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Sample records for aerosol particle chemical

  1. Measurement of mass distribution of chemical species in aerosol particles

    NASA Technical Reports Server (NTRS)

    Sinha, M. P.; Friedlander, S. K.

    1984-01-01

    Aerosols may be generated through the nebulizing of solutions and the evaporation of their solvent, leaving the dry solute particles. Attention is presently given to a method for the direct determination of the masses of chemical species in individual aerosol particles on a continuous, real-time basis, using mass spectrometry. After the aerosol particles are introduced into the ion source of a quadrupole mass spectrometer, the particles impinge on a hot rhenium filament in the mass spectrometer's ion source. The resulting vapor plume is ionized by electron bombardment, and a pulse of ions is generated by each particle. The intensities of different masses in the ion pulses can then be measured by the mass spectrometer.

  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 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

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

    PubMed

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

    2011-07-05

    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.

  5. 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.

  6. 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

  7. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

    NASA Astrophysics Data System (ADS)

    Asmi, E.; Frey, A.; Virkkula, A.; Ehn, M.; Manninen, H. E.; Timonen, H.; Tolonen-Kivimäki, O.; Aurela, M.; Hillamo, R.; Kulmala, M.

    2009-12-01

    The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm) and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

  8. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

    NASA Astrophysics Data System (ADS)

    Asmi, E.; Frey, A.; Virkkula, A.; Ehn, M.; Manninen, H. E.; Timonen, H.; Tolonen-Kivimäki, O.; Aurela, M.; Hillamo, R.; Kulmala, M.

    2010-05-01

    The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm) and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

  9. Atmospheric Black Carbon: Chemical Bonding and Structural Information of Individual Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Gilles, M. K.; Tivanski, A. V.; Hopkins, R. J.; Marten, B. D.

    2006-12-01

    The formation of aerosols from both natural and anthropogenic sources affects the Earth's temperature and climate by altering the radiative properties of the atmosphere. Aerosols containing black carbon (BC) that are released into the atmosphere from the burning of biomass, natural fires and the combustion of coals, diesel and jet fuels, contribute a large positive component to this radiative forcing, thus causing a heating of the atmosphere. A distinct type of biomass burn aerosol referred to as "tar balls" has recently been reported in the literature and is characterized by a spherical morphology, high carbon content and ability to efficiently scatter and absorb light. At present, very little is known about the exact nature and variation of the range of BC aerosols in the atmosphere with regards to optical, chemical and physical properties. Additionally, the similarity of these aerosols to surrogates used in the laboratory as atmospheric mimics remains unclear. The local chemical bonding, structural ordering and carbon-to-oxygen ratios of a plethora of black carbon standard reference materials (BC SRMs), high molecular mass humic-like substances (HULIS) and atmospheric aerosols from a variety of sources are examined using scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure (NEXAFS) spectroscopy. STXM/NEXAFS enables single aerosol particles of diameter upwards of 100 nm to be studied, which allows the diversity of atmospheric aerosol collected during a variety of field missions to be assessed. We apply a semi-quantitative peak fitting method to the recorded NEXAFS spectral fingerprints allowing comparison of BC SRMs and HULIS to BC aerosol originating from anthropogenic combustion and biomass burning events. This method allows us to distinguish between anthropogenic combustion and biomass burn aerosol using both chemical bonding and structural ordering information. The STXM/NEXAFS technique has also been utilized to

  10. Real-time characterization of the size and chemical composition of individual particles in ambient aerosol systems in Riverside, California

    SciTech Connect

    Noble, C.A.; Prather, K.A.

    1995-12-31

    Atmospheric aerosols, although ubiquitous, are highly diverse and continually fluctuating systems. A typical aerosol system may consist of particles with diameters between {approximately}0.002 {mu}m and {approximately}200 {mu}m. Even in rural or pristine areas, atmospheric particle concentration is significant, with concentrations up to 10{sup 8} particles/cm{sup 3} not being uncommon. Chemical composition of atmospheric particles vary from simple water droplets or acidic ices to soot particles and cigarette smoke. Due to changes in atmospheric conditions, processes such as nucleation, coagulation or heterogeneous chemistry may effect both physical and chemical properties of individual particles over relatively short time intervals. Recently, aerosol measurement techniques are focusing on determining the size and/or chemical composition of individual aerosol particles. This research group has recently developed aerosol time-of-flight mass spectrometry (ATOFMS), a technique which allows for real-time determination of the size and chemical composition of individual aerosol particles. Single particle measurements are performed in one instrument using dual laser aerodynamic particle sizing and time-of-flight mass spectrometry. Aerosol-time-of-flight mass spectrometry is briefly described in several other abstracts in this publication.

  11. Chemical Analysis of Individual Aerosols Particles by Electron Energy-Loss Spectroscopy (EELS)

    NASA Astrophysics Data System (ADS)

    Buseck, P. R.; Buseck, P. R.; Garvie, L. A.; Li, J.; Posfai, M.

    2001-12-01

    We use electron energy-loss spectroscopy (EELS) with a transmission electron microscope (TEM) to obtain chemical and bonding information on individual aerosol particles. EELS is ideally suited to this task because of its high spatial resolution and sensitivity to light elements such as C, N, and O. In addition, the spectral shapes provide information regarding bonding, atomic coordination and, for polyvalent elements, oxidation states. Our current focus is on carbonaceous aerosols both in the ambient air and emissions from biomass burning, with emphasis on the heterogeneous chemistry, particle structure, and chemical composition of soot particles. From the EELS spectra we were able to record for the first time, differences in composition between individual spherules within the same soot aggregate. We also found evidence of chemical variations even within individual soot spheres as small as 50 nm across. In the case of biomass burning, the most striking chemical differences are in the quantity of K, minor O and, in places, N. The quantity of elements associated with C decreases with the degree of graphitization of the soot spheres, as shown by the shapes of the C spectra and was corroborated by high-resolution TEM images of the analyzed particles. Knowledge of the degree of graphitization and quantity of associated elements is important for understanding and modeling their optical properties and in some case in source attributions.

  12. Chemical boundary conditions for the classification of aerosol particles using computer controlled electron probe microanalysis.

    PubMed

    Anaf, Willemien; Horemans, Benjamin; Van Grieken, René; De Wael, Karolien

    2012-11-15

    A method for the classification of individual aerosol particles using computer controlled electron probe microanalysis is presented. It is based on chemical boundary conditions (CBC) and enables quick and easy processing of a large set of elemental concentration data (mass%), derived from the X-ray spectra of individual particles. The particles are first classified into five major classes (sea salt related, secondary inorganic, minerals, iron-rich and carbonaceous), after which advanced data mining can be performed by examining the elemental composition of particles within each class into more detail (e.g., by ternary diagrams). The CBC method is validated and evaluated by comparing its results with the output obtained with hierarchical cluster analysis (HCA) for well-known standard particles as well as real aerosol particles collected with a cascade impactor. The CBC method gives reliable results and has a major advantage compared to HCA. CBC is based on boundary conditions that are derived from chemical logical thinking and does not require a translation of a mathematical algorithm output as does HCA. Therefore, the CBC method is more objective and enables comparison between samples without intermediate steps.

  13. Chemical characterization of submicron aerosol particles during wintertime in a northwest city of China using an Aerodyne aerosol mass spectrometry.

    PubMed

    Zhang, Xinghua; Zhang, Yangmei; Sun, Junying; Yu, Yangchun; Canonaco, Francesco; Prévôt, Andre S H; Li, Gang

    2017-03-01

    An Aerodyne quadrupole aerosol mass spectrometry (Q-AMS) was utilized to measure the size-resolved chemical composition of non-refractory submicron particles (NR-PM1) from October 27 to December 3, 2014 at an urban site in Lanzhou, northwest China. The average NR-PM1 mass concentration was 37.3 μg m(-3) (ranging from 2.9 to 128.2 μg m(-3)) under an AMS collection efficiency of unity and was composed of organics (48.4%), sulfate (17.8%), nitrate (14.6%), ammonium (13.7%), and chloride (5.7%). Positive matrix factorization (PMF) with the multi-linear engine (ME-2) solver identified six organic aerosol (OA) factors, including hydrocarbon-like OA (HOA), coal combustion OA (CCOA), cooking-related OA (COA), biomass burning OA (BBOA) and two oxygenated OA (OOA1 and OOA2), which accounted for 8.5%, 20.2%, 18.6%, 12.4%, 17.8% and 22.5% of the total organics mass on average, respectively. Primary emissions were the major sources of fine particulate matter (PM) and played an important role in causing high chemically resolved PM pollution during wintertime in Lanzhou. Back trajectory analysis indicated that the long-range regional transport air mass from the westerly was the key factor that led to severe submicron aerosol pollution during wintertime in Lanzhou.

  14. Long-term Chemical Characterization of Submicron Aerosol Particles in the Amazon Forest - ATTO Station

    NASA Astrophysics Data System (ADS)

    Carbone, S.; Brito, J.; Rizzo, L. V.; Holanda, B. A.; Cirino, G. G.; Saturno, J.; Krüger, M. L.; Pöhlker, C.; Ng, N. L.; Xu, L.; Andreae, M. O.; Artaxo, P.

    2015-12-01

    The study of the chemical composition of aerosol particles in the Amazon forest represents a step forward to understand the strong coupling between the atmosphere and the forest. For this reason submicron aerosol particles were investigated in the Amazon forest, where biogenic and anthropogenic aerosol particles coexist at the different seasons (wet/dry). The measurements were performed at the ATTO station, which is located about 150 km northeast of Manaus. At ATTO station the Aerosol chemical speciation monitor (ACSM, Aerodyne) and the Multiangle absorption photometer (MAAP, Thermo 5012) have been operated continuously from March 2014 to July 2015. In this study, long-term measurements (near-real-time, ~30 minutes) of PM1 chemical composition were investigated for the first time in this environment.The wet season presented lower concentrations than the dry season (~5 times). In terms of chemical composition, both seasons were dominated by organics (75 and 63%) followed by sulfate (11 and 13%). Nitrate presented different ratio values between the mass-to-charges 30 to 46 (main nitrate fragments) suggesting the presence of nitrate as inorganic and organic nitrate during both seasons. The results indicated that about 75% of the nitrate signal was from organic nitrate during the dry season. In addition, several episodes with elevated amount of chloride, likely in the form of sea-salt from the Atlantic Ocean, were observed during the wet season. During those episodes, chloride comprised up to 7% of the PM1. During the dry season, chloride was also observed; however, with different volatility, which suggested that Chloride was present in different form and source. Moreover, the constant presence of sulfate and BC during the wet season might be related to biomass burning emissions from Africa. BC concentration was 2.5 times higher during the dry season. Further characterization of the organic fraction was accomplished with the positive matrix factorization (PMF), which

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

  16. Single-particle aerosol mass spectrometry for the detection and identification of chemical warfare agent simulants.

    PubMed

    Martin, Audrey N; Farquar, George R; Frank, Matthias; Gard, Eric E; Fergenson, David P

    2007-08-15

    Single-particle aerosol mass spectrometry (SPAMS) was used for the real-time detection of liquid nerve agent simulants. A total of 1000 dual-polarity time-of-flight mass spectra were obtained for micrometer-sized single particles each of dimethyl methyl phosphonate, diethyl ethyl phosphonate, diethyl phosphoramidate, and diethyl phthalate using laser fluences between 0.58 and 7.83 nJ/microm2, and mass spectral variation with laser fluence was studied. The mass spectra obtained allowed identification of single particles of the chemical warfare agent (CWA) simulants at each laser fluence used although lower laser fluences allowed more facile identification. SPAMS is presented as a promising real-time detection system for the presence of CWAs.

  17. 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

  18. Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign

    SciTech Connect

    Lee, Y. -N.; Springston, S.; Jayne, J.; Wang, J.; Hubbe, J.; Senum, G.; Kleinman, L.; Daum, P. H.

    2014-01-01

    The chemical composition of aerosol particles (Dp ≤ 1.5 μm) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO42−, followed by Na+, Cl, Org (total organics), NH4+, and NO3, in decreasing order of importance; CH3SO3 (MSA), Ca2+, and K+ rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH4+ to SO42− equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl deficits caused by both HNO3 and H2SO4, but for the most part were externally mixed with particles, mainly SO42−. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH3 is present between 72° W and 76° W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31° S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol

  19. Chemical aerosol Raman detector

    NASA Astrophysics Data System (ADS)

    Aggarwal, R. L.; Farrar, L. W.; Di Cecca, S.; Amin, M.; Perkins, B. G.; Clark, M. L.; Jeys, T. H.; Sickenberger, D. W.; D'Amico, F. M.; Emmons, E. D.; Christesen, S. D.; Kreis, R. J.; Kilper, G. K.

    2017-03-01

    A sensitive chemical aerosol Raman detector (CARD) has been developed for the trace detection and identification of chemical particles in the ambient atmosphere. CARD includes an improved aerosol concentrator with a concentration factor of about 40 and a CCD camera for improved detection sensitivity. Aerosolized isovanillin, which is relatively safe, has been used to characterize the performance of the CARD. The limit of detection (SNR = 10) for isovanillin in 15 s has been determined to be 1.6 pg/cm3, which corresponds to 6.3 × 109 molecules/cm3 or 0.26 ppb. While less sensitive, CARD can also detect gases. This paper provides a more detailed description of the CARD hardware and detection algorithm than has previously been published.

  20. 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

  1. 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

  2. Chemical composition and sources of aerosol particles at Zeppelin Mountain (Ny Ålesund, Svalbard): An electron microscopy study

    NASA Astrophysics Data System (ADS)

    Weinbruch, Stephan; Wiesemann, David; Ebert, Martin; Schütze, Katharina; Kallenborn, Roland; Ström, Johan

    2012-03-01

    Aerosol particles were collected at the Zeppelin Mountain Atmospheric Research Station (474 m asl) near Ny Ålesund (Svalbard, Norway) on 27 different days between July 2007 and December 2008. The size, morphology and chemical composition of 57,617 individual particles were studied by high-resolution scanning electron microscopy and energy-dispersive X-ray microanalysis. Based on chemical composition, morphology, mixing state and stability under electron bombardment, the particles were assigned to one of the following groups: sea salt, aged sea salt, Ca sulphates, Na sulphates, carbonates, soot, silicates, fly ashes, secondary aerosol, secondary aerosol plus sodium, secondary aerosol plus soot, mixed particles and others. Sea salt, aged sea salt, silicates and mixed particles (mixtures of sea salt, silicates and Ca sulphates) are the most abundant groups for particles with aerodynamic diameters > 0.5 μm, secondary aerosol, mixed particles and secondary aerosol with soot inclusions below 0.5 μm. Silicate fly ashes (major source coal burning) and metal fly ashes (from metallurgical high temperature processes) occur only at very low number concentrations. In contrast to previous work, the fly ash abundance is not correlated with air masses that crossed industrialized regions in Central and Eastern Europe, Scandinavia or Russia. These observations indicate a significant reduction of long-range transport of heavy metals to Svalbard. Soot (external and internally mixed with secondary aerosol) shows a pronounced seasonal pattern with a much lower abundance during summer compared to spring, autumn and winter. The soot abundance is not correlated with the air mass back-trajectories. During summer (July and August), soot was only observed when cruise ships were present in the area around Ny Ålesund (Kongsfjorden). Pronounced seasonal patterns were observed for the abundance of the mineral dust component which is generally lower in summer compared to the other seasons. The

  3. The real part of the refractive indices and effective densities for chemically segregated ambient aerosols in Guangzhou by a single particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Zhang, G.; Bi, X.; Qiu, N.; Han, B.; Lin, Q.; Peng, L.; Chen, D.; Wang, X.; Peng, P.; Sheng, G.; Zhou, Z.

    2015-12-01

    Microphysical properties of atmospheric aerosols are essential to better evaluate their radiative forcing. This paper first presents an estimate of the real part of the refractive indices (n) and effective densities (ρeff) of chemically segregated atmospheric aerosols in China. Vacuum aerodynamic diameter, chemical compositions, and light scattering intensities of individual particles were simultaneously measured by a single particle aerosol mass spectrometer (SPAMS) during fall of 2012 in Guangzhou. On the basis of Mie theory, n and ρeff were estimated for 17 particle types in four categories: organics (OC), elemental carbon (EC), internally mixed EC and OC (ECOC), and metal rich, respectively. Results indicate the presence of spherical or nearly spherical shape for majority of particle types, whose partial scattering cross section vs. sizes were well fitted to Mie theoretical modeling results. While sharing n in a narrow range (1.47-1.53), majority of particle types exhibited a wide range of ρeff (0.87-1.51 g cm-3). OC group is associated with the lowest ρeff (0.87-1.07 g cm-3), while metal rich group with the highest ones (1.29-1.51 g cm-3). It is noteworthy that a specific EC type exhibits a complex scattering curve vs. size due to the presence of both compact and irregularly shape particles. Overall, the results on detailed relationship between physical and chemical properties benefits future researches on the impact of aerosols on visibility and climate.

  4. New approaches for the chemical and physical characterization of aerosols using a single particle mass spectrometry based technique

    NASA Astrophysics Data System (ADS)

    Spencer, Matthew Todd

    Aerosols affect the lives of people every day. They can decrease visibility, alter cloud formation and cloud lifetimes, change the energy balance of the earth and are implicated in causing numerous health problems. Measuring the physical and chemical properties of aerosols is essential to understand and mitigate any negative impacts that aerosols might have on climate and human health. Aerosol time-of-flight mass spectrometry (ATOFMS) is a technique that measures the size and chemical composition of individual particles in real time. The goal of this dissertation is to develop new and useful approaches for measuring the physical and/or chemical properties of particles using ATOFMS. This has been accomplished using laboratory experiments, ambient field measurements and sometimes comparisons between them. A comparison of mass spectra generated from petrochemical particles was made to light duty vehicle (LDV) and heavy duty diesel vehicle (HDDV) particle mass spectra. This comparison has given us new insight into how to differentiate between particles from these two sources. A method for coating elemental carbon (EC) particles with organic carbon (OC) was used to generate a calibration curve for quantifying the fraction of organic carbon and elemental carbon on particles using ATOFMS. This work demonstrates that it is possible to obtain quantitative chemical information with regards to EC and OC using ATOFMS. The relationship between electrical mobility diameter and aerodynamic diameter is used to develop a tandem differential mobility analyzer-ATOFMS technique to measure the effective density, size and chemical composition of particles. The method is applied in the field and gives new insight into the physical/chemical properties of particles. The size resolved chemical composition of aerosols was measured in the Indian Ocean during the monsoonal transition period. This field work shows that a significant fraction of aerosol transported from India was from biomass

  5. 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

  6. 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

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

    DOE PAGES

    Thalman, R.; Thalman, R.; Wang, J.; ...

    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

  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.; ...

    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

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

    SciTech Connect

    Thalman, R.; 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 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

  10. 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).

  11. Combined use of optical and electron microscopic techniques for the measurement of hygroscopic property, chemical composition, and morphology of individual aerosol particles.

    PubMed

    Ahn, Kang-Ho; Kim, Sun-Man; Jung, Hae-Jin; Lee, Mi-Jung; Eom, Hyo-Jin; Maskey, Shila; Ro, Chul-Un

    2010-10-01

    In this work, an analytical method for the characterization of the hygroscopic property, chemical composition, and morphology of individual aerosol particles is introduced. The method, which is based on the combined use of optical and electron microscopic techniques, is simple and easy to apply. An optical microscopic technique was used to perform the visual observation of the phase transformation and hygroscopic growth of aerosol particles on a single particle level. A quantitative energy-dispersive electron probe X-ray microanalysis, named low-Z particle EPMA, was used to perform a quantitative chemical speciation of the same individual particles after the measurement of the hygroscopic property. To validate the analytical methodology, the hygroscopic properties of artificially generated NaCl, KCl, (NH(4))(2)SO(4), and Na(2)SO(4) aerosol particles of micrometer size were investigated. The practical applicability of the analytical method for studying the hygroscopic property, chemical composition, and morphology of ambient aerosol particles is demonstrated.

  12. The real part of the refractive indices and effective densities for chemically segregated ambient aerosols in Guangzhou measured by a single-particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Zhang, Guohua; Bi, Xinhui; Qiu, Ning; Han, Bingxue; Lin, Qinhao; Peng, Long; Chen, Duohong; Wang, Xinming; Peng, Ping'an; Sheng, Guoying; Zhou, Zhen

    2016-03-01

    Knowledge on the microphysical properties of atmospheric aerosols is essential to better evaluate their radiative forcing. This paper presents an estimate of the real part of the refractive indices (n) and effective densities (ρeff) of chemically segregated atmospheric aerosols in Guangzhou, China. Vacuum aerodynamic diameter, chemical compositions, and light-scattering intensities of individual particles were simultaneously measured by a single-particle aerosol mass spectrometer (SPAMS) during the fall of 2012. On the basis of Mie theory, n at a wavelength of 532 nm and ρeff were estimated for 17 particle types in four categories: organics (OC), elemental carbon (EC), internally mixed EC and OC (ECOC), and Metal-rich. The results indicate the presence of spherical or nearly spherical shapes for the majority of particle types, whose partial scattering cross-section versus sizes were well fitted to Mie theoretical modeling results. While sharing n in a narrow range (1.47-1.53), majority of particle types exhibited a wide range of ρeff (0.87-1.51 g cm-3). The OC group is associated with the lowest ρeff (0.87-1.07 g cm-3), and the Metal-rich group with the highest ones (1.29-1.51 g cm-3). It is noteworthy that a specific EC type exhibits a complex scattering curve versus size due to the presence of both compact and irregularly shaped particles. Overall, the results on the detailed relationship between physical and chemical properties benefits future research on the impact of aerosols on visibility and climate.

  13. Properties and sources of individual particles and some chemical species in the aerosol of a metropolitan underground railway station

    NASA Astrophysics Data System (ADS)

    Salma, Imre; Pósfai, Mihály; Kovács, Kristóf; Kuzmann, Ernő; Homonnay, Zoltán; Posta, József

    Aerosol samples in PM 10-2.0 and PM 2.0 size fractions were collected on the platform of a metropolitan underground railway station in central Budapest. Individual aerosol particles were studied using atomic force microscopy, scanning electron microscopy and transmission electron microscopy with energy-dispersive X-ray spectrometry and electron diffraction. The bulk aerosol samples were investigated by 57Fe Mössbauer spectroscopy, and they were subjected to chemical speciation analysis for Cr. The particles were classified into groups of iron oxides and iron, carbonates, silicates, quartz and carbonaceous debris. Electron micrographs showed that the Fe-rich particles in the PM 2.0 size fraction typically consisted of aggregates of nano-sized hematite crystals that were randomly oriented, had round shapes and diameters of 5-15 nm. In addition to hematite, a minor fraction of the iron oxide particles also contained magnetite. In addition, the PM 2.0-fraction particles typically had a rugged surface with layered or granular morphologies. Mössbauer spectroscopy suggested that hematite was a major Fe-bearing species in the PM 10-2.0 size fraction; its mass contribution to the Fe was 36%. Further constituents (ferrite, carbides and FeOOH) were also identified. The water soluble amounts of Cr for the underground railway station and city center were similar. In the PM 10-2.0 size fraction, practically all dissolved Cr had an oxidation state of three, which corresponds to ambient conditions. In the PM 2.0 size fraction, however, approximately 7% of the dissolved Cr was present as Cr(VI), which was different from that for the urban aerosol. It is suggested that the increased adverse health effects of aerosol particles in metros with respect to ambient outdoor particles is linked to the differences in the oxidation states, surface properties or morphologies.

  14. Chemical Imaging of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

    SciTech Connect

    O'Brien, Rachel; Wang, Bingbing; Laskin, Alexander; Riemer, Nicole; West, Matthew; Zhang, Qi; Sun, Yele; Yu, Xiao-Ying; Alpert, Peter A.; Knopf, Daniel A.; Gilles, Mary K.; Moffet, Ryan

    2015-09-28

    A new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission x-ray microscopy/near edge x-ray absorption fine structure (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on June 27th and 28th during the 2010 Carbonaceous Aerosols and Radiative Effects (CARES) study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. Both microscopy imaging techniques showed more changes over these two days in the mixing state at the T0 site than at the T1 site. The STXM data showed evidence of changes in the mixing state associated with a build-up of organic matter confirmed by collocated measurements and the largest impact on the mixing state was due to an increase in soot dominant particles during this build-up. The CCSEM/EDX analysis showed the presence of two types of particle populations; the first was dominated by aged sea salt particles and had a higher mixing state index (indicating a more homogeneous population), the second was dominated by carbonaceous particles and had a lower mixing state index.

  15. Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

    DOE PAGES

    O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; ...

    2015-08-26

    In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near themore » Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.« less

  16. Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization

    SciTech Connect

    O'Brien, Rachel E.; Wang, Bingbing; Laskin, Alexander; Riemer, Nicole; West, Matthew; Zhang, Qi; Sun, Yele; Yu, Xiao -Ying; Alpert, Peter; Knopf, Daniel A.; Gilles, Mary K.; Moffet, Ryan C.

    2015-08-26

    In this study, a new parameterization for quantifying the mixing state of aerosol populations has been applied for the first time to samples of ambient particles analyzed using spectro-microscopy techniques. Scanning transmission X-ray microscopy/near edge X-ray absorption fine structure (STXM/NEXAFS) and computer-controlled scanning electron microscopy/energy dispersive X-ray spectroscopy (CCSEM/EDX) were used to probe the composition of the organic and inorganic fraction of individual particles collected on 27 and 28 June during the 2010 Carbonaceous Aerosols and Radiative Effects study in the Central Valley, California. The first field site, T0, was located in downtown Sacramento, while T1 was located near the Sierra Nevada Mountains. Mass estimates of the aerosol particle components were used to calculate mixing state metrics, such as the particle-specific diversity, bulk population diversity, and mixing state index, for each sample. The STXM data showed evidence of changes in the mixing state associated with a buildup of organic matter confirmed by collocated measurements, and the largest impact on the mixing state was due to an increase in soot dominant particles during this buildup. The mixing state from STXM was similar between T0 and T1, indicating that the increased organic fraction at T1 had a small effect on the mixing state of the population. The CCSEM/EDX analysis showed the presence of two types of particle populations: the first was dominated by aged sea-salt particles and had a higher mixing state index (indicating a more homogeneous population); the second was dominated by carbonaceous particles and had a lower mixing state index.

  17. Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds

    NASA Astrophysics Data System (ADS)

    Ebert, Martin; Weigel, Ralf; Kandler, Konrad; Günther, Gebhard; Molleker, Sergej; Grooß, Jens-Uwe; Vogel, Bärbel; Weinbruch, Stephan; Borrmann, Stephan

    2016-07-01

    Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed at a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSCs). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. In total 116 small silicate, Fe-rich, Pb-rich and aluminum oxide spheres were found. In contrast to ESSenCe in early winter, during the late-winter RECONCILE mission the air masses were subsiding inside the Arctic winter vortex from the upper stratosphere and mesosphere, thus initializing a transport of refractory aerosol particles into the lower stratosphere. During RECONCILE, 759 refractory particles with diameters above 500 nm were found consisting of silicates, silicate / carbon mixtures, Fe-rich particles, Ca-rich particles and complex metal mixtures. In the size range below 500 nm the presence of soot was also proven. While the data base is still sparse, the general tendency of a lower abundance of refractory particles during PSC events compared to non-PSC situations was observed. The detection of large refractory particles in the stratosphere, as well as the experimental finding that these particles were not observed in the particle samples (upper size limit ˜ 5 µm) taken during PSC events, strengthens the hypothesis that such particles are present in the lower polar stratosphere in late winter and have provided a surface for heterogeneous nucleation during PSC formation.

  18. 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

  19. The Microphysical and Chemical properties of aerosol particles from the United Arab Emirates Unified Aerosol Experiment (UAE2) and from the Bodele-BODEX Experiment

    NASA Astrophysics Data System (ADS)

    Martins, J.; Chaudhry, Z.; Todd, M.; Kaufman, Y.; Artaxo, P.

    2005-12-01

    Aerosol filters collected during the UAE2 experiment (August 2004), and during the BODEX experiment (in the Bodele region, February 2005) were analyzed for spectral absorption properties (from 350-2500nm), mass concentration (fine and coarse modes), electron microscopy, and chemical composition. The UAE2 samples show evidence of absorption by dust and urban pollution particles. In the fine mode, the urban pollution particles show spectral dependence inversely proportional to the wavelength, which is compatible with small black carbon aerosols. The coarse mode shows evidences of the internal mixture between dust and pollution, producing the typical strong absorption in UV-Visible wavelengths produced by dust, as well as significant absorption in the NIR (near infrared) coming from the dust-pollution combination. On the other hand, the Bodele samples show at least two types of dust absorption behavior: 1 - very strong absorption efficiency in the UV and visible wavelengths with nearly no absorption in the NIR; 2 - very strong absorption efficiency in the UV-VIS region with significant absorption in the NIR. Additional samples collected in the Amazon region, in Brazil, show evidence of long-range transport of dust from the Sahara. The chemical composition and microphysical properties of the Amazon Samples are compared with those measured in the UAE and Bodele regions. The chemical composition of these samples provides additional insight on previous theories of the fertilization of the Amazon by long-range transport of dust from the Sahara region.

  20. Chemical and physical characteristics of aerosol particles at a remote coastal location, Mace Head, Ireland, during NAMBLEX

    NASA Astrophysics Data System (ADS)

    Coe, H.; Allan, J. D.; Alfarra, M. R.; Bower, K. N.; Flynn, M. J.; McFiggans, G. B.; Topping, D. O.; Williams, P. I.; O'Dowd, C. D.; Dall'Osto, M.; Beddows, D. C. S.; Harrison, R. M.

    2006-08-01

    A suite of aerosol physical and chemical measurements were made at the Mace Head Atmospheric Research Station, Co. Galway, Ireland, a coastal site on the eastern seaboard of the north Atlantic Ocean during NAMBLEX. The data have been used in this paper to show that over a wide range of aerosol sizes there is no impact of the inter-tidal zone or the surf zone on measurements made at 7 m above ground level or higher. During the measurement period a range of air mass types were observed. During anticyclonic periods and conditions of continental outflow Aitken and accumulation mode were enhanced by a factor of 5 compared to the marine sector, whilst coarse mode particles were enhanced during westerly conditions. Baseline marine conditions were rarely met at Mace Head during NAMBLEX and high wind speeds were observed for brief periods only. The NAMBLEX experiment focussed on a detailed assessment of photochemistry in the marine environment, investigating the linkage between the HOx and the halogen radical cycles. Heterogeneous losses are important in both these cycles. In this paper loss rates of gaseous species to aerosol surfaces were calculated for a range of uptake coefficients. Even when the accommodation coefficient is unity, lifetimes due to heterogeneous loss of less than 10 s were never observed and rarely were they less than 500 s. Diffusional limitation to mass transfer is important in most conditions as the coarse mode is always significant. We calculate a minimum overestimate of 50% in the loss rate if this is neglected and so it should always be considered when calculating loss rates of gaseous species to particle surfaces. HO2 and HOI have accommodation coefficients of around 0.03 and hence we calculate lifetimes due to loss to particle surfaces of 2000 s or greater under the conditions experienced during NAMBLEX. Aerosol composition data collected during this experiment provide representative information on the input aerosol characteristics to western

  1. Chemical characteristics of aerosol particles (PM2.5) at a site of Horqin Sand-land in northeast China.

    PubMed

    Shen, Zhen-xing; Cao, Jun-ji; Li, Xu-xiang; Wang, Ya-qiang; Jie, Dong-mei; Zhang, Xiao-ye

    2006-01-01

    The objective of this study was to characterize the mass concentration and chemical composition of aerosol particles (PM2.5) collected at Tongliao (Inner Mongolia Autonomous Region, China), a site in Horqin Sand-land in northeast China. During spring 2005, the mass concentration for PM2.5 was (126 +/- 71)microg/m3 in average. Five dust storm events were monitored with higher concentration of (255 +/- 77)microg/m3 in average than the non dusty days of (106 +/- 44)microg/m3. Concentrations for 20 elements were obtained by the PIXE method. Mass concentrations of Al, Mg, Si, K, Ca, Ti, Mn, and V, which increased with the PM2.5 concentration, were higher than the pollution elements (S, Cl, Zn, Ar, Se, Br, and Pb). Enrichment factor relative to crust material was also calculated, which showed dust trace elements were mainly from earth upper crust and pollution elements were dominated the anthropogenic aerosols. The Si/Al, Ca/Al, and Fe/Al ratios in PM2.5 samples at Tongliao were 4.07, 0.94, and 0.82, respectively, which were remarkably different with those on other source regions, such as "Western desert source region", "North desert source region" and central Asia source. Air mass back-trajectory analysis identified three kinds of general pathways were associated with the aerosol particle transport to Tongliao, but have the similar elemental ratios, implying that elemental signatures for dust aerosol from Horqin Sand-land were different with other regions.

  2. Chemical characterization of submicron aerosol and particle growth events at a national background site (3295 m a.s.l.) on the Tibetan Plateau

    NASA Astrophysics Data System (ADS)

    Du, W.; Sun, Y. L.; Xu, Y. S.; Jiang, Q.; Wang, Q. Q.; Yang, W.; Wang, F.; Bai, Z. P.; Zhao, X. D.; Yang, Y. C.

    2015-09-01

    Atmospheric aerosols exert highly uncertain impacts on radiative forcing and also have detrimental effects on human health. While aerosol particles are widely characterized in megacities in China, aerosol composition, sources and particle growth in rural areas in the Tibetan Plateau remain less understood. Here we present the results from an autumn study that was conducted from 5 September to 15 October 2013 at a national background monitoring station (3295 m a.s.l.) in the Tibetan Plateau. The submicron aerosol composition and particle number size distributions were measured in situ with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) and a Scanning Mobility Particle Sizer (SMPS). The average mass concentration of submicron aerosol (PM1) is 11.4 μg m-3 (range: 1.0-78.4 μg m-3) for the entire study, which is much lower than observed at urban and rural sites in eastern China. Organics dominated PM1, accounting for 43 % on average, followed by sulfate (28 %) and ammonium (11 %). Positive Matrix Factorization analysis of ACSM organic aerosol (OA) mass spectra identified an oxygenated OA (OOA) and a biomass burning OA (BBOA). The OOA dominated OA composition, accounting for 85 % on average, 17 % of which was inferred from aged BBOA. The BBOA contributed a considerable fraction of OA (15 %) due to the burning of cow dung and straw in September. New particle formation and growth events were frequently observed (80 % of time) throughout the study. The average particle growth rate is 2.0 nm h-1 (range: 0.8-3.2 nm h-1). By linking the evolution of particle number size distribution to aerosol composition, we found an elevated contribution of organics during particle growth periods and also a positive relationship between the growth rate and the fraction of OOA in OA, which potentially indicates an important role of organics in particle growth in the Tibetan Plateau.

  3. 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.

  4. 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.

  5. Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield

    DOE PAGES

    Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; ...

    2015-03-18

    We performed a systematic intercomparison study of the chemistry and yields of secondary organic aerosol (SOA) generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0 × 108 to 2.2 × 1010 molec cm-3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2 × 106 to 2 × 107 molec cm-3 over exposure times of several hours. The OH concentration in themore » chamber experiments is close to that found in the atmosphere, but the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. In most cases, for a specific SOA type the most-oxidized chamber SOA and the least-oxidized flow reactor SOA have similar mass spectra, oxygen-to-carbon and hydrogen-to-carbon ratios, and carbon oxidation states at integrated OH exposures between approximately 1 × 1011 and 2 × 1011 molec cm-3 s, or about 1–2 days of equivalent atmospheric oxidation. This observation suggests that in the range of available OH exposure overlap for the flow reactor and chambers, SOA elemental composition as measured by an aerosol mass spectrometer is similar whether the precursor is exposed to low OH concentrations over long exposure times or high OH concentrations over short exposure times. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The influence of

  6. The application of single particle aerosol mass spectrometry for the detection and identification of high explosives and chemical warfare agents

    SciTech Connect

    Martin, Audrey Noreen

    2006-01-01

    Single Particle Aerosol Mass Spectrometry (SPAMS) was evaluated as a real-time detection technique for single particles of high explosives. Dual-polarity time-of-flight mass spectra were obtained for samples of 2,4,6-trinitrotoluene (TNT), 1,3,5-trinitro-1,3,5-triazinane (RDX), and pentaerythritol tetranitrate (PETN); peaks indicative of each compound were identified. Composite explosives, Comp B, Semtex 1A, and Semtex 1H were also analyzed, and peaks due to the explosive components of each sample were present in each spectrum. Mass spectral variability with laser fluence is discussed. The ability of the SPAMS system to identify explosive components in a single complex explosive particle (~1 pg) without the need for consumables is demonstrated. SPAMS was also applied to the detection of Chemical Warfare Agent (CWA) simulants in the liquid and vapor phases. Liquid simulants for sarin, cyclosarin, tabun, and VX were analyzed; peaks indicative of each simulant were identified. Vapor phase CWA simulants were adsorbed onto alumina, silica, Zeolite, activated carbon, and metal powders which were directly analyzed using SPAMS. The use of metal powders as adsorbent materials was especially useful in the analysis of triethyl phosphate (TEP), a VX stimulant, which was undetectable using SPAMS in the liquid phase. The capability of SPAMS to detect high explosives and CWA simulants using one set of operational conditions is established.

  7. Comparison of Aerosol Optical Depth from GOES Aerosol and Smoke Product (GASP) and MODIS to AERONET AOD and IMPROVE PM2.5 Mass at Bondville, Illinois Stratified by Chemical Composition, RH, Particle Size, and Season

    NASA Astrophysics Data System (ADS)

    Green, M. C.; Kondragunta, S.; Ciren, P.

    2008-05-01

    The USEPA is interested in using satellite remote sensing data to estimate levels of PM2.5. Here we report on comparisons of aerosol optical depth (AOD) from GOES Aerosol and Smoke Product (GASP) and the Moderate Resolution Imaging Spectroradiometer (MODIS) to IMPROVE network PM2.5 mass and AErosol RObotic NETwork (AERONET) ground-based AOD. Before we compare GASP and MODIS AOD to PM2.5, we first evaluate satellite AOD using the ground-based AERONET measurements and how it varies by aerosol chemical composition and size distribution. We focus attention on the Bondville, Illinois site because there is collocated IMPROVE sampling and an AERONET site. GASP provides aerosol optical depth at 0.55 um using top of atmosphere visible channel radiance measured from GOES east and GOES west. Time resolution is typically every 30 minutes during daylight hours. MODIS provides typically once per day AOD for any given location. The IMPROVE sampler provides a 24-hour integrated sample of PM10 mass, and PM2.5 mass and elemental composition on a one day in three schedule. AERONET provides aerosol optical depth at multiple wavelengths and aerosol size distribution as well as other derived parameters such as Angstrom exponent from ground based daytime measurements. We stratified cases by RH group, major chemical component, size distribution, and season. GOES AOD correlated best with PM2.5 mass during periods with mainly small particles, moderate RH, and sulfate dominated aerosol. It correlated poorly when RH is very high or low, aerosol is primarily organic, and when coarse to fine mass ratio is high. GASP AOD also correlated best with AERONET AOD when particles are mainly fine, suggesting the aerosol model assumptions (e.g. size distribution) may need to be varied geographically for GASP to achieve better AOD results.

  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.

  9. Chemical and physical characteristics of aerosol particles at a remote coastal location, Mace Head, Ireland, during NAMBLEX

    NASA Astrophysics Data System (ADS)

    Coe, H.; Allan, J. D.; Alfarra, M. R.; Bower, K. N.; Flynn, M. J.; McFiggans, G. B.; Topping, D. O.; Williams, P. I.; O'Dowd, C. D.; Dall'Osto, M.; Beddows, D. C. S.; Harrison, R. M.

    2005-11-01

    Aerosol number concentrations and size distributions from 3 nm to 20 µm diameter were measured at the Mace Head Atmospheric Research Station, Co. Galway, Ireland, a coastal site on the eastern seaboard of the north Atlantic Ocean. Both on and offline size resolved aerosol composition measurements were also made using an Aerodyne Aerosol Mass Spectrometer (AMS) and ion chromatographic analysis of daily samples collected using a Micro-Orifice Uniform Deposit Impactor (MOUDI). Particle number concentrations, size distributions and AMS measurements were determined at 7 and 22 m above ground level to investigate local effects on the aerosol size distribution induced by the tidal zone. During periods of new particle formation ultrafine particle number concentrations are large and variable, however, outside these periods no variability in particle number was observed at any size, nor was the particle composition variable. Analysis of particle size distributions show that within each air mass observed particle number concentrations were very consistent. During anticyclonic periods and conditions of continental outflow Aitken and accumulation mode were enhanced by a factor of 5 compared to the marine sector, whilst coarse mode particles were enhanced during westerly conditions. Baseline marine conditions were rarely met at Mace Head during NAMBLEX and high wind speeds were observed for brief periods only. Loss rates of gaseous species to aerosol surfaces were calculated for a range of uptake coefficients. Even when the accommodation coefficient is unity, lifetimes of less than 100 s were never observed and rarely were lifetimes less than 500 s. Diffusional limitation to mass transfer is important in most conditions as the coarse mode is always significant, we calculate a minimum overestimate of 50% in the loss rate if this is neglected and so it should always be considered when calculating loss rates of gaseous species to particle surfaces. HO2 and HOI have accommodation

  10. Differentiation of hydrophobic from hydrophilic submicrometer aerosol particles

    SciTech Connect

    Juozaitis, A.; Ulevicius, V.; Girgzdys, A. ); Willeke, K. )

    1993-02-01

    A method has been developed that differentiates hydrophobic from hydrophilic submicrometer aerosol particles in air environments containing polydisperse aerosols composed of different chemical species. First, a narrow particle size range is extracted from the polydisperse aerosol by an electrostatic aerosol classifier. Then the monodisperse aerosols of different origins are exposed to preselected supersaturation levels and are size-classified again by a second electrostatic classifier. Hydrophobic aerosol particles pass through the second classifier when its size window matches that of the first classifier. Hydrophilic aerosol particles grow to a larger size and are removed by the second classifier. The method has been applied in the field by measuring the fraction of hydrophobic atmospheric particles in a suburb of Vilnius, Lithuania, during a period of high emission of hydrophobic soot particles from residential coal and industrial oil burning in winter. 33 refs., 4 figs.

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

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  13. Chemical characterization of individual microparticles using an ion trap: real-time chemical analysis of aerosol particles

    SciTech Connect

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

    1996-10-01

    This paper describes initial experiments to perform laser ablation mass spectrometry in real time on airborne microparticles. The microparticles are sampled directly from the air by a particle inlet system into the vacuum chamber of a mass spectrometer. 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 in the mass spectrometer. The initial studies were made with an existing ion trap mass spectrometer with the particle sampling occurring at the center of the trap electrodes. Performance of the inlet system, particle detection, and preliminary results are described.

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

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

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

  15. Atmospheric aerosols as prebiotic chemical reactors

    PubMed Central

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

    2000-01-01

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

  16. Phase transition behaviour of sodium oleate aerosol particles

    NASA Astrophysics Data System (ADS)

    Nájera, Juan J.

    Field measurements have shown that organic surfactants are significant components of atmospheric aerosols. While fatty acids, among other surfactants, are prevalent in the atmosphere, the influence of these species on the chemical and physical properties of atmospheric aerosols remains not fully characterized. In order to assess the phase in which particles may exist, a detailed study of the deliquescence of a model surfactant aerosol has been carried out. Sodium oleate was chosen as a surfactant proxy relevant in atmospheric aerosol. Sodium oleate micelle aerosol particles were generated nebulizing a sodium oleate aqueous solution. In this study, the water uptake and phase transition of sodium oleate aerosol particles have been studied in a room temperature aerosol flow tube system (AFT) using Fourier transform infrared (FTIR) spectroscopy. Aerosol morphology and elemental composition were also analysed using scanning electron microscopy/energy dispersive X-ray analysis (SEM/EDX) techniques. The particles are homogeneously distributed as ellipsoidal-shape aggregates of micelles particles with an average size of ˜1.1 μm. The deliquescence by the sodium oleate aerosol particles was monitored by infrared extinction spectroscopy, where the dried aerosol particles were exposed to increasing relative humidity as they passed through the AFT. Observations of the infrared absorption features of condensed phase liquid water enable to determine the sodium oleate deliquescence phase transition at 88±2%.

  17. The effect of local sources on particle size and chemical composition and their role in aerosol-cloud interactions at Puijo measurement station

    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.

    2014-06-01

    Interactions between aerosols and liquid water clouds were studied during autumns 2010-2011 at a semiurban measurement station on Puijo tower in Kuopio, Finland. Cloud interstitial and total aerosol size distributions, particle chemical composition and hygroscopicity and cloud droplet size distribution were measured, with a focus on comparing clean air masses with those affected by local sources. On average, the polluted air contained more particles than the clean air masses, and generally the concentrations decreased during cloud events. Cloud processing was found to take place, especially in the clean air masses, and to a lesser extent in the polluted air. Some, mostly minor, differences in the average 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, with a special focus on the emissions from local sources, including a paper mill and a heating plant. This revealed larger variations in particle and cloud properties than the analysis of the whole data set. Clear differences in the total (between 214 and 2200 cm-3) and accumulation mode particle concentrations (between 62 and 169 cm-3) were observed. Particle chemical composition, especially the concentrations of organics (between 0.42 and 1.28 μg m-3) and sulfate (between 0.16 and 4.43 μg m-3), varied considerably. This affected the hygroscopic growth factor: for example, for 100 nm particles the range was from 1.21 to 1.45 at 90% relative humidity. Particularly, large particles, high hygroscopicities and elevated amounts of inorganics were linked with the pollutant plumes. Moreover, the particle hygroscopicity distributions in the polluted air were clearly bimodal, indicating externally mixed aerosol. The variable conditions also had an impact on cloud droplet

  18. Aerosol simulation including chemical and nuclear reactions

    SciTech Connect

    Marwil, E.S.; Lemmon, E.C.

    1985-01-01

    The numerical simulation of aerosol transport, including the effects of chemical and nuclear reactions presents a challenging dynamic accounting problem. Particles of different sizes agglomerate and settle out due to various mechanisms, such as diffusion, diffusiophoresis, thermophoresis, gravitational settling, turbulent acceleration, and centrifugal acceleration. Particles also change size, due to the condensation and evaporation of materials on the particle. Heterogeneous chemical reactions occur at the interface between a particle and the suspending medium, or a surface and the gas in the aerosol. Homogeneous chemical reactions occur within the aersol suspending medium, within a particle, and on a surface. These reactions may include a phase change. Nuclear reactions occur in all locations. These spontaneous transmutations from one element form to another occur at greatly varying rates and may result in phase or chemical changes which complicate the accounting process. This paper presents an approach for inclusion of these effects on the transport of aerosols. The accounting system is very complex and results in a large set of stiff ordinary differential equations (ODEs). The techniques for numerical solution of these ODEs require special attention to achieve their solution in an efficient and affordable manner. 4 refs.

  19. Measurements of aerosol-cloud interactions, including on-line particle chemical composition, at the Jungfraujoch Global Atmospheric Watch Station

    NASA Astrophysics Data System (ADS)

    Coe, H.; Allan, J. D.; Alfarra, M. R.; Williams, P. I.; Bower, K. N.; Gallagher, M. W.; Choularton, T. W.; Weingartner, E.; Corrigan, C.; Baltensperger, U.

    2003-04-01

    The Global Atmospheric Watch research laboratory is located in the Sphinx building, 3580 m asl; 46.55oN, 7.98oE on the Jungfraujoch in the Swiss Alps. The site is exposed to a wide range of conditions and frequently samples long range transported lower free tropospheric air, and is exposed to cloudy conditions. The Paul Scherrer Institute have previously developed a dual inlet system that allows measurements of the total sub-micron aerosol population (dry residuals and interstitial particles) and interstitial particles alone to be made alternately every few minutes. During July 2002 an Aerodyne Aerosol Mass Spectrometer was coupled to the dual inlet and was used to sample the composition of both the total particle distribution and the interstitial fraction and hence derive the mass loadings of the dry droplet residuals. In out of cloud conditions the aerosol composition can be linked to air mass history and age of the air mass. Microphysical measurements include cloud droplet size distributions made using an FSSP and also a new phase Doppler anemometry system. A comparison between these probes will be made. Two different types of cloud droplet spectra were observed. In the first type a large number of cloud droplets were measured with a single, narrow drop size distribution and modal diameter of around 10 um. In the second type, a bimodal cloud droplet spectrum occurred with a smaller mode (by number) at around 20 um, in addition to the 10 um mode. The aerosol mass spectrometry shows that the composition of the residuals from the two spectrum types is very different, the former type being composed mainly of sulphate, the latter a combination of nitrate, sulphate and organic material. We have also shown that the organic material observed is highly oxidized. We argue that the bimodality arises as a result of mixing of cloud droplets below the site that have been activated separately: the larger a less numerous mode in the widespread strato-cumulus forming under low

  20. Nozzles for Focusing Aerosol Particles

    DTIC Science & Technology

    2009-10-01

    control number. PLEASE DO NOT RETURN YOUR FORM TO THE ABOVE ADDRESS. 1. REPORT DATE ( DD -MM-YYYY) October 2009 2. REPORT TYPE Final 3. DATES...Figures Figure 1. The design of the first-generation aerodynamic focusing nozzle for aerosol particles used for SPFS and TAOS instrument prototypes...Some nozzles were fabricated in aluminum and some in steel. It has been used for SPFS and TAOS measurement technologies both in the laboratory and

  1. 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

  2. Sodium Nitrate Particles: Physical and Chemical Properties During Hydration and Dehydration, and Implications for Aged Sea Salt Aerosols

    SciTech Connect

    Hoffman, Rachel C.; Laskin, Alexander; Finlayson-Pitts, Barbara J.

    2004-07-01

    Experiments probing the phase and behavior of NaNO3 particles at different relative humidities, important for elucidating the role these play in the chemistry and radiative properties of marine regions, are presented. Changes in NaNO3 particles during hydration were studied using environmental scanning electron microscopy (ESEM) and conventional SEM coupled with energy dispersive X-ray analysis (SEM/EDX). Mixtures of NaNO3 and NaCl, which are typical of partially processed sea salt particles, were also studied. Complementary studies using long path FTIR were carried out to determine the extent of water association with NaNO3 aerosols, and for comparison, NaCl, MgCl2, and NH4NO3, as a function of relative humidity. The combination of these techniques shows that NaNO3 particles exist as unusual metastable, amorphous solids at low relative humidity that undergo continuous hygroscopic growth with increasing relative humidity. While other evidence for this phenomenon has been reported, this is the first direct observation using ESEM.

  3. 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.

  4. Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge

    SciTech Connect

    Gilles, Mary K; Moffet, R.C.; Henn, T.; Laskin, A.

    2011-01-20

    We have developed an automated data analysis method for atmospheric particles using scanning transmission X-ray microscopy coupled with near edge X-ray fine structure spectroscopy (STXM/NEXAFS). This method is applied to complex internally mixed submicrometer particles containing organic and inorganic material. Several algorithms were developed to exploit NEXAFS spectral features in the energy range from 278 to 320 eV for quantitative mapping of the spatial distribution of elemental carbon, organic carbon, potassium, and noncarbonaceous elements in particles of mixed composition. This energy range encompasses the carbon K-edge and potassium L2 and L3 edges. STXM/NEXAFS maps of different chemical components were complemented with a subsequent analysis using elemental maps obtained by scanning electron microscopy coupled with energy dispersive X-ray analysis (SEM/EDX). We demonstrate the application of the automated mapping algorithms for data analysis and the statistical classification of particles.

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

    DOE PAGES

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; ...

    2015-03-16

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-08-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

  8. 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.

  9. Nano-objects emitted during maintenance of common particle generators: direct chemical characterization with aerosol mass spectrometry and implications for risk assessments

    NASA Astrophysics Data System (ADS)

    Nilsson, Patrik T.; Isaxon, Christina; Eriksson, Axel C.; Messing, Maria E.; Ludvigsson, Linus; Rissler, Jenny; Hedmer, Maria; Tinnerberg, Håkan; Gudmundsson, Anders; Deppert, Knut; Bohgard, Mats; Pagels, Joakim H.

    2013-11-01

    Nanotechnology gives us materials with enhanced or completely new properties. At the same time, inhalation of manufactured nano-objects has been related to an array of adverse biological effects. We characterized particle emissions, which occurred during maintenance of common metal nanoparticle generators and contrasted the properties of the emitted particles with those originally produced by the generators. A new approach using online aerosol mass spectrometry (AMS), for time- and size-resolved measurements of the particle chemical composition, was applied in combination with more conventional techniques for particle sampling and analysis, including electron microscopy. Emissions during maintenance work, in terms of mass and surface area concentration in the size range of 0.02-10 μm, were dominated by large agglomerates (1-5 μm). With AMS, we show that the particle composition depends on both generator type and maintenance task being performed and that the instrument can be used for highly time-resolved selective studies of metal nanoparticle emissions. The emitted agglomerates have a relatively high probability to be deposited in the lower respiratory tract, since the mean particle diameter coincided with a peak in the lung deposition curve. Each of these agglomerates consisted of a very high number (103-105/agglomerate) of nanometer-sized primary particles originating from the particle synthesis process. This made them possess large surface areas, one of the key properties in nanotoxicology. Similar agglomerates may be emitted in a wide range of processes when nanoparticles are manufactured or handled. The fate of such agglomerates, once deposited in the respiratory tract, is unknown and should therefore be considered in future particle toxicological studies. Our results highlight the importance of including micrometer-sized particles in exposure and emission assessments.

  10. 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.

  11. Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors

    NASA Astrophysics Data System (ADS)

    Zhang, X. Y.; Wang, J. Z.; Wang, Y. Q.; Liu, H. L.; Sun, J. Y.; Zhang, Y. M.

    2015-11-01

    Since there have been individual reports of persistent haze-fog events in January 2013 in central-eastern China, questions on factors causing the drastic differences in changes in 2013 from changes in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributing to such changes is yet to be determined. The study intends to present the changes in daily based major water-soluble constituents, carbonaceous species, and mineral aerosol in PM10 at 13 stations within different haze regions in China from 2006 to 2013, which are associated with specific meteorological conditions that are highly related to aerosol pollution (parameterized as an index called Parameter Linking Aerosol Pollution and Meteorological Elements - PLAM). No obvious changes were found in annual mean concentrations of these various chemical components and PM10 in 2013, relative to 2012. By contrast, wintertime mass of these components was quite different. In Hua Bei Plain (HBP), sulfate, organic carbon (OC), nitrate, ammonium, element carbon (EC), and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21, and 130 μg m-3, respectively; these masses were approximately 2 to 4 times higher than those in background mass, which also exhibited a decline during 2006 to 2010 and then a rise till 2013. The mass of these concentrations and PM10, except minerals, respectively, increased by approximately 28 to 117 % and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze-fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In the Yangtze River Delta (YRD) area, winter masses of these components, unlike HBP, have not significantly increase since 2010; PLAM were also maintained at a similar level without

  12. The optical manipulation and characterisation of aerosol particles

    NASA Astrophysics Data System (ADS)

    Reid, Jonathan P.

    2008-08-01

    Aerosols play a crucial role in many areas of science, ranging from atmospheric chemistry and physics, to pharmaceutical aerosols and drug delivery to the lungs, to combustion science and spray drying. The development of new methods for characterising the properties and dynamics of aerosol particles is of crucial importance if the complex role that particles play is to be more fully understood. Optical tweezers provide a valuable new tool to address fundamental questions in aerosol science. Single or multiple particles 1-15 μm in diameter can be manipulated for indefinite timescales. Linear and non-linear Raman and fluorescence spectroscopies can be used to probe particle composition, phase, component mixing state, and size. In particular, size can be determined with nanometre accuracy, allowing accurate measurements of the thermodynamic properties of aerosols, the kinetics of particle transformation and of light absorption. Further, the simultaneous manipulation of multiple particles in parallel optical traps provides a method for performing comparative measurements on particles of different composition. We will present some latest work in which optical tweezers are used to characterise aerosol dynamics, demonstrating that optical tweezers can find application in studies of hygroscopicity, the mixing state of different chemical components, including the phase separation of immiscible phases, and the kinetics of chemical transformation.

  13. Chemical aerosol detection using femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Alexander, Dennis R.; Rohlfs, Mark L.; Stauffer, John C.

    1997-07-01

    Many chemical warfare agents are dispersed as small aerosol particles. In the past, most electro-optical excitation and detection schemes have used continuous or pulsed lasers with pulse lengths ranging from nanoseconds to microseconds. In this paper, we present interesting ongoing new results on femtosecond imaging and on the time dependent solutions to the scattering problem of a femtosecond laser pulse interacting with a single small aerosol particle. Results are presented for various incident pulse lengths. Experimental imaging results using femtosecond pulses indicate that the diffraction rings present when using nanosecond laser pulses for imaging are greatly reduced when femtosecond laser pulses are used. Results are presented in terms of the internal fields as a function of time and the optical size parameter.

  14. Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors

    NASA Astrophysics Data System (ADS)

    Zhang, X. Y.; Wang, J. Z.; Wang, Y. Q.; Liu, H. L.; Sun, J. Y.; Zhang, Y. M.

    2015-07-01

    Since individuals experienced persistent haze-fog events in January 2013 in central-eastern China, questions on factors causing differences in drastic changes in 2013 from those in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributed to such changes is yet to be determined. The study intends to present the changes in daily-based major water-soluble constituents, carbonaceous species and mineral aerosol in PM10 at 13 stations within different haze regions in China from 2006 to 2013, associated with specific meteorological conditions that are highly related with aerosol pollution (parameterized as an index called "PLAM"). No obvious changes were found in annual mean concentrations of these various chemical components and PM10 in 2013, relative to 2012. By contrast, wintertime mass of these components were quite different, in Hua Bei Plain (HBP), sulfate, OC, nitrate, ammonium, EC, and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21 and 130 μg m-3, respectively; these masses were approximately two to four times higher than those in background mass, also exhibiting a decline during 2006 to 2010, and then a rise till 2013. The mass of these concentrations and PM10, except mineral, respectively increased by approximately 28 to 117 and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze-fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In Yangtzi River Delta (YRD) area, winter masses of these components, unlike HBP, did not significantly increase since 2010; PLAM was also maintained at a similar level without significant changes. In the Pearl River Delta (PRD) area, the regional background concentrations of the major chemical components were similar

  15. Chemical Properties of Combustion Aerosols: An Overview

    EPA Science Inventory

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

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

    SciTech Connect

    Davidovits, Paul

    2015-10-20

    ) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in

  17. A conceptual framework for mixing structures in individual aerosol particles

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Sun, Jiaxing; Xu, Liang; Shi, Zongbo; Riemer, Nicole; Sun, Yele; Fu, Pingqing; Zhang, Jianchao; Lin, Yangting; Wang, Xinfeng; Shao, Longyi; Chen, Jianmin; Zhang, Xiaoye; Wang, Zifa; Wang, Wenxing

    2016-11-01

    This study investigated the particle size- and age-dependent mixing structures of individual particles in clean and polluted air. Aerosols were classified into eight components: sea salt, mineral dust, fly ash, metal, soot, sulfates, nitrates, and organic matter (OM). Based on our aerosol classification, a particle that consists of two or more aerosol components can be defined as an internally mixed particle. Otherwise, it is considered to be an externally mixed particle. Within the internally mixed particle class, we identified four heterogeneous mixing structures: core-shell, dumbbell, OM coating, and dispersed OM, as well as one homogeneous-like mixing structure. Homogeneous-like mixing mainly occurred in fine particles (<1 µm), while the frequency of heterogeneously mixed particles increased with particle size. Our study demonstrated that particle mixing structures depend on particle size and location and evolve with time. OM-coating and core-shell structures are important indicators for particle aging in air as long as they are distant from specific emission sources. Long-range transported particles tended to have core-shell and OM-coating structures. We found that secondary aerosol components (e.g., sulfates, nitrates, and organics) determined particle mixing structures, because their phases change following particle hydration and dehydration under different relative humidities. Once externally mixed particles are transformed into internally mixed particles, they cannot revert to their former state, except when semivolatile aerosol components are involved. Categorizing mixing structures of individual particles is essential for studying their optical and hygroscopic properties and for tracing the development of their physical or chemical properties over time.

  18. Detection of chemical agent aerosols

    NASA Astrophysics Data System (ADS)

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

    1999-05-01

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

  19. 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.

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

    SciTech Connect

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

    2015-03-16

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

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

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

  2. 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.

  3. 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

  4. 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.

  5. 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

  6. 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.

  7. 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.

  8. 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.

  9. Electronic cigarette aerosol particle size distribution measurements.

    PubMed

    Ingebrethsen, Bradley J; Cole, Stephen K; Alderman, Steven L

    2012-12-01

    The particle size distribution of aerosols produced by electronic cigarettes was measured in an undiluted state by a spectral transmission procedure and after high dilution with an electrical mobility analyzer. The undiluted e-cigarette aerosols were found to have particle diameters of average mass in the 250-450 nm range and particle number concentrations in the 10(9) particles/cm(3) range. These measurements are comparable to those observed for tobacco burning cigarette smoke in prior studies and also measured in the current study with the spectral transmission method and with the electrical mobility procedure. Total particulate mass for the e-cigarettes calculated from the size distribution parameters measured by spectral transmission were in good agreement with replicate determinations of total particulate mass by gravimetric filter collection. In contrast, average particle diameters determined for e-cigarettes by the electrical mobility method are in the 50 nm range and total particulate masses calculated based on the suggested diameters are orders of magnitude smaller than those determined gravimetrically. This latter discrepancy, and the very small particle diameters observed, are believed to result from almost complete e-cigarette aerosol particle evaporation at the dilution levels and conditions of the electrical mobility analysis. A much smaller degree, ~20% by mass, of apparent particle evaporation was observed for tobacco burning cigarette smoke. The spectral transmission method is validated in the current study against measurements on tobacco burning cigarette smoke, which has been well characterized in prior studies, and is supported as yielding an accurate characterization of the e-cigarette aerosol particle size distribution.

  10. CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

    EPA Science Inventory

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

  11. 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.

  12. 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.

  13. 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

  14. Aerosol particles and the formation of advection fog

    NASA Technical Reports Server (NTRS)

    Hung, R. J.; Liaw, G. S.; Vaughan, O. H., Jr.

    1979-01-01

    A study of numerical simulation of the effects of concentration, particle size, mass of nuclei, and chemical composition on the dynamics of warm fog formation, particularly the formation of advection fog, is presented. This formation is associated with the aerosol particle characteristics, and both macrophysical and microphysical processes are considered. In the macrophysical model, the evolution of wind components, water vapor content, liquid water content, and potential temperature under the influences of vertical turbulent diffusion, turbulent momentum, and turbulent energy transfers are taken into account. In the microphysical model, the supersaturation effect is incorporated with the surface tension and hygroscopic material solution. It is shown that the aerosol particles with the higher number density, larger size nuclei, the heavier nuclei mass, and the higher ratio of the Van't Hoff factor to the molecular weight favor the formation of the lower visibility advection fogs with stronger vertical energy transfer during the nucleation and condensation time period.

  15. 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

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

    EPA Science Inventory

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

  17. 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.

  18. 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.

  19. 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.

  20. 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

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

    EPA Science Inventory

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

  2. Spatial Variability of CCN Sized Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Asmi, A.; Väänänen, R.

    2014-12-01

    The computational limitations restrict the grid size used in GCM models, and for many cloud types they are too large when compared to the scale of the cloud formation processes. Several parameterizations for e.g. convective cloud formation exist, but information on spatial subgrid variation of the cloud condensation nuclei (CCNs) sized aerosol concentration is not known. We quantify this variation as a function of the spatial scale by using datasets from airborne aerosol measurement campaigns around the world including EUCAARI LONGREX, ATAR, INCA, INDOEX, CLAIRE, PEGASOS and several regional airborne campaigns in Finland. The typical shapes of the distributions are analyzed. When possible, we use information obtained by CCN counters. In some other cases, we use particle size distribution measured by for example SMPS to get approximated CCN concentration. Other instruments used include optical particle counters or condensational particle counters. When using the GCM models, the CCN concentration used for each the grid-box is often considered to be either flat, or as an arithmetic mean of the concentration inside the grid-box. However, the aircraft data shows that the concentration values are often lognormal distributed. This, combined with the subgrid variations in the land use and atmospheric properties, might cause that the aerosol-cloud interactions calculated by using mean values to vary significantly from the true effects both temporary and spatially. This, in turn, can cause non-linear bias into the GCMs. We calculate the CCN aerosol concentration distribution as a function of different spatial scales. The measurements allow us to study the variation of these distributions within from hundreds of meters up to hundreds of kilometers. This is used to quantify the potential error when mean values are used in GCMs.

  3. The relationship between aerosol particles chemical composition and optical properties to identify the biomass burning contribution to fine particles concentration: a case study for São Paulo city, Brazil.

    PubMed

    de Miranda, Regina Maura; Lopes, Fabio; do Rosário, Nilton Évora; Yamasoe, Marcia Akemi; Landulfo, Eduardo; de Fatima Andrade, Maria

    2016-12-01

    The air quality in the Metropolitan Area of São Paulo (MASP) is primarily determined by the local pollution source contribution, mainly the vehicular fleet, but there is a concern about the role of remote sources to the fine mode particles (PM2.5) concentration and composition. One of the most important remote sources of atmospheric aerosol is the biomass burning emissions from São Paulo state's inland and from the central and north portions of Brazil. This study presents a synergy of different measurements of atmospheric aerosol chemistry and optical properties in the MASP in order to show how they can be used as a tool to identify particles from local and remote sources. For the clear identification of the local and remote source contribution, aerosol properties measurements at surface level were combined with vertical profiles information. Over 15 days in the austral winter of 2012, particulate matter (PM) was collected using a cascade impactor and a Partisol sampler in São Paulo City. Mass concentrations were determined by gravimetry, black carbon concentrations by reflectance, and trace element concentrations by X-ray fluorescence. Aerosol optical properties were studied using a multifilter rotating shadowband radiometer (MFRSR), a Lidar system and satellite data. Optical properties, concentrations, size distributions, and elemental composition of atmospheric particles were strongly related and varied according to meteorological conditions. During the sampling period, PM mean mass concentrations were 17.4 ± 10.1 and 15.3 ± 6.9 μg/m(3) for the fine and coarse fractions, respectively. The mean aerosol optical depths at 415 nm and Ångström exponent (AE) over the whole period were 0.29 ± 0.14 and 1.35 ± 0.11, respectively. Lidar ratios reached values of 75 sr. The analyses of the impacts of an event of biomass burning smoke transport to the São Paulo city revealed significant changing on local aerosol concentrations and optical parameters

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

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

  5. 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.

  6. 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

  7. Aerosol reduction/expansion synthesis (A-RES) for zero valent metal particles

    DOEpatents

    Leseman, Zayd; Luhrs, Claudia; Phillips, Jonathan; Soliman, Haytham

    2016-04-12

    Various embodiments provide methods of forming zero valent metal particles using an aerosol-reductive/expansion synthesis (A-RES) process. In one embodiment, an aerosol stream including metal precursor compound(s) and chemical agent(s) that produces reducing gases upon thermal decomposition can be introduced into a heated inert atmosphere of a RES reactor to form zero valent metal particles corresponding to metals used for the metal precursor compound(s).

  8. 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

  9. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; Su, Hang; Pöschl, Ulrich; Wang, Jian; Knopf, Daniel A.

    2017-02-01

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation of liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.

  10. Initial size distributions and hygroscopicity of indoor combustion aerosol particles

    SciTech Connect

    Li, W.; Hopke, P.K.

    1993-10-01

    Cigarette smoke, incense smoke, natural gas flames, propane fuel flames, and candle flames are contributors of indoor aerosol particles. To provide a quantitative basis for the modeling of inhaled aerosol deposition pattern, the hygroscopic growth of particles from these five sources as well as the source size distributions were measured. Because the experiments were performed on the bases of particles of single size, it provided not only the averaged particle`s hygroscopic growth of each source, but also the detailed size change for particles of different sizes within the whole size spectrum. The source particle size distribution measurements found that cigarette smoke and incense smoke contained particles in the size range of 100-700 nm, while the natural gas, propane, and candle flames generated particles between 10 and 100 nm. The hygroscopic growth experiments showed that these combustion aerosol particles could grow 10% to 120%, depending on the particle sizes and origins. 18 refs., 15 figs., 3 tabs.

  11. 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.

  12. Chemical characterization of particle emissions from controlled burns of biomass fuels using a high resolution time-of-flight aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Qi, L.; Hosseini, S.; Jung, H.; Yokelson, B.; Weise, D.; Cocker, D., III; Huang, Y.

    2012-03-01

    A total of forty-nine burns were conducted at the Missoula Fire Sciences Lab consisting of nine fuel types; i.e., chamise scrub oak, ceanothus, maritime chaparral, coastal sage scrub, California sage brush, Manzanita, oak savanna, oak woodland and masticated mesquite. This paper focuses on the chemical characterization of fine particle emissions collected for flaming, mixed and smoldering phases using a HR ToF-AMS. The evolution of OM/OC, H/C, O/C and N/C from fire ignition to extinction was measured to capture the transient and integrated chemical composition of the non-refractory portion of bulk particles. Real time elemental ratios and empirical formulas derived with respect to modified combustion efficiency (MCE) are reported. For each fuel, the hydrogen fragment ions dominate the unit mass resolution (UMR) mass spectra with no specific fragment ions attributable to an individual ecological combination. An interference ion in the UMR m/z 73, a fragment normally attributed to levoglucosan, is noted. Therefore, the results imply that C2H4O2+ (m/z 60.021) plus C3H5O2+ (m/z 73.029) are more sufficient to estimate the contribution of levoglucosan. The results did not show significant variations of levoglucosan content in the organic particle with the overall average contribution fraction ranging from 0.74% for coastal sage to 1.93% for chamise.

  13. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2011-02-01

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

  15. Electron Microscopy and Raman Microspectroscopy as Characterization Tools and Probes of the Chemistry and Properties of Individual Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Grassian, V. H.

    2012-12-01

    Microscopic probes provide useful insights into the physicochemical properties of aerosol particles and their environmental and health effects. The focus of this talk is on the use of microscopic probes in a wide-range of laboratory studies to better understand the physicochemical properties (chemical heterogeneity, morphology, water uptake, infrared extinction and heterogeneous reactivity) of individual atmospheric aerosol particles. Microscopy coupled to energy dispersive X-ray analysis is used in these studies to characterize particles in terms of size and shape as individual particles or as aggregates particles as well as to follow chemical and physical transformations of particles as they undergo reactions under different environmental conditions. Raman microspectroscopy provides additional chemical specific information and the internal mixing of chemical constituents within individual particles. Several examples will be discussed for flyash, mineral dust and sea spray aerosol particles.

  16. A chemical analyzer for charged ultrafine particles

    NASA Astrophysics Data System (ADS)

    Gonser, S. G.; Held, A.

    2013-04-01

    New particle formation is a frequent phenomenon in the atmosphere and of major significance for the earth's climate and human health. To date the mechanisms leading to the nucleation of particles as well as to aerosol growth are not completely understood. A lack of appropriate measurement equipment for online analysis of the chemical composition of freshly nucleated particles is one major limitation. We have developed a Chemical Analyzer for Charged Ultrafine Particles (CAChUP) capable of analyzing particles with diameters below 30 nm. A bulk of size separated particles is collected electrostatically on a metal filament, resistively desorbed and consequently analyzed for its molecular composition in a time of flight mass spectrometer. We report of technical details as well as characterization experiments performed with the CAChUP. Our instrument was tested in the laboratory for its detection performance as well as for its collection and desorption capabilities. The manual application of known masses of camphene (C10H16) to the desorption filament resulted in a detection limit between 0.5 and 5 ng, and showed a linear response of the mass spectrometer. Flow tube experiments of 25 nm diameter secondary organic aerosol from ozonolysis of alpha-pinene also showed a linear relation between collection time and the mass spectrometer's signal intensity. The resulting mass spectra from the collection experiments are in good agreement with published work on particles generated by the ozonolysis of alpha-pinene. A sensitivity study shows that the current setup of CAChUP is ready for laboratory measurements and for the observation of new particle formation events in the field.

  17. A chemical analyzer for charged ultrafine particles

    NASA Astrophysics Data System (ADS)

    Gonser, S. G.; Held, A.

    2013-09-01

    New particle formation is a frequent phenomenon in the atmosphere and of major significance for the Earth's climate and human health. To date the mechanisms leading to the nucleation of particles as well as to aerosol growth are not completely understood. A lack of appropriate measurement equipment for online analysis of the chemical composition of freshly nucleated particles is one major limitation. We have developed a Chemical Analyzer for Charged Ultrafine Particles (CAChUP) capable of analyzing particles with diameters below 30 nm. A bulk of size-separated particles is collected electrostatically on a metal filament, resistively desorbed and subsequently analyzed for its molecular composition in a time of flight mass spectrometer. We report on technical details as well as characterization experiments performed with the CAChUP. Our instrument was tested in the laboratory for its detection performance as well as for its collection and desorption capabilities. The manual application of defined masses of camphene (C10H16) to the desorption filament resulted in a detection limit between 0.5 and 5 ng, and showed a linear response of the mass spectrometer. Flow tube experiments of 25 nm diameter secondary organic aerosol from ozonolysis of alpha-pinene also showed a linear relation between collection time and the mass spectrometer's signal intensity. The resulting mass spectra from the collection experiments are in good agreement with published work on particles generated by the ozonolysis of alpha-pinene. A sensitivity study shows that the current setup of CAChUP is ready for laboratory measurements and for the observation of new particle formation events in the field.

  18. Polycyclic Aromatic Aerosol Components: Chemical Analysis and Reactivity

    NASA Astrophysics Data System (ADS)

    Schauer, C.; Niessner, R.; Pöschl, U.

    Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous environmental pollutants in the atmosphere and originate primarily from incomplete combustion of organic matter and fossil fuels. Their main sources are anthropogenic (e.g. vehicle emissions, domes- tic heating or tobacco smoke), and PAHs consisting of more than four fused aromatic rings reside mostly on combustion aerosol particles, where they can react with atmo- spheric trace gases like O3, NOx or OH radicals leading to a wide variety of partially oxidized and nitrated derivatives. Such chemical transformations can strongly affect the activity of the aerosol particles as condensation nuclei, their atmospheric residence times, and consequently their direct and indirect climatic effects. Moreover some poly- cyclic aromatic compounds (PACs = PAHs + derivatives) are known to have a high carcinogenic, mutagenic and allergenic potential, and are thus of major importance in air pollution control. Furthermore PACs can be used as well defined soot model sub- stances, since the basic structure of soot can be regarded as an agglomerate of highly polymerized PAC-layers. For the chemical analysis of polycyclic aromatic aerosol components a new analyti- cal method based on LC-APCI-MS has been developed, and a data base comprising PAHs, Oxy-PAHs and Nitro-PAHs has been established. Together with a GC-HRMS method it will be applied to identify and quantify PAHs and Nitro-PAHs in atmo- spheric aerosol samples, diesel exhaust particle samples and model soot samples from laboratory reaction kinetics and product studies. As reported before, the adsorption and surface reaction rate of ozone on soot and PAH-like particle surfaces is reduced by competitive adsorption of water vapor at low relative humidity (< 25 %). Recent results at higher relative humidities (ca. 50 %), however, indicate re-enhanced gas phase ozone loss, which may be due to absorbtion of ozone into an aqueous surface layer. The interaction of ozone and nitrogen

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  20. Scanning Transmission X-ray microscopy Imaging of Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Gilles, M. K.; Kilcoyne, A.; Tyliszczak, T.; Shuh, D. K.; Fakra, S.; Robinson, M.; Chase, K.

    2003-12-01

    Scanning transmission x-ray microscopes (STXM) are used to image a diversity of carbon and metal containing items such as biofilms in soils, magnetic materials, polymers and meteorites. Studies on particles collected on SiO2 filters from biomass burns in Flagstaff, Arizona and individual aerosols collected in South Africa on TEM grids are underway at beamlines 5.3.2 and 11.0.2 at the Advanced Light Source of Lawrence Berkeley National Laboratory. Sub micron particles are imaged in the transmission mode over the energy range of 280 - 1900 eV. Spectromicroscopic studies on individual particles using near edge x-ray absorption fine structure (NEXAFS) probe multiple species within or on the same particle. In (STXM) an X-ray beam is focused with a zone plate onto a sample and the transmitted radiation is detected. Since the signal is obtained in the transmission mode, optically thin samples are required. Hence, atmospheric aerosols with submicron thickness and diameter are well suited for this method. Near edge spectra of various elements were scanned in step sizes from 0.1-0.5 eV around characteristic absorption edges, creating 2 dimensional images at each energy. While STXM images are taken with a lower spatial resolution (currently 40 nm) than microscopies such as scanning electron microscopy, transmission electron microscopy, and atomic force microscopy, detailed chemical information with spatial distributions, and oxidation states is obtained. A particular focus of this work is to obtain more detailed information on the type of carbons, multiply, or singly bonded and whether or not carbon is bonded to oxygen. The ultimate goal is discrimination between organic and black carbon within individual aerosol particles and determining if organic carbon, black carbon, and metal species are distributed homogeneously throughout aerosol particles. Initial scans of the samples from Flagstaff show spectral evidence of aromatic carbon, without distinct C=O signatures. NEXAFS

  1. 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

  2. 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.

  3. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2007-12-01

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

  5. Laser velocimeter seed particle sizing by the whisker particle collector and laser aerosol spectrometer methods

    NASA Astrophysics Data System (ADS)

    Crosswy, F. L.; Kingery, M. K.; Schaefer, H. J.; Pfeifer, H. J.

    1989-07-01

    Two different aerosol particle sizing systems, the Whisker Particle Collector (WPC) and the Laser Aerosol Spectrometer (LAS), were evaluated for sizing aerosol particles in the size range of 0.1 to 3.0 micrometers. The evaluation tests were conducted using an aerosol of alumina (Al2O3) particles, an aerosol commonly used to provide light scattering particles for laser velocimeter measurements in high temperature flows. The LAS and WPC measurements were then compared for samples taken from the alumina particle aerosols. Some difficulty was encountered in directly comparing these measurements. Other operational aspects of the two systems were also compared including on-line/off-line data presentation capabilities, field portability and measurement limitations at the small particle end of the size range of interest.

  6. Microphysical processing of aerosol particles in orographic clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

    2015-01-01

    An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice

  7. Microphysical processing of aerosol particles in orographic clouds

    NASA Astrophysics Data System (ADS)

    Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

    2015-08-01

    An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

  8. 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.

  9. 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.

  10. Influence of particle size and chemistry on the cloud nucleating properties of aerosols

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.

    2008-02-01

    The ability of an aerosol particle to act as a cloud condensation nuclei (CCN) is a function of the size of the particle, its composition and mixing state, and the supersaturation of the cloud. In-situ data from field studies provide a means to assess the relative importance of these parameters. During the 2006 Texas Air Quality - Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS-GoMACCS), the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources and chemistry in the potential activation of particles to form cloud droplets. Measurements were made of CCN concentrations, aerosol chemical composition in the size range relevant for particle activation in warm clouds, and aerosol size distributions. Variability in aerosol composition was parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA) for particle diameters less than 200 nm (vacuum aerodynamic). The HOA mass fraction in this size range was lowest for marine aerosol and highest for aerosol sampled close to anthropogenic sources. Combining all data from the experiment reveals that composition (defined by HOA mass fraction) explains 40% of the variance in the critical diameter for particle activation at the instrumental supersaturation (S) of 0.44%. Correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during TexAQS-GoMACCS, variability in particle composition played a significant role in determining the fraction of particles that could activate to form cloud droplets. Using a simple model based on Köhler theory and the assumption that HOA is insoluble, we estimate the degree to which calculated CCN

  11. 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.

  12. Chemical and Spatial Microscopy of Individual Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Tivanski, Alexei V.; Hopkins, Rebecca J.; Gilles, Mary K.

    2008-03-01

    Carbonaceous particles originating from biomass burning can account for a large fraction of organic aerosols in a local environment. Presently, their composition, physical, and chemical properties as well as their environmental effects are largely unknown. A distinct type of biomass burn particles, called ``tar balls'', have been observed in a number of field campaigns, both in fresh and aged smoke. They are characterized by their spherical morphology, high carbon content and ability to efficiently scatter and absorb light. Here, a combination of scanning transmission x-ray microscopy and near edge x-ray absorption fine structure spectroscopy is used to determine the shape, structure and size-dependent chemical composition of 150 individual tar ball particles ranging in size from 0.15 to 1.2 μm. Oxygen is present primarily as carboxylic carbonyls and oxygen-substituted alkyl functional groups. The observed chemical composition is distinctly different from black carbon and more closely resembles high molecular weight humic-like substances. A detailed examination of the carbonyl intensity as a function of particle size reveals the presence of a thin oxygenated interface layer on the tar balls, indicative of atmospheric processing of biomass burn particles.

  13. Resolving Changing Chemical and Physical Properties of SSA Particle Types during Laboratory Phytoplankton Blooms using Online Single Particle Analysis

    NASA Astrophysics Data System (ADS)

    Sultana, C. M.; Prather, K. A.; Richardson, R.; Wang, X.

    2015-12-01

    Changes in the chemical composition of sea spray aerosols (SSA) can modify their climate-relevant properties. Recent studies have shown a diverse set of distinct SSA particle types, however there are conflicting reports on how and whether biological activity controls the organic fraction and mixing state of SSA. This study leverages an aerosol time-of-flight mass spectrometer to give an accounting of the temporally resolved mixing state of primary SSA (0.4 - 3 µm vacuum aerodynamic diameter), encompassing 97% of particles detected over the course of laboratory phytoplankton blooms. The influence of biological activity on the climate relevant properties of defined particle types is also investigated. Spatial chemical particle heterogeneity and particularly the surface chemical composition of particles are described along with particle type specific water-particle interactions. These online measurements in tandem with chemical composition could give new insight on the link between seawater chemistry, marine aerosols, and climate properties.

  14. Mass Spectrometric Analysis of Pristine Aerosol Particles During the wet Season of Amazonia - Detection of Primary Biological Particles?

    NASA Astrophysics Data System (ADS)

    Schneider, J.; Zorn, S. R.; Freutel, F.; Borrmann, S.; Chen, Q.; Farmer, D. K.; Jimenez, J. L.; Flores, M.; Roldin, P.; Artaxo, P.; Martin, S. T.

    2008-12-01

    The contribution of primary biological aerosol (POA) particles to the natural organic aerosol is a subject of current research. Estimations of the POA contribution to the total aerosol particle concentration range between 25 and 80%, depending on location and season. Especially in the tropical rain forest it is expected that POA is a major source of supermicron, possibly also of submicron particles. During AMAZE (Amazonian Aerosol CharacteriZation Experiment), a field project near Manaus, Brazil, in February/March 2008, an Aerodyne ToF-AMS was equipped with a high pressure aerodynamic lens. This high pressure lens (operating pressure 14.6 torr) is designed with the objective to extend the detectable size range of the AMS into the supermicron size range where primary biological particles are expected. Size distribution measured by the AMS were compared with size distribution from an optical particle counter and indicate that the high pressure lens has a 50% cut-off at a vacuum aerodynamic diameter of about 1 μm, but still has significant transmission up to a vacuum aerodynamic diameter of about 2 μm, thus extending the detectable size range of the AMS into the coarse mode. The measuring instruments were situated in a container at ground level. The aerosol was sampled through a 40 m vertical, laminar inlet, which was heated and dried to maintain a relative humidity between 30 and 40%. The inlet was equipped with a 7 μm cut-off cyclone. Size distributions recorded with an optical particle counter parallel to the AMS show that the inlet transmitted aerosol particles up to an optically detected diameter of 10 μm. POA particles like plant fragments, pollen, spores, fungi, viruses etc. contain chemical compounds as proteins, sugars, amino acids, chlorophyll, and cellular material as cellulose. Laboratory experiments have been performed in order to identify typical mass spectral patterns of these compounds. These laboratory data were compared to size resolved particle

  15. 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

    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 particles of the same composition would allow proving that LLPS indeed occurs in particles of accumulation mode size. Up to now LLPS has not been studied for particles in this size range. References: 1. Bertram, et al. Atmos. Chem & Phys, 11(21), 10995-11006, 2011.
 2. Krieger, et al. Chemical Society Reviews, 41(19), 6631-6662, 2012 
3. Song, M. et al. Geophys Res Lett, 39(19), 2012b 4. Smith et al. Atmos Chem & Phys, 12(20), 9613- 9628, 2012.
 5. You, Y. et al. Proceedings of the National Academy of Sciences, 109(33), 13188-13193, 2012.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  18. Multi- year Arctic and Antarctic aerosol chemical characterization

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  19. Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean - potential impacts

    NASA Astrophysics Data System (ADS)

    Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier van der Gon, H. A. C.

    2010-07-01

    Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, indicating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols shows that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud, and by entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

  20. Chemically aged and mixed aerosols over the Central Atlantic Ocean - potential impacts

    NASA Astrophysics Data System (ADS)

    Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier van der Gon, H. A. C.

    2010-02-01

    Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates), natural (desert dust, sea salt) and chemically aged (sulphate and nitrate on dust) aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode) are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, designating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols indicates that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud and entrainment). The sodium (sea salt related) aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

  1. Hygroscopic and chemical characterisation of Po Valley aerosol

    NASA Astrophysics Data System (ADS)

    Bialek, J.; Dall Osto, M.; Vaattovaara, P.; Decesari, S.; Ovadnevaite, J.; Laaksonen, A.; O'Dowd, C.

    2014-02-01

    Continental summer-time aerosol in the Italian Po Valley was characterised in terms of hygroscopic properties and the influence of chemical composition therein. Additionally, the ethanol affinity of particles was analysed. The campaign-average minima in hygroscopic growth factors (HGFs, at 90% relative humidity) occurred just before and during sunrise from 03:00 to 06:00 LT (all data are reported in the local time), but, more generally, the hygroscopicity during the whole night is very low, particularly in the smaller particle sizes. The average HGFs recorded during the low HGF period were in a range from 1.18 (for the smallest, 35nm particles) to 1.38 (for the largest, 165 nm particles). During the day, the HGF gradually increased to achieve maximum values in the early afternoon hours 12:00-15:00, reaching 1.32 for 35 nm particles and 1.46 for 165 nm particles. Two contrasting case scenarios were encountered during the measurement period: Case 1 was associated with westerly air flow moving at a moderate pace and Case 2 was associated with more stagnant, slower moving air from the north-easterly sector. Case 1 exhibited weak diurnal temporal patterns, with no distinct maximum or minimum in HGF or chemical composition, and was associated with moderate non-refractory aerosol mass concentrations (for 50% size cut at 1 μ) of the order of 4.5 μg m-3. For Case 1, organics contributed typically 50% of the mass. Case 2 was characterised by >9.5 μg m-3 total non-refractory mass (<1 μ) in the early morning hours (04:00), decreasing to ~3 μg m-3 by late morning (10:00) and exhibited strong diurnal changes in chemical composition, particularly in nitrate mass but also in total organic mass concentrations. Specifically, the concentrations of nitrate peaked at night-time, along with the concentrations of hydrocarbon-like organic aerosol (HOA) and of semi-volatile oxygenated organic aerosol (SV-OOA). In general, organic growth factors (OGFs) followed a trend which was

  2. Contrasting the Evaporation and Condensation of Water from Glassy and Amorphous Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Reid, J. P.; Bones, D. L.; Power, R.; Lienhard, D.; Krieger, U. K.

    2012-04-01

    The partitioning of water between the condensed and gas phases in atmospheric aerosol is usually assumed to occur instantaneously and to be regulated by solution thermodynamics. However, the persistence of high viscosity, glassy and amorphous aerosol to low relative humidity without crystallisation occurring is now widely recognised, suggesting that the timescale for water transport to or from the particle during condensation or evaporation may be significant. A kinetic limitation on water transport could have important implications for understanding hygroscopic growth measurements made on ambient particles, the ability of particles to act as ice nuclei or cloud condensation nuclei, the kinetics of chemical aging/heterogeneous chemistry, and the rate or condensation/evaporation of semi-volatile organic components. In this study we will report on measurements of the timescale of water transport to and from glassy aerosol and ultra-high viscosity solution droplets using aerosol optical tweezers to investigate the time-response of single particles to changes in relative humidity. As a benchmark system, mixed component aerosol particles containing sucrose and sodium chloride have been used; varying the mole fractions of the two solutes allows a wide range of solution viscosities to be studied. We will show that coarse particles can take many thousands of seconds to equilibrate in size and that the timescale correlates with the estimated bulk viscosity of the particle. We will also confirm that significant inhomogeneities in particle composition can be established during evaporation or condensation. Using the experimental data to benchmark a model for equilibration time, predictions can be made of the timescale for the equilibration of accumulation mode particles during water condensation or evaporation and these predictions will be described and their significance explored. Finally, the coalescence dynamics of highly viscous aerosol particles will be reported

  3. New mass measurement method of aerosol particle using vibrating probe particle controlled by radiation pressure

    NASA Astrophysics Data System (ADS)

    Hariyama, Tatsuo; Takaya, Yasuhiro; Miyoshi, Takashi

    2005-11-01

    Aerosol particles with sub-micro meter size inhaled into respiratory systems cause serious damage to human body. In order to evaluate the health effects of the particles, classification methods of the particles with size and mass are needed. Several measurement methods of the particle size are established. However, conventional mass measurement methods are not enough to measure the particles with sub- pico gram. We propose a new mass measurement method of the aerosol particles based on laser trapping. In this method, an optically trapped silica particle is used as a measuring probe particle. The probe particle is trapped at a beam waist of the focused laser light and is forced to vibrate by deflecting the beam waist using AOD. The vibrating probe particle has a resonance frequency because it is governed by the spring-mass-damper system. When an aerosol particle is attached to the probe particle, the resonance frequency shifts according to the increase of the total mass. The mass of the aerosol particle can be measured from the shift of the resonance frequency. Experimentally, it is confirmed that the probe particle is governed by the spring-mass-damper system and has a resonance frequency. When a silica fine particle of 3pg in mass used as an aerosol particle is attached to the probe particle, the resonance frequency shift occurs as expected in the dynamic system and the fine particle mass can be measured based on the proposed method.

  4. 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.

  5. 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.

  6. Physical and chemical properties of aerosols at a coastal site Paposo (Chile) during VOCALS campaign

    NASA Astrophysics Data System (ADS)

    Cordova, A. M.; Chand, D.; Wood, R.; Wallace, D.; Hegg, D. A.; Shaw, G. E.; Krejci, R.; Fochesatto, G. J.; Gallardo, L.

    2009-12-01

    One of the primary goals of the VOCALS (VAMOS* Ocean-Cloud-Atmosphere-Land Study) Regional Experiment (REx) and associated modeling program is an improved understanding of aerosol indirect effects over the southeast Pacific (SEP). Details on the program are available online at www.eol.ucar.edu/projects/vocals/. To this end, detailed aerosol physical and chemical measurements were made during REx at a coastal land site at Paposo (25o 0.4' S, 70o 27.011' W, 690 masl) in northern Chile, a site ideally positioned for studying continental aerosol sources advecting over the SEP. We present initial analysis of data from Paposo. Detailed measurements of aerosol properties were made from mid October to mid November 2008. Observations from optical particle counters (OPC), nephelometers, aethalometer, scanning mobility particle sizer (SMPS) and the chemical analysis of the submicron aerosols samples collected on teflon filters are being used in this study. Large variations in aerosols parameters were observed which corresponded with changes in meteorology, as determined using trajectory analysis. Ion Chromatograph (IC) analysis of submicron aerosol samples shows that about 41% of submicron mass is sulfate. The light scattering coefficient shows a strong non-linear correlation with aerosol size observed using an OPC. Detailed results will be presented in the AGU meeting.

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

    PubMed

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

    2008-05-01

    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 degrees C are considered. Experimental observations indicate that when the reaction temperature is 1000 degrees C, submicron particles are produced, whereas the particle size is dominated by nanoscale for the temperature of 1400 degrees C. Thermogravimetric analysis of the aerosol particles stemming from the pyrolysis temperature of 1000 degrees 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 degrees C, the volatile- and weak-reaction stages almost merge together and evolve into a chemical-frozen stage. The submicron particles (i.e., 1000 degrees C) are mainly composed of volatiles, tar, and soot, with the main component of the nanoscale particles (i.e., 1400 degrees 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.

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

    PubMed

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

    2016-02-02

    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.

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

    SciTech Connect

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

    2014-03-06

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

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

    SciTech Connect

    Hallock, K.A.; Mazurek, M.A. ); Cass, G.R. . Dept. of Environmental Engineering Science)

    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.

  11. 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

  12. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  14. Mass spectrometric approaches for chemical characterisation of atmospheric aerosols: critical review of the most recent advances

    SciTech Connect

    Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.

    2012-06-29

    This manuscript presents an overview of the most recent instrument developments for the field and laboratory applications of mass spectrometry (MS) to investigate the chemistry and physics of atmospheric aerosols. A range of MS instruments, employing different sample introduction methods, ionisation and mass detection techniques are used both for ‘online’ and ‘offline’ characterisation of aerosols. Online MS techniques enable detection of individual particles with simultaneous measurement of particle size distributions and aerodynamic characteristics and are ideally suited for field studies that require high temporal resolution. Offline MS techniques provide a means for detailed molecular-level analysis of aerosol samples, which is essential to gain fundamental knowledge regarding aerosol chemistry, mechanisms of particle formation and atmospheric aging. Combined, complementary MS techniques provide comprehensive information on the chemical composition, size, morphology and phase of aerosols – data of key importance for evaluating hygroscopic and optical properties of particles, their health effects, understanding their origins and atmospheric evolution. Over the last few years, developments and applications of MS techniques in aerosol research have expanded remarkably as evident by skyrocketing publication statistics. Finally, the goal of this review is to present the most recent developments in the field of aerosol mass spectrometry for the time period of late 2010 to early 2012, which have not been conveyed in previous reviews.

  15. New apparatus of single particle trap system for aerosol visualization

    NASA Astrophysics Data System (ADS)

    Higashi, Hidenori; Fujioka, Tomomi; Endo, Tetsuo; Kitayama, Chiho; Seto, Takafumi; Otani, Yoshio

    2014-08-01

    Control of transport and deposition of charged aerosol particles is important in various manufacturing processes. Aerosol visualization is an effective method to directly observe light scattering signal from laser-irradiated single aerosol particle trapped in a visualization cell. New single particle trap system triggered by light scattering pulse signal was developed in this study. The performance of the device was evaluated experimentally. Experimental setup consisted of an aerosol generator, a differential mobility analyzer (DMA), an optical particle counter (OPC) and the single particle trap system. Polystylene latex standard (PSL) particles (0.5, 1.0 and 2.0 μm) were generated and classified according to the charge by the DMA. Singly charged 0.5 and 1.0 μm particles and doubly charged 2.0 μm particles were used as test particles. The single particle trap system was composed of a light scattering signal detector and a visualization cell. When the particle passed through the detector, trigger signal with a given delay time sent to the solenoid valves upstream and downstream of the visualization cell for trapping the particle in the visualization cell. The motion of particle in the visualization cell was monitored by CCD camera and the gravitational settling velocity and the electrostatic migration velocity were measured from the video image. The aerodynamic diameter obtained from the settling velocity was in good agreement with Stokes diameter calculated from the electrostatic migration velocity for individual particles. It was also found that the aerodynamic diameter obtained from the settling velocity was a one-to-one function of the scattered light intensity of individual particles. The applicability of this system will be discussed.

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

    SciTech Connect

    Meskhidze, Nicholas

    2013-10-21

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

  17. Isotope Analysis of Individual Aerosol Particles - a New Tool for Studying Heterogeneous Processes

    NASA Astrophysics Data System (ADS)

    Winterholler, B.; Hoppe, P.; Huth, J.; Andreae, M. O.; Foley, S.

    2006-12-01

    Sources of atmospheric sulfur and its oxidation pathways are studied by isotope analysis of sulfate particles. conventional gas mass spectrometry averages the isotopic compositions of millions of aerosol grains and, therefore, several different types of sulphur aerosol. The new Cameca NanoSIMS 50 ion microprobe technique permits isotope analyses of individual aerosol particles down to 0.5 μm diameter. Combining the chemical composition and isotopic signature of individual particles enables source apportionment of non-sea-salt (nss) sulfate and elucidating mixing processes between nss sulfate and sea-salt sulfate for each sample. Results from aerosol samples collected in Mace Head (Western Ireland) are presented. These samples represent different airmass types, such as clean marine boundary layer air, moderately polluted air and strongly polluted air transported from the continent. Fresh aerosol preserves the original isotopic signature of sea-salt and nss sulfate in separate particles, the latter being present predominantly in the form of ammonium sulfate. This enables us to identify oxidation of nss sulfate in deliquescent sea salt particles by means of their sulfur isotope ratio. Cloud processing however, leads to a complete homogenization as far as the sulfur isotopic signature is concerned.

  18. Detection of cw-related species in complex aerosol particles deposited on surfaces with an ion trap-based aerosol mass spectrometer

    SciTech Connect

    Harris, William A; Reilly, Pete; Whitten, William B

    2007-01-01

    A new type of aerosol mass spectrometer was developed by minimal modification of an existing commercial ion trap to analyze the semivolatile components of aerosols in real time. An aerodynamic lens-based inlet system created a well-collimated particle beam that impacted into the heated ionization volume of the commercial ion trap mass spectrometer. The semivolatile components of the aerosols were thermally vaporized and ionized by electron impact or chemical ionization in the source. The nascent ions were extracted and injected into the ion trap for mass analysis. The utility of this instrument was demonstrated by identifying semivolatile analytes in complex aerosols. This study is part of an ongoing effort to develop methods for identifying chemical species related to CW agent exposure. Our efforts focused on detection of CW-related species doped on omnipresent aerosols such as house dust particles vacuumed from various surfaces found in any office building. The doped aerosols were sampled directly into the inlet of our mass spectrometer from the vacuumed particle stream. The semivolatile analytes were deposited on house dust and identified by positive ion chemical ionization mass spectrometry up to 2.5 h after deposition. Our results suggest that the observed semivolatile species may have been chemisorbed on some of the particle surfaces in submonolayer concentrations and may remain hours after deposition. This research suggests that identification of trace CW agent-related species should be feasible by this technique.

  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. 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

  1. 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.

  2. Total reflection X-ray fluorescence (TXRF) for direct analysis of aerosol particle samples.

    PubMed

    Bontempi, E; Zacco, A; Benedetti, D; Borgese, L; Colombi, P; Stosnach, H; Finzi, G; Apostoli, P; Buttini, P; Depero, L E

    2010-04-14

    Atmospheric aerosol particles have a great impact on the environment and on human health. Routine analysis of the particles usually involves only the mass determination. However, chemical composition and phases provide fundamental information about the particles' origins and can help to prevent health risks. For example, these particles may contain heavy metals such as Pb, Ni and Cd, which can adversely affect human health. In this work, filter samples were collected in Brescia, an industrial town located in Northern Italy. In order to identify the chemical composition and the phases of the atmospheric aerosols, the samples were analysed by means of total reflection X-ray fluorescence (TXRF) spectrometry with a laboratory instrument and X-ray microdiffraction at Synchrotron Daresbury Laboratories, Warrington (Cheshire, UK). The results are discussed and correlated to identify possible pollution sources. The novelty of this analytical approach is that filter samples for TXRF were analysed directly and did not require chemical pretreatment to leach elements from the aerosol particulates. The results of this study clearly show that TXRF is a powerful technique for the analysis of atmospheric aerosols on 'as-received' filters, thereby leaving samples intact and unaltered for possible subsequent analyses by other methods. In addition, the low detection limits for many elements (low ng/cm2) indicate that this method may hold promise in various application fields, such as nanotechnology.

  3. Hygroscopic and chemical characterisation of Po Valley aerosol

    NASA Astrophysics Data System (ADS)

    Bialek, J.; Dall'Osto, M.; Vaattovaara, P.; Ovadnevaite, J.; Decesari, S.; Laaksonen, A.; O'Dowd, C.

    2013-02-01

    Continental summer-time aerosol in the Italian Po Valley was characterized in terms of hygroscopic properties and the influence of chemical composition therein. The campaign-average minima in hygroscopic growth factors (HGFs) occurred just before and during sunrise from 03:00-06:00, but more generally, the whole night shows very low hygroscopicity, particularly in the smaller particle sizes. The average HGFs increased from 1.18 for the smallest sized particles (35 nm) to 1.38 for the largest sizes (165 nm) for the lowest HGF period while during the day, the HGF gradually increased to achieve maximum values in the early afternoon hours from 12:00-15:00, reaching 1.32 for 35 nm particles and 1.46 for 165 nm particles. Two contrasting case scenarios were encountered during the measurement period: Case 1 was associated with westerly air flow moving at a moderate pace and Case 2 was associated with more stagnant, slower moving air from the north-easterly sector. Case 1 exhibited low diurnal temporal patterns and was associated with moderate non-refractory aerosol mass concentrations (for 50% size cut at 1 μm) of the order of 4.5 μg m-3. For Case 1, organics contributed typically to 50% of the mass. Case 2 was characterized by > 9.5 μg m-3 total mass (< 1 μm) in the early morning hours (04:00), decreasing to ∼ 3 μg m-3 by late morning (10:00) and exhibited strong diurnal changes in chemical composition, particularly in nitrate mass but also in total organic mass concentrations. Organic growth factors (OGFs) exhibited a minimum around 15:00, 1-2 h after the peak in HGF. Particles sized 165 nm exhibited moderate diurnal variability in HGF, ranging from 80% at night to 95% of "more hygroscopic" growth factors (i.e. GF = 1.35-1.9) around noon. The diurnal changes in HGF progressively became enhanced with decreasing particle size, decreasing from 95% "more hygroscopic" growth factor fraction at noon to 10% fraction at midnight, while the "less hygroscopic" growth

  4. MEASUREMENTS OF BLACK CARBON PARTICLES CHEMICAL, PHYSICAL, AND OPTICAL PROPERTIES

    SciTech Connect

    Onasch, T.B.; Sedlacek, A.; Cross, E. S.; Davidovits, P.; Worsnop, D. R.; Ahern, A.; Lack, D. A.; Cappa, C. D.; Trimborn, A.; Freedman, A.; Olfert, J. S.; Jayne, J. T.; Massoli, P.; Williams, L. R.; Mazzoleni, C.; Schwarz, J. P.; Thornhill, D. A.; Slowik, J. G.; Kok, G. L.; Brem, B. T.; Subramanian, R.; Spackman, J. R.; Freitag, S.; and Dubey, M. K.

    2009-12-14

    Accurate measurements of the chemical, physical, and optical properties of aerosol particles containing black carbon are necessary to improve current estimates of the radiative forcing in the atmosphere. A collaborative research effort between Aerodyne Research, Inc. and Boston College has focused on conducting field and laboratory experiments on carbonaceous particles and the development and characterization of new particulate instrumentation. This presentation will focus on the chemical, physical, and optical properties of black carbon particles measured in the laboratory in order to understand the effects of atmospheric processing on black carbon particles. Results from a three-week study during July 2008 of mass- and optical-based black carbon measurements will be presented. The project utilized the Boston College laboratory flame apparatus and aerosol conditioning and characterization equipment. A pre-mixed flat flame burner operating at controlled fuel-to-air ratios produced stable and reproducible concentrations of soot particles with known sizes, morphologies, and chemical compositions. In addition, other black carbon particle types, including fullerene soot, glassy carbon spheres, oxidized flame soot, Regal black, and Aquadag, were also atomized, size selected, and sampled. The study covered an experimental matrix that systematically selected particle mobility size (30 to 300 nm) and black carbon particle mass, particle number concentration, particle shape (dynamic shape factor and fractal dimension), and particle chemistry and density (changed via coatings). Particles were coated with a measured thickness (few nm to {approx}150 nm) of sulfuric acid or bis (2-ethylhexyl) sebacate and passed through a thermal denuder to remove the coatings. Highlights of the study to be presented include: (1) Characterization of the chemical and physical properties of various types of black carbon particles, (2) Mass specific absorption measurements as a function of fuel

  5. Aerosol particle microphotography and glare-spot absorption spectroscopy.

    PubMed

    Arnold, S; Holler, S; Li, J H; Serpengüzel, A; Auffermann, W F; Hill, S C

    1995-04-01

    The relative intensities of glare spots in the image of an electrodynamically trapped aerosol droplet are measured experimentally with an aerosol particle microscope and calculated theoretically. The theoretical calculations are in good agreement with these experiments and indicate that the intensities of these spots are extremely sensitive to the imaginary part of the refractive index. Experimentally, we obtain the molecular absorption spectrum of an impurity within a droplet by recording the spectrum of an individual glare spot produced by broadband illumination.

  6. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2012-03-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2012-09-01

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

  9. The generation of diesel exhaust particle aerosols from a bulk source in an aerodynamic size range similar to atmospheric particles

    PubMed Central

    Cooney, Daniel J; Hickey, Anthony J

    2008-01-01

    The influence of diesel exhaust particles (DEP) on the lungs and heart is currently a topic of great interest in inhalation toxicology. Epidemiological data and animal studies have implicated airborne particulate matter and DEP in increased morbidity and mortality due to a number of cardiopulmonary diseases including asthma, chronic obstructive pulmonary disorder, and lung cancer. The pathogeneses of these diseases are being studied using animal models and cell culture techniques. Real-time exposures to freshly combusted diesel fuel are complex and require significant infrastructure including engine operations, dilution air, and monitoring and control of gases. A method of generating DEP aerosols from a bulk source in an aerodynamic size range similar to atmospheric DEP would be a desirable and useful alternative. Metered dose inhaler technology was adopted to generate aerosols from suspensions of DEP in the propellant hydrofluoroalkane 134a. Inertial impaction data indicated that the particle size distributions of the generated aerosols were trimodal, with count median aerodynamic diameters less than 100 nm. Scanning electron microscopy of deposited particles showed tightly aggregated particles, as would be expected from an evaporative process. Chemical analysis indicated that there were no major changes in the mass proportion of 2 specific aromatic hydrocarbons (benzo[a]pyrene and benzo[k]fluoranthene) in the particles resulting from the aerosolization process. PMID:19337412

  10. Size-dependent chemical ageing of oleic acid aerosol under dry and humidified conditions

    NASA Astrophysics Data System (ADS)

    Al-Kindi, Suad S.; Pope, Francis D.; Beddows, David C.; Bloss, William J.; Harrison, Roy M.

    2016-12-01

    A chemical reaction chamber system has been developed for the processing of oleic acid aerosol particles with ozone under two relative humidity conditions: dry and humidified to 65 %. The apparatus consists of an aerosol flow tube, in which the ozonolysis occurs, coupled to a scanning mobility particle sizer (SMPS) and an aerosol time-of-flight mass spectrometer (ATOFMS) which measure the evolving particle size and composition. Under both relative humidity conditions, ozonolysis results in a significant decrease in particle size and mass which is consistent with the formation of volatile products that partition from the particle to the gas phase. Mass spectra derived from the ATOFMS reveal the presence of the typically observed reaction products: azelaic acid, nonanal, oxononanoic acid and nonanoic acid, as well as a range of higher molecular weight products deriving from the reactions of reaction intermediates with oleic acid and its oxidation products. These include octanoic acid and 9- and 10-oxooctadecanoic acid, as well as products of considerably higher molecular weight. Quantitative evaluation of product yields with the ATOFMS shows a marked dependence upon both particle size association (from 0.3 to 2.1 µm diameter) and relative humidity. Under both relative humidity conditions, the percentage residual of oleic acid increases with increasing particle size and the main lower molecular weight products are nonanal and oxononanoic acid. Under dry conditions, the percentage of higher molecular weight products increases with increasing particle size due to the poorer internal mixing of the larger particles. Under humidified conditions, the percentage of unreacted oleic acid is greater, except in the smallest particle fraction, with little formation of high molecular weight products relative to the dry particles. It is postulated that water reacts with reactive intermediates, competing with the processes which produce high molecular weight products. Whilst the

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  12. Composition of carbonaceous smoke particles from prescribed burning of a Canadian boreal forest: 1. Organic aerosol characterization by gas chromatography

    SciTech Connect

    Mazurek, M.A.; Laterza, C.; Newman, L.; Daum, P.; Cofer, W.R. III; Levine, J.S.; Winstead, E.L.

    1995-06-01

    In this study we examine the molecular organic constituents (C8 to C40 lipid compounds) collected as smoke particles from a Canadian boreal forest prescribed burn. Of special interest are (1) the molecular identity of polar organic aerosols, and (2) the amount of polar organic matter relative to the total mass of aerosol particulate carbon. Organic extracts of smoke aerosol particles show complex distributions of the lipid compounds when analyzed by capillary gas chromatography/mass spectrometry. The molecular constituents present as smoke aerosol are grouped into non-polar (hydrocarbons) and polar {minus}2 oxygen atoms) subtractions. The dominant chemical species found in the boreal forest smoke aerosol are unaltered resin compounds (C20 terpenes) which are abundant in unburned conifer wood, plus thermally altered wood lignins and other polar aromatic hydrocarbons. Our results show that smoke aerosols contain molecular tracers which are related to the biofuel consumed. These smoke tracers can be related structurally back to the consumed softwood and hardwood vegetation. In addition, combustion of boreal forest materials produces smoke aerosol particles that are both oxygen-rich and chemically complex, yielding a carbonaceous aerosol matrix that is enriched in polar substances. As a consequence, emissions of carbonaceous smoke particles from large-scale combustion of boreal forest land may have a disproportionate effect on regional atmospheric chemistry and on cloud microphysical processes.

  13. Chemical mechanisms governing atmospheric new particle formation

    NASA Astrophysics Data System (ADS)

    Bzdek, Bryan Richard

    The goal of this dissertation is to understand the chemistry that governs new particle formation, a ubiquitous and important atmospheric process. New particle formation occurs when gas phase precursors condense to create small molecular clusters on the order of 1 nm diameter. Those clusters must then grow rapidly and ultimately may serve as the seeds for cloud droplets. However, modelers have substantial difficulty predicting the frequency and efficiency of new particle formation. This predictive difficulty is an important contributor to the uncertainty in aerosol effects on global climate and therefore also contributes to the large uncertainty in anthropogenic effects on climate. To reduce these uncertainties, a more precise understanding of how particles nucleate and grow in the atmospheric is required. In this dissertation, mass spectrometry is used to determine the chemical processes involved in new particle formation. Gas phase species such as sulfuric acid, ammonia, amines, and organic matter are contributors but exactly how and how much each contributes to the growth of nanoparticles is not well understood. Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) and Nano Aerosol Mass Spectrometry (NAMS) are used to study the chemical composition and reactivity of clusters < 3 nm diameter and nanoparticles 10-20 nm diameter, respectively. The FTICR-MS studies are laboratory based, whereas the NAMS studies are field based. Measurements of cluster composition and reactivity using FTICR-MS permit prediction of the composition of ambient molecular clusters. For ambient molecular clusters to become relevant to climate by serving as cloud condensation nuclei, they must grow rapidly. NAMS measurements at 20 nm diameter permit determination of nanoparticle growth pathways. This dissertation shows that sulfuric acid adds to both clusters and nanoparticles in a collision limited manner. On the other hand, ammonia uptake in both size regimes may not

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  15. Impacts of new particle formation on aerosol cloud condensation nuclei (CCN) activity in Shanghai: case study

    NASA Astrophysics Data System (ADS)

    Leng, C.; Zhang, Q.; Zhang, D.; Zhang, H.; Xu, C.; Li, X.; Kong, L.; Tao, J.; Cheng, T.; Zhang, R.; Chen, J.; Qiao, L.; Lou, S.; Wang, H.; Chen, C.

    2014-07-01

    New particle formation (NPF) events and their impacts on cloud condensation nuclei (CCN) were investigated using continuous measurements collected in urban Shanghai from 1 to 30 April 2012. During the campaign, NPF occurred in 8 out of the 30 days and enhanced CCN number concentration (NCCN) by a actor of 1.2-1.8, depending on supersaturation (SS). The NPF event on 3 April 2012 was chosen as an example to investigate the NPF influence on CCN activity. In this NPF event, secondary aerosols were produced continuously and increased PM2.5 mass concentration at a~rate of 4.33 μg cm-3 h-1, and the growth rate (GR) and formation rate (FR) were on average 5 nm h-1 and 0.36 cm-3 s-1, respectively. The newly formed particles grew quickly from nucleation mode (10-20 nm) into CCN size range. NCCN increased rapidly at SS of 0.4-1.0% but weakly at SS of 0.2%. Correspondingly, aerosol CCN activities (fractions of activated aerosol particles in total aerosols, NCCN / NCN) were significantly enhanced from 0.24-0.60 to 0.30-0.91 at SS of 0.2-1.0% due to the NPF. On the basis of the κ-Köhler theory, aerosol size distributions and chemical composition measured simultaneously were used to predict NCCN. There was a good agreement between the predicted and measured NCCN (R2 = 0.96, Npredicted / Nmeasured = 1.04). This study reveals that NPF exerts large impacts on aerosol particle abundance and size spectra, thus significantly promotes NCCN and aerosol CCN activity in this urban environment. The GR of NPF is the key factor controlling the newly formed particles to become CCN at all SS levels, whereas the FR is an effective factor only under high SS (e.g. 1.0%) conditions.

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

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

    Modelling aerosol optical properties is a notoriously difficult task due to the particles' complex morphologies and compositions. Yet aerosols and their optical properties are important for Earth system modelling and remote sensing applications. Operational optics models often make drastic and non realistic approximations regarding morphological properties, which can introduce errors. In this study a new aerosol optics model is implemented, in which more realistic morphologies and mixing states are assumed, especially for black carbon aerosols. The model includes both external and internal mixing of all chemical species, it treats externally mixed black carbon as fractal aggregates, and it accounts for inhomogeneous internal mixing of black carbon by use of a novel "core-grey shell" model. Simulated results of radiative fluxes, backscattering coefficients and the Ångström exponent from the new optics model are compared with results from another model simulating particles as externally mixed homogeneous spheres. To gauge the impact on the optical properties from the new optics model, the known and important effects from using aerosol dynamics serves as a reference. The results show that using a more detailed description of particle morphology and mixing states influences the optical properties to the same degree as aerosol dynamics. This is an important finding suggesting that over-simplified optics models coupled to a chemical transport model can introduce considerable errors; this can strongly effect simulations of radiative fluxes in Earth-system models, and it can compromise the use of remote sensing observations of aerosols in model evaluations and chemical data assimilation.

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

    NASA Astrophysics Data System (ADS)

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

    2014-07-01

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

  18. 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

  19. Anthropogenic monoterpene pollution episodes in a forest environment in association with aerosol particles

    NASA Astrophysics Data System (ADS)

    Liao, L.; Taipale, R.; Dal Maso, M.; Ehn, M.; Junninen, H.; Nieminen, T.; Kerminen, V.; Kulmala, M. T.

    2010-12-01

    Monoterpenes (MT) present in troposphere affect atmospheric chemistry and air quality. The oxidation of monoterpenes leading to secondary organic aerosol formation can affect aerosol loadings, and further influence the climate system. Identified sources of MT include biogenic and anthropogenic origins. In this study, we present a four-year set observation of MT to examine: 1. the origin and the quantification of elevated MT concentrations. 2. The influence of enhanced MT emissions on local air chemistry and possible associated pollutants. 3. Possible influence of anthropogenic MT emissions on physical and chemical properties of enhanced aerosol particles. VOC observations were continuously con-ducted using a PTR-MS from Jun. 12 2006 to Sep. 24 2007 and from Jun. 1 2008 to Mar. 3 2009. As an example, MT observed on March 8, 2007 are plotted in Figure 1 along with DMPS. The DMPS spectra show simultaneous elevations of Aitken-mode particles seen as red colors when monoterpenes are dramatically elevated during six short periods on this day. Out of the four-year dataset amounting to 580 days in total, 27.4% of the days showed MT pollution episodes. The sum of the total episode durations is equal to 3.62% time of the whole PTR-MS measurement period. The average concentration of MT was increased from 0.205 to 0.270 ppbv, which roughly results in 32% overestimation of biogenic MT without considering the influence of these anthropogenic emissions. The origin of episodes is mainly from the Korkeakoski sawmill which is ca. 6 km away from the SMEAR II station and 130 degrees South East direction. VOCs are the main pollutants from sawmill. We did not see clear connections between MT and other gas pollutants during MT episodes. The case studies have shown that other associated pollutants may be occasionally emitted. The strong link between anthropogenic MT and aerosol particles suggest that sawmills could be a main source of anthropogenic VOCs, as well as aerosol loading at the

  20. 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.

  1. REDOX AND ELECTROPHILIC PROPERTIES OF VAPOR- AND PARTICLE-PHASE COMPONENTS OF AMBIENT AEROSOLS

    PubMed Central

    Eiguren-Fernandez, Arantzazu; Shinyashiki, Masaru; Schmitz, Debra A.; DiStefano, Emma; Hinds, William; Kumagai, Yoshito; Cho, Arthur K.; Froines, John R.

    2010-01-01

    Particulate matter (PM) has been the primary focus of studies aiming to understand the relationship between the chemical properties of ambient aerosols and adverse health effects. Size and chemical composition of PM have been linked to their oxidative capacity which has been postulated to promote or exacerbate pulmonary and cardiovascular diseases. But in the last few years, new studies have suggested that volatile and semivolatile components may also contribute to many adverse health effects. The objectives of this study were: i) assess for the first time the redox and electrophilic potential of vapor-phase components of ambient aerosols, and ii) evaluate the relative contributions of particle- and vapor-fractions to the hazard of a given aerosol. To achieve these objectives vapor- and particle-phase samples collected in Riverside (CA) were subjected to three chemical assays to determine their redox and electrophilic capacities. The results indicate that redox active components are mainly associated with the particle-phase, while electrophilic compounds are found primarily in the vapor-phase. Vapor-phase organic extracts were also capable of inducing the stress responding protein, heme-oxygenase-1 (HO-1), in RAW264.7 murine macrophages. These results demonstrate the importance of volatile components in the overall oxidative and electrophilic capacity of aerosols, and point out the need for inclusion of vapors in future health and risk assessment studies. PMID:20152964

  2. Measurements of Sea Salt Aerosols in the Marine Boundary Layer and Free Troposphere: Vertical Transport and Chemical Transformation

    NASA Astrophysics Data System (ADS)

    Hudson, P. K.; Murphy, D. M.; Cziczo, D. J.; Thomson, D. S.

    2002-12-01

    During the Intercontinental Transport and Chemical Transformation (ITCT) mission (Monterey, CA, spring 2002) nearly 400,000 positive and negative mass spectra of single atmospheric aerosols were acquired using the PALMS (Particle Analysis by Laser Mass Spectrometry) instrument. The primary focus of the mission was to investigate the composition of air masses along the western coast of the United States. Of particular interest to the mission was to study the influence of anthropogenic emissions from Asia on aerosol composition. To accomplish these goals, the WP-3 aircraft, equipped with a suite of instruments including PALMS, covered a large spatial area flying from 0 - 8000 m altitude covering most of the western coastline from Canada to southern California including flights over the San Francisco and Los Angeles metropolitan areas. The in situ measurements of single particle aerosol mass spectra by PALMS allow for good spatial and vertical resolution of the aerosol composition. By observing the changes in aerosol composition as a function of altitude, the vertical transport of sea salt aerosols over marine and urban environments is examined. Using measurements of other chemical tracers along with the aerosol composition, the chemical processing of these aerosols during transport both vertically and inland can be discerned. These results add insight into the transport and chemical evolution of sea salt aerosol.

  3. Heterogeneous particle deaggregation and its implication for therapeutic aerosol performance.

    PubMed

    Xu, Zhen; Mansour, Heidi M; Mulder, Tako; McLean, Richard; Langridge, John; Hickey, Anthony J

    2010-08-01

    Aerosolization performance of dry powder blends of drugs for the treatment of asthma or chronic obstructive pulmonary diseases have been reported in three previous articles. In vitro aerosolization was performed at defined shear stresses (0.624-13.143 N/m(2)). Formulations were characterized aerodynamically and powder aerosol deaggregation equations (PADE) and corresponding linear regression analyses for pharmaceutical aerosolization were applied. Particle deaggregation is the result of overcoming fundamental forces acting at the particle interface. A new method, PADE, describing dry powder formulation performance in a shear stress range has been developed which may allow a fundamental understanding of interparticulate and surface forces. The application of PADE predicts performance efficiency and reproducibility and supports rational design of dry powder formulations. The analogy of aerosol performance with surface molecular adsorption has important implications. Expressions describing surface adsorption were intended to allow elucidation of mechanisms involving surface heterogeneity, lateral interaction, and multilayer adsorption of a variety of materials. By using a similar expression for drug aerosolization performance, it is conceivable that an analogous mechanistic approach to the evaluation of particulate systems would be possible.

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

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

    SciTech Connect

    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.

  6. Parameterization of Aerosol Sinks in Chemical Transport Models

    NASA Technical Reports Server (NTRS)

    Colarco, Peter

    2012-01-01

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

  7. 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.

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

    SciTech Connect

    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; Yoder, Richard; Wheeler, Elizabeth K.; Farquar, George R.

    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 use 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.

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

    DOE PAGES

    Harding, Ruth N.; Hara, Christine A.; Hall, Sara B.; ...

    2016-03-22

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

  10. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  12. 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

  13. Individual-Particle Analysis of Aerosols From Southern Africa

    NASA Astrophysics Data System (ADS)

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

    2001-12-01

    Aerosol samples were collected on the University of Washington Convair-580 research aircraft over southern Africa during the Safari 2000 Experiment. Individual aerosol particles were analyzed using transmission electron microscopy (TEM) and field-emission scanning electron microscopy (FESEM) with energy-dispersive x-ray spectrometry (EDS). The objective of the study is to characterize the major aerosol emissions from biomass burning over southern Africa, with emphasis on the sizes, shapes, compositions, mixing states, and surface coatings of the aerosols. Aging and reaction of smoke aerosols with plume transport were investigated. Particulate emissions from combustion of different vegetation types and at different burning phases were compared. Preliminary results show that aerosols from biomass burning mainly consist of amorphous carbonaceous spherules ("tar balls"); soot; K salts including KCl, K2SO4, and probably KNO3 mixed with organic particles; and Ca-bearing particles including Ca carbonate, phosphate, and sulfate. Minor amounts of sea salt and minerals such as quartz, mica, smectite, and gypsum are also present. The relative concentrations of tar balls increase with distance from the fires. More KCl particles occur in fresh smoke plumes close to fire sources, whereas more K2SO4 and KNO3 particles are present in aged smoke. This change indicates that KCl forming from the fire was converted to K2SO4 and KNO3 through reactions with S- and N-bearing species emitted from biomass burning. The conversion of KCl resembles that of NaCl in sea salt particles, suggesting similar reaction mechanisms with the aging of smoke. More soot is present in smoke from flaming grass fires than bush and wood fires, which is probably related to the high fraction of flaming combustion of grass fires. The high abundance of organic particles and soluble salt may affect the hygroscopic properties of biomass burning aerosols and influence their role as cloud condensation nuclei

  14. Dimethylsulfide/cloud condensation nuclei/climate system - Relevant size-resolved measurements of the chemical and physical properties of atmospheric aerosol particles

    NASA Technical Reports Server (NTRS)

    Quinn, P. K.; Covert, D. S.; Bates, T. S.; Kapustin, V. N.; Ramsey-Bell, D. C.; Mcinnes, L. M.

    1993-01-01

    The mass and number relationships occurring within the atmospheric dimethylsulfide/cloud condensation nuclei (CCN)/climate system, using simultaneous measurements of particulate phase mass size distributions of nss SO4(2-), methanesulfonic acid (MSA), and NH4(+); number size distributions of particles having diameters between 0.02 and 9.6 microns; CCN concentrations at a supersaturation of 0.3 percent; relative humidity; and temperature, obtained for the northeastern Pacific Ocean in April and May 1991. Based on these measurements, particulate nss SO4(2-), MSA, and NH4(+) mass appeared to be correlated with both particle effective surface area and number in the accumulation mode size range (0.16 to 0.5 micron). No correlations were found in the size range below 0.16 micron. A correlation was also found between nss SO4(2-) mass and the CCN number concentration, such that a doubling of the SO4(2-) mass corresponded to a 40 percent increase in the CCN number concentration. However, no correlation was found between MSA mass and CCN concentration.

  15. Improved Tandem Measurement Techniques for Aerosol Particle Analysis

    NASA Astrophysics Data System (ADS)

    Rawat, Vivek Kumar

    Non-spherical, chemically inhomogeneous (complex) nanoparticles are encountered in a number of natural and engineered environments, including combustion systems (which produces highly non-spherical aggregates), reactors used in gas-phase materials synthesis of doped or multicomponent materials, and in ambient air. These nanoparticles are often highly diverse in size, composition and shape, and hence require determination of property distribution functions for accurate characterization. This thesis focuses on development of tandem mobility-mass measurement techniques coupled with appropriate data inversion routines to facilitate measurement of two dimensional size-mass distribution functions while correcting for the non-idealities of the instruments. Chapter 1 provides the detailed background and motivation for the studies performed in this thesis. In chapter 2, the development of an inversion routine is described which is employed to determine two dimensional size-mass distribution functions from Differential Mobility Analyzer-Aerosol Particle Mass analyzer tandem measurements. Chapter 3 demonstrates the application of the two dimensional distribution function to compute cumulative mass distribution function and also evaluates the validity of this technique by comparing the calculated total mass concentrations to measured values for a variety of aerosols. In Chapter 4, this tandem measurement technique with the inversion routine is employed to analyze colloidal suspensions. Chapter 5 focuses on application of a transverse modulation ion mobility spectrometer coupled with a mass spectrometer to study the effect of vapor dopants on the mobility shifts of sub 2 nm peptide ion clusters. These mobility shifts are then compared to models based on vapor uptake theories. Finally, in Chapter 6, a conclusion of all the studies performed in this thesis is provided and future avenues of research are discussed.

  16. Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles

    SciTech Connect

    Lin, Peng; Aiona, Paige K.; Li, Ying; Shiraiwa, Manabu; Laskin, Julia; Nizkorodov, Sergey A.; Laskin, Alexander

    2016-11-01

    Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly-emitted biomass burning organic aerosol (BBOA) samples collected during test burns of selected biomass fuels: sawgrass, peat, ponderosa pine, and black spruce. We characterize individual BrC chromophores present in these samples using high performance liquid chromatography coupled to a photodiode array detector and a high-resolution mass spectrometer. We demonstrate that both the overall BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels and burning conditions. Common BrC chromophores in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as potential markers of BrC originating from different biomass burning sources. On average, ~50% of the light absorption above 300 nm can be attributed to a limited number of strong BrC chromophores, which may serve as representative light-absorbing species for studying atmospheric processing of BrC aerosol. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of 16 hours. A “molecular corridors” analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low volatility (<1 g m-1) and will be retained in the particle phase under atmospherically relevant conditions.

  17. Development of the RAQM2 aerosol chemical transport model and predictions of the Northeast Asian aerosol mass, size, chemistry, and mixing type

    NASA Astrophysics Data System (ADS)

    Kajino, M.; Inomata, Y.; Sato, K.; Ueda, H.; Han, Z.; An, J.; Katata, G.; Deushi, M.; Maki, T.; Oshima, N.; Kurokawa, J.; Ohara, T.; Takami, A.; Hatakeyama, S.

    2012-12-01

    A new aerosol chemical transport model, the Regional Air Quality Model 2 (RAQM2), was developed to simulate the Asian air quality. We implemented a simple version of a triple-moment modal aerosol dynamics model (MADMS) and achieved a completely dynamic (non-equilibrium) solution of a gas-to-particle mass transfer over a wide range of aerosol diameters from 1 nm to super-μm. To consider a variety of atmospheric aerosol properties, a category approach was utilized in which the aerosols were distributed into four categories: particles in the Aitken mode (ATK), soot-free particles in the accumulation mode (ACM), soot aggregates (AGR), and particles in the coarse mode (COR). The aerosol size distribution in each category is characterized by a single mode. The condensation, evaporation, and Brownian coagulations for each mode were solved dynamically. A regional-scale simulation (Δx = 60 km) was performed for the entire year of 2006 covering the Northeast Asian region. The modeled PM1/bulk ratios of the chemical components were consistent with observations, indicating that the simulated aerosol mixing types were consistent with those in nature. The non-sea-salt SO42- mixed with ATK + ACM was the largest at Hedo in summer, whereas the SOSO42- was substantially mixed with AGR in the cold seasons. Ninety-eight percent of the modeled NO3- was mixed with sea salt at Hedo, whereas 53.7% of the NO3- was mixed with sea salt at Gosan, which is located upwind toward the Asian continent. The condensation of HNO3 onto sea salt particles during transport over the ocean accounts for the difference in the NO3- mixing type at the two sites. Because the aerosol mixing type alters the optical properties and cloud condensation nuclei activity, its accurate prediction and evaluation are indispensable for aerosol-cloud-radiation interaction studies.

  18. 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

  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. Aerosol physical, chemical and optical properties observed in the ambient atmosphere during haze pollution conditions

    NASA Astrophysics Data System (ADS)

    Li, Zhengqiang; Xie, Yisong; Li, Donghui; Li, Kaitao; Zhang, Ying; Li, Li; Lv, Yang; Qie, Lili; Xu, Hua

    Aerosol’s properties in the ambient atmosphere may differ significantly from sampling results due to containing of abundant water content. We performed sun-sky radiometer measurements in Beijing during 2011 and 2012 winter to obtain distribution of spectral and angular sky radiance. The measurements are then used to retrieve aerosol physical, chemical and optical properties, including single scattering albedo, size distribution, complex refractive indices and aerosol component fractions identified as black carbon, brown carbon, mineral dust, ammonium sulfate-like components and water content inside particle matters. We found that during winter haze condition aerosol is dominated by fine particles with center radius of about 0.2 micron. Fine particles contribute about 93% to total aerosol extinction of solar light, and result in serious decrease of atmospheric visibility during haze condition. The percentage of light absorption of haze aerosol can up to about 10% among its total extinction, much higher than that of unpolluted conditions, that causes significant radiative cooling effects suppressing atmospheric convection and dispersion of pollutants. Moreover, the average water content occupies about one third of the ambient aerosol in volume which suggests the important effect of ambient humidity in the formation of haze pollution.

  1. Magnetic targeting of aerosol particles for cancer therapy

    NASA Astrophysics Data System (ADS)

    Ally, Javed; Martin, Benjamin; Behrad Khamesee, Mir; Roa, Wilson; Amirfazli, Alidad

    2005-05-01

    An in vitro model was developed to study and demonstrate the potential and feasibility of magnetically targeted deposition of aerosols for potential applications in lung cancer treatment. Also, a numerical particle tracing model was developed to predict the targeting behavior of the in vitro system; the results from the numerical and experimental studies were in agreement.

  2. Single particle mass spectral signatures from vehicle exhaust particles and the source apportionment of on-line PM2.5 by single particle aerosol mass spectrometry.

    PubMed

    Yang, Jian; Ma, Shexia; Gao, Bo; Li, Xiaoying; Zhang, Yanjun; Cai, Jing; Li, Mei; Yao, Ling'ai; Huang, Bo; Zheng, Mei

    2017-03-24

    In order to accurately apportion the many distinct types of individual particles observed, it is necessary to characterize fingerprints of individual particles emitted directly from known sources. In this study, single particle mass spectral signatures from vehicle exhaust particles in a tunnel were performed. These data were used to evaluate particle signatures in a real-world PM2.5 apportionment study. The dominant chemical type originating from average positive and negative mass spectra for vehicle exhaust particles are EC species. Four distinct particle types describe the majority of particles emitted by vehicle exhaust particles in this tunnel. Each particle class is labeled according to the most significant chemical features in both average positive and negative mass spectral signatures, including ECOC, NaK, Metal and PAHs species. A single particle aerosol mass spectrometry (SPAMS) was also employed during the winter of 2013 in Guangzhou to determine both the size and chemical composition of individual atmospheric particles, with vacuum aerodynamic diameter (dva) in the size range of 0.2-2μm. A total of 487,570 particles were chemically analyzed with positive and negative ion mass spectra and a large set of single particle mass spectra was collected and analyzed in order to identify the speciation. According to the typical tracer ions from different source types and classification by the ART-2a algorithm which uses source fingerprints for apportioning ambient particles, the major sources of single particles were simulated. Coal combustion, vehicle exhaust, and secondary ion were the most abundant particle sources, contributing 28.5%, 17.8%, and 18.2%, respectively. The fraction with vehicle exhaust species particles decreased slightly with particle size in the condensation mode particles.

  3. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  5. A dual-wavelength single particle aerosol fluorescence monitor

    NASA Astrophysics Data System (ADS)

    Kaye, Paul H.; Stanley, Warren R.; Foot, Virginia; Baxter, Karen; Barrington, Stephen J.

    2005-10-01

    Laser diodes and light-emitting diodes capable of continuous sub-300 nm radiation emission will ultimately represent optimal excitation sources for compact and fieldable bio-aerosol monitors. However, until such devices are routinely available and whilst solid-state UV lasers remain relatively expensive, other low-cost sources of UV can offer advantages. This paper describes one such prototype that employs compact xenon discharge UV sources to excite intrinsic fluorescence from individual particles within an ambient aerosol sample. The prototype monitor samples ambient air via a laminar sheathed-flow arrangement such that particles within the sample flow column are rendered in single file as they intersect the beam from a continuous-wave 660nm diode laser. Each individual particle produces a scattered light signal from which an estimate of particle size (down to ~1 um) may be derived. This same signal also initiates the sequential firing (~10 us apart) of two xenon sources which irradiate the particle with UV pulses centred upon ~280 nm and ~370 nm wavelength, optimal for excitation of bio-fluorophores tryptophan and NADH respectively. For each excitation wavelength, fluorescence is detected across two bands embracing the peak emissions of the same bio-fluorophores. Thus, for each particle, a 2-dimensional fluorescence excitation-emission matrix is recorded together with an estimate of particle size. Current measurement rates are up to ~125 particles/s (limited by the xenon recharge time), corresponding to all particles for concentrations up to ~2 x 104 particles/l. Developments to increase this to ~500 particles/s are in hand. Analysis of results from aerosols of E.coli, BG spores, and a variety of non-biological materials are given.

  6. 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.

  7. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

    DOE PAGES

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

    2017-01-27

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

  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. 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.

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

    NASA Astrophysics Data System (ADS)

    Andersson, E.; Kahnert, M.

    2015-12-01

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

  12. Ambient particle characterization by single particle aerosol mass spectrometry in an urban area of Beijing

    NASA Astrophysics Data System (ADS)

    Li, Lei; Li, Mei; Huang, Zhengxu; Gao, Wei; Nian, Huiqing; Fu, Zhong; Gao, Jian; Chai, Fahe; Zhou, Zhen

    2014-09-01

    To investigate the composition and possible sources of aerosol particles in Beijing urban area, a single particle aerosol mass spectrometer (SPAMS) was deployed from April 22 to May 4, 2011. 510,341 particles out of 2,953,200 sized particles were characterized by SPAMS in combination with the ART-2a neural network algorithm. The particles were classified as rich-K (39.79%), carbonaceous species (32.7%), industry metal (19.2%), dust (5.7%), and rich-Na (1.76%). Industrial emissions related particles, rich-Fe, rich-Pb, and K-nitrate, were the major components of aerosol particles during haze periods, which were mainly from the steel plants and metal smelting processes around Beijing. Under stagnant meterological conditions, these regional emissions have a vital effect on haze formation. Organic carbon (OC) particles were attributed to biomass burning. NaK-EC was likely to come from local traffic emissions. Internally mixed organic and elemental carbon (OCEC) was found to be from possible sources of local traffic emission and biomass burning. It was found that coarse dust particles were mainly composed of four different types of dust particles, dust-Si, dust-Ca, dust-Al, and dust-Ti. It is the first time that SPAMS was used to study a dust storm in Beijing. Our results showed that SPAMS could be a powerful tool in the identification and apportionment of aerosol sources in Beijing, providing useful reference information for environmental control and management.

  13. Aerosol growth in Titan's ionosphere through particle charging

    NASA Astrophysics Data System (ADS)

    Lavvas, P.; Yelle, R. V.; Koskinen, T.; Bazin, A.; Vuitton, V.; Vigren, E.; Galand, M. F.; Wellbrock, A.; Coates, A. J.; Wahlund, J.; Crary, F.; Snowden, D. S.

    2012-12-01

    Observations of Titan's lower thermosphere and ionosphere by Cassini instruments demonstrate the presence of large mass negative ions of a few thousand amu, and the presence of positive ions up to a few hundred amu [1,2]. The mechanisms though responsible for the production of these large ions have so far remained elusive. A recent Titan flyby that probed deeper layers of Titan's thermosphere than usual, revealed a discrepancy in the observed positive ion and electron density, with the electron density lower than the abundance required to satisfy charge balance [3]. The remaining electron density was found in the form of the large mass negative ions. Aerosols can be charged on interaction with electrons and ions, while this charge can affect the particle coagulation, thus, their subsequent growth. Given the above observations we investigate here the potential role of aerosols in Titan's ionosphere and how this interaction affects the aerosol evolution. This investigation is performed with the use of a model that couples between the ionospheric photochemical evolution and the microphysical growth of aerosols in a self-consistent approach. Our results show that particle charging has an important role in the ionosphere. Most of the produced particles in the ionosphere attain a negative charge. Thus, they act as a sink for the free electrons with the remaining free electron densities consistent with the recent Cassini observations. Being negatively charged, the particles repel each other reducing in this way the coagulation rates and the growth of the aerosols. On the other hand, the negatively charged particles attract the abundant positive ions, which results to enhanced collisions between them. The mass added to the particles by the ions leads to an increase in their size and an increase in the resulting mass flux of the aerosols. Our simulated mass per charge spectra provide excellent fits to the observed positive and negative ion spectra from the Cassini Plasma

  14. Collection efficiency of α-pinene secondary organic aerosol particles explored via light-scattering single-particle aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Shipley Robinson, Ellis; Onasch, Timothy B.; Worsnop, Douglas; Donahue, Neil M.

    2017-03-01

    We investigated the collection efficiency and effective ionization efficiency for secondary organic aerosol (SOA) particles made from α-pinene + O3 using the single-particle capabilities of the aerosol mass spectrometer (AMS). The mean count-based collection efficiency (CEp) for SOA across these experiments is 0.30 (±0.04 SD), ranging from 0.25 to 0.40. The mean mass-based collection efficiency (CEm) is 0.49 (±0.07 SD). This sub-unit collection efficiency and delayed vaporization is attributable to particle bounce in the vaporization region. Using the coupled optical and chemical detection of the light-scattering single-particle (LSSP) module of the AMS, we provide clear evidence that delayed vaporization is somewhat of a misnomer for these particles: SOA particles measured as a part of the AMS mass distribution do not vaporize at a slow rate; rather, they flash-vaporize, albeit often not on the initial impact with the vaporizer but instead upon a subsequent impact with a hot surface in the vaporization region. We also find that the effective ionization efficiency (defined as ions per particle, IPP) decreases with delayed arrival time. CEp is not a function of particle size (for the mobility diameter range investigated, 170-460 nm), but we did see a decrease in CEp with thermodenuder temperature, implying that oxidation state and/or volatility can affect CEp for SOA. By measuring the mean ions per particle produced for monodisperse particles as a function of signal delay time, we can separately determine CEp and CEm and thus more accurately measure the relative ionization efficiency (compared to ammonium nitrate) of different particle types.

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

    NASA Astrophysics Data System (ADS)

    Andersson, Emma; Kahnert, Michael

    2016-05-01

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

  16. Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles.

    PubMed

    Lin, Peng; Aiona, Paige K; Li, Ying; Shiraiwa, Manabu; Laskin, Julia; Nizkorodov, Sergey A; Laskin, Alexander

    2016-11-01

    Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly emitted biomass burning organic aerosol (BBOA) samples collected during test burns of sawgrass, peat, ponderosa pine, and black spruce. We demonstrate that both the BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels. Common BrC chromophores in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as source-specific markers of BrC. On average, ∼50% of the light absorption in the solvent-extractable fraction of BBOA can be attributed to a limited number of strong BrC chromophores. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of ∼16 h. A "molecular corridor" analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low saturation mass concentration (<1 μg m(-3)) and will be retained in the particle phase under atmospherically relevant conditions.

  17. Semi-Continuous Measurements of Aerosol Chemical Composition During the Summer 2002 Yosemite National Park Special Study

    SciTech Connect

    Collette, J; Lee, T; Heath, J; Carrico, C; Herckes, P; Engling, G; McMeeking, G; Kreidenweis, S; Day, D; Malm, W; Cahill, T

    2003-02-16

    Semi-continuous measurements of fine particle composition were made over a period of several weeks in summer 2002 in Yosemite National Park, California. These included measurement of aerosol ionic composition (by PILS- Particle-Into-Liquid System) and aerosol carbon (by dual wavelength aethalometer and an R&P particulate carbon monitor). The data reveal that aerosol composition at the site is highly :variable in time, with a strong diurnal cycle. Interestingly, however, different diurnal cycles were sometimes observed for different chemical constituents of the particles. Organic carbon was observed to dominate fine particle mass, with some periods apparently associated with influx of smoke from wildfires in the western U.S. Measurements of fine particle carbon isotopes revealed the fraction of carbon from biogenic sources to range from approximately 73 to 95%. The ionic fraction of the aerosol was usually dominated by ammoniated sulfate. During most periods, PM{sub 2.5} nitrate was found primarily in sea salt particles from which chloride had been displaced. Strong variations in the extent of ammonia neutralization of sulfate were also observed. The ability to observe rapid changes in aerosol composition using these semi-continuous aerosol composition measurements is helpful for understanding the dynamic chemical composition of fine particles responsible for regional haze.

  18. Linking Remotely Sensed Aerosol Types to Their Chemical Composition

    NASA Technical Reports Server (NTRS)

    Dawson, Kyle William; Kacenelenbogen, Meloe S.; Johnson, Matthew S.; Burton, Sharon P.; Hostetler, Chris A.; Meskhidze, Nicholas

    2016-01-01

    Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% +/- 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into 'dark' and 'light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

  19. Surface Chemistry at Size-Selected Nano-Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Roberts, Jeffrey

    2005-03-01

    A method has been developed to conduct surface chemistry and extract surface kinetic rates from size-selected aerosol nanoparticles. The measurements encompass broad ranges of particle size, phase, and composition. Results will be presented on the uptake of water by aerosolized soot nanoparticles of radius between 10 and 40 nm. Water uptake was monitored by tandem differential mobility analysis (T-DMA), which is capable of measuring changes in particle diameter as little as 0.2 nm. Soot particles were produced in an ethene diffusion flame and extracted into an atmospheric pressure aerosol flow tube reactor. The particles were subjected to various thermal and oxidative treatments, and the effects of these treatments on the ability of soot to adsorb monolayer quantities of water was determined. The results are important because soot nucleates atmospheric cloud particles. More generally, the results represent one of the first kinetic and mechanistic studies of gas-phase nanoparticle reactivity. Co-author: Henry Ajo, University of Minnesota

  20. Liquid-liquid phase separation in aerosol particles: Imaging at the Nanometer Scale

    SciTech Connect

    O'Brien, Rachel; Wang, Bingbing; Kelly, Stephen T.; Lundt, Nils; You, Yuan; Bertram, Allan K.; Leone, Stephen R.; Laskin, Alexander; Gilles, Mary K.

    2015-04-21

    Atmospheric aerosols can undergo phase transitions including liquid-liquid phase separation (LLPS) while responding to changes in the ambient relative humidity (RH). Here, we report results of chemical imaging experiments using environmental scanning electron microscopy (ESEM) and scanning transmission x-ray microscopy (STXM) to investigate the LLPS of micron sized particles undergoing a full hydration-dehydration cycle. Internally mixed particles composed of ammonium sulfate (AS) and either: limonene secondary organic carbon (LSOC), a, 4-dihydroxy-3-methoxybenzeneaceticacid (HMMA), or polyethylene glycol (PEG-400) were studied. Events of LLPS with apparent core-shell particle morphology were observed for all samples with both techniques. Chemical imaging with STXM showed that both LSOC/AS and HMMA/AS particles were never homogeneously mixed for all measured RH’s above the deliquescence point and that the majority of the organic component was located in the shell. The shell composition was estimated as 65:35 organic: inorganic in LSOC/AS and as 50:50 organic: inorganic for HMMA/AS. PEG-400/AS particles showed fully homogeneous mixtures at high RH and phase separated below 89-92% RH with an estimated 50:50% organic to inorganic mix in the shell. These two chemical imaging techniques are well suited for in-situ analysis of the hygroscopic behavior, phase separation, and surface composition of collected ambient aerosol particles.

  1. Comparison of cloud residual and background aerosol particle composition during the hill cap cloud experiment HCCT 2010 in Central Germany

    NASA Astrophysics Data System (ADS)

    Roth, A.; Mertes, S.; van Pinxteren, D.; Klimach, T.; Herrmann, H.; Schneider, J.; Borrmann, S.

    2013-12-01

    Physical and chemical characterization of cloud residual and background aerosol particles as well as aerosol-cloud interactions were investigated during the Hill Cap Cloud Thuringia (HCCT) experiment in September and October 2010 on the mountain site Schmücke (938m a.s.l.) in Germany. Background aerosol particles were sampled by an interstitial inlet whereas cloud droplets from orographic clouds were collected by a counter flow virtual impactor (CVI). Chemical composition analysis and sizing of the particles was done by single particle mass spectrometry using the bipolar Aircraft-based Laser Ablation Aerosol Mass Spectrometer (ALABAMA, particle diameter range 150 nm - 900 nm; Brands et al., 2011) and by two Aerodyne Aerosol Mass Spectrometers (C-ToF, HR-ToF). Supplementary, the particle size distribution was measured with an optical particle counter (OPC, size range 0.25 μm - 32 μm). During the field campaign about 21000 positive and negative single particle mass spectra could be obtained from cloud residual particles and about 239000 from background aerosol particles. The data were clustered by means of the fuzzy c-means algorithm. The resulting clusters consisting of mass spectra with similar fragmentation patterns were, dependent on presence and combination of peaks, assigned to certain particle types. For both sampled particle types a large portion is internally mixed with nitrate and/or sulfate. This might be an explanation, why a comparison of the composition shows a higher fraction of soot particles and amine-containing particles among cloud residuals. Furthermore cloud residuals show a decreased fraction of particles being internally mixed only with nitrate (10%) compared to background aerosol particles (19%) of the same air masses, whereas the fraction of particles containing both nitrate and sulfate increases from 39% to 63% indicating cloud processing by uptake and oxidation of SO2 (Harris et al, 2013). Brands, M., Kamphus, M., Böttger, T., Schneider

  2. 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

  3. Thermophoretic motion of large heated aerosol spherical particles

    NASA Astrophysics Data System (ADS)

    Malai, N. V.; Limanskaya, A. V.; Shchukin, E. R.

    2016-03-01

    The stationary motion of a large spherical aerosol particle in the external field of a temperature gradient in zero gravity is theoretically described using the Stokes approximation and the assumption that the average temperature of the particle surface differs considerably from the temperature of the surrounding gaseous medium. The gas dynamics equations are solved taking into account the power-law temperature dependence of the molecular transport coefficients (viscosity, thermal conductivity) and the density of the gaseous medium. Numerical estimates show that the dependence of the thermophoretic force and velocity on the average temperature of the particle surface is nonlinear.

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

    EPA Science Inventory

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

  5. Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols

    PubMed Central

    Mills, Jessica B.; Park, Jae Hong; Peters, Thomas M.

    2016-01-01

    We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride, NaCl, and spark generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <103; Medium, 103–104; and High, >104 particles/cm3). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared to those measured with reference instruments, a scanning mobility particle sizer (SMPS) and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 21% of those measured by reference instruments for polydisperse aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +130% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm but caution should be exercised when particles larger than 300 nm are present. PMID:23473056

  6. Characterization of the Aerosol-based Synthesis of Uranium Particles as a Potential Reference Material for Micro Analytical Methods.

    PubMed

    Middendorp, Ronald; Dürr, Martin; Knott, Alexander; Pointurier, Fabien; Ferreira Sanchez, Dario; Samson, Valerie Ann; Grolimund, Daniel

    2017-03-27

    A process for production of micrometer-sized particles composed of uranium oxide using aerosol spray pyrolysis is characterized with respect to the various production parameters. The aerosol is generated using a vibrating orifice aerosol generator providing monodisperse droplets, which are oxidized in a subsequent heat treatment. The final particles are characterized with micro analytical methods to determine size, shape, internal morphology, chemical and structural properties in order to assess the suitability of the produced particles as a reference material for micro analytical methods, in particular for mass-spectrometry. It is demonstrated that physico-chemical processes during particle formation and the heat treatment to chemically transform particles into an oxide strongly influence the particle shape and the internal morphology. Synchrotron μ-X-ray based techniques combined with μ-Raman spectroscopy have been applied to demonstrate that the obtained micro particles consist of a triuranium octoxide phase. Our studies demonstrate that the process is capable of delivering spherical particles with determined uniform size and ele-mental as well as chemical composition. The particles therefore represent a suitable base material to fulfill the homogeneity and stability requirements of a reference material for micro analytical methods applied in, for example, international safeguards or nuclear forensics.

  7. Continuous measurements of aerosol particles in Arctic Russia and Finland

    NASA Astrophysics Data System (ADS)

    Asmi, Eija; Kondratyev, Vladimir; Brus, David; Lihavainen, Heikki; Laurila, Tuomas; Aurela, Mika; Hatakka, Juha; Viisanen, Yrjö; Reshetnikov, Alexander; Ivakhov, Victor; Uttal, Taneil; Makshtas, Alexander

    2013-04-01

    The Arctic and northern boreal regions of Eurasia are experiencing rapid environmental changes due to pressures by human activities. The largest anthropogenic climate forcings are due to aerosol particles and greenhouse gases (GHGs). The Arctic environment is highly sensitive to changes in aerosol concentrations or composition, largely due to the high surface reflectance for the most part of the year. Concentrations of aerosols in winter and spring Arctic are affected by 'Arctic Haze', a phenomenon suggested to arise from the transport of pollutants from lower latitudes and further strengthened by the strong stratification of the Arctic wintertime atmosphere. Sources and transport patterns of aerosols into the Arctic are, however, not fully understood. In order to monitor the changes within the Arctic region, as well as to understand the sources and feedback mechanisms, direct measurements of aerosols within the Arctic are needed. So far, direct year-round observations have been inadequate especially within the Russian side of the Arctic. This is the reason why a new climate observatory was founded in Tiksi, Russia. Tiksi meteorological observatory in northern Siberia (71o 36' N; 128o 53' E) on the shore of the Laptev Sea has been operating since 1930s. Recently, it was upgraded and joint in the network of the IASOA, in the framework of the International Polar Year Activity project. The project is run in collaboration between National Oceanic and Atmospheric Administration (NOAA) with the support of the National Science Foundation (NSF), Roshydromet (AARI and MGO units), government of the Republic of Sakha (Yakutia) and the Finnish Meteorological Institute (FMI). The research activities of FMI in Tiksi include e.g. continuous long-term measurements of aerosol physical properties, which have been successfully continued since summer 2010. These, together with the FMI measurements in Pallas station in northern Finland since 1999, provide important information on the

  8. Aerosol-halogen interaction: Change of physico-chemical properties of SOA by naturally released halogen species

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

    Reactive halogen species are released by various sources like photo-activated sea-salt aerosol or salt pans and salt lakes. These heterogeneous release mechanisms have been overlooked so far, although their potential of interaction with organic aerosols like Secondary Organic Aerosol (SOA), Biomass Burning Organic Aerosol (BBOA) or Atmospheric Humic LIke Substances (HULIS) is completely unknown. Such reactions can constitute sources of gaseous organo-halogen compounds or halogenated organic particles in the atmospheric boundary layer. To study the interaction of organic aerosols with reactive halogen species (RHS), SOA was produced from α-pinene, catechol and guaiacol using an aerosol smog-chamber. The model SOAs were characterized in detail using a variety of physico-chemical methods (Ofner et al., 2011). Those aerosols were exposed to molecular halogens in the presence of UV/VIS irradiation and to halogens, released from simulated natural halogen sources like salt pans, in order to study the complex aerosol-halogen interaction. The heterogeneous reaction of RHS with those model aerosols leads to different gaseous species like CO2, CO and small reactive/toxic molecules like phosgene (COCl2). Hydrogen containing groups on the aerosol particles are destroyed to form HCl or HBr, and a significant formation of C-Br bonds could be verified in the particle phase. Carbonyl containing functional groups of the aerosol are strongly affected by the halogenation process. While changes of functional groups and gaseous species were visible using FTIR spectroscopy, optical properties were studied using Diffuse Reflectance UV/VIS spectroscopy. Overall, the optical properties of the processed organic aerosols are significantly changed. While chlorine causes a "bleaching" of the aerosol particles, bromine shifts the maximum of UV/VIS absorption to the red end of the UV/VIS spectrum. Further physico-chemical changes were recognized according to the aerosol size-distributions or the

  9. PD-FiTE - an efficient method for calculating gas / liquid equilibria in atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Topping, D.; Lowe, D.; McFiggans, G.; Barley, M.

    2009-04-01

    Assessing the impact of atmospheric aerosol particles on the environment requires adequate representation of appropriate key processes within large scale models. In the absence of primary particulate material, interactions between the atmospheric gaseous components and particles means that the chemical nature of the particles is largely determined by the availability of condensable gaseous material, such as sulphuric and nitric acids, and by the ambient environmental conditions. Gas to particle mass transfer of semi-volatile components,driven by a difference in equilibrium and actual partial pressures above an aerosol particle, is an important factor in determining the evolving chemical composition of the particle and is necessary for predicting aerosol loading and composition. The design of an appropriate framework required for parameterizations of key variables is challenging. These thermodynamic frameworks are often numerically very complex, resulting in significant computational expense. Three dimensional chemical and aerosol transport models demand that computational expense be kept at a minimum,resulting in a trade-off between accuracy and efficiency. To calculate the equilibrium vapour pressure above a solution requires treatment of solution nonideality. This is manifest through activity coefficients of components pertinent to each condensing specie. However, activity coefficients are complex functions of the solution composition. Parameterisation of activity coefficients provides the main focus of this work largely because reducing the numerical complexity whilst retaining a good level of accuracy is very challenging. The approach presented here, the hybrid Partial Derivative Fitted Taylor Expansion (PDFiTE) (Topping et al 2008), builds on previously reported work, with an aim to derive parameters for an accurate and computationally efficient framework through coupling with a complex thermodynamic model. Such a reduction in complexity is important as it is

  10. Mass absorption indices of various types of natural aerosol particles in the infrared.

    PubMed

    Fischer, K

    1975-12-01

    The mass absorption index of aerosol particles has been measured in the 2-17-microm wavelength region. The measurements were performed on films of aerosol particles that were collected by an automatic jet impactor at polluted and various uncontaminated remote sites. All but marine aerosols possess strong absorption bands in the transparent part of the atmospheric long-wave spectrum, indicating marked influence of aerosol particles on the radiation budget of the atmosphere.

  11. Reconciling satellite aerosol optical thickness and surface fine particle mass through aerosol liquid water

    NASA Astrophysics Data System (ADS)

    Nguyen, Thien Khoi V.; Ghate, Virendra P.; Carlton, Annmarie G.

    2016-11-01

    Summertime aerosol optical thickness (AOT) over the southeast U.S. is sharply enhanced over wintertime values. This seasonal pattern is unique and of particular interest because temperatures there have not warmed over the past 100 years. Patterns in surface fine particle mass are inconsistent with satellite reported AOT. In this work, we attempt to reconcile the spatial and temporal distribution of AOT over the U.S. with particle mass measurements at the surface by examining trends in aerosol liquid water (ALW), a particle constituent that scatters radiation and affects satellite AOT but is removed in mass measurements at routine surface monitoring sites. We employ the thermodynamic model ISORROPIAv2.1 to estimate ALW mass concentrations at Interagency Monitoring of PROtected Visual Environments sites using measured ion mass concentrations and North American Regional Reanalysis meteorological data. Excellent agreement between Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations AOT and estimated ALW provides a plausible explanation for the discrepancies in the geographical patterns of AOT and aerosol mass measurements.

  12. 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...

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

    NASA Astrophysics Data System (ADS)

    Golobokova, Liudmila; Polkin, Victor

    2014-05-01

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

  14. Physical and Chemical Characterization of Carbonaceous Aerosols in Korea

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  15. Impacts of oxidation aging on secondary organic aerosol formation, particle growth rate, cloud condensation nuclei abundance, and aerosol climate forcing

    NASA Astrophysics Data System (ADS)

    Yu, F.; Luo, G.

    2014-12-01

    Particle composition measurements indicate that organic aerosol (OA) makes up ~20-90% of submicron particulate mass and secondary OA (SOA) accounts for a large fraction (~ 72 ±21%) of these OA masses at many locations around the globe. The volatility changes of secondary organic gases (SOG) associated with oxidation aging as well as the contribution of highly oxidized low volatile SOG (LV-SOG) to the condensational growth of secondary particles have been found to be important in laboratory and field measurements but are poorly represented in global models. A novel scheme to extend the widely used two-product SOA formation model, by adding a third product arising from the oxidation aging (i.e., LV-SOG) and considering the dynamic transfer of mass from higher to lower volatile products, has been developed and implemented into a global chemical transport model (GEOS-Chem) and a community atmosphere model (CESM-CAM5). The scheme requires only minor changes to the existing two-product SOA formation model and is computationally efficient. With the oxidation rate constrained by laboratory measurements, we show that the new scheme predicts a much higher SOA mass concentrations, improving the agreement with aerosol mass spectrometer SOA measurements. The kinetic condensation of LV-SOG on ultrafine particles, simulated by a size-resolved (sectional) advanced particle microphysics (APM) model incorporated into in GEOS-Chem and CAM5, increases the particle growth rate substantially and improves the agreement of simulated cloud condensation nuclei (CCN) concentrations with observations. Based on GEOS-Chem-APM simulations, the new SOA formation scheme increases global mean low troposphere SOA mass concentration by ~130% and CCN abundance by ~ 15%, and optical depth of secondary particles and coated black carbon and primary organic carbon particles by ~10%. As a result, aerosol radiative cooling effect (direct + first indirect) is enhanced by -0.9 W/m2, with large spatial

  16. Understanding hygroscopic growth and phase transformation of aerosols using single particle Raman spectroscopy in an electrodynamic balance.

    PubMed

    Lee, Alex K Y; Ling, T Y; Chan, Chak K

    2008-01-01

    Hygroscopic growth is one of the most fundamental properties of atmospheric aerosols. By absorbing or evaporating water, an aerosol particle changes its size, morphology, phase, chemical composition and reactivity and other parameters such as its refractive index. These changes affect the fate and the environmental impacts of atmospheric aerosols, including global climate change. The ElectroDynamic Balance (EDB) has been widely accepted as a unique tool for measuring hygroscopic properties and for investigating phase transformation of aerosols via single particle levitation. Coupled with Raman spectroscopy, an EDB/Raman system is a powerful tool that can be used to investigate both physical and chemical changes associated with the hygroscopic properties of individually levitated particles under controlled environments. In this paper, we report the use of an EDB/Raman system to investigate (1) contact ion pairs formation in supersaturated magnesium sulfate solutions; (2) phase transformation in ammonium nitrate/ammonium sulfate mixed particles; (3) hygroscopicity of organically coated inorganic aerosols; and (4) heterogeneous reactions altering the hygroscopicity of organic aerosols.

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

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

  18. 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.

  19. Aerosol Sampling System for Collection of Capstone Depleted Uranium Particles in a High-Energy Environment

    SciTech Connect

    Holmes, Thomas D.; Guilmette, Raymond A.; Cheng, Yung-Sung; Parkhurst, MaryAnn; Hoover, Mark D.

    2009-03-01

    The Capstone Depleted Uranium Aerosol Study was undertaken to obtain aerosol samples resulting from a kinetic-energy cartridge with a large-caliber depleted uranium (DU) penetrator striking an Abrams or Bradley test vehicle. The sampling strategy was designed to (1) optimize the performance of the samplers and maintain their integrity in the extreme environment created during perforation of an armored vehicle by a DU penetrator, (2) collect aerosols as a function of time post-impact, and (3) obtain size-classified samples for analysis of chemical composition, particle morphology, and solubility in lung fluid. This paper describes the experimental setup and sampling methodologies used to achieve these objectives. Custom-designed arrays of sampling heads were secured to the inside of the target in locations approximating the breathing zones of the vehicle commander, loader, gunner, and driver. Each array was designed to support nine filter cassettes and nine cascade impactors mounted with quick-disconnect fittings. Shielding and sampler placement strategies were used to minimize sampler loss caused by the penetrator impact and the resulting fragments of eroded penetrator and perforated armor. A cyclone train was used to collect larger quantities of DU aerosol for chemical composition and solubility. A moving filter sample was used to obtain semicontinuous samples for depleted uranium concentration determination. Control for the air samplers was provided by five remotely located valve control and pressure monitoring units located inside and around the test vehicle. These units were connected to a computer interface chassis and controlled using a customized LabVIEW engineering computer control program. The aerosol sampling arrays and control systems for the Capstone study provided the needed aerosol samples for physicochemical analysis, and the resultant data were used for risk assessment of exposure to DU aerosol.

  20. Aerosol sampling system for collection of Capstone depleted uranium particles in a high-energy environment.

    PubMed

    Holmes, Thomas D; Guilmette, Raymond A; Cheng, Yung Sung; Parkhurst, Mary Ann; Hoover, Mark D

    2009-03-01

    The Capstone Depleted Uranium (DU) Aerosol Study was undertaken to obtain aerosol samples resulting from a large-caliber DU penetrator striking an Abrams or Bradley test vehicle. The sampling strategy was designed to (1) optimize the performance of the samplers and maintain their integrity in the extreme environment created during perforation of an armored vehicle by a DU penetrator, (2) collect aerosols as a function of time post perforation, and (3) obtain size-classified samples for analysis of chemical composition, particle morphology, and solubility in lung fluid. This paper describes the experimental setup and sampling methodologies used to achieve these objectives. Custom-designed arrays of sampling heads were secured to the inside of the target in locations approximating the breathing zones of the crew locations in the test vehicles. Each array was designed to support nine filter cassettes and nine cascade impactors mounted with quick-disconnect fittings. Shielding and sampler placement strategies were used to minimize sampler loss caused by the penetrator impact and the resulting fragments of eroded penetrator and perforated armor. A cyclone train was used to collect larger quantities of DU aerosol for measurement of chemical composition and solubility. A moving filter sample was used to obtain semicontinuous samples for DU concentration determination. Control for the air samplers was provided by five remotely located valve control and pressure monitoring units located inside and around the test vehicle. These units were connected to a computer interface chassis and controlled using a customized LabVIEW engineering computer control program. The aerosol sampling arrays and control systems for the Capstone study provided the needed aerosol samples for physicochemical analysis, and the resultant data were used for risk assessment of exposure to DU aerosol.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  3. Accommodation coefficient of HOBr on deliquescent sodium bromide aerosol particles

    NASA Astrophysics Data System (ADS)

    Wachsmuth, M.; Gäggeler, H. W.; von Glasow, R.; Ammann, M.

    2002-06-01

    Uptake of HOBr on sea salt aerosol, sea salt brine or ice is believed to be a key process providing a source of photolabile bromine (Br2) and sustaining ozone depletion cycles in the Arctic troposphere. In the present study, uptake of HOBr on sodium bromide (NaBr) aerosol particles was investigated at an extremely low HOBr concentration of 300 cm-3 using the short-lived radioactive isotopes 83-86Br. Under these conditions, at maximum one HOBr molecule was taken up per particle. The rate of uptake was clearly limited by the mass accommodation coefficient, which was calculated to be 0.6 ± 0.2. This value is a factor of 10 larger than estimates used in earlier models. The atmospheric implications are discussed using the box model "MOCCA'', showing that the increase of the accommodation coefficient of HOBr by a factor of 10 only slightly affects net ozone loss, but significantly increases chlorine release.

  4. Detection of Free Tropospheric Air Masses With High So2 and Aerosol Concentrations: Evidence For New Aerosol Particle Formation By H2so4/h2o Nucleation

    NASA Astrophysics Data System (ADS)

    Katragkou, E.; Wilhelm, S.; Kiendler, A.; Arnold, F.; Minikin, A.; Schlager, H.; van Velthoven, P.

    Sulfur dioxide and aerosol measurements were performed in the free troposphere (FT) and the Planetary Boundary Layer (PBL) above continental Europe. The measure- ments took place on board of the German research aircraft "Falcon" in 18 April 2001 as a part of the SCAVEX campaign. A novel aircraft based CIMS (Chemical Ion- ization Mass Spectrometry) instrument equipped with an ion trap mass spectrometer (ITMS) with a low detection limit (50pptv) and a high time resolution (1.3s) operated by MPI-K was used to perform the SO2 measurements. For the aerosol measurements DLR-IPA operated a Condensation Particle Size Analyzer, detecting particles with diameters d > 4, 7, 9 and 20nm and a PCASP-100X aerosol spectrometer probe (d > 100nm). In the measurements made mostly around 5000m altitude SO2 rich air masses were occasionally observed with SO2 VMR of up to 2900pptv. The strong SO2 pollu- tion was due to fast vertical transport of polluted continental PBL air and small-scale deep convection, as indicated by the 5-day backward 3D trajectories. These observa- tions of strong SO2 pollution have interesting implications for aerosol processes, in- cluding efficient formation of gaseous sulfuric acid (GSA) and new aerosol particles. They also imply fast growth of freshly nucleated aerosol particles, which increases the chance for new particles to grow to the size of a CCN. Our analysis indicates the occurrence of new particle formation by H2SO4/H2O nucleation and fast new particle growth by H2SO4/H2O condensation and self-coagulation in the different air masses encountered during the flight.

  5. 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.

  6. 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

  7. Aerosol mass spectrometry: particle-vaporizer interactions and their consequences for the measurements

    NASA Astrophysics Data System (ADS)

    Drewnick, F.; Diesch, J.-M.; Faber, P.; Borrmann, S.

    2015-09-01

    The Aerodyne aerosol mass spectrometer (AMS) is a frequently used instrument for on-line measurement of the ambient sub-micron aerosol composition. With the help of calibrations and a number of assumptions on the flash vaporization and electron impact ionization processes, this instrument provides robust quantitative information on various non-refractory ambient aerosol components. However, when measuring close to certain anthropogenic or marine sources of semi-refractory aerosols, several of these assumptions may not be met and measurement results might easily be incorrectly interpreted if not carefully analyzed for unique ions, isotope patterns, and potential slow vaporization associated with semi-refractory species. Here we discuss various aspects of the interaction of aerosol particles with the AMS tungsten vaporizer and the consequences for the measurement results: semi-refractory components - i.e., components that vaporize but do not flash-vaporize at the vaporizer and ionizer temperatures, like metal halides (e.g., chlorides, bromides or iodides of Al, Ba, Cd, Cu, Fe, Hg, K, Na, Pb, Sr, Zn) - can be measured semi-quantitatively despite their relatively slow vaporization from the vaporizer. Even though non-refractory components (e.g., NH4NO3 or (NH4)2SO4) vaporize quickly, under certain conditions their differences in vaporization kinetics can result in undesired biases in ion collection efficiency in thresholded measurements. Chemical reactions with oxygen from the aerosol flow can have an influence on the mass spectra for certain components (e.g., organic species). Finally, chemical reactions of the aerosol with the vaporizer surface can result in additional signals in the mass spectra (e.g., WO2Cl2-related signals from particulate Cl) and in conditioning or contamination of the vaporizer, with potential memory effects influencing the mass spectra of subsequent measurements. Laboratory experiments that investigate these particle-vaporizer interactions are

  8. Airborne studies of aerosol emissions from savanna fires in southern Africa: 2. Aerosol chemical composition

    NASA Astrophysics Data System (ADS)

    Andreae, M. O.; Andreae, T. W.; Annegarn, H.; Beer, J.; Cachier, H.; Le Canut, P.; Elbert, W.; Maenhaut, W.; Salma, I.; Wienhold, F. G.; Zenker, T.

    1998-12-01

    We investigated smoke emissions from fires in savanna, forest, and agricultural ecosystems by airborne sampling of plumes close to prescribed burns and incidental fires in southern Africa. Aerosol samples were collected on glass fiber filters and on stacked filter units, consisting of a Nuclepore prefilter for particles larger than ˜1-2 μm and a Teflon second filter stage for the submicron fraction. The samples were analyzed for soluble ionic components, organic carbon, and black carbon. Onboard the research aircraft, particle number and volume distributions as a function of size were determined with a laser-optical particle counter and the black carbon content of the aerosol with an aethalometer. We determined the emission ratios (relative to CO2 and CO) and emission factors (relative to the amount of biomass burnt) for the various aerosol constituents. The smoke aerosols were rich in organic and black carbon, the latter representing 10-30% of the aerosol mass. K+ and NH4+ were the dominant cationic species in the smoke of most fires, while Cl- and SO42- were the most important anions. The aerosols were unusually rich in Cl-, probably due to the high Cl content of the semiarid vegetation. Comparison of the element budget of the fuel before and after the fires shows that the fraction of the elements released during combustion is highly variable between elements. In the case of the halogen elements, almost the entire amount released during the fire is present in the aerosol phase, while in the case of C, N, and S, only a small proportion ends up as particulate matter. This suggests that the latter elements are present predominantly as gaseous species in the fresh fire plumes studied here.

  9. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2013-03-01

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

  11. Aerosol particles from tropical convective systems: 2. Cloud bases

    NASA Astrophysics Data System (ADS)

    Kojima, Tomoko; Buseck, Peter R.; Reeves, J. Michael

    2005-05-01

    Aerosol particles were collected at the altitudes of cloud bases during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) and analyzed using transmission electron microscopy. The particles consist of ammonium sulfate (45-90% by number), sea salt (5-45%), mineral dust (1-20%), and anthropogenic materials such as soot and fly ash (<3%). Ammonium sulfate particles have rather uniform, submicron sizes (mostly 0.5 μm across). Sea-salt particles are larger, apparently having been deliquesced. However, submicron particles are also common. Many contain Na and mixed cation sulfates in addition to NaCl. Mineral dust consists largely of tabular clay particles. Samples from the 28 July flight contain much mineral dust, probably because of transport from the Saharan Desert. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are common. Such mixed aggregates are especially abundant in in-cloud samples. Cirrus samples from CRYSTAL-FACE contain many H2SO4 droplets (Kojima et al., 2004), but acidic sulfate particles are rare at the altitudes of cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. Sea salt and mineral dust have been reported to be abundant in cloud particles collected using a counterflow virtual impactor (Cziczo et al., 2004), suggesting that these particles were incorporated into the convective systems from the cloud bases and akted as ice nuclei while being vertically transported.

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

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

  13. Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

    NASA Astrophysics Data System (ADS)

    Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

    2007-12-01

    Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

  14. Aerosol Mass Spectrometry via Laser-Induced Incandescence Particle Vaporization Final Report

    SciTech Connect

    Timothy B. Onasch

    2011-10-20

    We have successfully developed and commercialized a soot particle aerosol mass spectrometer (SP-AMS) instrument to measure mass, size, and chemical information of soot particles in ambient environments. The SP-AMS instrument has been calibrated and extensively tested in the laboratory and during initial field studies. The first instrument paper describing the SP-AMS has been submitted for publication in a peer reviewed journal and there are several related papers covering initial field studies and laboratory studies that are in preparation. We have currently sold 5 SP-AMS instruments (either as complete systems or as SP modules to existing AMS instrument operators).

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

    NASA Astrophysics Data System (ADS)

    Adams, P. J.; Marks, M.

    2015-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2003-07-01

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

  17. 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.

  18. Simultaneous ion luminescence imaging and spectroscopy of individual aerosol particles with external proton or helium microbeams

    NASA Astrophysics Data System (ADS)

    Kada, Wataru; Satoh, Takahiro; Yokoyama, Akihito; Koka, Masashi; Kamiya, Tomihiro

    2014-08-01

    Simultaneous microscopic imaging and spectroscopy of individual aerosol particles were performed with an external microbeam. Visible luminescence induced by the external microbeam was successfully used as a probe to detect organic contaminants in the targets. Combined ion luminescence (IL)/particle-induced X-ray emission (PIXE) analysis of the aerosol targets revealed microscopic chemical and elemental composition distributions under ambient atmospheric conditions. The simple confocal micro-optics for the IL spectroscopy and microscopic imaging were sufficiently sensitive for detecting these molecules at sub-parts per million concentrations and at a wavelength resolution of less than 5 nm. The IL spectra were monitored to prevent severe damage to the samples. Furthermore, our IL system has the advantage that it is simple to add to a conventional micro-PIXE system.

  19. 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.

  20. Aerosol Particle Property Comparisons Between MISR and AERONET Retrieved Values

    NASA Astrophysics Data System (ADS)

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

    2005-12-01

    Aerosol optical depth (AOT) data from the Multi-angle ImagingSpectroRadiometer (MISR) instrument aboard the NASA Earth Observing System's Terra satellite have already been systematically compared with ground-based data from the AERONET network. As a result of that study, MISR data are now being reprocessed with improved aerosol algorithms and aerosol models. The follow-on study reported here systematically compares MISR and AERONET particle micro-physical properties. This project is currently underway. Our goal is to use the statistical power of numerous AERONET measurements to map the behavior of the MISR property retrievals, identify strength and surprises in the MISR data, and use this information both to refine further the MISR retrieval algorithms and to assess the likely error envelopes in the MISR products. Multi-year data from 36 carefully chosen sites having good long-term measurement records are stratified by broad classes of aerosol air mass types: maritime, biomass burning, desert dust, pollution, and continental aerosols. Available AERONET spectral AOT measurements for two-hour windows around MISR overpass times are interpolated to MISR wavelengths and averaged, and AOT variability over the two-hour window is noted. Sky-scan AERONET data, taken only once an hour, are also were interpolated to MISR wavelengths, and are averaged over a four-hour window provided the variability is smaller than MISR sensitivity to particle properties based on previous work. MISR retrievals over the 17.6 km standard retrieval regions that include the AERONET sites are preferentially used for the comparison. The MISR measurements are averages of over all "successful" aerosol type models in the MISR algorithm climatology, where success is measured by the degree to which multi-angle, multi-spectral top-of-atmosphere radiances match modeled radiances, using several chi-squared tests. Angstrom exponent, single scattering albedo, and size distribution mean values and variance

  1. Variations of the aerosol concentration and chemical composition over the arid steppe zone of Southern Russia in summer

    NASA Astrophysics Data System (ADS)

    Artamonova, M. S.; Gubanova, D. P.; Iordanskii, M. A.; Lebedev, V. A.; Maksimenkov, L. O.; Minashkin, V. M.; Obvintsev, Y. I.; Chketiani, O. G.

    2016-12-01

    Variations in the surface aerosol over the arid steppe zone of Southern Russia have been measured. The parameters of atmospheric aerosol (mass concentration, both dispersed and elemental compositions) and meteorological parameters were measured in Tsimlaynsk raion (Rostov oblast). The chemical composition of aerosol particles in the atmospheric surface layer has been determined, and the coefficients of enrichment of elements with respect to clarkes in the Earth's crust have been calculated. It is shown that, in summer, arid aerosols are transported from both alkaline and sandy soils of Kalmykia to the air basin over the observation zone. Aerosol particles in the surface air layer over this region have been found to contain the products of combustion of oil, coal, and ethylized fuel. These combustion products make a small contribution to the total mass concentration of atmospheric aerosol; however, they are most hazardous to the health of people because of their sizes and heavy-metal contents. A high concentration of submicron sulfur-containing aerosol particles of chemocondensation nature has been recorded. Sources of aerosol of both natural and anthropogenic origins in southern Russia are discussed.

  2. The relation between aerosol particles and lightning in Mexico

    NASA Astrophysics Data System (ADS)

    Kucienska, B.; Cervantes Villa, J. S.; Raga, G. B.

    2013-05-01

    The analysis of lightning activity registered by the World Wide Lightning Location Network and aerosol optical depth (AOD) derived from the Moderate Resolution Imaging Spectroradiometer indicate that spatial and temporal variations in cloud-to-ground lightning density over Mexico are linked to variations in aerosol amounts. Average lightning activity registered on days with moderate AOD is higher than that registered on days with low AOD for most of the continental areas and coastal maritime regions. This finding could be explained either by the aerosol effect on thunderstorms electrical activity or by a similar influence of meteorological conditions on both lightning and AOD. Analysis of temporal variations of electrical activity show that over large continental areas a significant lightning density is observed during spring, at the very beginning of rainy seasons. In May, when rainfall is relatively low, an exceptionally high lightning activity is also registered over the Pacific, in the region located south to Isthmus of Tehuantepec. This signal of high lightning density propagates hundreds of kilometers away from the coast. We hypothesize that high lightning activity during spring observed over both continental and oceanic regions is linked to the presence of aerosol particle generated by biomass burning which peaks in April and May.

  3. Chemical composition, main sources and temporal variability of PM1 aerosols in southern African grassland

    NASA Astrophysics Data System (ADS)

    Tiitta, P.; Vakkari, V.; Josipovic, M.; Croteau, P.; Beukes, J. P.; van Zyl, P. G.; Venter, A. D.; Jaars, K.; Pienaar, J. J.; Ng, N. L.; Canagaratna, M. R.; Jayne, J. T.; Kerminen, V.-M.; Kulmala, M.; Laaksonen, A.; Worsnop, D. R.; Laakso, L.

    2013-06-01

    Southern Africa is a significant source region of atmospheric pollution, yet long-term data on pollutant concentrations and properties from this region are rather limited. A recently established atmospheric measurement station in South Africa, Welgegund, is strategically situated to capture regional background emissions, as well as emissions from the major source regions in the interior of South Africa. We measured non-refractive submicron aerosols (NR-PM1) and black carbon over a one year period in Welgegund, and investigated the seasonal and diurnal patterns of aerosol concentration levels, chemical composition, acidity and oxidation level. Based on air mass back trajectories, four distinct source regions were determined for NR-PM1. Supporting data utilized in our analysis included particle number size distributions, aerosol absorption, trace gas concentrations, meteorological variables and the flux of carbon dioxide. The dominant submicron aerosol constituent during the dry season was organic aerosol, reflecting high contribution from savannah fires and other combustion sources. Organic aerosol concentrations were lower during the wet season, presumably due to wet deposition as well as reduced emissions from combustion sources. Sulfate concentrations were usually high and exceeded organic aerosol concentrations when air-masses were transported over regions containing major point sources. Sulfate and nitrate concentrations peaked when air masses passed over the industrial Highveld (iHV) area. In contrast, concentrations were much lower when air masses passed over the cleaner background (BG) areas. Air masses associated with the anti-cyclonic recirculation (ACBIC) source region contained largely aged OA. Positive Matrix Factorization (PMF) analysis of aerosol mass spectra was used to characterize the organic aerosol (OA) properties. The factors identified were oxidized organic aerosols (OOA) and biomass burning organic aerosols (BBOA) in the dry season and low

  4. Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the southeast Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Twohy, C. H.; Anderson, J. R.; Toohey, D. W.; Andrejczuk, M.; Adams, A.; Lytle, M.; George, R. C.; Wood, R.; Saide, P.; Spak, S.; Zuidema, P.; Leon, D.

    2013-03-01

    The southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics, including their significance, from eight flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number that influence droplet concentration. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were smaller in regions of enhanced particles near shore. However, physically thinner clouds, and not just higher droplet number concentrations from pollution, both contributed to the smaller droplets. Satellite measurements were used to show that cloud albedo was highest 500-1000 km offshore, and actually slightly lower closer to shore due to the generally thinner clouds and lower liquid water paths

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

    NASA Astrophysics Data System (ADS)

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

    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

  6. 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

  7. 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

  8. Chemical, Physical and Optical Properties of Saharan Dust Aerosols at a Marine Site in Puerto Rico

    NASA Astrophysics Data System (ADS)

    Ortiz Montalvo, D. L.; Mayol Bracero, O. L.; Morales, F.; Sheridan, P.; Ogren, J. A.

    2005-12-01

    Atmospheric dust particles blown from the Sahara across the Atlantic into the Caribbean have an impact on its climate and public health. These particles may play a significant role in radiative forcing, affecting the extinction of solar radiation and thus having an influence on climate. About half of the dust that travels from Africa contains particles that are small enough to inhale. Human breathe them into the respiratory system and they settle in the lungs causing respiratory problems. To have a better understanding of these effects, information is needed on the properties of these aerosols. As part of this study, chemical, physical and optical characterization is being performed on aerosol samples collected at a marine site on the northeastern tip of Puerto Rico (Cabezas de San Juan, Fajardo), during periods with and without Saharan incursions. Stacked-filter units (SFU) are used to collect particles with diameters smaller than 1.7 μm, using Nuclepore, quartz and Teflon filters. These filter samples are analyzed to obtain the chemical composition of the particles. Initially we are focusing on the carbonaceous fraction (elemental and organic carbon, EC, and OC) of the aerosol using thermal/optical analysis. Online measurements of total particle number concentrations and aerosol light scattering coefficients are performed using a condensation particle counter and an integrating nephelometer, respectively. In addition, a sunphotometer, part of AERONET (http://aeronet.gsfc.nasa.gov/), is used to obtain the aerosol optical thickness (AOT). Preliminary results include only samples collected from air masses under the influence of Saharan dust, as signified by AOT satellite images from MODIS and the results from the air masses backward trajectories calculated with the NOAA HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) model. In terms of the chemical composition, EC concentrations were at low-to-undetectable levels, indicating that OC concentrations

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

    NASA Astrophysics Data System (ADS)

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

    2002-05-01

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

  10. Three Compact, Robust Chemical Characterization Systems Suited To Sensitive, High Time Resolution Measurements Of Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Barrie, L. A.; Cowin, J. P.; Worsnop, D. R.

    2001-12-01

    In the past decade, the advancement of compact, robust and sensitive instrumentation to measure the chemical characteristics of atmospheric aerosols has lagged behind their physical characterization. There is a need for chemical instrumentation with these three qualities for use on airborne platforms and at infrequently attended ground level surveillance sites. Now chemical techniques are appearing that promise to fill this need. We discuss three chemical characterization systems that are emerging in atmospheric chemistry and climate research applications. These are: (i) the Aerodyne mass spectrometer for real time measurement of particle composition and two post-collection analysis techniques (ii) non-destructive, multi-elemental chemical analysis of size-resolved samples by high spatial resolution synchrotron x-ray and proton beams (S-XRF/PIXE/PESA/STIM) (iii) single particle characterization by automated scanning electron microscopy with energy-dispersed detection of X-rays (SEM/EDX). The key to post-collection analysis is automated aerosol sizing and collection systems and automated chemical analysis systems. Together these techniques provide unique, comprehensive information on the organic and inorganic composition and morphology of particles and yet are easy to deploy in the field. The sensitivity of each technique is high enough to permit the rapid sampling needed to resolve spatial gradients in composition from a moving platform like the Battelle Gulfstream-159 aircraft, traveling at 100m/s.

  11. Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

    PubMed

    Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

    2009-03-01

    During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

  12. ¹¹¹Indium-labeled ultrafine carbon particles; a novel aerosol for pulmonary deposition and retention studies.

    PubMed

    Sanchez-Crespo, Alejandro; Klepczynska-Nyström, Anna; Lundin, Anders; Larsson, Britt Marie; Svartengren, Magnus

    2011-02-01

    Continuous environmental or occupational exposure to airborne particulate pollution is believed to be a major hazard for human health. A technique to characterize their deposition and clearance from the lungs is fundamental to understand the underlying mechanisms behind their negative health effects. In this work, we describe a method for production and follow up of ultrafine carbon particles labeled with radioactive ¹¹¹Indium (¹¹¹In). The physicochemical and biological properties of the aerosol are described in terms of particle size and concentration, agglomeration rate, chemical bonding stability, and human lung deposition and retention. Preliminary in vivo data from a healthy human pilot exposure and 1-week follow up of the aerosol is presented. More than 98% of the generated aerosol was labeled with Indium and with particle sizes log normally distributed around 79  nm count median diameter. The aerosol showed good generation reproducibility and chemical stability, about 5% leaching 7 days after generation. During human inhalation, the particles were deposited in the alveolar space, with no central airways involvement. Seven days after exposure, the cumulative activity retention was 95.3%. Activity leaching tests from blood and urine samples confirmed that the observed clearance was explained by unbound activity, suggesting that there was no significant elimination of ultrafine particles. Compared to previously presented methods based on Technegas, ¹¹¹In-labelled ultrafine carbon particles allow for extended follow-up assessments of particulate pollution retention in healthy and diseased lungs.

  13. Chemical Composition of Atmospheric Aerosols Above a Pristine South East Asian Rainforest

    NASA Astrophysics Data System (ADS)

    Robinson, N. H.; Allan, J. D.; Williams, P. I.; Coe, H.; Hamilton, J.; Chen, Q.; Martin, S.; Trembath, J.

    2009-04-01

    conjunction with a constant pressure inlet. The aerosols' chemical origins have been further investigated by comparing these spectra to chamber experiments, mass spectral libraries and data from comparable experiments in other locations. These data are also being analysed in conjunction with offline techniques applied to samples collected using filters and a Particle-Into-Liquid Sampler (PILS). Methods used include liquid chromatography and comprehensive two-dimensional gas chromatography coupled to time of flight mass spectrometry. These techniques provide a more detailed chemical characterisation of the SOA and water soluble organic carbon, allowing direct links back to gas phase precursors. In conjunction with the field measurements, a programme of chamber experiments is being carried out at Manchester as part of the ACES project. This will generate comparable SOA under controlled conditions and subjecting them to similar analysis.

  14. Raman microscopy of size-segregated aerosol particles, collected at the Sonnblick Observatory in Austria

    NASA Astrophysics Data System (ADS)

    Ofner, Johannes; Kasper-Giebl, Anneliese; Kistler, Magdalena; Matzl, Julia; Schauer, Gerhard; Hitzenberger, Regina; Lohninger, Johann; Lendl, Bernhard

    2014-05-01

    Size classified aerosol samples were collected using low pressure impactors in July 2013 at the high alpine background site Sonnnblick. The Sonnblick Observatory is located in the Austrian Alps, at the summit of Sonnblick 3100 m asl. Sampling was performed in parallel on the platform of the Observatory and after the aerosol inlet. The inlet is constructed as a whole air inlet and is operated at an overall sampling flow of 137 lpm and heated to 30 °C. Size cuts of the eight stage low pressure impactors were from 0.1 to 12.8 µm a.d.. Alumina foils were used as sample substrates for the impactor stages. In addition to the size classified aerosol sampling overall aerosol mass (Sharp Monitor 5030, Thermo Scientific) and number concentrations (TSI, CPC 3022a; TCC-3, Klotz) were determined. A Horiba LabRam 800HR Raman microscope was used for vibrational mapping of an area of about 100 µm x 100 µm of the alumina foils at a resolution of about 0.5 µm. The Raman microscope is equipped with a laser with an excitation wavelength of 532 nm and a grating with 300 gr/mm. Both optical images and the related chemical images were combined and a chemometric investigation of the combined images was done using the software package Imagelab (Epina Software Labs). Based on the well-known environment, a basic assignment of Raman signals of single particles is possible at a sufficient certainty. Main aerosol constituents e.g. like sulfates, black carbon and mineral particles could be identified. First results of the chemical imaging of size-segregated aerosol, collected at the Sonnblick Observatory, will be discussed with respect to standardized long-term measurements at the sampling station. Further, advantages and disadvantages of chemical imaging with subsequent chemometric investigation of the single images will be discussed and compared to the established methods of aerosol analysis. The chemometric analysis of the dataset is focused on mixing and variation of single compounds at

  15. Physicochemical Characterization of Coarse Lake Spray Aerosol Particle from Lake Michigan

    NASA Astrophysics Data System (ADS)

    Ault, A. P.; Axson, J. L.; May, N.; Pratt, K.; Colon-Bernal, I. D.

    2015-12-01

    Wave breaking across bodies of water releases coarse particles into the air which can impact climate and human health. Freshwater lakes, such as the Great Lakes, can generate lake spray aerosols (LSA), similarly to how sea spray is generated, during periods of high winds and wave action. This LSA has the potential to impact climate through direct and indirect effects (ie. scattering/absorption and cloud nucleation) and are suggested to impact human health via inhalation of these particles during algal bloom periods characterized by toxic cyanobacteria. Very few studies have been conducted to assess the physicochemical properties of freshwater LSA. Prior work in our lab included the construction and characterization of a laboratory based LSA generator. In this work, we examine laboratory generated aerosol particles from laboratory based freshwater standards, freshwater samples collected from Lake Michigan, and ambient particles collected during a wave event on the shores of Lake Michigan in the summer of 2015. Particle size distributions, number concentrations, and chemical composition are presented and discussed as a function of laboratory generated and ambient collected LSA. Results indicate that there are characteristic particles that represent LSA. This study represents the next step towards evaluating and understanding the potential for coarse LSA to impact climate and health in the Great Lakes region.

  16. Composition of Stratospheric Aerosol Particles collected during the SOLVE campaign 2000

    NASA Astrophysics Data System (ADS)

    Schütze, Katharina; Nathalie, Benker; Martin, Ebert; Ralf, Weigel; Wilson James, C.; Stephan, Borrmann; Stephan, Weinbruch

    2016-04-01

    Stratospheric Aerosol particles were collected during the SAGE III Ozone loss and validation Experiment (SOLVE) in January-March 2000 in Kiruna/ Sweden onboard the scientific ER-2 aircraft with the Multi-Sample Aerosol Collection System. The particles are deposited on Cu transmission electron microscopy (TEM) grids. Particles of six samples from different flights (including one PSC sample) were analyzed by TEM and Energy Dispersive X-ray detection (EDX) regarding their size, chemical composition and morphology. Most particles are sulfates (formed from droplets of sulfuric acid) which are not resistant to the electron beam. In addition, refractory particles in the size range of 100-500 nm are found. They are either embedded in the sulfates or occur as single particles. The refractory particles are mainly carbonaceous showing only C and O as major peaks in their X-ray spectra. Some particles contain minor amounts of Si and Fe. Both, the O/C (median from 0.10-0.40), as well as Si/C (median from 0.05-0.32) ratios are increasing with time, from the middle of January to the end of February. The largest Fe/C ratio (median: 0.37) is found in a sample of the end of January. Based on the nanostructure and the absence of potassium as a tracer, biomass burning can be excluded as a source. Soot from diesel engines as well as from aircrafts show a nanostructure which is not found in the refractory particles. Due to the fact that large volcanic eruptions, which introduced material directly into the stratosphere, were missing since the eruption of Mt. Pinatubo in 1991, they are a very unlikely source of the refractory particles. The most likely source of the refractory particles is thus extraterrestrial material.

  17. Modal structure of chemical mass size distribution in the high Arctic aerosol

    NASA Astrophysics Data System (ADS)

    Hillamo, Risto; Kerminen, Veli-Matti; Aurela, Minna; MäKelä, Timo; Maenhaut, Willy; Leek, Caroline

    2001-11-01

    Chemical mass size distributions of aerosol particles were measured in the remote marine boundary layer over the central Arctic Ocean as part of the Atmospheric Research Program on the Arctic Ocean Expedition 1996 (AOE-96). An inertial impaction method was used to classify aerosol particles into different size classes for subsequent chemical analysis. The particle chemical composition was determined by ion chromatography and by the particle-induced X-ray emission technique. Continuous particle size spectra were extracted from the raw data using a data inversion method. Clear and varying modal structures for aerosols consisting of primary sea-salt particles or of secondary particles related to dimethyl sulfide emissions were found. Concentration levels of all modes decreased rapidly when the distance from open sea increased. In the submicrometer size range the major ions found by ion chromatography were sulfate, methane sulfonate, and ammonium. They had most of the time a clear Aitken mode and one or two accumulation modes, with aerodynamic mass median diameters around 0.1 μm, 0.3 μm, and between 0.5-1.0 μm, respectively. The overall submicron size distributions of these three ions were quite similar, suggesting that they were internally mixed over most of this size range. The corresponding modal structure was consistent with the mass size distributions derived from the particle number size distributions measured with a differential mobility particle sizer. The Aitken to accumulation mode mass ratio for nss-sulfate and MSA was substantially higher during clear skies than during cloudy periods. Primary sea-salt particles formed a mode with an aerodynamic mass median diameter around 2 μm. In general, the resulting continuous mass size distributions displayed a clear modal structure consistent with our understanding of the two known major source mechanisms. One is the sea-salt aerosol emerging from seawater by bubble bursting. The other is related to

  18. Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles

    NASA Astrophysics Data System (ADS)

    Massoli, P.; Lambe, A.; Ahern, A.; Williams, L. R.; Ehn, M.; Mikkila, J.; Canagaratna, M.; Brune, W. H.; Onasch, T. B.; Jayne, J.; Petdjd, T. T.; Kulmala, M. T.; Laaksonen, A.; Kolb, C. E.; Davidovits, P.; Worsnop, D. R.

    2010-12-01

    Laboratory experiments investigated the relationship between degree of oxidation and hygroscopic properties of secondary organic aerosol (SOA) particles. The hygroscopic growth factor (HGF), the CCN activity (κCCN) and the degree of aerosol oxidation (represented by the atomic O:C ratio) were measured for α-pinene, 1,3,5-trimethylbenzene (TMB), m-xylene and α pinene/m-xylene mixture SOA generated via OH radical oxidation in an aerosol flow reactor. Our results show that both HGF and κCCN increase with O:C. The TMB and m-xylene SOA were, respectively, the least and most hygroscopic of the system studied. An average HGF of 1.25 and a κCCN of 0.2 were measured at O:C of 0.65, in agreement with results reported for ambient data. The HGF based κ(κHGF) under predicted the κCCN values of 20 to 50% for all but the TMB SOA. Within the limitations of instrumental capabilities, we define the extent to which the hygroscopic properties of SOA particles can be predicted from their oxidation level and provide parameterizations suitable for interpreting ambient data.

  19. 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...

  20. Some physical and chemical properties of the arctic winter aerosol in Northeastern Canada

    NASA Astrophysics Data System (ADS)

    Leaitch, W. R.; Hoff, R. M.; Melnichuk, S.; Hogan, A. W.

    1984-06-01

    The results of surface and aircraft measurments of Arctic aerosol arriving at Igoolik, Northwest Territories, Canada during late February 1982 are reported. Concentrations of Aitken nuclei and cloud condensation nuclei as well as the aerosol light-scattering coefficient were measured several times a day. Little indication of any diurnal change in particle concentration was found in the size range betwen 0.2 and 4.0 millimicrons in diameter. A clear difference was detected in the quality of the air reaching Igoolik on one day, (Feb. 23) and this was associated with a doubling of the particle concentration the apparent particulate mass increased from about 6 to about 11 mg/cu. m. Over the same period impacted aerosols were composed of 15 to 50 percent water soluble compounds before 23 February and 40-100 percent thereafter. Sulfate was the dominant chemical species in all cases. Vertical profiles of the large aerosol particles obtained with an airborned nephelometer suggest a slightly enhanced concentration at the surface and a uniform concentration in the lower troposphere.

  1. 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.

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

    PubMed Central

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

    2012-01-01

    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

  3. 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.

  4. SPACCIM simulations of chemical aerosol-cloud interactions with the multiphase chemical mechanism MCM-CAPRAM3.0i

    NASA Astrophysics Data System (ADS)

    Tilgner, A.; Schrödner, R.; Bräuer, P.; Wolke, R.; Herrmann, H.

    2010-07-01

    Heterogeneous and multiphase processes in fog droplets, cloud droplets and deliquescent particles can potentially alter the physico-chemical composition of the tropospheric aerosol on global scale. In order to model such complex tropospheric multiphase chemical interactions of clouds, fogs and deliquescent aerosol particles, chemical mechanisms with a detailed description of chemical processes in both the gas and aqueous phase are required. Currently, both near-explicit gas and aqueous phase mechanisms are available. However, a near-explicit chemical multiphase mechanism was still missing. Therefore, the near-explicit chemical gas phase mechanism MCM v3 (Master Chemical Mechanism, Saunder et al., 2003) with about 13502 reactions and the explicit aqueous phase mechanism CAPRAM3.0i (Chemical Aqueous Phase Radical Mechanism, Herrmann et al., 2005) with about 777 reactions were coupled and integrated into the model framework SPACCIM (SPectral Aerosol Cloud Chemistry Interaction Model; Wolke et al., 2005). The parcel model SPACCIM combines a complex microphysical and multiphase chemistry model. First SPACCIM simulations have been carried out for different environmental conditions using a non-permanent cloud scenario. The model studies were aimed to investigate multiphase chemistry in tropospheric deliquescent aerosol particles, fogs and clouds in more detail. The model investigations were focused on the multiphase chemistry of tropospheric radical oxidants such as OH and NO3, organic compounds and closely linked chemical subsystems. The model results have been analysed including time-resolved reaction flux analyses. The obtained model results of the near-explicit multiphase mechanism MCM-CAPRAM3.0i have been compared with results of former model studies using the non-explicit gas phase mechanism RACM-MIM2ext and CAPRAM3.0i (Tilgner and Herrmann, 2010). Herrmann, H., Tilgner, A., Barzaghi, P., Majdik, Z., Gligorovski, S., Poulain, L., and Monod, A.: Towards a more

  5. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state: CLOUD ACTIVATION BY AGED ORGANIC AEROSOL

    DOE PAGES

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; ...

    2017-02-04

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation ofmore » liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.« less

  6. Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols.

    PubMed

    Mills, Jessica B; Park, Jae Hong; Peters, Thomas M

    2013-01-01

    We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride [NaCl] and spark-generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, <10(3); Medium, 10(3)-10(4); and High, >10(4) particles/cm(3)). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared with those measured with reference instruments, a scanning mobility particle sizer (SMPS), and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 16% of those measured by the CPC for polydispersed aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +101% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm, but caution should be exercised when particles larger than 300 nm are present. [Supplementary materials are available for this article. Go to the publisher's online edition of the Journal of Occupational and Environmental Hygiene for the following free supplemental resources: manufacturer-reported capabilities of instruments used, and information from the SMPS measurements for polydispersed test particles.].

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  8. Aerosols near by a coal fired thermal power plant: chemical composition and toxic evaluation.

    PubMed

    Jayasekher, T

    2009-06-01

    Industrial processes discharge fine particulates containing organic as well as inorganic compounds into the atmosphere which are known to induce damage to cell and DNA, both in vitro and in vivo. Source and area specific studies with respect to the chemical composition, size and shape of the particles, and toxicity evaluations are very much limited. This study aims to investigate the trace elements associated with the aerosol particles distributed near to a coal burning thermal power plant and to evaluate their toxicity through Comet assay. PM(10) (particles determined by mass passing an inlet with a 50% cut-off efficiency having a 10-microm aerodynamic diameter) samples were collected using respirable dust samplers. Twelve elements (Cr, Mn, Fe, Co, Ni, Cu, Zn, Cd, Pb, Se, Hg, and As) were analyzed using ICP-AES. Comet assay was done with the extracts of aerosols in phosphate buffered saline (PBS). Results show that Fe and Zn were found to be the predominant elements along with traces of other analyzed elements. Spherical shaped ultrafine particles of <1 microm aerodynamic diameter were detected through scanning electron microscope. PM(10) particles near to the coal burning power plant produced comets indicating their potential to induce DNA damage. DNA damage property is found to be depending upon the chemical characteristics of the components associated with the particles besides the physical properties such as size and shape.

  9. Introductory lecture: atmospheric organic aerosols: insights from the combination of measurements and chemical transport models.

    PubMed

    Pandis, Spyros N; Donahue, Neil M; Murphy, Benjamin N; Riipinen, Ilona; Fountoukis, Christos; Karnezi, Eleni; Patoulias, David; Skyllakou, Ksakousti

    2013-01-01

    The formation, atmospheric evolution, properties, and removal of organic particulate matter remain some of the least understood aspects of atmospheric chemistry despite the importance of organic aerosol (OA) for both human health and climate change. Here, we summarize our recent efforts to deal with the chemical complexity of the tens of thousands of organic compounds in the atmosphere using the volatility-oxygen content framework (often called the 2D-Volatility Basis Set, 2D-VBS). Our current ability to measure the ambient OA concentration as a function of its volatility and oxygen to carbon (O:C) ratio is evaluated. The combination of a thermodenuder, isothermal dilution and Aerosol Mass Spectrometry (AMS) together with a mathematical aerosol dynamics model is a promising approach. The development of computational modules based on the 2D-VBS that can be used in chemical transport models (CTMs) is described. Approaches of different complexity are tested against ambient observations, showing the challenge of simulating the complex chemical evolution of atmospheric OA. The results of the simplest approach describing the net change due to functionalization and fragmentation are quite encouraging, reproducing both the observed OA levels and O : C in a variety of conditions. The same CTM coupled with source-apportionment algorithms can be used to gain insights into the travel distances and age of atmospheric OA. We estimate that the average age of OA near the ground in continental locations is 1-2 days and most of it was emitted (either as precursor vapors or particles) hundreds of kilometers away. Condensation of organic vapors on fresh particles is critical for the growth of these new particles to larger sizes and eventually to cloud condensation nuclei (CCN) sizes. The semivolatile organics currently simulated by CTMs are too volatile to condense on these tiny particles with high curvature. We show that chemical aging reactions converting these semivolatile

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

    SciTech Connect

    Novick, Vincent J.

    1997-12-01

    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.

  11. 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.

  12. Aerosol mass spectrometry: particle-vaporizer interactions and their consequences for the measurements

    NASA Astrophysics Data System (ADS)

    Drewnick, F.; Diesch, J.-M.; Faber, P.; Borrmann, S.

    2015-04-01

    The Aerodyne Aerosol Mass Spectrometer (AMS) is a frequently used instrument for on-line measurement of the ambient sub-micron aerosol composition. With the help of calibrations and a number of assumptions on the flash vaporization and electron impact ionization processes this instrument provides robust quantitative information on various ambient aerosol components. However, when measuring close to certain anthropogenic sources or in marine environments, several of these assumptions may not be met and measurement results might easily be misinterpreted. Here we discuss various aspects of the interaction of aerosol particles with the AMS tungsten vaporizer and the consequences for the measurement results: semi-refractory components, i.e. components that vaporize but do not flash vaporize at the vaporizer and ionizer temperatures, like metal halides (e.g. chlorides, bromides or iodides of Al, Ba, Cd, Cu, Fe, Hg, K, Na, Pb, Sr, Zn) can be measured semi-quantitatively despite their relatively slow vaporization from the vaporizer. Even though non-refractory components (e.g. NH4NO3 or (NH4)2SO4) vaporize quickly, their differences in vaporization kinetics can result in undesired biases in ion collection efficiency in the measurements. Chemical reactions with water vapor and oxygen from the aerosol flow can have an influence on the mass spectra for certain components (e.g. NH4NO3, (NH4)2SO4, organic species). Finally, chemical reactions of the aerosol with the vaporizer surface can result in additional signals in the mass spectra (e.g. WO2C2-related signals from particulate Cl) and in conditioning or contamination of the vaporizer with potential memory effects influencing the mass spectra of subsequent measurements. Laboratory experiments that investigate these particle-vaporizer interactions are presented and are discussed together with field results showing that measurements of typical continental or urban aerosols are not significantly affected while laboratory

  13. Aging of Soot Particles: Remote Marine Free-tropospheric Aerosol at the Pico Mountain Observatory, Azores

    NASA Astrophysics Data System (ADS)

    China, S.; Mazzoleni, C.; Mazzoleni, L. R.; kumar, S.; Dziobak, M.; Fialho, P. J.; Dzepina, K.; Hueber, J.; Helmig, D.; Kramer, L. J.; Sharma, N.; Olsen, S. C.; Owen, R. C.

    2013-12-01

    Soot particles, often referred to as black carbon, are aggregates of carbonaceous monomers that strongly absorb light, significantly impacting the environment, Earth's radiation balance, atmospheric chemistry and properties of clouds. Soot can be transported over long distances, thus affecting global climate. During transport, soot aggregates undergo chemical and morphological changes such as oxidation, mixing, coating and restructuring. These changes have a significant impact on soot's light absorption and scattering efficiencies, and therefore on soot's effects on climate. Free tropospheric aerosols are being studied at the Pico Mountain Observatory, located near the top of the Pico Volcano in the Azores, Portugal (38.47°N, 28.40°W, 2225m asl). Typically above the marine boundary layer, this is an ideal site to study aerosol transported over long distances across the ocean, often from North America and sometimes from Africa and Europe. We studied the morphology and mixing state of individual soot particles using electron microscopy and energy dispersive X-ray spectroscopy. We also measured the optical properties of aerosols using light scattering data from a 3-wavelength nephelometer, and black carbon mass equivalent concentrations using a 7-wavelength aethalometer. In this presentation, we focus on samples collected during two events in July 2012. Back trajectory analysis shows that in both periods the air masses reaching Pico were traveling from west to east, apparently originating in North America. Soot particles were classified into four categories based on their coating and mixing state. We investigated the morphology of soot particles in the four categories, using various descriptors (e.g. aspect ratio, roundness and convexity), monomer size and fractal dimension. Most of the soot particles were coated. Bare or very thinly coated soot, exhibited very compacted structures and high convexity. The results of this study have implications on how soot particles

  14. 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.

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

    PubMed Central

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

    2013-01-01

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

  16. An investigation into particle shape effects on the light scattering properties of mineral dust aerosol

    NASA Astrophysics Data System (ADS)

    Meland, Brian Steven

    Mineral dust aerosol plays an important role in determining the physical and chemical equilibrium of the atmosphere. The radiative balance of the Earth's atmosphere can be affected by mineral dust through both direct and indirect means. Mineral dust can directly scatter or absorb incoming visible solar radiation and outgoing terrestrial IR radiation. Dust particles can also serve as cloud condensation nuclei, thereby increasing albedo, or provide sites for heterogeneous reactions with trace gas species, which are indirect effects. Unfortunately, many of these processes are poorly understood due to incomplete knowledge of the physical and chemical characteristics of the particles including dust concentration and global distribution, as well as aerosol composition, mixing state, and size and shape distributions. Much of the information about mineral dust aerosol loading and spatial distribution is obtained from remote sensing measurements which often rely on measuring the scattering or absorption of light from these particles and are thus subject to errors arising from an incomplete understanding of the scattering processes. The light scattering properties of several key mineral components of atmospheric dust have been measured at three different wavelengths in the visible. In addition, measurements of the scattering were performed for several authentic mineral dust aerosols, including Saharan sand, diatomaceous earth, Iowa loess soil, and palagonite. These samples include particles that are highly irregular in shape. Using known optical constants along with measured size distributions, simulations of the light scattering process were performed using both Mie and T-Matrix theories. Particle shapes were approximated as a distribution of spheroids for the T-Matrix calculations. It was found that the theoretical model simulations differed markedly from experimental measurements of the light scattering, particularly near the mid-range and near backscattering angles. In

  17. Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles

    NASA Astrophysics Data System (ADS)

    Massoli, P.; Lambe, A. T.; Ahern, A. T.; Williams, L. R.; Ehn, M.; Mikkilä, J.; Canagaratna, M. R.; Brune, W. H.; Onasch, T. B.; Jayne, J. T.; Petäjä, T.; Kulmala, M.; Laaksonen, A.; Kolb, C. E.; Davidovits, P.; Worsnop, D. R.

    2010-12-01

    Laboratory experiments investigated the relationship between oxidation level and hygroscopic properties of secondary organic aerosol (SOA) particles generated via OH radical oxidation in an aerosol flow reactor. The hygroscopic growth factor at 90% RH (HGF90%), the CCN activity ($\\kappa$ORG,CCN) and the level of oxidation (atomic O:C ratio) of the SOA particles were measured. Both HGF90% and $\\kappa$ORG,CCN increased with O:C; the HGF90% varied linearly with O:C, while $\\kappa$ORG,CCN mostly followed a nonlinear trend. An average HGF90% of 1.25 and $\\kappa$ORG,CCN of 0.19 were measured for O:C of 0.65, in agreement with results reported for ambient data. The $\\kappa$ORG values estimated from the HGF90% ($\\kappa$ORG,HGF) were 20 to 50% lower than paired $\\kappa$ORG,CCN values for all SOA particles except 1,3,5-trimethylbenzene (TMB), the least hygroscopic of the SOA systems. Within the limitations of instrumental capabilities, we show that differences in hygroscopic behavior among the investigated SOA systems may correspond to differences in elemental composition.

  18. Source apportionment of aerosol particles near a steel plant by electron microscopy.

    PubMed

    Ebert, Martin; Müller-Ebert, Dörthe; Benker, Nathalie; Weinbruch, Stephan

    2012-12-01

    The size, morphology and chemical composition of 37,715 individual particles collected over 22 sampling days in the vicinity of a large integrated steel production were studied by scanning and transmission electron microscopy. Based on the morphology, chemistry and beam stability the particles were classified into the following fourteen groups: silicates, sea salt, calcium sulfates, calcium carbonates, carbonate-silicate mixtures, sulfate-silicate mixtures, iron oxides, iron mixtures, metal oxide-metals, complex secondary particles, soot, Cl-rich particles, P-rich particles, and other particles. The majority of iron oxide (≈85%) and metal oxide-metal (≈70%) particles as well as ≈20% of the silicate particles are fly ashes from high temperature processes. The emissions from the steel work are dominated by iron oxide particles. For source apportionment, seven source categories and two sectors of local wind direction (industrial and urban background) were distinguished. In both sectors PM₁₀ consists of four major source categories: 35% secondary, 20% industrial, 17% soil and 16% soot in the urban background sector compared to 45% industrial, 20% secondary, 13% soil, and 9% soot in the industrial sector. As the secondary and the soot components are higher in the urban background sector than in the industrial sector, it is concluded that both components predominantly originate from urban background sources (traffic, coal burning, and domestic heating). Abatement measures should not only focus on the steel work but should also include the urban background aerosol.

  19. 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

    Stable carbon and nitrogen isotope ratio are successfully used in the atmospheric aerosol particle source identification [1, 2], transformation, pollution [3] research. The main purpose of this study was to evaluate the penetration of atmospheric aerosol particles from outdoor to indoor using stable carbon and nitrogen isotope ratios. Six houses in Kaunas (Lithuania) were investigated during February and March 2013. Electrical low pressure impactor was used to measure in real time concentration and size distribution of outdoor aerosol particles. ELPI+ includes 15 channels covering the size range from 0.017 to 10.0 µm. The 25 mm diameter aluminium foils were used to collect aerosol particles. Gravimetric analysis of samples was made using microbalance. In parallel, indoor aerosol samples were collected with a micro-orifice uniform deposition impactor (MOUDI model 110), where the aerosol particles were separated with the nominal D50 cut-off sizes of 0.056, 0.1, 0.18,0.32,0.56, 1.0, 1.8, 3.2, 5.6, 10, 18 μm for impactor stages 1-11, respectively. The impactor was run at a flow rate of 30 L/min. Air quality meters were used to record meteorological conditions (temperature, relative humidity) during the investigated period. All aerosol samples were analyzed for total carbon (TC) and total nitrogen (TN) contents and their isotopic compositions using elemental analyzer (EA) connected to the stable isotope ratio mass spectrometer (IRMS). TC concentration in indoors ranged from 1.5 to 247.5 µg/m3. During the sampling period outdoors TN levels ranged from 0.1 to 10.9 µg/m3. The obtained outdoor δ13C(PM2.5) values varied from -24.21 to -26.3‰, while the δ15N values varied from 2.4 to 11.1 ‰ (average 7.2±2.5 ‰). Indoors carbonaceous aerosol particles were depleted in 13C compared to outdoors in all sampling sites. This depletion in δ13C varied from 0.1 to 3.2 ‰. We think that this depletion occurs due ongoing chemical reactions (oxidation) when aerosol

  20. Characterization of Individual Aerosol Particles Associated with Clouds (CRYSTAL-FACE)

    NASA Technical Reports Server (NTRS)

    Buseck, Peter R.

    2004-01-01

    The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from near the bottoms and tops of the deep convective systems that lead to the generation of tropical cirrus clouds and to provide insights into the particles that serve as CCN or IN. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to compare the compositions, concentrations, size distributions, shapes, surface coatings, and degrees of aggregation of individual particles from cloud bases and the anvils near the tropopause. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are abundant in in-cloud samples. Cirrus samples contain many H2SO4 droplets, but acidic sulfate particles are rare at the cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. The relatively high extent of ammoniation in the upper troposphere in-cloud samples appears to have resulted from vertical transport by strong convection. The morphology of H2SO4 droplets indicates that they had been at least yartiy ammoniated at the time of collection. They are internally mixed with organic materials, metal sulfates, and solid particles of various compositions. Ammoniation and internal mixing of result in freezing at higher temperature than in pure H2SO4 aerosols. K- and S-bearing organic particles and Si-Al-rich particles are common throughout. Sea salt and mineral dust were incorporated into the convective systems from the cloud bases and worked as ice nuclei while being vertically transported. The nonsulfate particles originated from the lower troposphere and were transported to the upper troposphere and lower stratosphere.

  1. Characterization of Atmospheric Aerosol Particles from a Mining City in Southwest China Using Electron Probe microanalysis

    NASA Astrophysics Data System (ADS)

    Cheng, X.; Huang, Y.; Lu, H., III; Liu, Z., IV; Wang, N. V.

    2015-12-01

    Xin Cheng1, Yi Huang1*, Huilin Lu2, Zaidong Liu2, Ningming Wang21 Key Laboratory of Geological Nuclear Technology of Sichuan Province, College of Earth Science, Chengdu University of Technology, Chengdu 610059, China. ; E-mail:chengxin_cdut@163.com 2 College of Earth Science, Chengdu University of Technology, Chengdu 610059, China. ; *Corresponding author: E-mail: huangyi@cdut.cn Panzhihua is a mining city located at Pan-Xi Rift valley, southwest China. It has a long industrial history of vanadium-titanium magnetite mining, iron and steel smelting, and coal-fired power plants. Atomospheric environment has been seriously contaminated with airborne paticles, which is threatening human health.The harmful effects of aerosols are dependent on certain characteristics such as microphysical properties. However, few studsies have been carried out on morphological information contained on single atmospheric particles in this area. In this study, we provide a detailed morphologically and chemically characterization of airborne particles collected at Panzhihua city in October, 2014, using a quantitative single particle analysis based on EPXMA. The results indicate that based on their chemical composition, five major types of particles were identified. Among these, aluminosilicate particles have typical spherical shapes and are produced during the high-temperature combustion; Fe-containing particles contains high level of Mn, and more likely originated from mineralogical and steel industry; Si-containing particles can originate from mineralogical source; V-Ti-Mn-containing particles are also produced by steel industry; Ca-containing particles,these particles are CaCO3, mainly from the mining of limestone mine. The results help us on tracing and partitioning different sources of atomospheric particles in the industrial area. Fig.1 Fe-rich shperical particles

  2. 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.

  3. 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.

  4. Concentrations, size distributions and temporal variations of fluorescent biological aerosol particles in southern tropical India

    NASA Astrophysics Data System (ADS)

    Valsan, Aswathy; Krishna R, Ravi; CV, Biju; Huffman, Alex; Poschl, Ulrich; Gunthe, Sachin

    2015-04-01

    Biological aerosols constitute a wide range of dead and alive biological materials and structures that are suspended in the atmosphere. They play an important role in the atmospheric physical, chemical and biological processes and health of living being by spread of diseases among humans, plants, and, animals. The atmospheric abundance, sources, physical properties of PBAPs as compared to non-biological aerosols, however, is poorly characterized. The Indian tropical region, where large fraction of the world's total population is residing, experiences a distinctive meteorological phenomenon by means of Indian Summer Monsoon (IMS). Thus, the properties and characteristics of biological aerosols are also expected to be very diverse over the Indian subcontinent depending upon the seasons. Here we characterize the number concentration and size distribution of Fluorescent Biological Aerosol Particles (FBAP) at a high altitude continental site, Munnar (10.09 N, 77.06 E; 1605 m asl) in South India during the South-West monsoon, which constitute around 80 percent of the annual rainfall in Munnar. Continuous three months measurements (from 01 June 2014 to 21 Aug 2104) FBAPs were carried out at Munnar using Ultra Violet Aerodynamic Particle Sizer (UVAPS) during IMS. The mean number and mass concentration of coarse FBAP averaged over the entire campaign was 1.7 x 10-2 cm-3 and 0.24 µg m-3 respectively, which corresponds to 2 percent and 6 percent of total aerosol particle number and mass concentration. In agreement to other previous measurements the number size distribution of FBAP also peaks at 3.2 micron indicating the strong presence of fungal spores. This was also supported by the Scanning Electron Microscopic analysis of bioaerosols on filter paper. They also displayed a strong diurnal cycle with maximum concentration occurring at early morning hours. During periods of heavy and continuous rain where the wind is consistently blowing from South-West direction it was

  5. Measurement of the nucleation of atmospheric aerosol particles.

    PubMed

    Kulmala, Markku; Petäjä, Tuukka; Nieminen, Tuomo; Sipilä, Mikko; Manninen, Hanna E; Lehtipalo, Katrianne; Dal Maso, Miikka; Aalto, Pasi P; Junninen, Heikki; Paasonen, Pauli; Riipinen, Ilona; Lehtinen, Kari E J; Laaksonen, Ari; Kerminen, Veli-Matti

    2012-09-01

    The formation of new atmospheric aerosol particles and their subsequent growth have been observed frequently at various locations all over the world. The atmospheric nucleation rate (or formation rate) and growth rate (GR) are key parameters to characterize the phenomenon. Recent progress in measurement techniques enables us to measure atmospheric nucleation at the size (mobility diameter) of 1.5 (±0.4) nm. The detection limit has decreased from 3 to 1 nm within the past 10 years. In this protocol, we describe the procedures for identifying new-particle-formation (NPF) events, and for determining the nucleation, formation and growth rates during such events under atmospheric conditions. We describe the present instrumentation, best practices and other tools used to investigate atmospheric nucleation and NPF at a certain mobility diameter (1.5, 2.0 or 3.0 nm). The key instruments comprise devices capable of measuring the number concentration of the formed nanoparticles and their size, such as a suite of modern condensation particle counters (CPCs) and air ion spectrometers, and devices for characterizing the pre-existing particle number concentration distribution, such as a differential mobility particle sizer (DMPS). We also discuss the reliability of the methods used and requirements for proper measurements and data analysis. The time scale for realizing this procedure is 1 year.

  6. Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the Southeast Pacific ocean

    NASA Astrophysics Data System (ADS)

    Twohy, C. H.; Anderson, J. R.; Toohey, D. W.; Andrejczuk, M.; Adams, A.; Lytle, M.; George, R. C.; Wood, R.; Saide, P.; Spak, S.; Zuidema, P.; Leon, D.

    2012-08-01

    The Southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles such as power plants, urban pollution and smelters on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics from seven flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were more numerous and smaller near shore, and there was less drizzle. Higher droplet number concentration and physically thinner clouds both contributed to the smaller droplets near shore. Satellite measurements were used to show that cloud albedo was highest 500-1000 km offshore, and actually lower closer to shore due to the generally thinner clouds and lower liquid water paths there. Differences in the size

  7. Determining aerosol particles by in-air micro-IL analysis combined with micro-PIXE

    NASA Astrophysics Data System (ADS)

    Kada, Wataru; Satoh, Takahiro; Yokoyama, Akihito; Koka, Masashi; Kamiya, Tomihiro

    2013-07-01

    A new external ion microbeam ion luminescence (micro-IL) imaging system was developed on a microbeam line of a 3 MV single-ended accelerator at the TIARA facility of the Japan Atomic Energy Agency. Micro-IL was combined with an in-air micro-PIXE (particle-induced X-ray emission) system to determine the chemical composition and structures of microscopic airborne particles of several micrometers in size. The hardware and software for the combined in-air micro-IL analysis system, called ion luminescence microscopic imaging and spectroscopy (ILUMIS), were studied. Wavelength-dispersive optics, including a collimator lens, a monochromator, and a photon-counting photomultiplier, were installed on the beam line. The signal processing of the IL photon signals, which were collected as spectra and two-dimensional microscopic images, was examined. Several aerosol particles were characterized to demonstrate the ILUMIS/PIXE combined analysis. The external microbeam ILUMIS analysis method provided a variety of information on the chemical and elemental composition of the micrometer-sized aerosol targets under ambient atmospheric conditions.

  8. Determination of the passing efficiency for aerosol chemical species through a typical aircraft-mounted, diffuser-type aerosol inlet system

    NASA Astrophysics Data System (ADS)

    Sheridan, Patrick J.; Norton, Richard B.

    1998-04-01

    To assess the particle transmission efficiency of a conventional aircraft-mounted, diffuser-type inlet (CI), a new design inlet containing an internal filter basket assembly (aerosol filter inlet, or AFI) was constructed. All interior surfaces of the AFI were covered with filter material, and air was actively pulled through these filter walls during aerosol sampling. The AFI was demonstrated in the laboratory to trap nearly all particles entering its nozzle orifice, so it was considered usable as a baseline to judge the performance of other inlets. Wind tunnel studies were conducted at three different wind velocities that approximated typical research aircraft speeds. As wind velocity increased, particle transmission through the CI relative to the AFI decreased, as evidenced by chemical analysis of the filter deposits. Aircraft studies of the two inlets showed that particle transmission varied significantly with the measured species. Typical coarse-particle species such as Ca++, Mg++, Na+ and K+ showed 50-90% mass losses through a conventional diffuser-type inlet/curved intake tube system. Predominantly fine particle species such as SO4= and NH4+ passed the CI system with much higher efficiencies, with aerosol mass losses of 0-26% for most flights. Since the AFI traps nearly all particles aspirated into its nozzle orifice, these values indicate that on average, 80-90% of the SO4= and NH4+ aerosol mass passes through the CI and curved intake tube during airborne sampling. This finding suggests that the capability to sample fine (i.e., submicrometer) aerosols from aircraft is perhaps not as bad as has been previously reported, given that adequate attention is paid to inlet design, location, and orientation issues.

  9. Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

    NASA Astrophysics Data System (ADS)

    Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

    2016-04-01

    arises mainly from fossil fuel sources, whereas OC in larger particles from 200 nm to 1 μm has higher contribution from biomass burning/other sources. Moreover, there is a clear distinction in source contribution between the more volatile OC fraction and the more refractory fraction. The more refractory fraction is enriched in 13C by 1 to 2 ‰ for both small and large particles. These results show that the fossil fuel combustion is associated to a larger degree with more volatile carbon, whereas biomass burning is the main source of the more refractory particles. According to our source apportionment, the more volatile carbon fraction in the smallest particles is almost completely from fossil fuels, whereas the more refractory carbon fraction in the large size range is almost complete from biomass burning. The more refractory small particles and the less refractory large particles are roughly an even mix of these two sources. The detailed chemical speciation of the carbonaceous aerosol will be presented as well. Acknowledgements This study was funded by the Dutch Science Foundation (NWO grants Nr. 820.01.001, and 834.08.002).

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

    NASA Astrophysics Data System (ADS)

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

    2014-04-01

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

  11. 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

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

    SciTech Connect

    Lohmann,U.; Schwartz, S. E.

    2008-03-02

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

  13. SPACCIM simulations of chemical aerosol-cloud interactions with the multiphase chemistry mechanism MCM-CAPRAM3.0

    NASA Astrophysics Data System (ADS)

    Tilgner, A.; Schroedner, R.; Braeuer, P.; Wolke, R.; Herrmann, H.

    2010-12-01

    A wide variety of organic compounds is emitted into the troposphere and is then oxidised by complex multiphase degradations leading to secondary organics which partition between the tropospheric gas and aqueous phase, i.e. deliquescent particles and cloud droplets. Secondary organics play a key role in tropospheric chemistry and account for a substantial fraction of tropospheric aerosol mass. Heterogeneous and multiphase processes in fog droplets, cloud droplets and deliquescent particles can potentially alter the physico-chemical composition of the tropospheric aerosol on global scale. However, the chemical multiphase processing, i.e. secondary formation and aging mainly of organic aerosols remains poorly considered in current multiphase chemical mechanisms and models. In order to model such complex tropospheric multiphase chemical interactions of clouds, fogs and deliquescent aerosol particles, chemical mechanisms with a detailed description of chemical processes in both the gas and aqueous phase are required. Currently, both near-explicit gas and aqueous phase mechanisms are available. However, a near-explicit chemical multiphase mechanism was still missing. Therefore, the near-explicit chemical gas phase mechanism MCM v3 (Master Chemical Mechanism) with about 13502 reactions and the explicit aqueous phase mechanism CAPRAM3.0n (Chemical Aqueous Phase Radical Mechanism) with about 777 reactions were coupled and integrated into the model framework SPACCIM (SPectral Aerosol Cloud Chemistry Interaction Model). The parcel model SPACCIM combines a complex microphysical and multiphase chemistry model. First SPACCIM simulations have been carried out for different environmental conditions using a non-permanent cloud scenario. The model studies were aimed to investigate multiphase chemistry in tropospheric deliquescent aerosol particles, fogs and clouds in more detail. The present model studies were focused on multiphase chemistry of tropospheric oxidants and closely

  14. Chemical and Physical Properties of Bulk Aerosols within Four Sectors Observed during TRACE-P

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

    Chemical and physical aerosol data collected on the DC-8 during TRACE-P were grouped into four sectors based on back trajectories. The four sectors represent long-range transport from the west (WSW), regional circulation over the western Pacific and Southeast Asia (SE Asia), polluted transport from Northern Asia with substantial sea salt at low altitudes (NNW) and a substantial amount of dust (Channel). WSW has generally low mixing ratios at both middle and high altitudes, with the bulk of the aerosol mass due to non-sea-salt water-soluble inorganic species. Low altitude SE Asia also has low mean mixing ratios in general, with the majority of the aerosol mass comprised of non-sea-salts, however, soot is also relatively important m this region. "w had the highest mean sea salt mixing ratios, with the aerosol mass at low altitudes (a km) evenly divided between sea salts, mm-sea-salts, and dust. The highest mean mixing ratios of water-soluble ions and soot were observed at the lowest altitudes (a km) in the Channel sector. The bulk of the aerosol mass exported from Asia emanates h m Channel at both low and midaltitudes, due to the prevalence of dust compared to other sectors. Number densities show enhanced fine particles for Channel and NNW, while their volume distributions are enhanced due to sea salt and dust Low-altitude Channel exhibits the highest condensation nuclei ((34) number densities along with enhanced scattering coefficients, compared to the other sectors. At midaltitudes (2-7 km), low mean CN number densities coupled with a high proportion of nonvolatile particles (265%) observed in polluted sectors (Channel and NNW) are attributed to wet scavenging which removes hygroscopic CN particles. Low single scatter albedo m SE Asia reflects enhanced soot

  15. Investigate the relationship between multiwavelength lidar ratios and aerosol size distributions using aerodynamic particle sizer spectrometer

    NASA Astrophysics Data System (ADS)

    Zhao, Hu; Hua, Dengxin; Mao, Jiandong; Zhou, Chunyan

    2017-02-01

    The real aerosol size distributions were obtained by aerodynamic particle sizer spectrometer (APS) in China YinChuan. The lidar ratios at wavelengths of 355 nm, 532 nm and 1064 nm were calculated using Mie theory. The effective radius of aerosol particles reff and volume C/F ratio (coarse/fine) Vc/f were retrieved from the real aerosol size distributions. The relationship between multiwavelength lidar ratios and particle reff and Vc/f were investigated. The results indicate that the lidar ratio is positive correlated to the particle reff and Vc/f. The lidar ratio is more sensitive to the coarse particles. The short wavelength lidar ratio is more sensitive to the particle Vc/f and the long wavelength lidar ratio is more sensitive to the particle reff. The wavelength dependency indicated that the lidar ratios decrease with increasing the wavelength. The lidar ratios are almost irrelevant to the shape and total particles of aerosol size distributions.

  16. Aerosol effective density measurement using scanning mobility particle sizer and quartz crystal microbalance with the estimation of involved uncertainty

    NASA Astrophysics Data System (ADS)

    Sarangi, Bighnaraj; Aggarwal, Shankar G.; Sinha, Deepak; Gupta, Prabhat K.

    2016-03-01

    . It was found that in general, mid-day effective density of ambient aerosols increases with increase in CMD of particle size measurement but particle photochemistry is an important factor to govern this trend. It is further observed that the CMD has good correlation with O3, SO2 and ambient RH, suggesting that possibly sulfate secondary materials have a substantial contribution in particle effective density. This approach can be useful for real-time measurement of effective density of both laboratory-generated and ambient aerosol particles, which is very important for studying the physico-chemical properties of particles.

  17. Aerosol effective density measurement using scanning mobility particle sizer and quartz crystal microbalance with the estimation of involved uncertainty

    NASA Astrophysics Data System (ADS)

    Sarangi, B.; Aggarwal, S. G.; Sinha, D.; Gupta, P. K.

    2015-12-01

    factor to govern this trend. It is further observed that the CMD has good correlation with O3, SO2 and ambient RH, suggesting that possibly sulfate secondary materials have substantial contribution in particle effective density. This approach can be useful for real-time measurement of effective density of both laboratory generated and ambient aerosol particles, which is very important for studying the physico-chemical property of particles.

  18. 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

  19. Biomass burning aerosol over the Amazon during SAMBBA: impact of chemical composition on radiative properties

    NASA Astrophysics Data System (ADS)

    Morgan, William; Allan, James; Flynn, Michael; Darbyshire, Eoghan; Hodgson, Amy; Liu, Dantong; O'shea, Sebastian; Bauguitte, Stephane; Szpek, Kate; Langridge, Justin; Johnson, Ben; Haywood, Jim; Longo, Karla; Artaxo, Paulo; Coe, Hugh

    2014-05-01

    Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. Globally, biomass burning aerosols are thought to exert a small warming effect but with the uncertainty being 4 times greater than the central estimate. On regional scales, the impact is substantially greater, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, both in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated

  20. 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.

  1. 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

  2. Modeling the chemistry of the marine boundary layer: Sulphate formation and the role of sea-salt aerosol particles

    NASA Astrophysics Data System (ADS)

    van den Berg, Ad; Dentener, Frank; Lelieveld, Jos

    2000-05-01

    A one-dimensional model is presented that interactively simulates the dynamics and the gas-aqueous phase chemistry of the cloud-topped marine boundary layer. The model is described and tested using observations from the Atlantic Stratocumulus Transition Experiment/Marine Aerosol and Gas Exchange (ASTEX/MAGE) measurement campaign. The comparison generally indicates satisfactory agreement for dynamical properties and chemical species, except for SO2. We present several explanations for this discrepancy. However, a conclusive account is dependent on quantitative information about free tropospheric SO2 and H2O2 that is not available. Furthermore, a series of sensitivity runs is presented to explain the large quantities of non-sea-salt sulphate associated with sea-salt particles, as observed during ASTEX/MAGE. The main conclusions are that most sulphate associated with sea-salt particles is formed in cloud droplets that subsequently evaporate and that only a small amount is formed in deliquesced aerosol particles. The model results are sensitive to changes in the assumed sea-salt emission rate and the overall aerosol size distribution. The latter indicates that a shift in the sea-salt aerosol distribution toward the smaller particle sizes might explain the observed amount of sulphate associated with sea-salt particles.

  3. 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

  4. Advanced spray-dried design, physicochemical characterization, and aerosol dispersion performance of vancomycin and clarithromycin multifunctional controlled release particles for targeted respiratory delivery as dry powder inhalation aerosols.

    PubMed

    Park, Chun-Woong; Li, Xiaojian; Vogt, Frederick G; Hayes, Don; Zwischenberger, Joseph B; Park, Eun-Seok; Mansour, Heidi M

    2013-10-15

    Respirable microparticles/nanoparticles of the antibiotics vancomycin (VCM) and clarithromycin (CLM) were successfully designed and developed by novel organic solution advanced spray drying from methanol solution. Formulation optimization was achieved through statistical experimental design of pump feeding rates of 25% (Low P), 50% (Medium P) and 75% (High P). Systematic and comprehensive physicochemical characterization and imaging were carried out using scanning electron microscopy (SEM), hot-stage microscopy (HSM), differential scanning calorimetry (DSC), X-ray powder diffraction (XRPD), Karl Fischer titration (KFT), laser size diffraction (LSD), gravimetric vapor sorption (GVS), confocal Raman microscopy (CRM) and spectroscopy for chemical imaging mapping. These novel spray-dried (SD) microparticulate/nanoparticulate dry powders displayed excellent aerosol dispersion performance as dry powder inhalers (DPIs) with high values in emitted dose (ED), respirable fraction (RF), and fine particle fraction (FPF). VCM DPIs displayed better aerosol dispersion performance compared to CLM DPIs which was related to differences in the physicochemical and particle properties of VCM and CLM. In addition, organic solution advanced co-spray drying particle engineering design was employed to successfully produce co-spray-dried (co-SD) multifunctional microparticulate/nanoparticulate aerosol powder formulations of VCM and CLM with the essential lung surfactant phospholipid, dipalmitoylphosphatidylcholine (DPPC), for controlled release pulmonary nanomedicine delivery as inhalable dry powder aerosols. Formulation optimization was achieved through statistical experimental design of molar ratios of co-SD VCM:DPPC and co-SD CLM:DPPC. XRPD and DSC confirmed that the phospholipid bilayer structure in the solid-state was preserved following spray drying. Co-SD VCM:DPPC and co-SD CLM:DPPC dry powder aerosols demonstrated controlled release of antibiotic drug that was fitted to various

  5. Mineralogical, chemical and toxicological characterization of urban air particles.

    PubMed

    Čupr, Pavel; Flegrová, Zuzana; Franců, Juraj; Landlová, Linda; Klánová, Jana

    2013-04-01

    Systematic characterization of morphological, mineralogical, chemical and toxicological properties of various size fractions of the atmospheric particulate matter was a main focus of this study together with an assessment of the human health risks they pose. Even though near-ground atmospheric aerosols have been a subject of intensive research in recent years, data integrating chemical composition of particles and health risks are still scarce and the particle size aspect has not been properly addressed yet. Filling this gap, however, is necessary for reliable risk assessment. A high volume ambient air sampler equipped with a multi-stage cascade impactor was used for size specific particle collection, and all 6 fractions were a subject of detailed characterization of chemical (PAHs) and mineralogical composition of the particles, their mass size distribution and genotoxic potential of organic extracts. Finally, the risk level for inhalation exposure associated to the carcinogenic character of the studied PAHs has been assessed. The finest fraction (<0.45 μm) exhibited the highest mass, highest active surface, highest amount of associated PAHs and also highest direct and indirect genotoxic potentials in our model air sample. Risk assessment of inhalation scenario indicates the significant cancer risk values in PM 1.5 size fraction. This presented new approach proved to be a useful tool for human health risk assessment in the areas with significant levels of air dust concentration.

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

    NASA Astrophysics Data System (ADS)

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

    2014-01-01

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

  7. Laboratory and Ambient Studies Using an Automated Semi-Continuous Single-Particle Aerosol Raman Spectrometer

    NASA Astrophysics Data System (ADS)

    Doughty, D., III; Hill, S. C.

    2015-12-01

    Single-particle Raman spectra can yield extensive information about in-situ ambient particulate composition. However, Raman spectral measurements of individual aerosol particles typically require collection of samples in the field followed by offline Raman spectral measurements in a laboratory. The process requires considerable operator time. We report results obtained with an automated, single-particle Aerosol Raman Spectrometer built by Battelle, which is the core of Battelle's Resource Effective Bioidentification System (REBS). This instrument collects aerosol particles onto a metallized polymer tape and simultaneously measures Raman spectra of particles obtained during the previous collection period. At the end of each collection period (typically 15 minutes), the tape is advanced and the next collection and measurement period is begun. In this way, particles are semi-continuously sampled and their Raman spectra are measured. We show laboratory data from different sizes of polystyrene latex spheres. We also show results from calcium sulfate particles, vehicular emission soot, and other particles. We discuss the influence of imaging time on the quality of the Raman spectra measured and on the ability of the instrument to resolve aerosol particles. Finally, we present results from an outdoor sampling period during the summer of 2015 where the instrument ran unattended for more than one week collecting particles and measuring their Raman spectra. We suggest that the routine use of such an automated particle-sampling instrument should increase our understanding of inorganic and organic aerosols including biological aerosols and sources and fates of these particles.

  8. Composition and hygroscopicity of aerosol particles at Mt. Lu in South China: Implications for acid precipitation

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Chi, Jianwei; Shi, Zongbo; Wang, Xinfeng; Chen, Bin; Wang, Yan; Li, Tao; Chen, Jianmin; Zhang, Daizhou; Wang, Zifa; Shi, Chune; Liu, Liangke; Wang, Wenxing

    2014-09-01

    Physicochemical properties of aerosol particles were studied at Mt. Lu, an elevated site (115°59‧E, 29°35‧N, 1165 m) within the acid precipitation area. Northeast winds transport copious amounts of air pollutants and water vapor from the Yangtze River Delta into this acid precipitation area. NH4+ and SO42- are the dominant ions in PM2.5 and determine aerosol acidity. Individual particle analysis shows abundant S-rich and metals (i.e. Fe-, Zn-, Mn-, and Pb-rich) particles. Unlike aerosol particles in North China and urban areas, there are little soot and mineral particles at Mt. Lu. Lack of mineral particles contributed to the higher acidity in precipitation in the research area. Nano-sized spherical metal particles were observed to be embedded in 37% of S-rich particles. These metal particles were likely originated from heavy industries and fired-power plants. Hygroscopic experiments show that most particles start to deliquesce at 73-76% but organic coating lowers the particle deliquescence relative humidity (DRH) to 63-73%. The DRHs of these aerosol particles are clearly smaller than that of pure ammonium sulfate particles which is 80%. Since RH in ambient air was relatively high, ranging from 65% to 85% during our study period, most particles at our sampling site were in liquid phase. Our results suggest that liquid phase reactions in aerosol particles may contribute to SO2 to sulfuric acid conversion in the acid precipitation area.

  9. 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.

  10. 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

  11. Aerosol Physical and Chemical Properties Before and After the Manaus Plume in the GoAmazon2014 Experiment

    NASA Astrophysics Data System (ADS)

    Artaxo, P.; Barbosa, H. M.; Ferreira De Brito, J.; Wurm, F.; Holanda, B. A.; Carbone, S.; Arana, A.; Cirino, G. G.; Souza, R. A. F. D.; Rizzo, L. V.; Martin, S. T.; Andreae, M. O.; Holben, B. N.; Schafer, J.

    2014-12-01

    As part of the GoAmazon2014 experiment, several aerosol and trace gas monitoring stations are being operated for at least one year before and after the Manaus plume. Three sites are being operated in pristine conditions, with atmospheric properties under natural biogenic conditions. These three sites called T0 are: ATTO (Amazon Tall Tower Observatory), ZF2 ecological research site and a third site called EMBRAPA. After the air masses are exposed to the Manaus plume, one site (called T2) is being operated right on the opposite side of the Negro River under the direct influence of the Manaus plume at 5 Km downwind of Manaus. Finally, at about 150 Km downwind of Manaus is the T3 Manacapuru site. Aerosol chemical composition is being analyzed using filters for fine (PM2.5) and coarse mode aerosol as well as three Aerodyne ACSM (Aerosol Chemical Speciation Monitors) instruments. Aerosol absorption is being studied with several aethalometers and MAAP (Multi Angle Absorption Photometers). Aerosol light scattering are being measured at several wavelengths using nephelometers. Aerosol size distribution is determined using scanning mobility particle sizers. The aerosol column is measures using AERONET sunphotometers before and after the Manaus plume, as well as several Lidar systems. The three sites before the Manaus plume show remarkable similar variability in aerosol concentrations and optical properties. This pattern is very different at the T2 site, with large aerosol concentrations enhancing aerosol absorption and scattering significantly. The aerosol is very oxidized before being exposed to the Manaus plume, and this pattern changes significantly for T2 and T3 sites, with a much higher presence of less oxidized aerosol. Typical ozone concentrations at mid-day before Manaus plume is a low 10-12 ppb, value that changes to 50-70 ppb for air masses suffering the influence of Manaus plume. A detailed comparison of aerosol characteristics and composition for the several

  12. Experimental Protocol to Investigate Particle Aerosolization of a Product Under Abrasion and Under Environmental Weathering.

    PubMed

    Shandilya, Neeraj; Le Bihan, Olivier Louis; Bressot, Christophe; Morgeneyer, Martin

    2016-09-16

    The present article presents an experimental protocol to investigate particle aerosolization of a product under abrasion and under environmental weathering, which is a fundamental element to the approach of nanosafety-by-design of nanostructured products for their durable development. This approach is basically a preemptive one in which the focus is put on minimizing the emission of engineered nanomaterials' aerosols during the usage phase of the product's life cycle. This can be attained by altering its material properties during its design phase without compromising with any of its added benefits. In this article, an experimental protocol is presented to investigate the nanosafety-by-design of three commercial nanostructured products with respect to their mechanical solicitation and environmental weathering. The means chosen for applying the mechanical solicitation is an abrasion process and for the environmental weathering, it is an accelerated UV exposure in the presence of humidity and heat. The eventual emission of engineered nanomaterials is studied in terms of their number concentration, size distribution, morphology and chemical composition. The purpose of the protocol is to study the emission for test samples and experimental conditions which are corresponding to real life situations. It was found that the application of the mechanical stresses alone emits the engineered nanomaterials' aerosols in which the engineered nanomaterial is always embedded inside the product matrix, thus, a representative product element. In such a case, the emitted aerosols comprise of both nanoparticles as well as microparticles. But if the mechanical stresses are coupled with the environmental weathering, the experimental protocol reveals then the eventual deterioration of the product, after a certain weathering duration, may lead to the emission of the free engineered nanomaterial aerosols too.

  13. Aerosol fine fraction in the Venice Lagoon: Particle composition and sources

    NASA Astrophysics Data System (ADS)

    Prodi, F.; Belosi, F.; Contini, D.; Santachiara, G.; Di Matteo, L.; Gambaro, A.; Donateo, A.; Cesari, D.

    2009-04-01

    The work presents a characterisation of aerosol sampled during three campaigns conducted in the Venice Lagoon from 30 June to 21 July 2004, from 15 February to 10 March 2005 and from 8 May to 25 May 2006. The results yield information about the physical-chemical characteristics of fine aerosol, the possible sources and its fate. Sulphate (SO 42-), nitrate (NO 3-) and ammonium (NH 4+) are identified as the main water soluble components. The sum of these ions in the spring campaign 2006 varies from 51% to nearly 100% of PM2.5 fraction aerosol. NH 4+ is found to be significantly correlated to non-sea-salt sulphate (nss-SO 42-) and NO 3-, thus indicating the prevalent presence of ammonium nitrate and sulphate. The overall lack of a clear diurnal and seasonal cycle of sulphate suggests a transport from the Po Valley, while the diurnal and seasonal profile of nitrate concentrations suggests a prevalence of local generation. Sulphates from sea water through oxidation of dimethylsulfide (DMS) are not negligible (about 10% of the anthropogenic sulphate). The marine aerosol contribution to PM1 and PM2.5 fractions, calculated using Na + as a tracer of sea-salts, is low (range 1-6%). In some cases chlorine depletion is observed. The content of chlorine in the aerosol particle is mostly higher than expected for marine environments (considered on the basis of Cl -/Na + ratio). Therefore, specific sources for the element have been suggested. Oxalic acid anion, which accounts for 55% of the organic compounds examined, presents mean values 180 ng m - 3 and 161 ng m - 3 in the winter and spring campaigns, comparable with reported values in low polluted urban areas. In the winter campaign there is a high correlation between formate and acetate ( R2 = 0.93), suggesting that a common source makes a high contribution to the measured concentrations.

  14. Origin of nitrocatechols and alkylated-nitrocatechols in atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Marchand, Nicolas; Sylvestre, Alexandre; Ravier, Sylvain; Detournay, Anais; Bruns, Emily; Temime-Roussel, Brice; Slowik, Jay; El Haddad, Imad; Prevot, Andre

    2013-04-01

    Biomass burning constitutes one of the major sources of aerosol particles in most of the environments during winter. If a lot of information is available in the literature on the primary fraction of biomass burning aerosol particles, almost nothing is known regarding the formation of Secondary Organic Aerosol (SOA) from the chemical mixture emitted by this source. Recently methylated nitrocatechol have been identified in atmospheric particles collected in winter. These compounds are strongly associated with biomass burning tracers such as levoglucosan and are suspected to be of secondary origin since they can be formed through the oxidation of cresol significantly emitted by biomass burning. However, nitrocatechols are particularly difficult to analyze using classical techniques like HPLC-MS or GC-MS. In the present study, we adopt a new analytical approach. Direct analysis in real time (DART), introduced by Cody et al. (2005), allows direct analysis of gases, liquids, solids and materials on surfaces. Thus, for particles collected onto filters, the sample preparation step is simplified as much as possible, avoiding losses and reducing to the minimum the analytical procedure time. Two analytic modes can be used. In positive mode, [MH]+ ions are formed by proton transfer reaction ; whereas in negative ionization mode, [MH]-, M- and [MO2]- ions are formed. DART source enables soft ionization and produces simple mass spectra suitable for analysis of complex matrices, like organic aerosol, in only a few seconds. For this study, the DART source was coupled to a Q-ToF mass spectrometer (Synapt G2 HDMS, Waters), with a mass resolution up to 40 000. The analysis of atmospheric aerosol samples, collected in Marseille during winter 2011 (APICE project), with the DART/Q-ToF approach highlighted the abundance of nitrocatechols and alkylated nitrocatechols. Their temporal trends were also very similar to those of levoglucosan or dihydroabietic acid well known tracers of biomass

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

    NASA Astrophysics Data System (ADS)

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

    1994-05-01

    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°, 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 size distribution, based on the spectral dependence of the optical thickness, a, cannot estimate accurately the phase function (up to 50% error for λ = 0.87 μm). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with α. 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 distributions before the injection of stratospheric aerosol consistently show two modes, sulfate particles with rm

  16. Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

    NASA Astrophysics Data System (ADS)

    Gorzelska, K.; Talbot, R. W.; Klemm, K.; Lefer, B.; Klemm, O.; Gregory, G. L.; Anderson, B.; Barrie, L. A.

    1994-01-01

    Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July-August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) SB/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with"background"air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forested region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

  17. Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

    NASA Technical Reports Server (NTRS)

    Gorzelska, K.; Talbot, R. W.; Klemm, K.; Lefer, B.; Klemm, O.; Gregory, G. L.; Anderson, B.; Barrie, L. A.

    1994-01-01

    Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

  18. Observations and Modeling of the Green Ocean Amazon 2014/15: Transmission Electron Microscopy Analysis of Aerosol Particles Field Campaign Report

    SciTech Connect

    Buseck, Peter

    2016-03-01

    During two Intensive Operational Periods (IOP), we collected samples at 3-hour intervals for transmission electron microscopy analysis. The resulting transmission electron microscopy images and compositions were analyzed for the samples of interest. Further analysis will be done especially for the plume of interest. We found solid spherical organic particles from rebounded samples collected with Professor Scot Martin’s group (Harvard University). Approximately 30% of the rebounded particles at 95% relative humidity were spherical organic particles. Their sources and formation process are not known, but such spherical particles could be solid and will have heterogeneous chemical reactions. We observed many organic particles that are internally mixed with inorganic elements such as potassium and nitrogen. They are either homogeneously mixed or have inorganic cores with organic aerosol coatings. Samples collected from the Manaus, Brazil, pollution plume included many nano-size soot particles mixed with organic material and sulfate. Aerosol particles from clean periods included organic aerosol particles, sulfate, sea salt, dust, and primary biogenic aerosol particles. There was more dust, primary biogenic aerosol, and tar balls in samples taken during IOP1 than those taken during IOP2. Many dust particles were found between March 2 and 3.

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

    EPA Science Inventory

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

  20. Particle size distribution of ambient aerosols in an industrial area.

    PubMed

    Rao, B Padma; Srivastava, A; Yasmin, F; Ray, S; Gupta, N; Chauhan, C; Rao, C V C; Wate, S R

    2012-05-01

    Aerosol samples of PM(10) and PM(2.5) were collected from 38 sampling locations in and around the industrial area. The 24 h average mass concentration of PM(10) and PM(2.5) was 137.5 and 61.5 μg/m(3) respectively during summer, 122 and 97.5 μg/m(3) respectively in winter and 70 and 54 μg/m(3) respectively during post monsoon season. The relative contribution of coarse, fine and ultrafine particle to ambient air was analyzed for its temporal and seasonal variability in an industrialized area. This paper aims to establish baseline between PM(10) and PM(2.5) mass concentration levels.

  1. Infrared spectroscopic study of the effect of oleic acid on the deliquescence behaviour of ammonium sulfate aerosol particles.

    PubMed

    Nájera, Juan J; Horn, Andrew B

    2009-01-21

    In order to accurately assess the impact of fatty acids on the hygroscopic properties of atmospheric aerosol particles, (NH4)2SO4 (ammonium sulfate) and oleic acid (cis-9-octadecenoic acid) were chosen to perform this study as components of the particle phase. Micron-sized (700-900 nm) particles containing (NH4)2SO4 and oleic acid were generated by nebulising aqueous solutions of (NH4)2SO4 and sodium oleate. In this study, the effect of oleic acid on the deliquescence phase transition of particles was investigated in a room temperature aerosol flow tube (AFT) system using Fourier transform infrared (FTIR) spectroscopy. Particles morphologies and their chemical compositions were also analysed using a variety of techniques, including attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy and scanning electron microscopy/energy dispersive X-ray analysis (SEM/EDX). The deliquescence relative humidity (DRH) of the (NH4)2SO4 component, determined at 81+/-2%, was slightly lowered or not affected by the presence of different thickness of oleic acid (21 nm, 44 nm and 109 nm) present in the particles. Analyses of the results presented here are consistent with earlier studies about the possible effects of water-insoluble fatty acids coatings on the phase transitions of atmospheric aerosol particles.

  2. Time Resolved Chemical Analysis of Anthropogenic Aerosols in Norway, a Study of Long-Range Transport

    NASA Astrophysics Data System (ADS)

    Indresand, H.; Waddell, J. A.; Cliff, S. S.; Perry, K. D.; Yttri, K.; Dye, C.; Kelly, P. B.

    2004-12-01

    Anthropogenic fine particulate matter produced by the burning of carbonaceous fuels is a complex issue that transcends political and geographical boundaries. Anthropogenic fine aerosols are tranported to Norway from the British Isles and continental Europe. Two 3-DRUM impactor samplers were used to collect size-separated PM2.5 aerosol samples (2.5 - 1.15, 1.15-0.34, 0.34-0.1 µm Da) at two sites, Birkenes and Kjeller for a six-week period in June and July. The samples were analyzed with three-hour time resolution by Synchrotron X-ray Fluorescence and Time-of-Flight Mass Spectrometry. S-XRF determined three-hour mass averages for elements heavier than Na, while the TOFMS was used for chemical speciation as a function of time and size. Positive ion spectra showed K+, Na+ and organic molecular ions between 200 - 400 m/z. Negative ion spectra detected carbon clusters, Cl-, Br-, I-, NO2-, NO3-, CN-, CNO-, SO3-, HSO4-, methyl sulfonic acid (MSA), and various organic acid salts. The chemical signature of the sources are identified using high time resolution in combination with air mass back trajectories. Chemical modification of the aerosol during transport is examined as a function of particle size.

  3. 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

  4. Daily and hourly chemical impact of springtime transboundary aerosols on Japanese air quality

    NASA Astrophysics Data System (ADS)

    Moreno, T.; Kojima, T.; Amato, F.; Lucarelli, F.; de la Rosa, J.; Calzolai, G.; Nava, S.; Chiari, M.; Alastuey, A.; Querol, X.; Gibbons, W.

    2013-02-01

    The regular eastward drift of transboundary aerosol intrusions from the Asian mainland into the NW Pacific region has a pervasive impact on air quality in Japan, especially during springtime. Analysis of 24-h filter samples with Inductively Coupled Plasma Atomic Emission Spectroscopy (ICP-AES) and Mass Spectrometry (ICP-MS), and hourly Streaker with Particle Induced X-ray Emission (PIXE) samples collected continuously for six weeks reveal the chemistry of successive waves of natural mineral desert dust ("Kosa") and metalliferous sulphatic pollutants arriving in western Japan during spring 2011. The main aerosol sources recognised by Positive Matrix Factorization (PMF) analysis of Streaker data are mineral dust and fresh sea salt (both mostly in the coarser fraction PM2.5-10), As-bearing sulphatic aerosol (PM0.1-2.5), metalliferous sodic particulate matter (PM) interpreted as aged, industrially contaminated marine aerosol, and ZnCu-bearing aerosols. Whereas mineral dust arrivals are typically highly transient, peaking over a few hours, sulphatic intrusions build up and decline more slowly, and are accompanied by notable rises in ambient concentrations of metallic trace elements such as Pb, As, Zn, Sn and Cd. The magnitude of the loss in regional air quality due to the spread and persistence of pollution from mainland Asia is especially clear when cleansing oceanic air advects westward across Japan, removing the continental influence and reducing concentrations of the undesirable metalliferous pollutants by over 90%. Our new chemical database, especially the Streaker data, demonstrates the rapidly changing complexity of ambient air inhaled during these transboundary events, and implicates Chinese coal combustion as the main source of the anthropogenic aerosol component.

  5. 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.

  6. 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.

  7. 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.

  8. Molecular-scale evidence of aerosol particle formation via sequential addition of HIO3

    NASA Astrophysics Data System (ADS)

    Sipilä, Mikko; Sarnela, Nina; Jokinen, Tuija; Henschel, Henning; Junninen, Heikki; Kontkanen, Jenni; Richters, Stefanie; Kangasluoma, Juha; Franchin, Alessandro; Peräkylä, Otso; Rissanen, Matti P.; Ehn, Mikael; Vehkamäki, Hanna; Kurten, Theo; Berndt, Torsten; Petäjä, Tuukka; Worsnop, Douglas; Ceburnis, Darius; Kerminen, Veli-Matti; Kulmala, Markku; O'Dowd, Colin

    2016-09-01

    Homogeneous nucleation and subsequent cluster growth leads to the formation of new aerosol particles in the atmosphere. The nucleation of sulfuric acid and organic vapours is thought to be responsible for the formation of new particles over continents, whereas iodine oxide vapours have been implicated in particle formation over coastal regions. The molecular clustering pathways that are involved in atmospheric particle formation have been elucidated in controlled laboratory studies of chemically simple systems, but direct molecular-level observations of nucleation in atmospheric field conditions that involve sulfuric acid, organic or iodine oxide vapours have yet to be reported. Here we present field data from Mace Head, Ireland, and supporting data from northern Greenland and Queen Maud Land, Antarctica, that enable us to identify the molecular steps involved in new particle formation in an iodine-rich, coastal atmospheric environment. We find that the formation and initial growth process is almost exclusively driven by iodine oxoacids and iodine oxide vapours, with average oxygen-to-iodine ratios of 2.4 found in the clusters. On the basis of this high ratio, together with the high concentrations of iodic acid (HIO3) observed, we suggest that cluster formation primarily proceeds by sequential addition of HIO3, followed by intracluster restructuring to I2O5 and recycling of water either in the atmosphere or on dehydration. Our study provides ambient atmospheric molecular-level observations of nucleation, supporting the previously suggested role of iodine-containing species in the formation of new aerosol particles, and identifies the key nucleating compound.

  9. Molecular-scale evidence of aerosol particle formation via sequential addition of HIO3.

    PubMed

    Sipilä, Mikko; Sarnela, Nina; Jokinen, Tuija; Henschel, Henning; Junninen, Heikki; Kontkanen, Jenni; Richters, Stefanie; Kangasluoma, Juha; Franchin, Alessandro; Peräkylä, Otso; Rissanen, Matti P; Ehn, Mikael; Vehkamäki, Hanna; Kurten, Theo; Berndt, Torsten; Petäjä, Tuukka; Worsnop, Douglas; Ceburnis, Darius; Kerminen, Veli-Matti; Kulmala, Markku; O'Dowd, Colin

    2016-09-22

    Homogeneous nucleation and subsequent cluster growth leads to the formation of new aerosol particles in the atmosphere. The nucleation of sulfuric acid and organic vapours is thought to be responsible for the formation of new particles over continents, whereas iodine oxide vapours have been implicated in particle formation over coastal regions. The molecular clustering pathways that are involved in atmospheric particle formation have been elucidated in controlled laboratory studies of chemically simple systems, but direct molecular-level observations of nucleation in atmospheric field conditions that involve sulfuric acid, organic or iodine oxide vapours have yet to be reported. Here we present field data from Mace Head, Ireland, and supporting data from northern Greenland and Queen Maud Land, Antarctica, that enable us to identify the molecular steps involved in new particle formation in an iodine-rich, coastal atmospheric environment. We find that the formation and initial growth process is almost exclusively driven by iodine oxoacids and iodine oxide vapours, with average oxygen-to-iodine ratios of 2.4 found in the clusters. On the basis of this high ratio, together with the high concentrations of iodic acid (HIO3) observed, we suggest that cluster formation primarily proceeds by sequential addition of HIO3, followed by intracluster restructuring to I2O5 and recycling of water either in the atmosphere or on dehydration. Our study provides ambient atmospheric molecular-level observations of nucleation, supporting the previously suggested role of iodine-containing species in the formation of new aerosol particles, and identifies the key nucleating compound.

  10. A broad supersaturation scanning (BS2) approach for rapid measurement of aerosol particle hygroscopicity and cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Su, H.; Cheng, Y.; Ma, N.; Wang, Z.; Wang, X.; Pöhlker, M.; Nillius, B.; Wiedensohler, A.; Pöschl, U.

    2015-09-01

    The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to understand aerosol-cloud interactions and their climate impact. It can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach is also applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

  11. A broad supersaturation scanning (BS2) approach for rapid measurement of aerosol particle hygroscopicity and cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Su, Hang; Cheng, Yafang; Ma, Nan; Wang, Zhibin; Wang, Xiaoxiang; Pöhlker, Mira L.; Nillius, Björn; Wiedensohler, Alfred; Pöschl, Ulrich

    2016-10-01

    The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to the understanding of aerosol-cloud interactions and their impact on climate. They can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed the broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned, reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach may also be applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for aircraft and long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

  12. Surface submicron aerosol chemical composition: What fraction is not sulfate?

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Miller, T. L.; Coffman, D. J.; Johnson, J. E.; Harris, J. M.; Ogren, J. A.; Forbes, G.; Anderson, T. L.; Covert, D. S.; Rood, M. J.

    2000-03-01

    Measurements of submicron aerosol mass and the mass of major ionic components have been made over the past 5 years on cruises in the Pacific and Southern Oceans and at monitoring stations across North America (Barrow, Alaska; Cheeka Peak, Washington; Bondville, Illinois; and Sable Island, Nova Scotia). Reported here are submicron concentrations of aerosol mass, nonsea salt (nss) sulfate, sea salt, methanesulfonate, other nss inorganic ions, and residual, or chemically unanalyzed, mass. Residual mass concentrations are based on the difference between simultaneously measured aerosol mass and the mass of the major ionic components. A standardized sampling protocol was used for all measurements making the data from each location directly comparable. For the Pacific and Southern Oceans, concentrations of the chemical components are presented in zonally averaged 20° latitude bins. For the monitoring stations, mean concentrations are presented for distinct air mass types (marine, clean continental, and polluted based on air mass back trajectories). In addition, percentile information for each chemical component is given to indicate the variability in the measured concentrations. Mean nss sulfate submicron aerosol mass fractions for the different latitude bins of the Pacific ranged from 0.14±0.01 to 0.34±0.03 (arithmetic mean±absolute uncertainty at the 95% confidence level). The lowest average value occurred in the 40°-60°S latitude band where nss sulfate concentrations were low due to the remoteness from continental sources and sea salt concentrations were relatively high. Mean nss sulfate aerosol mass fractions were more variable at the monitoring stations ranging from 0.13±0.004 to 0.65±0.02. Highest values occurred in polluted air masses at Bondville and Sable Island. Sea salt mean mass fractions ranged between 0.20±0.02 and 0.53±0.03 at all latitude bands of the Pacific (except 20°-40°N where the residual mass fraction was relatively high) and at Barrow

  13. Optical properties of salt particles of a sea aerosol (laboratory experiment)

    NASA Astrophysics Data System (ADS)

    Gubareva, T. V.

    2002-02-01

    The scientific clause is devoted to complex examinations of optical properties of micro crystals of alkali-halides simulative an atmospheric salt aerosol. In laboratory requirements the interactions in system 'micro crystals of salts - gas phase' were explored at superimposition of high- energy fields. Thus the scale of radiation and cold air plasma was utilized ultraviolet, X-ray. Is shown, that the presence of high-energy fields gives in interaction of micro crystals and gas phase. At interaction the chemical composition, structure and optical properties of salt particles changes. The scientific clause is devoted to study of optical properties of salt particles mainly in infrared range of a spectrum. The purpose of operation is the study of transformation of salt micro crystals and its communications with optical parameters.

  14. Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

    NASA Technical Reports Server (NTRS)

    Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

    2013-01-01

    Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

  15. Evaluation of aerosol mixing state classes in the GISS modelE-MATRIX climate model using single-particle mass spectrometry measurements

    NASA Astrophysics Data System (ADS)

    Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

    2013-09-01

    Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 µm, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 µm contain large fractions of organic material, internally mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  17. Measurements of the absorption and scattering coefficients of aerosol particles in suburb of Nanjing (China)

    NASA Astrophysics Data System (ADS)

    Yin, Yan; Chen, Yu; Wang, Weiwei; Yan, Jiade; Qian, Ling; Tong, Yaoqing; Lin, Zhenyi

    2008-08-01

    The absorption and scattering coefficients of atmospheric aerosols were continuously measured with a Photoacoustic Soot Spectrometer (PASS, DMT Inc. USA) at a suburb site of Nanjing, one of the regions experiencing rapid industrialization in China. The measurements were carried out during autumn and winter 2007. A preliminary analysis of the data shows that, the scattering coefficient, Bscat, is two to ten times larger than the absorption coefficient, Babs, implying that the aerosols formed/emitted in this area are more scattering than previous assumed, and can be more important in cooling the Earth-atmosphere system. The results also indicate that the absolute values of both parameters are very much dependent on the meteorological conditions, such as wind speed and direction, fog, rain, etc. as well as the time of the day. Higher values often appear at nighttimes when wind is weak, especially when a temperature inverse layer is present near the surface. Higher values of Bscat and Babs were also observed under hazy and foggy weather conditions or when wind is blown from east, where a large industrial zone is located. Simultaneous measurements of the number concentrations, chemical compositions, and size distributions of aerosol particles are used to explain the characteristics of the changes in Bscat and Babs.

  18. Effects of Hydrodynamic Interaction in Aerosol Particle Settling: Mesoscopic Particle-level Full Dynamics Simulations

    NASA Astrophysics Data System (ADS)

    Li, Shuiqing; Yang, Mengmeng; Marshall, Jeffrey

    2014-11-01

    A new mesoscopic particle-level approach is developed for the full dynamics simulation (FDS) of the settling of systems of aerosol micro-particles. The approach efficiently combines an adhesive discrete-element method for particle motions and an Oseen dynamics method for hydrodynamic interactions. Compared to conventional Stokeslet and Oseenlet simulations, the FDS not only accounts for the cloud-scale fluid inertia effect and the particle inertia effect, but also overcomes the singularity problem using a soft-sphere model of adhesive contact. The effect of hydrodynamic interactions is investigated based on FDS results. The particle inertia is found to reduce the mobility of particle clouds and to elongate the cloud on vertical direction. Meanwhile, the fluid inertia decreases the settling velocity by weakening the hydrodynamic interaction and tends to flatten the cloud, leading to breakup. Expressions for the settling velocity of particle cloud are proposed with consideration of fluid inertia effect and the cloud shape. Finally, the transformation in settling behavior from a finite particle cloud to an unbounded uniform suspension is explained. This work has been funded by the National Natural Science Funds of China (No. 50976058), and by the National Key Basic Research and Development Program (2013CB228506).

  19. Iron Speciation and Mixing in Single Aerosol Particles from the Asian Continental Outflow

    SciTech Connect

    Moffet, Ryan C.; Furutani, Hiroshi; Rodel, Tobias; Henn, Tobias R.; Sprau, Peter; Laskin, Alexander; Uematsu, Mitsuo; Gilles, Marry K.

    2012-04-04

    Bioavailable iron from atmospheric aerosol is an essential nutrient that can control oceanic productivity, thereby impacting the global carbon budget and climate. Particles collected on Okinawa Island during an atmospheric pollution transport event from China were analyzed using complementary single particle techniques to determine the iron source and speciation. Comparing the spatial distribution of iron within ambient particles and standard Asian mineral dust, it was determined that field-collected atmospheric Fe-containing particles have numerous sources, including anthropogenic sources such as coal combustion. Fe-containing particles were found to be internally mixed with secondary species such as sulfate, soot, and organic carbon. The mass weighted average Fe(II) fraction (defined as Fe(II)/[Fe(II)+Fe(III)]) was determined to be 0.33 {+-} 0.08. Within the experimental uncertainty, this value lies close to the range of 0.26-0.30 determined for representative Asian mineral dust. Previous studies have indicated that the solubility of iron from combustion is much higher than that from mineral dust. Therefore, chemical and/or physical differences other than oxidation state may help explain the higher solubility of iron in atmospheric particles.

  20. A recirculation aerosol wind tunnel for evaluating aerosol samplers and measuring particle penetration through protective clothing materials.

    PubMed

    Jaques, Peter A; Hsiao, Ta-Chih; Gao, Pengfei

    2011-08-01

    A recirculation aerosol wind tunnel was designed to maintain a uniform airflow and stable aerosol size distribution for evaluating aerosol sampler performance and determining particle penetration through protective clothing materials. The oval-shaped wind tunnel was designed to be small enough to fit onto a lab bench, have optimized dimensions for uniformity in wind speed and particle size distributions, sufficient mixing for even distribution of particles, and minimum particle losses. Performance evaluation demonstrates a relatively high level of spatial uniformity, with a coefficient of variation of 1.5-6.2% for wind velocities between 0.4 and 2.8 m s(-1) and, in this range, 0.8-8.5% for particles between 50 and 450 nm. Aerosol concentration stabilized within the first 5-20 min with, approximately, a count median diameter of 135 nm and geometric standard deviation of 2.20. Negligible agglomerate growth and particle loss are suggested. The recirculation design appears to result in unique features as needed for our research.

  1. 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...

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

    NASA Technical Reports Server (NTRS)

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

    2014-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2014-01-01

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

  4. Direct photolysis of α-pinene ozonolysis secondary organic aerosol: effect on particle mass and peroxide content.

    PubMed

    Epstein, Scott A; Blair, Sandra L; Nizkorodov, Sergey A

    2014-10-07

    Primary and secondary organic aerosols (POA and SOA) contain a complex mixture of multifunctional chemicals, many of which are photolabile. Much of the previous work that aimed to understand the chemical evolution (aging) of POA and SOA has focused on the reactive uptake of gas-phase oxidants by particles. By stripping volatile compounds and ozone from α-pinene ozonolysis SOA with three 1-m-long denuders, and exposing the residual particles in a flow cell to near-ultraviolet (λ>300 nm) radiation, we find that condensed-phase photochemistry can induce significant changes in SOA particle size and chemical composition. The particle-bound organic peroxides, which are highly abundant in α-pinene ozonolysis SOA (22 ± 5% by weight), have an atmospheric photolysis lifetime of about 6 days at a 24-h average solar zenith angle (SZA) of 65° experienced at 34° latitude (Los Angeles) in the summer. In addition, the particle diameter shrinks 0.56% per day under these irradiation conditions as a result of the loss of volatile photolysis products. Experiments with and without the denuders show similar results, suggesting that condensed-phase processes dominate over heterogeneous reactions of particles with organic vapors, excess ozone, and gas-phase free radicals. These condensed-phase photochemical processes occur on atmospherically relevant time scales and should be considered when modeling the evolution of organic aerosol in the atmosphere.

  5. Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Arangio, Andrea M.; Tong, Haijie; Socorro, Joanna; Pöschl, Ulrich; Shiraiwa, Manabu

    2016-10-01

    Fine particulate matter plays a central role in the adverse health effects of air pollution. Inhalation and deposition of aerosol particles in the respiratory tract can lead to the release of reactive oxygen species (ROS), which may cause oxidative stress. In this study, we have detected and quantified a wide range of particle-associated radicals using electron paramagnetic resonance (EPR) spectroscopy. Ambient particle samples were collected using a cascade impactor at a semi-urban site in central Europe, Mainz, Germany, in May-June 2015. Concentrations of environmentally persistent free radicals (EPFR), most likely semiquinone radicals, were found to be in the range of (1-7) × 1011 spins µg-1 for particles in the accumulation mode, whereas coarse particles with a diameter larger than 1 µm did not contain substantial amounts of EPFR. Using a spin trapping technique followed by deconvolution of EPR spectra, we have also characterized and quantified ROS, including OH, superoxide (O2-) and carbon- and oxygen-centered organic radicals, which were formed upon extraction of the particle samples in water. Total ROS amounts of (0.1-3) × 1011 spins µg-1 were released by submicron particle samples and the relative contributions of OH, O2-, C-centered and O-centered organic radicals were ˜ 11-31, ˜ 2-8, ˜ 41-72 and ˜ 0-25 %, respectively, depending on particle sizes. OH was the dominant species for coarse particles. Based on comparisons of the EPR spectra of ambient particulate matter with those of mixtures of organic hydroperoxides, quinones and iron ions followed by chemical analysis using liquid chromatography mass spectrometry (LC-MS), we suggest that the particle-associated ROS were formed by decomposition of organic hydroperoxides interacting with transition metal ions and quinones contained in atmospheric humic-like substances (HULIS).

  6. Aerosol chemical vapor deposition of metal oxide films

    DOEpatents

    Ott, Kevin C.; Kodas, Toivo T.

    1994-01-01

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

  7. Using the Relationship between MODIS Aerosol Optical Thickness and OMI Trace Gas Columns to better understand Aerosol Formation and Chemical Composition

    NASA Astrophysics Data System (ADS)

    Veefkind, Pepijn; Boersma, Folkert; Wang, Jun; Levelt, Pieternel

    2010-05-01

    Aerosols are one of the leading uncertainties in global and regional climate change. One of the most important reasons for the limited understanding of the effects of aerosols is their strong temporal and spatial variability in chemical composition and size distribution. Important anthropogenic sources for aerosols are transportation, power plants, industries and biomass burning. Natural sources include windblown desert dust, sea spray, biogenic emissions, volcanoes, and biomass burning. Together, these sources form a complex chemical mixture of desert dust, sea salt, sulfates, nitrates and organic material. To better understand the Earth's climate system, accurate knowledge is needed on the complex relation between the emissions of precursor gases and primary aerosol particles, and aerosol composition. Satellite measurements have the horizontal and temporal coverage to assess the global effect of aerosols on climate. In addition to the information on aerosols, tropospheric columns of nitrogen dioxide (NO2), formaldehyde (HCHO) and sulfur dioxide (SO2) can be observed from space. In this contribution, the spatial and temporal correlations between AOT and tropospheric columns of NO2, SO2 and HCHO are used to derive information on the composition of the aerosols particles. Spatial correlation between AOT and NO2 indicate that the aerosols are from combustion processes, such as fossil fuel and biomass burning. The AOT to NO2 ratio provides zeroth order information on the combustion sources. This ratio is low for regions dominated by controlled fossil fuel combustion and high for biomass burning regions, whereas the difference of this ratio between these regions can be more than two orders of magnitude. Overall the GEOS-CHEM simulations can reproduce the observed AOT-NO2 ratios well. Spatial correlation between AOT and NO2 is found for many of the industrialized ad biomass burning regions in the world. Correlations with HCHO are especially important in biomass burning

  8. 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

  9. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2016-01-01

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

  12. Chemical Aging and Cloud Condensation Nuclei Activity of Biomass Burning Aerosol Proxies in the Presence of OH Radicals

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H., Jr.

    Biomass burning aerosol (BBA) can adversely impact regional and global air quality and represents a significant source of organic aerosol (OA) to the atmosphere that can affect climate. Aerosol particles can alter the transfer of radiation in earth's atmosphere directly by scattering and absorbing radiation or indirectly via cloud formation. Gas-to-particle, also termed heterogeneous, oxidation reactions can significantly alter the particle's physical and chemical properties. In turn, this can lead to the degradation of biomolecular markers for air quality-related aerosol source apportionment studies, the particles' lifetime, and modify the particles' abilities to serve as cloud condensation nuclei (CCN). However, the rates, mechanisms, and conditions by which these multiphase oxidation reactions occur and influence the CCN activity of OA is not well understood. The work presented here aims to determine the reactivity and products from the interaction of BBA surrogate-particles and trace gas-phase oxidants and to link the effects of OA chemical aging on the particles' ability to nucleate clouds. The reactive uptake of OH by BBA surrogate-substrates and particles, including levoglucosan, nitroguaiacol, abietic acid, and methyl-nitrocatechol, was determined as a function of both OH concentration and relative humidity (RH) using chemical ionization mass spectrometry coupled to various flow reactors. OH reactive uptake decreased with increasing OH concentration, indicative of OH adsorption followed by reaction. OH oxidation led to significant volatilization, i.e. mass loss of the organic material, as determined by application of high resolution proton transfer reaction time-of-flight mass spectrometry. Volatilized reaction products were identified, providing mechanistic insight of the chemical pathways in the heterogeneous OH oxidation of BBA. The reactive uptake of OH by levoglucosan particles increased with RH due to enhanced OH and organic bulk diffusivity. In

  13. Collective surfing of chemically active particles.

    PubMed

    Masoud, Hassan; Shelley, Michael J

    2014-03-28

    We study theoretically the collective dynamics of immotile particles bound to a 2D surface atop a 3D fluid layer. These particles are chemically active and produce a chemical concentration field that creates surface-tension gradients along the surface. The resultant Marangoni stresses create flows that carry the particles, possibly concentrating them. For a 3D diffusion-dominated concentration field and Stokesian fluid we show that the surface dynamics of active particle density can be determined using nonlocal 2D surface operators. Remarkably, we also show that for both deep or shallow fluid layers this surface dynamics reduces to the 2D Keller-Segel model for the collective chemotactic aggregation of slime mold colonies. Mathematical analysis has established that the Keller-Segel model can yield finite-time, finite-mass concentration singularities. We show that such singular behavior occurs in our finite-depth system, and study the associated 3D flow structures.

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

    SciTech Connect

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

    2009-11-27

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

  15. 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.

  16. 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.

  17. Regional-scale simulations of fungal spore aerosols using an emission parameterization adapted to local measurements of fluorescent biological aerosol particles

    NASA Astrophysics Data System (ADS)

    Hummel, M.; Hoose, C.; Gallagher, M.; Healy, D. A.; Huffman, J. A.; O'Connor, D.; Pöschl, U.; Pöhlker, C.; Robinson, N. H.; Schnaiter, M.; Sodeau, J. R.; Toprak, E.; Vogel, H.

    2014-04-01

    Fungal spores as a prominent type of primary biological aerosol particles (PBAP) have been incorporated into the COSMO-ART regional atmospheric model, using and comparing three different emission parameterizations. Two literature-based emission rates derived from fungal spore colony counts and chemical tracer measurements were used as a parameterization baseline for this study. A third, new emission parameterization was adapted to field measurements of fluorescent biological aerosol particles (FBAP) from four locations across Northern Europe. FBAP concentrations can be regarded as a lower estimate of total PBAP concentrations. Size distributions of FBAP often show a distinct mode at approx. 3 μm, corresponding to a diameter range characteristic for many fungal spores. Previous studies have suggested the majority of FBAP in several locations are dominated by fungal spores. Thus, we suggest that simulated fungal spore concentrations obtained from the emission parameterizations can be compared to the sum of total FBAP concentrations. A comparison reveals that parameterized estimates of fungal spore concentrations based on literature numbers underestimate measured FBAP concentrations. In agreement with measurement data, the model results show a diurnal cycle in simulated fungal spore concentrations, which may develop partially as a consequence of a varying boundary layer height between day and night. Measured FBAP and simulated fungal spore concentrations also correlate similarly with simulated temperature and humidity. These meteorological variables, together with leaf area index, were chosen to drive the new emission parameterization discussed here. Using the new emission parameterization on a model domain covering Western Europe, fungal spores in the lowest model layer comprise a fraction of 15% of the total aerosol mass over land and reach average number concentrations of 26 L-1. The results confirm that fungal spores and biological particles may account for a

  18. Influence of Aerosol Chemical Composition on Heterogeneous Ice Formation under Mid-Upper Troposphere Conditions

    NASA Astrophysics Data System (ADS)

    Kanji, Z. A.; Niemand, M.; Saathoff, H.; Möhler, O.; Chou, C.; Abbatt, J.; Stetzer, O.

    2011-12-01

    Aerosols are involved in cooling/warming the atmosphere directly via interaction with incoming solar radiation (aerosol direct effect), or via their ability to act as cloud condensation or ice nuclei (IN) and thus play a role in cloud formation (indirect effect). In particular, the physical properties of aerosols such as size and solubility and chemical composition can influence their behavior and fate in the atmosphere. Ice nucleation taking place via IN is termed as heterogeneous ice nucleation and can take place with via deposition (ice forming on IN directly from the vapor phase), condensation/immersion (freezing via formation of the liquid phase on IN) or condensation (IN colliding with supercooled liquid drops). This presentation shows how the chemical composition and surface area of various tropospherically relevant aerosols influence conditions of temperature (T) and relative humidity (RH) required for heterogeneous ice formation conditions in the mid-upper troposphere regime (253 - 220K)? Motivation for this comes first from, the importance of being able to predict ice formation accurately so as to understand the hydrological cycle since the ice is the primary initiator of precipitation forming clouds. Second, the tropospheric budget of water vapour, an especially active greenhouse gas is strongly influenced by ice nucleation and growth. Third, ice surfaces in the atmosphere act as heterogeneous surfaces for chemical reactions of trace gases (e.g., SO2, O3, NOx and therefore being able to accurately estimate ice formation rates and quantify ice surface concentrations will allow a more accurate calculation of trace gas budgets in the troposphere. Ice nucleation measurements were conducted using a self-developed continuous flow diffusion chamber and static chamber. A number of tropospherically relevant particulates with naturally-varying and laboratory-modified surface chemistry/structure were investigated for their ice formation efficiency based on highest

  19. Measurements of the Size-Resolved Chemical Composition of Marine Boundary Layer Aerosols in Asian Outflow During the ACE-Asia Campaign

    NASA Astrophysics Data System (ADS)

    Guazzotti, S. A.; Sodeman, D. A.; Moffet, R.; Prather, K. A.

    2003-12-01

    The size and chemical composition of individual particles were evaluated with high temporal resolution during the Asian Pacific Regional Aerosol Chemical Characterization Experiment (ACE-Asia) using a transportable aerosol time-of-flight mass spectrometer (ATOFMS) aboard the NOAA Research Vessel Ronald H. Brown. ATOFMS allows characterization of the aerodynamic diameter and chemical composition of individual particles from a polydisperse aerosol. This technique couples aerodynamic particle sizing with time-of-flight mass spectrometry in a single instrument, providing both positive and negative ion mass spectra for each detected particle which are employed to classify the particles into different classes using criteria based searches and a neural network algorithm, ART-2a. Size-resolved chemical characteristics of sampled particles under different synoptic meteorological patterns and at various locations and distances from continental influences are discussed in detail, with special focus given to the associations among different species and the variability in the degrees of aging, reaction, and/or mixing, which can alter the optical properties of these particles. Changes in the aerosol chemical characteristics due to heterogeneous reactions are evidenced in the mass spectra of detected particles by the presence and intensity of specific ion markers (e.g., sulfate, nitrate). The ability to differentiate between particles that have undergone heterogeneous reactions is relevant since these reactions affect several aerosol attributes, such as hygroscopic, optical, and radiative properties. Particularly, heterogeneous reactions/ nucleation on sea-salt and dust particles are discussed together with results of comparison efforts with some relevant laboratory and source characterization studies that allow determination of corresponding ion markers, relative ratios among species, and probable sources from a single particle perspective.

  20. Gas-particle partitioning of primary organic aerosol emissions: (1) Gasoline vehicle exhaust

    NASA Astrophysics Data System (ADS)

    May, Andrew A.; Presto, Albert A.; Hennigan, Christopher J.; Nguyen, Ngoc T.; Gordon, Timothy D.; Robinson, Allen L.

    2013-10-01

    The gas-particle partitioning of the primary organic aerosol (POA) emissions from fifty-one light-duty gasoline vehicles (model years 1987-2012) was investigated at the California Air Resources Board Haagen-Smit Laboratory. Each vehicle was operated over the cold-start unified cycle on a chassis dynamometer and its emissions were sampled using a constant volume sampler. Four independent yet complementary approaches were used to investigate POA gas-particle partitioning: sampling artifact correction of quartz filter data, dilution from the constant volume sampler into a portable environmental chamber, heating in a thermodenuder, and thermal desorption/gas chromatography/mass spectrometry analysis of quartz filter samples. This combination of techniques allowed gas-particle partitioning measurements to be made across a wide range of atmospherically relevant conditions - temperatures of 25-100 °C and organic aerosol concentrations of <1-600 μg m-3. The gas-particle partitioning of the POA emissions varied continuously over this entire range of conditions and essentially none of the POA should be considered non-volatile. Furthermore, for most vehicles, the low levels of dilution used in the constant volume sampler created particle mass concentrations that were greater than a factor of 10 or higher than typical ambient levels. This resulted in large and systematic partitioning biases in the POA emission factors compared to more dilute atmospheric conditions, as the POA emission rates may be over-estimated by nearly a factor of four due to gas-particle partitioning at higher particle mass concentrations. A volatility distribution was derived to quantitatively describe the measured gas-particle partitioning data using absorptive partitioning theory. Although the POA emission factors varied by more than two orders of magnitude across the test fleet, the vehicle-to-vehicle differences in gas-particle partitioning were modest. Therefore, a single volatility distribution

  1. Seasonality of ultrafine and sub-micron aerosols and the inferences on particle formation processes

    NASA Astrophysics Data System (ADS)

    Cheung, H. C.; Chou, C. C.-K.; Chen, M.-J.; Huang, W.-R.; Huang, S.-H.; Tsai, C.-Y.; Lee, C. S.-L.

    2015-08-01

    The aim of this study is to investigate the seasonal variations in the physicochemical properties of atmospheric ultrafine particles (UFPs, d ≤ 100nm) and submicron particles (PM1, d ≤ 1 μm) in an East-Asian urban area, which are hypothesized to be affected by the interchange of summer and winter monsoons. An observation experiment was conducted at the TARO, an urban aerosol station in Taipei, Taiwan, from October 2012 to August 2013. The measurements included the mass concentration and chemical composition of UFPs and PM1, as well as the particle number concentration (PNC) and size distribution (PSD) with size range of 4-736 nm. The results indicate that the mass concentration of PM1 was elevated during cold seasons with peak level of 18.5 μg m-3 in spring, whereas the highest UFPs concentration was measured in summertime with a seasonal mean of 1.62 μg m-3. Moreover, chemical analysis revealed that the UFPs and PM1 were characterized by distinct composition; UFPs were composed mostly of organics, whereas ammonium and sulfate were the major constituents in PM1. The seasonal median of total PNCs ranged from 13.9 × 103 cm-3 in autumn to 19.4 × 103 cm-3 in spring. The PSD information retrieved from the corresponding PNC measurements indicates that the nucleation mode PNC (N4-25) peaked at 11.6 × 103 cm-3 in winter, whereas the Aitken mode (N25-100) and accumulation mode (N100-736) exhibited summer maxima at 6.0 × 103 and 3.1 × 103 cm-3, respectively. The shift in PSD during summertime is attributed to the enhancement in the photochemical production of condensable organic matter that, in turn, contributes to the growth of aerosol particles in the atmosphere. In addition, remarkable photochemical production of particles was observed in spring and summer seasons, which was characterized with averaged particle growth and formation rates of 4.3 ± 0.8 nm h-1 and 1.6 ± 0.8 cm-3 s-1, respectively. The prevalence of new particle formation (NPF) in summer is

  2. 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/organi