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Sample records for aerosol inorganics model

  1. AEROSOL INORGANICS AND ORGANICS MODEL (AIOM) WITH USER DEFINED PROPERTIES FOR ORGANIC COMPOUNDS

    EPA Science Inventory

    The Aerosol Inorganics Model (AIM) is widely used to calculate gas/liquid/solid phase equilibrium in aerosol systems containing the species H+-NH4+-SO42--NO3--H2O over a range of tropospheric ...

  2. Thermodynamic Modeling of Organic-Inorganic Aerosols with the Group-Contribution Model AIOMFAC

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Luo, B. P.; Peter, T.

    2009-04-01

    Liquid aerosol particles are - from a physicochemical viewpoint - mixtures of inorganic salts, acids, water and a large variety of organic compounds (Rogge et al., 1993; Zhang et al., 2007). Molecular interactions between these aerosol components lead to deviations from ideal thermodynamic behavior. Strong non-ideality between organics and dissolved ions may influence the aerosol phases at equilibrium by means of liquid-liquid phase separations into a mainly polar (aqueous) and a less polar (organic) phase. A number of activity models exists to successfully describe the thermodynamic equilibrium of aqueous electrolyte solutions. However, the large number of different, often multi-functional, organic compounds in mixed organic-inorganic particles is a challenging problem for the development of thermodynamic models. The group-contribution concept as introduced in the UNIFAC model by Fredenslund et al. (1975), is a practical method to handle this difficulty and to add a certain predictability for unknown organic substances. We present the group-contribution model AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients), which explicitly accounts for molecular interactions between solution constituents, both organic and inorganic, to calculate activities, chemical potentials and the total Gibbs energy of mixed systems (Zuend et al., 2008). This model enables the computation of vapor-liquid (VLE), liquid-liquid (LLE) and solid-liquid (SLE) equilibria within one framework. Focusing on atmospheric applications we considered eight different cations, five anions and a wide range of alcohols/polyols as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are very well represented up to high ionic strength. We show that the semi-empirical middle-range parametrization of direct organic-inorganic interactions in alcohol-water-salt solutions enables accurate computations of vapor-liquid and liquid

  3. Modeling the Thermodynamics of Mixed Organic-Inorganic Aerosols to Predict Water Activities and Phase Equilibria

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Luo, B.; Peter, T.

    2008-12-01

    Tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behavior. While the thermodynamics of aqueous inorganic systems at atmospheric temperatures are well established, little is known about the physicochemistry of mixed organic-inorganic particles. Salting-out and salting-in effects result from organic-inorganic interactions and are used to improve industrial separation processes. In the atmosphere, they may influence the aerosol phases. Liquid-liquid phase separations into a mainly polar (aqueous) and a less polar organic phase may considerably influence the gas/particle partitioning of semi-volatile substances compared to a single phase estimation. Moreover, the phases present in the aerosol define the reaction medium for heterogeneous and multiphase chemistry occurring in aerosol particles. A correct description of these phases is needed when gas- or cloud-phase reaction schemes are adapted to aerosols. Non-ideal thermodynamic behavior in mixtures is usually described by an expression for the excess Gibbs energy. We present the group-contribution model AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients), which explicitly accounts for molecular interactions between solution constituents, both organic and inorganic, to calculate activities, chemical potentials and the total Gibbs energy of mixed systems. This model allows to compute vapor-liquid (VLE), liquid-liquid (LLE) and solid-liquid (SLE) equilibria within one framework. Focusing on atmospheric applications we considered eight different cations, five anions and a wide range of alcohols/polyols as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are very well represented up to high ionic strength. We show that the semiempirical middle

  4. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Luo, B. P.; Peter, T.

    2008-08-01

    Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) that is able to calculate activity coefficients covering inorganic, organic, and organic-inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999) that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH+4, Mg2+, Ca2+, Cl-, Br-, NO-3, HSO-4, and SO2-4 as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic-inorganic interactions in alcohol+water+salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid-liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also applicable for other research topics.

  5. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Luo, B. P.; Peter, Th.

    2008-03-01

    Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) that is able to calculate activity coefficients covering inorganic, organic, and organic-inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999) that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH4+, Mg2+, Ca2+, Cl-, Br-, NO3-, HSO4-, and SO42- as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic-inorganic interactions in alcohol + water + salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid-liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also applicable for other research topics.

  6. An SOA model for toluene oxidation in the presence of inorganic aerosols.

    PubMed

    Cao, Gang; Jang, Myoseon

    2010-01-15

    A predictive model for secondary organic aerosol (SOA) formation including both partitioning and heterogeneous reactions is explored for the SOA produced from the oxidation of toluene in the presence of inorganic seed aerosols. The predictive SOA model comprises the explicit gas-phase chemistry of toluene, gas-particle partitioning, and heterogeneous chemistry. The resulting products from the explicit gas phase chemistry are lumped into several classes of chemical species based on their vapor pressure and reactivity for heterogeneous reactions. Both the gas-particle partitioning coefficient and the heterogeneous reaction rate constant of each lumped gas-phase product are theoretically determined using group contribution and molecular structure-reactivity. In the SOA model, the predictive SOA mass is decoupled into partitioning (OM(P)) and heterogeneous aerosol production (OM(H)). OM(P) is estimated from the SOA partitioning model developed by Schell et al. (J. Geophys. Res. 2001, 106, 28275-28293 ) that has been used in a regional air quality model (CMAQ 4.7). OM(H) is predicted from the heterogeneous SOA model developed by Jang et al. (Environ. Sci. Technol. 2006, 40, 3013-3022 ). The SOA model is evaluated using a number of the experimental SOA data that are generated in a 2 m(3) indoor Teflon film chamber under various experimental conditions (e.g., humidity, inorganic seed compositions, NO(x) concentrations). The SOA model reasonably predicts not only the gas-phase chemistry, such as the ozone formation, the conversion of NO to NO(2), and the toluene decay, but also the SOA production. The model predicted that the OM(H) fraction of the total toluene SOA mass increases as NO(x) concentrations decrease: 0.73-0.83 at low NO(x) levels and 0.17-0.47 at middle and high NO(x) levels for SOA experiments with high initial toluene concentrations. Our study also finds a significant increase in the OM(H) mass fraction in the SOA generated with low initial toluene

  7. Modeling analysis of secondary inorganic aerosols over China: pollution characteristics, and meteorological and dust impacts.

    PubMed

    Fu, Xiao; Wang, Shuxiao; Chang, Xing; Cai, Siyi; Xing, Jia; Hao, Jiming

    2016-10-26

    Secondary inorganic aerosols (SIA) are the predominant components of fine particulate matter (PM2.5) and have significant impacts on air quality, human health, and climate change. In this study, the Community Multiscale Air Quality modeling system (CMAQ) was modified to incorporate SO2 heterogeneous reactions on the surface of dust particles. The revised model was then used to simulate the spatiotemporal characteristics of SIA over China and analyze the impacts of meteorological factors and dust on SIA formation. Including the effects of dust improved model performance for the simulation of SIA concentrations, particularly for sulfate. The simulated annual SIA concentration in China was approximately 10.1 μg/m(3) on domain average, with strong seasonal variation: highest in winter and lowest in summer. High SIA concentrations were concentrated in developed regions with high precursor emissions, such as the North China Plain, Yangtze River Delta, Sichuan Basin, and Pearl River Delta. Strong correlations between meteorological factors and SIA pollution levels suggested that heterogeneous reactions under high humidity played an important role on SIA formation, particularly during severe haze pollution periods. Acting as surfaces for heterogeneous reactions, dust particles significantly affected sulfate formation, suggesting the importance of reducing dust emissions for controlling SIA and PM2.5 pollution.

  8. Modeling analysis of secondary inorganic aerosols over China: pollution characteristics, and meteorological and dust impacts

    NASA Astrophysics Data System (ADS)

    Fu, Xiao; Wang, Shuxiao; Chang, Xing; Cai, Siyi; Xing, Jia; Hao, Jiming

    2016-10-01

    Secondary inorganic aerosols (SIA) are the predominant components of fine particulate matter (PM2.5) and have significant impacts on air quality, human health, and climate change. In this study, the Community Multiscale Air Quality modeling system (CMAQ) was modified to incorporate SO2 heterogeneous reactions on the surface of dust particles. The revised model was then used to simulate the spatiotemporal characteristics of SIA over China and analyze the impacts of meteorological factors and dust on SIA formation. Including the effects of dust improved model performance for the simulation of SIA concentrations, particularly for sulfate. The simulated annual SIA concentration in China was approximately 10.1 μg/m3 on domain average, with strong seasonal variation: highest in winter and lowest in summer. High SIA concentrations were concentrated in developed regions with high precursor emissions, such as the North China Plain, Yangtze River Delta, Sichuan Basin, and Pearl River Delta. Strong correlations between meteorological factors and SIA pollution levels suggested that heterogeneous reactions under high humidity played an important role on SIA formation, particularly during severe haze pollution periods. Acting as surfaces for heterogeneous reactions, dust particles significantly affected sulfate formation, suggesting the importance of reducing dust emissions for controlling SIA and PM2.5 pollution.

  9. Modeling analysis of secondary inorganic aerosols over China: pollution characteristics, and meteorological and dust impacts

    PubMed Central

    Fu, Xiao; Wang, Shuxiao; Chang, Xing; Cai, Siyi; Xing, Jia; Hao, Jiming

    2016-01-01

    Secondary inorganic aerosols (SIA) are the predominant components of fine particulate matter (PM2.5) and have significant impacts on air quality, human health, and climate change. In this study, the Community Multiscale Air Quality modeling system (CMAQ) was modified to incorporate SO2 heterogeneous reactions on the surface of dust particles. The revised model was then used to simulate the spatiotemporal characteristics of SIA over China and analyze the impacts of meteorological factors and dust on SIA formation. Including the effects of dust improved model performance for the simulation of SIA concentrations, particularly for sulfate. The simulated annual SIA concentration in China was approximately 10.1 μg/m3 on domain average, with strong seasonal variation: highest in winter and lowest in summer. High SIA concentrations were concentrated in developed regions with high precursor emissions, such as the North China Plain, Yangtze River Delta, Sichuan Basin, and Pearl River Delta. Strong correlations between meteorological factors and SIA pollution levels suggested that heterogeneous reactions under high humidity played an important role on SIA formation, particularly during severe haze pollution periods. Acting as surfaces for heterogeneous reactions, dust particles significantly affected sulfate formation, suggesting the importance of reducing dust emissions for controlling SIA and PM2.5 pollution. PMID:27782166

  10. Speciation of the major inorganic salts in atmospheric aerosols of Beijing, China: Measurements and comparison with model

    NASA Astrophysics Data System (ADS)

    Tang, Xiong; Zhang, Xiaoshan; Ci, Zhijia; Guo, Jia; Wang, Jiaqi

    2016-05-01

    In the winter and summer of 2013-2014, we used a sampling system, which consists of annular denuder, back-up filter and thermal desorption set-up, to measure the speciation of major inorganic salts in aerosols and the associated trace gases in Beijing. This sampling system can separate volatile ammonium salts (NH4NO3 and NH4Cl) from non-volatile ammonium salts ((NH4)2SO4), as well as the non-volatile nitrate and chloride. The measurement data was used as input of a thermodynamic equilibrium model (ISORROPIA II) to investigate the gas-aerosol equilibrium characteristics. Results show that (NH4)2SO4, NH4NO3 and NH4Cl were the major inorganic salts in aerosols and mainly existed in the fine particles. The sulfate, nitrate and chloride associated with crustal ions were also important in Beijing where mineral dust concentrations were high. About 19% of sulfate in winter and 11% of sulfate in summer were associated with crustal ions and originated from heterogeneous reactions or direct emissions. The non-volatile nitrate contributed about 33% and 15% of nitrate in winter and summer, respectively. Theoretical thermodynamic equilibrium calculations for NH4NO3 and NH4Cl suggest that the gaseous precursors were sufficient to form stable volatile ammonium salts in winter, whereas the internal mixing with sulfate and crustal species were important for the formation of volatile ammonium salts in summer. The results of the thermodynamic equilibrium model reasonably agreed with the measurements of aerosols and gases, but large discrepancy existed in predicting the speciation of inorganic ammonium salts. This indicates that the assumption on crustal species in the model was important for obtaining better understanding on gas-aerosol partitioning and improving the model prediction.

  11. Evaluating secondary inorganic aerosols in three dimensions

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

    The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the three-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e., sulfate, ammonium, and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000 to 2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model. Heterogeneous reactions on dust surfaces are an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3 / NH4+ partitioning which affects the HNO3 / NO3- partitioning.

  12. Evaluating Secondary Inorganic Aerosols in Three Dimensions

    NASA Technical Reports Server (NTRS)

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

    2016-01-01

    The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the three-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e., sulfate, ammonium, and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000 to 2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model. Heterogeneous reactions on dust surfaces are an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3/NH4(+) partitioning which affects the HNO3/NO3(-) partitioning.

  13. Water absorption by secondary organic aerosol and its effect on inorganic aerosol behavior

    SciTech Connect

    Ansari, A.S.; Pandis, S.N.

    2000-01-01

    The hygroscopic nature of atmospheric aerosol has generally been associated with its inorganic fraction. In this study, a group contribution method is used to predict the water absorption of secondary organic aerosol (SOA). Compared against growth measurements of mixed inorganic-organic particles, this method appears to provide a first-order approximation in predicting SOA water absorption. The growth of common SOA species is predicted to be significantly less than common atmospheric inorganic salts such as (NH{sub 4}){sub 2}SO{sub 4} and NaCl. Using this group contribution method as a tool in predicting SOA water absorption, an integrated modeling approach is developed combining available SOA and inorganic aerosol models to predict overall aerosol behavior. The effect of SOA on water absorption and nitrate partitioning between the gas and aerosol phases is determined. On average, it appears that SOA accounts for approximately 7% of total aerosol water and increases aerosol nitrate concentrations by approximately 10%. At high relative humidity and low SOA mass fractions, the role of SOA in nitrate partitioning and its contribution to total aerosol water is negligible. However, the water absorption of SOA appears to be less sensitive to changes in relative humidity than that of inorganic species, and thus at low relative humidity and high SOA mass fraction concentrations, SOA is predicted to account for approximately 20% of total aerosol water and a 50% increase in aerosol nitrate concentrations. These findings could improve the results of modeling studies where aerosol nitrate has often been underpredicted.

  14. 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

  15. Assessing sensitivity regimes of secondary inorganic aerosol formation in Europe with the CALIOPE-EU modeling system

    NASA Astrophysics Data System (ADS)

    Pay, María T.; Jiménez-Guerrero, Pedro; Baldasano, José M.

    2012-05-01

    Sulfur dioxide and nitrogen oxides form two of largest contributors to PM2.5 in Europe; ammonium sulfate ((NH4)2SO4) and ammonium nitrate (NH4NO3). In-situ observations of many chemical components are rather sparse, and thus neither can accurately characterize the distribution of pollutants nor predict the effectiveness of emission control. Understanding (and controlling) the formation regimes for these components is important for the achievement of the reduction objectives established in the European legislation for PM2.5 (20% of PM2.5 triennial for the mean of urban background levels between 2018 and 2020). For this purpose, the present work uses the CALIOPE high-resolution air quality modeling system (12 km × 12 km, 1 h) to investigate the formation of SIA (SO42-, NO3- and NH4+, which involve an important part of PM) and their gaseous precursors (SO2, HNO3 and NH3) over Europe during the year 2004. The CALIOPE system performs well at estimating SIAs when compared to the measurements from EMEP monitoring network, but errors are larger for gaseous precursors. NH3 is underestimated in the warmest months, HNO3 tends to be overestimated in the summer months, and SO2 appears to be systematically overestimated. The temporal treatment of ammonia emission is a probable source of uncertainty in the model representation of SIA. Furthermore, we discuss the annual pattern for each inorganic aerosol and gas precursor species over Europe estimated with the EMEP data and CALIOPE outputs, comparing the performance with other European studies. Spatial distribution of key indicators is used to characterize chemical regimes and understand the sensitivity of SIA components to their emission precursors. Results indicate that SO42- is not usually fully neutralized to ammonium sulfate in ambient measurements and is usually fully neutralized in model estimates. CALIOPE and EMEP observations agree that the continental regions in Europe tend to be HNO3-limited for nitrate formation

  16. Secondary Inorganic Soluble Aerosol in Hong Kong: Continuous Measurements, Formation Mechanism Discussion and Improvement of an Observation-Based Model to Study Control Strategies

    NASA Astrophysics Data System (ADS)

    Xue, Jian

    Work in this thesis focuses on half-hourly or hourly measurements of PM2.5 secondary inorganic aerosols (SIA) in two locations in Hong Kong (HK) using a continuous system, PILS (Particle-into-Liquid System) coupled to two ion chromatographs. The high-resolution data sets allow the examination of SIA temporal dynamics in the scale of hours that the filter-based approach is incapable of providing. (1) Impacts of local emissions, regional transports and their interactions on chemical composition and concentrations of PM2.5 SIA and other ionic species were investigated at the Hong Kong University of Science and Technology (HKUST), a receptor site, under three synoptic conditions. (2) Chemical compositions and size characteristics of ionic species were investigated at Tung Chung, a new town area located in the Southwest part of HK. The sampling period was from 17 to 26 December 2009, covering both normal conditions and an aerosol episode. The three major secondary inorganic ions, SO42, NH4+ and NO 3-, accounted for 47 +/- 6% of PM2.5 mass. Further examination of size characteristics of NO3 - shows that fine mode NO3- is more likely to occur in environments when the fine particles are less acidic and the sea-salt aerosol contributions are low. (3) The ionic chemical composition of PM2.5 and meteorological parameters (e.g., temperature, RH) obtained at the HKUST site under all three different synoptic conditions are input into Aerosol Inorganic Model (AIM-III) for estimation of in situ pH through calculation of H+ amount and aerosol liquid water content (LWC). The second part of this thesis work is to improve an observation-based model (OBAMAP) for SIA, which was first developed by Dr. Zibing Yuan (2006) to evaluate the sensitivity of formation of nitrate ad sulfate to changes in the emissions of their precursors (i.e., NOx, SO2, and VOCs). The improvement work includes incorporating updated chemical mechanisms, thermodynamic equilibrium for gas-aerosol phase

  17. 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

  18. 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.; ...

    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

  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. Mechanism for production of secondary organic aerosols and their representation in atmospheric models. Final report

    SciTech Connect

    Seinfeld, J.H.; Flagan, R.C.

    1999-06-07

    This document contains the following: organic aerosol formation from the oxidation of biogenic hydrocarbons; gas/particle partitioning of semivolatile organic compounds to model inorganic, organic, and ambient smog aerosols; and representation of secondary organic aerosol formation in atmospheric models.

  1. Effects of mineral dust on the semivolatile inorganic aerosol components in a polluted Megacity

    NASA Astrophysics Data System (ADS)

    Karydis, V. A.; Tsimpidi, A. P.; Fountoukis, C.; Nenes, A.; Zavala, M.; Lei, W.; Molina, L. T.; Pandis, S. N.

    2009-04-01

    Aerosols play a significant role in the atmosphere having adverse impacts on human health and directly affecting air quality, visibility and climate change. One of the most challenging tasks for models is the prediction of the partitioning of the semivolatile inorganic aerosol components (ammonia, nitric acid, hydrochloric acid, etc) between the gas and particulate phases. Moreover, the effects of mineral aerosols in the atmosphere remain largely uncertain. As a result, most current models have serious difficulties in reproducing the observed particulate nitrate and chloride concentrations. The improved aerosol thermodynamic model ISORROPIA II (Fountoukis and Nenes, 2007) simulating explicitly the chemistry of Ca, Mg, and K salts has been linked to the regional chemical transport model PMCAMx (Gaydos et al., 2007). PMCAMx also includes the CMU inorganic aerosol growth module (Gaydos et al., 2003; Koo et al., 2003a) and the VSRM aqueous-phase chemistry module (Fahey and Pandis, 2001). The hybrid approach (Koo et al., 2003b) for modeling aerosol dynamics is applied in order to accurately simulate the inorganic components in the coarse mode. This approach assumes that the smallest particles are in equilibrium, while the condensation/evaporation equation is solved for the larger ones. PMCAMx is applied to the Mexico City Metropolitan Area (MCMA). The emission inventory has been improved and now includes more accurate dust and NaCl emissions. The April 2003 (MCMA Campaign) and the March 2006 (MILAGRO campaign) datasets are used to evaluate the inorganic aerosol module of PMCAMx in order to test our understanding of inorganic aerosol. The results from the new modeling framework are also compared with the results from the previous version of PMCAMx in order to investigate the influence of each of the added features to the formation of the semivolatile inorganic components. References Fountoukis, C. and Nenes, A., (2007). ISORROPIA II: a computationally efficient

  2. Size-resolved simulations of the aerosol inorganic composition with the new hybrid dissolution solver HyDiS-1.0: description, evaluation and first global modelling results

    NASA Astrophysics Data System (ADS)

    Benduhn, François; Mann, Graham W.; Pringle, Kirsty J.; Topping, David O.; McFiggans, Gordon; Carslaw, Kenneth S.

    2016-11-01

    The dissolution of semi-volatile inorganic gases such as ammonia and nitric acid into the aerosol aqueous phase has an important influence on the composition, hygroscopic properties, and size distribution of atmospheric aerosol particles. The representation of dissolution in global models is challenging due to inherent issues of numerical stability and computational expense. For this reason, simplified approaches are often taken, with many models treating dissolution as an equilibrium process. In this paper we describe the new dissolution solver HyDiS-1.0, which was developed for the global size-resolved simulation of aerosol inorganic composition. The solver applies a hybrid approach, which allows for some particle size classes to establish instantaneous gas-particle equilibrium, whereas others are treated time dependently (or dynamically). Numerical accuracy at a competitive computational expense is achieved by using several tailored numerical formalisms and decision criteria, such as for the time- and size-dependent choice between the equilibrium and dynamic approaches. The new hybrid solver is shown to have numerical stability across a wide range of numerical stiffness conditions encountered within the atmosphere. For ammonia and nitric acid, HyDiS-1.0 is found to be in excellent agreement with a fully dynamic benchmark solver. In the presence of sea salt aerosol, a somewhat larger bias is found under highly polluted conditions if hydrochloric acid is represented as a third semi-volatile species. We present first results of the solver's implementation into a global aerosol microphysics and chemistry transport model. We find that (1) the new solver predicts surface concentrations of nitrate and ammonium in reasonable agreement with observations over Europe, the USA, and East Asia, (2) models that assume gas-particle equilibrium will not capture the partitioning of nitric acid and ammonia into Aitken-mode-sized particles, and thus may be missing an important

  3. PREDICTION OF MULTICOMPONENT INORGANIC ATMOSPHERIC AEROSOL BEHAVIOR. (R824793)

    EPA Science Inventory

    Many existing models calculate the composition of the atmospheric aerosol system by solving a set of algebraic equations based on reversible reactions derived from thermodynamic equilibrium. Some models rely on an a priori knowledge of the presence of components in certain relati...

  4. Influence of particle phase state on the hygroscopic behavior of mixed organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Mui, W.; Flagan, R. C.; Seinfeld, J. H.

    2014-12-01

    Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particle phase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids, to phase-separated particles, to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40-90%. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids, (2) forcing a single phase, but accounting for non-ideal interactions through activity coefficient calculations, and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation between the inorganic and organic components is assumed at all RH values, with water-uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquid-liquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrose-containing particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF

  5. Influence of particle-phase state on the hygroscopic behavior of mixed organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Mui, W.; Flagan, R. C.; Seinfeld, J. H.

    2015-05-01

    Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particle-phase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids to phase-separated particles to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40 to 90%. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids; (2) forcing a single phase but accounting for non-ideal interactions through activity coefficient calculations; and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation of the inorganic and organic components is assumed at all RH values, with water uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquid-liquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrose-containing particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF

  6. Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

    For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show that secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±1 standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52), and 0.15 (±0.24) μg m-3, contributing 44, 28, 14, 13, and 2 % to the total non-refractory submicron mass (NR-PM1) respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF), in which five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3 respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual

  7. Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

    NASA Astrophysics Data System (ADS)

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

    2014-07-01

    For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±one standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52) and 0.15 (±0.24) μg m-3, contributing 43, 28, 14, 13 and 2% to the total submicron mass, respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF) where five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3, respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species, due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual pollution events influence London

  8. A COMPARATIVE REVIEW OF INORGANIC AEROSOL THERMODYNAMIC EQUILIBRIUM MODULES: SIMILARITIES, DIFFERENCES, AND THEIR LIKELY CAUSES

    EPA Science Inventory

    A comprehensive comparison of five inorganic aerosol thermodynamic equilibrium modules, MARS-A, SEQUILIB, SCAPE2, EQUISOLV II, and AIM2, was conducted for a variety of atmospheric concentrations of particulate matter (PM) constituents, relative humidities (RHs), and temperatures....

  9. Inorganic and black carbon aerosols in the Los Angeles Basin during CalNex

    NASA Astrophysics Data System (ADS)

    Ensberg, J. J.; Craven, J. S.; Metcalf, A. R.; Allan, J. D.; Angevine, W. M.; Bahreini, R.; Brioude, J.; Cai, C.; Coe, H.; Gouw, J. A.; Ellis, R. A.; Flynn, J. H.; Haman, C. L.; Hayes, P. L.; Jimenez, J. L.; Lefer, B. L.; Middlebrook, A. M.; Murphy, J. G.; Neuman, J. A.; Nowak, J. B.; Roberts, J. M.; Stutz, J.; Taylor, J. W.; Veres, P. R.; Walker, J. M.; Seinfeld, J. H.

    2013-02-01

    We evaluate predictions from the Community Multiscale Air Quality (CMAQ version 4.7.1) model against a suite of airborne and ground-based meteorological measurements, gas- and aerosol-phase inorganic measurements, and black carbon (BC) measurements over Southern California during the CalNex field campaign in May/June 2010. Ground-based measurements are from the CalNex Pasadena ground site, and airborne measurements took place onboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Navy Twin Otter and the NOAA WP-3D aircraft. BC predictions are in general agreement with observations at the Pasadena ground site and onboard the WP-3D, but are consistently overpredicted when compared to Twin Otter measurements. Adjustments to predicted inorganic mass concentrations, based on predicted aerosol size distributions and the AMS transmission efficiency, are shown to be significant. Owing to recent shipping emission reductions, the dominant source of sulfate in the L.A. Basin may now be long-range transport. Sensitivity studies suggest that severely underestimated ammonia emissions, and not the exclusion of crustal species (Ca2 +, K+, and Mg2 +), are the single largest contributor to measurement/model disagreement in the eastern part of the L.A. Basin. Despite overstated NOx emissions, total nitrate concentrations are underpredicted, which suggests a missing source of HNO3 and/or overprediction of deposition rates. Adding gas-phase NH3 measurements and size-resolved measurements, up to 10 μm, of nitrate and various cations (e.g. Na+, Ca2 +, K+) to routine monitoring stations in the L.A. Basin would greatly facilitate interpreting day-to-day fluctuations in fine and coarse inorganic aerosol.

  10. Inorganic aerosols responses to emission changes in Yangtze River Delta, China.

    PubMed

    Dong, Xinyi; Li, Juan; Fu, Joshua S; Gao, Yang; Huang, Kan; Zhuang, Guoshun

    2014-05-15

    The new Chinese National Ambient Air Quality standards (CH-NAAQS) published on Feb. 29th, 2012 listed PM2.5 as criteria pollutant for the very first time. In order to probe into PM2.5 pollution over Yangtze River Delta, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Total PM2.5 concentration over YRD was found to have strong seasonal variation with higher values in winter months (up to 89.9 μg/m(3) in January) and lower values in summer months (down to 28.8 μg/m(3) in July). Inorganic aerosols were found to have substantial contribution to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3(-)) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3(-) concentration throughout the year. In winter, NO3(-) was found to increase under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4(+)) and sulfate (SO4(2-)), while other seasons showed decrease response of NO3(-). Sensitivity responses of NO3(-) under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3(-) formation was actually more sensitive to VOC than NOx due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols.

  11. Inorganic aerosols responses to emission changes in Yangtze River Delta, China

    SciTech Connect

    Dong, Xinyi; Li, Juan; Fu, Joshua S.; Gao, Yang; Huang, Kan; Zhuang, Guoshun

    2014-05-15

    China announced the Chinese National Ambient Air Quality standards (CH-NAAQS) on Feb. 29th, 2012, and PM2.5 is for the very first time included in the standards as a criteria pollutant. In order to probe into PM2.5 pollution over Yangtze River Delta, which is one of the major urban clusters hosting more than 80 million people in China, the integrated MM5/CMAQ modeling system is applied for a full year simulation to examine the PM2.5 concentration and seasonality, and also the inorganic aerosols responses to precursor emission changes. Both simulation and observation demonstrated that, inorganic aerosols have substantial contributions to PM2.5 over YRD, ranging from 37.1% in November to 52.8% in May. Nocturnal production of nitrate (NO3-) through heterogeneous hydrolysis of N2O5 was found significantly contribute to high NO3-concentration throughout the year. We also found that in winter NO3- was even increased under nitrogen oxides (NOx) emission reduction due to higher production of N2O5 from the excessive ozone (O3) introduced by attenuated titration, which further lead to increase of ammonium (NH4+) and sulfate (SO42-), while other seasons showed decrease response of NO3-. Sensitivity responses of NO3- under anthropogenic VOC emission reduction was examined and demonstrated that in urban areas over YRD, NO3- formation was actually VOC sensitive due to the O3-involved nighttime chemistry of N2O5, while a reduction of NOx emission may have counter-intuitive effect by increasing concentrations of inorganic aerosols.

  12. Simulating the SOA formation of isoprene from partitioning and aerosol phase reactions in the presence of inorganics

    NASA Astrophysics Data System (ADS)

    Beardsley, Ross L.; Jang, Myoseon

    2016-05-01

    The secondary organic aerosol (SOA) produced by the photooxidation of isoprene with and without inorganic seed is simulated using the Unified Partitioning Aerosol Phase Reaction (UNIPAR) model. Recent work has found the SOA formation of isoprene to be sensitive to both aerosol acidity ([H+], mol L-1) and aerosol liquid water content (LWC) with the presence of either leading to significant aerosol phase organic mass generation and large growth in SOA yields (YSOA). Classical partitioning models alone are insufficient to predict isoprene SOA formation due to the high volatility of photooxidation products and sensitivity of their mass yields to variations in inorganic aerosol composition. UNIPAR utilizes the chemical structures provided by a near-explicit chemical mechanism to estimate the thermodynamic properties of the gas phase products, which are lumped based on their calculated vapor pressure (eight groups) and aerosol phase reactivity (six groups). UNIPAR then determines the SOA formation of each lumping group from both partitioning and aerosol phase reactions (oligomerization, acid-catalyzed reactions and organosulfate formation) assuming a single homogeneously mixed organic-inorganic phase as a function of inorganic composition and VOC / NOx (VOC - volatile organic compound). The model is validated using isoprene photooxidation experiments performed in the dual, outdoor University of Florida Atmospheric PHotochemical Outdoor Reactor (UF APHOR) chambers. UNIPAR is able to predict the experimental SOA formation of isoprene without seed, with H2SO4 seed gradually titrated by ammonia, and with the acidic seed generated by SO2 oxidation. Oligomeric mass is predicted to account for more than 65 % of the total organic mass formed in all cases and over 85 % in the presence of strongly acidic seed. The model is run to determine the sensitivity of YSOA to [H+], LWC and VOC / NOx, and it is determined that the SOA formation of isoprene is most strongly related to [H

  13. Simulating the SOA formation of isoprene from partitioning and aerosol phase reactions in the presence of inorganics

    NASA Astrophysics Data System (ADS)

    Beardsley, R. L.; Jang, M.

    2015-11-01

    The secondary organic aerosol (SOA) produced by the photooxidation of isoprene with and without inorganic seed is simulated using the Unified Partitioning Aerosol Phase Reaction (UNIPAR) model. Recent work has found the SOA formation of isoprene to be sensitive to both aerosol acidity ([H+]) and aerosol liquid water content (LWC) with the presence of either leading to significant aerosol phase organic mass generation and large growth in SOA yields (YSOA). Classical partitioning models alone are insufficient to predict isoprene SOA formation due to the high volatility of the photooxidation products and the sensitivity of their mass yields to variations in inorganic aerosol composition. UNIPAR utilizes the chemical structures provided by a near-explicit chemical mechanism to estimate the thermodynamic properties of the gas phase products, which are lumped based on their calculated vapor pressure (8 groups) and aerosol phase reactivity (6 groups). UNIPAR then determines the SOA formation of each lumping group from both partitioning and aerosol phase reactions (oligomerization, acid catalyzed reactions, and organosulfate formation) assuming a single homogeneously mixed organic-inorganic phase as a function of inorganic composition and VOC / NOx. The model is validated using isoprene photooxidation experiments performed in the dual, outdoor UF APHOR chambers. UNIPAR is able to predict the experimental SOA formation of isoprene without seed, with H2SO4 seed gradually titrated by ammonia, and with the acidic seed generated by SO2 oxidation. Oligomeric mass is predicted to account for more than 65 % of the total OM formed in all cases and over 85 % in the presence of strongly acidic seed. The model is run to determine the sensitivity of YSOA to [H+], LWC, and VOC / NOx, and it is determined that the SOA formation of isoprene is most strongly related to [H+] but is dynamically related to all three parameters. For VOC / NOx > 10, with increasing NOx both experimental and

  14. Computation of Phase Equilibria, State Diagrams and Gas/Particle Partitioning of Mixed Organic-Inorganic Aerosols

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Peter, T.

    2009-04-01

    The chemical composition of organic-inorganic aerosols is linked to several processes and specific topics in the field of atmospheric aerosol science. Photochemical oxidation of organics in the gas phase lowers the volatility of semi-volatile compounds and contributes to the particulate matter by gas/particle partitioning. Heterogeneous chemistry and changes in the ambient relative humidity influence the aerosol composition as well. Molecular interactions between condensed phase species show typically non-ideal thermodynamic behavior. Liquid-liquid phase separations into a mainly polar, aqueous and a less polar, organic phase may considerably influence the gas/particle partitioning of semi-volatile organics and inorganics (Erdakos and Pankow, 2004; Chang and Pankow, 2006). Moreover, the phases present in the aerosol particles feed back on the heterogeneous, multi-phase chemistry, influence the scattering and absorption of radiation and affect the CCN ability of the particles. Non-ideal thermodynamic behavior in mixtures is usually described by an expression for the excess Gibbs energy, enabling the calculation of activity coefficients. We use the group-contribution model AIOMFAC (Zuend et al., 2008) to calculate activity coefficients, chemical potentials and the total Gibbs energy of mixed organic-inorganic systems. This thermodynamic model was combined with a robust global optimization module to compute potential liquid-liquid (LLE) and vapor-liquid-liquid equilibria (VLLE) as a function of particle composition at room temperature. And related to that, the gas/particle partitioning of semi-volatile components. Furthermore, we compute the thermodynamic stability (spinodal limits) of single-phase solutions, which provides information on the process type and kinetics of a phase separation. References Chang, E. I. and Pankow, J. F.: Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water - Part

  15. 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.

  16. Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water—Part 2: Consideration of phase separation effects by an X-UNIFAC model

    NASA Astrophysics Data System (ADS)

    Chang, Elsa I.; Pankow, James F.

    A thermodynamic model is presented for predicting the formation of particulate matter (PM) within an aerosol that contains organic compounds, inorganic salts, and water. Neutral components are allowed to partition from the gas phase to the PM, with the latter potentially composed of both a primarily aqueous ( α) liquid phase and a primarily organic ( β) liquid phase. Partitioning is allowed to occur without any artificial restraints: when both α and β PM phases are present, ionic constituents are allowed to partition to both. X-UNIFAC.2, an extended UNIFAC method based on Yan et al. (1999. Prediction of vapor-liquid equilibria in mixed-solvent electrolyte systems using the group contribution concept. Fluid Phase Equilibria 162, 97-113), was developed for activity coefficient estimation. X-UNIFAC.2 utilizes the standard UNIFAC terms, a Debye-Hückel term, and a virial equation term that represents the middle-range (MR) contribution to activity coefficient effects. A large number (234) of MR parameters are already available from Yan et al. (1999). Six additional MR parameters were optimized here to enable X-UNIFAC.2 to account for interactions between the carboxylic acid group and Na +, Cl -, and Ca 2+. Predictions of PM formation were made for a hypothetical sabinene/O 3 system with varying amounts of NaCl in the PM. Predictions were also made for the chamber experiments with α-pinene/O 3 (and CaCl 2 seed) carried out by Cocker et al. (2001. The effect of water on gas-particle partitioning of secondary organic aerosol. Part I. α-pinene/ozone system. Atmospheric Environment 35, 6049-6072); good agreement between the predicted and chamber-measured PM mass concentrations was achieved.

  17. Secondary inorganic aerosol formation and its shortwave direct radiative forcing in China

    NASA Astrophysics Data System (ADS)

    Huang, Xin

    2015-04-01

    Secondary inorganic aerosol (SIA), including sulfate, nitrate and ammonium, is an important part of fine particle. SIA plays a significant role in shortwave radiation transfer. Numerical simulation is usually used to study SIA formation and its climate effect. In this work, we used the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to study SIA formation and its direct radiative forcing (DRF) over China. SO2 oxidation pathways related to mineral aerosol, including transition metal-catalyzed oxidation in aqueous phase and heterogeneous reactions, play an important role in sulfate production, but they are not well treated in current atmospheric models. In this work, we improved the WRF-Chem model by simulating the enhancement role of mineral aerosol in sulfate production. Firstly, we estimated mineral cations based on local measurements in order to well represent aqueous phase acidity. Secondly, we scaled the transition metal concentration to the mineral aerosol levels according to the existing observations and improved transition metal-catalyzed oxidation calculation. Lastly, heterogeneous reactions of acid gases on the surface of mineral aerosol were included in this simulation. Accuracy in the prediction of sulfate by the model was significantly improved and we concluded that mineral aerosol can facilitate SO2 oxidation and subsequent sulfate formation. It was demonstrated that, over China, mineral aerosol was responsible for 21.8% of annual mean sulfate concentration. The enhanced aqueous oxidation was more significant compared to the heterogeneous reactions. In winter, mineral aerosol was responsible for 39.6% of sulfate production. In summer, gaseous oxidation and aqueous oxidation of SO2 by hydrogen peroxide and ozone were the dominant pathways of sulfate formation. Mineral aerosol only contributed 11.9% to the total sulfate production. The increase in annual mean sulfate concentration due to mineral aerosol could reach up to over 6

  18. Global modeling of nitrate and ammonium aerosols using EQSAM3

    NASA Astrophysics Data System (ADS)

    Xu, L.; Penner, J. E.

    2009-12-01

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

  19. Improvement and further development in CESM/CAM5: gas-phase chemistry and inorganic aerosol treatments

    NASA Astrophysics Data System (ADS)

    He, J.; Zhang, Y.

    2014-09-01

    Gas-phase chemistry and subsequent gas-to-particle conversion processes such as new particle formation, condensation, and thermodynamic partitioning have large impacts on air quality, climate, and public health through influencing the amounts and distributions of gaseous precursors and secondary aerosols. Their roles in global air quality and climate are examined in this work using the Community Earth System Model version 1.0.5 (CESM1.0.5) with the Community Atmosphere Model version 5.1 (CAM5.1) (referred to as CESM1.0.5/CAM5.1). CAM5.1 includes a simple chemistry that is coupled with a 7-mode prognostic Modal Aerosol Model (MAM7). MAM7 includes classical homogenous nucleation (binary and ternary) and activation nucleation (empirical first-order power law) parameterizations, and a highly simplified inorganic aerosol thermodynamics treatment that only simulates particulate-phase sulfate and ammonium. In this work, a new gas-phase chemistry mechanism based on the 2005 Carbon Bond Mechanism for Global Extension (CB05_GE) and several advanced inorganic aerosol treatments for condensation of volatile species, ion-mediated nucleation (IMN), and explicit inorganic aerosol thermodynamics for sulfate, ammonium, nitrate, sodium, and chloride have been incorporated into CESM/CAM5.1-MAM7. Compared to the simple gas-phase chemistry, CB05_GE can predict many more gaseous species, and thus could improve model performance for PM2.5, PM10, PM components, and some PM gaseous precursors such as SO2 and NH3 in several regions as well as aerosol optical depth (AOD) and cloud properties (e.g., cloud fraction (CF), cloud droplet number concentration (CDNC), and shortwave cloud forcing, SWCF) on the global scale. The modified condensation and aqueous-phase chemistry could further improve the prediction of additional variables such as HNO3, NO2, and O3 in some regions, and new particle formation rate (J) and AOD on the global scale. IMN can improve the prediction of secondary PM2

  20. Formation of semivolatile inorganic aerosols in the Mexico City Metropolitan Area during the MILAGRO campaign

    NASA Astrophysics Data System (ADS)

    Karydis, V. A.; Tsimpidi, A. P.; Lei, W.; Molina, L. T.; Pandis, S. N.

    2011-12-01

    One of the most challenging tasks for chemical transport models (CTMs) is the prediction of the formation and partitioning of the major semi-volatile inorganic aerosol components (nitrate, chloride, ammonium) between the gas and particulate phases. In this work the PMCAMx-2008 CTM, which includes the recently developed aerosol thermodynamic model ISORROPIA-II, is applied in the Mexico City Metropolitan Area in order to simulate the formation of the major inorganic aerosol components. The main sources of SO2 (such as the Miguel Hidalgo Refinery and the Francisco Perez Rios Power Plant) in the Mexico City Metropolitan Area (MCMA) are located in Tula, resulting in high predicted PM1 (particulate matter with diameter less than 1 μm) sulfate concentrations (over 25 μg m-3) in that area. The average predicted PM1 nitrate concentrations are up to 3 μg m-3 (with maxima up to 11 μg m-3) in and around the urban center, mostly produced from local photochemistry. The presence of calcium coming from the Tolteca area (7 μg m-3) as well as the rest of the mineral cations (1 μg m-3 potassium, 1 μg m-3 magnesium, 2 μg m-3 sodium, and 3 μg m-3 calcium) from the Texcoco Lake resulted in the formation of a significant amount of aerosol nitrate in the coarse mode with concentrations up to 3 μg m-3 over these areas. PM1-10 (particulate matter with diameter between 1 and 10 μm) chloride is also high and its concentration exceeds 2 μg m-3 in Texcoco Lake. PM1 ammonium concentrations peak at the center of Mexico City (2 μg m-3) and the Tula vicinity (2.5 μg m-3). The performance of the model for the major inorganic PM components (sulfate, ammonium, nitrate, chloride, sodium, calcium, and magnesium) is encouraging. At the T0 measurement site, located in the Mexico City urban center, the average measured values of PM1 sulfate, nitrate, ammonium, and chloride are 3.5 μg m-3, 3.5 μg m-3, 2.1 μg m-3, and 0.36 μg m-3, respectively. The corresponding predicted values are 3.7

  1. Improvement and further development in CESM/CAM5: gas-phase chemistry and inorganic aerosol treatments

    NASA Astrophysics Data System (ADS)

    He, J.; Zhang, Y.

    2013-10-01

    Gas-phase chemistry and subsequent gas-to-particle conversion processes such as new particle formation, condensation, and thermodynamic partitioning have large impacts on air quality, climate, and public health through influencing the amounts and distributions of gaseous precursors and secondary aerosols. Their roles in global air quality and climate are examined in this work using the Community Earth System Model version 1.0.5 (CESM1.0.5) with the Community Atmosphere Model version 5.1 (CAM5.1) (referred to as CESM1.0.5/CAM5.1). CAM5.1 includes a simple chemistry that is coupled with a 7-mode prognostic Modal Aerosol Model (MAM7). MAM7 includes classical homogenous nucleation (binary and ternary) and activation nucleation (empirical first-order power law) parameterizations, and a highly-simplified inorganic aerosol thermodynamics treatment that only simulates sulfate (SO42-) and ammonium (NH4+). In this work, a new gas-phase chemistry mechanism based on the 2005 Carbon Bond Mechanism for Global Extension (CB05_GE) and several advanced inorganic aerosol treatments for condensation of volatile species, ion-mediated nucleation (IMN), and explicit inorganic aerosol thermodynamics have been incorporated into CESM/CAM5.1-MAM7. Comparing to the simple gas-phase chemistry, CB05_GE can predict many more gaseous species, and improve model performance for PM2.5, PM10, PM2.5 components, and some PM gaseous precursors such as SO2 and NH3 in several regions, as well as aerosol optical depth (AOD) and cloud properties (e.g., cloud fraction (CF), cloud droplet number concentration (CDNC), and shortwave cloud forcing (SWCF)) on globe. The modified condensation and aqueous-phase chemistry further improves the predictions of additional variables such as HNO3, NO2, and O3 in some regions, and new particle formation rate (J) and AOD over globe. IMN can improve the predictions of secondary PM2.5 components, PM2.5, and PM10 over Europe, as well as AOD and CDNC over globe. The explicit

  2. Formation of semivolatile inorganic aerosols in the mexico city metropolitan area during the milagro campaign

    NASA Astrophysics Data System (ADS)

    Karydis, V. A.; Tsimpidi, A. P.; Lei, W.; Molina, L. T.; Pandis, S. N.

    2011-08-01

    One of the most challenging tasks for chemical transport models (CTMs) is the prediction of the formation and partitioning of the major semi-volatile inorganic aerosol components (nitrate, chloride, ammonium) between the gas and particulate phases. In this work the PMCAMx-2008 CTM, which includes the recently developed aerosol thermodynamic model ISORROPIA-II, is applied in the Mexico City Metropolitan Area in order to simulate the formation of the major inorganic aerosol components. The main sources of SO2 (such as the Miguel Hidalgo Refinery and the Francisco Perez Rios Power Plant) in the Mexico City Metropolitan Area (MCMA) are located in Tula, resulting in high predicted PM1 sulfate concentrations (over 25 μg m-3) in that area. The average predicted PM1 nitrate concentrations are up to 3 μg m-3 (with maxima up to 11 μg m-3) in and around the urban center, mostly produced from local photochemistry. The presence of calcium coming from the Tolteca area (7 μg m-3) as well as the rest of the mineral cations (1 μg m-3 potassium, 1 μg m-3 magnesium, 2 μg m-3 sodium, and 3 μg m-3 calcium) from the Texcoco Lake resulted in the formation of a significant amount of aerosol nitrate in the coarse mode with concentrations up to 3 μg m-3 over these areas. PM1-10 chloride is also high and its concentration exceeds 2 μg m-3 in Texcoco Lake. PM ammonium concentrations peak at the center of Mexico City (2 μg m-3) and the Tula vicinity (2.5 μg m-3). The performance of the model for the major inorganic PM components (sulfate, ammonium, nitrate, chloride, sodium, calcium, and magnesium) is encouraging. At T0, the average measured values of PM1 sulfate, nitrate, ammonium, and chloride are 3.6 μg m-3, 3.6 μg m-3, 2.1 μg m-3, and 0.35 μg m-3 respectively. The corresponding predicted values are 3.7 μg m-3, 2.8 μg m-3, 1.7 μg m-3, and 0.25 μg m-3. Additional improvements are possible by (i) using a day-dependent emission inventory, (ii) improving the performance of

  3. Aerosol Modeling for the Global Model Initiative

    NASA Technical Reports Server (NTRS)

    Weisenstein, Debra K.; Ko, Malcolm K. W.

    2001-01-01

    The goal of this project is to develop an aerosol module to be used within the framework of the Global Modeling Initiative (GMI). The model development work will be preformed jointly by the University of Michigan and AER, using existing aerosol models at the two institutions as starting points. The GMI aerosol model will be tested, evaluated against observations, and then applied to assessment of the effects of aircraft sulfur emissions as needed by the NASA Subsonic Assessment in 2001. The work includes the following tasks: 1. Implementation of the sulfur cycle within GMI, including sources, sinks, and aqueous conversion of sulfur. Aerosol modules will be added as they are developed and the GMI schedule permits. 2. Addition of aerosol types other than sulfate particles, including dust, soot, organic carbon, and black carbon. 3. Development of new and more efficient parameterizations for treating sulfate aerosol nucleation, condensation, and coagulation among different particle sizes and types.

  4. Effects of inorganic seed aerosols on the particulate products of aged 1,3,5-trimethylbenzene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Huang, Mingqiang; Hao, Liqing; Cai, Shunyou; Gu, Xuejun; Zhang, Weixiong; Hu, Changjin; Wang, Zhenya; Fang, Li; Zhang, Weijun

    2017-03-01

    Inorganic aerosols such as (NH4)2SO4, NaNO3 and CaCl2 are commonly present in the Chinese urban atmosphere. They could significantly affect the formation and aging of ambient secondary organic aerosols (SOA), but the underlying mechanisms remain unknown. In this work we studied SOA formation from the photooxidation reaction of 1,3,5-trimethylbenzene (135-TMB) with 100 μg/m3 of the above three types of inorganic aerosols as seeds in a laboratory chamber. We focused on the aging products of SOA particles by exposing them to high levels of oxidizing hydroxyl radicals (OH). The particulate products of SOA were measured using an aerosol laser time-of-flight mass spectrometer (ALTOFMS) and Fuzzy C-Means (FCM) were applied to organic mass spectra for clustering. In the presence of (NH4)2SO4 seeds, 4-methyl-1H-imidazole, 4-methyl-imidazole-2-acetaldehyde and other imidazole derivative compounds formed from reactions of NH4+ with methylglyoxal were detected as new aged products. We also observed aromatic nitrogen-containing organic compounds as the major aged products in the presence of NaNO3 seeds as a consequence of reaction with OH and NO2 radicals, which were generated by UV irradiation of acidic aqueous nitrate, inducing nitration reactions with phenolic compounds. As CaCl2 has the strongest hygroscopic properties of the three salt particles tested, the greater water content on the surface of the aerosol may facilitate the condensing of more gas-phase organic acid products to the hygroscopic CaCl2 seeds, forming H+ ions that catalyze the heterogeneous reaction of aldehydes, products of photooxidation of 135-TMB, and forming high-molecular-weight (HMW) compounds. These results provide new insight into the aromatic SOA aging mechanisms.

  5. Inorganic markers, carbonaceous components and stable carbon isotope from biomass burning aerosols in Northeast China.

    PubMed

    Cao, Fang; Zhang, Shi-Chun; Kawamura, Kimitaka; Zhang, Yan-Lin

    2016-12-01

    To better characterize the chemical compositions and sources of fine particulate matter (i.e. PM2.5) in Sanjiang Plain, Northeast China, total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions as well as stable carbon isotopic composition (δ(13)C) were measured in this study. Intensively open biomass burning episodes are identified from late September to early October by satellite fire and aerosol optical depth maps. During the biomass-burning episode, concentrations of PM2.5, OC, EC, and WSOC are increased by a factor of 4-12 compared to those during the non-biomass-burning period. Non-sea-salt potassium is strongly correlated with PM2.5, OC, EC and WSOC, demonstrating an important contribution from biomass-burning emissions. The enrichment in both the non-sea-salt potassium and chlorine is significantly larger than other inorganic species, suggesting that biomass-burning aerosols in Sanjiang Plain are mostly fresh and less aged. In addition, the WSOC-to-OC ratio is lower than that reported in biomass-burning aerosols in tropical regions, further supporting that biomass-burning aerosols in Sanjiang Plain are mostly primary and secondary organic aerosols may be not significant. A lower average δ(13)C value (-26.2‰) is observed during the biomass-burning period, indicating a dominant contribution from combustion of C3 plants in the studied region.

  6. Using a latent variable model with non-constant factor loadings to examine PM2.5 constituents related to secondary inorganic aerosols

    PubMed Central

    Zhang, Zhenzhen; O’Neill, Marie S.; Sánchez, Brisa N.

    2016-01-01

    Factor analysis is a commonly used method of modelling correlated multivariate exposure data. Typically, the measurement model is assumed to have constant factor loadings. However, from our preliminary analyses of the Environmental Protection Agency’s (EPA’s) PM2.5 fine speciation data, we have observed that the factor loadings for four constituents change considerably in stratified analyses. Since invariance of factor loadings is a prerequisite for valid comparison of the underlying latent variables, we propose a factor model that includes non-constant factor loadings that change over time and space using P-spline penalized with the generalized cross-validation (GCV) criterion. The model is implemented using the Expectation-Maximization (EM) algorithm and we select the multiple spline smoothing parameters by minimizing the GCV criterion with Newton’s method during each iteration of the EM algorithm. The algorithm is applied to a one-factor model that includes four constituents. Through bootstrap confidence bands, we find that the factor loading for total nitrate changes across seasons and geographic regions. PMID:27528825

  7. MATHEMATICAL MODEL FOR GAS/PARTICLE PARTITIONING OF SECONDARY ORGANIC AEROSOLS. (R824970)

    EPA Science Inventory

    A dynamic model is developed for gas-particle absorptive partitioning of semi-volatile organic aerosols. The model is applied to simulate a pair of m-xylene/NOx outdoor smog chamber experiments. In the presence of an inorganic seed aerosol a threshold ...

  8. Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China

    NASA Astrophysics Data System (ADS)

    Zheng, B.; Zhang, Q.; Zhang, Y.; He, K. B.; Wang, K.; Zheng, G. J.; Duan, F. K.; Ma, Y. L.; Kimoto, T.

    2015-02-01

    Severe regional haze pollution events occurred in eastern and central China in January 2013, which had adverse effects on the environment and public health. Extremely high levels of particulate matter with aerodynamic diameter of 2.5 μm or less (PM2.5) with dominant components of sulfate and nitrate are responsible for the haze pollution. Although heterogeneous chemistry is thought to play an important role in the production of sulfate and nitrate during haze episodes, few studies have comprehensively evaluated the effect of heterogeneous chemistry on haze formation in China by using the 3-D models due to of a lack of treatments for heterogeneous reactions in most climate and chemical transport models. In this work, the WRF-CMAQ model with newly added heterogeneous reactions is applied to East Asia to evaluate the impacts of heterogeneous chemistry and the meteorological anomaly during January 2013 on regional haze formation. As the parameterization of heterogeneous reactions on different types of particles is not well established yet, we arbitrarily selected the uptake coefficients from reactions on dust particles and then conducted several sensitivity runs to find the value that can best match observations. The revised CMAQ with heterogeneous chemistry not only captures the magnitude and temporal variation of sulfate and nitrate, but also reproduces the enhancement of relative contribution of sulfate and nitrate to PM2.5 mass from clean days to polluted haze days. These results indicate the significant role of heterogeneous chemistry in regional haze formation and improve the understanding of the haze formation mechanisms during the January 2013 episode.

  9. Inorganic Salt Interference on CO2(+) in Aerodyne AMS and ACSM Organic Aerosol Composition Studies.

    PubMed

    Pieber, Simone M; El Haddad, Imad; Slowik, Jay G; Canagaratna, Manjula R; Jayne, John T; Platt, Stephen M; Bozzetti, Carlo; Daellenbach, Kaspar R; Fröhlich, Roman; Vlachou, Athanasia; Klein, Felix; Dommen, Josef; Miljevic, Branka; Jiménez, José L; Worsnop, Douglas R; Baltensperger, Urs; Prévôt, André S H

    2016-10-04

    Aerodyne aerosol mass spectrometer (AMS) and Aerodyne aerosol chemical speciation monitor (ACSM) mass spectra are widely used to quantify organic aerosol (OA) elemental composition, oxidation state, and major environmental sources. The OA CO2(+) fragment is among the most important measurements for such analyses. Here, we show that a non-OA CO2(+) signal can arise from reactions on the particle vaporizer, ion chamber, or both, induced by thermal decomposition products of inorganic salts. In our tests (eight instruments, n = 29), ammonium nitrate (NH4NO3) causes a median CO2(+) interference signal of +3.4% relative to nitrate. This interference is highly variable between instruments and with measurement history (percentiles P10-90 = +0.4 to +10.2%). Other semi-refractory nitrate salts showed 2-10 times enhanced interference compared to that of NH4NO3, while the ammonium sulfate ((NH4)2SO4) induced interference was 3-10 times lower. Propagation of the CO2(+) interference to other ions during standard AMS and ACSM data analysis affects the calculated OA mass, mass spectra, molecular oxygen-to-carbon ratio (O/C), and f44. The resulting bias may be trivial for most ambient data sets but can be significant for aerosol with higher inorganic fractions (>50%), e.g., for low ambient temperatures, or laboratory experiments. The large variation between instruments makes it imperative to regularly quantify this effect on individual AMS and ACSM systems.

  10. SOA formation from partitioning and heterogeneous reactions: model study in the presence of inorganic species.

    PubMed

    Jang, Myoseon; Czoschke, Nadine M; Northcross, Amanda L; Cao, Gang; Shaof, David

    2006-05-01

    A predictive model for secondary organic aerosol (SOA) formation by both partitioning and heterogeneous reactions was developed for SOA created from ozonolysis of alpha-pinene in the presence of preexisting inorganic seed aerosols. SOA was created in a 2 m3 polytetrafluoroethylene film indoor chamber under darkness. Extensive sets of SOA experiments were conducted varying humidity, inorganic seed compositions comprising of ammonium sulfate and sulfuric acid, and amounts of inorganic seed mass. SOA mass was decoupled into partitioning (OM(P)) and heterogeneous aerosol production (OM(H)). The reaction rate constant for OM(H) production was subdivided into three categories (fast, medium, and slow) to consider different reactivity of organic products for the particle phase heterogeneous reactions. The influence of particle acidity on reaction rates was treated in a previous semiempirical model. Model OM(H) was developed with medium and strong acidic seed aerosols, and then extrapolated to OM(H) in weak acidic conditions, which are more relevant to atmospheric aerosols. To demonstrate the effects of preexisting glyoxal derivatives (e.g., glyoxal hydrate and dimer) on OM(H), SOA was created with a seed mixture comprising of aqueous glyoxal and inorganic species. Our results show that heterogeneous SOA formation was also influenced by preexisting reactive glyoxal derivatives.

  11. Simultaneous online monitoring of inorganic compounds in aerosols and gases in an industrialized area

    NASA Astrophysics Data System (ADS)

    Khezri, Bahareh; Mo, Huan; Yan, Zhen; Chong, Shey-Ling; Heng, Aik Kian; Webster, Richard D.

    2013-12-01

    The automatic MARGA (monitor for aerosols and gases in ambient air) sampling system was used to measure the inorganic ions Cl-, NO3-, SO42-, Na+, NH4+, K+, Mg2+ and Ca2+ in the PM2.5 aerosol phase and the corresponding inorganic gases HCl, HNO2, SO2, HNO3 and NH3 present in the gas phase. Samples were collected and analyzed hourly for 3 months between April and June, 2011, from a sampling site in Singapore close to a heavy industrial area containing extensive petrochemical refineries. The data (hourly and daily average) were analyzed, compared and discussed based on the ratios of HNO2/HNO3 and NH3/NH4+, the levels of nitrate and sulfate, the total nitrogen, the distribution of particulate matter and gaseous compounds, and the acidity of the aerosols. SO2 was the most abundant gas that appeared in an order of magnitude higher concentration than the other trace gases, and correspondingly SO42- was found to be at least 3-10 times higher than other anionic aerosol species. The concentration of major ions in aerosol samples and the related gaseous compounds followed the order of: SO42- > NH4+ > NO3- > K+ > Na+ > Cl- > Ca2+ > Mg2+ and SO2 > NH3 > HNO2 > HNO3, respectively. The maximum values for many of the target analytes occurred during the hazy period in May when there was significant contamination from regional fires. The elevated levels of HNO2 compared to HNO3 and high levels of HNO3 were rationalized based on artifacts in the denuder sampling methodology.

  12. CONTINUED DEVELOPMENT AND TESTING OF A NEW THERMODYNAMIC AEROSOL MODULE FOR URBAN AND REGIONAL AIR QUALITY MODELS. (R824793)

    EPA Science Inventory

    A computationally efficient and rigorous thermodynamic model (ISORROPIA) that predicts the physical state and composition of inorganic atmospheric aerosol is presented. The advantages of this particular model render it suitable for incorporation into urban and regional air qualit...

  13. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

    NASA Astrophysics Data System (ADS)

    Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

    2008-03-01

    Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/citric acid and in the ammonium sulfate/glutaric acid cases. However, we observe significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

  14. Aerosol measurement program strategy for global aerosol backscatter model development

    NASA Technical Reports Server (NTRS)

    Bowdle, David A.

    1985-01-01

    The purpose was to propose a balanced program of aerosol backscatter research leading to the development of a global model of aerosol backscatter. Such a model is needed for feasibility studies and systems simulation studies for NASA's prospective satellite-based Doppler lidar wind measurement system. Systems of this kind measure the Doppler shift in the backscatter return from small atmospheric aerosol wind tracers (of order 1 micrometer diameter). The accuracy of the derived local wind estimates and the degree of global wind coverage for such a system are limited by the local availability and by the global scale distribution of natural aerosol particles. The discussions here refer primarily to backscatter model requirements at CO2 wavelengths, which have been selected for most of the Doppler lidar systems studies to date. Model requirements for other potential wavelengths would be similar.

  15. Modeling the surface tension of complex, reactive organic-inorganic mixtures

    NASA Astrophysics Data System (ADS)

    Schwier, A. N.; Viglione, G. A.; Li, Z.; McNeill, V. Faye

    2013-11-01

    Atmospheric aerosols can contain thousands of organic compounds which impact aerosol surface tension, affecting aerosol properties such as heterogeneous reactivity, ice nucleation, and cloud droplet formation. We present new experimental data for the surface tension of complex, reactive organic-inorganic aqueous mixtures mimicking tropospheric aerosols. Each solution contained 2-6 organic compounds, including methylglyoxal, glyoxal, formaldehyde, acetaldehyde, oxalic acid, succinic acid, leucine, alanine, glycine, and serine, with and without ammonium sulfate. We test two semi-empirical surface tension models and find that most reactive, complex, aqueous organic mixtures which do not contain salt are well described by a weighted Szyszkowski-Langmuir (S-L) model which was first presented by Henning et al. (2005). Two approaches for modeling the effects of salt were tested: (1) the Tuckermann approach (an extension of the Henning model with an additional explicit salt term), and (2) a new implicit method proposed here which employs experimental surface tension data obtained for each organic species in the presence of salt used with the Henning model. We recommend the use of method (2) for surface tension modeling of aerosol systems because the Henning model (using data obtained from organic-inorganic systems) and Tuckermann approach provide similar modeling results and goodness-of-fit (χ2) values, yet the Henning model is a simpler and more physical approach to modeling the effects of salt, requiring less empirically determined parameters.

  16. Emissions of Black Carbon, Organic, and Inorganic Aerosols From Biomass Burning in North America and Asia in 2008

    NASA Technical Reports Server (NTRS)

    Kondo, Y.; Matsui, H.; Moteki, N.; Sahu, L.; Takegawa, N.; Kajino, M.; Zhao, Y.; Cubison, M. J.; Jimenez, J. L.; Vay, S.; Diskin, G. S.; Anderson, B.; Wisthaler, A.; Mikoviny, T.; Fuelberg, H. E.; Blake, D. R.; Huey, G.; Weinheimer, A. J.; Knapp, D. J.; Brune, W. H.

    2011-01-01

    Reliable assessment of the impact of aerosols emitted from boreal forest fires on the Arctic climate necessitates improved understanding of emissions and the microphysical properties of carbonaceous (black carbon (BC) and organic aerosols (OA)) and inorganic aerosols. The size distributions of BC were measured by an SP2 based on the laser-induced incandescence technique on board the DC-8 aircraft during the NASA ARCTAS campaign. Aircraft sampling was made in fresh plumes strongly impacted by wildfires in North America (Canada and California) in summer 2008 and in those transported from Asia (Siberia in Russia and Kazakhstan) in spring 2008. We extracted biomass burning plumes using particle and tracer (CO, CH3CN, and CH2Cl2) data. OA constituted the dominant fraction of aerosols mass in the submicron range. The large majority of the emitted particles did not contain BC. We related the combustion phase of the fire as represented by the modified combustion efficiency (MCE) to the emission ratios between BC and other species. In particular, we derived the average emission ratios of BC/CO = 2.3 +/- 2.2 and 8.5 +/- 5.4 ng/cu m/ppbv for BB in North America and Asia, respectively. The difference in the BC/CO emission ratios is likely due to the difference in MCE. The count median diameters and geometric standard deviations of the lognormal size distribution of BC in the BB plumes were 136-141 nm and 1.32-1.36, respectively, and depended little on MCE. These BC particles were thickly coated, with shell/core ratios of 1.3-1.6. These parameters can be used directly for improving model estimates of the impact of BB in the Arctic.

  17. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

    NASA Astrophysics Data System (ADS)

    Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

    2008-09-01

    Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/glutaric acid system; deviations up to 10% in mass growth factor (corresponding to deviations up to 3.5% in size growth factor) are observed for the ammonium sulfate/citric acid 1:1 mixture at 80% RH. We observe even more significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

  18. Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

    NASA Astrophysics Data System (ADS)

    Quan, Jiannong; Liu, Quan; Li, Xia; Gao, Yang; Jia, Xingcan; Sheng, Jiujiang; Liu, Yangang

    2015-12-01

    The effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM2.5), nitrate (NO3), sulfate (SO4), ammonium (NH4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO2), and ozone (O3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (Nratio) and S from SO2 to sulfate (Sratio) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO2 to their corresponding particle phases in the late haze period. Further analysis shows that Nratio and Sratio increased with increasing RH, with Nratio and Sratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60-80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of Nratio and Sratio to O3: the conversion ratios increase with decreasing O3 concentration when O3 concentration is lower than <15 ppb but increased with increasing O3 when O3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO2 and NOx, accelerated the formation of secondary

  19. Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

    SciTech Connect

    Quan, Jiannong; Liu, Yangang; Liu, Quan; Li, Xia; Gao, Yang; Jia, Xingcan; Sheng, Jiujiang

    2015-09-30

    In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM2.5), nitrate (NO3), sulfate (SO4), ammonium (NH4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO2), and ozone (O3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (Nratio) and S from SO2 to sulfate (Sratio) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO2 to their corresponding particle phases in the late haze period. Further analysis shows that Nratio and Sratio increased with increasing RH, with Nratio and Sratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of Nratio and Sratio to O3: the conversion ratios increase with decreasing O3 concentration when O3 concentration is lower than <15 ppb but increased with increasing O3 when O3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly

  20. Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

    DOE PAGES

    Quan, Jiannong; Liu, Yangang; Liu, Quan; ...

    2015-09-30

    In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM2.5), nitrate (NO3), sulfate (SO4), ammonium (NH4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO2), and ozone (O3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (Nratio) and S from SO2 to sulfate (Sratio) bothmore » significantly increased in haze events, suggesting enhanced conversions from NOx and SO2 to their corresponding particle phases in the late haze period. Further analysis shows that Nratio and Sratio increased with increasing RH, with Nratio and Sratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of Nratio and Sratio to O3: the conversion ratios increase with decreasing O3 concentration when O3 concentration is lower than <15 ppb but increased with increasing O3 when O3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO2 and NOx, accelerated the

  1. Individual aerosol particles from biomass burning in southern Africa: 2, Compositions and aging of inorganic particles

    NASA Astrophysics Data System (ADS)

    Li, Jia; Pósfai, MiháLy; Hobbs, Peter V.; Buseck, Peter R.

    2003-07-01

    Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen-bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

  2. Aerosol Behavior Log-Normal Distribution Model.

    SciTech Connect

    GIESEKE, J. A.

    2001-10-22

    HAARM3, an acronym for Heterogeneous Aerosol Agglomeration Revised Model 3, is the third program in the HAARM series developed to predict the time-dependent behavior of radioactive aerosols under postulated LMFBR accident conditions. HAARM3 was developed to include mechanisms of aerosol growth and removal which had not been accounted for in the earlier models. In addition, experimental measurements obtained on sodium oxide aerosols have been incorporated in the code. As in HAARM2, containment gas temperature, pressure, and temperature gradients normal to interior surfaces are permitted to vary with time. The effects of reduced density on sodium oxide agglomerate behavior and of nonspherical shape of particles on aerosol behavior mechanisms are taken into account, and aerosol agglomeration due to turbulent air motion is considered. Also included is a capability to calculate aerosol concentration attenuation factors and to restart problems requiring long computing times.

  3. Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Peter, T.; Seinfeld, J. H.

    2010-08-01

    Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of multicomponent systems. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system

  4. Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Marcolli, C.; Peter, T.; Seinfeld, J. H.

    2010-05-01

    Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of the phase diagram. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system simulation

  5. Global modeling of tropospheric iodine aerosol

    NASA Astrophysics Data System (ADS)

    Sherwen, Tomás. M.; Evans, Mat J.; Spracklen, Dominick V.; Carpenter, Lucy J.; Chance, Rosie; Baker, Alex R.; Schmidt, Johan A.; Breider, Thomas J.

    2016-09-01

    Natural aerosols play a central role in the Earth system. The conversion of dimethyl sulfide to sulfuric acid is the dominant source of oceanic secondary aerosol. Ocean emitted iodine can also produce aerosol. Using a GEOS-Chem model, we present a simulation of iodine aerosol. The simulation compares well with the limited observational data set. Iodine aerosol concentrations are highest in the tropical marine boundary layer (MBL) averaging 5.2 ng (I) m-3 with monthly maximum concentrations of 90 ng (I) m-3. These masses are small compared to sulfate (0.75% of MBL burden, up to 11% regionally) but are more significant compared to dimethyl sulfide sourced sulfate (3% of the MBL burden, up to 101% regionally). In the preindustrial, iodine aerosol makes up 0.88% of the MBL burden sulfate mass and regionally up to 21%. Iodine aerosol may be an important regional mechanism for ocean-atmosphere interaction.

  6. Impact of secondary inorganic aerosol and road traffic at a suburban air quality monitoring station.

    PubMed

    Megido, L; Negral, L; Castrillón, L; Fernández-Nava, Y; Suárez-Peña, B; Marañón, E

    2017-03-15

    PM10 from a suburban site in the northwest of Spain was assessed using data from chemical determinations, meteorological parameters, aerosol maps and five-day back trajectories of air masses. Temporal variations in the chemical composition of PM10 were subsequently related to stationary/mobile local sources and long-range transport stemming from Europe and North Africa. The presence of secondary inorganic species (sulphates, nitrates and ammonium) in airborne particulate matter constituted one of the main focuses of this study. These chemical species formed 16.5% of PM10 on average, in line with other suburban background sites in Europe. However, a maximum of 47.8% of PM10 were recorded after several days under the influence of European air masses. Furthermore, the highest values of these three chemical species coincided with episodes of poor air circulation and influxes of air masses from Europe. The relationship between SO4(2-) and NH4(+) (R(2) = 0.57, p-value<0.01) was found to improve considerably in summer and spring (R(2) = 0.88 and R(2) = 0.87, respectively, p-value<0.01), whereas NO3(-) and NH4(+) (R(2) = 0.55, p-value<0.01) reproduced this pattern in winter (R(2) = 0.91, p-value<0.01). The application of a receptor model to the dataset led to the identification of notable apportionments due to road traffic and other types of combustion processes. In fact, large amounts of particulate matter were released to the atmosphere during episodes of biomass burning in forest fires. On isolated days, combustion was estimated to contribute up to 21.0 μg PM/m(3) (50.8% of PM10). The contribution from industrial processes to this source is also worth highlighting given the presence of Ni and Co in its profile. Furthermore, African dust outbreaks at the sampling site, characterised by an arc through the Atlantic Ocean, were usually associated with a higher concentration of Al2O3 in PM10. Results evidenced the relevance of stationary (i.e., steelworks and

  7. Influence of collecting substrates on the characterization of hygroscopic properties of inorganic aerosol particles.

    PubMed

    Eom, Hyo-Jin; Gupta, Dhrubajyoti; Li, Xue; Jung, Hae-Jin; Kim, Hyekyeong; Ro, Chul-Un

    2014-03-04

    The influence of six collecting substrates with different physical properties on the hygroscopicity measurement of inorganic aerosol particle surrogates and the potential applications of these substrates were examined experimentally. Laboratory-generated single salt particles, such as NaCl, KCl, and (NH4)2SO4, 1-5 μm in size, were deposited on transmission electron microscopy grids (TEM grids), parafilm-M, Al foil, Ag foil, silicon wafer, and cover glass. The particle hygroscopic properties were examined by optical microscopy. Contact angle measurements showed that parafilm-M is hydrophobic, and cover glass, silicon wafer, Al foil, and Ag foil substrates are hydrophilic. The observed deliquescence relative humidity (DRH) values for NaCl, KCl, and (NH4)2SO4 on the TEM grids and parafilm-M substrates agreed well with the literature values, whereas the DRHs obtained on the hydrophilic substrates were consistently ∼1-2% lower, compared to those on the hydrophobic substrates. The water layer adsorbed on the salt crystals prior to deliquescence increases the Gibb's free energy of the salt crystal-substrate system compared to the free energy of the salt droplet-substrate system, which in turn reduces the DRHs. The hydrophilic nature of the substrate does not affect the measured efflorescence RH (ERH) values. However, the Cl(-) or SO4(2-) ions in aqueous salt droplets seem to have reacted with Ag foil to form AgCl or Ag2SO4, respectively, which in turn acts as seeds for the heterogeneous nucleation of the original salts, leading to higher ERHs. The TEM grids were found to be most suitable for the hygroscopic measurements of individual inorganic aerosol particles by optical microscopy and when multiple analytical techniques, such as scanning electron microscopy-energy dispersive X-ray spectroscopy, TEM-EDX, and/or Raman microspectrometry, are applied to the same individual particles.

  8. Effect of high concentrations of inorganic seed aerosols on secondary organic aerosol formation in the m-xylene/NO x photooxidation system

    NASA Astrophysics Data System (ADS)

    Lu, Zifeng; Hao, Jiming; Takekawa, Hideto; Hu, Lanhua; Li, Junhua

    High concentrations (>15 μm 3 cm -3) of CaSO 4, Ca(NO 3) 2 and (NH 4) 2SO 4 were selected as surrogates of dry neutral, aqueous neutral and dry acidic inorganic seed aerosols, respectively, to study the effects of inorganic seeds on secondary organic aerosol (SOA) formation in irradiated m-xylene/NO x photooxidation systems. The results indicate that neither ozone formation nor SOA formation is significantly affected by the presence of neutral aerosols (both dry CaSO 4 and aqueous Ca(NO 3) 2), even at elevated concentrations. The presence of high concentrations of (NH 4) 2SO 4 aerosols (dry acidic) has no obvious effect on ozone formation, but it does enhance SOA generation and increase SOA yields. In addition, the effect of dry (NH 4) 2SO 4 on SOA yield is found to be positively correlated with the (NH 4) 2SO 4 surface concentration, and the effect is pronounced only when the surface concentration reaches a threshold value. Further, it is proposed that the SOA generation enhancement is achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of dry (NH 4) 2SO 4 seed aerosols.

  9. 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

  10. Balloon observations of organic and inorganic chlorine in the stratosphere: the role of HClO4 production on sulfate aerosols

    NASA Technical Reports Server (NTRS)

    Jaegle, L.; Yung, Y. L.; Toon, G. C.; Sen, B.; Blavier, J. F.

    1996-01-01

    Simultaneous observations of stratospheric organic and inorganic chlorine were made in September 1993 out of Fort Sumner, New Mexico, using JPL balloon-borne MkIV interferometer. Between 15 and 20 km, a significant fraction (20-60%) of the inorganic chlorine could not be accounted for by the sum of measured HCl, ClONO2, and HOCl. Laboratory measurements of the reaction of ClO radicals on sulfuric acid solutions have indicated that, along with HCl, small amounts of perchloric acid, HClO4, were formed. Very little is known about the fate of HClO4 in the stratosphere and we use a photochemical box model to determine the impact of this new species on the partitioning of inorganic chlorine in the stratosphere. Assuming that HClO4 is photochemically stable, it is shown that in the enhanced aerosol loading conditions resulting from Mt. Pinatubo's eruption, HClO4 could represent a significant reservoir of chlorine in the lower stratosphere, sequestering up to 0.2 ppbv (or 50%) of the total inorganic chlorine at 16 km. The occurrence of this new species could bring to closure the inorganic chlorine budget deficiency made apparent by recent ER-2 aircraft in situ measurements of HCl.

  11. Balloon observations of organic and inorganic chlorine in the stratosphere: the role of HClO4 production on sulfate aerosols.

    PubMed

    Jaegle, L; Yung, Y L; Toon, G C; Sen, B; Blavier, J F

    1996-07-01

    Simultaneous observations of stratospheric organic and inorganic chlorine were made in September 1993 out of Fort Sumner, New Mexico, using JPL balloon-borne MkIV interferometer. Between 15 and 20 km, a significant fraction (20-60%) of the inorganic chlorine could not be accounted for by the sum of measured HCl, ClONO2, and HOCl. Laboratory measurements of the reaction of ClO radicals on sulfuric acid solutions have indicated that, along with HCl, small amounts of perchloric acid, HClO4, were formed. Very little is known about the fate of HClO4 in the stratosphere and we use a photochemical box model to determine the impact of this new species on the partitioning of inorganic chlorine in the stratosphere. Assuming that HClO4 is photochemically stable, it is shown that in the enhanced aerosol loading conditions resulting from Mt. Pinatubo's eruption, HClO4 could represent a significant reservoir of chlorine in the lower stratosphere, sequestering up to 0.2 ppbv (or 50%) of the total inorganic chlorine at 16 km. The occurrence of this new species could bring to closure the inorganic chlorine budget deficiency made apparent by recent ER-2 aircraft in situ measurements of HCl.

  12. Evolution of ozone, particulates, and aerosol direct radiative forcing in the vicinity of Houston using a fully coupled meteorology-chemistry-aerosol model

    NASA Astrophysics Data System (ADS)

    Fast, Jerome D.; Gustafson, William I.; Easter, Richard C.; Zaveri, Rahul A.; Barnard, James C.; Chapman, Elaine G.; Grell, Georg A.; Peckham, Steven E.

    2006-11-01

    A new fully coupled meteorology-chemistry-aerosol model is used to simulate the urban- to regional-scale variations in trace gases, particulates, and aerosol direct radiative forcing in the vicinity of Houston over a 5 day summer period. Model performance is evaluated using a wide range of meteorological, chemistry, and particulate measurements obtained during the 2000 Texas Air Quality Study. The predicted trace gas and particulate distributions were qualitatively similar to the surface and aircraft measurements with considerable spatial variations resulting from urban, power plant, and industrial sources of primary pollutants. Sulfate, organic carbon, and other inorganics were the largest constituents of the predicted particulates. The predicted shortwave radiation was 30 to 40 W m-2 closer to the observations when the aerosol optical properties were incorporated into the shortwave radiation scheme; however, the predicted hourly aerosol radiative forcing was still underestimated by 10 to 50 W m-2. The predicted aerosol radiative forcing was larger over Houston and the industrial ship channel than over the rural areas, consistent with surface measurements. The differences between the observed and simulated aerosol radiative forcing resulted from transport errors, relative humidity errors in the upper convective boundary layer that affect aerosol water content, secondary organic aerosols that were not yet included in the model, and uncertainties in the primary particulate emission rates. The current model was run in a predictive mode and demonstrates the challenges of accurately simulating all of the meteorological, chemical, and aerosol parameters over urban to regional scales that can affect aerosol radiative forcing.

  13. Effect of aerosol subgrid variability on aerosol optical depth and cloud condensation nuclei: implications for global aerosol modelling

    NASA Astrophysics Data System (ADS)

    Weigum, Natalie; Schutgens, Nick; Stier, Philip

    2016-11-01

    A fundamental limitation of grid-based models is their inability to resolve variability on scales smaller than a grid box. Past research has shown that significant aerosol variability exists on scales smaller than these grid boxes, which can lead to discrepancies in simulated aerosol climate effects between high- and low-resolution models. This study investigates the impact of neglecting subgrid variability in present-day global microphysical aerosol models on aerosol optical depth (AOD) and cloud condensation nuclei (CCN). We introduce a novel technique to isolate the effect of aerosol variability from other sources of model variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model. We compare WRF-Chem (Weather and Research Forecast model) runs in which aerosol and gases are simulated at 80 km and again at 10 km resolutions; in both simulations the other model components, such as meteorology and dynamics, are kept at the 10 km baseline resolution. We find that AOD is underestimated by 13 % and CCN is overestimated by 27 % when aerosol and gases are simulated at 80 km resolution compared to 10 km. The processes most affected by neglecting aerosol subgrid variability are gas-phase chemistry and aerosol uptake of water through aerosol-gas equilibrium reactions. The inherent non-linearities in these processes result in large changes in aerosol properties when aerosol and gaseous species are artificially mixed over large spatial scales. These changes in aerosol and gas concentrations are exaggerated by convective transport, which transports these altered concentrations to altitudes where their effect is more pronounced. These results demonstrate that aerosol variability can have a large impact on simulating aerosol climate effects, even when meteorology and dynamics are held constant. Future aerosol model development should focus on accounting for the effect of subgrid variability on these

  14. A smog chamber study coupling a photoionization aerosol electron/ion spectrometer to VUV synchrotron radiation: organic and inorganic-organic mixed aerosol analysis

    NASA Astrophysics Data System (ADS)

    Baeza-Romero, María Teresa; Gaie-Levrel, Francois; Mahjoub, Ahmed; López-Arza, Vicente; Garcia, Gustavo A.; Nahon, Laurent

    2016-07-01

    A reaction chamber was coupled to a photoionization aerosol time-of-flight mass spectrometer based on an electron/ion coincidence scheme and applied for on-line analysis of organic and inorganic-organic mixed aerosols using synchrotron tunable vacuum ultraviolet (VUV) photons as the ionization source. In this proof of principle study, both aerosol and gas phase were detected simultaneously but could be differentiated. Present results and perspectives for improvement for this set-up are shown in the study of ozonolysis ([O3] = 0.13-3 ppm) of α-pinene (2-3 ppm), and the uptake of glyoxal upon ammonium sulphate. In this work the ozone concentration was monitored in real time, together with the particle size distributions and chemical composition, the latter taking advantage of the coincidence spectrometer and the tuneability of the synchrotron radiation as a soft VUV ionization source.

  15. Aerosol simulation applying high resolution anthropogenic emissions with the EMAC chemistry-climate model

    NASA Astrophysics Data System (ADS)

    Pozzer, A.; de Meij, A.; Pringle, K. J.; Tost, H.; Doering, U. M.; van Aardenne, J.; Lelieveld, J.

    2011-09-01

    The new high resolution global anthropogenic emission inventory (EDGAR-CIRCE) of gas and aerosol pollutants has been incorporated in the chemistry general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). A high horizontal resolution simulation is performed for the years 2005-2008 to evaluate the capability of the model and the emissions to reproduce observed aerosol concentrations and aerosol optical depth (AOD) values. Model output is compared with observations from different measurement networks (CASTNET, EMEP and EANET) and AODs from remote sensing instruments (MODIS and MISR). The model reproduces the main spatial and temporal atmospheric features of the sulfate, ammonium and nitrate aerosol distributions. A good spatial agreement of the distribution of sulfate and ammonium aerosol is found when compared to observations, while calculated nitrate aerosol concentrations show some discrepancies. The simulated temporal development of the inorganic aerosols is in line with measurements of sulfate and nitrate aerosol, while for ammonium aerosol some deviations from observations occur over the USA. The calculated AODs agree well with the satellite observations in most regions, while a negative bias is found for the equatorial area and in the dust outflow regions (i.e. Central Atlantic and Northern Indian Ocean), due to an underestimation of biomass burning and aeolian dust emissions, respectively.

  16. The influence of meteorology on the organic and inorganic properties of aerosols in Hong Kong

    NASA Astrophysics Data System (ADS)

    Zheng, Mei; Guo, Zhigang; Fang, Ming; Kester, Dana R.

    2007-06-01

    The organic and inorganic species in total suspended particulates (TSP) collected from June to December in 1998 in Hong Kong were identified by gas chromatography-mass spectrometry (GC-MS) and inductively coupled plasma-mass spectrometry (ICP-MS) to investigate the sources of Hong Kong aerosols and the mechanisms that control the chemical compositions and variations in the atmosphere. These samples were classified according to the climate: wet, dry under the influence of southerly winds from the sea (Dry-S) and dry under the influence of northerly winds from the continent (Dry-N). There were significant increases of materials from crustal, biogenic and pollution sources in the Dry-N period by a factor of 5, 4, and 2, respectively. Since the crustal tracers (e.g., Al, Fe) could be from coal flyash, the estimate of crustal material in the Dry-N period may include some materials from pollution source. Therefore, a positive correlation between crustal and pollution elements was observed. From the analysis of solvent-extractable organics (SEOC), microbial and meat cooking sources showed slight increase (1.2-fold). Higher levels of plant wax materials in the Dry-N period were probably due to the higher wind speed during the winter monsoon. The percentage of crustal material in TSP was 47% in the Dry-N period, and only 22% in the wet season and the Dry-S period. Plant wax materials (biogenic source) had a higher percentage in the Dry-N period (39% of SEOC) while microbial and meat cooking sources accounted for 49% of SEOC in the wet season. This study revealed that wind direction and precipitation had a significant influence not only on the concentrations but also on the chemical compositions and sources of Hong Kong aerosols.

  17. Modeling aerosol-water interactions in subsaturated and supersaturated environments

    NASA Astrophysics Data System (ADS)

    Fountoukis, Christos

    The current dissertation is motivated by the need for an improved understanding of aerosol - water interactions both in subsaturated and supersaturated atmospheric conditions with a strong emphasis on air pollution and climate change modeling. A cloud droplet formation parameterization was developed to (i) predict droplet formation from a lognormal representation of aerosol size distribution and composition, and, (ii) include a size-dependant mass transfer coefficient for the growth of water droplets which explicitly accounts for the impact of organics on droplet growth kinetics. The parameterization unravels most of the physics of droplet formation and is in remarkable agreement with detailed numerical parcel model simulations, even for low values of the accommodation coefficient. The parameterization offers a much needed rigorous and computationally inexpensive framework for directly linking complex chemical effects on aerosol activation in global climate models. The new aerosol activation parameterization was also tested against observations from highly polluted clouds (within the vicinity of power plant plumes). Remarkable closure was achieved (much less than the 20% measurement uncertainty). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America. Aerosol-water interactions in ambient relative humidities less than 100% were studied using a thermodynamic equilibrium model for inorganic aerosol and a three dimensional air quality model. We developed a new thermodynamic equilibrium model, ISORROPIA-II, which predicts the partitioning of semi-volatiles and the phase state of K+/Ca2+/M g2+ /NH4+/Na+/SO4 2-/NO3-/Cl-/H2O aerosols. A comprehensive evaluation of its performance was conducted over a wide range of atmospherically relevant

  18. Characterization of water-soluble inorganic ions in size-segregated aerosols in coastal city, Xiamen

    NASA Astrophysics Data System (ADS)

    Zhao, Jinping; Zhang, Fuwang; Xu, Ya; Chen, Jinsheng

    2011-03-01

    The samples of water-soluble inorganic ions (WSIs), including anions (F-, Cl-, SO42-, NO3-) and cations (NH4+, K+, Na+, Ca2+, Mg2+) in 8 size-segregated particle matter (PM), were collected using a sampler (with 8 nominal cut-sizes ranged from 0.43 to 9.0 μm) from October 2008 to September 2009 at five sites in both polluted and background regions of a coastal city, Xiamen. The results showed that particulate matters in the fine mode (PM2.1, Dp < 2.1 μm) comprised large part of mass concentrations of aerosols, which accounted for 45.56-51.27%, 40.04-60.81%, 42.02-60.81%, and 40.46-57.07% of the total particulate mass in spring, summer, autumn, and winter, respectively. The water-soluble ionic species in the fine mode at five sampling sites varied from 15.33 to 33.82 (spring), 14.03 to 28.06 (summer), 33.47 to 72.52 (autumn), and 48.39 to 69.75 μg m- 3 (winter), respectively, which accounted for 57.30 ± 6.51% of the PM2.1 mass concentrations. Secondary pollutants of NH4+, SO42- and NO3- were the dominant contributors of WSIs, which suggested that pollutants from anthropogenic activities, such as SO2, NOx were formed in aerosols by photochemical reactions. The size distributions of Na+, Cl-, SO42- and NO3- were bimodal, peaking at 0.43-0.65 μm and 3.3-5.8 μm. Although some ions, such as NH4+ presented bimodal distributions, the coarse mode was insignificant compared to the fine mode. Ca2+ and Mg2+ exhibited unimodal distributions at all sampling sites, peaking at 2.1-3.3 μm, while K+ having a bimodal distributions with a major peak at 0.43-0.65 μm and a minor one at 3.3-4.7 μm, were used in most of samples. Seasonal and spatial variations in the size-distribution profiles suggested that meteorological conditions (seasonal patterns) and sampling locations (geographical patterns) were the main factors determining the formation of secondary aerosols and characteristics of size distributions for WSIs.

  19. Characteristics of Water-Soluble Inorganic Ions in Aerosol Particles in Jingjinji-Mega Typical Cities

    NASA Astrophysics Data System (ADS)

    Wang, Li

    2013-06-01

    Aerosol has important effects on climate, environment and human health and water-soluble ions are important chemical composition in aerosol. It is important to study concentration levels, sources and size distributions of water-soluble ions in aerosol. In recent years, with the increasing of energy consumption and the amount of automobile, regional pollution has become more serious in Beijing-Tianjin-Hebei Region. Especially since the haze happened frequently in Beijing-Tianjin-Hebei Region, it is an imminent study about water-soluble ions in aerosol.To investigate the concentration levels, sources and size distributions of water soluble inorganic ions (WSI), size-segregated aerosol samples were collected using Andersen cascade sampler from Aug2010to Aug2011in Beijing, Tianjin, Tangshan and Baoding. The WSI were analyzed by ion chromatography(IC).The results indicated that the order of total WSI (TWSI) concentration of TSP in the region was Tianjin-Baoding-Beijing-Tangshan. The order of TWSI of the fine particles in the region was Baoding-Tianjin-Beijing-Tangshan. The annual mean concentrations of TWSI in the coarse mode were 41.36±15.76,48.04±15.79,39.40±11.03,40.49±13.32μg m-3in Beijing, Tianjin, Tangshan and Baoding, respectively. The annual mean concentrations of TWSI in the fine mode were 66.54±47.95,69.12±34.85, 61.80±44.63,71.73±45.12μg m-3in Beijing, Tianjin, Tangshan and Baoding, respectively. All the annual mean concentrations of TWSIin the fine mode in the four sites had exceeded averaged concentration of PM2.5in the environmental quality standards (35μg m-3), which indicated that the pollution of TWSI was serious. Secondary water-soluble ions (SWSI)(SO42-, NO3-and NH4+) and Cl-were the main components, and were mainly found in the fine particles in the four sites of Beijing-Tianjin-Hebei Region. In the coarse particles, NO3-Ca2+ and SO42-were the dominant contributions to WSI. Almost all water-soluble ions in fine particles are similar

  20. A Study of Stratospheric Aerosols and Their Effect on Inorganic Chlorine Partitioning Using Balloon, In Situ, and Satellite Observations

    NASA Technical Reports Server (NTRS)

    Osterman, G. B.; Salawitch, R. J.; Sen, B.; Toon, G. C.

    1999-01-01

    Heterogeneous reactions on the surface of aerosols lead to a decrease in the concentration of nitrogen radicals and an increase in the concentration of chlorine and hydrogen radical species. As a consequence, enhanced sulfate aerosol levels in the lower stratosphere resulting from volcanic eruptions lead to lower concentrations of ozone due to more rapid loss by chlorine and hydrogen radicals. This study focuses on continuing the effort to quantify the effect of sulfate aerosols on the partitioning of inorganic chlorine species at midlatitudes. The study begins with an examination of balloon-borne measurements of key chlorine species obtained by the JPL MkIV interferometer for different aerosol loading conditions. A detailed comparison of the response of HCl to variations in aerosol surface area observed by MkIV, ER-2 instruments, HALOE, and ATMOS is carried out by examining HCl vs CH4 correlation diagrams, since CH4 is the only tracer measured on each platform. Finally, the consistency between theory and observed changes in ClO and HCl due to variations in aerosol surface area is examined.

  1. Condensing Organic Aerosols in a Microphysical Model

    NASA Astrophysics Data System (ADS)

    Gao, Y.; Tsigaridis, K.; Bauer, S.

    2015-12-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  2. Large-Scale Aerosol Modeling and Analysis

    DTIC Science & Technology

    2007-09-30

    to six days in advance anywhere on the globe. NAAPS and COAMPS are particularly useful for forecasts of dust storms in areas downwind of the large...in FY08. NAAPS forecasts of CONUS dust storms and long-range dust transport to CONUS were further evaluated in collaboration with CSU. These...visibility. The regional model ( COAMPS /Aerosol) became operational during OIF. The global model Navy Aerosol Analysis and Prediction System (NAAPS

  3. ATR-FTIR characterization of organic functional groups and inorganic ions in ambient aerosols at a rural site

    NASA Astrophysics Data System (ADS)

    Coury, Charity; Dillner, Ann M.

    An Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR) spectroscopic method was used to measure organic functional groups and inorganic ions at Tonto National Monument (TNM), an Interagency Monitoring of Protected Visual Environments (IMPROVE) sampling site in a rural area near Phoenix, Arizona. Functional groups and ions from common aerosol compound classes such as aliphatic and aromatic CH, methylene, methyl, aldehydes/ketones, carboxylic acids, ammonium sulfate and nitrate as well as functional groups from difficult to measure compound classes such as esters/lactones, acid anhydrides, carbohydrate hydroxyl and ethers, amino acids, and amines were quantified. On average, ˜33% of the PM 1.0 mass was composed of organic aerosol. The average (standard deviation) composition of the organic aerosol at TNM was 34% (6%) biogenic functional groups, 21% (5%) oxygenated functional groups, 28% (7%) aliphatic hydrocarbon functional groups (aliphatic CH, methylene and methyl) and 17% (1%) aromatic hydrocarbon functional groups. Compositional analysis, functional group correlations, and back trajectories were used to identify three types of events with source signatures: primary biogenic-influenced, urban-influenced, and regional background. The biogenic-influenced event had high concentrations of amino acids and carbohydrate hydroxyl and ether, as well as aliphatic CH and aromatic CH functional groups and qualitatively high levels of silicate. The urban-influenced events had back trajectories traveling directly from the Phoenix area and high concentrations of hydrocarbons, oxygenated functional groups, and inorganic ions. This aerosol characterization suggests that both primary emissions in Phoenix and secondary formation of aerosols from Phoenix emissions had a major impact on the aerosol composition and concentration at TNM. The regional background source had low concentrations of all functional groups, but had higher concentrations of biogenic functional

  4. Model analysis of influences of aerosol mixing state upon its optical properties in East Asia

    NASA Astrophysics Data System (ADS)

    Han, Xiao; Zhang, Meigen; Zhu, Lingyun; Xu, Liren

    2013-07-01

    The air quality model system RAMS (Regional Atmospheric Modeling System)-CMAQ (Models-3 Community Multi-scale Air Quality) coupled with an aerosol optical/radiative module was applied to investigate the impact of different aerosol mixing states (i.e., externally mixed, half externally and half internally mixed, and internally mixed) on radiative forcing in East Asia. The simulation results show that the aerosol optical depth (AOD) generally increased when the aerosol mixing state changed from externally mixed to internally mixed, while the single scattering albedo (SSA) decreased. Therefore, the scattering and absorption properties of aerosols can be significantly affected by the change of aerosol mixing states. Comparison of simulated and observed SSAs at five AERONET (Aerosol Robotic Network) sites suggests that SSA could be better estimated by considering aerosol particles to be internally mixed. Model analysis indicates that the impact of aerosol mixing state upon aerosol direct radiative forcing (DRF) is complex. Generally, the cooling effect of aerosols over East Asia are enhanced in the northern part of East Asia (Northern China, Korean peninsula, and the surrounding area of Japan) and are reduced in the southern part of East Asia (Sichuan Basin and Southeast China) by internal mixing process, and the variation range can reach ±5 W m-2. The analysis shows that the internal mixing between inorganic salt and dust is likely the main reason that the cooling effect strengthens. Conversely, the internal mixture of anthropogenic aerosols, including sulfate, nitrate, ammonium, black carbon, and organic carbon, could obviously weaken the cooling effect.

  5. Modeling of secondary organic aerosols from mobile sources in Mexico City

    NASA Astrophysics Data System (ADS)

    Zavala, M.; Lei, W.; Bei, N.; Li, G.; Tsimpidi, A. P.; Karydis, V. A.; Pandis, S.; Molina, L. T.

    2009-04-01

    Mobile sources are significant contributors of emissions of CO, NOx, hydrocarbons and particle matter (PM) that constitute critical precursors of ozone as well as secondary organic and inorganic particles that decisively impact the photochemical levels and aerosol loadings in the atmosphere. Currently there are large uncertainties in regional air quality models during the treatment of aerosol formation from aerosol precursors via the production of condensable organic gases. As a result, the modeling of the concentrations and properties of aerosols resulted from mobile emissions sources is an important challenge. In this study we compare aerosol simulations using the PM-CAMx air quality model linked to the SAPRC99 chemical mechanism with measured aerosol data obtained during the MILAGRO/MCMA-2006 field campaign in Mexico City. The PM-CAMx modeling framework is based on the volatility-basis approach: both primary and secondary organic components are assumed to be photochemically reactive and are logarithmically distributed in volatility bins. The distinction of the volatility properties of aerosols precursors is particularly important for diesel and gasoline emission sources due to their different organic carbon speciation emissions profiles. Using this volatility-basis technique, we will present results on the relative contributions from both gasoline and diesel vehicle fleet emission sources to the formation of secondary organic aerosols in an urban area.

  6. Mesoscale Modeling of the Atmosphere and Aerosols

    DTIC Science & Technology

    2000-09-30

    fires, or the dynamical and topographical forcing is small-scale, as in dust storms . A high-resolution COAMPS is needed to simulate the first stages of...context. However, the tightly coupled application is practical only for dynamically driven aerosols (e.g. dust storms ) or for planned (e.g. known...an imbedded aerosol module for COAMPS for use in the design and evaluation of techniques for coupling off-line transport and dispersion models to

  7. Ammonia concentrations and modeling of inorganic particulate matter in the vicinity of an egg production facility in Southeastern USA.

    PubMed

    Li, Qian-Feng; Wang-Li, Lingjuan; Shah, Sanjay B; Jayanty, R K M; Bloomfield, Peter

    2014-03-01

    Ammonia (NH3) is an important base gas and can react with acidic species to form atmospheric aerosols. Due to the rapid growth of poultry and swine production in the North Carolina Coastal Plain, atmospheric NH3 concentrations across the region have subsequently increased. Ammonia concentrations and inorganic particulate matter (PM) at four ambient stations in the vicinity of an egg production facility were measured for 1 year using PM2.5 speciation samplers with honeycomb denuders and ion chromatography (IC). Meanwhile, concentrations of NH3 and inorganic PM in one of the egg production houses were also simultaneously measured using a gas analyzer for NH3 and the filter pack plus IC method for inorganic PM. An equilibrium model-ISORROPIA II was applied to predict the behavior of inorganic aerosols in response to precursor gas concentrations and environmental parameters. Average ambient NH3 concentrations varied from 10.0 to 27.0 μg/m(3), and they were negatively correlated with the distances from the ambient location to the nearest egg production house exhausts. Ambient NH3 concentrations were higher in warm seasons than in cold seasons. Measured NH3 concentrations agreed well with ISORROPIA II model predictions at all sampling stations. For the ambient stations, there was a good agreement in particle phase NH4 (+) between the model simulation and observations. For the in-house station, the model simulation was applied to correct the overestimation of particle phase NH4 (+) due to gas phase NH3 breaking through the denuders. Changes in SO4 (2-), NO3 (-), and Cl(-) yield proportional changes in inorganic PM mass. Due to the abundance of NH3 gas in the vicinity area of the monitored farm, changes in NH3 concentrations had a small effect on inorganic PM mass. Aerosol equilibrium modeling may be used to assess the influence of precursor gas concentrations on inorganic PM formation when the measurements for some species are unavailable.

  8. Individual Aerosol Particles from Biomass Burning in Southern Africa Compositions and Aging of Inorganic Particles. 2; Compositions and Aging of Inorganic Particles

    NASA Technical Reports Server (NTRS)

    Li, Jia; Posfai, Mihaly; Hobbs, Peter V.; Buseck, Peter R.

    2003-01-01

    Individual aerosol particles collected over southern Africa during the SAFARI 2000 field study were studied using transmission electron microscopy and field-emission scanning electron microscopy. The sizes, shapes, compositions, mixing states, surface coatings, and relative abundances of aerosol particles from biomass burning, in boundary layer hazes, and in the free troposphere were compared, with emphasis on aging and reactions of inorganic smoke particles. Potassium salts and organic particles were the predominant species in the smoke, and most were internally mixed. More KCl particles occur in young smoke, whereas more K2SO4 and KNO3 particles were present in aged smoke. This change indicates that with the aging of the smoke, KCl particles from the fires were converted to K2SO4 and KNO3 through reactions with sulfur- and nitrogen- bearing species from biomass burning as well as other sources. More soot was present in smoke from flaming grass fires than bush and wood fires, probably due to the predominance of flaming combustion in grass fires. The high abundance of organic particles and soluble salts can affect the hygroscopic properties of biomass-burning aerosols and therefore influence their role as cloud condensation nuclei. Particles from biomass burning were important constituents of the regional hazes.

  9. Measured and Modeled Humidification Factors of Fresh Smoke Particles From Biomass Burning: Role of Inorganic Constituents

    SciTech Connect

    Hand, Jenny L.; Day, Derek E.; McMeeking, Gavin M.; Levin, Ezra; Carrico, Christian M.; Kreidenweis, Sonia M.; Malm, William C.; Laskin, Alexander; Desyaterik, Yury

    2010-07-09

    During the 2006 FLAME study (Fire Laboratory at Missoula Experiment), laboratory burns of biomass fuels were performed to investigate the physico-chemical, optical, and hygroscopic properties of fresh biomass smoke. As part of the experiment, two nephelometers simultaneously measured dry and humidified light scattering coefficients (bsp(dry) and bsp(RH), respectively) in order to explore the role of relative humidity (RH) on the optical properties of biomass smoke aerosols. Results from burns of several biomass fuels showed large variability in the humidification factor (f(RH) = bsp(RH)/bsp(dry)). Values of f(RH) at RH=85-90% ranged from 1.02 to 2.15 depending on fuel type. We incorporated measured chemical composition and size distribution data to model the smoke hygroscopic growth to investigate the role of inorganic and organic compounds on water uptake for these aerosols. By assuming only inorganic constituents were hygroscopic, we were able to model the water uptake within experimental uncertainty, suggesting that inorganic species were responsible for most of the hygroscopic growth. In addition, humidification factors at 85-90% RH increased for smoke with increasing inorganic salt to carbon ratios. Particle morphology as observed from scanning electron microscopy revealed that samples of hygroscopic particles contained soot chains either internally or externally mixed with inorganic potassium salts, while samples of weak to non-hygroscopic particles were dominated by soot and organic constituents. This study provides further understanding of the compounds responsible for water uptake by young biomass smoke, and is important for accurately assessing the role of smoke in climate change studies and visibility regulatory efforts.

  10. Measured and modeled humidification factors of fresh smoke particles from biomass burning: role of inorganic constituents

    NASA Astrophysics Data System (ADS)

    Hand, J. L.; Day, D. E.; McMeeking, G. M.; Levin, E. J. T.; Carrico, C. M.; Kreidenweis, S. M.; Malm, W. C.; Laskin, A.; Desyaterik, Y.

    2010-02-01

    During the 2006 FLAME study (Fire Laboratory at Missoula Experiment), laboratory burns of biomass fuels were performed to investigate the physico-chemical, optical, and hygroscopic properties of fresh biomass smoke. As part of the experiment, two nephelometers simultaneously measured dry and humidified light scattering coefficients (bsp(dry) and bsp(RH), respectively) in order to explore the role of relative humidity (RH) on the optical properties of biomass smoke aerosols. Results from burns of several biomass fuels showed large variability in the humidification factor (f(RH)=bsp(RH)/bsp(dry)). Values of f(RH) at RH=85-90% ranged from 1.02 to 2.15 depending on fuel type. We incorporated measured chemical composition and size distribution data to model the smoke hygroscopic growth to investigate the role of inorganic and organic compounds on water uptake for these aerosols. By assuming only inorganic constituents were hygroscopic, we were able to model the water uptake within experimental uncertainty, suggesting that inorganic species were responsible for most of the hygroscopic growth. In addition, humidification factors at 85-90% RH increased for smoke with increasing inorganic salt to carbon ratios. Particle morphology as observed from scanning electron microscopy revealed that samples of hygroscopic particles contained soot chains either internally or externally mixed with inorganic potassium salts, while samples of weak to non-hygroscopic particles were dominated by soot and organic constituents. This study provides further understanding of the compounds responsible for water uptake by young biomass smoke, and is important for accurately assessing the role of smoke in climate change studies and visibility regulatory efforts.

  11. Measured and modeled humidification factors of fresh smoke particles from biomass burning: role of inorganic constituents

    NASA Astrophysics Data System (ADS)

    Hand, J. L.; Day, D. E.; McMeeking, G. M.; Levin, E. J. T.; Carrico, C. M.; Kreidenweis, S. M.; Malm, W. C.; Laskin, A.; Desyaterik, Y.

    2010-07-01

    During the 2006 FLAME study (Fire Laboratory at Missoula Experiment), laboratory burns of biomass fuels were performed to investigate the physico-chemical, optical, and hygroscopic properties of fresh biomass smoke. As part of the experiment, two nephelometers simultaneously measured dry and humidified light scattering coefficients (bsp(dry) and bsp(RH), respectively) in order to explore the role of relative humidity (RH) on the optical properties of biomass smoke aerosols. Results from burns of several biomass fuels from the west and southeast United States showed large variability in the humidification factor (f(RH)=bsp(RH)/bsp(dry)). Values of f(RH) at RH=80-85% ranged from 0.99 to 1.81 depending on fuel type. We incorporated measured chemical composition and size distribution data to model the smoke hygroscopic growth to investigate the role of inorganic compounds on water uptake for these aerosols. By assuming only inorganic constituents were hygroscopic, we were able to model the water uptake within experimental uncertainty, suggesting that inorganic species were responsible for most of the hygroscopic growth. In addition, humidification factors at 80-85% RH increased for smoke with increasing inorganic salt to carbon ratios. Particle morphology as observed from scanning electron microscopy revealed that samples of hygroscopic particles contained soot chains either internally or externally mixed with inorganic potassium salts, while samples of weak to non-hygroscopic particles were dominated by soot and organic constituents. This study provides further understanding of the compounds responsible for water uptake by young biomass smoke, and is important for accurately assessing the role of smoke in climate change studies and visibility regulatory efforts.

  12. Modelling Aerosol Dispersion in Urban Street Canyons

    NASA Astrophysics Data System (ADS)

    Tay, B. K.; Jones, D. P.; Gallagher, M. W.; McFiggans, G. B.; Watkins, A. P.

    2009-04-01

    Flow patterns within an urban street canyon are influenced by various micrometeorological factors. It also represents an environment where pollutants such as aerosols accumulate to high levels due to high volumes of traffic. As adverse health effects are being attributed to exposure to aerosols, an investigation of the dispersion of aerosols within such environments is of growing importance. In particular, one is concerned with the vertical structure of the aerosol concentration, the ventilation characteristics of the street canyon and the influence of aerosol microphysical processes. Due to the inherent heterogeneity of the aerosol concentrations within the street canyon and the lack of spatial resolution of measurement campaigns, these issues are an on-going debate. Therefore, a modelling tool is required to represent aerosol dispersion patterns to provide insights to results of past measurement campaigns. Computational Fluid Dynamics (CFD) models are able to predict detailed airflow patterns within urban geometries. This capability may be further extended to include aerosol dispersion, by an Euler-Euler multiphase approach. To facilitate the investigation, a two-dimensional, multiphase CFD tool coupled with the k-epsilon turbulence model and with the capability of modelling mixed convection flow regimes arising from both wind driven flows and buoyancy effects from heated walls was developed. Assuming wind blowing perpendicularly to the canyon axis and treating aerosols as a passive scalar, an attempt will be made to assess the sensitivities of aerosol vertical structure and ventilation characteristics to the various flow conditions. Numerical studies were performed using an idealized 10m by 10m canyon to represent a regular canyon and 10m by 5m to represent a deep one. An aerosol emission source was assigned on the centerline of the canyon to represent exhaust emissions. The vertical structure of the aerosols would inform future directives regarding the

  13. Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

    SciTech Connect

    Roldin, P.; Eriksson, A. C.; Nordin, E. Z.; Hermansson, E.; Mogensen, Ditte; Rusanen, A.; Boy, Michael; Swietlicki, E.; Svenningsson, Birgitta; Zelenyuk, Alla; Pagels, J.

    2014-08-11

    We have developed the novel Aerosol Dynamics, gas- and particle- phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas phase Master Chemical Mechanism version 3.2, an aerosol dynamics and particle phase chemistry module (which considers acid catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study: 1) the mass transfer limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), 2) the slow and almost particle size independent evaporation of α-pinene secondary organic aerosol (SOA) particles, and 3) the influence of chamber wall effects on the observed SOA formation in smog chambers.

  14. Synergetic formation of secondary inorganic and organic aerosol: effect of SO2 and NH3 on particle formation and growth

    NASA Astrophysics Data System (ADS)

    Chu, Biwu; Zhang, Xiao; Liu, Yongchun; He, Hong; Sun, Yele; Jiang, Jingkun; Li, Junhua; Hao, Jiming

    2016-11-01

    The effects of SO2 and NH3 on secondary organic aerosol formation have rarely been investigated together, while the interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain. Here we studied the effects of SO2 and NH3 on secondary aerosol formation in the photooxidation system of toluene/NOx in the presence or absence of Al2O3 seed aerosols in a 2 m3 smog chamber. The presence of SO2 increased new particle formation and particle growth significantly, regardless of whether NH3 was present. Sulfate, organic aerosol, nitrate, and ammonium were all found to increase linearly with increasing SO2 concentrations. The increases in these four species were more obvious under NH3-rich conditions, and the generation of nitrate, ammonium, and organic aerosol increased more significantly than sulfate with respect to SO2 concentration, while sulfate was the most sensitive species under NH3-poor conditions. The synergistic effects between SO2 and NH3 in the heterogeneous process contributed greatly to secondary aerosol formation. Specifically, the generation of NH4NO3 was found to be highly dependent on the surface area concentration of suspended particles, and increased most significantly with SO2 concentration among the four species under NH3-rich conditions. Meanwhile, the absorbed NH3 might provide a liquid surface layer for the absorption and subsequent reaction of SO2 and organic products and, therefore, enhance sulfate and secondary organic aerosol (SOA) formation. This effect mainly occurred in the heterogeneous process and resulted in a significantly higher growth rate of seed aerosols compared to without NH3. By applying positive matrix factorisation (PMF) analysis to the AMS data, two factors were identified for the generated SOA. One factor, assigned to less-oxidised organic aerosol and some oligomers, increased with increasing SO2 under NH3-poor conditions, mainly due to the well-known acid catalytic effect of

  15. Size distributions of nano/micron dicarboxylic acids and inorganic ions in suburban PM episode and non-episodic aerosol

    NASA Astrophysics Data System (ADS)

    Hsieh, Li-Ying; Kuo, Su-Ching; Chen, Chien-Lung; Tsai, Ying I.

    The distribution of nano/micron dicarboxylic acids and inorganic ions in size-segregated suburban aerosol of southern Taiwan was studied for a PM episode and a non-episodic pollution period, revealing for the first time the distribution of these nanoscale particles in suburban aerosols. Inorganic species, especially nitrate, were present in higher concentrations during the PM episode. A combination of gas-to-nuclei conversion of nitrate particles and accumulation of secondary photochemical products originating from traffic-related emissions was likely a crucial cause of the PM episode. Sulfate, ammonium, and oxalic acid were the dominant anion, cation, and dicarboxylic acid, respectively, accounting for a minimum of 49% of the total anion, cation or dicarboxylic acid mass. Peak concentrations of these species occurred at 0.54 μm in the droplet mode during both non-episodic and PM episode periods, indicating an association with cloud-processed particles. On average, sulfate concentration was 16-17 times that of oxalic acid. Oxalic acid was nevertheless the most abundant dicarboxylic acid during both periods, followed by succinic, malonic, maleic, malic and tartaric acid. The mass median aerodynamic diameter (MMAD) of oxalic acid was 0.77 μm with a bi-modal presence at 0.54 μm and 18 nm during non-episodic pollution and an MMAD of 0.67 μm with mono-modal presence at 0.54 μm in PM episode aerosol. The concomitant formation of malonic acid and oxalic acid was attributed to in-cloud processes. During the PM episode in the 5-100 nm nanoscale range, an oxalic acid/sulfate mass ratio of 40.2-82.3% suggested a stronger formation potential for oxalic acid than for sulfate in the nuclei mode. For total cations (TC), total inorganic anions (TIA) and total dicarboxylic acids (TDA), major contributing particles were in the droplet mode, with least in the nuclei mode. The ratio of TDA to TIA in the nuclei mode increased greatly from 8.40% during the non-episodic pollution

  16. Chemical composition and acidity of size-fractionated inorganic aerosols of 2013-14 winter haze in Shanghai and associated health risk of toxic elements

    NASA Astrophysics Data System (ADS)

    Behera, Sailesh N.; Cheng, Jinping; Huang, Xian; Zhu, Qiongyu; Liu, Ping; Balasubramanian, Rajasekhar

    2015-12-01

    The severe winter haze episode that occurred in Shanghai from December 2013 to January 2014, characterized by elevated levels of particulate matter (PM), received considerable international attention because of its impacts on public health and disruption of day-to-day activities. To examine the characteristics of PM during this haze episode and to assess the chemistry behind formation of secondary inorganic aerosols (SIA) and associated health impacts due to exposure of toxic elements, we characterized eight water soluble inorganic (WSI) ions and twenty four trace elements in twelve size-fractionated PM (10 nm-9.9 μm). The average mass concentrations of coarse (1.8 μm < Dp < 9.9 μm), fine (Dp < 2.5 μm), ultrafine (0.01 μm < Dp < 0.10 μm) and nano (0.01 μm < Dp < 0.056 μm) particles during hazy days were 2.8, 5.2, 5.3 and 5.1 times higher than those during non-hazy days, respectively. The in-situ pH (pHIS), as predicted by the Aerosol Inorganic Model (AIM-IV) in all sizes of PM, was observed to be lower during hazy days (average of -0.64) than that during non-hazy days (average of -0.29); there was an increased acidity in haze aerosols. Based on the measured concentrations of particulate-bound toxic elements, health risk assessment was conducted, which revealed that the excess lifetime carcinogenic risk to individuals exposed to fine particles under haze events increased significantly (P < 0.05) to 69 ± 18 × 10-6 compared to non-hazy days (34 ± 10 × 10-6). The qualitative source attribution analysis suggested that the occurrence of haze could be due to a combination of increased emissions of PM from multiple anthropogenic sources followed by its accumulation under unfavourable meteorological conditions with lower mixing heights and less wind speeds and the formation of secondary aerosols.

  17. Physiologically Based Pharmacokinetic Model for Long-Circulating Inorganic Nanoparticles.

    PubMed

    Liang, Xiaowen; Wang, Haolu; Grice, Jeffrey E; Li, Li; Liu, Xin; Xu, Zhi Ping; Roberts, Michael S

    2016-02-10

    A physiologically based pharmacokinetic model was developed for accurately characterizing and predicting the in vivo fate of long-circulating inorganic nanoparticles (NPs). This model is built based on direct visualization of NP disposition details at the organ and cellular level. It was validated with multiple data sets, indicating robust inter-route and interspecies predictive capability. We suggest that the biodistribution of long-circulating inorganic NPs is determined by the uptake and release of NPs by phagocytic cells in target organs.

  18. Global Aerosol Optical Models and Lookup Tables for the New MODIS Aerosol Retrieval over Land

    NASA Technical Reports Server (NTRS)

    Levy, Robert C.; Remer, Loraine A.; Dubovik, Oleg

    2007-01-01

    Since 2000, MODIS has been deriving aerosol properties over land from MODIS observed spectral reflectance, by matching the observed reflectance with that simulated for selected aerosol optical models, aerosol loadings, wavelengths and geometrical conditions (that are contained in a lookup table or 'LUT'). Validation exercises have showed that MODIS tends to under-predict aerosol optical depth (tau) in cases of large tau (tau greater than 1.0), signaling errors in the assumed aerosol optical properties. Using the climatology of almucantur retrievals from the hundreds of global AERONET sunphotometer sites, we found that three spherical-derived models (describing fine-sized dominated aerosol), and one spheroid-derived model (describing coarse-sized dominated aerosol, presumably dust) generally described the range of observed global aerosol properties. The fine dominated models were separated mainly by their single scattering albedo (omega(sub 0)), ranging from non-absorbing aerosol (omega(sub 0) approx. 0.95) in developed urban/industrial regions, to neutrally absorbing aerosol (omega(sub 0) approx.90) in forest fire burning and developing industrial regions, to absorbing aerosol (omega(sub 0) approx. 0.85) in regions of savanna/grassland burning. We determined the dominant model type in each region and season, to create a 1 deg. x 1 deg. grid of assumed aerosol type. We used vector radiative transfer code to create a new LUT, simulating the four aerosol models, in four MODIS channels. Independent AERONET observations of spectral tau agree with the new models, indicating that the new models are suitable for use by the MODIS aerosol retrieval.

  19. Sea salt aerosols as a reactive surface for inorganic and organic acidic gases in the arctic troposphere

    NASA Astrophysics Data System (ADS)

    Chi, J. W.; Li, W. J.; Zhang, D. Z.; Zhang, J. C.; Lin, Y. T.; Shen, X. J.; Sun, J. Y.; Chen, J. M.; Zhang, X. Y.; Zhang, Y. M.; Wang, W. X.

    2015-06-01

    Sea salt aerosols (SSA) are dominant particles in the arctic atmosphere and determine the polar radiative balance. SSA react with acidic pollutants that lead to changes of physical and chemical properties of their surface, which in turn alter their hygroscopic and optical properties. Transmission electron microscopy with energy-dispersive X-ray spectrometry was used to analyze morphology, composition, size, and mixing state of individual SSA at Ny-Ålesund, Svalbard in summertime. Individual fresh SSA contained cubic NaCl coated by certain amounts of MgCl2 and CaSO4. Individual partially aged SSA contained irregular NaCl coated by a mixture of NaNO3, Na2SO4, Mg(NO3)2, and MgSO4. The comparison suggests the hydrophilic MgCl2 coating in fresh SSA likely intrigued the heterogeneous reactions at the beginning of SSA and acidic gases. Individual fully aged SSA normally had Na2SO4 cores and an amorphous coating of NaNO3. Elemental mappings of individual SSA particles revealed that as the particles ageing Cl gradually decreased but the C, N, O, and S content increased. 12C14N- mapping from nanoscale secondary ion mass spectrometry indicates that organic matter increased in the aged SSA compared with the fresh SSA. 12C14N- line scans further show that organic matter was mainly concentrated on the aged SSA surface. These new findings indicate that this mixture of organic matter and NaNO3 on particle surfaces determines their hygroscopic and optical properties. These abundant SSA, whose reactive surfaces absorb inorganic and organic acidic gases in the arctic troposphere, need to be incorporated into atmospheric chemical models.

  20. Sea salt aerosols as a reactive surface for inorganic and organic acidic gases in the Arctic troposphere

    NASA Astrophysics Data System (ADS)

    Chi, J. W.; Li, W. J.; Zhang, D. Z.; Zhang, J. C.; Lin, Y. T.; Shen, X. J.; Sun, J. Y.; Chen, J. M.; Zhang, X. Y.; Zhang, Y. M.; Wang, W. X.

    2015-10-01

    Sea salt aerosols (SSA) are dominant particles in the Arctic atmosphere and determine the polar radiative balance. SSA react with acidic pollutants that lead to changes in physical and chemical properties of their surface, which in turn alter their hygroscopic and optical properties. Transmission electron microscopy with energy-dispersive X-ray spectrometry was used to analyze morphology, composition, size, and mixing state of individual SSA at Ny-Ålesund, Svalbard, in summertime. Individual fresh SSA contained cubic NaCl coated by certain amounts of MgCl2 and CaSO4. Individual partially aged SSA contained irregular NaCl coated by a mixture of NaNO3, Na2SO4, Mg(NO3)2, and MgSO4. The comparison suggests the hydrophilic MgCl2 coating in fresh SSA likely intrigued the heterogeneous reactions at the beginning of SSA and acidic gases. Individual fully aged SSA normally had Na2SO4 cores and an amorphous coating of NaNO3. Elemental mappings of individual SSA particles revealed that as the particles ageing Cl gradually decreased, the C, N, O, and S content increased. 12C- mapping from nanoscale secondary ion mass spectrometry indicates that organic matter increased in the aged SSA compared with the fresh SSA. 12C- line scan further shows that organic matter was mainly concentrated on the aged SSA surface. These new findings indicate that this mixture of organic matter and NaNO3 on particle surfaces likely determines their hygroscopic and optical properties. These abundant SSA as reactive surfaces adsorbing inorganic and organic acidic gases can shorten acidic gas lifetime and influence the possible gaseous reactions in the Arctic atmosphere, which need to be incorporated into atmospheric chemical models in the Arctic troposphere.

  1. Optical Properties of Mixed Black Carbon, Inorganic and Secondary Organic Aerosols

    SciTech Connect

    Paulson, S E

    2012-05-30

    Summarizes the achievements of the project, which are divided into four areas: 1) Optical properties of secondary organic aerosols; 2) Development and of a polar nephelometer to measure aerosol optical properties and theoretical approaches to several optical analysis problems, 3) Studies on the accuracy of measurements of absorbing carbon by several methods, and 4) Environmental impacts of biodiesel.

  2. A Simple Model of Global Aerosol Indirect Effects

    SciTech Connect

    Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, K. J.; Carslaw, K. S.; Pierce, Jeffrey; Bauer, Susanne E.; Adams, P. J.

    2013-06-28

    Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth’s energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically-based model expresses the aerosol indirect effect using analytic representations of droplet nucleation, cloud and aerosol vertical structure, and horizontal variability in cloud water and aerosol concentration. Although the simple model is able to produce estimates of aerosol indirect effects that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates are found to be sensitive to several uncertain parameters, including the preindustrial cloud condensation nuclei concentration, primary and secondary anthropogenic emissions, the size of the primary particles, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Aerosol indirect effects are surprisingly linear in emissions. This simple model provides a much stronger physical basis for representing aerosol indirect effects than previous representations in integrated assessment models designed to quickly explore the parameter space of emissions-climate interactions. The model also produces estimates that depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models.

  3. Aerosol Models for the CALIPSO Lidar Inversion Algorithms

    NASA Technical Reports Server (NTRS)

    Omar, Ali H.; Winker, David M.; Won, Jae-Gwang

    2003-01-01

    We use measurements and models to develop aerosol models for use in the inversion algorithms for the Cloud Aerosol Lidar and Imager Pathfinder Spaceborne Observations (CALIPSO). Radiance measurements and inversions of the AErosol RObotic NETwork (AERONET1, 2) are used to group global atmospheric aerosols using optical and microphysical parameters. This study uses more than 105 records of radiance measurements, aerosol size distributions, and complex refractive indices to generate the optical properties of the aerosol at more 200 sites worldwide. These properties together with the radiance measurements are then classified using classical clustering methods to group the sites according to the type of aerosol with the greatest frequency of occurrence at each site. Six significant clusters are identified: desert dust, biomass burning, urban industrial pollution, rural background, marine, and dirty pollution. Three of these are used in the CALIPSO aerosol models to characterize desert dust, biomass burning, and polluted continental aerosols. The CALIPSO aerosol model also uses the coarse mode of desert dust and the fine mode of biomass burning to build a polluted dust model. For marine aerosol, the CALIPSO aerosol model uses measurements from the SEAS experiment 3. In addition to categorizing the aerosol types, the cluster analysis provides all the column optical and microphysical properties for each cluster.

  4. Simulations of Aerosol Microphysics in the NASA GEOS-5 Model

    NASA Technical Reports Server (NTRS)

    Colarco, Peter; Smith; Randles; daSilva

    2010-01-01

    Aerosol-cloud-chemistry interactions have potentially large but uncertain impacts on Earth's climate. One path to addressing these uncertainties is to construct models that incorporate various components of the Earth system and to test these models against data. To that end, we have previously incorporated the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) module online in the NASA Goddard Earth Observing System model (GEOS-5). GEOS-5 provides a platform for Earth system modeling, incorporating atmospheric and ocean general circulation models, a land surface model, a data assimilation system, and treatments of atmospheric chemistry and hydrologic cycle. Including GOCART online in this framework has provided a path for interactive aerosol-climate studies; however, GOCART only tracks the mass of aerosols as external mixtures and does not include the detailed treatments of aerosol size distribution and composition (internal mixtures) needed for aerosol-cloud-chemistry-climate studies. To address that need we have incorporated the Community Aerosol and Radiation Model for Atmospheres (CARMA) online in GEOS-5. CARMA is a sectional aerosol-cloud microphysical model, capable of treating both aerosol size and composition explicitly be resolving the aerosol distribution into a variable number of size and composition groupings. Here we present first simulations of dust, sea salt, and smoke aerosols in GEOS-5 as treated by CARMA. These simulations are compared to available aerosol satellite, ground, and aircraft data and as well compared to the simulated distributions in our current GOCART based system.

  5. Comparison of activity coefficient models for atmospheric aerosols containing mixtures of electrolytes, organics, and water

    NASA Astrophysics Data System (ADS)

    Tong, Chinghang; Clegg, Simon L.; Seinfeld, John H.

    Atmospheric aerosols generally comprise a mixture of electrolytes, organic compounds, and water. Determining the gas-particle distribution of volatile compounds, including water, requires equilibrium or mass transfer calculations, at the heart of which are models for the activity coefficients of the particle-phase components. We evaluate here the performance of four recent activity coefficient models developed for electrolyte/organic/water mixtures typical of atmospheric aerosols. Two of the models, the CSB model [Clegg, S.L., Seinfeld, J.H., Brimblecombe, P., 2001. Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds. Journal of Aerosol Science 32, 713-738] and the aerosol diameter dependent equilibrium model (ADDEM) [Topping, D.O., McFiggans, G.B., Coe, H., 2005. A curved multi-component aerosol hygroscopicity model framework: part 2—including organic compounds. Atmospheric Chemistry and Physics 5, 1223-1242] treat ion-water and organic-water interactions but do not include ion-organic interactions; these can be referred to as "decoupled" models. The other two models, reparameterized Ming and Russell model 2005 [Raatikainen, T., Laaksonen, A., 2005. Application of several activity coefficient models to water-organic-electrolyte aerosols of atmospheric interest. Atmospheric Chemistry and Physics 5, 2475-2495] and X-UNIFAC.3 [Erdakos, G.B., Change, E.I., Pandow, J.F., Seinfeld, J.H., 2006. Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water—Part 3: Organic compounds, water, and ionic constituents by consideration of short-, mid-, and long-range effects using X-UNIFAC.3. Atmospheric Environment 40, 6437-6452], include ion-organic interactions; these are referred to as "coupled" models. We address the question—Does the inclusion of a treatment of ion-organic interactions substantially improve the performance of the coupled models over

  6. Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

    2014-02-01

    Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability

  7. Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

    2014-08-01

    Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this

  8. Revisiting Aerosol Effects in Global Climate Models Using an Aerosol Lidar Simulator

    NASA Astrophysics Data System (ADS)

    Ma, P. L.; Chepfer, H.; Winker, D. M.; Ghan, S.; Rasch, P. J.

    2015-12-01

    Aerosol effects are considered a major source of uncertainty in global climate models and the direct and indirect radiative forcings have strong model dependency. These forcings are routinely evaluated (and calibrated) against observations, among them satellite retrievals are greatly used for their near-global coverage. However, the forcings calculated from model output are not directly comparable with those computed from satellite retrievals since sampling and algorithmic differences (such as cloud screening, noise reduction, and retrieval) between models and observations are not accounted for. It is our hypothesis that the conventional model validation procedures for comparing satellite observations and model simulations can mislead model development and introduce biases. Hence, we have developed an aerosol lidar simulator for global climate models that simulates the CALIOP lidar signal at 532nm. The simulator uses the same algorithms as those used to produce the "GCM-oriented CALIPSO Aerosol Product" to (1) objectively sample lidar signal profiles; and (2) derive aerosol fields (e.g., extinction profile, aerosol type, etc) from lidar signals. This allows us to sample and derive aerosol fields in the model and real atmosphere in identical ways. Using the Department of Energy's ACME model simulations, we found that the simulator-retrieved aerosol distribution and aerosol-cloud interactions are significantly different from those computed from conventional approaches, and that the model is much closer to satellite estimates than previously believed.

  9. Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements

    NASA Technical Reports Server (NTRS)

    Limbacher, J.; Patadia, F.; Petrenko, M.; Martin, M. Val; Chin, M.; Gaitley, B.; Garay, M.; Kalashnikova, O.; Nelson, D.; Scollo, S.

    2011-01-01

    As the aerosol products from the NASA Earth Observing System's Multi-angle Imaging SpectroRadiometer (MISR) mature, we are placing greater focus on ways of using the aerosol amount and type data products, and aerosol plume heights, to constrain aerosol transport models. We have demonstrated the ability to map aerosol air-mass-types regionally, and have identified product upgrades required to apply them globally, including the need for a quality flag indicating the aerosol type information content, that varies depending upon retrieval conditions. We have shown that MISR aerosol type can distinguish smoke from dust, volcanic ash from sulfate and water particles, and can identify qualitative differences in mixtures of smoke, dust, and pollution aerosol components in urban settings. We demonstrated the use of stereo imaging to map smoke, dust, and volcanic effluent plume injection height, and the combination of MISR and MODIS aerosol optical depth maps to constrain wildfire smoke source strength. This talk will briefly highlight where we stand on these application, with emphasis on the steps we are taking toward applying the capabilities toward constraining aerosol transport models, planet-wide.

  10. Analytic modeling of aerosol size distributions

    NASA Technical Reports Server (NTRS)

    Deepack, A.; Box, G. P.

    1979-01-01

    Mathematical functions commonly used for representing aerosol size distributions are studied parametrically. Methods for obtaining best fit estimates of the parameters are described. A catalog of graphical plots depicting the parametric behavior of the functions is presented along with procedures for obtaining analytical representations of size distribution data by visual matching of the data with one of the plots. Examples of fitting the same data with equal accuracy by more than one analytic model are also given.

  11. Optimized sparse-particle aerosol representations for modeling cloud-aerosol interactions

    NASA Astrophysics Data System (ADS)

    Fierce, Laura; McGraw, Robert

    2016-04-01

    Sparse representations of atmospheric aerosols are needed for efficient regional- and global-scale chemical transport models. Here we introduce a new framework for representing aerosol distributions, based on the method of moments. Given a set of moment constraints, we show how linear programming can be used to identify collections of sparse particles that approximately maximize distributional entropy. The collections of sparse particles derived from this approach reproduce CCN activity of the exact model aerosol distributions with high accuracy. Additionally, the linear programming techniques described in this study can be used to bound key aerosol properties, such as the number concentration of CCN. Unlike the commonly used sparse representations, such as modal and sectional schemes, the maximum-entropy moment-based approach is not constrained to pre-determined size bins or assumed distribution shapes. This study is a first step toward a new aerosol simulation scheme that will track multivariate aerosol distributions with sufficient computational efficiency for large-scale simulations.

  12. 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

  13. Mouse Model of Coxiella burnetii Aerosolization

    PubMed Central

    Melenotte, Cléa; Lepidi, Hubert; Nappez, Claude; Bechah, Yassina; Audoly, Gilles; Terras, Jérôme; Raoult, Didier

    2016-01-01

    Coxiella burnetii is mainly transmitted by aerosols and is responsible for multiple-organ lesions. Animal models have shown C. burnetii pathogenicity, but long-term outcomes still need to be clarified. We used a whole-body aerosol inhalation exposure system to mimic the natural route of infection in immunocompetent (BALB/c) and severe combined immunodeficient (SCID) mice. After an initial lung inoculum of 104 C. burnetii cells/lung, the outcome, serological response, hematological disorders, and deep organ lesions were described up to 3 months postinfection. C. burnetii-specific PCR, anti-C. burnetii immunohistochemistry, and fluorescent in situ hybridization (FISH) targeting C. burnetii-specific 16S rRNA completed the detection of the bacterium in the tissues. In BALB/c mice, a thrombocytopenia and lymphopenia were first observed, prior to evidence of C. burnetii replication. In all SCID mouse organs, DNA copies increased to higher levels over time than in BALB/c ones. Clinical signs of discomfort appeared in SCID mice, so follow-up had to be shortened to 2 months in this group. At this stage, all animals presented bone, cervical, and heart lesions. The presence of C. burnetii could be attested in situ for all organs sampled using immunohistochemistry and FISH. This mouse model described C. burnetii Nine Mile strain spread using aerosolization in a way that corroborates the pathogenicity of Q fever described in humans and completes previously published data in mouse models. C. burnetii infection occurring after aerosolization in mice thus seems to be a useful tool to compare the pathogenicity of different strains of C. burnetii. PMID:27160294

  14. Spatial and Temporal Variations of Aerosols Around Beijing in the Summer 2006: Model Evaluation and Source Apportionment

    SciTech Connect

    Matsui, Hitoshi; Koike, Makoto; Kondo, Yutaka; Takegawa, Nobuyuki; Kita, K.; Miyazaki, Y.; Hu, M.; Chang, S-Y; Blake, D. R.; Fast, Jerome D.; Zaveri, Rahul A.; Streets, D. G.; Zhang, Q.; Zhou, T.

    2009-08-15

    Regional aerosol model calculations were made using the WRF-CMAQ and WRF-chem models to study spatial and temporal variations of aerosols around Beijing, China, in August and September 2006 when the CAREBEIJING-2006 campaign was conducted. Model calculations were compared with in-situ observations made at the urban site in Beijing and suburb site in Yufa, which is 50 km to the south of Beijing. In general, the two model calculations reproduced features of temporal variations of meteorological parameters and concentrations of elemental carbon (EC) and inorganic aerosols (sulfate, ammonium, and nitrate). Spatial distributions of aerosol optical depth (AOD) obtained by the MODIS satellite sensor are also generally well reproduced. Model calculations show that enhancements in inorganic aerosol concentrations simultaneously observed at the two sites 4 to 5 times during the one-month observation period were resulted by accumulation of pollutants under stagnated air condition. Because Beijing is located at the north border the high anthropogenic emission area (the Great North China Plain), northward motion of air under the influence of anti-cyclone system caused enhancements in fine aerosol concentrations at Beijing. Concentrations of primary aerosols, such as EC, are found to be generally controlled by emissions within 100 km around Beijing within previous 24 hours. On the other hand, emissions as far as 500 km within previous 3 days were found to affect concentrations of secondary aerosols, such as sulfate. Because of significant contributions of secondary aerosols in Beijing, regional emission controls are found to be necessary for improvement of air quality in Beijing.

  15. Introducing the aerosol-climate model MAECHAM5-SAM2

    NASA Astrophysics Data System (ADS)

    Hommel, R.; Timmreck, C.; Graf, H. F.

    2009-04-01

    We are presenting a new global aerosol model MAECHAM5-SAM2 to study the aerosol dynamics in the UTLS under background and volcanic conditions. The microphysical core modul SAM2 treats the formation, the evolution and the transport of stratospheric sulphuric acid aerosol. The aerosol size distribution and the weight percentage of the sulphuric acid solution is calculated dependent on the concentrations of H2SO4 and H2O, their vapor pressures, the atmospheric temperature and pressure. The fixed sectional method is used to resolve an aerosol distribution between 1 nm and 2.6 micron in particle radius. Homogeneous nucleation, condensation and evaporation, coagulation, water-vapor growth, sedimentation and sulphur chemistry are included. The module is applied in the middle-atmosphere MAECHAM5 model, resolving the atmosphere up to 0.01 hPa (~80 km) in 39 layers. It is shown here that MAECHAM5-SAM2 well represents in-situ measured size distributions of stratospheric background aerosol in the northern hemisphere mid-latitudes. Distinct differences can be seen when derived integrated aerosol parameters (surface area, effective radius) are compared with aerosol climatologies based on the SAGE II satellite instrument (derived by the University of Oxford and the NASA AMES laboratory). The bias between the model and the SAGE II data increases as the moment of the aerosol size distribution decreases. Thus the modeled effective radius show the strongest bias, followed by the aerosol surface area density. Correspondingly less biased are the higher moments volume area density and the mass density of the global stratospheric aerosol coverage. This finding supports the key finding No. 2 of the SPARC Assessment of Stratospheric Aerosol Properties (2006), where it was shown that during periods of very low aerosol load in the stratosphere, the consistency between in-situ and satellite measurements, which exist in a volcanically perturbed stratosphere, breaks down and significant

  16. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect

    Richard A. Ferrare; David D. Turner

    2011-09-01

    Project goals: (1) Use the routine surface and airborne measurements at the ARM SGP site, and the routine surface measurements at the NSA site, to continue our evaluations of model aerosol simulations; (2) Determine the degree to which the Raman lidar measurements of water vapor and aerosol scattering and extinction can be used to remotely characterize the aerosol humidification factor; (3) Use the high temporal resolution CARL data to examine how aerosol properties vary near clouds; and (4) Use the high temporal resolution CARL and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thin continental cumulus clouds.

  17. Absorbing aerosols over Asia: A Geophysical Fluid Dynamics Laboratory general circulation model sensitivity study of model response to aerosol optical depth and aerosol absorption

    NASA Astrophysics Data System (ADS)

    Randles, C. A.; Ramaswamy, V.

    2008-11-01

    Forcing by absorbing atmospheric black carbon (BC) tends to heat the atmosphere, cool the surface, and reduce the surface latent and sensible heat fluxes. BC aerosol can have a large impact on regional climates and the hydrologic cycle. However, significant uncertainties remain concerning the increases in (1) the total amount of all aerosol species and (2) the amount of aerosol absorption that may have occurred over the 1950-1990 period. Focusing on south and east Asia, the sensitivity of a general circulation model's climate response (with prescribed sea surface temperatures and aerosol distributions) to such changes is investigated by considering a range of both aerosol absorption and aerosol extinction optical depth increases. We include direct and semidirect aerosol effects only. Precipitation changes are less sensitive to changes in aerosol absorption optical depth at lower aerosol loadings. At higher-extinction optical depths, low-level convergence and increases in vertical velocity overcome the stabilizing effects of absorbing aerosols and enhance the monsoonal circulation and precipitation in northwestern India. In contrast, the presence of increases in only scattering aerosols weakens the monsoonal circulation and inhibits precipitation here. Cloud amount changes can enhance or counteract surface solar flux reduction depending on the aerosol loading and absorption, with the changes also influencing the surface temperature and the surface energy balance. The results have implications for aerosol reduction strategies in the future that seek to mitigate air pollution concerns. At higher optical depths, if absorbing aerosol is present, reduction of scattering aerosol alone has a reduced effect on precipitation changes, implying that reductions in BC aerosols should be undertaken at the same time as reductions in sulfate aerosols.

  18. Towards a quasi-complete reconstruction of past atmospheric aerosol load and composition (organic and inorganic) over Europe since 1920 inferred from Alpine ice cores

    NASA Astrophysics Data System (ADS)

    Preunkert, S.; Legrand, M.

    2013-07-01

    Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps), are here used to reconstruct past aerosol load and composition of the free European troposphere from before World War II to present. Available ice core records include inorganic (Na+, Ca2+, NH4+, Cl-, NO3-, and SO42-) and organic (carboxylates, HCHO, humic-like substances, dissolved organic carbon, water-insoluble organic carbon, and black carbon) compounds and fractions that permit reconstructing the key aerosol components and their changes over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921-1951 to 1971-1988 years, mainly as a result of a large increase of sulfate (a factor of 5), ammonium and water-soluble organic aerosol (a factor of 3). Thus, not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water-soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarios dealing with climate forcing by atmospheric aerosol.

  19. Towards a quasi-complete reconstruction of past atmospheric aerosol load and composition (organic and inorganic) over Europe since 1920 inferred from Alpine ice cores

    NASA Astrophysics Data System (ADS)

    Preunkert, S.; Legrand, M.

    2013-02-01

    Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps) are here revisited in view to reconstruct past aerosol load of the free European troposphere from prior World War II to present. The extended array of inorganic (Na+, Ca2+, NH4+, Cl-, NO3-, and SO42-) and organic (carboxylates, HCHO, HUmic LIke Substances, dissolved organic carbon, water insoluble organic carbon, and black carbon) compounds and fractions already investigated permit to examine the overall aerosol composition and its change over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921-1951 to 1971-1988 years, mainly as a result of a large increase of sulfate (a factor of 5), ammonium and water-soluble organic aerosol (a factor of 3). It is shown that not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarii dealing with climate forcing by atmospheric aerosol.

  20. Model for STratospheric Aerosols -MOSTRA : Latest developments

    NASA Astrophysics Data System (ADS)

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

    We present the most recent work related to the development and use of the Model for STrato-spheric Aerosols (MOSTRA). This model is a 3D microphysical/transport model describing the evolution in time and space of the aerosol size distribution described using a set of particle bins. The microphysical module used in the model is based on the PSCBOX model developed by Larsen (2000). The transport module is based on the transport model used in the Belgian Assimilation System of Chemical Observations from Envisat (BASCOE), using a flux-form semi-Lagrangian scheme developed by Lin and Rood (1996). In this presentation, we discuss current challenges and issues, as well as our projects related to MOSTRA for the near future. References: N. Larsen, Polar Stratospheric Clouds, Microphysical and optical models, Scientific Report 00-06, Danish Meteorological Institute, 2000 Lin, S.-J. Rood, R.B., Multidimensional Flux-Form Semi-Lagrangian Transport Schemes, Monthly Weather Review, 124, 2046-2070, 1996.

  1. Parameterization of Aerosol Sinks in Chemical Transport Models

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2012-01-01

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

  2. Aerosol activation: parameterised versus explicit calculation for global models

    NASA Astrophysics Data System (ADS)

    Tost, H.; Pringle, K.; Metzger, S.; Lelieveld, J.

    2009-04-01

    A key process in studies of the aerosol indirect effects on clouds is the activation of particles into droplets at 100% relative humidity. To model this process in cloud, meteorological and climate models is a difficult undertaking because of the wide range of scales involved. The chemical composition of the atmospheric aerosol, originating from both air pollution and natural sources, substantially impacts the aerosol water uptake and growth due to its hygroscopicity. In this study a comparison of aerosol activation, using state-of-the-art aerosol activation parameterisations, and explicit activation due to hygroscopic growth is performed.For that purpose we apply the GMXe aerosol model - treating both dynamic and thermodynamic aerosol properties - within the EMAC (ECHAM5/MESSy Atmospheric chemistry, an atmospheric chemistry general circulation) model. This new aerosol model can explicitely calculate the water uptake of aerosols due to hygroscopicity, allowing the growth of aerosol particles into the regimes of cloud droplets in case of sufficient water vapour availability. Global model simulations using both activation schemes will be presented and compared, elucidating the advantages of each approach.

  3. A TEST OF THERMODYNAMIC EQUILIBRIUM MODELS AND 3-D AIR QUALITY MODELS FOR PREDICTIONS OF AEROSOL NO3-

    EPA Science Inventory

    The inorganic species of sulfate, nitrate and ammonium constitute a major fraction of atmospheric aerosols. The behavior of nitrate is one of the most intriguing aspects of inorganic atmospheric aerosols because particulate nitrate concentrations depend not only on the amount of ...

  4. Insights into different nitrate formation mechanisms from seasonal variations of secondary inorganic aerosols in Shanghai

    NASA Astrophysics Data System (ADS)

    Tao, Ye; Ye, Xingnan; Ma, Zhen; Xie, Yuanyuan; Wang, Ruyu; Chen, Jianmin; Yang, Xin; Jiang, Shuqin

    2016-11-01

    The dominant mechanisms for the formation of fine particulate nitrate during four seasons were proposed by evaluating the correlations between [NO3-]/[SO42-] and [NH4+]/[SO42-]. Size-resolved aerosols were collected in Shanghai from April 2013 to January 2014. The concentration of fine particulate nitrate was below one tenth of the concentration of sulfate in summer, whereas fine particulate nitrate dominated over sulfate in winter. Influenced by aged sea salt aerosols, the molar ratio of [Na+]/[NH4+] reached 53 ± 49% and the depletion of chloride was very significant (0.83) during autumn. In spring, the increase of nitrate concentration became evident for [NH4+]/[SO42-]>2, indicating that sulfate is fully neutralized. During summertime, nighttime hydrolysis of N2O5 dominated the fine particulate nitrate formation. The thresholds of [NH4+]/[SO42-] for nitrate formation in autumn and winter were wrongly characterized by the linear regression between [NO3-]/[SO42-] and [NH4+]/[SO42-], because considerable amounts of Na2SO4 and NH4Cl were present. Replaced by free ammonium in the function equation, it was established that the winter and spring aerosols shared the same nitrate formation mechanism. On the basis of free sulfate, it was evident that both homogeneous neutralization and hydrolysis of N2O5 mechanisms were involved during autumn.

  5. Impact of aerosol size representation on modeling aerosol-cloud interactions

    DOE PAGES

    Zhang, Y.; Easter, R. C.; Ghan, S. J.; ...

    2002-11-07

    In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach.more » The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).« less

  6. Impact of aerosol size representation on modeling aerosol-cloud interactions

    SciTech Connect

    Zhang, Y.; Easter, R. C.; Ghan, S. J.; Abdul-Razzak, H.

    2002-11-07

    In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach. The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).

  7. One-year observations of size distribution characteristics of major aerosol constituents at a coastal receptor site in Hong Kong - Part 1: Inorganic ions and oxalate

    NASA Astrophysics Data System (ADS)

    Bian, Q.; Huang, X. H. H.; Yu, J. Z.

    2014-09-01

    Size distribution data of major aerosol constituents are essential in source apportioning of visibility degradation, testing and verification of air quality models incorporating aerosols. We report here 1-year observations of mass size distributions of major inorganic ions (sulfate, nitrate, chloride, ammonium, sodium, potassium, magnesium and calcium) and oxalate at a coastal suburban receptor site in Hong Kong, China. A total of 43 sets of size-segregated samples in the size range of 0.056-18 μm were collected from March 2011 to February 2012. The size distributions of sulfate, ammonium, potassium and oxalate were characterized by a dominant droplet mode with a mass mean aerodynamic diameter (MMAD) in the range of ~ 0.7-0.9 μm. Oxalate had a slightly larger MMAD than sulfate on days with temperatures above 22 °C as a result of the process of volatilization and repartitioning. Nitrate was mostly dominated by the coarse mode but enhanced presence in fine mode was detected on winter days with lower temperature and lower concentrations of sea salt and soil particles. This data set reveals an inversely proportional relationship between the fraction of nitrate in the fine mode and product of the sum of sodium and calcium in equivalent concentrations and the dissociation constant of ammonium nitrate (i.e., (1/([Na+] + 2[Ca2+]) × (1/Ke')) when Pn_fine is significant (> 10%). The seasonal variation observed for sea salt aerosol abundance, with lower values in summer and winter, is possibly linked with the lower marine salinities in these two seasons. Positive matrix factorization was applied to estimate the relative contributions of local formation and transport to the observed ambient sulfate level through the use of the combined data sets of size-segregated sulfate and select gaseous air pollutants. On average, the regional/super-regional transport of air pollutants was the dominant source at this receptor site, especially on high-sulfate days while local formation

  8. One-year observations of size distribution characteristics of major aerosol constituents at a coastal receptor site in Hong Kong - Part 1: Inorganic ions and oxalate

    NASA Astrophysics Data System (ADS)

    Bian, Q.; Huang, X. H. H.; Yu, J. Z.

    2014-01-01

    Size distribution data of major aerosol constituents are essential in source apportioning of visibility degradation, testing and verification of air quality models incorporating aerosols. We report here one-year observations of mass size distributions of major inorganic ions (sulfate, nitrate, chloride, ammonium, sodium, potassium, magnesium and calcium) and oxalate at a coastal suburban receptor site in Hong Kong, China. A total of 43 sets of size segregated samples in the size range of 0.056-18 μm were collected from March 2011 to February 2012. The size distributions of sulfate, ammonium, potassium and oxalate were characterized by a dominant droplet mode with a mass mean aerodynamic diameter (MMAD) in the range of ~0.7-0.9 μm. Oxalate had a slightly larger MMAD than sulfate on days with temperatures above 22 °C as a result of the process of volatilization and repartitioning. Nitrate was mostly dominated by the coarse mode but enhanced presence in fine mode was detected on winter days with lower temperature and lower concentrations of sea salt and soil particles. This data set reveals an inversely proportional relationship between the fraction of nitrate in the fine mode and product of the sum of sodium and calcium in equivalent concentrations and the dissociation constant of ammonium nitrate (i.e., (1/[Na+] + 2[Ca2+]) × (1/Ke')). The seasonal variation observed for sea salt aerosol abundance, with lower values in summer and winter, is possibly linked with the lower marine salinities in these two seasons. Positive matrix factorization was applied to estimate the relative contributions of local formation and transport to the observed ambient sulfate level through the use of the combined datasets of size-segregated sulfate and select gaseous air pollutants. On average, the regional/super-regional transport of air pollutants was the dominant source at this receptor site, especially on high sulfate days, while local formation processes contributed approximately

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

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.

    2009-12-01

    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 and especially the indirect aerosol 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. Those aerosol characteristics determine their role in direct and indirect aerosol forcing, as their chemical composition and size distribution determine their optical properties and cloud activation potential. A new detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE climate model includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment and an uncertainty estimate of the impact of microphysical processes involving black carbon and its optical properties on aerosol cloud activation and radiative forcing. We calculate an anthropogenic net radiative forcing of -0.46 W/m2, relative to emission changes between 1750 and 2000. This study finds the direct and indirect aerosol effect to be very sensitivity towards the size distribution of the emitted black and organic particles. The total net radiative forcing can vary between -0.26 to -0.47 W/m2. The models radiation transfer scheme reacts even more sensitive to black carbon core shell structure assumptions. Assuming that sulfates, nitrates and secondary organics can lead to a coating shell around a black carbon core can turn the overall net radiative forcing from a negative to a positive number. In the light of these sensitivities, black carbon mitigation experiments can show no to up to very significant impact to slower global warming.

  10. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect

    Turner, David, D.; Ferrare, Richard, A.

    2011-07-06

    The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

  11. Asian Aerosols: A Geophysical Fluid Dynamics Laboratory general circulation model sensitivity study of model response to aerosol optical depth and aerosol absorption

    NASA Astrophysics Data System (ADS)

    Randles, C. A.; Ramaswamy, V.

    2007-12-01

    Atmospheric absorption by black carbon (BC) aerosol heats the atmosphere while simultaneously cooling the surface and reducing latent and sensible heat fluxes from the land. Recent studies have shown that absorbing BC aerosol can have a large impact on regional climates, including modification of the hydrological cycle. However, significant uncertainties remain with regards to (a) the total amount of all aerosol species and (b) the amount of aerosol absorption. Here we present a GCM sensitivity study focusing on the influences due to total aerosol amount and aerosol absorption in the south and east Asian regions. Six experiments are conducted to test the equilibrium response of the GFDL AM2 GCM (under conditions of prescribed, observed sea surface temperatures) to (i) changes in aerosol absorption caused by changes in BC aerosol amount, and (ii) aerosol extinction optical depth increases corresponding to the year 1990 relative to a control case of 1950. In order to systematically explore the uncertainties in aerosol loading and absorption, the sensitivity experiments are classified into four regimes: low extinction optical depth, low absorption; low extinction optical depth, high absorption; high extinction optical depth, low absorption; and high extinction optical depth, high absorption. Changes in surface temperature and changes in the hydrological cycle are generally insignificant when lower aerosol extinction optical depths are considered. For higher extinction optical depths, the change in the modeled regional circulation relative to the control circulation over south and east Asia is affected by the amount of aerosol absorption and contrasts sharply to the regional circulation change associated with increasing only scattering aerosols. When increasing absorbing aerosols over the region, low-level convergence and increases in vertical velocity overcome the stabilizing effects of the absorbing aerosol and enhance the monsoonal circulation and precipitation rate

  12. Aerosol Radiative Forcing and Weather Forecasts in the ECMWF Model

    NASA Astrophysics Data System (ADS)

    Bozzo, A.; Benedetti, A.; Rodwell, M. J.; Bechtold, P.; Remy, S.

    2015-12-01

    Aerosols play an important role in the energy balance of the Earth system via direct scattering and absorpiton of short-wave and long-wave radiation and indirect interaction with clouds. Diabatic heating or cooling by aerosols can also modify the vertical stability of the atmosphere and influence weather pattern with potential impact on the skill of global weather prediction models. The Copernicus Atmosphere Monitoring Service (CAMS) provides operational daily analysis and forecast of aerosol optical depth (AOD) for five aerosol species using a prognostic model which is part of the Integrated Forecasting System of the European Centre for Medium-Range Weather Forecasts (ECMWF-IFS). The aerosol component was developed during the research project Monitoring Atmospheric Composition and Climate (MACC). Aerosols can have a large impact on the weather forecasts in case of large aerosol concentrations as found during dust storms or strong pollution events. However, due to its computational burden, prognostic aerosols are not yet feasible in the ECMWF operational weather forecasts, and monthly-mean climatological fields are used instead. We revised the aerosol climatology used in the operational ECMWF IFS with one derived from the MACC reanalysis. We analyse the impact of changes in the aerosol radiative effect on the mean model climate and in medium-range weather forecasts, also in comparison with prognostic aerosol fields. The new climatology differs from the previous one by Tegen et al 1997, both in the spatial distribution of the total AOD and the optical properties of each aerosol species. The radiative impact of these changes affects the model mean bias at various spatial and temporal scales. On one hand we report small impacts on measures of large-scale forecast skill but on the other hand details of the regional distribution of aerosol concentration have a large local impact. This is the case for the northern Indian Ocean where the radiative impact of the mineral

  13. ModelE2-TOMAS development and evaluation using aerosol optical depths, mass and number concentrations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2014-09-01

    The TwO-Moment Aerosol Sectional microphysics model (TOMAS) has been integrated into the state-of-the-art general circulation model, GISS ModelE2. TOMAS has the flexibility to select a size resolution as well as the lower size cutoff. A computationally efficient version of TOMAS is used here, which has 15 size bins covering 3 nm to 10 μm aerosol dry diameter. For each bin, it simulates the total aerosol number concentration and mass concentrations of sulphate, pure elementary carbon (hydrophobic), mixed elemental carbon (hydrophilic), hydrophobic organic matter, hydrophilic organic matter, sea salt, mineral dust, ammonium, and aerosol-associated water. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the TOMAS model is compared to the default aerosol model in ModelE2, which is a bulk aerosol model. Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement with observations of sulphur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as the bulk aerosol model) cannot capture the observed vertical distribution of sulphur dioxide over the Pacific Ocean possibly due to overly strong convective transport. The TOMAS model successfully captures observed aerosol number concentrations and cloud condensation nuclei concentrations. Anthropogenic aerosol burdens in the bulk aerosol model running in the same host model as TOMAS (ModelE2) differ by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. Larger differences are found for naturally

  14. A note on the effects of inorganic seed aerosol on the oxidation state of secondary organic aerosol—α-Pinene ozonolysis

    NASA Astrophysics Data System (ADS)

    Huang, Dan Dan; Zhang, Xuan; Dalleska, Nathan F.; Lignell, Hanna; Coggon, Matthew M.; Chan, Chi-Ming; Flagan, Richard C.; Seinfeld, John H.; Chan, Chak K.

    2016-10-01

    We compare the oxidation state and molecular composition of α-pinene-derived secondary organic aerosol (SOA) by varying the types and surface areas of inorganic seed aerosol that are used to promote the condensation of SOA-forming vapors. The oxidation state of α-pinene SOA is found to increase with inorganic seed surface area, likely a result of enhanced condensation of low-volatility organic compounds on particles versus deposition on the chamber wall. α-Pinene SOA is more highly oxygenated in the presence of sodium nitrate (SN) seed than ammonium sulfate seed. The relative abundance of semivolatile monomers and low-volatility dimer components that account for more than half of α-pinene SOA mass is not significantly affected by the composition of seed aerosol. Enhanced uptake of highly oxidized small carboxylic acids onto SN seed particles is observed, which could potentially explain the observed higher SOA oxidation state in the presence of SN seed aerosol. Overall, our results demonstrate that a combined effect of seed aerosol composition and surface area leads to an increase in the O:C atomic ratio of α-pinene SOA by as much as a factor of 2.

  15. Modeling global organic aerosol formation and growth

    NASA Astrophysics Data System (ADS)

    Tsimpidi, Alexandra; Karydis, Vlasios; Pandis, Spyros; Lelieveld, Jos

    2014-05-01

    A computationally efficient framework for the description of organic aerosol (OA)-gas partitioning and chemical aging has been developed and implemented into the EMAC atmospheric chemistry-climate model. This model simulates the formation of primary (POA) and secondary organic aerosols (SOA) from semi-volatile (SVOC), intermediate-volatile (IVOC) and volatile organic compounds (VOC). POA are divided in two groups with saturation concentrations at 298 K 0.1, 10, 1000, 100000 µg m-3: OA from fossil fuel combustion and biomass burning. The first 2 surrogate species from each group represent the SVOC while the other surrogate species represent the IVOC. Photochemical reactions that change the volatility of the organics in the gas phase are taken into account. The oxidation products from each group of precursors (SVOC, IVOC, and VOC) are lumped into an additional set of oxidized surrogate species (S-SOA, I-SOA, and V-SOA, respectively) in order to track their source of origin. This model is used to i) estimate the relative contributions of SOA and POA to total OA, ii) determine how SOA concentrations are affected by biogenic and anthropogenic emissions, and iii) evaluate the effect of photochemical aging and long-range transport on OA budget over specific regions.

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

  17. Modeling the Relationships Between Aerosol Properties and the Direct and Indirect Effects of Aerosols on Climate

    NASA Technical Reports Server (NTRS)

    Toon, Owen B.

    1994-01-01

    Aerosols may affect climate directly by scattering and absorbing visible and infrared energy, They may also affect climate indirectly by modifying the properties of clouds through microphysical processes, and by altering abundances of radiatively important gases through heterogeneous chemistry. Researchers understand which aerosol properties control the direct effect of aerosols on the radiation budget. Unfortunately, despite an abundance of data on certain types of aerosols, much work remains to be done to determine the values of these properties. For instance we have little idea about the global distribution, seasonal variation, or interannual variability of the aerosol optical depth. Also we do not know the visible light absorption properties of tropical aerosols which may contain much debris from slash and burn agriculture. A positive correlation between aerosol concentrations and albedos of marine stratus clouds is observed, and the causative microphysics is understood. However, models suggest that it is difficult to produce new particles in the marine boundary layer. Some modelers have suggested that the particles in the marine boundary layer may originate in the free troposphere and be transported into the boundary layer. Others argue that the aerosols are created in the marine boundary layer. There are no data linking aerosol concentration and cirrus cloud albedo, and models suggest cirrus properties may not be very sensitive to aerosol abundance. There is clear evidence of a radiatively significant change in the global lower stratospheric ozone abundance during the past few decades. These changes are caused by heterogeneous chemical reactions occurring on the surfaces of particles. The rates of these reactions depend upon the chemical composition of the particles. Although rapid advances in understanding heterogeneous chemistry have been made, much remains to be done.

  18. The Effects of Mineral Dust on the Hygroscopic and Optical Properties of Inorganic Salt Aerosols

    NASA Astrophysics Data System (ADS)

    Attwood, A. R.; Greenslade, M. E.

    2011-12-01

    Mineral dust particles are a significant fraction of the total aerosol mass, thus they play an important role in the Earth's radiative budget by direct scattering and absorption of radiation. Assessing this impact is complicated by the variability of optical properties resulting from water uptake and changes in chemical composition due to atmospheric mixing. Internal mixtures of montmorillonite, a clay component of mineral dust, with sodium chloride and ammonium sulfate were studied optically using cavity ring down spectroscopy. The effects of the addition of the clay to the optically observed deliquescence relative humidity (DRH) and water uptake of these salts was considered by investigating a series of different salt mass fractions. In most cases, montmorillonite alters the hygroscopic properties and causes the DRH to occur at a lower relative humidity. For ammonium sulfate, optical properties can be approximated by volume weighted mixing rules with some minor deviations around the DRH. For sodium chloride, this approximation is only accurate below the DRH with enhanced water uptake at higher relative humidities. Our results show that salt particles may transition from solid to liquid at a lower relative humidity than is expected based on the salt alone, as observed with changes in optical properties. Further, they contradict current measurements in the literature that suggest little change in the hygroscopic behavior of salts when insoluble mineral dust components are added and should continue to be investigated. Accurate, direct measurements of the effect of the addition of clays to the optical properties of common aerosol species will allow for improvements in the prediction of the aerosol direct effect.

  19. Aerosols

    Atmospheric Science Data Center

    2013-04-17

    ... article title:  Aerosols over Central and Eastern Europe     View Larger Image ... last weeks of March 2003, widespread aerosol pollution over Europe was detected by several satellite-borne instruments. The Multi-angle ...

  20. Modeling Secondary Organic Aerosols over Europe: Impact of Activity Coefficients and Viscosity

    NASA Astrophysics Data System (ADS)

    Kim, Y.; Sartelet, K.; Couvidat, F.

    2014-12-01

    Semi-volatile organic species (SVOC) can condense on suspended particulate materials (PM) in the atmosphere. The modeling of condensation/evaporation of SVOC often assumes that gas-phase and particle-phase concentrations are at equilibrium. However, recent studies show that secondary organic aerosols (SOA) may not be accurately represented by an equilibrium approach between the gas and particle phases, because organic aerosols in the particle phase may be very viscous. The condensation in the viscous liquid phase is limited by the diffusion from the surface of PM to its core. Using a surrogate approach to represent SVOC, depending on the user's choice, the secondary organic aerosol processor (SOAP) may assume equilibrium or model dynamically the condensation/evaporation between the gas and particle phases to take into account the viscosity of organic aerosols. The model is implemented in the three-dimensional chemistry-transport model of POLYPHEMUS. In SOAP, activity coefficients for organic mixtures can be computed using UNIFAC for short-range interactions between molecules and AIOMFAC to also take into account the effect of inorganic species on activity coefficients. Simulations over Europe are performed and POLYPHEMUS/SOAP is compared to POLYPHEMUS/H2O, which was previously used to model SOA using the equilibrium approach with activity coefficients from UNIFAC. Impacts of the dynamic approach on modeling SOA over Europe are evaluated. The concentrations of SOA using the dynamic approach are compared with those using the equilibrium approach. The increase of computational cost is also evaluated.

  1. A Simple Model of Global Aerosol Indirect Effects

    NASA Technical Reports Server (NTRS)

    Ghan, Steven J.; Smith, Steven J.; Wang, Minghuai; Zhang, Kai; Pringle, Kirsty; Carslaw, Kenneth; Pierce, Jeffrey; Bauer, Susanne; Adams, Peter

    2013-01-01

    Most estimates of the global mean indirect effect of anthropogenic aerosol on the Earth's energy balance are from simulations by global models of the aerosol lifecycle coupled with global models of clouds and the hydrologic cycle. Extremely simple models have been developed for integrated assessment models, but lack the flexibility to distinguish between primary and secondary sources of aerosol. Here a simple but more physically based model expresses the aerosol indirect effect (AIE) using analytic representations of cloud and aerosol distributions and processes. Although the simple model is able to produce estimates of AIEs that are comparable to those from some global aerosol models using the same global mean aerosol properties, the estimates by the simple model are sensitive to preindustrial cloud condensation nuclei concentration, preindustrial accumulation mode radius, width of the accumulation mode, size of primary particles, cloud thickness, primary and secondary anthropogenic emissions, the fraction of the secondary anthropogenic emissions that accumulates on the coarse mode, the fraction of the secondary mass that forms new particles, and the sensitivity of liquid water path to droplet number concentration. Estimates of present-day AIEs as low as 5 W/sq m and as high as 0.3 W/sq m are obtained for plausible sets of parameter values. Estimates are surprisingly linear in emissions. The estimates depend on parameter values in ways that are consistent with results from detailed global aerosol-climate simulation models, which adds to understanding of the dependence on AIE uncertainty on uncertainty in parameter values.

  2. MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

    2015-01-01

    The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

  3. Springtime variations of organic and inorganic constituents in submicron aerosols (PM1.0) from Cape Hedo, Okinawa

    NASA Astrophysics Data System (ADS)

    Kunwar, Bhagawati; Torii, K.; Zhu, Chunmao; Fu, Pingqing; Kawamura, Kimitaka

    2016-04-01

    During the spring season with enhanced Asian outflow, we collected submicron aerosol (PM1.0) samples at Cape Hedo, Okinawa Island in the western North Pacific Rim. We analyzed the filter samples for diacids, oxoacids, pyruvic acid, α-dicarbonyls and fatty acids to better understand the sources and atmospheric processes in the outflow regions of Asian pollutants. Molecular distributions of diacids show a predominance of oxalic acid (C2) followed by malonic (C3) and succinic (C4) acids. Total diacids strongly correlated with secondary source tracers such as SO42- (r = 0.87), NH4+ (0.90) and methanesulfonate (MSA-) (0.84), suggesting that diacids are secondarily formed from their precursor compounds. We also found good correlations among C2, organic carbon (OC) and elemental carbon (EC) in the Okinawa aerosols, suggesting that diacids are mainly derived from anthropogenic sources. However, a weak correlation of diacids with levoglucosan, a biomass burning tracer, suggests that biomass buring is not the main source of diacids, rather diacids are secondarily formed by photochemical oxidation of organic precursors derived from fossil fuel combustion. We found a strong correlation (r = 0.98) between inorganic nitrogen (NO3-N + NH4-N) and total nitrogen (TN), to which organic nitrogen (ON) contributed 23%. Fatty acids were characterized by even carbon number predominance, suggesting that they are derived from biogenic sources. The higher abundances of short chain fatty acids (C20) further suggest that fatty acids are largely derived from marine phytoplankton during spring bloom.

  4. [Characteristics of aerosol water-soluble inorganic ions in three types air-pollution incidents of Nanjing City].

    PubMed

    Zhang, Qiu-Chen; Zhu, Bin; Su, Ji-Feng; Wang, Hong-Lei

    2012-06-01

    In order to compare aerosol water-soluble inorganic species in different air-pollution periods, samples of PM10, PM2.1, PM1.1 and the main water-soluble ions (NH4+, Mg2+, Ca2+, Na+, K+, NO2(-), F(-), NO3(-), Cl(-), SO4(2-)) were measured, which were from 3 air-pollution incidents (continued pollution in October 16-30 of 2009, sandstorm pollution in April 27-30 of 2010, and crop burning pollution in June 14 of 2010. The results show that aerosol pollution of 3 periods is serious. The lowest PM2.1/PM10 is only 0.27, which is from sandstorm pollution period, while the largest is 0. 7 from crop burning pollution period. In continued pollution periods, NO3(-) and SO4(2-) are the dominant ions, and the total anions account for an average of 18.62%, 32.92% and 33.53% of PM10, PM2.1 and PM1.1. Total water-soluble ions only account for 13.36%, 23.72% and 28.54% of PM10, PM2.1 and PM1.1 due to the insoluble species is increased in sandstorm pollution period. The mass concentration of Ca2+ in sandstorm pollution period is higher than the other two pollution periods, and which is mainly in coarse particles with diameter larger than 1 microm. All the ten water-soluble ions are much higher in crop burning pollution especially K+ which is the tracer from crop burning. The peak mass concentrations of NO3(-), SO4(2-) and NH4+ are in 0.43-0.65 microm.

  5. Origin of trace elements and inorganic ions in PM 10 aerosols to the South of Mexico City

    NASA Astrophysics Data System (ADS)

    Báez, P. A.; García, M. R.; Torres, B. M. del C.; Padilla, H. G.; Belmont, R. D.; Amador, O. M.; Villalobos-Pietrini, R.

    2007-07-01

    Measurements of trace metals and inorganic ions were carried out on PM 10 aerosols. Sampling was made in the southern section of downtown Mexico City. Samples were collected with an Andersen PM 10 high volume sampler, on glass fiber filters. The ions SO 42-, NO 3-, Cl -, and NH 4+ were analyzed by ion chromatography, Na +, K +, Ca 2+ and Mg 2+ by flame atomic absorption spectroscopy and the trace metals using an atomic absorption spectrometer with a graphite furnace attachment. The results indicated that SO 42- was the most abundant ion, and with respect to trace metals, Pb had the highest concentration in spite of the fact that lead tetraethyl content in gasoline is prohibited by Mexican Federal Law. Pearson's correlation, applied to all data, showed a high correlation among SO 42-, NO 3- and NH 4+, indicating a common anthropogenic origin. In addition the correlation found between Na + and K + indicated a crustal origin. No correlation among the trace metals was found. The scatter plots showed a high neutralization of SO 42- and NO 3- by NH 4+, (NH 4) 2SO 4 and NH 4NO 3 were the major species formed. Enrichment factors were calculated using K as a reference and the results reflected the possible origins of the elements: crustal or anthropogenic. In order to gain a better insight into the origin of trace metals and major inorganic ions, a Principal Component Analysis was applied to the results for 10 elements and 4 ions, for the years 2003 and 2004. Sources of anthropogenic species, such as industries and vehicles are discussed.

  6. Explicit Simulation of Aerosol Physics in a Cloud-Resolving Model: Aerosol Transport and Processing in the Free Troposphere.

    NASA Astrophysics Data System (ADS)

    Ekman, Annica M. L.; Wang, Chien; Ström, Johan; Krejci, Radovan

    2006-02-01

    Large concentrations of small aerosols have been previously observed in the vicinity of anvils of convective clouds. A 3D cloud-resolving model (CRM) including an explicit size-resolving aerosol module has been used to examine the origin of these aerosols. Five different types of aerosols are considered: nucleation mode sulfate aerosols (here defined by 0 d 5.84 nm), Aitken mode sulfate aerosols (here defined by 5.84 nm d 31.0 nm), accumulation mode sulfate aerosols (here defined by d 31.0 nm), mixed aerosols, and black carbon aerosols.The model results suggest that approximately 10% of the initial boundary layer number concentration of Aitken mode aerosols and black carbon aerosols are present at the top of the convective cloud as the cloud reaches its decaying state. The simulated average number concentration of Aitken mode aerosols in the cloud anvil (1.6 × 104 cm-3) is in the same order of magnitude as observations. Thus, the model results strongly suggest that vertical convective transport, particularly during the active period of the convection, is responsible for a major part of the appearance of high concentrations of small aerosols (corresponding to the Aitken mode in the model) observed in the vicinity of cloud anvils.There is some formation of new aerosols within the cloud, but the formation is small. Nucleation mode aerosols are also efficiently scavenged through impaction scavenging by precipitation. Accumulation mode and mixed mode aerosols are efficiently scavenged through nucleation scavenging and their concentrations in the cloud anvil are either very low (mixed mode) or practically zero (accumulation mode).In addition to the 3D CRM, a box model, including important features of the aerosol module of the 3D model, has been used to study the formation of new aerosols after the cloud has evaporated. The possibility of these aerosols to grow to suitable cloud condensation or ice nuclei size is also examined. Concentrations of nucleation mode aerosols

  7. Reallocation in modal aerosol models: impacts on predicting aerosol radiative effects

    NASA Astrophysics Data System (ADS)

    Korhola, T.; Kokkola, H.; Korhonen, H.; Partanen, A.-I.; Laaksonen, A.; Lehtinen, K. E. J.; Romakkaniemi, S.

    2014-01-01

    Atmospheric models often represent the aerosol particle size distribution with a modal approach, in which particles are described with log-normal modes within predetermined size ranges. This approach reallocates particles numerically from one mode to another for example during particle growth, potentially leading to artificial changes in the aerosol size distribution. In this study we analysed how the modal reallocation affects climate-relevant variables: cloud droplet number concentration (CDNC), aerosol-cloud interaction parameter (ACI) and light extinction coefficient (qext). The ACI parameter gives the response of CDNC to a change in total aerosol number concentration. We compared these variables between a modal model (with and without reallocation routines) and a high resolution sectional model, which was considered a reference model. We analysed the relative differences in the chosen variables in four experiments designed to assess the influence of atmospheric aerosol processes. We find that limiting the allowed size ranges of the modes, and subsequent remapping of the distribution, leads almost always to an underestimation of cloud droplet number concentrations (by up to 100%) and an overestimation of light extinction (by up to 20%). On the other hand, the aerosol-cloud interaction parameter can be either over- or underestimated by the reallocating model, depending on the conditions. For example, in the case of atmospheric new particle formation events followed by rapid particle growth, the reallocation can cause on average a 10% overestimation of the ACI parameter. Thus it is shown that the reallocation affects the ability of a model to estimate aerosol climate effects accurately, and this should be taken into account when using and developing aerosol models.

  8. 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.

  9. Distributions and regional budgets of aerosols and their precursors simulated with the EMAC chemistry-climate model

    NASA Astrophysics Data System (ADS)

    Pozzer, A.; de Meij, A.; Pringle, K. J.; Tost, H.; Doering, U. M.; van Aardenne, J.; Lelieveld, J.

    2012-01-01

    The new global anthropogenic emission inventory (EDGAR-CIRCE) of gas and aerosol pollutants has been incorporated in the chemistry general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). A relatively high horizontal resolution simulation is performed for the years 2005-2008 to evaluate the capability of the model and the emissions to reproduce observed aerosol concentrations and aerosol optical depth (AOD) values. Model output is compared with observations from different measurement networks (CASTNET, EMEP and EANET) and AODs from remote sensing instruments (MODIS and MISR). A good spatial agreement of the distribution of sulfate and ammonium aerosol is found when compared to observations, while calculated nitrate aerosol concentrations show some discrepancies. The simulated temporal development of the inorganic aerosols is in line with measurements of sulfate and nitrate aerosol, while for ammonium aerosol some deviations from observations occur over the USA, due to the wrong temporal distribution of ammonia gas emissions. The calculated AODs agree well with the satellite observations in most regions, while negative biases are found for the equatorial area and in the dust outflow regions (i.e. Central Atlantic and Northern Indian Ocean), due to an underestimation of biomass burning and aeolian dust emissions, respectively. Aerosols and precursors budgets for five different regions (North America, Europe, East Asia, Central Africa and South America) are calculated. Over East-Asia most of the emitted aerosols (precursors) are also deposited within the region, while in North America and Europe transport plays a larger role. Further, it is shown that a simulation with monthly varying anthropogenic emissions typically improves the temporal correlation by 5-10% compared to one with constant annual emissions.

  10. Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

    NASA Astrophysics Data System (ADS)

    Bellouin, N.; Mann, G. W.; Woodhouse, M. T.; Johnson, C.; Carslaw, K. S.; Dalvi, M.

    2013-03-01

    The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000-2006. HadGEM simulations of the aerosol optical depth using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. Because of differences in wet deposition rates, GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and abilities to affect cloud droplet number, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of -0.49 W m-2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This

  11. [Characteristics of mass distributions of aerosol particle and its inorganic water-soluble ions in summer over a suburb farmland in Beijing].

    PubMed

    Zhao, Peng; Zhu, Tong; Liang, Bao-sheng; Hu, Min; Kang, Ling; Gong, Ji-cheng

    2006-02-01

    Agricultural activity is one of the important sources of aerosol particle. To understand the mass distribution and sources of aerosol particle and its inorganic water-soluble ions in the suburb farmland of Beijing, particle samples were collected with a MOUDI cascade impactor in the summer of 2004 in a suburb vegetable field. The mass distributions of the particle and its inorganic water-soluble ions in the diameter range of 0.18 to approximately 18 microm were measured. The dominant ions in the fine particle were SO4(2-), NOS3(-) and NH4+. The association of day to day variation of the concentration of these ions with temperature, humidity and solar radiation suggests that they are formed by the reaction of NH3 released from the vegetable field with the acid species produced from photochemical reactions. K+ in the fine particle is likely from the vegetation emission and biomass burning. Ca2+, Mg2+, NO3(-) and SO4(2-) in the coarse particle are suggested to come from the mechanical process by which the soil particle entered the atmosphere, and from the reactions of the acid species at the surface of the soil particle. The results show that fertilizer and soil are possibly important factors determining the aerosol particle over the agricultural fields, and the vegetable fields in suburb Beijing could contribute significantly to the aerosol particle.

  12. Analysis of Atmospheric Aerosol Data Sets and Application of Radiative Transfer Models to Compute Aerosol Effects

    NASA Technical Reports Server (NTRS)

    Schmid, Beat; Bergstrom, Robert W.; Redemann, Jens

    2002-01-01

    This report is the final report for "Analysis of Atmospheric Aerosol Data Sets and Application of Radiative Transfer Models to Compute Aerosol Effects". It is a bibliographic compilation of 29 peer-reviewed publications (published, in press or submitted) produced under this Cooperative Agreement and 30 first-authored conference presentations. The tasks outlined in the various proposals are listed below with a brief comment as to the research performed. Copies of title/abstract pages of peer-reviewed publications are attached.

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

    SciTech Connect

    Lacis, A.A.; Carlson, B.E.; Mishchenko, M.I.

    1996-04-01

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

  14. Aerosol Indirect Effects on Cirrus Clouds in Global Aerosol-Climate Models

    NASA Astrophysics Data System (ADS)

    Liu, X.; Zhang, K.; Wang, Y.; Neubauer, D.; Lohmann, U.; Ferrachat, S.; Zhou, C.; Penner, J.; Barahona, D.; Shi, X.

    2015-12-01

    Cirrus clouds play an important role in regulating the Earth's radiative budget and water vapor distribution in the upper troposphere. Aerosols can act as solution droplets or ice nuclei that promote ice nucleation in cirrus clouds. Anthropogenic emissions from fossil fuel and biomass burning activities have substantially perturbed and enhanced concentrations of aerosol particles in the atmosphere. Global aerosol-climate models (GCMs) have now been used to quantify the radiative forcing and effects of aerosols on cirrus clouds (IPCC AR5). However, the estimate uncertainty is very large due to the different representation of ice cloud formation and evolution processes in GCMs. In addition, large discrepancies have been found between model simulations in terms of the spatial distribution of ice-nucleating aerosols, relative humidity, and temperature fluctuations, which contribute to different estimates of the aerosol indirect effect through cirrus clouds. In this presentation, four GCMs with the start-of-the art representations of cloud microphysics and aerosol-cloud interactions are used to estimate the aerosol indirect effects on cirrus clouds and to identify the causes of the discrepancies. The estimated global and annual mean anthropogenic aerosol indirect effect through cirrus clouds ranges from 0.1 W m-2 to 0.3 W m-2 in terms of the top-of-the-atmosphere (TOA) net radiation flux, and 0.5-0.6 W m-2 for the TOA longwave flux. Despite the good agreement on global mean, large discrepancies are found at the regional scale. The physics behind the aerosol indirect effect is dramatically different. Our analysis suggests that burden of ice-nucleating aerosols in the upper troposphere, ice nucleation frequency, and relative role of ice formation processes (i.e., homogeneous versus heterogeneous nucleation) play key roles in determining the characteristics of the simulated aerosol indirect effects. In addition to the indirect effect estimate, we also use field campaign

  15. Impact of the modal aerosol scheme GLOMAP-mode on aerosol forcing in the Hadley Centre Global Environmental Model

    NASA Astrophysics Data System (ADS)

    Bellouin, N.; Mann, G. W.; Woodhouse, M. T.; Johnson, C.; Carslaw, K. S.; Dalvi, M.

    2012-08-01

    The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000-2006. HadGEM simulations using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and cloud susceptibilities, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of -0.49 W m-2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This difference is compensated by changes in first indirect aerosol forcing: the forcing of -1.17 W m-2

  16. Reallocation in modal aerosol models: impacts on predicting aerosol radiative effects

    NASA Astrophysics Data System (ADS)

    Korhola, T.; Kokkola, H.; Korhonen, H.; Partanen, A.-I.; Laaksonen, A.; Lehtinen, K. E. J.; Romakkaniemi, S.

    2013-08-01

    In atmospheric modelling applications the aerosol particle size distribution is commonly represented by modal approach, in which particles in different size ranges are described with log-normal modes within predetermined size ranges. Such method includes numerical reallocation of particles from a mode to another for example during particle growth, leading to potentially artificial changes in the aerosol size distribution. In this study we analysed how this reallocation affects climatologically relevant parameters: cloud droplet number concentration, aerosol-cloud interaction coefficient and light extinction coefficient. We compared these parameters between a modal model with and without reallocation routines, and a high resolution sectional model that was considered as a reference model. We analysed the relative differences of the parameters in different experiments that were designed to cover a wide range of dynamic aerosol processes occurring in the atmosphere. According to our results, limiting the allowed size ranges of the modes and the following numerical remapping of the distribution by reallocation, leads on average to underestimation of cloud droplet number concentration (up to 100%) and overestimation of light extinction (up to 20%). The analysis of aerosol first indirect effect is more complicated as the ACI parameter can be either over- or underestimated by the reallocating model, depending on the conditions. However, for example in the case of atmospheric new particle formation events followed by rapid particle growth, the reallocation can cause around average 10% overestimation of the ACI parameter. Thus it is shown that the reallocation affects the ability of a model to estimate aerosol climate effects accurately, and this should be taken into account when using and developing aerosol models.

  17. Role of Clouds, Aerosols, and Aerosol-Cloud Interaction in 20th Century Simulations with GISS ModelE2

    NASA Technical Reports Server (NTRS)

    Nazarenko, Larissa; Rind, David; Bauer, Susanne; Del Genio, Anthony

    2015-01-01

    We use the new version of NASA Goddard Institute for Space Studies (GISS) climate model, modelE2 with 2º by 2.5º horizontal resolution and 40 vertical layers, with the model top at 0.1 hPa [Schmidt et al., 2014]. We use two different treatments of the atmospheric composition and aerosol indirect effect: (1) TCAD(I) version has fully interactive Tracers of Aerosols and Chemistry in both the troposphere and stratosphere. This model predicts total aerosol number and mass concentrations [Shindell et al., 2013]; (2) TCAM is the aerosol microphysics and chemistry model based on the quadrature methods of moments [Bauer et al., 2008]. Both TCADI and TCAM models include the first indirect effect of aerosols on clouds [Menon et al., 2010]; the TCAD model includes only the direct aerosol effect. We consider the results of the TCAD, TCADI and TCAM models coupled to "Russell ocean model" [Russell et al., 1995], E2-R. We examine the climate response for the "historical period" that include the natural and anthropogenic forcings for 1850 to 2012. The effect of clouds, their feedbacks, as well as the aerosol-cloud interactions are assessed for the transient climate change.

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

    SciTech Connect

    Lohmann,U.; Schwartz, S. E.

    2008-03-02

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

  19. A physical model of Titan's aerosols.

    PubMed

    Toon, O B; McKay, C P; Griffith, C A; Turco, R P

    1992-01-01

    Microphysical simulations of Titan's stratospheric haze show that aerosol microphysics is linked to organized dynamical processes. The detached haze layer may be a manifestation of 1 cm sec-1 vertical velocities at altitudes above 300 km. The hemispherical asymmetry in the visible albedo may be caused by 0.05 cm sec-1 vertical velocities at altitudes of 150 to 200 km, we predict contrast reversal beyond 0.6 micrometer. Tomasko and Smith's (1982, Icarus 51, 65-95) model, in which a layer of large particles above 220 km altitude is responsible for the high forward scattering observed by Rages and Pollack (1983, Icarus 55, 50-62), is a natural outcome of the detached haze layer being produced by rising motions if aerosol mass production occurs primarily below the detached haze layer. The aerosol's electrical charge is critical for the particle size and optical depth of the haze. The geometric albedo, particularly in the ultraviolet and near infrared, requires that the particle size be near 0.15 micrometer down to altitudes below 100 km, which is consistent with polarization observations (Tomasko and Smith 1982, West and Smith 1991, Icarus 90, 330-333). Above about 400 km and below about 150 km Yung et al.'s (1984, Astrophys. J. Suppl. Ser. 55, 465-506) diffusion coefficients are too small. Dynamical processes control the haze particles below about 150 km. The relatively large eddy diffusion coefficients in the lower stratosphere result in a vertically extensive region with nonuniform mixing ratios of condensable gases, so that most hydrocarbons may condense very near the tropopause rather than tens of kilometers above it. The optical depths of hydrocarbon clouds are probably less than one, requiring that abundant gases such as ethane condense on a subset of the haze particles to create relatively large, rapidly removed particles. The wavelength dependence of the optical radius is calculated for use in analyzing observations of the geometric albedo. The lower

  20. Stratospheric aerosol forcing for climate modeling: 1850-1978

    NASA Astrophysics Data System (ADS)

    Arfeuille, Florian; Luo, Beiping; Thomason, Larry; Vernier, Jean-Paul; Peter, Thomas

    2016-04-01

    We present here a stratospheric aerosol dataset produced using the available aerosol optical depth observations from the pre-satellite period. The scarce atmospheric observations are supplemented by additional information from an aerosol microphysical model, initialized by ice-core derived sulfur emissions. The model is used to derive extinctions at all altitudes, latitudes and times when sulfur injections are known for specific volcanic eruptions. The simulated extinction coefficients are then scaled to match the observed optical depths. In order to produce the complete optical properties at all wavelengths (and the aerosol surface area and volume densities) needed by climate models, we assume a lognormal size distribution of the aerosols. Correlations between the extinctions in the visible and the effective radius and distribution width parameters are taken from the better constrained SAGE II period. The aerosol number densities are then fitted to match the derived extinctions in the 1850-1978 period. From these aerosol size distributions, we then calculate extinction coefficients, single scattering albedos and asymmetry factors at all wavelengths using the Mie theory. The aerosol surface area densities and volume densities are also provided.

  1. Aerosol impacts in the Met Office global NWP model

    NASA Astrophysics Data System (ADS)

    Mulcahy, Jane P.; Brooks, Malcolm E.; Milton, Sean F.

    2010-05-01

    An accurate representation of the direct and indirect effect of aerosols is of growing concern for global numerical weather prediction (NWP). Increased scattering and absorption of incoming shortwave (SW) and outgoing longwave radiation (OLR) fields due to the presence of aerosol layers in the atmosphere modifies the atmospheric heating profile and can affect large-scale circulation patterns. The current representation of aerosols in the global NWP configuration of the Met Office Unified ModelTM (MetUM) is based on a simple aerosol climatology (Cusack et al., 1998). Profiles of water soluble dust, soot, oceanic and stratospheric sulphate aerosols are described separately for land and ocean surfaces and are distributed over the boundary layer, free troposphere and stratosphere (sulphates only). While this improved the reflected SW radiative bias at the top-of-atmosphere (TOA), there is evidence that the climatology is too absorbing leading to a temperature bias in the lower troposphere of approximately 0.5 K/day. Furthermore, the omission of the scattering and absorption properties of mineral dust and biomass burning aerosol particles in particular, is believed to be the principal cause of significant model biases (in the region of 50-56 W m-2) in both the model OLR at the TOA (Haywood et al., 2005) and the surface SW radiation fields (Milton et al., 2008). One of the objectives of the Global Aerosols (G-AER) component of the MACC (Monitoring Atmospheric Composition and Climate) project is to evaluate the impact of an improved aerosol representation on the performance of global NWP models. In a stepwise approach of increasing the aerosol complexity in the MetUM, the Cusack climatology is being replaced by the CLASSIC (Coupled Large-scale Aerosol Simulator for Studies in Climate) aerosol scheme, developed for the HadGEM (Hadley Centre Global Environmental Model) climate model. CLASSIC includes representations of external mixtures of sulphate, black carbon, organic

  2. Real-time measurements of ammonia, acidic trace gases and water-soluble inorganic aerosol species at a rural site in the Amazon Basin

    NASA Astrophysics Data System (ADS)

    Trebs, I.; Meixner, F. X.; Slanina, J.; Otjes, R.; Jongejan, P.; Andreae, M. O.

    2004-06-01

    We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2 and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3-), nitrite (NO2-), chloride (Cl- and sulfate (SO42-), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia - Smoke Aerosols, Clouds, Rainfall and Climate: Aerosols from Biomass Burning Perturb Global and Regional Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder (WAD) in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015ppb for acidic trace gases and aerosol anions and ≤0.118ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative

  3. Future premature mortality due to O3, secondary inorganic aerosols and primary PM in Europe--sensitivity to changes in climate, anthropogenic emissions, population and building stock.

    PubMed

    Geels, Camilla; Andersson, Camilla; Hänninen, Otto; Lansø, Anne Sofie; Schwarze, Per E; Skjøth, Carsten Ambelas; Brandt, Jørgen

    2015-03-04

    Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000-2009, 2050-2059 and 2080-2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future.

  4. Future Premature Mortality Due to O3, Secondary Inorganic Aerosols and Primary PM in Europe — Sensitivity to Changes in Climate, Anthropogenic Emissions, Population and Building Stock

    PubMed Central

    Geels, Camilla; Andersson, Camilla; Hänninen, Otto; Lansø, Anne Sofie; Schwarze, Per E.; Ambelas Skjøth, Carsten; Brandt, Jørgen

    2015-01-01

    Air pollution is an important environmental factor associated with health impacts in Europe and considerable resources are used to reduce exposure to air pollution through emission reductions. These reductions will have non-linear effects on exposure due, e.g., to interactions between climate and atmospheric chemistry. By using an integrated assessment model, we quantify the effect of changes in climate, emissions and population demography on exposure and health impacts in Europe. The sensitivity to the changes is assessed by investigating the differences between the decades 2000–2009, 2050–2059 and 2080–2089. We focus on the number of premature deaths related to atmospheric ozone, Secondary Inorganic Aerosols and primary PM. For the Nordic region we furthermore include a projection on how population exposure might develop due to changes in building stock with increased energy efficiency. Reductions in emissions cause a large significant decrease in mortality, while climate effects on chemistry and emissions only affects premature mortality by a few percent. Changes in population demography lead to a larger relative increase in chronic mortality than the relative increase in population. Finally, the projected changes in building stock and infiltration rates in the Nordic indicate that this factor may be very important for assessments of population exposure in the future. PMID:25749320

  5. 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.

  6. Robust calibration of a global aerosol model

    NASA Astrophysics Data System (ADS)

    Lee, L.; Carslaw, K. S.; Pringle, K. J.; Reddington, C.

    2013-12-01

    Comparison of models and observations is vital for evaluating how well computer models can simulate real world processes. However, many current methods are lacking in their assessment of the model uncertainty, which introduces questions regarding the robustness of the observationally constrained model. In most cases, models are evaluated against observations using a single baseline simulation considered to represent the models' best estimate. The model is then improved in some way so that its comparison to observations is improved. Continuous adjustments in such a way may result in a model that compares better to observations but there may be many compensating features which make prediction with the newly calibrated model difficult to justify. There may also be some model outputs whose comparison to observations becomes worse in some regions/seasons as others improve. In such cases calibration cannot be considered robust. We present details of the calibration of a global aerosol model, GLOMAP, in which we consider not just a single model setup but a perturbed physics ensemble with 28 uncertain parameters. We first quantify the uncertainty in various model outputs (CCN, CN) for the year 2008 and use statistical emulation to identify which of the 28 parameters contribute most to this uncertainty. We then compare the emulated model simulations in the entire parametric uncertainty space to observations. Regions where the entire ensemble lies outside the error of the observations indicate structural model error or gaps in current knowledge which allows us to target future research areas. Where there is some agreement with the observations we use the information on the sources of the model uncertainty to identify geographical regions in which the important parameters are similar. Identification of regional calibration clusters helps us to use information from observation rich regions to calibrate regions with sparse observations and allow us to make recommendations for

  7. If I know the aerosol compositional model identifier, how can I get information about the corresponding aerosol model?

    Atmospheric Science Data Center

    2014-12-08

    ... (APOP) and the Mixture files. The Mixture file lists the pure particles in each model identifier. The APOP then gives the detailed information for the pure particles. More information on the MISR aerosol model is available from ...

  8. Models to support active sensing of biological aerosol clouds

    NASA Astrophysics Data System (ADS)

    Brown, Andrea M.; Kalter, Jeffrey M.; Corson, Elizabeth C.; Chaudhry, Zahra; Boggs, Nathan T.; Brown, David M.; Thomas, Michael E.; Carter, Christopher C.

    2013-05-01

    Elastic backscatter LIght Detection And Ranging (LIDAR) is a promising approach for stand-off detection of biological aerosol clouds. Comprehensive models that explain the scattering behavior from the aerosol cloud are needed to understand and predict the scattering signatures of biological aerosols under varying atmospheric conditions and against different aerosol backgrounds. Elastic signatures are dependent on many parameters of the aerosol cloud, with two major components being the size distribution and refractive index of the aerosols. The Johns Hopkins University Applied Physics Laboratory (JHU/APL) has been in a unique position to measure the size distributions of released biological simulant clouds using a wide assortment of aerosol characterization systems that are available on the commercial market. In conjunction with the size distribution measurements, JHU/APL has also been making a dedicated effort to properly measure the refractive indices of the released materials using a thin-film absorption technique and laboratory characterization of the released materials. Intimate knowledge of the size distributions and refractive indices of the biological aerosols provides JHU/APL with powerful tools to build elastic scattering models, with the purpose of understanding, and ultimately, predicting the active signatures of biological clouds.

  9. Seasonal variation and secondary formation of size-segregated aerosol water-soluble inorganic ions during pollution episodes in Beijing

    NASA Astrophysics Data System (ADS)

    Huang, Xiaojuan; Liu, Zirui; Zhang, Junke; Wen, Tianxue; Ji, Dongsheng; Wang, Yuesi

    2016-02-01

    Particulate matter (PM) pollution is a serious issue that has aroused great public attention in Beijing. To examine the seasonal characteristics of aerosols in typical pollution episodes, water-soluble inorganic ions (SO42 -, NO3-, NH4+, Cl-, K+, Na+, Ca2 + and Mg2 +) in size-segregated PM collected by an Anderson sampler (equipped with 50% effective cut-off diameters of 9.0, 5.8, 4.7, 3.3, 2.1, 1.1, 0.65, 0.43 μm and an after filter) were investigated in four intensive campaigns from June 2013 to May 2014 in the Beijing urban area. Pronounced seasonal variation of TWSIs in fine particles (aerodynamic diameter less than 2.1 μm) was observed, with the highest concentration in summer (71.5 ± 36.3 μg/m3) and the lowest in spring (28.1 ± 15.2 μg/m3). Different ion species presented different seasonal characteristics of mass concentration and size distribution, reflecting their different dominant sources. As the dominant component, SO42 -, NO3- and NH4+ (SNA) in fine particles appeared to play an important role in the formation of high PM pollution since its contribution to the TWSIs and PM2.1 mass increased significantly during pollution episodes. Due to the hygroscopic growth and enhanced secondary formation in the droplet mode (0.65-2.1 μm) from clean days to polluted days, the size distribution peak of SNA in the fine mode tended to shift from 0.43-0.65 μm to 0.65-2.1 μm. Relative humidity (RH) and temperature contributed to influence the secondary formation and regulate the size distributions of sulfates and nitrates. Partial correlation analysis found that high RH would promote the sulfur and nitrogen oxidation rates in the fine mode, while high temperature favored the sulfur oxidation rate in the condensation mode (0.43-0.65 μm) and reduced the nitrogen oxidation rate in the droplet mode (0.65-2.1 μm). The NO3-/SO42 - mass ratio in PM2.1 (73% of the samples) exceeded 1.0, suggesting that vehicle exhaust currently makes a greater contribution to aerosol

  10. Analysis of organic and inorganic species on the surface of atmospheric aerosol using time-of-flight secondary ion mass spectrometry (TOF-SIMS)

    NASA Astrophysics Data System (ADS)

    Peterson, Richard E.; Tyler, Bonnie J.

    This work explores the utility of time-of-flight static secondary-ion mass spectrometry (TOF-SIMS) for the analysis of the surface organic layer on individual atmospheric aerosol particles. The surface sensitivity and minimal fragmentation available with TOF-SIMS suggest that it can be a powerful tool for the examination of the organic and inorganic species on the surface of individual particles. Cascade impactors were used to collect aerosol from summer 2000 Montana forest fires, winter snowmobile samples in Yellowstone National Park, Hawaiian lava and sea salt, from an Asian Dust event reaching Salt Lake City, Utah in April 2001 and from Salt Lake Valley summer urban aerosol. TOF-SIMS analysis and multivariate statistical techniques combined gave chemical and morphological information about the particles. Surfaces of the aerosol from forest fires, snowmobile exhaust, and sea salt were all dominated by aliphatic hydrocarbons and their amphiphilic derivatives. Each source showed a different organic chemical signature. The extent and composition of the organics layer which typically covers the surface of atmospheric particles are expected to effect all of the surface related aerosol properties such as health effects, the ability of the particle to activate and form cloud droplets, and the aggregation of particles as well as reactions between the particle and gas phase species.

  11. Reduction in biomass burning aerosol light absorption upon humidification: Roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

    SciTech Connect

    lewis, Kristen A.; Arnott, W. P.; Moosmuller, H.; Chakrabarti, Raj; Carrico, Christian M.; Kreidenweis, Sonia M.; Day, Derek E.; Malm, William C.; Laskin, Alexander; Jimenez, Jose L.; Ulbrich, Ingrid M.; Huffman, John A.; Onasch, Timothy B.; Trimborn, Achim; Liu, Li; Mishchenko, M.

    2009-11-27

    Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

  12. Role of clouds, aerosols, and aerosol-cloud interaction in 20th century simulations with GISS ModelE2

    NASA Astrophysics Data System (ADS)

    Nazarenko, L.; Rind, D. H.; Bauer, S.; Del Genio, A. D.

    2015-12-01

    Simulations of aerosols, clouds and their interaction contribute to the major source of uncertainty in predicting the changing Earth's energy and in estimating future climate. Anthropogenic contribution of aerosols affects the properties of clouds through aerosol indirect effects. Three different versions of NASA GISS global climate model are presented for simulation of the twentieth century climate change. All versions have fully interactive tracers of aerosols and chemistry in both the troposphere and stratosphere. All chemical species are simulated prognostically consistent with atmospheric physics in the model and the emissions of short-lived precursors [Shindell et al., 2006]. One version does not include the aerosol indirect effect on clouds. The other two versions include a parameterization of the interactive first indirect aerosol effect on clouds following Menon et al. [2010]. One of these two models has the Multiconfiguration Aerosol Tracker of Mixing state (MATRIX) that permits detailed treatment of aerosol mixing state, size, and aerosol-cloud activation. The main purpose of this study is evaluation of aerosol-clouds interactions and feedbacks, as well as cloud and aerosol radiative forcings, for the twentieth century climate under different assumptions and parameterizations for aerosol, clouds and their interactions in the climate models. The change of global surface air temperature based on linear trend ranges from +0.8°C to +1.2°C between 1850 and 2012. Water cloud optical thickness increases with increasing temperature in all versions with the largest increase in models with interactive indirect effect of aerosols on clouds, which leads to the total (shortwave and longwave) cloud radiative cooling trend at the top of the atmosphere. Menon, S., D. Koch, G. Beig, S. Sahu, J. Fasullo, and D. Orlikowski (2010), Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10,4559-4571, doi:10.5194/acp-10-4559-2010. Shindell, D., G. Faluvegi

  13. An Aerosol Condensation Model for Sulfur Trioxide

    SciTech Connect

    Grant, K E

    2008-02-07

    This document describes a model for condensation of sulfuric acid aerosol given an initial concentration and/or source of gaseous sulfur trioxide (e.g. fuming from oleum). The model includes the thermochemical effects on aerosol condensation and air parcel buoyancy. Condensation is assumed to occur heterogeneously onto a preexisting background aerosol distribution. The model development is both a revisiting of research initially presented at the Fall 2001 American Geophysical Union Meeting [1] and a further extension to provide new capabilities for current atmospheric dispersion modeling efforts [2]. Sulfuric acid is one of the most widely used of all industrial chemicals. In 1992, world consumption of sulfuric acid was 145 million metric tons, with 42.4 Mt (mega-tons) consumed in the United States [10]. In 2001, of 37.5 Mt consumed in the U.S., 74% went into producing phosphate fertilizers [11]. Another significant use is in mining industries. Lawuyi and Fingas [7] estimate that, in 1996, 68% of use was for fertilizers and 5.8% was for mining. They note that H{sub 2}SO{sub 4} use has been and should continue to be very stable. In the United States, the elimination of MTBE (methyl tertiary-butyl ether) and the use of ethanol for gasoline production are further increasing the demand for petroleum alkylate. Alkylate producers have a choice of either a hydrofluoric acid or sulfuric acid process. Both processes are widely used today. Concerns, however, over the safety or potential regulation of hydrofluoric acid are likely to result in most of the growth being for the sulfuric acid process, further increasing demand [11]. The implication of sulfuric acid being a pervasive industrial chemical is that transport is also pervasive. Often, this is in the form of oleum tankers, having around 30% free sulfur trioxide. Although sulfuric acid itself is not a volatile substance, fuming sulfuric acid (referred to as oleum) is [7], the volatile product being sulfur trioxide

  14. Indirect aerosol effect increases CMIP5 models projected Arctic warming

    SciTech Connect

    Chylek, Petr; Vogelsang, Timothy J.; Klett, James D.; Hengartner, Nicholas; Higdon, Dave; Lesins, Glen; Dubey, Manvendra K.

    2016-02-20

    Phase 5 of the Coupled Model Intercomparison Project (CMIP5) climate models’ projections of the 2014–2100 Arctic warming under radiative forcing from representative concentration pathway 4.5 (RCP4.5) vary from 0.9° to 6.7°C. Climate models with or without a full indirect aerosol effect are both equally successful in reproducing the observed (1900–2014) Arctic warming and its trends. However, the 2014–2100 Arctic warming and the warming trends projected by models that include a full indirect aerosol effect (denoted here as AA models) are significantly higher (mean projected Arctic warming is about 1.5°C higher) than those projected by models without a full indirect aerosol effect (denoted here as NAA models). The suggestion is that, within models including full indirect aerosol effects, those projecting stronger future changes are not necessarily distinguishable historically because any stronger past warming may have been partially offset by stronger historical aerosol cooling. In conclusion, the CMIP5 models that include a full indirect aerosol effect follow an inverse radiative forcing to equilibrium climate sensitivity relationship, while models without it do not.

  15. Volcanic Aerosol Evolution: Model vs. In Situ Sampling

    NASA Astrophysics Data System (ADS)

    Pfeffer, M. A.; Rietmeijer, F. J.; Brearley, A. J.; Fischer, T. P.

    2002-12-01

    Volcanoes are the most significant non-anthropogenic source of tropospheric aerosols. Aerosol samples were collected at different distances from 92°C fumarolic source at Poás Volcano. Aerosols were captured on TEM grids coated by a thin C-film using a specially designed collector. In the sampling, grids were exposed to the plume for 30-second intervals then sealed and frozen to prevent reaction before ATEM analysis to determine aerosol size and chemistry. Gas composition was established using gas chromatography, wet chemistry techniques, AAS and Ion Chromatography on samples collected directly from a fumarolic vent. SO2 flux was measured remotely by COSPEC. A Gaussian plume dispersion model was used to model concentrations of the gases at different distances down-wind. Calculated mixing ratios of air and the initial gas species were used as input to the thermo-chemical model GASWORKS (Symonds and Reed, Am. Jour. Sci., 1993). Modeled products were compared with measured aerosol compositions. Aerosols predicted to precipitate out of the plume one meter above the fumarole are [CaSO4, Fe2.3SO4, H2SO4, MgF2. Na2SO4, silica, water]. Where the plume leaves the confines of the crater, 380 meters distant, the predicted aerosols are the same, excepting FeF3 replacing Fe2.3SO4. Collected aerosols show considerable compositional differences between the sampling locations and are more complex than those predicted. Aerosols from the fumarole consist of [Fe +/- Si,S,Cl], [S +/- O] and [Si +/- O]. Aerosols collected on the crater rim consist of the same plus [O,Na,Mg,Ca], [O,Si,Cl +/- Fe], [Fe,O,F] and [S,O +/- Mg,Ca]. The comparison between results obtained by the equilibrium gas model and the actual aerosol compositions shows that an assumption of chemical and thermal equilibrium evolution is invalid. The complex aerosols collected contrast the simple formulae predicted. These findings show that complex, non-equilibrium chemical reactions take place immediately upon volcanic

  16. Real-time measurements of ammonia, acidic trace gases and water-soluble inorganic aerosol species at a rural site in the Amazon Basin

    NASA Astrophysics Data System (ADS)

    Trebs, I.; Meixner, F. X.; Slanina, J.; Otjes, R.; Jongejan, P.; Andreae, M. O.

    2004-02-01

    We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2) and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3-), nitrite (NO2-), chloride (Cl-) and sulfate (SO42-), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia Smoke Aerosols, Clouds, Rainfall and Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015 ppb for acidic trace gases and aerosol anions and ≤0.118 ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative humidity and temperature variations between day and night as well as to

  17. Particle size distribution and inorganic aerosol characterization during DAURE 2009 winter field campaign at Montseny site

    NASA Astrophysics Data System (ADS)

    Aranzazu Revuelta, M.; Gómez-Moreno, Francisco J.; Plaza, Javier; Coz, Esther; Pey, Jorge; Cusack, Michael; Pandolfi, Marco; Rodríguez-Maroto, Jesús J.; Pujadas, Manuel

    2010-05-01

    During DAURE 2009 winter field campaign, one of the sampling sites was Montseny, a rural background station located 40 km NNE from Barcelona and 25 km W from the Mediterranean Sea. It is a Natural Park and a protected area, thus with low human activity, mainly agriculture. The sampling station was located on a valley with it axis oriented on the direction NW-SE. At this site, a TSI-SMPS (DMA 3071 and CPC 3022) was installed in order to measure the particle number distribution in the size range 15-600 nm during the period March 19-27 with a measurement cycle of 12 minutes The particle mass distribution was measured by a micro-orifice uniform deposit impactor (MOUDI) using eleven size stages with aluminum substrates and a quartz fiber backup filter. Four samples were taken during the period 13-19 March, two during 24 hours and other two during 48 hours. This impactor has a wider size range allowing to measure from 56 to 18000 nm. The substrates and filters obtained were later analyzed for determining soluble ions (sulfate, nitrate, ammonium and calcium) by IC. There are mainly two different kinds of events measured with the SMPS. When the air masses were coming from SE, which meant that they could come from the park but also from the urban and industrial areas located in the pre-coastal depression, it was characterized by higher particle number concentrations and by size distributions centered on 80 nm. This meant it was an aged aerosol, which had grown up by coagulation, condensation and oxidation processes. When the air masses were coming from NW (the second valley axis side), the particle measured were much smaller, the instrument started to detect particles with 15 nm, but smaller ones could be possible. This meant that new particle nucleation could have occurred in the valley, just before arriving to the sampling point. From MOUDI samplings, two different types of events were also observed. Three of the four samplings coincided with stagnation of air masses or

  18. Modeling Gas-Particle Partitioning of SOA: Effects of Aerosol Physical State and RH

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Seinfeld, J.

    2011-12-01

    Aged tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. In liquid aerosol particles non-ideal mixing of all species determines whether the condensed phase undergoes liquid-liquid phase separation or whether it is stable in a single mixed phase, and whether it contains solid salts in equilibrium with their saturated solution. The extended thermodynamic model AIOMFAC is able to predict such phase states by representing the variety of organic components using functional groups within a group-contribution concept. The number and composition of different condensed phases impacts the diversity of reaction media for multiphase chemistry and the gas-particle partitioning of semivolatile species. Recent studies show that under certain conditions biogenic and other organic-rich particles can be present in a highly viscous, semisolid or amorphous solid physical state, with consequences regarding reaction kinetics and mass transfer limitations. We present results of new gas-particle partitioning computations for aerosol chamber data using a model based on AIOMFAC activity coefficients and state-of-the-art vapor pressure estimation methods. Different environmental conditions in terms of temperature, relative humidity (RH), salt content, amount of precursor VOCs, and physical state of the particles are considered. We show how modifications of absorptive and adsorptive gas-particle mass transfer affects the total aerosol mass in the calculations and how the results of these modeling approaches compare to data of aerosol chamber experiments, such as alpha-pinene oxidation SOA. For a condensed phase in a mixed liquid state containing ammonium sulfate, the model predicts liquid-liquid phase separation up to high RH in case of, on average, moderately hydrophilic organic compounds, such as first generation oxidation products of alpha-pinene. The computations also reveal that treating liquid phases as ideal

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

    NASA Astrophysics Data System (ADS)

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

    2001-10-01

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

  20. Implementing marine organic aerosols into the GEOS-Chem model

    NASA Astrophysics Data System (ADS)

    Gantt, B.; Johnson, M. S.; Crippa, M.; Prévôt, A. S. H.; Meskhidze, N.

    2014-09-01

    Marine organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

  1. Radiation Transfer Model for Aerosol Events in the Earth Atmosphere

    NASA Astrophysics Data System (ADS)

    Mukai, Sonoyo; Yokomae, Takuma; Nakata, Makiko; Sano, Itaru

    Recently large scale-forest fire, which damages the Earth environment as biomass burning and emission of carbonaceous particles, frequently occurs due to the unstable climate and/or global warming tendency. It is also known that the heavy soil dust is transported from the China continent to Japan on westerly winds, especially in spring. Furthermore the increasing emis-sions of anthropogenic particles associated with continuing economic growth scatter serious air pollutants. Thus atmospheric aerosols, especially in Asia, are very complex and heavy loading, which is called aerosol event. In the case of aerosol events, it is rather difficult to do the sun/sky photometry from the ground, however satellite observation is an effective for aerosol monitoring. Here the detection algorithms from space for such aerosol events as dust storm or biomass burn-ing are dealt with multispectral satellite data as ADEOS-2/GLI, Terra/Aqua/MODIS and/or GOSAT/CAI first. And then aerosol retrieval algorithms are examined based on new radiation transfer code for semi-infinite atmosphere model. The derived space-based results are validated with ground-based measurements and/or model simulations. Namely the space-or surface-based measurements, multiple scattering calculations and model simulations are synthesized together for aerosol retrieval in this work.

  2. Implementing marine organic aerosols into the GEOS-Chem model

    NASA Astrophysics Data System (ADS)

    Gantt, B.; Johnson, M. S.; Crippa, M.; Prévôt, A. S. H.; Meskhidze, N.

    2015-03-01

    Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

  3. Implementing Marine Organic Aerosols Into the GEOS-Chem Model

    NASA Technical Reports Server (NTRS)

    Johnson, Matthew S.

    2015-01-01

    Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

  4. A method to quantify organic functional groups and inorganic compounds in ambient aerosols using attenuated total reflectance FTIR spectroscopy and multivariate chemometric techniques

    NASA Astrophysics Data System (ADS)

    Coury, Charity; Dillner, Ann M.

    An attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopic technique and a multivariate calibration method were developed to quantify ambient aerosol organic functional groups and inorganic compounds. These methods were applied to size-resolved particulate matter samples collected in winter and summer of 2004 at three sites: a downtown Phoenix, Arizona location, a rural site near Phoenix, and an urban fringe site between the urban and rural site. Ten organic compound classes, including four classes which contain a carbonyl functional group, and three inorganic species were identified in the ambient samples. A partial least squares calibration was developed and applied to the ambient spectra, and 13 functional groups related to organic compounds (aliphatic and aromatic CH, methylene, methyl, alkene, aldehydes/ketones, carboxylic acids, esters/lactones, acid anhydrides, carbohydrate hydroxyl and ethers, amino acids, and amines) as well as ammonium sulfate and ammonium nitrate were quantified. Comparison of the sum of the mass measured by the ATR-FTIR technique and gravimetric mass indicates that this method can quantify nearly all of the aerosol mass on sub-micrometer size-segregated samples. Analysis of sample results shows that differences in organic functional group and inorganic compound concentrations at the three sampling sites can be measured with these methods. Future work will analyze the quantified data from these three sites in detail.

  5. Modeling wet deposition and concentration of inorganics over Northeast Asia with MRI-PM/c

    NASA Astrophysics Data System (ADS)

    Kajino, M.; Deushi, M.; Maki, T.; Oshima, N.; Inomata, Y.; Sato, K.; Ohizumi, T.; Ueda, H.

    2012-11-01

    We conducted a regional-scale simulation over Northeast Asia for the year 2006 using an aerosol chemical transport model, with time-varying lateral and upper boundary concentrations of gaseous species predicted by a global stratospheric and tropospheric chemistry-climate model. The present one-way nested global-through-regional-scale model is named the Meteorological Research Institute-Passive-tracers Model system for atmospheric Chemistry (MRI-PM/c). We evaluated the model's performance with respect to the major anthropogenic and natural inorganic components, SO42-, NH4+, NO3-, Na+ and Ca2+ in the air, rain and snow measured at the Acid Deposition Monitoring Network in East Asia (EANET) stations. Statistical analysis showed that approximately 40-50 % and 70-80 % of simulated concentration and wet deposition of SO42-, NH4+, NO3-and Ca2+ are within factors of 2 and 5 of the observations, respectively. The prediction of the sea-salt originated component Na+ was not successful at near-coastal stations (where the distance from the coast ranged from 150 to 700 m), because the model grid resolution (Δx=60 km) is too coarse to resolve it. The simulated Na+ in precipitation was significantly underestimated by up to a factor of 30.

  6. The Navy Oceanic Vertical Aerosol Model

    DTIC Science & Technology

    1993-12-01

    34windows" exist in the molecular absorption of the electromagnetic energy through which trans- missions in IR communication can take place. In these...the aerosol both scatters and absorbs electromagnetic energy . Of particular interest to the Navy is the role natural marine aerosols play within the...34 \\( )/ •dr12 This technique speeds up the calculations since the integrals can be calculated earlier and their values stored as numbers in a lookup table

  7. A fast aerosol microphysical model for the UTLS

    NASA Astrophysics Data System (ADS)

    Tripathi, S.; Grainger, R.; Rogers, H.

    2003-04-01

    A fast aerosol microphysical model for the UTLS (FAMMUS) has been developed to study aerosol behaviour in UTLS region. This model simulates homogeneous heteromolecular nucleation, condensational growth, coagulation and sedimentation of binary sulphuric acid-water particles together to predict the composition and size-distribution of stratospheric aerosols. This model has already been successfully applied to estimate the changes in background stratospheric aerosol surface area due to aircraft sulphur emission (Tripathi et al., 2002). The principal advantage with this model is that it is non-iterative (Jacobson, 1999), i.e. computing time is minimised by finding semi-implicit solutions to aerosol processes. Condensation and coagulation are solved using operator-split method. Hence the effect of coagulation is determined in a single iteration and the solution is volume conserving for any time-step. The semi-implicit solution for coagulation agrees well with the Smoluchowski's solution for a constant coagulation kernel. Similarly, starting from the fundamental growth equation, solution for condensational growth is derived which does not require iteration. The solution conserves mass exactly, and is unconditionally stable. In the model homogeneous nucleation and condensation is coupled in such a manner that it allows for a realistic competition between the two processes for the limited amount of vapour. With geometrically related size bin (44 bins for sulphuric acid-water particles in the range from 0.3 nm to 5mm) and a 600s time-step the model takes about half an hour to complete a 7 year simulation of stratospheric background aerosols on a work station. FAMMUS has been used to simulate background stratospheric aerosols and volcanically disturbed aerosol and model results are compared favourably with results from earlier model studies and observed data.

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

    PubMed

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

    2015-06-01

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

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

    PubMed Central

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

    2015-01-01

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

  10. Implementing marine organic aerosols into the GEOS-Chem model

    DOE PAGES

    Gantt, B.; Johnson, M. S.; Crippa, M.; ...

    2015-03-17

    Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Modelmore » predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.« less

  11. Evaluation of the global aerosol microphysical ModelE2-TOMAS model against satellite and ground-based observations

    NASA Astrophysics Data System (ADS)

    Lee, Y. H.; Adams, P. J.; Shindell, D. T.

    2015-03-01

    The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the-art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and overpredicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

  12. Climatic influence of background and volcanic stratosphere aerosol models

    NASA Technical Reports Server (NTRS)

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

    1982-01-01

    A simple modelization of the earth atmosphere system including tropospheric and stratospheric aerosols has been derived and tested. Analytical expressions are obtained for the albedo variation due to a thin stratospheric aerosol layer. Also outlined are the physical procedures and the respective influence of the main parameters: aerosol optical thickness, single scattering albedo and asymmetry factor, and sublayer albedo. The method is applied to compute the variation of the zonal and planetary albedos due to a stratospheric layer of background H2SO4 particles and of volcanic ash.

  13. Introduction of the aerosol feedback process in the model BOLCHEM

    NASA Astrophysics Data System (ADS)

    Russo, Felicita; Maurizi, Alberto; D'Isidoro, Massimo; Tampieri, Francesco

    2010-05-01

    The effect of aerosols on the climate is still one of the least understood processes in the atmospheric science. The use of models to simulate the interaction between aerosols and climate can help understanding the physical processes that rule this interaction and hopefully predicting the future effects of anthropogenic aerosols on climate. In particular regional models can help study the effect of aerosols on the atmospheric dynamics on a local scale. In the work performed here we studied the feedback of aerosols in the radiative transfer calculation using the regional model BOLCHEM. The coupled meteorology-chemistry model BOLCHEM is based on the BOLAM meteorological model. The BOLAM dynamics is based on hydrostatic primitive equations, with wind components u and v, potential temperature ?, specific humidity q, surface pressure ps, as dependent variables. The vertical coordinate σ is terrain-following with variables distributed on a non-uniformly spaced staggered Lorentz grid. In the standard configuration of the model a collection of climatological aerosol optical depth values for each aerosol species is used for the radiative transfer calculation. In the feedback exercise presented here the aerosol optical depth was calculated starting from the modeled aerosol concentrations using an approximate Mie formulation described by Evans and Fournier (Evans, B.T.N. and G.R. Fournier, Applied Optics, 29, 1990). The calculation was done separately for each species and aerosol size distribution. The refractive indexes for the different species were taken from P. Stier's work (P. Stier et al., Atmos. Chem. Phys., 5, 2005) and the aerosol extinction obtained by Mie calculation were compared with the results reported by OPAC (M. Hess et al., Bull. Am. Met. Soc., 79, 1998). Two model runs, with and without the aerosol feedback, were performed to study the effects of the feedback on meteorological parameters. As a first setup of the model runs we selected a domain over the

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

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Wright, D. L.; Koch, D.; Lewis, E. R.; McGraw, R.; Chang, L.-S.; Schwartz, S. E.; Ruedy, R.

    2008-10-01

    A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) are described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations. A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment. This is more likely due to

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    We have implemented the sectional aerosol dynamics model SALSA in the European scale chemistry-transport model MATCH (Multi-scale Atmospheric Transport and Chemistry). The new model is called MATCH-SALSA. It includes aerosol microphysics, with several formulations for nucleation, wet scavenging and condensation. The model reproduces observed higher particle number concentration (PNC) in central Europe and lower concentrations in remote regions. The model PNC size distribution peak occurs at the same or smaller particle size as the observed peak at five measurement sites spread across Europe. Total PNC is underestimated at Northern and Central European sites and accumulation mode PNC is underestimated at all investigated sites. On the other hand the model performs well for particle mass, including secondary inorganic aerosol components. Elemental and organic carbon concentrations are underestimated at many of the sites. Further development is needed, primarily for treatment of secondary organic aerosol, both in terms of biogenic emissions and chemical transformation, and for nitrogen gas-particle partitioning. Updating the biogenic SOA scheme will likely have a large impact on modeled PM2.5 and also affect the model performance for PNC through impacts on nucleation and condensation. An improved nitrogen partitioning model may also improve the description of condensational growth.

  16. Reactivity of inorganic sulfide species toward a heme protein model.

    PubMed

    Bieza, Silvina A; Boubeta, Fernando; Feis, Alessandro; Smulevich, Giulietta; Estrin, Darío A; Boechi, Leonardo; Bari, Sara E

    2015-01-20

    The reactivity of inorganic sulfide species toward heme peptides was explored under biorelevant conditions in order to unravel the molecular details of the reactivity of the endogenous hydrogen sulfide toward heme proteins. Unlike ferric porphyrinates, which are reduced by inorganic sulfide, some heme proteins can form stable Fe(III)-sulfide adducts. To isolate the protein factors ruling the redox chemistry, we used as a system model, the undecapeptide microperoxidase (MP11), a heme peptide derived from cytochrome c proteolysis that retains the proximal histidine bound to the Fe(III) atom. Upon addition of gaseous hydrogen sulfide (H2S) at pH 6.8, the UV-vis spectra of MP11 closely resembled those of the low-spin ferric hydroxo complex (only attained at an alkaline pH) and cysteine or alkylthiol derivatives, suggesting that the Fe(III) reduction was prevented. The low-frequency region of the resonance Raman spectrum revealed the presence of an Fe(III)-S band at 366 cm(-1) and the general features of a low-spin hexacoordinated heme. Anhydrous sodium sulfide (Na2S) was the source of sulfide of choice for the kinetic evaluation of the process. Theoretical calculations showed no distal stabilization mechanisms for bound sulfide species in MP11, highlighting a key role of the proximal histidine for the stabilization of the Fe(III)-S adducts of heme compounds devoid of distal counterparts, which is significant with regard to the biochemical reactivity of endogenous hydrogen sulfide.

  17. PARAGON: A Systematic, Integrated Approach to Aerosol Observation and Modeling

    NASA Technical Reports Server (NTRS)

    Diner, David J.; Kahn, Ralph A.; Braverman, Amy J.; Davies, Roger; Martonchik, John V.; Menzies, Robert T.; Ackerman, Thomas P.; Seinfeld, John H.; Anderson, Theodore L.; Charlson, Robert J.; Bosenberg, Jens; Collins, William D.; Rasch, Philip J.; Holben, Brent N.; Hostetler, Chris A.; Wielicki, Bruce A.; Miller, Mark A.; Schwartz, Stephen E.; Ogren, John A.; Penner, Joyce E.; Stephens, Graeme L.; Torres, Omar; Travis, Larry D.; Yu, Bin

    2004-01-01

    Aerosols are generated and transformed by myriad processes operating across many spatial and temporal scales. Evaluation of climate models and their sensitivity to changes, such as in greenhouse gas abundances, requires quantifying natural and anthropogenic aerosol forcings and accounting for other critical factors, such as cloud feedbacks. High accuracy is required to provide sufficient sensitivity to perturbations, separate anthropogenic from natural influences, and develop confidence in inputs used to support policy decisions. Although many relevant data sources exist, the aerosol research community does not currently have the means to combine these diverse inputs into an integrated data set for maximum scientific benefit. Bridging observational gaps, adapting to evolving measurements, and establishing rigorous protocols for evaluating models are necessary, while simultaneously maintaining consistent, well understood accuracies. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) concept represents a systematic, integrated approach to global aerosol Characterization, bringing together modern measurement and modeling techniques, geospatial statistics methodologies, and high-performance information technologies to provide the machinery necessary for achieving a comprehensive understanding of how aerosol physical, chemical, and radiative processes impact the Earth system. We outline a framework for integrating and interpreting observations and models and establishing an accurate, consistent and cohesive long-term data record.

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

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Wright, D.; Koch, D.; Lewis, E. R.; McGraw, R.; Chang, L.-S.; Schwartz, S. E.; Ruedy, R.

    2008-05-01

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

  19. Indirect aerosol effect increases CMIP5 models projected Arctic warming

    DOE PAGES

    Chylek, Petr; Vogelsang, Timothy J.; Klett, James D.; ...

    2016-02-20

    Phase 5 of the Coupled Model Intercomparison Project (CMIP5) climate models’ projections of the 2014–2100 Arctic warming under radiative forcing from representative concentration pathway 4.5 (RCP4.5) vary from 0.9° to 6.7°C. Climate models with or without a full indirect aerosol effect are both equally successful in reproducing the observed (1900–2014) Arctic warming and its trends. However, the 2014–2100 Arctic warming and the warming trends projected by models that include a full indirect aerosol effect (denoted here as AA models) are significantly higher (mean projected Arctic warming is about 1.5°C higher) than those projected by models without a full indirect aerosolmore » effect (denoted here as NAA models). The suggestion is that, within models including full indirect aerosol effects, those projecting stronger future changes are not necessarily distinguishable historically because any stronger past warming may have been partially offset by stronger historical aerosol cooling. In conclusion, the CMIP5 models that include a full indirect aerosol effect follow an inverse radiative forcing to equilibrium climate sensitivity relationship, while models without it do not.« less

  20. An Aerosol Physical Chemistry Model for the Upper Troposphere

    NASA Technical Reports Server (NTRS)

    Lin, Jin-Sheng

    2001-01-01

    This report is the final report for the Cooperative Agreement NCC2-1000. The tasks outlined in the various proposals are: (1) Development of an aerosol chemistry model; (2) Utilization of satellite measurements of trace gases along with analysis of temperatures and dynamic conditions to understand ice cloud formation, dehydration and sedimentation in the winter polar regions; (3) Comparison of the HALOE and SAGE II time dependencies of the Pinatubo aerosol decay. The publications are attached.

  1. On the Implications of aerosol liquid water and phase separation for modeled organic aerosol mass

    EPA Science Inventory

    Current chemical transport models assume that organic aerosol (OA)-forming compounds partition mostly to a water-poor, organic-rich phase in accordance with their vapor pressures. However, in the southeast United States, a significant fraction of ambient organic compounds are wat...

  2. MODELS-3 COMMUNITY MULTISCALE AIR QUALITY (CMAQ) MODEL AEROSOL COMPONENT 1: MODEL DESCRIPTION

    EPA Science Inventory

    The aerosol component of the Community Multiscale Air Quality (CMAQ) model is designed to be an efficient and economical depiction of aerosol dynamics in the atmosphere. The approach taken represents the particle size distribution as the superposition of three lognormal subdis...

  3. Easy Aerosol - a model intercomparison project to study aerosol-radiative interactions and their impact on regional climate

    NASA Astrophysics Data System (ADS)

    Voigt, A.; Bony, S.; Stevens, B. B.; Boucher, O.; Medeiros, B.; Pincus, R.; Wang, Z.; Zhang, K.; Lewinschal, A.; Bellouin, N.; Yang, Y. M.

    2015-12-01

    Recent studies illustrated the potential of aerosols to change the large-scale atmospheric circulation and precipitation patterns, but it remains unclear to what extent the proposed aerosol-induced changes reflect robust model behavior and are affected by the climate system's internal variability. "Easy Aerosol" addresses this question by subjecting nine comprehensive climate models with prescribed sea-surface temperatures (SSTs) to the same set of idealized "easy" aerosol perturbations. The aerosol perturbations are designed based on a global aerosol climatology and mimic the gravest mode of the anthropogenic aerosol. They both scatter and absorb shortwave radiation, but to focus on direct radiative effects aerosol-cloud interactions are omitted. Each model contributes seven simulations. A clean control case with no aerosol-radiative effects is compared to six perturbed simulations with differing aerosol loading, zonal aerosol distributions, and SSTs. To estimate the role of internal variability, one of the models contributes a 5-member ensemble for each simulation. When observed SSTs from years 1979-2005 are used, the aerosol leads to a local depression of precipitation at the Northern Hemisphere center of the aerosol and a northward shift of the intertropical convergence zone (ITCZ). This is consistent with the aerosol's shortwave atmospheric heating and the fact that SSTs are fixed. Moreover, the Northern hemisphere mid-latitude jet shifts poleward in the annual and zonal-mean. Due to large natura variability, however, these signals only emerge in ensemble runs or if the aerosol optical depth is increased by a factor of five compared to the observed magnitude of the present-day anthropogenic aerosol. When SSTs are adapted to include the cooling effect of the aerosol, the ITCZ and the Northern hemisphere jet shift southward in the annual and zonal-mean. The models exhibit very similar precipitation and zonal wind changes in response to the SST change, showing

  4. Modeling of Aerosol Vertical Profiles Using GIS and Remote Sensing

    PubMed Central

    Wong, Man Sing; Nichol, Janet E.; Lee, Kwon Ho

    2009-01-01

    The use of Geographic Information Systems (GIS) and Remote Sensing (RS) by climatologists, environmentalists and urban planners for three dimensional modeling and visualization of the landscape is well established. However no previous study has implemented these techniques for 3D modeling of atmospheric aerosols because air quality data is traditionally measured at ground points, or from satellite images, with no vertical dimension. This study presents a prototype for modeling and visualizing aerosol vertical profiles over a 3D urban landscape in Hong Kong. The method uses a newly developed technique for the derivation of aerosol vertical profiles from AERONET sunphotometer measurements and surface visibility data, and links these to a 3D urban model. This permits automated modeling and visualization of aerosol concentrations at different atmospheric levels over the urban landscape in near-real time. Since the GIS platform permits presentation of the aerosol vertical distribution in 3D, it can be related to the built environment of the city. Examples are given of the applications of the model, including diagnosis of the relative contribution of vehicle emissions to pollution levels in the city, based on increased near-surface concentrations around weekday rush-hour times. The ability to model changes in air quality and visibility from ground level to the top of tall buildings is also demonstrated, and this has implications for energy use and environmental policies for the tall mega-cities of the future. PMID:22408531

  5. Size Distributions and Formation Pathways of Organic and Inorganic Constituents in Spring Aerosols from Okinawa Island in the Western North Pacific Rim: An Outflow Region of Asian Dusts

    NASA Astrophysics Data System (ADS)

    Deshmukh, D. K.; Lazaar, M.; Kawamura, K.; Kunwar, B.; Tachibana, E.; Boreddy, S. K. R.

    2015-12-01

    Size-segregated aerosols (9-stages) were collected at Okinawa Island in the western North Pacific Rim in spring 2008. The samples were analyzed for diacids (C2-C12), ω-oxoacids (ωC2-ωC9), a-dicarbonyls (C2-C3), organic carbon (OC), water-soluble OC (WSOC) and major ions to understand the sources and atmospheric processes in the outflow region of Asian pollutants. The molecular distribution of diacids showed the predominance of oxalic acid (C2) followed by malonic and succinic acids in all the size-segregated aerosols. ω-Oxoacids showed the predominance of glyoxylic acid (ωC2) whereas glyoxal (Gly) was more abundant than methylglyoxal in all the sizes. The abundant presence of sulfate as well as phthalic and adipic acids in Okinawa aerosols suggested a significant contribution of anthropogenic sources in East Asia via long-range atmospheric transport. Diacids (C2-C5), ωC2 and Gly as well as WSOC and OC peaked at 0.65-1.1 µm in fine mode whereas azelaic (C9) and 9-oxononanoic (ωC9) acids peaked at 3.3-4.7 µm in coarse mode. Sulfate and ammonium are enriched in fine mode whereas sodium and chloride are in coarse mode. An important mechanism for the formation of these organic species in Okinawa aerosols is probably gas phase oxidation of VOCs and subsequent in-cloud processing during long-range transport. Their characteristics size distribution implies that fine particles enriched with these organic and inorganic species could act as CCN to develop the cloud cover over the western North Pacific. The major peak of C9 and ωC9 on coarse mode suggest that they are produced by photooxidation of unsaturated fatty acids mainly derived from phytoplankton via heterogeneous reactions on sea spray particles. This study demonstrates that anthropogenic aerosols emitted from East Asia have significant influence on the compositions of organic and inorganic aerosols in the western North Pacific Rim.

  6. Observations and regional modeling of aerosol optical properties, speciation and size distribution over Northern Africa and western Europe

    NASA Astrophysics Data System (ADS)

    Menut, Laurent; Siour, Guillaume; Mailler, Sylvain; Couvidat, Florian; Bessagnet, Bertrand

    2016-10-01

    The aerosol speciation and size distribution is modeled during the summer 2013 and over a large area encompassing Africa, Mediterranean and western Europe. The modeled aerosol is compared to available measurements such as the AERONET aerosol optical depth (AOD) and aerosol size distribution (ASD) and the EMEP network for surface concentrations of particulate matter PM2.5, PM10 and inorganic species (nitrate, sulfate and ammonium). The main goal of this study is to quantify the model ability to realistically model the speciation and size distribution of the aerosol. Results first showed that the long-range transport pathways are well reproduced and mainly constituted by mineral dust: spatial correlation is ≈ 0.9 for AOD and Ångström exponent, when temporal correlations show that the day-to-day variability is more difficult to reproduce. Over Europe, PM2.5 and PM10 have a mean temporal correlation of ≈ 0.4 but the lowest spatial correlation ( ≈ 0.25 and 0.62, respectively), showing that the fine particles are not well localized or transported. Being short-lived species, the uncertainties on meteorology and emissions induce these lowest scores. However, time series of PM2.5 with the speciation show a good agreement between model and measurements and are useful for discriminating the aerosol composition. Using a classification from the south (Africa) to the north (northern Europe), it is shown that mineral dust relative mass contribution decreases from 50 to 10 % when nitrate increases from 0 to 20 % and all other species, sulfate, sea salt, ammonium, elemental carbon, primary organic matter, are constant. The secondary organic aerosol contribution is between 10 and 20 % with a maximum at the latitude of the Mediterranean Sea (Spanish stations). For inorganic species, it is shown that nitrate, sulfate and ammonium have a mean temporal correlation of 0.25, 0.37 and 0.17, respectively. The spatial correlation is better (0.25, 0.5 and 0.87), showing that the mean

  7. 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.

  8. Polar organic and inorganic markers in PM10 aerosols from an inland city of China--seasonal trends and sources.

    PubMed

    Xie, Mingjie; Wang, Gehui; Hu, Shuyuan; Gao, Shixiang; Han, Qingyou; Xu, Yajuan; Feng, Jianfang

    2010-10-15

    Polar organic compounds and elements were quantified in PM(10) aerosols collected in urban and rural areas of Baoji, an inland city of China, during winter and spring 2008. Concentrations of biomass burning markers and high molecular weight n-alkanoic acids (HMW, >C(22:0)) were heavily increased in winter. In contrast, sugars presented in higher levels in the spring, among which sucrose was the most abundant with an average of 219ngm(-3) in winter and 473ngm(-3) in spring respectively. This suggests enhanced biotic activity in the warm season, whereas no obvious trend was observed for sugar alcohols, concentrations of the three sugar alcohols in spring were only 0.94-2.3 times as those in winter, indicating a second pathway of their formation other than fungal spores in cold season. Major crustal elements (i.e., Fe, K, Mn and Ti) in PM(10) aerosols were also observed in larger concentrations in spring samples than those in winter due to an enhancement of coarse particles from soil minerals. By using principal component analysis (PCA) and positive matrix factorization (PMF), sources and their contributions to the PM components were also investigated in this study. Four factors were extracted with both models, and the sources represented by different factors were based on the highest loaded marker species as follows: factor 1, soil and road dust (Fe, Sr and Ti); factor 2, biomass burning (levoglucosan, galactosan and syringic acid); factor 3, microbial emissions (fructose and sucrose); and factor 4, fossil fuel combustion and fungal spores influence (Pb, Zn, arabitol and mannitol). The high correlation between PM(10) and factor 1 suggested that PM(10) pollution in Baoji was dominated by soil and dust re-suspension.

  9. Isolating the effects of climate change in the variation of secondary inorganic aerosols (SIA) in Europe for the 21st century (1991-2100)

    NASA Astrophysics Data System (ADS)

    Jimenez-Guerrero, Pedro; Jose Gomez-Navarro, Juan; Jerez, Sonia; Lorente-Plazas, Raquel; Garcia-Valero, Juan Andres; Montavez, Juan Pedro

    2011-02-01

    The analysis of the influence of future climatic variations on air quality needs of methods that give a space-time display of large atmospheric data related to air pollution. Here a new approach in order to assess the impacts of climate change on the patterns of variation of secondary inorganic aerosols (SIA) over Europe is presented. The most widely used method of analysis (selected time-slices, future-minus-present method) is very sensitive to the chosen control and future periods because of the internal variability of the climate system. In order to overcome this limitation, full transient simulations for the period 1991-2100 under the SRES A2 scenario are analysed by the Empirical Orthogonal Functions (EOFs) methodology in order minimise the uncertainty associated to the internal variability due to the longer time series obtained. The results indicate that the EOF1 accounts for around 30-45% of the total variance for the SIA levels and points out a general increase of its trend over the entire domain ( p < 0.005), except in the case of nitrate, whose change signal is not significant ( p > 0.1). The correlation between SIA and meteorological parameters indicates that the trends and patterns of variation of aerosols are related to the higher temperature projected for the future climate. It favours the formation of sulphates and ammonium (increasing the concentrations of atmospheric oxidants) and the decomposition of ammonium nitrate, remaining in the gas phase. Further, the decreases in precipitation have a strong effect on the frequency of the washout and therefore in the levels of aerosols. The concentrations of aerosols decrease with increasing precipitation as wet deposition provides the main aerosol sink. The trend from a decreasing mixing height found in several areas of Europe is frequently related to a decrease in precipitation, representing an adding effect for the enhanced future SIA concentrations.

  10. Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

    NASA Astrophysics Data System (ADS)

    Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

    2009-11-01

    Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

  11. Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

    NASA Astrophysics Data System (ADS)

    Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

    2009-07-01

    Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

  12. Modeling Gas-phase Glyoxal and Associated Secondary Organic Aerosol Formation in a Megacity using WRF/Chem

    NASA Astrophysics Data System (ADS)

    Wang, K.; Hodzic, A.; Barth, M. C.; Jimenez, J. L.; Volkamer, R.; Ervens, B.; Zhang, Y.

    2011-12-01

    Organic aerosol (OA) as one of a major fine particulate matter in the atmosphere plays an important role in air pollution, human health, and climate forcing. OA is composed of directly emitted primary organic aerosol and chemically produced secondary organic aerosols (SOA). Despite much recent progress in understanding SOA formation, current air quality models cannot explain the magnitude and growth of atmospheric SOA, due to high uncertainties in sources, properties, and chemical reactions of precursors and formation pathways of SOA. Recent laboratory and modeling studies showed that glyoxal may serve as an important SOA precursor in the condensed solution of inorganic or organic aerosol particles (e.g., ammonium sulfate, fulvic acid, and amino acids). In this study, the Weather Research and Forecasting model with chemistry (WRF/Chem) is modified to account for the latest observed gas-phase yields of glyoxal from various volatile organic compounds (VOCs) and the associated SOA formation in the aqueous aerosol phase. The SOA formation in the aqueous aerosol phase is implemented using two approaches. In the first approach, two simplified parameterizations are used to represent the lumped particle-phase chemical processes under dark conditions and photochemical surface uptake. In the second approach, more detailed kinetic glyoxal reactions such as reversible glyoxal uptake, dimer formation of glyoxal, and oligomerization are treated and resolved explicitly. The updated WRF/Chem is assessed over the Mexico City and the surrounding region during March 2006 using the MILAGRO campaign data. Various observations such as organic matter from Aerodyne Aerosol Mass Spectrometer and VOCs from Proton-transfer Ion Trap Mass Spectrometry were compared. The preliminary results showed that the addition of the SOA formation from glyoxal in aqueous particles brings SOA predictions into a better agreement with field observations, in particular in presence of high relative humidity

  13. The cloud-aerosol-radiation (CAR) ensemble modeling system

    NASA Astrophysics Data System (ADS)

    Liang, X.-Z.; Zhang, F.

    2013-08-01

    A cloud-aerosol-radiation (CAR) ensemble modeling system has been developed to incorporate the largest choices of alternate parameterizations for cloud properties (cover, water, radius, optics, geometry), aerosol properties (type, profile, optics), radiation transfers (solar, infrared), and their interactions. These schemes form the most comprehensive collection currently available in the literature, including those used by the world's leading general circulation models (GCMs). CAR provides a unique framework to determine (via intercomparison across all schemes), reduce (via optimized ensemble simulations), and attribute specific key factors for (via physical process sensitivity analyses) the model discrepancies and uncertainties in representing greenhouse gas, aerosol, and cloud radiative forcing effects. This study presents a general description of the CAR system and illustrates its capabilities for climate modeling applications, especially in the context of estimating climate sensitivity and uncertainty range caused by cloud-aerosol-radiation interactions. For demonstration purposes, the evaluation is based on several CAR standalone and coupled climate model experiments, each comparing a limited subset of the full system ensemble with up to 896 members. It is shown that the quantification of radiative forcings and climate impacts strongly depends on the choices of the cloud, aerosol, and radiation schemes. The prevailing schemes used in current GCMs are likely insufficient in variety and physically biased in a significant way. There exists large room for improvement by optimally combining radiation transfer with cloud property schemes.

  14. Cloud-Aerosol-Radiation (CAR) ensemble modeling system

    NASA Astrophysics Data System (ADS)

    Liang, X.-Z.; Zhang, F.

    2013-04-01

    A Cloud-Aerosol-Radiation (CAR) ensemble modeling system has been developed to incorporate the largest choices of alternative parameterizations for cloud properties (cover, water, radius, optics, geometry), aerosol properties (type, profile, optics), radiation transfers (solar, infrared), and their interactions. These schemes form the most comprehensive collection currently available in the literature, including those used by the world leading general circulation models (GCMs). The CAR provides a unique framework to determine (via intercomparison across all schemes), reduce (via optimized ensemble simulations), and attribute specific key factors for (via physical process sensitivity analyses) the model discrepancies and uncertainties in representing greenhouse gas, aerosol and cloud radiative forcing effects. This study presents a general description of the CAR system and illustrates its capabilities for climate modeling applications, especially in the context of estimating climate sensitivity and uncertainty range caused by cloud-aerosol-radiation interactions. For demonstration purpose, the evaluation is based on several CAR standalone and coupled climate model experiments, each comparing a limited subset of the full system ensemble with up to 896 members. It is shown that the quantification of radiative forcings and climate impacts strongly depends on the choices of the cloud, aerosol and radiation schemes. The prevailing schemes used in current GCMs are likely insufficient in variety and physically biased in a significant way. There exists large room for improvement by optimally combining radiation transfer with cloud property schemes.

  15. SAGE II aerosol data validation based on retrieved aerosol model size distribution from SAGE II aerosol measurements

    NASA Technical Reports Server (NTRS)

    Wang, Pi-Huan; Mccormick, M. P.; Mcmaster, L. R.; Chu, W. P.; Swissler, T. J.; Osborn, M. T.; Russell, P. B.; Oberbeck, V. R.; Livingston, J.; Rosen, J. M.

    1989-01-01

    Consideration is given to aerosol correlative measurements experiments for the Stratospheric Aerosol and Gas Experiment (SAGE) II, conducted between November 1984 and July 1986. The correlative measurements were taken with an impactor/laser probe, a dustsonde, and an airborne 36-cm lidar system. The primary aerosol quantities measured by the ground-based instruments are compared with those calculated from the aerosol size distributions from SAGE II aerosol extinction measurements. Good agreement is found between the two sets of measurements.

  16. AeroCom INSITU Project: Comparing modeled and measured aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Andrews, Elisabeth; Schmeisser, Lauren; Schulz, Michael; Fiebig, Markus; Ogren, John; Bian, Huisheng; Chin, Mian; Easter, Richard; Ghan, Steve; Kokkola, Harri; Laakso, Anton; Myhre, Gunnar; Randles, Cynthia; da Silva, Arlindo; Stier, Phillip; Skeie, Ragnehild; Takemura, Toshihiko; van Noije, Twan; Zhang, Kai

    2016-04-01

    AeroCom, an open international collaboration of scientists seeking to improve global aerosol models, recently initiated a project comparing model output to in-situ, surface-based measurements of aerosol optical properties. The model/measurement comparison project, called INSITU, aims to evaluate the performance of a suite of AeroCom aerosol models with site-specific observational data in order to inform iterative improvements to model aerosol modules. Surface in-situ data has the unique property of being traceable to physical standards, which is an asset in accomplishing the overall goal of bettering the accuracy of aerosols processes and the predicative capability of global climate models. Here we compare dry, in-situ aerosol scattering and absorption data from ~75 surface, in-situ sites from various global aerosol networks (including NOAA, EUSAAR/ACTRIS and GAW) with a simulated optical properties from a suite of models participating in the AeroCom project. We report how well models reproduce aerosol climatologies for a variety of time scales, aerosol characteristics and behaviors (e.g., aerosol persistence and the systematic relationships between aerosol optical properties), and aerosol trends. Though INSITU is a multi-year endeavor, preliminary phases of the analysis suggest substantial model biases in absorption and scattering coefficients compared to surface measurements, though the sign and magnitude of the bias varies with location. Spatial patterns in the biases highlight model weaknesses, e.g., the inability of models to properly simulate aerosol characteristics at sites with complex topography. Additionally, differences in modeled and measured systematic variability of aerosol optical properties suggest that some models are not accurately capturing specific aerosol behaviors, for example, the tendency of in-situ single scattering albedo to decrease with decreasing aerosol extinction coefficient. The endgoal of the INSITU project is to identify specific

  17. On the implications of aerosol liquid water and phase separation for organic aerosol mass

    NASA Astrophysics Data System (ADS)

    Pye, Havala O. T.; Murphy, Benjamin N.; Xu, Lu; Ng, Nga L.; Carlton, Annmarie G.; Guo, Hongyu; Weber, Rodney; Vasilakos, Petros; Wyat Appel, K.; Hapsari Budisulistiorini, Sri; Surratt, Jason D.; Nenes, Athanasios; Hu, Weiwei; Jimenez, Jose L.; Isaacman-VanWertz, Gabriel; Misztal, Pawel K.; Goldstein, Allen H.

    2017-01-01

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM / OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM / OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH > SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM / OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model-measurement gap. When taking into account deviations from ideality, including both inorganic (when RH > SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from

  18. 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

  19. Large-Scale Aerosol Modeling and Analysis

    DTIC Science & Technology

    2008-09-30

    aerosol species up to six days in advance anywhere on the globe. NAAPS and COAMPS are particularly useful for forecasts of dust storms in areas...impact cloud processes globally. With increasing dust storms due to climate change and land use changes in desert regions, the impact of the...bacteria in large-scale dust storms is expected to significantly impact warm ice cloud formation, human health, and ecosystems globally. In Niemi et al

  20. Evaluation of aerosol properties simulated by the high resolution global coupled chemistry-aerosol-microphysics model C-IFS-GLOMAP

    NASA Astrophysics Data System (ADS)

    Dhomse, Sandip; Mann, Graham; Carslaw, Ken; Flemming, Johannes; Morcrette, Jean-Jacques; Engelen, Richard; Remy, Samuel; Boucher, Olivier; Benduhn, Francois; Hewson, Will; Woodhouse, Matthew

    2016-04-01

    The EU Framework Programme GEMS and MACC consortium projects co-ordinated by the European Centre for Medium-range Weather Forecasts (ECMWF) have developed an operational global forecasting and reanalysis system (Composition-IFS) for atmospheric composition including greenhouse gases, reactive gases and aerosol. The current operational C-IFS system uses a mass-based aerosol model coupled to data assimilation of Aerosol Optical Depth measured by satellite (MODIS) to predict global aerosol properties. During MACC, the GLOMAP-mode aerosol microphysics scheme was added to the system, providing information on aerosol size and number for improved representation of aerosol-radiation and aerosol-cloud interactions, accounting also for simulated global variations in size distribution and internally-mixed particle composition. The IFS-GLOMAP system has recently been upgraded to couple with the sulphur cycle simulated in the online TM5 tropospheric chemistry module for global reactive gases. This C-IFS-GLOMAP system is also being upgraded to use a new "nitrate-extended" version of GLOMAP which realistically treats the size-resolved gas-particle partitioning of semi volatile gases ammonia and nitric acid. In this poster we described C-IFS-GLOMAP and present an evaluation of the global sulphate aerosol distribution simulated in this coupled aerosol-chemistry C-IFS-GLOMAP, comparing to surface observations in Europe, North America and the North Atlantic and contrasting to the fixed timescale sulphate production scheme developed in GEMS. We show that the coupling to the TM5 sulphur chemistry improves the seasonal cycle of sulphate aerosol, for example addressing a persistent wintertime sulphate high bias in northern Europe. The improved skill in simulated sulphate aerosol seasonal cycle is a pre-requisite to realistically characterise nitrate aerosol since biases in sulphate affect the amount of free ammonia available to form ammonium nitrate.

  1. Evolution of secondary inorganic and organic aerosols during transport: A case study at a regional receptor site.

    PubMed

    Peng, Jianfei; Hu, Min; Gong, Zhaoheng; Tian, Xudong; Wang, Ming; Zheng, Jing; Guo, Qingfeng; Cao, Wei; Lv, Wei; Hu, Weiwei; Wu, Zhijun; Guo, Song

    2016-11-01

    Understanding the evolution of aerosols in the atmosphere is of great importance for improving air quality and reducing aerosol-related uncertainties in global climate simulations. Here, a unique haze episode at a regional receptor site near the East China Sea was examined as a case study of the aging process of atmospheric aerosols during transport. An increase in photochemical age from 5 h to more than 25 h and a progressive increase in the fitted mean particle diameter from 70 nm to approximately 300 nm were observed. According to the pollution features and meteorology conditions involved, pollution accumulation (PA), sea breeze (SB), and land breeze (LB) periods were identified. Concentrations of black carbon (BC), hydrocarbon-like organic aerosols (HOA), semi-volatile oxidized organic aerosols (SV-OOA), and nitrate increased by 7-fold up to 39-fold when the air masses passed through Taizhou, a nearby city. In addition, nitrate and SV-OOA dominated the aerosol composition in the urban outflow plumes (52% and 18%, respectively), yet they gradually decreased in concentration during transport. In contrast, sulfate and the low-volatile oxidized organic aerosols (LV-OOA) exhibited more regional footprints and potentially have similar formation mechanisms. The atomic oxygen-to-carbon (O/C) ratio also increased from 0.45 to 0.9, thereby suggesting that rapid formation of highly oxidized secondary organic aerosols (SOA) occurred during transport. Overall, these results provide valuable insight into the evolution of the chemical and physical features of aerosol pollution during transport and also highlight the need for regulatory controls of nitrogen oxides, sulfur dioxide, and VOCs to improve air quality on different scales.

  2. Source indicators of biomass burning associated with inorganic salts and carboxylates in dry season ambient aerosol in Chiang Mai Basin, Thailand

    NASA Astrophysics Data System (ADS)

    Tsai, Ying I.; Sopajaree, Khajornsak; Chotruksa, Auranee; Wu, Hsin-Ching; Kuo, Su-Ching

    2013-10-01

    PM10 aerosol was collected between February and April 2010 at an urban site (CMU) and an industrial site (TOT) in Chiang Mai, Thailand, and characteristics and provenance of water-soluble inorganic species, carboxylates, anhydrosugars and sugar alcohols were investigated with particular reference to air quality, framed as episodic or non-episodic pollution. Sulfate, a product of secondary photochemical reactions, was the major inorganic salt in PM10, comprising 25.9% and 22.3% of inorganic species at CMU and TOT, respectively. Acetate was the most abundant monocarboxylate, followed by formate. Oxalate was the dominant dicarboxylate. A high acetate/formate mass ratio indicated that primary traffic-related and biomass-burning emissions contributed to Chiang Mai aerosols during episodic and non-episodic pollution. During episodic pollution carboxylate peaks indicated sourcing from photochemical reactions and/or directly from traffic-related and biomass burning processes and concentrations of specific biomarkers of biomass burning including water-soluble potassium, glutarate, oxalate and levoglucosan dramatically increased. Levoglucosan, the dominant anhydrosugar, was highly associated with water-soluble potassium (r = 0.75-0.79) and accounted for 93.4% and 93.7% of anhydrosugars at CMU and TOT, respectively, during episodic pollution. Moreover, levoglucosan during episodic pollution was 14.2-21.8 times non-episodic lows, showing clearly that emissions from biomass burning are the major cause of PM10 episodic pollution in Chiang Mai. Additionally, the average levoglucosan/mannosan mass ratio during episodic pollution was 14.1-14.9, higher than the 5.73-7.69 during non-episodic pollution, indicating that there was more hardwood burning during episodic pollution. Higher concentrations of glycerol and erythritol during episodic pollution further indicate that biomass burning activities released soil biota from forest and farmland soils.

  3. Modelling inorganic biocide emission from treated wood in water.

    PubMed

    Tiruta-Barna, Ligia; Schiopu, Nicoleta

    2011-09-15

    The objective of this work is to develop a chemical model for explaining the leaching behaviour of inorganic biocides from treated wood. The standard leaching test XP CEN/TS14429 was applied to a commercial construction material made of treated Pinus sylvestris (Copper Boron Azole preservative). The experimental results were used for developing a chemical model under PHREEQC(®) (a geochemical software, with LLNL, MINTEQ data bases) by considering the released species detected in the eluates: main biocides Cu and B, other trace biocides (Cr and Zn), other elements like Ca, K, Cl, SO(4)(-2), dissolved organic matter (DOC). The model is based on chemical phenomena at liquid/solid interfaces (complexation, ion exchange and hydrolysis) and is satisfactory for the leaching behaviour representation. The simulation results confronted with the experiments confirmed the hypotheses of: (1) biocide fixation by surface complexation reactions with wood specific sites (carboxyl and phenol for Cu, Zn, Cr(III), aliphatic hydroxyl for B, ion exchange to a lesser extent) and (2) biocide mobilisation by extractives (DOC) coming from the wood. The maximum of Cu, Cr(III) and Zn fixation occurred at neutral pH (including the natural pH of wood), while B fixation was favoured at alkaline pH.

  4. Introducing GMXe: A new global aerosol dynamics and thermodynamics model for climate and air quality studies

    NASA Astrophysics Data System (ADS)

    Pringle, K.; Metzger, S.; Tost, H.; Steil, B.; Lelieveld, J.

    2009-04-01

    The treatment of aerosols in global atmospheric models has advanced significantly in the past decade, but the global aerosol distribution is very complex and simplifications must be made in order to treat aerosols in global models. One common simplification is in the treatment of the partitioning of semi-volatile species (e.g. NH3, HNO3 and H2O) between the gas and the aerosol phases, which is often neglected in models or treated in a simplified manner. The treatment of partitioning is, however, important as it controls the aerosol composition (including the aerosol water concentration) as well as affecting the concentration of both aerosol and gas phase pollutants. This paper introduces the newly developed GMXe aerosol model, which has been developed to investigate gas / aerosol partitioning on a global scale. The model (implemented within the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model) combines an extended version of an established aerosol microphysics model (the M7, Stier et al ACP 2005) with a thermodynamic equilibrium model (EQSAM3, Metzger et al ACP 2008). The resulting model is capable of calculating gas / aerosol partitioning with relatively little additional computational overhead. In this paper we give an overview of the modelling approach used and show various model inter-comparisons, including a detailed comparison of the results of the GMXe and M7 models. We show the effect of including additional aerosol components - such as nitrate aerosol - on the global aerosol distribution and on the behaviour of other aerosol species (e.g. sulphate). The water uptake behaviour of the aerosol is examined, a factor that is important for the aerosol lifetime and also for the aerosol radiative forcing. We examine our results in the context of future emissions scenarios and air quality standards.

  5. Microheterogeneity in phenyl group modified inorganic/organic hybrid gels after aerosol drying or slow solvent evaporation.

    PubMed

    Ulke, Simone; Koller, Hubert

    2011-01-01

    Sol-gel systems were prepared by co-hydrolysis and co-condensation of tetraethoxysilane (TEOS) and phenyltriethoxysilane (PhTES). The sols were transferred into silica gels by Evaporation Induced Self-Assembly (EISA) or Aerosol Assisted Self-Assembly (AASA) using a laboratory spray-dryer. The structural properties such as porosity and homogeneity/microheterogeneity of these different systems are compared by N(2) sorption measurements, thermal analysis (TG, DTG and DTA), (29)Si MAS NMR and (29)Si{(1)H} CP MAS NMR. The cross polarization of the AASA gels can be described with the conventional I-S dynamics of a homogeneous proton spin bath. The EISA gels are heterogeneous, and the I-I(*)-S model, or a bimodal I-S model, was employed for the simulation of CP dynamics. Microheterogeneities are observed by (1)H-(29)Si cross polarization on an EISA sample, whereas rapid drying (AASA) transfers the corresponding sol into homogeneous xerogels. The EISA gels are microporous after calcination at 923 K, and the AASA gels are dense.

  6. Aerosol cluster impact and break-up : model and implementation.

    SciTech Connect

    Lechman, Jeremy B.

    2010-10-01

    In this report a model for simulating aerosol cluster impact with rigid walls is presented. The model is based on JKR adhesion theory and is implemented as an enhancement to the granular (DEM) package within the LAMMPS code. The theory behind the model is outlined and preliminary results are shown. Modeling the interactions of small particles is relevant to a number of applications (e.g., soils, powders, colloidal suspensions, etc.). Modeling the behavior of aerosol particles during agglomeration and cluster dynamics upon impact with a wall is of particular interest. In this report we describe preliminary efforts to develop and implement physical models for aerosol particle interactions. Future work will consist of deploying these models to simulate aerosol cluster behavior upon impact with a rigid wall for the purpose of developing relationships for impact speed and probability of stick/bounce/break-up as well as to assess the distribution of cluster sizes if break-up occurs. These relationships will be developed consistent with the need for inputs into system-level codes. Section 2 gives background and details on the physical model as well as implementations issues. Section 3 presents some preliminary results which lead to discussion in Section 4 of future plans.

  7. Dust in the Sky: Atmospheric Composition. Modeling of Aerosol Optical Thickness

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Kinne, Stefan; Torres, Omar; Holben, Brent; Duncan, Bryan; Martin, Randall; Logan, Jennifer; Higurashi, Akiko; Nakajima, Teruyuki

    2000-01-01

    Aerosol is any small particle of matter that rests suspended in the atmosphere. Natural sources, such as deserts, create some aerosols; consumption of fossil fuels and industrial activity create other aerosols. All the microscopic aerosol particles add up to a large amount of material floating in the atmosphere. You can see the particles in the haze that floats over polluted cities. Beyond this visible effect, aerosols can actually lower temperatures. They do this by blocking, or scattering, a portion of the sun's energy from reaching the surface. Because of this influence, scientists study the physical properties of atmospheric aerosols. Reliable numerical models for atmospheric aerosols play an important role in research.

  8. Modeling the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study using CMAQ-MADRID

    NASA Astrophysics Data System (ADS)

    Knipping, E. M.; Kumar, N.; Pun, B.; Wu, S.; Seigneur, C.

    2003-12-01

    A scientifically rigorous treatment of particulate matter within the framework of the Community Multiscale Air Quality (CMAQ) model is provided by CMAQ-MADRID (Model for Aerosol Dynamics, Reaction, Ionization, and Dissolution). CMAQ-MADRID is used to simulate the fate and transport of ambient gases and particulate matter (PM) during the Big Bend Regional Aerosol and Visibility Observational (BRAVO) study. The configuration of CMAQ-MADRID used for this study comprises the Regional Acid Deposition Mechanism v.2 (RADM2) gas-phase chemistry mechanism, a sectional PM solver incorporating the ISORROPIA inorganic thermodynamics module and the AER/EPRI/Caltech (AEC) secondary organic aerosol (SOA) module, and the Carnegie Mellon University (CMU) cloud chemistry module. Boundary conditions for gas- and particle-phase species are prescribed by an outer domain simulated using the Regional Modeling System for Aerosols and Deposition REMSAD (whose domain comprises most of North America). Sulfur dioxide (SO2) and particulate sulfate boundary conditions for the REMSAD domain are provided by the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation Transport (GOCART) model. Concentrations of sulfur dioxide and particulate sulfate at the CMAQ boundary are scaled to observations from monitoring stations of the Clean Air Status and Trends Network (CASTNet) and Interagency Monitoring of Protected Visual Environments (IMPROVE) network. The performance of CMAQ-MADRID is evaluated by comparing predictions with field measurements of the principal components contributing to visibility degradation: salts of ammonium with sulfate and nitrate, organic mass, elemental carbon and "other" particulate matter constituents, e.g. dust, sea salt and metal oxides. Model performance with respect to sulfate predictions, including model performance for its gas-phase precursor, sulfur dioxide, is explored across the thirty-seven stations comprising the BRAVO Network. The performance of CMAQ

  9. Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility

    NASA Astrophysics Data System (ADS)

    Zappoli, S.; Andracchio, A.; Fuzzi, S.; Facchini, M. C.; Gelencsér, A.; Kiss, G.; Krivácsy, Z.; Molnár, Á.; Mészáros, E.; Hansson, H.-C.; Rosman, K.; Zebühr, Y.

    A chemical mass balance of fine aerosol (<1.5 μm AED) collected at three European sites was performed with reference to the water solubility of the different aerosol classes of components. The sampling sites are characterised by different pollution conditions and aerosol loading in the air. Aspvreten is a background site in central Sweden, K-puszta is a rural site in the Great Hungarian Plain and San Pietro Capofiume is located in the polluted Po Valley, northern Italy. The average fine aerosol mass concentration was 5.9 μg m -3 at the background site Aspvreten, 24 μg m -3 at the rural K-puszta and 38 μg m -3 at the polluted site San Pietro Capofiume. However, a similarly high soluble fraction of the aerosol (65-75%) was measured at the three sites, while the percentage of water soluble organic species with respect to the total soluble mass was much higher at the background site (ca. 50%) than at the other two sites (ca. 25%). A very high fraction (over 70%) of organic compounds in the aerosol consisted of polar species. The presence of water soluble macromolecular compounds was revealed in the samples from K-puszta and San Pietro Capofiume. At both sites these species accounted for between ca. 20-50% of the water soluble organic fraction. The origin of the compounds was tentatively attributed to biomass combustion.

  10. Inorganic and carbonaceous aerosols during the Southern African Regional Science Initiative (SAFARI 2000) experiment: Chemical characteristics, physical properties, and emission data for smoke from African biomass burning

    NASA Astrophysics Data System (ADS)

    Formenti, P.; Elbert, W.; Maenhaut, W.; Haywood, J.; Osborne, S.; Andreae, M. O.

    2003-07-01

    We collected filter samples of the atmospheric aerosol during the Southern African Regional Science Initiative (SAFARI 2000) experiment onboard the UK Met Office C-130 aircraft. The main operational area was the Atlantic Ocean offshore of Namibia and Angola, where biomass-smoke haze at least 1-2 days old was widespread. The size-fractionated aerosol samples were analyzed for the major inorganic ions, carbonaceous material (elemental and organic carbon), and elements with atomic numbers between 11 (Na) and 82 (Pb). The regional haze aerosol was composed mostly of carbonaceous aerosols (on the average, 81% of the submicron mass), with secondary inorganic aerosols (sulfate, ammonium, and nitrate) accounting for another 14%. K+ and Cl-, typical pyrogenic species, constituted only 2% of the mass. The aerosol chemical data were used to estimate mass emission fluxes for various aerosol components. For African savanna/grassland burning, the estimated emission flux of carbonaceous particles (particulate organic matter plus elemental carbon) is 14 ± 1 Tg yr-1, and that of the nitrogen species (nitrate and ammonium) is 2 ± 2 Tg yr-1. For the flight segments in regional haze, the mean particle scattering coefficient at 550 nm was σs = 101 ± 56 Mm-1 and the mean particle absorption coefficient σa at 565 nm averaged 8 ± 5 Mm-1 (mean single scattering albedo of 0.93 ± 0.06 at 550 nm). The dry mass scattering efficiency αs, calculated from the linear regression of the mean scattering versus the estimated submicron mass, is estimated to be between 4.2 ± and 4.6 ± 0.6 m2 g-1, depending on the assumptions made in calculating the aerosol mass. The dependence of the scattering enhancement ratios Δσs/ΔCO on the distance from the burning regions suggests that the evolution of particle size with time influences the light scattering efficiency. Fresh smoke was sampled during a dedicated flight in the proximity and within the plume of an active biomass burning fire. Here the

  11. Sensitivity studies using Regional Atmospheric Modeling System to analyze the impact of dust and aerosol on precipitation in the Colorado River Basin

    NASA Astrophysics Data System (ADS)

    Jha, V.; Cotton, W. R.; Carrio, G. G.; Pierce, J. R.

    2015-12-01

    A modeling study is performed in the Colorado River Basin by varying the ratio of dust and aerosol pollution. The Colorado State University Regional Atmospheric Modeling system (RAMS) version 6.0 is used for the analyses with the aerosol and dust pollution data being nudged from the GEOS-Chem. RAMS was modified to ingest GEOS-CHEM output data and periodically update aerosol fields. GEOS-CHEM is a chemical transport model which uses assimilated meteorological data from the NASA Goddard Earth Observation System (GEOS). The aerosol data comprise a sum of hydrophobic and hydrophilic black carbon and organic aerosol, hydrophilic SOAs, hydrocarbon oxidation and inorganic aerosols (nitrate, sulfate and ammonium). In addition, a RAMS-based dust source and transport model is used. The sensitivity studies are 5 different kinds. The base study has both the dust and aerosol pollution data ON. The Case 2 has dust OFF with only the aerosol sources ON. The Case 3 has the aerosol sources ON with dust multiplied by a factor of 3. Case 4 has the aerosol sources ON with dust multiplied by a factor of 10. Case 5 and Case 6 are the simulations where dust can act only as CCN and only as IN respectively. It was found that the precipitation increases when dust is increased 3 times. However, the response is non-monotonic when dust is increased 10 times and the response depends on the environmental conditions. Dust acting as CCN acts in opposition to dust acting as IN. In general, dust acting as IN tends to enhance precipitation in wintertime orographic clouds.

  12. Detecting Aerosol Effect on Deep Precipitation Systems: A Modeling Study

    NASA Astrophysics Data System (ADS)

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

    2006-05-01

    Urban cities produce high concentrations of anthropogenic aerosols. These aerosols are generally hygroscopic and may serve as Cloud Condensation Nuclei (CCN). This study focuses on the aerosol indirect effect on the deep convective systems over the land. These deep convective systems contribute to the majority of the summer time rainfall and are important for local hydrological cycle and weather forecast. In a companion presentation (Tao et al.) in this session, the mechanisms of aerosol-cloud-precipitation interactions in deep convective systems are explored using cloud-resolving model simulations. Here these model results will be analyzed to provide guidance to the detection of the impact of aerosols as CCN on summer time, deep convections using the currently available observation methods. The two-dimensional Goddard Cumulus Ensemble (GCE) model with an explicit microphysical scheme has been used to simulate the aerosol effect on deep precipitation systems. This model simulates the size distributions of aerosol particles, as well as cloud, rain, ice crystals, snow, graupel, and hail explicitly. Two case studies are analyzed: a midlatitude summer time squall in Oklahoma, and a sea breeze convection in Florida. It is shown that increasing the CCN number concentration does not affect the rainfall structure and rain duration in these two cases. The total surface rainfall rate is reduced in the squall case, but remains essentially the same in the sea breeze case. For the long-lived squall system with a significant portion of the stratiform rain, the surface rainfall PDF (probability density function) distribution is more sensitive to the change of the initial CCN concentrations compared with the total surface rainfall. The possibility of detecting the aerosol indirect effect in deep precipitation systems from the space is also studied in this presentation. The hydrometeors fields from the GCE model simulations are used as inputs to a microwave radiative transfer model

  13. Incorporation of advanced aerosol activation treatments into CESM/CAM5: model evaluation and impacts on aerosol indirect effects

    NASA Astrophysics Data System (ADS)

    Gantt, B.; He, J.; Zhang, X.; Zhang, Y.; Nenes, A.

    2014-07-01

    One of the greatest sources of uncertainty in the science of anthropogenic climate change is from aerosol-cloud interactions. The activation of aerosols into cloud droplets is a direct microphysical linkage between aerosols and clouds; parameterizations of this process link aerosol with cloud condensation nuclei (CCN) and the resulting indirect effects. Small differences between parameterizations can have a large impact on the spatiotemporal distributions of activated aerosols and the resulting cloud properties. In this work, we incorporate a series of aerosol activation schemes into the Community Atmosphere Model version 5.1.1 within the Community Earth System Model version 1.0.5 (CESM/CAM5) which include factors such as insoluble aerosol adsorption and giant cloud condensation nuclei (CCN) activation kinetics to understand their individual impacts on global-scale cloud droplet number concentration (CDNC). Compared to the existing activation scheme in CESM/CAM5, this series of activation schemes increase the computation time by ~10% but leads to predicted CDNC in better agreement with satellite-derived/in situ values in many regions with high CDNC but in worse agreement for some regions with low CDNC. Large percentage changes in predicted CDNC occur over desert and oceanic regions, owing to the enhanced activation of dust from insoluble aerosol adsorption and reduced activation of sea spray aerosol after accounting for giant CCN activation kinetics. Comparison of CESM/CAM5 predictions against satellite-derived cloud optical thickness and liquid water path shows that the updated activation schemes generally improve the low biases. Globally, the incorporation of all updated schemes leads to an average increase in column CDNC of 150% and an increase (more negative) in shortwave cloud forcing of 12%. With the improvement of model-predicted CDNCs and better agreement with most satellite-derived cloud properties in many regions, the inclusion of these aerosol activation

  14. Easy Aerosol - Robust and non-robust circulation responses to aerosol radiative forcing in comprehensive atmosphere models

    NASA Astrophysics Data System (ADS)

    Voigt, Aiko; Bony, Sandrine; Stevens, Bjorn; Boucher, Olivier; Medeiros, Brian; Pincus, Robert; Wang, Zhili; Zhang, Kai; Lewinschal, Anna; Bellouin, Nicolas; Yang, Young-Min

    2015-04-01

    A number of recent studies illustrated the potential of aerosols to change the large-scale atmospheric circulation and precipitation patterns. It remains unclear, however, to what extent the proposed aerosol-induced changes reflect robust model behavior or are affected by uncertainties in the models' treatment of parametrized physical processes, such as those related to clouds. "Easy Aerosol", a model-intercomparison project organized within the Grand Challenge on Clouds, Circulation and Climate Sensitivity of the World Climate Research Programme, addresses this question by subjecting a suite of comprehensive atmosphere general circulation models with prescribed sea-surface temperatures (SSTs) to the same set of idealized "easy" aerosol perturbations. This contribution discusses the aerosol perturbations as well as their impact on the model's precipitation and surface winds. The aerosol perturbations are designed based on a global aerosol climatology and mimic the gravest mode of the anthropogenic aerosol. Specifically, the meridional and zonal distributions of total aerosol optical depth are approximated by a superposition of Gaussian plumes; the vertical distribution is taken as constant within the lowest 1250m of the atmosphere followed by an exponential decay with height above. The aerosol both scatters and absorbs shortwave radiation, but in order to focus on direct radiative effects aerosol-cloud interactions are omitted. Each model contributes seven simulations. A clean control case with no aerosol-radiative effects at all is compared to six perturbed simulations with differing aerosol loading, zonal aerosol distributions, and SSTs. To estimate the role of natural variability, one of the models, MPI-ESM, contributes a 5-member ensemble for each simulation. If the observed SSTs from years 1979-2005 are prescribed, the aerosol leads to a local depression of precipitation at the Northern Hemisphere center of the aerosol and a northward shift of the

  15. Model evaluation of marine primary organic aerosol emission schemes

    NASA Astrophysics Data System (ADS)

    Gantt, B.; Johnson, M. S.; Meskhidze, N.; Sciare, J.; Ovadnevaite, J.; Ceburnis, D.; O'Dowd, C. D.

    2012-09-01

    In this study, several marine primary organic aerosol (POA) emission schemes have been evaluated using the GEOS-Chem chemical transport model in order to provide guidance for their implementation in air quality and climate models. These emission schemes, based on varying dependencies of chlorophyll a concentration ([chl a]) and 10 m wind speed (U10), have large differences in their magnitude, spatial distribution, and seasonality. Model comparison with weekly and monthly mean values of the organic aerosol mass concentration at two coastal sites shows that the source function exclusively related to [chl a] does a better job replicating surface observations. Sensitivity simulations in which the negative U10 and positive [chl a] dependence of the organic mass fraction of sea spray aerosol are enhanced show improved prediction of the seasonality of the marine POA concentrations. A top-down estimate of submicron marine POA emissions based on the parameterization that compares best to the observed weekly and monthly mean values of marine organic aerosol surface concentrations has a global average emission rate of 6.3 Tg yr-1. Evaluation of existing marine POA source functions against a case study during which marine POA contributed the major fraction of submicron aerosol mass shows that none of the existing parameterizations are able to reproduce the hourly-averaged observations. Our calculations suggest that in order to capture episodic events and short-term variability in submicron marine POA concentration over the ocean, new source functions need to be developed that are grounded in the physical processes unique to the organic fraction of sea spray aerosol.

  16. A model for predicting fog aerosol size distributions

    NASA Astrophysics Data System (ADS)

    Rudiger, Joshua J.; Book, Kevin; Baker, Brooke; deGrassie, John Stephen; Hammel, Stephen

    2016-09-01

    An accurate model and parameterization of fog is needed to increase the reliability and usefulness of electro-optical systems in all relevant environments. Current models vary widely in their ability to accurately predict the size distribution and subsequent optical properties of fog. The Advanced Navy Aerosol Model (ANAM), developed to model the distribution of aerosols in the maritime environment, does not currently include a model for fog. One of the more prevalent methods for modeling particle size spectra consists of fitting a modified gamma function to fog measurement data. This limits the fog distribution to a single mode. Here we establish an empirical model for predicting complicated multimodal fog droplet size spectra using machine learning techniques. This is accomplished through careful measurements of fog in a controlled laboratory environment and measuring fog particle size distributions during outdoor fog events.

  17. Advancing Models and Evaluation of Cumulus, Climate and Aerosol Interactions

    SciTech Connect

    Gettelman, Andrew

    2015-10-27

    This project was successfully able to meet its’ goals, but faced some serious challenges due to personnel issues. Nonetheless, it was largely successful. The Project Objectives were as follows: 1. Develop a unified representation of stratifom and cumulus cloud microphysics for NCAR/DOE global community models. 2. Examine the effects of aerosols on clouds and their impact on precipitation in stratiform and cumulus clouds. We will also explore the effects of clouds and precipitation on aerosols. 3. Test these new formulations using advanced evaluation techniques and observations and release

  18. An Aerosol Physical Chemistry Model for the Upper Troposphere

    NASA Technical Reports Server (NTRS)

    Lin, Jin-Sheng

    2001-01-01

    This report is the final report for the Cooperative Agreement NCC2-1000. The tasks outlined in the various proposals are listed with a brief comment as to the research performed. The publications titles are: The effects of particle size and nitric acid uptake on the homogenous freezing of sulfate aerosols; Parameterization of an aerosol physical chemistry model (APCM) for the NH3/H2SO4/HNO3/H2O system at cold temperatures; and The onset, extent and duration of dehydration in the Southern Hemisphere polar vortex.

  19. 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

  20. Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model

    NASA Astrophysics Data System (ADS)

    Bergman, T.; Kerminen, V.-M.; Korhonen, H.; Lehtinen, K. J.; Makkonen, R.; Arola, A.; Mielonen, T.; Romakkaniemi, S.; Kulmala, M.; Kokkola, H.

    2011-12-01

    We present the implementation and evaluation of a sectional aerosol microphysics model SALSA within the aerosol-climate model ECHAM5-HAM. This aerosol microphysics module has been designed to be flexible and computationally efficient so that it can be implemented in regional or global scale models. The computational efficiency has been achieved by keeping the number of variables needed to describe the size and composition distribution to the minimum. The aerosol size distribution is described using 20 size sections with 10 size sections in size space which cover diameters ranging from 3 nm to 10 μm divided to three subranges each having distinct optimised process and compound selection. The ability of the module to describe the global aerosol properties was evaluated by comparison against (1) measured continental and marine size distributions, (2) observed variability of continental modal number concentrations, (3) measured sulphate, organic carbon, black carbon and sea salt mass concentrations, (4) observations of AOD and other aerosol optical properties from satellites and AERONET network, (5) global aerosol budgets and concentrations from previous model studies, and (6) model results using M7 which is the default aerosol microphysics module in ECHAM5-HAM. The evaluation shows that the global aerosol properties can be reproduced reasonably well using the coarse resolution of 10 size sections in size space. The simulated global aerosol budgets are within the range of previous studies. Surface concentrations of sea salt, sulphate and carbonaceous species have an annual mean within a factor of five of the observations, while the simulated sea salt concentrations reproduce the observations less accurately and show high variability. Regionally, AOD is in relatively good agreement with the observations (within a factor of two). At mid-latitudes the observed AOD is captured well, while at high-latitudes as well as in some polluted and dust regions the modeled AOD is

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

    NASA Astrophysics Data System (ADS)

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

    2014-04-01

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

  2. High Resolution Aerosol Modeling: Decadal Changes in Radiative Forcing

    SciTech Connect

    Bergmann, D J; Chuang, C C; Govindasamy, B; Cameron-Smith, P J; Rotman, D A

    2005-02-01

    The Atmospheric Science Division of LLNL has performed high-resolution calculations of direct sulfate forcing using a DOE-provided computer resource at NERSC. We integrated our global chemistry-aerosol model (IMPACT) with the LLNL high-resolution global climate model (horizontal resolution as high as 100 km) to examine the temporal evolution of sulfate forcing since 1950. We note that all previous assessments of sulfate forcing reported in IPCC (2001) were based on global models with coarse spatial resolutions ({approx} 300 km or even coarser). However, the short lifetime of aerosols ({approx} days) results in large spatial and temporal variations of radiative forcing by sulfate. As a result, global climate models with coarse resolutions do not accurately simulate sulfate forcing on regional scales. It requires much finer spatial resolutions in order to address the effects of regional anthropogenic SO{sub 2} emissions on the global atmosphere as well as the effects of long-range transport of sulfate aerosols on the regional climate forcing. By taking advantage of the tera-scale computer resources at NERSC, we simulated the historic direct sulfate forcing at much finer spatial resolutions than ever attempted before. Furthermore, we performed high-resolution chemistry simulations and saved monthly averaged oxidant fields, which will be used in subsequent simulations of sulfate aerosol formation and their radiative impact.

  3. An Aerosolized Brucella spp. Challenge Model for Laboratory Animals

    Technology Transfer Automated Retrieval System (TEKTRAN)

    To characterize the optimal aerosol dosage of Brucella abortus strain 2308 (S2308) and B. melitensis (S16M) in a laboratory animal model of brucellosis, dosages of 10**3 to 10**10 CFU were nebulized to mice. Although tissue weights were minimally influenced, total colony-forming units (CFU) per tis...

  4. Modeling aerosol surface chemistry and gas-particle interaction kinetics with K2-SURF: PAH oxidation

    NASA Astrophysics Data System (ADS)

    Shiraiwa, M.; Garland, R.; Pöschl, U.

    2009-04-01

    Atmospheric aerosols are ubiquitous in the atmosphere. They have the ability to impact cloud properties, radiative balance and provide surfaces for heterogeneous reactions. The uptake of gaseous species on aerosol surfaces impacts both the aerosol particles and the atmospheric budget of trace gases. These subsequent changes to the aerosol can in turn impact the aerosol chemical and physical properties. However, this uptake, as well as the impact on the aerosol, is not fully understood. This uncertainty is due not only to limited measurement data, but also a dearth of comprehensive and applicable modeling formalizations used for the analysis, interpretation and description of these heterogeneous processes. Without a common model framework, comparing and extrapolating experimental data is difficult. In this study, a novel kinetic surface model (K2-SURF) [Ammann & Pöschl, 2007; Pöschl et al., 2007] was used to describe the oxidation of a variety of polycyclic aromatic hydrocarbons (PAHs). Integrated into this consistent and universally applicable kinetic and thermodynamic process model are the concepts, terminologies and mathematical formalizations essential to the description of atmospherically relevant physicochemical processes involving organic and mixed organic-inorganic aerosols. Within this process model framework, a detailed master mechanism, simplified mechanism and parameterizations of atmospheric aerosol chemistry are being developed and integrated in analogy to existing mechanisms and parameterizations of atmospheric gas-phase chemistry. One of the key aspects to this model is the defining of a clear distinction between various layers of the particle and surrounding gas phase. The processes occurring at each layer can be fully described using known fluxes and kinetic parameters. Using this system there is a clear separation of gas phase, gas-surface and surface bulk transport and reactions. The partitioning of compounds can be calculated using the flux

  5. Simulating Aerosol Indirect Effects with Improved Aerosol-Cloud- Precipitation Representations in a Coupled Regional Climate Model

    SciTech Connect

    Zhang, Yang; Leung, L. Ruby; Fan, Jiwen

    2016-04-27

    This is a collaborative project among North Carolina State University, Pacific Northwest National Laboratory, and Scripps Institution of Oceanography, University of California at San Diego to address the critical need for an accurate representation of aerosol indirect effect in climate and Earth system models. In this project, we propose to develop and improve parameterizations of aerosol-cloud-precipitation feedbacks in climate models and apply them to study the effect of aerosols and clouds on radiation and hydrologic cycle. Our overall objective is to develop, improve, and evaluate parameterizations to enable more accurate simulations of these feedbacks in high resolution regional and global climate models.

  6. Aerosol cloud processing with the global model ECHAM5-HAM-SALSA

    NASA Astrophysics Data System (ADS)

    Bergman, T.; Korhonen, H.; Zubair, M.; Romakkaniemi, S.; Lehtinen, K.; Kokkola, H.

    2012-04-01

    Atmospheric aerosols and their interactions with clouds constitute the largest uncertainty in the radiative forcing of the Earth's atmosphere. Increasing aerosol number concentrations increases the cloud droplet concentration and droplet surface and hence the cloud albedo. This mechanism is called the aerosol indirect effect on climate. Understanding the changes in cloud droplet number concentrations and size by anthropogenic aerosols are the key factors in the study of future climate change. Therefore the aerosols' formation and growth from nanoparticles to cloud condensation nuclei (CCN) must be described accurately. The formation and growth of aerosols are shown to be described more accurately with sectional representations than with bulk (total aerosol mass only), modal (lognormal modes describing mass and number size distribution) or moment (processes tied to different moments of particle number size distribution) approaches. Recently the sectional aerosol models have been implemented to global climate models. However, the resolution of sectional models must be optimised to reduce the computational cost. We have implemented the sectional aerosol model SALSA in ECHAM5-HAM. SALSA describes the aerosol population with 20 size sections. The dynamics are optimised for large scale applications and the model includes an improved moving center sectional method. The particulate mass consists of five compounds: sulphate, organic carbon, black carbon, sea salt and dust. The aerosol processing has been studied extensively and there are many numerical models used to predict CCN number concentrations. However, due to computational limitations many of them are not suitable for utilisation in global climate models. Therefore in most global climate studies on aerosol activation to CCN is examined using cloud activation parameterisations. We study the aerosol cloud processing and its affect on transport of aerosols using Abdul-Razzak-Ghan aerosol cloud activation

  7. On the implications of aerosol liquid water and phase ...

    EPA Pesticide Factsheets

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were hig

  8. LES Modeling of Aerosol and Drizzle Effects in Marine Stratocumulus

    DTIC Science & Technology

    2001-09-30

    research is based on the CIMMS LES model of boundary layer stratocumulus clouds with explicit formulation of aerosol and drop size-resolving...rates calculated from the CIMMS explicit microphysics LES model. The errors of parameterized expressions are an order of magnitude less than...framework of the CIMMS LES model where the errors of the parameterization can be assessed in a more realistic setting. The performance of the

  9. Impact of aging mechanism on model simulated carbonaceous aerosols

    PubMed Central

    Huang, Y.; Wu, S.; Dubey, M.K.; French, N. H. F.

    2013-01-01

    Carbonaceous aerosols including organic carbon and black carbon have significant implications for both climate and air quality. In the current global climate or chemical transport models, a fixed hydrophobic-to-hydrophilic conversion lifetime for carbonaceous aerosol (τ) is generally assumed, which is usually around one day. We have implemented a new detailed aging scheme for carbonaceous aerosols in a chemical transport model (GEOS-Chem) to account for both the chemical oxidation and the physical condensation-coagulation effects, where τ is affected by local atmospheric environment including atmospheric concentrations of water vapor, ozone, hydroxyl radical and sulfuric acid. The updated τ exhibits large spatial and temporal variations with the global average (up to 11 km altitude) calculated to be 2.6 days. The chemical aging effects are found to be strongest over the tropical regions driven by the low ozone concentrations and high humidity there. The τ resulted from chemical aging generally decreases with altitude due to increases in ozone concentration and decreases in humidity. The condensation-coagulation effects are found to be most important for the high-latitude areas, in particular the polar regions, where the τ values are calculated to be up to 15 days. When both the chemical aging and condensation-coagulation effects are considered, the total atmospheric burdens and global average lifetimes of BC, black carbon, (OC, organic carbon) are calculated to increase by 9% (3%) compared to the control simulation, with considerable enhancements of BC and OC concentrations in the Southern Hemisphere. Model evaluations against data from multiple datasets show that the updated aging scheme improves model simulations of carbonaceous aerosols for some regions, especially for the remote areas in the Northern Hemisphere. The improvement helps explain the persistent low model bias for carbonaceous aerosols in the Northern Hemisphere reported in literature. Further

  10. MATRIX-VBS (v1.0): implementing an evolving organic aerosol volatility in an aerosol microphysics model

    NASA Astrophysics Data System (ADS)

    Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

    2017-02-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  11. MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

    NASA Technical Reports Server (NTRS)

    Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

    2017-01-01

    The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

  12. Trace Gas/Aerosol Interactions and GMI Modeling Support

    NASA Technical Reports Server (NTRS)

    Penner, Joyce E.; Liu, Xiaohong; Das, Bigyani; Bergmann, Dan; Rodriquez, Jose M.; Strahan, Susan; Wang, Minghuai; Feng, Yan

    2005-01-01

    Current global aerosol models use different physical and chemical schemes and parameters, different meteorological fields, and often different emission sources. Since the physical and chemical parameterization schemes are often tuned to obtain results that are consistent with observations, it is difficult to assess the true uncertainty due to meteorology alone. Under the framework of the NASA global modeling initiative (GMI), the differences and uncertainties in aerosol simulations (for sulfate, organic carbon, black carbon, dust and sea salt) solely due to different meteorological fields are analyzed and quantified. Three meteorological datasets available from the NASA DAO GCM, the GISS-II' GCM, and the NASA finite volume GCM (FVGCM) are used to drive the same aerosol model. The global sulfate and mineral dust burdens with FVGCM fields are 40% and 20% less than those with DAO and GISS fields, respectively due to its heavier rainfall. Meanwhile, the sea salt burden predicted with FVGCM fields is 56% and 43% higher than those with DAO and GISS, respectively, due to its stronger convection especially over the Southern Hemispheric Ocean. Sulfate concentrations at the surface in the Northern Hemisphere extratropics and in the middle to upper troposphere differ by more than a factor of 3 between the three meteorological datasets. The agreement between model calculated and observed aerosol concentrations in the industrial regions (e.g., North America and Europe) is quite similar for all three meteorological datasets. Away from the source regions, however, the comparisons with observations differ greatly for DAO, FVGCM and GISS, and the performance of the model using different datasets varies largely depending on sites and species. Global annual average aerosol optical depth at 550 nm is 0.120-0.131 for the three meteorological datasets.

  13. A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation

    NASA Astrophysics Data System (ADS)

    Hossaini, Ryan; Chipperfield, Martyn P.; Saiz-Lopez, Alfonso; Fernandez, Rafael; Monks, Sarah; Feng, Wuhu; Brauer, Peter; Glasow, Roland

    2016-12-01

    Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth's troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by 2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5 × 104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to 4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of 12-13 Tg CH4/yr due the CH4 + Cl reaction ( 2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for 10 to >20% of total boundary layer CH4 oxidation in some locations.

  14. Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model

    NASA Astrophysics Data System (ADS)

    Bergman, T.; Kerminen, V.-M.; Korhonen, H.; Lehtinen, K. J.; Makkonen, R.; Arola, A.; Mielonen, T.; Romakkaniemi, S.; Kulmala, M.; Kokkola, H.

    2012-06-01

    We present the implementation and evaluation of a sectional aerosol microphysics module SALSA within the aerosol-climate model ECHAM5-HAM. This aerosol microphysics module has been designed to be flexible and computationally efficient so that it can be implemented in regional or global scale models. The computational efficiency has been achieved by minimising the number of variables needed to describe the size and composition distribution. The aerosol size distribution is described using 10 size classes with parallel sections which can have different chemical compositions. Thus in total, the module tracks 20 size sections which cover diameters ranging from 3 nm to 10 μm and are divided into three subranges, each with an optimised selection of processes and compounds. The implementation of SALSA into ECHAM5-HAM includes the main aerosol processes in the atmosphere: emissions, removal, radiative effects, liquid and gas phase sulphate chemistry, and the aerosol microphysics. The aerosol compounds treated in the module are sulphate, organic carbon, sea salt, black carbon, and mineral dust. In its default configuration, ECHAM5-HAM treats aerosol size distribution using the modal method. In this implementation, the aerosol processes were converted to be used in a sectional model framework. The ability of the module to describe the global aerosol properties was evaluated by comparing against (1) measured continental and marine size distributions, (2) observed variability of continental number concentrations, (3) measured sulphate, organic carbon, black carbon and sea-salt mass concentrations, (4) observations of aerosol optical depth (AOD) and other aerosol optical properties from satellites and AERONET network, (5) global aerosol budgets and concentrations from previous model studies, and (6) model results using M7, which is the default aerosol microphysics module in ECHAM5-HAM. The evaluation shows that the global aerosol properties can be reproduced reasonably well

  15. High Contributions of Secondary Inorganic Aerosols to PM2.5 under Polluted Levels at a Regional Station in Northern China

    PubMed Central

    Li, Yang; Tao, Jun; Zhang, Leiming; Jia, Xiaofang; Wu, Yunfei

    2016-01-01

    Daily PM2.5 samples were collected at Shangdianzi (SDZ) regional site in Beijing–Tianjin–Hebei (BTH) region in 2015. Samples were subject to chemical analysis for organic carbon (OC), elemental carbon (EC), and major water-soluble inorganic ions. The annual average PM2.5 mass concentration was 53 ± 36 μg·m−3 with the highest seasonal average concentration in spring and the lowest in summer. Water-soluble inorganic ions and carbonaceous aerosols accounted for 34% ± 15% and 33% ± 9%, respectively, of PM2.5 mass on annual average. The excellent, good, lightly polluted, moderately polluted, and heavily polluted days based on the Air Quality Index (AQI) of PM2.5 accounted for 40%, 42%, 11%, 4%, and 3%, respectively, of the year. The sum of the average concentration of sulfate, nitrate, and ammonium (SNA) increased from 4.2 ± 2.9 μg·m−3 during excellent days to 85.9 ± 22.4 μg·m−3 during heavily polluted days, and their contributions to PM2.5 increased from 15% ± 8% to 49% ± 10% accordingly. In contrast, the average concentration of carbonaceous aerosols increased from 9.2 ± 2.8 μg·m−3 to 51.2 ± 14.1 μg·m−3, and their contributions to PM2.5 decreased from 34% ± 6% to 29% ± 7%. Potential source contribution function (PSCF) analysis revealed that the major sources for high PM2.5 and its dominant chemical components were within the area mainly covering Shandong, Henan, and Hebei provinces. Regional pollutant transport from Shanxi province and Inner Mongolia autonomous region located in the west direction of SDZ was also important during the heating season. PMID:27983711

  16. On the relationship between aerosol model uncertainty and radiative forcing uncertainty

    PubMed Central

    Reddington, Carly L.; Carslaw, Kenneth S.

    2016-01-01

    The largest uncertainty in the historical radiative forcing of climate is caused by the interaction of aerosols with clouds. Historical forcing is not a directly measurable quantity, so reliable assessments depend on the development of global models of aerosols and clouds that are well constrained by observations. However, there has been no systematic assessment of how reduction in the uncertainty of global aerosol models will feed through to the uncertainty in the predicted forcing. We use a global model perturbed parameter ensemble to show that tight observational constraint of aerosol concentrations in the model has a relatively small effect on the aerosol-related uncertainty in the calculated forcing between preindustrial and present-day periods. One factor is the low sensitivity of present-day aerosol to natural emissions that determine the preindustrial aerosol state. However, the major cause of the weak constraint is that the full uncertainty space of the model generates a large number of model variants that are equally acceptable compared to present-day aerosol observations. The narrow range of aerosol concentrations in the observationally constrained model gives the impression of low aerosol model uncertainty. However, these multiple “equifinal” models predict a wide range of forcings. To make progress, we need to develop a much deeper understanding of model uncertainty and ways to use observations to constrain it. Equifinality in the aerosol model means that tuning of a small number of model processes to achieve model−observation agreement could give a misleading impression of model robustness. PMID:26848136

  17. Optical modeling of aerosol extinction for remote sensing in the marine environment

    NASA Astrophysics Data System (ADS)

    Kaloshin, G. A.

    2013-05-01

    A microphysical model is presented for the surface layer marine and coastal atmospheric aerosols that is based on long-term observations of size distributions for 0.01-100 μm particles in different geographic sites. The fundamental feature of the model is a parameterization of amplitudes and widths for aerosol modes of the aerosol size distribution function (ASDF) as functions of fetch and wind speed. The shape of the ASDF and its dependence on meteorological parameters, altitudes above sea level (H), fetch (X), wind speed (U) and relative humidity (RH) are investigated. The spectral profiles of the aerosol extinction coefficients calculated by MaexPro (Marine Aerosol Extinction Profiles) are in good agreement with observational data and the numerical results obtained from the Navy Aerosol Model (NAM) and the Advanced Navy Aerosol Model (ANAM). Moreover, MaexPro was found to be an accurate and reliable tool for investigation of the optical properties of atmospheric aerosols.

  18. Modeling the Role of Alkanes, Polycyclic Aromatic Hydrocarbons, and Their Oligomers in Secondary Organic Aerosol Formation

    EPA Science Inventory

    A computationally efficient method to treat secondary organic aerosol (SOA) from various length and structure alkanes as well as SOA from polycyclic aromatic hydrocarbons (PAHs) is implemented in the Community Multiscale Air Quality (CMAQ) model to predict aerosol concentrations ...

  19. Lessons Learned About Organic Aerosol Formation in the Southeast U.S. Using Observations and Modeling

    EPA Science Inventory

    Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA). In this work, modeling of isoprene SOA via heterogeneous uptake is explored and compared to observations from the Southern Oxidant and Aerosol Study (SOAS).

  20. Measurement of Organic and Inorganic Chemical Tracers for Source Apportionment of Tropospheric Aerosols Collected During the ACE-Asia Experiment

    NASA Astrophysics Data System (ADS)

    Schauer, J. J.; Park, J.; Duvall, R.; Bae, M.; Shafer, M. M.; Chuang, P.; Chuang, P.; Kim, Y. J.

    2001-12-01

    Naturally occurring dust and anthropogenic air pollutants are important contributors to tropospheric aerosols and impact air quality and the radiative balance of the Earth's atmosphere. In order to better understand the relationship between the origin, chemical composition and ultimate impact of Asian aerosols on climate forcing, aerosol samples were collected as part of the ACE-Asia experiment for detailed chemical analysis. Atmospheric particulate matter samples were collected from March 27, 2001 through May 6, 2001 at the ACE-Asia ground station located on Cheju Island, Korea. During this period, this region is impacted by anthropogenic air pollution emissions from highly urbanized region of Asia and by desert dust originating from northeastern Asia. As part of the experiment, atmospheric particulate matter samplers were also collected in urban and desert locations in Asia that represent regional sources of particulate matter in Asia. Size resolved aerosol samples were analyzed for trace metals by using microwave assisted-acid digestion and ICP-MS analysis, speciated organic compounds using solvent extraction and GC-MS analysis, as well as soluble ions and elemental and organic carbon (ECOC). These measurements provide fingerprints for source apportionment of the atmospheric particulate matter samples collected at the Cheju Island sampling site. The use of these chemical tracers for apportionment of wind-driven long range transported desert dust, local crustal derived dust, biogenically and anthropogenically derived sulfate, specific urban combustion source, and fossil fuel combustion will be presented.

  1. An automated analyzer to measure surface-atmosphere exchange fluxes of water soluble inorganic aerosol compounds and reactive trace gases.

    PubMed

    Thomas, Rick M; Trebs, Ivonne; Otjes, René; Jongejan, Piet A C; Ten Brink, Harry; Phillips, Gavin; Kortner, Michael; Meixner, Franz X; Nemitz, Eiko

    2009-03-01

    Here, we present a new automated instrument for semicontinuous gradient measurements of water-soluble reactive trace gas species (NH3, HNO3, HONO, HCl, and SO2) and their related aerosol compounds (NH4+, NO3-, Cl-, SO4(2-)). Gas and aerosol samples are collected simultaneously at two heights using rotating wet-annular denuders and steam-jet aerosol collectors, respectively. Online (real-time) analysis using ion chromatography (IC) for anions and flow injection analysis (FIA) for NH4+ and NH3 provide a half-hourly averaged gas and aerosol gradients within each hour. Through the use of syringe pumps, IC preconcentration columns, and high-quality purified water, the system achieves detection limits (3sigma-definition) under field conditions of typically: 136/207,135/114, 29/ 22,119/92, and 189/159 ng m(-3) for NH3/NH4+, HNO3/NO3-, HONO/ NO2-, HCl/Cl- and SO2/SO4(2-), respectively. The instrument demonstrates very good linearity and accuracy for liquid and selected gas phase calibrations over typical ambient concentration ranges. As shown by examples from field experiments, the instrument provides sufficient precision (3-9%), even at low ambient concentrations, to resolve vertical gradients and calculate surface-atmosphere exchange fluxes undertypical meteorological conditions of the atmospheric surface layer using the aerodynamic gradient technique.

  2. Organic and inorganic aerosol compositions in Ulaanbaatar, Mongolia, during the cold winter of 2007 to 2008: Dicarboxylic acids, ketocarboxylic acids, and α-dicarbonyls

    NASA Astrophysics Data System (ADS)

    Jung, Jinsang; Tsatsral, Batmunkh; Kim, Young J.; Kawamura, Kimitaka

    2010-11-01

    To investigate the distributions and sources of water-soluble organic acids in the Mongolian atmosphere, aerosol samples (PM2.5, n = 34) were collected at an urban site (47.92°N, 106.90°E, ˜1300 m above sea level) in Ulaanbaatar, the capital of Mongolia, during the cold winter. The samples were analyzed for water-soluble dicarboxylic acids (C2-C12) and related compounds (ketocarboxylic acids and α-dicarbonyls), as well as organic carbon (OC), elemental carbon, water-soluble OC, and inorganic ions. Distributions of dicarboxylic acids and related compounds were characterized by a predominance of terephthalic acid (tPh; 130 ± 51 ng m-3, 19% of total detected organic acids) followed by oxalic (107 ± 28 ng m-3, 15%), succinic (63 ± 20 ng m-3, 9%), glyoxylic (55 ± 18 ng m-3, 8%), and phthalic (54 ± 27 ng m-3, 8%) acids. Predominance of terephthalic acid, which has not been reported previously in atmospheric aerosols, was mainly due to uncontrolled burning of plastic bottles and bags in home stoves for heating and waste incineration during the cold winter. This study demonstrated that most of the air pollutants were directly emitted from local sources such as heat and power plants, home stoves, and automobiles. Development of an inversion layer (<700 m above ground level) over the basin of Ulaanbaatar accelerated the accumulation of pollutants, causing severe haze episodes during the winter season.

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

    NASA Technical Reports Server (NTRS)

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

    1995-01-01

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

  4. Dicarboxylic acids, ω-oxocarboxylic acids, α-dicarbonyls, WSOC, OC, EC, and inorganic ions in wintertime size-segregated aerosols from central India: Sources and formation processes.

    PubMed

    Deshmukh, Dhananjay K; Kawamura, Kimitaka; Deb, Manas K

    2016-10-01

    The size distributions of aerosols can provide evidences for their sources and formation processes in the atmosphere. Size-segregated aerosols (9-sizes) were collected in urban site (Raipur: 21.2°N and 82.3°E) in central India during winter of 2012-2013. The samples were analyzed for dicarboxylic acids (C2-C12), ω-oxocarboxylic acids (ωC2-ωC9), pyruvic acid and α-dicarbonyls (C2-C3) as well as elemental carbon (EC), organic carbon (OC), water-soluble OC (WSOC) and inorganic ions. Diacids showed a predominance of oxalic acid (C2) followed by succinic and azelaic acid whereas ω-oxoacids exhibited a predominance of glyoxylic acid and glyoxal was more abundant than methylglyoxal in all the sizes. Diacids, ω-oxoacids and α-dicarbonyls showed bimodal size distribution with peaks in fine and coarse modes. High correlations of fine mode diacids and related compounds with potassium and levoglucosan suggest that they were presumably due to a substantial contribution of primary emission from biomass burning and secondary production from biomass burning derived precursors. High correlations of C2 with higher carbon number diacids (C3-C9) suggest that they have similar sources and C2 may be produced via the decay of its higher homologous diacids in fine mode. Considerable portions of diacids and related compounds in coarse mode suggest that they were associated with mineral dust particles by their adsorption and photooxidation of anthropogenic and biogenic precursors via heterogeneous reaction on dust surface. This study demonstrates that biomass burning and dust particles are two major factors to control the size distribution of diacids and related compounds in the urban aerosols from central India.

  5. Modeling the Explicit Chemistry of Anthropogenic and Biogenic Organic Aerosols

    SciTech Connect

    Madronich, Sasha

    2015-12-09

    The atmospheric burden of Secondary Organic Aerosols (SOA) remains one of the most important yet uncertain aspects of the radiative forcing of climate. This grant focused on improving our quantitative understanding of SOA formation and evolution, by developing, applying, and improving a highly detailed model of atmospheric organic chemistry, the Generation of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) model. Eleven (11) publications have resulted from this grant.

  6. Sensitivity of Remote Aerosol Distributions to Representation of Cloud-Aerosol Interactions in a Global Climate Model

    SciTech Connect

    Wang, Hailong; Easter, Richard C.; Rasch, Philip J.; Wang, Minghuai; Liu, Xiaohong; Ghan, Steven J.; Qian, Yun; Yoon, Jin-Ho; Ma, Po-Lun; Vinoj, V.

    2013-06-05

    Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5), have large biases in predicting aerosols in remote regions such as upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol-climate model (PNNL-MMF) that explicitly represents convection and aerosol-cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC) due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the sub-grid scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a10-fold (5-fold) increase in the winter (summer) months, resulting in a much better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold) increase in

  7. Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multi-layer model ADCHAM

    NASA Astrophysics Data System (ADS)

    Roldin, P.; Eriksson, A. C.; Nordin, E. Z.; Hermansson, E.; Mogensen, D.; Rusanen, A.; Boy, M.; Swietlicki, E.; Svenningsson, B.; Zelenyuk, A.; Pagels, J.

    2014-01-01

    We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas phase Master Chemical Mechanism version 3.2, an aerosol dynamics and particle phase chemistry module (which considers acid catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study: (1) the mass transfer limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), (2) the slow and almost particle size independent evaporation of α-pinene secondary organic aerosol (SOA) particles, and (3) the influence of chamber wall effects on the observed SOA formation in smog chambers. ADCHAM is able to capture the observed α-pinene SOA mass increase in the presence of NH3(g). Organic salts of ammonium and carboxylic acids predominantly form during the early stage of SOA formation. These salts contribute substantially to the initial growth of the homogeneously nucleated particles. The model simulations of evaporating α-pinene SOA particles support the recent experimental findings that these particles have a semi-solid tar like amorphous phase state. ADCHAM is able to reproduce the main features of the observed slow evaporation rates if low-volatility and viscous oligomerized SOA material accumulates in the particle surface layer upon evaporation. The evaporation rate is mainly governed by the reversible decomposition of oligomers back to monomers. Finally, we demonstrate that the mass transfer limited uptake of condensable organic compounds onto wall deposited particles or directly onto the Teflon chamber walls of smog chambers can have profound influence on the

  8. MIRAGE: Model Description and Evaluation of Aerosols and Trace Gases

    SciTech Connect

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

    2004-10-27

    The MIRAGE (Model for Integrated Research on Atmospheric Global Exchanges) modeling system, designed to study the impacts of anthropogenic aerosols on the global environment, is described. MIRAGE consists of a chemical transport model coupled on line with a global climate model. The chemical transport model simulates trace gases, aerosol number, and aerosol chemical component mass [sulfate, MSA, organic matter, black carbon (BC), sea salt, mineral dust] for four aerosol modes (Aitken, accumulation, coarse sea salt, coarse mineral dust) using the modal aerosol dynamics approach. Cloud-phase and interstitial aerosol are predicted separately. The climate model, based on the CCM2, has physically-based treatments of aerosol direct and indirect forcing. Stratiform cloud water and droplet number are simulated using a bulk microphysics parameterization that includes aerosol activation. Aerosol and trace gas species simulated by MIRAGE are presented and evaluated using surface and aircraft measurements. Surface-level SO2 in N. American and European source regions is higher than observed. SO2 above the boundary layer is in better agreement with observations, and surface-level SO2 at marine locations is somewhat lower than observed. Comparison with other models suggests insufficient SO2 dry deposition; increasing the deposition velocity improves simulated SO2. Surface-level sulfate in N. American and European source regions is in good agreement with observations, although the seasonal cycle in Europe is stronger than observed. Surface-level sulfate at high-latitude and marine locations, and sulfate above the boundary layer, are higher than observed. This is attributed primarily to insufficient wet removal; increasing the wet removal improves simulated sulfate at remote locations and aloft. Because of the high sulfate bias, radiative forcing estimates for anthropogenic sulfur in Ghan et al. [2001c] are probably too high. Surface-level DMS is {approx}40% higher than observed

  9. Mass-based hygroscopicity parameter interaction model and measurement of atmospheric aerosol water uptake

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Merkulov, V.; Vlasenko, S.; Rose, D.; Pöschl, U.

    2011-11-01

    In this study we derive and apply a mass-based hygroscopicity parameter interaction model for efficient description of concentration-dependent water uptake by atmospheric aerosol particles. The model approach builds on the single hygroscopicity parameter model of Petters and Kreidenweis (2007). We introduce an observable mass-based hygroscopicity parameter κm, which can be deconvoluted into a dilute intrinsic hygroscopicity parameter (κm,∞) and additional self- and cross-interaction parameters describing non-ideal solution behavior and concentration dependencies of single- and multi-component systems. For sodium chloride, the κm-interaction model (KIM) captures the observed concentration and humidity dependence of the hygroscopicity parameter and is in good agreement with an accurate reference model based on the Pitzer ion-interaction approach (Aerosol Inorganic Model, AIM). For atmospheric aerosol samples collected from boreal rural air and from pristine tropical rainforest air (secondary organic aerosol) we present first mass-based measurements of water uptake over a wide range of relative humidity (1-99%) obtained with a new filter-based differential hygroscopicity analyzer (FDHA) technique. By application of KIM to the measurement data we can distinguish three different regimes of hygroscopicity in the investigated aerosol samples: (I) A quasi-eutonic regime at low relative humidity (~60% RH) where the solutes co-exist in an aqueous and non-aqueous phase; (II) a gradually deliquescent regime at intermediate humidity (~60%-90% RH) where different solutes undergo gradual dissolution in the aqueous phase; and (III) a dilute regime at high humidity (≳90% RH) where the solutes are fully dissolved approaching their dilute intrinsic hygroscopicity. The characteristic features of the three hygroscopicity regimes are similar for both samples, while the RH threshold values vary as expected for samples of different chemical composition. In each regime, the

  10. Evaluation of the modal aerosol model GMXe in the chemistry-climate model GEM-AC

    NASA Astrophysics Data System (ADS)

    Semeniuk, K.; Lupu, A.; Kaminski, J. W.; McConnell, J. C.; O'Neill, N. T.; Tost, H.

    2012-12-01

    We evaluate a modal aerosol model, GMXe, implemented in the atmospheric chemistry-climate model GEM-AC, against global ground-based observations of optical depths and speciated aerosol concentrations. The Global Environmental Multiscale Atmospheric Chemistry model (GEM-AC) is a global, tropospheric-stratospheric chemistry, general circulation model based on the GEM model developed by the Meteorological Service of Canada for operational weather forecasting. Gas-phase chemistry consists in detailed reactions of Ox, NOx, HOx, CO, CH4, NMVOCs, ClOx and BrOx. Tracers are advected using the semi-Lagrangian scheme native to GEM. The vertical transport includes parameterized subgrid scale turbulence and deep convection. Dry deposition is implemented as a flux boundary condition in the vertical diffusion equation. Wet removal comprises both in-cloud and below-cloud scavenging. The Global Modal-aerosol eXtension (GMXe) handles aerosol microphysics and gas-aerosol partitioning. The aerosol size distribution is described by the superposition of 4 hydrophilic and 3 hydrophobic interacting lognormal modes (nucleation, Aitken, accumulation and coarse). Aerosol dynamics includes nucleation, coagulation, and condensation/evaporation. Gas-aerosol partitioning is calculated by the thermodynamic equilibrium model ISORROPIA. The model was run for one year on a 1.5°×1.5° global grid with 73 hybrid levels from the surface to 0.15 hPa. We used aerosol emissions for year 2000 from AeroCom I. The output is compared with aerosol optical depth observations from AERONET, and with measured surface concentrations of sulfate, nitrate and ammonium from CASTNET, EMEP and EANET.

  11. MODELING THE FORMATION OF SECONDARY ORGANIC AEROSOL WITHIN A COMPREHENSIVE AIR QUALITY MODEL SYSTEM

    EPA Science Inventory

    The aerosol component of the CMAQ model is designed to be an efficient and economical depiction of aerosol dynamics in the atmosphere. The approach taken represents the particle size distribution as the superposition of three lognormal subdistributions, called modes. The proces...

  12. Evaluation of Aerosol-Cloud Interactions in GISS ModelE Using ASR Observations

    NASA Astrophysics Data System (ADS)

    de Boer, G.; Menon, S.; Bauer, S. E.; Toto, T.; Bennartz, R.; Cribb, M.

    2011-12-01

    The impacts of aerosol particles on clouds continue to rank among the largest uncertainties in global climate simulation. In this work we assess the capability of the NASA GISS ModelE, coupled to MATRIX aerosol microphysics, in correctly representing warm-phase aerosol-cloud interactions. This evaluation is completed through the analysis of a nudged, multi-year global simulation using measurements from various US Department of Energy sponsored measurement campaigns and satellite-based observations. Campaign observations include the Aerosol Intensive Operations Period (Aerosol IOP) and Routine ARM Arial Facility Clouds with Low Optical Water Depths (CLOWD) Optical Radiative Observations (RACORO) at the Southern Great Plains site in Oklahoma, the Marine Stratus Radiation, Aerosol, and Drizzle (MASRAD) campaign at Pt. Reyes, California, and the ARM mobile facility's 2008 deployment to China. This combination of datasets provides a variety of aerosol and atmospheric conditions under which to test ModelE parameterizations. In addition to these localized comparisons, we provide the results of global evaluations completed using measurements derived from satellite remote sensors. We will provide a basic overview of simulation performance, as well as a detailed analysis of parameterizations relevant to aerosol indirect effects.

  13. A one-dimensional sectional aerosol model integrated with mesoscale meteorological data to study marine boundary layer aerosol dynamics

    NASA Astrophysics Data System (ADS)

    Caffrey, Peter F.; Hoppel, William A.; Shi, Jainn J.

    2006-12-01

    The dynamics of aerosols in the marine boundary layer are simulated with a one-dimensional, multicomponent, sectional aerosol model using vertical profiles of turbulence, relative humidity, temperature, vertical velocity, cloud cover, and precipitation provided by 3-D mesoscale meteorological model output. The Naval Research Laboratory's (NRL) sectional aerosol model MARBLES (Fitzgerald et al., 1998a) was adapted to use hourly meteorological input taken from NRL's Coupled Ocean-Atmosphere Prediction System (COAMPS). COAMPS-generated turbulent mixing coefficients and large-scale vertical velocities determine vertical exchange within the marine boundary layer and exchange with the free troposphere. Air mass back trajectories were used to define the air column history along which the meteorology was retrieved for use with the aerosol model. Details on the integration of these models are described here, as well as a description of improvements made to the aerosol model, including transport by large-scale vertical motions (such as subsidence and lifting), a revised sea-salt aerosol source function, and separate tracking of sulfate mass from each of the five sources (free tropospheric, nucleated, condensed from gas phase oxidation products, cloud-processed, and produced from heterogeneous oxidation of S(IV) on sea-salt aerosol). Results from modeling air masses arriving at Oahu, Hawaii, are presented, and the relative contribution of free-tropospheric sulfate particles versus sea-salt aerosol from the surface to CCN concentrations is discussed. Limitations and benefits of the method are presented, as are sensitivity analyses of the effect of large-scale vertical motions versus turbulent mixing.

  14. Spatial distributions and seasonal cycles of aerosol climate effects in India seen in a global climate-aerosol model

    NASA Astrophysics Data System (ADS)

    Henriksson, S. V.; Pietikäinen, J.-P.; Hyvärinen, A.-P.; Räisänen, P.; Kupiainen, K.; Tonttila, J.; Hooda, R.; Lihavainen, H.; O'Donnell, D.; Backman, L.; Klimont, Z.; Laaksonen, A.

    2014-09-01

    Climate-aerosol interactions in India are studied by employing the global climate-aerosol model ECHAM5-HAM and the GAINS inventory for anthropogenic aerosol emissions. Model validation is done for black carbon surface concentrations in Mukteshwar and for features of the monsoon circulation. Seasonal cycles and spatial distributions of radiative forcing and the temperature and rainfall responses are presented for different model setups. While total aerosol radiative forcing is strongest in the summer, anthropogenic forcing is considerably stronger in winter than in summer. Local seasonal temperature anomalies caused by aerosols are mostly negative with some exceptions, e.g., parts of northern India in March-May. Rainfall increases due to the elevated heat pump (EHP) mechanism and decreases due to solar dimming mechanisms (SDMs) and the relative strengths of these effects during different seasons and for different model setups are studied. Aerosol light absorption does increase rainfall in northern India, but effects due to solar dimming and circulation work to cancel the increase. The total aerosol effect on rainfall is negative for northern India in the months of June-August, but during March-May the effect is positive for most model setups. These differences between responses in different seasons might help converge the ongoing debate on the EHPs and SDMs. Due to the complexity of the problem and known or potential sources for error and bias, the results should be interpreted cautiously as they are completely dependent on how realistic the model is. Aerosol-rainfall correlations and anticorrelations are shown not to be a reliable sole argument for deducing causality.

  15. 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

  16. Micro-capillary aerosol focusing device: theoretical modeling, experimental verification, and device fabrication.

    NASA Astrophysics Data System (ADS)

    Hoey, Justin; Akhatov, Iskander; Swenson, Orven; Schulz, Doug

    2007-11-01

    A theoretical model for the focusing of aerosol particles in a linearly-varying micro-capillary with a diameter on the order of 100 microns is presented. This theoretical model is experimentally verified by visualizing an aerosol beam of silver-ink aerosol particles of approximately 1 micron in diameter emitted from a micro-capillary. Additional validation is presented in the deposited lines where linewidth is a function of aerosol beamwidth. From the theoretical model a new design for the focusing of aerosol particles is developed, physically produced, and experimentally validated. The new device will be implemented in the areas of high frequency RFID manufacturing, and the semiconductor industry.

  17. Cloud-Resolving Model Simulations of Aerosol-Cloud Interactions Triggered by Strong Aerosol Emissions in the Arctic

    NASA Astrophysics Data System (ADS)

    Wang, H.; Kravitz, B.; Rasch, P. J.; Morrison, H.; Solomon, A.

    2014-12-01

    Previous process-oriented modeling studies have highlighted the dependence of effectiveness of cloud brightening by aerosols on cloud regimes in warm marine boundary layer. Cloud microphysical processes in clouds that contain ice, and hence the mechanisms that drive aerosol-cloud interactions, are more complicated than in warm clouds. Interactions between ice particles and liquid drops add additional levels of complexity to aerosol effects. A cloud-resolving model is used to study aerosol-cloud interactions in the Arctic triggered by strong aerosol emissions, through either geoengineering injection or concentrated sources such as shipping and fires. An updated cloud microphysical scheme with prognostic aerosol and cloud particle numbers is employed. Model simulations are performed in pure super-cooled liquid and mixed-phase clouds, separately, with or without an injection of aerosols into either a clean or a more polluted Arctic boundary layer. Vertical mixing and cloud scavenging of particles injected from the surface is still quite efficient in the less turbulent cold environment. Overall, the injection of aerosols into the Arctic boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. The pure liquid clouds are more susceptible to the increase in aerosol number concentration than the mixed-phase clouds. Rain production processes are more effectively suppressed by aerosol injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. Aerosol injection into a clean boundary layer results in a greater cloud albedo increase than injection into a polluted one, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, the impact of dynamical feedback due to precipitation changes is small. According to these results, which are dependent upon the representation of ice nucleation

  18. Interfacing the NRL 1-D High Vertical Resolution Aerosol Model with COAMPS

    DTIC Science & Technology

    2016-06-13

    TERM GOALS Identify, understand and quantify all the physical processes that govern the aerosols in the marine environment and develop a...size and composition distributions are required. Many of the aerosol source, sink and transformation processes are highly dependent on meteorological...parameters such as wind speed, humidity profile, clouds, precipitation scavenging, etc. The NRL 1-D aerosol- processes model includes all these

  19. simpleGAMMA - a reduced model of secondary organic aerosol formation in the aqueous aerosol phase (aaSOA)

    NASA Astrophysics Data System (ADS)

    Woo, J. L.; McNeill, V. F.

    2015-01-01

    There is increasing evidence that the uptake and aqueous processing of water-soluble volatile organic compounds (VOCs) by wet aerosols or cloud droplets is an important source of secondary organic aerosol (SOA). We recently developed GAMMA (Gas-Aerosol Model for Mechanism Analysis), a zero-dimensional kinetic model that couples gas-phase and detailed aqueous-phase atmospheric chemistry for speciated prediction of SOA and organosulfate formation in cloudwater or aqueous aerosols. Results from GAMMA simulations of SOA formation in aerosol water (McNeill et al., 2012) indicate that it is dominated by two pathways: isoprene epoxydiol (IEPOX) uptake followed by ring-opening chemistry (under low-NOx conditions) and glyoxal uptake. This suggested that it is possible to model the majority of aqueous aerosol phase SOA mass using a highly simplified reaction scheme. We have therefore developed a reduced version of GAMMA, simpleGAMMA. Close agreement in predicted aaSOA mass is observed between simpleGAMMA and GAMMA under all conditions tested (between pH 1-4 and RH 40-80%) after 12 h of simulation. simpleGAMMA is computationally efficient and suitable for coupling with larger-scale atmospheric chemistry models.

  20. Preliminary Results from an Assimilation of TOMS Aerosol Observations Into the GOCART Model

    NASA Technical Reports Server (NTRS)

    daSilva, Arlindo; Weaver, Clark J.; Ginoux, Paul; Torres, Omar; Einaudi, Franco (Technical Monitor)

    2000-01-01

    At NASA Goddard we are developing a global aerosol data assimilation system that combines advances in remote sensing and modeling of atmospheric aerosols. The goal is to provide high resolution, 3-D aerosol distributions to the research community. Our first step is to develop a simple assimilation system for Saharan mineral aerosol. The Goddard Chemistry and Aerosol Radiation model (GOCART) provides accurate 3-D mineral aerosol size distributions that compare well with TOMS satellite observations. Surface, mobilization, wet and dry deposition, convective and long-range transport are all driven by assimilated fields from the Goddard Earth Observing System Data Assimilation System, GEOS-DAS. Our version of GOCART transports sizes from.08-10 microns and only simulates Saharan dust. TOMS radiance observations in the ultra violet provide information on the mineral and carbonaceous aerosol fields. We use two main observables in this study: the TOMS aerosol index (AI) which is directly related to the ratio of the 340 and 380 radiances and the 380 radiance. These are sensitive to the aerosol optical thickness, the single scattering albedo and the height of the aerosol layer. The Goddard Aerosol Assimilation System (GAAS) uses the Data Assimilation Office's Physical-space Statistical Analysis System (PSAS) to combine TOMS observations and GOCART model first guess fields. At this initial phase we only assimilate observations into the the GOCART model over regions of Africa and the Atlantic where mineral aerosols dominant and carbonaceous aerosols are minimal, Our preliminary results during summer show that the assimilation with TOMS data modifies both the aerosol mass loading and the single scattering albedo. Assimilated aerosol fields will be compared with assimilated aerosol fields from GOCART and AERONET observations over Cape Verde.

  1. Continued development and testing of a new thermodynamic aerosol module for urban and regional air quality models

    NASA Astrophysics Data System (ADS)

    Nenes, Athanasios; Pandis, Spyros N.; Pilinis, Christodoulos

    A computationally efficient and rigorous thermodynamic model (ISORROPIA) that predicts the physical state and composition of inorganic atmospheric aerosol is presented. The advantages of this particular model render it suitable for incorporation into urban and regional air quality models. The model is embodied into the UAM-AERO air quality model, and the performance is compared with two other thermodynamic modules currently in use, SEQUILIB 1.5 and SEQUILIB 2.1. The new model yields predictions that agree with experimental measurements and the results of the other models, but at the same time proves to be much faster and computationally efficient. Using ISORROPIA accelerates the thermodynamic calculations by more than a factor of six, while the overall speed-up of UAM-AERO is at least twofold. This speedup is possible by the optimal solution of the thermodynamic equations, and the usage of precalculated tables, whenever possible.

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

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

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

    SciTech Connect

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

    2016-08-22

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

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

    SciTech Connect

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

    2016-08-22

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

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

    DOE PAGES

    Fast, Jerome D.; Berg, Larry K.; Zhang, Kai; ...

    2016-08-22

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

  6. Aerosol kinetic code "AERFORM": Model, validation and simulation results

    NASA Astrophysics Data System (ADS)

    Gainullin, K. G.; Golubev, A. I.; Petrov, A. M.; Piskunov, V. N.

    2016-06-01

    The aerosol kinetic code "AERFORM" is modified to simulate droplet and ice particle formation in mixed clouds. The splitting method is used to calculate condensation and coagulation simultaneously. The method is calibrated with analytic solutions of kinetic equations. Condensation kinetic model is based on cloud particle growth equation, mass and heat balance equations. The coagulation kinetic model includes Brownian, turbulent and precipitation effects. The real values are used for condensation and coagulation growth of water droplets and ice particles. The model and the simulation results for two full-scale cloud experiments are presented. The simulation model and code may be used autonomously or as an element of another code.

  7. A Wintertime Aerosol Model for the Ganga Basin, Northern India

    NASA Astrophysics Data System (ADS)

    Dey, S.; Tripathi, S. N.

    2006-05-01

    An aerosol model has been developed using mass size distributions of various chemical components measured at Kanpur (an urban location in the Ganga basin, GB, in Northern India) and applied to estimate the radiative effects of the aerosols over the entire GB during the winter season for the first time. The number size distribution of various species was derived from the measured mass concentration and the optical properties were calculated using OPAC model. The anthropogenic contribution to the total extinction was found to be more than 90%. The relative contribution of various species to the aerosol optical depth (AOD) at 0.5 μm are in the following order, (NH2)2SO4 (AS, 37%), nitrate (N, 28%), other salts (S, mainly NaCl and KCl, 19%), dust (9%) and black carbon, BC (7%). Contribution of AS, N, S to the observed AOD decreases with wavelength and that of dust increases with wavelength, whereas, BC contribution remains almost same. The extinction coefficient strongly depends on the relative humidity (RH), as the scattering by fine mode fraction (contributing 88% to the total extinction) is enhanced at high ambient RH. The spectral variation of absorption coefficient indicates that the most likely source of BC (as BC is the dominant absorbing species) in this region is fossil- fuel. The spectral variation of single scattering albedo (SSA) in the fine and coarse mode fractions and that of asymmetry parameter suggests that the internal mixing is more likely scenario, although the possibility of external mixing can not be ruled out. If the RH is lowered by ~20%, BC contribution to the AOD increases by ~3.5%, which implies that the RH is a strong controlling factor of the aerosol forcing. The mean shortwave clear sky top of the atmosphere (TOA) and surface forcing over Kanpur are -13±3 and -43±8 W m-2. Extending the TOA and surface efficiency over the entire GB, the mean TOA and surface forcing become -9±3 and -25±10 W m-2. This results in high atmospheric

  8. Atmospheric aerosol models for systems including the ions H+, NH4+, Na+, SO42-, NO3-, Cl-, Br-, and H2O

    NASA Astrophysics Data System (ADS)

    Wexler, Anthony S.; Clegg, Simon L.

    2002-07-01

    Mole fraction based equations for aqueous phase activities, together with equilibrium constants for the formation of gases and solids, have been combined with a Gibbs free energy minimization algorithm to create equilibrium phase partitioning models of inorganic atmospheric aerosols. The water content, phase state (solid or liquid), and gas/aerosol partitioning are predicted for known ionic composition, relative humidity, and temperature. The models are valid from <200 to 328 K for the subsystems (H+-SO42--NO3--Cl--Br--H2O) and (H+-NH4+-SO42--NO3--H2O), and 298.15 K only for (H+-NH4+-Na+-SO42--NO3--Cl--H2O). The models involve no simplifying assumptions and include all solid phases identified in bulk experiments, including hydrated and double salt forms not treated in most other studies. The Henry's law constant of H2SO4 is derived as a function of temperature, based upon available data, and the model treatment of the solubility of HBr in aqueous H2SO4 is revised. Phase diagrams are calculated for the (NH4)2SO4/H2SO4/H2O system to low temperature. The models are also used to explore the importance of the double salts in urban inorganic aerosols. These Aerosol Inorganics Model (AIM) models can be run on the Web for a variety of problem types at http://mae.ucdavis.edu/wexler/aim.html and http://www.uea.ac.uk/~e770/aim.html, and their use is summarized here.

  9. Establishing aerosol exposure predictive models based on vibration measurements.

    PubMed

    Soo, Jhy-Charm; Tsai, Perng-Jy; Lee, Shih-Chuan; Lu, Shih-Yi; Chang, Cheng-Ping; Liou, Yuh-When; Shih, Tung-Sheng

    2010-06-15

    This paper establishes particulate exposure predictive models based on vibration measurements under various concrete drilling conditions. The whole study was conducted in an exposure chamber using a full-scale mockup of concrete drilling simulator to simulate six drilling conditions. For each drilling condition, the vibration of the three orthogonal axes (i.e., a(x), a(y), and a(z)) was measured from the hand tool. Particulate exposure concentrations to the total suspended particulate (C(TSP)), PM(10) (C(PM10)), and PM(2.5) (C(PM2.5)) were measured at the downwind side of the drilling simulator. Empirical models for predicting C(TSP), C(PM10) and C(PM2.5) were done based on measured a(x), a(y), and a(z) using the generalized additive model. Good agreement between measured aerosol exposures and vibrations was found with R(2)>0.969. Our results also suggest that a(x) was mainly contributed by the abrasive wear. On the other hand, a(y) and a(z) were mainly contributed by both the impact wear and brittle fracture wear. The approach developed from the present study has the potential to provide a cheaper and convenient method for assessing aerosol exposures from various emission sources, particularly when conducting conventional personal aerosol samplings are not possible in the filed.

  10. Evaluation of a size-resolved aerosol model based on satellite and ground observations and its implication on aerosol forcing

    NASA Astrophysics Data System (ADS)

    Ma, Xiaoyan; Yu, Fangqun

    2016-04-01

    The latest AeroCom phase II experiments have showed a large diversity in the simulations of aerosol concentrations, size distribution, vertical profile, and optical properties among 16 detailed global aerosol microphysics models, which contribute to the large uncertainty in the predicted aerosol radiative forcing and possibly induce the distinct climate change in the future. In the last few years, we have developed and improved a global size-resolved aerosol model (Yu and Luo, 2009; Ma et al., 2012; Yu et al., 2012), GEOS-Chem-APM, which is a prognostic multi-type, multi-component, size-resolved aerosol microphysics model, including state-of-the-art nucleation schemes and condensation of low volatile secondary organic compounds from successive oxidation aging. The model is one of 16 global models for AeroCom phase II and participated in a couple of model inter-comparison experiments. In this study, we employed multi-year aerosol optical depth (AOD) data from 2004 to 2012 taken from ground-based Aerosol Robotic Network (AERONET) measurements and Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging SpectroRadiometer (MISR) and Sea-viewing Wide Field-of-view Sensor (SeaWiFS) satellite retrievals to evaluate the performance of the GEOS-Chem-APM in predicting aerosol optical depth, including spatial distribution, reginal variation and seasonal variabilities. Compared to the observations, the modelled AOD is overall good over land, but quite low over ocean possibly due to low sea salt emission in the model and/or higher AOD in satellite retrievals, specifically MODIS and MISR. We chose 72 AERONET sites having at least 36 months data available and representative of high spatial domain to compare with the model and satellite data. Comparisons in various representative regions show that the model overall agrees well in the major anthropogenic emission regions, such as Europe, East Asia and North America. Relative to the observations, the modelled AOD is

  11. 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.

  12. Online Simulations and Forecasts of the Global Aerosol Distribution in the NASA GEOS-5 Model

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2006-01-01

    We present an analysis of simulations of the global aerosol system in the NASA GEOS-5 transport, radiation, and chemistry model. The model includes representations of all major tropospheric aerosol species, including dust, sea salt, black carbon, particulate organic matter, and sulfates. The aerosols are run online for the period 2000 through 2005 in a simulation driven by assimilated meteorology from the NASA Goddard Data Assimilation System. Aerosol surface mass concentrations are compared with existing long-term surface measurement networks. Aerosol optical thickness is compared with ground-based AERONET sun photometry and space-based retrievals from MODIS, MISR, and OMI. Particular emphasis is placed here on consistent sampling of model and satellite aerosol optical thickness to account for diurnal variations in aerosol optical properties. Additionally, we illustrate the use of this system for providing chemical weather forecasts in support of various NASA and community field missions.

  13. On the implications of aerosol liquid water and phase separation for organic aerosol mass

    EPA Science Inventory

    Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to org...

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

  15. A simplified model of aerosol removal by containment sprays

    SciTech Connect

    Powers, D.A. ); Burson, S.B. . Div. of Safety Issue Resolution)

    1993-06-01

    Spray systems in nuclear reactor containments are described. The scrubbing of aerosols from containment atmospheres by spray droplets is discussed. Uncertainties are identified in the prediction of spray performance when the sprays are used as a means for decontaminating containment atmospheres. A mechanistic model based on current knowledge of the physical phenomena involved in spray performance is developed. With this model, a quantitative uncertainty analysis of spray performance is conducted using a Monte Carlo method to sample 20 uncertain quantities related to phenomena of spray droplet behavior as well as the initial and boundary conditions expected to be associated with severe reactor accidents. Results of the uncertainty analysis are used to construct simplified expressions for spray decontamination coefficients. Two variables that affect aerosol capture by water droplets are not treated as uncertain; they are (1) [open quote]Q[close quote], spray water flux into the containment, and (2) [open quote]H[close quote], the total fall distance of spray droplets. The choice of values of these variables is left to the user since they are plant and accident specific. Also, they can usually be ascertained with some degree of certainty. The spray decontamination coefficients are found to be sufficiently dependent on the extent of decontamination that the fraction of the initial aerosol remaining in the atmosphere, m[sub f], is explicitly treated in the simplified expressions. The simplified expressions for the spray decontamination coefficient are given. Parametric values for these expressions are found for median, 10 percentile, and 90 percentile values in the uncertainty distribution for the spray decontamination coefficient. Examples are given to illustrate the utility of the simplified expressions to predict spray decontamination of an aerosol-laden atmosphere.

  16. The Aerosol Models in MODTRAN: Incorporating Selected Measurements From Northern Australia

    DTIC Science & Technology

    2005-12-01

    tropopause. These include a background stratospheric aerosol model, volcanic aerosol models and an upper atmosphere aerosol model. These models will not...scaling factor is a function of VIS, the season and the volcanic conditions. The normalised attenuation coefficients are defined as ratios of the...different values of VIS: 2, 5, 10, 23 and 50 km. The upper altitude profiles are computed as a function of the season and volcanic conditions and stored

  17. Inorganic ions in ambient fine particles over a National Park in central India: Seasonality, dependencies between SO42-, NO3-, and NH4+, and neutralization of aerosol acidity

    NASA Astrophysics Data System (ADS)

    Kumar, Samresh; Sunder Raman, Ramya

    2016-10-01

    Twelve hour integrated ambient fine particles (PM2.5) were collected over an Van Vihar National Park (VVNP), in Bhopal, Central India. Samples were collected on filter substrates every-other-day for two years (2012 and 2013). In addition to PM2.5 mass concentration, water soluble inorganic ions (WSIIs) were also measured. Further, on-site meteorological parameters including temperature, wind speed, wind direction, relative humidity, rainfall and atmospheric pressure were recorded. During 2012, the average PM2.5 concentration was 40 ± 31 μgm-3 while during 2013 it was 48 ± 50 μgm-3. Further, in about 20% of the samples the 12 h integrated fine PM mass exceeded the daily (24 h) average standards (60 μgm-3). This observation suggests that the PM2.5 mass concentration at the study site is likely to be in violation of the National Ambient Air Quality Standard (NAAQS), India. During the study period the sum of three major ions (SO42-, NO3-, and NH4+) accounted for 19.4% of PM2.5 mass on average. Air parcel back trajectory ensembles revealed that emissions from thermal power plants were likely to be the main regional source of particulate SO42- and NO3- measured over VVNP. Further, local traffic activities appeared to have no significant impact on the concentrations of PM2.5 and its WSIIs constituents, as revealed by a day-of-the-week analysis. PM2.5 mass, SO42-, NO3-, and NH4+ showed a pronounced seasonal trend with winter (Jan, Feb) and post-monsoon (Oct, Nov, Dec) highs and pre-monsoon (Mar, Apr, May) and monsoon (Jun, Jul, Aug, Sep) lows, during both 2012 and 2013. Further, when the sum of SO42- and NO3- constituted greater than 90% of water soluble inorganic anions by mass, they were linearly dependent on one another and moderately anti-correlated (r2 = 0.60). The molar ratios of NH4+ and non-sea salt SO42- were examined to understand the aerosol neutralization mechanisms and particulate NO3- formation. An assessment of these ratios and subsequent analyses

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

  19. Reformulating Aerosol Thermodynamics and Cloud Microphysics

    NASA Astrophysics Data System (ADS)

    Metzger, S.

    2006-12-01

    Modeling aerosol composition and cloud microphysics is rather complex due to the required thermodynamics, even if chemical and thermodynamical equilibrium is assumed. We show, however, that for deliquescent atmospheric aerosols thermodynamics can be considerably simplified, if we reformulate chemical equilibrium to include water purely based on thermodynamic principles. In chemical and thermodynamical equilibrium, the relative humidity (RH) fixes the molality of atmospheric aerosols. Although this fact is in theory well known, it has hardly been utilized in aerosol modeling nor has been the fact that for the same reason also the aerosol activity (including activity coefficients) and water content are fixed (by RH) for a given aerosol concentration and type. The only model that successfully utilizes this fact is the computationally very efficient EQuilibrium Simplified thermodynamic gas/Aerosol partitioning Model, EQSAM (Metzger et al., 2002a), EQSAM2 (Metzger et al., 2006). In both versions the entire gas/liquid/solid aerosol equilibrium partitioning is solved analytically and hence non-iteratively a substantial advantage in aerosol composition modeling. Here we briefly present the theoretical framework of EQSAM2, which differs from EQSAM in a way that the calculation of the water activity of saturated binary or mixed inorganic/organic salt solutions of multi-component aerosols has been generalized by including the Kelvin-term, thus allowing for any solute activity above the deliquescence relative humidity, including supersaturation. With application of our new concept to a numerical whether prediction (NWP) model, we demonstrate its wide implications for the computation of various aerosol and cloud properties, as our new concept allows to consistently and efficiently link the modeling of aerosol thermodynamics and cloud microphysics through the aerosol water mass, which therefore deserves special attention in atmospheric chemistry, air pollution, NWP and climate

  20. Remote sensing of aerosol plumes: a semianalytical model.

    PubMed

    Alakian, Alexandre; Marion, Rodolphe; Briottet, Xavier

    2008-04-10

    A semianalytical model, named APOM (aerosol plume optical model) and predicting the radiative effects of aerosol plumes in the spectral range [0.4,2.5 microm], is presented in the case of nadir viewing. It is devoted to the analysis of plumes arising from single strong emission events (high optical depths) such as fires or industrial discharges. The scene is represented by a standard atmosphere (molecules and natural aerosols) on which a plume layer is added at the bottom. The estimated at-sensor reflectance depends on the atmosphere without plume, the solar zenith angle, the plume optical properties (optical depth, single-scattering albedo, and asymmetry parameter), the ground reflectance, and the wavelength. Its mathematical expression as well as its numerical coefficients are derived from MODTRAN4 radiative transfer simulations. The DISORT option is used with 16 fluxes to provide a sufficiently accurate calculation of multiple scattering effects that are important for dense smokes. Model accuracy is assessed by using a set of simulations performed in the case of biomass burning and industrial plumes. APOM proves to be accurate and robust for solar zenith angles between 0 degrees and 60 degrees whatever the sensor altitude, the standard atmosphere, for plume phase functions defined from urban and rural models, and for plume locations that extend from the ground to a height below 3 km. The modeling errors in the at-sensor reflectance are on average below 0.002. They can reach values of 0.01 but correspond to low relative errors then (below 3% on average). This model can be used for forward modeling (quick simulations of multi/hyperspectral images and help in sensor design) as well as for the retrieval of the plume optical properties from remotely sensed images.

  1. Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

    NASA Astrophysics Data System (ADS)

    Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

    2016-07-01

    The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a "simulated radiance" product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land-ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers.This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled.In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model subgrid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to

  2. Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

    NASA Technical Reports Server (NTRS)

    Wind, Galina; Da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

    2016-01-01

    The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a simulated radiance product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers. This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled. In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model sub grid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to

  3. Organic aerosols and inorganic species from post-harvest agricultural-waste burning emissions over northern India: impact on mass absorption efficiency of elemental carbon.

    PubMed

    Rajput, Prashant; Sarin, M M; Sharma, Deepti; Singh, Darshan

    2014-01-01

    Atmospheric PM2.5 (particulate matter with aerodynamic diameter of ≤ 2.5 μm), collected from a source region [Patiala: 30.2 °N; 76.3 °E; 250 m above mean sea level] of emissions from post-harvest agricultural-waste (paddy-residue) burning in the Indo-Gangetic Plain (IGP), North India, has been studied for its chemical composition and impact on regional atmospheric radiative forcing. On average, organic aerosol mass accounts for 63% of PM2.5, whereas the contribution of elemental carbon (EC) is ∼3.5%. Sulphate, nitrate and ammonium contribute up to ∼85% of the total water-soluble inorganic species (WSIS), which constitutes ∼23% of PM2.5. The potassium-to-organic carbon ratio from paddy-residue burning emissions (KBB(+)/OC: 0.05 ± 0.01) is quite similar to that reported from Amazonian and Savanna forest-fires; whereas non-sea-salt-sulphate-to-OC ratio (nss-SO4(2-)/OC: 0.21) and nss-SO4(2-)/EC ratio of 2.6 are significantly higher (by factor of 5 to 8). The mass absorption efficiency of EC (3.8 ± 1.3 m(2) g(-1)) shows significant decrease with a parallel increase in the concentrations of organic aerosols and scattering species (sulphate and nitrate). A cross plot of OC/EC and nss-SO4(2-)/EC ratios show distinct differences for post-harvest burning emissions from paddy-residue as compared to those from fossil-fuel combustion sources in south-east Asia.

  4. The Dynamics of Aerosols: Recent Developments In Regional and Global Modelling

    NASA Astrophysics Data System (ADS)

    Vignati, E.

    An efficient and accurate representation of aerosol size distributions and microphysi- cal processes is required to make physically consistent calculations of the direct and indirect radiative effects of aerosols and their impact on climate. Various modelling approaches have been developed to simulate the dynamical evolu- tion of natural and anthropogenic aerosol populations. Among the components of the particulate phase, sulphate, sea salt, black carbon, organic carbon and dust all play an important role. However their contributions vary from region to region. Modal models, in which the aerosol size distribution is represented by a number of modes, present a computational attractive approach for aerosol dynamic modelling in regional and global models. They can describe external as well as internal mixtures of aerosol particles and the full aerosol dynamics. The accuracy of modal models is however dependent on both the suitability of the lognormal approximation to the size distribution and the extent to which processes can be expressed in terms of distribution parameters. Simultaneously, recent developments have been made to treat many aerosol species in global models using discrete size bins. The detailed description allows a more ac- curate calculation of the aerosol water content, an important parameter required for calculations of aerosol optical properties. However, such a fine size resolution is usu- ally time consuming when used in large scale models, therefore sometimes not all the processes modifying aerosol properties are included. Modest requirements for storage and computations is one of the advantages of moment methods. These techniques have the capability of simultaneously represent the aerosol dynamic processes and transport in large scale models. An overview of recent developments of aerosol modelling in global and regional mod- els will be presented outlining the advantages and disadvantages of the various tech- niques for such large scales.

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

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

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

  6. SOIR/VEX mesospheric aerosols observations and modelling

    NASA Astrophysics Data System (ADS)

    Wilquet, Valérie; Carine Vandaele, Ann; Drummond, Rachel; Mahieux, Arnaud; Robert, Séverine; Daerden, Frank; Neary, Lori; Bertaux, Jean-Loup

    2013-04-01

    SPICAV/SOIR on-board Venus Express is able to target the layer of aerosols above the cloud layer at the terminator (Wilquet et al., 2009). A high temporal variability in the aerosol content in Venus' atmosphere was inferred from SOIR observations, as well as a latitudinal dependency of the aerosol loading (Wilquet et al., 2012). This is in agreement with results from previous missions and with the facts that (i) H2SO4 aerosol particles are formed through SO2 photo-oxidation and hydration at the cloud top of Venus, (ii) SO2 photolysis is more efficient at low latitudes, (iii) the altitude of the cloud top is up to one scale height lower in the polar region than at the equator. A increasing SO2 abundance with increasing altitude was recently observed with SPICAV-UV at altitudes of ~ 85-105 km (Belyaev et al., 2012) but also from microwave ground-based spectra in the Venus mesosphere (Sandor et al., 2010), which suggest a source of SO2 at high altitudes. Zhang et al. (2012) proposed a one dimensional photochemistry-diffusion model in order to reconcile these puzzling findings; he suggested that H2SO4 might be a source of SO2 above 90 km through aerosol evaporation followed by SO3 photolysis. This model and the observations are however disputed by others demonstrating the necessity for a more global interpretation of the observations and for modelling of the upper haze layer. For example, the variations in aerosol loading can be compared to other key parameters of the atmosphere retrieved from the same SOIR spectra such as water and SO2 composition or temperature. In addition, a microphysical model is being developed that will calculate the time dependent haze particle size distributions assuming an initial size distribution of background sulphate aerosols. The model will simulate the formation, growth, evaporation, and sedimentation of particles. Results of this on-going research will be presented and discussed. References : Belyaev, D.A., F. Montmessin, J.-L. Bertaux

  7. Aerosol microphysics modules in the framework of the ECHAM5 climate model - intercomparison under stratospheric conditions

    NASA Astrophysics Data System (ADS)

    Kokkola, H.; Hommel, R.; Kazil, J.; Niemeier, U.; Partanen, A.-I.; Feichter, J.; Timmreck, C.

    2009-07-01

    In this manuscript, we present an intercomparison of three different aerosol microphysics modules that are implemented in the climate model ECHAM5. The comparison was done between the modal aerosol microphysics module M7, which is currently the default aerosol microphysical core in ECHAM5, and two sectional aerosol microphysics modules SALSA, and SAM2. The detailed aerosol microphysical model MAIA was used as a reference to evaluate the results of the aerosol microphysics modules with respect to sulphate aerosol. The ability of the modules to describe the development of the aerosol size distribution was tested in a zero dimensional framework. We evaluated the strengths and weaknesses of different approaches under different types of stratospheric conditions. Also, we present an improved method for the time integration in M7 and study how the setup of the modal aerosol modules affects the evolution of the aerosol size distribution. Intercomparison simulations were carried out with varying SO2 concentrations from background conditions to extreme values arising from stratospheric injections by large volcanic eruptions. Under background conditions, all microphysics modules were in good agreement describing the shape of the aerosol size distribution, but the scatter between the model results increased with increasing SO2 concentrations. In particular in the volcanic case the setups of the aerosol modules have to be adapted in order to dependably capture the evolution of the aerosol size distribution, and to perform in global model simulations. In summary, this intercomparison serves as a review of the different aerosol microphysics modules which are currently available for the climate model ECHAM5.

  8. Modeling Electrical Structure of the Artificial Charged Aerosol Cloud

    NASA Astrophysics Data System (ADS)

    Davydenko, S.; Iudin, D.; Klimashov, V.; Kostinskiy, A. J.; Syssoev, V.

    2014-12-01

    The electric structure of the unipolar charged aerosol cloud is considered. The cloud of the volume about 30 cubic meters is generated in the open atmosphere by the original aeroelectrical facility consisting of the source of the aquated ions and the high-voltage discharger. Representing the charge density distribution as a superposition of regular and irregular parts, a model of the electrical structure of the cloud is developed. The regular part is calculated under the stationary current approximation taking into account the source current structure, the shape of the cloud, and results of the multi-point measurements of the electric field and conductivity in the vicinity of the cloud. The irregular part describes random spatiotemporal fluctuations of the charge density which are assumed to be proportional to the aerosol number density. It is shown that a quasi-electrostatic field of the charged aerosol is characterized by significant spatial fluctuations showing the scale invariance. The mean-square fluctuations of the voltage between different parts of the cloud are proportional to the square root of its linear dimensions and may reach significant values even in the absence of the regular field. The basic parameters of the fluctuating spatial structure of the electric field inside the charged aerosol cloud are estimated. It is shown that the charge density fluctuations could lead to a significant (up to 2,5 times) local enhancement of the electric field as compared to the field of the regular part of the charge density. The above effect could serve as one of the important mechanisms of the spark initiation.

  9. Development and application of an aerosol screening model for size-resolved urban aerosols.

    PubMed

    Stanier, Charles O; Lee, Sang-Rin

    2014-06-01

    Predictive models of vehicular ultrafine particles less than 0.1 microm in diameter (UFPs*) and other urban pollutants with high spatial and temporal variation are useful and important in applications such as (1) decision support for infrastructure projects, emissions controls, and transportation-mode shifts; (2) the interpretation and enhancement of observations (e.g., source apportionment, extrapolation, interpolation, and gap-filling in space and time); and (3) the generation of spatially and temporally resolved exposure estimates where monitoring is unfeasible. The objective of the current study was to develop, test, and apply the Aerosol Screening Model (ASM), a new physically based vehicular UFP model for use in near-road environments. The ASM simulates hourly average outdoor concentrations of roadway-derived aerosols and gases. Its distinguishing features include user-specified spatial resolution; use of the Weather Research and Forecasting (WRF) meteorologic model for winds estimates; use of a database of more than 100,000 road segments in the Los Angeles, California, region, including freeway ramps and local streets; and extensive testing against more than 9000 hours of observed particle concentrations at 11 sites. After initialization of air parcels at an upwind boundary, the model solves for vehicle emissions, dispersion, coagulation, and deposition using a Lagrangian modeling framework. The Lagrangian parcel of air is subdivided vertically (into 11 levels) and in the crosswind direction (into 3 parcels). It has overall dimensions of 10 m (downwind), 300 m (vertically), and 2.1 km (crosswind). The simulation is typically started 4 km upwind from the receptor, that is, the location at which the exposure is to be estimated. As parcels approach the receptor, depending on the user-specified resolution, step size is decreased, and crosswind resolution is enhanced through subdivision of parcels in the crosswind direction. Hourly concentrations and size

  10. Aerosol microphysics modules in the framework of the ECHAM5 climate model - intercomparison under stratospheric conditions

    NASA Astrophysics Data System (ADS)

    Kokkola, H.; Hommel, R.; Kazil, J.; Niemeier, U.; Partanen, A.-I.; Feichter, J.; Timmreck, C.

    2009-03-01

    In this manuscript, we present an intercomparison of three different aerosol microphysics modules that are implemented in the climate model ECHAM5. The comparison was done between the modal aerosol microphysics module M7, which is currently the default aerosol microphysical core in ECHAM5, and two sectional aerosol microphysics modules SALSA, and SAM2. A detailed aerosol microphycical model MAIA was used as a reference model to evaluate the results of the aerosol microphysics modules with respect to sulphate aerosol. The ability of the modules to describe the development of the aerosol size distribution was tested in a zero dimensional framework. We evaluated the strengths and weaknesses of different approaches under different types of stratospheric conditions. Also, we present an improved method for the time integration in M7 and study how the setup of the modal approach affects the evolution of the aerosol size distribution. Intercomparison simulations were carried out with varying SO2 concentrations from background conditions to extreme values arising from stratospheric injections of large volcanic eruptions. Under background conditions, all microphysics modules were in good agreement describing the shape of the size distribution but the scatter between the model results increased with increasing SO2 concentrations. In particular for the volcanic case the module setups have to be redefined to be applied in global model simulations capturing respective sulphate particle formation events. Summarized, this intercomparison serves as a review on the different aerosol microphysics modules which are currently available for the climate model ECHAM5.

  11. Propagation of global model uncertainties in aerosol forecasting: A field practitioner's opinion

    NASA Astrophysics Data System (ADS)

    Reid, J. S.; Benedetti, A.; Bozzo, A.; Brooks, I. M.; Brooks, M.; Colarco, P. R.; daSilva, A.; Flatau, M. K.; Kuehn, R.; Hansen, J.; Holz, R.; Kaku, K.; Lynch, P.; Remy, S.; Rubin, J. I.; Sekiyama, T. T.; Tanaka, T. Y.; Zhang, J.

    2015-12-01

    While aerosol forecasting has its own host of aerosol source, sink and microphysical challenges to overcome, ultimately any numerical weather prediction based aerosol model can be no better than its underlying meteorology. However, the scorecard elements that drive NWP model development have varying relationships to the key uncertainties and biases that are of greatest concern to aerosol forecasting. Here we provide opinions from member developers of the International Cooperative for Aerosol Prediction (ICAP) on NWP deficiencies related to multi-specie aerosol forecasting, as well as relevance of current NWP scorecard elements to aerosol forecasting. Comparisons to field mission data to simulations are used to demonstrate these opinions and show how shortcomings in individual processes in the global models cascade into aerosol prediction. While a number of sensitivities will be outlined, as one would expect, the most important processes relate to aerosol sources, sinks and, in the context of data assimilation, aerosol hygroscopicity. Thus, the pressing needs in the global models relate to boundary layer and convective processes in the context of large scale waves. Examples will be derived from tropical to polar field measurements, from simpler to more complex including a) network data on dust emissions and transport from Saharan Africa, b) boundary layer development, instability, and deep convection in the United States during Studies of Emissions and Atmospheric, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS); and c) 7 Southeast Asian Studies (7SEAS) data on aerosol influences by maritime convection up-scaled through tropical waves. While the focus of this talk is how improved meteorological model processes are important to aerosol modeling, we conclude with recent findings of the Arctic Summer Cloud Ocean Study (ASCOS) which demonstrate how aerosol processes may be important to global model simulations of polar cloud, surface energy and subsequently

  12. Monitoring of inorganic ions, carbonaceous matter and mass in ambient aerosol particles with online and offline methods

    NASA Astrophysics Data System (ADS)

    Timonen, H.; Aurela, M.; Saarnio, K.; Frey, A.; Saarikoski, S.; Teinilä, K.; Kulmala, M.; Hillamo, R.

    2011-10-01

    Year-long high timeresolution measurements of major chemical components in atmospheric sub-micrometer particles were conducted at an urban background station in Finland 2006-2007. Ions were analyzed using a particle-into-liquid sampler combined with an ion chromatograph (PILS-IC), organic and elemental carbon (OC and EC) by using a semicontinuos OC/EC aerosol carbon analyzer (RT-OCEC), and PM2.5 mass with a tapered element oscillating microbalance (TEOM). Long time series provides information on differences between the used measurement techniques as well as information about the diurnal and seasonal changes. Chemical mass closure was constructed by comparing the identified aerosol mass with the measured PM2.5. The sum of all components measured online (ions, particulate organic matter (POM), EC) represented only 65% of the total PM2.5 mass. The difference can be explained by the difference in cutoff sizes (PM1 for online measurements, PM2.5 for total mass) and by evaporation of the semivolatile/volatile components. In general, some differences in results were observed when the results of the continuous/semicontinuous instruments were compared with those of the conventional filter samplings. For non-volatile compounds, like sulfate and potassium, correlation between the filter samples and the PILS was good but greater differences were observed for the semivolatile compounds like nitrate and ammonium. For OC the results of the RT-OCEC were on average 10% larger than those of the filters. When compared to filter measurements, high resolution measurements provide important data on short pollution plumes as well as on diurnal changes. Clear seasonal and diurnal cycles were observed for nitrate and EC.

  13. Simulation of aerosol radiative properties with the ORISAM-RAD model during a pollution event (ESCOMPTE 2001)

    NASA Astrophysics Data System (ADS)

    Mallet, M.; Pont, V.; Liousse, C.; Roger, J. C.; Dubuisson, P.

    The aim of this study is to present the organic and inorganic spectral aerosol module-radiative (ORISAM-RAD) module, allowing the 3D distribution of aerosol radiative properties (aerosol optical depth, single scattering albedo and asymmetry parameter) from the ORISAM module. In this work, we test ORISAM-RAD for one selected day (24th June) during the ESCOMPTE (expérience sur site pour contraindre les modèles de pollution atmosphérique et de transport d'emissions) experiment for an urban/industrial aerosol type. The particle radiative properties obtained from in situ and AERONET observations are used to validate our simulations. In a first time, simulations obtained from ORISAM-RAD indicate high aerosol optical depth (AOD)˜0.50-0.70±0.02 (at 440 nm) in the aerosol pollution plume, slightly lower (˜10-20%) than AERONET retrievals. In a second time, simulations of the single scattering albedo ( ωo) have been found to well reproduce the high spatial heterogeneities observed over this domain. Concerning the asymmetry parameter ( g), ORISAM-RAD simulations reveal quite uniform values over the whole ESCOMPTE domain, comprised between 0.61±0.01 and 0.65±0.01 (at 440 nm), in excellent agreement with ground based in situ measurements and AERONET retrievals. Finally, the outputs of ORISAM-RAD have been used in a radiative transfer model in order to simulate the diurnal direct radiative forcing at different locations (urban, industrial and rural). We show that anthropogenic aerosols strongly decrease surface solar radiation, with diurnal mean surface forcings comprised between -29.0±2.9 and -38.6±3.9 W m -2, depending on the sites. This decrease is due to the reflection of solar radiations back to space (-7.3±0.8<Δ FTOA<-12.3±1.2 W m -2) and to its absorption into the aerosol layer (21.1±2.1<Δ FATM<26.3±2.6 W m -2). These values are found to be consistent with those measured at local scale.

  14. Large-Scale Aerosol Modeling and Analysis

    DTIC Science & Technology

    2010-09-30

    advance anywhere on the globe. NAAPS and COAMPS are particularly useful for forecasts of dust storms in areas downwind of the large deserts of the world... dust source regions in NAAPS. The DSD has been crucial for high-resolution dust forecasting in SW Asia using COAMPS (Walker et al., 2009). Dust ...6 Figure 2. Four-panel product used to compare multiple model forecasts of visibility in SW Asia dust storms . On the web the product is

  15. Simulation of Aerosols and Chemistry with a Unified Global Model

    NASA Technical Reports Server (NTRS)

    Chin, Mian

    2004-01-01

    This project is to continue the development of the global simulation capabilities of tropospheric and stratospheric chemistry and aerosols in a unified global model. This is a part of our overall investigation of aerosol-chemistry-climate interaction. In the past year, we have enabled the tropospheric chemistry simulations based on the GEOS-CHEM model, and added stratospheric chemical reactions into the GEOS-CHEM such that a globally unified troposphere-stratosphere chemistry and transport can be simulated consistently without any simplifications. The tropospheric chemical mechanism in the GEOS-CHEM includes 80 species and 150 reactions. 24 tracers are transported, including O3, NOx, total nitrogen (NOy), H2O2, CO, and several types of hydrocarbon. The chemical solver used in the GEOS-CHEM model is a highly accurate sparse-matrix vectorized Gear solver (SMVGEAR). The stratospheric chemical mechanism includes an additional approximately 100 reactions and photolysis processes. Because of the large number of total chemical reactions and photolysis processes and very different photochemical regimes involved in the unified simulation, the model demands significant computer resources that are currently not practical. Therefore, several improvements will be taken, such as massive parallelization, code optimization, or selecting a faster solver. We have also continued aerosol simulation (including sulfate, dust, black carbon, organic carbon, and sea-salt) in the global model to cover most of year 2002. These results have been made available to many groups worldwide and accessible from the website http://code916.gsfc.nasa.gov/People/Chin/aot.html.

  16. Modeling aerosol growth by aqueous chemistry in nonprecipitating stratiform cloud

    SciTech Connect

    Ovchinnikov, Mikhail; Easter, Richard C.

    2010-07-29

    A new microphysics module based on a two-dimensional (2D) joint size distribution function representing both interstitial and cloud particles is developed and applied to studying aerosol processing in non-precipitating stratocumulus clouds. The module is implemented in a three-dimensional dynamical framework of a large-eddy simulation (LES) model and in a trajectory ensemble model (TEM). Both models are used to study the modification of sulfate aerosol by the activation - aqueous chemistry - resuspension cycle in shallow marine stratocumulus clouds. The effect of particle mixing and different size-distribution representations on modeled aerosol processing are studied in a comparison of the LES and TEM simulations with the identical microphysics treatment exposes and a comparison of TEM simulations with a 2D fixed and moving bin microphysics. Particle mixing which is represented in LES and neglected in the TEM leads to the mean relative per particle dry mass change in the TEM simulations being about 30% lower than in analogous subsample of LES domain. Particles in the final LES spectrum are mixed in from different “parcels”, some of which have experienced longer in-cloud residence times than the TEM parcels, all of which originated in the subcloud layer, have. The mean relative per particle dry mass change differs by 14% between TEM simulations with fixed and moving bin microphysics. Finally, the TEM model with the moving bin microphysics is used to evaluate assumptions about liquid water mass partitioning among activated cloud condensation nuclei (CCN) of different dry sizes. These assumptions are used in large-scale models to map the bulk aqueous chemistry sulfate production, which is largely proportional to the liquid water mass, to the changes in aerosol size distribution. It is shown that the commonly used assumptions that the droplet mass is independent of CCN size or that the droplet mass is proportional to the CCN size to the third power do not perform

  17. Hygroscopic properties of NaCl and NaNO3 mixture particles as reacted inorganic sea-salt aerosol surrogates

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Kim, H.; Park, G.; Li, X.; Eom, H.-J.; Ro, C.-U.

    2014-12-01

    crystallized NaCl moiety in the center, surrounded either by the eutonic component (for XNaCl > 0.38) or NaNO3 (for XNaCl ≤ 0.38). During the humidifying or dehydration process, the amount of eutonic composed part drives particle/droplet growth or shrinkage at the MDRH or MERH (second ERH), respectively, and the amount of remnant pure salts (NaCl or NaNO3 in NaCl- or NaNO3-rich particles, respectively) drives the second DRHs or first ERHs, respectively. Therefore, their behavior can be a precursor to the optical properties and direct radiative forcing for these atmospherically relevant mixture particles representing the coarse, reacted inorganic SSAs. In addition, the NaCl-NaNO3 mixture aerosol particles can maintain an aqueous phase over a wider RH range than the genuine SSA surrogate (i.e., pure NaCl particles), making their heterogeneous chemistry more probable.

  18. Hygroscopic properties of NaCl and NaNO3 mixture particles as reacted inorganic sea-salt aerosol surrogates

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Kim, H.; Park, G.; Li, X.; Eom, H.-J.; Ro, C.-U.

    2015-03-01

    crystallized NaCl moiety in the center, surrounded either by the eutonic component (for XNaCl > 0.38) or NaNO3 (for XNaCl ≤ 0.38). During the humidifying or dehydration process, the amount of eutonic composed part drives particle/droplet growth or shrinkage at the MDRH or MERH (second ERH), respectively, and the amount of pure salts (NaCl or NaNO3 in NaCl- or NaNO3-rich particles, respectively) drives the second DRHs or first ERHs, respectively. Therefore, their behavior can be a precursor to the optical properties and direct radiative forcing for these atmospherically relevant mixture particles representing the coarse, reacted inorganic SSAs. In addition, the NaCl-NaNO3 mixture aerosol particles can maintain an aqueous phase over a wider RH range than pure NaCl particles as SSA surrogate, making their heterogeneous chemistry more probable.

  19. Regional simulation of aerosol radiative effects and their influence on rainfall over India using WRFChem model

    NASA Astrophysics Data System (ADS)

    Kedia, Sumita; Cherian, Ribu; Islam, Sahidul; Das, Subrata Kumar; Kaginalkar, Akshara

    2016-12-01

    A regional climate model, WRFChem has been utilized to simulate aerosol and rainfall distribution over India during July 2010 which was a normal monsoon year. Two identical simulations, one includes aerosol feedback via their direct and indirect effects and other one without any aerosol effect, are structured to understand the impact of aerosol net (direct + indirect) effect on rainfall pattern over India. Model results are accompanied by satellite and ground based observations to examine the robustness of the model simulations. It is shown that the model can reproduce the spatial and temporal characteristics of meteorological parameters, rainfall distribution, aerosol optical depth and single scattering albedo reasonably well. Model simulated spatial distribution and magnitude of aerosol optical depth over India are realistic, particularly over northwest India, where mineral dust is a major contributor to the total aerosol loading and over Indo-Gangetic Plain region (IGP) where AOD remains high throughout the year. Net (shortwave + longwave) atmospheric heating rate is the highest (> 0.27 K day - 1) over east IGP due to abundant dust and anthropogenic aerosols while it is the lowest over peninsular India and over the Thar desert (< 0.03 K day - 1) which can be attributed to less aerosol concentration and longwave cooling, respectively. It is shown that, inclusion of aerosol direct and indirect effects have strong influence ( ± 20%) on rainfall magnitude and its distribution over Indian subcontinent during monsoon.

  20. Modelling aerosol processes related to the atmospheric dispersion of sarin.

    PubMed

    Kukkonen, J; Riikonen, K; Nikmo, J; Jäppinen, A; Nieminen, K

    2001-08-17

    We have developed mathematical models for evaluating the atmospheric dispersion of selected chemical warfare agents (CWA), including the evaporation and settling of contaminant liquid droplets. The models and numerical results presented may be utilised for designing protection and control measures against the conceivable use of CWA's. The model AERCLOUD (AERosol CLOUD) was extended to treat two nerve agents, sarin and VX, and the mustard agent. This model evaluates the thermodynamical evolution of a five-component aerosol mixture, consisting of two-component droplets together with the surrounding three-component gas. We have performed numerical computations with this model on the evaporation and settling of airborne sarin droplets in characteristic dispersal and atmospheric conditions. In particular, we have evaluated the maximum radii (r(M)) of a totally evaporating droplet, in terms of the ambient temperature and contaminant vapour concentration. The radii r(M) range from approximately 15-80 microm for sarin droplets for the selected ambient conditions and initial heights. We have also evaluated deposition fractions in terms of the initial droplet size.

  1. Aerosol data assimilation in the chemical transport model MOCAGE during the TRAQA/ChArMEx campaign: aerosol optical depth

    NASA Astrophysics Data System (ADS)

    Sič, Bojan; El Amraoui, Laaziz; Piacentini, Andrea; Marécal, Virginie; Emili, Emanuele; Cariolle, Daniel; Prather, Michael; Attié, Jean-Luc

    2016-11-01

    In this study, we describe the development of the aerosol optical depth (AOD) assimilation module in the chemistry transport model (CTM) MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle). Our goal is to assimilate the spatially averaged 2-D column AOD data from the National Aeronautics and Space Administration (NASA) Moderate-resolution Imaging Spectroradiometer (MODIS) instrument, and to estimate improvements in a 3-D CTM assimilation run compared to a direct model run. Our assimilation system uses 3-D-FGAT (first guess at appropriate time) as an assimilation method and the total 3-D aerosol concentration as a control variable. In order to have an extensive validation dataset, we carried out our experiment in the northern summer of 2012 when the pre-ChArMEx (CHemistry and AeRosol MEditerranean EXperiment) field campaign TRAQA (TRAnsport à longue distance et Qualité de l'Air dans le bassin méditerranéen) took place in the western Mediterranean basin. The assimilated model run is evaluated independently against a range of aerosol properties (2-D and 3-D) measured by in situ instruments (the TRAQA size-resolved balloon and aircraft measurements), the satellite Spinning Enhanced Visible and InfraRed Imager (SEVIRI) instrument and ground-based instruments from the Aerosol Robotic Network (AERONET) network. The evaluation demonstrates that the AOD assimilation greatly improves aerosol representation in the model. For example, the comparison of the direct and the assimilated model run with AERONET data shows that the assimilation increased the correlation (from 0.74 to 0.88), and reduced the bias (from 0.050 to 0.006) and the root mean square error in the AOD (from 0.12 to 0.07). When compared to the 3-D concentration data obtained by the in situ aircraft and balloon measurements, the assimilation consistently improves the model output. The best results as expected occur when the shape of the vertical profile is correctly simulated by the direct model. We

  2. Modeling ozone and aerosol formation and transport in the pacific northwest with the community Multi-Scale Air Quality (CMAQ) modeling system.

    PubMed

    O'Neill, Susan M; Lamb, Brian K; Chen, Jack; Claiborn, Candis; Finn, Dennis; Otterson, Sally; Figueroa, Cristiana; Bowman, Clint; Boyer, Mike; Wilson, Rob; Arnold, Jeff; Aalbers, Steven; Stocum, Jeffrey; Swab, Christopher; Stoll, Matt; Dubois, Mike; Anderson, Mary

    2006-02-15

    The Community Multi-Scale Air Quality (CMAQ) modeling system was used to investigate ozone and aerosol concentrations in the Pacific Northwest (PNW) during hot summertime conditions during July 1-15, 1996. Two emission inventories (El) were developed: emissions for the first El were based upon the National Emission Trend 1996 (NET96) database and the BEIS2 biogenic emission model, and emissions for the second El were developed through a "bottom up" approach that included biogenic emissions obtained from the GLOBEIS model. The two simulations showed that elevated PM2.5 concentrations occurred near and downwind of the Interstate-5 corridor along the foothills of the Cascade Mountains and in forested areas of central Idaho. The relative contributions of organic and inorganic aerosols varied by region, but generally organic aerosols constituted the largest fraction of PM2.5. In wilderness areas near the 1-5 corridor, organic carbon from anthropogenic sources contributed approximately 50% of the total organic carbon with the remainder from biogenic precursors, while in wilderness areas in Idaho, biogenic organic carbon accounted for 80% of the total organic aerosol. Regional analysis of the secondary organic aerosol formation in the Columbia River Gorge, Central Idaho, and the Olympics/Puget Sound showed that the production rate of secondary organic carbon depends on local terpene concentrations and the local oxidizing capacity of the atmosphere, which was strongly influenced by anthropogenic emissions. Comparison with observations from 12 IMPROVE sites and 21 ozone monitoring sites showed that results from the two El simulations generally bracketed the average observed PM parameters and that errors calculated for the model results were within acceptable bounds. Analysis across all statistical parameters indicated that the NW-AIRQUEST El solution performed better at predicting PM2.5, PM1, and beta(ext) even though organic carbon PM was over-predicted, and the NET96 El

  3. Tropospheric aerosol size distributions simulated by three online global aerosol models using the M7 microphysics module

    SciTech Connect

    Zhang, Kai; Wan, Hui; Wang, Bin; Zhang, Meigen; Feichter, J.; Liu, Xiaohong

    2010-07-14

    Tropospheric aerosol size distributions are simulated by three online global models that employ exactly the same modal approach but differ in many aspects such as model meteorology, natural aerosol emissions, sulfur chemistry, and the parameterization of deposition processes. The main purpose of this study is to identify where the largest inter-model discrepancies occur and what the main reasons are. The number concentrations of different aerosol size ranges are compared among the three models and against observations. Overall all the three models can capture the basic features of the observed aerosol number spatial distributions. The magnitude of the number concentration of each mode is consistent among the three models. Quantitative differences are also clearly detectable. For the soluble and insoluble coarse mode and accumulation mode, inter-model discrepancies mainly result from differences in the sea salt and dust emissions, as well as the different strengths of the convective transport in the meteorological models. For the nucleation mode and the soluble Aitken mode, the spread of the model results is largest in the tropics and in the middle and upper troposphere. Diagnostics and sensitivity experiments suggest that this large spread is closely related to the sulfur cycle in the models, which is strongly affected by the choice of sulfur chemistry scheme, its coupling with the convective transport and wet deposition calculation, and the related meteorological fields such as cloud cover, cloud water content, and precipitation. The aerosol size distributions simulated by the three models are compared to observations in the boundary layer. The characteristic shape and magnitude of the distribution functions are reasonably reproduced in typical conditions (i.e., clean, polluted and transition areas). Biases in the mode parameters over the remote oceans and the China adjacent seas are probably caused by the fixed mode variance in the mathematical formulations used

  4. Tropospheric aerosol size distributions simulated by three online global aerosol models using the M7 microphysics module

    NASA Astrophysics Data System (ADS)

    Zhang, K.; Wan, H.; Wang, B.; Zhang, M.; Feichter, J.; Liu, X.

    2010-03-01

    Tropospheric aerosol size distributions are simulated by three online global models that employ exactly the same modal approach but differ in many aspects such as model meteorology, natural aerosol emissions, sulfur chemistry, and the parameterization of deposition processes. The main purpose of this study is to identify where the largest inter-model discrepancies occur and what the main reasons are. The number concentrations of different aerosol size ranges are compared among the three models and against observations. Overall all the three models can capture the basic features of the observed aerosol number spatial distributions. The magnitude of the number concentration of each mode is consistent among the three models. Quantitative differences are also clearly detectable. For the soluble and insoluble coarse mode and accumulation mode, inter-model discrepancies mainly result from differences in the sea salt and dust emissions, as well as the different strengths of the convective transport in the meteorological models. For the nucleation mode and the soluble Aitken mode, the spread of the model results is largest in the tropics and in the middle and upper troposphere. Diagnostics and sensitivity experiments suggest that this large spread is closely related to the sulfur cycle in the models, which is strongly affected by the choice of sulfur chemistry scheme, its coupling with the convective transport and wet deposition calculation, and the related meteorological fields such as cloud cover, cloud water content, and precipitation. The aerosol size distributions simulated by the three models are compared to observations in the boundary layer. The characteristic shape and magnitude of the distribution functions are reasonably reproduced in typical conditions (i.e., clean, polluted and transition areas). Biases in the mode parameters over the remote oceans and the China adjacent seas are probably caused by the fixed mode variance in the mathematical formulations used

  5. Wintertime organic and inorganic aerosols in Lanzhou, China: sources, processes, and comparison with the results during summer

    NASA Astrophysics Data System (ADS)

    Xu, Jianzhong; Shi, Jinsen; Zhang, Qi; Ge, Xinlei; Canonaco, Francesco; Prévôt, André S. H.; Vonwiller, Matthias; Szidat, Sönke; Ge, Jinming; Ma, Jianmin; An, Yanqing; Kang, Shichang; Qin, Dahe

    2016-12-01

    Lanzhou, which is located in a steep alpine valley in western China, is one of the most polluted cities in China during the wintertime. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a seven-wavelength aethalometer, and a scanning mobility particle sizer (SMPS) were deployed during 10 January to 4 February 2014 to study the mass concentrations, chemical processes, and sources of submicrometer particulate matter (PM1). The average PM1 concentration during this study was 57.3 µg m-3 (ranging from 2.1 to 229.7 µg m-3 for hourly averages), with organic aerosol (OA) accounting for 51.2 %, followed by nitrate (16.5 %), sulfate (12.5 %), ammonium (10.3 %), black carbon (BC, 6.4 %), and chloride (3.0 %). The mass concentration of PM1 during winter was more than twice the average value observed at the same site in summer 2012 (24.5 µg m-3), but the mass fraction of OA was similar in the two seasons. Nitrate contributed a significantly higher fraction to the PM1 mass in winter than summer (16.5 % vs. 10 %), largely due to more favored partitioning to the particle phase at low air temperature. The mass fractions of both OA and nitrate increased by ˜ 5 % (47 to 52 for OA and 13 to 18 % for nitrate) with the increase of the total PM1 mass loading, while the average sulfate fraction decreased by 6 % (17 to 11 %), indicating the importance of OA and nitrate for the heavy air pollution events in Lanzhou. The size distributions of OA, nitrate, sulfate, ammonium, and chloride all peaked at ˜ 500 nm, with OA being slightly broader, suggesting that aerosol particles were internally mixed during winter, likely due to frequently calm and stagnant air conditions during wintertime in Lanzhou (average wind speed: 0.82 m s-1).The average mass spectrum of OA showed a medium oxidation degree (average O / C ratio of 0.28), which was lower than that during summer 2012 (O / C = 0.33). This is consistent with weaker photochemical processing

  6. Modeling Organic Aerosols during MILAGRO: Application of the CHIMERE Model and Importance of Biogenic Secondary Organic Aerosols

    SciTech Connect

    Hodzic, Alma; Jimenez, Jose L.; Madronich, Sasha; Aiken, Allison; Bessagnet, Bertrand; Curci, Gabriele; Fast, Jerome D.; Lamarque, J.-F.; Onasch, Timothy B.; Roux, Gregory; Schauer, James J.; Stone, Elizabeth A.

    2009-09-22

    The meso-scale chemistry-transport model CHIMERE is used to assess our understanding of major sources and formation processes leading to a fairly large amount of organic aerosols [OA, including primary OA (POA) and secondary OA (SOA)] observed in Mexico City during the MILAGRO field project (March 2006). Chemical analyses of submicron aerosols from aerosol mass spectrometers (AMS) indicate that organic particles found in the Mexico City basin have a large fraction of oxygenated organic species (OOA), which have strong correspondence with SOA, and that their production actively continues downwind of the city. The SOA formation is modeled here by the first-generation oxidation of anthropogenic (i.e., aromatics, alkanes) and biogenic (i.e., monoterpenes and isoprene) precursors and their partitioning into both organic and aqueous phases. The near-surface model evaluation shows that predicted OA correlates reasonably well with measurements during the campaign, however it remains a factor of 2 lower than the measured total OA. Fairly good agreement is found between predicted and observed POA within the city suggesting that anthropogenic and biomass burning emissions are reasonably captured. Consistent with previous studies in Mexico City, large discrepancies are encountered for SOA species, with a factor of 5-10 model underestimate. When only anthropogenic SOA precursors were considered, the model was able to reproduce within a factor of two the sharp increase in SOA concentrations during the late morning at both urban and near-urban locations. However, predicted SOA concentrations were unrealistically low when photochemistry was not active, especially overnight. These nighttime discrepancies were not significantly reduced when greatly enhanced partitioning to the aerosol phase was assumed. Model sensitivity results suggest that observed nighttime SOA concentrations are strongly influenced by the regional background (~2µg/m3) from biogenic origin, which is transported

  7. Aerosol effect on the warm rain formation process: Satellite observations and modeling

    NASA Astrophysics Data System (ADS)

    Suzuki, Kentaroh; Stephens, Graeme L.; Lebsock, Matthew D.

    2013-01-01

    This study demonstrates how aerosols influence the liquid precipitation formation process. This demonstration is provided by the combined use of satellite observations and global high-resolution model simulations. Methodologies developed to examine the warm cloud microphysical processes are applied to both multi-sensor satellite observations and aerosol-coupled global cloud-resolving model (GCRM) results to illustrate how the warm rain formation process is modulated under different aerosol conditions. The observational analysis exhibits process-scale signatures of rain suppression due to increased aerosols, providing observational evidence of the aerosol influence on precipitation. By contrast, the corresponding statistics obtained from the model show a much faster rain formation even for polluted aerosol conditions and much weaker reduction of precipitation in response to aerosol increase. It is then shown that this reduced sensitivity points to a fundamental model bias in the warm rain formation process that in turn biases the influence of aerosol on precipitation. A method of improving the model bias is introduced in the context of a simplified single-column model (SCM) that represents the cloud-to-rain water conversion process in a manner similar to the original GCRM. Sensitivity experiments performed by modifying the model assumptions in the SCM and their comparisons to satellite statistics both suggest that the auto-conversion scheme has a critical role in determining the precipitation response to aerosol perturbations and also provide a novel way of constraining key parameters in the auto-conversion schemes of global models.

  8. Intercomparison of aerosol microphysics modules in the framework of the ECHAM5 climate model

    NASA Astrophysics Data System (ADS)

    Hommel, R.; Kokkola, H.; Kazil, J.; Niemeier, U.; Partanen, A. I.; Feichter, J.; Timmreck, C.

    2009-04-01

    Aerosols in the atmosphere are an elementary constituent of the atmospheric composition and affect the global climate through a variety of physical and chemical interactions in the troposphere and stratosphere. Large volcanic eruptions alter the Earth's radiative balance and interfere with the catalytic cycles of ozone depletion mainly by the formation of micrometer size aerosol particles above the tropopause. Recent experimental and numerical investigations of process oriented aerosol-climate interactions revealed that appropriate climate effects can only be modeled when informations about the aerosol size and number spectra are provided. Nevertheless in the majority of climate models volcanic perturbations of the stratosphere are either prescribed based on the aerosol parameters of interested (surface area, optical depth) or the aerosol microphysics is considered explicitly but with a heavily reduced number of degrees of freedom. This yields e.g. to underestimations of surface temperature effects in the fade of an eruption. To overcome that weakness, we tested three aerosol modules currently available in the framework of the climate model ECHAM5 in environmental conditions assumed to be representative in the stratosphere after the injection of SO2 from modest to large volcanic eruptions. The study focuses on the evolution of liquid H2SO4/H2O aerosol. The modal modal M7, currently the default aerosol scheme in ECHAM5, is compared with two sectional aerosol schemes: the moving centre sectional aerosol scheme SALSA, and the fixed sectional scheme SAM2. Since direct measurements of particle size informations during the initial stage of a volcanic injection in the stratosphere are not available, the detailed sectional aerosol model MAIA is used as a reference in this study. It is shown that all modules are able to represent a "typical" stratospheric background aerosol distribution when the particles are formed via the oxidation pathway of SO2. However, the modules

  9. Verification of the naval oceanic vertical aerosol model during FIRE

    NASA Technical Reports Server (NTRS)

    Davidson, K. L.; Deleeuw, G.; Gathman, S. G.; Jensen, D. R.

    1990-01-01

    The value of Naval Oceanic Vertical Aerosol Model (NOVAM) is illustrated for estimating the non-uniform and non-logarithmic extinction profiles, based on a severe test involving conditions close to and beyond the limits of applicability of NOVAM. A more comprehensive evaluation of NOVAM from the FIRE data is presented, which includes a clear-air case. For further evaluation more data are required on the vertical structure of the extinction in the marine atmospheric boundary layer (MABL), preferably for different meteorological conditions and in different geographic areas (e.g., ASTEX).

  10. Modeling the aerosols in the atmosphere of Titan

    NASA Astrophysics Data System (ADS)

    Thomas-Osip, Joanna Elizabeth

    2001-09-01

    A combination of laboratory experiments, theoretical modeling, and spacecraft in situ observations is employed to characterize the aerosols in the atmosphere of Titan. The scattering properties of model aerosols were measured using the Microwave Analog Light Scattering Facility at the University of Florida and complemented with theoretical modeling of single scattering characteristics and radiative transfer in Titan's atmosphere. This study compares these modeling results with photopolarimetric observations made over a range of phase angles by the Pioneer 11 and Voyagers 1 and 2 spacecraft approximately 20 years ago. Important results of this work include a survey of the scattering properties of different particle shapes necessary to accurately interpret these observations without introducing non-physical assumptions about the particles or requiring additional free parameters to the radiative transfer models. Previous studies use calculation methods which, due to computing memory and processing time requirements, a priori exclude much of the phase space that the microwave analog laboratory is ideal for exploring. The goal of the present work, to directly constrain aerosol physical characteristics, is addressed by studying in a consistent manner how a variety of particle morphologies affect polarization and intensity measurements of Titan's atmosphere. Single liquid drops are modeled using spheres for which scattering patterns can be easily calculated with Mie theory. Cubes are used as a representation of solids with sharp edges due to fragmentation. More complex particle morphologies are modeled as aggregates that are likely formed by collisions between semi-liquid spheres that stick together instead of merging. Radiative transfer calculations for model atmospheres containing these particles are constrained by direct comparison to in situ spacecraft observations. Based on these comparisons, many model morphologies are excluded from further consideration and the

  11. The role of aerosols in cloud drop parameterizations and its applications in global climate models

    SciTech Connect

    Chuang, C.C.; Penner, J.E.

    1996-04-01

    The characteristics of the cloud drop size distribution near cloud base are initially determined by aerosols that serve as cloud condensation nuclei and the updraft velocity. We have developed parameterizations relating cloud drop number concentration to aerosol number and sulfate mass concentrations and used them in a coupled global aerosol/general circulation model (GCM) to estimate the indirect aerosol forcing. The global aerosol model made use of our detailed emissions inventories for the amount of particulate matter from biomass burning sources and from fossil fuel sources as well as emissions inventories of the gas-phase anthropogenic SO{sub 2}. This work is aimed at validating the coupled model with the Atmospheric Radiation Measurement (ARM) Program measurements and assessing the possible magnitude of the aerosol-induced cloud effects on climate.

  12. Inorganic Nanovehicle Targets Tumor in an Orthotopic Breast Cancer Model

    NASA Astrophysics Data System (ADS)

    Choi, Goeun; Kwon, Oh-Joon; Oh, Yeonji; Yun, Chae-Ok; Choy, Jin-Ho

    2014-03-01

    The clinical efficacy of conventional chemotherapeutic agent, methotrexate (MTX), can be limited by its very short plasma half-life, the drug resistance, and the high dosage required for cancer cell suppression. In this study, a new drug delivery system is proposed to overcome such limitations. To realize such a system, MTX was intercalated into layered double hydroxides (LDHs), inorganic drug delivery vehicle, through a co-precipitation route to produce a MTX-LDH nanohybrid with an average particle size of approximately 130 nm. Biodistribution studies in mice bearing orthotopic human breast tumors revealed that the tumor-to-liver ratio of MTX in the MTX-LDH-treated-group was 6-fold higher than that of MTX-treated-one after drug treatment for 2 hr. Moreover, MTX-LDH exhibited superior targeting effect resulting in high antitumor efficacy inducing a 74.3% reduction in tumor volume compared to MTX alone, and as a consequence, significant survival benefits. Annexin-V and propidium iodine dual staining and TUNEL analysis showed that MTX-LDH induced a greater degree of apoptosis than free MTX. Taken together, our data demonstrate that a new MTX-LDH nanohybrid exhibits a superior efficacy profile and improved distribution compared to MTX alone and has the potential to enhance therapeutic efficacy via inhibition of tumor proliferation and induction of apoptosis.

  13. Assimilation of Aerosols from Biomass Burning by the Radiative Transfer Model Brasil-Sr

    NASA Astrophysics Data System (ADS)

    Costa, R. S.; Gonçalves, A. R.; Souza, J. G.; Martins, F. R.; Pereira, E. B.

    2015-12-01

    The radiative transfer model BRASIL-SR is the main tool used by the Earth System Science Centre from the National Institute for Space Research (CCST / INPE) for solar energy resource assessment. Due to large and frequent events of burning biomass in Brazil there is a need to improve the aerosol representation in this model, mainly during the dry season (September - November) in Northern and Central Brazil. The standard aerosol representation in this model is inadequate to capture these events. It is based on the mean monthly climatological horizontal visibility with latitudinal values based on coarse global observation data. To improve the aerosol representation, climatological data of daily horizontal visibility from National Institute of Meteorology (INMET) was used to generate monthly averages from 1999 to 2012. To do a better representation of aerosols from burning biomass events, from megacities aerosol generation, and from transport processes, horizontal visibility estimates performed using aerosol optical thickness at 550 nm data from MACC Project Reanalysis model were used to adjust the aerosol representation in regions were the simple horizontal visibility fails. A methodology to generate these new visibility data from the Reanalysis was made and the resulting data was compared with the average horizontal visibility to implement a new corrected database. The solar irradiation simulated by the model using this new aerosol representation proved to be better than the previous version of the model in all regions with high aerosol loading.

  14. Impacts of increasing the aerosol complexity in the Met Office global numerical weather prediction model

    NASA Astrophysics Data System (ADS)

    Mulcahy, J. P.; Walters, D. N.; Bellouin, N.; Milton, S. F.

    2014-05-01

    The inclusion of the direct and indirect radiative effects of aerosols in high-resolution global numerical weather prediction (NWP) models is being increasingly recognised as important for the improved accuracy of short-range weather forecasts. In this study the impacts of increasing the aerosol complexity in the global NWP configuration of the Met Office Unified Model (MetUM) are investigated. A hierarchy of aerosol representations are evaluated including three-dimensional monthly mean speciated aerosol climatologies, fully prognostic aerosols modelled using the CLASSIC aerosol scheme and finally, initialised aerosols using assimilated aerosol fields from the GEMS project. The prognostic aerosol schemes are better able to predict the temporal and spatial variation of atmospheric aerosol optical depth, which is particularly important in cases of large sporadic aerosol events such as large dust storms or forest fires. Including the direct effect of aerosols improves model biases in outgoing long-wave radiation over West Africa due to a better representation of dust. However, uncertainties in dust optical properties propagate to its direct effect and the subsequent model response. Inclusion of the indirect aerosol effects improves surface radiation biases at the North Slope of Alaska ARM site due to lower cloud amounts in high-latitude clean-air regions. This leads to improved temperature and height forecasts in this region. Impacts on the global mean model precipitation and large-scale circulation fields were found to be generally small in the short-range forecasts. However, the indirect aerosol effect leads to a strengthening of the low-level monsoon flow over the Arabian Sea and Bay of Bengal and an increase in precipitation over Southeast Asia. Regional impacts on the African Easterly Jet (AEJ) are also presented with the large dust loading in the aerosol climatology enhancing of the heat low over West Africa and weakening the AEJ. This study highlights the

  15. Impacts of increasing the aerosol complexity in the Met Office global NWP model

    NASA Astrophysics Data System (ADS)

    Mulcahy, J. P.; Walters, D. N.; Bellouin, N.; Milton, S. F.

    2013-11-01

    Inclusion of the direct and indirect radiative effects of aerosols in high resolution global numerical weather prediction (NWP) models is being increasingly recognised as important for the improved accuracy of short-range weather forecasts. In this study the impacts of increasing the aerosol complexity in the global NWP configuration of the Met Office Unified Model (MetUM) are investigated. A hierarchy of aerosol representations are evaluated including three dimensional monthly mean speciated aerosol climatologies, fully prognostic aerosols modelled using the CLASSIC aerosol scheme and finally, initialised aerosols using assimilated aerosol fields from the GEMS project. The prognostic aerosol schemes are better able to predict the temporal and spatial variation of atmospheric aerosol optical depth, which is particularly important in cases of large sporadic aerosol events such as large dust storms or forest fires. Including the direct effect of aerosols improves model biases in outgoing longwave radiation over West Africa due to a better representation of dust. However, uncertainties in dust optical properties propogate to its direct effect and the subsequent model response. Inclusion of the indirect aerosol effects improves surface radiation biases at the North Slope of Alaska ARM site due to lower cloud amounts in high latitude clean air regions. This leads to improved temperature and height forecasts in this region. Impacts on the global mean model precipitation and large-scale circulation fields were found to be generally small in the short range forecasts. However, the indirect aerosol effect leads to a strengthening of the low level monsoon flow over the Arabian Sea and Bay of Bengal and an increase in precipitation over Southeast Asia. Regional impacts on the African Easterly Jet (AEJ) are also presented with the large dust loading in the aerosol climatology enhancing of the heat low over West Africa and weakening the AEJ. This study highlights the importance

  16. An aerosol challenge model of tuberculosis in Mauritian cynomolgus macaques

    PubMed Central

    Sharpe, S. A.; White, A. D.; Sibley, L.; Gleeson, F.; Hall, G. A.; Basaraba, R. J.; McIntyre, A.; Clark, S. O.; Gooch, K.; Marsh, P. D.; Williams, A.; Dennis, M. J.

    2017-01-01

    Background New interventions for tuberculosis are urgently needed. Non-human primate (NHP) models provide the most relevant pre-clinical models of human disease and play a critical role in vaccine development. Models utilising Asian cynomolgus macaque populations are well established but the restricted genetic diversity of the Mauritian cynomolgus macaques may be of added value. Methods Mauritian cynomolgus macaques were exposed to a range of doses of M. tuberculosis delivered by aerosol, and the outcome was assessed using clinical, imaging and pathology-based measures. Results All macaques developed characteristic clinical signs and disease features of tuberculosis (TB). Disease burden and the ability to control disease were dependent on exposure dose. Mauritian cynomolgus macaques showed less variation in pulmonary disease burden and total gross pathology scores within exposure dose groups than either Indian rhesus macaques or Chinese cynomolgus macaques Conclusions The genetic homogeneity of Mauritian cynomolgus macaques makes them a potentially useful model of human tuberculosis. PMID:28273087

  17. Development towards a global operational aerosol consensus: basic climatological characteristics of the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME)

    NASA Astrophysics Data System (ADS)

    Sessions, W. R.; Reid, J. S.; Benedetti, A.; Colarco, P. R.; da Silva, A.; Lu, S.; Sekiyama, T.; Tanaka, T. Y.; Baldasano, J. M.; Basart, S.; Brooks, M. E.; Eck, T. F.; Iredell, M.; Hansen, J. A.; Jorba, O. C.; Juang, H.-M. H.; Lynch, P.; Morcrette, J.-J.; Moorthi, S.; Mulcahy, J.; Pradhan, Y.; Razinger, M.; Sampson, C. B.; Wang, J.; Westphal, D. L.

    2014-06-01

    Over the past several years, there has been a rapid development in the number and quality of global aerosol models intended for operational forecasting use. Indeed, most centers with global numerical weather prediction (NWP) capabilities have some program for aerosol prediction. These aerosol models typically have differences in their underlying meteorology as well as aerosol sources, sinks, microphysics and transformations. However, like similar diversity in aerosol climate models, the aerosol forecast models have fairly similar overall bulk error statistics for aerosol optical thickness (AOT)-one of the few aerosol metrics that is globally available. Experience in climate and weather prediction has shown that in situations such as this where there are several independent models, a multi-model ensemble or consensus will be top performing in many key error metrics. Further, multi-model ensembles provide a highly valuable tool for forecasters attempting to predict severe aerosol events. Here we present the first steps in developing a global multi-model aerosol forecasting ensemble intended for eventual operational and basic research use. Drawing from members of the International Cooperative for Aerosol Prediction (ICAP) latest generation of quasi-operational aerosol models, five day AOT forecasts are analyzed for December 2011 through November 2012 from four institutions: ECMWF, JMA, NASA GSFC, and NRL/FNMOC. For dust, we also include the NOAA NGAC product in our analysis. The Barcelona Supercomputing Centre (NMMC) and UK Met office dust product have also recent become available with ICAP, but have insufficient data to be included in this analysis period. A simple consensus ensemble of member and mean AOT fields for modal species (e.g., fine and coarse mode, and a separate dust ensemble) is used to create the ICAP Multi-Model Ensemble (ICAP-MME). The ICAP-MME is run daily at 0Z for 6 hourly forecasts out to 120 h. Basing metrics on comparisons to 21 regionally

  18. Chemical characterization of the inorganic fraction of aerosols and mechanisms of the neutralization of atmospheric acidity in Athens, Greece

    NASA Astrophysics Data System (ADS)

    Karageorgos, E. T.; Rapsomanikis, S.

    2007-06-01

    The PM10 mass concentration levels and inorganic chemical composition were determined on 12-h resolution sampling during August 2003 and March 2004, in the centre of Athens, Greece. The August 2003 campaign mean PM10 mass concentration, obtained by Beta Attenuation at 5 m above ground in Athinas Street, was 56 μg m-3 while the corresponding value for March 2004 was 92 μg m-3. In both campaigns the E.U. imposed daily limit of 50 μg m-3 was exceeded on several days. During the March campaign, in Athinas Street, additionally obtained DSFU-PM10 (PM10-2.5+PM2.5) gravimetric mass concentrations (mean: 121 μg m-3) in the "breathing zone", at 1.5 m above ground were significantly higher compared to the respective mean PM10 mass concentrations obtained by the same method at 25 m above ground, in a second site (AEDA; mean: 86 μg m-3) also in the centre of the city. The above findings suggest that, for a realistic estimation of the exposure of citizens to particulate matter, PM10 sampling in the "breathing zone" (1.5-3 m above ground) is necessary. Such data are presented for the first time for the centre of Athens. In both campaigns, calcium was found to be the predominant component of the coarse fraction while crust-related aluminosilicates and iron were the other major components. The above elements constitute the most important components of the fine fraction, together with the predominant sulphur. All toxic metals were found in concentrations below the established air quality limits, and most of them in lower concentrations compared to older studies. Lead in particular, appeared mostly in the fine fraction and in very low concentrations compared to studies dating more than a decade back. The predominant ions of the coarse fraction have been found to be Ca2+, NO3-, Na+ and Cl-, while SO42-, Ca2+ and NH4+ were the major ionic components of the fine fraction. In the fine particles, a low molar ratio of NH4+/SO42- indicated an ammonium-poor ambient air, and together

  19. EMAC model evaluation and analysis of atmospheric aerosol properties and distribution with a focus on the Mediterranean region

    NASA Astrophysics Data System (ADS)

    de Meij, A.; Pozzer, A.; Pringle, K. J.; Tost, H.; Lelieveld, J.

    2012-10-01

    The skill of the EMAC atmospheric chemistry-climate model to predict the aerosol optical depth (AOD) is evaluated by comparing with remote sensing data products from AERONET, MODIS, MISR and CALIOP with a focus on the Mediterranean region. In addition, calculated aerosol concentrations are compared with measurements from the CASTNET, IMPROVE, EMEP, EANET and CAWNET networks. Calculated sulphate concentrations are in good agreement with the measurements, whilst the agreement is less satisfactory for ammonium and nitrate, possibly because of measurement artefacts. The model reproduces the main spatial atmospheric distribution of the sulphate and ammonium aerosols. For nitrate some differences are found when compared to observations. The analysis of black and organic carbon (BC and OC) over Europe shows that the model typically overestimates observed BC concentrations by a factor of 1.6 and underestimates OC by a factor of 2.6. For the USA BC and OC are in general overestimated and for China BC and OC are in general underestimated by the model. The seasonal distribution of elevated AODs is well represented by the model when compared to MODIS and MISR, though AODs are somewhat low-biased. Calculated annual mean AODs are in general lower than of AERONET and the temporal correlation coefficients vary between 0.11 and 0.68. High temporal correlation coefficients are found for biomass burning regions (South America and West Africa), indicating that the seasonal cycle of this source category is well represented in the model, based on the GFED inventory. High temporal correlation coefficients are obtained for the Mediterranean region during summer, which indicates that the model captures the dust intrusions. Our model calculations show that inorganic particles and associated water are the most abundant aerosol components over Europe, North America and Asia, whilst over the Mediterranean during summer dust dominates the total AOD. An analysis of the meridional vertical

  20. Change in global aerosol composition since preindustrial times

    NASA Astrophysics Data System (ADS)

    Tsigaridis, K.; Krol, M.; Dentener, F. J.; Balkanski, Y.; Lathière, J.; Metzger, S.; Hauglustaine, D. A.; Kanakidou, M.

    2006-06-01

    To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. This is the first 3-d modeling study that focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3-, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34-42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has

  1. Change in global aerosol composition since preindustrial times

    NASA Astrophysics Data System (ADS)

    Tsigaridis, K.; Krol, M.; Dentener, F. J.; Balkanski, Y.; Lathière, J.; Metzger, S.; Hauglustaine, D. A.; Kanakidou, M.

    2006-11-01

    To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3aerosol loading is dampened by a 34-42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased

  2. Uncertainty associated with convective wet removal of entrained aerosols in a global climate model

    NASA Astrophysics Data System (ADS)

    Croft, B.; Pierce, J. R.; Martin, R. V.; Hoose, C.; Lohmann, U.

    2012-11-01

    The uncertainties associated with the wet removal of aerosols entrained above convective cloud bases are investigated in a global aerosol-climate model (ECHAM5-HAM) under a set of limiting assumptions for the wet removal of the entrained aerosols. The limiting assumptions for the wet removal of entrained aerosols are negligible scavenging and vigorous scavenging (either through activation, with size-dependent impaction scavenging, or with the prescribed fractions of the standard model). To facilitate this process-based study, an explicit representation of cloud-droplet-borne and ice-crystal-borne aerosol mass and number, for the purpose of wet removal, is introduced into the ECHAM5-HAM model. This replaces and is compared with the prescribed cloud-droplet-borne and ice-crystal-borne aerosol fraction scavenging scheme of the standard model. A 20% to 35% uncertainty in simulated global, annual mean aerosol mass burdens and optical depth (AOD) is attributed to different assumptions for the wet removal of aerosols entrained above convective cloud bases. Assumptions about the removal of aerosols entrained above convective cloud bases control modeled upper tropospheric aerosol concentrations by as much as one order of magnitude. Simulated aerosols entrained above convective cloud bases contribute 20% to 50% of modeled global, annual mean aerosol mass convective wet deposition (about 5% to 10% of the total dry and wet deposition), depending on the aerosol species, when including wet scavenging of those entrained aerosols (either by activation, size-dependent impaction, or with the prescribed fraction scheme). Among the simulations, the prescribed fraction and size-dependent impaction schemes yield the largest global, annual mean aerosol mass convective wet deposition (by about two-fold). However, the prescribed fraction scheme has more vigorous convective mixed-phase wet removal (by two to five-fold relative to the size-dependent impaction scheme) since nearly all

  3. Towards Improved MODIS Aerosol Retrieval over the US East Coast Region: Re-examining the Aerosol Model and Surface Assumptions

    NASA Technical Reports Server (NTRS)

    Levy, R. C.; Remer, L. A.; Kaufman, Y. J.; Holben, B. N.

    2002-01-01

    The MODerate resolution Imaging Spectrometer (MODIS) aboard the Terra and recently the Aqua platform, produces a set of aerosol products over both ocean and land regions. Previous validation efforts have shown that from a global perspective, aerosol optical depth (AOD) is successfully retrieved from MODIS. Even over coastal regions, the over- land and over-ocean retrievals are consistent with each other, and well matched with ground-based sunphotometer measurements (such as AERONET). However, the East Coast of the United States is one region where there is consistently a discrepancy between land and ocean retrievals. Over the ocean, MODIS AODs are consistent with coastal sunphotometer measurements, but over land, AODs are consistently over- estimated. In this study we use field data from the Chesapeake Lighthouse and Aircraft Measurements for Satellites experiment (CLAMS), (held during summer 2001) to determine the aerosol properties at a number of sites. Using the 6-S radiative transfer package, we compute simulated satellite radiances and compare them with observed MODIS radiances. We believe that the AOD over-estimation is not likely due to an incorrect choice of the urban/industrial aerosol models. Using 6-S to do an atmospheric correction for a very low AOD case, we show rather, that the discrepancies are likely a result of incorrect assumptions about the surface reflectance properties. Understanding and improving MODIS retrievals over the East Coast will not only improve the global quality of MODIS, but also would enable the use of MODIS as a tool for monitoring regional aerosol events.

  4. Characteristics-based sectional modeling of aerosol nucleation and condensation

    NASA Astrophysics Data System (ADS)

    Frederix, E. M. A.; Stanic, M.; Kuczaj, A. K.; Nordlund, M.; Geurts, B. J.

    2016-12-01

    A new numerical method for the solution of an internally mixed spatially homogeneous sectional model for aerosol nucleation and condensation is proposed. The characteristics method is used to predict droplet sizes within a discrete time step. The method is designed such that 1) a pre-specified number of moments of the droplet size distribution may be preserved, 2) there exists no time step stability restriction related to the condensation rate and section size, 3) highly skewed fixed sectional distributions may be used and 4) it is straightforward to extend to spatially inhomogeneous settings and to incorporate droplet coagulation and break-up. We derive, starting from mass conservation, a consistent internally mixed multi-species aerosol model. For certain condensational growth laws analytical solutions exist, against which the method is validated. Using two-moment and four-moment-preserving schemes, we find first order convergence of the numerical solution to the analytical result, as a function of the number of sections. As the four-moment-preserving scheme does not guarantee positivity of the solution, a hybrid scheme is proposed, which, when needed, locally reverts back to two-moment preservation, to prevent negativity. As an illustration, the method is applied to a complete multi-species homogeneous nucleation and condensation problem.

  5. Maritime Aerosol Network as a Component of AERONET - First Results and Comparison with Global Aerosol Models and Satellite Retrievals

    NASA Technical Reports Server (NTRS)

    Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.; Smyth, T. J.; Zielinski, T.; Zibordi, G.; Goes, J. I.; Harvey, M. J.; Quinn, P. K.; Nelson, N. B.; Radionov, V. F.; Duarte, C. M.; Remer, L. A.; Kahn, R. A.; Kleidman, R. G.; Gaitley, B. J.; Tan, Q.; Diehl, T. L.

    2011-01-01

    The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops handheld sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.

  6. Future aerosol emissions: a multi-model comparison

    SciTech Connect

    Smith, Steven J.; Rao, Shilpa; Riahi, Keywan; van Vuuren, Detlef P.; Calvin, Katherine V.; Kyle, Page

    2016-08-02

    This paper compares projections over the 21st century of SO2, BC, and OC emissions from three technologically detailed, long-term integrated assessment models. The character of the projections and the response of emissions due to a comprehensive climate policy are discussed. In a continuation of historical experience, aerosol and precursor emissions are increasingly decoupled from carbon dioxide emissions over the 21st century. Implementation of a comprehensive climate policy further reduces emissions, although there is significant variation in this response by sector and by model. Differences in model responses can be traced to specific characteristics of reference case end-use and supply-side technology deployment and emissions control assumptions, which are detailed by sector.

  7. Complex Coupling of Air Quality and Climate-Relevant Aerosols in a Chemistry-Aerosol Microphysics Model

    NASA Astrophysics Data System (ADS)

    Yoshioka, M.; Carslaw, K. S.; Reddington, C.; Mann, G.

    2013-12-01

    Controlling emissions of aerosols and their precursors to improve air quality will impact the climate through direct and indirect radiative forcing. We have investigated the impacts of changes in a range of aerosol and gas-phase emission fluxes and changes in temperature on air quality and climate change metrics using a global aerosol microphysics and chemistry model, GLOMAP. We investigate how the responses of PM2.5 and cloud condensation nuclei (CCN) are coupled, and how attempts to improve air quality could have inadvertent effects on CCN, clouds and climate. The parameter perturbations considered are a 5°C increase in global temperature, increased or decreased precursor emissions of anthropogenic SO2, NH3, and NOx, and biogenic monoterpenes, and increased or decreased primary emissions of organic and black carbon aerosols from wildfire, fossil fuel, and biofuel. To quantify the interactions, we define a new sensitivity metric in terms of the response of CCN divided by the response of PM in different regions. .Our results show that the coupled chemistry and aerosol processes cause complex responses that will make any co-benefit policy decision problematic. In particular, we show that reducing SO2 emissions effectively reduces surface-level PM2.5 over continental regions in summer when background PM2.5 is high, with a relatively small reduction in marine CCN (and hence indirect radiative cooling over ocean), which is beneficial for near-term climate. Reducing NOx emissions does not improve summertime air quality very effectively but leads to a relatively high reduction of marine CCN. Reducing NH3 emissions has moderate effects on both PM2.5 and CCN. These three species are strongly coupled chemically and microphysically and the effects of changing emissions of one species on mass and size distributions of aerosols are very complex and spatially and temporally variable. For example, reducing SO2 emissions leads to reductions in sulphate and ammonium mass

  8. A Pure Marine Aerosol Model, for Use in Remote Sensing Applications

    NASA Technical Reports Server (NTRS)

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

    2011-01-01

    Retrievals of aerosol optical depth (AOD) and related parameters from satellite measurements typically involve prescribed models of aerosol size and composition, and are therefore dependent on how well these models are able to represent the radiative behaviour of real aerosols, This study uses aerosol volume size distributions retrieved from Sun-photometer measurements at 11 Aerosol Robotic Network (AERONET) island sites, spread throughout the world's oceans, as a basis to define such a model for unpolluted maritime aerosols. Size distributions are observed to be bimodal and approximately lognormal, although the coarse mode is skewed with a long tail on the low-radius end, The relationship of AOD and size distribution parameters to meteorological conditions is also examined, As wind speed increases, so do coarse-mode volume and radius, The AOD and Angstrom exponent (alpha) show linear relationships with wind speed, although there is considerable scatter in all these relationships, limiting their predictive power. Links between aerosol properties and near-surface relative humidity, columnar water vapor, and sea surface temperature are also explored. A recommended bimodal maritime model, which is able to reconstruct the AERONET AOD with accuracy of order 0.01-0.02, is presented for use in aerosol remote sensing applications. This accuracy holds at most sites and for wavelengths between 340 nm and 1020 nm. Calculated lidar ratios are also provided, and differ significantly from those currently used in Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) processing.

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  10. Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

    NASA Astrophysics Data System (ADS)

    Roldin, P.; Eriksson, A. C.; Nordin, E. Z.; Hermansson, E.; Mogensen, D.; Rusanen, A.; Boy, M.; Swietlicki, E.; Svenningsson, B.; Zelenyuk, A.; Pagels, J.

    2014-08-01

    We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost particle-size-independent evaporation of α-pinene ozonolysis secondary organic aerosol (SOA) particles, (3) the mass-transfer-limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), and (4) the influence of chamber wall effects on the observed SOA formation in smog chambers. ADCHAM is able to capture the observed α-pinene SOA mass increase in the presence of NH3(g). Organic salts of ammonium and carboxylic acids predominantly form during the early stage of SOA formation. In the smog chamber experiments, these salts contribute substantially to the initial growth of the homogeneously nucleated particles. The model simulations of evaporating α-pinene SOA particles support the recent experimental findings that these particles have a semi-solid tar-like amorphous-phase state. ADCHAM is able to reproduce the main features of the observed slow evaporation rates if the concentration of low-volatility and viscous oligomerized SOA material at the particle surface increases upon evaporation. The evaporation rate is mainly governed by the reversible decomposition of oligomers back to monomers. Finally, we demonstrate that the mass-transfer-limited uptake of condensable organic compounds

  11. Impacts of increasing the aerosol complexity in the Met Office global NWP model

    NASA Astrophysics Data System (ADS)

    Mulcahy, Jane; Walters, David; Bellouin, Nicolas; Milton, Sean

    2014-05-01

    Inclusion of the direct and indirect radiative effects of aerosols in high resolution global numerical weather prediction (NWP) models is being increasingly recognised as important for the improved accuracy of short-range weather forecasts. In this study the impacts of increasing the aerosol complexity in the global NWP configuration of the Met Office Unified Model (MetUM) are investigated. A hierarchy of aerosol representations are evaluated including three dimensional monthly mean speciated aerosol climatologies, fully prognostic aerosols modelled using the CLASSIC aerosol scheme and finally, initialised aerosols using assimilated aerosol fields from the GEMS project. The prognostic aerosol schemes are better able to predict the temporal and spatial variation of atmospheric aerosol optical depth, which is particularly important in cases of large sporadic aerosol events such as large dust storms or forest fires. Including the direct effect of aerosols improves model biases in outgoing longwave radiation over West Africa due to a better representation of dust. Inclusion of the indirect aerosol effects has significant impacts on the SW radiation particularly at high latitudes due to lower cloud amounts in high latitude clean air regions. This leads to improved surface radiation biases at the North Slope of Alaska ARM site. Verification of temperature and height forecasts is also improved in this region. Impacts on the global mean model precipitation and large-scale circulation fields were found to be generally small in the short range forecasts. However, the indirect aerosol effect leads to a strengthening of the low level monsoon flow over the Arabian Sea and Bay of Bengal and an increase in precipitation over Southeast Asia. This study highlights the importance of including a more realistic treatment of aerosol-cloud interactions in global NWP models and the potential for improved global environmental prediction systems through the incorporation of more complex

  12. Representation and evaluation of aerosol mixing state in a climate model

    NASA Astrophysics Data System (ADS)

    Bauer, S. E.; Prather, K. A.; Ault, A. P.

    2011-12-01

    Aerosol particles in the atmosphere are composed out of multiple chemical species. The aerosol mixing state is an important aerosol property that will determine the interaction of aerosols with the climate system via radiative forcings and cloud activation. Through the introduction of aerosol microphysics into climate models, aerosol mixing state is by now taken into account to a certain extend in climate models, and evaluation of mixing state is the next challenge. Here we use data from the Aerosol Time of Flight Mass Spectrometer (ATOFMS) and compare the results to the GISS-modelE-MATRIX model, a global climate model including a detailed aerosol micro-physical scheme. We use data from various field campaigns probing, urban, rural and maritime air masses and compare those to climatological and nudged simulations for the years 2005 to 2009. ATOFMS provides information about the size distributions of several mixing state classes, including the chemical components of black and organic carbon, sulfates, dust and salts. MATRIX simulates 16 aerosol populations, which definitions are based on mixing state. We have grouped ATOFMS and MATRIX data into similar mixing state classes and compare the size resolved number concentrations against each other. As a first result we find that climatological simulations are rather difficult to evaluate with field data, and that nudged simulations give a much better agreement. However this is not just caused by the better fit of natural - meteorological driven - aerosol components, but also due to the interaction between meteorology and aerosol formation. The model seems to get the right amount of mixing state of black carbon material with sulfate and organic components, but seems to always overestimate the fraction of black carbon that is externally mixed. In order to understand this bias between model and the ATOFMS data, we will look into microphysical processes near emission sources and investigate the climate relevance of these sub

  13. Analysis of Measurement Requirements for the Aerosol Indirect Effect: A Synthesis of Observations and Modeling

    NASA Astrophysics Data System (ADS)

    Feingold, G.; Previdi, M.; Veron, D. E.

    2003-12-01

    The aerosol indirect effect has been measured for some time now by satellite remote sensors, and more recently by surface-based remote sensors. The indirect effect is often expressed in terms of a relative change in drop size for a relative change in aerosol optical depth or extinction. Here we present some recent results of surface based remote sensing of the indirect effect and assess whether aerosol optical depth or extinction is a suitable proxy for the aerosol affecting drop formation. To do so, we use multiple realizations of a cloud model to investigate the sensitivity of cloud drop effective radius re to aerosol parameters (size distribution and composition) and dynamical parameters (updraft and liquid water content). A breakdown of the individual aerosol terms contributing to drop size change shows that use of aerosol extinction as a proxy for size distribution and composition tends to underestimate the magnitude of the first indirect effect. The use of the aerosol index alleviates this problem somewhat. We show that re is most sensitive to cloud liquid water, a parameter often ignored in indirect effect analyses. The relative importance of the other parameters varies for different conditions but aerosol concentration Na is consistently important. Updraft plays an increasingly important role under high aerosol loadings. Requirements for measuring the indirect effect over polluted continents are shown to be more stringent than those over cleaner, remote oceans. This may influence interpretation of current satellite and surface remote measurements of the indirect effect.

  14. AeroCom INSITU Project: Comparison of Aerosol Optical Properties from In-situ Surface Measurements and Model Simulations

    NASA Astrophysics Data System (ADS)

    Schmeisser, L.; Andrews, E.; Schulz, M.; Fiebig, M.; Zhang, K.; Randles, C. A.; Myhre, G.; Chin, M.; Stier, P.; Takemura, T.; Krol, M. C.; Bian, H.; Skeie, R. B.; da Silva, A. M., Jr.; Kokkola, H.; Laakso, A.; Ghan, S.; Easter, R. C.

    2015-12-01

    AeroCom, an open international collaboration of scientists seeking to improve global aerosol models, recently initiated a project comparing model output to in-situ, surface-based measurements of aerosol optical properties. The model/measurement comparison project, called INSITU, aims to evaluate the performance of a suite of AeroCom aerosol models with site-specific observational data in order to inform iterative improvements to model aerosol modules. Surface in-situ data have the unique property of being traceable to physical standards, which is a big asset in accomplishing the overarching goal of bettering the accuracy of aerosol processes and predicative capability of global climate models. The INSITU project looks at how well models reproduce aerosol climatologies on a variety of time scales, aerosol characteristics and behaviors (e.g., aerosol persistence and the systematic relationships between aerosol optical properties), and aerosol trends. Though INSITU is a multi-year endeavor, preliminary phases of the analysis, using GOCART and other models participating in this AeroCom project, show substantial model biases in absorption and scattering coefficients compared to surface measurements, though the sign and magnitude of the bias varies with location and optical property. Spatial patterns in the biases highlight model weaknesses, e.g., the inability of models to properly simulate aerosol characteristics at sites with complex topography (see Figure 1). Additionally, differences in modeled and measured systematic variability of aerosol optical properties suggest that some models are not accurately capturing specific aerosol co-dependencies, for example, the tendency of in-situ surface single scattering albedo to decrease with decreasing aerosol extinction coefficient. This study elucidates specific problems with current aerosol models and suggests additional model runs and perturbations that could further evaluate the discrepancies between measured and modeled

  15. Toward a Minimal Representation of Aerosols in Climate Models: Comparative Decomposition of Aerosol Direct, Semidirect, and Indirect Radiative Forcing

    SciTech Connect

    Ghan, Steven J.; Liu, Xiaohong; Easter, Richard C.; Zaveri, Rahul A.; Rasch, Philip J.; Yoon, Jin-Ho; Eaton, Brian

    2012-10-01

    The authors have decomposed the anthropogenic aerosol radiative forcing into direct contributions from each aerosol species to the planetary energy balance through absorption and scattering of solar radiation, indirect effects of anthropogenic aerosol on solar and infrared radiation through droplet and crystal nucleation on aerosol, and semidirect effects through the influence of solar absorption on the distribution of clouds. A three-mode representation of the aerosol in version 5.1 of the Community Atmosphere Model (CAM5.1) yields global annual mean radiative forcing estimates for each of these forcing mechanisms that are within 0.1 W m–2 of estimates using a more complex seven-mode representation that distinguishes between fresh and aged black carbon and primary organic matter. Simulating fresh black carbon particles separately from internally mixed accumulation mode particles is found to be important only near fossil fuel sources. In addition to the usual large indirect effect on solar radiation, this study finds an unexpectedly large positive longwave indirect effect (because of enhanced cirrus produced by homogenous nucleation of ice crystals on anthropogenic sulfate), small shortwave and longwave semidirect effects, and a small direct effect (because of cancelation and interactions of direct effects of black carbon and sulfate). Differences between the threemode and seven-mode versions are significantly larger (up to 0.2 W m–2) when the hygroscopicity of primary organic matter is decreased from 0.1 to 0 and transfer of the primary carbonaceous aerosol to the accumulation mode in the seven-mode version requires more hygroscopic material coating the primary particles. Radiative forcing by cloudborne anthropogenic black carbon is only 20.07 W m–2.

  16. 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

  17. Modeling aerosol water uptake in the arctic based on the κ-Kohler theory

    NASA Astrophysics Data System (ADS)

    Rastak, N.; Ekman, A.; Silvergren, S.; Zieger, P.; Wideqvist, U.; Ström, J.; Svenningsson, B.; Tunved, P.; Riipinen, I.

    2013-05-01

    Water uptake or hygroscopicity is one of the most fundamental properties of atmospheric aerosols. Aerosol particles containing soluble materials can grow in size by absorbing water in ambient atmosphere. This property is measured by a parameter known as growth factor (GF), which is defined as the ratio of the wet diameter to the dry diameter. Hygroscopicity controls the size of an aerosol particle and therefore its optical properties in the atmosphere. Hygroscopic growth depends on the dry size of the particle, its chemical composition and the relative humidity in the ambient air (Fitzgerald, 1975; Pilinis et al., 1995). One of the typical problems in aerosol studies is the lack of measurements of aerosol size distributions and optical properties in ambient conditions. The gap between dry measurements and the real humid atmosphere is filled in this study by utilizing a hygroscopic model which calculates the hygroscopic growth of aerosol particles at Mt Zeppelin station, Ny Ålesund, Svalbard during 2008.

  18. Phase transformation and growth of hygroscopic aerosols

    SciTech Connect

    Tang, I.N.

    1995-09-01

    Ambient aerosols frequently contain large portions of hygroscopic inorganic salts such as chlorides, nitrates, and sulfates in either pure or mixed forms. Such inorganic salt aerosols exhibit the properties of deliquescence and efflorescence in air. The phase transformation from a solid particle to a saline droplet usually occurs spontaneously when the relative humidity of the atmosphere reaches a level specific to the chemical composition of the aerosol particle. Conversely, when the relative humidity decreases and becomes low enough, the saline droplet will evaporate and suddenly crystallize, expelling all its water content. The phase transformation and growth of aerosols play an important role in many atmospheric processes affecting air quality, visibility degradation, and climate changes. In this chapter, an exposition of the underlying thermodynamic principles is given, and recent advances in experimental methods utilizing single-particle levitation are discussed. In addition, pertinent and available thermodynamic data, which are needed for predicting the deliquescence properties of single and multi-component aerosols, are compiled. This chapter is useful to research scientists who are either interested in pursuing further studies of aerosol thermodynamics, or required to model the dynamic behavior of hygroscopic aerosols in a humid environment.

  19. Estimation of biomass burning influence on air pollution around Beijing from an aerosol retrieval model.

    PubMed

    Mukai, Sonoyo; Yasumoto, Masayoshi; Nakata, Makiko

    2014-01-01

    We investigate heavy haze episodes (with dense concentrations of atmospheric aerosols) occurring around Beijing in June, when serious air pollution was detected by both satellite and ground measurements. Aerosol retrieval is achieved by radiative transfer simulation in an Earth atmosphere model. We solve the radiative transfer problem in the case of haze episodes by successive order of scattering. We conclude that air pollution around Beijing in June is mainly due to increased emissions of anthropogenic aerosols and that carbonaceous aerosols from agriculture biomass burning in Southeast Asia also contribute to pollution.

  20. Inorganic bromine in the marine boundary layer: a critical review

    NASA Astrophysics Data System (ADS)

    Sander, R.; Keene, W. C.; Pszenny, A. A. P.; Arimoto, R.; Ayers, G. P.; Baboukas, E.; Cainey, J. M.; Crutzen, P. J.; Duce, R. A.; Hönninger, G.; Huebert, B. J.; Maenhaut, W.; Mihalopoulos, N.; Turekian, V. C.; van Dingenen, R.

    2003-06-01

    The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is depleted in bromine by about 50% relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that these depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. However, currently available techniques cannot reliably quantify many \\chem{Br}-containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans, excluding the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br-containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize

  1. Assessing the effects of anthropogenic aerosols on Pacific storm track using a multiscale global climate model.

    PubMed

    Wang, Yuan; Wang, Minghuai; Zhang, Renyi; Ghan, Steven J; Lin, Yun; Hu, Jiaxi; Pan, Bowen; Levy, Misti; Jiang, Jonathan H; Molina, Mario J

    2014-05-13

    Atmospheric aerosols affect weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the effects of anthropogenic aerosols on the Pacific storm track, using a multiscale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and preindustrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and longwave cloud radiative forcing at the top of atmosphere are changed by -2.5 and +1.3 W m(-2), respectively, by emission changes from preindustrial to present day, and an increased cloud top height indicates invigorated midlatitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides, for the first time to the authors' knowledge, a global perspective of the effects of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multiscale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on a global scale.

  2. Assessing the Effects of Anthropogenic Aerosols on Pacific Storm Track Using a Multiscale Global Climate Model

    SciTech Connect

    Wang, Yuan; Wang, Minghuai; Zhang, Renyi; Ghan, Steven J.; Lin, Yun; Hu, Jiaxi; Pan, Bowen; Levy, Misti; Jiang, Jonathan; Molina, Mario J.

    2014-05-13

    Atmospheric aerosols impact weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the impacts of anthropogenic aerosols on the Pacific storm track using a multi-scale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and pre-industrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and longwave cloud radiative forcing at the top of atmosphere are changed by - 2.5 and + 1.3 W m-2, respectively, by emission changes from pre-industrial to present day, and an increased cloud-top height indicates invigorated mid-latitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides for the first time a global perspective of the impacts of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multi-scale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on the global scale.

  3. Assessment of aloft aerosol layers by ground-based lidar, satellite CALIPSO and model

    NASA Astrophysics Data System (ADS)

    Wu, Y.; Cordero, L.; Nazmi, C.; Gross, B.; Moshary, F.; Ahmed, S. A.

    2013-12-01

    Aloft aerosol layers injected from dust storms and biomass burning are often transported over the long-distance, thus playing important roles in climate radiative forcing and air quality in the regional and continental scale. In particular, they are critical to satellite remote sensing of air quality, e.g. using satellite column aerosol optical depth (AOD) to evaluate surface PM2.5 concentration, because the aloft aerosol layer can make a substantial contribution to total AOD. These aloft aerosol plumes have been extensively observed or identified by the ground-lidar and space-borne lidar CALIOP/CALIPSO, as well as the global aerosol transport such as NRL-NAAPS. In this study, the aloft aerosol layers are investigated with a regional NOAA-CREST Lidar Network (CLN) in the East Coast of U.S., spaceborne lidar CAIPSO observations and NAAPS model forecast. We first analyze the height distribution and seasonal occurrence of aloft aerosol plumes from the multi-year CLN-lidar dataset. We also explore specific aloft aerosol layers and type classifications between NAAPS-model and CLN-lidar observations to asses NAAPS with special attention to time slices when MODIS AOD assimilation is present or not. Moreover, we assess the potential of NAAPS to identify and separate between aloft aerosol layers ('unclear' sky) and the non-aloft-layer ('clear' sky). This identification is very important in filtering the use of satellite AOD retrievals in potential PM2.5 estimators.

  4. Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

    NASA Astrophysics Data System (ADS)

    Alvarado, Matthew J.; Lonsdale, Chantelle R.; Macintyre, Helen L.; Bian, Huisheng; Chin, Mian; Ridley, David A.; Heald, Colette L.; Thornhill, Kenneth L.; Anderson, Bruce E.; Cubison, Michael J.; Jimenez, Jose L.; Kondo, Yutaka; Sahu, Lokesh K.; Dibb, Jack E.; Wang, Chien

    2016-07-01

    Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction

  5. Implementation of the Missing Aerosol Physics into LLNL IMPACT

    SciTech Connect

    Chuang, C

    2005-02-09

    characteristics and composition of aerosols. These processes, together with other physical properties (i.e., size, density, and refractive index), determine the atmospheric lifetime of aerosols and their radiative forcing. To better represent physical properties of aerosols, we adapted an aerosol microphysics model that simulates aerosol size distribution. Work toward this goal was done in collaboration with Professor Anthony Wexler of University of California at Davis. Professor Wexler's group has developed sectional models of atmospheric aerosol dynamics that include an arbitrary number of size sections and chemical compounds or compound classes. The model, AIM (Aerosol Inorganic Model), is designed to predict the mass distribution and composition of urban and regional particulate matter (''Sun and Wexler'', 1998a, b). This model is currently incorporated into EPA's Models-3 air quality modeling platform/CMAQ (Community Multiscale Air Quality) to test its performance with previous simulations of CMAQ over the continental US.

  6. Modeling of microphysics and optics of aerosol particles in the marine environments

    NASA Astrophysics Data System (ADS)

    Kaloshin, Gennady

    2013-05-01

    We present a microphysical model for the surface layer marine and coastal atmospheric aerosols that is based on long-term observations of size distributions for 0.01-100 μm particles. The fundamental feature of the model is a parameterization of amplitudes and widths for aerosol modes of the aerosol size distribution function (ASDF) as functions of fetch and wind speed. The shape of ASDF and its dependence on meteorological parameters, height above sea level (H), fetch (X), wind speed (U) and relative humidity (RH), are investigated. At present, the model covers the ranges H = 0 - 25 m, U = 3 - 18 km s-1, X ≤ 120 km and RH = 40 - 98%. The latest version of the Marine Aerosol Extinction Profiles model (MaexPro) is described and applied for the computation and analysis of the spectral profiles of aerosol extinction coefficients α(λ) in the wavelength band λ = 0.2-12 μm. MaexPro is based on the aforementioned aerosol model assuming spherically shaped aerosol particles and the well-known Mie theory. The spectral profiles of α(λ) calculated by MaexPro are in good agreement with observational data and the numerical results. Moreover, MaexPro was found to be an accurate and reliable tool for investigating the optical properties of atmospheric aerosols.

  7. Cloud/Aerosol Parameterizations: Application and Improvement of General Circulation Models

    SciTech Connect

    Penner, Joyce

    2012-06-30

    One of the biggest uncertainties associated with climate models and climate forcing is the treatment of aerosols and their effects on clouds. The effect of aerosols on clouds can be divided into two components: The first indirect effect is the forcing associated with increases in droplet concentrations; the second indirect effect is the forcing associated with changes in liquid water path, cloud morphology, and cloud lifetime. Both are highly uncertain. This project applied a cloud-resolving model to understand the response of clouds under a variety of conditions to changes in aerosols. These responses are categorized according to the large-scale meteorological conditions that lead to the response. Meteorological conditions were sampled from various fields, which, together with a global aerosol model determination of the change in aerosols from present day to pre-industrial conditions, was used to determine a first order estimate of the response of global cloud fields to changes in aerosols. The response of the clouds in the NCAR CAM3 GCM coupled to our global aerosol model were tested by examining whether the response is similar to that of the cloud resolving model and methods for improving the representation of clouds and cloud/aerosol interactions were examined.

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

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

    Modelling aerosol optical properties is a notoriously difficult task due to the particles' complex morphologies and compositions. Yet aerosols and their optical properties are important for Earth system modelling and remote sensing applications. Operational optics models often make drastic and non realistic approximations regarding morphological properties, which can introduce errors. In this study a new aerosol optics model is implemented, in which more realistic morphologies and mixing states are assumed, especially for black carbon aerosols. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey shell" model. Simulated results of radiative fluxes, backscattering coefficients and the Ångström exponent from the new optics model are compared with results from another model simulating particles as externally mixed homogeneous spheres. To gauge the impact on the optical properties from the new optics model, the known and important effects from using aerosol dynamics serves as a reference. The results show that using a more detailed description of particle morphology and mixing states influences the optical properties to the same degree as aerosol dynamics. This is an important finding suggesting that over-simplified optics models coupled to a chemical transport model can introduce considerable errors; this can strongly effect simulations of radiative fluxes in Earth-system models, and it can compromise the use of remote sensing observations of aerosols in model evaluations and chemical data assimilation.

  9. Program Models A Laser Beam Focused In An Aerosol Spray

    NASA Technical Reports Server (NTRS)

    Barton, J. P.

    1996-01-01

    Monte Carlo analysis performed on packets of light. Program for Analysis of Laser Beam Focused Within Aerosol Spray (FLSPRY) developed for theoretical analysis of propagation of laser pulse optically focused within aerosol spray. Applied for example, to analyze laser ignition arrangement in which focused laser pulse used to ignite liquid aerosol fuel spray. Scattering and absorption of laser light by individual aerosol droplets evaluated by use of electromagnetic Lorenz-Mie theory. Written in FORTRAN 77 for both UNIX-based computers and DEC VAX-series computers. VAX version of program (LEW-16051). UNIX version (LEW-16065).

  10. A Global Aerosol Model Forecast for the ACE-Asia Field Experiment

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Ginoux, Paul; Lucchesi, Robert; Huebert, Barry; Weber, Rodney; Anderson, Tad; Masonis, Sarah; Blomquist, Byron; Bandy, Alan; Thornton, Donald

    2003-01-01

    We present the results of aerosol forecast during the Aerosol Characterization Experiment (ACE-Asia) field experiment in spring 2001, using the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model and the meteorological forecast fields from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). The aerosol model forecast provides direct information on aerosol optical thickness and concentrations, enabling effective flight planning, while feedbacks from measurements constantly evaluate the model, making successful model improvements. We verify the model forecast skill by comparing model predicted total aerosol extinction, dust, sulfate, and SO2 concentrations with those quantities measured by the C-130 aircraft during the ACE-Asia intensive operation period. The GEOS DAS meteorological forecast system shows excellent skills in predicting winds, relative humidity, and temperature for the ACE-Asia experiment area as well as for each individual flight, with skill scores usually above 0.7. The model is also skillful in forecast of pollution aerosols, with most scores above 0.5. The model correctly predicted the dust outbreak events and their trans-Pacific transport, but it constantly missed the high dust concentrations observed in the boundary layer. We attribute this missing dust source to the desertification regions in the Inner Mongolia Province in China, which have developed in recent years but were not included in the model during forecasting. After incorporating the desertification sources, the model is able to reproduce the observed high dust concentrations at low altitudes over the Yellow Sea. Two key elements for a successful aerosol model forecast are correct source locations that determine where the emissions take place, and realistic forecast winds and convection that determine where the aerosols are transported. We demonstrate that our global model can not only account for the large

  11. 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.

  12. Characterization and calibration of a viscoelastic simplified potential energy clock model for inorganic glasses

    SciTech Connect

    Chambers, Robert S.; Tandon, Rajan; Stavig, Mark E.

    2015-07-07

    In this study, to analyze the stresses and strains generated during the solidification of glass-forming materials, stress and volume relaxation must be predicted accurately. Although the modeling attributes required to depict physical aging in organic glassy thermosets strongly resemble the structural relaxation in inorganic glasses, the historical modeling approaches have been distinctly different. To determine whether a common constitutive framework can be applied to both classes of materials, the nonlinear viscoelastic simplified potential energy clock (SPEC) model, developed originally for glassy thermosets, was calibrated for the Schott 8061 inorganic glass and used to analyze a number of tests. A practical methodology for material characterization and model calibration is discussed, and the structural relaxation mechanism is interpreted in the context of SPEC model constitutive equations. SPEC predictions compared to inorganic glass data collected from thermal strain measurements and creep tests demonstrate the ability to achieve engineering accuracy and make the SPEC model feasible for engineering applications involving a much broader class of glassy materials.

  13. Characterization and calibration of a viscoelastic simplified potential energy clock model for inorganic glasses

    DOE PAGES

    Chambers, Robert S.; Tandon, Rajan; Stavig, Mark E.

    2015-07-07

    In this study, to analyze the stresses and strains generated during the solidification of glass-forming materials, stress and volume relaxation must be predicted accurately. Although the modeling attributes required to depict physical aging in organic glassy thermosets strongly resemble the structural relaxation in inorganic glasses, the historical modeling approaches have been distinctly different. To determine whether a common constitutive framework can be applied to both classes of materials, the nonlinear viscoelastic simplified potential energy clock (SPEC) model, developed originally for glassy thermosets, was calibrated for the Schott 8061 inorganic glass and used to analyze a number of tests. A practicalmore » methodology for material characterization and model calibration is discussed, and the structural relaxation mechanism is interpreted in the context of SPEC model constitutive equations. SPEC predictions compared to inorganic glass data collected from thermal strain measurements and creep tests demonstrate the ability to achieve engineering accuracy and make the SPEC model feasible for engineering applications involving a much broader class of glassy materials.« less

  14. Impact of Asian Aerosols on Precipitation Over California: An Observational and Model Based Approach

    NASA Technical Reports Server (NTRS)

    Naeger, Aaron R.; Molthan, Andrew L.; Zavodsky, Bradley T.; Creamean, Jessie M.

    2015-01-01

    Dust and pollution emissions from Asia are often transported across the Pacific Ocean to over the western United States. Therefore, it is essential to fully understand the impact of these aerosols on clouds and precipitation forming over the eastern Pacific and western United States, especially during atmospheric river events that account for up to half of California's annual precipitation and can lead to widespread flooding. In order for numerical modeling simulations to accurately represent the present and future regional climate of the western United States, we must account for the aerosol-cloud-precipitation interactions associated with Asian dust and pollution aerosols. Therefore, we have constructed a detailed study utilizing multi-sensor satellite observations, NOAA-led field campaign measurements, and targeted numerical modeling studies where Asian aerosols interacted with cloud and precipitation processes over the western United States. In particular, we utilize aerosol optical depth retrievals from the NASA Moderate Resolution Imaging Spectroradiometer (MODIS), NOAA Geostationary Operational Environmental Satellite (GOES-11), and Japan Meteorological Agency (JMA) Multi-functional Transport Satellite (MTSAT) to effectively detect and monitor the trans-Pacific transport of Asian dust and pollution. The aerosol optical depth (AOD) retrievals are used in assimilating the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) in order to provide the model with an accurate representation of the aerosol spatial distribution across the Pacific. We conduct WRF-Chem model simulations of several cold-season atmospheric river events that interacted with Asian aerosols and brought significant precipitation over California during February-March 2011 when the NOAA CalWater field campaign was ongoing. The CalWater field campaign consisted of aircraft and surface measurements of aerosol and precipitation processes that help extensively validate our WRF

  15. Intercomparison of Models Representing Direct Shortwave Radiative Forcing by Sulfate Aerosols

    NASA Technical Reports Server (NTRS)

    Boucher, O.; Schwartz, S. E.; Ackerman, T. P.; Anderson, T. L.; Bergstrom, B.; Bonnel, B.; Dahlback, A.; Fouquart, Y.; Chylek, P.; Fu, Q.; Halthore, R. N.; Haywood, J. M.; Iversen, T.; Kato, S.; Kinne, S.; Kirkevag, A.; Knapp, K. R.; Lacis, A.; Laszlo, I.; Mishchenko, M. I.

    2000-01-01

    The importance of aerosols as agents of climate change has recently been highlighted. However, the magnitude of aerosol forcing by scattering of shortwave radiation (direct forcing) is still very uncertain even for the relatively well characterized sulfate aerosol. A potential source of uncertainty is in the model representation of aerosol optical properties and aerosol influences on radiative transfer in the atmosphere. Although radiative transfer methods and codes have been compared in the past, these comparisons have not focused on aerosol forcing (change in net radiative flux at the top of the atmosphere). Here we report results of a project involving 12 groups using 15 models to examine radiative forcing by sulfate aerosol for a wide range of values of particle radius, aerosol optical depth, surface albedo, and solar zenith angle. Among the models that were employed were high and low spectral resolution models incorporating a variety of radiative transfer approximations as well as a line-by-line model. The normalized forcings (forcing per sulfate column burden) obtained with the several radiative transfer models were examined, and the discrepancies were characterized. All models simulate forcings of comparable amplitude and exhibit a similar dependence on input parameters. As expected for a non-light-absorbing aerosol, forcings were negative (cooling influence) except at high surface albedo combined with small solar zenith angle. The relative standard deviation of the zenith-angle-averaged normalized broadband forcing for 15 models-was 8% for particle radius near the maximum in this forcing (approx. 0.2 microns) and at low surface albedo. Somewhat greater model-to-model discrepancies were exhibited at specific solar zenith angles. Still greater discrepancies were exhibited at small particle radii and much greater discrepancies were exhibited at high surface albedos, at which the forcing changes sign; in these situations, however, the normalized forcing is

  16. The application of mechanical aerosol delivery systems in an in vitro model of mechanically ventilated neonates.

    PubMed

    Ehtezazi, Touraj; Turner, Mark A

    2013-12-01

    Delivery of medication to the neonatal lung using current methods is inefficient. Aerosols offer one way to improve delivery to small airways. In this in vitro work, aerosol delivery by using a micropump or a rotary valve has been evaluated in a model of the neonatal setting with a pressurised metered dose inhaler plus spacer outside of the inspiratory limb. Drug depositions were assessed by spectrophotometric analyses. Drug lung deposition was increased by adjusting the rotary valve for co-ordination between the inhalation and aerosol delivery, but this intermittent mode decreased the aerosol delivery by using the micropump. Also, decreasing the volume of spacer decreased drug deposition in test lungs by using the micropump system. At the optimum conditions, the rotary valve aerosol delivery system delivered 3.68±0.91% of the Qvar nominal dose to the test lungs, and this was 2.34±0.01% for the micropump system. In conclusion, the rotary valve aerosol delivery system provided higher amounts of drug particles to the test lungs compared to the micropump system. The advantages of these methods were that the humidity in the ventilation circuit did not affect the aerosol particles in the spacer. Further optimisation is required to improve aerosol deposition in the test lungs. The article has also a short section of recent patents relevant to aerosol delivery.

  17. Comparison of abundances, compositions and sources of elements, inorganic ions and organic compounds in atmospheric aerosols from Xi'an and New Delhi, two megacities in China and India.

    PubMed

    Li, Jianjun; Wang, Gehui; Aggarwal, Shankar G; Huang, Yao; Ren, Yanqin; Zhou, Bianhong; Singh, Khem; Gupta, Prabhat K; Cao, Junji; Zhang, Rong

    2014-04-01

    Wintertime TSP samples collected in the two megacities of Xi'an, China and New Delhi, India were analyzed for elements, inorganic ions, carbonaceous species and organic compounds to investigate the differences in chemical compositions and sources of organic aerosols. The current work is the first time comparing the composition of urban organic aerosols from China and India and discussing their sources in a single study. Our results showed that the concentrations of Ca, Fe, Ti, inorganic ions, EC, PAHs and hopanes in Xi'an are 1.3-2.9 times of those in New Delhi, which is ascribed to the higher emissions of dust and coal burning in Xi'an. In contrast, Cl(-), levoglucosan, n-alkanes, fatty alcohols, fatty acids, phthalates and bisphenol A are 0.4-3.0 times higher in New Delhi than in Xi'an, which is attributed to strong emissions from biomass burning and solid waste incineration. PAHs are carcinogenic while phthalates and bisphenol A are endocrine disrupting. Thus, the significant difference in chemical compositions of the above TSP samples may suggest that residents in Xi'an and New Delhi are exposed to environmental hazards that pose different health risks. Lower mass ratios of octadecenoic acid/octadecanoic acid (C18:1/C18:0) and benzo(a)pyrene/benzo(e)pyrene (BaP/BeP) demonstrate that aerosol particles in New Delhi are photochemically more aged. Mass closure reconstructions of the wintertime TSP indicate that crustal material is the most abundant component of ambient particles in Xi'an and New Delhi, accounting for 52% and 48% of the particle masses, respectively, followed by organic matter (24% and 23% in Xi'an and New Delhi, respectively) and secondary inorganic ions (sulfate, nitrate plus ammonium, 16% and 12% in Xi'an and New Delhi, respectively).

  18. Assessing conceptual models for subsurface reactive transport of inorganic contaminants

    USGS Publications Warehouse

    Davis, James A.; Yabusaki, Steven B.; Steefel, Carl; Zachara, John M.; Curtis, Gary P.; Redden, George D.; Criscenti, Louise J.; Honeyman, Bruce D.

    2004-01-01

    In many subsurface situations where human health and environmental quality are at risk (e.g., contaminant hydrogeology petroleum extraction, carbon sequestration, etc.),scientists and engineers are being asked by federal agency decision-makers to predict the fate of chemical species under conditions where both reactions and transport are processes of first-order importance.In 2002, a working group (WG) was formed by representatives of the U.S. Geological Survey, Environmental Protection Agency, Department of Energy Nuclear Regulatory Commission, Department of Agriculture, and Army Engineer Research and Development Center to assess the role of reactive transport modeling (RTM) in addressing these situations. Specifically the goals of the WG are to (1) evaluate the state of the art in conceptual model development and parameterization for RTM, as applied to soil,vadose zone, and groundwater systems, and (2) prioritize research directions that would enhance the practical utility of RTM.

  19. Evaluation of Black Carbon Estimations in Global Aerosol Models

    SciTech Connect

    Koch, D.; Schulz, M.; Kinne, Stefan; McNaughton, C. S.; Spackman, J. R.; Balkanski, Y.; Bauer, S.; Berntsen, T.; Bond, Tami C.; Boucher, Olivier; Chin, M.; Clarke, A. D.; De Luca, N.; Dentener, F.; Diehl, T.; Dubovik, O.; Easter, Richard C.; Fahey, D. W.; Feichter, J.; Fillmore, D.; Freitag, S.; Ghan, Steven J.; Ginoux, P.; Gong, S.; Horowitz, L.; Iversen, T.; Kirkevag, A.; Klimont, Z.; Kondo, Yutaka; Krol, M.; Liu, Xiaohong; Miller, R.; Montanaro, V.; Moteki, N.; Myhre, G.; Penner, J.; Perlwitz, Ja; Pitari, G.; Reddy, S.; Sahu, L.; Sakamoto, H.; Schuster, G.; Schwarz, J. P.; Seland, O.; Stier, P.; Takegawa, Nobuyuki; Takemura, T.; Textor, C.; van Aardenne, John; Zhao, Y.

    2009-11-27

    We evaluate black carbon (BC) model predictions from the AeroCom model intercomparison project by considering the diversity among year 2000 model simulations and comparing model predictions with available measurements. These model-measurement intercomparisons include BC surface and aircraft concentrations, aerosol absorption optical depth (AAOD) from AERONET and OMI retrievals and BC column estimations based on AERONET. In regions other than Asia, most models are biased high compared to surface concentration measurements. However compared with (column) AAOD or BC burden retreivals, the models are generally biased low. The average ratio of model to retrieved AAOD is less than 0.7 in South American and 0.6 in African biomass burning regions; both of these regions lack surface concentration measurements. In Asia the average model to observed ratio is 0.6 for AAOD and 0.5 for BC surface concentrations. Compared with aircraft measurements over the Americas at latitudes between 0 and 50N, the average model is a factor of 10 larger than observed, and most models exceed the measured BC standard deviation in the mid to upper troposphere. At higher latitudes the average model to aircraft BC is 0.6 and underestimate the observed BC loading in the lower and middle troposphere associated with springtime Arctic haze. Low model bias for AAOD but overestimation of surface and upper atmospheric BC concentrations at lower latitudes suggests that most models are underestimating BC absorption and should improve estimates for refractive index, particle size, and optical effects of BC coating. Retrieval uncertainties and/or differences with model diagnostic treatment may also contribute to the model-measurement disparity. Largest AeroCom model diversity occurred in northern Eurasia and the remote Arctic, regions influenced by anthropogenic sources. Changing emissions, aging, removal, or optical properties within a single model generated a smaller change in model predictions than the

  20. Epoxide pathways improve model predictions of isoprene markers and reveal key role of acidity in aerosol formation

    EPA Science Inventory

    Isoprene significantly contributes to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, the Community Multiscale Air Quality model is updated to predict isoprene aerosol from epoxides produced under both ...

  1. A global average model of atmospheric aerosols for radiative transfer calculations

    NASA Technical Reports Server (NTRS)

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

    1976-01-01

    A global average model is proposed for the size distribution, chemical composition, and optical thickness of stratospheric and tropospheric aerosols. This aerosol model is designed to specify the input parameters to global average radiative transfer calculations which assume the atmosphere is horizontally homogeneous. The model subdivides the atmosphere at multiples of 3 km, where the surface layer extends from the ground to 3 km, the upper troposphere from 3 to 12 km, and the stratosphere from 12 to 45 km. A list of assumptions made in construction of the model is presented and discussed along with major model uncertainties. The stratospheric aerosol is modeled as a liquid mixture of 75% H2SO4 and 25% H2O, while the tropospheric aerosol consists of 60% sulfate and 40% soil particles above 3 km and of 50% sulfate, 35% soil particles, and 15% sea salt below 3 km. Implications and consistency of the model are discussed.

  2. Direct radiative effects of aerosols over South Asia from observations and modeling

    NASA Astrophysics Data System (ADS)

    Nair, Vijayakumar S.; Babu, S. Suresh; Manoj, M. R.; Moorthy, K. Krishna; Chin, Mian

    2016-10-01

    Quantitative assessment of the seasonal variations in the direct radiative effect (DRE) of composite aerosols as well as the constituent species over the Indian sub continent has been carried out using a synergy of observations from a dense network of ground based aerosol observatories and modeling based on chemical transport model simulations. Seasonal variation of aerosol constituents depict significant influence of anthropogenic aerosol sources in winter and the dominance of natural sources in spring, even though the aerosol optical depth doesn't change significantly between these two seasons. A significant increase in the surface cooling and atmospheric warming has been observed as season changes from winter (DRESUR = -28 ± 12 W m-2 and DREATM = +19.6 ± 9 W m-2) to spring (DRESUR = -33.7 ± 12 W m-2 and DREATM = +27 ± 9 W m-2). Interestingly, springtime aerosols are more absorptive in nature compared to winter and consequently the aerosol induced diabatic heating of the atmosphere goes as high as 1 K day-1 during spring, especially over eastern India. The atmospheric DRE due to dust aerosols (+14 ± 7 W m-2) during spring overwhelms that of black carbon DRE (+11.8 ± 6 W m-2) during winter. The DRE at the top of the atmosphere is mostly governed by the anthropogenic aerosols during all the seasons. The columnar aerosol loading, its anthropogenic fraction and radiative effects shows a steady increase with latitude across Indian mainland leading to a larger aerosol-induced atmospheric warming during spring than in winter.

  3. Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean - potential impacts

    NASA Astrophysics Data System (ADS)

    Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier van der Gon, H. A. C.

    2010-07-01

    Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, indicating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols shows that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud, and by entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

  4. THERMODYNAMIC MODELING OF LIQUID AEROSOLS CONTAINING DISSOLVED ORGANICS AND ELECTROLYTES

    EPA Science Inventory

    Many tropospheric aerosols contain large fractions of soluble organic material, believed to derive from the oxidation of precursors such alpha-pinene. The chemical composition of aerosol organic matter is complex and not yet fully understood.

    The key properties of solu...

  5. Modeling Trends in Tropospheric Aerosol Burden & Its Radiative Effects

    EPA Science Inventory

    Large changes in emissions of aerosol precursors have occurred across the southeast U.S., North America, as well as the northern hemisphere. The spatial heterogeneity and contrasting trends in the aerosol burden is resulting in differing effects on regional radiative balance. Mul...

  6. Towards improved MODIS aerosol retrieval over the US East Coast region: Re-examining the aerosol model and surface assumptions

    NASA Astrophysics Data System (ADS)

    Levy, R. C.; Remer, L. A.; Kaufman, Y. J.; Holben, B. N.

    2002-12-01

    The MODerate resolution Imaging Spectrometer (MODIS) aboard the Terra and recently the Aqua platform, produces a set of aerosol products over both ocean and land regions. Previous validation efforts have shown that from a global perspective, aerosol optical depth (AOD) is successfully retrieved from MODIS. Even over coastal regions, the over-land and over-ocean retrievals are consistent with each other, and well matched with ground-based sunphotometer measurements (such as AERONET). However, the East Coast of the United States is one region where there is consistently a discrepancy between land and ocean retrievals. Over the ocean, MODIS AODs are consistent with coastal sunphotometer measurements, but over land, AODs are consistently over-estimated. In this study we use field data from the Chesapeake Lighthouse and Aircraft Measurements for Satellites experiment (CLAMS), (held during summer 2001) to determine the aerosol properties at a number of sites. Using the 6-S radiative transfer package, we compute simulated satellite radiances and compare them with observed MODIS radiances. We believe that the AOD over-estimation is not likely due to an incorrect choice of the urban/industrial aerosol models. Using 6-S to do an atmospheric correction for a very low AOD case, we show rather, that the discrepancies are likely a result of incorrect assumptions about the surface reflectance properties. Understanding and improving MODIS retrievals over the East Coast will not only improve the global quality of MODIS, but also would enable the use of MODIS as a tool for monitoring regional aerosol events.

  7. Simulation of aromatic SOA formation using the lumping model integrated with explicit gas-phase kinetic mechanisms and aerosol-phase reactions

    NASA Astrophysics Data System (ADS)

    Im, Y.; Jang, M.; Beardsley, R. L.

    2014-04-01

    The Unified Partitioning-Aerosol phase Reaction (UNIPAR) model has been developed to predict the secondary organic aerosol (SOA) formation through multiphase reactions. The model was evaluated with aromatic SOA data produced from the photooxidation of toluene and 1,3,5-trimethylbenzene (135-TMB) under various concentrations of NOx and SO2 using an outdoor reactor (University of Florida Atmospheric PHotochemical Outdoor Reactor (UF-APHOR) chamber). When inorganic species (sulfate, ammonium and water) are present in aerosol, the prediction of both toluene SOA and 135-TMB SOA, in which the oxygen-to-carbon (O : C) ratio is lower than 0.62, are approached under the assumption of a complete organic/electrolyte-phase separation below a certain relative humidity. An explicit gas-kinetic model was employed to express gas-phase oxidation of aromatic hydrocarbons. Gas-phase products are grouped based on their volatility (6 levels) and reactivity (5 levels) and exploited to construct the stoichiometric coefficient (αi,j) matrix, the set of parameters used to describe the concentrations of organic compounds in multiphase. Weighting of the αi,j matrix as a function of NOx improved the evaluation of NOx effects on aromatic SOA. The total amount of organic matter (OMT) is predicted by two modules in the UNIPAR model: OMP by a partitioning process and OMAR by aerosol-phase reactions. The OMAR module predicts multiphase reactions of organic compounds, such as oligomerization, acid-catalyzed reactions, and organosulfate (OS) formation. The model reasonably simulates SOA formation under various aerosol acidities, NOx concentrations, humidities and temperatures. Furthermore, the OS fractions in the SOA predicted by the model were in good agreement with the experimentally measured OS fractions.

  8. Evaluation of the aerosol vertical distribution in global aerosol models through comparison against CALIOP measurements: AeroCom phase II results: AEROSOL PROFILES IN AEROCOM II GCM

    SciTech Connect

    Koffi, Brigitte; Schulz, Michael; Bréon, François-Marie; Dentener, Frank; Steensen, Birthe Marie; Griesfeller, Jan; Winker, David; Bauer, Susanne E.; Bellouin, Nicolas; Berntsen, Terje; Bian, Huisheng; Chin, Mian; Diehl, Thomas; Easter, Richard; Ghan, Steven; Hauglustaine, Didier A.; Iversen, Trond; Kirkevåg, Alf; Liu, Xiaohong; Lohmann, Ulrike; Myhre, Gunnar; Rasch, Phil; Seland, Øyvind; Skeie, Ragnhild B.; Steenrod, Stephen D.; Stier, Philip; Tackett, Jason; Takemura, Toshihiko; Tsigaridis, Kostas; Vuolo, Maria Raffaella; Yoon, Jinho; Zhang, Kai

    2016-06-27

    The ability of eleven models in simulating the aerosol vertical distribution from regional to global scales, as part of the second phase of the AeroCom model inter-comparison initiative (AeroCom II) is assessed and compared to results of the first phase. The evaluation is performed using a global monthly gridded dataset of aerosol extinction profiles built on purpose from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Layer Product 3.01. Results over 12 sub-continental regions show that five models improved whereas three degraded in reproducing the Zα 0-6 km mean extinction height diagnostic, which is computed over the 0-6 km altitude range for each studied region and season. While the models’ performance remains highly variable, it has generally improved in terms of inter-regional diversity and seasonality. The biases in Zα 0-6 km have notably decreased in the U.S. and European industrial and downwind maritime regions, whereas the timing of the Zα 0-6 km peak season has improved for all but two models. However, most of the models now show a Zα 0-