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Sample records for aerosol processing study

  1. Overview of the Cumulus Humilis Aerosol Processing Study.

    SciTech Connect

    Berg, L. K.; Berkowitz, C. M.; Ogren, J. A.; Hostetler, C. A.; Ferrare, R. A.; Dubey, M.; Andrews, E.; Coulter, R. L.; Hair, J. W.; Hubbe, J. M.Lee, Y. N.; Mazzoleni, C; Olfert, J; Springston, SR; Environmental Science Division; PNNL; NOAA Earth System Research Lab.; NASA Langley Research Center; LANL; BNL; Univ.of Alberta; Univ. of Colorado

    2009-11-01

    Aerosols influence climate directly by scattering and absorbing radiation and indirectly through their influence on cloud microphysical and dynamical properties. The Intergovernmental Panel on Climate Change (IPCC) concluded that the global radiative forcing due to aerosols is large and in general cools the planet. But the uncertainties in these estimates are also large due to our poor understanding of many of the important processes related to aerosols and clouds. To address this uncertainty an integrated strategy for addressing issues related to aerosols and aerosol processes was proposed. Using this conceptual framework, the Cumulus Humilis Aerosol Processing Study (CHAPS) is a stage 1 activity, that is, a detailed process study. The specific focus of CHAPS was to provide concurrent observations of the chemical composition of the activated [particles that are currently serving as cloud condensation nuclei (CCN)] and nonactivated aerosols, the scattering and extinction profiles, and detailed aerosol and droplet size spectra in the vicinity of Oklahoma City, Oklahoma, during June 2007. Numerous campaigns have examined aerosol properties downwind from large pollution sources, including the Megacity Initiative: Local and Global Research Observations (MILAGRO) campaign and the two of the three Aerosol Characterization Experiments, ACE-2 and ACE-Asia. Other studies conducted near cities have examined changes in both aerosols and clouds downwind of urban areas. For example wintertime stratiform clouds associated with the urban plumes of Denver, Colorado, and Kansas City, Missouri, have a larger number concentration and smaller median volume diameter of droplets than clouds that had not been affected by the urban plume. Likewise, a decrease in precipitation in polluted regions along the Front Range of the Rocky Mountains was discovered. In a modeling study, it was found that precipitation downwind of urban areas may be influenced by changes in aerosols as well as the

  2. Puerto Rico - 2002 : field studies to resolve aerosol processes.

    SciTech Connect

    Gaffney, J. S.; Marley, N. A.; Ravelo, R.

    1999-10-05

    A number of questions remain concerning homogeneous aerosol formation by natural organics interacting with anthropogenic pollutants. For example, chlorine has been proposed as a potential oxidant in the troposphere because of its very high reactivity with a wide range of organics (Finlayson-Pitts, 1993). Indeed, sea salt aerosol in the presence of ozone has been shown to produce chlorine atoms in heterogeneous photochemical reactions under laboratory conditions. Whether chlorine can initiate oxidation of natural organics such as monoterpene hydrocarbons and can generate homogeneous nucleation or condensable material that contributes to aerosol loadings needs to be assessed. The nighttime reactions of ozone and nitrate radical can also result in monoterpene reactions that contribute to aerosol mass. We are currently planning field studies in Puerto Rico to assess these aerosol issues and other atmospheric chemistry questions. Puerto Rico has a number of key features that make it very attractive for a field study of this sort. The principal feature is the island's very regular meteorology and its position in the Caribbean Sea relative to the easterly trade winds. This meteorology and the island's rectangular shape (100 x 35 miles) make it highly suitable for simplification of boundary layer conditions. In addition, the long stretch between Puerto Rico and the nearest pollution sources in Africa and southern Europe make the incoming background air relatively clean and constant. Furthermore, Puerto Rico has approximately 3.5 million people with a very well defined source region and a central area of rain forest vegetation. These features make Puerto Rico an ideal locale for assessing aerosol processes. The following sections describe specific areas of atmospheric chemistry that can be explored during the proposed field study.

  3. RACORO aerosol data processing

    SciTech Connect

    Elisabeth Andrews

    2011-10-31

    The RACORO aerosol data (cloud condensation nuclei (CCN), condensation nuclei (CN) and aerosol size distributions) need further processing to be useful for model evaluation (e.g., GCM droplet nucleation parameterizations) and other investigations. These tasks include: (1) Identification and flagging of 'splash' contaminated Twin Otter aerosol data. (2) Calculation of actual supersaturation (SS) values in the two CCN columns flown on the Twin Otter. (3) Interpolation of CCN spectra from SGP and Twin Otter to 0.2% SS. (4) Process data for spatial variability studies. (5) Provide calculated light scattering from measured aerosol size distributions. Below we first briefly describe the measurements and then describe the results of several data processing tasks that which have been completed, paving the way for the scientific analyses for which the campaign was designed. The end result of this research will be several aerosol data sets which can be used to achieve some of the goals of the RACORO mission including the enhanced understanding of cloud-aerosol interactions and improved cloud simulations in climate models.

  4. Satellite observations and EMAC model calculations of sulfate aerosols from Kilauea: a study of aerosol formation, processing, and loss

    NASA Astrophysics Data System (ADS)

    Penning de Vries, Marloes; Beirle, Steffen; Brühl, Christoph; Dörner, Steffen; Pozzer, Andrea; Wagner, Thomas

    2016-04-01

    The currently most active volcano on Earth is Mount Kilauea on Hawaii, as it has been in a state of continuous eruption since 1983. The opening of a new vent in March 2008 caused half a year of strongly increased SO2 emissions, which in turn led to the formation of a sulfate plume with an extent of at least two thousand kilometers. The plume could be clearly identified from satellite measurements from March to November, 2008. The steady trade winds in the region and the lack of interfering sources allowed us to determine the life time of SO2 from Kilauea using only satellite-based measurements (no a priori or model information). The current investigation focuses on sulfate aerosols: their formation, processing and subsequent loss. Using space-based aerosol measurements by MODIS, we study the evolution of aerosol optical depth, which first increases as a function of distance from the volcano due to aerosol formation from SO2 oxidation, and subsequently decreases as aerosols are deposited to the surface. The outcome is compared to results from calculations using the EMAC (ECHAM/MESSy Atmospheric Chemistry) model to test the state of understanding of the sulfate aerosol life cycle. For this comparison, a particular focus is on the role of clouds and wet removal processes.

  5. Aerosol-stratocumulus Interactions over the Southeast Pacific: A Process Study Using WRF-Chem

    NASA Astrophysics Data System (ADS)

    Qiu, Y.; Chen, G.; Wang, W. C.; Liao, H.; Chen, J. P.; Xue, H.

    2015-12-01

    The recent WRF study by Chen et al. (2015) showed that the shortwave radiative forcing by the stratocumulus over the southeast Pacific (SEP) is much enhanced by anthropogenic aerosols from South America. Here we further investigate the aerosol-stratocumulus interactions on the process level using the WRF-Chem model which explicitly simulates the aerosol emissions and formations. Two cloud microphysics schemes are used: the widely-applied Lin scheme and the physics-based two-moment scheme used in Chen et al. (2015). The simulations with the Lin scheme captured some observed features of aerosols (e.g., aerosol mass and optical depth decreases westward along 20°S) and key aerosol-cloud microphysics interactions (e.g., more cloud droplet numbers near the coast). However, biases were also noticed, such as the overestimation of cloud droplet number near the coast, and the underestimation of aerosol concentration over the remote ocean. These could be caused by the inadequacy in cloud process parameterization, such as a lack of aerosol recycling from rain droplets in coupling with chemistry and microphysical modules (Saide et al, 2012). The two-moment scheme that explicitly addresses these processes is expected to minimize the biases. Detailed investigations of the cloud microphysics processes using the two schemes, and, to the extent possible, comparisons with observations will be presented and discussed. Chen, G.-X., W.-C. Wang, and J.-P. Chen, 2015: Aerosol-stratocumulus-radiation interactions over Southeast Pacific. J. Atmos. Sci., 72, 2612-2621. Saide, P. E. (and 16 co-authors), 2012: Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx, Atmos. Chem. Phys., 12, 3045-3064.

  6. A Study of Cloud Processing of Organic Aerosols Using Models and CHAPS Data

    SciTech Connect

    Ervens, Barbara

    2012-01-17

    The main theme of our work has been the identification of parameters that mostly affect the formation and modification of aerosol particles and their interaction with water vapor. Our detailed process model studies led to simplifications/parameterizations of these effects that bridge detailed aerosol information from laboratory and field studies and the need for computationally efficient expressions in complex atmospheric models. One focus of our studies has been organic aerosol mass that is formed in the atmosphere by physical and/or chemical processes (secondary organic aerosol, SOA) and represents a large fraction of atmospheric particulate matter. Most current models only describe SOA formation by condensation of low volatility (or semivolatile) gas phase products and neglect processes in the aqueous phase of particles or cloud droplets that differently affect aerosol size and vertical distribution and chemical composition (hygroscopicity). We developed and applied models of aqueous phase SOA formation in cloud droplets and aerosol particles (aqSOA). Placing our model results into the context of laboratory, model and field studies suggests a potentially significant contribution of aqSOA to the global organic mass loading. The second focus of our work has been the analysis of ambient data of particles that might act as cloud condensation nuclei (CCN) at different locations and emission scenarios. Our model studies showed that the description of particle chemical composition and mixing state can often be greatly simplified, in particular in aged aerosol. While over the past years many CCN studies have been successful performed by using such simplified composition/mixing state assumptions, much more uncertainty exists in aerosol-cloud interactions in cold clouds (ice or mixed-phase). Therefore we extended our parcel model that describes warm cloud formation by ice microphysics and explored microphysical parameters that determine the phase state and lifetime of

  7. A case study of aerosol processing and evolution in summer in New York City

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Chen, W. N.; Bae, M. S.; Lin, Y. C.; Hung, H. M.; Demerjian, K. L.

    2011-09-01

    We have investigated an aerosol processing and evolution event from 21-22 July during the summer 2009 Field Intensive Study at Queens College in New York City (NYC). The evolution processes are characterized by three consecutive stages: (1) aerosol wet scavenging, (2) nighttime nitrate formation, and (3) photochemical production and evolution of secondary aerosol species. Our results suggest that wet scavenging of aerosol species tends to be strongly related to their hygroscopicities and also mixing states. The scavenging leads to a significant change in bulk aerosol composition and average carbon oxidation state because of scavenging efficiencies in the following order: sulfate > low-volatility oxygenated organic aerosol (LV-OOA) > semi-volatile OOA (SV-OOA) > hydrocarbon-like OA (HOA). The second stage involves a quick formation of nitrate from heterogeneous reactions at nighttime. During the third stage, simultaneous increases of sulfate and SV-OOA were observed shortly after sunrise, indicating secondary aerosol formation. Organic aerosol particles become highly oxidized in ~half day as the result of photochemical processing, consistent with previously reported results from the CO-tracer method (OA/ΔCO). The photochemical reactions appear to progress gradually associated with a transformation of semi-volatile OOA to low-volatility species based on the evolution trends of oxygen-to-carbon (O/C) ratio, relationship between f44 (fraction of m/z 44 in OA) and f43 (fraction of m/z 43 in OA), and size evolution of OOA and HOA. Aerosols appear to become more internally mixed during the processing. Our results suggest that functionalization by incorporation of both C and O plays a major role in the early period of OA oxidation (O/C <0.5). Our results also show that photochemical production of LV-OOA during this event is approximately a few hours behind of sulfate production, which might explain the sometimes lack of correlations between LV-OOA and sulfate, two

  8. A case study of aerosol processing and evolution in summer in New York City

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Chen, W. N.; Bae, M. S.; Lin, Y. C.; Hung, H. M.; Demerjian, K. L.

    2011-12-01

    We have investigated an aerosol processing and evolution event from 21-22 July during the summer 2009 Field Intensive Study at Queens College in New York City (NYC). The evolution processes are characterized by three consecutive stages: (1) aerosol wet scavenging, (2) nighttime nitrate formation, and (3) photochemical production and evolution of secondary aerosol species. Our results suggest that wet scavenging of aerosol species tends to be strongly related to their hygroscopicities and also mixing states. The scavenging leads to a significant change in bulk aerosol composition and average carbon oxidation state because of scavenging efficiencies in the following order: sulfate > low-volatility oxygenated organic aerosol (LV-OOA) > semi-volatile OOA (SV-OOA) > hydrocarbon-like OA (HOA). The second stage involves a quick formation of nitrate from heterogeneous reactions at nighttime. During the third stage, simultaneous increases of sulfate and SV-OOA were observed shortly after sunrise, indicating secondary aerosol formation. Organic aerosols become highly oxidized in ~ half day as the result of photochemical processing, consistent with previously reported results from the CO-tracer method (OA/ΔCO). The photochemical reactions appear to progress gradually associated with a transformation of SV- OOA to low-volatility species based on the evolution trends of oxygen-to-carbon (O/C) ratio, relationship between f44 (fraction of m/z 44 in OA) and f43 (fraction of m/z 43 in OA), and size evolution of OOA and HOA. Aerosols appear to become more internally mixed during the processing. Our results suggest that functionalization by incorporation of both C and O plays a major role in the early period of OA oxidation (O/C < 0.5). Our results also show that photochemical production of LV-OOA during this event is approximately 2-3 h behind of sulfate production, which might explain, sometimes, the lack of correlations between LV-OOA and sulfate, two secondary aerosol species

  9. Laboratory Studies of Processing of Carbonaceous Aerosols by Atmospheric Oxidants/Hygroscopicity and CCN Activity of Secondary & Processed Primary Organic Aerosols

    SciTech Connect

    Ziemann, P.J.; Arey, J.; Atkinson, R.; Kreidenweis, S.M.; Petters, M.D.

    2012-06-13

    The atmosphere is composed of a complex mixture of gases and suspended microscopic aerosol particles. The ability of these particles to take up water (hygroscopicity) and to act as nuclei for cloud droplet formation significantly impacts aerosol light scattering and absorption, and cloud formation, thereby influencing air quality, visibility, and climate in important ways. A substantial, yet poorly characterized component of the atmospheric aerosol is organic matter. Its major sources are direct emissions from combustion processes, which are referred to as primary organic aerosol (POA), or in situ processes in which volatile organic compounds (VOCs) are oxidized in the atmosphere to low volatility reaction products that subsequent condense to form particles that are referred to as secondary organic aerosol (SOA). POA and VOCs are emitted to the atmosphere from both anthropogenic and natural (biogenic) sources. The overall goal of this experimental research project was to conduct laboratory studies under simulated atmospheric conditions to investigate the effects of the chemical composition of organic aerosol particles on their hygroscopicity and cloud condensation nucleation (CCN) activity, in order to develop quantitative relationships that could be used to more accurately incorporate aerosol-cloud interactions into regional and global atmospheric models. More specifically, the project aimed to determine the products, mechanisms, and rates of chemical reactions involved in the processing of organic aerosol particles by atmospheric oxidants and to investigate the relationships between the chemical composition of organic particles (as represented by molecule sizes and the specific functional groups that are present) and the hygroscopicity and CCN activity of oxidized POA and SOA formed from the oxidation of the major classes of anthropogenic and biogenic VOCs that are emitted to the atmosphere, as well as model hydrocarbons. The general approach for this project was

  10. Technology Solutions Case Study: Apartment Compartmentalization with an Aerosol-Based Sealing Process

    SciTech Connect

    2015-07-01

    Air sealing of building enclosures is a difficult and time-consuming process. Current methods in new construction require laborers to physically locate small and sometimes large holes in multiple assemblies and then manually seal each of them. This research study by Building America team Consortium for Advanced Residential Buildings demonstrated the automated air sealing and compartmentalization of buildings through the use of an aerosolized sealant developed by the Western Cooling Efficiency Center at University of California Davis. CARB demonstrated this new technology application in a multifamily building in Queens, NY. The effectiveness of the sealing process was evaluated by three methods: air leakage testing of overall apartment before and after sealing, point-source testing of individual leaks, and pressure measurements in the walls of the target apartment during sealing. Aerosolized sealing was successful by several measures in this study. Many individual leaks that are labor-intensive to address separately were well sealed by the aerosol particles. In addition, many diffuse leaks that are difficult to identify and treat were also sealed. The aerosol-based sealing process resulted in an average reduction of 71% in air leakage across three apartments and an average apartment airtightness of 0.08 CFM50/SF of enclosure area.

  11. Project Overview: Cumulus Humilis Aerosol Processing Study (CHAPS): Proposed Summer 2007 ASP Field Campaign

    SciTech Connect

    Berkowitz, Carl M.; Berg, Larry K.; Ogren, J. A.; Hostetler, Chris A.; Ferrare, Richard

    2006-05-18

    This white paper presents the scientific motivation and preliminary logistical plans for a proposed ASP field campaign to be carried out in the summer of 2007. The primary objective of this campaign is to use the DOE Gulfstream-1 aircraft to make measurements characterizing the chemical, physical and optical properties of aerosols below, within and above large fields of fair weather cumulus and to use the NASA Langley Research Center’s High Spectral Resolution Lidar (HSRL) to make independent measurements of aerosol backscatter and extinction profiles in the vicinity of these fields. Separate from the science questions to be addressed by these observations will be information to add in the development of a parameterized cumulus scheme capable of including multiple cloud fields within a regional or global scale model. We will also be able to compare and contrast the cloud and aerosol properties within and outside the Oklahoma City plume to study aerosol processes within individual clouds. Preliminary discussions with the Cloud and Land Surface Interaction Campaign (CLASIC) science team have identified overlap between the science questions posed for the CLASIC Intensive Operation Period (IOP) and the proposed ASP campaign, suggesting collaboration would benefit both teams.

  12. Solubilisation of aerosol trace metals by cloud processing: A laboratory study

    SciTech Connect

    Spokes, L.J.; Jickells, T.D.; Lim, B. )

    1994-08-01

    The atmosphere has now been recognized as a major source of both trace metals and nutrients to the oceans, with wet deposition being a major contributor to the flux. Solution pH has been suggested to be the major control on metal solubility in rainwater, but for many trace metals this relationship is not a simple one. Aerosols are typically exposed to [approximately]10 condensation/evaporation cloud cycles before removal in rain and, as a result of H[sub 2]SO[sub 4] and HNO[sub 3] uptake and SO[sub 2] oxidation, cloudwater pH can be very low. Laboratory studies have been conducted, using Saharan and Urban aerosols, to assess the effect of pH on trace metal solubility. The results for the crustal elements Al and Fe in the Saharan aerosol show that metal solubility is a strong function of pH with highest solubilities seen under low pH conditions, comparable to those found in clouds. Increasing the pH to simulate neutralization of acidity by ammonia and crustal material results in almost complete removal of these elements from the solution phase, suggesting that a simple relationship between pH and solubility should exist in rainwater. For Al and Fe in the Urban aerosol there is evidence that some of the material solubilized at low pH is kept in solution at high pH, perhaps as the result of complexation by organic matter. Manganese shows high solubility after the initial acidification from both the Saharan and Urban materials with only slight removal from solution at increased pH. For this element it appears, therefore, that the pH-dependent dissolution process is not reversible. It is tentatively suggested that Fe in the Urban aerosol, under these experimental conditions, is under solubility control.

  13. A new modeling system for studying aerosol - cloud -radiation interaction processes

    NASA Astrophysics Data System (ADS)

    Solomos, S.; Kallos, G.; Kuhsta, J.; Tremback, C.

    2008-12-01

    Links and feedbacks between air pollution and climate are complicated and are not accurately described in existing atmospheric models. In an attempt to better understand such links and feedbacks the new Integrated Community Limited Area Modeling System - ICLAMS has been developed. ICLAMS is an enhanced version of RAMS.6 modeling system. It includes submodels for the dust and sea salt cycles, gas and aqueous phase chemistry, gas to particle conversion and heterogeneous chemistry processes. All these processes are directly coupled with meteorology. RAMS has an explicit cloud microphysical scheme with eight categories of hydrometeors. The photochemical processes are directly linked to the RAMS radiative transfer scheme. The system is capable to be configured on two-way interactive nesting with any number of nested grids with resolution ranging from tens of kilometers to a few tens of meters. The system has been developed to study air pollution transport and transformation processes in the Greater Euro-Mediterranean Region and East Atlantic. This area is well known for its regional characteristics where the mixture of different age of anthropogenic air pollutants with Saharan dust and sea salt may lead to the formation of other particles with different characteristics. The mixture of the aerosols and gases from anthropogenic and natural origin (desert dust and sea salt) results in the formation of new types of PM with different physico-chemical properties and especially hygroscopicity (e.g. inside clouds or within the marine boundary layer) through heterogeneous processes. In this presentation, we demonstrate the transport and transformation processes at various spatiotemporal scales and discuss implications related to aerosol composition and their impacts on clouds and radiation (CCN and IN formation). We discuss the composition of the aerosols in the atmosphere along the long paths from Europe to North Africa and Atlantic. The composition changes and therefore the

  14. Collaborative research. Study of aerosol sources and processing at the GVAX Pantnagar Supersite

    SciTech Connect

    Worsnop, Doug; Volkamer, Rainer

    2012-08-13

    The Two Column Aerosol Project (TCAP) investigated uncertainties in the aerosol direct effect in the northern hemisphere mid-latitudes. The University of Colorado 2D-MAX-DOAS and LED-CE-DOAS instruments were collocated with DOE’s Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) and Mobile Aerosol Observing System (MAOS) during the TCAP-1 campaign at Cape Cod, MA (1 July to 13 August 2012). We have performed atmospheric radiation closure studies to evaluate the use of a novel parameter, i.e., the Raman Scattering Probability (RSP). We have performed first measurements of RSP almucantar scans, and measure RSP in spectra of scattered solar photons at 350nm and 430nm. Radiative Transfer Modelling of RSP demonstrate that the RSP measurement is maximally sensitive to infer even extremely low aerosol optical depth (AOD < 0.01) reliably by DOAS at low solar relative azimuth angles. We further assess the role of elevated aerosol layers on near surface observations of oxygen collision complexes, O 2-O2. Elevated aerosol layers modify the near surface absorption of O2-O2 and RSP. The combination of RSP and O2-O2 holds largely unexplored potential to better constrain elevated aerosol layers and measure column aerosol optical properties such as aerosol effective radius, extinction, aerosol phase functions and refractive indices. The TCAP deployment also provides a time series of reactive trace gas vertical profiles, i.e., nitrogen dioxide (NO2) and glyoxal (C2H2O2), which are measured simultaneously with the aerosol optical properties by DOAS. NO2 is an important precursor for ozone (O3) that modifies oxidative capacity. Glyoxal modifies oxidative capacity and is a source for brown carbon by forming secondary organic aerosol (SOA) via multiphase reactions in aerosol and cloud water. We have performed field measurements of these gases

  15. Properties of aerosol processed by ice clouds

    NASA Astrophysics Data System (ADS)

    Rudich, Y.; Adler, G.; Moise, T.; Erlick-Haspel, C.

    2012-12-01

    We suggest that highly porous aerosol (HPA) can form in the upper troposphere/lower stratosphere when ice particles encounter sub-saturation leading to ice sublimation similar to freeze drying. This process can occur at the lower layers of cirrus clouds (few km), at anvils of high convective clouds and thunderstorms, in clouds forming in atmospheric gravitational waves, in contrails and in high convective clouds injecting to the stratosphere. A new experimental system that simulates freeze drying of proxies for atmospheric aerosol at atmospheric pressure was constructed and various proxies for atmospheric soluble aerosol were studied. The properties of resulting HPA were characterized by various methods. It was found that the resulting aerosol have larger sizes (extent depends on substance and mixing), lower density (largevoid fraction), lower optical extinction and higher CCN activity and IN activity. Implication of HPA's unique properties and their atmospheric consequences to aerosol processing in ice clouds and to cloud cycles will be discussed.

  16. Aerosol typing - key information from aerosol studies

    NASA Astrophysics Data System (ADS)

    Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  17. A pathway analysis of global aerosol processes

    NASA Astrophysics Data System (ADS)

    Schutgens, Nick; Stier, Philip

    2014-05-01

    Although budgets for aerosol emission and deposition (macrophysical fluxes) have been studied before, much less is known about the budgets of processes e.g. nucleation, coagulation and condensation. A better understanding of their relative importance would improve our understanding of the aerosol system and help model development and evaluation. Aerosols are not only emitted from and deposited to the Earth's surface but are modified during their transport. The processes for these modifications include nucleation of H2SO4 gas into new aerosol, coagulation with other aerosol and condensation of H2SO4 unto existing aerosol. As a result of these processes, aerosol grow in size and change their chemical composition, often becoming hydrophilic where they were hydrophobic before. This affects their characteristics for various deposition processes (sedimentation, dry or wet deposition) as well as their radiative properties and hence climate forcing by aerosol. We present a complete budget of all aerosol processes in the aerosol-climate model ECHAM-HAM including the M7 microphysics. This model treats aerosol as 7 distinct but interacting two-moment modes of mixed species (soot, organic carbons, sulfate, sea salt and dust). We will show both global budgets as well as regional variations in dominant processes. Some of our conclusions are: condensation of H2SO4 gas onto pre-existing particles is an important process, dominating the growth of small particles in the nucleation mode to the Aitken mode and the ageing of hydrophobic matter. Together with in-cloud production of H2SO4, it significantly contributes to (and often dominates) the mass burden (and hence composition) of the hydrophilic Aitken and accumulation mode particles. Particle growth itself is the leading source of number densities in the hydrophilic Aitken and accumulation modes, with their hydrophobic counterparts contributing (even locally) relatively little. However, the coarse mode is mostly decoupled from the

  18. Impact of Aerosol Processing on Orographic Clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, Sara; Zubler, Elias M.; Lohmann, Ulrike

    2010-05-01

    Aerosol particles undergo significant modifications during their residence time in the atmosphere. Physical processes like coagulation, coating and water uptake, and aqueous surface chemistry alter the aerosol size distribution and composition. At this, clouds play a primary role as physical and chemical processing inside cloud droplets contributes considerably to the changes in aerosol particles. A previous study estimates that on global average atmospheric particles are cycled three times through a cloud before being removed from the atmosphere [1]. An explicit and detailed treatment of cloud-borne particles has been implemented in the regional weather forecast and climate model COSMO-CLM. The employed model version includes a two-moment cloud microphysical scheme [2] that has been coupled to the aerosol microphysical scheme M7 [3] as described by Muhlbauer and Lohmann, 2008 [4]. So far, the formation, transfer and removal of cloud-borne aerosol number and mass were not considered in the model. Following the parameterization for cloud-borne particles developed by Hoose et al., 2008 [5], distinction between in-droplet and in-crystal particles is made to more physically account for processes in mixed-phase clouds, such as the Wegener-Bergeron-Findeisen process and contact and immersion freezing. In our model, this approach has been extended to allow for aerosol particles in five different hydrometeors: cloud droplets, rain drops, ice crystals, snow flakes and graupel. We account for nucleation scavenging, freezing and melting processes, autoconversion, accretion, aggregation, riming and selfcollection, collisions between interstitial aerosol particles and hydrometeors, ice multiplication, sedimentation, evaporation and sublimation. The new scheme allows an evaluation of the cloud cycling of aerosol particles by tracking the particles even when scavenged into hydrometeors. Global simulations of aerosol processing in clouds have recently been conducted by Hoose et al

  19. Modeling aerosol processes at the local scale

    SciTech Connect

    Lazaridis, M.; Isukapalli, S.S.; Georgopoulos, P.G.

    1998-12-31

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

  20. A global model study of processes controlling aerosol size distributions in the Arctic spring and summer

    NASA Astrophysics Data System (ADS)

    Korhonen, Hannele; Carslaw, Kenneth S.; Spracklen, Dominick V.; Ridley, David A.; StröM, Johan

    2008-04-01

    We use a global chemical transport model (CTM) with size-resolved aerosol microphysics to evaluate our understanding of the processes that control Arctic aerosol, focussing on the seasonal changes in the particle size distribution during the transition from Arctic haze in spring to cleaner conditions in summer. This period presents several challenges for a global model simulation because of changes in meteorology, which affect transport pathways and precipitation scavenging rates, changes in the ocean-atmosphere flux of trace gases and particulates associated with sea ice break-up and increased biological activity, and changes in photolysis and oxidation rates which can affect particle nucleation and growth rates. Observations show that these changes result in a transition from an accumulation mode-dominated aerosol in spring to one dominated by Aitken and nucleation mode particles in summer. We find that remote Arctic aerosol size distribution is very sensitive to the model treatment of wet removal. In order to simulate the high accumulation mode concentrations typical of winter and spring it was necessary to substantially reduce the scavenging of these particles during transport. The resulting increases in accumulation mode lead to improvement in the modeled Aitken mode particle concentrations (which fall, due to increased scavenging in the free troposphere) and produce aerosol optical depths in good agreement with observations. The summertime increase in nucleation and Aitken mode particles is consistent with changes in local aerosol nucleation rates driven mainly by increased photochemical production of sulphuric acid vapor and, to a lesser extent, by decreases in the condensation sink as Arctic haze decreases. Alternatively, to explain the observed summertime Aitken mode particle concentrations in terms of ultrafine sea spray particles requires a sea-air flux a factor 5-25greater than predicted by current wind speed and sea surface temperature dependent flux

  1. Modeling the feedback between aerosol and boundary layer processes: a case study in Beijing, China.

    PubMed

    Miao, Yucong; Liu, Shuhua; Zheng, Yijia; Wang, Shu

    2016-02-01

    Rapid development has led to frequent haze in Beijing. With mountains and sea surrounding Beijing, the pollution is found to be influenced by the mountain-plain breeze and sea-land breeze in complex ways. Meanwhile, the presence of aerosols may affect the surface energy balance and impact these boundary layer (BL) processes. The effects of BL processes on aerosol pollution and the feedback between aerosol and BL processes are not yet clearly understood. Thus, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to investigate the possible effects and feedbacks during a haze episode on 23 September 2011. Influenced by the onshore prevailing wind, sea-breeze, and upslope breeze, about 45% of surface particulate matter (PM)2.5 in Beijing are found to be contributed by its neighbor cities through regional transport. In the afternoon, the development of upslope breeze suppresses the growth of BL in Beijing by imposing a relatively low thermal stable layer above the BL, which exacerbates the pollution. Two kinds of feedback during the daytime are revealed as follows: (1) as the aerosols absorb and scatter the solar radiation, the surface net radiation and sensible heat flux are decreased, while BL temperature is increased, resulting in a more stable and shallower BL, which leads to a higher surface PM2.5 concentration in the morning and (2) in the afternoon, as the presence of aerosols increases the BL temperature over plains, the upslope breeze is weakened, and the boundary layer height (BLH) over Beijing is heightened, resulting in the decrease of the surface PM2.5 concentration there. PMID:26490909

  2. Modeling the feedback between aerosol and boundary layer processes: a case study in Beijing, China.

    PubMed

    Miao, Yucong; Liu, Shuhua; Zheng, Yijia; Wang, Shu

    2016-02-01

    Rapid development has led to frequent haze in Beijing. With mountains and sea surrounding Beijing, the pollution is found to be influenced by the mountain-plain breeze and sea-land breeze in complex ways. Meanwhile, the presence of aerosols may affect the surface energy balance and impact these boundary layer (BL) processes. The effects of BL processes on aerosol pollution and the feedback between aerosol and BL processes are not yet clearly understood. Thus, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to investigate the possible effects and feedbacks during a haze episode on 23 September 2011. Influenced by the onshore prevailing wind, sea-breeze, and upslope breeze, about 45% of surface particulate matter (PM)2.5 in Beijing are found to be contributed by its neighbor cities through regional transport. In the afternoon, the development of upslope breeze suppresses the growth of BL in Beijing by imposing a relatively low thermal stable layer above the BL, which exacerbates the pollution. Two kinds of feedback during the daytime are revealed as follows: (1) as the aerosols absorb and scatter the solar radiation, the surface net radiation and sensible heat flux are decreased, while BL temperature is increased, resulting in a more stable and shallower BL, which leads to a higher surface PM2.5 concentration in the morning and (2) in the afternoon, as the presence of aerosols increases the BL temperature over plains, the upslope breeze is weakened, and the boundary layer height (BLH) over Beijing is heightened, resulting in the decrease of the surface PM2.5 concentration there.

  3. Study of Heterogeneouse Processes Related to the Chemistry of Tropospheric Oxidants and Aerosols

    SciTech Connect

    Davidovits, Paul; Worsnop, D R; Jayne, J T; Colb, C E

    2013-02-13

    The objective of the studies was to elucidate the heterogeneous chemistry of tropospheric aerosols. Experiments were designed to measure both specifically needed parameters, and to obtain systematic data required to build a fundamental understanding of the nature of gas-surface physical and chemical interactions

  4. A pathway analysis of global aerosol processes

    NASA Astrophysics Data System (ADS)

    Schutgens, N. A. J.; Stier, P.

    2014-06-01

    We present a detailed budget of the changes in atmospheric aerosol mass and numbers due to various processes: emission, nucleation, coagulation, H2SO4 condensation and in-cloud production, ageing and deposition. The budget is created from monthly-averaged tracer tendencies calculated by the global aerosol model ECHAM5.5-HAM2 and allows us to investigate process contributions at various length- and time-scales. As a result, we show in unprecedented detail what processes drive the evolution of aerosol. In particular, we show that the processes that affect aerosol masses are quite different from those affecting aerosol numbers. Condensation of H2SO4 gas onto pre-existing particles is an important process, dominating the growth of small particles in the nucleation mode to the Aitken mode and the ageing of hydrophobic matter. Together with in-cloud production of H2SO4, it significantly contributes to (and often dominates) the mass burden (and hence composition) of the hydrophilic Aitken and accumulation mode particles. Particle growth itself is the leading source of number densities in the hydrophilic Aitken and accumulation modes, with their hydrophobic counterparts contributing (even locally) relatively little. As expected, the coarse mode is dominated by primary emissions and mostly decoupled from the smaller modes. Our analysis also suggests that coagulation serves mainly as a loss process for number densities and that, relative to other processes, it is a rather unimportant contributor to composition changes of aerosol. The analysis is extended with sensitivity studies where the impact of a lower model resolution or pre-industrial emissions is shown to be small. We discuss the use of the current budget for model simplification, prioritisation of model improvements, identification of potential structural model errors and model evaluation against observations.

  5. A pathway analysis of global aerosol processes

    NASA Astrophysics Data System (ADS)

    Schutgens, N. A. J.; Stier, P.

    2014-11-01

    We present a detailed budget of the changes in atmospheric aerosol mass and numbers due to various processes: emission (including instant condensation of soluble biogenic emissions), nucleation, coagulation, H2SO4 condensation and in-cloud production, aging and deposition. The budget is created from monthly averaged tracer tendencies calculated by the global aerosol model ECHAM5.5-HAM2 and allows us to investigate process contributions at various length-scales and timescales. As a result, we show in unprecedented detail what processes drive the evolution of aerosol. In particular, we show that the processes that affect aerosol masses are quite different from those that affect aerosol numbers. Condensation of H2SO4 gas onto pre-existing particles is an important process, dominating the growth of small particles in the nucleation mode to the Aitken mode and the aging of hydrophobic matter. Together with in-cloud production of H2SO4, it significantly contributes to (and often dominates) the mass burden (and hence composition) of the hydrophilic Aitken and accumulation mode particles. Particle growth itself is the leading source of number densities in the hydrophilic Aitken and accumulation modes, with their hydrophobic counterparts contributing (even locally) relatively little. As expected, the coarse mode is dominated by primary emissions and mostly decoupled from the smaller modes. Our analysis also suggests that coagulation serves mainly as a loss process for number densities and that, relative to other processes, it is a rather unimportant contributor to composition changes of aerosol. The analysis is extended with sensitivity studies where the impact of a lower model resolution or pre-industrial emissions is shown to be small. We discuss the use of the current budget for model simplification, prioritization of model improvements, identification of potential structural model errors and model evaluation against observations.

  6. Developing a model system for studying the ozone processing of atmospheric aerosols by following changes in surface properties

    NASA Astrophysics Data System (ADS)

    Gonzalez-Labrada, Erick

    Atmospheric aerosols have a significant organic composition as determined by field measurement studies. This organic material is released to the atmosphere from both natural and anthropogenic sources, such as wind bursting of the ocean surface, car exhausts, and meat cooking, among others. An inverted micelle model has been proposed in order to explain the high concentration of organic compounds in aerosol particles. The model describes an organic film coating the air-liquid interface of an aqueous aerosol core. Chemical processing of this organic film by atmospheric oxidants (such as OH radicals, O3, and NO3) through heterogeneous and multiphase reactions can activate the aerosol to participate in atmospheric chemistry. After reaction, the particle has an increased role in the absorption and scattering of incoming solar radiation and cloud formation. Another consequence of this oxidation is the decrease of the atmospheric budget of gas-phase trace species, as well as the formation of volatile products. Several studies have proposed that the ozonolysis of organic films in aerosols takes place mainly at the surface. Therefore, the objective of this research was to develop a suitable model system for following the reaction through quantitative changes of a property inherent to the surface. Several attempts were made to examine the ozonolysis of organic monolayers at either solid or liquid surfaces. The studied monolayers contained unsaturated organic compounds as the only component or as part of a binary mixture with saturated compounds. The study of the ozone processing of monolayers deposited on solid substrates revealed information about changes in the hydrophobic character of the surface that occurred because of the reaction. On the other hand, the processing of a monolayer spread on a pendant drop allowed a real-time monitoring of surface pressure changes. This permitted a kinetic study of the reaction that yielded parameters related exclusively to processes

  7. Evaluating Aerosol Process Modules within the Framework of the Aerosol Modeling Testbed

    NASA Astrophysics Data System (ADS)

    Fast, J. D.; Velu, V.; Gustafson, W. I.; Chapman, E.; Easter, R. C.; Shrivastava, M.; Singh, B.

    2012-12-01

    Factors that influence predictions of aerosol direct and indirect forcing, such as aerosol mass, composition, size distribution, hygroscopicity, and optical properties, still contain large uncertainties in both regional and global models. New aerosol treatments are usually implemented into a 3-D atmospheric model and evaluated using a limited number of measurements from a specific case study. Under this modeling paradigm, the performance and computational efficiency of several treatments for a specific aerosol process cannot be adequately quantified because many other processes among various modeling studies (e.g. grid configuration, meteorology, emission rates) are different as well. The scientific community needs to know the advantages and disadvantages of specific aerosol treatments when the meteorology, chemistry, and other aerosol processes are identical in order to reduce the uncertainties associated with aerosols predictions. To address these issues, an Aerosol Modeling Testbed (AMT) has been developed that systematically and objectively evaluates new aerosol treatments for use in regional and global models. The AMT consists of the modular Weather Research and Forecasting (WRF) model, a series testbed cases for which extensive in situ and remote sensing measurements of meteorological, trace gas, and aerosol properties are available, and a suite of tools to evaluate the performance of meteorological, chemical, aerosol process modules. WRF contains various parameterizations of meteorological, chemical, and aerosol processes and includes interactive aerosol-cloud-radiation treatments similar to those employed by climate models. In addition, the physics suite from the Community Atmosphere Model version 5 (CAM5) have also been ported to WRF so that they can be tested at various spatial scales and compared directly with field campaign data and other parameterizations commonly used by the mesoscale modeling community. Data from several campaigns, including the 2006

  8. The Role of Aerosols on Precipitation Processes

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

    2006-01-01

    Cloud physics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distribution below the clouds. Therefore, the size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral--bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.

  9. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    NASA Astrophysics Data System (ADS)

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-01

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain-Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud-aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as -50% when cloud-aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is anticipated

  10. Tropospheric Ozone Lidar Network (TOLNet) - Long-term Tropospheric Ozone and Aerosol Profiling for Satellite Continuity and Process Studies

    NASA Astrophysics Data System (ADS)

    Newchurch, M.; Al-Saadi, J. A.; Alvarez, R. J.; Burris, J.; Cantrell, W.; Chen, G.; De Young, R.; Hardesty, R.; Hoff, R. M.; Kaye, J. A.; kuang, S.; Langford, A. O.; LeBlanc, T.; McDermid, I. S.; McGee, T. J.; Pierce, R.; Senff, C. J.; Sullivan, J. T.; Szykman, J.; Tonnesen, G.; Wang, L.

    2012-12-01

    An interagency research initiative for ground-based ozone and aerosol lidar profiling recently funded by NASA has important applications to air-quality studies in addition to the goal of serving the GEO-CAPE and other air-quality missions. Ozone is a key trace-gas species, a greenhouse gas, and an important pollutant in the troposphere. High spatial and temporal variability of ozone affected by various physical and photochemical processes motivates the high spatio-temporal lidar profiling of tropospheric ozone for improving the simulation and forecasting capability of the photochemical/air-quality models, especially in the boundary layer where the resolution and precision of satellite retrievals are fundamentally limited. It is well known that there are large discrepancies between the surface and upper-air ozone due to titration, surface deposition, diurnal processes, free-tropospheric transport, and other processes. Near-ground ozone profiling has been technically challenging for lidars due to some engineering difficulties, such as near-range saturation, field-of-view overlap, and signal processing issues. This initiative provides an opportunity for us to solve those engineering issues and redesign the lidars aimed at long-term, routine ozone/aerosol observations from the near surface to the top of the troposphere at multiple stations (i.e., NASA/GSFC, NASA/LaRC, NASA/JPL, NOAA/ESRL, UAHuntsville) for addressing the needs of NASA, NOAA, EPA and State/local AQ agencies. We will present the details of the science investigations, current status of the instrumentation development, data access/protocol, and the future goals of this lidar network. Ozone lidar/RAQMS comparison of laminar structures.

  11. COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

    SciTech Connect

    Worsnop, Douglas R.

    2014-07-28

    This project funded the participation of scientists from seven research groups, running more than thirty instruments, in the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London. The primary science questions for the ClearfLo Winter IOP were, 1) what is the urban increment of particulate matter (PM) and other pollutants in the greater London area, and, 2) what is the contribution of solid fuel use for home heating to wintertime PM? An additional motivation for the Detling measurements was the question of whether coatings on black carbon particles enhance absorption. The following four key accomplishments have been identified so far: 1) Chemical, physical and optical characterization of PM from local and regional sources (Figures 2, 4, 5 and 6). 2) Measurement of urban increment in particulate matter and gases in London (Figure 3). 3) Measurement of optical properties and chemical composition of coatings on black carbon containing particles indicates absorption enhancement. 4) First deployment of chemical ionization instrument (MOVI-CI-TOFMS) to measure both particle-phase and gas-phase organic acids. (See final report from Joel Thornton, University of Washington, for details.) Analysis of the large dataset acquired in Detling is ongoing and will yield further key accomplishments. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal. The measurement of absorption enhancement by coatings on black carbon will contribute to improved modeling of the direct radiative properties of PM.

  12. Aerosol processing in stratiform clouds in ECHAM6-HAM

    NASA Astrophysics Data System (ADS)

    Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

    2013-04-01

    chemical components as well as 5 tracers for aerosol particles in ice crystals. This allows simulations of aerosol processing in warm, mixed-phase (e.g. through the Bergeron-Findeisen process) and ice clouds. The fixed scavenging ratios used for wet deposition in clouds in standard HAM are replaced by an explicit treatment of collision of cloud droplets/ice crystals with interstitial aerosol particles. Nucleation scavenging of aerosol particles by acting as cloud condensation nuclei or ice nuclei, freezing and evaporation of cloud droplets and melting and sublimation of ice crystals are treated explicitly. In extension to previous studies, aerosol particles from evaporating precipitation are released to modes which correspond to their size. Cloud processing of aerosol particles changes their size distribution and hence influences cloud droplet and ice crystal number concentrations as well as precipitation rate, which in turn affects aerosol concentrations. Results will be presented at the conference. Hoose et al., JGR, 2008a, doi: 10.1029/2007JD009251 Hoose et al., ACP, 2008b, doi: 10.5194/acp-8-6939-2008 Stevens et al., 2013, submitted Stier et al., ACP, 2005, doi: 10.5194/acp-5-1125-2005

  13. The Aerosol Modeling Testbed: A community tool to objectively evaluate aerosol process modules

    SciTech Connect

    Fast, Jerome D.; Gustafson, William I.; Chapman, Elaine G.; Easter, Richard C.; Rishel, Jeremy P.; Zaveri, Rahul A.; Grell, Georg; Barth, Mary

    2011-03-02

    This study describes a new modeling paradigm that significantly advances how the third activity is conducted while also fully exploiting data and findings from the first two activities. The Aerosol Modeling Testbed (AMT) is a computational framework for the atmospheric sciences community that streamlines the process of testing and evaluating aerosol process modules over a wide range of spatial and temporal scales. The AMT consists of a fully-coupled meteorology-chemistry-aerosol model, and a suite of tools to evaluate the performance of aerosol process modules via comparison with a wide range of field measurements. The philosophy of the AMT is to systematically and objectively evaluate aerosol process modules over local to regional spatial scales that are compatible with most field campaigns measurement strategies. The performance of new treatments can then be quantified and compared to existing treatments before they are incorporated into regional and global climate models. Since the AMT is a community tool, it also provides a means of enhancing collaboration and coordination among aerosol modelers.

  14. Building America Case Study: Apartment Compartmentalization with an Aerosol-Based Sealing Process - Queens, NY; Technology Solutions for New and Existing Homes, Energy Efficiency & Renewable Energy (EERE)

    SciTech Connect

    2015-07-01

    Air sealing of building enclosures is a difficult and time-consuming process. Current methods in new construction require laborers to physically locate small and sometimes large holes in multiple assemblies and then manually seal each of them. The innovation demonstrated under this research study was the automated air sealing and compartmentalization of buildings through the use of an aerosolized sealant, developed by the Western Cooling Efficiency Center at University of California Davis.
    CARB sought to demonstrate this new technology application in a multifamily building in Queens, NY. The effectiveness of the sealing process was evaluated by three methods: air leakage testing of overall apartment before and after sealing, point-source testing of individual leaks, and pressure measurements in the walls of the target apartment during sealing. Aerosolized sealing was successful by several measures in this study. Many individual leaks that are labor-intensive to address separately were well sealed by the aerosol particles. In addition, many diffuse leaks that are difficult to identify and treat were also sealed. The aerosol-based sealing process resulted in an average reduction of 71% in air leakage across three apartments and an average apartment airtightness of 0.08 CFM50/SF of enclosure area.

  15. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    DOE PAGES

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it

  16. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    SciTech Connect

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is

  17. Mexico City aerosol study

    SciTech Connect

    Falcon, Y.I. ); Ramirez, C.R. )

    1988-01-01

    Mexico City is located in a valley at high elevation (2,268 m) and is subject to atmospheric inversion related problems similar to those found in Denver, Colorado. In addition, Mexico City has a tropical climate (latitude 19{degrees} 25 minutes N), and therefore has more sunlight available for production of photochemical smog. There are approximately 9.5 million people spread in a 1,500 km{sup 2} (25 sq. mi) urban area, and more than two million automobiles (D.G.P.T. 1979) which use leaded gasoline. Furthermore, Mexico City is the principal industrial center in the country with more than 131,000 industries. The growth of the city has led to a serious air pollution problem, and there is concern over the possible pollutant effects on human health. The authors discuss work done to characterize the chemical composition of the aerosol. It is shown that many of the organic compounds which have been detected in urban aerosols are carcinogens.

  18. Aerosol backscatter studies supporting LAWS

    NASA Technical Reports Server (NTRS)

    Rothermel, Jeffry

    1989-01-01

    Optimized Royal Signals and Radar Establishment (RSRE), Laser True Airspeed System (LATAS) algorithm for low backscatter conditions was developed. The algorithm converts backscatter intensity measurements from focused continuous-wave (CW) airborne Doppler lidar into backscatter coefficients. The performance of optimized algorithm under marginal backscatter signal conditions was evaluated. The 10.6 micron CO2 aerosol backscatter climatologies were statistically analyzed. Climatologies reveal clean background aerosol mode near 10(exp -10)/kg/sq m/sr (mixing ratio units) through middle and upper troposhere, convective mode associated with planetary boundary layer convective activity, and stratospheric mode associated with volcanically-generated aerosols. Properties of clean background mode are critical to design and simulation studies of Laser Atmospheric Wind Sounder (LAWS), a MSFC facility Instrument on the Earth Observing System (Eos). Previous intercomparisons suggested correlation between aerosol backscatter at CO2 wavelength and water vapor. Field measurements of backscatter profiles with MSFC ground-based Doppler lidar system (GBDLS) were initiated in late FY-88 to coincide with independent program of local rawinsonde releases and overflights by Multi-spectral Atmospheric Mapping Sensor (MAMS), a multi-channel infrared radiometer capable of measuring horizontal and vertical moisture distributions. Design and performance simulation studies for LAWS would benefit from the existence of a relationship between backscatter and water vapor.

  19. Evolution of stratospheric sulfate aerosol from the 1991 Pinatubo eruption: Roles of aerosol microphysical processes

    NASA Astrophysics Data System (ADS)

    Sekiya, T.; Sudo, K.; Nagai, T.

    2016-03-01

    This study investigates the role of aerosol microphysics in stratospheric sulfate aerosol changes after the 1991 Mount Pinatubo eruption using an atmospheric general circulation model that is coupled interactively with a chemistry module and a modal aerosol microphysical module with three modes. Our model can reproduce the global mean stratospheric aerosol optical depth (SAOD) observed by the Stratospheric Aerosol and Gas Experiment (SAGE) II during June 1991 to January 1993. The model underestimates the observed SAOD before the eruption and after January 1993. The model also underestimates the integrated backscatter coefficient observed by ground-based lidar at Tsukuba, Naha, and Lauder. The modeled effective radius becomes larger (about 0.5 μm) and agrees with the balloon-borne measurements at Laramie, Wyoming (41°N, 105°W). We further investigate effects of the inclusion of evaporation along with the condensation processes and the inclusion of van der Waals and viscous forces in the coagulation processes. The inclusion of evaporation along with the condensation processes reduces the global mean effective radius by up to 0.04 μm and increases the global burden of stratospheric sulfate aerosols (about 15% in late 1993). The inclusion of van der Waals and viscous forces in the coagulation processes increases the global mean effective radius by up to 0.06-0.07 μm and decreases the global burden (15-30% in late 1993). The effects of van der Waals and viscous forces differ between two schemes. However, we do not conclude which simulation is superior because all simulations fall within error bars.

  20. Oxidation enhancement of submicron organic aerosols by fog processing

    NASA Astrophysics Data System (ADS)

    Zhang, Q.; Ge, X.; Collier, S.; Setyan, A.; Xu, J.; Sun, Y.

    2011-12-01

    During 2010 wintertime, a measurement study was carried out at Fresno, California, using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) combined with a Scanning Mobility Particle Sizer (SMPS). Four fog events occurred during the first week of the campaign. While ambient aerosol was sampled into the HR-ToF-AMS, fog water samples were collected, and were later aerosolized and analyzed via HR-TOF-AMS in the laboratory. We performed Positive Matrix Factorization (PMF) on the AMS ambient organic mass spectra, and identified four OA factors: hydrocarbon-like OA (HOA) likely from vehicle emissions, cooking influenced OA (COA), biomass burning OA (BBOA) representing residential wood combustion, and an oxygenated OA (OOA) that has an average O/C ratio of 0.42. The time series of the OOA factor correlates best with that of sulfate (R2 =0.54 ) during fog events, suggesting that aqueous phase processing may have strongly affected OOA production during wintertime in Fresno. We further investigate the OOA compositions and elemental ratios before, during, and after the fog events, as well as those of dissolved organic matter (DOM) in fog waters to study the influence of aqueous phase processing on OA compositions. Results of fog sample analysis shows an enhancement of oxidation of DOM in 11 separate fog samples. Further factor analysis of the fog DOM data will elucidate the possible mechanisms by which fog processing enhances oxidation of aerosol. In addition, in order to investigate the influence of aqueous processing on OA, we used the Extended Aerosol Inorganic Model (E-AIM) (http://www.aim.env.uea.ac.uk/aim/aim.php) to estimate aerosol phase water contents based on the AMS measured aerosol composition. The predicted water content has a good correlation with sulfate and OOA . We will further explore the correlations between particle phase water with organic aerosol characteristics to discuss the influence of aqueous phase processing on

  1. Design of Nanomaterial Synthesis by Aerosol Processes

    PubMed Central

    Buesser, Beat; Pratsinis, Sotiris E.

    2013-01-01

    Aerosol synthesis of materials is a vibrant field of particle technology and chemical reaction engineering. Examples include the manufacture of carbon blacks, fumed SiO2, pigmentary TiO2, ZnO vulcanizing catalysts, filamentary Ni, and optical fibers, materials that impact transportation, construction, pharmaceuticals, energy, and communications. Parallel to this, development of novel, scalable aerosol processes has enabled synthesis of new functional nanomaterials (e.g., catalysts, biomaterials, electroceramics) and devices (e.g., gas sensors). This review provides an access point for engineers to the multiscale design of aerosol reactors for the synthesis of nanomaterials using continuum, mesoscale, molecular dynamics, and quantum mechanics models spanning 10 and 15 orders of magnitude in length and time, respectively. Key design features are the rapid chemistry; the high particle concentrations but low volume fractions; the attainment of a self-preserving particle size distribution by coagulation; the ratio of the characteristic times of coagulation and sintering, which controls the extent of particle aggregation; and the narrowing of the aggregate primary particle size distribution by sintering. PMID:22468598

  2. Aerosol chemistry in Titan's ionosphere: simultaneous growth and etching processes

    NASA Astrophysics Data System (ADS)

    Carrasco, Nathalie; Cernogora, Guy; Jomard, François; Etcheberry, Arnaud; Vigneron, Jackie

    2016-10-01

    Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan's ionosphere [1]. This unexpected chemistry can be further investigated in the laboratory with plasma experiments simulating the complex ion-neutral chemistry starting from N2-CH4 [2]. Two sorts of solid organic samples can be produced in laboratory experiments simulating Titan's atmospheric reactivity: grains in the volume and thin films on the reactor walls. We expect that grains are more representative of Titan's atmospheric aerosols, but films are used to provide optical indices for radiative models of Titan's atmosphere.The aim of the present study is to address if these two sorts of analogues are chemically equivalent or not, when produced in the same N2-CH4 plasma discharge. The chemical compositions of both these materials are measured by using elemental analysis, XPS analysis and Secondary Ion Mass Spectrometry. We find that films are homogeneous but significantly less rich in nitrogen and hydrogen than grains produced in the same experimental conditions. This surprising difference in their chemical compositions is explained by the efficient etching occurring on the films, which stay in the discharge during the whole plasma duration, whereas the grains are ejected after a few minutes [3]. The impact for our understanding of Titan's aerosols chemical composition is important. Our study shows that chemical growth and etching process are simultaneously at stake in Titan's ionosphere. The more the aerosols stay in the ionosphere, the more graphitized they get through etching process. In order to infer Titan's aerosols composition, our work highlights a need for constraints on the residence time of aerosols in Titan's ionosphere. [1] Waite et al. (2009) Science , 316, p. 870[2] Szopa et al. (2006) PSS, 54, p. 394[3] Carrasco et al. (2016) PSS, 128, p. 52

  3. Natural Radionuclides and Isotopic Signatures for Determining Carbonaceous Aerosol Sources, Aerosol Lifetimes, and Washout Processes

    SciTech Connect

    Gaffney, Jeffrey

    2012-12-12

    This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

  4. AEROSOL PARTICLE COLLECTOR DESIGN STUDY

    SciTech Connect

    Lee, S; Richard Dimenna, R

    2007-09-27

    A computational evaluation of a particle collector design was performed to evaluate the behavior of aerosol particles in a fast flowing gas stream. The objective of the work was to improve the collection efficiency of the device while maintaining a minimum specified air throughput, nominal collector size, and minimal power requirements. The impact of a range of parameters was considered subject to constraints on gas flow rate, overall collector dimensions, and power limitations. Potential improvements were identified, some of which have already been implemented. Other more complex changes were identified and are described here for further consideration. In addition, fruitful areas for further study are proposed.

  5. New Photosensitized Processes at Aerosol and Ocean Surfaces

    NASA Astrophysics Data System (ADS)

    Rossignol, S.; Aregahegn, K. Z.; Ciuraru, R.; Bernard, F.; Tinel, L.; Fine, L.; George, C.

    2014-12-01

    From a few years now, there is a growing body of evidence that photoinduced processes could be of great importance for the tropospheric chemistry. Here, we would like to present two additional outcomes of this new area of research, firstly the photosensitized direct VOC uptake by aerosols and, secondly, the photoinduced chemical formation of unsaturated VOC from marine microlayer proxy. It was recently shown that the chemistry of glyoxal toward ammonium ions into droplets and wet aerosols leads to the formation of light-absorbing compounds. Among them, we found that imidazole-2-carboxaldehyde (IC) acts as a photosensitizer and is able to initiate the growth of organic aerosols via the uptake of VOC, such as limonene. Given its potential importance, the mechanism of this photoinduced uptake was investigated thanks to aerosol flow tube experiments and UPLC-ESI-HRMS analysis. Results reveal hydrogen abstraction on the VOC molecule by the triplet state of IC leading to the VOC oxidation without any traditional oxidant. As well as aerosol, the sea-surface microlayer, known to be enriched in light-absorbing organics, is largely impacted by photochemical processes. Recent studies have pointed out for example the role of photosentitized processes in the loss of NO2 and ozone at water surfaces containing photoactive compounds such as chlorophyll. In order to go further, we worked from sea-surface microlayer proxy containing humic acids as photoactive material and organic acids as surfactants. Beside oxidation processes, we monitored by high resolution PTR-MS the release in the gas phase of unsaturated compounds, including C5 dienes (isoprene ?). A strong correlation between the measured surface tension and the C5 diene concentration in the gas phase was evidenced, clearly pointing toward an interfacial process. This contribution will highlight the similarities between both systems and will attempt to present a general chemical scheme for photosensitized chemistry at

  6. Aqueous phase processing of secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Liu, Yao; Tritscher, T.; Praplan, A. P.; Decarlo, P. F.; Temime-Roussel, B.; Quivet, E.; Marchand, N.; Dommen, J.; Baltensperger, U.; Monod, A.

    2011-07-01

    The aging of secondary organic aerosol (SOA) by photooxidation in the aqueous phase was experimentally investigated. To simulate multiphase processes, the following experiments were sequentially performed in a smog chamber and in an aqueous phase photoreactor: (1) Gas-phase photooxidation of three different volatile organic compounds (VOC): isoprene, α-pinene, and 1,3,5-trimethylbenzene (TMB) in the presence of NOx, leading to the formation of SOA which was subjected to on-line physical and chemical analysis; (2) particle-to-liquid transfer of water soluble species of SOA using filter sampling and aqueous extraction; (3) aqueous-phase photooxidation of the obtained water extracts; and (4) nebulization of the solutions for a repetition of the on-line characterization. SOA concentrations in the chamber measured with a scanning mobility particle sizer (SMPS) were higher than 200 μg m-3, as the experiments were conducted under high initial concentrations of volatile organic compounds (VOC) and NOx. The aging of SOA through aqueous phase processing was investigated by measuring the physical and chemical properties of the particles online before and after processing using a high resolution time-of-flight aerosol mass spectrometer (AMS) and a hygroscopicity tandem differential mobility analyzer (H-TDMA). It was shown that, after aqueous phase processing, the particles were significantly more hygroscopic, and contained more fragmentation ions at m/z = 44 and less ions at m/z = 43, thus showing a significant impact on SOA aging for the three different precursors. Additionally, the particles were analyzed with a thermal desorption atmospheric pressure ionization aerosol mass spectrometer (TD-API-AMS). Comparing the smog chamber SOA composition and non processed nebulized aqueous extracts with this technique revealed that sampling, extraction and/or nebulization did not significantly impact the chemical composition of SOA formed from isoprene and α-pinene, whereas it

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

    NASA Technical Reports Server (NTRS)

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

    2016-01-01

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

  8. Predicted modification of the O/C ratio of SOA due to cloud and aerosol processing

    NASA Astrophysics Data System (ADS)

    Carlton, A. G.; Ervens, B.

    2011-12-01

    The formation of secondary organic aerosol formation in cloud and aerosol water (aqSOA) has attracted great attention over the past years and many laboratory data are available to describe such processes in detail. While it has been recognized that aqSOA formation might significantly contribute to the total SOA budget in humid and cloudy regions, the modification of individual aerosol properties, such as oxygenation state (O/C ratio), size (distribution), and light-absorbing properties has not been explored by means of model studies. Precursors of aqSOA are more highly oxidized and water-soluble than those for traditional (gas)SOA and thus aqSOA products have also distinctly higher O/C ratio. Since aqSOA occurs in clouds and in aerosol water at elevated RH, aerosols modified by such processes exhibit a unique vertical profile as compared to gasSOA and add to the organic carbon budget aloft. In this process model study, we will show the extent to which the O/C ratio of aerosols is modified due to aqSOA formation in cloud and aerosol water. The O/C ratio can be considered as a proxy for other aerosol properties such as hygroscopicity (particle growth and CCN activity) and interactions with light (scattering/absorption) which affect the direct and indirect aerosol effects on radiation. Implications of aqSOA formation on these aerosol properties as a function of vertical profile will be discussed.

  9. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    SciTech Connect

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-04-09

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m{sup 2} between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m{sup 2} depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  10. Evaluation of aerosol processes between roadside and neighbourhood scale

    NASA Astrophysics Data System (ADS)

    Karl, Matthias; Kukkonen, Jaakko; Pirjola, Liisa; Keuken, Menno P.

    2015-04-01

    Particle emissions from road transport include vehicle exhaust emissions, tire/brake wear and re-suspension of road dust. Vehicle exhaust emissions usually constitute the most significant source of ultrafine particles (UFP), i.e. particles with diameters <100 nm, in urban environments. Several toxicological studies have concluded that UFP are more toxic than larger particles with the same chemical composition and at the same mass concentration. Since UFP contribute negligibly to the mass concentration of PM10 and PM2.5, they should be described in terms of particle number (PN) concentration. However, only PM10 and PM2.5 are regulated by current air pollution legislation. UFP emitted from road traffic are subject to complex dilution and transformation processes in the urban environment. This model study evaluates the influence of aerosol processes on PN concentration on the spatial and temporal range between the roadside, typically represented by measurements at a traffic monitoring site, and the neighbourhood scale, extending from several hundred meters to several kilometres. Several dispersion scenarios for the cities Oslo, Helsinki and Rotterdam were simulated using the multicomponent aerosol dynamics process model MAFOR, approximating dilution by a power-law function. Aerosol processes considered in this study were condensation/evaporation of n-alkanes, coagulation and the dry deposition of particles. Under typical dispersion conditions dilution clearly dominated the change of total PN on the neighbourhood scale. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamical processes controlling the removal of particles from emitted from vehicular exhaust on urban time scales. The effect of condensation/evaporation of organic vapours emitted by vehicles on particle numbers and on particle size distributions was examined. A simplified parameterization for the implementation of coagulation and dry deposition of particles in

  11. Assessing the Performance of Computationally Simple and Complex Representations of Aerosol Processes using a Testbed Methodology

    NASA Astrophysics Data System (ADS)

    Fast, J. D.; Ma, P.; Easter, R. C.; Liu, X.; Zaveri, R. A.; Rasch, P.

    2012-12-01

    Predictions of aerosol radiative forcing in climate models still contain large uncertainties, resulting from a poor understanding of certain aerosol processes, the level of complexity of aerosol processes represented in models, and the ability of models to account for sub-grid scale variability of aerosols and processes affecting them. In addition, comparing the performance and computational efficiency of new aerosol process modules used in various studies is problematic because different studies often employ different grid configurations, meteorology, trace gas chemistry, and emissions that affect the temporal and spatial evolution of aerosols. To address this issue, we have developed an Aerosol Modeling Testbed (AMT) to systematically and objectively evaluate aerosol process modules. The AMT consists of the modular Weather Research and Forecasting (WRF) model, a series of testbed cases for which extensive in situ and remote sensing measurements of meteorological, trace gas, and aerosol properties are available, and a suite of tools to evaluate the performance of meteorological, chemical, aerosol process modules. WRF contains various parameterizations of meteorological, chemical, and aerosol processes and includes interactive aerosol-cloud-radiation treatments similar to those employed by climate models. In addition, the physics suite from a global climate model, Community Atmosphere Model version 5 (CAM5), has also been ported to WRF so that these parameterizations can be tested at various spatial scales and compared directly with field campaign data and other parameterizations commonly used by the mesoscale modeling community. In this study, we evaluate simple and complex treatments of the aerosol size distribution and secondary organic aerosols using the AMT and measurements collected during three field campaigns: the Megacities Initiative Local and Global Observations (MILAGRO) campaign conducted in the vicinity of Mexico City during March 2006, the

  12. Halogenation processes of secondary organic aerosol and implications on halogen release mechanisms

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Schmitt-Kopplin, P.; Platt, U.; Zetzsch, C.

    2012-01-01

    Reactive halogen species (RHS), such as X·, X2 and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA) and organic aerosol derived from biomass-burning (BBOA) has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols. Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS released from simulated natural halogen sources like salt pans. Subsequently the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which result in new functional groups, changed UV/VIS absorption, or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

  13. Studies of Ambient and Chamber Aerosol Composition using the Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Craven, Jill Suzanne

    This thesis presents composition measurements for atmospherically relevant inorganic and organic aerosol from laboratory and ambient measurements using the Aerodyne aerosol mass spectrometer. Studies include the oxidation of dodecane in the Caltech environmental chambers, and several aircraft- and ground-based field studies, which include the quantification of wildfire emissions off the coast of California, and Los Angeles urban emissions. The oxidation of dodecane by OH under low NO conditions and the formation of secondary organic aerosol (SOA) was explored using a gas-phase chemical model, gas-phase CIMS measurements, and high molecular weight ion traces from particlephase HR-TOF-AMS mass spectra. The combination of these measurements support the hypothesis that particle-phase chemistry leading to peroxyhemiacetal formation is important. Positive matrix factorization (PMF) was applied to the AMS mass spectra which revealed three factors representing a combination of gas-particle partitioning, chemical conversion in the aerosol, and wall deposition. Airborne measurements of biomass burning emissions from a chaparral fire on the central Californian coast were carried out in November 2009. Physical and chemical changes were reported for smoke ages 0--4 h old. CO 2 normalized ammonium, nitrate, and sulfate increased, whereas the normalized OA decreased sharply in the first 1.5--2 h, and then slowly increased for the remaining 2 h (net decrease in normalized OA). Comparison to wildfire samples from the Yucatan revealed that factors such as relative humidity, incident UV radiation, age of smoke, and concentration of emissions are important for wildfire evolution. Ground-based aerosol composition is reported for Pasadena, CA during the sumix mer of 2009. The OA component, which dominated the submicron aerosol mass, was deconvolved into hydrocarbon-like organic aerosol (HOA), semi-volatile oxidized organic aerosol (SVOOA), and low-volatility oxidized organic aerosol

  14. Secondary organic aerosol formation through cloud processing of aromatic VOCs

    NASA Astrophysics Data System (ADS)

    Herckes, P.; Hutchings, J. W.; Ervens, B.

    2010-12-01

    Field observations have shown substantial concentrations (20-5,500 ng L-1) of aromatic volatile organic compounds (VOC) in cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric laboratory conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction rates decreased with increasing organic carbon content. Kinetic data derived from these experiments were used as input to a multiphase box model in order to evaluate the secondary organic aerosol (SOA) mass formation potential of cloud processing of BTEX. Model results will be presented that quantify the SOA amounts from these aqueous phase pathways. The efficiency of this multiphase SOA source will be compared to SOA yields from the same aromatics as treated in traditional SOA models that are restricted to gas phase oxidation and subsequent condensation on particles.

  15. Field and Laboratory Studies of Atmospheric Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Coggon, Matthew Mitchell

    This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of

  16. Understanding the Processes Controlling Aerosol-Cloud Interactions in the Arctic Marine Boundary Layer

    NASA Astrophysics Data System (ADS)

    Browse, J.; Carslaw, K. S.; Pringle, K.; Mann, G.; Reddington, C.; Brooks, I. M.; Mulcahy, J.; Young, G.; Allan, J. D.; Liu, D.; Trembath, J.; Dean, A.; Yoshioka, M.

    2015-12-01

    Here we use multiple configurations of the UKCA chemistry and aerosol scheme in a global climate model, capable of simulating cloud condensation nuclei (CCN) and cloud droplet number, to understand the processes controlling aerosol-cloud interactions in the marine Arctic boundary layer. Evaluation against an unprecedented number of aerosol and cloud observations made available through the Global Aerosol Synthesis and Science Project (GASSP), International Arctic Systems for Observing the Atmosphere (IASOA) and the 2013 ACCACIA campaign, suggest that Arctic summertime CCN is well represented in the model. Sensitivity studies indicate that DMS derived nucleation events are the primary source of Arctic summertime aerosol increasing mean (median) surface CCN concentrations north of 70N from 21(14) cm-3 to 46(33) cm-3. However, evaluation against observed aerosol size distributions suggests that UKCA overestimates nucleation mode (~10nm) particle concentrations either due to overestimation of boundary layer nucleation rates or underestimation of the Arctic marine boundary layer condensation sink.

  17. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3− aerosol during the 2013 Southern Oxidant and Aerosol Study

    DOE PAGES

    Allen, H. M.; Draper, D. C.; Ayres, B. R.; Ault, A.; Bondy, A.; Takahama, S.; Modini, R. L.; Baumann, K.; Edgerton, E.; Knote, C.; et al

    2015-09-25

    Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3−) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3more » and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. In addition, calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3− is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3− and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.« less

  18. Photoacoustic study of airborne and model aerosols

    NASA Astrophysics Data System (ADS)

    Alebić-Juretić, A.; Zetzsch, C.; Dóka, O.; Bicanic, D.

    2003-01-01

    Airborne particulates of either natural or anthropogenic origin constitute a significant portion of atmospheric pollution. Environmental xenobiotics, among which are polynuclear aromatic hydrocarbons (PAHs) and pesticides, often adsorb to aerosols and as such are transported through the atmosphere with the physicochemical properties of the aerosols determining the lifetime of these organic compounds. As an example, the resistance of some PAHs against the photolysis is explained by the effect of the aerosol's "inner filter" that reduces the intensity of incident light reaching the mineral particles. On the other hand, some constituents of the aerosols can act as catalytic and/or stoichiometric reagents in atmospheric reactions on the solid surfaces. In the study described here the photoacoustic (PA) spectroscopy in the UV-Vis was used to investigate natural and model aerosols. The PA spectra obtained from coal and wood ashes and of Saharan sand, all three representatives of airborne aerosols, provide the evidence for the existence of the "inner filter." Furthermore, valuable information about the different nature of the interaction between the model aerosols and adsorbed organics (e.g., PAH-pyranthrene and silica, alumina, and MgO) has been obtained. Finally, the outcome of the study conducted with powdered mixtures of chalk and black carbon suggests that the PA method is a candidate method for determination of carbon content in stack ashes.

  19. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

    SciTech Connect

    Davidovits, Paul

    2015-10-20

    Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

  20. An experimental method for quantitatively evaluating the elemental processes of indoor radioactive aerosol behavior.

    PubMed

    Yamazawa, H; Yamada, S; Xu, Y; Hirao, S; Moriizumi, J

    2015-11-01

    An experimental method for quantitatively evaluating the elemental processes governing the indoor behaviour of naturally occurring radioactive aerosols was proposed. This method utilises transient response of aerosol concentrations to an artificial change in aerosol removal rate by turning on and off an air purifier. It was shown that the indoor-outdoor exchange rate and the indoor deposition rate could be estimated by a continuous measurement of outdoor and indoor aerosol number concentration measurements and by the method proposed in this study. Although the scatter of the estimated parameters is relatively large, both the methods gave consistent results. It was also found that the size distribution of radioactive aerosol particles and hence activity median aerodynamic diameter remained not largely affected by the operation of the air purifier, implying the predominance of the exchange and deposition processes over other processes causing change in the size distribution such as the size growth by coagulation and the size dependence of deposition.

  1. Aerosol physical properties and their impact on climate change processes

    NASA Astrophysics Data System (ADS)

    Strzalkowska, Agata; Zielinski, Tymon; Petelski, Tomasz; Makuch, Przemyslaw; Pakszys, Paulina; Markuszewski, Piotr; Piskozub, Jacek; Drozdowska, Violetta; Gutowska, Dorota; Rozwadowska, Anna

    2013-04-01

    Characterizing aerosols involves the specification of not only their spatial and temporal distributions but their multi-component composition, particle size distribution and physical properties as well. Due to their light attenuation and scattering properties, aerosols influence radiance measured by satellite for ocean color remote sensing. Studies of marine aerosol production and transport are important for many earth sciences such as cloud physics, atmospheric optics, environmental pollution studies, and interaction between ocean and atmosphere. It was one of the reasons for the growth in the number of research programs dealing with marine aerosols. Sea salt aerosols are among the most abundant components of the atmospheric aerosol, and thus it exerts a strong influence on radiation, cloud formation, meteorology and chemistry of the marine atmosphere. An accurate understanding and description of these mechanisms is crucial to modeling climate and climate change. This work provides information on combined aerosol studies made with lidars and sun photometers onboard the ship and in different coastal areas. We concentrate on aerosol optical thickness and its variations with aerosol advections into the study area. We pay special attention to the problem of proper data collection and analyses techniques. We showed that in order to detect the dynamics of potential aerosol composition changes it is necessary to use data from different stations where measurements are made using the same techniques. The combination of such information with air mass back-trajectories and data collected at stations located on the route of air masses provides comprehensive picture of aerosol variations in the study area both vertically and horizontally. Acknowledgements: The support for this study was provided by the project Satellite Monitoring of the Baltic Sea Environment - SatBałtyk founded by European Union through European Regional Development Fund contract No. POIG 01

  2. The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

    NASA Astrophysics Data System (ADS)

    Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

    2014-12-01

    Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

  3. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, Xiaowen; Khain, Alexander; Matsui, Toshihisa; Lang, Stephen; Simpson, Joanne

    2008-01-01

    Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al ., 2001]." Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 19991. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd, 2005

  4. Parameter sensitivity study of Arctic aerosol vertical distribution in CAM5

    NASA Astrophysics Data System (ADS)

    Jiao, C.; Flanner, M.

    2015-12-01

    Arctic surface temperature response to light-absorbing aerosols (black carbon, brown carbon and dust) depends strongly on their vertical distributions. Improving model simulations of three dimensional aerosol fields in the remote Arctic region will therefore lead to improved projections of the climate change caused by aerosol emissions. In this study, we investigate how different physical parameterizations in the Community Atmosphere Model version 5 (CAM5) influence the simulated vertical distribution of Arctic aerosols. We design experiments to test the sensitivity of the simulated aerosol fields to perturbations of selected aerosol process-related parameters in the Modal Aerosol Module with seven lognormal modes (MAM7), such as those govern aerosol aging, in-cloud and below-cloud scavenging, aerosol hygroscopicity and so on. The simulations are compared with observed aerosol vertical distributions and total optical depth to assess model performance and quantify uncertainties associated with these model parameterizations. Observations applied here include Arctic aircraft measurements of black carbon and sulfate vertical profiles, along with Aerosol Robotic Network (AERONET) optical depth measurements. We also assess the utility of using High Spectral Resolution Lidar (HSRL) measurements from the ARM Barrow site to infer vertical profiles of aerosol extinction. The sensitivity study explored here will provide guidance for optimizing global aerosol simulations.

  5. Ground-based Network and Supersite Measurements for Studying Aerosol Properties and Aerosol-Cloud Interactions

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee; Holben, Brent N.

    2008-01-01

    From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations contain large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite datasets. The development and deployment of AERONET (AErosol RObotic NETwork) sunphotometer network and SMART-COMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile supersite are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To characterize the regional natural and anthropogenic aerosols, AERONET is an internationally federated network of unique sunphotometry that contains more than 250 permanent sites worldwide. Since 1993, there are more than 480 million aerosol optical depth observations and about 15 sites have continuous records longer than 10 years for annual/seasonal trend analyses. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instrument into three categories: flux radiometer, radiance sensor and in-situ probe. Through participation in many satellite remote-sensing/retrieval and validation projects over eight years, SMART-COMMIT have gradually refine( and been proven vital for field deployment. In this paper, we will demonstrate the

  6. Secondary organic aerosol formation through fog processing of VOCs

    NASA Astrophysics Data System (ADS)

    Herckes, P.; Hutchings, J. W.

    2010-07-01

    Volatile Organic Compounds (VOCs) including benzene, toluene, ethylbenzene and xylenes (BTEX) have been determined in highly concentrated amounts (>1 ug/L) in intercepted clouds in northern Arizona (USA). These VOCs are found in concentrations much higher than predicted by partitioning alone. The reactivity of BTEX in the fog/cloud aqueous phase was investigated through laboratory studies. BTEX species showed fast degradation in the aqueous phase in the presence of peroxides and light. Observed half-lives ranged from three and six hours, substantially shorter than the respective gas phase half-lives (several days). The observed reaction rates were on the order of 1 ppb/min but decreased substantially with increasing concentrations of organic matter (TOC). The products of BTEX oxidation reactions were analyzed using HPLC-UV and LCMS. The first generation of products identified included phenol and cresols which correspond to the hydroxyl-addition reaction to benzene and toluene. Upon investigating of multi-generational products, smaller, less volatile species are predominant although a large variety of products is found. Most reaction products have substantially lower vapor pressure and will remain in the particle phase upon droplet evaporation. The SOA generation potential of cloud and fog processing of BTEX was evaluated using simple calculations and showed that in ideal situations these reactions could add up to 9% of the ambient aerosol mass. In more conservative scenarios, the contribution of the processing of BTEX was around 1% of ambient aerosol concentrations. Overall, cloud processing of VOC has the potential to contribute to the atmospheric aerosol mass. However, the contribution will depend upon many factors such as the irradiation, organic matter content in the droplets and droplet lifetime.

  7. On the Physicochemical Processes Controlling Organic Aerosol Hygroscopicity

    NASA Astrophysics Data System (ADS)

    Petters, Sarah Suda

    Aerosol particles in the atmosphere can influence air quality and climate through their interaction with water. Aerosols are an important factor in cloud formation because they serve as cloud condensation nuclei (CCN). Organic compounds contribute a large fraction of the atmospheric aerosol mass but their ability to serve as CCN is less certain relative to inorganic compounds. Limitations of the measurement techniques and theoretical gaps in understanding have prevented agreement between predicted and measured CCN. One way to quantify a compound's CCN activity is by the hygroscopicity parameter, kappa. This dissertation presents research towards constraining the variability of organic aerosol kappa at the process level using three approaches: developing a measurement technique; measuring the dependence of kappa on molecular functional groups; and measuring the effect of surface active molecules on kappa for mixtures. Chapter 2 presents a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) instrument to measure aerosol water uptake at high relative humidity (RH). Measurements up to 99% RH were achieved by improving the precision of aerosol sizing, actively controlling temperature, and calibrating RH between measurements. Osmotic coefficients were obtained within +/-20% for organic aerosols sized between 30 and 200 nanometers. These results may improve water uptake models by providing accurate data at high RH. Chapter 3 presents a study of the sensitivity of kappa to changes in molecular functional group composition for pure compounds. Molecules were synthesized via gas and liquidphase reactions varying the type and location of functional groups, purified by High Performance Liquid Chromatography (HPLC), and routed for CCN measurement. The hydroxyl (-OH) and carbon chain length (-CH2-) changed kappa most, where hydroxyl groups increase kappa and longer carbon chains decrease kappa. This suggests that hydroxyl groups and molecular size dominate the

  8. Development of budesonide nanocluster dry powder aerosols: processing.

    PubMed

    El-Gendy, Nashwa; Selvam, Parthiban; Soni, Pravin; Berkland, Cory

    2012-09-01

    Aerosolized medicine is one of the fastest growing areas in the pharmaceutical industry. Dry powder aerosols of pharmaceutical compounds are particularly attractive for the prevention and treatment of respiratory diseases but are also emerging as a treatment option for systemic diseases. Engineering particles in dry powder formulations can overcome many of the limitations of traditional inhaled pharmaceuticals. Here, a wet milling process for producing agglomerated budesonide nanoparticles (i.e., "NanoClusters") was explored. Parameters such as milling time and drug concentration were investigated, and the aerosol performance of dried budesonide NanoClusters was characterized. The wet milling process was able to produce aerosol particles composed entirely of budesonide. High emitted fraction and a large fine particle fraction suggested that the NanoCluster budesonide formulation would offer highly efficient delivery of drug throughout the lung.

  9. Processing of aerosol particles within the Habshan pollution plume

    NASA Astrophysics Data System (ADS)

    Semeniuk, T. A.; Bruintjes, R.; Salazar, V.; Breed, D.; Jensen, T.; Buseck, P. R.

    2015-03-01

    The Habshan industrial site in the United Arab Emirates produces a regional-scale pollution plume associated with oil and gas processing, discharging high loadings of sulfates and chlorides into the atmosphere, which interact with the ambient aerosol population. Aerosol particles and trace gas chemistry at this site were studied on two flights in the summer of 2002. Measurements were collected along vertical plume profiles to show changes associated with atmospheric processing of particle and gas components. Close to the outlet stack, particle concentrations were over 10,000 cm-3, dropping to <2000 cm-3 in more dilute plume around 1500 m above the stack. Particles collected close to the stack and within the dilute plume were individually measured for size, morphology, composition, and mixing state using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy. Close to the stack, most coarse particles consisted of mineral dust and NaCl crystals from burning oil brines, while sulfate droplets dominated the fine mode. In more dilute plume, at least 1500 m above the stack, the particle spectrum was more diverse, with a significant increase in internally mixed particle types. Dilute plume samples consisted of coarse NaCl/silicate aggregates or NaCl-rich droplets, often with a sulfate component, while fine-fraction particles were of mixed cation sulfates, also internally mixed with nanospherical soot or silicates. Thus, both chloride and sulfate components of the pollution plume rapidly reacted with ambient mineral dust to form coated and aggregate particles, enhancing particle size, hygroscopicity, and reactivity of the coarse mode. The fine-fraction sulfate-bearing particles formed in the plume contribute to regional transport of sulfates, while coarse sulfate-bearing fractions locally reduced the SO2 loading through sedimentation. The chloride- and sulfate-bearing internally mixed particles formed in the plume markedly changed the

  10. CARES: Carbonaceous Aerosol and Radiative Effects Study Science Plan

    SciTech Connect

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-05-27

    Carbonaceous aerosol components, which include black carbon (BC), urban primary organic aerosols (POA), biomass burning aerosols, and secondary organic aerosols (SOA) from both urban and biogenic precursors, have been previously shown to play a major role in the direct and indirect radiative forcing of climate. The primary objective of the CARES 2010 intensive field study is to investigate the evolution of carbonaceous aerosols of different types and their effects on optical and cloud formation properties.

  11. 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.

  12. Modelling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

    NASA Astrophysics Data System (ADS)

    Karl, M.; Kukkonen, J.; Keuken, M. P.; Lützenkirchen, S.; Pirjola, L.; Hussein, T.

    2015-12-01

    This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of one hour, i.e. on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using an aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of n-alkanes, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. It was not necessary to model the nucleation of gas-phase vapors, as the computations were started with roadside conditions. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The effect of condensation and evaporation of organic vapors emitted by vehicles on particle numbers and on particle size distributions was examined. Under inefficient dispersion conditions, condensational growth contributed significantly to the evolution of PN from roadside to the neighborhood scale. The simplified parameterization of aerosol processes can predict particle number concentrations between roadside and the urban background with an inaccuracy of ∼ 10 %, compared to the fully size-resolved MAFOR model.

  13. TEM Study of SAFARI-2000 Aerosols

    NASA Technical Reports Server (NTRS)

    Buseck, Peter R.

    2004-01-01

    The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from biomass smoke plume s in southern Africa and from air masses in the region that are affec ted by the smoke. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and ele ctron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to study aerosol particles from several smoke and haz e samples and from a set of cloud samples.

  14. Halogenation processes of secondary organic aerosol and implications on halogen release mechanisms

    NASA Astrophysics Data System (ADS)

    Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Schmitt-Kopplin, Ph.; Platt, U.; Zetzsch, C.

    2012-07-01

    Reactive halogen species (RHS), such as X·, X2 and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA) and organic aerosol derived from biomass-burning (BBOA) has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols. Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS, released from simulated natural halogen sources like salt pans. Subsequently, the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which results in new functional groups (FTIR spectroscopy), changes UV/VIS absorption, chemical composition (ultrahigh resolution mass spectroscopy (ICR-FT/MS)), or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

  15. Apartment Compartmentalization With an Aerosol-Based Sealing Process

    SciTech Connect

    Maxwell, S.; Berger, D.; Harrington, C.

    2015-03-01

    Air sealing of building enclosures is a difficult and time-consuming process. Current methods in new construction require laborers to physically locate small and sometimes large holes in multiple assemblies and then manually seal each of them. The innovation demonstrated under this research study was the automated air sealing and compartmentalization of buildings through the use of an aerosolized sealant, developed by the Western Cooling Efficiency Center at University of California Davis. CARB sought to demonstrate this new technology application in a multifamily building in Queens, NY. The effectiveness of the sealing process was evaluated by three methods: air leakage testing of overall apartment before and after sealing, point-source testing of individual leaks, and pressure measurements in the walls of the target apartment during sealing.

  16. Spectroscopic Studies of Atmospheric Aerosol Chemistry

    NASA Astrophysics Data System (ADS)

    Wamsley, R.; Leather, K.; Horn, A. B.; Percival, C.

    2008-12-01

    Particles are ubiquitous in the troposphere and are involved in chemical and physical processes affecting the composition of the atmosphere, climate, cloud albedo and human health (Finlayson-Pitts and Pitts, 2000). Organic species, such as alcohols, carboxylic acids, ketones, aldehydes, aromatics, alkenes and alkanes, originate both from anthropogenic and natural sources and comprise a large component of atmospheric particles. Gas-phase species, such as ozone, can oxidize these organics, changing the particle's oxygen-to carbon ratio and potentially altering its hygroscopicity, viscosity, morphology and reactivity. One reaction in particular, that between ozone and oleic acid, has been the focus of several recent studies and extensively researched by Ziemann (2005). Oleic acid reacts readily with ozone and has a low vapor pressure making this reaction convenient to study in the laboratory and has become the benchmark for studying heterogeneous reactions representing the oxidative processing of atmospheric organic aerosols. A critical source of uncertainty in reactivity estimates is a lack of understanding of the mechanism through which some VOCs are oxidized. This knowledge gap is especially critical for aromatic compounds. Because the intermediate reaction steps and products of aromatics oxidation are unknown, chemical mechanisms incorporate parameters estimated from environmental chamber experiments to represent their overall contribution to ozone formation, e.g. Volkamer et al. ( 2006). Previous studies of uncertainties in incremental reactivity estimates for VOCs found that the representation of aromatics chemistry contributed significantly to the estimated 40 - 50% uncertainties in the incremental reactivities of common aromatic compounds Carter et al. (2002). This study shows development of an effective IR method that can monitor the reaction and hence obtain the kinetics of the ozonolysis of an aromatic compound in the aerosol phase. The development of such

  17. Representing Cloud Processing of Aerosol in Numerical Models

    SciTech Connect

    Mechem, D.B.; Kogan, Y.L.

    2005-03-18

    The satellite imagery in Figure 1 provides dramatic examples of how aerosol influences the cloud field. Aerosol from ship exhaust can serve as nucleation centers in otherwise cloud-free regions, forming ship tracks (top image), or can enhance the reflectance/albedo in already cloudy regions. This image is a demonstration of the first indirect effect, in which changes in aerosol modulate cloud droplet radius and concentration, which influences albedo. It is thought that, through the effects it has on precipitation (drizzle), aerosol can also affect the structure and persistence of planetary boundary layer (PBL) clouds. Regions of cellular convection, or open pockets of cloudiness (bottom image) are thought to be remnants of strongly drizzling PBL clouds. Pockets of Open Cloudiness (POCs) (Stevens et al. 2005) or Albrecht's ''rifts'' are low cloud fraction regions characterized by anomalously low aerosol concentrations, implying they result from precipitation. These features may in fact be a demonstration of the second indirect effect. To accurately represent these clouds in numerical models, we have to treat the coupled cloud-aerosol system. We present the following series of mesoscale and large eddy simulation (LES) experiments to evaluate the important aspects of treating the coupled cloud-aerosol problem. 1. Drizzling and nondrizzling simulations demonstrate the effect of drizzle on a mesoscale forecast off the California coast. 2. LES experiments with explicit (bin) microphysics gauge the relative importance of the shape of the aerosol spectrum on the 3D dynamics and cloud structure. 3. Idealized mesoscale model simulations evaluate the relative roles of various processes, sources, and sinks.

  18. a Study of the Origin of Atmospheric Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Hildemann, Lynn Mary

    1990-01-01

    The sources of ambient organic particulate matter in urban areas are investigated through a program of emission source measurements, atmospheric measurements, and mathematical modeling of source/receptor relationships. A dilution sampler intended to collect fine organic aerosol from combustion sources is designed to simulate atmospheric cooling and dilution processes, so that organic vapors which condense under ambient conditions will be collected as particulate matter. This system is used to measure the emissions from a boiler burning distillate oil, a home fireplace, catalyst and noncatalyst automobiles, heavy-duty diesel trucks, natural gas home appliances, and meat cooking operations. Alternate techniques are used to sample the particulate matter emitted from cigarette smoking, a roofing tar pot, paved road dust, brake lining wear, tire wear, and vegetative detritus. The bulk chemical characteristics of the fine aerosol fraction are presented for each source. Over half of the fine aerosol mass emitted from automobiles, wood burning, meat cooking, home appliances, cigarettes, and tar pots is shown to consist of organic compounds. The organic material collected from these sources is analyzed using high-resolution gas chromatography. Using a simple analytical protocol, a quantitative, 50-parameter characterization of the elutable fine organic aerosol emitted from each source type is obtained, which proves to be a unique fingerprint that can be used to distinguish most sources from each other. A mathematical model is used to predict the characteristics of fine ambient organic aerosol in the Los Angeles area that would prevail if the primary organic emissions are transported without chemical reaction. The model is found to track the seasonal variations observed in the ambient aerosol at the three sites studied. Emissions from vehicles and fireplaces are identified as significant sources of solvent-extractable organic aerosol. Differences between the model

  19. Combined effects of organic aerosol loading and fog processing on organic aerosols oxidation and composition

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Tripathi, Sachchida; Gupta, Tarun

    2016-04-01

    Fog is a natural meteorological phenomenon that occurs throughout the world, it contains substantial quantity of liquid water and generally seen as a natural cleansing agent but it also has the potential to form highly oxidized secondary organic aerosols (SOA) via aqueous processing of ambient aerosols. On the other hand higher organic aerosols (OA) loading tend to decrease the overall oxidation level (O/C) of the particle phase organics, due to enhanced partitioning of less oxidized organics from gas to particle phase. However, combined impact of these two parameters; aqueous oxidation and OA loading, on the overall oxidation ratio (O/C) of ambient OA has never been studied. To assess this, real time ambient sampling using HR-ToF-AMS was carried out at Kanpur, India from 15 December 2014 - 10 February 2015. In first 3 weeks of this campaign, very high OA loading is (134 ± 42 μg/m3) observed (termed as high loading or HL period) while loading is substantially reduced from 2nd January, 2016 (56 ± 20 μg/m3, termed as low loading or LL period) . However, both the loading period was affected by several fog episodes (10 in HL and 7 in LL), thus providing the opportunity of studying the combined effects of fog and OA loading on OA oxidation. It is found that O/C ratio is very strongly anti-correlated with OA loading in both the loading period, however, slope of this ant-correlation is much steep during HL period than in LL period. Source apportionment of OA revealed that there is drastic change in the types of OA from HL to LL period, clearly indicating difference in OA composition from HL to LL period. During foggy night continuous oxidation of OA is observed from early evening to early morning with 15-20% enhancement in O/C ratio, while the same is absent during non-foggy period, clearly indicating the efficient fog processing of ambient OA. It is also found that night time fog aqueous oxidation can be as effective as daytime photo chemistry in oxidation of OA. Fog

  20. Fluorescent lidar for organic aerosol study

    NASA Astrophysics Data System (ADS)

    Matvienko, G. G.; Timofeev, V. I.; Grishin, A. I.; Fateyeva, N. L.

    2005-10-01

    The paper describes the fluorescent lidar created for monitoring of the atmosphere and for estimating the content of fluorescent components of organic aerosol. The lidar operation is based on the use of ultraviolet radiation of harmonics of Nd:YAG solid state laser for exciting the atmospheric fluorescence and the spectral analysis of the atmospheric fluorescence is used in the near ultraviolet and blue spectral range with the resolution of 2 nm. The lidar was found to be efficient for remote analysis of organic aerosol occurring as a result of vegetation emission of secondary metabolites to the atmosphere. Fluorescence spectra processing allows us to select some organic compounds, which molecules contain 7 and more carbon atoms. Taking into account the availability of interconnection between organic aerosol and vegetation, in lidar the second harmonic of Nd:YAG laser is also used for exciting the fluorescence of vegetation covers. In this case the receiving system detects the fluorescence of vegetation in the red spectral range conditioned by the chlorophyll of vegetation. Simultaneous detection of the fluorescence from the atmosphere and from vegetation makes it possible to obtain data on the interaction of the atmosphere and underlying surface covered by vegetation. It has been found that a disruption in the vegetation feeding or the impact of pollutions on vegetation resulted in a sharp increase of the fluorescence intensity of vegetation chlorophyll in the red spectral range and in the simultaneous appearance of organic aerosol in the atmosphere adjacent to vegetation in the region of negative impact.

  1. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3- aerosol during the 2013 Southern Oxidant and Aerosol Study

    SciTech Connect

    Allen, Hannah M.; Draper, Danielle C.; Ayres, Benjamin R.; Ault, Andrew P.; Bondy, Amy L.; Takahama, S.; Modini, Robert; Baumann, K.; Edgerton, Eric S.; Knote, Christoph; Laskin, Alexander; Wang, Bingbing; Fry, Juliane L.

    2015-09-25

    The inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 1 June to 15 July 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA), an ion chromatograph coupled with a wet rotating denuder and a steam-jet aerosol collector for monitoring of ambient inorganic gas and aerosol species, revealed two periods of high aerosol nitrate (NO3 ) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of coarse mode mineral or sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 um) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of mineral dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. Calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3 is produced primarily by this process, and is likely limited by the availability of mineral dust surface area. Modeling of NO3 and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas/aerosol phase partitioning.

  2. Processes influencing secondary aerosol formation in the San Joaquin Valley during winter

    SciTech Connect

    Frederick W. Lurmann; Steven G. Brown; Michael C. McCarthy; Paul T. Roberts

    2006-12-15

    Air quality data collected in the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM2.5) mass concentrations in California ({le} 188 {mu}g/m{sup 3} 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NOx)-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NOx and volatile organic compound (VOC) emissions plus background O{sub 3} levels are expected to determine NOx oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter. 59 refs., 11 figs., 1 tab.

  3. Enhancement of aerosol responses to changes in emissions over East Asia by gas-oxidant-aerosol coupling and detailed aerosol processes

    NASA Astrophysics Data System (ADS)

    Matsui, H.; Koike, M.

    2016-06-01

    We quantify the responses of aerosols to changes in emissions (sulfur dioxide, black carbon (BC), primary organic aerosol, nitrogen oxides (NOx), and volatile organic compounds) over East Asia by using simulations including gas-oxidant-aerosol coupling, organic aerosol (OA) formation, and BC aging processes. The responses of aerosols to NOx emissions are complex and are dramatically changed by simulating gas-phase chemistry and aerosol processes online. Reduction of NOx emissions by 50% causes a 30-40% reduction of oxidant (hydroxyl radical and ozone) concentrations and slows the formation of sulfate and OA by 20-30%. Because the response of OA to changes in NOx emissions is sensitive to the treatment of emission and oxidation of semivolatile and intermediate volatility organic compounds, reduction of the uncertainty in these processes is necessary to evaluate gas-oxidant-aerosol coupling accurately. Our simulations also show that the sensitivity of aerosols to changes in emissions is enhanced by 50-100% when OA formation and BC aging processes are resolved in the model. Sensitivity simulations show that the increase of NOx emissions from 1850 to 2000 explains 70% (40%) of the enhancement of aerosol mass concentrations (direct radiative effects) over East Asia during that period through enhancement of oxidant concentrations and that this estimation is sensitive to the representation of OA formation and BC aging processes. Our results demonstrate the importance of simultaneous simulation of gas-oxidant-aerosol coupling and detailed aerosol processes. The impact of NOx emissions on aerosol formation will be a key to formulating effective emission reduction strategies such as BC mitigation and aerosol reduction policies in East Asia.

  4. Analysis of aerosol emission and hazard evaluation of electrical discharge machining (EDM) process.

    PubMed

    Jose, Mathew; Sivapirakasam, S P; Surianarayanan, M

    2010-01-01

    The safety and environmental aspects of a manufacturing process are important due to increased environmental regulations and life quality. In this paper, the concentration of aerosols in the breathing zone of the operator of Electrical Discharge Machining (EDM), a commonly used non traditional manufacturing process is presented. The pattern of aerosol emissions from this process with varying process parameters such as peak current, pulse duration, dielectric flushing pressure and the level of dielectric was evaluated. Further, the HAZOP technique was employed to identify the inherent safety aspects and fire risk of the EDM process under different working conditions. The analysis of aerosol exposure showed that the concentration of aerosol was increased with increase in the peak current, pulse duration and dielectric level and was decreased with increase in the flushing pressure. It was also found that at higher values of peak current (7A) and pulse duration (520 micros), the concentration of aerosols at breathing zone of the operator was above the permissible exposure limit value for respirable particulates (5 mg/m(3)). HAZOP study of the EDM process showed that this process is vulnerable to fire and explosion hazards. A detailed discussion on preventing the fire and explosion hazard is presented in this paper. The emission and risk of fire of the EDM process can be minimized by selecting proper process parameters and employing appropriate control strategy.

  5. An experimental study of dense aerosol aggregations

    NASA Astrophysics Data System (ADS)

    Dhaubhadel, Rajan

    We demonstrated that an aerosol can gel. This gelation was then used for a one-step method to produce an ultralow density porous carbon or silica material. This material was named an aerosol gel because it was made via gelation of particles in the aerosol phase. The carbon and silica aerosol gels had high specific surface area (200--350 sq m2/g for carbon and 300--500 sq m2/g for silica) and an extremely low density (2.5--6.0 mg/cm3), properties similar to conventional aerogels. Key aspects to form a gel from an aerosol are large volume fraction, ca. 10-4 or greater, and small primary particle size, 50 nm or smaller, so that the gel time is fast compared to other characteristic times. Next we report the results of a study of the cluster morphology and kinetics of a dense aggregating aerosol system using the small angle light scattering technique. The soot particles started as individual monomers, ca. 38 nm radius, grew to bigger clusters with time and finally stopped evolving after spanning a network across the whole system volume. This spanning is aerosol gelation. The gelled system showed a hybrid morphology with a lower fractal dimension at length scales of a micron or smaller and a higher fractal dimension at length scales greater than a micron. The study of the kinetics of the aggregating system showed that when the system gelled, the aggregation kernel homogeneity lambda attained a value 0.4 or higher. The magnitude of the aggregation kernel showed an increase with increasing volume fraction. We also used image analysis technique to study the cluster morphology. From the digitized pictures of soot clusters the cluster morphology was determined by two different methods: structure factor and perimeter analysis. We find a hybrid, superaggregate morphology characterized by a fractal dimension of Df ≈ to 1.8 between the monomer size, ca. 50 nm, and 1 mum micron and Df ≈ to 2.6 at larger length scales up to ˜ 10 mum. The superaggregate morphology is a

  6. Modeling aerosols and their interactions with shallow cumuli during the 2007 CHAPS field study

    SciTech Connect

    Shrivastava, ManishKumar B.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Laskin, Alexander; Chapman, Elaine G.; Gustafson, William I.; Liu, Ying; Berkowitz, Carl M.

    2013-02-07

    The Weather Research and Forecasting model coupled with chemistry (WRF-Chem) is used to simulate relationships between aerosols and clouds in the vicinity of Oklahoma City during the June 2007 Cumulus Humilis Aerosol Processing Study (CHAPS). The regional scale simulation completed using 2 km horizontal grid spacing evaluates four important relationships between aerosols and shallow cumulus clouds observed during CHAPS. First, the model reproduces the trends of higher nitrate volume fractions in cloud droplet residuals compared to interstitial non-activated aerosols, as measured using the Aerosol Mass Spectrometer. Comparing simulations with cloud chemistry turned on and off, we show that nitric acid vapor uptake by cloud droplets explains the higher nitrate content of cloud droplet residuals. Second, as documented using an offline code, both aerosol water and other inorganics (OIN), which are related to dust and crustal emissions, significantly affect predicted aerosol optical properties. Reducing the OIN content of wet aerosols by 50% significantly improves agreement of model predictions with measurements of aerosol optical properties. Third, the simulated hygroscopicity of aerosols is too high as compared to their hygroscopicity derived from cloud condensation nuclei and particle size distribution measurements, indicating uncertainties associated with simulating size-dependent chemical composition and treatment of aerosol mixing state within the model. Fourth, the model reasonably represents the observations of the first aerosol indirect effect where pollutants in the vicinity of Oklahoma City increase cloud droplet number concentrations and decrease the droplet effective radius. While previous studies have often focused on cloud-aerosol interactions in stratiform and deep convective clouds, this study highlights the ability of regional-scale models to represent some of the important aspects of cloud-aerosol interactions associated with fields of short

  7. Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

    NASA Astrophysics Data System (ADS)

    Lee, Hsiang-He; Chen, Shu-Hua; Kleeman, Michael J.; Zhang, Hongliang; DeNero, Steven P.; Joe, David K.

    2016-07-01

    The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and was applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-D chemical variable (X, Z, Y, size bins, source types, species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and long-wave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into cloud condensation nuclei (CCN) at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

  8. Some results of an experimental study of the atmospheric aerosol in Tomsk: A combined approach

    SciTech Connect

    Zuev, V.V.

    1996-04-01

    As widely accepted, aerosols strongly contribute to the formation of the earth`s radiation balance through the absorption and scattering of solar radiation. In addition, aerosols, being active condensation nuclei, also have a role in the cloud formation process. In this paper, results are presented of aerosol studies undertaken at the field measurement sites of the Institute of Atmospheric Optics in Tomsk and the Tomsk region.

  9. Field and Laboratory Studies of Atmospheric Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Coggon, Matthew Mitchell

    This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of

  10. Experimental studies of gas-aerosol reactions

    NASA Astrophysics Data System (ADS)

    Gupta, Anand

    1991-05-01

    The aqueous phase oxidation of SO2 by H2O2 is believed to the principle mechanism for atmospheric sulfate formation in cloud droplets. However, no studies in noncloud aerosol systems have been reported. The objective is to quantify the importance of the noncloud liquid phase reactions of SO2 by H2O2 in the atmosphere. Growth rates of submicron droplets exposed to SO2 and H2O2 were measured using the tandem differential mobility analyzer (TDMA) technique (Rader and McMurry, 1986). The technique uses differential mobility analyzers (DMA's) to generate monodisperse particles and to measure particle size after the reaction. To facilitate submicron monodisperse droplet production with the DMA, a low-ion-concentration charter capable of generating singly charged particles up to 1.0 microns was developed and experimentally evaluated. The experiments were performed using dry and deliquesced (NH4)2SO4 particles with SO2 and H2O2 concentrations from 0-860 ppb and 0-150 ppb, respectively. No growth was observed for dry particles. For droplets greater than or equal to 0.3 microns, the fractional diameter growth was independent of particle size and for droplets less than or equal to 0.2 microns, it decreased as particle size decreased. The observed decrease is due to NH3 evaporation. As ammonia evaporates, droplet pH decreases causing the oxidation rate to decrease, leading to a lower growth rate. To predict the size-dependent growth rates, a theoretical model was developed using solution thermodynamics, gas/particle equilibrium, and chemical kinetics. The experimental and theoretical results are in reasonable agreement. For dry (NH4)2SO4 particles exposed to SO2, H2O2, NH3, and H2O vapor, surface reaction-controlled growth was observed. Particle growth was very sensitive to particle composition. No growth was observed for Polystyrene latex particles, whereas (NH4)2SO4 particles doped with catalysts (Fe(2+), Fe(3+), Mn(2+) and Cu(2+)) in a molar ratio of 1:500 grew slower than

  11. Studying Taklamakan aerosol properties with lidar (STAPL)

    NASA Astrophysics Data System (ADS)

    Cottle, Paul; Mueller, Detlef; Shin, Dong-Ho; Zhang, Xiao Xiao; Feng, Guanglong; McKendry, Ian; Strawbridge, Kevin

    2013-10-01

    By now, the global impacts of atmospheric dust have been well-established. Nevertheless, relevant properties such as size distribution, depolarization ratio, and even single-scattering albedo have been shown to vary substantially between dust producing regions and are also strongly dependant on the conditions under which the dust is emitted. Even greater variations have been documented during the process of long-range transport. With continued improvement of detection technologies, research focus is increasingly turning to refinement of our knowledge of these properties of dust in order to better account for the presence of dust in models and data analysis. The purpose of this study is to use a combination of lidar data and models to directly observe the changing properties of dust layers as they are transported from their origin in the Taklamakan Desert of western China. With the co-operation of the Xinjiang Institute of Ecology and Geography, a portable micropulse lidar system was installed at Aksu National Field on the northern edge of the Tarim Basin in late April 2013, during the Spring dust storm season. Over six days, data were collected on the optical properties of dust emissions passing over this location. The measurements of this lidar have shown the dust over Aksu on these days to have a significantly higher depolarization ratio than has been previously reported for the region. Model results show this dust was then transported across the region at least as far as Korea and Japan. Models from the Naval Aerosol Analysis and Prediction System (NAAPS) show that during transport the dust layers became intermixed with sulfate emissions from industrial sources in China as well as smoke from wildfires burning in south-east Asia and Siberia. The multi-wavelength raman-elastic lidar located in Gwangju South Korea was used to observe the vertical structure of the layers as well as optical properties such as colour ratio, depolarization ratio and extinction

  12. A study of the origin of atmospheric organic aerosols

    SciTech Connect

    Hildemann, L.M.

    1990-01-01

    The sources of ambient organic particulate matter in urban areas are investigated through a program of emission source measurements, atmospheric measurements, and mathematical modeling of source/receptor relationships. A dilution sampler intended to collect fine organic aerosol from combustion sources is designed to simulate atmospheric cooling and dilution processes, so that organic vapors which condense under ambient conditions will be collected as particulate matter. This system is used to measure the emissions from a boiler burning distillate oil, a home fireplace, catalyst and noncatalyst automobiles, heavy-duty diesel trucks, natural gas home appliances, and meat-cooking operations. Alternate techniques are used to sample the particulate matter emitted from cigarette smoking, a roofing tar pot, paved road dust, brake lining wear, tire wear, and vegetative detritus. The bulk chemical characteristics of the fine aerosol fraction are presented for each source. Over half of the fine aerosol mass emitted from automobiles, wood burning, meat cooking, home appliances, cigarettes, and tar pots is shown to consist of organic compounds. The organic material collected from these sources is analyzed using high-resolution gas chromatography. Using a simple analytical protocol, a quantitative, 50-parameter characterization of the elutable fine organic aerosol emitted from each source type is obtained, which proves to be a unique fingerprint that can be used to distinguish most sources from each other. A mathematical model is used to predict the characteristics of fine ambient organic aerosol in the Los Angeles area that would prevail if the primary organic emissions are transported without chemical reaction. The model is found to track the seasonal variations observed in the ambient aerosol at the three sites studied.

  13. Study on Dicarboxylic Acids in Aerosol Samples with Capillary Electrophoresis

    PubMed Central

    Adler, Heidi; Sirén, Heli

    2014-01-01

    The research was performed to study the simultaneous detection of a homologous series of α, ω-dicarboxylic acids (C2–C10), oxalic, malonic, succinic, glutaric, adipic, pimelic, suberic, azelaic, and sebacic acids, with capillary electrophoresis using indirect UV detection. Good separation efficiency in 2,6-pyridinedicarboxylic acid as background electrolyte modified with myristyl trimethyl ammonium bromide was obtained. The dicarboxylic acids were ionised and separated within five minutes. For the study, authentic samples were collected onto dry cellulose membrane filters of a cascade impactor (12 stages) from outdoor spring aerosols in an urban area. Hot water and ultrasonication extraction methods were used to isolate the acids from membrane filters. Due to the low concentrations of acids in the aerosols, the extracts were concentrated with solid-phase extraction (SPE) before determination. The enrichment of the carboxylic acids was between 86 and 134% with sample pretreatment followed by 100-time increase by preparation of the sample to 50 μL. Inaccuracy was optimised for all the sample processing steps. The aerosols contained dicarboxylic acids C2–C10. Then, mostly they contained C2, C5, and C10. Only one sample contained succinic acid. In the study, the concentrations of the acids in aerosols were lower than 10 ng/m3. PMID:24729915

  14. Importance of relative humidity in the oxidative ageing of organic aerosols: case study of the ozonolysis of maleic acid aerosol

    NASA Astrophysics Data System (ADS)

    Gallimore, P. J.; Achakulwisut, P.; Pope, F. D.; Davies, J. F.; Spring, D. R.; Kalberer, M.

    2011-12-01

    Many important atmospheric aerosol processes depend on the chemical composition of the aerosol, e.g. water uptake and particle cloud interactions. Atmospheric ageing processes, such as oxidation reactions, significantly and continuously change the chemical composition of aerosol particles throughout their lifetime. These ageing processes are often poorly understood. In this study we utilize an aerosol flow tube set up and an ultra-high resolution mass spectrometer to explore the effect of relative humidity (RH) in the range of <5-90% on the ozonolysis of maleic acid aerosol which is employed as model organic aerosol system. Due to the slow reaction kinetics relatively high ozone concentrations of 160-200 ppm were used to achieve an appreciable degree of oxidation of maleic acid. The effect of oxidative ageing on the hygroscopicity of maleic acid particles is also investigated using an electrodynamic balance and thermodynamic modelling. RH has a profound effect on the oxidation of maleic acid particles. Very little oxidation is observed at RH < 50% and the only observed reaction products are glyoxylic acid and formic acid. In comparison, when RH > 50% there are about 15 oxidation products identified. This increased oxidation was observed even when the particles were exposed to high humidities long after a low RH ozonolysis reaction. This result might have negative implications for the use of water as an extraction solvent for the analysis of oxidized organic aerosols. These humidity-dependent differences in the composition of the ozonolyzed aerosol demonstrate that water is both a key reactant in the oxidation scheme and a determinant of particle phase and hence diffusivity. The measured chemical composition of the processed aerosol is used to model the hygroscopic growth, which compares favourably with water uptake results from the electrodynamic balance measurements. A reaction mechanism is presented which takes into account the RH dependent observations. This

  15. Aqueous phase processing of secondary organic aerosol from isoprene photooxidation

    NASA Astrophysics Data System (ADS)

    Liu, Y.; Monod, A.; Tritscher, T.; Praplan, A. P.; DeCarlo, P. F.; Temime-Roussel, B.; Quivet, E.; Marchand, N.; Dommen, J.; Baltensperger, U.

    2012-07-01

    Transport of reactive air masses into humid and wet areas is highly frequent in the atmosphere, making the study of aqueous phase processing of secondary organic aerosol (SOA) very relevant. We have investigated the aqueous phase processing of SOA generated from gas-phase photooxidation of isoprene using a smog chamber. The SOA collected on filters was extracted by water and subsequently oxidized in the aqueous phase either by H2O2 under dark conditions or by OH radicals in the presence of light, using a photochemical reactor. Online and offline analytical techniques including SMPS, HR-AMS, H-TDMA, TD-API-AMS, were employed for physical and chemical characterization of the chamber SOA and nebulized filter extracts. After aqueous phase processing, the particles were significantly more hygroscopic, and HR-AMS data showed higher signal intensity at m/z 44 and a lower signal intensity at m/z 43, thus showing the impact of aqueous phase processing on SOA aging, in good agreement with a few previous studies. Additional offline measurement techniques (IC-MS, APCI-MS2 and HPLC-APCI-MS) permitted the identification and quantification of sixteen individual chemical compounds before and after aqueous phase processing. Among these compounds, small organic acids (including formic, glyoxylic, glycolic, butyric, oxalic and 2,3-dihydroxymethacrylic acid (i.e. 2-methylglyceric acid)) were detected, and their concentrations significantly increased after aqueous phase processing. In particular, the aqueous phase formation of 2-methylglyceric acid and trihydroxy-3-methylbutanal was correlated with the consumption of 2,3-dihydroxy-2-methyl-propanal, and 2-methylbutane-1,2,3,4-tetrol, respectively, and an aqueous phase mechanism was proposed accordingly. Overall, the aging effect observed here was rather small compared to previous studies, and this limited effect could possibly be explained by the lower liquid phase OH concentrations employed here, and/or the development of oligomers

  16. Primary and secondary aerosols in Beijing in winter: sources, variations and processes

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

    2016-07-01

    Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size

  17. Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Volkamer, R.

    2010-09-01

    This study presents a modeling framework based on laboratory data to describe the kinetics of glyoxal reactions that form secondary organic aerosol (SOA) in aqueous aerosol particles. Recent laboratory results on glyoxal reactions are reviewed and a consistent set of empirical reaction rate constants is derived that captures the kinetics of glyoxal hydration and subsequent reversible and irreversible reactions in aqueous inorganic and water-soluble organic aerosol seeds. Products of these processes include (a) oligomers, (b) nitrogen-containing products, (c) photochemical oxidation products with high molecular weight. These additional aqueous phase processes enhance the SOA formation rate in particles and yield two to three orders of magnitude more SOA than predicted based on reaction schemes for dilute aqueous phase (cloud) chemistry for the same conditions (liquid water content, particle size). The application of the new module including detailed chemical processes in a box model demonstrates that both the time scale to reach aqueous phase equilibria and the choice of rate constants of irreversible reactions have a pronounced effect on the predicted atmospheric relevance of SOA formation from glyoxal. During day time, a photochemical (most likely radical-initiated) process is the major SOA formation pathway forming ∼5 μg m-3 SOA over 12 h (assuming a constant glyoxal mixing ratio of 300 ppt). During night time, reactions of nitrogen-containing compounds (ammonium, amines, amino acids) contribute most to the predicted SOA mass; however, the absolute predicted SOA masses are reduced by an order of magnitude as compared to day time production. The contribution of the ammonium reaction significantly increases in moderately acidic or neutral particles (5 < pH < 7). Glyoxal uptake into ammonium sulfate seed under dark conditions can be represented with a single reaction parameter keffupt that does not depend on aerosol loading or water content, which indicates a

  18. Solar thermal aerosol flow reaction process

    SciTech Connect

    Weimer, Alan W.; Dahl, Jaimee K.; Pitts, J. Roland; Lewandowski, Allan A.; Bingham, Carl; Tamburini, Joseph R.

    2005-03-29

    The present invention provides an environmentally beneficial process using concentrated sunlight to heat radiation absorbing particles to carry out highly endothermic gas phase chemical reactions ultimately resulting in the production of hydrogen or hydrogen synthesis gases.

  19. The Aerosol Measurement and Processing System: New Capabilities and Results

    NASA Astrophysics Data System (ADS)

    Braverman, A.; Kalashnikova, O.; Manipon, G.; Paradise, S.; Penner, J.; Wilson, B.; Xing, Z.; Xu, L.

    2008-12-01

    The Aerosol Measurement and Processing System (AMAPS) is a grid based, distributed computing environment for aerosol science. AMAPS is motivated by the community's call for a modern infrastructure to access, manipulate and analyze aerosol data (see the Bulletin of the American Meteorological Society, October 2003). AMAPS offers access, subsetting, and data analysis functions for level 2 aerosol data products from MISR, MODIS, and AERONET, including the new AERONET Maritime Network. The system is available in two modes: service user mode and power user mode. Service users access data and computational capabilities through pre-constructed web pages that call workflows: web service functions chained together in XML documents. Power users access computational capabilities from the command line of AMAPS-enabled computers, by embedding web service calls directly in their python programs. The AMAPS python package also offers streamlined functions to read, extract and manipulate data over the internet. In this talk, we review the latest improvements and enhancements including the addition of the MODIS level 2 cloud product, and discuss recent science findings enabled by the AMAPS system.

  20. Processes controlling the annual cycle of Arctic aerosol number and size distributions

    NASA Astrophysics Data System (ADS)

    Croft, Betty; Martin, Randall V.; Leaitch, W. Richard; Tunved, Peter; Breider, Thomas J.; D'Andrea, Stephen D.; Pierce, Jeffrey R.

    2016-03-01

    Measurements at high-Arctic sites (Alert, Nunavut, and Mt. Zeppelin, Svalbard) during the years 2011 to 2013 show a strong and similar annual cycle in aerosol number and size distributions. Each year at both sites, the number of aerosols with diameters larger than 20 nm exhibits a minimum in October and two maxima, one in spring associated with a dominant accumulation mode (particles 100 to 500 nm in diameter) and a second in summer associated with a dominant Aitken mode (particles 20 to 100 nm in diameter). Seasonal-mean aerosol effective diameter from measurements ranges from about 180 in summer to 260 nm in winter. This study interprets these annual cycles with the GEOS-Chem-TOMAS global aerosol microphysics model. Important roles are documented for several processes (new-particle formation, coagulation scavenging in clouds, scavenging by precipitation, and transport) in controlling the annual cycle in Arctic aerosol number and size. Our simulations suggest that coagulation scavenging of interstitial aerosols in clouds by aerosols that have activated to form cloud droplets strongly limits the total number of particles with diameters less than 200 nm throughout the year. We find that the minimum in total particle number in October can be explained by diminishing new-particle formation within the Arctic, limited transport of pollution from lower latitudes, and efficient wet removal. Our simulations indicate that the summertime-dominant Aitken mode is associated with efficient wet removal of accumulation-mode aerosols, which limits the condensation sink for condensable vapours. This in turn promotes new-particle formation and growth. The dominant accumulation mode during spring is associated with build up of transported pollution from outside the Arctic coupled with less-efficient wet-removal processes at colder temperatures. We recommend further attention to the key processes of new-particle formation, interstitial coagulation, and wet removal and their delicate

  1. Processes Controlling the Seasonal Cycle of Arctic Aerosol Number and Size Distributions

    NASA Astrophysics Data System (ADS)

    Wentworth, G.; Croft, B.; Martin, R.; Leaitch, W. R.; Tunved, P.; Breider, T. J.; D'Andrea, S.; Pierce, J. R.; Murphy, J. G.; Kodros, J.; Abbatt, J.

    2015-12-01

    Measurements at high-Arctic sites show a strong seasonal cycle in aerosol number and size. The number of aerosols with diameters larger than 20 nm exhibits a maximum in late spring associated with a dominant accumulation mode, and a second maximum in the summer associated with a dominant Aitken mode. Seasonal-mean aerosol effective diameter ranges from about 160 nm in summer to 250 nm in winter. This study interprets these seasonal cycles with the GEOS-Chem-TOMAS global aerosol microphysics model. We find improved agreement with in situ measurements (SMPS) of aerosol size at both Alert, Nunavut, and Mt. Zeppelin, Svalbard following model developments: 1) increase the efficiency of wet scavenging in the Arctic summer and 2) represent coagulation between interstitial aerosols and aerosols activated to form cloud droplets. Our simulations indicate that the dominant summer-time Aitken mode is associated with increased efficiency of wet removal, which limits the number of larger aerosols and promotes local new-aerosol formation. We also find an important role of interstitial coagulation in clouds in the Arctic, which limits the number of Aitken-mode aerosols in the non-summer seasons when direct wet removal of these aerosols is inefficient. The summertime Arctic atmosphere is particularly pristine and strongly influenced by natural regional emissions which have poorly understood climate impacts. Especially influenced are the climatic roles of atmospheric particles and clouds. Here we present evidence that ammonia (NH3) emissions from migratory-seabird guano (dung) are the primary contributor to summertime free ammonia levels recently measured in the Canadian Arctic atmosphere. These findings suggest that ammonia from seabird guano is a key factor contributing to bursts of new-particle formation, which are observed every summer in the near-surface atmosphere at Alert, Canada. Chemical transport model simulations show that these newly formed particles can grow by vapour

  2. Experimental Technique for Studying Aerosols of Lyophilized Bacteria

    PubMed Central

    Cox, Christopher S.; Derr, John S.; Flurie, Eugene G.; Roderick, Roger C.

    1970-01-01

    An experimental technique is presented for studying aerosols generated from lyophilized bacteria by using Escherichia coli B, Bacillus subtilis var. niger, Enterobacter aerogenes, and Pasteurella tularensis. An aerosol generator capable of creating fine particle aerosols of small quantities (10 mg) of lyophilized powder under controlled conditions of exposure to the atmosphere is described. The physical properties of the aerosols are investigated as to the distribution of number of aerosol particles with particle size as well as to the distribution of number of bacteria with particle size. Biologically unstable vegetative cells were quantitated physically by using 14C and Europium chelate stain as tracers, whereas the stable heat-shocked B. subtilis spores were assayed biologically. The physical persistence of the lyophilized B. subtilis aerosol is investigated as a function of size of spore-containing particles. The experimental result that physical persistence of the aerosol in a closed aerosol chamber increases as particle size is decreased is satisfactorily explained on the bases of electrostatic, gravitational, inertial, and diffusion forces operating to remove particles from the particular aerosol system. The net effect of these various forces is to provide, after a short time interval in the system (about 2 min), an aerosol of fine particles with enhanced physical stability. The dependence of physical stability of the aerosol on the species of organism and the nature of the suspending medium for lyophilization is indicated. Also, limitations and general applicability of both the technique and results are discussed. PMID:4992657

  3. Glass formation processes in mixed inorganic/organic aerosol particles.

    PubMed

    Dette, Hans P; Koop, Thomas

    2015-05-14

    Recent experiments suggest that organic aerosol particles may transform into a glassy state at room temperature under dry conditions. Information on glass forming processes in mixed inorganic/organic aerosol particles is sparse, however, because inorganic crystal nucleation is usually very likely in such mixtures. Here we investigate the glass transition temperatures Tg of various organics (trehalose, sucrose, citric acid, sorbitol, and glycerol as well as 3-MBTCA) in binary mixtures with either NaNO3 or NH4HSO4 at different mass fractions. The glassy samples were prepared with the MARBLES technique by atomizing dilute aqueous solutions into aerosol particles and subsequent diffusion drying. The resulting aerosol particles were collected and their phase behavior was investigated using differential scanning calorimetry. At small and intermediate inorganic mass fractions salt crystallization did not occur. Instead, the single-phase mixtures remained in an amorphous state upon drying such that determination of their Tg was possible. From these measurements the Tg value of pure NaNO3 and pure NH4HSO4 could be inferred through extrapolation, resulting in values of Tg(NaNO3) ≈ 290 K and Tg(NH4HSO4) ≈ 220 K. Upon drying of NH4HSO4/3-MBTCA mixtures, phase-separated samples formed in which the inorganic-rich and organic-rich phases each show an independent glass transition. Our measurements provide a route toward establishing Tg values of inorganic salts that usually crystallize readily, and they may explain the reported contradicting observations of NaNO3 aerosol particles to either crystallize or remain amorphous upon drying at room temperature. PMID:25490407

  4. 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.

  5. Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

    NASA Astrophysics Data System (ADS)

    Karl, Matthias; Kukkonen, Jaakko; Keuken, Menno P.; Lützenkirchen, Susanne; Pirjola, Liisa; Hussein, Tareq

    2016-04-01

    This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of two organic vapors, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from -76 to +64 %. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of condensation and

  6. A Study on the Aqueous Formation of Secondary Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Sinclair, K.; Tsigaridis, K.

    2013-12-01

    The effect aerosols have on radiative forcing in the atmosphere is recognized as one of the largest uncertainties in the radiation budget. About 80% of organic aerosol mass in the atmosphere is estimated to be created though secondary processes. Recently, the aqueous formation of secondary organic aerosols (SOA) has become recognized as important when considering the source, transformation and radiative impacts of SOA. This work focuses on implementing a mechanism for aqueous SOA formation that can be used in atmospheric chemistry and models of all scales, from box to global. A box model containing a simplified chemical mechanism for the aqueous production of precursors of aqueous SOA (Myriokefalitakis et al. (2011) is coupled to gas-phase chemistry which uses the carbon bond mechanism (CBM) IV is presented. The model implements aqueous chemistry of soluble gases, both in-cloud and aerosol water, including organic compounds such as glyoxal and methylglyoxal, which have been shown as potentially significant sources for dissolved secondary organic aerosols. This mechanism implements aqueous phase mass transfer and molecular dissociation. The model's performance is evaluated against previous box model studies from the literature. A comparison is conducted between the detailed GAMMA model (McNeill et al., 2012), which is constrained with chamber experiments and the one developed here. The model output under different atmospheric conditions is explored and differences and sensitivities are assessed. The objective of this work is to create a robust framework for simulating aqueous phase formation of SOA and maximizing the computational efficiency of the model, while maintaining accuracy, in order to later use the exact mechanism in global climate simulations.

  7. Cloud water and aerosol studies in a background marine environment

    NASA Astrophysics Data System (ADS)

    Gioda, A.; Mayol-Bracero, O. L.; Reyes-Rodriguez, G.; Santos-Figueroa, G.; Morales-de Jesus, R.; Collett, J.; Decesari, S.; de Aquino Neto, F. R.; Klaus, C.; Bezerra, H.

    2007-12-01

    The study of aerosol and cloud water chemical composition is essential to understand cloud processing of different compounds, determining which species are more efficiently removed and which ones stay longer in the atmosphere and, therefore, are more important for aerosol climate forcing. As part of the Rain In Cumulus over the Ocean Experiment (RICO), cloud water and aerosol samples were collected in Puerto Rico. We present concentrations of water-soluble ions, total and dissolved organic carbon (TOC and DOC), total nitrogen (TN), and the speciation of nitrogen compounds (amino acids) for water and aerosol samples collected at East Peak and Cape San Juan, Puerto Rico. Mass and elemental/organic carbon (EC, OC) concentrations were also determined for the aerosol samples. The results show average concentrations of TOC and TN in cloud water of about 1.1 mg/L and for DOC about 0.9 mg/L. The DOC/TOC ratio averaged 0.78, indicating that most of the organic compounds present are dissolved in the cloud water. TOC was composed mainly of organic acids (47 percent) and TN of inorganic species (80 percent). With respect to the aerosol samples, the average mass concentration of fine particles (Dp < 1.7 um) was 2.4 ug/m3. EC was found at low-to-non detectable levels (< 0.5 ng/m3). The concentrations of OC, DOC, TOC, and TN ranged from 30 to 100 ng/m3. The size distributions showed that OC and TN were mainly present in the fine particle fractions (Dp < 1 um). The predominant ions for both cloud and aerosol samples were Cl- and Na+, the primary components of sea salt. However, when air masses arrived from Northwest Africa or from islands upwind of Puerto Rico there was a decrease in Na+ and Cl- concentrations and an increase in SO42-, NH3+ and Ca2+ concentrations, likely reflecting anthropogenic and crustal sources of these species. Overall, the average concentrations of all species are similar to those typically found in background (remote) environments; however, these

  8. Ozone, Iodine, and MSA - Case studies in Antarctic aerosol composition from the 2ODIAC Campaign

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Kalnajs, L.; Deshler, T.; Davis, S. M.; Johnson, A.; Slater, A. G.; Goetz, J. D.; Mukherjee, A. D.; DeCarlo, P. F.

    2015-12-01

    Aerosol generation and transport over the Polar Regions, and especially Antarctica, remains a source of uncertainty for geophysical scientists. A characterization of aerosol sources, production, and lifecycle processes in the Polar Regions is required to better understand the polar atmosphere. In an attempt to better characterize Antarctic aerosol and trace gas interactions, the Two-Season, Ozone Depletion and Interaction with Aerosols Campaign (2ODIAC) was launched over the Austral Spring/Summer of 2014 and Austral Winter of 2015. One highlight of the campaign is the first ever deployment of a high-resolution aerosol mass spectrometer to Antarctica. In conjunction with trace gas, meteorology, and aerosol sizing measurements, this presentation will focus on case studies from the campaign relevant to the atmospheric science community. Questions about the role of iodine, MSA, and ozone depletion events in regards to aerosol composition will be examined. Specific attention will be paid to aerosol compositional changes before, during, and after particle bursts especially where changes in aerosol sulfate oxidation occurred (SO2 -> SO4)

  9. Optical closure study on light-absorbing aerosols

    NASA Astrophysics Data System (ADS)

    Petzold, Andreas; Bundke, Ulrich; Freedman, Andrew; Onasch, Timothy B.; Massoli, Paola; Andrews, Elizabeth; Hallar, Anna G.

    2014-05-01

    The in situ measurement of atmospheric aerosol optical properties is an important component of quantifying climate change. In particular, the in-situ measurement of the aerosol single-scattering albedo (SSA), which is the ratio of aerosol scattering to aerosol extinction, is identified as a key challenge in atmospheric sciences and climate change research. Ideally, the complete set of aerosol optical properties is measured through optical closure studies which simultaneous measure aerosol extinction, scattering and absorption coefficients. The recent development of new optical instruments have made real-time in situ optical closure studies attainable, however, many of these instruments are state-of-the-art but not practical for routine monitoring. In our studies we deployed a suit of well-established and recently developed instruments including the cavity attenuated phase shift (CAPS) method for aerosol light extinction, multi-angle absorption photometer (MAAP) and particle soot absorption photometer (PSAP) for aerosol light absorption, and an integrating nephelometer (NEPH) for aerosol light scattering measurements. From these directly measured optical properties we calculated light absorption from extinction minus scattering (difference method), light extinction from scattering plus absorption, and aerosol single-scattering albedo from combinations CAPS + MAAP, NEPH + PSAP, NEPH + MAAP, CAPS + NEPH. Closure studies were conducted for laboratory-generated aerosols composed of various mixtures of black carbon (Regal 400R pigment black, Cabot Corp.) and ammonium sulphate, urban aerosol (Billerica, MA), and background aerosol (Storm Peak Lab.). Key questions addressed in our closure studies are: (1) how well can we measure aerosol light absorption by various methods, and (2) how well can we measure the aerosol single-scattering albedo by various instrument combinations? In particular we investigated (3) whether the combination of a CAPS and NEPH provides a reasonable

  10. Light Scattering Study of Titania Aerosols

    NASA Astrophysics Data System (ADS)

    Oh, Choonghoon; Sorensen, Chris

    1997-03-01

    We studied the fractal morphology of titania aerosols by light scattering. Titania aerosols were generated by the thermal decomposition of titanium tetraisopropoxide (TTIP) in a silica tube furnace. TTIP was evaporated at temperatures up to 80^circC and its vapor was carried by dry nitrogen to a furnace with temperature in the range of 400 - 600^circC. A TEM analysis of the generated particles showed a typical DLCA structure with a monomer diameter about 50 nm. The particles were then made to flow through a narrow outlet as a laminar stream. The light scattering from these particles was measured using a He-Ne laser as a light source. The measured structure factor clearly showed the Rayleigh, Guinier, and fractal regimes. The fractal morphological parameters, such as the cluster radius of gyration, the fractal dimension, and the fractal prefactor were studied from the structure factor as a function of particle generation conditions. The cluster radius of gyration was about 1 μm and showed a modest dependency on the generation conditions. The fractal dimension was about 1.7 in all cases. These results are in good agreement with the TEM analysis.

  11. Remote sensing for studying atmospheric aerosols in Malaysia

    NASA Astrophysics Data System (ADS)

    Kanniah, Kasturi D.; Kamarul Zaman, Nurul A. F.

    2015-10-01

    The aerosol system is Southeast Asia is complex and the high concentrations are due to population growth, rapid urbanization and development of SEA countries. Nevertheless, only a few studies have been carried out especially at large spatial extent and on a continuous basis to study atmospheric aerosols in Malaysia. In this review paper we report the use of remote sensing data to study atmospheric aerosols in Malaysia and document gaps and recommend further studies to bridge the gaps. Satellite data have been used to study the spatial and seasonal patterns of aerosol optical depth (AOD) in Malaysia. Satellite data combined with AERONET data were used to delineate different types and sizes of aerosols and to identify the sources of aerosols in Malaysia. Most of the aerosol studies performed in Malaysia was based on station-based PM10 data that have limited spatial coverage. Thus, satellite data have been used to extrapolate and retrieve PM10 data over large areas by correlating remotely sensed AOD with ground-based PM10. Realising the critical role of aerosols on radiative forcing numerous studies have been conducted worldwide to assess the aerosol radiative forcing (ARF). Such studies are yet to be conducted in Malaysia. Although the only source of aerosol data covering large region in Malaysia is remote sensing, satellite observations are limited by cloud cover, orbital gaps of satellite track, etc. In addition, relatively less understanding is achieved on how the atmospheric aerosol interacts with the regional climate system. These gaps can be bridged by conducting more studies using integrated approach of remote sensing, AERONET and ground based measurements.

  12. Developing a stronger understanding of aerosol sources and the impact of aqueous phase processing on coastal air quality

    NASA Astrophysics Data System (ADS)

    Prather, K. A.

    2014-12-01

    Atmospheric aerosols are produced by a variety of sources including emissions from cars and trucks, wildfires, ships, dust, and sea spray and play a significant role in impacting air pollution and regional climate. The ability of an aerosol to uptake water and undergo aqueous phase processing strongly depends on composition. On-line single particle mass spectrometry can provide insight into how particle composition impacts the degree of photochemical and aging processes atmospheric aerosols undergo. In particular, specific sulfur species including sulfate, hydroxymethanesulfate (HMS), and methanesulfonic acid (MSA) can serve as indicators of when an air mass has undergone aqueous phase processing. This presentation will describe recent field studies conducted at coastal sites to demonstrate how different aerosol sources and secondary processing impact coastal air quality.

  13. On the Feasibility of Studying Shortwave Aerosol Radiative Forcing of Climate Using Dual-Wavelength Aerosol Backscatter Lidar

    NASA Technical Reports Server (NTRS)

    Redemann, Jens; Russell, Philip B.; Winker, David M.; McCormick, M. Patrick; Hipskind, R. Stephen (Technical Monitor)

    2000-01-01

    The current low confidence in the estimates of aerosol-induced perturbations of Earth's radiation balance is caused by the highly non-uniform compositional, spatial and temporal distributions of tropospheric aerosols on a global scale owing to their heterogeneous sources and short lifetimes. Nevertheless, recent studies have shown that the inclusion of aerosol effects in climate model calculations can improve agreement with observed spatial and temporal temperature distributions. In light of the short lifetimes of aerosols, determination of their global distribution with space-borne sensors seems to be a necessary approach. Until recently, satellite measurements of tropospheric aerosols have been approximate and did not provide the full set of information required to determine their radiative effects. With the advent of active aerosol remote sensing from space (e.g., PICASSO-CENA), the applicability fo lidar-derived aerosol 180 deg -backscatter data to radiative flux calculations and hence studies of aerosol effects on climate needs to be investigated.

  14. Extending "Deep Blue" aerosol retrieval coverage to cases of absorbing aerosols above clouds: Sensitivity analysis and first case studies

    NASA Astrophysics Data System (ADS)

    Sayer, A. M.; Hsu, N. C.; Bettenhausen, C.; Lee, J.; Redemann, J.; Schmid, B.; Shinozuka, Y.

    2016-05-01

    Cases of absorbing aerosols above clouds (AACs), such as smoke or mineral dust, are omitted from most routinely processed space-based aerosol optical depth (AOD) data products, including those from the Moderate Resolution Imaging Spectroradiometer (MODIS). This study presents a sensitivity analysis and preliminary algorithm to retrieve above-cloud AOD and liquid cloud optical depth (COD) for AAC cases from MODIS or similar sensors, for incorporation into a future version of the "Deep Blue" AOD data product. Detailed retrieval simulations suggest that these sensors should be able to determine AAC AOD with a typical level of uncertainty ˜25-50% (with lower uncertainties for more strongly absorbing aerosol types) and COD with an uncertainty ˜10-20%, if an appropriate aerosol optical model is known beforehand. Errors are larger, particularly if the aerosols are only weakly absorbing, if the aerosol optical properties are not known, and the appropriate model to use must also be retrieved. Actual retrieval errors are also compared to uncertainty envelopes obtained through the optimal estimation (OE) technique; OE-based uncertainties are found to be generally reasonable for COD but larger than actual retrieval errors for AOD, due in part to difficulties in quantifying the degree of spectral correlation of forward model error. The algorithm is also applied to two MODIS scenes (one smoke and one dust) for which near-coincident NASA Ames Airborne Tracking Sun photometer (AATS) data were available to use as a ground truth AOD data source, and found to be in good agreement, demonstrating the validity of the technique with real observations.

  15. Extending "Deep Blue" Aerosol Retrieval Coverage to Cases of Absorbing Aerosols Above Clouds: Sensitivity Analysis and First Case Studies

    NASA Technical Reports Server (NTRS)

    Sayer, A. M.; Hsu, N. C.; Bettenhausen, C.; Lee, J.; Redemann, J.; Schmid, B.; Shinozuka, Y.

    2016-01-01

    Cases of absorbing aerosols above clouds (AACs), such as smoke or mineral dust, are omitted from most routinely processed space-based aerosol optical depth (AOD) data products, including those from the Moderate Resolution Imaging Spectroradiometer (MODIS). This study presents a sensitivity analysis and preliminary algorithm to retrieve above-cloud AOD and liquid cloud optical depth (COD) for AAC cases from MODIS or similar sensors, for incorporation into a future version of the "Deep Blue" AOD data product. Detailed retrieval simulations suggest that these sensors should be able to determine AAC AOD with a typical level of uncertainty approximately 25-50 percent (with lower uncertainties for more strongly absorbing aerosol types) and COD with an uncertainty approximately10-20 percent, if an appropriate aerosol optical model is known beforehand. Errors are larger, particularly if the aerosols are only weakly absorbing, if the aerosol optical properties are not known, and the appropriate model to use must also be retrieved. Actual retrieval errors are also compared to uncertainty envelopes obtained through the optimal estimation (OE) technique; OE-based uncertainties are found to be generally reasonable for COD but larger than actual retrieval errors for AOD, due in part to difficulties in quantifying the degree of spectral correlation of forward model error. The algorithm is also applied to two MODIS scenes (one smoke and one dust) for which near-coincident NASA Ames Airborne Tracking Sun photometer (AATS) data were available to use as a ground truth AOD data source, and found to be in good agreement, demonstrating the validity of the technique with real observations.

  16. Study of Aerosol/Cloud/Radiation Interactions over the ARM SGP Site

    SciTech Connect

    Chuang, C; Chin, S

    2006-03-14

    While considerable advances in the understanding of atmospheric processes and feedbacks in the climate system have led to a better representation of these mechanisms in general circulation models (GCMs), the greatest uncertainty in predictability of future climate arises from clouds and their interactions with radiation. To explore this uncertainty, cloud resolving model has been evolved as one of the main tools for understanding and testing cloud feedback processes in climate models, whereas the indirect effects of aerosols are closely linked with cloud feedback processes. In this study we incorporated an existing parameterization of cloud drop concentration (Chuang et al., 2002a) together with aerosol prediction from a global chemistry/aerosol model (IMPACT) (Rotman et al., 2004; Chuang et al., 2002b; Chuang et al., 2005) into LLNL cloud resolving model (Chin, 1994; Chin et al., 1995; Chin and Wilhelmson, 1998) to investigate the effects of aerosols on cloud/precipitation properties and the resulting radiation fields over the Southern Great Plains.

  17. Air pollution and asthma: clinical studies with sulfuric acid aerosols

    SciTech Connect

    Utell, M.J.; Frampton, M.W.; Morrow, P.E. )

    1991-11-01

    Until recently, acid deposition has been widely considered a serious ecological problem but not a threat to human health. The controlled clinical study is an important approach in linking acidic aerosol inhalation with respiratory effects. Asthmatic patients represent a subpopulation most responsive to sulfuric acid aerosols. In a series of studies with asthmatic volunteers, several factors have been identified that may modulate the intensity of the bronchoconstrictor response to inhaled acidic aerosols. We found (1) enhancement of the bronchoconstrictor response during exercise, (2) the more acidic aerosols provoke the greatest changes in lung function, and (3) mitigation of airway responses during sulfuric acid aerosol inhalation caused by high respiratory ammonia concentrations. Additional factors influencing responsiveness await identification.

  18. Spectroscopic studies of the size and composition of single aerosol droplets

    NASA Astrophysics Data System (ADS)

    Reid, Jonathan P.; Meresman, Helena; Mitchem, Laura; Symes, Rachel

    The characterization of aerosol properties and processes, non-intrusively and directly, poses a severe analytical challenge. In order to understand the role of aerosols in often complex environments, it is necessary to probe the particles in situ and without perturbation. Sampling followed by end-of-line analysis can lead to perturbations in particle composition, morphology and size, particularly when analysing liquid aerosol droplets containing volatile components. Optical spectroscopy can provide a strategy for the direct assessment of particle size, composition and phase. We review here the application of linear and non-linear Raman spectroscopies in the characterization of liquid aerosol droplets. Spontaneous Raman scattering can allow the unambiguous identification of chemical components and the determination of droplet composition. Stimulated Raman spectroscopy can allow the determination of droplet size with nanometre accuracy and can allow the characterization of near-surface composition. When combined, the mixing state and homogeneity in droplet composition can be investigated. We highlight some applications of these spectroscopic techniques in studies of the kinetics of particle transformation, the equilibrium composition of aqueous aerosol droplets, and the coagulation and mixing state of organic and aqueous aerosol components. Specifically, we examine the heat and mass transfer accompanying the evaporation of volatile components from liquid droplets, the equilibrium size of aqueous/sodium chloride droplets with varying relative humidity, and the mixing of the immiscible decane and water components during droplet coagulation. We conclude by considering the potential of these techniques for improving our understanding of aerosol properties and processes.

  19. Low-temperature Bessel beam trap for single submicrometer aerosol particle studies

    SciTech Connect

    Lu, Jessica W.; Chasovskikh, Egor; Stapfer, David; Isenor, Merrill; Signorell, Ruth

    2014-09-01

    We report on a new instrument for single aerosol particle studies at low temperatures that combines an optical trap consisting of two counter-propagating Bessel beams (CPBBs) and temperature control down to 223 K (−50 °C). The apparatus is capable of capturing and stably trapping individual submicrometer- to micrometer-sized aerosol particles for up to several hours. First results from studies of hexadecane, dodecane, and water aerosols reveal that we can trap and freeze supercooled droplets ranging in size from ∼450 nm to 5500 nm (radius). We have conducted homogeneous and heterogeneous freezing experiments, freezing-melting cycles, and evaporation studies. To our knowledge, this is the first reported observation of the freezing process for levitated single submicrometer-sized droplets in air using optical trapping techniques. These results show that a temperature-controlled CPBB trap is an attractive new method for studying phase transitions of individual submicrometer aerosol particles.

  20. THE DETROIT EXPOSURE AND AEROSOL RESEARCH STUDY (DEARS)

    EPA Science Inventory

    Field data collections for the Detroit Exposure and Aerosol Research Study (DEARS) have completed one-half of the planned study design. The DEARS is collecting personal, residential indoor, residential outdoor and central community monitoring data involving particulate matter, v...

  1. Molecular dynamics studies of organic-coated nano aerosols

    NASA Astrophysics Data System (ADS)

    Chakraborty, Purnendu

    2008-10-01

    Atmospheric aerosols play an important role in atmospheric processes. These aerosol particles can affect climate through scattering, transmission and absorption of radiation as well as acting as cloud condensation nuclei. It has recently been found that fatty acids reside on the surfaces of marine and continental aerosols. In this research, an attempt has been made to understand the structures and properties of such organic coated aerosols using Molecular Dynamics simulation. The model particle consisted of a water droplet coated with fatty acid. The density profile (using both Coarse-Grained and Atomistic/United atom models) demonstrated that such aerosol particles have an inverted micelle structure consisting of an aqueous core and with the hydrophobic hydrocarbon tails exposed to the atmosphere. For smaller chains, with the organic molecules directed radially outwards from the water---organic interface) the normal pressure profile showed that the organic coating is under tension resulting in a 'negative' surface tension. As a result, such particles would have an inverse Kelvin vapor pressure effect and would be able to process water vapor despite the hydrophobic surface. Following the work on surface tension, the rate of water uptake by coated aerosols was computed. It was found that the sticking coefficient of water vapor on such particles was about a sixth of that on pure water droplets. This may seem to imply that the net condensation rate is lower, but we also need to take into account the evaporation of water from such particles. With a significant reduction in the evaporation rate (the coating lends greater stability to the particle resulting in reduced evaporation rate), the equilibrium vapor pressure of water on such particles reduced, resulting in a "net water attractor". Thus if such structures were created in sufficient concentration, they might be important contributors in the cloud condensation process. Next the effect of longer Fatty acid molecules

  2. Generation and delivery of coal liquid aerosols for inhalation studies

    SciTech Connect

    Springer, D.L.; Clark, M.L.; Willard, D.H.; Mahlum, D.D.

    1982-07-01

    To aid in the toxicologic evaluation of solvent refined coal (SRC) materials, we developed an aerosol generation system for whole-body inhalation exposure of experimental animals to coal liquids. The main components of the exposure system were an aerosol generator, a manifold for delivery of the aerosol, three exposure chambers and an exhaust system. High-boiling coal liquids from the SRC-l and the SRC-ll processes were as test materials. Aerosol concentrations were measured by drawing aerosol samples from the chambers through a Metricel filter and eluting the coal liquid into chloroform.Since these coal liquids have an ultraviolet absorption peak at 254 mm, the absorbance was determined at this wavelength. As part of the experiment, we evaluated the Solo-Sphere, Rec and Collison neubulizer as aerosol generators for the coal liquids. Both the Solo-Sphere and Retec provided adequate concentrations of respirable particles; however, aerosol concentrations within the exposure chamber provided adequate concentrations of respirable particles; however, aerosol concentrations within the exposure chamber were more consistent with the Solo-Sphere. Low mass output and plugging were encountered with the Collison. Use of the Solo-Sphere generator and manifold delivery system resulted in consistent and uniform aerosol concentrations and particle sizes in the exposure chamber over a 15-day test period. Analysis of the chamber atmosphere when SRC-l process solvent was used indicated the presence of vapors as well as particles. The ultraviolet absorption spectrum suggested that two-ring polynuclear aromatic compounds were the major constituents of the vapor phase.

  3. A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

    NASA Technical Reports Server (NTRS)

    Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

    2010-01-01

    Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

  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.

    2014-06-01

    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

  5. Artificial ultra-fine aerosol tracers for highway transect studies

    NASA Astrophysics Data System (ADS)

    Cahill, Thomas A.; Barnes, David E.; Wuest, Leann; Gribble, David; Buscho, David; Miller, Roger S.; De la Croix, Camille

    2016-07-01

    The persistent evidence of health impacts of roadway aerosols requires extensive information for urban planning to avoid putting populations at risk, especially in-fill projects. The required information must cover both highway aerosol sources as well as transport into residential areas under a variety of roadway configurations, traffic conditions, downwind vegetation, and meteorology. Such studies are difficult and expensive to do, but were easier in the past when there was a robust fine aerosol tracer uniquely tied to traffic - lead. In this report we propose and test a modern alternative, highway safety flare aerosols. Roadway safety flares on vehicles in traffic can provide very fine and ultra-fine aerosols of unique composition that can be detected quantitatively far downwind of roadways due to a lack of upwind interferences. The collection method uses inexpensive portable aerosol collection hardware and x-ray analysis protocols. The time required for each transect is typically 1 h. Side by side tests showed precision at ± 4%. We have evaluated this technique both by aerosol removal in vegetation in a wind tunnel and by tracking aerosols downwind of freeways as a function of season, highway configuration and vegetation coverage. The results show that sound walls for at-grade freeways cause freeway pollution to extend much farther downwind than standard models predict. The elevated or fill section freeway on a berm projected essentially undiluted roadway aerosols at distances well beyond 325 m, deep into residential neighborhoods. Canopy vegetation with roughly 70% cover reduced very fine and ultra-fine aerosols by up to a factor of 2 at distances up to 200 m downwind.

  6. UV Studies of Jupiter's Aerosols and Hydrocarbons

    NASA Technical Reports Server (NTRS)

    Pryor, Wayne

    2004-01-01

    This project funded research related to our involvement in the Galileo Ultraviolet Spectrometer experiment. Pryor was a Co-I on that experiment, which recently ended when Galileo crashed into Jupiter's atmosphere. It also funded related research on HST observations of Jupiter's atmosphere, and Cassini observations of Jupiter's atmosphere, and ground-based studies of Jupiter's atmosphere using the facilities of McDonald Observatory. Specific activities related to this grant include study of UV spectra returned by Galileo UVS and Cassini UVIS, development of simple models to explain these spectra, participation in archiving activities for these data sets, travel to conferences, and publication of scientific papers. Highlights of our Jupiter research efforts include: 1.) evidence for heavy hydrocarbons in Jupiter's atmosphere (from HST) (Clarke et al. poster), that may be the source of Jupiter's stratospheric aerosols, 2.) detection of auroral flares in Jupiter's atmosphere from Galileo (Pryor et al., 2001). 3.) establishing a connection between coronal mass ejections and auroral outbursts (Gurnett et al., 2002), and 4) establishing a connection between short-term variations in Jupiter's auroral emissions and radio emissions (Pryor et al. presented at AGU in 2002, paper in preparation).

  7. São Paulo aerosol characterization study.

    PubMed

    Alonso, C D; Martins, M H; Romano, J; Godinho, R

    1997-12-01

    The São Paulo Metropolitan area (SPMA) is characterized as having one of the worst air pollution problems in Brazil, with frequent violations of air quality standards for particulate matter. This paper presents the results of a receptor model source apportionment study carried out to develop a quantitative database on which a control strategy could be developed. The study was conducted in four sites with distinct land uses. Fine, coarse (CP), and total suspended particles (TSP) samples were collected on Teflon and glass filters and analyzed by x-ray fluorescence (XRF), ion chromatography, and thermal evolution. The sources were characterized by similar methodology. Chemical mass balance (CMB) receptor modeling indicated that carbonaceous material plays an important role in the aerosol composition; that the three major source categories contributing to the fine particles are vehicles, secondary carbon, and sulfates; and that the main contributors to CP and TSP are road dust and vehicles. All sampling sites presented the same general pattern in terms of source contribution, although this contribution varied from site to site.

  8. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    NASA Technical Reports Server (NTRS)

    Zaveri, R. A.; Shaw, W. J.; Cahill, J. F.; Cairns, Brian; Cappa, C. D.; Ottaviani, Matteo; Cziczo, D. J.; Ferrare, Richard A.; Alexander, M. L.; Alexandrov, Mikhail Dmitrievic; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Schmid, B.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Flowers, B. A.; Fortner, E.; Baidar, S.; Hair, J.; Hostetler, C.; Obland, M. D.; Rogers, R. R.; Floerchinger, C.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.

    2012-01-01

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climaterelated properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data

  9. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    SciTech Connect

    Zaveri, Rahul A.; Shaw, William J.; Cziczo, D. J.; Schmid, Beat; Ferrare, R.; Alexander, M. L.; Alexandrov, Mikhail; Alvarez, R. J.; Arnott, W. P.; Atkinson, D.; Baidar, Sunil; Banta, Robert M.; Barnard, James C.; Beranek, Josef; Berg, Larry K.; Brechtel, Fred J.; Brewer, W. A.; Cahill, John F.; Cairns, Brian; Cappa, Christopher D.; Chand, Duli; China, Swarup; Comstock, Jennifer M.; Dubey, Manvendra K.; Easter, Richard C.; Erickson, Matthew H.; Fast, Jerome D.; Floerchinger, Cody; Flowers, B. A.; Fortner, Edward; Gaffney, Jeffrey S.; Gilles, Mary K.; Gorkowski, K.; Gustafson, William I.; Gyawali, Madhu S.; Hair, John; Hardesty, Michael; Harworth, J. W.; Herndon, Scott C.; Hiranuma, Naruki; Hostetler, Chris A.; Hubbe, John M.; Jayne, J. T.; Jeong, H.; Jobson, Bertram T.; Kassianov, Evgueni I.; Kleinman, L. I.; Kluzek, Celine D.; Knighton, B.; Kolesar, K. R.; Kuang, Chongai; Kubatova, A.; Langford, A. O.; Laskin, Alexander; Laulainen, Nels S.; Marchbanks, R. D.; Mazzoleni, Claudio; Mei, F.; Moffet, Ryan C.; Nelson, Danny A.; Obland, Michael; Oetjen, Hilke; Onasch, Timothy B.; Ortega, Ivan; Ottaviani, M.; Pekour, Mikhail S.; Prather, Kimberly A.; Radney, J. G.; Rogers, Ray; Sandberg, S. P.; Sedlacek, Art; Senff, Christoph; Senum, Gunar; Setyan, Ari; Shilling, John E.; Shrivastava, ManishKumar B.; Song, Chen; Springston, S. R.; Subramanian, R.; Suski, Kaitlyn; Tomlinson, Jason M.; Volkamer, Rainer M.; Wallace, Hoyt A.; Wang, J.; Weickmann, A. M.; Worsnop, Douglas R.; Yu, Xiao-Ying; Zelenyuk, Alla; Zhang, Qi

    2012-08-22

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and 'aged' urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: a) the scientific background and motivation for the study, b) the operational and logistical information pertinent to the execution of the study, c) an overview of key observations and initial results from the aircraft and ground-based sampling platforms, and d) a roadmap of planned data

  10. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    SciTech Connect

    Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Ferrare, R. A.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kassianov, E. I.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Kubátová, A.; Langford, A. O.; Laskin, A.; Laulainen, N.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Suski, K.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Worsnop, D. R.; Yu, X. -Y.; Zelenyuk, A.; Zhang, Q.

    2012-01-01

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program’s Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites – one within the Sacramento urban area and another about 40 km to the northeast in the foothills area – were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and “aged” urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: a) the scientific background and motivation for the study, b) the operational and logistical information pertinent to the execution of the study, c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and d) a roadmap of

  11. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    NASA Astrophysics Data System (ADS)

    Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Ferrare, R. A.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kassianov, E. I.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Kubátová, A.; Langford, A. O.; Laskin, A.; Laulainen, N.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Suski, K.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Worsnop, D. R.; Yu, X.-Y.; Zelenyuk, A.; Zhang, Q.

    2012-08-01

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data

  12. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    NASA Astrophysics Data System (ADS)

    Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Langford, A. O.; Laskin, A.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Yu, X.-Y.; Zelenyuk, A.; Zhang, Q.

    2012-01-01

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial results from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data

  13. Formation and Processing of Secondary Organic Aerosol from Catechol as a Model for Atmospheric HULIS

    NASA Astrophysics Data System (ADS)

    Ofner, Johannes; Krüger, Heinz-Ulrich; Grothe, Hinrich; Zetzsch, Cornelius

    2010-05-01

    A particular fraction of the secondary organic aerosol (SOA) termed HUmic Like Substances (HULIS) attracted attention only recently in atmospheric aerosol, initiating a discourse about their aromaticity and other properties, such as reactivity and hygroscopicity. A major portion of HULIS originates from volatile organic compounds, which are formed by abiotic oxidation reactions involving mainly OH radicals, ozone, nitrogen oxides and possibly halogens. Subsequently, the particles provide surface for heterogeneous reactions with atmospheric trace gases. Thus, aerosol smog-chamber studies with appropriate precursors are needed to generate SOA with HULIS qualities in situ inside the smog chamber and study their possible interactions. Catechol and guaiacol were chosen as aromatic precursors for synthetic HULIS production. The SOA was produced in a 700 L aerosol smog chamber, equipped with a solar simulator. SOA formation from each precursor was investigated at simulated environmental conditions (humidity, light, and presence of oxidizers) and characterized with respect to HULIS properties by particle classifiers, Fourier Transform IR spectroscopy (by long-path absorption and attenuated total reflection), UV/VIS spectroscopy, high-resolution mass-spectroscopy and temperature-programmed-desorption mass-spectrometry. High-resolution imaging was obtained using Field Emission Gun Scanning Electron Microscopy (FEGSEM). After HULIS formation the aerosol particles were exposed to atmospheric halogen species to study their processing with those trace gases, released by sea salt-activation. Those investigations show that aromatic precursors like catechol and guaiacol are suitable to form synthetic HULIS for laboratory-scale measurements with physical and chemical properties described in literature. However, sunlight and relative humidity play a major role in particle production and composition of functional groups, which are the anchor points for heterogeneous atmospheric

  14. Atmospheric pressure flow reactor / aerosol mass spectrometer studies of tropospheric aerosol nucleat and growth kinetics. Final report, June, 2001

    SciTech Connect

    Worsnop, Douglas R.

    2001-06-01

    The objective of this program was to determine the mechanisms and rates of growth and transformation and growth processes that control secondary aerosol particles in both the clear and polluted troposphere. The experimental plan coupled an aerosol mass spectrometer (AMS) with a chemical ionization mass spectrometer to provide simultaneous measurement of condensed and particle phases. The first task investigated the kinetics of tropospheric particle growth and transformation by measuring vapor accretion to particles (uptake coefficients, including mass accommodation coefficients and heterogeneous reaction rate coefficients). Other work initiated investigation of aerosol nucleation processes by monitoring the appearance of submicron particles with the AMS as a function of precursor gas concentrations. Three projects were investigated during the program: (1) Ozonolysis of oleic acid aerosols as model of chemical reactivity of secondary organic aerosol; (2) Activation of soot particles by measurement deliquescence in the presence of sulfuric acid and water vapor; (3) Controlled nucleation and growth of sulfuric acid aerosols.

  15. An Overview of the 2010 Carbonaceous Aerosol and Radiative Effects Study (CARES) Field Campaign

    NASA Astrophysics Data System (ADS)

    Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.

    2010-12-01

    The primary objective of the DOE Carbonaceous Aerosol and Radiative Effects Study (CARES) in June 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume. Carbonaceous aerosol components, which include black carbon (BC), urban primary organic aerosols (POA), biomass burning aerosols, and secondary organic aerosols (SOA) from both urban and biogenic precursors, have been shown to play a major role in the direct and indirect radiative forcing of climate. However, significant knowledge gaps and uncertainties still exist in the process-level understanding of: 1) SOA formation, 2) BC mixing state evolution, and 3) the optical and hygroscopic properties of fresh and aged carbonaceous aerosols. The CARES 2010 field study was designed to address several specific science questions under these three topics. During summer the Sacramento-Blodgett Forest corridor effectively serves as a mesoscale daytime flow reactor in which the urban aerosols undergo significant aging as they are transported to the northeast by upslope flow. The CARES campaign observation strategy consisted of the DOE G-1 aircraft sampling upwind, within, and outside of the evolving Sacramento urban plume in the morning and again in the afternoon. The G-1 payload consisted of a suite of instruments to measure trace gases, aerosol size distribution, composition, and optical properties. The NASA B-200 aircraft carrying a High Spectral Resolution Lidar (HSRL) and a Research Scanning Polarimeter (RSP) was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties. The aircraft measurements were complemented by heavily-instrumented ground sites within the Sacramento urban area and at a downwind site in Cool, California, to characterize the diurnal evolution of meteorological variables, trace gases, aerosol precursors, aerosol

  16. Study of the CCN formation as a function of aerosol components

    NASA Astrophysics Data System (ADS)

    Fanourgakis, George S.; Myriokefalitakis, Stelios; Kanakidou, Maria

    2016-04-01

    Understanding the role of aerosols in Earth's climate through direct and indirect effects has attracted a lot of attention over the last years. Due to the chemical complexity of aerosols along with the variety of the primary emissions sources and the conversions from gas to particle in atmosphere, accurate predictions for the aerosols impact on a regional and global scale still remains a challenging problem. In this study, we examine the relative contribution of directly emitted particles in the atmosphere (primary particles) and particles formed from gas-to-particle conversion (secondary particles) to the global aerosols and to the cloud condensation nuclei (CCN) formation. The Chemistry Transport Model v4.0 (TM4-ECPL) coupled with an extended version of the aerosol micro-physics model M7, which describes microphysical processes (nucleation, coagulation, condensation of gas-phase species) for sulfate, black carbon, organic carbon sea salt, dust and various secondary organic aerosols, is here used. A systematic analysis on the CCN production as a function of the aerosol chemical composition is performed. The sensitivity of the results to physical parameters that affect the CCN formation and cannot be accurately determined, such as hygroscopicity, is investigated based on a detailed sensitivity analysis. This work has been supported by the European FP7 collaborative project BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding).

  17. Aerosol analysis for the regional air pollution study. Final report

    SciTech Connect

    Jaklevic, J.M.; Gatti, R.C.; Goulding, F.S.; Loo, B.W.; Thompson, A.C.

    1980-05-01

    The design and operation of an aerosol sampling and analysis program implemented during the 1975 to 1977 St. Louis Regional Air Pollution Study is described. A network of ten samplers were operated at selected sites in the St. Louis area and the total mass and elemental composition of the collected particulates were determined. Sampling periods of 2 to 24 hours were employed. The samplers were capable of collecting aerosol particles in two distinct size ranges corresponding to fine (< 2.4 ..mu..m diameter) and coarse (> 2.4 ..mu..m diameter) particles. This unique feature allowed the separation of the particulate samples into two distinct fractions with differing chemical origins and health effects. The analysis methods were also newly developed for use in the St. Louis RAPS study. Total particulate mass was measured by a beta-particle attenuation method in which a precision of +- 5 ..mu..m/cm/sup 2/ could be obtained in a one minute measurement time. Elemental compositions of the samples were determined using an energy dispersive x-ray fluorescence method in which detectable limits of 5 ng/cm/sup 2/ or less were routinely achieved for elements ranging in atomic number from Al to Pb. The advantages of these analytical methods over more conventional techniques arise from the ability to automate the measurements. During the course of the two year study, a total of more than 35,000 individual samples were processed and a total of 28 concentrations measured for each sample.

  18. Study of fifteen respirable aerosol samplers used in occupational hygiene.

    PubMed

    Görner, P; Wrobel, R; Micka, V; Skoda, V; Denis, J; Fabriès, J F

    2001-01-01

    European and international standards lay down criteria for the size-selective aerosol sampling in occupational hygiene. Aerosol samplers are supposed to match these target sampling criteria. This study focused on 15 aerosol samplers used to sample the conventional respirable fraction. An aerodynamic particle sizer (APS) method was used to measure the sampling efficiency of the samplers in a low-velocity wind tunnel. Polydisperse coal dust was generated as the test aerosol. The data were fitted by an appropriate mathematical model. For some instruments the results show serious deviations from the conventional target curve, whereas other devices meet the convention quite well. The flow rate of certain cyclone-separator-based instruments was optimized to adjust their sampling efficiency. The mass concentration bias and accuracy of the samplers were calculated for a number of ranges of particle size distributions of aerosols commonly found in industrial workplaces. Finally, the performance of each sampler was evaluated using bias and accuracy maps. Most of these samplers are suitable for sampling the CEN-ISO-ACGIH respirable fraction of aerosols, but several require modification of the flow rate. For real industrial situations, the rough knowledge of the aerosol size distribution can guide the choice of an appropriate sampling technique.

  19. 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.

  20. 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.

  1. Fast Airborne Size Distribution Measurements of an Aerosol Processes and Aging

    NASA Astrophysics Data System (ADS)

    Kapustin, V.; Clarke, A. D.; Zhou, J.; Brekhovskikh, V.; McNaughton, C. S.; Howell, S.

    2009-12-01

    During MILAGRO/INTEX experiment the Hawaii Group for Environmental Aerosol Research (HIGEAR) deployed a wide range of aerosol instrumentation aboard NSF C-130 and NASA DC-8. These were designed to provide rapid information on aerosol composition, state of mixing (internal or external), spectral optical properties (scattering and absorption), the humidity dependence of light scattering - f(RH), and the role of condensed species in changing the absorption properties of black carbon (BC) and inferred properties of organic carbon (OC). We also flew the Fast Mobility Particle Spectrometer (FMPS, TSI Inc.) to measure aerosol size distributions in a range 5.6 - 560 nm. For all our flights around Mexico City, an aerosol number concentration usually was well above the nominal FMPS sensitivity (from ~100 particles/cc @ Dp = 5.6 nm to 1 part/cc @ 560nm), providing us with reliable size distributions even at 1 sec resolution. FMPS measurements revealed small scale structure of an aerosol and allowed us to examine size distributions varying over space and time associated with mixing processes previously unresolved. These 1-Hz measurements during aircraft profiles captured variations in size distributions within shallow layers. Other dynamic processes observed included orography induced aerosol layers and evolution of the nanoparticles formed by nucleation. We put FMPS high resolution size distribution data in a context of aerosol evolution and aging, using a range of established (for MIRAGE/INTEX) chemical, aerosol and transport aging parameters.

  2. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3 aerosol during the 2013 Southern Oxidant and Aerosol Study

    SciTech Connect

    Allen, H. M.; Draper, D. C.; Ayres, B. R.; Ault, A.; Bondy, A.; Takahama, S.; Modini, R. L.; Baumann, K.; Edgerton, E.; Knote, C.; Laskin, A.; Wang, B.; Fry, J. L.

    2015-09-25

    Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. In addition, calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3 is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3 and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.

  3. Generation and Characterization of Indoor Fungal Aerosols for Inhalation Studies

    PubMed Central

    Larsen, Søren T.; Koponen, Ismo K.; Kling, Kirsten I.; Barooni, Afnan; Karottki, Dorina Gabriela; Tendal, Kira; Wolkoff, Peder

    2016-01-01

    In the indoor environment, people are exposed to several fungal species. Evident dampness is associated with increased respiratory symptoms. To examine the immune responses associated with fungal exposure, mice are often exposed to a single species grown on an agar medium. The aim of this study was to develop an inhalation exposure system to be able to examine responses in mice exposed to mixed fungal species aerosolized from fungus-infested building materials. Indoor airborne fungi were sampled and cultivated on gypsum boards. Aerosols were characterized and compared with aerosols in homes. Aerosols containing 107 CFU of fungi/m3 air were generated repeatedly from fungus-infested gypsum boards in a mouse exposure chamber. Aerosols contained Aspergillus nidulans, Aspergillus niger, Aspergillus ustus, Aspergillus versicolor, Chaetomium globosum, Cladosporium herbarum, Penicillium brevicompactum, Penicillium camemberti, Penicillium chrysogenum, Penicillium commune, Penicillium glabrum, Penicillium olsonii, Penicillium rugulosum, Stachybotrys chartarum, and Wallemia sebi. They were all among the most abundant airborne species identified in 28 homes. Nine species from gypsum boards and 11 species in the homes are associated with water damage. Most fungi were present as single spores, but chains and clusters of different species and fragments were also present. The variation in exposure level during the 60 min of aerosol generation was similar to the variation measured in homes. Through aerosolization of fungi from the indoor environment, cultured on gypsum boards, it was possible to generate realistic aerosols in terms of species composition, concentration, and particle sizes. The inhalation-exposure system can be used to study responses to indoor fungi associated with water damage and the importance of fungal species composition. PMID:26921421

  4. Numerical studies of microphysical modulations of stratospheric aerosol within ROMIC-ROSA

    NASA Astrophysics Data System (ADS)

    Hommel, René; von Savigny, Christian; Rozanov, Alexei; Burrows, John; Zalach, Jakob

    2016-04-01

    The stratospheric aerosol layer (so-called Junge layer) is an inherent part of the Brewer-Dobson circulation (BDC). Stratospheric aerosols play a large role in the Earth's climate system because they interact with catalytic cycles depleting ozone, directly alter the atmosphere's radiative balance and modulate the strength of polar vortices, in particular when this system is perturbed. In terms of mass the layer is predominantly composed of liquid sulphate-water droplets and is fed from the oxidation of gaseous precursors reaching the stratosphere either by direct volcanic injections (mainly supplying SO2) or troposphere-stratosphere exchange processes. In volcanically quiescent periods, latter processes predominantly maintain the so-called background state of aerosol layer through oxidation of OCS above 22 km, and SO2 below. The Junge layer begins to develop 2-3 km above the tropopause and reaches a height of about 35 km, with a largest vertical extent in the tropics and spring-time polar regions. Above the TTL, the layer's vertical extent varies between 2 km and 8 km (about 35% of its mean vertical expansion), depending on the phase of the QBO. The QBO-induced meridional circulation, overlying the BDC, and accompanied signatures in the stratospheric temperature directly affect the life cycle of stratospheric aerosol. Mainly by modulating the equilibrium between microphysical processes which maintain the layer. Effects caused by QBO modulations of the advective transport in the upwelling region of the BDC are smaller and difficult to quantify, because the overlying sedimentation of aerosol is also being modulated and counteract the aerosol lofting. Here we show results from numerical studies performed within the project ROMIC-ROSA (Role of Stratospheric Aerosol in Climate and Atmospheric Science). We further explored relationships between QBO forcing and aerosol processes in the lower stratosphere. We examined whether similar process interferences can be caused by

  5. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

    2005-01-01

    Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds, Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.

  6. The Role of Aerosols on Precipitation Processes: Cloud Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Matsui, T.

    2012-01-01

    Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, the sub-tropics (Florida) and midlatitudes using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CeN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for these cases. It is shown that since the low (CN case produces fewer droplets, larger sizes develop due to greater condensational and collection growth, leading to a broader size spectrum in comparison to the high CCN case. Sensitivity tests were performed to

  7. Characterization of aerosols above the Northern Adriatic Sea: Case studies of offshore and onshore wind conditions

    NASA Astrophysics Data System (ADS)

    Piazzola, J.; Mihalopoulos, N.; Canepa, E.; Tedeschi, G.; Prati, P.; Zarmpas, P.; Bastianini, M.; Missamou, T.; Cavaleri, L.

    2016-05-01

    Aerosol particles in coastal areas result from a complex mixing between sea spray aerosols locally generated at the sea surface by the wind-waves interaction processes and a continental component resulting from natural and/or anthropogenic sources. This paper presents a physical and chemical analysis of the aerosol data acquired from May to September 2014 in the Adriatic Sea. Aerosol distributions were measured on the Acqua Alta platform located 15 km off the coast of Venice using two Particle Measuring System probes and a chemical characterization was made using an Ion Chromatography analysis (IC). Our aim is to study both the sea-spray contribution and the anthropogenic influence in the coastal aerosol of this Mediterranean region. To this end, we focus on a comparison between the present data and the aerosol size distributions measured south of the French Mediterranean coast. For air masses of marine origin transported by southern winds on the French coast and by the Sirocco in the Adriatic, we note a good agreement between the concentrations of super-micrometer aerosols measured in the two locations. This indicates a similar sea surface production of sea-spray aerosols formed by bubble bursting processes in the two locations. In contrast, the results show larger concentrations of submicron particles in the North-Western Mediterranean compared to the Adriatic, which result probably from a larger anthropogenic background for marine conditions. In contrast, for a coastal influence, the chemical analysis presented in the present paper seems to indicate a larger importance of the anthropogenic impact in the Northern Adriatic compared to the North-Western Mediterranean.

  8. Laboratory studies of stratospheric aerosol chemistry

    NASA Technical Reports Server (NTRS)

    Molina, Mario J.

    1996-01-01

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

  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. The impact of relative humidity on aerosol composition and evolution processes during wintertime in Beijing, China

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Wang, Zifa; Fu, Pingqing; Jiang, Qi; Yang, Ting; Li, Jie; Ge, Xinlei

    2013-10-01

    Non-refractory submicron aerosol (NR-PM1) species measured by an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) along with collocated gaseous species are used to investigate the impacts of relative humidity (RH) on aerosol composition and evolution processes during wintertime in Beijing, China. Aerosol species exhibit strong, yet different RH dependence between low and high RH levels. At low RH levels (<50%), all aerosol species increase linearly as a function of RH, among which organics present the largest mass increase rate at 11.4 μg m-3/10% RH. Because the particle liquid water predicted by E-AIM model is very low and the temperature is relatively constant, the enhancement of aerosol species is primarily due to the decrease of wind speed. While the rates of increase for most aerosol species are reduced at high RH levels (>50%), sulfate presents an even faster increasing rate, indicating the significant impact of liquid water on sulfate production. The RH dependence of organic aerosol (OA) components is also quite different. Among OA components, coal combustion OA (CCOA) presents the largest enhancement in both mass concentration and contribution as a function of RH. Our results elucidate the important roles of liquid water in aerosol processing at elevated RH levels, in particular affecting sulfate and CCOA via aqueous-phase reaction and gas-particle partitioning associated with water uptake, respectively. It is estimated that aqueous-phase processing can contribute more than 50% of secondary inorganic species production along with an increase of aerosol particle acidity during the fog periods. However, it appears not to significantly enhance secondary organic aerosol (SOA) formation and the oxidation degree of OA.

  11. CCN Study at Urban Supersite (T0) During MILAGRO: the Essential Information for Prediction of Aerosol CCN Concentrations

    NASA Astrophysics Data System (ADS)

    Wang, J.; Cubison, M.; Aiken, A. C.; Jimenez, J. L.; Collins, D. R.

    2009-12-01

    The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols often consist of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban supersite in Mexico City during MILAGRO are analyzed and the degree of closure is evaluated. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition using extended Köhler theory to concurrent CCN measurements at five supersaturations ranging from 0.11% to 0.35%. The closure agreement and its diurnal variation are studied. CCN concentrations are also derived using various simplifications of the measured aerosol mixing state and chemical composition. The uncertainties associated with these simplifications are compared for different supersaturations and the variation of the uncertainties is examined as a function of aerosol age. The results show that the simplification of internally mixed

  12. A simplified model of aerosol removal by natural processes in reactor containments

    SciTech Connect

    Powers, D.A.; Washington, K.E.; Sprung, J.L.; Burson, S.B.

    1996-07-01

    Simplified formulae are developed for estimating the aerosol decontamination that can be achieved by natural processes in the containments of pressurized water reactors and in the drywells of boiling water reactors under severe accident conditions. These simplified formulae were derived by correlation of results of Monte Carlo uncertainty analyses of detailed models of aerosol behavior under accident conditions. Monte Carlo uncertainty analyses of decontamination by natural aerosol processes are reported for 1,000, 2,000, 3,000, and 4,000 MW(th) pressurized water reactors and for 1,500, 2,500, and 3,500 MW(th) boiling water reactors. Uncertainty distributions for the decontamination factors and decontamination coefficients as functions of time were developed in the Monte Carlo analyses by considering uncertainties in aerosol processes, material properties, reactor geometry and severe accident progression. Phenomenological uncertainties examined in this work included uncertainties in aerosol coagulation by gravitational collision, Brownian diffusion, turbulent diffusion and turbulent inertia. Uncertainties in aerosol deposition by gravitational settling, thermophoresis, diffusiophoresis, and turbulent diffusion were examined. Electrostatic charging of aerosol particles in severe accidents is discussed. Such charging could affect both the coagulation and deposition of aerosol particles. Electrostatic effects are not considered in most available models of aerosol behavior during severe accidents and cause uncertainties in predicted natural decontamination processes that could not be taken in to account in this work. Median (50%), 90 and 10% values of the uncertainty distributions for effective decontamination coefficients were correlated with time and reactor thermal power. These correlations constitute a simplified model that can be used to estimate the decontamination by natural aerosol processes at 3 levels of conservatism. Applications of the model are described.

  13. Type-segregated aerosol effects on regional monsoon activity: A study using ground-based experiments and model simulations

    NASA Astrophysics Data System (ADS)

    Vijayakumar, K.; Devara, P. C. S.; Sonbawne, S. M.

    2014-12-01

    Classification of observed aerosols into key types [e.g., clean-maritime (CM), desert-dust (DD), urban-industrial/biomass-burning (UI/BB), black carbon (BC), organic carbon (OC) and mixed-type aerosols (MA)] would facilitate to infer aerosol sources, effects, and feedback mechanisms, not only to improve the accuracy of satellite retrievals but also to quantify the assessment of aerosol radiative impacts on climate. In this paper, we report the results of a study conducted in this direction, employing a Cimel Sun-sky radiometer at the Indian Institute of Tropical Meteorology (IITM), Pune, India during 2008 and 2009, which represent two successive contrasting monsoon years. The study provided an observational evidence to show that the local sources are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle over Pune, a tropical urban station in India. The results revealed the absence of CM aerosols in the pre-monsoon as well as in the monsoon seasons of 2009 as opposed to 2008. Higher loading of dust aerosols is observed in the pre-monsoon and monsoon seasons of 2009; majority may be coated with fine BC aerosols from local emissions, leading to reduction in regional rainfall. Further, significant decrease in coarse-mode AOD and presence of carbonaceous aerosols, affecting the aerosol-cloud interaction and monsoon-rain processes via microphysics and dynamics, is considered responsible for the reduction in rainfall during 2009. Additionally, we discuss how optical depth, contributed by different types of aerosols, influences the distribution of monsoon rainfall over an urban region using the Monitoring Atmospheric Composition and Climate (MACC) aerosol reanalysis. Furthermore, predictions of the Dust REgional Atmospheric Model (DREAM) simulations combined with HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) cluster model are also discussed in support of the

  14. Rural continental aerosol properties and processes observed during the Hohenpeissenberg Aerosol Characterization Experiment (HAZE2002)

    NASA Astrophysics Data System (ADS)

    Hock, N.; Schneider, J.; Borrmann, S.; Römpp, A.; Moortgat, G.; Franze, T.; Schauer, C.; Pöschl, U.; Plass-Dülmer, C.; Berresheim, H.

    2007-06-01

    Detailed investigations of the chemical and microphysical properties of rural continental aerosols were performed during the HAZE2002 experiment, which was conducted in May 2002 at the Meteorological Observatory Hohenpeissenberg (DWD) in Southern Germany. The online measurement data and techniques included: size-resolved chemical composition of submicron particles by aerosol mass spectrometry (AMS); total particle number concentrations and size distributions over the diameter range of 3 nm to 9 μm (CPC, SMPS, OPC); monoterpenes determined by gas chromatography- ion trap mass spectrometry; OH and H2SO4 determined by atmospheric pressure chemical ionization mass spectrometry (CIMS). Filter sampling and offline analytical techniques were used to determine: fine particle mass (PM2.5), organic, elemental and total carbon in PM2.5 (OC2.5, EC2.5, TC2.5), and selected organic compounds (dicarboxylic acids, polycyclic aromatic hydrocarbons, proteins). Overall, the non-refractory components of submicron particles detected by aerosol mass spectrometry (PM1, 6.6±5.4 μg m-3, arithmetic mean and standard deviation) accounted for ~62% of PM2.5 determined by filter gravimetry (10.6±4.7 μg m-3). The relative proportions of non-refractory submicron particle components were: 11% ammonium, 19% nitrate, 20% sulfate, and 50% organics (OM1). In spite of strongly changing meteorological conditions and absolute concentration levels of particulate matter (3-13 μg m-3 PM1), OM1 was closely correlated with PM1 (r2=0.9) indicating a near-constant ratio of non-refractory organics and inorganics. In contrast, the ratio of nitrate to sulfate was highly dependent on temperature (14-32°C) and relative humidity (20-100%), which could be explained by thermodynamic model calculations of NH3/HNO3/NH4NO3 gas-particle partitioning. From the combination of optical and other sizing techniques (OPC, AMS, SMPS), an average refractive index of 1.40-1.45 was inferred for the measured rural aerosol

  15. A modeling study of seasonal variation of atmospheric aerosols over East Asia

    NASA Astrophysics Data System (ADS)

    Li, Jiawei; Han, Zhiwei

    2012-01-01

    In this study, a regional air quality model system (RAQMS) was applied to investigate the spatial distributions and seasonal variations of atmospheric aerosols in 2006 over East Asia. Model validations demonstrated that RAQMS was able to reproduce the evolution processes of aerosol components reasonably well. Ground-level PM10 (particles with aerodynamic diameter ≤10 µm) concentrations were highest in spring and lowest in summer and were characterized by three maximum centers: the Taklimakan Desert (˜1000 µg m-3), the Gobi Desert (˜ 400 µg m-3), and the Huabei Plain (˜ 300 µg m-3) of China. Vertically, high PM10 concentrations ranging from 100 µg m-3 to 250 µg m-3 occurred from the surface to an altitude of 6000 m at 30°-45°N in spring. In winter, the vertical gradient was so large that most aerosols were restricted in the boundary layer. Both sulfate and ammonium reached their highest concentrations in autumn, while nitrate reached its maximum level in winter. Black carbon and organic carbon aerosol concentrations reached maximums in winter. Soil dust were strongest in spring, whereas sea salt exerted the strongest influence on the coastal regions of eastern China in summer. The estimated burden of anthropogenic aerosols was largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate burden accounted for ˜42% of the total anthropogenic aerosol burden. The dust burden was about twice the anthropogenic aerosol burden, implying the potentially important impacts of the natural aerosols on air quality and climate over East Asia.

  16. Cloud processing of organic compounds: Secondary organic aerosol and nitrosamine formation

    NASA Astrophysics Data System (ADS)

    Hutchings, James W., III

    Cloud processing of atmospheric organic compounds has been investigated through field studies, laboratory experiments, and numerical modeling. Observational cloud chemistry studies were performed in northern Arizona and fog studies in central Pennsylvania. At both locations, the cloud and fogs showed low acidity due to neutralization by soil dust components (Arizona) and ammonia (Pennsylvania). The field observations showed substantial concentrations (20-5500 ng•L -1) of volatile organic compounds (VOC) in the cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase with half lives of approximately three hours. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction kinetics decreased with increasing organic carbon content, resulting in half lives of approximately 7 hours. The secondary organic aerosol (SUA) mass formation potential of cloud processing of BTEX was evaluated. SOA mass formation by cloud processing of BTEX, while strongly dependent on the atmospheric conditions, could contribute up to 9% of the ambient atmospheric aerosol mass, although typically ˜1% appears realistic. Field observations also showed the occurrence of N-nitrosodimethylamine (NDMA), a potent carcinogen, in fogs and clouds (100-340 ng•L -1). Laboratory studies were conducted to investigate the formation of NDMA from nitrous acid and dimethylamine in the homogeneous aqueous phase within cloud droplets. While NDMA was produced in the cloud droplets, the low yields (<1%) observed could not explain observational concentrations

  17. Rural continental aerosol properties and processes observed during the Hohenpeissenberg Aerosol Characterization Experiment (HAZE2002)

    NASA Astrophysics Data System (ADS)

    Hock, N.; Schneider, J.; Borrmann, S.; Römpp, A.; Moortgat, G.; Franze, T.; Schauer, C.; Pöschl, U.; Plass-Dülmer, C.; Berresheim, H.

    2008-02-01

    Detailed investigations of the chemical and microphysical properties of rural continental aerosols were performed during the HAZE2002 experiment, which was conducted in May 2002 at the Meteorological Observatory Hohenpeissenberg (DWD) in Southern Germany. Online measurements included: Size-resolved chemical composition of submicron particles; total particle number concentrations and size distributions over the diameter range of 3 nm to 9 μm; gas-phase concentration of monoterpenes, CO, O3, OH, and H2SO4. Filter sampling and offline analytical techniques were used to determine: Fine particle mass (PM2.5), organic, elemental and total carbon in PM2.5 (OC2.5, EC2.5, TC2.5), and selected organic compounds (dicarboxylic acids, polycyclic aromatic hydrocarbons, proteins). Overall, the non-refractory components of submicron particles detected by aerosol mass spectrometry (PM1, 6.6±5.4 μg m-3, arithmetic mean and standard deviation) accounted for ~62% of PM2.5 determined by filter gravimetry (10.6±4.7 μg m-3). The relative proportions of non-refractory submicron particle components were: (23±39)% ammonium nitrate, (27±23)% ammonium sulfate, and (50±40)% organics (OM1). OM1 was closely correlated with PM1 (r2=0.9) indicating a near-constant ratio of non-refractory organics and inorganics. The average ratio of OM1 to OC2.5 was 2.1±1.4, indicating a high proportion of heteroelements in the organic fraction of the sampled rural aerosol. This is consistent with the high ratio of oxygenated organic aerosol (OOA) over hydrocarbon-like organic aerosol (HOA) inferred from the AMS results (4:1), and also with the high abundance of proteins (~3%) indicating a high proportion of primary biological material (~30%) in PM2.5. This finding was confirmed by low abundance of PAHs (<1 ng m-3) and EC (<1 μg m-3) in PM2.5 and detection of several secondary organic aerosol compounds (dicarboxylic acids) and their precursors (monoterpenes). New particle formation was observed almost

  18. Improvement on lidar data processing for stratospheric aerosol measurements.

    PubMed

    Likura, Y; Sugimoto, N; Sasano, Y; Shimzu, H

    1987-12-15

    For lidar measurements of stratospheric aerosols; signal-induced noise (SIN) from a photomultiplier (PMT) has been a problem of particular interest. In this paper, we succeed in simulating lidar signals affected by the PMT, after finding a long tail with a decay time of ~200 micros in the PMT's response to an impulselike light exposure. The PMT studied was an RCA 8852. Computer simulation quantitatively revealed that the SIN caused by the delayed response became greater than the real signal at high altitudes. Based on the results of simulation, a proposal was made to find a practical method for identifying and removing the SIN from the actual lidar signals. In addition, an improved method for the lidar signal calibration was proposed by taking into account the systematic noise component, including background light as well as SIN, in formulating the clean air calibration (the matching method). Validity of the proposed methods was demonstrated by using them both with an actual lidar signal and a simulated lidar signal with SIN.

  19. Stable carbon isotopic compositions of total carbon, dicarboxylic acids and glyoxylic acid in the tropical Indian aerosols: Implications for sources and photochemical processing of organic aerosols

    NASA Astrophysics Data System (ADS)

    Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.; Tachibana, Eri

    2011-09-01

    The tropical Indian aerosols (PM10) collected on day- and nighttime bases in winter and summer, 2007 from Chennai (13.04°N; 80.17°E) were studied for stable carbon isotopic compositions (δ13C) of total carbon (TC), individual dicarboxylic acids (C2-C9) and glyoxylic acid (ωC2). δ13C values of TC ranged from -23.9‰ to -25.9‰ (-25.0 ± 0.6‰; n = 49). Oxalic (C2) (-17.1 ± 2.5‰), malonic (C3) (-20.8 ± 1.8‰), succinic (C4) (-22.5 ± 1.5‰) and adipic (C6) (-20.6 ± 4.1‰) acids and ωC2 acid (-22.4 ± 5.5‰) were found to be more enriched with 13C compared to TC. In contrast, suberic (C8) (-29.4 ± 1.8‰), phthalic (Ph) (-30.1 ± 3.5‰) and azelaic (C9) (-28.4 ± 5.8‰) acids showed smaller δ13C values than TC. Based on comparisons of δ13C values of TC in Chennai aerosols to those (-24.7 ± 2.2‰) found in unburned cow-dung samples collected from Chennai and isotopic signatures of the particles emitted from point sources, we found that biofuel/biomass burning are the major sources of carbonaceous aerosols in South and Southeast Asia. The decrease in δ13C values of C9 diacid by about 5‰ from winter to summer suggests that tropical plant emissions also significantly contribute to organic aerosol in this region. Significant increase in δ13C values from C4 to C2 diacids in Chennai aerosols could be attributed for their photochemical processing in the tropical atmosphere during long-range transport from source regions.

  20. Aerosol Properties and Processes: A Path from Field and Laboratory Measurements to Global Climate Models

    SciTech Connect

    Ghan, Steven J.; Schwartz, Stephen E.

    2007-07-01

    Aerosols exert a substantial influence on climate and climate change through a variety of complex mechanisms. Consequently there is a need to represent aerosol effects in global climate models, and models have begun to include representations of these effects. However, the treatment of aerosols in current global climate models is presently highly simplified, omitting many important processes and feedbacks. Consequently there is need for substantial improvement. Here we describe the U. S. Department of Energy strategy for improving the treatment of aerosol properties and processes in global climate models. The strategy begins with a foundation of field and laboratory measurements that provide the basis for modules of selected aerosol properties and processes. These modules are then integrated in regional aerosol models, which are evaluated by comparing with field measurements. Issues of scale are then addressed so that the modules can be applied to global aerosol models, which are evaluated by comparing with global satellite measurements. Finally, the validated set of modules are applied to global climate models for multi-century simulations. This strategy can be applied to successive generations of global climate models.

  1. Photochemistry of Glyoxal in Wet Aerosols: Smog Chamber Study

    NASA Astrophysics Data System (ADS)

    Lim, Y. B.; Kim, H.; Turpin, B. J.

    2015-12-01

    Aqueous chemistry is an important pathway for the formation of secondary organic aerosol (SOA). Reaction vessel studies provide evidence that in the aqueous phase photooxidation of water soluble organic compounds (e.g., glyoxal, methylglyoxal) form multifunctional organic products and oligomers. In this work, we extend this bulk-phase chemistry to the condensed-phase chemistry that occurs in/on aerosols by conducting smog chamber experiments — photooxidation of ammonium sulfate and sulfuric acid aerosols containing glyoxal and hydrogen peroxide in the presence of NOx under dry/humid conditions. Particles were analyzed using ultra performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). In the irradiated chamber, photooxidation products of glyoxal as seen in reaction vessel experiments (e.g., oxalic acids and tartaric acids) were also formed in both ammonium sulfate aerosols and sulfuric acid aerosols at humid and even dry conditions. However, the major products were organosulfurs (CHOS), organonitrogens (CHON), and nitrooxy-organosulfates (CHONS), which were also dominantly formed in the dark chamber. These products were formed via non-radical reactions, which depend on acidity and humidity. However, the real-time profiles in the dark chamber and the irradiated chamber were very different, suggesting photochemistry substantially affects non-radical formation in the condensed phase.

  2. CARES: Carbonaceous Aerosol and Radiative Effects Study Operations Plan

    SciTech Connect

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-07-12

    The CARES field campaign is motivated by the scientific issues described in the CARES Science Plan. The primary objectives of this field campaign are to investigate the evolution and aging of carbonaceous aerosols and their climate-affecting properties in the urban plume of Sacramento, California, a mid-size, mid-latitude city that is located upwind of a biogenic volatile organic compound (VOC) emission region. Our basic observational strategy is to make comprehensive gas, aerosol, and meteorological measurements upwind, within, and downwind of the urban area with the DOE G-1 aircraft and at strategically located ground sites so as to study the evolution of urban aerosols as they age and mix with biogenic SOA precursors. The NASA B-200 aircraft, equipped with the High Spectral Resolution Lidar (HSRL), digital camera, and the Research Scanning Polarimeter (RSP), will be flown in coordination with the G-1 to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties, and to provide the vertical context for the G-1 and ground in situ measurements.

  3. Atmospheric aerosol optical parameters, deep convective clouds and hail occurence - a correlation study

    NASA Astrophysics Data System (ADS)

    Talianu, Camelia; Andrei, Simona; Toanca, Florica; Stefan, Sabina

    2016-04-01

    Among the severe weather phenomena, whose frequency has increased during the past two decades, hail represents a major threat not only for agriculture but also for other economical fields. Generally, hail are produced in deep convective clouds, developed in an unstable environment. Recent studies have emphasized that besides the state of the atmosphere, the atmospheric composition is also very important. The presence of fine aerosols in atmosphere could have a high impact on nucleation processes, initiating the occurrence of cloud droplets, ice crystals and possibly the occurrence of graupel and/or hail. The presence of aerosols in the atmosphere, correlated with specific atmospheric conditions, could be predictors of the occurrence of hail events. The atmospheric investigation using multiwavelength Lidar systems can offer relevant information regarding the presence of aerosols, identified using their optical properties, and can distinguish between spherical and non-spherical shape, and liquid and solid phase of these aerosols. The aim of this study is to analyse the correlations between the presence and the properties of aerosols in atmosphere, and the production of hail events in a convective environment, using extensive and intensive optical parameters computed from lidar and ceilometer aerosols measurements. From these correlations, we try to evaluate if these aerosols can be taken into consideration as predictors for hail formation. The study has been carried out in Magurele - Romania (44.35N, 26.03E, 93m ASL) using two collocated remote sensing systems: a Raman Lidar (RALI) placed at the Romanian Atmospheric 3D Observatory and a ceilometer CL31 placed at the nearby Faculty of Physics, University of Bucharest. To evaluate the atmospheric conditions, radio sounding and satellite images were used. The period analysed was May 1st - July 15th, 2015, as the May - July period is climatologically favorable for deep convection events. Two hail events have been

  4. Precipitation and aerosol studies in India.

    PubMed

    Parashar, D C; Kulshrestha, U C; Jain, M

    2001-01-01

    In India, rain water and atmospheric aerosols are observed to be alkaline in nature due to the influence of soil-derived particles which are rich in components like Ca and Mg. These components increase the neutralization potential of rain water and have a greater influence at rural site compared to urban site. However, if there are continuous rains, the concentration of crustal components becomes lower resulting in lower pH of rain water. Unlike the characteristics of rain water on continent, the pH of rain water has been observed to be acidic in all the events over the Indian Ocean during Pre-campaigns of Indian Ocean Experiment (INDOEX). The possible reason for acidic rains over Indian Ocean could be the anthropogenic contribution from continent transported by NE winds coming towards the ocean during this period.

  5. Experimental Studies on Dynamic Properties of Fibrous Aerosols

    NASA Astrophysics Data System (ADS)

    Yang, Miintsong

    Throughout the development of the theory of fibrous aerosol particles, the dynamic behaviour of fibrous aerosol particles has most often been approximated by prolate spheroids. During recent experiments with chain-like particles of axis ratios between 5 and 1000, it became clear that the dynamics of fibrous particles needs to be well studied. This work addresses this need by studying both translational and rotational motions using various techniques. One of the measurements described below extends the classical work done with macroscopic bodies in oil tanks. The determination of drag and shape factors of chains and cylinders relative to that of prolate spheroids was obtained with chains of equal sized spheres and tungsten cylinders of various axis ratios between 2 and 50. Re was kept below ca. 0.01 for all particles by using silicone oil with a viscosity of ca. 110 poise. Empirical wall corrections in both principal orientations were developed for prolated bodies moving along the axis of an "infinitely long" cylindrical tube. Respective uncertainties for shape factors and wall corrections were typically (+OR-)1% and (+OR-)10%. The other measurement studied measures electrical light scattering of fibrous aerosols. Due to Brownian rotational motion, the size distribution function to nonspherical aerosols was determined after removing the electrical field which had been applied to the aerosol flow by measuring the decay of intensity of scattered light in a small foward angle with respect to the laser beam. Some necessary inter -instrument comparisons were made by using three different sizes of chain-like aerosols. Whether NNLS, nonlinear regression, or lognormal fittings were used they yielded very consistent results. The agreement of the count median between comparisons was very satisfactory. The uncertainty of the mean size was typically (+OR-)3%.

  6. Evaluation of Slit Sampler in Quantitative Studies of Bacterial Aerosols

    PubMed Central

    Ehrlich, Richard; Miller, Sol; Idoine, L. S.

    1966-01-01

    Quantitative studies were conducted to evaluate the efficiency of the slit sampler in collecting airborne Serratia marcescens and Bacillus subtilis var. niger, and to compare it with the collecting efficiency of the all-glass impinger AGI-30. The slit sampler was approximately 50% less efficient than the AGI-30. This ratio remained the same whether liquid or dry cultures were disseminated when the sample was taken at 2 min of aerosol cloud life. At 30 min of aerosol cloud life, this ratio was approximately 30% for B. subtilis var. niger. S. marcescens recoveries by the slit sampler were, however, only 17% lower than the AGI-30 at 30 min of cloud age, indicating a possible interaction involving the more labile vegetative cells, aerosol age, and method of collection. PMID:4961550

  7. Comparison of five bacteriophages as models for viral aerosol studies.

    PubMed

    Turgeon, Nathalie; Toulouse, Marie-Josée; Martel, Bruno; Moineau, Sylvain; Duchaine, Caroline

    2014-07-01

    Bacteriophages are perceived to be good models for the study of airborne viruses because they are safe to use, some of them display structural features similar to those of human and animal viruses, and they are relatively easy to produce in large quantities. Yet, only a few studies have investigated them as models. It has previously been demonstrated that aerosolization, environmental conditions, and sampling conditions affect viral infectivity, but viral infectivity is virus dependent. Thus, several virus models are likely needed to study their general behavior in aerosols. The aim of this study was to compare the effects of aerosolization and sampling on the infectivity of five tail-less bacteriophages and two pathogenic viruses: MS2 (a single-stranded RNA [ssRNA] phage of the Leviviridae family), Φ6 (a segmented double-stranded RNA [dsRNA] phage of the Cystoviridae family), ΦX174 (a single-stranded DNA [ssDNA] phage of the Microviridae family), PM2 (a double-stranded DNA [dsDNA] phage of the Corticoviridae family), PR772 (a dsDNA phage of the Tectiviridae family), human influenza A virus H1N1 (an ssRNA virus of the Orthomyxoviridae family), and the poultry virus Newcastle disease virus (NDV; an ssRNA virus of the Paramyxoviridae family). Three nebulizers and two nebulization salt buffers (with or without organic fluid) were tested, as were two aerosol sampling devices, a liquid cyclone (SKC BioSampler) and a dry cyclone (National Institute for Occupational Safety and Health two-stage cyclone bioaerosol sampler). The presence of viruses in collected air samples was detected by culture and quantitative PCR (qPCR). Our results showed that these selected five phages behave differently when aerosolized and sampled. RNA phage MS2 and ssDNA phage ΦX174 were the most resistant to aerosolization and sampling. The presence of organic fluid in the nebulization buffer protected phages PR772 and Φ6 throughout the aerosolization and sampling with dry cyclones. In this

  8. Comparison of Five Bacteriophages as Models for Viral Aerosol Studies

    PubMed Central

    Turgeon, Nathalie; Toulouse, Marie-Josée; Martel, Bruno; Moineau, Sylvain

    2014-01-01

    Bacteriophages are perceived to be good models for the study of airborne viruses because they are safe to use, some of them display structural features similar to those of human and animal viruses, and they are relatively easy to produce in large quantities. Yet, only a few studies have investigated them as models. It has previously been demonstrated that aerosolization, environmental conditions, and sampling conditions affect viral infectivity, but viral infectivity is virus dependent. Thus, several virus models are likely needed to study their general behavior in aerosols. The aim of this study was to compare the effects of aerosolization and sampling on the infectivity of five tail-less bacteriophages and two pathogenic viruses: MS2 (a single-stranded RNA [ssRNA] phage of the Leviviridae family), Φ6 (a segmented double-stranded RNA [dsRNA] phage of the Cystoviridae family), ΦX174 (a single-stranded DNA [ssDNA] phage of the Microviridae family), PM2 (a double-stranded DNA [dsDNA] phage of the Corticoviridae family), PR772 (a dsDNA phage of the Tectiviridae family), human influenza A virus H1N1 (an ssRNA virus of the Orthomyxoviridae family), and the poultry virus Newcastle disease virus (NDV; an ssRNA virus of the Paramyxoviridae family). Three nebulizers and two nebulization salt buffers (with or without organic fluid) were tested, as were two aerosol sampling devices, a liquid cyclone (SKC BioSampler) and a dry cyclone (National Institute for Occupational Safety and Health two-stage cyclone bioaerosol sampler). The presence of viruses in collected air samples was detected by culture and quantitative PCR (qPCR). Our results showed that these selected five phages behave differently when aerosolized and sampled. RNA phage MS2 and ssDNA phage ΦX174 were the most resistant to aerosolization and sampling. The presence of organic fluid in the nebulization buffer protected phages PR772 and Φ6 throughout the aerosolization and sampling with dry cyclones. In this

  9. Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

    NASA Astrophysics Data System (ADS)

    Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

    2014-12-01

    Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

  10. The NASA-AMES Research Center Stratospheric Aerosol Model. 1. Physical Processes and Computational Analogs

    NASA Technical Reports Server (NTRS)

    Turco, R. P.; Hamill, P.; Toon, O. B.; Whitten, R. C.; Kiang, C. S.

    1979-01-01

    A time-dependent one-dimensional model of the stratospheric sulfate aerosol layer is presented. In constructing the model, a wide range of basic physical and chemical processes are incorporated in order to avoid predetermining or biasing the model predictions. The simulation, which extends from the surface to an altitude of 58 km, includes the troposphere as a source of gases and condensation nuclei and as a sink for aerosol droplets. The size distribution of aerosol particles is resolved into 25 categories with particle radii increasing geometrically from 0.01 to 2.56 microns such that particle volume doubles between categories.

  11. Modelling aerosol-cloud-meteorology interaction: A case study with a fully coupled air quality model (GEM-MACH)

    NASA Astrophysics Data System (ADS)

    Gong, W.; Makar, P. A.; Zhang, J.; Milbrandt, J.; Gravel, S.; Hayden, K. L.; Macdonald, A. M.; Leaitch, W. R.

    2015-08-01

    A fully coupled on-line air quality forecast model, GEM-MACH, was used to study aerosol-cloud interactions for a case of an urban-industrial plume impacting stratocumulus. The aerosol effect on the cloud microphysics was achieved by the use of parameterization of cloud droplet nucleation predicted from the on-line size- and composition-resolved aerosols and coupled with a double-moment cloud microphysics parameterization. The model simulations with and without the on-line aerosol effect on cloud microphysics were compared and evaluated against in-situ aerosol and cloud observations from ICARTT 2004. Inclusion of the on-line aerosol interaction with cloud resulted in an increase in modelled cloud amount and cloud liquid water content (LWC) due to increased cloud droplet number concentration (Nd), a decrease in cloud droplet size and a reduction in warm precipitation. The modelled LWC and Nd agreed more closely with the observations when the on-line aerosol was allowed to affect the cloud than when aerosol effects on cloud were not explicitly simulated. The increased cloud amount due to the aerosol effects reduced the modelled downward shortwave radiative flux and air temperature at the surface, contributing to a decrease in ozone over the region of enhanced cloud and an increase in particle sulphate from an increased capacity for aqueous-phase production. Aerosol activation is shown to have a significant influence on the cloud microphysics and cloud processing of trace gases and aerosols. The importance of reasonable parameterization of cloud updraft speed is demonstrated.

  12. 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.

  13. (PORTUGAL)THE DETROIT EXPOSURE AND AEROSOL RESEARCH STUDY

    EPA Science Inventory

    The Detroit Exposure and Aerosol Research Study (DEARS) represents an intensive examination of personal, residential and community-based particulate matter and related co-pollutant measurements in Detroit, Michigan. Data from the DEARS will be used as inputs into air quality, la...

  14. 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

  15. Study of radioactive contamination in silts and aerosols at Aldama City, Mexico, due to the operation of a yellow-cake processing plant.

    PubMed

    Montelongo, Michel Y; Herrera, Eduardo F; Ramirez, Elias; Carrillo, Jorge I; Campos, Alfredo; Gomez, Ramón; Montero, Maria E; Rodriguez, Luis M

    2015-08-01

    The city of Aldama, Chihuahua, Mexico is located 30 km NNE of Chihuahua city. Three high-volume collectors with PM10 heads were placed in specific locations in Aldama during the year 2011 to measure radioisotope concentrations in the air. The city area of 16 km² was divided into 64 squares of 500 × 500 m. At the vertices of the grid, silt samples were taken between January and June 2011, before the rains began. The concentrations of natural, cosmogenic, and anthropogenic radioactive isotopes were calculated in both filters and silts samples. The isotopes selected for the measurement were ²³⁸U, ²³²Th, (7)Be, ¹³⁷Cs, and ⁴⁰K. Measurements of PM10 and silts were performed during 2011, coinciding with the accident at Fukushima, Japan, on March 11. For this reason, we could see the ¹³⁷Cs in PM10 increase between April and July; with the arrival of the rains, the ¹³⁷Cs concentration began to decrease in the air. The concentration of PM10 measured by the equipment located at the Mexican Uranium plant (URAMEX, initials in Spanish) that was processing radioactive ores exceeded the standard values in February and March, when the air velocity increases. At City Hall, the concentration of PM10 surpassed the value of the standard between May and July. This increased concentration is likely due to increased automobile traffic because City Hall is located in the city center. At a private home, the concentration of PM10 surpassed the standard on several days during the year because the home is located on the outskirts of the city, where most of the streets are not paved. Due to the high concentrations of PM10, especially at the collection point located at the private home, it is necessary to start taking steps to mitigate their spread before they cause health problems in the younger population and in older adults.

  16. Study of radioactive contamination in silts and aerosols at Aldama City, Mexico, due to the operation of a yellow-cake processing plant.

    PubMed

    Montelongo, Michel Y; Herrera, Eduardo F; Ramirez, Elias; Carrillo, Jorge I; Campos, Alfredo; Gomez, Ramón; Montero, Maria E; Rodriguez, Luis M

    2015-08-01

    The city of Aldama, Chihuahua, Mexico is located 30 km NNE of Chihuahua city. Three high-volume collectors with PM10 heads were placed in specific locations in Aldama during the year 2011 to measure radioisotope concentrations in the air. The city area of 16 km² was divided into 64 squares of 500 × 500 m. At the vertices of the grid, silt samples were taken between January and June 2011, before the rains began. The concentrations of natural, cosmogenic, and anthropogenic radioactive isotopes were calculated in both filters and silts samples. The isotopes selected for the measurement were ²³⁸U, ²³²Th, (7)Be, ¹³⁷Cs, and ⁴⁰K. Measurements of PM10 and silts were performed during 2011, coinciding with the accident at Fukushima, Japan, on March 11. For this reason, we could see the ¹³⁷Cs in PM10 increase between April and July; with the arrival of the rains, the ¹³⁷Cs concentration began to decrease in the air. The concentration of PM10 measured by the equipment located at the Mexican Uranium plant (URAMEX, initials in Spanish) that was processing radioactive ores exceeded the standard values in February and March, when the air velocity increases. At City Hall, the concentration of PM10 surpassed the value of the standard between May and July. This increased concentration is likely due to increased automobile traffic because City Hall is located in the city center. At a private home, the concentration of PM10 surpassed the standard on several days during the year because the home is located on the outskirts of the city, where most of the streets are not paved. Due to the high concentrations of PM10, especially at the collection point located at the private home, it is necessary to start taking steps to mitigate their spread before they cause health problems in the younger population and in older adults. PMID:26211631

  17. 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.

  18. Predicting the mineral composition of dust aerosols - Part 2: Model evaluation and identification of key processes with observations

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

    A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

  19. Predicting the Mineral Composition of Dust Aerosols. Part 2; Model Evaluation and Identification of Key Processes with Observations

    NASA Technical Reports Server (NTRS)

    Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

    2015-01-01

    A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

  20. Experimental studies of silver iodide pyrotechnic aerosol ice forming efficiency dynamics

    NASA Astrophysics Data System (ADS)

    Shilin, A. G.; Drofa, A. S.; Ivanov, V. N.; Savchenko, A. V.; Shilin, V. A.

    2013-05-01

    The study concerns the problems connected with the temporal variability of aerosol ice forming activity at introduction into the sub-cloud layer and the comparison of aerosol efficiency of produced pyrotechnic mixtures with different silver contents.

  1. Sources and source processes of organic nitrogen aerosols in the atmosphere

    NASA Astrophysics Data System (ADS)

    Erupe, Mark E.

    The research in this dissertation explored the sources and chemistry of organic nitrogen aerosols in the atmosphere. Two approaches were employed: field measurements and laboratory experiments. In order to characterize atmospheric aerosol, two ambient studies were conducted in Cache Valley in Northern Utah during strong winter inversions of 2004 and 2005. The economy of this region is heavily dependent on agriculture. There is also a fast growing urban population. Urban and agricultural emissions, aided by the valley geography and meteorology, led to high concentrations of fine particles that often exceeded the national ambient air quality standards. Aerosol composition was dominated by ammonium nitrate and organic species. Mass spectra from an aerosol mass spectrometer revealed that the organic ion peaks were consistent with reduced organic nitrogen compounds, typically associated with animal husbandry practices. Although no direct source characterization studies have been undertaken in Cache Valley with an aerosol mass spectrometer, spectra from a study at a swine facility in Ames, Iowa, did not show any evidence of reduced organic nitrogen species. This, combined with temporal and diurnal characteristics of organic aerosol peaks, was a pointer that the organic nitrogen species in Cache Valley likely formed from secondary chemistry. Application of multivariate statistical analyses to the organic aerosol spectra further supported this hypothesis. To quantify organic nitrogen signals observed in ambient studies as well as understand formation chemistry, three categories of laboratory experiments were performed. These were calibration experiments, smog chamber studies, and an analytical method development. Laboratory calibration experiments using standard calibrants indicated that quantifying the signals from organic nitrogen species was dependent on whether they formed through acid-base chemistry or via secondary organic aerosol pathway. Results from smog chamber

  2. Cloud condensation nuclei closure study on summer arctic aerosol

    NASA Astrophysics Data System (ADS)

    Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

    2011-11-01

    We present an aerosol - cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble

  3. Chemical characterization of emissions from vegetable oil processing and their contribution to aerosol mass using the organic molecular markers approach.

    PubMed

    Kavouras, I G; Stratigakis, N; Stephanou, E G

    2001-04-01

    The organic fraction of aerosol emitted from a vegetable oil processing plant was studied to investigate the contribution of emissions to ambient particles in the surrounding area. Solvent-soluble particulate organic compounds emitted from the plant accounted for 10% of total suspended particles. This percentage was lower in the receptor sites (less than 6% of total aerosol mass). Nonpolar, moderate polar, polar, and acidic compounds were detected in both emitted and ambient aerosol samples. The processing and combustion of olive pits yielded a source with strong biogenic characteristics, such as the high values of the carbon preference index (CPI) for all compound classes. Polycyclic aromatic hydrocarbons (PAHs) detected in emissions were associated with both olive pits and diesel combustion. The chromatographic profile of dimethylphenanthrenes (DMPs) was characteristic of olive pit combustion. Organic aerosols collected in two receptor sites provided a different pattern. The significant contribution of vehicular emissions was identified by CPI values (approximately 1) of n-alkanes and the presence of the unresolved complex mixture (UCM). In addition, PAH concentration diagnostic ratios indicated that emissions from catalyst and noncatalyst automobiles and heavy trucks were significant. The strong even-to-odd predominance of n-alkanols, n-alkanoic acids, and their salts indicated the contribution of a source with biogenic characteristics. However, the profile of DMPs at receptor sites was similar to that observed for diesel particulates. These differences indicated that the contribution of vegetable oil processing emissions to the atmosphere was negligible.

  4. Development studies towards an 11-year global gridded aerosol optical thickness reanalysis for climate and applied applications

    NASA Astrophysics Data System (ADS)

    Lynch, P.; Reid, J. S.; Westphal, D. L.; Zhang, J.; Hogan, T. F.; Hyer, E. J.; Curtis, C. A.; Hegg, D. A.; Shi, Y.; Campbell, J. R.; Rubin, J. I.; Sessions, W. R.; Turk, F. J.; Walker, A. L.

    2015-12-01

    While standalone satellite and model aerosol products see wide utilization, there is a significant need in numerous climate and applied applications for a fused product on a regular grid. Aerosol data assimilation is an operational reality at numerous centers, and like meteorological reanalyses, aerosol reanalyses will see significant use in the near future. Here we present a standardized 2003-2013 global 1° × 1° and 6 hourly modal aerosol optical thickness (AOT) reanalysis product. This dataset can be applied to basic and applied earth system science studies of significant aerosol events, aerosol impacts on numerical weather prediction, and electro-optical propagation and sensor performance, among other uses. This paper describes the science of how to develop and score an aerosol reanalysis product. This reanalysis utilizes a modified Navy Aerosol Analysis and Prediction System (NAAPS) at its core and assimilates quality controlled retrievals of AOT from the Moderate Resolution Imaging Spectroradiometer (MODIS) on Terra and Aqua and the Multi-angle Imaging SpectroRadiometer (MISR) on Terra. The aerosol source functions, including dust and smoke, were regionally tuned to obtain the best match between the model fine and coarse mode AOTs and the Aerosol Robotic Network (AERONET) AOTs. Other model processes, including deposition, were tuned to minimize the AOT difference between the model and satellite AOT. Aerosol wet deposition in the tropics is driven with satellite retrieved precipitation, rather than the model field. The final reanalyzed fine and coarse mode AOT at 550 nm is shown to have good agreement with AERONET observations, with global mean root mean square error around 0.1 for both fine and coarse mode AOTs. This paper includes a discussion of issues particular to aerosol reanalyses that make them distinct from standard meteorological reanalyses, considerations for extending such a reanalysis outside of the NASA A-Train era, and examples of how the

  5. Impact of aerosol and freezing level on orographic clouds: A sensitivity study

    NASA Astrophysics Data System (ADS)

    Xiao, Hui; Yin, Yan; Chen, Qian; Zhao, Pengguo

    2016-07-01

    The response of clouds and precipitation to changes in aerosol properties is variable with the ambient meteorological conditions, which is important for the distribution of water resources, especially in mountain regions. In this study, a detailed bin microphysics scheme is coupled into the Weather Research and Forecasting (WRF) model to investigate how orographic clouds and precipitation respond to changes in aerosols under different thermodynamic profiles. The model results suggest that when the initial aerosol number concentration changes from a clean continental background (4679 cm- 3) to a polluted urban environment (23,600 cm- 3), the accumulated surface precipitation amount can be increased up to 14% mainly due to the enhanced riming process which results from more droplets of 10-30 μm in diameter. When the freezing level is lowered from 2.85 km to 0.9 km (above 1000 hPa level), the growth of ice-phase particles via riming process is enhanced, leading to more precipitation. However, the response of surface precipitation amount to increase in aerosol particle concentration is not linear with lowering freezing level, and there is a maximum precipitation enhancement caused by aerosols (about 14%) as the freezing level is at 1.4 km. Further sensitivity tests show that, the response of riming growth to increase in aerosol particle concentration becomes more significant with lowering the freezing level, but this effect becomes less significant as the freezing level is further lowered due to the limited liquid water. Moreover, the growth of raindrops through collision and coalescence is suppressed with lowering freezing level, due to the shorter distance between the melting level and the ground.

  6. Dissolved organic matter in sea spray: a transfer study from marine surface water to aerosols

    NASA Astrophysics Data System (ADS)

    Schmitt-Kopplin, P.; Liger-Belair, G.; Koch, B. P.; Flerus, R.; Kattner, G.; Harir, M.; Kanawati, B.; Lucio, M.; Tziotis, D.; Hertkorn, N.; Gebefügi, I.

    2012-04-01

    Atmospheric aerosols impose direct and indirect effects on the climate system, for example, by absorption of radiation in relation to cloud droplets size, on chemical and organic composition and cloud dynamics. The first step in the formation of Organic primary aerosols, i.e. the transfer of dissolved organic matter from the marine surface into the atmosphere, was studied. We present a molecular level description of this phenomenon using the high resolution analytical tools of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and nuclear magnetic resonance spectroscopy (NMR). Our experiments confirm the chemoselective transfer of natural organic molecules, especially of aliphatic compounds from the surface water into the atmosphere via bubble bursting processes. Transfer from marine surface water to the atmosphere involves a chemical gradient governed by the physicochemical properties of the involved molecules when comparing elemental compositions and differentiating CHO, CHNO, CHOS and CHNOS bearing compounds. Typical chemical fingerprints of compounds enriched in the aerosol phase were CHO and CHOS molecular series, smaller molecules of higher aliphaticity and lower oxygen content, and typical surfactants. A non-targeted metabolomics analysis demonstrated that many of these molecules corresponded to homologous series of oxo-, hydroxy-, methoxy-, branched fatty acids and mono-, di- and tricarboxylic acids as well as monoterpenes and sugars. These surface active biomolecules were preferentially transferred from surface water into the atmosphere via bubble bursting processes to form a significant fraction of primary organic aerosols. This way of sea spray production leaves a selective biological signature of the surface water in the corresponding aerosol that may be transported into higher altitudes up to the lower atmosphere, thus contributing to the formation of secondary organic aerosol on a global scale or transported laterally with

  7. Evaluating WRF-Chem multi-scale model in simulating aerosol radiative properties over the tropics – A case study over India

    SciTech Connect

    Seethala, C.; Pandithurai, G.; Fast, Jerome D.; Polade, Suraj D.; Reddy, M. S.; Peckham, Steven E.

    2012-01-24

    We utilized WRF-Chem multi-scale model to simulate the regional distribution of aerosols, optical properties and its effect on radiation over India for a winter month. The model is evaluated using measurements obtained from upper-air soundings, AERONET sun photometers, various satellite instruments, and pyranometers operated by the Indian Meteorological Department. The simulated downward shortwave flux was overestimated when the effect of aerosols on radiation and clouds was neglected. Downward shortwave radiation from a simulation that included aerosol-radiation interaction processes was 5 to 25 Wm{sup -2} closer to the observations, while a simulation that included aerosol-cloud interaction processes were another 1 to 20 Wm{sup -2} closer to the observations. For the few observations available, the model usually underestimated particulate concentration. This is likely due to turbulent mixing, transport errors and the lack of secondary organic aerosol treatment in the model. The model efficiently captured the broad regional hotspots such as high aerosol optical depth over Indo-Gangetic basin as well as the northwestern and southern part of India. The regional distribution of aerosol optical depth compares well with AVHRR aerosol optical depth and the TOMS aerosol index. The magnitude and wavelength-dependence of simulated aerosol optical depth was also similar to the AERONET observations across India. Differences in surface shortwave radiation between simulations that included and neglected aerosol-radiation interactions were as high as -25 Wm{sup -2}, while differences in surface shortwave radiation between simulations that included and neglect aerosol-radiation-cloud interactions were as high as -30 Wm{sup -2}. The spatial variations of these differences were also compared with AVHRR observation. This study suggests that the model is able to qualitatively simulate the impact of aerosols on radiation over India; however, additional measurements of particulate

  8. Effect of operation conditions of the drop-on-demand aerosol generator on aerosol characteristics: Pseudo-cinematographic and plasma mass spectrometric studies

    NASA Astrophysics Data System (ADS)

    Orlandini v. Niessen, Jan O.; Krone, Karin M.; Bings, Nicolas H.

    2014-02-01

    The recently presented drop-on-demand (DOD) aerosol generator overcomes some of the drawbacks of pneumatic nebulization, as its aerosol is no longer generated by gas-liquid interaction. In the current study, an advanced imaging technique is presented, based on a CCD camera equipped with magnifying telecentric optics to allow for fast, automated and precise aerosol characterization as well as fundamental studies on the droplet generation processes by means of pseudo-cinematography. The DOD aerosol generator is thoroughly characterized regarding its droplet size distribution, which shows few distinct populations rather than a continuous distribution. Other important figures, such as the Sauter diameter (D3,2) of 22 μm and the span of 0.4 were also determined. Additionally, the influence of the electrical operation conditions of the dosing device on the aerosol generation process is described. The number and volume of the generated droplets were found to be very reproducible and user-variable, e.g. from 17 to 27 μm (D3,2), within a span of 0.07-0.89. The performances of different setups of the DOD as liquid sample introduction system in ICP-MS are correlated to the respective achievable aerosol characteristics and are also compared to the performance of a state-of-the-art μ-flow nebulizer (EnyaMist). The DOD system allowed for improved sensitivity, but slightly elevated signal noise and overall comparable limits of detection. The results are critically discussed and future directions are outlined.

  9. SeReNA Project: studying aerosol interactions with cloud microphysics in the Amazon Basin

    NASA Astrophysics Data System (ADS)

    Correia, A. L.; Catandi, P. B.; Frigeri, F. F.; Ferreira, W. C.; Martins, J.; Artaxo, P.

    2012-12-01

    Cloud microphysics and its interaction with aerosols is a key atmospheric process for weather and climate. Interactions between clouds and aerosols can impact Earth's radiative balance, its hydrological and energetic cycles, and are responsible for a large fraction of the uncertainty in climatic models. On a planetary scale, the Amazon Basin is one of the most significant land sources of moisture and latent heat energy. Moreover, every year this region undergoes mearked seasonal shifts in its atmospheric state, transitioning from clean to heavily polluted conditions due to the occurrence of seasonal biomass burning fires, that emit large amounts of smoke to the atmosphere. These conditions make the Amazon Basin a special place to study aerosol-cloud interactions. The SeReNA Project ("Remote sensing of clouds and their interaction with aerosols", from the acronym in Portuguese, @SerenaProject on Twitter) is an ongoing effort to experimentally investigate the impact of aerosols upon cloud microphysics in Amazonia. Vertical profiles of droplet effective radius of water and ice particles, in single convective clouds, can be derived from measurements of the emerging radiation on cloud sides. Aerosol optical depth, cloud top properties, and meteorological parameters retrieved from satellites will be correlated with microphysical properties derived for single clouds. Maps of cloud brightness temperature will allow building temperature vs. effective radius profiles for hydrometeors in single clouds. Figure 1 shows an example extracted from Martins et al. (2011), illustrating a proof-of-concept for the kind of result expected within the framework for the SeReNA Project. The results to be obtained will help foster the quantitative knowledge about interactions between aerosols and clouds in a microphysical level. These interactions are a fundamental process in the context of global climatic changes, they are key to understanding basic processes within clouds and how aerosols

  10. Aerosol Composition in the Los Angeles Basin Studied by High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Hayes, P. L.; Ortega, A. M.; Cubison, M.; Hu, W.; Toohey, D. W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Alvarez, S. L.; Rappenglueck, B.; Allan, J. D.; Taylor, J.; Holloway, J. S.; Gilman, J. B.; Kuster, W. C.; De Gouw, J. A.; Massoli, P.; Zhang, X.; Weber, R.; Zhao, Y.; Cliff, S. S.; Wexler, A. S.; Isaacman, G. A.; Worton, D. R.; Kreisberg, N. M.; Hering, S. V.; Goldstein, A. H.; Jimenez, J. L.

    2011-12-01

    Atmospheric aerosols impact climate and health, but their sources and composition are poorly understood. To address this knowledge gap, a high-resolution aerosol mass spectrometer (AMS) and complementary instrumentation were deployed during the 2010 CalNex campaign to characterize aerosol composition in the Los Angeles (LA) area. Total mass concentrations as well as the species concentrations measured by the AMS compare well with most other instruments. Nitrate dominates in the mornings, but its concentration is reduced in the afternoon when organic aerosols (OA) increase and dominate. The diurnal variations in concentrations are strongly influenced by emission transport from the source-rich western basin. The average OA to enhanced CO ratio increases with photochemical age from 25 to 80 μg m-3 ppm-1, which indicates significant secondary OA (SOA) production and that a large majority of OA is secondary in aged air. The ratio values are similar to those from Mexico City as well as New England and the Mid-Atlantic States. Positive matrix factorization (PMF) is used to assess the concentrations of different OA components. The major OA classes are oxygenated OA (OOA, a surrogate for total SOA), and hydrocarbon-like OA (HOA, a surrogate for primary combustion OA). Several subclasses of OA are identified as well including diesel-influenced HOA (DI-HOA) and non-diesel HOA. DI-HOA exhibits low concentrations on Sundays consistent with the well-known weekday/weekend effect in LA. PMF analysis finds that OOA is 67% of the total OA concentration. A strong correlation between OOA and Ox (O3 + NO2) concentrations is observed with a slope of 0.15 that suggests the production of fresh SOA in Pasadena. Plotting the OA elemental ratios in a Van Krevelen diagram (H:C vs. O:C) yields a slope of -0.6, which is less steep than that observed in Riverside during the SOAR-2005 campaign. The difference in slopes may be attributed to the highly oxidized HOA present in Pasadena that is

  11. Apportionment of Primary and Secondary Organic Aerosols in Southern California During the 2005 Study of Organic Aerosols in Riverside (SOAR-1)

    EPA Science Inventory

    Ambient sampling was conducted in Riverside, California during the 2005 Study of Organic Aerosols in Riverside to characterize the composition and sources of organic aerosol using a variety of state-of-the-art instrumentation and source apportionment techniques.

  12. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

    2004-01-01

    Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles (i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail). Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, in the sub-tropics (Florida) and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low 'clean' concentration and a high 'dirty' concentration.

  13. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.; Johnson, D.; Remer, L.

    2004-01-01

    Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembel (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and in the mid-latitude continent with different concentrations of CCN: a low "c1ean"concentration and a high "dirty" concentration. In addition, differences and similarities between bulk microphysics and spectral-bin microphysical schemes will be examined and discussed.

  14. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.; Johnson, D.; Remer, L.

    2004-01-01

    Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, r d a U production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembe1 (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and platelike), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and in the mid-latitude continent with different concentrations of CCN: a low "c1ean"concentration and a high "dirty" concentration. In addition, differences and similarities between bulk microphysics and spectral-bin microphysical schemes will be examined and discussed.

  15. A Systematic Evaluation of the Extent of Photochemical Processing in Different Types of Secondary Organic Aerosols in the Aqueous Phase

    NASA Astrophysics Data System (ADS)

    Romonosky, D.; Lee, H.; Epstein, S. A.; Nizkorodov, S.; Laskin, J.; Laskin, A.

    2013-12-01

    A significant fraction of atmospheric organic compounds are predominantly found in condensed phases, such as organic phase in aerosol particles or aqueous phase in cloud droplets. The oxidation of VOCs followed by the condensation of products into particles was thought to be the main mechanism of organic aerosol (OA) formation. However, in the last several years, scientists have realized that a large fraction, if not the majority of organic particles, is produced through cloud and fog photochemical processes. Many of these organic compounds are photolabile, and can degrade through direct photolysis or indirect photooxidation processes on time scales that are comparable to the typical lifetimes of droplets (hours) and particles (days). We previously reported that compounds in secondary organic aerosol (SOA) from ozonolysis of d-limonene efficiently photodegrade in both organic (Walser et al., 2007) and aqueous phases (Bateman et al., 2011). Significant photolysis was also observed in an aqueous extract of SOA from high-NOx photooxidation of isoprene (Nguyen et al., 2012). More recent experiments studying the response to irradiation of complex aqueous mixtures (as opposed to solutions of isolated compounds) found surprising resilience to photodegradation in aqueous extracts of SOA prepared by photooxidation of alpha-pinene (Romonosky et al., unpublished). We present a systematic investigation of the extent of photochemical processing in different types of SOA from various biogenic and anthropogenic precursors. Chamber- or flowtube-generated SOA is collected on an inert substrate, extracted in a methanol/water solution (70:30), photolyzed in the aqueous solution, and the extent of change in the molecular level composition of the material is assessed with high-resolution mass spectrometry (HR-MS). The outcome of this study will be improved understanding of the role of condensed-phase photochemistry in chemical aging of aerosol particles and cloud droplets. Bateman et

  16. Predicting the mineral composition of dust aerosols - Part 2: Model evaluation and identification of key processes with observations

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

    A global compilation from nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match those of the soil. The MMT is based upon soil measurements after wet sieving, where soil aggregates are broken into smaller particles. The second method approximately reconstructs the aggregates and size distribution of the original soil that is subject to wind erosion. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observation. Only the AMF method restores phyllosilicate mass to silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in closer agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at separate clay and silt particle sizes are shown to be more useful for evaluation of the models, compared to the sum over all particles sizes that is susceptible to compensating errors in the SMF experiment. Model errors suggest that apportionment of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining uncertainty. Substantial uncertainty remains in evaluating both models and the MMT due to the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

  17. Impact of the North Atlantic Oscillation on the variations of aerosol ground levels through local processes over Europe

    NASA Astrophysics Data System (ADS)

    Jerez, S.; Jimenez-Guerrero, P.; Montávez, J. P.; Trigo, R. M.

    2013-05-01

    This contribution assesses non-antropogenic variations in ground-level aerosol concentrations over Europe associated to changes in the phase of the North Atlantic Oscillation (NAO). The NAO controls a large amount of the European climate variability with asymmetric impacts in both time and space. Based on simulated data and focusing on how the local atmospheric processes (without considering large-scale mechanisms) governed by the NAO affect the levels of various aerosol species, this study highlights that positive NAO phases favor increased aerosols levels in southern (northern) regions in winter (summer), while negative NAO phases enhance them in northern (southern) regions in winter (summer). Variations are up to and over 100% for most aerosols, being clearly related to the NAO-impact on precipitation and wind, as they act to clean the atmosphere through removal and dispersion processes, and to the NAO-impact on the radiation balance (i.e. cloudiness) as it rebounds on the biogenic emitting activity and on the oxidative capacity of the atmosphere. Beyond deepening on the understanding of fundamental interactions between climate and air quality, these results provide a basis for improving the potential predictability of this later since much work is being done in order to gain accuracy in the NAO predictions.

  18. Airborne observations of aerosol microphysical properties and particle ageing processes in the troposphere above Europe

    NASA Astrophysics Data System (ADS)

    Hamburger, T.; McMeeking, G.; Minikin, A.; Petzold, A.; Coe, H.; Krejci, R.

    2012-08-01

    In-situ measurements of aerosol microphysical properties were performed in May 2008 during the EUCAARI-LONGREX campaign. Two aircraft, the FAAM BAe-146 and DLR Falcon 20, operated from Oberpfaffenhofen, Germany. A comprehensive data set was obtained comprising the wider region of Europe north of the Alps throughout the whole tropospheric column. Prevailing stable synoptic conditions enabled measurements of accumulating emissions inside the continental boundary layer reaching a maximum total number concentration of 19 000 particles cm-3 stp. Nucleation events were observed within the boundary layer during high pressure conditions and after updraft of emissions induced by frontal passages above 8 km altitude in the upper free troposphere. Aerosol ageing processes during air mass transport are analysed using trajectory analysis. The ratio of particles containing a non-volatile core (250 °C) to the total aerosol number concentration was observed to increase within the first 12 to 48 h from the particle source from 50 to 85% due to coagulation. Aged aerosol also features an increased fraction of accumulation mode particles of approximately 40% of the total number concentration. The presented analysis provides an extensive data set of tropospheric aerosol microphysical properties on a continental scale which can be used for atmospheric aerosol models and comparisons of satellite retrievals.

  19. Airborne observations of aerosol microphysical properties and particle ageing processes in the troposphere above Europe

    NASA Astrophysics Data System (ADS)

    Hamburger, T.; McMeeking, G.; Minikin, A.; Petzold, A.; Coe, H.; Krejci, R.

    2012-12-01

    In-situ measurements of aerosol microphysical properties were performed in May 2008 during the EUCAARI-LONGREX campaign. Two aircraft, the FAAM BAe-146 and DLR Falcon 20, operated from Oberpfaffenhofen, Germany. A comprehensive data set was obtained comprising the wider region of Europe north of the Alps throughout the whole tropospheric column. Prevailing stable synoptic conditions enabled measurements of accumulating emissions inside the continental boundary layer reaching a maximum total number concentration of 19 000 particles cm-3 stp. Ultra-fine particles as indicators for nucleation events were observed within the boundary layer during high pressure conditions and after updraft of emissions induced by frontal passages above 8 km altitude in the upper free troposphere. Aerosol ageing processes during air mass transport are analysed using trajectory analysis. The ratio of particles containing a non-volatile core (250 °C) to the total aerosol number concentration was observed to increase within the first 12 to 48 h from the particle source from 50 to 85% due to coagulation. Aged aerosol also features an increased fraction of accumulation mode particles of approximately 40% of the total number concentration. The presented analysis provides an extensive data set of tropospheric aerosol microphysical properties on a continental scale which can be used for atmospheric aerosol models and comparisons of satellite retrievals.

  20. A study of remotely sensed aerosol properties from ground-based sun and sky scanning radiometers

    NASA Astrophysics Data System (ADS)

    Giles, David M.

    Aerosol particles impact human health by degrading air quality and affect climate by heating or cooling the atmosphere. The Indo-Gangetic Plain (IGP) of Northern India, one of the most populous regions in the world, produces and is impacted by a variety of aerosols including pollution, smoke, dust, and mixtures of them. The NASA Aerosol Robotic Network (AERONET) mesoscale distribution of Sun and sky-pointing instruments in India was established to measure aerosol characteristics at sites across the IGP and around Kanpur, India, a large urban and industrial center in the IGP, during the 2008 pre-monsoon (April-June). This study focused on detecting spatial and temporal variability of aerosols, validating satellite retrievals, and classifying the dominant aerosol mixing states and origins. The Kanpur region typically experiences high aerosol loading due to pollution and smoke during the winter and high aerosol loading due to the addition of dust to the pollution and smoke mixture during the pre-monsoon. Aerosol emissions in Kanpur likely contribute up to 20% of the aerosol loading during the pre-monsoon over the IGP. Aerosol absorption also increases significantly downwind of Kanpur indicating the possibility of the black carbon emissions from aerosol sources such as coal-fired power plants and brick kilns. Aerosol retrievals from satellite show a high bias when compared to the mesoscale distributed instruments around Kanpur during the pre-monsoon with few high quality retrievals due to imperfect aerosol type and land surface characteristic assumptions. Aerosol type classification using the aerosol absorption, size, and shape properties can identify dominant aerosol mixing states of absorbing dust and black carbon particles. Using 19 long-term AERONET sites near various aerosol source regions (Dust, Mixed, Urban/Industrial, and Biomass Burning), aerosol absorption property statistics are expanded upon and show significant differences when compared to previous work

  1. Accelerated simulation of stochastic particle removal processes in particle-resolved aerosol models

    NASA Astrophysics Data System (ADS)

    Curtis, J. H.; Michelotti, M. D.; Riemer, N.; Heath, M. T.; West, M.

    2016-10-01

    Stochastic particle-resolved methods have proven useful for simulating multi-dimensional systems such as composition-resolved aerosol size distributions. While particle-resolved methods have substantial benefits for highly detailed simulations, these techniques suffer from high computational cost, motivating efforts to improve their algorithmic efficiency. Here we formulate an algorithm for accelerating particle removal processes by aggregating particles of similar size into bins. We present the Binned Algorithm for particle removal processes and analyze its performance with application to the atmospherically relevant process of aerosol dry deposition. We show that the Binned Algorithm can dramatically improve the efficiency of particle removals, particularly for low removal rates, and that computational cost is reduced without introducing additional error. In simulations of aerosol particle removal by dry deposition in atmospherically relevant conditions, we demonstrate about 50-times increase in algorithm efficiency.

  2. Laboratory studies of thin films representative of atmospheric sulfate aerosol

    NASA Astrophysics Data System (ADS)

    Fortin, Tara Jean

    Sulfate aerosols are present globally in both the upper troposphere and lower stratosphere. These aerosols are of great interest because they have a profound influence on Earth's radiation balance, heterogeneous chemistry, and cloud formation mechanisms throughout the atmosphere. The magnitude of these effects is ultimately determined by the size, phase, and chemical composition of the aerosols themselves. This thesis explores some of the questions that remain concerning the phase of these aerosols under atmospheric conditions and the effects of their chemical composition on heterogeneous chemistry and cloud formation mechanisms. In the upper troposphere, cirrus clouds are thought to form via the homogeneous nucleation of ice out of dilute sulfate aerosols such as ammonium sulfate ((NH4)2SO4). To investigate this, the low-temperature phase behavior of ammonium sulfate films has been studied using Fourier transform infrared (FTIR) spectroscopy. Experiments performed as a function of increasing relative humidity demonstrate that a phase transition from crystalline (NH 4)2SO4 to a metastable aqueous solution can occur at temperatures below the eutectic at 254 K. However, on occasion, direct deposition of ice from the vapor phase was observed, possibly indicating selective heterogeneous nucleation. In addition to serving as nuclei for cirrus clouds, sulfate aerosols can participate in heterogeneous reactions. The interaction of HNO3 with ammonium sulfate has been investigated as a possible loss mechanism for gas-phase HNO3 using a Knudsen cell reactor coupled with transmission FTIR spectroscopy. The results show that HNO3 reacts with solid ammonium sulfate to produce ammonium nitrate and letovicite at 203 K. Furthermore, this reaction is enhanced as a function of relative humidity from 0 to 41%. In the lower stratosphere, polar stratospheric clouds (PSCs) are important for springtime ozone depletion. The vapor deposition of ice on sulfuric acid tetrahydrate (SAT) has

  3. Studies of Ice Nucleating Aerosol Particles in Arctic Cloud Systems

    NASA Technical Reports Server (NTRS)

    Rogers, David C.; DeMott, Paul J.; Kreidenweis, Sonia M.

    2001-01-01

    The focus of this research is to improve the understanding of ice nucleating aerosol particles (IN) and the role they play in ice formation in Arctic clouds. IN are important for global climate issues in a variety of ways. The primary effect is their role in determining the phase (liquid or solid) of cloud particles. The microscale impact is on cloud particle size, growth rate, shape, fall speed, concentration, radiative properties, and scavenging of gases and aerosols. On a larger scale, ice formation affects the development of precipitation (rate, amount, type, and distribution), latent heat release (rate and altitude), ambient humidity, the persistence of clouds, and cloud albedo. The overall goals of our FIRE 3 research are to characterize the concentrations and variability of Arctic IN during the winter-spring transition, to compare IN measurements with ice concentrations in Arctic clouds, and to examine selected IN samples for particle morphology and chemical there are distinguishable chemical signatures. The results can be combined with other measurements of aerosols, gaseous species, and cloud characteristics in order to understand the processes that determine the phase and concentration of cloud particles.

  4. New understanding and quantification of the regime dependence of aerosol-cloud interaction for studying aerosol indirect effects

    DOE PAGES

    Chen, Jingyi; Liu, Yangang; Zhang, Minghua; Peng, Yiran

    2016-02-28

    In this study, aerosol indirect effects suffer from large uncertainty in climate models and among observations. This study focuses on two plausible factors: regime dependence of aerosol-cloud interactions and the effect of cloud droplet spectral shape. We show, using a new parcel model, that combined consideration of droplet number concentration (Nc) and relative dispersion (ε, ratio of standard deviation to mean radius of the cloud droplet size distribution) better characterizes the regime dependence of aerosol-cloud interactions than considering Nc alone. Given updraft velocity (w), ε increases with increasing aerosol number concentration (Na) in the aerosol-limited regime, peaks in the transitionalmore » regime, and decreases with further increasing Na in the updraft-limited regime. This new finding further reconciles contrasting observations in literature and reinforces the compensating role of dispersion effect. The nonmonotonic behavior of ε further quantifies the relationship between the transitional Na and w that separates the aerosol- and updraft-limited regimes.« less

  5. Process-model simulations of cloud albedo enhancement by aerosols in the Arctic.

    PubMed

    Kravitz, Ben; Wang, Hailong; Rasch, Philip J; Morrison, Hugh; Solomon, Amy B

    2014-12-28

    A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN), either through geoengineering or other increased sources of Arctic aerosols. An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus, the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation owing to precipitation changes are small. According to these results, which are dependent upon the representation of ice nucleation processes in the employed microphysical scheme, Arctic geoengineering is unlikely to be effective as the sole means of altering the global radiation budget but could have substantial local radiative effects.

  6. The Impact of Detailed Urban Scale Processing on the Simulation of the Concentration and Distribution of Aerosols in Asia

    NASA Astrophysics Data System (ADS)

    Cohen, J. B.; Wang, C.; Prinn, R. G.

    2009-12-01

    The chemical and physical processing of aerosols and their precursors at the urban scale is highly non-linear. Yet, global scale models use a simple dilution and processing approach, wherein they use the grid-box average or some statistical approach to determine what the actual concentrations and distributions of aerosols and their precursors are on the urban scale. To achieve a more realistic representation of the fast processing that occurs on the sub-grid scale, we have updated and extended the approach of Mayer et al. [2000]. This new approach uses the Comprehensive Air Pollution Model with Extensions (CAMx) which takes into account detailed chemical, physical, meteorological, and anthropogenic factors that control the emissions and processing of not only gas-phase species, but also aerosols and their precursors (including BC, OC, SOA, SO2, H2SO4, and sulfate aerosol). Additionally, this approach has been applied in such a way that urban areas have been separately modeled for different regions, with different representations currently available for urban regions in China, India, Developing Nations (such as those found in South East Asia), and Developed Nations (such as Japan). This detailed urban process model has been successfully integrated into the interactive climate and aerosol model developed at MIT, based on CAM3 [Kim et al. 2008]. The combined model can be used globally, but this study has a specific emphasis on the results and impacts of the urban scale processing occurring throughout Asia. This is of particularly importance, since the most effective way to demonstrate the importance of including detailed urban processing is to apply it to Asia, which is the continent with the most number and highest density of large urban areas. Different approximations of the emissions from urban areas (such as those from the MIT Joint Program on the Science and Policy of Global Change and Index-B) are also considered within this context. The point of this modeling

  7. Laboratory photochemical processing of aqueous aerosols: formation and degradation of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls

    NASA Astrophysics Data System (ADS)

    Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Swaminathan, T.

    2015-07-01

    To better understand the photochemical processing of dicarboxylic acids and related polar compounds, we conducted batch UV irradiation experiments on two types of aerosol samples collected from India, which represent anthropogenic (AA) and biogenic (BA) aerosols, for time periods of 0.5 to 120 h. The irradiated samples were analyzed for molecular compositions of diacids, oxoacids and α-dicarbonyls. The results show that photochemical degradation of oxalic (C2), malonic (C3) and other C8-C12 diacids overwhelmed their production in aqueous aerosols, whereas succinic acid (C4) and C5-C7 diacids showed a significant increase (ca. 10 times) during the course of irradiation experiments. The photochemical formation of oxoacids and α-dicarbonyls overwhelmed their degradation during the early stages of experiment except for ω-oxooctanoic acid (ωC8), which showed a similar pattern to that of C4. We also found a gradual decrease in the relative abundance of C2 to total diacids and an increase in the relative abundance of C4 during prolonged experiment. Based on the changes in concentrations and mass ratios of selected species with the irradiation time, we hypothesize that iron-catalyzed photolysis of C2 and C3 diacids controls their concentrations in Fe-rich atmospheric waters, whereas photochemical formation of C4 diacid (via ωC8) is enhanced with photochemical processing of aqueous aerosols in the atmosphere. This study demonstrates that the ambient aerosols contain abundant precursors that produce diacids, oxoacids and α-dicarbonyls, although some species such as oxalic acid decompose extensively during an early stage of photochemical processing.

  8. Laboratory photochemical processing of aqueous aerosols: formation and degradation of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls

    NASA Astrophysics Data System (ADS)

    Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Swaminathan, T.

    2015-01-01

    To better understand the photochemical processing of dicarboxylic acids and related polar compounds, we conducted batch UV irradiation experiments on two types of aerosol samples collected from India, which represent anthropogenic (AA) and biogenic aerosols (BA), for time periods of 0.5 to 120 h. The irradiated samples were analyzed for molecular compositions of diacids, oxoacids and α-dicarbonyls. The results show that photochemical degradation of oxalic (C2) and malonic (C3) and other C8-C12 diacids overwhelmed their production in aqueous aerosols whereas succinic acid (C4) and C5-C7 diacids showed a significant increase (ca. 10 times) during the course of irradiation experiments. The photochemical formation of oxoacids and α-dicarbonyls overwhelmed their degradation during the early stages of experiment, except for ω-oxooctanoic acid (ωC8) that showed a similar pattern to that of C4. We also found a gradual decrease in the relative abundance of C2 to total diacids and an increase in the relative abundance of C4 during prolonged experiment. Based on the changes in concentrations and mass ratios of selected species with the irradiation time, we hypothesize that iron-catalyzed photolysis of C2 and C3 diacids dominates their concentrations in Fe-rich atmospheric waters, whereas photochemical formation of C4 diacid (via ωC8) is enhanced with photochemical processing of aqueous aerosols in the atmosphere. This study demonstrates that the ambient aerosols contain abundant precursors that produce diacids, oxoacids and α-dicarbonyls, although some species such as oxalic acid decompose extensively during an early stage of photochemical processing.

  9. North Atlantic Oscillation affecting aerosols ground levels over Europe through local processes: asymmetries in time and space

    NASA Astrophysics Data System (ADS)

    Jerez, Sonia; Jimenez-Guerrero, Pedro; Montávez, Juan Pedro; Trigo, Ricardo M.

    2013-04-01

    Air pollution is a major environmental and health problem. Hence, understanding when and why episodes of air pollution arise becomes essential. Besides emissions, air pollution levels depend on the atmospheric conditions handling and transforming them through processes related to chemistry, transport and removal. In this sense, this contribution assesses the variation in ground-level aerosols concentrations over Europe associated to changes in the phase of the North Atlantic Oscillation (NAO) motivated by the well-known strong impact of the NAO on the European climate variability. For that we used a high-resolution (25 km) air quality simulation spanning the period 1970-1999 and covering western Europe and most of the Mediterranean basin. Additionally, we used observed aerosol data from the EMEP database whose observational periods range between 1993 and 2010. The simulation was performed by using climatological boundary conditions for the aerosols concentrations, hence allowing to isolate the influence of the local atmospheric processes, as they are governed by the NAO, on the levels of the various aerosol species analyzed (namely sea salt, wind-blown and resuspended dust, secondary inorganic aerosols, organic matter and elemental carbon) from the influence of large-scale mechanisms. The results highlight that positive NAO phases favor increased aerosols levels in southern (northern) regions in winter (summer), while negative NAO phases enhance them in northern (southern) regions in winter (summer), being generally in good agreement with the analysis based on the observational database. Variations are up to and over 100% for most aerosols, being clearly related to the NAO-impact on local precipitation and wind, as they act to clean the atmosphere through removal and dispersion processes, but equally resulting from the NAO-impact on the radiation balance (i.e. cloudiness) as it rebounds on the biogenic emitting activity and on the oxidative capacity of the

  10. [Characteristics of Number Concentration Size Distributions of Aerosols Under Processes in Beijing].

    PubMed

    Su, Jie; Zhao, Pu-sheng; Chen, Yi-na

    2016-04-15

    The aerosol number concentration size distributions were measured by a Wide-Range Particle Spectrometer (WPS-1000XP) at an urban site of Beijing from 2012 to 2014; and the characteristics of the size distributions in different seasons and weather conditions were discussed. The results showed that the daily average number concentration of Aitken mode aerosols was highest in the spring and lowest in the autumn; the daily average number concentration of accumulation mode aerosols was bigher in the spring and winter, while lowest in summer; and the average concentration of coarse mode was highest during the winter. The Aitken mode particles had the most significant diurnal variations resulted from the traffic sources and the summer photochemical reactions. In the spring, autumn and winter, the number concentrations of accumulation mode of the nighttime was higher than that of the daytime. The coarse mode particles did not have obvious diurnal variation. During the heavy pollution process, the accumulation mode aerosols played a decisive role in PM₂.₅ concentrations and was usually removed by the north wind. The precipitation could effectively eliminate the coarse mode particles, but it bad no obvious effect on the accumulation mode particles under small speed wind and zero speed wind. During the dust process, the concentrations of coarse mode particles increased significantly, while the accumulation mode aerosol concentration was obviously decreased. PMID:27548939

  11. Studies of seasonal variations of aerosol optical properties with use of remote techniques

    NASA Astrophysics Data System (ADS)

    Strzalkowska, Agata; Zielinski, Tymon; Petelski, Tomasz; Pakszys, Paulina; Markuszewski, Piotr; Makuch, Przemyslaw

    2014-05-01

    According to the IPCC report, atmospheric aerosols due to their properties -extinction of Sun and Earth radiation and participation in processes of creation of clouds, are among basic "unknowns" in climate studies. Aerosols have large effect on the radiation balance of the Earth which has a significant impact on climate changes. They are also a key issue in the case of remote sensing measurements. The optical properties of atmospheric aerosols depend not only on their type but also on physical parameters such as pressure, humidity, wind speed and direction. The wide range of properties in which atmospheric aerosols affect Earth's climate is the reason of high unrelenting interest of scientists from different disciplines such as physics, chemistry and biology. Numerous studies have dealt with aerosol optical properties, e.g. Dubovik et al. (2002), but only in a few have regarded the influence of meteorological parameters on the optical properties of aerosols in the Baltic Sea area. Studies of aerosol properties over the Baltic were conducted already in the last forty years, e.g. Zielinski T. et. al. (1999) or Zielinski T. & A. Zielinski (2002). The experiments carried out at that time involved only one measuring instrument -e.g. LIDAR (range of 1 km) measurements and they were conducted only in selected areas of the Polish coastal zone. Moreover in those publications authors did not use measurements performed on board of research vessel (R/V Oceania), which belongs to Institute of Oceanology Polish Academy of Science (IO PAN) or data received from satellite measurements. In 2011 Zdun and Rozwadowska performed an analysis of all data derived from the AERONET station on the Gotland Island. The data were divided into seasons and supplemented by meteorological factors. However, so far no comprehensive study has been carried out for the entire Baltic Sea area. This was the reason to conduct further research of SEasonal Variations of Aerosol optical depth over the Baltic

  12. 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

  13. Functional group composition of organic aerosol from combustion emissions and secondary processes at two contrasted urban environments

    NASA Astrophysics Data System (ADS)

    El Haddad, Imad; Marchand, Nicolas; D'Anna, Barbara; Jaffrezo, Jean Luc; Wortham, Henri

    2013-08-01

    The quantification of major functional groups in atmospheric organic aerosol (OA) provides a constraint on the types of compounds emitted and formed in atmospheric conditions. This paper presents functional group composition of organic aerosol from two contrasted urban environments: Marseille during summer and Grenoble during winter. Functional groups were determined using a tandem mass spectrometry approach, enabling the quantification of carboxylic (RCOOH), carbonyl (RCOR‧), and nitro (RNO2) functional groups. Using a multiple regression analysis, absolute concentrations of functional groups were combined with those of organic carbon derived from different sources in order to infer the functional group contents of different organic aerosol fractions. These fractions include fossil fuel combustion emissions, biomass burning emissions and secondary organic aerosol (SOA). Results clearly highlight the differences between functional group fingerprints of primary and secondary OA fractions. OA emitted from primary sources is found to be moderately functionalized, as about 20 carbons per 1000 bear one of the functional groups determined here, whereas SOA is much more functionalized, as in average 94 carbons per 1000 bear a functional group under study. Aging processes appear to increase both RCOOH and RCOR‧ functional group contents by nearly one order of magnitude. Conversely, RNO2 content is found to decrease with photochemical processes. Finally, our results also suggest that other functional groups significantly contribute to biomass smoke and SOA. In particular, for SOA, the overall oxygen content, assessed using aerosol mass spectrometer measurements by an O:C ratio of 0.63, is significantly higher than the apparent O:C* ratio of 0.17 estimated based on functional groups measured here. A thorough examination of our data suggests that this remaining unexplained oxygen content can be most probably assigned to alcohol (ROH), organic peroxides (ROOH

  14. Studies of toxic aerosols via elastic and inelastic light scattering

    SciTech Connect

    Foss, W.; Li, W.; Allen, T.M.; Blair, D.S.; Davis, E.J. )

    1993-02-01

    Evaporation rates and chemical characteristics of potentially toxic aerosols have been determined by elastic and inelastic light-scattering measurements. The aerosol systems examined were a commercial catalyst consisting of a mixture of stannous octanoate (SNO) and 2-ethylhexanoic acid (EHA) and droplets emitted from open tanks of chromic acid solutions used for anodizing aluminum. The heavy metals contained in these aerosols represent a danger to the workplace if such materials are inhaled. Nanogram amounts of the solutions were studied by suspending single microdroplets in electrodynamic balances in a flow of air to measure evaporation rates and to obtain Raman spectra. Elastic scattering data include phase functions and morphological resonance spectra from which droplet sizes are determined. The inelastic light-scattering data or Raman spectra provide molecular vibrational bond information. It was found that EHA spectra agree with bulk data in the literature, and that SNO Raman spectra, which are not available in the literature, are consistent with infrared spectra for bulk SNO. At room temperature the vapor pressure of SNO is on the order of 0.01 Pa while that of EHA is on the order of 0.1 Pa. Raman data for the residue of evaporated chromic acid solutions show the presence of chromium oxides (Cr[sup 6+] compounds), surfactants, and bound (nonvolatile) water. 31 refs., 14 figs.

  15. NORTHERN OHIO AEROSOL STUDY: STAPHYLOCOCCUS AUREUS EVALUATION

    EPA Science Inventory

    A consortium of Universities, located in northwest Ohio have received funds to conduct a comprehensive evaluation of land applied biosolids in that state. This USDA funded study includes observing land application practices and evaluating biosolids, soils, runoff water and bioaer...

  16. Impacts of Combustion Conditions and Photochemical Processing on the Light Absorption of Biomass Combustion Aerosol.

    PubMed

    Martinsson, J; Eriksson, A C; Nielsen, I Elbæk; Malmborg, V Berg; Ahlberg, E; Andersen, C; Lindgren, R; Nyström, R; Nordin, E Z; Brune, W H; Svenningsson, B; Swietlicki, E; Boman, C; Pagels, J H

    2015-12-15

    The aim was to identify relationships between combustion conditions, particle characteristics, and optical properties of fresh and photochemically processed emissions from biomass combustion. The combustion conditions included nominal and high burn rate operation and individual combustion phases from a conventional wood stove. Low temperature pyrolysis upon fuel addition resulted in "tar-ball" type particles dominated by organic aerosol with an absorption Ångström exponent (AAE) of 2.5-2.7 and estimated Brown Carbon contributions of 50-70% to absorption at the climate relevant aethalometer-wavelength (520 nm). High temperature combustion during the intermediate (flaming) phase was dominated by soot agglomerates with AAE 1.0-1.2 and 85-100% of absorption at 520 nm attributed to Black Carbon. Intense photochemical processing of high burn rate flaming combustion emissions in an oxidation flow reactor led to strong formation of Secondary Organic Aerosol, with no or weak absorption. PM1 mass emission factors (mg/kg) of fresh emissions were about an order of magnitude higher for low temperature pyrolysis compared to high temperature combustion. However, emission factors describing the absorption cross section emitted per kg of fuel consumed (m(2)/kg) were of similar magnitude at 520 nm for the diverse combustion conditions investigated in this study. These results provide a link between biomass combustion conditions, emitted particle types, and their optical properties in fresh and processed plumes which can be of value for source apportionment and balanced mitigation of biomass combustion emissions from a climate and health perspective. PMID:26561964

  17. Impacts of Combustion Conditions and Photochemical Processing on the Light Absorption of Biomass Combustion Aerosol.

    PubMed

    Martinsson, J; Eriksson, A C; Nielsen, I Elbæk; Malmborg, V Berg; Ahlberg, E; Andersen, C; Lindgren, R; Nyström, R; Nordin, E Z; Brune, W H; Svenningsson, B; Swietlicki, E; Boman, C; Pagels, J H

    2015-12-15

    The aim was to identify relationships between combustion conditions, particle characteristics, and optical properties of fresh and photochemically processed emissions from biomass combustion. The combustion conditions included nominal and high burn rate operation and individual combustion phases from a conventional wood stove. Low temperature pyrolysis upon fuel addition resulted in "tar-ball" type particles dominated by organic aerosol with an absorption Ångström exponent (AAE) of 2.5-2.7 and estimated Brown Carbon contributions of 50-70% to absorption at the climate relevant aethalometer-wavelength (520 nm). High temperature combustion during the intermediate (flaming) phase was dominated by soot agglomerates with AAE 1.0-1.2 and 85-100% of absorption at 520 nm attributed to Black Carbon. Intense photochemical processing of high burn rate flaming combustion emissions in an oxidation flow reactor led to strong formation of Secondary Organic Aerosol, with no or weak absorption. PM1 mass emission factors (mg/kg) of fresh emissions were about an order of magnitude higher for low temperature pyrolysis compared to high temperature combustion. However, emission factors describing the absorption cross section emitted per kg of fuel consumed (m(2)/kg) were of similar magnitude at 520 nm for the diverse combustion conditions investigated in this study. These results provide a link between biomass combustion conditions, emitted particle types, and their optical properties in fresh and processed plumes which can be of value for source apportionment and balanced mitigation of biomass combustion emissions from a climate and health perspective.

  18. A New WRF-Chem Treatment for Studying Regional Scale Impacts of Cloud-Aerosol Interactions in Parameterized Cumuli

    SciTech Connect

    Berg, Larry K.; Shrivastava, ManishKumar B.; Easter, Richard C.; Fast, Jerome D.; Chapman, Elaine G.; Liu, Ying

    2015-01-01

    A new treatment of cloud-aerosol interactions within parameterized shallow and deep convection has been implemented in WRF-Chem that can be used to better understand the aerosol lifecycle over regional to synoptic scales. The modifications to the model to represent cloud-aerosol interactions include treatment of the cloud dropletnumber mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. Thesechanges have been implemented in both the WRF-Chem chemistry packages as well as the Kain-Fritsch cumulus parameterization that has been modified to better represent shallow convective clouds. Preliminary testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS) as well as a high-resolution simulation that does not include parameterized convection. The simulation results are used to investigate the impact of cloud-aerosol interactions on the regional scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column integrated BC can be as large as -50% when cloud-aerosol interactions are considered (due largely to wet removal), or as large as +35% for sulfate in non-precipitating conditions due to the sulfate production in the parameterized clouds. The modifications to WRF-Chem version 3.2.1 are found to account for changes in the cloud drop number concentration (CDNC) and changes in the chemical composition of cloud-drop residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to WRF-Chem version 3.5, and it is anticipated that they

  19. Climate effects of anthropogenic aerosols over East Asia based on modeling study

    NASA Astrophysics Data System (ADS)

    Mukai, Makiko

    The increasing emission of anthropogenic aerosols causes serious air pollution episodes and various effects on the climate by the aerosols interacting with the radiation budget by directly absorbing and scattering the solar radiation, and by them indirectly modifying the optical properties and lifetimes of clouds. In East Asia anthropogenic aerosol concentrations are rapidly increasing. It is therefore necessary to evaluate the sensitivity of anthropogenic aerosols upon the radiative forcing in this region. For this purpose we utilize an atmospheric general circulation model (AGCM) with an aerosol transport and radiation model and an ocean mixed-layer model. The model in this study was a three-dimensional aerosol transport-radiation model (SPRINTARS), driven by the AGCM developed by CCSR (Center for Climate System Research), NIES (National Institute for Environmental Studies), and FRCGC (Frontier Research Center for Global Change). This model incorporates sulfate, carbonaceous, sea salt, and mineral dust aerosols, the first three of which are assumed to acts as cloud condensation nuclei that generate cloud droplets whose number increases with the number of nuclei. We assumed sulfate and carbonaceous aerosol from fuel burning for anthropogenic aerosol. And the model simulations of equilibrium experiments were performed to investigate the impact of anthropogenic aerosols based on present-day emission data and the preindustrial-era emission data. Our simulation results showed that copious anthropogenic aerosol loading causes significant decrease in the surface downward shortwave radiation flux (SDSWRF), which indicates that a direct effect of aerosols has the greatest influence on the surface radiation. It is found from our model simulations that low-level clouds increase but convective clouds decrease due to reduced convective activity caused by surface cooling when anthropogenic aerosol increases. It was also found that the contributions of aerosols to the radiation

  20. Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

  1. Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, coating by heterogeneous uptake of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the resulting aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent in a soil whose aggregates are dispersed by wet sieving during analysis. We reconstruct the undispersed size distribution of the original soil that is subject to wind erosion. An empirical constraint upon the relative emission of clay and silt is applied that further differentiates the soil and aerosol mineral composition. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the extension brings the model into better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

  2. Predicting the Mineral Composition of Dust Aerosols. Part 1; Representing Key Processes

    NASA Technical Reports Server (NTRS)

    Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

    2015-01-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

  3. Aerosol-cloud closure study using RPAS measurements

    NASA Astrophysics Data System (ADS)

    Calmer, R.; Roberts, G.; Sanchez, K. J.; Nicoll, K.; Preissler, J.; Ovadnevaite, J.; Sciare, J.; Bronz, M.; Hattenberger, G.; Rosenfeld, D.; Lauda, S.; Hashimshoni, E.

    2015-12-01

    Enhancements in Remotely Piloted Aircraft Systems (RPAS) have increased their possible uses in many fields for the past two decades. For atmospheric research, ultra-light RPAS (< 2.5kg) are now able to fly at altitudes greater than 3 km and even in cloud, which opens new opportunities to understand aerosol-cloud interactions. We are deploying the RPAS as part of the European project BACCHUS (Impact of Biogenic versus Anthropogenic Emissions on Clouds and Climate: towards a Holistic Understanding). Field experiments in Cyprus and Ireland have already been conducted to study aerosol-cloud interactions in climatically different environments. The RPAS are being utilized in this study with the purpose of complementing ground-based observations of cloud condensation nuclei (CCN) to conduct aerosol-cloud closure studies Cloud microphysical properties such as cloud drop number concentration and size can be predicted directly from the measured CCN spectrum and the observed updraft, the vertical component of the wind vector [e.g., Conant et al, 2004]. On the RPAS, updraft measurements are obtained from a 5-hole probe synchronized with an Inertial Measurement Unit (IMU). The RPA (remotely piloted aircraft) are programmed to fly at a level leg just below cloud base to measure updraft measurements while a scanning CCN counter is stationed at ground level. Vertical profiles confirm that CCN measurements on the ground are representative to those at cloud base. An aerosol-cloud parcel model is implemented to model the cloud droplet spectra associated with measured updraft velocities. The model represents the particle size domain with internally mixed chemical components, using a fixed-sectional approach [L. M. Russell and Seinfeld, 1998]. The model employs a dual moment (number and mass) algorithm to calculate growth of particles from one section to the next for non-evaporating species. Temperature profiles, cloud base, updraft velocities and aerosol size and composition, all

  4. Use of ARM Mobile Facility (AMF) Data to Study Aerosol Indirect Effects in China

    SciTech Connect

    Li, Zhanqing

    2012-12-19

    General goals: 1) Facilitating the deployment of the ARM Mobile Facility (AMF) and Ancillary Facility (AAF) in China in 2008, 2) Processing, retrieving, improving and analyzing observation data from ground-based, air-borne and space-borne instruments; 3) Conducting a series of studies to gain insights into the direct and indirect effects of these aerosols on radiation, clouds, and precipitation using both

  5. DETROIT EXPOSURE AND AEROSOL RESEARCH STUDY

    EPA Science Inventory

    The DEARS is a three-year field monitoring study that will be conducted in Detroit, Michigan and is designed to measure exposure and describe exposure relationships for air toxics, PM components, PM from specific sources, and criteria pollutants. Detroit, Michigan was considered ...

  6. Using global aerosol models and satellite data for air quality studies: Challenges and data needs

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2006-01-01

    Aerosol particles, also known as PM2.5 (particle diameter less than 2.5 pm) and PM10 (particle diameter less than 10 pm), are one of the key atmospheric components that determines air quality. Yet, air quality forecasts for PM are still in their infancy and remain a challenging task. It is difficult to simply relate PM levels to local meteorological conditions, and large uncertainties exist in regional air quality model emission inventories and initial and boundary conditions. Especially challenging are periods when a significant amount of aerosol comes from outside the regional modeling domain through long-range transport. In the past few years, NASA has launched several satellites with global aerosol measurement capabilities, providing large-scale chemical weather pictures. NASA has also supported development of global models which simulate atmospheric transport and transformation processes of important atmospheric gas and aerosol species. I will present the current modeling and satellite capabilities for PM2.5 studies, the possibilities and challenges in using satellite data for PM2.5 forecasts, and the needs of future remote sensing data for improving air quality monitoring and modeling.

  7. Formation of Oxidized Organic Aerosol (OOA) through Fog Processing in the Po Valley

    NASA Astrophysics Data System (ADS)

    Gilardoni, S.; Paglione, M.; Rinaldi, M.; Giulianelli, L.; Massoli, P.; Hillamo, R. E.; Carbone, S.; Lanconelli, C.; Laaksonen, A. J.; Russell, L. M.; Poluzzi, V.; Fuzzi, S.; Facchini, C.

    2014-12-01

    Aqueous phase chemistry might be responsible for the formation of a significant fraction of the organic aerosol (OA) observed in the atmosphere, and could explain some of the discrepancies between OA concentration and properties predicted by models and observed in the environment. Aerosol - fog interaction and its effect on submicron aerosol properties were investigated in the Po Valley (northern Italy) during fall 2011, in the framework of the Supersite project (ARPA Emilia Romagna). Composition and physical properties of submicron aerosol were measured online by a High Resolution- Time of Flight - Aerosol Mass Spectrometer (HR-TOF-AMS), a Soot Photometer - Aerosol Mass Spectrometer (SP-AMS), and a Tandem Differential Mobility Particle Sizer (TDMPS). Organic functional group analysis was performed off-line by Hydrogen - Nuclear Magnetic Resonance (H-NMR) spectrometry and by Fourier Transform Infrared (FTIR) spectrometry. Aerosol absorption, scattering, and total extinction were measured simultaneously with a Particle Soot Absorption Photometer (PSAP), a Nephelometer, and a Cavity Attenuated Phase Shift Spectrometer particle extinction monitor (CAPS PMex), respectively. Water-soluble organic carbon in fog-water was characterized off-line by HR-TOF-AMS. Fourteen distinct fog events were observed. Fog dissipation left behind an aerosol enriched in particles larger than 400 nm, typical of fog and cloud processing, and dominated by secondary species, including ammonium nitrate, ammonium sulfate and oxidized OA (OOA). Source apportionment of OA allowed us to identify OOA as the difference between total OA and primary OA (hydrocarbon like OA and biomass burning OA). The formation of OOA through fog processing is proved by the correlation of OOA concentration with hydroxyl methyl sulfonate signal and by the similarity of OOA spectra with organic mass spectra obtained by re-aerosolization of fog water samples. The oxygen to carbon ratio and the hydrogen to carbon ratio of

  8. Optical and Hygroscopic Studies of Aerosols In Simulated Planetary Atmospheres

    NASA Astrophysics Data System (ADS)

    Hasenkopf, Christa A.

    2011-08-01

    Basic characteristics of the early Earth climate, the only known environment in the Universe in which life has been known to emerge and thrive, remain a mystery. In particular, little is understood about the Earth's atmosphere 2.8 billion years ago. From climate models and laboratory studies, it is postulated that an organic haze, much like that found on Saturn's largest moon Titan, covered the early Earth. This haze, generated from photolysis of carbon dioxide (CO2) and methane (CH4), may have had profound climatic consequences. Climate models of the early Earth that include this haze have had to rely upon optical properties of a Titan laboratory analog. Titan haze, though thought to be similar, is formed from a different combination of precursor gases and by different energy sources than early Earth haze. This thesis examines the direct and indirect radiative effects of aerosol on early Earth climate by studying the optical and hygroscopic properties of a laboratory analog. A Titan analog is studied for comparison and to better understand spacecraft-retrieved haze chemical and optical properties from Titan. The properties of the laboratory analogs, generated in a flowing reactor cell with a continuum ultraviolet (UV) light source, were primarily measured using cavity ringdown aerosol extinction spectroscopy and UV-visible (UV-Vis) transmission spectroscopy. We find that the optical properties of our early Earth analog are significantly different than those of the Titan analog from Khare et al. (1984). In both the UV and visible, when modeled as fractals, particles with the optical properties of the early Earth analog have approximately 30% larger extinction efficiencies than particles with Khare et al. (1984) values. This result implies our early Earth haze analog would provide a more efficient UV shield and have a stronger antigreenhouse effect than the Khare et al. (1984) Titan analog. Our Titan analog has significantly smaller imaginary refractive index values

  9. Ion balances of size-resolved tropospheric aerosol samples: implications for the acidity and atmospheric processing of aerosols

    NASA Astrophysics Data System (ADS)

    Kerminen, Veli-Matti; Hillamo, Risto; Teinilä, Kimmo; Pakkanen, Tuomo; Allegrini, Ivo; Sparapani, Roberto

    A large set of size-resolved aerosol samples was inspected with regard to their ion balance to shed light on how the aerosol acidity changes with particle size in the lower troposphere and what implications this might have for the atmospheric processing of aerosols. Quite different behaviour between the remote and more polluted environments could be observed. At the remote sites, practically the whole accumulation mode had cation-to-anion ratios clearly below unity, indicating that these particles were quite acidic. The supermicron size range was considerably less acidic and may in some cases have been close to neutral or even alkaline. An interesting feature common to the remote sites was a clear jump in the cation-to-anion ratio when going from the accumulation to the Aitken mode. The most likely reason for this was cloud processing which, via in-cloud sulphate production, makes the smallest accumulation-mode particles more acidic than the non-activated Aitken-mode particles. A direct consequence of the less acidic nature of the Aitken mode is that it can take up semi-volatile, water-soluble gases much easier than the accumulation mode. This feature may have significant implications for atmospheric cloud condensation nuclei production in remote environments. In rural and urban locations, the cation-to-anion ratio was close to unity over most of the accumulation mode, but increased significantly when going to either larger or smaller particle sizes. The high cation-to-anion ratios in the supermicron size range were ascribed to carbonate associated with mineral dust. The ubiquitous presence of carbonate in these particles indicates that they were neutral or alkaline, making them good sites for heterogeneous reactions involving acidic trace gases. The high cation-to-anion ratios in the Aitken mode suggest that these particles contained some water-soluble anions not detected by our chemical analysis. This is worth keeping in mind when investigating the hygroscopic

  10. 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.

  11. Integrated Analyses of Multiple Worldwide Aerosol Mass Spectrometer Datasets for Improved Understanding of Aerosol Sources and Processes and for Comparison with Global Models

    SciTech Connect

    Zhang, Qi; Jose, Jimenez Luis

    2014-04-28

    The AMS is the only current instrument that provides real-time, quantitative, and size-resolved data on submicron non-refractory aerosol species with a time resolution of a few minutes or better. The AMS field data are multidimensional and massive, containing extremely rich information on aerosol chemistry, microphysics and dynamics—basic information that is required to evaluate and quantify the radiative climate forcing of atmospheric aerosols. The high time resolution of the AMS data also reveals details of aerosol dynamic variations that are vital to understanding the physico-chemical processes of atmospheric aerosols that govern aerosol properties relevant to the climate. There are two primary objectives of this 3-year project. Our first objective is to perform highly integrated analysis of dozens of AMS datasets acquired from various urban, forested, coastal, marine, mountain peak, and rural/remote locations around the world and synthesize and inter-compare results with a focus on the sources and the physico-chemical processes that govern aerosol properties relevant to aerosol climate forcing. Our second objective is to support our collaboration with global aerosol modelers, in which we will supply the size-resolved aerosol composition and temporal variation data (via a public web interface) and our analysis results for use in model testing and validation and for translation of the rich AMS database into model constraints that can improve climate forcing simulations. Several prominent global aerosol modelers have expressed enthusiastic support for this collaboration. The specific tasks that we propose to accomplish include 1) to develop, validate, and apply multivariate analysis techniques for improved characterization and source apportionment of organic aerosols; 2) to evaluate aerosol source regions and relative contributions based on back-trajectory integration (PSCF method); 3) to summarize and synthesize submicron aerosol information, including

  12. Study of Mechanisms of Aerosol Indirect Effects on Glaciated Clouds: Progress during the Project Final Technical Report

    SciTech Connect

    None, None

    2013-10-18

    This 3-year project has studied how aerosol pollution influences glaciated clouds. The tool applied has been an 'aerosol-cloud model'. It is a type of Cloud-System Resolving Model (CSRM) modified to include 2-moment bulk microphysics and 7 aerosol species, as described by Phillips et al. (2009, 2013). The study has been done by, first, improving the model and then performing sensitivity studies with validated simulations of a couple of observed cases from ARM. These are namely the Tropical Warm Pool International Cloud Experiment (TWP-ICE) over the tropical west Pacific and the Cloud and Land Surface Interaction Campaign (CLASIC) over Oklahoma. During the project, sensitivity tests with the model showed that in continental clouds, extra liquid aerosols (soluble aerosol material) from pollution inhibited warm rain processes for precipitation production. This promoted homogeneous freezing of cloud droplets and aerosols. Mass and number concentrations of cloud-ice particles were boosted. The mean sizes of cloud-ice particles were reduced by the pollution. Hence, the lifetime of glaciated clouds, especially ice-only clouds, was augmented due to inhibition of sedimentation and ice-ice aggregation. Latent heat released from extra homogeneous freezing invigorated convective updrafts, and raised their maximum cloud-tops, when aerosol pollution was included. In the particular cases simulated in the project, the aerosol indirect effect of glaciated clouds was twice than of (warm) water clouds. This was because glaciated clouds are higher in the troposphere than water clouds and have the first interaction with incoming solar radiation. Ice-only clouds caused solar cooling by becoming more extensive as a result of aerosol pollution. This 'lifetime indirect effect' of ice-only clouds was due to higher numbers of homogeneously nucleated ice crystals causing a reduction in their mean size, slowing the ice-crystal process of snow production and slowing sedimentation. In addition

  13. Impact of clouds and precipitation on atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Andronache, Constantin

    2015-04-01

    Aerosols have a significant impact on the dynamics and microphysics of continental mixed-phase convective clouds. High aerosol concentrations provide enhanced cloud condensation nuclei that can lead to the invigoration of convection and increase of surface rainfall. Such effects are dependent on environmental conditions and aerosol properties. Clouds are not only affected by aerosol, they also alter aerosol properties by various processes. Cloud processing of aerosol includes: convective redistribution, modification in the number and size of aerosol particles, chemical processing, new particle formation around clouds, and aerosol removal by rainfall to the surface. Among these processes, the wet removal during intense rain events, in polluted continental regions, can lead to spikes in acidic deposition into environment. In this study, we address the effects of clouds and precipitation on the aerosol distribution in cases of convective precipitation events in eastern US. We examine the effects of clouds and precipitation on various aerosol species, as well as their temporal and spatial variability.

  14. Multiphase processing of organic hydroxynitrates in secondary organic aerosol from the radical-initiated oxidation of multi-olefinic monoterpenes

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Lee, L. S.; Shepson, P. B.; De Perre, C.

    2015-12-01

    One of the greatest challenges facing atmospheric and climate science is understanding the impacts human activities have on the natural environment and atmospheric chemistry. The production of condensable organic compounds due to interactions between atmospheric oxidants, nitrogenous pollutants, and biogenic volatile organic compounds (BVOCs) emitted from the terrestrial biosphere can contribute significantly to the formation and growth of secondary organic aerosol (SOA). Aerosol particles influence atmospheric radiative transfer, cloud formation, and thus atmospheric temperatures. Due to their solubility in water and adsorptive nature, hydroxylated organic nitrates (HORONO2) may contribute significantly to the formation and chemical aging of SOA, and serve as an important sink for NOx (NO+NO2). We recently observed that a monoterpene β-hydroxy-organic nitrate (C10H17NO4), produced from the OH oxidation of α-pinene in the presence of NOx, undergoes rapid processing in the aerosol phase via an acid-catalyzed and pH-dependent hydrolysis mechanism, potentially impacting SOA growth and molecular composition. Further processing in the aerosol phase via polymerization and formation of organosulfates is expected, yet studies related to product identification and their formation mechanisms are limited. In this presentation, I will discuss recent laboratory-based reaction chamber studies of gas-phase organic nitrate production, SOA formation, and acidity-dependent aerosol-phase processing of organic nitrates produced from the NO3 oxidation of γ-terpinene. This BVOC is a diolefin, which as modeling studies suggest, may be an important nighttime organic nitrate precursor. Gas-phase organic nitrate compounds resulting from NO3 oxidation were qualitatively identified applying I- chemical ionization mass spectrometry (CIMS) and quantified via calibration using synthetic standards generated in our laboratory. Aerosol-phase analysis was carried out employing Fourier transform

  15. Importance of Raman Lidar Aerosol Extinction Measurements for Aerosol-Cloud Interaction Studies

    NASA Astrophysics Data System (ADS)

    Han, Zaw; Wu, Yonghua; Moshary, Fred; Gross, Barry; Gilerson, Alex

    2016-06-01

    Using a UV Raman Lidar for aerosol extinction, and combining Microwave Radiometer derived Liquid Water Path (LWP) with Multifilter Rotating Shadowband Radiometer derived Cloud Optical depth, to get cloud effective radius (Reff), we observe under certain specialized conditions, clear signatures of the Twomey Aerosol Indirect effect on cloud droplet properties which are consistent with the theoretical bounds. We also show that the measurement is very sensitive to how far the aerosol layer is from the cloud base and demonstrate that surface PM25 is far less useful. Measurements from both the DOE ARM site and new results at CCNY are presented.

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

    NASA Technical Reports Server (NTRS)

    Kasibhatla, Prasad

    1996-01-01

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

  17. Validation studies using multiwavelength Cryogenic Limb Array Etalon Spectrometer (CLAES) observations of stratospheric aerosol

    NASA Astrophysics Data System (ADS)

    Massie, Steven T.; Gille, John C.; Edwards, David P.; Bailey, Paul L.; Lyjak, Lawrence V.; Craig, Cheryl A.; Cavanaugh, Charles P.; Mergenthaler, John L.; Roche, Aidan E.; Kumer, John B.; Lambert, Alyn; Grainger, Roy G.; Rodgers, Clive D.; Taylor, Frederic W.; Russell, James M.; Park, Jae H.; Deshler, Terry; Hervig, Mark E.; Fishbein, Evan F.; Waters, Joe W.; Lahoz, William A.

    1996-04-01

    Validation studies of multiwavelength Cryogenic Limb Array Etalon Spectrometer (CLAES) observations of stratospheric aerosol are discussed. An error analysis of the CLAES aerosol extinction data is presented. Aerosol extinction precision values are estimated at latitudes and times at which consecutive Upper Atmosphere Research Satellite (UARS) orbits overlap. Comparisons of CLAES aerosol data with theoretical Mie calculations, based upon in situ particle size measurements at Laramie, Wyoming, are presented. CLAES aerosol data are also compared to scaled aerosol extinction measured by the Stratospheric Aerosol and Gas Experiment (SAGE II) and Atmospheric Trace Molecule Spectroscopy (ATMOS) experiments. Observed and calculated extinction spectra, from CLAES, Improved Stratospheric and Mesospheric Sounder (ISAMS), and Halogen Occultation Experiment (HALOE) data, are compared. CLAES extinction data have precisions between 10 and 25%, instrumental biases near 30%, and accuracies between 33 and 43%.

  18. Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

    NASA Astrophysics Data System (ADS)

    Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Skrotzki, J.; Leisner, T.; Wilson, T. W.; Malkin, T. L.; Murray, B. J.

    2012-04-01

    The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA), levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition) before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosols that have re-vitrified in contact with the

  19. Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

    NASA Astrophysics Data System (ADS)

    Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Skrotzki, J.; Leisner, T.; Wilson, T. W.; Malkin, T. L.; Murray, B. J.

    2012-09-01

    The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA), levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition) before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosol particles that have re-vitrified in contact

  20. Glyoxal processing outside clouds: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Volkamer, R.

    2010-05-01

    This study presents a modeling framework based on laboratory data to describe the kinetics of glyoxal reactions in aqueous aerosol particles that form secondary organic aerosol (SOA). Recent laboratory results on glyoxal reactions are reviewed and a consistent set of reaction rate constants is derived that captures the kinetics of glyoxal hydration and subsequent reversible and irreversible reactions in aqueous inorganic and water-soluble organic aerosol seeds to form (a) oligomers, (b) nitrogen-containing products, (c) photochemical oxidation products with high molecular weight. These additional aqueous phase processes enhance the SOA formation rate in particles compared to cloud droplets and yield two to three orders of magnitude more SOA than predicted based on reaction schemes for dilute aqueous phase (cloud) chemistry. The application of this new module in a chemical box model demonstrates that both the time scale to reach aqueous phase equilibria and the choice of rate constants of irreversible reactions have a pronounced effect on the atmospheric relevance of SOA formation from glyoxal. During day time a photochemical (most likely radical-initiated) process is the major SOA formation pathway forming ~5 μg m-3 SOA over 12 h (assuming a constant glyoxal mixing ratio of 300 ppt). During night time, reactions of nitrogen-containing compounds (ammonium, amines, amino acids) contribute most to the predicted SOA mass; however, the absolute predicted SOA masses are reduced by an order of magnitude as compared to day time production. The contribution of the ammonium reaction significantly increases in moderately acidic or neutral particles (5

  1. Study the polarization and depolarization properties of atmospheric aerosol multiple scattering based on the successive order of scattering

    NASA Astrophysics Data System (ADS)

    Hou, Weizhen; Sun, Bin; Li, Zhengqiang; Sun, Xiaobing; Hong, Jin; Qie, Lili; Wang, Han

    2015-10-01

    With the polynomial fitting of source function in each order of scattering calculation and the effective process of aerosol forward scattering peak, a polarized radiative transfer (RT) model based on the improved successive order of scattering (SOS) method has been developed to solve the vector radiative transfer equation. By our RT model, not only the total Stokes parameters [I, Q, U] measured by the satellite (aircraft) and ground-based sensors with linear polarization could be approximately simulated, but also the results of parameters for each scattering order event could conveniently calculated, which are very helpful to study the polarization properties for the atmospheric aerosol multiple scattering. In this study, the synchronous measured aerosol results including aerosol optical depth, complex refractive index and particle size distribution from AERONET under different air conditions, are considered as the input parameters for the successive scattering simulations. With our polarized RT model and the Mie code combined, the Stokes parameters as well as the degree of polarization for each scattering order are simulated and presented; meanwhile, the polarization (depolarization) properties of multiply scattering are preliminary analyzed and compared with different air quality (clear and pollution). Those results could provide a significant support for the further research of polarized aerosol remote sensing and inversion. Polarization properties of aerosol, successive order of scattering, vector radiative transfer equation, polynomial fitting of source function , multiply scattering

  2. A key process controlling the wet removal of aerosols: new observational evidence

    PubMed Central

    Ohata, Sho; Moteki, Nobuhiro; Mori, Tatsuhiro; Koike, Makoto; Kondo, Yutaka

    2016-01-01

    The lifetime and spatial distributions of accumulation-mode aerosols in a size range of approximately 0.05–1 μm, and thus their global and regional climate impacts, are primarily constrained by their removal via cloud and precipitation (wet removal). However, the microphysical process that predominantly controls the removal efficiency remains unidentified because of observational difficulties. Here, we demonstrate that the activation of aerosols to cloud droplets (nucleation scavenging) predominantly controls the wet removal efficiency of accumulation-mode aerosols, using water-insoluble black carbon as an observable particle tracer during the removal process. From simultaneous ground-based observations of black carbon in air (prior to removal) and in rainwater (after removal) in Tokyo, Japan, we found that the wet removal efficiency depends strongly on particle size, and the size dependence can be explained quantitatively by the observed size-dependent cloud-nucleating ability. Furthermore, our observational method provides an estimate of the effective supersaturation of water vapour in precipitating cloud clusters, a key parameter controlling nucleation scavenging. These novel data firmly indicate the importance of quantitative numerical simulations of the nucleation scavenging process to improve the model’s ability to predict the atmospheric aerosol burden and the resultant climate forcings, and enable a new validation of such simulations. PMID:27703169

  3. A key process controlling the wet removal of aerosols: new observational evidence

    NASA Astrophysics Data System (ADS)

    Ohata, Sho; Moteki, Nobuhiro; Mori, Tatsuhiro; Koike, Makoto; Kondo, Yutaka

    2016-10-01

    The lifetime and spatial distributions of accumulation-mode aerosols in a size range of approximately 0.05–1 μm, and thus their global and regional climate impacts, are primarily constrained by their removal via cloud and precipitation (wet removal). However, the microphysical process that predominantly controls the removal efficiency remains unidentified because of observational difficulties. Here, we demonstrate that the activation of aerosols to cloud droplets (nucleation scavenging) predominantly controls the wet removal efficiency of accumulation-mode aerosols, using water-insoluble black carbon as an observable particle tracer during the removal process. From simultaneous ground-based observations of black carbon in air (prior to removal) and in rainwater (after removal) in Tokyo, Japan, we found that the wet removal efficiency depends strongly on particle size, and the size dependence can be explained quantitatively by the observed size-dependent cloud-nucleating ability. Furthermore, our observational method provides an estimate of the effective supersaturation of water vapour in precipitating cloud clusters, a key parameter controlling nucleation scavenging. These novel data firmly indicate the importance of quantitative numerical simulations of the nucleation scavenging process to improve the model’s ability to predict the atmospheric aerosol burden and the resultant climate forcings, and enable a new validation of such simulations.

  4. Photolytic processing of secondary organic aerosols dissolved in cloud droplets

    SciTech Connect

    Bateman, Adam P; Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2011-05-26

    The effect of UV irradiation on the molecular composition of aqueous extracts of secondary organic aerosol (SOA) was investigated. SOA was prepared by the dark reaction of ozone and d-limonene at 0.05 - 1 ppm precursor concentrations and collected with a particle-into-liquid sampler (PILS). The PILS extracts were photolyzed by 300 - 400 nm radiation for up to 24 hours. Water-soluble SOA constituents were analyzed using high-resolution electrospray ionization mass spectrometry (HR-ESI-MS) at different stages of photolysis for all SOA precursor concentrations. Exposure to UV radiation increased the average O/C ratio and decreased the average double bond equivalent (DBE) of the dissolved SOA compounds. Oligomeric compounds were significantly reduced by photolysis relative to the monomeric compounds. Direct pH measurements showed that compounds containing carboxylic acids increased upon photolysis. Methanol reactivity analysis revealed significant photodissociation of molecules containing carbonyl groups and formation of carboxylic acids. Aldehydes, such as limononaldehyde, were almost completely removed. The removal of carbonylswas confirmed by the UV-Vis absorption spectroscopy of the SOA extracts where the absorbance in the carbonyl n→π* band decreased significantly upon photolysis. The effective quantum yield (the number of carbonyls destroyed per photon absorbed) was estimated as ~ 0.03. The concentration of peroxides did not change significantly during photolysis as quantified with an iodometric test. Although organic peroxides were photolyzed, the likely end products of photolysis were smaller peroxides, including hydrogen peroxide, resulting in a no net change in the peroxide content.

  5. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Astrophysics Data System (ADS)

    Tao, W.; Li, X.; Khain, A.; Simpson, J.

    2004-12-01

    Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, in the sub-tropics (Florida) and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for the two

  6. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Khain, A.; Simpson, S.; Johnson, D.; Li, X.; Remer, L.

    2003-01-01

    Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e.,pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size categor, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case

  7. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Khain, A.; Simpson, S.; Johnson, D.; Li, X.; Remer, L.

    2003-01-01

    Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distribution parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembel (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), groupel and frozen drops/hall] Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bim model explicitly calculates and allows for the examination of both the mass and number concentration of cpecies in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low

  8. Studies of the aerosol indirect effect from sulfate and black carbon aerosols

    NASA Astrophysics Data System (ADS)

    Kristjánsson, Jón Egill

    2002-08-01

    The indirect effect of anthropogenic aerosols is investigated using the global climate model National Center for Atmospheric Research Community Climate Model Version 3 (NCAR CCM3). Two types of anthropogenic aerosols are considered, i.e., sulfate and black carbon aerosols. The concentrations and horizontal distributions of these aerosols were obtained from simulations with a life-cycle model incorporated into the global climate model. They are then combined with size-segregated background aerosols. The aerosol size distributions are subjected to condensation, coagulation, and humidity swelling. By making assumptions on supersaturation, we determine cloud droplet number concentrations in water clouds. Cloud droplet sizes and top of atmosphere (TOA) radiative fluxes are in good agreement with satellite observations. Both components of the indirect effect, i.e., the radius and lifetime effects, are computed as pure forcing terms. Using aerosol data for 2000 from the Intergovernmental Panel on Climate Change (IPCC), we find, globally averaged, a 5% decrease in cloud droplet radius and a 5% increase in cloud water path due to anthropogenic aerosols. The largest changes are found over SE Asia, followed by the North Atlantic, Europe, and the eastern United States. This is also the case for the radiative forcing (``indirect effect''), which has a global average of -1.8 W m-2. When the experiment is repeated using data for 2100 from the IPCC A2 scenario, an unchanged globally averaged radiative forcing is found, but the horizontal distribution has been shifted toward the tropics. Sensitivity experiments show that the radius effect is ~3 times as important as the lifetime effect and that black carbon only contributes marginally to the overall indirect effect.

  9. A Cough Aerosol Simulator for the Study of Disease Transmission by Human Cough-Generated Aerosols

    PubMed Central

    Lindsley, William G.; Reynolds, Jeffrey S.; Szalajda, Jonathan V.; Noti, John D.; Beezhold, Donald H.

    2015-01-01

    Aerosol particles expelled during human coughs are a potential pathway for infectious disease transmission. However, the importance of airborne transmission is unclear for many diseases. To better understand the role of cough aerosol particles in the spread of disease and the efficacy of different types of protective measures, we constructed a cough aerosol simulator that produces a humanlike cough in a controlled environment. The simulated cough has a 4.2 l volume and is based on coughs recorded from influenza patients. In one configuration, the simulator produces a cough aerosol containing particles from 0.1 to 100 µm in diameter with a volume median diameter (VMD) of 8.5 µm and a geometric standard deviation (GSD) of 2.9. In a second configuration, the cough aerosol has a size range of 0.1–30 µm, a VMD of 3.4 µm, and a GSD of 2.3. The total aerosol volume expelled during each cough is 68 µl. By generating a controlled and reproducible artificial cough, the simulator allows us to test different ventilation, disinfection, and personal protection scenarios. The system can be used with live pathogens, including influenza virus, which allows isolation precautions used in the healthcare field to be tested without risk of exposure for workers or patients. The information gained from tests with the simulator will help to better understand the transmission of infectious diseases, develop improved techniques for infection control, and improve safety for healthcare workers and patients. PMID:26500387

  10. Rain-aerosol coupling in urban area: Scavenging ratio measurement and identification of some transfer processes

    NASA Astrophysics Data System (ADS)

    Jaffrezo, J.-L.; Colin, J.-L.

    Coupling between rain and associated aerosol has been studied for 1 year in Paris. Sampling techniques were chosen so as to describe the interacting phases as precisely as possible: exclusion of dry deposition, separation of successive rain events by an automatic sequential collector and aerosol collection over 6-h periods only. Study of interphase correlations for 82 events reveals three groups of species with distinctly different behaviour: insolubles—Al, Si, Fe; solubles—SO 42-, K, Ca, Zn, Mg; and the extreme case of Na and Cl. Interphase relationships decrease in this order. Variations of the scavenging ratio are in good agreement with the theoretical curve for collection efficiency. Noteworthy is the rise of the experimental curve for sub-μm particles. An interpretation based on the origin and hygroscopy of the species is attempted. Apart from their predictive ability in geochemical assessment, scavenging ratios appear useful for investigating the mechanisms of transfer between aerosols and precipitation.

  11. he Impact of Primary Marine Aerosol on Atmospheric Chemistry, Radiation and Climate: A CCSM Model Development Study

    SciTech Connect

    Keene, William C.; Long, Michael S.

    2013-05-20

    This project examined the potential large-scale influence of marine aerosol cycling on atmospheric chemistry, physics and radiative transfer. Measurements indicate that the size-dependent generation of marine aerosols by wind waves at the ocean surface and the subsequent production and cycling of halogen-radicals are important but poorly constrained processes that influence climate regionally and globally. A reliable capacity to examine the role of marine aerosol in the global-scale atmospheric system requires that the important size-resolved chemical processes be treated explicitly. But the treatment of multiphase chemistry across the breadth of chemical scenarios encountered throughout the atmosphere is sensitive to the initial conditions and the precision of the solution method. This study examined this sensitivity, constrained it using high-resolution laboratory and field measurements, and deployed it in a coupled chemical-microphysical 3-D atmosphere model. First, laboratory measurements of fresh, unreacted marine aerosol were used to formulate a sea-state based marine aerosol source parameterization that captured the initial organic, inorganic, and physical conditions of the aerosol population. Second, a multiphase chemical mechanism, solved using the Max Planck Institute for Chemistry's MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) system, was benchmarked across a broad set of observed chemical and physical conditions in the marine atmosphere. Using these results, the mechanism was systematically reduced to maximize computational speed. Finally, the mechanism was coupled to the 3-mode modal aerosol version of the NCAR Community Atmosphere Model (CAM v3.6.33). Decadal-scale simulations with CAM v.3.6.33, were run both with and without reactive-halogen chemistry and with and without explicit treatment of particulate organic carbon in the marine aerosol source function. Simulated results were interpreted (1) to evaluate influences of

  12. Potential source regions and processes of aerosol in the summer Arctic

    NASA Astrophysics Data System (ADS)

    Heintzenberg, J.; Leck, C.; Tunved, P.

    2015-06-01

    Sub-micrometer particle size distributions measured during four summer cruises of the Swedish icebreaker Oden 1991, 1996, 2001, and 2008 were combined with dimethyl sulfide gas data, back trajectories, and daily maps of pack ice cover in order to investigate source areas and aerosol formation processes of the boundary layer aerosol in the central Arctic. With a clustering algorithm, potential aerosol source areas were explored. Clustering of particle size distributions together with back trajectories delineated five potential source regions and three different aerosol types that covered most of the Arctic Basin: marine, newly formed and aged particles over the pack ice. Most of the pack ice area with < 15% of open water under the trajectories exhibited the aged aerosol type with only one major mode around 40 nm. For newly formed particles to occur, two conditions had to be fulfilled over the pack ice: the air had spent 10 days while traveling over ever more contiguous ice and had traveled over less than 30% open water during the last 5 days. Additionally, the air had experienced more open water (at least twice as much as in the cases of aged aerosol) during the last 4 days before arrival in heavy ice conditions at Oden. Thus we hypothesize that these two conditions were essential factors for the formation of ultrafine particles over the central Arctic pack ice. In a comparison the Oden data with summer size distribution data from Alert, Nunavut, and Mt. Zeppelin, Spitsbergen, we confirmed the Oden findings with respect to particle sources over the central Arctic. Future more frequent broken-ice or open water patches in summer will spur biological activity in surface water promoting the formation of biological particles. Thereby low clouds and fogs and subsequently the surface energy balance and ice melt may be affected.

  13. Meeting Review: Airborne Aerosol Inlet Workshop

    NASA Technical Reports Server (NTRS)

    Baumgardner, Darrel; Huebert, Barry; Wilson, Chuck

    1991-01-01

    Proceedings from the Airborne Aerosol Inlet Workshop are presented. The two central topics of discussion were the role of aerosols in atmospheric processes and the difficulties in characterizing aerosols. The following topics were discussed during the working sessions: airborne observations to date; identification of inlet design issues; inlet modeling needs and directions; objectives for aircraft experiments; and future laboratory and wind tunnel studies.

  14. 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

  15. Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

    NASA Astrophysics Data System (ADS)

    Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

    2015-12-01

    degrees during the aging processes were further illustrated in a case study of a severe haze episode. Our results elucidated a complex response of aerosol chemistry to emission controls, which has significant implications that emission controls over regional scales can substantially reduce secondary particulates. However, stricter emission controls for local source emissions are needed for further mitigating air pollution in the megacity of Beijing.

  16. Organic Aerosol Formation and Processing in the Los Angeles Basin: Role of Gasoline vs. Diesel Emissions

    NASA Astrophysics Data System (ADS)

    Bahreini, R.; Middlebrook, A. M.; De Gouw, J. A.; Warneke, C.; Trainer, M.; Brown, S. S.; Dube, B.; Holloway, J. S.; Perring, A. E.; Schwarz, J. P.; Spackman, J. R.; Stark, H.; Wagner, N.; Parrish, D. D.

    2011-12-01

    During the CalNex-2010 field project in May-June 2010, the NOAA WP-3D aircraft performed flights up- and down-wind of metropolitan, industrial, agricultural and animal feeding sites in central-southern California. Here airborne data on organic aerosol (OA) properties as measured by a compact time-of-flight aerosol mass spectrometer along with measurements of trace gases affecting secondary production of aerosols in the Los Angeles Basin are presented. The analysis presented indicates that the ratio of organic aerosol to carbon monoxide (OA/CO) is significantly higher than the previously observed ratios of primary OA/CO downwind of urban areas, indicating that even on short time scales of transport within the basin, there is significant production of secondary organic aerosol (SOA). The increase in the ratio of OA/CO is also accompanied by an increase in the fraction of oxygenated species of OA, providing evidence for production of more oxidized SOA as air masses are photochemically processed. Despite a smaller contribution from Diesel vehicles to traffic on weekends, analysis of the weekend vs. weekday data indicates that similar values of ΔOA/ΔCO are observed on the weekends compared to weekdays, for air masses with similar degrees of photochemical processing. This indicates that emissions of gas phase organic species from Diesel vehicles are not significant for OA production in the LA Basin. Our calculated steady-state concentrations of hydroxyl radical (OH) indicate that OH concentrations at mid-day are substantially higher on weekends compared to weekdays, indicating faster chemical processing of air masses during a fixed length of time on the weekends compared to weekdays.

  17. Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

    NASA Astrophysics Data System (ADS)

    Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

    2005-07-01

    Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

  18. Mesoscale modeling of combined aerosol and photo-oxidant processes in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Lazaridis, M.; Spyridaki, A.; Solberg, S.; Smolík, J.; Ždímal, V.; Eleftheriadis, K.; Aleksandropoulou, V.; Hov, O.; Georgopoulos, P. G.

    2004-09-01

    Particulate matter and photo-oxidant processes in the Eastern Mediterranean have been studied using the UAM-AERO mesoscale air quality model in conjunction with the NILU-CTM regional model. Meteorological data were obtained from the RAMS prognostic meteorological model. The modeling domain includes the eastern Mediterranean area between the Greek mainland and the island of Crete. The modeling system is applied to study the atmospheric processes in three periods, i.e. 13-16 July 2000, 26-30 July 2000 and 7-14 January 2001. The spatial and temporal distributions of both gaseous and particulate matter pollutants have been extensively studied together with the identification of major emission sources in the area. The modeling results were compared with field data obtained in the same period. Comparison of the modeling results with measured data was performed for a number of gaseous and aerosol species. The UAM-AERO model underestimates the PM10 measured concentrations during summer but better comparison has been obtained for the winter data.

  19. Aerosolization Characteristics of Dry Powder Inhaler Formulations for the Excipient Enhanced Growth (EEG) Application: Effect of Spray Drying Process Conditions on Aerosol Performance

    PubMed Central

    Son, Yoen-Ju; Longest, P. Worth; Hindle, Michael

    2013-01-01

    The aim of this study was to develop a spray dried submicrometer powder formulation suitable for the excipient enhanced growth (EEG) application. Combination particles were prepared using the Buchi Nano spray dryer B-90. A number of spray drying and formulation variables were investigated with the aims of producing dry powder formulations that were readily dispersed upon aerosolization and maximizing the fraction of submicrometer particles. Albuterol sulfate, mannitol, L-leucine, and poloxamer 188 were selected as a model drug, hygroscopic excipient, dispersibility enhancer and surfactant, respectively. Formulations were assessed by scanning electron microscopy and aerosol performance following aerosolization using an Aerolizer® dry powder inhaler (DPI). In vitro drug deposition was studied using a realistic mouth-throat (MT) model. Based on the in vitro aerosolization results, the best performing submicrometer powder formulation consisted of albuterol sulfate, mannitol, L-leucine and poloxamer 188 in a ratio of 30:48:20:2, containing 0.5% solids in a water:ethanol (80:20% v/v) solution which was spray dried at 70 °C. The submicrometer particle fraction (FPF1μm/ED) of this final formulation was 28.3% with more than 80% of the capsule contents being emitted during aerosolization. This formulation also showed 4.1% MT deposition. The developed combination formulation delivered a powder aerosol developed for the EEG application with high dispersion efficiency and low MT deposition from a convenient DPI device platform. PMID:23313343

  20. Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

    NASA Technical Reports Server (NTRS)

    Igel, Adele L.; Van Den Heever, Susan C.; Naud, Catherine M.; Saleeby, Stephen M.; Posselt, Derek J.

    2013-01-01

    An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.

  1. Exhaled Aerosol Pattern Discloses Lung Structural Abnormality: A Sensitivity Study Using Computational Modeling and Fractal Analysis

    PubMed Central

    Xi, Jinxiang; Si, Xiuhua A.; Kim, JongWon; Mckee, Edward; Lin, En-Bing

    2014-01-01

    Background Exhaled aerosol patterns, also called aerosol fingerprints, provide clues to the health of the lung and can be used to detect disease-modified airway structures. The key is how to decode the exhaled aerosol fingerprints and retrieve the lung structural information for a non-invasive identification of respiratory diseases. Objective and Methods In this study, a CFD-fractal analysis method was developed to quantify exhaled aerosol fingerprints and applied it to one benign and three malign conditions: a tracheal carina tumor, a bronchial tumor, and asthma. Respirations of tracer aerosols of 1 µm at a flow rate of 30 L/min were simulated, with exhaled distributions recorded at the mouth. Large eddy simulations and a Lagrangian tracking approach were used to simulate respiratory airflows and aerosol dynamics. Aerosol morphometric measures such as concentration disparity, spatial distributions, and fractal analysis were applied to distinguish various exhaled aerosol patterns. Findings Utilizing physiology-based modeling, we demonstrated substantial differences in exhaled aerosol distributions among normal and pathological airways, which were suggestive of the disease location and extent. With fractal analysis, we also demonstrated that exhaled aerosol patterns exhibited fractal behavior in both the entire image and selected regions of interest. Each exhaled aerosol fingerprint exhibited distinct pattern parameters such as spatial probability, fractal dimension, lacunarity, and multifractal spectrum. Furthermore, a correlation of the diseased location and exhaled aerosol spatial distribution was established for asthma. Conclusion Aerosol-fingerprint-based breath tests disclose clues about the site and severity of lung diseases and appear to be sensitive enough to be a practical tool for diagnosis and prognosis of respiratory diseases with structural abnormalities. PMID:25105680

  2. MARINE AEROSOLS ALTER SOIL PROCESSES IN COASTAL FORESTS

    EPA Science Inventory

    Most models of watershed biogeochemistry include the movement of materials from land to rivers and eventually the ocean. Few conceptual views, however, acknowledge the influence of materials derived from the ocean on terrestrial ecosystems processes. Based on spatial patterns o...

  3. Airborne studies of submicron aerosol in the troposphere over West Siberia

    SciTech Connect

    Panchenko, M.V.; Zuev, V.E.; Belan, B.D.; Terpugova, S.A.

    1996-04-01

    Submicron fraction particles that have the longest lifespan and are included in almost all atmospheric processes are of special importance among the great variety of sizes of particles present in the atmosphere. Submicron particles mainly determine the opticle state of the atmosphere in the visible spectral range, essentially cause the absorption of infrared radiation and, since they are the products and participants in all aerosol-to-gas transformations, accumulate of a lot of various chemical compounds and transfer them to large distances. Investigation of the processes of the spatial-temporal variability of aerosol particles for different climatic zones of the earth is the experimental base for studying their effect on climatically and ecologically significant factors and estimating their unfavorable tendencies. The increasing anthropogenic loading of the earth`s atmosphere is creating an urgency for aerosol research. Regardless of how perfect the analytical and numerical methods of solving radiation problems may be, success in forecasting climatic change is mainly determined by the reliability of the experimental data on optical parameters of the atmosphere and of the description of their variability under the effect of external factors.

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

    NASA Astrophysics Data System (ADS)

    Miller, Mary Rawlings Lamberton

    2000-09-01

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

  5. Electron-molecule chemistry and charging processes on organic ices and Titan's icy aerosol surrogates

    NASA Astrophysics Data System (ADS)

    Pirim, C.; Gann, R. D.; McLain, J. L.; Orlando, T. M.

    2015-09-01

    Electron-induced polymerization processes and charging events that can occur within Titan's atmosphere or on its surface were simulated using electron irradiation and dissociative electron attachment (DEA) studies of nitrogen-containing organic condensates. The DEA studies probe the desorption of H- from hydrogen cyanide (HCN), acetonitrile (CH3CN), and aminoacetonitrile (NH2CH2CN) ices, as well as from synthesized tholin materials condensed or deposited onto a graphite substrate maintained at low temperature (90-130 K). The peak cross sections for H- desorption during low-energy (3-15 eV) electron irradiation were measured and range from 3 × 10-21 to 2 × 10-18 cm2. Chemical and structural transformations of HCN ice upon 2 keV electron irradiation were investigated using X-ray photoelectron and Fourier-transform infrared spectroscopy techniques. The electron-beam processed materials displayed optical properties very similar to tholins produced by conventional discharge methods. Electron and negative ion trapping lead to 1011 charges cm-2 on a flat surface which, assuming a radius of 0.05 μm for Titan aerosols, is ∼628 charges/radius (in μm). The facile charge trapping indicates that electron interactions with nitriles and complex tholin-like molecules could affect the conductivity of Titan's atmosphere due to the formation of large negative ion complexes. These negatively charged complexes can also precipitate onto Titan's surface and possibly contribute to surface reactions and the formation of dunes.

  6. Laboratory Experiments and Instrument Development for the Study of Atmospheric Aerosols

    SciTech Connect

    Davidovits, Paul

    2011-12-10

    Soot particles are generated by incomplete combustion of fossil and biomass fuels. Through direct effects clear air aerosols containing black carbon (BC) such as soot aerosols, absorb incoming light heating the atmosphere, while most other aerosols scatter light and produce cooling. Even though BC represents only 1-2% of the total annual emissions of particulate mass to the atmosphere, it has been estimated that the direct radiative effect of BC is the second-most important contributor to global warming after absorption by CO2. Ongoing studies continue to underscore the climate forcing importance of black carbon. However, estimates of the radiative effects of black carbon on climate remain highly uncertain due to the complexity of particles containing black carbon. Quantitative measurement of BC is challenging because BC often occurs in highly non-spherical soot particles of complex morphology. Freshly emitted soot particles are typically fractal hydrophobic aggregates. The aggregates consist of black carbon spherules with diameters typically in the range of about 15-40 nm, and they are usually coated by adsorbed polyaromatic hydrocarbons (PAHs) produced during combustion. Diesel-generated soot particles are often emitted with an organic coating composed primarily of lubricating oil and unburned fuel, as well as well as PAH compounds. Sulfuric acid has also been detected in diesel and aircraft-emitted soot particles. In the course of aging, these particle coatings may be substantially altered by chemical reactions and/or the deposition of other materials. Such processes transform the optical and CCN properties of the soot aerosols in ways that are not yet well understood. Our work over the past seven years consisted of laboratory research, instrument development and characterization, and field studies with the central focus of improving our understanding of the black carbon aerosol climate impacts. During the sixth year as well as during this seventh year (no

  7. GLOBE Aerosol Field Campaign - U.S. Pilot Study 2016

    NASA Technical Reports Server (NTRS)

    Pippin, Margaret; Marentette, Christina; Bujosa, Robert; Taylor, Jessica; Lewis, Preston

    2016-01-01

    During the spring of 2016, from April 4 - May 27, sixteen GLOBE schools participated in the GLOBE Aerosol Field Campaign - U.S. Pilot Study. Thirteen teachers from these schools had previously participated in the NASA LEARN program (Long-term Experience in Authentic Research with NASA) where they were GLOBE trained in Atmosphere protocols, and engaged in 1-3 years of research under the mentorship of NASA scientists. Each school was loaned two aerosol instruments for the Campaign duration, either 2 GLOBE sun photometers, 2 Calitoo sun photometers, or 1 of each. This allowed for students to make measurements side-by-side and in the case of the Calitoos, to compare AOT results immediately with each other for better consistency in data collection. Additionally, as part of the Field Campaign evaluation, multiple instruments allow for an assessment of the ease of use of each instrument for grade level of students, whether in middle school or high school. Before the Campaign, all GLOBE and Calitoo instruments were 'checked out' against an AERONET, then checked again upon return after the Campaign. By examining all data, before, during and after the Campaign, this gives an indication of instrument performance and proficiency obtained by the students. Support was provided to each teacher and their students at the level requested, via email, phone or video conferencing.

  8. Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

    DOE PAGES

    Zhou, Shan; Collier, Sonya; Xu, Jianzhong; Mei, Fan; Wang, Jian; Lee, Yin -Nan; Sedlacek, III, Arthur J.; Springston, Stephen R.; Sun, Yele; Zhang, Qi

    2016-05-19

    Continuous real-time measurements of atmospheric aerosol with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the Department of Energy Aerosol Life Cycle Intensive Operational Period campaign. BNL was frequently downwind of emissions from the New York metropolitan area and was exposed to various combinations of anthropogenic, biogenic, and marine emissions based on air mass history. The average concentration of submicrometer aerosol (PM1) during this study was 12.6 µg m–3 with 64% of the mass being organic. Organic aerosol (OA) at BNLmore » was found to be overwhelmingly secondary, consisting of (1) a fresher, semivolatile oxygenated organic aerosol (SV-OOA; oxygen-to-carbon ratio (O/C) = 0.54; 63% of OA mass) that was strongly influenced by transported urban plumes; (2) a regional, more aged, low-volatility OOA (LV-OOA; O/C = 0.97; 29% of OA mass) influenced by aqueous-phase processing; and (3) a nitrogen-enriched OA (NOA; nitrogen-to-carbon ratio (N/C) = 0.185; 8% of OA mass) likely composed of amine salts formed from acid-base reactions in industrial emissions. Urban emissions from the New York metropolitan areas to the W and SW in particular led to elevated PM1 mass concentration and altered aerosol composition at BNL. Transported urban plumes and local biogenic emissions likely interacted to enhance secondary organic aerosol production, primarily represented by SV-OOA. Lastly, these results suggest an important role that urban anthropogenic emissions play in affecting ambient PM concentration, composition, and physical-chemical properties at rural areas in the Northeast U.S.« less

  9. Study of aerosols collected in a speleotherapeutic cave situated below Budapest, Hungary

    NASA Astrophysics Data System (ADS)

    Kertész, Zs.; Borbély-Kiss, I.; Hunyadi, I.

    1999-04-01

    The Szemlőhegy-cave is one of the well-known hydrothermal caves of the Rózsadomb area of Budapest, which have been used for speleotherapy of respiratory diseases for years. It is known from the periodically changing airborne radon activity concentration data, that airflow of seasonally reversed direction are formed along the cave passages and fissures due to the temperature difference between the surface and cave air. This means that an intensive interaction takes place between the cave and its environment. The pollution of nearby waters and the urban atmospheric air represents a real danger for these caves below Buda, which recently became the part of the UNESCO World Heritage. The study of cave aerosols should be very important from the point of view of either the control possibilities of the environmental impact or speleotherapy, and probably helps in getting acquainted with the cave-forming processes. In this work we applied our standard aerosol sampling method to the high-humidity environment of the caves, and we studied the elemental composition, size fractionation as well as the spatial distribution and the seasonal variation of cave aerosols. Thanks to the sensitivity of PIXE traces of anthropogenic pollution of the Budapest air are shown in the Szemlőhegy-cave. Measured elemental concentrations remained less than one-tenth the air quality standard valid for the increasingly protected areas.

  10. Cells (MC3T3-E1)-laden alginate scaffolds fabricated by a modified solid-freeform fabrication process supplemented with an aerosol spraying.

    PubMed

    Ahn, SeungHyun; Lee, HyeongJin; Bonassar, Lawrence J; Kim, GeunHyung

    2012-09-10

    In this study, we propose a new cell encapsulation method consisting of a dispensing method and an aerosol-spraying method. The aerosol spray using a cross-linking agent, calcium chloride (CaCl(2)), was used to control the surface gelation of dispensed alginate struts during dispensing. To show the feasibility of the method, we used preosteoblast (MC3T3-E1) cells. By changing the relationship between the various dispensing/aerosol-spraying conditions and cell viability, we could determine the optimal cell-dispensing process: a nozzle size (240 μm) and an aerosol spray flow rate (0.93 ± 0.12 mL min(-1)), 10 mm s(-1) nozzle moving speed, a 10 wt % concentration of CaCl(2) in the aerosol solution, and 2 wt % concentration of CaCl(2) in the second cross-linking process. Based on these optimized process conditions, we successfully fabricated a three-dimensional, pore-structured, cell-laden alginate scaffold of 20 × 20 × 4.6 mm(3) and 84% cell viability. During long cell culture periods (16, 25, 33, and 45 days), the preosteoblasts in the alginate scaffold survived and proliferated well.

  11. Evolution of Submicrometer Organic Aerosols during a Complete Residential Coal Combustion Process.

    PubMed

    Zhou, Wei; Jiang, Jingkun; Duan, Lei; Hao, Jiming

    2016-07-19

    In the absence of particulate matter (PM) control devices, residential coal combustion contributes significantly to ambient PM pollution. Characterizing PM emissions from residential coal combustion with high time resolution is beneficial for developing control policies and evaluating the environmental impact of PM. This study reports the evolution of submicrometer organic aerosols (OA) during a complete residential coal combustion process, that is, from fire start to fire extinction. Three commonly used coal types (bituminous, anthracite, and semicoke coals) were evaluated in a typical residential stove in China. For all three types of coal, the OA emission exhibited distinct characteristics in the four stages, that is, ignition, fierce combustion, relatively stable combustion, and ember combustion. OA emissions during the ignition stage accounted for 58.2-85.4% of the total OA emission of a complete combustion process. The OA concentration decreased rapidly during the fierce combustion stage and remained low during the relatively stable combustion stage. During these two stages, a significant ion peak of m/z 73 from organic acids were observed. The degree of oxidation of the OA increased from the first stage to the last stage. Implications for ambient OA source-apportionment and residential PM emission characterization and control are discussed. PMID:27298095

  12. Apartment Compartmentalization With an Aerosol-Based Sealing Process

    SciTech Connect

    Maxwell, Sean; Berger, David; Harrington, Curtis

    2015-03-01

    The U.S. Department of Energy Building America Team, Consortium for Advanced Residential Buildings, sought to demonstrate this new technology application in a new construction multifamily building in Queens, New York. The effectiveness of the sealing process was evaluated by three methods: air leakage testing of overall apartment before-and-after sealing, point-source testing of individual leaks, and pressure measurements in the walls of an apartment during sealing.

  13. Towards climatological study on the characteristics of aerosols in Central Africa and Mediterranean sites

    NASA Astrophysics Data System (ADS)

    Benkhalifa, Jamel; Chaabane, Mabrouk

    2016-02-01

    The atmosphere contains molecules, clouds and aerosols that are sub-millimeter particles having a large variability in size, shape, chemical composition, lifetime and contents. The aerosols concentration depends greatly on the geographical situation, meteorological and environmental conditions, which makes aerosol climatology difficult to assess. Setting up a solar photometer (automatic, autonomous and portable instrument) on a given site allows carrying out the necessary measurements for aerosol characterization. The particle microphysical and optical properties are obtained from photometric measurements. The objective of this study is to analyze the spatial variability of aerosol optical thickness (AOT) in several Mediterranean regions and Central Africa, we considered a set of simultaneous data in the AErosol RObotic NETwork (AERONET) from six sites, two of which are located in Central Africa (Banizoumbou and Zinder Airport) and the rest are Mediterranean sites (Barcelona, Malaga, Lampedusa, and Forth Crete). The results have shown that the physical properties of aerosols are closely linked to the climate nature of the studied site. The optical thickness, single scattering albedo and aerosols size distribution can be due to the aging of the dust aerosol as they are transported over the Mediterranean basin.

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

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

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

  15. Aerosols in the study of convective acinar mixing

    NASA Technical Reports Server (NTRS)

    Darquenne, Chantal; Prisk, G. Kim

    2005-01-01

    Convective mixing (CM) refers to the different transport mechanisms except Brownian diffusion that irreversibly transfer inspired air into resident air and can be studied using aerosol bolus inhalations. This paper provides a review of the present understanding of how each of these mechanisms contributes to CM. Original data of the combined effect of stretch and fold and gravitational sedimentation on CM are also presented. Boli of 0.5 microm-diameter particles were inhaled at penetration volumes (V(p)) of 300 and 1200 ml in eight subjects. Inspiration was followed by a 10-s breath hold, during which small flow reversals (FR) were imposed, and expiration. There was no physiologically significant dependence in dispersion and deposition with increasing FR. The results were qualitatively similar to those obtained in a previous study in microgravity in which it was speculated that the phenomenon of stretch and fold occurred during the first breathing cycle without the need of any subsequent FR.

  16. Evaluation of a coupled dispersion and aerosol process model against measurements near a major road

    NASA Astrophysics Data System (ADS)

    Pohjola, M. A.; Pirjola, L.; Karppinen, A.; Härkönen, J.; Ketzel, M.; Kukkonen, J.

    2007-02-01

    A field measurement campaign was conducted near a major road "Itäväylä" in an urban area in Helsinki in 17-20 February 2003. Aerosol measurements were conducted using a mobile laboratory "Sniffer" at various distances from the road, and at an urban background location. Measurements included particle size distribution in the size range of 7 nm-10 μm (aerodynamic diameter) by the Electrical Low Pressure Impactor (ELPI) and in the size range of 3-50 nm (mobility diameter) by Scanning Mobility Particle Sizer (SMPS), total number concentration of particles larger than 3 nm detected by an ultrafine condensation particle counter (UCPC), temperature, relative humidity, wind speed and direction, driving route of the mobile laboratory, and traffic density on the studied road. In this study, we have compared measured concentration data with the predictions of the road network dispersion model CAR-FMI used in combination with an aerosol process model MONO32. The vehicular exhaust emissions, and atmospheric dispersion and transformation of fine and ultrafine particles was evaluated within the distance scale of 200 m (corresponding to a time scale of a couple of minutes). We computed the temporal evolution of the number concentrations, size distributions and chemical compositions of various particle size classes. The atmospheric dilution rate of particles is obtained from the roadside dispersion model CAR-FMI. Considering the evolution of total number concentration, dilution was shown to be the most important process. The influence of coagulation and condensation on the number concentrations of particle size modes was found to be negligible at this distance scale. Condensation was found to affect the evolution of particle diameter in the two smallest particle modes. The assumed value of the concentration of condensable organic vapour of 1012 molecules cm-3 was shown to be in a disagreement with the measured particle size evolution, while the modelling runs with the

  17. Process analysis of regional aerosol pollution during spring in the Pearl River Delta region, China

    NASA Astrophysics Data System (ADS)

    Fan, Qi; Lan, Jing; Liu, Yiming; Wang, Xuemei; Chan, Pakwai; Hong, Yingying; Feng, Yerong; Liu, Yexin; Zeng, Yanjun; Liang, Guixiong

    2015-12-01

    A numerical simulation analysis was performed for three air pollution episodes in the Pearl River Delta (PRD) region during March 2012 using the third-generation air quality modeling system Models-3/CMAQ. The results demonstrated that particulate matter was the primary pollutant for all three pollution episodes and was accompanied by relatively low visibility in the first two episodes. Weather maps indicate that the first two episodes occurred under the influence of warm, wet southerly air flow systems that led to high humidity throughout the region. The liquid phase reaction of gaseous pollutants resulted in the generation of fine secondary particles, which were identified as the primary source of pollution in the first two episodes. The third pollution episode occurred during a warming period following a cold front. Relative humidity was lower during this episode, and coarse particles were the major pollution contributor. Results of process analysis indicated that emissions sources, horizontal transport and vertical transport were the primary factors affecting pollutant concentrations within the near-surface layer during all three episodes, while aerosol processes, cloud processes, horizontal transport and vertical transport had greater influence at approximately 900 m above ground. Cloud processes had a greater impact during the first two pollution episodes because of the higher relative humidity. In addition, by comparing pollution processes from different cities (Guangzhou and Zhongshan), the study revealed that the first two pollution episodes were the result of local emissions within the PRD region and transport between surrounding cities, while the third episode exhibited prominent regional pollution characteristics and was the result of regional pollutant transport.

  18. Integrated Modeling of Aerosol, Cloud, Precipitation and Land Processes at Satellite-Resolved Scales

    NASA Technical Reports Server (NTRS)

    Peters-Lidard, Christa; Tao, Wei-Kuo; Chin, Mian; Braun, Scott; Case, Jonathan; Hou, Arthur; Kumar, Anil; Kumar, Sujay; Lau, William; Matsui, Toshihisa; Miller, Tim; Santanello, Joseph, Jr.; Shi, Jainn; Starr, David; Tao, Qian; Zaitchik, Benjamin

    2012-01-01

    In this talk, I will present recent results from a project led at NASA/GSFC, in collaboration with NASA/MSFC and JHU, focused on the development and application of an observation-driven integrated modeling system that represents aerosol, cloud, precipitation and land processes at satellite-resolved scales. The project, known as the NASA Unified WRF (NU-WRF), is funded by NASA's Modeling and Analysis Program, and leverages prior investments from the Air Force Weather Agency and NASA's Earth Science Technology Office (ESTO). We define "satellite-resolved" scales as being within a typical mesoscale atmospheric modeling grid (roughly 1-25 km), although this work is designed to bridge the continuum between local (microscale), regional (mesoscale) and global (synoptic) processes. NU-WRF is a superset of the standard NCAR Advanced Research WRF model, achieved by fully integrating the GSFC Land Information System (LIS, already coupled to WRF), the WRF/Chem enabled version of the Goddard Chemistry Aerosols Radiation Transport (GOCART) model, the Goddard Satellite Data Simulation Unit (SDSU), and boundary/initial condition preprocessors for MERRA and GEOS-5 into a single software release (with source code available by agreement with NASA/GSFC). I will show examples where the full coupling between aerosol, cloud, precipitation and land processes is critical for predicting local, regional, and global water and energy cycles, including some high-impact phenomena such as floods, hurricanes, mesoscale convective systems, droughts, and monsoons.

  19. Coupling Aerosol-Cloud-Radiative Processes in the WRF-Chem Model: Investigating the Radiative Impact of Elevated Point Sources

    SciTech Connect

    Chapman, Elaine G.; Gustafson, William I.; Easter, Richard C.; Barnard, James C.; Ghan, Steven J.; Pekour, Mikhail S.; Fast, Jerome D.

    2009-02-01

    The local and regional influence of elevated point sources on summertime aerosol forcing and cloud-aerosol interactions in northeastern North America was investigated using the WRF-Chem community model. The direct effects of aerosols on incoming solar radiation were simulated using existing modules to relate aerosol sizes and chemical composition to aerosol optical properties. Indirect effects were simulated by adding a prognostic treatment of cloud droplet number and adding modules that activate aerosol particles to form cloud droplets, simulate aqueous phase chemistry, and tie a two-moment treatment of cloud water (cloud water mass and cloud droplet number) to an existing radiation scheme. Fully interactive feedbacks thus were created within the modified model, with aerosols affecting cloud droplet number and cloud radiative properties, and clouds altering aerosol size and composition via aqueous processes, wet scavenging, and gas-phase-related photolytic processes. Comparisons of a baseline simulation with observations show that the model captured the general temporal cycle of aerosol optical depths (AODs) and produced clouds of comparable thickness to observations at approximately the proper times and places. The model slightly overpredicted SO2 mixing ratios and PM2.5 mass, but reproduced the range of observed SO2 to sulfate aerosol ratios, suggesting that atmospheric oxidation processes leading to aerosol sulfate formation are captured in the model. The baseline simulation was compared to a sensitivity simulation in which all emissions at model levels above the surface layer were set to zero, thus removing stack emissions. Instantaneous, site-specific differences for aerosol and cloud related properties between the two simulations could be quite large, as removing above-surface emission sources influenced when and where clouds formed within the modeling domain. When summed spatially over the finest resolution model domain (the extent of which corresponds to

  20. Seasonal differences of urban organic aerosol composition - an ultra-high resolution mass spectrometry study

    NASA Astrophysics Data System (ADS)

    Rincon, A. G.; Calvo, A. I.; Dietzel, M.; Kalberer, M.

    2012-04-01

    The understanding of the chemical composition of atmospheric aerosols, their properties and reactivity are important for assessing aerosol effects upon both global climate change and human health. The composition of organic aerosols is poorly understood mainly due to their highly complex chemical composition with several thousand compounds. In the present study the water-soluble organic fraction of ambient particles collected at an urban site in Cambridge, UK, during different seasons were analysed with ultra-high resolution mass spectrometry. For several thousand peaks in the mass specta (between 3000-6000) an elemental composition could be assigned and summer samples generally contained more components than winter samples. Up to 80% of the peaks in the mass spectra contain nitrogen and/or sulphur functional groups and only about 20% of the compounds contain only C, H and O atoms. In summer the fraction of compounds with oxidized nitrogen and sulphur groups increases compared to winter indicating a photo-chemical formation route of these multifunctional compounds. In addition to oxidized nitrogen compounds a large number of highly unsaturated reduced nitrogen-containing compounds were detected, corresponding likely to cyclic amines. A significant number of oxidized PAHs have been detected in summer samples, which were not present in winter, indicating again photo-chemical aging processes. Both, amines and long-chain aliphatic acids (also frequently observed in these urban samples) are likely signatures of biomass burning and primary biological sources. Potential biomass burning markers are discussed. Particle-phase oligomerisation reactions have only been observed to a very limited degree. Compounds larger than m/z 350 almost exclusively contained N and/or S functional groups indicating that the high molecular weight compounds in these organic aerosol extracts might be mainly due to particle-phase heterogeneous reactions of organic compounds with inorganic

  1. Increase of Cloud Droplet Size with Aerosol Optical Depth: An Observational and Modeling Study

    SciTech Connect

    Yuan, Tianle; Li, Zhanqing; Zhang, Renyi; Fan, Jiwen

    2008-02-21

    Cloud droplet effective radius (DER) is generally negatively correlated with aerosol optical depth (AOD) as a proxy of cloud condensation nuclei. In this study, cases of positive correlation were found over certain portions of the world by analyzing the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite products, together with a general finding that DER may increase or decrease with aerosol loading depending on environmental conditions. The slope of the correlation between DER and AOD is driven primarily by water vapor amount, which explains 70% of the variance in our study. Various potential artifacts that may cause the positive relation are investigated including water vapor swelling, partially cloudy, atmospheric dynamics, cloud three-dimensional (3-D) and surface influence effects. None seems to be the primary cause for the observed phenomenon, although a certain degree of influence exists for some of the factors. Analyses are conducted over seven regions around the world representing different types of aerosols and clouds. Only two regions show positive dependence of DER on AOD, near coasts of the Gulf of Mexico and South China Sea, which implies physical processes may at work. Using a 2-D spectral-bin microphysics Goddard Cumulus Ensemble model (GCE) which incorporated a reformulation of the Köhler theory, two possible physical mechanisms are hypothesized. They are related to the effects of slightly soluble organics (SSO) particles and giant CCNs. Model simulations show a positive correlation between DER and AOD, due to a decrease in activated aerosols with an increasing SSO content. Addition of a few giant CCNs also increases the DER. Further investigations are needed to fully understand and clarify the observed phenomenon.

  2. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing.

    PubMed

    Zhang, Renyi; Khalizov, Alexei F; Pagels, Joakim; Zhang, Dan; Xue, Huaxin; McMurry, Peter H

    2008-07-29

    The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by approximately 10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing.

  3. A study on the extent of neutralization of sulphate aerosol through laboratory and field experiments using an ATOFMS and a GPIC

    NASA Astrophysics Data System (ADS)

    Yao, Xiaohong; Rehbein, Peter J. G.; Lee, Colin J.; Evans, Greg J.; Corbin, Joel; Jeong, Cheol-Heon

    2011-11-01

    Extent of neutralization (EoN) of atmospheric aerosol is an important parameter in understanding related nucleation mechanisms, acid-catalyzed reactions and gas-aerosol partitioning. Ion m/ z -195 (HSOHSO4-) detected by the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) has been used as an indicator of incompletely-neutralized sulphate aerosol, but there are no laboratory data to support this assumption. In this study, experiments using artificially generated sulphuric acid nucleated aerosol and metal sulphate aerosol across a range of EoN found that the peak area ratio and hit ratio of ion m/ z -195 (HSOHSO4-) to ion m/ z -97 (HSO4-) detected by the ATOFMS increased with decreasing EoN. Area ratio and hit ratio are sensitive to EoN at the low and high value zones, respectively. In ambient air measured by the ATOFMS and a Gas Particle Ion Chromatograph (GPIC) in Toronto, Canada, ion m/ z -195 was always detected in ammonium sulphate aerosol, and its hit number and peak area varied widely, regardless of EoN indicated by the equivalent ratio of NH4+ to (SO42-+NO3-). Thus, ion m/ z -195 alone is not an indicator of acidic sulphate aerosol. The combined approach using the ATOFMS and the GPIC found that cloud-processing formed incompletely-neutralized acidic sulphate aerosol in 2 out of 35 days sampled in winter in Toronto, Canada. It is interesting that the two episodes both occurred at night. Formation of incompletely-neutralized acidic sulphate aerosol caused a decrease in the concentration of particulate nitrate. This can be explained by acidic sulphate aerosol reacting with ammonium nitrate, leading to the release of HNO 3 to the gas phase. It was also found that the GPIC results occasionally suffered a positive artifact of NH4+ concentration caused by the clogging-induced high back-pressure in the instrument.

  4. 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.

  5. Carbonaceous Aerosols and Radiative Effects Study (CARES), g1-aircraft, sedlacek sp2

    DOE Data Explorer

    Sedlacek, Art

    2011-08-30

    The primary objective of the Carbonaceous Aerosol and Radiative Effects Study (CARES) in 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume.

  6. MODIS aerosol product at 3 km spatial resolution for urban and air quality studies

    NASA Astrophysics Data System (ADS)

    Mattoo, S.; Remer, L. A.; Levy, R. C.; Holben, B. N.; Smirnov, A.

    2008-12-01

    The MODerate resolution Imaging Spectroradiometer (MODIS) aboard the Terra and Aqua satellites has been producing an aerosol product since early 2000. The original product reports aerosol optical depth and a variety of other aerosol parameters at a spatial resolution of 10 km over both land and ocean. The 10 km product is actually constructed from 500 m pixels, which permits a strict selection process to choose the "best" or "cleanest" pixels in each 10 km square for use in the aerosol retrieval. Thus, the original 10 km product provides a useful product, accurate in many applications. However, the 10 km product can miss narrow aerosol plumes and the spatial variability associated with urban air pollution. The MODIS aerosol team will be introducing a finer resolution aerosol product over land regions in the next release of the product (Collection 6). The new product will be produced at 3 km resolution. It is based on the same procedures as the original product and benefits from the same spatial variability criteria for finding and masking cloudy pixels. The 3 km product does capture the higher spatial variability associated with individual aerosol plumes. However, it is noisier than the 10 km product. Both products will be available operationally in Collection 6. The new 3km product offers new synergistic possibilities with PM2.5 monitoring networks, AERONET and various air quality models such as CMAQ.

  7. Mutagenicity assessment of aerosols in emissions from domestic combustion processes.

    PubMed

    Canha, Nuno; Lopes, Isabel; Vicente, Estela Domingos; Vicente, Ana M; Bandowe, Benjamin A Musa; Almeida, Susana Marta; Alves, Célia A

    2016-06-01

    Domestic biofuel combustion is one of the major sources of regional and local air pollution, mainly regarding particulate matter and organic compounds, during winter periods. Mutagenic and carcinogenic activity potentials of the ambient particulate matter have been associated with the fraction of polycyclic aromatic hydrocarbons (PAH) and their oxygenated (OPAH) and nitrogenated (NPAH) derivatives. This study aimed at assessing the mutagenicity potential of the fraction of this polycyclic aromatic compound in particles (PM10) from domestic combustion by using the Ames assays with Salmonella typhimurium TA98 and TA100. Seven biofuels, including four types of pellets and three agro-fuels (olive pit, almond shell and shell of pine nuts), were tested in an automatic pellet stove, and two types of wood (Pinus pinaster, maritime pine, and Eucalyptus globulus, eucalypt) were burned in a traditional wood stove. For this latter appliance, two combustion phases-devolatilisation and flaming/smouldering-were characterised separately. A direct-acting mutagenic effect for the devolatilisation phase of pine combustion and for both phases of eucalypt combustion was found. Almond shell revealed a weak direct-acting mutagenic effect, while one type of pellets, made of recycled wastes, and pine (devolatilisation) presented a cytotoxic effect towards strain TA100. Compared to the manually fired appliance, the automatic pellet stove promoted lower polyaromatic mutagenic emissions. For this device, only two of the studied biofuels presented a weak mutagenic or cytotoxic potential. PMID:26893179

  8. Mutagenicity assessment of aerosols in emissions from domestic combustion processes.

    PubMed

    Canha, Nuno; Lopes, Isabel; Vicente, Estela Domingos; Vicente, Ana M; Bandowe, Benjamin A Musa; Almeida, Susana Marta; Alves, Célia A

    2016-06-01

    Domestic biofuel combustion is one of the major sources of regional and local air pollution, mainly regarding particulate matter and organic compounds, during winter periods. Mutagenic and carcinogenic activity potentials of the ambient particulate matter have been associated with the fraction of polycyclic aromatic hydrocarbons (PAH) and their oxygenated (OPAH) and nitrogenated (NPAH) derivatives. This study aimed at assessing the mutagenicity potential of the fraction of this polycyclic aromatic compound in particles (PM10) from domestic combustion by using the Ames assays with Salmonella typhimurium TA98 and TA100. Seven biofuels, including four types of pellets and three agro-fuels (olive pit, almond shell and shell of pine nuts), were tested in an automatic pellet stove, and two types of wood (Pinus pinaster, maritime pine, and Eucalyptus globulus, eucalypt) were burned in a traditional wood stove. For this latter appliance, two combustion phases-devolatilisation and flaming/smouldering-were characterised separately. A direct-acting mutagenic effect for the devolatilisation phase of pine combustion and for both phases of eucalypt combustion was found. Almond shell revealed a weak direct-acting mutagenic effect, while one type of pellets, made of recycled wastes, and pine (devolatilisation) presented a cytotoxic effect towards strain TA100. Compared to the manually fired appliance, the automatic pellet stove promoted lower polyaromatic mutagenic emissions. For this device, only two of the studied biofuels presented a weak mutagenic or cytotoxic potential.

  9. Investigating the two-component model of solid fuel organic aerosol in London: processes, PM1 contributions, and seasonality

    NASA Astrophysics Data System (ADS)

    Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Harrison, R. M.; Yin, J.; Flynn, M. J.; Gallagher, M. W.; Coe, H.

    2014-08-01

    Solid fuel emissions, including those from biomass burning, are increasing in urban areas across the European Union due to rising energy costs and government incentives to use renewable energy sources for heating. In order to help protect human health as well as to improve air quality and pollution abatement strategies, the sources of combustion aerosols, their contributions, and the processes they undergo need to be better understood. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was therefore deployed at an urban background site between January and February 2012 to investigate solid fuel organic aerosols (SFOA) in London. The variability of SFOA was examined and the factors governing the split between the two SFOA factors derived from positive matrix factorisation (PMF) were assessed. The concentrations of both factors were found to increase during the night and during cold periods, consistent with domestic space heating activities. The split between the two factors is likely governed predominantly by differences in burn conditions where SFOA1 best represents more efficient burns in the south and SFOA2 best represents less efficient burns in the east and west. The differences in efficiency may be due to burner types or burn phase, for example. Different fuel types and levels of atmospheric processing also likely contribute to the two factors. As the mass spectral profile of SFOA is highly variable, the findings from this study have implications for improving future source apportionment and factorisation analyses. During the winter, SFOA was found to contribute 38% to the total submicron organic aerosol (OA) mass, with SFOA2 contributing slightly more than SFOA1 (20% compared to 18%). A similar contribution of SFOA was derived for the same period from compact time-of-flight AMS (cToF-AMS), which measured for a full calendar year at the same site. The seasonality of SFOA was investigated using the year-long data set where concentrations

  10. Investigating a two-component model of solid fuel organic aerosol in London: processes, PM1 contributions, and seasonality

    NASA Astrophysics Data System (ADS)

    Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Harrison, R. M.; Yin, J.; Flynn, M. J.; Gallagher, M. W.; Coe, H.

    2015-03-01

    Solid fuel emissions, including those from biomass burning, are increasing in urban areas across the European Union due to rising energy costs and government incentives to use renewable energy sources for heating. In order to help protect human health as well as to improve air quality and pollution abatement strategies, the sources of combustion aerosols, their contributions, and the processes they undergo need to be better understood. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was therefore deployed at an urban background site between January and February 2012 to investigate solid fuel organic aerosols (SFOA) in London. The variability of SFOA was examined and the factors governing the split between the two SFOA factors derived from Positive Matrix Factorisation (PMF) were assessed. The concentrations of both factors were found to increase during the night and during cold periods, consistent with domestic space heating activities. The split between the two factors is likely governed predominantly by differences in burn conditions where SFOA1 best represents more efficient burns and SFOA2 best represents less efficient burns. The differences in efficiency may be due to burner types or burn phase, for example. Different fuel types and levels of atmospheric processing also likely contribute to the two factors. As the mass spectral profile of SFOA is highly variable, the findings from this study may have implications for improving future source apportionment and factorisation analyses. During the winter, SFOA was found to contribute 38% to the total non-refractory submicron organic aerosol (OA) mass, with similar contributions from both SFOA factors (20% from SFOA1 and 18% from SFOA2). A similar contribution of SFOA was derived for the same period from a compact time-of-flight AMS (cToF-AMS), which measured for a full calendar year at the same site. The seasonality of SFOA was investigated using the year-long data set where concentrations

  11. Atmospheric Processing of Iron-Containing Mineral Dust Aerosol: A Major Source of Bioavailable Iron to Ocean Life

    NASA Astrophysics Data System (ADS)

    Rubasinghege, G. R. S.; Hurub, O. A.

    2015-12-01

    In the present day, it has become more apparent that redox reactions involving mineral dust are of great interest, especially for Fe-containing mineral dust, as they transported and deposited into certain regions of the ocean that dissolved iron is often a limiting nutrient for ocean life. Given that heterogeneous reactions of Fe-containing mineral dust with acidic gases and their precursors, i.e. HNO3, dimethyl sulfide( DMS), lead to lower pH environments, the amount of bioavailable iron can increase as they are transported through the atmosphere. The current work focuses on chemical and photochemical processing of Fe-containing mineral dust particles in the presence of HNO3, SO2 and DMS under atmospherically relevant conditions. Here, various spectroscopic methods are combined with dissolution measurements to investigate atmospheric processing of iron containing aerosol dust, with a specific focus on mineralogy and environmental conditions, i.e. pH, relative humidity, temperature and solar flux. Ilmenite (FeTiO3) is used as one of the proxies for Fe-containing minerals that have enough complexity to mimic the mineral dust, yet simple enough to know the details of the reaction pathways. During these studies, above factors are found to play significant roles in the dissolution of iron from mineral dust aerosol. More importantly, data suggest that presence of titanium in the lattice structure of ilmenite enhances iron dissolution, at least by 3-fold in a comparison with hematite. Further, growth and activity of ocean diatoms (Cyclotella meneghiniana) are monitored in the presence of Fe-containing mineral dust under the same conditions. Here, diatoms are added to the reactors containing pre-dissolved iron from a prior 48hr reaction. Results show a high correlation between the growth of diatoms and the amount of bioavailable from iron containing minerals. The current study thus highlights these important, yet unconsidered, factors in the atmospheric processing of iron

  12. Process-model simulations of cloud albedo enhancement by aerosols in the Arctic

    PubMed Central

    Kravitz, Ben; Wang, Hailong; Rasch, Philip J.; Morrison, Hugh; Solomon, Amy B.

    2014-01-01

    A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN), either through geoengineering or other increased sources of Arctic aerosols. An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus, the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol–cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation owing to precipitation changes are small. According to these results, which are dependent upon the representation of ice nucleation processes in the employed microphysical scheme, Arctic geoengineering is unlikely to be effective as the sole means of altering the global radiation budget but could have substantial local radiative effects. PMID:25404677

  13. Process-model Simulations of Cloud Albedo Enhancement by Aerosols in the Arctic

    SciTech Connect

    Kravitz, Benjamin S.; Wang, Hailong; Rasch, Philip J.; Morrison, H.; Solomon, Amy

    2014-11-17

    A cloud-resolving model is used to simulate the effectiveness of Arctic marine cloud brightening via injection of cloud condensation nuclei (CCN). An updated cloud microphysical scheme is employed, with prognostic CCN and cloud particle numbers in both liquid and mixed-phase marine low clouds. Injection of CCN into the marine boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. Because nearly all of the albedo effects are in the liquid phase due to the removal of ice water by snowfall when ice processes are involved, albedo increases are stronger for pure liquid clouds than mixed-phase clouds. Liquid precipitation can be suppressed by CCN injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. CCN injection into a clean regime results in a greater albedo increase than injection into a polluted regime, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, dynamical changes in circulation due to precipitation changes are small.

  14. Halogen-induced organic aerosol (XOA) formation and decarboxylation of carboxylic acids by reactive halogen species - a time-resolved aerosol flow-reactor study

    NASA Astrophysics Data System (ADS)

    Ofner, Johannes; Zetzsch, Cornelius

    2013-04-01

    Reactive halogen species (RHS) are released to the atmosphere from various sources like photo-activated sea-salt aerosol and salt lakes. Recent studies (Cai et al., 2006 and 2008, Ofner et al., 2012) indicate that RHS are able to interact with SOA precursors similarly to common atmospheric oxidizing gases like OH radicals and ozone. The reaction of RHS with SOA precursors like terpenes forms so-called halogen-induced organic aerosol (XOA). On the other hand, RHS are also able to change the composition of functional groups, e.g. to initiate the decarboxylation of carboxylic acids (Ofner et al., 2012). The present study uses a 50 cm aerosol flow-reactor, equipped with a solar simulator to investigate the time-resolved evolution and transformation of vibrational features in the mid-infrared region. The aerosol flow-reactor is coupled to a home-made multi-reflection cell (Ofner et al., 2010), integrated into a Bruker IFS 113v FTIR spectrometer. The reactor is operated with an inlet feed (organic compound) and a surrounding feed (reactive halogen species). The moveable inlet of the flow reactor allows us to vary reaction times between a few seconds and up to about 3 minutes. Saturated vapours of different SOA precursors and carboxylic acids were fed into the flow reactor using the moveable inlet. The surrounding feed inside the flow reactor was a mixture of zero air with molecular chlorine as the precursor for the formation of reactive halogen species. Using this setup, the formation of halogen-induced organic aerosol could be monitored with a high time resolution using FTIR spectroscopy. XOA formation is characterized by hydrogen-atom abstraction, carbon-chlorine bond formation and later, even formation of carboxylic acids. Several changes of the entire structure of the organic precursor, caused by the reaction of RHS, are visible. While XOA formation is a very fast process, the decarboxylation of carboxylic acids, induced by RHS is rather slow. However, XOA formation

  15. Gas phase emissions from cooking processes and their secondary aerosol production potential

    NASA Astrophysics Data System (ADS)

    Klein, Felix; Platt, Stephen; Bruns, Emily; Termime-roussel, Brice; Detournay, Anais; Mohr, Claudia; Crippa, Monica; Slowik, Jay; Marchand, Nicolas; Baltensperger, Urs; Prevot, Andre; El Haddad, Imad

    2014-05-01

    Long before the industrial evolution and the era of fossil fuels, high concentrations of aerosol particles were alluded to in heavily populated areas, including ancient Rome and medieval London. Recent radiocarbon measurements (14C) conducted in modern megacities came as a surprise: carbonaceous aerosol (mainly organic aerosol, OA), a predominant fraction of particulate matter (PM), remains overwhelmingly non-fossil despite extensive fossil fuel combustion. Such particles are directly emitted (primary OA, POA) or formed in-situ in the atmosphere (secondary OA, SOA) via photochemical reactions of volatile organic compounds (VOCs). Urban levels of non-fossil OA greatly exceed the levels measured in pristine environments strongly impacted by biogenic emissions, suggesting a contribution from unidentified anthropogenic non-fossil sources to urban OA. Positive matrix factorization (PMF) techniques applied to ambient aerosol mass spectrometer (AMS, Aerodyne) data identify primary cooking emissions (COA) as one of the main sources of primary non-fossil OA in major cities like London (Allan et al., 2010), New York (Sun et al., 2011) and Beijing (Huang et al., 2010). Cooking processes can also emit VOCs that can act as SOA precursors, potentially explaining in part the high levels of oxygenated OA (OOA) identified by the AMS in urban areas. However, at present, the chemical nature of these VOCs and their secondary aerosol production potential (SAPP) remain virtually unknown. The approach adopted here involves laboratory quantification of PM and VOC emission factors from the main primary COA emitting processes and their SAPP. Primary emissions from deep-fat frying, vegetable boiling, vegetable frying and meat cooking for different oils, meats and vegetables were analysed under controlled conditions after ~100 times dilution. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a high resolution proton transfer time-of-flight mass spectrometer (PTR

  16. Mesoscale modeling of combined aerosol and photo-oxidant processes in the Eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Lazaridis, M.; Spyridaki, A.; Solberg, S.; Smolík, J.; Zdímal, V.; Eleftheriadis, K.; Aleksanropoulou, V.; Hov, O.; Georgopoulos, P. G.

    2005-03-01

    Particulate matter and photo-oxidant processes in the Eastern Mediterranean have been studied using the UAM-AERO mesoscale air quality model in conjunction with the NILU-CTM regional model. Meteorological data were obtained from the RAMS prognostic meteorological model. The modeling domain includes the eastern Mediterranean area between the Greek mainland and the island of Crete. The modeling system is applied to study the atmospheric processes in three periods, i.e. 13-16 July 2000, 26-30 July 2000 and 7-14 January 2001. The spatial and temporal distributions of both gaseous and particulate matter pollutants have been extensively studied together with the identification of major emission sources in the area. The modeling results were compared with field data obtained in the same period. The objective of the current modeling work was mainly to apply the UAM-AERO mesoscale model in the eastern Mediterranean in order to assess the performed field campaigns and determine that the applied mesoscale model is fit for this purpose. Comparison of the modeling results with measured data was performed for a number of gaseous and aerosol species. The UAM-AERO model underestimates the PM10 measured concentrations during summer and winter campaigns. Discrepancies between modeled and measured data are attributed to unresolved particulate matter emissions. Particulate matter in the area is mainly composed by sulphate, sea salt and crustal materials, and with significant amounts of nitrate, ammonium and organics. During winter the particulate matter and oxidant concentrations were lower than the summer values.

  17. A long term source apportionment study of wood burning and traffic aerosols for three measurement sites in Switzerland

    NASA Astrophysics Data System (ADS)

    Herich, Hanna; Hüglin, Christoph; Buchmann, Brigitte

    2010-05-01

    Besides their effects on radiative forcing soot aerosols have been found to cause health effects as they are carcinogenic. Diesel engines and incomplete biomass burning are the major emission sources of soot particles. Especially during winter, the wood burning (WB) emissions from residential heating have been found to contribute significantly to the total carbonaceous material (CM). To investigate the contribution of fossil fuel (FF) and WB emissions seven-wavelength aethalometers have been deployed in previous studies (Sandradewi et al. 2008, Favez et al. 2009). In these studies, the stronger light absorption of WB aerosols in the blue and ultraviolet compared to the light absorption of aerosols from FF combustion was used. Linear regression modelling of CM against the light absorption coefficient of FF combustion aerosols in the infrared (950 nm) and the light absorption coefficient of WB aerosols in the blue (470 nm) was proposed for source apportionment. In this study we present long term aethalometer measurements at two rural and one urban background measurement stations in Switzerland from 2008 - 2010. At these stations organic (OC) and elemental carbon (EC) were also measured by thermochemical analysis providing estimates for total CM. Above described linear regession modelling was applied for determination of the contribution of FF and WB emissions to total CM. Sensitivity tests for different regression models and for varying light absorption exponents were performed. It was found that the regression modelling approach is only limited suitable for long term datasets because of significant fractions of CM resulting from sources and processes other than FF and WB. Thus in a different approach we focused on black carbon (BC). The contribution of WB and FF to BC was directly determined from the absorption coefficients of FF and WB aerosols which were calculated with the use of absorption exponents taken from literature. First results show that in winter the

  18. Laboratory Investigation of Contact Freezing and the Aerosol to Ice Crystal Transformation Process

    SciTech Connect

    Shaw, Raymond A.

    2014-10-28

    This project has been focused on the following objectives: 1. Investigations of the physical processes governing immersion versus contact nucleation, specifically surface-induced crystallization; 2. Development of a quadrupole particle trap with full thermodynamic control over the temperature range 0 to –40 °C and precisely controlled water vapor saturation ratios for continuous, single-particle measurement of the aerosol to ice crystal transformation process for realistic ice nuclei; 3. Understanding the role of ice nucleation in determining the microphysical properties of mixed-phase clouds, within a framework that allows bridging between laboratory and field measurements.

  19. The impact of detailed urban-scale processing on the composition, distribution, and radiative forcing of anthropogenic aerosols

    NASA Astrophysics Data System (ADS)

    Cohen, Jason Blake; Prinn, Ronald G.; Wang, Chien

    2011-05-01

    Detailed urban-scale processing has not been included in global 3D chemical transport models due to its large computational demands. Here we present a metamodel for including this processing, and compare it with the use of the traditional approach of dilution of emissions into large grid boxes. This metamodel is used in a global 3D model to simulate the effects of cities around the world on aerosol chemistry, physics, and radiative effects at the global scale. We show that the biases caused by ignoring urban processing on the global values of total aerosol surface concentration, the total aerosol column abundance, the aerosol optical depth (AOD), the absorbing aerosol optical depth (AAOD), and the top of the atmosphere radiative forcing (TOA) respectively are +26 ± 32%, +51 ± 1012%, +42 ± 810%, +8 ± 1618%, and -0.27 ± 0.140.10 W/m2. These results show that failure to consider urban scale processing leads to significantly more negative aerosol radiative forcing compared to when detailed urban scale processing is considered.

  20. Sugars in Antarctic aerosol

    NASA Astrophysics Data System (ADS)

    Barbaro, Elena; Kirchgeorg, Torben; Zangrando, Roberta; Vecchiato, Marco; Piazza, Rossano; Barbante, Carlo; Gambaro, Andrea

    2015-10-01

    The processes and transformations occurring in the Antarctic aerosol during atmospheric transport were described using selected sugars as source tracers. Monosaccharides (arabinose, fructose, galactose, glucose, mannose, ribose, xylose), disaccharides (sucrose, lactose, maltose, lactulose), alcohol-sugars (erythritol, mannitol, ribitol, sorbitol, xylitol, maltitol, galactitol) and anhydrosugars (levoglucosan, mannosan and galactosan) were measured in the Antarctic aerosol collected during four different sampling campaigns. For quantification, a sensitive high-pressure anion exchange chromatography was coupled with a single quadrupole mass spectrometer. The method was validated, showing good accuracy and low method quantification limits. This study describes the first determination of sugars in the Antarctic aerosol. The total mean concentration of sugars in the aerosol collected at the "Mario Zucchelli" coastal station was 140 pg m-3; as for the aerosol collected over the Antarctic plateau during two consecutive sampling campaigns, the concentration amounted to 440 and 438 pg m-3. The study of particle-size distribution allowed us to identify the natural emission from spores or from sea-spray as the main sources of sugars in the coastal area. The enrichment of sugars in the fine fraction of the aerosol collected on the Antarctic plateau is due to the degradation of particles during long-range atmospheric transport. The composition of sugars in the coarse fraction was also investigated in the aerosol collected during the oceanographic cruise.

  1. 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

  2. Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

    NASA Astrophysics Data System (ADS)

    Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

    2015-08-01

    processes were further illustrated in a case study of a severe haze episode. Our results elucidated a complex response of aerosol chemistry to emission controls, which has significant implications that emission controls over regional scales can substantially reduce secondary particulates. However, stricter emission controls for local source emissions are needed for further mitigating air pollution in the megacity of Beijing.

  3. Anthropogenic Aerosols and Tropical Precipitation

    NASA Astrophysics Data System (ADS)

    Wang, C.; Kim, D.; Ekman, A. M. L.; Barth, M. C.; Rasch, P. J.

    2009-04-01

    Anthropogenic aerosols can affect the radiative balance of the Earth-atmosphere system and precipitation by acting as cloud condensation nuclei (CCN) or ice nuclei (IN) and thus modifying the optical and microphysical properties as well as lifetimes of clouds. Recent studies have also suggested that the direct radiative effect of anthropogenic aerosols, particularly absorbing aerosols, can perturb the large-scale circulation and cause a significant change in both quantity and distribution of critical tropical precipitation systems ranging from Pacific and Indian to Atlantic Oceans. This effect of aerosols on precipitation often appears in places away from aerosol-concentrated regions and current results suggest that the precipitation changes caused by it could be much more substantial than that by the microphysics-based aerosol effect. To understand the detailed mechanisms and strengths of such a "remote impact" and the climate response/feedback to anthropogenic aerosols in general, an interactive aerosol-climate model has been developed based on the Community Climate System Model (CCSM) of NCAR. Its aerosol module describes size, chemical composition, and mixing states of various sulfate and carbonaceous aerosols. Several model processes are derived based on 3D cloud-resolving model simulations. We have conducted a set of long integrations using the model driven by radiative effects of different combinations of various carbonaceous and sulfate aerosols and their mixtures. The responses of tropical precipitation systems to the forcing of these aerosols are analyzed using both model and observational data. Detailed analyses on the aerosol-precipitation causal relations of two systems: i.e., the Indian summer monsoon and Pacific ITCZ will be specifically presented.

  4. Fast oxidation processes from emission to ambient air introduction of aerosol emitted by residential log wood stoves

    NASA Astrophysics Data System (ADS)

    Nalin, Federica; Golly, Benjamin; Besombes, Jean-Luc; Pelletier, Charles; Aujay-Plouzeau, Robin; Verlhac, Stéphane; Dermigny, Adrien; Fievet, Amandine; Karoski, Nicolas; Dubois, Pascal; Collet, Serge; Favez, Olivier; Albinet, Alexandre

    2016-10-01

    Little is known about the impact of post-combustion processes, condensation and dilution, on the aerosol concentration and chemical composition from residential wood combustion. The evolution of aerosol emitted by two different residential log wood stoves (old and modern technologies) from emission until it is introduced into ambient air was studied under controlled "real" conditions. The first objective of this research was to evaluate the emission factors (EF) of polycyclic aromatic hydrocarbons (PAH) and their nitrated and oxygenated derivatives from wood combustion. These toxic substances are poorly documented in the literature. A second objective was to evaluate the oxidation state of the wood combustion effluent by studying these primary/secondary compounds. EFs of Σ37PAHs and Σ27Oxy-PAHs were in the same range and similar to those reported in literature (4-240 mg kg-1). Σ31Nitro-PAH EFs were 2-4 orders of magnitude lower (3.10-2-8.10-2 mg kg-1) due to the low temperature and low emission of NO2 from wood combustion processes. An increase of equivalent EF of PAH derivatives was observed suggesting that the oxidation state of the wood combustion effluent from the emission point until its introduction in ambient air changed in a few seconds. These results were confirmed by the study of both, typical compounds of SOA formation from PAH oxidation and, PAH ratio-ratio plots commonly used for source evaluation.

  5. A study of aerosol properties over Lahore (Pakistan) by using AERONET data

    NASA Astrophysics Data System (ADS)

    Ali, Muhammad; Tariq, Salman; Mahmood, Khalid; Daud, Asim; Batool, Adila; Zia-ul-Haq

    2014-02-01

    It is well established that aerosols affect the climate in a variety of ways. In order to understand these effects, we require an insight into the properties of aerosols. In this paper we present a study of aerosol properties such as aerosol optical depth (AOD), single scattering albedo (SSA) and aerosol radiative forcing (ARF) over mega city of Lahore (Pakistan). The data from Aerosol Robotic Network (AERONET) have been used for the period December 2009 to October 2011. The seasonal average values of AOD, asymmetry parameter (ASY) and volume size distribution in coarse mode were observed to be highest in summer. On the other hand, the average values of Angstrom exponent (AE) and imaginary part of refractive index (RI) were found to be maximum in winter. The average value of real part of RI was found to be higher in spring than in all other seasons. The SSA exhibited an increasing trend with wavelength in the range 440 nm-1020 nm in spring, summer and fall indicating the dominance of coarse particles (usually dust). However, a decreasing trend was found in winter in the range 675 nm-1020 nm pointing towards the dominance of biomass and urban/industrial aerosols. As far as aerosol radiative forcing (ARF) is concerned, we have found that during the spring season ARF was lowest at the surface of Earth and highest at top of the atmosphere (TOA). This indicates that the atmosphere was warmer in spring than in all the remaining seasons.

  6. A closure study of aerosol optical properties at a regional background mountainous site in Eastern China.

    PubMed

    Yuan, Liang; Yin, Yan; Xiao, Hui; Yu, Xingna; Hao, Jian; Chen, Kui; Liu, Chao

    2016-04-15

    There is a large uncertainty in evaluating the radiative forcing from aerosol-radiation and aerosol-cloud interactions due to the limited knowledge on aerosol properties. In-situ measurements of aerosol physical and chemical properties were carried out in 2012 at Mt. Huang (the Yellow Mountain), a continental background mountainous site in eastern China. An aerosol optical closure study was performed to verify the model outputs by using the measured aerosol optical properties, in which a spherical Mie model with assumptions of external and core-shell mixtures on the basis of a two-component optical aerosol model and high size-segregated element carbon (EC) ratio was applied. Although the spherical Mie model would underestimate the real scattering with increasing particle diameters, excellent agreement between the calculated and measured values was achieved with correlation coefficients above 0.98. Sensitivity experiments showed that the EC ratio had a negligible effect on the calculated scattering coefficient, but largely influenced the calculated absorption coefficient. The high size-segregated EC ratio averaged over the study period in the closure was enough to reconstruct the aerosol absorption coefficient in the Mie model, indicating EC size resolution was more important than time resolution in retrieving the absorption coefficient in the model. The uncertainties of calculated scattering and absorption coefficients due to the uncertainties of measurements and model assumptions yielded by a Monte Carlo simulation were ±6% and ±14% for external mixture and ±9% and ±31% for core-shell mixture, respectively. This study provided an insight into the inherent relationship between aerosol optical properties and physicochemical characteristics in eastern China, which could supplement the database of aerosol optical properties for background sites in eastern China and provide a method for regions with similar climate.

  7. Final Report: Process Models of the Equilibrium Size & State of Organic/Inorganic Aerosols for the Development of Large Scale Atmospheric Models & the Analysis of Field Data

    SciTech Connect

    Wexler, Anthony Stein; Clegg, Simon Leslie

    2013-10-26

    Our work addressed the following elements of the Call for Proposals: (i) “to improve the theoretical representation of aerosol processes studied in ASP laboratory or field studies”, (ii) “to enhance the incorporation of aerosol process information into modules suitable for large-scale or global atmospheric models”, and (iii) “provide systematic experimental validation of process model predictions ... using data from targeted laboratory and field experiments”. Achievements to the end of 2012 are described in four previous reports, and include: new models of densities and surface tensions of pure (single solute) and mixed aqueous solutions of typical aerosol composition under all atmospheric conditions (0 to 100% RH and T > 150 K); inclusion of these models into the widely used Extended Aerosol Inorganics model (E-AIM, http://www.aim.env.uea.ac.uk/aim/aim.php); the addition of vapor pressure calculators for organic compounds to the E-AIM website; the ability of include user-defined organic compounds and/or lumped surrogates in gas/aerosol partitioning calculations; the development of new equations to represent the properties of soluble aerosols over the entire concentration range (using methods based upon adsorption isotherms, and derived using statistical mechanics), including systems at close to zero RH. These results are described in publications 1-6 at the end of this report, and on the “News” page of the E-AIM website (http://www.aim.env.uea.ac.uk/aim/info/news.html). During 2012 and 2013 we have collaborated in a combined observation and lab-based study of the water uptake of the organic component of atmospheric aerosols (PI Gannet Hallar, of the Desert Research Institute). The aerosol samples were analyzed using several complementary techniques (GC/MS, FT-ICR MS, and ion chromatography) to produce a very complete organic “speciation” including both polar and non-polar compounds. Hygroscopic growth factors of the samples were measured, and

  8. Improving Aerosol Simulation over South Asia for Climate and Air Quality Studies

    NASA Technical Reports Server (NTRS)

    Pan, Xiaohua; Chin, Mian; Bian, Huisheng; Gautam, Ritesh

    2014-01-01

    Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, the water cycle, and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions found there. However, it has been proved quite challenging to adequately represent the aerosol spatial distribution and magnitude over this critical region in global models (Pan et al. 2014), with the surface concentrations, aerosol optical depth (AOD), and absorbing AOD (AAOD) significantly underestimated, especially in October-January when the agricultural waste burning and anthropogenic aerosol dominate over dust aerosol. In this study, we aim to investigate the causes for such discrepancy in winter by conducting sets of model experiments with NASA's GEOS-5 in terms of (1) spatial resolution, (2) emission amount, and (3) meteorological fields.

  9. Influence of aerosols on the life cycle of a radiation fog event. A numerical and observational study

    NASA Astrophysics Data System (ADS)

    Stolaki, S.; Haeffelin, M.; Lac, C.; Dupont, J.-C.; Elias, T.; Masson, V.

    2015-01-01

    Despite the knowledge gained on the physical processes dominating the formation, development and dissipation of radiation fog events, uncertainties still exist about the role of the microphysical processes related to aerosol characteristics. The objective of this work is to analyze the sensitivity of fog to aerosols through their impacts on the fog droplets. A radiation fog event that formed on 15/11/2011 at the SIRTA Observatory near Paris in the context of the 2011-2012 ParisFog field campaign is the basis of this study. The selected case is one that initially forms a few hundred meters above the surface and within half an hour lowers down to the surface. A combination of SIRTA's sophisticated observations and 1D numerical simulations is employed with the aim of better understanding the influence of thermodynamics and microphysics on the life-cycle of the fog event and the degree to which aerosol characteristics such as concentration of potentially activated aerosols, size and solubility affect its characteristics. It results that the model simulates fairly well the fog life cycle, with only one half hour advance in the onset and one hour in the dissipation at the surface. The quality of the reference simulation is evaluated against several in-situ and remote sensing measurements. A numerical sensitivity analysis shows that the fog characteristics are strongly influenced by the aerosols. Doubling (halving) the cloud condensation nuclei (CCN) number translates into a 160% increase (65% decrease) in the production of fog droplets, and a 60% increase (40% decrease) of the liquid water path (LWP). The aerosols influence up to 10% the fog geometrical thickness. The necessity for more detailed local forcings that will produce better thermohygrometric conditions in the upper levels above the formed fog layer is underlined, as well as the addition of microphysical measurements in the vertical that will allow to improve two-moment microphysics schemes.

  10. Simulation of South Asian aerosols for regional climate studies

    NASA Astrophysics Data System (ADS)

    Nair, Vijayakumar S.; Solmon, Fabien; Giorgi, Filippo; Mariotti, Laura; Babu, S. Suresh; Moorthy, K. Krishna

    2012-02-01

    Extensive intercomparison of columnar and near-surface aerosols, simulated over the South Asian domain using the aerosol module included in the regional climate model (RegCM4) of the Abdus Salam International Centre for Theoretical Physics (ICTP) have been carried out using ground-based network of Sun/sky Aerosol Robotic Network (AERONET) radiometers, satellite sensors such as Moderate Resolution Imaging Spectroradiometer (MODIS) and Multiangle Imaging Spectroradiometer (MISR), and ground-based black carbon (BC) measurements made at Aerosol Radiative Forcing over India (ARFI) network stations. In general, RegCM4 simulations reproduced the spatial and seasonal characteristics of aerosol optical depth over South Asia reasonably well, particularly over west Asia, where mineral dust is a major contributor to the total aerosol loading. In contrast, RegCM4 simulations drastically underestimated the BC mass concentrations over most of the stations, by a factor of 2 to 5, with a large spatial variability. Seasonally, the discrepancy between the measured and simulated BC tended to be higher during winter and periods when the atmospheric boundary layer is convectively stable (such as nighttime and early mornings), while during summer season and during periods when the boundary layer is convectively unstable (daytime) the discrepancies were much lower, with the noontime values agreeing very closely with the observations. A detailed analysis revealed that the model does not reproduce the nocturnal high in BC, observed at most of the Indian sites especially during winter, because of the excessive vertical transport of aerosols under stable boundary layer conditions. As far as the vertical distribution was concerned, the simulated vertical profiles of BC agreed well with airborne measurements during daytime. This comprehensive validation exercise reveals the strengths and weaknesses of the model in simulating the spatial and temporal heterogeneities of the aerosol fields over

  11. The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, Xiaowen; Khain, Alexander; Matsui, Toshihisa; Lang, Stephen; Simpson, Joanne

    2012-01-01

    Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and summertime convection over a mid-latitude continent with different concentrations of CCN: a low clean concentration and a high dirty concentration. The impact of atmospheric aerosol concentration on cloud and precipitation will be investigated.

  12. Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass apectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2011-02-01

    Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer during the summer 2009 Field Intensive Study at Queens College in New York, NY. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of the total PM1 mass. The average mass-based size distribution of OA presents a small mode peaking at ~150 nm (Dva) and an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of both sulfate and OA peak between 01:00-02:00 p.m. EST due to photochemical production. The average (±σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012 (±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62 (±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified two primary OA (POA) sources, traffic and cooking, and three secondary OA (SOA) components including a highly oxidized, regional low-volatility oxygenated OA (LV-OOA; O/C = 0.63), a less oxidized, semi-volatile SV-OOA (O/C = 0.38) and a unique nitrogen-enriched OA (NOA; N/C = 0.053) characterized with prominent CxH2x + 2N+ peaks likely from amino compounds. Our results indicate that cooking and traffic are two distinct and mass-equivalent POA sources in NYC, together contributing ~30% of the total OA mass during this study. The OA composition is dominated by secondary species, especially during high PM events. SV-OOA and LV-OOA on average account for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC appears to progress with a continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that organic nitrogen

  13. Characterization of the sources and processes of organic and inorganic aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2010-10-01

    peaking around local lunch and dinner times. In addition, NOA is characterized with prominent CxH2x+2N+ peaks likely from amine compounds. Our results indicate that cooking-related activities are a major source of POA in NYC, releasing comparable amounts of POA as traffic emissions. POA=HOA+COA) on average accounts for ~30% of the total OA mass during this study while SOA dominates the OA composition with SV-OOA and LV-OOA on average accounting for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC involves a~continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that nitrogen-containing organic species such as amines might have played an important role in the atmospheric processing of OA in NYC, likely involving acid-base chemistry. Analysis of air mass trajectories and satellite imagery of aerosol optical depth (AOD) indicates that the high potential source regions of secondary sulfate and aged OA are mainly located in regions to the west and southwest of the city.

  14. Interactions of mineral dust with pollution and clouds: An individual-particle TEM study of atmospheric aerosol from Saudi Arabia

    NASA Astrophysics Data System (ADS)

    Pósfai, Mihály; Axisa, Duncan; Tompa, Éva; Freney, Evelyn; Bruintjes, Roelof; Buseck, Peter R.

    2013-03-01

    Aerosol particles from desert dust interact with clouds and influence climate on regional and global scales. The Riyadh (Saudi Arabia) aerosol campaign was initiated to study the effects of dust particles on cloud droplet nucleation and cloud properties. Here we report the results of individual-particle studies of samples that were collected from an aircraft in April 2007. We used analytical transmission electron microscopy, including energy-dispersive X-ray spectrometry, electron diffraction, and imaging techniques for the morphological, chemical, and structural characterization of the particles. Dust storms and regional background conditions were encountered during four days of sampling. Under dusty conditions, the coarse (supermicrometer) fraction resembles freshly crushed rock. The particles are almost exclusively mineral dust grains and include common rock-forming minerals, among which clay minerals, particularly smectites, are most abundant. Unaltered calcite grains also occur, indicating no significant atmospheric processing. The particles have no visible coatings but some contain traces of sulfur. The fine (submicrometer) fraction is dominated by particles of anthropogenic origin, primarily ammonium sulfate (with variable organic coating and some with soot inclusions) and combustion-derived particles (mostly soot). In addition, submicrometer, iron-bearing clay particles also occur, many of which are internally mixed with ammonium sulfate, soot, or both. We studied the relationships between the properties of the aerosol and the droplet microphysics of cumulus clouds that formed above the aerosol layer. Under dusty conditions, when a large concentration of coarse-fraction mineral particles was in the aerosol, cloud drop concentrations were lower and droplet diameters larger than under regional background conditions, when the aerosol was dominated by submicrometer sulfate particles.

  15. Generation of Li combustion aerosols for animal inhalation studies.

    PubMed

    Allen, M D; Greenspan, B J; Briant, J K; Hoover, M D

    1986-07-01

    A system was developed for generating Li aerosols to determine the potential health hazards of postulated accidents associated with the use of Li as a fusion reactor blanket or coolant. The aerosol was generated by sweeping Ar through a stainless steel chamber filled with Li metal that was heated inductively to temperatures up to 1300 degrees C. Argon carried the Li vapor into a burning chamber where it was mixed with air. The reaction of Li vapor with air formed an intense white flame that produced typical branched-chain condensation aerosol particles. This system generated well-controlled concentrations up to 2500 mg/m3 for periods of 4 h. The mass median aeordynamic diameter of the aerosol was approximately 0.66 micron with a geometric standard deviation of 1.5. Aerosols could be generated that were greater than 96% Li2O and LiOH, LiOH.H2O, or Li2CO3 by controlling the CO2 and H2O concentrations in the supply air. The system is currently being used to investigate the acute toxicity of Li combustion aerosols in laboratory animals.

  16. Aerosol-radiation-cloud and precipitation processes during dust events (Invited)

    NASA Astrophysics Data System (ADS)

    Kallos, G. B.; Solomos, S.; Kushta, J.; Mitsakou, C.; Athanasiadis, P.; Spyrou, C.; Tremback, C.

    2010-12-01

    In places like the Mediterranean region where anthropogenic aerosols coexist with desert dust the aerosol-radiation-cloud processes are rather complicated. The mixture of different age of air pollutants of anthropogenic origin with Saharan dust and sea salt may lead to the formation of other particles with different characteristics. The mixture of the aerosols and gases from anthropogenic and natural origin (desert dust and sea salt) results in the formation of new types of PM with different physico-chemical properties and especially hygroscopicity (e.g. inside clouds or within the marine boundary layer) through heterogeneous processes. The new particle formation has different characteristics and therefore they have different impacts on cloud formation and precipitation. In an attempt to better understand links and feedbacks between air pollution and climate the new Integrated Community Limited Area Modeling System - ICLAMS has been developed. ICLAMS is an enhanced version of RAMS.v6 modeling system. It includes sub-models for the dust and sea salt cycles, gas and aqueous phase chemistry, gas to particle conversion and heterogeneous chemistry processes. All these processes are directly coupled with meteorology. RAMS has an explicit cloud microphysical scheme with eight categories of hydrometeors. The cloud droplets spectrum is explicitly calculated from model meteorology and prognostic CCN and IN properties (total number concentration, size distribution properties and chemical composition). Sulphate coated dust particles are efficient CCN because of their increased hygroscopicity while uncoated dust particles are efficient IN. The photochemical processes are directly linked to the RAMS radiative transfer scheme, which in the new model is RRTM. Absorption of short wave solar radiation from airborne dust leads to heating of the dust layer which can also affect the cloud processes. Mid and low tropospheric warming by dust is one of the new features that the model can

  17. Using High-Resolution Airborne Remote Sensing to Study Aerosol Near Clouds

    NASA Technical Reports Server (NTRS)

    Levy, Robert; Munchak, Leigh; Mattoo, Shana; Marshak, Alexander; Wilcox, Eric; Gao, Lan; Yorks, John; Platnick, Steven

    2016-01-01

    The horizontal space in between clear and cloudy air is very complex. This so-called twilight zone includes activated aerosols that are not quite clouds, thin cloud fragments that are not easily observable, and dying clouds that have not quite disappeared. This is a huge challenge for satellite remote sensing, specifically for retrieval of aerosol properties. Identifying what is cloud versus what is not cloud is critically important for attributing radiative effects and forcings to aerosols. At the same time, the radiative interactions between clouds and the surrounding media (molecules, surface and aerosols themselves) will contaminate retrieval of aerosol properties, even in clear skies. Most studies on aerosol cloud interactions are relevant to moderate resolution imagery (e.g. 500 m) from sensors such as MODIS. Since standard aerosol retrieval algorithms tend to keep a distance (e.g. 1 km) from the nearest detected cloud, it is impossible to evaluate what happens closer to the cloud. During Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), the NASA ER-2 flew with the enhanced MODIS Airborne Simulator (eMAS), providing MODIS-like spectral observations at high (50 m) spatial resolution. We have applied MODIS-like aerosol retrieval for the eMAS data, providing new detail to characterization of aerosol near clouds. Interpretation and evaluation of these eMAS aerosol retrievals is aided by independent MODIS-like cloud retrievals, as well as profiles from the co-flying Cloud Physics Lidar (CPL). Understanding aerosolcloud retrieval at high resolution will lead to better characterization and interpretation of long-term, global products from lower resolution (e.g.MODIS) satellite retrievals.

  18. 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

  19. 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

  20. 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

  1. Model analysis of secondary organic aerosol formation by glyoxal in laboratory studies: the case for photoenhanced chemistry.

    PubMed

    Sumner, Andrew J; Woo, Joseph L; McNeill, V Faye

    2014-10-21

    The reactive uptake of glyoxal by atmospheric aerosols is believed to be a significant source of secondary organic aerosol (SOA). Several recent laboratory studies have been performed with the goal of characterizing this process, but questions remain regarding the effects of photochemistry on SOA growth. We applied GAMMA (McNeill et al. Environ. Sci. Technol. 2012, 46, 8075-8081), a photochemical box model with coupled gas-phase and detailed aqueous aerosol-phase chemistry, to simulate aerosol chamber studies of SOA formation by the uptake of glyoxal by wet aerosol under dark and irradiated conditions (Kroll et al. J. Geophys. Res. 2005, 110 (D23), 1-10; Volkamer et al. Atmos. Chem. Phys. 2009, 9, 1907-1928; Galloway et al. Atmos. Chem. Phys. 2009, 9, 3331- 306 3345 and Geophys. Res. Lett. 2011, 38, L17811). We find close agreement between simulated SOA growth and the results of experiments conducted under dark conditions using values of the effective Henry's Law constant of 1.3-5.5 × 10(7) M atm(-1). While irradiated conditions led to the production of some organic acids, organosulfates, and other oxidation products via well-established photochemical mechanisms, these additional product species contribute negligible aerosol mass compared to the dark uptake of glyoxal. Simulated results for irradiated experiments therefore fell short of the reported SOA mass yield by up to 92%. This suggests a significant light-dependent SOA formation mechanism that is not currently accounted for by known bulk photochemistry, consistent with recent laboratory observations of SOA production via photosensitizer chemistry.

  2. Impact of the aging process of black carbon aerosols on their spatial distribution, hygroscopicity, and radiative forcing in a global climate model

    NASA Astrophysics Data System (ADS)

    Goto, D.; Oshima, N.; Nakajima, T.; Takemura, T.; Ohara, T.

    2012-11-01

    Black carbon (BC) absorbs shortwave radiation more strongly than any other type of aerosol, and an accurate simulation of the aging processes of BC-containing particle is required to properly predict aerosol radiative forcing (ARF) and climate change. However, BC aging processes have been simplified in general circulation models (GCMs) due to limited computational resources. In particular, differences in the representation of the mixing states of BC-containing particles between GCMs constitute one of main reasons for the uncertainty in ARF estimates. To understand an impact of the BC aging processes and the mixing state of BC on the spatial distribution of BC and ARF caused by BC (BC-ARF), we implemented three different methods of incorporating BC aging processes into a global aerosol transport model, SPRINTARS: (1) the "AGV" method, using variable conversion rates of BC aging based on a new type of parameterization depending on both BC amount and sulfuric acid; (2) the "AGF" method, using a constant conversion rate used worldwide in GCMs; and (3) the "ORIG" method, which is used in the original SPRINTARS. First, we found that these different methods produced different BC burden within 10% over industrial areas and 50% over remote oceans. Second, a ratio of water-insoluble BC to total BC (WIBC ratio) was very different among the three methods. Near the BC source region, for example, the WIBC ratios were estimated to be 80-90% (AGV and AGF) and 50-60% (ORIG). Third, although the BC aging process in GCMs had small impacts on the BC burden, they had a large impact on BC-ARF through a change in both the WIBC ratio and non-BC compounds coating on BC cores. As a result, possible differences in the treatment of the BC aging process between aerosol modeling studies can produce a difference of approximately 0.3 Wm-2 in the magnitude of BC-ARF, which is comparable to the uncertainty suggested by results from a global aerosol modeling intercomparison project, AeroCom. The

  3. Dissolved organic matter in sea spray: a transfer study from marine surface water to aerosols

    NASA Astrophysics Data System (ADS)

    Schmitt-Kopplin, P.; Liger-Belair, G.; Koch, B. P.; Flerus, R.; Kattner, G.; Harir, M.; Kanawati, B.; Lucio, M.; Tziotis, D.; Hertkorn, N.; Gebefügi, I.

    2011-12-01

    Atmospheric aerosols impose direct and indirect effects on the climate system, for example, by adsorption of radiation in relation to cloud droplets size, on chemical and organic composition and cloud dynamics. The first step in the formation of primary marine aerosols, i.e., the transfer of dissolved organic matter from the marine surface into the atmosphere was studied, and we present a molecular level description of this phenomenon using high resolution analytical tools (Fourier transform ion cyclotron resonance = FT-ICR MS and NMR). We could experimentally confirm the chemo-selective transfer of natural organic molecules, especially of aliphatic compounds from the surface water into the atmosphere via bubble bursting processes. Transfer from marine surface water to the atmosphere involves a chemical gradient governed by the physicochemical properties of the involved molecules when comparing elemental compositions and differentiating CHO, CHNO, CHOS and CHNOS bearing compounds. Typical chemical fingerprints of concentrated compounds were CHO and CHOS type of molecules, smaller molecules of higher aliphaticity and lower oxygen content and typical surfactants. A non-targeted mass spectrometric analysis of the samples showed that many of these molecules correspond to homologous series of oxo-, hydroxyl-, methoxy-, branched fatty acids and mono-, di- and tricarboxylic acids as well as monoterpenes and sugars. These surface active biomolecules were preferentially transferred from surface water into the atmosphere via bubble bursting processes to form a significant fraction of primary organic aerosols. This way of production of sea spray leaves a specific biological signature of the surface water in the corresponding lower atmosphere that can be transported laterally in the context of global cycling.

  4. Freezing Behavior of Stratospheric Sulfate Aerosols Inferred from Trajectory Studies

    NASA Technical Reports Server (NTRS)

    Tabazadeh, A.; Toon, O. B.; Hamill, Patrick

    1995-01-01

    Based on the trajectory analysis presented in this paper, a new mechanism is described for the freezing of the stratospheric sulfate aerosols. Temperature histories based on 10-day back trajectories for six ER-2 flights during AASE-I (1989) and AAOE (1987) are presented. The mechanism requires, as an initial step, the cooling of a H2SO4/H2O aerosol to low temperatures. If a cooling cycle is then followed up by a warming to approximately 196-198 K, the aerosols may freeze due to the growth of the crystallizing embryos formed at the colder temperature. The HNO3 absorbed at colder temperatures may increase the nucleation rate of the crystalling embryos and therefore influence the crystallization of the supercooled aerosols upon warming. Of all the ER-2 flights described, only the polar stratospheric clouds (PSC), observed on the flights of January 24, and 25, 1989 are consistent with the thermodynamics of liquid ternary solutions of H2SO4/HNO3/H2O (type Ib PSCs). For those two days, back trajectories indicate that the air mass was exposed to sulfuric acid tetrahydrate (SAT) melting temperatures about 24 hours prior to being sampled by the ER-2. Temperature histories, recent laboratory measurements, and the properties of glassy solids suggest that stratospheric H2SO4 aerosols may undergo a phase transition to SAT upon warming at approximately 198 K after going through a cooling cycle to about 194 K or lower.

  5. A study on major inorganic ion composition of atmospheric aerosols.

    PubMed

    Salve, P R; Krupadam, R J; Wate, S R

    2007-04-01

    Atmospheric aerosol samples were collected from Akola and Buldana region covering around 40 sqkm area during October-November 2002 and were analyzed for ten major inorganic ions namely F-, Cl-, NO3-, SO4(2-), PO4(2-), Na+, K+, Ca2+, Mg2+ and NH4+ using ion chromatographic technique. The average mass of aerosols was found to be 225.81 microg/m3 with standard deviation of 31.29 and average total water soluble load of total cations and anions was found to be 4.32 microg/m3. The concentration of ions in samples showed a general pattern as SO4(2-) > NO3- > Cl- > PO4(2-) > F- for anions and Na+ > Ca2+ > NH4+ > Mg2+ > K+ for cations. The overall composition of the aerosols was taken into account to identify the sources. The trend showed higher concentration of sodium followed by calcium, sulfate, nitrate, phosphate and ammoinum and found to be influenced by terrestrial sources. The presence of SO4(2-) and NO3- in aerosols may be due to re-suspension of soil particles. Ca2+, Mg2+ and Cl- are to be derived from soil materials. The presence of NH4+ may be attributed to the reaction of NH3 vapors with acidic gases may react or condense on an acidic particle surface of anthropogenic origin. The atmospheric aerosol is slightly acidic due to neutralization of basicity by SO2 and NO(x).

  6. Sensitivity of spectral reflectance to aerosol optical properties in UV and visible wavelength range: Preparatory study for aerosol retrieval from Geostationary Environmental Monitoring Spectrometer (GEMS)

    NASA Astrophysics Data System (ADS)

    KIM, M.; Kim, J.; Lee, J.

    2011-12-01

    Asia, with its rapid increase in industrialization and population, has been receiving great attention as one of important source regions of pollutants including aerosols and trace gases. Since the spatio-temporal distribution of the pollutants varies rapidly, demands to monitor air quality in a geostationary satellite have increased recently. In these perspectives, the Ministry of Environment of Korea initiated a geostationary satellite mission to launch the Geostationary Environmental Monitoring Spectrometer (GEMS) onboard the GEO-KOMPSAT in 2017-2018 timeframe. From the Ozone Monitoring Instrument (OMI) measurements, it has been found that the low surface reflectance and strong interaction between aerosol absorption and molecular scattering in UV wavelength range can be advantageous in retrieving aerosol optical properties, such as aerosol optical thickness (AOT) and optical type (or single scattering albedo), over the source regions as well as ocean areas. In addition, GEMS is expected to have finer spatial resolution compared to OMI (13 x 24 km2 at nadir), thereby less affected by sub-pixel clouds. In this study, we present sensitivity of spectral reflectance to aerosol optical properties in ultraviolet (UV) and visible wavelength range for a purpose to retrieve aerosol optical properties from GEMS. The so called UV-VIS algorithm plans to use spectral reflectance in 350-650 nm. The algorithm retrieves AOT and aerosol type using an inversion method, which adopts pre-calculated lookup table (LUT) for a set of assumed aerosol models. For the aerosol models optimized in Asia areas, the inversion data of Aerosol Robotic Network (AERONET) located in the target areas are selectively used to archive aerosol optical properties. As a result, major aerosol types representing dust, polluted dust, and absorbing/non-absorbing anthropogenic aerosols are constructed and used for the LUT calculations. We analyze the effect of cloud contamination on the retrieved AOT by

  7. Feasibility Study For A Spaceborne Ozone/Aerosol Lidar System

    NASA Technical Reports Server (NTRS)

    Campbell, Richard E.; Browell, Edward V.; Ismail, Syed; Dudelzak, Alexander E.; Carswell, Allan I.; Ulitsky, Arkady

    1997-01-01

    Because ozone provides a shield against harmful ultraviolet radiation, determines the temperature profile in the stratosphere, plays important roles in tropospheric chemistry and climate, and is a health risk near the surface, changes in natural ozone layers at different altitudes and their global impact are being intensively researched. Global ozone coverage is currently provided by passive optical and microwave satellite sensors that cannot deliver high spatial resolution measurements and have particular limitations in the troposphere. Vertical profiling DIfferential Absorption Lidars (DIAL) have shown excellent range-resolved capabilities, but these systems have been large, inefficient, and have required continuous technical attention for long term operations. Recently, successful, autonomous DIAL measurements have been performed from a high-altitude aircraft (LASE - Lidar Atmospheric Sensing Experiment), and a space-qualified aerosol lidar system (LITE - Laser In-space Technology Experiment) has performed well on Shuttle. Based on the above successes, NASA and the Canadian Space Agency are jointly studying the feasibility of developing ORACLE (Ozone Research with Advanced Cooperative Lidar Experiments), an autonomously operated, compact DIAL instrument to be placed in orbit using a Pegasus class launch vehicle.

  8. A high-resolution study of surfactant partitioning and kinetic limitations for two-component internally mixed aerosols

    NASA Astrophysics Data System (ADS)

    Suda, S. R.; Petters, M. D.

    2013-12-01

    Atmospheric aerosols serve as cloud condensation nuclei (CCN), altering cloud properties and ultimately affecting climate through their effect on the radiative balance. Aerosol CCN activity depends in part on aerosol composition and surfactant compounds are of particular interest because surfactants are enriched at the water/air interface, resulting in a radial concentration gradient within the aqueous droplet. Accurate treatment of the surfactant concentration gradient complicates the otherwise straightforward predictions of CCN activity for aerosols of known composition. To accurately evaluate predictions made by theory, laboratory studies investigating the relationship between critical supersaturation and dry diameter of particles that include surfactants require significant reduction in measurement uncertainty for both water-uptake and CCN measurements. Furthermore, uncertainties remain regarding kinetic limitations to surfactant partitioning that could result in deviation from predictions based on equilibrium thermodynamics. This study attempts to address some of these issues through high-resolution analysis of CCN activity of two-component mixed surfactant/non-surfactant aerosols at different internal mixing ratios performed with and without a water-uptake time delay to ascertain whether or not the observed effects are kinetically limited. We present new data for the aerosols consisting of 1) the ionic surfactant sodium dodecyl sulfate (SDS) with ammonium sulfate, 2) SDS with sodium chloride and 3) the strong non-ionic fluorosurfactant Zonyl with an organic proxy glucose. As a point of reference we also evaluated the mixture of ammonium sulfate with glucose. Aerosol activation diameters were determined using CCN analysis in conjunction with scanning mobility size classification and high sheath-to-aerosol flow ratios. This resulted in CCN-derived kappa values that could be determined within +/-5% relative error. To test whether dynamic surfactant partitioning

  9. Stability and aerosolization of pressurized metered dose inhalers containing thymopentin nanoparticles produced using a bottom-up process.

    PubMed

    Tan, Yinhe; Yang, Zhiwen; Pan, Xin; Chen, Meiwan; Feng, Min; Wang, Lili; Liu, Hu; Shan, Ziyun; Wu, Chuanbin

    2012-05-10

    The objective of this study was to investigate the stability and aerosolization of pressurized metered dose inhalers (pMDIs) containing thymopentin nanoparticles. Thymopentin nanoparticles, fabricated by a bottom-up process, were suspended in hydrofluoroalkane (HFA) 134a together with cineole and/or n-heptane to produce pMDI formulations. The stability study of the pMDIs obtained was carried out at ambient temperature for 6 months. The amount of thymopentin and the aerosolization properties of pMDIs were determined using high-performance liquid chromatography (HPLC) and a twin-stage impinger (TSI), respectively. Based on the results, thymopentin nanoparticles were readily suspended in HFA 134a with the aid of cineole and/or n-heptane to form physically stable pMDI formulations, and more than 98% of the labeled amount of thymopentin and over 50% of the fine particle fraction (FPF) of the pMDIs were achieved. During storage, it was found that for all pMDIs more than 97% of the labeled amount of thymopentin and FPF greater than 47% were achieved. Moreover, the size of thymopentin nanoparticles in propellant containing cineole and n-heptane showed little change. It is, therefore, concluded that the pMDIs comprising thymopentin nanoparticles developed in this study were stable and suitable for inhalation therapy for systemic action. PMID:22343132

  10. A case study on the aerosol-meteorology feedback for Europe with WRF/Chem

    NASA Astrophysics Data System (ADS)

    Forkel, R.; Werhahn, J.; McKeen, S.; Peckham, S.; Grell, G.; Suppan, P.

    2012-04-01

    A main topic of the investigations with online coupled meteorology-chemistry models, such as WRF/Chem is the feedback of air pollution on meteorology. For the current case study three WRF/Chem simulations for Europe and the North Atlantic are compared: a baseline case without any aerosol feedback on meteorology, a simulation with the direct effect of aerosol on radiation included, and a simulation including the direct effect as well as the indirect aerosol effect. An episode covering June and July in 2006 was considered. WRF/Chem's 3-modal MADE/SORGAM aerosol module was applied for this investigation, which was motivated by the AQMEII (Air Quality Model Evaluation International Initiative) model inter-comparison exercise. For the simulation including just the direct effect, the aerosol-radiation induced changes in temperature, boundary layer height, and clouds ("semi-direct effect") were found to dominate after some time. Over Central Europe the mean reduction of global radiation due to aerosol extinction alone was mostly 3 - 7 W m-2, but changes in cloud cover due to semi-direct effects resulted in monthly mean changes of ± 50 W m-2. The inclusion of the indirect aerosol effect resulted in an up to 70% lower cloud water content and a significantly higher mean rain water content over the North Atlantic. The simulated low cloud droplet and CCN concentrations there are a result of the low aerosol concentrations in this area. However, model analysis suggests these results are sensitive to boundary conditions and a possible underestimation of aerosol sources over the North Atlantic. In spite of the higher aerosol concentrations over continental Europe, the inclusion of the indirect aerosol effect also results sometimes in smaller cloud droplet numbers than the fixed droplet number that is assumed in the absence of aerosol-cloud interactions. The agreement between observed and simulated global radiation over Europe was found to be better for cloudy conditions when the

  11. Optimization of a counterflow virtual impactor (CVI) for studying aerosol effects on cloud droplet number

    SciTech Connect

    Anderson, T.L.

    1992-01-01

    This dissertation considers the problem of collecting cloud droplets in order to study the relatioship between droplet-nucleating particles and cloud droplet number concentration. Aerosol-induced modulation of cloud droplet number is potentially significant to global climate. The key activity was optimization of a Counterflow Virtual Impactor (CVI) for performing the cloud droplet collection. This involved numerical modeling of the collection process, construction and calibration of a new version of the CVI,and deployment of the new CVI in a field experiment. Numerical modeling revealed, with one cavent, that CVI measurements will not be significantly distorted either by droplet evaporation ahead of the collection plane or by droplet collisions during collection. The cavent is that if large (drizzle-size) droplets shatter upon collisions with smaller droplets, the measurement of droplet number could be distorted upwards. Laboratory calibration activities showed the new version to perform its size selection as predicted by theory and to have excellent cut sharpness. In addition, evidence of droplet shattering in the presence of large droplets was obtained. Thus, both laboratory and modeling evidence regarding large droplets lead to the suggestion that these be excluded from the inlet in field applications. The field experiment studying coastal stratiform clouds showed the CVI to perform well and to provide a large and unique data set relevant to examining the relationship between aerosol loading (number or volume) and cloud droplet number. Key resutls were (1) the majority of cloud droplet residue particles were smaller than one-tenth micrometer (diameter) in both clean and continentally influenced conditions, (2) total particle number variations were not correlated to cloud droplet number variations on any time scale, and (3) dominant sources of cloud variation, which tended to obscure the detection of aerosol effects, were meterology and cloud patchiness.

  12. Plume Aerosol Size Distribution Modeling and Comparisons to PrAIRie2005 Field Study Data

    NASA Astrophysics Data System (ADS)

    Cho, S.; Liggio, J.; Makar, P.; Li, S.; Racinthe, J.

    2006-12-01

    As part of the analysis phase of the PrAIRie2005 field study, the effects of different Edmonton-area emission sources on local air-quality are being examined. Four large coal-fired power-plants are located to the West of the city. Here, the effects of these power-plants on urban and regional air-quality will be examined, using both plume and regional air-quality models. During the last few decades, coal-fired power plants have been found to be as a major source of pollution, affecting public-health. According to NACEC (North American Commission for Environmental Corporation, 2001)'s report, 46 of the top 50 air polluters in North America were power plants. The importance of such sources has resulted in several attempts to improve understanding of the basic formation mechanisms of plume particulate matter. Sulphur dioxide contributes to acidifying emissions and to the production of secondary acidic aerosols that have been linked to a number of serious human health problems, acid rain and visibility (Seinfeld and Pandis, 1998; Hidy, 1984; Wilson and McMurray, 1981). Primary particulate matter originating directly from coal-fired power plants may also increase secondary particulate mass by providing a surface for sulphuric acid absorption . Environment Canada's PrAIRie2005 field study between August 12th and September 7th, 2005 included overflights and downwind measurements near the Edmonton powerplants (Wabamun, Sundance, Keephills and Genesee). The data collected consisted of particle size distributions, ozone, NOX, total mass and the chemical composition of fine particles. In order to investigate and improve our understanding of the formation mechanisms and physical properties of power-plant-generated aerosols in the Edmonton area, the Plume Aerosol Microphysical (PAM) model has been employed. This model accounts for gas-phase chemistry, aerosol microphysical processes (i.e. homogeneous/heterogeneous nucleation, condensation/evaporation and coagulation) and

  13. FTIR studies of low temperature sulfuric acid aerosols

    NASA Technical Reports Server (NTRS)

    Anthony, S. E.; Tisdale, R. T.; Disselkamp, R. S.; Tolbert, M. A.; Wilson, J. C.

    1995-01-01

    Sub-micrometer sized sulfuric acid H2SO4 particles were generated using a constant output atomizer source. The particles were then exposed to water vapor before being injected into a low temperature cell. Multipass transmission Fourier Transformation Infrared (FTIR) spectroscopy was used to determine the phase and composition of the aerosols as a function of time for periods of up to five hours. Binary H2SO4H2O aerosols with compositions from 35 to 95 wt % H2SO4 remained liquid for over 3 hours at room temperatures ranging from 189-240 K. These results suggest that it is very difficut to freeze SSAs via homogeneous nucleation. Attempts to form aerosols more dilute than 35 wt % H2SO4 resulted in ice formation.

  14. Synergy of Satellite-Surface Observations for Studying the Properties of Absorbing Aerosols in Asia

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee

    2010-01-01

    Through interaction with clouds and alteration of the Earth's radiation budget, atmospheric aerosols significantly influence our weather and climate. Monsoon rainfalls, for example, sustain the livelihood of more than half of the world's population. Thus, understanding the mechanism that drives the water cycle and freshwater distribution is high-lighted as one of the major near-term goals in NASA's Earth Science Enterprise Strategy. Every cloud droplet/ice-crystal that serves as an essential element in portraying water cycle and distributing freshwater contains atmospheric aerosols at its core. In addition, the spatial and temporal variability of atmospheric aerosol properties is complex due to their dynamic nature. In fact, the predictability of the tropical climate system is much reduced during the boreal spring, which is associated with the peak season of biomass burning activities and regional/long-range transport of dust aerosols. Therefore, to accurately assess the impact of absorbing aerosols on regional-to-global climate requires not only modeling efforts but also continuous observations from satellites, aircraft, networks of ground-based instruments and dedicated field experiments. Since 1997 NASA has been successfully launching a series of satellites the Earth Observing System - to intensively study, and gain a better understanding of, the Earth as an integrated system. Through participation in many satellite remote-sensing/retrieval and validation projects over the years, we have gradually developed and refined the SMART (Surface-sensing Measurements for Atmospheric Radiative Transfer) and COMMIT (Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile observatories, a suite of surface remote sensing and in-situ instruments that proved to be vital in providing high temporal measurements, which complement the satellite observations. In this talk, we will present SMART-COMMIT which has played key roles, serving as network or supersite

  15. High-efficiency particulate air filter test stand and aerosol generator for particle loading studies.

    PubMed

    Arunkumar, R; Hogancamp, Kristina U; Parsons, Michael S; Rogers, Donna M; Norton, Olin P; Nagel, Brian A; Alderman, Steven L; Waggoner, Charles A

    2007-08-01

    This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30 x 30 x 29 cm(3) nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5 to 12 standard m(3)/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150 degrees C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7 standard m(3)/min, high mass concentrations (approximately 25 mg/m(3)) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160 nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions.

  16. High-efficiency particulate air filter test stand and aerosol generator for particle loading studies.

    PubMed

    Arunkumar, R; Hogancamp, Kristina U; Parsons, Michael S; Rogers, Donna M; Norton, Olin P; Nagel, Brian A; Alderman, Steven L; Waggoner, Charles A

    2007-08-01

    This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30 x 30 x 29 cm(3) nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5 to 12 standard m(3)/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150 degrees C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7 standard m(3)/min, high mass concentrations (approximately 25 mg/m(3)) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160 nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions. PMID

  17. High-efficiency particulate air filter test stand and aerosol generator for particle loading studies

    NASA Astrophysics Data System (ADS)

    Arunkumar, R.; Hogancamp, Kristina U.; Parsons, Michael S.; Rogers, Donna M.; Norton, Olin P.; Nagel, Brian A.; Alderman, Steven L.; Waggoner, Charles A.

    2007-08-01

    This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30×30×29cm3 nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5to12standardm3/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150°C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7standardm3/min, high mass concentrations (˜25mg/m3) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions.

  18. Comparative Burkholderia pseudomallei natural history virulence studies using an aerosol murine model of infection

    PubMed Central

    Massey, Shane; Yeager, Linsey A.; Blumentritt, Carla A.; Vijayakumar, Sudhamathi; Sbrana, Elena; Peterson, Johnny W.; Brasel, Trevor; LeDuc, James W.; Endsley, Janice J.; Torres, Alfredo G.

    2014-01-01

    Melioidosis is an endemic disease caused by the bacterium Burkholderia pseudomallei. Concerns exist regarding B. pseudomallei use as a potential bio-threat agent causing persistent infections and typically manifesting as severe pneumonia capable of causing fatal bacteremia. Development of suitable therapeutics against melioidosis is complicated due to high degree of genetic and phenotypic variability among B. pseudomallei isolates and lack of data establishing commonly accepted strains for comparative studies. Further, the impact of strain variation on virulence, disease presentation, and mortality is not well understood. Therefore, this study evaluate and compare the virulence and disease progression of B. pseudomallei strains K96243 and HBPUB10303a, following aerosol challenge in a standardized BALB/c mouse model of infection. The natural history analysis of disease progression monitored conditions such as weight, body temperature, appearance, activity, bacteremia, organ and tissue colonization (pathological and histological analysis) and immunological responses. This study provides a detailed, direct comparison of infection with different B. pseudomallei strains and set up the basis for a standardized model useful to test different medical countermeasures against Burkholderia species. Further, this protocol serves as a guideline to standardize other bacterial aerosol models of infection or to define biomarkers of infectious processes caused by other intracellular pathogens. PMID:24603493

  19. Study of the efficacy of aerosol versus nonaerosol laundry products. Final report

    SciTech Connect

    Boggs, R.R.; Belmont, B.

    1987-10-01

    The California Air Resources Board estimates that 6.6 tons of photochemically reactive organic compounds (PROC) are released into the environment in California every day because of the use of aerosol laundry products. The project studied the efficacy, ease of product use, and PROC content for three major brands of pre-wash stain removers in available product forms and for five starch products in their available product forms. Efficacy of pre-wash products was generally found to be limited. They were particularly useful for oil and ball point ink removal. Aerosols were found to be slightly superior. PROC content varied from 16-76% on aerosols; none was found in nonaerosols. Aerosols were found to be slightly easier to use by the laboratory investigator. For starches, on synthetic fabrics Faultless aerosol was found to be superior. For natural fabrics, results were mixed. Efficacy per unit cost was found to be high for bulk starches. PROC content for the two aerosols was 5.8% for Faultless and 8.5% for Niagra. Aerosols were easiest to use and bulk products rather difficult to use.

  20. Retrieval of stratospheric aerosol distributions from SCIAMACHY limb measurements: methodology, sensitivity studies and first results

    NASA Astrophysics Data System (ADS)

    Ernst, Florian; von Savigny, Christian; Rozanov, Alexei; Rozanov, Vladimir; Bovensmann, Heinrich; Burrows, John P.

    Stratospheric aerosols play an important role for the global radiation budget and may signif-icantly affect the retrieval of trace gases from satellite observations. SAGE I -III provided a 25-year record of stratospheric aerosols by means of solar occultation technique. Since the demise of SAGE II and III in 2005/2006, the long-term stratospheric aerosol satellite record is jeopardized. The main goal of this work is to demonstrate that aerosol extinction profiles can be retrieved from SCIAMACHY limb scatter measurements to sustain the time series. Since the eruption of Pinatubo in 1991 was the last large source of volcanic aerosols in the strato-sphere, we have now the opportunity to retrieve background aerosol profiles. The radiative transfer model and retrieval package SCIATRAN is used to derive aerosol extinction profiles from SCIAMACHY limb data. The algorithm is based on a color-index ratio using limb radi-ance profiles at 470 nm and 750 nm wavelength. The algorithm, sensitivity studies and first results are presented here.

  1. Aqueous organic chemistry in the atmosphere: sources and chemical processing of organic aerosols.

    PubMed

    McNeill, V Faye

    2015-02-01

    Over the past decade, it has become clear that aqueous chemical processes occurring in cloud droplets and wet atmospheric particles are an important source of organic atmospheric particulate matter. Reactions of water-soluble volatile (or semivolatile) organic gases (VOCs or SVOCs) in these aqueous media lead to the formation of highly oxidized organic particulate matter (secondary organic aerosol; SOA) and key tracer species, such as organosulfates. These processes are often driven by a combination of anthropogenic and biogenic emissions, and therefore their accurate representation in models is important for effective air quality management. Despite considerable progress, mechanistic understanding of some key aqueous processes is still lacking, and these pathways are incompletely represented in 3D atmospheric chemistry and air quality models. In this article, the concepts, historical context, and current state of the science of aqueous pathways of SOA formation are discussed.

  2. A study of regional-scale aerosol assimilation using a Stretch-NICAM

    NASA Astrophysics Data System (ADS)

    Misawa, S.; Dai, T.; Schutgens, N.; Nakajima, T.

    2013-12-01

    Although aerosol is considered to be harmful to human health and it became a social issue, aerosol models and emission inventories include large uncertainties. In recent studies, data assimilation is applied to aerosol simulation to get more accurate aerosol field and emission inventory. Most of these studies, however, are carried out only on global scale, and there are only a few researches about regional scale aerosol assimilation. In this study, we have created and verified an aerosol assimilation system on regional scale, in hopes to reduce an error associated with the aerosol emission inventory. Our aerosol assimilation system has been developed using an atmospheric climate model, NICAM (Non-hydrostaric ICosahedral Atmospheric Model; Satoh et al., 2008) with a stretch grid system and coupled with an aerosol transport model, SPRINTARS (Takemura et al., 2000). Also, this assimilation system is based on local ensemble transform Kalman filter (LETKF). To validate this system, we used a simulated observational data by adding some artificial errors to the surface aerosol fields constructed by Stretch-NICAM-SPRINTARS. We also included a small perturbation in original emission inventory. This assimilation with modified observational data and emission inventory was performed in Kanto-plane region around Tokyo, Japan, and the result indicates the system reducing a relative error of aerosol concentration by 20%. Furthermore, we examined a sensitivity of the aerosol assimilation system by varying the number of total ensemble (5, 10 and 15 ensembles) and local patch (domain) size (radius of 50km, 100km and 200km), both of which are the tuning parameters in LETKF. The result of the assimilation with different ensemble number 5, 10 and 15 shows that the larger the number of ensemble is, the smaller the relative error become. This is consistent with ensemble Kalman filter theory and imply that this assimilation system works properly. Also we found that assimilation system

  3. The 5-6 December 1991 FIRE IFO II jet stream cirrus case study: Possible influences of volcanic aerosols

    SciTech Connect

    Sassen, K.; Starr, D.O.C.; Melfi, S.H.; Spinhirne, J.D.; Poellot, M.R.; Eberhard, W.L.; Eloranta, E.W.; Hagen, D.E.; Hallett, J.

    1995-01-01

    In presenting an overview of the cirrus clouds comprehensively studied by ground-based and airborne sensors from Coffeyville, Kansas, during the 5-6 December 1992 Project FIRE IFO II case study period, evidence is provided that volcanic aerosols from the June 1991 Pinatubo eruptions may have significantly influenced the formation and maintenance of the cirrus. Following the local appearance of a spur of stratospheric volcanic debris from the subtropics, a series of jet streaks subsequently conditioned the troposphere through tropopause foldings with sulfur-based particles that became effective cloud-forming nuclei in cirrus clouds. Aerosol and ozone measurements suggest a complicated history of stratospheric-tropospheric exchanges embedded within the upper-level flow, and cirrus cloud formation was noted to occur locally at the boundaries of stratospheric aerosol-enriched layers that became humidified through diffusion, precipitation, or advective processes. Apparent cirrus cloud alterations include abnormally high ice crystal concentrations (up to {approximately}600 L{sup {minus}1}), complex radial ice crystal types, and relatively large haze particles in cirrus uncinus cell heads at temperatures between {minus}40{degrees} and {minus}50{degrees}C. Implications for volcanic-cirrus cloud climate effects and usual (nonvolcanic aerosol) jet stream cirrus cloud formation are discussed. 42 refs., 25 figs., 3 tabs.

  4. The 5-6 December 1991 FIRE IFO 2 Jet Stream Cirrus Case Study: Possible Influences of Volcanic Aerosols

    NASA Technical Reports Server (NTRS)

    Sassen, Kenneth; Starr, David OC.; Mace, Gerald G.; Poellot, Michael R.; Melfi, S. H.; Eberhard, Wynn L.; Spinhirne, James D.; Eloranta, E. W.; Hagen, Donald E.; Hallett, John

    1996-01-01

    In presenting an overview of the cirrus clouds comprehensively studied by ground based and airborne sensors from Coffeyville, Kansas, during the 5-6 December 1992 First ISCCP Regional Experiment (FIRE) intensive field observation (IFO) case study period, evidence is provided that volcanic aerosols from the June 1991 Pinatubo eruptions may have significantly influenced the formation and maintenance of the cirrus. Following the local appearance of a spur of stratospheric volcanic debris from the subtropics, a series of jet streaks subsequently conditioned the troposphere through tropopause foldings with sulfur based particles that became effective cloud forming nuclei in cirrus clouds. Aerosol and ozone measurements suggest a complicated history of stratospheric-tropospheric exchanges embedded with the upper level flow, and cirrus cloud formation was noted to occur locally at the boundaries of stratospheric aerosol enriched layers that became humidified through diffusion, precipitation, or advective processes. Apparent cirrus cloud alterations include abnormally high ice crystal concentrations (up to approximately 600 L(exp. 1)), complex radial ice crystal types, and relatively large haze particles in cirrus uncinus cell heads at temperatures between -40 and -50 degrees C. Implications for volcanic-cirrus cloud climate effects and unusual (nonvolcanic) aerosol jet stream cirrus cloud formation are discussed.

  5. A satellite view of aerosols in the climate system

    NASA Technical Reports Server (NTRS)

    Kaufman, Yoram J.; Tanre, Didier; Boucher, Olivier

    2002-01-01

    Anthropogenic aerosols are intricately linked to the climate system and to the hydrologic cycle. The net effect of aerosols is to cool the climate system by reflecting sunlight. Depending on their composition, aerosols can also absorb sunlight in the atmosphere, further cooling the surface but warming the atmosphere in the process. These effects of aerosols on the temperature profile, along with the role of aerosols as cloud condensation nuclei, impact the hydrologic cycle, through changes in cloud cover, cloud properties and precipitation. Unravelling these feedbacks is particularly difficult because aerosols take a multitude of shapes and forms, ranging from desert dust to urban pollution, and because aerosol concentrations vary strongly over time and space. To accurately study aerosol distribution and composition therefore requires continuous observations from satellites, networks of ground-based instruments and dedicated field experiments. Increases in aerosol concentration and changes in their composition, driven by industrialization and an expanding population, may adversely affect the Earth's climate and water supply.

  6. OH Radical Aging of Model Primary Organic Aerosols In Smog Chamber Studies

    NASA Astrophysics Data System (ADS)

    Lambe, A. T.; Zhang, J.; Sage, A. M.; Donahue, N. M.

    2006-12-01

    Most of the fine primary organic carbon (OC) in the atmosphere is saturated. Thus, by OC mass balance alone, OH radicals should be important in organic aerosol processing because saturated OC is unreactive to ozone and vulnerable to NO3 oxidation only at night. However, the importance of OH-induced heterogeneous oxidation remains uncertain because laboratory and ambient analysis is a challenge. Most laboratory aging studies have been conducted in flow tube reactors with extremely high radical concentrations and short exposure times. While these pioneering experiments have revealed efficient OH uptake, a confounding issue remains that both oxidant and reagent losses are rate-limited by diffusion of the oxidant to the phase interface. Examining these systems over much longer timescales in smog chamber experiments is therefore desirable, but established methods of OH radical production in smog chamber studies typically require some combination of UV illumination, high NOx, or radical cycling. Thus, employing these methods results in experimental conditions that either do not represent atmospheric conditions or cannot produce a sufficiently high flux of OH radicals - these shortcomings are acceptable for some applications, but are significant hindrances when heterogeneous aging is the experimental objective. Our approach has been to use alkene ozonolysis as a continuous, low-NOx, dark source of OH. Specifically, we use 2,3-dimethyl-2-butene (tetramethylethylene, TME) because ozonolysis results in an OH yield near unity. Furthermore, the organic TME ozonolysis products have high vapor pressures, so they do not participate directly in condensed-phase chemistry. To maintain a constant radical production rate, fresh reagents are delivered to the chamber to replenish TME and O3 as they react. TME is delivered continuously via capillary liquid flow with constant evaporation from a droplet at the capillary tip into a carrier stream. Ozone is held at a constant, high value by

  7. Case study of modeled aerosol optical properties during the SAFARI 2000 campaign.

    PubMed

    Kuzmanoski, Maja; Box, Michael A; Schmid, Beat; Russell, Philip B; Redemann, Jens

    2007-08-01

    We present modeled aerosol optical properties (single scattering albedo, asymmetry parameter, and lidar ratio) in two layers with different aerosol loadings and particle sizes, observed during the Southern African Regional Science Initiative 2,000 (SAFARI 2,000) campaign. The optical properties were calculated from aerosol size distributions retrieved from aerosol layer optical thickness spectra, measured using the NASA Ames airborne tracking 14-channel sunphotometer (AATS-14) and the refractive index based on the available information on aerosol chemical composition. The study focuses on sensitivity of modeled optical properties in the 0.3-1.5 microm wavelength range to assumptions regarding the mixing scenario. We considered two models for the mixture of absorbing and nonabsorbing aerosol components commonly used to model optical properties of biomass burning aerosol: a layered sphere with absorbing core and nonabsorbing shell and the Maxwell-Garnett effective medium model. In addition, comparisons of modeled optical properties with the measurements are discussed. We also estimated the radiative effect of the difference in aerosol absorption implied by the large difference between the single scattering albedo values (approximately 0.1 at midvisible wavelengths) obtained from different measurement methods for the case with a high amount of biomass burning particles. For that purpose, the volume fraction of black carbon was varied to obtain a range of single scattering albedo values (0.81-0.91 at lambda=0.50 microm). The difference in absorption resulted in a significant difference in the instantaneous radiative forcing at the surface and the top of the atmosphere (TOA) and can result in a change of the sign of the aerosol forcing at TOA from negative to positive.

  8. Study of aerosol behavior on the basis of morphological characteristics during festival events in India

    NASA Astrophysics Data System (ADS)

    Agrawal, Anubha; Upadhyay, Vinay K.; Sachdeva, Kamna

    2011-07-01

    Two important festival events were selected to assess their impacts on atmospheric chemistry by understanding settling velocity and emission time of aerosols. Using high volume sampler, aerosols were collected in a sequential manner to understand settling velocity and emission time of aerosols on a particular day. Composition and total suspended particulate load of the aerosols collected during the festivals were used as markers for strengthening the assessment. Terminal settling velocity of the aerosols were calculated using morphological and elemental compositional data, obtained from scanning electron microcopy (SEM) and energy dispersive X-ray (EDX) study. Aerosol load, black carbon, aromatic carbon and terminal velocity calculations were correlated to obtain conclusion that aerosols collected on the festival day might have been emitted prior to the festival. Settling time of aerosols collected on 17th and 19th October'09 during Diwali were found to be 36.5 (1.5 days) and 12.8 h, respectively. Carbon concentration estimated using EDX was found to be almost double in the sample collected after 2 days of the festival event. This strengthens our inference of time calculation where carbon with high concentration of load must have settled approximately after two days of the event. Settling time of aerosols collected on Holi morning and afternoon was found to be 1.7 and 24.8 h, respectively. Further, because of the small distance of 5.4 km between the meteorological station and sampling site, observed TSP values were compared with theoretical load values, calculated by using visibility values taken from the meteorological data. And it was found that both experimental and calculated values are close to each other about 50% of the times, which proves the assumption that experimental and meteorological data are comparable.

  9. Ground-based SMART-COMMIT Measurements for Studying Aerosol and Cloud Properties

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee

    2008-01-01

    From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations cover large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and/or the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite data sets. The development and deployment of SMARTCOMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile facilities are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instruments fall into three categories: flux radiometer, radiance sensor and in-situ probe. In this paper, we will demonstrate the capability of SMART-COMMIT in recent field campaigns (e.g., CRYSTAL-FACE, UAE 2, BASEASIA, NAMMA) that were designed and executed to study the compelling variability in temporal scale of both anthropogenic and natural aerosols (e.g., biomass-burning smoke, airborne dust) and cirrus clouds. We envision robust approaches in which well-collocated ground-based measurements and space-borne observations will greatly advance our knowledge of extensive aerosols and clouds.

  10. A Study of the Stratospheric Aerosols on Jupiter Using Hubble Space Telescope Data

    NASA Astrophysics Data System (ADS)

    Frost, J.; Valera, N.; Fernandez, J.; Smyth, B.; Erazo, J.; Carlson, B. E.

    2011-12-01

    We present a study of the stratospheric aerosols in Jupiter's atmosphere using Hubble Space Telescope Data taken in September 1997 with the Wide Field Planetary Camera 2. It was during this time that Jupiter's Great Dark Spot was observed and we present some results concerning the Great Dark Spot. Jupiter's Great Dark Spot was roughly twice the size of Earth and was located in the north pole. The phenomenon lasted only a few weeks, and was observed first in 1977, and then again in 2000 by NASA's Cassini flyby of Jupiter. The composition of the spot is uncertain; is it made of aerosols or something else? We also will give a comparative study of the aerosols in the north and south poles. The Hubble Data used was at wavelength filters of 218, 255, 336, 410, 673, 890, and 953 nanometers. It was found that a ratio plot of 410nm data divided by the 218nm data gave very clear structural features of the Dark Spot and other aerosol regions. Data analysis was performed on these different regions and the results were compared. The Data analysis consisted of creating spectral plots of the average intensity versus wavelength for the different regions. Our results show that as you move poleward, the aerosol concentration increases. Also, there are differences between the concentration and composition of the aerosols in the north and south poles. The aerosols in the south pole are thicker than the aerosols in the north pole. We also found that the aerosols in the north showed little variation in composition and concentration with respect to changes in longitude, whereas the aerosols in the south pole are more concentrated at a System III Central Meridian Longitude value of zero. The analysis of the Great Dark Spot showed that the Dark Spot is darker (more absorptive) in the ultra violet 218 to 336 nm and is slightly brighter at 890nm (methane abortion band) than any other regions in the north pole. This would suggest that the Dark Spot is made of aerosols and contains more

  11. Production and Study of Titan's Aerosols Analogues with A RF Low Pressure Plasma Discharge

    SciTech Connect

    Szopa, C.; Cernogora, G.; Correia, J.J.; Boufendi, L.; Jolly, A.

    2005-10-31

    The atmosphere of Titan, the biggest satellite of Saturn, contains aerosols produced by the organic chemistry induced by the photochemistry of N2 and CH4, the major gaseous atmospheric compounds. In spite of their importance for the properties of the Titan's atmosphere, and for organic chemistry, only few direct information are available about them because of the limitations of the observational techniques, and their processes of formation and growth are not understood. In order to bring answers to these questions, we developed a new type of laboratory simulation to produce analogues of Titan's aerosols (known as tholins) with a low pressure Radio Frequency plasma discharge. The main originality of this experiment (named PAMPRE) comes from its ability to produce particles in volume, as they are maintained in levitation by electrostatic forces compensating gravity, whereas the other experiments produce tholins on the reactors walls or a substrate. We initiated our investigations by a study of the properties of the produced particles as a function of the plasma operating conditions (i.e. amount of CH4 in N2, injected RF power, pressure, and gas flow). We here present the results of this study.

  12. Retrieval of Aerosol Optical Depth in Vicinity of Broken Clouds from Reflectance Ratios: Case Study

    SciTech Connect

    Kassianov, Evgueni I.; Ovchinnikov, Mikhail; Berg, Larry K.; McFarlane, Sally A.; Flynn, Connor J.; Ferrare, Richard; Hostetler, Chris A.; Alexandrov, Mikhail

    2010-10-06

    A recently developed reflectance ratio (RR) method for the retrieval of aerosol optical depth (AOD) is evaluated using extensive airborne and ground-based data sets collected during the Cloud and Land Surface Interaction Campaign (CLASIC) and the Cumulus Humilis Aerosol Processing Study (CHAPS), which took place in June 2007 over the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains site. A detailed case study is performed for a field of single-layer shallow cumuli observed on June 12, 2007. The RR method is applied to retrieve the spectral values of AOD from the reflectance ratios measured by the MODIS Airborne Simulator (MAS) for two pairs of wavelengths (660 and 470 nm and 870 and 470 nm) collected at a spatial resolution of 0.05 km. The retrieval is compared with an independent AOD estimate from three ground-based Multi-filter Rotating Shadowband Radiometers (MFRSRs). The interpolation algorithm that is used to project MFRSR point measurements onto the aircraft flight tracks is tested using AOD derived from NASA Langley High Spectral Resolution Lidar (HSRL). The RR AOD estimates are in a good agreement (within 5%) with the MFRSR-derived AOD values for the 660-nm wavelength. The AODs obtained from MAS reflectance ratios overestimate those derived from MFRSR measurements by 15-30% for the 470-nm wavelength and underestimate the 870-nm AOD by the same amount.

  13. Aerosolized antibiotics for ventilator-associated pneumonia: lessons from experimental studies.

    PubMed

    Rouby, Jean-Jacques; Bouhemad, Belaïd; Monsel, Antoine; Brisson, Hélène; Arbelot, Charlotte; Lu, Qin

    2012-12-01

    The aim of this review is to perform a critical analysis of experimental studies on aerosolized antibiotics and draw lessons for clinical use in patients with ventilator-associated pneumonia. Ultrasonic or vibrating plate nebulizers should be preferred to jet nebulizers. During the nebulization period, specific ventilator settings aimed at decreasing flow turbulence should be used, and discoordination with the ventilator should be avoided. The appropriate dose of aerosolized antibiotic can be determined as the intravenous dose plus extrapulmonary deposition. If these conditions are strictly respected, then high lung tissue deposition associated with rapid and efficient bacterial killing can be expected. For aerosolized aminoglycosides and cephalosporins, a decrease in systemic exposure leading to reduced toxicity is not proven by experimental studies. Aerosolized colistin, however, does not easily cross the alveolar-capillary membrane even in the presence of severe lung infection, and high doses can be delivered by nebulization without significant systemic exposure. PMID:23135264

  14. Feasibility study for GCOM-C/SGLI: Retrieval algorithms for carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Mukai, Sonoyo; Sano, Itaru; Yasumoto, Masayoshi; Fujito, Toshiyuki; Nakata, Makiko; Kokhanovsky, Alexander

    2016-04-01

    possibility of GCOM-C1 / SGLI related to remote sensing for aerosols and/or clouds can be examined. [1] Mukai, S., M. Yasumoto and M. Nakata, 2014: Estimation of biomass burning influence on air pollution around Beijing from an aerosol retrieval model. The Scientific World Journal, Article ID 649648. [2] Mukai, S., M. Nakata, M. Yasumoto, I. Sano and A. Kokhanovsky, 2015:A study of aerosol pollution episode due to agriculture biomass burning in the east-central China using satellite data, Front. Environ. Sci., 3:57, doi: 10.3389/fenvs.2015.00057.

  15. Aerosols and past environments: A global investigation into cave aerosol identification, distribution, and contribution to speleothem geochemistry

    NASA Astrophysics Data System (ADS)

    Dredge, J. A.; Fairchild, I. J.; Harrison, R. M.; Woodhead, J. D.; Hellstrom, J.; Mattey, D.

    2013-12-01

    A new sector of interest is developing within cave science regarding the influence of aerosols on the cave environment and the potential speleothem palaeoenvironmental aerosol record which may be preserved. This paper presents the results from a global collaboration project which explored all aspects of aerosols in the cave environment. Cave aerosol identification, introduction and distribution Cave aerosol multivariable environmental monitoring projects were carried out in the UK, Spain, Austria and Australia. Results demonstrate that cave ventilation is the predominant control on the introduction and distribution of aerosols throughout the cave environment (Dredge et al., 2013). Consequently, aerosol transportation processes vary as a result of seasonal ventilation changes and cave morphological features. Cave aerosol contribution to speleothem geochemistry Aerosol contributions to speleothem geochemistry were determined by comparing monitored aerosol deposition to speleothem trace element data. Significant aerosol contribution scenarios were identified as: hiatus events, high aerosol flux situations and secondary microbial concentration processes. Modelling indicates that a >99.9% reduction in drip water flow rates is required to reduce trace element supply quantities to equal that of aerosol supply (Dredge et al., 2013). Aerosol palaeoclimate and palaeoenvironmental records Aerosol contributions and the ability to utilise aerosol records in speleothem are investigated in samples from Gibraltar and Australia. Long range dust sources and past atmospheric circulation over several glacial cycles is studied through Sr isotope analysis of a Flowstone core from Gibraltar. Results of organic fire proxy analysis from Australian speleothem samples indicate an aerosol deposition forest fire record. In addition to primary fire deposition, secondary biological feedbacks and subsequent bioaccumulation processes in the cave environment are explored by microbial analysis

  16. A numerical simulation of atmospheric photochemical processes including interactions with aerosol particles

    SciTech Connect

    Hackler, M.A.

    1989-01-01

    We propose a comprehensive model of atmospheric photochemical processes that can be used to investigate the interactions between gas species and aerosol particles. We considered both gas and particle phase reactions, transport of material between these phases, convection, turbulent diffusion, particle growth, coagulation, nucleation, and sources. The aerosol particle phase is not forced to follow the gas phase in equilibrium; transport to the particles is described by diffusion to the particle surface. The resulting model treats 33 gas phase species and 39 particles phase species; 16 of these are transported between the phases. The particle size distribution is approximated by 9 sections between 0.01 and 10 {mu}m diameter. Strong interactions between the gas and particles are seen. Higher relative humidity results in more particle volume and surface area, allowing the interphase transport to become competitive with the reaction terms. In particular, at high relative humidities the increased scavenging of HO{sub 2} radicals by particles reduces the O{sub 3} maximum concentration. This effect is seen only on days when the maximum relative humidity exceeds 90%. This conclusion has implications for the applicability of models developed for the Los Angeles Basin, where the maximum relative humidity rarely exceeds 75%, to more humid climates like Houston.

  17. Kinetic study of esterification of sulfuric acid with alcohols in aerosol bulk phase

    NASA Astrophysics Data System (ADS)

    Li, J.; Jang, M.

    2013-09-01

    In this study, we hypothesize that the formation of organosulfates through the reactions between sulfuric acid and alcohols in the aerosol bulk phase is more efficient than that in solution chemistry. To prove this hypothesis, the kinetics of the organosulfate formation was investigated for both aliphatic alcohol with single OH group (e.g., 1-heptanol) and the multialcohols ranging from semivolatiles (e.g., hydrated-glyoxal and glycerol) to nonvolatiles (e.g., sucrose) using analytical techniques directly monitoring aerosol bulk phase. Both the forward (k1) and the backward (k-1) reaction rate constants of organosulfate formation via the particle phase esterification of 1-heptanol with sulfuric acid were estimated using a Fourier Transform Infrared (FTIR) spectrometer equipped with a flow chamber under varying humidities. Both k1 and k-1 are in orders of 10-3 L mol-1 min-1, which are three orders of magnitude higher than the reported values obtained in solution chemistry. The formation of organosulfate in the H2SO4 aerosol internally mixed with multialcohols was studied by measuring the proton concentration of the aerosol collected on the filter using a newly developed Colorimetry integrated with a Reflectance UV-Visible spectrometer (C-RUV). The formation of organosulfate significantly decreases aerosol acidity due to the transformation of H2SO4 into dialkylsulfates. The forward reaction rate constants for the dialkylsulfate formation in the multialcohol-H2SO4 aerosols were also three orders of magnitude greater than the reported values in solution chemistry. The water content (MH2O) in the multialcohol-H2SO4 particle was monitored using the FTIR spectrometer. A large reduction of MH2O accords with the high yield of organosulfate in aerosol. Based on this study, we conclude that organosulfate formation in atmospheric aerosol, where both alcohols and sulfuric acid are found together, is significant.

  18. Use of the ARM Measurements of Spectral Zenith Radiance for Better Understanding of 3D Cloud-Radiation Processes & Aerosol-Cloud Interaction

    SciTech Connect

    Alexander Marshak; Warren Wiscombe; Yuri Knyazikhin; Christine Chiu

    2011-05-24

    We proposed a variety of tasks centered on the following question: what can we learn about 3D cloud-radiation processes and aerosol-cloud interaction from rapid-sampling ARM measurements of spectral zenith radiance? These ARM measurements offer spectacular new and largely unexploited capabilities in both the temporal and spectral domains. Unlike most other ARM instruments, which average over many seconds or take samples many seconds apart, the new spectral zenith radiance measurements are fast enough to resolve natural time scales of cloud change and cloud boundaries as well as the transition zone between cloudy and clear areas. In the case of the shortwave spectrometer, the measurements offer high time resolution and high spectral resolution, allowing new discovery-oriented science which we intend to pursue vigorously. Research objectives are, for convenience, grouped under three themes: • Understand radiative signature of the transition zone between cloud-free and cloudy areas using data from ARM shortwave radiometers, which has major climatic consequences in both aerosol direct and indirect effect studies. • Provide cloud property retrievals from the ARM sites and the ARM Mobile Facility for studies of aerosol-cloud interactions. • Assess impact of 3D cloud structures on aerosol properties using passive and active remote sensing techniques from both ARM and satellite measurements.

  19. Research highlights: laboratory studies of the formation and transformation of atmospheric organic aerosols.

    PubMed

    Borduas, Nadine; Lin, Vivian S

    2016-04-01

    Atmospheric particles are emitted from a variety of anthropogenic and natural precursors and have direct impacts on climate, by scattering solar irradiation and nucleating clouds, and on health, by causing oxidative stress in the lungs when inhaled. They may also form from gaseous precursors, creating complex mixtures of organic and inorganic material. The chemical composition and the physical properties of aerosols will evolve during their one-week lifetime which will consequently change their impact on climate and health. The heterogeneity of aerosols is difficult to model and thus atmospheric aerosol research strives to characterize the mechanisms involved in nucleating and transforming particles in the atmosphere. Recent advances in four laboratory studies of aerosol formation and aging are highlighted here.

  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 polarization effects on atmospheric correction and aerosol retrievals in ocean color remote sensing.

    PubMed

    Wang, Menghua

    2006-12-10

    The current ocean color data processing system for the Sea-viewing Wide Field-of-View Sensor (SeaWiFS) and the moderate resolution imaging spectroradiometer (MODIS) uses the Rayleigh lookup tables that were generated using the vector radiative transfer theory with inclusion of the polarization effects. The polarization effects, however, are not accounted for in the aerosol lookup tables for the ocean color data processing. I describe a study of the aerosol polarization effects on the atmospheric correction and aerosol retrieval algorithms in the ocean color remote sensing. Using an efficient method for the multiple vector radiative transfer computations, aerosol lookup tables that include polarization effects are generated. Simulations have been carried out to evaluate the aerosol polarization effects on the derived ocean color and aerosol products for all possible solar-sensor geometries and the various aerosol optical properties. Furthermore, the new aerosol lookup tables have been implemented in the SeaWiFS data processing system and extensively tested and evaluated with SeaWiFS regional and global measurements. Results show that in open oceans (maritime environment), the aerosol polarization effects on the ocean color and aerosol products are usually negligible, while there are some noticeable effects on the derived products in the coastal regions with nonmaritime aerosols.

  2. An Observational Study of the Relationship between Cloud, Aerosol and Meteorology in Broken Low-Level Cloud Conditions

    NASA Technical Reports Server (NTRS)

    Loeb, Norman G.; Schuster, Gregory L.

    2008-01-01

    Global satellite analyses showing strong correlations between aerosol optical depth and 3 cloud cover have stirred much debate recently. While it is tempting to interpret the results as evidence of aerosol enhancement of cloud cover, other factors such as the influence of meteorology on both the aerosol and cloud distributions can also play a role, as both aerosols and clouds depend upon local meteorology. This study uses satellite observations to examine aerosol-cloud relationships for broken low-level cloud regions off the coast of Africa. The analysis approach minimizes the influence of large-scale meteorology by restricting the spatial and temporal domains in which the aerosol and cloud properties are compared. While distributions of several meteorological variables within 5deg 5deg latitude-longitude regions are nearly identical under low and high aerosol optical depth, the corresponding distributions of single-layer low cloud properties and top-of-atmosphere radiative fluxes differ markedly, consistent with earlier studies showing increased cloud cover with aerosol optical depth. Furthermore, fine-mode fraction and Angstrom Exponent are also larger in conditions of higher aerosol optical depth, even though no evidence of systematic latitudinal or longitudinal gradients between the low and high aerosol optical depth populations are observed. When the analysis is repeated for all 5deg 5deg latitude-longitude regions over the global oceans (after removing cases in which significant meteorological differences are found between the low and high aerosol populations), results are qualitatively similar to those off the coast of Africa.

  3. Advantages and Challenges in using Multi-Sensor Data for Studying Aerosols from Space

    NASA Astrophysics Data System (ADS)

    Leptoukh, Gregory

    We are living now in the golden era of numerous sensors measuring aerosols from space, e.g., MODIS, MISR, MERIS, OMI, POLDER, etc. Data from multiple sensors provide a more complete coverage of physical phenomena than data from a single sensor. These sensors are rather different from each other, are sensitive to various parts of the atmosphere, use different aerosol models and treat surface differently when retrieving aerosols. However, they complement each other thus providing more information about spatial, vertical and temporal distribution of aerosols. In addition to differences in instrumentation, retrieval algorithms and calibration, there are quite substantial differences in processing algorithms from Level 0 up to Level 3 and 4. Some of these differences in processing steps, at times not well documented and not widely known by users, can lead to quite significant differences in final products. Without documenting all the steps leading to the final product, data users will not trust the data and/or may use data incorrectly. Data by themselves without quality assessment and provenance are not sufficient to make accurate scientific conclusions. In this paper we provide examples of striking differences between aerosol optical depth data from MODIS, MISR, and MERIS that can be attributed to differences in a certain threshold, aggregation methods, and the dataday definition. We talk about challenges in developing processing provenance. Also, we address issues of harmonization of data, quality and provenance that is needed to guide the multi-sensor data usage and avoid apples-to-oranges comparison and fusion.

  4. What Can We Learn From Laboratory Studies of Inorganic Sea Spray Aerosol?

    NASA Astrophysics Data System (ADS)

    Salter, M. E.; Zieger, P.; Acosta Navarro, J. C.; Grythe, H.; Kirkevag, A.; Rosati, B.; Riipinen, I.; Nilsson, E. D.

    2015-12-01

    Since 2013 we have been operating a temperature-controlled plunging-jet sea spray aerosol chamber at Stockholm University using inorganic artificial seawater. Using size-resolved measurements of the foam bubbles responsible for the aerosol production we were able to show that it is changes to these foam bubbles which drive the observed changes in aerosol production and size distribution as water temperature changes (Salter et al., 2014). Further, by combining size-resolved measurements of aerosol production as a function of water temperature with measurements of air entrainment by the plunging-jet we have developed a temperature-dependent sea spray source function for deployment in large-scale models (Salter et al., 2015). We have also studied the hygroscopicity, morphology, and chemical composition of the inorganic sea spray aerosol produced in the chamber. The sea spray aerosol generated from artificial seawater exhibited lower hygroscopic growth than both pure NaCl and output from the E-AIM aerosol thermodynamics model when all relevant inorganic ions in the sea salt were included. Results from sensitivity tests using a large-scale earth system model suggest that the lower hygroscopicity observed in our laboratory measurements has important implications for calculations of the radiative balance of the Earth. In addition, size-dependent chemical fractionation of several inorganic ions was observed relative to the artificial seawater with potentially important implications for the chemistry of the marine boundary layer. Each of these studies suggest that there is still much to be learned from rigorous experiments using inorganic seawater proxies. Salter et al., (2014), On the seawater temperature dependence of the sea spray aerosol generated by a continuous plunging jet. J. Geophys. Res. Atmos., 119, 9052-9072, doi: 10.1002/2013JD021376 Salter et al., (2015), An empirically derived inorganic sea spray source function incorporating sea surface temperature. Atmos

  5. A study of aerosol optical properties at the global GAW station Bukit Kototabang, Sumatra, Indonesia

    NASA Astrophysics Data System (ADS)

    Nurhayati, N.; Nakajima, Teruyuki

    2012-01-01

    There have been very few studies carried out in Indonesia on the atmospheric aerosol optical properties and their impact on the earth climate. This study utilized solar radiation and aerosol measurement results of Indonesian GAW station Bukit Kototabang in Sumatra. The radiation data of nine years were used as input to a radiation simulation code for retrieving optically equivalent parameters of aerosols, i.e., aerosol optical thickness (AOT), coarse particle to fine particle ratio ( γ-ratio), and soot fraction. Retrieval of aerosol properties shows that coarse particles dominated at the station due to high relative humidity (RH) reaching more than 80% throughout the year. AOT time series showed a distinct two peak structure with peaks in MJJ and NDJ periods. The second peak corresponds to the period of high RH suggesting it was formed by active particle growth with large RH near 90%. On the other hand the time series of hot spot number, though it is only for the year of 2004, suggests the first peak was strongly contributed by biomass burning aerosols. The γ-ratio took a value near 10 throughout the year except for November and December when it took a larger value. The soot fraction varies in close relation with the γ-ratio, i.e. low values when γ was large, as consistent with our proposal of active particle growth in the high relative periods.

  6. A comparison between the processing of Titan aerosols analogs by ionizing photons and energetic cosmic rays.

    NASA Astrophysics Data System (ADS)

    De Araujo Vasconcelos, Fredson; Pilling, Sergio; Boduch, Philippe; Alexandre Souza Bergantini, M.; Ding, M. Jingjie J.; Rothard, Hermann; Robson Rocha, Will

    Titan, the largest satellite of Saturn, has an atmosphere mainly made of N_{2} and CH_{4} and includes traces of several simple organic compounds. This atmosphere also partly consists of haze and erosol particles which during the last 4.5 gigayears have been processed by electric discharges, ions, and ionizing photons, being slowly deposited over Titańs surface. In this work, we investigate the possible effects produced by ionizing photons (vacuum ultraviolet and soft X-rays) and cosmic ray analogs (15.7 MeV (16) O (+5) ) on Titan aerosol analogs in an attempt to simulate some prebiotic photochemistry. For photons, the experiments have been performed using a high vacuum portable chamber from the Laboratorio de Astroquimica e Astrobiologia (LASA/UNIVAP) coupled to the the Brazilian Synchrotron Light Source (LNLS) in Campinas, Brazil. For ions, the investigation was performed at the Grand Accelerateur National d’Ions Lourds (GANIL) Caen, France. In-situ sample analyses were performed by a Fourier transform infrared spectrometer at different fluences. During the sample processing, the infrared spectra have presented several new organic molecules, including nitriles, HCN and aromatic CN compounds. The processing of the sample by fast ions has enhanced the formation of daughter species in the Titan aerosol sample when compared with the products from the employing VUV and soft X-rays photons. The destruction cross section of the parent species was determined, as well as, the formation cross section for some selected daughter species. Molecular Half-lives were extrapolated to the Titańs environment. This investigation confirms previous results which showed that the organic chemistry on frozen moons inside Solar system can be very complex and extremely rich in prebiotic compounds. Authors would like to tanks the agencies FAPESP (JP-2009/18304-0), CAPES-Cofecub (569/2007), INCT-A and CNPq for the financial support.

  7. On-line Meteorology-Chemistry/Aerosols Modelling and Integration for Risk Assessment: Case Studies

    NASA Astrophysics Data System (ADS)

    Bostanbekov, Kairat; Mahura, Alexander; Nuterman, Roman; Nurseitov, Daniyar; Zakarin, Edige; Baklanov, Alexander

    2016-04-01

    On regional level, and especially in areas with potential diverse sources of industrial pollutants, the risk assessment of impact on environment and population is critically important. During normal operations, the risk is minimal. However, during accidental situations, the risk is increased due to releases of harmful pollutants into different environments such as water, soil, and atmosphere where it is following processes of continuous transformation and transport. In this study, the Enviro-HIRLAM (Environment High Resolution Limited Area Model) was adapted and employed for assessment of scenarios with accidental and continuous emissions of sulphur dioxide (SO2) for selected case studies during January of 2010. The following scenarios were considered: (i) control reference run; (ii) accidental release (due to short-term 1 day fire at oil storage facility) occurred at city of Atyrau (Kazakhstan) near the northern part of the Caspian Sea; and (iii) doubling of original continuous emissions from three locations of metallurgical enterprises on the Kola Peninsula (Russia). The implemented aerosol microphysics module M7 uses 5 types - sulphates, sea salt, dust, black and organic carbon; as well as distributed in 7 size modes. Removal processes of aerosols include gravitational settling and wet deposition. As the Enviro-HIRLAM model is the on-line integrated model, both meteorological and chemical processes are simultaneously modelled at each time step. The modelled spatio-temporal variations for meteorological and chemical patterns are analyzed for both European and Kazakhstan regions domains. The results of evaluation of sulphur dioxide concentration and deposition on main populated cities, selected regions, countries are presented employing GIS tools. As outcome, the results of Enviro-HIRLAM modelling for accidental release near the Caspian Sea are integrated into the RANDOM (Risk Assessment of Nature Detriment due to Oil spill Migration) system.

  8. Studies of dynamical processes affecting global climate

    SciTech Connect

    Keller, C.; Cooper, D.; Eichinger, W.

    1998-12-31

    This is the final report of a three-year, Laboratory Directed Research and Development project at the Los Alamos National Laboratory (LANL). The main objective was, by a combined theoretical and observational approach, to develop improved models of dynamic processes in the oceans and atmosphere and to incorporate them into large climate codes, chiefly in four main areas: numerical physics, chemistry, water vapor, and ocean-atmosphere interactions. Main areas of investigation included studies of: cloud parameterizations for global climate codes, Lidar and the planetary boundary layer, chemistry, climate variability using coupled ocean-atmospheric models, and numerical physical methods. This project employed a unique approach that included participation of a number of University of California faculty, postdoctoral fellows and graduate students who collaborated with Los Alamos research staff on specific tasks, thus greatly enhancing the research output. Overall accomplishments during the sensing of the atmospheric planetary were: (1) first two- and three-dimensional remote sensing of the atmospheric planetary boundary layer using Lidars, (2) modeling of 20-year cycle in both pressure and sea surface temperatures in North Pacific, (3) modeling of low frequency internal variability, (4) addition of aerosols to stratosphere to simulate Pinatubo effect on ozone, (5) development of fast, comprehensive chemistry in the troposphere for urban pollution studies, (6) new prognostic cloud parameterization in global atmospheric code remedied problems with North Pacific atmospheric circulation and excessive equatorial precipitation, (7) development of a unique aerosol analysis technique, the aerosol time-of-flight mass spectrometer (ATOFMS), which allows real-time analysis of the size and chemical composition of individual aerosol particles, and (8) numerical physics applying Approximate Inertial Manifolds to ocean circulation. 14 refs., 6 figs.

  9. SOA Formation from Glyoxal in the Aerosol Aqueous Phase: A case study from Mexico City using an explicit laboratory-based model

    NASA Astrophysics Data System (ADS)

    Waxman, E.; Dzepina, K.; Lee-Taylor, J.; Ervens, B.; Volkamer, R.

    2012-04-01

    Glyoxal is an important contributor to secondary organic aerosol (SOA) formation via aerosol aqueous phase processing. This work takes a glyoxal-SOA model parameterization based on laboratory data and applies the box model to ambient measurements. For the Mexico City Metropolitan Area (MCMA) case study on April 9, 2003 the aerosol uptake and processing of glyoxal in aerosol water is investigated, and found able to rationalize the previously observed gas phase glyoxal imbalance (Volkamer et al., 2007) for the first time based on laboratory data. Our aerosol size distribution resolving model is constrained with time resolved distributions of aerosol chemical composition, and supports a surface limited uptake mechanism of glyoxal in Mexico City. We compare the AMS-measured OOA to SOA predictions using our glyoxal model combined with background aerosol, traditional VOC precursor (e.g., aromatics) SOA, and three parameterizations for SOA formation from S/IVOC, i.e., based on (1) Robinson et al., 2007, (2) Grieshop et al., 2009, and (3) GECKO-A (Lee-Taylor et al., 2011), which account for the bulk of SOA mass, but give very different results for the O/C ratio of predicted SOA. This presents to our knowledge the first comparison of a molecular perspective of S/IVOC ageing with empirical parameterizations. We compare the mass weighted O/C ratio from these different SOA sources to AMS-measured O/C ratios, in an attempt to use the rapidly increasing O/C to test for closure, and advance our understanding of aerosol ageing in Mexico City.

  10. Aircraft observations of aerosol composition and ageing in New England and Mid-Atlantic States during the summer 2002 New England Air Quality Study field campaign

    NASA Astrophysics Data System (ADS)

    Kleinman, Lawrence I.; Daum, Peter H.; Lee, Yin-Nan; Senum, Gunnar I.; Springston, Stephen R.; Wang, Jian; Berkowitz, Carl; Hubbe, John; Zaveri, Rahul A.; Brechtel, Fred J.; Jayne, John; Onasch, Timothy B.; Worsnop, Douglas

    2007-05-01

    Aerosol chemical composition, size distribution, and optical properties were measured during 17 aircraft flights in New England and Middle Atlantic States as part of the summer 2002 New England Air Quality Study field campaign. An Aerodyne aerosol mass spectrometer (AMS) was operated with a measurement cycle of 30 s, about an order of magnitude faster than used for ground-based measurements. Noise levels within a single measurement period were sub μg m-3. Volume data derived from the AMS were compared with volume measurements from a Passive Cavity Aerosol Spectrometer (PCASP) optical particle detector and a Twin Scanning Electrical Mobility Spectrometer (TSEMS); calculated light scattering was compared with measured values from an integrating nephelometer. The median ratio for AMS/TSEMS volume was 1.25 (1.33 with an estimated refractory component); the median ratio for AMS/nephelometer scattering was 1.18. A dependence of the AMS collection efficiency on aerosol acidity was quantified by a comparison between AMS and PCASP volumes in two high sulfate plumes. For the entire field campaign, the average aerosol concentration was 11 μg m-3. Compared with monitoring data from the IMPROVE network, the organic component made up a large fraction of total mass, varying from 70% in clean air to 40% in high concentration sulfate plumes. In combination with other optical and chemical measurements, the AMS gave information on secondary organic aerosol (SOA) production and the time evolution of aerosol light absorption. CO is taken as a conservative tracer of urban emissions and the ratios of organic aerosol and aerosol light absorption to CO examined as a function of photochemical age. Comparisons were made to ratios determined from surface measurements under conditions of minimal atmospheric processing. In air masses in which the NOx to NOy ratio has decreased to 10%, the ratio of organic aerosol to CO has quadrupled indicating that 75% of the organic aerosol is secondary

  11. A study of aerosol optical properties during ozone pollution episodes in 2013 over Shanghai, China

    NASA Astrophysics Data System (ADS)

    Shi, Chanzhen; Wang, Shanshan; Liu, Rui; Zhou, Rui; Li, Donghui; Wang, Wenxin; Li, Zhengqiang; Cheng, Tiantao; Zhou, Bin

    2015-02-01

    Aerosol optical property is essential to the tropospheric ozone formation mechanism while it was rarely measured in ozone-rich environment for a specific study. With the retrieved products of the sun-photometer, a comparative investigation was conducted on aerosol optical depth (AOD), single scattering albedo (SSA) and size distribution during ozone-polluted episodes and clean background. Contrary to expectations, aerosol loading was found to be positively-correlated with ozone concentration: daily averaged AOD at 500 nm in ozone episodes (~ 0.78) displayed 2.4 times higher than that in clean days (~ 0.32). Large Ångström exponent (~ 1.51) along with heavy aerosol loading indicated a considerable impact of fine particles on optical extinction. The dynamic diurnal fluctuation of these parameters also implied a complex interaction between aerosols and photo-chemical reactions. The bimodal lognormal distribution pattern for aerosol size spectra exhibited in both ozone-polluted and clean days. The occurrence of maximum volume concentration (~ 0.28) in fine mode (radius < 0.6 μm) was observed at 3 p.m. (local time), when ozone was substantially generated. Pronounced scattering feature of aerosol was reproduced in high-concentration ozone environment. SSA tended to increase continuously from morning (~ 0.91 at 440 nm) to afternoon (~ 0.99), which may be associated with secondary aerosol formation. The scattering aerosol (with moderately high aerosol loading) may favor the ozone formation through increasing solar flux in boundary layer. Utilizing the micro-pulse lidar (MPL), a more developed planet boundary layer (PBL, top height ~ 1.96 km) was discovered during ozone-polluted days than clean condition (~ 1.4 km). In episodes, the maximum extinction ratio (~ 0.5 km- 1) was presented at a height of 1.2 km in the late afternoon. The humidity profile by sounding also showed the extreme value at this altitude. It suggested that optical extinction was mainly attributed to

  12. Study on aerosol optical properties and radiative effect in cloudy weather in the Guangzhou region.

    PubMed

    Deng, Tao; Deng, XueJiao; Li, Fei; Wang, ShiQiang; Wang, Gang

    2016-10-15

    Currently, Guangzhou region was facing the problem of severe air pollution. Large amount of aerosols in the polluted air dramatically attenuated solar radiation. This study investigated the vertical optical properties of aerosols and inverted the height of boundary layer in the Guangzhou region using the lidar. Simultaneously, evaluated the impact of different types of clouds on aerosol radiation effects using the SBDART. The results showed that the height of the boundary layer and the surface visibility changed consistently, the average height of the boundary layer on the hazy days was only 61% of that on clear days. At the height of 2km or lower, the aerosol extinction coefficient profile distribution decreased linearly along with height on clear days, but the haze days saw an exponential decrease. When there was haze, the changing of heating rate of atmosphere caused by the aerosol decreased from 3.72K/d to 0.9K/d below the height of 2km, and the attenuation of net radiation flux at the ground surface was 97.7W/m(2), and the attenuation amplitude was 11.4%; when there were high clouds, the attenuation was 125.2W/m(2) and the attenuation amplitude was 14.6%; where there were medium cloud, the attenuation was 286.4W/m(2) and the attenuation amplitude was 33.4%. Aerosol affected mainly shortwave radiation, and affected long wave radiation very slightly. PMID:27295588

  13. A new Technique for Studying Aerosol-Cloud Interactions in Marine Stratocumulus.

    NASA Astrophysics Data System (ADS)

    Ghate, V. P.; Albrecht, B.; Kollias, P.; Jonsson, H.; Breed, D.

    2006-12-01

    A cloud seeding experiment conducted off-shore of Monterey, California in June 2006 was designed to establish the feasibility of perturbing aerosol concentrations and composition artificially as a method for studying aerosol-cloud interactions in marine stratocumulus. Perturbations in aerosols were made using hygroscopic (Magnesium/Potassium Perchlorate) flares (manufactured by Ice Crystal Engineering (ICE)) burned within a cloud deck. Responses to the resulting aerosol perturbations were observed using in-situ aerosol, cloud, and drizzle probes and a 95 GHz FMCW radar operating from the CIRPAS Twin Otter research aircraft. This method is demonstrated using results from 28 June 2006, when ICE flares were burned creating two seeded lines in a 300 m thick cloud with a mean cloud droplet concentration of 200 cm{-3}. In-cloud plume intersects (total of 16) were made during a 35 min period with the Twin-Otter. Each plume crossing was identified by a strong aerosol concentration increase in the 0.1-3 μm range. During this time, direct observations of the evolution of cloud and drizzle were made in conjunction with background cloud conditions. Results from cloud evolution characterization, the merits of this approach and potential for future applications will be discussed.

  14. Study on aerosol optical properties and radiative effect in cloudy weather in the Guangzhou region.

    PubMed

    Deng, Tao; Deng, XueJiao; Li, Fei; Wang, ShiQiang; Wang, Gang

    2016-10-15

    Currently, Guangzhou region was facing the problem of severe air pollution. Large amount of aerosols in the polluted air dramatically attenuated solar radiation. This study investigated the vertical optical properties of aerosols and inverted the height of boundary layer in the Guangzhou region using the lidar. Simultaneously, evaluated the impact of different types of clouds on aerosol radiation effects using the SBDART. The results showed that the height of the boundary layer and the surface visibility changed consistently, the average height of the boundary layer on the hazy days was only 61% of that on clear days. At the height of 2km or lower, the aerosol extinction coefficient profile distribution decreased linearly along with height on clear days, but the haze days saw an exponential decrease. When there was haze, the changing of heating rate of atmosphere caused by the aerosol decreased from 3.72K/d to 0.9K/d below the height of 2km, and the attenuation of net radiation flux at the ground surface was 97.7W/m(2), and the attenuation amplitude was 11.4%; when there were high clouds, the attenuation was 125.2W/m(2) and the attenuation amplitude was 14.6%; where there were medium cloud, the attenuation was 286.4W/m(2) and the attenuation amplitude was 33.4%. Aerosol affected mainly shortwave radiation, and affected long wave radiation very slightly.

  15. Cloud Regimes as a Tool for Systematic Study of Various Aerosol-Cloud-Precipitation Interactions

    NASA Technical Reports Server (NTRS)

    Oreopoulos, Lazaros; Cho, Nayeong; Lee, Dongmin

    2016-01-01

    Systematic changes of clouds and precipitation are notoriously difficult to ascribe to aerosols. This presentation will showcase yet one more attempt to at least credibly detect the signal of aerosol-cloud-precipitation interactions. We surmise that the concept of cloud regimes (CRs) is appropriate to conduct such an investigation. Previous studies focused on what we call here dynamical CRs, and while we continue to adopt those too for our analysis, we have found that a different way of organizing cloud systems, namely via microphysical regimes is also promising. Our analysis relies on MODIS Collection 6 Level-3 data for clouds and aerosols, and TRMM-TMPA data for precipitation. The regimes are derived by applying clustering analysis on MODIS joint histograms, and once each grid cell is assigned a regime, aerosol and precipitation data can be spatiotemporally matched and composited by regime. The composites of various cloud and precipitation variables for high (upper quartile of distribution) and low (lower quartile) aerosol loadings can then be contrasted. We seek evidence of aerosol effects both in regimes with large fractions of deep ice-rich clouds, as well as regimes where low liquid phase clouds dominate. Signals can be seen, especially when the analysis is broken by land-ocean and when additional filters are applied, but there are of course caveats which will be discussed.

  16. Rapid Measurements of Aerosol Ionic Composition and 3-10 nm Particle Size Distributions On The NASA P3 To Better Quantify Processes Affecting Aerosols Advected From East Asia

    NASA Technical Reports Server (NTRS)

    Weber, Rodney J.

    2004-01-01

    The Particle Into Liquid Sample (PILS) was deployed on the NASA P3 for airborne measurements of fine particle ionic chemical composition. The data have been quality assured and reside in the NASA data archive. We have analyzed our data to characterize the sources and atmospheric processing of fine aerosol particles advected from the region during the experiments. Fine particle water-soluble potassium was found to serve as a useful aerosol tracer for biomass smoke. Ratios of PILS potassium to sulfate are used as a means of estimating the percent contribution of biomass burning to fine particle mass in mixed plumes advecting from Asia. The high correlations between K+ and NO3(sup -) and NH4(sup +)' indicated that biomass burning was a significant source of these aerosol compounds in the region. It is noteworthy that the air mass containing the highest concentrations of fine particles recorded in all of ACE-Asia and TRACE-P appeared to be advecting from the Bejing/Tientsin urban region and also had the highest K(+), NO3(sup -) and NH4(sup +) concentrations of both studies. Based on K+/SO4(sup 2-) ratio's, we estimated that the plume was composed of approx. 60% biomass burning emissions, possibly from the use of bio-fuels in the urban regions.

  17. Nucleation-assisted process for the removal of fine aerosol particles

    SciTech Connect

    ChinCheng Chen; HanKuan Shu; YeunKwei Yang . Dept. of Chemical Engineering)

    1993-07-01

    An efficient (up to 99%) multistage process that removes a wide range of fine particles (several microns down to 0.1 [mu]m) assisted by a nucleation method is proposed. In each stage, as a gas stream passed through a supersaturated vapor in a mixing chamber, water vapor condenses onto the particles which grow to bigger sizes in a subsequent cooling chamber and is removed in a cyclone after being accelerated through a nozzle. The desired efficiency can be assured by employing several stages in series. A single-stage bench-scale model is designed, and four types of test aerosol are used to demonstrate the cleaning efficiency. The efficiency increases with increasing ratio of steam to gas stream, wettability of particles, particle size, and degree of cooling in the cooling chamber, and decreases as particle concentration increases. Suggestions on how to achieve desired efficiencies at less cost are also given.

  18. Investigations of aerosol impacts on MCSs convection and precipitation: a modeling study

    NASA Astrophysics Data System (ADS)

    Clavner, M.; Cotton, W. R.

    2014-12-01

    Mesoscale Convective Systems (MCSs) are important contributors to rainfall in the High Plains of the United States. It is therefore of interest to understand how different vertical distributions and concentrations of aerosols serving as cloud condensation nuclei (CCN) may impact the amount, intensity, and spatial distribution of precipitation produced by MCSs. Unlike ordinary cumulonimbi, MCSs are organized convection systems composed of convective upright updrafts and downdrafts, as well as slowly ascending and descending slantwise motions. These motions can supply moisture to the stratiform-anvil of the MCS without passing through the convective cores. Moreover, the slantwise ascending motions originate some 3-5km above ground level thereby consisting of air with different properties than upright convective updrafts. In order to study the impact of enhanced potential CCN concentrations on MCS precipitation, it is important to understand aerosol microphysical impacts on the dynamics of the different modes of convection within the MCS. In this study, different aerosol concentrations and their effects on the dynamics of the different modes of MCS convection are examined by simulating a case study using the Regional Atmospheric Modeling System (RAMS). Four simulations were conducted, where each simulation differed in the initial aerosol concentrations as well as their vertical distributions. Previous studies have shown that enhanced aerosols invigorate upright convective updrafts, however, the microphysical effects of increased aerosols and their impact on the dynamics of the slow ascending slantwise motion within an MCS, as of yet, have not been studied. In this presentation, the effects of aerosols on the upright convection, slantwise convection and the resulting impacts on precipitation will be discussed.

  19. Global Atmospheric Aerosol Modeling

    NASA Technical Reports Server (NTRS)

    Hendricks, Johannes; Aquila, Valentina; Righi, Mattia

    2012-01-01

    Global aerosol models are used to study the distribution and properties of atmospheric aerosol particles as well as their effects on clouds, atmospheric chemistry, radiation, and climate. The present article provides an overview of the basic concepts of global atmospheric aerosol modeling and shows some examples from a global aerosol simulation. Particular emphasis is placed on the simulation of aerosol particles and their effects within global climate models.

  20. A global aerosol classification algorithm incorporating multiple satellite data sets of aerosol and trace gas abundances

    NASA Astrophysics Data System (ADS)

    Penning de Vries, M. J. M.; Beirle, S.; Hörmann, C.; Kaiser, J. W.; Stammes, P.; Tilstra, L. G.; Tuinder, O. N. E.; Wagner, T.

    2015-09-01

    with GACA. Whereas the presented study is of exploratory nature, we show that the developed algorithm is well suited to evaluate climate and atmospheric composition models by including aerosol type and source obtained from measurements into the comparison, instead of focusing on a single parameter, e.g., AOD. The approach could be adapted to constrain the mix of aerosol types during the process of a combined data assimilation of aerosol and trace gas observations.

  1. Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes During Boreal Spring and Summer

    NASA Technical Reports Server (NTRS)

    Lau, William K. M.; Kim, M. K.; Kim, K. M.; Chin, Mian

    2005-01-01

    Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol

  2. Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes during Boreal Spring and Summer

    NASA Technical Reports Server (NTRS)

    Lau, William K. M.; Kim, M. K.; Chin, Mian; Kim, K. M.

    2005-01-01

    Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and.black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol

  3. CCN activation and efficiency of nucleation and impaction removal process of biomass burning aerosols in Brazil: preliminary results.

    NASA Astrophysics Data System (ADS)

    Sánchez Gácita, Madeleine; Longo, Karla M.; Freitas, Saulo R.; Martin, Scot T.

    2015-04-01

    The biomass burning activity constitutes an important source of aerosols and trace gases to the atmosphere globally. In South America, during the dry season, aerosols prevenient from biomass burning are typically transported to long distances from its sources before being removed though contributing significantly to the aerosol budget on a continental scale. The uncertainties in the magnitude of the impacts on the hydrological cycle, the radiation budget and the biogeochemical cycles on a continental scale are still noteworthy. The still unknowns on the efficiency of biomass burning aerosol to act as cloud condensation nuclei (CCN) and the effectiveness of the nucleation and impaction scavenging mechanisms in removing them from the atmosphere contribute to such uncertainties. In the present work, the explicit modelling of the early stages of cloud development using a parcel model for the typical conditions of the dry season and dry-to-wet transition periods in Amazonia allowed an estimation of the efficiency of nucleation scavenging process and the ability of South American biomass burning aerosol to act as CCN. Additionally, the impaction scavenging was simulated for the same aerosol population following a method based on the widely used concept of the efficiency of collision between a raindrop and an aerosol particle. DMPS and H-TDMA data available in the literature for biomass burning aerosol population in the region indicated the presence of a nearly hydrophobic fraction (on average, with specific hygroscopic parameter κ=0.04, and relative abundance of 73 %) and nearly hygroscopic fraction (κ=0.13, 27 %), externally mixed. The hygroscopic parameters and relative abundances of each hygroscopic group, as well as the weighted average specific hygroscopic parameter for the entire population κ=0.06, were used in calculations of aerosol activation and population mass and number concentration scavenged by nucleation. Results from both groups of simulations are

  4. A sensitivity study of atmospheric reflectance to aerosol layer height based on multi-angular polarimetric measurements

    NASA Astrophysics Data System (ADS)

    Qie, Lili; Li, Donghui; Li, Zhengqiang; Zhang, Ying; Hou, Weizhen; Chen, Xingfeng

    2015-10-01

    The reflected Solar radiance at top of atmosphere (TOA) are, to some degree, sensitive to the vertical distribution of absorbing aerosols, especially at short wavelengths (i.e. blue and UV bands). If properly exploited, it may enable the extraction of basic information on aerosol vertical distribution. In recent years, rapid development of the advanced spectral multi-angle polarimetric satellite observation technology and aerosol inversion algorithm makes the extraction of more aerosol information possible. In this study, we perform a sensitivity analysis of the reflection function at TOA to the aerosol layer height, to explore the potential for aerosol height retrievals by using multi-angle total and polarized reflectance passive observations at short wavelength. Employing a vector doubling-adding method radiative transfer code RT3, a series of numerical experiments were conducted considering different aerosol model, optical depth (AOD), single-scattering albedo (SSA), and scale height (H), also the wavelength, solar-viewing geometry, etc. The sensitivity of both intensity and polarization signals to the aerosol layer height as well as the interacted impactions with SSA and AOD are analyzed. It's found that the sensitivity of the atmospheric reflection function to aerosol scale height increase with aerosol loading (i.e. AOD) and aerosol absorption (i.e. SSA), and decrease with wavelength. The scalar reflectance is sensitive to aerosol absorption while the polarized reflectance is more influenced by the altitude. Then the aerosol H and SSA may be derived simultaneously assuming that the total and polarized radiances in UV bands deconvolve the relative influences of height and absorption. Aerosol layer height, Atmospheric reflection function, Sensitivity, Ultraviolet (UV) band.

  5. Studies of ice nuclei at the Leipzig Aerosol Cloud Interaction Simulator and their implications

    NASA Astrophysics Data System (ADS)

    Wex, Heike

    2013-04-01

    Ice containing clouds permanently cover 40% of the earth's surface. Ice formation processes have a large impact on the formation of precipitation, cloud radiative properties, cloud electrification and hence influence both, weather and climate. Our understanding of the physical and chemical processes underlying ice formation is limited. However what we know is that the two main pathways of atmospheric ice formation are homogeneous and heterogeneous ice nucleation. The latter involves aerosol particles that act as ice nuclei inducing cloud droplet freezing at temperatures significantly above the homogeneous freezing threshold temperature. Particles acting as IN are e.g. dust particles, but also biological particles like bacteria, pollen and fungal spores. Different heterogeneous freezing mechanisms do exit, with their relative importance for atmospheric clouds still being debated. However, there are strong indications that immersion freezing is the most important mechanism when considering mixed phase clouds. What we are still lacking is a) the fundamental process understanding on how aerosol particles induce ice nucleation and b) means to quantify ice nucleation in atmospheric models. Concerning a) there most likely is not only one answer, considering the variety of IN found in the atmosphere. With respect to b) different approaches based on either the stochastic or singular hypotheses have been suggested. However it is still being debated which would be a suitable way to parameterize laboratory data for use in atmospheric modeling. In this presentation, both topics will be addressed. Using the Leipzig Aerosol Cloud Interaction Simulator (LACIS) (Hartmann et al., 2011), we examined different types of dust particles with and without coating, and biological particles such as bacteria and pollen, with respect to their immersion freezing behaviour. We will summarize our findings concerning the properties controlling the ice nucleation behaviour of these particles and

  6. Constraining Predicted Secondary Organic Aerosol Formation and Processing Using Real-Time Observations of Aging Urban Emissions in an Oxidation Flow Reactor

    NASA Astrophysics Data System (ADS)

    Ortega, A. M.; Palm, B. B.; Hayes, P. L.; Day, D. A.; Cubison, M.; Brune, W. H.; Hu, W.; Graus, M.; Warneke, C.; Gilman, J.; De Gouw, J. A.; Jimenez, J. L.

    2014-12-01

    To investigate atmospheric processing of urban emissions, we deployed an oxidation flow reactor with measurements of size-resolved chemical composition of submicron aerosol during CalNex-LA, a field study investigating air quality and climate change at a receptor site in the Los Angeles Basin. The reactor produces OH concentrations up to 4 orders of magnitude higher than in ambient air, achieving equivalent atmospheric aging of hours to ~2 weeks in 5 minutes of processing. The OH exposure (OHexp) was stepped every 20 min to survey the effects of a range of oxidation exposures on gases and aerosols. This approach is a valuable tool for in-situ evaluation of changes in organic aerosol (OA) concentration and composition due to photochemical processing over a range of ambient atmospheric conditions and composition. Combined with collocated gas-phase measurements of volatile organic compounds, this novel approach enables the comparison of measured SOA to predicted SOA formation from a prescribed set of precursors. Results from CalNex-LA show enhancements of OA and inorganic aerosol from gas-phase precursors. The OA mass enhancement from aging was highest at night and correlated with trimethylbenzene, indicating the importance of relatively short-lived VOC (OH lifetime of ~12 hrs or less) as SOA precursors in the LA Basin. Maximum net SOA production is observed between 3-6 days of aging and decreases at higher exposures. Aging in the reactor shows similar behavior to atmospheric processing; the elemental composition of ambient and reactor measurements follow similar slopes when plotted in a Van Krevelen diagram. Additionally, for air processed in the reactor, oxygen-to-carbon ratios (O/C) of aerosol extended over a larger range compared to ambient aerosol observed in the LA Basin. While reactor aging always increases O/C, often beyond maximum observed ambient levels, a transition from net OA production to destruction occurs at intermediate OHexp, suggesting a transition

  7. Chemical composition, sources, and aging process of submicron aerosols in Beijing: Contrast between summer and winter

    NASA Astrophysics Data System (ADS)

    Hu, Weiwei; Hu, Min; Hu, Wei; Jimenez, Jose L.; Yuan, Bin; Chen, Wentai; Wang, Ming; Wu, Yusheng; Chen, Chen; Wang, Zhibin; Peng, Jianfei; Zeng, Limin; Shao, Min

    2016-02-01

    To investigate the seasonal characteristics of submicron aerosol (PM1) in Beijing urban areas, a high-resolution time-of-flight aerosol-mass-spectrometer (HR-ToF-AMS) was utilized at an urban site in summer (August to September 2011) and winter (November to December 2010), coupled with multiple state of the art online instruments. The average mass concentrations of PM1 (60-84 µg m-3) and its chemical compositions in different campaigns of Beijing were relatively consistent in recent years. In summer, the daily variations of PM1 mass concentrations were stable and repeatable. Eighty-two percent of the PM1 mass concentration on average was composed of secondary species, where 62% is secondary inorganic aerosol and 20% secondary organic aerosol (SOA). In winter, PM1 mass concentrations changed dramatically because of the different meteorological conditions. The high average fraction (58%) of primary species in PM1 including primary organic aerosol (POA), black carbon, and chloride indicates primary emissions usually played a more important role in the winter. However, aqueous chemistry resulting in efficient secondary formation during occasional periods with high relative humidity may also contribute substantially to haze in winter. Results of past OA source apportionment studies in Beijing show 45-67% of OA in summer and 22-50% of OA in winter can be composed of SOA. Based on the source apportionment results, we found 45% POA in winter and 61% POA in summer are from nonfossil sources, contributed by cooking OA in both seasons and biomass burning OA (BBOA) in winter. Cooking OA, accounting for 13-24% of OA, is an important nonfossil carbon source in all years of Beijing and should not be neglected. The fossil sources of POA include hydrocarbon-like OA from vehicle emissions in both seasons and coal combustion OA (CCOA) in winter. The CCOA and BBOA were the two main contributors (57% of OA) for the highest OA concentrations (>100 µg m-3) in winter. The POA

  8. Mechanistic study of secondary organic aerosol components formed from nucleophilic addition reactions of methacrylic acid epoxide

    NASA Astrophysics Data System (ADS)

    Birdsall, A. W.; Miner, C. R.; Mael, L. E.; Elrod, M. J.

    2014-08-01

    Recently, methacrylic acid epoxide (MAE) has been proposed as a precursor to an important class of isoprene-derived compounds found in secondary organic aerosol (SOA): 2-methylglyceric acid (2-MG) and a set of oligomers, nitric acid esters and sulfuric acid esters related to 2-MG. However, the specific chemical mechanisms by which MAE could form these compounds have not been previously studied. In order to determine the relevance of these processes to atmospheric aerosol, MAE and 2-MG have been synthesized and a series of bulk solution-phase experiments aimed at studying the reactivity of MAE using nuclear magnetic resonance (NMR) spectroscopy have been performed. The present results indicate that the acid-catalyzed MAE reaction is more than 600 times slower than a similar reaction of an important isoprene-derived epoxide, but is still expected to be kinetically feasible in the atmosphere on more acidic SOA. The specific mechanism by which MAE leads to oligomers was identified, and the reactions of MAE with a number of atmospherically relevant nucleophiles were also investigated. Because the nucleophilic strengths of water, sulfate, alcohols (including 2-MG), and acids (including MAE and 2-MG) in their reactions with MAE were found to be of a similar magnitude, it is expected that a diverse variety of MAE + nucleophile product species may be formed on ambient SOA. Thus, the results indicate that epoxide chain reaction oligomerization will be limited by the presence of high concentrations of non-epoxide nucleophiles (such as water); this finding is consistent with previous environmental chamber investigations of the relative humidity-dependence of 2-MG-derived oligomerization processes and suggests that extensive oligomerization may not be likely on ambient SOA because of other competitive MAE reaction mechanisms.

  9. Mechanistic study of secondary organic aerosol components formed from nucleophilic addition reactions of methacrylic acid epoxide

    NASA Astrophysics Data System (ADS)

    Birdsall, A. W.; Miner, C. R.; Mael, L. E.; Elrod, M. J.

    2014-12-01

    Recently, methacrylic acid epoxide (MAE) has been proposed as a precursor to an important class of isoprene-derived compounds found in secondary organic aerosol (SOA): 2-methylglyceric acid (2-MG) and a set of oligomers, nitric acid esters, and sulfuric acid esters related to 2-MG. However, the specific chemical mechanisms by which MAE could form these compounds have not been previously studied with experimental methods. In order to determine the relevance of these processes to atmospheric aerosol, MAE and 2-MG have been synthesized and a series of bulk solution-phase experiments aimed at studying the reactivity of MAE using nuclear magnetic resonance (NMR) spectroscopy have been performed. The present results indicate that the acid-catalyzed MAE reaction is more than 600 times slower than a similar reaction of an important isoprene-derived epoxide, but is still expected to be kinetically feasible in the atmosphere on more acidic SOA. The specific mechanism by which MAE leads to oligomers was identified, and the reactions of MAE with a number of atmospherically relevant nucleophiles were also investigated. Because the nucleophilic strengths of water, sulfate, alcohols (including 2-MG), and acids (including MAE and 2-MG) in their reactions with MAE were found to be of similar magnitudes, it is expected that a diverse variety of MAE + nucleophile product species may be formed on ambient SOA. Thus, the results indicate that epoxide chain reaction oligomerization will be limited by the presence of high concentrations of non-epoxide nucleophiles (such as water); this finding is consistent with previous environmental chamber investigations of the relative humidity dependence of 2-MG-derived oligomerization processes and suggests that extensive oligomerization may not be likely on ambient SOA because of other competitive MAE reaction mechanisms.

  10. Aerosol characteristics in the UTLS region: A satellite-based study over north India

    NASA Astrophysics Data System (ADS)

    Srivastava, A. K.; Misra, A.; Kanawade, Vijay P.; Devara, P. C. S.

    2016-01-01

    Vertical profiles of aerosol backscatter coefficient and depolarization ratio, obtained from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, were studied in the upper troposphere and lower stratosphere (UTLS) region over North India (21-30° N and 72-90° E), covering the highly polluted Indo-Gangetic Plain (IGP) for one-year period from December 2011 to November 2012. An enhanced aerosol layer was observed between 15 and 18 km altitude, in the vicinity of tropopause, with a broad layer depth of about 2 km. The aerosol layer showed strong seasonal, monthly as well as day and night time variability, with a peak value of backscatter coefficient during monsoon season (˜5.54 × 10-3 sr-1 in September). The corresponding depolarization ratio indicates anisotropic (non-spherical) nature of particles. The aerosol layer was found to be highly linked with the variability in tropopause height, showing a positive correlation between tropopause height and the height of maximum backscatter coefficient (correlation coefficient of 0.8). However, it was found to be negatively correlated with the integrated backscatter coefficient (IBC), with a correlation coefficient of 0.3. We further analyzed outgoing long-wave radiation (OLR) data during the study period to investigate the link between the observed enhanced aerosol layer in the UTLS region and prevailing deep convective activities over the study region. Low values of OLR during monsoon (about 214 W m-2) indicate the occurrence of deep convection over this region, which may cause a large-scale circulation-driven vertical transport of boundary-layer pollution into the atmosphere of UTLS region. Results may have potential implications for better understanding and assessing the chemical and radiative impacts of these aerosols in the tropical UTLS region.

  11. Apportionment of primary and secondary organic aerosols in southern California during the 2005 study of organic aerosols in riverside (SOAR-1).

    PubMed

    Docherty, Kenneth S; Stone, Elizabeth A; Ulbrich, Ingrid M; DeCarlo, Peter F; Snyder, David C; Schauer, James J; Peltier, Richard E; Weber, Rodney J; Murphy, Shane M; Seinfeld, John H; Grover, Brett D; Eatough, Delbert J; Jimenez, Jose L

    2008-10-15

    Ambient sampling was conducted in Riverside, California during the 2005 Study of Organic Aerosols in Riverside to characterize the composition and sources of organic aerosol using a variety of state-of-the-art instrumentation and source apportionmenttechniques. The secondary organic aerosol (SOA) mass is estimated by elemental carbon and carbon monoxide tracer methods, water soluble organic carbon content, chemical mass balance of organic molecular markers, and positive matrix factorization of high-resolution aerosol mass spectrometer data. Estimates obtained from each ofthese methods indicate that the organic fraction in ambient aerosol is overwhelmingly secondary in nature during a period of several weeks with moderate ozone concentrations and that SOA is the single largest component of PM1 aerosol in Riverside. Average SOA/OA contributions of 70-90% were observed during midday periods, whereas minimum SOA contributions of approximately 45% were observed during peak morning traffic periods. These results are contraryto previous estimates of SOAthroughout the Los Angeles Basin which reported that, other than during severe photochemical smog episodes, SOA was lower than primary OA. Possible reasons for these differences are discussed. PMID:18983089

  12. Uptake of Elements From Aerosols by Humans ~ A Case Study From Delhi & Bangalore Cities

    NASA Astrophysics Data System (ADS)

    Anand, S.; Yadav, S.; Jain, V. K.

    2006-05-01

    Aerosol research has gained tremendous importance globally due to the cumulative effects of increasing industrialization and urbanization on aerosol production which can have an alarming impact on the climate of the planet as well as the health of its inhabitants. Therefore, there is an increasing need to study aerosols for all of their physicochemical and biological aspects on both local and global scales. World over extensive research has gone into studying the physical and the chemical aspects of aerosols. However, little information is yet available on the health impacts of aerosols particularly in the Asian context. Here we report uptake of various elements that are concentrated in aerosols by the human body in Delhi and Bangalore cities and their possible health effects. In many urban areas, for example in Delhi, inhalable fractions of aerosols are known to have high concentrations of elements such as Cu, Zn, Pb, Ba, Ni and Cr (Yadav and Rajamani 2004). Also aerosols in the North West part of India seem to be particularly enriched in these elements. If so, there is a high possibility of these elements getting into the human system either directly or indirectly through water and food. To determine the concentrations of these elements that are present in significant concentrations in the inhalable fractions of aerosols, human hair and blood samples are used as proxies. Both these regions have contrasting geographic and climatic conditions. Delhi (altitude : 213-305m above MSL) located on the fringes of the Thar desert which supplies considerable amount of dust, is semi-arid with annual rainfall of 60-80 cms & temperatures varying between 1° - 45°. Bangalore (altitude of 900m above MSL) receives a high annual rainfall of 80-100 cms and being located on the fringes of tropical forests of the Sahyadri Mountains (Western Ghats) receives little crustal contribution to the aerosols. Samples from least polluted mountainous areas of Himalayas (Gangothri) and Sahyadri

  13. Weekly variability of precipitation induced by anthropogenic aerosols: A case study in Korea in summer 2004.

    PubMed

    Bae, Soo Ya; Jeong, Jaein I; Park, Rokjin J; Lim, Kyo-Sun Sunny; Hong, Song-You

    2016-01-15

    We examine the effect of anthropogenic aerosols on the weekly variability of precipitation in Korea in summer 2004 by using Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) models. We conduct two WRF simulations including a baseline simulation with empirically based cloud condensation nuclei (CCN) number concentrations and a sensitivity simulation with our implementation to account for the effect of aerosols on CCN number concentrations. The first simulation underestimates observed precipitation amounts, particularly in northeastern coastal areas of Korea, whereas the latter shows higher precipitation amounts that are in better agreement with the observations. In addition, the sensitivity model with the aerosol effects reproduces the observed weekly variability, particularly for precipitation frequency with a high R at 0.85, showing 20% increase of precipitation events during the weekend than those during weekdays. We find that the aerosol effect results in higher CCN number concentrations during the weekdays and a three-fold increase of the cloud water mixing ratio through enhanced condensation. As a result, the amount of warm rain is generally suppressed because of the low auto-conversion process from cloud water to rain water under high aerosol conditions. The inefficient conversion, however, leads to higher vertical development of clouds in the mid-atmosphere with stronger updrafts in the sensitivity model, which increases by 21% cold-phase hydrometeors including ice, snow, and graupel relative to the baseline model and ultimately results in higher precipitation amounts in summer.

  14. Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

    NASA Technical Reports Server (NTRS)

    Wang, Jian; Collins, Don; Covert, David; Elleman, Robert; Ferrare, Richard A.; Gasparini, Roberto; Jonsson, Haflidi; Ogren, John; Sheridan, Patrick; Tsay, Si-Chee

    2006-01-01

    Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

  15. Photochemistry of Model Organic Aerosol Systems

    NASA Astrophysics Data System (ADS)

    Mang, S. A.; Bateman, A. P.; Dailo, M.; Do, T.; Nizkorodov, S. A.; Pan, X.; Underwood, J. S.; Walser, M. L.

    2007-05-01

    Up to 90 percent of urban aerosol particles have been shown to contain organic molecules. Reactions of these particles with atmospheric oxidants and/or sunlight result in large changes in their composition, toxicity, and ability to act as cloud condensation nuclei. For this reason, chemistry of model organic aerosol particles initiated by oxidation and direct photolysis is of great interest to atmospheric, climate, and health scientists. Most studies in this area have focused on identifying the products of oxidation of the organic aerosols, while the products of direct photolysis of the resulting molecules remaining in the aerosol particle have been left mostly unexplored. We have explored direct photolytic processes occurring in selected organic aerosol systems using infrared cavity ringdown spectroscopy to identify small gas phase products of photolysis, and mass-spectrometric and photometric techniques to study the condensed phase products. The first model system was secondary organic aerosol formed from the oxidation of several monoterpenes by ozone in the presence and absence of NOx, under different humidities. The second system modeled after oxidatively aged primary organic aerosol particles was a thin film of either alkanes or saturated fatty acids oxidized in several different ways, with the oxidation initiated by ozone, chlorine atom, or OH. In every case, the general conclusion was that the photochemical processing of model organic aerosols is significant. Such direct photolysis processes are believed to age organic aerosol particles on time scales that are short compared to the particles' atmospheric lifetimes.

  16. Laboratory studies of nitric acid hydrate and sulfuric acid aerosols: Implications for polar stratospheric cloud formation

    SciTech Connect

    Miller, R.E.

    1995-12-31

    The optical properties of atmospheric aerosols are important in a number of modeling and remote sensing applications. We have devised a new approach for determining the frequency dependent real and imaginary refractive indices directly from the observation of the infrared spectra of the aerosols. We have applied this method to the study of water ice aerosols and comparisons with previous measurements confirm that the method is sound and accurate. The temperature dependence of the refractive index of ice has also been measured over the range 130 K to 210 K, which includes the region of interest for the study of Polar Stratospheric Clouds (PSC`s). The method has also been applied to the study of nitric acid dehydrate (NAD) and nitric acid trihydrate (NAT). Sulfuric acid/nitric acid/water ternary systems are also being studied with the aim of determining the nature of the phases formed and the associated freezing points as a function of the concentrations of the acids.

  17. Ultraviolet Studies of Jupiter's Hydrocarbons and Aerosols from Galileo

    NASA Technical Reports Server (NTRS)

    Gladstone, G. Randall

    2001-01-01

    This is the final report for this project. The purpose of this project was to support PI Wayne Pryor's effort to reduce and analyze Galileo UVS (Ultraviolet Spectrometer) data under the JSDAP program. The spectral observations made by the Galileo UVS were to be analyzed to determine mixing ratios for important hydrocarbon species (and aerosols) in Jupiter's stratosphere as a function of location on Jupiter. Much of this work is still ongoing. To date, we have concentrated on analyzing the variability of the auroral emissions rather than the absorption signatures of hydrocarbons, although we have done some work in this area with related HST-STIS data.

  18. Aerosol characterization study using multi-spectrum remote sensing measurement techniques.

    SciTech Connect

    Glen, Crystal Chanea; Sanchez, Andres L.; Lucero, Gabriel Anthony; Schmitt, Randal L.; Johnson, Mark S.; Tezak, Matthew S; Servantes, Brandon Lee

    2013-09-01

    A unique aerosol flow chamber coupled with a bistatic LIDAR system was implemented to measure the optical scattering cross sections and depolarization ratio of common atmospheric particulates. Each of seven particle types (ammonium sulfate, ammonium nitrate, sodium chloride, potassium chloride, black carbon and Arizona road dust) was aged by three anthropogenically relevant mechanisms: 1. Sulfuric acid deposition, 2. Toluene ozonolysis reactions, and 3. m-Xylene ozonolysis reactions. The results of pure particle scattering properties were compared with their aged equivalents. Results show that as most particles age under industrial plume conditions, their scattering cross sections are similar to pure black carbon, which has significant impacts to our understanding of aerosol impacts on climate. In addition, evidence emerges that suggest chloride-containing aerosols are chemically altered during the organic aging process. Here we present the direct measured scattering cross section and depolarization ratios for pure and aged atmospheric particulates.

  19. Characteristics of solid aerosols produced by optical catapulting studied by laser-induced breakdown spectroscopy

    NASA Astrophysics Data System (ADS)

    Fortes, F. J.; Laserna, J. J.

    2010-08-01

    Optical catapulting (OC) constitutes an effective method to transport small amounts of different materials in the form of a solid aerosol. In this report, laser-induced breakdown spectroscopy (LIBS) is used for the analysis of those aerosols produced by OC. For this purpose, materials were catapulted using a Q-switch Nd:YAG laser. A second Q-switch Nd:YAG laser was used for LIBS analysis of the ejected particles. Data processing of aerosols was conducted using conditional data analysis. Also, the standard deviation method was used for the qualitative identification of the ejected particles. Two modes of interaction in OC (OC with focused or defocused pulses) have been evaluated and discussed. LIBS demonstrates that the distribution (spreading) of the ejected particles along the propagation axis increased as a function of the interpulse delay time. The mass density and the thickness of the target also play an important role in OC-LIBS.

  20. Time- and size-resolved chemical composition of submicron particles in Pittsburgh: Implications for aerosol sources and processes

    NASA Astrophysics Data System (ADS)

    Zhang, Qi; Canagaratna, Manjula R.; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis

    2005-04-01

    An Aerodyne aerosol mass spectrometer (AMS) was deployed at the Pittsburgh Environmental Protection Agency Supersite from 7 to 22 September 2002 as part of the Pittsburgh Air Quality Study (PAQS). The main objectives of this deployment were to characterize the concentrations, size distributions, and temporal variations of nonrefractory (NR) chemical species in submicron particles (approximately PM1) and to further develop and evaluate the AMS. Reasonably good agreement was observed on particle concentrations, composition, and size distributions between the AMS data and measurements from collocated instruments (given the difference between the PM1 and PM2.5 size cuts), including TEOM, semicontinuous sulfate, 2-hour- and 24-hour-averaged organic carbon, SMPS, 4-hour-averaged ammonium, and micro-orifice uniform deposit impactor. Total NR-PM1 mass concentration in Pittsburgh accumulates over periods of several days punctuated with rapid cleaning due to rain or air mass changes. Sulfate and organics are the major NR-PM1 components while the concentrations of nitrate and chloride are generally low. Significant amounts of ammonium, which most of the time are consistent with sulfate present as ammonium sulfate, are also present in particles. However, there are periods when the aerosols are relatively acidic and more than 50% of sulfate is estimated to be in the form of ammonium bisulfate. No major enhancement of the organic concentration is observed during these acidic periods, which suggests that acid-catalyzed SOA formation was not an important process during this study. Size distributions of particulate sulfate, ammonium, organics, and nitrate vary on timescales of hours to days, showing unimodal, bimodal and even trimodal characteristics. The accumulation mode (peaking around 350-600 nm in vacuum aerodynamic diameter for the mass distributions) and the ultrafine mode (<100 nm) are observed most frequently. The accumulation mode is dominated by sulfate that appears to

  1. Stable carbon isotopic compositions of low-molecular-weight dicarboxylic acids, oxocarboxylic acids, α-dicarbonyls, and fatty acids: implications for atmospheric processing of organic aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, Y.; Kawamura, K.; Cao, F.; Lee, M.

    2015-12-01

    Stable carbon isotopic compositions (δ13C) were measured for 23 individual organic species including 9 dicarboxylic acids, 7 oxocarboxylic acids, 1 tricarboxylic acid, 2 α-dicarbonyls and 4 fatty acids in the aerosols from Gosan background site in East Asia. δ13C of particle-phase glyoxal and methylglyoxal are significantly higher than those previously reported for isoprene and other precursors, associated with isotope fractionation during atmospheric oxidation. 13C is consistently more enriched for oxalic acid (C2), glyoxylic acid, pyruvic acid, glyoxal and methylglyoxal compared to other organic compounds identified, which can be explained by the kinetic isotope effects during aqueous-phase processing and the subsequent gas-particle partitioning after clouds or wet aerosols evaporation δ13C of C2 is positively correlated with C2 and organic carbon ratio, indicating that a photochemical production of C2 is more pronounced than its degradation process during long-range transport. The 13C results also suggest that aqueous-phase oxidation of glyoxal and methylglyoxal is major formation process of oxalic acid production via the major intermediates glyoxylic acid and pyruvic acid. This study provides evidence that organic aerosols are intensively photo-chemically aged in this region.

  2. Light Scattering by Aerosols Over the Remote Ocean: Clear-Sky Point and Column Radiative Closure Studies

    NASA Astrophysics Data System (ADS)

    Fridlind, A. M.; Jacobson, M. Z.

    2001-12-01

    Field data gathered by ship and aircraft during leg 2 of the First Aerosol Characterization Experiment (ACE 1) were used to study clear-sky radiative closure over the remote Southern Ocean. Closure was evaluated by comparing observations with modeled values of: (i) aerosol light scattering coefficients in the marine boundary layer and free troposphere, (ii) total aerosol optical depth, and (iii) total solar radiation at the ocean surface. Point modeling using the ship data benefited from an existing study of closure on the ship, expanding the number of data points considered in that study from 22 to 887. Point and column modeling using the aircraft data provide the first such studies to date. Aerosol light scattering coefficients were calculated from size-distributed measurements of aerosol chemical composition and number concentration, and were compared with observations at three wavelengths (450, 550, and 700 nm) on both ship and aircraft. Point closure on the ship could be achieved at all wavelengths for both total and hemispheric backscattering coefficients if the model accounted for experimental uncertainties in aerosol chemistry, nephelometer nonidealities, and the likely nonsphericity of dried sea salt aerosols. Point closure on the aircraft could be achieved at most wavelengths for total scattering coefficients, but could not be achieved at any wavelengths for hemispheric backscattering coefficients. Deviations between predicted and observed backscattering coefficients on the aircraft were widely scattered rather than biased, indicating that a low signal to noise ratio in observed backscattering coefficients was the likely cause for lack of closure. Aerosol optical depth and solar radiation at the ocean surface were calculated for the two days with clear-sky periods when the aircraft measured aerosol profiles near the ship. Input gas and meteorological data were the observed profiles of ozone, water vapor, temperature, and pressure from the surface to

  3. Aerosol properties from 4STAR observations: A sensitivity study

    NASA Astrophysics Data System (ADS)

    Kassianov, E.; Flynn, C.; Redemann, J.; Livingston, J. M.; Schmid, B.; Russell, P. B.; Sinyuk, A.

    2011-12-01

    Multi-spectral direct-beam observations of atmospheric aerosol and gas constituents have been taken successfully at a number of sites around the world by the airborne 14-Channel NASA Ames Airborne Tracking Sunphotometer (AATS-14). The recently developed airborne Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) is the next generation of AATS-14 with ultraviolet, visible and near-infrared spectral coverage, increased number of channels (more than 1500 pixels) and the sky-scanning ability of the ground-based AERONET sun/sky photometers. While it is generally agreed that more measurements in terms of independent wavelengths and scattering angles would offer enhanced aerosol retrievals, the potential afforded by improved observational capabilities of the 4STAR has not yet been fully characterized. This paper will attempt to place the importance of improved spectrally- and angularly-