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Sample records for aerosol hygroscopic properties

  1. [Hygroscopic Properties of Aerosol Particles in North Suburb of Nanjing in Spring].

    PubMed

    Xu, Bin; Zhang, Ze-feng; Li, Yan-weil; Qin, Xin; Miao, Qing; Shen, Yan

    2015-06-01

    The hygroscopic properties of submicron aerosol particles have significant effects on spectral distribution, CCN activation, climate forcing, human health and so on. A Hygroscopic Tandem Differential Mobility Analyzer (HTDMA) was utilized to analyze the hygroscopic properties of aerosol particles in the northern suburb of Nanjing during 16 April to 21 May, 2014. At relative humidity (RH) of 90%, for particles with dry diameters 30-230 nm, the probability distribution of GF (GF-PDF) shows a distinct bimodal pattern, with a dominant more-hygroscopic group and a smaller less-hygroscopic group. A contrast analysis between day and night suggests that, aerosol particles during day time have a stronger hygroscopicity and a higher number fraction of more-hygroscopic group than that at night overall. Aerosol particles during night have a higher degree of externally mixed state. Backward trajectory analysis using HYSPLIT mode reveals that, the sampling site is mainly affected by three air masses. For aitken nuclei, northwest continental air masses experience a longer aging process and have a stronger hygroscopicity. For condensation nuclei, east air masses have a stronger hygroscopicity and have a higher number fraction of more-hygroscopic group. Aerosol particles in local air masses have a high number fraction of more-hygroscopic group in the whole diameter range.

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

    NASA Astrophysics Data System (ADS)

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

    2007-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  4. Hygroscopic properties of levoglucosan and related organic compounds characteristic to biomass burning aerosol particles

    NASA Astrophysics Data System (ADS)

    Mochida, Michihiro; Kawamura, Kimitaka

    2004-11-01

    Biomass burning, which is characterized by pyrolysis as well as vaporization and condensation of biomass constituents, is a significant source of atmospheric organic aerosols. In this study, hygroscopic properties of five organic compounds (levoglucosan, D-glucose, and vanillic, syringic, and 4-hydroxybenozoic acids), which are major pyrolysis products of wood, were measured using a tandem differential mobility analyzer. Levoglucosan, which is typically the most abundant species in wood burning aerosols, showed a significant hygroscopic growth for particles with a diameter of 100 nm. No efflorescence was observed under the measured relative humidity, and a supersaturated condition of levoglucosan-water particles was observed. The growth factors of levoglucosan are 1.08, 1.18, 1.23, and 1.38 at relative humidity (RH) of 60, 80, 85, and 90%, respectively. The measured hygroscopic curves are in general consistent with those estimated from ideal solution theory and Uniquac Functional-Group Activity Coefficient (UNIFAC) and Conductor-Like Screening Model for Real Solvent (COSMO-RS) methods. Significant hygroscopic growth was also observed for D-glucose, whose growth factor is quite similar to that of levoglucosan. However, three model pyrolysis products of lignin (i.e., vanillic-, syringic-, and 4-hydroxybenzoic acids) did not show any hygroscopic growth under the RH conditions up to 95%. On the basis of the organic composition of wood burning aerosols, the water absorption attributed to levoglucosan in wood burning aerosols is calculated to be up to 30% of the organic mass at 90% RH. This study demonstrates that oxygenated organics emitted from biomass burning could significantly enhance the hygroscopic properties of atmospheric aerosols.

  5. Vertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, Bernadette; Gysel, Martin; Rubach, Florian; Mentel, Thomas F.; Goger, Brigitta; Poulain, Laurent; Schlag, Patrick; Miettinen, Pasi; Pajunoja, Aki; Virtanen, Annele; Klein Baltink, Henk; Bas Henzing, J. S.; Größ, Johannes; Gobbi, Gian Paolo; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Decesari, Stefano; Facchini, Maria Cristina; Weingartner, Ernest; Baltensperger, Urs

    2016-06-01

    Vertical profiles of the aerosol particles hygroscopic properties, their mixing state as well as chemical composition were measured above northern Italy and the Netherlands. An aerosol mass spectrometer (AMS; for chemical composition) and a white-light humidified optical particle spectrometer (WHOPS; for hygroscopic growth) were deployed on a Zeppelin NT airship within the PEGASOS project. This allowed one to investigate the development of the different layers within the planetary boundary layer (PBL), providing a unique in situ data set for airborne aerosol particles properties in the first kilometre of the atmosphere. Profiles measured during the morning hours on 20 June 2012 in the Po Valley, Italy, showed an increased nitrate fraction at ˜ 100 m above ground level (a.g.l.) coupled with enhanced hygroscopic growth compared to ˜ 700 m a. g. l. This result was derived from both measurements of the aerosol composition and direct measurements of the hygroscopicity, yielding hygroscopicity parameters (κ) of 0.34 ± 0.12 and 0.19 ± 0.07 for 500 nm particles, at ˜ 100 and ˜ 700 m a. g. l., respectively. The difference is attributed to the structure of the PBL at this time of day which featured several independent sub-layers with different types of aerosols. Later in the day the vertical structures disappeared due to the mixing of the layers and similar aerosol particle properties were found at all probed altitudes (mean κ ≈ 0.18 ± 0.07). The aerosol properties observed at the lowest flight level (100 m a. g. l.) were consistent with parallel measurements at a ground site, both in the morning and afternoon. Overall, the aerosol particles were found to be externally mixed, with a prevailing hygroscopic fraction. The flights near Cabauw in the Netherlands in the fully mixed PBL did not feature altitude-dependent characteristics. Particles were also externally mixed and had an even larger hygroscopic fraction compared to the results in Italy. The mean κ from

  6. Hygroscopic Properties of Aircraft Engine Exhaust Aerosol Produced From Traditional and Alternative Fuels

    NASA Astrophysics Data System (ADS)

    Moore, R.; Ziemba, L. D.; Beyersdorf, A. J.; Thornhill, K. L.; Winstead, E. L.; Crumeyrolle, S.; Chen, G.; Anderson, B. E.

    2012-12-01

    Aircraft emissions of greenhouse gases and aerosols constitute an important component of anthropogenic climate forcing, of which aerosol-cloud interactions remain poorly understood. It is currently thought that the ability of these aerosols to alter upper tropospheric cirrus cloud properties may produce radiative forcings many times larger than the impact of linear contrails alone and which may partially offset the impact of greenhouse gas emissions from aviation (Burkhardt and Karcher, Nature, 2011). Consequently, it is important to characterize the ability of these engine-emitted aerosol to act as cloud condensation nuclei (CCN) and ice nuclei (IN) to form clouds. While a number of studies in the literature have examined aerosol-cloud interactions for laboratory-generated soot or from aircraft engines burning traditional fuels, limited attention has been given to how switching to alternative jet fuels impacts the ability of engine-emitted aerosols to form clouds. The key to understanding these changes is the aerosol hygroscopicity. To address this need, the second NASA Alternative Aviation Fuel Experiment (AAFEX-II) was conducted in 2011 to examine the aerosol emissions from the NASA DC-8 under a variety of different engine power and fuel type conditions. Five fuel types were considered including traditional JP-8 fuel, synthetic Fischer-Tropsh (FT) fuel , sulfur-doped FT fuel (FTS) , hydrotreated renewable jet (HRJ) fuel, and a 50:50 blend of JP-8 with HRJ. Emissions were sampled from the DC-8 on the airport jetway at a distance of 145 meters downwind of the engine by a comprehensive suite of aerosol instrumentation that provided information on the aerosol concentration, size distribution, soot mass, and CCN activity. Concurrent measurements of carbon dioxide were used to account for plume dilution so that characteristic emissions indices could be determined. It is found that both engine power and fuel type significantly influence the hygroscopic properties of

  7. Vertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, B.; Gysel, M.; Rubach, F.; Mentel, T. F.; Goger, B.; Poulain, L.; Schlag, P.; Miettinen, P.; Pajunoja, A.; Virtanen, A.; Bialek, J.; Klein Baltink, H.; Henzing, J. S.; Größ, J.; Gobbi, G. P.; Wiedensohler, A.; Kiendler-Scharr, A.; O'Dowd, C.; Decesari, S.; Facchini, M. C.; Weingartner, E.; Baltensperger, U.

    2015-03-01

    Airborne measurements of the aerosol hygroscopic and optical properties as well as chemical composition were performed in the Netherlands and northern Italy on board of a Zeppelin NT airship during the PEGASOS field campaigns in 2012. The vertical changes in aerosol properties during the development of the mixing layer were studied. Hygroscopic growth factors (GF) at 95% relative humidity were determined using the white-light humidified optical particles spectrometer (WHOPS) for dry diameters of 300 and 500 nm particles. These measurements were supplemented by an aerosol mass spectrometer (AMS) and an aethalometer providing information on the aerosol chemical composition. Several vertical profiles between 100 and 700 m a.g. were flown just after sunrise close to the San Pietro Capofiume ground station in the Po Valley, Italy. During the early morning hours the lowest layer (newly developing mixing layer) contained a high nitrate fraction (20%) which was coupled with enhanced hygroscopic growth. In the layer above (residual layer) small nitrate fractions of ~ 2% were measured as well as low GFs. After full mixing of the layers, typically around noon and with increased temperature, the nitrate fraction decreased to 2% at all altitudes and led to similar hygroscopicity values as found in the residual layer. These distinct vertical and temporal changes underline the importance of airborne campaigns to study aerosol properties during the development of the mixed layer. The aerosol was externally mixed with 22 and 67% of the 500 nm particles in the range GF < 1.1 and GF > 1.5, respectively. Contributors to the non-hygroscopic mode in the observed size range are most likely mineral dust and biological material. Mean hygroscopicity parameters (κ) were 0.34, 0.19 and 0.18 for particles in the newly forming mixing layer, residual layer and fully mixed layer, respectively. These results agree well with those from chemical analysis which found values of κ = 0.27, 0.21 and 0

  8. Aerosol optical properties in the southeastern United States in summer - Part 1: Hygroscopic growth

    NASA Astrophysics Data System (ADS)

    Brock, C. A.; Wagner, N. L.; Anderson, B. E.; Attwood, A. R.; Beyersdorf, A.; Campuzano-Jost, P.; Carlton, A. G.; Day, D. A.; Diskin, G. S.; Gordon, T. D.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Markovic, M. Z.; Middlebrook, A. M.; Ng, N. L.; Perring, A. E.; Richardson, M. S.; Schwarz, J. P.; Washenfelder, R. A.; Welti, A.; Xu, L.; Ziemba, L. D.; Murphy, D. M.

    2015-09-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made during May-September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at three relative humidities and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. Using this approach, the hygroscopicity parameter κ for the organic fraction of the aerosol must have been < 0.10 to be consistent with 75 % of the observations within uncertainties. This subsaturated κ value for the organic aerosol in the southeastern US is consistent with several field studies in rural environments. We present a new parameterization of the change in aerosol extinction as a function of relative humidity that better describes the observations than does the widely used power-law (gamma, γ) parameterization. This new single-parameter κext formulation is based upon κ-Köhler and Mie theories and relies upon the well-known approximately linear relationship between particle volume (or mass) and optical extinction (Charlson et al., 1967). The fitted parameter, κext, is nonlinearly related to the chemically derived κ parameter used in κ-Köhler theory. The values of κext we determined from airborne measurements are consistent with independent observations at a nearby ground site.

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

    PubMed

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

    2008-07-29

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

  10. Hygroscopicity, CCN and volatility properties of submicron atmospheric aerosol in a boreal forest environment during the summer of 2010

    NASA Astrophysics Data System (ADS)

    Hong, J.; Häkkinen, S. A. K.; Paramonov, M.; Äijälä, M.; Hakala, J.; Nieminen, T.; Mikkilä, J.; Prisle, N. L.; Kulmala, M.; Riipinen, I.; Bilde, M.; Kerminen, V.-M.; Petäjä, T.

    2014-05-01

    A Volatility-Hygroscopicity Tandem Differential Mobility Analyzer (VH-TDMA) was applied to study the hygroscopicity and volatility properties of submicron atmospheric aerosol particles in a boreal forest environment in Hyytiälä, Finland during the summer of 2010. Aitken and accumulation mode internally mixed particles (50 nm, 75 nm and 110 nm in diameter) were investigated. Hygroscopicity was found to increase with particle size. The relative mass fraction of organics and SO42- is probably the major contributor to the fluctuation of the hygroscopicity for all particle sizes. The Cloud Condensation Nuclei Counter (CCNC)-derived hygroscopicity parameter κ was observed to be slightly higher than κ calculated from VH-TDMA data under sub-saturated conditions, potential reasons for this behavior are discussed shortly. Also, the size-resolved volatility properties of particles were investigated. Upon heating, more small particles evaporated compared to large particles. There was a significant amount of aerosol volume (non-volatile material) left, even at heating temperatures of 280 °C. Using size resolved volatility-hygroscopicity analysis, we concluded that there was always hygroscopic material remaining in the particles at different heating temperatures, even at 280 °C. This indicates that the observed non-volatile aerosol material did not consist solely of black carbon.

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

    NASA Astrophysics Data System (ADS)

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

    2014-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

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

  13. Using environmental scanning electron microscopy to determine the hygroscopic properties of agricultural aerosols

    NASA Astrophysics Data System (ADS)

    Hiranuma, Naruki; Brooks, Sarah D.; Auvermann, Brent W.; Littleton, Rick

    A field study at a cattle feedlot in the Texas Panhandle was conducted to characterize the hygroscopic, morphological, and chemical properties of agricultural aerosols and to identify possible correlations between these properties. To explore the hygroscopic nature of the agricultural particles, we have collected size-resolved aerosol samples using a cascade impactor system and have used an environmental scanning electron microscope (ESEM) to determine the water uptake by individual particles in those samples as a function of relative humidity (RH). In addition, complementary determination of the elemental composition of single particles was performed using energy dispersive X-ray spectroscopy (EDS). Our results indicate that most of the agricultural particles do not take up significant amounts of water when exposed to up to 96% RH. However, a small fraction of particles in the coarse mode deliquesced at approximately 75% RH and reached twice their original sizes by 96% RH. The observed changes in particle size with increased RH may significantly impact total aerosol extinction, visibility, and human health.

  14. Physiochemical properties of carbonaceous aerosol from agricultural residue burning: Density, volatility, and hygroscopicity

    NASA Astrophysics Data System (ADS)

    Li, Chunlin; Hu, Yunjie; Chen, Jianmin; Ma, Zhen; Ye, Xingnan; Yang, Xin; Wang, Lin; Wang, Xinming; Mellouki, Abdelwahid

    2016-09-01

    Size-resolved effective density, mixing state, and hygroscopicity of smoke particles from five kinds of agricultural residues burning were characterized using an aerosol chamber system, including a volatility/hygroscopic tandem differential mobility analyzer (V/H-TDMA) combined with an aerosol particle mass analyzer (APM). To profile relationship between the thermodynamic properties and chemical compositions, smoke PM1.0 and PM2.5 were also measured for the water soluble inorganics, mineral elements, and carbonaceous materials like organic carbon (OC) and elemental carbon (EC). Smoke particle has a density of 1.1-1.4 g cm-3, and hygroscopicity parameter (κ) derived from hygroscopic growth factor (GF) of the particles ranges from 0.20 to 0.35. Size- and fuel type-dependence of density and κ are obvious. The integrated effective densities (ρ) and hygroscopicity parameters (κ) both scale with alkali species, which could be parameterized as a function of organic and inorganic mass fraction (forg &finorg) in smoke PM1.0 and PM2.5: ρ-1 =finorg ·ρinorg-1 +forg · ρorg-1 and κ =finorg ·κinorg +forg ·κorg . The extrapolated values of ρinorg and ρorg are 2.13 and 1.14 g cm-3 in smoke PM1.0, while the characteristic κ values of organic and inorganic components are about 0.087 and 0.734, which are similar to the bulk density and κ calculated from predefined chemical species and also consistent with those values observed in ambient air. Volatility of smoke particle was quantified as volume fraction remaining (VFR) and mass fraction remaining (MFR). The gradient temperature of V-TDMA was set to be consistent with the splitting temperature in the OC-EC measurement (OC1 and OC2 separated at 150 and 250 °C). Combing the thermogram data and chemical composition of smoke PM1.0, the densities of organic matter (OM1 and OM2 correspond to OC1 and OC2) are estimated as 0.61-0.90 and 0.86-1.13 g cm-3, and the ratios of OM1/OC1 and OM2/OC2 are 1.07 and 1.29 on average

  15. Physiochemical properties of carbonaceous aerosol from agricultural residue burning: Density, volatility, and hygroscopicity

    NASA Astrophysics Data System (ADS)

    Li, Chunlin; Hu, Yunjie; Chen, Jianmin; Ma, Zhen; Ye, Xingnan; Yang, Xin; Wang, Lin; Wang, Xinming; Mellouki, Abdelwahid

    2016-09-01

    Size-resolved effective density, mixing state, and hygroscopicity of smoke particles from five kinds of agricultural residues burning were characterized using an aerosol chamber system, including a volatility/hygroscopic tandem differential mobility analyzer (V/H-TDMA) combined with an aerosol particle mass analyzer (APM). To profile relationship between the thermodynamic properties and chemical compositions, smoke PM1.0 and PM2.5 were also measured for the water soluble inorganics, mineral elements, and carbonaceous materials like organic carbon (OC) and elemental carbon (EC). Smoke particle has a density of 1.1-1.4 g cm-3, and hygroscopicity parameter (κ) derived from hygroscopic growth factor (GF) of the particles ranges from 0.20 to 0.35. Size- and fuel type-dependence of density and κ are obvious. The integrated effective densities (ρ) and hygroscopicity parameters (κ) both scale with alkali species, which could be parameterized as a function of organic and inorganic mass fraction (forg &finorg) in smoke PM1.0 and PM2.5: ρ-1 =finorg · ρinorg-1 +forg · ρorg-1 and κ =finorg ·κinorg +forg ·κorg . The extrapolated values of ρinorg and ρorg are 2.13 and 1.14 g cm-3 in smoke PM1.0, while the characteristic κ values of organic and inorganic components are about 0.087 and 0.734, which are similar to the bulk density and κ calculated from predefined chemical species and also consistent with those values observed in ambient air. Volatility of smoke particle was quantified as volume fraction remaining (VFR) and mass fraction remaining (MFR). The gradient temperature of V-TDMA was set to be consistent with the splitting temperature in the OC-EC measurement (OC1 and OC2 separated at 150 and 250 °C). Combing the thermogram data and chemical composition of smoke PM1.0, the densities of organic matter (OM1 and OM2 correspond to OC1 and OC2) are estimated as 0.61-0.90 and 0.86-1.13 g cm-3, and the ratios of OM1/OC1 and OM2/OC2 are 1.07 and 1.29 on average

  16. Optical and Physicochemical Properties of Brown Carbon Aerosol: Light Scattering, FTIR Extinction Spectroscopy, and Hygroscopic Growth.

    PubMed

    Tang, Mingjin; Alexander, Jennifer M; Kwon, Deokhyeon; Estillore, Armando D; Laskina, Olga; Young, Mark A; Kleiber, Paul D; Grassian, Vicki H

    2016-06-23

    in the mid-IR range (800 to 7000 cm(-1)) also showed no significant changes in either the real or the imaginary parts of the refractive indices for brown carbon aerosol particles when compared to ammonium sulfate. Therefore, changes in the optical properties of ammonium sulfate in the mid-IR spectral range due to reaction with methylglyoxal appear to be insignificant. In addition to these measurements, we have characterized additional physicochemical properties of the brown carbon aerosol particles including hygroscopic growth using a tandem-differential mobility analyzer. Compared to ammonium sulfate, brown carbon aerosol particles are found to have lower deliquescence relative humidity (DRH), efflorescence relative humidity (ERH), and hygroscopic growth at the same relative humidities. Overall, our study provides new details of the optical and physicochemical properties of a class of secondary organic aerosol which may have important implications for atmospheric chemistry and climate.

  17. Optical and Physicochemical Properties of Brown Carbon Aerosol: Light Scattering, FTIR Extinction Spectroscopy, and Hygroscopic Growth.

    PubMed

    Tang, Mingjin; Alexander, Jennifer M; Kwon, Deokhyeon; Estillore, Armando D; Laskina, Olga; Young, Mark A; Kleiber, Paul D; Grassian, Vicki H

    2016-06-23

    in the mid-IR range (800 to 7000 cm(-1)) also showed no significant changes in either the real or the imaginary parts of the refractive indices for brown carbon aerosol particles when compared to ammonium sulfate. Therefore, changes in the optical properties of ammonium sulfate in the mid-IR spectral range due to reaction with methylglyoxal appear to be insignificant. In addition to these measurements, we have characterized additional physicochemical properties of the brown carbon aerosol particles including hygroscopic growth using a tandem-differential mobility analyzer. Compared to ammonium sulfate, brown carbon aerosol particles are found to have lower deliquescence relative humidity (DRH), efflorescence relative humidity (ERH), and hygroscopic growth at the same relative humidities. Overall, our study provides new details of the optical and physicochemical properties of a class of secondary organic aerosol which may have important implications for atmospheric chemistry and climate. PMID:27253434

  18. Comparative analysis of hygroscopic properties of atmospheric aerosols at ZOTTO Siberian background station during summer and winter campaigns of 2011

    NASA Astrophysics Data System (ADS)

    Ryshkevich, T. I.; Mironov, G. N.; Mironova, S. Yu.; Vlasenko, S. S.; Chi, X.; Andreae, M. O.; Mikhailov, E. F.

    2015-09-01

    The results of measurements of hygroscopic properties and chemical analysis of atmospheric aerosol samples collected from June 10 to 20 and December 15 to 25, 2011, at the ZOTTO background stations (60.8° N, 89.35° E) in Central Siberia are presented. The sorption properties of aerosols are studied with the help of a differential analyzer of absorbed water mass in the relative humidity range of 5 to 99%. It has been found that the hygroscopic growth factor of aerosol particles collected during the winter campaign is on average 45% higher than that of the aerosol collected in the summer campaign, which leads to a 40% decrease in the critical supersaturation threshold of cloud activation of particles. The measurement data are analyzed and parameterized using a new approach that takes into account the concentration effects in the particle—water vapor system at low humidities. Based on the chemical analysis, the content of water-soluble substances in the winter sample is 2.5 times higher than in the summer sample. Here, the amount of sulfates and nitrates increases 20 and 88 times, respectively. A trajectory analysis of air mass motion shows that the increased content of inorganic ions in aerosols for the winter sample is caused by long-range transport of pollutants from industrial areas of Siberia. This difference in the chemical composition is the main source of the observed difference in hygroscopic and condensation properties of the aerosol particles.

  19. Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain

    NASA Astrophysics Data System (ADS)

    Liu, P. F.; Zhao, C. S.; Göbel, T.; Hallbauer, E.; Nowak, A.; Ran, L.; Xu, W. Y.; Deng, Z. Z.; Ma, N.; Mildenberger, K.; Henning, S.; Stratmann, F.; Wiedensohler, A.

    2011-01-01

    The hygroscopic properties of submicron aerosol particles were determined at a suburban site (Wuqing) in the North China Plain among a cluster of cities during the period 17 July to 12 August 2009. A High Humidity Tandem Differential Mobility Analyser (HH-TDMA) instrument was applied to measure the hygroscopic growth factor (GF) at 90%, 95% and 98.5% relative humidity (RH) for particles with dry diameter between 50-250 nm. The probability distribution of GF (GF-PDF) averaged over the period shows a distinct bimodal pattern, namely, a dominant more-hygroscopic (MH) group and a smaller nearly-hydrophobic (NH) group. The MH group particles were highly hygroscopic, and their GF was relatively constant during the period with average values of 1.54±0.02, 1.81±0.04 and 2.45±0.07 at 90%, 95% and 98.5% RH (D0=100 nm), respectively. The NH group particles grew very slightly when exposed to high RH, with GF values of 1.08±0.02, 1.13±0.06 and 1.24±0.13, respectively at 90%, 95% and 98.5% RH (D0=100 nm). The hygroscopic growth behaviours at different RHs were well represented by the hygroscopicity parameter κ with a single-parameter Köhler model. Thus, the calculation of GF as a function of RH and dry diameter could be facilitated by an empirical parameterization of κ as function of dry diameter. A strong diurnal pattern in number fraction of different hygroscopic groups was observed, indicating a diurnal variation of aerosol mixing state and/or chemical composition. The average number fraction of NH particles during the day was about 8%, while during the nighttime fractions up to 20% were reached. Correspondingly, the state of mixing in terms of water uptake varied significantly during a day. The high fraction of NH particles measured during the night denotes a high degree of external mixing of ambient aerosols, while during the day the degree of external mixing decreased. Simulations using a particle-resolved aerosol box model (PartMC-MOSAIC) suggest that the diurnal

  20. Chemical and hygroscopic properties of aerosol organics at Storm Peak Laboratory

    NASA Astrophysics Data System (ADS)

    Hallar, A. Gannet; Lowenthal, Douglas H.; Clegg, Simon L.; Samburova, Vera; Taylor, Nathan; Mazzoleni, Lynn R.; Zielinska, Barbara K.; Kristensen, Thomas B.; Chirokova, Galina; McCubbin, Ian B.; Dodson, Craig; Collins, Don

    2013-05-01

    A combined field and laboratory study was conducted to improve our understanding of the chemical and hygroscopic properties of organic compounds in aerosols sampled in the background continental atmosphere. PM2.5 (particles with aerodynamic diameters smaller than 2.5 µm) aerosols were collected from 24 June to 28 July 2010 at Storm Peak Laboratory (SPL) in the Park Range of northwestern Colorado. New particle formation (NPF) was frequent at SPL during this campaign, and the samples were not influenced by regional dust storms. Filter samples were analyzed for organic carbon (OC) and elemental carbon (EC), water soluble OC (WSOC), major inorganic ions, and detailed organic speciation. WSOC was isolated from inorganic ions using solid phase absorbents. Hygroscopic growth factors (GFs) and cloud condensation nucleus (CCN) activity of the WSOC were measured in the laboratory. Organic compounds compose the majority (average of 64% with a standard deviation (SD) of 9%) of the mass of measured species and WSOC accounted for an average of 89% (with a SD of 21%) of OC mass. Daily samples were composited according to back trajectories. On average, organic acids, sugars, and sugar alcohols accounted for 12.5 ± 6.2% (average ± SD) of WSOC. Based on the composition of these compounds and that of high molecular weight compounds identified using ultra high resolution mass spectrometry, the organic mass to OC ratio of the WSOC is estimated to be 2.04. The average hygroscopic GFs at RH = 80% (GF80) were 1.10 ± 0.03 for particles derived from isolated WSOC and 1.27 ± 0.03 for particles derived from the total water-soluble material (WSM). CCN activity followed a similar pattern. The critical diameters at a super-saturation of 0.35% were 0.072 ± 0.009 and 0.094 ± 0.006 µm for particles derived from WSM and isolated WSOC, respectively. These GF results compare favorably with estimates from thermodynamic models, which explicitly relate the water activity (RH) to concentration for

  1. A 12-year observation of chemical and hygroscopic properties of marine aerosols over the western North Pacific

    NASA Astrophysics Data System (ADS)

    Boreddy, S. K. R.; Kawamura, K.

    2015-12-01

    Anthropogenic emissions from East Asia, especially in China, have significantly increased over the recent decades due to the rapid industrial development. They are implausible to decline in the next 20 years and may have a strong impact on tropospheric chemistry in marine boundary layer and cloud properties over the western North Pacific. To better understand the long-term observation of aerosol characterization and their effect on the hygroscopicity and precipitation process over the western North Pacific, we collected TSP aerosol samples on a weekly basis during the 2001-2012 at a remote marine island, Chichijima (27°04'E; 142°13'N), which is located in the outflow region of Asian dust and East Asian anthropogenic pollutants. We present here long-term observations of seasonal and annual variation of chemical and hygroscopic properties of water-soluble matter, extracted from the remote marine aerosols, based on the measurement of major inorganic ions, total organic carbon and hygroscopicity by HTDMA. Concentrations of nss-SO42- are high in winter and spring and low in summer, whereas hygroscopicity is high in summer to autumn and low in winter to spring, probably due to the influence of long-range transport of anthropogenic pollutants and dusts. Annual variation of nss-SO42- increased from 2001 to 2006 and continuously decreased from 2007 to 2012, probably due to the decreased SO2 emissions in East Asia especially in China. In contrast, hygroscopicity (g(90%)ZSR) showed a decrease from 2001 to 2006 and an increase from 2007 to 2012. These results demonstrate that although WSOM often suppress the hygroscopicity of marine aerosols, long-range atmospheric transport of nss-SO42- seriously suppress the hygroscopicity and thus affect the precipitation process over the western North Pacific. This study also demonstrates that Asian dusts can act as an important source of nutrients for phytoplankton and thus sea-to-air emission of dimethyl sulfide and subsequent

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

    PubMed

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

    2012-09-01

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

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

    PubMed Central

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

    2012-01-01

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

  4. 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.

  5. Variations in organic aerosol optical and hygroscopic properties upon heterogeneous OH oxidation

    NASA Astrophysics Data System (ADS)

    Cappa, Christopher D.; Che, Daphne L.; Kessler, Sean H.; Kroll, Jesse H.; Wilson, Kevin R.

    2011-08-01

    Measurements of the evolution of organic aerosol extinction cross sections (σext) and subsaturated hygroscopicity upon heterogeneous OH oxidation are reported for two model compounds, squalane (a C30 saturated hydrocarbon) and azelaic acid (a C9 dicarboxylic acid). For both compounds, the σext values at 532 nm increase substantially as the particles undergo oxidation, exhibiting a logarithmic increase with OH exposure. The increase in σext correlates with both an increase in the particle oxygen to carbon (O:C) atomic ratio and density and a decrease in mean molecular weight. The measurements have been used to calculate the variation with oxidation of the mean polarizability, α, of the molecules comprising the particles. The absolute α values for the two systems are shown to be related through the variation in the particle chemical composition, specifically the relative abundances of C, O, and H atoms and the mean molecular weight. Unlike σext, it was found that the evolution of the particle hygroscopicity upon oxidation is quite different for the two model systems considered. Hygroscopicity was quantified by measuring γext, which is a single-parameter representation of hygroscopicity that describes the increase in extinction upon exposure of the particles to a high-relative humidity environment (here, 75% and 85% RH). For unoxidized squalane, γext was zero and only increased slowly as the particles were oxidized by OH radicals. In contrast, γext for azelaic acid increased rapidly upon exposure to OH, eventually reaching a plateau at high OH exposures. In general, γext appears to vary sigmoidally with O:C, reaching a plateau at high O:C.

  6. Hygroscopic properties and mixing state of aerosol measured at the high altitude site Puy de Dôme (1465 m a.s.l.), France

    NASA Astrophysics Data System (ADS)

    Holmgren, H.; Sellegri, K.; Hervo, M.; Rose, C.; Freney, E.; Villani, P.; Laj, P.

    2014-03-01

    A Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France from September 2008 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal, and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of marine aerosol may be explained by large proportions of inorganic aerosol and sea salts, and it is speculated that continental particles are more hygroscopic than local and African ones due to ageing of fresh combustion aerosol. Aerosol measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less hygroscopic mode (GF < 1.3), a hygroscopic mode (GF 1.3-1.7) and a more hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less hygroscopic mode or the hygroscopic mode, and only few of them have more hygroscopic properties. The

  7. Direct comparison of the hygroscopic properties of ammonium sulfate and sodium chloride aerosol at relative humidities approaching saturation.

    PubMed

    Walker, Jim S; Wills, Jon B; Reid, Jonathan P; Wang, Liangyu; Topping, David O; Butler, Jason R; Zhang, Yun-Hong

    2010-12-01

    Holographic optical tweezers are used to make comparative measurements of the hygroscopic properties of single component aqueous aerosol containing sodium chloride and ammonium sulfate over a range of relative humidity from 84% to 96%. The change in RH over the course of the experiment is monitored precisely using a sodium chloride probe droplet with accuracy better than ±0.09%. The measurements are used to assess the accuracy of thermodynamic treatments of the relationship between water activity and solute mass fraction with particular attention focused on the dilute solute limit approaching saturation vapor pressure. The consistency of the frequently used Clegg-Brimblecombe-Wexler (CBW) treatment for predicting the hygroscopic properties of sodium chloride and ammonium sulfate aerosol is confirmed. Measurements of the equilibrium size of ammonium sulfate aerosol are found to agree with predictions to within an uncertainty of ±0.2%. Given the accuracy of treating equilibrium composition, the inconsistencies highlighted in recent calibration measurements of critical supersaturations of sodium chloride and ammonium sulfate aerosol cannot be attributed to uncertainties associated with the thermodynamic predictions and must have an alternative origin. It is concluded that the CBW treatment can allow the critical supersaturation to be estimated for sodium chloride and ammonium sulfate aerosol with an accuracy of better than ±0.002% in RH. This corresponds to an uncertainty of ≤1% in the critical supersaturation for typical supersaturations of 0.2% and above. This supports the view that these systems can be used to accurately calibrate instruments that measure cloud condensation nuclei concentrations at selected supersaturations. These measurements represent the first study in which the equilibrium properties of two particles of chemically distinct composition have been compared simultaneously and directly alongside each other in the same environment.

  8. Hygroscopic properties and mixing state of aerosol measured at the high-altitude site Puy de Dôme (1465 m a.s.l.), France

    NASA Astrophysics Data System (ADS)

    Holmgren, H.; Sellegri, K.; Hervo, M.; Rose, C.; Freney, E.; Villani, P.; Laj, P.

    2014-09-01

    A Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France, periodically from September 2008 to January 2010, and almost continuously from October 2010 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values, GFs, are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of oceanic aerosol can be explained by large proportions of inorganic aerosol and sea salts. Aerosols measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less-hygroscopic mode (GF < 1.3), a hygroscopic mode (GF 1.3-1.7) and a more-hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less-hygroscopic mode or the hygroscopic mode, and only few of them have more-hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when

  9. Hygroscopic properties of ultrafine aerosol particles in the boreal forest: diurnal variation, solubility and the influence of sulfuric acid

    NASA Astrophysics Data System (ADS)

    Ehn, M.; Petäjä, T.; Aufmhoff, H.; Aalto, P.; Hämeri, K.; Arnold, F.; Laaksonen, A.; Kulmala, M.

    2006-10-01

    Freshly formed atmospheric aerosol particles are neither large enough to efficiently scatter incoming solar radiation nor able to act as cloud condensation nuclei. As the particles grow larger, their hygroscopicity determines the limiting size after which they are important in both of the aforementioned processes. The condensing species resulting in growth alter the hygroscopicity of the particles. We have measured hygroscopic growth of aerosol particles present in a boreal forest, along with the very hygroscopic atmospheric trace gas sulfuric acid. The focus was on days with new particle formation by nucleation. The measured hygroscopic growth factors (GF) correlated positively with gaseous phase sulfuric acid concentrations. This correlation had a strong size dependency; the smaller the particle, the more condensing sulfuric acid is bound to alter the GF due to initially smaller mass. In addition, water uptake of nucleation mode particles was monitored during new particle formation events and followed during their growth to Aitken mode sizes. As the modal diameter increased, the solubility of the particles decreased. This indicated that initially more hygroscopic particles transformed into less hygroscopic or even hydrophobic particles. A similar behavior was seen also during days with no particle formation, with GF decreasing during the evenings and increasing during early morning. This can be tentatively explained by day- and nighttime differences in the hygroscopicity of condensable vapors.

  10. How Important Is Organic Aerosol Hygroscopicity to Aerosol Indirect Forcing?

    SciTech Connect

    Liu, Xiaohong; Wang, Jian

    2010-12-07

    Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation and yield of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR Community Atmospheric Model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (“κ” value) of POA and SOA. Our model simulation indicates that in the present-day condition changing “κ” value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S=0.1% by 40-60% over the POA source regions, while changing “κ” value of SOA by ±50% (from 0.14 to 0.07 and 0.21) changes the CCN within 30%. Changes in the in-cloud droplet number concentrations (CDNC) are within 20% in most locations on the globe with the above changes in “κ” value of POA and SOA. Global annual mean anthropogenic aerosol indirect forcing (AIF) between present-day (PD) and pre-industrial (PI) conditions change by 0.4 W m-2 with the control run of -1.3 W m-2. AIF reduces with the increase hygroscopicity of organic aerosol, indicating the important role of natural organic aerosol in buffering the relative change of CDNC from PI to PD.

  11. Hygroscopicity Behavior, Activation Properties and Chemical Composition of Atmospheric Aerosol at a Background Site in the Megacity Region of Peking

    NASA Astrophysics Data System (ADS)

    Henning, Silvia; Nowak, Andreas; Mildenberger, Katrin; Göbel, Tina; Nekat, Bettina; van Pinxteren, Dominik; Herrmann, Hartmut; Zhao, Chunsheng; Wiedensohler, Alfred; Stratmann, Frank

    2010-05-01

    Large areas of China suffer from heavy air pollution (both gaseous and particulate) caused by strong economic growth in the last two decades. However, knowledge concerning the physical and chemical properties of the resulting aerosol particles populations, and their effects on the optical properties of the atmosphere, is still sparse. In the framework of the investigations presented here, comprehensive measurements concerning aerosol particle hygroscopicity, CCN ability, composition, and optical properties were performed. The investigations are part of the DFG-funded project HaChi (Haze in China) and are conducted in collaboration with the Peking University. A conclusive parameterization of aerosol hygroscopicity and activation data is aimed for, which will then be implemented in a meso-scale model to investigate aerosol-cloud-radiation and precipitation interactions. During two intensive measurements campaigns (March 2009 and July/ August 2009), in-situ aerosol measurements have been performed in an air-conditioned mobile laboratory next to the Wuqing Meteorological Station (39°23'8.53"N, 117°1'25.88"E), which is located between Bejing and Tijanjin and is thereby an ideal background site in a megacity region. The particle number size distribution (TDMPS), the particle optical properties (MAAP and nephelometer) and their hygroscopic properties at high RH (HH-TDMA, LACIS-mobile) were characterized as well as their cloud nucleating properties above supersaturation (DMT-CCNC). 24 h PM1 particle samples were continuously collected over the two campaigns in winter and summer using a DIGITEL high volume sampler (DHA-80). Additionally two 6h size-resolved samples (daytime and night-time) were collected each day applying an 11-stage Berner impactor. The size-selection of HH-TDMA, LACIS and the CCNC was synchronized with the Berner stages. Opening analysis of the winter campaign data showed that the HH-TDMA usually detected a hydrophobic and a hygroscopic mode, i.e., the

  12. In-Situ Measurements of Aerosol Optical and Hygroscopic Properties at the Look Rock Site during SOAS 2013

    NASA Astrophysics Data System (ADS)

    Zhang, X.; Zimmermann, K.; Bertram, T. H.; Corrigan, A. L.; Guzman, J. M.; Russell, L. M.; Budisulistiorini, S.; Li, X.; Surratt, J. D.; Hicks, W.; Bairai, S. T.; Cappa, C. D.

    2013-12-01

    One of the main goals of the Southern Oxidant and Aerosol Study (SOAS) is to characterize the climate-relevant properties of aerosols over the southeastern United States at the interface of biogenic and anthropogenic emissions. As part of the SOAS campaign, the UCD cavity ringdown/photoacoustic spectrometer was deployed to make in-situ measurements of aerosol light extinction, absorption and sub-saturated hygroscopicity at the Look Rock site (LRK) in the Great Smoky Mountains National Park, TN from June 1 to July 15, 2013. The site is influenced by substantial biogenic emissions with varying impacts from anthropogenic pollutants, allowing for direct examination of the optical and hygroscopic properties of anthropogenic-influenced biogenic secondary organic aerosols (SOA). During the experiment period, the average dry aerosol extinction (Bext), absorption (Babs) coefficients and single scattering albedo (SSA) at 532 nm were 30.3 × 16.5 Mm-1, 1.12 × 0.78 Mm-1 and 0.96 × 0.06. The Babs at 532 nm was well correlated (r2 = 0.79) with the refractory black carbon (rBC) number concentration determined by a single particle soot spectrometer (SP2). The absorption by black carbon (BC), brown carbon (BrC) and the absorption enhancement due to the 'lensing' effect were quantified by comparing the Babs of ambient and thermo-denuded aerosols at 405 nm and 532 nm. The optical sub-saturated hygroscopic growth factor was derived from extinction and particle size distribution measurements at dry and elevated relative humidity. In addition, to explore the extent to which ammonia mediated chemistry leads to BrC formation, as suggested in recent laboratory studies(1,2), we performed an NH3 perturbation experiment in-situ for 1 week during the study, in which ambient aerosols were exposed to approximately 100 ppb NH3 with a residence time of ~ 3hr. The broader implications of these observational data at LRK will be discussed in the context of the concurrent gas and aerosol chemical

  13. Hygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: implications for regional direct radiative forcing under clean and polluted conditions

    NASA Astrophysics Data System (ADS)

    Stock, M.; Cheng, Y. F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.

    2011-05-01

    This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70-80 %, up to 50-70 % of the calculated visibility reduction was

  14. Hygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: implications for regional direct radiative forcing under clean and polluted conditions

    NASA Astrophysics Data System (ADS)

    Stock, M.; Cheng, Y. F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.

    2010-11-01

    This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer - Aerodynamic Particle Sizer (H-DMA-APS). Like in several studies before, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The hygroscopic particle growth factors at 90% RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. All data recorded between 12 August and 20 October, 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp ≥ 150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in more continentally influenced air masses. Particle size distributions and hygroscopic growth factors were employed to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its daytime values around 70-80% in summer, up to 50-70% of the calculated visibility

  15. The hygroscopicity of indoor aerosol particles

    SciTech Connect

    Wei, L.

    1993-07-01

    A system to study the hygroscopic growth of particle was developed by combining a Tandem Differential Mobility Analyzer (TDMA) with a wetted wall reactor. This system is capable of mimicking the conditions in human respiratory tract, and measuring the particle size change due to the hygroscopic growth. The performance of the system was tested with three kinds of particles of known composition, NaCl, (NH{sub 4}){sub 2}SO{sub 4}, and (NH{sub 4})HS0{sub 4} particles. The hygroscopicity of a variety of common indoor aerosol particles was studied including combustion aerosols (cigarette smoking, cooking, incenses and candles) and consumer spray products such as glass cleaner, general purpose cleaner, hair spray, furniture polish spray, disinfectant, and insect killer. Experiments indicate that most of the indoor aerosols show some hygroscopic growth and only a few materials do not. The magnitude of hygroscopic growth ranges from 20% to 300% depending on the particle size and fraction of water soluble components.

  16. Hygroscopic Characteristics of Alkylaminium Carboxylate Aerosols.

    PubMed

    Gomez-Hernandez, Mario; McKeown, Megan; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Lavi, Avi; Rudich, Yinon; Collins, Don R; Zhang, Renyi

    2016-03-01

    The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity for a series of alkylaminium carboxylate aerosols have been measured using a hygroscopicity tandem differential mobility analyzer coupled to a condensation particle counter and a CCN counter. The particles, consisting of the mixtures of mono- (acetic, propanoic, p-toluic, and cis-pinonic acid) and dicarboxylic (oxalic, succinic, malic, adipic, and azelaic acid) acid with alkylamine (mono-, di-, and trimethylamines), represent those commonly found under diverse environmental conditions. The hygroscopicity parameter (κ) of the alkylaminium carboxylate aerosols was derived from the HGF and CCN results and theoretically calculated. The HGF at 90% RH is in the range of 1.3 to 1.8 for alkylaminium monocarboxylates and 1.1 to 2.2 for alkylaminium dicarboxylates, dependent on the molecular functionality (i.e., the carboxylic or OH functional group in organic acids and methyl substitution in alkylamines). The κ value for all alkylaminium carboxylates is in the range of 0.06-1.37 derived from the HGF measurements at 90% RH, 0.05-0.49 derived from the CCN measurements, and 0.22-0.66 theoretically calculated. The measured hygroscopicity of the alkylaminium carboxylates increases with decreasing acid to base ratio. The deliquescence point is apparent for several of the alkylaminium dicarboxylates but not for the alkylaminium monocarboxylates. Our results reveal that alkylaminium carboxylate aerosols exhibit distinct hygroscopic and deliquescent characteristics that are dependent on their molecular functionality, hence regulating their impacts on human health, air quality, and direct and indirect radiative forcing on climate. PMID:26794419

  17. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    NASA Astrophysics Data System (ADS)

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-03-01

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ∼34% in the accumulation vs. ∼47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ∼70%, while efflorescence occurred at different humidities, i.e., at ∼35% RH for submicron particles vs. ∼50% RH for supermicron particles. This ∼15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ∼0.15 for

  18. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    DOE PAGES

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J. -D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; et al

    2015-03-16

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water solublemore » fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the

  19. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    NASA Astrophysics Data System (ADS)

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-08-01

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws

  20. Vertical profiles of cloud condensation nuclei, aerosol hygroscopicity, water uptake, and scattering across the United States

    NASA Astrophysics Data System (ADS)

    Lin, J. J.; Bougiatioti, A.; Nenes, A.; Anderson, B. E.; Beyersdorf, A. J.; Brock, C. A.; Gordon, T. D.; Lack, D.; Law, D. C.; Liao, J.; Middlebrook, A. M.; Richardson, M.; Thornhill, K. L., II; Winstead, E.; Wagner, N. L.; Welti, A.; Ziemba, L. D.

    2014-12-01

    The evolutions of vertical distributions of aerosol chemical, microphysical, hygroscopic, and optical properties present fundamental challenges to the understanding of ground-level air quality and radiative transfer, and few datasets exist to date for evaluation of atmospheric models. Data collected from recent NASA and NOAA field campaigns in the California Central Valley (DISCOVER-AQ), southeast United States (SENEX, SEAC4RS) and Texas (DISCOVER-AQ) allow for a unique opportunity to constrain vertical profiles of climate-relevant aerosol properties. This work presents in-situ aircraft measurements of cloud condensation nuclei (CCN) concentration and derivations of aerosol hygroscopicity, water uptake, and light scattering. Aerosol hygroscopicity is derived from CCN and aerosol measurements. Inorganic water uptake is calculated from aerosol composition using ISORROPIA, a chemical thermodynamic model, while organic water uptake is calculated from organic hygroscopicity. Aerosol scattering closure is performed between scattering from water uptake calculations and in-situ scattering measurements.

  1. Hygroscopic growth of urban aerosol particles during the 2009 Mirage-Shanghai Campaign

    NASA Astrophysics Data System (ADS)

    Ye, Xingnan; Tang, Chen; Yin, Zi; Chen, Jianmin; Ma, Zhen; Kong, Lingdong; Yang, Xin; Gao, Wei; Geng, Fuhai

    2013-01-01

    The hygroscopic properties of submicrometer urban aerosol particles were studied during the 2009 Mirage-Shanghai Campaign. The urban aerosols were composed of more-hygroscopic and nearly-hydrophobic particles, together with a trace of less-hygroscopic particles. The mean hygroscopicity parameter κ of the more-hygroscopic mode varied in the range of 0.27-0.39 depending on particle size. The relative abundance of the more-hygroscopic particles at any size was ca. 70%, slightly increasing with particle size. The number fraction of the nearly-hydrophobic particles fluctuated between 0.1 and 0.4 daily, in accordance with traffic emissions and atmospheric diffusion. The results from relative humidity dependence on hygroscopic growth and chemical analysis of fine particles indicated that particulate nitrate formation through the homogenous gas-phase reaction was suppressed under ammonia-deficient atmosphere in summer whereas the equilibrium was broken by more available NH3 during adverse meteorological conditions.

  2. Water Uptake and Hygroscopic Growth of Organosulfate Aerosol.

    PubMed

    Estillore, Armando D; Hettiyadura, Anusha P S; Qin, Zhen; Leckrone, Erin; Wombacher, Becky; Humphry, Tim; Stone, Elizabeth A; Grassian, Vicki H

    2016-04-19

    Organosulfates (OS) are important components of secondary organic aerosol (SOA) that have been identified in numerous field studies. This class of compounds within SOA can potentially affect aerosol physicochemical properties such as hygroscopicity because of their polar and hydrophilic nature as well as their low volatility. Currently, there is a dearth of information on how aerosol particles that contain OS interact with water vapor in the atmosphere. Herein we report a laboratory investigation on the hygroscopic properties of a structurally diverse set of OS salts at varying relative humidity (RH) using a Hygroscopicity-Tandem Differential Mobility Analyzer (H-TDMA). The OS studied include the potassium salts of glycolic acid sulfate, hydroxyacetone sulfate, 4-hydroxy-2,3-epoxybutane sulfate, and 2-butenediol sulfate and the sodium salts of benzyl sulfate, methyl sulfate, ethyl sulfate, and propyl sulfate. In addition, mixtures of OS and sodium chloride were also studied. The results showed gradual deliquescence of these aerosol particles characterized by continuous uptake and evaporation of water in both hydration and dehydration processes for the OS, while the mixture showed prompt deliquescence and effloresce transitions, albeit at a lower relative humidity relative to pure sodium chloride. Hygroscopic growth of these OS at 85% RH were also fit to parameterized functional forms. This new information provided here has important implications about the atmospheric lifetime, light scattering properties, and the role of OS in cloud formation. Moreover, results of these studies can ultimately serve as a basis for the development and evaluation of thermodynamic models for these compounds in order to consider their impact on the atmosphere. PMID:26967467

  3. Hygroscopic properties of large aerosol particles using the example of aged Saharan mineral dust - a semi-automated electron microscopy approach

    NASA Astrophysics Data System (ADS)

    Hartmann, Markus; Heim, Lars-Oliver; Ebert, Martin; Weinbruch, Stephan; Kandler, Konrad

    2015-04-01

    Hygroscopic properties of large aerosol particles using the example of aged Saharan mineral dust - a semi-automated electron microscopy approach Markus Hartmann(1), Lars-Oliver Heim(2), Martin Ebert(1), Stephan Weinbruch(1), Konrad Kandler(1) The Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) took place at Barbados from June 10 to July 15 2013. During this period, dust was frequently transported from Africa across the Atlantic Ocean toward the Caribbean. In this study, we investigate the atmospheric aging of the dust aerosol based on its hygroscopicity. Aerosol samples were collected ground-based at Ragged Point (13°9'54.4"N, 59°25'55.7"W) with a single round jet cascade impactor on nickel-substrates. The particles from the stage with a 50% efficiency cutoff size of 1 µm were analyzed with an Environmental Scanning Electron Microscope (ESEM) equipped with an energy-dispersive X-ray detector (EDX) and a cooling stage. In an initial automated run, information on particle size and chemical composition for elements heavier than carbon were gathered. Afterwards, electron microscope images of the same sample areas as before were taken during a stepwise increase of relative humidities (between 50 % and 92%), so that the hygroscopic growth of the droplets could be directly observed. The observed hygroscopic growth can be correlated to the chemical composition of the respective particles. For the automated analysis of several hundred images of droplets an image processing algorithm in Python was developed. The algorithm is based on histogram equalization and watershed segmentation. Since SEM images can only deliver two-dimensional information, but the hygroscopic growth factor usually refers to the volume of a drop, Atomic Force Microscopy (AFM) was used to derive an empirical function for the drop volume depending on the apparent drop diameter in the electron images. Aside from the mineral dust, composed of mostly silicates and

  4. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    SciTech Connect

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J. -D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-03-16

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode.

    The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments.

    The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was

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

    NASA Astrophysics Data System (ADS)

    Jing, Bo; Tong, Shengrui; Liu, Qifan; Li, Kun; Wang, Weigang; Zhang, Yunhong; Ge, Maofa

    2016-03-01

    Water-soluble organic compounds (WSOCs) are important components of organics in the atmospheric fine particulate matter. Although WSOCs play an important role in the hygroscopicity of aerosols, knowledge on the water uptake behavior of internally mixed WSOC aerosols remains limited. Here, the hygroscopic properties of single components such as levoglucosan, oxalic acid, malonic acid, succinic acid, phthalic acid, and multicomponent WSOC aerosols mainly involving oxalic acid are investigated with the hygroscopicity tandem differential mobility analyzer (HTDMA). The coexisting hygroscopic species including levoglucosan, malonic acid, and phthalic acid have a strong influence on the hygroscopic growth and phase behavior of oxalic acid, even suppressing its crystallization completely during the drying process. The phase behaviors of oxalic acid/levoglucosan mixed particles are confirmed by infrared spectra. The discrepancies between measured growth factors and predictions from Extended Aerosol Inorganics Model (E-AIM) with the Universal Quasi-Chemical Functional Group Activity Coefficient (UNIFAC) method and Zdanovskii-Stokes-Robinson (ZSR) approach increase at medium and high relative humidity (RH) assuming oxalic acid in a crystalline solid state. For the internal mixture of oxalic acid with levoglucosan or succinic acid, there is enhanced water uptake at high RH compared to the model predictions based on reasonable oxalic acid phase assumption. Organic mixture has more complex effects on the hygroscopicity of ammonium sulfate than single species. Although hygroscopic species such as levoglucosan account for a small fraction in the multicomponent aerosols, they may still strongly influence the hygroscopic behavior of ammonium sulfate by changing the phase state of oxalic acid which plays the role of "intermediate" species. Considering the abundance of oxalic acid in the atmospheric aerosols, its mixtures with hygroscopic species may significantly promote water uptake

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

    NASA Astrophysics Data System (ADS)

    Jing, B.; Tong, S. R.; Liu, Q. F.; Li, K.; Wang, W. G.; Zhang, Y. H.; Ge, M. F.

    2015-08-01

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

  7. Relating the hygroscopic properties of submicron aerosol to both gas- and particle-phase chemical composition in a boreal forest environment

    NASA Astrophysics Data System (ADS)

    Hong, J.; Kim, J.; Nieminen, T.; Duplissy, J.; Ehn, M.; Äijälä, M.; Hao, L. Q.; Nie, W.; Sarnela, N.; Prisle, N. L.; Kulmala, M.; Virtanen, A.; Petäjä, T.; Kerminen, V.-M.

    2015-10-01

    Measurements of the hygroscopicity of 15-145 nm particles in a boreal forest environment were conducted using two Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) systems during the Pan-European Gas-Aerosols-climate interaction Study (PEGASOS) campaign in spring 2013. Measurements of the chemical composition of non-size segregated particles were also performed using a high-resolution aerosol mass spectrometer (HR-AMS) in parallel with hygroscopicity measurements. On average, the hygroscopic growth factor (HGF) of particles was observed to increase from the morning until afternoon. In case of accumulation mode particles, the main reasons for this behavior were increases in the ratio of sulfate to organic matter and oxidation level (O : C ratio) of the organic matter in the particle phase. Using an O : C dependent hygroscopic growth factor of organic matter (HGForg), fitted using the inverse Zdanovskii-Stokes-Robinson (ZSR) mixing rule, clearly improved the agreement between measured HGF and that predicted based on HR-AMS composition data. Besides organic oxidation level, the influence of inorganic species was tested when using the ZSR mixing rule to estimate the hygroscopic growth factor of organics in the aerosols. While accumulation and Aitken mode particles were predicted fairly well by the bulk aerosol composition data, the hygroscopicity of nucleation mode particles showed little correlation. However, we observed them to be more sensitive to the gas phase concentration of condensable vapors: the more sulfuric acid in the gas phase, the more hygroscopic the nucleation mode particles were. No clear dependence was found between the extremely low-volatility organics concentration (ELVOC) and the HGF of particles of any size.

  8. Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

    NASA Astrophysics Data System (ADS)

    Denjean, C.; Formenti, P.; Picquet-Varrault, B.; Pangui, E.; Zapf, P.; Katrib, Y.; Giorio, C.; Tapparo, A.; Monod, A.; Temime-Roussel, B.; Decorse, P.; Mangeney, C.; Doussin, J. F.

    2015-03-01

    Secondary organic aerosol (SOA) were generated from the ozonolysis of α-pinene in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber. The SOA formation and aging were studied by following their optical, hygroscopic and chemical properties. The optical properties were investigated by determining the particle complex refractive index (CRI). The hygroscopicity was quantified by measuring the effect of relative humidity (RH) on the particle size (size growth factor, GF) and on the scattering coefficient (scattering growth factor, f(RH)). The oxygen to carbon atomic ratios (O : C) of the particle surface and bulk were used as a sensitive parameter to correlate the changes in hygroscopic and optical properties of the SOA composition during their formation and aging in CESAM. The real CRI at 525 nm wavelength decreased from 1.43-1.60 (±0.02) to 1.32-1.38 (±0.02) during the SOA formation. The decrease in the real CRI correlated to the O : C decrease from 0.68 (±0.20) to 0.55 (±0.16). In contrast, the GF remained roughly constant over the reaction time, with values of 1.02-1.07 (±0.02) at 90% (±4.2%) RH. Simultaneous measurements of O : C of the particle surface revealed that the SOA was not composed of a homogeneous mixture, but contained less oxidised species at the surface which may limit water absorption. In addition, an apparent change in both mobility diameter and scattering coefficient with increasing RH from 0 to 30% was observed for SOA after 14 h of reaction. We postulate that this change could be due to a change in the viscosity of the SOA from a predominantly glassy state to a predominantly liquid state.

  9. Relating the hygroscopic properties of submicron aerosol to both gas- and particle-phase chemical composition in a boreal forest environment

    NASA Astrophysics Data System (ADS)

    Hong, J.; Kim, J.; Nieminen, T.; Duplissy, J.; Ehn, M.; Äijälä, M.; Hao, L.; Nie, W.; Sarnela, N.; Prisle, N. L.; Kulmala, M.; Virtanen, A.; Petäjä, T.; Kerminen, V.-M.

    2015-06-01

    Measurements of the hygroscopicity of 15-145 nm particles in a boreal forest environment were conducted using two Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) systems during the Pan-European Gas-AeroSOIs-climate interaction Study (PEGASOS) campaign in spring 2013. Measurements of the chemical composition of non-size segregated particles were also performed using a High-Resolution Aerosol Mass Spectrometer (HR-AMS) in parallel with hygroscopicity measurements. On average, the hygroscopic growth factor (HGF) of particles was observed to increase from the morning until afternoon. In case of accumulation mode particles, the main reasons for this behavior were increases in the ratio of sulfate to organic matter and oxidation level (O : C ratio) of the organic matter in the particle phase. Using an O : C dependent hygroscopic growth factor of organic matter (HGForg), fitted using the inverse Zdanovskii-Stokes-Robinson (ZSR) mixing rule, clearly improved the agreement between measured HGF and that predicted based on HR-AMS composition data. Besides organic oxidation level, the influence of inorganic species was tested when using the ZSR mixing rule to estimate the hygroscopic growth factor of organics in the aerosols. While accumulation and Aitken mode particles were predicted fairly well by the bulk aerosol composition data, the hygroscopicity of nucleation mode particles showed little correlation. However, we observed them to be more sensitive to the gas phase concentration of condensable vapors: the more there was sulfuric acid in the gas phase, the more hygroscopic the nucleation mode particles were. No clear dependence was found between the extremely low-volatility organics (ELVOCs) concentration and the HGF of particles of any size.

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

    NASA Astrophysics Data System (ADS)

    Hasenkopf, Christa A.

    2011-08-01

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

  11. Comparison of aerosol hygroscopicity and mixing state between winter and summer seasons in Pearl River Delta region, China

    NASA Astrophysics Data System (ADS)

    Jiang, Rongxin; Tan, Haobo; Tang, Lili; Cai, Mingfu; Yin, Yan; Li, Fei; Liu, Li; Xu, Hanbing; Chan, P. W.; Deng, Xuejiao; Wu, Dui

    2016-03-01

    Hygroscopic properties of aerosol particles are important for determining aerosol size distributions, and thus determining scattering and absorption coefficients at ambient atmospheric conditions. In this study, hygroscopic properties of aerosol particles at an urban site in Guangzhou, China, were measured using a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) system during the winter and the summer. The results show that the urban aerosols were composed of more-hygroscopic, less-hygroscopic and non-hygroscopic particles. For less-hygroscopic particles of 40-200 nm in diameter, the hygroscopic parameter κLH was around 0.15. For more-hygroscopic particles, the κMH was from 0.290 to 0.339 with a particle size from 40 to 200 nm. For non-hygroscopic particles, the κNH was about 0.015. It was found that the number fraction of less-hygroscopic particles (NFLH) was correlated with the atmospheric oxidation which can be presented by OC/EC. This paper attributed the larger NFLH in winter to the higher value of OC/EC (3.0). Such conditions may lead to more formation of less-hygroscopic particles. Backward trajectories cluster analysis shows that there is a certain link between air mass origin and aerosol hygroscopicity, but it seems to be independent of the level of pollution. The difference of NFNH indicates that the mixing state of aerosol particles can also be affected by air mass origin. Diurnal variations in aerosol hygroscopic parameters in both seasons show that during daytime, aerosol particles tend to have a low degree of external mixing or quasi-internal mixing, resulting in a higher NFMH and a larger κmean; during nighttime and early mornings, they tend to be mixed externally, resulting in a lower NFMH and a smaller κmean. This can be attributed to atmospheric aging effect and evolution of mixing layer height and implies that soot (non-hygroscopic) particles present to a large extent as internal mixtures by the time they leave the urban

  12. Aqueous Phase Photo-Oxidation of Succinic Acid: Changes in Hygroscopic Properties and Reaction Products

    NASA Astrophysics Data System (ADS)

    Hudson, P. K.; Ninokawa, A.; Hofstra, J.; de Lijser, P.

    2013-12-01

    Atmospheric aerosol particles have been identified as important factors in understanding climate change. The extent to which aerosols affect climate is determined, in part, by hygroscopic properties which can change as a result of atmospheric processing. Dicarboxylic acids, components of atmospheric aerosol, have a wide range of hygroscopic properties and can undergo oxidation and photolysis reactions in the atmosphere. In this study, the hygroscopic properties of succinic acid aerosol, a non-hygroscopic four carbon dicarboxylic acid, were measured with a humidified tandem differential mobility analyzer (HTDMA) and compared to reaction products resulting from the aqueous phase photo-oxidation reaction of hydrogen peroxide and succinic acid. Reaction products were determined and quantified using gas chromatography-flame ionization detection (GC-FID) and GC-mass spectrometry (GC-MS) as a function of hydrogen peroxide:succinic acid concentration ratio and photolysis time. Although reaction products include larger non-hygroscopic dicarboxylic acids (e.g. adipic acid) and smaller hygroscopic dicarboxylic acids (e.g. malonic and oxalic acids), comparison of hygroscopic growth curves to Zdanovskii-Stokes-Robinson (ZSR) predictions suggests that the hygroscopic properties of many of the product mixtures are largely independent of the hygroscopicity of the individual components. This study provides a framework for future investigations to fully understand and predict the role of chemical reactions in altering atmospheric conditions that affect climate.

  13. In-cloud measurements highlight the role of aerosol hygroscopicity in cloud droplet formation

    NASA Astrophysics Data System (ADS)

    Väisänen, Olli; Ruuskanen, Antti; Ylisirniö, Arttu; Miettinen, Pasi; Portin, Harri; Hao, Liqing; Leskinen, Ari; Komppula, Mika; Romakkaniemi, Sami; Lehtinen, Kari E. J.; Virtanen, Annele

    2016-08-01

    The relationship between aerosol hygroscopicity and cloud droplet activation was studied at the Puijo measurement station in Kuopio, Finland, during the autumn 2014. The hygroscopic growth of 80, 120 and 150 nm particles was measured at 90 % relative humidity with a hygroscopic tandem differential mobility analyzer. Typically, the growth factor (GF) distributions appeared bimodal with clearly distinguishable peaks around 1.0-1.1 and 1.4-1.6. However, the relative contribution of the two modes appeared highly variable reflecting the probable presence of fresh anthropogenic particle emissions. The hygroscopicity-dependent activation properties were estimated in a case study comprising four separate cloud events with varying characteristics. At 120 and 150 nm, the activation efficiencies within the low- and high-GF modes varied between 0-34 and 57-83 %, respectively, indicating that the less hygroscopic particles remained mostly non-activated, whereas the more hygroscopic mode was predominantly scavenged into cloud droplets. By modifying the measured GF distributions, it was estimated how the cloud droplet concentrations would change if all the particles belonged to the more hygroscopic group. According to κ-Köhler simulations, the cloud droplet concentrations increased up to 70 % when the possible feedback effects on effective peak supersaturation (between 0.16 and 0.29 %) were assumed negligible. This is an indirect but clear illustration of the sensitivity of cloud formation to aerosol chemical composition.

  14. Application of Aerosol Hygroscopicity Measured at the Atmospheric Radiation Measurement Program's Southern Great Plains Site to Examine Composition and Evolution

    NASA Technical Reports Server (NTRS)

    Gasparini, Roberto; Runjun, Li; Collins, Don R.; Ferrare, Richard A.; Brackett, Vincent G.

    2006-01-01

    A Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) was used to measure submicron aerosol size distributions, hygroscopicity, and occasionally volatility during the May 2003 Aerosol Intensive Operational Period (IOP) at the Central Facility of the Atmospheric Radiation Measurement Program's Southern Great Plains (ARM SGP) site. Hygroscopic growth factor distributions for particles at eight dry diameters ranging from 0.012 micrometers to 0.600 micrometers were measured throughout the study. For a subset of particle sizes, more detailed measurements were occasionally made in which the relative humidity or temperature to which the aerosol was exposed was varied over a wide range. These measurements, in conjunction with backtrajectory clustering, were used to infer aerosol composition and to gain insight into the processes responsible for evolution. The hygroscopic growth of both the smallest and largest particles analyzed was typically less than that of particles with dry diameters of about 0.100 micrometers. It is speculated that condensation of secondary organic aerosol on nucleation mode particles is largely responsible for the minimal hygroscopic growth observed at the smallest sizes considered. Growth factor distributions of the largest particles characterized typically contained a nonhygroscopic mode believed to be composed primarily of dust. A model was developed to characterize the hygroscopic properties of particles within a size distribution mode through analysis of the fixed size hygroscopic growth measurements. The performance of this model was quantified through comparison of the measured fixed size hygroscopic growth factor distributions with those simulated through convolution of the size-resolved concentration contributed by each of the size modes and the mode-resolved hygroscopicity. This transformation from sizeresolved hygroscopicity to mode-resolved hygroscopicity facilitated examination of changes in the hygroscopic

  15. Relationship between volatility, hygroscopicity, and CCN activity of winter aerosols: Kanpur, Indo-Gangetic Basin

    NASA Astrophysics Data System (ADS)

    Bhattu, Deepika; Tripathi, Sachchida

    2016-04-01

    Aerosol volatility is one of the key property in deciding their lifetime and fate. The volatile species have the potential to affect SOA estimation, so their characterization and establishment of relationship with mass loading, chemical composition, hygroscopicity and CCN activity is required. A 42 days long winter campaign was conducted in an anthropogenically polluted location (Kanpur, India) where CCN activity of both ambient and thermally treated aerosols was characterized. Enhanced partitioning of semi-volatile molecules into particle phase at higher loading conditions was observed. Unexpectedly, the most oxidized organic factor was observed both least volatile and hygroscopic in nature. Lower

  16. Measurements of Hygroscopicity- and Size-Resolved Sea Spray Aerosol

    NASA Astrophysics Data System (ADS)

    Phillips, B.; Dawson, K. W.; Royalty, T. M.; Reed, R. E.; Petters, M.; Meskhidze, N.

    2015-12-01

    Atmospheric aerosols play a central role in many environmental processes by influencing the Earth's radiative balance, tropospheric chemistry, clouds, biogeochemical cycles, and visibility as well as adversely impacting human health. Based on their origin, atmospheric aerosols can be defined as anthropogenic or natural. Recent studies have shown that a large fraction of uncertainty in the radiative effects of anthropogenic aerosols is related to uncertainty in natural—background—aerosols. Marine aerosols are of particular interest due to the abundance of oceans covering the Earth's surface. Despite their importance, limited information is currently available for size- and composition-resolved marine aerosol emission fluxes. Our group has designed and built an instrument for measuring the size- and hygroscopicity-resolved sea spray aerosol fluxes. The instrument was first deployed during spring 2015 at the end of the 560 m pier of the US Army Corps of Engineers' Field Research Facility in Duck, NC. Measurements include 200 nm-sized diameter growth factor (hygroscopicity) distributions, sea spray particle flux measurements, and total sub-micron sized aerosol concentration. Ancillary ocean data includes salinity, pH, sea surface temperature, dissolved oxygen content, and relative fluorescence (proxy for [Chl-a]). Hygroscopicity distribution measurements show two broad peaks, one indicative of organics and sulfates and another suggestive of sea salt. The fraction of 200 nm-sized salt particles having hygroscopicity similar to that of sea-spray aerosol contributes up to ~24% of the distribution on days with high-speed onshore winds and up to ~3% on calm days with winds blowing from the continent. However, the total concentration of sea-spray-like particles originating from offshore versus onshore winds was relatively similar. Changes in the relative contribution of sea-salt to number concentration were caused by a concomitant changes in total aerosol concentration

  17. Aerosol hygroscopicity and cloud droplet activation of extracts of filters from biomass burning experiments

    NASA Astrophysics Data System (ADS)

    Carrico, Christian M.; Petters, Markus D.; Kreidenweis, Sonia M.; Collett, Jeffrey L.; Engling, Guenter; Malm, William C.

    2008-04-01

    In this laboratory closure study, we compare sub- and supersaturated water uptake properties for aerosol particles possessing a range of hygroscopicity. Measurements for water sub-saturated conditions used a hygroscopic tandem differential mobility analyzer (HTDMA). Simultaneously, measurements of particle critical supersaturation were conducted on the same sample stream with a continuous flow cloud condensation nuclei (CCN) counter. For these experiments, we used filter-collected samples of biomass smoke generated in the combustion of two common wildland fire fuels, western sagebrush and Alaskan duff core. Extractions of separate sections of the filter were performed using two solvents, ultrapure water and methanol. The extracts were subsequently atomized, producing aerosols having a range of hygroscopic responses. HTDMA and CCN measurements were fit to a single-parameter model of water uptake, in which the fit parameter is denoted κ, the hygroscopicity parameter. Here, for the four extracts we observed mean values of the hygroscopicity parameter of 0.06 < κ < 0.30, similar to the range found previously for numerous pure organic compounds. Particles generated from the aqueous extracts of the filters had consistently larger κ than methanol extracts, while western sagebrush extract aerosols κ exceeded those from Alaskan duff core. HTDMA- and CCN-derived values of κ for each experiment agreed within approximately 20%. Applicability of the κ-parameterization to other multicomponent aerosols relevant to the atmosphere remains to be tested.

  18. Hygroscopic Behavior of Multicomponent Aerosols Involving NaCl and Dicarboxylic Acids.

    PubMed

    Peng, Chao; Jing, Bo; Guo, Yu-Cong; Zhang, Yun-Hong; Ge, Mao-Fa

    2016-02-25

    Atmospheric aerosols are usually complex mixtures of inorganic and organic compounds. The hygroscopicity of mixed particles is closely related to their chemical composition and interactions between components, which is still poorly understood. In this study, the hygroscopic properties of submicron particles composed of NaCl and dicarboxylic acids including oxalic acid (OA), malonic acid (MA), and succinic acid (SA) with various mass ratios are investigated with a hygroscopicity tandem differential mobility analyzer (HTDMA) system. Both the Zdanovskii-Stokes-Robinson (ZSR) method and extended aerosol inorganics model (E-AIM) are applied to predict the water uptake behaviors of sodium chloride/dicarboxylic acid mixtures. For NaCl/OA mixed particles, the measured growth factors were significantly lower than predictions from the model methods, indicating a change in particle composition caused by chloride depletion. The hygroscopic growth of NaCl/MA particles was well described by E-AIM, and that of NaCl/SA particles was dependent upon mixing ratio. Compared with model predictions, it was determined that water uptake of the NaCl/OA mixture could be enhanced and could be closer to the predictions by addition of levoglucosan or malonic acid, which retained water even at low relative humidity (RH), leading to inhibition of HCl evaporation during dehydration. These results demonstrate that the coexisting hygroscopic species have a strong influence on the phase state of particles, thus affecting chemical interactions between inorganic and organic compounds as well as the overall hygroscopicity of mixed particles. PMID:26820230

  19. Relating hygroscopicity and composition of organic aerosol particulate matter

    SciTech Connect

    Duplissy, J.; DeCarlo, P. F.; Dommen, J.; Alfarra, M. R.; Metzger, A.; Barmpadimos, I.; Prevot, A. S. H.; Weingartner, E.; Tritscher, T.; Gysel, M.; Aiken, A. C.; Jimenez, J. L.; Canagaratna, M. R.; Worsnop, D. R.; Collins, D. R.; Tomlinson, J.; Baltensperger, U.

    2011-01-01

    A hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopicity) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS), and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f44). m/z 44 is due mostly to the ion fragment CO2+ for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfraujoch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation between the hygroscopicity of OA at subsaturated RH, as given by the hygroscopic growth factor (GF) or "κorg" parameter, and f44 was determined and is given by κorg = 2.2 × f44 - 0.13. This approximation can be further verified and refined as the database for AMS and HTDMA measurements is constantly being expanded around the world. Finally, the use of this approximation could introduce an important simplification in the parameterization of hygroscopicity of OA in atmospheric models, since f44 is correlated with the photochemical age of an air mass.

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

    PubMed

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

    2015-08-01

    A novel approach based on a combination of a pulse RH controlling system and a rapid scan vacuum FTIR spectrometer (PRHCS-RSVFTIR) was utilized to investigate dynamic hygroscopicity of two atmospheric aerosols: ammonium sulfate ((NH4)2SO4) and magnesium sulfate (MgSO4). In this approach, rapid-scan infrared spectra of water vapor and aerosols were obtained to determine relative humidity (RH) in sample cell and hygroscopic property of aerosols with a subsecond time resolution. Heterogeneous nucleation rates of (NH4)2SO4 were, for the first time, measured under low RH conditions (<35% RH). In addition, studies of MgSO4 aerosols revealed that water mass transport may be limited by different processes depending on RH values (surface limited at 40% < RH < 52% and bulk phase limited at RH < 40%). Furthermore, we are also the first to report water diffusion constants in micron size MgSO4 aerosols at very low RH values. Our results have shown that the PRHCS-RSVFTIR is well-suited for determination of hygroscopicity of atmospheric aerosols and water transport and nucleation kinetics of liquid aerosols.

  1. The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol

    PubMed Central

    2015-01-01

    Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle–particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle–particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate. PMID:27162963

  2. The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

    PubMed

    Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

    2015-06-24

    Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

  3. The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

    PubMed

    Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

    2015-06-24

    Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate. PMID:27162963

  4. Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

    DOE PAGES

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2015-04-17

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined heremore » as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1–0.15 and 0.9–1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.« less

  5. Control over hygroscopic growth of saline aqueous aerosol using Pluronic polymer additives.

    PubMed

    Haddrell, Allen E; Hargreaves, Graham; Davies, James F; Reid, Jonathan P

    2013-02-25

    The hygroscopic properties of an aerosol originating from a nebulizer solution can affect the extent of peripheral deposition within the respiratory tract, which in turn affects drug efficacy of drugs delivered to the lungs. Thus, the ability to tailor the degree and rate of hygroscopic growth of an aerosol produced by a nebulizer through modification of the formulation would serve to improve drug efficacy through targeted lung deposition. In this study, the kinetic and thermodynamic hygroscopic properties of sodium chloride aerosol mixed with commercially available Pluronic polymers, specifically F77 and F127, are reported using three complementary single aerosol analysis techniques, specifically aerosol optical tweezers, a double ring electrodynamic balance and a concentric cylinder electrodynamic balance. The F77 polymer is shown to have a predictable effect on the hygroscopic properties of the aerosol: the ability of the droplet to uptake water from the air depends on the solute weight percent of sodium chloride present in a linear dose dependant manner. Unlike the smaller F77, a non-linear relationship was observed for the larger molecular weight F127 polymer, with significant suppression of hygroscopic growth (>50% by mass) for solution aerosol containing even only 1 wt% of the polymer and 99 wt% sodium chloride. The suppression of growth is shown to be consistent with the formation of mixed phase aerosol particles containing hydrophilic inorganic rich domains and hydrophobic polymer rich domains that sequester some of the inorganic component, with the two phases responding to changes in relative humidity independently. This independence of coupling with the gas phase is apparent in both the equilibrium state and the kinetics of water evaporation/condensation. By starting with a saline nebulizer solution with a concentration of F127 ∼10(-2)mM, a 12% reduction in the radius of all aerosol produced at a relative humidity (RH) of 84% is possible. The

  6. Aerosol optical hygroscopicity measurements during the 2010 CARES Campaign

    DOE PAGES

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2014-12-10

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 CARES study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GF) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles, yielding κ = 0.1–0.15 and 0.9–1.0, respectively. Themore » derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.« less

  7. Reconciling Organic Aerosol Volatility, Hygroscopicity, and Oxidation State During the Colorado DISCOVER-AQ Deployment

    NASA Astrophysics Data System (ADS)

    Hite, J. R.; Moore, R.; Martin, R.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.; Nenes, A.

    2014-12-01

    The organic fraction of submicron aerosol can profoundly impact radiative forcing on climate directly, through enhancement of extinction, or indirectly through modulation of cloud formation. Semi-volatile constituents of organic ambient aerosol are of particular interest as their partitioning between the vapor and aerosol phases is not well constrained by current atmospheric models and appears to play an important role in the formation of cloud condensation nuclei (CCN) as suggested by recent research. An experimental setup consisting of a DMT CCN counter and SMPS downstream of a custom-built thermodenuder assembly was deployed during the summer 2014 DISCOVER-AQ field campaign to retrieve simultaneous, size-resolved volatility and hygroscopicity - through the use of scanning mobility CCN analysis (SMCA). Housed in the NASA Langley mobile laboratory, a suite of complimentary measurements were made available onboard including submicron aerosol composition and oxidation state provided by an HR-ToF-AMS, and aerosol optical properties provided by a range of other instruments including an SP2. Air masses sampled from locations across the Central Colorado region include influences from regional aerosol nucleation/growth events, long-range transport of Canadian biomass burning aerosols, cattle feedlot emissions and influences of the Denver urban plume - amidst a backdrop of widespread oil and gas exploration. The analysis focuses on the reconciliation of the retrieved aerosol volatility distributions and corresponding hygroscopicity and oxidation state observations, including the use of AMS factor analysis.

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

    NASA Astrophysics Data System (ADS)

    Tang, Ignatius N.

    1996-08-01

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

  9. Marine aerosol hygroscopicity and volatility, measured on the Chatham Rise (New Zealand)

    NASA Astrophysics Data System (ADS)

    Cravigan, Luke; Mallet, Marc; Ristovski, Zoran; Vaattovaara, Petri; Talbot, Nick; Olivares, Gustavo; Harvey, Mike; Law, Cliff

    2013-05-01

    The Surface Ocean Aerosol Production (SOAP) study was undertaken in February/ March 2012 in the biologically active waters of the Chatham Rise, NZ. Aerosol hygroscopicity and volatility were examined with a volatility hygroscopicity tandem differential mobility analyser. These observations confirm results from other hygroscopicity-based studies that the dominant fraction of the observed remote marine particles were non-sea salt sulfates. Further observations are required to clarify the influences of seawater composition, meteorology and analysis techniques seasonally across different ocean basins.

  10. Hygroscopic Measurements of Aerosol Particles in Colorado during the Discover AQ Campaign 2014

    NASA Astrophysics Data System (ADS)

    Orozco, D.; Delgado, R.; Espinosa, R.; Martins, J. V.; Hoff, R. M.

    2014-12-01

    In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground observations with other optical aerosol measurements such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. In the summer of 2014, the DISCOVER-AQ campaign was held in Colorado, where systematic and concurrent observations of column- integrated surface, and vertically-resolved distributions of aerosols and trace gases relevant to air quality and their evolution during the day were observed. Aerosol optical properties were measured in the UMBC trailer at the city of Golden using a TSI-3563 nephelometer and an in-situ Polarized Imaging Nephelometer (PI-NEPH) designed and built by the LACO group at UMBC. The PI-NEPH measures aerosol phase matrix components in high angular range between 2 and 178 degrees scattering angle at three wavelengths (λ=473, 532 and 671nm). The two measured elements of the phase matrix, intensity (P11) and linear polarization (P12) provide extensive characterization of the scattering properties of the studied aerosol. The scattering coefficient, P11 and P12 were measured under different humidity conditions to obtain the enhancement factor f(RH) and the dependence of P11 and P12 to RH using a humidifier dryer system covering a RH range from 20 to 90%. The ratio between scattering coefficients at high and low humidity in Golden Colorado showed relatively low hygroscopic growth in the aerosol particles f(RH=80%) was 1.27±0.19 for the first three weeks of sampling. According to speciated measurements performed at the UMBC trailer, the predominance of dust and organic aerosols over more hygroscopic nitrate and sulfate in the

  11. Hygroscopic properties of ultrafine particles in coastal and forest environments

    NASA Astrophysics Data System (ADS)

    Hämeri, K.; Väkevä, M.

    2000-08-01

    The hygroscopic properties of recently produced ultrafine particles were measured in forestal and coastal environments using an Ultrafine Tandem Differential Mobility Analyser. The size range of the ambient aerosol particles that was investigated ranged from 8 nm to 30 nm in dry diameter. The measurements in a boreal forest site (SMEAR II station, Hyytiälä, Finland) showed that the growth factors during the days with production of ultrafine particles have a clear diurnal behavior. The minimum growth factor was ca. 1.12-1.13 and was obtained during nighttime. The maximum values were obtained between 13:00 and 16:00. The median values for the maximum growth factor for 10 nm dry diameter particles was 1.26 and for 20 nm dry size 1.28. The measurements in a coastal site (Mace Head station, Carna, Ireland) showed that the new particles produced during nucleation bursts were non- or slightly hygroscopic, with growth factor ca. 1.0-1.1 for 8 nm and 10 nm particles. The background ultrafine particles that were not connected with nucleation bursts were found to be more hygroscopic.

  12. Sensitivity of depositions to the size and hygroscopicity of Cs-bearing aerosols released from the Fukushima nuclear accident

    NASA Astrophysics Data System (ADS)

    Kajino, Mizuo; Adachi, Kouji; Sekiyama, Tsuyoshi; Zaizen, Yuji; Igarashi, Yasuhito

    2014-05-01

    We recently revealed that the microphysical properties of aerosols carrying the radioactive Cs released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) at an early stage (March 14-15, 2011) of the accident could be very different from what we assumed previously: super-micron and non-hygroscopic at the early stage, whereas sub-micron and hygroscopic afterwards (at least later than March 20-22). In the study, two sensitivity simulations with the two different aerosol microphysical properties were conducted using a regional scale meteorology- chemical transport model (NHM-Chem). The impact of the difference was quite significant. 17% (0.001%) of the radioactive Cs fell onto the ground by dry (wet) deposition processes, and the rest was deposited into the ocean or was transported out of the model domain, which is central and northern part of the main land of Japan, under the assumption that Cs-bearing aerosols are non-hygroscopic and super-micron. On the other hand, 5.7% (11.3%) fell onto the ground by dry (wet) deposition, for the cases under the assumption that the Cs-bearing aerosols are hygroscopic and sub-micron. For the accurate simulation of the deposition of radionuclides, knowledge of the aerosol microphysical properties is essential as well as the accuracy of the simulated wind fields and precipitation patterns.

  13. Hygroscopicity of internally mixed multi-component aerosol particles of atmospheric relevance

    NASA Astrophysics Data System (ADS)

    Liu, Qifan; Jing, Bo; Peng, Chao; Tong, Shengrui; Wang, Weigang; Ge, Maofa

    2016-01-01

    The hygroscopic properties of two water-soluble organic compounds (WSOCs) relevant to urban haze pollution (phthalic acid and levoglucosan) and their internally mixtures with inorganic salts (ammonium sulfate and ammonium nitrate) are investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA) system. The multi-component particles uptake water gradually in the range 5-90% relative humidity (RH). The experimental results are compared with the thermodynamic model predictions. For most mixtures, Extended Aerosol Inorganic Model (E-AIM) predictions agree well with the measured growth factors. The hygroscopic growth of mixed particles can be well described by the Zdanovskii-Stokes-Robinson (ZSR) relation as long as the mixed particles are completely liquid. ZSR calculations underestimate the water uptake of mixed particles at moderate RH due to the partial dissolution of ammonium sulfate in the organic and ammonium nitrate solution in this RH region. The phase of ammonium nitrate in the initial dry particles changes dramatically with the composition of mixtures. The presence of organics in the mixed particles can inhibit the crystallization of ammonium nitrate during the drying process and results in water uptake at low RH (RH < 60%). These results demonstrate that certain representative WSOCs can substantially influence the hygroscopicity of inorganic salts and overall water uptake of particles.

  14. The effect of low solubility organic acids on the hygroscopicity of sodium halide aerosols

    NASA Astrophysics Data System (ADS)

    Miñambres, L.; Méndez, E.; Sánchez, M. N.; Castaño, F.; Basterretxea, F. J.

    2014-10-01

    In order to accurately assess the influence of fatty acids on the hygroscopic and other physicochemical properties of sea salt aerosols, hexanoic, octanoic or lauric acid together with sodium halide salts (NaCl, NaBr and NaI) have been chosen to be investigated in this study. The hygroscopic properties of sodium halide sub-micrometre particles covered with organic acids have been examined by Fourier-transform infrared spectroscopy in an aerosol flow cell. Covered particles were generated by flowing atomized sodium halide particles (either dry or aqueous) through a heated oven containing the gaseous acid. The obtained results indicate that gaseous organic acids easily nucleate onto dry and aqueous sodium halide particles. On the other hand, scanning electron microscopy (SEM) images indicate that lauric acid coating on NaCl particles makes them to aggregate in small clusters. The hygroscopic behaviour of covered sodium halide particles in deliquescence mode shows different features with the exchange of the halide ion, whereas the organic surfactant has little effect in NaBr particles, NaCl and NaI covered particles experience appreciable shifts in their deliquescence relative humidities, with different trends observed for each of the acids studied. In efflorescence mode, the overall effect of the organic covering is to retard the loss of water in the particles. It has been observed that the presence of gaseous water in heterogeneously nucleated particles tends to displace the cover of hexanoic acid to energetically stabilize the system.

  15. The effect of low solublility organic acids on the hygroscopicity of sodium halide aerosols

    NASA Astrophysics Data System (ADS)

    Miñambres, L.; Méndez, E.; Sánchez, M. N.; Castaño, F.; Basterretxea, F. J.

    2014-02-01

    In order to accurately assess the influence of fatty acids on the hygroscopic and other physicochemical properties of sea salt aerosols, hexanoic, octanoic or lauric acid together with sodium halide salts (NaCl, NaBr and NaI) have been chosen to be performed in this study. The hygroscopic properties of sodium halide submicrometer particles covered with organic acids have been examined by Fourier-transform infrared spectroscopy in an aerosol flow cell. Covered particles were generated by flowing atomized sodium halide particles (either dry or aqueous) through a heated oven containing the gaseous acid. The obtained results indicate that gaseous organic acids easily nucleate onto dry and aqueous sodium halide particles. On the other hand, Scanning Electron Microscopy (SEM) images indicate that lauric acid coating on NaCl particles makes them to aggregate in small clusters. The hygroscopic behaviour of covered sodium halide particles in deliquescence mode shows different features with the exchange of the halide ion: whereas the organic covering has little effect in NaBr particles, NaCl and NaI covered particles change their deliquescence relative humidities, with different trends observed for each of the acids studied. In efflorescence mode, the overall effect of the organic covering is to retard the loss of water in the particles. It has been observed that the presence of gaseous water in heterogeneously nucleated particles tends to displace the cover of hexanoic acid to energetically stabilize the system.

  16. CCN, hygroscopicity, and activation kinetics of Los Angeles aerosol

    NASA Astrophysics Data System (ADS)

    Lin, J. J.; Lathem, T. L.; Nenes, A.; Suski, K.; Cahill, J. F.; Prather, K. A.; Craven, J. S.; Metcalf, A. R.; Jonsson, H. H.; Flagan, R. C.; Seinfeld, J. H.

    2010-12-01

    The CalNex field campaign was designed as a comprehensive regional air quality and climate assessment study with an emphasis on the interaction between air quality and climate change. The southern California region is an excellent location for the study of air quality and climate change due to the existence and interaction of biogenic, dust, and urban plumes. Research flights aboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter platform focused on the origin and evolution of the Los Angeles plume as it is advected across the basin and outflows into the Coachella valley and Mojave Desert. This study focuses on cloud condensation nuclei (CCN) measurements taken aboard the Twin Otter. A continuous flow streamwise thermal gradient chamber operating in scanning flow CCN analysis (SFCA) mode provided high resolution, in situ CCN spectra (0.4-0.8% supersaturation) once every 40 seconds. In conjuncture with other aerosol instrumentation aboard the Twin Otter, the data provide a comprehensive picture of the interaction of ambient aerosol with water vapor. The analysis presented then quantifies the relationship between aerosol size, chemical composition, mixing state, hygroscopicity, and activation kinetics of aerosol from the variety of sources sampled.

  17. Reformulating atmospheric aerosol thermodynamics and hygroscopic growth into fog, haze and clouds

    NASA Astrophysics Data System (ADS)

    Metzger, S.; Lelieveld, J.

    2007-06-01

    Modeling atmospheric aerosol and cloud microphysics is rather complex, even if chemical and thermodynamical equilibrium is assumed. We show, however, that the thermodynamics can be considerably simplified by reformulating equilibrium to consistently include water, and transform laboratory-based concepts to atmospheric conditions. We generalize the thermodynamic principles that explain hydration and osmosis - merely based on solute solubilities - to explicitly account for the water mass consumed by hydration. As a result, in chemical and thermodynamical equilibrium the relative humidity (RH) suffices to determine the saturation molality, including solute and solvent activities (and activity coefficients), since the water content is fixed by RH for a given aerosol concentration and type. As a consequence, gas/liquid/solid aerosol equilibrium partitioning can be solved analytically and non-iteratively. Our new concept enables an efficient and accurate calculation of the aerosol water mass and directly links the aerosol hygroscopic growth to fog, haze and cloud formation. We apply our new concept in the 3rd Equilibrium Simplified Aerosol Model (EQSAM3) for use in regional and global chemistry-transport and climate models. Its input is limited to the species' solubilities from which a newly introduced stoichiometric coefficient for water is derived. Analogously, we introduce effective stoichiometric coefficients for the solutes to account for complete or incomplete dissociation. We show that these coefficients can be assumed constant over the entire activity range and calculated for various inorganic, organic and non-electrolyte compounds, including alcohols, sugars and dissolved gases. EQSAM3 calculates the aerosol composition and gas/liquid/solid partitioning of mixed inorganic/organic multicomponent solutions and the associated water uptake for almost 100 major compounds. It explicitly accounts for particle hygroscopic growth by computing aerosol properties such as

  18. The contribution of aerosol hygroscopic growth to the modeled aerosol radiative effect

    NASA Astrophysics Data System (ADS)

    Kokkola, Harri; Kühn, Thomas; Kirkevåg, Alf; Romakkaniemi, Sami; Arola, Antti

    2016-04-01

    The hygroscopic growth of atmospheric aerosols can have a significant effect on the direct radiative effect of atmospheric aerosol. However, there are significant uncertainties concerning how much of the radiative forcing is due to different chemical compounds, especially water. For example, modeled optical depth of water in global aerosol-climate models varies by more than a factor of two. These differences can be attributed to differences in modeled 1) hygroscopicity, 2) ambient relative humidity, and/or 3) aerosol size distribution. In this study, we investigate which of these above-mentioned factors cause the largest variability in the modeled optical depth of water. In order to do this, we have developed a tool that calculates aerosol extinction using interchangeable global 3D data of aerosol composition, relative humidity, and aerosol size distribution fields. This data is obtained from models that have taken part in the open international initiative AeroCom (Aerosol Comparisons between Observations and Models). In addition, we use global 3D data for relative humidity from the Atmospheric Infrared Sounder (AIRS) flying on board NASA's Aqua satellite and the National Centers for Environmental Prediction (NCEP) reanalysis data. These observations are used to evaluate the modeled relative humidity fields. In the first stage of the study, we made a detailed investigation using the aerosol-chemistry-climate model ECHAM-HAMMOZ in which most of the aerosol optical depth is caused by water. Our results show that the model significantly overestimates the relative humidity over the oceans while over land, the overestimation is lower or it is underestimated. Since this overestimation occurs over the oceans, the water optical depth is amplified as the hygroscopic growth is very sensitive to changes in high relative humidities. Over land, error in modeled relative humidity is unlikely to cause significant errors in water optical depth as relative humidities are generally

  19. Water Activity Limits the Hygroscopic Growth Factor of Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Rodriguez, L. I.; Cabrera, J. A.; Golden, D.; Tabazadeh, A.

    2007-12-01

    In this work we study the hygroscopic behavior of organic aerosols, which has important implications for Earth's climate. The hygroscopic growth factor (HGF) is defined as the ratio of the diameter of a spherical particle when it is exposed to dry conditions to that at humid conditions. We present a new formulation to express the HGF of an aerosol particle as a function of water activity (aw) in the aqueous phase. This new formulation matches reported HGFs for common inorganic salts and water-miscible organic particles that are known to deliquesce into aqueous drops at high relative humidities (RH). Many studies use tandem differential mobility analyzers (TDMA) to determine the HGF of organic aerosols. For example, Brooks et al. used a TDMA to measure a HGF of 1.2 for 2 μm phthalic acid (PA) particles at 90% RH (aw= 0.9). However, water activity limits the growth of a particle that can be attributed to water uptake. We have assembled a vapor pressure apparatus to measure aw of aqueous solutions at room temperature. Measured water activities for PA, used in our growth formulation, yield a HGF of ~ 1.0005 for 2 μm PA particles at 90% RH. Comparing our results against Brooks et al. suggests that TDMA experiments may grossly overestimate the HGF of PA particles since water activity limits this growth to below 1.0005. Alternatively, we suggest that the adsorption of a negligible mass of water by a highly porous PA particle can lead to an apparent growth in particle size by changing its morphology. Other studies also use TDMAs to measure HGFs of secondary organic aerosols (SOAs). HGFs reported for SOAs are very similar to PA, suggesting that the observed growth may be due to morphological changes in particle size rather than water uptake as commonly assumed. We built a smog chamber where an organic precursor, such as d-limonene, reacts with nitrogen oxides under UV radiation to produce SOAs. We compare the HGFs for SOAs obtained with our method to those obtained with

  20. Airborne measurements of hygroscopicity and mixing state of aerosols in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, Bernadette; Weingartner, Ernest; Gysel, Martin; Rubach, Florian; Mentel, Thomas; Baltensperger, Urs

    2014-05-01

    Aerosols interact directly with the incident solar radiation by scattering or absorbing the light. The optical properties of an aerosol particle can strongly be altered at enhanced relative humidity (RH). Depending on the particle's chemical composition, it can experience hygroscopic growth, leading to a change in size and index of refraction compared to the dry particle (Zieger et al., 2011). Besides, aerosols can exist in different mixing states which are usually divided into internal and external mixtures. If all particles of a certain size have the same chemical composition, they are described as internally mixed, whereas if particles of equal size have different chemical composition, they are defined as externally mixed. Depending on the mixture the hygroscopic behavior will change: internally mixed aerosols will grow uniformly with increasing RH, while the different substances in external mixtures will experience different growing behaviors leading to a mode-splitting or broadened size distribution. Laboratory studies are commonly performed at dry conditions but it is known that temperature and RH as well as chemical composition are changing with altitude (Morgan et al., 2010). This further leads to the conclusion that the in-situ measurements of optical properties at different heights are crucial for climate forcing calculations. Within the Pan-European Gas-Aerosols-climate interaction Study (PEGASOS) the white- light humidified optical particle spectrometer (WHOPS) was developed and installed on the Zeppelin to investigate changes of light scattering with regard to water uptake and altitude. This instrument firstly selects a dry monodisperse aerosol by its electrical mobility and then exposes it to a well-defined RH (typically 95%). Alternately, the dry and humidified particles are measured in a white-light optical particle spectrometer (WELAS). In this way it is possible to infer the effective index of refraction of the dry particles, their hygroscopic

  1. On the Physicochemical Processes Controlling Organic Aerosol Hygroscopicity

    NASA Astrophysics Data System (ADS)

    Petters, Sarah Suda

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

  2. Cloud Condensation Nuclei Activity, Droplet Growth Kinetics and Hygroscopicity of Biogenic and Anthropogenic Secondary Organic Aerosol (SOA)

    NASA Astrophysics Data System (ADS)

    Zhao, Defeng; Buchholz, Angela; Kortner, Birthe; Schlag, Patrick; Rubach, Florian; Hendrik, Fucks; Kiendler-Scharr, Astrid; Tillmann, Ralf; Wahner, Andreas; Hallquist, Mattias; Flores, Michel; Rudich, Yinon; Glasius, Marianne; Kourtchev, Ivan; Kalberer, Markus; Mentel, Thomas

    2015-04-01

    Recent field data and model analysis show that secondary organic aerosol (SOA) formation is enhanced under anthropogenic influences (de Gouw et al. 2005, Spracklen et al. 2011). The interaction of biogenic VOCs (BVOCs) with anthropogenic emissions such as anthropogenic VOCs (AVOCs) could change the particle formation yields and the aerosol properties, as was recently demonstrated (Emanuelsson et al., 2013; Flores et al., 2014). However, the effect of the interaction of BVOCs with AVOCs on cloud condensation nuclei (CCN) activity and hygroscopicity of SOA remains elusive. Characterizing such changes is necessary in order to assess the indirect radiative forcing of biogenic aerosols that form under anthropogenic influence. In this study, we investigated the influence of AVOCs on CCN activation and hygroscopic growth of BSOA. SOA was formed from photooxidation of monoterpenes and aromatics as representatives of BVOCs and AVOCs, respectively. The hygroscopicity and CCN activation of BSOA were studied and compared with that of anthropogenic SOA (ASOA) and the mixture of ASOA and BSOA (ABSOA). We found that ASOA had a significantly higher hygroscopicity than BSOA at similar OH dose, which is attributed to a higher oxidation level of ASOA. While the ASOA fraction had an enhancing effect on the hygroscopicity of ABSOA compared to BSOA, the hygroscopicity of ABSOA cannot be explained by a linear combination of the pure ASOA and BSOA systems, indicating potentially additional non-linear effects such as oligomerization. However, in contrast to hygroscopicity, ASOA showed similar CCN activity as BSOA, in spite of its higher oxidation level. The ASOA fraction did not enhance the CCN activity of ABSOA. The discrepancy between hygroscopicity and CCN activity is discussed. In addition, BSOA, ABSOA and ASOA formed similar droplet size with ammonium sulfate in CCN at a given supersaturation, indicating none of these aerosols had a delay in the water uptake in the supersaturated

  3. Hygroscopicity of dicarbonyl-amine secondary organic aerosol products investigated with HTDMA

    NASA Astrophysics Data System (ADS)

    Hawkins, L. N.; de Haan, D. O.

    2010-12-01

    Recent studies have shown the importance of amine-dicarbonyl chemistry as a secondary organic aerosol (SOA) formation pathway, producing imines, imidazoles, and N-containing oligomers. Preliminary work in our group has suggested that some of these products may be surface active. Therefore, the presence of these products may result in important changes to submicron particle hygroscopicity that affect aerosol scattering and cloud condensation nuclei (CCN) activity, especially in regions with significant amine-containing particles. To investigate their hygroscopicity, we have designed a hygroscopicity tandem differential mobility analyzer (HTDMA) system around a 300 L Teflon chamber that allows for longer humidification times needed for some organic aerosol components that are only slightly hygroscopic. This modification provides a range of residence times from 2.5 minutes up to 1 hour, unlike previously published systems that vary from 2-30 seconds. Using the modified hygroscopicity tandem differential mobility analyzer (HTDMA), we have measured the hygroscopic growth factor (HGF) of SOA formed from reactions of glyoxal (and methylglyoxal) with methylamine, ammonium sulfate, and several amino acids. Changes to inorganic aerosol HGF in response to the presence of SOA products are also investigated.

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

    SciTech Connect

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

    2012-06-13

    to carry out reactions of representative anthropogenic and biogenic VOCs and organic particles with ozone (O3), and hydroxyl (OH), nitrate (NO3), and chlorine (Cl) radicals, which are the major atmospheric oxidants, under simulated atmospheric conditions in large-volume environmental chambers. A combination of on-line and off-line analytical techniques were used to monitor the chemical and physical properties of the particles including their hygroscopicity and CCN activity. The results of the studies were used to (1) improve scientific understanding of the relationships between the chemical composition of organic particles and their hygroscopicity and CCN activity, (2) develop an improved molecular level theoretical framework for describing these relationships, and (3) establish a large database that is being used to develop parameterizations relating organic aerosol chemical properties and SOA sources to particle hygroscopicity and CCN activity for use in regional and global atmospheric air quality and climate models.

  5. Changes in droplet surface tension affect the observed hygroscopicity of photochemically aged biomass burning aerosol.

    PubMed

    Giordano, Michael R; Short, Daniel Z; Hosseini, Seyedehsan; Lichtenberg, William; Asa-Awuku, Akua A

    2013-10-01

    This study examines the hygroscopic and surface tension properties as a function of photochemical aging of the aerosol emissions from biomass burning. Experiments were conducted in a chamber setting at the UC-Riverside Center for Environmental Research and Technology (CE-CERT) Atmospheric Processes Lab using two biomass fuel sources, manzanita and chamise. Cloud condensation nuclei (CCN) measurements and off-line filter sample analysis were conducted. The water-soluble organic carbon content and surface tension of the extracted filter samples were measured. Surface tension information was then examined with Köhler theory analysis to calculate the hygroscopicity parameter, κ. Laboratory measurement of biomass burning smoke from two chaparral fuels is shown to depress the surface tension of water by 30% or more at organic matter concentrations relevant at droplet activation. Accounting for surface tension depression can lower the calculated κ by a factor of 2. This work provides evidence for surface tension depression in an important aerosol system and may provide closure for differing sub- and supersaturated κ measurements. PMID:23957441

  6. Changes in droplet surface tension affect the observed hygroscopicity of photochemically aged biomass burning aerosol.

    PubMed

    Giordano, Michael R; Short, Daniel Z; Hosseini, Seyedehsan; Lichtenberg, William; Asa-Awuku, Akua A

    2013-10-01

    This study examines the hygroscopic and surface tension properties as a function of photochemical aging of the aerosol emissions from biomass burning. Experiments were conducted in a chamber setting at the UC-Riverside Center for Environmental Research and Technology (CE-CERT) Atmospheric Processes Lab using two biomass fuel sources, manzanita and chamise. Cloud condensation nuclei (CCN) measurements and off-line filter sample analysis were conducted. The water-soluble organic carbon content and surface tension of the extracted filter samples were measured. Surface tension information was then examined with Köhler theory analysis to calculate the hygroscopicity parameter, κ. Laboratory measurement of biomass burning smoke from two chaparral fuels is shown to depress the surface tension of water by 30% or more at organic matter concentrations relevant at droplet activation. Accounting for surface tension depression can lower the calculated κ by a factor of 2. This work provides evidence for surface tension depression in an important aerosol system and may provide closure for differing sub- and supersaturated κ measurements.

  7. 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

  8. 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

  9. Low hygroscopic scattering enhancement of boreal aerosol and the implications for a columnar optical closure study

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Aalto, P. P.; Aaltonen, V.; Äijälä, M.; Backman, J.; Hong, J.; Komppula, M.; Krejci, R.; Laborde, M.; Lampilahti, J.; de Leeuw, G.; Pfüller, A.; Rosati, B.; Tesche, M.; Tunved, P.; Väänänen, R.; Petäjä, T.

    2015-07-01

    Ambient aerosol particles can take up water and thus change their optical properties depending on the hygroscopicity and the relative humidity (RH) of the surrounding air. Knowledge of the hygroscopicity effect is of crucial importance for radiative forcing calculations and is also needed for the comparison or validation of remote sensing or model results with in situ measurements. Specifically, particle light scattering depends on RH and can be described by the scattering enhancement factor f(RH), which is defined as the particle light scattering coefficient at defined RH divided by its dry value (RH <30-40 %). Here, we present results of an intensive field campaign carried out in summer 2013 at the SMEAR II station at Hyytiälä, Finland. Ground-based and airborne measurements of aerosol optical, chemical and microphysical properties were conducted. The f(RH) measured at ground level by a humidified nephelometer is found to be generally lower (e.g. 1.63±0.22 at RH = 85 % and λ = 525 nm) than observed at other European sites. One reason is the high organic mass fraction of the aerosol encountered at Hyytiälä to which f(RH) is clearly anti-correlated (R2≈0.8). A simplified parametrization of f(RH) based on the measured chemical mass fraction can therefore be derived for this aerosol type. A trajectory analysis revealed that elevated values of f(RH) and the corresponding elevated inorganic mass fraction are partially caused by transported hygroscopic sea spray particles. An optical closure study shows the consistency of the ground-based in situ measurements. Our measurements allow to determine the ambient particle light extinction coefficient using the measured f(RH). By combining the ground-based measurements with intensive aircraft measurements of the particle number size distribution and ambient RH, columnar values of the particle extinction coefficient are determined and compared to columnar measurements of a co-located AERONET sun photometer. The water

  10. The impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2 photolysis rate coefficient

    NASA Astrophysics Data System (ADS)

    Tao, Jiangchuan; Zhao, Chunsheng

    2016-04-01

    Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number-size distribution and hygroscopic growth factor (at RH values above 90 %) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty ofω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90 %). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98 % at the height of 1 km increases by 30.4 %, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.

  11. Comparison Between Lidar and Nephelometer Measurements of Aerosol Hygroscopicity at the Southern Great Plains Atmospheric Radiation Measurement Site

    NASA Technical Reports Server (NTRS)

    Pahlow, M.; Feingold, G.; Jefferson, A.; Andrews, E.; Ogren, J. A.; Wang, J.; Lee, Y.-N.; Ferrare, R. A.

    2004-01-01

    Aerosol hygroscopicity has a significant effect on radiative properties of aerosols. Here a lidar method, applicable to cloud-capped, well-mixed atmospheric boundary layers, is employed to determine the hygroscopic growth factor f(RH) under unperturbed, ambient atmospheric conditions. The data used for the analysis were collected under a wide range of atmospheric aerosol levels during both routine measurement periods and during the intensive operations period (IOP) in May 2003 at the Southern Great Plains (SGP) Climate Research Facility in Oklahoma, USA, as part of the Atmospheric Radiation Measurement (ARM) program. There is a good correlation (approx. 0.7) between a lidar-derived growth factor (measured over the range 85% RH to 96% RH) with a nephelometer-derived growth factor measured over the RH range 40% to 85%. For these RH ranges, the slope of the lidar-derived growth factor is much steeper than that of the nephelometer-derived growth factor, reflecting the rapid increase in particle size with increasing RH. The results are corroborated by aerosol model calculations of lidar and nephelometer equivalent f(RH) based on in situ aerosol size and composition measurements during the IOP. It is suggested that the lidar method can provide useful measurements of the dependence of aerosol optical properties on relative humidity, and under conditions closer to saturation than can currently be achieved with humidified nephelometers.

  12. Size matters in the water uptake and hygroscopic growth of atmospherically relevant multicomponent aerosol particles.

    PubMed

    Laskina, Olga; Morris, Holly S; Grandquist, Joshua R; Qin, Zhen; Stone, Elizabeth A; Tivanski, Alexei V; Grassian, Vicki H

    2015-05-14

    Understanding the interactions of water with atmospheric aerosols is crucial for determining the size, physical state, reactivity, and climate impacts of this important component of the Earth's atmosphere. Here we show that water uptake and hygroscopic growth of multicomponent, atmospherically relevant particles can be size dependent when comparing 100 nm versus ca. 6 μm sized particles. It was determined that particles composed of ammonium sulfate with succinic acid and of a mixture of chlorides typical of the marine environment show size-dependent hygroscopic behavior. Microscopic analysis of the distribution of components within the aerosol particles show that the size dependence is due to differences in the mixing state, that is, whether particles are homogeneously mixed or phase separated, for different sized particles. This morphology-dependent hygroscopicity has consequences for heterogeneous atmospheric chemistry as well as aerosol interactions with electromagnetic radiation and clouds.

  13. Online hygroscopicity and chemical measurement of urban aerosol in Shanghai, China

    NASA Astrophysics Data System (ADS)

    Wang, Xinning; Ye, Xingnan; Chen, Hong; Chen, Jianmin; Yang, Xin; Gross, Deborah S.

    2014-10-01

    Submicron aerosol hygroscopicity and composition were simultaneously measured with a Hygroscopicity-Tandem Differential Mobility Analyzer (HTDMA) in-line with an Aerosol Time-of-Flight mass spectrometer (ATOFMS) in wintertime of 2009 in Shanghai. 250 nm dry diameter aerosol particles were humidified (85% RH) and selected based on their hygroscopicity. Two Growth Factor (GF) modes were observed persistently: a weak nearly-hydrophobic (NH) mode with GF at around 1.05 and a strong hydrophilic mode with GF around 1.46. Aerosol particles at different GFs were chemically analyzed by ATOFMS to link the aerosol hygroscopicity and chemistry. Particles were grouped into five major classes: inorganic dust/ash, biomass burning particles (BB), elemental carbon and organic carbon mixed particles (ECOC), Amine rich organic carbon particles (OC-Amine), and high mass organic carbon particles (HMOC). Different particle types were found enriched in the two GF modes. ECOC and OC-Amine particles internally mixed with secondary inorganic species were found mostly in the hydrophilic mode. Pure EC particles and a small group of clay particles among the dust/ash type with strong signals of aluminum and silicon oxides appeared in the NH mode. HMOC particles were exclusively found in the NH mode. Chemical signature intensities were analyzed to examine the particle mixing states and their impact on the diversity of hygroscopicity for each particle type. BB particles in the NH mode had stronger organic carbon signals, while those in hydrophilic mode had stronger potassium salt signals. In general, an elevated OC mass fraction increased particle's hydrophobicity. Amine and secondary inorganic species such as nitrate strongly increased particle's hygroscopicity.

  14. Dynamics of aerosol size during inhalation: hygroscopic growth of commercial nebulizer formulations.

    PubMed

    Haddrell, Allen E; Davies, James F; Miles, Rachael E H; Reid, Jonathan P; Dailey, Lea Ann; Murnane, Darragh

    2014-03-10

    The size of aerosol particles prior to, and during, inhalation influences the site of deposition within the lung. As such, a detailed understanding of the hygroscopic growth of an aerosol during inhalation is necessary to accurately model the deposited dose. In the first part of this study, it is demonstrated that the aerosol produced by a nebulizer, depending on the airflows rates, may experience a (predictable) wide range of relative humidity prior to inhalation and undergo dramatic changes in both size and solute concentration. A series of sensitive single aerosol analysis techniques are then used to make measurements of the relative humidity dependent thermodynamic equilibrium properties of aerosol generated from four common nebulizer formulations. Measurements are also reported of the kinetics of mass transport during the evaporation or condensation of water from the aerosol. Combined, these measurements allow accurate prediction of the temporal response of the aerosol size prior to and during inhalation. Specifically, we compare aerosol composed of pure saline (150 mM sodium chloride solution in ultrapure water) with two commercially available nebulizer products containing relatively low compound doses: Breath®, consisting of a simple salbutamol sulfate solution (5 mg/2.5 mL; 1.7 mM) in saline, and Flixotide® Nebules, consisting of a more complex stabilized fluticasone propionate suspension (0.25 mg/mL; 0.5 mM in saline. A mimic of the commercial product Tobi© (60 mg/mL tobramycin and 2.25 mg/mL NaCl, pH 5.5-6.5) is also studied, which was prepared in house. In all cases, the presence of the pharmaceutical was shown to have a profound effect on the magnitude, and in some cases the rate, of the mass flux of water to and from the aerosol as compared to saline. These findings provide physical chemical evidence supporting observations from human inhalation studies, and suggest that using the growth dynamics of a pure saline aerosol in a lung inhalation model

  15. Dynamics of aerosol size during inhalation: hygroscopic growth of commercial nebulizer formulations.

    PubMed

    Haddrell, Allen E; Davies, James F; Miles, Rachael E H; Reid, Jonathan P; Dailey, Lea Ann; Murnane, Darragh

    2014-03-10

    The size of aerosol particles prior to, and during, inhalation influences the site of deposition within the lung. As such, a detailed understanding of the hygroscopic growth of an aerosol during inhalation is necessary to accurately model the deposited dose. In the first part of this study, it is demonstrated that the aerosol produced by a nebulizer, depending on the airflows rates, may experience a (predictable) wide range of relative humidity prior to inhalation and undergo dramatic changes in both size and solute concentration. A series of sensitive single aerosol analysis techniques are then used to make measurements of the relative humidity dependent thermodynamic equilibrium properties of aerosol generated from four common nebulizer formulations. Measurements are also reported of the kinetics of mass transport during the evaporation or condensation of water from the aerosol. Combined, these measurements allow accurate prediction of the temporal response of the aerosol size prior to and during inhalation. Specifically, we compare aerosol composed of pure saline (150 mM sodium chloride solution in ultrapure water) with two commercially available nebulizer products containing relatively low compound doses: Breath®, consisting of a simple salbutamol sulfate solution (5 mg/2.5 mL; 1.7 mM) in saline, and Flixotide® Nebules, consisting of a more complex stabilized fluticasone propionate suspension (0.25 mg/mL; 0.5 mM in saline. A mimic of the commercial product Tobi© (60 mg/mL tobramycin and 2.25 mg/mL NaCl, pH 5.5-6.5) is also studied, which was prepared in house. In all cases, the presence of the pharmaceutical was shown to have a profound effect on the magnitude, and in some cases the rate, of the mass flux of water to and from the aerosol as compared to saline. These findings provide physical chemical evidence supporting observations from human inhalation studies, and suggest that using the growth dynamics of a pure saline aerosol in a lung inhalation model

  16. 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.

  17. The hygroscopic properties of dicarboxylic and multifunctional acids: measurements and UNIFAC predictions.

    PubMed

    Peng, C; Chan, M N; Chan, C K

    2001-11-15

    The role of water-soluble organic compounds on the hygroscopic properties of atmospheric aerosols has recently been the subject of many studies. In particular, low molecular weight dicarboxylic acids and some multifunctional organic acids have been found or are expected to exist in atmospheric aerosols in urban, semiurban, rural, and remote sites. Unlike for their inorganic counterparts, the hygroscopic properties of organic acids have not been well characterized. In this study, the hygroscopic properties of selected water-soluble dicarboxylic acids (oxalic acid, malonic acid, succinic acid, and glutaric acid) and multifunctional acids (citric acid, DL-malic acid, and L-(+)-tartaric acid) were studied using single droplets levitated in an electrodynamic balance at 25 degrees C. The water activities of bulk samples of dilute solutions were also measured. Solute evaporation was observed in the dicarboxylic acids but not in the multifunctional acids. Oxalic acid, succinic acid, and glutaric acid droplets crystallize upon evaporation of water, but, except for glutaric acid droplets, do not deliquesce even at 90% relative humidity (RH). Mass transfer limitation of the deliquescence process was observed in glutaric acid. Neither crystallization nor deliquescence was observed in malonic acid, citric acid, DL-malic acid, or L-(+)-tartaric acid. Malonic acid and these three hydroxy-carboxylic acids absorb water even at RH much lower than their respective deliquescence RH. The growth factor (Gf), defined as the ratio of the particle diameter at RH = 10% to that at RH = 90%, of oxalic acid and succinic acid was close to unity, indicating no hygroscopicity in this range. The remaining acids (malonic acid, glutaric acid, citric acid, malic acid, and tartaric acid) showed roughly similar hygroscopicity of a Gf of 1.30-1.53, which is similar to that of "more hygroscopic" aerosols in field measurements reported in the literature. A generalized equation for these four acids, Gf

  18. Accurate Measurements of Aerosol Hygroscopic Growth over a Wide Range in Relative Humidity.

    PubMed

    Rovelli, Grazia; Miles, Rachael E H; Reid, Jonathan P; Clegg, Simon L

    2016-06-30

    Using a comparative evaporation kinetics approach, we describe a new and accurate method for determining the equilibrium hygroscopic growth of aerosol droplets. The time-evolving size of an aqueous droplet, as it evaporates to a steady size and composition that is in equilibrium with the gas phase relative humidity, is used to determine the time-dependent mass flux of water, yielding information on the vapor pressure of water above the droplet surface at every instant in time. Accurate characterization of the gas phase relative humidity is provided from a control measurement of the evaporation profile of a droplet of know equilibrium properties, either a pure water droplet or a sodium chloride droplet. In combination, and by comparison with simulations that account for both the heat and mass transport governing the droplet evaporation kinetics, these measurements allow accurate retrieval of the equilibrium properties of the solution droplet (i.e., the variations with water activity in the mass fraction of solute, diameter growth factor, osmotic coefficient or number of water molecules per solute molecule). Hygroscopicity measurements can be made over a wide range in water activity (from >0.99 to, in principle, <0.05) on time scales of <10 s for droplets containing involatile or volatile solutes. The approach is benchmarked for binary and ternary inorganic solution aerosols with typical uncertainties in water activity of <±0.2% at water activities >0.9 and ∼±1% below 80% RH, and maximum uncertainties in diameter growth factor of ±0.7%. For all of the inorganic systems examined, the time-dependent data are consistent with large values of the mass accommodation (or evaporation) coefficient (>0.1). PMID:27285052

  19. Hygroscopic growth of urban aerosol particles in Beijing (China) during wintertime: a comparison of three experimental methods

    NASA Astrophysics Data System (ADS)

    Meier, J.; Wehner, B.; Massling, A.; Birmili, W.; Nowak, A.; Gnauk, T.; Brüggemann, E.; Herrmann, H.; Min, H.; Wiedensohler, A.

    2009-09-01

    The hygroscopic properties of atmospheric aerosols are highly relevant for the quantification of radiative effects in the atmosphere, but also of interest for the assessment of particle health effects upon inhalation. This article reports measurements of aerosol particle hygroscopicity in the highly polluted urban atmosphere of Beijing, China in January 2005. The meteorological conditions corresponded to a relatively cold and dry atmosphere. Three different methods were used: 1) A combination of Humidifying Differential Mobility Particle Sizer (H-DMPS) and Twin Differential Mobility Particle Sizer (TDMPS) measurements, 2) A Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), and 3) A simplistic solubility model fed by chemical particle composition determined from Micro Orifice Uniform Deposit Impactor (MOUDI) samples. From the H-DMPS and TDMPS particle number size distributions, a size-resolved descriptive hygroscopic growth factor (DHGF) was determined for the relative humidities (RH) 55%, 77% and 90%, and particle diameters between 30 and 400 nm. In Beijing, the highest DHGFs were observed for accumulation mode particles, 1.40 (±0.03) at 90% RH. DHGF decreased significantly with particle size, reaching 1.04 (±0.15) at 30 nm. H-TDMA data also suggest a decrease in growth factor towards the biggest particles investigated (350 nm), associated with an increasing fraction of nearly hydrophobic particles. The agreement between the H-DMPS/TDMPS and H-TDMA methods was satisfactory in the accumulation mode size range (100-400 nm). In the Aitken mode range (<100 nm), the H-DMPS/TDMPS method yielded growth factors lower by up to 0.1 at 90% RH. The application of the solubility model based on measured chemical composition clearly reproduced the size-dependent trend in hygroscopic particle growth observed by the other methods. In the case of aerosol dominated by inorganic ions, the composition-derived growth factors tended to agree (± 0.05) or underestimate (up to

  20. Hygroscopicity of Amine Secondary Aerosol - Mixtures of Organic and Inorganic Components

    NASA Astrophysics Data System (ADS)

    Tang, X.; Cocker, D. R.; Purvis-Roberts, K.; Asa-Awuku, A. A.

    2012-12-01

    Aliphatic amines are emitted from both biogenic and anthropogenic sources and contribute to the formation of secondary aerosol in reactions with atmospheric radicals. However, the cloud condensation nuclei (CCN) ability of amine aerosol has not been explored yet. Here, we study the hygroscopicity of aerosol formed from three aliphatic amines (trimethylamine, diethylamine and butylamine) in the UCR environmental chamber. Amines can react with NO3, a dominant night time oxidant in acid-base and/or oxidation reactions. The mass fraction of organic and inorganic components of formed aerosol was measured by Particle-into-Liquid Sampler coupled to dual ion chromatographs (PILS-ICs) and Scanning Mobility Particle Sizer (SMPS). CCN counter was used to measure the water-uptake ability of these particles. Significantly high hygroscopicity (κ>0.3) was observed for aerosols formed from diethylamine and butylamine with NO3 radicals, which comprised >40% inorganic salt. Compared with amines oxidized by hydroxyl radicals, the presence of aminium salts formed in acid-base reactions greatly improved CCN activity of NO3-initiated aerosol. The effect of water vapor on the formation of aminium salts and aerosol hygroscopicity was also studied. Our results will significantly impact the estimation and role of amines in atmospheric chemistry and global climate models.

  1. Study of aerosol hygroscopic events over the Cabauw experimental site for atmospheric research (CESAR) using the multi-wavelength Raman lidar Caeli

    NASA Astrophysics Data System (ADS)

    Fernández, A. J.; Apituley, A.; Veselovskii, I.; Suvorina, A.; Henzing, J.; Pujadas, M.; Artíñano, B.

    2015-11-01

    This article presents a study of aerosol optical and microphysical properties under different relative humidity (RH) but well mixed layer conditions using optical and microphysical aerosol properties from multi-wavelength (MW) Raman lidar and in-situ aerosol observations collected at the Cabauw Experimental Site for Atmospheric Research (CESAR). Two hygroscopic events are described through 3 backscatter (β) and 2 extinction (α) coefficients which in turn provide intensive parameters such as the backscatter-related Ångström exponent (åβ) and the lidar ratio (LR). Along with it, profiles of RH were inferred from Raman lidar observations and therefore, as a result of varying humidity conditions, a shift on the aerosol optical properties can be described. Thus, it is observed that as RH increases, aerosols uptake water vapour, augment their size and consequently the åβ diminishes whereas the LR increases. The enhancement factor based on the backscatter coefficient at 532 nm, which characterizes the aerosol from hygroscopic standpoint, is also estimated. Finally, microphysical properties that are necessary for aerosol radiative forcing estimates - such as volume, effective radii, refractive index and size distribution, all vertically resolved - are retrieved using the inversion with regularization. Using this method, two hygroscopic events are described in detail.

  2. Aerosol hygroscopicity and CCN activation kinetics in a boreal forest environment during the 2007 EUCAARI campaign

    NASA Astrophysics Data System (ADS)

    Cerully, K. M.; Raatikainen, T.; Lance, S.; Tkacik, D.; Tiitta, P.; Petäjä, T.; Ehn, M.; Kulmala, M.; Worsnop, D. R.; Laaksonen, A.; Smith, J. N.; Nenes, A.

    2011-12-01

    Measurements of size-resolved cloud condensation nuclei (CCN) concentrations, subsaturated hygroscopic growth, size distribution, and chemical composition were collected from March through May, 2007, in the remote Boreal forests of Hyytiälä, Finland, as part of the European Integrated project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaign. Hygroscopicity parameter, κ, distributions were derived independently from Continuous Flow-Streamwise Thermal Gradient CCN Chamber (CFSTGC) and Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) measurements. CFSTGC-derived κ values for 40, 60, and 80 nm particles range mostly between 0.10 and 0.40 with an average characteristic of highly oxidized organics of 0.20 ± 0.10, indicating that organics play a dominant role for this environment. HTDMA-derived κ were generally 30% lower. Diurnal trends of κ show a minimum at sunrise and a maximum in the late afternoon; this trend covaries with inorganic mass fraction and the m/z 44 organic mass fraction given by a quadrupole aerosol mass spectrometer, further illustrating the importance of organics in aerosol hygroscopicity. The chemical dispersion inferred from the observed κ distributions indicates that while 60 and 80 nm dispersion increases around midday, 40 nm dispersion remains constant. Additionally, 80 nm particles show a markedly higher level of chemical dispersion than both 40 and 60 nm particles. An analysis of droplet activation kinetics for the sizes considered indicates that most of the CCN activate as rapidly as (NH4)2SO4 calibration aerosol.

  3. Aerosol hygroscopicity and CCN activation kinetics in a boreal forest environment during the 2007 EUCAARI campaign

    NASA Astrophysics Data System (ADS)

    Cerully, K. M.; Raatikainen, T.; Lance, S.; Tkacik, D.; Tiitta, P.; Petäjä, T.; Ehn, M.; Kulmala, M.; Worsnop, D. R.; Laaksonen, A.; Smith, J. N.; Nenes, A.

    2011-05-01

    Measurements of size-resolved cloud condensation nuclei (CCN), subsaturated hygroscopic growth, size distribution, and chemical composition were collected from March through May, 2007, in the remote Boreal forests of Hyytiälä, Finland, as part of the European Integrated project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaign. Hygroscopicity parameter, κ, distributions were derived independently from Continuous Flow-Streamwise Thermal Gradient CCN Chamber (CFSTGC) and Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) measurements. CFSTGC-derived κ values for 40, 60, and 80 nm particles range mostly between 0.10 and 0.40 with an average of 0.20 ± 0.10; this is characteristic of highly oxidized organics and reflect their dominant influence in this environment. HTDMA-derived κ were generally 30 % lower. Diurnal trends of κ show a minimum at sunrise and a maximum in the late afternoon; this trend covaries with inorganic mass fraction and the m/z 44 organic mass fraction given by a quadrupole aerosol mass spectrometer, further illustrating the importance of ageing on aerosol hygroscopicity. The chemical dispersion inferred from the observed κ distributions indicates that while 60 and 80 nm dispersion increases around midday, 40 nm dispersion remains constant. Additionally, 80 nm particles show a markedly higher level of chemical dispersion than both 40 and 60 nm particles. An analysis of droplet activation kinetics for the sizes considered indicates that the CCN activate as rapidly as (NH4)2SO4 calibration aerosol.

  4. Microphysical and Chemical Properties of Agricultural Aerosols

    NASA Astrophysics Data System (ADS)

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

    2005-12-01

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

  5. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2014-12-01

    Atmospheric aerosols have the ability to act as cloud condensation nuclei (CCN), initiating the formation of clouds and hereby influencing the climate system. The ability of aerosols to act as CCN is believed to depend on particle size and chemical composition. Organosulfates (OS), e.g sulfate esters, have been observed as constituents of secondary organic aerosols in numerous atmospheric environments, even as far as the Arctic, where OS have been found to comprise 7-15% of total organic matter and 9-11% of submicron organic matter in two independent studies. However, the properties of particulate OS have not yet been investigated. Here limonene derived OS were synthesized and the hygroscopic properties of these OS and their mixtures with ammonium sulfate (AS) were examined through a series of laboratory experiments. Laboratory generated particles of limonene-derived OS and AS were analysed using a unique set-up splitting the particle flow between a Hygroscopicity Tandem Differential Mobility Analyzer and a Cloud Condensation Nuclei counter, enabling simultaneous measurements of hygroscopic growth and CCN activation. Limonene-derived OS were chosen as study components, since monoterpenes (including limonene) have been identified as important precursors of OS in field samples as well as in smog chamber experiments. AS was used as a representative of the inorganic fraction in atmospheric aerosols. The preliminary results show that limonene-derived OS exhibit weak hygroscopic growth as well as CCN activation potential, however, not as strong as AS. For the organic-inorganic mixtures, it was observed that AS dominated the hygroscopic properties over the limonene-derived OS and became dictating for the measured values of hygroscopic growth and CCN activation, when the mass fraction of AS reached 20% or above. The results will be discussed further and supplementary measurements of OS surface tension and water activity will be presented.

  6. Toward Quantifying the Mass-Based Hygroscopicity of Individual Submicron Atmospheric Aerosol Particles with STXM/NEXAFS and SEM/EDX

    NASA Astrophysics Data System (ADS)

    Yancey Piens, D.; Kelly, S. T.; OBrien, R. E.; Wang, B.; Petters, M. D.; Laskin, A.; Gilles, M. K.

    2014-12-01

    The hygroscopic behavior of atmospheric aerosols influences their optical and cloud-nucleation properties, and therefore affects climate. Although changes in particle size as a function of relative humidity have often been used to quantify the hygroscopic behavior of submicron aerosol particles, it has been noted that calculations of hygroscopicity based on size contain error due to particle porosity, non-ideal volume additivity and changes in surface tension. We will present a method to quantify the hygroscopic behavior of submicron aerosol particles based on changes in mass, rather than size, as a function of relative humidity. This method results from a novel experimental approach combining scanning transmission x-ray microscopy with near-edge x-ray absorption fine spectroscopy (STXM/NEXAFS), as well as scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDX) on the same individual particles. First, using STXM/NEXAFS, our methods are applied to aerosol particles of known composition ‒ for instance ammonium sulfate, sodium bromide and levoglucosan ‒ and validated by theory. Then, using STXM/NEXAFS and SEM/EDX, these methods are extended to mixed atmospheric aerosol particles collected in the field at the DOE Atmospheric Radiation Measurement (ARM) Climate Research Facility at the Southern Great Planes sampling site in Oklahoma, USA. We have observed and quantified a range of hygroscopic behaviors which are correlated to the composition and morphology of individual aerosol particles. These methods will have implications for parameterizing aerosol mixing state and cloud-nucleation activity in atmospheric models.

  7. Characterizing the Hygroscopicity of Nascent Sea Spray Aerosol from Synthetic Blooms

    NASA Astrophysics Data System (ADS)

    Forestieri, S.; Cappa, C. D.; Sultana, C. M.; Lee, C.; Wang, X.; Helgestad, T.; Moore, K.; Prather, K. A.; Cornwell, G.; Novak, G.; Bertram, T. H.

    2015-12-01

    Marine sea spray aerosol (SSA) particles make up a significant portion of natural aerosols and are therefore important in establishing the baseline for anthropogenic aerosol climate impacts. Scattering of solar radiation by aerosols affects Earth's radiative budget and the degree of scattering is size-dependent. Thus, aerosols scatter more light at elevated relative humidities when they grow larger via water uptake. This growth depends critically on chemical composition. SSA can become enriched in organics during phytoplankton blooms, becoming less salty and therefore less hygroscopic. Subsaturated hygroscopic growth factors at 85% relative humidity (GF(85%)) of SSA particles were quantified during two mesocosm experiments in enclosed marine aerosol reference tanks (MARTs). The two experiments were conducted with filtered seawater collected at separate times from the Scripps Institute of Oceanography Pier in La Jolla, CA. Phytoplankton blooms in each tank were induced via the addition of nutrients and photosynthetically active radiation. The "indoor" MART was illuminated with fluorescent light and the other "outdoor" MART was illuminated with sunlight. The peak chlorophyll-a concentrations were 59 micrograms/L and 341 micrograms /L for the indoor and outdoor MARTs, respectively. GF(85%) values for SSA particles were quantified using a humidified cavity ringdown spectrometer and particle size distributions. Particle composition was monitored with a single particle aerosol mass spectrometer (ATOFMS) and an Aerodyne aerosol mass spectrometer (AMS). Relationships between the observed particle GFs and the particle composition markers will be discussed.

  8. Ambient black carbon particle hygroscopic properties controlled by mixing state and composition

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J.; Whitehead, J.; Young, D.; Flynn, M.; Coe, H.; McFiggans, G.; Fleming, Z. L.; Bandy, B.

    2013-02-01

    The wet removal of black carbon aerosol (BC) in the atmosphere is a crucial factor in determining its atmospheric lifetime and thereby the vertical and horizontal distributions, dispersion on local and regional scales, and the direct, semi-direct and indirect radiative forcing effects. The in-cloud scavenging and wet deposition rate of freshly emitted hydrophobic BC will be increased on acquisition of more-hydrophilic components by coagulation or coating processes. The lifetime of BC is still subject to considerable uncertainty for most of the model inputs, which is largely due to the insufficient constraints on the BC hydrophobic-to-hydrophilic conversion process from observational field data. This study was conducted at a site along UK North Norfolk coastline, where the BC particles were transported from different regions within Western Europe. A hygroscopicity tandem differential mobility analyser (HTDMA) was coupled with a single particle soot photometer (SP2) to measure the hygroscopic properties of BC particles and associated mixing state in real time. In addition, a Soot Particle AMS (SP-AMS) measured the chemical compositions of additional material associated with BC particles. The ensemble of BC particles persistently contained a less-hygroscopic mode at a growth factor (gf) of around 1.05 at 90% RH (dry diameter 163 nm). Importantly, a more-hygroscopic mode of BC particles was observed throughout the experiment, the gf of these BC particles extended up to ~1.4-1.6 with the minimum between this and the less hygroscopic mode at a gf ~1.25, or equivalent effective hygroscopicity parameter κ ~0.1. The gf of BC particles (gfBC) was highly influenced by the composition of associated soluble material: increases of gfBC were associated with secondary inorganic components, and these increases were more pronounced when ammonium nitrate was in the BC particles; however the presence of secondary organic matter suppressed the gfBC below that of pure inorganics. The

  9. Ambient black carbon particle hygroscopic properties controlled by mixing state and composition

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J.; Whitehead, J.; Young, D.; Flynn, M.; Coe, H.; McFiggans, G.; Fleming, Z.; Bandy, B.

    2012-11-01

    The wet removal of black carbon aerosol (BC) in the atmosphere is a crucial factor in determining its atmospheric lifetime and thereby the vertical and horizontal distributions, dispersion on local and regional scales, and the direct, semi-direct and indirect radiative forcing effects. The in-cloud scavenging and wet deposition rate of freshly emitted hydrophobic BC will be increased on acquisition of more-hydrophilic components by coagulation or coating processes. The lifetime of BC is still subject to considerable uncertainty for most of the model inputs, which is largely due to the insufficient constraints on the BC hydrophobic-to-hydrophilic conversion process from observational field data. This study was conducted at a site along UK North Norfolk coastline, where the BC particles were transported from different regions within Western Europe. A hygroscopicity tandem differential mobility analyser (HTDMA) was coupled with a single particle soot photometer (SP2) to measure the hygroscopic properties of BC particles and associated mixing state in real time. In addition, a Soot Particle AMS (SP-AMS) measured the chemical compositions of additional material associated with BC particles. The ensemble of BC particles persistently contained a less-hygroscopic mode at a growth factor (gf) of around 1.05 at 90% RH (dry diameter 163 nm). Importantly, a more-hygroscopic mode of BC particles was observed throughout the experiment, the gf of these BC particles extended up to ~1.4-1.6 with the minimum between this and the less hygroscopic mode at a gf ~1.25, or equivalent effective hygroscopicity parameter κ = ~0.1. The gf of BC particles (gfBC) was highly influenced by the composition of associated soluble material: increases of gfBC were associated with secondary inorganic components, and these increases were more pronounced when ammonium nitrate was in the BC particles; however the presence of secondary organic matter suppressed the gfBC below that of pure inorganics. The

  10. 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.

  11. Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation.

    PubMed

    Tang, Mingjin; Cziczo, Daniel J; Grassian, Vicki H

    2016-04-13

    Mineral dust aerosol is one of the major types of aerosol present in the troposphere. The molecular level interactions of water vapor with mineral dust are of global significance. Hygroscopicity, light scattering and absorption, heterogneous reactivity and the ability to form clouds are all related to water-dust interactions. In this review article, experimental techniques to probe water interactions with dust and theoretical frameworks to understand these interactions are discussed. A comprehensive overview of laboratory studies of water adsorption, hygroscopicity, cloud condensation, and ice nucleation of fresh and atmspherically aged mineral dust particles is provided. Finally, we relate laboratory studies and theoretical simulations that provide fundemental insights into these processes on the molecular level with field measurements that illustrate the atmospheric significance of these processes. Overall, the details of water interactions with mineral dust are covered from multiple perspectives in this review article. PMID:27015126

  12. Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation.

    PubMed

    Tang, Mingjin; Cziczo, Daniel J; Grassian, Vicki H

    2016-04-13

    Mineral dust aerosol is one of the major types of aerosol present in the troposphere. The molecular level interactions of water vapor with mineral dust are of global significance. Hygroscopicity, light scattering and absorption, heterogneous reactivity and the ability to form clouds are all related to water-dust interactions. In this review article, experimental techniques to probe water interactions with dust and theoretical frameworks to understand these interactions are discussed. A comprehensive overview of laboratory studies of water adsorption, hygroscopicity, cloud condensation, and ice nucleation of fresh and atmspherically aged mineral dust particles is provided. Finally, we relate laboratory studies and theoretical simulations that provide fundemental insights into these processes on the molecular level with field measurements that illustrate the atmospheric significance of these processes. Overall, the details of water interactions with mineral dust are covered from multiple perspectives in this review article.

  13. Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

    DOE PAGES

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2015-07-24

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased duringmore » photo-oxidation, and the final OA OSc ranged from -0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  14. Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

    NASA Astrophysics Data System (ADS)

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2015-07-01

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OSc ranged from -0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.

  15. Simultaneous analysis of the equilibrium hygroscopicity and water transport kinetics of liquid aerosol.

    PubMed

    Davies, James F; Haddrell, Allen E; Rickards, Andrew M J; Reid, Jonathan P

    2013-06-18

    We demonstrate that the equilibrium hygroscopic response of an aerosol droplet and the kinetics of water condensation and evaporation can be retrieved with high accuracy, even close to saturation, through comparative measurements of probe and sample aerosol droplets. The experimental methodology is described and is based on an electrodynamic balance with a newly designed trapping chamber. Through use of a probe aerosol, composed of either pure water or a sodium chloride solution of known concentration, the gas-phase relative humidity (RH) can be accurately measured with an uncertainty of typically <0.005. By fast manipulation of the airflows into the chamber, a step-change in RH over a time scale of <0.5 s can be achieved. Using this approach, the kinetics of mass transfer are studied using the comparative procedure, and results are compared to theoretical mass flux predictions. The time-dependent measured mass fluxes for sodium chloride, ammonium sulfate, sorbitol, and galactose are used to calculate droplet water activities as a function of the droplet growth factor, allowing retrieval of a hygroscopic growth curve in a matter of seconds. Comparisons with both new and established thermodynamic predictions of hygroscopicity, as well as to optical tweezers measurements, are presented, demonstrating good agreement within the experimental uncertainties. PMID:23662676

  16. Deriving aerosol hygroscopic mixing state from size-resolved CCN activity and HR-ToF-AMS measurements

    NASA Astrophysics Data System (ADS)

    Bhattu, Deepika; Tripathi, S. N.; Chakraborty, Abhishek

    2016-10-01

    The ability of a particle to uptake water and form a cloud droplet depends on its hygroscopicity. To understand its impact on cloud properties and ultimately radiative forcing, knowledge of chemically-resolved mixing state information or the one based on hygroscopic growth is crucial. Typically, global models assume either pure internal or external mixing state which might not be true for all conditions and sampling locations. To investigate into this, the current study employed an indirect approach to infer the probable mixing state. The hygroscopic parameters derived from κ-Kohler theory using size-resolved CCN measurements (κCCN) and bulk/size-resolved aerosol mass spectrometer (AMS) measurements (κAMS) were compared. The accumulation mode particles were found to be more hygroscopic (κCCN = 0.24) than Aitken mode (κCCN = 0.13), perhaps due to increased ratio of inorganic to organic mass fraction. The activation diameter calculated from size-resolved CCN activity measurements at 5 different supersaturation (SS) levels varied in the range of 115 nm-42 nm with κCCN = 0.13-0.23 (avg = 0.18 ± 0.10 (±1σ)). Further, κAMS>κCCN was observed possibly due to the fact that organic and inorganic mass present in the Aitken mode was not correctly represented by bulk chemical composition and size-resolved fractional contribution of oxidized OA was not accurately accounted. Better correlation of organic fraction (forg) and κCCN at lower SS explained this behaviour. The decrease in κCCN with the time of the day was more pronounced at lower SS because of the relative mass reduction of soluble inorganic species by ∼17%. Despite the large differences between κ measured from two approaches, less over-prediction (up to 18%) between measured and predicted CCN concentration suggested lower impact of chemical composition and mixing state at higher SS. However, at lower SS, presences of externally mixed CCN-inactive aerosols lead to CCN over-prediction reflecting the

  17. Measuring and modeling the hygroscopic growth of two humic substances in mixed aerosol particles of atmospheric relevance

    NASA Astrophysics Data System (ADS)

    Zamora, I. R.; Jacobson, M. Z.

    2013-09-01

    The hygroscopic growth of atmospheric particles affects atmospheric chemistry and Earth's climate. Water-soluble organic carbon (WSOC) constitutes a significant fraction of the dry submicron mass of atmospheric aerosols, thus affecting their water uptake properties. Although the WSOC fraction is comprised of many compounds, a set of model substances can be used to describe its behavior. For this study, mixtures of Nordic aquatic fulvic acid reference (NAFA) and Fluka humic acid (HA), with various combinations of inorganic salts (sodium chloride and ammonium sulfate) and other representative organic compounds (levoglucosan and succinic acid), were studied. We measured the equilibrium water vapor pressure over bulk solutions of these mixtures as a function of temperature and solute concentration. New water activity (aw) parameterizations and hygroscopic growth curves at 25 °C were calculated from these data for particles of equivalent composition. We examined the effect of temperature on the water activity and found a maximum variation of 9% in the 0-30 °C range, and 2% in the 20-30 °C range. Five two-component mixtures were studied to understand the effect of adding a humic substance (HS), such as NAFA and HA, to an inorganic salt or a saccharide. The deliquescence point at 25 °C for HS-inorganic mixtures did not change significantly from that of the pure inorganic species. However, the hygroscopic growth of HA / inorganic mixtures was lower than that exhibited by the pure salt, in proportion to the added mass of HA. The addition of NAFA to a highly soluble solute (ammonium sulfate, sodium chloride or levoglucosan) in water had the same effect as the addition of HA to the inorganic species for most of the water activity range studied. Yet, the water uptake of these NAFA mixtures transitioned to match the growth of the pure salt or saccharide at high aw values. The remaining four mixtures were based on chemical composition data for different aerosol types. As

  18. The impact of marine surface organic enrichment on the measured hygroscopicity parameter of laboratory generated sea-spray aerosols

    NASA Astrophysics Data System (ADS)

    Schill, S.; Novak, G.; Zimmermann, K.; Bertram, T. H.

    2014-12-01

    The ocean serves as a major source for atmospheric aerosol particles, yet the chemicophysical properties of sea spray aerosol to date are not well characterized. Understanding the transfer of organic compounds, present in the sea surface microlayer (SSML), to sea-spray particles and their resulting impact on cloud formation is important for predicting aerosol impact on climate in remote marine environments. Here, we present a series of laboratory experiments designed to probe the fractionation of select organic molecules during wave breaking. We use a representative set of organic mimics (e.g. sterols, sugars, lipids, proteins, fatty acids) to test a recent physically based model of organic enrichment in sea-spray aerosol [Burrows et al., 2014] that is based on Langmuir absorption equilibria. Experiments were conducted in the UCSD Marine Aerosol Reference Tank (MART) permitting accurate representation of wave breaking processes in the laboratory. We report kappa values for the resulting sea-spray aerosols and compare them to a predictions made using Kappa-Köhler Theory driven by a linear combination of the pure component kappa values. Hygroscopicity determinations made using the model systems are discussed within the context of measurements of CCN activity made using natural, coastal water.

  19. 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.

  20. The effects of models of aerosol hygroscopicity on the apportionment of extinction

    NASA Astrophysics Data System (ADS)

    Malm, William C.; Kreidenweis, Sonia M.

    The role that aerosols play in climate forcing and visibility issues has been the subject of research for several decades. Recent research efforts have focused on assessing the contribution of individual species to scattering and absorption under ambient conditions and on how scattering and absorption change as one or more species are removed from the atmosphere. A key concern is the distribution of water among aerosols as a function of mixing assumptions. As an illustrative and relevant example, we examine the roles of sulfates and organics in visibility and climate forcing, and in particular, the implications of assumptions regarding hygroscopic growth behavior upon the assignment of mass-scattering efficiencies to these species. We demonstrate that the total scattering computed for an aerosol sample is relatively insensitive to the choice of internal or external mixture, and can be insensitive to the exact formulation of the hygroscopic growth of the sample. Since the atmospheric aerosol is generally a complex mixture of chemical species, with the precise distribution of species on a particle-by-particle basis not known, the use of semi-empirical models of multicomponent aerosol hygroscopicity is appropriate for the calculation of atmospheric aerosol scattering and/or extinction, particularly since these details appear to be unimportant in most cases. In contrast, the apportionment of percentages of the total scattering to individual chemical species is quite sensitive to the choice of assumption regarding the aerosol microphysical structure. The use of semi-empirical hygroscopic growth models for computing the change in species scattering efficiency can lead to incorrect predictions in the limit of the complete removal of all but one chemical component. We propose a model that invokes the Zdanovskii, Stokes, and Robinson (ZSR) assumptions for the water content of multicomponent mixtures, and demonstrate that this method both approximates the predictions of

  1. CCN Activity, Hygroscopicity, and Droplet Activation Kinetics of Secondary Organic Aerosol Resulting from the 2010 Gulf Oil Spill

    NASA Astrophysics Data System (ADS)

    Moore, R.; Lathem, T. L.; Cerully, K.; Bahreini, R.; Brock, C. A.; Langridge, J. M.; Middlebrook, A. M.; Nenes, A.; Calnex Science Team

    2010-12-01

    We present an analysis of the hygroscopicity and droplet activation kinetics of cloud condensation nuclei (CCN) sampled onboard the National Oceanic and Atmospheric Administration WP-3D aircraft downwind of the Deepwater Horizon oil spill site on June 8th and 10th, 2010. This set of measurements provides a unique case study for assessing in-situ the impact of fresh, hydrocarbonlike aerosols, which are expected to be formed via gas-to-particle conversion of the semi-volatile vapors released from oil evaporation. Similar hydrocarbon-rich aerosols constitute an important local emissions source in urban areas, but often coexist as an external/partially-internal mixture with more-oxidized, aged organic and sulfate aerosol. The DWH site provides the means to study the hygroscopic properties of these less-oxidized organic aerosols above a cleaner environmental background typical of marine environments in order to better discern their contribution to CCN activity and droplet growth. Measurements were performed with a Droplet Measurement Technologies Streamwise, Thermal-Gradient CCN counter, operating both as a counter (s=0.3%) and as a spectrometer (s=0.2-0.6%) using the newly-developed Scanning Flow CCN Analysis (SFCA) technique [1]. The instrument measures both the number concentration of particles able to nucleate droplets and also their resulting droplet sizes. The measured size information combined with a comprehensive computational fluid dynamics instrument model enables us to determine the rate of water uptake onto the particles and parameterize it in terms of an effective mass transfer coefficient [2], a key parameter needed to predict the number of activated droplets in ambient clouds. Non-refractory aerosol chemical composition was measured with an Aerodyne compact time-of-flight aerosol mass spectrometer. It was observed that the aerosols sampled downwind of the site on both days were composed predominantly of organics with a low degree of oxidation and low

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  3. Aerosol mixing state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    NASA Astrophysics Data System (ADS)

    Lance, S.; Raatikainen, T.; Onasch, T. B.; Worsnop, D. R.; Yu, X.-Y.; Alexander, M. L.; Stolzenburg, M. R.; McMurry, P. H.; Smith, J. N.; Nenes, A.

    2013-05-01

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic hygroscopicity parameter, κ*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions (forg) are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which predictions of the hygroscopicity parameter are compared against κ*. Strong diurnal changes in aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN at 0.51% ± 0.06% supersaturation can surpass by more than a factor of two the corresponding concentrations of 100 nm particles. We also find that at 06:00-08:00 LT throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally mixed fraction for 40 nm particles and 30% externally mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as "internally mixed". Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour" and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing state and the presence of refractory material not measured

  4. Competing effects of viscosity and surface-tension depression on the hygroscopicity and CCN activity of laboratory surrogates for oligomers in atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Shiraiwa, M.; Flagan, R. C.; Seinfeld, J.; Schilling, K.; Berkemeier, T.

    2015-12-01

    The presence of oligomers in biomass burning aerosol, as well as secondary organic aerosol derived from other sources, influences particle viscosity and can introduce kinetic limitations to water uptake. This, in turn, impacts aerosol optical properties and the efficiency with which these particles serve as cloud condensation nuclei (CCN). To explore the influence of organic-component viscosity on aerosol hygroscopicity, the water-uptake behavior of aerosol systems comprised of polyethylene glycol (PEG) and mixtures of PEG and ammonium sulfate (AS) was measured under sub- and supersaturated relative humidity (RH) conditions. Experiments were conducted with systems containing PEG with average molecular weights ranging from 200 to 10,000 g/mol, corresponding to a range in viscosity of 0.004 - 4.5 Pa s under dry conditions. While evidence suggests that viscous aerosol components can suppress water uptake at RH < 90%, under supersaturated conditions (with respect to RH), an increase in CCN activity with increasing PEG molecular weight was observed. We attribute this to an increase in the efficiency with which PEG serves as a surfactant with increasing molecular weight. This effect is most pronounced for PEG-AS mixtures and, in fact, a modest increase in CCN activity is observed for the PEG 10,000-AS mixture as compared to pure AS, as evidenced by a 4% reduction in critical activation diameter. Experimental results are compared with calculations of hygroscopic growth at thermodynamic equilibrium using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients model and the potential influence of kinetic limitations to observed water uptake is further explored with the Kinetic Multi-Layer Model of Gas-Particle Interactions. Results suggest the competing effects of organic-component viscosity and surface-tension depression may lead to RH-dependent differences in hygroscopicity for oligomers and other surface-active compounds present in atmospheric

  5. Organic component vapor pressures and hygroscopicities of aqueous aerosol measured by optical tweezers.

    PubMed

    Cai, Chen; Stewart, David J; Reid, Jonathan P; Zhang, Yun-hong; Ohm, Peter; Dutcher, Cari S; Clegg, Simon L

    2015-01-29

    Measurements of the hygroscopic response of aerosol and the particle-to-gas partitioning of semivolatile organic compounds are crucial for providing more accurate descriptions of the compositional and size distributions of atmospheric aerosol. Concurrent measurements of particle size and composition (inferred from refractive index) are reported here using optical tweezers to isolate and probe individual aerosol droplets over extended timeframes. The measurements are shown to allow accurate retrievals of component vapor pressures and hygroscopic response through examining correlated variations in size and composition for binary droplets containing water and a single organic component. Measurements are reported for a homologous series of dicarboxylic acids, maleic acid, citric acid, glycerol, or 1,2,6-hexanetriol. An assessment of the inherent uncertainties in such measurements when measuring only particle size is provided to confirm the value of such a correlational approach. We also show that the method of molar refraction provides an accurate characterization of the compositional dependence of the refractive index of the solutions. In this method, the density of the pure liquid solute is the largest uncertainty and must be either known or inferred from subsaturated measurements with an error of <±2.5% to discriminate between different thermodynamic treatments.

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

    EPA Science Inventory

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

  7. Variations in hygroscopic growth of sub- and super-micron sea spray aerosols during a phytoplankton bloom

    NASA Astrophysics Data System (ADS)

    Forestieri, S.; Jayarathne, T. S.; Stone, E. A.; Laskina, O.; Grassian, V. H.; Lee, C.; Sultana, C. M.; Moore, K.; Cornwell, G.; Novak, G.; Bertram, T. H.; Prather, K. A.; Cappa, C. D.

    2014-12-01

    Marine sea spray aerosols (SSA) make up an important portion of natural aerosols (prior to anthropogenic influence) and are therefore important in establishing the baseline for anthropogenic aerosol climate impacts. One way aerosols impact climate is by scattering solar radiation, and how much light is scattered depends upon the size of aerosols. Aerosols grow larger via water uptake and thus scatter more light at elevated relative humidities. This growth depends on composition. SSA can become enriched in organics during phytoplankton blooms, becoming less salty and therefore less hygroscopic. Aerosol hygroscopicity of SSA sampled during an in-lab phytoplankton bloom were measured during the CAICE-IMPACTS 2014 study. SSA were generated via breaking waves in an enclosed 33 m wave channel filled with natural seawater. Aerosol hygroscopicity was characterized by measuring light extinction at 532 nm of dry aerosols and of aerosols humidified to 85% relative humidity using a Cavity Ringdown Spectrometer. These optical growth factors (humidified extinction/dry extinction) were converted to physical growth factors using Mie Theory calculations and aerosol size distributions measured with a scanning electrical mobility spectrometer (SEMS) and an aerodynamic particle sizer (APS). Growth factors for super- and sub-micron SSA were quantified separately through the use of a PM2.5 cyclone or PM1 impactor. The observed SSA growth factors will be linked to SSA and source water chemical composition determined by both offline and online analysis of samples. The SSA bulk growth factors will also be compared with concurrent measurements of the efficiency with which SSA act as cloud condensation nuclei. Observed SSA growth factors will also be compared to offline hygroscopic growth measurements.

  8. Aerosol Size Distribution, Composition, and Hygroscopicity Measurements During CSTRIPE Using an Aerosol Mass Spectrometer and a Dual Differential Mobility Analyzer

    NASA Astrophysics Data System (ADS)

    Bahreini, R.; Varutbangkul, V.; Conant, W. C.; Flagan, R. C.; Seinfeld, J. H.; Buzorius, G.; Jonsson, H. H.

    2003-12-01

    During July 2003, the CIRPAS Twin Otter aircraft was deployed in the CSTRIPE (Coastal STRatocumulus Imposed Perturbation Experiment) field experiment in order to quantify the effects of aerosols on the microphysics and dynamics of marine stratocumulus clouds. In order to characterize the effects of different aerosol types on stratocumulus clouds, various air masses were sampled, including local fire plumes, pollution over the San Joaquin valley, unperturbed marine stratocumulus clouds, and stratocumulus clouds perturbed by seeding flares. Some research flights were also dedicated to characterize the seeding flares in the clear sky. Measurements of aerosol mass distribution and composition, using an Aerodyne Aerosol Mass Spectrometer (AMS), and size distribution and hygroscopic behavior, using a Dual Differential Mobility Analyzer (Dual DMA) with one column at dry conditions and another at a relative humidity of approximately 70 percent, will be presented here. During a number of in-cloud sampling periods, the Counter-flow Virtual Impactor (CVI) was used to select and dry cloud droplets, which were then analyzed by the AMS and the Dual DMA. The AMS composition measurements showed that sulfate and organics comprised most of the mass of the non-refractory components of the aerosol. The DMA showed a mixture of unimodal and bimodal size distributions in most types of air masses. The air mass over the San Joaquin valley, however, showed strong evidence of freshly nucleated particles, with aerosol number concentrations often above 80,000 cm-3.

  9. Estimation of surface-level PM concentration from satellite observation taking into account the aerosol vertical profiles and hygroscopicity.

    PubMed

    Kim, Kwanchul; Lee, Kwon H; Kim, Ji I; Noh, Youngmin; Shin, Dong H; Shin, Sung K; Lee, Dasom; Kim, Jhoon; Kim, Young J; Song, Chul H

    2016-01-01

    Surface-level PM10 distribution was estimated from the satellite aerosol optical depth (AOD) products, taking the account of vertical profiles and hygroscopicity of aerosols over Jeju, Korea during March 2008 and October 2009. In this study, MODIS AOD data from the Terra and Aqua satellites were corrected with aerosol extinction profiles and relative humidity data. PBLH (Planetary Boundary Layer Height) was determined from MPLNET lidar-derived aerosol extinction coefficient profiles. Through statistical analysis, better agreement in correlation (R = 0.82) between the hourly PM10 concentration and hourly average Sunphotometer AOD was the obtained when vertical fraction method (VFM) considering Haze Layer Height (HLH) and hygroscopic growth factor f(RH) was used. The validity of the derived relationship between satellite AOD and surface PM10 concentration clearly demonstrates that satellite AOD data can be utilized for remote sensing of spatial distribution of regional PM10 concentration. PMID:26421659

  10. Estimation of surface-level PM concentration from satellite observation taking into account the aerosol vertical profiles and hygroscopicity.

    PubMed

    Kim, Kwanchul; Lee, Kwon H; Kim, Ji I; Noh, Youngmin; Shin, Dong H; Shin, Sung K; Lee, Dasom; Kim, Jhoon; Kim, Young J; Song, Chul H

    2016-01-01

    Surface-level PM10 distribution was estimated from the satellite aerosol optical depth (AOD) products, taking the account of vertical profiles and hygroscopicity of aerosols over Jeju, Korea during March 2008 and October 2009. In this study, MODIS AOD data from the Terra and Aqua satellites were corrected with aerosol extinction profiles and relative humidity data. PBLH (Planetary Boundary Layer Height) was determined from MPLNET lidar-derived aerosol extinction coefficient profiles. Through statistical analysis, better agreement in correlation (R = 0.82) between the hourly PM10 concentration and hourly average Sunphotometer AOD was the obtained when vertical fraction method (VFM) considering Haze Layer Height (HLH) and hygroscopic growth factor f(RH) was used. The validity of the derived relationship between satellite AOD and surface PM10 concentration clearly demonstrates that satellite AOD data can be utilized for remote sensing of spatial distribution of regional PM10 concentration.

  11. The single scattering properties of hygroscopic soot aggregates with water coated monomers

    NASA Astrophysics Data System (ADS)

    YU, W.; Tianhai, C.; Hao, C.; Lijuan, Z.

    2013-12-01

    Anthropogenic aerosols, such as soot, have modified the Earth's radiation balance by scattering and absorbing solar and long-wave radiative transmission, which have largely influenced the global climate change since the industrial era. Based on transmission electron microscope images (TEM), soot particles are shown as the complex, fractal-like aggregate structures. In humid atmospheric environments, these soot aggregates tend to acquire a water coating, which introduces further complexity to the problem of determining the optical properties of the aggregates. The hygroscopic growth of soot aggregates is important for the aging of these absorbing aerosols, which can significantly influence the optical properties of these kinds of soot particles. In this paper, according to the specific volume fractions of soot core in the water coated soot particle, the monomers of fractal soot aggregates are modeled as semi-external mixtures (physical contact) with constant radius of soot core and variable size of water coating. The single scattering properties of these hygroscopic soot particles, such as phase function, the cross sections of extinction, absorption and scatting, single scattering albedo (SSA), and asymmetry parameter (ASY), are calculated using the numerically exact superposition T-matrix method. The morphological effects are compared with different monomer numbers and fractal dimension of the soot aggregates, as well as different size of water coating for these spherical monomers. The results have shown that the extinction and absorption cross sections are decreased for the soot aggregates with more thick water coating on monomers, but the single scattering albedo is increased for the larger water coating. It is found that the SSA of aged soot aggregates with hygroscopic grown are remarkably (~50% for volume fraction of soot aggregates is 0.5) larger than fresh soot particles without the consideration of water coating, due to the size of water coating and the

  12. Discontinuities in hygroscopic growth below and above water saturation for laboratory surrogates of oligomers in organic atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, Natasha; Zuend, Andreas; Schilling, Katherine; Berkemeier, Thomas; Shiraiwa, Manabu; Flagan, Richard C.; Seinfeld, John H.

    2016-10-01

    Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. However, uncertainty remains regarding the factors that contribute to observations of low hygroscopic growth below water saturation but enhanced cloud condensation nuclei (CCN) activity for a given aerosol population. Utilizing laboratory surrogates for oligomers in atmospheric aerosols, we explore the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors. Measurements of hygroscopic growth under subsaturated conditions and the CCN activity of aerosols comprised of polyethylene glycol (PEG) with average molecular masses ranging from 200 to 10 000 g mol-1 and mixtures of PEG with ammonium sulfate (AS) were conducted. Experimental results are compared to calculations of hygroscopic growth at thermodynamic equilibrium conducted with the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model, and the potential influence of kinetic limitations on observed water uptake was further explored through estimations of water diffusivity in the PEG oligomers. Particle-phase behavior, including the prevalence of liquid-liquid phase separation (LLPS), was also modeled with AIOMFAC. Under subsaturated relative humidity (RH) conditions, we observed little variability in hygroscopic growth across PEG systems with different molecular masses; however, an increase in CCN activity with increasing PEG molecular mass was observed. This effect is most pronounced for PEG-AS mixtures, and, in fact, an enhancement in CCN activity was observed for the PEG10000-AS mixture as compared to pure AS, as evidenced by a 15 % reduction in critical activation diameter at a supersaturation of 0.8 %. We also

  13. Effect of hygroscopic growth on the aerosol light-scattering coefficient: A review of measurements, techniques and error sources

    NASA Astrophysics Data System (ADS)

    Titos, G.; Cazorla, A.; Zieger, P.; Andrews, E.; Lyamani, H.; Granados-Muñoz, M. J.; Olmo, F. J.; Alados-Arboledas, L.

    2016-09-01

    Knowledge of the scattering enhancement factor, f(RH), is important for an accurate description of direct aerosol radiative forcing. This factor is defined as the ratio between the scattering coefficient at enhanced relative humidity, RH, to a reference (dry) scattering coefficient. Here, we review the different experimental designs used to measure the scattering coefficient at dry and humidified conditions as well as the procedures followed to analyze the measurements. Several empirical parameterizations for the relationship between f(RH) and RH have been proposed in the literature. These parameterizations have been reviewed and tested using experimental data representative of different hygroscopic growth behavior and a new parameterization is presented. The potential sources of error in f(RH) are discussed. A Monte Carlo method is used to investigate the overall measurement uncertainty, which is found to be around 20-40% for moderately hygroscopic aerosols. The main factors contributing to this uncertainty are the uncertainty in RH measurement, the dry reference state and the nephelometer uncertainty. A literature survey of nephelometry-based f(RH) measurements is presented as a function of aerosol type. In general, the highest f(RH) values were measured in clean marine environments, with pollution having a major influence on f(RH). Dust aerosol tended to have the lowest reported hygroscopicity of any of the aerosol types studied. Major open questions and suggestions for future research priorities are outlined.

  14. Hygroscopicity of aerosol particles and CCN activity of nearly hydrophobic particles in the urban atmosphere over Japan during summer

    NASA Astrophysics Data System (ADS)

    Ogawa, Shuhei; Setoguchi, Yoshitaka; Kawana, Kaori; Nakayama, Tomoki; Ikeda, Yuka; Sawada, Yuuki; Matsumi, Yutaka; Mochida, Michihiro

    2016-06-01

    We investigated the hygroscopicity of 150 nm particles and the number-size distributions and the cloud condensation nuclei (CCN) activity of nearly hydrophobic particles in aerosols over Nagoya, Japan, during summer. We analyzed the correlations between the number concentrations of particles in specific hygroscopic growth factor (g) ranges and the mass concentrations of chemical components. This analysis suggests the association of nearly hydrophobic particles with hydrocarbon-like organic aerosol, elemental carbon and semivolatile oxygenated organic aerosol (SV-OOA), that of less hygroscopic particles with SV-OOA and nitrate and that of more hygroscopic particles with low-volatile oxygenated organic aerosol (LV-OOA) and sulfate. The hygroscopicity parameter (κ) of organics was derived based on the g distributions and chemical composition of 150 nm particles. The κ of the organics correlated positively with the fraction of the total organic mass spectral signal at m/z 44 and the volume fraction of the LV-OOA to the organics, indicating that organics with highly oxygenated structures including carboxylic acid groups contribute to the water uptake. The number-size distributions of the nearly hydrophobic particles with g around 1.0 and 1.1 correlated with the mass concentrations of chemical components. The results show that the chemical composition of the particles with g around 1.0 was different between the Aitken mode and the accumulation mode size ranges. An analysis for a parameter Fmax of the curves fitted to the CCN efficiency spectra of the particles with g around 1.0 suggests that the coating by organics associated with SV-OOA elevated the CCN activity of these particles.

  15. Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

    NASA Astrophysics Data System (ADS)

    Forestieri, Sara D.; Cornwell, Gavin C.; Helgestad, Taylor M.; Moore, Kathryn A.; Lee, Christopher; Novak, Gordon A.; Sultana, Camille M.; Wang, Xiaofei; Bertram, Timothy H.; Prather, Kimberly A.; Cappa, Christopher D.

    2016-07-01

    The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative

  16. Hygroscopic properties of internally mixed particles composed of NaCl and water-soluble organic acids.

    PubMed

    Ghorai, Suman; Wang, Bingbing; Tivanski, Alexei; Laskin, Alexander

    2014-02-18

    Atmospheric aging of naturally emitted marine aerosol often leads to formation of internally mixed particles composed of sea salts and water-soluble organic compounds of anthropogenic origin. Mixing of sea salt and organic components has profound effects on the evolving chemical composition and hygroscopic properties of the resulted particles, which are poorly understood. Here, we have studied chemical composition and hygroscopic properties of laboratory generated NaCl particles mixed with malonic acid (MA) and glutaric acid (GA) at different molar ratios using micro-FTIR spectroscopy, atomic force microscopy, and X-ray elemental microanalysis. Hygroscopic properties of internally mixed NaCl and organic acid particles were distinctly different from pure components and varied significantly with the type and amount of organic compound present. Experimental results were in a good agreement with the AIM modeling calculations of gas/liquid/solid partitioning in studied systems. X-ray elemental microanalysis of particles showed that Cl/Na ratio decreased with increasing organic acid component in the particles with MA yielding lower ratios relative to GA. We attribute the depletion of chloride to the formation of sodium malonate and sodium glutarate salts resulted by HCl evaporation from dehydrating particles. PMID:24437520

  17. Hygroscopic Properties of Internally Mixed Particles Composed of NaCl and Water-Soluble Organic Acids

    SciTech Connect

    Ghorai, Suman; Wang, Bingbing; Tivanski, Alexei V.; Laskin, Alexander

    2014-02-18

    Atmospheric aging of naturally emitted marine aerosol often leads to formation of internally mixed particles composed of sea salts and water soluble organic compounds of anthropogenic origin. Mixing of sea salt and organic components has profound effects on the evolving chemical composition and hygroscopic properties of the resulted particles, which are poorly understood. Here, we have studied chemical composition and hygroscopic properties of laboratory generated NaCl particles mixed with malonic acid (MA) and glutaric acid (GA) at different molar ratios using micro-FTIR spectroscopy and X-ray elemental microanalysis.Hygroscopic properties of inte rnally mixed NaCl and organic acid particles were distinctly different from pure components and varied significantly with the type and amount of organic compound present. Experimental results were in a good agreement with the AIM modeling calculations of gas/liquid/solid partitioning in studied systems. X-ray elemental microanalysis of particles showed that Cl/Na ratio decreased with increasing organic acid component in the particles with MA yielding lower ratios relative to GA. We attribute the depletion of chloride to the formation of Na-malonate and Na-glutarate salts resulted by HCl evaporation from dehydrating particles.

  18. Beyond the Alphabet Soup: Molecular Properties of Aerosol Components Influence Optics. (Invited)

    NASA Astrophysics Data System (ADS)

    Thompson, J. E.

    2013-12-01

    Components within atmospheric aerosols exhibit almost every imaginable model of chemical bonding and physical diversity. The materials run the spectrum from crystalline to amorphous, covalent to ionic, and have varying viscosities, phase, and hygroscopicity. This seminar will focus on the molecular properties of materials that influence the optical behavior of aerosols. Special focus will be placed on the polarizability of materials, hygroscopic growth, and particle phase.

  19. Direct measurements of the optical cross sections and refractive indices of individual volatile and hygroscopic aerosol particles.

    PubMed

    Mason, B J; Cotterell, M I; Preston, T C; Orr-Ewing, A J; Reid, J P

    2015-06-01

    We present measurements of the evolving extinction cross sections of individual aerosol particles (spanning 700-2500 nm in radius) during the evaporation of volatile components or hygroscopic growth using a combination of a single particle trap formed from a Bessel light beam and cavity ring-down spectroscopy. For single component organic aerosol droplets of 1,2,6-hexanetriol, polyethylene glycol 400, and glycerol, the slow evaporation of the organic component (over time scales of 1000 to 10,000 s) leads to a time-varying size and extinction cross section that can be used to estimate the refractive index of the droplet. Measurements on binary aqueous-inorganic aerosol droplets containing one of the inorganic solutes ammonium bisulfate, ammonium sulfate, sodium nitrate, or sodium chloride (over time scales of 1000 to 15,000 s) under conditions of changing relative humidity show that extinction cross-section measurements are consistent with expectations from accepted models for the variation in droplet refractive index with hygroscopic growth. In addition, we use these systems to establish an experimental protocol for future single particle extinction measurements. The advantages of mapping out the evolving light extinction cross-section of an individual particle over extended time frames accompanied by hygroscopic cycling or component evaporation are discussed.

  20. Phase, morphology, and hygroscopicity of mixed oleic acid/sodium chloride/water aerosol particles before and after ozonolysis.

    PubMed

    Dennis-Smither, Benjamin J; Hanford, Kate L; Kwamena, Nana-Owusua A; Miles, Rachael E H; Reid, Jonathan P

    2012-06-21

    Aerosol optical tweezers are used to probe the phase, morphology, and hygroscopicity of single aerosol particles consisting of an inorganic component, sodium chloride, and a water insoluble organic component, oleic acid. Coagulation of oleic acid aerosol with an optically trapped aqueous sodium chloride droplet leads to formation of a phase-separated particle with two partially engulfed liquid phases. The dependence of the phase and morphology of the trapped particle with variation in relative humidity (RH) is investigated by cavity enhanced Raman spectroscopy over the RH range <5% to >95%. The efflorescence and deliquescence behavior of the inorganic component is shown to be unaffected by the presence of the organic phase. Whereas efflorescence occurs promptly (<1 s), the deliquescence process requires both dissolution of the inorganic component and the adoption of an equilibrium morphology for the resulting two phase particle, occurring on a time-scale of <20 s. Comparative measurements of the hygroscopicity of mixed aqueous sodium chloride/oleic acid droplets with undoped aqueous sodium chloride droplets show that the oleic acid does not impact on the equilibration partitioning of water between the inorganic component and the gas phase or the time response of evaporation/condensation. The oxidative aging of the particles through reaction with ozone is shown to increase the hygroscopicity of the organic component.

  1. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2015-06-01

    Even though organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments spanning from the subtropics to the high Arctic, their hygroscopic properties have not been investigated prior to this study. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesized and used for simultaneous measurements with a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Cloud Condensation Nuclei Counter (CCNC) to determine the hygroscopicity parameter, κ, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The κ values derived from measurements with H-TDMA decreased with increasing particle dry size for all chemical compositions investigated, indicating size dependency and/or surface effects. For pure L-OS 250, κ was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in κ between the sub- and supersaturated measurements were observed for L-OS 250, whereas κ of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical activation diameter and κ for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with ≥ 20 % w/w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24 % from the pure water-value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of κ obtained from the

  2. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2015-12-01

    Organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments; however their hygroscopic properties remain uncharacterised. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesised and used for simultaneous measurements with a hygroscopicity tandem differential mobility analyser (H-TDMA) and a cloud condensation nuclei counter (CCNC) to determine the hygroscopicity parameter, κ, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The κ values derived from measurements with H-TDMA decreased with increasing particle dry diameter for all chemical compositions investigated, indicating that κH-TDMA depends on particle diameter and/or surface effects; however, it is not clear if this trend is statistically significant. For pure L-OS 250, κ was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in κ between the sub- and supersaturated measurements were observed for L-OS 250, whereas κ of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical particle diameter and κ for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with ≥ 20 % w / w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24 % from the pure water value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of κ

  3. Aerosol mixingstate, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    SciTech Connect

    Lance, Sara; Raatikainen, T.; Onasch, Timothy B.; Worsnop, Douglas R.; Yu, Xiao-Ying; Alexander, M. L.; Stolzenberg, Mark; McMurry, Peter; Smith, James N.; Nenes, Athanasios

    2013-05-15

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. K¨ohler theory is used to evaluate the characteristic water uptake coefficient, k*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions, (forg), are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which kAMS is inferred and compared against k*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased k* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% +/- 0.06%. We also find that at 0600-0800 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as “internally-mixed”. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning “rush hour”, and the entire campaign. We show that k* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for k* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the

  4. Aerosol mixing-state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    NASA Astrophysics Data System (ADS)

    Lance, S.; Raatikainen, T.; Onasch, T.; Worsnop, D. R.; Yu, X.-Y.; Alexander, M. L.; Stolzenburg, M. R.; McMurry, P. H.; Smith, J. N.; Nenes, A.

    2012-06-01

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic water uptake coefficient, κ*, for the CCN active aerosol population using both size-resolved HTDMA and size-resolved CCNc measurements. Organic mass fractions, forg, are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which κAMS is inferred and compared against κ*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% ± 0.06%. We also find that at 06:00-08:00 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as internally-mixed. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour", and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the AMS

  5. Hygroscopic growth of size-resolved, emission-source classified, aerosol particles sampled across the United States

    NASA Astrophysics Data System (ADS)

    Shingler, T.; Crosbie, E. C.; Ziemba, L. D.; Anderson, B. E.; Campuzano Jost, P.; Jimenez, J. L.; Mikoviny, T.; Wisthaler, A.; Sorooshian, A.

    2014-12-01

    The hygroscopic growth of atmospheric aerosol particles is a key air quality parameter, impacting the radiation budget, visibility, and cloud formation. During the DC3 and SEAC4RS field campaigns (>300 total flight hours), measurements were made over 32 US states, Canada, the Pacific Ocean, and the Gulf of Mexico, between the surface and 41,000 feet ASL. The aircraft research payloads included a suite of in-situ aerosol and gas phase instruments. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) and the Langley Aerosol Research Group Experiment (LARGE) humidified nephelometer instrument applied different techniques to measure water uptake by aerosol particles at prescribed relative humidity values. Size-resolved growth factor (GF ≡ Dp,wet/Dp,dry) measurements by the DASH-SP are compared to bulk scattering measurements (f(RH) ≡ σscat,wet/σscat,dry) by the LARGE instrument. Spatial location and volatile organic compound tracers such as isoprene and acetonitrile are used to classify the origin of distinct air masses, including: forest fires, biogenic-emitting forests, agricultural use lands, marine boundary layer, urban, and rural background. Analyses of GF results by air mass origin are reported and results are compared with f(RH) measurements. A parameterization between the f(RH) and GF measurements and its potential uses are discussed.

  6. Aging of secondary organic aerosol from small aromatic VOCs. Changes in chemical composition, mass yield, volatility and hygroscopicity

    DOE PAGES

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2014-12-12

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form and transform SOA from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx. The effects of chemical aging on organic aerosol (OA) composition, mass yield, volatility and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state OSC) and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OSmore » C ranged from -0.29 to 0.45 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  7. Size Resolved measurements of aerosol hygroscopicity and mixing state during Green Ocean Amazon (GoAmazon) 2014

    NASA Astrophysics Data System (ADS)

    Thalman, R. M.; Artaxo, P.; Campuzano Jost, P.; Barbosa, H. M.; Day, D. A.; de Sá, S. S.; Hu, W.; Jimenez, J. L.; Kuang, C.; Palm, B. B.; Krüger, M. L.; Manzi, A. O.; Martin, S. T.; Poeschl, U.; Sedlacek, A. J., III; Senum, G.; Souza, R. A. F. D.; Springston, S. R.; Alexander, M. L.; Watson, T. B.; Wang, J.

    2014-12-01

    Measurements of size-resolved cloud condensation nucleai (CCN) spectra were performed at the T3 site of the Green Ocean Amazon (GoAmazon) field project located near Manacapuru, Brazil during 2014. The T3 site is a receptor site for both polluted urban down-wind (Manaus, BR a city of several million 70 km up wind) and background (Amazon rainforest) air-masses and can provide a contrast between clean and polluted conditions. Particle hygroscopicity (kappa) and mixing state were calculated from the particle activation spectrum measured by size selecting aerosols and exposing them to a wide range of supersaturation in the CCN counter (Droplet Measurement Technologies Continuous-Flow Streamwise Thermal Gradient CCN Chamber). The supersaturation was varied between 0.07 and 1.1% by changing a combination of both total flow rate and temperature gradient in the CCN counter. Measured spectra were examined for air masses with different level of influence from Manaus plume. Particle hygroscopicity generally peaked near noon local time which was broadly consistent with the trend in aerosol sulfate. The average kappa values during the first intensive operation period were 0.14±0.05, 0.14±0.04 and 0.16±0.06 for 75, 112 and 171 nm particles respectively. Evaluation of particle hygroscopicity and dispersion (mixing state) will be presented with respect to size and level of pollution.

  8. Interaction of aerosol particles composed of protein and salts with water vapor: hygroscopic growth and microstructural rearrangement

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Niessner, R.; Pöschl, U.

    2003-09-01

    decomposition products NH3 and HNO3. The efflorescence threshold of NaCl-BSA particles decreased with increasing BSA dry mass fraction, i.e. the protein inhibited the formation of salt crystals and enhanced the stability of supersaturated solution droplets. The H-TDMA and TEM results indicate that the protein was enriched at the surface of the mixed particles and formed an envelope, which inhibits the access of water vapor to the particle core and leads to kinetic limitations of hygroscopic growth, phase transitions, and microstructural rearrangement processes. Besides these surface and kinetic effects, proteins and comparable organic macromolecules may also influence the thermodynamic properties of the aqueous bulk solution (solubilities, vapor pressures, and chemical equilibria, e.g. for the decomposition and evaporation of NH4NO3. The observed effects should be taken into account in the analysis of data from laboratory experiments and field measurements and in the modelling of aerosol processes involving water vapor and particles with complex composition. They can strongly influence experimental results, and depending on ambient conditions they may also play a significant role in the atmosphere (deliquescence, efflorescence, and CCN activation of particles). In fact, irregular hygroscopic growth curves similar to the ones observed in this study have recently been reported from H-TDMA experiments with water-soluble organics extracted from real air particulate matter and with humic-like substances. The Köhler theory calculations performed with different models demonstrate that the hygroscopic growth of particles composed of inorganic salts and proteins can be efficiently described with a simple volume additivity approach, provided that the correct dry solute mass equivalent diameter and composition are known. A simple parameterisation of the osmotic coefficient has been derived from an osmotic pressure virial equation and appears to be well-suited for proteins and comparable

  9. Estimating aerosol light-scattering enhancement from dry aerosol optical properties at different sites

    NASA Astrophysics Data System (ADS)

    Titos, Gloria; Jefferson, Anne; Sheridan, Patrick; Andrews, Elisabeth; Lyamani, Hassan; Ogren, John; Alados-Arboledas, Lucas

    2014-05-01

    Microphysical and optical properties of aerosol particles are strongly dependent on the relative humidity (RH). Knowledge of the effect of RH on aerosol optical properties is of great importance for climate forcing calculations and for comparison of in-situ measurements with satellite and remote sensing retrievals. The scattering enhancement factor, f(RH), is defined as the ratio of the scattering coefficient at a high and reference RH. Predictive capability of f(RH) for use in climate models would be enhanced if other aerosol parameters could be used as proxies to estimate hygroscopic growth. Toward this goal, we explore the relationship between aerosol light-scattering enhancement and dry aerosol optical properties such as the single scattering albedo (SSA) and the scattering Ångström exponent (SAE) at multiple sites around the world. The measurements used in this study were conducted by the US Department of Energy at sites where different aerosol types predominate (pristine marine, polluted marine, dust dominated, agricultural and forest environments, among others). In all cases, the scattering enhancement decreases as the SSA decreases, that is, as the contribution of absorbing particles increases. On the other hand, for marine influenced environments the scattering enhancement clearly increases as the contribution of coarse particles increases (SAE decreases), evidence of the influence of hygroscopic coarse sea salt particles. For other aerosol types the relationship between f(RH) and SAE is not so straightforward. Combining all datasets, f(RH) was found to exponentially increase with SSA with a high correlation coefficient.

  10. Properties of jet engine combustion particles during the PartEmis experiment. Hygroscopic growth at supersaturated conditions

    NASA Astrophysics Data System (ADS)

    Hitzenberger, R.; Giebl, H.; Petzold, A.; Gysel, M.; Nyeki, S.; Weingartner, E.; Baltensperger, U.; Wilson, C. W.

    2003-07-01

    During the EU Project PartEmis, the microphysical properties of aircraft combustion aerosol were investigated. This study is focused on the ability of exhaust aerosols to act as cloud condensation nuclei (CCN). The combustor was operated at two different conditions representing old and modern aircraft engine technology. CCN concentrations were measured with the University of Vienna CCN counter [ Giebl et al., 2002] at supersaturations around 0.7%. The activation ratio (fraction of CCN in total aerosol) depended on the fuel sulphur content (FSC) and also on the operation conditions. CCN/CN ratios increased from 0.93 through 1.43 to 5.15 . 10-3 (old cruise conditions) and 0.67 through 3.04 to 7.94 . 10-3 (modern cruise conditions) when FSC increased from 50 through 410 to1270 μg/g. The activation behaviour was modelled using classical theories and with a semi-empirical model [ Gysel et al., 2003] based on measured hygroscopicity of the aerosol under subsaturated conditions, which gave the best agreement.

  11. Aerosol Activity and Hygroscopicity Combined with Lidar Data in the Urban Atmosphere of Athens, Greece in the Frame of the HYGRA_CD Campaign

    NASA Astrophysics Data System (ADS)

    Bougiatioti, Aikaterini; Papayannis, Alexandros; Vratolis, Stergios; Argyrouli, Athina; Mihalopoulos, Nikolaos; Tsagkaraki, Maria; Nenes, Athanasios; Eleftheriadis, Konstantinos

    2016-06-01

    Measurements of cloud condensation nuclei (CCN) concentrations between 0.2-1.0% supersaturation and aerosol size distribution were performed at an urban background site of Athens during HygrA-CD. The site is affected by local and long-range transported emissions as portrayed by the external mixing of the particles, as the larger ones appear to be more hygroscopic and more CCN-active than smaller ones. Activation fractions at all supersaturations exhibit a diurnal variability with minimum values around noon, which are considerably lower than unity. This reinforces the conclusion that the aerosol is mostly externally mixed between "fresher", less hygroscopic components with more aged, CCN active constituents.

  12. Measurements of the evaporation and hygroscopic response of single fine-mode aerosol particles using a Bessel beam optical trap.

    PubMed

    Cotterell, Michael I; Mason, Bernard J; Carruthers, Antonia E; Walker, Jim S; Orr-Ewing, Andrew J; Reid, Jonathan P

    2014-02-01

    A single horizontally-propagating zeroth order Bessel laser beam with a counter-propagating gas flow was used to confine single fine-mode aerosol particles over extended periods of time, during which process measurements were performed. Particle sizes were measured by the analysis of the angular variation of light scattered at 532 nm by a particle in the Bessel beam, using either a probe beam at 405 nm or 633 nm. The vapour pressures of glycerol and 1,2,6-hexanetriol particles were determined to be 7.5 ± 2.6 mPa and 0.20 ± 0.02 mPa respectively. The lower volatility of hexanetriol allowed better definition of the trapping environment relative humidity profile over the measurement time period, thus higher precision measurements were obtained compared to those for glycerol. The size evolution of a hexanetriol particle, as well as its refractive index at wavelengths 532 nm and 405 nm, were determined by modelling its position along the Bessel beam propagation length while collecting phase functions with the 405 nm probe beam. Measurements of the hygroscopic growth of sodium chloride and ammonium sulfate have been performed on particles as small as 350 nm in radius, with growth curves well described by widely used equilibrium state models. These are the smallest particles for which single-particle hygroscopicity has been measured and represent the first measurements of hygroscopicity on fine mode and near-accumulation mode aerosols, the size regimes bearing the most atmospheric relevance in terms of loading, light extinction and scattering. Finally, the technique is contrasted with other single particle and ensemble methods, and limitations are assessed.

  13. Measurements of the evaporation and hygroscopic response of single fine-mode aerosol particles using a Bessel beam optical trap.

    PubMed

    Cotterell, Michael I; Mason, Bernard J; Carruthers, Antonia E; Walker, Jim S; Orr-Ewing, Andrew J; Reid, Jonathan P

    2014-02-01

    A single horizontally-propagating zeroth order Bessel laser beam with a counter-propagating gas flow was used to confine single fine-mode aerosol particles over extended periods of time, during which process measurements were performed. Particle sizes were measured by the analysis of the angular variation of light scattered at 532 nm by a particle in the Bessel beam, using either a probe beam at 405 nm or 633 nm. The vapour pressures of glycerol and 1,2,6-hexanetriol particles were determined to be 7.5 ± 2.6 mPa and 0.20 ± 0.02 mPa respectively. The lower volatility of hexanetriol allowed better definition of the trapping environment relative humidity profile over the measurement time period, thus higher precision measurements were obtained compared to those for glycerol. The size evolution of a hexanetriol particle, as well as its refractive index at wavelengths 532 nm and 405 nm, were determined by modelling its position along the Bessel beam propagation length while collecting phase functions with the 405 nm probe beam. Measurements of the hygroscopic growth of sodium chloride and ammonium sulfate have been performed on particles as small as 350 nm in radius, with growth curves well described by widely used equilibrium state models. These are the smallest particles for which single-particle hygroscopicity has been measured and represent the first measurements of hygroscopicity on fine mode and near-accumulation mode aerosols, the size regimes bearing the most atmospheric relevance in terms of loading, light extinction and scattering. Finally, the technique is contrasted with other single particle and ensemble methods, and limitations are assessed. PMID:24346588

  14. Characterization of solvent-extractable organics in urban aerosols based on mass spectrum analysis and hygroscopic growth measurement.

    PubMed

    Mihara, Toshiyuki; Mochida, Michihiro

    2011-11-01

    To characterize atmospheric particulate organics with respect to polarity, aerosol samples collected on filters in the urban area of Nagoya, Japan, in 2009 were extracted using water, methanol, and ethyl acetate. The extracts were atomized and analyzed using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a hygroscopicity tandem differential mobility analyzer. The atmospheric concentrations of the extracted organics were determined using phthalic acid as a reference material. Comparison of the organic carbon concentrations measured using a carbon analyzer and the HR-ToF-AMS suggests that organics extracted with water (WSOM) and ethyl acetate (EASOM) or those extracted with methanol (MSOM) comprise the greater part of total organics. The oxygen-carbon ratios (O/C) of the extracted organics varied: 0.51-0.75 (WSOM), 0.37-0.48 (MSOM), and 0.27-0.33 (EASOM). In the ion-group analysis, WSOM, MSOM, and EASOM were clearly characterized by the different fractions of the CH and CO(2) groups. On the basis of the hygroscopic growth measurements of the extracts, κ of organics at 90% relative humidity (κ(org)) were estimated. Positive correlation of κ(org) with O/C (r 0.70) was found for MSOM and EASOM, but no clear correlation was found for WSOM.

  15. A case study of Asian dust storm particles: chemical composition, reactivity to SO2 and hygroscopic properties.

    PubMed

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

    2012-01-01

    Mineral dust comprises a great fraction of the global aerosol loading, but remains the largest uncertainty in predictions of the future climate due to its complexity in composition and physico-chemical properties. In this work, a case study characterizing Asian dust storm particles was conducted by multiple analysis methods, including SEM-EDS, XPS, FT-IR, BET, TPD/mass and Knudsen cell/mass. The morphology, elemental fraction, source distribution, true uptake coefficient for SO2, and hygroscopic behavior were studied. The major components of Asian dust storm particles are aluminosilicate, SiO2 and CaCO3, with organic compounds and inorganic nitrate coated on the surface. It has a low reactivity towards SO2 with a true uptake coefficient, 5.767 x 10(-6), which limits the conversion of SO2 to sulfate during dust storm periods. The low reactivity also means that the heterogeneous reactions of SO2 in both dry and humid air conditions have little effect on the hygroscopic behavior of the dust particles. PMID:22783615

  16. The Effect Of Organic Surfactants On The Properties Of Common Hygroscopic Particles: Effective Densities, Reactivity And Water Evaporation Of Surfactant Coated Particles

    NASA Astrophysics Data System (ADS)

    Cuadrarodriguez, L.; Zelenyuk, A.; Imre, D.; Ellison, B.

    2006-12-01

    Measurements of atmospheric aerosol compositions routinely show that organic compounds account for a very large fraction of the particle mass. The organic compounds that make up this aerosol mass represent a wide range of molecules with a variety of properties. Many of the particles are composed of hygroscopic salts like sulfates, nitrates and sea-salt internally mixed with organics. While the properties of the hygroscopic salts are known, the effect of the organic compounds on the microphysical and chemical properties which include CCN activity is not clear. .One particularly interesting class of internally mixed particles is composed of aqueous salts solutions that are coated with organic surfactants which are molecules with long aliphatic chain and a water soluble end. Because these molecules tend to coat the particles' surfaces, a monolayer might be sufficient to drastically alter their hygroscopic properties, their CCN activity, and reactivity. The aliphatic chains, being exposed to the oxidizing atmosphere are expected to be transformed through heterogeneous chemistry, yielding complex products with mixed properties. We will report the results from a series of observations on ammonium sulfate, sodium chloride and sea salt particles coated with three types of surfactant molecules: sodium lauryl sulfate, sodium oleate and laurtrimonium chloride. We have been able to measure the effective densities of internally mixed particles with a range of surfactant concentration that start below a monolayer and extend all the way to particles composed of pure surfactant. For many of the measurements the data reveal a rather complex picture that cannot be simply interpreted in terms of the known pure-compound densities. For unsaturated hydrocarbons we observed and quantified the effect of oxidation by ozone on particle size, effective density and individual particle mass spectral signatures. One of the more important properties of these surfactants is that they can form a

  17. Raman lidar observations of particle hygroscopicity during COPS

    NASA Astrophysics Data System (ADS)

    Stelitano, D.; Di Girolamo, P.; Summa, D.

    2012-04-01

    The characterization of particle hygroscopicity has primary importance for climate monitoring and prediction. Model studies have demonstrated that relative humidity (RH) has a critical influence on aerosol climate forcing. The relationship between aerosol backscattering and relative humidity has been investigated in numerous studies (among others, Pahlow et al., 2006; Wulfmeyer and Feingold, 2000; Veselovskii et al., 2009). Hygroscopic properties of aerosols influence particle size distribution and refractive index and hence their radiative effects. Aerosol particles tend to grow at large relative humidity values as a result of their hygroscopicity. Raman lidars with aerosol, water vapour and temperature measurement capability are potentially attractive tools for studying aerosol hygroscopicity as in fact they can provide continuous altitude-resolved measurements of particle optical, size and microphysical properties, as well as relative humidity, without perturbing the aerosols or their environment. Specifically, the University of Basilicata Raman lidar system (BASIL) considered for the present study, has the capability to perform all-lidar measurements of relative humidity based on the application of both the rotational and the vibrational Raman lidar techniques in the UV. BASIL was operational in Achern (Black Forest, Lat: 48.64 ° N, Long: 8.06 ° E, Elev.: 140 m) between 25 May and 30 August 2007 in the framework of the Convective and Orographically-induced Precipitation Study (COPS). During COPS, BASIL collected more than 500 hours of measurements, distributed over 58 measurement days and 34 intensive observation periods (IOPs). The present analysis is focused on selected case studies characterized by the presence of different aerosol types with different hygroscopic behaviour. The observed behaviour, dependent upon aerosol composition, may range from hygrophobic to strongly hygroscopic. Results from the different case studies will be illustrated and

  18. Quantifying the Relationship between Organic Aerosol Composition and Hygroscopicity/CCN Activity

    SciTech Connect

    Ziemann, Paul J.; Kreidenweis, Sonia M.; Petters, Markus D.

    2013-06-30

    The overall objective for this project was to provide the data and underlying process level understanding necessary to facilitate the dynamic treatment of organic aerosol CCN activity in future climate models. The specific objectives were as follows: (1) employ novel approaches to link organic aerosol composition and CCN activity, (2) evaluate the effects of temperature and relative humidity on organic aerosol CCN activity, and (3) develop parameterizations to link organic aerosol composition and CCN activity.

  19. Modeling of aerosol properties related to direct climate forcing

    NASA Astrophysics Data System (ADS)

    Koloutsou-Vakakis, Sotiria; Rood, Mark J.; Nenes, Athanasios; Pilinis, Christodoulos

    1998-07-01

    A long-term local experiment was designed with the purpose to accurately quantify aerosol parameters needed in order to estimate aerosol climate forcing at an anthropogenically perturbed continental site. Total light-scattering σλ,sp and backscattering σλ,bsp coefficients at wavelength λ, the hygroscopic growth factors with respect to scattering, ƒ(RH)λ,s, and the backscatter ratio bλ are the parameters considered in the paper. Reference and controlled relative humidity nephelometry measurements were taken at a ground level field sampling station, located near Bondville Illinois (40°03'12″N, W 88°22'19″W). Aerosol particle chemical composition and mass particle size distributions were also measured. The target parameters were also estimated from models. The modeling approach involved a two-step process. In the first step, aerosol properties were parameterized with an approach that made use of a modified thermodynamic equilibrium model, published laboratory measurements of single hygroscopic particle properties, and empirical mixing rules. In the second step, the parameterized aerosol properties were used as inputs into a code that calculate σλ,sp and σλ,bsp as functions of λ, RH, particle size, and composition. Comparison between the measured and the modeled results showed that depending on the assumptions, the differences between the modeled and observed results were within 5 to 28% for ƒ(RH)λ,s and within 22-35% for bλ at low RH and 0-20% for bλ at high RH. The temporal variation of the particle size distribution, the equilibrium state of the particles, and the hygroscopicity of the material characterized as residual were the major factors limiting the predictive ability of the models.

  20. Influence of biomass burning on CCN number and hygroscopicity during summertime in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Bougiatioti, A.; Bezantakos, S.; Stavroulas, I.; Kalivitis, N.; Kokkalis, P.; Biskos, G.; Mihalopoulos, N.; Papayannis, A.; Nenes, A.

    2015-08-01

    This study investigates the CCN activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean. Air masses sampled were subject to a range of atmospheric processing (several hours up to 3 days). Values of the hygroscopicity parameter, κ, were derived from cloud condensation nuclei (CCN) measurements and a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA). An Aerosol Chemical Speciation Monitor (ACSM) was also used to determine the chemical composition and mass concentration of non-refractory components of the submicron aerosol fraction. During fire events, the increased organic content (and lower inorganic fraction) of the aerosol decreases the hygroscopicity parameter, κ, for all particle sizes. The reason, however, for this decrease was not the same for all size modes; smaller particle sizes appeared to be richer in less hygroscopic, less CCN-active components due to coagulation processes while larger particles become less hygroscopic during the biomass burning events due to condensation of less hygroscopic gaseous compounds. In addition, smaller particles exhibited considerable chemical dispersion (where hygroscopicity varied up to 100 % for particles of same size); larger particles, however, exhibited considerably less dispersion owing to the effects of aging and retained high levels of CCN activity. These conclusions are further supported by the observed mixing state determined by the HTDMA measurements. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles and a large fraction of the CCN concentrations sampled. Based on Positive Matrix Factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend with the BBOA component, with enhancements of CCN in biomass burning plumes ranging between 65 and 150 %, for supersaturations ranging between 0.2 and 0.7 %. Using multilinear regression, we determine the

  1. A case study of single hygroscopicity parameter and its link to the functional groups and phase transition for urban aerosols in Taipei City

    NASA Astrophysics Data System (ADS)

    Hung, Hui-Ming; Hsu, Chia-Hung; Lin, Wei-Ting; Chen, Yu-Quan

    2016-05-01

    The hygroscopicity, functional groups and phase transitions of urban aerosol particles in Taipei City were studied using a cloud condensation nuclei counter (CCNc) with a scanning mobility particle sizer (SMPS) and an attenuated total reflectance with infrared (ATR-IR) detection technique. With the assumption of larger particles being activated first, the derived single hygroscopicity parameter (κ) exhibited an increasing trend with particle size, i.e., from 0.022 ± 0.01 at 87 ± 10 nm to 0.13 ± 0.03 at 240 ± 20 nm. The collected size-selected particles were characterized using ATR-IR for the functional groups of alkyl, carbonyl, ammonium, sulfate and nitrate, which showed various size dependence patterns, linked to different formation mechanisms. The hygroscopic response based on the ratio (xW_solute) for sample film of absorption by the enhanced water-stretching peak to that by the selected solute showed a better consistency with pure ammonium sulfate for sub-micron size particles. Based on the derived ammonium sulfate volume fraction from IR analysis, the κ received from CCNc measurements was concluded mainly contributed by ammonium sulfate for sub-micrometer particles. The increasing trend of sodium nitrate absorbance at aerosol diameter ≥1 μm was due to a reaction of nitric acid with sea salt particles. The micrometer sized particles were apparent not only in a significantly higher xW_solute than pure sodium nitrate but also had a deliquescence RH of 69 ± 1%, similar to that of sodium nitrate-sodium chloride mixtures. Overall, the organic species in this study exhibited a low hygroscopicity with less than 0.036 of contribution for the overall κ, and the major hygroscopic material of urban aerosols consisted primarily of ammonium sulfate in the sub-micrometer particles and sodium nitrate with sea salt in the coarse particles.

  2. Aerosol activation properties and CCN closure during TCAP

    NASA Astrophysics Data System (ADS)

    Mei, F.; Tomlinson, J. M.; Shilling, J. E.; Wilson, J. M.; Zelenyuk, A.; Chand, D.; Comstock, J. M.; Hubbe, J.; Berg, L. K.; Schmid, B.

    2013-12-01

    The indirect effects of atmospheric aerosols currently remain the most uncertain components in forcing of climate change over the industrial period (IPCC, 2007). This large uncertainty is partially due to our incomplete understanding of the ability of particles to form cloud droplets under atmospherically relevant supersaturation. In addition, there is a large uncertainty in the aerosol optical depth (AOD) simulated by climate models near the North American coast and a wide variety in the types of clouds are observed over this region. The goal of the US Department of Energy Two Column Aerosol Project (TCAP) is to understand the processes responsible for producing and maintaining aerosol distributions and associated radiative and cloud forcing off the coast of North America. During the TCAP study, aerosol total number concentration, cloud condensation nuclei (CCN) spectra and aerosol chemical composition were in-situ measured from the DOE Gulfstream 1 (G-1) research aircraft during two Intensive Operations Periods (IOPs), one conducted in July 2012 and the other in February 2013. An overall aerosol size distribution was achieved by merging the observations from several instruments, including Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A, DMT), Passive Cavity Aerosol Spectrometer Probe (PCASP-200, DMT), and Cloud Aerosol Spectrometer (CAS, DMT). Aerosol chemical composition was characterized using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Inc.) and single particle mass spectrometer, mini-SPLAT. Based on the aerosol size distribution, CCN number concentration (characterized by a DMT dual column CCN counter with a range from 0.1% to 0.4%), and chemical composition, a CCN closure was obtained. The sensitivity of CCN closure to organic hygroscopicity was investigated. The differences in aerosol/CCN properties between two columns, and between two phases, will be discussed.

  3. Interaction of aerosol particles composed of protein and salts with water vapor: hygroscopic growth and microstructural rearrangement

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Niessner, R.; Pöschl, U.

    2004-02-01

    The interaction of aerosol particles composed of the protein bovine serum albumin (BSA) and the inorganic salts sodium chloride and ammonium nitrate with water vapor has been investigated by hygroscopicity tandem differential mobility analyzer (H-TDMA) experiments complemented by transmission electron microscopy (TEM) and Köhler theory calculations (100-300nm particle size range, 298K, 960hPa). BSA was chosen as a well-defined model substance for proteins and other macromolecular compounds, which constitute a large fraction of the water-soluble organic component of air particulate matter.

    Pure BSA particles exhibited deliquescence and efflorescence transitions at sim35% relative humidity (RH) and a hygroscopic diameter increase by up to sim10% at 95% RH in good agreement with model calculations based on a simple parameterisation of the osmotic coefficient. Pure NaCl particles were converted from near-cubic to near-spherical shape upon interaction with water vapor at relative humidities below the deliquescence threshold (partial surface dissolution and recrystallisation), and the diameters of pure NH4NO3 particles decreased by up to 10% due to chemical decomposition and evaporation.

    Mixed NaCl-BSA and NH4NO3-BSA particles interacting with water vapor exhibited mobility equivalent diameter reductions of up to 20%, depending on particle generation, conditioning, size, and chemical composition (BSA dry mass fraction 10-90%). These observations can be explained by formation of porous agglomerates (envelope void fractions up to 50%) due to ion-protein interactions and electric charge effects on the one hand, and by compaction of the agglomerate structure due to capillary condensation effects on the other. The size of NH4NO3-BSA particles was apparently also influenced by volatilisation of NH4NO3, but not as much as for pure salt particles, i.e. the protein inhibited the decomposition of NH4NO3 or the

  4. Vapour pressures and hygroscopicity of semi-volatile organic components in ternary organic/inorganic/water aerosol droplet trapped by aerosol optical tweezers

    NASA Astrophysics Data System (ADS)

    Cai, Chen; Zhang, Yunhong

    2016-04-01

    Knowledge of the vapour pressures of semi-volatile organic compounds is of critical importance in determining their partitioning behaviour into atmospheric aerosol. Quantifying the gas/particle partitioning of organic compounds is of great importance since at present published results of the vapour pressures of compounds of interest (typically with vapour pressures lower than 0.01 Pa) can be different by several orders of magnitude and influences on SVOCs evaporation from participation of inorganic compounds remains unclear. In this study we present a new method for the retrieval of SVOCs vapour pressures from single aerosol droplets in an aerosol optical tweezers system. Measurements of the concentration of SVOC (derived from experimentally determined RI) and radius of SVOC aqueous droplets are correlated in an expression derived from the Maxwell gas phase diffusion equation for the determination of vapour pressure. ( ) dmi-= 4π dr3Conc + dConcir3 = 4πrMiDi,gas-(p - p) dt 3 dt i dt RT i,∞ i,r Relationship between r dr/dt (nm2s-1) and r2dConcentration/dt (nm2gL-1s-1) is presented, in which the slope is derived for determination of hygroscopic line whilst the axis intercept can be determined to estimate vapour pressure. Briefly the method relies on the levitation of a droplet (3-7 μm radius) in an aerosol optical tweezers system. In this system the droplet acts as a microcavity and the size and refractive index of the particle can be extracted by using Mie theory to fit the positions of the "whispering gallery modes" in the cavity enhanced Raman spectroscopy fingerprint. The vapour pressure can then be extracted from the correlation between the rate of change of particle radius with the rate of change of composition (refractive index, n). We will show that information about the hygroscopicity of the particle and how this changes as the particle evaporates can also be determined from the changing slopes of these plots.

  5. Meteorological and aerosol effects on marine cloud microphysical properties

    NASA Astrophysics Data System (ADS)

    Sanchez, K. J.; Russell, L. M.; Modini, R. L.; Frossard, A. A.; Ahlm, L.; Corrigan, C. E.; Roberts, G. C.; Hawkins, L. N.; Schroder, J. C.; Bertram, A. K.; Zhao, R.; Lee, A. K. Y.; Lin, J. J.; Nenes, A.; Wang, Z.; Wonaschütz, A.; Sorooshian, A.; Noone, K. J.; Jonsson, H.; Toom, D.; Macdonald, A. M.; Leaitch, W. R.; Seinfeld, J. H.

    2016-04-01

    Meteorology and microphysics affect cloud formation, cloud droplet distributions, and shortwave reflectance. The Eastern Pacific Emitted Aerosol Cloud Experiment and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets studies provided measurements in six case studies of cloud thermodynamic properties, initial particle number distribution and composition, and cloud drop distribution. In this study, we use simulations from a chemical and microphysical aerosol-cloud parcel (ACP) model with explicit kinetic drop activation to reproduce observed cloud droplet distributions of the case studies. Four cases had subadiabatic lapse rates, resulting in fewer activated droplets, lower liquid water content, and higher cloud base height than an adiabatic lapse rate. A weighted ensemble of simulations that reflect measured variation in updraft velocity and cloud base height was used to reproduce observed droplet distributions. Simulations show that organic hygroscopicity in internally mixed cases causes small effects on cloud reflectivity (CR) (<0.01), except for cargo ship and smoke plumes, which increased CR by 0.02 and 0.07, respectively, owing to their high organic mass fraction. Organic hygroscopicity had larger effects on droplet concentrations for cases with higher aerosol concentrations near the critical diameter (namely, polluted cases with a modal peak near 0.1 µm). Differences in simulated droplet spectral widths (k) caused larger differences in CR than organic hygroscopicity in cases with organic mass fractions of 60% or less for the cases shown. Finally, simulations from a numerical parameterization of cloud droplet activation suitable for general circulation models compared well with the ACP model, except under high organic mass fraction.

  6. Characterization of particle hygroscopicity by Raman lidar: Selected case studies from the convective and orographically-induced precipitation study

    NASA Astrophysics Data System (ADS)

    Stelitano, Dario; Di Girolamo, Paolo; Summa, Donato

    2013-05-01

    The characterization of particle hygroscopicity has primary importance for climate monitoring and prediction. Model studies have demonstrated that relative humidity (RH) has a critical influence on aerosol climate forcing. Hygroscopic properties of aerosols influence particle size distribution and refractive index and hence their radiative effects. Aerosol particles tend to grow at large relative humidity values as a result of their hygroscopicity. Raman lidars with aerosol, water vapor and temperature measurement capability are potentially attractive tools for studying aerosol hygroscopicity as in fact they can provide continuous altitude-resolved measurements of particle optical, size and microphysical properties, as well as relative humidity, without perturbing the aerosols or their environment. Specifically, the University of Basilicata Raman lidar system (BASIL) considered for the present study, has the capability to perform all-lidar measurements of relative humidity based on the application of both the rotational and the vibrational Raman lidar techniques in the UV. BASIL was operational in Achern (Black Forest, Lat: 48.64° N, Long: 8.06° E, Elev.: 140 m) between 25 May and 30 August 2007 in the framework of the Convective and Orographically-induced Precipitation Study (COPS). The present analysis is focused on selected case studies characterized by the presence of different aerosol types with different hygroscopic behavior. The observed behavior, dependent upon aerosol composition, may range from hygrophobic to strongly hygroscopic.

  7. Internal Structure, Hygroscopic and Reactive Properties of Mixed Sodium Methanesulfonate-Sodium Chloride Particles

    SciTech Connect

    Liu, Ying; Minofar, Babak; Desyaterik, Yury; Dames, E. E.; Zhu, Zihua; Cain, Jeremy P.; Hopkins, Rebecca J.; Gilles, Marry K.; Wang, Hai; Jungwirth, Pavel; Laskin, Alexander

    2011-01-01

    Internal structures, hygroscopic properties and heterogeneous reactivity of mixed CH3SO3Na/NaCl particles were investigated using a combination of computer modeling and experimental approaches. Surfactant properties of CH3SO3 ions and their surface accumulation in wet, deliquesced particles were assessed using molecular dynamics (MD) simulations and surface tension measurements. Internal structures of dry CH3SO3Na/NaCl particles were investigated using scanning electron microscopy (SEM) assisted with X-ray microanalysis mapping, and time-of-flight secondary ion mass spectrometry (TOF-SIMS). The combination of these techniques shows that dry CH3SO3Na/NaCl particles are composed of a NaCl core surrounded by a CH3SO3Na shell. Hygroscopic growth, deliquescence and efflorescence phase transitions of mixed CH3SO3Na/NaCl particles were determined and compared to those of pure NaCl particles. These results indicate that particles undergo a two step deliquescence transition: first at ~69% relative humidity (RH) the CH3SO3Na shell takes up water, and then at ~75% RH the NaCl core deliquesces. Reactive uptake coefficients for the particle HNO3 heterogeneous reaction were determined at different CH3SO3Na/NaCl mixing ratios and RH. The net reaction probability decreased notably with increasing CH3SO3Na and at lower RH.

  8. Internal structure, hygroscopic and reactive properties of mixed sodium methanesulfonate-sodium chloride particles.

    PubMed

    Liu, Y; Minofar, B; Desyaterik, Y; Dames, E; Zhu, Z; Cain, J P; Hopkins, R J; Gilles, M K; Wang, H; Jungwirth, P; Laskin, A

    2011-07-01

    Internal structures, hygroscopic properties and heterogeneous reactivity of mixed CH(3)SO(3)Na/NaCl particles were investigated using a combination of computer modeling and experimental approaches. Surfactant properties of CH(3)SO(3)(-) ions and their surface accumulation in wet, deliquesced particles were assessed using molecular dynamics (MD) simulations and surface tension measurements. Internal structures of dry CH(3)SO(3)Na/NaCl particles were investigated using scanning electron microscopy (SEM) assisted with X-ray microanalysis mapping, and time-of-flight secondary ion mass spectrometry (TOF-SIMS). The combination of these techniques shows that dry CH(3)SO(3)Na/NaCl particles are composed of a NaCl core surrounded by a CH(3)SO(3)Na shell. Hygroscopic growth, deliquescence and efflorescence phase transitions of mixed CH(3)SO(3)Na/NaCl particles were determined and compared to those of pure NaCl particles. These results indicate that particles undergo a two step deliquescence transition: first at ∼69% relative humidity (RH) the CH(3)SO(3)Na shell takes up water, and then at ∼75% RH the NaCl core deliquesces. Reactive uptake coefficients for the particle-HNO(3) heterogeneous reaction were determined at different CH(3)SO(3)Na/NaCl mixing ratios and RH. The net reaction probability decreased notably with increasing CH(3)SO(3)Na and at lower RH.

  9. Airborne characterization of subsaturated aerosol hygroscopicity and dry refractive index from the surface to 6.5 km during the SEAC4RS campaign

    NASA Astrophysics Data System (ADS)

    Shingler, Taylor; Crosbie, Ewan; Ortega, Amber; Shiraiwa, Manabu; Zuend, Andreas; Beyersdorf, Andreas; Ziemba, Luke; Anderson, Bruce; Thornhill, Lee; Perring, Anne E.; Schwarz, Joshua P.; Campazano-Jost, Pedro; Day, Douglas A.; Jimenez, Jose L.; Hair, Johnathan W.; Mikoviny, Tomas; Wisthaler, Armin; Sorooshian, Armin

    2016-04-01

    In situ aerosol particle measurements were conducted during 21 NASA DC-8 flights in the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys field campaign over the United States, Canada, Pacific Ocean, and Gulf of Mexico. For the first time, this study reports rapid, size-resolved hygroscopic growth and real refractive index (RI at 532 nm) data between the surface and upper troposphere in a variety of air masses including wildfires, agricultural fires, biogenic, marine, and urban outflow. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) quantified size-resolved diameter growth factors (GF = Dp,wet/Dp,dry) that are used to infer the hygroscopicity parameter κ. Thermokinetic simulations were conducted to estimate the impact of partial particle volatilization within the DASH-SP across a range of sampling conditions. Analyses of GF and RI data as a function of air mass origin, dry size, and altitude are reported, in addition to κ values for the inorganic and organic fractions of aerosol. Average RI values are found to be fairly constant (1.52-1.54) for all air mass categories. An algorithm is used to compare size-resolved DASH-SP GF with bulk scattering f(RH = 80%) data obtained from a pair of nephelometers, and the results show that the two can only be reconciled if GF is assumed to decrease with increasing dry size above 400 nm (i.e., beyond the upper bound of DASH-SP measurements). Individual case studies illustrate variations of hygroscopicity as a function of dry size, environmental conditions, altitude, and composition.

  10. Aerosol hygroscopicity and its impact on atmospheric visibility and radiative forcing in Guangzhou during the 2006 PRIDE-PRD campaign

    NASA Astrophysics Data System (ADS)

    Liu, Xingang; Zhang, Yuanhang; Cheng, Yafang; Hu, Min; Han, Tingting

    2012-12-01

    The objective of this study is to quantify the relation of aerosol chemical compositions and optical properties, and to assess the impact of relative humidity (RH) on atmospheric visibility and aerosol direct radiative forcing (ADRF). Mass concentration and size distribution of aerosol chemical compositions as well as aerosol optical properties were concurrently measured at Guangzhou urban site during the PRD (Pearl River Delta) campaign from 1 to 31 July, 2006. Gaseous pollutant NO2 and meteorological parameter were simultaneously monitored. Compared with its dry condition, atmospheric ambient extinction coefficient σext(RH) averagely increased about 51% and atmospheric visibility deceased about 35%, among which RH played an important role on the optical properties of water soluble inorganic salts. (NH4)2SO4 is the most important component responsible for visibility degradation at Guangzhou. In addition, the asymmetry factor g increased from 0.64 to 0.74 with the up-scatter fraction β decreasing from 0.24 to 0.19 when RH increasing from 40% to 90%. At 80% RH, the ADRF increased about 280% compared to that at dry condition and it averagely increased about 100% during the campaign under ambient conditions. It can be inferred that aerosol water content is a key factor and could not be ignored in assessing the role of aerosols in visibility impairment and radiative forcing, especially in the regions with high RH.

  11. Atmospheric aerosols: Their Optical Properties and Effects

    NASA Technical Reports Server (NTRS)

    1976-01-01

    Measured properties of atmospheric aerosol particles are presented. These include aerosol size frequency distribution and complex retractive index. The optical properties of aerosols are computed based on the presuppositions of thermodynamic equilibrium and of Mie-theory.

  12. Aerosol optical properties in the Marine Environment during the TCAP-I campaign

    NASA Astrophysics Data System (ADS)

    Chand, D.; Berg, L. K.; Barnard, J.; Berkowitz, C. M.; Burton, S. P.; Chapman, E. G.; Comstock, J. M.; Fast, J. D.; Ferrare, R. A.; Connor, F. J.; Hair, J. W.; Hostetler, C. A.; Hubbe, J.; Kluzek, C.; Mei, F.; Pekour, M. S.; Sedlacek, A. J.; Schmid, B.; Shilling, J. E.; Shinozuka, Y.; Tomlinson, J. M.; Wilson, J. M.; Zelenyuk-Imre, A.

    2013-12-01

    The role of direct radiative forcing by atmospheric aerosol is one of the largest sources of uncertainty in predicting climate change. Much of this uncertainty comes from the limited knowledge of observed aerosol optical properties. In this presentation we discuss derived aerosol optical properties based on measurements made during the summer 2012 Two-Column Aerosol Project-I (TCAP) campaign and relate these properties to the corresponding chemical and physical properties of the aerosol. TCAP was designed to provide simultaneous, in-situ observations of the size distribution, chemical properties, and optical properties of aerosol within and between two atmospheric columns over the Atlantic Ocean near the eastern seaboard of the United States. These columns are separated by 200-300 km and were sampled in July 2012 during a summer intensive operation period (IOP) using the U.S. Department of Energy's Gulfstream-1 (G-1) and NASA's B200 aircraft, winter IOP using G-1 aircraft in February 2013, and the surface-based DOE Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) located on Cape Cod. In this presentation we examine the spectral dependence of the aerosol optical properties measured from the aircraft over the TCAP-I domain, with an emphasis on in-situ derived intensive properties measured by a 3-λ Nephelometer, a Particle Soot Absorption Photometer (PSAP), a humidograph (f(RH)), and a Single Particle Soot Photometer (SP2). Preliminary results indicate that the aerosol are more light-absorbing as well as more hygroscopic at higher altitudes (2-4 km) compared to the corresponding values made within residual layers near the surface (0-2 km altitude). The average column (0-4 km) single scattering albedo (ω) and hygroscopic scattering factor (F) are found to be ~0.96 and 1.25, respectively. Additional results on key aerosol intensive properties such as the angstrom exponent (å), asymmetry parameter (g), backscattering fraction (b), and gamma parameter (

  13. Volcanic Aerosol Radiative Properties

    NASA Technical Reports Server (NTRS)

    Lacis, Andrew

    2015-01-01

    Large sporadic volcanic eruptions inject large amounts of sulfur bearing gases into the stratosphere which then get photochemically converted to sulfuric acid aerosol droplets that exert a radiative cooling effect on the global climate system lasting for several years.

  14. Mixing properties of individual submicrometer aerosol particles in Vienna

    NASA Astrophysics Data System (ADS)

    Okada, Kikuo; Hitzenberger, Regina M.

    Individual aerosol particles were collected on 5 days with different meteorological conditions in March, April and June 1991 in the urban atmosphere of Vienna in Austria. The samples collected with an impactor were examined by electron microscopy. The mixing properties of submicrometer aerosol particles with radii between 0.1 and 1 μm were studied by using the dialysis (extraction) of water-soluble material. The averaged results showed that more than 85% of particles with radii between 0.1 and 0.7 μm were hygroscopic. However, more than 50% of particles with radii larger than 0.2 μm were mixed particles (hygroscopic particles with water-insoluble inclusions), and they were dominant (80%) in the size range 0.5-0.7 μm radius. The results also showed that the number proportion of mixed particles increased with increasing radius and the abundance increased with increasing particle loading in the atmosphere. The volume fraction of water-soluble material ( ɛ) in mixed particles tended to decrease with increasing radius, implying the formation of mixed particles by heterogeneous processes such as condensation and/or surface reaction. Some results of elemental composition in individual particles analyzed with an energy-dispersive X-ray (EDX) analyzer equipped with an electron microscope are also presented in this paper.

  15. Aerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters

    NASA Astrophysics Data System (ADS)

    Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Welti, Andre; Ziemba, Luke D.; Murphy, Daniel M.

    2016-04-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0-4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry-climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ˜ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1-0.5 µm diameter dominates aerosol extinction.

  16. Aqueous aerosol SOA formation: impact on aerosol physical properties.

    PubMed

    Woo, Joseph L; Kim, Derek D; Schwier, Allison N; Li, Ruizhi; McNeill, V Faye

    2013-01-01

    Organic chemistry in aerosol water has recently been recognized as a potentially important source of secondary organic aerosol (SOA) material. This SOA material may be surface-active, therefore potentially affecting aerosol heterogeneous activity, ice nucleation, and CCN activity. Aqueous aerosol chemistry has also been shown to be a potential source of light-absorbing products ("brown carbon"). We present results on the formation of secondary organic aerosol material in aerosol water and the associated changes in aerosol physical properties from GAMMA (Gas-Aerosol Model for Mechanism Analysis), a photochemical box model with coupled gas and detailed aqueous aerosol chemistry. The detailed aerosol composition output from GAMMA was coupled with two recently developed modules for predicting a) aerosol surface tension and b) the UV-Vis absorption spectrum of the aerosol, based on our previous laboratory observations. The simulation results suggest that the formation of oligomers and organic acids in bulk aerosol water is unlikely to perturb aerosol surface tension significantly. Isoprene-derived organosulfates are formed in high concentrations in acidic aerosols under low-NO(x) conditions, but more experimental data are needed before the potential impact of these species on aerosol surface tension may be evaluated. Adsorption of surfactants from the gas phase may further suppress aerosol surface tension. Light absorption by aqueous aerosol SOA material is driven by dark glyoxal chemistry and is highest under high-NO(x) conditions, at high relative humidity, in the early morning hours. The wavelength dependence of the predicted absorption spectra is comparable to field observations and the predicted mass absorption efficiencies suggest that aqueous aerosol chemistry can be a significant source of aerosol brown carbon under urban conditions. PMID:24601011

  17. Influences of relative humidity and particle chemical composition on aerosol scattering properties during the 2006 PRD campaign

    NASA Astrophysics Data System (ADS)

    Liu, Xingang; Cheng, Yafang; Zhang, Yuanhang; Jung, Jinsang; Sugimoto, Nobuo; Chang, Shih-Yu; Kim, Young J.; Fan, Shaojia; Zeng, Limin

    In situ measurements of the physical, chemical, and optical properties of aerosols were carried out in Guangzhou city, China, from 1 to 31 July 2006 during the Pearl River Delta (PRD) Campaign. The light extinction coefficient of the ambient atmosphere, the aerosol scattering coefficient under dry conditions, the aerosol absorption coefficient under ambient conditions, NO 2 concentration, and relative humidity (RH) were measured by transmissionmeter, an integrating nephelometer, a multi-angle absorption photometer (MAAP), a NO X analyzer, and an automatic meteorological station, respectively. Meanwhile, the molecular scattering coefficient was calculated by the Rayleigh scattering function using the US Standard Atmosphere. A method to calculate the aerosol hygroscopic growth factor f(RH), defined as the ratio of the aerosol scattering coefficient under a wet condition to that under a dry condition (40% RH), is proposed based on these optical parameters. The mean and standard deviation aerosol hygroscopic growth factors at 80% RH ( f(RH)=80%) in Ganzhou were 2.04±0.28, 2.29±0.28, and 2.68±0.59 for urban aerosols, mixed aerosols, and marine aerosols, respectively, with the air mass classification being based on the air mass source region. The relationship between f(RH) and RH is fitted by empirical equations and the fitting parameters are calculated. The relationships between f(RH)=80% and total carbon mass fraction (TCF) in PM 2.5, the water-soluble mass fraction (WSF) in PM 10, and the sea-salt aerosol mass fraction (SSF) in PM 10 reveal that the hygroscopic properties of the observed aerosol have a good positive correlation with the WSF and SSF, but have a negative correlation with the TCF.

  18. Inorganic salts interact with organic di-acids in sub-micron particles to form material with low hygroscopicity and volatility

    NASA Astrophysics Data System (ADS)

    Drozd, G.; Woo, J.; Häkkinen, S. A. K.; Nenes, A.; McNeill, V. F.

    2013-11-01

    Volatility and hygroscopicity are two key properties of organic aerosol components, and both are strongly related to chemical identity. Here we show that inorganic-organic component interactions typically not considered in atmospheric models may strongly affect aerosol volatility and hygroscopicity. In particular, bi-dentate binding of di-carboxylic acids (DCA) to soluble inorganic ions can lead to very strongly bound metal-organic complexes with largely undetermined hygroscopicity and volatility. These reactions profoundly impact particle hygroscopicity, transforming hygroscopic components into irreversibly non-hygroscopic material. While the hygroscopicities of pure salts, DCA, and DCA salts are known, the hygroscopicity of internal mixtures of hygroscopic salts and DCA, as they are typically found in the atmosphere, has not been fully characterized. We have studied the volatility of pure, dry organic salt particles and the hygroscopicity of internal mixtures of oxalic acid (OxA, the dominant DCA in the atmosphere) and a number of salts, both mono- and di-valent. The formation of very low volatility organic salts was confirmed, with minimal evaporation of oxalate salt particles below 75 °C. Dramatic increases in the CCN activation diameter for particles with divalent salts (e.g. CaCl2) and relatively small particle mass fractions of OxA indicate that standard volume additivity rules for hygroscopicity do not apply. Thus small organic compounds with high O:C are capable of forming low volatility and very low hygroscopicity particles. Given current knowledge of the formation mechanisms of OxA and M-Ox salts, surface enrichment of insoluble M-Ox salts is expected. The resulting formation of an insoluble coating of metal-oxalate salts can explain low particle hygroscopicities. The formation of particles with a hard coating could offer an alternative explanation for observations of glass-like particles with very low viscosity.

  19. Optical Aerosol Properties Over the Asian Pacific Ocean during ACE-Asia

    NASA Astrophysics Data System (ADS)

    Rood, M. J.; Carrico, C. M.; Kus, P.

    2001-12-01

    The effect of aerosol particles on the atmospheric radiative-energy balance at critical locations around the globe is an area or research that to be better characterized. This research has allowed shipboard measurements of climatically relevant ambient-aerosol optical properties between Hawaii and the coast of China to characterize "clean marine conditions" and then along the coast of China to characterize "polluted conditions" and "mineral dust conditions." Aerosol light scattering properties and in particular the increase in light scattering coefficient with increasing controlled relative humidity (f(RH)) during ACE-Asia showed a wider diversity of profiles than during ACE-1, ACE-2 or at a U.S. continental site. During the Pacific crossing, the signature was clearly marine-seasalt dominated (very hygroscopic with large magnitude growth with a clear deliquescent/crystallization hysteresis loop) and quite similar to the background marine conditions of Cape Grim during ACE-1. Other times when flow was off the Asian continent, the dependence of scattering on controlled RH was quite similar to results obtained in Sagres Portugal during outflow of European air masses (ACE-2, hygroscopic with smoother changes in scattering with increasing RH conditions though some deliquescent/crystallization features). When the aerosol consisted of a large part mineral dust species, the hygroscopic growth in light scattering was quite suppressed. Mineral dust dominated aerosols showed very little growth in light scattering as a function of RH and at times was nearly hygrophobic. However, along with the suppressed hygroscopic growth, deliquescent (step-change) features were often more pronounced than the cases of the more hygroscopic urban-industrial influenced aerosols. These results will also be integrated with laboratory light scattering measurements and field absorption measurements for comparison of light scattering and albedo measurements made by other independent techniques

  20. Ageing of aerosol and their radiative properties in the Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Roberts, Greg; Léon, Jean-François; Pont, Véronique; Mallet, Marc; Augustin, Patrick; Dulac, François; Junkermann, Wolfgang

    2014-05-01

    The VESSAER campaign (VErtical Structure and Sources of AERosols in the Mediterranean Region) identified different sources of aerosol in the Mediterranean Basin and assessed the regional impact of aerosol on cloud microphysical and radiative properties. The airborne aspect of VESSAER was conducted on an ultra-light aircraft in summer 2012. Ground-based activities included observations in the central and northern regions of Corsica, as well as aerosol LIDAR and sun photometer measurements on the eastern coast. The main scientific goals were to investigate local versus long-range sources of aerosol and cloud condensation nuclei (CCN) and their vertical structure in the lower troposphere, study evolution and ageing related to atmospheric processes, and determine aerosol direct radiative impacts over a larger spatial scale in the Mediterranean Basin. Even though Corsica is separated by from the European continent by ca. 100 km with no immediate sources of urban aerosol, the background concentrations in Corsica were similar to those in the continental European boundary layer. The background total aerosol concentrations within the boundary layer in Corsica are nearly 2000 cm-3. Nearly all of the particles in the boundary layer (> 90%) are CCN-active at 0.37% supersaturation as they had become hygroscopic during their transport. Ageing (with respect to CCN-activity) of European emissions occurred exclusively in the boundary layer and not in aerosol layers aloft. In contrast, aerosol hygroscopicity did not change as a function of transport time in elevated aerosol layers, suggesting that photochemical ageing of less hygroscopic material is relatively slow compared to ageing processes in the boundary layer. The vertical profiles clearly show the long-range transport of dust from the Saharan Desert and pollution from the European continent -- which were the two major sources of aerosol during the campaign. Two of the research flights coincided with CALIPSO overpasses, when

  1. Aerosol optical properties and radiative effects in the Yangtze Delta region of China

    NASA Astrophysics Data System (ADS)

    Xia, Xiangao; Li, Zhanqing; Holben, Brent; Wang, Pucai; Eck, Tom; Chen, Hongbin; Cribb, Maureen; Zhao, Yanxia

    2007-11-01

    One year's worth of aerosol and surface irradiance data from September 2005 to August 2006 were obtained at Taihu, the second supersite for the East Asian Study of Tropospheric Aerosols: An International Regional Experiment (EAST-AIRE). Aerosol optical properties derived from measurements by a Sun photometer were analyzed. The aerosol data were used together with surface irradiance data to quantitatively estimate aerosol effects on surface shortwave radiation (SWR) and photosynthetically active radiation (PAR). The annual mean aerosol optical depth at 500 nm is 0.77, and mean Ångstrom wavelength exponent is 1.17. The annual mean aerosol single scattering albedo and mean aerosol asymmetry factor at 440 nm are 0.90 and 0.72, respectively. Both parameters show a weak seasonal variation, with small values occurring during the winter and larger values during the summer. Clear positive relationships between relative humidity and aerosol properties suggest aerosol hygroscopic growth greatly modifies aerosol properties. The annual mean aerosol direct radiative forcing at the surface (ADRF) is -38.4 W m-2 and -17.8 W m-2 for SWR and PAR, respectively. Because of moderate absorption, the instantaneous ADRF at the top of the atmosphere derived from CERES SSF data is close to zero. Heavy aerosol loading in this region leads to -112.6 W m-2 and -45.5 W m-2 reduction in direct and global SWR, but 67.1 W m-2 more diffuse SWR reaching the surface. With regard to PAR, the annual mean differences in global, direct and diffuse irradiance are -23.1 W m-2, -65.2 W m-2 and 42.1 W m-2 with and without the presence of aerosol, respectively.

  2. Hygroscopic Properties and Respiratory System Deposition Behavior of Particulate Matter Emitted By Mining and Smelting Operations

    PubMed Central

    Youn, Jong-sang; Csavina, Janae; Rine, Kyle P.; Shingler, Taylor; Taylor, Mark Patrick; Sáez, A. Eduardo; Betterton, Eric A.; Sorooshian, Armin

    2016-01-01

    This study examines size-resolved physicochemical data for particles sampled near mining and smelting operations and a background urban site in Arizona with a focus on how hygroscopic growth impacts particle deposition behavior. Particles with aerodynamic diameters between 0.056 – 18 μm were collected at three sites: (i) an active smelter operation in Hayden, AZ, (ii) a legacy mining site with extensive mine tailings in Iron King, AZ, and (iii) an urban site, inner-city Tucson, AZ. Mass size distributions of As and Pb exhibit bimodal profiles with a dominant peak between 0.32-0.56 μm and a smaller mode in the coarse range (> 3 μm). The hygroscopicity profile did not exhibit the same peaks owing to dependence on other chemical constituents. Sub-micrometer particles were generally more hygroscopic than super-micrometer ones at all three sites with finite water-uptake ability at all sites and particle sizes examined. Model calculations at a relative humidity of 99.5% reveal significant respiratory system particle deposition enhancements at sizes with the largest concentrations of toxic contaminants. Between dry diameters of 0.32 and 0.56 μm, for instance, ICRP and MPPD models predict deposition fraction enhancements of 171%-261% and 33%-63%, respectively, at the three sites. PMID:27700056

  3. Experimental characterization of the hygroscopic properties of wood during convective drying using digital holographic interferometry.

    PubMed

    Kumar, Manoj; Shakher, Chandra

    2016-02-10

    In this paper, an application of digital holography for the measurement of surface deformations and the strain field to understand the shrinkage behavior of wood during convective drying is presented. Moisture absorption and desorption induce the dimensional changes and deformations in wood that leads to failure of certain components made of wood. The knowledge of the dimensional changes in wood, deformations, strain distribution and their causes are important for the best utilization of wood. For the study, lensless Fourier transform digital holographic interferometry is used to measure moisture- induced deformation, strain distribution, and the coefficient of hygroscopic shrinkage in different samples of wood. The technique is highly sensitive and enables the observation of deformation and strain distribution during the variations of moisture content in the wood. The wet wood sample was exposed to convective drying, which leads to changes in the moisture content and the associated deformations. The deformation/strain in each step of drying process is used to evaluate the coefficient of hygroscopic shrinkage in different wood samples. The experiments were repeated for differently treated woods. The experimental results show that the strain and coefficient of hygroscopic shrinkage can be minimized if the wood is dried in the presence of the proper moisture content. PMID:26906359

  4. Chemical Properties of Combustion Aerosols: An Overview

    EPA Science Inventory

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

  5. Meteorological and Aerosol effects on Marine Cloud Microphysical Properties

    NASA Astrophysics Data System (ADS)

    Sanchez, K. J.; Russell, L. M.; Modini, R. L.; Frossard, A. A.; Ahlm, L.; Roberts, G.; Hawkins, L. N.; Schroder, J. C.; Wang, Z.; Lee, A.; Abbatt, J.; Lin, J.; Nenes, A.; Wonaschuetz, A.; Sorooshian, A.; Noone, K.; Jonsson, H.; Albrecht, B. A.; Desiree, T. S.; Macdonald, A. M.; Seinfeld, J.; Zhao, R.

    2015-12-01

    Both meteorology and microphysics affect cloud formation and consequently their droplet distributions and shortwave reflectance. The Eastern Pacific Emitted Aerosol Cloud Experiment (EPEACE) and the Stratocumulus Observations of Los-Angeles Emissions Derived Aerosol-Droplets (SOLEDAD) studies provide detailed measurements in 6 case studies of both cloud thermodynamic properties and initial particle number distribution and composition, as well as the resulting cloud drop distribution and composition. This study uses simulations of a detailed chemical and microphysical aerosol-cloud parcel (ACP) model with explicit kinetic drop activation to reproduce the observed cloud droplet distribution and composition. Four of the cases examined had a sub-adiabatic lapse rate, which was shown to have fewer droplets due to decreased maximum supersaturation, lower LWC and higher cloud base height, consistent with previous findings. These detailed case studies provided measured thermodynamics and microphysics that constrained the simulated droplet size distribution sufficiently to match the droplet number within 6% and the size within 19% for 4 of the 6 cases, demonstrating "closure" or consistency of the measured composition with the measured CCN spectra and the inferred and modeled supersaturation. The contribution of organic components to droplet formation shows small effects on the droplet number and size in the 4 marine cases that had background aerosol conditions with varying amounts of coastal, ship or other non-biogenic sources. In contrast, the organic fraction and hygroscopicity increased the droplet number and size in the cases with generated smoke and cargo ship plumes that were freshly emitted and not yet internally mixed with the background particles. The simulation results show organic hygroscopicity causes small effects on cloud reflectivity (<0.7%) with the exception of the cargo ship plume and smoke plume which increased absolute cloud reflectivity fraction by 0

  6. Aerosol properties in Titan's upper atmosphere

    NASA Astrophysics Data System (ADS)

    Lavvas, Panayotis; Koskinen, Tommi; Royer, Emilie; Rannou, Pascal; West, Robert

    2016-06-01

    Multiple Cassini observations reveal that the abundant aerosol particles in Titan's atmosphere are formed at high altitudes, particularly in the thermosphere. They subsequently fall towards the lower atmosphere and in their path their size, shape, and population change in reflection to the variable atmospheric condition. Although multiple observations can help us retrieve information for the aerosol properties in the lower atmosphere, we have limited information for the aerosol properties between their formation region in the thermosphere and the upper region of the main haze layer or the detached aerosol layer. Observations at UV wavelengths are the only way to probe this part of the atmosphere and help us retrieve the aerosol properties. The presentation will provide an overview of the available observations, and discuss their implications for the production and evolution of Titan's aerosols.

  7. Aerosol Observing System (AOS) Handbook

    SciTech Connect

    Jefferson, A

    2011-01-17

    The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earth’s radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

  8. Morphology and Optical Properties of Mixed Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Fard, Mehrnoush M.; Krieger, Ulrich; Rudich, Yinon; Marcolli, Claudia; Peter, Thomas

    2015-04-01

    Experiments and modeling studies have shown that deliquesced aerosols can be present not only as one-phase system containing organics, inorganic salts and water, but often as two-phase systems consisting of a predominantly organic and a predominantly inorganic aqueous phase 1,2. Recent laboratory studies conducted with model mixtures representing tropospheric aerosols1,2,3, secondary organic aerosol (SOA) from smog chamber experiments4, and field measurements5 suggest that liquid- liquid phase separations (LLPS) is indeed a common phenomenon in mixed organic/ ammonium sulfate (AS) particles. During LLPS, particles may adopt different morphologies mainly core- shell and partially engulfed. A core- shell configuration will have consequences for heterogeneous chemistry and hygroscopicity and as a result will alter the optical properties of the particles since the aqueous inorganic-rich phase will be totally enclosed by a probably highly viscous organic coating with low diffusivity for reactants and water. The primary objective of this project is to establish a method for investigating the morphology of mixed inorganic and absorbing organic compounds of atmospheric relevance and study their radiative properties before, during, and after phase transitions mainly during LLPS. This will be the first study looking into the radiative effect of LLPS in detail. In this first experiment, the behavior of single droplets of carminic acid (CA)/ AS/ H2O mixture was monitored during relative humidity (RH) cycles using optical microscopy. The same mixture particle was levitated in an electrodynamic balance (EDB) and the change in its absorption properties was measured at varying RH. We also intend to determine the occurrence of LLPS in accumulation- sized particles and the change in their absorption using a cavity ring down aerosol spectrometer. If LLPS alters the absorptive properties of the suggested model aerosols significantly, absorption measurements of accumulation mode

  9. A study of aerosol optical properties using a lightweight optical particle spectrometer and sun photometer from an unmanned aerial system

    NASA Astrophysics Data System (ADS)

    Telg, H.; Murphy, D. M.; Bates, T. S.; Johnson, J. E.; Gao, R. S.

    2015-12-01

    A miniaturized printed optical particle spectrometer (POPS) and sun photometer (miniSASP) have been developed recently for unmanned aerial systems (UAS) and balloon applications. Here we present the first scientific data recorded by the POPS and miniSASP from a Manta UAS during a field campaign on Svalbard, Norway, in April 2015. As part of a payload composed of five different aerosol instruments (absorption photometer, condensation particle counter, filter sampler, miniSASP and POPS) we collected particle size distributions, the optical depth (OD) and the sky brightness from 0 to 3000 m altitude. The complementary measurement approaches of the miniSASP and POPS allow us to calculate aerosol optical properties such as the aerosol optical depth and the angstrom exponent or the asymmetry parameter independently. We discuss deviation between results with respect to aerosol properties, e.g. hygroscopicity and absorption, as well as instrumental limitations.

  10. Demonstration of Aerosol Property Profiling by Multi-wavelength Lidar Under Varying Relative Humidity Conditions

    NASA Technical Reports Server (NTRS)

    Whiteman, D.N.; Veselovskii, I.; Kolgotin, A.; Korenskii, M.; Andrews, E.

    2008-01-01

    The feasibility of using a multi-wavelength Mie-Raman lidar based on a tripled Nd:YAG laser for profiling aerosol physical parameters in the planetary boundary layer (PBL) under varying conditions of relative humidity (RH) is studied. The lidar quantifies three aerosol backscattering and two extinction coefficients and from these optical data the particle parameters such as concentration, size and complex refractive index are retrieved through inversion with regularization. The column-integrated, lidar-derived parameters are compared with results from the AERONET sun photometer. The lidar and sun photometer agree well in the characterization of the fine mode parameters, however the lidar shows less sensitivity to coarse mode. The lidar results reveal a strong dependence of particle properties on RH. The height regions with enhanced RH are characterized by an increase of backscattering and extinction coefficient and a decrease in the Angstrom exponent coinciding with an increase in the particle size. We present data selection techniques useful for selecting cases that can support the calculation of hygroscopic growth parameters using lidar. Hygroscopic growth factors calculated using these techniques agree with expectations despite the lack of co-located radiosonde data. Despite this limitation, the results demonstrate the potential of multi-wavelength Raman lidar technique for study of aerosol humidification process.

  11. Regional Haze from Forest Fires and San Joaquin Valley Pollution: Aerosol Properties at Yosemite National Park

    NASA Astrophysics Data System (ADS)

    Carrico, C. M.; Day, D.; Heath, J.; Lee, T.; Herckes, P.; Engling, G.; Kreidenweis, S. M.; Collett, J. L.; Bench, G.; Malm, W.

    2002-12-01

    The impact of forest fire smoke on air quality and visibility in national parks is a growing concern, particularly in light of EPA's new Regional Haze rule. The summer of 2002 proved to be a very active year for wildfires in the western U.S. with double the average acres burned. To improve understanding of smoke aerosols, an intensive campaign to measure aerosol chemical, physical, optical, and in particular hygroscopic properties, was conducted in Yosemite National Park in July-September 2002. High time resolution chemical measurements allowed speciation of major ions and carbon with 15 and 60 minute time resolution, respectively. Preliminary results show a predominant contribution of organic carbon with concentrations ranging from ~5-15 μgm-3 while major ions were dominated by sulfate, nitrate and ammonium and totaled approximately 2 μgm-3. Carbon isotopic analysis showed that during the haziest periods most carbon had a biogenic source. Soluble potassium and UV light absorption were observed to be useful indicators of smoke impact. During smoky periods, dry light scattering coefficients ranged from roughly 50-200 Mm-1, comparable to the most polluted US cities. Measurements using light scattering and diameter growth techniques both showed limited aerosol hygroscopicity. Diameter and light scattering growth factors ranged from roughly 1.05-1.2 and 1.1-1.5, respectively, at RH = 80%. Measurements of the aerosol dry size distribution during hazy periods showed a mode in the optically efficient size of several hundred nm in addition to a typical number concentration mode around 100 nm. In general, the aerosol properties at Yosemite were observed to have strong influences from smoke likely transported from massive regional wildfires as well as pollution likely from agricultural and population centers of Central California.

  12. Study of aerosol optical properties at Kunming in southwest China and long-range transport of biomass burning aerosols from North Burma

    NASA Astrophysics Data System (ADS)

    Zhu, J.; Xia, X.; Che, H.; Wang, J.; Zhang, J.; Duan, Y.

    2016-03-01

    Seasonal variation of aerosol optical properties and dominant aerosol types at Kunming (KM), an urban site in southwest China, is characterized. Substantial influences of the hygroscopic growth and long-range transport of biomass burning (BB) aerosols on aerosol optical properties at KM are revealed. These results are derived from a detailed analysis of (a) aerosol optical properties (e.g. aerosol optical depth (AOD), columnar water vapor (CWV), single scattering albedo (SSA) and size distribution) retrieved from sunphotometer measurements during March 2012-August 2013, (b) satellite AOD and active fire products, (c) the attenuated backscatter profiles from the space-born lidar, and (d) the back-trajectories. The mean AOD440nm and extinction Angstrom exponent (EAE440 - 870) at KM are 0.42 ± 0.32 and 1.25 ± 0.35, respectively. Seasonally, high AOD440nm (0.51 ± 0.34), low EAE440 - 870 (1.06 ± 0.34) and high CWV (4.25 ± 0.97 cm) during the wet season (May - October) contrast with their counterparts 0.17 ± 0.11, 1.40 ± 0.31 and 1.91 ± 0.37 cm during the major dry season (November-February) and 0.53 ± 0.29, 1.39 ± 0.19, and 2.66 ± 0.44 cm in the late dry season (March-April). These contrasts between wet and major dry season, together with the finding that the fine mode radius increases significantly with AOD during the wet season, suggest the importance of the aerosol hygroscopic growth in regulating the seasonal variation of aerosol properties. BB and Urban/Industrial (UI) aerosols are two major aerosol types. Back trajectory analysis shows that airflows on clean days during the major dry season are often from west of KM where the AOD is low. In contrast, air masses on polluted days are from west (in late dry season) and east (in wet season) of KM where the AOD is often large. BB air mass is found mostly originated from North Burma where BB aerosols are lifted upward to 5 km and then subsequently transported to southwest China via prevailing westerly winds.

  13. Retrieval of optical and microphysical properties of aerosols from a hybrid multiwavelength lidar dataset

    NASA Astrophysics Data System (ADS)

    Sawamura, Patricia

    Over the past decade the development of inversion techniques for the retrievals of aerosol microphysical properties (e.g. effective radius, volume and surface-area concentrations) and aerosol optical properties (e.g. complex index of refraction and single scattering albedo) from multiwavelength lidar systems brought a new perspective in the study of the vertical distribution of aerosols. In this study retrievals of such parameters were obtained from a hybrid multiwavelength lidar dataset for the first time. In July of 2011, in the Baltimore-Washington DC region, synergistic profiling of optical and microphysical properties of aerosols with both airborne in-situ and ground-based remote sensing systems was performed during the first deployment of DISCOVER-AQ. The hybrid multiwavelength lidar dataset combines elastic ground-based measurements at 355 nm with airborne High Spectral Resolution Lidar (HSRL) measurements at 532 nm and elastic measurements at 1064 nm that were obtained less than 5 km apart of each other. This was the first study to our knowledge in which optical and microphysical retrievals from lidar were obtained during the day and directly compared to AERONET and in-situ measurements for eleven cases. Good agreement was observed between lidar and AERONET retrievals. Larger discrepancies were observed between lidar retrievals and in-situ measurements obtained by the aircraft and aerosol hygroscopic effects are believed to be the main factor of such discrepancies.

  14. How Does a Raindrop Grow?: Precipitation in natural clouds may develop from ice crystals or from large hygroscopic aerosols.

    PubMed

    Braham, R R

    1959-01-16

    On the basis of presently available data, combined with present-day knowledge of the physics and chemistry of cloud particle development, it is possible to make the following generalizations about the mode of precipitation in natural clouds. 1) The all-water mechanism begins to operate as soon as a parcel of cloud air is formed and continues to operate throughout the life of the cloud. The ice-crystal mechanism, on the other hand, can begin to operate only after the top of the cloud has reached levels where ice nuclei can be effective (about -15 degrees C). Some clouds never reach this height; any precipitation from them must be through the all-water mechanism. In cold climates and at high levels in the atmosphere, the cloud bases may be very close to this critical temperature. In the tropics, approximately 25,000 feet separate the bases of low clouds from the natural ice level. 2) The number of large hygroscopic nuclei in maritime air over tropical oceans is entirely adequate to rain-out any cloud with a base below about 10,000 feet, provided the cloud duration and cloud depth is sufficient for the precipitation process to operate. Extensive trajectories over land will decrease the number of sea-salt particles, both because of sedimentation and removal in rain. Measurements show an order-of-magnitude decrease in the number of large particles as maritime air moves from the Gulf of Mexico to the vicinity of St. Louis, during the summer months. Measurements in Arizona and New Mexico show even smaller chloride concentrations, presumably because of the long overland trajectories required in reaching these areas. The maritime particles lost in overland trajectories apparently are more than replaced by particles of land origin. The latter are usually of mixed composition and are less favorable for the formation of outsized solution droplets. 3) Ice nuclei, required for the formation of ice crystals and for droplet freezing, are rather rare at temperatures higher than

  15. Aerosol and Cloud Microphysical Properties in the Asir region of Saudi Arabia

    NASA Astrophysics Data System (ADS)

    Axisa, Duncan; Kucera, Paul; Burger, Roelof; Li, Runjun; Collins, Don; Freney, Evelyn; Posada, Rafael; Buseck, Peter

    2010-05-01

    In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region of Saudi Arabia as part of a Precipitation Enhancement Feasibility Study. Ground measurements of aerosol size distributions, hygroscopic growth factor, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were done in the Asir region of Saudi Arabia in August 2009. Research aircraft operations focused primarily on conducting measurements in clouds that are targeted for cloud top-seeding, on their microphysical characterization, especially the preconditions necessary for precipitation; understanding the evolution of droplet coalescence, supercooled liquid water, cloud ice and precipitation hydrometeors is necessary if advances are to be made in the study of cloud modification by cloud seeding. Non-precipitating mixed-phase clouds less than 3km in diameter that developed on top of the stable inversion were characterized by flying at the convective cloud top just above the inversion. Aerosol measurements were also done during the climb to cloud base height. The presentation will include a summary of the analysis and results with a focus on the unique features of the Asir region in producing convective clouds, characterization of the

  16. Properties of aerosol processed by ice clouds

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  17. Global Analysis of Aerosol Properties Above Clouds

    NASA Technical Reports Server (NTRS)

    Waquet, F.; Peers, F.; Ducos, F.; Goloub, P.; Platnick, S. E.; Riedi, J.; Tanre, D.; Thieuleux, F.

    2013-01-01

    The seasonal and spatial varability of Aerosol Above Cloud (AAC) properties are derived from passive satellite data for the year 2008. A significant amount of aerosols are transported above liquid water clouds on the global scale. For particles in the fine mode (i.e., radius smaller than 0.3 m), including both clear sky and AAC retrievals increases the global mean aerosol optical thickness by 25(+/- 6%). The two main regions with man-made AAC are the tropical Southeast Atlantic, for biomass burning aerosols, and the North Pacific, mainly for pollutants. Man-made AAC are also detected over the Arctic during the spring. Mineral dust particles are detected above clouds within the so-called dust belt region (5-40 N). AAC may cause a warming effect and bias the retrieval of the cloud properties. This study will then help to better quantify the impacts of aerosols on clouds and climate.

  18. Hygroscopic behavior of NaCl-MgCl2 mixture particles as nascent sea-spray aerosol surrogates and observation of efflorescence during humidification

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Eom, H.-J.; Cho, H.-R.; Ro, C.-U.

    2015-10-01

    As Na+, Mg2+, and Cl- are major ionic constituents of seawater, NaCl-MgCl2 mixture particles might represent sea-spray aerosols (SSAs) better than pure NaCl. However, there have been very few hygroscopic studies of pure MgCl2 and NaCl-MgCl2 mixture aerosol particles despite the MgCl2 moiety playing a major role in the hygroscopic behavior of nascent SSAs. Laboratory-generated pure MgCl2 and NaCl-MgCl2 mixture aerosol particles with 12 mixing ratios (0.01 ≤ mole fraction of NaCl (XNaCl) ≤ 0.9) were examined systematically by optical microscopy (OM), in situ Raman micro-spectrometry (RMS), and scanning electron microscopy/energy dispersive X-ray spectrometry (SEM/EDX) elemental X-ray mapping to observe their hygroscopic behavior, derive the experimental phase diagrams, and obtain the chemical micro-structures. Dry-deposited MgCl2 ⋅ 6H2O particles exhibited a deliquescence relative humidity (DRH) of ~ 33.0 % and an efflorescence RH (ERH) of 10.8-9.1 %, whereas the nebulized pure MgCl2 and MgCl2-dominant particles of XNaCl = 0.026 (eutonic) and 0.01 showed single-stage transitions at DRH of ~ 15.9 % and ERH of 10.1-3.2 %. The characteristic OH-stretching Raman signatures indicated the crystallization of MgCl2 ⋅ 4H2O at low relative humidities (RHs), suggesting that the kinetic barrier to MgCl2 ⋅ 6H2O crystallization is not overcome in the timescale of the dehydration measurements. The NaCl-MgCl2 mixture particles of 0.05 ≤ XNaCl ≤ 0.9 generally showed two-stage deliquescence: first at the mutual DRH (MDRH) of ~ 15.9 %; and second with the complete dissolution of NaCl at the second DRHs depending on the mixing ratios, resulting in a phase diagram composed of three distinct phases. During dehydration, most particles of 0.05 ≤ XNaCl ≤ 0.9 exhibited two-stage efflorescence: first, by the homogeneous nucleation of NaCl; and second, at mutual ERH (MERH) of ~ 10.4-2.9 %, by the crystallization of the MgCl2 ⋅ 4H2O moiety, also resulting in three

  19. Hygroscopic behavior of NaCl-MgCl2 mixture particles as nascent sea-spray aerosol surrogates and observation of efflorescence during humidifying process

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Eom, H.-J.; Cho, H.-R.; Ro, C.-U.

    2015-07-01

    NaCl and MgCl2 are the two major constituents of seawater, so NaCl-MgCl2 mixture particles can be a better representative of sea-spray aerosols (SSAs) than pure NaCl. However, there have been very few hygroscopic studies of pure MgCl2 and NaCl-MgCl2 mixture aerosol particles despite the MgCl2 moiety playing a major role in the hygroscopic behavior of nascent SSAs. Laboratory-generated pure MgCl2 and NaCl-MgCl2 mixture aerosol particles with 12 mixing ratios (0.01 ≤ mole fraction of NaCl (XNaCl) ≤ 0.9) were examined systematically by optical microscopy, in-situ Raman microspectrometry (RMS), and scanning electron microscopy/energy dispersive X-ray spectrometry (SEM/EDX) elemental X-ray mapping to observe their hygroscopic behavior, derive the experimental phase diagrams, and obtain the chemical micro-structures. Dry-deposited MgCl2·6H2O particles exhibited a deliquescence relative humidity (DRH) of ∼ 33.0 % and an efflorescence RH (ERH) of 10.8-9.1 %, whereas the nebulized pure MgCl2 and MgCl2-dominant particles of XNaCl = 0.026 (eutonic) and 0.01 showed single-stage transitions at DRH of ∼ 15.9 % and ERH of 10.1-3.2 %. The characteristic OH-stretching Raman signatures indicated the crystallization of MgCl2·4H2O at low RHs, suggesting that the kinetic barrier to MgCl2·6H2O crystallization is not overcome in the timescale of the dehydration measurements. The NaCl-MgCl2 mixture particles of 0.05 ≤ XNaCl ≤ 0.9 generally showed two-stage deliquescence: first at the mutual DRH (MDRH) of ~ 15.9 %; and second with the complete dissolution of NaCl at the second DRHs depending on the mixing ratios, resulting in a phase diagram composed of three distinct phases. During dehydration, most particles of 0.05 ≤ XNaCl ≤ 0.9 exhibited two-stage efflorescence: first, by the homogeneous nucleation of NaCl; and second, at mutual ERH (MERH) of ∼ 10.4-2.9 %, by the crystallization of the MgCl2·4H2O moiety, also resulting in three distinct phases. Interestingly

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  1. Measurements of physical and chemical properties of urban aerosols and their CCN activities in Seoul during the KORUS-AQ pre-campaign

    NASA Astrophysics Data System (ADS)

    Kim, N.; Yum, S. S.; Park, M.; Shin, H. J.; Bae, G. N.; Kwak, K. H.; Park, J. S.; Park, S. M.; Ahn, J.

    2015-12-01

    Interest in cloud condensation nuclei (CCN) has been increasing for the last few decades due to their first order effects on radiative and microphysical properties of clouds. Particularly, scientific understanding of CCN from anthropogenic sources becomes important because it is now considered that large uncertainties in climate change predictions stem from insufficient understanding of CCN. CCN activity is influenced by size and chemical component of aerosols. The KORUS-AQ campaign, jointly organized by National Institute of Environmental Research (NIER) of Korea and National Aeronautics and Space Administration (NASA) aims at understanding various aspects of air quality problem in Korea and will be held in spring, 2016. In preparation for this campaign, pre-campaign was held during May 18-June 13, 2015, in Seoul where numerous local anthropogenic sources exist and influence of Chinese continental outflow directly affects. Here we present some of the important results from the pre-campaign. Chemical properties of aerosols were measured with AMS. Aerosol and CCN number concentrations, aerosol size distribution and aerosol hygroscopic growth factor were measured by CPC, CCN counter, SMPS and H-TDMA, respectively. Average diurnal variation of aerosol number concentration showed three dominant peaks at around 0600_UTC and morning and evening rush hours. Each peak seemed to have different characteristics and therefore detailed analyses of physical and chemical properties of aerosols during the peaks as well as during some special events will be made. The hygroscopicity parameter, kappa, will be estimated by examining CCN activity, H-TDMA measured hygroscopic growth factor and mixing rule of aerosol chemical components, and the result will be compared as well.

  2. Aerosol physical properties from satellite horizon inversion

    NASA Technical Reports Server (NTRS)

    Gray, C. R.; Malchow, H. L.; Merritt, D. C.; Var, R. E.; Whitney, C. K.

    1973-01-01

    The feasibility is investigated of determining the physical properties of aerosols globally in the altitude region of 10 to 100 km from a satellite horizon scanning experiment. The investigation utilizes a horizon inversion technique previously developed and extended. Aerosol physical properties such as number density, size distribution, and the real and imaginary components of the index of refraction are demonstrated to be invertible in the aerosol size ranges (0.01-0.1 microns), (0.1-1.0 microns), (1.0-10 microns). Extensions of previously developed radiative transfer models and recursive inversion algorithms are displayed.

  3. Evolution of the Physicochemical and Activation Properties of Aerosols within Smoke Plumes during the Biomass Burning Observation Project (BBOP)

    NASA Astrophysics Data System (ADS)

    Tomlinson, J. M.; Mei, F.; Wang, J.; Comstock, J. M.; Hubbe, J. M.; Pekour, M. S.; Shilling, J. E.; Fortner, E.; Chand, D.; Sedlacek, A. J., III; Kleinman, L. I.; Senum, G.; Schmid, B.

    2014-12-01

    Biomass burning from wildfires and controlled agricultural burns are known to be a major source of fine particles and organic aerosols at northern temperate latitudes during the summer months. However, the evolution of the physicochemical properties of the aerosol during transport and the potential impact of this evolution on cloud condensation nuclei (CCN) activity has rarely been studied for these events. During the DOE-sponsored Biomass Burning Observation Project (BBOP) conducted in the summer and fall of 2013, over 30 research flights sampled biomass burning plumes from wildfires in the Northwestern United States and agricultural burns in the Mid-South region of the United States. A large suite of instruments aboard the DOE G-1 (Gulfstream-1) measured the chemical, physical, and optical properties of biomass burning aerosol with an emphasis on black carbon. A Fast Integrated Mobility Spectrometer (FIMS), Ultra High Sensitivity Aerosol Spectrometer - Airborne (UHSAS-A), and Passive Cavity Aerosol Spectrometer (PCASP) were used to measure the aerosol size distribution from 15 - 3,000 nm at 1-Hz. A dual column CCN counter measured the CCN number concentration at supersaturations of 0.25% and 0.50% at a time resolution of 1-Hz and the aerosol chemical composition was measured using a soot particle aerosol mass spectrometer (SP-AMS, Aerodyne, Inc). The SP-AMS was operated in two modes: (i) as a traditional high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Inc.), which measured chemical composition of non-refractory aerosols and (ii) as the SP-AMS which measured chemical composition of the refractory black carbon-containing (rBC) particle coating and rBC aerosol mass. Utilizing the aforementioned measurements, a CCN closure study is used to investigate the emitted aerosol hygroscopicity, the evolution of the physicochemical properties of the aerosol, and the potential impacts on cloud microphysics from the different fuel sources.

  4. Aerosol and CCN properties at Princess Elisabeth station, East Antarctica: seasonality, new particle formation events and properties around precipitation events

    NASA Astrophysics Data System (ADS)

    Mangold, Alexander; Laffineur, Quentin; De Backer, Hugo; Herenz, Paul; Wex, Heike; Gossart, Alexandra; Souverijns, Niels; Gorodetskaya, Irina; Van Lipzig, Nicole

    2016-04-01

    Since 2010, several complementary ground-based instruments for measuring the aerosol composition of the Antarctic atmosphere have been operated at the Belgian Antarctic research station Princess Elisabeth, in Dronning Maud Land, East Antarctica (71.95° S, 23.35° E, 1390 m asl.). In addition, three ground-based remote sensing instruments for cloud and precipitation observations have been installed for continuous operation, including a ceilometer (cloud base height, type, vertical extent), a 24 Ghz micro-rain radar (vertical profiles of radar effective reflectivity and Doppler velocity), and a pyrometer (cloud base temperature). The station is inhabited from November to end of February and operates under remote control during the other months. In this contribution, the general aerosol and cloud condensation nuclei (CCN) properties will be described with a special focus on new particle formation events and around precipitation events. New particle formation events are important for the atmospheric aerosol budget and they also show that aerosols are not only transported to Antarctica but are also produced there, also inland. Aerosols are essential for cloud formation and therefore also for precipitation, which is the only source for mass gain of the Antarctic ice sheet. Measured aerosol properties comprise size distribution, total number, total mass concentration, mass concentration of light-absorbing aerosol and absorption coefficient and total scattering coefficient. In addition, a CCN counter has been operated during austral summers 2013/14, 2014/15 and 2015/16. The baseline total number concentration N-total was around some hundreds of particles/cm3. During new particle formation events N-total increased to some thousands of particles/cm3. Simultaneous measurements of N-total, size distribution and CCN number revealed that mostly the number of particles smaller than 100 nm increased and that the concentration of cloud condensation nuclei increased only very

  5. Hygroscopic Growth and Activation of Particles containing Algea-Exudate

    NASA Astrophysics Data System (ADS)

    Wex, Heike; Fuentes, Elena; Tsagkogeorgas, Georgios; Voigtländer, Jens; Clauss, Tina; Kiselev, Alexei; Green, David; Coe, Hugh; McFiggans, Gordon; Stratmann, Frank

    2010-05-01

    A large amount of the Earth is covered by oceans, which provide a constant source of marine aerosol particles, produced due to bubble bursting processes that depend on wind speed (O'Dowd and de Leeuw, 2007). In general, marine particles can be assumed to play an important role for the Earth atmosphere on a global scale, due to their abundance and due to their effect on clouds. E.g. marine stratus and stratocumulus clouds contribute about 30% to 40% to the Earth's albedo (Randall et al., 1984). The activation of aerosol particles to cloud droplets depends on the hygroscopic properties of the particles, which, in turn, depend on their chemical composition. For marine particles, is has been and still is discussed what the effects of organic substances being present in the particles might be. These substances originate from marine biota where they enrich at the ocean surface. To mimic marine aerosol particles, algae-exudates of different algae species were mixed with artificial sea-water. These samples were used in the laboratory to produce particles via a bubble bursting process (Fuentes et al., 2009). The hygroscopic growth and activation of the (size selected) particles was measured, using LACIS (Leipzig Aerosol Cloud Interaction Simulator, Stratmann et al., 2004) and the DMT-CCNc (Cloud Condensation Nucleus counter from Droplet Measurement Technologies, Roberts and Nenes, 2005). The hygroscopic growth was measured twice, 3 and 10 seconds after humidification, and no difference in the grown size was detected, i.e. no kinetic effect was observed for the examined time range. From LACIS and CCNc measurements, the hygroscopicity was deduced through determination of the amount of ions being effective in the particle / droplet solution (Rho(ion), Wex et al., 2007). A concentration dependent non-ideal behaviour was found for particles produced from an artificial sea-water sample that contained only inorganic salts, as can be expected (see e.g. Niedermeier et al., 2008

  6. Remote sensing of aerosol properties during CARES

    NASA Astrophysics Data System (ADS)

    Kassianov, Evgueni; Barnard, James; Pekour, Mikhail; Flynn, Connor; Ferrare, Richard; Hostetler, Chris; Hair, John; Jobson, Bertram T.

    2011-11-01

    One month of MFRSR data collected at two sites in the central California (USA) region during the CARES campaign are processed and the MFRSR-derived AODs at 500 nm wavelength are compared with available AODs provided by AERONET measurements. We find that the MFRSR and AERONET AODs are small (~0.05) and comparable. A reasonable quantitative agreement between column aerosol size distributions (up to 2 μm) from the MFRSR and AERONET retrievals is illustrated as well. Analysis of the retrieved (MFRSR and AERONET) and in situ measured aerosol size distributions suggests that the contribution of the coarse mode to aerosol optical properties is substantial for several days. The results of a radiative closure experiment performed for the two sites and one-month period show a favorable agreement between the calculated and measured broadband downwelling irradiances (bias does not exceed about 3 Wm-2), and thus imply that the MFRSR-derived aerosol optical properties are reasonable.

  7. Remote Sensing of Aerosol Properties during CARES

    SciTech Connect

    Kassianov, Evgueni I.; Barnard, James C.; Pekour, Mikhail S.; Flynn, Connor J.; Ferrare, R.; Hostetler, Chris A.; Hair, John; Jobson, Bertram Thomas

    2011-10-01

    One month of MFRSR data collected at two sites in the central California (USA) region during the CARES campaign are processed and the MFRSR-derived AODs at 500 nm wavelength are compared with available AODs provided by AERONET measurements. We find that the MFRSR and AERONET AODs are small ({approx}0.05) and comparable. A reasonable quantitative agreement between column aerosol size distributions (up to 2 um) from the MFRSR and AERONET retrievals is illustrated as well. Analysis of the retrieved (MFRSR and AERONET) and in situ measured aerosol size distributions suggests that the contribution of the coarse mode to aerosol optical properties is substantial for several days. The results of a radiative closure experiment performed for the two sites and one-month period show a favorable agreement between the calculated and measured broadband downwelling irradiances (bias does not exceed about 3 Wm-2), and thus imply that the MFRSR-derived aerosol optical properties are reasonable.

  8. Long-term observations of aerosol optical properties at Wuhan, an urban site in Central China

    NASA Astrophysics Data System (ADS)

    Wang, Lunche; Gong, Wei; Xia, Xiangao; Zhu, Jun; Li, Jun; Zhu, Zhongmin

    2015-01-01

    Aerosol optical properties including aerosol optical depth (AOD), Ångström exponent (α), single scattering albedo (SSA), aerosol size distribution and refractive index at urban Wuhan in Central China are investigated based on the measurements from a CIMEL sun-photometer during 2007-2013. AOD500 nm is found to be relatively high all year round and the highest value 1.52 occurs in June 2012 and the lowest (0.57) in November 2012. α shows a significant monthly variation, with the highest value in June 2010 (1.71) and the lowest value (0.78) in April 2012. Analysis of AOD and α frequencies indicate that this region is populated with fine-mode particles. Monthly variations of SSA for total, fine and coarse-mode particles are closely related to the aerosol hygroscopic growth, fossil fuel and biomass burning. The aerosol volume size distributions (bi-modal pattern) show distinct differences in particle radius for different seasons, the radius for fine-mode particles generally increase from spring to summer month, for example, the highest peak is around radius 0.15 μm in March, while the peak radius is around 0.25 μm in June. Finally, monthly statistics of real and imaginary parts of the complex refractive index are analyzed, the highest averages of real (1.50) and imaginary parts (0.0395) are found in spring and autumn, respectively at wavelength 440-1020 nm.

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

    NASA Astrophysics Data System (ADS)

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

    2005-07-01

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

  10. [Aerosol optical properties during different air-pollution episodes over Beijing].

    PubMed

    Shi, Chan-Zhen; Yu, Xing-Na; Zhou, Bin; Xiang, Lei; Nie, Hao-Hao

    2013-11-01

    Based on the 2005-2011 data from Aerosol Robotic Network (AERONET), this study conducted analysis on aerosol optical properties over Beijing during different air-pollution episodes (biomass burning, CNY firework, dust storm). The aerosol optical depth (AOD) showed notable increases in the air-pollution episodes while the AOD (at 440 nm) during dust storm was 4. 91, 4. 07 and 2.65 times higher as background, biomass burning and firework aerosols. AOD along with Angstrom exponent (alpha) can be used to determine the aerosol types. The dust aerosol had the highest AOD and the lowest alpha. The alpha value of firework (1.09) was smaller than biomass burning (1.21) and background (1.27), indicating that coarse particles were dominant in the former type. Higher AOD of burnings (than background) can be attributed to the optical extinction capability of black carbon aerosol. The single scattering albedo (SSA) was insensitive to wavelength. The SSA value of dust (0.934) was higher than background (0.878), biomass burning (0.921) and firework (0.905). Additionally, the extremely large SSA of burnings here maybe was caused by the aging smoke, hygroscopic growth and so on. The peak radius of aerosol volume size distributions were 0.1-0.2 microm and 2.24 -3.85 microm in clear and polluted conditions. The value of volume concentration ratio between coarse and fine particles was in the order of clear background (1.04), biomass burning (1.10), CNY firework (1.91) and dust storm (4.96) episode. PMID:24455916

  11. [Aerosol optical properties during different air-pollution episodes over Beijing].

    PubMed

    Shi, Chan-Zhen; Yu, Xing-Na; Zhou, Bin; Xiang, Lei; Nie, Hao-Hao

    2013-11-01

    Based on the 2005-2011 data from Aerosol Robotic Network (AERONET), this study conducted analysis on aerosol optical properties over Beijing during different air-pollution episodes (biomass burning, CNY firework, dust storm). The aerosol optical depth (AOD) showed notable increases in the air-pollution episodes while the AOD (at 440 nm) during dust storm was 4. 91, 4. 07 and 2.65 times higher as background, biomass burning and firework aerosols. AOD along with Angstrom exponent (alpha) can be used to determine the aerosol types. The dust aerosol had the highest AOD and the lowest alpha. The alpha value of firework (1.09) was smaller than biomass burning (1.21) and background (1.27), indicating that coarse particles were dominant in the former type. Higher AOD of burnings (than background) can be attributed to the optical extinction capability of black carbon aerosol. The single scattering albedo (SSA) was insensitive to wavelength. The SSA value of dust (0.934) was higher than background (0.878), biomass burning (0.921) and firework (0.905). Additionally, the extremely large SSA of burnings here maybe was caused by the aging smoke, hygroscopic growth and so on. The peak radius of aerosol volume size distributions were 0.1-0.2 microm and 2.24 -3.85 microm in clear and polluted conditions. The value of volume concentration ratio between coarse and fine particles was in the order of clear background (1.04), biomass burning (1.10), CNY firework (1.91) and dust storm (4.96) episode.

  12. Atmospheric Aerosol Properties and Climate Impacts

    NASA Technical Reports Server (NTRS)

    Chin, Mian; Kahn, Ralph A.; Remer, Lorraine A.; Yu, Hongbin; Rind, David; Feingold, Graham; Quinn, Patricia K.; Schwartz, Stephen E.; Streets, David G.; DeCola, Phillip; Halthore, Rangasayi

    2009-01-01

    This report critically reviews current knowledge about global distributions and properties of atmospheric aerosols, as they relate to aerosol impacts on climate. It assesses possible next steps aimed at substantially reducing uncertainties in aerosol radiative forcing estimates. Current measurement techniques and modeling approaches are summarized, providing context. As a part of the Synthesis and Assessment Product in the Climate Change Science Program, this assessment builds upon recent related assessments, including the Fourth Assessment Report of the Intergovernmental Panel on Climate Change (IPCC AR4, 2007) and other Climate Change Science Program reports. The objectives of this report are (1) to promote a consensus about the knowledge base for climate change decision support, and (2) to provide a synthesis and integration of the current knowledge of the climate-relevant impacts of anthropogenic aerosols for policy makers, policy analysts, and general public, both within and outside the U.S government and worldwide.

  13. Aerosol Properties over the Eastern North Pacific based on Measurements from the MAGIC Field Campaign

    NASA Astrophysics Data System (ADS)

    Lewis, E. R.; Senum, G.; Springston, S. R.; Kuang, C.

    2015-12-01

    The MAGIC field campaign, funded and operated by the ARM (Atmospheric Radiation Measurement) Climate Research Facility of the US Department of Energy, occurred between September 2012 and October, 2013 aboard the Horizon Lines cargo container ship Spirit making regular trips between Los Angeles, CA and Honolulu, HI. Along this route, which lies very near the GPCI (GCSS Pacific Cross-section Intercomparison) transect, the predominant cloud regime changes from stratocumulus near the California coast to trade-wind cumulus near Hawaii. The transition between these two regimes is poorly understood and not accurately represented in models. The goal of MAGIC was to acquire statistic of this transition and thus improve its representation in models by making repeated transects through this region and measuring properties of clouds and precipitation, aerosols, radiation, and atmospheric structure. To achieve these goals, the Second ARM Mobile Facility (AMF2) was deployed on the Horizon Spirit as it ran its regular route between Los Angeles and Honolulu. AMF2 consists of three 20-foot SeaTainers and includes three radars and other instruments to measure properties of clouds and precipitation; the Aerosol Observing System (AOS), which has a suite of instruments to measure properties of aerosols; and other instruments to measure radiation, meteorological quantities, and sea surface temperature. Two technicians accompanied the AMF2, and scientists rode the ship as observers. MAGIC made nearly 20 round trips between Los Angeles and Honolulu (and thus nearly 40 excursions through the stratocumulus-to-cumulus transition) and spent 200 days at sea, collecting an unprecedented data set. Aerosol properties measured with the AOS include number concentration and size distribution, CCN activity, hygroscopic growth, and light-scattering and absorption. Additionally, more than one hundred filter samples were collected. Aerosol properties and their spatial and temporal behavior are discussed

  14. Morphology and Optical Properties of Mixed Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Fard, Mehrnoush M.; Krieger, Ulrich; Rudich, Yinon; Marcolli, Claudia; Peter, Thomas

    2016-04-01

    Experiments and modeling studies have shown that deliquesced aerosols can exist not only as one-phase system containing organics, inorganic salts and water, but often as two-phase systems consisting of a predominantly organic and a predominantly inorganic aqueous phase (1,2). Recent laboratory studies conducted with model mixtures representing tropospheric aerosols (1,2,3), secondary organic aerosol (SOA) from smog chamber experiments (4), and field measurements (5) suggest that liquid-liquid phase separations (LLPS) is indeed a common phenomenon in mixed organic/ inorganic particles. During LLPS, particles may adopt different morphologies mainly core-shell and partially engulfed. A core-shell configuration will have consequences for heterogeneous chemistry and hygroscopicity and as a result will alter the optical properties of the particles in particular for organic phases containing absorbing molecules, e.g. brown carbon. The primary objective of this project is to establish a method for investigating the morphology of mixed inorganic and absorbing organic compounds of atmospheric relevance and study their radiative properties before, during, and after phase transitions mainly during LLPS. This will be the first study looking into the radiative effect of LLPS in detail. Our ternary model system consist of ammonium sulfate (AS)/ Polyethylene Glycol (PEG)/ and water (H2O). Carminic acid (CA) was added as a proxy for an absorbing organic compound to the system. The behavior of single droplets of above ternary mixture was monitored during relative humidity (RH) cycles using optical microscopy. The same ternary mixture particle was levitated in an electrodynamic balance (EDB) and the change in its absorption properties was measured at varying RH. In addition, Mie-code modeling is used to predict the absorption efficiency of the same ternary system and the result will be compared with the data obtained from EDB experiment. We also intend to determine the occurrence of

  15. Relations Between Cloud Condensation Nuclei And Aerosol Optical Properties Relevant to Remote Sensing: Airborne Measurements in Biomass Burning, Pollution and Dust Aerosol Over North America

    NASA Astrophysics Data System (ADS)

    Shinozuka, Y.; Clarke, A.; Howell, S.; Kapustin, V.; McNaughton, C.; Zhou, J.; Decarlo, P.; Jimenez, J.; Roberts, G.; Tomlinson, J.; Collins, D.

    2008-12-01

    Remote sensing of the concentration of cloud condensation nuclei (CCN) would help investigate the indirect effect of tropospheric aerosols on clouds and climate. In order to assess its feasibility, this paper evaluates the spectral-based retrieval technique for aerosol number and seeks one for aerosol solubility, using in-situ aircraft measurements of aerosol size distribution, chemical composition, hygroscopicity, CCN activity and optical properties. Our statistical analysis reveals that the CCN concentration over Mexico can be optically determined to a relative error of <20%, smaller than that for the mainland US and the surrounding oceans (~a factor of 2). Mexico's advantage is four-fold. Firstly, many particles originating from the lightly regulated industrial combustion and biomass burning are large enough to significantly affect light extinction, elevating the correlation between extinction and CCN number in absence of substantial dust. Secondly, the generally low ambient humidity near the major aerosol sources limits the error in the estimated response of particle extinction to humidity changes. Thirdly, because many CCN contain black carbon, light absorption also provides a measure of the CCN concentration. Fourthly, the organic fraction of volatile mass of submicron particles (OMF) is anti-correlated with the wavelength dependence of extinction due to preferential anion uptake by coarse dust, which provides a potential tool for remote-sensing OMF and the particle solubility.

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

    EPA Science Inventory

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  18. Volatility and Hygroscopicity of Atlanta CCN During New Particle Formation Events in Summer 2009

    NASA Astrophysics Data System (ADS)

    Moore, R.; Scheckman, J.; Williams, B. J.; Jiang, J.; McMurry, P. H.; Zhao, J.; Smith, J. N.; Nenes, A.

    2011-12-01

    New particle formation (NPF) has the potential to substantially impact the population of cloud condensation nuclei (CCN) by both by altering their number concentrations and the hygroscopic properties. It is currently thought that while NPF proceeds via condensation of gas-phase sulfuric acid, subsequent growth must be dominated by the condensation of secondary organic species in order to reconcile field observations with theory1,2. This implies size-dependent aerosol composition with varying amounts of organic species, yet the impact of these organics on cloud droplet formation remains one of the largest sources of uncertainty in aerosol-cloud-climate interactions studies. Consequently, there is a need for in-situ, size-resolved field measurements of CCN to unravel these complex effects. // // We present a comprehensive characterization of aerosol and CCN sampled in Midtown Atlanta during the August 2009 Nucleation and CCN intensive campaign (NCCN) at the Jefferson Street monitoring site. A Droplet Measurement Technologies Continuous-Flow Stream-wise Thermal-Gradient Chamber was operated in spectrometer mode using Scanning Flow CCN Analysis (SFCA)3 to provide size-resolved CCN concentrations over a variety of particle sizes (20-50 nm) and supersaturations (0.3-2%) with high temporal resolution (~30 seconds/scan). Continuous measurements of the aerosol size distribution (1-1000 nm) and chemical composition were also made. The inferred hygroscopicity increased substantially during NPF from ~0.2-0.3 (consistent with soluble secondary organic species) to ~0.6-0.8, consistent with sulfate species or organic salts. This finding is contrary to previous work suggesting less-CCN-active aerosol during NPF4. During two special experiments, a volatility tandem differential mobility analyzer (VTDMA) was coupled with the CCN instrument to examine the volatility-dependence of the CCN hygroscopicity of 40-nm particles. Heating particles in the VTDMA was observed to increase their

  19. Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

    NASA Astrophysics Data System (ADS)

    McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

    2011-09-01

    Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

  20. Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime

    NASA Astrophysics Data System (ADS)

    Wu, Z. J.; Zheng, J.; Shang, D. J.; Du, Z. F.; Wu, Y. S.; Zeng, L. M.; Wiedensohler, A.; Hu, M.

    2016-02-01

    Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the mean hygroscopicity parameters (κs) of 50, 100, 150, 200, and 250 nm particles were respectively 0.16 ± 0.07, 0.19 ± 0.06, 0.22 ± 0.06, 0.26 ± 0.07, and 0.28 ± 0.10, showing an increasing trend with increasing particle size. Such size dependency of particle hygroscopicity was similar to that of the inorganic mass fraction in PM1. The hydrophilic mode (hygroscopic growth factor, HGF > 1.2) was more prominent in growth factor probability density distributions and its dominance of hydrophilic mode became more pronounced with increasing particle size. When PM2.5 mass concentration was greater than 50 μg m-3, the fractions of the hydrophilic mode for 150, 250, and 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high-time-resolution size-resolved chemical composition derived from aerosol mass spectrometer (AMS) measurements using the Zdanovskii-Stokes-Robinson (ZSR) mixing rule. The organic hygroscopicity parameter (κorg) showed a positive correlation with the oxygen to carbon ratio. During the new particle formation event associated with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particles with the same sizes not during new particle formation (NPF) periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example, 250 nm particles) was observed. Such transformations may modify the state of the mixture of pre-existing particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.

  1. Organic Carbon: Correlating UV-Vis Absorption Spectral Patterns to Hygroscopicity

    NASA Astrophysics Data System (ADS)

    Kanu, A. M.; Bond, T. C.

    2005-12-01

    The complex composition of organic aerosols (OC) in the atmosphere results from an array of sources. Thousands of individual organic compounds within these aerosols are difficult to identify: however, studies suggest these mixtures affect the radiative balance of Earth's atmosphere. Therefore, it is at least as vital to study the absorption and scattering of incoming solar radiation by aerosols as it is to distinguish and quantify the myriad compounds. OC can represent significant fractions of atmospheric aerosol and can play a prominent role in atmospheric radiative forcing. My research focuses on identifying organic carbon with different hygroscopic and optical properties--both of which are affected by composition. We use gradient chromatographic elution with reverse-phase and ion-exchange chromatography columns. We examine aerosols from wood combustion generated within strict temperature regimes. Results demonstrate distinct clusters according to different water affinities. Furthermore, each cluster absorbs in staggered regimes of ultraviolet and visible light, depending on the combustion temperature at which the OC fraction is generated. The association between various absorbing features and hygroscopic properties may imply distinct climate forcing potentials for different fractions of the organic carbon.

  2. Biomass-burning impact on CCN number, hygroscopicity and cloud formation during summertime in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Bougiatioti, Aikaterini; Bezantakos, Spiros; Stavroulas, Iasonas; Kalivitis, Nikos; Kokkalis, Panagiotis; Biskos, George; Mihalopoulos, Nikolaos; Papayannis, Alexandros; Nenes, Athanasios

    2016-06-01

    This study investigates the concentration, cloud condensation nuclei (CCN) activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean and their impacts on cloud droplet formation. Air masses sampled were subject to a range of atmospheric processing (several hours up to 3 days). Values of the hygroscopicity parameter, κ, were derived from CCN measurements and a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA). An Aerosol Chemical Speciation Monitor (ACSM) was also used to determine the chemical composition and mass concentration of non-refractory components of the submicron aerosol fraction. During fire events, the increased organic content (and lower inorganic fraction) of the aerosol decreases the values of κ, for all particle sizes. Particle sizes smaller than 80 nm exhibited considerable chemical dispersion (where hygroscopicity varied up to 100 % for particles of same size); larger particles, however, exhibited considerably less dispersion owing to the effects of condensational growth and cloud processing. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles (having a diameter of ˜ 100 nm at dry conditions) sampled. Based on positive matrix factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend as the biomass-burning organic aerosol (BBOA) component, with the former being enhanced between 65 and 150 % (for supersaturations ranging between 0.2 and 0.7 %) with the arrival of the smoke plumes. Using multilinear regression of the PMF factors (BBOA, OOA-BB and OOA) and the observed hygroscopicity parameter, the inferred hygroscopicity of the oxygenated organic aerosol components is determined. We find that the transformation of freshly emitted biomass burning (BBOA) to more oxidized organic aerosol (OOA-BB) can result in a 2-fold increase of the inferred organic hygroscopicity; about 10

  3. Optical properties of aerosols over a tropical rain forest in Xishuangbanna, South Asia

    NASA Astrophysics Data System (ADS)

    Ma, Yongjing; Xin, Jinyuan; Zhang, Wenyu; Wang, Yuesi

    2016-09-01

    Observation and analysis of the optical properties of atmospheric aerosols in a South Asian tropical rain forest showed that the annual mean aerosol optical depth (AOD) and aerosol Ångström exponent (α) at 500 nm were 0.47 ± 0.30 (± value represents the standard deviation) and 1.35 ± 0.32, respectively, from 2012 to 2014, similar with that of Amazon region. Aerosol optical properties in this region varied significantly between the dry and wet seasons. The mean AOD and α were 0.50 ± 0.32 and 1.41 ± 0.28, respectively, in the dry season and 0.41 ± 0.20 and 1.13 ± 0.41 in the wet season. Because of the combustion of the rich biomass in the dry season, fine modal smoke aerosols increased, which led to a higher AOD and smaller aerosol control mode than in the wet season. The average atmospheric humidity in the wet season was 85.50%, higher than the 79.67% during the dry season. In the very damp conditions of the wet season, the aerosol control mode was relatively larger, while AOD appeared to be lower because of the effect of aerosol hygroscopic growth and wet deposition. The trajectories were similar both in dry and wet, but with different effects on the aerosol concentration. The highest AOD values 0.66 ± 0.34 (in dry) and 0.45 ± 0.21 (in wet) both occurred in continental air masses, while smaller (0.38-0.48 in dry and 0.30-0.35 in wet) in oceanic air masses. The range of AOD values during the wet season was relatively narrow (0.30-0.45), but the dry season range was wider (0.38-0.66). For the Ångström exponent, the range in the wet season (0.74-1.34) was much greater than that in the dry season (1.33-1.54).

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

    DOE Data Explorer

    Sedlacek, Art

    2011-08-30

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

  5. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions.

    PubMed

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

    2009-09-28

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which

  6. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions.

    PubMed

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

    2009-09-28

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which

  7. Toward Creating A Global Retrospective Climatology of Aerosol Properties

    NASA Technical Reports Server (NTRS)

    Curran, Robert J.; Mishchenko, Michael I.; Hansen, James E. (Technical Monitor)

    2000-01-01

    Tropospheric aerosols are thought to cause a significant direct and indirect climate forcing, but the magnitude of this forcing remains highly uncertain because of poor knowledge of global aerosol characteristics and their temporal changes. The standard long-term global product, the one-channel Advanced Very-High-Resolution Radiometer (AVHRR) aerosol optical thickness over the ocean, relies on a single predefined aerosol model and can be inaccurate in many cases. Furthermore, it provides no information on aerosol column number density, thus making it impossible to estimate the indirect aerosol effect on climate. Total Ozone Mapping Spectrometer (TOMS) data can be used to detect absorbing aerosols over land, but are insensitive to aerosols located below one kilometer. It is thus clear that innovative approaches must be employed in order to extract a more quantitative and accurate aerosol climatology from available satellite and other measurements, thus enabling more reliable estimates of the direct and indirect aerosol forcings. The Global Aerosol Climatology Project (GACP) was established in 1998 as part of the Global Energy and Water Cycle Experiment (GEWEX). Its main objective is to analyze satellite radiance measurements and field observations to infer the global distribution of aerosols, their properties, and their seasonal and interannual variations. The overall goal is to develop advanced global aerosol climatologies for the period of satellite data and to make the aerosol climatologies broadly available through the GACP web site.

  8. Self-assembly of marine exudate particles and their impact on the CCN properties of nascent marine aerosol

    NASA Astrophysics Data System (ADS)

    Schill, S.; Zimmermann, K.; Ryder, O. S.; Campbell, N.; Collins, D. B.; Gianneschi, N.; Bertram, T. H.

    2013-12-01

    Spontaneous self-assembly of marine exudate particles has previously been observed in filtered seawater samples. The chemicophysical properties of these particles may alter the chemical composition and CCN properties of nascent marine aerosol, yet to date simultaneous measurement of seawater exudate particle formation rates and number distributions, with aerosol particle formation rates and CCN activity are lacking. Here, we use a novel Marine Aerosol Reference Tank (MART) system to experimentally mimic a phytoplankton bloom via sequential addition of biological surrogates, including sterol, galactose, lipopolysaccharide, BSA protein, and dipalmitoylphosphatidylcholine. Nascent sea-spray aerosol are generated in the MART system via a continuous plunging waterfall. Exudate particle assembly in the water is monitored via dynamic light scattering (DLS) and transmission electron microscopy (TEM) to obtain both the assembly kinetics of the particles as well as particle number distributions Simultaneous characterization of both particle production rates and super-saturated particle hygroscopicity are also discussed. This study permits analysis of the controlling role of the molecular composition of dissolved organic carbon in setting the production rates of colloidal material in the surface oceans.

  9. Cloud droplet nucleation and its connection to aerosol properties

    SciTech Connect

    Schwartz, S.E.

    1996-04-01

    Anthropogenic aerosols influence the earth`s radiation balance and climate directly, by scattering shortwave (solar) radiation in cloud-free conditions and indirectly, by increasing concentrations of cloud droplets thereby enhancing cloud shortwave reflectivity. These effects are thought to be significant in the context of changes in the earth radiation budget over the industrial period, exerting a radiative forcing that is of comparable magnitude to that of increased concentrations of greenhouse gases over this period but opposite in sign. However the magnitudes of both the direct and indirect aerosol effects are quite uncertain. Much of the uncertainty of the indirect effect arises from incomplete ability to describe changes in cloud properties arising from anthropogenic aerosols. This paper examines recent studies pertaining to the influence of anthropogenic aerosols on loading and properties of aerosols affecting their cloud nucleating properties and indicative of substantial anthropogenic influence on aerosol and cloud properties over the North Atlantic.

  10. Polarization properties of aerosol particles over western Japan: classification, seasonal variation, and implications for air quality

    NASA Astrophysics Data System (ADS)

    Pan, Xiaole; Uno, Itsushi; Hara, Yukari; Osada, Kazuo; Yamamoto, Shigekazu; Wang, Zhe; Sugimoto, Nobuo; Kobayashi, Hiroshi; Wang, Zifa

    2016-08-01

    Ground-based observation of the polarization properties of aerosol particles using a polarization optical particle counter (POPC) was made from 27 October 2013, to 31 December 2015, at a suburban site in the Kyushu area of Japan. We found that the depolarization ratio (DR, the fraction of s-polarized signal in the total backward light scattering signal) of aerosol particles showed prominent seasonal variability, with peaks in spring (0.21-0.23) and winter (0.19-0.23), and a minimum value (0.09-0.14) in summer. The aerosol compositions in both fine mode (aerodynamic diameter of particle, Dp < 2.5 µm) and coarse mode (2.5 µm < Dp < 10 µm), and the size-dependent polarization characteristics were analyzed for long-range transport dust particles, sea salt, and anthropogenic pollution-dominant aerosols. The DR value increased with increasing particle size, and DR = 0.1 was a reliable threshold value to identify the sphericity of supermicron (Dp > 1 µm) particles. Occurrence of substandard air quality days in Kyushu was closely related with mixed type (coexistence of anthropogenic pollutants and dust particles in the atmosphere), especially in winter and spring, indicating that dust events in the Asian continent played a key role in the cross-boundary transport of continental pollution. Backward trajectory analysis demonstrated that air masses originating from the western Pacific contained large amounts of spherical particles due to the influence of sea salt, especially in summer; however, for air masses from the Asian continent, the dependence of number fraction of spherical particles on air relative humidity was insignificant, indicating the predominance of less-hygroscopic substances (e.g., mineral dust), although the mass concentrations of anthropogenic pollutants were elevated.

  11. The sources, properties, and evolution of organic aerosols in the atmosphere

    NASA Astrophysics Data System (ADS)

    Jimenez, J. L.

    2015-12-01

    Organic aerosols (OA) account for about 1/2 of the submicron particle mass in the atmosphere leading to important impacts on climate, human health, and other issues, but their sources, properties, and evolution are poorly understood. OA is comprised of primary OA (POA, emitted in the particle phase) and secondary OA (SOA, formed by gas-to-particle conversion). Together with others in the community and contrary to the understanding at the time, we demonstrated in the mid-2000s that SOA dominates over POA at most locations. This paradigm shift has led to intense research on the sources, processing, properties, and fate of SOA. Because pre-existing and commercial instruments were very limited for the analysis of the complex mixtures of highly oxidized species comprising real OA, we developed or co-developed several experimental and data analysis techniques aimed at extracting more information out of ambient and laboratory air, and pioneered their application in field experiments. We proposed a new paradigm (Jimenez et al., Science, 2009) that is consistent with worldwide measurements and in which OA and OA precursor gases evolve continuously by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. The amount of SOA formed from urban air is remarkably consistent across the world, although the contributions of different sources remain a subject of debate. Biomass burning emissions rarely form additional OA mass after emission, although rapid chemical aging is always observed. Global model-measurement comparisons suggest the need for a large (100 Tg/yr) "anthropogenically-controlled" SOA source, thought to be dominated by anthropogenically-enhanced biogenic SOA. SOA formed from several pathways from biogenic emissions is starting to be better characterized, as are key SOA properties such as

  12. Deliquescence: Hygroscopicity of Water-Soluble Crystalline Solids.

    PubMed

    Tereshchenko, Anatoly G

    2015-11-01

    A thermodynamic approach to the description of hygroscopic properties of crystal-soluble solids is introduced. Isotherms of water vapor sorption by a pure substance and the products with a heterogeneous or homogeneous impurity are compared. Solubility diagrams of substances in water are used to evaluate the influence of impurities on the hygroscopic properties of the products. Evidence demonstrates that water vapor sorption by a chemical product below the hygroscopic point of a basic component is determined by heterogeneous impurities. The introduction of the term "a hygroscopically pure substance" removes inconsistencies between the experimental results related to water vapor sorption and abstract theorems. The paper discusses relevant publications, concerning hygroscopicity of soluble substances, where the impurities are ignored resulting in procedural and theoretical errors.

  13. Does the long-range transport of African mineral dust across the Atlantic enhance their hygroscopicity?

    NASA Astrophysics Data System (ADS)

    Denjean, Cyrielle; Caquineau, Sandrine; Desboeufs, Karine; Laurent, Benoit; Quiñones Rosado, Mariana; Vallejo, Pamela; Mayol-Bracero, Olga; Formenti, Paola

    2015-04-01

    Influence of mineral dust on radiation balance is largely dependent on their ability to interact with water. While fresh mineral dusts are highly hydrophobic, various transformation processes (coagulation, heterogeneous chemical reaction) can modify the dust physical and chemical properties during long-range transport, which, in turn, can change the dust hygroscopic properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of dust hygroscopic properties, and their temporal evolution during long-range transport. We present the first direct surface measurements of the hygroscopicity of Saharan dust after long-range transport over the Atlantic Ocean, their relationship with chemical composition, their influence on particle size and shape and implications for optical properties. Particles were collected during the DUST Aging and TransporT from Africa to the Caribbean (Dust-AttaCk) campaign at the Cape San Juan Puerto Rico station in June-July 2012. Environmental scanning electron microscopy (ESEM) was used to analyze the size, shape, chemical composition and hygroscopic properties of individual particles. At different levels of concentrations in summertime, the coarse mode of atmospheric aerosols in Puerto Rico is dominated by Saharan mineral dust. Most of aged dust particles survived atmospheric transport intact with no observed internal mixture with other species and did not show hygroscopic growth up to 94% relative humidity. This is certainly due to the fact that in summertime dust is mostly transported above the marine boundary layer. A minor portion of mineral dust (approximately 19-28% by number) were involved in atmospheric heterogeneous reactions with acidic gases (likely SO2 and HCl) and sea salt aggregation. While sulfate- and chloride-coated dust remained extremely hydrophobic, dust particles in internal mixing with NaCl underwent profound changes in their hygroscopicity, therefore in size and shape. We

  14. Overview of aerosol properties associated with air masses sampled by the ATR-42 during the EUCAARI campaign (2008)

    NASA Astrophysics Data System (ADS)

    Crumeyrolle, S.; Schwarzenboeck, A.; Roger, J. C.; Sellegri, K.; Burkhart, J. F.; Stohl, A.; Gomes, L.; Quennehen, B.; Roberts, G.; Weigel, R.; Villani, P.; Pichon, J. M.; Bourrianne, T.; Laj, P.

    2013-05-01

    Within the frame of the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Météo-France aircraft ATR-42 performed 22 research flights over central Europe and the North Sea during the intensive observation period in May 2008. For the campaign, the ATR-42 was equipped to study the aerosol physical, chemical, hygroscopic and optical properties, as well as cloud microphysics. For the 22 research flights, retroplume analyses along the flight tracks were performed with FLEXPART in order to classify air masses into five sectors of origin, allowing for a qualitative evaluation of emission influence on the respective air parcel. This study shows that the extensive aerosol parameters (aerosol mass and number concentrations) show vertical decreasing gradients and in some air masses maximum mass concentrations (mainly organics) in an intermediate layer (1-3 km). The observed mass concentrations (in the boundary layer (BL): between 10 and 30 μg m-3; lower free troposphere (LFT): 0.8 and 14 μg m-3) are high especially in comparison with the 2015 European norms for PM2.5 (25 μg m-3) and with previous airborne studies performed over England (Morgan et al., 2009; McMeeking et al., 2012). Particle number size distributions show a larger fraction of particles in the accumulation size range in the LFT compared to BL. The chemical composition of submicron aerosol particles is dominated by organics in the BL, while ammonium sulphate dominates the submicron aerosols in the LFT, especially in the aerosol particles originated from north-eastern Europe (~ 80%), also experiencing nucleation events along the transport. As a consequence, first the particle CCN acting ability, shown by the CCN/CN ratio, and second the average values of the scattering cross sections of optically active particles (i.e. scattering coefficient divided by the optical active particle concentration) are increased in the LFT compared to BL.

  15. Thermochemical, cloud condensation nucleation ability and optical properties of alkyl aminium sulfate aerosols

    NASA Astrophysics Data System (ADS)

    Lavi, A.; Bluvshtein, N.; Segre, E.; Segev, L.; Flores, J.; Rudich, Y.

    2013-12-01

    The increased interest in the chemistry of alkylamines and their possible roles in the atmosphere increased recently due to field observations of the correlation between new particle formation and post nucleation growth events and the presence of alkylamines in their cationic form. Due to their high saturation vapor pressure it is unlikely that short chain alkylamines will contribute to particle formation or growth by condensation. Therefore, it was previously suggested that their contribution to particulate phase is the result of acid-base reactions between the basic alkylamines and atmospherically relevant acids such as sulfuric and nitric acid. In this study we present laboratory data on the thermochemical, CCN activity and optical properties of selected atmospherically relevant alkyl aminium sulfate salts: Monomethyl aminium sulfate (MMAS), dimethyaminium sulfate (DMAS), trimethylaminium sulfate, monoethylaminium sulfate (MEAS), diethylaminium sulfate (DEAS) and triethylaminium sulfate (TEAS)). We found that the vapor pressure of these aminium salts is 1-3 orders of magnitude lower than that of ammonium sulfate and as such they can contribute to new aerosols and secondary aerosols formation. We infer that these species have very high CCN activity, with hygroscopicity parameter that is lower but close to that ammonium sulfate. Finally, we present the optical properties of these alkyl aminium sulfate salts between 360 and 420 nm. These compounds are less scattering than ammonium sulfate and show minimal wavelength dependence in this range. These compounds also do not absorb light. These derived parameters can contribute to the better understanding and characterization of the role that these compounds play in atmospheric chemical reactions, gas-solid partitioning and their possible contribution to the microphysical and radiative effects of atmospheric aerosols.

  16. The chemical and microphysical properties of secondary organic aerosols from Holm Oak emissions

    NASA Astrophysics Data System (ADS)

    Lang-Yona, N.; Rudich, Y.; Mentel, Th. F.; Buchholz, A.; Kiendler-Scharr, A.; Kleist, E.; Spindler, C.; Tillmann, R.; Wildt, J.

    2010-02-01

    The Mediterranean region is expected to experience substantial climatic change in the next 50 years. But, possible effects of climate change on biogenic volatile organic compound (VOC) emissions as well as on the formation of secondary organic aerosols (SOA) produced from these VOC are yet unexplored. To address such issues, the effects of temperature and light intensity on the VOC emissions of Mediterranean Holm Oak have been studied in the Jülich plant aerosol atmosphere chamber, as well as the optical and microphysical properties of the resulting SOA. Monoterpenes dominated the VOC emissions from Holm Oak (97.5%) and temperature increase enhanced the emission strength under variation of the emission pattern. The amount of SOA increased linearly with the emission strength with a fractional mass yield of 5.7±1%, independent of the detailed emission pattern. The particles were highly scattering with no absorption abilities. Their average hygroscopic growth factor was 1.13±0.03 at 90% RH with a critical diameter of droplet activation of 100±4 nm at a supersaturation of 0.4%. All microphysical properties did not depend on the detailed emission pattern, in accordance with an invariant O/C ratio (0.57(+0.03/-0.1)) of the SOA observed by high resolution aerosol mass spectrometry. The increase of Holm oak emissions with temperature (≈20% per degree) was stronger than e.g. for Boreal tree species (≈10% per degree). Increasing mean temperature in Mediterranean areas therefore may have a stronger impact on VOC emissions and SOA formation than in areas with Boreal forests.

  17. The chemical and microphysical properties of secondary organic aerosols from Holm Oak emissions

    NASA Astrophysics Data System (ADS)

    Lang-Yona, N.; Rudich, Y.; Mentel, Th. F.; Bohne, A.; Buchholz, A.; Kiendler-Scharr, A.; Kleist, E.; Spindler, C.; Tillmann, R.; Wildt, J.

    2010-08-01

    The Mediterranean region is expected to experience substantial climatic change in the next 50 years. But, possible effects of climate change on biogenic volatile organic compound (VOC) emissions as well as on the formation of secondary organic aerosols (SOA) produced from these VOC are yet unexplored. To address such issues, the effects of temperature on the VOC emissions of Mediterranean Holm Oak and small Mediterranean stand of Wild Pistacio, Aleppo Pine, and Palestine Oak have been studied in the Jülich plant aerosol atmosphere chamber. For Holm Oak the optical and microphysical properties of the resulting SOA were investigated. Monoterpenes dominated the VOC emissions from Holm Oak (97.5%) and Mediterranean stand (97%). Higher temperatures enhanced the overall VOC emission but with different ratios of the emitted species. The amount of SOA increased linearly with the emission strength with a fractional mass yield of 6.0±0.6%, independent of the detailed emission pattern. The investigated particles were highly scattering with no absorption abilities. Their average hygroscopic growth factor of 1.13±0.03 at 90% RH with a critical diameter of droplet activation was 100±4 nm at a supersaturation of 0.4%. All microphysical properties did not depend on the detailed emission pattern, in accordance with an invariant O/C ratio (0.57(+0.03/-0.1)) of the SOA observed by high resolution aerosol mass spectrometry. The increase of Holm oak emissions with temperature (≈20% per degree) was stronger than e.g. for Boreal tree species (≈10% per degree). The SOA yield for Mediterranean trees determined here is similar as for Boreal trees. Increasing mean temperature in Mediterranean areas could thus have a stronger impact on BVOC emissions and SOA formation than in areas with Boreal forests.

  18. Climatology of Aerosol Optical Properties in Southern Africa

    NASA Technical Reports Server (NTRS)

    Queface, Antonio J.; Piketh, Stuart J.; Eck, Thomas F.; Tsay, Si-Chee

    2011-01-01

    A thorough regionally dependent understanding of optical properties of aerosols and their spatial and temporal distribution is required before we can accurately evaluate aerosol effects in the climate system. Long term measurements of aerosol optical depth, Angstrom exponent and retrieved single scattering albedo and size distribution, were analyzed and compiled into an aerosol optical properties climatology for southern Africa. Monitoring of aerosol parameters have been made by the AERONET program since the middle of the last decade in southern Africa. This valuable information provided an opportunity for understanding how aerosols of different types influence the regional radiation budget. Two long term sites, Mongu in Zambia and Skukuza in South Africa formed the core sources of data in this study. Results show that seasonal variation of aerosol optical thicknesses at 500 nm in southern Africa are characterized by low seasonal multi-month mean values (0.11 to 0.17) from December to May, medium values (0.20 to 0.27) between June and August, and high to very high values (0.30 to 0.46) during September to November. The spatial distribution of aerosol loadings shows that the north has high magnitudes than the south in the biomass burning season and the opposite in none biomass burning season. From the present aerosol data, no long term discernable trends are observable in aerosol concentrations in this region. This study also reveals that biomass burning aerosols contribute the bulk of the aerosol loading in August-October. Therefore if biomass burning could be controlled, southern Africa will experience a significant reduction in total atmospheric aerosol loading. In addition to that, aerosol volume size distribution is characterized by low concentrations in the non biomass burning period and well balanced particle size contributions of both coarse and fine modes. In contrast high concentrations are characteristic of biomass burning period, combined with

  19. Studying Taklamakan aerosol properties with lidar (STAPL)

    NASA Astrophysics Data System (ADS)

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

    2013-10-01

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

  20. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2012-11-01

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

  2. 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.

  3. Application of aerosol optical properties to estimate aerosol type from ground-based remote sensing observation at urban area of northeastern China

    NASA Astrophysics Data System (ADS)

    Che, Huizheng; Zhao, Hujia; Wu, Yunfei; Xia, Xiangao; Zhu, Jun; Dubovik, Oleg; Estelles, Victor; Ma, Yanjun; Wang, Yangfeng; Wang, Hong; Wang, Yaqiang; Zhang, Xiaoye; Shi, Guangyu

    2015-09-01

    Aerosol optical properties were derived from ground-based sunphotometer observations between 2009-2013 at three urban sites of Shenyang, Anshan, Fushun in northeastern China. The annual means for extinction aerosol optical depths (EAOD) at 500 nm were 0.57±0.38, 0.52±0.35, and 0.41±0.31 at Shenyang, Anshan, Fushun, respectively. The corresponding annual means for the extinction Angstrom exponents (EAE) computed for the wavelengths of 440 and 870 nm were 0.86±0.32, 0.86±0.34 and 0.91±0.35, respectively, indicating that urban area of Northeast China were affected by both coarse and fine particles. Hygroscopic growth in summer and incursions of dust aerosols in spring were evidently revealed from the analysis of the relationship between EAE and δEAE (the EAE difference, δEAE=EAE(440,670)-EAE(670,870)). The annual mean absorption aerosol optical depths (AAOD440 nm) values at Shenyang, Anshan, Fushun were 0.15±0.11, 0.10±0.07, 0.08±0.04, respectively. The annual mean absorption Angstrom exponents (AAE440-870 nm) values were 0.86±0.24, 1.19±0.39, 1.33±0.36 at Shenyang, Anshan, Fushun, respectively. When the AAEs were close to unity at Anshan, the absorption aerosol particles evidently consisted of black carbon from coal combustion and motor vehicles. Larger AAEs at Fushun were indicative of absorbing aerosols mainly from biomass burning and mineral dust. The AAE at Shenyang was<1 which may be consistent with black carbon particles with absorbing or non-absorbing coatings. Analysis of the relationship between the AAEs and extinction Angstrom exponents showed that the aerosol populations at these three sites could be classified as "mixed-small particles" including anthropogenic particles and secondary organic aerosol with highly variable sphericity fractions.

  4. An investigation of aerosol optical properties: Atmospheric implications and influences

    NASA Astrophysics Data System (ADS)

    Penaloza-Murillo, Marcos A.

    An experimental, observational, and theoretical investigation of aerosol optical properties has been made in this work to study their implications and influences on the atmosphere. In the laboratory the scientific and instrumental methodology consisted of three parts, namely, aerosol generation, optical and mass concentration measurements, and computational calculations. In particular the optical properties of ammonium sulfate and caffeine aerosol were derived from measurements made with a transmissometer cell-reciprocal- integrating nephelometer (TCRIN), equipped with a laser beam at 632.8 nm, and by applying a Mie theory computer code The aerosol generators, optical equipment and calibration procedures were reviewed. The aerosol shape and size distribution were studied by means of scanning electron microscopy and the Gumprecht- Sliepcevich/Lipofsky-Green extinction-sedimentation method. In particular the spherical and cylindrical shape were considered. During this investigation, an alternative method for obtaining the optical properties of monodisperse spherical non-absorbing aerosol using a cell-transmissometer, which is based on a linearisation of the Lambert-Beer law, was found. In addition, adapting the TCRIN to electrooptical aerosol studies, the optical properties of a circular-cylindrical aerosol of caffeine were undertaken under the condition of random orientation in relation with the laser beam, and perpendicular orientation to it. A theoretical study was conducted to assess the sensitivity of aerosol to a change of shape under different polarisation modes. The aerosol optical properties, obtained previously in the laboratory, were then used to simulate the direct radiative forcing. The calculations and results were obtained by applying a one- dimensional energy-balance box model. The influence of atmospheric aerosol on the sky brightness due to a total solar eclipse was studied using the photometric and meteorological observations made during the

  5. CMAQ validation of optical parameters and PM2.5 based on lidar and sky radiometers: a sensitivity study of optical parameters to hygroscopic aerosols

    NASA Astrophysics Data System (ADS)

    Vladutescu, Daniela Viviana; Garofalo, Erika; Gross, Barry; Moshary, Fred; Ahmed, Samir

    2009-08-01

    With the dramatically climate changing we are facing today atmospheric monitoring is of major importance. Several atmospheric monitoring instruments are used for measuring atmospheric composition, optical coefficients, PM2.5, aerosol optical depth, size distribution, PBL height and many other parameters. However an inexpensive method of determining these parameters is by use of models and one model that depicts the aerosol dynamics in the atmosphere is the Community Multi-scale Air Quality (CMAQ) model. Our paper is focused on converting CMAQ retrieval outputs into optical coefficients that can then be comparing the lidar, AERONET and TEOM measurements performed at City College of the City University of New York . Differences between the full approach and parameterized methods such as the MALM formula used in AIR-NOW are observed and comparisons with AERONET show the full modeling is in general superior to the MALM formula.

  6. Overview of ACE-Asia Spring 2001 Investigations on Aerosol Radiative Effects and Related Aerosol Properties

    NASA Technical Reports Server (NTRS)

    Russell, Philip B.; Valero, F. P. J.; Flatau, P. J.; Bergin, M.; Holben, B.; Nakajima, T.; Pilewskie, P.; Bergstrom, R.; Hipskind, R. Stephen (Technical Monitor)

    2001-01-01

    A primary, ACE-Asia objective was to quantify the interactions between aerosols and radiation in the Asia-Pacific region. Toward this end, radiometric and related aerosol measurements were made from ocean, land, air and space platforms. Models that predict aerosol fields guided the measurements and are helping integrate and interpret results. Companion overview's survey these measurement and modeling components. Here we illustrate how these components were combined to determine aerosol radiative. impacts and their relation to aerosol properties. Because clouds can obscure or change aerosol direct radiative effects, aircraft and ship sorties to measure these effects depended on predicting and finding cloud-free areas and times with interesting aerosols present. Pre-experiment satellite cloud climatologies, pre-flight aerosol and cloud forecasts, and in-flight guidance from satellite imagery all helped achieve this. Assessments of aerosol regional radiative impacts benefit from the spatiotemporal coverage of satellites, provided satellite-retrieved aerosol properties are accurate. Therefore, ACE-Asia included satellite retrieval tests, as part of many comparisons to judge the consistency (closure) among, diverse measurements. Early results include: (1) Solar spectrally resolved and broadband irradiances and optical depth measurements from the C-130 aircraft and at Kosan, Korea yielded aerosol radiative forcing efficiencies, permitting comparisons between efficiencies of ACE-Asia and INDOEX aerosols, and between dust and "pollution" aerosols. Detailed results will be presented in separate papers. (2) Based on measurements of wavelength dependent aerosol optical depth (AOD) and single scattering albedo the estimated 24-h a average aerosol radiative forcing efficiency at the surface for photosynthetically active radiation (400 - 700 nm) in Yulin, China is approx. 30 W sq m per AOD(500 nm). (3) The R/V Brown cruise from Honolulu to Sea of Japan sampled an aerosol optical

  7. Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

    NASA Technical Reports Server (NTRS)

    Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Dickerson, R. R.; Thompson, A. M.; Slutsker, I.; Li, Z.; Tripathi, S. N.; Singh, R. P.; Zibordi, G.

    2010-01-01

    Aerosols are generated in the atmosphere through anthropogenic and natural mechanisms. These sources have signatures in the aerosol optical and microphysical properties that can be used to identify the aerosol type/mixture. Spectral aerosol absorption information (absorption Angstrom exponent; AAE) used in conjunction with the particle size parameterization (extinction Angstrom exponent; EAE) can only identify the dominant absorbing aerosol type in the sample volume (e.g., black carbon vs. iron oxides in dust). This AAE/EAE relationship can be expanded to also identify non-absorbing aerosol types/mixtures by applying an absorption weighting. This new relationship provides improved aerosol type distinction when the magnitude of absorption is not equal (e.g, black carbon vs. sulfates). The Aerosol Robotic Network (AERONET) data provide spectral aerosol optical depth and single scattering albedo - key parameters used to determine EAE and AAE. The proposed aerosol type/mixture relationship is demonstrated using the long-term data archive acquired at AERONET sites within various source regions. The preliminary analysis has found that dust, sulfate, organic carbon, and black carbon aerosol types/mixtures can be determined from this AAE/EAE relationship when applying the absorption weighting for each available wavelength (Le., 440, 675, 870nm). Large, non-spherical dust particles absorb in the shorter wavelengths and the application of 440nm wavelength absorption weighting produced the best particle type definition. Sulfate particles scatter light efficiently and organic carbon particles are small near the source and aggregate over time to form larger less absorbing particles. Both sulfates and organic carbon showed generally better definition using the 870nm wavelength absorption weighting. Black carbon generation results from varying combustion rates from a number of sources including industrial processes and biomass burning. Cases with primarily black carbon showed

  8. Influence of semi-volatile aerosol on physical and optical properties of aerosol in Kathmandu valley

    NASA Astrophysics Data System (ADS)

    Shrestha, Sujan; Praveen, Ps; Adhikary, Bhupesh; Shrestha, Kundan; Panday, Arnico

    2016-04-01

    A field study was conducted in the urban atmosphere of Kathmandu valley to study the influence of the semi-volatile aerosol fraction on physical and optical properties of aerosols. The study was carried out during the 2015 pre-monsoon period. Experimental setup consisted of air from an ambient air inlet being split to two sets of identical sampling instruments. The first instrument received the ambient sample directly, while the second instrument received the air sample through a thermodenuder (TDD). Four sets of experiments were conducted to understand aerosol number, size distribution, scattering and absorption properties using Condensation Particle Counter (CPC), Scanning Mobility Particle Sizer (SMPS), Aethalometer (AE33) and Nephelometer. The influence of semi-volatile aerosols was calculated from the fraction of particles evaporated in the TDD at set temparetures: room temperature, 50°C, 100°C, 150°C, 200°C, 250°C and 300°C. Results show that, with increasing temperature, the evaporated fraction of semi-volatile aerosol also increased. At room temperature the fraction of semi-volatile aerosols was 12% while at 300°C it was as high as to 49%. Aerosol size distribution analysis shows that with an increase in TDD temperature from 50°C to 300°C, peak mobility diameter of particles shifted from around 60nm to 40nm. However we found little change in effective diameter of aerosol size distribution with increase in set TDD temperature. The change in size of aerosols due to loss of semi-volatile component has a stronger influence (~70%) in higher size bins when compared to at lower size bins (~20%). Studies using the AE33 showed that absorption by black carbon (BC) is amplified due to influence of semi-volatile aerosols by upto 37% at 880nm wavelength. Similarly nephelometer measurements showed that upto 71% of total scattering was found to be contributed by semi-volatile aerosol fraction. The scattering Angstrom Exponent (SAE) of semi-volatile aerosol

  9. Comparison of the aerosol optical properties and size distribution retrieved by sun photometer with in situ measurements at midlatitude

    NASA Astrophysics Data System (ADS)

    Chauvigné, Aurélien; Sellegri, Karine; Hervo, Maxime; Montoux, Nadège; Freville, Patrick; Goloub, Philippe

    2016-09-01

    Aerosols influence the Earth radiative budget through scattering and absorption of solar radiation. Several methods are used to investigate aerosol properties and thus quantify their direct and indirect impacts on climate. At the Puy de Dôme station, continuous high-altitude near-surface in situ measurements and low-altitude ground-based remote sensing atmospheric column measurements give the opportunity to compare the aerosol extinction measured with both methods over a 1-year period. To our knowledge, it is the first time that such a comparison is realised with continuous measurements of a high-altitude site during a long-term period. This comparison addresses to which extent near-surface in situ measurements are representative of the whole atmospheric column, the aerosol mixing layer (ML) or the free troposphere (FT). In particular, the impact of multi-aerosol layers events detected using lidar backscatter profiles is analysed. A good correlation between in situ aerosol extinction coefficient and aerosol optical depth (AOD) measured by the Aerosol Robotic Network (AERONET) sun photometer is observed with a correlation coefficient around 0.80, indicating that the in situ measurements station is representative of the overall atmospheric column. After filtering for multilayer cases and correcting for each layer optical contribution (ML and FT), the atmospheric structure seems to be the main factor influencing the comparison between the two measurement techniques. When the site lies in the ML, the in situ extinction represents 45 % of the sun photometer ML extinction while when the site lies within the FT, the in situ extinction is more than 2 times higher than the FT sun photometer extinction. Moreover, the assumption of a decreasing linear vertical aerosol profile in the whole atmosphere has been tested, significantly improving the instrumental agreement. Remote sensing retrievals of the aerosol particle size distributions (PSDs) from the sun photometer

  10. Retrieval of Spectral Aerosol Optical Properties and Their Relationship to Aerosol Chemistry During ARCTAS

    NASA Astrophysics Data System (ADS)

    Corr, C. A.; Hall, S. R.; Ullmann, K.; Shetter, R.; Anderson, B. E.; Beyersdorf, A. J.; Thornhill, K. L.; Cubison, M.; Jimenez, J. L.; Dibb, J. E.

    2010-12-01

    Aerosols are known to both absorb and scatter radiation at UV wavelengths with the degree of absorption/scattering largely dependent on aerosol chemistry. The interactions of aerosols with the UV radiation field were examined during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). Analysis focused on two case studies; one flight from the first phase of ARCTAS over Alaska and the Arctic ocean (Flight 10, April 2008) and the other from the second phase over northern Canada (Flight 17, June 2008). These flights were chosen based on availability of aircraft profiles through pollution layers and biomass burning smoke plumes with high loadings of organic aerosol during flight. Aerosol single scattering albedo (ω) was retrieved at near-UV (350-400nm) wavelengths at 1nm resolution from spectral actinic flux data collected aboard the NASA DC-8 aircraft during ARCTAS using two CCD Actinic Flux Spectroradiometers. Retrievals were performed using the Tropospheric Ultraviolet Model version 4.6 (TUV 4.6). Inputs of trace gas (e.g., NO2, SO2) concentrations, aerosol optical depth, location, time, pressure, etc. required by TUV were determined from ancillary aircraft measurements made from the DC-8. Values of ω were subsequently used to determine absorption optical depth (τabs) for each of the examined flights. Retrieval and calculation results were compared to aerosol optical properties in the visible (calculated from measurements of absorption and scattering aboard the DC-8) and the spectral dependencies characterized. Spectral ω and τabs were compared with aerosol chemistry data collected by an Aerosol Mass Spectrometer (AMS) to provide insight into the role of aerosol composition on absorption in the UV wavelength range. In particular, spectral dependencies were compared to the oxidation state of the organic aerosol (determined from AMS data) to examine the impact of aerosol processing/aging on spectral ω and τabs.

  11. Aerosol Optical Properties in Southeast Asia From AERONET Observations

    NASA Astrophysics Data System (ADS)

    Eck, T. F.; Holben, B. N.; Boonjawat, J.; Le, H. V.; Schafer, J. S.; Reid, J. S.; Dubovik, O.; Smirnov, A.

    2003-12-01

    There is little published data available on measured optical properties of aerosols in the Southeast Asian region. The AERONET project and collaborators commenced monitoring of aerosol optical properties in February 2003 at four sites in Thailand and two sites in Viet Nam to measure the primarily anthropogenic aerosols generated by biomass burning and fossil fuel combustion/ industrial emissions. Automatic sun/sky radiometers at each site measured spectral aerosol optical depth in 7 wavelengths from 340 to 1020 nm and combined with directional radiances in the almucantar, retrievals were made of spectral single scattering albedo and aerosol size distributions. Angstrom exponents, size distributions and spectral single scattering albedo of primarily biomass burning aerosols at rural sites are compared to measurements made at AERONET sites in other major biomass burning regions in tropical southern Africa, South America, and in boreal forest regions. Additionally, the aerosol single scattering albedo and size distributions measured in Bangkok, Thailand are compared with those measured at other urban sites globally. The influences of aerosols originating from other regions outside of Southeast Asia are analyzed using trajectory analyses. Specifically, cases of aerosol transport and mixing from Southern China and from India are presented.

  12. Aerosol Properties under Air Quality Control Measures of APEC 2014 in Beijing

    NASA Astrophysics Data System (ADS)

    Chen, X.; Xu, H.; Lv, Y.; Xie, Y.; Li, K.; Li, Z.; Li, D.; Ma, Y.; Mei, X.

    2015-12-01

    Because the economic and society were developing fast in the middle of last century, Los Angeles and London both were polluted by photochemical smog, which massacred thousands of people. Now, many regions are often covered by heavy haze in those large developing countries, especially in China and India. The Asia-Pacific Economic Cooperation (APEC) was held in Beijing during 5-11 November 2014. Beijing, Hebei, Tianjin, Shandong, Shanxi, Inner Mongolia reduced air pollution emissions for the APEC 2014 meeting held in Beijing. Only in Hebei province, there were 1028 factories stopped or restricted and 881 construction sites stopped. Half of the cars were prohibited driving even in the Zibo city which is 400 km far from Beijing. For scientific aims, these control measures were indeed a huge and uncommon atmospheric experiment led by the government. During the experiment, what did the "APEC Blue" mean? We analyzed aerosol properties with the data of an AERONET site in Beijing which is located 500m far from the main reception hall of APEC 2014. The Cimel solar photometers can give a series parameters of aerosol and water vapor. In this paper, we used CE318 solar photometer which is the main instrument of NASA AERONET. The CE318 of RADI belongs to the Chinese SONET (Sun-sky radiometer Observation NETwork) too. We analyzed the total, coarse and fine Aerosol Optical Depth (AOD), Fine-Mode Fraction (FMF) and Ångström exponent, Size Distribution and Real Refractive Index. In conclusion, the aerosol properties were analysed with the measurements of a sun photometer. During the APEC 2014, AOD decreased obviously with a 0.27 mean value compared with the annual mean 0.7. Around Beijing, the southern is polluted emission area including the cross part of Shandong, Shanxi, Hebei, Henan four provinces, and the northern is clean for less fine mode particles emission in the large Inner Mongolia province. In fact, during the APEC 2014, the weather condition was not good for the

  13. Seasonal behavior of PM2.5 deliquescence, crystallization, and hygroscopic growth in the Po Valley (Milan): Implications for remote sensing applications

    NASA Astrophysics Data System (ADS)

    D'Angelo, Luca; Rovelli, Grazia; Casati, Marco; Sangiorgi, Giorgia; Perrone, Maria Grazia; Bolzacchini, Ezio; Ferrero, Luca

    2016-07-01

    Atmospheric aerosols deliquescence and crystallization relative humidity (DRH and CRH) are rarely measured compared to the worldwide number of hygroscopicity measurements; this feature comes from the lack of an efficient method able to capture the whole complexity of chemical composition of aerosols. Despite this, the knowledge of both DRH and CRH are crucial for a correct parameterization of the aerosol hygroscopic growth used in different applications, among which the remote sensing is very important. In this paper, a newly developed technique (direct current conductance method) was applied in an aerosol chamber to Milan PM2.5 samples, to identify aerosol DRH and CRH both during winter and summer. These results were compared with those independently obtained by gravimetric measurements conducted in the chamber using a microbalance. Microbalance data allowed also the determination of the mass hygroscopic growth factor on the collected PM2.5 samples. Results evidenced first a good agreement between the two methods (RMSE = 2.7% and 2.3% for DRH and CRH, respectively). Collected data evidenced the hysteresis behavior of ambient particles and variability in both DRH and CRH between the two seasons. Summer samples showed higher DRH and CRH (on average 71.4 ± 1.0% RH and 62.6 ± 1.2% RH, respectively) than the winter ones (on average 55.2 ± 0.7% RH and 46.9 ± 0.6% RH). This behavior was related to the higher content of sulfates during the summer season. Conversely, the mass hygroscopic growth factor at 90% RH was higher for winter samples (2.76 ± 0.06) with respect to the summer ones (1.91 ± 0.11). Since hysteresis behavior affects optical properties of aerosols, when RH conditions are within the loop, the hygroscopic growth factor could be assigned in a wrong way. Thus, the growth factor was calculated within the hysteresis loop for both upper and lower branches: results showed that difference in hygroscopic growth factor could reach up the 24%.

  14. 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.

  15. Optical properties of aerosol contaminated cloud derived from MODIS instrument

    NASA Astrophysics Data System (ADS)

    Mei, Linlu; Rozanov, Vladimir; Lelli, Luca; Vountas, Marco; Burrows, John P.

    2016-04-01

    The presence of absorbing aerosols above/within cloud can reduce the amount of up-welling radiation in visible (VIS) and short-wave infrared and darken the spectral reflectance when compared with a spectrum of a clean cloud observed by satellite instruments (Jethva et al., 2013). Cloud properties retrieval for aerosol contaminated cases is a great challenge. Even small additional injection of aerosol particles into clouds in the cleanest regions of Earth's atmosphere will cause significant effect on those clouds and on climate forcing (Koren et al., 2014; Rosenfeld et al., 2014) because the micro-physical cloud process are non-linear with respect to the aerosol loading. The current cloud products like Moderate Resolution Imaging Spectroradiometer (MODIS) ignoring the aerosol effect for the retrieval, which may cause significant error in the satellite-derived cloud properties. In this paper, a new cloud properties retrieval method, considering aerosol effect, based on the weighting-function (WF) method, is presented. The retrieval results shows that the WF retrieved cloud properties (e.g COT) agrees quite well with MODIS COT product for relative clear atmosphere (AOT ≤ 0.4) while there is a large difference for large aerosol loading. The MODIS COT product is underestimated for at least 2 - 3 times for AOT>0.4, and this underestimation increases with the increase of AOT.

  16. Aerosol physical properties in the stratosphere (APPS) radiometer design

    NASA Technical Reports Server (NTRS)

    Gray, C. R.; Woodin, E. A.; Anderson, T. J.; Magee, R. J.; Karthas, G. W.

    1977-01-01

    The measurement concepts and radiometer design developed to obtain earth-limb spectral radiance measurements for the Aerosol Physical Properties in the Stratosphere (APPS) measurement program are presented. The measurements made by a radiometer of this design can be inverted to yield vertical profiles of Rayleigh scatterers, ozone, nitrogen dioxide, aerosol extinction, and aerosol physical properties, including a Junge size-distribution parameter, and a real and imaginary index of refraction. The radiometer design provides the capacity for remote sensing of stratospheric constituents from space on platforms such as the space shuttle and satellites, and therefore provides for global measurements on a daily basis.

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  18. Satellite remote sensing of aerosol and cloud properties over Eurasia

    NASA Astrophysics Data System (ADS)

    Sogacheva, Larisa; Kolmonen, Pekka; Saponaro, Giulia; Virtanen, Timo; Rodriguez, Edith; Sundström, Anu-Maija; Atlaskina, Ksenia; de Leeuw, Gerrit

    2015-04-01

    Satellite remote sensing provides the spatial distribution of aerosol and cloud properties over a wide area. In our studies large data sets are used for statistical studies on aerosol and cloud interaction in an area over Fennoscandia, the Baltic Sea and adjacent regions over the European mainland. This area spans several regimes with different influences on aerosol cloud interaction such as a the transition from relative clean air over Fennoscandia to more anthropogenically polluted air further south, and the influence maritime air over the Baltic and oceanic air advected from the North Atlantic. Anthropogenic pollution occurs in several parts of the study area, and in particular near densely populated areas and megacities, but also in industrialized areas and areas with dense traffic. The aerosol in such areas is quite different from that produced over the boreal forest and has different effects on air quality and climate. Studies have been made on the effects of aerosols on air quality and on the radiation balance in China. The aim of the study is to study the effect of these different regimes on aerosol-cloud interaction using a large aerosol and cloud data set retrieved with the (Advanced) Along Track Scanning Radiometer (A)ATSR Dual View algorithm (ADV) further developed at Finnish Meteorological Institute and aerosol and cloud data provided by MODIS. Retrieval algorithms for aerosol and clouds have been developed for the (A)ATSR, consisting of a series of instruments of which we use the second and third one: ATSR-2 which flew on the ERS-2 satellite (1995-2003) and AATSR which flew on the ENVISAT satellite (2002-2012) (both from the European Space Agency, ESA). The ADV algorithm provides aerosol data on a global scale with a default resolution of 10x10km2 (L2) and an aggregate product on 1x1 degree (L3). Optional, a 1x1 km2 retrieval products is available over smaller areas for specific studies. Since for the retrieval of AOD no prior knowledge is needed on

  19. Summer-winter differences in the relationships among background southeastern U.S. aerosol optical, micro-physical, and chemical properties

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    Relationships among aerosol optical, micro-physical, and chemical properties are useful for evaluating regional climate models, developing satellite-based aerosol retrievals, and understanding aerosol sources and processes. Since aerosol loading and optical properties vary primarily on seasonal scales in the southeastern U.S., it is important that such studies be carried out over multiple seasons but few (if any) such multi-season studies have been conducted in the region. The high-elevation, semi-rural AppalAIR facility at Appalachian State University in Boone, NC (1080m ASL, 36.210N, 81.690W) is home to the only co-located NOAA-ESRL and AERONET monitoring sites in the eastern U.S. Measurements of size-resolved, non-refractory sub-1μm aerosol composition were also made by a co-located AMS during the 2012-2013 summers and 2013 winter. Systematic relationships among aerosol optical, microphysical, and chemical properties were developed to better understand aerosol sources and processes and for use in higher-dimension aerosol classification schemes. Some of the major findings will be presented. Higher values of lower tropospheric aerosol light scattering coefficient at 550nm (a proxy for aerosol loading) are associated with higher single-scattering albedo (SSA) and lower hemispheric backscatter fraction (b) during both summer and winter. Absorption Angstrom exponent (AAE) is typically well under 1 during summer and near 1.3-1.4 during winter. Lowest summer AAE values coincide with large, highly-reflective particles and higher aerosol light scattering coefficient but summer AAE is only weakly anti-correlated with organic and sulfate mass concentrations. Winter AAE is consistent with a mixture of elemental carbon and light-absorbing organic carbon, possibly influenced by regional residential wood-burning during winter. The hygroscopic dependence of visible light scattering is sensitive to sulfate and organic aerosol mass fractions during both summer and winter

  20. An aerosol climatology for a rapidly growing arid region (southern Arizona): Major aerosol species and remotely sensed aerosol properties

    PubMed Central

    Sorooshian, Armin; Wonaschütz, Anna; Jarjour, Elias G.; Hashimoto, Bryce I.; Schichtel, Bret A.; Betterton, Eric A.

    2014-01-01

    This study reports a comprehensive characterization of atmospheric aerosol particle properties in relation to meteorological and back trajectory data in the southern Arizona region, which includes two of the fastest growing metropolitan areas in the United States (Phoenix and Tucson). Multiple data sets (MODIS, AERONET, OMI/TOMS, MISR, GOCART, ground-based aerosol measurements) are used to examine monthly trends in aerosol composition, aerosol optical depth (AOD), and aerosol size. Fine soil, sulfate, and organics dominate PM2.5 mass in the region. Dust strongly influences the region between March and July owing to the dry and hot meteorological conditions and back trajectory patterns. Because monsoon precipitation begins typically in July, dust levels decrease, while AOD, sulfate, and organic aerosol reach their maximum levels because of summertime photochemistry and monsoon moisture. Evidence points to biogenic volatile organic compounds being a significant source of secondary organic aerosol in this region. Biomass burning also is shown to be a major contributor to the carbonaceous aerosol budget in the region, leading to enhanced organic and elemental carbon levels aloft at a sky-island site north of Tucson (Mt. Lemmon). Phoenix exhibits different monthly trends for aerosol components in comparison with the other sites owing to the strong influence of fossil carbon and anthropogenic dust. Trend analyses between 1988 and 2009 indicate that the strongest statistically significant trends are reductions in sulfate, elemental carbon, and organic carbon, and increases in fine soil during the spring (March–May) at select sites. These results can be explained by population growth, land-use changes, and improved source controls. PMID:24707452

  1. Airborne Lidar Measurements of Aerosol Optical Properties During SAFARI-2000

    NASA Technical Reports Server (NTRS)

    McGill, M. J.; Hlavka, D. L.; Hart, W. D.; Welton, E. J.; Campbell, J. R.; Starr, David OC. (Technical Monitor)

    2002-01-01

    The Cloud Physics Lidar (CPL) operated onboard the NASA ER-2 high altitude aircraft during the SAFARI-2000 field campaign. The CPL provided high spatial resolution measurements of aerosol optical properties at both 1064 nm and 532 nm. We present here results of planetary boundary layer (PBL) aerosol optical depth analysis and profiles of aerosol extinction. Variation of optical depth and extinction are examined as a function of regional location. The wide-scale aerosol mapping obtained by the CPL is a unique data set that will aid in future studies of aerosol transport. Comparisons between the airborne CPL and ground-based MicroPulse Lidar Network (MPL-Net) sites are shown to have good agreement.

  2. Retrieval of Aerosol Microphysical Properties from MFRSR Observations

    SciTech Connect

    Kassianov, Evgueni I; Barnard, James C; Ackerman, Thomas P

    2006-05-01

    Aerosols can have significant impact on the radiative and heat balance of the Earth-atmosphere system by absorbing and scattering solar radiation (direct aerosol effect) and altering cloud optical properties and suppressing precipitation (indirect aerosol effect). However, both the sign and magnitude of the aerosol impact has proven difficult to determine due to incomplete knowledge of aerosol properties and their strong temporal and spatial variations. Reduction of these uncertainties requires an accurate global inventory of aerosol microphysical properties, such as size distribution and the refractive index. Multi-filter Rotating Shadowband Radiometers (MFRSRs) are widely deployed over the world (e.g., the surface radiation budget network). These radiometers provide measurements of the direct and the diffuse solar irradiances at six wavelengths (0.415, 0.5, 0.615, 0.673, 0.870 and 0.94 ). Currently, the direct irradiance observations are used to derive routinely spectral values of the aerosol optical depth only. We propose a simple retrieval technique that significantly extends the capability of the MFRSR to study atmospheric aerosols. In our retrieval, we assume the shape of aerosol size distribution (e.g., combination of three lognormal distributions) and the value of the real refractive index. The technique consists of three steps that compose an iterative scheme. The first step obtains the aerosol size distribution from the spectral measurements of the direct irradiance (for a given complex refractive index). To reduce the effect of ozone and water vapor contamination, we use wavelengths where ozone and water vapor weakly affect the direct irradiance (0.415 mu and 0.870 mu). The second step determines the effective value of the imaginary refractive index from the diffuse irradiance (for the aerosol size distribution determined during the first step). To reduce the effect of the surface albedo on the retrievals, we select a wavelength where the surface albedo

  3. Experimentally measured morphology of biomass burning aerosol and its impacts on CCN ability

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Espinoza, C.; Asa-Awuku, A.

    2014-05-01

    This study examines the morphological properties of freshly emitted and atmospherically aged aerosols from biomass burning. The impacts of particle morphology assumptions on hygroscopic predictions are examined. Chamber experiments were conducted at the UC-Riverside Center for Environmental Research and Technology (CE-CERT) Atmospheric Processes Lab using two biomass fuel sources, manzanita and chamise. Morphological data was obtained through the use of an aerosol particle mass analyzer (APM), scanning mobility particle sizer (SMPS) system and transmission electron microscopy (TEM). Data from these instruments was used to calculate both a dynamic shape factor and a fractal-like dimension for the biomass burning emissions. This data was then used with κ-Köhler theory to adjust the calculated hygroscopicity for experimentally determined morphological characteristics of the aerosol. Laboratory measurement of biomass burning aerosol from two chaparral fuels show that particles are non-spherical with dynamic shape factors greater than 1.15 for aerosol sizes relevant to cloud condensation nuclei (CCN) activation. Accounting for particle morphology can shift the hygroscopicity parameter κ by 0.15 or more. To our knowledge, this work provides the first laboratory chamber measurements of morphological characteristics for biomass burning cloud condensation nuclei and provides experimental particle shape evidence to support the variation in reported hygroscopicities of the complex aerosol.

  4. Experimentally measured morphology of biomass burning aerosol and its impacts on CCN ability

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Espinoza, C.; Asa-Awuku, A.

    2015-02-01

    This study examines the morphological properties of freshly emitted and atmospherically aged aerosols from biomass burning. The impacts of particle morphology assumptions on hygroscopic predictions are examined. Chamber experiments were conducted at the University of California, Riverside, Center for Environmental Research and Technology (CE-CERT) atmospheric processes lab using two biomass fuel sources: manzanita and chamise. Morphological data was obtained through the use of an aerosol particle mass analyzer (APM), scanning mobility particle sizer (SMPS) system and transmission electron microscope (TEM). Data from these instruments was used to calculate both a dynamic shape factor and a fractal-like dimension for the biomass burning emissions. This data was then used with κ-Köhler theory to adjust the calculated hygroscopicity for experimentally determined morphological characteristics of the aerosol. Laboratory measurement of biomass burning aerosol from two chaparral fuels show that particles are nonspherical with dynamic shape factors greater than 1.15 for aerosol sizes relevant to cloud condensation nuclei (CCN) activation. Accounting for particle morphology can shift the hygroscopicity parameter by 0.15 or more. To our knowledge, this work provides the first laboratory chamber measurements of morphological characteristics for biomass burning cloud condensation nuclei and provides experimental particle shape evidence to support the variation in reported hygroscopicities of the complex aerosol.

  5. Aerosol properties over south india during different seasons

    NASA Astrophysics Data System (ADS)

    Sivaprasad, P.; Babu, C. A.; Jayakrishnan, P. R.

    Aerosols play an important role in the radiation balance and cloud properties, thereby affect the entire climatology of the earth-atmosphere system. Besides natural sources like dust, seasalt and natural sulphates, anthropogenic activities also inject aerosols like soot and industrial sulphates. Of these sea-salt and sulphates scatter the solar radiation. Soot is an absorbing aerosol while soil dust and organic matters are partly absorbing aerosols. Wind and rainfall are major factors affecting the transportation and deposition of the aerosols. India is a country blessed with plenty of monsoon rains. Winter (December to February), summer (March to May), monsoon (June to September) and post monsoon (October to November) are the four seasons over the region. Aerosol properties vary according to the season. Natural aerosols blown from the deserts have a major role in the aerosol optical depth over India. Of this, dust from Arabian desert that is carried by the winds are most important. The aerosol optical depth of south India is entirely different from that of north India. Maximum aerosol concentration is found over Gangetic plane in most of the seasons, whereas entire south India shows less aerosol optical depth. In the present study the aerosol properties of south India is analysed in general. Particular analysis is carried out for the four regions in the east and west coasts around Chennai, Kolkotha, Mumbai and Cochin. Chennai and Kolkotha are situated in the east coast whereas Cochin and Mumbai are in the west coast. These are industrial cities in India. Chennai region does not get monsoon rainfall since it is situated in the leeward side of Western ghats. But in the post monsoon season Chennai gets good amount of rainfall. Other three regions get good amount of rainfall during monsoon season. The study uses Terra MODIS, TOMS, NCEP/NCAR and TRMM data. Aerosol properties are analysed using Terra MODIS and Nimbus TOMS data. The variations of the aerosol optical

  6. Particle Property Data Quality Flags for the MISR Aerosol Product

    NASA Astrophysics Data System (ADS)

    Gaitley, B. J.; Kahn, R. A.; Garay, M. J.

    2013-12-01

    The MISR instrument aboard the NASA Earth Observing System's Terra satellite has the unique capability to retrieve aerosol properties under favorable conditions. General aerosol type retrieval quality guidelines are provided in the MISR Data Quality Statement and related publications. The retrieved value of aerosol type is more sensitive to scene conditions than aerosol optical depth, and more difficult to validate, as there is very little coincident aerosol type validation data. Here we report on the steps we are taking to provide an aerosol-type data quality flag, to be provided with each individual retrieval result. Due to the lack of validation data for comparison, our main approach is to evaluate the self-consistency of aerosol type retrieval values for regions where particular aerosol types are known to dominate. Some factors affecting aerosol type retrieval quality that can be assessed pre-retrieval are the number of MISR cameras available, the range of scattering angles viewed, and surface conditions such as shallow water or seasonal coastal runoff. Factors that must be assessed post-retrieval include values of retrieved aerosol optical depth and the number and type of mixtures successfully passing the MISR algorithm acceptance criteria. Regional monthly plots with MISR measurements binned at 0.5 degree resolution and color-coded stratification of one or more parameters are the main tools for identifying locations and times where different aerosol types are retrieved. The statistics of individual MISR values such as mid-visible AOD, number and type of mixtures passing, number of cameras used, the range and maximum scattering angles, are studied as joint distributions on a region-by-region basis. From these, a synthesis of the self-consistency and agreement with expectation is made, effectively indicating the quality of the aerosol type constrains to the extent possible, and thresholds for assigning quality flags are assessed. Multiple-month summaries

  7. Estimation of aerosol optical properties from all-sky imagers

    NASA Astrophysics Data System (ADS)

    Kazantzidis, Andreas; Tzoumanikas, Panagiotis; Salamalikis, Vasilios; Wilbert, Stefan; Prahl, Christoph

    2015-04-01

    Aerosols are one of the most important constituents in the atmosphere that affect the incoming solar radiation, either directly through absorbing and scattering processes or indirectly by changing the optical properties and lifetime of clouds. Under clear skies, aerosols become the dominant factor that affect the intensity of solar irradiance reaching the ground. It has been shown that the variability in direct normal irradiance (DNI) due to aerosols is more important than the one induced in global horizontal irradiance (GHI), while the uncertainty in its calculation is dominated by uncertainties in the aerosol optical properties. In recent years, all-sky imagers are used for the detection of cloud coverage, type and velocity in a bouquet of applications including solar irradiance resource and forecasting. However, information about the optical properties of aerosols could be derived with the same instrumentation. In this study, the aerosol optical properties are estimated with the synergetic use of all-sky images, complementary data from the Aerosol Robotic Network (AERONET) and calculations from a radiative transfer model. The area of interest is Plataforma Solar de Almería (PSA), Tabernas, Spain and data from a 5 month period are analyzed. The proposed methodology includes look-up-tables (LUTs) of diffuse sky radiance of Red (R), Green (G) and Blue (B) channels at several zenith and azimuth angles and for different atmospheric conditions (Angström α and β, single scattering albedo, precipitable water, solar zenith angle). Based on the LUTS, results from the CIMEL photometer at PSA were used to estimate the RGB radiances for the actual conditions at this site. The methodology is accompanied by a detailed evaluation of its robustness, the development and evaluation of the inversion algorithm (derive aerosol optical properties from RGB image values) and a sensitivity analysis about how the pre-mentioned atmospheric parameters affect the results.

  8. Climatology and Characteristics of Aerosol Optical Properties in the Arctic

    NASA Astrophysics Data System (ADS)

    Schmeisser, Lauren; Ogren, John; Backman, John; Asmi, Eija; Andrews, Elisabeth; Jefferson, Anne; Bergin, Michael; Tunved, Peter; Sharma, Sangeeta; Starkweather, Sandra

    2016-04-01

    Within the Arctic, climate forcers like atmospheric aerosols are important contributors to the observed warming and environmental changes in the region. Quantifying the forcing by aerosols in the Arctic is especially difficult, given short aerosol lifetimes, annual variability in illumination and surface albedo, stratified atmospheric conditions, complex feedbacks, and long-range aerosol transport. However, in-situ surface measurements of Arctic aerosol optical properties can be used to constrain variability of light scattering and absorption, identify potential particle sources, and help evaluate the resulting forcing. Data from six WMO Global Atmosphere Watch stations are presented: Alert, Canada (ALT); Barrow, Alaska (BRW); Pallas, Finland (PAL); Summit, Greenland (SUM); Tiksi, Russia (TIK); and Zeppelin Mountain, Norway (ZEP). These sites contribute to the International Arctic System for Observing the Atmosphere (IASOA), which facilitates Arctic-wide data collection and analysis. Climatologies of aerosol optical properties from each station show differences in magnitude and variability of observed parameters. For example, most stations (ALT, BRW, SUM, TIK, ZEP) experience maximum scattering in winter/spring, while PAL exhibits maximum scattering in the summer. The observed range in scattering across these sites is large (almost an order of magnitude) - SUM has the lowest annual median scattering at 0.82 Mm-1 while BRW has the highest at 6.9 Mm-1. A closer look at systematic variability between optical properties at each station, as well as site back trajectories, suggest differences in aerosol processes, sources and transport. The development of consistent climatologies and additional analyses like the ones presented here can help provide a better understanding of trans-Arctic aerosol variability, which can be an asset for improving aerosol models in this unique and remote region.

  9. Improving satellite-retrieved aerosol microphysical properties using GOCART data

    NASA Astrophysics Data System (ADS)

    Li, S.; Kahn, R.; Chin, M.; Garay, M. J.; Liu, Y.

    2015-03-01

    The Multi-angle Imaging SpectroRadiometer (MISR) aboard the NASA Earth Observing System's Terra satellite can provide more reliable aerosol optical depth (AOD) and better constraints on particle size (Ångström exponent, or ANG), sphericity, and single-scattering albedo (SSA) than many other satellite instruments. However, many aerosol mixtures pass the algorithm acceptance criteria, yielding a poor constraint, when the particle-type information in the MISR radiances is low, typically at low AOD. We investigate adding value to the MISR aerosol product under these conditions by filtering the list of MISR-retrieved mixtures based on agreement between the mixture ANG and absorbing AOD (AAOD) values, and simulated aerosol properties from the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. MISR-GOCART ANG difference and AAOD ratio thresholds for applying GOCART constraints were determined based on coincident AOD, ANG, and AAOD measurements from the AErosol RObotic NETwork (AERONET). The results were validated by comparing the adjusted MISR aerosol optical properties over the contiguous USA between 2006 and 2009 with additional AERONET data. The correlation coefficient (r) between the adjusted MISR ANG derived from this study and AERONET improves to 0.45, compared to 0.29 for the MISR Version 22 standard product. The ratio of the adjusted MISR AAOD to AERONET increases to 0.74, compared to 0.5 for the MISR operational retrieval. These improvements occur primarily when AOD < 0.2 for ANG and AOD < 0.5 for AAOD. Spatial and temporal differences among the aerosol optical properties of MISR V22, GOCART, and the adjusted MISR are traced to (1) GOCART underestimation of AOD and ANG in polluted regions; (2) aerosol mixtures lacking in the MISR Version 22 algorithm climatology; (3) low MISR sensitivity to particle type under some conditions; and (4) parameters and thresholds used in our method.

  10. CCN Hygroscopicity Variability

    NASA Astrophysics Data System (ADS)

    Hudson, J. G.; Jha, V.; Noble, S.

    2008-12-01

    Lack of variability of CCN sizes led Dusek et al. (2006) to suggest that CCN could be deduced from particle size measurements alone, which are easier, more readily available, less controversial and more amenable to remote sensing. However, Hudson and Da (1996) and Hudson (2007) showed much more CCN size variability that makes it impossible to deduce CCN concentrations from size distribution measurements using a single relationship between size and CCN. But Dusek et al. (2006) also suggested that CCN sizes may be consistent within various air masses. This was indeed suggested by Hudson and Da (2006) and Hudson (2007). CCN were generally found to be larger (less hygroscopic) in more polluted air masses. This led Andreae and Rosenfeld (2008) to reassert the claim by Dusek et al. that as long as the air mass can be characterized as maritime or continental/polluted then particle size measurements can be used to approximate CCN concentrations. Here we present further measurements of CCN sizes that discount even this. The recent measurements, all of which are from aircraft, come from the PASE project in Aug.-Sep., 2007 at Christmas Island 2 degrees N latitude directly south of Honolulu, the ICE-L project, Nov.-Dec., 2007 over Colorado and Wyoming, and the POST project July-Aug., 2008 off the central California coast. The extremely remote PASE measurements were generally consistent with previous maritime measurements in that the CCN were very hygroscopic, similar to soluble salts like ammonium sulfate. However, the larger particles (>~150nm) were consistently less hygroscopic. This mixture of hygroscopicities (B) where B decreased with particle size was unexpected and would complicate deductions of CCN concentrations from size distribution measurements. Although the POST measurements displayed nearly identical total particle (CN) and CCN concentrations to the PASE measurements, the CCN were significantly less hygroscopic than PASE. The POST B values were intermediate to

  11. Remote Sensing of Spectral Aerosol Properties: A Classroom Experience

    NASA Technical Reports Server (NTRS)

    Levy, Robert C.; Pinker, Rachel T.

    2006-01-01

    Bridging the gap between current research and the classroom is a major challenge to today s instructor, especially in the sciences where progress happens quickly. NASA Goddard Space Flight Center and the University of Maryland teamed up in designing a graduate class project intended to provide a hands-on introduction to the physical basis for the retrieval of aerosol properties from state-of-the-art MODIS observations. Students learned to recognize spectral signatures of atmospheric aerosols and to perform spectral inversions. They became acquainted with the operational MODIS aerosol retrieval algorithm over oceans, and methods for its evaluation, including comparisons with groundbased AERONET sun-photometer data.

  12. Combined aerosol in-situ measurements during the SALTRACE field experiment for the investigation of Saharan mineral dust microphysical and CCN properties and their spatial-temporal evolution during trans-Atlantic long-range transport

    NASA Astrophysics Data System (ADS)

    Walser, Adrian; Dollner, Maximilian; Sauer, Daniel; Weinzierl, Bernadett

    2015-04-01

    The Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) was a field experiment conducted in June/July 2013, which aimed to investigate the transport and modification of Saharan mineral dust from the Sahara across the Atlantic Ocean to the Caribbean. In addition to ground-based measurements and satellite remote sensing, the DLR Falcon research aircraft was equipped with a number of aerosol in-situ instruments to gain direct information on the properties of airborne aerosol such as size distributions, microphysical, optical and cloud-condensation nuclei (CCN) properties. For the first time, several outbreaks of Saharan dust were probed with the same airborne instrumentation on both sides of the Atlantic. During transport, various processes may take place that modify the aerosol composition. Dry and wet deposition lead to a size-dependent aerosol removal. In case of wet deposition, the removal additionally depends on the particle's ability to act as CCN. Processes in the aqueous phase in subsequently re-evaporating cloud droplets can further alter microphysical and CCN properties of re-released particles. All resulting changes in the size distribution and particle properties impact the radiative feedback and CCN activity of the aged aerosol. This study aims to use combined airborne in-situ measurements to retrieve and compare vertically resolved aerosol size distributions, microphysical and CCN properties for both, short-range transported Saharan dust in the Cape Verde region and long-range transported dust in the Caribbean. We use this data to investigate the influence of long-range transport and associated processes on those properties. We will present vertical profiles of size-resolved aerosol concentrations and volatile fractions as well as CCN activated fractions and draw conclusions for aerosol mixing state, CCN activation diameters and particle hygroscopicities. We will discuss differences in vertical profiles and

  13. UManSysProp: An online and open-source facility for molecular property prediction and atmospheric aerosol calculations

    NASA Astrophysics Data System (ADS)

    Topping, David; Barley, Mark; McFiggans, Gordon; Aumont, Bernard

    2016-04-01

    The many thousands of individual aerosol components ensure that explicit manual calculation of properties that influence their environmental impacts is laborious and time-consuming. The emergence of explicit automatic mechanism generation techniques, including up to many millions of individual gas phase products as aerosol precursors, renders manual calculations impossible and automation is necessary. It can be difficult to establish what factors are responsible for the outcome of a model prediction. This is particularly true when the number of components might be high in, for example, SOA mass partitioning simulations. It then becomes difficult for others in the community to assess the results presented. This might be complicated by the need to include pure component vapour pressures or activity coefficient predictions for a wide range of highly multifunctional compounds. It isn't clear to what extent replication of results is ever achieved for a range of aerosol simulations. Whilst this might also be an issue with results from instrumentation, the development of community driven software at least enables modellers to tackle this problem directly. Here we describe the development and application of a new web based facility, UManSysProp, to tackle such issues. Current facilities include: pure component vapour pressures, critical properties and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential of mixed inorganic/organic aerosol particles with associated Kappa-Kohler values; absorptive partitioning calculations with/without a treatment of non-ideality. The website can be found here: http://umansysprop.seaes.manchester.ac.uk/

  14. Organic Aerosols from SÃO Paulo and its Relationship with Aerosol Absorption and Scattering Properties

    NASA Astrophysics Data System (ADS)

    Artaxo, P.; Brito, J. F.; Rizzo, L. V.

    2012-12-01

    The megacity of São Paulo with its 19 million people and 7 million cars is a challenge from the point of view of air pollution. High levels of organic aerosols, PM10, black carbon and ozone and the peculiar situation of the large scale use of ethanol fuel makes it a special case. Little is known about the impact of ethanol on air quality and human health and the increase of ethanol as vehicle fuel is rising worldwide An experiment was designed to physico-chemical properties of aerosols in São Paulo, as well as their optical properties. Aerosol size distribution in the size range of 1nm to 10 micrometers is being measured with a Helsinki University SMPS (Scanning Mobility Particle Sizer), an NAIS (Neutral ion Spectrometer) and a GRIMM OPC (Optical Particle Counter). Optical properties are being measured with a TSI Nephelometer and a Thermo MAAP (Multi Angle Absorption Photometer). A CIMEL sunphotometer from the AERONET network measure the aerosol optical depth. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to real-time VOC analysis and aerosol composition, respectively. The ACSM was operated for 3 months continuosly during teh wintertime of 2012. The measured total particle concentration typically varies between 10,000 and 30,000 cm-3 being the lowest late in the night and highest around noon and frequently exceeding 50,000 cm-3. Clear diurnal patterns in aerosol optical properties were observed. Scattering and absorption coefficients typically range between 20 and 100 Mm-1 at 450 nm, and between 10 to 40 Mm-1 at 637 nm, respectively, both of them peaking at 7:00 local time, the morning rush hour. The corresponding single scattering albedo varies between 0.50 and 0.85, indicating a significant contribution of primary absorbing particles to the aerosol population. During the first month a total of seven new particle formation events were observed with growth rates ranging from 9 to 25

  15. Aerosol optical properties and their radiative effects in northern China

    NASA Astrophysics Data System (ADS)

    Li, Zhanqing; Xia, Xiangao; Cribb, Maureen; Mi, Wen; Holben, Brent; Wang, Pucai; Chen, Hongbin; Tsay, Si-Chee; Eck, T. F.; Zhao, Fengsheng; Dutton, E. G.; Dickerson, R. E.

    2007-11-01

    As a fast developing country covering a large territory, China is experiencing rapid environmental changes. High concentrations of aerosols with diverse properties are emitted in the region, providing a unique opportunity for understanding the impact of environmental changes on climate. Until very recently, few observational studies were conducted in the source regions. The East Asian Study of Tropospheric Aerosols: An International Regional Experiment (EAST-AIRE) attempts to characterize the physical, optical and chemical properties of the aerosols and their effects on climate over China. This study presents some preliminary results using continuous high-quality measurements of aerosol, cloud and radiative quantities made at the first EAST-AIRE baseline station at Xianghe, about 70 km east of Beijing over a period of one year (September 2004 to September 2005). It was found that the region is often covered by a thick layer of haze (with a yearly mean aerosol optical depth equal to 0.82 at 500 nm and maximum greater than 4) due primarily to anthropogenic emissions. An abrupt "cleanup" of the haze often took place in a matter of one day or less because of the passage of cold fronts. The mean single scattering albedo is approximately 0.9 but has strong day-to-day variations with maximum monthly averages occurring during the summer. Large aerosol loading and strong absorption lead to a very large aerosol radiative effect at the surface (the annual 24-hour mean values equals 24 W m-2), but a much smaller aerosol radiative effect at the top of the atmosphere (one tenth of the surface value). The boundary atmosphere is thus heated dramatically during the daytime, which may affect atmospheric stability and cloud formation. In comparison, the cloud radiative effect at the surface is only moderately higher (-41 W m-2) than the aerosol radiative effect at the surface.

  16. The Chemical and Microphysical Properties of Secondary Organic Aerosols from Holm Oak Emissions

    NASA Astrophysics Data System (ADS)

    Lang-Yona, Naama; Rudich, Yinon; Thomas, Mentel; Angela, Buchholz; Astrid, Kiendler-Scharr; Einhard, Kleist; Christian, Spindler; Ralf, Tillmann; Jürgen, Wildt

    2010-05-01

    Plant-emitted volatile organic compounds (VOC) undergo atmospheric oxidation, which leads to the formation of secondary organic aerosols (SOA). Large uncertainties exist about possible climatic effects on SOA formation from biogenic sources. Therefore it is important to investigate the impact of environmental conditions on the plants' emissions, on the formation of biogenic SOA, and on SOA properties in order to understand possible climatic impacts. The Mediterranean region is expected to experience substantial climatic change in the next 50 years and the possible effects on biogenic emissions are yet unexplored. To address such issues, the effects of temperature and light intensity on Mediterranean Holm Oak VOC emissions, as well as on microphysical properties and chemical composition of the resulting SOA have been studied in the Jülich plant aerosol atmosphere chamber. We studied SOA formation from Holm Oak under conditions possibly simulating future climate warming. Monoterpenes dominate the VOC emissions from Holm Oak (97.5%) and temperature increase enhanced the emission strength and changed the emission pattern. Enhanced emissions lead to linearly enhanced SOA formation with a fractional mass yield of SOA (5.7±1%) independent of the detailed emission pattern. The particles are highly scattering with no absorption abilities. Their average hygroscopic growth factor was 1.13±0.03 at 90% RH with a critical diameter of droplet activation was 100±4 nm at a supersaturation of 0.4%. All microphysical properties were not dependent on the detailed emission pattern, in accordance with an invariant O/C ratio (0.57(+0.03/-0.1)) of the SOA as derived from high resolution aerosol mass spectrometry. The temperature increase for the plants essentially led to stronger VOC emissions with the SOA mass being linearly related to the VOC concentrations. However, the increase of Holm oak emissions with temperature (≈ 20 % per degree) was stronger than for Boreal tree species

  17. Improving satellite retrieved aerosol microphysical properties using GOCART data

    NASA Astrophysics Data System (ADS)

    Li, S.; Kahn, R.; Chin, M.; Garay, M. J.; Chen, L.; Liu, Y.

    2014-09-01

    The Multi-Angle Imaging Spectro-Radiometer (MISR) instrument on NASA's Terra satellite can provide more reliable Aerosol Optical Depth (AOD, τ) and more particle information, such as constraints on particle size (Angström exponent or ANG, α), particle shape, and single-scattering albedo (SSA, ω), than many other satellite instruments. However, MISR's ability to retrieve aerosol properties is weakened at low AOD levels. When aerosol-type information content is low, many candidate aerosol mixtures can match the observed radiances. We propose an algorithm to improve MISR aerosol retrievals by constraining MISR mixtures' ANG and absorbing AOD (AAOD) with Goddard Chemistry Aerosol Radiation and Transport (GOCART) model-simulated aerosol properties. To demonstrate this approach, we calculated MISR aerosol optical properties over the contiguous US from 2006 to 2009. Sensitivities associated with the thresholds of MISR-GOCART differences were analyzed according to the agreement between our results (AOD, ANG, and AAOD) and AErosol RObotic NETwork (AERONET) observations. Overall, our AOD has a good agreement with AERONET because the MISR AOD retrieval is not sensitive to different mixtures under many retrieval conditions. The correlation coefficient (r) between our ANG and AERONET improves to 0.45 from 0.29 for the MISR Version 22 standard product and 0.43 for GOCART when all data points are included. However, when only cases having AOD > 0.2, the MISR product itself has r ~ 0.40, and when only AOD > 0.2 and the best-fitting mixture are considered, r ~ 0.49. So as expected, the ANG improvement occurs primarily when the model constraint is applied in cases where the particle type information content of the MISR radiances is low. Regression analysis for AAOD shows that MISR Version 22 and GOCART misestimate AERONET by a ratio (mean retrieved AAOD to mean AERONET AAOD) of 0.5; our method improves this ratio to 0.74. Large discrepancies are found through an inter

  18. The thermal infrared radiance properties of dust aerosol over ocean

    NASA Astrophysics Data System (ADS)

    Hao, Zengzhou; Pan, Delu; Tu, Qianguang; Gong, Fang; Chen, Jianyu

    2015-10-01

    Asian dust storms, which can long-range transport to ocean, often occur on spring. The present of Asian dust aerosols over ocean makes some difficult for other studies, such as cloud detection, and also take some advantage for ocean, such as take nutrition into the ocean by dry or wet deposition. Therefore, it is important to study the dust aerosol and retrieve the properties of dust from satellite observations that is mainly from the thermal infrared radiance. In this paper, the thermal infrared radiance properties of dust aerosol over ocean are analyzed from MODIS and MTSAT2 observations and Streamer model simulations. By analyzing some line samples and a series of dust aerosol region, it shows that the dust aerosol brightness temperature at 12μm (BT12) is always greater than BT11 and BT8.5, and BT8.5 is general greater than BT11. The brightness temperature different between 11μm and 12μm (BTD11-12) increases with the dust intensity. And the BTD11-12 will become positive when the atmospheric relative humidity is greater than 70%. The BTD11-12 increases gradually with the surface temperature while the effect on BTD11-12 of dust layer temperature is not evident. Those are caused by the transmission of the dust aerosol is different at the two thermal infrared channels. During daytime, dust infrared brightness temperature at mid-infrared bands should reduce the visual radiance, which takes about 25K or less. In general, BT3.7 is greater than BT11 for dust aerosol. Those results are helpful to monitor or retrieve dust aerosol physical properties over ocean from satellite.

  19. THERMAL PROPERTIES OF SECONDARY ORGANIC AEROSOLS

    EPA Science Inventory

    Volume concentrations of steady-state secondary organic aerosol (SOA) were measured in several hydrocarbon/NOx irradiation experiments. These measurements were used to estimate the thermal behavior of the particles that may be formed in the atmosphere. These laborator...

  20. Droplet activation properties of organic aerosols observed at an urban site during CalNex-LA

    SciTech Connect

    Mei, Fan; Hayes, Patrick L.; Ortega, Amber; Taylor, Jonathan W.; Allan, James D.; Gilman, Jessica; Kuster, William; de Gouw, Joost; Jimenez, Jose L.; Wang, Jian

    2013-04-11

    Size-resolved cloud condensation nuclei (CCN) spectra and aerosol chemical composition were characterized at an urban supersite in Pasadena, California, from 15 May to 4 June 2010, during the CalNex campaign. The derived hygroscopicityCCN) of CCN-active particles with diameter between 97 and 165 nm ranged from 0.05 to 0.4. Diurnal variation showed a slight decrease of κCCN from 8:00 to 16:00 (from 0.24 to 0.20), which is attributed to increasing organics volume fraction resulted from secondary organic aerosol (SOA) formation. The derived hygroscopicity distribution and maximum activated fraction of the size selected particles were examined as functions of photochemical age. The result indicates that condensation of secondary species (e.g., SOA and sulfate) quickly converted hydrophobic particles to hydrophilic ones, and during daytime, nearly every particle became a CCN at ~0.4% in just a few hours. Based on κCCN and aerosol chemical composition, the organic hygroscopicityorg) was derived, and ranged from 0.05 to 0.23 with an average value of 0.13, consistent with the results from earlier studies. The derived κorg generally increased with the organic oxidation level, and most of the variation in κorg could be explained by the variation of the organic O : C atomic ratio alone. The least squares fit of the data yielded κorg = (0.83 ± 0.06) × (O:C) + (-0.19 ± 0.02). Compared to previous results based on CCN measurements of laboratory generated aerosols, κorg derived from measurements during the CalNex campaign exhibited stronger increase with O : C atomic ratio and therefore substantially higher values for organics with average O : C greater than 0.5.

  1. Simultaneous Measurement of Size, Composition, Hygroscopicity, and Density of Single Ambient Particles

    NASA Astrophysics Data System (ADS)

    Zelenyuk, A.; Imre, D. G.; Han, J.; Oatis, S.

    2003-12-01

    The holly grail in aerosol climate interaction is a roadmap that takes one from emissions of aerosol and aerosol precursors through aerosol transformations, to optical and cloud effects and finally to climate impacts. A critical element on this path must be the behavior of aerosol as a function of atmospheric relative humidity, which in turn requires an understanding of the correlation between aerosol composition and hygroscopicity. For single component particles this problem is tractable and reasonably understood. But, the vast majority of particles in the real atmosphere are internal mixtures of hygroscopic salts, organic acids and or bases, long chain hydrocarbons, soot, mineral dust and the list go on. Hundreds of organic compounds with highly varying hygroscopicities can be found in single particles. It would be unrealistic to expect global climate models to include and track each of these compounds. A similar problem faces the experimental world, where measuring the size, detailed molecular composition and hygroscopicity of individual particles although, in principle possible, is impractical. Single particle mass spectroscopy can be used to classify particles as organics mixed with sulfate, for example. Or in some cases pinpoint the class of some of the organics found in the mixture. But it cannot yield a quantitative measure of relative amounts. In an attempt to address this issue we have developed the method to measure simultaneously hygroscopicity, size, and composition of individual ambient particles. However, the data from Long Island NY, where the vast majority of particles were internally mixed sulfate with organics, the correlation between composition and hygroscopicity was rather weak. This is due to the fact that single-laser single particle mass spectra cannot quantitatively measure the ratio of organics to sulfates. In contrast, we found a very clear correlation between hygroscopicity and particle density for a given class of particles. In this

  2. Measuring Aerosol Optical Properties with the Ozone Monitoring Instrument (OMI)

    NASA Technical Reports Server (NTRS)

    Veefkind, J. P.; Torres, O.; Syniuk, A.; Decae, R.; deLeeuw, G.

    2003-01-01

    The Ozone Monitoring Instrument (OMI) is the Dutch-Finnish contribution to the NASA EOS-Aura mission scheduled for launch in January 2004. OM1 is an imaging spectrometer that will measure the back-scattered Solar radiance between 270 an 500 nm. With its relatively high spatial resolution (13x24 sq km at nadir) and daily global coverage. OM1 will make a major contribution to our understanding of atmospheric chemistry and to climate research. OM1 will provide data continuity with the TOMS instruments. One of the pleasant surprises of the TOMS data record was its information on aerosol properties. First, only the absorbing aerosol index, which is sensitive to elevated lay- ers of aerosols such as desert dust and smoke aerosols, was derived. Recently these methods were further improved to yield aerosol optical thickness and single scattering albedo over land and ocean for 19 years of TOMS data (1979-1992,1997-2002), making it one of the longest and most valuable time series for aerosols presently available. Such long time series are essential to quantify the effect of aerosols on the Earth& climate. The OM1 instrument is better suited to measure aerosols than the TOMS instruments because of the smaller footprint, and better spectral coverage. The better capabilities of OMI will enable us to provide an improved aerosol product, but the knowledge will also be used for further analysis of the aerosol record from TOMS. The OM1 aerosol product that is currently being developed for OM1 combines the TOMS experience and the multi-spectral techniques that are used in the visible and near infrared. The challenge for this new product is to provide aerosol optical thickness and single scattering albedo from the near ultraviolet to the visible (330-500 nm) over land and ocean. In this presentation the methods for deriving the OM1 aerosol product will be presented. Part of these methods developed for OM1 can already be applied to TOMS data and results of such analysis will be shown.

  3. Global Aerosol Radiative Forcing Derived from Sea WiFS-Inferred Aerosol Optical Properties

    NASA Technical Reports Server (NTRS)

    Chou, Ming-Dah; Chan, Pui-King; Wang, Menghua

    1999-01-01

    Aerosol optical properties inferred from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) radiance measurements are used to compute the aerosol shortwave radiative forcing using a radiative transfer model. The aerosol optical thickness at the wavelength of 865-nm is taken from the SeaWIFS archive. It is found that the nominal optical thickness over oceans ranges from 0.1 to 0.2. Using a maritime aerosol model and the radiances measured at the various SeaWiFS channels, the Angstrom exponent is determined to be 0.2174, the single-scattering albedo to be 0.995, and the asymmetry factor to be 0.786. The radiative transfer model has eight bands in the visible and ultraviolet spectral regions and three bands in the near infrared. It includes the absorption due to aerosols, water vapor, carbon dioxide, and oxygen, and the scattering due to aerosols and gases (Rayleigh scattering). The radiative forcing is computed over global oceans for four months (January, April, July, and October, 1998) to represent four seasons. It is found that the aerosol radiative forcing is large and changes significantly with seasons near the continents with large-scale forest fires and desert dust. Averaged over oceans and the four months, the aerosol radiative forcing is approximately 7 W/sq m at the top of the atmosphere. This large radiative forcing is expected to have a significant cooling effect on the Earth's climate as implied from simulations of a number of general circulation models.

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

    NASA Technical Reports Server (NTRS)

    Pueschel, Rudolf F. (Editor)

    1991-01-01

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

  5. Aerosol Radiative Forcing Derived From SeaWIFS - Retrieved Aerosol Optical Properties

    NASA Technical Reports Server (NTRS)

    Chou, Mong-Dah; Chan, Pui-King; Wang, Menghua; Einaudi, Franco (Technical Monitor)

    2000-01-01

    To understand climatic implications of aerosols over global oceans, the aerosol optical properties retrieved from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) are analyzed, and the effects of the aerosols on the Earth's radiation budgets (aerosol radiative forcing, ARF) are computed using a radiative transfer model. It is found that the distribution of the SeaWiFS-retrieved aerosol optical thickness is distinctively zonal. The maximum in the equatorial region coincides with the Intertropical Convergence Zone, and the maximum in the Southern Hemispheric high latitudes coincides with the region of prevailing westerlies. The minimum aerosol optical thickness is found in the subtropical high pressure regions, especially in the Southern Hemisphere. These zonal patterns clearly demonstrate the influence of atmospheric circulation on the oceanic aerosol distribution. Over global oceans, aerosols reduce the annual mean net downward solar flux by 5.4 W m-2 at the top of the atmosphere and by 6.1 W m-2 at the surface. The largest ARF is found in the tropical Atlantic, Arabian Sea, Bay of Bengal, the coastal regions of Southeast and East Asia, and the Southern Hemispheric high latitudes. During the period of the Indonesian big fires (September-December 1997), the cooling due to aerosols is greater than 15 W m-2 at the top of the atmosphere and greater than 30 W m(exp -1) at the surface in the vicinity of the maritime continents. The atmosphere receives extra solar radiation by greater than 15 W m(exp -1) over a large area. These large changes in radiative fluxes are expected to have enhanced the atmospheric stability, weakened the atmospheric circulation, and augmented the drought condition during that period. It would be very instructive to simulate the regional climatic. The model-calculated clear sky solar flux at the top of the atmosphere is compared with that derived from the Clouds and the Earth's Radiant Energy System (CERES). The net downward solar flux of

  6. Aerosol Properties and Radiative Forcing over Kanpur during Severe Aerosol Loading Conditions

    SciTech Connect

    Kaskaoutis, D. G.; Sinha, P. R.; Vinoj, V.; Kosmopoulos, P. G.; Tripathi, S. N.; Misra, Amit; Sharma, M.; Singh, R. P.

    2013-11-01

    Atmospheric aerosols over India exhibit large spatio-temporal fluctuation driven by the local monsoon system, emission rates and seasonally-changed air masses. The northern part of India is well-known for its high aerosol loading throughout the year due to anthropogenic emissions, dust influence and biomass burning. On certain circumstances and, under favorable weather conditions, the aerosol load can be severe, causing significant health concerns and climate implications. The present work analyzes the aerosol episode (AE) days and examines the modification in aerosol properties and radiative forcing during the period 2001-2010 based on Kanpur-AERONET sun photometer data. As AEs are considered the days having daily-mean aerosol optical depth (AOD) above the decadal mean + 1 STD (standard deviation); the threshold value is defined at 0.928. The results identify 277 out of 2095 days (13.2%) of AEs over Kanpur, which are most frequently observed during post-monsoon (78 cases, 18.6%) and monsoon (76, 14.7%) seasons due to biomass-burning episodes and dust influence, respectively. On the other hand, the AEs in winter and pre-monsoon are lower in both absolute and percentage values (65, 12.5% and 58, 9.1%, respectively). The modification in aerosol properties on the AE days is strongly related to season. Thus, in post-monsoon and winter the AEs are associated with enhanced presence of fine-mode aerosols and Black Carbon from anthropogenic pollution and any kind of burning, while in pre-monsoon and monsoon seasons they are mostly associated with transported dust. Aerosol radiative forcing (ARF) calculated using SBDART shows much more surface (~-69 to -97 Wm-2) and Top of Atmosphere cooling (-20 to -30 Wm-2) as well as atmospheric heating (~43 to 71 Wm-2) during the AE days compared to seasonal means. These forcing values are mainly controlled by the higher AODs and the modified aerosol characteristics (Angstrom α, SSA) during the AE days in each season and may cause

  7. Global dust infrared aerosol properties retrieved using hyperspectral sounders

    NASA Astrophysics Data System (ADS)

    Capelle, Virginie; Chédin, alain; Pondrom, Marc; Pierangelo, Clémence; Armante, Raymond; Crevoisier, Cyril; Crépeau, Laurent; Scott, Noëlle

    2015-04-01

    Observations from infrared hyperspectral sounders, here IASI and AIRS, are interpreted in terms of dust aerosol properties (AOD and mean altitude). The method is based on a "Look-Up-Table" (LUT) approach, where all radiative transfer computation is performed once for all and "off-line", for a large selection of atmospheric situations, of observing conditions, of surface characteristics (in particular the surface emissivity and temperature), and different aerosol refractive index models. The inversion scheme follows two main steps: first, determination of the observed atmospheric thermodynamic situation, second, simultaneous retrieval of the 10µm coarse-mode AOD and of the mean altitude. The method is here applied over sea and over land, at daily scale daytime and nighttime, and at the satellite pixel resolution (12 km at nadir). The geographical study area studied includes the northern tropics from west Atlantic to the Arabian peninsula and Indian ocean, and the Mediterranean basin, all of them characterized by strong, regular dust events. A special focus is given to the hourly variation of aerosol properties within a day. In this context, both IASI overpasses are processed, providing two measurements at 9:30AM and 9:30PM (equator local time) each day. First results obtained from AIRS observations, made at 1:30 AM and PM, open the way to the analysis of the aerosol diurnal cycle. For the AOD, comparisons are made with AERONET ground-based data , when available, in order to 1) evaluate our results, and 2) show the importance of a better knowledge of the aerosol diurnal cycle, especially close to the sources. Mean aerosol layer altitude obtained from IASI is compared at local scale with the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP/CALIPSO) aerosol altitude.

  8. Optical Properties of Polymers Relevant to Secondary Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Marrero-Ortiz, W.; Gomez-Hernandez, M. E.; Xu, W.; Guo, S.; Zhang, R.

    2014-12-01

    Atmospheric aerosols play a critical role in climate directly by scattering and absorbing solar radiation and indirectly by modifying the cloud formation. Currently, the direct and indirect effects of aerosols represent the largest uncertainty in climate predictions models. Some aerosols are directly emitted, but the majority are formed in the atmosphere by the oxidation of gaseous precursors. However, the formation of aerosols at the molecular level is not fully characterized. Certain category of secondary organic aerosols (SOA), which represent a significant fraction of the total aerosol burden, can be light-absorbing, also known as brown carbon. However, the overall contribution of SOA to the brown carbon and the related climate forcing is poorly understood. Such incomplete understanding is due in part to the chemical complexity of SOA and the lack of knowledge regarding SOA formation, transformation, and optical properties. Based on previous laboratory experiments, field measurements, and modeling studies, it has been suggested that the polymers and oligomers play an important role in the SOA formation. Atmospheric polymers could be produced by the hydration or heterogeneous reactions of epoxides and small α-dicarbonyls. Their aqueous chemistry products have been shown to give light-absorbing and high molecular weight oligomeric species, which increase the SOA mass production and alter the direct and indirect effect of aerosols. In this paper, the aerosol chemistry of small α-dicarbonyl compounds with amines is investigated and the associated optical properties are measured using spectroscopic techniques. The differences between primary, secondary and tertiary amines with glyoxal and methylglyoxal are evaluated in terms of SOA browning efficiency. Atmospheric implications of our present work for understanding the formation of light-absorbing SOA will be presented, particularly in terms of the product distribution of light-absorbing SOA formed by aqueous phase

  9. CCN activation of ambient and "synthetic ambient" urban aerosol

    NASA Astrophysics Data System (ADS)

    Burkart, Julia; Reischl, Georg; Steiner, Gerhard; Bauer, Heidi; Leder, Klaus; Kistler, Magda; Puxbaum, Hans; Hitzenberger, R.

    2013-05-01

    In this study, the Cloud Condensation Nuclei (CCN) activation properties of the urban aerosol in Vienna, Austria, were investigated in a long term (11 month) field study. Filter samples of the aerosol below 100 nm were taken in parallel to these measurements, and later used to generate "synthetic ambient" aerosols. Activation parameters of this "synthetic ambient" aerosol were also obtained. Hygroscopicity parameters κ [1] were calculated both for the urban and the "synthetic ambient" aerosol and also from the chemical composition. Average κ for the "synthetic ambient" aerosol ranged from 0.20 to 0.30 with an average value of 0.24, while the κ from the chemical composition of this "synthetic ambient" aerosol was significantly higher (average 0.43). The full results of the study are given elsewhere [2,3].

  10. Water uptake of multicomponent organic mixtures and their influence on hygroscopicity of inorganic salts.

    PubMed

    Wang, Yuanyuan; Jing, Bo; Guo, Yucong; Li, Junling; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

    2016-07-01

    The hygroscopic behaviors of atmospherically relevant multicomponent water soluble organic compounds (WSOCs) and their effects on ammonium sulfate (AS) and sodium chloride were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA) in the relative humidity (RH) range of 5%-90%. The measured hygroscopic growth was compared with predictions from the Extended-Aerosol Inorganics Model (E-AIM) and Zdanovskii-Stokes-Robinson (ZSR) method. The equal mass multicomponent WSOCs mixture containing levoglucosan, succinic acid, phthalic acid and humic acid showed gradual water uptake without obvious phase change over the whole RH range. It was found that the organic content played an important role in the water uptake of mixed particles. When organic content was dominant in the mixture (75%), the measured hygroscopic growth was higher than predictions from the E-AIM or ZSR relation, especially under high RH conditions. For mass fractions of organics not larger than 50%, the hygroscopic growth of mixtures was in good agreement with model predictions. The influence of interactions between inorganic and organic components on the hygroscopicity of mixed particles was related to the salt type and organic content. These results could contribute to understanding of the hygroscopic behaviors of multicomponent aerosol particles. PMID:27372129

  11. Aerosol measurements at a high-elevation site: composition, size, and cloud condensation nuclei activity

    SciTech Connect

    Friedman, Beth; Zelenyuk, Alla; Beranek, Josef; Kulkarni, Gourihar R.; Pekour, Mikhail S.; Hallar, Anna G.; McCubbin, Ian; Thornton, Joel A.; Cziczo, D. J.

    2013-12-09

    We present measurements of CCN concentrations and associated aerosol composition and size properties at a high-elevation research site in March 2011. CCN closure and aerosol hygroscopicity were assessed using simplified assumptions of bulk aerosol properties as well as a new method utilizing single particle composition and size to assess the importance of particle mixing state in CCN activation. Free troposphere analysis found no significant difference between the CCN activity of free tropospheric aerosol and boundary layer aerosol at this location. Closure results indicate that using only size and number information leads to adequate prediction, in the majority of cases within 50%, of CCN concentrations, while incorporating the hygroscopicity parameters of the individual aerosol components measured by single particle mass spectrometry adds to the agreement, in most cases within 20%, between predicted and measured CCN concentrations. For high-elevation continental sites, with largely aged aerosol and low amounts of local area emissions, a lack of chemical knowledge and hygroscopicity may not hinder models in predicting CCN concentrations. At sites influenced by fresh emissions or more heterogeneous particle types, single particle composition information may be more useful in predicting CCN concentrations and understanding the importance of particle mixing state on CCN activation.

  12. Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US

    NASA Astrophysics Data System (ADS)

    Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.; Taylor, Nathan F.; Miettinen, Pasi; Palm, Brett B.; Mikkonen, Santtu; Collins, Don R.; Jimenez, Jose L.; Virtanen, Annele

    2016-09-01

    During the summer 2013 Southern Aerosol and Oxidant Study (SOAS) field campaign in a rural site in the southeastern United States, the effect of hygroscopicity and composition on the phase state of atmospheric aerosol particles dominated by the organic fraction was studied. The analysis is based on hygroscopicity measurements by a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA), physical phase state investigations by an Aerosol Bounce Instrument (ABI) and composition measurements using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). To study the effect of atmospheric aging on these properties, an OH-radical oxidation flow reactor (OFR) was used to simulate longer atmospheric aging times of up to 3 weeks. Hygroscopicity and bounce behavior of the particles had a clear relationship showing higher bounce at elevated relative humidity (RH) values for less hygroscopic particles, which agrees well with earlier laboratory studies. Additional OH oxidation of the aerosol particles in the OFR increased the O : C and the hygroscopicity resulting in liquefying of the particles at lower RH values. At the highest OH exposures, the inorganic fraction starts to dominate the bounce process due to production of inorganics and concurrent loss of organics in the OFR. Our results indicate that at typical ambient RH and temperature, organic-dominated particles stay mostly liquid in the atmospheric conditions in the southeastern US, but they often turn semisolid when dried below ˜ 50 % RH in the sampling inlets. While the liquid phase state suggests solution behavior and equilibrium partitioning for the SOA particles in ambient air, the possible phase change in the drying process highlights the importance of thoroughly considered sampling techniques of SOA particles.

  13. Optical Properties of Atmospheric Aerosol in Maritime Environments.

    NASA Astrophysics Data System (ADS)

    Smirnov, Alexander; Holben, Brent N.; Kaufman, Yoram J.; Dubovik, Oleg; Eck, Thomas F.; Slutsker, Ilya; Pietras, Christophe; Halthore, Rangasayi N.

    2002-02-01

    Systematic characterization of aerosol over the oceans is needed to understand the aerosol effect on climate and on transport of pollutants between continents. Reported are the results of a comprehensive optical and physical characterization of ambient aerosol in five key island locations of the Aerosol Robotic Network (AERONET) of sun and sky radiometers, spanning over 2-5 yr. The results are compared with aerosol optical depths and size distributions reported in the literature over the last 30 yr. Aerosol found over the tropical Pacific Ocean (at three sites between 20°S and 20°N) still resembles mostly clean background conditions dominated by maritime aerosol. The optical thickness is remarkably stable with mean value of a(500 nm) = 0.07, mode value at am = 0.06, and standard deviation of 0.02-0.05. The average Ångström exponent range, from 0.3 to 0.7, characterizes the wavelength dependence of the optical thickness. Over the tropical to subtropical Atlantic (two stations at 7°S and 32°N) the optical thickness is significantly higher: a(500 nm) = 0.14 and am = 0.10 due to the frequent presence of dust, smoke, and urban-industrial aerosol. For both oceans the atmospheric column aerosol is characterized by a bimodal lognormal size distribution with a fine mode at effective radius Reff = 0.11 ± 0.01 m and coarse mode at Reff = 2.1 ± 0.3 m. A review of the published 150 historical ship measurements from the last three decades shows that am was around 0.07 to 0.12 in general agreement with the present finding. The information should be useful as a test bed for aerosol global models and aerosol representation in global climate models. With global human population expansion and industrialization, these measurements can serve in the twenty-first century as a basis to assess decadal changes in the aerosol concentration, properties, and radiative forcing of climate.

  14. Measuring Mass-Based Hygroscopicity of Atmospheric Particles through in Situ Imaging.

    PubMed

    Piens, Dominique S; Kelly, Stephen T; Harder, Tristan H; Petters, Markus D; O'Brien, Rachel E; Wang, Bingbing; Teske, Ken; Dowell, Pat; Laskin, Alexander; Gilles, Mary K

    2016-05-17

    Quantifying how atmospheric particles interact with water vapor is critical for understanding the effects of aerosols on climate. We present a novel method to measure the mass-based hygroscopicity of particles while characterizing their elemental and carbon functional group compositions. Since mass-based hygroscopicity is insensitive to particle geometry, it is advantageous for probing the hygroscopic behavior of atmospheric particles, which can have irregular morphologies. Combining scanning electron microscopy with energy dispersive X-ray analysis (SEM/EDX), scanning transmission X-ray microscopy (STXM) analysis, and in situ STXM humidification experiments, this method was validated using laboratory-generated, atmospherically relevant particles. Then, the hygroscopicity and elemental composition of 15 complex atmospheric particles were analyzed by leveraging quantification of C, N, and O from STXM, and complementary elemental quantification from SEM/EDX. We found three types of hygroscopic responses, and correlated high hygroscopicity with Na and Cl content. The mixing state of 158 other particles from the sample broadly agreed with those of the humidified particles, indicating the potential to infer atmospheric hygroscopic behavior from a selected subset of particles. These methods offer unique quantitative capabilities to characterize and correlate the hygroscopicity and chemistry of individual submicrometer atmospheric particles.

  15. Measuring mass-based hygroscopicity of atmospheric particles through in situ imaging

    DOE PAGES

    Piens, Dominique S.; Kelly, Stephen T.; Harder, Tristan H.; Petters, Markus D.; O’Brien, Rachel E.; Wang, Bingbing; Teske, Ken; Dowell, Pat; Laskin, Alexander; Gilles, Mary K.

    2016-04-18

    Quantifying how atmospheric particles interact with water vapor is critical for understanding the effects of aerosols on climate. We present a novel method to measure the mass-based hygroscopicity of particles while characterizing their elemental and carbon functional group compositions. Since mass-based hygroscopicity is insensitive to particle geometry, it is advantageous for probing the hygroscopic behavior of atmospheric particles, which can have irregular morphologies. Combining scanning electron microscopy with energy dispersive X-ray analysis (SEM/EDX), scanning transmission X-ray microscopy (STXM) analysis, and in situ STXM humidification experiments, this method was validated using laboratory-generated, atmospherically relevant particles. Then, the hygroscopicity and elemental compositionmore » of 15 complex atmospheric particles were analyzed by leveraging quantification of C, N, and O from STXM, and complementary elemental quantification from SEM/EDX. We found three types of hygroscopic responses, and correlated high hygroscopicity with Na and Cl content. The mixing state of 158 other particles from the sample broadly agreed with those of the humidified particles, indicating the potential to infer atmospheric hygroscopic behavior from a selected subset of particles. As a result, these methods offer unique quantitative capabilities to characterize and correlate the hygroscopicity and chemistry of individual submicrometer atmospheric particles.« less

  16. Measuring Mass-Based Hygroscopicity of Atmospheric Particles through in Situ Imaging.

    PubMed

    Piens, Dominique S; Kelly, Stephen T; Harder, Tristan H; Petters, Markus D; O'Brien, Rachel E; Wang, Bingbing; Teske, Ken; Dowell, Pat; Laskin, Alexander; Gilles, Mary K

    2016-05-17

    Quantifying how atmospheric particles interact with water vapor is critical for understanding the effects of aerosols on climate. We present a novel method to measure the mass-based hygroscopicity of particles while characterizing their elemental and carbon functional group compositions. Since mass-based hygroscopicity is insensitive to particle geometry, it is advantageous for probing the hygroscopic behavior of atmospheric particles, which can have irregular morphologies. Combining scanning electron microscopy with energy dispersive X-ray analysis (SEM/EDX), scanning transmission X-ray microscopy (STXM) analysis, and in situ STXM humidification experiments, this method was validated using laboratory-generated, atmospherically relevant particles. Then, the hygroscopicity and elemental composition of 15 complex atmospheric particles were analyzed by leveraging quantification of C, N, and O from STXM, and complementary elemental quantification from SEM/EDX. We found three types of hygroscopic responses, and correlated high hygroscopicity with Na and Cl content. The mixing state of 158 other particles from the sample broadly agreed with those of the humidified particles, indicating the potential to infer atmospheric hygroscopic behavior from a selected subset of particles. These methods offer unique quantitative capabilities to characterize and correlate the hygroscopicity and chemistry of individual submicrometer atmospheric particles. PMID:27088454

  17. Retrieval of aerosol optical properties over land using PMAp

    NASA Astrophysics Data System (ADS)

    Grzegorski, Michael; Munro, Rosemary; Lang, Ruediger; Poli, Gabriele; Holdak, Andriy

    2015-04-01

    The retrieval of aerosol optical properties is an important task for industry and climate forecasting. An ideal instrument should include observations with moderate spectral and high spatial resolutions for a wide range of wavelengths (from the UV to the TIR), measurements of the polarization state at different wavelengths and measurements of the same scene for different observation geometries. As such an ideal instrument is currently unavailable the usage of different instruments on one satellite platform is an alternative choice. Since February 2014, the Polar Multi sensor Aerosol product (PMAp) is delivered as operational GOME product to our customers. The algorithms retrieve aerosol optical properties over ocean (AOD, volcanic ash, aerosol type) using a multi-sensor approach (GOME, AVHRR, IASI). The next releases of PMAp will provide an extended set of aerosol and cloud properties which include AOD over land and an improved volcanic ash retrieval combining AVHRR and IASI. This presentation gives an overview on the existing product and the prototypes in development. The major focus is the discussion of the AOD retrieval over land implemented in the upcoming PMAp2 release. In addition, the results of our current validation studies (e.g. comparisons to AERONET, other satellite platforms and model data) are shown.

  18. Observations of relative humidity effects on aerosol light scattering in the Yangtze River Delta of China

    NASA Astrophysics Data System (ADS)

    Zhang, L.; Sun, J. Y.; Shen, X. J.; Zhang, Y. M.; Che, H.; Ma, Q. L.; Zhang, Y. W.; Zhang, X. Y.; Ogren, J. A.

    2015-07-01

    Scattering of solar radiation by aerosol particles is highly dependent on relative humidity (RH) as hygroscopic particles take up water with increasing RH. To achieve a better understanding of the effect of aerosol hygroscopic growth on light scattering properties and radiative forcing, the aerosol scattering coefficients at RH in the range of 40 to ~ 90 % were measured using a humidified nephelometer system in the Yangtze River Delta of China in March 2013. In addition, the aerosol size distribution and chemical composition were measured. During the observation period, the mean and standard deviation (SD) of enhancement factors at RH = 85 % for the scattering coefficient (f(85 %)), backscattering coefficient (fb(85 %)), and hemispheric backscatter fraction (fβ(85 %)) were 1.58 ± 0.12, 1.25 ± 0.07, and 0.79 ± 0.04, respectively, i.e., aerosol scattering coefficient and backscattering coefficient increased by 58 and 25 % as the RH increased from 40 to 85 %. Concurrently, the aerosol hemispheric backscatter fraction decreased by 21 %. The relative amount of organic matter (OM) or inorganics in PM1 was found to be a main factor determining the magnitude of f(RH). The highest values of f(RH) corresponded to the aerosols with a small fraction of OM, and vice versa. The relative amount of NO3- in fine particles was strongly correlated with f(85 %), which suggests that NO3- played a vital role in aerosol hygroscopic growth during this study. The mass fraction of nitrate also had a close relationship to the curvature of the humidograms; higher mass fractions of nitrate were associated with humidograms that had the least curvature. Aerosol hygroscopic growth caused a 47 % increase in the calculated aerosol direct radiative forcing at 85 % RH, compared to the forcing at 40 % RH.

  19. Effect of CALIPSO Cloud Aerosol Discrimination (CAD) Confidence Levels on Observations of Aerosol Properties near Clouds

    NASA Technical Reports Server (NTRS)

    Yang, Weidong; Marshak, Alexander; Varnai, Tamas; Liu, Zhaoyan

    2012-01-01

    CALIPSO aerosol backscatter enhancement in the transition zone between clouds and clear sky areas is revisited with particular attention to effects of data selection based on the confidence level of cloud-aerosol discrimination (CAD). The results show that backscatter behavior in the transition zone strongly depends on the CAD confidence level. Higher confidence level data has a flatter backscatter far away from clouds and a much sharper increase near clouds (within 4 km), thus a smaller transition zone. For high confidence level data it is shown that the overall backscatter enhancement is more pronounced for small clear-air segments and horizontally larger clouds. The results suggest that data selection based on CAD reduces the possible effects of cloud contamination when studying aerosol properties in the vicinity of clouds.

  20. Synthesis of information on aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Liu, Hongqing; Pinker, R. T.; Chin, M.; Holben, B.; Remer, L.

    2008-04-01

    In a previous study (Liu et al., 2005) obtained are global scale estimates of aerosol optical depth at 0.55 μm based on spatial and temporal variation patterns from models and satellite observations, regulated by the Aerosol Robotic Network (AERONET) measurements. In this study an approach is developed to obtain information on global distribution of the single scattering albedo (ω0), the asymmetry parameter (g), and the normalized extinction coefficient over shortwave (SW) spectrum. Since space observations of ω0 are in early stages of development and none are available for g, first an approach was developed to infer them from relevant information from the Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model, Moderate Resolution Imaging Spectroradiometer (MODIS) and AERONET retrievals. The single scattering albedo is generated by extending GOCART ω0 at 0.55 μm to the entire SW spectrum using spectral dependence derived from AERONET retrievals. The asymmetry parameter over the solar spectrum is derived from the MODIS Ångström wavelength exponent, utilizing a relationship based on AERONET almucantar observations. The normalized extinction coefficient is estimated from the MODIS Ångström wavelength exponent. The methodology was implemented as a "proof of concept" with one year of data. The approach described here is a step in preparedness for utilizing information from new observing systems (e.g., MISR, A-Train constellation) when available. The impact of the newly derived information on the quality of satellite based estimates of surface radiative fluxes was evaluated and is presented by Liu and Pinker (2008).

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

    NASA Astrophysics Data System (ADS)

    Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

    2016-01-01

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

  2. Cloud activation properties of organic aerosols observed at an urban site during CalNex-LA

    NASA Astrophysics Data System (ADS)

    Mei, F.; Hayes, P. L.; Ortega, A. M.; Jimenez, J.; Wang, J.

    2010-12-01

    hygroscopicity (κ, Petters and Kreidenweis, 2007, ACP) derived from the size-resolved CCN measurements ranges from 0.2 to 0.3 under the range of measured supersaturations. The derived particle κ increases with increasing particle diameter, which is consistent with observed decrease in organics volume fraction as particle size increases from 100 nm to 300 nm. Based on the particle hygroscopicity and aerosol chemical composition, the organics hygroscopicity (κOrg) was derived as 0.18±0.06, in agreement with κ of organics with the same O:C ratio reported in earlier studies (Chang et al. 2010 ACP; Duplissy et.al 2010 ACPD). Whereas organics strongly influence particle critical supersaturation, size-classified organic particles exhibit similar growth kinetics when compared to (NH4)2SO4 particles with the same critical supersaturation, suggesting aerosol organics observed during CalNex do not inhibit droplet growth through reducing the mass accommodation coefficient of water vapor.

  3. Properties of Stratospheric Aerosol Estimated from HALOE Data

    NASA Technical Reports Server (NTRS)

    Lee, Kwang-Mog; Park, Jae H.; Massie, Steven T.; Choi, Wookap

    2001-01-01

    Extinction coefficients for stratospheric aerosols at 8 HALOE (HALogen Occultation Experiment) wavelengths are determined by comparing transmittances data for two adjacent solar occultation measurements, where one limb path is loaded with aerosols but the other path is free of aerosols. These extinction coefficients are used to infer the aerosol properties such as composition and size distribution parameters. Mie theory has been used to calculate the extinction coefficients, and a nonlinear least square method is applied to determine the aerosol properties. Sixteen cases are selected for the retrieval in southern hemisphere at latitudes from 21 to 48 deg S for the period of 29 Mar - 31 May 1992. Retrieved size width ranges from 1.1 to 1.5 and radius ranges from 0.25 to 0.45 micrometers. These size parameters are within the ranges of in situ measurements at Laramie, Wyoming. Retrieved weight percent of H2SO4 is larger than the equilibrium value by about 5 to approximately 10 weight percent, similar to the results for northern hemisphere at latitudes 20 to 55 deg N for the period from Nov 1991 to Feb. 1992.

  4. Composition and physical properties of the Asian Tropopause Aerosol Layer and the North American Tropospheric Aerosol Layer

    PubMed Central

    Yu, Pengfei; Toon, Owen B; Neely, Ryan R; Martinsson, Bengt G; Brenninkmeijer, Carl A M

    2015-01-01

    Recent studies revealed layers of enhanced aerosol scattering in the upper troposphere and lower stratosphere over Asia (Asian Tropopause Aerosol Layer (ATAL)) and North America (North American Tropospheric Aerosol Layer (NATAL)). We use a sectional aerosol model (Community Aerosol and Radiation Model for Atmospheres (CARMA)) coupled with the Community Earth System Model version 1 (CESM1) to explore the composition and optical properties of these aerosol layers. The observed aerosol extinction enhancement is reproduced by CESM1/CARMA. Both model and observations indicate a strong gradient of the sulfur-to-carbon ratio from Europe to the Asia on constant pressure surfaces. We found that the ATAL is mostly composed of sulfates, surface-emitted organics, and secondary organics; the NATAL is mostly composed of sulfates and secondary organics. The model also suggests that emission increases in Asia between 2000 and 2010 led to an increase of aerosol optical depth of the ATAL by 0.002 on average which is consistent with observations. Key Points The Asian Tropopause Aerosol Layer is composed of sulfate, primary organics, and secondary organics The North American Tropospheric Aerosol Layer is mostly composed of sulfate and secondary organics Aerosol Optical Depth of Asian Tropopause Aerosol Layer increases by 0.002 from 2000 to 2010 PMID:26709320

  5. Neonatal hygroscopic condenser humidifier.

    PubMed

    Gedeon, A; Mebius, C; Palmer, K

    1987-01-01

    A hygroscopic condenser humidifier was developed for neonates on mechanical ventilation and was evaluated by laboratory tests and clinically. Humidification provided by the unit was measured in the 10- to 50-ml tidal-volume range at ambient temperatures of 24 degrees C and 38 degrees C. The effect of a leaking patient connection on device performance was investigated. Leakage rates were measured routinely in a neonatal ICU and surgery to determine the clinical significance. In the entire tidal volume and temperature range, the unit provided an inspiratory water content in excess of 30 g/m3 when the leak fraction (volume leaked/volume delivered at Y-piece) was less than 15%. This was found in three out of four cases. In about one out of ten cases, the leak exceeded 30%, which invariably led to corrective action, such as repositioning or changing the endotracheal tube. However, even at a 30% leak, a water content of about 26 g/m3 was still available for humidifying the inspired gas, which corresponds to normal physiologic conditions found in the trachea for nasal breathing of room air.

  6. New Concepts In Retrieving Aerosol Properties Using MISR

    NASA Astrophysics Data System (ADS)

    Martonchik, J.; Diner, D.; Kahn, R.; Bull, M.; Paradise, S.; Gaitley, B.; Garay, M.

    2006-12-01

    Since March 2000 the nine camera Multi-angle Imaging SpectroRadiometer (MISR) aboard NASA's EOS Terra platform has been providing information about aerosols over both land and ocean. During this period many incremental improvements to the individual ocean and land aerosol retrieval algorithms have been made but the fundamental ideas behind each have remained essentially unchanged. Here we explore some new algorithmic concepts, multiangular in nature, which may provide a considerable increase in the accuracy of retrieved aerosol properties from space. The current MISR retrieval algorithm over ocean nominally utilizes only the red (672 nm) and near IR (866 nm) spectral bands, assuming that neither band has any significant contamination from water-leaving radiance (WLR). This approach provides a good determination of aerosol optical depth but the retrieved Angstrom exponent is subject to much more uncertainty because of the relatively small wavelength separation of the red and near IR bands. The concept being explored for improving the ocean algorithm is to also include the remaining blue (446 nm) and green (558 nm) MISR bands under the assumptions that 1) only the near IR band has near-zero WLR and 2) the WLR in the remaining three bands is isotropic. An algorithm with these conditions should provide a more accurate retrieval of aerosol properties and, simultaneously, the retrieval of WLR (ocean color). Over land the current aerosol retrieval algorithm is composed of two parts. The first is an angular shape comparison of the directional surface reflectance among the four MISR spectral bands, testing for similarity, a constraint that filters out the least probable aerosol models in the retrieval process. This procedure is then followed by a principal component analysis of the change in surface contrast with view angle and the final selection of retrieved aerosol models. This algorithm has produced high quality retrievals of aerosol optical depth over a wide variety of

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

    NASA Technical Reports Server (NTRS)

    Tsay, Si-Chee; Holben, Brent N.

    2008-01-01

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

  8. Retrieval of Aerosol Optical Properties under Thin Cirrus from MODIS

    NASA Technical Reports Server (NTRS)

    Lee, Jaehwa; Hsu, Nai-Yung Christina; Bettenhausen, Corey; Sayer, Andrew Mark.

    2014-01-01

    Retrieval of aerosol optical properties using shortwave bands from passive satellite sensors, such as MODIS, is typically limited to cloud-free areas. However, if the clouds are thin enough (i.e. thin cirrus) such that the satellite-observed reflectance contains signals under the cirrus layer, and if the optical properties of this cirrus layer are known, the TOA reflectance can be corrected for the cirrus layer to be used for retrieving aerosol optical properties. To this end, we first correct the TOA reflectances in the aerosol bands (0.47, 0.55, 0.65, 0.86, 1.24, 1.63, and 2.12 micron for ocean algorithm and 0.412, 0.47, and 0.65 micron for deep blue algorithm) for the effects of thin cirrus using 1.38 micron reflectance and conversion factors that convert cirrus reflectance in 1.38 micron band to those in aerosol bands. It was found that the conversion factors can be calculated by using relationships between reflectances in 1.38 micron band and minimum reflectances in the aerosol bands (Gao et al., 2002). Refer to the example in the figure. Then, the cirrus-corrected reflectance can be calculated by subtracting the cirrus reflectance from the TOA reflectance in the optically thin case. A sensitivity study suggested that cloudy-sky TOA reflectances can be calculated with small errors in the form of simple linear addition of cirrus-only reflectances and clear-sky reflectances. In this study, we correct the cirrus signals up to TOA reflectance at 1.38 micron of 0.05 where the simple linear addition is valid without extensive radiative transfer simulations. When each scene passes the set of tests shown in the flowchart, the scene is corrected for cirrus contamination and passed into aerosol retrieval algorithms.

  9. Study on optical and microphysical properties of mixed aerosols from lidar during the EMEP 2012 summer campaign at 45oN 26oE

    NASA Astrophysics Data System (ADS)

    Talianu, Camelia; Nicolae, Doina; Belegante, Livio; Marmureanu, Luminita

    2013-04-01

    Aerosols optical and chemical properties in the upper layers of the atmosphere and near ground are variable, as function of the different mixtures of aerosol components resulting from their origin and transport over polluted areas. Due to a complex dynamics of air masses, the Romanian atmosphere has strong influences from dust and biomass-burning transported from South, West or East Europe. The dominant transport, and consequently the dominant aerosol type, depends on the season. As a result of the transport distance from the source and depending on the chemical and physical characteristics of the particles, tropospheric aerosols detected at Magurele, Romania, show different optical and microphysical properties than at the originating source. The differences are caused by the mixing with local particles, and also by the ageing processes and hygroscopic growth during the transport. This paper presents a statistical analysis of tropospheric aerosol optical properties during the EMEP (European Monitoring and Evaluation Programme) summer campaign (08 June - 17 July 2012), as retrieved from multiwavelength Raman and depolarization lidar data. Three elastic (1064, 532 and 355 nm), two Raman (607 and 387 nm) and one depolarization channel (532 nm parallel / 532 nm cross) are used to independently retrieve the backscatter coefficient, extinction coefficient and linear particle depolarization ratio of aerosols between 0.8 and 10 km altitude. Intensive optical parameters (Angstrom exponent, color ratios and color indexes) and microphysical parameters (effective radius, complex refractive index) from multiwavelength optical data inversion of the layer mean values are obtained. During the campaign, aerosol profiles were measured daily around sunset, following EARLINET standards. An intensive 3-days continuous measurements exercise was also performed. Layers were generally present above 2 km and bellow 6 km altitude, but descent of air masses from the free troposphere to the

  10. Estimate of the aerosol properties over the ocean with POLDER

    NASA Astrophysics Data System (ADS)

    Deuzé, J. L.; Goloub, P.; Herman, M.; Marchand, A.; Perry, G.; Susana, S.; Tanré, D.

    2000-06-01

    The wide field of view imaging spectroradiometer Polarization and Directionality of the Earth's Reflectance (POLDER) developed by Centre National d'Etudes Spatiales and operated aboard the Japanese heliosynchronous platform Advanced Earth Observation Satellite (ADEOS) from October 30, 1996, to June 30, 1997, provided the first global systematic measurements of the spectral, directional, and polarized characteristics of the solar radiation reflected by the Earth/atmosphere system. These original observational capabilities offer an opportunity to enhance the characterization of several components of the global environment, especially the oceanic and terrestrial vegetal primary production, the aerosol physical and optical properties, and the tridimensional structure and microphysics of clouds. Here we examine the remote sensing of aerosols over the oceans. In a first step the aerosol optical thickness and Ångström exponent are derived from the radiance measurements. In a second step the polarization measurements are used for the retrieval of the aerosol refractive index. The inversion algorithm assumes spherical, nonabsorbing particles with monomodal lognormal size distribution. The adequacy of this modeling is discussed for a representative set of aerosol observations. Successful retrieval is generally achieved in the presence of small aerosols with Ångström exponent larger than ˜1.0. For such particles, polarization may provide information on the particle refractive index. As the Ångstrom exponent of the particle decreases, the data fitting residual errors increase, especially in polarized light, which prevents the retrieval of the aerosol refractive index. The trends of the discrepancies point out two shortcomings of the aerosol modeling. The theoretical results systematically underestimate the contribution of small polarizing particles in the polarization measurements for side-scattering angles ranging from 80° to 120°. This indicates very probably that

  11. Wintertime Experimental investigation of Morphology, Mixing States and Columnar Optical Properties of Aerosols over a Desert location in India

    NASA Astrophysics Data System (ADS)

    Mishra, S.; Kumar, T.; Sharma, C.; Prasad, M. V. S. N.; Singh, S.; Agnihotri, R.; Arya, B. C.; Gupta, B.; Naaraayanan, T.; Gautam, S.; Kumar, D.; Sood, K. N.; Tawale, J. S.; Sharma, A. K.; Mitra, A. K.

    2014-12-01

    Indian Desert (The Thar Desert) is considered as the source of mineral dust in the Indo-Gangetic Plain (IGP) especially in pre-monsoon period due to large scale convective activities during hot summer. To study the physico-chemical characteristics of aerosols over the Thar Desert (Jaisalmer, Rajasthan) during winter (December, 2013), a field campaign has been carried out in Jaisalmer in Rajasthan state. Experiments were conducted inside the city as well as far from the city. The faraway location is close to international border of another country i.e. Pakistan. PM2.5 and PM10 were collected within the city while PM5 was collected far from the city. Particles were collected on Teflon filters for bulk analysis with Fourier Transform Infrared Spectroscopy (FTIR), on Tin substrate for individual particle morphology and elemental composition analysis with Scanning Electron Microscope (SEM) equipped with Energy Dispersive Spectrometer (EDS) and on the Cu-TEM grid for individual particle morphology and mixing state characterization using High Resolution-Transmission Electron Microscope (HRTEM). Together with this, aerosol size distribution observation and columnar spectral aerosol optical properties have been carried out with OPC (Optical Particle Counter, GRIMM Model 1.108) and hand held Microtops-II, respectively. HRTEM analysis reveals occurrence of carbonaceous fractals found in various mixing states 1) aged with some hygroscopic species 2) embedded in sulfate host 3) semi-externally mixed with sulfate and other species. Core-shell particles were also observed with varying core composition (carbon, typical mineral dust, and calcite) and shell thickness (shell comprising of water). The back trajectory analysis reveals the source of wind from Karachi and Islamabad from Pakistan which may be the potential source of carbonaceous species over the sampling site. SEM-EDS analysis reveals occurrence of mineral dust 1) pure mineral dust (Ca and Si rich) 2) polluted mineral

  12. Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

    SciTech Connect

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2007-09-30

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  13. Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

    SciTech Connect

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2009-03-05

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  14. Influence of Delhi Pollution on Aerosol Properties Over Greater Noida

    NASA Astrophysics Data System (ADS)

    Sharma, M.; Singh, R. P.; Kumar, R.

    2015-12-01

    Influence of Delhi Pollution on Aerosol Properties over Greater NoidaManish Sharma1, Ramesh P. Singh2 and Rajesh Kumar3 1Research and Technology Development Centre, Sharda University, Greater Noida, India. 2School of Earth and Environmental Sciences, Schmid College of Science, Chapman University, Orange 92866, USA 3School of Basic Sciences and Research, Sharda University, Greater Noida, India. Delhi capital of India is highly polluted during winter and summer seasons. Due to dominant westerly winds the air mass influence its neighboring city Greater Noida which is located 60 km south east of Delhi. Detailed analysis of multi satellite data and ground observations have been carried out during 2001-2015. The ground observation and satellite data show dynamic aerosol optical parameters over Greater Noida. During winter and summer seasons, dominant westerly wind outflow pollutants of Delhi that mix with the local anthropogenic emissions of Greater Noida influencing aerosol properties at different pressure levels. The characteristics of trace gases and aerosol parameters over Delhi and Greater Noida will be presented. The air quality is severely affected from the outflow of pollutants from Delhi which is threat to people living in the area. Due to dominant winds the air mass further transported towards eastern parts of Indo-Gangetic plains affecting weather conditions of the major cities.

  15. Optical properties of aerosols over the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Bryant, C.; Eleftheriadis, K.; Smolik, J.; Zdimal, V.; Mihalopoulos, N.; Colbeck, I.

    Measurements of aerosol optical properties, size distribution and chemical composition were conducted at Finokalia, a remote coastal site on the Greek island of Crete (35°19'N, 25°40'E) during July 2000 and January 2001. During the summer campaign the total scattering coefficient, σ, (at a wavelength of 550 nm) ranged from 13 to 120 Mm -1 (mean=44.2 Mm -1, standard deviation=17.5) whilst during the winter it ranged from 7.22 to 37.8 Mm -1 (mean=18.42 Mm -1, standard deviation=6.61). A distinct diurnal variation in scattering coefficients was observed, with minima occurring during the early morning and maxima in the late afternoon during the summer and late evening during the winter. The mean value of the Ångström exponent was 1.47 during the summer and 1.28 during the winter, suggesting a larger fraction of smaller particles at the site during the summer. This was confirmed by continuous measurements of the aerosol size distribution. An analysis of the single scattering albedo suggests that there is a more absorbing fraction in the particle composition in the summer than during the winter. An investigation of air mass origins on aerosol optical properties indicated that those from Turkey and Central/Eastern Europe were highly polluted with a corresponding impact on aerosol optical properties. A linear relationship was obtained between the total scattering coefficient and both the non-sea-salt sulphate concentrations and the fine aerosol fraction.

  16. Aerosols physical properties at Hada Al Sham, western Saudi Arabia

    NASA Astrophysics Data System (ADS)

    Lihavainen, H.; Alghamdi, M. A.; Hyvärinen, A.-P.; Hussein, T.; Aaltonen, V.; Abdelmaksoud, A. S.; Al-Jeelani, H.; Almazroui, M.; Almehmadi, F. M.; Al Zawad, F. M.; Hakala, J.; Khoder, M.; Neitola, K.; Petäjä, T.; Shabbaj, I. I.; Hämeri, K.

    2016-06-01

    This is the first time to clearly derive the comprehensive physical properties of aerosols at a rural background area in Saudi Arabia. Aerosol measurements station was established at a rural background area in the Western Saudi Arabia to study the aerosol properties. This study gives overview of the aerosol physical properties (PM10, PM2.5, black carbon and total number concentration) over the measurement period from November 2012 to February 2015. The average PM10 and PM2.5 concentrations were 95 ± 78 μg m-3 (mean ± STD, at ambient conditions) and 33 ± 68 μg m-3 (at ambient conditions), respectively. As expected PM10 concentration was dominated by coarse mode particles (PM10-PM2.5), most probably desert dust. Especially from February to June the coarse mode concentrations were high because of dust storm season. Aerosol mass concentrations had clear diurnal cycle. Lower values were observed around noon. This behavior is caused by wind direction and speed, during night time very calm easterly winds are dominating whereas during daytime the stronger westerly winds are dominating (sea breeze). During the day time the boundary layer is evolving, causing enhanced mixing and dilution leading to lower concentration. PM10 and PM2.5 concentrations were comparable to values measured at close by city of Jeddah. Black carbon concentration was about 2% and 6% of PM10 and PM2.5 mass, respectively. Total number concentration was dominated by frequent new particle formation and particle growth events. The typical diurnal cycle in particle total number concentration was clearly different from PM10 and PM2.5.

  17. Aerosol composition and variability in the Baltimore-Washington, DC region

    NASA Astrophysics Data System (ADS)

    Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

    2015-08-01

    In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type, such as composition, size and hygroscopicity, and to the surrounding atmosphere, such as temperature, relative humidity (RH) and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in-situ atmospheric profiling in the Baltimore, MD-Washington, DC region was performed during fourteen flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 49 %) due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of ammonium sulfate increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity causing an increase in the water content of the aerosol. Conversely, low aerosol loading days had lower ammonium sulfate and higher black carbon contributions causing lower single scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km decreasing to 35 ng m-3

  18. 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

  19. Vertical Profiles of Cloud Condensation Nuclei, Condensation Nuclei, Optical Aerosol, Aerosol Optical Properties, and Aerosol Volatility Measured from Balloons

    NASA Technical Reports Server (NTRS)

    Deshler, T.; Snider, J. R.; Vali, G.

    1998-01-01

    Under the support of this grant a balloon-borne gondola containing a variety of aerosol instruments was developed and flown from Laramie, Wyoming, (41 deg N, 105 deg W) and from Lauder, New Zealand (45 deg S, 170 deg E). The gondola includes instruments to measure the concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), optically detectable aerosol (OA.) (r greater than or equal to 0.15 - 2.0 microns), and optical scattering properties using a nephelometer (lambda = 530 microns). All instruments sampled from a common inlet which was heated to 40 C on ascent and to 160 C on descent. Flights with the CN counter, OA counter, and nephelometer began in July 1994. The CCN counter was added in November 1994, and the engineering problems were solved by June 1995. Since then the flights have included all four instruments, and were completed in January 1998. Altogether there were 20 flights from Laramie, approximately 5 per year, and 2 from Lauder. Of these there were one or more engineering problems on 6 of the flights from Laramie, hence the data are somewhat limited on those 6 flights, while a complete data set was obtained from the other 14 flights. Good CCN data are available from 12 of the Laramie flights. The two flights from Lauder in January 1998 were successful for all measurements. The results from these flights, and the development of the balloon-bome CCN counter have formed the basis for five conference presentations. The heated and unheated CN and OA measurements have been used to estimate the mass fraction of the aerosol volatile, while comparisons of the nephelometer measurements were used to estimate the light scattering, associated with the volatile aerosol. These estimates were calculated for 0.5 km averages of the ascent and descent data between 2.5 km and the tropopause, near 11.5 km.

  20. A COMPARISON OF CMAQ-BASED AEROSOL PROPERTIES WITH IMPROVE, MODIS, AND AERONET DATA

    EPA Science Inventory

    We compare select aerosol Properties derived from the Community Multiscale Air Quality (CMAQ) model-simulated aerosol mass concentrations with routine data from the National Aeronautics and Space Administration (NASA) satellite-borne Moderate Resolution Imaging Spectro-radiometer...

  1. Retrieval of stratospheric aerosol size distributions and integral properties from simulated lidar backscatter measurements.

    PubMed

    Yue, G K

    2000-10-20

    A new approach for retrieving aerosol properties from extinction spectra is extended to retrieve aerosol properties from lidar backscatter measurements. In this method it is assumed that aerosol properties are expressed as a linear combination of backscatters at three or fewer wavelengths commonly used in lidar measurements. The coefficients in the weighted linear combination are obtained by minimization of the retrieval error averaged for a set of testing size distributions. The formulas can be used easily by investigators to retrieve aerosol properties from lidar backscatter measurements such as the Lidar In-Space Technology Experiment and Pathfinder Instruments for Clouds and Aerosols Spaceborne Observations.

  2. Automated Measurements of Ambient Aerosol Chemical Composition and its Dry and Wet Size Distributions at Pittsburgh Supersite

    NASA Astrophysics Data System (ADS)

    Khlystov, A. Y.; Stanier, C.; Chun, W.; Vayenas, D.; Mandiro, M.; Pandis, S. N.

    2001-12-01

    Ambient aerosol particles change size with changes in ambient relative humidity. The magnitude of the size change depends on the hygroscopic properties of the particles, which is determined by their chemical composition. Hygroscopic properties of particles influence many environmentally important aerosol qualities, such as light scattering and partitioning between the gas and particle phases of semivolitile compounds. Studying the hygroscopic growth of ambient particles is thus of paramount importance. The highroscopic growth of ambient particles and their chemical composition are measured continuously within the Pittsburgh Air Quality Study (EPA supersite program). The hygroscopic size changes are measured using an automated system built for this study. The system consists of two Scanning Mobility Particle Sizers (SMPS, TSI Inc.) and an Aerodynamic Particle Sizer (APS, TSI Inc.). The three instruments measure aerosol size distribution between 5 nanometers and 10 micrometers in diameter. The inlets of the instruments and the sheath air lines of the SMPS systems are equipped with computer controlled valves that direct air through Nafion dryers (PermaPure Inc.) or bypass them. The Nafion dryers are drying the air stream below 40% RH at which point ambient particles are expected to lose most or all water and thus be virtually dry. To avoid changes in relative humidity and evaporation of volatile particles due to temperature differences the system is kept at ambient temperature. The system measures alternatively dry (below 40% RH) and wet (actual ambient RH) aerosol size distributions every 6 minutes. The hygroscopic growth observed with the size-spectrometer system is compared with theoretic predictions based on the chemical composition of aerosol particles. A modified semi-continuous Steam-Jet Aerosol Collector provides the total available budget (particles and gas) of water-soluble species, which is used as an input to the thermodynamic model. The model calculates

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

    NASA Astrophysics Data System (ADS)

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

    2007-06-01

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

  4. 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.

  5. 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.

  6. 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

  7. Particle Property Data Quality Flags for the MISR Aerosol Product

    NASA Astrophysics Data System (ADS)

    Gaitley, B. J.; Kahn, R. A.; Garay, M. J.

    2012-12-01

    The MISR instrument aboard the NASA Earth Observing System's Terra satellite has the unique capability to retrieve aerosol properties under favorable conditions. General aerosol type retrieval quality guidelines are provided in the MISR Data Quality Statement and related publications. Here we report on the steps we are taking to provide an aerosol-type data quality flag, to be provided with each individual retrieval result. Some factors affecting retrieval quality that can be assessed pre-retrieval are the number of cameras available, the range of scattering angles and surface conditions such as shallow water or seasonal coastal runoff. Factors that must be assessed post-retrieval include low values of retrieved optical depth and the number and type of mixtures successfully passing the MISR algorithm acceptance criteria. Regional monthly plots with MISR measurements binned at 0.5 degree resolution with color-coded stratification of one or more parameters is the main method for identifying locations and times where particle properties are retrieved. Individual MISR values such as mid-visible AOD, number and type of mixtures passing, number of cameras used, the range and maximum scattering angles are plotted individually or as joint distributions. Initially, thresholds and conditions are determined for each MISR parameter separately. Finally, MISR parameters are combined for a given month and region, with their thresholds, to show the overall quality of the retrieval for determining particle properties. Multi-month summaries for more than twelve years of MISR data will aid in assessing quality. Seasons and regions that regularly show poorly constrained aerosol type results are identified, as are times and places where particle property information can be used with confidence. This work is performed in part at the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration and in part at the NASA

  8. Studing Taklamakan aerosol properties with Lidar (STAPL)

    Technology Transfer Automated Retrieval System (TEKTRAN)

    By now, the global impacts of atmospheric dust have been well-established. Nevertheless, relevant properties such as size distribution, depolarization ratio, and even single-scattering albedo have been shown to vary substantially between dust producing regions and are also strongly dependent on the ...

  9. Aerosol properties and associated radiative effects over Cairo (Egypt)

    NASA Astrophysics Data System (ADS)

    El-Metwally, M.; Alfaro, S. C.; Wahab, M. M. Abdel; Favez, O.; Mohamed, Z.; Chatenet, B.

    2011-02-01

    Cairo is one of the largest megacities in the World and the particle load of its atmosphere is known to be particularly important. In this work we aim at assessing the temporal variability of the aerosol's characteristics and the magnitude of its impacts on the transfer of solar radiation. For this we use the level 2 quality assured products obtained by inversion of the instantaneous AERONET sunphotometer measurements performed in Cairo during the Cairo Aerosol CHaracterization Experiment (CACHE), which lasted from the end of October 2004 to the end of March 2006. The analysis of the temporal variation of the aerosol's optical depth (AOD) and spectral dependence suggests that the aerosol is generally a mixture of at least 3 main components differing in composition and size. This is confirmed by the detailed analysis of the monthly-averaged size distributions and associated optical properties (single scattering albedo and asymmetry parameter). The components of the aerosol are found to be 1) a highly absorbing background aerosol produced by daily activities (traffic, industry), 2) an additional, 'pollution' component produced by the burning of agricultural wastes in the Nile delta, and 3) a coarse desert dust component. In July, an enhancement of the accumulation mode is observed due to the atmospheric stability favoring its building up and possibly to secondary aerosols being produced by active photochemistry. More generally, the time variability of the aerosol's characteristics is due to the combined effects of meteorological factors and seasonal production processes. Because of the large values of the AOD achieved during the desert dust and biomass burning episodes, the instantaneous aerosol radiative forcing (RF) at both the top (TOA) and bottom (BOA) of the atmosphere is maximal during these events. For instance, during the desert dust storm of April 8, 2005 RF BOA, RF TOA, and the corresponding atmospheric heating rate peaked at - 161.7 W/m 2, - 65.8 W/m 2

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

    NASA Astrophysics Data System (ADS)

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

    2008-02-01

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

  11. Evaluation of Aerosol Properties in GCMs using Satellite Measurements

    NASA Astrophysics Data System (ADS)

    Wang, Y.; Jiang, J. H.; Su, H.; Zhang, H.

    2015-12-01

    Atmospheric aerosols from natural or anthropogenic sources have profound impacts on the regional and global climate. Currently the radiative forcing of aerosols predicted by global climate models remains highly uncertain, representing the largest uncertainty in climate predictions. The uncertainty mainly arises from the complicated aerosol chemical and physical properties, coarse emission inventories for pre-cursor gases as well as unrealistic representations of aerosol activation and cloud processing in global climate models. In this study, we will utilize multiple satellite measurements including MODIS, MISR and CALIPSO to quantitatively evaluate aerosol simulations from climate models. Our analyses show that the global means in AOD climatology from NCAR CAM5 and GFDL AM3 simulations are comparable with satellite measurements. However, the overall correlation coefficient between the AOD spatial patterns from CAM5 and satellite is only 0.4. Moreover, at finer scales, the magnitude of AOD in CAM5 is much lower than satellite measurements for most of the non-dust regions, especially over East Asia. GFDL AM3 shows better AOD simulations over East Asia. The underestimated AOD over remote maritime areas in CAM5 was attributed to the unrealistic wet removal processes in convective clouds of CAM5. Over continents, biases on AOD could stem from underestimations in the emissions inventory and unresolved sub-grid variations of relative humidity due to the model's coarse resolution. Uncertainty from emission inventory over developing countries in East Asia will be assessed using the newly updated Regional Emission inventory in Asia (REAS) and Multi-resolution Emission Inventory in China (MEIC) in the model simulations.

  12. Optical and microphysical properties of atmospheric aerosols in Moldova

    NASA Astrophysics Data System (ADS)

    Aculinin, Alexandr; Smicov, Vladimir

    2010-05-01

    Measurements of aerosol properties in Kishinev, Moldova are being carried out within the framework of the international AERONET program managed by NASA/GSFC since 1999. Direct solar and sky diffuse radiances are measured by using of sunphotometer Cimel-318. Aerosol optical properties are retrieved from measured radiances by using of smart computational procedures developed by the AERONET's team. The instrument is situated at the ground-based solar radiation monitoring station giving the opportunity to make simultaneous spectral (win sunphotometer) and broadband (with the set of sensors from radiometric complex) solar radiation. Detailed description of the station and investigations in progress can be found at the http://arg.phys.asm.md. Ground station is placed in an urban environment of Kishinev city (47.00N; 28.56E; 205 m a.s.l). Summary of aerosol optical and microphysical properties retrieved from direct solar and diffuse sky radiance observations at Moldova site from September 1999 to June 2009 are presented below. Number of measurements (total): 1695 Number of measurements (for ?o, n, k): 223 Range of aerosol optical depth (AOD) @440 nm: 0.03 < ?(440) < 2.30, < ?(440)>=0.25 Range of Ångström parameter < α440_870 >: 0.14 < α < 2.28 Asymmetry factor (440/670/870/1020): 0.70/0.63/0.59/0.58 ±0.04 Refraction (n) and absorption (k) indices@440 nm: 1.41 ± 0.06; 0.009 ± 0.005 Single scattering albedo < ?o >(440/670/870/1020): 0.93/0.92/0.90/0.89 ±0.04 Parameters of volume particle size distribution function: (fine mode) volume median radius r v,f , μm: 0.17 ± 0.06 particle volume concentration Cv,f, μm3/μm2: 0.04 ± 0.03 (coarse mode) volume median radius rv,c , μm: 3.08 ± 0.64 particle volume concentration Cv,c, μm3/μm2: 0.03 ± 0.03 Climatic norms of AOD@500 nm and Ångström parameter < α440_870 > at the site of observation are equal to 0.21 ± 0.06 and 1.45 ± 0.14, respectively. The aerosol type in Moldova may be considered as 'urban

  13. Vertical Profile of Aerosol Properties at Pico Mountain, Azores

    NASA Astrophysics Data System (ADS)

    Wright, K.; Mazzoleni, C.; Mazzoleni, L. R.; Dzepina, K.; Hueber, J.; China, S.; Sharma, N.

    2013-12-01

    of aerosol properties in a marine environment from the boundary layer to the free troposphere. The analysis of these data will help us understand the role of aerosol aging, vertical transport and distribution in a marine environment.

  14. Star Photometry for the Characterization of Columnar Aerosol Properties

    NASA Astrophysics Data System (ADS)

    Perez-Ramirez, D.; Lyamani, H.; Olmo Reyes, F. J.; Alados-Arboledas, L.; Whiteman, D. N.; Aceituno, J.

    2015-12-01

    Knowledge of columnar aerosol particles at nighttime is essential to completely understand aerosol dynamics and so will largely improve aerosol models. However, the current knowledge columnar nighttime aerosol is poor due to the lack of continuous measurements partly associated with previous technological limitations. Here we present the development, set up, calibration and data quality algorithms for the star photometer at the station of Granada (37.16 N, 3.60 W, 680 m a.s.l.) in Spain. The main advantage of this instrument is that make uses of a CCD camera as detector allowing direct star flux measurements. Filters center at 380, 440, 500, 670, 880 and 1020 nm allows spectral aerosol optical depth (AOD) measurements. Among all the stars, only those that are isolated and possess constant extratarrestial flux are considered. Two methods for the calibration of the system at high mountain places are presented. The first one consists of doing a Langley calibration of a selected star together with measurements of other stars. From the Langley calibration, we transferred AOD and get the calibration constants for other stars. The second method is the Astronomical Langley Method that consists of dividing the measurements by the optical air mass and so more stable calibration constant are obtained. On the other hand, the atmospheric turbulence is important for very short exposure times (< 1 s) and so uncertainties in AOD are of ±0.02 for λ < 800nm and ±0.01 for λ > 800nm. The instrument operated continuously for more than four consecutive years and so a large database was created. Cloud screening and data quality algorithms following AERONET inheritance were developed. Basically, moving averages are applied with different temporal-windows combined with a procedure to detect outliers. On the other hand, with quality data guaranteed the analysis of day-to-night columnar aerosol properties is presented. Mean AOD(440 nm) (0.18 ± 0.10 and 0.19 ± 0.11 for daytime and

  15. Aerosol Optical Properties During The SAMUM-2 Experiment

    NASA Astrophysics Data System (ADS)

    Toledano, C.; Freudenthaler, V.; Gross, S.; Seefeldner, M.; Gasteiger, J.; Garhammer, M.; Esselborn, M.; Wiegner, M.; Koepke, P.

    2009-03-01

    A field campaign of the Saharan Mineral Dust Experiment (SAMUM-2) took place in the Cape Verde islands in January-February 2008, to investigate the properties of long-range transported dust over the Atlantic. The Meteorological Institute of the University of Munich deployed a set of active and passive remote sensing instruments: one sun photometer, for the measurement of the direct sun irradiance and sky radiances; a broad-band UV radiometer; and 2 tropospheric lidar systems. The measurements were made in close cooperation with the other participating groups. During the measurement period the aerosol scenario over Cape Verde mostly consisted of a dust layer below 2 km and a smoke layer above 2 km height. The Saharan dust arrived in the site from the NE, whereas the smoke originated in the African equatorial region is transported from the SE. The aerosol load was also very variable over this area, with AOD (500 nm) ranging from 0.04 to 0.74. The optical properties of the layers are shown: extinction and particle depolarization ratio profiles at 3 wavelengths, as well as aerosol optical depth (in the range 340-1550 nm), Ångström exponent, size distribution and single scattering albedo.

  16. Sodium Nitrate Particles: Physical and Chemical Properties During Hydration and Dehydration, and Implications for Aged Sea Salt Aerosols

    SciTech Connect

    Hoffman, Rachel C.; Laskin, Alexander; Finlayson-Pitts, Barbara J.

    2004-07-01

    Experiments probing the phase and behavior of NaNO3 particles at different relative humidities, important for elucidating the role these play in the chemistry and radiative properties of marine regions, are presented. Changes in NaNO3 particles during hydration were studied using environmental scanning electron microscopy (ESEM) and conventional SEM coupled with energy dispersive X-ray analysis (SEM/EDX). Mixtures of NaNO3 and NaCl, which are typical of partially processed sea salt particles, were also studied. Complementary studies using long path FTIR were carried out to determine the extent of water association with NaNO3 aerosols, and for comparison, NaCl, MgCl2, and NH4NO3, as a function of relative humidity. The combination of these techniques shows that NaNO3 particles exist as unusual metastable, amorphous solids at low relative humidity that undergo continuous hygroscopic growth with increasing relative humidity. While other evidence for this phenomenon has been reported, this is the first direct observation using ESEM.

  17. Laboratory Studies of the Reactive Chemistry and Changing CCN Properties of Secondary Organic Aerosol, Including Model Development

    SciTech Connect

    Scot Martin

    2013-01-31

    The chemical evolution of secondary-organic-aerosol (SOA) particles and how this evolution alters their cloud-nucleating properties were studied. Simplified forms of full Koehler theory were targeted, specifically forms that contain only those aspects essential to describing the laboratory observations, because of the requirement to minimize computational burden for use in integrated climate and chemistry models. The associated data analysis and interpretation have therefore focused on model development in the framework of modified kappa-Koehler theory. Kappa is a single parameter describing effective hygroscopicity, grouping together several separate physicochemical parameters (e.g., molar volume, surface tension, and van't Hoff factor) that otherwise must be tracked and evaluated in an iterative full-Koehler equation in a large-scale model. A major finding of the project was that secondary organic materials produced by the oxidation of a range of biogenic volatile organic compounds for diverse conditions have kappa values bracketed in the range of 0.10 +/- 0.05. In these same experiments, somewhat incongruently there was significant chemical variation in the secondary organic material, especially oxidation state, as was indicated by changes in the particle mass spectra. Taken together, these findings then support the use of kappa as a simplified yet accurate general parameter to represent the CCN activation of secondary organic material in large-scale atmospheric and climate models, thereby greatly reducing the computational burden while simultaneously including the most recent mechanistic findings of laboratory studies.

  18. The influence of meteoric smoke particles on stratospheric aerosol properties

    NASA Astrophysics Data System (ADS)

    Mann, Graham; Brooke, James; Dhomse, Sandip; Plane, John; Feng, Wuhu; Neely, Ryan; Bardeen, Chuck; Bellouin, Nicolas; Dalvi, Mohit; Johnson, Colin; Abraham, Luke

    2016-04-01

    The ablation of metors in the thermosphere and mesosphere introduces a signficant source of particulate matter into the polar upper stratosphere. These meteoric smoke particles (MSP) initially form at nanometre sizes but in the stratosphere have grown to larger sizes (tens of nanometres) following coagulation. The presence of these smoke particles may represent a significant mechanism for the nucleation of polar stratospheric clouds and are also known to influence the properties of the stratospheric aerosol or Junge layer. In this presentation we present findings from experiments to investigate the influence of the MSP on the Junge layer, carried out with the UM-UKCA composition-climate model. The UM-UKCA model is a high-top (up to 80km) version of the general circulation model with well-resolved stratospheric dynamics, includes the aerosol microphysics module GLOMAP and has interactive sulphur chemistry suitable for the stratosphere and troposphere (Dhomse et al., 2014). We have recently added to UM-UKCA a source of meteoric smoke particles, based on prescribing the variation of the smoke particles from previous simulations with the Whole Atmosphere Community Climate Model (WACCM). In UM-UKCA, the MSP particles are transported within the GLOMAP aerosol framework, alongside interactive stratospheric sulphuric acid aerosol. For the experiments presented here, we have activated the interaction between the MSP and the stratospheric sulphuric acid aerosol. The MSP provide an important sink term for the gas phase sulphuric acid simulated in the model, with subsequent effects on the formation, growth and temporal evolution of stratospheric sulphuric acid aerosol particles. By comparing simulations with and without the MSP-sulphur interactions we quantify the influence of the meteoric smoke on the properties of volcanically-quiescent Junge layer. We also investigate the extent to which the MSP may modulate the effects from SO2 injected into the stratosphere from volcanic

  19. Radiative Properties of Smoke and Aerosol Over Land Surfaces

    NASA Technical Reports Server (NTRS)

    King, Michael D.

    2000-01-01

    This talk discusses smoke and aerosol's radiative properties with particular attention to distinguishing the measurement over clear sky from clouds over land, sea, snow, etc. surfaces, using MODIS Airborne Simulator data from (Brazil, arctic sea ice and tundra and southern Africa, west Africa, and other ecosystems. This talk also discusses the surface bidirectional reflectance using Cloud Absorption Radiometer, BRDF measurements of Saudi Arabian desert, Persian Gulf, cerrado and rain forests in Brazil, sea ice, tundra, Atlantic Ocean, Great Dismal Swamp, Kuwait oil fire smoke. Recent upgrades to instrument (new TOMS UVA channels at 340 and 380 planned use in Africa (SAFARI 2000) and possibly for MEIDEX will also be discussed. This talk also plans to discuss the spectral variation of surface reflectance over land and the sensitivity of off-nadir view angles to correlation between visible near-infrared reflectance for use in remote sensing of aerosol over land.

  20. Ice Nucleation Properties of Amospherically Aged Biomass Burning Aerosol

    NASA Astrophysics Data System (ADS)

    Polen, M.; Lawlis, E.; Sullivan, R. C.

    2015-12-01

    Biomass burning can sometimes emit surprisingly active ice nucleating particles, though these emissions are not at all consistent between biomass fuel sources and burns. Soot from biomass combustion has been attributed to some but not all of the ice nucleating potential of biomass burning aerosol (BBA), while fossil fuel combustion soot emits very weak ice nucleants. The causes of the sometimes significant but variable ice nucleating ability of BBA are still largely unknown. BBA experiences significant atmospheric aging as the plume evolves and mixes with background air, yet almost no reports exploring the effects of atmospheric aging on the freezing properties of BBA have been made. We have performed some of the first experiments to determine the effects of simulated atmospheric aging on these ice nucleation properties, using a chamber reactor. The fresh and aged BBA was collected for subsequent droplet freezing array analysis using an impinger sampler to collect aerosol in water, and by deposition onto substrates in a MOUDI sampler. Droplets containing the chamber particles were then suspended in oil on a cold plate for freezing temperature spectrum measurement. Aging of Sawgrass flaming-phase combustion BBA by exposure to hydroxyl radicals (from H2O2 photolysis) enhanced the ice nucleation ability, observed by a shift to warmer droplet freezing temperatures by ~2-3°C. The changes in the aerosol's chemical composition during aging were observed using a laser ablation single-particle mass spectrometer and a soot-particle aerosol mass spectrometer. We will report our observations of the effects of other types of simulated aging (including photochemistry under high and low NOx conditions, dark ozonolysis, and nitric acid exposure) on Sawgrass and BBA from other grass and palm fuels.

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

    EPA Science Inventory

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

  2. Study of the effect of humidity, particle hygroscopicity and size on the mass loading capacity of HEPA filters

    SciTech Connect

    Gupta, A.

    1992-01-01

    The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake porosity estimates, the agreement was poor.

  3. Study of the effect of humidity, particle hygroscopicity and size on the mass loading capacity of HEPA filters

    SciTech Connect

    Gupta, A.

    1992-09-01

    The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake porosity estimates, the agreement was poor.

  4. 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

  5. Pathophysiological and disease constraints on aerosol delivery

    SciTech Connect

    Gerrity, T.R.

    1989-01-01

    The dose of inhaled particles to the respiratory tract depends upon many factors. These factors include the size of the particles, the pattern of breathing (flow and tidal volume), the physical properties of the articles (hygroscopic or non-hygroscopic), anatomy of the respiratory tract, and the pathophysiologic status of the respiratory tract. In addition to these factors, which are primarily related to the deposition of particles, the rate of particle clearance from the respiratory tract also influences the dose of particles. The paper is a review of the various factors influencing dose of inhaled particles to the respiratory tract. The emphasis of the paper is on therapeutic aerosol particles, though the principals discussed also apply to toxic particles as well. An important area of consideration is the influence of disease on the delivery of particle dose. From the point of view of toxic particles this is important when considering potential susceptible populations.

  6. Remote Sensing of Aerosol and Cloud Properties from Ground Based and Satellite Remote Sensors to Explore Aerosol-Cloud Interaction

    NASA Astrophysics Data System (ADS)

    He, Yuzhe

    The measurements of both aerosol and cloud properties are critical for climate studies since these mechanisms have the largest uncertainty in energy balance calculations. In addition, aerosols and clouds do not act independently but can significantly couple to each other. It is clear that being able to quantify these interactions is crucial to climate models. While there are many possible aerosol-cloud interactions, we limit our investigation to the Twomey indirect effect which relates how aerosols can modify the physical properties of clouds thereby changing the radiative properties. Verifying and quantifying such mechanisms on a global scale requires accurate measurements of both aerosols and clouds from satellites. Unfortunately, assessing this mechanism has been very difficult from satellites since both aerosols and cloud properties would have to be simultaneously measured. Therefore, only statistical approaches have been tried but it is easy to see that such approaches will tend to obscure the interpretation of local interaction mechanisms. In this thesis, we investigate the potential of both satellites and ground based approaches to measure Aerosol Cloud Interaction parameters. After assessing the limitations of satellite based approaches, we focus on the use of ground based remote sensing using a combination of Lidar, Microwave radiometry, Doppler Lidar and sky radiometry. This instrumentation suite offers a more direct approach that can probe the properties of both aerosols and clouds simultaneously allowing us to investigate real time aerosol-cloud processes which occur on time scale < 1 minute. To this end, we first provide a thorough description of the multi-sensor approach and how it can be implemented including a sensitivity analysis taking into account both atmospheric and surface variability as well as uncertainty in both the Liquid Water Path (LWP) and diffuse transmittance measurements. In addition, we use the Southern Great Plain (SGP) data to

  7. Aerosols optical properties in Titan's Detached Haze Layer

    NASA Astrophysics Data System (ADS)

    Seignovert, Benoit; Rannou, Pascal; Lavvas, Panayotis; West, Robert

    2016-10-01

    Titan's Detached Haze Layer (DHL) was first observed in 1983 by Rages and Pollack during the Voyager 2 is a consistent spherical haze feature surrounding Titan's upper atmosphere and detached from the main haze. Since 2005, the Imaging Science Subsystem (ISS) instrument on board the Cassini mission performs a continuous survey of the Titan's atmosphere and confirmed its persistence at 500 km up to the equinox (2009) before its drop and disappearance in 2012 (West et al. 2011). Previous analyses showed, that this layer corresponds to the transition area between small spherical aerosols and large fractal aggregates and play a key role in the aerosols formation in Titan's atmosphere (Rannou et al. 2000, Lavvas et al. 2009, Cours et al. 2011).In this talk we will present the UV photometric analyses based on radiative transfer inversion to retrieve aerosols particles properties in the DHL (bulk and monomer radius and local density) performed on ISS observations taken from 2005 to 2007.References:- Rages and Pollach, Icarus 55 (1983)- West, et al., Icarus 38 (2011)- Rannou, et al., Icarus 147 (2000)- Lavvas, et al., Icarus 201 (2009)- Cours, et al., ApJ Lett. 741 (2015)

  8. Chemical and physicochemial properties of submicron aerosol agglomerates

    SciTech Connect

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

    1998-12-31

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

  9. Sensitivity of aerosol optical depth, single scattering albedo, and phase function calculations to assumptions on physical and chemical properties of aerosol

    EPA Science Inventory

    In coupled chemistry-meteorology simulations, the calculation of aerosol optical properties is an important task for the inclusion of the aerosol effects on the atmospheric radiative budget. However, the calculation of these properties from an aerosol profile is not uniquely defi...

  10. Impact of particle nonsphericity on the development and properties of aerosol models for East Asia

    NASA Astrophysics Data System (ADS)

    Chen, Hao; Cheng, Tianhai; Gu, Xingfa; Wu, Yu

    2015-01-01

    In this paper, the effects of aerosol nonsphericity information on the classification of aerosol models and the associated radiative properties over East Asia are investigated. The radiance measurements and inversions of the Aerosol Robotic Network (AERONET) are used. Four aerosol models over East Asia are obtained by adding the shape information to the clustering analysis. These four aerosols are identified on the basis of their optical properties. Compared to the results without sphericity parameter, adding the sphericity parameter in the clustering process contributes to the extraction of a strongly absorbing aerosol. Furthermore, the effect of the physical and optical properties of the aerosol on the top of atmospheric (TOA) total reflectance and polarized reflectance are investigated. The results indicate that the addition of the sphericity parameter in the clustering process leads to a change in the total reflectance by up to 16% and a change in the polarized reflectance by up to 100%.

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

    NASA Astrophysics Data System (ADS)

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

    2005-03-01

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

  12. Upper-atmosphere Aerosols: Properties and Natural Cycles

    NASA Technical Reports Server (NTRS)

    Turco, Richard P.

    1992-01-01

    The middle atmosphere is rich in its variety of particulate matter, which ranges from meteorite debris, to sulfate aerosols, to polar stratospheric ice clouds. Volcanic eruptions strongly perturb the stratospheric sulfate (Junge) layer. High-altitude 'noctilucent' ice clouds condense at the summer mesopause. The properties of these particles, including their composition, sizes, and geographical distribution, are discussed, and their global effects, including chemical, radiative, and climatic roles, are reviewed. Polar stratospheric clouds (PSCs) are composed of water and nitric acid in the form of micron-sized ice crystals. These particles catalyze reactions of chlorine compounds that 'activate' otherwise inert chlorine reservoirs, leading to severe ozone depletions in the southern polar stratosphere during austral spring. PSCs also modify the composition of the polar stratosphere through complex physiocochemical processes, including dehydration and denitrification, and the conversion of reactive nitrogen oxides into nitric acid. If water vapor and nitric acid concentrations are enhanced by high-altitude aircraft activity, the frequency, geographical range, and duration of PSCs might increase accordingly, thus enhancing the destruction of the ozone layer (which would be naturally limited in geographical extent by the same factors that confine the ozone hole to high latitudes in winter). The stratospheric sulfate aerosol layer reflects solar radiation and increases the planetary albedo, thereby cooling the surface and possibly altering the climate. Major volcanic eruptions, which increase the sulfate aerosol burden by a factor of 100 or more, may cause significant global climate anomalies. Sulfate aerosols might also be capable of activating stratospheric chlorine reservoirs on a global scale (unlike PCSs, which represent a localized polar winter phenomenon), although existing evidence suggests relatively minor perturbations in chlorine chemistry. Nevertheless, if

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

    NASA Astrophysics Data System (ADS)

    Giles, David M.

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

  14. Optical Properties of Black and Brown Carbon Aerosols from Laboratory Combustion of Wildland Fuels

    NASA Astrophysics Data System (ADS)

    Beres, N. D.; Molzan, J.

    2015-12-01

    Aerosol light absorption in the solar spectral region (300 nm - 2300 nm) of the atmosphere is key for the direct aerosol radiative forcing, which is determined by aerosol single scattering albedo (SSA), asymmetry parameter, and by the albedo of the underlying surface. SSA is of key importance for the sign and quantity of aerosol direct radiative forcing; that is, does the aerosol make the earth look darker (heating) or whiter (cooling)? In addition, these optical properties are needed for satellite retrievals of aerosol optical depth and properties. During wildland fires, aerosol optical absorption is largely determined by black carbon (BC) and brown carbon (BrC) emissions. BC is strongly absorbing throughout the solar spectrum, while BrC absorption strongly increases toward shorter wavelength and can be neglected in the red and infrared. Optical properties of BrC emitted from wildland fires are poorly understood and need to be studied as function of fuel type and moisture content and combustion conditions. While much more is known about BC optical properties, knowledge for the ultraviolet (UV) spectral region is still lacking and critically needed for satellite remote sensing (e.g., TOMS, OMI) and for modeling of tropospheric photochemistry. Here, a project to better characterize biomass burning aerosol optical properties is described. It utilizes a laboratory biomass combustion chamber to generate aerosols through combustion of different wildland fuels of global and regional importance. Combustion aerosol optics is characterized with an integrating nephelometer to measure aerosol light scattering and a photoacoustic instrument to measure aerosol light absorption. These measurements will yield optical properties that are needed to improve qualitative and quantitative understanding of aerosol radiative forcing and satellite retrievals for absorbing carbonaceous aerosols from combustion of wildland fuels.

  15. Titan's aerosol optical properties with VIMS observations at the limb

    NASA Astrophysics Data System (ADS)

    Rannou, Pascal; Seignovert, Benoit; Le Mouelic, Stephane; Sotin, Christophe

    2016-06-01

    The study of Titan properties with remote sensing relies on a good knowledge of the atmosphere properties. The in-situ observations made by Huygens combined with recent advances in the definition of methane properties enable to model and interpret observations with a very good accuracy. Thanks to these progresses, we can analyze in this work the observations made at the limb of Titan in order to retrieve information on the haze properties as its vertical profiles but also the spectral behaviour between 0.88 and 5.2 µm. To study the haze layer and more generally the source of opacities in the stratosphere, we use some observation made at the limb of Titan by the VIMS instrument onboard Cassini. We used a model in spherical geometry and in single scattering, and we accounted for the multiple scattering with a parallel plane model that evaluate the multiple scattering source function at the plane of the limb. Our scope is to retrieve informations about the vertical distribution of the haze, its spectral properties, but also to obtain details about the shape of the methane windows to desantangle the role of the methane and of the aerosols. We started our study at the latitude of 55°N, with a image taken in 2006 with a relatively high spatial resolution (for VIMS). Our preliminary results shows the spectral properties of the aerosols are the same whatever the altitude. This is a consequence of the large scale mixing. From limb profile between 0.9 and 5.2 µm, we can probe the haze layer from about 500 km (at 0.9 µm) to the ground (at 5.2 µm). We find that the vertical profile of the haze layer shows three distinct scale heights with transitions around 250 km and 350 km. We also clearly a transition around 70-90 km that may be due to the top of a condensation layer.

  16. Spatial variation of aerosol optical properties in North China Plain

    NASA Astrophysics Data System (ADS)

    Fan, Xuehua

    2013-04-01

    The column-integrated optical properties of aerosol in Beijing and Xianghe situated at North China Plain were investigated based on Sun/sky radiometer measurements made at Aerosol Robotic Network (AERONET) sites. Only version 2 and level 2 quality-assured data were presented and analyzed in this paper. Time intervals differ for the two sites, with Beijing having 9 years of data (Mar.-May, 2001; Apr., 2002-Dec., 2011),while Xianghe having 6 years of data (Mar.-Apr., 2001;Sep., 2004-Dec.,2011). Monthly mean 500 nm AOT values reach a maximum in June (0.95) and exceed 0.55 from March through September, and the minimum values occur during the late fall and winter months of November through February at Beijing. The monthly mean AOT values at Xianghe are very close to those measured at Beijing. The absolute differences of AOT between the two sites are less than 0.1 except in June and July. The reason of large difference in June and July is the frequently cloud contamination in summer result in the monthly means over the two sites computed from a large number of measurements of different date. The monthly averaged AOT with the same date in June and July are re-computed and the absolute difference of AOT between Beijing and Xianghe reduced to 0.01 and 0.03 in June and July respectively. The monthly mean Angstrom Exponent (AE) in Beijing and Xianghe sites are very close, with the absolute difference less than 0.075. The monthly mean AE in the two sites varied between ~1.0 and ~1.3 except in spring (March-May), therefore clearly dominated by fine mode aerosol for most of the year. All monthly averaged SSA at Beijing showed much lower value as compared to Xianghe though the seasonal variations are similar for the two sites, which indicates that aerosol absorption is greater in Beijing. All monthly averaged imaginary part of refractive index at Beijing has much higher value than Xianghe. The absolute differences of SSA between the two sites range from 0.016 to 0.037 except that

  17. New algorithm to derive the microphysical properties of the aerosols from lidar measurements using OPAC aerosol classification schemes

    NASA Astrophysics Data System (ADS)

    Talianu, Camelia; Labzovskii, Lev; Toanca, Florica

    2014-05-01

    This paper presents a new method to retrieve the aerosol complex refractive index and effective radius from multiwavelength lidar data, using an integrated model-measurement approach. In the model, aerosols are assumed to be a non-spherical ensemble of internally mixed components, with variable proportions. OPAC classification schemes and basic components are used to calculate the microphysical properties, which are then fed into the T-matrix calculation code to generate the corresponding optical parameters. Aerosol intensive parameters (lidar ratios, extinction and backscatter Angstrom coefficients, and linear particle depolarization ratios) are computed at the altitude of the aerosol layers determined from lidar measurements, and iteratively compared to the values obtained by simulation for a certain aerosol type, for which the critical component's proportion in the overall mixture is varied. Microphysical inversion based on the Truncated Singular Value Decomposition (TSVD) algorithm is performed for selected cases of spherical aerosols, and comparative results of the two methods are shown. Keywords: Lidar, aerosols, Data inversion, Optical parameters, Complex Refractive Index Acknowledgments: This work has been supported by grants of the Romanian National Authority for Scientific Research, Programme for Research- Space Technology and Advanced Research - STAR, project numbers 38/2012 - CAPESA and 55/2013 - CARESSE, and by the European Community's FP7-INFRASTRUCTURES-2010-1 under grant no. 262254 - ACTRIS and by the European Community's FP7-PEOPLE-2011-ITN under grant no. 289923 - ITARS

  18. UManSysProp v1.0: an online and open-source facility for molecular property prediction and atmospheric aerosol calculations

    NASA Astrophysics Data System (ADS)

    Topping, David; Barley, Mark; Bane, Michael K.; Higham, Nicholas; Aumont, Bernard; Dingle, Nicholas; McFiggans, Gordon

    2016-03-01

    In this paper we describe the development and application of a new web-based facility, UManSysProp (http://umansysprop.seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN (cloud condensation nuclei) activation potential of mixed inorganic-organic aerosol particles; and absorptive partitioning calculations with/without a treatment of non-ideality. The aim of this new facility is to provide a single point of reference for all properties relevant to atmospheric aerosol that have been checked for applicability to atmospheric compounds where possible. The group contribution approach allows users to upload molecular information in the form of SMILES (Simplified Molecular Input Line Entry System) strings and UManSysProp will automatically extract the relevant information for calculations. Built using open-source chemical informatics, and hosted at the University of Manchester, the facilities are provided via a browser and device-friendly web interface, or can be accessed using the user's own code via a JSON API (application program interface). We also provide the source code for all predictive techniques provided on the site, covered by the GNU GPL (General Public License) license to encourage development of a user community. We have released this via a Github repository (doi:10.5281/zenodo.45143). In this paper we demonstrate its use with specific examples that can be simulated using the web-browser interface.

  19. Atmospheric aerosols: Their Optical Properties and Effects (supplement)

    NASA Technical Reports Server (NTRS)

    1976-01-01

    A digest of technical papers is presented. Topics include aerosol size distribution from spectral attenuation with scattering measurements; comparison of extinction and backscattering coefficients for measured and analytic stratospheric aerosol size distributions; using hybrid methods to solve problems in radiative transfer and in multiple scattering; blue moon phenomena; absorption refractive index of aerosols in the Denver pollution cloud; a two dimensional stratospheric model of the dispersion of aerosols from the Fuego volcanic eruption; the variation of the aerosol volume to light scattering coefficient; spectrophone in situ measurements of the absorption of visible light by aerosols; a reassessment of the Krakatoa volcanic turbidity, and multiple scattering in the sky radiance.

  20. Validation of Retrieved Aerosol Optical Properties over Northeast Asia for Five Years from GOSAT TANSO-Cloud and Aerosol Imager

    NASA Astrophysics Data System (ADS)

    Kim, J.; Lee, S.; KIM, M.; Choi, M.; Go, S.; Lim, H.; Goo, T. Y.; Nakajima, T.; Kuze, A.; Shiomi, K.; Yokota, T.

    2015-12-01

    An aerosol retrieval algorithm was developed from Thermal And Near infrared Sensor for carbon Observation-Cloud and Aerosol Imager (TANSO-CAI) onboard the Greenhouse Gases Observing Satellite (GOSAT). The algorithm retrieves aerosol optical depth (AOD), size distribution of aerosol, and aerosol type in 0.1 degree grid resolution by look-up tables, which is used in retrieving optical properties of aerosol using inversion products from Aerosol Robotic NETwork (AERONET) sun-photometer observation. To improve the accuracy of aerosol algorithm, first, this algorithm considered the annually estimated radiometric degradation factor of TANSO-CAI suggested by Kuze et al. (2014). Second, surface reflectance was determined by two methods: one using the clear sky composite method from CAI measurements and the other the database from MODerate resolution Imaging Sensor (MODIS) surface reflectance data. At a given pixel, the surface reflectance is selected by using normalized difference vegetation index (NDVI) depending on season (Hsu et al., 2013). In this study, the retrieved AODs were compared with those of AERONET and MODIS dataset for different season over five years. Comparisons of AODs between AERONET and CAI show reasonable agreement with correlation coefficients of 0.65 ~ 0.97 and regression slopes between 0.7 and 1.2 for the whole period, depending on season and sites. Moreover, those between MODIS and CAI for the same period show agreements with correlation coefficients of 0.7 ~ 0.9 and regression slopes between 0.7 and 1.0, depending on season and regions. The results show reasonably good correlation, however, the largest error source in aerosol retrieval has been surface reflectance of TANSO-CAI due to its 3-days revisit orbit characteristics.

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

    NASA Astrophysics Data System (ADS)

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

    2003-11-01

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

  2. 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.

  3. X-Ray Microspectroscopic Investigations of Remote Aerosol Composition and Changes in Aerosol Microstructure and Phase State upon Hydration

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Artaxo, P.; Bechtel, M.; Förster, J. D.; Kilcoyne, A. L. D.; Krüger, M. L.; Pöhlker, C.; Saturno, J.; Weigand, M.; Wiedemann, K. T.

    2014-12-01

    Atmospheric aerosols play a crucial role in the Earth's climate system and hydrological cycle by scattering and absorbing sunlight and affecting the formation and development of clouds and precipitation. Our research focuses on aerosols in remote regions, in order to characterize the properties and sources of natural aerosol particles and the extent of human perturbations of the aerosol burden. The phase and mixing state of atmospheric aerosols, and particularly their hygroscopic response to relative humidity (RH) variations, is a central determinant of their atmospheric life cycle and impacts. We present an investigation using X-ray microspectroscopy on submicrometer aerosols under variable RH conditions, showing in situ changes in morphology, microstructure, and phase state upon humidity cycling. We applied Scanning Transmission X-ray Microscopy with Near-Edge X-ray Absorption Fine Structure spectroscopy (STXM-NEXAFS) under variable RH conditions to standard aerosols for a validation of the experimental approach and to internally mixed aerosol particles from the Amazonian rain forest collected during periods with anthropogenic pollution. The measurements were conducted at X-ray microscopes at the synchrotron facilities Advanced Light Source (ALS) in Berkeley, USA, and BESSY II in Berlin, Germany. Upon hydration, we observed substantial and reproducible changes in microstructure of the Amazonian particles (internal mixture of secondary organic material, ammoniated sulfate, and soot), which appear as mainly driven by efflorescence and recrystallization of sulfate salts. Multiple solid and liquid phases were found to coexist, especially in intermediate humidity regimes (60-80% RH). This shows that X-ray microspectroscopy under variable RH is a valuable technique to analyze the hygroscopic response of individual ambient aerosol particles. Our initial results underline that RH changes can trigger strong particle restructuring, in agreement with previous studies on

  4. Weekly periodicities of aerosol properties observed at an urban location in India

    SciTech Connect

    Satheesh, S K; Vinoj, V; Moorthy, K Krishna

    2011-07-01

    Multi-year (~7 years) observations of aerosol optical and microphysical properties were conducted at a tropical urban location in Bangalore, India. As a consequence of rapid urbanization, Bangalore presents high local atmospheric emissions, which makes it an interesting site to study the effect of anthropogenic activities on aerosol properties. It has been found that both column (aerosol optical depth, AOD) and ground-level measurements (black carbon (BC) and composite aerosol mass) exhibit a weekly cycle with low aerosol concentrations on weekends. In comparison to the weekdays, the weekend reductions of aerosol optical depth, black carbon and composite aerosol mass concentrations were ~15%, 25% and 24%, respectively. The magnitude of weekend reduction of black carbon is as much as ~1 μg m-3. The similarity in the weekly cycle between the column and surface measurements suggests that the aerosol column loading at this location is governed by local anthropogenic emissions. The strongest weekly cycle in composite aerosol mass concentration was observed in the super micron mass range (>1 μm). The weekly cycle of composite aerosol mass in the sub micron mass range (<1 μm) was weak in comparison to the super micron aerosol mass.

  5. Hygroscopicity Evaluation of Halide Scintillators

    SciTech Connect

    Zhuravleva, M; Stand, L; Wei, H; Hobbs, C. L.; Boatner, Lynn A; Ramey, Joanne Oxendine; Burger, Arnold; Rowe, E; Bhattacharya, P.; Tupitsyn, E; Melcher, Charles L

    2014-01-01

    A collaborative study of relative hygroscopicity of anhydrous halide scintillators grown at various laboratories is presented. We have developed a technique to evaluate moisture sensitivity of both raw materials and grown crystals, in which the moisture absorption rate is measured using a gravimetric analysis. Degradation of the scintillation performance was investigated by recording gamma-ray spectra and monitoring the photopeak position, count rate and energy resolution. The accompanying physical degradation of the samples exposed to ambient atmosphere was photographically recorded as well. The results were compared with ben

  6. The spatial-temporal variations in optical properties of atmosphere aerosols over China and its application in remote sensing

    NASA Astrophysics Data System (ADS)

    Chen, H.; Cheng, T.

    2013-12-01

    The atmospheric and climate response to the aerosol forcing are assessed by climate models regionally and globally under the past, present and future conditions. However, large uncertainties exist because of incomplete knowledge concerning the distribution and the physical and chemical properties of aerosols as well as aerosol-cloud interactions. Reduction in these uncertainties requires long-term monitoring of detailed properties of different aerosol types. China is one of the heavily polluted areas with high concentration of aerosols in the world. The complex source, composition of China aerosol led to the worse accuracy of aerosol radiative forcing assessment in the world, which urgently calls for improvements on the understanding of China regional aerosol properties. The spatial-temporal properties of aerosol types over China are studied using the radiance measurements and inversions data at 4 Aerosol Robotic Network (AERONET) stations. Five aerosol classes were identified including a coarse-size dominated aerosol type (presumably dust) and four fine-sized dominated aerosol types ranging from non-absorbing to highly absorbing fine aerosols. The mean optical properties of different aerosol types in China and their seasonal variations were also investigated. Based on the cluster analysis, the improved ground-based aerosol model is applied to the MODIS dark target inversion algorithm. Validation with MODIS official product and CE318 is also included.

  7. Aerosol properties from 4STAR observations: A sensitivity study

    NASA Astrophysics Data System (ADS)

    Kassianov, E.; Flynn, C.; Redemann, J.; Livingston, J. M.; Schmid, B.; Russell, P. B.; Sinyuk, A.

    2011-12-01

    Multi-spectral direct-beam observations of atmospheric aerosol and gas constituents have been taken successfully at a number of sites around the world by the airborne 14-Channel NASA Ames Airborne Tracking Sunphotometer (AATS-14). The recently developed airborne Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) is the next generation of AATS-14 with ultraviolet, visible and near-infrared spectral coverage, increased number of channels (more than 1500 pixels) and the sky-scanning ability of the ground-based AERONET sun/sky photometers. While it is generally agreed that more measurements in terms of independent wavelengths and scattering angles would offer enhanced aerosol retrievals, the potential afforded by improved observational capabilities of the 4STAR has not yet been fully characterized. This paper will attempt to place the importance of improved spectrally- and angularly-resolved 4STAR observations within the context of the well-known AERONET intensive-property retrieval. In particular, we have developed model data sets comparable to the 4STAR measurements of direct sun and sky radiances and evaluated the impact on the retrieval from subsampling in wavelength and scattering angle.

  8. Water nucleation properties of chaparral fire aerosol particles

    SciTech Connect

    Hudson, J.G.; Rogers, C.F.; Hallett, J.

    1989-05-01

    In December, 1986, planned and prescribed forest management burns took place at Lodi Canyon, on the north side of the Los Angeles Basin, California. These fires involved a mixture of species of small trees and shrubs, including scrub oak, chamise, and mountain mahogany, known collectively as ''chaparral'' in the Western US. Over a period of about two weeks, about 200 hectares of chaparral were consumed. This prescribed burn presented an opportunity for three days of airborne measurements of aerosol properties including total particle or condensation nuclei (CN) concentrations and cloud condensation nuclei (CCN) concentrations. This study is in coordination with other efforts conducted simultaneously; here the emphasis will be on the airborne CN and CCN measurements and on related studies conducted on a laboratory scale. In this study, we distinguish between CCN and the total aerosol particle population as gauged by the CN count. CCN and CN concentrations and CCN/CN ratios will be presented for the airborne measurements and for laboratory measurements employing a similar fuel. Ancillary ion chromatography (IC) and scanning electron microscopy (SEM) information will also be presented for the laboratory-scale chaparral burn. 11 refs., 4 figs., 4 tabs.

  9. Discernible signals of aerosol effects on the diurnal, weekly and decadal variations in thunderstorm activities

    NASA Astrophysics Data System (ADS)

    Li, Z.

    2015-12-01

    Aerosol can affect atmospheric convection, cloud and precipitation in a variety of means by altering energy balance at the surface and in the atmospheric column, and by altering cloud micro- and macro-physical properties. The effects are often contingent upon meteorological variables and aerosol properties. By reducing surface energy budget, aerosol tends to suppress convection, but aerosol-induced heating in the lower atmosphere can destabilize the upper atmosphere and strengthen convection. Aerosol-induced altering cloud microphysics may also suppress or invigorate cloud development pending on various factors. In this talk, I will illustrate how aerosols likely contribute to the thunderstorm variability on three distinct time scales from diurnal, weekly to decadal and how different types of aerosols and varying meteorological conditions may affect with the observed trends. I will first demonstrate the opposite effects of conservative scattering and hygroscopic aerosols versus absorbing and hydrophobic aerosol on the long-term trends of thunderstorms. I will then illustrate that aerosol can have a discernible effect on the weekly cycle of thunderstorms and there is the dependence of the phase of the weekly cycle on aerosol types. Last, I will show how aerosol delays the occurrence of thunderstorms. Of course, the plausible connections are subject to various uncertainties that should be tackled with more rigorous modeling and extensive observation studies.

  10. Background Southeast United States Aerosol Optical Properties and Their Dependence Upon Meteorology

    NASA Astrophysics Data System (ADS)

    Pawlyszyn, C.; West, M.; Sherman, J. P.; Link, M.; Zhou, Y.

    2015-12-01

    Aerosol effects on SE U.S. radiation budget are highly-seasonal. Aerosol loading is much higher in summer, due largely to high levels of biogenic secondary organic aerosol and sulfates. Aerosol loading is lowest in winter. Aerosol optical properties relevant to radiative forcing have been measured continuously at the Appalachian Atmospheric Interdisciplinary Research facility (AppalAIR) since the summer of 2009. AppalAIR is the only site in the eastern US to house co-located NOAA ESRL and NASA AeroNET instrumentation and is located in the mountains of Boone, NC. Lower tropospheric sub-micron (PM1) light scattering and absorption coefficients measured over seven summers and six winters are presented here, in addition to PM1 organic and sulfate aerosol mass concentrations measured during summers 2012-2013 as well as winter 2013. The objective is to determine the influence of aerosol sources and meteorology along the air mass back-trajectories on aerosol loading and composition. PM1 aerosol mass was dominated by organic aerosol and sulfate during the periods measured. Aerosol light scattering and organic aerosol concentrations were positively correlated during summer with temperature and solar flux along the parcel back-trajectory and negatively-correlated with rainfall along the back-trajectory. Wet deposition was a major factor in the difference between the upper and lower scattering coefficient quartiles for both summer and winter. Summer PM1 light scattering coefficient declined by approximately 30-40% since 2009, with smaller decreases during winter months. Long-term studies of aerosol optical properties from the regionally-representative AppalAIR site are necessary to determine the relationships between changing SE U.S. air quality and aerosol effects on regional climate and weather.

  11. Influences of external vs. core-shell mixing on aerosol optical properties at various relative humidities.

    PubMed

    Ramachandran, S; Srivastava, Rohit

    2013-05-01

    Aerosol optical properties of external and core-shell mixtures of aerosol species present in the atmosphere are calculated in this study for different relative humidities. Core-shell Mie calculations are performed using the values of radii, refractive indices and densities of aerosol species that act as core and shell, and the core-shell radius ratio. The single scattering albedo (SSA) is higher when the absorbing species (black carbon, BC) is the core, while for a sulfate core SSA does not vary significantly as the BC in the shell dominates the absorption. Absorption gets enhanced in core-shell mixing of absorbing and scattering aerosols when compared to their external mixture. Thus, SSA is significantly lower for a core-shell mixture than their external mixture. SSA is more sensitive to core-shell ratio than mode radius when BC is the core. The extinction coefficient, SSA and asymmetry parameter are higher for external mixing when compared to BC (core)-water soluble aerosol (shell), and water soluble aerosol (core)-BC (shell) mixtures in the relative humidity range of 0 to 90%. Spectral SSA exhibits the behaviour of the species which acts as a shell in core-shell mixing. The asymmetry parameter for an external mixture of water soluble aerosol and BC is higher than BC (core)-water soluble aerosol (shell) mixing and increases as function of relative humidity. The asymmetry parameter for the water soluble aerosol (core)-BC (shell) is independent of relative humidity as BC is hydrophobic. The asymmetry parameter of the core-shell mixture decreases when BC aerosols are involved in mixing, as the asymmetry parameter of BC is lower. Aerosol optical depth (AOD) of core-shell mixtures increases at a higher rate when the relative humidity exceeds 70% in continental clean and urban aerosol models, whereas AOD remains the same when the relative humidity exceeds 50% in maritime aerosol models. The SSA for continental aerosols varies for core-shell mixing of water soluble

  12. Stratospheric aerosol properties and their effects on infrared radiation.

    NASA Technical Reports Server (NTRS)

    Remsberg, E. E.

    1973-01-01

    This paper presents a stratospheric aerosol model and infers its effects on terrestrial radiation. Composition of the aerosol is assumed to be concentrated sulfuric acid. An appropriate size distribution has been determined from available size distribution measurements of other investigators. Aerosols composed of concentrated sulfuric acid emit energy in the atmospheric window region of the infrared spectrum, 8-13 microns. Laboratory measurements of optical constant data obtained at room temperature are presented for 75 and 90% aqueous sulfuric acid. Calculations of an aerosol extinction coefficient are then performed by using the above data. Effects of changes in aerosol phase and temperature are discussed but not resolved.

  13. Cloud Nucleating Properties of Aerosols During TexAQS - GoMACCS 2006: Influence of Aerosol Sources, Composition, and Size

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.; Onasch, T. B.; Alllan, J. D.; Worsnop, D.

    2006-12-01

    TexAQS - GoMACCS 2006 was conducted from July to September 2006 in the Gulf of Mexico and Houston Ship Channel to investigate sources and processing of gas and particulate phase species and to determine their impact on regional air quality and climate. As part of the experiment, the NOAA R.V. Ronald H. Brown transited from Charleston, S.C. to the study region. The ship was equipped with a full compliment of gas and aerosol instruments. To determine the cloud nucleating properties of aerosols, measurements were made of the aerosol number size distribution, aerosol chemical composition, and cloud condensation nuclei (CCN) concentration at five supersaturations. During the transit and over the course of the experiment, a wide range of aerosol sources and types was encountered. These included urban and industrial emissions from the S.E. U.S. as the ship left Charleston, a mixture of Saharan dust and marine aerosol during the transit around Florida and across the Gulf of Mexico, urban emissions from Houston, and emissions from the petrochemical industries, oil platforms, and marine vessels in the Gulf coast region. Highest activation ratios (ratio of CCN to total particle number concentration at 0.4 percent supersaturation) were measured in anthropogenic air masses when the aerosol was composed primarily of ammonium sulfate salts and in marine air masses with an aerosol composed of sulfate and sea salt. A strong gradient in activation ratio was measured as the ship moved from the Gulf of Mexico to the end of the Houston Ship Channel (values decreasing from about 0.8 to less than 0.1) and the aerosol changed from marine to industrial. The activation ratio under these different regimes in addition to downwind of marine vessels and oil platforms will be discussed in the context of the aerosol size distribution and chemical composition. The discussion of composition will include the organic mass fraction of the aerosol, the degree of oxidation of the organics, and the water

  14. Simultaneous Retrieval of Aerosol and Cloud Properties During the MILAGRO Field Campaign

    NASA Technical Reports Server (NTRS)

    Knobelspiesse, K.; Cairns, B.; Redemann, J.; Bergstrom, R. W.; Stohl, A.

    2011-01-01

    Estimation of Direct Climate Forcing (DCF) due to aerosols in cloudy areas has historically been a difficult task, mainly because of a lack of appropriate measurements. Recently, passive remote sensing instruments have been developed that have the potential to retrieve both cloud and aerosol properties using polarimetric, multiple view angle, and multi spectral observations, and therefore determine DCF from aerosols above clouds. One such instrument is the Research Scanning Polarimeter (RSP), an airborne prototype of a sensor on the NASA Glory satellite, which unfortunately failed to reach orbit during its launch in March of 2011. In the spring of 2006, the RSP was deployed on an aircraft based in Veracruz, Mexico, as part of the Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign. On 13 March, the RSP over flew an aerosol layer lofted above a low altitude marine stratocumulus cloud close to shore in the Gulf of Mexico. We investigate the feasibility of retrieving aerosol properties over clouds using these data. Our approach is to first determine cloud droplet size distribution using the angular location of the cloud bow and other features in the polarized reflectance. The selected cloud was then used in a multiple scattering radiative transfer model optimization to determine the aerosol optical properties and fine tune the cloud size distribution. In this scene, we were able to retrieve aerosol optical depth, the fine mode aerosol size distribution parameters and the cloud droplet size distribution parameters to a degree of accuracy required for climate modeling. This required assumptions about the aerosol vertical distribution and the optical properties of the coarse aerosol size mode. A sensitivity study was also performed to place this study in the context of future systematic scanning polarimeter observations, which found that the aerosol complex refractive index can also be observed accurately if the aerosol optical depth is

  15. Understanding the contributions of aerosol properties and parameterization discrepancies to droplet number variability in a global climate model

    NASA Astrophysics Data System (ADS)

    Morales Betancourt, R.; Nenes, A.

    2014-05-01

    Aerosol indirect effects in climate models strongly depend on the representation of the aerosol activation process. In this study, we assess the process-level differences across activation parameterizations that contribute to droplet number uncertainty by using the adjoints of the Abdul-Razzak and Ghan (2000) and Fountoukis and Nenes (2005) droplet activation parameterizations in the framework of the Community Atmospheric Model version 5.1 (CAM5.1). The adjoint sensitivities of Nd to relevant input parameters are used to (i) unravel the spatially resolved contribution of aerosol number, mass, and chemical composition to changes in Nd between present-day and pre-industrial simulations and (ii) identify the key variables responsible for the differences in Nd fields and aerosol indirect effect estimates when different activation schemes are used within the same modeling framework. The sensitivities are computed online at minimal computational cost. Changes in aerosol number and aerosol mass concentrations were found to contribute to Nd differences much more strongly than chemical composition effects. The main sources of discrepancy between the activation parameterizations considered were the treatment of the water uptake by coarse mode particles, and the sensitivity of the parameterized Nd accumulation mode aerosol geometric mean diameter. These two factors explain the different predictions of Nd over land and over oceans when these parameterizations are employed. Discrepancies in the sensitivity to aerosol size are responsible for an exaggerated response to aerosol volume changes over heavily polluted regions. Because these regions are collocated with areas of deep clouds, their impact on shortwave cloud forcing is amplified through liquid water path changes. The same framework is also utilized to efficiently explore droplet number uncertainty attributable to hygroscopicity parameter of organic aerosol (primary and secondary). Comparisons between the parameterization

  16. Implementation of the Missing Aerosol Physics into LLNL IMPACT

    SciTech Connect

    Chuang, C

    2005-02-09

    In recent assessments of climate forcing, the Intergovernmental Panel on Climate Change lists aerosol as one o f the most important anthropogenic agents that influence climate. Atmospheric aerosols directly affect the radiative fluxes at the surface and top of the Earth's atmosphere by scattering and/or absorbing radiation. Further, aerosols indirectly change cloud microphysical properties (such as cloud drop effective radius) that also affect the radiative fluxes. However, the estimate of the magnitude of aerosol climatic effect varies widely, and aerosol/cloud interactions remain one of the most uncertain aspects of climate models today. The Atmospheric Sciences Division has formulated a plan to enhance and expand our modeling expertise in aerosol/cloud/climate interactions. Under previous LDRD support, we successfully developed a computationally efficient version of IMPACT to simulate aerosol climatology. This new version contains a compact chemical mechanism for the prediction of sulfate and also predicts the distributions of organic carbon (OC), black carbon (BC), dust, and sea salt. Furthermore, we implemented a radiation package into IMPACT to calculate the radiative forcing and heating/cooling rates by aerosols. This accomplishment built the foundation of our currently funded projects under the NASA Global Modeling and Analysis Program as well as the DOE Atmospheric Radiation Program. Despite the fact that our research is being recognized as an important effort to quantify the effects of anthropogenic aerosols on climate, the major shortcoming of our previous simulations on aerosol climatic effects is the over simplification of spatial and temporal variations of aerosol size distributions that are shaped by complicated nucleation, growth, transport and removal processes. Virtually all properties of atmospheric aerosols and clouds depend strongly on aerosol size distribution. Moreover, molecular processing on aerosol surfaces alters the hygroscopic

  17. Aerosol particle properties in a South American megacity

    NASA Astrophysics Data System (ADS)

    Ulke, Ana; Torres-Brizuela, Marcela; Raga, Graciela; Baumgardner, Darrel; Cancelada, Marcela

    2015-04-01

    The subtropical city of Buenos Aires is located on the western shore of Río de la Plata, on the southeastern coast of Argentina. It is the second largest metropolitan area in South America, with a population density of around 14 thousand people per km2. When all 24 counties of the Great Buenos Aires Metropolitan Area are included it is the third-largest conurbation in Latin America, with a population of around fifteen million inhabitants. The generalized worldwide trend to concentrate human activities in urban regions that continue to expand in area, threatens the local and regional environment. Air pollution in the Buenos Aires airshed is due to local sources (mainly the mobile sources, followed by the electric power plants and some industries) and to distant sources (like biomass burning, dust, marine aerosols and occasionally volcanic ash) whose products arrive in the city area due to the regional transport patterns. Previous research suggests that ambient aerosol particle concentrations should be considered an air quality problem. A field campaign was conducted in Buenos Aires in 2011 in order to characterize some aerosol particles properties measured for the first time in the city. Measurements began in mid- April and continued until December. The field observations were done in a collaborative effort between the Universities of Mexico (UNAM) and Buenos Aires (UBA). A suite of instruments was installed on the roof of an UBA laboratory and classroom buildings (34.54° S, 58.44° W) at an altitude of approximately 30 m above sea level. The measurements included the number concentration of condensation nuclei (CN) larger than approximately 50 nm, the mass concentration of particle-bound polycyclic aromatic hydrocarbons (PPAH), the scattering (Bscat) and absorption (Babs) coefficients at 550 nm and the vertical profiles of backscattered light from aerosols at a wavelength of 910 nm using a ceilometer. In addition, a weather station recorded the meteorological

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

    NASA Astrophysics Data System (ADS)

    Carlton, A. G.; Ervens, B.

    2011-12-01

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

  19. Aerosol Characterization and New Instrumentation for Better Understanding Snow Radiative Properties

    NASA Astrophysics Data System (ADS)

    Beres, N. D.

    2015-12-01

    Snow albedo is determined by snowpack thickness and grain size, but also affected by contamination with light-absorbing, microscopic (e.g., mineral dust, combustion aerosols, bio-aerosols) and macroscopic (e.g., microalgae, plant debris, sand, organisms) compounds. Most currently available instruments for measuring snow albedo utilize the natural, downward flux of solar radiation and the reflected upward flux. This reliance on solar radiation (and, thus, large zenith angles and clear-sky conditions) leads to severe constraints, preventing characterization of detailed diurnal snow albedo cycles. Here, we describe instrumentation and methodologies to address these limitations with the development and deployment of new snow radiation sensors for measuring surface spectral and in-snow radiative properties. This novel instrumentation will be tested at the CRREL/UCSB Eastern Sierra (CUES) Snow Study Site at Mammoth Mountain, which is extensively instrumented for characterizing snow properties including snow albedo and surface morphology. However, it has been lacking instrumentation for the characterization of aerosols that can be deposited on the snow surface through dry and wet deposition. Currently, we are installing aerosol instrumentation at the CUES site, which are also described. This includes instruments for the multi-wavelength measurement of aerosol scattering and absorption coefficients and for the characterization of aerosol size distribution. Knowledge of aerosol concentration and physical and optical properties will allow for the study of aerosol deposition and modification of snow albedo and for establishing an aerosol climatology for the CUES site.

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

    NASA Technical Reports Server (NTRS)

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

    2004-01-01

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

  1. A comprehensive climatology of Arctic aerosol properties on the North Slope of Alaska

    NASA Astrophysics Data System (ADS)

    Creamean, Jessie; de Boer, Gijs; Shupe, Matthew; McComiskey, Allison

    2016-04-01

    Evaluating aerosol properties has implications for the formation of Arctic clouds, resulting in impacts on cloud lifetime, precipitation processes, and radiative forcing. There are many remaining uncertainties and large discrepancies regarding modeled and observed Arctic aerosol properties, illustrating the need for more detailed observations to improve simulations of Arctic aerosol and more generally, projections of the components of the aerosol-driven processes that impact sea ice loss/gain. In particular, the sources and climatic effects of Arctic aerosol particles are severely understudied. Here, we present a comprehensive, long-term record of aerosol observations from the North Slope of Alaska baseline site at Barrow. These measurements include sub- and supermicron (up to 10 μm) total mass and number concentrations, sub- and supermicron soluble inorganic and organic ion concentrations, submicron metal concentrations, submicron particle size distributions, and sub- and supermicron absorption and scattering properties. Aerosol extinction and number concentration measurements extend back to 1976, while the remaining measurements were implemented since. Corroboration between the chemical, physical, and optical property measurements is evident during periods of overlapping observations, demonstrating the reliability of the measurements. During the Arctic Haze in the winter/spring, high concentrations of long-range transported submicron sea salt, mineral dust, industrial metals, pollution (non-sea salt sulfate, nitrate, ammonium), and biomass burning species are observed concurrent with higher concentrations of particles with sizes that span the submicron range, enhanced absorption and scattering coefficients, and largest Ångström exponents. The summer is characterized by high concentrations of small biogenic aerosols (< 100 nm) and low extinction coefficients. Fall is characterized by clean conditions, with supermicron sea salt representing the dominant aerosol

  2. Characterization of Spectral Absorption Properties of Aerosols Using Satellite Observations

    NASA Technical Reports Server (NTRS)

    Torres, O.; Jethva, H.; Bhartia, P. K.; Ahn, C.

    2012-01-01

    The wavelength-dependence of aerosol absorption optical depth (AAOD) is generally represented in terms of the Angstrom Absorption Exponent (AAE), a parameter that describes the dependence of AAOD with wavelength. The AAE parameter is closely related to aerosol composition. Black carbon (BC) containing aerosols yield AAE values near unity whereas Organic carbon (OC) aerosol particles are associated with values larger than 2. Even larger AAE values have been reported for desert dust aerosol particles. Knowledge of spectral AAOD is necessary for the calculation of direct radiative forcing effect of aerosols and for inferring aerosol composition. We have developed a satellitebased method of determining the spectral AAOD of absorbing aerosols. The technique uses high spectral resolution measurements of upwelling radiation from scenes where absorbing aerosols lie above clouds as indicated by the UV Aerosol Index. For those conditions, the satellite measured reflectance (rho lambda) is approximately given by Beer's law rho lambda = rho (sub 0 lambda) e (exp -mtau (sub abs lambda)) where rho(sub 0 lambda) is the cloud reflectance, m is the geometric slant path and tau (sub abs lambda) is the spectral AAOD. The rho (sub 0 lambda) term is determined by means of radiative transfer calculations using as input the cloud optical depth derived as described in Torres et al. [JAS, 2012] that accounts for the effects of aerosol absorption. In the second step, corrections for molecular and aerosol scattering effects are applied to the cloud reflectance term, and the spectral AAOD is then derived by inverting the equation above. The proposed technique will be discussed in detail and application results will be presented. The technique can be easily applied to hyper-spectral satellite measurements that include UV such as OMI, GOME and SCIAMACHY, or to multi-spectral visible measurements by other sensors provided that the aerosol-above-cloud events are easily identified.

  3. On the Water Uptake and CCN Activation of Tropospheric Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Rastak, Narges; Pajunoja, Aki; Acosta Navarro, Juan-Camilo; Leong, Yu Jun; Cerully, Kate M.; Nenes, Athanasios; Kirkevåg, Alf; Topping, David; Virtanen, Annele; Riipinen, Ilona

    2016-04-01

    Aerosol particles introduce high uncertainties to radiative climate forcing. If exposed to a given relative humidity (RH), aerosol particles containing soluble material can absorb water and grow in size (hygroscopic growth). If RH is increased further beyond supersaturation (RH >100%) the particles can act as cloud condensation nuclei (CCN). Aerosol particles interactions with water vapour determine to a large extent their influence on climate. Organic aerosols (OA) contribute a large fraction (20-90%) of atmospheric submicron particulate mass, on the other hand they often consist of thousands of compounds with different properties. One of these properties is solubility, which affects the hygroscopic growth and cloud condensation nucleus (CCN) activation of the organic particles. We investigate the hygroscopic behaviour of complex organic aerosols accounting for the distribution of solubilities present in these mixtures. We use the SPARC method to estimate the solubility distributions of isoprene (IP) and monoterpene (MT) SOA based on their chemical composition, as predicted by the Master Chemical Mechanism (MCM). Combining these solubility distributions with the adsorption theory along with the non-ideal behaviour of organic mixtures, we predict the expected hygroscopic growth factors (HGFs), CCN activation behaviour and the related hygroscopicity parameters kappa for these mixtures. The predictions are compared to laboratory measurements as well as field data from MT- and IP-dominated measurement sites. The predicted solubility distributions do a good job in explaining the water uptake of these two mixture types at high relative humidities (RH around 90%), as well as their CCN activation - including the potential differences between the kappa values derived from HGF vs. CCN data. At lower relative humidities, however, the observed water uptake is higher than predicted on solubility alone, particularly for the MT-derived SOA. The data from the low RHs are further

  4. Vertical distribution of aerosol optical properties based on aircraft measurements over the Loess Plateau in China.

    PubMed

    Li, Junxia; Liu, Xingang; Yuan, Liang; Yin, Yan; Li, Zhanqing; Li, Peiren; Ren, Gang; Jin, Lijun; Li, Runjun; Dong, Zipeng; Li, Yiyu; Yang, Junmei

    2015-08-01

    Vertical distributions of aerosol optical properties based on aircraft measurements over the Loess Plateau were measured for the first time during a summertime aircraft campaign, 2013 in Shanxi, China. Data from four flights were analyzed. The vertical distributions of aerosol optical properties including aerosol scattering coefficients (σsc), absorption coefficients (σab), Angström exponent (α), single scattering albedo (ω), backscattering ratio (βsc), aerosol mass scattering proficiency (Qsc) and aerosol surface scattering proficiency (Qsc(')) were obtained. The mean statistical values of σsc were 77.45 Mm(-1) (at 450 nm), 50.72 Mm(-1) (at 550n m), and 32.02 Mm(-1) (at 700 nm). The mean value of σab was 7.62 Mm(-1) (at 550 nm). The mean values of α, βsc and ω were 1.93, 0.15, and 0.91, respectively. Aerosol concentration decreased with altitude. Most effective diameters (ED) of aerosols were less than 0.8 μm. The vertical profiles of σsc,, α, βsc, Qsc and Qsc(') showed that the aerosol scattering properties at lower levels contributed the most to the total aerosol radiative forcing. Both α and βsc had relatively large values, suggesting that most aerosols in the observational region were small particles. The mean values of σsc, α, βsc, Qsc, Qsc('), σab and ω at different height ranges showed that most of the parameters decreased with altitude. The forty-eight hour backward trajectories of air masses during the observation days indicated that the majority of aerosols in the lower level contributed the most to the total aerosol loading, and most of these particles originated from local or regional pollution emissions.

  5. Optical properties and radiative forcing of urban aerosols in Nanjing, China

    NASA Astrophysics Data System (ADS)

    Zhuang, B. L.; Wang, T. J.; Li, S.; Liu, J.; Talbot, R.; Mao, H. T.; Yang, X. Q.; Fu, C. B.; Yin, C. Q.; Zhu, J. L.; Che, H. Z.; Zhang, X. Y.

    2014-02-01

    Continuous measurements of atmospheric aerosols were made in Nanjing, a megacity in China, from 18 January to 18 April, 2011 (Phase 1) and from 22 April 2011 to 21 April 2012 (Phase 2). Aerosol characteristics, optical properties, and direct radiative forcing (DRF) were studied through interpretations of these measurements. We found that during Phase 1, mean PM2.5, black carbon (BC), and aerosol scattering coefficient (Bsp) in Nanjing were 76.1 ± 59.3 μg m-3, 4.1 ± 2.2 μg m-3, and 170.9 ± 105.8 M m-1, respectively. High pollution episodes occurred during Spring and Lantern Festivals when hourly PM2.5 concentrations reached 440 μg m-3, possibly due to significant discharge of fireworks. Temporal variations of PM2.5, BC, and Bsp were similar to each other. It is estimated that inorganic scattering aerosols account for about 49 ± 8.6% of total aerosols while BC only accounted for 6.6 ± 2.9%, and nitrate was larger than sulfate. In Phase 2, optical properties of aerosols show great seasonality. High relative humidity (RH) in summer (June, July, August) likely attributed to large optical depth (AOD) and small Angstrom exponent (AE) of aerosols. Due to dust storms, AE of total aerosols was the smallest in spring (March, April, May). Annual mean 550-nm AOD and 675/440-nm AE were 0.6 ± 0.3 and 1.25 ± 0.29 for total aerosols, 0.04 ± 0.02 and 1.44 ± 0.50 for absorbing aerosols, 0.48 ± 0.29 and 1.64 ± 0.29 for fine aerosols, respectively. Annual single scattering albedo of aerosols ranged from 0.90 to 0.92. Real time wavelength-dependent surface albedo from the Moderate Resolution Imaging Spectroradiometer (MODIS) was used to assess aerosol DRFs. Both total and absorbing aerosol DRFs had significant seasonal variations in Nanjing and they were the strongest in summer. Annual mean clear sky TOA DRF (including daytime and nighttime) of total and absorbing aerosols was about -6.9 and +4.5 W m-2, respectively. Aerosol DRFs were found to be sensitive to surface

  6. An Analysis of AERONET Aerosol Absorption Properties and Classifications Representative of Aerosol Source Regions

    NASA Technical Reports Server (NTRS)

    Giles, David M.; Holben, Brent N.; Eck, Thomas F.; Sinyuk, Aliaksandr; Smirnov, Alexander; Slutsker, Ilya; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

    2012-01-01

    Partitioning of mineral dust, pollution, smoke, and mixtures using remote sensing techniques can help improve accuracy of satellite retrievals and assessments of the aerosol radiative impact on climate. Spectral aerosol optical depth (tau) and single scattering albedo (omega (sub 0) ) from Aerosol Robotic Network (AERONET) measurements are used to form absorption [i.e., omega (sub 0) and absorption Angstrom exponent (alpha(sub abs))] and size [i.e., extinction Angstrom exponent (alpha(sub ext)) and fine mode fraction of tau] relationships to infer dominant aerosol types. Using the long-term AERONET data set (1999-2010), 19 sites are grouped by aerosol type based on known source regions to: (1) determine the average omega (sub 0) and alpha(sub abs) at each site (expanding upon previous work); (2) perform a sensitivity study on alpha(sub abs) by varying the spectral omega (sub 0); and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral omega (sub 0) averages indicate slightly more aerosol absorption (i.e., a 0.0 < delta omega (sub 0) <= 0.02 decrease) than in previous work and optical mixtures of pollution and smoke with dust show stronger absorption than dust alone. Frequency distributions of alpha(sub abs) show significant overlap among aerosol type categories and at least 10% of the alpha(sub abs) retrievals in each category are below 1.0. Perturbing the spectral omega (sub 0) by +/- 0.03 induces significant alpha(sub abs) changes from the unperturbed value by at least approx. +/- 0.6 for Dust, approx. +/-0.2 for Mixed, and approx. +/-0.1 for Urban/Industrial and Biomass Burning. The omega (sub 0)440nm and alpha(sub ext) 440-870nm relationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

  7. Quantitative retrieval of aerosol optical properties by means of ceilometers

    NASA Astrophysics Data System (ADS)

    Wiegner, Matthias; Gasteiger, Josef; Geiß, Alexander

    2016-04-01

    In the last few years extended networks of ceilometers have been established by several national weather services. Based on improvements of the hardware performance of these single-wavelength backscatter lidars and their 24/7 availability they are increasingly used to monitor mixing layer heights and to derive profiles of the particle backscatter profile. As a consequence they are used for a wide range of applications including the dispersion of volcanic ash plumes, validation of chemistry transport models and air quality studies. In this context the development of automated schemes to detect aerosol layers and to identify the mixing layer are essential, in particular as the latter is often used as a proxy for air quality. Of equal importance is the calibration of ceilometer signals as a pre-requisite to derive quantitative optical properties. Recently, it has been emphasized that the majority of ceilometers are influenced by water vapor absorption as they operate in the spectral range of 905 - 910 nm. If this effect is ignored, errors of the aerosol backscatter coefficient can be as large as 50%, depending on the atmospheric water vapor content and the emitted wavelength spectrum. As a consequence, any other derived quantity, e.g. the extinction coefficient or mass concentration, would suffer from a significant uncertainty in addition to the inherent errors of the inversion of the lidar equation itself. This can be crucial when ceilometer derived profiles shall be used to validate transport models. In this presentation, the methodology proposed by Wiegner and Gasteiger (2015) to correct for water vapor absorption is introduced and discussed.

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

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

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

  9. Retrieval of Aerosol Absorption Properties from Satellite Observations

    NASA Technical Reports Server (NTRS)

    Torres, Omar; Bhartia, Pawan K.; Jethva, H.; Ahn, Chang-Woo

    2012-01-01

    The Angstrom Absorption Exponent (AAE) is a parameter commonly used to characterize the wavelength-dependence of aerosol absorption optical depth (AAOD). It is closely related to aerosol composition. Black carbon (BC) containing aerosols yield AAE values near unity whereas Organic carbon (OC) aerosol particles are associated with values larger than 2. Even larger AAE values have been reported for desert dust aerosol particles. Knowledge of spectral AAOD is necessary for the calculation of direct radiative forcing effect of aerosols and for inferring aerosol composition. We have developed a satellitebased method of determining the spectral AAOD of absorbing aerosols. The technique uses multi-spectral measurements of upwelling radiation from scenes where absorbing aerosols lie above clouds as indicated by the UV Aerosol Index. For those conditions, the satellite measurement can be explained, using an approximations of Beer's Law (BL), as the upwelling reflectance at the cloud top attenuated by the absorption effects of the overlying aerosol layer. The upwelling reflectance at the cloud-top in an aerosol-free atmospheric column is mainly a function of cloud optical depth (COD). In the proposed method of AAE derivation, the first step is determining COD which is retrieved using a previously developed color-ratio based approach. In the second step, corrections for molecular scattering effects are applied to both the observed ad the calculated cloud reflectance terms, and the spectral AAOD is then derived by an inversion of the BL approximation. The proposed technique will be discussed in detail and application results making use of OMI multi-spectral measurements in the UV-Vis. will be presented.

  10. The effects of hygroscopicity of fossil fuel BC on mixed-phase and cirrus ice clouds

    NASA Astrophysics Data System (ADS)

    Yun, Y.; Penner, J. E.

    2010-12-01

    Fossil fuel burning BC aerosols are often emitted together with sulfate, which coats the surface of these BC particles and changes their hygroscopicity. The ice forming capability of the fossil fuel burning BC can differ widely as a result of the amount of soluble coating on their surface. Due to the abundance of fossil fuel burning BC particles, a small change in their activated fraction can produce a large difference in their climate forcing. To better quantify the role of fossil fuel burning BC in climate change, a 3-BC (hydrophobic, hydrophilic and hygroscopic BC) scheme is developed to replace the 1-BC scheme in a coupled climate and aerosol transport model (CAM-IMPACT). The new scheme explicitly calculates the condensation and coagulation of sulfate on BC particles and keeps track of their coating in the 3-BC states. The hygroscopicity of BC is determined by the layers of sulfate coating on their surface according to criteria developed in laboratory observations. The ice formation scheme in mixed-phase and cirrus clouds is also updated to treat the 3 hygroscopicity BC groups separately according to their different ice freezing capabilities. This paper will report the climate forcing associated with the new BC scheme as well as comparison with observations.

  11. Baseline Maritime Aerosol: Methodology to Derive the Optical Thickness and Scattering Properties

    NASA Technical Reports Server (NTRS)

    Kaufman, Yoram J.; Smirnov, Alexander; Holben, Brent N.; Dubovik, Oleg; Einaudi, Franco (Technical Monitor)

    2001-01-01

    Satellite Measurements of the global distribution of aerosol and their effect on climate should be viewed in respect to a baseline aerosol. In this concept, concentration of fine mode aerosol particles is elevated above the baseline by man-made activities (smoke or urban pollution), while coarse mode by natural processes (e.g. dust or sea-spray). Using 1-3 years of measurements in 10 stations of the Aerosol Robotic network (ACRONET we develop a methodology and derive the optical thickness and properties of this baseline aerosol for the Pacific and Atlantic Oceans. Defined as the median for periods of stable optical thickness (standard deviation < 0.02) during 2-6 days, the median baseline aerosol optical thickness over the Pacific Ocean is 0.052 at 500 am with Angstrom exponent of 0.77, and 0.071 and 1.1 respectively, over the Atlantic Ocean.

  12. Analysis of aerosol properties derived from sun photometer and lidar over Dunhuang radiometric calibration site

    NASA Astrophysics Data System (ADS)

    Chen, Lin; Jing, Yingying; Zhang, Peng; Hu, Xiuqing

    2016-05-01

    Duhuang site has been selected as China Radiation Calibration Site (CRCS) for Remote Sensing Satellite Sensors since 1996. With the economic development of Dunhuang city, the ambient of the radiation calibration field has changed in recent years. Taking into account the key role of aerosol in radiometric calibration, it is essential to investigate the aerosol optical properties over Dunhuang radiometric calibration site. In this paper, the CIMEL sun photometer (CE-318) and Mie-scattering Lidar are simultaneously used to measure aerosol optical properties in Dunhuang site. Data from aerosol-bands of sun photometer are used in a Langley method to determine spectral optical depths of aerosol. And Lidar is utilized to obtain information of vertical profile and integrated aerosol optical depths at different heights. The results showed that the aerosol optical depth at 500 nm wavelength during the in-situ measurement campaigns varied from 0.1 to 0.3 in Dunhuang site. And the observation results also indicated that high aerosol concentration layer mostly located at the height of about 2~4 km. These results implies that the aerosol concentration of atmosphere in Dunhuang was relatively small and suitable for in-flight calibration for remote sensing satellite sensors.

  13. North Atlantic Aerosol Properties and Direct Radiative Effects: Key Results from TARFOX and ACE-2

    NASA Technical Reports Server (NTRS)

    Russell, P. B.; Livingston, J. M.; Schmid, B.; Bergstrom, R. A.; Hignett, P.; Hobbs, P. V.; Durkee, P. A.; Condon, Estelle (Technical Monitor)

    1998-01-01

    Aerosol effects on atmospheric radiative fluxes provide a forcing function that can change the climate in potentially significant ways. This aerosol radiative Forcing is a major source of uncertainty in understanding the observed climate change of the past century and in predicting, future climate. To help reduce this uncertainty, the International Global Atmospheric Chemistry Project (IGAC) has endorsed a series of multiplatform aerosol field campaigns. The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the second Aerosol Characterization Experiment (ACE-2) were the first IGAC campaigns to address the impact of anthropogenic aerosols. Both TARFOX and ACE-2 gathered extensive data sets on aerosol properties and radiative effects. TARFOX focused on the urban-industrial haze plume flowing from the eastern United States over the western Atlantic Ocean, whereas ACE-2 studied aerosols carried over the eastern Atlantic from both European urban/industrial and African mineral sources. These aerosols often have a marked influence on the top-of-atmosphere radiances measured by satellites, as illustrated in Figure 1. Shown there are contours of aerosol optical depth derived from radiances measured by the AVHRR sensor on the NOAA-11 satellite. The contours readily show that aerosols originating in North America, Europe, and Africa impact the radiative properties of air over the North Atlantic. However, the accurate derivation of flux chances, or radiative forcing, from the satellite-measured radiances or 'etrieved optical depths remains a difficult challenge. In this paper we summarize key Initial results from TARFOX and, to a lesser extent ACE-2, with a focus on those results that allow an improved assessment of the flux changes caused by North Atlantic aerosols at middle and high latitudes.

  14. North Atlantic Aerosol Properties and Direct Radiative Effects: Key Results from TARFOX and ACE-2

    NASA Technical Reports Server (NTRS)

    Russell, P. B.; Livingston, J. M.; Schmid, B.; Bergstrom, Robert A.; Hignett, P.; Hobbs, P. V.; Durkee, P. A.

    2000-01-01

    Aerosol effects on atmospheric radiative fluxes provide a forcing function that can change the climate In potentially significant ways. This aerosol radiative forcing is a major source of uncertainty in understanding the observed climate change of the past century and in predicting future climate. To help reduce this uncertainty, the International Global Atmospheric Chemistry Project (IGAC) has endorsed a series of multiplatform aerosol field campaigns. The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the second Aerosol Characterization Experiment (ACE-2) were the first IGAC campaigns to address the impact of anthropogenic aerosols, Both TARFOX and ACE-2 gathered extensive data sets on aerosol properties and radiative effects, TARFOX focused on the urban-industrial haze plume flowing from the eastern United States over the western Atlantic Ocean, whereas ACE-2 studied aerosols carried over the eastern Atlantic from both European urban/industrial and African mineral sources. These aerosols often have a marked influence on the top-of-atmosphere radiances measured by satellites. Shown there are contours of aerosol optical depth derived from radiances measured by the AVHRR sensor on the NOAA-11 satellite. The contours readily show that aerosols originating in North America, Europe, and Africa impact the radiative properties of air over the North Atlantic. However, the accurate derivation of flux changes, or radiative forcing, from the satellite measured radiances or retrieved optical depths remains a difficult challenge. In this paper we summarize key initial results from TARFOX and, to a lesser extent, ACE-2, with a focus on those results that allow an improved assessment of the flux changes caused by North Atlantic aerosols at middle latitudes.

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

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

    SciTech Connect

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

    2001-04-01

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

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

    PubMed

    Yuan, Liang; Yin, Yan; Xiao, Hui; Yu, Xing