 lidar in detecting such an attack. Testing occurred at Dugway Proving Grounds, Utah and involved the simulation of an explosive airburst chemical attack. Explosions occurred at a height of 30 m and liquid droplets from two chemicals, PEG-200 (polyethylene glycol 200) and TEP (triethylphosphate), were expelled and fell to the ground. The munition was the U.S. Army M9 Simulator, Projectile, Airburst, Liquid (SPAL) system that is designed for chemical warfare training exercises. The instrument that was used to detect the presence of the aerosols was the Laser Standoff Chemical Detector (LSCD) which is a light detection and ranging (LIDAR) system that utilizes a rapidly tunable, pulsed CO2 laser. The LIDAR scanned a horizontal path approximately 5 - 8 m above the ground in order to measure the concentration of liquid deposition. The LIDAR data were later correlated with card data to determine how well the system could predict the location and quantity of liquid deposition on the ground.

  9. Chemical composition of size-segregated aerosol collected all year-round at Concordia Station (Dome C, Antarctica). Transport processes and climatic implications.

    NASA Astrophysics Data System (ADS)

    Udisti, Roberto; Becagli, Silvia; Frosini, Daniele; Galli, Gaia; Ghedini, Costanza; Rugi, Francesco; Severi, Mirko; Traversi, Rita

    2010-05-01

    Ice-core stratigraphies of chemical components of atmospheric gases and aerosols trapped in the snow layers by scavenging processes are a powerful tool in understanding past climatic and environmental changes. The deep ice core drilled at Dome C in the framework of the EPICA project allowed reconstructing the last 8 glacial-interglacial cycles and highlightened the complex relationships between climatic forcings and environmental feedback processes. In interpreting ice core records as a function of past climatic variations, some difficulties arise from uncertainties in considering selected chemical species as reliable markers of climatic and environmental processes and in attributing the different load and composition of aerosols over Antarctica to changes in source intensity (such as aridity, wind strength, emersion of continental platform by sea-level lowering etc..) and/or to variations in atmospheric processes (such as meridional and zonal atmospheric circulation, polar vortex intensity, scavenging efficiency, transport pathways etc..). Besides, two new aspects are actually under discussions: the possible use of Na as sea-ice cover marker (via frost flower formation on the sea-ice surface during the pack-ice formation) and the identification of continental source areas for mineral dust reaching internal regions of Antarctica during glacial and interglacial periods. In order to better address such controversial issues, since 2005 a continuous, high temporal resolution size-segregated aerosol and surface snow sampling has been performed at Dome C (central East Antarctic Plateau, 75° 06' S, 123° 23' E), in the framework of "Station Concordia" Project (a Italian PNRA- French IPEV joint program). The chemical analysis of size-segregated aerosol and daily superficial snow samples, collected all year-round for more than 4 years, can contribute to clarify some of the above mentioned topics. In particular: the possible seasonal pattern of sea spray aerosol could be

  10. Global aerosol modeling with the online NMMB/BSC Chemical Transport Model: sensitivity to fire injection height prescription and secondary organic aerosol schemes

    NASA Astrophysics Data System (ADS)

    Spada, Michele; Jorba, Oriol; Pérez García-Pando, Carlos; Tsigaridis, Kostas; Soares, Joana; Obiso, Vincenzo; Janjic, Zavisa; Baldasano, Jose M.

    2015-04-01

    We develop and evaluate a fully online-coupled model simulating the life-cycle of the most relevant global aerosols (i.e. mineral dust, sea-salt, black carbon, primary and secondary organic aerosols, and sulfate) and their feedbacks upon atmospheric chemistry and radiative balance. Following the capabilities of its meteorological core, the model has been designed to simulate both global and regional scales with unvaried parameterizations: this allows detailed investigation on the aerosol processes bridging the gap between global and regional models. Since the strong uncertainties affecting aerosol models are often unresponsive to model complexity, we choose to introduce complexity only when it clearly improves results and leads to a better understanding of the simulated aerosol processes. We test two important sources of uncertainty - the fires injection height and secondary organic aerosol (SOA) production - by comparing a baseline simulation with experiments using more advanced approaches. First, injection heights prescribed by Dentener et al. (2006, ACP) are compared with climatological injection heights derived from satellite measurements and produced through the Integrated Monitoring and Modeling System For Wildland Fires (IS4FIRES). Also global patterns of SOA produced by the yield conversion of terpenes as prescribed by Dentener et al. (2006, ACP) are compared with those simulated by the two-product approach of Tsigaridis et al. (2003, ACP). We evaluate our simulations using a variety of observations and measurement techniques. Additionally, we discuss our results in comparison to other global models within AEROCOM and ACCMIP.

  11. Evaluation of chemical transport model predictions of primary organic aerosol for air masses classified by particle-component-based factor analysis

    NASA Astrophysics Data System (ADS)

    Stroud, C. A.; Moran, M. D.; Makar, P. A.; Gong, S.; Gong, W.; Zhang, J.; Slowik, J. G.; Abbatt, J. P. D.; Lu, G.; Brook, J. R.; Mihele, C.; Li, Q.; Sills, D.; Strawbridge, K. B.; McGuire, M. L.; Evans, G. J.

    2012-02-01

    Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in southern Ontario (ON), Canada, were used to evaluate Environment Canada's regional chemical transport model predictions of primary organic aerosol (POA). Environment Canada's operational numerical weather prediction model and the 2006 Canadian and 2005 US national emissions inventories were used as input to the chemical transport model (named AURAMS). Particle-component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. Co-located carbon monoxide (CO), PM2.5 black carbon (BC), and PM1 SO4 measurements were also used for evaluation and interpretation, permitting a detailed diagnostic model evaluation. At the urban site, good agreement was observed for the comparison of daytime campaign PM1 POA and HOA mean values: 1.1 μg m-3 vs. 1.2 μg m-3, respectively. However, a POA overprediction was evident on calm nights due to an overly-stable model surface layer. Biases in model POA predictions trended from positive to negative with increasing HOA values. This trend has several possible explanations, including (1) underweighting of urban locations in particulate matter (PM) spatial surrogate fields, (2) overly-coarse model grid spacing for resolving urban-scale sources, and (3) lack of a model particle POA evaporation process during dilution of vehicular POA tail-pipe emissions to urban scales. Furthermore, a trend in POA bias was observed at the urban site as a function of the BC/HOA ratio, suggesting a possible association of POA underprediction for diesel combustion sources. For several time periods, POA overprediction was also observed for sulphate-rich plumes, suggesting that our model POA fractions for the PM2.5 chemical speciation profiles may be too high for these point sources. At the rural Harrow site

  12. CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

    EPA Science Inventory

    This chapter surveys the analytical techniques used to determine the concentrations of aerosol mass and its chemical components. The techniques surveyed include mass, major ions (sulfate, nitrate, ammonium), organic carbon, elemental carbon, and trace elements. As reported in...

  13. Secondary inorganic aerosol evaluation: Application of a transport chemical model in the eastern part of the Po Valley

    NASA Astrophysics Data System (ADS)

    Pecorari, Eliana; Squizzato, Stefania; Longo, Andrea; Visin, Flavia; Rampazzo, Giancarlo

    2014-12-01

    Secondary inorganic aerosol (SIA) represents an important component of fine particulate matter in Europe. A photochemical model has been used to assess the distribution of secondary inorganic ions (sulfate, nitrate and ammonium) in the eastern part of the Po Valley, close to Venice. Specific meteorological and environmental conditions and very highly urbanized and industrialized areas make this domain one of the most polluted in Europe. Several studies have been conducted to assess particulate matter (PM10 and PM2.5) areal distribution. However, SIA formation dynamics are still a research subject especially in the transition environments, where the changes in the orography and in the land-use can affect air mass movements and atmospheric composition. This paper is a first attempt to simulate SIA distribution by using a photochemical model in the sea/land Venice transition area. Moreover, a modeling approach with clean boundary conditions has been used to check local and regional influence on SIA levels in the domain. Results reveal that, despite the importance of regional influences, local formation processes are important in SIA distribution especially during warm periods. SO42- and NH4+ are more linked to emission sources distribution than NO3- that tends to be more diffused in the study area. The use of a photochemical model, suitably tested in a such complex area, can improve air pollution knowledge and can help in air quality decision making.

  14. Evaluation of chemical transport model predictions of primary organic aerosol for air masses classified by particle component-based factor analysis

    NASA Astrophysics Data System (ADS)

    Stroud, C. A.; Moran, M. D.; Makar, P. A.; Gong, S.; Gong, W.; Zhang, J.; Slowik, J. G.; Abbatt, J. P. D.; Lu, G.; Brook, J. R.; Mihele, C.; Li, Q.; Sills, D.; Strawbridge, K. B.; McGuire, M. L.; Evans, G. J.

    2012-09-01

    Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in Southern Ontario, Canada, were used to evaluate predictions of primary organic aerosol (POA) and two other carbonaceous species, black carbon (BC) and carbon monoxide (CO), made for this summertime period by Environment Canada's AURAMS regional chemical transport model. Particle component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. A novel diagnostic model evaluation was performed by investigating model POA bias as a function of HOA mass concentration and indicator ratios (e.g. BC/HOA). Eight case studies were selected based on factor analysis and back trajectories to help classify model bias for certain POA source types. By considering model POA bias in relation to co-located BC and CO biases, a plausible story is developed that explains the model biases for all three species. At the rural sites, daytime mean PM1 POA mass concentrations were under-predicted compared to observed HOA concentrations. POA under-predictions were accentuated when the transport arriving at the rural sites was from the Detroit/Windsor urban complex and for short-term periods of biomass burning influence. Interestingly, the daytime CO concentrations were only slightly under-predicted at both rural sites, whereas CO was over-predicted at the urban Windsor site with a normalized mean bias of 134%, while good agreement was observed at Windsor for the comparison of daytime PM1 POA and HOA mean values, 1.1 μg m-3 and 1.2 μg m-3, respectively. Biases in model POA predictions also trended from positive to negative with increasing HOA values. Periods of POA over-prediction were most evident at the urban site on calm nights due to an overly-stable model surface layer. This model behaviour can be explained by a combination of model under

  15. Atmospheric aerosols as prebiotic chemical reactors

    PubMed Central

    Dobson, Christopher M.; Ellison, G. Barney; Tuck, Adrian F.; Vaida, Veronica

    2000-01-01

    Aerosol particles in the atmosphere have recently been found to contain a large number of chemical elements and a high content of organic material. The latter property is explicable by an inverted micelle model. The aerosol sizes with significant atmospheric lifetimes are the same as those of single-celled organisms, and they are predicted by the interplay of aerodynamic drag, surface tension, and gravity. We propose that large populations of such aerosols could have afforded an environment, by means of their ability to concentrate molecules in a wide variety of physical conditions, for key chemical transformations in the prebiotic world. We also suggest that aerosols could have been precursors to life, since it is generally agreed that the common ancestor of terrestrial life was a single-celled organism. The early steps in some of these initial transformations should be accessible to experimental investigation. PMID:11035775

  16. Atmospheric aerosols as prebiotic chemical reactors

    NASA Astrophysics Data System (ADS)

    Dobson, Christopher M.; Ellison, G. Barney; Tuck, Adrian F.; Vaida, Veronica

    2000-10-01

    Aerosol particles in the atmosphere have recently been found to contain a large number of chemical elements and a high content of organic material. The latter property is explicable by an inverted micelle model. The aerosol sizes with significant atmospheric lifetimes are the same as those of single-celled organisms, and they are predicted by the interplay of aerodynamic drag, surface tension, and gravity. We propose that large populations of such aerosols could have afforded an environment, by means of their ability to concentrate molecules in a wide variety of physical conditions, for key chemical transformations in the prebiotic world. We also suggest that aerosols could have been precursors to life, since it is generally agreed that the common ancestor of terrestrial life was a single-celled organism. The early steps in some of these initial transformations should be accessible to experimental investigation.

  17. Microphysical and Chemical Properties of Agricultural Aerosols

    NASA Astrophysics Data System (ADS)

    Brooks, S. D.; Moon, S.; Littleton, R.; Auvermann, B.

    2005-12-01

    Due to significant atmospheric loadings of agricultural dust aerosols, the aerosol's ability to contribute significantly to climate forcing on a regional to global level has been a topic of recent interest. Efforts have been made to quantify both the aerosol extinction of the total aerosol population and the hygroscopic and chemical properties of individual particles at a cattle feedyard near Canyon, Texas. Measurements of aerosol extinction are made using open-path transmissometry. Our results show that extinction varies significantly with relative humidity. To further explore the hygroscopic nature of the particles, size-resolved aerosol samples are collected using a cascade impactor system (7 stages ranging from 0.6 micron to 16 micron diameter) and hygroscopicity measurements are conducted on these using an Environmental Scanning Electron Microscope (ESEM). Complimentary determination of the elemental composition of individual particles is performed using Energy Dispersive X-ray Spectroscopy. Results of the optical properties, hygroscopicity and chemical composition of aerosols will be presented and atmospheric implications discussed.

  18. Physical and Chemical Properties of Anthropogenic Aerosols: An Overview

    EPA Science Inventory

    Aerosol chemical composition is complex. Combustion aerosols can comprise tens of thousands of organic compounds, refractory brown and black carbon, heavy metals, cations, anions, salts, and other inorganic phases. Aerosol organic matter normally contains semivolatile material th...

  19. Physical and Chemical Properties of Anthropogenic Aerosols: An overview

    EPA Science Inventory

    A wide variety of anthropogenic sources emit fine aerosols to the atmosphere. The physical and chemical properties of these aerosols are of interest due to their influence on climate, human health, and visibility. Aerosol chemical composition is complex. Combustion aerosols can c...

  20. Sensitivity of aerosol properties to new particle formation mechanism and to primary emissions in a continental-scale chemical transport model

    SciTech Connect

    Chang,L.S.; Schwartz, S.E.; McGraw, R.; Lewis, E.R.

    2009-04-02

    Four theoretical formulations of new particle formation (NPF) and one empirical formulation are used to examine the sensitivity of observable aerosol properties to NPF formulation and to properties of emitted particles in a continental-scale model for the United States over a 1-month simulation (July 2004). For each formulation the dominant source of Aitken mode particles is NPF with only a minor contribution from primary emissions, whereas for the accumulation mode both emissions and transfer of particles from the Aitken mode are important. The dominant sink of Aitken mode number is coagulation, whereas the dominant sink of accumulation mode number is wet deposition (including cloud processing), with a minor contribution from coagulation. The aerosol mass concentration, which is primarily in the accumulation mode, is relatively insensitive to NPF formulation despite order-of-magnitude differences in the Aitken mode number concentration among the different parameterizations. The dominant sensitivity of accumulation mode number concentration is to the number of emitted particles (for constant mass emission rate). Comparison of modeled aerosol properties with aircraft measurements shows, as expected, better agreement in aerosol mass concentration than in aerosol number concentration for all NPF formulations considered. These comparisons yield instances of rather accurate simulations in the planetary boundary layer, with poor model performance in the free troposphere attributed mainly to lack of representation of biomass burning and/or to long-range transport of particles from outside the model domain. Agreement between model results and measurements is improved by using smaller grid cells (12 km versus 60 km).

  1. Multi- year Arctic and Antarctic aerosol chemical characterization

    NASA Astrophysics Data System (ADS)

    Udisti, Roberto; Becagli, Silvia; Caiazzo, Laura; Calzolai, Giulia; Cappelletti, David; Giardi, Fabio; Grotti, Marco; Malandrino, Mery; Nava, Silvia; Severi, Mirko; Traversi, Rita

    2016-04-01

    Long term measurements of aerosol chemical composition in polar region are particularly relevant to investigate potential climatic effects of atmospheric components arising from both natural and anthropogenic emissions. In order to improve our knowledge on the atmospheric load and chemical composition of polar aerosol, several measurements and sampling campaigns were carried out both in Antarctica and in the Arctic since 2005.The main results are here reported. As regard as Antarctica, a continuous all-year-round sampling of size-segregated aerosol was carried from 2005 to 2013 at Dome C (East Antarctica; 75° 60' S, 123° 200' E, 3220 m a.s.l. and 1100 km away from the nearest coast). Aerosol was collected by PM10 and PM2.5 samplers and by multi-stage impactors (Dekati 4-stage impactor). Chemical analysis was carried out by Ion Chromatography (ions composition) and ICP-MS (trace metals). Sea spray showed a sharp seasonal pattern, with winter (Apr-Nov) concentrations about ten times larger than summer (Dec-Mar). Besides, in winter, sea spray particles are mainly sub micrometric, while the summer size-mode is around 1-2 um. Meteorological analysis and air mass back trajectory reconstructions allowed the identification of two major air mass pathways: micrometric fractions for transport from the closer Indian-Pacific sector, and sub-micrometric particles for longer trajectories over the Antarctic Plateau. The markers of oceanic biogenic emission (methanesulfonic acid - MSA, and non-sea-salt sulphate) exhibit a seasonal cycle with summer maxima (Nov-Mar). Their size distributions show two modes (0.4- 0.7 um and 1.1-2.1 um) in early summer and just one sub-micrometric mode in full summer. The two modes are related to different transport pathways. In early summer, air masses came primarily from the Indian Ocean and spent a long time over the continent. The transport of sulphur compounds is related to sea spray aerosols and the resulting condensation of H2SO4 and MSA over

  2. Vertical Transport of Aerosol Particles across Mountain Topography near the Los Angeles Basin

    NASA Astrophysics Data System (ADS)

    Murray, J. J.; Schill, S.; Freeman, S.; Bertram, T. H.; Lefer, B. L.

    2015-12-01

    Transport of aerosol particles is known to affect air quality and is largely dependent on the characteristic topography of the surrounding region. To characterize this transport, aerosol number distributions were collected with an Ultra-High Sensitivity Aerosol Spectrometer (UHSAS, DMT) during the 2015 NASA Student Airborne Research Program (SARP) in and around the Los Angeles Basin in Southern California. Increases in particle number concentration and size were observed over mountainous terrain north of Los Angeles County. Chemical analysis and meteorological lagrangian trajectories suggest orographic lifting processes, known as the "chimney effect". Implications for spatial transport and distribution will be discussed.

  3. Evolution of Asian aerosols during transpacific transport in INTEX-B

    SciTech Connect

    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.

  4. Chemical characterization of aerosol particles by laser Raman spectroscopy. Revision

    SciTech Connect

    Fung, K.H.

    1999-12-01

    The importance of aerosol particles in many branches of science, such as atmospheric chemistry, combustion, interfacial science, and material processing, has been steadily growing during the past decades. One of the unique properties of these particles is the very high surface-to-volume ratios, thus making them readily serve as centers for gas-phase condensation and heterogeneous reactions. These particles must be characterized by size, shape, physical state, and chemical composition. Traditionally, optical elastic scattering has been applied to obtain the physical properties of these particle (e.g., particle size, size distribution, and particle density). These physical properties are particularly important in atmospheric science as they govern the distribution and transport of atmospheric aerosols.

  5. Sources, Transport, and Climate Impacts of Biomass Burning Aerosols

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2010-01-01

    In this presentation, I will first talk about fundamentals of modeling of biomass burning emissions of aerosols, then show the results of GOCART model simulated biomass burning aerosols. I will compare the model results with observations of satellite and ground-based network in terms of total aerosol optical depth, aerosol absorption optical depth, and vertical distributions. Finally the long-range transport of biomass burning aerosols and the climate effects will be addressed. I will also discuss the uncertainties associated with modeling and observations of biomass burning aerosols

  6. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOEpatents

    Lee, Yin-Nan E.; Weber, Rodney J.

    2003-01-01

    An apparatus and method for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution are provided. The apparatus includes a modified particle size magnifier for producing activated aerosol particles and a collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical methods. The method provided for on-line measurement of chemical composition of aerosol particles includes exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

  7. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOEpatents

    Lee, Yin-Nan E.; Weber, Rodney J.; Orsini, Douglas

    2006-04-18

    An apparatus for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution is provided. The apparatus includes an enhanced particle size magnifier for producing activated aerosol particles and an enhanced collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical means. Methods for on-line measurement of chemical composition of aerosol particles are also provided, the method including exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; and flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

  8. Modeling comprehensive chemical composition of weathered oil following a marine spill to predict ozone and potential secondary aerosol formation and constrain transport pathways

    NASA Astrophysics Data System (ADS)

    Drozd, Greg T.; Worton, David R.; Aeppli, Christoph; Reddy, Christopher M.; Zhang, Haofei; Variano, Evan; Goldstein, Allen H.

    2015-11-01

    Releases of hydrocarbons from oil spills have large environmental impacts in both the ocean and atmosphere. Oil evaporation is not simply a mechanism of mass loss from the ocean, as it also causes production of atmospheric pollutants. Monitoring atmospheric emissions from oil spills must include a broad range of volatile organic compounds (VOC), including intermediate-volatile and semivolatile compounds (IVOC, SVOC), which cause secondary organic aerosol (SOA) and ozone production. The Deepwater Horizon (DWH) disaster in the northern Gulf of Mexico during Spring/Summer of 2010 presented a unique opportunity to observe SOA production due to an oil spill. To better understand these observations, we conducted measurements and modeled oil evaporation utilizing unprecedented comprehensive composition measurements, achieved by gas chromatography with vacuum ultraviolet time of flight mass spectrometry (GC-VUV-HR-ToFMS). All hydrocarbons with 10-30 carbons were classified by degree of branching, number of cyclic rings, aromaticity, and molecular weight; these hydrocarbons comprise ˜70% of total oil mass. Such detailed and comprehensive characterization of DWH oil allowed bottom-up estimates of oil evaporation kinetics. We developed an evaporative model, using solely our composition measurements and thermodynamic data, that is in excellent agreement with published mass evaporation rates and our wind-tunnel measurements. Using this model, we determine surface slick samples are composed of oil with a distribution of evaporative ages and identify and characterize probable subsurface transport of oil.

  9. Projected effect of 2000-2050 changes in climate and emissions on aerosol levels in China and associated transboundary transport

    EPA Science Inventory

    We investigate projected 2000–2050 changes in concentrations of aerosols in China and the associated transboundary aerosol transport by using the chemical transport model GEOS-Chem driven by the Goddard Institute for Space Studies (GISS) general circulation model (GCM) 3 at 4° × ...

  10. Street canyon aerosol pollutant transport measurements.

    PubMed

    Longley, I D; Gallagher, M W; Dorsey, J R; Flynn, M; Bower, K N; Allan, J D

    2004-12-01

    Current understanding of dispersion in street canyons is largely derived from relatively simple dispersion models. Such models are increasingly used in planning and regulation capacities but are based upon a limited understanding of the transport of substances within a real canyon. In recent years, some efforts have been made to numerically model localised flow in idealised canyons (e.g., J. Appl. Meteorol. 38 (1999) 1576-89) and stepped canyons (Assimakopoulos V. Numerical modelling of dispersion of atmospheric pollution in and above urban canopies. PhD thesis, Imperial College, London, 2001) but field studies in real canyons are rare. To further such an understanding, a measurement campaign has been conducted in an asymmetric street canyon with busy one-way traffic in central Manchester in northern England. The eddy correlation method was used to determine fluxes of size-segregated accumulation mode aerosol. Measurements of aerosol at a static location were made concurrently with measurements on a platform lift giving vertical profiles. Size-segregated measurements of ultrafine and coarse particle concentrations were also made simultaneously at various heights. In addition, a small mobile system was used to make measurements of turbulence at various pavement locations within the canyon. From this data, various features of turbulent transport and dispersion in the canyon will be presented. The concentration and the ventilation fluxes of vehicle-related aerosol pollutants from the canyon will be related to controlling factors. The results will also be compared with citywide ventilation data from a separate measurement campaign conducted above the urban canopy.

  11. Evaluating global atmospheric transport of plutonium with dust aerosols

    NASA Astrophysics Data System (ADS)

    Velarde, R.; Arimoto, R.; Gill, T. E.; Kang, C.; Goodell, P.

    2009-12-01

    The resuspension of soils contaminated with radionuclides from nuclear weapons tests is a mechanism by which plutonium can be re-distributed throughout the environment. To better understand the global atmospheric transport of plutonium, we measured the activity of Pu in aerosol samples from four widely separated sites that receive dust from distant sources in both Asia and Africa. High-volume aerosol samples were collected from Barbados (2005 - 2006); Gosan, South Korea (2005 - 2006); Izaña, Canary Islands (1989 - 1996); and Mauna Loa Observatory, Hawaii (2005 - 2006) to evaluate the relationship between Pu activity and mineral dust concentrations (using crustal elements such as aluminum as a dust proxy). The activity of 239,240Pu (239Pu + 240Pu) in the aerosol samples was determined by alpha spectrometry following a series of chemical separations. Concentrations of other elements were determined by a variety of techniques. Pu activity was below the detection limit in many samples. In those samples where it was detected, the Gosan site had the highest dust concentrations and highest total plutonium activity, while Mauna Loa Observatory had the lowest dust concentrations and lowest 239,240Pu activity. The Izaña samples had the second highest concentrations of dust and plutonium activity, while Barbados had the third highest levels of both crustal aerosols and plutonium activity. The dust concentrations are consistent with previous observations at these remote sites, and we propose that the plutonium (primarily from past atmospheric nuclear weapons testing, much of which took place in arid lands) was deposited on erodible soil surfaces and subsequently transported as part of the overall mineral dust load. The results of this study have implications for the global transport and fate of Pu through its association with dust, the biogeochemical and environmental impacts of other substances associated with dust, and the workings of the dust cycle itself.

  12. MELCOR aerosol transport module modification for NSSR-1

    SciTech Connect

    Merrill, B.J.; Hagrman, D.L.

    1996-03-01

    This report describes modifications of the MELCOR computer code aerosol transport module that will increase the accuracy of calculations for safety analysis of the International Thermonuclear Experimental Reactor (ITER). The modifications generalize aerosol deposition models to consider gases other than air, add specialized models for aerosol deposition during high speed gas flows in ducts, and add models for resuspension of aerosols that are entrained in coolants when these coolants flash. Particular attention has been paid to the adhesion of aerosol particles once they are transported to duct walls. The results of calculations with the modified models have been successfully compared to data from Light Water Reactor Aerosol Containment Experiments (LACE) conducted by an international consortium at Hanford, Washington.

  13. Aerosol Size and Chemical Composition in the Canadian High Arctic

    NASA Astrophysics Data System (ADS)

    Chang, R. Y. W.; Hayes, P. L.; Leaitch, W. R.; Croft, B.; O'Neill, N. T.; Fogal, P.; Drummond, J. R.; Sloan, J. J.

    2015-12-01

    Arctic aerosol have a strong annual cycle, with winter months dominated by long range transport from lower latitudes resulting in high mass loadings. Conversely, local emissions are more prominent in the summer months because of the decreased influence of transported aerosol, allowing us to regularly observe both transported and local aerosol. This study will present observations of aerosol chemical composition and particle number size distribution collected at the Polar Environment Artic Research Laboratory and the Alert Global Atmospheric Watch Observatory at Eureka (80N, 86W) and Alert (82N, 62W), Nunavut, respectively. Summer time observations of the number size distribution reveal a persistent mode of particles centered between 30-50 nm, with occasional bursts of smaller particles. The non-refractory aerosol chemical composition, measured by the Canadian Network for the Detection of Atmospheric Change quadrupole aerosol mass spectrometer, is primarily organic, with contributions from both aged and fresher organic aerosol. Factor analysis will be conducted to better understand these sources. The site at Eureka is more susceptible to long range transport since it is at the top of a mountain ridge (610 m above sea level) and will be compared to the site at Alert on an elevated plain (200 m above sea level). This will allow us to determine the relative contributions from processes and sources at the sites at different elevations. Comparisons with aerosol optical depth and GEOS-Chem model output will also be presented to put these surface measurements into context with the overlying and regional atmosphere. Results from this study contribute to our knowledge of aerosol in the high Arctic.

  14. Evaluation of liquid aerosol transport through porous media.

    PubMed

    Hall, R; Murdoch, L; Falta, R; Looney, B; Riha, B

    2016-07-01

    Application of remediation methods in contaminated vadose zones has been hindered by an inability to effectively distribute liquid- or solid-phase amendments. Injection as aerosols in a carrier gas could be a viable method for achieving useful distributions of amendments in unsaturated materials. The objectives of this work were to characterize radial transport of aerosols in unsaturated porous media, and to develop capabilities for predicting results of aerosol injection scenarios at the field-scale. Transport processes were investigated by conducting lab-scale injection experiments with radial flow geometry, and predictive capabilities were obtained by developing and validating a numerical model for simulating coupled aerosol transport, deposition, and multi-phase flow in porous media. Soybean oil was transported more than 2m through sand by injecting it as micron-scale aerosol droplets. Oil saturation in the sand increased with time to a maximum of 0.25, and decreased with radial distance in the experiments. The numerical analysis predicted the distribution of oil saturation with only minor calibration. The results indicated that evolution of oil saturation was controlled by aerosol deposition and subsequent flow of the liquid oil, and simulation requires including these two coupled processes. The calibrated model was used to evaluate field applications. The results suggest that amendments can be delivered to the vadose zone as aerosols, and that gas injection rate and aerosol particle size will be important controls on the process.

  15. Evaluation of liquid aerosol transport through porous media

    NASA Astrophysics Data System (ADS)

    Hall, R.; Murdoch, L.; Falta, R.; Looney, B.; Riha, B.

    2016-07-01

    Application of remediation methods in contaminated vadose zones has been hindered by an inability to effectively distribute liquid- or solid-phase amendments. Injection as aerosols in a carrier gas could be a viable method for achieving useful distributions of amendments in unsaturated materials. The objectives of this work were to characterize radial transport of aerosols in unsaturated porous media, and to develop capabilities for predicting results of aerosol injection scenarios at the field-scale. Transport processes were investigated by conducting lab-scale injection experiments with radial flow geometry, and predictive capabilities were obtained by developing and validating a numerical model for simulating coupled aerosol transport, deposition, and multi-phase flow in porous media. Soybean oil was transported more than 2 m through sand by injecting it as micron-scale aerosol droplets. Oil saturation in the sand increased with time to a maximum of 0.25, and decreased with radial distance in the experiments. The numerical analysis predicted the distribution of oil saturation with only minor calibration. The results indicated that evolution of oil saturation was controlled by aerosol deposition and subsequent flow of the liquid oil, and simulation requires including these two coupled processes. The calibrated model was used to evaluate field applications. The results suggest that amendments can be delivered to the vadose zone as aerosols, and that gas injection rate and aerosol particle size will be important controls on the process.

  16. Improving Aerosol Transport to the Arctic in CAM5

    NASA Astrophysics Data System (ADS)

    Wang, H.; Easter, R. C.; Rasch, P.; Wang, M.; Liu, X.; Ghan, S.; Qian, Y.; Yoon, J.; Ma, P.; Vinoj, V.

    2011-12-01

    Of the many factors contributing to the rapid arctic climate change, arctic haze has been identified as a potentially important forcing agent. It has been well established that arctic aerosols largely originate from lower latitudes. Hence, the long-range atmospheric transport of aerosols to the Arctic is of great concern for studying arctic climate change. The treatment of aerosol and cloud processes has been substantially improved in the current version of the Community Atmosphere Model (CAM5) which is widely used in the research of aerosol effects on clouds and climate. However, like many other global models, the CAM5 produces a relatively poor simulation of arctic aerosols and clouds. For example, previous studies have shown that the standard version of CAM5 remarkably underpredicts arctic aerosol concentrations, particularly during the arctic haze season, compared to various measurements. In this study, we focus on improving processes associated with aerosol-cloud interactions, cloud microphysics and macrophysics, and aerosol emission, transformation, removal, and deposition that are key to determining the amount of aerosols reaching the Arctic. Sensitivity experiments are conducted to understand the role of each of the processes and to identify sources of uncertainties, and improvements are made to processes that are not well represented in the CAM5. The evaluation and improvement are guided by aerosol and cloud measurements together with process-oriented model results from the multi-scale aerosol-climate model (PNNL-MMF) that embeds a cloud-resolving model in each CAM5 grid column to explicitly represent convection and aerosol-cloud interactions. Results show that including black carbon (BC) aging process through a more complete 7-mode version of the aerosol module in CAM5 can substantially increase the amount of arctic BC, compared to simulations with the standard 3-mode version, but has minimal effect on other species such as dust and sulfate. Excessive mid

  17. Aerosol Chemical and Physical Characterization in Central Amazonia during the 2013 Dry Season

    NASA Astrophysics Data System (ADS)

    Artaxo, P.; Stern, R.; Brito, J.; Carbone, S.

    2015-12-01

    During the dry season, the central Amazon forest is highly influenced by forest fires transported through large distances, changing drastically the atmospheric composition even in remote places. This work focuses on a physical-chemical characterization of the aerosol population over a pristine site in Central Amazonia during the dry season. The submicrometer organic aerosols were measured with the Aerodyne ACSM (Aerosol Chemical Speciation Monitor, Aerodyne Inc). Optical properties, size distribution and other micro-physical characteristics were also analyzed. Other instruments were simultaneously used. The measurements were taken during the dry season of 2013 in the Cuieiras ecological reserve (ZF2), northwest of Manaus. The statistical analysis of the data was done with the PMF (Positive Matrix Factorization) technique, in which the organic aerosol was separated into different factors, and then its sources and forming processes were attributed. Results show that the mean aerosol loading was 5,91 μg m-3, from which 78% are of organic composition, 8.5% are sulfate, 6.5% are equivalent black carbon, 4% are ammonium and 3% are nitrate. The mass spectra variability can be explained by 3 factors only, determined with the PMF technique. They were identified as BBOA (Biomass Burning Organic Aerosol), representing 12% of the total organic mass, OOA (Oxygenated Organic Aerosol), representing 66% of the total organic mass and IEPOX-SOA (Isoprene derived Epoxydiol-Secondary Organic Aerosol), representing 21% of the total organic mass. Even in remote and pristine regions, Central Amazonia is highly impacted by biomass burning. Biogenic secondary organic aerosols are also present during the dry season, and the suppression of its wet deposition processes increases their concentration. The oxidation level and other physical-chemical characteristics indicate that the long range transport is responsible for the regional range of this impact.

  18. Measurement of the emission rate of an aerosol source--comparison of aerosol and gas transport coefficients.

    PubMed

    Bémer, D; Callé, S; Godinot, S; Régnier, R; Dessagne, J M

    2000-12-01

    A measuring method of the emission rate of an atmospheric pollutant source, based on the use of a tracer gas (helium) and developed in the case of a gaseous source, was tested for an aerosol source. The influence of both particle sedimentation and wall depositions was studied. The transport coefficients of the tracer gas and of alumina particles of various particle sizes (MMAD from 8 to 36 microns) were measured on a vertical axis close to the source, in a 71 m3 room swept by a piston flow. The measurements clearly demonstrated the predominant influence of sedimentation in the case of particles with aerodynamic diameters greater than 10 microns. Particle wall deposition was determined by measuring the gas and particle concentration decay in the ventilated room. To do this, a new tracing method using a fluorescent aerosol was developed. The measured aerosol deposition rates are much higher than those calculated from the formula of Corner for a cubical volume. Aerosol sedimentation and wall deposition are two phenomena limiting the use of a tracer gas to measure the aerosol emission rate. The chemical substances and materials used in work premises are likely to be released into the atmosphere and lead to the formation of pollutants. These emissions stem from either physical or chemical processes (evaporation of a solvent) or from mechanical processes (dispersion of oil droplets at the source of mists).

  19. Simulation of aerosol chemical compositions in the Western Mediterranean Sea

    NASA Astrophysics Data System (ADS)

    Chrit, Mounir; Kata Sartelet, Karine; Sciare, Jean; Marchand, Nicolas; Pey, Jorge; Sellegri, Karine

    2016-04-01

    This work aims at evaluating the chemical transport model (CTM) Polair3d of the air-quality modelling platform Polyphemus during the ChArMex summer campaigns of 2013, using ground-based measurements performed at ERSA (Cape Corsica, France), and at determining the processes controlling organic aerosol concentrations at ERSA. Simulations are compared to measurements for concentrations of both organic and inorganic species, as well as the ratio of biogenic versus anthropogenic particles, and organic aerosol properties (oxidation state). For inorganics, the concentrations of sulphate, sodium, chloride, ammonium and nitrate are compared to measurements. Non-sea-salt sulphate and ammonium concentrations are well reproduced by the model. However, because of the geographic location of the measurement station at Cape Corsica which undergoes strong wind velocities and sea effects, sea-salt sulphate, sodium, chloride and nitrate concentrations are strongly influenced by the parameterizations used for sea-salt emissions. Different parameterizations are compared and a parameterization is chosen after comparison to sodium measurements. For organics, the concentrations are well modelled when compared to experimental values. Anthropogenic particles are influenced by emission of semi-volatile organic compounds (SVOC). Measurements allow us to refine the estimation of those emissions, which are currently missing in emission inventories. Although concentrations of biogenic particles are well simulated, the organic chemical compounds are not enough oxidised in the model. The observed oxidation state of organics shows that the oligomerisation of pinonaldehyde was over-estimated in Polyphemus. To improve the oxidation property of organics, the formation of extremely low volatile organic compounds from autoxidation of monoterpenes is added to Polyphemus, using recently published data from chamber experiments. These chemical compounds are highly oxygenated and are formed rapidly, as first

  20. Results from simulated upper-plenum aerosol transport and aerosol resuspension experiments

    SciTech Connect

    Wright, A.L.; Pattison, W.L.

    1984-01-01

    Recent calculational results published as part of the Battelle-Columbus BMI-2104 source term study indicate that, for some LWR accident sequences, aerosol deposition in the reactor primary coolant system (PCS) can lead to significant reductions in the radionuclide source term. Aerosol transport and deposition in the PCS have been calculated in this study using the TRAP-MELT 2 computer code, which was developed at Battelle-Columbus; the status of validation of the TRAP-MELT 2 code has been described in an Oak Ridge National Laboratory (ORNL) report. The objective of the ORNL TRAP-MELT Validation Project, which is sponsored by the Fuel Systems Behavior Research Branch of the US Nuclear Regulatory Commission, is to conduct simulated reactor-vessel upper-plenum aerosol deposition and transport tests. The results from these tests will be used in the ongoing effort to validate TRAP-MELT 2. The TRAP-MELT Validation Project includes two experimental subtasks. In the Aerosol Transport Tests, aerosol transport in a vertical pipe is being studied; this geometry was chosen to simulate aerosol deposition and transport in the reactor-vessel upper-plenum. To date, four experiments have been performed; the results from these tests are presented in this paper. 7 refs., 4 figs., 4 tabs.

  1. Chemical characterization of secondary organic aerosol constituents from isoprene ozonolysis in the presence of acidic aerosol

    NASA Astrophysics Data System (ADS)

    Riva, Matthieu; Budisulistiorini, Sri Hapsari; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.

    2016-04-01

    Isoprene is the most abundant non-methane hydrocarbon emitted into Earth's atmosphere and is predominantly derived from terrestrial vegetation. Prior studies have focused largely on the hydroxyl (OH) radical-initiated oxidation of isoprene and have demonstrated that highly oxidized compounds, such as isoprene-derived epoxides, enhance the formation of secondary organic aerosol (SOA) through heterogeneous (multiphase) reactions on acidified sulfate aerosol. However, studies on the impact of acidified sulfate aerosol on SOA formation from isoprene ozonolysis are lacking and the current work systematically examines this reaction. SOA was generated in an indoor smog chamber from isoprene ozonolysis under dark conditions in the presence of non-acidified or acidified sulfate seed aerosol. The effect of OH radicals on SOA chemical composition was investigated using diethyl ether as an OH radical scavenger. Aerosols were collected and chemically characterized by ultra performance liquid chromatography/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) and gas chromatography/electron impact ionization-mass spectrometry (GC/EI-MS). Analysis revealed the formation of highly oxidized compounds, including organosulfates (OSs) and 2-methylterols, which were significantly enhanced in the presence of acidified sulfate seed aerosol. OSs identified in the chamber experiments were also observed and quantified in summertime fine aerosol collected from two rural locations in the southeastern United States during the 2013 Southern Oxidant and Aerosol Study (SOAS).

  2. Measurements of aerosol chemical composition in boreal forest summer conditions

    NASA Astrophysics Data System (ADS)

    ńijälä, M.; Junninen, H.; Ehn, M.; Petäjä, T.; Vogel, A.; Hoffmann, T.; Corrigan, A.; Russell, L.; Makkonen, U.; Virkkula, A.; Mäntykenttä, J.; Kulmala, M.; Worsnop, D.

    2012-04-01

    Boreal forests are an important biome, covering vast areas of the northern hemisphere and affecting the global climate change via various feedbacks [1]. Despite having relatively few anthropogenic primary aerosol sources, they always contain a non-negligible aerosol population [2]. This study describes aerosol chemical composition measurements using Aerodyne Aerosol Mass Spectrometer (C-ToF AMS, [3]), carried out at a boreal forest area in Hyytiälä, Southern Finland. The site, Helsinki University SMEAR II measurement station [4], is situated at a homogeneous Scots pine (Pinus sylvestris) forest stand. In addition to the station's permanent aerosol, gas phase and meteorological instruments, during the HUMPPA (Hyytiälä United Measurements of Photochemistry and Particles in Air) campaign in July 2010, a very comprehensive set of atmospheric chemistry measurement instrumentation was provided by the Max Planck Institute for chemistry, Johannes Gutenberg-University, University of California and the Finnish Meteorological institute. In this study aerosol chemical composition measurements from the campaign are presented. The dominant aerosol chemical species during the campaign were the organics, although periods with elevated amounts of particulate sulfates were also seen. The overall AMS measured particle mass concentrations varied from near zero to 27 μg/m observed during a forest fire smoke episode. The AMS measured aerosol mass loadings were found to agree well with DMPS derived mass concentrations (r2=0.998). The AMS data was also compared with three other aerosol instruments. The Marga instrument [5] was used to provide a quantitative semi-online measurement of inorganic chemical compounds in particle phase. Fourier Transform Infrared Spectroscopy (FTIR) analysis was performed on daily filter samples, enabling the identification and quantification of organic aerosol subspecies. Finally an Atmospheric Pressure Chemical Ionization Ion Trap Mass Spectrometer (APCI

  3. Characterization of aerosol transport in a recoil transfer chamber for heavy element chemistry

    NASA Astrophysics Data System (ADS)

    Lopez Morales, Gabriel; Tereshatov, Evgeny; Folden, Charles

    2014-09-01

    Heavy elements (HE) are elements with Z >103 that can be synthesized via target material bombardment by accelerated charged particles. Production and investigation of properties of new elements result in understanding of upper limit of Periodic Table of Elements. Study of chemical behavior of HE is usually based on comparison with their light homologue properties. Such experiments require transportation of elements of interest from a target chamber to a radiochemical laboratory within several seconds. Aerosol transport is a widely known way to transfer non-volatile elements in on-line experiments. This particular project is devoted to design, characterization and optimization of aerosol transport for implementation in future experiments at Cyclotron Institute, Texas A&M University. Different types of aerosol generators and particle parameters such as: size distribution, concentration and charge have been considered. Results showing procedure development will be presented. *Funded by DOE and NSF-REU Program.

  4. Chemical distribution in high-solids paint overspray aerosols.

    PubMed

    D'Arcy, J B; Chan, T L

    1990-03-01

    The chemical composition of high-solids basecoat paint overspray aerosols was determined as a function of particle size. Detailed information on the chemical composition of the overspray aerosols is important in health hazard evaluation since the composition and distribution within the airborne particles may differ significantly from the bulk paint material. This study was conducted in a typical down-draft paint booth equipped with air-atomized spray painting equipment. A fixed paint target was used to simulate typical overspray generation conditions and the aerosols were collected isokinetically with a seven-stage cascade impactor for size-fractionated analysis. The overspray aerosol from six paints consisted of organic paint binders with varying amounts of inorganic species as pigments or luster enhancers. These overspray aerosols had mass median aerodynamic diameters (MMAD) ranging from 2.9 to 9.7 microns. The size-fractionated paint samples collected on the impaction stages were analyzed by energy dispersive X-ray spectrometry on a scanning electron microscope (SEM-EDXRS) to identify the metallic elements. Atomic absorption spectrometry was used to determine the mass distribution of aluminum and iron as indicators of nonuniform distribution. Three of the aerosols containing aluminum were found to have bimodal distributions with most aluminum distributions having cumulative MMADs larger than the total aerosol. Iron in the aerosols was bimodal for three of the paints with all samples having an overall iron MMAD less than or equal to the overspray aerosol MMAD. Analysis using ultraviolet spectrometry revealed that the organic compounds present in the size-fractionated particulate samples consisted of a single, polydispersed mode with an MMAD similar to that of the total overspray aerosol.(ABSTRACT TRUNCATED AT 250 WORDS) PMID:2327324

  5. Chemical distribution in high-solids paint overspray aerosols

    SciTech Connect

    D'Arcy, J.B.; Chan, T.L. )

    1990-03-01

    The chemical composition of high-solids basecoat paint overspray aerosols was determined as a function of particle size. Detailed information on the chemical composition of the overspray aerosols is important in health hazard evaluation since the composition and distribution within the airborne particles may differ significantly from the bulk paint material. This study was conducted in a typical down-draft paint booth equipped with air-atomized spray painting equipment. A fixed paint target was used to simulate typical overspray generation conditions and the aerosols were collected isokinetically with a seven-stage cascade impactor for size-fractionated analysis. The overspray aerosol from six paints consisted of organic paint binders with varying amounts of inorganic species as pigments or luster enhancers. These overspray aerosols had mass median aerodynamic diameters (MMAD) ranging from 2.9 to 9.7 microns. The size-fractionated paint samples collected on the impaction stages were analyzed by energy dispersive X-ray spectrometry on a scanning electron microscope (SEM-EDXRS) to identify the metallic elements. Atomic absorption spectrometry was used to determine the mass distribution of aluminum and iron as indicators of nonuniform distribution. Three of the aerosols containing aluminum were found to have bimodal distributions with most aluminum distributions having cumulative MMADs larger than the total aerosol. Iron in the aerosols was bimodal for three of the paints with all samples having an overall iron MMAD less than or equal to the overspray aerosol MMAD. Analysis using ultraviolet spectrometry revealed that the organic compounds present in the size-fractionated particulate samples consisted of a single, polydispersed mode with an MMAD similar to that of the total overspray aerosol.

  6. CCN frequency distributions and aerosol chemical composition from long-term observations at European ACTRIS supersites

    NASA Astrophysics Data System (ADS)

    Decesari, Stefano; Rinaldi, Matteo; Schmale, Julia Yvonne; Gysel, Martin; Fröhlich, Roman; Poulain, Laurent; Henning, Silvia; Stratmann, Frank; Facchini, Maria Cristina

    2016-04-01

    Cloud droplet number concentration is regulated by the availability of aerosol acting as cloud condensation nuclei (CCN). Predicting the air concentrations of CCN involves knowledge of all physical and chemical processes that contribute to shape the particle size distribution and determine aerosol hygroscopicity. The relevance of specific atmospheric processes (e.g., nucleation, coagulation, condensation of secondary organic and inorganic aerosol, etc.) is time- and site-dependent, therefore the availability of long-term, time-resolved aerosol observations at locations representative of diverse environments is strategic for the validation of state-of-the-art chemical transport models suited to predict CCN concentrations. We focused on long-term (year-long) datasets of CCN and of aerosol composition data including black carbon, and inorganic as well as organic compounds from the Aerosol Chemical Speciation Monitor (ACSM) at selected ACTRIS supersites (http://www.actris.eu/). We discuss here the joint frequency distribution of CCN levels and of aerosol chemical components concentrations for two stations: an alpine site (Jungfraujoch, CH) and a central European rural site (Melpitz, DE). The CCN frequency distributions at Jungfraujoch are broad and generally correlated with the distributions of the concentrations of aerosol chemical components (e.g., high CCN concentrations are most frequently found for high organic matter or black carbon concentrations, and vice versa), which can be explained as an effect of the strong seasonality in the aerosol characteristics at the mountain site. The CCN frequency distributions in Melpitz show a much weaker overlap with the distributions of BC concentrations or other chemical compounds. However, especially at high CCN concentration levels, a statistical correlation with organic matter (OM) concentration can be observed. For instance, the number of CCN (with particle diameter between 20 and 250 nm) at a supersaturation of 0.7% is

  7. Analysis of the chemical and physical properties of combustion aerosols: Properties overview

    EPA Science Inventory

    Aerosol chemical composition is remarkably complex. Combustion aerosols can comprise tens of thousands of organic compounds and fragments, refractory carbon, metals, cations, anions, salts, and other inorganic phases and substituents [Hays et al., 2004]. Aerosol organic matter no...

  8. Physical and Chemical Characterization of Carbonaceous Aerosols in Korea

    NASA Astrophysics Data System (ADS)

    Choung, S.; Jin, J. S.; Hwang, G. S.; Jang, K. S.; Han, W. S.; OH, J.; Kwon, Y.

    2014-12-01

    Atmospheric aerosols have been recently paid attention more in environmental research due to their negative effects on air quality, public health, and climate change. The aerosols contain approximately >20-50% carbonaceous components such as organic carbon (OC) and black carbon (BC) (or elemental carbon [EC]) derived from organic compounds, biomass burning, and incomplete combustion of fossil fuels. The physical, chemical, and biological properties of atmospheric aerosols are strongly dependent on the carbonaceous components. In particular, the BC could significantly affect the regional air quality in the northeastern Asia, because China is one of the foremost BC emission country in the world. Previous studies have mainly focused on the quantification and source identification for carbonaceous aerosols. However, understanding of physical and chemical properties for the carbonaceous aerosols related to environmental contamination and toxicity was still incomplete due to analytical difficulties. This study is addressed to evaluate the contribution of carbonaceous aerosols to air pollution through the surface, mass spectroscopic, and electron microscopic analyses, and determination of chemical composition and structure using the air particulate matter (PM2.5 and >PM2.5) samples.

  9. Physical and chemical characterization of marine atmospheric aerosols over the North and South Pacific Oceans using single particle mass spectrometry

    NASA Astrophysics Data System (ADS)

    Furutani, H.; Jung, J.; Miura, K.; Uematsu, M.

    2010-12-01

    Physical and chemical properties of marine atmospheric aerosols were characterized and compared over the North and South Pacific Ocean during two trans-Pacific cruises (from Japan to Chile and Australia to Japan) during the period of January-June 2009, which cover broad region of Pacific Ocean from 40°N to 55°S and 140°E to 70°W. The measured parameters of aerosol properties were single particle size-resolved chemical composition (D = 100 ~ 1500 nm), cloud condensation nuclei (CCN) and condensation nuclei (CN) concentrations, size distribution from 10 nm to 5 μm, total aerosol nitrate and sulfate concentrations, and filter-based chemical composition. Trace gas concentrations of O3 and CO were also measured to aid air parcel categorization during the cruises. Reflecting larger anthropogenic emission in the Northern Hemisphere, pronounced concentration gradient between the North and South Pacific Ocean was observed for aerosol nitrate, CO, and O3. Aerosol sulfate also showed a similar concentration drop in the equatorial region, relatively higher sulfate concentration was observed in 30°S-40°S and 55°S regions, which was associated with increased aerosol methanesulfonic acid (MSA) concentration but little increase in local marine chlorophyll concentration, suggesting contribution of long-range transported marine biogenic sulfur from the high primary production area over the South Pacific high latitude region. Aerosol chemical classification by single particle chemical analysis revealed that certain aerosol types, such as biomass burning, elemental carbon, and elemental/organic carbon mixed type, were mainly observed in the North Pacific region, while several specific organic aerosol types with abundant aged organic and disulfur composition were identified in the South Pacific region. Further comparison of aerosol properties, aerosol sources, and atmospheric aerosol processing in the North and South Pacific Oceans will be discussed.

  10. Chemical Transport--Coping with Disasters.

    ERIC Educational Resources Information Center

    Rawls, Rebecca L.

    1980-01-01

    Describes operations of CHEMTREC, a chemical emergency information system supported by the Chemical Manufacturer's Association. Presents data on transportation incidents involving hazardous materials and the most frequently involved chemicals in transportation incidents. (CS)

  11. On the Vertical Distribution of Aerosols and Long-Range Transport Inferred from Calipso Satellite Observations

    NASA Astrophysics Data System (ADS)

    Trepte, Charles; Winker, David; Kittaka, Chieko

    Knowledge on the long-range transport and evolution of aerosols originating from natural and anthropogenic sources is important for understanding their impact on the composition of the atmosphere and the climate system. Over the past several decades a wealth of information on aerosol distributions has been obtained from ground-based instrument networks, dedicated field experiments, and passive remote sensing satellite instruments that has helped to establish the primary aerosol transport pathways over the globe. In many instances, these pathways are broadly reproduced geographically in different chemical-transport models. The models, however, have difficulties at times with accurately projecting the vertical distribution of aerosols, which can lead to significant discrepancies in the lifetimes of the modeled aerosols. This issue is compounded at high latitudes where observations are especially sparse. New measurements from the CALIPSO satellite mission can provide additional insight on the vertical distribution of aerosols over the globe. The mission is a joint effort between the United States (NASA) and France (CNES) and was launched on April 28, 2008 into the A-train satellite constellation. CALIPSO's primary instrument is a two-wavelength polarization-sensitive lidar operating at 532 and 1064 nm with a repetition rate of 20.16 Hz. Lidar observations in the lower troposphere (¡ 8 km) have a vertical resolution of 30 m for the 532 nm channel and 60 m for the 1064 channel. The instrument has been operational since early June 2006. The CALIPSO data set reveals a rich distribution of aerosols in clear and cloudy scenes for both day and night conditions. Information on aerosol type is also available based on their wavelength dependence and polarization characteristics. From these data, a climatology on the vertical and geographic distribution and optical characteristics of aerosols (and clouds) is being developed that can aid diagnostic studies of aerosol transport

  12. Seasonal variations in the physico-chemical characteristics of aerosols in North Taiwan

    NASA Astrophysics Data System (ADS)

    Chou, Charles

    2014-05-01

    From 2007 to 2012, this study investigated the mass concentration and chemical composition of ambient aerosols (i.e. PM10, PM2.5, and PMc = PM10-PM2.5) at Cape Fuguei, Yangminshan, and NTU (National Taiwan University) stations in northern Taiwan. It was found that the concentration and composition of aerosols exhibited significant seasonal variations but without an inter-annual trend during the study period. Moderate correlations (R2 = 0.4-0.6) were observed among the aerosol concentrations at the respective stations, indicating that the aerosol concentrations were dominated by factors on regional scales. During the seasons of northeasterly winter monsoons, long range transport of dust and particulate air pollutants from the Asia Continent had negatively impacted the atmospheric environment in this area. On the other hand, as a highly developed urban area, Taipei has substantial local emissions of air pollutants that should have transported to the surrounding areas of Taipei basin and caused deterioration of air quality and visibility in Cape Fuguei and Yangminshan. The results indicated that the major components of aerosols in Taipei include sulfate, sea salts, dust, and organic matters. In addition, contributions from nitrate, ammonium, and elemental carbon were also significant. In terms of mass concentration, most of the sea salts and dust particles existed in the coarse mode of aerosols, whereas sulfate and EC were confined within PM2.5. This suggests that the dust and sea salts particles were externally mixed with EC and sulfate in the aerosols over Taipei area. Further, it was found that nitrate were closely associated with sea salts in aerosols, suggesting the reaction between nitric acid and sea salt particles. Different seasonality was observed for sea salt and dust: sea salts peaked in fall and dust reached the maximal level in springtime, implying their sources were regulated by independent seasonal factors. Particulate pollutants (i.e. sulfate, nitrate

  13. Stratospheric aerosol modification by supersonic transport operations with climate implications

    NASA Technical Reports Server (NTRS)

    Toon, O. B.; Turco, R. P.; Pollack, J. B.; Whitten, R. C.; Poppoff, I. G.; Hamill, P.

    1980-01-01

    The potential effects on stratospheric aerosois of supersonic transport emissions of sulfur dioxide gas and submicron size soot granules are estimated. An interactive particle-gas model of the stratospheric aerosol is used to compute particle changes due to exhaust emissions, and an accurate radiation transport model is used to compute the attendant surface temperature changes. It is shown that a fleet of several hundred supersonic aircraft, operating daily at 20 km, could produce about a 20% increase in the concentration of large particles in the stratosphere. Aerosol increases of this magnitude would reduce the global surface temperature by less than 0.01 K.

  14. Chemical characterizations of soluble aerosols in southern China.

    PubMed

    Wu, Dui; Tie, Xuexi; Deng, Xuejiao

    2006-07-01

    Soluble aerosols are measured at Guangdong and Hainan Provinces of southern China. The measured chemical composition of aerosols includes F-, Cl-, NO3-, SO4=, Na+, NH4+, K+, Ca2+, and Mg2+. The locations of measurements include a mega city (Guangzhou), a medium city along the coastline (Haiko), a small city along the coastline (Shanya), and a remote island site in the South China Sea (Yongxing island). The results reveal that aerosols in this region are complex and heterogeneous. Sulfate aerosol (SO4=) has the highest concentrations in Guangzhou (approximately 41% of total soluble aerosol mass), suggesting that anthropogenic activities (e.g., coal burning) play important roles in controlling aerosol concentrations in Guangzhou. By contrast, the concentrations of chlorine (Cl-) and sodium (Na+) are higher in Yongxing than in Guangzhou, indicating that the sea salt is the dominant aerosol in this marine environment site. In the medium (Haiko) and small (Shanya) city sites, the effects of anthropogenic and marine activities on aerosols fall in between the values in the mega city and the remote island site. The measured ratio of Cl-/Na+ shows that the ratio is less than 1.16 in all observation sites. The ratio in the Guangzhou city, the Haiko city, the Shanya city, and the Yongxing island is 0.52, 0.91, 0.24, and 0.53, respectively, indicating that significantly heterogeneous chemical reactions occur on sea salt particles. Unlike those in Europe and North America, there are high concentrations of calcium (Ca+) in all observation sites. The percentage of calcium mass to the measured total soluble aerosols mass is 21, 32, 34, and 30 at Guangzhou, Haiko, Sanya, and Yongxing, respectively. The calculations show that calcium plays an important role in neutralizing aerosols. The calculated "cation/anion" (summation operator[ion+]/summation operator[ion-]) ratio is 2.5, 2.5, 3.2, and 2.1, at Guangzhou, Haiko, Shanya, and Yongxing, respectively. The high "cation/anion" ratios

  15. Intercontinental Transport of Aerosols: Implication for Regional Air Quality

    NASA Technical Reports Server (NTRS)

    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 < 10 microns) and PM2.5 (particles with diameter 2.5 microns) are 50 pg/cu m and 15 pg/cu m, respectively. While local and regional emission sources are the main cause of 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.

  16. All year round chemical composition of aerosol reaching the inner Antarctic Plateau (Dome C - East Antarctica)

    NASA Astrophysics Data System (ADS)

    Udisti, R.; Becagli, S.; Castellano, E.; Cerri, O.; Marino, F.; Morganti, A.; Nava, S.; Rugi, F.; Severi, M.; Traversi, R.

    2009-04-01

    Since 2005, continuous, all-year-round aerosol sampling was carried out at Dome C (Central East Antarctica, 3233 m a.s.l., about 1100 km far from the coast-line), in the framework of Station Concordia project. Size-segregated aerosol samples were collected in summer and winter period by using different low- and medium-volume systems, including pre-selected cut-off samplers (with PM10, PM2.5 and PM1 heads) and multi-stage (Andersen 8-stage and Dekati 4-stage) impactors. Sampling resolution and volume range from 1 day to 1 month and from 2.3 to 12 m3/h respectively. Aerosol study at Dome C aims to improve our knowledge on present day source intensity, transport efficiency and pathways (including stratosphere-to-troposphere interchanges) of particles reaching internal sites of Antarctica and to understand size- and chemical-fractionation effects occurring during the transport (by comparison with coastal aerosol composition). Besides, more information on atmosphere-snow interaction, including depositional and post depositional processes, as well as the effect of sublimation/condensation processes on snow surface, improves the reconstruction of past atmosphere composition from EPICA-DC deep ice core, drilled in the same site. Here we report some results of the chemical composition of the Antarctic background aerosol reaching Dome C, pointing out the seasonal pattern and the temporal trend of some ionic components used as tracers of sea spray, marine biogenic and crustal emissions. The atmospheric load in the summer is more than one order of magnitude lower than that measured in coastal sites and chemical composition is dominated by secondary aerosol, mainly originated by biological marine activity (S-cycle), and distributed in the finest aerosol fractions. H2SO4 from oxidation of biogenic DMS is the main component, while the contribution of HNO3 to the ionic budget is difficult to evaluate because of the re-emission into the atmosphere from the filter surface (acidic

  17. Long-range transport of aerosols from agriculture crop residue burning in Indo-Gangetic Plains—A study using LIDAR, ground measurements and satellite data

    NASA Astrophysics Data System (ADS)

    Badarinath, K. V. S.; Kumar Kharol, Shailesh; Rani Sharma, Anu

    2009-01-01

    Agriculture crop residue burning in tropics is an important source of atmospheric aerosols and monitoring their long-range transport is an important element in climate change studies. Synchronous measurements using micro-pulsed lidar, MICROTOPS-II sun photometer, multi-filter rotating shadow band radiometer (MFRSR) on aerosol optical depth and ground reaching solar irradiance were carried at an urban location in central region of India. Aerosol backscatter profiles obtained from micro-pulse lidar showed elevated aerosol layers up to ~3 km on certain days during October 2007. Satellite data observations on aerosol properties suggested transport of particles from agriculture crop residue burning in Indo-Gangetic Plains over large regions. Radiative forcing of aerosols estimated from SBDART model with input information on aerosol chemical properties, aerosol optical depth and single scattering albedo and broadband solar irradiance measurements using MFRSR showed good correlation (R=0.98).

  18. Physico-chemical properties of aerosols in Sao Paulo, Brazil and mechanisms of secondary organic aerosol formation.

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Ferreira de Brito, Joel; Varanda Rizzo, Luciana; Luiza Godoy, Maria; Godoy, Jose Marcus

    2013-04-01

    Megacities emissions are increasingly becoming a global issue, where emissions from the transportation sector play an increasingly important role. Sao Paulo is a megacity with a population of about 18 million people, 7 million cars and large-scale industrial emissions. As a result of the vehicular and industrial emissions, the air quality in Sao Paulo is bellow WMO standards for aerosol particles and ozone. Many uncertainties are found on gas- and particulate matter vehicular emission factors and their following atmospheric processes, e.g. secondary organic aerosol formation. Due to the uniqueness of the vehicular fuel in Brazil, largely based on ethanol use, such characterization currently holds further uncertainties. To improve the understanding of the role of this unique emission characteristics, we are running a source apportionment study in Sao Paulo focused on the mechanisms of organic aerosol formation. One of the goals of this study is a quantitative aerosol source apportionment focused on vehicular emissions, including ethanol and gasohol (both fuels used by light-duty vehicles). This study comprises four sampling sites with continuous measurements for one year, where trace elements and organic aerosol are being measured for PM2.5 and PM10 along with real-time NOx, O3, PM10 and CO measurements. Aerosol optical properties and size distribution are being measured on a rotation basis between sampling stations. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to measure in real time VOCs and aerosol composition, respectively. Trace elements were measured using XRF and OC/EC analysis was determined with a Sunset OC/EC instrument. A TSI Nephelometer with 3 wavelengths measure light scattering and a MAAP measure black carbon. Results show aerosol number concentrations ranging between 10,000 and 35,000 cm-3, mostly concentrated in the nucleation and Aitken modes, with a peak in size at 80

  19. Atmospheric Transport of Arid Aerosol from Desert Regions of Central Asia

    NASA Astrophysics Data System (ADS)

    Chen, Boris; Solomon, Paul; Sitnov, Sergei; Grechko, Evgeny; Maximenkov, Leonid; Artamonova, Maria; Pogarski, Fedor

    2010-05-01

    Investigation of atmospheric transport of arid aerosol from Central Asia was held within the ISTC project 3715. Particular attention was paid to the removal of aerosol from the Aral Sea region and its further transport, because aerosol and pollutants emission from Central Asia affect the airspace of the entire Asian continent. At the same time measurements of aerosols in the atmosphere of Central Asia are holding in a small number of stations, and currently available data are insufficient to define the initial conditions and/or verification of models of long-range transport. To identify sources of pollution transported from Central Asia, in Kyrgyzstan measurement and sampling of air were organized: at the station on the northern slope of the Kirgiz Range, 30 km south of Bishkek, at an altitude of 1700 m above sea level (Bishkek Site, 42,683N; 74,694E ), and on permanent alpine Teploklyuchenka lidar station in the Central Tien Shan at an altitude of 2000 m above sea level (Lidar Site, 42,467N; 78,533E). The chemical analysis of collected aerosol and soils samples was carried out. Measurements of aerosol at these stations have been merged with the simulation of the trajectories of air masses in the study region and with the satellite (the Terra and Aqua satellites) observations of aerosol optical thickness in this region. Satellite data for the region 43-47 N, and 58-62 E (Aral Sea) from April 2008 to September 2009 were analyzed. The moments were selected, when the value of aerosol optical thickness (AOT) was greatest (more than 0.5), and the transport from the Aral Sea region to the observation sites took place. For each of these days, the forward trajectories, which started at 6 points within the region, were calculated using the HYSPLIT model. The days, on which the trajectories reached the BISHKEK and LIDAR sites, were determined from the data obtained. Calculations on the basis of the RAMS model were performed for these days. These calculations were performed

  20. Transported acid aerosols measured in southern Ontario

    NASA Astrophysics Data System (ADS)

    Keeler, Gerald J.; Spengler, John D.; Koutrakis, Petros; Allen, George A.; Raizenne, Mark; Stern, Bonnie

    During the period 29 June 1986-9 August 1986, a field health study assessing the acute health effects of air pollutants on children was conducted at a summer girls' camp on the northern shore of Lake Erie in SW Ontario. Continuous air pollution measurements of SO 2, O 3, NO x, particulate sulfates, light scattering, and meteorological measurements including temperature, dew point, and wind speed and direction were made. Twelve-hour integrated samples of size fractioned particles were also obtained using dichotomous samplers and Harvard impactors equipped with an ammonia denuder for subsequent hydrogen ion determination. Particulate samples were analyzed for trace elements by X-ray fluorescence and Neutron Activation, and for organic and elemental carbon by a thermal/optical technique. The measured aerosol was periodically very acidic with observed 12-h averaged H + concentrations in the range < 10-560 nmoles m -3. The aerosol H + appeared to represent the net strong acidity after H 2SO 4 reaction with NH 3(g). Average daytime concentrations were higher than night-time for aerosol H +, sulfate, fine mass and ozone. Prolonged episodes of atmospheric acidity, sulfate, and ozone were associated with air masses arriving at the measurement site from the west and from the southwest over Lake Erie. Sulfate concentrations measured at the lakeshore camp were more than twice those measured at inland sites during extreme pollution episodes. The concentration gradient observed with onshore flow was potentially due to enhanced deposition near the lakeshore caused by discontinuities in the meteorological fields in this region.

  1. Hand calculations for transport of radioactive aerosols through sampling systems.

    PubMed

    Hogue, Mark; Thompson, Martha; Farfan, Eduardo; Hadlock, Dennis

    2014-05-01

    Workplace air monitoring programs for sampling radioactive aerosols in nuclear facilities sometimes must rely on sampling systems to move the air to a sample filter in a safe and convenient location. These systems may consist of probes, straight tubing, bends, contractions and other components. Evaluation of these systems for potential loss of radioactive aerosols is important because significant losses can occur. However, it can be very difficult to find fully described equations to model a system manually for a single particle size and even more difficult to evaluate total system efficiency for a polydispersed particle distribution. Some software methods are available, but they may not be directly applicable to the components being evaluated and they may not be completely documented or validated per current software quality assurance requirements. This paper offers a method to model radioactive aerosol transport in sampling systems that is transparent and easily updated with the most applicable models. Calculations are shown with the R Programming Language, but the method is adaptable to other scripting languages. The method has the advantage of transparency and easy verifiability. This paper shows how a set of equations from published aerosol science models may be applied to aspiration and transport efficiency of aerosols in common air sampling system components. An example application using R calculation scripts is demonstrated. The R scripts are provided as electronic attachments.

  2. Hand calculations for transport of radioactive aerosols through sampling systems.

    PubMed

    Hogue, Mark; Thompson, Martha; Farfan, Eduardo; Hadlock, Dennis

    2014-05-01

    Workplace air monitoring programs for sampling radioactive aerosols in nuclear facilities sometimes must rely on sampling systems to move the air to a sample filter in a safe and convenient location. These systems may consist of probes, straight tubing, bends, contractions and other components. Evaluation of these systems for potential loss of radioactive aerosols is important because significant losses can occur. However, it can be very difficult to find fully described equations to model a system manually for a single particle size and even more difficult to evaluate total system efficiency for a polydispersed particle distribution. Some software methods are available, but they may not be directly applicable to the components being evaluated and they may not be completely documented or validated per current software quality assurance requirements. This paper offers a method to model radioactive aerosol transport in sampling systems that is transparent and easily updated with the most applicable models. Calculations are shown with the R Programming Language, but the method is adaptable to other scripting languages. The method has the advantage of transparency and easy verifiability. This paper shows how a set of equations from published aerosol science models may be applied to aspiration and transport efficiency of aerosols in common air sampling system components. An example application using R calculation scripts is demonstrated. The R scripts are provided as electronic attachments. PMID:24667389

  3. Lake Spray Aerosol: A Chemical Signature from Individual Ambient Particles.

    PubMed

    Axson, Jessica L; May, Nathaniel W; Colón-Bernal, Isabel D; Pratt, Kerri A; Ault, Andrew P

    2016-09-20

    Aerosol production from wave breaking on freshwater lakes, including the Laurentian Great Lakes, is poorly understood in comparison to sea spray aerosol (SSA). Aerosols from freshwater have the potential to impact regional climate and public health. Herein, lake spray aerosol (LSA) is defined as aerosol generated from freshwater through bubble bursting, analogous to SSA from seawater. A chemical signature for LSA was determined from measurements of ambient particles collected on the southeastern shore of Lake Michigan during an event (July 6-8, 2015) with wave heights up to 3.1 m. For comparison, surface freshwater was collected, and LSA were generated in the laboratory. Single particle microscopy and mass spectrometry analysis of field and laboratory-generated samples show that LSA particles are primarily calcium (carbonate) with lower concentrations of other inorganic ions and organic material. Laboratory number size distributions show ultrafine and accumulation modes at 53 (±1) and 276 (±8) nm, respectively. This study provides the first chemical signature for LSA. LSA composition is shown to be coupled to Great Lakes water chemistry (Ca(2+) > Mg(2+) > Na(+) > K(+)) and distinct from SSA. Understanding LSA physicochemical properties will improve assessment of LSA impacts on regional air quality, climate, and health. PMID:27548099

  4. Lake Spray Aerosol: A Chemical Signature from Individual Ambient Particles.

    PubMed

    Axson, Jessica L; May, Nathaniel W; Colón-Bernal, Isabel D; Pratt, Kerri A; Ault, Andrew P

    2016-09-20

    Aerosol production from wave breaking on freshwater lakes, including the Laurentian Great Lakes, is poorly understood in comparison to sea spray aerosol (SSA). Aerosols from freshwater have the potential to impact regional climate and public health. Herein, lake spray aerosol (LSA) is defined as aerosol generated from freshwater through bubble bursting, analogous to SSA from seawater. A chemical signature for LSA was determined from measurements of ambient particles collected on the southeastern shore of Lake Michigan during an event (July 6-8, 2015) with wave heights up to 3.1 m. For comparison, surface freshwater was collected, and LSA were generated in the laboratory. Single particle microscopy and mass spectrometry analysis of field and laboratory-generated samples show that LSA particles are primarily calcium (carbonate) with lower concentrations of other inorganic ions and organic material. Laboratory number size distributions show ultrafine and accumulation modes at 53 (±1) and 276 (±8) nm, respectively. This study provides the first chemical signature for LSA. LSA composition is shown to be coupled to Great Lakes water chemistry (Ca(2+) > Mg(2+) > Na(+) > K(+)) and distinct from SSA. Understanding LSA physicochemical properties will improve assessment of LSA impacts on regional air quality, climate, and health.

  5. The Cloud-Aerosol Transport System (CATS): Demonstrating New Techniques for Cloud and Aerosol Measurements

    NASA Astrophysics Data System (ADS)

    Yorks, J. E.; McGill, M. J.; Palm, S. P.; Hlavka, D. L.; Nowottnick, E. P.; Selmer, P. A.

    2015-12-01

    The Cloud-Aerosol Transport System (CATS) is an elastic backscatter lidar that provides vertical profiles of cloud and aerosol properties. The CATS payload has been operating since early February 2015 from the International Space Station (ISS). CATS was designed to operate for six months, and up to three years, providing a combination of operational science, in-space technology demonstration, and technology risk reduction for future Earth Science missions. One of the primary project goals of CATS is to demonstrate technology in support of future space-based lidar mission development. The CATS instrument has been demonstrating the high repetition rate laser and photon counting detection approach to lidar observations, in contrast to the low repetition rate, high energy technique employed by CALIPSO. Due to this technique, cloud and aerosol profile data exhibit high spatial and temporal resolution, which was never before possible from a space-based platform. Another important science goal of the CATS-FO project is accurate determination of aerosol type on a global scale. CATS provided the first space-based depolarization measurements at multiple wavelengths (532 and 1064 nm), and first measurements at 1064 nm from space. The ratio of the depolarization measurements at these two wavelengths enables significant improvement in aerosol typing. The CATS retrievals at 1064 nm also provide improvements to detecting aerosols above clouds. The CATS layer identification algorithm is a threshold-based layer detection method that uses the 1064 nm attenuated scattering ratio and also includes a routine to identify clouds embedded within aerosol layers. This technique allows CATS to detect the full extent of the aerosol layers above the cloud, and differentiate these two layers so that the optical properties can be more accurately determined.

  6. Evolution of a Canadian biomass burning aerosol smoke plume transported to the U.S. East Coast

    NASA Astrophysics Data System (ADS)

    Miller, D. J.; Sun, K.; Zondlo, M. A.; Kanter, D.; Ginoux, P. A.

    2010-12-01

    We synthesize ground-based and satellite measurements to track the physical and chemical evolution of a biomass burning aerosol plume emitted in central Canada as it was transported to the U.S. East Coast. Biomass burning emissions strongly influence both air quality and radiative processes through trace gas and aerosol emissions. Organic carbon and black carbon smoke aerosols can be transported long distances downwind of the emissions source region. In some cases, biomass burning aerosol emissions have larger impacts than anthropogenic emissions, with implications for human health and aerosol radiative forcing on climate. Boreal forest fires in Canada on July 4, 2006 led to significant smoke aerosol emissions that were transported in layers at different altitudes over the Great Lakes to the northeastern United States. We track the aerosol plume with space-borne remote sensing satellite instrument (MODIS, OMI, MISR and CALIOP lidar) data as well as ground-based in-situ and remote aerosol observations (AERONET CIMEL sky/sun photometer, MPLNET lidar, IMPROVE and EPA AirNow). Combining total column, surface and vertical profile observations, we illustrate how plume altitude can affect spatial and temporal transport as well as optical and chemical properties. Convective lofting elevated smoke emissions above the boundary layer into the free troposphere (~3 km altitude) where higher speed winds led to rapid, long-range upper level transport to the Atlantic Ocean in 4-5 days. A lower aerosol layer led to enhancements in surface fine particulate matter (PM-2.5) mass concentrations accompanied by changes in aerosol composition as the plume mixed with anthropogenic sulfate aerosols. The extensive coverage of this smoke plume over the U.S. East Coast, a heavily populated region known for high anthropogenic aerosol loadings, significantly influenced regional air quality. Average PM-2.5 concentrations across Pennsylvania exceeded the U.S. EPA 24-hour PM-2.5 standard by 20.37

  7. Chemical Composition and Size Distributions of Coastal Aerosols Observed on the U.S. East Coast

    NASA Astrophysics Data System (ADS)

    Xia, L.; Song, F.; Jusino-Atresino, R.; Thuman, C.; Gao, Y.

    2008-12-01

    Aerosol input is an important source of certain limiting nutrients, such as iron, for phytoplankton growth in several large oceanic regions. As the efficiency of biological uptake of nutrients may depend on the aerosol properties, a better knowledge of aerosol properties is critically important. Characterizing aerosols over the coastal ocean needs special attention, because the properties of aerosols could be altered by many anthropogenic processes in this land-ocean transition zone before they are transported over the remote ocean. The goal of this experiment was to examine aerosol properties, in particular chemical composition, particle-size distributions and iron solubility, over the US Eastern Seaboard, an important boundary for the transport of continental substances from North America to the North Atlantic Ocean. Our field sampling site was located at Tuckerton (39°N, 74°W) on the southern New Jersey coast. Fourteen sets of High-Volume aerosol samples and three sets of size segregated aerosol samples by a 10-stage MOUDI impactor were collected during 2007 and 2008. The ICP-MS methodology was used to analyze aerosol samples for the concentrations of thirteen trace elements: Al, Fe, Mn, Sc, Cd, Pb, Sb, Ni, Co, Cr, Cu, Zn and V. The IC procedures were applied to determine five cations (sodium, ammonium, potassium, magnesium and calcium) and eleven anions (fluoride, acetate, propionate, formate, MSA, chloride, nitrate, succinate, malonate, sulfate and oxalate). The UV spectrometry was employed for the determination of iron solubility. Preliminary results suggest three major sources of aerosols: anthropogenic, crustal and marine. At this location, the concentrations of iron (II) ranged from 2.8 to 29ng m-3, accounting for ~20% of the total iron. The iron concentrations at this coastal site were substantially lower than those observed in Newark, an urban site in northern NJ. High concentrations of iron (II) were associated with both fine and coarse aerosol

  8. The conservative characteristic FD methods for atmospheric aerosol transport problems

    NASA Astrophysics Data System (ADS)

    Fu, Kai; Liang, Dong

    2016-01-01

    In the paper, we develop the new conservative characteristic finite difference methods (C-CFD) for the atmospheric aerosol transport problems. We propose the time second-order and spatial high-order conservative characteristic finite difference methods for the aerosol vertical advection-diffusion process and the two-dimensional conservative characteristic finite difference methods for aerosol horizontal transport process in the second-order splitting algorithm. Based on the characteristic form of advection-diffusion equations tracking back along the characteristic curve, we treat the integrals over the tracking cells at the previous time level by the conservative interpolations and propose to treat the diffusion terms by the average along the characteristics, where the high-order discrete fluxes are obtained by approximating the cumulative mass function and are continuous at the tracking points. The important feature is that the proposed C-CFD schemes preserve mass and have second-order accuracy in time and high-order accuracy in space. Numerical tests are taken to show the accuracy in time and space and mass conservation of our C-CFD schemes, compared with the standard CFD method. A real case of air quality modelling during the 2008 Beijing Olympics and a severe haze in North China are further simulated and analyzed by using our C-CFD algorithm. Simulated results are in good agreement with observations. The developed C-CFD algorithm can be used for efficiently solving large scale atmospheric aerosol transport problems.

  9. Unique DNA-barcoded aerosol test particles for studying aerosol transport

    DOE PAGES

    Harding, Ruth N.; Hara, Christine A.; Hall, Sara B.; Vitalis, Elizabeth A.; Thomas, Cynthia B.; Jones, A. Daniel; Day, James A.; Tur-Rojas, Vincent R.; Jorgensen, Trond; Herchert, Edwin; et al

    2016-03-22

    Data are presented for the first use of novel DNA-barcoded aerosol test particles that have been developed to track the fate of airborne contaminants in populated environments. Until DNATrax (DNA Tagged Reagents for Aerosol eXperiments) particles were developed, there was no way to rapidly validate air transport models with realistic particles in the respirable range of 1–10 μm in diameter. The DNATrax particles, developed at Lawrence Livermore National Laboratory (LLNL) and tested with the assistance of the Pentagon Force Protection Agency, are the first safe and effective materials for aerosol transport studies that are identified by DNA molecules. The usemore » of unique synthetic DNA barcodes overcomes the challenges of discerning the test material from pre-existing environmental or background contaminants (either naturally occurring or previously released). The DNATrax particle properties are demonstrated to have appropriate size range (approximately 1–4.5 μm in diameter) to accurately simulate bacterial spore transport. As a result, we describe details of the first field test of the DNATrax aerosol test particles in a large indoor facility.« less

  10. Characterization of the physical, chemical, and optical properties of atmospheric aerosol particles in New Hampshire

    NASA Astrophysics Data System (ADS)

    Slater, John Frederick

    Tropospheric aerosol particles directly affect the radiative budget of the Earth, and degrade visibility, by scattering and absorbing short-wavelength solar radiation. However, the radiative effect of aerosols is highly uncertain due to the non-uniform spatial distribution of the particles over Earth, their heterogeneous chemical composition, and their variable size. This dissertation quantifies some of the physical, chemical, and optical (radiative) properties of aerosols at different locations within New Hampshire (NH) from spring 2000 to fall 2001. During spring 2000, a 1-month study conducted at a mountaintop location adjacent to the White Mountain National Forest in northern NH showed that synoptic-scale air mass transport heavily influenced aerosol properties, and hence regional visibility. During W/SW flow, aerosol parameters and haziness were generally twice as high as times of N/NE flow. Similar transport dependent results were observed in October 2000 during a regional pollution event. Pollutants built-up in concentration during 22--28 October, culminated on 28 October, and then dropped 10-fold to background levels within a 6-hour period. Synoptic weather conditions during the transition from high to low pollutant levels indicated that an intense frontal boundary traversed the region, serving as a divide between a warm, humid, and polluted air mass from the W/SW, and a cold, dry, and clean air mass advancing out of Canada. Further work connecting air mass transport and aerosol variability in southern NH revealed that maximum aerosol optical depth (AOD) occurred in summer and was primarily associated with W/SW flow. Minimum AOD occurred in winter and was generally associated with N/NE flow. Mass scattering and absorption efficiencies of PM2.5 did not vary significantly between times of transport from different source regions and were very close to theoretical values. Maximum positive values of aerosol direct radiative forcing occurred in winter and maximum

  11. Aerosol transport from Chiang Mai, Thailand to Mt. Lulin, Taiwan - Implication of aerosol aging during long-range transport

    NASA Astrophysics Data System (ADS)

    Chuang, Ming-Tung; Lee, Chung-Te; Chou, Charles C.-K.; Engling, Guenter; Chang, Shih-Yu; Chang, Shuenn-Chin; Sheu, Guey-Rong; Lin, Neng-Huei; Sopajaree, Khajornsak; Chang, You-Jia; Hong, Guo-Jun

    2016-07-01

    The transport of biomass burning (BB) aerosol from Indochina may cause a potential effect on climate change in Southeast Asia, East Asia, and the Western Pacific. Up to now, the understanding of BB aerosol composition modification during long-range transport (LRT) is still very limited due to the lack of observational data. In this study, atmospheric aerosols were collected at the Suthep/Doi Ang Khang (DAK) mountain sites in Chiang Mai, Thailand and the Lulin Atmospheric Background Station (Mt. Lulin) in central Taiwan from March to April 2010 and from February to April 2013, respectively. During the study period, an upwind and downwind relationship between the Suthep/DAK and Lulin sites (2400 km apart) was validated by backward trajectories. Comprehensive aerosol properties were resolved for PM2.5 water-soluble inorganic ions, carbonaceous content, water-soluble/insoluble organic carbon (WSOC/WIOC), dicarboxylic acids and their salts (DCAS), and anhydrosugars. A Modification Factor (MF) is proposed by employing non-sea-salt potassium ion (nss-K+) or fractionalized elemental carbon evolved at 580 °C after pyrolized OC correction (EC1-OP) as a BB aerosol tracer to evaluate the mass fraction changes of aerosol components from source to receptor regions during LRT. The MF values of nss-SO42-, NH4+, NO3-, OC1 (fractionalized organic carbon evolved from room temperature to 140 °C), OP (pyrolized OC fraction), DCAS, and WSOC were above unity, which indicated that these aerosol components were enhanced during LRT as compared with those in the near-source region. In contrast, the MF values of anhydrosugars ranged from 0.1 to 0.3, indicating anhydrosugars have degraded during LRT.

  12. Predicting the Mineral and Chemical Composition of Dust Aerosols: Evaluation and Implications

    NASA Astrophysics Data System (ADS)

    Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

    2014-12-01

    Soil dust aerosols in Earth system models are typically assumed to have globally uniform properties. However, important climate processes related to dust depend on the aerosol mineral and chemical composition, which varies regionally. Such processes include aerosol radiative forcing, transport of bioavailable iron that catalyzes marine photosynthesis, heterogeneous chemistry, ice nucleation, and cloud condensation.We have implemented a new version of the soil dust aerosol scheme in the NASA GISS Earth System ModelE that takes into account the mineral composition of the dust particles. Dust aerosols are represented as an external mixture of minerals such as illite, kaolinite, smectite, carbonates, quartz, feldspar and gypsum, as well as iron oxides and accretions of iron oxides with each of the these minerals.We present a new publically available compilation of measurements of mineral fractions derived from ca. 50 references from the literature. This compilation is used to evaluate our new model of mineral and elemental composition within ModelE. We discuss the challenges of comparing simulated mineral fractions to measurements, which often come from field campaigns and ship cruises of limited duration. Despite uncertainties of the measurements, we show the importance of estimating the undisturbed size distribution of the parent soil prior to wet sieving, along with the modification of this size distribution during emission. In particular, our new model reproduces measurements showing greater amount of aerosols at silt sizes (whose diameters exceed 2 μm) including significant amounts of clay mineral aerosols (like illite) at silt sizes. Our model also reduces the systematic overestimation of quartz, while allowing iron to be transported farther from its source as impurities than in its pure, crystalline form.

  13. Aerosol chemical composition in cloud events by high resolution time-of-flight aerosol mass spectrometry.

    PubMed

    Hao, Liqing; Romakkaniemi, Sami; Kortelainen, Aki; Jaatinen, Antti; Portin, Harri; Miettinen, Pasi; Komppula, Mika; Leskinen, Ari; Virtanen, Annele; Smith, James N; Sueper, Donna; Worsnop, Douglas R; Lehtinen, Kari E J; Laaksonen, Ari

    2013-03-19

    This study presents results of direct observations of aerosol chemical composition in clouds. A high-resolution time-of-flight aerosol mass spectrometer was used to make measurements of cloud interstitial particles (INT) and mixed cloud interstitial and droplet residual particles (TOT). The differences between these two are the cloud droplet residuals (RES). Positive matrix factorization analysis of high-resolution mass spectral data sets and theoretical calculations were performed to yield distributions of chemical composition of the INT and RES particles. We observed that less oxidized hydrocarbon-like organic aerosols (HOA) were mainly distributed into the INT particles, whereas more oxidized low-volatile oxygenated OA (LVOOA) mainly in the RES particles. Nitrates existed as organic nitrate and in chemical form of NH(4)NO(3). Organic nitrates accounted for 45% of total nitrates in the INT particles, in clear contrast to 26% in the RES particles. Meanwhile, sulfates coexist in forms of acidic NH(4)HSO(4) and neutralized (NH(4))(2)SO(4). Acidic sulfate made up 64.8% of total sulfates in the INT particles, much higher than 10.7% in the RES particles. The results indicate a possible joint effect of activation ability of aerosol particles, cloud processing, and particle size effects on cloud formation.

  14. Winter time chemical characteristics of aerosols over the Bay of Bengal: continental influence.

    PubMed

    Aryasree, S; Nair, Prabha R; Girach, I A; Jacob, Salu

    2015-10-01

    As part of the Integrated Campaign for Aerosols, gases and Radiation Budget (ICARB) conducted under the Geosphere Biosphere Programme of Indian Space Research Organisation, ship-based aerosol sampling was carried out over the marine environment of Bay of Bengal (BoB) during the northern winter months of December 2008 to January 2009. About 101 aerosol samples were collected, covering the region from 3.4° to 21° N latitude and 76° to 98° E longitude-the largest area covered-including the south east (SE) BoB for the first time. These samples were subjected to gravimetric and chemical analysis and the total aerosol loading as well the mass concentration of the ionic species namely F(-), Cl(-), Br(-), NO2 (-), NO3 (-), PO4 (2-), SO4 (2-), NH4 (+), etc. and the metallic species, Na, Mg, Ca, K, Al, Fe, Mn, Zn, and Pb were estimated for each sample. Based on the spatial distribution of individual chemical species, the air flow pattern, and airmass back trajectory analysis, the source characteristics of aerosols for different regions of BoB were identified. Significant level of continental pollution was noticed over BoB during winter. While transport of pollution from Indo-Gangetic Plain (IGP) contributed to aerosols over north BoB, those over SE BoB were influenced by SE Asia. A quantitative study on the wind-induced production of sea salt aerosols and a case study on the species dependent effect of rainfall are also presented in this paper. PMID:25994269

  15. Optical, physical, and chemical properties of springtime aerosol over Barrow Alaska in 2008

    SciTech Connect

    Shantz, Nicole C.; Gultepe, Ismail; Andrews, Elisabeth; Earle, Michael; MacDonald, A. M.; Liu, Peter S.K.; Leaitch, W. R.

    2014-03-06

    Airborne observations from four flights during the 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) are used to examine some cloud-free optical, physical, and chemical properties of aerosol particles in the springtime Arctic troposphere. The number concentrations of particles larger than 0.12 μm (Na>120), important for light extinction and cloud droplet formation, ranged from 15 to 2260 cm-3, with the higher Na>120 cases dominated by measurements from two flights of long-range transported biomass burning (BB) aerosols. The two other flights examined here document a relatively clean aerosol and an Arctic Haze aerosol impacted by larger particles largely composed of dust. For observations from the cleaner case and the BB cases, the particle light scattering coefficients at low relative humidity (RH<20%) increased nonlinearly with increasing Na>120, driven mostly by an increase in mean sizes of particles with increasing Na>120 (BB cases). For those three cases, particle light absorption coefficients also increased nonlinearly with increasing Na>120 and linearly with increasing submicron particle volume concentration. In addition to black carbon, brown carbon was estimated to have increased light absorption coefficients by 27% (450 nm wavelength) and 14% (550 nm) in the BB cases. For the case with strong dust influence, the absorption relative to submicron particle volume was small compared with the other cases. There was a slight gradient of Passive Cavity Aerosol Spectrometer Probe (PCASP) mean volume diameter (MVD) towards smaller sizes with increasing height, which suggests more scavenging of the more elevated particles, consistent with a typically longer lifetime of particles higher in the atmosphere. However, in approximately 10% of the cases, the MVD increased (>0.4 μm) with increasing altitude, suggesting transport of larger fine particle mass (possibly coarse particle mass) at high levels over the Arctic. This may be because of transport of

  16. Sarychev Volcanic Aerosol and Chemical measurements over Eureka, Canada

    NASA Astrophysics Data System (ADS)

    Perro, C. W.; Duck, T. J.; Bitar, L.; Nott, G. J.; Lesins, G. B.; O'Neill, N. T.; Eloranta, E.; Strong, K.; Carn, S. A.; Lindenmaier, R.; Batchelor, R.; Saha, A.; Pike-Thackray, C.; Drummond, J. R.

    2010-12-01

    On July 01, 2009, lidar measurements from Eureka, Canada (80°N, 85°W) detected unusually high amounts of aerosol in the lower stratosphere which are believed to have originated from the Sarychev Eruption on the Kuril Islands in Russia (48°N,153°E). The suite of instruments that are part of the Canadian Network for the Detection of Atmospheric Change (CANDAC) have been used to measure the optical and chemical properties of the volcanic plume over Eureka. Lidar measurements show significant structure in the stratospheric aerosol that reaches altitudes of approximately 17 km. Initially there were several layers of aerosol in the lower stratosphere, which began to mix vertically so that by the end of August the aerosol was mixed into one homogeneous layer in the lower stratosphere. Lidar and sun photometer measurements are used to track the change in the integrated volume backscatter cross section from July 2009, with an initial peak value of 0.007 sr-1 until March 2010 when values have returned to background levels. Lidar measurements also show the plume descending over time. Satellite data from OMI and CALIPSO are used to track the SO2 and aerosols in the plume as it travels from the Kuril Islands to Eureka. Ground based measurements from a UV-VIS Spectrophotometer detected SO2 that correlated with OMI measurements over Eureka on July 01. A fourier transform spectrometer was used to monitor a number of chemical species in the UTLS region with HCL for example spiking during the same period. Effects of the stratospheric aerosols on the incoming short wave radiation during the summer months are also examined.

  17. Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

    NASA Astrophysics Data System (ADS)

    Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilde, S.; Zhang, Y.; Dall'Osto, M.

    2014-04-01

    The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterized by a less dense urbanization. We present here the results obtained in San Pietro Capofiume, which is located in a sparsely inhabited sector of the Po Valley, Italy. The experiment was carried out in summer 2009 in the framework of the EUCAARI project ("European Integrated Project on Aerosol, Cloud Climate Aerosol Interaction"). For the first time in Europe, six state-of-the-art techniques were used in parallel: (1) on-line TSI aerosol time-of-flight mass spectrometer (ATOFMS), (2) on-line Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), (3) soot particle aerosol mass spectrometer (SP-AMS), (4) on-line high resolution time-of-flight mass spectrometer-thermal desorption aerosol gas chromatograph (HR-ToFMS-TAG), (5) off-line twelve-hour resolution proton nuclear magnetic resonance (H-NMR) spectroscopy, and (6) chemical ionization mass spectrometry (CIMS) for the analysis of gas-phase precursors of secondary aerosol. Data from each aerosol spectroscopic method were analysed individually following ad-hoc tools (i.e. PMF for AMS, Art-2a for ATOFMS). The results obtained from each techniques are herein presented and compared. This allows us to clearly link the modifications in aerosol chemical composition to transitions in air mass origin and meteorological regimes. Under stagnant conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC

  18. Code System to Calculate Particle Penetration Through Aerosol Transport Lines.

    1999-07-14

    Version 00 Distribution is restricted to US Government Agencies and Their Contractors Only. DEPOSITION1.03 is an interactive software program which was developed for the design and analysis of aerosol transport lines. Models are presented for calculating aerosol particle penetration through straight tubes of arbitrary orientation, inlets, and elbows. An expression to calculate effective depositional velocities of particles on tube walls is derived. The concept of maximum penetration is introduced, which is the maximum possible penetrationmore » through a sampling line connecting any two points in a three-dimensional space. A procedure to predict optimum tube diameter for an existing transport line is developed. Note that there is a discrepancy in this package which includes the DEPOSITION 1.03 executable and the DEPOSITION 2.0 report. RSICC was unable to obtain other executables or reports.« less

  19. Uranium Oxide Aerosol Transport in Porous Graphite

    SciTech Connect

    Blanchard, Jeremy; Gerlach, David C.; Scheele, Randall D.; Stewart, Mark L.; Reid, Bruce D.; Gauglitz, Phillip A.; Bagaasen, Larry M.; Brown, Charles C.; Iovin, Cristian; Delegard, Calvin H.; Zelenyuk, Alla; Buck, Edgar C.; Riley, Brian J.; Burns, Carolyn A.

    2012-01-23

    The objective of this paper is to investigate the transport of uranium oxide particles that may be present in carbon dioxide (CO2) gas coolant, into the graphite blocks of gas-cooled, graphite moderated reactors. The transport of uranium oxide in the coolant system, and subsequent deposition of this material in the graphite, of such reactors is of interest because it has the potential to influence the application of the Graphite Isotope Ratio Method (GIRM). The GIRM is a technology that has been developed to validate the declared operation of graphite moderated reactors. GIRM exploits isotopic ratio changes that occur in the impurity elements present in the graphite to infer cumulative exposure and hence the reactor’s lifetime cumulative plutonium production. Reference Gesh, et. al., for a more complete discussion on the GIRM technology.

  20. Molecular corridors represent the multiphase chemical evolution of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Shiraiwa, M.; Berkemeier, T.; Schilling-Fahnestock, K. A.; Seinfeld, J. H.; Pöschl, U.

    2014-03-01

    The dominant component of atmospheric organic aerosol is that derived from the oxidation of volatile organic compounds (VOCs), so-called secondary organic aerosol (SOA). SOA consists of a multitude of organic compounds, only a small fraction of which has historically been identified. Formation and evolution of SOA is a complex process involving coupled chemical reaction and mass transport in the gas and particle phases. Current SOA models do not embody the full spectrum of reaction and transport processes nor do they identify the dominant rate-limiting steps in SOA formation. The recent advent of soft ionization mass spectrometry methods now facilitates a more complete molecular identification of SOA than heretofore possible. Based on such novel measurements, we show here that the chemical evolution of SOA from a variety of VOC precursors adheres to characteristic "molecular corridors" with a tight inverse correlation between volatility and molar mass. Sequential and parallel reaction oxidation and dimerization pathways progress along these corridors through characteristic regimes of reaction-, diffusion-, or accommodation-limited multiphase chemical kinetics that can be classified according to reaction location, degree of saturation, and extent of heterogeneity of gas and particle phases. These molecular corridors constrain the properties of unidentified products and reaction pathways and rates of SOA evolution, thereby facilitating the further development of aerosol models for air quality and climate.

  1. The Saharan Aerosol Long-range Transport and Aerosol-Cloud Interaction Experiment (SALTRACE 2013) - An overview

    NASA Astrophysics Data System (ADS)

    Weinzierl, Bernadett; Ansmann, Albert; Reitebuch, Oliver; Freudenthaler, Volker; Müller, Thomas; Kandler, Konrad; Althausen, Dietrich; Chouza, Fernando; Dollner, Maximilian; Farrell, David; Groß, Silke; Heinold, Bernd; Kristensen, Thomas B.; Mayol-Bracero, Olga L.; Omar, Ali; Prospero, Joseph; Sauer, Daniel; Schäfler, Andreas; Toledano, Carlos; Tegen, Ina

    2015-04-01

    Saharan mineral dust is regularly transported over long distances impacting air quality, health, weather and climate thousands of kilometers downwind of the Sahara. During transport, the properties of mineral dust may be modified thereby changing the associated impact on the radiation budget. Although mineral dust is of key importance for the climate system many questions such as the change of the dust size distribution during long-range transport, the role of wet and dry removal mechanisms, and the complex interaction between mineral dust and clouds remain open. To investigate the aging and modification of Saharan mineral dust during long-range transport across the Atlantic Ocean, the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE: http://www.pa.op.dlr.de/saltrace) was conducted in June/July 2013. SALTRACE was designed as a closure experiment combining ground-based lidar, in-situ and sun photometer instruments deployed on Cape Verde, Barbados and Puerto Rico, with airborne measurements of the DLR research aircraft Falcon, satellite observations and model simulations. During SALTRACE, mineral dust from five dust outbreaks was studied under different atmospheric conditions and a unique data set on the chemical, microphysical and optical properties of aged mineral dust was gathered. For the first time, Lagrangian sampling of a dust plume in the Cape Verde area on 17 June 2013 which was again measured with the same instrumentation on 21 and 22 June 2013 near Barbados was realized. Further highlights of SALTRACE include the formation and evolution of tropical storm Chantal in a dusty environment and the interaction of dust with mixed-phase clouds. In our presentation, we give an overview of the SALTRACE study, discuss the meteorological situation and the dust transport during SALTRACE and highlight selected results from SALTRACE.

  2. Commuter exposure to aerosol pollution on public transport in Singapore

    NASA Astrophysics Data System (ADS)

    Tan, S.; Velasco, E.; Roth, M.; Norford, L.

    2013-12-01

    Personal exposure to aerosol pollutants in the transport microenvironment of Singapore has not been well documented. Studies from many cities suggest that brief periods of exposure to high concentrations of airborne pollutants may have significant health impacts. Thus, a large proportion of aerosol exposure may be experienced during daily commuting trips due to the proximity to traffic. A better understanding of the variability across transport modes is therefore needed to design transport policies that minimize commuters' exposure. In light of this, personal exposure measurements of PM10 and PM2.5, particle number (PN), black carbon (BC), carbon monoxide (CO), particle-bound polycyclic aromatic hydrocarbons (pPAH), and active surface area (SA) were conducted on a selected route in downtown Singapore. Portable and real-time monitoring instruments were carried onto three different modes of public transport (bus, taxi, subway) and by foot. Simultaneous measurements were taken at a nearby park to capture the background concentrations. Large variability was observed amongst the various transport modes investigated. For example, the particle number concentration was on average 1.5, 1.6, 0.8, and 2.2 times higher inside buses, taxis, subway and by foot, respectively, than at the background site. Based on the results, it is possible to come up with a ranking of the 'cleanest' transport mode for Singapore.

  3. Quantification of aerosol chemical composition using continuous single particle measurements

    NASA Astrophysics Data System (ADS)

    Jeong, C.-H.; McGuire, M. L.; Godri, K. J.; Slowik, J. G.; Rehbein, P. J. G.; Evans, G. J.

    2011-01-01

    Mass concentrations of particulate matter (PM) chemical components were determined from data for 0.3 to 3.0 μm particles measured by an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) data at an urban and rural site. Hourly-averaged concentrations of nitrate, sulphate, ammonium, organic carbon, and elemental carbon, estimated based on scaled ATOFMS peak intensities of corresponding ion marker species, were compared with collocated chemical composition measurements by an Aerosol Mass Spectrometer (AMS), a Gas-Particle Ion Chromatograph (GPIC), and a Sunset Lab field OCEC analyzer. The highest correlation was found for nitrate, with correlation coefficients (Pearson r) of 0.89 and 0.85 at the urban and rural sites, respectively. ATOFMS mass calibration factors, determined for the urban site, were used to calculate mass concentrations of the major PM chemical components at the rural site. Mass reconstruction using this ATOFMS based composition data agreed very well with the total PM mass measured at the rural site. Size distributions of the ten main types of particles were resolved for the rural site and the mass composition of each particle type was determined in terms of sulphate, nitrate, ammonium, organic carbon and elemental carbon. This is the first study to estimate hourly mass concentrations of individual aerosol components and the mass composition of individual particle-types based on ATOFMS single particle measurements.

  4. Chemical and physicochemial properties of submicron aerosol agglomerates

    SciTech Connect

    Scripsick, R.C.; Ehrman, S.; Friedlander, S.K.

    1998-12-31

    This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory. The formation of nanometer-sized aerosol particles in a premixed methane flame from both solid-phase aerosol precursors and gas-phase precursors was investigated. Techniques were developed to determine the distribution of the individual chemical species as a function of agglomerate size by using inductively coupled plasma atomic emission spectroscopy (ICP-AES). To determine the distribution of chemical species both from particle to particle and within the particles on a nanometer scale, we used the analytical electron microscopy techniques of energy dispersive x-ray spectrometry (EDS) and electron energy loss spectrometry (EELS) coupled with transmission electron microscopy (TEM). The observed distribution of individual chemical species as a function of agglomerate size was linked to the material properties of the solid-phase precursors. For aerosol formed from gas-phase precursors by gas-to-particle conversion, the distribution of species on a manometer scale was found to correspond to the equilibrium phase distribution expected from equilibrium for the system at the flame temperatures.

  5. Chemical evolution of multicomponent aerosol particles during evaporation

    NASA Astrophysics Data System (ADS)

    Zardini, Alessandro; Riipinen, Ilona; Pagels, Joakim; Eriksson, Axel; Worsnop, Douglas; Switieckli, Erik; Kulmala, Markku; Bilde, Merete

    2010-05-01

    Atmospheric aerosol particles have an important but not well quantified effect on climate and human health. Despite the efforts made in the last decades, the formation and evolution of aerosol particles in the atmosphere is still not fully understood. The uncertainty is partly due to the complex chemical composition of the particles which comprise inorganic and organic compounds. Many organics (like dicarboxylic acids) can be present both in the gas and in the condensed phase due to their low vapor pressure. Clearly, an understanding of this partition is crucial to address any other issue in atmospheric physics and chemistry. Moreover, many organics are water soluble, and their influence on the properties of aqueous solution droplets is still poorly characterized. The solid and sub-cooled liquid state vapor pressures of some organic compounds have been previously determined by measuring the evaporation rate of single-compound crystals [1-3] or binary aqueous droplets [4-6]. In this work, we deploy the HTDMA technique (Hygroscopicity Tandem Differential Mobility Analyzer) coupled with a 3.5m laminar flow-tube and an Aerosol Mass Spectrometer (AMS) for determining the chemical evolution during evaporation of ternary droplets made of one dicarboxylic acid (succinic acid, commonly found in atmospheric samples) and one inorganic compound (sodium chloride or ammonium sulfate) in different mixing ratios, in equilibrium with water vapor at a fixed relative humidity. In addition, we investigate the evaporation of multicomponent droplets and crystals made of three organic species (dicarboxylic acids and sugars), of which one or two are semi-volatile. 1. Bilde M. and Pandis, S.N.: Evaporation Rates and Vapor Pressures of Individual Aerosol Species Formed in the Atmospheric Oxidation of alpha- and beta-Pinene. Environmental Science and Technology, 35, 2001. 2. Bilde M., et al.: Even-Odd Alternation of Evaporation Rates and Vapor Pressures of C3-C9 Dicarboxylic Acid Aerosols

  6. Size distribution and optical properties of mineral dust aerosols transported in the western Mediterranean

    NASA Astrophysics Data System (ADS)

    Denjean, C.; Cassola, F.; Mazzino, A.; Triquet, S.; Chevaillier, S.; Grand, N.; Bourrianne, T.; Momboisse, G.; Sellegri, K.; Schwarzenbock, A.; Freney, E.; Mallet, M.; Formenti, P.

    2016-02-01

    This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June-July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1-5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals

  7. Aerosol sampling and Transport Efficiency Calculation (ASTEC) and application to surtsey/DCH aerosol sampling system: Code version 1. 0: Code description and user's manual

    SciTech Connect

    Yamano, N.; Brockmann, J.E.

    1989-05-01

    This report describes the features and use of the Aerosol Sampling and Transport Efficiency Calculation (ASTEC) Code. The ASTEC code has been developed to assess aerosol transport efficiency source term experiments at Sandia National Laboratories. This code also has broad application for aerosol sampling and transport efficiency calculations in general as well as for aerosol transport considerations in nuclear reactor safety issues. 32 refs., 31 figs., 7 tabs.

  8. Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

    NASA Astrophysics Data System (ADS)

    Deguillaume, L.; Leriche, M.; Amato, P.; Ariya, P. A.; Delort, A.-M.; Pöschl, U.; Chaumerliac, N.; Bauer, H.; Flossmann, A. I.; Morris, C. E.

    2008-07-01

    This paper discusses the influence of primary biological aerosols (PBA) on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that PBA represent a significant fraction of air particulate matter and hence affect the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms, namely fungal spores and bacteria, can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of PBA in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere.

  9. Optical and Chemical Characterization of Aerosols Produced from Cooked Meats

    NASA Astrophysics Data System (ADS)

    Niedziela, R. F.; Foreman, E.; Blanc, L. E.

    2011-12-01

    Cooking processes can release a variety compounds into the air immediately above a cooking surface. The distribution of compounds will largely depend on the type of food that is being processed and the temperatures at which the food is prepared. High temperatures release compounds from foods like meats and carry them away from the preparation surface into cooler regions where condensation into particles can occur. Aerosols formed in this manner can impact air quality, particularly in urban areas where the amount of food preparation is high. Reported here are the results of laboratory experiments designed to optically and chemically characterize aerosols derived from cooking several types of meats including ground beef, salmon, chicken, and pork both in an inert atmosphere and in synthetic air. The laboratory-generated aerosols are studied using a laminar flow cell that is configured to accommodate simultaneous optical characterization in the mid-infrared and collection of particles for subsequent chemical analysis by gas chromatography. Preliminary optical results in the visible and ultra-violet will also be presented.

  10. Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: an AQMEII-2 perspective

    EPA Science Inventory

    The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model in...

  11. Complete chemical analysis of aerosol particles in real-time

    SciTech Connect

    Yang, Mo; Reilly, P.T.A.; Gieray, R.A.; Whitten, W.B.; Ramsey, J.M.

    1996-12-31

    Real-time mass spectrometry of individual aerosol particles using an ion trap mass spectrometer is described. The microparticles are sampled directly from the air by a particle inlet system into the vacuum chamber. An incoming particle is detected as it passes through two CW laser beams and a pulsed laser is triggered to intercept the particle for laser ablation ionization at the center of the ion trap. The produced ions are analyzed by the ion trap mass spectrometer. Ions of interest are selected and dissociated through collision with buffer gas atoms for further fragmentation analysis. Real-time chemical analyses of inorganic, organic, and bacterial aerosol articles have been demonstrated. It has been confirmed that the velocity and the size of the incoming particles highly correlate to each other. The performance of the inlet system, particle detection, and preliminary results are discussed.

  12. Properties of transported African mineral dust aerosols in the Mediterranean region

    NASA Astrophysics Data System (ADS)

    Denjean, Cyrielle; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Triquet, Sylvain; Zapf, Pascal; Loisil, Rodrigue; Bourrianne, Thierry; Freney, Evelyn; Dupuy, Regis; Sellegri, Karine; Schwarzenbock, Alfons; Torres, Benjamin; Mallet, Marc; Cassola, Federico; Prati, Paolo; Formenti, Paola

    2015-04-01

    The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), one intensive airborne campaign (ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) has been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to the dust origin and transport. Case studies of dust transport

  13. Computational modeling and experimental characterization of indoor aerosol transport

    SciTech Connect

    Konecni, S.; Whicker, J. J.; Martin, R. A.

    2002-01-01

    When a hazardous aerosol or gas is inadvertently or deliberately released in an occupied facility, the airborne material presents a hazard to people. Inadvertent accidents and exposures continue to occur in Los Alamos and other nuclear facilities despite state-of-art engineering and administrative controls, and heightened diligence. Despite the obvious need in occupational settings and for homeland defense, the body of research in hazardous aerosol dispersion and control in large, complex, ventilated enclosures is extremely limited. The science governing generation, transport, inhalation, and detection of airborne hazards is lacking and must be developed to where it can be used by engineers or safety professionals in the prediction of worker exposure, in the prevention of accidents, or in the mitigation of terrorist actions. In this study, a commercial computational fluid dynamics (CFD) code, CFX5.4, and experiments were used to assess flow field characteristics, and to investigate aerosol release and transport in a large, ventilated workroom in a facility at Savannah River Site. Steady state CFD results illustrating a complex, ventilation-induced, flow field with vortices, velocity gradients, and quiet zones are presented, as are time-dependent CFD and experimental aerosol dispersion results. The comparison of response times between CFD and experimental results was favorable. It is believed that future applications of CFD and experiments can have a favorable impact on the design of ventilation (HVAC) systems and worker safety with consideration to facility costs. Ultimately, statistical methods will be used in conjunction with CFD calculations to determine the optimal number and location of detectors, as well as optimal egress routes in event of a release.

  14. Effects of Chemical Aging on Global Secondary Organic Aerosol using the Volatility Basis Set Approach

    NASA Astrophysics Data System (ADS)

    Park, R.; Jo, D.; Kim, M.; Spracklen, D. V.; Hodzic, A.

    2014-12-01

    Organic aerosol (OA) constitutes significant mass fractions (20-90%) of total dry fine aerosols in the atmosphere. However, global models of OA have shown large discrepancies when compared to the observations because of the limited capability to simulate secondary OA (SOA). For reducing the discrepancies between observations and models, recent studies have shown that chemical aging reactions in the atmosphere are important because they can lead to decreases in organic volatility, resulting in increase of SOA mass yields. To efficiently simulate chemical aging of SOA in the atmosphere, we implemented the volatility basis set approach in a global 3-D chemical transport model (GEOS-Chem). We present full-year simulations and their comparisons with multiple observations - global aerosol mass spectrometer dataset, the Interagency Monitoring of Protected Visual Environments from the United States, the European Monitoring and Evaluation Programme dataset and water-soluble organic carbon observation data collected over East Asia. Using different input parameters in the model, we also explore the uncertainty of the SOA simulation for which we use an observational constraint to find the optimized values with which the model reduces the discrepancy from the observations. Finally, we estimate the effect of OA on climate using our best simulation results.

  15. Chemical Equilibrium And Transport (CET)

    NASA Technical Reports Server (NTRS)

    Mcbride, B. J.

    1991-01-01

    Powerful, machine-independent program calculates theoretical thermodynamic properties of chemical systems. Aids in design of compressors, turbines, engines, heat exchangers, and chemical processing equipment.

  16. Comparison of Aerosol Mass Spectrometer and Aerosol Chemical Speciation Monitor Measurements of Secondary Organic Aerosol Formation in Smog Chamber Studies

    NASA Astrophysics Data System (ADS)

    Croteau, P. L.; Hunter, J. F.; Daumit, K. E.; Carrasquillo, A. J.; Cross, E. S.; Canagaratna, M.; Jayne, J.; Worsnop, D. R.; Kroll, J. H.

    2012-12-01

    Thermal vaporization-electron impact ionization (TV-EI) mass spectrometry is a powerful tool for understanding the chemistry of secondary organic aerosol (SOA) formation and atmospheric aging. The Aerodyne Aerosol Mass Spectrometer (AMS) and recently developed Aerosol Chemical Speciation Monitor (ACSM) are two instruments that utilize the same TV-EI technique. The ACSM trades the particle sizing capability, sensitivity, speed, and resolution of the AMS for simplicity, affordability, and ease of operation - enabling stand-alone continuous sampling for extended periods of time. Here we present results of an intercomparison between a high-resolution AMS and an ACSM. Three well-studied SOA formation chamber experiments were conducted: isoprene photooxidation under high NOx conditions, m-xylene photooxidation under high NOx conditions, and α-pinene ozonolysis under low NOx conditions. Comparisons between time-series and mass spectra from these experiments, along with positive matrix factorization analysis results demonstrate that the ACSM, while it does not provide the same level of detail as an AMS, is a suitable tool for exploring the chemistry of SOA formation in chamber studies.

  17. Chemical Pollution from Transportation Vehicles

    PubMed Central

    Starkman, Ernest S.

    1969-01-01

    Recent publicity on electrically powered vehicles notwithstanding, the gasoline engine will probably be the principal power plant for passenger cars for at least the next decade. Chemical pollutants discharged by the gasoline engine are now under partial control. Motor cars of 1968 and 1969 model discharge only about 30 percent as much carbon monoxide and unburned hydrocarbons as do older models. In theory, carbon monoxide, unburned hydrocarbons and oxides of nitrogen ultimately can be completely removed from gasoline engine exhaust. In order to accomplish this it would be necessary to modify cars to operate satisfactorily on a lean mixture and perhaps to use a catalyst in the exhaust system. Present designs of gas turbines for aircraft and for future projected application to ground vehicles yield pollutants (except for smoke) at levels below those of gasoline engines for a decade to come. It has also been shown possible to eliminate smoke as well as odor from the gas turbine. Thus with proper effort it is feasible to reduce pollution of the atmosphere due to transportation to an acceptable level, even if electrically or alternatively powered vehicles cannot be developed for a decade. PMID:4183827

  18. Aerosol Optical Properties and Chemical Composition Measured on the Ronald H. Brown During ACE-Asia

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Miller, T. L.; Coffman, D.

    2001-12-01

    Measurements of aerosol chemical, physical, and optical properties were made onboard the NOAA R/V Ronald H. Brown during the ACE-Asia Intensive Field Program to characterize Asian aerosol as it was transported across the Pacific Ocean. The ship traveled across the Pacific from Hawaii to Japan and into the East China Sea and the Sea of Japan. Trajectories indicate that remote marine air masses were sampled on the transit to Japan. In the ACE-Asia study region air masses from Japan, China, Mongolia, and the Korea Peninsula were sampled. A variety of aerosol types were encountered including those of marine, volcanic, crustal, and industrial origin. Presented here, for the different air masses encountered, are aerosol optical properties (scattering and absorption coefficients, single scattering albedo, Angstrom Exponent, and aerosol optical depth) and chemical composition (major ions, total organic and black carbon, and trace elements). Scattering by submicron aerosol (55 % RH and 550 nm) was less than 20 1/Mm during the transit from Hawaii to Japan. In continental air masses, values ranged from 60 to 320 1/Mm with the highest submicron scattering coefficients occurring during prefrontal conditions with a low marine boundary layer height and trajectories from Japan. For the continental air masses, the ratio of scattering by submicron to sub-10 micron aerosol during polluted conditions averaged 0.8 and during a dust event 0.41. Aerosol optical depth (500 nm) ranged from 0.08 during the Pacific transit to 1.3 in the prefrontal conditions described above. Optical depths during dust events ranged from 0.2 to 0.6. Submicron non-sea salt (nss) sulfate concentrations ranged from 0.5 ug/m-3 during the Pacific transit to near 30 ug/m-3 during the prefrontal conditions described above. Black carbon to total carbon mass ratios in air masses from Asia averaged 0.18 with highest values (0.32) corresponding to trajectories crossing the Yangtze River valley.

  19. Satellite perspective of aerosol intercontinental transport: From qualitative tracking to quantitative characterization

    NASA Astrophysics Data System (ADS)

    Yu, Hongbin; Remer, Lorraine A.; Kahn, Ralph A.; Chin, Mian; Zhang, Yan

    2013-04-01

    Evidence of aerosol intercontinental transport (ICT) is both widespread and compelling. Model simulations suggest that ICT could significantly affect regional air quality and climate, but the broad inter-model spread of results underscores a need of constraining model simulations with measurements. Satellites have inherent advantages over in situ measurements to characterize aerosol ICT, because of their spatial and temporal coverage. Significant progress in satellite remote sensing of aerosol properties during the Earth Observing System (EOS) era offers the opportunity to increase quantitative characterization and estimates of aerosol ICT beyond the capability of pre-EOS era satellites that could only qualitatively track aerosol plumes. EOS satellites also observe emission strengths and injection heights of some aerosols, aerosol precursors, and aerosol-related gases, which can help characterize aerosol ICT. We review how the current generation of satellite measurements have been used to (1) characterize the evolution of aerosol plumes (e.g., both horizontal and vertical transport, and properties) on an episodic basis, (2) understand the seasonal and inter-annual variations of aerosol ICT and their control factors, (3) estimate the export and import fluxes of aerosols, and (4) evaluate and constrain model simulations. Substantial effort is needed to further explore an integrated approach using measurements from on-orbit satellites (e.g., A-Train synergy) for observational characterization and model constraint of aerosol intercontinental transport and to develop advanced sensors for future missions.

  20. Satellite Perspective of Aerosol Intercontinental Transport: From Qualitative Tracking to Quantitative Characterization

    NASA Technical Reports Server (NTRS)

    Yu, Hongbin; Remer, Lorraine A.; Kahn, Ralph A.; Chin, Mian; Zhang, Yan

    2012-01-01

    Evidence of aerosol intercontinental transport (ICT) is both widespread and compelling. Model simulations suggest that ICT could significantly affect regional air quality and climate, but the broad inter-model spread of results underscores a need of constraining model simulations with measurements. Satellites have inherent advantages over in situ measurements to characterize aerosol ICT, because of their spatial and temporal coverage. Significant progress in satellite remote sensing of aerosol properties during the Earth Observing System (EOS) era offers opportunity to increase quantitative characterization and estimates of aerosol ICT, beyond the capability of pre-EOS era satellites that could only qualitatively track aerosol plumes. EOS satellites also observe emission strengths and injection heights of some aerosols, aerosol precursors, and aerosol-related gases, which can help characterize aerosol ICT. After an overview of these advances, we review how the current generation of satellite measurements have been used to (1) characterize the evolution of aerosol plumes (e.g., both horizontal and vertical transport, and properties) on an episodic basis, (2) understand the seasonal and inter-annual variations of aerosol ICT and their control factors, (3) estimate the export and import fluxes of aerosols, and (4) evaluate and constrain model simulations. Substantial effort is needed to further explore an integrated approach using measurements from on-orbit satellites (e.g., A-Train synergy) for observational characterization and model constraint of aerosol intercontinental transport and to develop advanced sensors for future missions.

  1. Size distribution and optical properties of mineral dust aerosols transported in the western Mediterranean

    NASA Astrophysics Data System (ADS)

    Denjean, C.; Cassola, F.; Mazzino, A.; Triquet, S.; Chevaillier, S.; Grand, N.; Bourrianne, T.; Momboisse, G.; Sellegri, K.; Schwarzenbock, A.; Freney, E.; Mallet, M.; Formenti, P.

    2015-08-01

    This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June-July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of tranport (1-5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried higher concentration of pollution particles at intermediate altitude (1-3 km) than at elevated altitude (> 3 km), resulting in scattering Angstrom exponent up to 2.2 within the intermediate altitude. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate light absorption of the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00 ± 0.04. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assimilated to those of native dust in radiative transfer simulations, modeling studies and

  2. Chemical and physical properties of bulk aerosols within four sectors observed during TRACE-P

    NASA Astrophysics Data System (ADS)

    Jordan, C. E.; Anderson, B. E.; Talbot, R. W.; Dibb, J. E.; Fuelberg, H. E.; Hudgins, C. H.; Kiley, C. M.; Russo, R.; Scheuer, E.; Seid, G.; Thornhill, K. L.; Winstead, E.

    2003-11-01

    Chemical and physical aerosol data collected on the DC-8 during TRACE-P were grouped into four sectors based on back trajectories. The four sectors represent long-range transport from the west (WSW), regional circulation over the western Pacific and Southeast Asia (SE Asia), polluted transport from northern Asia with substantial sea salt at low altitudes (NNW) and a substantial amount of dust (Channel). WSW has generally low mixing ratios at both middle and high altitudes, with the bulk of the aerosol mass due to non-sea-salt water-soluble inorganic species. Low altitude SE Asia also has low mean mixing ratios in general, with the majority of the aerosol mass comprised of non-sea-salts, however, soot is also relatively important in this region. NNW had the highest mean sea salt mixing ratios, with the aerosol mass at low altitudes (<2 km) evenly divided between sea salts, non-sea-salts, and dust. The highest mean mixing ratios of water-soluble ions and soot were observed at the lowest altitudes (<2 km) in the Channel sector. The bulk of the aerosol mass exported from Asia emanates from Channel at both low and midaltitudes, due to the prevalence of dust compared to other sectors. Number densities show enhanced fine particles for Channel and NNW, while their volume distributions are enhanced due to sea salt and dust. Low-altitude Channel exhibits the highest condensation nuclei (CN) number densities along with enhanced scattering coefficients, compared to the other sectors. At midaltitudes (2-7 km), low mean CN number densities coupled with a high proportion of nonvolatile particles (≥65%) observed in polluted sectors (Channel and NNW) are attributed to wet scavenging which removes hygroscopic CN particles. Low single scatter albedo in SE Asia reflects enhanced soot.

  3. Aerosol chemical vapor deposition of metal oxide films

    DOEpatents

    Ott, Kevin C.; Kodas, Toivo T.

    1994-01-01

    A process of preparing a film of a multicomponent metal oxide including: forming an aerosol from a solution comprised of a suitable solvent and at least two precursor compounds capable of volatilizing at temperatures lower than the decomposition temperature of said precursor compounds; passing said aerosol in combination with a suitable oxygen-containing carrier gas into a heated zone, said heated zone having a temperature sufficient to evaporate the solvent and volatilize said precursor compounds; and passing said volatilized precursor compounds against the surface of a substrate, said substrate having a sufficient temperature to decompose said volatilized precursor compounds whereby metal atoms contained within said volatilized precursor compounds are deposited as a metal oxide film upon the substrate is disclosed. In addition, a coated article comprising a multicomponent metal oxide film conforming to the surface of a substrate selected from the group consisting of silicon, magnesium oxide, yttrium-stabilized zirconium oxide, sapphire, or lanthanum gallate, said multicomponent metal oxide film characterized as having a substantially uniform thickness upon said FIELD OF THE INVENTION The present invention relates to the field of film coating deposition techniques, and more particularly to the deposition of multicomponent metal oxide films by aerosol chemical vapor deposition. This invention is the result of a contract with the Department of Energy (Contract No. W-7405-ENG-36).

  4. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Dubovik, Oleg; Holben, Brent; Kaufman, Yoram; chu, Allen; Anderson, Tad; Quinn, Patricia

    2003-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  5. Aerosol Sources, Absorption, and Intercontinental Transport: Synergies Among Models, Remote Sensing, and Atmospheric Measurements

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Chu, Allen; Levy, Robert; Remer, Lorraine; Kaufman, Yoram; Dubovik, Oleg; Holben, Brent; Eck, Tom; Anderson, Tad; Quinn, Patricia

    2004-01-01

    Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, .biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERON" at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

  6. 76 FR 34240 - Chemical Transportation Advisory Committee

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-06-13

    ... public dockets in the January 17, 2008, issue of the Federal Register (73 FR 3316). Establishment of the... SECURITY Coast Guard Chemical Transportation Advisory Committee AGENCY: Coast Guard, DHS. ACTION: Committee... that the establishment of the Chemical Transportation Advisory Committee (CTAC) is necessary and in...

  7. 78 FR 55278 - Chemical Transportation Advisory Committee

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-09-10

    ... Federal Register (73 FR 3316). Re-Establishment of the Committee For the reasons set forth below, the... SECURITY Coast Guard Chemical Transportation Advisory Committee AGENCY: Coast Guard, DHS. ACTION: Committee... that the re- establishment of the Chemical Transportation Advisory Committee (CTAC) is necessary and...

  8. Smoke aerosol transport patterns over the Maritime Continent

    NASA Astrophysics Data System (ADS)

    Xian, Peng; Reid, Jeffrey S.; Atwood, Samuel A.; Johnson, Randall S.; Hyer, Edward J.; Westphal, Douglas L.; Sessions, Walter

    2013-03-01

    Smoke transport patterns over the Maritime Continent (MC) are studied through a combination of approaches, including a) analyzing AODs obtained from satellite products; b) aerosol transport modeling with AOD assimilation along with the atmospheric flow patterns; c) analyzing smoke wet deposition distributions; and d) examining forward trajectories for smoke events defined in this study. It is shown that smoke transport pathways are closely related to the low-level atmospheric flow, i.e., during June-Sept, smoke originating from the MC islands with a dominant source over central and southern Sumatra, and southern and western Borneo, is generally transported northwestward south of the equator and northeastward north of the equator with the cross-equatorial flow, to the South China Sea (SCS), the Philippines and even further to the western Pacific. During the October-November transitional period, smoke transport paths are more zonally oriented compared to June-September. Smoke originating from Java, Bali, Timor etc, and southern New Guinea, which are in the domain of easterlies and southeasterlies during the boreal summer (June-November), is generally transported westward. It is also found that smoke transport over the MC exhibits multi-scale variability. Smoke typically lives longer and can be transported farther in El Niño years and later MJO phases compared with non El Niño years and earlier MJO phases. During El Niño periods there is much stronger westward transport to the east tropical Indian Ocean. Finally, orographic effect on smoke transport over the MC is also clearly discernable.

  9. Quantification of aerosol chemical composition using continuous single particle measurements

    NASA Astrophysics Data System (ADS)

    Jeong, C.-H.; McGuire, M. L.; Godri, K. J.; Slowik, J. G.; Rehbein, P. J. G.; Evans, G. J.

    2011-07-01

    Mass concentrations of sulphate, nitrate, ammonium, organic carbon (OC), elemental carbon (EC) were determined from real time single particle data in the size range 0.1-3.0 μm measured by an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) at urban and rural sites in Canada. To quantify chemical species within individual particles measured by an ATOFMS, ion peak intensity of m/z -97 for sulphate, -62 for nitrate, +18 for ammonium, +43 for OC, and +36 for EC were scaled using the number and size distribution data by an Aerodynamic Particle Sizer (APS) and a Fast Mobility Particle Sizer (FMPS). Hourly quantified chemical species from ATOFMS single-particle analysis were compared with collocated fine particulate matter (aerodynamic diameter < 2.5 μm, PM2.5) chemical composition measurements by an Aerosol Mass Spectrometer (AMS) at a rural site, a Gas-Particle Ion Chromatograph (GPIC) at an urban site, and a Sunset Lab field OCEC analyzer at both sites. The highest correlation was found for nitrate, with correlation coefficients (Pearson r) of 0.89 (ATOFMS vs. GPIC) and 0.85 (ATOFMS vs. AMS). ATOFMS mass calibration factors, determined for the urban site, were used to calculate mass concentrations of the major PM2.5 chemical components at the rural site near the US border in southern Ontario. Mass reconstruction using the ATOFMS mass calibration factors agreed very well with the PM2.5 mass concentrations measured by a Tapered Element Oscillating Microbalance (TEOM, r = 0.86) at the urban site and a light scattering monitor (DustTrak, r = 0.87) at the rural site. In the urban area nitrate was the largest contributor to PM2.5 mass in the winter, while organics and sulphate contributed ~64 % of the summer PM2.5 in the rural area, suggesting a strong influence of regional/trans-boundary pollution. The mass concentrations of five major species in ten size-resolved particle-types and aerosol acidity of each particle-type were determined for the rural site. On a mass basis

  10. Hygroscopic, Morphological, and Chemical Properties of Agricultural Aerosols

    NASA Astrophysics Data System (ADS)

    Hiranuma, N.; Brooks, S. D.; Cheek, L.; Thornton, D. C.; Auvermann, B. W.; Littleton, R.

    2007-12-01

    Agricultural fugitive dust is a significant source of localized air pollution in the semi-arid southern Great Plains. In the Texas Panhandle, daily episodes of ground-level fugitive dust emissions from the cattle feedlots are routinely observed in conjunction with increased cattle activity in the late afternoons and early evenings. We conducted a field study to characterize size-selected agricultural aerosols with respect to hygroscopic, morphological, and chemical properties and to attempt to identify any correlations between these properties. To explore the hygroscopic nature of agricultural particles, we have collected size-resolved aerosol samples using a cascade impactor system at a cattle feedlot in the Texas Panhandle and have used the Environmental Scanning Electron Microscope (ESEM) to determine the water uptake by individual particles in those samples as a function of relative humidity. To characterize the size distribution of agricultural aerosols as a function of time, A GRIMM aerosol spectrometer and Sequential Mobility Particle Sizer and Counter (SMPS) measurements were simultaneously performed in an overall size range of 11 nm to 20 µm diameters at a cattle feedlot. Complementary determination of the elemental composition of individual particles was performed using Energy Dispersive X-ray Spectroscopy (EDS). In addition to the EDS analysis, an ammonia scrubber was used to collect ammonia and ammonium in the gas and particulate phases, respectively. The concentration of these species was quantified offline via UV spectrophotometry at 640 nanometers. The results of this study will provide important particulate emission data from a feedyard, needed to improve our understanding of the role of agricultural particulates in local and regional air quality.

  11. Modeling regional secondary organic aerosol using the Master Chemical Mechanism

    NASA Astrophysics Data System (ADS)

    Li, Jingyi; Cleveland, Meredith; Ziemba, Luke D.; Griffin, Robert J.; Barsanti, Kelley C.; Pankow, James F.; Ying, Qi

    2015-02-01

    A modified near-explicit Master Chemical Mechanism (MCM, version 3.2) with 5727 species and 16,930 reactions and an equilibrium partitioning module was incorporated into the Community Air Quality Model (CMAQ) to predict the regional concentrations of secondary organic aerosol (SOA) from volatile organic compounds (VOCs) in the eastern United States (US). In addition to the semi-volatile SOA from equilibrium partitioning, reactive surface uptake processes were used to simulate SOA formation due to isoprene epoxydiol, glyoxal and methylglyoxal. The CMAQ-MCM-SOA model was applied to simulate SOA formation during a two-week episode from August 28 to September 7, 2006. The southeastern US has the highest SOA, with a maximum episode-averaged concentration of ∼12 μg m-3. Primary organic aerosol (POA) and SOA concentrations predicted by CMAQ-MCM-SOA agree well with AMS-derived hydrocarbon-like organic aerosol (HOA) and oxygenated organic aerosol (OOA) urban concentrations at the Moody Tower at the University of Houston. Predicted molecular properties of SOA (O/C, H/C, N/C and OM/OC ratios) at the site are similar to those reported in other urban areas, and O/C values agree with measured O/C at the same site. Isoprene epoxydiol is predicted to be the largest contributor to total SOA concentration in the southeast US, followed by methylglyoxal and glyoxal. The semi-volatile SOA components are dominated by products from β-caryophyllene oxidation, but the major species and their concentrations are sensitive to errors in saturation vapor pressure estimation. A uniform decrease of saturation vapor pressure by a factor of 100 for all condensable compounds can lead to a 150% increase in total SOA. A sensitivity simulation with UNIFAC-calculated activity coefficients (ignoring phase separation and water molecule partitioning into the organic phase) led to a 10% change in the predicted semi-volatile SOA concentrations.

  12. Chemical composition of Eastern Black Sea aerosol--preliminary results.

    PubMed

    Balcılar, Ilker; Zararsız, Abdullah; Kalaycı, Yakup; Doğan, Güray; Tuncel, Gürdal

    2014-08-01

    Trace element composition of atmospheric particles collected at a high altitude site on the Eastern Black Sea coast of Turkey was investigated to understand atmospheric transport of pollutants to this semi-closed basin. Aerosol samples were collected at a timber-storage area, which is operated by the General Directorate of Forestry. The site is situated at a rural area and is approximately 50 km to the Black Sea coast and 200 km to the Georgia border of Turkey. Coarse (PM2.5-10) and fine (PM2.5) aerosol samples were collected between 2011 and 2013 using a "stacked filter unit". Collected samples were shipped to the Middle East Technical University in Ankara, where Na, Mg, Al, Si, S, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Ba, Pb were measured by Energy dispersive x-ray fluorescence technique (EDXRF). Comparison of measured concentrations of elements with corresponding data generated at other parts of Turkey demonstrated that concentrations of pollution derived elements are higher at Eastern Black Sea than their corresponding concentrations measured at other parts of Turkey, which is attributed to frequent transport of pollutants from north wind sector. Positive matric factorization revealed four factors including three anthropogenic and a crustal factor. Southeastern parts of Turkey, Georgia and Black Sea coast of Ukraine were identified as source regions affecting composition of particles at our site, using trajectory statistics, namely "potential source contribution function" (PSCF). PMID:24373640

  13. Aerosol assisted chemical vapor deposition of superconducting YBa 2Cu 3O 7-χ

    NASA Astrophysics Data System (ADS)

    Salazar, K. V.; Ott, K. C.; Dye, R. C.; Hubbard, K. M.; Peterson, E. J.; Coulter, J. Y.; Kodas, T. T.

    1992-08-01

    A hybrid process, aerosol-assisted chemical vapor deposotion (AACVD), is described for reproducible preparation of superconducting thin films of YBa 2Cu 3O 7-χ. The process consists of atomizing a toluene solution of the Y, Ba, and Cu tetramethylheptanedionato complexes using an aerosol generator. The aerosol is transported into a CVD reactor where solvent and precursor evaporation and deposition occur at atmospheric pressure on heated substrates. The process provides stable evaporation rates for all three precursors, yielding constant film stoichiometry throughout the deposition period and from film to film. Superconducting films may be deposited in-situ at substrate heater temperatures above 825°C, or may be formed at lower temperatures by deposition followed by post-deposition annealing at higher temperatures. The microstructure and quality of films are highly dependent on the conditions employed in deposition and in the case of films deposited below 825°C, the post-deposition annealing conditions. Superconducting films prepared by the AACVD/post-annealing process have a metallic normal state resistivity signature with a zero resistance temperature typically above 88K, and are highly c-axis oriented. Transport critical current densities measured at 75 K on polycrystalline films prepared by the AACVD process are 220 000 A/cm 2 and 84 000 A/cm 2 at self-field and 0.1 T, respectively.

  14. Improving Molecular Level Chemical Speciation of Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Worton, D. R.; Decker, M.; Isaacman, G. A.; Chan, A.; Wilson, K. R.; Goldstein, A. H.

    2013-12-01

    A substantial fraction of fine mode aerosols are organic with the majority formed in the atmosphere through oxidation of gas phase compounds emitted from a variety of natural and man-made sources. As a result, organic aerosols are comprised of thousands of individual organic species whose complexity increases exponentially with carbon number and degree of atmospheric oxidation. Chemical characterization of individual compounds present in this complex mixture provides information on sources and transformation processes that are critical for apportioning organic carbon from an often convoluted mixture of sources and to constrain oxidation mechanisms needed for atmospheric models. These compounds also affect the physical and optical properties of the aerosol but the vast majority remain unidentified and missing from published mass spectral libraries because of difficulties in separating and identifying them. We have developed improved methodologies for chemical identification in order to better understand complex environmental mixtures. Our approach has been to combine two-dimensional gas chromatography with high resolution time of flight mass spectrometry (GC×GC-HRTOFMS) and both traditional electron ionization (EI) and vacuum ultraviolet (VUV) photoionization. GC×GC provides improved separation of individual compounds over traditional one dimensional GC and minimizes co-elution of peaks resulting in mass spectra that are virtually free of interferences. VUV ionization is a ';soft' ionization technique that reduces fragmentation and enhances the abundance of the parent or molecular ion, which when combined with high resolution mass spectrometry can provide molecular formulas for chromatographic peaks. We demonstrate our methodology by applying it to identify more than 500 individual compounds in aerosol filter samples collected at Blodgett Forest, a rural site in the Sierra Nevada Mountains. Using the EI NIST mass spectral library and molecular formulas determined

  15. The long-range transport of southern African aerosols to the tropical South Atlantic

    NASA Astrophysics Data System (ADS)

    Swap, R.; Garstang, M.; Macko, S. A.; Tyson, P. D.; Maenhaut, W.; Artaxo, P.; KâLlberg, P.; Talbot, R.

    1996-10-01

    Two episodes of long-range aerosol transport (4000 km) from southern Africa into the central tropical South Atlantic are documented. Stable nitrogen isotope analysis, multielemental analysis, and meteorological observations on local and regional scales are used to describe the observed surface aerosol chemistry during these transport episodes. The chemical, kinematic, and thermodynamic analyses suggest that for the central tropical South Atlantic, west Africa between 0° and 10°S is the primary air mass source region (over 50%) during austral spring. Over 70% of all air arriving in the lower and middle troposphere in the central tropical South Atlantic comes from a broad latitudinal band extending from 20°S to 10°N. Air coming from the east subsides and is trapped below the midlevel and trade wind inversion layers. Air from the west originates at higher levels (500 hPa) and contributes less than 30% of the air masses arriving in the central tropical South Atlantic. The source types of aerosols and precursor trace gases extend over a broad range of biomes from desert and savanna to the rain forest. During austral spring, over this broad region, processes include production from vegetation, soils, and biomass burning. The aerosol composition of air masses over and the atmospheric chemistry of the central South Atlantic is a function of the supply of biogenic, biomass burning, and aeolian emissions from tropical Africa. Rainfall is a common controlling factor for all three sources. Rain, in turn, is governed by the large-scale circulations which show pronounced interannual variability. The field measurements were taken in an extremely dry year and reflect the circulation and transport fields typical of these conditions.

  16. Chemical insights, explicit chemistry and yields of secondary organic aerosol from methylglyoxal and glyoxal

    NASA Astrophysics Data System (ADS)

    Lim, Y. B.; Tan, Y.; Turpin, B. J.

    2013-02-01

    Atmospherically abundant, volatile water soluble organic compounds formed through gas phase chemistry (e.g., glyoxal (C2), methylglyoxal (C3) and acetic acid) have great potential to form secondary organic aerosol (SOA) via aqueous chemistry in clouds, fogs and wet aerosols. This paper (1) provides chemical insights into aqueous-phase OH radical-initiated reactions leading to SOA formation from methylglyoxal and (2) uses this and a previously published glyoxal mechanism (Lim et al., 2010) to provide SOA yields for use in chemical transport models. Detailed reaction mechanisms including peroxy radical chemistry and a full kinetic model for aqueous photochemistry of acetic acid and methylglyoxal are developed and validated by comparing simulations with the experimental results from previous studies (Tan et al., 2010, 2012). This new methylglyoxal model is then combined with the previous glyoxal model (Lim et al., 2010), and is used to simulate the profiles of products and to estimate SOA yields. At cloud relevant concentrations (∼ 10-6-∼ 10-3 M; Munger et al., 1995) of glyoxal and methylglyoxal, the major photooxidation products are oxalic acid and pyruvic acid, and simulated SOA yields (by mass) are ∼ 120% for glyoxal and ∼ 80% for methylglyoxal. Oligomerization of unreacted aldehydes during droplet evaporation could enhance yields. In wet aerosols, where total dissolved organics are present at much higher concentrations (∼ 10 M), the major products are oligomers formed via organic radical-radical reactions, and simulated SOA yields (by mass) are ∼ 90% for both glyoxal and methylglyoxal.

  17. Inland transport of marine aerosols in southern Sweden

    NASA Astrophysics Data System (ADS)

    Gustafsson, Mats E. R.; Franzén, Lars G.

    The transport of marine aerosols across southern Sweden was studied using six meteorological stations in a transect from west- to east-coast. Measurements were made during dry westerlies on 10 occasions during 1995. The concentration and flux of salt in the air was measured using "salt vanes". It is concluded that marine salt is transported along the whole transect at all occasions and that the concentration and flux of salt decrease with downwind distance from the coast as an inversed power function. The two easternmost stations show a slight increase towards the east-coast. Variability of the data is high on the west coast due to strong influence from the coastal production of aerosols. This effect diminishes along downwind forming lower, less variable concentration further inland. Statistical models based on the data are in relatively good agreement with previous models and data. Further, salt content on Scots Pine ( Pinus sylvestris, L) needles after two westerly gale occasions, in profiles from west- to east-coast, were analysed. The Cl -/Na +, Ca 2+/Na +, K +/Na +, Mg 2+/Na + and SO 42-/Na + ratios were studied revealing a clear downwind decrease in Ca 2+/Na + and Mg 2+/Na +, a close to sea water ratio for Cl -/Na + and an excess of SO 42- along the profile. Also, the importance of degree of exposure was studied concluding that the roughness of the upwind surface is an important factor for the deposition onto trees in forest edges.

  18. Gas uptake and chemical aging of semisolid organic aerosol particles.

    PubMed

    Shiraiwa, Manabu; Ammann, Markus; Koop, Thomas; Pöschl, Ulrich

    2011-07-01

    Organic substances can adopt an amorphous solid or semisolid state, influencing the rate of heterogeneous reactions and multiphase processes in atmospheric aerosols. Here we demonstrate how molecular diffusion in the condensed phase affects the gas uptake and chemical transformation of semisolid organic particles. Flow tube experiments show that the ozone uptake and oxidative aging of amorphous protein is kinetically limited by bulk diffusion. The reactive gas uptake exhibits a pronounced increase with relative humidity, which can be explained by a decrease of viscosity and increase of diffusivity due to hygroscopic water uptake transforming the amorphous organic matrix from a glassy to a semisolid state (moisture-induced phase transition). The reaction rate depends on the condensed phase diffusion coefficients of both the oxidant and the organic reactant molecules, which can be described by a kinetic multilayer flux model but not by the traditional resistor model approach of multiphase chemistry. The chemical lifetime of reactive compounds in atmospheric particles can increase from seconds to days as the rate of diffusion in semisolid phases can decrease by multiple orders of magnitude in response to low temperature or low relative humidity. The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate.

  19. Chemical Characterization of the Aerosol During the CLAMS Experiment Using Aircraft and Ground Stations

    NASA Astrophysics Data System (ADS)

    Castanho, A. D.; Martins, J.; Artaxo, P.; Hobbs, P. V.; Remer, L.; Yamasoe, M.; Fattori, A.

    2002-05-01

    During the Chesapeake Lighthouse and Aircraft Measurements for Satellites (CLAMS) Experiment Nuclepore filters were collected in two ground stations and aboard the University of Wasghington's Convair 580 Reserarch Aircraft. The two ground stations were chosen in strategic positions to characterize the chemical composition, the mass concentration, black carbon (BC) content, and the absorption properties of the aerosol particles at the surface level. One of the stations was located at the Cheasapeake lighthouse (25 km from the coast) and the other one was located at the Wallops Island. Aerosol particles where collected in two stages, fine (d<2.5um) and coarse mode (2.5aerosol in the atmospheric column in the CLAMS Experiment area. Some of the filters were also submitted to Scanning Electron Microscopy analysis. The particulate matter mass for all the samples were obtained gravimetrically. The concentration of black carbon in the fine filters was optically determined by a broadband reflectance technique. The spectral (from UV to near IR) reflectance in the fine and coarse mode filter were also obtained with a FieldSpec ASD spectrometer. Aerosol elemental characterization (Na through Pb) was obtained by the PIXE (Particle induced X ray emission) analyses of the nuclepore filters. The sources of the aerosol measured at the ground stations were estimated by principal component analyses mainly in the Wallops Island, where a longer time series was collected. One of the main urban components identified in the aerosol during the experiment was sulfate. Black carbon

  20. Chemical characterization of springtime submicrometer aerosol in Po Valley, Italy

    NASA Astrophysics Data System (ADS)

    Saarikoski, S.; Carbone, S.; Decesari, S.; Giulianelli, L.; Angelini, F.; Canagaratna, M.; Ng, N. L.; Trimborn, A.; Facchini, M. C.; Fuzzi, S.; Hillamo, R.; Worsnop, D.

    2012-09-01

    The chemistry of submicron particles was investigated at San Pietro Capofiume (SPC) measurement station in the Po Valley, Italy, in spring 2008. The measurements were performed by using both off-line and on-line instruments. Organic carbon (OC) and elemental carbon, organic acids and biomass burning tracers were measured off-line by using a 24-h PM1 filter sampling. More detailed particle chemistry was achieved by using a Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and analyzing the data by positive matrix factorization (PMF). Oxalic acid had the highest concentrations of organic acids (campaign-average 97.4 ng m-3) followed by methane sulfonic, formic, malonic, and malic acids. Samples were also analyzed for glyoxylic, succinic, azelaic and maleic acids. In total, the nine acids composed 1.9 and 3.8% of OC and water-soluble OC, respectively (average), in terms of carbon atoms. Levoglucosan concentration varied from 17.7 to 495 ng m-3 with the concentration decreasing in the course of the campaign most likely due to the reduced use of domestic heating with wood. Six factors were found for organic aerosol (OA) at SPC by PMF: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), nitrogen-containing OA (N-OA) and three different oxygenated OAs (OOA-a, OOA-b and OOA-c). Most of the OA mass was composed of OOA-a, HOA and OOA-c (26, 24 and 22%, respectively) followed by OOA-b (13%), BBOA (8%) and N-OA (7%). As expected, OOAs were the most oxygenated factors with organic matter:organic carbon (OM : OC) ratios ranging from 1.9 to 2.2. The diurnal variability of the aerosol chemical composition was greatly affected by the boundary layer meteorology. Specifically, the effect of the nocturnal layer break-up in morning hours was most evident for nitrate and N-OA indicating that these compounds originated mainly from the local sources in the Po Valley. For sulfate and OOA-a the concentration did not change during the break-up suggesting their

  1. Chemical characterization of springtime submicrometer aerosol in Po Valley, Italy

    NASA Astrophysics Data System (ADS)

    Saarikoski, S.; Carbone, S.; Decesari, S.; Giulianelli, L.; Angelini, F.; Teinilä, K.; Canagaratna, M.; Ng, N. L.; Trimborn, A.; Facchini, M. C.; Fuzzi, S.; Hillamo, R.; Worsnop, D.

    2012-03-01

    The chemistry of submicron particles was investigated at San Pietro Capofiume (SPC) measurement station in the Po Valley, Italy, in spring 2008. The measurements were performed by using both off-line and on-line instruments. Organic carbon (OC) and elemental carbon, organic acids and biomass burning tracers were measured off-line by using a 24-h PM1 filter sampling. More detailed particle chemistry was achieved by using an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and analyzing the data by positive matrix factorization (PMF). Oxalic acid had the highest concentrations of organic acids (campaign-average 97.4 ng m-3) followed by methane sulfonic, formic, malonic, and malic acids. Samples were also analyzed for glyoxylic, succinic, azelaic and maleic acids. In total, the nine acids composed 1.9 and 3.8% of OC and water-soluble OC, respectively (average), in terms of carbon atoms. Levoglucosan concentration varied from 17.7 to 495 ng m-3 with the concentration decreasing in the course of the campaign most likely due to the reduced use of domestic heating with wood. Six factors were found for organic aerosol (OA) at SPC by PMF: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), nitrogen-containing OA (N-OA) and three different oxygenated OAs (OOA-a, OOA-b and OOA-c). Most of the OA mass was composed of OOA-a, HOA and OOA-c (26, 24 and 22%, respectively) followed by OOA-b (13%), BBOA (8%) and N-OA (7%). As expected, OOAs were the most oxygenated factors with organic matter:organic carbon (OM:OC) ratios ranging from 1.9 to 2.2. The diurnal variability of the aerosol chemical composition was greatly affected by the boundary layer meteorology. Specifically, the effect of the nocturnal layer break-up in morning hours was most evident for nitrate and N-OA indicating that these compounds originated mainly from the local sources in the Po Valley. For sulfate and OOA-a the concentration did not change during the break-up suggesting their

  2. Trans-Pacific transport and evolution of aerosols: evaluation of quasi-global WRF-Chem simulation with multiple observations

    NASA Astrophysics Data System (ADS)

    Hu, Zhiyuan; Zhao, Chun; Huang, Jianping; Leung, L. Ruby; Qian, Yun; Yu, Hongbin; Huang, Lei; Kalashnikova, Olga V.

    2016-05-01

    interannual variability of aerosol characteristics for 2010-2014 averaged over three Pacific sub-regions. The evaluation in this study demonstrates that the WRF-Chem quasi-global simulation can be used for investigating trans-Pacific transport of aerosols and providing reasonable inflow chemical boundaries for the western USA, allowing one to further understand the impact of transported pollutants on the regional air quality and climate with high-resolution nested regional modeling.

  3. Trans-Pacific transport and evolution of aerosols: Evaluation of quasi-global WRF-Chem simulation with multiple observations

    DOE PAGES

    Hu, Zhiyuan; Zhao, Chun; Huang, Jianping; Leung, L. Ruby; Qian, Yun; Yu, Hongbin; Huang, Lei; Kalashnikova, Olga V.

    2016-05-10

    small interannual variability of aerosol characteristics for 2010–2014 averaged over three Pacific sub-regions. Furthermore, the evaluation in this study demonstrates that the WRF-Chem quasi-global simulation can be used for investigating trans-Pacific transport of aerosols and providing reasonable inflow chemical boundaries for the western USA, allowing one to further understand the impact of transported pollutants on the regional air quality and climate with high-resolution nested regional modeling.« less

  4. Trans-Pacific transport and evolution of aerosols: evaluation of quasi-global WRF-Chem simulation with multiple observations

    SciTech Connect

    Hu, Zhiyuan; Zhao, Chun; Huang, Jianping; Leung, L. Ruby; Qian, Yun; Yu, Hongbin; Huang, Lei; Kalashnikova, Olga V.

    2016-01-01

    interannual variability of aerosol characteristics for 2010–2014 averaged over three Pacific sub-regions. The evaluation in this study demonstrates that the WRF-Chem quasi-global simulation can be used for investigating trans-Pacific transport of aerosols and providing reasonable inflow chemical boundaries for the western USA, allowing one to further understand the impact of transported pollutants on the regional air quality and climate with high-resolution nested regional modeling.

  5. Microbiology and atmospheric processes: chemical interactions of Primary Biological Aerosols

    NASA Astrophysics Data System (ADS)

    Deguillaume, L.; Leriche, M.; Amato, P.; Ariya, P. A.; Delort, A.-M.; Pöschl, U.; Chaumerliac, N.; Bauer, H.; Flossmann, A. I.; Morris, C. E.

    2008-02-01

    This paper discusses the influence of bioaerosols on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that biological matter represents a significant fraction of air particulate matter and hence affects the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of primary biological particles in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere.

  6. Water-Soluble Organic Species in Biomass Burning Aerosols in Southern Africa: Their Chemical Identification and Spatial Distribution

    NASA Astrophysics Data System (ADS)

    Gao, S.; Hegg, D. A.; Hobbs, P. V.; Kirchstetter, T. W.; Magi, B.

    2001-12-01

    diacids, during aerosol upward transport and aging. It was also found that smoldering fires produced much more anhydrosugars and other tarry material than flaming fires. These results provide support for some earlier laboratory studies of biomass burning, but also pose new questions as to the complicated chemical reactions involved. Furthermore, it is evident that besides chemical reactions, fire types, meteorological conditions, and the properties of the reaction products, such as volatility, all play important and interconnected roles in aerosol formation in smokes. Implications of these results for the CCN activity of aerosols from biomass burning will be discussed briefly.

  7. Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Shiraiwa, M.; Berkemeier, T.; Schilling-Fahnestock, K. A.; Seinfeld, J. H.; Pöschl, U.

    2014-08-01

    The dominant component of atmospheric, organic aerosol is that derived from the oxidation of volatile organic compounds (VOCs), so-called secondary organic aerosol (SOA). SOA consists of a multitude of organic compounds, only a small fraction of which has historically been identified. Formation and evolution of SOA is a complex process involving coupled chemical reaction and mass transport in the gas and particle phases. Current SOA models do not embody the full spectrum of reaction and transport processes, nor do they identify the dominant rate-limiting steps in SOA formation. Based on molecular identification of SOA oxidation products, we show here that the chemical evolution of SOA from a variety of VOC precursors adheres to characteristic "molecular corridors" with a tight inverse correlation between volatility and molar mass. The slope of these corridors corresponds to the increase in molar mass required to decrease volatility by one order of magnitude (-dM / dlogC0). It varies in the range of 10-30 g mol-1, depending on the molecular size of the SOA precursor and the O : C ratio of the reaction products. Sequential and parallel reaction pathways of oxidation and dimerization or oligomerization progressing along these corridors pass through characteristic regimes of reaction-, diffusion-, or accommodation-limited multiphase chemical kinetics that can be classified according to reaction location, degree of saturation, and extent of heterogeneity of gas and particle phases. The molecular corridors and kinetic regimes help to constrain and describe the properties of the products, pathways, and rates of SOA evolution, thereby facilitating the further development of aerosol models for air quality and climate.

  8. Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Shiraiwa, M.; Berkemeier, T.; Schilling-Fahnestock, K.; Seinfeld, J.; Poeschl, U.

    2014-12-01

    The dominant component of atmospheric organic aerosol is that derived from the oxidation of volatile organic compounds (VOCs), so-called secondary organic aerosol (SOA). SOA consists of a multitude of organic compounds, only a small fraction of which has historically been identified. Formation and evolution of SOA is a complex process involving coupled chemical reaction and mass transport in the gas and particle phases. Current SOA models do not embody the full spectrum of reaction and transport processes nor do they identify the dominant rate-limiting steps in SOA formation. Based on molecular identification of SOA oxidation products, we show here that the chemical evolution of SOA from a variety of VOC precursors adheres to characteristic "molecular corridors" with a tight inverse correlation between volatility and molar mass. The slope of these corridors corresponds to the increase in molar mass required to decrease volatility by one order of magnitude (-dM/dlogC0). It varies in the range of 10-30 g mol-1 depending on the molecular size of the SOA precursor and the O:C ratio of the reaction products. Sequential and parallel reaction pathways of oxidation and dimerization or oligomerization progressing along these corridors pass through characteristic regimes of reaction-, diffusion-, or accommodation-limited multiphase chemical kinetics that can be classified according to reaction location, degree of saturation, and extent of heterogeneity of gas and particle phases. The molecular corridors and kinetic regimes help to constrain and described the properties of the products, pathways and rates of SOA evolution, thereby facilitating the further development of aerosol models for air quality and climate.

  9. Chemical characteristics of ambient aerosols contributed by cooking process at Noorpur village near New Delhi

    NASA Astrophysics Data System (ADS)

    Singh, Sudha

    Generally, industrial and transport sectors are considered as major contributors of air pollution but recently, biomass burning is also reported as a major source of atmospheric aerosols (1, 2) especially in the developing world where solid fuels such as dung cake, wood and crop residues are used in traditional cooking which are responsible for poor air quality, respiratory problems and radiative forcing etc .In India, most of the research has been focused on emission estimates from biomass burning and cooking. No effort has been made to understand the chemistry and sources of fine aerosols in rural areas during cooking hours. This study fills this knowledge gap and strengthens our understanding about abundance of various chemical constituents of atmospheric aerosols emitted during cooking hours.Aerosol samples were collected from village called Noorpur (28.470 N, 77.030 E) which lies near Delhi city. Sampling was carried out during August 2011-May 2012 by using handy sampler (Envirotech model APM 821) installed at the terrace of a building (~6m). The aerosol samples were collected on 8 hourly basis at a flow rate of 1 LPM. Water extracts of these filters were analyzed for major anions (F-, Cl-, NO3-, SO42-) and major cations (Na+, NH4+, K+, Ca2+ Mg2+) by ion chromatography (Metrohm 883 Basic IC Plus). During cooking period, the concentration of the major ions followed the order of Ca2+> SO42-> NO3-> Cl-> K+> NH4+> Mg2+> Na2+> F-. Among anion SO42 (5 µg/m3) showed highest value and in case of cations Ca2+ (7.32µg/m3) has highest value.

  10. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-06-01

    An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed along with a Scanning Mobility Particle Sizer (SMPS) and a Multi Angle Absorption Photometers (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1) in Lanzhou, northwest China, during 12 July-7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution mass spectra of organic aerosols (OA) identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns both with peak at ~07:00-11:00 (BJT: UTC +8) corresponding to the morning rush hours, while cooking OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00-15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00-13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity with that of

  11. INFLUENCE OF MACROMOLECULES ON CHEMICAL TRANSPORT

    EPA Science Inventory

    Macromolecules in the pore fluid influence the mobility of hydrophobic compounds through soils. his study evaluated the significance of macromolecules in facilitating chemical transport under laboratory conditions. Partition coefficients between 14C-labeled hexachlorobenzene and ...

  12. Aerosol transport and deposition efficiency in the respiratory airways

    NASA Astrophysics Data System (ADS)

    Nicolaou, Laura; Zaki, Tamer

    2015-11-01

    Prediction of aerosol deposition in the respiratory system is important for improving the efficiency of inhaled drug delivery and for assessing the toxicity of airborne pollutants. Particle deposition in the airways is typically described as a function of the Stokes number based on a reference flow timescale. This choice leads to significant scatter in deposition data since the velocity and length scales experienced by the particles as they are advected through the flow deviate considerably from the reference values in many sections of the airways. Therefore, the use of an instantaneous Stokes number based on the local properties of the flow field is proposed instead. We define the effective Stokes number as the time-average of the instantaneous value. Our results demonstrate that this average, or effective, Stokes number can deviate significantly from the reference value particularly in the intermediate Stokes number range. In addition, the effective Stokes number shows a very clear correlation with deposition efficiency, and is therefore a more appropriate parameter to describe aerosol transport.

  13. Assessing Impact of Aerosol Intercontinental Transport on Regional Air Quality and Climate: What Satellites Can Help

    NASA Technical Reports Server (NTRS)

    Yu, Hongbin

    2011-01-01

    Mounting evidence for intercontinental transport of aerosols suggests that aerosols from a region could significantly affect climate and air quality in downwind regions and continents. Current assessment of these impacts for the most part has been based on global model simulations that show large variability. The aerosol intercontinental transport and its influence on air quality and climate involve many processes at local, regional, and intercontinental scales. There is a pressing need to establish modeling systems that bridge the wide range of scales. The modeling systems need to be evaluated and constrained by observations, including satellite measurements. Columnar loadings of dust and combustion aerosols can be derived from the MODIS and MISR measurements of total aerosol optical depth and particle size and shape information. Characteristic transport heights of dust and combustion aerosols can be determined from the CALIPSO lidar and AIRS measurements. CALIPSO liar and OMI UV technique also have a unique capability of detecting aerosols above clouds, which could offer some insights into aerosol lofting processes and the importance of above-cloud transport pathway. In this presentation, I will discuss our efforts of integrating these satellite measurements and models to assess the significance of intercontinental transport of dust and combustion aerosols on regional air quality and climate.

  14. Assessing the influence of secondary organic aerosols on long-range atmospheric PAH transport

    NASA Astrophysics Data System (ADS)

    Friedman, C. L.; Selin, N. E.

    2013-12-01

    We incorporate recent experimental findings on the synergy between secondary organic aerosols (SOA) and polycyclic aromatic hydrocarbons (PAHs) in a global atmospheric chemical transport model to test the influence of different gas-particle partitioning parameterizations on long-range atmospheric transport of PAHs. PAHs, byproducts of organic combustion, are toxic compounds that have been measured in areas distant from sources, such as the Arctic. Historically, the transport of PAHs in the atmosphere has been modeled by assuming that PAHs instantaneously and reversibly equilibrate between the gas phase and a particulate phase, with observed particulate fractions often times exceeding model results for unknown reasons. Recently obtained laboratory-based findings suggest PAHs become trapped in SOA particles during SOA formation and are thus prevented from evaporation and/or oxidation, possibly explaining discrepancies between observed and modeled particulate fractions. Here, we use the global atmospheric chemical transport model GEOS-Chem to investigate whether incorporation of pyrene, a four-ring PAH, into SOA upon formation better represents atmospheric long-range transport and gas-particle speciation of PAHs compared to our default partitioning scheme, in which PAHs instantaneously equilibrate between the gas phase, primary organic carbon aerosols (OC), and black carbon aerosols (BC). In general, we find that BC plays an important role in pyrene transport and gas-particle partitioning, with a model that includes BC producing the best match to observed seasonal variation and magnitude of pyrene particulate fraction. Incorporation of 100% of pyrene into SOA upon emission with fractional evaporation thereafter results in a reasonable match to observed total pyrene concentrations in the northern hemisphere mid-latitudes, but severely overestimates particulate fraction. Assuming that pyrene partitions to SOA following an octanol-air equilibrium partition coefficient

  15. Characterization of Microphysical Properties of Saharan Dust Aerosols During Trans-Atlantic Transport

    NASA Astrophysics Data System (ADS)

    Roldan, L.; Morris, V. R.

    2005-12-01

    The NOAA Center in Atmospheric Sciences (NCAS) Trans-Atlantic Saharan Dust AERosol and Ocean Science Expedition (AEROSE) 2004 was a 27 day mission aboard the NOAA Ship Ronald H. Brown (RHB). The AEROSE mission took place during February 29th thru March 26th, departing from Barbados to the Canary Islands and ending in Puerto Rico. The cruise tracks for AEROSE 2004 coincided with one of the biggest dust storms to date for this season. One of the goals of the mission was to provide a set of critical measurements to characterize the impacts and microphysical evolution of Saharan dust aerosol during Trans-Atlantic transport. A Laser Particle Counter (LPC) was used to retrieve in-situ number density distribution. A Quartz Crystal Microbalance Cascade Impactor (QCM) was used to retrieve in-situ mass density distributions. The QCM also provides a sampling platform for post analysis to determine morphological properties and elemental chemical composition. The morphological properties were determined with the use of a Scanning Electron Microscope (SEM). The combination of the SEM with an Energy Dispersive X-Ray Microanalysis system provides the elemental composition details. I will present the evolution of the chemical elements as a function of size as they are transported. The elemental analysis has identified elements such as Fe, Al, Si, Zn, Ti, Co, S, and C all which are characteristics of Saharan dust origin.

  16. All-year-round aerosol chemical composition at Dome C, Antarctica

    NASA Astrophysics Data System (ADS)

    Udisti, Roberto; Becagli, Silvia; Frosini, Daniele; Galli, Gaia; Ghedini, Costanza; Rugi, Francesco; Severi, Mirko; Traversi, Rita

    2010-05-01

    Since 2005, continuous, all-year-round aerosol sampling was carried out at Dome C (Central East Antarctica, 3233 m a.s.l., about 1100 km far from the coastline), in the framework of "Station Concordia" project, an Italian PNRA - French IPEV joint program. Size-segregated aerosol samples were collected in summer and winter periods by using different low- and medium-volume systems, including pre-selected cut-off samplers (with PM10, PM2.5 and PM1 cut-off heads) and multi-stage (Andersen 8-stage and Dekati 4-stage) impactors. Sampling resolution and volumes ranged from 1 day to 1 month and from 2.3 to 12 m3/h, respectively. Aerosol study at Dome C is expected improving our knowledge on present-day source intensity, transport efficiency and pathways (including stratosphere-troposphere interchanges) of particles reaching internal sites of Antarctica. Besides, more detailed information on atmosphere-snow interactions, including depositional and post-depositional processes, as well as the effect of sublimation/condensation processes on snow surface, will be used for improving the reconstruction of past atmosphere composition from ice core chemical stratigraphies (EPICA Dome C ice core). Here we report major results from the chemical composition of the Antarctic background aerosol reaching Dome C, pointing out the seasonal pattern and the temporal trend of some ionic components used as tracers of sea spray, marine biogenic and crustal emissions. Oxidised sulfur compounds are assumed to affect the climate system by influencing the Earth's radiative budget, both directly (solar light scattering) and indirectly (acting as cloud condensation nuclei). Among these compounds, methanesulphonic acid (MSA) and H2SO4 (arising from the atmospheric oxidation of phytoplanktonic dimethylsulphide - DMS), are considered the best tracers of marine productivity. Their use as reliable markers of oceanic biogenic emissions is hindered by poorly known mechanisms (temperature and photochemistry

  17. Columnar aerosol optical properties at AERONET sites in central eastern Asia and aerosol transport to the tropical mid-Pacific

    NASA Astrophysics Data System (ADS)

    Eck, T. F.; Holben, B. N.; Dubovik, O.; Smirnov, A.; Goloub, P.; Chen, H. B.; Chatenet, B.; Gomes, L.; Zhang, X.-Y.; Tsay, S.-C.; Ji, Q.; Giles, D.; Slutsker, I.

    2005-03-01

    The column-integrated optical properties of aerosol in the central eastern region of Asia and midtropical Pacific were investigated based on Sun/sky radiometer measurements made at Aerosol Robotic Network (AERONET) sites in these regions. Characterization of aerosol properties in the Asian region is important due to the rapid growth of both population and economic activity, with associated increases in fossil fuel combustion, and the possible regional and global climatic impacts of related aerosol emissions. Multiyear monitoring over the complete annual cycle at sites in China, Mongolia, South Korea, and Japan suggest spring and/or summer maximum in aerosol optical depth (τa) and a winter minimum; however, more monitoring is needed to establish accurate climatologies. The annual cycle of Angstrom wavelength exponent (α) showed a springtime minimum associated with dust storm activity; however, the monthly mean α440-870 was >0.8 even for the peak dust season at eastern Asian sites suggesting that fine mode pollution aerosol emitted from population centers in eastern Asia dominates the monthly aerosol optical influence even in spring as pollution aerosol mixes with coarse mode dust originating in western source regions. Aerosol optical depth peaks in spring in the tropical mid-Pacific Ocean associated with seasonal shifts in atmospheric transport from Asia, and ˜35% of the springtime τa500 enhancement occurs at altitudes above 3.4 km. For predominately fine mode aerosol pollution cases, the average midvisible (˜550 nm) single scattering albedo (ω0) at two continental urban sites in China averaged ˜0.89, while it was significantly higher, ˜0.93, at two relatively rural coastal sites in South Korea and Japan. Differences in fine mode absorption between these regions may result from a combination of factors including aerosol aging during transport, relative humidity differences, sea salt at coastal sites, and fuel type and combustion differences in the two

  18. Atmospheric Modelling of Aerosols Long-Range Transport over the Himalayas

    NASA Astrophysics Data System (ADS)

    Surapipith, V.; Adhikary, B.; Bhave, P.; Panday, A. K.; Mukherji, A.

    2014-12-01

    An Atmospheric Modelling System has been set up at International Centre for Integrated Mountain Development (ICIMOD) Headquarters in Kathmandu, Nepal, for the assessment of air quality in the Hindukush Himalaya region. The Weather Research and Forecasting with Chemistry (WRF-Chem) model version 3.6 is being implemented over a regional domain stretching across 4995 x 4455 km centred at Kathmandu, where an intensive field campaign, Sustainable Atmosphere for the Kathmandu Valley (SusKat) took place from December 2012 to February 2013. Seven stations around the valley collected data on meteorology and chemical parameters. WRF-Chem simulation are carried out for the winter time period at high horizontal resolution (1 km × 1 km), which is achieved by nesting the domain of interest, e.g. Kathmandu Valley, inside three coarser domains. Model validation is performed against the field data as well as satellite data, focusing on aerosols. The challenge of capturing the necessary atmospheric processes is discussed. The effort aims for a better understanding of atmospheric processes and aerosol impacts, as well as the impact of long-range transport, particularly of black carbon aerosol upon the radiative budget over the Himalayan glaciers. The rapid melting of Himalayan glaciers and snowfields, and the shrinkage of permafrost as noticed by glaciologists is a concern. Based on physically adjusted schemes, the WRF meteorological model performs well with Pearson correlation coefficients higher than 0.8 for temperature and solar radiation, although it has a tendency to overestimate wind speed. The WRF with chemistry is then used with local and regional emission databases, in combination and after comparison with the global inventory, as input for describing the long-range transport of aerosols. Improved aerosol prediction will allow us to provide crucial information needed for mitigation and adaptation strategies that save people's lives across the Himalaya. The regional

  19. Chemical, physical, and optical evolution of biomass burning aerosols: a case study

    NASA Astrophysics Data System (ADS)

    Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

    2011-02-01

    In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.

  20. Elucidating the Chemical Complexity of Organic Aerosol Constituents Measured During the Southeastern Oxidant and Aerosol Study (SOAS)

    NASA Astrophysics Data System (ADS)

    Yee, L.; Isaacman, G. A.; Spielman, S. R.; Worton, D. R.; Zhang, H.; Kreisberg, N. M.; Wilson, K. R.; Hering, S. V.; Goldstein, A. H.

    2013-12-01

    Thousands of volatile organic compounds are uniquely created in the atmosphere, many of which undergo chemical transformations that result in more highly-oxidized and often lower vapor pressure species. These species can contribute to secondary organic aerosol, a complex mixture of organic compounds that is still not chemically well-resolved. Organic aerosol collected on filters taken during the Southeastern Oxidant and Aerosol Study (SOAS) constitute hundreds of unique chemical compounds. Some of these include known anthropogenic and biogenic tracers characterized using standardized analytical techniques (e.g. GC-MS, UPLC, LC-MS), but the majority of the chemical diversity has yet to be explored. By employing analytical techniques involving sample derivatization and comprehensive two-dimensional gas chromatography (GC x GC) with high-resolution-time-of-flight mass spectrometry (HR-ToF-MS), we elucidate the chemical complexity of the organic aerosol matrix along the volatility and polarity grids. Further, by utilizing both electron impact (EI) and novel soft vacuum ultraviolet (VUV) ionization mass spectrometry, a greater fraction of the organic mass is fully speciated. The GC x GC-HR-ToF-MS with EI/VUV technique efficiently provides an unprecedented level of speciation for complex ambient samples. We present an extensive chemical characterization and quantification of organic species that goes beyond typical atmospheric tracers in the SOAS samples. We further demonstrate that complex organic mixtures can be chemically deconvoluted by elucidation of chemical formulae, volatility, functionality, and polarity. These parameters provide insight into the sources (anthropogenic vs. biogenic), chemical processes (oxidation pathways), and environmental factors (temperature, humidity), controlling organic aerosol growth in the Southeastern United States.

  1. A new Isotope Tracer to Identify Long Range Transport and Transformation of Aerosol

    NASA Astrophysics Data System (ADS)

    Shaheen, R.; Abramian, A.; Dominguez, G.; Bluen, B.; Jackson, T.; Thiemens, M. H.

    2007-12-01

    It is of interest to understand the intercontinental transport of dust particles because they can accumulate anthropogenic nitrate, sulphate and carbonaceous compounds (black carbon and aromatic hydrocarbon) on their surfaces by adsorption during transportation. Carbonate is a prominent component of the soils in north western China where much of the Asian dust is produced. Carbonate can affect atmospheric chemical processes and aerosol characteristics because the acid neutralizing capacity of this species facilitates the heterogeneous conversion of sulphate and nitrate The primary goal of this work is to develop an isotope methodology for carbonates that can be used as a chemical marker for the origin of polluted air plumes. The results will be compared with other established tracers such as nitrate and sulphate that possess anomalous oxygen isotopic composition in polluted environments from reaction with ozone. Aerosol samples were collected on filter papers using Anderson Cascade Impactors at two different locations in La Jolla, California: one at the Scripps Pier and the other one at coastal Mount Soledad (800 ft). The particulate samples were allowed to react with excess H3PO4 at 28 oC for 14h and the gaseous compounds released were collected at liquid nitrogen. CO2 gas was separated from other reaction products by gas chromatography. In order to measure the oxygen isotope composition, CO2 gas was fluorinated to release oxygen gas to be analysed on the isotope ratio mass spectrometer. We discuss the carbon and oxygen isotope composition of the CO2 released from the fine (< 1 um) and coarse (> 1um) particles collected at two different sites (Mt. Soledad and Scripps Pier) and its utility as a tracer to identify the long range transport of aerosol from local pollution events. The secondary organic oxidation products and concomitant isotope may provide a new indicator of chemical transformation. The transport situation of the air parcels will be analyzed through

  2. Global and Regional Impacts of HONO on the Chemical Composition of Clouds and Aerosols

    NASA Technical Reports Server (NTRS)

    Elshorbany, Y. F.; Crutzen, P. J.; Steil, B.; Pozzer, A.; Tost, H.; Lelieveld, J.

    2014-01-01

    Recently, realistic simulation of nitrous acid (HONO) based on the HONO / NOx ratio of 0.02 was found to have a significant impact on the global budgets of HOx (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation

  3. Global and Regional Impacts of HONO on the Chemical Composition of Clouds and Aerosols

    NASA Technical Reports Server (NTRS)

    Elshorbany, Y. F.; Crutzen, P. J.; Steil, B.; Pozzer, A.; Tost, H.; Lelieveld, J.

    2014-01-01

    Recently, realistic simulation of nitrous acid (HONO) based on the HONO/NO(sub x) ratio of 0.02 was found to have a significant impact on the global budgets of HO(sub x) (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation.

  4. Sources of atmospheric aerosol from long-term measurements (5 years) of chemical composition in Athens, Greece.

    PubMed

    Paraskevopoulou, D; Liakakou, E; Gerasopoulos, E; Mihalopoulos, N

    2015-09-15

    To identify the sources of aerosols in Greater Athens Area (GAA), a total of 1510 daily samples of fine (PM 2.5) and coarse (PM 10-2,5) aerosols were collected at a suburban site (Penteli), during a five year period (May 2008-April 2013) corresponding to the period before and during the financial crisis. In addition, aerosol sampling was also conducted in parallel at an urban site (Thissio), during specific, short-term campaigns during all seasons. In all these samples mass and chemical composition measurements were performed, the latest only at the fine fraction. Particulate organic matter (POM) and ionic masses (IM) are the main contributors of aerosol mass, equally contributing by accounting for about 24% of the fine aerosol mass. In the IM, nss-SO4(-2) is the prevailing specie followed by NO3(-) and NH4(+) and shows a decreasing trend during the 2008-2013 period similar to that observed for PM masses. The contribution of water in fine aerosol is equally significant (21 ± 2%), while during dust transport, the contribution of dust increases from 7 ± 2% to 31 ± 9%. Source apportionment (PCA and PMF) and mass closure exercises identified the presence of six sources of fine aerosols: secondary photochemistry, primary combustion, soil, biomass burning, sea salt and traffic. Finally, from winter 2012 to winter 2013 the contribution of POM to the urban aerosol mass is increased by almost 30%, reflecting the impact of wood combustion (dominant fuel for domestic heating) to air quality in Athens, which massively started in winter 2013.

  5. Sources of atmospheric aerosol from long-term measurements (5 years) of chemical composition in Athens, Greece.

    PubMed

    Paraskevopoulou, D; Liakakou, E; Gerasopoulos, E; Mihalopoulos, N

    2015-09-15

    To identify the sources of aerosols in Greater Athens Area (GAA), a total of 1510 daily samples of fine (PM 2.5) and coarse (PM 10-2,5) aerosols were collected at a suburban site (Penteli), during a five year period (May 2008-April 2013) corresponding to the period before and during the financial crisis. In addition, aerosol sampling was also conducted in parallel at an urban site (Thissio), during specific, short-term campaigns during all seasons. In all these samples mass and chemical composition measurements were performed, the latest only at the fine fraction. Particulate organic matter (POM) and ionic masses (IM) are the main contributors of aerosol mass, equally contributing by accounting for about 24% of the fine aerosol mass. In the IM, nss-SO4(-2) is the prevailing specie followed by NO3(-) and NH4(+) and shows a decreasing trend during the 2008-2013 period similar to that observed for PM masses. The contribution of water in fine aerosol is equally significant (21 ± 2%), while during dust transport, the contribution of dust increases from 7 ± 2% to 31 ± 9%. Source apportionment (PCA and PMF) and mass closure exercises identified the presence of six sources of fine aerosols: secondary photochemistry, primary combustion, soil, biomass burning, sea salt and traffic. Finally, from winter 2012 to winter 2013 the contribution of POM to the urban aerosol mass is increased by almost 30%, reflecting the impact of wood combustion (dominant fuel for domestic heating) to air quality in Athens, which massively started in winter 2013. PMID:25958364

  6. Characterization of chemical agent transport in paints.

    PubMed

    Willis, Matthew P; Gordon, Wesley; Lalain, Teri; Mantooth, Brent

    2013-09-15

    A combination of vacuum-based vapor emission measurements with a mass transport model was employed to determine the interaction of chemical warfare agents with various materials, including transport parameters of agents in paints. Accurate determination of mass transport parameters enables the simulation of the chemical agent distribution in a material for decontaminant performance modeling. The evaluation was performed with the chemical warfare agents bis(2-chloroethyl) sulfide (distilled mustard, known as the chemical warfare blister agent HD) and O-ethyl S-[2-(diisopropylamino)ethyl] methylphosphonothioate (VX), an organophosphate nerve agent, deposited on to two different types of polyurethane paint coatings. The results demonstrated alignment between the experimentally measured vapor emission flux and the predicted vapor flux. Mass transport modeling demonstrated rapid transport of VX into the coatings; VX penetrated through the aliphatic polyurethane-based coating (100 μm) within approximately 107 min. By comparison, while HD was more soluble in the coatings, the penetration depth in the coatings was approximately 2× lower than VX. Applications of mass transport parameters include the ability to predict agent uptake, and subsequent long-term vapor emission or contact transfer where the agent could present exposure risks. Additionally, these parameters and model enable the ability to perform decontamination modeling to predict how decontaminants remove agent from these materials.

  7. Biokinetics and dosimetry of inhaled Cm aerosols in beagles: effect of aerosol chemical form.

    PubMed

    Guilmette, R A; Kanapilly, G M

    1988-12-01

    This study was designed to provide tissue distribution data of 244Cm that was inhaled by beagle dogs. Two chemical forms that were presumed to bracket the solubility of pure Cm compounds in vivo were used: 244Cm2O3 (oxide) and 244Cm(NO3)3 (nitrate). Adult dogs of both sexes received a single brief pernasal exposure to either a monodisperse aerosol of 244Cm2O3 (1.4 micron activity median aerodynamic diameter, AMAD, and 1.16 geometric standard deviation, sigma g) or a polydisperse aerosol of 244Cm(NO3)3 (1.1 micron AMAD, 1.74 sigma g). The resulting initial pulmonary burdens (IPB) were 1.5 and 1.7 kBq kg-1 body mass for the oxide and nitrate groups, respectively. The tissue distribution data obtained from the dogs that were serially sacrificed from 4 h to 2 y after exposure showed that both chemical forms were very soluble in vivo. For the oxide group, 78% IPB was cleared from the lung with a T 1/2 of 7.6 d, whereas for the nitrate group, 42% IPB cleared with a T 1/2 of 0.6 d. The lung retention for each group was described by three-component exponential functions. Most of the Cm that cleared the lung was redeposited in the liver (37% IPB) and skeleton (27% IPB), with lesser amounts in the muscle, fat and connective tissue (3.5% IPB) and kidney (approximately 2% IPB). The only significant difference noted in the biokinetics of Cm for the two exposure groups was a more rapid translocation of Cm from the lung to liver and bone during the first 10-20 d after exposure to the nitrate compared to the oxide chemical form. Extrapolation of these data to obtain estimates of committed dose equivalents for man indicate substantial agreement with the limits for occupational exposure specified by ICRP 30 (1979). PMID:3198400

  8. Monitoring and tracking the trans-Pacific transport of aerosols using multi-satellite aerosol optical depth retrievals

    NASA Astrophysics Data System (ADS)

    Naeger, A. R.; Gupta, P.; Zavodsky, B.; McGrath, K. M.

    2015-10-01

    The primary goal of this study was to generate a near-real time (NRT) aerosol optical depth (AOD) product capable of providing a comprehensive understanding of the aerosol spatial distribution over the Pacific Ocean in order to better monitor and track the trans-Pacific transport of aerosols. Therefore, we developed a NRT product that takes advantage of observations from both low-earth orbiting and geostationary satellites. In particular, we utilize AOD products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Suomi National Polar-orbiting Partnership (NPP) Visible Infrared Imaging Radiometer Suite (VIIRS) satellites. Then, we combine these AOD products with our own retrieval algorithms developed for the NOAA Geostationary Operational Environmental Satellite (GOES-15) and Japan Meteorological Agency (JMA) Multi-functional Transport Satellite (MTSAT-2) to generate a NRT daily AOD composite product. We present examples of the daily AOD composite product for a case study of trans-Pacific transport of Asian pollution and dust aerosols in mid-March 2014. Overall, the new product successfully tracks this aerosol plume during its trans-Pacific transport to the west coast of North America. However, we identify several areas across the domain of interest from Asia to North America where the new product can encounter significant uncertainties due to the inclusion of the geostationary AOD retrievals. The uncertainties associated with geostationary AOD retrievals are expected to be minimized after the successful launch of the next-generation advanced NOAA GOES-R and recently launched JMA Himawari satellites. Observations from these advanced satellites will ultimately provide an enhanced understanding of the spatial and temporal distribution of aerosols over the Pacific.

  9. Chemical characterization and physico-chemical properties of aerosols at Villum Research Station, Greenland during spring 2015

    NASA Astrophysics Data System (ADS)

    Glasius, M.; Iversen, L. S.; Svendsen, S. B.; Hansen, A. M. K.; Nielsen, I. E.; Nøjgaard, J. K.; Zhang, H.; Goldstein, A. H.; Skov, H.; Massling, A.; Bilde, M.

    2015-12-01

    The effects of aerosols on the radiation balance and climate are of special concern in Arctic areas, which have experienced warming at twice the rate of the global average. As future scenarios include increased emissions of air pollution, including sulfate aerosols, from ship traffic and oil exploration in the Arctic, there is an urgent need to obtain the fundamental scientific knowledge to accurately assess the consequences of pollutants to environment and climate. In this work, we studied the chemistry of aerosols at the new Villum Research Station (81°36' N, 16°40' W) in north-east Greenland during the "inauguration campaign" in spring 2015. The chemical composition of sub-micrometer Arctic aerosols was investigated using a Soot Particle Time-of-Flight Aerosol Mass Spectrometer (SP-ToF-AMS). Aerosol samples were also collected on filters using both a high-volume sampler and a low-volume sampler equipped with a denuder for organic gases. Chemical analyses of filter samples include determination of inorganic anions and cations using ion-chromatography, and analysis of carboxylic acids and organosulfates of anthropogenic and biogenic origin using ultrahigh-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UHPLC-QTOF-MS). Previous studies found that organosulfates constitute a surprisingly high fraction of organic aerosols during the Arctic Haze period in winter and spring. Investigation of organic molecular tracers provides useful information on aerosol sources and atmospheric processes. The physico-chemical properties of Arctic aerosols are also under investigation. These measurements include particle number size distribution, water activity and surface tension of aerosol samples in order to deduct information on their hygroscopicity and cloud-forming potential. The results of this study are relevant to understanding aerosol sources and processes as well as climate effects in the Arctic, especially during the Arctic haze

  10. Molecular corridors and parameterizations of volatility in the chemical evolution of organic aerosols

    NASA Astrophysics Data System (ADS)

    Li, Ying; Pöschl, Ulrich; Shiraiwa, Manabu

    2016-03-01

    The formation and aging of organic aerosols (OA) proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the saturation mass concentration of organic compounds containing oxygen, nitrogen, and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less-oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle-phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.

  11. Chemical composition of atmospheric aerosols between Moscow and Vladivostok

    NASA Astrophysics Data System (ADS)

    Kuokka, S.; Teinilä, K.; Saarnio, K.; Aurela, M.; Sillanpää, M.; Hillamo, R.; Kerminen, V.-M.; Vartiainen, E.; Kulmala, M.; Skorokhod, A. I.; Elansky, N. F.; Belikov, I. B.

    2007-05-01

    The TROICA-9 expedition (Trans-Siberian Observations Into the Chemistry of the Atmosphere) was carried out at the Trans-Siberian railway between Moscow and Vladivostok in October 2005. Measurements of aerosol physical and chemical properties were made from an observatory carriage connected to a passenger train. Black carbon (BC) concentrations in fine particles (PM2.5, aerodynamic diameter <2.5 μm) were measured with an aethalometer using a five-minute time resolution. Concentrations of inorganic ions and some organic compounds (Cl-, NO3-, SO42-, Na+, NH4+, K+, Ca2+, Mg2+, oxalate and methane sulphonate) were measured continuously by using an on-line system with a 15-min time resolution. In addition, particle volume size distributions were determined for particles in the diameter range 3-850 nm using a 10-min. time resolution. The continuous measurements were completed with 24-h. PM2.5 filter samples which were stored in a refrigerator and later analyzed in chemical laboratory. The analyses included mass concentrations of PM2.5, ions, monosaccharide anhydrides (levoglucosan, galactosan and mannosan) and trace elements (Al, As, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb, Sb, V and Zn). The mass concentrations of PM2.5 varied in the range of 4.3-34.8 μg m-3 with an average of 21.6 μg m-3. Fine particle mass consisted mainly of BC (average 27.6%), SO42- (13.0%), NH4+ (4.1%), and NO3- (1.4%). One of the major constituents was obviously also organic carbon which was not determined. The contribution of BC was high compared with other studies made in Europe and Asia. High concentrations of ions, BC and particle volume were observed between Moscow and roughly 4000 km east of it, as well as close to Vladivostok, primarily due to local anthropogenic sources. In the natural background area between 4000 and 7200 km distance from Moscow, observed concentrations were low, even though there were local particle sources, such as forest fires, that increased occasionally concentrations. The

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

    NASA Astrophysics Data System (ADS)

    Potter, Lauren E.

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

  13. Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

    NASA Astrophysics Data System (ADS)

    Fast, Jerome D.; Berg, Larry K.; Zhang, Kai; Easter, Richard C.; Ferrare, Richard A.; Hair, Johnathan W.; Hostetler, Chris A.; Liu, Ying; Ortega, Ivan; Sedlacek, Arthur; Shilling, John E.; Shrivastava, Manish; Springston, Stephen R.; Tomlinson, Jason M.; Volkamer, Rainer; Wilson, Jacqueline; Zaveri, Rahul A.; Zelenyuk, Alla

    2016-08-01

    The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two-Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy's Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts, and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surface measurements during July, and 2 days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher-resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser-resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. While a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.

  14. Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

    NASA Technical Reports Server (NTRS)

    da Silva, Arlindo

    2010-01-01

    A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

  15. Effects of aerosol sources and chemical compositions on cloud drop sizes and glaciation temperatures

    NASA Astrophysics Data System (ADS)

    Zipori, Assaf; Rosenfeld, Daniel; Tirosh, Ofir; Teutsch, Nadya; Erel, Yigal

    2015-09-01

    The effect of aerosols on cloud properties, such as its droplet sizes and its glaciation temperatures, depends on their compositions and concentrations. In order to examine these effects, we collected rain samples in northern Israel during five winters (2008-2011 and 2013) and determined their chemical composition, which was later used to identify the aerosols' sources. By combining the chemical data with satellite-retrieved cloud properties, we linked the aerosol types, sources, and concentrations with the cloud glaciation temperatures (Tg). The presence of dust increased Tg from -26°C to -12°C already at relatively low dust concentrations. This result is in agreement with the conventional wisdom that desert dust serves as good ice nuclei (INs). With higher dust concentrations, Tg saturated at -12°C, even though cloud droplet sizes decreased as a result of the cloud condensation nucleating (CCN) activity of the dust. Marine air masses also encouraged freezing, but in this case, freezing was enhanced by the larger cloud droplet sizes in the air masses (caused by low CCN concentrations) and not by IN concentrations or by aerosol type. An increased fraction of anthropogenic aerosols in marine air masses caused a decrease in Tg, indicating that these aerosols served as poor IN. Anthropogenic aerosols reduced cloud droplet sizes, which further decreased Tg. Our results could be useful in climate models for aerosol-cloud interactions, as we investigated the effects of aerosols of different sources on cloud properties. Such parameterization can simplify these models substantially.

  16. Drug Transport and Pharmacokinetics for Chemical Engineers

    ERIC Educational Resources Information Center

    Simon, Laurent; Kanneganti, Kumud; Kim, Kwang Seok

    2010-01-01

    Experiments in continuous-stirred vessels were proposed to introduce methods in pharmacokinetics and drug transport to chemical engineering students. The activities can be incorporated into the curriculum to illustrate fundamentals learned in the classroom. An appreciation for the role of pharmacokinetics in drug discovery will also be gained…

  17. Methodology for the passive detection and discrimination of chemical and biological aerosols

    NASA Astrophysics Data System (ADS)

    Marinelli, William J.; Shokhirev, Kirill N.; Konno, Daisei; Rossi, David C.; Richardson, Martin

    2013-05-01

    The standoff detection and discrimination of aerosolized biological and chemical agents has traditionally been addressed through LIDAR approaches, but sensor systems using these methods have yet to be deployed. We discuss the development and testing of an approach to detect these aerosols using the deployed base of passive infrared hyperspectral sensors used for chemical vapor detection. The detection of aerosols requires the inclusion of down welling sky and up welling ground radiation in the description of the radiative transfer process. The wavelength and size dependent ratio of absorption to scattering provides much of the discrimination capability. The approach to the detection of aerosols utilizes much of the same phenomenology employed in vapor detection; however, the sensor system must acquire information on non-line-of-sight sources of radiation contributing to the scattering process. We describe the general methodology developed to detect chemical or biological aerosols, including justifications for the simplifying assumptions that enable the development of a real-time sensor system. Mie scattering calculations, aerosol size distribution dependence, and the angular dependence of the scattering on the aerosol signature will be discussed. This methodology will then be applied to two test cases: the ground level release of a biological aerosol (BG) and a nonbiological confuser (kaolin clay) as well as the debris field resulting from the intercept of a cruise missile carrying a thickened VX warhead. A field measurement, conducted at the Utah Test and Training Range will be used to illustrate the issues associated with the use of the method.

  18. Long-term Measurements of Submicrometer Aerosol Chemistry at the Southern Great Plains (SGP) Using an Aerosol Chemical Speciation Monitor (ACSM)

    SciTech Connect

    Parworth, Caroline; Fast, Jerome D.; Mei, Fan; Shippert, Timothy R.; Sivaraman, Chitra; Tilp, Alison; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the U.S. Department of Energy’s Southern Great Plains (SGP) site are discussed. Over the period of 19 months (Nov. 20, 2010 – June 2012) highly time resolved (~30 min.) NR-PM1 data was recorded. Using this dataset the value-added product (VAP) of deriving organic aerosol components (OACOMP) is introduced. With this VAP, multivariate analysis of the measured organic mass spectral matrix can be performed on long term data to return organic aerosol (OA) factors that are associated with distinct sources, evolution processes, and physiochemical properties. Three factors were obtained from this VAP including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when nitrate increased due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations showed little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increased and were mainly associated with local fires. Isoprene and carbon monoxide emission rates were computed by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) to represent the spatial distribution of biogenic and anthropogenic sources, respectively. From this model there is evidence to support that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  19. Monitoring and tracking the trans-Pacific transport of aerosols using multi-satellite aerosol optical depth composites

    NASA Astrophysics Data System (ADS)

    Naeger, Aaron R.; Gupta, Pawan; Zavodsky, Bradley T.; McGrath, Kevin M.

    2016-06-01

    The primary goal of this study was to generate a near-real time (NRT) aerosol optical depth (AOD) product capable of providing a comprehensive understanding of the aerosol spatial distribution over the Pacific Ocean, in order to better monitor and track the trans-Pacific transport of aerosols. Therefore, we developed a NRT product that takes advantage of observations from both low-earth orbiting and geostationary satellites. In particular, we utilize AOD products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Suomi National Polar-orbiting Partnership (NPP) Visible Infrared Imaging Radiometer Suite (VIIRS) satellites. Then, we combine these AOD products with our own retrieval algorithms developed for the NOAA Geostationary Operational Environmental Satellite (GOES-15) and Japan Meteorological Agency (JMA) Multi-functional Transport Satellite (MTSAT-2) to generate a NRT daily AOD composite product. We present examples of the daily AOD composite product for a case study of trans-Pacific transport of Asian pollution and dust aerosols in mid-March 2014. Overall, the new product successfully tracks this aerosol plume during its trans-Pacific transport to the west coast of North America as the frequent geostationary observations lead to a greater coverage of cloud-free AOD retrievals equatorward of about 35° N, while the polar-orbiting satellites provide a greater coverage of AOD poleward of 35° N. However, we note several areas across the domain of interest from Asia to North America where the GOES-15 and MTSAT-2 retrieval algorithms can introduce significant uncertainties into the new product.

  20. Direct aerosol chemical composition measurements to evaluate the physicochemical differences between controlled sea spray aerosol generation schemes

    NASA Astrophysics Data System (ADS)

    Collins, D. B.; Zhao, D. F.; Ruppel, M. J.; Laskina, O.; Grandquist, J. R.; Modini, R. L.; Stokes, M. D.; Russell, L. M.; Bertram, T. H.; Grassian, V. H.; Deane, G. B.; Prather, K. A.

    2014-11-01

    Controlled laboratory studies of the physical and chemical properties of sea spray aerosol (SSA) must be under-pinned by a physically and chemically accurate representation of the bubble-mediated production of nascent SSA particles. Bubble bursting is sensitive to the physico-chemical properties of seawater. For a sample of seawater, any important differences in the SSA production mechanism are projected into the composition of the aerosol particles produced. Using direct chemical measurements of SSA at the single-particle level, this study presents an intercomparison of three laboratory-based, bubble-mediated SSA production schemes: gas forced through submerged sintered glass filters ("frits"), a pulsed plunging-waterfall apparatus, and breaking waves in a wave channel filled with natural seawater. The size-resolved chemical composition of SSA particles produced by breaking waves is more similar to particles produced by the plunging waterfall than those produced by sintered glass filters. Aerosol generated by disintegrating foam produced by sintered glass filters contained a larger fraction of organic-enriched particles and a different size-resolved elemental composition, especially in the 0.8-2 μm dry diameter range. Interestingly, chemical differences between the methods only emerged when the particles were chemically analyzed at the single-particle level as a function of size; averaging the elemental composition of all particles across all sizes masked the differences between the SSA samples. When dried, SSA generated by the sintered glass filters had the highest fraction of particles with spherical morphology compared to the more cubic structure expected for pure NaCl particles produced when the particle contains relatively little organic carbon. In addition to an intercomparison of three SSA production methods, the role of the episodic or "pulsed" nature of the waterfall method on SSA composition was under-taken. In organic-enriched seawater, the continuous

  1. Chemical and size effects of hygroscopic aerosols on light scattering coefficients

    NASA Astrophysics Data System (ADS)

    Tang, Ignatius N.

    1996-08-01

    The extensive thermodynamic and optical properties recently reported [Tang and Munkelwitz, 1994a] for sulfate and nitrate solution droplets are incorporated into a visibility model for computing light scattering by hygroscopic aerosols. The following aerosol systems are considered: NH4HSO4, (NH4)2SO4, (NH4)3H(SO4), NaHSO4, Na2SO4, NH4NO3, and NaNO3. In addition, H2SO4 and NaCl are included to represent freshly formed sulfate and background sea-salt aerosols, respectively. Scattering coefficients, based on 1 μg dry salt per cubic meter of air, are calculated as a function of relative humidity for aerosols of various chemical compositions and lognormal size distributions. For a given size distribution the light scattered by aerosol particles per unit dry-salt mass concentration is only weakly dependent on chemical constituents of the hygroscopic sulfate and nitrate aerosols. Sulfuric acid and sodium chloride aerosols, however, are exceptions and scatter light more efficiently than all other inorganic salt aerosols considered in this study. Both internal and external mixtures exhibit similar light-scattering properties. Thus for common sulfate and nitrate aerosols, since the chemical effect is outweighed by the size effect, it follows that observed light scattering by the ambient aerosol can be approximated, within practical measurement uncertainties, by assuming the aerosol being an external mixture. This has a definite advantage for either visibility degradation or climatic impact modeling calculations, because relevant data are now available for external mixtures but only very scarce for internal mixtures.

  2. Biosensor discovery of thyroxine transport disrupting chemicals

    SciTech Connect

    Marchesini, Gerardo R. Meimaridou, Anastasia; Haasnoot, Willem; Meulenberg, Eline; Albertus, Faywell; Mizuguchi, Mineyuki; Takeuchi, Makoto; Irth, Hubertus; Murk, Albertinka J.

    2008-10-01

    Ubiquitous chemicals may interfere with the thyroid system that is essential in the development and physiology of vertebrates. We applied a surface plasmon resonance (SPR) biosensor-based screening method for the fast screening of chemicals with thyroxine (T4) transport disrupting activity. Two inhibition assays using the main thyroid hormone transport proteins, T4 binding globulin (TBG) and transthyretin (TTR), in combination with a T4-coated biosensor chip were optimized and automated for screening chemical libraries. The transport protein-based biosensor assays were rapid, high throughput and bioeffect-related. A library of 62 chemicals including the natural hormones, polychlorinated biphenyls (PCBs), polybrominated diphenylethers (PBDEs) and metabolites, halogenated bisphenol A (BPA), halogenated phenols, pharmaceuticals, pesticides and other potential environmentally relevant chemicals was tested with the two assays. We discovered ten new active compounds with moderate to high affinity for TBG with the TBG assay. Strikingly, the most potent binding was observed with hydroxylated metabolites of the brominated diphenyl ethers (BDEs) BDE 47, BDE 49 and BDE 99, that are commonly found in human plasma. The TTR assay confirmed the activity of previously identified hydroxylated metabolites of PCBs and PBDEs, halogenated BPA and genistein. These results show that the hydroxylated metabolites of the ubiquitous PBDEs not only target the T4 transport at the TTR level, but also, and to a great extent, at the TBG level where most of the T4 in humans is circulating. The optimized SPR biosensor-based transport protein assay is a suitable method for high throughput screening of large libraries for potential thyroid hormone disrupting compounds.

  3. Dispersion and transport of tropospheric aerosol and pollutants in the Western Mediterranean: the role of the Po Valley under different transport regimes

    NASA Astrophysics Data System (ADS)

    Bucci, Silvia; Fierli, Federico; Ravetta, François; Raut, Jean Christophe; Cristofanelli, Paolo; Decesari, Stefano; Diliberto, Luca; Größ, Johannes; Pap, Ines; Weinhold, Kay; Wiedensohler, Alfred; Cairo, Francesco

    2016-04-01

    This work reports a characterization of the vertical variability of tropospheric aerosol and gaseous pollutants, over the western Mediterranean, during the 2012 summer season. In particular, we investigate the role of the Po Valley region as a receptor and emissive region of both natural and anthropogenic aerosol. The observational analysis, based on a comprehensive database of meteorological, aerosol and chemical measurements, is integrated with a model analysis using the Lagrangian transport system FLEXPART combined with emission databases, and WRF-Chem, the Weather Research and Forecasting (WRF) model coupled with Chemistry. Observations have been performed in the framework of the Supersito project by Regional Agency of Prevention and Environment of the Emilia Romagna region (ARPA-ER, Ital), the TRAQA campaign (TRAnsport et Qualité de l'Air au dessus du bassin Méditerranéen) performed in the ChArMEx (Chemistry-Aerosol Mediterranean Experiment) project, and the european project PEGASOS (Pan-European Gas-AeroSOl-climate interaction Study). An alternation between different transport regimes characterized the 2012 summer, resulting in a large variability of aerosol and pollution at different time and spatial scales. Particles of different nature have been discriminated basing on optical properties retrieved from lidar data and supported by in-situ observations and transport analysis. Results show that, during the analysed season, aerosol in the Po Valley was mainly confined below 2000 m and dominated (50% of detections) by spherical particles. Two events of dust advection from northern Africa were identified (19th-21th June and 29th June-2nd July), with intrusion and mixing with local pollution in the PBL and a non-negligible occurrence (~7%) of dust at the ground. Frequent events (22% of occurrence) of non-spherical particles resuspension, likely due to uplift of mineral soil particles, were observed from the ground to 2000 m during afternoon and evening. In the

  4. Size-segregated aerosol chemical composition at a boreal site in southern Finland, during the QUEST project

    NASA Astrophysics Data System (ADS)

    Cavalli, F.; Facchini, M. C.; Decesari, S.; Emblico, L.; Mircea, M.; Jensen, N. R.; Fuzzi, S.

    2006-03-01

    Size-segregated aerosol samples were collected during the QUEST field campaign at Hyytiää;, a boreal forest site in Southern Finland, during spring 2003. Aerosol samples were selectively collected during both particle formation events and periods in which no particle formation occurred.

    A comprehensive characterisation of the aerosol chemical properties (water-soluble inorganic and organic fraction) and an analysis of the relevant meteorological parameters revealed how aerosol chemistry and meteorology combine to determine a favorable "environment" for new particle formation. The results indicated that all events, typically favored during northerly air mass advection, were background aerosols (total mass concentrations range between 1.97 and 4.31 µg m-3), with an increasingly pronounced marine character as the northerly air flow arrived progressively from the west and, in contrast, with a moderate SO2-pollution influence as the air arrived from more easterly directions. Conversely, the non-event aerosol, transported from the south, exhibited the chemical features of European continental sites, with a marked increase in the concentrations of all major anthropogenic aerosol constituents. The higher non-event mass concentration (total mass concentrations range between 6.88 and 16.30 µg m-3) and, thus, a larger surface area, tended to suppress new particle formation, more efficiently depleting potential gaseous precursors for nucleation. The analysis of water-soluble organic compounds showed that clean nucleation episodes were dominated by aliphatic biogenic species, while non-events were characterised by a large abundance of anthropogenic oxygenated species. Interestingly, a significant content of α-pinene photo-oxidation products was observed in the events aerosol, accounting for, on average, 72% of their WSOC; while only moderate amounts of these species were found in the non-event aerosol. If the organic vapors condensing onto

  5. Size-segregated aerosol chemical composition at a boreal site in southern Finland, during the QUEST project

    NASA Astrophysics Data System (ADS)

    Cavalli, F.; Facchini, M. C.; Decesari, S.; Emblico, L.; Mircea, M.; Jensen, N. R.; Fuzzi, S.

    2005-09-01

    Size-segregated aerosol samples were collected during the QUEST field campaign at Hyytiälä, a boreal forest site in Southern Finland, during spring 2003. Aerosol samples were selectively collected during both particle formation events and periods in which no particle formation occurred. A comprehensive characterisation of the aerosol chemical properties (water-soluble inorganic and organic fraction) and an analysis of the relevant meteorological parameters revealed how aerosol chemistry and meteorology combine to determine a favorable "environment" for new particle formation. The results indicated that all events, typically favored during northerly air mass advection, were background aerosols (total mass concentrations range between 1.97 and 4.31 μg m-3), with an increasingly pronounced marine character as the northerly air flow arrived progressively from the west and, in contrast, with a moderate SO2-pollution influence as the air arrived from more easterly directions. Conversely, the non-event aerosol, transported from the south, exhibited the chemical features of European continental sites, with a marked increase in the concentrations of all major anthropogenic aerosol constituents. The higher non-event mass concentration (total mass concentrations range between 6.88 and 16.30 μg m-3) and, thus, a larger surface area, tended to suppress new particle formation, more efficiently depleting potential gaseous precursors for nucleation. The analysis of water-soluble organic compounds showed that clean nucleation episodes were dominated by aliphatic biogenic species, while non-events were characterised by a large abundance of anthropogenic oxygenated species. Interestingly, a significant content of α-pinene photo-oxidation products was observed in the events aerosol, accounting for, on average, 72% of their WSOC; while only moderate amounts of these species were found in the non-event aerosol. If the organic vapors condensing onto accumulation mode particles are

  6. Chemical Characterization of Submicron Aerosol Particles in São Paulo, Brazil

    NASA Astrophysics Data System (ADS)

    Ferreira De Brito, J.; Rizzo, L. V.; Godoy, J.; Godoy, M. L.; de Assunção, J. V.; Alves, N. D.; Artaxo, P.

    2013-12-01

    Megacities, large urban conglomerates with a population of 10 million or more inhabitants, are increasingly receiving attention as strong pollution hotspots with significant global impact. The emissions from such large centers in both the developed and developing parts of the world are strongly impacted by the transportation sector. The São Paulo Metropolitan Area (SPMA), located in the Southeast of Brazil, is a megacity with a population of 18 million people and 7 million vehicles, many of which fuelled by a considerably amount of anhydrous ethanol. Such fleet is considered a unique case of large scale biofuel usage worldwide. Despite the large impact on human health and atmospheric chemistry/dynamics, many uncertainties are found in terms of gas and particulate matter emissions from vehicles and their atmospheric reactivity, e.g. secondary organic aerosol formation. In order to better understand aerosol life cycle on such environment, a suite of instruments for gas and particulate matter characterization has been deployed in two sampling sites within the SPMA, including an Aerosol Chemical Speciation Monitor (ACSM). The instrumentation was deployed at the rooftop of a 45m high building in the University of São Paulo during winter/spring 2012. The site is located roughly 6km downwind of the city center with little influence from local sources. The second site is located in a downtown area, sampling at the top floor of the Public Health Faculty, approximately 10m above ground. The instrumentation was deployed at the Downtown site during summer/fall 2013. The average non-refractory submicron aerosol concentration at the University site was 6.7 μg m-3, being organics the most abundant specie (70%), followed by NO3 (12%), NH4 (8%), SO4 (8%) and Chl (2%). At the Downtown site, average aerosol concentration was 15.1 μg m-3, with Organics composing 65% of the mass, followed by NH4 (12%), NO3 (11%), SO4 (11%) and Chl (1%). The analysis of specific fragmentation

  7. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    NASA Astrophysics Data System (ADS)

    Parworth, Caroline; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Tilp, Alison; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ∼30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations of the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  8. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    SciTech Connect

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations of the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  9. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    DOE PAGES

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

  10. Metals and Rare Earth Elements in polar aerosol as specific markers of natural and anthropogenic aerosol sources areas and atmospheric transport processes

    NASA Astrophysics Data System (ADS)

    Giardi, Fabio; Becagli, Silvia; Caiazzo, Laura; Cappelletti, David; Grotti, Marco; Malandrino, Mery; Salzano, Roberto; Severi, Mirko; Traversi, Rita; Udisti, Roberto

    2016-04-01

    Metals and Rare Earth Elements (REEs) in the aerosol have conservative properties from the formation to the deposition and can be useful to identify and quantify their natural and anthropic sources and to study the atmospheric transport processes. In spite of their importance relatively little is known about metals and especially REEs in the Artic atmosphere due to their low concentration in such environment. The present work reports the first attempt to determine and interpret the behaviour of metals and REEs in polar aerosol at high temporal resolution. Daily PM10 samples of arctic atmospheric particulate were collected on Teflon filters, during six spring-summer campaigns, since 2010, in the laboratory of Gruvebadet in Ny Ålesund (78°56' N, 11°56' E, Svalbard Islands, Norway). Chemical analyses were carried out through Inductively Coupled Plasma Mass Spectrometer provided with a desolvation nebulizer inlet system, allowing to reduce isobaric interferences and thus to quantify trace and ultra-trace metals in very low concentration in the Arctic aerosol samples. The results are useful in order to study sources areas, transport processes and depositional effects of natural and anthropic atmospheric particulate reaching the Arctic from southern industrialized areas; moreover, the observed seasonal trends give information about the different impact of natural and anthropic emissions driven by phenomena such as the Arctic Haze and the melting of the snow. In particular Rare Earth Elements (often in the ppt range) can be considered as soil's fingerprints of the particulate source areas and their determination, together with air-mass backtrajectory analysis, allow to identify dust source areas for the arctic mineral aerosol.

  11. Physical and Chemical Characterization of Particles in the Upper Troposphere and Lower Stratosphere: Microanalysis of Aerosol Impactor Samples

    NASA Technical Reports Server (NTRS)

    Sheridan, Patrick J.

    1999-01-01

    Herein is reported activities to support the characterization of the aerosol in the upper troposphere (UT) and lower stratosphere (LS) collected during the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA) missions in 1994. Through a companion proposal, another group was to measure the size distribution of aerosols in the 0.008 to 2 micrometer diameter range and to collect for us impactor samples of particles larger than about 0.02 gm. In the first year, we conducted laboratory studies related to particulate deposition patterns on our collection substrates, and have performed the analysis of many ASHOE/MAESA aerosol samples from 1994 using analytical electron microscopy (AEM). We have been building an "aerosol climatology" with these data that documents the types and relative abundances of particles observed at different latitudes and altitudes. The second year (and non-funded extension periods) saw continued analyses of impactor aerosol samples, including more ASHOE/MAESA samples, some northern hemisphere samples from the NASA Stratospheric Photochemistry Aerosols and Dynamics Expedition (SPADE) program for comparison, and a few aerosol samples from the NASA Stratospheric TRacers of Atmospheric Transport (STRAT) program. A high-resolution field emission microscope was used for the analysis and re-analysis of a number of samples to determine if this instrument was superior in performance to our conventional electron microscope. In addition, some basic laboratory studies were conducted to determine the minimum detectable and analyzable particle size for different types of aerosols. In all, 61 aerosol samples were analyzed, with a total of over 30,000 individual particle analyses. In all analyzed samples, sulfate particles comprised the major aerosol number fraction. It must be stressed that particles composed of more than one species, for example sulfate and organic carbon, were classified

  12. Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in downtown Atlanta, Georgia

    NASA Astrophysics Data System (ADS)

    Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

    2014-07-01

    Currently, there are a limited number of field studies that evaluate the long-term performance of the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) against established monitoring networks. In this study, we present seasonal intercomparisons of the ACSM with collocated fine aerosol (PM2.5) measurements at the Southeastern Aerosol Research and Characterization (SEARCH) Jefferson Street (JST) site near downtown Atlanta, GA, during 2011-2012. Intercomparison of two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21) indicating that ACSM instruments are capable of stable and reproducible operation. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the filter-adjusted continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Correlations of the ACSM NR-PM1 (non-refractory particulate matter with aerodynamic diameter less than or equal to 1 μm) plus elemental carbon (EC) with tapered element oscillating microbalance (TEOM) PM2.5 and Federal Reference Method (FRM) PM1 mass are strong with r2 > 0.7 and r2 > 0.8, respectively. Discrepancies might be attributed to evaporative losses of semi-volatile species from the filter measurements used to adjust the collocated continuous measurements. This suggests that adjusting the ambient aerosol continuous measurements with results from filter analysis introduced additional bias to the measurements. We also recommend to calibrate the ambient aerosol monitoring instruments using aerosol standards rather than gas-phase standards. The fitting approach for ACSM relative ionization for sulfate was shown to improve the comparisons between ACSM and collocated measurements in the absence of calibrated values, suggesting the importance of adding sulfate calibration into the ACSM calibration routine.

  13. Chemical characterization of atmospheric aerosol in urban areas with different anthropic impact.

    NASA Astrophysics Data System (ADS)

    Fattori, I.; Bellandi, S.; Innocenti, M.; Largiuni, O.; Lucarelli, F.; Mannini, A.; Udisti, R.

    2003-04-01

    Several sampling campaigns, in the last four years, were carried out in the Florence (Italy) city and surrounding areas in order to identify main aerosol contributions and their changes in time and in different meteorological conditions. The sampling sites were located in the city centre (60 m a.s.l.), in a suburban site (150 m a.s.l.) at the altitude of the usual thermal inversion level and in a hilly and woody site (750 m a.s.l.), as a reference for low anthropic inputs. To discriminate between primary sources, mainly related to the coarse fraction, and secondary contributions, dominant in the finest particles, the sampling was performed by a stacked filter unit holding two sequential polycarbonate membrane filters at different porosity (coarse fraction: 8 and 5 um; fine fraction: 1 and 0.45 um - depending on the campaigns). Each membrane filter was analysed for ionic components (by IC), soluble (at pH=2) fraction of selected heavy metals (by GFAAS) and their total content (by PIXE). For the different sites and different dimensional classes, a Principal Component Analysis (PCA) was applied in order to group components coming from common aerosol sources or transport processes. The typical anthropic components (sulphate, nitrate, carboxylic acid, heavy metals such as Pb, V, Cu) dominate the finest fraction collected in the city centre and their contribution decreases as distance and altitude increase. In the highest site, relatively far from direct vehicular emissions, natural contributions (sea spray, crustal and vegetation inputs) were enlightened by the PCA, in both size fractions. A comparison between total heavy metal content (measured by PIXE) and soluble (pH=2) fraction (by GFAAS) allowed evaluating the metal percentage more toxic for the environment. In the finest particles Pb, in spite of the Pb-gasoline reduction, constitutes the main component of the "soluble" metal fraction. Indeed, the Pb is mainly in soluble form (GFAAS/PIXE = 0.8). The effect of wind

  14. Analysis of the Effects of Chemical Composition and Humidity on Visibility using Highly Time Resolved Aerosol Data

    NASA Astrophysics Data System (ADS)

    Lunden, M. M.; Brown, N. J.; Liu, D.; Tonse, S.

    2005-12-01

    Transported aerosols from populated and industrial areas result in regional haze that causes visibility degradation in areas valued for their scenic beauty, such as the National Parks. These areas are designated as Class I Areas in the United States, and there are specific visibility goals put forth to ultimately return these areas to natural conditions. To both understand current conditions and chart progress towards meeting these goals requires measurement of important aerosol species and an understanding of how these different aerosol species affect light attenuation to allow for predictive modeling capabilities. The current investigation seeks to understand if more highly time resolved measurements of chemically speciated particle mass, relative humidity, scattering, and absorption would enable a better estimation of extinction as the relationship between these variables is non-linear. Our particular objective is to explore the contributions of the aerosol species mentioned above to visibility degradation, and the role played by relative humidity. We performed analyses on a data set collected in Central California from the intensive ambient aerosol sampling campaign conducted from 2000 summer-2001 winter1. The data include PM-2.5 mass concentrations of nitrate, sulfate, organic carbon and black carbon aerosol, as well as simultaneous measurements on light scattering, ambient temperature and relative humidity. The dataset is highly time-resolved, allowing the affect of temporal variations of particle chemical composition and meteorological features to be considered. The final results provide response curves that allow calculation of light scattering given aerosol concentrations and relative humidity. Our results are compared with those obtained using formulae suggested for analysis of IMPROVE (a regional haze monitoring network2) data collected under lower temporal resolution to understand the effects of temporal resolution on the characteristics of the

  15. Uncertainties in aerosol direct and indirect effects attributed to uncertainties in convective transport parameterizations

    NASA Astrophysics Data System (ADS)

    Storelvmo, T.

    2012-11-01

    Deep convection is an important transport mechanism for aerosol particles, allowing them to be lifted to levels where they are subject to long-range transport from source regions to remote regions. The sensitivity of regional aerosol effects to the rate of entrainment in deep moist convection has been explored in a global modeling framework, and found to be crucial for the radiative balance both at the surface and at the top of the atmosphere. The fact that regions where deep convection is frequent often coincide with regions of particularly high black carbon emissions is found to be an important factor in understanding this sensitivity to entrainment. More entrainment leads to shallower convective plumes and less aerosol transport from the boundary layer to the upper troposphere in source regions. As a result, boundary layer aerosol concentrations are increased in source regions, while upper tropospheric aerosol concentrations are reduced globally. This generally leads to stronger aerosol effects in polluted regions and weaker aerosol effects in remote regions. Because black carbon particles have the ability to absorb solar radiation, reducing their concentration leads to more solar radiation reflected back to space, especially over bright surfaces. Conversely, at the surface more entrainment means more downwelling shortwave radiation everywhere but in source regions. Regions that experience increased aerosol concentrations in the boundary layer in response to increased entrainment observed a stronger aerosol indirect effect, while the opposite was true everywhere else. This study highlights that the relative strengths of the aerosol direct and indirect effects in clean versus polluted regions depend crucially on the rate of entrainment in deep convective clouds, a process that is presently not well understood and quantified.

  16. The chemical evolution & physical properties of organic aerosol: A molecular structure based approach

    NASA Astrophysics Data System (ADS)

    Wei, Yiyi; Cao, Tingting; Thompson, Jonathan E.

    2012-12-01

    Global climate, atmospheric chemistry, and air quality are affected by tropospheric particulate matter. Recent measurements suggest organic compounds present in this haze comprise roughly half of total aerosol fine mass concentration globally. Unlike the well-constrained processes which result in formation of nitrate or sulfate aerosol, the oxidation of volatile organics in the atmosphere can lead to thousands of stable compounds in the aerosol phase. Development of a tractable framework to consider the chemical and physical evolution of the organic aerosol is crucial for modeling its effect on global climate. Here we show coupling a 3-dimensional coordinate system defined by the molecular descriptors of molecular weight, heteroatom mass, and double bond equivalents (D.B.E.) with high-resolution molecular mass spectrometry is a powerful approach for describing key properties of the organic aerosol. The scheme is conceptually simple, yet maintains sufficient complexity to be compatible with quantitative structure-property relationships (QSPRs) used to predict chemical and physical properties that govern aerosol behavior. From available data, both ambient organic aerosol and laboratory generated organic aerosol frequently occupy the region characterized by <10 D.B.E. <600 M.W. and <200 heteroatom mass. A QSPR analysis conducted illustrates spatial trends within the 3D space for volatility and Henry's law constants for 31,000 organic compounds considered.

  17. Research of transport and deposition of aerosol in human airway replica

    NASA Astrophysics Data System (ADS)

    Lizal, Frantisek; Jedelsky, Jan; Elcner, Jakub; Durdina, Lukas; Halasova, Tereza; Mravec, Filip; Jicha, Miroslav

    2012-04-01

    Growing concern about knowledge of aerosol transport in human lungs is caused by great potential of use of inhaled pharmaceuticals. Second substantial motive for the research is an effort to minimize adverse effects of particular matter emitted by traffic and industry on human health. We created model geometry of human lungs to 7th generation of branching. This model geometry was used for fabrication of two physical models. The first one is made from thin walled transparent silicone and it allows a measurement of velocity and size of aerosol particles by Phase Doppler Anemometry (PDA). The second one is fabricated by stereolithographic method and it is designed for aerosol deposition measurements. We provided a series of measurements of aerosol transport in the transparent model and we ascertained remarkable phenomena linked with lung flow. The results are presented in brief. To gather how this phenomena affects aerosol deposition in human lungs we used the second model and we developed a technique for deposition fraction and deposition efficiency assessment. The results confirmed that non-symmetric and complicated shape of human airways essentially affects transport and deposition of aerosol. The research will now focus on deeper insight in aerosol deposition.

  18. Long-range Transport of Aerosol at a Mountain Site in the Western Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Roberts, Greg; Corrigan, Craig; Ritchie, John; Pont, Véronique; Claeys, Marine; Sciare, Jean; Dulac, François

    2016-04-01

    The Mediterranean Region has been identified as sensitive to changes in the hydrological cycle, which could affect the water resources for millions of people by the turn of the century. However, prior to recent observations, most climate models have not accounted for the impacts of aerosol in this region. Past airborne studies have shown that aerosol sources from Europe and Africa are often transported throughout the lower troposphere; yet, because of their complex vertical distribution, it is a challenge to capture the variability and quantify the contribution of these sources to the radiative budget and precipitation processes. The PAEROS ChArMEx Mountain Experiment (PACMEx) complemented the regional activities by collecting aerosol data from atop a mountain on the island of Corsica, France in order to assess boundary layer / free troposphere atmospheric processes. In June/July 2013, PACMEx instruments were deployed at 2000 m.asl near the center of Corsica, France to complement ground-based aerosol observations at 550 m.asl on the northern peninsula, as well as airborne measurements. Comparisons between the peninsula site and the mountain site show similar general trends in aerosol properties; yet, differences in aerosol properties reveal the myriad transport mechanisms over the Mediterranean Basin. Using aerosol physicochemical data coupled with back trajectory analysis, different sources have been identified including Saharan dust transport, residual dust mixed with sea salt, anthropogenic emissions from Western Europe, and a period of biomass burning from Eastern Europe. Each period exhibits distinct signatures in the aerosol related to transport processes above and below the boundary layer. In addition, the total aerosol concentrations at the mountain site revealed a strong diurnal cycling the between the atmospheric boundary layer and the free troposphere, which is typical of mountain-top observations. PACMEx was funded by the National Science Foundation

  19. Transport and Evolution of Aerosol Above/Below the Boundary Layer in the Western Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Corrigan, C.; Ritchie, J.; Pont, V.; Claeys, M.; Sciare, J.; Mallet, M.; Dulac, F.

    2014-12-01

    The Mediterranean Region has been identified as sensitive to changes in the hydrological cycle, which could affect the water resources for millions of people by the turn of the century. However, prior to recent observations, most climate models have not accounted for the impacts of aerosol in this region. Past airborne studies have shown that aerosol sources from Europe and Africa are often transported throughout the lower troposphere; yet, because of their complex vertical distribution, it is a challenge to capture the variability and quantify the contribution of these sources to the radiative budget and precipitation processes. The PAEROS ChArMEx Mountain Experiment (PACMEx) complemented the regional activities of the ChArMEx/ADRIMED summer 2013 campaign by collecting aerosol data from atop a mountain on the island of Corsica, France in order to assess boundary layer / free troposphere atmospheric processes. In June/July 2013, PACMEx instruments were deployed at 2000 m.asl near the center of Corsica to complement ground-based aerosol observations at 550 m.asl on the northern peninsula, as well as airborne measurements. Comparisons between the peninsula site and the mountain site show similar general trends in aerosol properties; yet, differences in aerosol properties reveal the myriad transport mechanisms over the Mediterranean Basin. Using aerosol physicochemical data coupled with back trajectory analysis, different sources have been identified including Saharan dust transport, residual dust mixed with sea salt, anthropogenic emissions from Western Europe, and a period of biomass burning from Eastern Europe. Each period exhibits distinct signatures in the aerosol related to transport processes above and below the boundary layer. In addition, the total aerosol concentrations at the mountain site revealed a strong diurnal cycling between the atmospheric boundary layer and the free troposphere, which is typical of mountain-top observations. PACMEx was funded by the

  20. Microphysical properties of transported biomass burning aerosols in coastal regions, and application to improving retrievals of aerosol optical depth from SeaWiFS data

    NASA Astrophysics Data System (ADS)

    Sayer, A. M.; Hsu, N. C.; Bettenhausen, C.

    2013-05-01

    Due to the limited measurement capabilities of heritage and current spaceborne passive imaging radiometers, algorithms for the retrieval of aerosol optical depth (AOD) and related quantities must make assumptions relating to aerosol microphysical properties and surface reflectance. Over the ocean, surface reflectance can be relatively well-modelled, but knowledge of aerosol properties can remain elusive. Several field campaigns and many studies have examined the microphysical properties of biomass burning (smoke) aerosol. However, these largely focus on properties over land and near to the source regions. In coastal and open-ocean regions the properties of transported smoke may differ, due to factors such as aerosol aging, wet/dry deposition, and mixture with other aerosol sources (e.g. influence of maritime, pollution, or mineral dust aerosols). Hence, models based on near-source aerosol observations may be less representative of such transported smoke aerosols, introducing additional uncertainty into satellite retrievals of aerosol properties. This study examines case studies of transported smoke from select globally-distributed coastal and island Aerosol Robotic Network (AERONET) sites. These are used to inform improved models for over-ocean transported smoke aerosol for AOD retrievals from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS). These models are used in an updated version of the SeaWiFS Ocean Aerosol Retrieval (SOAR) algorithm, which has been combined with the Deep Blue algorithm over land to create a 13-year (1997-2010) high-quality record of AOD over land and ocean. Applying these algorithms to other sensors will enable the creation of a long-term global climate data record of spectral AOD.

  1. New Measurements of Aerosol Vertical Structure from Space using the NASA Geoscience Laser Altimeter System (GLAS): Applications for Aerosol Transport Models

    NASA Technical Reports Server (NTRS)

    Welton, E. J.; Spinhime, J.; Palm, S.; Hlavka, D.; Hart, W.; Ginoux, P.; Chin, M.; Colarco, P.

    2004-01-01

    In the past, satellite measurements of aerosols have only been possible using passive sensors. Analysis of passive satellite data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth,s climate. However, direct measurement of aerosol vertical distribution has not been possible using only the passive data. Knowledge of aerosol vertical distribution is important to correctly assess the impact of aerosol absorption, for certain atmospheric correction procedures, and to help constrain height profiles in aerosol transport models. On January 12,2003 NASA launched the first satellite-based lidar, the Geoscience Laser Altimeter System (GLAS), onboard the ICESat spacecraft. GLAS is both an altimeter and an atmospheric lidar, and obtains direct measurements of aerosol and cloud heights. Here we show an overview of GLAS, provide an update of its current status, and discuss how GLAS data will be useful for modeling efforts. In particular, a strategy of using GLAS to characterize the height profile of dust plumes over source regions will be presented, along with initial results. Such information can be used to validate and improve output from aerosol transport models. Aerosol height profile comparisons between GLAS and transport models will be shown for regions downwind of aerosol sources. We will also discuss the feasibility of assimilating GLAS profiles into the models in order to improve their output.

  2. New Measurements of Aerosol Vertical Structure from Space Using the NASA Geoscience Laser Altimeter System (GLAS): Applications for Aerosol Transport Models

    NASA Technical Reports Server (NTRS)

    Welton, Ellsworth J.; Ginoux, Paul; Colarco, Peter; Chin, Mian; Spinhirne, James D.; Palm, Steven P.; Hlavka, Dennis; Hart, William

    2003-01-01

    In the past, satellite measurements of aerosols have only been possible using passive sensors. Analysis of passive satellite data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth s climate. However, direct measurement of aerosol vertical distribution has not been possible using only the passive data. Knowledge of aerosol vertical distribution is important to correctly assess the impact of aerosol absorption, for certain atmospheric correction procedures, and to help constrain height profiles in aerosol transport models. On January 12,2003 NASA launched the first satellite-based lidar, the Geoscience Laser Altimeter System (GLAS), onboard the ICESat spacecraft. GLAS is both an altimeter and an atmospheric lidar, and obtains direct measurements of aerosol and cloud heights. Here we show an overview of GLAS, provide an update of its current status, and discuss how GUS data will be useful for modeling efforts. In particular, a strategy of using GLAS to characterize the height profile of dust plumes over source regions will be presented, along with initial results. Such information can be used to validate and improve output from aerosol transport models. Aerosol height profile comparisons between GLAS and transport models will be shown for regions downwind of aerosol sources. We will also discuss the feasibility of assimilating GLAS profiles into the models in order to improve their output,

  3. Chemically driven fluid transport in long microchannels

    NASA Astrophysics Data System (ADS)

    Shen, Mingren; Ye, Fangfu; Liu, Rui; Chen, Ke; Yang, Mingcheng; Ripoll, Marisol

    2016-09-01

    Chemical gradients maintained along surfaces can drive fluid flows by diffusio-osmosis, which become significant at micro- and nano-scales. Here, by means of mesoscopic simulations, we show that a concentration drop across microchannels with periodically inhomogeneous boundary walls can laterally transport fluids over arbitrarily long distances along the microchannel. The driving field is the secondary local chemical gradient parallel to the channel induced by the periodic inhomogeneity of the channel wall. The flow velocity depends on the concentration drop across the channel and the structure and composition of the channel walls, but it is independent of the overall channel length. Our work thus presents new insight into the fluid transport in long microchannels commonly found in nature and is useful for designing novel micro- or nano-fluidic pumps.

  4. Impacts of intercontinental transport of aerosols on human mortality

    NASA Astrophysics Data System (ADS)

    Anenberg, S.; West, J. J.; Schulz, M.; Hemispheric Transport of Air Pollution (HTAP) modelers

    2011-12-01

    Fine particulate matter (PM2.5) is associated with deleterious health impacts, including premature death from cardiopulmonary disease and lung cancer. Although the lifetime of tropospheric PM2.5 is roughly only a week, observations and modeling studies demonstrate that PM2.5 can be transported long distances, impacting air quality and health on regional or global scales. We estimate the mortality impacts of 20% primary PM and PM precursor emission reductions in four major world regions - North America, Europe, East Asia, and South Asia. We use surface concentrations simulated by an ensemble of global chemical transport models convened by the Task Force on Hemispheric Transport of Air Pollution and epidemiologically-derived concentration-response functions to calculate mortality impacts. We estimate that while >90% of avoided premature deaths resulting from these emission reductions occur within the source region, about 9,600 annual avoided deaths occur in other parts of the world. Reducing emissions in Europe avoids the most extra-regional premature deaths, due to large downwind populations in relatively close proximity. Compared with a previous study of 20% ozone precursor emission reductions, we find that the impacts of intercontinental ozone are greater than or equal to those of PM2.5 for most source-receptor pairs, due to the longer atmospheric lifetime and greater transport efficiency for ozone. However, impacts of intercontinental PM2.5 are greater for source-receptor pairs not separated by an ocean, due to the stronger relationship of PM2.5 with mortality. We examine the sensitivity of estimated premature deaths to the shape and magnitude of the concentration-response function, as well as the inter-model variation in simulated PM2.5 responses to emission reductions.

  5. Silicon refinement by chemical vapor transport

    NASA Technical Reports Server (NTRS)

    Olson, J.

    1984-01-01

    Silicon refinement by chemical vapor transport is discussed. The operating characteristics of the purification process, including factors affecting the rate, purification efficiency and photovoltaic quality of the refined silicon were studied. The casting of large alloy plates was accomplished. A larger research scale reactor is characterized, and it is shown that a refined silicon product yields solar cells with near state of the art conversion efficiencies.

  6. Chemically generated convective transport in microfluidic system

    NASA Astrophysics Data System (ADS)

    Shklyaev, Oleg; Das, Sambeeta; Altemose, Alicia; Shum, Henry; Balazs, Anna; Sen, Ayusman

    High precision manipulation of small volumes of fluid, containing suspended micron sized objects like cells, viruses, and large molecules, is one of the main goals in designing modern lab-on-a-chip devices which can find a variety of chemical and biological applications. To transport the cargo toward sensing elements, typical microfluidic devices often use pressure driven flows. Here, we propose to use enzymatic chemical reactions which decompose reagent into less dense products and generate flows that can transport particles. Density variations that lead to flow in the assigned direction are created between the place where reagent is fed into the solution and the location where it is decomposed by enzymes attached to the surface of the microchannel. When the reagent is depleted, the fluid motion stops and particles sediment to the bottom. We demonstrate how the choice of chemicals, leading to specific reaction rates, can affect the transport properties. In particular, we show that the intensity of the fluid flow, the final location of cargo, and the time for cargo delivery are controlled by the amount and type of reagent in the system.

  7. Near Real Time Vertical Profiles of Clouds and Aerosols from the Cloud-Aerosol Transport System (CATS) on the International Space Station

    NASA Astrophysics Data System (ADS)

    Yorks, J. E.; McGill, M. J.; Nowottnick, E. P.

    2015-12-01

    Plumes from hazardous events, such as ash from volcanic eruptions and smoke from wildfires, can have a profound impact on the climate system, human health and the economy. Global aerosol transport models are very useful for tracking hazardous plumes and predicting the transport of these plumes. However aerosol vertical distributions and optical properties are a major weakness of global aerosol transport models, yet a key component of tracking and forecasting smoke and ash. The Cloud-Aerosol Transport System (CATS) is an elastic backscatter lidar designed to provide vertical profiles of clouds and aerosols while also demonstrating new in-space technologies for future Earth Science missions. CATS has been operating on the Japanese Experiment Module - Exposed Facility (JEM-EF) of the International Space Station (ISS) since early February 2015. The ISS orbit provides more comprehensive coverage of the tropics and mid-latitudes than sun-synchronous orbiting sensors, with nearly a three-day repeat cycle. The ISS orbit also provides CATS with excellent coverage over the primary aerosol transport tracks, mid-latitude storm tracks, and tropical convection. Data from CATS is used to derive properties of clouds and aerosols including: layer height, layer thickness, backscatter, optical depth, extinction, and depolarization-based discrimination of particle type. The measurements of atmospheric clouds and aerosols provided by the CATS payload have demonstrated several science benefits. CATS provides near-real-time observations of cloud and aerosol vertical distributions that can be used as inputs to global models. The infrastructure of the ISS allows CATS data to be captured, transmitted, and received at the CATS ground station within several minutes of data collection. The CATS backscatter and vertical feature mask are part of a customized near real time (NRT) product that the CATS processing team produces within 6 hours of collection. The continuous near real time CATS data

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

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

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

  9. INTEX-NA: Intercontinental Chemical Transport Experiment - North America

    NASA Technical Reports Server (NTRS)

    Singh, Hanwant B.; Jacob, D.; Pfister, L.; Hipskind, R. Stephen (Technical Monitor)

    2002-01-01

    INTEX-NA is an integrated atmospheric chemistry field experiment to be performed over North America using the NASA DC-8 and P-3B aircraft as its primary platforms. It seeks to understand the exchange of chemicals and aerosols between continents and the global troposphere. The constituents of interest are ozone and its precursors (hydrocarbons, NOX and HOX), aerosols, and the major greenhouse gases (CO2, CH4, N2O). INTEX-NA will provide the observational database needed to quantify inflow, outflow, and transformations of chemicals over North America. INTEX-NA is to be performed in two phases. Phase A will take place during the period of May-August 2004 and Phase B during March-June 2006. Phase A is in summer when photochemistry is most intense and climatic issues involving aerosols and carbon cycle are most pressing, and Phase B is in spring when Asian transport to North America is at its peak. INTEX-NA will coordinate its activities with concurrent measurement programs including satellites (e. g. Terra, Aura, Envisat), field activities undertaken by the North American Carbon Program (NACP), and other U.S. and international partners. However, it is being designed as a 'stand alone' mission such that its successful execution is not contingent on other programs. Synthesis of the ensemble of observation from surface, airborne, and space platforms, with the help of global/regional models is an important It is anticipated that approximately 175 flight hours for each of the aircraft (DC-8 and P-3B) will be required for each Phase. Principal operational sites are tentatively selected to be Bangor, ME; Wallops Island, VA; Seattle, WA; Rhinelander, WI; Lancaster, CA; and New Orleans, LA. These coastal and continental sites can support large missions and are suitable for INTEX-NA objectives. The experiment will be supported by forecasts from meteorological and chemical models, satellite observations, surface networks, and enhanced O3,-sonde releases. In addition to

  10. Chemical composition, sources and evolution processes of aerosol at an urban site in Yangtze River Delta, China during wintertime

    NASA Astrophysics Data System (ADS)

    Zhang, Yunjiang; Tang, Lili; Yu, Hongxia; Wang, Zhuang; Sun, Yele; Qin, Wei; Chen, Wentai; Chen, Changhong; Ding, Aijun; Wu, Jing; Ge, Shun; Chen, Cheng; Zhou, Hong-cang

    2015-12-01

    To investigate the composition, sources and evolution processes of submicron aerosol during wintertime, a field experiment was conducted during December 1-31, 2013 in urban Nanjing, a megacity in Yangtze River Delta of China. Non-refractory submicron aerosol (NR-PM1) species were measured with an Aerodyne Aerosol Chemical Speciation Monitor. NR-PM1 is dominated by secondary inorganic aerosol (55%) and organic aerosol (OA, 42%) during haze periods. Six OA components were identified by positive matrix factorization of the OA mass spectra. The hydrocarbon-like OA and cooking-related OA represent the local traffic and cooking sources, respectively. A highly oxidized factor related to biomass burning OA accounted for 15% of the total OA mass during haze periods. Three types of oxygenated OA (OOA), i.e., a less-oxidized OOA (LO-OOA), a more-oxidized OOA (MO-OOA), and a low-volatility OOA (LV-OOA), were identified. LO-OOA is likely associated with fresh urban secondary OA. MO-OOA likely represents photochemical products showing a similar diurnal cycle to nitrate with a pronounced noon peak. LV-OOA appears to be a more oxidized factor with a pronounced noon peak. The OA composition is dominated by secondary species, especially during haze events. LO-OOA, MO-OOA and LV-OOA on average account for 11%, (18%), 24% (21%) and 23% (18%) of the total OA mass for the haze (clean) periods respectively. Analysis of meteorological influence suggested that regional transport from the northern and southeastern areas of the city is responsible for large secondary and low-volatility aerosol formation.

  11. Contributions of local sources, long-range and mountain wind transport for aerosols over an eastern Himalayan high-altitude station in India

    NASA Astrophysics Data System (ADS)

    Chatterjee, Abhijit; Sarkar, Chirantan; Singh, Ajay; Ghosh, Sanjay; Raha, Sibaji; Das, Sanat

    A long-term study (2010-2013) on aerosols mass concentrations (PM2.5), number concentrations of size segregated aerosols and mass concentration of total suspended black carbon aerosols has been made over Darjeeling (27.01 N, 88.15 E), a high altitude (2200 m asl) station at eastern Himalaya in India. Seasonal and diurnal variation of all types of aerosols, their chemical composition and source apportionment revealed that aerosols over this part of Himalaya are mainly of two types; locally generated and long-range transported aerosols. The diurnal variation of aerosols including black carbon showed distinct feature of up-slope mountain wind transport mainly during premonsoon (Mar-May) which brings aerosol particles from low land regions. This present study focuses on the estimation of the individual contributions from local emissions (LE), long-range transport (LRT) and mountain wind transport (MWT) towards the total aerosol loading over Darjeeling. Several strike events (called by local political party) were observed at Darjeeling over the entire period of study (2008-2013) when all the local activities (schools, colleges, offices, vehicular, industrial etc) were stopped fully. Most of the strike events occurred during premonsoon. We have observed three types of events during premonsoon over the entire study period; 1) strike events with the contribution of LRT+MWT with zero local emissions (LE=0), 2) normal days with the contribution of LE+LRT+MWT, 3) normal days with the contribution of LE+MWT with zero long-range contribution (LRT=0). On normal days, the diurnal variation of aerosols during premonsoon showed sharp morning and evening peaks associated to local anthropogenic activities with the effect of up-slope mountain wind during afternoon. During strike events, the morning and evening peaks were absent but a broad peak was observed during afternoon associated to up-slope mountain wind. The increase in aerosol concentrations during afternoon on strike days

  12. Quantum Chemical Calculations Resolved Identification of Methylnitrocatechols in Atmospheric Aerosols.

    PubMed

    Frka, Sanja; Šala, Martin; Kroflič, Ana; Huš, Matej; Čusak, Alen; Grgić, Irena

    2016-06-01

    Methylnitrocatechols (MNCs) are secondary organic aerosol (SOA) tracers and major contributors to atmospheric brown carbon; however, their formation and aging processes in atmospheric waters are unknown. To investigate the importance of aqueous-phase electrophilic substitution of 3-methylcatechol with nitronium ion (NO2(+)), we performed quantum calculations of their favorable pathways. The calculations predicted the formation of 3-methyl-5-nitrocatechol (3M5NC), 3-methyl-4-nitrocatechol (3M4NC), and a negligible amount of 3-methyl-6-nitrocatechol (3M6NC). MNCs in atmospheric PM2 samples were further inspected by LC/(-)ESI-MS/MS using commercial as well as de novo synthesized authentic standards. We detected 3M5NC and, for the first time, 3M4NC. In contrast to previous reports, 3M6NC was not observed. Agreement between calculated and observed 3M5NC/3M4NC ratios cannot unambiguously confirm the electrophilic mechanism as the exclusive formation pathway of MNCs in aerosol water. However, the examined nitration by NO2(+) is supported by (1) the absence of 3M6NC in the ambient aerosols analyzed and (2) the constant 3M5NC/3M4NC ratio in field aerosol samples, which indicates their common formation pathway. The magnitude of error one could make by incorrectly identifying 3M4NC as 3M6NC in ambient aerosols was also assessed, suggesting the importance of evaluating the literature regarding MNCs with special care.

  13. Quantum Chemical Calculations Resolved Identification of Methylnitrocatechols in Atmospheric Aerosols.

    PubMed

    Frka, Sanja; Šala, Martin; Kroflič, Ana; Huš, Matej; Čusak, Alen; Grgić, Irena

    2016-06-01

    Methylnitrocatechols (MNCs) are secondary organic aerosol (SOA) tracers and major contributors to atmospheric brown carbon; however, their formation and aging processes in atmospheric waters are unknown. To investigate the importance of aqueous-phase electrophilic substitution of 3-methylcatechol with nitronium ion (NO2(+)), we performed quantum calculations of their favorable pathways. The calculations predicted the formation of 3-methyl-5-nitrocatechol (3M5NC), 3-methyl-4-nitrocatechol (3M4NC), and a negligible amount of 3-methyl-6-nitrocatechol (3M6NC). MNCs in atmospheric PM2 samples were further inspected by LC/(-)ESI-MS/MS using commercial as well as de novo synthesized authentic standards. We detected 3M5NC and, for the first time, 3M4NC. In contrast to previous reports, 3M6NC was not observed. Agreement between calculated and observed 3M5NC/3M4NC ratios cannot unambiguously confirm the electrophilic mechanism as the exclusive formation pathway of MNCs in aerosol water. However, the examined nitration by NO2(+) is supported by (1) the absence of 3M6NC in the ambient aerosols analyzed and (2) the constant 3M5NC/3M4NC ratio in field aerosol samples, which indicates their common formation pathway. The magnitude of error one could make by incorrectly identifying 3M4NC as 3M6NC in ambient aerosols was also assessed, suggesting the importance of evaluating the literature regarding MNCs with special care. PMID:27136117

  14. A Satellite-based Assessment of Trans-Pacific Transport of Pollution Aerosol

    NASA Technical Reports Server (NTRS)

    Yu, Hongbin; Remer, Lorraine; Chin, Mian; Bian, Huisheng; Kleidman, Richard; Diehl. Thomas

    2007-01-01

    It has been well documented that pollution aerosol and dust from East Asia can transport across the North Pacific basin, reaching North America and beyond. Such intercontinental transport extends the impact of aerosols for climate change, air quality, atmospheric chemistry, and ocean biology from local and regional scales to hemispheric and global scales. Long term, measurement-based studies are necessary to adequately assess the implications of these wider impacts. A satellite-based assessment can augment intensive field campaigns by expanding temporal and spatial scales and also serve as constraints for model simulations. Satellite imagers have been providing a wealth of evidence for the intercontinental transport of aerosols for more than two decades. Quantitative assessments, however, became feasible only recently as a result of the much improved measurement accuracy and enhanced new capabilities of satellite sensors. In this study, we generated a 4-year (2002 to 2005) climatology of optical depth for pollution aerosol (defined as a mixture of aerosols from urbanlindustrial pollution and biomass burning in this study) over the North Pacific from MODerate resolution Imaging Spectro-radiometer (MODIS) observations of fine- and coarse-mode aerosol optical depths. The pollution aerosol mass loading and fluxes were then calculated using measurements of the dependence of aerosol mass extinction efficiency on relative humidity and of aerosol vertical distributions from field campaigns and available satellite observations in the region. We estimated that about 18 Tg/year pollution aerosol is exported from East Asia to the northwestern Pacific Ocean, of which about 25% reaches the west coast of North America. The pollution fluxes are largest in spring and smallest in summer. For the period we have examined the strongest export and import of pollution particulates occurred in 2003, due largely to record intense Eurasia wildfires in spring and summer. The overall

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

    NASA Technical Reports Server (NTRS)

    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.

  16. Aerosol chemistry during the wet season in central Amazonia - The influence of long-range transport

    NASA Technical Reports Server (NTRS)

    Talbot, R. W.; Andreae, M. O.; Berresheim, H.; Artaxo, P.; Garstang, M.

    1990-01-01

    The temporal variation in the concentration and chemistry of the atmospheric aerosol over central Amazonia, Brazil, during the 1987 wet season is discussed based on ground and aircraft collected data obtained during the NASA GTE ABLE 2B expedition conducted in April/May 1987. It is found that wet-season aerosol concentrations and composition are variable in contrast to the more uniform biogenic aerosol observed during the 1985 dry season; four distinct intervals of enhanced aerosol concentration coincided with short periods (3 to 5 d) of extensive rainfall. It is hypothesized that aerosol chemistry in Amazonia during the wet season is strongly influenced by long-range transport of soil dust, marine aerosol, and possibly biomass combustion products advected into the central Basin by large-scale tropospheric circulation, producing periodic pulses of material input to local boundary layer air. The resultant wet-season aerosol regime is dynamic, in contrast to the uniformity of natural biogenic aerosols during the dry season.

  17. New capabilities for space-based cloud and aerosols measurements: The Cloud-Aerosol Transport System (CATS)

    NASA Astrophysics Data System (ADS)

    Yorks, J. E.; McGill, M. J.; Hlavka, D. L.; Palm, S. P.; Hart, W. D.; Nowottnick, E. P.; Vaughan, M.; Rodier, S. D.; Colarco, P. R.; da Silva, A.; Buchard-Marchant, V.

    2013-12-01

    Current uncertainties in cloud and aerosol properties limit our ability to accurately model the Earth's climate system and predict climate change. These limitations are due primarily to difficulties in adequately measuring aerosols and clouds on a global scale. NASA's A-Train satellites provide an unprecedented opportunity to address these uncertainties. In particular, the Cloud-Aerosol Lidar Infrared Pathfinder Spaceborne Observations (CALIPSO) satellite provides vertical profiles of cloud and aerosol properties. The CALIOP lidar onboard CALIPSO has reached its seventh year of operation, well past its expected lifetime. The ATLID lidar on EarthCARE is not expected to launch until 2016 or later. If the CALIOP lidar fails before a new mission is operational, there will be a gap in global lidar measurements. The Cloud-Aerosol Transport System (CATS), built at NASA Goddard Space Flight Center as a payload for the International Space Station (ISS), is set to launch in the summer of 2014. CATS is an elastic backscatter lidar with three wavelengths (1064, 532, 355 nm) and HSRL capability at 532 nm. Depolarization measurements will be made at all three wavelengths. The ISS orbit is a 51 degree inclination orbit at an altitude of about 405 km. This orbit provides more comprehensive coverage of the tropics and mid-latitudes than sun-synchronous orbiting sensors, with nearly a three day repeat cycle. Thus, science applications of CATS include cloud and aerosol climate studies, air quality monitoring, and smoke/volcanic plume tracking. The primary science objectives of CATS include: continuing the CALIPSO aerosol and cloud vertical profile data record, providing near real time data to support operational applications such as air quality modeling, and advancing technology in support of future mission development using the HSRL channel. Furthermore, the vertical profiles of cloud and aerosol properties provided by CATS will complement current and future passive satellite

  18. Multi-Decadal Variation of Aerosols: Sources, Transport, and Climate Effects

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Diehl, Thomas; Bian, Huisheng; Streets, David

    2008-01-01

    We present a global model study of multi-decadal changes of atmospheric aerosols and their climate effects using a global chemistry transport model along with the near-term to longterm data records. We focus on a 27-year time period of satellite era from 1980 to 2006, during which a suite of aerosol data from satellite observations, ground-based measurements, and intensive field experiments have become available. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which involves a time-varying, comprehensive global emission dataset that we put together in our previous investigations and will be improved/extended in this project. This global emission dataset includes emissions of aerosols and their precursors from fuel combustion, biomass burning, volcanic eruptions, and other sources from 1980 to the present. Using the model and satellite data, we will analyze (1) the long-term global and regional aerosol trends and their relationship to the changes of aerosol and precursor emissions from anthropogenic and natural sources, (2) the intercontinental source-receptor relationships controlled by emission, transport pathway, and climate variability.

  19. Cumulus parameterizations in chemical transport models

    NASA Astrophysics Data System (ADS)

    Mahowald, Natalie M.; Rasch, Philip J.; Prinn, Ronald G.

    1995-12-01

    Global three-dimensional chemical transport models (CTMs) are valuable tools for studying processes controlling the distribution of trace constituents in the atmosphere. A major uncertainty in these models is the subgrid-scale parametrization of transport by cumulus convection. This study seeks to define the range of behavior of moist convective schemes and point toward more reliable formulations for inclusion in chemical transport models. The emphasis is on deriving convective transport from meteorological data sets (such as those from the forecast centers) which do not routinely include convective mass fluxes. Seven moist convective parameterizations are compared in a column model to examine the sensitivity of the vertical profile of trace gases to the parameterization used in a global chemical transport model. The moist convective schemes examined are the Emanuel scheme [Emanuel, 1991], the Feichter-Crutzen scheme [Feichter and Crutzen, 1990], the inverse thermodynamic scheme (described in this paper), two versions of a scheme suggested by Hack [Hack, 1994], and two versions of a scheme suggested by Tiedtke (one following the formulation used in the ECMWF (European Centre for Medium-Range Weather Forecasting) and ECHAM3 (European Centre and Hamburg Max-Planck-Institut) models [Tiedtke, 1989], and one formulated as in the TM2 (Transport Model-2) model (M. Heimann, personal communication, 1992). These convective schemes vary in the closure used to derive the mass fluxes, as well as the cloud model formulation, giving a broad range of results. In addition, two boundary layer schemes are compared: a state-of-the-art nonlocal boundary layer scheme [Holtslag and Boville, 1993] and a simple adiabatic mixing scheme described in this paper. Three tests are used to compare the moist convective schemes against observations. Although the tests conducted here cannot conclusively show that one parameterization is better than the others, the tests are a good measure of the

  20. Aplication of LIRIC algorithm to study aerosol transport over Belsk, Poland

    NASA Astrophysics Data System (ADS)

    Pietruczuk, Aleksander; Posyniak, Michał

    2015-04-01

    In this work synergy of measurements done by of a LIDAR and a sun-sky scanning photometer is presented. The LIdar-Radiometer Inversion Code (LIRIC) was applied to study periodic events of increased values of the aerosol optical depth (AOD) observed at Belsk (Poland). Belsk is a background site located in a rural area around 50 km south from Warsaw. Events of increased AOD occur mainly during spring and they coincide with events of elevated concentrations of particulate matter (PM10). This phenomenon is observed in all eastern Europe, e.g. in Minsk, and is caused by long range aerosol transport. Our previous work showed aerosol transport from the border between Belarus, Ukraine and Russia in the planetary boundary layer (PBL), and from north Africa in the free troposphere. The LIRIC algorithm, which uses optical and microphysical properties of the aerosol derived from photometric measurements and LIDAR profiles, was applied to study vertical distribution of fine and coarse modes of aerosol. The analysis of the airmass backward trajectories and models results (DREAM and NAAPS)was also used to determine a possible aerosol type and its source region. This study proved our previous findings. Most of events with increased AODs are observed during spring. In this season the fine mode aerosol is mainly present in the PBL. On the basis of the trajectory analysis and the NAAPS results we presume that it is the absorbing aerosol originating from the regions of seasonal biomass burning in eastern Europe, i.e. the area mentioned above. The events with increased AODs were also found during summer. In this case the fine mode aerosol is transported in the PBL a like to spring season. However, our analysis of trajectories and model results indicated western Europe as a source region. It is probably urban/industrial aerosol. The coarse mode aerosol is transported mainly in the free troposphere as separate layers. The analysis of backward trajectories indicates northern Africa as a

  1. Aerosol variability and atmospheric transport in the Himalayan region from CALIOP 2007-2010 observations

    NASA Astrophysics Data System (ADS)

    Bucci, S.; Cagnazzo, C.; Cairo, F.; Di Liberto, L.; Fierli, F.

    2014-05-01

    This work quantifies the spatial distribution of different aerosol types, their seasonal variability and sources.The analysis of four years of CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) vertically resolved aerosol data allows the identification of spatial patterns of desert dust and carbonaceous particles in different atmospheric layers. Clusters of Lagrangian back trajectories highlight the transport pathways from source regions during the dusty spring season. The analysis shows a prevalence of dust; at low heights it occurs frequently (up to 70% of available observations) and is distributed north of the Tibetan Plateau with a main contribution from the Gobi and Taklamakan deserts, and west of the Tibetan Plateau, originating from the deserts of southwest Asia and advected by the Westerlies. Above the Himalayas the dust amount is minor but still not negligible (occurrence around 20%) and mainly affected by the transport from more distant deserts sources (Sahara and Arabian Peninsula). Carbonaceous aerosol, produced mainly in northern India and eastern China, is subject to shorter-range transport and is indeed observed closer to the sources, while there is a limited amount reaching the top of the plateau. Data analysis reveals a clear seasonal variability in the frequencies of occurrence for the main aerosol types; dust is regulated principally by the monsoon dynamics, with maximal occurrence in spring. We also highlight relevant interannual differences, showing a larger presence of aerosol in the region during 2007 and 2008. The characterization of the aerosol spatial and temporal distribution in terms of observational frequency is a key piece of information that can be directly used for the evaluation of global aerosol models.

  2. Impacts of Long-Range Transport of Metals from East Asia in Bulk Aerosols Collected at the Okinawa Archipelago, Japan

    NASA Astrophysics Data System (ADS)

    A, Sotaro; S, Yuka; I, Moriaki; N, Fumiya; H, Daishi; A, Takemitsu; T, Akira

    2010-05-01

    Economy of East Asia has been growing rapidly, and atmospheric aerosols discharged from this region have been transported to Japan. Okinawa island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km of south Korea. Its location in Asian is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air mass which has been affected by anthropogenic activities. Therefore, Okinawa region is suitable area for studying impacts of air pollutants from East Asia. We simultaneously collected bulk aerosol samples by using the same type of high volume air samplers at Cape Hedo Atmospheric Aerosol Monitoring Station (CHAAMS, Okinawa island), Kume island (ca. 160 km south-west of CHAAMS), and Minami-Daitou island (ca. 320 km south-east of CHAAMS). We determined the concentrations of acid-digested metals using atomic absorption spectrometer and inductively-coupled plasma mass spectrometry (ICP-MS). We report and discuss spatial and temporal distribution of metals in the bulk atmospheric aerosols collected at CHAAMS, Kume island and Minami-Daitou island during June, 2008 to June 2009. We also determined 'background' concentration of metals in Okinawa archipelago. We then compare each chemical component among CHAAMS, Kume island and Minami-Daitou island to elucidate the influence of the transport processes and distances from Asian continent on metal concentrations.

  3. Continuous measurements at the urban roadside in an Asian megacity by Aerosol Chemical Speciation Monitor (ACSM): particulate matter characteristics during fall and winter seasons in Hong Kong

    NASA Astrophysics Data System (ADS)

    Sun, C.; Lee, B. P.; Huang, D.; Jie Li, Y.; Schurman, M. I.; Louie, P. K. K.; Luk, C.; Chan, C. K.

    2016-02-01

    Non-refractory submicron aerosol is characterized using an Aerosol Chemical Speciation Monitor (ACSM) in the fall and winter seasons of 2013 on the roadside in an Asian megacity environment in Hong Kong. Organic aerosol (OA), characterized by application of Positive Matrix Factorization (PMF), and sulfate are found to be dominant. Traffic-related organic aerosol shows good correlation with other vehicle-related species, and cooking aerosol displays clear mealtime concentration maxima and association with surface winds from restaurant areas. Contributions of individual species and OA factors to high NR-PM1 are analyzed for hourly data and daily data; while cooking emissions in OA contribute to high hourly concentrations, particularly during mealtimes, secondary organic aerosol components are responsible for episodic events and high day-to-day PM concentrations. Clean periods are either associated with precipitation, which reduces secondary OA with a lesser impact on primary organics, or clean oceanic air masses with reduced long-range transport and better dilution of local pollution. Haze events are connected with increases in contribution of secondary organic aerosol, from 30 to 50 % among total non-refractory organics, and the influence of continental air masses.

  4. Continuous measurements at the urban roadside in an Asian Megacity by Aerosol Chemical Speciation Monitor (ACSM): particulate matter characteristics during fall and winter seasons in Hong Kong

    NASA Astrophysics Data System (ADS)

    Sun, C.; Lee, B. P.; Huang, D.; Li, Y. J.; Schurman, M. I.; Louie, P. K. K.; Luk, C.; Chan, C. K.

    2015-07-01

    Non-refractory submicron aerosol is characterized using an Aerosol Chemical Speciation Monitor (ACSM) in the fall and winter seasons of 2013 at the roadside in an Asian megacity environment in Hong Kong. Organic aerosol (OA), characterized by application of Positive Matrix Factorization (PMF), and sulfate are found dominant. Traffic-related organic aerosol shows good correlation with other vehicle-related species, and cooking aerosol displays clear meal-time concentration maxima and association with surface winds from restaurant areas. Contributions of individual species and OA factors to high NR-PM1 are analyzed for hourly data and daily data; while cooking emissions in OA contribute to high hourly concentrations, particularly during meal times, secondary organic aerosol components are responsible for episodic events and high day-to-day PM concentrations. Clean periods are either associated with precipitation, which reduces secondary OA with a~lesser impact on primary organics, or clean oceanic air masses with reduced long-range transport and better dilution of local pollution. Haze events are connected with increases in contribution of secondary organic aerosol, from 30 to 50 % among total non-refractory organics, and influence of continental air masses.

  5. The Cloud-Aerosol Transport System (CATS): a New Lidar for Aerosol and Cloud Profiling from the International Space Station

    NASA Technical Reports Server (NTRS)

    Welton, Ellsworth J.; McGill, Matthew J.; Yorks, John E.; Hlavka, Dennis L.; Hart, William D.; Palm, Stephen P.; Colarco, Peter R.

    2011-01-01

    Spaceborne lidar profiling of aerosol and cloud layers has been successfully implemented during a number of prior missions, including LITE, ICESat, and CALIPSO. Each successive mission has added increased capability and further expanded the role of these unique measurements in wide variety of applications ranging from climate, to air quality, to special event monitoring (ie, volcanic plumes). Many researchers have come to rely on the availability of profile data from CALIPSO, especially data coincident with measurements from other A-Train sensors. The CALIOP lidar on CALIPSO continues to operate well as it enters its fifth year of operations. However, active instruments have more limited lifetimes than their passive counterparts, and we are faced with a potential gap in lidar profiling from space if the CALIOP lidar fails before a new mission is operational. The ATLID lidar on EarthCARE is not expected to launch until 2015 or later, and the lidar component of NASA's proposed Aerosols, Clouds, and Ecosystems (ACE) mission would not be until after 2020. Here we present a new aerosol and cloud lidar that was recently selected to provide profiling data from the International Space Station (ISS) starting in 2013. The Cloud-Aerosol Transport System (CATS) is a three wavelength (1064, 532, 355 nm) elastic backscatter lidar with HSRL capability at 532 nm. Depolarization measurements will be made at all wavelengths. The primary objective of CATS is to continue the CALIPSO aerosol and cloud profile data record, ideally with overlap between both missions and EarthCARE. In addition, the near real time data capability of the ISS will enable CATS to support operational applications such as air quality and special event monitoring. The HSRL channel will provide a demonstration of technology and a data testbed for direct extinction retrievals in support of ACE mission development. An overview of the instrument and mission will be provided, along with a summary of the science

  6. Aerosol chemical characterization and role of carbonaceous aerosol on radiative effect over Varanasi in central Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Tiwari, S.; Dumka, U. C.; Kaskaoutis, D. G.; Ram, Kirpa; Panicker, A. S.; Srivastava, M. K.; Tiwari, Shani; Attri, S. D.; Soni, V. K.; Pandey, A. K.

    2016-01-01

    This study investigates the chemical composition of PM10 aerosols at Varanasi, in the central Indo-Gangetic Plain (IGP) during April to July 2011, with emphasis on examining the contribution of elemental carbon (EC) to the estimates of direct aerosol radiative effect (DARE). PM10 samples are analysed for carbonaceous aerosols (Organic Carbon, OC and EC) and water-soluble ionic species (WSIS: Cl-, SO42-, NO3-, PO42- NH4+, Na+, K+, Mg2+ and Ca2+) and several diagnostic ratios (OC/EC, K+/EC, etc) have been also used for studying the aerosol sources at Varanasi. PM10 mass concentration varies between 53 and 310 μg m-3 (mean of 168 ± 73 μg m-3), which is much higher than the National and International air quality standards. The OC mass concentration varies from 6 μg m-3 to 24 μg m-3 (mean of 12 ± 5 μg m-3; 7% of PM10 mass), whereas EC ranges between 1.0 and 14.3 μg m-3 (4.4 ± 3.9 μg m-3; ˜3% of PM10 mass). The relative low OC/EC of 3.9 ± 2.0 and strong correlation (R2 = 0.82) between them suggest the dominance of primary carbonaceous aerosols. The contribution of WSIS to PM10 is found to be ˜12%, out of which ˜57% and 43% are anions and cations, respectively. The composite DARE estimates via SBDART model reveal significant radiative effect and atmospheric heating rates (0.9-2.3 K day-1). Although the EC contributes only ˜3% to the PM10 mass, its contribution to the surface and atmospheric forcing is significantly high (37-63% and 54-77%, respectively), thus playing a major role in climate implications over Varanasi.

  7. Effect of particle settling on lidar profiles of long-range transported Saharan aerosols

    NASA Astrophysics Data System (ADS)

    Gasteiger, Josef; Groß, Silke

    2016-04-01

    A large amount of desert aerosol is transported in the Saharan Air Layer (SAL) westwards from Africa over the Atlantic Ocean. Lidar profiles of transported Saharan aerosol may contain some information about the vertically-resolved aerosol microphysics that could be used to characterize processes that affected the measured aerosol during transport. We present modelled lidar profiles of long-range transported Saharan aerosol assuming that initially the SAL is well-mixed and that there is no vertical mixing of air within the SAL as soon as it reaches the Atlantic. We consider Stokes gravitational settling of aerosol particles over the ocean. The lidar profiles are calculated using optical models for irregularly-shaped mineral dust particles assuming settling-induced particle removal as function of distance from the SAL top. Within the SAL we find a decrease of both the backscatter coefficients and the linear depolarization ratios with decreasing distance from the SAL top. For example, the linear depolarization ratio at a wavelength of 532nm decreases from 0.289 at 1000m to 0.256 at 200m and 0.215 at 100m below SAL top. We compare the modelled backscatter coefficients and linear depolarization ratios to ground-based lidar measurements performed during the SALTRACE field campaign in Barbados (Caribbean) and find agreement within the estimated uncertainties. We discuss the uncertainties of our modeling approach in our presentation. Assumed mineral dust particle shapes, assumed particle mixture properties, and assumptions about processes in the SAL over the continent and the ocean are important aspects to be considered. Uncertainties are relevant for the potential of lidar measurements of transported Saharan dust to learn something about processes occuring in the SAL during long-range transport. We also compare our modeling results to modeling results previously published in the literature.

  8. MATCH-SALSA - Multi-scale Atmospheric Transport and CHemistry model coupled to the SALSA aerosol microphysics model - Part 1: Model description and evaluation

    NASA Astrophysics Data System (ADS)

    Andersson, C.; Bergström, R.; Bennet, C.; Robertson, L.; Thomas, M.; Korhonen, H.; Lehtinen, K. E. J.; Kokkola, H.

    2015-02-01

    We have implemented the sectional aerosol dynamics model SALSA (Sectional Aerosol module for Large Scale Applications) in the European-scale chemistry-transport model MATCH (Multi-scale Atmospheric Transport and Chemistry). The new model is called MATCH-SALSA. It includes aerosol microphysics, with several formulations for nucleation, wet scavenging and condensation. The model reproduces observed higher particle number concentration (PNC) in central Europe and lower concentrations in remote regions. The modeled PNC size distribution peak occurs at the same or smaller particle size as the observed peak at four measurement sites spread across Europe. Total PNC is underestimated at northern and central European sites and accumulation-mode PNC is underestimated at all investigated sites. The low nucleation rate coefficient used in this study is an important reason for the underestimation. On the other hand, the model performs well for particle mass (including secondary inorganic aerosol components), while elemental and organic carbon concentrations are underestimated at many of the sites. Further development is needed, primarily for treatment of secondary organic aerosol, in terms of biogenic emissions and chemical transformation. Updating the biogenic secondary organic aerosol (SOA) scheme will likely have a large impact on modeled PM2.5 and also affect the model performance for PNC through impacts on nucleation and condensation.

  9. Pdf - Transport equations for chemically reacting flows

    NASA Technical Reports Server (NTRS)

    Kollmann, W.

    1989-01-01

    The closure problem for the transport equations for pdf and the characteristic functions of turbulent, chemically reacting flows is addressed. The properties of the linear and closed equations for the characteristic functional for Eulerian and Lagrangian variables are established, and the closure problem for the finite-dimensional case is discussed for pdf and characteristic functions. It is shown that the closure for the scalar dissipation term in the pdf equation developed by Dopazo (1979) and Kollmann et al. (1982) results in a single integral, in contrast to the pdf, where double integration is required. Some recent results using pdf methods obtained for turbulent flows with combustion, including effects of chemical nonequilibrium, are discussed.

  10. Effects on stratospheric ozone from high-speed civil transport: Sensitivity to stratospheric aerosol loading

    NASA Technical Reports Server (NTRS)

    Weisenstein, Debra K.; Ko, Malcolm K. W.; Rodriguez, Jose M.; Sze, Nien-Dak

    1993-01-01

    The potential impact of high-speed civil transport (HSCT) aircraft emissions on stratospheric ozone and the sensitivity of these results to changes in aerosol loading are examined with a two-dimensional model. With aerosols fixed at background levels, calculated ozone changes due to HSCT aircraft emissions range from negligible up to 4-6% depletions in column zone at northern high latitudes. The magnitude of the ozone change depends mainly on the NO(x) increase due to aircraft emissions, which depends on fleet size, cruise altitude, and engine design. The partitioning of the odd nitrogen species in the lower stratosphere among NO, NO2, N2O5, is strongly dependent on the concentration of sulfuric acid aerosol particles, and thus the sensitivity of O3 to NO(x) emissions changes when the stratospheric aerosol loading changes. Aerosol concentrations 4 times greater than background levels have not been unusual in the last 2 decades. Our model results show that a factor of 4 increase in aerosol loading would significantly reduce the calculated ozone depletion due to HSCT emissions. Because of the neutral variabiltiy of stratospheric aerosols, the possible impact of HSCT emissions on ozone must be viewed as a range of possible results.

  11. Aerosol transport and wet scavenging in deep convective clouds: a case study and model evaluation using a multiple passive tracer analysis approach

    SciTech Connect

    Yang, Qing; Easter, Richard C.; Campuzano-Jost, Pedro; Jimenez, Jose L.; Fast, Jerome D.; Ghan, Steven J.; Wang, Hailong; Berg, Larry K.; Barth, Mary; Liu, Ying; Shrivastava, ManishKumar B.; Singh, Balwinder; Morrison, H.; Fan, Jiwen; Ziegler, Conrad L.; Bela, Megan; Apel, Eric; Diskin, G. S.; Mikoviny, Tomas; Wisthaler, Armin

    2015-08-20

    The effect of wet scavenging on ambient aerosols in deep, continental convective clouds in the mid-latitudes is studied for a severe storm case in Oklahoma during the Deep Convective Clouds and Chemistry (DC3) field campaign. A new passive-tracer based transport analysis framework is developed to characterize the convective transport based on the vertical distribution of several slowly reacting and nearly insoluble trace gases. The passive gas concentration in the upper troposphere convective outflow results from a mixture of 47% from the lower level (0-3 km), 21% entrained from the upper troposphere, and 32% from mid-atmosphere based on observations. The transport analysis framework is applied to aerosols to estimate aerosol transport and wet-scavenging efficiency. Observations yield high overall scavenging efficiencies of 81% and 68% for aerosol mass (Dp < 1μm) and aerosol number (0.03< Dp < 2.5μm), respectively. Little chemical selectivity to wet scavenging is seen among observed submicron sulfate (84%), organic (82%), and ammonium (80%) aerosols, while nitrate has a much lower scavenging efficiency of 57% likely due to the uptake of nitric acid. Observed larger size particles (0.15 - 2.5μm) are scavenged more efficiently (84%) than smaller particles (64%; 0.03 - 0.15μm). The storm is simulated using the chemistry version of the WRF model. Compared to the observation based analysis, the standard model underestimates the wet scavenging efficiency for both mass and number concentrations with low biases of 31% and 40%, respectively. Adding a new treatment of secondary activation significantly improves simulation results, so that the bias in scavenging efficiency in mass and number concentrations is reduced to <10%. This supports the hypothesis that secondary activation is an important process for wet removal of aerosols in deep convective storms.

  12. The chemical composition of organic nitrogen in marine rainwater and aerosols

    NASA Astrophysics Data System (ADS)

    Altieri, K. E.; Hastings, M. G.; Peters, A.; Sigman, D. M.

    2010-12-01

    The current state of knowledge on organic nitrogen in the atmosphere is very limited. Atmospheric water soluble organic nitrogen (WSON) is a subset of the complex water soluble organic matter measured in atmospheric aerosols and rainwater; as such, it impacts cloud condensation processes and aerosol chemical and optical properties. In marine and continental atmospheric deposition, the organic N fraction can be 20-80% of total N potentially influencing receiving ecosystems. Therefore, atmospheric WSON plays an important role in both atmospheric chemistry and the global biogeochemical N cycle. However, the sources (i.e., anthropogenic vs. terrestrial vs. marine), composition (e.g., reduced or oxidized N), potential connections to inorganic N (NO3- and NH4+), and spatio-temporal variability of atmospheric WSON are largely unknown. Samples were collected on or near the island of Bermuda (32.27°N, 64.87°W), which is located in the western North Atlantic and experiences seasonal changes in transport that allow for study of both anthropogenically and primarily marine influenced air masses. Rainwater samples (n=7) and aqueous extracted aerosol samples (n=4) were analyzed by positive ion ultra-high resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS) to characterize the chemical composition of the water soluble organic N on a per compound level. We found ~ 800 N containing compounds in 8 compound classes. The CHON+ compound class contained the largest number of N compounds (~ 460). Compared to continental rainwater [Altieri et al., ES&T, 2009], the CHON+ compounds in the marine samples are as dominant in number, yet have less regular patterns and lower O:C ratios for comparable N:C ratios. In fact, average O:C ratios of all N containing compound classes were lower in the marine samples than in continental rainwater samples. No organosulfates or nitrooxy-organosulfates were detected in the marine samples, both of

  13. A Comparison of Aerosol Optical, Microphysical, and Chemical Measurements between LAX and Long Beach Harbor

    NASA Astrophysics Data System (ADS)

    Thornhill, K. L.; Anderson, B. E.; Chen, G.; Winstead, E.; Ziemba, L. D.; Beyersdorf, A. J.; Diskin, G. S.; Nenes, A.; Lathem, T. L.; Arctas Science Team

    2010-12-01

    In the summer of 2008, measurements of aerosols were made on-board the NASA DC-8 over the state of California, as part of the second phase of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) on behalf of the California Air resources Board (CARB). The DC-8 made four flights, between 18 June and 26 June, totaling 33 hours, to examine California’s atmosphere to better understand the chemical dynamics of smog and greenhouse gases over the state. The NASA DC-8 had a suite of aerosol instruments, capable of measuring the number concentrations, optical properties, and size distributions of aerosols between 0.003 and 1500 um. In this presentation, we will compare aerosol observations made at two areas within the Los Angeles Basin, Los Angeles International airport (LAX) and Long Beach Harbor. LAX is in the middle of the second most populated metropolitan area in the United States and is the fifth busiest airport in the world, while Long Beach Harbor (20 miles south of LAX) is the world’s 2nd busiest container port. Initial results suggest a greater aerosol loading and additional presence of ultrafine aerosols during the week due to vehicular emissions. We will also present analysis of aerosol observations as a function of time of day from the four missed approaches at LAX and four over flights of Long Beach Harbor.

  14. Tracking Transport and Transformation of Aerosols using C and O-triple Isotopic Composition of Carbonates: CSI La Jolla

    NASA Astrophysics Data System (ADS)

    Thiemens, M. H.; Shaheen, R.; Chong, K.; Hill, A.; Wong, J.; Zhang, Z.; Dominguez, G.

    2012-12-01

    Aerosols affect climate in numerous ways, including change in the earth's energy balance by absorbing and scattering solar radiations, alteration of the hydrological cycle by serving as cloud condensation nuclei, change in biogeochemical cycles by providing nutrients. Another significant process is the effect on the chemical composition of the atmosphere by providing surfaces for heterogeneous chemical reactions. Fine particles of aerodynamic diameter less than 2.5μm (PM2.5) also impinge upon human health by admission to the respiratory system causing a range of cardiopulmonary diseases. Both climate and public health aspects depend on their physical and chemical properties, therefore, understanding physico-chemical and photochemical transformations on aerosol surfaces is important for predicting their effects on climate change, atmospheric chemistry and human health. Here we present initial findings on the processes occurring on aerosol surfaces using isotopes to delineate day and night time chemistry, thus resolving photochemistry effects, and to identify their sources by way of the carbon isotopes. Aerosols were collected on filter papers for 12h during the day and at night time from June-Dec. 2011in La Jolla, CA., using high volume, multi stage cascade impactors. CO2 released after treating these filter papers with 100% phosphoric acid at 27oC was collected, purified chromatographically and analyzed for both C and O isotopes. Our data indicate that both C and O isotopes can be used to distinguish between heterogeneous and photochemical transformations. Aerosol carbonates collected during the day time were depleted in δ13Cday = -23 to -28‰ and δ18Oday = +3 to +10‰ and were isotopically distinct from the carbonates collected at night time δ13Cnight = 0 to -12‰, δ18Onightnight = +23 to +32‰. Higher chloride concentration in the samples collected at night time indicated the transport of marine air masses whereas higher nitrate and sulfate concentration

  15. Aerosol release and transport program. Semiannual progress report, October 1985-March 1986. Volume 3, No. 1

    SciTech Connect

    Adams, R.E.; Tobias, M.L.

    1986-06-01

    This report summarizes progress for the Aerosol Release and Transport Program sponsored by the Nuclear Regulatory Commission, Office of Nuclear Regulatory Research, Division of Accident Evaluation, for the period October 1985-March 1986. Topics discussed include (1) Aerosol-Moisture Interaction Test (AMIT) experiments 5002 through 5006; (2) efforts to measure the aerodynamic shape factor chi during these experiments; (3) a development test for determining parameters for generating concrete aerosols; (4) data concerning water-vapor generation during plasma torch operation; (5) the use of the ideal gas law in calculating relative humidity; (6) initial comparisons of CONTAIN code results with experimental data for an iron oxide aerosol-steam experiment in the NSPP Facility; (7) pretest predictions using the CONTAIN code for LACE experiment LA-2.

  16. Latitudinal Variation of Chemical Composition in Marine Aerosol Over the Central North Pacific in the Summer

    NASA Astrophysics Data System (ADS)

    Uematsu, M.; Narita, Y.; Mano, Y.; Iguchi, H.; Yoshida, K.; Iwamoto, Y.; Miura, K.

    2006-12-01

    Aeolian dust and gaseous and particulate pollutants from the Asian continent are transported eastward over the North Pacific. These natural and anthropogenic materials in the atmosphere can influence regional and global climate by altering the Earth's radiative balance. From the view of biogeochemical cycles, the atmospheric deposition of aerosols containing iron and other essential trace elements may contribute in sustaining primary productivity of phytoplankton, food web structure and chemical properties of marine atmosphere in the central North Pacific region. During the South-North cross-section cruise from 8 August to 21 September 2005, we conducted atmospheric sampling of aerosol and gaseous components on board R/V Hakuho Maru. Results from 10S to 53N along 160E revealed high nitrate concentration in the high latitude zone corresponded with back-air trajectories to subarctic North Pacific from the Asian continent during the summer. The atmospheric supply of nitrogen compounds may affect the primary production of stratified surface layer in the region. Non-sea-salt sulfate concentration was also high over the subarctic region, and downwind of the Hawaii islands. Volcanic and anthropogenic sulfur are suspected to be the sources of nss-sulfate. However, as an indicator of marine biogenic sulfate, methane sulfonic acid (MSA) is also correlated well with the concentration peaks of nss-sulfate both the vicinity of Hawaii islands and subarctic region. We will attempt to separate nss-sulfate into two fractions, marine biogenic and anthropogenic by using the relation between trace metals and sulfate over the source regions.

  17. The global impact of the transport sectors on atmospheric aerosol in 2030 - Part 2: Aviation

    NASA Astrophysics Data System (ADS)

    Righi, Mattia; Hendricks, Johannes; Sausen, Robert

    2016-04-01

    We use the EMAC (ECHAM/MESSy Atmospheric Chemistry) global climate-chemistry model coupled to the aerosol module MADE (Modal Aerosol Dynamics model for Europe, adapted for global applications) to simulate the impact of aviation emissions on global atmospheric aerosol and climate in 2030. Emissions of short-lived gas and aerosol species follow the four Representative Concentration Pathways (RCPs) designed in support of the Fifth Assessment Report of the Intergovernmental Panel on Climate Change. We compare our findings with the results of a previous study with the same model configuration focusing on year 2000 emissions. We also characterize the aviation results in the context of the other transport sectors presented in a companion paper. In spite of a relevant increase in aviation traffic volume and resulting emissions of aerosol (black carbon) and aerosol precursor species (nitrogen oxides and sulfur dioxide), the aviation effect on particle mass concentration in 2030 remains quite negligible (on the order of a few ng m-3), about 1 order of magnitude less than the increase in concentration due to other emission sources. Due to the relatively small size of the aviation-induced aerosol, however, the increase in particle number concentration is significant in all scenarios (about 1000 cm-3), mostly affecting the northern mid-latitudes at typical flight altitudes (7-12 km). This largely contributes to the overall change in particle number concentration between 2000 and 2030, which also results in significant climate effects due to aerosol-cloud interactions. Aviation is the only transport sector for which a larger impact on the Earth's radiation budget is simulated in the future: the aviation-induced radiative forcing in 2030 is more than doubled with respect to the year 2000 value of -15 mW m-2 in all scenarios, with a maximum value of -63 mW m-2 simulated for RCP2.6.

  18. Direct aerosol chemical composition measurements to evaluate the physicochemical differences between controlled sea spray aerosol generation schemes

    NASA Astrophysics Data System (ADS)

    Collins, D. B.; Zhao, D. F.; Ruppel, M. J.; Laskina, O.; Grandquist, J. R.; Modini, R. L.; Stokes, M. D.; Russell, L. M.; Bertram, T. H.; Grassian, V. H.; Deane, G. B.; Prather, K. A.

    2014-07-01

    Controlled laboratory studies of the physical and chemical properties of sea spray aerosol (SSA) must be underpinned by a physically and chemically accurate representation of the bubble mediated production of nascent SSA particles. Since bubble bursting is sensitive to the physicochemical properties of seawater, any important differences in the SSA production mechanism are projected into SSA composition. Using direct chemical measurements of SSA at the single-particle level, this study presents an inter-comparison of three laboratory-based, bubble-mediated SSA production schemes: gas forced through submerged sintered glass filters ("frits"), a pulsed plunging waterfall apparatus, and breaking waves in a wave channel filled with natural seawater. The size-resolved chemical composition of SSA particles produced by breaking waves is more similar to particles produced by the plunging waterfall than sintered glass filters. Aerosol generated by disintegrating foam produced by sintered glass filters contained a larger fraction of organic enriched particles and a different size-resolved elemental composition, especially in the 0.8-2 μm size range. These particles, when dried, had more spherical morphologies compared to the more cubic structure expected for pure NaCl particles, which can be attributed to the presence of additional organic carbon. In addition to an inter-comparison of three SSA production methods, the role of the episodic or "pulsed" nature of the waterfall method utilized in this study on SSA composition was undertaken. In organic-enriched seawater, the continuous operation of the plunging waterfall mechanism resulted in the accumulation of surface foam and an over-expression of organic matter in SSA particles compared to pulsed plunging waterfall. Throughout this set of experiments, comparative differences in the SSA number size distribution were coincident with differences in aerosol composition, indicating that the production mechanism of SSA exerts

  19. Influence of aqueous chemistry on the chemical composition of fog water and interstitial aerosol in Fresno

    NASA Astrophysics Data System (ADS)

    Kim, Hwajin; Ge, Xinlei; Collier, Sonya; Xu, Jianzhong; Sun, Yele; Wang, Youliang; Herckes, Pierre; Zhang, Qi

    2015-04-01

    A measurement study was conducted in the Central Valley (Fresno) of California in January 2010, during which radiation fog events were frequently observed. Fog plays important roles in atmospheric chemistry by scavenging aerosol particles and trace gases and serving as a medium for various aqueous-phase reactions. Understanding the effects of fog on the microphysical and chemical processing of aerosol particles requires detailed information on their chemical composition. In this study, we characterized the chemical composition of fog water and interstitial aerosol particles to study the effects of fog processing on aerosol properties. Fog water samples were collected during the 2010 Fresno campaigns with a Caltech Active Strand Cloud water Collector (CASCC) while interstitial submicron aerosols were characterized in real time with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and a scanning Mobility Particle Sizer (SMPS). The fog water samples were later analyzed using the HR-ToF-AMS, ion chromatography, and a total carbon analyzer. The chemical composition and characteristics of interstitial particles during the fog events were compared to those of dissolved inorganic and organic matter in fog waters. Compared to interstitial aerosols, fog water is composed of a higher fraction of ammonium nitrate and oxygenated organics, due to aqueous formation of secondary aerosol species as well as enhanced gas-to-particle partitioning of water soluble species under water rich conditions. Sulfate is formed most efficiently in fog water although its contribution to total dissolved mass is relatively low. The HR-ToF-AMS mass spectra of organic matter in fog water (FOM) are very similar to that of oxygenated organic aerosols (OOA) derived from positive matrix factorization (PMF) of the HR-ToF-AMS spectra of ambient aerosol (r2 = 0.96), but FOM appears to contain a large fraction of acidic functional groups than OOA. FOM is also enriched of

  20. Modelling multi-component aerosol transport problems by the efficient splitting characteristic method

    NASA Astrophysics Data System (ADS)

    Liang, Dong; Fu, Kai; Wang, Wenqia

    2016-11-01

    In this paper, a splitting characteristic method is developed for solving general multi-component aerosol transports in atmosphere, which can efficiently compute the aerosol transports by using large time step sizes. The proposed characteristic finite difference method (C-FDM) can solve the multi-component aerosol distributions in high dimensional domains over large ranges of concentrations and for different aerosol types. The C-FDM is first tested to compute the moving of a Gaussian concentration hump. Comparing with the Runge-Kutta method (RKM), our C-FDM can use very large time step sizes. Using Δt = 0.1, the accuracy of our C-FDM is 10-4, but the RKM only gets the accuracy of 10-2 using a small Δt = 0.01 and the accuracy of 10-3 even using a much smaller Δt = 0.002. A simulation of sulfate transport in a varying wind field is then carried out by the splitting C-FDM, where the sulfate pollution is numerically showed expanding along the wind direction and the effects of the different time step sizes and different wind speeds are analyzed. Further, a realistic multi-component aerosol transport over an area in northeastern United States is studied. Concentrations of PM2.5 sulfate, ammonium, nitrate are high in the urban area, and low in the marine area, while sea salts of sodium and chloride mainly exist in the marine area. The normalized mean bias and the normalized mean error of the predicted PM2.5 concentrations are -6.5% and 24.1% compared to the observed data measured at monitor stations. The time series of numerical aerosol concentration distribution show that the strong winds can move the aerosol concentration peaks horizontally for a long distance, such as from the urban area to the rural area and from the marine area to the urban and rural area. Moreover, we also show the numerical time duration patterns of the aerosol concentration distributions due to the affections of the turbulence and the deposition removal. The developed splitting C-FDM algorithm

  1. Activation of "synthetic ambient" aerosols - Relation to chemical composition of particles <100 nm

    NASA Astrophysics Data System (ADS)

    Burkart, J.; Hitzenberger, R.; Reischl, G.; Bauer, H.; Leder, K.; Puxbaum, H.

    2012-07-01

    Cloud condensation nuclei (CCN) are an important fraction of atmospheric aerosols because of their role in cloud formation. Experimental studies focus either on direct field measurements of complex ambient aerosols or laboratory investigations on well defined aerosols produced from single substances or substance mixtures. In this study, we focussed on the ultrafine aerosol because in terms of number concentration, the majority of the CCN are expected to have sizes in this range. A field study was performed from July 2007 to October 2008 to investigate the activation behaviour of the atmospheric aerosol in Vienna (Burkart et al., 2011). Filter samples of the aerosol <0.1 μm aerodynamic equivalent diameter were collected, elutriated and used to generate "synthetic ambient" aerosol in a nebulizer. Chemical analyses of the ultrafine water soluble material were also performed. The CCN properties of the "synthetic ambient" aerosol were obtained using the University of Vienna CCN counter (Giebl et al., 2002; Dusek et al., 2006b) at a nominal supersaturation (SS) of 0.5%. Activation diameters dact ranged from 54.5 nm to 66 nm, were larger than dact of typical single inorganic salts and showed no seasonal pattern in contrast to the fraction of water soluble organic carbon (WSOC), which ranged from 44% in spring to 15% in winter. The average hygroscopicity parameter κ (Petters and Kreidenweis, 2007) obtained from the activation curves ranged from 0.20 to 0.30 (average 0.24), which was significantly lower than κchem calculated from the chemical composition (0.43 ± 0.07).

  2. Aerosol vertical distribution, optical properties and transport over Corsica (western Mediterranean)

    NASA Astrophysics Data System (ADS)

    Léon, J.-F.; Augustin, P.; Mallet, M.; Bourrianne, T.; Pont, V.; Dulac, F.; Fourmentin, M.; Lambert, D.; Sauvage, B.

    2015-03-01

    This paper presents the aerosol vertical distribution observed in the western Mediterranean between February and April 2011 and between February 2012 and August 2013. An elastic backscattering lidar was continuously operated at a coastal site in the northern part of Corsica Island (Cap Corse) for a total of more than 14 000 h of observations. The aerosol extinction coefficient retrieved from cloud-free lidar profiles are analyzed along with the SEVIRI satellite aerosol optical depth (AOD). The SEVIRI AOD was used to constrain the retrieval of the aerosol extinction profiles from the lidar range-corrected signal and to detect the presence of dust or pollution aerosols. The daily average AOD at 550 nm is 0.16 (±0.09) and ranges between 0.05 and 0.80. A seasonal cycle is observed with minima in winter and maxima in spring-summer. High AOD days (above 0.3 at 550 nm) represent less than 10% of the totality of daily observations and correspond to the large scale advection of desert dust from Northern Africa or pollution aerosols from Europe. The respective origin of the air masses is confirmed using FLEXPART simulations in the backward mode. Dust events are characterized by a large turbid layer between 2 and 5 km height while pollution events show a lower vertical development with a thick layer below 3 km in altitude. However low level dust transport is also reported during spring while aerosol pollution layer between 2 and 4 km height has been also observed. We report an effective lidar ratio at 355 nm for pollution aerosols 68 (±13) Sr while it is 63 (±18) Sr for dust. The daily mean AOD at 355 nm for dust events is 0.61 (±0.14) and 0.71 (±0.16) for pollution aerosols events.

  3. Effects of Chemical Aging on the Heterogeneous Freezing of Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Collier, K.; Brooks, S. D.

    2014-12-01

    Organic aerosols are emitted into the atmosphere from a variety of sources and display a wide range of effectiveness in promoting the nucleation of ice in clouds. Soot and polycyclic aromatic hydrocarbons (PAHS) arise from incomplete combustion and other pollutant sources. Hydrocarbon compounds in diesel motor oil and other fuel blends include compounds such as octacosane (a straight saturated alkane), squalane (a branched saturated alkane) and squalene (an unsaturated branched alkene). At temperatures above -36°C, the formation of ice crystals in the atmosphere is facilitated by heterogeneous freezing processes in which atmospheric aerosols act as ice nuclei (IN). The variability in ability of organic particles to facilitate heterogeneous ice nucleation causes major uncertainties in predictions of aerosol effects on climate. Further, atmospheric aerosol composition and ice nucleation ability can be altered via chemical aging and reactions with atmospheric oxidants such as ozone. In this study, we take a closer look at the role of chemical oxidation on the efficiency of specific IN during contact freezing laboratory experiments. The freezing temperatures of droplets in contact with representative organic aerosols are determined through the use of an optical microscope apparatus equipped with a cooling stage and a digital camera. Chemical changes at the surface of aerosols due to ozone exposure are characterized using Raman Microspectroscopy and Fourier Transform Infrared Spectroscopy with Horizontal Attenuated Total Reflectance. Our results indicate that oxidation of certain atmospheric organics (soot and PAHS) enhances their ice nucleation ability. In this presentation, results of heterogeneous nucleation on various types of organic aerosols will be presented, and the role of structure in promoting freezing will be discussed.

  4. Tying Biological Activity to Changes in Sea Spray Aerosol Chemical Composition via Single Particle Analyses

    NASA Astrophysics Data System (ADS)

    Sultana, C. M.; Lee, C.; Collins, D. B.; Axson, J. L.; Laskina, O.; Grandquist, J. R.; Grassian, V. H.; Prather, K. A.

    2014-12-01

    In remote marine environments, sea spray aerosols (SSA) often represent the greatest aerosol burden, thus having significant impacts on direct radiative interactions and cloud processes. Previous studies have shown that SSA is a complex mixture of inorganic salts and an array of dissolved and particulate organic components. Enrichment of SSA organic content is often correlated to seawater chlorophyll concentrations, a measure of oceanic biological activity. As the physical and chemical properties of aerosols control their radiative effects, recent studies conducted by the Center for Aerosol Impacts on Climate and the Environment have endeavored to further elucidate the ties between marine biological activity and primary SSA chemical composition using highly time resolved single particle analyses. A series of experiments performed in the recently developed Marine Aerosol Reference Tank evaluated the effect of changing marine microbial populations on SSA chemical composition, which was monitored via an aerosol time-of-flight mass spectrometer and a variety of offline spectroscopic and microscopic techniques. Each experiment was initiated using unfiltered and untreated seawater, thus maintaining a high level of biogeochemical complexity. This study is the first of its kind to capture daily changes in the primary SSA mixing state over the growth and death of a natural phytoplankton bloom. Increases in organic aerosol types (0.4-3 μm), internally and externally mixed with sea salt, could not be correlated to chlorophyll concentrations. Maximum production of these populations occurred two to four days after the in vivo chlorophyll fluorescence peaked in intensity. This work is in contrast to the current paradigm of correlating SSA organic content to seawater chlorophyll concentration.

  5. The Pasadena Aerosol Characterization Observatory (PACO): chemical and physical analysis of the Western Los Angeles Basin aerosol

    NASA Astrophysics Data System (ADS)

    Hersey, S. P.; Craven, J. S.; Schilling, K. A.; Metcalf, A. R.; Sorooshian, A.; Chan, M. N.; Flagan, R. C.; Seinfeld, J. H.

    2011-02-01

    The Pasadena Aerosol Characterization Observatory (PACO) represents the first major aerosol characterization experiment centered in the Western/Central Los Angeles Basin. The sampling site, located on the campus of the California Institute of Technology in Pasadena, was positioned to sample a continuous afternoon influx of transported urban aerosol with a photochemical age of 1-2 h and generally free from major local contributions. Sampling spanned 5 months during the summer of 2009, which were broken into 3 regimes on the basis of distinct meteorological conditions. Regime I was characterized by a series of low pressure systems, resulting in high humidity and rainy periods with clean conditions. Regime II typified early summer meteorology, with significant morning marine layers and warm, sunny afternoons. Regime III was characterized by hot, dry conditions with little marine layer influence. Organic aerosol (OA) is the most significant constituent of Los Angeles aerosol (42, 43, and 55% of total submicron mass in regimes I, II, and III, respectively), and that the overall oxidation state remains relatively constant on timescales of days to weeks (O:C = 0.44 ± 0.08, 0.55 ± 0.05, and 0.48 ± 0.08 during regimes I, II, and III, respectively), with no difference in O:C between morning and afternoon periods. Periods characterized by significant morning marine layer influence followed by photochemically favorable afternoons displayed significantly higher aerosol mass and O:C ratio, suggesting that aqueous processes may be important in the generation of secondary aerosol and oxidized organic aerosol (OOA) in Los Angeles. Water soluble organic mass (WSOM) reaches maxima near 14:00-15:00 local time (LT), but the percentage of AMS organic mass contributed by WSOM remains relatively constant throughout the day. Sulfate and nitrate reside predominantly in accumulation mode aerosol, while afternoon SOA production coincides with the appearance of a distinct fine mode

  6. The Cloud-Aerosol Transport System (CATS): A New Lidar for Aerosol and Cloud Profiling from the International Space Station

    NASA Technical Reports Server (NTRS)

    Welton, Ellsworth J.; McGill, Mathew J.; Yorks. John E.; Hlavka, Dennis L.; Hart, William D.; Palm, Stephen P.; Colarco, Peter R.

    2012-01-01

    Spaceborne lidar profiling of aerosol and cloud layers has been successfully implemented during a number of prior missions, including LITE, ICESat, and CALIPSO. Each successive mission has added increased capability and further expanded the role of these unique measurements in wide variety of applications ranging from climate, to air quality, to special event monitoring (ie, volcanic plumes). Many researchers have come to rely on the availability of profile data from CALIPSO, especially data coincident with measurements from other A-Train sensors. The CALIOP lidar on CALIPSO continues to operate well as it enters its fifth year of operations. However, active instruments have more limited lifetimes than their passive counterparts, and we are faced with a potential gap in lidar profiling from space if the CALIOP lidar fails before a new mission is operational. The ATLID lidar on EarthCARE is not expected to launch until 2015 or later, and the lidar component of NASA's proposed Aerosols, Clouds, and Ecosystems (ACE) mission would not be until after 2020. Here we present a new aerosol and cloud lidar that was recently selected to provide profiling data from the International Space Station (ISS) starting in 2013. The Cloud-Aerosol Transport System (CATS) is a three wavelength (1064,532,355 nm) elastic backscatter lidar with HSRL capability at 532 nm. Depolarization measurements will be made at all wavelengths. The primary objective of CATS is to continue the CALIPSO aerosol and cloud profile data record, ideally with overlap between both missions and EarthCARE. In addition, the near real time (NRT) data capability ofthe ISS will enable CATS to support operational applications such as aerosol and air quality forecasting and special event monitoring. The HSRL channel will provide a demonstration of technology and a data testbed for direct extinction retrievals in support of ACE mission development. An overview of the instrument and mission will be provided, along with a

  7. A Model for the Transport of Sea-Spray Aerosols in the Coastal Zone

    NASA Astrophysics Data System (ADS)

    Piazzola, J.; Tedeschi, G.; Demoisson, A.

    2015-05-01

    We study the dynamics of sea-spray particles in the coastal region of La Reunion Island on the basis of numerical simulations using the transport aerosol model MACMod (Marine Aerosol Concentration Model) and a survey of the aerosol size distributions measured at four locations at two different heights in the north-west part of the island. This allows evaluation of the performance of our model in case of pure marine air masses with implementation of accurate boundary conditions. First of all, an estimate of the aerosol concentration at 10-m height at the upwind boundary of the calculation domain is obtained using a revisited version of the MEDEX (Mediterranean Extinction) model. Estimates of the vertical profile of aerosol concentrations are then provided using aerosol data obtained at two different heights at the upwind boundary of the calculation domain. A parametrization of the vertical profiles of aerosol concentrations for maritime environment is proposed. The results are then compared to the vertical profiles of 0.532 m aerosol particle extinction coefficient obtained from lidar data provided by the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) and also to the data provided by the Aerosol Robotic Network (AERONET). This allows validation of the complete vertical profiles in the mixed layer and shows the validity of satellite data for determination of the vertical profiles. Two kinds of simulation were made: one without a particle advection flux at the upwind boundary of the numerical domain, whereas the second simulation was made with a particle advection flux. In the first case, the influence of the distance to the shoreline on the local sea-spray dynamics is investigated. In the second set of simulation, the particles issued from the local production in the surf zone near the shoreline are mixed with aerosols advected from the remote ocean. A good agreement between the model calculations using our boundary conditions and the data was found. The

  8. Assessment of microphysical and chemical factors of aerosols over seas of the Russian Artic Eastern Section

    NASA Astrophysics Data System (ADS)

    Golobokova, Liudmila; Polkin, Victor

    2014-05-01

    The newly observed kickoff of the Northern Route development drew serious attention to state of the Arctic Resource environment. Occurring climatic and environmental changes are more sensitively seen in polar areas in particular. Air environment control allows for making prognostic assessments which are required for planning hazardous environmental impacts preventive actions. In August - September 2013, RV «Professor Khlustin» Northern Sea Route expeditionary voyage took place. En-route aerosol sampling was done over the surface of the Beringov, Chukotka and Eastern-Siberia seas (till the town of Pevek). The purpose of sampling was to assess spatio-temporal variability of optic, microphysical and chemical characteristics of aerosol particles of the surface layer within different areas adjacent to the Northern Sea Route. Aerosol test made use of automated mobile unit consisting of photoelectric particles counter AZ-10, aetalometr MDA-02, aspirator on NBM-1.2 pump chassis, and the impactor. This set of equipment allows for doing measurements of number concentration, dispersed composition of aerosols within sizes d=0.3-10 mkm, mass concentration of submicron sized aerosol, and filter-conveyed aerosols sampling. Filter-conveyed aerosols sampling was done using method accepted by EMEP and EANET monitoring networks. The impactor channel was upgraded to separate particles bigger than 1 mkm in size, and the fine grain fraction settled down on it. Reverse 5-day and 10-day trajectories of air mass transfer executed at heights of 10, 1500 and 3500 m were analyzed. The heights were selected by considerations that 3000 m is the height which characterizes air mass trend in the lower troposphere. 1500 m is the upper border of the atmospheric boundary layer, and the sampling was done in the Earth's surface layer at less than 10 m. Minimum values of the bespoken microphysical characteristics are better characteristic of higher latitudes where there are no man induced sources of

  9. Systematic Relationships among Background SE U.S. Aerosol Optical, Micro-physical, and Chemical Properties-Development of an Optically-based Aerosol Characterization

    NASA Astrophysics Data System (ADS)

    Sherman, J. P.; Link, M. F.; Zhou, Y.

    2014-12-01

    Remote sensing-based retrievals of aerosol composition require known or assumed relationships between aerosol optical properties and types. Most optically-based aerosol classification schemes apply some combination of the spectral dependence of aerosol light scattering and absorption-using the absorption and either scattering or extinction Angstrom exponents (AAE, SAE and EAE), along with single-scattering albedo (SSA). These schemes can differentiate between such aerosol types as dust, biomass burning, and urban/industrial but no such studies have been conducted in the SE U.S., where a large fraction of the background aerosol is a variable mixture of biogenic SOA, sulfates, and black carbon. In addition, AERONET retrievals of SSA are often highly uncertain due to low AOD in the region during most months. The high-elevation, semi-rural AppalAIR facility at Appalachian State University in Boone, NC (1090m ASL, 36.210N, 81.690W) is home to the only co-located NOAA-ESRL and AERONET monitoring sites in the eastern U.S. Aerosol chemistry measured at AppalAIR is representative of the background SE U.S (Link et al. 2014) Dried aerosol light absorption and dried and humidified aerosol light scattering and hemispheric backscattering at 3 visible wavelengths and 2 particle size cuts (sub-1μm and sub-10μm) are measured continuously. Measurements of size-resolved, non-refractory sub-1μm aerosol composition were made by a co-located AMS during the 2012-2013 summers and 2013 winter. Systematic relationships among aerosol optical, microphysical, and chemical properties were developed to better understand aerosol sources and processes and for use in higher-dimension aerosol classification schemes. The hygroscopic dependence of visible light scattering is sensitive to the ratio of sulfate to organic aerosol(OA), as are SSA and AAE. SAE is a less sensitive indicator of fine-mode aerosol size than hemispheric backscatter fraction (b) and is more sensitive to fine-mode aerosol

  10. Simulation of the recent evolution of stratospheric aerosols by the MOSTRA Simulation of the recent evolution of stratospheric aerosols by the MOSTRA microphysical/transport model

    NASA Astrophysics Data System (ADS)

    Bingen, Christine; Errera, Quentin; Vanhellemont, Filip; Fussen, Didier; Mateshvili, Nina; Dekemper, Emmanuel; Loodts, Nicolas

    2010-05-01

    We present recent advances in the development of a microphysical/transport model for stratospheric aerosols, called MOdel for STRatospheric Aerosols (MOSTRA). MOSTRA is a 3D model describing the evolution in time and space of the stratospheric aerosol distribution described using a set of discrete size bins. The microphysical module used in this model makes use of the PSCBOX model developed by Larsen (2000). The transport module is based on the flux-form semi-Lagragian scheme by Lin and Rood (1996). The model structure will be presented with simulations of the evolution of the volcanic aerosol plume after recent volcanic eruptions. References: N. Larsen, Polar Stratospheric Clouds, Microphysical and optical models, Scientific Report 00-06, Danish Meteorological Institute, 2000 Lin, S.-J. Rood, R.B., Multidimensional Flux-Form Semi-Lagrangian Transport Schemes, Monthly Weather Review, 124, 2046-2070, 1996.

  11. Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

    NASA Astrophysics Data System (ADS)

    Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

    2013-12-01

    The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles <100 nm generated by means of jets

  12. Investigation of biomass burning and aerosol loading and transport in South America utilizing geostationary satellites

    NASA Technical Reports Server (NTRS)

    Menzel, Paul; Prins, Elaine

    1995-01-01

    This study attempts to assess the extent of burning and associated aerosol transport regimes in South America and the South Atlantic using geostationary satellite observations, in order to explore the possible roles of biomass burning in climate change and more directly in atmospheric chemistry and radiative transfer processes. Modeling and analysis efforts have suggested that the direct and indirect radiative effects of aerosols from biomass burning may play a major role in the radiative balance of the earth and are an important factor in climate change calculations. One of the most active regions of biomass burning is located in South America, associated with deforestation in the selva (forest), grassland management, and other agricultural practices. As part of the NASA Aerosol Interdisciplinary Program, we are utilizing GOES-7 (1988) and GOES-8 (1995) visible and multispectral infrared data (4, 11, and 12 microns) to document daily biomass burning activity in South America and to distinguish smoke/aerosols from other multi-level clouds and low-level moisture. This study catalogues the areal extent and transport of smoke/aerosols throughout the region and over the Atlantic Ocean for the 1988 (July-September) and 1995 (June-October) biomass burning seasons. The smoke/haze cover estimates are compared to the locations of fires to determine the source and verify the haze is actually associated with biomass burning activities. The temporal resolution of the GOES data (half-hourly in South America) makes it possible to determine the prevailing circulation and transport of aerosols by considering a series of visible and infrared images and tracking the motion of smoke, haze and adjacent clouds. The study area extends from 40 to 70 deg W and 0 to 40 deg S with aerosol coverage extending over the Atlantic Ocean when necessary. Fire activity is estimated with the GOES Automated Biomass Burning Algorithm (ABBA). To date, our efforts have focused on GOES-7 and GOES-8 ABBA

  13. Time-resolved inorganic chemical composition of fine aerosol and associated precursor gases over an urban environment in western India: Gas-aerosol equilibrium characteristics

    NASA Astrophysics Data System (ADS)

    Sudheer, A. K.; Rengarajan, R.

    2015-05-01

    Inorganic ionic constituents (Na+, NH4+, K+, Mg2+, Ca2+, Cl-, NO3- and SO42-) of PM2.5 and associated trace gases (NH3, HNO3 and HCl) were measured simultaneously by Ambient Ion Monitor - Ion Chromatograph (AIM-IC) system with a time resolution of one hour at an urban location in semi-arid region of western India during summer and winter. The average NH3, HNO3 and HCl concentrations were 11.6 ± 5.0, 2.9 ± 0.8 and 0.15 μg m-3, respectively, during winter. During summer, NH3 and HNO3 concentrations were of similar magnitude, whereas HCl concentration was less than ∼0.03 μg m-3. NH3 concentration exhibited a distinct diurnal variation during both seasons. However, HNO3 did not show a specific diurnal trend during the observation period in both seasons. The data obtained were used to study gas-aerosol equilibrium characteristics using a thermodynamic equilibrium model, ISORROPIA II. The results suggest that NH3 exists in equilibrium between measured fine-mode particle and gas phase with a systematic bias of ∼14%, whereas HCl and HNO3 deviate significantly from the modelled data. These observations have implications on thermodynamic equilibrium assumptions used for estimating various aerosol parameters such as liquid water content, pH, etc., thus causing significant bias in chemical transport model results over the study region.

  14. Status of the solar and infrared radiation submodels in the LLNL 1-D and 2-D chemical-transport models

    SciTech Connect

    Grant, K.E.; Taylor, K.E.; Ellis, J.S.; Wuebbles, D.J.

    1987-07-01

    The authors have implemented a series of state of the art radiation transport submodels in previously developed one dimensional and two dimensional chemical transport models of the troposphere and stratosphere. These submodels provide the capability of calculating accurate solar and infrared heating rates. They are a firm basis for further radiation submodel development as well as for studying interactions between radiation and model dynamics under varying conditions of clear sky, clouds, and aerosols. 37 refs., 3 figs.

  15. Production Mechanism, Number Concentration, Size Distribution, Chemical Composition, and Optical Properties of Sea Spray Aerosols Workshop, Summer 2012

    SciTech Connect

    Meskhidze, Nicholas

    2013-10-21

    The objective of this workshop was to address the most urgent open science questions for improved quantification of sea spray aerosol-radiation-climate interactions. Sea spray emission and its influence on global climate remains one of the most uncertain components of the aerosol-radiation-climate problem, but has received less attention than other aerosol processes (e.g. production of terrestrial secondary organic aerosols). Thus, the special emphasis was placed on the production flux of sea spray aerosol particles, their number concentration and chemical composition and properties.

  16. The ambient organic aerosol soluble in water: Measurements, chemical characterization, and an investigation of sources

    NASA Astrophysics Data System (ADS)

    Sullivan, Amy P.

    This thesis characterizes the ambient fine organic carbon (OC) aerosol and investigates its sources through the development and deployment of new analytical measurement techniques. Recognizing that OC is highly chemically complex, the approach was to develop methods capable of quantitatively measuring a large chemical fraction of the aerosol instead of specific chemical speciation. The focus is on organic compounds that are soluble in water (WSOC) since little is known about its chemical nature. The results from this thesis show that WSOC has mainly two sources: biomass burning and secondary organic aerosol (SOA). In urban areas, WSOC increases with plume age, and tracks other photochemically produced compounds. Chemical analysis of WSOC suggests that in urban Atlanta, the SOA is mainly small-chain aliphatic compounds indirectly linked to vehicle emissions. A method was first developed for quantitative on-line measurements of WSOC by extending the application of the Particle-into-Liquid Sampler (PILS) from inorganic to organic aerosol measurements. In this approach a PILS captures ambient particles into a flow of purified water, which is then forced through a liquid filter and the carbonaceous content quantified on-line by a Total Organic Carbon (TOC) analyzer. An instrument was first developed for ground-based measurements and then modified for airborne deployment. Ground-based measurements at the St. Louis - Midwest Supersite during the summer of 2003 showed that the fraction of OC that is water-soluble can have a highly diurnal pattern with WSOC to OC ratios reaching 0.80 during the day and lows of 0.40 during the night. During extended periods under stagnation pollution events, this pattern was well correlated with ozone concentrations. The results are consistent with formation of SOA. Airborne PILS-TOC measurements from the NOAA WP-3D during the New England Air Quality Study/Intercontinental Transport and Chemical Transformation (NEAQS/ITCT) 2004 program

  17. The Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment SALTRACE 2013 - Overview and Early Results (Invited)

    NASA Astrophysics Data System (ADS)

    Weinzierl, B.; Ansmann, A.; Reitebuch, O.; Freudenthaler, V.; Müller, T.; Kandler, K.; Althausen, D.; Busen, R.; Dollner, M.; Dörnbrack, A.; Farrell, D. A.; Gross, S.; Heimerl, K.; Klepel, A.; Kristensen, T. B.; Mayol-Bracero, O. L.; Minikin, A.; Prescod, D.; Prospero, J. M.; Rahm, S.; Rapp, M.; Sauer, D. N.; Schaefler, A.; Toledano, C.; Vaughan, M.; Wiegner, M.

    2013-12-01

    Mineral dust is an important player in the global climate system. In spite of substantial progress in the past decade, many questions in our understanding of the atmospheric and climate effects of mineral dust remain open such as the change of the dust size distribution during transport across the Atlantic Ocean and the associated impact on the radiation budget, the role of wet and dry dust removal mechanisms during transport, and the complex interaction between mineral dust and clouds. To close gaps in our understanding of mineral dust in the climate system, the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE: http://www.pa.op.dlr.de/saltrace) was conducted in June/July 2013. SALTRACE is a German initiative combining ground-based and airborne in-situ and lidar measurements with meteorological data, long-term measurements, satellite remote sensing and modeling. During SALTRACE, the DLR research aircraft Falcon was based on Sal, Cape Verde, between 11 and 17 June, and on Barbados between 18 June and 11 July 2013. The Falcon was equipped with a suite of in-situ instruments for the measurement of microphysical and optical aerosol properties and with a nadir-looking 2-μm wind lidar. Ground-based lidar and in-situ instruments were deployed in Barbados and Puerto Rico. Mineral dust from several dust outbreaks was measured by the Falcon between Senegal and Florida. On the eastern side of the Atlantic, dust plumes extended up to 6 km altitude, while the dust layers in the Caribbean were mainly below 4.5 km. The aerosol optical thickness of the dust outbreaks studied ranged from 0.2 to 0.6 at 500 nm in Barbados. Highlights during SALTRACE included the sampling of a dust plume in the Cape Verde area on 17 June which was again measured with the same instrumentation on 21 and 22 June near Barbados. The event was also captured by the ground-based lidar and in-situ instrumentation. Another highlight was the formation of tropical storm

  18. AERONET-based microphysical and optical properties of smoke-dominated aerosol near source regions and transported over oceans, and implications for satellite retrievals of aerosol optical depth

    NASA Astrophysics Data System (ADS)

    Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

    2013-09-01

    Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad ''families'' of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA ∼0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA ∼0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savannah at Mongu (Zambia), with average SSA ∼0.85 in the midvisible. These can serve as candidate sets of aerosol microphysical/optical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.

  19. Aeronet-based Microphysical and Optical Properties of Smoke-dominated Aerosol near Source Regions and Transported over Oceans, and Implications for Satellite Retrievals of Aerosol Optical Depth

    NASA Technical Reports Server (NTRS)

    Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

    2013-01-01

    Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad families of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA 0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA 0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savanna at Mongu (Zambia), with average SSA 0.85 in the midvisible. These can serve as candidate sets of aerosol microphysicaloptical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.

  20. Aerosol chemical vapor deposition of metal oxide films

    DOEpatents

    Ott, K.C.; Kodas, T.T.

    1994-01-11

    A process of preparing a film of a multicomponent metal oxide including: forming an aerosol from a solution comprised of a suitable solvent and at least two precursor compounds capable of volatilizing at temperatures lower than the decomposition temperature of said precursor compounds; passing said aerosol in combination with a suitable oxygen-containing carrier gas into a heated zone, said heated zone having a temperature sufficient to evaporate the solvent and volatilize said precursor compounds; and passing said volatilized precursor compounds against the surface of a substrate, said substrate having a sufficient temperature to decompose said volatilized precursor compounds whereby metal atoms contained within said volatilized precursor compounds are deposited as a metal oxide film upon the substrate is disclosed. In addition, a coated article comprising a multicomponent metal oxide film conforming to the surface of a substrate selected from the group consisting of silicon, magnesium oxide, yttrium-stabilized zirconium oxide, sapphire, or lanthanum gallate, said multicomponent metal oxide film characterized as having a substantially uniform thickness upon said substrate.

  1. Long- and/or short-range transportation of local Asian aerosols in DRAGON-Osaka Experiment

    NASA Astrophysics Data System (ADS)

    Nakata, M.; Sano, I.; Mukai, S.; Holben, B. N.

    2013-12-01

    This work intends to demonstrate the spatial and temporal variation of atmospheric particles in East Asia, especially around AERONET (Aerosol Robotics Network) -Osaka site during Dragon Asia period in the spring of 2012, named Dragon-Osaka. It is known that the air pollution in East Asia becomes to be severe due to both the increasing emissions of the anthropogenic aerosols associated with economic growth and the complicated behavior of natural aerosols. Thus the precise observations of atmospheric particles in East Asia are desired. Osaka is the second big city in Japan and a typical Asian urban area. The population of the region is around 20 millions including neighbor prefectures. Therefore, air quality in the region is slightly bad compared to remote area due to industries and auto mobiles. In recent years, Asian dusts and anthropogenic small particles transported from China and cover those cities throughout year. AERONET Osaka site was established in 2002 on the campus of Kinki University. Nowadays, LIDAR (Light Detection and Ranging), an SPM sampler (SPM-613D, Kimoto Electric, Japan) and others are available on the roof of a building. The site data are useful for algorithm development of aerosol retrieval over busy city. On the other hand, human activities in this region also emit the huge amount of pollutions, thus it is needed to investigate the local distribution of aerosols in this region. In order to investigate change of aerosol properties, PM-individual analysis is made with scanning electron microscope (SEM) coupled with energy dispersive X-ray analyzer (EDX). SEM/EDX is an effective instrument to observe the surface microstructure and analyze the chemical composition of such materials as metals, powders, biological specimens, etc. We used sampling data from the SPM sampler at AERONET Osaka site. During a period of DRAGON-Asia, high concentrations of air pollutant were observed on the morning of March 11 in Fukue Island in the East China Sea. On the

  2. Chemical Characterization of Secondary Organic Aerosol from Oxidation of Isoprene Hydroxyhydroperoxides.

    PubMed

    Riva, Matthieu; Budisulistiorini, Sri H; Chen, Yuzhi; Zhang, Zhenfa; D'Ambro, Emma L; Zhang, Xuan; Gold, Avram; Turpin, Barbara J; Thornton, Joel A; Canagaratna, Manjula R; Surratt, Jason D

    2016-09-20

    Atmospheric oxidation of isoprene under low-NOx conditions leads to the formation of isoprene hydroxyhydroperoxides (ISOPOOH). Subsequent oxidation of ISOPOOH largely produces isoprene epoxydiols (IEPOX), which are known secondary organic aerosol (SOA) precursors. Although SOA from IEPOX has been previously examined, systematic studies of SOA characterization through a non-IEPOX route from 1,2-ISOPOOH oxidation are lacking. In the present work, SOA formation from the oxidation of authentic 1,2-ISOPOOH under low-NOx conditions was systematically examined with varying aerosol compositions and relative humidity. High yields of highly oxidized compounds, including multifunctional organosulfates (OSs) and hydroperoxides, were chemically characterized in both laboratory-generated SOA and fine aerosol samples collected from the southeastern U.S. IEPOX-derived SOA constituents were observed in all experiments, but their concentrations were only enhanced in the presence of acidified sulfate aerosol, consistent with prior work. High-resolution aerosol mass spectrometry (HR-AMS) reveals that 1,2-ISOPOOH-derived SOA formed through non-IEPOX routes exhibits a notable mass spectrum with a characteristic fragment ion at m/z 91. This laboratory-generated mass spectrum is strongly correlated with a factor recently resolved by positive matrix factorization (PMF) of aerosol mass spectrometer data collected in areas dominated by isoprene emissions, suggesting that the non-IEPOX pathway could contribute to ambient SOA measured in the Southeastern United States. PMID:27466979

  3. A model for studying the composition and chemical effects of stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Tabazadeh, Azadeh; Turco, Richard P.; Jacobson, Mark Z.

    1994-01-01

    We developed polynomial expressions for the temperature dependence of the mean binary and water activity coefficients for H2SO4 and HNO3 solutions. These activities were used in an equilibrium model to predict the composition of stratospheric aerosols under a wide range of environmental conditions. For typical concentrations of H2O, H2SO4, HNO3, HCl, HBr, HF, and HOCl in the lower stratosphere, the aerosol composition is estimated as a function of the local temperature and the ambient relative humidity. For temperatures below 200 K, our results indicate that (1) HNO3 contributes a significant mass fraction to stratospheric aerosols, and (2) HCl solubility is considerably affected by HNO3 dissolution into sulfate aerosols. We also show that, in volcanically disturbed periods, changes in stratospheric aerosol composition can significantly alter the microphysics that leads to the formation of polar stratospheric clouds. The effects caused by HNO3 dissolution on the physical and chemical properties of stratospheric aerosols are discussed.

  4. Physical and Chemical Properties of Aerosols at the Tropical Coastal Site, Trivandrum

    NASA Astrophysics Data System (ADS)

    George, Susan K.; Nair, Prabha R.; Parameswaran, Krishnaswamy; Jacob, Salu; Abraham, Annamma; Abhilash, K. S.

    The influence of tropospheric aerosols on the regional climate is fairly well accepted though there exists large uncertainties in assessing its exact magnitude. This is mainly due to the fact that the aerosol properties are highly variable at short spatial and temporal extents and the information available is rather limited. To overcome these deficiency it is highly essential to gather and analyse long term data covering different seasons over varying climatic regimes. Trivandrum (8.55o N, 77o E), a tropical coastal site situated near the southern tip of Indian Peninsula, is a location where systematic monitoring of different aerosol parameters are being carried out since last two decades. With progressing time new techniques and instruments are also being incorporated. This paper presents the results from the observations on aerosols carried out during the period 2003 to 2005 at this location. Different aerosol properties such as total mass concentration, number density, size distribution, optical depth, chemical composition, etc. are studied systematically during this period. A High Volume Sampler (for measuring total mass loading), Aerosol Spectrometer (for measuring size segregated number density from which size distribution can be derived), and Microtops Sunphotometer (which measures optical depth at 1020 nm) are used to study the physical/optical properties of aerosols. The chemical composition of atmospheric aerosols is examined employing Ion Chromatography, Atomic Absorption Spectroscopy and Inductively Couple Plasma - Atomic Emission Spectroscopy. The mean mass concentration of aerosols observed at this site is 54 µg m-3 , which varies by ±19 µg m-3 depending on season and prevailing meteorology. The aerosol number density is 108 particles/m3 . The mass loading at this location is significantly low compared to the northern parts of India as well as the national ambient air quality standards indicating that the environment is relatively less polluted as

  5. Aerosol transport over Siberia: analysis of the summer 2013 YAK-AEROSIB aircraft campaign

    NASA Astrophysics Data System (ADS)

    Ancellet, Gerard; Penner, Johannes; Kokhanenko, Grigorii; Arshinov, Mikhail; Chernov, Dimitry; Kozlov, Valery; Paris, Jean Daniel; Pruvost, Arnaud; Belan, Boris; Nedelec, Philippe; Pelon, Jacques; Law, Kathy

    2014-05-01

    Transport and transformation of aerosols related to forest fires and Eastern Asia anthropogenic emissions have been identified as very important questions to understand the Arctic climate. Two aircraft campaigns have been conducted over Siberia in summer 2012 and 2013 with in-situ measurements by aerosol spectrometers and also by a 532 nm backscatter lidar in 2013. The aerosol data can be also combined with CO measurements measured on-board the aircraft to identify the aerosol pollution sources. The analysis of the transport processes has been performed with the FLEXPART Lagrangian model run either in the forward or backward mode. While the 2012 campaign is characterized by anticyclonic conditions and strong forest fire emissions, the 2013 campaign corresponds to upward lifting of Northern China emissions. Comparisons with satellite data obtained with the CALIPSO mission for the two summer periods will be presented to identify the spatial extent and the temporal evolution of the pollution plumes and also to test the ability of the satellite data to derive the aerosol types. This work was funded by CNRS (France), the French Ministry of Foreign Affairs, CEA (France), Presidium of RAS (Program No. 4), Brunch of Geology, Geophysics and Mining Sciences of RAS (Program No. 5), Interdisciplinary integration projects of Siberian Branch of RAS (No. 35, No. 70, No. 131), Russian Foundation for Basic Research (grants No 14-05-00526, 14-05-00590).

  6. Ozone Measurements and a 3D Chemical Transport Model

    NASA Technical Reports Server (NTRS)

    Stolarski, Richard S.; Douglass, Anne R.; Frith, Stacey; Steenrod, Steven; Polansky, Brian

    2004-01-01

    We have used our three-dimensional chemical transport model (CTM) to calculate the expected reponse of stratospheric composition over the past 30 years to forcing by chlorine and bromine compounds, solar ultraviolet, and volcanic aerosols. The CTM uses off-line winds and temperatures fiom a 50-year run of the finite volume general circulation model (FVGCM). We compare the total column ozone and the ozone profile fiom the CTM output to a variety of data sources. These include a merged total ozone data set from TOMS and SBUV using the new version 8 algorithm. Total ozone fiom the CTM are compared to ground-station measurements of total ozone at specific locations. Ozone profiles are compared to satellite meausrements fiom SBUV, SAGE, and HALOE. Profiles are also compared to ozonesondes over several locations. The results of the comparisons are quantified by using a time-series statistical analysis to determine trends, solar cycle, and volcanic reponse in both the model and in the data. Initial results indicate that the model responds to forcings in a way that is similar to the observed atmospheric response. The model does seem to be more sensitive to the chlorine and bromine perturbation ihan is the data. Further details and comparisons wiii be discussed.

  7. A HTAP Multi-Model Assessment of the Influence of Regional Anthropogenic Emission Reductions on Aerosol Direct Radiative Forcing and the Role of Intercontinental Transport

    NASA Technical Reports Server (NTRS)

    Yu, Hongbin; Chin, Mian; West, J. Jason; Atherton, Cynthia S.; Bellouin, Nicolas; Bergmann, Dan; Bey, Isabelle; Bian, Huisheng; Diehl, Thomas; Forberth, Gerd; Hess, Peter; Schulz, Michael; Shindell, Drew; Takemura, Toshihiko; Tan, Qian

    2012-01-01

    In this study, we assess changes of aerosol optical depth (AOD) and direct radiative forcing (DRF) in response to the reduction of anthropogenic emissions in four major pollution regions in the northern hemisphere by using results from 10 global chemical transport models in the framework of the Hemispheric Transport of Air Pollution (HTAP). The multi-model results show that on average, a 20% reduction of anthropogenic emissions in North America, Europe, East Asia and South Asia lowers the global mean AOD and DRF by about 9%, 4%, and 10% for sulfate, organic matter, and black carbon aerosol, respectively. The impacts of the regional emission reductions on AOD and DRF extend well beyond the source regions because of intercontinental transport. On an annual basis, intercontinental transport accounts for 10-30% of the overall AOD and DRF in a receptor region, with domestic emissions accounting for the remainder, depending on regions and species. While South Asia is most influenced by import of sulfate aerosol from Europe, North America is most influenced by import of black carbon from East Asia. Results show a large spread among models, highlighting the need to improve aerosol processes in models and evaluate and constrain models with observations.

  8. Hygroscopic and chemical properties of aerosols collected near a copper smelter: implications for public and environmental health.

    PubMed

    Sorooshian, Armin; Csavina, Janae; Shingler, Taylor; Dey, Stephen; Brechtel, Fred J; Sáez, A Eduardo; Betterton, Eric A

    2012-09-01

    Particulate matter emissions near active copper smelters and mine tailings in the southwestern United States pose a potential threat to nearby environments owing to toxic species that can be inhaled and deposited in various regions of the body depending on the composition and size of the particles, which are linked by particle hygroscopic properties. This study reports the first simultaneous measurements of size-resolved chemical and hygroscopic properties of particles next to an active copper smelter and mine tailings by the towns of Hayden and Winkelman in southern Arizona. Size-resolved particulate matter samples were examined with inductively coupled plasma mass spectrometry, ion chromatography, and a humidified tandem differential mobility analyzer. Aerosol particles collected at the measurement site are enriched in metals and metalloids (e.g., arsenic, lead, and cadmium) and water-uptake measurements of aqueous extracts of collected samples indicate that the particle diameter range of particles most enriched with these species (0.18-0.55 μm) overlaps with the most hygroscopic mode at a relative humidity of 90% (0.10-0.32 μm). These measurements have implications for public health, microphysical effects of aerosols, and regional impacts owing to the transport and deposition of contaminated aerosol particles. PMID:22852879

  9. Hygroscopic and Chemical Properties of Aerosols collected near a Copper Smelter: Implications for Public and Environmental Health

    PubMed Central

    Sorooshian, Armin; Csavina, Janae; Shingler, Taylor; Dey, Stephen; Brechtel, Fred J.; Sáez, A. Eduardo; Betterton, Eric A.

    2012-01-01

    Particulate matter emissions near active copper smelters and mine tailings in the southwestern United States pose a potential threat to nearby environments owing to toxic species that can be inhaled and deposited in various regions of the body depending on the composition and size of the particles, which are linked by particle hygroscopic properties. This study reports the first simultaneous measurements of size-resolved chemical and hygroscopic properties of particles next to an active copper smelter and mine tailings by the towns of Hayden and Winkelman in southern Arizona. Size-resolved particulate matter samples collected near an active copper smelter were examined with inductively coupled plasma mass spectrometry, ion chromatography, and a humidified tandem differential mobility analyzer. Aerosol particles collected at the measurement site are enriched in metals and metalloids (e.g. arsenic, lead, and cadmium) and water-uptake measurements of aqueous extracts of collected samples indicate that the particle diameter range of particles most enriched with these species (0.18–0.55 µm) overlaps with the most hygroscopic mode at a relative humidity of 90% (0.10–0.32 µm). These measurements have implications for public health, microphysical effects of aerosols, and regional impacts owing to the transport and deposition of contaminated aerosol particles. PMID:22852879

  10. Atmospheric aerosols: A literature summary of their physical characteristics and chemical composition

    NASA Technical Reports Server (NTRS)

    Harris, F. S., Jr.

    1976-01-01

    This report contains a summary of 199 recent references on the characterization of atmospheric aerosols with respect to their composition, sources, size distribution, and time changes, and with particular reference to the chemical elements measured by modern techniques, especially activation analysis.

  11. Uncertainty in Cloud Aerosol Transport System (CATS) Doppler Lidar Products and Measurements

    NASA Astrophysics Data System (ADS)

    Selmer, P. A.

    2010-12-01

    The Cloud Aerosol Transport System (CATS) is both a high spectral resolution lidar and Doppler lidar currently being developed at NASA Goddard Space Flight Center for use as a demonstrator instrument for NASA’s Aerosol Cloud Ecosystem (ACE) Mission. CATS is intended to fly on NASA’s high-altitude ER-2 aircraft. CATS will be capable of measuring both aerosol properties and horizontal wind velocity as a function of altitude. The accuracy of these measurements is important to the success of the instrument and the ACE mission. Uncertainty equations for both the aerosol and wind products are derived. Initially the only sources of error are assumed to be instrument error in the spectral measurements. Using simulated CATS spectral measurements from simulated atmospheric profiles (an atmosphere with only a cirrus layer, an atmosphere with only a cumulus layer, an atmosphere with only an aerosol layer, and an atmosphere with no clouds or aerosols), the uncertainty in the aerosol and wind products are calculated. These calculated uncertainties are found to be within reason. Also worthy of consideration is the effect of aircraft motion on CATS’ wind measurements and products. An equation for the the nadir angle (assumed to be about 45 degrees for CATS), as well as the uncertainty in this angle, in terms of aircraft pitch and roll is derived. The effect of uncertainty in this angle on the uncertainty in CATS aerosol and wind products is calculated using the same simulated data previously mentioned, which is found to be insignificant for normal, steady flight.

  12. Inland Transport of Aerosolized Florida Red Tide Toxins.

    PubMed

    Kirkpatrick, Barbara; Pierce, Richard; Cheng, Yung Sung; Henry, Michael S; Blum, Patricia; Osborn, Shannon; Nierenberg, Kate; Pederson, Bradley A; Fleming, Lora E; Reich, Andrew; Naar, Jerome; Kirkpatrick, Gary; Backer, Lorraine C; Baden, Daniel

    2010-02-01

    Florida red tides, an annual event off the west coast of Florida, are caused by the toxic dinoflagellate, Karenia brevis. K. brevis produces a suite of potent neurotoxins, brevetoxins, which kill fish, sea birds, and marine mammals, as well as sickening humans who consume contaminated shellfish. These toxins become part of the marine aerosol, and can also be inhaled by humans and other animals. Recent studies have demonstrated a significant increase in symptoms and decrease lung function in asthmatics after only one hour of beach exposure during an onshore Florida red tide bloom.This study constructed a transect line placing high volume air samplers to measure brevetoxins at sites beginning at the beach, moving approximately 6.4 km inland. One non-exposure and 2 exposure studies, each of 5 days duration, were conducted. No toxins were measured in the air during the non-exposure period. During the 2 exposure periods, the amount of brevetoxins varied considerably by site and by date. Nevertheless, brevetoxins were measured at least 4.2 kilometers from the beach and/or 1.6 km from the coastal shoreline. Therefore, populations sensitive to brevetoxins (such as asthmatics) need to know that leaving the beach may not discontinue their environmental exposure to brevetoxin aerosols.

  13. Urban aerosol in Oporto, Portugal: Chemical characterization of PM10 and PM2.5

    NASA Astrophysics Data System (ADS)

    Custódio, Danilo; Ferreira, Catarina; Alves, Célia; Duarte, Mácio; Nunes, Teresa; Cerqueira, Mário; Pio, Casimiro; Frosini, Daniele; Colombi, Cristina; Gianelle, Vorne; Karanasiou, Angeliki; Querol, Xavier

    2014-05-01

    Several urban and industrial areas in Southern Europe are not capable of meeting the implemented EU standards for particulate matter. Efficient air quality management is required in order to ensure that the legal limits are not exceeded and that the consequences of poor air quality are controlled and minimized. Many aspects of the direct and indirect effects of suspended particulate matter on climate and public health are not well understood. The temporal variation of the chemical composition is still demanded, since it enables to adopt off-set strategies and to better estimate the magnitude of anthropogenic forcing on climate. This study aims to provide detailed information on concentrations and chemical composition of aerosol from Oporto city, an urban center in Southern Europe. This city is located near the coast line in the North of Portugal, being the country's second largest urban area. Moreover, Oporto city economic prospects depend heavily on a diversified industrial park, which contribute to air quality degradation. Another strong source of air pollution is traffic. The main objectives of this study are: 1) to characterize the chemical composition of PM10 and PM2.5 by setting up an orchestra of aerosol sampling devices in a strategic place in Oporto; 2) to identify the sources of particles exploring parameters such as organic and inorganic markers (e.g. sugars as tracers for biomass burning; metals and elemental carbon for industrial and vehicular emissions); 3) to evaluate long range transport of pollutants using back trajectory analysis. Here we present data obtained between January 2013 and January 2014 in a heavy traffic roadside sampling site located in the city center. Different PM10 and PM2.5 samplers were operated simultaneously in order to collect enough mass on different filter matrixes and to fulfill the requirements of analytical methodologies. More than 100 aerosol samples were collected and then analysed for their mass concentration and

  14. Aerosol variability and atmospheric transport in the Himalayan region from CALIOP 2007-2010 observations

    NASA Astrophysics Data System (ADS)

    Bucci, S.; Cagnazzo, C.; Cairo, F.; Di Liberto, L.; Fierli, F.

    2013-06-01

    Himalayan Plateau is surrounded by regions with high natural and anthropogenic aerosol emissions that have a strong impact on regional climate. This is particularly critical for the Himalayan glaciers whose equilibrium is also largely influenced by radiative direct and indirect effects induced by aerosol burden. This work focuses on the spatial and vertical distribution of different aerosol types, their seasonal variability and sources. The analysis of the 2007-2010 yr of CALIPSO vertically resolved satellite data allows the identification of spatial patterns of desert dust and carbonaceous particles in different atmospheric layers. Clusters of Lagrangian back-trajectories highlight the transport pathways from source regions during the dusty spring season. The analysis shows a prevalence of dust; at low heights they are distributed mainly north (with a main contribution from the Gobi and Taklamakan deserts) and west of the Tibetan Plateau (originating from the deserts of South-West Asia and advected by the westerlies). Above the Himalayas the dust amount is minor but still not negligible (detectable in around 20% of the measurements), and transport from more distant deserts (Sahara and Arabian Peninsula) is important. Smoke aerosol, produced mainly in North India and East China, is subject to shorter range transport and is indeed observed closer to the sources while there is a limited amount reaching the top of the plateau. Data analysis reveals a clear seasonal variability in the frequencies of occurrence for the main aerosol types; dust is regulated principally by the monsoon dynamics, with maxima of occurrence in spring. The study also highlights relevant interannual differences, showing a larger presence of aerosol in the region during 2007 and 2008 yr.

  15. High-Resolution Desorption Electrospray Ionization Mass Spectrometry for Chemical Characterization of Organic Aerosols

    SciTech Connect

    Laskin, Julia; Laskin, Alexander; Roach, Patrick J.; Slysz, Gordon W.; Anderson, Gordon A.; Nizkorodov, Serguei; Bones, David L.; Nguyen, Lucas

    2010-03-01

    Characterization of the chemical composition and chemical transformations of secondary organic aerosol (SOA) is both a major challenge and the area of greatest uncertainty in current aerosol research. This study presents the first application of desorption electrospray ionization combined with high-resolution mass spectrometry (DESI-MS) for detailed chemical characterization and studies of chemical aging of OA collected on Teflon substrates. DESI-MS offers unique advantages both for detailed characterization of chemically labile components in OA that cannot be detected using more traditional electrospray ionization mass spectrometry (ESI-MS) and for studying chemical aging of OA. DESI-MS enables rapid characterization of OA samples collected on substrates by eliminating the sample preparation stage. In addition, it enables detection and structural characterization of chemically labile molecules in OA samples by minimizing the residence time of analyte in the solvent. SOA produced by the ozonolysis of limonene (LSOA) was allowed to react with gaseous ammonia. Chemical aging resulted in measurable changes in the optical properties of LSOA observed using UV- visible spectroscopy. DESI-MS combined with tandem mass spectrometry experiments (MS/MS) enabled identification of species in aged LSOA responsible for absorption of the visible light. Detailed analysis of the experimental data allowed us to identify chemical changes induced by reactions of LSOA constituents with ammonia and distinguish between different mechanisms of chemical aging.

  16. Coupled Effects of Vadose Zone Hydrodynamics and Anionic Surfactant Aerosol-22 on the Transport of Cryptosporidium parvum in Soil

    NASA Astrophysics Data System (ADS)

    Darnault, C. J.; Jacobson, A. R.; Powelson, D.; Baveye, P.; Peng, Z.; Yu, C.

    2013-12-01

    Cryptosporidium parvum is a microbial pathogen that may be found in soil, surface and groundwater resources. We studied their transport behavior under conditions where both C. parvum oocysts and chemicals that may affect their mobility are present in soils. Surfactants occur widely in soils due to agricultural practices such as wastewater irrigation and application of agrichemicals. Surfactants decrease the surface tension of the soil solution, which may reduce the ability of C. parvum oocysts to be retained at gas-water interfaces. Understanding the fate and transport of C. parvum oocysts following land application of manure and use of surfactants in rural and agricultural watersheds is critical to assess the threat to water resources. We investigated the coupled effects of vadose zone hydrodynamics and an anionic surfactant Aerosol-22 on the transport of C. parvum oocysts in natural structured and non-structured agricultural or range soils from Illinois and Utah. Column transport experiments consisted of unsaturated flow subject to macropore and fingered flows resulting from simulated rainfall with and without surfactant. To assess the behavior of C. parvum oocysts in soils, the breakthrough and distribution of C. parvum oocysts in soil profiles were obtained using qPCR. We observed that surfactant enhanced the transport of C. parvum oocysts when preferential flow paths are present. However, when the interconnection between macropores is not established in the soils, surfactant limited the transport of C. parvum oocysts through the soil matrix by forming oocyst-surfactant-Ca flocs.

  17. Influence of atmospheric parameters on vertical profiles and horizontal transport of aerosols generated in the surf zone

    NASA Astrophysics Data System (ADS)

    Kusmierczyk-Michulec, J.; Tedeschi, G.; Van Eijk, A. M. J.; Piazzola, J.

    2013-10-01

    The vertical and horizontal transport of aerosols generated over the surf zone is discussed. Experimental data were collected during the second campaign of the Surf Zone Aerosol Experiment that took place in Duck NC (USA) in November 2007. The Empirical Orthogonal Function (EOF) method was used to analyze the vertical concentration gradients, and allowed separating the surf aerosols from aerosols advected from elsewhere. The numerical Marine Aerosol Concentration Model (MACMod) supported the analysis by confirming that the concentration gradients are more pronounced under stable conditions and that aerosol plumes are then more confined to the surface. The model also confirmed the experimental observations made during two boat runs along the offshore wind vector that surf-generated aerosols are efficiently advected out to sea over several tens of kilometers.

  18. Chemical properties and outflow patterns of anthropogenic and dust particles on Rishiri Island during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia)

    NASA Astrophysics Data System (ADS)

    Matsumoto, Kiyoshi; Uyama, Yukiko; Hayano, Teruaki; Tanimoto, Hiroshi; Uno, Itsushi; Uematsu, Mitsuo

    2003-12-01

    Investigations of chemical properties and transport mechanisms of continental aerosols are necessary for estimating their influences on global radiative budget and on the global material cycle. Intensive measurements of atmospheric aerosols and the associated species on Rishiri Island, near the northern tip of Japan, were conducted from March to May 2001, in order to understand the chemical properties, source regions, transport pathways, and transport patterns of anthropogenic and mineral aerosols over the east Asian Pacific Rim region during the spring. Mean concentrations of nss-SO42-, NO3-, NH4+, nss-Ca2+ in aerosols were 2.48, 0.64, 0.72, and 0.17 μg m-3, respectively. Elemental carbon and organic carbon in fine particles (d < 2.5 μm) yielded mean concentrations of 0.25 and 0.80 μg m-3, respectively. The concentrations of these species frequently increased to higher values because of outbreaks of continental polluted air masses, whereas under background conditions, they decreased to lower values similar to those observed over the remote ocean. Our results demonstrate that nss-SO42- and NH4+ coexist in fine particles, that NO3- and nss-Ca2+ coexist in coarse particles, and that each set is transported in an alternate manner. Continentally derived NO3- is transported as coarse particle to the east Asian Pacific Rim region. Anthropogenic pollutants and dust particles are not necessarily transported together. It was often found that anthropogenic fine particles containing abundant nss-SO42- appeared first and were then followed by large mineral particles that had absorbed NO3-. Short-term intrusion of the air masses containing abundant particulate carbonaceous compounds, probably due to the influence of biomass burning, also often occurred during the outflow events of continental air masses. Atmospheric behaviors of sulfate, nitrate, and carbonaceous species are different from one another, although they are all derived mainly from combustion processes.

  19. In situ physical and chemical characterisation of the Eyjafjallajökull aerosol plume in the free troposphere over Italy

    NASA Astrophysics Data System (ADS)

    Sandrini, S.; Giulianelli, L.; Decesari, S.; Fuzzi, S.; Cristofanelli, P.; Marinoni, A.; Bonasoni, P.; Chiari, M.; Calzolai, G.; Canepari, S.; Perrino, C.; Facchini, M. C.

    2014-01-01

    Continuous measurements of physical and chemical properties at the Mt. Cimone (Italy) GAW-WMO (Global Atmosphere Watch, World Meteorological Organization) Global Station (2165 m a.s.l.) have allowed the detection of the volcanic aerosol plume resulting from the Eyjafjallajökull (Iceland) eruption of spring 2010. The event affected the Mt. Cimone site after a transport over a distance of more than 3000 km. Two main transport episodes were detected during the eruption period, showing a volcanic fingerprint discernible against the free tropospheric background conditions typical of the site, the first from April 19 to 21 and the second from 18 to 20 May 2010. This paper reports the modification of aerosol characteristics observed during the two episodes, both characterised by an abrupt increase in fine and, especially, coarse mode particle number. Analysis of major, minor and trace elements by different analytical techniques (ionic chromatography, particle induced X-ray emission-particle induced gamma-ray emission (PIXE-PIGE) and inductively coupled plasma mass spectrometry (ICP-MS)) were performed on aerosols collected by ground-level discrete sampling. The resulting database allows the characterisation of aerosol chemical composition during the volcanic plume transport and in background conditions. During the passage of the volcanic plume, the fine fraction was dominated by sulphates, denoting the secondary origin of this mode, mainly resulting from in-plume oxidation of volcanic SO2. By contrast, the coarse fraction was characterised by increased concentration of numerous elements of crustal origin, such as Fe, Ti, Mn, Ca, Na, and Mg, which enter the composition of silicate minerals. Data analysis of selected elements (Ti, Al, Fe, Mn) allowed the estimation of the volcanic plume's contribution to total PM10, resulting in a local enhancement of up to 9.5 μg m-3, i.e. 40% of total PM10 on 18 May, which was the most intense of the two episodes. These results appear

  20. a Study on the Physical and Chemical Properties of Stratospheric Aerosols.

    NASA Astrophysics Data System (ADS)

    Tabazadeh, Azadeh

    The physical and chemical properties of stratospheric aerosols under background and perturbed conditions are discussed. First, a multi-component aerosol physical chemistry model was developed to study the composition and reactivity of stratospheric aerosols. The compositions are predicted from an equilibrium assumption between the condensed-and gas-phases, and they are calculated as a function of ambient temperature, relative humidity, and the total mass of nitric acid and sulfuric acid present per unit volume of air. The water and solute activity parameters in the aerosol model are derived from various laboratory sources, and the set of equilibrium equations are solved using a unique numerical scheme. The aerosol model is applied to study the formation of nitric acid-containing aerosols in the stratosphere. Also, the equilibrium compositions are used to estimate the extent of aqueous phase processing of chlorine species in the aerosol solutions. This processing can contribute to the depletion of the stratospheric ozone layer, especially after major volcanic eruptions where sulfate aerosols are more abundant. Second, a surface chemistry model was constructed that includes Langmuir trace-gas adsorption and desorption, Brunauer, Emmett and Teller adsorption of water vapor, surface poisoning, solvation and diffusion of molecules on the surface, chemical activation and reaction of adsorbates, and product desorption or reaction. This model is used to study the effects of relative humidity and other physical parameters on the efficiency of heterogeneous chemical processes which occur on the surfaces of solid polar stratospheric clouds. These heterogeneous chemical processes are responsible for the formation of the "ozone hole", can contribute to global ozone depletion, and may have tropospheric significance. Finally, a fluid dynamics and thermodynamics model of volcanic eruption columns was used to develop a scheme for predicting the extent of HCl removal from volcanic

  1. Chemical characterisation of african dust transported to Canary Region

    NASA Astrophysics Data System (ADS)

    Gelado, M. D.; López, P.; Prieto, S.; Collado, C.; Hernández, J. J.

    2009-04-01

    African dust pulses have important effects on the climate conditions and the marine biogeochemistry in the Canary Region. Aerosol samples have been collected at three stations on Gran Canaria Island (Taliarte at sea level, Tafira 269 m a.s.l. and Pico de la Gorra 1930 m a.s.l.) during 2000-2008. Elemental characterisation of the collected mineral aerosol and back trajectories of the air masses are used to distinguish regional African sources of dust. Dust aerosol samples from North Sahara (Morocco, North Algeria and Tunisia), West and Central Sahara (20°-30°N, 18°W-50°E) and Sahel (0°-20°N, 18°W-50°E) have shown different Ca/Ti, Al/Ti and Fe/Al ratios. Ti appears as a better tracer element of specific source of dust than Fe, probably due to a less mineral alteration during the atmospheric transport.

  2. Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in Downtown Atlanta, Georgia

    NASA Astrophysics Data System (ADS)

    Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

    2013-12-01

    The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was recently developed to provide long-term real-time continuous measurements of ambient non-refractory (i.e., organic, sulfate, ammonium, nitrate, and chloride) submicron particulate matter (NR-PM1). Currently, there are a limited number of field studies that evaluate the long-term performance of the ACSM against established monitoring networks. In this study, we present seasonal intercomparisons of the ACSM with collocated fine aerosol (PM2.5) measurements at the Southeastern Aerosol Research and Characterization (SEARCH) Jefferson Street (JST) site near downtown Atlanta, GA, during 2011-2012. The collocated measurements included a second ACSM, continuous and integrated sulfate, nitrate, and ammonium measurements, as well as a semi-continuous Sunset organic carbon/elemental carbon (OC/EC) analyzer, continuous tapered element oscillating microbalance (TEOM), 24 h integrated Federal Reference Method (FRM) filters, and continuous scanning electrical mobility system-mixing condensation particle counter (SEMS-MCPC). Intercomparison of the two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21); mass concentration for all chemical species agreed within ±27%, indicating that ACSM instruments are capable of stable and reproducible operation. Chemical constituents measured by the ACSM are also compared with those obtained from the continuous measurements from JST. Since the continuous measurement concentrations are adjusted to match the integrated filter measurements, these comparisons reflect the combined uncertainties of the ACSM, continuous, and filter measurements. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Differences between ACSM mass concentrations and the filter-adjusted JST continuous data are 5-27%, 4

  3. Long-range-transported Saharan dust in the Caribbean - an electron microscopy perspective of aerosol composition and modification

    NASA Astrophysics Data System (ADS)

    Kandler, Konrad; Hartmann, Markus; Ebert, Martin; Weinbruch, Stephan; Weinzierl, Bernadett; Walser, Adrian; Sauer, Daniel; Wadinga Fomba, Khanneh

    2015-04-01

    From June to July in 2013, the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) was performed in the Caribbean. Airborne aerosol sampling was performed onboard the DLR Falcon aircraft in altitudes between 300 m and 5500 m. Ground-based samples were collected at Ragged Point (Barbados, 13.165 °N, 59.432 °W) and at the Cape Verde Atmospheric Observatory (Sao Vicente, 16.864 °N, 24.868 °W). Different types of impactors and sedimentation samplers were used to collect particles between 0.1 µm and 4 µm (airborne) and between 0.1 µm and 100 µm (ground-based). Particles were analyzed by scanning electron microscopy with attached energy-dispersive X-ray analysis, yielding information on particle size, particle shape and chemical composition for elements heavier than nitrogen. A particle size correction was applied to the chemical data to yield better quantification. A total of approximately 100,000 particles were analyzed. For particles larger than 0.7 µm, the aerosol in the Caribbean during the campaign was a mixture of mineral dust, sea-salt at different aging states, and sulfate. Inside the Saharan dust plume - outside the marine boundary layer (MBL) - the aerosol is absolutely dominated by mineral dust. Inside the upper MBL, sea-salt exists as minor component in the aerosol for particles smaller than 2 µm in diameter, larger ones are practically dust only. When crossing the Soufriere Hills volcano plume with the aircraft, an extremely high abundance of small sulfate particles could be observed. At Ragged Point, in contrast to the airborne measurements, aerosol is frequently dominated by sea-salt particles. Dust relative abundance at Ragged Point has a maximum between 5 µm and 10 µm particles diameter; at larger sizes, sea-salt again prevails due to the sea-spray influence. A significant number of dust particles larger than 20 µm was encountered. The dust component in the Caribbean - airborne as well as ground

  4. Chemical composition, sources, and processes of urban aerosols during summertime in northwest China: insights from high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-12-01

    An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with a scanning mobility particle sizer (SMPS) and a multi-angle absorption photometer (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of submicron particulate matter (PM1) in Lanzhou, northwest China, during 11 July-7 August 2012. The average (PM1 mass concentration including non-refractory (PM1 (NR-(PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105 μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. Organic aerosol (OA) on average consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution organic mass spectra identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns, both with peak at ~ 07:00-11:00 (BJT: UTC +8), corresponding to the morning rush hours, while cooking-emission related OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ~ 07:00 and 15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak between ~ 08:00-13:00. The later morning and early afternoon maximum in the diurnal profiles of secondary aerosol species was likely caused by downward mixing of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during nighttime. The mass spectrum of SV-OOA was

  5. Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol

    PubMed Central

    Prather, Kimberly A.; Bertram, Timothy H.; Grassian, Vicki H.; Deane, Grant B.; Stokes, M. Dale; DeMott, Paul J.; Aluwihare, Lihini I.; Palenik, Brian P.; Azam, Farooq; Seinfeld, John H.; Moffet, Ryan C.; Molina, Mario J.; Cappa, Christopher D.; Geiger, Franz M.; Roberts, Gregory C.; Russell, Lynn M.; Ault, Andrew P.; Baltrusaitis, Jonas; Collins, Douglas B.; Corrigan, Craig E.; Cuadra-Rodriguez, Luis A.; Ebben, Carlena J.; Forestieri, Sara D.; Guasco, Timothy L.; Hersey, Scott P.; Kim, Michelle J.; Lambert, William F.; Modini, Robin L.; Mui, Wilton; Pedler, Byron E.; Ruppel, Matthew J.; Ryder, Olivia S.; Schoepp, Nathan G.; Sullivan, Ryan C.; Zhao, Defeng

    2013-01-01

    The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60–180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties. PMID:23620519

  6. Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol.

    PubMed

    Prather, Kimberly A; Bertram, Timothy H; Grassian, Vicki H; Deane, Grant B; Stokes, M Dale; Demott, Paul J; Aluwihare, Lihini I; Palenik, Brian P; Azam, Farooq; Seinfeld, John H; Moffet, Ryan C; Molina, Mario J; Cappa, Christopher D; Geiger, Franz M; Roberts, Gregory C; Russell, Lynn M; Ault, Andrew P; Baltrusaitis, Jonas; Collins, Douglas B; Corrigan, Craig E; Cuadra-Rodriguez, Luis A; Ebben, Carlena J; Forestieri, Sara D; Guasco, Timothy L; Hersey, Scott P; Kim, Michelle J; Lambert, William F; Modini, Robin L; Mui, Wilton; Pedler, Byron E; Ruppel, Matthew J; Ryder, Olivia S; Schoepp, Nathan G; Sullivan, Ryan C; Zhao, Defeng

    2013-05-01

    The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60-180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties.

  7. Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol.

    PubMed

    Prather, Kimberly A; Bertram, Timothy H; Grassian, Vicki H; Deane, Grant B; Stokes, M Dale; Demott, Paul J; Aluwihare, Lihini I; Palenik, Brian P; Azam, Farooq; Seinfeld, John H; Moffet, Ryan C; Molina, Mario J; Cappa, Christopher D; Geiger, Franz M; Roberts, Gregory C; Russell, Lynn M; Ault, Andrew P; Baltrusaitis, Jonas; Collins, Douglas B; Corrigan, Craig E; Cuadra-Rodriguez, Luis A; Ebben, Carlena J; Forestieri, Sara D; Guasco, Timothy L; Hersey, Scott P; Kim, Michelle J; Lambert, William F; Modini, Robin L; Mui, Wilton; Pedler, Byron E; Ruppel, Matthew J; Ryder, Olivia S; Schoepp, Nathan G; Sullivan, Ryan C; Zhao, Defeng

    2013-05-01

    The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60-180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties. PMID:23620519

  8. Aerosol optical and physical properties during winter monsoon pollution transport in an urban environment.

    PubMed

    Verma, S; Bhanja, S N; Pani, S K; Misra, A

    2014-04-01

    We analysed aerosol optical and physical properties in an urban environment (Kolkata) during winter monsoon pollution transport from nearby and far-off regions. Prevailing meteorological conditions, viz. low temperature and wind speed, and a strong downdraft of air mass, indicated weak dispersion and inhibition of vertical mixing of aerosols. Spectral features of WinMon aerosol optical depth (AOD) showed larger variability (0.68-1.13) in monthly mean AOD at short-wavelength (SW) channels (0.34-0.5 μm) compared to that (0.28-0.37) at long-wavelength (LW) channels (0.87-1.02 μm), thereby indicating sensitivity of WinMon AOD to fine aerosol constituents and the predominant contribution from fine aerosol constituents to WinMon AOD. WinMon AOD at 0.5 μm (AOD 0. 5) and Angstrom parameter ( α) were 0.68-0.82 and 1.14-1.32, respectively, with their highest value in December. Consistent with inference from spectral features of AOD, surface aerosol loading was primarily constituted of fine aerosols (size 0.23-3 μm) which was 60-70 % of aerosol 10- μm (size 0.23-10 μm) concentration. Three distinct modes of aerosol distribution were obtained, with the highest WinMon concentration at a mass median diameter (MMD) of 0.3 μm during December, thereby indicating characteristics of primary contribution related to anthropogenic pollutants that were inferred to be mostly due to contribution from air mass originating in nearby region having predominant emissions from biofuel and fossil fuel combustion. A relatively higher contribution from aerosols in the upper atmospheric layers than at the surface to WinMon AOD was inferred during February compared to other months and was attributed to predominant contribution from open burning emissions arising from nearby and far-off regions. A comparison of ground-based measurements with Moderate Resolution Imaging Spectroradiometer (MODIS) data showed an underestimation of MODIS AOD and α values for most of the days. Discrepancy in

  9. The Pasadena Aerosol Characterization Observatory (PACO): chemical and physical analysis of the Western Los Angeles basin aerosol

    NASA Astrophysics Data System (ADS)

    Hersey, S. P.; Craven, J. S.; Schilling, K. A.; Metcalf, A. R.; Sorooshian, A.; Chan, M. N.; Flagan, R. C.; Seinfeld, J. H.

    2011-08-01

    The Pasadena Aerosol Characterization Observatory (PACO) represents the first major aerosol characterization experiment centered in the Western/Central Los Angeles Basin. The sampling site, located on the campus of the California Institute of Technology in Pasadena, was positioned to sample a continuous afternoon influx of transported urban aerosol with a photochemical age of 1-2 h and generally free from major local contributions. Sampling spanned 5 months during the summer of 2009, which were broken into 3 regimes on the basis of distinct meteorological conditions. Regime I was characterized by a series of low pressure systems, resulting in high humidity and rainy periods with clean conditions. Regime II typified early summer meteorology, with significant morning marine layers and warm, sunny afternoons. Regime III was characterized by hot, dry conditions with little marine layer influence. Regardless of regime, organic aerosol (OA) is the most significant constituent of nonrefractory submicron Los Angeles aerosol (42, 43, and 55 % of total submicron mass in regimes I, II, and III, respectively). The overall oxidation state remains relatively constant on timescales of days to weeks (O:C = 0.44 ± 0.08, 0.55 ± 0.05, and 0.48 ± 0.08 during regimes I, II, and III, respectively), with no difference in O:C between morning and afternoon periods. Periods characterized by significant morning marine layer influence followed by photochemically favorable afternoons displayed significantly higher aerosol mass and O:C ratio, suggesting that aqueous processes may be important in the generation of secondary aerosol and oxidized organic aerosol (OOA) in Los Angeles. Online analysis of water soluble organic carbon (WSOC) indicates that water soluble organic mass (WSOM) reaches maxima near 14:00-15:00 local time (LT), but the percentage of AMS organic mass contributed by WSOM remains relatively constant throughout the day. Sulfate and nitrate reside predominantly in accumulation

  10. A new method for assessing the aerosol to rain chemical composition relationships

    NASA Astrophysics Data System (ADS)

    Bourcier, L.; Masson, O.; Laj, P.; Chausse, P.; Pichon, J. M.; Paulat, P.; Bertrand, G.; Sellegri, K.

    2012-11-01

    Measurements were conducted at three sampling sites located at different altitudes in the centre of France during two years, both in the rain and aerosol phases. The rain was sampled at a boundary layer site while the aerosol particles were collected at two different altitudes, which allow a better characterization of the vertical atmospheric column being washed out. Various chemical analyses were performed to characterize reactive (NO3-, SO42-, NH4+ and K+) and inert (7Be, 210Pb and 137Cs) species transfer from the aerosol to the rain phase. This set-up was ideal to calculate the washout ratio (WR) using different concentrations of the aerosol phase. Using the classical WR calculated with the aerosol concentration sampled at the same altitude than the rain collectors, we observed a seasonality of WR, with higher value in winter and lower value in summer for radionuclides. At the higher altitude site, local contaminations do not influence the aerosol concentration, which then should be representative of the whole atmospheric column. The annual variability is high at this site maybe because aerosol concentrations can be less concentrated than the whole atmospheric column when this later one is not well mixed. In order to increase the reliability of the WR, we propose a new method for calculating washout ratio from measurements at the rain collector level. This new calculation takes into account the height of the boundary layer, we observed that it decreased the variability of the washout ratio (for 7Be, 210Pb and NO3-), with less dependence to the season.

  11. Experimental Determination of Chemical Diffusion within Secondary Organic Aerosol Particles

    SciTech Connect

    Abramson, Evan H.; Imre, D.; Beranek, Josef; Wilson, Jacqueline; Zelenyuk, Alla

    2013-02-28

    Formation, properties, transformations, and temporal evolution of secondary organic aerosols (SOA) particles strongly depend on particle phase. Recent experimental evidence from a number of groups indicates that SOA is in a semi-solid phase, the viscosity of which remained unknown. We find that when SOA is made in the presence of vapors of volatile hydrophobic molecules the SOA particles absorb and trap them. Here, we illustrate that it is possible to measure the evaporation rate of these molecules that is determined by their diffusion in SOA, which is then used to calculate a reasonably accurate value for the SOA viscosity. We use pyrene as a tracer molecule and a-pinene SOA as an illustrative case. It takes ~24 hours for half the pyrene to evaporate to yield a viscosity of 10^8 Pa s for a-pinene. This viscosity is consistent with measurements of particle bounce and evaporation rates. We show that viscosity of 10^8 Pa s implies coalescence times of minutes, consistent with the findings that SOA particles are spherical. Similar measurements on aged SOA particles doped with pyrene yield a viscosity of 10^9 Pa s, indicating that hardening occurs with time, which is consistent with observed decrease in water uptake and evaporation rate with aging.

  12. Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

    NASA Astrophysics Data System (ADS)

    Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

    2014-11-01

    The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

  13. Aerosol bolus transport through a hollow airway cast by steady flow in different gases

    SciTech Connect

    Briant, J.K.; Lippmann, M. )

    1993-07-01

    Transport of aerosol through the airways of a hollow cast of a canine tracheobronchial tree was measured for steady flow in different gas mixtures. A small bolus of 0.5-[mu]m aerosol particles was inserted as a tracer of convective motion in the flow at the entrance of the trachea, and particles were collected and counted as they arrived at a flow-balanced sampling bag at a peripheral segment of the cast. Transport was fastest in the gas of highest kinematic viscosity (helium), and slowest in the gas of lowest kinematic viscosity (sulfur hexafluoride). This is consistent with the lubrication theory that describes an axial core in the divergent flow field of the bronchial tree. The finer core in helium transports the particles at a greater velocity to distal airways. Transport of gases through the in vivo respiratory tract should also be influenced by these fluid mechanics of convection resembling Poiseuille flow that is substantially modified according to lubrication theory. As predicted by some other investigators, gas and aerosol particles penetrate much deeper into the lungs than the volumetric depth of inhalation. 25 refs., 7 figs., 2 tabs.

  14. Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically-resolved aerosol fluxes

    NASA Astrophysics Data System (ADS)

    Farmer, D. K.; Kimmel, J. R.; Phillips, G.; Docherty, K. S.; Worsnop, D. R.; Sueper, D.; Nemitz, E.; Jimenez, J. L.

    2010-12-01

    Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM1 fluxes. Average deposition velocity for total NR-PM1 aerosol at noon was 2.05 ± 0.04 mm/s. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm/s and are dominated by deposition of ammonium sulphate.

  15. Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

    NASA Astrophysics Data System (ADS)

    Farmer, D. K.; Kimmel, J. R.; Phillips, G.; Docherty, K. S.; Worsnop, D. R.; Sueper, D.; Nemitz, E.; Jimenez, J. L.

    2011-06-01

    Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM1 fluxes. Average deposition velocities for total NR-PM1 aerosol at noon were 2.05 ± 0.04 mm s-1. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s-1 and are dominated by deposition of ammonium sulphate.

  16. Transport and scavenging of biomass burning aerosols in the maritime continent

    NASA Astrophysics Data System (ADS)

    Lee, H. H.; Wang, C.

    2014-12-01

    Biomass burning frequently occurs in summertime over the maritime continent, especially in Malaysia peninsula, Sumatra, and Borneo. Under certain weather conditions, particulate matters emitted from such fires cause degrade of air quality and thus occurrence of often weekly long haze in downwind locations such as Singapore. It is possible that these biomass burning aerosols may have influenced convective clouds in the maritime continent though such cases have not been well simulated and understood. In order to improve understanding of the spatiotemporal coverage and influence of biomass burning aerosols in the maritime continent, we have used the Weather Research and Forecasting (WRF) model to study the transport of biomass burning aerosols from Malaysia peninsula, Sumatra, and Borneo, using biomass burning emissions from the Fire INventory from NCAR (FINN) version 1.0. We choose to use emissions from the month of August because the annual emissions peak often occurs within this month. Based on a multi-year ensemble simulation, we have examined the influences of various meteorological regimes on the aerosol transport and wet removal.

  17. Sulfate aerosol as a potential transport medium of radiocesium from the Fukushima nuclear accident.

    PubMed

    Kaneyasu, Naoki; Ohashi, Hideo; Suzuki, Fumie; Okuda, Tomoaki; Ikemori, Fumikazu

    2012-06-01

    To date, areas contaminated by radionuclides discharged from the Fukushima Dai-ichi nuclear power plant accident have been mapped in detail. However, size of the radionuclides and their mixing state with other aerosol components, which are critical in their removal from the atmosphere, have not yet been revealed. We measured activity size distributions of (134)Cs and (137)Cs in aerosols collected 47 days after the accident at Tsukuba, Japan, and found that the activity median aerodynamic diameters of (134)Cs and (137)Cs in the first sample (April 28-May 12) were 0.54 and 0.53 μm, respectively, and those in the second sample (May 12-26) were both 0.63 μm. The activity size distributions of these radiocesium were within the accumulation mode size range and almost overlapped with the mass size distribution of non-sea-salt sulfate aerosol. From the analysis of other aerosol components, we found that sulfate was the potential transport medium for these radionuclides, and resuspended soil particles that attached radionuclides were not the major airborne radioactive substances at the time of measurement. This explains the relatively similar activity sizes of radiocesium measured at various sites during the Chernobyl accident. Our results can serve as basic data for modeling the transport/deposition of radionuclides.

  18. Chemistry and processes of aerosols at Mt. Bachelor, a high elevation site in the Pacific Northwest U.S.: influences from regional transport and wildfire plumes

    NASA Astrophysics Data System (ADS)

    Collier, S.; Zhou, S.; Hee, J.; Jaffe, D. A.; Wigder, N. L.; Zhang, Q.

    2013-12-01

    The Mt. Bachelor Observatory (MBO; 43.9794° N, 121.6885° W, altitude 2,763 m asl)) has been used for 10 years to study wildfire impacts on CO, O3, aerosols and other pollutants in the free troposphere. In the summer of 2013, we deployed an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) at the summit of MBO to obtain high resolution data on the chemical composition of aerosols, with an emphasis on biomass burning aerosols, as part of the DOE sponsored Biomass Burning Observation Project (BBOP). A main goal of BBOP is to study the downwind time evolution of the microphysical, morphological, chemical, hygroscopic, and optical properties of carbonaceous aerosol generated by biomass burning (BB). MBO is an ideal location for studying remote and high elevation aerosol and the location allows for free tropospheric air masses to be sampled during the night and air coming from the boundary layer during daytime. Our ground-based measurements are also complimentary to simultaneous aircraft BB plume measurements. Our observations indicate a dynamic variation in the chemical composition and physical properties of aerosols with repeatable diurnal patterns. Periods of low particulate matter (PM) loading show distinctly oxidized organic aerosol (OA) with oxygen-to-carbon atomic ratios (O/C) reaching above 1 as well as containing an ammonium sulfate fraction of up to 50% of submicron aerosol (PM1) mass. Methanesulfonic acid (MSA) is also present during low loading periods, which, together with an aerosol size distribution characteristic of a droplet accumulation mode centered at 500-600 nm in vacuum aerodynamic diameter (Dva), suggests that aqueous-phase processing plays an important role in the regional aerosol sampled at this site. During these same measurements, contrasting periods of higher loading and markedly different characteristics have been observed due to effects from injection of wildfire plumes into air masses transported to MBO

  19. The Effect of the Anionic Surfactant Aerosol-80 on the Transport of Cryptosporidium parvum Oocysts through Soil

    NASA Astrophysics Data System (ADS)

    Jacobson, A. R.; Powelson, D.; Darnault, C.

    2012-12-01

    Transport of the pathogenic protozoan Cryptosporidium parvum through soils threatens ground and surface waters. C. parvum may be introduced into soils in the manure of infected calves. The presence of other chemicals in the soil applied as or with amendments, may affect the transport of the C. parvum oocysts. Surfactants, which are used in many herbicide formulations, decrease water tension and may disrupt the air-water interface where oocysts are thought to accumulate. We investigate the effect of the anionic surfactant Aerosol-80, at two concentrations, on the transport of C. parvum oocysts by unsaturated flow through "undisturbed" soil columns from Illinois and Utah. Following each experiment oocysts in the leachate and distributed throughout the soil profile are quantified by real time PCR. We find that the presence of the surfactant accelerates the transport of the oocysts through preferential flow paths. On the other hand, when connected macropores are not present in the soils, the presence of the surfactant retards the transport of the oocysts through the soil matrix by straining oocyst-surfactant-Ca flocs. Surfactant efficacy is affected by soil type.

  20. Stratospheric Sulphur - 3D Chemical Transport Model Simulations and MIPAS/ENVISAT Satellite Measurements

    NASA Astrophysics Data System (ADS)

    Günther, Annika; Höpfner, Michael; Sinnhuber, Björn-Martin; Stiller, Gabriele; Clarmann, Thomas

    2016-04-01

    In this study processes that regulate the atmospheric distribution, and the budget of carbonyl sulphide (OCS), sulphur dioxide (SO2) and stratospheric sulphate aerosols are investigated in the upper troposphere / lower stratosphere. Sulphate aerosols impact the Earth's climate by backscattering parts of the incoming solar radiation. This negative radiative forcing can lead to reduced surface temperatures and is thought of as one reason for the recent global warming "hiatus". Our study is based on the comparison of modeled and observed data. An isentropic chemical transport model is used, spanning the region from 330 to 3000 K potential temperature (~ 8 - 66 km), driven by ERA-Interim Reanalysis data. The simulations are compared to observations from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), a limb sounder on the satellite ENVISAT that was operational from July 2002 to April 2012. The focus of our study lies on volcanically emitted SO2 and its dispersion, as main precursor for sulphate aerosol during volcanically perturbed times, with its simulated distribution and lifetime, in comparison to MIPAS SO2 measurements. Moreover data for OCS, as the main source for stratospheric sulphur during volcanically quiescent periods. Furthermore, first results of sulphuric aerosol-mass retrievals from MIPAS are presented. These will be combined with the gaseous sulphur species to obtain a global budget of stratospheric sulphur.

  1. Possible indicators of long-range transport for aerosol emitted from various source regions in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Park, S.; Kim, C.

    2013-12-01

    Air pollutant is affected by both long-range transboundary processes and local air pollution emission. Therefore it is important to identify the origin of air pollutant, for example, by classifying air pollutants into long-range transport (LRT) dominant process and local emission dominant (LED) cases. This study proposed several chemical and physical indicators of LRT process of aerosol concentrations observed at Korean peninsula. In order to identify the source regions and to estimate the contributions of both LRT and LED, we performed Lagrangian particle dispersion model(FLEXPART) and selected high pollution days over the three source regions in China inland and one Korea peninsula defined in this study; LRT-I to III and LED case. Next, we investigated the chemical and physical characteristics of LRT process of aerosol, and contrasted to those in the LED case over the Northeast Asia. We examined the difference of both modeled features simulated by CMAQ and as well measured aerosol optical properties of satellite-based sensor MODIS and AERONET data. Modeling study showed that the most effective indicator is the sulfur conversion ratios such as SO42-/(SO2+ SO42-) and SO42-/ SO2 for high sulfate condition. The ratio of N-containing species such as NOx (or NOy) to CO were the next best alternative indicators. In the meteorological fields, the results showed that pressure pattern and streamline flow are similar on a case by case basis. For observational physical features, we obtained the spatial distributions of the mean AOD, fine mode fraction (FMF), angstrom exponent (AE) by taking the average of MODIS aerosol products for the each analysis period. The highest AOD was found over the industrialized coastal region regardless of cases. AERONET data showed that aerosol size distribution showed significantly higher concentration of fine-mode particle in LED cases in comparison with that of LRT groups, suggesting that the amplitude fine modes of LRT relative to LED could

  2. Transport of surgically produced aerosols in an operating room.

    PubMed

    Buchanan, C R; Dunn-Rankin, D

    1998-06-01

    The particle transport characteristics of two ventilation configurations commonly used in hospital operating rooms (ORs), cross-flow and impinging-flow ventilation, were investigated. The computational fluid dynamics software FLUENT was used to simulate turbulent airflow with mixed convection in a three-dimensional, rectangular OR. Two OR personnel, a patient, OR spotlights, an anesthetics cart, and an operating table were represented in the room. Heat loads from the personnel, patient, and lights affected the airflow through buoyancy. Particles produced at the operation site with various sizes and initial conditions were tracked through the room. A stochastic model was used to include the random effects of turbulence on particle trajectories. Simulation results show that heat loads from the personnel, patient, and OR spotlights had an important effect on the airflow through natural convection. Particle trajectories were influenced greatly by the flow field structure, particle launch position, and turbulence in the flow, and somewhat by particle size. However, particle paths were insensitive to the launch velocity. Virtually identical trajectories were obtained for particles with launch velocities ranging from 0 to 1 m/sec in magnitude. Changes in ventilation configuration dramatically affected particle transport. The cross-flow ventilation configuration performed better, based on the criteria of removing particles from the breathing zone of room occupants. Proper flow field design and contaminant source placement can be used to control particle transport. Numerical simulations allow quick and inexpensive comparisons between room designs and provide details about airflow and contaminant transport.

  3. Organic aerosol characterization by complementary measurements of chemical bonds and molecular fragments

    NASA Astrophysics Data System (ADS)

    Russell, Lynn M.; Bahadur, Ranjit; Hawkins, Lelia N.; Allan, James; Baumgardner, Darrel; Quinn, Patricia K.; Bates, Timothy S.

    2009-12-01

    Organic aerosol chemical markers from normalized concentrations of independent measurements of mass fragments (using Aerosol Mass Spectrometry, AMS) are compared to bond-based functional groups (from Fourier Transform Infrared spectroscopy, FTIR) during eight field projects in the western hemisphere. Several field projects show weak correlations between alcohol group fractions and m/ z 60 fractions, consistent with the organic hydroxyl groups and the fragmentation of saccharides, but the weakness of the correlations indicate chemical differences among the relationships for ambient aerosols in different regions. Carboxylic acid group fractions and m/ z 44 fractions are correlated weakly for three projects, with correlations expected for aerosols dominated by di-acid compounds since their fragmentation is typically dominated by m/ z 44. Despite differences for three projects with ratios of m/ z 44 to m/ z 57 fragments less than 10, five projects showed a linear trend between the project-average m/ z 44 to m/ z 57 ratio and the ratio of acid and alkane functional groups. While this correlation explains only a fraction of the fragment and bond variability measured, the consistency of this relationship at multiple sites indicates a general agreement with the interpretation of the relative amount of m/ z 44 as a carboxylic acid group marker and m/ z 57 as an alkane group marker.

  4. Hygroscopic properties of the Paris urban aerosol in relation to its chemical composition

    NASA Astrophysics Data System (ADS)

    Kamilli, K. A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.

    2014-01-01

    Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m-3, e.g., during winter.

  5. Hygroscopic properties of the Paris urban aerosol in relation to its chemical composition

    NASA Astrophysics Data System (ADS)

    Kamilli, K. A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.

    2013-05-01

    Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site LHVP in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m3, e.g. during winter.

  6. Evaluation of long range transport of fossil fuel originated organic aerosol at a background site in Northeast Asia

    NASA Astrophysics Data System (ADS)

    Hwang, Eun Jin; Lee, Ji Yi; Park, Jin Soo; Lee, Seok Jo; Kim, Hyun Jae; Jeon, Ha Eun; Sung, Min Young

    2013-04-01

    Northeast Asia is heavy air pollution region due to usage of large amounts of fossil fuel. In addition, meteorological conditions represented as prevailing westerlies in Northeast Asia region causes long range transport of anthropogenic pollutants emitted from China to Korea and Japan and even the United States across the Pacific Ocean (Bey et al., 2001). The Baengnyeong Island of Korea is located at the northwestern part of the Korean peninsula and close by North Korea and China, thus this site is regarded as an ideal place for background air measurements in Northeast Asia. Also, it has low local anthropogenic emissions and is frequently influenced by various air masses from China and North Korea in the Island. In this study, we performed intensive sampling during summer and winter in the Baengnyeong Island and analyzed various organic compounds including fossil fuel originated organic markers such as hopanes and PAHs using thermal desorption two dimensional gas chromatography with time of flight mass spectrometry (TD-GC×GC-TOFMS). We also analyzed ~20 urban aerosol samples collected at Seoul, a representative urban site in Northeast Asia region to compare organic compounds distributions of aerosol samples at the Baengnyeong Island. By applying air mass back trajectory analysis and comparing organic compounds distributions in aerosol samples of the Baengnyeong Island and Seoul, the impact of long-range transport of fossil fuel originated organic pollutants at a background site in Northeast Asia were evaluated. (References) Bey, I., Jacob, D.J., Logan, J.A., Yantosca, R.M., 2001. Asian chemical outflow to the Pacific in spring: origins, pathways, and budgets. Journal of Geophysical Research-Atmosphere 106, 23097-23113.

  7. Evaluate and characterize mechanisms controlling transport, fate, and effects of army smokes in the aerosol wind tunnel: Transport, transformations, fate, and terrestrial ecological effects of hexachloroethane obscurant smokes

    SciTech Connect

    Cataldo, D.A.; Ligotke, M.W.; Bolton, H. Jr.; Fellows, R.J.; Van Voris, P.; McVeety, B.D.; Li, Shu-mei W.; McFadden, K.M.

    1989-09-01

    The terrestrial transport, chemical fate, and ecological effects of hexachloroethane (HC) smoke were evaluated under controlled wind tunnel conditions. The primary objectives of this research program are to characterize and assess the impacts of smoke and obscurants on: (1) natural vegetation characteristic of US Army training sites in the United States; (2) physical and chemical properties of soils representative of these training sites; and (3) soil microbiological and invertebrate communities. Impacts and dose/responses were evaluated based on exposure scenarios, including exposure duration, exposure rate, and sequential cumulative dosing. Key to understanding the environmental impacts of HC smoke/obscurants is establishing the importance of environmental parameters such as relative humidity and wind speed on airborne aerosol characteristics and deposition to receptor surfaces. Direct and indirect biotic effects were evaluated using five plant species and two soil types. HC aerosols were generated in a controlled atmosphere wind tunnel by combustion of hexachloroethane mixtures prepared to simulate normal pot burn rates and conditions. The aerosol was characterized and used to expose plant, soil, and other test systems. Particle sizes of airborne HC ranged from 1.3 to 2.1 {mu}m mass median aerodynamic diameter (MMAD), and particle size was affected by relative humidity over a range of 20% to 85%. Air concentrations employed ranged from 130 to 680 mg/m{sup 3}, depending on exposure scenario. Chlorocarbon concentrations within smokes, deposition rates for plant and soil surfaces, and persistence were determined. The fate of principal inorganic species (Zn, Al, and Cl) in a range of soils was assessed.

  8. Chemical Composition of Atmospheric Aerosols Above a Pristine South East Asian Rainforest

    NASA Astrophysics Data System (ADS)

    Robinson, N. H.; Allan, J. D.; Williams, P. I.; Coe, H.; Hamilton, J.; Chen, Q.; Martin, S.; Trembath, J.

    2009-04-01

    conjunction with a constant pressure inlet. The aerosols' chemical origins have been further investigated by comparing these spectra to chamber experiments, mass spectral libraries and data from comparable experiments in other locations. These data are also being analysed in conjunction with offline techniques applied to samples collected using filters and a Particle-Into-Liquid Sampler (PILS). Methods used include liquid chromatography and comprehensive two-dimensional gas chromatography coupled to time of flight mass spectrometry. These techniques provide a more detailed chemical characterisation of the SOA and water soluble organic carbon, allowing direct links back to gas phase precursors. In conjunction with the field measurements, a programme of chamber experiments is being carried out at Manchester as part of the ACES project. This will generate comparable SOA under controlled conditions and subjecting them to similar analysis.

  9. Contribution of long-range transported aerosols to aerosol optical and physical properties: 3-year measurements at Gosan, Korea

    NASA Astrophysics Data System (ADS)

    Heo, J.; Kim, S. W.; Kim, J. H.; Ogren, J. A.; Yoon, S. C.

    2015-12-01

    Recently, more attentions have been paid to air quality in East Asia due to the enhanced loading of atmospheric pollutants related to rapid industrialization. Gosan Climate Observatory (GCO), Korea is regarded as an ideal site to study the transport of atmospheric pollutants because it is frequently influenced by various airmasses from China, Korea, Japan and Pacific Ocean. In order to understand aerosol optical and physical properties according to airmass transport routes, three-year (2012-2014) continuous measurements of aerosol scattering/absorption coefficient and number size distribution were analyzed, together with 48-hour backward trajectory calculations. The averaged aerosol absorption (σa) and scattering coefficient (σs) for airmasses transported from North China (NC; 36% of all trajectories) were 6.65 Mm-1 and 94.72 Mm-1 at 550 nm wavelength, respectively, which were similar to those for stagnant airmasses (ST; 22% of all trajectories; σa: 6.26 Mm-1, σs: 93.99 Mm-1). The highest values of σa (7.03 Mm-1) and σs (108.34 Mm-1) were observed when airmasses were traveled from South China (SC; 11% of all trajectories). σa and σs for airmasses from Korean Peninsula (KP; 7% of all trajectories) and Pacific Ocean (PO; 14% of all trajectories; in parenthesis) were 5.63 (2.76) Mm-1 and 73.63 (50.93) Mm-1, respectively. Compared to other airmasses, the higher values of Scattering Angstrom Exponent (SAE) for ST (1.65) is thought to be the build-up of anthropogenic fine particulate pollutants. The Absorption Angstrom Exponent (AAE) was estimated to be 1.32 for NC airmass and 1.02 for SC airmass. Over the study period, 130 days of total 557 days were identified as new particle formation and growth event (NPF) from Scanning Mobility Particle Sizer (SMPS) measurements by Cyclostationary Empirical Orthogonal Function (CSEOF) approach. Especially, 55.4% (72 days) of total 130 NPF days were found when a cold and dry airmass comes from NC after passing the frontal

  10. Aerosol Chemical and Physical Properties Observed over Puerto Rico in the Tropical North Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Jusino-Atresino, R.; Xia, L.; Song, F.; Gao, Y.

    2008-12-01

    Tropospheric aerosols that originate in Africa and are transported over the Atlantic Ocean have potential impacts over the Caribbean region. To investigate aerosol properties over this region, air sampling was conducted at San Juan Cape (18.46°N, 66.12°W), Puerto Rico during the summer months in 2006. Aerosol samples were collected by both commercial PM2.5 sampler and in-house fabricated TSP sampler. Analyses of aerosols were made through the use of the following instrumental methods: (1)Ion Chromatography for the determinations of water-soluble cations (sodium, ammonium, potassium, magnesium and calcium) and anions (fluoride, acetate, propionate, methanesulfonate, chloride, nitrate, succinate, malonate, sulfate and oxalate); (2)Inductively Coupled Plasma Mass Spectrometry for the concentrations of selected trace elements (Al, Fe, Mn, Sc, Cd, Pb, Sb, Ni, Co, Cr, Cu, Zn and V); (3)Scanning Electron Microscopy for individual aerosol particle characterization. Crustal enrichment factors were calculated to determine the strength of crustal source. Preliminary results indicate that sodium (22 - 99 μg m- 3) and ammonium (1.1 - 50 μg m-3) were the major cations and chloride (1.5 - 99 μg m-3) and sulfate (35 μg m-3) were the dominant anions. Malonate (3.8 - 6.9 μg m- 3) was the most abundant organic anion. Atmospheric concentrations of iron ranged 0.30 - 3.3 ng m- 3. The elements, Sc, Cd, Pb, Sb, Ni, Co, Cr, Cu, Zn and V, were enriched by factors of 600 to 40,000 relative to their natural abundance in crustal soil. Principal components analysis indicates six assemblages of fifteen types of aerosol particles, dominated by Si - rich particles.

  11. Chemical Analysis of Fractionated Halogens in Atmospheric Aerosols Collected in Okinawa, Japan

    NASA Astrophysics Data System (ADS)

    Tsuhako, A.; Miyagi, Y.; Somada, Y.; Azechi, S.; Handa, D.; Oshiro, Y.; Murayama, H.; Arakaki, T.

    2013-12-01

    Halogens (Cl, Br and I) play important roles in the atmosphere, e.g. ozone depletion by Br during spring in Polar Regions. Sources of halogens in atmospheric aerosols are mainly from ocean. But, for example, when we analyzed Br- with ion chromatography, its concentrations were almost always below the detection limit, which is also much lower than the estimated concentrations from sodium ion concentrations. We hypothesized that portions of halogens are escaped to the atmosphere, similar to chlorine loss, changed their chemical forms to such as BrO3- and IO3-, and/or even formed precipitates. There was few reported data so far about fractionated halogen concentrations in atmospheric aerosols. Thus, purpose of this study was to determine halogen concentrations in different fractions; free ion, water-soluble chemically transformed ions and precipitates using the authentic aerosols. Moreover, we analyzed seasonal variation for each fraction. Atmospheric aerosol samples were collected at Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS) of Okinawa, Japan during January 2010 and August 2013. A high volume air sampler was used for collecting total particulate matters on quartz filters on a weekly basis. Ultrapure water was used to extract water-soluble factions of halogens. The extracted solutions were filtered with the membrane filter and used for chemical analysis with ion chromatography and ICP-MS. Moreover, the total halogens in aerosols were obtained after digesting aerosols with tetramethylammonium hydroxide (TMAH) using the microwave and analysis with ICP-MS. For Cl, water-soluble Cl- accounted for about 70% of the estimates with Na content. No other forms of water-soluble Cl were found. About 30% of Cl was assumed volatilized to the gas-phase. For Br, water-soluble Br accounted for about 43% of the estimates with Na content, and within the 43%, about 10% of Br was not in the form of Br-. About 46% of Br was assumed volatilized to the gas-phase. For I

  12. Biomass burning aerosol over the Amazon during SAMBBA: impact of chemical composition on radiative properties

    NASA Astrophysics Data System (ADS)

    Morgan, William; Allan, James; Flynn, Michael; Darbyshire, Eoghan; Hodgson, Amy; Liu, Dantong; O'shea, Sebastian; Bauguitte, Stephane; Szpek, Kate; Langridge, Justin; Johnson, Ben; Haywood, Jim; Longo, Karla; Artaxo, Paulo; Coe, Hugh

    2014-05-01

    Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. Globally, biomass burning aerosols are thought to exert a small warming effect but with the uncertainty being 4 times greater than the central estimate. On regional scales, the impact is substantially greater, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, both in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated

  13. Thermodynamic and transport properties of gaseous tetrafluoromethane in chemical equilibrium

    NASA Technical Reports Server (NTRS)

    Hunt, J. L.; Boney, L. R.

    1973-01-01

    Equations and in computer code are presented for the thermodynamic and transport properties of gaseous, undissociated tetrafluoromethane (CF4) in chemical equilibrium. The computer code calculates the thermodynamic and transport properties of CF4 when given any two of five thermodynamic variables (entropy, temperature, volume, pressure, and enthalpy). Equilibrium thermodynamic and transport property data are tabulated and pressure-enthalpy diagrams are presented.

  14. Simulating Secondary Inorganic Aerosols using the chemistry transport model MOCAGE version R2.15.0

    NASA Astrophysics Data System (ADS)

    Guth, J.; Josse, B.; Marécal, V.; Joly, M.

    2015-04-01

    In this study we develop a Secondary Inorganic Aerosol (SIA) module for the chemistry transport model MOCAGE developed at CNRM. Based on the thermodynamic equilibrium module ISORROPIA II, the new version of the model is evaluated both at the global scale and at the regional scale. The results show high concentrations of secondary inorganic aerosols in the most polluted regions being Europe, Asia and the eastern part of North America. Asia shows higher sulfate concentrations than other regions thanks to emissions reduction in Europe and North America. Using two simulations, one with and the other without secondary inorganic aerosol formation, the model global outputs are compared to previous studies, to MODIS AOD retrievals, and also to in situ measurements from the HTAP database. The model shows a better agreement in all geographical regions with MODIS AOD retrievals when introducing SIA. It also provides a good statistical agreement with in situ measurements of secondary inorganic aerosol composition: sulfate, nitrate and ammonium. In addition, the simulation with SIA gives generally a better agreement for secondary inorganic aerosols precursors (nitric acid, sulfur dioxide, ammonia) in particular with a reduction of the Modified Normalised Mean Bias (MNMB). At the regional scale, over Europe, the model simulation with SIA are compared to the in situ measurements from the EMEP database and shows a good agreement with secondary inorganic aerosol composition. The results at the regional scale are consistent with those obtained with the global simulations. The AIRBASE database was used to compare the model to regulated air quality pollutants being particulate matter, ozone and nitrogen dioxide concentrations. The introduction of the SIA in MOCAGE provides a reduction of the PM2.5 MNMB of 0.44 on a yearly basis and even 0.52 on a three spring months period (March, April, May) when SIA are maximum.

  15. Characterization of Transport Errors in Chemical Forecasts from a Global Tropospheric Chemical Transport Model

    NASA Technical Reports Server (NTRS)

    Bey, I.; Jacob, D. J.; Liu, H.; Yantosca, R. M.; Sachse, G. W.

    2004-01-01

    We propose a new methodology to characterize errors in the representation of transport processes in chemical transport models. We constrain the evaluation of a global three-dimensional chemical transport model (GEOS-CHEM) with an extended dataset of carbon monoxide (CO) concentrations obtained during the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft campaign. The TRACEP mission took place over the western Pacific, a region frequently impacted by continental outflow associated with different synoptic-scale weather systems (such as cold fronts) and deep convection, and thus provides a valuable dataset. for our analysis. Model simulations using both forecast and assimilated meteorology are examined. Background CO concentrations are computed as a function of latitude and altitude and subsequently subtracted from both the observed and the model datasets to focus on the ability of the model to simulate variability on a synoptic scale. Different sampling strategies (i.e., spatial displacement and smoothing) are applied along the flight tracks to search for systematic model biases. Statistical quantities such as correlation coefficient and centered root-mean-square difference are computed between the simulated and the observed fields and are further inter-compared using Taylor diagrams. We find no systematic bias in the model for the TRACE-P region when we consider the entire dataset (i.e., from the surface to 12 km ). This result indicates that the transport error in our model is globally unbiased, which has important implications for using the model to conduct inverse modeling studies. Using the First-Look assimilated meteorology only provides little improvement of the correlation, in comparison with the forecast meteorology. These general statements can be refined when the entire dataset is divided into different vertical domains, i.e., the lower troposphere (less than 2 km), the middle troposphere (2-6 km), and the upper troposphere (greater than

  16. Daily and hourly chemical impact of springtime transboundary aerosols on Japanese air quality

    NASA Astrophysics Data System (ADS)

    Moreno, T.; Kojima, T.; Amato, F.; Lucarelli, F.; de la Rosa, J.; Calzolai, G.; Nava, S.; Chiari, M.; Alastuey, A.; Querol, X.; Gibbons, W.

    2013-02-01

    The regular eastward drift of transboundary aerosol intrusions from the Asian mainland into the NW Pacific region has a pervasive impact on air quality in Japan, especially during springtime. Analysis of 24-h filter samples with Inductively Coupled Plasma Atomic Emission Spectroscopy (ICP-AES) and Mass Spectrometry (ICP-MS), and hourly Streaker with Particle Induced X-ray Emission (PIXE) samples collected continuously for six weeks reveal the chemistry of successive waves of natural mineral desert dust ("Kosa") and metalliferous sulphatic pollutants arriving in western Japan during spring 2011. The main aerosol sources recognised by Positive Matrix Factorization (PMF) analysis of Streaker data are mineral dust and fresh sea salt (both mostly in the coarser fraction PM2.5-10), As-bearing sulphatic aerosol (PM0.1-2.5), metalliferous sodic particulate matter (PM) interpreted as aged, industrially contaminated marine aerosol, and ZnCu-bearing aerosols. Whereas mineral dust arrivals are typically highly transient, peaking over a few hours, sulphatic intrusions build up and decline more slowly, and are accompanied by notable rises in ambient concentrations of metallic trace elements such as Pb, As, Zn, Sn and Cd. The magnitude of the loss in regional air quality due to the spread and persistence of pollution from mainland Asia is especially clear when cleansing oceanic air advects westward across Japan, removing the continental influence and reducing concentrations of the undesirable metalliferous pollutants by over 90%. Our new chemical database, especially the Streaker data, demonstrates the rapidly changing complexity of ambient air inhaled during these transboundary events, and implicates Chinese coal combustion as the main source of the anthropogenic aerosol component.

  17. Daily and hourly chemical impact of springtime transboundary aerosols on Japanese air quality

    NASA Astrophysics Data System (ADS)

    Moreno, T.; Kojima, T.; Amato, F.; Lucarelli, F.; Nava, S.; de la Rosa, J.; Calzolai, G.; Chiari, M.; Alastuey, A.; Querol, X.; Gibbons, W.

    2012-09-01

    The regular eastward drift of transboundary aerosol intrusions from the Asian mainland into the NW Pacific region has a~pervasive impact on air quality in Japan, especially during springtime. Analysis of 24-h filter samples (ICP-AES and ICP-MS) and hourly Streaker (PIXE) samples of particulate matter collected continuously for six weeks reveal the chemistry of successive waves of natural mineral desert dust ("Kosa") and metalliferous sulphatic pollutants arriving in Western Japan during spring 2011. The main aerosol sources recognised by PMF analysis of Streaker data are mineral dust and fresh sea salt (both mostly in the coarser fraction PM2.5-10), As-bearing sulphatic aerosol (PM0.1-2.5), metalliferous sodic PM interpreted as aged, industrially contaminated marine aerosol, and ZnCu-bearing aerosols. Whereas mineral dust arrivals are typically highly transient, peaking over a few hours, sulphatic intrusions build up and decline more slowly, and are accompanied by notable rises in ambient concentrations of metallic trace elements such as Pb, As, Zn, Sn and Cd. The magnitude of the loss in regional air quality due to the spread and persistence of pollution from mainland Asia is especially clear when cleansing oceanic air advects westward across Japan, removing the continental influence and reducing concentrations of the more undesirable metalliferous pollutants by over 90%. Our new chemical database, especially the Streaker data, demonstrates the rapidly changing complexity of ambient air inhaled during these transboundary events, and implicates Chinese coal combustion as the main source of the anthropogenic aerosol component.

  18. Persistence and transport potential of chemicals in a multimedia environment

    SciTech Connect

    van de Meent, D.; McKone, T.E.; Parkerton, T.; Matthies, M.; Scheringer, M.; Wania, F.; Purdy, R.; Bennett, D.H.

    2000-02-01

    Persistence in the environment and potential for long-range transport are related since time in the environment is required for transport. A persistent chemical will travel longer distances than a reactive chemical that shares similar chemical properties. Scheringer (1997) has demonstrated the correlation between persistence and transport distance for different organic chemicals. However, this correlation is not sufficiently robust to predict one property from the other. Specific chemicals that are persistent mayor may not exhibit long-range transport potential. Persistence and long-range transport also present different societal concerns. Persistence concerns relate to the undesired possibility that chemicals produced and used now may somehow negatively affect future generations. Long-range transport concerns relate to the undesired presence of chemicals in areas where these compounds have not been used. Environmental policy decisions can be based on either or both considerations depending on the aim of the regulatory program. In this chapter, definitions and methods for quantifying persistence and transport potential of organic chemicals are proposed which will assist in the development of sound regulatory frameworks.

  19. The long range transport of sulfurous aerosol to Scandinavia

    SciTech Connect

    Ottar, B.

    1980-01-01

    Results of the LRTAP program and other European studies are discussed which show that considerable long-range transport of air pollutants from the UK and central Europe to Scandinavia occurs. Data are examined which reveal that the sulfate deposition pattern in Scandinavia is largely governed by precipitation and wind direction and that sulfates deposition reaches maximum values of 3 to 5 metric tons/sq km in southern Scandinavia. The contribution from precipitation is found to outweigh the dry deposition, particularly in southern Norway.

  20. Development of aerosol assisted chemical vapor deposition for thin film fabrication

    NASA Astrophysics Data System (ADS)

    Maulana, Dwindra Wilham; Marthatika, Dian; Panatarani, Camellia; Mindara, Jajat Yuda; Joni, I. Made

    2016-02-01

    Chemical vapor deposition (CVD) is widely used to grow a thin film applied in many industrial applications. This paper report the development of an aerosol assisted chemical vapor deposition (AACVD) which is one of the CVD methods. Newly developed AACVD system consists of a chamber of pyrex glass, two wire-heating elements placed to cover pyrex glass, a substrate holder, and an aerosol generator using an air brush sprayer. The temperature control system was developed to prevent condensation on the chamber walls. The control performances such as the overshoot and settling time were obtained from of the developed temperature controller. Wire-heating elements were controlled at certain setting value to heat the injected aerosol to form a thin film in the substrate. The performance of as-developed AACVD system tested to form a thin film where aerosol was sprayed into the chamber with a flow rate of 7 liters/minutes, and vary in temperatures and concentrations of precursor. The temperature control system have an overshoot around 25 °C from the desired set point temperature, very small temperature ripple 2 °C and a settling time of 20 minutes. As-developed AACVD successfully fabricated a ZnO thin film with thickness of below 1 µm. The performances of system on formation of thin films influenced by the generally controlled process such as values of setting temperature and concentration where the aerosol flow rate was fixed. Higher temperature was applied, the more uniform ZnO thin films were produced. In addition, temperature of the substrate also affected on surface roughness of the obtained films, while concentration of ZnO precursor determined the thickness of produce films. It is concluded that newly simple AACVD can be applied to produce a thin film.

  1. Online hygroscopicity and chemical measurement of urban aerosol in Shanghai, China

    NASA Astrophysics Data System (ADS)

    Wang, Xinning; Ye, Xingnan; Chen, Hong; Chen, Jianmin; Yang, Xin; Gross, Deborah S.

    2014-10-01

    Submicron aerosol hygroscopicity and composition were simultaneously measured with a Hygroscopicity-Tandem Differential Mobility Analyzer (HTDMA) in-line with an Aerosol Time-of-Flight mass spectrometer (ATOFMS) in wintertime of 2009 in Shanghai. 250 nm dry diameter aerosol particles were humidified (85% RH) and selected based on their hygroscopicity. Two Growth Factor (GF) modes were observed persistently: a weak nearly-hydrophobic (NH) mode with GF at around 1.05 and a strong hydrophilic mode with GF around 1.46. Aerosol particles at different GFs were chemically analyzed by ATOFMS to link the aerosol hygroscopicity and chemistry. Particles were grouped into five major classes: inorganic dust/ash, biomass burning particles (BB), elemental carbon and organic carbon mixed particles (ECOC), Amine rich organic carbon particles (OC-Amine), and high mass organic carbon particles (HMOC). Different particle types were found enriched in the two GF modes. ECOC and OC-Amine particles internally mixed with secondary inorganic species were found mostly in the hydrophilic mode. Pure EC particles and a small group of clay particles among the dust/ash type with strong signals of aluminum and silicon oxides appeared in the NH mode. HMOC particles were exclusively found in the NH mode. Chemical signature intensities were analyzed to examine the particle mixing states and their impact on the diversity of hygroscopicity for each particle type. BB particles in the NH mode had stronger organic carbon signals, while those in hydrophilic mode had stronger potassium salt signals. In general, an elevated OC mass fraction increased particle's hydrophobicity. Amine and secondary inorganic species such as nitrate strongly increased particle's hygroscopicity.

  2. Chemical and isotopic characterization of fatty acids and polycyclic aromatic hydrocarbons in aerosols - implications for biomass burning

    SciTech Connect

    Ballentine, D.C.

    1995-12-31

    Emissions of organic materials during biomass burning have been suggested to influence the biogeochemical distribution of nutrients in a range of ecosystems. Additionally, some organic components survive pyrolytic processes and are of regional and global biogeochemical significance because they may serve as tracers for transport of biomass burning products. Two classes of compounds that are of interest in determining the transport of these products are polycyclic aromatic hydrocarbons (PAH) and fatty acids. Polycyclic aromatic hydrocarbons are stable to biodegradation and are typically produced during natural and anthropogenic combustion processes. Fatty acids are also stable to atmospheric degradation and have been implicated as useful biomarkers for atmospheric transport. In this study, PAH and fatty acids emitted during controlled low and high temperature burns of sugar cane have been chemically and isotopically characterized using GC/MS and GC/IRMS, respectively. In order to determine if these species are suitable biomarkers for the transport of biomass burning materials, aerosols collected during sugar cane burning in South Africa have been similarly analyzed.

  3. Monitoring aerosol elemental composition in particle size fractions of long-range transport

    NASA Astrophysics Data System (ADS)

    Metternich, P.; Georgii, H.-W.; Groeneveld, K. O.

    1983-04-01

    Collection of atmospheric samples was performed at Malta, a semi-remote environment in the Mediterranean, in case of long-range transport studies of pollutants and natural substances. Using PIXE as a non-destructive trace-element analytical tool, the elemental composition of these samples was determined. Atmospheric concentrations obtained in this study were of one magnitude higher than those observed over the open North Alantic in purely marine air. For most of the anomalously enriched elements in the Mediterranean aerosol, the high concentrations can be explained by long-range transport.

  4. Aerosol-halogen interaction: Change of physico-chemical properties of SOA by naturally released halogen species

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Krüger, H.; Platt, U.; Schmitt-Kopplin, P.; Zetzsch, C.

    2011-12-01

    Reactive halogen species are released by various sources like photo-activated sea-salt aerosol or salt pans and salt lakes. These heterogeneous release mechanisms have been overlooked so far, although their potential of interaction with organic aerosols like Secondary Organic Aerosol (SOA), Biomass Burning Organic Aerosol (BBOA) or Atmospheric Humic LIke Substances (HULIS) is completely unknown. Such reactions can constitute sources of gaseous organo-halogen compounds or halogenated organic particles in the atmospheric boundary layer. To study the interaction of organic aerosols with reactive halogen species (RHS), SOA was produced from α-pinene, catechol and guaiacol using an aerosol smog-chamber. The model SOAs were characterized in detail using a variety of physico-chemical methods (Ofner et al., 2011). Those aerosols were exposed to molecular halogens in the presence of UV/VIS irradiation and to halogens, released from simulated natural halogen sources like salt pans, in order to study the complex aerosol-halogen interaction. The heterogeneous reaction of RHS with those model aerosols leads to different gaseous species like CO2, CO and small reactive/toxic molecules like phosgene (COCl2). Hydrogen containing groups on the aerosol particles are destroyed to form HCl or HBr, and a significant formation of C-Br bonds could be verified in the particle phase. Carbonyl containing functional groups of the aerosol are strongly affected by the halogenation process. While changes of functional groups and gaseous species were visible using FTIR spectroscopy, optical properties were studied using Diffuse Reflectance UV/VIS spectroscopy. Overall, the optical properties of the processed organic aerosols are significantly changed. While chlorine causes a "bleaching" of the aerosol particles, bromine shifts the maximum of UV/VIS absorption to the red end of the UV/VIS spectrum. Further physico-chemical changes were recognized according to the aerosol size-distributions or the

  5. Transport of aerosols into the UTLS and their impact on the Asian monsoon region as seen in a global model simulation

    NASA Astrophysics Data System (ADS)

    Fadnavis, S.; Semeniuk, K.; Pozzoli, L.; Schultz, M. G.; Ghude, S. D.; Das, S.; Kakatkar, R.

    2013-09-01

    An eight-member ensemble of ECHAM5-HAMMOZ simulations for a boreal summer season is analysed to study the transport of aerosols in the upper troposphere and lower stratosphere (UTLS) during the Asian summer monsoon (ASM). The simulations show persistent maxima in black carbon, organic carbon, sulfate, and mineral dust aerosols within the anticyclone in the UTLS throughout the ASM (period from July to September), when convective activity over the Indian subcontinent is highest, indicating that boundary layer aerosol pollution is the source of this UTLS aerosol layer. The simulations identify deep convection and the associated heat-driven circulation over the southern flanks of the Himalayas as the dominant transport pathway of aerosols and water vapour into the tropical tropopause layer (TTL). Comparison of model simulations with and without aerosols indicates that anthropogenic aerosols are central to the formation of this transport pathway. Aerosols act to increase cloud ice, water vapour, and temperature in the model UTLS. Evidence of ASM transport of aerosols into the stratosphere is also found, in agreement with aerosol extinction measurements from the Halogen Occultation Experiment (HALOE) and Stratospheric Aerosol and Gas Experiment (SAGE) II. As suggested by the observations, aerosols are transported into the Southern Hemisphere around the tropical tropopause by large-scale mixing processes. Aerosol-induced circulation changes also include a weakening of the main branch of the Hadley circulation and a reduction of monsoon precipitation over India.

  6. New Lidar Capabilities in Space: An Overview of the Cloud-Aerosol Transport System (CATS)

    NASA Astrophysics Data System (ADS)

    McGill, M. J.; Yorks, J. E.; Hlavka, D. L.; Selmer, P. A.; Hart, W. D.; Palm, S. P.; Nowottnick, E. P.; Vaughan, M.; Rodier, S. D.; Colarco, P. R.; da Silva, A.; Buchard, V.

    2014-12-01

    The Cloud-Aerosol Transport System (CATS), built at NASA Goddard Space Flight Center as a payload for the International Space Station (ISS), is set to launch in the late 2014. CATS is an elastic backscatter lidar operating in one of three science modes with three wavelengths (1064, 532, 355 nm) and HSRL capability at 532 nm. Depolarization measurements will be made at the 532 and 1064 nm wavelengths. The CATS science modes are described in Figure 1. The ISS orbit is a 51 degree inclination orbit at an altitude of about 405 km. This orbit provides more comprehensive coverage of the tropics and mid-latitudes than sun-synchronous orbiting sensors, with nearly a three day repeat cycle. Thus, science applications of CATS include cloud and aerosol climate studies, air quality monitoring, and smoke/volcanic plume tracking. Current uncertainties in cloud and aerosol properties limit our ability to accurately model the Earth's climate system and predict climate change. These limitations are due primarily to difficulties in adequately measuring aerosols and clouds on a global scale. A primary science objectives of CATS is to provide global aerosol and cloud vertical profile data in near real time to for assimilation in aerosol transport models such as the NASA GEOS-5 model. Furthermore, the vertical profiles of cloud and aerosol properties provided by CATS will complement current and future passive satellite sensors. Another important science objective of CATS is to advance technology in support of future mission development. CATS will employ 355 nm and HSRL capabilities, as well as depolarization at multiple wavelengths. These expanded measurement capabilities will provide the science community with new and improved global data products that have yet to be retrieved from space-based lidar. In preparation for launch, simulations of the CATS lidar signal are produced using GEOS5 model data to develop and test future data products. An example of the simulated CATS attenuated

  7. MATCH-SALSA - Multi-scale Atmospheric Transport and CHemistry model coupled to the SALSA aerosol microphysics model - Part 1: Model description and evaluation

    NASA Astrophysics Data System (ADS)

    Andersson, C.; Bergström, R.; Bennet, C.; Robertson, L.; Thomas, M.; Korhonen, H.; Lehtinen, K. E. J.; Kokkola, H.

    2014-05-01

    We have implemented the sectional aerosol dynamics model SALSA in the European scale chemistry-transport model MATCH (Multi-scale Atmospheric Transport and Chemistry). The new model is called MATCH-SALSA. It includes aerosol microphysics, with several formulations for nucleation, wet scavenging and condensation. The model reproduces observed higher particle number concentration (PNC) in central Europe and lower concentrations in remote regions. The model PNC size distribution peak occurs at the same or smaller particle size as the observed peak at five measurement sites spread across Europe. Total PNC is underestimated at Northern and Central European sites and accumulation mode PNC is underestimated at all investigated sites. On the other hand the model performs well for particle mass, including secondary inorganic aerosol components. Elemental and organic carbon concentrations are underestimated at many of the sites. Further development is needed, primarily for treatment of secondary organic aerosol, both in terms of biogenic emissions and chemical transformation, and for nitrogen gas-particle partitioning. Updating the biogenic SOA scheme will likely have a large impact on modeled PM2.5 and also affect the model performance for PNC through impacts on nucleation and condensation. An improved nitrogen partitioning model may also improve the description of condensational growth.

  8. Transport and Mixing Patterns over Central California during the Carbonaceous Aerosol and Radiative Effects Study (CARES)

    SciTech Connect

    Fast, Jerome D.; Gustafson, William I.; Berg, Larry K.; Shaw, William J.; Pekour, Mikhail S.; Shrivastava, ManishKumar B.; Barnard, James C.; Ferrare, R.; Hostetler, Chris A.; Hair, John; Erickson, Matthew H.; Jobson, Tom; Flowers, Bradley; Dubey, Manvendra K.; Springston, Stephen R.; Pirce, Bradley R.; Dolislager, Leon; Pederson, J. R.; Zaveri, Rahul A.

    2012-02-17

    We describe the synoptic and regional-scale meteorological conditions that affected the transport and mixing of trace gases and aerosols in the vicinity of Sacramento, California during June 2010 when the Carbonaceous Aerosol and Radiative Effects Study (CARES) was conducted. The meteorological measurements collected by various instruments deployed during the campaign and the performance of the chemistry version of the Weather Research and Forecasting model (WRF-Chem) are both discussed. WRF-Chem was run daily during the campaign to forecast the spatial and temporal variation of carbon monoxide emitted from 20 anthropogenic source regions in California to guide aircraft sampling. The model is shown to reproduce the overall circulations and boundary-layer characteristics in the region, although errors in the upslope wind speed and boundary-layer depth contribute to differences in the observed and simulated carbon monoxide. Thermally-driven upslope flows that transported pollutants from Sacramento over the foothills of the Sierra Nevada occurred every afternoon, except during three periods when the passage of mid-tropospheric troughs disrupted the regional-scales flow patterns. The meteorological conditions after the passage of the third trough were the most favorable for photochemistry and likely formation of secondary organic aerosols. Meteorological measurements and model forecasts indicate that the Sacramento pollutant plume was likely transported over a downwind site that collected trace gas and aerosol measurements during 23 periods; however, direct transport occurred during only eight of these periods. The model also showed that emissions from the San Francisco Bay area transported by intrusions of marine air contributed a large fraction of the carbon monoxide in the vicinity of Sacramento, suggesting that this source likely affects local chemistry. Contributions from other sources of pollutants, such as those in the Sacramento Valley and San Joaquin Valley

  9. Transport and mixing patterns over Central California during the carbonaceous aerosol and radiative effects study (CARES)

    SciTech Connect

    Fast J. D.; Springston S.; Gustafson Jr., W. I.; Berg, L. K.; Shaw, W. J.; Pekour, M.; Shrivastava, M.; Barnard, J. C.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. A.; Erickson, M.; Jobson, B. T.; Flowers, B.; Dubey, M. K.; Pierce, R. B.; Dolislager, L.; Pederson, J.; Zaveri, R. A.

    2012-02-17

    We describe the synoptic and regional-scale meteorological conditions that affected the transport and mixing of trace gases and aerosols in the vicinity of Sacramento, California during June 2010 when the Carbonaceous Aerosol and Radiative Effects Study (CARES) was conducted. The meteorological measurements collected by various instruments deployed during the campaign and the performance of the chemistry version of the Weather Research and Forecasting model (WRF-Chem) are both discussed. WRF-Chem was run daily during the campaign to forecast the spatial and temporal variation of carbon monoxide emitted from 20 anthropogenic source regions in California to guide aircraft sampling. The model is shown to reproduce the overall circulations and boundary-layer characteristics in the region, although errors in the upslope wind speed and boundary-layer depth contribute to differences in the observed and simulated carbon monoxide. Thermally-driven upslope flows that transported pollutants from Sacramento over the foothills of the Sierra Nevada occurred every afternoon, except during three periods when the passage of mid-tropospheric troughs disrupted the regional-scale flow patterns. The meteorological conditions after the passage of the third trough were the most favorable for photochemistry and likely formation of secondary organic aerosols. Meteorological measurements and model forecasts indicate that the Sacramento pollutant plume was likely transported over a downwind site that collected trace gas and aerosol measurements during 23 time periods; however, direct transport occurred during only eight of these periods. The model also showed that emissions from the San Francisco Bay area transported by intrusions of marine air contributed a large fraction of the carbon monoxide in the vicinity of Sacramento, suggesting that this source likely affects local chemistry. Contributions from other sources of pollutants, such as those in the Sacramento Valley and San Joaquin

  10. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.

    2015-12-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under CMA chemical weather modeling system GRAPES/CUACE. Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) is fed online interactively into a two-moment cloud scheme (WDM6) and a convective parameterization to drive the cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred. The results show that interactive aerosols with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content and cloud droplet number concentrations while decrease the mean diameter of cloud droplets with varying magnitudes of the changes in each case and region. These interactive micro-physical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24% to 48% enhancements of TS scoring for 6-h precipitation in almost all regions. The interactive aerosols with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3°C.

  11. Growth of ultra long multiwall carbon nanotube arrays by aerosol-assisted chemical vapor deposition.

    PubMed

    Byeon, Heejun; Kim, Sang Yong; Koh, Ken Ha; Lee, Soonil

    2010-09-01

    Using a home-made aerosol nebulizer, we developed a new aerosol-assisted chemical vapor deposition (AACVD) process that made it possible to synthesize vertically-aligned carbon nanotube (VACNT) arrays with heights over a few millimeters routinely. An essential part of this technique was in-situ formation of metal catalyst nanoparticles via pyrolysis of ferrocene-ethanol aerosol right before CNT synthesis. Through the optimization of aerosol supply and CVD process parameters, we were able to synthesize clean VACNT arrays as long as 4.38 mm with very low metal contents in 20 min. Furthermore, it is worthy noting that such an outstanding height is achieved very quickly without supporting materials and water-assistance. By taking advantage of almost complete inhibition of CNT growth on low melting-temperature metals, we were able to fabricate patterned VACNT arrays by combining AACVD process with a conventional photolithograpic patterning of gold lines. Characterizations of as-grown nanotubes such as morphology, purity, and metal contents are presented. PMID:21133158

  12. Investigating the Chemical Pathways to PAH- and PANH-Based Aerosols in Titan's Atmospheric chemistry

    NASA Technical Reports Server (NTRS)

    Sciamma-O'Brien, Ella Marion; Contreras, Cesar; Ricketts, Claire Louise; Salama, Farid

    2011-01-01

    A complex organic chemistry between Titan's two main constituents, N2 and CH4, leads to the production of more complex molecules and subsequently to solid organic aerosols. These aerosols are at the origin of the haze layers giving Titan its characteristic orange color. In situ measurements by the Ion Neutral Mass Spectrometer (INMS) and Cassini Plasma Spectrometer (CAPS) instruments onboard Cassini have revealed the presence of large amounts of neutral, positively and negatively charged heavy molecules in the ionosphere of Titan. In particular, benzene (C6H6) and toluene (C6H5CH3), which are critical precursors of polycyclic aromatic hydrocarbon (PAH) compounds, have been detected, suggesting that PAHs might play a role in the production of Titan s aerosols. Moreover, results from numerical models as well as laboratory simulations of Titan s atmospheric chemistry are also suggesting chemical pathways that link the simple precursor molecules resulting from the first steps of the N2-CH4 chemistry (C2H2, C2H4, HCN ...) to benzene, and to PAHs and nitrogen-containing PAHs (or PANHs) as precursors to the production of solid aerosols.

  13. Real-Time Chemical Analysis of E-Cigarette Aerosols By Means Of Secondary Electrospray Ionization Mass Spectrometry.

    PubMed

    García-Gómez, Diego; Gaisl, Thomas; Barrios-Collado, César; Vidal-de-Miguel, Guillermo; Kohler, Malcolm; Zenobi, Renato

    2016-02-12

    Chemical analysis of aerosols collected from electronic cigarettes (ECs) has shown that these devices produce vapors that contain harmful and potentially harmful compounds. Conventional analytical methods used for the analysis of electronic cigarettes do not reflect the actual composition of the aerosols generated because they usually neglect the changes in the chemical composition that occur during the aerosol generation process and after collection. The aim of this work was to develop and apply a method for the real-time analysis of electronic cigarette aerosols, based on the secondary electrospray ionization technique coupled to high-resolution mass spectrometry, by mimicking the "vaping" process. Electronic cigarette aerosols were successfully analyzed and quantitative differences were found between the liquids and aerosols. Thanks to the high sensitivity shown by this method, more than 250 chemical substances were detected in the aerosols, some of them showing a high correlation with the operating power of the electronic cigarettes. The method also allows proper quantification of several chemical components such as alkaloids and flavor compounds.

  14. Long-term Chemical Characterization of Submicron Aerosol Particles in the Amazon Forest - ATTO Station

    NASA Astrophysics Data System (ADS)

    Carbone, S.; Brito, J.; Rizzo, L. V.; Holanda, B. A.; Cirino, G. G.; Saturno, J.; Krüger, M. L.; Pöhlker, C.; Ng, N. L.; Xu, L.; Andreae, M. O.; Artaxo, P.

    2015-12-01

    The study of the chemical composition of aerosol particles in the Amazon forest represents a step forward to understand the strong coupling between the atmosphere and the forest. For this reason submicron aerosol particles were investigated in the Amazon forest, where biogenic and anthropogenic aerosol particles coexist at the different seasons (wet/dry). The measurements were performed at the ATTO station, which is located about 150 km northeast of Manaus. At ATTO station the Aerosol chemical speciation monitor (ACSM, Aerodyne) and the Multiangle absorption photometer (MAAP, Thermo 5012) have been operated continuously from March 2014 to July 2015. In this study, long-term measurements (near-real-time, ~30 minutes) of PM1 chemical composition were investigated for the first time in this environment.The wet season presented lower concentrations than the dry season (~5 times). In terms of chemical composition, both seasons were dominated by organics (75 and 63%) followed by sulfate (11 and 13%). Nitrate presented different ratio values between the mass-to-charges 30 to 46 (main nitrate fragments) suggesting the presence of nitrate as inorganic and organic nitrate during both seasons. The results indicated that about 75% of the nitrate signal was from organic nitrate during the dry season. In addition, several episodes with elevated amount of chloride, likely in the form of sea-salt from the Atlantic Ocean, were observed during the wet season. During those episodes, chloride comprised up to 7% of the PM1. During the dry season, chloride was also observed; however, with different volatility, which suggested that Chloride was present in different form and source. Moreover, the constant presence of sulfate and BC during the wet season might be related to biomass burning emissions from Africa. BC concentration was 2.5 times higher during the dry season. Further characterization of the organic fraction was accomplished with the positive matrix factorization (PMF), which

  15. Study of aerosol optical properties at Kunming in southwest China and long-range transport of biomass burning aerosols from North Burma

    NASA Astrophysics Data System (ADS)

    Zhu, J.; Xia, X.; Che, H.; Wang, J.; Zhang, J.; Duan, Y.

    2016-03-01

    Seasonal variation of aerosol optical properties and dominant aerosol types at Kunming (KM), an urban site in southwest China, is characterized. Substantial influences of the hygroscopic growth and long-range transport of biomass burning (BB) aerosols on aerosol optical properties at KM are revealed. These results are derived from a detailed analysis of (a) aerosol optical properties (e.g. aerosol optical depth (AOD), columnar water vapor (CWV), single scattering albedo (SSA) and size distribution) retrieved from sunphotometer measurements during March 2012-August 2013, (b) satellite AOD and active fire products, (c) the attenuated backscatter profiles from the space-born lidar, and (d) the back-trajectories. The mean AOD440nm and extinction Angstrom exponent (EAE440 - 870) at KM are 0.42 ± 0.32 and 1.25 ± 0.35, respectively. Seasonally, high AOD440nm (0.51 ± 0.34), low EAE440 - 870 (1.06 ± 0.34) and high CWV (4.25 ± 0.97 cm) during the wet season (May - October) contrast with their counterparts 0.17 ± 0.11, 1.40 ± 0.31 and 1.91 ± 0.37 cm during the major dry season (November-February) and 0.53 ± 0.29, 1.39 ± 0.19, and 2.66 ± 0.44 cm in the late dry season (March-April). These contrasts between wet and major dry season, together with the finding that the fine mode radius increases significantly with AOD during the wet season, suggest the importance of the aerosol hygroscopic growth in regulating the seasonal variation of aerosol properties. BB and Urban/Industrial (UI) aerosols are two major aerosol types. Back trajectory analysis shows that airflows on clean days during the major dry season are often from west of KM where the AOD is low. In contrast, air masses on polluted days are from west (in late dry season) and east (in wet season) of KM where the AOD is often large. BB air mass is found mostly originated from North Burma where BB aerosols are lifted upward to 5 km and then subsequently transported to southwest China via prevailing westerly winds.

  16. A 12-year observation of chemical and hygroscopic properties of marine aerosols over the western North Pacific

    NASA Astrophysics Data System (ADS)

    Boreddy, S. K. R.; Kawamura, K.

    2015-12-01

    Anthropogenic emissions from East Asia, especially in China, have significantly increased over the recent decades due to the rapid industrial development. They are implausible to decline in the next 20 years and may have a strong impact on tropospheric chemistry in marine boundary layer and cloud properties over the western North Pacific. To better understand the long-term observation of aerosol characterization and their effect on the hygroscopicity and precipitation process over the western North Pacific, we collected TSP aerosol samples on a weekly basis during the 2001-2012 at a remote marine island, Chichijima (27°04'E; 142°13'N), which is located in the outflow region of Asian dust and East Asian anthropogenic pollutants. We present here long-term observations of seasonal and annual variation of chemical and hygroscopic properties of water-soluble matter, extracted from the remote marine aerosols, based on the measurement of major inorganic ions, total organic carbon and hygroscopicity by HTDMA. Concentrations of nss-SO42- are high in winter and spring and low in summer, whereas hygroscopicity is high in summer to autumn and low in winter to spring, probably due to the influence of long-range transport of anthropogenic pollutants and dusts. Annual variation of nss-SO42- increased from 2001 to 2006 and continuously decreased from 2007 to 2012, probably due to the decreased SO2 emissions in East Asia especially in China. In contrast, hygroscopicity (g(90%)ZSR) showed a decrease from 2001 to 2006 and an increase from 2007 to 2012. These results demonstrate that although WSOM often suppress the hygroscopicity of marine aerosols, long-range atmospheric transport of nss-SO42- seriously suppress the hygroscopicity and thus affect the precipitation process over the western North Pacific. This study also demonstrates that Asian dusts can act as an important source of nutrients for phytoplankton and thus sea-to-air emission of dimethyl sulfide and subsequent

  17. Long-term measurement of aerosol chemical composition in Athens, Greece.

    NASA Astrophysics Data System (ADS)

    Paraskevopoulou, Despina; Liakakou, Eleni; Theodosi, Christina; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos

    2014-05-01

    The collection of our samples was conducted for a period of five years (2008 - 2013) in Athens, Greece. The site is situated at the premises of the National Observatory of Athens on Penteli Hill, northeast Athens suburbs, and is considered an urban background station. The aim of our study was a first long-term estimation of the chemical mass closure of aerosol. For the purposes of the study, we applied three filter samplers during the sampling period: two Partisol FRM Model 2000 air samplers (one of them collecting PM10 and the other PM2.5 fractions of aerosol) and one Dichotomous Partisol auto-sampler (with PM2.5 and PM2.5-10 inlet). Aerosols were collected on Whatman QM-A quartz fiber filters and the mass of the collected samples was estimated by weighing the pre-combusted filters before and after sampling, under controlled conditions, using a microbalance. All quartz filters were analysed for organic (OC) and elemental carbon (EC) by a thermal - optical transmission technique. The concentration of water soluble organic carbon (WSOC) was defined for each filter using a total organic carbon analyzer, while the content in main water soluble ions (Cl-, Br-, NO-3, SO4-2, PO4-3, C2O4-2, NH4+, K+, Na+, Mg+2, Ca+2) was determined by ion chromatography. Additionally the filters were analyzed for trace metals by inductively coupled plasma optical emission spectrometry (ICP-OES). Aerosol chemical mass closure calculations were conducted for the PM2.5 fraction. The area of Athens is characterized by aged aerosol that can originate from the marine boundary layer, the European mainland and occasionally from North African desert areas. The contribution of dust and particulate organic matter on PM levels was estimated taking into consideration the location of the sampling site, while identification and evaluation of sources was performed. Additionally, non-sea salt concentrations of the main ions were estimated to complete the chemical closure in the extended area. According to

  18. Multisensor analyzer detector (MSAD) for low cost chemical and aerosol detection and pattern fusion

    NASA Astrophysics Data System (ADS)

    Swanson, David C.; Merdes, Daniel W.; Lysak, Daniel B., Jr.; Curtis, Richard C.; Lang, Derek C.; Mazzara, Andrew F.; Nicholas, Nicholas C.

    2002-08-01

    MSAD is being developed as a low-cost point detection chemical and biological sensor system designed around an information fusion inference engine that also allows additional sensors to be included in the detection process. The MSAD concept is based on probable cause detection of hazardous chemical vapors and aerosols of either chemical or biological composition using a small portable unit containing an embedded computer system and several integrated sensors with complementary capabilities. The configuration currently envisioned includes a Surface-Enhanced Raman Spectroscopy (SERS) sensor of chemical vapors and a detector of respirable aerosols based on Fraunhofer diffraction. Additional sensors employing Ion Mobility Spectrometry (IMS), Surface Acoustic Wave (SAW) detection, Flame Photometric Detection (FPD), and other principles are candidates for integration into the device; also, available commercial detectors implementing IMS, SAW, and FPD will be made accessible to the unit through RS232 ports. Both feature and decision level information fusion is supported using a Continuous Inference Network (CINET) of fuzzy logic. Each class of agents has a unique CINET with information inputs from a number of available sensors. Missing or low confidence sensor information is gracefully blended out of the output confidence for the particular agent. This approach constitutes a plug and play arrangement between the sensors and the information pattern recognition algorithms. We are currently doing simulant testing and developing out CINETs for actual agent testing at Edgewood Chemical and Biological Center (ECBC) later this year.

  19. Transport of anthropogenic and biomass burning aerosols from Europe to the Arctic during spring 2008

    NASA Astrophysics Data System (ADS)

    Marelle, L.; Raut, J.-C.; Thomas, J. L.; Law, K. S.; Quennehen, B.; Ancellet, G.; Pelon, J.; Schwarzenboeck, A.; Fast, J. D.

    2015-04-01

    During the POLARCAT-France airborne campaign in April 2008, pollution originating from anthropogenic and biomass burning emissions was measured in the European Arctic. We compare these aircraft measurements with simulations using the WRF-Chem model to investigate model representation of aerosols transported from Europe to the Arctic. Modeled PM2.5 is evaluated using European Monitoring and Evaluation Programme (EMEP) measurements in source regions and POLARCAT aircraft measurements in the Scandinavian Arctic. Total PM2.5 agrees well with the measurements, although the model overestimates nitrate and underestimates organic carbon in source regions. Using WRF-Chem in combination with the Lagrangian model FLEXPART-WRF, we find that during the campaign the research aircraft sampled two different types of European plumes: mixed anthropogenic and fire plumes from eastern Europe and Russia transported below 2 km, and anthropogenic plumes from central Europe uplifted by warm conveyor belt circulations to 5-6 km. Both modeled plume types had undergone significant wet scavenging (> 50% PM10) during transport. Modeled aerosol vertical distributions and optical properties below the aircraft are evaluated in the Arctic using airborne lidar measurements. Model results show that the pollution event transported aerosols into the Arctic (> 66.6° N) for a 4-day period. During this 4-day period, biomass burning emissions have the strongest influence on concentrations between 2.5 and 3 km altitudes, while European anthropogenic emissions influence aerosols at both lower (~ 1.5 km) and higher altitudes (~ 4.5 km). As a proportion of PM2.5, modeled black carbon and SO4= concentrations are more enhanced near the surface in anthropogenic plumes. The European plumes sampled during the POLARCAT-France campaign were transported over the region of springtime snow cover in northern Scandinavia, where they had a significant local atmospheric warming effect. We find that, during this transport

  20. Transport of anthropogenic and biomass burning aerosols from Europe to the Arctic during spring 2008

    DOE PAGES

    Marelle, L.; Raut, Jean-Christophe; Thomas, J. L.; Law, K. S.; Quennehen, Boris; Ancellet, G.; Pelon, J.; Schwarzenboeck, A.; Fast, Jerome D.

    2015-04-10

    During the POLARCAT-France airborne campaign in April 2008, pollution originating from anthropogenic and biomass burning emissions was measured in the European Arctic. We compare these aircraft measurements with simulations using the WRF-Chem model to investigate model representation of aerosols transported from Europe to the Arctic. Modeled PM2.5 is evaluated using European Monitoring and Evaluation Programme (EMEP) measurements in source regions and POLARCAT aircraft measurements in the Scandinavian Arctic. Total PM2.5 agrees well with the measurements, although the model overestimates nitrate and underestimates organic carbon in source regions. Using WRF-Chem in combination with the Lagrangian model FLEXPART-WRF, we find that duringmore » the campaign the research aircraft sampled two different types of European plumes: mixed anthropogenic and fire plumes from eastern Europe and Russia transported below 2 km, and anthropogenic plumes from central Europe uplifted by warm conveyor belt circulations to 5–6 km. Both modeled plume types had undergone significant wet scavenging (> 50% PM10) during transport. Modeled aerosol vertical distributions and optical properties below the aircraft are evaluated in the Arctic using airborne lidar measurements. Model results show that the pollution event transported aerosols into the Arctic (> 66.6° N) for a 4-day period. During this 4-day period, biomass burning emissions have the strongest influence on concentrations between 2.5 and 3 km altitudes, while European anthropogenic emissions influence aerosols at both lower (~ 1.5 km) and higher altitudes (~ 4.5 km). As a proportion of PM2.5, modeled black carbon and SO4= concentrations are more enhanced near the surface in anthropogenic plumes. The European plumes sampled during the POLARCAT-France campaign were transported over the region of springtime snow cover in northern Scandinavia, where they had a significant local atmospheric warming effect. We find that, during this

  1. Transport of anthropogenic and biomass burning aerosols from Europe to the Arctic during spring 2008

    SciTech Connect

    Marelle, L.; Raut, Jean-Christophe; Thomas, J. L.; Law, K. S.; Quennehen, Boris; Ancellet, G.; Pelon, J.; Schwarzenboeck, A.; Fast, Jerome D.

    2015-04-10

    During the POLARCAT-France airborne campaign in April 2008, pollution originating from anthropogenic and biomass burning emissions was measured in the European Arctic. We compare these aircraft measurements with simulations using the WRF-Chem model to investigate model representation of aerosols transported from Europe to the Arctic. Modeled PM2.5 is evaluated using European Monitoring and Evaluation Programme (EMEP) measurements in source regions and POLARCAT aircraft measurements in the Scandinavian Arctic. Total PM2.5 agrees well with the measurements, although the model overestimates nitrate and underestimates organic carbon in source regions. Using WRF-Chem in combination with the Lagrangian model FLEXPART-WRF, we find that during the campaign the research aircraft sampled two different types of European plumes: mixed anthropogenic and fire plumes from eastern Europe and Russia transported below 2 km, and anthropogenic plumes from central Europe uplifted by warm conveyor belt circulations to 5–6 km. Both modeled plume types had undergone significant wet scavenging (> 50% PM10) during transport. Modeled aerosol vertical distributions and optical properties below the aircraft are evaluated in the Arctic using airborne lidar measurements. Model results show that the pollution event transported aerosols into the Arctic (> 66.6° N) for a 4-day period. During this 4-day period, biomass burning emissions have the strongest influence on concentrations between 2.5 and 3 km altitudes, while European anthropogenic emissions influence aerosols at both lower (~ 1.5 km) and higher altitudes (~ 4.5 km). As a proportion of PM2.5, modeled black carbon and SO4= concentrations are more enhanced near the surface in anthropogenic plumes. The European plumes sampled during the POLARCAT-France campaign were transported over the region of springtime snow cover in northern Scandinavia, where they had a significant

  2. Investigation of the detailed chemical composition of organic aerosol in a South East Asian Rainforest

    NASA Astrophysics Data System (ADS)

    Hamilton, Jacqueline; Ward, Martyn; Rami Alfarra, M.; Lewis, Alastair; McFiggans, Gordon; Robinson, Niall

    2010-05-01

    The formation of secondary organic aerosol (SOA) in tropical regions is a key uncertainty in quantifying the effect of man made emissions on the climate. Large quantities of volatile organic compounds are emitted from natural biogenic sources in the tropics, including isoprene, monoterpenes and sequiterpenes. There are very few studies of the detailed chemical composition of organic aerosols in tropical rainforest regions, but these would provide information on the importance of primary versus secondary organic aerosols, the key VOC precursors, oxidation state and volatility. Particle samples were collected in a tropical rainforest at Danum Valley in Borneo as part of the OP3 field campaign in 2008. Twenty four hour filter samples were collected at the Global Atmospheric Watch station at a height of around 10 m and shipped back to the laboratory (below -4 °C) for offline analysis. The OA composition was studied using multiple high resolution chromatographic techniques including comprehensive two dimensional gas chromatography coupled to time of flight mass spectrometry (GCXGC-TOFMS) and liquid chromatography coupled to ion trap mass spectrometry (LC-MSn). The composition was directly compared to chamber generated SOA (as part of the Aerosol Coupling in the Earths System , ACES, experiment) to determine SOA tracers. A biogenic SOA tracer MS fragmentation library was constructed and a number of SOA components from limonene, linalool and -pinene were identified in the rainforest OA. Very high resolution mass spectrometry (Fourier Transform Ion Cyclotron Resonance FTICR-MS) allowed the O:C and H:C ratios to be determined and these will be compared to those obtained by aerosol mass spectrometry (AMS). In addition, the OA composition from the rainforest will be compared to other locations.

  3. Relating aerosol absorption due to soot, organic carbon, and dust to emission sources determined from in-situ chemical measurements

    NASA Astrophysics Data System (ADS)

    Cazorla, A.; Bahadur, R.; Suski, K. J.; Cahill, J. F.; Chand, D.; Schmid, B.; Ramanathan, V.; Prather, K. A.

    2013-09-01

    Estimating the aerosol contribution to the global or regional radiative forcing can take advantage of the relationship between the spectral aerosol optical properties and the size and chemical composition of aerosol. Long term global optical measurements from observational networks or satellites can be used in such studies. Using in-situ chemical mixing state measurements can help us to constrain the limitations of such estimates. In this study, the Absorption Ångström Exponent (AAE) and the Scattering Ångström Exponent (SAE) derived from 10 operational AERONET sites in California are combined for deducing chemical speciation based on wavelength dependence of the optical properties. In addition, in-situ optical properties and single particle chemical composition measured during three aircraft field campaigns in California between 2010 and 2011 are combined in order to validate the methodology used for the estimates of aerosol chemistry using spectral optical properties. Results from this study indicate a dominance of mixed types in the classification leading to an underestimation of the primary sources, however secondary sources are better classified. The distinction between carbonaceous aerosols from fossil fuel and biomass burning origins is not clear, since their optical properties are similar. On the other hand, knowledge of the aerosol sources in California from chemical studies help to identify other misclassification such as the dust contribution.

  4. The long-range transport of atmospheric aerosols from South Asia to Himalayas

    NASA Astrophysics Data System (ADS)

    Cong, Zhiyuan; Kang, Shichang; Kawamura, Kimitaka

    2016-04-01

    High levels of carbonaceous aerosol exist over South Asia, the area adjacent to the Himalayas and Tibetan Plateau. Little is known about if they can be transported across the Himalayas, and as far inland as the Tibetan Plateau. To resolve such scientific questions, aerosol samples were collected weekly from August 2009 to July 2010 at Qomolangma (Mt. Everest) Station for Atmospheric and Environmental Observation and Research(QOMS, 4276 m a.s.l.). In the laboratory, major ions, elemental carbon, organic carbon, levoglucosan, water-soluble organic carbon, and organic acids were analyzed. The concentration levels of OC and EC at QOMS are comparable to those at high-elevation sites on the southern slopes of the Himalayas (Langtang and NCO-P), but 3 to 6 times lower than those at Manora Peak, India, and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate. The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. OC, EC and other ionic species (NH+4 , K+, NO- and SO2-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season, being similar to the seasonal trends of aerosol compo-sition reported previously from the southern slope of the Himalayas. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they mainly originated from biomass burning. Molecular distributions of dicarboxylic acids and related compounds (malonic acid/ succinic acid, maleic acid/fumaric acid) further support this finding. The fire spots observed by MODIS and backward air-mass trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. In addition to large-scale atmospheric circulation, the unique mountain/valley breeze system can also have an important effect on air-pollutant transport.With the consideration of the darkening force of

  5. The long-range transport of atmospheric aerosols from South Asia to Himalayas

    NASA Astrophysics Data System (ADS)

    Cong, Zhiyuan; Kang, Shichang; Kawamura, Kimitaka

    2016-04-01

    High levels of carbonaceous aerosol exist over South Asia, the area adjacent to the Himalayas and Tibetan Plateau. Little is known about if they can be transported across the Himalayas, and as far inland as the Tibetan Plateau. To resolve such scientific questions, aerosol samples were collected weekly from August 2009 to July 2010 at Qomolangma (Mt. Everest) Station for Atmospheric and Environmental Observation and Research(QOMS, 4276 m a.s.l.). In the laboratory, major ions, elemental carbon, organic carbon, levoglucosan, water-soluble organic carbon, and organic acids were analyzed. The concentration levels of OC and EC at QOMS are comparable to those at high-elevation sites on the southern slopes of the Himalayas (Langtang and NCO-P), but 3 to 6 times lower than those at Manora Peak, India, and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate. The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. OC, EC and other ionic species (NH+4 , K+, NO‑ and SO2‑) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season, being similar to the seasonal trends of aerosol compo-sition reported previously from the southern slope of the Himalayas. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they mainly originated from biomass burning. Molecular distributions of dicarboxylic acids and related compounds (malonic acid/ succinic acid, maleic acid/fumaric acid) further support this finding. The fire spots observed by MODIS and backward air-mass trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. In addition to large-scale atmospheric circulation, the unique mountain/valley breeze system can also have an important effect on air-pollutant transport.With the consideration of the darkening force of

  6. Halogen-induced organic aerosol (XOA): a study on ultra-fine particle formation and time-resolved chemical characterization.

    PubMed

    Ofner, Johannes; Kamilli, Katharina A; Held, Andreas; Lendl, Bernhard; Zetzsch, Cornelius

    2013-01-01

    The concurrent presence of high values of organic SOA precursors and reactive halogen species (RHS) at very low ozone concentrations allows the formation of halogen-induced organic aerosol, so-called XOA, in maritime areas where high concentrations of RHS are present, especially at sunrise. The present study combines aerosol smog-chamber and aerosol flow-reactor experiments for the characterization of XOA. XOA formation yields from alpha-pinene at low and high concentrations of chlorine as reactive halogen species (RHS) were determined using a 700 L aerosol smog-chamber with a solar simulator. The chemical transformation of the organic precursor during the aerosol formation process and chemical aging was studied using an aerosol flow-reactor coupled to an FTIR spectrometer. The FTIR dataset was analysed using 2D correlation spectroscopy. Chlorine induced homogeneous XOA formation takes place at even 2.5 ppb of molecular chlorine, which was photolysed by the solar simulator. The chemical pathway of XOA formation is characterized by the addition of chlorine and abstraction of hydrogen atoms, causing simultaneous carbon-chlorine bond formation. During further steps of the formation process, carboxylic acids are formed, which cause a SOA-like appearance of XOA. During the ozone-free formation of secondary organic aerosol with RHS a special kind of particulate matter (XOA) is formed, which is afterwards transformed to SOA by atmospheric aging or degradation pathways.

  7. Intra and inter-continental aerosol transport and local and regional impacts

    NASA Astrophysics Data System (ADS)

    Charles, Leona Ann Marie

    Under the Clean Air Act, the Environmental Protection Agency (EPA) is required to establish a nationally uniform air quality index for the reporting of air quality. In 1976, the EPA established this index, then called the Pollutant Standards Index, for use by state and local communities across the country. The Index provides information on pollutant concentrations for ground-level ozone, particulate matter, carbon monoxide, sulfur dioxide, and nitrogen dioxide. On July 18, 1997, the EPA revised the ozone and particulate matter standards, in light of a comprehensive review of new scientific evidence including refined fine particulate matter standards.* Any program which is designed to improve air quality must devise tools in which emissions, meteorology, air chemistry and transport are understood. Clearly, the complexity of this task requires measurements at both regional and mesoscale ranges, as well as on a continental scale to investigate long range transport. Unfortunately, determination of fine particulate matter (PM) concentrations is particularly difficult since an accurate measurement of PM2.5 relies on costly equipment which cannot provide the complete transport story and the mixing and dispersion of particulate matter is much more complex than that for trace gases. Besides the need for accurate measurements as a way of documenting air quality standards, the EPA is required in the near future to implement a 24 hour Air Quality Forecast. Current forecast tools are usually based on emission inventories and meteorological forecasts, but significant work is being done in trying to assimilate both ground measurements as well as satellite measurements into these schemes. Clearly, the 'Holy Grail' would be the capability of assimilating full 3D (+ time) measurements. However, since satellite measurements are primarily passive, only total air column properties such as aerosol optical depth can be retrieved. In particular, it is not possible to determine the

  8. Aerosol Physical and Chemical Properties Before and After the Manaus Plume in the GoAmazon2014 Experiment

    NASA Astrophysics Data System (ADS)

    Artaxo, P.; Barbosa, H. M.; Ferreira De Brito, J.; Wurm, F.; Holanda, B. A.; Carbone, S.; Arana, A.; Cirino, G. G.; Souza, R. A. F. D.; Rizzo, L. V.; Martin, S. T.; Andreae, M. O.; Holben, B. N.; Schafer, J.

    2014-12-01

    As part of the GoAmazon2014 experiment, several aerosol and trace gas monitoring stations are being operated for at least one year before and after the Manaus plume. Three sites are being operated in pristine conditions, with atmospheric properties under natural biogenic conditions. These three sites called T0 are: ATTO (Amazon Tall Tower Observatory), ZF2 ecological research site and a third site called EMBRAPA. After the air masses are exposed to the Manaus plume, one site (called T2) is being operated right on the opposite side of the Negro River under the direct influence of the Manaus plume at 5 Km downwind of Manaus. Finally, at about 150 Km downwind of Manaus is the T3 Manacapuru site. Aerosol chemical composition is being analyzed using filters for fine (PM2.5) and coarse mode aerosol as well as three Aerodyne ACSM (Aerosol Chemical Speciation Monitors) instruments. Aerosol absorption is being studied with several aethalometers and MAAP (Multi Angle Absorption Photometers). Aerosol light scattering are being measured at several wavelengths using nephelometers. Aerosol size distribution is determined using scanning mobility particle sizers. The aerosol column is measures using AERONET sunphotometers before and after the Manaus plume, as well as several Lidar systems. The three sites before the Manaus plume show remarkable similar variability in aerosol concentrations and optical properties. This pattern is very different at the T2 site, with large aerosol concentrations enhancing aerosol absorption and scattering significantly. The aerosol is very oxidized before being exposed to the Manaus plume, and this pattern changes significantly for T2 and T3 sites, with a much higher presence of less oxidized aerosol. Typical ozone concentrations at mid-day before Manaus plume is a low 10-12 ppb, value that changes to 50-70 ppb for air masses suffering the influence of Manaus plume. A detailed comparison of aerosol characteristics and composition for the several

  9. Providing Size-Resolved Mixing State Inputs to Improve Aerosol Optics Models: Comparison of ACE-Asia Aerosol Chemical Measurements for Different Source Regions With Simultaneous Optical Measurements

    NASA Astrophysics Data System (ADS)

    Sullivan, R. C.; Poon, G.; Guazzotti, S.; Sodeman, D.; Holecek, J.; Spencer, M.; Prather, K.

    2005-12-01

    Measurements made of the aerodynamic size and chemical composition of single aerosol particles on board the R/V Ronald H. Brown sailing between Hawaii and the Sea of Japan during ACE-Asia in 2001 revealed a complex mixture of mineral dust, organic carbon, elemental carbon, sulfates, nitrates, chloride, ammonium, and sea salt. The air mass source regions included influences from the Pacific Ocean, Miyakejima volcano, Gobi and Taklimakan Deserts, Shanghai, Japan, and Korea. The particle composition sampled from each of these regions showed unique changes in the aerosol's mixing state. This complexity presents major challenges in accurately modeling the optical properties of the Asian aerosol. The degree of closure between the measured chemical and optical properties of this aerosol and those predicted by models has been presented by Quinn et al. [JGR, 109, D19S01, doi: 10.1029/2003JD004010, 2004]. Differences between measured and calculated aerosol absorption coefficients were partly attributed to the assumption of internally mixed homogeneous spheres for the aerosol population. Good correlations between measured and calculated aerosol mass and light scattering were found but relied on particle shapes not confirmed by measurements. To better our understanding of the relationship between aerosol chemistry and optical measurements, and provide more detailed inputs to improve the predictions of optical models, we present size-resolved single-particle mixing state results obtained by an ATOFMS for the seven air mass source regions described by Quinn et al. (2004). Our results do not support the assumption of a homogeneous internally mixed aerosol population for many of the source regions. Particular focus is given to the mixing state and chemical associations of sulfate, nitrate, chloride, ammonium, OC, EC, dust, and sea salt. We demonstrate the segregation of ammonium, sulfate, and nitrate within individual particles throughout the study and discuss the different

  10. Aerosol transport of biomass burning to the Bolivian Andean region from remote sensing measurements

    NASA Astrophysics Data System (ADS)

    Perez-Ramirez, Daniel; Whiteman, David; Andrade, Marcos; Gasso, Santiago; Stein, Ariel; Torres, Omar; Eck, Tom; Velarde, Fernando; Aliaga, Diego

    2016-04-01

    This work deals with the analysis of columnar aerosol optical and microphysical properties obtained by the AERONET network in the region of Bolivia and its border with Brazil. Through the long record AERONET measurements we focus in the transport of biomass-burning aerosol from the Amazon basin (stations at Rio Branco, Cuiba, Ji Parana and Santa Cruz) to the Andean Altiplano (altitude above 3000 m a.s.l. at the station in the city of La Paz). Also, measurements from the space-sensors MODIS and OMI are used to understand spatial distribution. The main results is the high impact in the aerosol load during the months of August, September and August with mean values of aerosol optical depth at 500 nm (AOD) at the low lands of ≈ 0.60 ± 0.60 and Angstrom exponent (α(440-870)) of ≈ 1.52 ± 0.38. Satellite measurements also follow very similar patterns. Also, that season is characterized by some extreme events that can reach AOD of up to 6.0. Those events are cloud-screened by MODIS but not by OMI sensor, which is attributed to different pixel resolutions. The biomass-burning is clearly transport to the Andean region where higher values of AOD (~ 0.12 ± 0.06 versus 0.09 ± 0.04 in the no biomass-burning season) and α(440-870) (~ 0.95 ± 0.30 versus 0.84 ± 0.3 in the no biomass-burning season). However, the intensity of the biomass-burning season varies between different years. Analysis of precipitation anomalies using TRNM satellites indicates a strong correlation with AOD, which suggest that on dry years there is less vegetation to burn and so less aerosol load. The opposite is found for positive anomalies of precipitation. In the transport of biomass burning larger values of the effective radius (reff) are observed in La Paz (reff = 0.26 ± 0.10 μm) than in the low lands (reff = 0.63 ± 0.24 μm), which has been explained by aerosol aging processes. Moreover, although the spectral dependence is similar, single scattering albedo (SSA) is larger in the low lands

  11. Chemical Kinetic Modeling of Advanced Transportation Fuels

    SciTech Connect

    PItz, W J; Westbrook, C K; Herbinet, O

    2009-01-20

    Development of detailed chemical kinetic models for advanced petroleum-based and nonpetroleum based fuels is a difficult challenge because of the hundreds to thousands of different components in these fuels and because some of these fuels contain components that have not been considered in the past. It is important to develop detailed chemical kinetic models for these fuels since the models can be put into engine simulation codes used for optimizing engine design for maximum efficiency and minimal pollutant emissions. For example, these chemistry-enabled engine codes can be used to optimize combustion chamber shape and fuel injection timing. They also allow insight into how the composition of advanced petroleum-based and non-petroleum based fuels affect engine performance characteristics. Additionally, chemical kinetic models can be used separately to interpret important in-cylinder experimental data and gain insight into advanced engine combustion processes such as HCCI and lean burn engines. The objectives are: (1) Develop detailed chemical kinetic reaction models for components of advanced petroleum-based and non-petroleum based fuels. These fuels models include components from vegetable-oil-derived biodiesel, oil-sand derived fuel, alcohol fuels and other advanced bio-based and alternative fuels. (2) Develop detailed chemical kinetic reaction models for mixtures of non-petroleum and petroleum-based components to represent real fuels and lead to efficient reduced combustion models needed for engine modeling codes. (3) Characterize the role of fuel composition on efficiency and pollutant emissions from practical automotive engines.

  12. Chemical, Physical and Optical Properties of Saharan Dust Aerosols at a Marine Site in Puerto Rico

    NASA Astrophysics Data System (ADS)

    Ortiz Montalvo, D. L.; Mayol Bracero, O. L.; Morales, F.; Sheridan, P.; Ogren, J. A.

    2005-12-01

    Atmospheric dust particles blown from the Sahara across the Atlantic into the Caribbean have an impact on its climate and public health. These particles may play a significant role in radiative forcing, affecting the extinction of solar radiation and thus having an influence on climate. About half of the dust that travels from Africa contains particles that are small enough to inhale. Human breathe them into the respiratory system and they settle in the lungs causing respiratory problems. To have a better understanding of these effects, information is needed on the properties of these aerosols. As part of this study, chemical, physical and optical characterization is being performed on aerosol samples collected at a marine site on the northeastern tip of Puerto Rico (Cabezas de San Juan, Fajardo), during periods with and without Saharan incursions. Stacked-filter units (SFU) are used to collect particles with diameters smaller than 1.7 μm, using Nuclepore, quartz and Teflon filters. These filter samples are analyzed to obtain the chemical composition of the particles. Initially we are focusing on the carbonaceous fraction (elemental and organic carbon, EC, and OC) of the aerosol using thermal/optical analysis. Online measurements of total particle number concentrations and aerosol light scattering coefficients are performed using a condensation particle counter and an integrating nephelometer, respectively. In addition, a sunphotometer, part of AERONET (http://aeronet.gsfc.nasa.gov/), is used to obtain the aerosol optical thickness (AOT). Preliminary results include only samples collected from air masses under the influence of Saharan dust, as signified by AOT satellite images from MODIS and the results from the air masses backward trajectories calculated with the NOAA HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) model. In terms of the chemical composition, EC concentrations were at low-to-undetectable levels, indicating that OC concentrations

  13. Observations of the Interaction and/or Transport of Aerosols with Cloud or Fog during DRAGON Campaigns from AERONET Ground-Based Remote Sensing

    NASA Astrophysics Data System (ADS)

    Eck, Thomas; Holben, Brent; Schafer, Joel; Giles, David; Kim, Jhoon; Kim, Young; Sano, Itaru; Reid, Jeffrey; Pickering, Kenneth; Crawford, James; Sinyuk, Alexander; Trevino, Nathan

    2014-05-01

    Ground-based remote sensing observations from Aerosol Robotic Network (AERONET) sun-sky radiometers have recently shown several instances where cloud-aerosol interaction had resulted in modification of aerosol properties and/or in difficulty identifying some major pollution transport events due to aerosols being imbedded in cloud systems. AERONET has established Distributed Regional Aerosol Gridded Observation Networks (DRAGON) during field campaigns that are short-term (~2-3 months) relatively dense spatial networks of ~15 to 45 sun and sky scanning photometers. Recent major DRAGON field campaigns in Japan and South Korea (Spring 2012) and California (Winter 2013) have yielded observations of aerosol transport associated with clouds and/or aerosol properties modification as a result of fog interaction. Analysis of data from the Korean and Japan DRAGON campaigns shows that major fine-mode aerosol transport events are sometimes associated with extensive cloud cover and that cloud-screening of observations often filter out significant pollution aerosol transport events. The Spectral De-convolution Algorithm (SDA) algorithm was utilized to isolate and analyze the fine-mode aerosol optical depth signal for these cases of persistent and extensive cloud cover. Additionally, extensive fog that was coincident with aerosol layer height on some days in both Korea and California resulted in large increases in fine mode aerosol radius, with a mode of cloud-processed or residual aerosol of radius ~0.4-0.5 micron sometimes observed. Cloud processed aerosol may occur much more frequently than AERONET data suggest due to inherent difficulty in observing aerosol properties near clouds from remote sensing observations. These biases of aerosols associated with clouds would likely be even greater for satellite remote sensing retrievals of aerosol properties near clouds due to 3-D effects and sub-pixel cloud contamination issues.

  14. Vertical Structure, Transport, and Mixing of Ozone and Aerosols Observed During NEAQS/ICARTT 2004

    NASA Astrophysics Data System (ADS)

    Senff, C. J.; Hardesty, R. M.; Brewer, W. A.; Alvarez, R. J.; Sandberg, S. P.; Tucker, S. C.; Intrieri, J. M.; Marchbanks, R. D.; McCarty, B. J.; Banta, R. M.; Darby, L. S.; White, A. B.

    2005-12-01

    During the 2004 New England Air Quality Study (NEAQS), which was conducted within the framework of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) field experiment, airborne and shipborne lidar remote sensing instruments were deployed to characterize the 3-dimensional structure of ozone, aerosol, and low-level wind fields in the New England region. The 2004 measurements confirmed findings from the smaller-scale NEAQS 2002 experiment: the vertical structure and transport patterns of pollutant plumes from the Boston and New York City urban areas are strongly modified when they are advected over the Gulf of Maine. Because of strong vertical wind shear and a very stable atmosphere over the cold ocean water the plumes tend to get sheared apart and the resulting pieces of the plumes stay confined in layers aloft, isolated from the surface. Most notably, ozone concentrations aloft are very often significantly higher than ozone levels near the ocean surface. These elevated pollution plumes over the Gulf of Maine can affect air quality in coastal New England only when they are transported back over land. This can be accomplished by the large-scale flow or by local circulations such as the sea breeze. Once over land the elevated plumes may impact surface air quality by direct transport to higher terrain (e.g., Cadillac Mountain, ME) or by being fumigated down to the surface. Alternatively, but probably more rarely, an elevated pollution plume over the ocean may be mixed down to the surface by mechanically generated turbulence and then transported back to land within the marine boundary layer. We will use airborne and shipborne lidar remote sensing data to characterize the vertical distribution of ozone and aerosols over coastal New England, in particular the difference in plume structure over land and water. We will also show observational evidence for several of the processes described above that may mix down and transport

  15. MBAS (Methylene Blue Active Substances) and LAS (Linear Alkylbenzene Sulphonates) in Mediterranean coastal aerosols: Sources and transport processes

    NASA Astrophysics Data System (ADS)

    Becagli, S.; Ghedini, C.; Peeters, S.; Rottiers, A.; Traversi, R.; Udisti, R.; Chiari, M.; Jalba, A.; Despiau, S.; Dayan, U.; Temara, A.

    2011-12-01

    Methylene Blue Active Substances (MBAS) and Linear Alkylbenzene Sulphonates (LAS) concentrations, together with organic carbon and ions were measured in atmospheric coastal aerosols in the NW Mediterranean Basin. Previous studies have suggested that the presence of surfactants in coastal aerosols may result in vegetation damage without specifically detecting or quantifying these surfactants. Coastal aerosols were collected at a remote site (Porquerolles Island-Var, France) and at a more anthropised site (San Rossore National Park-Tuscany, Italy). The chemical data were interpreted according to a comprehensive local meteorological analysis aiming to decipher the airborne source and transport processes of these classes of compounds. The LAS concentration (anthropogenic surfactants) was measured in the samples using LC-MS/MS, a specific analytical method. The values were compared with the MBAS concentration, determined by a non-specific analytical method. At Porquerolles, the MBAS concentration (103 ± 93 ng m -3) in the summer samples was significantly higher than in the winter samples. In contrast, LAS concentrations were rarely greater than in the blank filters. At San Rossore, the mean annual MBAS concentration (887 ± 473 ng m -3 in PM10) contributed about 10% to the total atmospheric particulate organic matter. LAS mean concentration in these same aerosol samples was 11.5 ± 10.5 ng m -3. A similar MBAS (529 ± 454 ng m -3) - LAS (7.1 ± 4.1 ng m -3 LAS) ratio of ˜75 was measured in the fine (PM2.5) aerosol fraction. No linear correlation was found between MBAS and LAS concentrations. At San Rossore site the variation of LAS concentrations was studied on a daily basis over a year. The LAS concentrations in the coarse fraction (PM10-2.5) were higher during strong sea storm conditions, characterized by strong air flow coming from the sea sector. These events, occurring with more intensity in winter, promoted the formation of primary marine aerosols containing LAS

  16. Three-Dimension Analysis of the TRACE-P Aircraft Observations using the STEM Regional-Scale Chemical Transport Model

    NASA Astrophysics Data System (ADS)

    Tang, Y.; Carmichael, G. R.; Uno, I.; Woo, J.; Kurata, G.; Guttikunda, S. K.; Street, D. G.; Shetter, R. E.; Huang, H.

    2002-12-01

    A three-dimensional regional-scale chemical transport model, STEM, coupled with a detailed radiation computation scheme is used to calculate the transport and chemistry of trace gases and aerosols in Asia during the TRACE-P experiment. Extensive comparison of calculated results with aircraft observations will be presented, and it is found that many of the important features observed in the behavior of trace gases and aerosols are captured by the model. Based on these results, we evaluate various factors influencing the distribution of trace gases during the TRACE-P period. Clouds are shown to have a large impact on photolysis rates during the observation period of TRACE-P. Clouds are shown to decrease J[NO2] by 22% below clouds and enhance photolysis rates by 33% from 1 km to 10km. Clouds also exert a dominant influence on short-lived species, like OH and HO2. For example, clouds reduce OH by 23% at altitudes below 1km and increase OH by 25% above 1km. Asian aerosols contain large amounts of carbonaceous material, inorganic components such as sulfates, and mineral oxides. These aerosols significantly influence J-values and photochemical processes. When averaged over all TRACE-P DC-8 and P-3 scientific flights, the aerosol influence via affecting J-values is to reduce OH by 41% below 1km, and by 24% above 1km. Aerosols have a stronger impact on longer-lived chemical species than clouds do, because aerosols tend to be co-emitted with precursors and have a longer contact time with the polluted air masses than clouds do. The accumulated aerosol impact generally is to reduce O3 concentrations by about 6ppbv in the biomass plumes emitted from Southeast Asia. In megacity plumes, aerosols can increase NOx concentration by 40% via reducing its photolytic loss, and reduce NOz concentration by a similar amount. Biomass burning plays a very important role during March of 2001. Our simulations show that biomass emissions contributed 15% of CO and 69% of Black Carbon during the

  17. Aerosol optical properties at Mauna Loa Observatory - Long-range transport from Kuwait?

    NASA Astrophysics Data System (ADS)

    Bodhaine, B. A.; Harris, J. M.; Ogren, J. A.; Hofmann, D. J.

    1992-03-01

    Aerosol light absorption has been measured continuously at Mauna Loa Observatory, Hawaii (MLO), since April 1990. During the spring of 1991, after oil wells were fired in Kuwait, there was speculation among scientists concerning long-range transport of smoke particles and its possible effect on global climate. The MLO light absorption record from April 1990 to June 1991 shows low values in the 0.1-1 x 10 exp -7 per m range in the summer of 1990, and an increased baseline level of about 2-4 x 10 exp -7 per m with numerous superimposed events in the 5-10 x 10 exp -7 per m range in the spring of 1991. These levels correspond to black carbon (BC) concentrations of 1-10, 20-40, and 50-100 ng/cu m, respectively, under the assumption that BC is the dominant light absorbing species and has a specific absorption of 10 sq m/g. Large-scale 500-hPa trajectories calculated backwards from MLO sometimes show direct transport paths from China and Kuwait to Hawaii that coincide with the black carbon events. These measurements set an upper limit on the possible contribution of Kuwaiti black carbon to the background troposphere near MLO during periods of rapid transport. The aerosol observed at MLO is expected to cause a net cooling of the atmosphere.

  18. Carbonaceous and inorganic composition in long-range transported aerosols over northern Japan: Implication for aging of water-soluble organic fraction

    NASA Astrophysics Data System (ADS)

    Aggarwal, Shankar Gopala; Kawamura, Kimitaka

    To better understand the influence of sources and atmospheric processing on aerosol chemical composition, we collected atmospheric particles in Sapporo, northern Japan during spring and early summer 2005 under the air mass transport conditions from Siberia, China and surrounding seas. The aerosols were analyzed for inorganic ions, organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and the major water-soluble organic compound classes (i.e., dicarboxylic acids and sugars). SO 42- is the most abundant inorganic constituent (average 44% of the identified inorganic ion mass) followed by NH 4+ (21%) and NO 3- (13%). Concentrations of OC, EC, and WSOC ranged from 2.0-16, 0.24-2.9, and 0.80-7.9 μg m -3 with a mean of 7.4, 1.0, and 3.1 μg m -3, respectively. High OC/EC ratios (range: 3.6-19, mean: 8.7) were obtained, however WSOC/OC ratios (0.23-0.69, 0.44) do not show any significant diurnal changes. These results suggest that the Sapporo aerosols were already aged, but were not seriously affected by local photochemical processes. Identified water-soluble organic compounds (diacids + sugars) account for <10% of WSOC. Based on some marker species and air mass back trajectory analyses, and using stable carbon isotopic compositions of shorter-chain diacids (i.e., C 2-C 4) as photochemical aging factor of organic aerosols, the present study suggests that a fraction of WSOC in OC is most likely influenced by aerosol aging, although the OC loading in aerosols may be more influenced by their sources and source regions.

  19. Intercomparisons of Airborne Measurements of Aerosol Ionic Chemical Composition during TRACE-P and ACE-Asia

    NASA Technical Reports Server (NTRS)

    Ma, Y.; Weber, R. J.; Maxwell-Meier, K.; Orsini, D. A.; Lee, Y.-N.; Huebert, B. J.; Howell, S. G.; Bertram, T.; Talbot, R. W.

    2003-01-01

    As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P), and the Asian Aerosol Characterization Experiment (ACEAsia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the Particle Into Liquid Sampler (PILS) for measurement of a suite of fine particle ionic compounds and a mist chamber (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and multi-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r(sup 2) of 0.95), but were systematically different by 10 +/- 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an 3 of 0.78 and a relative difference of 39% +/- 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 pm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% +/- 6% and correlated with an r(sup 2) of 0.87. Most ionic compounds were within f 30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30-40%.

  20. Intercomparisons of airborne measurements of aerosol ionic chemical composition during TRACE-P and ACE-Asia

    NASA Astrophysics Data System (ADS)

    Ma, Y.; Weber, R. J.; Maxwell-Meier, K.; Orsini, D. A.; Lee, Y.-N.; Huebert, B. J.; Howell, S. G.; Bertram, T.; Talbot, R. W.; Dibb, J. E.; Scheuer, E.

    2004-08-01

    As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P) and the Asian Aerosol Characterization Experiment (ACE-Asia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the particle into liquid sampler (PILS) for measurement of a suite of fine particle a mist chamber/ion chromatograph (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and micro-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r2 of 0.95), but were systematically different by 10 ± 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low-turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an r2 of 0.78 and a relative difference of 39% ± 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 μm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% ± 6% and correlated with an r2 of 0.87. Most ionic compounds were within ±30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30-40%.

  1. 18. VIEW OF THE CEILING, THE PIPING TRANSPORTED CHEMICALS FROM ...

    Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

    18. VIEW OF THE CEILING, THE PIPING TRANSPORTED CHEMICALS FROM A CHEMICAL PREPARATION ROOM ON THE SECOND FLOOR TO THE FIRST FLOOR PROCESS AREAS. (6/12/73) - Rocky Flats Plant, Plutonium Recovery & Fabrication Facility, North-central section of plant, Golden, Jefferson County, CO

  2. The real part of the refractive indices and effective densities for chemically segregated ambient aerosols in Guangzhou by a single particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Zhang, G.; Bi, X.; Qiu, N.; Han, B.; Lin, Q.; Peng, L.; Chen, D.; Wang, X.; Peng, P.; Sheng, G.; Zhou, Z.

    2015-12-01

    Microphysical properties of atmospheric aerosols are essential to better evaluate their radiative forcing. This paper first presents an estimate of the real part of the refractive indices (n) and effective densities (ρeff) of chemically segregated atmospheric aerosols in China. Vacuum aerodynamic diameter, chemical compositions, and light scattering intensities of individual particles were simultaneously measured by a single particle aerosol mass spectrometer (SPAMS) during fall of 2012 in Guangzhou. On the basis of Mie theory, n and ρeff were estimated for 17 particle types in four categories: organics (OC), elemental carbon (EC), internally mixed EC and OC (ECOC), and metal rich, respectively. Results indicate the presence of spherical or nearly spherical shape for majority of particle types, whose partial scattering cross section vs. sizes were well fitted to Mie theoretical modeling results. While sharing n in a narrow range (1.47-1.53), majority of particle types exhibited a wide range of ρeff (0.87-1.51 g cm-3). OC group is associated with the lowest ρeff (0.87-1.07 g cm-3), while metal rich group with the highest ones (1.29-1.51 g cm-3). It is noteworthy that a specific EC type exhibits a complex scattering curve vs. size due to the presence of both compact and irregularly shape particles. Overall, the results on detailed relationship between physical and chemical properties benefits future researches on the impact of aerosols on visibility and climate.

  3. Integrating biomass, sulphate and sea-salt aerosol responses into a microphysical chemical parcel model: implications for climate studies.

    PubMed

    Ghosh, S; Smith, M H; Rap, A

    2007-11-15

    Aerosols are known to influence significantly the radiative budget of the Earth. Although the direct effect (whereby aerosols scatter and absorb solar and thermal infrared radiation) has a large perturbing influence on the radiation budget, the indirect effect (whereby aerosols modify the microphysical and hence the radiative properties and amounts of clouds) poses a greater challenge to climate modellers. This is because aerosols undergo chemical and physical changes while in the atmosphere, notably within clouds, and are removed largely by precipitation. The way in which aerosols are processed by clouds depends on the type, abundance and the mixing state of the aerosols concerned. A parametrization with sulphate and sea-salt aerosol has been successfully integrated within the Hadley Centre general circulation model (GCM). The results of this combined parametrization indicate a significantly reduced role, compared with previous estimates, for sulphate aerosol in cloud droplet nucleation and, consequently, in indirect radiative forcing. However, in this bicomponent system, the cloud droplet number concentration, N(d) (a crucial parameter that is used in GCMs for radiative transfer calculations), is a smoothly varying function of the sulphate aerosol loading. Apart from sea-salt and sulphate aerosol particles, biomass aerosol particles are also present widely in the troposphere. We find that biomass smoke can significantly perturb the activation and growth of both sulphate and sea-salt particles. For a fixed salt loading, N(d) increases linearly with modest increases in sulphate and smoke masses, but significant nonlinearities are observed at higher non-sea-salt mass loadings. This non-intuitive N(d) variation poses a fresh challenge to climate modellers.

  4. Influences of relative humidity and particle chemical composition on aerosol scattering properties during the 2006 PRD campaign

    NASA Astrophysics Data System (ADS)

    Liu, Xingang; Cheng, Yafang; Zhang, Yuanhang; Jung, Jinsang; Sugimoto, Nobuo; Chang, Shih-Yu; Kim, Young J.; Fan, Shaojia; Zeng, Limin

    In situ measurements of the physical, chemical, and optical properties of aerosols were carried out in Guangzhou city, China, from 1 to 31 July 2006 during the Pearl River Delta (PRD) Campaign. The light extinction coefficient of the ambient atmosphere, the aerosol scattering coefficient under dry conditions, the aerosol absorption coefficient under ambient conditions, NO 2 concentration, and relative humidity (RH) were measured by transmissionmeter, an integrating nephelometer, a multi-angle absorption photometer (MAAP), a NO X analyzer, and an automatic meteorological station, respectively. Meanwhile, the molecular scattering coefficient was calculated by the Rayleigh scattering function using the US Standard Atmosphere. A method to calculate the aerosol hygroscopic growth factor f(RH), defined as the ratio of the aerosol scattering coefficient under a wet condition to that under a dry condition (40% RH), is proposed based on these optical parameters. The mean and standard deviation aerosol hygroscopic growth factors at 80% RH ( f(RH)=80%) in Ganzhou were 2.04±0.28, 2.29±0.28, and 2.68±0.59 for urban aerosols, mixed aerosols, and marine aerosols, respectively, with the air mass classification being based on the air mass source region. The relationship between f(RH) and RH is fitted by empirical equations and the fitting parameters are calculated. The relationships between f(RH)=80% and total carbon mass fraction (TCF) in PM 2.5, the water-soluble mass fraction (WSF) in PM 10, and the sea-salt aerosol mass fraction (SSF) in PM 10 reveal that the hygroscopic properties of the observed aerosol have a good positive correlation with the WSF and SSF, but have a negative correlation with the TCF.

  5. Organic aerosol evolution and transport observed at Mt. Cimone (2165 m a.s.l.), Italy, during the PEGASOS campaign

    NASA Astrophysics Data System (ADS)

    Rinaldi, M.; Gilardoni, S.; Paglione, M.; Sandrini, S.; Fuzzi, S.; Massoli, P.; Bonasoni, P.; Cristofanelli, P.; Marinoni, A.; Poluzzi, V.; Decesari, S.

    2015-10-01

    High-resolution aerosol mass spectrometer measurements were performed, for the first time, at the Mt. Cimone Global Atmosphere Watch (GAW) station between June and July 2012, within the EU project PEGASOS and the ARPA-Emilia-Romagna project SUPERSITO. Submicron aerosol was dominated by organics (63 %), with sulfate, ammonium and nitrate contributing the remaining 20, 9 and 7 %, respectively. Organic aerosol (OA) was in general highly oxygenated, consistent with the remote character of the site; our observations suggest that oxidation and secondary organic aerosol (SOA) formation processes occurred during aerosol transport to high altitudes. All of the aerosol component concentrations as well as the OA elemental ratios showed a clear daily trend, driven by the evolution of the planetary boundary layer (PBL) and by the mountain wind regime. Higher loadings and lower OA oxidation levels were observed during the day, when the site was within the PBL, and therefore affected by relatively fresh aerosol transported from lower altitudes. Conversely, lower loadings and higher OA oxidation levels were observed at night, when the top of Mt. Cimone resided in the free troposphere although affected by the transport of residual layers on several days of the campaign. Analysis of the elemental ratios in a Van Krevelen space shows that OA oxidation follows a slope comprised between -0.5 and -1, consistent with addition of carboxylic groups, with or without fragmentation of the parent molecules. The increase of carboxylic groups during OA ageing is confirmed by the increased contribution of organic fragments containing more than one oxygen atom in the free troposphere night-time mass spectra. Finally, positive matrix factorization was able to deconvolve the contributions of relatively fresh OA (OOAa) originating from the PBL, more aged OA (OOAb) present at high altitudes during periods of atmospheric stagnation, and very aged aerosols (OOAc) transported over long distances in the

  6. Long Range Transport of Aerosols and Trace Gases from China: The Role of Dry Convection.

    NASA Astrophysics Data System (ADS)

    Dickerson, R. R.; Levy, R.; Li, C.; Li, Z.; Lackson, M. T.; Jeffrey, S.

    2006-05-01

    Substantial concentrations of trace gases and aerosols are lofted and carried from Asia over the Pacific producing an inter-hemispheric impact on atmospheric chemistry and climate. The meteorological mechanism leading to this large-scale transport of dust and pollutants remains a major uncertainty in quantifying the global effects of emissions from the developing world. Models and downwind measurements have identified isentropic advection associated with wave cyclones (warm conveyor belt, WCB,circulation) as an important mechanism. We present data from a case study conducted s part of EAST-AIRE in April 2005 in which upstream convection, rather that WCB lofting appears to dominate. Observations from instrumented aircraft flights (O3, CO, SO2, and aerosol optical properties), back trajectories, and satellite images of clouds (GOES) and aerosols (MODIS) are analyzed. These show that dry (non-precipitating) convection ahead of cold fronts can be an important mechanism for converting local air pollution problems into regional or global atmospheric chemistry problems. Climatological spring (MAM) precipitation over NE China is low, about 90 mm compared to 290 mm over the NE US. Cloud cover, however, is similar with cumulus clouds reported about 7% of the time over NE China and about 9% of the time over the NE US suggesting that this is not an isolated event. Evaluation of models' convective schemes and further observations near the source regions are called for.

  7. Formation and chemical aging of secondary organic aerosol during the β-caryophyllene oxidation

    NASA Astrophysics Data System (ADS)

    Tasoglou, A.; Pandis, S. N.

    2015-06-01

    The secondary organic aerosol (SOA) production during the oxidation of β-caryophyllene by ozone (O3) and hydroxyl radicals (OH) and the subsequent chemical aging of the products during reactions with OH were investigated. Experiments were conducted with ozone and with hydroxyl radicals at low NOx (zero added NOx) and at high NOx (hundreds of parts per billion). The SOA mass yield at 10 μg m-3 of organic aerosol was 27% for the ozonolysis, 20% for the reaction with OH at low NOx, and 38% at high NOx under dry conditions, 20 °C, and ozone excess. Parameterizations of the fresh SOA yields have been developed. The average fresh SOA atomic O : C ratio varied from 0.24 to 0.34 depending on the oxidant and the NOx level, while the H : C ratio was close to 1.5 for all systems examined. An average density of 1.06 ± 0.1 μg m-3 of the β-caryophyllene SOA was estimated. The exposure to UV light had no effect on the β-caryophyllene SOA concentration and aerosol mass spectrometer (AMS) measurements. The chemical aging of the β-caryophyllene SOA produced was studied by exposing the fresh SOA to high concentrations (107 molecules cm-3) of OH for several hours. These additional reactions increased the SOA concentration by 15-40% and O : C by approximately 25%. A limited number of experiments suggested that there was a significant impact of the relative humidity on the chemical aging of the SOA. The evaporation rates of β-caryophyllene SOA were quantified by using a thermodenuder allowing us to estimate the corresponding volatility distributions and effective vaporization enthalpies.

  8. Aging of Secondary Organic Aerosol from β-Pinene: Changes in Chemical Composition, Density and Morphology

    NASA Astrophysics Data System (ADS)

    Sarrafzadeh, M.; Hastie, D. R.

    2013-12-01

    Biogenic volatile organic compounds (VOC) are emitted in large quantities into the atmosphere. These VOC, which includes β-pinene, can react to produce secondary organic aerosols (SOA), which contribute to a substantial fraction of ambient organic aerosols and are known to adversely affect visibility, climate and health. Despite this, the current knowledge regarding the SOA composition, their physical properties and the chemical aging processes they undergo in the atmosphere is limited. In this study, chemical aging of SOA generated from the photooxidation of β-pinene was investigated in the York University smog chamber. The formation and aging of both gas and particle phase products were analyzed using an atmospheric pressure chemical ionization triple quadrupole mass spectrometer. The density of secondary organic matter was also simultaneously measured over the course of the aging experiments, allowing us to improve our understanding in changes in particle composition that may occur. In addition, particle phase and shape was investigated for generated particles from β-pinene oxidation by scanning electron microscope (SEM). Results of this work, including particle density and morphology will be presented as well as comparisons of gas and particle phase products time profiles during aging.

  9. Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

    DOE PAGES

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2015-07-24

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased duringmore » photo-oxidation, and the final OA OSc ranged from -0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  10. Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

    NASA Astrophysics Data System (ADS)

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2015-07-01

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OSc ranged from -0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.

  11. Effect of phytoplankton biomass in seawater on chemical properties of sea spray aerosols.

    PubMed

    Park, Jiyeon; Kim, Dohyung; Lee, Kwangyul; Han, Seunghee; Kim, Hyunji; Williams, Leah R; Joo, Hung Soo; Park, Kihong

    2016-09-15

    This study is to investigate the effect of biological seawater properties on sea spray aerosols (SSA). Concentrations of chlorophyll-a and bacteria were measured at coastal site in Korea in fall and summer seasons. Also, aerosol mass spectrometer (AMS) was used to determine chemical constituents (organics, sulfate, nitrate, ammonium, and chloride) of non-refractory submicrometer aerosols sprayed from seawaters using a bubble bursting system. The average concentration of chlorophyll-a in seawater in fall was 1.75±0.78μg/l, whereas it significantly increased to 5.11±2.16μg/l in summer. It was found that the fraction of organics in the submicrometer SSA was higher in summer (68%) than fall (49%), and that the organic fraction in the SSA increased as the concentration of chlorophyll-a increased in seawater, suggesting that the high phytoplankton biomass in seawater could lead to the enhancement of organic species in the SSA.

  12. Aerosol chemical characteristics of an island site in the Bay of Bengal (Bhola-Bangladesh).

    PubMed

    Salam, Abdus; Bauer, Heidi; Kassin, Karin; Ullah, Shah Mohammad; Puxbaum, Hans

    2003-06-01

    Aerosol constituents (elemental carbon, organic carbon, soluble ions including organic acids, and selected trace metals) were investigated from samples of a field campaign taking place at Bhola Island in the Bay of Bengal (Bangladesh). The campaign took place in the pre-monsoon season (May 2001) using low volume samplers. Carbonaceous material comprised the majority of the analysed components. The average concentrations of EC and OC were 2.8 and 4.6 microg m(-3), respectively. Oxalic acid was the most abundant dicarboxylic acid (average 268 ng m(-3)) followed by malonic and malic acid. The contribution of carboxylic acids-carbon to organic carbon was 2.0%. Average concentrations observed for sulfate and nitrate were 3.7 microg m(-3) and 1.5 microg m(-3). Two different types of aerosol were identified at the rural background site on Bhola Island during southerly synoptic flow by means of trajectory analysis: air masses were transported from the Bay of Bengal to the sampling site in all cases. However, during "Period 1" they experienced longer residence times over the Indian Ocean, while the "Period 2" trajectories came along the Indian coast or passed over the Indian continent. During Period 1 the concentration levels of soluble ions were a factor of 4-6 lower than during Period 2. The concentrations of EC, OC and K differed less than a factor of 1.5 between the two periods. The Period 1 aerosol showed similarities to the haze layers observed during winter-monsoon conditions south of India during the INDOEX experiment. Based on EC/TC and K/EC ratios we find that around 80% of the carbonaceous aerosol from Period 1 in Bhola is from fossil fuel and only around 50% from Period 2. Absolute concentrations of carbonaceous species, soluble ions and trace metals indicate that the background site on Bhola Island is affected by emissions from urbanized regions of Southeast Asia.

  13. Aerosol assisted chemical vapour deposition control parameters for selective deposition of tungsten oxide nanostructures.

    PubMed

    Vallejos, S; Umek, P; Blackman, C

    2011-09-01

    Tungsten oxide films were deposited via Aerosol Assisted Chemical Vapour Deposition (AACVD) from the single-source precursor W(OPh)6. Film morphology and optimum deposition temperatures for formation of quasi-one-dimensional structures is influenced by the solvent 'carrier' used for deposition of the films with bulk porous films and nanostructured needles, hollow tubes and fibres obtained dependent on the solvent used and the deposition temperature. This influence of solvent could be exploited for the synthesis of other nanomaterials, and so provide a new and versatile route to develop and integrate nanostructured materials for device applications. PMID:22097557

  14. Long Range Transport of Amazon Aerosol in the Free Troposphere: Influence of Amazon Combustion Aerosol on CCN in the Pacific Marine Boundary Layer

    NASA Astrophysics Data System (ADS)

    Howell, S. G.; Clarke, A. D.; Freitag, S.; Kapustin, V.; Hudson, J.; Campos, T.; Pollack, I. B.; Heizer, C. G.; Weinheimer, A. J.

    2008-12-01

    The Pacific Atmosphere Sulfur Experiment (PASE, Sept. 2007) on the NCAR C-130 aircraft was based in the Equatorial Pacific to explore the remote marine sulfur cycle. We investigated sources that control particle number and cloud condensation nuclei, CCN, in the clean marine boundary layer (MBL). Earlier studies here demonstrated particle number above the MBL was dominated by natural production of new volatile particles in cloud outflow. However, during PASE we also found coated refractory aerosol (non-volatile at 350C) aloft were linearly related to ozone concentrations and were effective CCN at 0.2% supersaturation. These aerosol had larger diameters than naturally produced volatile aerosol and trajectory analysis traced them back to deep convection in biomass burning haze over the Amazon basin over 10,000km away. These refractory soot and/or organic aerosol appear to be detrained from deep convective clouds after the near- source scavenging of larger sizes that dominate the smoke/haze aerosol mass. Following transport and once mixed into MBL they were found to account for as much as 30% of the CCN at the value of 0.2%S (a typical value for small trade-wind cumulus clouds). Hence, cloud-scavenged combustion derived aerosol, too small to be detectable optically in satellite plumes, appears to provide seed nuclei for CCN in the remote marine boundary layer. This acts over hemispheric scales for this region and presumably elsewhere. Hence; various mechanisms including convective scavenging, long range transport, particle production aloft, entrainment into the MBL, boundary layer nucleation and sea-salt production all need to be considered in modeling the MBL CCN population.

  15. Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign

    SciTech Connect

    Lee, Y. -N.; Springston, S.; Jayne, J.; Wang, J.; Hubbe, J.; Senum, G.; Kleinman, L.; Daum, P. H.

    2014-01-01

    The chemical composition of aerosol particles (Dp ≤ 1.5 μm) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO42−, followed by Na+, Cl, Org (total organics), NH4+, and NO3, in decreasing order of importance; CH3SO3 (MSA), Ca2+, and K+ rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH4+ to SO42− equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl deficits caused by both HNO3 and H2SO4, but for the most part were externally mixed with particles, mainly SO42−. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH3 is present between 72° W and 76° W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31° S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol

  16. Long-term real-time chemical characterization of submicron aerosols at Montsec (Southern Pyrenees, 1570 m a.s.l.)

    NASA Astrophysics Data System (ADS)

    Ripoll, A.; Minguillón, M. C.; Pey, J.; Jimenez, J. L.; Day, D. A.; Querol, X.; Alastuey, A.

    2014-11-01

    Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the Western Mediterranean Basin (WMB) were conducted for 10 months (July 2011-April 2012). An Aerosol Chemical Speciation Monitor (ACSM) was co-located with other on-line and off-line PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time for this region. Seasonal trends in PM1 components are attributed to variations in: evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM1 components and causes the formation of reserve strata at relatively high altitudes. Sporadically, MSC is affected by air masses from North Africa. The combination of all these atmospheric processes at local, regional and continental scales results in a high variability of PM1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly oxygenated organic aerosol (OOA), with two different types: semi-volatile (SV-OOA) and low-volatile (LV-OOA), and both showed marked diurnal cycles regardless of the air mass origin, especially SV-OOA. This different diurnal variation compared to inorganic aerosols suggested that OA components at MSC are not only associated with anthropogenic and long-range-transported secondary OA (SOA), but also with recently-produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere

  17. Improving aerosol interaction with clouds and precipitation in a regional chemical weather modeling system

    NASA Astrophysics Data System (ADS)

    Zhou, C.; Zhang, X.; Gong, S.; Wang, Y.; Xue, M.

    2016-01-01

    A comprehensive aerosol-cloud-precipitation interaction (ACI) scheme has been developed under a China Meteorological Administration (CMA) chemical weather modeling system, GRAPES/CUACE (Global/Regional Assimilation and PrEdiction System, CMA Unified Atmospheric Chemistry Environment). Calculated by a sectional aerosol activation scheme based on the information of size and mass from CUACE and the thermal-dynamic and humid states from the weather model GRAPES at each time step, the cloud condensation nuclei (CCN) are interactively fed online into a two-moment cloud scheme (WRF Double-Moment 6-class scheme - WDM6) and a convective parameterization to drive cloud physics and precipitation formation processes. The modeling system has been applied to study the ACI for January 2013 when several persistent haze-fog events and eight precipitation events occurred.

    The results show that aerosols that interact with the WDM6 in GRAPES/CUACE obviously increase the total cloud water, liquid water content, and cloud droplet number concentrations, while decreasing the mean diameters of cloud droplets with varying magnitudes of the changes in each case and region. These interactive microphysical properties of clouds improve the calculation of their collection growth rates in some regions and hence the precipitation rate and distributions in the model, showing 24 to 48 % enhancements of threat score for 6 h precipitation in almost all regions. The aerosols that interact with the WDM6 also reduce the regional mean bias of temperature by 3 °C during certain precipitation events, but the monthly means bias is only reduced by about 0.3 °C.

  18. Chemical Nature Of Titan’s Organic Aerosols Constrained from Spectroscopic and Mass Spectrometric Observations

    NASA Astrophysics Data System (ADS)

    Imanaka, Hiroshi; Cruikshank, D. P.

    2012-10-01

    The Cassini-Huygens observations greately extend our knowledge about Titan’s organic aerosols. The Cassini INMS and CAPS observations clearly demonstrate the formation of large organic molecules in the ionosphere [1, 2]. The VIMS and CIRS instruments have revealed spectral features of the haze covering the mid-IR and far-IR wavelengths [3, 4, 5, 6]. This study attempts to speculate the possible chemical nature of Titan’s aerosols by comparing the currently available observations with our laboratory study. We have conducted a series of cold plasma experiment to investigate the mass spectrometric and spectroscopic properties of laboratory aerosol analogs [7, 8]. Titan tholins and C2H2 plasma polymer are generated with cold plasma irradiations of N2/CH4 and C2H2, respectively. Laser desorption mass spectrum of the C2H2 plasma polymer shows a reasonable match with the CAPS positive ion mass spectrum. Furthermore, spectroscopic features of the the C2H2 plasma polymer in mid-IR and far-IR wavelegths qualitatively show reasonable match with the VIMS and CIRS observations. These results support that the C2H2 plasma polymer is a good candidate material for Titan’s aerosol particles at the altitudes sampled by the observations. We acknowledge funding supports from the NASA Cassini Data Analysis Program, NNX10AF08G, and from the NASA Exobiology Program, NNX09AM95G, and the Cassini Project. [1] Waite et al. (2007) Science 316, 870-875. [2] Crary et al. (2009) Planet. Space Sci. 57, 1847-1856. [3] Bellucci et al. (2009) Icarus 201, 198-216. [4] Anderson and Samuelson (2011) Icarus 212, 762-778. [5] Vinatier et al. (2010) Icarus 210, 852-866. [6] Vinatier et al. (2012) Icarus 219, 5-12. [7] Imanaka et al. (2004) Icarus 168, 344-366. [8] Imanaka et al. (2012) Icarus 218, 247-261.

  19. Influence of Aerosol Chemical Composition on Heterogeneous Ice Formation under Mid-Upper Troposphere Conditions

    NASA Astrophysics Data System (ADS)

    Kanji, Z. A.; Niemand, M.; Saathoff, H.; Möhler, O.; Chou, C.; Abbatt, J.; Stetzer, O.

    2011-12-01

    Aerosols are involved in cooling/warming the atmosphere directly via interaction with incoming solar radiation (aerosol direct effect), or via their ability to act as cloud condensation or ice nuclei (IN) and thus play a role in cloud formation (indirect effect). In particular, the physical properties of aerosols such as size and solubility and chemical composition can influence their behavior and fate in the atmosphere. Ice nucleation taking place via IN is termed as heterogeneous ice nucleation and can take place with via deposition (ice forming on IN directly from the vapor phase), condensation/immersion (freezing via formation of the liquid phase on IN) or condensation (IN colliding with supercooled liquid drops). This presentation shows how the chemical composition and surface area of various tropospherically relevant aerosols influence conditions of temperature (T) and relative humidity (RH) required for heterogeneous ice formation conditions in the mid-upper troposphere regime (253 - 220K)? Motivation for this comes first from, the importance of being able to predict ice formation accurately so as to understand the hydrological cycle since the ice is the primary initiator of precipitation forming clouds. Second, the tropospheric budget of water vapour, an especially active greenhouse gas is strongly influenced by ice nucleation and growth. Third, ice surfaces in the atmosphere act as heterogeneous surfaces for chemical reactions of trace gases (e.g., SO2, O3, NOx and therefore being able to accurately estimate ice formation rates and quantify ice surface concentrations will allow a more accurate calculation of trace gas budgets in the troposphere. Ice nucleation measurements were conducted using a self-developed continuous flow diffusion chamber and static chamber. A number of tropospherically relevant particulates with naturally-varying and laboratory-modified surface chemistry/structure were investigated for their ice formation efficiency based on highest

  20. Chemical speciation of chlorine in atmospheric aerosol samples by high-resolution proton induced X-ray emission spectroscopy

    NASA Astrophysics Data System (ADS)

    Kertész, Zsófia; Furu, Enikő; Kavčič, Matjaž

    2013-01-01

    Chlorine is a main elemental component of atmospheric particulate matter (APM). The knowledge of the chemical form of chlorine is of primary importance for source apportionment and for estimation of health effects of APM. In this work the applicability of high-resolution wavelength dispersive proton induced X-ray emission (PIXE) spectroscopy for chemical speciation of chlorine in fine fraction atmospheric aerosols is studied. A Johansson-type crystal spectrometer with energy resolution below the natural linewidth of Cl K lines was used to record the high-resolution Kα and Kβ proton induced spectra of several reference Cl compounds and two atmospheric aerosol samples, which were collected for conventional PIXE analysis. The Kα spectra which refers to the oxidation state, showed very minor differences due to the high electronegativity of Cl. However, the Kβ spectra exhibited pronounced chemical effects which were significant enough to perform chemical speciation. The major chlorine component in two fine fraction aerosol samples collected during a 2010 winter campaign in Budapest was clearly identified as NaCl by comparing the high-resolution Cl Kβ spectra from the aerosol samples with the corresponding reference spectra. This work demonstrates the feasibility of high-resolution PIXE method for chemical speciation of Cl in aerosols.

  1. CET89 - CHEMICAL EQUILIBRIUM WITH TRANSPORT PROPERTIES, 1989

    NASA Technical Reports Server (NTRS)

    Mcbride, B.

    1994-01-01

    Scientists and engineers need chemical equilibrium composition data to calculate the theoretical thermodynamic properties of a chemical system. This information is essential in the design and analysis of equipment such as compressors, turbines, nozzles, engines, shock tubes, heat exchangers, and chemical processing equipment. The substantial amount of numerical computation required to obtain equilibrium compositions and transport properties for complex chemical systems led scientists at NASA's Lewis Research Center to develop CET89, a program designed to calculate the thermodynamic and transport properties of these systems. CET89 is a general program which will calculate chemical equilibrium compositions and mixture properties for any chemical system with available thermodynamic data. Generally, mixtures may include condensed and gaseous products. CET89 performs the following operations: it 1) obtains chemical equilibrium compositions for assigned thermodynamic states, 2) calculates dilute-gas transport properties of complex chemical mixtures, 3) obtains Chapman-Jouguet detonation properties for gaseous species, 4) calculates incident and reflected shock properties in terms of assigned velocities, and 5) calculates theoretical rocket performance for both equilibrium and frozen compositions during expansion. The rocket performance function allows the option of assuming either a finite area or an infinite area combustor. CET89 accommodates problems involving up to 24 reactants, 20 elements, and 600 products (400 of which may be condensed). The program includes a library of thermodynamic and transport properties in the form of least squares coefficients for possible reaction products. It includes thermodynamic data for over 1300 gaseous and condensed species and transport data for 151 gases. The subroutines UTHERM and UTRAN convert thermodynamic and transport data to unformatted form for faster processing. The program conforms to the FORTRAN 77 standard, except for

  2. Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

    uncertainties by "the I-beams". Only an uncertainty range rather than a best estimate is presented for direct aerosol forcing by mineral dust and for indirect aerosol forcing. An assessment of the present level of scientific understanding is indicated at the bottom of the figure (reproduced by permission of Intergovernmental Panel on Climate Change). The importance of atmospheric aerosols to issues of societal concern has motivated much research intended to describe their loading, distribution, and properties and to develop understanding of the controlling processes to address such issues as air pollution, acid deposition, and climate influences of aerosols. However, description based wholly on measurements will inevitably be limited in its spatial and temporal coverage and in the limited characterization of aerosol properties. These limitations are even more serious for predictions of future emissions and provide motivation for concurrent theoretical studies and development of model-based description of atmospheric aerosols.An important long-range goal, which has already been partly realized, is to develop quantitative understanding of the processes that control aerosol loading, composition, and microphysical properties as well as the resultant optical and cloud-nucleating properties. An objective is to incorporate these results into chemical transport models that can be used for predictions. Such models are required, for example, to design approaches to achieve air quality standards and to assess and predict aerosol influences on climate change. Much current research is directed toward enhancing this understanding and to evaluating it by comparison of model results and observations. However, compared to gases, models involving particles are far more complex because of the need to specify additional parameters such as particle sizes and size distributions, compositions as a function of size, particle shapes, and temporal and spatial variations, including reactions that occur

  3. Effects of crop residue burning on aerosol properties, plume characteristics, and long-range transport over northern India

    NASA Astrophysics Data System (ADS)

    Kaskaoutis, D. G.; Kumar, S.; Sharma, D.; Singh, R. P.; Kharol, S. K.; Sharma, M.; Singh, A. K.; Singh, S.; Singh, Atinderpal; Singh, D.

    2014-05-01

    Aerosol emissions from biomass burning are of specific interest over the globe due to their strong radiative impacts and climate implications. The present study examines the impact of paddy crop residue burning over northern India during the postmonsoon (October-November) season of 2012 on modification of aerosol properties, as well as the long-range transport of smoke plumes, altitude characteristics, and affected areas via the synergy of ground-based measurements and satellite observations. During this period, Moderate Resolution Imaging Spectroradiometer (MODIS) images show a thick smoke/hazy aerosol layer below 2-2.5 km in the atmosphere covering nearly the whole Indo-Gangetic Plains (IGP). The air mass trajectories originating from the biomass-burning source region over Punjab at 500 m reveal a potential aerosol transport pathway along the Ganges valley from west to east, resulting in a strong aerosol optical depth (AOD) gradient. Sometimes, depending upon the wind direction and meteorological conditions, the plumes also influence central India, the Arabian Sea, and the Bay of Bengal, thus contributing to Asian pollution outflow. The increased number of fire counts (Terra and Aqua MODIS data) is associated with severe aerosol-laden atmospheres (AOD500 nm > 1.0) over six IGP locations, high values of Ångström exponent (>1.2), high particulate mass 2.5 (PM2.5) concentrations (>100-150 µgm-3), and enhanced Ozone Monitoring Instrument Aerosol Index gradient (~2.5) and NO2 concentrations (~6 × 1015 mol/cm2), indicating the dominance of smoke aerosols from agricultural crop residue burning. The aerosol size distribution is shifted toward the fine-mode fraction, also exhibiting an increase in the radius of fine aerosols due to coagulation processes in a highly turbid environment. The spectral variation of the single-scattering albedo reveals enhanced dominance of moderately absorbing aerosols, while the aerosol properties, modification, and mixing atmospheric

  4. Transport of Aerosols from Asia and Their Radiative Effects Over the Western Pacific: A 3-D Model Study for ACE-Asia Experiment During Spring 2001

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Flatau, Piotr; Anderson, Tad; Masonis, Sarah; Russell, Phil; Schmid, Beat; Livingston, John; Redemann, Jens; Kahn, Ralph; Bhartia, P. K. (Technical Monitor)

    2001-01-01

    The Aerosol Characterization Experiment-Asia (ACE-Asia) took place in Spring 2001 in the East Asia-West Pacific Ocean. During the ACE-Asia intensive field operation period, high concentrations of dust and anthropogenic aerosols were observed over the Yellow Sea and the Sea of Japan, which were transported out from the Asian continent, with the plume often extending to 6-8 km altitude. The multi-component aerosols originated from Asia are expected to exert a significant radiative forcing over the Pacific region. We present here results from the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model of aerosol transport and radiative forcing in the context of ACE-Asia. The model calculated aerosol concentrations, extinctions, optical thickness, size distributions, and vertical profiles are compared with the aircraft and ship measurements, and the distributions of aerosols are compared with satellite data. The model will be used to understand the origins of the aerosols observed in ACE-Asia, estimate the contributions from anthropogenic and natural aerosols to the total aerosol optical thickness, investigate the effects of humidification and clouds on aerosol properties, and assess the radiative forcing of Asian aerosols over the Pacific region and in the northern hemisphere.

  5. GUIDE TO CALCULATING TRANSPORT EFFICIENCY OF AEROSOLS IN OCCUPATIONAL AIR SAMPLING SYSTEMS

    SciTech Connect

    Hogue, M.; Hadlock, D.; Thompson, M.; Farfan, E.

    2013-11-12

    This report will present hand calculations for transport efficiency based on aspiration efficiency and particle deposition losses. Because the hand calculations become long and tedious, especially for lognormal distributions of aerosols, an R script (R 2011) will be provided for each element examined. Calculations are provided for the most common elements in a remote air sampling system, including a thin-walled probe in ambient air, straight tubing, bends and a sample housing. One popular alternative approach would be to put such calculations in a spreadsheet, a thorough version of which is shared by Paul Baron via the Aerocalc spreadsheet (Baron 2012). To provide greater transparency and to avoid common spreadsheet vulnerabilities to errors (Burns 2012), this report uses R. The particle size is based on the concept of activity median aerodynamic diameter (AMAD). The AMAD is a particle size in an aerosol where fifty percent of the activity in the aerosol is associated with particles of aerodynamic diameter greater than the AMAD. This concept allows for the simplification of transport efficiency calculations where all particles are treated as spheres with the density of water (1g cm-3). In reality, particle densities depend on the actual material involved. Particle geometries can be very complicated. Dynamic shape factors are provided by Hinds (Hinds 1999). Some example factors are: 1.00 for a sphere, 1.08 for a cube, 1.68 for a long cylinder (10 times as long as it is wide), 1.05 to 1.11 for bituminous coal, 1.57 for sand and 1.88 for talc. Revision 1 is made to correct an error in the original version of this report. The particle distributions are based on activity weighting of particles rather than based on the number of particles of each size. Therefore, the mass correction made in the original version is removed from the text and the calculations. Results affected by the change are updated.

  6. Measurements of the chemical, physical, and optical properties of single aerosol particles

    NASA Astrophysics Data System (ADS)

    Moffet, Ryan Christopher

    Knowledge of aerosol physical, chemical, optical properties is essential for judging the effect that particulates have on human health, climate and visibility. The aerosol time-of-flight mass spectrometer (ATOFMS) is capable of measuring, in real-time, the size and chemical composition of atmospheric aerosols. This was exemplified by the recent deployments of the ATOFMS to Mexico City and Riverside. The ATOFMS provided rapid information about the major particle types present in the atmosphere. Industrial sources of particles, such as fine mode particles containing lead, zinc and chloride were detected in Mexico City. The rapid time response of the ATOFMS was also exploited to characterize a coarse particle concentrator used in human health effects studies. The ATOFMS showed the ability to detect changes in particle composition with a time resolution of 15 min during short 2 hour human exposure studies. As a major component of this work, an optical measurement has been added to the ATOFMS. The scattered light intensity was acquired for each sized and chemically analyzed particle. This scattering information together with the particle aerodynamic diameter, enabled the refractive index and density of the aerosol to be retrieved. This method was validated in the laboratory using different test particles such as oils, aqueous salt solutions and black carbon particles. It was found that the nozzle-type inlet does not evaporate aqueous salt particles as has been observed for aerodynamic lens inlets. These new optical and microphysical measurements were integrated into the ATOFMS for field deployment in Riverside and Mexico City. For both cities, the different mixing states were found to have unique refractive indexes and densities. A fraction of the strongly absorbing elemental carbon particles were observed to have a spherical morphology due to heavy mixing with secondary species. In addition to the quantitative refractive index and effective density measurements

  7. Chemical properties and morphology of Marine Aerosol in the Mediterranean atmosphere: a mesocosm study

    NASA Astrophysics Data System (ADS)

    D'Anna, Barbara; Sellegri, Karine; Charrière, Bruno; Sempéré, Richard; Mas, Sébastien; Marchand, Nicolas; George, Christian; Même, Aurèlie; R'mili, Badr; Delmont, Anne; Schwier, Allison; Rose, Clémence; Colomb, Aurèlie; Pey, Jorge; Langley Dewitt, Helen

    2014-05-01

    The Mediterranean Sea is a special marine environment characterized by low biological activity and high anthropogenic pressure. It is often difficult to discriminate the contribution of Primary Sea Salt Aerosol formed at the sea surface from background level of the aerosol. An alternative tool to study the sea-air exchanges in a controlled environment is provided by the mesocosms, which represent an important link between field studies and laboratory experiments. The sea-air transfer of particles and gases was investigated in relation to water chemical composition and biological activity during a mesocosm experiment within the SAM project (Sources of marine Aerosol in the Mediterranean) at the Oceanographic and Marine Station STARESO in Western Corsica (May 2013). Three 2 m mesocosms were filled with screened (<1000 µm) 2260 L of subsurface (1 m) seawater and covered with a transparent Teflon film dome to minimize atmospheric contamination. The mesocosms were equipped with a pack of optical and physicochemical sensors and received different treatments: one was left unchanged as control and two were enriched by addition of nitrates and phosphates respecting Redfield ratio (N:P = 16). The evolution of the three systems was followed for 20 days. The set of sensors in each mesocosm was allowed to monitor, at high frequency (every 10 min), the water temperature, conductivity, pH, incident light, fluorescence of chlorophyll a and dissolved oxygen concentration. The mesocosm seawaters were daily sampled for chemical (colored dissolved organic matter, particulate matter and related polar compounds, transparent polysaccharides and nutrients concentration) and biological (chlorophyll a, virus, phytoplankton and zooplankton) analyses. Both dissolved and gaseous VOCs were also analyzed. In addition, few liters of seawater from each mesocosm were daily and immediately collected and transferred to a bubble-bursting apparatus to simulate nascent sea spray aerosol. On

  8. Modal structure of chemical mass size distribution in the high Arctic aerosol

    NASA Astrophysics Data System (ADS)

    Hillamo, Risto; Kerminen, Veli-Matti; Aurela, Minna; MäKelä, Timo; Maenhaut, Willy; Leek, Caroline

    2001-11-01

    Chemical mass size distributions of aerosol particles were measured in the remote marine boundary layer over the central Arctic Ocean as part of the Atmospheric Research Program on the Arctic Ocean Expedition 1996 (AOE-96). An inertial impaction method was used to classify aerosol particles into different size classes for subsequent chemical analysis. The particle chemical composition was determined by ion chromatography and by the particle-induced X-ray emission technique. Continuous particle size spectra were extracted from the raw data using a data inversion method. Clear and varying modal structures for aerosols consisting of primary sea-salt particles or of secondary particles related to dimethyl sulfide emissions were found. Concentration levels of all modes decreased rapidly when the distance from open sea increased. In the submicrometer size range the major ions found by ion chromatography were sulfate, methane sulfonate, and ammonium. They had most of the time a clear Aitken mode and one or two accumulation modes, with aerodynamic mass median diameters around 0.1 μm, 0.3 μm, and between 0.5-1.0 μm, respectively. The overall submicron size distributions of these three ions were quite similar, suggesting that they were internally mixed over most of this size range. The corresponding modal structure was consistent with the mass size distributions derived from the particle number size distributions measured with a differential mobility particle sizer. The Aitken to accumulation mode mass ratio for nss-sulfate and MSA was substantially higher during clear skies than during cloudy periods. Primary sea-salt particles formed a mode with an aerodynamic mass median diameter around 2 μm. In general, the resulting continuous mass size distributions displayed a clear modal structure consistent with our understanding of the two known major source mechanisms. One is the sea-salt aerosol emerging from seawater by bubble bursting. The other is related to

  9. Non-spherical aerosol transport under oscillatory shear flows at low-Reynolds numbers

    NASA Astrophysics Data System (ADS)

    Shachar Berman, Lihi; Delorme, Yann; Hofemeier, Philipp; Frankel, Steven; Sznitman, Josue

    2014-11-01

    Most airborne particles are intrinsically non-spherical. In particular, non-spherical particles with high aspect ratios, such as fibers, are acknowledged to be more hazardous than their spherical counterparts due to their ability to penetrate into deeper lung regions, causing serious pulmonary diseases. Not only do particle properties such as size, shape, and density have a major impact on particle transport, for non-spherical aerosols, their orientations also greatly influence particle trajectories due to modified lift and drag characteristics. Until present, however, most of our understanding of the dynamics of inhaled particles in the deep airways of the lungs has been limited to spherical particles only. In the present work, we seek to quantify through numerical simulations the transport of non-spherical airborne particles and their deposition under oscillatory shear flows at low Reynolds numbers, characteristic of acinar airways. Here, the Euler-Lagrangian model is used to solve the translational movement of a fiber, whereas the Eulerian rotational equations are introduced and solved to predict detailed unsteady fiber orientations. Overall, our efforts provide new insight into realistic dynamics of inhaled non-spherical aerosols under characteristic breathing motions.

  10. Chemical method to enhance transungual transport and iontophoresis efficiency.

    PubMed

    Hao, Jinsong; Smith, Kelly A; Li, S Kevin

    2008-06-01

    Transungual transport is hindered by the inherent small effective pore size of the nail even when it is fully hydrated. The objectives of this study were to determine the effects of chemical enhancers thioglycolic acid (TGA), glycolic acid (GA), and urea (UR) on transungual transport and iontophoresis efficiency. In vitro passive and iontophoretic transport experiments of model permeants mannitol (MA), UR, and tetraethylammonium (TEA) ion across the fully hydrated, enhancer-treated and untreated human nail plates were performed in phosphate-buffered saline. The transport experiments consisted of several stages, alternating between passive and anodal iontophoretic transport at 0.1mA. Nail water uptake experiments were conducted to determine the water content of the enhancer-treated nails. The effects of the enhancers on transungual electroosmosis were also evaluated. Nails treated with GA and UR did not show any transport enhancement. Treatment with TGA at 0.5M enhanced passive and iontophoretic transungual transport of MA, UR, and TEA. Increasing the TGA concentration to 1.8M did not further increase TEA iontophoresis efficiency. The effect of TGA on the nail plates was irreversible. The present study shows the possibility of using a chemical enhancer to reduce transport hindrance in the nail plate and thus enhance passive and iontophoretic transungual transport. PMID:18321669

  11. Chemical method to enhance transungual transport and iontophoresis efficiency.

    PubMed

    Hao, Jinsong; Smith, Kelly A; Li, S Kevin

    2008-06-01

    Transungual transport is hindered by the inherent small effective pore size of the nail even when it is fully hydrated. The objectives of this study were to determine the effects of chemical enhancers thioglycolic acid (TGA), glycolic acid (GA), and urea (UR) on transungual transport and iontophoresis efficiency. In vitro passive and iontophoretic transport experiments of model permeants mannitol (MA), UR, and tetraethylammonium (TEA) ion across the fully hydrated, enhancer-treated and untreated human nail plates were performed in phosphate-buffered saline. The transport experiments consisted of several stages, alternating between passive and anodal iontophoretic transport at 0.1mA. Nail water uptake experiments were conducted to determine the water content of the enhancer-treated nails. The effects of the enhancers on transungual electroosmosis were also evaluated. Nails treated with GA and UR did not show any transport enhancement. Treatment with TGA at 0.5M enhanced passive and iontophoretic transungual transport of MA, UR, and TEA. Increasing the TGA concentration to 1.8M did not further increase TEA iontophoresis efficiency. The effect of TGA on the nail plates was irreversible. The present study shows the possibility of using a chemical enhancer to reduce transport hindrance in the nail plate and thus enhance passive and iontophoretic transungual transport.

  12. Trend of surface solar radiation over Asia simulated by aerosol transport-climate model

    NASA Astrophysics Data System (ADS)

    Takemura, T.; Ohmura, A.

    2009-12-01

    Long-term records of surface radiation measurements indicate a decrease in the solar radiation between the 1950s and 1980s (“global dimming”), then its recovery afterward (“global brightening”) at many locations all over the globe [Wild, 2009]. On the other hand, the global brightening is delayed over the Asian region [Ohmura, 2009]. It is suggested that these trends of the global dimming and brightening are strongly related with a change in aerosol loading in the atmosphere which affect the climate change through the direct, semi-direct, and indirect effects. In this study, causes of the trend of the surface solar radiation over Asia during last several decades are analyzed with an aerosol transport-climate model, SPRINTARS. SPRINTARS is coupled with MIROC which is a general circulation model (GCM) developed by Center for Climate System Research (CCSR)/University of Tokyo, National Institute for Environmental Studies (NIES), and Frontier Research Center for Global Change (FRCGC) [Takemura et al., 2000, 2002, 2005, 2009]. The horizontal and vertical resolutions are T106 (approximately 1.1° by 1.1°) and 56 layers, respectively. SPRINTARS includes the transport, radiation, cloud, and precipitation processes of all main tropospheric aerosols (black and organic carbons, sulfate, soil dust, and sea salt). The model treats not only the aerosol mass mixing ratios but also the cloud droplet and ice crystal number concentrations as prognostic variables, and the nucleation processes of cloud droplets and ice crystals depend on the number concentrations of each aerosol species. Changes in the cloud droplet and ice crystal number concentrations affect the cloud radiation and precipitation processes in the model. Historical emissions, that is consumption of fossil fuel and biofuel, biomass burning, aircraft emissions, and volcanic eruptions are prescribed from database provided by the Aerosol Model Intercomparison Project (AeroCom) and the latest IPCC inventories

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

    NASA Astrophysics Data System (ADS)

    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

  14. Chemical sinks of organic aerosol: kinetics and products of the heterogeneous oxidation of erythritol and levoglucosan.

    PubMed

    Kessler, Sean H; Smith, Jared D; Che, Dung L; Worsnop, Douglas R; Wilson, Kevin R; Kroll, Jesse H

    2010-09-15

    The heterogeneous oxidation of pure erythritol (C(4)H(10)O(4)) and levoglucosan (C(6)H(10)O(5)) particles was studied in order to evaluate the effects of atmospheric aging on the mass and chemical composition of atmospheric organic aerosol. In contrast to what is generally observed for the heterogeneous oxidation of reduced organics, substantial volatilization is observed in both systems. However, the ratio of the decrease in particle mass to the decrease in the concentration of the parent species is about three times higher for erythritol than for levoglucosan, indicating that details of chemical structure (such as carbon number, cyclic moieties, and oxygen-containing functional groups) play a governing role in the importance of volatilization reactions. The kinetics of the reaction indicate that while both compounds react at approximately the same rate, reactions of their oxidation products appear to be slowed substantially. Estimates of volatilities of organic species based on elemental composition measurements suggest that the heterogeneous oxidation of oxygenated organics may be an important loss mechanism of organic aerosol.

  15. Aerosol-Assisted Chemical Vapor Deposited Thin Films for Space Photovoltaics

    NASA Technical Reports Server (NTRS)

    Hepp, Aloysius F.; McNatt, Jeremiah; Dickman, John E.; Jin, Michael H.-C.; Banger, Kulbinder K.; Kelly, Christopher V.; AquinoGonzalez, Angel R.; Rockett, Angus A.

    2006-01-01

    Copper indium disulfide thin films were deposited via aerosol-assisted chemical vapor deposition using single source precursors. Processing and post-processing parameters were varied in order to modify morphology, stoichiometry, crystallography, electrical properties, and optical properties in order to optimize device-quality material. Growth at atmospheric pressure in a horizontal hot-wall reactor at 395 C yielded best device films. Placing the susceptor closer to the evaporation zone and flowing a more precursor-rich carrier gas through the reactor yielded shinier, smoother, denser-looking films. Growth of (112)-oriented films yielded more Cu-rich films with fewer secondary phases than growth of (204)/(220)-oriented films. Post-deposition sulfur-vapor annealing enhanced stoichiometry and crystallinity of the films. Photoluminescence studies revealed four major emission bands (1.45, 1.43, 1.37, and 1.32 eV) and a broad band associated with deep defects. The highest device efficiency for an aerosol-assisted chemical vapor deposited cell was 1.03 percent.

  16. Aerosols near by a coal fired thermal power plant: chemical composition and toxic evaluation.

    PubMed

    Jayasekher, T

    2009-06-01

    Industrial processes discharge fine particulates containing organic as well as inorganic compounds into the atmosphere which are known to induce damage to cell and DNA, both in vitro and in vivo. Source and area specific studies with respect to the chemical composition, size and shape of the particles, and toxicity evaluations are very much limited. This study aims to investigate the trace elements associated with the aerosol particles distributed near to a coal burning thermal power plant and to evaluate their toxicity through Comet assay. PM(10) (particles determined by mass passing an inlet with a 50% cut-off efficiency having a 10-microm aerodynamic diameter) samples were collected using respirable dust samplers. Twelve elements (Cr, Mn, Fe, Co, Ni, Cu, Zn, Cd, Pb, Se, Hg, and As) were analyzed using ICP-AES. Comet assay was done with the extracts of aerosols in phosphate buffered saline (PBS). Results show that Fe and Zn were found to be the predominant elements along with traces of other analyzed elements. Spherical shaped ultrafine particles of <1 microm aerodynamic diameter were detected through scanning electron microscope. PM(10) particles near to the coal burning power plant produced comets indicating their potential to induce DNA damage. DNA damage property is found to be depending upon the chemical characteristics of the components associated with the particles besides the physical properties such as size and shape.

  17. Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) - chemical composition, origins and organic aerosol sources

    NASA Astrophysics Data System (ADS)

    Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Canonaco, F.; Henne, S.; Herrmann, E.; Gysel, M.; Steinbacher, M.; Baltensperger, U.; Prévôt, A. S. H.

    2015-07-01

    Chemically resolved (organic, nitrate, sulphate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high altitude site Jungfraujoch (3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations shows that the highest (especially sulphate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71-88 %), with lesser contributions from local tourism-related activities (7-12 %) and hydrocarbon-like OA related to regional vertical transport (3-9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence enabling the assessment of the composition for each. Most nitrate and part of the OA is injected from the regional PBL while sulphate is mainly produced in the FT. The south/north gradient of sulphate is also pronounced in FT air masses (sulphate mass fraction from the south: 45 %, from

  18. Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) - chemical composition, origins and organic aerosol sources

    NASA Astrophysics Data System (ADS)

    Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Canonaco, F.; Croteau, P. L.; Gysel, M.; Henne, S.; Herrmann, E.; Jayne, J. T.; Steinbacher, M.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

    2015-10-01

    Chemically resolved (organic, nitrate, sulfate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high-altitude site Jungfraujoch (JFJ; 3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations show that the highest (especially sulfate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ, while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71-88 %), with lesser contributions from local tourism-related activities (7-12 %) and hydrocarbon-like OA related to regional vertical transport (3-9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long-range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small-scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence, enabling the assessment of the composition for each. Most nitrate and part of the OA are injected from the regional PBL, while sulfate is mainly produced in the FT. The south/north gradient of sulfate is also pronounced in FT air masses (sulfate mass fraction from the south: 45

  19. Morphological and chemical changes of aerosolized E. coli treated with a dielectric barrier discharge.

    PubMed

    Romero-Mangado, Jaione; Nordlund, Dennis; Soberon, Felipe; Deane, Graham; Maughan, Kevin; Sainio, Sami; Singh, Gurusharan; Daniels, Stephen; Saunders, Ian T; Loftus, David; Meyyappan, M; Koehne, Jessica; Gandhiraman, Ram P

    2016-06-01

    This study presents the morphological and chemical modification of the cell structure of aerosolized Escherichia coli treated with a dielectric barrier discharge (DBD). Exposure to DBD results in severe oxidation of the bacteria, leading to the formation of hydroxyl groups and carbonyl groups and a significant reduction in amine functionalities and phosphate groups. Near edge x-ray absorption fine structure (NEXAFS) measurements confirm the presence of additional oxide bonds upon DBD treatment, suggesting oxidation of the outer layer of the cell wall. Electron microscopy images show that the bacteria undergo physical distortion to varying degrees, resulting in deformation of the bacterial structure. The electromagnetic field around the DBD coil causes severe damage to the cell structure, possibly resulting in leakage of vital cellular materials. The oxidation and chemical modification of the bacterial components are evident from the Fourier transform infrared spectroscopy and NEXAFS results. The bacterial reculture experiments confirm inactivation of airborne E. coli upon treating with DBD. PMID:26872580

  20. Analysis of the Interaction and Transport of Aerosols with Cloud or Fog in East Asia from AERONET and Satellite Remote Sensing: 2012 DRAGON Campaigns and Climatological Data

    NASA Astrophysics Data System (ADS)

    Eck, T. F.; Holben, B. N.; Reid, J. S.; Lynch, P.; Schafer, J.; Giles, D. M.; Kim, J.; Kim, Y. J.; Sano, I.; Arola, A. T.; Munchak, L. A.; O'Neill, N. T.; Lyapustin, A.; Sayer, A. M.; Hsu, N. Y. C.; Randles, C. A.; da Silva, A. M., Jr.; Govindaraju, R.; Hyer, E. J.; Pickering, K. E.; Crawford, J. H.; Sinyuk, A.; Smirnov, A.

    2015-12-01

    Ground-based remote sensing observations from Aerosol Robotic Network (AERONET) sun-sky radiometers have recently shown several instances where cloud-aerosol interaction had resulted in modification of aerosol properties and/or in difficulty identifying some major pollution transport events due to aerosols being imbedded in cloud systems. Major Distributed Regional Aerosol Gridded Observation Networks (DRAGON) field campaigns involving multiple AERONET sites in Japan and South Korea during Spring of 2012 have yielded observations of aerosol transport associated with clouds and/or aerosol properties modification as a result of fog interaction. Analysis of data from the Korean and Japan DRAGON campaigns shows that major fine-mode aerosol transport events are sometimes associated with extensive cloud cover and that cloud-screening of observations often filter out significant pollution aerosol transport events. The Spectral De-convolution Algorithm (SDA) algorithm was utilized to isolate and analyze the fine-mode aerosol optical depth (AODf) signal from AERONET data for these cases of persistent and extensive cloud cover. Satellite retrievals of AOD from MODIS sensors (from Dark Target, Deep Blue and MAIAC algorithms) were also investigated to assess the issue of detectability of high AOD events associated with high cloud fraction. Underestimation of fine mode AOD by the Navy Aerosol Analysis and Prediction System (NAAPS) and by the NASA Modern-Era Retrospective Analysis For Research And Applications Aerosol Re-analysis (MERRAaero) models at very high AOD at sites in China and Korea was observed, especially for observations that are cloud screened by AERONET (Level 2 data). Additionally, multi-year monitoring at several AERONET sites are examined for climatological statistics of cloud screening of fine mode aerosol events. Aerosol that has been affected by clouds or the near-cloud environment may be more prevalent than AERONET data suggest due to inherent difficulty in

  1. Long-Range Transport of Perchlorate Observed in the Atmospheric Aerosols Collected at Okinawa Island, Japan

    NASA Astrophysics Data System (ADS)

    Handa, D.; Okada, K.; Kuroki, Y.; Nakama, Y.; Nakajima, H.; Arakaki, T.; Tanahara, A.; Oomori, T.; Miyagi, T.; Kadena, H.; Ishizaki, T.; Nakama, F.

    2007-12-01

    aerosols collected at CHAAMS was probably transported from the Asian continent.

  2. Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

    NASA Astrophysics Data System (ADS)

    Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

    2013-12-01

    Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

  3. [Chemical Composition of the Single Particle Aerosol in Winter in Nanning Using SPAMS].

    PubMed

    Liu, Hui-lin; Song, Hong-jun; Chen, Zhi-ming; Huang, Jiong-li; Yang, Jun-chao; Mao, Jing-ying; Li, Hong; Liang, Gui-yun; Mo, Zhao-yu

    2016-02-15

    Single Particle Aerosol Mass Spectrometry (SPAMS) was performed to characterize the PM2.5 in Nanning from 15 to 24 February 2015. The correlation (R2) between the PM2.5 number concentration and the mass concentration of PM2.5 obtained using SPAMS was 0.76. The particle number concentration could reflect the atmospheric pollution situation to some degree. The Art-2a classification method was used to classify the chemical composition of PM2.5. The results showed that the principal chemical constituents were elemental carbon, organic elements carbon hybrid particles, organic carbon, rich potassium particles, mineral substance, rich sodium particles, second inorganic particles, levoglucosan and other heavy metals. Among them, the composition of elemental carbon was the highest, followed by organic carbon and rich potassium particles. The particle size of 80% of PM2.5 was mainly concentrated in the range of 0.2 microm to 1.0 microm with a peak value occurring at 0. 62 microm. The particle size distribution characteristics of different chemical components were similar. The number concentration of the chemical components in PM2.5 had the same variation tread with the mass concentration of PM2.5 over time. To a certain extent, the change in chemical composition could reflect the instantaneous pollution source.

  4. [Chemical Composition of the Single Particle Aerosol in Winter in Nanning Using SPAMS].

    PubMed

    Liu, Hui-lin; Song, Hong-jun; Chen, Zhi-ming; Huang, Jiong-li; Yang, Jun-chao; Mao, Jing-ying; Li, Hong; Liang, Gui-yun; Mo,