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Sample records for activated aerosol particles

  1. Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

    2016-04-01

    Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more

  2. Apparatus having reduced background for measuring radiation activity in aerosol particles

    DOEpatents

    Rodgers, John C.; McFarland, Andrew R.; Oritz, Carlos A.; Marlow, William H.

    1992-01-01

    Apparatus having reduced background for measuring radiation activity in aerosol particles. A continuous air monitoring sampler is described for use in detecting the presence of alpha-emitting aerosol particles. An inlet fractionating screen has been demonstrated to remove about 95% of freshly formed radon progeny from the aerosol sample, and approximately 33% of partially aged progeny. Addition of an electrical condenser and a modified dichotomous virtual impactor are expected to produce considerable improvement in these numbers, the goal being to enrich the transuranic (TRU) fraction of the aerosols. This offers the possibility of improving the signal-to-noise ratio for the detected alpha-particle energy spectrum in the region of interest for detecting TRU materials associated with aerosols, thereby enhancing the performance of background-compensation algorithms for improving the quality of alarm signals intended to warn personnel of potentially harmful quantities of TRU materials in the ambient air.

  3. The effect of phase partitioning of semivolatile compounds on the measured CCN activity of aerosol particles

    NASA Astrophysics Data System (ADS)

    Romakkaniemi, S.; Jaatinen, A.; Laaksonen, A.; Nenes, A.; Raatikainen, T.

    2013-09-01

    The effect of inorganic semivolatile aerosol compounds on the CCN activity of aerosol particles was studied by using a computational model for a DMT-CCN counter, a cloud parcel model for condensation kinetics and experiments to quantify the modelled results. Concentrations of water vapour and semivolatiles as well as aerosol trajectories in the CCN column were calculated by a computational fluid dynamics model. These trajectories and vapour concentrations were then used as an input for the cloud parcel model to simulate mass transfer kinetics of water and semivolatiles between aerosol particles and the gas phase. Two different questions were studied: (1) how big fraction of semivolatiles is evaporated from particles before activation in the CCN counter? (2) How much the CCN activity can be increased due to condensation of semivolatiles prior to the maximum water supersaturation in the case of high semivolatile concentration in the gas phase? The results show that, to increase the CCN activity of aerosol particles, a very high gas phase concentration (as compared to typical ambient conditions) is needed. We used nitric acid as a test compound. A concentration of several ppb or higher is needed for measurable effect. In the case of particle evaporation, we used ammonium nitrate as a test compound and found that it partially evaporates before maximum supersaturation is reached in the CCN counter, thus causing an underestimation of CCN activity. The effect of evaporation is clearly visible in all supersaturations, leading to an underestimation of the critical dry diameter by 10 to 15 nanometres in the case of ammonium nitrate particles in different supersaturations. This result was also confirmed by measurements in supersaturations between 0.1 and 0.7%.

  4. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  6. Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

    NASA Astrophysics Data System (ADS)

    Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

    2016-04-01

    Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice

  7. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    DOE PAGES

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-14

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed tomore » OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions

  8. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    DOE PAGES

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-06

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH andmore » O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  9. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging

  10. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

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

    NASA Astrophysics Data System (ADS)

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

    2012-07-01

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

  12. Glass shards, pumice fragments and volcanic aerosol particles - diagenesis a recorder of volcanic activity?

    NASA Astrophysics Data System (ADS)

    Obenholzner, J. H.; Schroettner, H.; Poelt, P.; Delgado, H.

    2003-04-01

    Detailed SEM/EDS studies of Triassic (Southern Alps, A, I, Sl) and Miocene (Mixteca Alta, Mexico) tuffs revealed that volcanic glass shards can be replaced by zeolites (analcite), chlorites and smectites preserving the shape of primary shards (1). The Triassic pyroclastic deposits have been incorporated in the pre-Alpine burial diagenesis, the Miocene pyroclastic deposits are bentonites. The volcanologist is impressed by the circumstances that million years old pyroclast relict textures can be sized. Shape parameters obtained by image analysis can be compared with much younger pyroclastic deposits (2). Both deposits have not been effected by shearing. The alteration of pumice fragments of Triassic age is not a simple replacement process. Intergrowth of different illites and chlorites and probably vesicle filling by SiO2 and subsequent overgrowth make a reconstruction sometimes difficult. These processes are accompanied by the formation of REE-, Y- and Zr-bearing minerals as well as with the alteration of zircons. Studies of recently erupted ash from Popocatepetl volcano reveal the presence of a variety of µm-sized contact-metamorphosed clasts being a part of the volcanic ash (3). Such clasts should be present in many older pyroclastic deposits, especially where volcanoes had been situated on massive sedimentary units providing contact metamorphism in the realm of a magma chamber or during magma ascent. Volcanic aerosol particles collected in 1997 from the passively degassing plume of Popocatepetl volcano revealed in FESEM/EDS analysis (H. Schroettner and P. Poelt) a wide spectrum of fluffy, spherical and coagulated spherical particles (µm-sized). Under pre-vacuum conditions they remained stable for ca. 3 years (3). In nature the fate of these particles in the atmosphere is unknown. Are there relicts in marine, lacustrine sediments and ice cores, which could be used as proxies of volcanic activity? (1) Obenholzner &Heiken,1999. Ann.Naturhist.Mus.Wien, 100 A, 13

  13. Variability of CCN Activation Behaviour of Aerosol Particles in the Marine Boundary Layer of the Northern and Southern Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Henning, Silvia; Dieckmann, Katrin; Hartmann, Susan; Schäfer, Michael; Wu, Zhijun; Merkel, Maik; Wiedensohler, Alfred; Stratmann, Frank

    2013-04-01

    The variability of cloud condensation nucleus (CCN) activation behaviour and total CCN number concentrations was investigated during three ship cruises. Measurements were performed in a mobile laboratory on the German research vessel FS Polarstern cruising between Cape Town and Bremerhaven (April / May and October / November 2011) as well as between Punta Arenas and Bremerhaven (April / May 2012). CCN size distributions were measured for supersaturations between 0.1% and 0.4% using a Cloud Condensation Nucleus Counter (DMT, USA). Aerosol particle and CCN total number concentrations as well as the hygroscopicity parameter κ (Petters and Kreidenweis, 2007) were determined. Furthermore, size distribution data were collected. The hygroscopicity parameter κ featured a high variability during the cruises, with a median κ-value of 0.52 ± 0.26. The κ-values are depended on air mass origin; and are as expected mainly dominated by marine influences, but also long range transport of aerosol particles was detected. In the Celtic Sea, κ was found to be lower than that of clean marine aerosol particles (0.72 ± 0.24; Pringle et al., 2010) with κ-values ~0.2, possibly influenced by anthropogenic emissions from Europe. Close to the West African coast particle hygroscopicity was found to be influenced by the Saharan dust plume, resulting in low κ-values ~0.25. Petters, M.D. and S.M. Kreidenweis (2007), A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. and Phys., 7, 1961-1971. Pringle, K.J., H. Tost, A. Pozzer, U. Pöschl, and J. Lelieveld (2010), Global distribution of the effective aerosol hygroscopicity parameter for CCN activation, Atmos. Chem. Phys., 10, 5241-5255.

  14. Enhanced High-Temperature Ice Nucleation Ability of Crystallized Aerosol Particles after Pre-Activation at Low Temperature

    NASA Astrophysics Data System (ADS)

    Wagner, R.; Moehler, O.; Saathoff, H.; Schnaiter, M.

    2014-12-01

    The term pre-activation in heterogeneous ice nucleation describes the observation that the ice nucleation ability of solid ice nuclei may improve after they have already been involved in ice crystal formation or have been exposed to a temperature lower than 235 K. This can be explained by the retention of small ice embryos in cavities or crevices at the particle surface or by the capillary condensation and freezing of supercooled water, respectively. In recent cloud chamber experiments with crystallized aqueous ammonium sulfate, oxalic acid, and succinic acid solution droplets, we have unraveled a further pre-activation mechanism under ice subsaturated conditions which does not require the preceding growth of ice on the seed aerosol particles (Wagner, R. et al., J. Geophys. Res. Atmos., 119, doi: 10.1002/2014JD021741). First cloud expansion experiments were performed at a high temperature (267 - 244 K) where the crystallized particles did not promote any heterogeneous ice nucleation. Ice nucleation at this temperature, however, could be triggered by temporarily cooling the crystallized particles to a lower temperature. This is because upon crystallization, residuals of the aqueous solution are trapped within the crystals. These captured liquids can freeze when cooled below their respective homogeneous or heterogeneous freezing temperature, leading to the formation of ice pockets in the crystalline particles. When warmed again to the higher temperature, ice formation by the pre-activated particles occurred via depositional and deliquescence-induced ice growth, with ice active fractions ranging from 1 to 4% and 4 to 20%, respectively. Pre-activation disappeared above the eutectic temperature, which for the organic acids are close to the melting point of ice. This mechanism could therefore contribute to the very small fraction of atmospheric aerosol particles that are still ice active well above 263 K.

  15. Laser-Assisted Analysis of Aerosol Particles

    NASA Technical Reports Server (NTRS)

    Sinha, M. P.; Giffin, C. E.; Norris, D. D.; Friedlander, S. K.

    1985-01-01

    Proposed instrument makes rapid mass-spectrometric analyses of individual particles in aerosols. Each particle vaporized and ionized by intense laser pulse, which creates ions of minimum complexity. Ability to analyze single aerosol particles continuously makes technique suitable for detection of toxic aerosol particles on real-time basis and for identification of their sources.

  16. Wind reduction by aerosol particles

    NASA Astrophysics Data System (ADS)

    Jacobson, Mark Z.; Kaufman, Yoram J.

    2006-12-01

    Aerosol particles are known to affect radiation, temperatures, stability, clouds, and precipitation, but their effects on spatially-distributed wind speed have not been examined to date. Here, it is found that aerosol particles, directly and through their enhancement of clouds, may reduce near-surface wind speeds below them by up to 8% locally. This reduction may explain a portion of observed ``disappearing winds'' in China, and it decreases the energy available for wind-turbine electricity. In California, slower winds reduce emissions of wind-driven soil dust and sea spray. Slower winds and cooler surface temperatures also reduce moisture advection and evaporation. These factors, along with the second indirect aerosol effect, may reduce California precipitation by 2-5%, contributing to a strain on water supply.

  17. Investigating primary marine aerosol properties: CCN activity of sea salt and mixed particles

    NASA Astrophysics Data System (ADS)

    King, S. M.; Butcher, A. C.; Rosenoern, T.; Coz, E.; Lieke, K. I.; de Leeuw, G.; Nilsson, E. D.; Bilde, M.

    2012-04-01

    Sea salt particles ejected as a result of bubbles bursting from artificial seawater in a closed stainless steel tank were sampled for size distribution, morphology, and cloud condensation nucleus (CCN) activity. The two-component artificial seawater consisted of salt, either NaCl or sea salt, and one organic compound in deionized water. Several organic molecules representative of oceanic organic matter were investigated. Bubbles were generated either by aeration through a porous diffuser or by water jet impingement on the surface of the artificial seawater. The effect of bubble lifetime, which was controlled by varying the depth of the diffuser in the water column, on particle size and CCN activity was investigated and was found to be insignificant for the organic compounds studied. The CCN activities of particles produced from diffuser-generated bubbles were generally governed by the high hygroscopicity of salt, such that activation was indistinguishable from that of salt, except in the case of very low mass ratio of salt to organic matter in the seawater solution. There was, however, a considerable decrease in CCN activity for particles produced from jet impingement on seawater that had a salinity of 10‰ and contained 0.45 mM of sodium laurate, an organic surfactant. The production of a thick foam layer from impingement may explain the difference in activation and supports hypotheses that particle production from the two methods of generating bubbles is not similar. Accurate conclusions from observed CCN activities of particles from artificial seawater containing organic matter require knowledge of the CCN activity of the inorganic component, especially as a small amount of the inorganic can heavily influence activation. Therefore, the CCN activity of both artificial sea salt and NaCl were measured and compared. Part of the discrepancy observed between the CCN activities of the two salts may be due to morphological differences, which were investigated using

  18. Photochemical Aging of Organic Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Nizkorodov, S. A.; Bateman, A. P.; Dailo, M.; Do, T.; Mang, S. A.; Pan, X.; Underwood, J. S.; Walser, M. L.

    2007-05-01

    Secondary Organic Aerosol (SOA) particles are produced in the atmosphere as a result of oxidation of volatile organic compounds (VOC). Primary Organic Aerosol (POA) particles are directly emitted in the atmosphere by their sources. This research focuses on the mechanisms of direct photochemical processes taking place in model SOA and POA particles, the role of such processes in aging of organic aerosol particles, and the effect of photochemistry on particles' physicochemical properties. To address these questions, artificial SOA and POA particles are investigated with several laboratory-based approaches relying on cavity ring-down spectroscopy and mass-spectrometry. SOA particles generated by dark oxidation of d-Limonene, alpha-Pinene, and beta-Pinene by ozone are all found to absorb radiation in the tropospheric actinic window. The UV absorption photolyzes SOA constituents resulting in a release of small VOC molecules back in the gas-phase, and considerable change in SOA chemical composition. For terpenes featuring a terminal double bond, the main SOA photolysis products are invariably found to be formaldehyde and formic acid. Similar observations are obtained for products of ozonolysis of thin films of unsaturated fatty acids and self-assembled monolayers of unsaturated alkenes. For the case of fatty acids, a very detailed mechanism of ozonolysis and subsequent photolysis is proposed. The photolytic activity is primarily attributed to organic peroxides and aldehydes. These results convincingly demonstrate that photochemical processes occurring inside SOA and POA particles age the particles on time scales that are shorter than typical lifetimes of aerosol particles in the atmosphere.

  19. Vapor scavenging by atmospheric aerosol particles

    SciTech Connect

    Andrews, E.

    1996-05-01

    Particle growth due to vapor scavenging was studied using both experimental and computational techniques. Vapor scavenging by particles is an important physical process in the atmosphere because it can result in changes to particle properties (e.g., size, shape, composition, and activity) and, thus, influence atmospheric phenomena in which particles play a role, such as cloud formation and long range transport. The influence of organic vapor on the evolution of a particle mass size distribution was investigated using a modified version of MAEROS (a multicomponent aerosol dynamics code). The modeling study attempted to identify the sources of organic aerosol observed by Novakov and Penner (1993) in a field study in Puerto Rico. Experimentally, vapor scavenging and particle growth were investigated using two techniques. The influence of the presence of organic vapor on the particle`s hydroscopicity was investigated using an electrodynamic balance. The charge on a particle was investigated theoretically and experimentally. A prototype apparatus--the refractive index thermal diffusion chamber (RITDC)--was developed to study multiple particles in the same environment at the same time.

  20. AEROSOL PARTICLE COLLECTOR DESIGN STUDY

    SciTech Connect

    Lee, S; Richard Dimenna, R

    2007-09-27

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

  1. Sources and transformations of atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Cross, Eben Spencer

    Aerosol particles are an important component of the Earth-Atmosphere system because of their influence on the radiation budget both directly (through absorption and scattering) and indirectly (through cloud condensation nuclei (CCN) activity). The magnitude of the raditaive forcing attributed to the direct and indirect aerosol effects is highly uncertain, leading to large uncertainties in projections of global climate change. Real-time measurements of aerosol properties are a critical step toward constraining the uncertainties in current global climate modeling and understanding the influence that anthropogenic activities have on the climate. The objective of the work presented in this thesis is to gain a more complete understanding of the atmospheric transformations of aerosol particles and how such transformations influence the direct and indirect radiative effects of the particles. The work focuses on real-time measurements of aerosol particles made with the Aerodyne Aerosol Mass Spectrometer (AMS) developed in collaboration with the Boston College research group. A key feature of the work described is the development of a light scattering module for the AMS. Here we present the first results obtained with the integrated light scattering - AMS system. The unique and powerful capabilities of this new instrument combination are demonstrated through laboratory experiments and field deployments. Results from two field studies are presented: (1) The Northeast Air Quality Study (NEAQS), in the summer of 2004, conducted at Chebogue Point, Nova Scotia and (2) The Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in and around Mexico City, Mexico in March of 2006. Both field studies were designed to study the transformations that occur within pollution plumes as they are transported throughout the atmosphere. During the NEAQS campaign, the pollution plume from the Northeastern United States was intercepted as it was

  2. Test-Aerosol Generator For Calibrating Particle Counters

    NASA Technical Reports Server (NTRS)

    Mogan, Paul A.; Adams, Alois J.; Schwindt, Christian J.; Hodge, Timothy R.; Mallow, Tim J.; Duong, Anh A.; Bukauskas, Vyto V.

    1996-01-01

    Apparatus generates clean, stable aerosol stream for use in testing and calibrating laser-based aerosol-particle counter. Size and concentration of aerosol particles controlled to ensure accurate calibration. Cheap, widely available medical nebulizers used to generate aerosols.

  3. Sulfur speciation in individual aerosol particles

    NASA Astrophysics Data System (ADS)

    Neubauer, Kenneth R.; Sum, Stephen T.; Johnston, Murray V.; Wexler, Anthony S.

    1996-08-01

    Sulfur aerosols play an important role in acid deposition and the Earth's energy balance. Important species in these aerosols include methanesulfonates, hydroxymethanesulfonates, sulfates, and sulfites. Because the relative amounts of these species indicate different sources and atmospheric processes, it is important to distinguish them in single-aerosol particles. To accomplish this task, we use rapid single-particle mass spectrometry (RSMS), a technique that permits individual particles to be analyzed in an online mode. Each sulfur species produces a characteristic set of ions in the mass spectra. In simulated marine and urban aerosols the relative amounts of methanesulfonic acid (MSA) and sodium hydroxymethanesulfonate (NaHMSA) in a single particle can be determined from peak area ratios in the mass spectra. Improved quantitation is possible by application of the classification and regression tree (CART) algorithm to distinguish the mass spectra of particles having different compositions. Factors that influence speciation include particle size, morphology, and laser fluence.

  4. Air mass origin and its influence on radionuclide activities ( 7Be and 210Pb) in aerosol particles at a coastal site in the western Mediterranean

    NASA Astrophysics Data System (ADS)

    Dueñas, C.; Orza, J. A. G.; Cabello, M.; Fernández, M. C.; Cañete, S.; Pérez, M.; Gordo, E.

    2011-07-01

    Studies of radionuclide activities in aerosol particles provide a means for evaluating the integrated effects of transport and meteorology on the atmospheric loadings of substances with different sources. Measurements of aerosol mass concentration and specific activities of 7Be and 210Pb in aerosols at Málaga (36° 43' 40″ N; 4° 28' 8″ W) for the period 2000-2006 were used to obtain the relationships between radionuclide activities and airflow patterns by comparing the data grouped by air mass trajectory clusters. The average concentration values of 7Be and 210Pb over the 7 year period have been found to be 4.6 and 0.58 mBq m -3, respectively, with mean aerosol mass concentration of 53.6 μg m -3. The identified air flow types arriving at Málaga reflect the transitional location of the Iberian Peninsula and show significant differences in radionuclide activities. Air concentrations of both nuclides and the aerosol mass concentration are controlled predominantly by the synoptic scenarios leading to the entrance of dust-laden continental flows from northern Africa and the arrival of polar maritime air masses, as implied by the strong correlations found between the monthly frequencies of the different air masses and the specific activities of both radionuclides. Correlations between activity concentrations and precipitation are significant though lower than with air masses.

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

    NASA Astrophysics Data System (ADS)

    Fierce, Laura; McGraw, Robert

    2016-04-01

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

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

    SciTech Connect

    Davidovits, Paul

    2015-10-20

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

  7. Characteristics of aerosolized ice forming marine biogenic particles

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.

    Ice particles are ubiquitous in the atmosphere existing as the sole constituents of glaciated cirrus clouds or coexisting with supercooled liquid droplets in mixed-phase clouds. Aerosol particles serving as heterogeneous ice nuclei for ice crystal formation impact the global radiative balance by modification of cloud radiative properties, and thus climate. Atmospheric ice formation is not a well understood process and represents great uncertainty for climate prediction. The oceans which cover the majority of the earth's surface host nearly half the total global primary productivity and contribute to the greatest aerosol production by mass. However, the effect of biological activity on particle aerosolization, particle composition, and ice nucleation is not well established. This dissertation investigates the link between marine biological activity, aerosol particle production, physical/chemical particle characteristics, and ice nucleation under controlled laboratory conditions. Dry and humidified aerosol size distributions of particles from bursting bubbles generated by plunging water jets and aeration through frits in a seawater mesocosm containing bacteria and/or phytoplankton cultures, were measured as a function of biological activity. Total particle production significantly increases primarily due to enhanced aerosolization of particles ≤100 nm in diameter attributable to the presence and growth of phytoplankton. Furthermore, hygroscopicity measurements indicate primary organic material associated with the sea salt particles, providing additional evidence for the importance of marine biological activity for ocean derived aerosol composition. Ice nucleation experiments show that these organic rich particles nucleate ice efficiently in the immersion and deposition modes, which underscores their importance in mixed-phase and cirrus cloud formation processes. In separate ice nucleation experiments employing pure cultures of Thalassiosira pseudonana, Nannochloris

  8. The on-line analysis of aerosol-delivered pharmaceuticals via single particle aerosol mass spectrometry.

    PubMed

    Morrical, Bradley D; Balaxi, Maria; Fergenson, David

    2015-07-15

    The use of single particle aerosol mass spectrometry (SPAMS) was evaluated for the analysis of inhaled pharmaceuticals to determine the mass distribution of the individual active pharmaceutical ingredients (API) in both single ingredient and combination drug products. SPAMS is an analytical technique where the individual aerodynamic diameters and chemical compositions of many aerosol particles are determined in real-time. The analysis was performed using a Livermore Instruments SPAMS 3.0, which allowed the efficient analysis of aerosol particles with broad size distributions and can acquire data even under a very large particle load. Data similar to what would normally require roughly three days of experimentation and analysis was collected in a five minute period and analyzed automatically. The results were computed to be comparable to those returned by a typical Next Generation Impactor (NGI) particle size distribution experiment.

  9. CCN activity of aliphatic amine secondary aerosol

    NASA Astrophysics Data System (ADS)

    Tang, X.; Price, D.; Praske, E.; Vu, D.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-01-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3), contains less volatile compounds than the primary aliphatic amine (BA) aerosol. TMA + N2O5 form semi-volatile organics in low RH conditions that have κ ~ 0.20, indicative of slightly soluble organic material. As RH increases, several inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. Higher CCN activity (κ > 0.3) was also observed for humid BA+N2O5 aerosols compared with dry aerosol (κ ~ 0.2), as a result of the formation of inorganic salts such as NH4NO3 and butylamine nitrate (C4H11N · HNO3). Compared with TMA, BA+N2O5 reactions produce more volatile aerosols. The BA+N2O5 aerosol products under humid experiments were found to be very sensitive to the temperature within the stream-wise continuous flow thermal gradient CCN counter. The CCN counter, when set above a 21 °C temperature difference, evaporates BA+N2O5 aerosol formed at RH ≥ 30%; κ ranges from 0.4 to 0.7 and is dependent on the instrument supersaturation (ss) settings. The aerosol behaves non-ideally, hence simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems κ ranges from 0.2 < κ < 0.7. This work indicates that

  10. Online measurements of ambient fluorescent aerosol particles by WIBS at a polluted regional site in the North China Plain: potential impact of burning activities

    NASA Astrophysics Data System (ADS)

    Su, H.; Wang, Z.; Cheng, Y.; Xie, Z.; Kecorius, S.; McMeeking, G. R.; Yu, X.; Pöhlker, C.; Zhang, M.; Wiedensohler, A.; Kuhn, U.; Poeschl, U.; Huffman, J. A.

    2015-12-01

    Online measurements of ambient fluorescent aerosol particles by WIBS at a polluted regional site in the North China Plain: potential impact of burning activities Zhibin Wang1, Xiawei Yu1,3, Simonas Kecorius2, Zhouqing Xie3, Gavin McMeeking4, Christopher Pöhlker1, Minghui, Zhang1, Alfred Wiedensohler2, Uwe Kuhn1, Yafang Cheng1, Ulrich Pöschl1, Hang Su1,*1Multiphase Chemistry and Biogeochemistry Departments, Max Planck Institute for Chemistry, Mainz 55128, Germany2Leibniz-Institute for Tropospheric Research, Leipzig 04318, Germany3School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China4Droplet Measurement Technologies, Boulder 80301, USA ABSTRACTBioaerosols are the main subset of super-micron particles, and significantly influence the evolution of cloud and precipitation, as well as the public health. Currently, the detection of ambient biological materials in real-time is mainly based on the presence of fluorophores in the particles. In this study, we present the wideband integrated bioaerosol spectrometer (WIBS) measurement results to characterize the fluorescent aerosol particles (FAP) at a polluted regional site (Xianghe, 39.80 °N, 116.96 °E) in the North China Plain. We observed substantially much higher number concentration of FAP as compared with those of previous studies in clean environments. We found the good agreement between the FAP number fraction in coarse mode particles (> 1 mm) and BC mass fraction in fine particles (< 1 mm), possibly indicating a majority of the observed FAP is to a certain extent related to the anthropogenic burning activities nearby. This interference and uncertainty should be especially noticed when performing fluorescence measurements in the polluted area, where the certain non-biological compounds (such as SOA, PAH and soot) may significantly lead to a positive fluorescence measurement artifacts and an overestimation of actual fluorescent biological aerosol particles. We also

  11. Ice Phase Transitions by Atmospheric Aerosol Particles of Varied Composition

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; Prenni, A. J.; Archuleta, C. A.; Kreidenweis, S. M.; Cziczo, D. J.; Murphy, D. M.; Thomson, D. S.

    2001-12-01

    This paper describes laboratory and field study measurements of water uptake and ice nucleation by surrogate and real atmospheric aerosol particles. Laboratory measurements of water uptake are made using a humidified tandem differential mobility analyzer (HTDMA) and a cloud condensation nucleus (CCN) instrument operating at 20 to 30 \\deg C. Measurements of ice nucleation are made using a continuous flow ice-thermal diffusion chamber (CFDC) operated to -60 \\deg C for relevance toward understanding cirrus cloud formation. Extending earlier laboratory studies of single composition aerosols, we are investigating water uptake and ice nucleation rates and mechanisms by mixed aerosols of various types, including sulfate-nitrate, sulfate-organic, mineral oxide-sulfate and black carbon-sulfate types. Methodologies will be described and results will be summarized. Field measurements are planned to study heterogeneous and homogeneous ice nucleation by free tropospheric aerosols at a high altitude laboratory. The field study will include measurements of the compositions of aerosols that activate ice formation by homogeneous and heterogeneous ice nucleation mechanisms. This aspect of the study will be facilitated by interfacing the CFDC to the PALMS (Particle Analysis by Laser Mass Spectrometry) instrument. This combined instrument system was tested in the laboratory to quantify sampling efficiencies and validate specificity for sampling ice nucleus aerosol particles. Initial field data, if available at conference time, will be compared and contrasted with the results obtained for laboratory surrogate particles.

  12. Standard aerosols for particle velocimeters

    NASA Technical Reports Server (NTRS)

    Deepark, A.; Ozarski, R.; Thomson, J. A. L.

    1976-01-01

    System consists of laser-scattering counter (LSC) and photographic system. Photographic system provides absolute method of measuring aerosol size-distribution independently of their light scattering properties. LSC comprises 1-mW He/Ne laser, input optics, collecting optics, photodetector, and signal-processing electronics.

  13. The Life Cycle of Stratospheric Aerosol Particles

    NASA Technical Reports Server (NTRS)

    Hamill, Patrick; Jensen, Eric J.; Russell, P. B.; Bauman, Jill J.

    1997-01-01

    This paper describes the life cycle of the background (nonvolcanic) stratospheric sulfate aerosol. The authors assume the particles are formed by homogeneous nucleation near the tropical tropopause and are carried aloft into the stratosphere. The particles remain in the Tropics for most of their life, and during this period of time a size distribution is developed by a combination of coagulation, growth by heteromolecular condensation, and mixing with air parcels containing preexisting sulfate particles. The aerosol eventually migrates to higher latitudes and descends across isentropic surfaces to the lower stratosphere. The aerosol is removed from the stratosphere primarily at mid- and high latitudes through various processes, mainly by isentropic transport across the tropopause from the stratosphere into the troposphere.

  14. Particle size dependent response of aerosol counters

    NASA Astrophysics Data System (ADS)

    Ankilov, A.; Baklanov, A.; Colhoun, M.; Enderle, K.-H.; Gras, J.; Julanov, Yu.; Kaller, D.; Lindner, A.; Lushnikov, A. A.; Mavliev, R.; McGovern, F.; O'Connor, T. C.; Podzimek, J.; Preining, O.; Reischl, G. P.; Rudolf, R.; Sem, G. J.; Szymanski, W. W.; Vrtala, A. E.; Wagner, P. E.; Winklmayr, W.; Zagaynov, V.

    During an international workshop at the Institute for Experimental Physics of the University of Vienna, Austria, which was coordinated within the Committee on Nucleation and Atmospheric Aerosols (IAMAS-IUGG), 10 instruments for aerosol number concentration measurement were studied, covering a wide range of methods based on various different measuring principles. In order to investigate the detection limits of the instruments considered with respect to particle size, simultaneous number concentration measurements were performed for monodispersed aerosols with particle sizes ranging from 1.5 to 50 nm diameter and various compositions. The instruments considered show quite different response characteristics, apparently related to the different vapors used in the various counters to enlarge the particles to an optically detectable size. A strong dependence of the 50% cutoff diameter on the particle composition in correlation with the type of vapor used in the specific instrument was found. An enhanced detection efficiency for ultrafine hygroscopic sodium chloride aerosols was observed with water operated systems, an analogous trend was found for n-butanol operated systems with nonhygroscopic silver and tungsten oxide particles.

  15. Aerosol particle analysis by Raman scattering technique

    SciTech Connect

    Fung, K.H.; Tang, I.N.

    1992-10-01

    Laser Raman spectroscopy is a very versatile tool for chemical characterization of micron-sized particles. Such particles are abundant in nature, and in numerous energy-related processes. In order to elucidate the formation mechanisms and understand the subsequent chemical transformation under a variety of reaction conditions, it is imperative to develop analytical measurement techniques for in situ monitoring of these suspended particles. In this report, we outline our recent work on spontaneous Raman, resonance Raman and non-linear Raman scattering as a novel technique for chemical analysis of aerosol particles as well as supersaturated solution droplets.

  16. 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.

  17. Phase transitions and morphologies of aerosol particles

    NASA Astrophysics Data System (ADS)

    Song, M.; Marcolli, C.; Krieger, U.; Zuend, A.; Peter, T.

    2012-12-01

    Tropospheric aerosol particles consisting of complex mixtures of organic compounds, ammonium sulfate (AS) and water undergo phase transitions such as liquid-liquid phase separation (LLPS), efflorescence and deliquescence as a consequence of changes in ambient relative humidity (RH). These phase transitions in the mixed aerosol particles may lead to different particle configurations such as core-shell or partially engulfed structures. However, the physical states and morphologies of these aerosol particles are still poorly understood. In this study, we investigate the phase transitions and morphological changes of various internally mixed organics/AS/water particles with different organic-to-inorganic ratios (OIR), namely OIR = 6:1, 2:1, 1:2 and 1:6 during humidity cycles using optical microscopy and Raman spectroscopy. Particularly, we explore how the properties of different organic functional groups and the compositional complexity of the organic aerosol fraction influence the occurrence of LLPS in the relationship with the organic oxygen-to-carbon (O:C) ratios. We found that LLPS occurred for all mixtures with O:C < 0.56, for none of the mixtures with O:C > 0.80, and depended on the specific types and compositions of organic functional groups for 0.56 < O:C < 0.80. Moreover, the number of mixture components and the spread of the O:C range did not notably influence the conditions for LLPS to occur. Since in ambient aerosols O:C and OIR range typically between 0.2 and 1.0, and between 4:1 and 1:5, respectively, LLPS is expected to be a common feature of tropospheric aerosols. AS in the mixed particles effloresced between 0 and 47 %RH and deliquesced between 71 and 80 %RH during humidity cycles. Compared to a deliquescence relative humidity (DRH) of 80 % for pure AS, the DRH in the mixed particles showed slightly lower values. A strong reduction or complete inhibition of efflorescence occurred for mixtures with high OIR that did not exhibit LLPS. Both core-shell and

  18. Fatty Acids as Surfactants on Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Tervahattu, H.; Juhanoja, J.; Niemi, J.

    2003-12-01

    Fatty acids (n-alcanoic acids) are common compounds in numerous anthropogenic and natural emissions. According to Rogge et al. (1993), catalyst-equipped automobiles emitted more than 600 μg km-1 of fatty acids which was over 50% of all identified organics in fine aerosol emissions. Coal burning produces fatty acids ranging from about 1700 mg kg-1 for bituminous coal to over 10000 mg kg-1 for lignite (Oros and Simoneit, 2000). Similarly, biomass burning is an important source for aerosol fatty acids. They are the major identified compound group in deciduous tree smoke, their total emission factor being measured as 1589 mg kg-1 which was 56% of all identified organic compounds (Oros and Simoneit, 2001a). Large amounts of fatty acid are also emitted from burning of conifer trees and grass (Oros and Simoneit, 2001a; Simoneit, 2002). Fatty acids have been reported to be major constituents of marine aerosols in many investigations (Barger and Garrett, 1976; Gagosian et. al, 1981; Sicre et al., 1990; Stephanou, 1992). It has been suggested that as the marine aerosol particles form, they acquire a coating of organic surfactants (Blanchard, 1964; Gill et al., 1983; Middlebrook et al., 1998; Ellison et al., 1999). Amphiphilic molecules, including lipids, can be assembled as monomolecular layers at air/water interfaces as well as transported to a solid support. Recently, we could show by time-of-flight secondary ion mass spectrometry that fatty acids are important ingredients of the outermost surface layer of the sea-salt aerosol particles (Tervahattu et al., 2002). In their TOF-SIMS studies on the surface composition of atmospheric aerosols, Peterson and Tyler (2002) found fatty acids on the surface of Montana forest fire particles. In this work we have studied by TOF-SIMS the surface chemical composition of aerosol particles emitted from field fires in the Baltic and other East European countries and transported to Finland as well as aerosol particles transported from

  19. Particle-resolved simulation of aerosol size, composition, mixing state, and the associated optical and cloud condensation nuclei activation properties in an evolving urban plume

    SciTech Connect

    Zaveri, Rahul A.; Barnard, James C.; Easter, Richard C.; Riemer, Nicole; West, Matthew

    2010-09-11

    The recently developed particle-resolved aerosol box model PartMC-MOSAIC was used to simulate the evolution of aerosol mixing state and the associated optical and cloud condensation nuclei (CCN) activation properties in an idealized urban plume. The model explicitly resolved the size and composition of individual particles from a number of sources and tracked their evolution due to condensation/evaporation, coagulation, emission, and dilution. The ensemble black carbon (BC) specific absorption cross section increased by 40% over the course of two days as a result of BC aging by condensation and coagulation. Three- and four-fold enhancements in CCN/CN ratios were predicted to occur within 6 hours for 0.2% and 0.5% supersaturations (S), respectively. The particle-resolved results were used to evaluate the errors in the optical and CCN activation properties that would be predicted by a conventional sectional framework that assumes monodisperse, internally-mixed particles within each bin. This assumption artificially increased the ensemble BC specific absorption by 14-30% and decreased the single scattering albedo by 0.03-0.07 while the bin resolution had a negligible effect. In contrast, the errors in CCN/CN ratios were sensitive to the bin resolution, and they depended on the chosen supersaturation. For S = 0.2%, the CCN/CN ratio predicted using 100 internally-mixed bins was up to 25% higher than the particle-resolved results, while it was up to 125% higher using 10 internally-mixed bins. Errors introduced in the predicted optical and CCN properties by neglecting coagulation were also quantified.

  20. Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Hansen, Kristen J.

    different source and process components, and to examine concentration changes in groups of variables with respect to time of day and meteorological conditions. Seven orthogonal groups of variables resulted from the statistical analysis; the groups serve as molecular markers for different biologic and anthropogenic emission sources. In addition, the results of the statistical analysis were used to investigate how several emission source contributions vary with respect to local atmospheric dynamics. Field studies were conducted in the urban environment in and around Boulder, CO. to characterize the dynamics, chemistry, and emission sources which affect the composition and concentration of different size-fractions of aerosol particles in the Boulder air mass. Relationships between different size fractions of particles and some gas-phase pollutants were elucidated. These field studies included an investigation of seasonal variations in the organic content and concentration of aerosol particles, and how these characteristics are related to local meteorology and to the concentration of some gas-phase pollutants. The elemental and organic composition of aerosol particles was investigated according to particle size in preliminary studies of size-differentiated samples of aerosol particles. In order to aid in future studies of urban aerosol particles, samples were collected at a forest fire near Boulder. Molecular markers specific to wood burning processes will be useful indicators of residential wood burning activities in future field studies.

  1. Sulfur speciation of single aerosol particles

    SciTech Connect

    Neubauer, K.R.; Sum, S.T.; Johnston, M.V.; Wexler, A.S.

    1995-12-31

    Sulfur enters the atmosphere as gaseous species emitted from both natural and anthropogenic sources. These species can undergo a variety of oxidation reactions that ultimately yield hexavalent sulfur aerosols. Since the final products play an important role in acid rain production and the earth`s energy balance, it is important to distinguish tetravalent and hexavalent sulfur aerosols, as well as differentiate those arising from natural and anthropogenic sources. To attain these goals the authors chose to examine five target compounds that are present in the atmosphere: sodium sulfate, ammonium sulfate, ammonium sulfite, methanesulfonic acid (MSA), and the sodium salt of hydroxymethanesulfonic acid (NaHMSA). Sodium sulfate is observed in oceanic aerosols, while both ammonium salts are observed over land. MSA is found only in the marine environment and originates solely from natural emissions, while HMSA is formed in urban hazes and primarily arises from anthropogenic sources. Thus, MSA and HMSA serve as tracers for distinguishing natural and anthropogenic sulfur emissions. To differentiate these compounds, the authors used Rapid Single-Particle Mass Spectrometry (RSMS), a method that allows single particles to be analyzed on-line and in real time. With RSMS, particles are drawn directly into the source region of a reflectron time-of-flight mass spectrometer where they are detected by light scattering of a continuous laser beam and then ablated by an excimer laser pulse. With this sequence of events, each mass spectrum results from a single laser pulse ablating a single particle.

  2. Composition and formation of organic aerosol particles in the Amazon

    NASA Astrophysics Data System (ADS)

    Pöhlker, C.; Wiedemann, K.; Sinha, B.; Shiraiwa, M.; Gunthe, S. S.; Artaxo, P.; Gilles, M. K.; Kilcoyne, A. L. D.; Moffet, R. C.; Smith, M.; Weigand, M.; Martin, S. T.; Pöschl, U.; Andreae, M. O.

    2012-04-01

    We applied scanning transmission X-ray microscopy with near edge X-ray absorption fine structure (STXM-NEXAFS) analysis to investigate the morphology and chemical composition of aerosol samples from a pristine tropical environment, the Amazon Basin. The samples were collected in the Amazonian rainforest during the rainy season and can be regarded as a natural background aerosol. The samples were found to be dominated by secondary organic aerosol (SOA) particles in the fine and primary biological aerosol particles (PBAP) in the coarse mode. Lab-generated SOA-samples from isoprene and terpene oxidation as well as pure organic compounds from spray-drying of aqueous solution were measured as reference samples. The aim of this study was to investigate the microphysical and chemical properties of a tropical background aerosol in the submicron size range and its internal mixing state. The lab-generated SOA and pure organic compounds occurred as spherical and mostly homogenous droplet-like particles, whereas the Amazonian SOA particles comprised a mixture of homogeneous droplets and droplets having internal structures due to atmospheric aging. In spite of the similar morphological appearance, the Amazon samples showed considerable differences in elemental and functional group composition. According to their NEXAFS spectra, three chemically distinct types of organic material were found and could be assigned to the following three categories: (1) particles with a pronounced carboxylic acid (COOH) peak similar to those of laboratory-generated SOA particles from terpene oxidation; (2) particles with a strong hydroxy (COH) signal similar to pure carbohydrate particles; and (3) particles with spectra resembling a mixture of the first two classes. In addition to the dominant organic component, the NEXAFS spectra revealed clearly resolved potassium (K) signals for all analyzed particles. During the rainy season and in the absence of anthropogenic influence, active biota is

  3. Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

    NASA Astrophysics Data System (ADS)

    Metcalf, A. R.; Dutcher, C. S.

    2014-12-01

    Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

  4. Particle size distribution of indoor aerosol sources

    SciTech Connect

    Shah, K.B.

    1990-10-24

    As concern about Indoor Air Quality (IAQ) has grown in recent years, it has become necessary to determine the nature of particles produced by different indoor aerosol sources and the typical concentration that these sources tend to produce. These data are important in predicting the dose of particles to people exposed to these sources and it will also enable us to take effective mitigation procedures. Further, it will also help in designing appropriate air cleaners. A new state of the art technique, DMPS (Differential Mobility Particle Sizer) System is used to determine the particle size distributions of a number of sources. This system employs the electrical mobility characteristics of these particles and is very effective in the 0.01--1.0 {mu}m size range. A modified system that can measure particle sizes in the lower size range down to 3 nm was also used. Experimental results for various aerosol sources is presented in the ensuing chapters. 37 refs., 20 figs., 2 tabs.

  5. Activation of the Solid Silica Layer of Aerosol-Based C/SiO₂ Particles for Preparation of Various Functional Multishelled Hollow Microspheres.

    PubMed

    Li, Xiangcun; Luo, Fan; He, Gaohong

    2015-05-12

    Double-shelled C/SiO2 hollow microspheres with an outer nanosheet-like silica shell and an inner carbon shell were reported. C/SiO2 aerosol particles were synthesized first by a one-step rapid aerosol process. Then the solid silica layer of the aerosol particles was dissolved and regrown on the carbon surface to obtain novel C/SiO2 double-shelled hollow microspheres. The new microspheres prepared by the facile approach possess high surface area and pore volume (226.3 m(2) g(-1), 0.51 cm(3) g(-1)) compared with the original aerosol particles (64.3 m(2) g(-1), 0.176 cm(3) g(-1)), providing its enhanced enzyme loading capacity. The nanosheet-like silica shell of the hollow microspheres favors the fixation of Au NPs (C/SiO2/Au) and prevents them from growing and migrating at 500 °C. Novel C/C and C/Au/C (C/Pt/C) hollow microspheres were also prepared based on the hollow nanostructure. C/C microspheres (482.0 m(2) g(-1), 0.92 cm(3) g(-1)) were ideal electrode materials. In particular, the Au NPs embedded into the two carbon layers (C/Au/C, 431.2 m(2) g(-1), 0.774 cm(3) g(-1)) show a high catalytic activity and extremely chemical stability even at 850 °C. Moreover, C/SiO2/Au, C/Au/C microspheres can be easily recycled and reused by an external magnetic field because of the presence of Fe3O4 species in the inner carbon shell. The synthetic route reported here is expected to simplify the fabrication process of double-shelled or yolk-shell microspheres, which usually entails multiple steps and a previously synthesized hard template. Such a capability can facilitate the preparation of various functional hollow microspheres by interfacial design.

  6. Glassy aerosols heterogeneously nucleate cirrus ice particles

    NASA Astrophysics Data System (ADS)

    Wilson, Theodore W.; Murray, Benjamin J.; Dobbie, Steven; Cui, Zhiqiang; Al-Jumur, Sardar M. R. K.; Möhler, Ottmar; Schnaiter, Martin; Wagner, Robert; Benz, Stefan; Niemand, Monika; Saathoff, Harald; Ebert, Volker; Wagner, Steven; Kärcher, Bernd

    2010-05-01

    Ice clouds in the tropical tropopause layer (TTL, ~12-18 km, ~180-200 K) play a key role in dehydrating air entering the stratosphere. However, in-situ measurements show that air within these clouds is unexpectedly supersaturated(1); normally the growth of ice crystals rapidly quenches any supersaturation. A number of explanations for high in-cloud humidity have been put forward, but recent research suggests high humidity may be related to the low numbers of ice crystals found within these clouds(1). Low ice number densities can be produced through selective nucleation by a small subset of aerosol particles. This is inconsistent with homogeneous nucleation of ice in liquid aerosols. However, droplets rich in organic material, ubiquitous in the TTL, are known to become glassy (amorphous, non-crystalline solid) under TTL conditions(2,3). Here we show, using a large cloud simulation chamber, that glassy solution droplets nucleate ice heterogeneously at low supersaturations. Using a one-dimensional cirrus model we also show that nucleation by glassy aerosol in the TTL may explain low TTL ice number densities and high in-cloud humidity. Recent measurements of the composition of TTL cirrus residues are consistent with our findings(4). (1) Krämer, M. et al. Ice supersaturations and cirrus cloud crystal numbers. Atm. Chem. Phys. 9, 3505-3522 (2009). (2) Murray, B. J. Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets. Atm. Chem. Phys. 8, 5423-5433 (2008). (3) Zobrist, B., Marcolli, C., Pedernera, D. A. & Koop, T. Do atmospheric aerosols form glasses? Atm. Chem. Phys. 8, 5221-5244 (2008). (4) Froyd, K. D., Murphy, D. M., Lawson, P., Baumgardner, D. & Herman, R. L. Aerosols that form subvisible cirrus at the tropical tropopause. Atmos. Chem. Phys. 10, 209-218 (2010).

  7. 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.

  8. 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

  9. 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

  10. 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

  11. Effect of the secondary organic aerosol coatings on black carbon water uptake, cloud condensation nuclei activity, and particle collapse

    EPA Science Inventory

    The ability of black carbon aerosols to absorb water and act as a cloud condensation nuclei (CCN) directly controls their lifetime in the atmosphere as well as their impact on cloud formation, thus impacting the earth’s climate. Black carbon emitted from most combustion pro...

  12. Characteristics of Chinese aerosols determined by individual-particle analysis

    NASA Astrophysics Data System (ADS)

    Gao, Yuan; Anderson, James R.

    2001-08-01

    Tropospheric aerosols that originate in China and are transported over the North Pacific Ocean have potentially significant impacts on regional and global climate. These aerosols are complex mixtures of soil dust and anthropogenic particles from a variety of sources, including fossil fuel combustion, biomass burning, mining, smelting, and other industrial processes, plus reaction products of heterogeneous processes that affect these particles during transport. In the coastal marine atmosphere, these particles could be further mixed with marine aerosols. To provide examples of the diversity of chemical and physical properties of east Asian aerosols in the spring, individual aerosol particle samples were collected in April and May 1999 in three different environments in China: Qingdao on the coast of the East China Sea, Beijing in the northeast interior, and Mount Waliguan in remote northwestern China. Results reveal that aerosols in this region are complex and heterogeneous. In addition to significant differences in aerosol composition and size distributions among the samples, each sample contains a large number of polyphase aggregates. Many of the particles also have irregular shapes; for a number of the particle types, the irregular shapes should persist even at high ambient RH. Because composition, degree and nature of polyphase aggregation, and shape all effect aerosol radiative properties, the complex state of east Asian aerosols presents a challenge for the modeling of aerosol radiative forcing in the region.

  13. Chemistry and Composition of Atmospheric Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Kolb, Charles E.; Worsnop, Douglas R.

    2012-05-01

    For more than two decades a cadre of physical chemists has focused on understanding the formation processes, chemical composition, and chemical kinetics of atmospheric aerosol particles and droplets with diameters ranging from a few nanometers to ˜10,000 nm. They have adapted or invented a range of fundamental experimental and theoretical tools to investigate the thermochemistry, mass transport, and chemical kinetics of processes occurring at nanoscale gas-liquid and gas-solid interfaces for a wide range of nonideal, real-world substances. State-of-the-art laboratory methods devised to study molecular spectroscopy, chemical kinetics, and molecular dynamics also have been incorporated into field measurement instruments that are deployed routinely on research aircraft, ships, and mobile laboratories as well as at field sites from megacities to the most remote jungle, desert, and polar locations. These instruments can now provide real-time, size-resolved aerosol particle physical property and chemical composition data anywhere in Earth's troposphere and lower stratosphere.

  14. Workplace aerosol mass concentration measurement using optical particle counters.

    PubMed

    Görner, Peter; Simon, Xavier; Bémer, Denis; Lidén, Göran

    2012-02-01

    Direct-reading aerosol measurement usually uses the optical properties of airborne particles to detect and measure particle concentration. In the case of occupational hygiene, mass concentration measurement is often required. Two aerosol monitoring methods are based on the principle of light scattering: optical particle counting (OPC) and photometry. The former analyses the light scattered by a single particle, the latter by a cloud of particles. Both methods need calibration to transform the quantity of scattered light detected into particle concentration. Photometers are simpler to use and can be directly calibrated to measure mass concentration. However, their response varies not only with aerosol concentration but also with particle size distribution, which frequently contributes to biased measurement. Optical particle counters directly measure the particle number concentration and particle size that allows assessment of the particle mass provided the particles are spherical and of known density. An integrating algorithm is used to calculate the mass concentration of any conventional health-related aerosol fraction. The concentrations calculated thus have been compared with simultaneous measurements by conventional gravimetric sampling to check the possibility of field OPC calibration with real workplace aerosols with a view to further monitoring particle mass concentration. Aerosol concentrations were measured in the food industry using the OPC GRIMM® 1.108 and the CIP 10-Inhalable and CIP 10-Respirable (ARELCO®) aerosol samplers while meat sausages were being brushed and coated with calcium carbonate. Previously, the original OPC inlet had been adapted to sample inhalable aerosol. A mixed aerosol of calcium carbonate and fungi spores was present in the workplace. The OPC particle-size distribution and an estimated average particle density of both aerosol components were used to calculate the mass concentration. The inhalable and respirable aerosol fractions

  15. Workplace aerosol mass concentration measurement using optical particle counters.

    PubMed

    Görner, Peter; Simon, Xavier; Bémer, Denis; Lidén, Göran

    2012-02-01

    Direct-reading aerosol measurement usually uses the optical properties of airborne particles to detect and measure particle concentration. In the case of occupational hygiene, mass concentration measurement is often required. Two aerosol monitoring methods are based on the principle of light scattering: optical particle counting (OPC) and photometry. The former analyses the light scattered by a single particle, the latter by a cloud of particles. Both methods need calibration to transform the quantity of scattered light detected into particle concentration. Photometers are simpler to use and can be directly calibrated to measure mass concentration. However, their response varies not only with aerosol concentration but also with particle size distribution, which frequently contributes to biased measurement. Optical particle counters directly measure the particle number concentration and particle size that allows assessment of the particle mass provided the particles are spherical and of known density. An integrating algorithm is used to calculate the mass concentration of any conventional health-related aerosol fraction. The concentrations calculated thus have been compared with simultaneous measurements by conventional gravimetric sampling to check the possibility of field OPC calibration with real workplace aerosols with a view to further monitoring particle mass concentration. Aerosol concentrations were measured in the food industry using the OPC GRIMM® 1.108 and the CIP 10-Inhalable and CIP 10-Respirable (ARELCO®) aerosol samplers while meat sausages were being brushed and coated with calcium carbonate. Previously, the original OPC inlet had been adapted to sample inhalable aerosol. A mixed aerosol of calcium carbonate and fungi spores was present in the workplace. The OPC particle-size distribution and an estimated average particle density of both aerosol components were used to calculate the mass concentration. The inhalable and respirable aerosol fractions

  16. Real-time detection method and system for identifying individual aerosol particles

    DOEpatents

    Gard, Eric E.; Coffee, Keith R.; Frank, Matthias; Tobias, Herbert J.; Fergenson, David P.; Madden, Norm; Riot, Vincent J.; Steele, Paul T.; Woods, Bruce W.

    2007-08-21

    An improved method and system of identifying individual aerosol particles in real time. Sample aerosol particles are collimated, tracked, and screened to determine which ones qualify for mass spectrometric analysis based on predetermined qualification or selection criteria. Screening techniques include one or more of determining particle size, shape, symmetry, and fluorescence. Only qualifying particles passing all screening criteria are subject to desorption/ionization and single particle mass spectrometry to produce corresponding test spectra, which is used to determine the identities of each of the qualifying aerosol particles by comparing the test spectra against predetermined spectra for known particle types. In this manner, activation cycling of a particle ablation laser of a single particle mass spectrometer is reduced.

  17. Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

    NASA Astrophysics Data System (ADS)

    Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

    2014-12-01

    Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could

  18. Organic aggregate formation in aerosols and its impact on the physicochemical properties of atmospheric particles

    NASA Astrophysics Data System (ADS)

    Tabazadeh, Azadeh

    Fatty acid salts and "humic" materials, found in abundance in atmospheric particles, are both anionic surfactants. Such materials are known to form organic aggregates or colloids in solution at very low aqueous concentrations. In a marine aerosol, micelle aggregates can form at a low fatty acid salt molality of ˜10 -3 m. In other types of atmospheric particles, such as biomass burning, biogenic, soil dust, and urban aerosols, "humic-like" materials exist in sufficient quantities to form micelle-like aggregates in solution. I show micelle formation limits the ability of surface-active organics in aerosols to reduce the surface tension of an atmospheric particle beyond about 10 dyne cm -1. A general phase diagram is presented for anionic surfactants to explain how surface-active organics can change the water uptake properties of atmospheric aerosols. Briefly such molecules can enhance and reduce water uptake by atmospheric aerosols at dry and humid conditions, respectively. This finding is consistent with a number of unexplained field and laboratory observations. Dry electron microscope images of atmospheric particles often indicate that organics may coat the surface of particles in the atmosphere. The surfactant phase diagram is used to trace the particle path back to ambient conditions in order to determine whether such coatings can exist on wet ambient aerosols. Finally, I qualitatively highlight how organic aggregate formation in aerosols may change the optical properties and chemical reactivity of atmospheric particles.

  19. Particle size distributions of several commonly used seeding aerosols

    NASA Technical Reports Server (NTRS)

    Crosswy, F. L.

    1985-01-01

    During the course of experimentation, no solid particle powder could be found which produced an aerosol with a narrow particle size distribution when fluidization was the only flow process used in producing the aerosol. The complication of adding particle size fractionation processes to the aerosol generation effort appears to be avoidable. In this regard, a simple sonic orifice is found to be effective in reducing the percentage of agglomerates in the several metal oxide powders tested. Marginally beneficial results are obtained for a 0.5/99.5 percent by weight mixture of the flow agent and metal oxide powder. However, agglomeration is observed to be enhanced when the flow agent percentage is increased to 5 percent. Liquid atomization using the Collison nebulizer as well as a version of the Laskin nozzle resulted in polydispersed aerosols with particle size distributions heavily weighted by the small particle end of the size spectrum. The aerosol particle size distributions produced by the vaporization/condensation seeder are closer to the ideal monodispersed aerosol than any of the other aerosols tested. In addition, this seeding approach affords a measure of control over particle size and particle production rate.

  20. Aerosol stability of infectious and potentially infectious reovirus particles.

    PubMed Central

    Adams, D J; Spendlove, J C; Spendlove, R S; Barnett, B B

    1982-01-01

    The aerosol stability of two particle forms, infectious and potentially infectious, of reovirus were examined under static conditions for a range of relative humidities at 21 and 24 degrees C. Virus aerosolization efficiency was determined for two methods of dissemination: Collison nebulizer and Chicago atomizer. Suspensions of Bacillus subtilis var. niger spores were added to reovirus preparations that included both particle forms and disseminated into a dynamic aerosol toroid to estimate the physical decay of the aerosols. At 90 to 100% relative humidity, both reovirus particle forms showed less than 10-fold loss of infectivity after 12 h of aging. At lower relative humidities the aerosol decay curve showed rapid initial decay followed by a markedly lower decay rate. Our findings reveal that reovirus particles are relatively stable in the airborne state. PMID:7149719

  1. Fatty acids on continental sulfate aerosol particles

    NASA Astrophysics Data System (ADS)

    Tervahattu, H.; Juhanoja, J.; Vaida, V.; Tuck, A. F.; Niemi, J. V.; Kupiainen, K.; Kulmala, M.; VehkamäKi, H.

    2005-03-01

    Surface analyses of atmospheric aerosols from different continental sources, such as forest fires and coal and straw burning, show that organic surfactants are found on such aerosols. The predominant organic species detected by time-of-flight secondary ion mass spectrometry on the sulfate aerosols are fatty acids of different carbon chain length up to the C32 acid. These observations are consistent with literature accounts of functional group analysis of bulk samples, but this is the first direct evidence of fatty acid films on the surface of sulfate aerosols. Surface analysis leads to the conclusion that fatty acid films on continental aerosols may be more common than has been previously suggested.

  2. Spectro-microscopy of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

    NASA Astrophysics Data System (ADS)

    OBrien, R. E.; Wang, B.; Laskin, A.; West, M.; Riemer, N. S.; Gilles, M. K.; Moffet, R.

    2014-12-01

    Individual aerosol particles are often mixtures of multiple components such as inorganic salts, soot or elemental carbon, and organic molecules. The amounts of the different components in each particle and the particle morphologies will impact the CCN activity and the radiative properties of the aerosol population. A recent parameterization of the mixing state developed by Nicole Riemer and Matthew West provides a clear transition between ambient measurements of aerosol components and particle mixing states employed in climate models. Single particle spectro-microscopy techniques including scanning transmission x-ray microscopy/near-edge x-ray absorption fine structure spectroscopy (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) are used to measure the composition of aerosol particles from the CARES campaign at both T0 and T1. Here, we present results from the application of the per particle composition to a parameterization of the mixing state and provide constraints on the mixing state of ambient aerosol particles. The two microscopy techniques yield complementary information on the mixing state of the aerosol populations; STXM/NEXAFS provides information on the mixing state of the organic fraction while CCSEM/EDX provides information on the inorganic fraction.

  3. [Investigation of Aerosol Mixed State and CCN Activity in Nanjing].

    PubMed

    Zhu, Lin; Ma, Yan; Zheng, Jun; Li, Shi-zheng; Wang, Li-peng

    2016-04-15

    During 11-18 September 2014, the size-resolved aerosol Cloud Condensation Nuclei (CCN) activity and mixing state were measured using Cloud Condensation Nuclei Counter (CCNC), Aerosol Particle Mass (APM) and Scanning Mobility Particle Sizer (SMPS). The results showed that aerosols mainly existed as an internal mixture. For 76, 111, 138 and 181 nm particles, black carbon (BC) accounted for 5.4%, 10%, l0.7% and 6.7% of the particle mass, but as high as 51%, 57%, 70% and 59% of the particle number concentrations, respectively, suggesting that BC was a type of important condensation nuclei in the atmosphere and made significant contributions to particle numbers. The occasionally observed external mixtures were mainly present in 111 and 138 nm particles. The critical supersaturation was 0.25%, 0.13%, 0.06% and 0.015% for 76, 111, 138 and 181 nm particles, respectively. Precipitation and haze had significant effects on the particle CCN activity. The hygroscopicity parameter K was 0.37, 0.29 and 0.39 in rainy, clear and hazy days, respectively. Particle density and CCN activity were impacted by chemical compositions. Compared with clear days, higher contents of inorganic salts and lower contents of organics were found on hazy days, accompanied by lower particle density and higher CCN activity. PMID:27548938

  4. Surface-active organics in atmospheric aerosols.

    PubMed

    McNeill, V Faye; Sareen, Neha; Schwier, Allison N

    2014-01-01

    Surface-active organic material is a key component of atmospheric aerosols. The presence of surfactants can influence aerosol heterogeneous chemistry, cloud formation, and ice nucleation. We review the current state of the science on the sources, properties, and impacts of surfactants in atmospheric aerosols. PMID:23408277

  5. MASS SPECTROMETRY OF INDIVIDUAL AEROSOL PARTICLES. (R823980)

    EPA Science Inventory

    Typically, in real-time aerosol mass spectrometry (RTAMS), individual airborne particles
    are ablated and ionized with a single focused laser pulse. This technique yields information that
    permits bulk characterization of the particle, but information about the particle's sur...

  6. Cloud condensation nuclei (CCN) activity of aliphatic amine secondary aerosol

    NASA Astrophysics Data System (ADS)

    Tang, X.; Price, D.; Praske, E.; Vu, D. N.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-06-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g., hydroxyl radical and nitrate radical). The particle can contain both secondary organic aerosol (SOA) and inorganic salts. The ratio of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ, ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3) contains less volatile compounds than the primary aliphatic amine (BA) aerosol. As relative humidity (RH) increases, inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. The humid BA + N2O5 aerosol products were found to be very sensitive to the temperature at which the measurements were made within the streamwise continuous-flow thermal gradient CCN counter; κ ranges from 0.4 to 0.7 dependent on the instrument supersaturation (ss) settings. The variance of the measured aerosol κ values indicates that simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems' κ ranges within 0.2 < κ < 0.7. This work indicates that aerosols formed via nighttime reactions with amines are likely to produce hygroscopic and volatile aerosol, whereas photochemical reactions with OH produce secondary organic aerosol of lower CCN activity. The contributions of semivolatile secondary organic and inorganic material from aliphatic amines must be considered for accurate hygroscopicity and CCN predictions from aliphatic amine systems.

  7. Equilibrium absorptive partitioning theory between multiple aerosol particle modes

    NASA Astrophysics Data System (ADS)

    Crooks, Matthew; Connolly, Paul; Topping, David; McFiggans, Gordon

    2016-10-01

    An existing equilibrium absorptive partitioning model for calculating the equilibrium gas and particle concentrations of multiple semi-volatile organics within a bulk aerosol is extended to allow for multiple involatile aerosol modes of different sizes and chemical compositions. In the bulk aerosol problem, the partitioning coefficient determines the fraction of the total concentration of semi-volatile material that is in the condensed phase of the aerosol. This work modifies this definition for multiple polydisperse aerosol modes to account for multiple condensed concentrations, one for each semi-volatile on each involatile aerosol mode. The pivotal assumption in this work is that each aerosol mode contains an involatile constituent, thus overcoming the potential problem of smaller particles evaporating completely and then condensing on the larger particles to create a monodisperse aerosol at equilibrium. A parameterisation is proposed in which the coupled non-linear system of equations is approximated by a simpler set of equations obtained by setting the organic mole fraction in the partitioning coefficient to be the same across all modes. By perturbing the condensed masses about this approximate solution a correction term is derived that accounts for many of the removed complexities. This method offers a greatly increased efficiency in calculating the solution without significant loss in accuracy, thus making it suitable for inclusion in large-scale models.

  8. Thermophoretic separation of aerosol particles from a sampled gas stream

    DOEpatents

    Postma, Arlin K.

    1986-01-01

    A method for separating gaseous samples from a contained atmosphere that includes aerosol particles uses the step of repelling particles from a gas permeable surface or membrane by heating the surface to a temperature greater than that of the surrounding atmosphere. The resulting thermophoretic forces maintain the gas permeable surface clear of aerosol particles. The disclosed apparatus utilizes a downwardly facing heated plate of gas permeable material to combine thermophoretic repulsion and gravity forces to prevent particles of any size from contacting the separating plate surfaces.

  9. Redox activity of naphthalene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    McWhinney, R. D.; Zhou, S.; Abbatt, J. P. D.

    2013-04-01

    Chamber secondary organic aerosol (SOA) from low-NOx photooxidation of naphthalene by hydroxyl radical was examined with respect to its redox cycling behaviour using the dithiothreitol (DTT) assay. Naphthalene SOA was highly redox active, consuming DTT at an average rate of 118 ± 14 pmol per minute per μg of SOA material. Measured particle-phase masses of the major previously identified redox active products, 1,2- and 1,4-naphthoquinone, accounted for only 21 ± 3% of the observed redox cycling activity. The redox-active 5-hydroxy-1,4-naphthoquinone was identified as a new minor product of naphthalene oxidation, and including this species in redox activity predictions increased the predicted DTT reactivity to 30 ± 5% of observations. Similar attempts to predict redox behaviour of oxidised two-stroke engine exhaust particles by measuring 1,2-naphthoquinone, 1,4-naphthoquinone and 9,10-phenanthrenequinone predicted DTT decay rates only 4.9 ± 2.5% of those observed. Together, these results suggest that there are substantial unidentified redox-active SOA constituents beyond the small quinones that may be important toxic components of these particles. A gas-to-SOA particle partitioning coefficient was calculated to be (7.0 ± 2.5) × 10-4 m3 μg-1 for 1,4-naphthoquinone at 25 °C. This value suggests that under typical warm conditions, 1,4-naphthoquinone is unlikely to contribute strongly to redox behaviour of ambient particles, although further work is needed to determine the potential impact under conditions such as low temperatures where partitioning to the particle is more favourable. As well, higher order oxidation products that likely account for a substantial fraction of the redox cycling capability of the naphthalene SOA are likely to partition much more strongly to the particle phase.

  10. 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

  11. Formation and growth of indoor air aerosol particles as a result of D-limonene oxidation

    NASA Astrophysics Data System (ADS)

    Vartiainen, E.; Kulmala, M.; Ruuskanen, T. M.; Taipale, R.; Rinne, J.; Vehkamäki, H.

    Oxidation of D-limonene, which is a common monoterpene, can lead to new aerosol particle formation in indoor environments. Thus, products containing D-limonene, such as citrus fruits, air refresheners, household cleaning agents, and waxes, can act as indoor air aerosol particle sources. We released D-limonene into the room air by peeling oranges and measured the concentration of aerosol particles of three different size ranges. In addition, we measured the concentration of D-limonene, the oxidant, and the concentration of ozone, the oxidizing gas. Based on the measurements we calculated the growth rate of the small aerosol particles, which were 3-10 nm in diameter, to be about 6300nmh-1, and the losses of the aerosol particles that were due to the coagulation and condensation processes. From these, we further approximated the concentration of the condensable vapour and its source rate and then calculated the formation rate of the small aerosol particles. For the final result, we calculated the nucleation rate and the maximum number of molecules in a critical cluster. The nucleation rate was in the order of 105cm-3s-1 and the number of molecules in a critical-sized cluster became 1.2. The results were in agreement with the activation theory.

  12. Physicochemical characterization of Capstone depleted uranium aerosols II: particle size distributions as a function of time.

    PubMed

    Cheng, Yung Sung; Kenoyer, Judson L; Guilmette, Raymond A; Parkhurst, Mary Ann

    2009-03-01

    The Capstone Depleted Uranium (DU) Aerosol Study, which generated and characterized aerosols containing DU from perforation of armored vehicles with large-caliber DU penetrators, incorporated a sampling protocol to evaluate particle size distributions. Aerosol particle size distribution is an important parameter that influences aerosol transport and deposition processes as well as the dosimetry of the inhaled particles. These aerosols were collected on cascade impactor substrates using a pre-established time sequence following the firing event to analyze the uranium concentration and particle size of the aerosols as a function of time. The impactor substrates were analyzed using proportional counting, and the derived uranium content of each served as input to the evaluation of particle size distributions. Activity median aerodynamic diameters (AMADs) of the particle size distributions were evaluated using unimodal and bimodal models. The particle size data from the impactor measurements were quite variable. Most size distributions measured in the test based on activity had bimodal size distributions with a small particle size mode in the range of between 0.2 and 1.2 microm and a large size mode between 2 and 15 microm. In general, the evolution of particle size over time showed an overall decrease of average particle size from AMADs of 5 to 10 microm shortly after perforation to around 1 microm at the end of the 2-h sampling period. The AMADs generally decreased over time because of settling. Additionally, the median diameter of the larger size mode decreased with time. These results were used to estimate the dosimetry of inhaled DU particles. PMID:19204485

  13. Single-particle measurements of phase partitioning between primary and secondary organic aerosols.

    PubMed

    Robinson, Ellis Shipley; Donahue, Neil M; Ahern, Adam T; Ye, Qing; Lipsky, Eric

    2016-07-18

    Organic aerosols provide a measure of complexity in the urban atmosphere. This is because the aerosols start as an external mixture, with many populations from varied local sources, that all interact with each other, with background aerosols, and with condensing vapors from secondary organic aerosol formation. The externally mixed particle populations start to evolve immediately after emission because the organic molecules constituting the particles also form thermodynamic mixtures - solutions - in which a large fraction of the constituents are semi-volatile. The external mixtures are thus well out of thermodynamic equilibrium, with very different activities for many constituents, and yet also have the capacity to relax toward equilibrium via gas-phase exchange of semi-volatile vapors. Here we describe experiments employing quantitative single-particle mass spectrometry designed to explore the extent to which various primary organic aerosol particle populations can interact with each other or with secondary organic aerosols representative of background aerosol populations. These methods allow us to determine when these populations will and when they will not mix with each other, and then to constrain the timescales for that mixing.

  14. Carbonaceous aerosol particles from common vegetation in the Grand Canyon

    SciTech Connect

    Hallock, K.A.; Mazurek, M.A.; Cass, G.R.

    1992-05-01

    The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon.

  15. Regional signatures in the organic composition of marine aerosol particles

    NASA Astrophysics Data System (ADS)

    Frossard, Amanda A.; Russell, Lynn M.; Keene, William C.; Kieber, David J.; Quinn, Patricia K.; Bates, Timothy S.

    2013-05-01

    Marine aerosol particles play an important role in the earth's radiative balance, yet the sources and composition of the organic fraction remain largely unconstrained. Recent measurements have been made in order to characterize the sources, composition, and concentration of aerosol particles in the marine boundary layer. The organic composition of submicron particles derived from multiple seawater regions have been measured using Fourier Transform Infrared (FTIR) spectroscopy. Cluster analysis of FTIR organic spectra suggest different spectral signatures based on collection location, seawater composition, and ambient conditions. Measurements including non-refractory aerosol composition from a high-resolution time of flight aerosol mass spectrometer (HR-ToF-AMS), seawater composition, and wind speed were used to interpret the cluster results, depending on the availability from each campaign. FTIR spectra of ambient particles are compared to FTIR spectra of primary marine particles generated from model ocean systems to infer the ambient particle production mechanisms and aging processes. Recent measurements used in the comparison include ambient and generated marine aerosol particles measured off the coast of California during CalNex in May and June 2010. Remote ambient marine aerosol particles were collected 100 miles off the coast of Monterey in the eastern Pacific during the EPEACE experiment in July 2011. Ambient and generated marine particles were measured in two different seawater types during WACS 2012 including colder, more productive water off the coast of the northeastern United States and warmer, oligotrophic water in the Sargasso Sea. These particles are also compared with those measured in the southeastern Pacific during VOCALS and the north Atlantic during ICEALOT.

  16. Transmission electron microscopy study of aerosol particles from the brown hazes in northern China

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Shao, Longyi

    2009-05-01

    Airborne aerosol collections were performed in urban areas of Beijing that were affected by regional brown haze episodes over northern China from 31 May to 12 June 2007. Morphologies, elemental compositions, and mixing states of 810 individual aerosol particles of different sizes were obtained by transmission electron microscopy coupled with energy-dispersive X-ray spectrometry. The phases of some particles were verified using selected-area electron diffraction. Aerosol particle types less than 10 μm in diameter include mineral, complex secondary (Ca-S, K-, and S-rich), organic, soot, fly ash, and metal (Fe-rich and Zn-bearing). Most soot, fly ash, and organic particles are less than 2 μm in diameter. Approximately 84% of the analyzed mineral particles have diameters between 2 and 10 μm, while 81% of the analyzed complex secondary and metal particles are much smaller, from 0.1 to 2 μm. Trajectory analysis with fire maps show that southerly air masses arriving at Beijing have been transported through many agricultural biomass burning sites and heavy industrial areas. Spherical fly ash and Fe-rich particles were from industrial emissions, and abundant K-rich and organic particles likely originated from field burning of crop residues. Abundant Zn-bearing particles are associated with industrial activities and local waste incinerators. On the basis of the detailed analysis of 443 analyzed aerosol particles, about 70% of these particles are internally mixed with two or more aerosol components from different sources. Most mineral particles are covered with visible coatings that contain N, O, Ca (or Mg), minor S, and Cl. K- and S-rich particles tend to be coagulated with fly ash, soot, metal, and fine-grained mineral particles. Organic materials internally mixed with K- and S-rich particles can be their inclusions and coatings.

  17. Simultaneous In-Situ Measurement of Local Particle Size, Particle Concentration, and Velocity of Aerosols.

    PubMed

    Weber; Schweiger

    1999-02-01

    Photon correlation spectroscopy has been applied to the characterization of (quasi-)monodisperse aerosols. The experiments were carried out with an experimental standard pin hole setup on laminar flowing aerosols of the submicrometer particle size range. It is shown that beside local mean particle size and local aerosol velocity simultaneously the local particle number concentration may be obtained from a single measured autocorrelation function. The proposed procedure does not require calibration. It is pointed out that measurement conditions can be adapted to the properties of the aerosol to be characterized, thus allowing characterization of aerosols over a wide parameter range, e.g., it is not restricted to the case of low particle concentration. The experimental results are compared to data from literature, data from reference measurements and data from a theoretical model, respectively. The method can also be usefull for characterization of other fluid-particle systems as hydrosols. Copyright 1999 Academic Press.

  18. Polarization resolved angular optical scattering of aerosol particles

    NASA Astrophysics Data System (ADS)

    Redding, B.; Pan, Y.; Wang, C.; Videen, G.; Cao, Hui

    2014-05-01

    Real-time detection and identification of bio-aerosol particles are crucial for the protection against chemical and biological agents. The strong elastic light scattering properties of airborne particles provides a natural means for rapid, non-invasive aerosol characterization. Recent theoretical predictions suggested that variations in the polarization dependent angular scattering cross section could provide an efficient means of classifying different airborne particles. In particular, the polarization dependent scattering cross section of aggregate particles is expected to depend on the shape of the primary particles. In order to experimentally validate this prediction, we built a high throughput, sampling system, capable of measuring the polarization resolved angular scattering cross section of individual aerosol particles flowing through an interrogating volume with a single shot of laser pulse. We calibrated the system by comparing the polarization dependent scattering cross section of individual polystyrene spheres with that predicted by Mie theory. We then used the system to study different particles types: Polystyrene aggregates composed 500 nm spheres and Bacillus subtilis (BG, Anthrax simulant) spores composed of elongated 500 nm × 1000 nm cylinder-line particles. We found that the polarization resolved scattering cross section depends on the shape of the constituent elements of the aggregates. This work indicates that the polarization resolved scattering cross section could be used for rapid discrimination between different bio-aerosol particles.

  19. LASER DESORPTION IONIZATION OF ULTRAFINE AEROSOL PARTICLES. (R823980)

    EPA Science Inventory

    On-line analysis of ultrafine aerosol particle in the 12 to 150 nm size range is performed by
    laser desorption/ionization. Particles are size selected with a differential mobility analyzer and then
    sent into a linear time-of-flight mass spectrometer where they are ablated w...

  20. Intercomparison of number concentration measurements by various aerosol particle counters

    NASA Astrophysics Data System (ADS)

    Ankilov, A.; Baklanov, A.; Colhoun, M.; Enderle, K.-H.; Gras, J.; Julanov, Yu.; Kaller, D.; Lindner, A.; Lushnikov, A. A.; Mavliev, R.; McGovern, F.; Mirme, A.; O'Connor, T. C.; Podzimek, J.; Preining, O.; Reischl, G. P.; Rudolf, R.; Sem, G. J.; Szymanski, W. W.; Tamm, E.; Vrtala, A. E.; Wagner, P. E.; Winklmayr, W.; Zagaynov, V.

    Total aerosol particle number concentrations, as measured by means of 16 different measurement systems, have been quantitatively compared during an international workshop at the Institute for Experimental Physics of the University of Vienna, Austria, which was coordinated within the Committee on Nucleation and Atmospheric Aerosols (ICCP-IUGG). The range of measuring instruments includes Pollak counters (PCO) in use already for several decades, presently available commercial particle counters, as well as laboratory prototypes. The operation of the instruments considered was based on different measurement principles: (1) adiabatic expansion condensation particle counter, (2) flow diffusion condensation particle counter, (3) turbulent mixing condensation particle counter, (4) laser optical particle counter, and (5) electrostatic particle measurement system. Well-defined test aerosols with various chemical compositions were considered: DEHS, sodium chloride, silver, hydrocarbons, and tungsten oxide. The test aerosols were nearly monodispersed with mean particle diameters between 4 and 520 nm, the particle number concentrations were varied over a range from about 4×10 1 to 7×10 6 cm -3. A few measurements were performed with two-component aerosol mixtures. For simultaneous concentration measurements, the various instruments considered were operated under steady state conditions in a linear flow system. A series of at least 10 single concentration measurements was performed by each individual instrument at each set of test aerosol parameters. The average of the concentration data measured by the various instruments was defined as a common reference. The number concentrations obtained from the various instruments typically agreed within a factor of about two over the entire concentration range considered. The agreement of the measured concentrations is notable considering the various different measurement principles applied in this study, and particularly in view of the

  1. SAGE II aerosol validation - Selected altitude measurements, including particle micromeasurements

    NASA Technical Reports Server (NTRS)

    Oberbeck, Verne R.; Russell, Philip B.; Pueschel, Rudolf F.; Snetsinger, Kenneth G.; Ferry, Guy V.; Livingston, John M.; Rosen, James N.; Osborn, Mary T.; Kritz, Mark A.

    1989-01-01

    The validity of particulate extinction coefficients derived from limb path solar radiance measurements obtained during the Stratospheric Aerosol and Gas Experiment (SAGE) II is tested. The SAGE II measurements are compared with correlative aerosol measurements taken during January 1985, August 1985, and July 1986 with impactors, laser spectrometers, and filter samplers on a U-2 aircraft, an upward pointing lidar on a P-3 aircraft, and balloon-borne optical particle counters. The data for July 29, 1986 are discussed in detail. The aerosol measurements taken on this day at an altitude of 20.5 km produce particulate extinction values which validate the SAGE II values for similar wavelengths.

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

    SciTech Connect

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

    1996-12-31

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

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

    SciTech Connect

    Fung, K.H.

    1999-12-01

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

  4. Reactions and mass spectra of complex particles using Aerosol CIMS

    NASA Astrophysics Data System (ADS)

    Hearn, John D.; Smith, Geoffrey D.

    2006-12-01

    Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

  5. Phosphorus-bearing Aerosol Particles From Volcanic Plumes

    NASA Astrophysics Data System (ADS)

    Obenholzner, J. H.; Schroettner, H.; Poelt, P.; Delgado, H.; Caltabiano, T.

    2003-12-01

    Particles rich in P or bulk geochemical data of volcanic aerosol particles showing high P contents are known from many volcanic plumes (Stanton, 1994; Obenholzner et al., 2003). FESEM/EDS analysis of individual particles obtained from the passively degassing plume of Popocatepetl volcano, Mx. (1997) and from the plume of Stromboli (May 2003) show P frequently. Even at the high resolution of the FESEM, euhedral apatite crystals could not be observed. At Popocatepetl (1997) spherical Ca-P-O particles are common. Fluffy, fractal or botryoidal particles also can contain EDS-detectable amounts of P. The EDS spectrum of such particles can comprise various elements. However most particles show P, S and Cl. P-S and P-S-metal species are known in chemistry but do they occur in volcanic plumes? Stoichiometric considerations had been made in the past suggesting the existence of P-S species in plumes (Stanton 1994), gas sampling and remote gas monitoring systems have not detected yet such molecules in plumes. The particle spectrum of the reawakened Popocateptel volcano might be related to accumulation of volatiles at the top of a magma chamber during the phase of dormancy. P-Fe rich, Ca-free aggregates are also known from the eruption of El Chichon 1982 (SEM/EDS by M. Sheridan, per. comm. 08-24-2003). Persistently active volcanoes (i.e. Stromboli) represent a different category according to continuous degassing and aerosol particle formation. A particle collector ( ca. 90 ml/min) accompanied a COSPEC helicopter flight at Stromboli (May 15, 2003) after one of the rare types of sub-plinian events on April 5 2003. P-bearing particles are very common. For instance, an Fe oxide grain (diam. = 2 æm) is partially covered by fluffy and euhedral P-bearing matter. The elements detected are P, Cl, Na, Mg, Al, Si, K, Ca, Ti and (Fe). The fluffy and the euhedral (rhombohedral?) matter show in SE-BSE-mix image almost identical grey colors. At Stromboli and Popocatepetl particles on which

  6. [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.

  7. Limits of DPUI application associated with the number of particles within actinide aerosols.

    PubMed

    Fritsch, P; Raynaud, P; Blanchin, N; Mièle, A

    2007-01-01

    Dose per unit intake (DPUI) of radionuclides is obtained using International Commission on Radiological Protection (ICRP) models. After inhalation exposure, the first model calculates the fraction of activity deposited within the different regions of the respiratory tract, assuming that the aerosol contains an infinite number of particles. Using default parameters for workers, an exposure to one annual limit of intake (ALI) corresponds to an aerosol of 239PuO2 containing approximately 1 x 10(6) particles. To reach such an exposure, very low particle number might be involved especially for compounds having a high specific activity. This study provides examples of exposures to actinide aerosols for which the number of particles is too low for a standard application of the ICRP model. These examples, which involve physical studies of aerosols collected at the workplace and interpretation of bioassay data, show that the number of particles of the aerosol can be the main limit for the application of DPUI after inhalation exposure.

  8. 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

  9. Influence of refractive index on the accuracy of size determination of aerosol particles with light-scattering aerosol counters.

    PubMed

    Quenzel, H

    1969-01-01

    The scattering properties of single aerosol particles with different indices of refraction have been computed from the Mie theory considering the spectral response of light-scattering aerosol counters commercially available. It is demonstrated that high resolution of the aerosol size distribution is impossible, particularly because of the different refractive indices of the atmospheric aerosol particles. By using other ranges of scattering angle for the measurement, one may, in some cases, obtain better results.

  10. Thermophoretic separation of aerosol particles from a sampled gas stream

    DOEpatents

    Postma, A.K.

    1984-09-07

    This disclosure relates to separation of aerosol particles from gas samples withdrawn from within a contained atmosphere, such as containment vessels for nuclear reactors or other process equipment where remote gaseous sampling is required. It is specifically directed to separation of dense aerosols including particles of any size and at high mass loadings and high corrosivity. The United States Government has rights in this invention pursuant to Contract DE-AC06-76FF02170 between the US Department of Energy and Westinghouse Electric Corporation.

  11. 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

    , extending over more than twelve years of MISR data, aid in the assessment. Comparisons with the limited available AERONET aerosol type data are also made and evaluated as appropriate. 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 Goddard Space Flight Center.

  12. New aerosol particles formation in the Sao Paulo Metropolitan Area

    NASA Astrophysics Data System (ADS)

    Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

    2016-04-01

    The Sao Paulo Metropolitan Area (SPMA), in the southeast region of Brazil, is considered a megalopolis comprised of Sao Paulo city and more 38 municipalities. The air pollutant emissions in the SPMA are related to the burning of the fuels: etanol, gasohol (gasoline with 25% ethanol) and diesel. According to CETESB (2013), the road vehicles contributed up to about 97, 87, and 80% of CO, VOCs and NOx emissions in 2012, respectively, being most of NOx associated to diesel combustion and most of CO and VOCs from gasohol and ethanol combustion. Studies conducted on ambient air pollution in the SPMA have shown that black carbon (BC) explains 21% of mass concentration of PM2.5 compared with 40% of organic carbon (OC), 20% of sulfates, and 12% of soil dust (Andrade et al., 2012). Most of the observed ambient PM2.5 mass concentration usually originates from precursors gases such as sulphur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOx) and VOCs as well as through the physico-chemical processes such as the oxidation of low volatile hydrocarbons transferring to the condensed phase (McMurry et al., 2004). The Weather Research and Forecasting with Chemistry model (WRF-Chem; Grell et al. 2005), configured with three nested grid cells: 75, 15, and 3 km, is used as photochemical modeling to describe the physico-chemical processes leading to evolution of particles number and mass size distribution from a vehicular emission model developed by the IAG-USP laboratory of Atmospheric Processes and based on statistical information of vehicular activity. The spatial and temporal distributions of emissions in the finest grid cell are based on road density products compiled by the OpenStreetMap project and measurements performed inside tunnels in the SPMA, respectively. WRF-Chem simulation with coupled primary aerosol (dust and sea-salt) and biogenic emission modules and aerosol radiative effects turned on is conducted as the baseline simulation (Case_0) to evaluate the model

  13. FTIR Analysis of Functional Groups in Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Shokri, S. M.; McKenzie, G.; Dransfield, T. J.

    2012-12-01

    Secondary organic aerosols (SOA) are suspensions of particulate matter composed of compounds formed from chemical reactions of organic species in the atmosphere. Atmospheric particulate matter can have impacts on climate, the environment and human health. Standardized techniques to analyze the characteristics and composition of complex secondary organic aerosols are necessary to further investigate the formation of SOA and provide a better understanding of the reaction pathways of organic species in the atmosphere. While Aerosol Mass Spectrometry (AMS) can provide detailed information about the elemental composition of a sample, it reveals little about the chemical moieties which make up the particles. This work probes aerosol particles deposited on Teflon filters using FTIR, based on the protocols of Russell, et al. (Journal of Geophysical Research - Atmospheres, 114, 2009) and the spectral fitting algorithm of Takahama, et al (submitted, 2012). To validate the necessary calibration curves for the analysis of complex samples, primary aerosols of key compounds (e.g., citric acid, ammonium sulfate, sodium benzoate) were generated, and the accumulated masses of the aerosol samples were related to their IR absorption intensity. These validated calibration curves were then used to classify and quantify functional groups in SOA samples generated in chamber studies by MIT's Kroll group. The fitting algorithm currently quantifies the following functionalities: alcohols, alkanes, alkenes, amines, aromatics, carbonyls and carboxylic acids.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

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

    DOE PAGES

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

    2016-03-22

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

  16. Selection of quasi-monodisperse super-micron aerosol particles

    NASA Astrophysics Data System (ADS)

    Rösch, Michael; Pfeifer, Sascha; Wiedensohler, Alfred; Stratmann, Frank

    2014-05-01

    Size-segregated quasi monodisperse particles are essential for e.g. fundamental research concerning cloud microphysical processes. Commonly a DMA (Differential Mobility Analyzer) is used to produce quasi-monodisperse submicron particles. Thereto first, polydisperse aerosol particles are bipolarly charged by a neutralizer, and then selected according to their electrical mobility with the DMA [Knutson et al. 1975]. Selecting a certain electrical mobility with a DMA results in a particle size distribution, which contains singly charged particles as well as undesired multiply charged larger particles. Often these larger particles need to either be removed from the generated aerosol or their signals have to be corrected for in the data inversion and interpretation process. This problem becomes even more serious when considering super-micron particles. Here we will present two different techniques for generating quasi-monodisperse super-micron aerosol particles with no or only an insignificant number of larger sized particles being present. First, we use a combination of a cyclone with adjustable aerodynamic cut-off diameter and our custom-built Maxi-DMA [Raddatz et al. 2013]. The cyclone removes particles larger than the desired ones prior to mobility selection with the DMA. This results in a reduction of the number of multiply charged particles of up to 99.8%. Second, we utilize a new combination of cyclone and PCVI (Pumped Counterflow Virtual Impactor), which is based on purely inertial separation and avoids particle charging. The PCVI instrument was previously described by Boulter et al. (2006) and Kulkarni et al. (2011). With our two setups we are able to produce quasi-monodisperse aerosol particles in the diameter range from 0.5 to 4.4 µm without a significant number of larger undesired particles being present. Acknowledgements: This work was done within the framework of the DFG funded Ice Nucleation research UnIT (INUIT, FOR 1525) under WE 4722/1-1. References

  17. Single particle atmospheric aerosol analysis using digital holographic microscopy

    NASA Astrophysics Data System (ADS)

    Mihailescu, Mona; Cojocaru, Ruxandra Elena; Kusko, C.; Toanca, Flori; Dinescu, A.; Schiopu, P.

    2011-06-01

    The aim of this research is to calculate the refractive index of transparent atmospheric aerosols, which have biological origin, using a digital holographic microscopy technique (DHM). The samples are collected on filters, using miniature impactors for particles with dimensions smaller than 10μm (on even one axis), from a height of over 20 meters, in Magurele, a rural location near the urban and industrial agglomeration of the capital city, Bucharest. Due to their organic or inorganic origin, each atmospheric aerosol particle has different size, shape and optical properties which have a determinant role in LIDAR measurements. We record on a CCD camera hundreds of holograms which contain the diffraction pattern from every aerosol particle superposed with the reference wave. Digitally, we scan the entire volume of one particle with nanometric resolution (using an algorithm based on the Fresnel approximation). The calibration was done using an object with known dimensions fabricated by e-beam lithography and some complementary measurements were done in confocal microscopy. Our analysis separates four main classes of atmospheric aerosols particles (wires, columns, spherical fragments, and irregular). The predominant class in the investigated period is the first one, which has biological origin and the refractive index was calculated starting from the phase shift introduced by them in the optical path and models for their cylindrical shape. The influence of spatial filtering in the reconstructed object images was investigated.

  18. Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

    NASA Astrophysics Data System (ADS)

    Wollny, A. G.; Garland, R.; Pöschl, U.

    2009-04-01

    Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

  19. The weather dependence of particle size distribution of indoor radioactive aerosol associated with radon decay products.

    PubMed

    Mostafa, A M A; Tamaki, K; Moriizumi, J; Yamazawa, H; Iida, T

    2011-07-01

    This study was performed to measure the activity size distribution of aerosol particles associated with short-lived radon decay products in indoor air at Nagoya University, Nagoya, Japan. The measurements were performed using a low pressure Andersen cascade impactor under variable meteorological conditions. The results showed that the greatest activity fraction was associated with aerosol particles in the accumulation size range (100-1000 nm) with a small fraction of nucleation mode (10-100 nm). Regarding the influence of the weather conditions, the decrease in the number of accumulation particles was observed clearly after rainfall without significant change in nucleation particles, which may be due to a washout process for the large particles.

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

    PubMed

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

    2016-09-20

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

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

    PubMed

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

    2016-09-20

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

  2. New Particle Formation and Secondary Organic Aerosol in Beijing

    NASA Astrophysics Data System (ADS)

    Hu, M.; Yue, D.; Guo, S.; Hu, W.; Huang, X.; He, L.; Wiedensohler, A.; Zheng, J.; Zhang, R.

    2011-12-01

    Air pollution in Beijing has been a major concern due to being a mega-city and green Olympic Games requirements. Both long term and intensive field measurements have been conducted at an Urban Air Quality Monitoring Station in the campus of Peking University since 2004. Aerosol characteristics vary seasonally depending on meteorological conditions and source emissions. Secondary compositions of SNA (sum of sulfate, nitrate, and ammonium) and SOA (secondary organic aerosol) become major fraction of fine particles, which may enhance aerosol impacts on visibility and climate change. The transformation processes of new particle formation (NPF) and secondary organic aerosol have been focused on. It was found that gaseous sulfuric acid, ammonia, and organic compounds are important precursors to NPF events in Beijing and H2SO4-NH3-H2O ternary nucleation is one of the important mechanisms. The contributions of condensation and neutralization of sulfuric acid, coagulation, and organics to the growth of the new particles are estimated as 45%, 34%, and 21%, respectively. Tracer-based method to estimate biogenic and anthropogenic SOA was established by using gas chromatography-mass spectrometry. Secondary organic tracers derived from biogenic (isoprene, α-pinene, β-caryophyllene) and anthropogenic (toluene) contributed 32% at urban site and 35% at rural site, respectively. Other source apportionment techniques were also used to estimate secondary organic aerosols, including EC tracer method, water soluble organic carbon content, chemical mass balance model, and AMS-PMF method.

  3. 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.

  4. Simulating the Evolution of Soot Mixing State with a Particle-Resolved Aerosol Model

    SciTech Connect

    Riemer, Nicole; West, Matt; Zaveri, Rahul A.; Easter, Richard C.

    2009-05-05

    The mixing state of soot particles in the atmosphere is of crucial importance for assessing their climatic impact, since it governs their chemical reactivity, cloud condensation nuclei activity and radiative properties. To improve the mixing state representation in models, we present a new approach, the stochastic particle-resolved model PartMC-MOSAIC, which explicitly resolves the composition of individual particles in a given population of different types of aerosol particles. This approach accurately tracks the evolution of the mixing state of particles due to emission, dilution, condensation and coagulation. To make this direct stochastic particle-based method practical, we implemented a new multiscale stochastic coagulation method. With this method we achieved optimal efficiency for applications when the coagulation kernel is highly non-uniform, as is the case for many realistic applications. PartMC-MOSAIC was applied to an idealized urban plume case representative of a large urban area to simulate the evolution of carbonaceous aerosols of different types due to coagulation and condensation. For this urban plume scenario we quantified the individual processes that contribute to the aging of the aerosol distribution, illustrating the capabilities of our modeling approach. The results showed for the first time the multidimensional structure of particle composition, which is usually lost in internally-mixed sectional or modal aerosol models.

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

    NASA Astrophysics Data System (ADS)

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

    2012-09-01

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

  6. TEM Study of Aerosol Particles in Brown Haze Episodes over Northern China in Spring 2007

    NASA Astrophysics Data System (ADS)

    Li, W.; Shao, L.; Buseck, P. R.

    2008-12-01

    Airborne aerosol collections were performed in eight brown haze episodes from 31 May to 21 June 2007 in Beijing, China. Morphologies, compositions, and mixing states of individual aerosol particles having different sizes were obtained using transmission electron microscopy (TEM). Aerosol particle types less than 2 μ m in diameter include mineral dust, fly ash, soot, organic material, and K-rich, S-rich, and metal particles (Fe- and Zn-rich). Mineral dust particles dominate in the range of 2 to 10 μ m. In addition to finding contributions from vehicle emissions and soil dust in Beijing, TEM results from the study provide new insights into sources such as agricultural biomass burning, industrial activities, and waste incineration. These sources can contribute not only great amounts of K-rich and metal particles but also reactive gases such as NH3, NOx, SO2, and VOCs to the haze. More than 80% of the analyzed aerosol particles are internally mixed. K- and S-rich particles tend to be coagulated with fly ash, soot, metal, and fine-grained mineral dust particles. Organic materials can act as inclusions in the K- and S-rich particles and their coatings. Over 90% of the analyzed internally mixed mineral particles are covered with Ca-, Mg-, or Na-rich coatings, and only 8% are associated with K- or S-rich coatings. The compositions of Ca-, Mg-, and Na-rich coatings suggest that they are possibly nitrates mixed with minor sulfates and chlorides. Calcium sulfate particles with diameters from 10 to 500 nm were also detected within Ca(NO3)2 and Mg(NO3)2 coatings. These results indicate that mineral dust particles in the brown haze episodes participated in heterogeneous reactions in the atmosphere with one or more of SO2, NO2, HCl, and HNO3. The development of coatings altered some mineral dust particles from hydrophobic to hydrophilic.

  7. Processing of aerosol particles within the Habshan pollution plume

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

  8. Organic aerosol mixing observed by single-particle mass spectrometry.

    PubMed

    Robinson, Ellis Shipley; Saleh, Rawad; Donahue, Neil M

    2013-12-27

    We present direct measurements of mixing between separately prepared organic aerosol populations in a smog chamber using single-particle mass spectra from the high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Docosane and docosane-d46 (22 carbon linear solid alkane) did not show any signs of mixing, but squalane and squalane-d62 (30 carbon branched liquid alkane) mixed on the time scale expected from a condensational-mixing model. Docosane and docosane-d46 were driven to mix when the chamber temperature was elevated above the melting point for docosane. Docosane vapors were shown to mix into squalane-d62, but not the other way around. These results are consistent with low diffusivity in the solid phase of docosane particles. We performed mixing experiments on secondary organic aerosol (SOA) surrogate systems finding that SOA derived from toluene-d8 (a surrogate for anthropogenic SOA (aSOA)) does not mix into squalane (a surrogate for hydrophobic primary organic aerosol (POA)) but does mix into SOA derived from α-pinene (biogenic SOA (bSOA) surrogate). For the aSOA/POA, the volatility of either aerosol does not limit gas-phase diffusion, indicating that the two particle populations do not mix simply because they are immiscible. In the aSOA/bSOA system, the presence of toluene-d8-derived SOA molecules in the α-pinene-derived SOA provides evidence that the diffusion coefficient in α-pinene-derived SOA is high enough for mixing on the time scale of 1 min. The observations from all of these mixing experiments are generally invisible to bulk aerosol composition measurements but are made possible with single-particle composition data.

  9. Impact of aerosols and atmospheric particles on plant leaf proteins

    NASA Astrophysics Data System (ADS)

    Yan, Xing; Shi, Wen Z.; Zhao, Wen J.; Luo, Na N.

    2014-05-01

    Aerosols and atmospheric particles can diffuse and absorb solar radiation, and directly affect plant photosynthesis and related protein expression. In this study, for the first time, we performed an extensive investigation of the effects of aerosols and atmospheric particles on plant leaf proteins by combining Geographic Information System and proteomic approaches. Data on particles with diameters of 0.1-1.0 μm (PM1) from different locations across the city of Beijing and the aerosol optical depth (AOD) over the past 6 years (2007-2012) were collected. In order to make the study more reliable, we segregated the influence of soil pollution by measuring the heavy metal content. On the basis of AOD and PM1, two regions corresponding to strong and weak diffuse solar radiations were selected for analyzing the changes in the expression of plant proteins. Our results demonstrated that in areas with strong diffuse solar radiations, plant ribulose bisphosphate carboxylase was expressed at higher levels, but oxygen evolved in enhancer protein and light-harvesting complex II protein were expressed at lower levels. The expression of ATP synthase subunit beta and chlorophyll a-b binding protein were similar in both regions. By analyzing the changes in the expression of these leaf proteins and their functions, we conclude that aerosols and atmospheric particles stimulate plant photosynthesis facilitated by diffuse solar radiations.

  10. Light Absorption of Biogenic Aerosol Particles in Amazonia

    NASA Astrophysics Data System (ADS)

    Holanda, B. A.; Artaxo, P.; Ferreira De Brito, J.; Barbosa, H. M.; Andreae, M. O.; Saturno, J.; Pöhlker, C.; Holben, B. N.; Schafer, J.

    2014-12-01

    Aerosol absorption is a key issue in proper calculation of aerosol radiative forcing. Especially in the tropics with the dominance of natural biogenic aerosol and brown carbon, the so called anomalous absorption is of particular interest. A special experiment was designed to study the wavelength dependence of aerosol absorption for PM2.5 as well as for PM10 particles in the wet season in Central Amazonia. Aerosol analysis occurred from May to August 2014, in the ZF2 ecological reservation, situated at about 55 km North of Manaus in very pristine conditions Two 7 wavelengths AE33 Aethalometers were deployed measuring in parallel, but with a PM2.5 and PM10 inlets. Two MAAP (Multiangle Aerosol Absorption Photometer) were operated in parallel with the AE33 exactly at the same PM2.5 and PM10 inlets. Organic and elemental carbon was analyzed using collection with quartz filters and analysis using a Sunset OC/EC analyzer. Aerosol light scattering for 3 wavelengths was measured using Air Photon and TSI Nephelometers. Aerosol size distribution was measured with one TSI SMPS and a GRIMM OPC to have the size range from 10 nm to 10 micrometers. Particles were measured under dry conditions using diffusion dryers. Aerosol optical depth and absorption was also measured with an AERONET sunphotometer operated close to the site. As the experiment was run in the wet season, very low equivalent black carbon (EBC) were measured, with average concentrations around 50 ng/m³ during May, increasing to 130 ng/m³ in June and July. The measurements adjusted for similar wavelengths shows excellent agreement between the MAAP and AE33 for both inlets (PM2.5 and PM10). It was not possible statistically infer absorption from the coarse mode biogenic particles, since the absorption was completely dominated by fine mode particles. AERONET measurements shows very low values of AOD, at 0.17 at 500 nm and 0.13 at 870 nm, with very low absorption AOD values at 0.00086 at 676 nm and 0.0068 at 872 nm

  11. Dominant Aerosol Particle Type/Mixture Identification at Worldwide Locations Using the Aerosol Robotic Network (AERONET)

    NASA Astrophysics Data System (ADS)

    Giles, D. M.; Holben, B.; Eck, T. F.; Sinyuk, A.; Smirnov, A.; Slutsker, I.; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

    2011-12-01

    Aerosol absorption results in atmospheric heating for various forms of particulate matter - we address means of partitioning mineral dust, pollution (e.g., black and brown carbon), and mixtures of the two using remote sensing techniques. Remotely sensed spectral aerosol optical depth (AOD) and single scattering albedo (SSA) derived from Aerosol Robotic Network (AERONET) sun photometer measurements can be used to calculate the absorption aerosol optical depth (AAOD) at 440, 675, and 870 nm. The spectral change in AAOD with wavelength on logarithmic scales provides the absorption Angstrom exponent (AAE). Recently, a few studies have shown that the relationship between aerosol absorption (i.e., AAE or SSA) and aerosol size [i.e., Angstrom exponent (AE) or fine mode fraction (FMF) of the AOD] can estimate the dominant aerosol particle types/mixtures (i.e., dust, pollution, and dust and pollution mixtures) [Bergstrom et al., 2007; Russell et al., 2010; Lee et al. 2010; Giles et al., 2011]. To evaluate these methods, approximately 20 AERONET sites were grouped into various aerosol categories (i.e., dust, mixed, urban/industrial, and biomass burning) based on aerosol types/mixtures identified in previous studies. For data collected between 1999 and 2010, the long-term data set was analyzed to determine the magnitude of spectral AAOD, perform a sensitivity study on AAE by varying the spectral AOD and SSA, and identify dominant aerosol particle types/mixtures. An assessment of the spectral AAOD showed, on average, that the mixed (dust and pollution) category had the highest absorption (AAE ~1.5) followed by biomass burning (AAE~1.3), dust (AAE~1.7), and urban/industrial (AAE~1.2) categories with AAOD (440 nm) varying between 0.03 and 0.09 among these categories. Perturbing input parameters based on the expected uncertainties for AOD (±0.01) and SSA [±0.03; for cases where AOD(440 nm)>0.4], the sensitivity study showed the perturbed AAE mean varied from the unperturbed

  12. Indoor/outdoor radon decay products associated aerosol particle-size distributions and their relation to total number concentrations.

    PubMed

    Moriizumi, Jun; Yamada, Shinya; Xu, Yang; Matsuki, Satoru; Hirao, Shigekazu; Yamazawa, Hiromi

    2014-07-01

    The activity size distributions of indoor and outdoor radioactive aerosol associated with short-lived radon decay products were observed at Nagoya, Japan, for some periods from 2010 to 2012, following the indoor observation by Mostafa et al. [Mostafa, A. M. A., Tamaki, K., Moriizumi, J., Yamazawa, H. and Iida, T. The weather dependence of particle size distribution of indoor radioactive aerosol associated with radon decay products. Radiat. Prot. Dosim. 146: (1-3), 19-22 (2011)]. The tendency of smaller indoor activity median aerodynamic diameter (AMAD) after rainfalls showed in the previous study was not consistently obtained, while the consistent tendency of less indoor radioactive particles with diameters in the accumulation mode was observed again after rainfalls. The indoor aerosols showed activity size distributions similar to the outdoor ones. Non-radioactive aerosol particle concentrations measured with a laser particle counter suggested a somewhat liner relationship with AMAD.

  13. Lightning activity and aerosols over the Mediterranean

    NASA Astrophysics Data System (ADS)

    Proestakis, Emmanouil; Kazadzis, Stelios; Kotroni, Vassiliki; Lagouvardos, Kostas; Kazantzidis, Andreas

    2015-04-01

    Lightning activity has received extended scientific attention over the past decades. Several international studies on lightning activity and initiation mechanisms have related the increased aerosol concentrations to lightning enhancement. In the frame of TALOS project, we investigated the effect of aerosols on lightning activity over the Mediterranean Sea. Cloud to ground lightning activity data from ZEUS lightning detection network operated and maintained by the National Observatory of Athens, were used along with atmospheric optical depth (AOD) data retrieved by MODIS, on board Aqua satellite. The analysis covers a period of nine years, spanning from 2005 up to 2013. The results show the importance of aerosols in lightning initiation and enhancement. It is shown that the mean AOD of the days with lightning activity per season is larger than the mean seasonal AOD in 90% of the under study domain. Furthermore, lightning activity increase with increasing aerosol loading was found to be more pronounced during summertime and for atmospheric optical depth values up to 0.4. Additionally, during summertime, the spatial analysis showed that the percentage of days with lightning activity is increasing with increasing aerosol loading. Finally, time series for the period 2005-2013 of the days with lightning activity and AOD differences showed similar temporal behavior. Overall, both the spatial and temporal analysis showed that lightning activity is correlated to aerosol loading and that this characteristic is consistent for all seasons.

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

    NASA Astrophysics Data System (ADS)

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

    2011-01-01

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

  15. Single particle multichannel bio-aerosol fluorescence sensor

    NASA Astrophysics Data System (ADS)

    Kaye, P. H.; Stanley, W. R.; Hirst, E.; Foot, E. V.; Baxter, K. L.; Barrington, S. J.

    2005-05-01

    We describe a prototype low-cost multi-channel aerosol fluorescence sensor designed for unattended deployment in medium to large area bio-aerosol detection networks. Individual airborne particles down to ~1μm in size are detected and sized by measurement of light scattered from a continuous-wave diode laser (660nm). This scatter signal is then used to trigger the sequential firing of two xenon sources which irradiate the particle with UV pulses at ~280 nm and ~370 nm, optimal for excitation of bio-fluorophores tryptophan and NADH (nicotinamide adenine dinucleotide) respectively. For each excitation wavelength, fluorescence is detected across two bands embracing the peak emissions of the same bio-fluorophores. Current measurement rates are up to ~125 particles/s, corresponding to all particles for concentrations up to 1.3 x 104 particles/l. Developments to increase this to ~500 particles/s are in hand. Device sensitivity is illustrated in preliminary data recorded from aerosols of E.coli, BG spores, and a variety of non-biological materials.

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

    NASA Astrophysics Data System (ADS)

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

    2012-04-01

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

  17. Measurements of aerosol chemistry during new particle formation events at a remote rural mountain site.

    PubMed

    Creamean, Jessie M; Ault, Andrew P; Ten Hoeve, John E; Jacobson, Mark Z; Roberts, Gregory C; Prather, Kimberly A

    2011-10-01

    Determining the major sources of particles that act as cloud condensation nuclei (CCN) represents a critical step in the development of a more fundamental understanding of aerosol impacts on cloud formation and climate. Reported herein are direct measurements of the CCN activity of newly formed ambient particles, measured at a remote rural site in the Sierra Nevada Mountains of Northern California. Nucleation events in the winter of 2009 occurred during two pristine periods following precipitation, with higher gas-phase SO(2) concentrations during the second period, when faster particle growth occurred (7-8 nm/h). Amines, as opposed to ammonia, and sulfate were detected in the particle phase throughout new particle formation (NPF) events, increasing in number as the particles grew to larger sizes. Interestingly, long-range transport of SO(2) from Asia appeared to potentially play a role in NPF during faster particle growth. Understanding the propensity of newly formed particles to act as CCN is critical for predicting the effects of NPF on orographic cloud formation during winter storms along the Sierra Nevada Mountain range. The potential impact of newly formed particles in remote regions needs to be compared with that of transported urban aerosols when evaluating the impact of aerosols on clouds and climate.

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

    PubMed

    Dette, Hans P; Koop, Thomas

    2015-05-14

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

  19. Impeded ice nucleation in glassy and highly viscous aerosol particles: the role of water diffusion

    NASA Astrophysics Data System (ADS)

    Marcolli, C.; Peter, T.; Zobrist, B.; Krieger, U. K.; Luo, B. P.; Soonsin, V.; Pedernera, D. A.; Koop, T.

    2010-05-01

    In situ and remote observations in the upper troposphere have disclosed the existence of water vapor pressures up to and even above water saturation. Under such conditions ice particle formation by homogeneous nucleation is expected to set in followed by ice crystal growth until the supersaturation is consumed. While the highest measured water vapor values might not withstand rigorous quality checks, values up to water saturation seem to be occurring. Since air masses appear to contain sufficient numbers of aerosol particles for cloud formation, the question arises why these aerosols are not successful at nucleating ice. The atmospheric aerosol is a complex mixture of various inorganic and organic components, whereas the organic fraction can represent more than 50% of the total aerosol mass. The homogeneous ice nucleation threshold was established for atmospherically relevant salt solutions and sulfuric acid, but only for a few organic species. The organic aerosol fraction tends to remain liquid instead of crystallizing as the temperature is decreased and, thus, organic aerosol particles may form highly viscous liquids. When the viscosity of such liquids reaches values in the order of 1012 Pa s, the molecular motion becomes so slow, that the sample vitrifies at the glass transition temperature Tg. If aerosol particles were present as glasses, this would influence several physical and chemical processes in the atmosphere significantly: Water uptake from the gas phase would be drastically impeded and ice nucleation inhibited. We investigated the glass transition temperature of a series of aqueous organic solutions such as polyols, sugars and dicarboxylic acids as a function of the solute concentration using a differential scanning calorimeter (DSC). These measurements show that the higher the molar mass of the organic solutes, the higher Tg of their respective solutions at a given water activity. Aerosol particles containing larger (≥150 g mol-1) organic molecules

  20. Dispersion of aerosol particles in the atmosphere: Fukushima

    NASA Astrophysics Data System (ADS)

    Haszpra, Tímea; Lagzi, István; Tél, Tamás

    2013-04-01

    Investigation of dispersion and deposition of aerosol particles in the atmosphere is an essential issue, because they have an effect on the biosphere and atmosphere. Moreover, aerosol particles have different transport properties and chemical and physical transformations in the atmosphere compared to gas phase air pollutants. The motion of a particle is described by a set of ordinary differential equations. The large-scale dynamics in the horizontal direction can be described by the equations of passive scalar advection, but in the vertical direction a well-defined terminal velocity should be taken into account as a term added to the vertical wind component. In the planetary boundary layer turbulent diffusion has an important role in the particle dispersion, which is taken into account by adding stochastic terms to the deterministic equations above. Wet deposition is also an essential process in the lower levels of the atmosphere, however, its precise parameterization is a challenge. For the simulations the wind field and other necessary data were taken from the ECMWF ERA-Interim database. In the case of the Fukushima Daiichi nuclear disaster (March-April 2011) radioactive aerosol particles were also released in the planetary boundary layer. Simulations (included the continuous and varying emission from the nuclear power plant) will be presented for the period of 14-23 March. Results show that wet deposition also has to be taken into consideration in the lower levels of the atmosphere. Furthermore, dynamical system characteristics are evaluated for the aerosol particle dynamics. The escape rate of particles was estimated both with and without turbulent diffusion, and in both cases when there was no wet deposition and also when wet deposition was taken into consideration.

  1. Design of Aerosol Particle Coating: Thickness, Texture and Efficiency

    PubMed Central

    Buesser, B.; Pratsinis, S.E.

    2013-01-01

    Core-shell particles preserve the performance (e.g. magnetic, plasmonic or opacifying) of a core material while modifying its surface with a shell that facilitates (e.g. by blocking its reactivity) their incorporation into a host liquid or polymer matrix. Here coating of titania (core) aerosol particles with thin silica shells (films or layers) is investigated at non-isothermal conditions by a trimodal aerosol dynamics model, accounting for SiO2 generation by gas phase and surface oxidation of hexamethyldisiloxane (HMDSO) vapor, coagulation and sintering. After TiO2 particles have reached their final primary particle size (e.g. upon completion of sintering during their flame synthesis), coating starts by uniformly mixing them with HMDSO vapor that is oxidized either in the gas phase or on the particles’ surface resulting in SiO2 aerosols or deposits, respectively. Sintering of SiO2 deposited onto the core TiO2 particles takes place transforming rough into smooth coating shells depending on process conditions. The core-shell characteristics (thickness, texture and efficiency) are calculated for two limiting cases of coating shells: perfectly smooth (e.g. hermetic) and fractal-like. At constant TiO2 core particle production rate, the influence of coating weight fraction, surface oxidation and core particle size on coating shell characteristics is investigated and compared to pertinent experimental data through coating diagrams. With an optimal temperature profile for complete precursor conversion, the TiO2 aerosol and SiO2-precursor (HMDSO) vapor concentrations have the strongest influence on product coating shell characteristics. PMID:23729833

  2. Spatial and Temporal Variability of Aerosol Particles in Arctic Spring

    SciTech Connect

    Shantz, Nicole C.; Gultepe, Ismail; Liu, Peter; Earle, Michael; Zelenyuk, Alla

    2012-10-01

    The objective of this work is to investigate the variability in the particle number concentration that may affect climate change assessment for Arctic regions. The Indirect and Semi-Direct Aerosol Campaign (ISDAC) was conducted in April 2008, in the vicinities of Fairbanks and Barrow, Alaska. Measurements of particle number concentrations and size distributions were conducted using a Passive Cavity Aerosol Spectrometer Probe (PCASP-100X) mounted under the Convair-580 aircraft wing. Total number concentration of particles (Na) with diameters in the range 0.12-3 μm was determined for polluted and clean air masses during times when the air was free of clouds and/or precipitation. Variability in Na was considered for both vertical profiles and constant altitude (horizontal) flight legs. This variability can have important implications for estimates of particle properties used in global climate model (GCM) simulations. When aerosol particle layers were encountered, Na rapidly increased from 25 cm-3 up to 550 cm-3 within relatively clean air masses, and reached up to 2200 cm-3 within polluted air masses, dominated by biomass burning pollution. When averaging Na over different distance scales, it was found that Na=140 cm-3 represent an average value for the majority of the encountered clean cases; while Na=720 cm-3 is a mean for polluted cases dominated by biomass burning plumes. These estimates, however, would not capture the details of particle layers encountered during most of the flights. Average aerosol particle characteristics can be difficult to interpret, especially during polluted cases, due to small-scale spatial and temporal variability.

  3. Characterization of aerosol particles at the forested site in Lithuania

    NASA Astrophysics Data System (ADS)

    Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

    2009-04-01

    Atmospheric particulate matter (PM), especially fine particles (particles with aerodynamic diameter less than 1 m, PM1), has been found to play an important role in global climate change, air quality, and human health. The continuous study of aerosol parameters is therefore imperative for better understanding the environmental effects of the atmospheric particles, as well as their sources, formation and transformation processes. The particle size distribution is particularly important, since this physical parameter determines the mass and number density, lifetime and atmospheric transport, or optical scattering behavior of the particles in the atmosphere (Jaenicke, 1998). Over the years several efforts have been made to improve the knowledge about the chemical composition of atmospheric particles as a function of size (Samara and Voutsa, 2005) and to characterize the relative contribution of different components to the fine particulate matter. It is well established that organic materials constitute a highly variable fraction of the atmospheric aerosol. This fraction is predominantly found in the fine size mode in concentrations ranging from 10 to 70% of the total dry fine particle mass (Middlebrook et al., 1998). Although organic compounds are major components of the fine particles, the composition, formation mechanism of organic aerosols are not well understood. This is because particulate organic matter is part of a complex atmospheric system with hundreds of different compounds, both natural and anthropogenic, covering a wide range of chemical properties. The aim of this study was to characterize the forest PM1, and investigate effects of air mass transport on the aerosol size distribution and chemical composition, estimate and provide insights into the sources and characteristics of carbonaceous aerosols through analysis ^13C/12C isotopic ratio as a function of the aerosol particles size. The measurements were performed at the Rugšteliškis integrated

  4. Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

    NASA Astrophysics Data System (ADS)

    Xu, Lingling; Chen, Jinsheng

    2016-04-01

    Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

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

    NASA Technical Reports Server (NTRS)

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

    2001-01-01

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

  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. 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

  8. Coagulation of monodisperse aerosol particles by isotropic turbulence

    NASA Astrophysics Data System (ADS)

    Chun, J.; Koch, D. L.

    2005-02-01

    The rate of coagulation of initially monodisperse aerosols due to isotropic turbulence is studied with particular emphasis on the effects of noncontinuum hydrodynamics and particle inertia. The prevalence of these two factors distinguishes aerosol coagulation from the coagulation of colloidal particles. The turbulent flow seen by an interacting pair of particles is modelled as a stochastically varying flow field that is a linear function of position. This approximation is valid because the 1-10 micron diameter particles for which turbulence dominates coagulation are much smaller than the smallest eddies of a typical turbulent flow field. It is shown that the finite mean-free path of the gas enhances the rate of coagulation and leads to a finite coagulation rate even in the absence of van der Waals attractions. The coupled effects of turbulent shear and Brownian motion are treated. As in the case of laminar shear flows, it is found that Brownian motion plays an important role in the coagulation process even when the Peclet number is moderately large. It is shown that particle inertia increases the coagulation rate in two ways. First, preferential concentration increases the radial distribution function on length scales intermediate between the Kolmogorov length scale and the particle diameter. Second, the greater persistence of particles' relative motion during their local interaction leads to an increase in coagulation rate with increasing particle Stokes number.

  9. Endotoxin in Size-Separated Metal Working Fluid Aerosol Particles.

    PubMed

    Dahlman-Höglund, Anna; Lindgren, Åsa; Mattsby-Baltzer, Inger

    2016-08-01

    Patients with airway symptoms working in metal working industries are increasing, despite efforts to improve the environmental air surrounding the machines. Our aim was to analyse the amount of endotoxin in size-separated airborne particles of metal working fluid (MWF) aerosol, by using the personal sampler Sioutas cascade impactor, to compare filter types, and to compare the concentration of airborne endotoxin to that of the corresponding MWFs. In a pilot field study, aerosols were collected in two separate machine halls on totally 10 occasions, using glass fibre and polytetrafluoroethylene (PTFE) filters in parallel at each station. Airborne endotoxin was distributed over all size fractions. While a major part was found in the largest size fraction (72%, 2.5-10 µm), up to 8% of the airborne endotoxin was detected in the smallest size fraction (<0.25 µm). Comparing the efficiency of the filter types, a significantly higher median endotoxin level was found with glass fibres filters collecting the largest particle-size fraction (1.2-fold) and with PTFE filters collecting the smallest ones (5-fold). The levels of endotoxin in the size-separated airborne particle fractions correlated to those of the MWFs supporting the aerosol-generating machines. Our study indicates that a significant part of inhalable aerosols of MWFs consists of endotoxin-containing particles below the size of intact bacteria, and thus small enough to readily reach the deepest part of the lung. Combined with other chemical irritants of the MWF, exposure to MWF aerosols containing endotoxin pose a risk to respiratory health problems. PMID:27268595

  10. Chemical evolution of multicomponent aerosol particles during evaporation

    NASA Astrophysics Data System (ADS)

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

    2010-05-01

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

  11. Production, Organic Characterization, and Phase Transformations of Marine Particles Aerosolized from a Laboratory Mesocosm Phytoplankton Bioreactor

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

    Previous studies have shown that particles emitted from bubble bursting and wave breaking of ocean waters with high biological activity can contain sea salts associated with organic material, with smaller particles containing a larger mass fraction of organics than larger particles. This likely indicates a link between phytoplankton productivity in oceans and particulate organic material in marine air. Once aerosolized, particles with significant amount of organic material can affect cloud activation and formation of ice crystals, among other atmospheric processes, thus influencing climate. This is significant for clouds and climate particularly over nutrient rich polar seas, in which concentrations of biological organisms can reach up to 109 cells per ml during spring phytoplankton blooms. Here we present results of bubble bursting aerosol production from a seawater mesocosm containing artificial seawater, natural seawater and unialgal cultures of three representative phytoplankton species. These phytoplankton (Thalassiosira pseudonana, Emilianaia huxleyi, and Nannochloris atomus), possessed siliceous frustules, calcareous frustules and no frustules, respectively. Bubbles were generated employing recirculating impinging water jets or glass frits. Dry and humidified aerosol size distributions and bulk aerosol organic composition were measured as a function of phytoplankton growth, and chlorophyll composition and particulate and dissolved organic carbon in the water were determined. Finally, particles were collected on substrates for ice nucleation and water uptake experiments, their elemental compositions were determined using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEMEDAX), and their carbon speciation was determined using scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Particle size distributions exposed to dry and humidified air employing

  12. Measurements of mesospheric aerosol particles during the ECOMA/MASS campaign 2007.

    NASA Astrophysics Data System (ADS)

    Strelnikova, Irina; Rapp, Markus; Strelnikov, Boris; Latteck, Ralph; Baumgarten, Gerd; Brattli, Alvin; Friedrich, Martin; Gumbel, Jorg; Robertson, Scott

    In August 2007 the joint European-American ECOMA/MASS (Existence and Charge state Of Meteoric smoke particles in the middle Atmosphere/Dust MASS Analyzer) sounding rocket and ground-based campaign took place at the Andøya Rocket Range (ARR) (69° N). This campaign was devoted to the investigation of mesospheric aerosol particles. During this campaign, three instrumented sounding rockets were launched under the PMSE and NLC conditions. All rockets were carrying instruments to characterize mesospheric aerosol particles and their environment. The ECOMA rocket was launched during the first salvo shortly (30 min) after the MASS payload. At that time, the EISCAT (69° N, 19° E) VHF and ALWIN radars observed a double layered PMSE. Also an NLC layer was detected by lidar and photometers onboard each rocket. The main instrument of the ECOMA payload is the "ECOMA particle detector". This instrument comprises a classical Faraday cup with a xenon-flash lamp for the active photoionization/photodetachment of mesospheric smoke particles (MSPs) and the subsequent detection of corresponding photoelectrons. Comparing direct Faraday cup measurements and photocurrents we are able to derive particle properties like number densities and particle radii. We present the results of these measurements that show the presence of aerosol particles inside the NLC and PMSE layer, but not below or above these layers. These results are consistent with model predictions, which account for global transport of meteoric smoke. This implies that ice nucleation in the polar summer needs to be reconsidered.

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

    NASA Astrophysics Data System (ADS)

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

    2011-07-01

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

  14. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

    PubMed

    Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

    2013-07-16

    Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

  15. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

    PubMed

    Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

    2013-07-16

    Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

  16. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

    PubMed Central

    Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

    2013-01-01

    Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

  17. PARTICLE SIZE DISTRIBUTIONS FOR AN OFFICE AEROSOL

    EPA Science Inventory

    The article discusses an evaluation of the effect of percent outdoor air supplied and occupation level on the particle size distributions and mass concentrations for a typical office building. (NOTE: As attention has become focused on indoor air pollution control, it has become i...

  18. Morphologies of aerosol particles consisting of two liquid phases

    NASA Astrophysics Data System (ADS)

    Song, Mijung; Marcolli, Claudia; Krieger, Ulrich; Peter, Thomas

    2013-04-01

    Recent studies have shown that liquid-liquid phase separation (LLPS) might be a common feature in mixed organic/ammonium sulfate (AS)/H2O particles. Song et al. (2012) observed that in atmospheric relevant organic/AS/H2O mixtures LLPS always occurred for organic aerosol compositions with O:C < 0.56, depended on the specific functional groups of organics in the range of 0.56 < O:C < 0.80 and never appeared for O:C > 0.80. The composition of the organic fraction and the mixing state of aerosol particles may influence deliquescence relative humidity (DRH) and efflorescence relative humidity (ERH) of inorganic salts during RH cycles and also aerosol morphology. In order to determine how the deliquescence and efflorescence of AS in mixed organic/AS/H2O particles is influenced by LLPS and to identify the corresponding morphologies of the particles, we subjected organic/AS/H2O particles deposited on a hydrophobically coated substrate to RH cycles and observed the phase transitions using optical microscopy and Raman spectroscopy. In this study, we report results from 21 organic/AS/H2O systems with O:C ranging from 0.55 - 0.85 covering aliphatic and aromatic oxidized compounds. Eight systems did not show LLPS for all investigated organic-to-inorganic ratios, nine showed core-shell morphology when present in a two-liquid-phases state and four showed both, core-shell or partially engulfed configurations depending on the organic-to-inorganic ratio. While AS in aerosol particles with complete LLPS showed almost constant values of ERH = 44 ± 4 % and DRH = 77 ± 2 %, a strong reduction or complete inhibition of efflorescence occurred for mixtures that did not exhibit LLPS. To confirm these findings, we performed supplementary experiments on levitated particles in an electrodynamic balance and compared surface and interfacial tensions of the investigated mixtures. Reference Song, M., C. Marcolli, U. K. Krieger, A. Zuend, and T. Peter (2012), Liquid-liquid phase separation in

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

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Seinfeld, J.

    2011-12-01

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

  20. Neural networks for aerosol particles characterization

    NASA Astrophysics Data System (ADS)

    Berdnik, V. V.; Loiko, V. A.

    2016-11-01

    Multilayer perceptron neural networks with one, two and three inputs are built to retrieve parameters of spherical homogeneous nonabsorbing particle. The refractive index ranges from 1.3 to 1.7; particle radius ranges from 0.251 μm to 56.234 μm. The logarithms of the scattered radiation intensity are used as input signals. The problem of the most informative scattering angles selection is elucidated. It is shown that polychromatic illumination helps one to increase significantly the retrieval accuracy. In the absence of measurement errors relative error of radius retrieval by the neural network with three inputs is 0.54%, relative error of the refractive index retrieval is 0.84%. The effect of measurement errors on the result of retrieval is simulated.

  1. Glyoxal and Methylglyoxal in Atlantic Seawater and marine Aerosol Particles

    NASA Astrophysics Data System (ADS)

    van Pinxteren, Manuela; Herrmann, Hartmut

    2014-05-01

    The two α-dicarbonyls glyoxal (CHOCHO; GLY) and methylglyoxal (CH3COCHO; MGLY) have attracted increasing attention over the past years because of their potential role in secondary organic aerosol formation. Recently Sinreich et al. (2010) suggested the open ocean as an important (so far unknown) source for GLY in the atmosphere. To date, there are few available field data of these compounds in the marine area. In this study we present measurements of GLY and MGLY in seawater and marine aerosol particles sampled during a transatlantic Polarstern cruise in spring 2011. In seawater we especially investigated the sea surface microlayer (sampled with the glass plate technique) as it is the direct interface between ocean and atmosphere. Analytical measurements were based on derivatisation with o-(2,3,4,5,6-Pentafluorobenzyl)-hydroxylamine reagent, solvent extraction and GC-MS (SIM) analysis. The results show that GLY and MGLY are present in the sea surface microlayer of the ocean and corresponding bulkwater with average concentrations of 228 ng L-1 (GLY) and 196 ng L-1 (MGLY). Significant enrichment (factor of 4) of GLY and MGLY in the sea surface microlayer was found implying photochemical production of the two carbonyls though a clear connection to global radiation was not observed. On aerosol particles, both carbonyls were detected (average concentration 0.2 ng m-3) and are strongly connected to each other, suggesting similar formation mechanisms. Both carbonyls show a very good correlation with particulate oxalate, supporting the idea of a secondary formation of oxalic acid via GLY and MGLY. A slight correlation of the two carbonyls in the sea surface microlayer and in the aerosol particles was found at co-located sampling areas. In summary, the results of GLY and MGLY in marine aerosol particles and in the oceanic water give first insights towards interaction processes of these alpha dicarbonyls between ocean and atmosphere (van Pinxteren and Herrmann (2013

  2. 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

  3. Fluorescence lifetime imaging of optically levitated aerosol: a technique to quantitatively map the viscosity of suspended aerosol particles.

    PubMed

    Fitzgerald, C; Hosny, N A; Tong, H; Seville, P C; Gallimore, P J; Davidson, N M; Athanasiadis, A; Botchway, S W; Ward, A D; Kalberer, M; Kuimova, M K; Pope, F D

    2016-08-21

    We describe a technique to measure the viscosity of stably levitated single micron-sized aerosol particles. Particle levitation allows the aerosol phase to be probed in the absence of potentially artefact-causing surfaces. To achieve this feat, we combined two laser based techniques: optical trapping for aerosol particle levitation, using a counter-propagating laser beam configuration, and fluorescent lifetime imaging microscopy (FLIM) of molecular rotors for the measurement of viscosity within the particle. Unlike other techniques used to measure aerosol particle viscosity, this allows for the non-destructive probing of viscosity of aerosol particles without interference from surfaces. The well-described viscosity of sucrose aerosol, under a range of relative humidity conditions, is used to validate the technique. Furthermore we investigate a pharmaceutically-relevant mixture of sodium chloride and salbutamol sulphate under humidities representative of in vivo drug inhalation. Finally, we provide a methodology for incorporating molecular rotors into already levitated particles, thereby making the FLIM/optical trapping technique applicable to real world aerosol systems, such as atmospheric aerosols and those generated by pharmaceutical inhalers. PMID:27430158

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

    1999-07-14

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

  5. Characterization of aerosol particles at the forested site in Lithuania

    NASA Astrophysics Data System (ADS)

    Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

    2009-04-01

    Atmospheric particulate matter (PM), especially fine particles (particles with aerodynamic diameter less than 1 m, PM1), has been found to play an important role in global climate change, air quality, and human health. The continuous study of aerosol parameters is therefore imperative for better understanding the environmental effects of the atmospheric particles, as well as their sources, formation and transformation processes. The particle size distribution is particularly important, since this physical parameter determines the mass and number density, lifetime and atmospheric transport, or optical scattering behavior of the particles in the atmosphere (Jaenicke, 1998). Over the years several efforts have been made to improve the knowledge about the chemical composition of atmospheric particles as a function of size (Samara and Voutsa, 2005) and to characterize the relative contribution of different components to the fine particulate matter. It is well established that organic materials constitute a highly variable fraction of the atmospheric aerosol. This fraction is predominantly found in the fine size mode in concentrations ranging from 10 to 70% of the total dry fine particle mass (Middlebrook et al., 1998). Although organic compounds are major components of the fine particles, the composition, formation mechanism of organic aerosols are not well understood. This is because particulate organic matter is part of a complex atmospheric system with hundreds of different compounds, both natural and anthropogenic, covering a wide range of chemical properties. The aim of this study was to characterize the forest PM1, and investigate effects of air mass transport on the aerosol size distribution and chemical composition, estimate and provide insights into the sources and characteristics of carbonaceous aerosols through analysis ^13C/12C isotopic ratio as a function of the aerosol particles size. The measurements were performed at the Rugšteliškis integrated

  6. An amorphous solid state of biogenic secondary organic aerosol particles.

    PubMed

    Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas; Kannosto, Jonna; Yli-Pirilä, Pasi; Leskinen, Jani; Mäkelä, Jyrki M; Holopainen, Jarmo K; Pöschl, Ulrich; Kulmala, Markku; Worsnop, Douglas R; Laaksonen, Ari

    2010-10-14

    Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90 billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate.

  7. Tracking Water Diffusion Fronts in a Highly Viscous Aerosol Particle

    NASA Astrophysics Data System (ADS)

    Bastelberger, Sandra; Krieger, Ulrich; Peter, Thomas

    2016-04-01

    Field measurements indicate that atmospheric secondary aerosol particles can be present in a highly viscous, glassy state [1]. In contrast to liquid state particles, the gas phase equilibration is kinetically limited and governed by condensed phase diffusion. In recent water diffusion experiments on highly viscous single aerosol particles levitated in an electrodynamic balance (EDB) we observed a characteristic shift behavior of the Mie whispering gallery modes (WGM) indicative of the changing radial structure of the particle, thus providing us with an experimental method to track the diffusion process inside the particle. When a highly viscous, homogeneous particle is exposed to an abrupt increase in relative humidity, the rapid gas phase diffusion and strong concentration dependence of the diffusion coefficient in the condensed phase lead to extremely steep water concentration gradients inside the particle, reminiscent of diffusion fronts. The resulting quasi step-like concentration profile motivates the introduction of a simple core-shell model describing the morphology of the non-equilibrium particle during humidification. The subsequent particle growth and reduction of the shell refractive index can be observed as red and blueshift behavior of the WGM, respectively. The shift pattern can be attributed to a core-shell radius ratio and particle radius derived from model calculations [2]. If supplemented with growth information obtained from the WGM redshift and thermodynamic equilibrium data, we can infer a comprehensive picture of the time evolution of the diffusion fronts in the framework of our core-shell model. The measured time dependent concentration profile is then compared with simulations solving the non-linear diffusion equation [3] [1] Virtanen, A., et al., Nature, 467, 824-827, 2010 [2] Kaiser, T., Schweiger, G., Computers in Physics, Vol. 7, No. 6, 682-686, Nov/Dec 1993 [3] Zobrist, B., Soonsin, V., Luo, B.P., Peter, T. et al., Phys. Chem. Chem

  8. An amorphous solid state of biogenic secondary organic aerosol particles.

    PubMed

    Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas; Kannosto, Jonna; Yli-Pirilä, Pasi; Leskinen, Jani; Mäkelä, Jyrki M; Holopainen, Jarmo K; Pöschl, Ulrich; Kulmala, Markku; Worsnop, Douglas R; Laaksonen, Ari

    2010-10-14

    Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90 billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate. PMID:20944744

  9. Biological aerosol detection with combined passive-active infrared measurements

    NASA Astrophysics Data System (ADS)

    Ifarraguerri, Agustin I.; Vanderbeek, Richard G.; Ben-David, Avishai

    2004-12-01

    A data collection experiment was performed in November of 2003 to measure aerosol signatures using multiple sensors, all operating in the long-wave infrared. The purpose of this data collection experiment was to determine whether combining passive hyperspectral and LIDAR measurements can substantially improve biological aerosol detection performance. Controlled releases of dry aerosols, including road dust, egg albumin and two strains of Bacillus Subtilis var. Niger (BG) spores were performed using the ECBC/ARTEMIS open-path aerosol test chamber located in the Edgewood Area of Aberdeen Proving Grounds, MD. The chamber provides a ~ 20' path without optical windows. Ground truth devices included 3 aerodynamic particle sizers, an optical particle size spectrometer, 6 nephelometers and a high-volume particle sampler. Two sensors were used to make measurements during the test: the AIRIS long-wave infrared imaging spectrometer and the FAL CO2 LIDAR. The AIRIS and FAL data sets were analyzed for detection performance relative to the ground truth. In this paper we present experimental results from the individual sensors as well as results from passive-active sensor fusion. The sensor performance is presented in the form of receiver operating characteristic curves.

  10. 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

  11. Virtual Impactor for Sub-micron Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Bolshakov, A. A.; Strawa, A. W.; Hallar, A. G.

    2005-12-01

    The objective of a virtual impactor is to separate out the larger particles in a flow from the smaller particles in such a way that both sizes of particles are available for sampling. A jet of particle-laden air is accelerated toward a collection probe so that a small gap exists between the acceleration nozzle and the probe. A vacuum is applied to deflect a major portion of the airstream away form the collection probe. Particles larger than a certain size have sufficient momentum so that they cross the deflected streamlines and enter the collection probe, whereas smaller particles follow the deflected streamlines. The result is that the collection probe will contain a higher concentration of larger particles than is in the initial airstream. Typically, virtual impactors are high-flow devices used to separate out particles greater than several microns in diameter. We have developed a special virtual impactor to concentrate aerosol particles of diameters between 0.5 to 1 micron for the purpose of calibrating the optical cavity ring-down instrument [1]. No similar virtual impactors are commercially available. In our design, we have exploited considerations described earlier [2-4]. Performance of our virtual impactor was evaluated in an experimental set-up using TSI 3076 nebulizer and TSI 3936 scanning mobility particle size spectrometer. Under experimental conditions optimized for the best performance of the virtual impactor, we were able to concentrate the 700-nm polystyrene particles no less than 15-fold. However, under experimental conditions optimized for calibrating our cavity ring-down instrument, a concentration factor attainable was from 4 to 5. During calibration experiments, maximum realized particle number densities were 190, 300 and 1600 cm-3 for the 900-nm, 700-nm and 500-nm spheres, respectively. This paper discusses the design of the impactor and laboratory studies verifying its performance. References: 1. A.W. Strawa, R. Castaneda, T. Owano, D.S. Baer

  12. Hydrolysis of organonitrate functional groups in aerosol particles

    SciTech Connect

    Liu, Shang; Shilling, John E.; Song, Chen; Hiranuma, Naruki; Zaveri, Rahul A.; Russell, Lynn M.

    2012-10-19

    Organonitrate (ON) groups are important substituents in secondary organic aerosols. Model simulations and laboratory studies indicate a large fraction of ON groups in aerosol particles, but much lower quantities are observed in the atmosphere. Hydrolysis of ON groups in aerosol particles has been proposed recently. To test this hypothesis, we simulated formation of ON molecules in a reaction chamber under a wide range of relative humidity (0% to 90%). The mass fraction of ON groups (5% to 20% for high-NOx experiments) consistently decreased with increasing relative humidity, which was best explained by hydrolysis of ON groups at a rate of 4 day-1 (lifetime of 6 hours) for reactions under relative humidity greater than 20%. In addition, we found that secondary nitrogen-containing molecules absorb light, with greater absorption under dry and high-NOx conditions. This work provides the first evidence for particle-phase hydrolysis of ON groups, a process that could substantially reduce ON group concentration in the atmosphere.

  13. Composition and Particle Size Retrievals for Homogeneous Binary Aerosols

    NASA Astrophysics Data System (ADS)

    Niedziela, R. F.; Argon, P.; Bejcek, L.

    2014-12-01

    Tropospheric aerosols have widely varying compositions, shapes, and sizes. The ability to measure these physical characteristics, coupled with knowledge about their optical properties, can provide insight as to how these particles might participate in atmospheric processes, including their interaction with light. Over the past several years, our laboratory has been involved in developing methods to determine basic physical properties of laboratory-generated particles based on the analysis of infrared extinction spectra of multi-component aerosols. Here we report the results of a complete study on the applicability of well-known refractive index mixing rules to homogeneous binary liquid organic aerosols in an effort to yield in situ measurements of particle size and composition. In particular, we present results for terpenoid (carvone/nopinone) and long-chain hydrocarbon (squalane/squalene) mixtures. The included image shows model carvone/nopinone extinction spectra that were computed using the Lorentz-Lorenz mixing rule on complex refractive index data for the pure components.

  14. Particle Characterization and Ice Nucleation Efficiency of Field-Collected Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Wang, B.; Gilles, M. K.; Laskin, A.; Moffet, R.; Nizkorodov, S.; Roedel, T.; Sterckx, L.; Tivanski, A.; Knopf, D. A.

    2011-12-01

    Atmospheric ice formation by heterogeneous nucleation is one of the least understood processes resulting in cirrus and mixed-phase clouds which affect the global radiation budget, the hydrological cycle, and water vapor distribution. In particular, how organic aerosol affect ice nucleation is not well understood. Here we report on heterogeneous ice nucleation from particles collected during the CalNex campaign at the Caltech campus site, Pasadena, on May 19, 2010 at 6am-12pm (A2) and 12pm-6pm (A3) and May 23 at 6am-12pm (B2) and 6pm-12am (B4). The ice nucleation onsets and water uptake were determined as a function of temperature (200-273 K) and relative humidity with respect to ice (RHice). The ice nucleation efficiency was related to the particle chemical composition. Single particle characterization was provided by using computer controlled scanning electron microscopy with energy dispersive analysis of X-rays (CCSEM/EDX) and scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). The STXM/NEXAFS analysis indicates that the morning sample (A2) constitutes organic particles and organic particles with soot and inorganic inclusions. The afternoon sample (A3) is dominated by organic particles with a potentially higher degree of oxidation associated with soot. The B2 sample shows a higher number fraction of magnesium-containing particle indicative of a marine source and ~93% of the particles contained sulfur besides oxygen and carbon as derived from CCSEM/EDX analysis. The B4 sample lacks the strong marine influence and shows higher organic content. Above 230 K, we observed water uptake followed by condensation freezing at mean RH of 93-100% and 89-95% for A2 and A3, respectively. This indicates that the aged A3 particles are efficient ice nuclei (IN) for condensation freezing. Below 230 K A2 and A3 induced deposition ice nucleation between 125-155% RHice (at mean values of 134-150% RHice). The B2 and B4

  15. DEVELOPMENT OF AN RH -DENUDED MIE ACTIVE SAMPLING SYSTEM AND TARGETED AEROSOL CALIBRATION

    EPA Science Inventory

    The MIE pDR 1200 nephelometer provides time resolved aerosol concentrations during personal and fixed-site sampling. Active (pumped) operation allows defining an upper PM2.5 particle size, however, this dramatically increases the aerosol mass passing through the phot...

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

    NASA Technical Reports Server (NTRS)

    Sheridan, Patrick J.

    1999-01-01

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

  17. Graphical techniques for interpreting the composition of individual aerosol particles

    NASA Astrophysics Data System (ADS)

    Yuan, Hui; Rahn, Kenneth A.; Zhuang, Guoshun

    A graphical technique that uses X- Y and ternary plots is presented for interpreting elemental data for individual aerosol particles. By revealing the multiple functional relationships between the elements, it offers more insight into the groups of particles and the transitions between them than traditional techniques such as factor analysis and cluster analysis alone are able to. For a sample of dust storm aerosol from Beijing in March 2002, X-Y plots revealed areas, lines, and "dots" that represented clays, smooth transitions to asymptotes of pure single-component minerals, and pure minor minerals or special particles, respectively. Ternary plots further revealed ratios of elements and potential minerals. Careful use of cluster analysis revealed subgroups of particles that were not separated by clear borders. The dust storm had three major components, clay/quartz (Al 2O 3, SiO 2, etc.), basic calcium (CaO, CaCO 3), and salts (sulfate, phosphate, chloride). Some sulfates, including CaSO 4 and (NH 4) xH 2-xSO 4, were mixed with the quartz and clay. A five-step sequence that combines graphics, basic statistics, cluster analysis, and SEM photography seems to extract the maximum information from suites of single particles.

  18. Cooling enhancement of aerosol particles due to surfactant precipitation.

    PubMed

    Beaver, Melinda R; Freedman, Miriam A; Hasenkopf, Christa A; Tolbert, Margaret A

    2010-07-01

    Light extinction by particles in Earth's atmosphere is strongly dependent on the particle size, chemical composition, and ability to take up water. In this work, we have measured the optical growth factors, fRH(ext)(RH, dry), for complex particles composed of an inorganic salt, sodium nitrate, and an anionic surfactant, sodium dodecyl sulfate. In contrast with previous studies using soluble and slightly soluble organic compounds, optical growth in excess to that expected based on the volume weighted water uptake of the individual components is observed. We explored the relationship between optical growth and concentration of surfactant by investigating the role of particle density, the effect of a surfactant monolayer, and increased light extinction by surfactant aggregates and precipitates. For our experimental conditions, it is likely that surfactant precipitates are responsible for the observed increase in light scattering. The contribution of surfactant precipitates to light scattering of aerosol particles has not been previously explored and has significant implications for characterizing the aerosol direct effect.

  19. Characterization of indoor cooking aerosol using neutron activation analysis

    SciTech Connect

    Wu, D.; Landsberger, S.; Larson, S. )

    1993-01-01

    Suspended particles in air are potentially harmful to human health, depending on their sizes and chemical composition. Residential indoor particles mainly come from (a) outdoor sources that are transported indoors, (b) indoor dust that is resuspended, and (c) indoor combustion sources, which include cigarette smoking, cooking, and heating. Jedrychowski stated that chronic phlegm in elderly women was strongly related to the cooking exposure. Kamens et al. indicated that cooking could generate small particles (<0.1 [mu]m), and cooking one meal could contribute [approximately]5 to 18% of total daytime particle volume exposure. Although cooking is a basic human activity, there are not many data available on the properties of particles generated by this activity. Some cooking methods, such as stir-frying and frying, which are the most favored for Chinese and other Far East people, generate a large quantity of aerosols. This research included the following efforts: 1. investigating particle number concentrations, distributions, and their variations with four different cooking methods and ventilation conditions; 2. measuring the chemical composition of cooking aerosol samples by instrumental neutron activation analysis.

  20. 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.

  1. Observational Evidence of Aerosol Enhancement of Lightning Activity and Convective Invigoration

    NASA Technical Reports Server (NTRS)

    Yuan, Tianle; Remer, Lorraine A.; Pickering, Kenneth E.; Yu, Hongbin

    2011-01-01

    Lightning activity over the West Pacific Ocean east of the Philippines is usually much less frequent than over the nearby maritime continents. However, in 2005 the Lightning Imaging Sensor (LIS) aboard the TRMM satellite observed anomalously high lightning activity in that area. In the same year the Moderate resolution Imaging Spectroradiometer (MODIS) measured anomalously high aerosol loading. The high aerosol loading was traced to volcanic activity, and not to any factor linked to meteorology, disentangling the usual convolution between aerosols and meteorology. We show that in general lightning activity is tightly correlated with aerosol loadings at both inter-annual and biweekly time scales. We estimate that a approximately 60% increase in aerosol loading leads to more than 150% increase in lightning flashes. Aerosols increase lightning activity through modification of cloud microphysics. Cloud ice particle sizes are reduced and cloud glaciation is delayed to colder temperature when aerosol loading is increased. TRMM precipitation radar measurements indicate that anomalously high aerosol loading is associated with enhanced cloud mixed phase activity and invigorated convection over the maritime ocean. These observed associations between aerosols, cloud microphysics, morphology and lightning activity are not related to meteorological variables or ENSO events. The results have important implications for understanding the variability of lightning and resulting aerosol-chemistry interactions.

  2. Contact nucleation of ice induced by biological aerosol particles

    NASA Astrophysics Data System (ADS)

    Kiselev, Alexei; Hoffmann, Nadine; Schaefer, Manfred; Duft, Denis; Leisner, Thomas

    2014-05-01

    The contact freezing of supercooled water droplets is one of the potentially important and the least understood heterogeneous mechanism of ice formation in tropospheric clouds. On the time scales of cloud lifetime the freezing of supercooled water droplets via contact mechanism may occur at higher temperature compared to the same IN immersed in the droplet. Recently we have developed an experimental method allowing for quantification of the freezing probability on a single droplet-particle collision event [1]. In the previous experimental studies with mineral dust (kaolinite, illite, feldspar, and hematite) we have been able to show that the rate of freezing at a given temperature is governed by the rate of droplet - particle collisions, and by the properties of the contact ice nuclei: its size, morphology and composition [1, 2]. In this contribution, we focus on the contact freezing efficiency of biological ice nuclei. We demonstrate that the contact freezing efficiency of Snomax (freeze-dried fragments of Pseudomonas syringae bacteria) follows very similar pattern observed in immersion freezing experiments, indicating that the INA-protein identified as the ice nucleation agent in the immersion freezing mode is also responsible for initiation of contact freezing. The same similarity is observed for contact freezing induced by semi-dry residual particles of birch pollen washing water, providing an evidence for the importance of organic macromolecules of biological origin for nucleation of atmospheric ice. Finally, our experiments show that mixing the birch pollen washing water with mineral dust (illite) significantly increases the IN efficiency of mineral dust and extends the temperature range of its IN activity. These findings suggest a possible route of multiplication of the effect of biological IN beyond observed atmospheric concentrations of pollen grains. [1] - Hoffmann, N., Kiselev, A., Rzesanke, D., Duft, D., and Leisner, T.: Experimental quantification of

  3. 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

  4. Ozone and secondary aerosol formation — Analysis of particle observations in the 2009 SHARP campaign

    NASA Astrophysics Data System (ADS)

    Cowin, J.; Yu, X.; Laulainen, N.; Iedema, M.; Lefer, B. L.; Anderson, D.; Pernia, D.; Flynn, J. H.

    2010-12-01

    Particulate matters (PM) play important roles in the formation and transformation of ozone. Although photooxidation of volatile organic compounds with respect to ozone formation in the gas phase is well understood, many unknowns still exist in heterogeneous mechanisms that process soot, secondary aerosols (both inorganic and organic), and key radical precursors such as formaldehyde and nitrous acid. Our main objective is to answer two key science questions: 1) will reduction of fine PM reduce ozone formation? 2) What sources of PM are most culpable? Are they from local chemistry or long-range transport? The field data collected in the 2009 Study of Houston Atmospheric Radical Precursors (SHARP) by our group at the Moody Tower consist of 1) real-time photolysis rates of ozone precursors, 2) particle size distributions, 3) organic carbon and elemental carbon, and 4) an archive of single particle samples taken with the Time Resolved Aerosol Collector (TRAC) sampler. The time resolution of the TRAC sampler is 30 minutes for routine measurements, and 15 minutes during some identified “events” (usually in the mid-afternoon) of high ozone and secondary organic or sulfate particle formation. The latter events last typically about an hour. Five ozone exceedance days occurred during the 6 weeks of deployment. Strong correlation between photochemical activities and organic carbon was observed. Initial data analysis indicates that secondary organic aerosol is a major component of the carbonaceous aerosols observed in Houston. Soot, secondary sulfate, seal salt, and mineral dust particles are determined from single particle analysis using scanning electron microscope and transmission electron microcopy coupled with energy dispersive X-ray spectroscopy. Compared with observations in 2000, the mass percentage of organics is higher (60 vs. 30%), and lower for sulfate (20% vs. 32%). On-going data analysis will focus on the composition, sources, and transformation of primary and

  5. Measurements of Primary Biogenic Aerosol Particles with an Ultraviolet Aerodynamic Particle Sizer (UVAPS) During AMAZE-08

    NASA Astrophysics Data System (ADS)

    Wollny, A. G.; Garland, R.; Pöschl, U.

    2008-12-01

    Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the AMazonian Aerosol CharacteriZation Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. The presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 μm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as 'viable aerosols' or 'fluorescent bioparticles' (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. First data analyses show a pronounced peak of FBAP at diameters around 2-3 μm. In this size range the biogenic particle fraction was

  6. A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

    NASA Technical Reports Server (NTRS)

    Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

    1980-01-01

    The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

  7. Individual Aerosol Particle Types Produced by Savanna Burning

    NASA Astrophysics Data System (ADS)

    Posfai, M.; Simonics, R.; Li, J.; Hobbs, P. V.; Buseck, P. R.; Buseck, P. R.

    2001-12-01

    We used analytical transmission electron microscopy (TEM) to study individual aerosol particles that were collected on the University of Washington Convair-580 research aircraft over southern Africa during the Safari2000 Dry Season Experiment. Our goals were to study the compositions, morphologies, and mixing states of carbonaceous particles, in order to better understand the physical and chemical properties of biomass smoke on the individual-particle level. The compositions of single particles were determined using energy-dispersive x-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS). Energy-loss maps obtained with the TEM are useful for studying the spatial distribution of light elements such as carbon within the particles; thus, they provide a detailed picture of complex particles. Carbonaceous particles were assigned into three main groups on the basis of morphology and composition: "organic particles with inorganic inclusions," "tar balls," and "soot." Soot is recognized by its characteristic morphology and microstructure. The distinction between "organic particles with inorganic inclusions" and "tar balls" is somewhat arbitrary, since the two criteria that are used for their distinction (composition and aspect ratio) change continually. The relative concentrations of the three major particle types vary with the type of fire and distance from fire. In the plume of a smoldering fire west of Beria (August 31) the relative concentration of tar balls increased with aging of the plume. Tar balls have a fairly narrow size distribution with a maximum between 100 and 200 nm (diameter). The inorganic K-salt inclusions (KCl, K2SO4, KNO3) within "organic particles" should make these particles hygroscopic, regardless of the properties of the organic compounds. Aging causes the conversion of KCl into K2SO4, KNO3. Aerosol production from flaming and smoldering fires was compared over Kruger National Park on August 17; more soot and more Cl-rich inclusions

  8. Surface tensions, viscosities, and diffusion constants in mixed component single aerosol particles

    NASA Astrophysics Data System (ADS)

    Bzdek, Bryan; Marshall, Frances; Song, Young-Chul; Haddrell, Allen; Reid, Jonathan

    2016-04-01

    Surface tension and viscosity are important aerosol properties but are challenging to measure on individual particles owing to their small size and mass. Aerosol viscosity impacts semivolatile partitioning from the aerosol phase, molecular diffusion in the bulk of the particle, and reaction kinetics. Aerosol surface tension impacts how particles activate to serve as cloud condensation nuclei. Knowledge of these properties and how they change under different conditions hinders accurate modelling of aerosol physical state and atmospheric impacts. We present measurements made using holographic optical tweezers to directly determine the viscosity and surface tension of optically trapped droplets containing ~1-4 picolitres of material (corresponding to radii of ~5-10 micrometres). Two droplets are captured in the experimental setup, equilibrated to a relative humidity, and coalesced through manipulation of the relative trap positions. The moment of coalescence is captured using camera imaging as well as from elastically backscattered light connected to an oscilloscope. For lower viscosity droplets, the relaxation in droplet shape to a sphere follows the form of a damped oscillator and gives the surface tension and viscosity. For high viscosity droplets, the relaxation results in a slow merging of the two droplets to form a sphere and the timescale of that process permits determination of viscosity. We show that droplet viscosity and surface tension can be quantitatively determined to within <10% of the expected value for low viscosity droplets and to better than 1 order of magnitude for high viscosity droplets. Examples illustrating how properties such as surface tension can change in response to environmental conditions will be discussed. Finally, a study of the relationship between viscosity, diffusion constants, vapour pressures, and reactive uptake coefficients for a mixed component aerosol undergoing oxidation and volatilisation will be discussed.

  9. Desert dust in rural western US; the influence of dust storms, large particles, and land-use change on aerosol loads

    NASA Astrophysics Data System (ADS)

    Parks, D.; MacDonald, A. E.; Rosen, R. D.; Edmonds, H. N.; Key, E.; Swanberg, N.; Wiseman, W. J.; Sandgathe, S. A.; Neff, J. C.; Fernandez, D.; Munson, S.; Reynolds, R. L.

    2011-12-01

    Atmospheric aerosols are common in urban settings as well as dryland rural environments and are important to both climate and biogeochemical cycling. Most urban and far traveled aerosols are less than 10 micrometers in diameter with many particles in the less than 2.5 or 1 micrometer-size classes. Small aerosols, including many generated by industrial activity, are the focus of federal environmental law and have a major impact on human health. In rural areas of the western US, however, these small industrially derived particles appear to make up a small part of the overall aerosol load. Rather, dust in the rural West is dominated by mineral aerosols including a large amount of particles that range in size from 10 to 40 microns. These particles can travel for hundreds of kilometers, particularly during periods when dust storms are common. In the dusty spring and summer periods in and around Canyonlands and Mesa Verde National Parks, large particles (particles greater than 10 micrometers in diameter) appear to contribute between 50 and 90% to the overall particle load several meters above the ground. During large dust storms, concentrations of total suspended particulates increase by a factor of 8 to 10 while particles less than 10 micrometers in diameter are minimally affected. The presence of large particles in the atmosphere of the rural West is notable for several reasons. First, the majority of the existing aerosol monitoring networks focus on the small particle-size classes of less than 2.5 and 10 microns. Because many aerosol-collection instruments are designed with specific particle-size cutoff criteria, these instruments and the networks that depend on them are effectively blind to the larger particles that can dominate aerosol loads in the West. Second, for large portions of the year including the spring and summer months when dust storms are common, large particles likely play a major role in visibility restrictions across the protected airsheds of the

  10. Radial inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy (Invited)

    NASA Astrophysics Data System (ADS)

    Krieger, U. K.; Steimer, S.; Lienhard, D.; Bastelberger, S.

    2013-12-01

    Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous MBTCA (3-methyl-1,2,3-Butanetricarboxylic acid) and shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a 'white light ' LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. Potential implications for

  11. Atmospheric Condensational Properties of Ultrafine Chain and Fractal Aerosol Particles

    NASA Technical Reports Server (NTRS)

    Marlow, William H.

    1997-01-01

    The purpose for the research sponsored by this grant was to lay the foundations for qualitative understanding and quantitative description of the equilibrium vapor pressure of water vapor over the irregularly shaped, carbonaceous particles that are present in the atmosphere. This work apparently was the first systematic treatment of the subject. Research was conducted in two complementary components: 1. Calculations were performed of the equilibrium vapor pressure of water over particles comprised of aggregates of spheres in the 50-200 nm radius range. The purposes of this work were two-fold. First, since no systematic treatment of this subject had previously been conducted, its availability would be directly useful for quantitative treatment for a limited range of atmospheric aerosols. Second, it would provide qualitative indications of the effects of highly irregular particle shape on equilibrium vapor pressure of aggregates comprised of smaller spheres.

  12. Physical characterization of aerosol particles during the Chinese New Year’s firework events

    NASA Astrophysics Data System (ADS)

    Zhang, Min; Wang, Xuemei; Chen, Jianmin; Cheng, Tiantao; Wang, Tao; Yang, Xin; Gong, Youguo; Geng, Fuhai; Chen, Changhong

    2010-12-01

    Measurements for particles 10 nm to 10 μm were taken using a Wide-range Particle Spectrometer during the Chinese New Year (CNY) celebrations in 2009 in Shanghai, China. These celebrations provided an opportunity to study the number concentration and size distribution of particles in an especial atmospheric pollution situation due to firework displays. The firework activities had a clear contribution to the number concentration of small accumulation mode particles (100-500 nm) and PM 1 mass concentration, with a maximum total number concentration of 3.8 × 10 4 cm -3. A clear shift of particles from nucleation and Aitken mode to small accumulation mode was observed at the peak of the CNY firework event, which can be explained by reduced atmospheric lifetimes of smaller particles via the concept of the coagulation sink. High particle density (2.7 g cm -3) was identified as being particularly characteristic of the firework aerosols. Recalculated fine particles PM 1 exhibited on average above 150 μg m -3 for more than 12 hours, which was a health risk to susceptible individuals. Integral physical parameters of firework aerosols were calculated for understanding their physical properties and further model simulation.

  13. Estimating Black Carbon Aging Time-Scales with a Particle-Resolved Aerosol Model

    SciTech Connect

    Riemer, Nicole; West, Matt; Zaveri, Rahul A.; Easter, Richard C.

    2010-01-13

    Understanding the aging process of aerosol particles is important for assessing their chemical reactivity, cloud condensation nuclei activity, radiative properties and health impacts. In this study we investigate the aging of black carbon containing particles in an idealized urban plume using a new approach, the particleresolved aerosol model PartMC-MOSAIC. We present a method to estimate aging time-scales using an aging criterion based on cloud condensation nuclei activation. The results show a separation into a daytime regime where condensation dominates and a nighttime regime where coagulation dominates. For the chosen urban plume scenario, depending on the supersaturation threshold, the values for the aging timescales vary between 0.06 hours and 10 hours during the day, and between 6 hours and 20 hours during the night.

  14. Susceptibility of Tribolium confusum (Coleoptera: Tenebrionidae) to pyrethrin aerosol: effects of aerosol particle size, concentration, and exposure conditions

    Technology Transfer Automated Retrieval System (TEKTRAN)

    A series of laboratory studies were conducted to assess effect of droplet size on efficacy of pyrethrin aerosol against adults of Tribolium confusum Jacqueline DuVal, the confused flour beetle. A vertical flow aerosol exposure chamber that generated a standardized particle size diameter was used for...

  15. A New Electrospray Aerosol Generator with High Particle Transmission Efficiency.

    PubMed

    Fu, Huijing; Patel, Anand C; Holtzman, Michael J; Chen, Da-Ren

    2011-01-01

    A new single-capillary electrospray (ES) aerosol generator has been developed for monodisperse particle production with maximal transmission efficiency. The new generator consists of both a spray chamber in a point-to-orifice-plate configuration and a charge reduction chamber that can hold up to 4 Nuclespot ionizers (Model P-2042, NRD Inc.). The 2 chambers are partitioned by an orifice plate. To optimize the particle transmission efficiency of the prototype, a systematic study was performed on the generator by varying the system setup and operation. Two key dimensions of the generator setup, the orifice diameter and the distance from the capillary tip to the orifice plate, were varied. Fluorescence analysis was applied to characterize the loss of ES-generated particles at different locations of the prototype. It was found that particle loss in the generator could be reduced by either increasing the orifice diameter or decreasing the distance between the capillary tip and the orifice plate. Increasing either the total radioactivity of the ionizers or the flowrate of the particle carrier gas also further decreased the particle loss in the system. The maximum particle transmission efficiency of 88.0% was obtained with the spray chamber fully opened to the charge reduction chamber, the capillary tip at the same level as the orifice plate, and 4 bipolar ionizers installed.

  16. A method to resolve the phase state of aerosol particles

    NASA Astrophysics Data System (ADS)

    Saukko, E.; Kuuluvainen, H.; Virtanen, A.

    2012-01-01

    The phase state of atmospheric aerosols has an impact on their chemical aging and their deliquescence and thus their ability to act as cloud condensation nuclei (CCN). The phase change of particles can be induced by the deliquescence or efflorescence of water or by chemical aging. Existing methods, such as tandem differential mobility analysis rely on the size change of particles related to the water uptake or release. To address the need to study the phase change induced by mass-preserving and nearly mass-preserving processes a new method has been developed. The method relies on the physical impaction of particles on a smooth substrate and subsequent counting of bounced particles by a condensation particle counter (CPC). The connection between the bounce probability and physical properties of particles is so far qualitative. To evaluate the performance of this method, the phase state of ammonium sulfate and levoglucosan, crystalline and amorphous solid, in the presence of water vapor was studied. The results show a marked difference in particle bouncing properties between substances - not only at the critical relative humidity level, but also on the slope of the bouncing probability with respect to humidity. This suggests that the method can be used to differentiate between amorphous and crystalline substances as well as to differentiate between liquid and solid phases.

  17. A method to resolve the phase state of aerosol particles

    NASA Astrophysics Data System (ADS)

    Saukko, E.; Kuuluvainen, H.; Virtanen, A.

    2011-10-01

    The phase state of atmospheric aerosols has impact on their chemical aging and their deliquescence and thus their ability to act as cloud condensation nuclei (CCN). The phase change of particles can be induced by the deliquescence or efflorescence of water or by chemical aging. Existing methods, such as tandem differential mobility analysis rely on the size change of particles related to the water uptake or release related to deliquescence and efflorescence. To address the need to study the phase change induced by mass-preserving and nearly mass-preserving processes a new method has been developed. The method relies on the physical impaction of particles on a smooth substrate and subsequent counting of bounced particles by condensation particle counter (CPC). The connection between the bounce probability and physical properties of particles is so far qualitative. To evaluate the performance of this method, the phase state of ammonium sulfate and levoglucosan, crystalline and amorphous solid, in the presence of water vapor was studied. The results show a marked difference in particle bouncing properties between substances - not only at the critical relative humidity level, but also on the slope of the bouncing probability with respect to humidity. This suggests that the method can be used to differentiate between amorphous and crystalline substances as well as to differentiate between liquid and solid phases.

  18. Method and apparatus for aerosol particle absorption spectroscopy

    DOEpatents

    Campillo, Anthony J.; Lin, Horn-Bond

    1983-11-15

    A method and apparatus for determining the absorption spectra, and other properties, of aerosol particles. A heating beam source provides a beam of electromagnetic energy which is scanned through the region of the spectrum which is of interest. Particles exposed to the heating beam which have absorption bands within the band width of the heating beam absorb energy from the beam. The particles are also illuminated by light of a wave length such that the light is scattered by the particles. The absorption spectra of the particles can thus be determined from an analysis of the scattered light since the absorption of energy by the particles will affect the way the light is scattered. Preferably the heating beam is modulated to simplify the analysis of the scattered light. In one embodiment the heating beam is intensity modulated so that the scattered light will also be intensity modulated when the particles absorb energy. In another embodiment the heating beam passes through an interferometer and the scattered light reflects the Fourier Transform of the absorption spectra.

  19. A New Electrospray Aerosol Generator with High Particle Transmission Efficiency.

    PubMed

    Fu, Huijing; Patel, Anand C; Holtzman, Michael J; Chen, Da-Ren

    2011-01-01

    A new single-capillary electrospray (ES) aerosol generator has been developed for monodisperse particle production with maximal transmission efficiency. The new generator consists of both a spray chamber in a point-to-orifice-plate configuration and a charge reduction chamber that can hold up to 4 Nuclespot ionizers (Model P-2042, NRD Inc.). The 2 chambers are partitioned by an orifice plate. To optimize the particle transmission efficiency of the prototype, a systematic study was performed on the generator by varying the system setup and operation. Two key dimensions of the generator setup, the orifice diameter and the distance from the capillary tip to the orifice plate, were varied. Fluorescence analysis was applied to characterize the loss of ES-generated particles at different locations of the prototype. It was found that particle loss in the generator could be reduced by either increasing the orifice diameter or decreasing the distance between the capillary tip and the orifice plate. Increasing either the total radioactivity of the ionizers or the flowrate of the particle carrier gas also further decreased the particle loss in the system. The maximum particle transmission efficiency of 88.0% was obtained with the spray chamber fully opened to the charge reduction chamber, the capillary tip at the same level as the orifice plate, and 4 bipolar ionizers installed. PMID:22829715

  20. 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

  1. 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

  2. Inhomogeneities in particle composition of single, levitated aerosol particles observed by Mie resonance spectroscopy

    NASA Astrophysics Data System (ADS)

    Krieger, Ulrich; Lienhard, Daniel; Bastelberger, Sandra; Steimer, Sarah

    2014-05-01

    Recent observations have indicated that organic aerosol particles in the atmosphere may exist in an amorphous semi-solid or even solid (i.e. glassy) state, e.g. [1]. The influence of highly viscous and glassy states on the timescale of aerosol particle equilibration with respect to water vapor have been investigated for some model systems of atmospheric aerosol, e.g. [2,3]. In particular, it has been shown that the kinetics of the water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules for a highly viscous aerosol particle. A liquid phase diffusion model based on numerically solving the non-linear diffusion equation predicts strong internal gradients in water concentration when condensed phase diffusion impedes the water uptake from the gas phase [2]. Here we observe and quantify the internal concentration gradients in single, levitated, micron size aerosol particles of aqueous shikimic acid using elastic Mie resonance spectroscopy. A single, aqueous particle is levitated in an electro-dynamic balance (for details see [2]), dried for several days at room temperature, cooled to the target temperature and exposed to a rapid change in relative humidity. In addition to measuring the elastically backscattered light of a "white light" LED source and recording the full spectrum with a spectrograph as in [2], we use a tunable diode laser (TDL) to scan high resolution TE- and TM spectra. This combination allows observing various Mie resonance mode orders simultaneously. Since we perform the experiment at low temperatures and low humidities the changes in the Mie-spectra due to water uptake are sufficiently slow to resolve the kinetics. Experimental Mie resonance spectra are inverted to concentration profiles of water within the particle by applying the numerical diffusion model [2] in conjunction with Mie calculations of multilayered spheres [4]. [1] A. Virtanen et al. (2010): An amorphous solid state of biogenic secondary

  3. Generation and characterization of large-particle aerosols using a center flow tangential aerosol generator with a nonhuman-primate, head-only aerosol chamber

    PubMed Central

    Bohannon, J. Kyle; Lackemeyer, Matthew G.; Kuhn, Jens H.; Wada, Jiro; Bollinger, Laura; Jahrling, Peter B.; Johnson, Reed F.

    2016-01-01

    Aerosol droplets or particles produced from infected respiratory secretions have the potential to infect another host through inhalation. These respiratory particles can be polydisperse and range from 0.05–500 μm in diameter. Animal models of infection are generally established to facilitate the potential licensure of candidate prophylactics and/or therapeutics. Consequently, aerosol-based animal infection models are needed to properly study and counter airborne infections. Ideally, experimental aerosol exposure should reliably result in animal disease that faithfully reproduces the modelled human disease. Few studies have been performed to explore the relationship between exposure particle size and induced disease course for infectious aerosol particles. The center flow tangential aerosol generator (CenTAG™) produces large-particle aerosols capable of safely delivering a variety of infectious aerosols to nonhuman primates within a Class III Biological Safety Cabinet (BSC) for establishment or refinement of nonhuman primate infectious disease models. Here we report the adaptation of this technology to the Animal Biosafety Level 4 (ABSL-4) environment for the future study of high-consequence viral pathogens and the characterization of CenTAG™-created sham (no animal, no virus) aerosols using a variety of viral growth media and media supplements. PMID:25970823

  4. Generation and characterization of large-particle aerosols using a center flow tangential aerosol generator with a non-human-primate, head-only aerosol chamber.

    PubMed

    Bohannon, J Kyle; Lackemeyer, Matthew G; Kuhn, Jens H; Wada, Jiro; Bollinger, Laura; Jahrling, Peter B; Johnson, Reed F

    2015-01-01

    Aerosol droplets or particles produced from infected respiratory secretions have the potential to infect another host through inhalation. These respiratory particles can be polydisperse and range from 0.05 to 500 µm in diameter. Animal models of infection are generally established to facilitate the potential licensure of candidate prophylactics and/or therapeutics. Consequently, aerosol-based animal infection models are needed to properly study and counter airborne infections. Ideally, experimental aerosol exposure should reliably result in animal disease that faithfully reproduces the modeled human disease. Few studies have been performed to explore the relationship between exposure particle size and induced disease course for infectious aerosol particles. The center flow tangential aerosol generator (CenTAG™) produces large-particle aerosols capable of safely delivering a variety of infectious aerosols to non-human primates (NHPs) within a Class III Biological Safety Cabinet (BSC) for establishment or refinement of NHP infectious disease models. Here, we report the adaptation of this technology to the Animal Biosafety Level 4 (ABSL-4) environment for the future study of high-consequence viral pathogens and the characterization of CenTAG™-created sham (no animal, no virus) aerosols using a variety of viral growth media and media supplements. PMID:25970823

  5. 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

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

    PubMed

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

    2011-07-01

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

  7. Method for determining aerosol particle size device for determining aerosol particle size

    DOEpatents

    Novick, Vincent J.

    1998-01-01

    A method for determining the mass median diameter D of particles contained in a fluid is provided wherein the data of the mass of a pre-exposed and then a post-exposed filter is mathematically combined with data concerning the pressure differential across the same filter before and then after exposure to a particle-laden stream. A device for measuring particle size is also provided wherein the device utilizes the above-method for mathematically combining the easily quantifiable data.

  8. SAGE II aerosol validation: selected altitude measurements, including particle micromeasurements.

    PubMed

    Oberbeck, V R; Livingston, J M; Russell, P B; Pueschel, R F; Rosen, J N; Osborn, M T; Kritz, M A; Snetsinger, K G; Ferry, G V

    1989-06-20

    Correlative aerosol measurements taken at a limited number of altitudes during coordinated field experiments are used to test the validity of particulate extinction coefficients derived from limb path solar radiance measurements taken by the Stratospheric Aerosol and Gas Experiment (SAGE) II Sun photometer. In particular, results are presented from correlative measurement missions that were conducted during January 1985, August 1985, and July 1986. Correlative sensors included impactors, laser spectrometers, and filter samplers aboard an U-2-airplane, an upward pointing lidar aboard a P-3 airplane, and balloon-borne optical particle counters (dustsondes). The main body of this paper focuses on the July 29, 1986, validation experiment, which minimized the many difficulties (e.g., spatial and temporal inhomogeneities, imperfect coincidences) that can complicate the validation process. On this day, correlative aerosol measurements taken at an altitude of 20.5 km agreed with each other within their respective uncertainties, and particulate extinction values calculated at SAGE II wavelengths from these measurements validated corresponding SAGE II values. Additional validation efforts on days when measurement and logistical conditions were much less favorable for validation are discussed in an appendix.

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

    SciTech Connect

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

    2013-02-28

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

  10. 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.

  11. A Robust Computational Method for Coupled Liquid-liquid Phase Separation and Gas-particle Partitioning Predictions of Multicomponent Aerosols

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Di Stefano, A.

    2014-12-01

    Providing efficient and reliable model predictions for the partitioning of atmospheric aerosol components between different phases (gas, liquids, solids) is a challenging problem. The partitioning of water, various semivolatile organic components, inorganic acids, bases, and salts, depends simultaneously on the chemical properties and interaction effects among all constituents of a gas + aerosol system. The effects of hygroscopic particle growth on the water contents and physical states of potentially two or more liquid and/or solid aerosol phases in turn may significantly affect multiphase chemistry, the direct effect of aerosols on climate, and the ability of specific particles to act as cloud condensation or ice nuclei. Considering the presence of a liquid-liquid phase separation in aerosol particles, which typically leads to one phase being enriched in rather hydrophobic compounds and the other phase enriched in water and dissolved electrolytes, adds a high degree of complexity to the goal of predicting the gas-particle partitioning of all components. Coupled gas-particle partitioning and phase separation methods are required to correctly account for the phase behaviour of aerosols exposed to varying environmental conditions, such as changes to relative humidity. We present new theoretical insights and a substantially improved algorithm for the reliable prediction of gas-particle partitioning at thermodynamic equilibrium based on the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. We introduce a new approach for the accurate prediction of the phase distribution of multiple inorganic ions between two liquid phases, constrained by charge balance, and the coupling of the liquid-liquid equilibrium model to a robust gas-particle partitioning algorithm. Such coupled models are useful for exploring the range of environmental conditions leading to complete or incomplete miscibility of aerosol constituents which will affect

  12. EVALUATION OF ACOUSTIC FORCES ON A PARTICLE IN AEROSOL MEDIUM

    SciTech Connect

    Lee, S; Richard Dimenna, R

    2007-09-27

    The acoustic force exerted on a solid particle was evaluated to develop a fundamental understanding of the critical physical parameters or constraints affecting particle motion and capture in a collecting device. The application of an acoustic force to the collection of a range of submicron-to-micron particles in a highly turbulent airflow stream laden with solid particles was evaluated in the presence of other assisting and competing forces. This scoping estimate was based on the primary acoustic force acting directly on particles in a dilute aerosol system, neglecting secondary interparticle effects such as agglomeration of the sub-micron particles. A simplified analysis assuming a stable acoustic equilibrium with an infinite sound speed in the solid shows that for a solid-laden air flow in the presence of a standing wave, particles will move toward the nearest node. The results also show that the turbulent drag force on a 1-{micro}m particle resulting from eddy motion is dominant when compared with the electrostatic force or the ultrasonic acoustic force. At least 180 dB acoustic pressure level at 1 MHz is required for the acoustic force to be comparable to the electrostatic or turbulent drag forces in a high-speed air stream. It is noted that particle size and pressure amplitude are dominant parameters for the acoustic force. When acoustic pressure level becomes very large, the acoustic energy will heat up the surrounding air medium, which may cause air to expand. With an acoustic power of about 600 watts applied to a 2000-lpm air flow, the air temperature can increase by as much as 15 C at the exit of the collector.

  13. The ice nucleation activity of biological aerosols

    NASA Astrophysics Data System (ADS)

    Grothe, H.; Pummer, B.; Bauer, H.; Bernardi, J.

    2012-04-01

    Primary Biological Aerosol Particles (PBAPs), including bacteria, spores and pollen may be important for several atmospheric processes. Particularly, the ice nucleation caused by PBAPs is a topic of growing interest, since their impact on ice cloud formation and thus on radiative forcing, an important parameter in global climate is not yet fully understood. In laboratory model studies we investigated the ice nucleation activity of selected PBAPs. We studied the immersion mode freezing using water-oil emulsion, which we observed by optical microscopy. We particularly focused on pollen. We show that pollen of different species strongly differ in their ice nucleation behavior. The average freezing temperatures in laboratory experiments range from 240 K to 255 K. As the most efficient nuclei (silver birch, Scots pine and common juniper pollen) have a distribution area up to the Northern timberline, their ice nucleation activity might be a cryoprotective mechanism. For comparison the ice nucleation activity of Snomax, fungal spores, and mushrooms will be discussed as well. In the past, pollen have been rejected as important atmospheric IN, as they are not as abundant in the atmosphere as bacteria or mineral dust and are too heavy to reach higher altitudes. However, in our experiments (Pummer et al. 2011) it turned out that water, which had been in contact with pollen and then been separated from the bodies, nucleates as good as the pollen grains themselves. So the ice nuclei have to be easily-suspendable macromolecules (100-300 kDa) located on the pollen. Once extracted, they can be distributed further through the atmosphere than the heavy pollen grains and so augment the impact of pollen on ice cloud formation even in the upper troposphere. It is widely known, that material from the pollen, like allergens and sugars, can indeed leave the pollen body and be distributed independently. The most probable mechanism is the pollen grain bursting by rain, which releases

  14. Calibration correction of an active scattering spectrometer probe to account for refractive index of stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Overbeck, V. R.; Snetsinger, K. G.; Russell, P. B.; Ferry, G. V.

    1990-01-01

    The use of the active scattering spectrometer probe (ASAS-X) to measure sulfuric acid aerosols on U-2 and ER-2 research aircraft has yielded results that are at times ambiguous due to the dependence of particles' optical signatures on refractive index as well as physical dimensions. The calibration correction of the ASAS-X optical spectrometer probe for stratospheric aerosol studies is validated through an independent and simultaneous sampling of the particles with impactors; sizing and counting of particles on SEM images yields total particle areas and volumes. Upon correction of calibration in light of these data, spectrometer results averaged over four size distributions are found to agree with similarly averaged impactor results to within a few percent: indicating that the optical properties or chemical composition of the sample aerosol must be known in order to achieve accurate optical aerosol spectrometer size analysis.

  15. Transmission Electron Microscopy Analysis of Submicronic Aerosol Particles Sampled at Jungfraujoch, Switzerland (CLACE-4)

    NASA Astrophysics Data System (ADS)

    Grobéty, B.; Lorenzo, R.

    2007-05-01

    Submicronic aerosol particles were collected in two sampling campaigns during CLACE-4 and -5 ("the Cloud and Aerosol Characterisation Experiment in the Free Troposphere") at the high alpine research station on top of Jungfraujoch (altitude: 3580 m.a.s.l.). The particles were deposited directly on transmission electron microscopy (TEM) grids placed in a home-made, calibrated thermophoretic sampling device. The samples were taken during periods of clear skies and temperatures below 0°C. Average sampling time was two days. The primary state of the particles was either solid, mixed solid-liquid or completely liquid. EDS spectra of solid particles without visible traces of a liquid coating contain only carbon and oxygen peaks. Mixed solid-fluid particles, however, have either carbon (C), mixed carbon-silicate (CS) or silicate (S) (probably SiO2) nuclei. The condensates remaining after evaporation of the liquid components contain sulfate (sulfur and oxygen peaks in EDS spectra), but no nitrate was found. The fraction > 500 nm is dominated by C and CS particles, the silicate particles have a narrow size distribution around 100 nm and contain, if at all, only faint sulfur peaks in their EDS spectra. The results are qualitatively consistent with analyses of samples collected during the same campaign (Weinbruch et al., 2005), but during mixed cloud events. There seem to be, however a differrence in the amount of particles with sulfate coatings, which is higher for samples taken under clear sky conditions. Weinbruch, S., Ebert, S., Worringen, A., and Brenker (2005), Identification of the ice forming fraction of the atmospheric aerosol in mixed-phase clouds by environmental scanning electron microscopy. Activity report 2005, International Foundation HFSJG.

  16. Method for determining aerosol particle size, device for determining aerosol particle size

    DOEpatents

    Novick, V.J.

    1998-10-06

    A method for determining the mass median diameter D of particles contained in a fluid is provided wherein the data of the mass of a pre-exposed and then a post-exposed filter is mathematically combined with data concerning the pressure differential across the same filter before and then after exposure to a particle-laden stream. A device for measuring particle size is also provided wherein the device utilizes the above-method for mathematically combining the easily quantifiable data. 2 figs.

  17. Dynamics of Aerosol Particles in Stationary, Isotropic Turbulence

    NASA Technical Reports Server (NTRS)

    Collins, Lance R.; Meng, Hui

    2004-01-01

    A detailed study of the dynamics of sub-Kolmogorov-size aerosol particles in stationary isotropic turbulence has been performed. The study combined direct numerical simulations (DNS; directed by Prof. Collins) and high-resolution experimental measurements (directed by Prof. Meng) under conditions of nearly perfect geometric and parametric overlap. The goal was to measure the accumulation of particles in low-vorticity regions of the flow that arises from the effect commonly referred to as preferential concentration. The grant technically was initiated on June 13, 2000; however, funding was not available until July 11, 2000. The grant was originally awarded to Penn State University (numerical simulations) and SUNY-Buffalo (experiments); however, Prof. Collins effort was moved to Cornell University on January 2002 when he joined that university. He completed the study there. A list of the specific tasks that were completed under this study is presented.

  18. Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Knopf, Daniel A.

    2014-07-01

    Organic aerosol can exhibit different phase states in response to changes in relative humidity (RH), thereby influencing heterogeneous reaction rates with trace gas species. OH radical uptake by laboratory-generated levoglucosan and methyl-nitrocatechol particles, serving as surrogates for biomass burning aerosol, is determined as a function of RH. Increasing RH lowers the viscosity of amorphous levoglucosan aerosol particles enabling enhanced OH uptake. Conversely, OH uptake by methyl-nitrocatechol aerosol particles is suppressed at higher RH as a result of competitive coadsorption of H2O that occupies reactive sites. This is shown to have substantial impacts on organic aerosol lifetimes with respect to OH oxidation. The results emphasize the importance of organic aerosol phase state to accurately describe the multiphase chemical kinetics and thus chemical aging process in atmospheric models to better represent the evolution of organic aerosol and its role in air quality and climate.

  19. 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.

  20. Real-Time Detection Method And System For Identifying Individual Aerosol Particles

    DOEpatents

    Gard, Eric Evan; Fergenson, David Philip

    2005-10-25

    A method and system of identifying individual aerosol particles in real time. Sample aerosol particles are compared against and identified with substantially matching known particle types by producing positive and negative test spectra of an individual aerosol particle using a bipolar single particle mass spectrometer. Each test spectrum is compared to spectra of the same respective polarity in a database of predetermined positive and negative spectra for known particle types and a set of substantially matching spectra is obtained. Finally the identity of the individual aerosol particle is determined from the set of substantially matching spectra by determining a best matching one of the known particle types having both a substantially matching positive spectrum and a substantially matching negative spectrum associated with the best matching known particle type.

  1. Quantitative ED-EPMA of Individual Particles and its Application for Characterization of Atmospheric Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Ro, C.

    2008-12-01

    An electron probe X-ray microanalysis (EPMA) technique using an energy-dispersive X-ray detector with an ultra-thin window, named low-Z particle EPMA, has been developed. The low-Z particle EPMA allows the quantitative determination of concentrations of low-Z elements such as C, N, and O, as well as higher-Z elements that can be analyzed by conventional energy-dispersive EPMA (ED-EPMA). The quantitative determination of low-Z elements (using full Monte Carlo simulations, from the electron impact to the X-ray detection) in individual environmental particles has improved the applicability of single-particle analysis, especially in atmospheric environmental aerosol research; many environmentally important atmospheric particles, e.g. sulfates, nitrates, ammonium, and carbonaceous particles, contain low-Z elements. In addition, an expert system that can perform chemical speciation from the elemental composition data obtained by the low-Z particle EPMA has been developed. The low-Z particle EPMA was applied to characterize K-feldspar particle samples of which the chemical compositions are well defined by the use of various bulk analytical methods. Chemical compositions of the K-feldspar samples obtained from the low-Z particle EPMA turn out to be very close to those from bulk analyses. The low-Z particle EPMA technique has been applied for the characterization of atmospheric aerosol particle samples, including Asian dust, urban, and indoor particulate samples: (1) The extent of chemical modification of Asian dust particles sampled in Chuncheon and Incheon, Korea, during several Asian dust storm events occurred in 2002-2006 was investigated. Mixing of Asian dust with air pollutants and sea-salts strongly depends on the characteristics of Asian dust storm events such as air-mass backward trajectories. For instance, no significant chemical modification of mineral dust corresponded to fast moving air-masses at high altitudes. Inversely, extensive chemical modification was

  2. Microscopic Characterization of Carbonaceous Aerosol Particle Aging in the Outflow from Mexico City

    SciTech Connect

    Moffet, R. C.; Henn, T. R.; Tivanski, A. V.; Hopkins, R. J.; Desyaterik, Y.; Kilcoyne, A. L. D.; Tyliszczak, T.; Fast, J.; Barnard, J.; Shutthanandan, V.; Cliff, S.S.; Perry, K. D.; Laskin, A.; Gilles, M. K.

    2009-09-16

    This study was part of the Megacities Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in Mexico City Metropolitan Area during spring 2006. The physical and chemical transformations of particles aged in the outflow from Mexico City were investigated for the transport event of 22 March 2006. A detailed chemical analysis of individual particles was performed using a combination of complementary microscopy and micro-spectroscopy techniques. The applied techniques included scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure spectroscopy (NEXAFS) and computer controlled scanning electron microscopy with an energy dispersive X-ray analyzer (CCSEM/EDX). As the aerosol plume evolves from the city center, the organic mass per particle increases and the fraction of carbon-carbon double bonds (associated with elemental carbon) decreases. Organic functional groups enhanced with particle age include: carboxylic acids, alkyl groups, and oxygen bonded alkyl groups. At the city center (T0) the most prevalent aerosol type contained inorganic species (composed of sulfur, nitrogen, oxygen, and potassium) coated with organic material. At the T1 and T2 sites, located northeast of T0 (~;;29 km and ~;;65 km, respectively), the fraction of homogenously mixed organic particles increased in both size and number. These observations illustrate the evolution of the physical mixing state and organic bonding in individual particles in a photochemically active environment.

  3. Morphological characterization of soot aerosol particles during LACIS Experiment in November (LExNo)

    NASA Astrophysics Data System (ADS)

    Kiselev, A.; Wennrich, C.; Stratmann, F.; Wex, H.; Henning, S.; Mentel, T. F.; Kiendler-Scharr, A.; Schneider, J.; Walter, S.; Lieberwirth, I.

    2010-06-01

    Combined mobility and aerodynamic measurements were used to characterize the morphology of soot particles in an experimental campaign on the hygroscopic growth and activation of an artificial biomass burning aerosol. A custom-made, single-stage low-pressure impactor and two aerosol mass spectrometers (AMS) operating in the free molecular regime were used to measure the vacuum aerodynamic diameter of mobility-selected artificial soot particles that were produced in a spark discharge generator and then modified by condensation of ammonium hydrogen sulfate or levoglucosan as a coating to change their hydroscopic activity. Transmission electron microscope images revealed a relationship between the electrical mobility diameter and the diameter of the enveloping sphere, thus enabling evaluation of the effective density of soot agglomerates. A fractal description of the morphology of the soot aggregates allowed for evaluation of the average mass of the hygroscopic material per particle. The average mass of the hygroscopic material per particle was also measured directly with the two AMS instruments, and the agreement between the two methods was found satisfactory. This tandem approach allows detection of small changes in the particle effective density and morphology caused by condensation of organic material.

  4. Uptake of 13N-labeled N2O5 to citric acid aerosol particles

    NASA Astrophysics Data System (ADS)

    Grzinic, Goran; Bartels-Rausch, Thorsten; Birrer, Mario; Türler, Andreas; Ammann, Markus

    2013-04-01

    Dinitrogen pentoxide is a significant reactive intermediate in the night time chemistry of nitrogen oxides. Depending on atmospheric conditions it can act either as a NO3 radical reservoir or as a major NOx sink by heterogeneous hydrolysis on aerosol surfaces. As such, it can influence tropospheric ozone production and therefore the oxidative capacity of the atmosphere. Furthermore it's suspected of being a non negligible source of tropospheric Cl, even over continental areas [1,2]. We used the short-lived radioactive tracer 13N delivered by PSI's PROTRAC facility [3] in conjunction with an aerosol flow tube reactor in order to study N2O5 uptake kinetics on aerosol particles. 13NO is mixed with non labeled NO and O3 in a gas reactor where N2O5 is synthesized under dry conditions to prevent hydrolysis on the reactor walls. The resulting N2O5 flow is fed into an aerosol flow tube reactor together with a humidified aerosol flow. By using movable inlets we can vary the length of the aerosol flow tube and thus the reaction time. The gas feed from the reactor is then directed into a narrow parallel plate diffusion denuder system that allows for selective separation of the gaseous species present in the gas phase. Aerosol particles are trapped on a particle filter placed at the end of the denuder system. The activity of 13N labeled species trapped on the denuder plates and in the particle filter can be monitored via scintillation counters. Aerosol uptake measurements were performed with citric acid aerosols in a humidity range of 27-61.5% RH. The results obtained from our measurements have shown that the uptake coefficient increases with humidity from 1.65±0.3x10-3 (~27% RH) to 1.25±0.3x10-2 (45% RH) and 2.00±0.3x10-2 (61.5% RH). Comparison to literature data shows that this is similar to values reported for some polycarboxylic acids (like malonic acid), while being higher than some others [4]. The increase is likely related to the increasing amount of water associated

  5. Review: engineering particles using the aerosol-through-plasma method

    SciTech Connect

    Phillips, Jonathan; Luhrs, Claudia C; Richard, Monique

    2009-01-01

    For decades, plasma processing of materials on the nanoscale has been an underlying enabling technology for many 'planar' technologies, particularly virtually every aspect of modern electronics from integrated-circuit fabrication with nanoscale elements to the newest generation of photovoltaics. However, it is only recent developments that suggest that plasma processing can be used to make 'particulate' structures of value in fields, including catalysis, drug delivery, imaging, higher energy density batteries, and other forms of energy storage. In this paper, the development of the science and technology of one class of plasma production of particulates, namely, aerosol-through-plasma (A-T-P), is reviewed. Various plasma systems, particularly RF and microwave, have been used to create nanoparticles of metals and ceramics, as well as supported metal catalysts. Gradually, the complexity of the nanoparticles, and concomitantly their potential value, has increased. First, unique two-layer particles were generated. These were postprocessed to create unique three-layer nanoscale particles. Also, the technique has been successfully employed to make other high-value materials, including carbon nanotubes, unsupported graphene, and spherical boron nitride. Some interesting plasma science has also emerged from efforts to characterize and map aerosol-containing plasmas. For example, it is clear that even a very low concentration of particles dramatically changes plasma characteristics. Some have also argued that the local-thermodynamic-equilibrium approach is inappropriate to these systems. Instead, it has been suggested that charged- and neutral-species models must be independently developed and allowed to 'interact' only in generation terms.

  6. Particle emission factors during cooking activities

    NASA Astrophysics Data System (ADS)

    Buonanno, G.; Morawska, L.; Stabile, L.

    Exposure to particles emitted by cooking activities may be responsible for a variety of respiratory health effects. However, the relationship between these exposures and their subsequent effects on health cannot be evaluated without understanding the properties of the emitted aerosol or the main parameters that influence particle emissions during cooking. Whilst traffic-related emissions, stack emissions and concentrations of ultrafine particles (UFPs, diameter < 100 nm) in urban ambient air have been widely investigated for many years, indoor exposure to UFPs is a relatively new field and in order to evaluate indoor UFP emissions accurately, it is vital to improve scientific understanding of the main parameters that influence particle number, surface area and mass emissions. The main purpose of this study was to characterise the particle emissions produced during grilling and frying as a function of the food, source, cooking temperature and type of oil. Emission factors, along with particle number concentrations and size distributions were determined in the size range 0.006-20 μm using a Scanning Mobility Particle Sizer (SMPS) and an Aerodynamic Particle Sizer (APS). An infrared camera was used to measure the temperature field. Overall, increased emission factors were observed to be a function of increased cooking temperatures. Cooking fatty foods also produced higher particle emission factors than vegetables, mainly in terms of mass concentration, and particle emission factors also varied significantly according to the type of oil used.

  7. Deposition flux of aerosol particles and 15 polycyclic aromatic hydrocarbons in the North China Plain.

    PubMed

    Wang, Xilong; Liu, Shuzhen; Zhao, Jingyu; Zuo, Qian; Liu, Wenxin; Li, Bengang; Tao, Shu

    2014-04-01

    The present study examined deposition fluxes of aerosol particles and 15 polycyclic aromatic hydrocarbons (PAHs) associated with the particles in the North China Plain. The annual mean deposition fluxes of aerosol particles and 15 PAHs were 0.69 ± 0.46 g/(m(2) ×d) and 8.5 ± 6.2 μg/(m(2) ×d), respectively. Phenanthrene, fluoranthene, pyrene, chrysene, benzo[b]fluoranthene, and benzo[k]fluoranthene were the dominant PAHs bound to deposited aerosol particles throughout the year. The total concentration of 15 PAHs in the deposited aerosol particles was the highest in winter but lowest in spring. The highest PAH concentration in the deposited aerosol particles in winter was because the heating processes highly increased the concentration in atmospheric aerosol particles. Low temperature and weak sunshine in winter reduced the degradation rate of deposited aerosol particle-bound PAHs, especially for those with low molecular weight. The lowest PAH concentration in deposited aerosol particles in spring resulted from the frequently occurring dust storms, which diluted PAH concentrations. The mean deposition flux of PAHs with aerosol particles in winter (16 μg/[m(2) ×d]) reached 3 times to 5 times that in other seasons (3.5-5.0 μg/[m(2) ×d]). The spatial variation of the deposition flux of PAHs with high molecular weight (e.g., benzo[a]pyrene) was consistent with their concentrations in the atmospheric aerosol particles, whereas such a phenomenon was not observed for those with low molecular weight (e.g., phenanthrene) because of their distinct hydrophobicity, Henry's law constant, and the spatially heterogeneous meteorological conditions.

  8. Experimental Assessment of Collection Efficiency of Submicron Aerosol Particles by Cloud Droplets

    NASA Astrophysics Data System (ADS)

    Huang, Y.; Ardon-Dryer, K.; Cziczo, D. J.

    2013-12-01

    The interplay between aerosol particles and water droplets in the atmosphere, especially in clouds, influences both aerosol and cloud properties. The major uncertainty in our understanding of climate arises in the indirect effect of aerosol and their ability to impact cloud formation and consequently alter the global radiative balance. The collision between a water droplet and aerosol particles that results in coalescence is termed 'collection' or 'coagulation'. Coagulation can lead to aerosol removal from the atmosphere or induce ice nucleation via contact freezing at temperatures below 0 C. Theoretical studies have shown that for aerosol particles smaller than 0.1 micrometers, Brownian motion is important, and for particles with diameters larger than 1 micrometer, inertial force dominates. There is a collection efficiency minimum for particles between 0.1-2 micrometers, called the 'Greenfield Gap'. Experimental efforts, however, have been limited to very large drizzle and rain drops until recently, and constrained parameters necessary to describe particle collection efficiency by cloud droplets have not been available. One reason is that laboratory setups that allow for coagulation to be observed on a single-particle basis have been lacking. Collection efficiency is also an important parameter for studying and assessing contact ice nucleation. Contact ice nucleation is currently the least understood ice nucleation mechanism and can be potentially important for mixed-phase cloud formation. The significance of experimentally assessing collection efficiency is therefore two-fold: to first understand the frequency of contacts and to then understand the fraction that lead to ice nucleation. We have constructed the MIT-Contact Freezing Chamber (MIT-CFC) to study collection efficiency of submicron aerosol particles by cloud droplets and contact freezing. A stream of 30-micron cloud droplets fall freely into the chamber and collide with aerosol particles. The outflow

  9. Use of stable carbon and nitrogen isotope ratios in size segregated aerosol particles for the O/I penetration evaluation

    NASA Astrophysics Data System (ADS)

    Garbaras, Andrius; Garbariene, Inga; Masalaite, Agne; Ceburnis, Darius; Krugly, Edvinas; Kvietkus, Kestutis; Remeikis, Vidmantas; Martuzevicius, Dainius

    2015-04-01

    particles penetrates from outside to inside. Observed isotope ratio depletion indicates that information about aerosol sources can be lost if measurements are performed only inside house. Using carbon and nitrogen isotope ratios data set, we were able to identify and distinguish main aerosol sources (traffic, heating activities) and penetration of aerosol particles from outdoor to indoor. Acknowledgment This work was supported by Research Council of Lithuania under grant "Pollution Control in Biomass Combustion: from Pollutant Formation to Human Exposure" (BioMassPoll), Project no. ATE05/2012. EPA Ireland is acknowledged for the fellowship grant of D. Ceburnis 1. Garbaras, A. Masalaite, I. Garbariene, D. Ceburnis, E. Krugly V. Remeikis, E. Puida K. Kvietkus, D. Martuzevicius, Stable carbon fractionation in size-segregated aerosol particles produced by controlled biomass burning, Journal of Aerosol Science, Vol. 79, p. 86-96 (2015); 2. D. Ceburnis, A. Garbaras, S. Szidat, M. Rinaldi, S. Fahrni, N. Perron, L. Wacker, S. Leinert, V. Remeikis, M. C. Facchini, A. S. H. Prevot, S. G. Jennings, and C. D. O'Dowd, Quantification of the carbonaceous matter origin in submicron marine aerosol particles by dual carbon isotope analysis, Atmospheric Chemistry and Physics, Vol 11, pp. 8593-8606 (2011); 3. V. Ulevicius, S. Bycenkiene, V. Remeikis, A. Garbaras, S. Kecorius, J. Andriejauskiene, D. Jasineviciene, G. Mocnik, Characterization of pollution events in the East Baltic region affected by regional biomass fire emissions, Atmospheric Research, Vol. 98 (2-4), pp. 190-200 (2010).

  10. Individual aerosol particles in and below clouds along a Mt. Fuji slope: Modification of sea-salt-containing particles by in-cloud processing

    NASA Astrophysics Data System (ADS)

    Ueda, S.; Hirose, Y.; Miura, K.; Okochi, H.

    2014-02-01

    Sizes and compositions of atmospheric aerosol particles can be altered by in-cloud processing by absorption/adsorption of gaseous and particulate materials and drying of aerosol particles that were formerly activated as cloud condensation nuclei. To elucidate differences of aerosol particles before and after in-cloud processing, aerosols were observed along a slope of Mt. Fuji, Japan (3776 m a.s.l.) during the summer in 2011 and 2012 using a portable laser particle counter (LPC) and an aerosol sampler. Aerosol samples for analyses of elemental compositions were obtained using a cascade impactor at top-of-cloud, in-cloud, and below-cloud altitudes. To investigate composition changes via in-cloud processing, individual particles (0.5-2 μm diameter) of samples from five cases (days) collected at different altitudes under similar backward air mass trajectory conditions were analyzed using a transmission electron microscope (TEM) equipped with an energy dispersive X-ray analyzer. For most cases (four cases), most particles at all altitudes mainly comprised sea salts: mainly Na with some S and/or Cl. Of those, in two cases, sea-salt-containing particles with Cl were found in below-cloud samples, although sea-salt-containing particles in top-of-cloud samples did not contain Cl. This result suggests that Cl in the sea salt was displaced by other cloud components. In the other two cases, sea-salt-containing particles on samples at all altitudes were without Cl. However, molar ratios of S to Na (S/Na) of the sea-salt-containing particles of top-of-cloud samples were higher than those of below-cloud samples, suggesting that sulfuric acid or sulfate was added to sea-salt-containing particles after complete displacement of Cl by absorption of SO2 or coagulation with sulfate. The additional volume of sulfuric acid in clouds for the two cases was estimated using the observed S/Na values of sea-salt-containing particles. The estimation revealed that size changes by in

  11. 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.

  12. 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.

  13. Use of analytical electron microscopy for the individual particle analysis of the Arctic haze aerosol

    SciTech Connect

    Sheridan, P.J.

    1986-01-01

    To explore the usefulness of the analytical electron microscope for the analysis and source apportionment of individual aerosol particles, aerosol samples amenable to individual particle analysis were collected from a remote region. These samples were from the Arctic haze aerosol, and were collected on board a research aircraft during the Arctic Gas and Aerosol Sampling Program in spring 1983. Before elemental analysis by analytical electron microscopy (AEM) could be performed, an extensive relative sensitivity factor study was undertaken to calibrate the microscope/detector system for quanitative x-ray microanalysis. Subsequently determined elemental data, along with morphological information, were used to group the particles into classes with similar characteristics. Forty-seven classes of particles were found in the Arctic samples, the most populous classes containing H/sub 2/SO/sub 4/ droplets, carbonaceous particles, lithophilic particles, CaSO/sub 4/ or NaCl. Several classes containing anthropogenic particles were also identified.

  14. Modeling the evolution of aerosol particles in a ship plume using PartMC-MOSAIC

    NASA Astrophysics Data System (ADS)

    Tian, J.; Riemer, N.; Pfaffenberger, L.; Schlager, H.; Petzold, A.

    2013-06-01

    This study investigates the evolution of ship-emitted aerosol particles using the stochastic particle-resolved model PartMC-MOSAIC. Comparisons of our results with observations from the QUANTIFY Study in 2007 in the English channel and the Gulf of Biscay showed that the model was able to reproduce the observed evolution of total number concentration and the vanishing of the nucleation mode consisting of sulfate particles. Further process analysis revealed that during the first hour after emission, dilution reduced the total number concentration by four orders of magnitude, while coagulation reduced it by an additional order of magnitude. Neglecting coagulation resulted in an overprediction of more than one order of magnitude in the number concentration of particles smaller than 40 nm at a plume age of 100 s. Coagulation also significantly altered the mixing state of the particles, leading to a continuum of internal mixtures of sulfate and black carbon. The impact on cloud condensation nuclei (CCN) concentrations depended on the supersaturation threshold S at which CCN activity was evaluated. For the base case conditions simulated here, characterized by a low formation rate of secondary aerosol species, neglecting coagulation led to an underestimation of CCN concentrations of about 20% for S=0.6% and of about 40% for S=0.3%. For S=0.1% the differences between simulations including coagulation and neglecting coagulation were negligible.

  15. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

    PubMed

    Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

    2013-12-17

    The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

  16. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds

    PubMed Central

    Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H.; Rudich, Yinon

    2013-01-01

    The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges. PMID:24297908

  17. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

    PubMed

    Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

    2013-12-17

    The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges. PMID:24297908

  18. 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.

  19. Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

    NASA Technical Reports Server (NTRS)

    Kaufman, Y. J.; Gitelson, A.; Karnieli, A.; Ganor, E. (Editor); Fraser, R. S.; Nakajima, T.; Mattoo, S.; Holben, B. N.

    1994-01-01

    Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  1. The effect of local sources on particle size and chemical composition and their role in aerosol-cloud interactions

    NASA Astrophysics Data System (ADS)

    Portin, H.; Leskinen, A.; Hao, L.; Kortelainen, A.; Miettinen, P.; Jaatinen, A.; Laaksonen, A.; Lehtinen, K. E. J.; Romakkaniemi, S.; Komppula, M.

    2013-12-01

    The effects of local pollutant sources and particle chemical composition on aerosol-cloud interactions were investigated by measuring cloud interstitial and total aerosol size distributions, particle chemical composition and hygroscopic growth factors and cloud droplet size distributions on an observation tower, with a special focus on comparing clean air masses with those affected by local sources. The polluted air masses contained more particles than the clean air masses in all size classes, excluding the accumulation mode. This was caused by cloud processing, which was also observed for the polluted air but to a lesser extent. Some, mostly minor, differences in the particle chemical composition between the air masses were observed. The average size and number concentration of activating particles were quite similar for both air masses, producing average droplet populations with only minor distinctions. As a case study, a long cloud event was analyzed in detail regarding emissions from local sources, including a paper mill and a heating plant. Clear differences in the total and accumulation mode particle concentrations, particle hygroscopicity and chemical composition during the cloud event were observed. Particularly, larger particles, higher hygroscopicities and elevated amounts of inorganic constituents, especially SO4, were linked with the pollutant plumes. In the air masses affected by traffic and domestic wood combustion, a bimodal particle hygroscopicity distribution was observed, indicating externally mixed aerosol. The variable conditions during the event had a clear impact on cloud droplet formation.

  2. Cloud condensation nuclei activity of aliphatic amine secondary aerosol

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The resulting particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate ...

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  4. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Shiraiwa, M.; Yee, L. D.; Schilling, K.; Loza, C. L.; Craven, J. S.; Zuend, A.; Ziemann, P. J.; Seinfeld, J.

    2013-12-01

    Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosol (SOA). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multi-generation gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a mid-experiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. The results of the current work have a number of implications for SOA models. While the dynamics of an aerosol size distribution reflects the mechanism of growth, we demonstrate here that it provides a key constraint in interpreting laboratory and ambient SOA formation. This work, although carried out specifically for the long chain alkane, dodecane, is expected to be widely applicable to other major classes of SOA precursors. SOA consists of a myriad of organic compounds containing various functional groups, which can generally undergo heterogeneous/multiphase reactions forming low-volatility products such as oligomers and other high molecular mass compounds. If particle-phase chemistry is indeed

  5. 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

  6. Cloud Formation Potential of Biomass Burning Aerosol Surrogate-Particles Chemically Aged by OH

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R. M.; Wang, J.; Li, Z. Q.; Knopf, D. A.

    2014-12-01

    Heterogeneous or multiphase reactions between trace gases such as OH and atmospheric aerosol can influence physicochemical properties of the particles including composition, morphology and lifetime. In this work, the cloud condensation nuclei (CCN) activity of laboratory-generated biomass burning aerosol (BBA) exposed to OH radicals is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type and OH exposure ([OH]×time) using a CCN counter coupled to a custom-built aerosol flow reactor (AFR). The composition of particles collected by a micro-orifice uniform deposit impactor (MOUDI) first subjected to different OH exposures is analyzed by Raman and scanning transmission X-ray microscopy coupled with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative compounds found in BBA that have different hygroscopicity, chemical functionalities, and reactivity with OH radicals. BBA surrogate-particles are generated following atomization of aqueous solutions with mass ratios LEV:MNC:KS of 1:0:0, 0:1:0, 0:0:1, 1:1:0, 0:1:1, 1:0:1, 1:1:1, and 1:0.03:0.3. OH radicals are generated in the AFR following photolysis of O3 in the presence of H2O using a variable intensity ultra-violet (UV) lamp, which allows equivalent atmospheric OH exposures from days to weeks. In addition, we investigate how κ changes i) in response to varying [O3] with and without OH, and ii) at a fixed OH exposure while varying RH. The impact of OH exposure on the CCN activity of BBA will be presented and its atmospheric implications will be discussed.

  7. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions.

    PubMed

    Che, H C; Zhang, X Y; Wang, Y Q; Zhang, L; Shen, X J; Zhang, Y M; Ma, Q L; Sun, J Y; Zhang, Y W; Wang, T T

    2016-01-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

  8. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

    NASA Astrophysics Data System (ADS)

    Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

    2016-04-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate.

  9. Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

    PubMed Central

    Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

    2016-01-01

    To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

  10. Glass transition measurements in mixed organic and organic/inorganic aerosol particles

    NASA Astrophysics Data System (ADS)

    Dette, Hans Peter; Qi, Mian; Schröder, David; Godt, Adelheid; Koop, Thomas

    2014-05-01

    The recent proposal of a semi-solid or glassy state of secondary organic aerosol (SOA) particles has sparked intense research in that area. In particular, potential effects of a glassy aerosol state such as incomplete gas-to-particle partitioning of semi-volatile organics, inhibited chemical reactions and water uptake, and the potential to act as heterogeneous ice nuclei have been identified so far. Many of these studies use well-studied proxies for oxidized organics such as sugars or other polyols. There are, however, few measurements on compounds that do exist in atmospheric aerosol particles. Here, we have performed studies on the phase state of organics that actually occur in natural SOA particles arising from the oxidation of alpha-pinene emitted in boreal forests. We have investigated the two marker compounds pinonic acid and 3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA) and their mixtures. 3-MBCTA was synthesized from methyl isobutyrate and dimethyl maleate in two steps. In order to transfer these substances into a glassy state we have developed a novel aerosol spray drying technique. Dilute solutions of the relevant organics are atomized into aerosol particles which are dried subsequently by diffusion drying. The dried aerosol particles are then recollected in an impactor and studied by means of differential scanning calorimetry (DSC), which provides unambiguous information on the aerosols' phase state, i.e. whether the particles are crystalline or glassy. In the latter case DSC is used to determine the glass transition temperature Tg of the investigated samples. Using the above setup we were able to determine Tg of various mixtures of organic aerosol compounds as a function of their dry mass fraction, thus allowing to infer a relation between Tg and the O:C ratio of the aerosols. Moreover, we also studied the glass transition behavior of mixed organic/inorganic aerosol particles, including the effects of liquid-liquid phase separation upon drying.

  11. METHODS OF CALCULATINAG LUNG DELIVERY AND DEPOSITION OF AEROSOL PARTICLES

    EPA Science Inventory


    Lung deposition of aerosol is measured by a variety of methods. Total lung deposition can be measured by monitoring inhaled and exhaled aerosols in situ by laser photometry or by collecting the aerosols on filters. The measurements can be performed accurately for stable monod...

  12. Cloud condensation nuclei activation of limited solubility organic aerosol

    NASA Astrophysics Data System (ADS)

    Huff Hartz, Kara E.; Tischuk, Joshua E.; Chan, Man Nin; Chan, Chak K.; Donahue, Neil M.; Pandis, Spyros N.

    The cloud condensation nuclei (CCN) activation of 19 organic species with water solubilities ( Csat) ranging from 10 -4 to 10 2 g solute 100 g -1 H 2O was measured. The organic particles were generated by nebulization of an aqueous or an alcohol solution. Use of alcohols as solvents enables the measurement of low solubility, non-volatile organic CCN activity and reduces the likelihood of residual water in the aerosol. The activation diameter of organic species with very low solubility in water ( Csat<0.3 g 100 g -1 H 2O) is in agreement with Köhler theory using the bulk solubility (limited solubility case) of the organic in water. Many species, including 2-acetylbenzoic acid, aspartic acid, azelaic acid, glutamic acid, homophthalic acid, phthalic acid, cis-pinonic acid, and salicylic acid are highly CCN active in spite of their low solubility (0.3 g 100 g -1 H 2O< Csat<1 g 100 g -1 H 2O), and activate almost as if completely water soluble. The CCN activity of most species is reduced, if the particles are produced using non-aqueous solvents. The existence of the particles in a metastable state at low RH can explain the observed enhancement in CCN activity beyond the levels suggested by their solubility.

  13. 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].

  14. Resuspension of Aerosol Particles from Evaporated Rain Drops to the Coarse Mode

    NASA Astrophysics Data System (ADS)

    Wang, H.; Easter, R. C.; Ganguly, D.; Singh, B.; Rasch, P. J.

    2015-12-01

    Precipitation scavenging (i.e., wet removal) has long been recognized as one of the major removal processes for tropospheric aerosol particles, and the dominant one for accumulation-mode size particles. When rain drops evaporate, the aerosol material contained in drops is resuspended, and this process has received much less attention. Unlike the resuspension from evaporated cloud droplets, the aerosol particles resuspended from evaporated rain drops have much larger sizes than most of the aerosol particles that acted as cloud condensation nuclei (CCN), became cloud borne, and then were collected by rain drops, because each rain drop generally collects thousands of cloud droplets. Here we present some aspects of this resuspension process obtained from modeling studies. First, we investigate some details of the process using a simple drop-size resolved model of raindrop evaporation in sub-saturated air below cloud base. Using these results, we then investigate different treatments of this process in a global aerosol and climate model that employs a modal aerosol representation. Compared to the model's original treatment of this process in which rain-borne aerosol is resuspended to the mode that it came from with its original size, the new treatment that resuspends to the coarse mode produces notable reductions in global CCN concentrations, as well as sulfate, black carbon, and organic aerosol mass, because the resuspended aerosol particles have much shorter lifetimes due to their larger sizes. Somewhat surprisingly, there are also notable reductions in coarse-mode sea salt and mineral dust burdens. These species are resuspended to the coarse mode in both the original and new treatments, but these resuspended particles are fewer in number and larger in size in the new treatment. This finding highlights some issues of the modal aerosol treatment for coarse mode particles.

  15. Parameterization of the Cloud Nucleating Activity of Fresh, Aged, and Internally-Mixed Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Kreidenweis, S.; Petters, M.; Demott, P.; Prenni, A.; Ziemann, P.

    2006-12-01

    Carbonaceous particle types affect global climate, visibility, and human health, but their primary and secondary sources, sinks, and tropospheric lifetimes are highly uncertain. The size and hygroscopicity of particles, and in particular their activity as cloud condensation nuclei (CCN), plays a large role in determining their atmospheric impacts and lifetimes. However, hygroscopicity is difficult to parameterize for many organic species for which no thermodynamic data exist, and for complex, multicomponent aerosols of undefined composition. We propose a simple method to describe the relationship between dry particle diameter and CCN activity using a single hygroscopicity parameter, κ. We derive values of κ from fitting of experimental CCN-activity data from the literature and from recent experiments, including oxidation-aged organic particles and secondary organic aerosols. Values of κ are between 0.5 and 2 for highly-CCN- active salts such as sodium chloride, between 0.01 and 0.5 for slightly to very hygroscopic organic aerosols such as those produced in biomass burning and as secondary organic aerosols, and 0 for nonhygroscopic components. The hygroscopicity of internal mixtures can be calculated as a volume fraction weighted average of the hygroscopicity parameters of the individual species comprising the mixture. Aging of aerosol, understood as changes in hygroscopicity due to condensation of hydrophilic species, coagulation of aerosol populations, or heterogeneous chemical reactions, are described conveniently by changes in κ. Our studies show that oxidative aging that proceeds by addition of functional groups to the CHx carbon backbone leads to only small changes in κ, and thus the process alone is inefficient at rendering small, initially- hydrophobic primary organic particles capable of being scavenged by cloud-drop nucleation. Other processes, such as coagulation and condensation, control the rate of hydrophobic-to-hydrophilic conversion of primary

  16. Inferring ammonium and sulfate aerosol concentrations using laser particle counters and condensation nuclei counters at summit, Greenland

    SciTech Connect

    Kuhns, H.; Davidson, C.; Bergin, M.

    1995-12-31

    Atmospheric measurements have been conducted in central Greenland over the last 10 years in connection with ice core research. While the primary objective of this research is to facilitate the quantitative interpretation of ice cores, interesting findings are being made in the field of Arctic air chemistry. In recent years, aerosol filters were run simultaneously with laser particle counters (LPC`s) and condensation nuclei counters (CNC`s). The LPC`s used in the this study count particles with diameters greater than 0.5 {mu}m, while the CNC`s count particles larger than approximately 0.01 {mu}m. Results from summertime aerosol sampling at Summit, Greenland are presented from the 1994 field season. Excellent agreement is observed between LPC data and particulate ammonium and sulfate. The correlation between ammonium and LPC data is r=0.88. Of all of the ionic species measured on the filters, the CNC results are in best agreement with MSA. The correlation for CNC and MSA is r=0.58. The relationship between the real-time particle sensor data and the aerosol chemistry has significant implications. The link between MSA and CNC supports the theory that marine biological activity enhances the production of cloud condensation nuclei. Also, this technique shows promise for remote sensing applications since once calibrated, the real time particle count data could be used to infer high temporal resolution aerosol chemistry.

  17. Modeling the evolution of aerosol particles in a ship plume using PartMC-MOSAIC

    NASA Astrophysics Data System (ADS)

    Tian, J.; Riemer, N.; West, M.; Pfaffenberger, L.; Schlager, H.; Petzold, A.

    2014-06-01

    This study investigates the evolution of ship-emitted aerosol particles using the stochastic particle-resolved model PartMC-MOSAIC (Particle Monte Carlo model-Model for Simulating Aerosol Interactions and Chemistry). Comparisons of our results with observations from the QUANTIFY (Quantifying the Climate Impact of Global and European Transport Systems) study in 2007 in the English Channel and the Gulf of Biscay showed that the model was able to reproduce the observed evolution of total number concentration and the vanishing of the nucleation mode consisting of sulfate particles. Further process analysis revealed that during the first hour after emission, dilution reduced the total number concentration by four orders of magnitude, while coagulation reduced it by an additional order of magnitude. Neglecting coagulation resulted in an overprediction of more than one order of magnitude in the number concentration of particles smaller than 40 nm at a plume age of 100 s. Coagulation also significantly altered the mixing state of the particles, leading to a continuum of internal mixtures of sulfate and black carbon. The impact on cloud condensation nuclei (CCN) concentrations depended on the supersaturation threshold S at which CCN activity was evaluated. For the base case conditions, characterized by a low formation rate of secondary aerosol species, neglecting coagulation, but simulating condensation, led to an underestimation of CCN concentrations of about 37% for S = 0.3% at the end of the 14-h simulation. In contrast, for supersaturations higher than 0.7%, neglecting coagulation resulted in an overestimation of CCN concentration, about 75% for S = 1%. For S lower than 0.2% the differences between simulations including coagulation and neglecting coagulation were negligible. Neglecting condensation, but simulating coagulation did not impact the CCN concentrations below 0.2% and resulted in an underestimation of CCN concentrations for larger supersaturations, e.g., 18

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

    SciTech Connect

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

    2012-06-13

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

  19. Electron mean free path from angle-dependent photoelectron spectroscopy of aerosol particles

    SciTech Connect

    Goldmann, Maximilian; Miguel-Sánchez, Javier; West, Adam H. C.; Yoder, Bruce L.; Signorell, Ruth

    2015-06-14

    We propose angle-resolved photoelectron spectroscopy of aerosol particles as an alternative way to determine the electron mean free path of low energy electrons in solid and liquid materials. The mean free path is obtained from fits of simulated photoemission images to experimental ones over a broad range of different aerosol particle sizes. The principal advantage of the aerosol approach is twofold. First, aerosol photoemission studies can be performed for many different materials, including liquids. Second, the size-dependent anisotropy of the photoelectrons can be exploited in addition to size-dependent changes in their kinetic energy. These finite size effects depend in different ways on the mean free path and thus provide more information on the mean free path than corresponding liquid jet, thin film, or bulk data. The present contribution is a proof of principle employing a simple model for the photoemission of electrons and preliminary experimental data for potassium chloride aerosol particles.

  20. Experimental Assessment of Collection Efficiency of Submicron Aerosol Particles by Cloud Droplets

    NASA Astrophysics Data System (ADS)

    Huang, Y.; Oo, K.; Brown, M. D.; Dhaniyala, S.; Cziczo, D. J.

    2012-12-01

    An experimental setup has been constructed to measure the collection efficiency of submicron aerosol particles by cloud droplets. The collection efficiency study is a prelude to studying contact nucleation, which is a potentially important ice nucleation mode that is not well-understood. This laboratory setup is a step closer to experimentally assessing the importance of contact nucleation. Water droplets with 20 micron diameter and submicron aerosol particles are brought into contact in an injector situated inside a chilled glass flow tube. The water droplets that collect aerosol particles are allowed to pass through a counterflow virtual impactor (CVI), which accepts large droplets and rejects aerosol particles that have not coagulated with the water droplets. The collected droplets are sent into the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument which performs in situ chemical analysis of a single particle. The number of aerosol particles collected by the single water droplet is quantified by calibrating the PALMS with known concentrations of aerosol particles. The water droplets contain a known amount of ammonium sulfate for identification purpose in the mass spectrometry. Preliminary results from the experiment will be discussed and compared with previous theoretical and experimental studies.

  1. 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.

  2. Emissions and Characteristics of Ice Nucleating Particles Associated with Laboratory Generated Nascent Sea Spray Aerosol

    NASA Astrophysics Data System (ADS)

    McCluskey, C. S.; Hill, T. C. J.; Beall, C.; Sultana, C. M.; Moore, K.; Cornwell, G.; Lee, C.; Al-Mashat, H.; Laskina, O.; Trueblood, J.; Grassian, V. H.; Prather, K. A.; Kreidenweis, S. M.; DeMott, P. J.

    2015-12-01

    Accurate emission rates and activity spectra of atmospheric ice nucleating particles (INPs) are required for proper representation of aerosol-cloud interactions in atmospheric modeling studies. However, few investigations have quantified or characterized oceanic INP emissions. In conjunction with the Center for Aerosol Impacts on the Climate and the Environment, we have directly measured changes in INP emissions and properties of INPs from nascent sea spray aerosol (SSA) through the evolution of phytoplankton blooms. Multiple offline and online instruments were used to monitor aerosol chemistry and size, and bulk water characteristics during two phytoplankton bloom experiments. Two methods were utilized to monitor the number concentrations of INPs from 0 to -34 °C: The online CSU continuous flow diffusion chamber (CFDC) and collections processed offline using the CSU ice spectrometer. Single particle analyses were performed on ice crystal residuals downstream of the CFDC, presumed to be INPs, via scanning transmission electron microscopy (STEM) and Raman microspectroscopy. Preliminary results indicate that laboratory-generated nascent SSA corresponds to number concentrations of INPs that are generally consistent with open ocean regions, based on current knowledge. STEM analyses revealed that the sizes of ice crystal residuals that were associated with nascent SSA ranged from 0.3 to 2.5 μm. Raman microspectroscopy analysis of 1 μm sized residuals found a variety of INP identities, including long chain organics, diatom fragments and polysaccharides. Our data suggest that biological processes play a significant role in ocean INP emissions by generating the species and compounds that were identified during these studies.

  3. Identification of characteristic mass spectrometric markers for primary biological aerosol particles and comparison with field data from submicron pristine aerosol particles

    NASA Astrophysics Data System (ADS)

    Freutel, F.; Schneider, J.; Zorn, S. R.; Drewnick, F.; Borrmann, S.; Hoffmann, T.; Martin, S. T.

    2009-04-01

    The contribution of primary biological aerosol (PBA) to the total aerosol particle concentration is estimated to range between 25 and 80%, depending on location and season. Especially in the tropical rain forest it is expected that PBA is a major source of particles in the supermicron range, and is also an important fraction of the submicron aerosol. PBA particles like plant fragments, pollen, spores, fungi, viruses etc. contain chemical compounds as proteins, sugars, amino acids, chlorophyll, and cellular material as cellulose. For this reason we have performed mass spectrometric laboratory measurements (Aerodyne C-ToF and W-ToF AMS, single particle laser ablation instrument SPLAT) on pure submicron aerosol particles containing typical PBA compounds in order to identify typical mass spectral patterns of these compounds and to explain the observed fragmentation patterns on the basis of molecular structures. These laboratory data were compared to submicron particle mass spectra obtained during AMAZE-08 (Amazonian Aerosol CharacteriZation Experiment, Brazil, February/March 2008). The results indicate that characteristic m/z ratios for carbohydrates (e.g., glucose, saccharose, levoglucosan, mannitol) can be identified, for example m/z = 60(C2H4O2+) or m/z = 61(C2H5O2+). Certain characteristic peaks for amino acids were also identified in the laboratory experiments. In the field data from AMAZE-08, these characteristic peaks for carbohydrates and amino acids were found, and their contribution to the total organic mass was estimated to about 5%. Fragment ions from peptides and small proteins were also identified in laboratory experiments. Larger proteins, however, seem to become oxidized to CO2+ to a large extend in the vaporizing process of the AMS. Thus, detection of proteins in atmospheric aerosol particles with the AMS appears to be difficult.

  4. 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

    Atmospheric aerosols strongly influence the global energy budget by scattering and absorbing sunlight (direct effects) and by changing the microphysical structure, lifetime, and coverage of clouds (indirect effects). Currently, the indirect effects of aerosols remain the most uncertain components in forcing of climate change over the industrial period. This large uncertainty is in part due to our incomplete understanding of the ability of aerosol particles to form cloud droplets under climatically relevant supersaturations. During CalNex study, size-resolved cloud condensation nuclei (CCN) spectrum and aerosol chemical composition were measured at an urban supersite in Pasadena, California from May 15 to June 6, 2010. Monodispersed aerosol particles are first classified using a differential mobility analyzer at sizes ranging from 25 to 320 nm. The activation efficiency of the classified aerosol, defined as the ratio of its CCN concentration (characterized by a DMT CCN counter) to total CN concentration (measured by a condensation particle counter, TSI 3771), is derived as a function of both particle size and supersaturation, which ranges from 0.08% to 0.39%. Aerosol chemical composition was characterized using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). In most of days, increases in aerosol mode diameter, organics mass loading, and aerosol organics volume fraction were observed from 10:00 AM to 15:00 PM. These increases are attributed to formation of secondary organic aerosols through photochemical reactions. On average, the aerosol was dominated by organics (~65% by volume), with the contribution from ammonium sulfate (~20%) and ammonium nitrate (~15%), and the balance being made up of elemental carbon. Positive matrix factorization (PMF) analysis shows the oxygenated organic aerosol (OOA) (~75%) was the dominant organics component. Additionally, the organics O:C ratio was within a narrow range of 0.50±0.12. Particle overall

  5. Enhanced high-temperature ice nucleation ability of crystallized aerosol particles after preactivation at low temperature

    NASA Astrophysics Data System (ADS)

    Wagner, Robert; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin

    2014-07-01

    In cloud chamber experiments with crystallized aqueous ammonium sulfate, oxalic acid, and succinic acid solution droplets, we have studied a preactivation mechanism that markedly enhances the particles' heterogeneous ice nucleation ability. First cloud expansion experiments were performed at a high temperature (267-244 K) where the crystallized particles did not promote any heterogeneous ice nucleation. Ice nucleation at this temperature, however, could be triggered by temporarily cooling the crystallized particles to a lower temperature. This is because upon crystallization, residuals of the aqueous solution are trapped within the crystals. These captured liquids can freeze when cooled below their respective homogeneous or heterogeneous freezing temperature, leading to the formation of ice pockets in the crystalline particles. When warmed again to the higher temperature, ice formation by the preactivated particles occurred via depositional and deliquescence-induced ice growth, with ice active fractions ranging from 1 to 4% and from 4 to 20%, respectively. Preactivation disappeared above the eutectic temperature, which for the organic acids are close to the melting point of ice. This mechanism could therefore contribute to the very small fraction of atmospheric aerosol particles that are still ice active well above 263 K.

  6. Investigating the Internal Structure of Individual Aerosol Particles Using Atomic Force and Raman Microscopies

    NASA Astrophysics Data System (ADS)

    Freedman, M. A.; Baustian, K. J.; Wise, M. E.; Tolbert, M. A.

    2009-12-01

    We have used Atomic Force Microscopy (AFM) and Raman Microscopy to probe aerosol internal structures in order to understand the optical properties of aerosols composed of mixtures of organic and inorganic components. While AFM gives only topographical information about the particles, indirect chemical information can be obtained by using substrates with different surface properties. With Raman microscopy, chemical signatures of the components of the aerosol are obtained, but we have limited spatial resolution. We have explored the use of these two techniques to look at aerosol internal structure using a range of different model aerosols composed of mixtures of ammonium sulfate with organic compounds of various solubilities such as sucrose, succinic acid, and palmitic acid. At the extremes of solubility, AFM provides suitable information for interpreting aerosol microstructure. For example, AFM clearly shows the presence of core-shell structures for aerosol particles composed of palmitic acid and ammonium sulfate, while the results for aerosol particles composed of succinic acid and ammonium sulfate are more difficult to interpret. Information about size and shape can be obtained when hydrophilic particles are impacted on hydrophobic substrates and vise versa. With Raman microscopy, core-shell structures were readily identified for ammonium sulfate with palmitic acid or succinic acid coatings. For the case of succinic acid and ammonium sulfate mixtures, we are using microscopy results to aid in interpreting the refractive indices we retrieved from cavity ring-down studies.

  7. Evaluation of cell sorting aerosols and containment by an optical airborne particle counter.

    PubMed

    Xie, Mike; Waring, Michael T

    2015-08-01

    Understanding aerosols produced by cell sorting is critical to biosafety risk assessment and validation of containment efficiency. In this study an Optical Airborne Particle Counter was used to analyze aerosols produced by the BD FACSAria and to assess the effectiveness of its aerosol containment. The suitability of using this device to validate containment was directly compared to the Glo-Germ method put forth by the International Society for Advancement of Cytometry (ISAC) as a standard for testing. It was found that high concentrations of aerosols ranging from 0.3 µm to 10 µm can be detected in failure mode, with most less than 5 µm. In most cases, while numerous aerosols smaller than 5 µm were detected by the Optical Airborne Particle Counter, no Glo-Germ particles were detected, indicating that small aerosols are under-evaluated by the Glo-Germ method. The results demonstrate that the Optical Airborne Particle Counter offers a rapid, economic, and quantitative analysis of cell sorter aerosols and represents an improved method over Glo-Germ for the task of routine validation and monitoring of aerosol containment for cell sorting. PMID:26012776

  8. A Micro Aerosol Sensor for the Measurement of Airborne Ultrafine Particles.

    PubMed

    Zhang, Chao; Zhu, Rong; Yang, Wenming

    2016-01-01

    Particle number concentration and particle size are the two key parameters used to characterize exposure to airborne nanoparticles or ultrafine particles that have attracted the most attention. This paper proposes a simple micro aerosol sensor for detecting the number concentration and particle size of ultrafine particles with diameters from 50 to 253 nm based on electrical diffusion charging. The sensor is composed of a micro channel and a couple of planar electrodes printed on two circuit boards assembled in parallel, which thus integrate charging, precipitating and measurement elements into one chip, the overall size of which is 98 × 38 × 25 mm³. The experiment results demonstrate that the sensor is useful for measuring monodisperse aerosol particles with number concentrations from 300 to 2.5 × 10⁴ /cm³ and particle sizes from 50 to 253 nm. The aerosol sensor has a simple structure and small size, which is favorable for use in handheld devices. PMID:26999156

  9. A Micro Aerosol Sensor for the Measurement of Airborne Ultrafine Particles

    PubMed Central

    Zhang, Chao; Zhu, Rong; Yang, Wenming

    2016-01-01

    Particle number concentration and particle size are the two key parameters used to characterize exposure to airborne nanoparticles or ultrafine particles that have attracted the most attention. This paper proposes a simple micro aerosol sensor for detecting the number concentration and particle size of ultrafine particles with diameters from 50 to 253 nm based on electrical diffusion charging. The sensor is composed of a micro channel and a couple of planar electrodes printed on two circuit boards assembled in parallel, which thus integrate charging, precipitating and measurement elements into one chip, the overall size of which is 98 × 38 × 25 mm3. The experiment results demonstrate that the sensor is useful for measuring monodisperse aerosol particles with number concentrations from 300 to 2.5 × 104 /cm3 and particle sizes from 50 to 253 nm. The aerosol sensor has a simple structure and small size, which is favorable for use in handheld devices. PMID:26999156

  10. Photochemical Activation of Chlorine by Iron and Iron Oxide Aerosol

    NASA Astrophysics Data System (ADS)

    Wittmer, J.; Zetzsch, C.

    2015-12-01

    The photochemical activation of chlorine by dissolved iron in sea-salt aerosol droplets and by highly dispersed Fe2O3 aerosol particles (mainly hematite, specific surface > 100 m2/g), exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic Cl. When the artificial sea salt aerosols contained suspended Fe2O3 alone at pH 6, no significant Cl production could be observed, even if the dissolution of iron was forced by "weathering" (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol/L, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8 × 1021 atoms cm-2 h-1, respectively. Exposing the pure Fe2O3 aerosol in the absence of salt to various gaseous HCl concentrations resulted in rates ranging from 8 × 1020 Cl atoms cm-2 h-1 (at ~4 ppb HCl) to 5 × 1022 Cl atoms cm-2 h-1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2-5 % mol/mol, depending on the relative humidity). The relevance for environmental processes in the atmosphere will be discussed.

  11. [Factors influencing particle measurement of aerosols and their retention in the lung].

    PubMed

    Le Bouffant, L

    1977-01-01

    The dimensional characteristics of the particles of an aerosol depend on the means used for producing them. Mechanical spray and ultrasonic dispersion give polydispersed particles. On the other hand, centrifugal atomization produces a monodispersed aerosol. Particle retention in the lung system depends on the particle diameter. In addition, retention varies according to the respiratory characteristics: it is minimal for about 15 inspirations per minute. Using iron-59 labeled particles, it was shown that the degree of retention varies considerably from one individual to the other and accessibility to the depths of the lungs is decreased under the effect of certain lesions. Bronchial retention appears to be increased in smokers.

  12. Estimating Marine Aerosol Particle Volume and Number from Maritime Aerosol Network Data

    NASA Technical Reports Server (NTRS)

    Sayer, A. M.; Smirnov, A.; Hsu, N. C.; Munchak, L. A.; Holben, B. N.

    2012-01-01

    As well as spectral aerosol optical depth (AOD), aerosol composition and concentration (number, volume, or mass) are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN) cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET) inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS) data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The average solution MODIS dataset agrees more closely with MAN than the best solution dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data.

  13. Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions

    NASA Astrophysics Data System (ADS)

    Mason, R. H.; Si, M.; Li, J.; Chou, C.; Dickie, R.; Toom-Sauntry, D.; Pöhlker, C.; Yakobi-Hancock, J. D.; Ladino, L. A.; Jones, K.; Leaitch, W. R.; Schiller, C. L.; Abbatt, J. P. D.; Huffman, J. A.; Bertram, A. K.

    2015-11-01

    Information on what aerosol particle types are the major sources of ice nucleating particles (INPs) in the atmosphere is needed for climate predictions. To determine which aerosol particles are the major sources of immersion-mode INPs at a coastal site in Western Canada, we investigated correlations between INP number concentrations and both concentrations of different atmospheric particles and meteorological conditions. We show that INP number concentrations are strongly correlated with the number concentrations of fluorescent bioparticles between -15 and -25 °C, and that the size distribution of INPs is most consistent with the size distribution of fluorescent bioparticles. We conclude that biological particles were likely the major source of ice nuclei at freezing temperatures between -15 and -25 °C at this site for the time period studied. At -30 °C, INP number concentrations are also well correlated with number concentrations of the total aerosol particles ≥ 0.5 μm, suggesting that non-biological particles may have an important contribution to the population of INPs active at this temperature. As we found that black carbon particles were unlikely to be a major source of ice nuclei during this study, these non-biological INPs may include mineral dust. Furthermore, correlations involving chemical tracers of marine aerosols and marine biological activity, sodium and methanesulfonic acid, indicate that the majority of INPs measured at the coastal site likely originated from terrestrial rather than marine sources. Finally, six existing empirical parameterizations of ice nucleation were tested to determine if they accurately predict the measured INP number concentrations. We found that none of the parameterizations selected are capable of predicting INP number concentrations with high accuracy over the entire temperature range investigated. This finding illustrates that additional measurements are needed to improve parameterizations of INPs and their

  14. Ambient measurement of fluorescent aerosol particles with a WIBS in the Yangtze River Delta of China: potential impacts of combustion-related aerosol particles

    NASA Astrophysics Data System (ADS)

    Yu, Xiawei; Wang, Zhibin; Zhang, Minghui; Kuhn, Uwe; Xie, Zhouqing; Cheng, Yafang; Pöschl, Ulrich; Su, Hang

    2016-09-01

    Fluorescence characteristics of aerosol particles in a polluted atmosphere were studied using a wideband integrated bioaerosol spectrometer (WIBS-4A) in Nanjing, Yangtze River Delta area of China. We observed strong diurnal and day-to-day variations of fluorescent aerosol particles (FAPs). The average number concentrations of FAPs (1-15 µm) detected in the three WIBS measurement channels (FL1: 0.6 cm-3, FL2: 3.4 cm-3, FL3: 2.1 cm-3) were much higher than those observed in forests and rural areas, suggesting that FAPs other than bioaerosols were detected. We found that the number fractions of FAPs were positively correlated with the black carbon mass fraction, especially for the FL1 channel, indicating a large contribution of combustion-related aerosols. To distinguish bioaerosols from combustion-related FAPs, we investigated two classification schemes for use with WIBS data. Our analysis suggests a strong size dependence for the fractional contributions of different types of FAPs. In the FL3 channel, combustion-related particles seem to dominate the 1-2 µm size range while bioaerosols dominate the 2-5 µm range. The number fractions of combustion-related particles and non-combustion-related particles to total aerosol particles were ˜ 11 and ˜ 5 %, respectively.

  15. Aerosol-CFD modelling of ultrafine and black carbon particle emission, dilution, and growth near roadways

    NASA Astrophysics Data System (ADS)

    Huang, L.; Gong, S. L.; Gordon, M.; Liggio, J.; Staebler, R. M.; Stroud, C. A.; Lu, G.; Mihele, C.; Brook, J. R.; Jia, C. Q.

    2014-05-01

    Many studies have shown that on-road vehicle emissions are the dominant source of ultrafine particles (UFP; diameter < 100 nm) in urban areas and near-roadway environments. In order to advance our knowledge on the complex interactions and competition among atmospheric dilution, dispersion and dynamics of UFPs, an aerosol dynamics-CFD coupled model is developed and validated against field measurements. A unique approach of applying periodic boundary conditions is proposed to model pollutant dispersion and dynamics in one unified domain from the tailpipe level to the ambient near-road environment. This approach significantly reduces the size of the computational domain, and therefore, allows fast simulation of multiple scenarios. The model is validated against measured turbulent kinetic energy (TKE) and pollution gradients near a major highway. Through a model sensitivity analysis, the relative importance of individual aerosol dynamical processes on the total particle number concentration (N) and particle number-size distribution (PSD) near a highway is investigated. The results demonstrate that (1) coagulation has a negligible effect on N and particle growth, (2) binary homogeneous nucleation (BHN) of H2SO4-H2O is likely responsible for elevated N closest to the road, (3) N and particle growth are very sensitive to the condensation of semi-volatile organics (SVOCs), particle dry deposition, and the interaction between these processes. The results also indicate that, without the proper treatment of atmospheric boundary layer (i.e. its wind profile and turbulence quantities), the nucleation rate would be underestimated by a factor of 5 in the vehicle wake region due to overestimated mixing. Therefore, introducing ABL conditions to activity-based emission models may potentially improve their performance in estimating UFP traffic emissions.

  16. Mixing state of ambient aerosols in Nanjing city by single particle mass spectrometry

    NASA Astrophysics Data System (ADS)

    Wang, Honglei; An, Junlin; Shen, Lijuan; Zhu, Bin; Xia, Li; Duan, Qing; Zou, Jianan

    2016-05-01

    To investigate the mixing state and size-resolved aerosol in Nanjing, measurements were carried out for the period 14th January-1st February 2013 by using a Single Particle Aerosol Mass Spectrometer (SPAMS). A total of 10,864,766 particles were sized with vacuum aerodynamic diameter (dva) in the range of 0.2-2.0 μm. Of which, 1,989,725 particles were successfully ionized. Aerosol particles employed for analyzing SPAMS data utilized 96% of the hit particles to identify 5 main particle groups. The particle classes include: K-rich particles (K-CN, K-Nitrate, K-Sulfate and K-Secondary), sodium particles, ammonium particles, carbon-rich particles (OC, EC and OCEC) and heavy-metal particles (Fe-Secondary, Pb-Nitrate, Cu-Mn-Secondary and V-Secondary). EC was the largest contributor with a fraction of 21.78%, followed by K-Secondary (17.87%), K-Nitrate (12.68%) and K-CN (11.25%). High particle level and high RH (relative humidity) are two important factors decreasing visibility in Nanjing. Different particle classes have distinct extinction effects. It anti-correlated well with visibility for the K-secondary, sodium, ammonium, EC, Fe-Secondary and K-Nitrate particles. The proportion of EC particles at 0.65-1.4 μm was up to 25% on haze days and was below 10% on clean days.

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

    DOE PAGES

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

    2015-09-25

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

  18. 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.

  19. Field observations in continental stratiform clouds: Partitioning of cloud particles between droplets and unactivated interstitial aerosols

    NASA Astrophysics Data System (ADS)

    Gillani, N. V.; Schwartz, S. E.; Leaitch, W. R.; Strapp, J. W.; Isaac, G. A.

    1995-09-01

    The partitioning of cloud particles between activated droplets and unactivated interstitial aerosols is a primary determinant of cloud microphysical, radiative, and chemical properties. In the present study, high-resolution aircraft measurements (1 s, ˜60 m) of the number concentrations (Namp and Ncd) of accumulation-mode particles (AMP, 0.17 to 2.07 μm diameter) and cloud droplets (CD, 2 to 35 μm diameter), made during 10 flights in and around continental stratiform clouds near Syracuse, New York, in autumn 1984 have been used to study the local and instantaneous nature of cloud particle partitioning throughout the sampled clouds. The partitioning is defined as the activated fraction F (≡Ncd/Ntot) of all measured cloud particles (Ntot ≡ Namp + Ncd). F may be interpreted approximately as the AMP activation efficiency which is often assumed to be unity in all clouds. In the present study, F varied over its full possible range (0 to 1), being low especially in cloud edges. Even in the near-adiabatic parts of cloud interior, its variation ranged from 0.1 to 1 over the 10 days. Statistically, its value in cloud interior exceeded 0.9 in 36% of the data but was below 0.6 in 28%. On 5 of the 10 days, stratocumulus clouds were embedded in cool, dry, and relatively clean (Ntot < 600 cm-3) northerly air masses. In such cases, cloud droplet concentration increased approximately linearly with increasing total particle loading, and F in cloud interior was near unity and relatively insensitive to changes in the influencing variables. On the other days, especially in stratus clouds embedded in warm and polluted southerly air masses, F was significantly less than unity, with particles in the smallest size ranges (0.17 to 0.37 μm) activating only fractionally depending on several factors. An important feature of the clouds sampled in this study was the existence of multiple cloud layers and complex vertical thermal structure on most days. Consequently, our analysis of the

  20. Particle size distribution of the stratospheric aerosol from SCIAMACHY limb measurements

    NASA Astrophysics Data System (ADS)

    Rozanov, Alexei; Malinina, Elizaveta; Rozanov, Vladimir; Hommel, Rene; Burrows, John

    2016-04-01

    Stratospheric aerosols are of a great scientific interest because of their crucial role in the Earth's radiative budget as well as their contribution to chemical processes resulting in ozone depletion. While the permanent aerosol background in the stratosphere is determined by the tropical injection of SO2, COS and sulphate particles from the troposphere, major perturbations of the stratospheric aerosol layer result form an uplift of SO2 after strong volcanic eruptions. Satellite measurements in the visible spectral range represent one of the most important sources of information about the vertical distribution of the stratospheric aerosol on the global scale. This study employs measurements of the scattered solar light performed in the limb viewing geometry from the space borne spectrometer SCIAMACHY, which operated onboard the ENVISAT satellite, from August 2002 to April 2012. A retrieval approach to obtain parameters of the stratospheric aerosol particle size distribution will be reported along with the sensitivity studies and first results.

  1. Microspectroscopic Analysis of Anthropogenic- and Biogenic-Influenced Aerosol Particles during the SOAS Field Campaign

    NASA Astrophysics Data System (ADS)

    Ault, A. P.; Bondy, A. L.; Nhliziyo, M. V.; Bertman, S. B.; Pratt, K.; Shepson, P. B.

    2013-12-01

    During the summer, the southeastern United States experiences a cooling haze due to the interaction of anthropogenic and biogenic aerosol sources. An objective of the summer 2013 Southern Oxidant and Aerosol Study (SOAS) was to improve our understanding of how trace gases and aerosols are contributing to this relative cooling through light scattering and absorption. To improve understanding of biogenic-anthropogenic interactions through secondary organic aerosol (SOA) formation on primary aerosol cores requires detailed physicochemical characterization of the particles after uptake and processing. Our measurements focus on single particle analysis of aerosols in the accumulation mode (300-1000 nm) collected using a multi orifice uniform deposition impactor (MOUDI) at the Centreville, Alabama SEARCH site. Particles were characterized using an array of microscopic and spectroscopic techniques, including: scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray analysis (EDX), and Raman microspectroscopy. These analyses provide detailed information on particle size, morphology, elemental composition, and functional groups. This information is combined with mapping capabilities to explore individual particle spatial patterns and how that impacts structural characteristics. The improved understanding will be used to explore how sources and processing (such as SOA coating of soot) change particle structure (i.e. core shell) and how the altered optical properties impact air quality/climate effects on a regional scale.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  3. The effect of aerosol vertical profiles on satellite-estimated surface particle sulfate concentrations

    SciTech Connect

    Liu, Yang; Wang, Zifeng; Wang, Jun; Ferrare, Richard A.; Newsom, Rob K.; Welton, Ellsworth J.

    2011-02-15

    The aerosol vertical distribution is an important factor in determining the relationship between satellite retrieved aerosol optical depth (AOD) and ground-level fine particle pollution concentrations. We evaluate how aerosol profiles measured by ground-based lidar and simulated by models can help improve the association between AOD retrieved by the Multi-angle Imaging Spectroradiometer (MISR) and fine particle sulfate (SO4) concentrations using matched data at two lidar sites. At the Goddard Space Flight Center (GSFC) site, both lidar and model aerosol profiles marginally improve the association between SO4 concentrations and MISR fractional AODs, as the correlation coefficient between cross-validation (CV) and observed SO4 concentrations changes from 0.87 for the no-scaling model to 0.88 for models scaled with aerosol vertical profiles. At the GSFC site, a large amount of urban aerosols resides in the well-mixed boundary layer so the column fractional AODs are already excellent indicators of ground-level particle pollution. In contrast, at the Atmospheric Radiation Measurement Program (ARM) site with relatively low aerosol loadings, scaling substantially improves model performance. The correlation coefficient between CV and observed SO4 concentrations is increased from 0.58 for the no-scaling model to 0.76 in the GEOS-Chem scaling model, and the model bias is reduced from 17% to 9%. In summary, despite the inaccuracy due to the coarse horizontal resolution and the challenges of simulating turbulent mixing in the boundary layer, GEOS-Chem simulated aerosol profiles can still improve methods for estimating surface aerosol (SO4) mass from satellite-based AODs, particularly in rural areas where aerosols in the free troposphere and any long-range transport of aerosols can significantly contribute to the column AOD.

  4. Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi

    NASA Astrophysics Data System (ADS)

    Kumar, Sudhanshu

    2012-07-01

    {Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi } Tracing of aerosol sources is an important task helpful for making control strategy, and for climate change study. However, it is a difficult job as aerosols have several sources, involve in complex atmospheric processing, degradation and removal processes. Several approaches have been used for this task, e.g., models, which are based on the input of chemical species; stable- and radio-isotope compositions of certain species; chemical markers in which trace metals are the better options because they persist in atmosphere until the life of a particle. For example, K and Hg are used for biomass and coal burning tracings, respectively. Open waste burning has recently been believed to be a considerable source of aerosols in several mega cities in India and China. To better understand this source contribution in New Delhi aerosols, we have conducted aerosol sampling at a landfill site (Okhla), and in proximity (within 1 km distance) of this site. Aerosol filter samples were acid digested in microwave digestion system and analyzed using inductively coupled plasma -- high resolution mass spectrometry (ICP-HRMS) for getting metal signatures in particles. The metals, e.g., Sn, Sb and As those are found almost negligible in remote aerosols, are maximized in these waste burning aerosols. Sample collected in other location of New Delhi also shows the considerable presence of these metals in particles. Preliminary studies of isotopic ratios of these metals suggested that these metals, especially Sn can be used as marker for tracing the open waste burning sources of aerosols in New Delhi.

  5. 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.

  6. Metal and Silicate Particles Including Nanoparticles Are Present in Electronic Cigarette Cartomizer Fluid and Aerosol

    PubMed Central

    Williams, Monique; Villarreal, Amanda; Bozhilov, Krassimir; Lin, Sabrina; Talbot, Prue

    2013-01-01

    Background Electronic cigarettes (EC) deliver aerosol by heating fluid containing nicotine. Cartomizer EC combine the fluid chamber and heating element in a single unit. Because EC do not burn tobacco, they may be safer than conventional cigarettes. Their use is rapidly increasing worldwide with little prior testing of their aerosol. Objectives We tested the hypothesis that EC aerosol contains metals derived from various components in EC. Methods Cartomizer contents and aerosols were analyzed using light and electron microscopy, cytotoxicity testing, x-ray microanalysis, particle counting, and inductively coupled plasma optical emission spectrometry. Results The filament, a nickel-chromium wire, was coupled to a thicker copper wire coated with silver. The silver coating was sometimes missing. Four tin solder joints attached the wires to each other and coupled the copper/silver wire to the air tube and mouthpiece. All cartomizers had evidence of use before packaging (burn spots on the fibers and electrophoretic movement of fluid in the fibers). Fibers in two cartomizers had green deposits that contained copper. Centrifugation of the fibers produced large pellets containing tin. Tin particles and tin whiskers were identified in cartridge fluid and outer fibers. Cartomizer fluid with tin particles was cytotoxic in assays using human pulmonary fibroblasts. The aerosol contained particles >1 µm comprised of tin, silver, iron, nickel, aluminum, and silicate and nanoparticles (<100 nm) of tin, chromium and nickel. The concentrations of nine of eleven elements in EC aerosol were higher than or equal to the corresponding concentrations in conventional cigarette smoke. Many of the elements identified in EC aerosol are known to cause respiratory distress and disease. Conclusions The presence of metal and silicate particles in cartomizer aerosol demonstrates the need for improved quality control in EC design and manufacture and studies on how EC aerosol impacts the health of

  7. Size Resolved Measurements of Springtime Aerosol Particles over the Northern South China Sea

    NASA Technical Reports Server (NTRS)

    Atwood, Samuel A.; Reid, Jeffrey S.; Kreidenweis, Sonia M.; Cliff, Stephen S.; Zhao, Yongjing; Lin, Neng-Huei; Tsay, Si-Chee; Chu, Yu-Chi; Westphal, Douglas L.

    2012-01-01

    Large sources of aerosol particles and their precursors are ubiquitous in East Asia. Such sources are known to impact the South China Sea (henceforth SCS), a sometimes heavily polluted region that has been suggested as particularly vulnerable to climate change. To help elucidate springtime aerosol transport into the SCS, an intensive study was performed on the remote Dongsha (aka Pratas) Islands Atoll in spring 2010. As part of this deployment, a Davis Rotating-drum Uniform size-cut Monitor (DRUM) cascade impactor was deployed to collect size-resolved aerosol samples at the surface that were analyzed by X-ray fluorescence for concentrations of selected elements. HYSPLIT backtrajectories indicated that the transport of aerosol observed at the surface at Dongsha was occurring primarily from regions generally to the north and east. This observation was consistent with the apparent persistence of pollution and dust aerosol, along with sea salt, in the ground-based dataset. In contrast to the sea-level observations, modeled aerosol transport suggested that the westerly flow aloft (w700 hPa) transported smoke-laden air toward the site from regions from the south and west. Measured aerosol optical depth at the site was highest during time periods of modeled heavy smoke loadings aloft. These periods did not coincide with elevated aerosol concentrations at the surface, although the model suggested sporadic mixing of this free-tropospheric aerosol to the surface over the SCS. A biomass burning signature was not clearly identified in the surface aerosol composition data, consistent with this aerosol type remaining primarily aloft and not mixing strongly to the surface during the study. Significant vertical wind shear in the region also supports the idea that different source regions lead to varying aerosol impacts in different vertical layers, and suggests the potential for considerable vertical inhomogeneity in the SCS aerosol environment.

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

    SciTech Connect

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

    2014-09-01

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

  9. Single Particle Fluorescence & Mass Spectrometry for the Detection of Biological Aerosols

    SciTech Connect

    Coffee, K; Riot, V; Woods, B; Steele, P; Gard, E E

    2005-04-25

    Biological Aerosol Mass Spectrometry (BAMS) is an emerging technique for the detection of biological aerosols, which is being developed at Lawrence Livermore National Laboratory. The current system uses several orthogonal analytical methods to improve system selectivity, sensitivity and speed in order to maximize its utility as a biological aerosol detection system with extremely low probability of false alarm and high probability of detection. Our approach is to pre-select particles of interest by size and fluorescence prior to mass spectral analysis. The ability to distinguish biological aerosols from background and to discriminate bacterial spores, vegetative cells, viruses and toxins from one another will be shown. Data from particle standards of known chemical composition will be discussed. Analysis of ambient particles will also be presented.

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  11. Influenza virus aerosols in human exhaled breath: particle size, culturability, and effect of surgical masks.

    PubMed

    Milton, Donald K; Fabian, M Patricia; Cowling, Benjamin J; Grantham, Michael L; McDevitt, James J

    2013-03-01

    The CDC recommends that healthcare settings provide influenza patients with facemasks as a means of reducing transmission to staff and other patients, and a recent report suggested that surgical masks can capture influenza virus in large droplet spray. However, there is minimal data on influenza virus aerosol shedding, the infectiousness of exhaled aerosols, and none on the impact of facemasks on viral aerosol shedding from patients with seasonal influenza. We collected samples of exhaled particles (one with and one without a facemask) in two size fractions ("coarse">5 µm, "fine"≤5 µm) from 37 volunteers within 5 days of seasonal influenza onset, measured viral copy number using quantitative RT-PCR, and tested the fine-particle fraction for culturable virus. Fine particles contained 8.8 (95% CI 4.1 to 19) fold more viral copies than did coarse particles. Surgical masks reduced viral copy numbers in the fine fraction by 2.8 fold (95% CI 1.5 to 5.2) and in the coarse fraction by 25 fold (95% CI 3.5 to 180). Overall, masks produced a 3.4 fold (95% CI 1.8 to 6.3) reduction in viral aerosol shedding. Correlations between nasopharyngeal swab and the aerosol fraction copy numbers were weak (r = 0.17, coarse; r = 0.29, fine fraction). Copy numbers in exhaled breath declined rapidly with day after onset of illness. Two subjects with the highest copy numbers gave culture positive fine particle samples. Surgical masks worn by patients reduce aerosols shedding of virus. The abundance of viral copies in fine particle aerosols and evidence for their infectiousness suggests an important role in seasonal influenza transmission. Monitoring exhaled virus aerosols will be important for validation of experimental transmission studies in humans.

  12. Cloud condensation nuclei activity of isoprene secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Engelhart, Gabriella J.; Moore, Richard H.; Nenes, Athanasios; Pandis, Spyros N.

    2011-01-01

    This work explores the cloud condensation nuclei (CCN) activity of isoprene secondary organic aerosol (SOA), likely a significant source of global organic particulate matter and CCN, produced from the oxidation with OH from HONO/HOOH photolysis in a temperature-controlled SOA chamber. CCN concentrations, activation diameter, and droplet growth kinetic information were monitored as a function of supersaturation (from 0.3% to 1.5%) for several hours using a cylindrical continuous-flow streamwise thermal gradient CCN counter connected to a scanning mobility particle sizer. The initial SOA concentrations ranged from 2 to 30 μg m-3 and presented CCN activity similar to monoterpene SOA with an activation diameter of 35 nm for 1.5% supersaturation and 72 nm for 0.6% supersaturation. The CCN activity improved slightly in some experiments as the SOA aged chemically and did not depend significantly on the level of NOx during the SOA production. The measured activation diameters correspond to a hygroscopicity parameter κ value of 0.12, similar to κ values of 0.1 ± 0.04 reported for monoterpene SOA. Analysis of the water-soluble carbon extracted from filter samples of the SOA suggest that it has a κ of 0.2-0.3 implying an average molar mass between 90 and 150 g mol-1 (assuming a zero and 5% surface tension reduction with respect to water, respectively). These findings are consistent with known oxidation products of isoprene. Using threshold droplet growth analysis, the CCN activation kinetics of isoprene SOA was determined to be similar to pure ammonium sulfate aerosol.

  13. The chemical composition of fine ambient aerosol particles in the Beijing area

    NASA Astrophysics Data System (ADS)

    Nekat, Bettina; van Pinxteren, Dominik; Iinuma, Yoshiteru; Gnauk, Thomas; Müller, Konrad; Herrmann, Hartmut

    2010-05-01

    The strong economical growth in China during the last few decades led to heavy air pollution caused by significantly increased particle emissions. The aerosol particles affect not only the regional air quality and visibility, but can also influence cloud formation processes and the radiative balance of the atmosphere by their optical and microphysical properties. The ability to act as Cloud Condensation Nuclei (CCN) is related to microphysical properties like the hygroscopic growth or the cloud droplet activation. The chemical composition of CCN plays an important role on these properties and varies strongly with the particle size and the time of day. Hygroscopic or surface active substances can increase the hygroscopicity and lower the surface tension of the particle liquid phase, respectively. The presence of such compounds may result in faster cloud droplet activation by faster water uptake. The DFG project HaChi (Haze in China) aimed at studying physical and chemical parameters of urban aerosol particles in the Beijing area in order to associate the chemical composition of aerosol particles with their ability to act as CCN. To this end, two measurement campaigns were performed at the Wuqing National Ordinary Meteorological Observing Station, which is a background site near Beijing. The winter campaign was realized in March 2009 and the summer campaign took place from mid July 2009 to mid August 2009. Fine particles with an aerodynamic diameter smaller than or equal 1 μm were continuously sampled for 24h over the two campaigns using a DIGITEL high volume sampler (DHA-80). The present contribution presents and discusses the results of the chemical characterization of the DIGITEL filters samples. The filters were analyzed for the mass concentration, inorganic ions and carbon sum parameters like elemental (EC), organic (OC) and water soluble organic carbon (WSOC). The WSOC fraction was further characterized for hygroscopic substances like low molecular

  14. 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.

  15. Middle East measurements of concentration and size distribution of aerosol particles for coastal zones

    NASA Astrophysics Data System (ADS)

    Bendersky, Sergey; Kopeika, Norman S.; Blaunstein, Natan S.

    2005-10-01

    Recently, an extension of the Navy Aerosol Model (NAM) was proposed based on analysis of an extensive series of measurements at the Irish Atlantic Coast and at the French Mediterranean Coast. We confirm the relevance of that work for the distant eastern Meditteranean and extend several coefficients of that coastal model, proposed by Piazzola et al. for the Meditteranean Coast (a form of the Navy Aerosol Model), to midland Middle East coastal environments. This analysis is based on data collected at three different Middle East coastal areas: the Negev Desert (Eilat) Red Sea Coast, the Sea of Galilee (Tiberias) Coast, and the Mediterranean (Haifa) Coast. Aerosol size distributions are compared with those obtained through measurements carried out over the Atlantic, Pacific, and Indian Ocean Coasts, and Mediterranean, and Baltic Seas Coasts. An analysis of these different results allows better understanding of the similarities and differences between different coastal lake, sea, and open ocean zones. It is shown that in the coastal regions in Israel, compared to open ocean and other sea zones, larger differences in aerosol particle concentration are observed. The aerosol particle concentrations and their dependences on wind speed for these coastal zones are analyzed and discussed. We propose to classify the aerosol distribution models to either: 1. a coastal model with marine aerosol domination; 2. a coastal model with continental aerosol domination (referred to as midland coast in this work); or 3. a coastal model with balanced marine and continental conditions.

  16. Modeling of microphysics and optics of aerosol particles in the marine environments

    NASA Astrophysics Data System (ADS)

    Kaloshin, Gennady

    2013-05-01

    We present a microphysical model for the surface layer marine and coastal atmospheric aerosols that is based on long-term observations of size distributions for 0.01-100 μm particles. The fundamental feature of the model is a parameterization of amplitudes and widths for aerosol modes of the aerosol size distribution function (ASDF) as functions of fetch and wind speed. The shape of ASDF and its dependence on meteorological parameters, height above sea level (H), fetch (X), wind speed (U) and relative humidity (RH), are investigated. At present, the model covers the ranges H = 0 - 25 m, U = 3 - 18 km s-1, X ≤ 120 km and RH = 40 - 98%. The latest version of the Marine Aerosol Extinction Profiles model (MaexPro) is described and applied for the computation and analysis of the spectral profiles of aerosol extinction coefficients α(λ) in the wavelength band λ = 0.2-12 μm. MaexPro is based on the aforementioned aerosol model assuming spherically shaped aerosol particles and the well-known Mie theory. The spectral profiles of α(λ) calculated by MaexPro are in good agreement with observational data and the numerical results. Moreover, MaexPro was found to be an accurate and reliable tool for investigating the optical properties of atmospheric aerosols.

  17. Organic films on atmospheric aerosol particles, fog droplets, cloud droplets, raindrops, and snowflakes

    NASA Astrophysics Data System (ADS)

    Gill, P. S.; Graedel, T. E.; Weschler, C. J.

    1983-05-01

    If surface-active organic molecules are present as surface films, the transfer of gases into the atmospheric water system could be impeded, evaporation could be slowed, and the aqueous chemical reactions could be influenced. The results of new measurements of the surface tension of aqueous solutions of common atmospheric organic compounds (beta-pinene, n-hexanol, eugenol, and anethole) are reported, and it is shown that the compounds produce films with properties similar to those of the better known surfactants. It is concluded that organic films are probably common on atmospheric aerosol particles and that they may occur under certain circumstances on fog droplets, cloud droplets, and snowflakes. If they are present, they will increase the lifetimes of aerosol particles, fog droplets, and cloud droplets, both by inhibiting water vapor evaporation and by reducing the efficiency with which these atmospheric components are scavenged. It is thought likely that the transport of gaseous molecules into and out of the aqueous solution will be impeded by factors of several hundred or more when organic films are present.

  18. Photocatalytic atrazine degradation by synthetic minerals, atmospheric aerosols, and soil particles.

    PubMed

    Lackhoff, Marion; Niessner, Reinhard

    2002-12-15

    In this work, the photocatalytic atrazine degradation by seven synthetic minerals and five environmental particle samples was examined to investigate a possible contribution of photocatalysis to the abiotic degradation of atrazine in the environment. Particle suspensions containing 500 ng/L atrazine were irradiated with a sun simulator, and the atrazine degradation was monitored by enzyme-linked immunosorbent assay (ELISA). Atrazine detection by ELISA proved to be an useful analytical tool because of low cross-reactivity of atrazine metabolites and high sensitivity with detection limits in the lower nanograms per liter range. The atrazine degradation followed first-order kinetics, and the obtained rate coefficients were compared with the rate of direct photolysis. Known photocatalysts, such as TiO2 and ZnO, showed the expected fast photocatalytic degradation (k = 27-327 x 10(-3) min(-1)) of atrazine. The degradation rates detected upon irradiation of titanium-, zinc-, or iron-containing minerals were orders of magnitudes lower (k = 0.15-0.70 x 10(-3) min(-1)) but still significantly faster than direct photolysis without particles (k = 0.10 x 10(-3) min(-1)). With environmental particle samples (soot, fly ash, sand, road dust, and volcanic ash), however, no significant photocatalytic activity was observed (k = 0.07-0.16 x 10(-3) min(-1)). The atrazine degradation rates were in the range of direct photolysis. Thus photocatalysis by aerosol or soil particles appears not to enhance abiotic atrazine degradation in the environment.

  19. Protection of firefighters against combustion aerosol particles: simulated workplace protection factor of a half-mask respirator (pilot study).

    PubMed

    Dietrich, James; Yermakov, Michael; Reponen, Tiina; Kulkarni, Pramod; Qi, Chaolong; Grinshpun, Sergey A

    2015-01-01

    The present pilot study investigated the penetration of ultrafine particles originated by combustion of different materials into elastomeric half-mask respirators equipped with two P100 filters. We determined the Simulated Workplace Protection Factor (SWPF) for 11 firefighters wearing elastomeric half-mask respirators and performing activities simulating those conducted during fire overhaul operations. The tests were performed in a controlled laboratory setting. A newly-developed battery-operated Portable Aerosol Mobility Spectrometer (PAMS) was used to measure size-resolved aerosol particle concentrations outside (C(out)) and inside (Cin) of an air-purifying respirator donned on a firefighter, and the SWPF was calculated as C(out)/C(in). Based on the total aerosol concentration, the "total" SWPF ranged from 4,222 (minimum) to 35,534 (maximum) with values falling primarily in a range from 11,171 (25 percentile) to 26,604 (75 percentile) and a median value being ≈15,000. This is consistent with the recently reported fit factor (FF) data base.((1)) The size-resolved SWPF data revealed a dependency on the particle size. It was concluded that a portable device such as PAMS can be used on firefighters during overhaul operations (as well as on other workers wearing elastomeric half-mask respirators) to monitor the aerosol concentrations in real time and ultimately help prevent overexposure. PMID:25625543

  20. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds

    NASA Astrophysics Data System (ADS)

    Rudich, Yinon; Adler, Gabriela; Koop, Thomas; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven; Haspel, Carynelisa

    2014-05-01

    In cold high altitude cirrus clouds and anvils of high convective clouds in the tropics and mid-latitudes, ice partciles that are exposed to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. In this talk we will describe experiements that simulate the atmospheric freeze-drying cycle of aerosols. We find that aerosols with high organic content can form highly porous particles (HPA) with a larger diameter and a lower density than the initial homogenous aerosol following ice subliation. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure follwoing ice sublimation. We find that the highly porous aerosol scatter solar light less efficiently than non-porous aerosol particles. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

  1. Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Wang, Junfeng; Ge, Xinlei; Chen, Yanfang; Shen, Yafei; Zhang, Qi; Sun, Yele; Xu, Jianzhong; Ge, Shun; Yu, Huan; Chen, Mindong

    2016-07-01

    In this work, the Aerodyne soot particle - aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m-3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ˜ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (< 100 nm vacuum aerodynamic diameter) were dominated by organics and rBC, while large particles had significant contributions from secondary inorganic species. Source apportionment of organic aerosols (OA) yielded four OA subcomponents, including hydrocarbon-like OA (HOA), cooking-related OA (COA), semi-volatile oxygenated OA (SV-OOA), and low-volatility oxygenated OA (LV-OOA). Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA) dominated the total OA mass (55.5 %), but primary organic aerosol (POA, equal to the sum of HOA and COA) can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species

  2. A method for the direct measurement of surface tension of collected atmospherically relevant aerosol particles using atomic force microscopy

    NASA Astrophysics Data System (ADS)

    Hritz, Andrew D.; Raymond, Timothy M.; Dutcher, Dabrina D.

    2016-08-01

    Accurate estimates of particle surface tension are required for models concerning atmospheric aerosol nucleation and activation. However, it is difficult to collect the volumes of atmospheric aerosol required by typical instruments that measure surface tension, such as goniometers or Wilhelmy plates. In this work, a method that measures, ex situ, the surface tension of collected liquid nanoparticles using atomic force microscopy is presented. A film of particles is collected via impaction and is probed using nanoneedle tips with the atomic force microscope. This micro-Wilhelmy method allows for direct measurements of the surface tension of small amounts of sample. This method was verified using liquids, whose surface tensions were known. Particles of ozone oxidized α-pinene, a well-characterized system, were then produced, collected, and analyzed using this method to demonstrate its applicability for liquid aerosol samples. It was determined that oxidized α-pinene particles formed in dry conditions have a surface tension similar to that of pure α-pinene, and oxidized α-pinene particles formed in more humid conditions have a surface tension that is significantly higher.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  4. Size, composition, and mixing state of individual aerosol particles in a South China coastal city.

    PubMed

    Li, Weijun; Shao, Longyi; Wang, Zhishi; Shen, Rongrong; Yang, Shusheng; Tang, Uwa

    2010-01-01

    Aerosol samples were collected in summer in Macao, a coastal city of the Pearl River Delta Region in China. Morphology, size, elemental composition, and mixing state of individual aerosol particles were determined by scanning electron microscopy coupled energy dispersive X-ray (SEM/EDX) and transmission electron microscopy (TEM). Based on the morphologies of 5711 aerosol particles, they consist of soot (32%), mineral (17%), secondary (22%), and unknown fine particles (29%). The sizes of these particles were mostly distributed between 0.1 and 0.4 microm. Compositions of 202 mineral particles were obtained by SEM/EDX. Mineral particles were mainly classified into three types: Si-rich, Ca-rich, and Na-rich. The compositions of typical mineral particles can indicate their sources in sampling location. For example, mineral particles, collected along the main street, were associated with trace amounts of heavy metals, such as Zn, Ti, Mn, Ba, Pb, and As. TEM observations indicate that most Na-rich particles were aged sea salt particles (e.g., Na2SO4 and NaNO3) which formed through heterogeneous chemical reactions between sea salt and acidic gases. Additionally, aging time of soot was short in Macao due to high humidity, high temperature, and high levels of sunlight in Macao. Most of soot and fine mineral dust particles were internally mixed with secondary particles.

  5. Activity size distribution and residence time of 7Be aerosols in the Arctic atmosphere

    NASA Astrophysics Data System (ADS)

    Ioannidou, Alexandra; Paatero, Jussi

    2014-05-01

    The activity size distributions of the natural radionuclide tracer 7Be in different size range fractions (<0.39 μm, 0.39-0.69 μm, 0.69-1.3 μm, 1.3-2.1 μm, 2.1-4.2 μm, 4.2-10.2 μm and >10.2 μm) were determined in the boreal atmosphere in the Arctic Research Centre of the Finnish Meteorological Institute (FMI) at Sodankylä, Finland (67°22‧ N, 26°38‧ E, 180 m asl). The activity median aerodynamic diameter (AMAD) ranged from 0.54 μm to 1.05 μm (average 0.83 μm). A residence time of about 8 days applies to aerosols of 0.83 μm diameter, representing the residence of aerosol particles in arctic environment. The observed positive correlation between AMAD values and RH% can be explained by the fact that condensation during high relative humidity conditions becomes more intense, resulting in increased particle sizes of atmospheric aerosols. However, greater aerosol particle sizes means higher wet scavenging rate of aerosols and as a result lower activity concentration of 7Be in the atmosphere, explaining the anti-correlation between the AMAD values and activity concentrations of 7Be. But this associated with possibly higher scavenging rates of aerosols does not necessarily alone explain the anti-correlation between the AMAD and the 7Be activities. The air mass origin associated with synoptic scale weather phenomena may contribute to that too. The Flextra model was used to assess the transport pattern and to explain the deviation in radionuclide activity concentrations and AMAD values observed in the site of investigation.

  6. Wide-range particle characterization and elemental concentration in Beijing aerosol during the 2013 Spring Festival.

    PubMed

    Jing, Hui; Li, Yu-Feng; Zhao, Jiating; Li, Bai; Sun, Jialong; Chen, Rui; Gao, Yuxi; Chen, Chunying

    2014-09-01

    The number and mass concentration, size distribution, and the concentration of 16 elements were studied in aerosol samples during the Spring Festival celebrations in 2013 in Beijing, China. Both the number and mass concentration increased sharply in a wide range from 10 nm to 10 μm during the firecrackers and fireworks activities. The prominent increase of the number concentration was in 50 nm-500 nm with a peak of 1.7 × 10(5)/cm(3) at 150 nm, which is 8 times higher than that after 1.5 h. The highest mass concentration was in 320-560 nm, which is 4 times higher than the control. K, Mg, Sr, Ba and Pb increased sharply during the firework activities in PM10. Although the aerosol emission from firework activities is a short-term air quality degradation event, there may be a substantial hazard arising from the chemical composition of the emitted particles. PMID:24975025

  7. Wide-range particle characterization and elemental concentration in Beijing aerosol during the 2013 Spring Festival.

    PubMed

    Jing, Hui; Li, Yu-Feng; Zhao, Jiating; Li, Bai; Sun, Jialong; Chen, Rui; Gao, Yuxi; Chen, Chunying

    2014-09-01

    The number and mass concentration, size distribution, and the concentration of 16 elements were studied in aerosol samples during the Spring Festival celebrations in 2013 in Beijing, China. Both the number and mass concentration increased sharply in a wide range from 10 nm to 10 μm during the firecrackers and fireworks activities. The prominent increase of the number concentration was in 50 nm-500 nm with a peak of 1.7 × 10(5)/cm(3) at 150 nm, which is 8 times higher than that after 1.5 h. The highest mass concentration was in 320-560 nm, which is 4 times higher than the control. K, Mg, Sr, Ba and Pb increased sharply during the firework activities in PM10. Although the aerosol emission from firework activities is a short-term air quality degradation event, there may be a substantial hazard arising from the chemical composition of the emitted particles.

  8. Formation characteristics of aerosol particles from pulverized coal pyrolysis in high-temperature environments

    SciTech Connect

    Wei-Hsin Chen; Shan-Wen Du; Hsi-Hsien Yang; Jheng-Syun Wu

    2008-05-15

    The formation characteristics of aerosol particles from pulverized coal pyrolysis in high temperatures are studied experimentally. By conducting a drop-tube furnace, fuel pyrolysis processes in industrial furnaces are simulated in which three different reaction temperatures of 1000, 1200, and 1400{sup o}C are considered. Experimental observations indicate that when the reaction temperature is 1000{sup o}C, submicron particles are produced, whereas the particle size is dominated by nanoscale for the temperature of 1400{sup o}C. Thermogravimetric analysis of the aerosol particles stemming from the pyrolysis temperature of 1000{sup o}C reveals that the thermal behavior of the aerosol is characterized by a three-stage reaction with increasing heating temperature: (1) a volatile-reaction stage, (2) a weak-reaction stage, and (3) a soot-reaction stage. However, with the pyrolysis temperature of 1400{sup o}C, the volatile- and weak-reaction stages almost merge together and evolve into a chemical-frozen stage. The submicron particles (i.e., 1000{sup o}C) are mainly composed of volatiles, tar, and soot, with the main component of the nanoscale particles (i.e., 1400{sup o}C) being soot. The polycyclic aromatic hydrocarbons (PAHs) contained in the aerosols are also analyzed. It is found that the PAH content in generated aerosols decreases dramatically as the pyrolysis temperature increases. 31 refs., 9 figs., 1 tab.

  9. Fluorescence properties of biochemicals in dry NaCl composite aerosol particles and in solutions

    NASA Astrophysics Data System (ADS)

    Putkiranta, M.; Manninen, A.; Rostedt, A.; Saarela, J.; Sorvajärvi, T.; Marjamäki, M.; Hernberg, R.; Keskinen, J.

    2010-06-01

    Several fluorophores, such as tryptophan, NADH, NADPH, and riboflavin are found in airborne micro-organisms. In this work, the fluorescence properties of these biochemicals were studied both in dry NaCl composite aerosol particles and in saline solutions by means of laser-induced fluorescence. Fluorescence spectra were measured from individual, airborne aerosol particles and from solutions in cuvette. The excitation wavelength was varied in steps from 210 nm to 419 nm and the fluorescence was detected within a wavelength band of 310-670 nm. For each sample, the measured fluorescence emission spectra were combined into fluorescence maps. The fluorescence maximum of riboflavin in a dry NaCl composite particle is 20 nm red-shifted compared with the solution, whereas the maxima are blue-shifted by about 25 nm for tryptophan and 15 nm for NADH and NADPH. The molecular fluorescence cross sections have significant differences between the aerosol particles and the solutions, except for tryptophan. For NADH and NADPH the cross sections are over 20 times larger in the aerosol particles than in the solutions probably as a result of partial quenching of fluorescence in solution caused by the collision or stacking with the adenine moiety. The fluorescence cross section of riboflavin is almost 60 times larger in the solution than in the dry NaCl composite aerosol. This is probably caused by the different microenvironment around the fluorophore molecule and by the concentration quenching in the particles where the fluorescing molecules are relatively close to each other.

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

    NASA Astrophysics Data System (ADS)

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

    2012-08-01

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

  11. Characterization of a Quadrotor Unmanned Aircraft System for Aerosol-Particle-Concentration Measurements.

    PubMed

    Brady, James M; Stokes, M Dale; Bonnardel, Jim; Bertram, Timothy H

    2016-02-01

    High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking. PMID:26730457

  12. Characterization of a Quadrotor Unmanned Aircraft System for Aerosol-Particle-Concentration Measurements.

    PubMed

    Brady, James M; Stokes, M Dale; Bonnardel, Jim; Bertram, Timothy H

    2016-02-01

    High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking.

  13. Particle resuspension via human activity

    NASA Astrophysics Data System (ADS)

    Qian, Jing

    This dissertation consists of three correlated parts that are related to particle resuspension from floorings in indoor environment. The term resuspension in this dissertation refers the re-entrainment of deposited particles into atmosphere via mechanic disturbances by human activity indoors, except where it is specified. The first part reviews the literature related to particle resuspension. Fundamental concepts and kinetics of resuspension of particles were extracted from previous studies. Suggestions for future research on indoor particle resuspension have been given based on the literature reviews and the findings of part 2 and part 3. The second part involved 54 resuspension experiments conducted in a room-scale environmental chamber. Three floorings types and two ventilation configurations were tested. Air exchange rate were fixed during the experiments, and the temperature/RH were monitored. The airborne particle concentration was measured by an array of optical particle counters (OPCs) in the chamber. Resuspension rates were estimated in size ranges of 0.8--1, 1.0--2.0, 2.0--5.0, and 5.0--10 mum ranging from 10-5--10 -2 hr-1, with higher resuspension rates associated with larger particles. Resuspension via walking activity varied from experiment to experiment. A "heavy and fast" walking style was associated with a higher resuspension rate than a less active style. Given the same floor loading of the test particles, resuspension rates for the carpeted floor were on the same order of magnitude but significantly higher than those for the hard floor. In the third part, an image analysis method (IAM) was adapted to characterize the particle distribution on fabric floorings. The IAM results showed the variability of particles loading on various carpets. The dust particles on fibers from ten carpets vary in sizes. The normal dust loading varies from house to house from 3.6x106 particles/cm2 to 8.2x106 particles/cm2. The dust particle number distribution for size

  14. Physical properties, chemical composition, sources, spatial distribution and sinks of indoor aerosol particles in a university lecture hall

    NASA Astrophysics Data System (ADS)

    Salma, I.; Dosztály, K.; Borsós, T.; Söveges, B.; Weidinger, T.; Kristóf, G.; Péter, N.; Kertész, Zs.

    2013-01-01

    PM10 mass, particle number (N) and CO2 concentrations, particle number size distributions and meteorological parameters were determined with high time resolution, and daily aerosol samples were collected in the PM10-2.0 and PM2.0 size fractions for chemical analysis in the middle of a university lecture hall for one week. Median concentrations for the PM10 mass and N of 15.3 μg m-3 and 3.7 × 103 cm-3, respectively were derived. The data are substantially smaller than the related outdoor levels or typical values for residences. There were considerable concentration differences for workdays, weekends and various lectures. Main sources of PM10 mass include the usage of chalk sticks for writing, wiping the blackboard, ordinary movements and actions of students and cleaning. High PM10 mass concentration levels up to 100 μg m-3 were realised for short time intervals after wiping the blackboard. The mass concentrations decreased rapidly after the emission source ceased to be active. Two classes of coarse particles were identified. General indoor dust particles exhibited a residence time of approximately 35 min, while the residence time for the chalk dust particles was approximately 20 min as lower estimates. Emission source rate for wiping the blackboard was estimated to be between 8 and 14 mg min-1. This represents a substantial emission rate but the source is active only up to 1 min. Suspension of the chalk (made mainly of gypsum) dust particles was confirmed by enrichment of Ca and S in the hall with respect to ambient urban aerosol. Contribution of ambient aerosol via the heating, ventilation and air conditioning (HVAC) facility was considerable for time intervals when the indoor sources of PM10 mass were not intensive. The HVAC facility introduces, however, the major amount of aerosol particles from the outdoors as far as their number concentration is regarded. Mean contribution of ultrafine particles to the total particle number was (69 ± 7)%, which is smaller

  15. Particle-Resolved Modeling of Aerosol Mixing State in an Evolving Ship Plume

    NASA Astrophysics Data System (ADS)

    Riemer, N. S.; Tian, J.; Pfaffenberger, L.; Schlager, H.; Petzold, A.

    2011-12-01

    The aerosol mixing state is important since it impacts the particles' optical and CCN properties and thereby their climate impact. It evolves continuously during the particles' residence time in the atmosphere as a result of coagulation with other particles and condensation of secondary aerosol species. This evolution is challenging to represent in traditional aerosol models since they require the representation of a multi-dimensional particle distribution. While modal or sectional aerosol representations cannot practically resolve the aerosol mixing state for more than a few species, particle-resolved models store the composition of many individual aerosol particles directly. They thus sample the high-dimensional composition state space very efficiently and so can deal with tens of species, fully resolving the mixing state. Here we use the capabilities of the particle-resolved model PartMC-MOSAIC to simulate the evolution of particulate matter emitted from marine diesel engines and compare the results to aircraft measurements made in the English Channel in 2007 as part of the European campaign QUANTIFY. The model was initialized with values of gas concentrations and particle size distributions and compositions representing fresh ship emissions. These values were obtained from a test rig study in the European project HERCULES in 2006 using a serial four-stroke marine diesel engine operating on high-sulfur heavy fuel oil. The freshly emitted particles consisted of sulfate, black carbon, organic carbon and ash. We then tracked the particle population for several hours as it evolved undergoing coagulation, dilution with the background air, and chemical transformations in the aerosol and gas phase. This simulation was used to compute the evolution of CCN properties and optical properties of the plume on a per-particle basis. We compared our results to size-resolved data of aged ship plumes from the QUANTIFY Study in 2007 and showed that the model was able to reproduce

  16. Investigation of Aerosol Surface Area Estimation from Number and Mass Concentration Measurements: Particle Density Effect

    PubMed Central

    Ku, Bon Ki; Evans, Douglas E.

    2015-01-01

    For nanoparticles with nonspherical morphologies, e.g., open agglomerates or fibrous particles, it is expected that the actual density of agglomerates may be significantly different from the bulk material density. It is further expected that using the material density may upset the relationship between surface area and mass when a method for estimating aerosol surface area from number and mass concentrations (referred to as “Maynard’s estimation method”) is used. Therefore, it is necessary to quantitatively investigate how much the Maynard’s estimation method depends on particle morphology and density. In this study, aerosol surface area estimated from number and mass concentration measurements was evaluated and compared with values from two reference methods: a method proposed by Lall and Friedlander for agglomerates and a mobility based method for compact nonspherical particles using well-defined polydisperse aerosols with known particle densities. Polydisperse silver aerosol particles were generated by an aerosol generation facility. Generated aerosols had a range of morphologies, count median diameters (CMD) between 25 and 50 nm, and geometric standard deviations (GSD) between 1.5 and 1.8. The surface area estimates from number and mass concentration measurements correlated well with the two reference values when gravimetric mass was used. The aerosol surface area estimates from the Maynard’s estimation method were comparable to the reference method for all particle morphologies within the surface area ratios of 3.31 and 0.19 for assumed GSDs 1.5 and 1.8, respectively, when the bulk material density of silver was used. The difference between the Maynard’s estimation method and surface area measured by the reference method for fractal-like agglomerates decreased from 79% to 23% when the measured effective particle density was used, while the difference for nearly spherical particles decreased from 30% to 24%. The results indicate that the use of

  17. Mapping of soot particles in a weakly sooting diffusion flame by aerosol techniques

    SciTech Connect

    Hepp, H.; Siegmann, K.

    1998-10-01

    The evolution of detailed particle size distributions has been measured along the centerline of an axisymmetric diffusion flame of CH{sub 4} + Ar burning in air at 1 atm. Soot particles with mean diameters of 3--18 nm were observed. Changes in the size distribution exhibited zones where either nucleation, coagulation, or destruction of soot particles dominated. These highly sensitive measurements were made by microprobe sampling with an immediate dilution of 1:400, to quench the aerosol, and by subsequent application of aerosol measurement techniques. In parallel, the yield of photoemitted electrons from size-selected particles was determined. The yield shows a characteristic dependence on location in the flame, indicating changes of the particle`s surface. Multiphoton, time-of-flight mass spectrometry was used to investigate the correlation between polycyclic aromatic hydrocarbons in the flame and enhanced photoemission yield from the soot particles.

  18. Experimental Assessment of Collection Efficiency of Submicron Aerosol Particles by Cloud Droplets

    NASA Astrophysics Data System (ADS)

    Huang, Y. W.; Ardon-Dryer, K.; Cziczo, D. J.

    2014-12-01

    The interplay between aerosol particles and water droplets in the atmosphere, especially in clouds, influences both aerosol and cloud properties. The major uncertainty in our understanding of climate arises in the indirect effect of aerosol and their ability to impact cloud formation and consequently alter the global radiative balance. The collision between a water droplet and aerosol particles that results in coalescence is termed "collection" or "coagulation". Coagulation can lead to aerosol removal from the atmosphere or induce ice nucleation via contact freezing. There is a theoretical collection efficiency minimum of particles with diameter between 0.1-2 µm, called the "Greenfield Gap". Experimental effort, however, was limited to drizzle and rain drops until recently, and has not constrained parameters that describe particle collection efficiency by cloud droplets. Collection efficiency is also an important parameter for assessing contact freezing, the least known ice nucleation mechanism today. Experimentally assessing collection efficiency can prove the existence of the "Greenfield Gap" and lay the foundation for studying contact freezing. We recently constructed the MIT-Contact Freezing Chamber (MIT-CFC) to study coagulation experimentally. A stream of 40 µm cloud droplets fall freely into the chamber and collide with aerosol particles with known size and concentration. The outflow goes through a series of dryers before entering the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument for chemical composition analysis. PALMS is a true single-particle instrument and gives information on the size and the chemical composition of each particle. Coagulated particles from the MIT-CFC have mass spectral signatures of both the aerosol particles and the droplet residuals, while the droplet residual contains no signature of the aerosol particles. To our knowledge, this is the first time coagulation has been seen on a single-particle basis. We will

  19. HUMIDITY EFFECTS ON THE MASS SPECTRA OF SINGLE AEROSOL PARTICLES. (R823980)

    EPA Science Inventory

    On-line laser desorption ionization mass spectrometry has developed into a widely used method for chemical characterization of individual aerosol particles. In the present study, the spectra of laboratory-generated particles were obtained as a function of relative humidity to elu...

  20. 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

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

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Volkamer, R.

    2010-09-01

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

  2. Discrimination and classification of bio-aerosol particles using optical spectroscopy and scattering

    NASA Astrophysics Data System (ADS)

    Eversole, Jay D.

    2011-03-01

    For more than a decade now, there has been significant emphasis for development of sensors of agent aerosols, especially for biological warfare (BW) agents. During this period, the Naval Research Laboratory (NRL) and other labs have explored the application of optical and spectroscopic methods relevant to biological composition discrimination to aerosol particle characterization. I will first briefly attempt to establish the connection between sensor performance metrics which are statistically determined, and aerosol particle measurements through the use of computational models, and also describe the challenge of ambient background characterization that would be needed to establish more reliable and deterministic sensor performance predictions. Greater attention will then be devoted to a discussion of basic particle properties and their measurement. The NRL effort has adopted an approach based on direct measurements on individual particles, principally of elastic scatter and laser-induced fluorescence (LIF), rather than populations of particles. The development of a LIF instrument using two sequential excitation wavelengths to detect fluorescence in discrete spectral bands will be described. Using this instrument, spectral characteristics of particles from a variety of biological materials including BW agent surrogates, as well as other ``calibration'' particles and some known ambient air constituents will be discussed in terms of the dependence of optical signatures on aerosol particle composition, size and incident laser fluence. Comparison of scattering and emission measurements from particles composed of widely different taxa, as well as from similar species under different growth conditions highlight the difficulties of establishing ground truth for complex biological material compositions. One aspect that is anticipated to provide greater insight to this type of particle classification capability is the development of a fundamental computational model of

  3. High-efficiency particulate air filter test stand and aerosol generator for particle loading studies.

    PubMed

    Arunkumar, R; Hogancamp, Kristina U; Parsons, Michael S; Rogers, Donna M; Norton, Olin P; Nagel, Brian A; Alderman, Steven L; Waggoner, Charles A

    2007-08-01

    This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30 x 30 x 29 cm(3) nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5 to 12 standard m(3)/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150 degrees C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7 standard m(3)/min, high mass concentrations (approximately 25 mg/m(3)) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160 nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions.

  4. High-efficiency particulate air filter test stand and aerosol generator for particle loading studies.

    PubMed

    Arunkumar, R; Hogancamp, Kristina U; Parsons, Michael S; Rogers, Donna M; Norton, Olin P; Nagel, Brian A; Alderman, Steven L; Waggoner, Charles A

    2007-08-01

    This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30 x 30 x 29 cm(3) nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5 to 12 standard m(3)/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150 degrees C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7 standard m(3)/min, high mass concentrations (approximately 25 mg/m(3)) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160 nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions. PMID

  5. High-efficiency particulate air filter test stand and aerosol generator for particle loading studies

    NASA Astrophysics Data System (ADS)

    Arunkumar, R.; Hogancamp, Kristina U.; Parsons, Michael S.; Rogers, Donna M.; Norton, Olin P.; Nagel, Brian A.; Alderman, Steven L.; Waggoner, Charles A.

    2007-08-01

    This manuscript describes the design, characterization, and operational range of a test stand and high-output aerosol generator developed to evaluate the performance of 30×30×29cm3 nuclear grade high-efficiency particulate air (HEPA) filters under variable, highly controlled conditions. The test stand system is operable at volumetric flow rates ranging from 1.5to12standardm3/min. Relative humidity levels are controllable from 5%-90% and the temperature of the aerosol stream is variable from ambient to 150°C. Test aerosols are produced through spray drying source material solutions that are introduced into a heated stainless steel evaporation chamber through an air-atomizing nozzle. Regulation of the particle size distribution of the aerosol challenge is achieved by varying source solution concentrations and through the use of a postgeneration cyclone. The aerosol generation system is unique in that it facilitates the testing of standard HEPA filters at and beyond rated media velocities by consistently providing, into a nominal flow of 7standardm3/min, high mass concentrations (˜25mg/m3) of dry aerosol streams having count mean diameters centered near the most penetrating particle size for HEPA filters (120-160nm). Aerosol streams that have been generated and characterized include those derived from various concentrations of KCl, NaCl, and sucrose solutions. Additionally, a water insoluble aerosol stream in which the solid component is predominantly iron (III) has been produced. Multiple ports are available on the test stand for making simultaneous aerosol measurements upstream and downstream of the test filter. Types of filter performance related studies that can be performed using this test stand system include filter lifetime studies, filtering efficiency testing, media velocity testing, evaluations under high mass loading and high humidity conditions, and determination of the downstream particle size distributions.

  6. Laboratory measurements of the angular light-scattering properties of internally mixed organic and sea-salt aerosol particles using polar nephelometry

    NASA Astrophysics Data System (ADS)

    Curtis, D. B.; Tinilau, S. S.

    2013-12-01

    Aerosol particles play an important, but relatively poorly understood, role in Earth's climate. Sea-salt aerosol is one of the most prevalent naturally occurring aerosols and is therefore expected to have a large effect on climate by scattering incoming solar radiation back to space. While sea-salt aerosol has been thought to be mainly composed of sodium chloride and other salts, measurements have shown the presence of biogenic organic compounds, such as glucose, in primary sea-salt aerosol particles. In addition, the sea-salt aerosol particles can become coated by secondary organics from anthropogenic activities. In order to better understand the potential climate effects of internally mixed organic and sea-salt particles, the angular scattering properties of laboratory-generated aerosols were measured at a wavelength of 532 nm using polar nephelometry. The polar nephelometer collected scattered light with an elliptical mirror and focused it across a linear CCD detector. The instrument was therefore capable of measuring the scattering intensity as a function of scattering angle (the phase function). Two incident polarizations were studied, parallel and perpendicular to the scattering plane, which were then used to calculate the degree of linear polarization. The scattering measurements along with size distribution measurements were used to retrieve the refractive index of the particles by comparison with Mie theory. Particles were generated from solutions of sodium chloride with varying concentrations of organics such as glucose and oxalic acid. In addition, particles generated from authentic sea-water were studied for comparison. Preliminary results indicate that the effective refractive indices of the mixed particles differ significantly from pure sodium chloride and do not follow simple mixing rules used to calculate refractive index from individual components.

  7. 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.

  8. LOAC (Light Optical Particle Counter): a new small aerosol counter with particle characterization capabilities for surface and airborne measurements

    NASA Astrophysics Data System (ADS)

    Renard, Jean-Baptiste; Berthet, Gwenael; Jégou, Fabrice; Jeannot, Matthieu; Jourdain, Line; Dulac, François; Mallet, Marc; Dupont, Jean-Charles; Thaury, Claire; Tonnelier, Thierry; Verdier, Nicolas; Charpentier, Patrick

    2013-04-01

    The determination of the size distribution of tropospheric and stratospheric aerosols with conventional optical counters is difficult when different natures of particles are present (droplets, soot, mineral dust, secondary organic or mineral particles...). Also, a light and cheap aerosol counter that can be used at ground, onboard drones or launched under all kinds of atmospheric balloons can be very useful during specific events as volcanic plumes, desert dust transport or local pollution episodes. These goals can be achieved thanks to a new generation of aerosol counter, called LOAC (Light Optical Aerosol Counter). The instrument was developed in the frame of a cooperation between French scientific laboratories (CNRS), the Environnement-SA and MeteoModem companies and the French Space Agency (CNES). LOAC is a small optical particle counter/sizer of ~250 grams, having a low electrical power consumption. The measurements are conducted at two scattering angles. The first one, at 12°, is used to determine the aerosol particle concentrations in 19 size classes within a diameter range of 0.3-100 micrometerers. At such an angle close to forward scattering, the signal is much more intense and the measurements are the least sensitive to the particle nature. The second angle is at 60°, where the scattered light is strongly dependent on the particle refractive index and thus on the nature of the aerosols. The ratio of the measurements at the two angles is used to discriminate between the different types of particles dominating the nature of the aerosol particles in the different size classes. The sensor particularly discriminates wet or liquid particles, soil dust and soot. Since 2011, we have operated LOAC in various environments (Arctic, Mediterranean, urban and peri-urban…) under different kinds of balloons including zero pressure stratospheric, tethered, drifting tropospheric, and meteorological sounding balloons. For the last case, the total weight of the gondola

  9. The scavenging of two different types of marine aerosol particles calculated using a two-dimensional detailed cloud model

    NASA Astrophysics Data System (ADS)

    Flossmann, Andrea I.

    1991-07-01

    Our 2-D dynamic model including spectral microphysics and scavenging has been evaluated for a warm precipitating convective cloud at Day 261 (18 September 1974) of the GATE campaign. Two different chemical species ((NH4)2SO4 and NaCl) of aerosol particles were followed in the air, inside the drops in the cloud, and inside the drops reaching the ground. Concerning the dynamics and microphysics, as well as the scavenging and wet deposition, the model results agree quite well with available observations. The cloud rained after 19min of cloud life time. For the considered aerosol loading of the atmosphere, rough estimates are derived for the total material processed by such a warm convective cloud as input for larger scale models. In particular, the following conclusions could be drawn for the situation considered. (1) If a drop spectrum forms on an aerosol spectrum where the small particles consist of (NH4)2SO4 and the large ones of NaCl, the resulting small drops also mainly consist of (NH4)2SO4 and the larger drops of NaCl. Collision and coalescence causes a redistribution of the chemical species such that the precipitation sized drops consist of NaCl to about 70%. (2) The mixing ratio of aerosol material in the drops is a function of the age of the drops and their history and therefore the variation of the mixing ratio with drop size depends on the entrainment and evoluion of the relative humidity. The mixing ratio decreased with increasing drop radius at almost all grid points due to continuous activation of fresh particles. (3) Assuming that the sulfate aerosol would not consist of (NH4)2SO4 particles but instead consist of NH4 HSO4 particles the acidic cloud water has a pH of 4.7 which agrees with observations of marine precipitation. (4) The scavenging efficiency of the cloud considered is closely related to its precipitation efficiency (both near 40%). About 90% of the total amount of aerosol material scavenged is incorporated into the cloud water through

  10. Sea spray aerosol as a unique source of ice nucleating particles

    NASA Astrophysics Data System (ADS)

    DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.; Prather, Kimberly A.; Collins, Douglas B.; Sullivan, Ryan C.; Ruppel, Matthew J.; Mason, Ryan H.; Irish, Victoria E.; Lee, Taehyoung; Hwang, Chung Yeon; Siek Rhee, Tae; Snider, Jefferson R.; McMeeking, Gavin R.; Dhaniyala, Suresh; Lewis, Ernie R.; Wentzell, Jeremy J. B.; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M.; Ault, Andrew P.; Axson, Jessica L.; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M. Dale; Deane, Grant B.; Mayol-Bracero, Olga L.; Grassian, Vicki H.; Bertram, Timothy H.; Bertram, Allan K.; Moffett, Bruce F.; Franc, Gary D.

    2016-05-01

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.

  11. Sea spray aerosol as a unique source of ice nucleating particles.

    PubMed

    DeMott, Paul J; Hill, Thomas C J; McCluskey, Christina S; Prather, Kimberly A; Collins, Douglas B; Sullivan, Ryan C; Ruppel, Matthew J; Mason, Ryan H; Irish, Victoria E; Lee, Taehyoung; Hwang, Chung Yeon; Rhee, Tae Siek; Snider, Jefferson R; McMeeking, Gavin R; Dhaniyala, Suresh; Lewis, Ernie R; Wentzell, Jeremy J B; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M; Ault, Andrew P; Axson, Jessica L; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M Dale; Deane, Grant B; Mayol-Bracero, Olga L; Grassian, Vicki H; Bertram, Timothy H; Bertram, Allan K; Moffett, Bruce F; Franc, Gary D

    2016-05-24

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean. PMID:26699469

  12. Sea spray aerosol as a unique source of ice nucleating particles

    PubMed Central

    DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.; Prather, Kimberly A.; Ruppel, Matthew J.; Mason, Ryan H.; Irish, Victoria E.; Lee, Taehyoung; Hwang, Chung Yeon; Snider, Jefferson R.; McMeeking, Gavin R.; Dhaniyala, Suresh; Lewis, Ernie R.; Wentzell, Jeremy J. B.; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M.; Ault, Andrew P.; Axson, Jessica L.; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M. Dale; Deane, Grant B.; Mayol-Bracero, Olga L.; Grassian, Vicki H.; Bertram, Timothy H.; Bertram, Allan K.; Moffett, Bruce F.; Franc, Gary D.

    2016-01-01

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using “dry” geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean. PMID:26699469

  13. Sea spray aerosol as a unique source of ice nucleating particles.

    PubMed

    DeMott, Paul J; Hill, Thomas C J; McCluskey, Christina S; Prather, Kimberly A; Collins, Douglas B; Sullivan, Ryan C; Ruppel, Matthew J; Mason, Ryan H; Irish, Victoria E; Lee, Taehyoung; Hwang, Chung Yeon; Rhee, Tae Siek; Snider, Jefferson R; McMeeking, Gavin R; Dhaniyala, Suresh; Lewis, Ernie R; Wentzell, Jeremy J B; Abbatt, Jonathan; Lee, Christopher; Sultana, Camille M; Ault, Andrew P; Axson, Jessica L; Diaz Martinez, Myrelis; Venero, Ingrid; Santos-Figueroa, Gilmarie; Stokes, M Dale; Deane, Grant B; Mayol-Bracero, Olga L; Grassian, Vicki H; Bertram, Timothy H; Bertram, Allan K; Moffett, Bruce F; Franc, Gary D

    2016-05-24

    Ice nucleating particles (INPs) are vital for ice initiation in, and precipitation from, mixed-phase clouds. A source of INPs from oceans within sea spray aerosol (SSA) emissions has been suggested in previous studies but remained unconfirmed. Here, we show that INPs are emitted using real wave breaking in a laboratory flume to produce SSA. The number concentrations of INPs from laboratory-generated SSA, when normalized to typical total aerosol number concentrations in the marine boundary layer, agree well with measurements from diverse regions over the oceans. Data in the present study are also in accord with previously published INP measurements made over remote ocean regions. INP number concentrations active within liquid water droplets increase exponentially in number with a decrease in temperature below 0 °C, averaging an order of magnitude increase per 5 °C interval. The plausibility of a strong increase in SSA INP emissions in association with phytoplankton blooms is also shown in laboratory simulations. Nevertheless, INP number concentrations, or active site densities approximated using "dry" geometric SSA surface areas, are a few orders of magnitude lower than corresponding concentrations or site densities in the surface boundary layer over continental regions. These findings have important implications for cloud radiative forcing and precipitation within low-level and midlevel marine clouds unaffected by continental INP sources, such as may occur over the Southern Ocean.

  14. Stratospheric aerosol particle size information in Odin-OSIRIS limb scatter spectra

    NASA Astrophysics Data System (ADS)

    Rieger, L. A.; Bourassa, A. E.; Degenstein, D. A.

    2014-02-01

    The Optical Spectrograph and InfraRed Imaging System (OSIRIS) onboard the Odin satellite has now taken over a decade of limb scatter measurements that have been used to retrieve the version 5 stratospheric aerosol extinction product. This product is retrieved using a representative particle size distribution to calculate scattering cross sections and scattering phase functions for the forward model calculations. In this work the information content of OSIRIS measurements with respect to stratospheric aerosol is systematically examined for the purpose of retrieving particle size information along with the extinction coefficient. The benefit of using measurements at different wavelengths and scattering angles in the retrieval is studied, and it is found that incorporation of the 1530 nm radiance measurement is key for a robust retrieval of particle size information. It is also found that using OSIRIS measurements at the different solar geometries available on the Odin orbit simultaneously provides little additional benefit. Based on these results, an improved aerosol retrieval algorithm is developed that couples the retrieval of aerosol extinction and mode radius of a log-normal particle size distribution. Comparison of these results with coincident measurements from SAGE III shows agreement in retrieved extinction to within approximately 10% over the bulk of the aerosol layer, which is comparable to version 5. The retrieved particle size, when converted to Ångström coefficient, shows good qualitative agreement with SAGE II measurements made at somewhat shorter wavelengths.

  15. [Concentration and Particle Size Distribution of Microbiological Aerosol During Haze Days in Beijing].

    PubMed

    Hu, Ling-fei; Zhang, Ke; Wang, Hong-bao; Li, Na; Wang, Jie; Yang, Wen-hui; Yin, Zhe; Jiao, Zhou-guang; Wen, Zhan-bo; Li, Jin-song

    2015-09-01

    In this study, we evaluated the bacterial, fungal aerosol concentration, and particle size distribution using microbiological aerosol sampler, and analyzed the particles count concentration of PM1.0, PM2.5, PM5.0 and PM10.0 using aerodynamic particle sizer during clear and haze days in Beijing during Jan 8th, 2013 to Feb 4th, 2013. The concentration of bacterial, fungal aerosol, air particulate matter and aerosol distribution were compared between haze days and clear days. Our results indicated that the proportion of fungal particles smaller than 5 micron, which could deposit in lungs or deeper regions, was much higher than bacterial particles. The biological concentration of bacteria and fungi were higher in clear days than in haze days, and there was no statistic difference of the microbiological aerosol distribution. The concentration of air particulate matter were higher in haze days than in clear days, PM10 was the main particulate matters both in clear days and haze days.

  16. Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

    NASA Astrophysics Data System (ADS)

    Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

    During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

  17. Chemometric analysis of multi-sensor hyperspectral images of coarse mode aerosol particles for the image-based investigation on aerosol particles

    NASA Astrophysics Data System (ADS)

    Ofner, Johannes; Kamilli, Katharina A.; Eitenberger, Elisabeth; Friedbacher, Gernot; Lendl, Bernhard; Held, Andreas; Lohninger, Hans

    2015-04-01

    Multi-sensor hyperspectral imaging is a novel technique, which allows the determination of composition, chemical structure and pure components of laterally resolved samples by chemometric analysis of different hyperspectral datasets. These hyperspectral datasets are obtained by different imaging methods, analysing the same sample spot and superimposing the hyperspectral data to create a single multi-sensor dataset. Within this study, scanning electron microscopy (SEM), Raman and energy-dispersive X-ray spectroscopy (EDX) images were obtained from size-segregated aerosol particles, sampled above Western Australian salt lakes. The particles were collected on aluminum foils inside a 2350 L Teflon chamber using a Sioutas impactor, sampling aerosol particles of sizes between 250 nm and 10 µm. The complex composition of the coarse-mode particles can be linked to primary emissions of inorganic species as well as to oxidized volatile organic carbon (VOC) emissions. The oxidation products of VOC emissions are supposed to form an ultra-fine nucleation mode, which was observed during several field campaigns between 2006 and 2013. The aluminum foils were analysed using chemical imaging and electron microscopy. A Horiba LabRam 800HR Raman microscope was used for vibrational mapping of an area of about 100 µm x 100 µm of the foils at a resolution of about 1 µm. The same area was analysed using a Quanta FEI 200 electron microscope (about 250 nm resolution). In addition to the high-resolution image, the elemental composition could be investigated using energy-dispersive X-ray spectroscopy. The obtained hyperspectral images were combined into a multi-sensor dataset using the software package Imagelab (Epina Software Labs, www.imagelab.at). After pre-processing of the images, the multi-sensor hyperspectral dataset was analysed using several chemometric methods such as principal component analysis (PCA), hierarchical cluster analysis (HCA) and other multivariate methods. Vertex

  18. Two-dimensional Guinier analysis: application to single aerosol particles in-flight.

    PubMed

    Berg, Matthew J; Hill, Steve C; Pan, Yong-Le; Videen, Gorden

    2010-10-25

    This work presents an apparatus that measures near-forward two-dimensional elastic scattering patterns of single aerosol particles and proposes a two-angle extension of the Guinier law to analyze these patterns. The particles, which approximately range from 2 to 8 micrometers in size, flow through the apparatus in an aerosol stream. A spatial filtering technique separates the near-forward portion of the patterns from the illumination light. Contours intended to represent the geometrical profile of the particles are generated from the patterns using the extension of the Guinier law. The analysis is applied to spherical and nonspherical particles, and the resulting contours are found to be consistent with particle shape only for spherical particles.

  19. Retrievals of Aerosol and Cloud Particle Microphysics Using Polarization and Depolarization Techniques

    NASA Technical Reports Server (NTRS)

    Mishchenko, Michael; Hansen, James E. (Technical Monitor)

    2001-01-01

    The recent availability of theoretical techniques for computing single and multiple scattering of light by realistic polydispersions of spherical and nonspherical particles and the strong dependence of the Stokes scattering matrix on particle size, shape, and refractive index make polarization and depolarization measurements a powerful particle characterization tool. In this presentation I will describe recent applications of photopolarimetric and lidar depolarization measurements to remote sensing characterization of tropospheric aerosols, polar stratospheric clouds (PSCs), and contrails. The talk will include (1) a short theoretical overview of the effects of particle microphysics on particle single-scattering characteristics; (2) the use of multi-angle multi-spectral photopolarimetry to retrieve the optical thickness, size distribution, refractive index, and number concentration of tropospheric aerosols over the ocean surface; and (3) the application of the T-matrix method to constraining the PSC and contrail particle microphysics using multi-spectral measurements of lidar backscatter and depolarization.

  20. Progress Towards Identifying and Quantifying the Organic Ice Nucleating Particles in Soils and Aerosols

    NASA Astrophysics Data System (ADS)

    Hill, T. C. J.; DeMott, P. J.; Fröhlich-Nowoisky, J.; Tobo, Y.; Suski, K. J.; Levin, E. J.; Kreidenweis, S. M.; Franc, G. D.

    2014-12-01

    Soil and plant surfaces emit ice nucleating particles (INP) to the atmosphere, especially when disturbed by wind, harvesting, rain or fire. Organic (biogenic) INP are abundant in most soils and dominate the population that nucleate >-15°C. For example, the sandy topsoil of sagebrush shrubland, a widespread ecotype prone to wind erosion after fire, contains ~106 organic INP g-1 at -6°C. The relevance of organic INP may also extend to colder temperatures than previously thought: Particles of soil organic matter (SOM) have been shown to be more important than mineral particles for the ice nucleating ability of agricultural soil dusts to -34°C. While the abundance of ice nucleation active (INA) bacteria on plants has been established, the identity of the organic INP in and emitted by soils remains a 40-year-old mystery. The need to understand their production and release is highlighted by recent findings that INA bacteria (measured with qPCR) account for few, if any, of the warm-temperature organic INP that predominate in boundary layer aerosols and snow; organic INP lofted with soil dusts seem a likely source. The complexity of SOM hinders its investigation. It contains decomposing plant materials, a diverse microbial and microfaunal community, humus, and inert organic matter. All are biochemically complex and all may contain ice nucleating constituents, either by design or by chance. Indeed the smoothness of the INP temperature spectra of soils is indicative of numerous, overlapping distributions of INP. We report recent progress in identifying and quantifying the organic INP in soils and boundary layer aerosols representative of West Central U.S. ecosystems, and how their characteristics may affect their dispersal. Chemical, enzymatic and DNA-based tests were used to assess contributions of INP from plant tissues, INA bacteria, INA fungi, organic crystals, monolayers of aliphatic alcohols, carbohydrates, and humic substances, while heat- and peroxide-based tests

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

    SciTech Connect

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

    2015-09-25

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

  2. On the growth of nitric and sulfuric acid aerosol particles under stratospheric conditions

    NASA Technical Reports Server (NTRS)

    Hamill, Patrick; Turco, R. P.; Toon, O. B.

    1988-01-01

    A theory for the formation of frozen aerosol particles in the Antarctic stratosphere was developed and applied to the formation of polar stratospheric clouds. The theory suggests that the condensed ice particles are composed primarily of nitric acid and water, with small admixtures of sulfuric and hydrochloric acids in solid solution. The proposed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinction observed in the winter polar stratosphere.

  3. Impact of new particle formation on the concentrations of aerosol number and cloud condensation nuclei around Beijing

    SciTech Connect

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Takegawa, Nobuyuki; Wiedensohler, A.; Fast, Jerome D.; Zaveri, Rahul A.

    2011-10-13

    New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosol number (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduced a new aerosol model representation with 20 size bins between 1 nm and 10 {mu}m and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the CARE-Beijing 2006 campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurements (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20-30% of CN concentrations (> 10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of pre-existing particles through the competition of condensable gases between new particles and pre-existing particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.

  4. Spontaneous Aerosol Ejection: Origin of Inorganic Particles in Biomass Pyrolysis.

    PubMed

    Teixeira, Andrew R; Gantt, Rachel; Joseph, Kristeen E; Maduskar, Saurabh; Paulsen, Alex D; Krumm, Christoph; Zhu, Cheng; Dauenhauer, Paul J

    2016-06-01

    At high thermal flux and temperatures of approximately 500 °C, lignocellulosic biomass transforms to a reactive liquid intermediate before evaporating to condensable bio-oil for downstream upgrading to renewable fuels and chemicals. However, the existence of a fraction of nonvolatile compounds in condensed bio-oil diminishes the product quality and, in the case of inorganic materials, catalyzes undesirable aging reactions within bio-oil. In this study, ablative pyrolysis of crystalline cellulose was evaluated, with and without doped calcium, for the generation of inorganic-transporting aerosols by reactive boiling ejection from liquid intermediate cellulose. Aerosols were characterized by laser diffraction light scattering, inductively coupled plasma spectroscopy, and high-speed photography. Pyrolysis product fractionation revealed that approximately 3 % of the initial feed (both organic and inorganic) was transported to the gas phase as aerosols. Large bubble-to-aerosol size ratios and visualization of significant late-time ejections in the pyrolyzing cellulose suggest the formation of film bubbles in addition to the previously discovered jet formation mechanism.

  5. Microfluidic Electrochemical Sensor for On-line Monitoring of Aerosol Oxidative Activity

    PubMed Central

    Sameenoi, Yupaporn; Koehler, Kirsten; Shapiro, Jeff; Boonsong, Kanokporn; Sun, Yele; Collett, Jeffrey; Volckens, John; Henry, Charles S.

    2012-01-01

    Particulate matter (PM) air pollution has a significant impact on human morbidity and mortality; however, the mechanisms of PM-induced toxicity are poorly defined. A leading hypothesis states that airborne PM induces harm by generating reactive oxygen species (ROS) in and around human tissues, leading to oxidative stress. We report here, a system employing a microfluidic electrochemical sensor coupled directly to a Particle-into-Liquid-Sampler (PILS) system to measure aerosol oxidative activity in an on-line format. The oxidative activity measurement is based on the dithiothreitol assay (DTT assay) where after oxidized by PM, the remaining reduced DTT was analyzed by the microfluidic sensor. The sensor consists of an array of working, reference, and auxiliary electrodes fabricated in a poly(dimethylsiloxane) (PDMS)-based microfluidic device. Cobalt (II) phthalocyanine (CoPC)-modified carbon paste was used as the working electrode material allowing selective detection of reduced DTT. The electrochemical sensor was validated off-line against the traditional DTT assay using filter samples taken from urban environments and biomass burning events. After off-line characterization, the sensor was coupled to a PILS to enable on-line sampling/analysis of aerosol oxidative activity. Urban dust and industrial incinerator ash samples were aerosolized in an aerosol chamber and analyzed for their oxidative activity. The on-line sensor reported DTT consumption rates (oxidative activity) in good correlation with aerosol concentration (R2 from 0.86–.97) with a time-resolution of approximately 3 minutes. PMID:22651886

  6. Light scattering and absorption properties of aerosol particles in the urban environment of Granada, Spain

    NASA Astrophysics Data System (ADS)

    Lyamani, H.; Olmo, F. J.; Alados-Arboledas, L.

    Surface measurements of optical and physical aerosol properties were made at an urban site, Granada (Spain) (37.18°N, 3.58°W, 680 m a.s.l), during winter 2005-2006. Measurements included the aerosol scattering, σsca, and backscattering coefficients, σbsca, at three wavelengths (450, 550 and 700 nm) measured at low relative humidity (RH<50%) by an integrating nephelometer, the absorption coefficient at 670 nm, σabs, measured with a multi-angle absorption photometer, and aerosol size distribution in the 0.5-20 μm aerodynamic diameter range registered by an aerodynamic aerosol sizer (APS-3321, TSI). The hourly average of σsca (550 nm) ranged from 2 to 424 M m -1 with an average value of 84±62 M m -1 (±S.D.). The Angstrom exponent presented an average value of 1.8±0.3, suggesting a large fraction of fine particles at the site, an observation confirmed by aerosol size distribution measurements. The hourly average of σabs (670 nm) ranged from 1.7 to 120.5 M m -1 with an average value of 28±20 M m -1. The results indicate that the aerosol absorption coefficient in Granada was relatively large. The largest σsca value was associated with air masses that passed over heavily polluted European areas and local stagnation conditions. High absorbing aerosol level was obtained during dust transport from North Africa probably due to the presence of hematite. Based on the measured scattering and absorption coefficients, a very low average value of the single scattering albedo of 0.66±0.11 at 670 nm was calculated, suggesting that urban aerosols in this region contain a large fraction of absorbing material. A clear diurnal pattern was observed in scattering and absorption coefficients and particle concentrations with two local maxima occurring in early morning and late evening. This behavior can be explained in terms of local conditions that control the particle sources associated with traffic and upward mixing of the aerosol during the daytime development of a

  7. Mass Analysis of Charged Aerosol Particles During the MASS/ECOMA Campaign

    NASA Astrophysics Data System (ADS)

    Knappmiller, S.; Robertson, S.; Horanyi, M.; Sternovsky, Z.

    2008-12-01

    . The Mesospheric Aerosol Sampling Spectrometer (MASS) instrument was launched on two sounding rockets in August 2007 from Andoya, Norway to find the masses of charged aerosol particles in the polar mesosphere in NLC/PMSE conditions (3 August) and PMSE conditions alone (6 August). We compare and contrast the four data sets from the uplegs and downlegs. The MASS instrument collected ions, cluster ions, and charged nanometer-sized particles on four pairs of electrically-biased graphite plates that collect positive and negative particles separately. Electron collection was prevented by the negative potential on the rocket body. For the 3 August upleg, the data show charged particle collection on all channels with number densities of order several thousand per cubic centimeter in the four size ranges < 0.5 nm, 0.5-1 nm, 1-2 nm, and > 3 nm. The occurrence of positively charged aerosol particles in the smallest sizes suggests positive ions as the nucleation sites because the smallest particles have negligible probability of charging by photoionization. The signals were smaller on the 3 August downleg as a consequence of the spatial variability of the cloud. For the 6 August upleg into PMSE alone, only smaller particles (< 2 nm) were detected and these were both positive and negative with number densities of several thousand per cubic centimeter. On the downleg, 1-2 nm negatively charged particles were detected, but there were no positive particles in this mass range.

  8. Thermal desorption single particle mass spectrometry of ambient aerosol in Shanghai

    NASA Astrophysics Data System (ADS)

    Zhai, Jinghao; Wang, Xinning; Li, Jingyan; Xu, Tingting; Chen, Hong; Yang, Xin; Chen, Jianmin

    2015-12-01

    Submicron aerosol volatility, chemical composition, and mixing state were simultaneously measured using a thermodenuder (TD) in-line with a single particle aerosol mass spectrometry (SPAMS) during Nov.12 to Dec. 11 of 2014 in Shanghai. By heating up to 250 °C, the signals of refractory species such as elemental carbon, metallic compounds, and mineral dust in aerosols were enhanced in the mass spectra. At 250 °C, the main particle types present in the size range of 0.2-1.0 μm were biomass burning (37% by number) and elemental carbon (20%). From 1.0 to 2.0 μm, biomass burning (30%), dust (19%) and metal-rich (18%) were the primary particle types. CN- signal remained in the mass spectra of the heated biomass burning particles suggests the existence of some extremely low-volatility nitrogen-containing organics. Laboratory experiments were conducted by burning rice straws, the main source material of biomass burning particles in Southern China, to confirm the less volatile composition contributed by biomass burning. Strong CN- with relative area >0.21 was observed in most of the laboratory-made biomass burning particles when heated above 200 °C and was selected as a new marker to identify the biomass burning particles in the field. The TD-SPAMS measured the size-resolved chemical composition of the individual particle residues at different temperatures and offered more information on the aging processes of primary particles and their sources.

  9. Individual aerosol particles in ambient and updraft conditions below convective cloud bases in the Oman mountain region

    NASA Astrophysics Data System (ADS)

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

    2014-03-01

    An airborne study of cloud microphysics provided an opportunity to collect aerosol particles in ambient and updraft conditions of natural convection systems for transmission electron microscopy (TEM). Particles were collected simultaneously on lacey carbon and calcium-coated carbon (Ca-C) TEM grids, providing information on particle morphology and chemistry and a unique record of the particle's physical state on impact. In total, 22 particle categories were identified, including single, coated, aggregate, and droplet types. The fine fraction comprised up to 90% mixed cation sulfate (MCS) droplets, while the coarse fraction comprised up to 80% mineral-containing aggregates. Insoluble (dry), partially soluble (wet), and fully soluble particles (droplets) were recorded on Ca-C grids. Dry particles were typically silicate grains; wet particles were mineral aggregates with chloride, nitrate, or sulfate components; and droplets were mainly aqueous NaCl and MCS. Higher numbers of droplets were present in updrafts (80% relative humidity (RH)) compared with ambient conditions (60% RH), and almost all particles activated at cloud base (100% RH). Greatest changes in size and shape were observed in NaCl-containing aggregates (>0.3 µm diameter) along updraft trajectories. Their abundance was associated with high numbers of cloud condensation nuclei (CCN) and cloud droplets, as well as large droplet sizes in updrafts. Thus, compositional dependence was observed in activation behavior recorded for coarse and fine fractions. Soluble salts from local pollution and natural sources clearly affected aerosol-cloud interactions, enhancing the spectrum of particles forming CCN and by forming giant CCN from aggregates, thus, making cloud seeding with hygroscopic flares ineffective in this region.

  10. Aerosol and Cloud-Nucleating Particle Observations during an Atmospheric River Event

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; McCluskey, C. S.; Petters, M.; Suski, K. J.; Levin, E. J.; Hill, T. C. J.; Atwood, S. A.; Schill, G. P.; Rocci, K.; Boose, Y.; Martin, A.; Cornwell, G.; Al-Mashat, H.; Moore, K.; Prather, K. A.; Rothfuss, N.; Taylor, H.; Leung, L. R.; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Rosenfeld, D.; Spackman, J. R.; Fairall, C. W.; Creamean, J.; White, A. B.; Kreidenweis, S. M.

    2015-12-01

    The multi-agency CalWater 2015 project occurred over North Central CA and the Eastern Pacific during January to March 2015 (Spackman et al., this session). The goals of the campaign were to document the structure of atmospheric rivers (ARs) that deliver much of the water vapor associated with major winter storms along the U.S. West Coast and to investigate the modulating effect of aerosols on precipitation. Aerosol sources that may influence orographic cloud properties for air lifted over the mountains in California in winter include pollution, biomass burning, soil dusts and marine aerosols, but their roles will also be influenced by transport, vertical stratification, and scavenging processes. We present results from a comprehensive study of aerosol distributions, compositions, and cloud nucleating properties during an intense winter storm during February 2015, including data from an NSF-supported measurement site at Bodega Bay, from the DOE-ARM Cloud Aerosol Precipitation Experiment that included sampling on the NOAA RV Ron Brown offshore and the G-1 aircraft over ocean and land, and with context provided by other NOAA aircraft and remote sensing facilities. With a special focus on the coastal site, we discuss changes in aerosol distributions, aerosol hygroscopicity, and number concentrations of fluorescent particles, cloud condensation nuclei (CCN), and ice nucleating particles (INPs) during the AR event. We compare with periods preceding and following the event. For example, total aerosol number and surface area concentrations at below 0.5 μm diameter decreased from typical values of a few thousand cm-3 and 100 μm2 cm-3, respectively, to a few hundred cm-3 and 10 μm2cm-3 at Bodega Bay during the AR event. CCN concentrations were similarly lower, but hygroscopicity parameter (kappa) increased from typical values of 0.2 to values > 0.5 during the AR.INP and fluorescent particle number concentrations were generally lower during the AR event than at any other

  11. 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

  12. Aerosol number size distributions over a coastal semi urban location: Seasonal changes and ultrafine particle bursts.

    PubMed

    Babu, S Suresh; Kompalli, Sobhan Kumar; Moorthy, K Krishna

    2016-09-01

    Number-size distribution is one of the important microphysical properties of atmospheric aerosols that influence aerosol life cycle, aerosol-radiation interaction as well as aerosol-cloud interactions. Making use of one-yearlong measurements of aerosol particle number-size distributions (PNSD) over a broad size spectrum (~15-15,000nm) from a tropical coastal semi-urban location-Trivandrum (Thiruvananthapuram), the size characteristics, their seasonality and response to mesoscale and synoptic scale meteorology are examined. While the accumulation mode contributed mostly to the annual mean concentration, ultrafine particles (having diameter <100nm) contributed as much as 45% to the total concentration, and thus constitute a strong reservoir, that would add to the larger particles through size transformation. The size distributions were, in general, bimodal with well-defined modes in the accumulation and coarse regimes, with mode diameters lying in the range 141 to 167nm and 1150 to 1760nm respectively, in different seasons. Despite the contribution of the coarse sized particles to the total number concentration being meager, they contributed significantly to the surface area and volume, especially during transport of marine air mass highlighting the role of synoptic air mass changes. Significant diurnal variation occurred in the number concentrations, geometric mean diameters, which is mostly attributed to the dynamics of the local coastal atmospheric boundary layer and the effect of mesoscale land/sea breeze circulation. Bursts of ultrafine particles (UFP) occurred quite frequently, apparently during periods of land-sea breeze transitions, caused by the strong mixing of precursor-rich urban air mass with the cleaner marine air mass; the resulting turbulence along with boundary layer dynamics aiding the nucleation. These ex-situ particles were observed at the surface due to the transport associated with boundary layer dynamics. The particle growth rates from

  13. Aerosol number size distributions over a coastal semi urban location: Seasonal changes and ultrafine particle bursts.

    PubMed

    Babu, S Suresh; Kompalli, Sobhan Kumar; Moorthy, K Krishna

    2016-09-01

    Number-size distribution is one of the important microphysical properties of atmospheric aerosols that influence aerosol life cycle, aerosol-radiation interaction as well as aerosol-cloud interactions. Making use of one-yearlong measurements of aerosol particle number-size distributions (PNSD) over a broad size spectrum (~15-15,000nm) from a tropical coastal semi-urban location-Trivandrum (Thiruvananthapuram), the size characteristics, their seasonality and response to mesoscale and synoptic scale meteorology are examined. While the accumulation mode contributed mostly to the annual mean concentration, ultrafine particles (having diameter <100nm) contributed as much as 45% to the total concentration, and thus constitute a strong reservoir, that would add to the larger particles through size transformation. The size distributions were, in general, bimodal with well-defined modes in the accumulation and coarse regimes, with mode diameters lying in the range 141 to 167nm and 1150 to 1760nm respectively, in different seasons. Despite the contribution of the coarse sized particles to the total number concentration being meager, they contributed significantly to the surface area and volume, especially during transport of marine air mass highlighting the role of synoptic air mass changes. Significant diurnal variation occurred in the number concentrations, geometric mean diameters, which is mostly attributed to the dynamics of the local coastal atmospheric boundary layer and the effect of mesoscale land/sea breeze circulation. Bursts of ultrafine particles (UFP) occurred quite frequently, apparently during periods of land-sea breeze transitions, caused by the strong mixing of precursor-rich urban air mass with the cleaner marine air mass; the resulting turbulence along with boundary layer dynamics aiding the nucleation. These ex-situ particles were observed at the surface due to the transport associated with boundary layer dynamics. The particle growth rates from

  14. Individual Aerosol Particles from Biomass Burning in Southern Africa. 1; Compositions and Size Distributions of Carbonaceous Particles

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

    Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

  15. Penetration of Combustion Aerosol Particles Through Filters of NIOSH-Certified Filtering Facepiece Respirators (FFRs).

    PubMed

    Gao, Shuang; Kim, Jinyong; Yermakov, Michael; Elmashae, Yousef; He, Xinjian; Reponen, Tiina; Grinshpun, Sergey A

    2015-01-01

    Filtering facepiece respirators (FFRs) are commonly worn by first responders, first receivers, and other exposed groups to protect against exposure to airborne particles, including those originated by combustion. Most of these FFRs are NIOSH-certified (e.g., N95-type) based on the performance testing of their filters against charge-equilibrated aerosol challenges, e.g., NaCl. However, it has not been examined if the filtration data obtained with the NaCl-challenged FFR filters adequately represent the protection against real aerosol hazards such as combustion particles. A filter sample of N95 FFR mounted on a specially designed holder was challenged with NaCl particles and three combustion aerosols generated in a test chamber by burning wood, paper, and plastic. The concentrations upstream (Cup) and downstream (Cdown) of the filter were measured with a TSI P-Trak condensation particle counter and a Grimm Nanocheck particle spectrometer. Penetration was determined as (Cdown/Cup) ×100%. Four test conditions were chosen to represent inhalation flows of 15, 30, 55, and 85 L/min. Results showed that the penetration values of combustion particles were significantly higher than those of the "model" NaCl particles (p < 0.05), raising a concern about applicability of the N95 filters performance obtained with the NaCl aerosol challenge to protection against combustion particles. Aerosol type, inhalation flow rate and particle size were significant (p < 0.05) factors affecting the performance of the N95 FFR filter. In contrast to N95 filters, the penetration of combustion particles through R95 and P95 FFR filters (were tested in addition to N95) were not significantly higher than that obtained with NaCl particles. The findings were attributed to several effects, including the degradation of an N95 filter due to hydrophobic organic components generated into the air by combustion. Their interaction with fibers is anticipated to be similar to those involving "oily" particles

  16. Penetration of Combustion Aerosol Particles Through Filters of NIOSH-Certified Filtering Facepiece Respirators (FFRs).

    PubMed

    Gao, Shuang; Kim, Jinyong; Yermakov, Michael; Elmashae, Yousef; He, Xinjian; Reponen, Tiina; Grinshpun, Sergey A

    2015-01-01

    Filtering facepiece respirators (FFRs) are commonly worn by first responders, first receivers, and other exposed groups to protect against exposure to airborne particles, including those originated by combustion. Most of these FFRs are NIOSH-certified (e.g., N95-type) based on the performance testing of their filters against charge-equilibrated aerosol challenges, e.g., NaCl. However, it has not been examined if the filtration data obtained with the NaCl-challenged FFR filters adequately represent the protection against real aerosol hazards such as combustion particles. A filter sample of N95 FFR mounted on a specially designed holder was challenged with NaCl particles and three combustion aerosols generated in a test chamber by burning wood, paper, and plastic. The concentrations upstream (Cup) and downstream (Cdown) of the filter were measured with a TSI P-Trak condensation particle counter and a Grimm Nanocheck particle spectrometer. Penetration was determined as (Cdown/Cup) ×100%. Four test conditions were chosen to represent inhalation flows of 15, 30, 55, and 85 L/min. Results showed that the penetration values of combustion particles were significantly higher than those of the "model" NaCl particles (p < 0.05), raising a concern about applicability of the N95 filters performance obtained with the NaCl aerosol challenge to protection against combustion particles. Aerosol type, inhalation flow rate and particle size were significant (p < 0.05) factors affecting the performance of the N95 FFR filter. In contrast to N95 filters, the penetration of combustion particles through R95 and P95 FFR filters (were tested in addition to N95) were not significantly higher than that obtained with NaCl particles. The findings were attributed to several effects, including the degradation of an N95 filter due to hydrophobic organic components generated into the air by combustion. Their interaction with fibers is anticipated to be similar to those involving "oily" particles

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

    SciTech Connect

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

    2014-08-11

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

  18. Heavy duty diesel engine exhaust aerosol particle and ion measurements.

    PubMed

    Lähde, Tero; Rönkkö, Topi; Virtanen, Annele; Schuck, Tanja J; Pirjola, Liisa; Hämeri, Kaarle; Kulmala, Markku; Arnold, Frank; Rothe, Dieter; Keskinen, Jorma

    2009-01-01

    Heavy duty EURO 4 diesel engine exhaust particle and ion size distributions were measured atthetailpipe using dynamometer testing. Measurements of particle volatility and electrical charge were undertaken to clarify diesel exhaust nucleation mode characteristics with different exhaust after-treatment systems. Nucleation mode particle volatility and charging probability were dependent on exhaust after-treatment particles were volatile and uncharged when the engine was equipped with diesel particulate filter and partly volatile and partly charged in exhaust without any after-treatment or with an oxidation catalyst only. The absence of charged particles in the nucleation mode of diesel particulate filtered exhaust excludes the ion mediated process as a nucleation particle formation mechanism.

  19. CCN activation of pure and coated carbon black particles.

    PubMed

    Dusek, U; Reischl, G P; Hitzenberger, R

    2006-02-15

    The CCN (cloud condensation nucleus) activation of pure and coated carbon black particles was investigated using the University of Vienna cloud condensation nuclei counter (Giebl, H.; Berner, A.; Reischl, G.; Puxbaum, H.; Kasper-Giebl, A.; Hitzenberger, R. J. Aerosol Sci. 2002, 33, 1623-1634). The particles were produced by nebulizing an aqueous suspension of carbon black in a Collison atomizer. The activation of pure carbon black particles was found to require higher supersaturations than predicted by calculations representing the particles as insoluble, wettable spheres with mobility equivalent diameter. To test whether this effect is an artifact due to heating of the light-absorbing carbon black particles in the laser beam, experiments at different laser powers were conducted. No systematic dependence of the activation of pure carbon black particles on laser power was observed. The observations could be modeled using spherical particles and an effective contact angle of 4-6 degrees of water at their surface. The addition of a small amount of NaCl to the carbon black particles (by adding 5% by mass NaCl to the carbon black suspension) greatly enhanced their CCN efficiency. The measured CCN efficiencies were consistent with Kohler theory for particles consisting of insoluble and hygroscopic material. However, coating the carbon black particles with hexadecanol (a typical film-forming compound with one hydrophobic and one hydrophilic end) efficiently suppressed the CCN activation of the carbon black particles.

  20. 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.

  1. 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.

  2. Anthropogenic Influence on Secondary Aerosol Formation and Total Water-Soluble Carbon on Atmospheric Particles

    NASA Astrophysics Data System (ADS)

    Gioda, Adriana; Mateus, Vinicius; Monteiro, Isabela; Taira, Fabio; Esteves, Veronica; Saint'Pierre, Tatiana

    2013-04-01

    On a global scale, the atmosphere is an important source of nutrients, as well as pollutants, because of its interfaces with soil and water. Important compounds in the gaseous phase are in both organic and inorganic forms, such as organic acids, nitrogen, sulfur and chloride. In spite of the species in gas form, a huge number of process, anthropogenic and natural, are able to form aerosols, which may be transported over long distances. Sulfates e nitrates are responsible for rain acidity; they may also increase the solubility of organic compounds and metals making them more bioavailable, and also can act as cloud condensation nuclei (CCN). Aerosol samples (PM2.5) were collected in a rural and industrial area in Rio de Janeiro, Brazil, in order to quantify chemical species and evaluate anthropogenic influences in secondary aerosol formation and organic compounds. Samples were collected during 24 h every six days using a high-volume sampler from August 2010 to July 2011. The aerosol mass was determined by Gravimetry. The water-soluble ionic composition (WSIC) was obtained by Ion Chromatography in order to determine the major anions (NO3-, SO4= and Cl-); total water-soluble carbon (TWSC) was determined by a TOC analyzer. The average aerosol (PM2.5) concentrations ranged from 1 to 43 ug/m3 in the industrial site and from 4 to 35 ug/m3 in the rural area. Regarding anions, the highest concentrations were measured for SO42- (10.6 μg/m3-12.6 μg/m3); where the lowest value was found in the rural site and the highest in the industrial. The concentrations for NO3- and Cl- ranged from 4.2 μg/m3 to 9.3 μg/m3 and 3.1 μg/m3 to 6.4 μg /m3, respectively. Sulfate was the major species and, like nitrate, it is related to photooxidation in the atmosphere. Interestingly sulfate concentrations were higher during the dry period and could be related to photochemistry activity. The correlations between nitrate and non-sea-salt sulfate were weak, suggesting different sources for these

  3. Measurement of particle size characteristics of metered dose inhaler (MDI) aerosols.

    PubMed

    Dolovich, M

    1991-01-01

    Measurement of the aerodynamic size of an aerosol allows a prediction of its deposition efficiency and behaviour in the lung. The dynamics of volatile or pressurized (MDI) aerosols presents problems not encountered in the characterization of solid or liquid particles alone. For example, the data obtained in real-time sampling as opposed to measuring an aged aerosol provide a truer representation of circumstances during actual clinical use, yet this may be difficult to achieve due to propellent evaporation. A number of particle sizing systems have been developed based upon light scattering techniques and aerodynamic principles. Each method has its limitations; in general, they successfully measure the aerodynamic size distributions of MDI aerosols. Cascade impactors, the "gold standard" of the industry have the advantage that they allow analysis of drug mass as well as other tracers within the aerosol, but the process as a whole is labour intensive, with limited resolution. Highly automated laser-based systems developed over the past 10 years measure the surface characteristics of the aerosol rather than the direct measurement of mass. Because of different values obtained from various sizing systems, it is suggested that all MDI drugs be sized using cascade impactors but that parallel data be obtained using an alternative sizing system.

  4. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOEpatents

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

    2003-01-01

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

  5. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOEpatents

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

    2006-04-18

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

  6. The influence of marine microbial activities on aerosol production: A laboratory mesocosm study

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.; Kilthau, Wendy P.; Bothe, Dylan W.; Radway, JoAnn C.; Aller, Josephine Y.; Knopf, Daniel A.

    2015-09-01

    The oceans cover most of the Earth's surface, contain nearly half the total global primary biomass productivity, and are a major source of atmospheric aerosol particles. Here we experimentally investigate links between biological activity in seawater and sea spray aerosol (SSA) flux, a relationship of potential significance for organic aerosol loading and cloud formation over the oceans and thus for climate globally. Bubbles were generated in laboratory mesocosm experiments either by recirculating impinging water jets or glass frits. Experiments were conducted with Atlantic Ocean seawater collected off the eastern end of Long Island, NY, and with artificial seawater containing cultures of bacteria and phytoplankton Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Changes in SSA size distributions occurred during all phases of bacterial and phytoplankton growth, as characterized by cell concentrations, dissolved organic carbon, total particulate carbon, and transparent exopolymer particles (gel-forming polysaccharides representing a major component of biogenic exudate material). Over a 2 week growth period, SSA particle concentrations increased by a factor of less than 2 when only bacteria were present and by a factor of about 3 when bacteria and phytoplankton were present. Production of jet-generated SSA particles of diameter less than 200 nm increased with time, while production of all particle diameters increased with time when frits were used. The implications of a marine biological activity dependent SSA flux are discussed.

  7. 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.

  8. Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouch, N.; Pichon, J.-M.; Prévôt, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2013-09-01

    The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA

  9. Characterizing the impact of urban emissions on regional aerosol particles: airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouche, N.; Pichon, J.-M.; Bourianne, T.; Gomes, L.; Prevot, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2014-02-01

    The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation

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

    NASA Astrophysics Data System (ADS)

    Gasteiger, Josef; Groß, Silke

    2016-04-01

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

  11. 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

  12. Ultrasensitive detection of inhaled organic aerosol particles by accelerator mass spectrometry.

    PubMed

    Parkhomchuk, E V; Gulevich, D G; Taratayko, A I; Baklanov, A M; Selivanova, A V; Trubitsyna, T A; Voronova, I V; Kalinkin, P N; Okunev, A G; Rastigeev, S A; Reznikov, V A; Semeykina, V S; Sashkina, K A; Parkhomchuk, V V

    2016-09-01

    Accelerator mass spectrometry (AMS) was shown to be applicable for studying the penetration of organic aerosols, inhaled by laboratory mice at ultra-low concentration ca. 10(3) cm(-3). We synthesized polystyrene (PS) beads, composed of radiocarbon-labeled styrene, for testing them as model organic aerosols. As a source of radiocarbon we used methyl alcohol with radioactivity. Radiolabeled polystyrene beads were obtained by emulsifier-free emulsion polymerization of synthesized (14)C-styrene initiated by K2S2O8 in aqueous media. Aerosol particles were produced by pneumatic spraying of diluted (14)C-PS latex. Mice inhaled (14)C-PS aerosol consisting of the mix of 10(3) 225-nm particles per 1 cm(3) and 5·10(3) 25-nm particles per 1 cm(3) for 30 min every day during five days. Several millions of 225-nm particles deposited in the lungs and slowly excreted from them during two weeks of postexposure. Penetration of particles matter was also observed for liver, kidneys and brain, but not for a heart. PMID:27281540

  13. Design of Gas-phase Synthesis of Core-Shell Particles by Computational Fluid – Aerosol Dynamics

    PubMed Central

    Buesser, B.; Pratsinis, S.E.

    2013-01-01

    Core-shell particles preserve the bulk properties (e.g. magnetic, optical) of the core while its surface is modified by a shell material. Continuous aerosol coating of core TiO2 nanoparticles with nanothin silicon dioxide shells by jet injection of hexamethyldisiloxane precursor vapor downstream of titania particle formation is elucidated by combining computational fluid and aerosol dynamics. The effect of inlet coating vapor concentration and mixing intensity on product shell thickness distribution is presented. Rapid mixing of the core aerosol with the shell precursor vapor facilitates efficient synthesis of hermetically coated core-shell nanoparticles. The predicted extent of hermetic coating shells is compared to the measured photocatalytic oxidation of isopropanol by such particles as hermetic SiO2 shells prevent the photocatalytic activity of titania. Finally the performance of a simpler, plug-flow coating model is assessed by comparisons to the present detailed CFD model in terms of coating efficiency and silica average shell thickness and texture. PMID:23729817

  14. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

    PubMed

    Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

    2015-03-01

    Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a.

  15. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

    PubMed

    Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

    2015-03-01

    Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a. PMID:25766014

  16. 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

  17. 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

  18. Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a Central European mountain site during HCCT-2010

    NASA Astrophysics Data System (ADS)

    Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.

    2015-09-01

    Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm have been analysed by on-line single particle aerosol mass spectrometry during the six-week study HCCT-2010 in September/October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in Central Germany. More than 170 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 14 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters indicating a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while in general organic particles were less abundant in the cloud residues. In the case of amines this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulphate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulphate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of the particles

  19. Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a central European mountain site during HCCT-2010

    NASA Astrophysics Data System (ADS)

    Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.

    2016-01-01

    Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm were analysed by online single particle aerosol mass spectrometry during the 6-week study Hill Cap Cloud Thuringia (HCCT)-2010 in September-October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in central Germany. More than 160 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 13 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters having a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues, the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while, in general, organic particles were less abundant in the cloud residues. In the case of amines, this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulfate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulfate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of

  20. A numerical simulation of atmospheric photochemical processes including interactions with aerosol particles

    SciTech Connect

    Hackler, M.A.

    1989-01-01

    We propose a comprehensive model of atmospheric photochemical processes that can be used to investigate the interactions between gas species and aerosol particles. We considered both gas and particle phase reactions, transport of material between these phases, convection, turbulent diffusion, particle growth, coagulation, nucleation, and sources. The aerosol particle phase is not forced to follow the gas phase in equilibrium; transport to the particles is described by diffusion to the particle surface. The resulting model treats 33 gas phase species and 39 particles phase species; 16 of these are transported between the phases. The particle size distribution is approximated by 9 sections between 0.01 and 10 {mu}m diameter. Strong interactions between the gas and particles are seen. Higher relative humidity results in more particle volume and surface area, allowing the interphase transport to become competitive with the reaction terms. In particular, at high relative humidities the increased scavenging of HO{sub 2} radicals by particles reduces the O{sub 3} maximum concentration. This effect is seen only on days when the maximum relative humidity exceeds 90%. This conclusion has implications for the applicability of models developed for the Los Angeles Basin, where the maximum relative humidity rarely exceeds 75%, to more humid climates like Houston.

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

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

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

  2. The single scattering properties of the aerosol particles as aggregated spheres

    NASA Astrophysics Data System (ADS)

    Wu, Y.; Gu, X.; Cheng, T.; Xie, D.; Yu, T.; Chen, H.; Guo, J.

    2012-08-01

    The light scattering and absorption properties of anthropogenic aerosol particles such as soot aggregates are complicated in the temporal and spatial distribution, which introduce uncertainty of radiative forcing on global climate change. In order to study the single scattering properties of anthorpogenic aerosol particles, the structures of these aerosols such as soot paticles and soot-containing mixtures with the sulfate or organic matter, are simulated using the parallel diffusion limited aggregation algorithm (DLA) based on the transmission electron microscope images (TEM). Then, the single scattering properties of randomly oriented aerosols, such as scattering matrix, single scattering albedo (SSA), and asymmetry parameter (AP), are computed using the superposition T-matrix method. The comparisons of the single scattering properties of these specific types of clusters with different morphological and chemical factors such as fractal parameters, aspect ratio, monomer radius, mixture mode and refractive index, indicate that these different impact factors can respectively generate the significant influences on the single scattering properties of these aerosols. The results show that aspect ratio of circumscribed shape has relatively small effect on single scattering properties, for both differences of SSA and AP are less than 0.1. However, mixture modes of soot clusters with larger sulfate particles have remarkably important effects on the scattering and absorption properties of aggregated spheres, and SSA of those soot-containing mixtures are increased in proportion to the ratio of larger weakly absorbing attachments. Therefore, these complex aerosols come from man made pollution cannot be neglected in the aerosol retrievals. The study of the single scattering properties on these kinds of aggregated spheres is important and helpful in remote sensing observations and atmospheric radiation balance computations.

  3. Stable Carbon Fractionation In Size Segregated Aerosol Particles Produced By Controlled Biomass Burning

    NASA Astrophysics Data System (ADS)

    Masalaite, Agne; Garbaras, Andrius; Garbariene, Inga; Ceburnis, Darius; Martuzevicius, Dainius; Puida, Egidijus; Kvietkus, Kestutis; Remeikis, Vidmantas

    2014-05-01

    Biomass burning is the largest source of primary fine fraction carbonaceous particles and the second largest source of trace gases in the global atmosphere with a strong effect not only on the regional scale but also in areas distant from the source . Many studies have often assumed no significant carbon isotope fractionation occurring between black carbon and the original vegetation during combustion. However, other studies suggested that stable carbon isotope ratios of char or BC may not reliably reflect carbon isotopic signatures of the source vegetation. Overall, the apparently conflicting results throughout the literature regarding the observed fractionation suggest that combustion conditions may be responsible for the observed effects. The purpose of the present study was to gather more quantitative information on carbonaceous aerosols produced in controlled biomass burning, thereby having a potential impact on interpreting ambient atmospheric observations. Seven different biomass fuel types were burned under controlled conditions to determine the effect of the biomass type on the emitted particulate matter mass and stable carbon isotope composition of bulk and size segregated particles. Size segregated aerosol particles were collected using the total suspended particle (TSP) sampler and a micro-orifice uniform deposit impactor (MOUDI). The results demonstrated that particle emissions were dominated by the submicron particles in all biomass types. However, significant differences in emissions of submicron particles and their dominant sizes were found between different biomass fuels. The largest negative fractionation was obtained for the wood pellet fuel type while the largest positive isotopic fractionation was observed during the buckwheat shells combustion. The carbon isotope composition of MOUDI samples compared very well with isotope composition of TSP samples indicating consistency of the results. The measurements of the stable carbon isotope ratio in

  4. A case study of urban particle acidity and its influence on secondary organic aerosol.

    PubMed

    Zhang, Qi; Jimenez, Jose L; Worsnop, Douglas R; Canagaratna, Manjula

    2007-05-01

    Size-resolved indicators of aerosol acidity, including H+ ion concentrations (H+Aer) and the ratio of stoichiometric neutralization are evaluated in submicrometer aerosols using highly time-resolved aerosol mass spectrometer (AMS) data from Pittsburgh. The pH and ionic strength within the aqueous particle phase are also estimated using the Aerosol Inorganics Model (AIM). Different mechanisms that contribute to the presence of acidic particles in Pittsburgh are discussed. The largest H+Aer loadings and lowest levels of stoichiometric neutralization were detected when PM1 loadings were high and dominated by SO4(2-). The average size distribution of H+Aer loading shows an accumulation mode at Dva approximately 600 nm and an enhanced smaller mode that centers at Dva approximately 200 nm and tails into smaller sizes. The acidity in the accumulation mode particles suggests that there is generally not enough gas-phase NH3 available on a regional scale to completely neutralize sulfate in Pittsburgh. The lack of stoichiometric neutralization in the 200 nm mode particles is likely caused by the relatively slow mixing of gas-phase NH3 into SO2-rich plumes containing younger particles. We examined the influence of particle acidity on secondary organic aerosol (SOA) formation by comparing the mass concentrations and size distributions of oxygenated organic aerosol (00A--surrogate for SOA in Pittsburgh) during periods when particles are, on average, acidic to those when particles are bulk neutralized. The average mass concentration of ODA during the acidic periods (3.1 +/- 1.7 microg m(-3)) is higher than that during the neutralized periods (2.5 +/- 1.3 microg m(-3)). Possible reasons for this enhancement include increased condensation of SOA species, acid-catalyzed SOA formation, and/or differences in air mass transport and history. However, even if the entire enhancement (approximately 0.6 microg m(-3)) can be attributed to acid catalysis, the upperbound increase of SOA mass

  5. Elucidating determinants of aerosol composition through particle-type-based receptor modeling

    NASA Astrophysics Data System (ADS)

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

    2011-03-01

    An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in Southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources were reflected through three factors: two biomass burning factors and a highly chemically processed long range transport factor. The biomass burning factors were separated by PMF due to differences in chemical processing which were caused in part by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range

  6. Elucidating determinants of aerosol composition through particle-type-based receptor modeling

    NASA Astrophysics Data System (ADS)

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

    2011-08-01

    An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

  7. Chemical composition of individual aerosol particles from working areas in a nickel refinery.

    PubMed

    Höflich, B L; Wentzel, M; Ortner, H M; Weinbruch, S; Skogstad, A; Hetland, S; Thomassen, Y; Chaschin, V P; Nieboer, E

    2000-06-01

    Individual aerosol particles (n = 1170) collected at work stations in a nickel refinery were analyzed by wavelength-dispersive electron-probe microanalysis. By placing arbitrary restrictions on the contents of sulfur and silicon, the particles could be divided into four main groups. Scanning electron images indicated that most of the particles examined were relatively small (< or = 2 microm, equivalent projected area diameter), and that their morphology suggested formation from a melt. There was an absence of well-defined phases and simple stoichiometries, indicating that exposures to pure substances such as nickel subsulfide or specific oxides appeared not to occur. Although the elemental composition of particles varied greatly, a rough association was evident with the known elemental content of the refinery intermediates. The implications of the findings for aerosol speciation measurements, toxicological studies and interpretation of adverse health effects are explored. PMID:11256701

  8. Heterogeneous Reactivity of Nitric Acid with Nascent Sea Spray Aerosol: Large Differences Observed between and within Individual Particles.

    PubMed

    Ault, Andrew P; Guasco, Timothy L; Baltrusaitis, Jonas; Ryder, Olivia S; Trueblood, Jonathan V; Collins, Douglas B; Ruppel, Matthew J; Cuadra-Rodriguez, Luis A; Prather, Kimberly A; Grassian, Vicki H

    2014-08-01

    Current climate and atmospheric chemistry models assume that all sea spray particles react as if they are pure NaCl. However, recent studies of sea spray aerosol particles have shown that distinct particle types exist (including sea salt, organic carbon, and biological particles) as well as mixtures of these and, within each particle type, there is a range of single-particle chemical compositions. Because of these differences, individual particles should display a range of reactivities with trace atmospheric gases. Herein, to address this, we study the composition of individual sea spray aerosol particles after heterogeneous reaction with nitric acid. As expected, a replacement reaction of chloride with nitrate is observed; however, there is a large range of reactivities spanning from no reaction to complete reaction between and within individual sea spray aerosol particles. These data clearly support the need for laboratory studies of individual, environmentally relevant particles to improve our fundamental understanding as to the properties that determine reactivity.

  9. Aerosols in Amazonia: Natural biogenic particles and large scale biomass burning impacts

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Barbosa, Henrique M. J.; Rizzo, Luciana V.; Brito, Joel F.; Sena, Elisa T.; Cirino, Glauber G.; Arana, Andrea

    2013-05-01

    The Large Scale Biosphere Atmosphere Experiment in Amazonia (LBA) is a long term (20 years) research effort aimed at the understanding of the functioning of the Amazonian ecosystem. In particular, the strong biosphere-atmosphere interaction is a key component looking at the exchange processes between vegetation and the atmosphere, focusing on aerosol particles. Two aerosol components are the most visible: The natural biogenic emissions of aerosols and VOCs, and the biomass burning emissions. A large effort was done to characterize natural biogenic aerosols that showed detailed organic characterization and optical properties. The biomass burning component in Amazonia is important in term of aerosol and trace gases emissions, with deforestation rates decreasing, from 27,000 Km2 in 2004 to about 5,000 Km2 in 2011. Biomass burning emissions in Amazonia increases concentrations of aerosol particles, CO, ozone and other species, and also change the surface radiation balance in a significant way. Long term monitoring of aerosols and trace gases were performed in two sites: a background site in Central Amazonia, 55 Km North of Manaus (called ZF2 ecological reservation) and a monitoring station in Porto Velho, Rondonia state, a site heavily impacted by biomass burning smoke. Several instruments were operated to measured aerosol size distribution, optical properties (absorption and scattering at several wavelengths), composition of organic (OC/EC) and inorganic components among other measurements. AERONET and MODIS measurements from 5 long term sites show a large year-to year variability due to climatic and socio-economic issues. Aerosol optical depths of more than 4 at 550nm was observed frequently over biomass burning areas. In the pristine Amazonian atmosphere, aerosol scattering coefficients ranged between 1 and 200 Mm-1 at 450 nm, while absorption ranged between 1 and 20 Mm-1 at 637 nm. A strong seasonal behavior was observed, with greater aerosol loadings during the

  10. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    PubMed

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-01

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

  11. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    PubMed

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-01

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry. PMID:26348650

  12. Pulse height response of an optical particle counter to monodisperse aerosols

    NASA Technical Reports Server (NTRS)

    Wilmoth, R. G.; Grice, S. S.; Cuda, V.

    1976-01-01

    The pulse height response of a right angle scattering optical particle counter has been investigated using monodisperse aerosols of polystyrene latex spheres, di-octyl phthalate and methylene blue. The results confirm previous measurements for the variation of mean pulse height as a function of particle diameter and show good agreement with the relative response predicted by Mie scattering theory. Measured cumulative pulse height distributions were found to fit reasonably well to a log normal distribution with a minimum geometric standard deviation of about 1.4 for particle diameters greater than about 2 micrometers. The geometric standard deviation was found to increase significantly with decreasing particle diameter.

  13. Deposition of aerosol particles in human lungs: in vivo measurements and modeling

    EPA Science Inventory

    The deposition dose and site of inhaled particles within the lung are the key determinants in health risk assessment of particulate pollutants. Accurate dose estimation, however, is a formidable task because aerosol transport and deposition in the lung are governed by many factor...

  14. USE OF CONTINUOUS MEASUREMENTS OF INTEGRAL AEROSOL PARAMETERS TO ESTIMATE PARTICLE SURFACE AREA

    EPA Science Inventory

    This study was undertaken because of interest in using particle surface area as an indicator for studies of the health effects of particulate matter. First, we wished to determine the integral parameter of the size distribution measured by the electrical aerosol detector. Secon...

  15. Measurement of Fluorescence Spectra from Ambient Aerosol Particles Using Laser-induced Fluorescence Technique

    NASA Astrophysics Data System (ADS)

    Taketani, F.; Kanaya, Y.; Nakamura, T.; Moteki, N.; Takegawa, N.

    2011-12-01

    To obtain the information of composition of organic aerosol particles in atmosphere, we developed an instrument using laser-induced fluorescence (LIF) technique. To measure the fluorescence from a particle, we employed two lasers. Scattering light signal derived from a single particle upon crossing the 635nm-CW laser triggers the 266nm-pulsed laser to excite the particle. Fluorescence from the particle in the wavelength range 300-600nm is spectrally dispersed by a grating spectrometer and then detected by a 32-Ch photo-multiplier tube(PMT). The aerosol stream is surrounded by a coaxial sheath air flow and delivered to the optical chamber at atmospheric pressure. Using PSL particles with known sizes, we made a calibration curve to estimate particle size from scattering light intensity. With the current setup of the instrument we are able to detect both scattering and fluorescence from particles whose diameters are larger than 0.5um. Our system was able to differentiate particles composed of mono-aromatic species (e.g. Tryptophan) from those of Riboflavin, by their different fluorescence wavelengths. Also, measurements of fluorescence spectra of ambient particles were demonstrated in our campus in Yokosuka city, facing Tokyo bay in Japan. We obtained several types of florescence spectra in the 8 hours. Classification of the measured fluorescence spectra will be discussed in the presentation.

  16. The Composition of Individual Aerosol Particles over the North Slope of Alaska during ISDAC

    NASA Astrophysics Data System (ADS)

    Zelenyuk, A.; Imre, D.; Liu, P.; MacDonald, A.; Leaitch, R.

    2008-12-01

    During the month of April 2008 a single particle mass spectrometer, SPLAT II, was deployed on board the Canadian National Research Council Convair 580 aircraft for participation in the Indirect and Semi-Direct Aerosol Campaign (ISDAC). ISDAC's main scientific objective was to improve our understanding of the relationship between the properties of aerosol particles over the North Pole and their impact on the regional climate. During ISDAC SPLAT II participated in all 27 flights that lasted slightly over 100 hrs. It measured the size of more than 10 million particles and characterized the composition of over 3 million of them. When sampling in clear air SPLAT II measured a wide range of particle compositions, including sulfates mixed with organics, nitrates mixed with organic, processed and freshly emitted sea-salt, a few dust particles, and a significant number of biomass burning particles. Many of these particle types appeared in aerosol layers that had horizontal and vertical filamentous structures. Biomass burning particles, many of which were transported from Asia, were rather prevalent over the North Slope of Alaska during the campaign. Since one of the main goals of this campaign was to characterize cloud properties, large fraction of the data was collected through the CVI inlet. The ice-clouds sampled in ISDAC had typically very low ice crystal concentrations; correspondingly, when sampled through the CVI inlet the number of characterized particles drops precipitously. Despite the low number concentrations SPLAT was able to measure the size and composition of thousands of ice-nuclei. Since the CVI inlet transmits, in addition to ice crystals, liquid droplets, SPLAT was able to characterize a large number of particles that served as cloud condensation nuclei as well. We will present a preliminary analysis of the single particle data collected during this campaign.

  17. Organic carbon in the sea surface microlayer and in submicron aerosol particles - measurements from the Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    van Pinxteren, Manuela; Wadinga Fomba, Kanneh; Müller, Konrad; Barthel, Stefan; von Tümpling, Wolf; Herrmann, Hartmut

    2016-04-01

    The export of organic compounds from the oceans can establish a considerable carbon flux in the Earth system. The detailed transport processes and especially the impact of environmental drivers in the organic carbon transfer are not yet fully understood. Here we present a broad study of measured dissolved organic carbon (DOC) and particulate organic carbon (POC) concentrations and enrichment in the sea surface microlayer (SML) as well as equivalent measurements in marine aerosol particles. For the first time, enrichment factors of organic carbon in marine ambient aerosol are reported that based on concerted measurements of seawater and aerosol particles. The measurements were conducted at different field campaigns in the Atlantic Ocean: at the Cape Verde islands, during two Atlantic transects with the RV Polarstern, and during a campaign at the Raune Fjord in Bergen, Norway. In oceanic water, concentration of DOC were in average 161 μmol/L in bulk water and 225 μmol/L in the SML. Average POC concentrations were 13 μmol/L in bulk water and 17 μmol/L in the SML. Instead of a constant enrichment of DOC or POC there are rather two pattern: high enrichment in samples with low concentrations and low enrichment when concentration were high. In seawater (bulk water and SML) small, mostly insignificant effects, concerning concentration and enrichment of DOC and POC were found regarding the impact of wind stress and chl-a concentrations. Differences between SML and bulk water concentrations are more pronounced at times of high chl-a, but all in all these effects are not strong. The thickness of the SML is affected by biological activity but probably caused by a more surface-active part of the DOC/POC pool and this is not reflected in the sum parameters. In the ambient marine aerosol particles water-soluble organic carbon (WSOC) and water-insoluble organic carbon (WISOC) concentrations were in average about 0.2 μg m-3, respectively. Higher concentration differences of

  18. Particle fallout/activity sensor

    NASA Astrophysics Data System (ADS)

    Curtis, Ihlefeld M.; Youngquist, Robert C.; Moerk, John S.; Rose, Kenneth A., III

    1995-05-01

    A particle fallout/activity sensor measures relative amounts of dust or other particles which collect on a mirror in an area to be monitored. The sensor includes a sensor module and a data acquisition module, both of which can be operated independently of one another or in combination with one another. The sensor module includes a housing containing the mirror, an LED assembly for illuminating the mirror and an optical detector assembly for detecting light scattered off of the mirror by dust or other particles collected thereon. A microprocessor controls operation of the sensor module's components and displays results of a measurement on an LCD display mounted on the housing. A push button switch is also mounted on the housing which permits manual initiation of a measurement. The housing is constructed of light absorbing material, such as black delrin, which minimizes detection of light by the optical detector assembly other than that scattered by dust or particles on the mirror. The data acquisition module can be connected to the sensor module and includes its own microprocessor, a timekeeper and other digital circuitry for causing the sensor module to make a measurement periodically and send the measurement data to the data acquisition module for display and storage in memory for later retrieval and transfer to a separate computer. The time tagged measurement data can also be used to determine the relative level of activity in the monitored area since this level is directly related to the amount of dust or particle fallout in the area.

  19. Mass concentration and mineralogical characteristics of aerosol particles collected at Dunhuang during ACE-Asia

    NASA Astrophysics Data System (ADS)

    Shen, Z. X.; Cao, J. J.; Li, X. X.; Okuda, T.; Wang, Y. Q.; Zhang, X. Y.

    2006-03-01

    Measurements were performed in spring 2001 and 2002 to determine the characteristics of soil dust in the Chinese desert region of Dunhuang, one of the ground sites of the Asia-Pacific Regional Aerosol Characterization Experiment (ACE-Asia). The mean mass concentrations of total suspended particle matter during the spring of 2001 and 2002 were 317 mu g m(-3) and 307 mu g m(-3) respectively. Eleven dust storm events were observed with a mean aerosol concentration of 1095 mu g m(-3), while the non-dusty days with calm or weak wind speed had a background aerosol loading of 196 mu g m(-3) on average in the springtime. The main minerals detected in the aerosol samples by X-ray diffraction were illite, kaolinite, chlorite, quartz, feldspar, calcite and dolomite. Gypsum, halite and amphibole were also detected in a few samples. The mineralogical data also show that Asian dust is characterized by a kaolinite to chlorite (K/C) ratio lower than 1 whereas Saharan dust exhibits a K/C ratio larger than 2. Air mass back- trajectory analysis show that three families of pathways are associated with the aerosol particle transport to Dunhuang, but these have similar K/C ratios, which further demonstrates that the mineralogical characteristics of Asian dust are different from African dust.

  20. Microscopy and Spectroscopy Techniques to Guide Parameters for Modeling Mineral Dust Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Veghte, D. P.; Moore, J. E.; Jensen, L.; Freedman, M. A.

    2013-12-01

    Mineral dust aerosol particles are the second largest emission by mass into the atmosphere and contribute to the largest uncertainty in radiative forcing. Due to the variation in size, composition, and shape, caused by physical and chemical processing, uncertainty exists as to whether mineral dust causes a net warming or cooling effect. We have used Cavity Ring-Down Aerosol Extinction Spectroscopy (CRD-AES), Scanning Electron Microscopy (SEM), and Transmission Electron Microscopy (TEM) to measure extinction cross sections and morphologies of size-selected, non-absorbing and absorbing mineral dust aerosol particles. We have found that microscopy is essential for characterizing the polydispersity of the size selection of non-spherical particles. Through the combined use of CRD-AES, microscopy, and computation (Mie theory and Discreet Dipole Approximation), we have determined the effect of shape on the optical properties of additional species including clay minerals, quartz, and hematite in the sub-micron regime. Our results have shown that calcite can be treated as polydisperse spheres while quartz and hematite need additional modeling parameters to account for their irregularity. Size selection of clay minerals cannot be performed due to their irregular shape, but microscopy techniques can be used to better quantify the particle aspect ratio. Our results demonstrate a new method that can be used to extend cavity ring-down spectroscopy for the measurement of the optical properties of non-spherical particles. This characterization will lead to better aerosol extinction parameters for modeling aerosol optical properties in climate models and satellite retrieval algorithms.

  1. Real-time measurement of sodium chloride in individual aerosol particles by mass spectrometry

    NASA Technical Reports Server (NTRS)

    Sinha, M. P.; Friedlander, S. K.

    1985-01-01

    The method of particle analysis by mass spectrometry has been applied to the quantitative measurement of sodium chloride in individual particles on a real-time basis. Particles of known masses are individually introduced, in the form of a beam, into a miniature Knudsen cell oven (1600 K). The oven is fabricated from rhenium metal sheet (0.018 mm thick) and is situated in the ion source of a quadrupole mass spectrometer. A particle once inside the oven is trapped and completely volatilized; this overcomes the problem of partial volatilization due to particles bouncing from the filament surface. Individual particles are thermally volatilized and ionized inside the rhenium oven, and produce discrete sodium ion pulses whose intensities are measured with the quadrupole mass spectrometer. An ion pulse width of several milliseconds (4-12 ms) is found for particles in the mass range 1.3 x 10 to the -13th to 5.4 x 10 to the -11th g. The sodium ion intensity is found to be proportional to the particle mass to the 0.86-power. The intensity distribution for monodisperse aerosol particles possesses a geometric standard deviation of 1.09, showing that the method can be used for the determination of the mass distribution function with good resolution in a polydisperse aerosol.

  2. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight.

    PubMed

    Loh, N D; Hampton, C Y; Martin, A V; Starodub, D; Sierra, R G; Barty, A; Aquila, A; Schulz, J; Lomb, L; Steinbrener, J; Shoeman, R L; Kassemeyer, S; Bostedt, C; Bozek, J; Epp, S W; Erk, B; Hartmann, R; Rolles, D; Rudenko, A; Rudek, B; Foucar, L; Kimmel, N; Weidenspointner, G; Hauser, G; Holl, P; Pedersoli, E; Liang, M; Hunter, M S; Hunter, M M; Gumprecht, L; Coppola, N; Wunderer, C; Graafsma, H; Maia, F R N C; Ekeberg, T; Hantke, M; Fleckenstein, H; Hirsemann, H; Nass, K; White, T A; Tobias, H J; Farquar, G R; Benner, W H; Hau-Riege, S P; Reich, C; Hartmann, A; Soltau, H; Marchesini, S; Bajt, S; Barthelmess, M; Bucksbaum, P; Hodgson, K O; Strüder, L; Ullrich, J; Frank, M; Schlichting, I; Chapman, H N; Bogan, M J

    2012-06-28

    The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis.

  3. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight.

    PubMed

    Loh, N D; Hampton, C Y; Martin, A V; Starodub, D; Sierra, R G; Barty, A; Aquila, A; Schulz, J; Lomb, L; Steinbrener, J; Shoeman, R L; Kassemeyer, S; Bostedt, C; Bozek, J; Epp, S W; Erk, B; Hartmann, R; Rolles, D; Rudenko, A; Rudek, B; Foucar, L; Kimmel, N; Weidenspointner, G; Hauser, G; Holl, P; Pedersoli, E; Liang, M; Hunter, M S; Hunter, M M; Gumprecht, L; Coppola, N; Wunderer, C; Graafsma, H; Maia, F R N C; Ekeberg, T; Hantke, M; Fleckenstein, H; Hirsemann, H; Nass, K; White, T A; Tobias, H J; Farquar, G R; Benner, W H; Hau-Riege, S P; Reich, C; Hartmann, A; Soltau, H; Marchesini, S; Bajt, S; Barthelmess, M; Bucksbaum, P; Hodgson, K O; Strüder, L; Ullrich, J; Frank, M; Schlichting, I; Chapman, H N; Bogan, M J

    2012-06-28

    The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis. PMID:22739316

  4. Single-particle light-scattering measurement: photochemical aerosols and atmospheric particulates.

    PubMed

    Phillips, D T; Wyatt, P J

    1972-09-01

    The use of single-particle light-scattering measurements to determine the origin of atmospheric hazes has been explored by measurement of laboratory aerosols, field samples, and computer analysis of the light-scattering data. The refractive index of measured spherical particles 800 nm to 1000 nm in diameter was determined within 2%. For particles of diameter less than 500 nm the measurement of absolute scattering intensity is required for complete analysis. Distinctive nonspherical and absorbing particles were observed both in automotive exhaust and atmospheric samples. Electrostatic suspension of atmospheric particulates is demonstrated to provide a practical approach to optical measurement of single particles. The technique may be used to calibrate optical particle counters or identify particles with unique shape or refractive index.

  5. GAS-PARTICLE PARTITIONING OF SEMI-VOLATILE ORGANICS ON ORGANIC AEROSOLS USING A PREDICTIVE ACTIVITY COEFFICIENT MODEL: ANALYSIS OF THE EFFECTS OF PARAMETER CHOICES ON MODEL PERFORMANCE. (R826771)

    EPA Science Inventory

    The partitioning of a diverse set of semivolatile organic compounds (SOCs) on a variety of organic aerosols was studied using smog chamber experimental data. Existing data on the partitioning of SOCs on aerosols from wood combustion, diesel combustion, and the Incorporation of advanced aerosol activation treatments into CESM/CAM5: model evaluation and impacts on aerosol indirect effects

    NASA Astrophysics Data System (ADS)

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

    2014-07-01

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

  6. Ice nucleus activity measurements of solid rocket motor exhaust particles

    NASA Technical Reports Server (NTRS)

    Keller, V. W. (Compiler)

    1986-01-01

    The ice Nucleus activity of exhaust particles generated from combustion of Space Shuttle propellant in small rocket motors has been measured. The activity at -20 C was substantially lower than that of aerosols generated by unpressurized combustion of propellant samples in previous studies. The activity decays rapidly with time and is decreased further in the presence of moist air. These tests corroborate the low effectivity ice nucleus measurement results obtained in the exhaust ground cloud of the Space Shuttle. Such low ice nucleus activity implies that Space Shuttle induced inadvertent weather modification via an ice phase process is extremely unlikely.

  7. The Effect of Particle Size on Iron Solubility in Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Marcotte, A. R.; Majestic, B. J.; Anbar, A. D.; Herckes, P.

    2012-12-01

    The long range transport of mineral dust aerosols, which contain approximately 3% iron by mass, results in an estimated 14-16 Tg of iron deposited into the oceans annually; however, only a small percentage of the deposited iron is soluble. In high-nutrient, low chlorophyll ocean regions iron solubility may limit phytoplankton primary productivity. Although the atmospheric transport processes of mineral dust aerosols have been well studied, the role of particle size has been given little attention. In this work, the effect of particle size on iron solubility in atmospheric aerosols is examined. Iron-containing minerals (illite, kaolinite, magnetite, goethite, red hematite, black hematite, and quartz) were separated into five size fractions (10-2.5, 2.5-1, 1-0.5, 0.5-0.25, and <0.25μm) and extracted into buffer solutions simulating environments in the transport of aerosol particles for 150 minutes. Particle size was confirmed by scanning electron microscopy (SEM). Soluble iron content of the extracted mineral solutions was determined by inductively coupled plasma-mass spectrometry (ICP-MS). Extracted mineral solutions were also analyzed for Fe(II) and Fe(III) content using a ferrozine/UV-VIS method. Preliminary results show that differences in solution composition are more important than differences in size. When extracted into acetate and cloudwater buffers (pH 4.25-4.3), < 0.3% of the Fe in iron oxides (hematite, magnetite, and goethite) is transferred to solution as compared to ~0.1-35% for clays (kaolinite and illite). When extracted into a marine aerosol solution (pH 1.7), the percentage of Fe of the iron oxides and clays transferred to solution increases to approximately 0.5-3% and 5-70%, respectively. However, there is a trend of increased %Fe in the minerals transferred to solution in the largest and smallest size fractions (~0.01-0.3% and ~0.5-35% for iron oxides and clays, respectively), and decreased %Fe in the minerals transferred to solution in the mid

  8. Particle growth by acid-catalyzed heterogeneous reactions of organic carbonyls on preexisting aerosols.

    PubMed

    Jang, Myoseon; Carroll, Brian; Chandramouli, Bharadwaj; Kamens, Richard M

    2003-09-01

    Aerosol growth by the heterogeneous reactions of different aliphatic and alpha,beta-unsaturated carbonyls in the presence/absence of acidified seed aerosols was studied in a 2 m long flow reactor (2.5 cm i.d.) and a 0.5-m3 Teflon film bag under darkness. For the flow reactor experiments, 2,4-hexadienal, 5-methyl-3-hexen-2-one, 2-cyclohexenone, 3-methyl-2-cyclopentenone, 3-methyl-2-cyclohexenone, and octanal were studied. The carbonyls were selected based on their reactivity for acid-catalyzed reactions, their proton affinity, and their similarity to the ring-opening products from the atmospheric oxidation of aromatics. To facilitate acid-catalyzed heterogeneous hemiacetal/acetal formation, glycerol was injected along with inorganic seed aerosols into the flow reactor system. Carbonyl heterogeneous reactions were accelerated in the presence of acid catalysts (H2SO4), leading to higher aerosol yields than in their absence. Aldehydes were more reactive than ketones for acid-catalyzed reactions. The conjugated functionality also resulted in higher organic aerosol yieldsthan saturated aliphatic carbonyls because conjugation with the olefinic bond increases the basicity of the carbonyl leading to increased stability of the protonated carbonyl. Aerosol population was measured from a series of sampling ports along the length of the flow reactor using a scanning mobility particle sizer. Fourier transform infrared spectrometry of either an impacted liquid aerosol layer or direct reaction of carbonyls as a thin liquid layer on a zinc selenide FTIR disk was employed to demonstrate the direct transformation of chemical functional groups via the acid-catalyzed reactions. These results strongly indicate that atmospheric multifunctional organic carbonyls, which are created by atmospheric photooxidation reactions, can contribute significantly to secondary organic aerosol formation through acid-catalyzed heterogeneous reactions. Exploratory studies in 25- and 190-m3 outdoor chambers

  9. Hazardous particle binder, coagulant and re-aerosolization inhibitor

    DOEpatents

    Krauter, Paula; Zalk, David; Hoffman, D. Mark

    2011-04-12

    A copolymer and water/ethanol solvent solution capable of binding with airborne contaminants or potential airborne contaminants, such as biological weapon agents or toxic particulates, coagulating as the solvent evaporates, and adhering the contaminants to a surface so as to inhibit the re-suspension of such contaminants. The solution uses a water or ethanol/water mixture for the solvent, and a copolymer having one of several functional group sets so as to have physical and chemical characteristics of high adhesion, low viscosity, low surface tension, negative electrostatic charge, substantially neutral pH, and a low pKa. Use of the copolymer solution prevents re-aerosolization and transport of unwanted, reactive species thus increasing health and safety for personnel charged with decontamination of contaminated buildings and areas.

  10. Hazardous particle binder, coagulant and re-aerosolization inhibitor

    DOEpatents

    Krauter, Paula; Zalk, David; Hoffman, D. Mark

    2012-07-10

    A copolymer and water/ethanol solvent solution capable of binding with airborne contaminants or potential airborne contaminants, such as biological weapon agents or toxic particulates, coagulating as the solvent evaporates, and adhering the contaminants to a surface so as to inhibit the re-suspension of such contaminants. The solution uses a water or ethanol/water mixture for the solvent, and a copolymer having one of several functional group sets so as to have physical and chemical characteristics of high adhesion, low viscosity, low surface tension, negative electrostatic charge, substantially neutral pH, and a low pKa. Use of the copolymer solution prevents re-aerosolization and transport of unwanted, reactive species thus increasing health and safety for personnel charged with decontamination of contaminated buildings and areas.

  11. Gas-particle partitioning of semivolatile organic compounds (SOCs) on mixtures of aerosols in a smog chamber.

    PubMed

    Chandramouli, Bharadwaj; Jang, Myoseon; Kamens, Richard M

    2003-09-15

    The partitioning behavior of a set of diverse SOCs on two and three component mixtures of aerosols from different sources was studied using smog chamber experimental data. A set of SOCs of different compound types was introduced into a system containing a mixture of aerosols from two or more sources. Gas and particle samples were taken using a filter-filter-denuder sampling system, and a partitioning coefficient Kp was estimated using Kp = Cp/(CgTSP). Particle size distributions were measured using a differential mobility analyzer and a light scattering detector. Gas and particle samples were analyzed using GCMS. The aerosol composition in the chamber was tracked chemically using a combination of signature compounds and the organic matter mass fraction (f(om)) of the individual aerosol sources. The physical nature of the aerosol mixture in the chamber was determined using particle size distributions, and an aggregate Kp was estimated from theoretically calculated Kp on the individual sources. Model fits for Kp showed that when the mixture involved primary sources of aerosol, the aggregate Kp of the mixture could be successfully modeled as an external mixture of the Kp on the individual aerosols. There were significant differences observed for some SOCs between modeling the system as an external and as an internal mixture. However, when one of the aerosol sources was secondary, the aggregate model Kp required incorporation of the secondary aerosol products on the preexisting aerosol for adequate model fits. Modeling such a system as an external mixture grossly overpredicted the Kp of alkanes in the mixture. Indirect evidence of heterogeneous, acid-catalyzed reactions in the particle phase was also seen, leading to a significant increase in the polarity of the resulting aerosol mix and a resulting decrease in the observed Kp of alkanes in the chamber. The model was partly consistent with this decrease but could not completely explain the reduction in Kp because of

  12. Single-Particle Black Carbon Aerosol Verticle Profiles From the Boundary Layer to the Lower Stratosphere

    NASA Astrophysics Data System (ADS)

    Schwarz, J. P.; Gao, R. S.; Fahey, D. W.; Laurel, W. A.; Thomson, D. S.; Kok, G. L.; Baumgardner, D.; Wilson, J. C.; Lopez, J.; Aikin, K.; Jost, H.; Thompson, T. L.; Reeves, J. M.; Lowenstein, M.

    2005-12-01

    A single-particle soot photometer (SP2) was flown on a NASA WB-57F high-altitude research aircraft in November 2004 from Houston, TX. The SP2 uses laser-induced incandescence to directly measure the mass of individual black-carbon (BC) particles in the mass range of ~0.3-300 fg. Scattered light is used to size non-absorbing aerosols in the range of ~150 - 700 nm diameter. Data from two mid-latitude flights has been used to generate size distributions and profiles of both aerosol types from the boundary layer to the lower stratosphere. Results for scattering aerosol concentrations are in good agreement with typical particle spectrometer measurements in the same region. Mass mixing ratios of BC between 5 and 18.7 km were roughly an order of magnitude lower than typical values as reported with wire impactor measurements and as predicted by two global BC models. The impact of this discrepancy on estimates of direct radiative forcing of BC aerosol will also be discussed.

  13. Single particle characterization using a light scattering module coupled to a time-of-flight aerosol mass spectrometer

    SciTech Connect

    Cross, E.; Onasch, Timothy B.; Canagaratna, Manjula; Jayne, J. T.; Kimmel, Joel; Yu, Xiao-Ying; Alexander, M. L.; Worsnop, Douglas R.; Davidovits, Paul

    2009-10-01

    To accurately model the radiative forcing of aerosol particles, one must measure in real-time the size, shape, density, chemical composition, and mixing state of ambient particles. This is a formidable challenge because the chemical and physical properties of the aerosol particles are highly complex, dependent on the emission sources, the geography and meteorology of the surroundings, and the gas phase composition of the regional atmosphere.

  14. Gas-particle partitioning of primary organic aerosol emissions: 3. Biomass burning

    NASA Astrophysics Data System (ADS)

    May, Andrew A.; Levin, Ezra J. T.; Hennigan, Christopher J.; Riipinen, Ilona; Lee, Taehyoung; Collett, Jeffrey L.; Jimenez, Jose L.; Kreidenweis, Sonia M.; Robinson, Allen L.

    2013-10-01

    organic aerosol concentrations depend in part on the gas-particle partitioning of primary organic aerosol (POA) emissions. Consequently, heating and dilution were used to investigate the volatility of biomass-burning smoke particles from combustion of common North American trees/shrubs/grasses during the third Fire Lab at Missoula Experiment. Fifty to eighty percent of the mass of biomass-burning POA evaporated when isothermally diluted from plume- (~1000 µg m-3) to ambient-like concentrations (~10 µg m-3), while roughly 80% of the POA evaporated upon heating to 100°C in a thermodenuder with a residence time of ~14 sec. Therefore, the majority of the POA emissions were semivolatile. Thermodenuder measurements performed at three different residence times indicated that there were not substantial mass transfer limitations to evaporation (i.e., the mass accommodation coefficient appears to be between 0.1 and 1). An evaporation kinetics model was used to derive volatility distributions and enthalpies of vaporization from the thermodenuder data. A single volatility distribution can be used to represent the measured gas-particle partitioning from the entire set of experiments, including different fuels, organic aerosol concentrations, and thermodenuder residence times. This distribution, derived from the thermodenuder measurements, also predicts the dilution-driven changes in gas-particle partitioning. This volatility distribution and associated emission factors for each fuel studied can be used to update emission inventories and to simulate the gas-particle partitioning of biomass-burning POA emissions in chemical transport models.

  15. Aerosol-fluorescence spectrum analyzer: real-time measurement of emission spectra of airborne biological particles

    NASA Astrophysics Data System (ADS)

    Hill, Steven C.; Pinnick, Ronald G.; Nachman, Paul; Chen, Gang; Chang, Richard K.; Mayo, Michael W.; Fernandez, Gilbert L.

    1995-10-01

    We have assembled an aerosol-fluorescence spectrum analyzer (AFS), which can measure the fluorescence spectra and elastic scattering of airborne particles as they flow through a laser beam. The aerosols traverse a scattering cell where they are illuminated with intense (50 kW/cm 2) light inside the cavity of an argon-ion laser operating at 488 nm. This AFS can obtain fluorescence spectra of individual dye-doped polystyrene microspheres as small as 0.5 mu m in diameter. The spectra obtained from microspheres doped with pink and green-yellow dyes are clearly different. We have also detected the fluorescence spectra of airborne particles (although not single particles) made from various

  16. Evidence for the role of organics in aerosol particle formation under atmospheric conditions

    PubMed Central

    Metzger, Axel; Verheggen, Bart; Dommen, Josef; Duplissy, Jonathan; Prevot, Andre S. H.; Weingartner, Ernest; Riipinen, Ilona; Kulmala, Markku; Spracklen, Dominick V.; Carslaw, Kenneth S.; Baltensperger, Urs

    2010-01-01

    New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H2SO4 and organic condensable species. Nucleation occurs at H2SO4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H2SO4 and an organic molecule. This suggests that only one H2SO4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs. PMID:20133603

  17. Single-particle characterization of biomass burning organic aerosol (BBOA): evidence for non-uniform mixing of high molecular weight organics and potassium

    NASA Astrophysics Data System (ADS)

    Lee, Alex K. Y.; Willis, Megan D.; Healy, Robert M.; Wang, Jon M.; Jeong, Cheol-Heon; Wenger, John C.; Evans, Greg J.; Abbatt, Jonathan P. D.

    2016-05-01

    Biomass burning organic aerosol (BBOA) can be emitted from natural forest fires and human activities such as agricultural burning and domestic energy generation. BBOA is strongly associated with atmospheric brown carbon (BrC) that absorbs near-ultraviolet and visible light, resulting in significant impacts on regional visibility degradation and radiative forcing. The mixing state of BBOA can play a critical role in the prediction of aerosol optical properties. In this work, single-particle measurements from a Soot-Particle Aerosol Mass Spectrometer coupled with a light scattering module (LS-SP-AMS) were performed to examine the mixing state of BBOA, refractory black carbon (rBC), and potassium (K, a tracer for biomass burning aerosol) in an air mass influenced by wildfire emissions transported from northern Québec to Toronto, representing aged biomass burning plumes. Cluster analysis of single-particle measurements identified five BBOA-related particle types. rBC accounted for 3-14 wt % of these particle types on average. Only one particle type exhibited a strong ion signal for K+, with mass spectra characterized by low molecular weight organic species. The remaining four particle types were classified based on the apparent molecular weight of the BBOA constituents. Two particle types were associated with low potassium content and significant amounts of high molecular weight (HMW) organic compounds. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and illustrate that HMW BBOA can be a key contributor to low-volatility BrC observed in BBOA particles. The average mass absorption efficiency of low-volatility BBOA is about 0.8-1.1 m2 g-1 based on a theoretical closure calculation. Our estimates indicate that low-volatility BBOA contributes ˜ 33-44 % of thermo-processed particle absorption at 405 nm; and almost all of the BBOA absorption was associated with low-volatility organics.

  18. Origin and impact of particle-to-particle variations in composition measurements with the nano-aerosol mass spectrometer.

    PubMed

    Klems, Joseph P; Johnston, Murray V

    2013-09-01

    In the nano-aerosol mass spectrometer, individual particles in the 10-30 nm size range are trapped and irradiated with a high pulse energy laser beam. The laser pulse generates a plasma that disintegrates the particle into atomic ions, from which the elemental composition is determined. Particle-to-particle variations among the mass spectra are shown to arise from plasma energetics: Low ionization energy species are enhanced in some spectra while high ionization energy species are enhanced in others. These variations also limit the accuracy and precision of elemental analysis, with higher deviations generally observed when low ionization energy species are dominant in the mass spectrum. For standard datasets generated from nominally identical particles, it is shown that that the error associated with composition measurement is random and that averaging the spectra from a few tens of particles is sufficient for measuring the mole fractions of common elements to within about 10% of the expected value. Averaging a greater number of particles offers limited improvement of the measurement precision but has the deleterious effect of degrading the measurement time-resolution, which is given by the time needed to obtain the required number of particle spectra for averaging. An internally mixed ambient particle dataset was found to give a similar result to the standard datasets, that is, the measured elemental composition converged to the average value after a few tens of particles were averaged.

  19. Extractive Electrospray Ionization Mass Spectrometry of Heterogeneous Particles: Implications for Applications to Complex Atmospheric Aerosol

    NASA Astrophysics Data System (ADS)

    Longin, T.; Waring-Kidd, C.; Wingen, L. M.; Lyster, K.; Anderson, C.; Kumbhani, S.; Finlayson-Pitts, B. J.

    2015-12-01

    Extractive electrospray ionization mass spectrometry (EESI-MS) is a direct, real time technique for obtaining mass spectra of gases, liquid droplets, solid particles, and aerosols with little sample processing. EESI-MS involves the interaction of charged electrospray droplets with a separate spray containing the analyte of interest, but the exact mechanism by which the solvent droplets extract analyte from the sample is unclear. Possible mechanisms include complete coalescence of the sample particle with the solvent droplet in which all of the analyte is incorporated into the solvent or a more temporary interaction such that only some of the analyte is transferred to the solvent. Previous studies of the mechanism of EESI-MS on homogeneous particles indicate that both mechanisms are possible. We studied the behavior of EESI-MS toward heterogeneous particles created by coating NaCl particles with various thicknesses of organic diacids. Our results indicate that the signal strength depends on the solubility of the organic acid in the electrospray solvent, in agreement with previous studies, and also that the outer 10-15 nm of the particles are most susceptible to extraction into the electrospray droplets. Our results combined with those of previous studies suggest that the mass spectra obtained with EESI will not necessarily reflect the overall particle composition, especially for particles that are spatially inhomogeneous, and hence caution in interpretation of the data is advised for application to complex atmospheric aerosol.

  1. Effect of typhoon on atmospheric aerosol particle pollutants accumulation over Xiamen, China.

    PubMed

    Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Zhang, Miming

    2016-09-01

    Great influence of typhoon on air quality has been confirmed, however, rare data especially high time resolved aerosol particle data could be used to establish the behavior of typhoon on air pollution. A single particle aerosol spectrometer (SPAMS) was employed to characterize the particles with particle number count in high time resolution for two typhoons of Soulik (2013) and Soudelor (2015) with similar tracks. Three periods with five events were classified during the whole observation time, including pre - typhoon (event 1 and event 2), typhoon (event 3 and event 4) and post - typhoon (event 5) based on the meteorological parameters and particle pollutant properties. First pollutant group appeared during pre-typhoon (event 2) with high relative contributions of V - Ni rich particles. Pollution from the ship emissions and accumulated by local processes with stagnant meteorological atmosphere dominated the formation of the pollutant group before typhoon. The second pollutant group was present during typhoon (event 3), while typhoon began to change the local wind direction and increase wind speed. Particle number count reached up to the maximum value. High relative contributions of V - Ni rich and dust particles with low value of NO3(-)/SO4(2-) was observed during this period, indicating that the pollutant group was governed by the combined effect of local pollutant emissions and long-term transports. The analysis of this study sheds a deep insight into understand the relationship between the air pollution and typhoon. PMID:27295441

  2. Fine and ultrafine TiO2 particles in aerosol in Kraków (Poland)

    NASA Astrophysics Data System (ADS)

    Wilczyńska-Michalik, Wanda; Rzeźnikiewicz, Kamil; Pietras, Bartłomiej; Michalik, Marek

    2014-12-01

    During single particle analysis of aerosol in Kraków (Poland) we noticed a new component, that is, aggregates of TiO2 particles. These aggregates are from 0.5 to 4 μm and are composed of individual particles whose size typically varies from between 100 and 350 nm. Smaller particles (below 100 nm) also occur. TiO2 particles are relatively abundant in the summer. The size distribution of the particles corresponds to "pigmentary" TiO2, which indicates that they could be derived from paints and building materials. TiO2 particles were not previously identified in aerosol samples in Kraków, and therefore this phenomenon is likely to be related to the common usage of new building materials and paints. A review of the literature suggests that TiO2 particles, especially within the nanosize range, could result in health and environmental impacts; however, evaluation of the actual threat is difficult.

  3. Real time analysis of lead-containing atmospheric particles in Beijing during springtime by single particle aerosol mass spectrometry.

    PubMed

    Ma, Li; Li, Mei; Huang, Zhengxu; Li, Lei; Gao, Wei; Nian, Huiqing; Zou, Lilin; Fu, Zhong; Gao, Jian; Chai, Fahe; Zhou, Zhen

    2016-07-01

    Using a single particle aerosol mass spectrometer (SPAMS), the chemical composition and size distributions of lead (Pb)-containing particles with diameter from 0.1 μm to 2.0 μm in Beijing were analyzed in the spring of 2011 during clear, hazy, and dusty days. Based on mass spectral features of particles, cluster analysis was applied to Pb-containing particles, and six major classes were acquired consisting of K-rich, carboneous, Fe-rich, dust, Pb-rich, and Cl-rich particles. Pb-containing particles accounted for 4.2-5.3%, 21.8-22.7%, and 3.2% of total particle number during clear, hazy and dusty days, respectively. K-rich particles are a major contribution to Pb-containing particles, varying from 30.8% to 82.1% of total number of Pb-containing particles, lowest during dusty days and highest during hazy days. The results reflect that the chemical composition and amount of Pb-containing particles has been affected by meteorological conditions as well as the emissions of natural and anthropogenic sources. K-rich particles and carbonaceous particles could be mainly assigned to the emissions of coal combustion. Other classes of Pb-containing particles may be associated with metallurgical processes, coal combustion, dust, and waste incineration etc. In addition, Pb-containing particles during dusty days were first time studied by SPAMS. This method could provide a powerful tool for monitoring and controlling of Pb pollution in real time.

  4. The influence of small aerosol particles on the properties of water and ice clouds.

    PubMed

    Choularton, T W; Bower, K N; Weingartner, E; Crawford, I; Coe, H; Gallagher, M W; Flynn, M; Crosier, J; Connolly, P; Targino, A; Alfarra, M R; Baltensperger, U; Sjogren, S; Verheggen, B; Cozic, J; Gysel, M

    2008-01-01

    In this paper, results are presented of the influence of small organic- and soot-containing particles on the formation of water and ice clouds. There is strong evidence that these particles have grown from nano particle seeds produced by the combustion of oil products. Two series of field experiments are selected to represent the observations made. The first is the CLoud-Aerosol Characterisation Experiment (CLACE) series of experiments performed at a high Alpine site (Jungfraujoch), where cloud was in contact with the ground and the measuring station. Both water and ice clouds were examined at different times of the year. The second series of experiments is the CLOud Processing of regional Air Pollution advecting over land and sea (CLOPAP) series, where ageing pollution aerosol from UK cities was observed, from an airborne platform, to interact with warm stratocumulus cloud in a cloud-capped atmospheric boundary layer. Combining the results it is shown that aged pollution aerosol consists of an internal mixture of organics, sulfate, nitrate and ammonium, the organic component is dominated by highly oxidized secondary material. The relative contributions and absolute loadings of the components vary with location and season. However, these aerosols act as Cloud Condensation Nuclei (CCN) and much of the organic material, along with the other species, is incorporated into cloud droplets. In ice and mixed phase cloud, it is observed that very sharp transitions (extending over just a few metres) are present between highly glaciated regions and regions consisting of supercooled water. This is a unique finding; however, aircraft observations in cumulus suggest that this kind of structure may be found in these cloud types too. It is suggested that this sharp transition is caused by ice nucleation initiated by oxidised organic aerosol coated with sulfate in more polluted regions of cloud, sometimes enhanced by secondary ice particle production in these regions.

  5. Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

    PubMed

    Canagaratna, Manjula R; Massoli, Paola; Browne, Eleanor C; Franklin, Jonathan P; Wilson, Kevin R; Onasch, Timothy B; Kirchstetter, Thomas W; Fortner, Edward C; Kolb, Charles E; Jayne, John T; Kroll, Jesse H; Worsnop, Douglas R

    2015-05-14

    Black carbon is an important constituent of atmospheric aerosol particle matter (PM) with significant effects on the global radiation budget and on human health. The soot particle aerosol mass spectrometer (SP-AMS) has been developed and deployed for real-time ambient measurements of refractory carbon particles. In the SP-AMS, black carbon or metallic particles are vaporized through absorption of 1064 nm light from a CW Nd:YAG laser. This scheme allows for continuous "soft" vaporization of both core and coating materials. The main focus of this work is to characterize the extent to which this vaporization scheme provides enhanced chemical composition information about aerosol particles. This information is difficult to extract from standard SP-AMS mass spectra because they are complicated by extensive fragmentation from the harsh 70 eV EI ionization scheme that is typically used in these instruments. Thus, in this work synchotron-generated vacuum ultraviolet (VUV) light in the 8-14 eV range is used to measure VUV-SP-AMS spectra with minimal fragmentation. VUV-SP-AMS spectra of commercially available carbon black, fullerene black, and laboratory generated flame soots were obtained. Small carbon cluster cations (C(+)-C5(+)) were found to dominate the VUV-SP-AMS spectra of all the samples, indicating that the corresponding neutral clusters are key products of the SP vaporization process. Intercomparisons of carbon cluster ratios observed in VUV-SP-AMS and SP-AMS spectra are used to confirm spectral features that could be used to distinguish between different types of refractory carbon particles. VUV-SP-AMS spectra of oxidized organic species adsorbed on absorbing cores are also examined and found to display less thermally induced decomposition and fragmentation than spectra obtained with thermal vaporization at 200 °C (the minimum temperature needed to quantitatively vaporize ambient oxidized organic aerosol with a continuously heated surface). The particle cores

  6. Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

    PubMed

    Canagaratna, Ma